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From Mitragotri \"Immunization without Needles\"", "language": "en", "security": "internal", "license": "other", "main": "Copyright agreement for Figure 1-1.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "copyright" }, { "id": "/id/document/140977", "doc_id": 140977, "rev_number": 7, "files": [ { "id": "/id/file/423860", "fileid": 423860, "datasetid": "document", "objectid": 140977, "filename": "Copyright agreement for Figure 1-3.pdf", "mime_type": "application/pdf", "hash": "e5b905baee4e77e77cc3e20504be38d0", "hash_type": "MD5", "filesize": 86376, "mtime": "2024-02-07 11:00:29", "url": "/16289/2/Copyright agreement for Figure 1-3.pdf" } ], "eprint_id": 16289, "pos": 2, "placement": 6, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "For Figure 1-3 in thesis. From O'Brien et al \"Biolistic transfection of neuronal cultures using a hand-held gene gun\"", "language": "en", "security": "internal", "license": "other", "main": "Copyright agreement for Figure 1-3.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "copyright" }, { "id": "/id/document/140978", "doc_id": 140978, "rev_number": 7, "files": [ { "id": "/id/file/423862", "fileid": 423862, "datasetid": "document", "objectid": 140978, "filename": "Copyright agreement for Figure 1-4.pdf", "mime_type": "application/pdf", "hash": "7566706da5187495f6761edd64dd3d5f", "hash_type": "MD5", "filesize": 46350, "mtime": "2024-02-07 11:00:33", "url": "/16289/3/Copyright agreement for Figure 1-4.pdf" } ], "eprint_id": 16289, "pos": 3, "placement": 7, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "For Figure 1-4 in thesis. From Rinberg et al \"Pneumatic capillary gun for ballistic delivery of microparticles\"", "language": "en", "security": "internal", "license": "other", "main": "Copyright agreement for Figure 1-4.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "copyright" }, { "id": "/id/document/140979", "doc_id": 140979, "rev_number": 7, "files": [ { "id": "/id/file/423864", "fileid": 423864, "datasetid": "document", "objectid": 140979, "filename": "Permission for Figure 1-6.pdf", "mime_type": "application/pdf", "hash": "aa43056c94a73b4c13bdb364dc21c0bb", "hash_type": "MD5", "filesize": 48157, "mtime": "2024-02-07 11:00:45", "url": "/16289/4/Permission for Figure 1-6.pdf" } ], "eprint_id": 16289, "pos": 4, "placement": 8, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "For Figure 1-6 in thesis. My advisor, Julie Kornfield, made this figure and gave me permission to use it. She combined figures from other sources, see caption in thesis for more sourcing info.", "language": "en", "security": "internal", "license": "other", "main": "Permission for Figure 1-6.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "copyright" }, { "id": "/id/document/140980", "doc_id": 140980, "rev_number": 7, "files": [ { "id": "/id/file/423866", "fileid": 423866, "datasetid": "document", "objectid": 140980, "filename": "Copyright agreement for Figure 4-13.pdf", "mime_type": "application/pdf", "hash": "1065ebf18fe3bd010ee1a72d8788a423", "hash_type": "MD5", "filesize": 86345, "mtime": "2024-02-07 11:00:49", "url": "/16289/5/Copyright agreement for Figure 4-13.pdf" } ], "eprint_id": 16289, "pos": 5, "placement": 9, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "For Figure 4-13 in thesis. From Bauer et al \"Particle-Mediated Administration of Plasmid DNA on Corneas of BALB/c Mice\"", "language": "en", "security": "internal", "license": "other", "main": "Copyright agreement for Figure 4-13.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "copyright" }, { "id": "/id/document/140993", "doc_id": 140993, "rev_number": 9, "files": [ { "id": "/id/file/423906", "fileid": 423906, "datasetid": "document", "objectid": 140993, "filename": "Dennis Ko Submitted Embargo Request.pdf", "mime_type": "application/pdf", "hash": "fabf1a86485c9ac690e5545a01827a07", "hash_type": "MD5", "filesize": 36821, "mtime": "2024-02-07 12:08:56", "url": "/16289/10/Dennis Ko Submitted Embargo Request.pdf" } ], "eprint_id": 16289, "pos": 10, "placement": 10, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Dennis Ko request for partial embargo 20240201", "language": "en", "security": "internal", "license": 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"eprint_status": "archive", "userid": 12935, "dir": "disk0/00/01/62/89", "datestamp": "2024-02-12 18:05:29", "lastmod": "2024-02-20 17:39:22", "status_changed": "2024-02-12 18:05:29", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "dennislko@gmail.com", "id": "Ko-Dennis-Lok", "name": { "family": "Ko", "given": "Dennis Lok" }, "orcid": "0000-0001-8700-0844", "show_email": "YES" } ] }, "title": "Design and Implementation of a Microparticle Delivery Device for the Cornea", "ispublished": "unpub", "full_text_status": "public", "keywords": "ocular drug delivery; cornea; microparticles; biolistics; therapeutics; stroma; epithelium;", "abstract": "
Biolistic drug delivery offers an alternative path for delivering therapeutics into the cornea. Until now, none of the commercially available gene guns are suitable for clinical delivery of therapeutics due to tissue damage caused by high speed gas used to accelerate microparticles. Here, we demonstrated the use of a device that both eliminates the exit gas, only allowing high speed particles through, and one that works in a clinical setting.
\r\n\r\nMicroparticles ranging from 5 to 22 \u03bcm were accelerated and delivered into both the agarose gels and ex vivo corneas. In gels, we found that normalized penetration depth was proportional to particle diameter and density. As the standoff distance between the device and the target increased, more particles were left stranded at the surface, as their penetrating power decreased, and their dispersion from the center of mass on the target increased. The orifice size served to control both the number of particles and the amount of exit gas. Increasing the inlet pressure did not a show significant increase in the penetration depth of microparticles.
\r\n\r\nIn the cornea, we found that we were able to use our device to deliver particles into both the epithelium and the stroma, although only higher density particles were able to enter the stroma. There was little to no damage to the cornea due to particle delivery. If epithelial defects were detected in the cornea due to particle penetration, they were quickly resolved within 30 minutes. Our device demonstrated performance (penetration depth) comparable to previous biolistic delivery methods in the cornea, while also maintaining clinical relevance by eliminating exit gas flow.
", "date": "2024", "date_type": "degree", "id_number": "CaltechTHESIS:02072024-100209417", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:02072024-100209417", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "NSF Graduate Research Fellowship" }, { "agency": "Jacobs Institute for Molecular Engineering for Medicine" } ] }, "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Released redacted thesis 2024-02-20.\r\n\r\n// Full thesis embargo until 2024-08-09\r\n\r\n// Partial embargo requested 20240201.\r\n\r\n// Abstract currently partially redacted. Replace with full Abstract when full thesis is released / Kathy 20240207", "deposited_by": "Dennis Ko", "deposited_on": "2024-02-12 18:05:29", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "mikhail@caltech.edu", "id": "Shapiro-M-G", "name": { "family": "Shapiro", "given": "Mikhail G." }, "orcid": "0000-0002-0291-4215", "role": "chair" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "member" }, { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "orcid": "0000-0003-3175-4596", "role": "member" }, { "email": "mgharib@caltech.edu", "id": "Gharib-M", "name": { "family": "Gharib", "given": "Morteza" }, "orcid": "0000-0003-0754-4193", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2023-12-08", "gradofc_approval_date": "2024-02-09", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2024", "author_list": "Ko, Dennis Lok", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Shapiro, Mikhail G.; Kornfield, Julia A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/15161", "eprint_id": 15161, "rev_number": 63, "documents": [ { "id": "/id/document/138875", "doc_id": 138875, "rev_number": 4, "files": [ { "id": "/id/file/408674", "fileid": 408674, "datasetid": "document", "objectid": 138875, "filename": "Learsch thesis Latex.zip", "mime_type": "application/zip", "hash": "d11ca24eda99633f44d7793e1672e37d", "hash_type": "MD5", "filesize": 898694752, "mtime": "2023-05-27 03:36:45", "url": "/15161/4/Learsch thesis Latex.zip" } ], "eprint_id": 15161, "pos": 4, "placement": 5, "mime_type": "application/zip", "format": "application/zip", "format_desc": "Source files", "language": "en", "security": "internal", "license": "other", "main": "Learsch thesis Latex.zip", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "archival" }, { "id": "/id/document/138876", "doc_id": 138876, "rev_number": 7, "files": [ { "id": "/id/file/408677", "fileid": 408677, "datasetid": "document", "objectid": 138876, "filename": "20230526 Learsch thesis.pdf", "mime_type": "application/pdf", "hash": "c632054e50e3edc55bb8e49ea881cc12", "hash_type": "MD5", "filesize": 18007745, "mtime": "2023-05-27 03:38:28", "url": "/15161/5/20230526 Learsch thesis.pdf" } ], "eprint_id": 15161, "pos": 5, "placement": 4, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Full thesis", "language": "en", "security": "public", "license": "other", "main": "20230526 Learsch thesis.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final" }, { "id": "/id/document/138877", "doc_id": 138877, "rev_number": 1, "files": [ { "id": "/id/file/408681", "fileid": 408681, "datasetid": "document", "objectid": 138877, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "977acaac08850dbebc49065c2092fafb", "hash_type": "MD5", "filesize": 35429, "mtime": "2023-05-27 03:57:06", "url": "/15161/6/indexcodes.txt" } ], "eprint_id": 15161, "pos": 6, "placement": 6, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "validuser", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/138876" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/138876" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/138876" } ] } }, { "id": "/id/document/139051", "doc_id": 139051, "rev_number": 3, "files": [ { "id": "/id/file/409078", "fileid": 409078, "datasetid": "document", "objectid": 139051, "filename": "Robert Learsch campus only request 20230526.pdf", "mime_type": "application/pdf", "hash": "18d3e866a954a7593d4b14bf045ac634", "hash_type": "MD5", "filesize": 765500, "mtime": "2023-05-30 15:52:07", "url": "/15161/7/Robert Learsch campus only request 20230526.pdf" } ], "eprint_id": 15161, "pos": 7, "placement": 7, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Robert Learsch campus only request 20230526", "language": "en", "security": "internal", "license": "other", "main": "Robert Learsch campus only request 20230526.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "embargoform" }, { "id": "/id/document/139052", "doc_id": 139052, "rev_number": 1, "files": [ { "id": "/id/file/409091", "fileid": 409091, "datasetid": "document", "objectid": 139052, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "7485efe465211d915a4581fa0dfade3f", "hash_type": "MD5", "filesize": 1585, "mtime": "2023-05-30 16:02:09", "url": "/15161/8/indexcodes.txt" } ], "eprint_id": 15161, "pos": 8, "placement": 8, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "internal", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/139051" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/139051" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/139051" } ] } }, { "id": "/id/document/140661", "doc_id": 140661, "rev_number": 3, "files": [ { "id": "/id/file/421731", "fileid": 421731, "datasetid": "document", "objectid": 140661, "filename": "learsch-robert_release-permission.pdf", "mime_type": "application/pdf", "hash": "7cf9b1515c1e11cbdce97ac270ced351", "hash_type": "MD5", "filesize": 96637, "mtime": "2023-11-27 19:19:16", "url": "/15161/9/learsch-robert_release-permission.pdf" } ], "eprint_id": 15161, "pos": 9, "placement": 9, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Author approval 2023-11-22", "language": "en", "security": "internal", "license": "other", "main": "learsch-robert_release-permission.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "release" }, { "id": "/id/document/140662", "doc_id": 140662, "rev_number": 1, "files": [ { "id": "/id/file/421738", "fileid": 421738, "datasetid": "document", "objectid": 140662, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "8c38fb0761928fd3edb8ca3b92b2694a", "hash_type": "MD5", "filesize": 1246, "mtime": "2023-11-27 19:29:48", "url": "/15161/10/indexcodes.txt" } ], "eprint_id": 15161, "pos": 10, "placement": 10, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "internal", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/140661" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/140661" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/140661" } ] } } ], "eprint_status": "archive", "userid": 12109, "dir": "disk0/00/01/51/61", "datestamp": "2023-06-06 15:11:48", "lastmod": "2023-12-05 17:35:24", "status_changed": "2023-06-06 15:11:48", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "rlearsch.phd@gmail.com", "id": "Learsch-Robert-Whitson", "name": { "family": "Learsch", "given": "Robert Whitson" }, "orcid": "0000-0001-6329-5879", "show_email": "YES" } ] }, "title": "Droplet Control in Aqueous and Hydrocarbon Fluids: Long, End-Associative Polymers Dictate Fluid Behavior Under Elongational Flows", "ispublished": "unpub", "full_text_status": "public", "keywords": "Polymer Science, Rheology, Extensional Flow, Polymer Physics", "abstract": "Modifying elongational flows seen in sprayed mists, turbulent flows, and droplet spreading and retraction following impact, is of interest in diverse industries, including agriculture and aviation. Long flexible polymers (with fully extended lengths 1 to 10 \u00b5m) modify the elongational flow behavior of a fluid to which they are added. At low concentrations (1 to 10% of their overlap concentrations), their effect is mild under shear flow (shear viscosity increases < 50%), but dramatic under elongational flows (extensional viscosity increases \u2265 300).
\r\n\r\nThese long polymers are not widely used in practice because they degrade under strong flows, such as passing through pumps and filters, that typically precede spray. Pairwise end-associative polymers can overcome this limitation. Pulling apart non-covalent associative bonds under such strong flow conditions relieves the tension along the polymer backbone. The pairwise end-associative polymers that are effective in mist control and drag reduction are individually short enough to avoid chain scission in flows that would break long covalent polymers, yet long enough that 6 to 8 associative polymers connected end-to-end create supermolecules that are as effective as their long covalent counterparts.
\r\n\r\nThis thesis systematically compares the effect of long covalent and long end-associative polymers on the fluid\u2019s extensional flow properties and the polymers' performance in controlling droplet impact and spray breakup. To measure the elongational flow properties, I implemented and enhanced the Dripping onto Substrate Extensional Rheometry (DoSER) technique (Chapter 2) and applied it to long covalent polymers (Chapter 3) and to end-to-end associative polymers (Chapter 4). Preparing solutions in which the polymers negligibly affect the interfacial tension (< 10%) allows us to explore the relationship between extensional flow properties and droplet impact (Chapter 5) and spray (Chapter 6).
\r\n\r\nBy combining the quantitative measurements of extensional viscosity and extensional relaxation time with the corresponding behavior in impact and spray, I correlate the structure of polymers to the solution behavior in droplet rebound and spray breakup. This work has the potential to reduce pesticide contamination of soil, water, and air from agricultural sprays and fire hazard associated with hydrocarbon lubricants.
", "date": "2023", "date_type": "degree", "id_number": "CaltechTHESIS:05102023-041835603", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:05102023-041835603", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "Dow Chemical Company" }, { "agency": "NSF Graduate Research Fellowship" }, { "agency": "Army Research Office (ARO)" } ] }, "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "suggestions": "2023-12-05 released with author approval (see internal files).", "deposited_by": "Robert Learsch", "deposited_on": "2023-06-06 15:11:48", "doi": "10.7907/zkpd-bq33", "divisions": { "items": [ "div_eng" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "ktfaber@caltech.edu", "id": "Faber-K-T", "name": { "family": "Faber", "given": "Katherine T." }, "orcid": "0000-0001-6585-2536", "role": "chair" }, { "email": "stroian@caltech.edu", "id": "Troian-S-M", "name": { "family": "Troian", "given": "Sandra M." }, "orcid": "0000-0003-1224-6377", "role": "member" }, { "email": "CWNelson@dow.com", "id": "Nelson-Chris-W", "name": { "family": "Nelson", "given": "Chris W." }, "role": "member" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2022-10-22", "gradofc_approval_date": "2023-06-05", "review_status": "approved", "option_major": { "items": [ "matsci" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2023", "author_list": "Learsch, Robert Whitson", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Faber, Katherine T.; Troian, Sandra M.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/15216", "eprint_id": 15216, "rev_number": 31, "documents": [ { "id": "/id/document/138882", "doc_id": 138882, "rev_number": 4, "files": [ { "id": "/id/file/408708", "fileid": 408708, "datasetid": "document", "objectid": 138882, "filename": "2023-05-26_Xiong_Thesis.pdf", "mime_type": "application/pdf", "hash": "adf23d98784cdcd8db67f0cd5cc52ba7", "hash_type": "MD5", "filesize": 68354418, "mtime": "2023-05-27 16:34:37", "url": "/15216/1/2023-05-26_Xiong_Thesis.pdf" } ], "eprint_id": 15216, "pos": 1, "placement": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": "2023-05-26_Xiong_Thesis.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final" }, { "id": "/id/document/138883", "doc_id": 138883, "rev_number": 2, "files": [ { "id": "/id/file/408710", "fileid": 408710, "datasetid": "document", "objectid": 138883, "filename": "2023-05-26_Xiong_Thesis.zip", "mime_type": "application/zip", "hash": "4c22d0a57a148ed018bbbd8cdebb9a6d", "hash_type": "MD5", "filesize": 69583330, "mtime": "2023-05-27 16:36:57", "url": "/15216/2/2023-05-26_Xiong_Thesis.zip" } ], "eprint_id": 15216, "pos": 2, "placement": 2, "mime_type": "application/zip", "format": "application/zip", "format_desc": "source files", "language": "en", "security": "internal", "license": "other", "main": "2023-05-26_Xiong_Thesis.zip", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "archival" }, { "id": "/id/document/138884", "doc_id": 138884, "rev_number": 1, "files": [ { "id": "/id/file/408713", "fileid": 408713, "datasetid": "document", "objectid": 138884, "filename": "indexcodes.txt", "mime_type": "text/x-c", "hash": "5ec2bbe5da6db31f7d1b8e299ee57f0e", "hash_type": "MD5", "filesize": 23550, "mtime": "2023-05-27 16:44:40", "url": "/15216/3/indexcodes.txt" } ], "eprint_id": 15216, "pos": 3, "placement": 3, "mime_type": "text/x-c", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/138882" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/138882" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/138882" } ] } } ], "eprint_status": "archive", "userid": 11216, "dir": "disk0/00/01/52/16", "datestamp": "2023-06-01 15:37:35", "lastmod": "2023-11-08 00:39:39", "status_changed": "2023-06-01 15:37:35", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "lealia.xiong@gmail.com", "id": "Xiong-Lealia-Li", "name": { "family": "Xiong", "given": "Lealia Li" }, "orcid": "0000-0001-7636-5936", "show_email": "NO" } ] }, "title": "Expanding the Toolbox for Thermal Control of E. coli: Cold-Activated Transcription with Applications in Temperature Self-Regulation", "ispublished": "unpub", "full_text_status": "public", "keywords": "engineered living materials; microbial synthetic biology; thermal control; temperature self-regulation", "abstract": "Temperature can be used to control engineered E. coli \u2014 for example, the living component of an engineered living material (ELM) - through the use of thermolabile transcription factors. Sharp induction of gene expression with heat has been established using these bacteria- and phage-derived proteins. Here, we expand the toolbox for thermal control of E. coli through both direct cold-induced gene expression and through the construction of genetic circuits to invert heat-induced gene expression.
\r\n\r\nWe accomplish direct induction at low temperatures through the use of temperature-sensitive mutants of Lambda repressor as transcriptional activators. In addition, we show that a temperature-sensitive mutant of Lambda repressor can serve as an activator and a repressor of different genes simultaneously in one genetic circuit, leading to opposite thermal responses and serving as a temperature switch.
\r\n\r\nNext, we demonstrate inversion of a temperature-sensitive repressor using a temperature insensitive repressor. We apply this multicomponent switch to engineer a temperature self-regulation circuit for E. coli-based ELMs. Seasonal variation in ambient temperature presents a challenge in deploying ELMs outside of a laboratory environment, because E. coli growth rate is impaired both below and above 37\u00b0C. Our construct enables E. coli to produce a light-absorptive pigment in response to environmental temperature below 36\u00b0C with the goal of allowing the cells to absorb sunlight and locally warm to their optimal growth temperature. We demonstrate the efficacy of our pigment temperature switch in a model flat ELM growing at 32\u00b0C and 42\u00b0C in a home-built illuminated growth chamber. Below 36\u00b0C, our engineered E. coli increase in pigmentation, causing an increase in sample temperature and growth rate above non-pigmented bacteria. On the other hand, above 36\u00b0C, they decrease in pigmentation, protecting their growth compared to bacteria with temperature- independent high pigmentation. Integrating our temperature homeostasis circuit into an ELM has the potential to improve ELM performance by optimizing growth and protein production in the face of seasonal temperature changes.
", "date": "2023", "date_type": "degree", "id_number": "CaltechTHESIS:05272023-161541041", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:05272023-161541041", "related_url": { "items": [ { "description": "Article adapted for Ch. 2", "type": "doi", "url": "https://doi.org/10.1021/acssynbio.2c00093" }, { "description": "Article adapted for Ch. 4", "type": "doi", "url": "https://doi.org/10.1101/2023.03.11.532239" } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "Defense Advanced Research Projects Agency (DARPA)", "grant_number": "HR0011-17-2-0037" }, { "agency": "Institute for Collaborative Biotechnologies", "grant_number": "W911NF-09-0001" }, { "agency": "NSF Graduate Research Fellowship" }, { "agency": "Howard Hughes Medical Institute" }, { "agency": "Jacobs Institute for Molecular Engineering for Medicine" } ] }, "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Released 2023-06-08 after 1-week embargo.", "deposited_by": "Lealia Xiong", "deposited_on": "2023-06-01 15:37:35", "doi": "10.7907/5w59-0667", "divisions": { "items": [ "div_eng" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "mikhail@caltech.edu", "id": "Shapiro-M-G", "name": { "family": "Shapiro", "given": "Mikhail G." }, "orcid": "0000-0002-0291-4215", "role": "co-advisor" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "viviana@caltech.edu", "id": "Gradinaru-V", "name": { "family": "Gradinaru", "given": "Viviana" }, "orcid": "0000-0001-5868-348X", "role": "chair" }, { "email": "weigao@caltech.edu", "id": "Gao-Wei", "name": { "family": "Gao", "given": "Wei" }, "orcid": "0000-0002-8503-4562", "role": "member" }, { "email": "mikhail@caltech.edu", "id": "Shapiro-M-G", "name": { "family": "Shapiro", "given": "Mikhail G." }, "orcid": "0000-0002-0291-4215", "role": "member" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2022-12-13", "gradofc_approval_date": "2023-05-31", "review_status": "approved", "option_major": { "items": [ "medeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. 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"http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/137648" } ] } } ], "eprint_status": "archive", "userid": 11502, "dir": "disk0/00/01/50/07", "datestamp": "2022-08-26 19:02:16", "lastmod": "2023-11-08 00:30:09", "status_changed": "2022-08-26 19:02:16", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "khojin0206@gmail.com", "id": "Kim-Hojin", "name": { "family": "Kim", "given": "Hojin" }, "orcid": "0000-0002-0257-7300", "show_email": "NO" } ] }, "title": "New Long End-Associative Polymers for Mist Control in I. Aqueous Solutions and II. Hydrocarbon Solvents", "ispublished": "unpub", "full_text_status": "public", "keywords": "Long end associative polymer; water-soluble polymer; hydrocarbon-soluble polymer; polymer functionalization", "abstract": "Ultralong linear polymers are well known to be useful in a variety of applications such as mist control, drag reduction, and agricultural spray drift control. However, the application of ultralong linear polymers is limited by shear degradation of the ultralong polymer chains that occurs under strong flow conditions. To overcome the issue of shear degradation, our group previously designed long end-associative polymers that can self-assemble into megasupramolecules (Mw > 2000 kg/mol) in low polarity solvents like jet fuel. The previously developed long end associative polymers had polycyclooctadiene backbones (1,4 polybutadiene) with carboxylic acid or tertiary amine end groups that associated via hydrogen bonding. They were shear degradation resistant and used as mist-control agents that provided fire-protection to jet fuel at concentrations as low as 0.3wt%.
\r\n\r\nBuilding upon the previous work, this thesis describes efforts toward expanding the applicability of long end-associative polymers. We first describe the design and synthesis of water-soluble long end-associative polymers for agricultural spray mist-control. We synthesized telechelic polyacrylamides using reversible addition fragmentation chain transfer (RAFT) polymerization. We explored two types of associations that can form stable supramolecules in water: host-guest interactions between adamantane and beta-cyclodextrin (Chapter 1), and metal-ligand association between terpyridine and transition metal ions (Chapter 2). Careful optimization of polymerization conditions allowed the synthesis of ultra-high molecular weight telechelic polyacrylamides with narrow polydispersity. We found that the terpyridine functionalized polyacrylamides with Mw 820 kg/mol could assemble into megasupramolecules (Mw > 2000 kg/mol) upon addition of Fe(II) or Ni(II).
\r\n\r\nIn Chapters 3 and 4, we return to long end-associative polymers in hydrocarbon solvents. In Chapter 3, we tackle the issue of poor solubility of the previous generation of associative PCODs in a highly nonpolar solvent, PAO. In Chapter 4, we develop a new generation of end groups for improved solubility and ease of synthesis.
\r\n\r\nFinally in Chapter 5, we discuss polyDODT (poly(3,6-dioxa-1,8-octanedithiol)), a polydisulfide that tends to form a mixture of linear and cyclic species. We present new methods to detect the presence of linear species in the mixture, as well as an alternative synthesis route for synthesis of polyDODT.
", "date": "2023", "date_type": "degree", "id_number": "CaltechTHESIS:08252022-035254306", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:08252022-035254306", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "Dow Chemical Company" }, { "agency": "Army Research Office (ARO)" }, { "agency": "Department of Energy (DOE)" } ] }, "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Released 2022-09-02 after 1-week embargo.", "deposited_by": "Hojin Kim", "deposited_on": "2022-08-26 19:02:16", "doi": "10.7907/rsx9-qt39", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jfbrady@caltech.edu", "id": "Brady-J-F", "name": { "family": "Brady", "given": "John F." }, "orcid": "0000-0001-5817-9128", "role": "chair" }, { "email": "jak@caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "member" }, { "email": "zgw@caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "orcid": "0000-0002-3361-6114", "role": "member" }, { "email": "mrobb@caltech.edu", "id": "Robb-Maxwell-J", "name": { "family": "Robb", "given": "Maxwell J." }, "orcid": "0000-0002-0528-9857", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2022-08-10", "gradofc_approval_date": "2022-08-26", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. 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\u2013 are complex materials whose features span many length scales, ranging from bulk cohesive material properties, to mesoscale structural and compositional heterogeneity, down to the microscopic cellular morphology and cell-cell interaction chemistry.
\r\n\r\nHere, we demonstrate a tool to study the mechanical properties of biofilms across length scales from the mesoscale (0.2 mm) to the bulk (1 mm) using a simplified model system based on genetically engineered E. coli. Using a custom millifluidic device that suspends a 3 mm dia. biofilm across a support, we impose tunable hydrostatic pressure drops in the Pa-kPa range across the biofilm. The resulting deformation of the film through an aperture is visualized with optical coherence tomography and used to estimate bulk and mesoscale mechanical properties of the film. Our method requires only microliters of material, causes minimal disruption to the film structure, and allows for estimates of both average properties as well as local heterogeneity as a function of cell-cell interaction chemistry and biofilm damage and healing. In the final chapter we introduce other model biofilm systems for their unique optical and mechanical properties.
", "date": "2023", "date_type": "degree", "id_number": "CaltechTHESIS:08282022-230140735", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:08282022-230140735", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "DARPA", "grant_number": "HR0011-17-2-0037" }, { "agency": "Caltech Center for Environmental Microbial Interactions (CEMI)" } ] }, "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Released to public view 20231129. // Restricted to Caltech community only until 28 February 2023.", "deposited_by": "Priya Chittur", "deposited_on": "2022-08-30 23:17:18", "doi": "10.7907/e1yv-mr74", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "orcid": "0000-0003-3175-4596", "role": "chair" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "member" }, { "email": "ravi@caltech.edu", "id": "Ravichandran-G", "name": { "family": "Ravichandran", "given": "Guruswami" }, "orcid": "0000-0002-2912-0001", "role": "member" }, { "email": "mo@caltech.edu", "id": "Okumura-M", "name": { "family": "Okumura", "given": "Mitchio" }, "orcid": "0000-0001-6874-1137", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2022-08-17", "gradofc_approval_date": "2022-08-30", "review_status": "approved", "option_major": { "items": [ "chemistry" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2023", "author_list": "Chittur, Priya K.", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Tirrell, David A.; Kornfield, Julia A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/14523", "eprint_id": 14523, "rev_number": 119, "documents": [ { "id": "/id/document/136973", "doc_id": 136973, "rev_number": 4, "files": [ { "id": "/id/file/395383", "fileid": 395383, "datasetid": "document", "objectid": 136973, "filename": "ylitaloa_thesis.pdf", "mime_type": "application/pdf", "hash": "7a4f6c0d4082b93761c58d102b3f63ec", "hash_type": "MD5", "filesize": 30804754, "mtime": "2022-06-02 01:02:05", "url": "/14523/13/ylitaloa_thesis.pdf" } ], "eprint_id": 14523, "pos": 13, "placement": 13, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Final version of thesis", 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"title": "A Bubble Is Born: Nucleation and Early Growth of CO\u2082 Bubbles in Polymer Foams", "ispublished": "unpub", "full_text_status": "public", "keywords": "bubble nucleation carbon dioxide polymer foam microfluidics phase equilibrium high pressure polyurethane string method density functional theory PC-SAFT energy barrier flow instabilities bebop image processing diffusion", "abstract": "Gas bubble nucleation is a fundamental phenomenon both throughout the natural sciences and in the production of foams for lightweight, functional materials; it is also the basis for many a bubbly beverage. Enhancing bubble nucleation in polyurethane insulating foams used for refrigeration can further reduce their low thermal conductivity without resorting to hazardous blowing agents used in the past. Experimental challenges of measuring the kinetics of the rapid, multiscale process of bubble nucleation pose a roadblock to investigation of suitable processing conditions, as well as the development of theoretical models of bubbles and foams.
\r\n \r\nHere, using a microfluidic flow-focusing technique developed for measurement of protein and chemical kinetics, we built a microfluidic cell to probe gas bubble nucleation of CO\u2082 in polyol, a model system for polyurethane insulating foams, at controlled pressure with millisecond resolution over acquisition times sufficient for optical, IR, and X-ray measurements. This technique allows for repeated measurements of bubble nucleation at any degree of supersaturation without the interference of heterogeneous nucleation from surfaces. By extrapolating a model fit to high-speed optical microscopy measurements of bubble growth backward in time, we estimated the degree of supersaturation at nucleation for thousands of bubbles. Estimates of the nucleation rate based on Poisson statistics were consistent with predictions by a string method model based on density functional theory and G-ADSA measurements. This model predicted that the addition of cyclopentane (a common physical blowing agent in polyurethane foams) can dramatically reduce the nucleation energy barrier due to the formation of a liquid-like layer of cyclopentane and CO\u2082 along the surface of the bubble that reduces the interfacial tension, which previous models have only predicted at significantly higher saturation pressures. This prediction was supported by thermodynamic measurement of a three-phase coexistence under similar conditions, which is a known fingerprint for such nucleation pathways, and measurement of significantly higher bubble nucleation rates upon the addition of cyclopentane. These findings shed light on the possibility of a previously unappreciated role of physical blowing agents like cyclopentane in enhancing bubble nucleation by opening up a qualitatively distinct and more favorable nucleation pathway.
", "date": "2022", "date_type": "degree", "id_number": "CaltechTHESIS:03222022-221436705", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:03222022-221436705", "related_url": { "items": [ { "description": "Software repository for G-ADSA analysis described in Ch. 2", "type": "doi", "url": "https://doi.org/10.22002/D1.12621" } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "NSF Graduate Research Fellowship", "grant_number": "1745301" }, { "agency": "Dow Chemical" } ] }, "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "suggestions": "2022-06-09 released after 1-week embargo.", "deposited_by": "Andrew Ylitalo", "deposited_on": "2022-06-02 19:53:31", "doi": "10.7907/cdgw-7c18", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "advisor" }, { "email": "zgw@cheme.caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "orcid": "0000-0002-3361-6114", "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "jfb@cheme.caltech.edu", "id": "Brady-J-F", "name": { "family": "Brady", "given": "John F." }, "orcid": "0000-0001-5817-9128", "role": "chair" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "member" }, { "email": "mo@caltech.edu", "id": "Okumura-M", "name": { "family": "Okumura", "given": "Mitchio" }, "orcid": "0000-0001-6874-1137", "role": "member" }, { "email": "rustem@caltech.edu", "id": "Ismagilov-R-F", "name": { "family": "Ismagilov", "given": "Rustem F." }, "orcid": "0000-0002-3680-4399", "role": "member" }, { "email": "flagan@caltech.edu", "id": "Flagan-R-C", "name": { "family": "Flagan", "given": "Richard C." }, "orcid": "0000-0001-5690-770X", "role": "member" }, { "email": "zgw@cheme.caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "orcid": "0000-0002-3361-6114", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2022-05-20", "gradofc_approval_date": "2022-06-02", "thesis_awards": "Constantin G. Economou Memorial Prize, 2018.", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2022", "author_list": "Ylitalo, Andrew Samuel", "advisor_list": "Kornfield, Julia A. and Wang, Zhen-Gang", "comittee_list": "Brady, John F.; Kornfield, Julia A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/14457", "eprint_id": 14457, "rev_number": 52, "documents": [ { "id": "/id/document/135635", "doc_id": 135635, "rev_number": 6, "files": [ { "id": "/id/file/387707", "fileid": 387707, "datasetid": "document", "objectid": 135635, "filename": "Partitioned source material_record-14458.zip", "mime_type": "application/zip", "hash": "a5206027de37cd1e8982d3d8eb1437cb", "hash_type": "MD5", "filesize": 20179596, "mtime": "2021-12-22 18:43:50", "url": "/14457/7/Partitioned source material_record-14458.zip" } ], "eprint_id": 14457, "pos": 7, "placement": 2, "mime_type": "application/zip", "format": 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"/id/document/135637" } ] } } ], "eprint_status": "archive", "userid": 12702, "dir": "disk0/00/01/44/57", "datestamp": "2022-01-05 17:02:49", "lastmod": "2022-07-13 22:13:21", "status_changed": "2022-01-05 17:02:49", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "obateman1612@gmail.com", "id": "Bateman-Orland-Christopher-Lycurgue", "name": { "family": "Bateman", "given": "Orland Christopher Lycurgue" }, "orcid": "0000-0002-6985-494X", "show_email": "NO" } ] }, "title": "Design and Application of Novel Membrane Materials", "ispublished": "unpub", "full_text_status": "public", "keywords": "Mixed-matrix membranes; composite membranes; phase inversion micromoulding; protein chromatography; membranes; membrane charactization; ceramic membrane, PVDF crystal phase", "abstract": "Membrane technology is uniquely suited to meet the growing need for more sustainable processes due to membranes\u2019 tailorable selectivity and energy efficiency. Efforts to further improve membrane performance and modify them for new applications have found success in academic studies with a versatile class of membranes known as mixed-matrix membranes (MMM). Mixed-matrix membranes combine the strength and controlled morphology of semicrystalline polymeric membranes with superior functionality of a separate material dispersed in the polymer matrix. The strength and toughness of the resulting membranes depends on polymer morphology, including degree of crystallinity and pore structure. Control of the membrane morphology is achieved by kinetically trapping a partially phase separated state, for example, using Nonsolvent Induced Phase Separation (NIPS) to drive liquid-liquid and solid-liquid demixing. However, the processes used to control the polymer morphology are influenced by the functional particles and can result in novel morphologies. In Chapter 2, we used a promising strategy for stably incorporating functional polymeric particles in a structural polymer matrix to investigate the role of the particles during NIPS. The interplay of functional polymeric particle loading and nonsolvent induced phase separation are examined using x-ray diffraction (to deduce the crystal morph adopted by polyvinylidene difluoride, PVDF) and scanning electron microscopy (to observe membrane morphology and the size and distribution of functional particles). We found that the interaction between nonsolvent and functional particles enables a shift in crystal phase usually not attainable with our solvent.
\r\n\r\nIn addition to studying the fundamentals underlying MMM formation, we investigated two applications for novel membrane materials: purification of therapeutic antibodies and size-selective particle capture. Purification of proteins for medical use requires several chromatographic steps in order to produce solutions of sufficient purity. For many years, the gold standard in the field was resin-based packed bed chromatography; however, more recently membrane chromatography has gained prevalence due to its faster processing time, lower cost, and low operating pressure. With these advantages come the drawbacks of low binding capacity and a sensitivity to the concentration of salt ions in the solution. To address these two drawbacks, we investigated the chromatographic abilities of a modified MMM, in Chapter 3, and a novel membrane material comprising an MMM-ceramic composite, in Chapter 4. We discovered that the performance of the modified MMM is dependent on crosslinker chemistry and crosslink density. Upon optimization, the modified membrane demonstrated a binding capacity consistent with the upper range of available literature values as well as reduced sensitivity to salt. In addition, the development of the novel MMM-ceramic composite enables the use of a broader range of polymer matrix compositions for membrane chromatography.
\r\n\r\nCapture of pathogens from complex fluids, such as blood, has received substantial attention due to rising rates of sepsis and antibiotic resistance. \tIn Chapter 5, we pursued the capture of pathogens from model fluids using the size-based separation capabilities of dendritic ceramic membranes. We found that interactions between the ceramic surface and the suspended particles played a significant role in membrane performance.
", "date": "2022", "date_type": "degree", "id_number": "CaltechTHESIS:12222021-065913893", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:12222021-065913893", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "suggestions": "Released after 1-week embargo expired 2022-01-12.", "deposited_by": "Orland Bateman", "deposited_on": "2022-01-05 17:02:49", "doi": "10.7907/9w23-ax66", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "advisor" }, { "email": "diallo@caltech.edu", "id": "Diallo-Mamadou-S", "name": { "family": "Diallo", "given": "Mamadou S." }, "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "ktfaber@caltech.edu", "id": "Faber-K-T", "name": { "family": "Faber", "given": "Katherine T." }, "orcid": "0000-0001-6585-2536", "role": "chair" }, { "email": "jfb@cheme.caltech.edu", "id": "Brady-J-F", "name": { "family": "Brady", "given": "John F." }, "orcid": "0000-0001-5817-9128", "role": "member" }, { "email": "zgw@caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "orcid": "0000-0002-3361-6114", "role": "member" }, { "email": "diallo@caltech.edu", "id": "Diallo-Mamadou-S", "name": { "family": "Diallo", "given": "Mamadou S." }, "role": "member" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2021-09-08", "gradofc_approval_date": "2022-01-04", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2022", "author_list": "Bateman, Orland Christopher Lycurgue", "advisor_list": "Kornfield, Julia A. and Diallo, Mamadou S.", "comittee_list": "Faber, Katherine T.; Brady, John F.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/14630", "eprint_id": 14630, "rev_number": 62, "documents": [ { "id": "/id/document/136688", "doc_id": 136688, "rev_number": 6, "files": [ { "id": "/id/file/393329", "fileid": 393329, "datasetid": "document", "objectid": 136688, "filename": "20220526_LhotaR_thesis.pdf", "mime_type": "application/pdf", "hash": "6eecd0d345983d72ab9f752b2e86d8df", "hash_type": "MD5", "filesize": 6574294, "mtime": "2022-05-26 23:39:09", "url": "/14630/1/20220526_LhotaR_thesis.pdf" } ], "eprint_id": 14630, "pos": 1, "placement": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Lhota, Red C. Complete Thesis", "language": "en", "security": "public", "license": "other", "main": "20220526_LhotaR_thesis.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final" }, { "id": "/id/document/136689", "doc_id": 136689, "rev_number": 5, "files": [ { "id": "/id/file/393333", "fileid": 393333, "datasetid": "document", "objectid": 136689, "filename": "20220526_LhotaR_thesis_chapter_1.pdf", "mime_type": "application/pdf", "hash": "7f7226fe4a7578998f4560f3b0cf8be8", "hash_type": "MD5", "filesize": 1033744, "mtime": "2022-05-26 23:40:27", "url": "/14630/2/20220526_LhotaR_thesis_chapter_1.pdf" } ], "eprint_id": 14630, "pos": 2, "placement": 2, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Chapter 1: Controlling Fluid Properties through Polymer Additives", "language": "en", "security": "public", "license": "other", "main": "20220526_LhotaR_thesis_chapter_1.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final" }, { "id": "/id/document/136690", "doc_id": 136690, "rev_number": 6, "files": [ { "id": "/id/file/393335", "fileid": 393335, "datasetid": "document", "objectid": 136690, "filename": "20220526_LhotaR_thesis_chapter_2.pdf", "mime_type": "application/pdf", "hash": "bc0fb54398b067f1bb2c6fd7c08babf2", "hash_type": "MD5", "filesize": 815599, "mtime": "2022-05-26 23:41:23", "url": "/14630/3/20220526_LhotaR_thesis_chapter_2.pdf" } ], "eprint_id": 14630, "pos": 3, "placement": 3, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Chapter 2: Characterizing Chain Scission in Aqueous Polymer Solutions", "language": "en", "security": "public", "license": "other", "main": "20220526_LhotaR_thesis_chapter_2.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final" }, { "id": "/id/document/136691", "doc_id": 136691, "rev_number": 5, "files": [ { "id": "/id/file/393337", "fileid": 393337, "datasetid": "document", "objectid": 136691, "filename": "20220526_LhotaR_thesis_chapter_3.pdf", "mime_type": "application/pdf", "hash": "1190274f46bce7967fcdd9ffee8c5856", "hash_type": "MD5", "filesize": 1129964, "mtime": "2022-05-26 23:42:10", "url": "/14630/4/20220526_LhotaR_thesis_chapter_3.pdf" } ], "eprint_id": 14630, "pos": 4, "placement": 4, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Chapter 3: Measurements of Drag Reduction and Extensional Rheology of Degrading Polymer Solutions", "language": "en", "security": "public", "license": "other", "main": "20220526_LhotaR_thesis_chapter_3.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final" }, { "id": "/id/document/136692", "doc_id": 136692, "rev_number": 5, "files": [ { "id": "/id/file/393340", "fileid": 393340, "datasetid": "document", "objectid": 136692, "filename": "20220526_LhotaR_thesis_chapter_4.pdf", "mime_type": "application/pdf", "hash": "3a21ad5620abc61d7e81b655736923fa", "hash_type": "MD5", "filesize": 2673949, "mtime": "2022-05-26 23:42:14", "url": "/14630/5/20220526_LhotaR_thesis_chapter_4.pdf" } ], "eprint_id": 14630, "pos": 5, "placement": 5, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Chapter 4: Effects of Solvent Quality and Viscosity on the Behavior of End-Associative Polymers", "language": "en", "security": "public", "license": "other", "main": "20220526_LhotaR_thesis_chapter_4.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final" }, { "id": "/id/document/136693", "doc_id": 136693, "rev_number": 5, "files": [ { "id": "/id/file/393342", "fileid": 393342, "datasetid": "document", "objectid": 136693, "filename": "20220526_LhotaR_thesis_chapter_5.pdf", "mime_type": "application/pdf", "hash": "3da8fdc1a8d67eddbfd4fbf555fd21ce", "hash_type": "MD5", "filesize": 1043965, "mtime": "2022-05-26 23:42:18", "url": "/14630/6/20220526_LhotaR_thesis_chapter_5.pdf" } ], "eprint_id": 14630, "pos": 6, "placement": 6, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Chapter 5: End-Functionality Detection through Shear Rheology", "language": "en", "security": "public", "license": "other", "main": "20220526_LhotaR_thesis_chapter_5.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final" }, { "id": "/id/document/136694", "doc_id": 136694, "rev_number": 5, "files": [ { "id": "/id/file/393344", "fileid": 393344, "datasetid": "document", "objectid": 136694, "filename": "20220526_LhotaR_thesis_chapter_6.pdf", "mime_type": "application/pdf", "hash": "873fefffddf4b407448e60c114a60d76", "hash_type": "MD5", "filesize": 1010463, "mtime": "2022-05-26 23:42:22", "url": "/14630/7/20220526_LhotaR_thesis_chapter_6.pdf" } ], "eprint_id": 14630, "pos": 7, "placement": 7, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Chapter 6: Incorporating Evidence-Based Teaching Techniques into Caltech Classrooms", "language": "en", "security": "public", "license": "other", "main": "20220526_LhotaR_thesis_chapter_6.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final" }, { "id": "/id/document/136695", "doc_id": 136695, "rev_number": 5, "files": [ { "id": "/id/file/393346", "fileid": 393346, "datasetid": "document", "objectid": 136695, "filename": "20220526_LhotaR_thesis_appendix_A.pdf", "mime_type": "application/pdf", "hash": "3cee0354818d934ba23b89b94927e1d4", "hash_type": "MD5", "filesize": 535146, "mtime": "2022-05-26 23:42:25", "url": "/14630/8/20220526_LhotaR_thesis_appendix_A.pdf" } ], "eprint_id": 14630, "pos": 8, "placement": 8, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Appendix A: Automating Analysis of Dripping-Onto-Substrate Extensional Rheometry", "language": "en", "security": "public", "license": "other", "main": "20220526_LhotaR_thesis_appendix_A.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final" }, { "id": "/id/document/136696", "doc_id": 136696, "rev_number": 5, "files": [ { "id": "/id/file/393348", "fileid": 393348, "datasetid": "document", "objectid": 136696, "filename": "20220526_LhotaR_thesis_appendix_B_and_C.pdf", "mime_type": "application/pdf", "hash": "34d3e323cc128628e6ce507b642e330c", "hash_type": "MD5", "filesize": 477576, "mtime": "2022-05-26 23:42:27", "url": "/14630/9/20220526_LhotaR_thesis_appendix_B_and_C.pdf" } ], "eprint_id": 14630, "pos": 9, "placement": 9, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Appendix B and Appendix C", "language": "en", 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"language": "en", "security": "internal", "license": "other", "main": "lhota-red_release-permission.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "release" } ], "eprint_status": "archive", "userid": 10922, "dir": "disk0/00/01/46/30", "datestamp": "2022-05-27 23:25:47", "lastmod": "2023-11-08 00:30:09", "status_changed": "2022-05-27 23:25:47", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "rlhota13@gmail.com", "id": "Lhota-Red-C", "name": { "family": "Lhota", "given": "Red C." }, "orcid": "0000-0002-8481-3716", "show_email": "NO" } ] }, "title": "Rheological Characterization of Polymer Additives for Mist Control and Drag Reduction", "ispublished": "unpub", "full_text_status": "public", "keywords": "rheology, polymers, mist control, drag reduction, megasupramolecules", "abstract": "Long flexible polymers in solution at low concentrations strongly change the extensional properties of fluids due to chain stretching that resists flow, while their compact conformation in shear has weak effects. This dramatic difference between their effects on extension and shear is desirable in a variety of applications--controlling drop size in sprayed mists, reducing drag in turbulent flow, and preventing rebound in drop impact. Traditional long covalent polymers, however, are not practical in many applications because they undergo mechanical degradation, i.e. chain scission, under strong flow conditions. Megasupramolecular polymer systems, consisting of long end-associative telechelic polymers that assemble in solutions into multi-million molecular weight supramolecules, meet this practical need. Through association, they act like traditional covalently-bonded polymers in extension, while reversibly dissociating under the strong flows that cause scission for those long polymers.
\r\nThis thesis examines the interplay of flow and degradation that imposes an upper-bound on useful lengths of invididual end-associative chains (how long is too long) (Chapters 2 and 3); the quiescent coil size that affects the onset of stretching in fluids of interest (water and polyalphaolefin lubricant) (Chapters 2 and 4);\r\nrheological approachs to detect variations in the degree of end-functionalization that affect formation of ultra-long supramolecules (Chapter 5); and the changes to turbulent flow when long polymers are present at low concentration (Chapter 2). Ultimately, the audience who might enjoy this thesis is limited by barriers of rheological jargon. In the pursuit of broader rheological and overall scientific understanding, I describe evidence-based pedagogical techniques and my approach to implementing them in chemical engineering and polymer physics classrooms (Chapter 6).
", "date": "2022", "date_type": "degree", "id_number": "CaltechTHESIS:05262022-231652129", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:05262022-231652129", "projects": { "items": [ "Dow Mist UPI" ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "Dow Chemical Company" }, { "agency": "Army Research Office (ARO)" }, { "agency": "NSF Graduate Research Fellowship" } ] }, "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "suggestions": "Released 2022-11-28 with author approval.\r\n\r\n// 1-week embargo expires 2022-06-03; restriction to campus for full thesis and chapter 2 expires 2022-11-28; all other files can be released publicly after 1-week embargo\r\n\r\n// Mixed access / restriction to campus until 2022-11-28 // From author: Chapter 2 of my thesis is a UPI project with Dow Chemical Company and we are required to submit all publishedmaterials for review with them prior to publication. I submitted a version of my chapter to them April 16th and have notyet heard back if the chapter is approved for public release.", "deposited_by": "Red Lhota", "deposited_on": "2022-05-27 23:25:47", "doi": "10.7907/wav1-4t47", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia" }, "orcid": "0000-0001-6746-8634", "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jfbrady@caltech.edu", "id": "Brady-J-F", "name": { "family": "Brady", "given": "John F." }, "orcid": "0000-0001-5817-9128", "role": "chair" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "member" }, { "email": "zgw@caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "orcid": "0000-0002-3361-6114", "role": "member" }, { "email": "mckeon@caltech.edu", "id": "McKeon-B-J", "name": { "family": "McKeon", "given": "Beverley J." }, "orcid": "0000-0003-4220-1583", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2022-05-16", "gradofc_approval_date": "2022-05-27", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2022", "author_list": "Lhota, Red C.", "advisor_list": "Kornfield, Julia", "comittee_list": "Brady, John F.; Kornfield, Julia A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/13980", "eprint_id": 13980, "rev_number": 44, "documents": [ { "id": "/id/document/112581", "doc_id": 112581, "rev_number": 3, "files": [ { "id": "/id/file/342797", "fileid": 342797, "datasetid": "document", "objectid": 112581, "filename": "20201026_benlaccettithesiscompleted.docx.zip", "mime_type": "application/zip", "hash": "73f0846761eb4a7887479c1aaaea2c64", "hash_type": "MD5", "filesize": 158733465, "mtime": "2020-10-26 18:51:05", "url": "/13980/1/20201026_benlaccettithesiscompleted.docx.zip" } ], "eprint_id": 13980, "pos": 1, "placement": 1, "mime_type": "application/zip", "format": "application/msword", "format_desc": "Word version of thesis", "language": "en", "security": "internal", "license": "other", "main": "20201026_benlaccettithesiscompleted.docx.zip", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "updated" }, { "id": "/id/document/112582", "doc_id": 112582, "rev_number": 6, "files": [ { "id": "/id/file/342799", "fileid": 342799, "datasetid": "document", "objectid": 112582, "filename": "20201026_benlaccettithesiscompleted.pdf", "mime_type": "application/pdf", "hash": "3f4ad7729d71a7dabf29314fa9b594a3", "hash_type": "MD5", "filesize": 72197654, "mtime": "2020-10-26 19:24:32", "url": "/13980/2/20201026_benlaccettithesiscompleted.pdf" } ], "eprint_id": 13980, "pos": 2, "placement": 2, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": "20201026_benlaccettithesiscompleted.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final" }, { "id": "/id/document/112590", "doc_id": 112590, "rev_number": 3, "files": [ { "id": "/id/file/342831", "fileid": 342831, "datasetid": "document", "objectid": 112590, "filename": "10262020 - third party content licences.docx", "mime_type": "application/vnd.openxmlformats-officedocument.wordprocessingml.document", "hash": "35c5e0a3176f821abb189a72218d262d", "hash_type": "MD5", "filesize": 39121, "mtime": "2020-10-28 16:44:40", "url": "/13980/3/10262020 - third party content licences.docx" } ], "eprint_id": 13980, "pos": 3, "placement": 3, "mime_type": "application/vnd.openxmlformats-officedocument.wordprocessingml.document", "format": "application/msword", "language": "en", "security": "internal", "license": "other", "main": "10262020 - third party content licences.docx", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "copyright" }, { "id": "/id/document/131358", "doc_id": 131358, "rev_number": 1, "files": [ { "id": "/id/file/376797", "fileid": 376797, "datasetid": "document", "objectid": 131358, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "fca6292781a8c4910b9ab1a2f0b2feb5", "hash_type": "MD5", "filesize": 33688, "mtime": "2021-06-24 17:49:20", "url": "/13980/4/indexcodes.txt" } ], "eprint_id": 13980, "pos": 4, "placement": 4, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/112582" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/112582" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/112582" } ] } }, { "id": "/id/document/131359", "doc_id": 131359, "rev_number": 1, "files": [ { "id": "/id/file/376798", "fileid": 376798, "datasetid": "document", "objectid": 131359, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "1a2d93606751fa7147db8e68d7561668", "hash_type": "MD5", "filesize": 6715, "mtime": "2021-06-24 17:49:20", "url": "/13980/5/indexcodes.txt" } ], "eprint_id": 13980, "pos": 5, "placement": 5, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/msword to indexcodes", "language": "en", "security": "internal", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/112590" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/112590" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/112590" } ] } } ], "eprint_status": "archive", "userid": 11016, "dir": "disk0/00/01/39/80", "datestamp": "2020-11-04 00:50:12", "lastmod": "2021-11-01 23:27:26", "status_changed": "2020-11-04 00:50:12", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "blaccetti@gmail.com", "id": "Laccetti-Benjamin-Joseph", "name": { "family": "Laccetti", "given": "Benjamin Joseph" }, "orcid": "0000-0002-0399-1204", "show_email": "YES" } ] }, "title": "Therapeutic Microparticles and Biolistic Drug-Delivery to the Cornea", "ispublished": "unpub", "full_text_status": "public", "keywords": "Drug-delivery, cornea, biolistics", "abstract": "The ability to deliver therapeutic compounds to the cornea using high-velocity microparticles is assessed and a method to synthesize therapeutic particles suitable for the cornea is demonstrated. Using a commercial gene gun (BioRad; PDS1000), a pneumatic capillary gun, and custom biolistic technology, microparticles were accelerated and made to embed in target materials: either homogeneous gels or corneal tissue. In homogeneous gels, penetration was shown to be directly proportional to particle size and density. In contrast, penetration of microparticles into the cornea is insensitive to particle size and density: varying the sectional density by 680% failed to penetrate beyond the epithelium (ca. 50 microns). The corneal epithelium exhibits two distinct kinetic energy thresholds that must be exceeded to first embed particles in the epithelium (rather than stopping on its anterior surface) and second to embed particles in the stroma (rather than stopping at the posterior surface of the epithelium). Penetration profiles show that the stroma is a highly effective stopping medium for high velocity microparticles. Despite the high water content of corneal tissue (76 w%) compared to the stratum corneum of skin (40 w%), the resistance to penetration of the cornea is comparable to literature values for skin. Ideal particles for drug delivery to the cornea would dissolve away completely, leaving no residue that might scatter light. With a vibrating orifice aerosol generator and a temperature-controlled column, 30-50 \u00b5m particles were composed of 1% Eosin Y with poly(ethylene glycol). Using low density polymer particles with a therapeutic agent payload, it was demonstrated that bulk material can be ballistically delivered to the central 1 cm\u00b2 of the corneal epithelium rapidly, in an even, quantifiable layer.", "date": "2021", "date_type": "degree", "id_number": "CaltechTHESIS:10182020-133113205", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:10182020-133113205", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "deposited_by": "Benjamin Laccetti", "deposited_on": "2020-11-04 00:50:12", "doi": "10.7907/nf29-gy82", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "flagan@caltech.edu", "id": "Flagan-R-C", "name": { "family": "Flagan", "given": "Richard C." }, "orcid": "0000-0001-5690-770X", "role": "chair" }, { "email": "jak@caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "member" }, { "email": "ravi@caltech.edu", "id": "Ravichandran-G", "name": { "family": "Ravichandran", "given": "Guruswami" }, "orcid": "0000-0002-2912-0001", "role": "member" }, { "email": "weigao@caltech.edu", "id": "Gao-Wei", "name": { "family": "Gao", "given": "Wei" }, "orcid": "0000-0002-8503-4562", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2020-06-26", "gradofc_approval_date": "2020-11-03", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2021", "author_list": "Laccetti, Benjamin Joseph", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Flagan, Richard C.; Kornfield, Julia A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/14123", "eprint_id": 14123, "rev_number": 27, "documents": [ { "id": "/id/document/114656", "doc_id": 114656, "rev_number": 3, "files": [ { "id": "/id/file/354680", "fileid": 354680, "datasetid": "document", "objectid": 114656, "filename": "Ford_Rachel_R_thesis.docx", "mime_type": "application/vnd.openxmlformats-officedocument.wordprocessingml.document", "hash": "8751979b170ebaa0f8c75f5cc28f77b4", "hash_type": "MD5", "filesize": 23955645, "mtime": "2021-04-19 20:46:58", "url": "/14123/1/Ford_Rachel_R_thesis.docx" } ], "eprint_id": 14123, "pos": 1, "placement": 1, "mime_type": "application/vnd.openxmlformats-officedocument.wordprocessingml.document", "format": "application/msword", "format_desc": "Source document", "language": "en", "security": "internal", "license": "other", "main": "Ford_Rachel_R_thesis.docx", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "archival" }, { "id": "/id/document/114657", "doc_id": 114657, "rev_number": 5, "files": [ { "id": "/id/file/354682", "fileid": 354682, "datasetid": "document", "objectid": 114657, "filename": "Ford_Rachel_R_thesis.pdf", "mime_type": "application/pdf", "hash": "342422b08a24dcb9c70cb2f0721b83b2", "hash_type": "MD5", "filesize": 3697813, "mtime": "2021-04-19 20:47:11", "url": "/14123/2/Ford_Rachel_R_thesis.pdf" } ], "eprint_id": 14123, "pos": 2, "placement": 2, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": "Ford_Rachel_R_thesis.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final" }, { "id": "/id/document/131548", "doc_id": 131548, "rev_number": 1, "files": [ { "id": "/id/file/376987", "fileid": 376987, "datasetid": "document", "objectid": 131548, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "9f93622f478009d1f0ce48290434661e", "hash_type": "MD5", "filesize": 24161, "mtime": "2021-06-24 18:01:57", "url": "/14123/3/indexcodes.txt" } ], "eprint_id": 14123, "pos": 3, "placement": 3, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/114657" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/114657" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/114657" } ] } }, { "id": "/id/document/131549", "doc_id": 131549, "rev_number": 1, "files": [ { "id": "/id/file/376988", "fileid": 376988, "datasetid": "document", "objectid": 131549, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "3a74c2b7a9a3d00a6158c6e6a2438ba3", "hash_type": "MD5", "filesize": 34863, "mtime": "2021-06-24 18:01:58", "url": "/14123/4/indexcodes.txt" } ], "eprint_id": 14123, "pos": 4, "placement": 4, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/msword to indexcodes", "language": "en", "security": "internal", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/114656" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/114656" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/114656" } ] } } ], "eprint_status": "archive", "userid": 12552, "dir": "disk0/00/01/41/23", "datestamp": "2021-04-20 22:34:00", "lastmod": "2021-11-01 23:18:59", "status_changed": "2021-04-20 22:34:00", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "rrford34@gmail.com", "id": "Ford-Rachel-Rae", "name": { "family": "Ford", "given": "Rachel Rae" }, "orcid": "0000-0001-9844-1557", "show_email": "NO" } ] }, "title": "Controlling the Dynamics of Microstructure Formation in Mixed-Matrix Polymeric-Particle Membranes", "ispublished": "unpub", "full_text_status": "public", "keywords": "polymer membranes; mixed-matrix membranes; microstructure formation; microgel synthesis; polymerization-induced phase separation; ultra-small-angle neutron scattering; small-angle neutron scattering", "abstract": "Polymer membranes are increasingly important in energy generation, water purification, and resource recovery. Control over chemistry, morphology, and mechanical properties gives organic polymers unparalleled advantages for membrane technology\u2014but only if these complementary functions can be married into a cohesive material. Herein I have sought to expand upon the chemical tools for integrating diverse polymers into multifunctional membrane materials, making them easily tunable to various applications. To overcome a fundamental challenge in polymer science\u2014namely, that polymers with different functions often do not mix\u2014the functional polymer is grown in situ in a solution containing a preformed scaffold polymer, a method pioneered by co-advisor Mamadou Diallo. The hierarchical structure of the resulting mixed matrix polymeric-particle (M2P2) membrane is governed by the kinetic competition between polymerization and phase separation of the functional polymer from the scaffold polymer. This competition is quenched by immersion in a nonsolvent, which rapidly solidifies the material to trap the metastable structure formed during synthesis.
\r\n\r\nIn my quest to understand how these competing processes interact to inform multifunctional membrane design, I developed a general method for studying transient structure using ultra-small angle neutron scattering (Chapter II), working closely with Kornfield Group alumnus Dr. Joey Kim. I then investigated the synergistic effects of incorporating different functional polymer architectures in M2P2 membranes (Chapter III), working with fellow graduate student Orland Bateman. By combining low-generation dendrimers with randomly hyperbranched oligomers bearing similar chemical functionality, we can systematically tune the characteristic length of domains formed during synthesis. In the final chapter I discuss the main conclusions and describe future directions for understanding structure during processing in M2P2 membranes. My thesis ultimately provides a broadly relevant platform for membrane design and synthesis, one in which the favorable properties of different polymers may be combined to strike a balance between function, stability, and ease of fabrication.
", "date": "2021", "date_type": "degree", "id_number": "CaltechTHESIS:04192021-200916929", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:04192021-200916929", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "Resnick Sustainability Institute Graduate Research Fellowship" } ] }, "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Rachel Ford", "deposited_on": "2021-04-20 22:34:00", "doi": "10.7907/fqgq-vd04", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "advisor" }, { "email": "mdiallo@nsf.gov", "id": "Diallo-Mamadou-S", "name": { "family": "Diallo", "given": "Mamadou S." }, "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "wag@wag.caltech.edu", "id": "Goddard-W-A-III", "name": { "family": "Goddard", "given": "William A., III" }, "orcid": "0000-0003-0097-5716", "role": "chair" }, { "email": "rhg@caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "orcid": "0000-0002-0057-7817", "role": "member" }, { "email": "lwei@caltech.edu", "id": "Wei-Lu", "name": { "family": "Wei", "given": "Lu" }, "role": "member" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "member" }, { "email": "mdiallo@nsf.gov", "id": "Diallo-Mamadou-S", "name": { "family": "Diallo", "given": "Mamadou S." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2020-09-11", "gradofc_approval_date": "2021-04-20", "review_status": "approved", "option_major": { "items": [ "chemistry" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2021", "author_list": "Ford, Rachel Rae", "advisor_list": "Kornfield, Julia A. and Diallo, Mamadou S.", "comittee_list": "Goddard, William A., III; Grubbs, Robert H.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/14186", "eprint_id": 14186, "rev_number": 38, "documents": [ { "id": "/id/document/119105", "doc_id": 119105, "rev_number": 5, "files": [ { "id": "/id/file/361505", "fileid": 361505, "datasetid": "document", "objectid": 119105, "filename": "zhou-dan_restriction-request.pdf", "mime_type": "application/pdf", "hash": "0ee0642ffca3046445ea535289464df2", "hash_type": "MD5", "filesize": 88611, "mtime": "2021-05-28 15:54:49", "url": "/14186/2/zhou-dan_restriction-request.pdf" } ], "eprint_id": 14186, "pos": 2, "placement": 2, "mime_type": "application/pdf", "format": "application/pdf", 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diabetic retinopathy (DR) are the leading causes of blindness in the developed world and on the rise globally due to the growth of an aging population and an increasing number of diabetics. Antibodies of vascular endothelial growth factor (VEGF), which target neovascularization in the advanced stages of both diseases, have been the main treatment for the past decade. However, anti-VEGF therapies suffer from short half-life and high cost inherent to antibodies, limiting the medical availability to a broader population.
\r\n\r\nTo fill the unmet medical need for treating retinal diseases, a novel therapeutic oligopeptide, risuteganib, is currently in Phase II clinical trials. Results from completed trials suggest that risuteganib has comparable drug efficacy to anti-VEGF therapies, long half-life, low cost, and absence of drug-related adverse events in several hundred patients enrolled in clinical trials for diabetic macular edema (DME) and dry AMD. Risuteganib was originally designed to target neovascularization, intending to inhibit integrin cell-surface receptors and thereby block adhesion and migration of abnormal blood vessel cells. Early in our study, we found experimental evidence contrary to this mechanism of action (MOA).
\r\n\r\nOur journey began with an unbiased search for the binding loci in retinal tissue, using peptide-directed fluorescent labeling. We found out that risuteganib specifically binds to a monolayer of cells, the retinal pigment epithelium (RPE), which has essential functions in maintaining the homeostasis of the retina, and its dysfunction is the hallmark for both blinding retinal diseases. In vitro study in an RPE cell model, ARPE19, showed that risuteganib protects cells against elevated oxidative stress that is associated with AMD and DR. This protective effect correlates with maintaining mitochondrial function. Further study of mitochondrial bioenergetics, in collaboration with Dr. Cris Kenney at UCI, revealed that risuteganib supports oxidative phosphorylation metabolism in the mitochondria.
\r\n\r\nBased on the chemical similarity of risuteganib with a natural product, we hypothesized that risuteganib may act through a mitochondrial enzyme, pyruvate dehydrogenase kinase (PDK), specifically PDK1 that is responsive to disease-related hypoxia-inducible factor 1 alpha (HIF-1\u03b1). Protein phosphorylation assay and enzymatic assay confirmed that risuteganib inhibits PDK1, as a result, reducing phosphorylation of an essential enzyme, pyruvate dehydrogenase (PDH). Leaving PDH in its unphosphorylated form allows its continued activity in oxidative phosphorylation metabolism, which offers a molecular explanation of the ability to support mitochondrial activity. This leads to our current hypothesis that risuteganib\u2019s mechanism of action (MOA) is through inhibition of PDK and protection of mitochondrial functions in RPE cells for treating retinal diseases.
\r\n\r\nProtecting mitochondrial functions may be beneficial to other cell types and in other diseases that subject cells to oxidative stress. As the mitochondria targeting is a potential therapy for diverse life-threatening diseases, including inflammatory disease, cardiovascular disease, and cancer, the present hypothesis invites us to expand our scope of view for this study to broader applications.
", "date": "2021", "date_type": "degree", "id_number": "CaltechTHESIS:05282021-020006678", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:05282021-020006678", "related_url": { "items": [ { "description": "ARVO annual meeting abstract related for Ch. 2 and 3", "type": "related", "url": "https://iovs.arvojournals.org/article.aspx?articleid=2768773" } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "Allegro Ophthalmics" }, { "agency": "Caltech" }, { "agency": "Schlumberger Foundation" } ] }, "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "suggestions": "Released to public view 25 Jan 2023. Resounding silence from advisor and student when asked about need for extensions. Kathy. // \r\n\r\n//Restricted to Caltech community only until 8 August 2022. Extension approved 8Feb2022.//\r\n\r\n// Restricted to Caltech community only until 3 January 2022. Extended another month to allow extension request for scooping to be handled. Kornfield has contacted Kaushik. Kathy 07Dec2021 // From author: The thesis work includes unpublished data and information. We are preparing manuscripts.", "deposited_by": "Dan Zhou", "deposited_on": "2021-06-03 15:40:48", "doi": "10.7907/9kqf-yr35", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "mikhail@caltech.edu", "id": "Shapiro-M-G", "name": { "family": "Shapiro", "given": "Mikhail G." }, "orcid": "0000-0002-0291-4215", "role": "chair" }, { "email": "clemons@caltech.edu", "id": "Clemons-W-M", "name": { "family": "Clemons", "given": "William M." }, "orcid": "0000-0002-0021-889X", "role": "member" }, { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "orcid": "0000-0003-3175-4596", "role": "member" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2021-05-14", "gradofc_approval_date": "2021-06-03", "review_status": "approved", "option_major": { "items": [ "chemistry" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. 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"language": "en", "security": "internal", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/104760" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/104760" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/104760" } ] } } ], "eprint_status": "archive", "userid": 11714, "dir": "disk0/00/01/15/70", "datestamp": "2019-06-10 22:47:03", "lastmod": "2019-12-12 21:37:30", "status_changed": "2019-06-10 22:47:03", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "zach.shao@gmail.com", "id": "Shao-Zixuan", "name": { "family": "Shao", "given": "Zixuan" }, "orcid": "0000-0002-4676-6023", "show_email": "YES" } ] }, "title": "Biological Responses to Therapeutic Treatments of Human Vascular Diseases", "ispublished": "unpub", "full_text_status": "public", "keywords": "Transcriptome, proteomics, drug, RNA-seq, vascular disease, eye, software, biomaterial", "abstract": "Diseases of the retina affect hundreds of millions of patients worldwide, with limited treatment options available. ALG-1001 is an investigational drug that showed success in mitigating disease symptoms in animal models and improved patient vision in multiple clinical trials. To gain a better understanding of the drug\u2019s mechanism of action, RNA sequencing (RNA-seq) and shotgun proteomics were employed to study the drug-induced transcriptome change in retinal tissue and cell culture models. Chapter 2 focuses on application of this approach in an animal model of the disease that showed the drug can reversely modulate hypoxia-activated angiogenesis and inflammation gene expression changes. Chapter 3 discusses the study of drug-induced transcriptome response in two cell culture models relevant to pathophysiology of the retinal diseases. Chapter 4 explores retinal cell transcriptome after short and long-term exposure to disease-relevant hypoxia condition and after hypoxia recovery. Appendix A documents our shotgun proteomics protocol and includes results from the application of this method in the study of drug mechanism.
\r\n\r\nTypical RNA-seq studies use few biological replicates for differential expression analysis, mainly due to the high cost of generating sequencing data. As a result, not all comparisons have the proper statistical power, which result in false positives and false negatives that can lead the researcher to the wrong conclusion. Chapter 5 discusses a novel algorithm and software that help users perform quality control of their dataset to identify whether the appropriate sample size was used for differential gene discovery. The chapter covers demonstration of the software with four publicly available RNA-seq datasets to illustrate its utility.
\r\n\r\nBioresorbable vascular scaffolds (BVSs) are the application of biocompatible polymer in the treatment of coronary heart disease, one of the leading causes of death worldwide. BVSs are designed to replace metal stents, which stay permanently in the body after surgery and can lead to various complications, such as lethal thrombosis. In contrast, BVSs provide the necessary support and are resorbed by the body to leave behind a healthy artery after 2-3 years. Improving on the existing BVS material, chapter 6 explores a new polymer nanocomposite that increases the structure\u2019s radial strength in a thinner profile and provides radio-opacity to enhance surgery success.
", "date": "2019", "date_type": "degree", "id_number": "CaltechTHESIS:05302019-145256322", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:05302019-145256322", "related_url": { "items": [ { "description": "Supplementary data for Chapters 2, 3, 4 and Appendix.", "type": "doi", "url": "https://doi.org/10.22002/D1.1246" }, { "description": "ERSSA: Empirical RNA-seq Sample Size Analysis Software Package, described in Chapter 5", "type": "doi", "url": "https://doi.org/doi:10.18129/B9.bioc.ERSSA" } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "NIH", "grant_number": "T32GM112592" }, { "agency": "Rosen Center for Bioengineering at Caltech" }, { "agency": "Allegro Ophthalmic" }, { "agency": "Caltech" } ] }, "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "suggestions": "Released to public view 12122019 // Restricted to Caltech community only until 10 December 2019. // From author: We are pursuing publication of several studies (Chapter 2, 5 and 6) included in the thesis.", "deposited_by": "Zixuan Shao", "deposited_on": "2019-06-10 22:47:03", "doi": "10.7907/P2S4-AY40", "divisions": { "items": [ "div_bbe" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "woldb@caltech.edu", "id": "Wold-B-J", "name": { "family": "Wold", "given": "Barbara J." }, "role": "member" }, { "email": "melowitz@caltech.edu", "id": "Elowitz-M-B", "name": { "family": "Elowitz", "given": "Michael B." }, "role": "member" }, { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "chair" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2018-12-21", "gradofc_approval_date": "2019-06-10", "review_status": "approved", "option_major": { "items": [ "bioeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2019", "author_list": "Shao, Zixuan", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Wold, Barbara J.; Elowitz, Michael B.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/11276", "eprint_id": 11276, "rev_number": 50, "documents": [ { "id": "/id/document/95159", "doc_id": 95159, "rev_number": 12, "files": [ { "id": "/id/file/271038", "fileid": 271038, "datasetid": "document", "objectid": 95159, "filename": "Movie S5-2.mov", "mime_type": "video/quicktime", "hash": "21fd6dd8065908f50a5f0473e0c5a593", "hash_type": "MD5", "filesize": 58093361, "mtime": "2018-11-16 22:24:02", "url": "/11276/1/Movie S5-2.mov" } ], "eprint_id": 11276, "pos": 1, "placement": 5, "mime_type": "video/quicktime", "format": "video/quicktime", "format_desc": "Movie S5.2 reference in Chapter 5", "language": "en", 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"media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/104766" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/104766" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/104766" } ] } } ], "eprint_status": "archive", "userid": 11372, "dir": "disk0/00/01/12/76", "datestamp": "2018-11-27 19:45:48", "lastmod": "2021-05-25 23:22:13", "status_changed": "2018-11-27 19:45:48", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "karthikramachandran711@gmail.com", "id": "Ramachandran-Karthik", "name": { "family": "Ramachandran", "given": "Karthik" }, "orcid": "0000-0003-1820-7555", "show_email": "YES" } ] }, "title": "Bioresorbable Vascular Scaffolds Gain Ductility, Resistance to Hydrolysis, and Radial Strength via a Unique Poly L-lactide Microstructure", "ispublished": "unpub", "full_text_status": "public", "keywords": "Poly L-lactide, Bioresorbable Vascular Scaffolds, X-ray Microdiffraction, Coronary Heart Disease, Tungsten Disulfide, Nanocomposites", "abstract": "Advances in tissue engineering over the past few decades are poised to revolutionize drug delivery and biomedical implants. Bioresorbable vascular scaffolds (BVS), which are made from the semicrystalline polymer poly (L-lactide), are an example of polymers saving and improving the quality of human life. BVSs are emerging as a promising alternative to metal stents for the treatment of coronary heart disease (CHD), one of the leading causes of death in the world. In contrast to permanent stents, BVSs are designed to have a limited lifespan in the body; they restore blood flow through the occluded artery by lending it support for 3-6 months, but are completely resorbed in 2-3 years, leaving behind a healthy artery. This transient character of BVS restores vasomotion in the treated artery and can eliminate the risk of thrombosis, a dreaded complication regarded as the bane of stenting.
\r\n\r\nThe promising success of the first and currently only clinically-approved BVS (FDA-approval in 2016) provides an impetus to continue its development. The struts of the BVS (~ 150\u03bcm) are nearly two times thicker than in metal stents (~ 80\u03bcm). A thicker device is challenging to implant and is unable to treat smaller and tortuous arteries. Furthermore, clinicians speculate that irregular blow flow over thicker struts may contribute towards thrombosis. An added complication of working with BVSs is that they are difficult to visualize with X-rays owing to the low atomic mass of polymers. The need for a BVS that is thinner, stronger, and radio-opaque is the motivation for this thesis, which aims to extend the benefits of transient implants to a broader patient population. Chapter I provides a brief chronological overview of the evolution of cardiovascular therapeutics to combat CHD. Chapters II and III elucidate micron-scale gradients in the PLLA microstructure of the clinically-approved BVS that overcome PLLA\u2019s inherent brittleness and provide lasting radial support to the artery. Chapter IV discusses the fabrication of novel instrumentation to establish structure-property relationships for scaffolds, and Chapter V explores polylactide nanocomposites that not only increase radial strength in a thinner profile but also provide radio-opacity.
", "date": "2019", "date_type": "degree", "id_number": "CaltechTHESIS:11162018-140640407", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:11162018-140640407", "related_url": { "items": [ { "description": "Article based on Chapter 2 (published in PNAS).", "type": "doi", "url": "https://doi.org/10.1073/pnas.1602311113" }, { "description": "Article based on Chapter 3 (published in Polymers).", "type": "doi", "url": "https://doi.org/10.3390/polym10030288" }, { "description": "Article based on Chapter 4 (published in PNAS).", "type": "doi", "url": "https://doi.org/10.1073/pnas.1807347115" } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "Abbott (United States)" }, { "agency": "Caltech" }, { "agency": "NIH", "grant_number": "5F31HL137308" } ] }, "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "suggestions": "Released to public view 27 November 2019.\r\n\r\nEmbargo extension request approved per KJ 6/11/19 // Withheld until 27 November 2019 // From author: The last chapter of this thesis is undergoing revisions for resubmission to Biomacromolecules (ACS journal). The revised manuscript should be submitted in the next month.\r\n// Original embargo request // Withheld until 27 May 2019. From author: The last chapter of this thesis will be submitted to the journal Biomacromolecules in December 2018. The journal requires that any form of the manuscript should not appear online prior to publication of the manuscript.", "deposited_by": "Karthik Ramachandran", "deposited_on": "2018-11-27 19:45:48", "doi": "10.7907/9146-5159", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "zgw@cheme.caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" }, { "email": "rustem@caltech.edu", "id": "Ismagilov-R-F", "name": { "family": "Ismagilov", "given": "Rustem F." }, "role": "member" }, { "email": "mrobb@caltech.edu", "id": "Robb-Maxwell-J", "name": { "family": "Robb", "given": "Maxwell J." }, "role": "member" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2018-10-02", "gradofc_approval_date": "2018-11-27", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2019", "author_list": "Ramachandran, Karthik", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Wang, Zhen-Gang; Ismagilov, Rustem F.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/11567", "eprint_id": 11567, "rev_number": 28, "documents": [ { "id": "/id/document/99592", "doc_id": 99592, "rev_number": 3, "files": [ { "id": "/id/file/286709", "fileid": 286709, "datasetid": "document", "objectid": 99592, "filename": "2019_Thesis_JoeyKim_Final.docx", "mime_type": "application/vnd.openxmlformats-officedocument.wordprocessingml.document", "hash": "0005d7863bd1a91fc7f3c7fb941a8911", "hash_type": "MD5", "filesize": 106150766, "mtime": "2019-05-30 18:40:11", "url": "/11567/1/2019_Thesis_JoeyKim_Final.docx" } ], "eprint_id": 11567, "pos": 1, "placement": 1, "mime_type": 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"media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/99653" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/99653" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/99653" } ] } }, { "id": "/id/document/132202", "doc_id": 132202, "rev_number": 1, "files": [ { "id": "/id/file/377647", "fileid": 377647, "datasetid": "document", "objectid": 132202, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "9e2d2097ccf9e233599283ca93ef569a", "hash_type": "MD5", "filesize": 38493, "mtime": "2021-06-24 18:42:19", "url": "/11567/15/indexcodes.txt" } ], "eprint_id": 11567, "pos": 15, "placement": 15, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/msword to indexcodes", "language": "en", "security": "internal", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/99592" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/99592" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/99592" } ] } } ], "eprint_status": "archive", "userid": 10406, "dir": "disk0/00/01/15/67", "datestamp": "2019-05-31 19:46:03", "lastmod": "2019-10-04 00:26:01", "status_changed": "2019-05-31 19:46:03", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "sikeimjk@gmail.com", "id": "Kim-Joey-Dongjin", "name": { "family": "Kim", "given": "Joey Dongjin" }, "orcid": "0000-0002-3359-4875", "show_email": "YES" } ] }, "title": "Effects of Branching on Conformation, Crystallization, and Self-Assembly of Polymers", "ispublished": "unpub", "full_text_status": "public", "keywords": "Polymers; bottlebrush polymers; conformation; self-assembly; crystallization", "abstract": "The central feature of bottlebrush polymers is the stiffening of the main-chain (MC) due to side-chain side-chain (SC-SC) repulsion, amplified by densely grafting long SCs, particularly in good solvent conditions. The expectation of stiffening has led most prior studies to refer to bottlebrush polymers as \"worm-like,\" \"cylindrical\" or a \"self-avoiding walk (SAW) of superblobs\". However, there is no direct evidence of stiffening of the main-chain and measurements of the overall segment distribution of the whole molecule have failed to discriminate between competing models. Here, we provide a set of measurements of the main-chain conformation (neutron scattering in a solvent that is contrast matched to the side chains) together with the overall conformation of the bottlebrush as a whole (light, X-ray, and neutron scattering) under conditions that highlight SC-SC repulsion: the side-chains are relatively long compared to prior literature, the concentration of bottlebrushes is low, and the solvent quality is good. Surprisingly, the main-chain has a conformation that does not conform to any prior models: all three main-chain lengths examined showed a window of length scales in which the scattering power increased less than linearly with length scale. In particular, the MC conformation is not worm-like. Direct observation of the main-chain conformation and the overall conformation discriminates among models more powerfully than the overall conformation alone. Inspired by the Paturej-Rubinstein tension blob model, we examined a conceptual model in which tension of the MC accumulates with distance from the ends of the MC and found that it can capture the salient features of both the MC- and whole bottlebrush scattering more gradually than previous theoretical models predicted. The conceptual model also explains our observation of a substantial increase in anisometry with increasing MC length, opposite to a worm-like chain. The results indicate that synthetically accessible bottlebrushes are not fractals; they cannot have self-similar (fractal) conformation because each increase in main-chain length accesses greater side-chain crowding than any of its shorter siblings. We expanded the work to understand the behavior in \u03b8 conditions and shorter side-chains expected to have reduced tension as well as the behavior at different concentrations.
\r\n\r\nIn addition, we characterized the interplay of self-assembly and polymer crystallization through analysis of three representative bottlebrush copolymer systems. Our results revealed a surprising number of unexpected behaviors ranging from unexpected morphologies, control of thermal properties even to complete suppression of phase transitions, and control of the orientation of crystal stem with respect to the morphological interface, which highlights the potential of the bottlebrush architecture.
", "date": "2019", "date_type": "degree", "id_number": "CaltechTHESIS:05302019-112215583", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:05302019-112215583", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "deposited_by": "Joey Kim", "deposited_on": "2019-05-31 19:46:03", "doi": "10.7907/8AFE-YC54", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jfb@cheme.caltech.edu", "id": "Brady-J-F", "name": { "family": "Brady", "given": "John F." }, "role": "chair" }, { "email": "zgw@cheme.caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" }, { "email": "mikhail@caltech.edu", "id": "Shapiro-M-G", "name": { "family": "Shapiro", "given": "Mikhail G." }, "role": "member" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2019-04-10", "gradofc_approval_date": "2019-05-31", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2019", "author_list": "Kim, Joey Dongjin", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Brady, John F.; Wang, Zhen-Gang; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/9805", "eprint_id": 9805, "rev_number": 22, "documents": [ { "id": "/id/document/68905", "doc_id": 68905, "rev_number": 4, "files": [ { "id": "/id/file/189266", "fileid": 189266, "datasetid": "document", "objectid": 68905, "filename": "Boyu Li's thesis.pdf", "mime_type": "application/pdf", "hash": "ac8889225b2a508821048ddb3a5cc28c", "hash_type": "MD5", "filesize": 6823920, "mtime": "2016-05-28 00:19:32", "url": "/9805/1/Boyu Li's thesis.pdf" }, { "id": "/id/file/203632", "fileid": 203632, "datasetid": "document", "objectid": 68905, "filename": "Boyu Li=0027s thesis.pdf", "mime_type": "application/pdf", "filesize": 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thumbnail_small", "language": "en", "security": "public", "license": "other", "main": "small.jpg", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/68905" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/68905" }, { "type": "http://eprints.org/relation/issmallThumbnailVersionOf", "uri": "/id/document/68905" } ] } }, { "id": "/id/document/130580", "doc_id": 130580, "rev_number": 1, "files": [ { "id": "/id/file/376017", "fileid": 376017, "datasetid": "document", "objectid": 130580, "filename": "indexcodes.txt", "mime_type": "text/x-c", "hash": "5a3d5a9f640626eb3bc1542e7845d480", "hash_type": "MD5", "filesize": 25898, "mtime": "2021-06-24 05:06:41", "url": "/9805/5/indexcodes.txt" } ], "eprint_id": 9805, "pos": 5, "placement": 5, "mime_type": "text/x-c", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/68905" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/68905" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/68905" } ] } } ], "eprint_status": "archive", "userid": 9768, "dir": "disk0/00/00/98/05", "datestamp": "2016-05-31 19:11:12", "lastmod": "2019-10-04 00:13:42", "status_changed": "2016-05-31 19:11:12", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "lucyliboyu@gmail.com", "id": "Li-Boyu", "name": { "family": "Li", "given": "Boyu" }, "orcid": "0000-0002-7648-3745", "show_email": "NO" } ] }, "title": "Ring/Chain versus Network: Architecture Induced by Self- versus Pairwise-Association of Telechelic Polymers", "ispublished": "unpub", "full_text_status": "public", "keywords": "Associative telechelic polymer ; assembly", "abstract": "Non-covalent associations, including hydrophobic interaction or ionic interaction for self-association, and metal coordination or hydrogen-bonding for complementary-association, have been widely used as key interactions in supramolecules formation with telechelic associative polymers. And a specific application of long associative telechelic polymers has been developed by our group for the mist-control and drag-reduction of liquid fuels. During the research on this project, self- and pairwise-associative telechelic polymers are able to be compared for the first time, and are shown to display distinct associative patterns. In order to design materials with the desired properties, it is imperative to understand the relationships between polymer chemical structure and their topology and dynamics.
\r\n\r\nIn this thesis, self-associative telechelic polymer refers to \u03b1,\u03c9-di(isophthalic acid) polycyclooctadiene (DA-PCOD), which can associate with itself through its acid ends. When tertiary amine-ended polymer is added into the mixture, isophthalic acid preferably associates pairwisely with tertiary amine due to the higher binding strength of charge-assisted hydrogen bond. And the 1:1 molar ratio mixture of \u03b1,\u03c9-di(isophthalic acid) and \u03b1,\u03c9-di(di(tertiary amine)) PCOD (DA/DB-PCOD) is named as pairwise-associative telechelic polymers. DA-PCOD is capable of multimeric association via directional hydrogen bonding due to the specific chemical structure of the isophthalic acid end, while DA/DB-PCOD exhibits dynamics that strikingly resembles that for linear covalent polymers. Temperature determines the binding strength of self- and pairwise- end association, and furthermore, the fraction of unbound ends and the distribution and topology of formed supramolecules/aggregates. Polymer length affects the dynamics of DA-PCOD mainly through determining the concentration of the end groups. And the net effect of chain length on the dynamics of DA/DB-PCOD is non-monotonic and varies with the specific temperature and concentration. The knowledge of structure-property relationships obtained from this work will enable future design of end group entities and other properties of these associative telechelic polymers for their specific applications.
\r\n", "date": "2016", "date_type": "degree", "id_number": "CaltechTHESIS:05272016-171126982", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:05272016-171126982", "related_url": { "items": [ { "description": "Mega-supramolecules for safer, cleaner fuel by end-association of long telechelic polymers", "type": "related", "url": "http://dx.doi.org/10.1126/science.aab0642" }, { "description": "A Molecular Picture for the Thermo-Reversibility of Gels Formed by Isophthalic Acid-Ended Telechelic Polymers", "type": "related", "url": "http://dx.doi.org/10.1557/opl.2015.638" }, { "description": "Mega-supramolecules by end-association of very long telechelics: Highly potent rheology modifiers.", "type": "related", "url": "http://www.acs.org/content/acs/en/meetings/spring-2014.html" } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Restricted to Caltech community only until 1 June 2017.// Released to public view 09132017", "deposited_by": "Boyu Li", "deposited_on": "2016-05-31 19:11:12", "doi": "10.7907/Z9NS0RTW", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." } } ] }, "thesis_committee": { "items": [ { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." } }, { "email": "rhg@caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." } }, { "email": "weitekamp@caltech.edu", "id": "Weitekamp-D-P", "name": { "family": "Weitekamp", "given": "Daniel P." } }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." } } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2016-05-10", "gradofc_approval_date": "2016-05-31", "review_status": "approved", "option_major": { "items": [ "chemistry" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2016", "author_list": "Li, Boyu", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Tirrell, David A.; Grubbs, Robert H.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/8893", "eprint_id": 8893, "rev_number": 35, "documents": [ { "id": "/id/document/56863", "doc_id": 56863, "rev_number": 4, "files": [ { "id": "/id/file/161590", "fileid": 161590, "datasetid": "document", "objectid": 56863, "filename": "AmyFu2015_Thesis.pdf", "mime_type": "application/pdf", "hash": "8b6b4128690c64e1eed1d59030ce6ee7", "hash_type": "MD5", "filesize": 22043453, "mtime": "2015-05-28 18:04:47", "url": "/8893/1/AmyFu2015_Thesis.pdf" } ], "eprint_id": 8893, "pos": 1, "placement": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": 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"0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/56863" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/56863" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/56863" } ] } } ], "eprint_status": "archive", "userid": 10490, "dir": "disk0/00/00/88/93", "datestamp": "2015-05-28 19:27:24", "lastmod": "2019-10-04 00:08:13", "status_changed": "2015-05-28 19:27:24", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "amyfu.hy@gmail.com", "id": "Fu-Amy-Hau-Yu", "name": { "family": "Fu", "given": "Amy Hau Yu" }, "show_email": "YES" } ] }, "title": "Mitigating Scarring and Inflammation during Corneal Wound Healing using Nanofiber-Hydrogel Scaffolds", "ispublished": "unpub", "full_text_status": "public", "keywords": "cornea; wound healing; scaffolds", "abstract": "Due to the universal lack of donor tissue, there has been emerging interest in engineering materials to stimulate living cells to restore the features and functions of injured organs. We are particularly interested in developing materials for corneal use, where the necessity to maintain the tissue\u2019s transparency presents an additional challenge. Every year, there are 1.5 \u2013 2 million new cases of monocular blindness due to irregular healing of corneal injuries, dwarfing the approximately 150,000 corneal transplants performed. The large gap between the need and availability of cornea transplantation motivates us to develop a wound-healing scaffold that can prevent corneal blindness.
\r\n\r\nTo develop such a scaffold, it is necessary to regulate the cells responsible for repairing the damaged cornea, namely myofibroblasts, which are responsible for the disordered and non-refractive index matched scar that leads to corneal blindness. Using in vitro assays, we identified that protein nanofibers of certain orientation can promote cell migration and modulate the myofibroblast phenotype. The nanofibers are also transparent, easy to handle and non-cytotoxic. To adhere the nanofibers to a wound bed, we examined the use of two different in situ forming hydrogels: an artificial extracellular matrix protein (aECM)-based gel and a photo-crosslinkable heparin-based gel. Both hydrogels can be formed within minutes, are transparent upon gelation and are easily tunable.
\r\n\r\nUsing an in vivo mouse model for epithelial defects, we show that our corneal scaffolds (nanofibers together with hydrogel) are well-tolerated (no inflammatory response or turbidity) and support epithelium regrowth. We developed an ex vivo corneal tissue culture model where corneas that are wounded and treated with our scaffold can be cultured while retaining their ability to repair wounds for up to 21 days. Using this technique, we found that the aECM-based treatment induced a more favorable wound response than the heparin-based treatment, prompting us to further examine the efficacy of the aECM-based treatment in vivo using a rabbit model for stromal wounds. Results show that treated corneas have fewer myofibroblasts and immune cells than untreated ones, indicating that our corneal scaffold shows promise in promoting a calmer wound response and preventing corneal haze formation.
\r\n", "date": "2015", "date_type": "degree", "id_number": "CaltechTHESIS:05272015-172038281", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:05272015-172038281", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Restricted to Caltech community only until 19 May 2016. Released 1 June 2016.", "deposited_by": "Amy Fu", "deposited_on": "2015-05-28 19:27:24", "doi": "10.7907/Z9Q81B00", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "member" }, { "email": "mdavis@cheme.caltech.edu", "id": "Davis-M-E", "name": { "family": "Davis", "given": "Mark E." }, "role": "member" }, { "email": "mikhail@caltech.edu", "id": "Shapiro-M-G", "name": { "family": "Shapiro", "given": "Mikhail G." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2015-05-19", "gradofc_approval_date": "2015-05-28", "thesis_awards": "Constantin G. Economou Memorial Prize, 2011", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2015", "author_list": "Fu, Amy Hau Yu", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Tirrell, David A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/8001", "eprint_id": 8001, "rev_number": 55, "documents": [ { "id": "/id/document/43701", "doc_id": 43701, "rev_number": 6, "files": [ { "id": "/id/file/130059", "fileid": 130059, "datasetid": "document", "objectid": 43701, "filename": "Ming-Hsin_Wei_2014_thesis.pdf", "mime_type": "application/pdf", "hash": "9b7dcd0996d29673b3f6ac1701fca18c", "hash_type": "MD5", "filesize": 6936655, "mtime": "2013-10-25 01:00:53", "url": "/8001/1/Ming-Hsin_Wei_2014_thesis.pdf" } ], "eprint_id": 8001, "pos": 1, "placement": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", 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"media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/43701" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/43701" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/43701" } ] } } ], "eprint_status": "archive", "userid": 3209, "dir": "disk0/00/00/80/01", "datestamp": "2016-05-03 17:02:19", "lastmod": "2019-10-04 00:03:03", "status_changed": "2016-05-03 17:02:19", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "jeremy.mh.wei@gmail.com", "id": "Wei-Ming-Hsin", "name": { "family": "Wei", "given": "Ming-Hsin" }, "show_email": "NO" } ] }, "title": "Synthesis and Potency of Long End-Associative Polymers for Mist Control", "ispublished": "unpub", "full_text_status": "public", "keywords": "mist control; telechelic; associative polymer; hydrogen bonding; shear resistance; supramolecule; high molecular weight", "abstract": "Long linear polymers that are end-functionalized with associative groups were studied as additives to hydrocarbon fluids to mitigate the fire hazard associated with the presence of mist in a crash scenario. These polymers were molecularly designed to overcome both the shear-degradation of long polymer chains in turbulent flows, and the chain collapse induced by the random placement of associative groups along polymer backbones. Architectures of associative groups on the polymer chain ends that were tested included clusters of self-associative carboxyl groups and pairs of hetero-complementary associative units.
\r\n\r\nLinear polymers with clusters of discrete numbers of carboxyl groups on their chain ends were investigated first: an innovative synthetic strategy was devised to achieve unprecedented backbone lengths and precise control of the number of carboxyl groups on chain ends (N). We found that a very narrow range of N allows the co-existence of sufficient end-association strength and polymer solubility in apolar media. Subsequent steady-flow rheological study on solution behavior of such soluble polymers in apolar media revealed that the end-association of very long chains in apolar media leads to the formation of flower-like micelles interconnected by bridging chains, which trap significant fraction of polymer chains into looped structures with low contribution to mist-control. The efficacy of very long 1,4-polybutadiene chains end-functionalized with clusters of four carboxyl groups as mist-control additives for jet fuel was further tested. In addition to being shear-resistant, the polymer was found capable of providing fire-protection to jet fuel at concentrations as low as 0.3wt%. We also found that this polymer has excellent solubility in jet fuel over a wide range of temperature (-30 to +70\u00b0C) and negligible interference with dewatering of jet fuel. It does not cause an adverse increase in viscosity at concentrations where mist-control efficacy exists.
\r\n\r\nFour pairs of hetero-complementary associative end-groups of varying strengths were subsequently investigated, in the hopes of achieving supramolecular aggregates with both mist-control ability and better utilization of polymer building blocks. Rheological study of solutions of the corresponding complementary associative polymer pairs in apolar media revealed the strength of complementary end-association required to achieve supramolecular aggregates capable of modulating rheological properties of the solution.
\r\n\r\nBoth self-associating and complementary associating polymers have therefore been found to resist shear degradation. The successful strategy of building soluble, end-associative polymers with either self-associative or complementary associative groups will guide the next generation of mist-control technology.
", "date": "2014", "date_type": "degree", "id_number": "CaltechTHESIS:10192013-181502465", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:10192013-181502465", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Withheld until 31 December 2015. Released 5/3/2016\r\n\r\n//Jeremy. Patenting and potential commercial venues under consideration. skj 12/02/2014//", "deposited_by": "Ming Hsin Wei", "deposited_on": "2016-05-03 17:02:19", "doi": "10.7907/Z91834FW", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "mdavis@cheme.caltech.edu", "id": "Davis-M-E", "name": { "family": "Davis", "given": "Mark E." }, "role": "member" }, { "email": "virendra.sarohia@jpl.nasa.gov", "id": "Sarohia-V", "name": { "family": "Sarohia", "given": "Virendra" }, "role": "member" }, { "email": "zgw@cheme.caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2013-09-04", "gradofc_approval_date": "2013-11-13", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. 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Physics, SANS, DLS, Bottlebrush, Telechelic, Side-Group Liquid Crystalline Polymer, ROMP, ATRP, Scattering", "abstract": "The solution behavior of linear polymer chains is well understood, having been the subject of intense study throughout the previous century. As plastics have become ubiquitous in everyday life, polymer science has grown into a major field of study. The conformation of a polymer in solution depends on the molecular architecture and its interactions with the surroundings. Developments in synthetic techniques have led to the creation of precision-tailored polymeric materials with varied topologies and functionalities. In order to design materials with the desired properties, it is imperative to understand the relationships between polymer architecture and their conformation and behavior. To meet that need, this thesis investigates the conformation and self-assembly of three architecturally complex macromolecular systems with rich and varied behaviors driven by the resolution of intramolecular conflicts. First we describe the development of a robust and facile synthetic approach to reproducible bottlebrush polymers (Chapter 2). The method was used to produce homologous series of bottlebrush polymers with polynorbornene backbones, which revealed the effect of side-chain and backbone length on the overall conformation in both good and theta solvent conditions (Chapter 3). The side-chain conformation was obtained from a series of SANS experiments and determined to be indistinguishable from the behavior of free linear polymer chains. Using deuterium-labeled bottlebrushes, we were able for the first time to directly observe the backbone conformation of a bottlebrush polymer which showed self-avoiding walk behavior. Secondly, a series of SANS experiments was conducted on a homologous series of Side Group Liquid Crystalline Polymers (SGLCPs) in a perdeuterated small molecule liquid crystal (5CB). Monodomain, aligned, dilute samples of SGLCP-b-PS block copolymers were seen to self-assemble into complex micellar structures with mutually orthogonally oriented anisotropies at different length scales (Chapter 4). Finally, we present the results from the first scattering experiments on a set of fuel-soluble, associating telechelic polymers. We observed the formation of supramolecular aggregates in dilute (\u22640.5wt%) solutions of telechelic polymers and determined that the choice of solvent has a significant effect on the strength of association and the size of the supramolecules (Chapter 5). A method was developed for the direct estimation of supramolecular aggregation number from SANS data. The insight into structure-property relationships obtained from this work will enable the more targeted development of these molecular architectures for their respective applications. ", "date": "2014", "date_type": "degree", "id_number": "CaltechTHESIS:11182013-104133647", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:11182013-104133647", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Withheld until 1 October 2015. Released Nov. 2, 2015", "deposited_by": "Paul Pirogovsky", "deposited_on": "2015-11-02 17:28:52", "doi": "10.7907/0DXJ-3H18", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "mdavis@cheme.caltech.edu", "id": "Davis-M-E", "name": { "family": "Davis", "given": "Mark E." }, "role": "member" }, { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "member" }, { "email": "zgw@cheme.caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2013-11-01", "gradofc_approval_date": "2013-11-25", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. 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"media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/49703" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/49703" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/49703" } ] } } ], "eprint_status": "archive", "userid": 264, "dir": "disk0/00/00/84/50", "datestamp": "2016-09-20 18:56:55", "lastmod": "2019-10-04 00:05:26", "status_changed": "2016-09-20 18:56:55", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "artemis.ailianou@gmail.com", "id": "Ailianou-Artemis", "name": { "family": "Ailianou", "given": "Artemis" }, "show_email": "NO" } ] }, "title": "Development of Semicrystalline Morphology of Poly(L-lactic Acid) during Processing of a Vascular Scaffold", "ispublished": "unpub", "full_text_status": "public", "keywords": "semicrystalline, PLLA, vascular, scaffold", "abstract": "New and promising treatments for coronary heart disease are enabled by vascular scaffolds made of poly(L-lactic acid) (PLLA), as demonstrated by Abbott Vascular\u2019s bioresorbable vascular scaffold. PLLA is a semicrystalline polymer whose degree of crystallinity and crystalline microstructure depend on the thermal and deformation history during processing. In turn, the semicrystalline morphology determines scaffold strength and biodegradation time. However, spatially-resolved information about the resulting material structure (crystallinity and crystal orientation) is needed to interpret in vivo observations.
\r\n \r\nThe first manufacturing step of the scaffold is tube expansion in a process similar to injection blow molding. Spatial uniformity of the tube microstructure is essential for the consistent production and performance of the final scaffold. For implantation into the artery, solid-state deformation below the glass transition temperature is imposed on a laser-cut subassembly to crimp it into a small diameter. Regions of localized strain during crimping are implicated in deployment behavior.
\r\n\r\nTo examine the semicrystalline microstructure development of the scaffold, we employed complementary techniques of scanning electron and polarized light microscopy, wide-angle X-ray scattering, and X-ray microdiffraction. These techniques enabled us to assess the microstructure at the micro and nano length scale. The results show that the expanded tube is very uniform in the azimuthal and axial directions and that radial variations are more pronounced. The crimping step dramatically changes the microstructure of the subassembly by imposing extreme elongation and compression. Spatial information on the degree and direction of chain orientation from X-ray microdiffraction data gives insight into the mechanism by which the PLLA dissipates the stresses during crimping, without fracture. Finally, analysis of the microstructure after deployment shows that it is inherited from the crimping step and contributes to the scaffold\u2019s successful implantation in vivo.
\r\n", "date": "2014", "date_type": "degree", "id_number": "CaltechTHESIS:05302014-173923900", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:05302014-173923900", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "Abbot Vascular" } ] }, "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Withheld until 1 June 2016. Released 9/20/2016.", "deposited_by": "Artemis Ailianou", "deposited_on": "2016-09-20 18:56:55", "doi": "10.7907/Z9VT1Q26", "alt_title": { "items": [ "Development of Semicrystalline Morphology of Poly (L-lactic Acid) during Processing of a Vascular Scaffold" ] }, "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "rhg@caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "role": "member" }, { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "member" }, { "email": "mikhail@caltech.edu", "id": "Shapiro-M-G", "name": { "family": "Shapiro", "given": "Mikhail G." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2014-05-05", "gradofc_approval_date": "2014-06-02", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. 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"main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/82949" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/82949" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/82949" } ] } }, { "id": "/id/document/128492", "doc_id": 128492, "rev_number": 1, "files": [ { "id": "/id/file/373928", "fileid": 373928, "datasetid": "document", "objectid": 128492, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "58621df6b22107fa19e16a36d5de1b25", "hash_type": "MD5", "filesize": 35669, "mtime": "2021-06-24 02:55:33", "url": "/7882/29/indexcodes.txt" } ], "eprint_id": 7882, "pos": 29, "placement": 29, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/83066" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/83066" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/83066" } ] } } ], "eprint_status": "archive", "userid": 1170, "dir": "disk0/00/00/78/82", "datestamp": "2017-09-26 16:10:23", "lastmod": "2019-10-04 00:02:16", "status_changed": "2017-09-26 16:10:23", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "zuleikha.kurji@gmail.com", "id": "Kurji-Zuleikha", "name": { "family": "Kurji", "given": "Zuleikha" }, "show_email": "NO" } ] }, "title": "Molecular Design of Side-Group Liquid Crystalline Polymers: Understanding Their Interactions with Small Molecule Liquid Crystal Solvent", "ispublished": "unpub", "full_text_status": "public", "keywords": "polymers, liquid crystals, side-group liquid crystal polymers, side chain liquid crystal polymers, nematic, ferroelectric, vertically aligned, small angle x-ray scattering, small angle neutron scattering", "abstract": "Liquid crystal (LC) gels \u2013 the combination of macromolecules with small molecule LCs \u2013 couple the\r\nelasticity and mechanical strength of polymers to the order inherent to LCs and are attractive to many\r\nresearchers hoping to marry liquid crystals' optical and electro-optical responsiveness with polymers'\r\nmechanical strength and ease of processing. In particular, side-group liquid crystal polymers (SGLCPs)\r\nare flexible-chain polymers that are functionalized with LC side-groups. Here we introduce the concept\r\nof polymer dopants: homogenously dissolved LC-containing SGLCP homopolymers that are molecularly\r\ndesigned for solubility in and coupling to small molecule LC solvents. Using polymer analogous\r\nchemistry (changing the molecular makeup of the side groups and their linkers, while keeping backbone\r\nmolecular weight, polydispersity index, and degree of polymerization constant), we\u2019ve targeted the effect\r\nof side-group orientation, dipole position and strength, spacer length and linking-group type on\r\npolymer solubility and bulk material properties. We've shown that, at low concentration, these dopants\r\ncan have significant effects on the bulk material properties of two types of LCs: ferroelectric and vertically\r\naligned nematic LCs.", "date": "2013", "date_type": "degree", "id_number": "CaltechTHESIS:06102013-114658448", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:06102013-114658448", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Final thesis delivered to library 09/25/2017.\r\n\r\n\r\n\r\n", "deposited_by": "Zuleikha Kurji", "deposited_on": "2017-09-26 16:10:23", "doi": "10.7907/Z9WH2N6R", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "wag@wag.caltech.edu", "id": "Goddard-W-A-III", "name": { "family": "Goddard", "given": "William A., III" }, "role": "chair" }, { "email": "rhg@its.caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "role": "member" }, { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "member" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2013-06-03", "gradofc_approval_date": "2013-06-11", "review_status": "approved", "option_major": { "items": [ "chemistry" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2013", "author_list": "Kurji, Zuleikha", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Goddard, William A., III; Grubbs, Robert H.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/6947", "eprint_id": 6947, "rev_number": 27, "documents": [ { "id": "/id/document/45650", "doc_id": 45650, "rev_number": 5, "files": [ { "id": "/id/file/133914", "fileid": 133914, "datasetid": "document", "objectid": 45650, "filename": "Thesis_Final.pdf", "mime_type": "application/pdf", "hash": "64970b372e21e2c67c4b0d5b5351274c", "hash_type": "MD5", "filesize": 14140320, "mtime": "2014-02-04 17:16:15", "url": "/6947/1/Thesis_Final.pdf" } ], "eprint_id": 6947, "pos": 1, "placement": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", 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indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/45650" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/45650" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/45650" } ] } } ], "eprint_status": "archive", "userid": 9074, "dir": "disk0/00/00/69/47", "datestamp": "2014-06-30 18:13:52", "lastmod": "2019-10-03 23:55:18", "status_changed": "2014-06-30 18:13:52", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "ryanmatthewturner@gmail.com", "id": "Turner-Ryan-Matthew", "name": { "family": "Turner", "given": "Ryan Matthew" }, "show_email": "NO" } ] }, "title": "Reshaping Elastomers with Light: First Principles Model of Diffusion-Induced Deformation", "ispublished": "unpub", "full_text_status": "public", "keywords": "light-adjustable lens, photopolymer, diffusion, deformation, finite-element, elastomer, theory", "abstract": "Elastomeric photopolymers are a new class of materials originally developed at Caltech for use as intraocular lenses. These materials consist of a host network swollen with short-chain, photoreactive \"macromers.\" Using a light source for selective photopolymerization, gradients in free macromer molecules are created, driving diffusion-induced shape change. Although models exist for external flow of solvent into a swelling gel or for gel deswelling caused by externally imposed forces, no known model exists to account for reaction-induced diffusion-deformation for a force-free material in which solvent can neither enter nor leave. To predict this unique reaction-diffusion-induced shape change, we propose a simple \"two-component\" model which treats macromer as converting directly into network strands. This model is first shown to be in good agreement with experimental data on the equilibrium swelling of elastomeric photopolymers. We then use mixture theory to develop constitutive laws for the system stress and the flux of macromer by ensuring that the second law of thermodynamics holds. Finally, we implement the theory to a variety of problems - including a finite-element model of the light-adjustable lens - in each case systematically detailing the relative importance of the material parameters on the magnitude and rate of shape change. We determined that the shape change depends upon the rate of consumption of macromer (specified by the initial extent of reaction profile and the initial volume fraction of macromer) and is independent of the network modulus or the macromer molar mass. In addition, we found that the macromer molar mass serves only to determine the rate at which the deformation proceeds, whereas the network modulus serves to determine the magnitude of the internal forces experienced in the photopolymer.", "date": "2012", "date_type": "degree", "id_number": "CaltechTHESIS:04192012-094254839", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:04192012-094254839", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Ryan Turner", "deposited_on": "2014-06-30 18:13:52", "doi": "10.7907/RVVD-2J26", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "zgw@caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" }, { "email": "jfb@caltech.edu", "id": "Brady-J-F", "name": { "family": "Brady", "given": "John F." }, "role": "member" }, { "email": "robinselinger@gmail.com", "id": "Selinger-R-L-B", "name": { "family": "Selinger", "given": "Robin L. B." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2012-02-12", "gradofc_approval_date": "2012-04-30", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2012", "author_list": "Turner, Ryan Matthew", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Wang, Zhen-Gang; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/6412", "eprint_id": 6412, "rev_number": 31, "documents": [ { "id": "/id/document/34597", "doc_id": 34597, "rev_number": 4, "files": [ { "id": "/id/file/109744", "fileid": 109744, "datasetid": "document", "objectid": 34597, "filename": "thesis release request for Joyce Huynh jan 2013.txt", "mime_type": "message/rfc822\\0117bit", "hash": "6f13235f971049933b9b99535208f68f", "hash_type": "MD5", "filesize": 1455, "mtime": "2013-01-11 22:49:45", "url": "/6412/6/thesis release request for Joyce Huynh jan 2013.txt" } ], "eprint_id": 6412, "pos": 6, "placement": 6, "mime_type": "message/rfc822\\0117bit", "format": 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Protein-protein cross-links include disulfide bonds, enzymatic cross-links and non-enzymatic cross-links. Disulfide bonds and enzymatic cross-links are closely regulated in the body. Non-enzymatic cross-links accumulate in an uncontrolled manner, often leading to deleterious effects. Clinically, non-enzymatic cross-links can be inserted in a controlled manner, both temporally and spatially, using photo-activation to achieve effects ranging from killing tumors to stabilizing ocular shape.
\r\n\r\nThe shape of the eye is maintained by the ocular coat\u2014the cornea and sclera. Diseases that result in progressive shape changes can lead to blindness (degenerative myopia) or necessitate a corneal transplant (keratoconus and post-LASIK ectasia). Photodynamic corneal cross-linking, pioneered by Wollensak et al. using riboflavin activated by near-ultraviolet light (riboflavin/UVA), halts the progression of keratoconus; if applied to the sclera, it might halt the progression of degenerative myopia, as well. However, this treatment suffers from severe cytotoxicity. The literature to date implicitly assumes that photodynamic cross-linking is inherently toxic. The present research demonstrates that protein-protein cross-linking can be achieved with minimal toxicity using eosin Y activated by visible light (eosin Y/visible).
\r\n\r\nAt a molecular level, both eosin Y/visible and riboflavin/UVA are shown to act through a singlet oxygen mechanism; therefore, they are expected to produce similar covalent modifications of collagenous tissues. Real-time measurements of the increase in elastic modulus during irradiation show that the eosin Y/visible and riboflavin/UVA produce similar rates of cross-linking. The transport coefficients of both eosin Y and riboflavin were measured for both sclera and de-epithelialized cornea. The diffusivity and partition coefficient values, together with the cross-linking kinetics, were used in a predictive model of the cross-linking profile as a function of treatment parameters. The predictive model also serves as an optimization tool for guiding the selection of treatment parameters in pre-clinical studies. In contrast to the dramatic toxicity of the riboflavin/UVA treatment (which kills all of the keratocytes and the endothelium in the rabbit model), the eosin Y/visible treatment achieves comparable cross-linking with negligible phototoxicity.
\r\n", "date": "2011", "date_type": "degree", "id_number": "CaltechTHESIS:05202011-143758537", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:05202011-143758537", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Joyce Huynh", "deposited_on": "2013-03-01 19:51:00", "doi": "10.7907/GQ57-4J30", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "member" }, { "email": "mdavis@cheme.caltech.edu", "id": "Davis-M-E", "name": { "family": "Davis", "given": "Mark E." }, "role": "member" }, { "email": "schwartz7@mindspring.com", "id": "Schwartz-Daniel-S", "name": { "family": "Schwartz", "given": "Daniel S." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2011-05-06", "gradofc_approval_date": "2011-05-27", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2011", "author_list": "Huynh, Joyce", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Tirrell, David A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/5818", "eprint_id": 5818, "rev_number": 62, "documents": [ { "id": "/id/document/10289", "doc_id": 10289, "rev_number": 8, "files": [ { "id": "/id/file/65759", "fileid": 65759, "datasetid": "document", "objectid": 10289, "filename": "YX_Table_of_Contents.pdf", "mime_type": "application/pdf", "filesize": 149560, "mtime": "2012-12-26 03:25:51", "url": "/5818/1/YX_Table_of_Contents.pdf" } ], "eprint_id": 5818, "pos": 1, "placement": 2, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "table of contents", "language": "en", "security": "public", "license": "other", "main": 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"Xia", "given": "Yan" }, "show_email": "NO" } ] }, "title": "Syntheses of Polymers with Diverse Architectures via Metathesis Polymerization and Investigation of Their Structure-Property Relationships", "ispublished": "unpub", "full_text_status": "public", "keywords": "metathesis polymerization, cyclic polymer, brush polymer, liquid crystalline network", "abstract": "Metathesis polymerization using highly active, functional-group-tolerant catalysts is a powerful and versatile method for polymer synthesis. This thesis focuses on the preparation of a variety of advanced polymer architectures using well-defined ruthenium-based metathesis catalysts and the study of materials properties dictated by those unique macromolecular structures.
\r\n\r\nChapter 1 introduces olefin metathesis, metathesis polymerization, and recent developments in living/controlled polymerization and polymer functionalization. The goal is to provide a summary of the current toolbox of polymer chemists. The second part of Chapter 1 describes using these tools to synthesize different macromolecular architectures.
\r\n\r\nChapters 2 and 3 describe ring-expansion metathesis polymerization (REMP) using cyclic catalysts. Chapter 2 focuses on catalyst development, while Chapter 3 focuses on the REMP mechanism and cyclic polymer characterization.
\r\n\r\nChapters 4 and 5 focus on brush polymers. Chapter 4 describes the syntheses of linear and cyclic brush polymers using ring-opening metathesis polymerization (ROMP) and REMP of macromonomers (MMs), respectively. Chapter 5 describes the efficient synthesis of brush copolymers and the study of their melt state self-assembly into highly ordered nanostructures.
\r\n\r\nChapter 6 describes the synthesis and electro-optic response of well-defined liquid crystalline (LC) gels that were made from controlled end-linking of telechelic LC polymers. These gels possessed very fast, reversible electro-optic switching; the degree of response was closely related to network structure.
", "date": "2010-06-11", "date_type": "degree", "id_number": "CaltechTHESIS:05192010-182707354", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:05192010-182707354", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Gayle Hammer", "deposited_by": "Yan Xia", "deposited_on": "2010-06-04 17:27:06", "doi": "10.7907/WTBS-F528", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "rhg@caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "role": "advisor" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "chair" }, { "email": "heath@caltech.edu", "id": "Heath-J-R", "name": { "family": "Heath", "given": "James R." }, "role": "member" }, { "email": "mdavis@cheme.caltech.edu", "id": "Davis-M-E", "name": { "family": "Davis", "given": "Mark E." }, "role": "member" }, { "email": "rhg@caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "role": "member" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2010-04-19", "gradofc_approval_date": "2010-05-28", "review_status": "approved", "option_major": { "items": [ "chemistry" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2010", "author_list": "Xia, Yan", "advisor_list": "Grubbs, Robert H. and Kornfield, Julia A.", "comittee_list": "Tirrell, David A.; Heath, James R.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/3476", "eprint_id": 3476, "rev_number": 37, "documents": [ { "id": "/id/document/6019", "doc_id": 6019, "rev_number": 6, "files": [ { "id": "/id/file/35892", "fileid": 35892, "datasetid": "document", "objectid": 6019, "filename": "APPENDIX_A.pdf", "mime_type": "application/pdf", "filesize": 74976, "mtime": "2012-12-26 03:00:13", "url": "/3476/1/APPENDIX_A.pdf" } ], "eprint_id": 3476, "pos": 1, "placement": 8, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "APPENDIX_A.pdf", "language": "en", "security": "public", "license": "other", "main": "APPENDIX_A.pdf", 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"dir": "disk0/00/00/34/76", "datestamp": "2009-09-15", "lastmod": "2019-11-08 18:06:35", "status_changed": "2009-09-25 02:59:01", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "dssmirnova@gmail.com", "id": "Smirnova-Diana-Sergeievna", "name": { "family": "Smirnova", "given": "Diana Sergeievna" }, "show_email": "YES" } ] }, "title": "Application of Two-Dimensional Correlation Analysis to Explosives Detection and Polymer Crystallization", "ispublished": "unpub", "full_text_status": "public", "keywords": "2D correlation; explosives; morphology; polymer crystallization; raman; x-ray", "abstract": "This thesis presents two novel applications of two-dimensional (2D) correlation analysis: (1) long standoff detection of explosives and (2) morphology development in semicrystalline materials.
\r\n\r\nDue to the dangers of improvised explosive devices (IEDs), effective detection of explosives at standoff distances can save lives. A scheme based on 2D correlation analysis in conjunction with thermal modulation is proposed to overcome weak signals that plague long standoff detection. Implementation of 2D correlation analysis results in significant enhancement of explosive signals relative to background. Effective separation of explosive features resulting from their unstable nature compared to common contaminants is demonstrated for two biogenic compounds. Several aspects of 2D correlation analysis are examined to optimize effectiveness of detection.
\r\n\r\nUltimate physical properties of semicrystalline materials are directly related to their morphology through molecular characteristics and processing conditions. The effects of different molecular characteristics on morphology of model hydrogenated polybutadienes are examined by 2D correlation analysis of x-ray scattering data.
\r\n\r\nModel short-chain branched (SCB) polyethylenes are found to crystallize in three regimes during quiescent temperature ramps. \"Primary-irreversible\" crystallization occurs at the highest temperatures as primary lamellae propagate through unconstrained melt. During \"secondary-irreversible\" crystallization at intermediate temperatures, secondary lamellae grow in the largest non-crystalline regions between primary lamellae. \u201cReversible\u201d crystallization at low temperatures is marked by the formation of fringed micelles. This is the first time that a physical justification is presented for the separation of the irreversible crystallization into primary- and secondary-irreversible regimes.
\r\n\r\nEach regime is identified by unique features in 2D correlation plots. Two-dimensional correlation analysis provides unique insight into subtle changes in morphology, such as the development of density heterogeneities in non-crystalline regions.
\r\n\r\nThe presence of short-chain branches is found to have a profound, diminishing effect on the formation of oriented structures in response to flow-induced crystallization, which is further examined through blends containing linear and SCB polyethylene. Evidence presented suggests that a buildup of chain defects at the growth front results in a transition from oriented to isotropic crystallization. It is proposed that size of crystal structures can be controlled by dictating the amount of copolymer incorporated during crystallization.
\r\n", "date": "2010", "date_type": "degree", "id_number": "CaltechETD:etd-09112009-132932", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-09112009-132932", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2009-09-15", "doi": "10.7907/7PAR-VK52", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "member" }, { "email": "flagan@caltech.edu", "id": "Flagan-R-C", "name": { "family": "Flagan", "given": "Richard C." }, "role": "member" }, { "email": "rhg@caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2009-09-11", "thesis_defense_date": "2009-09-03", "thesis_approved_date": "2009-09-15", "gradofc_approval_date": "2009-09-15", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. 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"2008-06-02", "lastmod": "2019-12-18 22:22:44", "status_changed": "2009-09-25 02:18:32", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "MikeMackel@gmail.com", "id": "Mackel-Michael-John", "name": { "family": "Mackel", "given": "Michael John" }, "show_email": "YES" } ] }, "title": "Hydrophilic Polymers in Gels and Solutions: Surface Properties and Structure", "ispublished": "unpub", "full_text_status": "public", "keywords": "azobenzene; friction; hydrogel; light responsive; malachite green; thin film; tribology; wettability", "abstract": "Changes in the wetting properties of thin films of polyethyleneglycol (PEG) end-capped with fluoroalkyl groups are measured when the films are equilibrated at various relative humidity (RH). At high RH, the advancing contact angle on the surfaces is 20\u00ba higher than the advancing contact angle measured at low RH. The surprising transition to non-wetting character at high RH is attributed to fluoroalkyl groups ordering at the air-hydrogel interface when they are liberated by dissolution of PEG crystallites above 85% RH.
\r\n\r\nNext, the structure and tribology of a semi-interpenetrating hydrogel of agarose and an anionic polysaccharide (either hyaluronic acid or dextran sulfate) were studied. The porous structure of agarose allows incorporation of up to 2% dextran sulfate without weakening the gel\u2019s mechanical properties. Addition of the polyelectrolyte endows the gels with shape memory upon drying and reswelling; the gel can be dehydrated and rapidly swollen back to its original dimensions. The addition of both dextran sulfate and hyaluronic acid (HA) increases the lubricity of agarose when tested against hydrophilic clean glass or hydrophobic fluorinated glass. Migration of the polyelectrolytes out of the gel is believed to make the gels self-lubricating.
\r\n\t\r\nFinally, hydrophilic polymers were functionalized with photoresponsive hyrophobes in an attempt to control polymer self-assembly with light. Micelles of PEG end-capped with azobenzene molecules showed no change in size when the solutions were irradiated with UV light. PEG block copolymers were also functionalized with azobenzene and used to modify gold surfaces, but photoresponsive contact angles could not be measured. Finally, acrylamides copolymerized with the vinyl derivatives of malachite green were also studied, but the copolymers proved unsuitable for use at moderate pH.
\r\n", "date": "2008", "date_type": "degree", "id_number": "CaltechETD:etd-05192008-134942", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05192008-134942", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Released to public view 01292018 // Partially withheld: Prelim pages, ch. 1,6.// 03152017: Withheld Files Released and Restricted to Caltech community only until 15 September 2017.", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-06-02", "doi": "10.7907/5ZVF-6156", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "anand@cheme.caltech.edu", "id": "Asthagiri-A-R", "name": { "family": "Asthagiri", "given": "Anand R." }, "role": "member" }, { "email": "jfb@cheme.caltech.edu", "id": "Brady-J-F", "name": { "family": "Brady", "given": "John F." }, "role": "member" }, { "email": "flagan@cheme.caltech.edu", "id": "Flagan-R-C", "name": { "family": "Flagan", "given": "Richard C." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-05-19", "thesis_defense_date": "2008-01-29", "thesis_approved_date": "2008-06-02", "gradofc_approval_date": "2008-05-30", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2008", "author_list": "Mackel, Michael John", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Asthagiri, Anand R.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/2173", "eprint_id": 2173, "rev_number": 37, "documents": [ { "id": "/id/document/3954", "doc_id": 3954, "rev_number": 5, "files": [ { "id": "/id/file/23137", "fileid": 23137, "datasetid": "document", "objectid": 3954, "filename": "Appendix_B.pdf", "mime_type": "application/pdf", "filesize": 766173, "mtime": "2012-12-26 02:47:44", "url": "/2173/2/Appendix_B.pdf" } ], "eprint_id": 2173, "pos": 2, "placement": 4, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Appendix_B.pdf", "language": "en", "security": "validuser", "license": "other", "main": "Appendix_B.pdf", 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22:22:57", "status_changed": "2009-09-25 02:28:28", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "David-Ralph-Leonard-Ameri", "name": { "family": "David", "given": "Ralph Leonard Ameri" }, "show_email": "NO" } ] }, "title": "Associative Polymers as Antimisting Agents and Other Functional Materials via Thiol-ene Coupling", "ispublished": "unpub", "full_text_status": "mixed", "keywords": "associative polymers; extensional rheology; mist-suppression; polymer functionalization; thiol-ene addition", "abstract": "Associating polymers of varying molecular design were studied as potential additives to aviation fuel, aimed to suppress misting and thereby reduce the fuel\u2019s fire hazard in crash scenarios. Molecular architectures investigated varied from random placement along polymer chains of associating groups (referred to throughout this work as \u201cstickers\u201d) to selective clustering of the stickers at chain ends. Linear chains possessing associating functional groups grafted at random positions along the entire chain were investigated first. Model polymers with matched backbone length were synthesized to examine the effects of degree of functionalization and type of interaction (self-associating or donor-acceptor) on shear and extensional rheology of both dilute and semi-dilute solutions in non-polar hydrocarbon solvents. We found that intramolecular associations dominate the behavior of self-associating chains even in semi-dilute concentrations, leading to chain collapse and reduced shear and extensional viscosities. Mixtures of donor-acceptor chains show much more favorable intermolecular pairing in dilute solutions (as evidenced by the formation of large aggregates), but nevertheless display reduced solution elasticity and extensional viscosity relative to unmodified homologues: sticker pairing interfered with the stretching of the chains in elongational flow. Molecular designs that overcome chain collapse by clustering stickers at the ends of polymer chains were studied next. We showed by theoretical modeling that symmetric linear chains displaying strongly associating endgroups suffer instead from loop formation, which traps the bulk of the polymer into small cyclic aggregates with low mist-control properties. Therefore, we suggest molecular architectures that preclude formation of cyclic supramolecules by employing several different donor-acceptor pairs that do not affect one another (\u201corthogonal\u201d pairs). This presents a synthetic challenge, i.e., the development of simple and rapid protocols for the preparation of functional polymer materials of controlled architecture and functionality. We developed such convenient protocols (fast, non-wasteful, and scalable procedures) for the functionalization of polybutadiene by thiol-ene addition to yield functional polymers of narrow polydispersity. These powerful, versatile synthetic tools can potentially be applied to add any side-group onto any polymer, copolymer, or block copolymer displaying pendant vinyl groups, with exciting potential applications in fields ranging from organic electronics to drug delivery.", "date": "2008", "date_type": "degree", "id_number": "CaltechETD:etd-05272008-194010", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05272008-194010", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Partially withheld: full thesis and ch.2-4, and App.A.\r\nInternal docs also show patent litigation related to thesis. ", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-06-04", "doi": "10.7907/9AHR-A213", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "rhg@caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "role": "member" }, { "email": "virendra.sarohia@jpl.nasa.gov", "id": "Sarohia-V", "name": { "family": "Sarohia", "given": "Virendra" }, "role": "member" }, { "email": "zgw@cheme.caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-05-27", "thesis_defense_date": "2008-03-07", "thesis_approved_date": "2008-06-04", "gradofc_approval_date": "2008-06-03", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2008", "author_list": "David, Ralph Leonard Ameri", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Grubbs, Robert H.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/5210", "eprint_id": 5210, "rev_number": 41, "documents": [ { "id": "/id/document/36302", "doc_id": 36302, "rev_number": 6, "files": [ { "id": "/id/file/113886", "fileid": 113886, "datasetid": "document", "objectid": 36302, "filename": "MSM_Thesis_7May2008.pdf", "mime_type": "application/pdf", "hash": "81a68fda8d5a3e9d1744ea1431a5e9fe", "hash_type": "MD5", "filesize": 4241288, "mtime": "2013-03-21 21:34:16", "url": "/5210/1/MSM_Thesis_7May2008.pdf" } ], "eprint_id": 5210, "pos": 1, "placement": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Full thesis", "language": 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"media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/36344" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/36344" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/36344" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/52/10", "datestamp": "2008-05-30", "lastmod": "2020-01-29 00:44:22", "status_changed": "2014-03-18 20:47:24", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "mattson@caltech.edu", "id": "Mattson-Matthew-Sanford", "name": { "family": "Mattson", "given": "Matthew Sanford" }, "show_email": "NO" } ] }, "title": "Understanding and Treating Eye Diseases: Mechanical Characterization and Photochemical Modification of the Cornea and Sclera", "ispublished": "unpub", "full_text_status": "public", "keywords": "biomechanics; cornea; crosslinking; eye; keratoconus; myopia; sclera", "abstract": "Proper vision depends on the physical properties of the eye tissues. Diseases that alter the chemical and mechanical states of the tissue can result in a loss of functionality. Degenerative myopia and keratoconus are diseases that exhibit such changes in the sclera and cornea, respectively. These diseases may be treatable by engineering the mechanical properties of the sclera and cornea.
\r\n\r\nWe have developed an intact globe expansion method for mechanical characterization of eyes in vitro, which provides reliable measurements, with relatively few samples, and mimics the type and distribution of stresses inherent in the natural boundary conditions of the eye. Furthermore, application of high intraocular pressures provides a way to study shape changes of the sclera and cornea which are similar to those exhibited in myopia and keratoconus. Potential treatments that show an ability to prevent ocular distension in this method have a chance of preventing the deformations that occur in vivo in the diseases.
\r\n\r\nOur studies in vitro indicate that crosslinking can improve tissue mechanical stability and resistance to deformation. Light activated crosslinking provides spatial and temporal control of treatments, and photoinitiator systems such as Eosin Y (EY) and triethanolamine (TEOA) allow this control with safe doses of visible light.
\r\n\r\nFor myopia treatment, we demonstrate in vitro stabilization of eyes using the intact globe method after drug is delivered to the sclera in vitro or in vivo on 2\u20133 week old rabbits. Biocompatibility studies of the scleral treatments indicate excellent tolerance to the light and drug in both rabbits and guinea pigs. Further, we have developed treatment protocols for use in a guinea pig form-deprivation model of myopia. In normally growing guinea pig eyes, treatments can create substantial changes to eye shape. These changes are manifested in shifts in the refractive error and ocular length that persist for the duration over which the animals are monitored.
\r\n\r\nFor keratoconus, treatment in vitro on rabbit eyes using EY/TEOA demonstrates similar capabilities of corneal stabilization as a treatment currently in clinical trials. The EY/TEOA treatment shows advantages of reduced treatment time and the possibility of treatment without removal of the epithelium.
", "date": "2008", "date_type": "degree", "id_number": "CaltechETD:etd-05282008-163501", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05282008-163501", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-05-30", "doi": "10.7907/DXGR-GV57", "divisions": { "items": [ "div_eng" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "guochin@caltech.edu", "id": "Guo-Chin-Lin", "name": { "family": "Guo", "given": "Chin-Lin" }, "role": "member" }, { "email": "melowitz@caltech.edu", "id": "Elowitz-M-B", "name": { "family": "Elowitz", "given": "Michael B." }, "role": "member" }, { "email": "sefraser@caltech.edu", "id": "Fraser-S-E", "name": { "family": "Fraser", "given": "Scott E." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-05-28", "thesis_defense_date": "2008-05-07", "thesis_approved_date": "2008-05-30", "gradofc_approval_date": "2008-05-29", "review_status": "approved", "option_major": { "items": [ "appliedphys" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2008", "author_list": "Mattson, Matthew Sanford", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Guo, Chin-Lin; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1681", "eprint_id": 1681, "rev_number": 14, "documents": [ { "id": "/id/document/2659", "doc_id": 2659, "rev_number": 4, "files": [ { "id": "/id/file/16340", "fileid": 16340, "datasetid": "document", "objectid": 2659, "filename": "LFB_thesis_final_04may2007.pdf", "mime_type": "application/pdf", "filesize": 3010267, "mtime": "2012-12-26 02:40:37", "url": "/1681/1/LFB_thesis_final_04may2007.pdf" } ], "eprint_id": 1681, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": "LFB_thesis_final_04may2007.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/19398" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/19398" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/19398" } ] } }, { "id": "/id/document/15955", "doc_id": 15955, "rev_number": 3, "files": [ { "id": "/id/file/201609", "fileid": 201609, "datasetid": "document", "objectid": 15955, "filename": "Fernandez-Ballester_Lucia_2007.PDF", "mime_type": "application/pdf", "filesize": 44346, "mtime": "2016-08-22 21:15:02", "url": "/1681/2/Fernandez-Ballester_Lucia_2007.PDF" } ], "eprint_id": 1681, "pos": 2, "format": "application/pdf", "language": "en", "security": "internal", "license": "other", "main": "Fernandez-Ballester_Lucia_2007.PDF", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "approvalform" }, { "id": "/id/document/19398", "doc_id": 19398, "rev_number": 2, "files": [ { "id": "/id/file/16338", "fileid": 16338, "datasetid": "document", "objectid": 19398, "filename": "preview.png", "mime_type": "image/png", "hash": "fc15c5cab351584fa81aae5d951d0d3b", "hash_type": "MD5", "filesize": 10247, "mtime": "2012-12-26 02:40:37", "url": "/1681/3/preview.png" } ], "eprint_id": 1681, "pos": 3, "placement": 3, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "validuser", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/2659" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/2659" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/2659" } ] } }, { "id": "/id/document/121059", "doc_id": 121059, "rev_number": 1, "files": [ { "id": "/id/file/366449", "fileid": 366449, "datasetid": "document", "objectid": 121059, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "7c79ed11b340976adf78c9e429d1c35b", "hash_type": "MD5", "filesize": 23739, "mtime": "2021-06-23 21:15:43", "url": "/1681/4/indexcodes.txt" } ], "eprint_id": 1681, "pos": 4, "placement": 4, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/2659" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/2659" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/2659" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/16/81", "datestamp": "2007-05-10", "lastmod": "2020-02-28 22:58:17", "status_changed": "2009-09-25 02:11:43", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "luciafb@gmail.com", "id": "Fern\u00e1ndez-Ballester-Ballester-Lucia", "name": { "family": "Fern\u00e1ndez-Ballester", "given": "Lucia" }, "orcid": "0000-0001-6956-5104", "show_email": "NO" } ] }, "title": "Formation of Oriented Precursors in Flow-Induced Polymer Crystallization: Experimental Methods and Model Materials", "ispublished": "unpub", "full_text_status": "public", "keywords": "lamella; long chains; orientation; polymer processing; polyolefin; polypropylene; semicrystalline; shear-induced; shish-kebab", "abstract": "This thesis presents new insights into the early events of formation of oriented precursors in flow-induced crystallization of polymers, specifically isotactic polypropylene. Experimental approaches are developed to follow the creation of thread-like precursors during flow. The use of model bimodal polymers provides insight on the role of long chains in the mechanism of formation of oriented precursors. The addition of very long chains (3500 kg/mol) at low concentration (< 1% wt) dramatically reduced the stress required to trigger formation of thread-like precursors, which opened a wide range of conditions in which to discover how oriented precursors form. The combination of powerful new methods and model materials exposed a kinetic and mechanistic step prior to propagation of oriented precursors that had not been addressed in prior literature. Furthermore, the present model systems provide a bridge to the flow-induced crystallization phenomena that occur in commercial resins, making it very likely that these well-defined polymers will reveal the underlying physics that governs the effects of flow on morphology and final properties of polymers, and providing a rational basis for molecular design of polyolefins to expand the envelope of accessible properties.
\r\n\r\nThe phenomenological effects of flow on polymer crystallization have been known for decades, manifested dramatically in most processing techniques due to the high stresses imposed onto the polymer melt. Processing flows can accelerate the kinetics of crystallization by orders of magnitude, and can induce the formation of highly oriented crystallites that, in turn, impact the final material properties in the solid state. The formation of oriented thread-like precursors is at the heart of these effects of flow on polymer crystallization; however, the fundamental mechanisms underlying their development remain elusive. This lack of understanding frustrates the formulation of a predictive model that relates the polymer molecular characteristics and the imposed processing conditions to the ensuing crystallization kinetics, the final morphology, and hence, the ultimate material properties. Here, we develop experimental approaches that provide insight into the physics of formation of the oriented precursors, which identify the essential elements required in a truly predictive model of flow-induced crystallization.
\r\n\r\nIn this work, we build on experimental capabilities of imposing well-defined flow and thermal histories onto a polymer melt, and of utilizing small quantities of material so that model polymers can be investigated, which allows us to isolate the effect of specific molecular characteristics and flow conditions. Our apparatus provides us with real-time measurements that probe a range of shear stresses throughout a slit flow channel; thus, we develop a \"depth sectioning method\" as a strategy to isolate the contribution to the real-time signal that arises from a specific level of shear stress. This method is of utmost importance since the formation of thread-like precursors depends strongly on stress. To separate the development of oriented precursors during flow from the growth of oriented crystallites on them, we develop an experimental approach, the \"temperature-jump,\" inspired by classical nucleation studies.
\r\n\r\nWe use a small concentration of ultra-high molecular weight isotactic polypropylene in a matrix of shorter chains to examine the role of long chains in the creation of thread-like precursors. The use of such high molecular weight chains has revealed a richer behavior than could be observed in earlier studies, indicating that there are two stages in thread formation, kick-off and propagation, and that the stress requirement for the first step is more stringent than for the second. The data are consistent with the hypothesis that the interaction of long chains with the tip of a shish creates a local orientation that is not found elsewhere in the flowing melt.
\r\n\r\nFinally, we combine the two experimental approaches to perform measurements that capture the development of the threads during flow. For intermediate shearing times, our results are well described by the most promising model currently available, the \"recoverable strain model,\" and lay the groundwork for determining the velocity of propagation of threads at different shearing stresses. Also, it suggests that some modifications to the recoverable strain model should be included to correctly capture kick-off and saturation of the formation of threads. The experimental tools described here can be extended to other model materials, for example, to expose the effects of long chain length > 3500 kg/mol and of the stereo-regularity of the long chains. A larger parameter space can be surveyed in the future to provide additional data to test predictive models that connect molecular characteristics of a resin to structure formation under processing conditions.
", "date": "2007", "date_type": "degree", "id_number": "CaltechETD:etd-05082007-152644", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05082007-152644", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Released to public view 01292018 // ", "deposited_by": "Imported from ETD-db", "deposited_on": "2007-05-10", "doi": "10.7907/HMNK-HP78", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "member" }, { "email": "flagan@cheme.caltech.edu", "id": "Flagan-R-C", "name": { "family": "Flagan", "given": "Richard C." }, "role": "member" }, { "email": "zgw@cheme.caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2007-05-08", "thesis_defense_date": "2007-04-20", "thesis_approved_date": "2007-05-10", "gradofc_approval_date": "2007-05-10", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2007", "author_list": "Fern\u00e1ndez-Ballester, Lucia", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Tirrell, David A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/558", "eprint_id": 558, "rev_number": 64, "documents": [ { "id": "/id/document/805", "doc_id": 805, "rev_number": 7, "files": [ { "id": "/id/file/5155", "fileid": 5155, "datasetid": "document", "objectid": 805, "filename": "Abstract.pdf", "mime_type": "application/pdf", "filesize": 39560, "mtime": "2012-12-26 02:30:27", "url": "/558/1/Abstract.pdf" } ], "eprint_id": 558, "pos": 1, "placement": 3, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Abstract.pdf", "language": "en", "security": "public", "license": "other", "main": "Abstract.pdf", "media_duration": "0", 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"mtime": "2021-06-23 20:31:04", "url": "/558/40/indexcodes.txt" } ], "eprint_id": 558, "pos": 40, "placement": 40, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/817" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/817" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/817" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/05/58", "datestamp": "2007-02-12", "lastmod": "2020-03-04 00:14:33", "status_changed": "2009-09-25 01:40:08", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "rafael.verduzco@gmail.com", "id": "Verduzco-Rafael", "name": { "family": "Verduzco", "given": "Rafael" }, "orcid": "0000-0002-3649-3455", "show_email": "YES" } ] }, "title": "Self-Assembled Liquid Crystal Polymer Gels", "ispublished": "unpub", "full_text_status": "public", "keywords": "block copolymer; elastomers; gels; liquid crystal gels; liquid crystal polymer; liquid crystals; polymer; polymer network; self-assembled gel; self-assembly", "note": "In 2007 Commencement Program, thesis is entitled: Texture Transitions, Electro-Optics, and Dynamics of Polymer Liquid Crystal Gels with Novel Network Architectures", "abstract": "The combination of liquid crystals (LCs) with polymer networks results in fascinating materials in which the elasticity of the polymer network is coupled to LC order, and they hold promise for a variety of applications which depend on an optical or a mechanical response to external stimuli. Unfortunately, the methods for preparing LC networks are limited. In this work, we present two types of LC gels with novel network architectures: a physical gel made by polymer self-assembly in an LC solvent and a chemical gel made by crosslinking telechelic side-group liquid crystalline polymers (SGLCPs). The physical gel thermoreversibly transitions to a liquid on heating, and it can be uniformly aligned using electric, magnetic, or flow fields. The gel exhibits a fast electro-optical response, making it potentially viable for display applications. The physical gel also reveals novel equilibrium and dynamic properties that arise due the coupling between LC order and the polymer network. When confined between cell substrates prohibiting macroscopic shape change, it exhibits a temperature-sensitive striped texture transition. We provide a theoretical model that captures the striped texture by accounting for the compromise between nematic rubber elasticity and LC elasticity. Dynamic light scattering studies reveal two distinct director relaxation modes, in contrast to covalent gels, which show a single relaxation mode. We argue that the slower dynamics arise from the coupling between the director and the physically associated network which restructures on long time scales. We also investigate the self-assembled micellar structure of the gel via neutron scattering and rheometry studies, and these studies reveal that the gels' structure changes dramatically across the nematic-to-isotropic phase transition. Finally, we investigate model LC networks made by crosslinking telechelic SGLCPs using \"click\" chemistry. These chemical networks can be swollen in a small-molecule LC, and they exhibit a low-threshold electro-optic response and a temperature dependent size. These novel physical and chemical LC gels provide insight into the role of network structure in determining the material properties of liquid crystalline elastomers and gels.\r\n", "date": "2007", "date_type": "degree", "id_number": "CaltechETD:etd-02082007-153627", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-02082007-153627", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2007-02-12", "doi": "10.7907/VAAF-0809", "alt_title": { "items": [ "Texture Transitions, Electro-Optics, and Dynamics of Polymer Liquid Crystal Gels with Novel Network Architectures" ] }, "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "member" }, { "email": "jfb@cheme.caltech.edu", "id": "Brady-J-F", "name": { "family": "Brady", "given": "John F." }, "role": "member" }, { "email": "zgw@cheme.caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2007-02-08", "thesis_defense_date": "2007-02-05", "thesis_approved_date": "2007-02-12", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2007", "author_list": "Verduzco, Rafael", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Tirrell, David A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/685", "eprint_id": 685, "rev_number": 38, "documents": [ { "id": "/id/document/1014", "doc_id": 1014, "rev_number": 2, "files": [ { "id": "/id/file/6394", "fileid": 6394, "datasetid": "document", "objectid": 1014, "filename": "00_Scruggs_Thesis_Full.pdf", "mime_type": "application/pdf", "filesize": 10731416, "mtime": "2012-12-26 02:31:31", "url": "/685/1/00_Scruggs_Thesis_Full.pdf" } ], "eprint_id": 685, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "00_Scruggs_Thesis_Full.pdf", "language": "en", "security": "public", "license": "other", "main": 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"abstract": "The discontinuous change in solvent quality of a liquid crystal (LC) solvent, 5CB, at the nematic-isotropic phase transition produces abrupt changes in the phase behavior of solutions of coil and LC-polymers and in the self-assembly of coil-LC block copolymers. Nematic 5CB is strongly selective for a side-group liquid crystal polymer (SGLCP) and isotropic 5CB is a good solvent for both SGLCP and a random coil (polystyrene, PS). In nematic 5CB, unfavorable LC-PS interactions drive phase separation in SGLCP-PS-LC ternary solutions and drive micellization of PS-SGLCP diblocks. In isotropic 5CB, rich phase behavior occurs in both ternary solutions and block copolymer solutions. Despite the fact that isotropic 5CB is a good solvent for both SGLCP and PS, segregation can occur due to the asymmetric solvent effect (i.e., the preference of the solvent for the SGLCP). In concentrated isotropic solutions, unfavorable SGLCP-PS interactions become dominant.
\r\n\r\nIn binary solutions of SGLCP and 5CB, the delicate thermodynamic balance between LC order and polymer entropy manifests itself in a non-monotonic concentration dependence of the solutions' clearing points. The frustration between LC order and polymer entropy in an SGLCP melt is partially relieved by the addition of small molecule LC, greatly increasing the polymer's configurational freedom and stabilizing the nematic phase. In dilute solutions, the polymer adopts an anisotropic conformation because of its coupling to the LC solvent's prevailing director field; the sense and the magnitude of the anisotropy depend on the architecture of the SGLCP (end-on or side-on mesogens).
\r\n\r\nCoil-SGLCP-coil triblock copolymers self-assemble in 5CB to form liquid crystalline gels in which nematic order is coupled to an associative polymer network. The network's dynamic restructuring couples to fluctuations in the LC's local order to provide an additional relaxation process that is not present in SGLCP solutions or LC elastomers, and the importance of this process is highly dependent on the underlying anisotropy of the SGLCP-based network. The network furthermore provides a memory of the LC orientation state: when the LC is reoriented by electric-magnetic fields or mechanical shear, the network structure prevents the orientation from relaxing back to a random distribution when the aligning force is removed.
", "date": "2007", "date_type": "degree", "id_number": "CaltechETD:etd-02202007-131552", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-02202007-131552", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Author changed his name to Neal Carty sometime after graduation / skj 03032020", "deposited_by": "Imported from ETD-db", "deposited_on": "2007-02-22", "doi": "10.7907/68XG-G726", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "flagan@caltech.edu", "id": "Flagan-R-C", "name": { "family": "Flagan", "given": "Richard C." }, "role": "member" }, { "email": "rhg@its.caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "role": "member" }, { "email": "zgw@cheme.caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2007-02-20", "thesis_defense_date": "2007-02-15", "thesis_approved_date": "2007-02-22", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2007", "author_list": "Scruggs, Neal Robert", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Flagan, Richard C.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/2111", "eprint_id": 2111, "rev_number": 10, "documents": [ { "id": "/id/document/3857", "doc_id": 3857, "rev_number": 2, "files": [ { "id": "/id/file/22538", "fileid": 22538, "datasetid": "document", "objectid": 3857, "filename": "APOThesis.pdf", "mime_type": "application/pdf", "filesize": 3586495, "mtime": "2012-12-26 02:47:13", "url": "/2111/1/APOThesis.pdf" } ], "eprint_id": 2111, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "APOThesis.pdf", "language": "en", "security": "public", "license": "other", "main": "APOThesis.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/20506" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/20506" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/20506" } ] } }, { "id": "/id/document/16345", "doc_id": 16345, "rev_number": 3, "files": [ { "id": "/id/file/202559", "fileid": 202559, "datasetid": "document", "objectid": 16345, "filename": "Olsen_Adam_Paul_2006.PDF", "mime_type": "application/pdf", "filesize": 43682, "mtime": "2016-08-22 21:15:34", "url": "/2111/2/Olsen_Adam_Paul_2006.PDF" } ], "eprint_id": 2111, "pos": 2, "format": "application/pdf", "language": "en", "security": "internal", "license": "other", "main": "Olsen_Adam_Paul_2006.PDF", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "approvalform" }, { "id": "/id/document/20506", "doc_id": 20506, "rev_number": 2, "files": [ { "id": "/id/file/22536", "fileid": 22536, "datasetid": "document", "objectid": 20506, "filename": "preview.png", "mime_type": "image/png", "hash": "337a315af37167ab6aea99615913e57f", "hash_type": "MD5", "filesize": 8087, "mtime": "2012-12-26 02:47:13", "url": "/2111/3/preview.png" } ], "eprint_id": 2111, "pos": 3, "placement": 3, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "public", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/3857" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/3857" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/3857" } ] } }, { "id": "/id/document/122133", "doc_id": 122133, "rev_number": 1, "files": [ { "id": "/id/file/367527", "fileid": 367527, "datasetid": "document", "objectid": 122133, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "bd24cb5013cc0ba2094fa08ef03907ac", "hash_type": "MD5", "filesize": 20098, "mtime": "2021-06-23 21:47:35", "url": "/2111/4/indexcodes.txt" } ], "eprint_id": 2111, "pos": 4, "placement": 4, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/3857" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/3857" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/3857" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/21/11", "datestamp": "2006-06-01", "lastmod": "2020-04-16 22:27:54", "status_changed": "2009-09-25 02:27:21", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "olsen.ap@gmail.com", "id": "Olsen-Adam-Paul", "name": { "family": "Olsen", "given": "Adam Paul" }, "show_email": "YES" } ] }, "title": "Scanning Activity Gravimetric Analysis (SAGA) of Aqueous Polyethylene Oxide", "ispublished": "unpub", "full_text_status": "public", "keywords": "athermal nuclei; crystallization; levitation; polymers", "abstract": "This thesis introduces a new technique\u2014scanning activity gravimetric analysis (SAGA)\u2014for investigating phase transitions in semicrystalline polymers. Isothermal growth and dissolution of polymer crystallites within picogram to milligram samples are manifested by mass changes in response to changes in the activity of sorbed solvent vapor. Single charged particles are levitated and weighed in an electrostatic field, providing access to highly supersaturated states. Phase transitions are inferred from simultaneous equilibrium sorption and light scattering measurements. Analogous to differential scanning calorimetry, scanning solvent activity up and down exposes broad transitions between the semicrystalline solid state and the dissolved state, which are influenced by sample history. We demonstrate dissolution and crystallization of nanogram samples of polyethylene oxide by controlling the activity of sorbed water vapor and observe self-nucleation of crystallites from partially states and fully dissolved states.
\r\n\r\nMemory effects in semicrystalline polymers have been documented for a variety of systems in which the rate of crystallization depends on the temperature and duration of a prior melting step. We report analogous observations of memory effects in aqueous solution droplets of polyethylene oxide. Remnants of the crystalline phase\u2014clusters of chain folded molecules\u2014that are too small to be detected by gravimetric or optical means persist for long times in solution after macroscopic crystals have been dissolved, and they then serve as athermal nuclei when the concentration of the polymer solution droplet is increased. These remnants evolve under certain conditions toward increasing or decreasing thickness, as indicated by a shift in the conditions at which they effectively catalyze crystal growth. Although memory effects in semicrystalline polymers have usually been attributed exclusively to sluggish kinetics of melting or dissolution, thermodynamic considerations may also play an important role. A simple model describing the free energy of a lamellar crystal based on insights of Janeschitz-Kriegl captures the metastability of lamellar remnants and their evolution in thickness. The qualitative successes of the model lend support to the thermodynamic rationalization of memory effects in semicrystalline polymers.
", "date": "2006", "date_type": "degree", "id_number": "CaltechETD:etd-05262006-133416", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05262006-133416", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2006-06-01", "doi": "10.7907/5X91-2F81", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Flagan-R-C", "name": { "family": "Flagan", "given": "Richard C." }, "role": "advisor" }, { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "flagan@caltech.edu", "id": "Flagan-R-C", "name": { "family": "Flagan", "given": "Richard C." }, "role": "chair" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "co-chair" }, { "email": "seinfeld@caltech.edu", "id": "Seinfeld-J-H", "name": { "family": "Seinfeld", "given": "John H." }, "role": "member" }, { "email": "zgw@cheme.caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2006-05-26", "thesis_defense_date": "2006-05-23", "thesis_approved_date": "2006-06-01", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2006", "author_list": "Olsen, Adam Paul", "advisor_list": "Flagan, Richard C. and Kornfield, Julia A.", "comittee_list": "Flagan, Richard C.; Kornfield, Julia A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/974", "eprint_id": 974, "rev_number": 27, "documents": [ { "id": "/id/document/1515", "doc_id": 1515, "rev_number": 3, "files": [ { "id": "/id/file/9395", "fileid": 9395, "datasetid": "document", "objectid": 1515, "filename": "CSN_CH1.pdf", "mime_type": "application/pdf", "filesize": 1004952, "mtime": "2012-12-26 02:34:17", "url": "/974/1/CSN_CH1.pdf" } ], "eprint_id": 974, "pos": 1, "placement": 2, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "CSN_CH1.pdf", "language": "en", "security": "public", "license": "other", "main": "CSN_CH1.pdf", "media_duration": 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"dir": "disk0/00/00/09/74", "datestamp": "2006-01-31", "lastmod": "2020-04-16 22:22:18", "status_changed": "2009-09-25 01:52:07", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Nickerson-Charles-Sellers", "name": { "family": "Nickerson", "given": "Charles Sellers" }, "show_email": "NO" } ] }, "title": "Engineering the Mechanical Properties of Ocular Tissues", "ispublished": "unpub", "full_text_status": "public", "keywords": "Cornea; glyceraldehyde; Tissue Engineering; urea; Vitreous", "abstract": "Age and disease can cause changes in the mechanical properties of ocular tissues, which compromise visual acuity and can lead to blindness. Thus, there is great interest in understanding the mechanical properties of ocular tissues and in developing appropriate therapeutic strategies. The goal of this thesis is to discover and manipulate the molecular mechanisms that determine the bulk physical properties of the vitreous and the cornea. Both tissues are ordered biocomposites of fibrous collagen embedded in soft matrices of proteoglycans (PGs) and glycosaminoglycans (GAGs). The hydration state, mole fraction, and organization of these components determine the mechanical properties of their respective tissues. We describe the use of a novel \"cleat geometry\" for rheometry in shear to quantitatively measure the rheological properties of vitreous and other soft biomaterials. Where as the mechanical strength of these tissues has traditionally been attributed to their collagenous components, results from coordinated mechanical and biochemical analyses suggest that PGs and GAGs also make significant contributions. We hypothesize that hyaluronan contributes to the mechanical properties of the vitreous through a Donnan swelling mechanism that induces a state of tension in the collagen network. We hypothesize that the PG/GAG matrix plays a significant role in the mechanics of the cornea by restricting the translation and deformation of the collagen fibrils.
\r\n\r\nOur therapeutic goal in the vitreous is liquefaction: we seek pharmacological agents capable of separating the vitreous from the retina and destabilizing the network without damaging the adjacent tissues (retina and lens). We present evidence that using urea to disrupt hydrogen bonds may provide clinical benefits by inducing posterior vitreous detachment and reducing the shear modulus of the vitreous.
\r\n\r\nOur therapeutic goal in the cornea is to stabilize its mechanical properties against the softening associated with keratoconus. We report a clinically-relevant rise in the modulus of corneas treated with glyceraldehyde to induce crosslinking through glycation. We hypothesize that the mechanically-relevant crosslinks are those that change the properties of the soft PG/GAG matrix and its coupling to the collagen fibrils, rather than the much more numerous crosslinks that form within fibrils.
", "date": "2006", "date_type": "degree", "id_number": "CaltechETD:etd-03172005-145045", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-03172005-145045", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2006-01-31", "doi": "10.7907/0R13-2109", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "Tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "chair" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "member" }, { "email": "lhw@caltech.edu", "id": "Hsieh-Wilson-L-C", "name": { "family": "Hsieh-Wilson", "given": "Linda C." }, "role": "member" }, { "email": "rhg@its.caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2005-03-17", "thesis_defense_date": "2005-11-01", "thesis_approved_date": "2006-01-31", "review_status": "approved", "option_major": { "items": [ "chemistry" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2006", "author_list": "Nickerson, Charles Sellers", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Tirrell, David A.; Kornfield, Julia A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/4746", "eprint_id": 4746, "rev_number": 10, "documents": [ { "id": "/id/document/7623", "doc_id": 7623, "rev_number": 3, "files": [ { "id": "/id/file/46688", "fileid": 46688, "datasetid": "document", "objectid": 7623, "filename": "Thesis-Derek_Thurman.pdf", "mime_type": "application/pdf", "filesize": 8030245, "mtime": "2012-12-26 03:11:29", "url": "/4746/1/Thesis-Derek_Thurman.pdf" } ], "eprint_id": 4746, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Thesis-Derek_Thurman.pdf", "language": "en", "security": "public", "license": "other", "main": "Thesis-Derek_Thurman.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/24142" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/24142" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/24142" } ] } }, { "id": "/id/document/24142", "doc_id": 24142, "rev_number": 2, "files": [ { "id": "/id/file/46686", "fileid": 46686, "datasetid": "document", "objectid": 24142, "filename": "preview.png", "mime_type": "image/png", "hash": "f48a592cacb0ca33e310e81f7a2bb141", "hash_type": "MD5", "filesize": 8134, "mtime": "2012-12-26 03:11:29", "url": "/4746/2/preview.png" } ], "eprint_id": 4746, "pos": 2, "placement": 2, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "validuser", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/7623" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/7623" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/7623" } ] } }, { "id": "/id/document/124518", "doc_id": 124518, "rev_number": 1, "files": [ { "id": "/id/file/369948", "fileid": 369948, "datasetid": "document", "objectid": 124518, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "02f821db1682083b94b1c8a1682aa7c0", "hash_type": "MD5", "filesize": 29879, "mtime": "2021-06-23 23:39:22", "url": "/4746/3/indexcodes.txt" } ], "eprint_id": 4746, "pos": 3, "placement": 3, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/7623" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/7623" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/7623" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/47/46", "datestamp": "2005-12-05", "lastmod": "2020-05-20 19:26:30", "status_changed": "2009-09-25 03:25:21", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Thurman-Derek-Wade", "name": { "family": "Thurman", "given": "Derek Wade" }, "show_email": "NO" } ] }, "title": "Molecular Aspects of Flow-Induced Crystallization of Polypropylene", "ispublished": "unpub", "full_text_status": "public", "keywords": "crystallization; flow-induced; polymer; polypropylene; semicrystalline", "abstract": "Polyolefins, semicrystalline polymers also known as thermoplastics, are highly desirable because of their material properties, low cost, and ease in processing. The flow and thermal history experienced during processing are known to affect dramatic changes in crystalline kinetics and morphology, dictating the final material properties of solidified products. However, the underlying physics that control crystalline orientation and kinetics is not well understood. To optimize processing conditions and maximize material performance, it is desirable to understand how the interplay of molecular character and flow conditions shape crystalline microstructure.
\r\n\r\nIn the last decade, advances in catalyst technology have produced well defined materials enabling the systematic study of molecular influences on flow-induced crystallization. We investigate bimodal blends of polypropylenes (PP) in which we vary the molecular character (concentration, molecular weight, regularity) of the high molecular weight mode. We apply a number of in situ characterization tools (rheo-optics, rheo-WAXD) to the development of transient structure and interpret our findings in light of ex situ examination (polarized light microscopy, TEM) of the final morphology.
\r\n\r\nBlending a well-characterized high molecular weight isotactic polypropylene into a \"base iPP\" at various concentrations (c), we determined that blends with less than 1% of chains with Mw five times larger than the Mw of the base resin profoundly affected the crystallization kinetics and crystalline morphology of a sheared melt. Beyond unambiguously demonstrating the important role of long chains in the formation of anisotropic crystallization under flow, this approach allowed us to be specific about the length that is meant by \"long chains\" and the concentration of these chains in the melt. Varying the concentration from below to above c* revealed that the effect of the long chains involves cooperative interactions, evident in the non-linear relationship of the long chain concentration, particularly as c approaches the long chain-long chain overlap concentration. The long chains greatly enhance the formation of threadlike precursors but only mildly enhance the formation of pointlike precursors.
\r\n\r\nIn studying a series of blends in which the Mw of the long chain mode was varied, we found that increasing the Mw of the long chain portion of a bimodal blend increased the tendency to form threadlike precursors to oriented crystallization. This was highlighted by a marked decrease in the threshold stress necessary to induce oriented crystalline growth and is related to the separation in time scales between the slowest relaxing chains and the average. Thus, the propagation of shish varies strongly with the separation in time scales between the slowest relaxing chains and the average. Below a threshold ratio of relaxation times (tau_L/tau_S ~ 100) addition of long chains did not change the behavior from that of Base-PP itself.
\r\n\r\nOur analysis of real-time rheo-optical and rheo-WAXD experiments combined with depth dependent information from a novel \"depth sectioning\" analysis technique uncovers several keys to understanding how anisotropic crystallization is induced by flow. Threads first form near the channel wall, where stress is highest, and grow in length with prolonged flow. After sufficient time, thread length per unit volume saturates, perhaps due to collisions with other threads or crystalline overgrowth from those threads. Prior to saturation, when crystalline overgrowth is negligible, the thread propagation appears to be linear with shearing time. The propagation of threads varies in a nonlinear manner with stress. Finally, we identify a promising set of conditions that can be used to measure the thread propagation velocity for this material if the appropriate length scale can be assigned by microscopy.
\r\n\r\nWe examined the effects of long chain regularity on the formation of threadlike precursors, showing that addition of molecular level defects to the high end of the molecular weight distribution effectively raises the threshold stress and mitigates the formation of oriented precursors induced by flow. Our study included a model bimodal blend of isotactic and atactic polypropylene as well as large scale bimodal blends of isotactic polypropylene and a propylene-ethylene copolymer fit for pilot-scale production of nonwoven fabrics. It is noteworthy that the qualitative behavior observed in the melt-spinning process accords well with the trends evident in isothermal shear-induced crystallization. This has value in two respects. Scientifically, it is significant that idealized flow and thermal conditions may well reveal the physics relevant to polymer processing, which involves mixed shear and extension under non-isothermal conditions. Technologically, the ability to screen different resin compositions on a small scale can be used to optimize flow-induced crystallization characteristics prior to scale up.
", "date": "2006", "date_type": "degree", "id_number": "CaltechETD:etd-12032005-115154", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-12032005-115154", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2005-12-05", "doi": "10.7907/wew1-af68", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "bercaw@caltech.edu", "id": "Bercaw-J-E", "name": { "family": "Bercaw", "given": "John E." }, "role": "chair" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "member" }, { "email": "rhg@caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "role": "member" }, { "email": "wag@wag.caltech.edu", "id": "Goddard-W-A-III", "name": { "family": "Goddard", "given": "William A., III" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2005-12-03", "thesis_defense_date": "2005-11-29", "thesis_approved_date": "2005-12-05", "review_status": "approved", "option_major": { "items": [ "chemistry" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2006", "author_list": "Thurman, Derek Wade", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Bercaw, John E.; Kornfield, Julia A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/4704", "eprint_id": 4704, "rev_number": 8, "documents": [ { "id": "/id/document/7579", "doc_id": 7579, "rev_number": 3, "files": [ { "id": "/id/file/46374", "fileid": 46374, "datasetid": "document", "objectid": 7579, "filename": "Pape_thesis_overall.pdf", "mime_type": "application/pdf", "filesize": 1093686, "mtime": "2012-12-26 03:11:09", "url": "/4704/1/Pape_thesis_overall.pdf" } ], "eprint_id": 4704, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Pape_thesis_overall.pdf", "language": "en", "security": "public", "license": "other", "main": "Pape_thesis_overall.pdf", 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"/4704/6/indexcodes.txt" } ], "eprint_id": 4704, "pos": 6, "placement": 6, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from text/plain to indexcodes", "language": "en", "security": "internal", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/12473" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/12473" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/12473" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/47/04", "datestamp": "2005-12-02", "lastmod": "2019-12-21 01:32:52", "status_changed": "2009-09-25 03:24:41", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "pape@caltech.edu", "id": "Pape-E-A", "name": { "family": "Pape", "given": "Eric A" }, "show_email": "NO" } ] }, "title": "Light adjustable macromer-doped elastomers : the thermodynamics, transport, and photochemistry of silicones", "ispublished": "unpub", "full_text_status": "public", "keywords": "elastomer, photopolymer, polymer", "abstract": "Novel elastomeric photopolymer systems that exhibit macroscopic optical and mechanical changes when polymerized were designed and synthesized. These photopolymers consist of a well-defined polydimethylsiloxane matrix, an UV absorbing photoiniator, and a reactive macromer with methacrylate endgroups and a siloxane based midblock. Model elastomer matrices were synthesized, swollen with macromer, macromer was photopolymerized, and mechanical, transport, and thermodynamic behaviors of the resulting photoelastomers were measured.\r\n\r\nModulus increases of 50 to 150% were seen for sequential interpenetrating networks (IPNs) formed by photopolymerizing different length macromers in model networks. Modulus change was independent of network structure but highly dependent on macromer length and extent of macromer doping. With increased macromer doping, the modulus increase seen on photopolymerization changed from a theoretical dispersed phase behavior to bicontinuous phase behavior. Unexpectedly, mechanical properties were independent of photopolymerization conditions; increased photoinitiator content and irradiation intensity did not alter cured photopolymer modulus.\r\n\r\nSwelling behavior for model networks and IPNs was independent of network precursor molecular weight and polymer volume fraction at network preparation. As macromer molecular weight increased, experimental scaling behavior approached theoretical values. For photopolymerized IPNs, macromer was a poorer solvent than in model networks. Macromer containing phenyl groups also showed significant decreases in solubility.\r\n\r\nDiffusivity values ranged from 2x10^-11 to 2x10^-12 m2/s for 1 to 5kg/mol macromer molecular weight in both model and interpenetrating networks, were dependent on penetrant molecular weight and host network modulus, and were independent of thermodynamic interaction parameters. Diffusivities of bimodal molecular weight distributions indicated dependence on host network modulus due to molecular sieving.\r\n\r\nPhotopolymerization of macromer swollen in networks showed unusual reaction kinetics. Although reaction rates scaled linearly with reactive endgroup concentration for a specific macromer molecular weight, they exhibited variable dependence on initiation rate for different photoiniator concentrations and irradiation intensities. High irradiation intensity and photoinitiator concentration led to reaction rate independence on the initiation rate. Different macromer molecular weights showed unique reaction trajectories; maximum reaction rates and the time and extent of conversion at which they occur are not explained with simple scaling behavior. Chain length dependent termination measurements were used to describe reaction rate trajectories.", "date": "2006", "date_type": "degree", "id_number": "CaltechETD:etd-12012005-203446", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-12012005-203446", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2005-12-02", "doi": "10.7907/342T-6796", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "id": "Sandstedt-C-A", "name": { "family": "Sandstedt", "given": "Christian A." }, "role": "member" }, { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "member" }, { "email": "rhg@caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2005-12-01", "thesis_defense_date": "2005-11-28", "thesis_approved_date": "2005-12-02", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2006", "author_list": "Pape, Eric A", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Sandstedt, Christian A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1774", "eprint_id": 1774, "rev_number": 32, "documents": [ { "id": "/id/document/2875", "doc_id": 2875, "rev_number": 3, "files": [ { "id": "/id/file/17518", "fileid": 17518, "datasetid": "document", "objectid": 2875, "filename": "Chapter1.pdf", "mime_type": "application/pdf", "filesize": 225638, "mtime": "2012-12-26 02:41:49", "url": "/1774/1/Chapter1.pdf" } ], "eprint_id": 1774, "pos": 1, "placement": 2, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Chapter1.pdf", "language": "en", "security": "public", "license": "other", "main": "Chapter1.pdf", "media_duration": "0", 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"2005-05-16", "lastmod": "2023-11-08 00:37:57", "status_changed": "2009-09-25 02:15:01", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "shenx104@umn.edu", "id": "Shen-Wei", "name": { "family": "Shen", "given": "Wei" }, "show_email": "NO" } ] }, "title": "Structure, Dynamics, and Properties of Artificial Protein Hydrogels Assembled Through Coiled-Coil Domains", "ispublished": "unpub", "full_text_status": "public", "keywords": "biomaterial; coiled-coil; dynamics; hydrogel; leucine zipper; protein engineering; structure", "abstract": "The structure-property relationships of an artificial protein hydrogel, which was constructed from a triblock protein (designated AC10A) that contained two associative leucine-zipper endblocks and a water-soluble random coil midblock, were investigated to provide guidelines for the rational design of new generations of artificial protein hydrogels. The leucine zipper A domain is composed of six heptad repeating units designated as abcdefg, where the a and d positions are occupied by hydrophobic residues, and the e and g positions are mainly occupied by glutamic acid residues. In contrast to hydrogels formed from synthetic hydrophobically modified polymers, the normalized plateau storage modulus G/nkT of the AC10A gel was below 13% at all concentrations examined. This indirect evidence that AC10A tends to form a substantial fraction of looped configurations was supported by a fluorescence quenching experiment: significant quenching occurred in labeled d-AC10A-a (d=tryptophan at the N-terminus, a=coumarin at the C terminus) chains mixed with a great excess of unlabelled AC10A chains in a solution. The strong tendency to form loops originates in large part from the compact size of the random coil midblock domain (mean RH, C10~20 A, determined from quasi-elastic light scattering of C10). Despite the small aggregation number of the leucine zipper domains (tetrameric aggregates, determined from multi-angle static light scattering of AC10 diblock), the average center-to-center distance between aggregates in a 7% w/v AC10A solution is roughly 3 times the radius of gyration and 1.5 times the average end-to-end distance of the C10 domain. To avoid the energy penalty for stretching the C10 domain to form bridges, the chains tend to form loops. The importance of loops explains the nonmonotonic effect of pH on modulus and the decrease in modulus with increasing ionic strength. It also led to the design concept of increasing the midblock length or charge density to increase storage modulus.
\r\n \r\nDynamic properties of the AC10A hydrogel show correlation between network relaxation behavior and molecular exchange kinetics of the associative domain. The longest stress relaxation time changes from ca. 70 seconds at pH 8.0 to ca. 1000 seconds at pH 7.0, determined by creep measurements on 7% w/v gels. In a parallel manner, the characteristic time of the leucine zipper strand exchange varies from ca. 200 seconds at pH 8.0 to ca. 4500 seconds at pH 7.0, determined by fluorescence de-quenching after mixing a fluorescein-labeled leucine zipper solution (in which fluorescence was quenched) with a great excess of an unlabeled leucine zipper solution. Both time scales vary strongly with pH due to the associated change in charge on the e and g residues of the leucine zipper.
\r\n\r\nThe observed structure-property relationships suggest that the rapid dissolution that occurs with AC10A hydrogels in open systems originates from the tendency of the protein to form loops, the small aggregation number of the associative domains, and the transient nature of association. For applications in which materials are surrounded by excess fluids, we demonstrated two molecular design approaches to avoid the rapid dissolution. One way to slow dissolution is to suppress loops by engineering a triblock protein with dissimilar associative endblocks, PC10A, such that P associates only with P and A associates only with A. A PC10A gel erodes 500 times more slowly and exhibits a 5-fold increase in modulus compared to an AC10A gel at the same concentration. Alternatively, hydrogel stability in open systems can be improved by engineering a cysteine residue into each leucine zipper domain to allow covalent bond formation following physical association of leucine zippers. Asymmetric placement of the cysteine residue in each leucine zipper domain suppresses locking-in loops and creates linked \"multichains\". The increased valency of the building units stabilizes the hydrogels in open systems, while the physical nature of their association retains the reversibility of gelation. The gel networks dissolve at pH 12.2, where the helicity of the leucine zipper domains is reduced by ca. 90%, and re-form upon acidification.
\r\n\r\nThe ability to form robust artificial protein hydrogels in open systems opens the way to biomedical applications. Therefore, we examined their toxicity and incorporated an RGD cell-binding domain into the midblock backbone. Viability assays for mammalian 3T3 fibroblast cells cultured in the presence of the AC10A protein revealed no evidence of toxicity. Anchorage-dependent epithelial cells spread well on hydrogel films bearing an RGD cell-binding domain. In contrast, cells remained round on films without the cell-binding domain; significant apoptosis was induced. Encapsulated 3T3 fibroblast cells remained viable inside the hydrogel for at least 12 hours, suggesting that these materials have proper permeability for transferring oxygen, nutrients, and metabolic waste. The hydrogel containing the RGD domain was micropatterned on a PEG-modified glass surface and limited cell adhesion to the hydrogel region.
\r\n", "date": "2005", "date_type": "degree", "id_number": "CaltechETD:etd-05132005-114413", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05132005-114413", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2005-05-16", "doi": "10.7907/NXST-MZ65", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "advisor" }, { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "chair" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "co-chair" }, { "email": "rhg@caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "role": "member" }, { "email": "zgw@cheme.caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2005-05-13", "thesis_defense_date": "2004-12-15", "thesis_approved_date": "2005-05-16", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "option_minor": { "items": [ "biology" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2005", "author_list": "Shen, Wei", "advisor_list": "Tirrell, David A. and Kornfield, Julia A.", "comittee_list": "Tirrell, David A.; Kornfield, Julia A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/2937", "eprint_id": 2937, "rev_number": 11, "documents": [ { "id": "/id/document/5305", "doc_id": 5305, "rev_number": 3, "files": [ { "id": "/id/file/31142", "fileid": 31142, "datasetid": "document", "objectid": 5305, "filename": "Thesis_Mike_Kempe.pdf", "mime_type": "application/pdf", "filesize": 5162032, "mtime": "2012-12-26 02:55:36", "url": "/2937/1/Thesis_Mike_Kempe.pdf" } ], "eprint_id": 2937, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Thesis_Mike_Kempe.pdf", "language": "en", "security": "public", "license": "other", "main": "Thesis_Mike_Kempe.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/21853" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/21853" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/21853" } ] } }, { "id": "/id/document/21853", "doc_id": 21853, "rev_number": 3, "files": [ { "id": "/id/file/31140", "fileid": 31140, "datasetid": "document", "objectid": 21853, "filename": "preview.png", "mime_type": "image/png", "hash": "d7a4e3a31e23c8ba0fdf00ab65b7c395", "hash_type": "MD5", "filesize": 30236, "mtime": "2012-12-26 02:55:36", "url": "/2937/2/preview.png" } ], "eprint_id": 2937, "pos": 2, "placement": 2, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "public", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/5305" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/5305" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/5305" } ] } }, { "id": "/id/document/123244", "doc_id": 123244, "rev_number": 1, "files": [ { "id": "/id/file/368652", "fileid": 368652, "datasetid": "document", "objectid": 123244, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "601ef5b062ac9d6756fbfb97efe7b392", "hash_type": "MD5", "filesize": 29845, "mtime": "2021-06-23 22:28:13", "url": "/2937/3/indexcodes.txt" } ], "eprint_id": 2937, "pos": 3, "placement": 3, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/5305" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/5305" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/5305" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/29/37", "datestamp": "2003-07-24", "lastmod": "2021-02-02 22:26:02", "status_changed": "2009-09-25 02:47:44", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "mdkempe@hotmail.com", "id": "Kempe-Michael-David", "name": { "family": "Kempe", "given": "Michael David" }, "orcid": "0000-0003-3312-0482", "show_email": "YES" } ] }, "title": "Rheology and Dynamics of Side-Group Liquid Crystalline Polymers in Nematic Solvents", "ispublished": "unpub", "full_text_status": "public", "keywords": "block copolymer; liquid crystal polymer; nematic solvents; rheology", "abstract": "To form a liquid crystalline (LC) gel that retains the ability to respond rapidly to applied fields, it is necessary to work with low polymer concentrations. In turn, to form a dilute polymer network it is necessary to use very long polymers that are soluble in the small molecule LC. This research focuses on the synthesis of ultra-long side-group liquid crystalline polymers (SGLCPs), their properties when dissolved in nematic hosts, and the self-assembly of a nematic gel using an ABA triblock with an SGLCP midblock and LC-phobic end-blocks. Typically, LCs are made from small molecules that can be quickly reoriented. In applications such as artificial muscles, flexible displays, or compensating films, a more robust LC gel is desired. Prior routes to LC gels, typically using in situ polymerization, suffer from director misorientation, lack of control over cross-link density, polymer network inhomogeneity, undesired phase separation, and slow responses to applied fields. The present research (at the intersection of block copolymers, gels, and LCs) has demonstrated that an optically uniform LC gel with fast reorientational response can be achieved using a self-assembling ABA triblock copolymer.
\r\n\r\nTo provide the fundamental underpinning for the design of a self-assembling gel, we first advanced the synthesis of model SGLCPs that have well-defined length even at high degrees of polymerization. The polymerization method must provide narrow length distribution, be applicable to block copolymers, and preferably enable chains of varied side-group structure to be prepared. These requirements were met by starting from an anionically produced prepolymer and attaching the mesogen in a second step (a ?polymer analogous? approach). Homopolymers were made and characterized to determine how polymer structure affects solubility, rheological response, electro-optic response and chain conformation. This showed that cyanobiphenyl (CB) side-groups provide excellent solubility in CB-based small molecule LCs even for SGLCPs an order of magnitude longer than those investigated in solution previously; that ultra-long SGLCPs have unprecedented effects on the flow behavior of LC solutions, and that the anisotropy (R^/R?1.6) is insensitive to spacer length and degree of polymerization.
\r\n\r\nThe size of a polymer is related to the concentration necessary to form a gel network; however, there have been few studies of SGLCP dimensions in LC solvents. Since it is the polymer backbone conformation that is of interest, researchers use polymers labeled on the backbone to avoid scattering from the side groups. Unfortunately in a dilute solution this provides unacceptably low scattered intensity. Therefore, we demonstrate a method for measuring the dimensions of an unlabeled SGLCP in a perdeuterated nematic solvent, in which scattering originates from both the backbone and the pendant side groups. Since it is the backbone conformation that is of interest, we developed a method to mathematically account for scattering due to the side groups.
\r\n\r\nInformation gained from homopolymer studies guided the design of ABA block copolymers for nematic gels. We demonstrated that an optically uniform nematic gel can form in a small molecule LC even at low polymer concentrations using a triblock composed of an SGLCP center block and end-blocks that microphase separate to form physical cross-links. The key to making a dilute gel was using well-solvated, very long SGLCP midblocks. The necessity of cross-linking very dilute chain ends is prohibitive using covalent linking, but facile using end-blocks that spontaneously aggregate. In contrast to prior LC gels, these dilute gels maintain both the optical uniformity and fast reorientational responses of the small molecule LC host.
", "date": "2004", "date_type": "degree", "id_number": "CaltechETD:etd-07202003-103429", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-07202003-103429", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Michael.Kempe@nrel.gov", "deposited_by": "Imported from ETD-db", "deposited_on": "2003-07-24", "doi": "10.7907/W41E-KB03", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "member" }, { "email": "rhg@its.caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "role": "member" }, { "email": "zgw@cheme.caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2003-07-20", "thesis_defense_date": "2003-06-09", "thesis_approved_date": "2003-07-24", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2004", "author_list": "Kempe, Michael David", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Tirrell, David A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/2934", "eprint_id": 2934, "rev_number": 15, "documents": [ { "id": "/id/document/5302", "doc_id": 5302, "rev_number": 4, "files": [ { "id": "/id/file/31119", "fileid": 31119, "datasetid": "document", "objectid": 5302, "filename": "Tae_g_2002.pdf", "mime_type": "application/pdf", "filesize": 5606627, "mtime": "2012-12-26 02:55:35", "url": "/2934/1/Tae_g_2002.pdf" } ], "eprint_id": 2934, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": "Tae_g_2002.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/21850" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/21850" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/21850" } ] } }, { "id": "/id/document/21850", "doc_id": 21850, "rev_number": 3, "files": [ { "id": "/id/file/31117", "fileid": 31117, "datasetid": "document", "objectid": 21850, "filename": "preview.png", "mime_type": "image/png", "hash": "500eaea50aacfeab49f515e2503e3dc8", "hash_type": "MD5", "filesize": 10758, "mtime": "2012-12-26 02:55:35", "url": "/2934/2/preview.png" } ], "eprint_id": 2934, "pos": 2, "placement": 2, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "public", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/5302" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/5302" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/5302" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/29/34", "datestamp": "2007-07-20", "lastmod": "2022-01-14 01:12:47", "status_changed": "2009-09-25 02:47:42", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Tae-Giyoong", "name": { "family": "Tae", "given": "Giyoong" }, "show_email": "NO" } ] }, "title": "In situ Forming Hydrogels Using Self-Assembly of Fluoroalkyl-Ended Poly(ethylene Glycol)s", "ispublished": "unpub", "full_text_status": "public", "keywords": "(Chemical Engineering)", "abstract": "Telechelic polymers with hydrophilic midblocks (poly(ethylene glycol), PEG) and hydrophobic end groups (fluoroalkyl, Rf) are synthesized and explored as candidates for in situ forming hydrogels for biomedical applications. Relevant physical properties, including phase behavior, rheology and erosion kinetics, are characterized to guide rational design of polymers for specific applications, including controlled release of therapeutic proteins and deposition of biocompatible surface layers. Disruption of the aggregation of the end groups using biocompatible complexing agents or solvents produces a low viscosity liquid that is injectable; self-assembly of the gel once inside the body can be achieved gently by diffusion of the complexing agent or solvent out into the surrounding tissue. By modulating molecular structure, the mechanical and erosion properties of these hydrogels can be systematically varied over a wide range for desired applications.
\r\n\r\nWith increasing fluoroalkyl length relative to PEG length, the phase behavior of these fluoroalkyl-ended PEGs (Rf-PEGs) polymers in aqueous solution changes from singlephase behavior (continuous transition in properties from solution-like to gel-like with increasing concentration), to sol-gel coexistence, to an insoluble precipitate (Chapter 2). For sol-gel coexisting polymers, the equilibrium gel concentration and the modulus of the gel phase are governed by the length of the PEG midblock, whereas the relaxation time is determined by the hydrophobe length. The erosion characteristics of these hydrogels correlate with their phase behavior: the gels of sol-gel coexisting species exhibit surface erosion in an open system with slow dissolution rate controlled by the end-group length, whereas gels showing single-phase behavior exhibit bulk erosion that is relatively fast.
\r\n\r\nAqueous solutions of Rf-PEGs exhibit ordering transitions, with increasing concentration (Chapter 3). The hydrophobic cores of the micelle-like aggregates order into a body-centered-cubic (BCC) structure. The aggregated state of the hydrophobic core is determined by the length of the hydrophobic end group, and is insensitive to the concentration of the polymer solution or the temperature. A shorter PEG length for a given end group produces a much enhanced ordering compared to a longer one. This micelle packing effect is manifested in changes in the viscoelastic properties: the single-relaxation behavior evolves to the appearance of a new low frequency elastic plateau in the dynamic moduli, and a linear response changes to a yielding behavior in creep.
\r\n\t\r\nThe gel phase of sol-gel coexisting polymers can be transformed into an injectable state by the addition of a bio-tolerable organic solvent, such as N-methyl pyrrolidone (NMP), and this solution can be restored to a hydrogel state quickly after injection by removal of the organic solvent by diffusion. Release of Human growth hormone (hGH) using this injectable formulation (Chapter 4) reveals that hGH remains stable inside the hydrogel formed, and more than 2 weeks of prolonged release of hGH pretreated with zinc is obtained using the injectable formulation without irreversible aggregation. For the Rf-PEGs examined here, the release rate of hGH is determined by the rate of diffusion through the hydrogel.
\r\n\r\nThe telechelic Rf-PEGs that exhibit sol-gel equilibrium or precipitated gel phase behavior provide a facile route to hydrophilic modification of poly(tetrafluoroethylene) (PTFE) surfaces that are frequently encountered in biomedical devices (Chapter 5). Dip coating of PTFE into 1 wt % Rf-PEGs in ethanol, followed by immersing into water, converts the surface of PTFE from hydrophobic to hydrophilic. The lifetime of this modification is correlated to the phase behavior of the bulk gel state, and stable in the various ranges of shear rates. An Rf-PEG that is insoluble in water gave a stable modification over a period of weeks in the absence of shear, and persisted for days when subjected to the highest shear stresses encountered in arteries (3-4Pa). Telechelic Rf-PEGs are effective, while monofunctional PEGs with a single fluoroalkyl group are not.
\r\n\r\nThe swelling and drying behaviors of thin films of RfPEGs (~0.1 [mu]m) show abnormalities relative to glassy and semi-crystalline films (Chapter 6). In a humidity ramp test starting from a dry state, thin films of Rf-PEGs show a distinctive hysteresis behavior; as humidity increases, little swelling occurs until ~ 85% humidity, then the film swells rapidly; as the humidity decreases, a rapid deswelling occurs near ~75% humidity. In a humidity step test, following a step-up the mass increase shows an overshoot, followed by a gradual approach to the equilibrium value, whereas the film tracks the equilibrium state very rapidly and monotonically following a step down from high to low humidity.
", "date": "2002", "date_type": "degree", "id_number": "CaltechETD:etd-07192007-103729", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-07192007-103729", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2007-07-20", "doi": "10.7907/xrnv-yh71", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "advisor" }, { "id": "Hubbell-J-A", "name": { "family": "Hubbell", "given": "Jeffrey A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "chair" }, { "id": "Davis-M-E", "name": { "family": "Davis", "given": "Mark E." }, "orcid": "0000-0001-8294-1477", "role": "member" }, { "id": "Hubbell-J-A", "name": { "family": "Hubbell", "given": "Jeffrey A." }, "role": "member" }, { "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "orcid": "0000-0002-3361-6114", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2007-07-19", "thesis_defense_date": "2001-11-12", "thesis_approved_date": "2007-07-20", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2002", "author_list": "Tae, Giyoong", "advisor_list": "Kornfield, Julia A. and Hubbell, Jeffrey A.", "comittee_list": "Kornfield, Julia A.; Davis, Mark E.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/3274", "eprint_id": 3274, "rev_number": 14, "documents": [ { "id": "/id/document/5777", "doc_id": 5777, "rev_number": 4, "files": [ { "id": "/id/file/34245", "fileid": 34245, "datasetid": "document", "objectid": 5777, "filename": "Zhou_w_2001.pdf", "mime_type": "application/pdf", "filesize": 7877319, "mtime": "2012-12-26 02:58:39", "url": "/3274/1/Zhou_w_2001.pdf" } ], "eprint_id": 3274, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": "Zhou_w_2001.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/22318" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/22318" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/22318" } ] } }, { "id": "/id/document/22318", "doc_id": 22318, "rev_number": 3, "files": [ { "id": "/id/file/34243", "fileid": 34243, "datasetid": "document", "objectid": 22318, "filename": "preview.png", "mime_type": "image/png", "hash": "5c5ac1a7de0aa217b2b8f1954c8e37ec", "hash_type": "MD5", "filesize": 10042, "mtime": "2012-12-26 02:58:39", "url": "/3274/2/preview.png" } ], "eprint_id": 3274, "pos": 2, "placement": 2, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "public", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/5777" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/5777" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/5777" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/32/74", "datestamp": "2008-08-29", "lastmod": "2022-11-30 00:37:24", "status_changed": "2009-09-25 02:55:39", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Zhou-Weijun", "name": { "family": "Zhou", "given": "Weijun" }, "show_email": "NO" } ] }, "title": "Dynamics and Shear Alignment Behavior of a Model Thermotropic Liquid Crystalline Polymer", "ispublished": "unpub", "full_text_status": "public", "keywords": "Chemical Engineering", "abstract": "Although liquid crystalline polymers (LCPs) emerged as important engineering materials in the early 1970s, the current level of understanding still falls short of allowing deliberate manipulation of macroscopic orientation, leading to poor control of morphology and material properties. The flow behavior of rod-like LCP solutions (lyotropic) are fairly well understood, yet little progress has been made on LCP melts (thermotropic) because of the formidable experimental difficulties with commercial thermotropes. A simple extension of the knowledge obtained from rod-like LCP solutions to thermotropic LCPs is unlikely to hold due to the enhanced molecular flexibility and intimate molecular contact in LCP melts.
\r\n\r\nThe primary concern of this thesis is therefore the flow behavior of thermotropic LCPs, with an emphasis on how flow influences orientation and morphology and how this depends on molecular structure. For this purpose we synthesized a model thermotropic LCP selected for its chemical stability, wide nematic range and optical transparency. This main-chain LCP, designated as DHMS-7,9, has alternating mesogen and spacer structure with dihydroxy-[alpha]-methylstilbene as mesogen and two different lengths of alkyl spacers (-C\u2087H\u2081\u2084- and -C\u2089H\u2081\u2088-). A range of molecular weights were prepared to probe the effects of chain flexibility (ratio of chain length of persistence length). Synthesis was scaled up to provide adequate quantities for physical studies (rheology, rheo-conoscopy and rheo-WAXS).
\r\n\r\nThe director response of a monodomain during shear flow is followed by in situ optical conoscopy using a custom-made shear cell. We observe that the director rotates opposite to the vorticity in shear for DHMS-7,9 using planar monodomain samples, demonstrating conclusively that it is flow aligning throughout its nematic temperature range. Director rotation is solely a function of applied strain, independent of shear rate, showing that the Leslie-Ericksen theory is applicable to polymeric nematics for shear rates that are low relative to their molecular relaxation. Comparisons of the observed tumbling parameter of DHMS-7,9 with predictions from available molecular models lead us to infer that molecular flexibility produces shear alignment for this class of thermotropic LCPs. To identify the effect of chain flexibility on the dynamics of this LCP, the rotational viscosity and shear viscosity were measured as functions of molecular weight. Both viscosities showed weaker sensitivity to molecular weight above a characteristic molecular weight, suggesting a crossover to semiflexible character at high molecular weight.
\r\n\r\nRheology and shear orientation behavior of DHMS-7,9 are markedly different from that of nematic lyotropic LCPs. Synchrotron WAXS measurements in steady shear show that molecular orientation is relatively high and nearly independent of shear rate. In transient shear during flow inception, flow reversal, and step up/down shear rate, neither shear stress nor orientation parameter shows multiple oscillations. Thus, both steady and transient responses of DHMS-7,9 are characteristic of flow-aligning liquid crystals, in contrast to tumbling rod-like LCPs, which show complex shear rate dependence in steady shear and oscillatory response to these transient flows.
\r\n\r\nAn interesting feature of DHMS-7,9 is the existence of a mysterious liquid crystalline phase--Phase X. The flow behavior of Phase X is completely different from that of the nematic phase. A striking flip of the orientation from the flow direction to the vorticity direction occurs below a critical shear rate. This orientational flipping is reversible in response to step changes of temperature and/or shear rate. In addition, we found that oscillatory shear flow also induces a similar type of orientational flipping. Examination of the linear viscoelastic properties as a function of orientation in Phase X suggests rheological similarity to layered fluids.
", "date": "2001", "date_type": "degree", "id_number": "CaltechETD:etd-08292008-110129", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-08292008-110129", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-08-29", "doi": "10.7907/dv2d-w145", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "advisor" } ] }, "thesis_committee": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "chair" }, { "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "orcid": "0000-0003-3175-4596", "role": "member" }, { "id": "Gavalas-G-R", "name": { "family": "Gavalas", "given": "George R." }, "orcid": "0000-0003-1468-6835", "role": "member" }, { "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "orcid": "0000-0002-3361-6114", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-08-29", "thesis_defense_date": "2000-09-29", "thesis_approved_date": "2008-08-29", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2001", "author_list": "Zhou, Weijun", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Tirrell, David A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/3783", "eprint_id": 3783, "rev_number": 10, "documents": [ { "id": "/id/document/6421", "doc_id": 6421, "rev_number": 3, "files": [ { "id": "/id/file/38535", "fileid": 38535, "datasetid": "document", "objectid": 6421, "filename": "Kumaraswamy_g_2000.pdf", "mime_type": "application/pdf", "filesize": 10060303, "mtime": "2012-12-26 03:02:57", "url": "/3783/1/Kumaraswamy_g_2000.pdf" } ], "eprint_id": 3783, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Kumaraswamy_g_2000.pdf", "language": "en", "security": "public", "license": "other", "main": "Kumaraswamy_g_2000.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/22953" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/22953" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/22953" } ] } }, { "id": "/id/document/11895", "doc_id": 11895, "rev_number": 3, "files": [ { "id": "/id/file/204177", "fileid": 204177, "datasetid": "document", "objectid": 11895, "filename": "Kumaraswamy_Permission.txt", "mime_type": "text/plain", "filesize": 1829, "mtime": "2016-08-22 21:16:58", "url": "/3783/2/Kumaraswamy_Permission.txt" } ], "eprint_id": 3783, "pos": 2, "format": "text/plain", "format_desc": "Author OK 2011", "language": "en", "security": "internal", "license": "other", "main": "Kumaraswamy_Permission.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "release" }, { "id": "/id/document/22953", "doc_id": 22953, "rev_number": 2, "files": [ { "id": "/id/file/38533", "fileid": 38533, "datasetid": "document", "objectid": 22953, "filename": "preview.png", "mime_type": "image/png", "hash": "d33c46af925caaf2faeed7f2f07bf064", "hash_type": "MD5", "filesize": 10847, "mtime": "2012-12-26 03:02:57", "url": "/3783/3/preview.png" } ], "eprint_id": 3783, "pos": 3, "placement": 3, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "public", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/6421" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/6421" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/6421" } ] } }, { "id": "/id/document/123845", "doc_id": 123845, "rev_number": 1, "files": [ { "id": "/id/file/369273", "fileid": 369273, "datasetid": "document", "objectid": 123845, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "524c24c81175b6b8722ee7e7cd5a81a0", "hash_type": "MD5", "filesize": 948, "mtime": "2021-06-23 23:02:03", "url": "/3783/4/indexcodes.txt" } ], "eprint_id": 3783, "pos": 4, "placement": 4, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from text/plain to indexcodes", "language": "en", "security": "internal", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/11895" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/11895" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/11895" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/37/83", "datestamp": "2005-09-26", "lastmod": "2019-12-20 19:49:12", "status_changed": "2009-09-25 03:05:51", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Kumaraswamy-G", "name": { "family": "Kumaraswamy", "given": "Guruswamy" }, "show_email": "NO" } ] }, "title": "The effect of flow history on the crystallization of semicrystalline polymers", "ispublished": "unpub", "full_text_status": "public", "keywords": "Chemical Engineering", "abstract": "Semicrystalline polymers constitute well over half of all the polymers produced worldwide. Their material properties depend sensitively on the thermal and flow history experienced during processing which strongly influences the kinetics of phase change and the morphology of the final crystalline microstructure. Therefore, it is of considerable interest to understand the mechanisms of flow effects on the rate and geometry of nucleation and crystal growth.\r\n\r\nMicrostructural development under the influence of flow is controlled by the interplay between melt relaxation processes and crystallization processes: the thermodynamic and kinetic aspects give rise to rich physics that are not well understood. This thesis elucidates key fundamentals of this process. We develop novel instrumentation that improves over prior approaches by examining the development of order at all the length scales of interest (in-situ rheo-optics, synchrotron small angle X-ray scattering (SAXS), and wide angle X-ray diffraction (WAXD), and ex-situ electron and optical microscopy); and by reducing the sample requirement by about three orders of magnitude, opening the way to study of model materials. We investigate a polydisperse, commercial Ziegler-Natta isotactic polypropylene (iPP) using the short term shearing protocol pioneered by the group of Janeschitz-Kriegl which imposes a well defined thermal and flow history on the polymer.\r\n\r\nRheo-optical investigations reveal that imposition of brief intervals of shear (less than a thousandth of the quiescent crystallization time) reduces the crystallization time by two orders of magnitude at a crystallization temperature of 141\u00b0C. Above a critical value of the shear stress, there is a transition to highly oriented growth with increase in shearing duration. This transition is correlated with changes in the transient behavior during flow and the semicrystalline morphology observed exsitu. During flow, we observe the generation of long-lived, highly oriented structures (evident in the transient birefringence) under all conditions that induce subsequent growth of highly oriented crystallites. In turn, the development of oriented crystallites observed in-situ after cessation of flow correlates with development of a \"skin-core\" morphology observed ex-situ.\r\n\r\nThe transient structures that develop during flow are identified as oriented [alpha]-phase crystals by WAXD, and show an unexpected temperature dependence for their time of formation: with increase in temperature, they occur at shorter times after startup of flow. This very unusual temperature dependence is strikingly similar to that for rheological processes, and is in contrast to the exponential increase expected for crystallization time-scales. Thus, the transition to anisotropic nucleation in polymers subjected to flow follows a non-classical kinetic pathway controlled by the formation of a transient, highly oriented metastable melt state.\r\n\r\nIn-situ synchrotron SAXS and WAXD reveal that for shearing conditions that lead to anisotropic morphologies, crystals that are highly oriented in the flow direction develop during shear, templating the formation of crystallites after flow cessation. In the densely nucleated skin regions, ex-situ TEM shows lamellae growing radially from oriented central \"shish\" structures until they impinge to form the \"shish-kebab\" or row-nucleated structures. Under milder shear conditions, the rate of crystallization is gradual compared to strong shearing, and less oriented morphologies develop. Interestingly the ratio of parent to the crosshatched, epitaxial daughter lamellae for the oriented crystallites increases with increase in shearing time, imposed wall shear stress and temperature.\r\n\r\nOur data suggests a mechanistic model for shear-enhanced crystallization: the rheologically-controlled formation of a critical anisotropic distribution of chain segments in the melt upon imposition of flow nucleates oriented crystallites. For intense shearing conditions, these line-nuclei are long and dense. Row nucleated structures develop from these line nuclei as lamellae grow radially to form fully impinged structures. For milder shearing conditions, lower nucleation densities lead to the development of less oriented structures.\r\n", "date": "2000", "date_type": "degree", "id_number": "CaltechETD:etd-09262005-074935", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-09262005-074935", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Julie Guan", "deposited_by": "Imported from ETD-db", "deposited_on": "2005-09-26", "doi": "10.7907/8SJ5-HM09", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "email": "bercaw@caltech.edu", "id": "Bercaw-J-E", "name": { "family": "Bercaw", "given": "John E." }, "role": "member" }, { "email": "rhg@its.caltech.edu", "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "role": "member" }, { "email": "zgw@cheme.caltech.edu", "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2005-09-26", "thesis_defense_date": "2000-03-01", "thesis_approved_date": "2005-09-26", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2000", "author_list": "Kumaraswamy, Guruswamy", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Bercaw, John E.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/325", "eprint_id": 325, "rev_number": 21, "documents": [ { "id": "/id/document/484", "doc_id": 484, "rev_number": 5, "files": [ { "id": "/id/file/3091", "fileid": 3091, "datasetid": "document", "objectid": 484, "filename": "Chen_zr_1998.pdf", "mime_type": "application/pdf", "filesize": 29462132, "mtime": "2012-12-26 02:28:55", "url": "/325/1/Chen_zr_1998.pdf" } ], "eprint_id": 325, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Original scanned version. 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"media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/94717" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/94717" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/94717" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/03/25", "datestamp": "2008-02-15", "lastmod": "2023-08-08 22:15:58", "status_changed": "2009-09-25 01:34:28", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Chen-Zhong-Ren", "name": { "family": "Chen", "given": "Zhong-Ren" }, "orcid": "0000-0002-2929-9566", "show_email": "NO" } ] }, "title": "I. Dynamics of Block Copolymer Nanostructures. II. Polymerizability of Cyclic Olefins and Ring-Closing Metathesis", "ispublished": "unpub", "full_text_status": "public", "keywords": "(Chemical Engineering and Chemistry)", "abstract": "Self-assembly of block copolymers provide versatile means to create nanostructures with potential applications in nanotechnologies. The form and size of these structures are controlled by the type and the length of each block, and the number of blocks. Active processing using symmetry-breaking fields such as flow can extend self-assembled order into the macroscopic dimensions, thus gain desired directional properties, such as transport, optical, and electrical properties.
\r\n\r\nTowards the integrated synthesis and processing of functional block copolymer nanostructures, dynamics and thermodynamics of block copolymer nanostructures must be understood. The dynamics of flow-induced alignment of block copolymers will provide the basis to predict the direction, rate, and degree of alignment, while defect dynamics and thermodynamics will give insight into the possibilities of formation of desired nanostructures. In chapter 1, I will overview key issues of flow-induced alignment based on literature and new results from the first two chapters of the thesis. A three-dimensional mapping summarizes the flow behavior of diblock copolymers in terms of molecular characteristics and processing conditions. Various mechanisms that had been proposed since two decades ago are reviewed and re-evaluated.
\r\n\r\nIn chapter 2, I will present detailed results revealed by a powerful experimental method, which combines in-situ rheo-optical measurements and ex-situ structural characterization by electron microscopy and x-ray scattering. A PS-PI (10K-10K) diblock is used as a model system. Three different trajectories of alignment are investigated: perpendicular alignment and two qualitatively different routes to parallel alignment. At the highest frequencies, symmetry arguments explain the transient development of a bimodal texture en route to alignment of layers parallel to the planes of shear. At lower frequencies, larger scale relaxations introduce rearrangements out of the deformation plane that permit formation of lamellae perpendicular to the shear plane. These explain the change in character of the pathway to parallel alignment and the emergence of perpendicular alignment with decreasing frequency. For each trajectory in general, the initial 'fast' process enhances not only the projection of the orientation distribution that corresponds to the final state, but also increases other projections of the distribution; the late-stage 'slow' process eliminates these other projections and perfects a single alignment.
\r\n\r\nABC triblock copolymer can form a fascinating array of nanostructures. Phase behavior, dynamics of oscillatory-shear alignment, and other issues raised by ABC triblock copolymers, such as dynamics of lamellar perforation in three-nanophase-separated states will be discussed in chapter 3. Both thermotropical and shear-induced phase transitions are observed. Dramatic changes of morphology and alignment behavior are induced simply by switching the permutation of the blocks, molecular size, shear condition, and temperature. In three-nanophase-separated lamellar materials, a new type of defect is found: correlated perforation. As these defects annihilate upon annealing, long range correlations produce striking patterns, including those that resemble a ship's wake. The creation and evolution of these defect structures present challenge and opportunities in developing novel nanostructures.
\r\n\r\nOlefin metathesis by transition metal complex has been a powerful method in polymer and organic synthesis. In chapter 4, I will present a model to predict the ring-chain equilibria in ring-opening-closing reaction. Statistical mechanics and molecular mechanics provide the basic tools in problem formulation and parameter determination. Polymerizability of cyclic olefins are predicted by this model, and agree well with ring-opening metathesis polymerization experiments. We have extended this model to assist ring-closing metathesis of eight-member rings, which can be a useful starting material for drug synthesis.
", "date": "1998", "date_type": "degree", "id_number": "CaltechETD:etd-01242008-095827", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-01242008-095827", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-02-15", "doi": "10.7907/xd1r-aj40", "alt_title": { "items": [ "Dynamics of Block Copolymer Nanostructures", "Polymerizability of Cyclic Olefins and Ring-Closing Metathesis" ] }, "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "advisor" }, { "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "orcid": "0000-0002-0057-7817", "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "orcid": "0000-0001-6746-8634", "role": "chair" }, { "id": "Grubbs-R-H", "name": { "family": "Grubbs", "given": "Robert H." }, "orcid": "0000-0002-0057-7817", "role": "member" }, { "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "orcid": "0000-0002-3361-6114", "role": "member" }, { "id": "Ko-Chan-U", "name": { "family": "Ko", "given": "Chan U." }, "role": "member" }, { "id": "Doi-Masao", "name": { "family": "Doi", "given": "Masao" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-01-24", "thesis_defense_date": "1997-12-09", "thesis_approved_date": "2008-02-15", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "option_minor": { "items": [ "chemistry" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "1998", "author_list": "Chen, Zhong-Ren", "advisor_list": "Kornfield, Julia A. and Grubbs, Robert H.", "comittee_list": "Kornfield, Julia A.; Grubbs, Robert H.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/4988", "eprint_id": 4988, "rev_number": 9, "documents": [ { "id": "/id/document/7910", "doc_id": 7910, "rev_number": 3, "files": [ { "id": "/id/file/48661", "fileid": 48661, "datasetid": "document", "objectid": 7910, "filename": "Gupta_vk_1996.pdf", "mime_type": "application/pdf", "filesize": 8373125, "mtime": "2012-12-26 03:13:33", "url": "/4988/1/Gupta_vk_1996.pdf" } ], "eprint_id": 4988, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Gupta_vk_1996.pdf", "language": "en", "security": "public", "license": "other", "main": "Gupta_vk_1996.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/24420" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/24420" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/24420" } ] } }, { "id": "/id/document/24420", "doc_id": 24420, "rev_number": 3, "files": [ { "id": "/id/file/48659", "fileid": 48659, "datasetid": "document", "objectid": 24420, "filename": "preview.png", "mime_type": "image/png", "hash": "a209d37e75b91b31ce4778af783d56ef", "hash_type": "MD5", "filesize": 13340, "mtime": "2012-12-26 03:13:32", "url": "/4988/2/preview.png" } ], "eprint_id": 4988, "pos": 2, "placement": 2, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "public", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/7910" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/7910" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/7910" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/49/88", "datestamp": "2007-12-14", "lastmod": "2021-04-19 22:29:55", "status_changed": "2009-09-25 03:30:20", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Gupta-V-K", "name": { "family": "Gupta", "given": "Vinay Kumar" }, "show_email": "NO" } ] }, "title": "Controlling molecular and microstructural alignment in anisotropic polymer systems", "ispublished": "unpub", "full_text_status": "public", "abstract": "Molecular and microstructural orientation plays a key role in determining the useful mechanical, optical and electrical properties of a large class of polymeric materials. Realization of the technological promise of these materials requires rational control of the microstructure and understanding of the processing-structure-property relationships. Towards this end, we focus on the material properties and dynamical processes that affect molecular order of two complex polymeric systems (a) Ultra-thin Langmuir-Blodgett films of a hairy-rodlike polymer, and (b) Lamellar diblock copolymer melts of polystyrene and polyisoprene (PS-PI).\n\nWe accomplish our objective by improving and tying together existing analytic techniques into instruments extremely effective for measuring molecular orientation and order. For fundamental insights into the nature of alignment in ultra-thin (~ few nanometers thick) LB films, we integrate laser scanning microscopy (LSM) with polarization-modulation (PM) polarimetry. PM-LSM possesses high spatial resolution, sensitivity and speed, and allows us to image the anisotropy in films as thin as two molecular layers. To monitor the dynamics of flow alignment in diblock copolymers, in situ and in real time, we combine polarization-modulation polarimetry with rheometry. This rheo-optical technique enables us to monitor the evolution of microstructure by measuring the optical anisotropy, and correlate it with changes in macroscopic mechanical observables, such as stress and strain.\n\nUsing PM-LSM we have investigated the interplay of molecular weight, layer thickness and thermal annealing in controlling molecular order in rodlike polymer LB films. Upon investigating two different molecular weights of the polymer, we find lowering of molecular order in deposited films with increase in molecular weight. Furthermore, thermal annealing improves alignment only for films of shorter rodlike polymers (~ lower molecular weight). We believe that the underlying cause for these results is a difference in the structure of the deposited films for the longer polymer because of the relative changes in timescales for the macromolecular relaxation and the monolayer deformation during deposition. We also find that for both molecular weights, the substrate exerts an anchoring effect on the first two layers adjacent to it and suppresses improvement in alignment on annealing. This inability to improve alignment has important consequences for applications such as molecular electronics where monolayers or bilayers having a high degree of orientation are required.\n\nIn-situ measurement of flow birefringence during oscillatory shear alignment, clarifies the evolution of the lamellar orientation distribution for a diblock copolymer melt. Shearing results in \"parallel\" or \"perpendicular\" alignment i. e. layers normal to either the velocity gradient or the vorticity axis, respectively (Figure 1.1). Both states of alignment occur via an initial \"fast\" process followed by a \"slow\" one. The fast process is dominated by the depletion of the projection of the orientation distribution along either the perpendicular direction or the \"transverse\" direction (layers normal to the flow). This resulting biaxial distribution is then transformed into a well-aligned uniaxial one during the slow process. Surprisingly, at particular frequencies, the projection along the perpendicular direction can disappear faster than the projection along the transverse direction. In both the fast and the slow processes the time evolution of birefringence follows a highly non-linear scaling with strain; the scaling being different for the fast and slow processes. A systematic study of the effects of strain on shear alignment in block copolymers led to the discovery that strain affects not only the dynamics of alignment, but also the direction. This phenomenon expands the range of parameters that can be used to flip the direction of alignment. In relation to previous studies that examined the regimes of alignment only in terms of temperature and frequency, this phenomenon necessitates consideration of a third dimension - strain.", "date": "1996", "date_type": "degree", "id_number": "CaltechETD:etd-12132007-085351", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-12132007-085351", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2007-12-14", "doi": "10.7907/xb3f-3a10", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "id": "Gavalas-G-R", "name": { "family": "Gavalas", "given": "George R." }, "role": "member" }, { "id": "Brady-J-F", "name": { "family": "Brady", "given": "John F." }, "role": "member" }, { "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2007-12-13", "thesis_defense_date": "1995-06-01", "thesis_approved_date": "2007-12-14", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "1996", "author_list": "Gupta, Vinay Kumar", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Gavalas, George R.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/3319", "eprint_id": 3319, "rev_number": 10, "documents": [ { "id": "/id/document/5839", "doc_id": 5839, "rev_number": 3, "files": [ { "id": "/id/file/34640", "fileid": 34640, "datasetid": "document", "objectid": 5839, "filename": "Wang_bh_1996.pdf", "mime_type": "application/pdf", "filesize": 6378516, "mtime": "2012-12-26 02:59:03", "url": "/3319/1/Wang_bh_1996.pdf" } ], "eprint_id": 3319, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Wang_bh_1996.pdf", "language": "en", "security": "public", "license": "other", "main": "Wang_bh_1996.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/22380" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/22380" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/22380" } ] } }, { "id": "/id/document/22380", "doc_id": 22380, "rev_number": 3, "files": [ { "id": "/id/file/34638", "fileid": 34638, "datasetid": "document", "objectid": 22380, "filename": "preview.png", "mime_type": "image/png", "hash": "53b1e2e52a8b9126c2d63f9aed8d4a3a", "hash_type": "MD5", "filesize": 11120, "mtime": "2012-12-26 02:59:03", "url": "/3319/2/preview.png" } ], "eprint_id": 3319, "pos": 2, "placement": 2, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "public", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/5839" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/5839" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/5839" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/33/19", "datestamp": "2008-09-03", "lastmod": "2021-04-16 23:06:47", "status_changed": "2009-09-25 02:56:42", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Wang-B-H", "name": { "family": "Wang", "given": "Barbara Helen" }, "show_email": "NO" } ] }, "title": "Rheo-optical investigation of the dynamics of miscible polymers: blends and diblock copolymers", "ispublished": "unpub", "full_text_status": "public", "abstract": "The dynamics of each component in miscible blends of polyisoprene / polyvinylethylene (PIP/PVE) are studied using dynamic stress-optical measurements. We first examine blends in which the two components are nearly equally entangled in order to avoid the effects of polydispersity on the dynamic moduli of each species. While the homopolymers are thermorheologically simple and obey the stress-optic rule, the blends show failure of time-temperature superposition and complex stress-optic behavior. The way in which the stress-optic rule fails reveals the relaxation dynamics of each species. The blend dynamic modulus and complex birefringence coefficient are analyzed to infer the dynamics of each component. Orientational coupling, which affects the birefringence but not the stress, is incorporated based on the value of the coupling coefficient determined from rheo-optical studies of unequally entangled blends. While we cannot rule out contributions of compositional heterogeneity to thermorheological complexity in the PIP/PVE system, it is intrinsic differences between the temperature dependencies of the two species' dynamics which dominate the observed failure of time-temperature superposition.\n\nThe entanglement molecular weight, M[subscript e,i](\u03c6), and monomeric friction coefficient,\u03b6[subscript o,i](\u03c6,T), of each species are determined from the component dynamic moduli, as functions of blend composition, \u03c6 and temperature, T. The effect of blending on M[subscript e,i] of each component is small, with the values varying by only ~ 30% from those of the pure components over the range of composition. Blending has a much more dramatic effect on \u03b6[subscript o,i] of each species: it strongly speeds the rate of relaxation of the component with the higher glass transition temperature, T[subscript g], (PVE), while more modestly slowing the relaxation of the low-T[subscript g] component (PIP). The dynamics of each species have different temperature dependencies in the blend, which leads to the failure of the superposition principle. Furthermore, both the difference between the friction coefficients of the two species and the difference in their temperature dependencies is greater in blends rich in the high-T[subscript g], material (PVE).\n\nWe then look at blends in which the two species are unequally entangled and the effect of orientational coupling can be characterized. Since orientational coupling contributes to the birefringence but not the stress, simultaneous analysis of these observables allows us to extract the coupling coefficient, \u03b5. For blends in which PIP is the faster-relaxing species and couples to a slower-relaxing PVE matrix, \u03b5[subscript PIP,PVE] \u2248 0.35 \u00b1 0.04. Analogous blends are also studied, where PVE is the faster-relaxing species coupling to a PIP matrix, for which \u03b5[subscript PVE,PIP] \u2248 0.27 \u00b1 0.08. Thus, within experimental uncertainty, it appears appropriate to use a single, average value of \u03b5. No dependence of \u03b5 on composition or temperature were detected. Once \u03b5 was determined we extracted the component dynamic moduli in each blend over a range of temperatures and blend compositions. The trends observed for the equally entangled blends remain valid and the values determined for M[subscript e,i] and \u03b6[subscript o,i](\u03c6,T) are reproduced. Although failure of time-temperature superposition in these blends is again due to the distinct temperature dependencies of the species' monomeric friction coefficients, both the contrast in friction coefficient and the relative molecular weights of the components determine the degree to which complex thermorheological behavior is observed.\n\nFinally, the dynamics of nearly ideal, disordered PIP-PVE diblock copolymer melts are characterized using the same rheo-optical techniques, for two block compositions (\u03c6[subscript PIP] = 0.25 and 0.75). Unlike miscible blends of PIP and PVE, for which time-temperature superposition fails, the dynamic moduli of the block copolymers suggest that they are thermorheologically simple. Here we show that this apparent paradox can be resolved by examining the relaxation of the constituent blocks, which can be determined from stress-optic measurements. In block copolymers rich in the low-T[subscript g] component (high \u03c6[subscript PIP]), thermorheologically simple behavior is observed because both blocks have similar friction coefficients, in accord with our results on PIP/PVE blends. In copolymers rich in the high-T[subscript g] component (low \u03c6[supscript PIP]), the individual blocks show distinct temperature dependencies, again in accord with the blend results. The reason that departure from time-temperature superposition was not previously observed in these diblocks is that the change in \u03b6[subscript o],PVE/\u03b6[subscript o],PIP produces subtle changes in the overall relaxation spectrum relative to a linear chain of uniform friction.\n", "date": "1996", "date_type": "degree", "id_number": "CaltechETD:etd-09032008-074923", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-09032008-074923", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-09-03", "doi": "10.7907/3t4r-ym20", "divisions": { "items": [ "div_pma" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "name": { "family": "Unknown", "given": "Unknown" } } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-09-03", "thesis_defense_date": "1995-12-20", "thesis_approved_date": "2008-09-03", "review_status": "approved", "option_major": { "items": [ "physics" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "1996", "author_list": "Wang, Barbara Helen", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Unknown, Unknown" }, { "id": "https://thesis.library.caltech.edu/id/eprint/15", "eprint_id": 15, "rev_number": 10, "documents": [ { "id": "/id/document/55", "doc_id": 55, "rev_number": 3, "files": [ { "id": "/id/file/266", "fileid": 266, "datasetid": "document", "objectid": 55, "filename": "Rubin_sf_1996.pdf", "mime_type": "application/pdf", "filesize": 12348211, "mtime": "2012-12-26 02:26:48", "url": "/15/1/Rubin_sf_1996.pdf" } ], "eprint_id": 15, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Rubin_sf_1996.pdf", "language": "en", "security": "public", "license": "other", "main": "Rubin_sf_1996.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/16883" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/16883" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/16883" } ] } }, { "id": "/id/document/16883", "doc_id": 16883, "rev_number": 3, "files": [ { "id": "/id/file/264", "fileid": 264, "datasetid": "document", "objectid": 16883, "filename": "preview.png", "mime_type": "image/png", "hash": "9b45d09d35344187643c26cef1e3c5e7", "hash_type": "MD5", "filesize": 13505, "mtime": "2012-12-26 02:26:48", "url": "/15/2/preview.png" } ], "eprint_id": 15, "pos": 2, "placement": 2, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "public", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/55" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/55" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/55" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/00/15", "datestamp": "2008-01-10", "lastmod": "2021-04-16 22:33:09", "status_changed": "2009-09-25 01:26:29", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Rubin-S-F", "name": { "family": "Rubin", "given": "Susan Felicia" }, "show_email": "NO" } ] }, "title": "Viscoelasticity and dynamics of alignment in side-group liquid crystalline polymers", "ispublished": "unpub", "full_text_status": "public", "keywords": "liquid crystalline polymers", "abstract": "NOTE: Text or symbols not renderable in plain ASCII are indicated by [...]. Abstract is included in .pdf document.\r\n\r\nSide-group liquid-crystalline polymers (SG-LCPs) consist of a flexible polymeric backbone and rigid mesogens (molecules forming LC phases), attached laterally to the backbone via flexible spacers. Since the dynamics of the mesogen field and polymeric backbone are partially decoupled, uniformly-aligned SG-LCP materials show promise in a variety of applications such as non-linear optical materials, optical data storage media, and stress sensors, which require switching of the mesogen orientation. Recent work has shown that uniform alignment of SG-LCP materials can be accomplished using flow-fields. However, the mechanisms of alignment, which are essential for the development of effective and rational processing strategies for the SG-LCP materials, remain poorly understood. To address this need, we focus on the viscoelastic properties of nematic and smectic SG-LCPs and the dynamics of field-induced alignment of SG-LCPs.\r\n\r\nWe have investigated the dynamic mechanical response of SG-LCPs having methacrylate backbone, hexamethylene spacer, and phenyl benzoate mesogens as a function of molecular weight in the isotropic, nematic, and smectic phases [...], and have discovered a unique molecular-weight dependence of the sensitivity of the dynamic modulus to nematic order of the melt. Nematic order produced a profound change in the dynamics of the entangled SG-LPCs relative to the isotropic phase; however, this effect was absent in the unentangled SG-LCPs. In SGLCPs with smectic order, there was increase in the elastic character of the fluid with smectic ordering, but the incremental effect in a system that was entangled was relatively small. Oscillatory shear with large amplitude [...] induced macroscopic alignment in the nematic phase for all the SG-LCPs studied and could be used to alter the microstructure in the smectic liquid. Shearing the smectic phase produced a decrease in modulus, whereas shearing in the nematic phase followed by cooling into the smectic phase produced an increase in modulus.\r\n\r\nTo assess the effect of the coupling between the mesogen and the backbone on field- induced orientation of nematic SG-LCPs, we have compared magnetically aligned and flow-aligned nematic SG-LCPs. Magnetic forces act primarily on the mesogens, and the backbone conformation changes to accommodate the torques on its pendant mesogens. In contrast, oscillatory shear can couple to the relaxation modes of both the director field and backbone. We have discovered that while the flow-aligned material exhibits distinct low-frequency relaxation dynamics, the relaxation of magnetically- aligned monodomains is indistinguishable from that of polydomain nematic melts. This suggests that flow alignment and magnetic alignment produce qualitatively distinct changes in the fluid miscostructure. We have further compared the processes of shear- and magnetic-alignment by monitoring the evolution of director orientation in nematic SG-LCP melts, in-situ, through visible transmittance (related to the liquid-crystalline domain size) and visible birefringence (related to the molecular orientation).", "date": "1996", "date_type": "degree", "id_number": "CaltechETD:etd-01032008-082416", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-01032008-082416", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-01-10", "doi": "10.7907/bdjk-n270", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "id": "Gavalas-G-R", "name": { "family": "Gavalas", "given": "George R." }, "role": "member" }, { "id": "Hubbell-J-A", "name": { "family": "Hubbell", "given": "Jeffrey A." }, "role": "member" }, { "id": "Brady-J-F", "name": { "family": "Brady", "given": "John F." }, "role": "member" }, { "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-01-03", "thesis_defense_date": "1996-06-10", "thesis_approved_date": "2008-01-10", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "1996", "author_list": "Rubin, Susan Felicia", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Gavalas, George R.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/3630", "eprint_id": 3630, "rev_number": 9, "documents": [ { "id": "/id/document/6202", "doc_id": 6202, "rev_number": 3, "files": [ { "id": "/id/file/37157", "fileid": 37157, "datasetid": "document", "objectid": 6202, "filename": "Chung_gc_1995.pdf", "mime_type": "application/pdf", "filesize": 5476828, "mtime": "2012-12-26 03:01:29", "url": "/3630/1/Chung_gc_1995.pdf" } ], "eprint_id": 3630, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Chung_gc_1995.pdf", "language": "en", "security": "public", "license": "other", "main": "Chung_gc_1995.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/22740" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/22740" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/22740" } ] } }, { "id": "/id/document/22740", "doc_id": 22740, "rev_number": 3, "files": [ { "id": "/id/file/37155", "fileid": 37155, "datasetid": "document", "objectid": 22740, "filename": "preview.png", "mime_type": "image/png", "hash": "74e916d9a7cc7c500ec9d6b95ad9ff94", "hash_type": "MD5", "filesize": 10616, "mtime": "2012-12-26 03:01:29", "url": "/3630/2/preview.png" } ], "eprint_id": 3630, "pos": 2, "placement": 2, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "public", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/6202" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/6202" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/6202" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/36/30", "datestamp": "2007-10-17", "lastmod": "2021-04-16 22:16:40", "status_changed": "2009-09-25 03:01:56", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Chung-Geun-Chang", "name": { "family": "Chung", "given": "Geun-Chang" }, "show_email": "NO" } ] }, "title": "Segmental dynamics of individual species in a miscible polymer blend", "ispublished": "unpub", "full_text_status": "public", "abstract": "NOTE: Text or symbols not renderable in plain ASCII are indicated by [...]. Abstract is included in .pdf document.\r\n\r\nThe segmental motion of each species in polyisoprene/poly(vinylethylene) (PI/PVE) miscible blends is studied at three different compositions using two-dimensional deuteron exchange NMR. The individual species exhibit widely different mean mobilities and broad mobility distributions near the glass transition of each blend. As PVE content increases, both the difference in mean mobilities between the two species and the width of mobility distribution for both components increase. Such enhancement of these two types of dynamic heterogeneity with PVE content appears to produce the anomalous broadening of the glass transition. The mean reorientational correlation times of each component can differ by two orders of magnitude under identical conditions. The mean correlation times and the monomeric friction coefficients can be described by a common temperature dependence, which differs for individual species. This difference can be described in terms of distinct effective glass transition temperatures, [...], for the two species. The separation between the two effective glass transition temperatures increases with PVE content, consistent with more pronounced thermorheological complexity of blends rich in PVE. The individual [...] also exhibit different compositional dependence from that of the calorimetric [...] of blend. This behavior can give rise to the complex compositional dependence of individual mobilities, apparent when mobilities are compared at the same [...], with respect to the calorimetric [...] of blend. Origins of these two types of dynamic heterogeneity are examined further by using a simple model that takes into account effect of random compositional variations. Although compositional variations can give rise to the observed width of mobility distribution and its compositional dependence, the observed difference in mean mobilities cannot be explained at the same time. This suggests that the observed dynamic heterogeneities can be explained only by including two distinct contributions: local compositional variations in the blend and intrinsic difference in chain mobilities. Distinct dynamic constraints between the two species can arise from their structural differences. In light of phenomenological models of cooperative local dynamics, distinct mobilities can arise from the difference in critical size of free volume or in cooperativity.\r\n", "date": "1995", "date_type": "degree", "id_number": "CaltechETD:etd-09182007-103953", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-09182007-103953", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2007-10-17", "doi": "10.7907/dp5v-gt76", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "name": { "family": "Unknown", "given": "Unknown" } } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2007-09-18", "thesis_defense_date": "1994-06-01", "thesis_approved_date": "2007-10-17", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "1995", "author_list": "Chung, Geun-Chang", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Unknown, Unknown" }, { "id": "https://thesis.library.caltech.edu/id/eprint/4039", "eprint_id": 4039, "rev_number": 11, "documents": [ { "id": "/id/document/6713", "doc_id": 6713, "rev_number": 3, "files": [ { "id": "/id/file/40617", "fileid": 40617, "datasetid": "document", "objectid": 6713, "filename": "Kannan_r_1995.pdf", "mime_type": "application/pdf", "filesize": 7865566, "mtime": "2012-12-26 03:04:57", "url": "/4039/1/Kannan_r_1995.pdf" } ], "eprint_id": 4039, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Kannan_r_1995.pdf", "language": "en", "security": "public", "license": "other", "main": "Kannan_r_1995.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/23247" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/23247" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/23247" } ] } }, { "id": "/id/document/11712", "doc_id": 11712, "rev_number": 3, "files": [ { "id": "/id/file/204227", "fileid": 204227, "datasetid": "document", "objectid": 11712, "filename": "Kannan_Permission.txt", "mime_type": "text/plain", "filesize": 1502, "mtime": "2016-08-22 21:17:07", "url": "/4039/2/Kannan_Permission.txt" } ], "eprint_id": 4039, "pos": 2, "format": "text/plain", "format_desc": "Author OK 2010", "language": "en", "security": "internal", "license": "other", "main": "Kannan_Permission.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "release" }, { "id": "/id/document/23247", "doc_id": 23247, "rev_number": 2, "files": [ { "id": "/id/file/40615", "fileid": 40615, "datasetid": "document", "objectid": 23247, "filename": "preview.png", "mime_type": "image/png", "hash": "21aa65041a600e0802361a59d640366e", "hash_type": "MD5", "filesize": 11445, "mtime": "2012-12-26 03:04:57", "url": "/4039/3/preview.png" } ], "eprint_id": 4039, "pos": 3, "placement": 3, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "public", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/6713" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/6713" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/6713" } ] } }, { "id": "/id/document/123963", "doc_id": 123963, "rev_number": 1, "files": [ { "id": "/id/file/369392", "fileid": 369392, "datasetid": "document", "objectid": 123963, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "ddb08515c11099cb67ce30e1b3408dc3", "hash_type": "MD5", "filesize": 761, "mtime": "2021-06-23 23:10:54", "url": "/4039/4/indexcodes.txt" } ], "eprint_id": 4039, "pos": 4, "placement": 4, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from text/plain to indexcodes", "language": "en", "security": "internal", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/11712" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/11712" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/11712" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/40/39", "datestamp": "2007-10-12", "lastmod": "2019-12-21 01:26:24", "status_changed": "2009-09-25 03:10:27", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Kannan-R-M", "name": { "family": "Kannan", "given": "Rangaramanujam Mudumbai" }, "show_email": "NO" } ] }, "title": "Flow-induced alignment in intrinsically anisotropic polymeric materials", "ispublished": "unpub", "full_text_status": "public", "keywords": "Chemical Engineering", "abstract": "To understand the processing behavior of complex polymeric materials, it is imperative that we understand the distinct underlying molecular and microstructural contributions to macroscopic mechanical response. We have developed rheo-optical methods to isolate the dynamics at such length scales, by combining conventional mechanical testing with polarimetry. The rheology and flow-induced alignment in side-group liquid-crystalline polymers (SG-LCPs) and lamellar diblock copolymers (BCPs) have been investigated using the rheo-optical apparatus.\r\n\r\nThe rheology of SG-LCPs arises from a combination of the polymeric nature of the backbone, the ordering tendency of the mesogens, and the coupling between the two introduced by the spacer. Contrary to previous studies, we find that the nematic order can significantly affects the macroscopic viscoelastic response in SG-LCP melts. In the nematic state, we have discovered that oscillatory shear is effective in inducing macroscopic orientation of the sample. Shear flow may prove to be an economical, efficient way to obtain macroscopically aligned SGLCPs, which have potential as optical data storage media and nonlinear optical materials. In contrast to magnetic field induced alignment, the mechanism of shear induced alignment appears to bedriven by the distortion of the polymer backbone.\r\n\r\nWe study the mechanisms of flow-induced alignment in a poly(ethylenepropylene)-poly(ethylethylene) lamellar diblock copolymer, which produce macroscopic alignment with lamellae normal along the shear gradient direction ('parallel' alignment), or along the vorticity direction ('perpendicular' alignment). We accomplish this by monitoring the evolution of the microstructure and viscoelasticity in situ during the alignment process. Our results suggest that 'parallel' alignment occurs due to irreversible 'rocking' of grains which tends to align the grains along the shear direction, whereas 'perpendicular' alignment occurs at conditions where the microscale deformation is nearly homogeneous.", "date": "1995", "date_type": "degree", "id_number": "CaltechETD:etd-10112007-104204", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-10112007-104204", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Julie Guan", "deposited_by": "Imported from ETD-db", "deposited_on": "2007-10-12", "doi": "10.7907/ZDCX-2W89", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "chair" }, { "id": "Brady-J-F", "name": { "family": "Brady", "given": "John F." }, "role": "member" }, { "id": "Flagan-R-C", "name": { "family": "Flagan", "given": "Richard C." }, "role": "member" }, { "id": "Wang-Zhen-Gang", "name": { "family": "Wang", "given": "Zhen-Gang" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2007-10-11", "thesis_defense_date": "1994-05-13", "thesis_approved_date": "2007-10-12", "review_status": "approved", "option_major": { "items": [ "chemeng" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "1995", "author_list": "Kannan, Rangaramanujam Mudumbai", "advisor_list": "Kornfield, Julia A.", "comittee_list": "Kornfield, Julia A.; Brady, John F.; et el." } ]