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As discussed in the Introduction, the main objective is to provide fundamental limits on the length and time scales involved in protein folding. Protein folding is also placed within the broader context of macromolecular dynamics, which is extensively studied in the unfolded, folded, and unfolding regimes for the key molecular motifs of cellular biochemistry, including lipids, nucleic acids, and proteins. The effect of the water hydration and temperature are systematically probed to elucidate the crucial role of the environment in macromolecular stability and dynamics. For a wide range of bio-molecular phenomena, the observed collective behavior is shown to arise directly from first principles. Throughout, the emphasis is on analytic results free of tunable parameters, supported by ensemble-converging computational simulations, and corroborated by experimental evidence. ", "date": "2012", "date_type": "degree", "id_number": "CaltechTHESIS:05282012-103610958", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:05282012-103610958", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "DOE CSGF (Department of Energy Computational Science Graduate Fellowship)", "grant_number": "DE-FG02-97ER25308" }, { "agency": "Krell Institute" }, { "agency": "U.S. Department of Energy" } ] }, "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Milo Lin", "deposited_on": "2012-05-30 21:10:42", "doi": "10.7907/CSW5-WY69", "divisions": { "items": [ "div_pma" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "chair" }, { "email": "mcc@caltech.edu", "id": "Cross-M-C", "name": { "family": "Cross", "given": "Michael Clifford" }, "role": "member" }, { "email": "tfm@caltech.edu", "id": "Miller-T-F", "name": { "family": "Miller", "given": "Thomas F." }, "role": "member" }, { "email": "dcrees@caltech.edu", "id": "Rees-D-C", "name": { "family": "Rees", "given": "Douglas C." }, "role": "member" }, { "email": "tat@caltech.edu", "id": "Tombrello-T-A", "name": { "family": "Tombrello", "given": "Thomas A." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2012-05-16", "gradofc_approval_date": "2012-05-30", "thesis_awards": "Milton and Francis Clauser Doctoral Prize, 2012", "review_status": "approved", "option_major": { "items": [ "physics" ] }, "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": "Lin, Milo Miaoyu", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Zewail, Ahmed H.; Cross, Michael Clifford; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/6278", "eprint_id": 6278, "rev_number": 42, "documents": [ { "id": "/id/document/12589", "doc_id": 12589, "rev_number": 6, "files": [ { "id": "/id/file/80161", "fileid": 80161, "datasetid": "document", "objectid": 12589, "filename": "Thesis.pdf", "mime_type": "application/pdf", "filesize": 44878324, "mtime": "2012-12-26 04:33:39", "url": "/6278/3/Thesis.pdf" } ], "eprint_id": 6278, "pos": 3, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Thesis", "language": "en", "security": "public", "license": "other", "main": "Thesis.pdf", "media_duration": "0", "media_aspect_ratio": "0", 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"type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "agahlman@caltech.edu", "id": "Gahlmann-Andreas", "name": { "family": "Gahlmann", "given": "Andreas" }, "orcid": "0000-0001-7521-6787", "show_email": "NO" } ] }, "title": "Ultrafast Electron Diffraction: Pulsed Laser Desorption Enables Time-Resolved Structural Determination of Thermally Labile Chromophores", "ispublished": "unpub", "full_text_status": "public", "keywords": "Ultrafast Electron Diffraction; Structural Determination; Time-Resolved; Gas Phase", "abstract": "
The construction and utilization of the fourth-generation ultrafast electron diffraction apparatus, UED4, is the subject of this thesis. With UED4 and its novel and universal sample delivery method based on laser desorption, we were able to vaporize thermally labile molecular samples and determine their ground-state structures and the structures of their photochemical and photophysical reaction products. Each component part of the new UED4 apparatus is described, and the experimental and computational procedures used to extract structural information from the time-resolved diffraction patterns are presented.
\r\n\r\nSeveral molecules were studied in their ground states and photoinduced excited states or product states on the time scale of picoseconds and nanoseconds. With UED3, nitrobenzene was shown to undergo intramolecular rearrangement prior to NO loss in an ultrafast fragmentation reaction. In indole, the chromophore of the amino acid tryptophan, the involvement of a dark structure, formed on the picosecond time scale, was revealed in the nonradiative decay pathway of the initially excited state. By determining the ground state structures of the thermally labile nucleobases uracil and guanine, the first use of surface-assisted laser desorption in a pulsed electron diffraction experiment was reported using the newly developed UED4 apparatus. The determined structures of the photochemically generated species of the photochromic molecule 6-nitro-BIPS further demonstrated the capability of laser desorption electron diffraction to function as a time-resolved experiment. Finally, the fragmentation reaction of the amino acid tryptophan upon UV laser irradiation was studied with UED4. The ability to deliver increasingly large and conformationally heterogeneous molecules into the gas phase now provides new challenges and opportunities of both experimental and theoretical nature for the field of ultrafast electron diffraction.
", "date": "2011", "date_type": "degree", "id_number": "CaltechTHESIS:04042011-112659805", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:04042011-112659805", "referencetext": { "items": [ "1.\tSrinivasan, R., Lobastov, V. A., Ruan, C.-Y. & Zewail, A. H. Ultrafast electron diffraction (UED) - A new development for the 4D determination of transient molecular structures. Helv. Chim. Acta 86, 1763-1838 (2003).\r\n2.\tPark, S. T., Feenstra, J. S. & Zewail, A. H. Ultrafast electron diffraction: Excited state structures and chemistries of aromatic carbonyls. J. Chem. Phys. 124, 174707 (2006).\r\n3.\tHe, Y. G., Gahlmann, A., Feenstra, J. S., Park, S. T. & Zewail, A. H. Ultrafast electron diffraction: Structural dynamics of molecular rearrangement in the NO release from nitrobenzene. Chem. Asian J. 1, 56-63 (2006).\r\n4.\tGahlmann, A., Park, S. T. & Zewail, A. H. Ultrashort electron pulses for diffraction, crystallography and microscopy: Theoretical and experimental resolutions. Phys. Chem. Chem. Phys. 10, 2894-2909 (2008).\r\n5.\tPark, S. T., Gahlmann, A., He, Y., Feenstra, J. S. & Zewail, A. H. Ultrafast electron diffraction reveals dark structures of the biological chromophore indole. Angew. Chem. Int. Ed. 47, 9496-9499 (2008).\r\n6.\tXu, S. J., Park, S. T., Feenstra, J. S., Srinivasan, R. & Zewail, A. H. Ultrafast electron diffraction: Structural dynamics of the elimination reaction of acetylacetone. J. Phys. Chem. A 108, 6650-6655 (2004).\r\n7.\tSrinivasan, R., Feenstra, J. S., Park, S. T., Xu, S. J. & Zewail, A. H. Dark structures in molecular radiationless transitions determined by ultrafast diffraction. Science 307, 558-563 (2005).\r\n8.\tWilliamson, J. C. Ultrafast gas-phase electron diffraction. PhD Dissertation, California Institute of Technology (1997).\r\n9.\tSrinivasan, R. 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J., Chabalowski," ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "Gordon and Betty Moore Foundation" }, { "agency": "Air Force Office of Scientific Research", "grant_number": "FA9550-07-1-0484" }, { "agency": "Air Force Office of Scientific Research", "grant_number": "F49620-03-1-0070" }, { "agency": "National Science Foundation", "grant_number": "NSF-DMR 0504854" }, { "agency": "National Science Foundation", "grant_number": "NSF-CHE-0117850" }, { "agency": "National Science Foundation", "grant_number": "NSF-CHE 0096400" } ] }, "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "ag5vu@virginia.edu", "deposited_by": "Andreas Gahlmann", "deposited_on": "2011-05-17 23:18:05", "doi": "10.7907/YACJ-HG30", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "dervan@caltech.edu", "id": "Dervan-P-B", "name": { "family": "Dervan", "given": "Peter B." }, "role": "chair" }, { "email": "aron@caltech.edu", "id": "Kuppermann-A", "name": { "family": "Kuppermann", "given": "Aron" }, "role": "member" }, { "email": "jensen@caltech.edu", "id": "Jensen-G-J", "name": { "family": "Jensen", "given": "Grant J." }, "role": "member" }, { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2011-04-27", "gradofc_approval_date": "2011-05-17", "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. 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{ "items": [ { "email": "irlee@caltech.edu", "id": "Lee-I-Ren", "name": { "family": "Lee", "given": "I-Ren" }, "show_email": "NO" } ] }, "title": "Femtosecond Time-resolved Spectroscopy of Gas-phase Anions: Electron Solvation and Isolated Chromophore Dynamics", "ispublished": "unpub", "full_text_status": "public", "keywords": "Femtochemistry, Photoelectron, Gas-phase, Anion, Clusters, Photoactive Yellow Protein, Photoisomerization", "abstract": "This thesis presents the studies of ultrafast dynamics of negatively charged molecules and clusters in the gas phase using femtosecond photoelectron spectroscopy. The core motifs of two distinct complex systems \u2014 solvated electrons and protein chromophores \u2014 were studied in the gas phase.
\r\n\r\nFor the solvated electron systems \u2014 hydrated electrons and ammoniated electrons \u2014 were studied in finite-sized clusters in the gas phase. Interestingly, the results show a significant difference. In the hydrated electron, ground-state vibrational cooling is evident by the transient photoelectron spectra, while, in the ammoniated electron, a coherent motion with a 500-fs relaxation is observed. The difference is attributed to the cage rigidity, which results in different solvent motions for the electron\u2019s interaction with water (libration) or ammonia (phonon-like).
\r\n\r\nThe photocycle of the photoactive yellow protein (PYP) has been studied extensively, but the dynamics of the isolated chromophore responsible for the transduction of phototacticity is less known. The anionic chromophore model molecule was investigated in the gas phase using femtosecond photoelectron spectroscopy and the results indicate that the protein function is in directing efficient conversion to the cis-structure and in impeding radical formation within the protein. Finally, a classic system of conformational twisting, stilbene, was studied in its anionic radical state. Ultrafast conversions from both trans- and cis- isomers are accompanied with coherent oscillation, in contrast to observations in the solution phase, and this suggests that a major solvent retardation take place. Dynamic studies of the photochemistry of gas-phase anions are very scarce due to the experimental difficulties. However, our results successfully resolve the photophysics and photochemistry of the isolated species and, thereby, elucidate the effect of solution.
", "date": "2011", "date_type": "degree", "id_number": "CaltechTHESIS:12082010-143906786", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:12082010-143906786", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "I-Ren Lee", "deposited_on": "2010-12-23 19:29:50", "doi": "10.7907/BAYG-2G33", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "mckoy@caltech.edu", "id": "McKoy-B-V", "name": { "family": "McKoy", "given": "Basil Vincent" }, "role": "chair" }, { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "member" }, { "email": "dervan@caltech.edu", "id": "Dervan-P-B", "name": { "family": "Dervan", "given": "Peter B." }, "role": "member" }, { "email": "mo@caltech.edu", "id": "Okumura-M", "name": { "family": "Okumura", "given": "Mitchio" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2010-11-22", "gradofc_approval_date": "2010-12-20", "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": "2011", "author_list": "Lee, I-Ren", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "McKoy, Basil Vincent; Zewail, Ahmed H.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1685", "eprint_id": 1685, "rev_number": 60, "documents": [ { "id": "/id/document/2663", "doc_id": 2663, "rev_number": 4, "files": [ { "id": "/id/file/16381", "fileid": 16381, "datasetid": "document", "objectid": 2663, "filename": "00TitlePageAcknowledgeAbstractLists.pdf", "mime_type": "application/pdf", "filesize": 196597, "mtime": "2012-12-26 02:40:38", "url": "/1685/1/00TitlePageAcknowledgeAbstractLists.pdf" } ], "eprint_id": 1685, "pos": 1, "placement": 2, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "00TitlePageAcknowledgeAbstractLists.pdf", "language": "en", "security": "public", 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"dir": "disk0/00/00/16/85", "datestamp": "2009-05-14", "lastmod": "2019-11-26 20:36:59", "status_changed": "2009-09-25 02:11:47", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "yang@uh.edu", "id": "Yang-Ding-Shyue-Jerry", "name": { "family": "Yang", "given": "Ding-Shyue (Jerry)" }, "orcid": "0000-0003-2713-9128", "show_email": "NO" } ] }, "title": "Ultrafast Electron Crystallography: Principles and Applications", "ispublished": "unpub", "full_text_status": "public", "keywords": "electron-lattice coupling; nanostructures; phase transition", "abstract": "During the last 20 to 30 years, the development and application of time-resolved experimental techniques with a femtosecond temporal resolution have brought to us much knowledge about the fundamental processes in physics, chemistry and biology. Nevertheless, standard spectroscopic methods have their limitation in the determination of the transient structures during ultrafast dynamics at the atomic level, because the spatial resolution is restricted by the wavelength of the probe pulse used. In contract, with the scheme of femtosecond optical initiation and electron probing and through the diffraction phenomenon, ultrafast electron crystallography (UEC) was recently developed as a time-resolved structure-probing technique for condensed-matter studies. The short wavelength and small pulse duration of the highly accelerated electrons used provide the atomic-scale spatiotemporal resolution. In addition, the large electron\u2013matter interaction enables the detection of small transient changes as well as the investigation of surface and interfacial phenomena.
\r\n\r\nThis thesis describes the principles of UEC and its applications to a variety of systems, ranging from nanometer-scale structures to highly correlated materials and to interfacial assemblies. By using a prototype semiconducting material, we elucidated the fundamental processes at work in different parts of the femtosecond-to-nanosecond time range; this investigation led to a conceptual change from the consideration of laser-induced heating to the examination of nonequilibrium structural modifications as a result of the transient dynamical changes in, e.g., carriers, the crystal potential, and phonons. On the basis of such an understanding, we observed and understood the colossal unidirectional expansion induced by the photoexcitation of nanostructures to be a potential-driven result rather than a thermal one.
\r\n\r\nFor highly correlated materials, we showed the effectiveness of UEC in resolving the transient intermediate structures during phase transformations as well as identifying new phases in the nonequilibrium state. An important breakthrough made by UEC was the confirmation of the anisotropic involvement of lattice in the electron pairing mechanism for high-temperature superconductors. In interfacial assemblies, we also found a nonequilibrium phase transformation in water and the phenomenon of ultrafast annealing for a better order in a self-assembled monolayer. With these successful experiences, we expect more condensed-matter studies by UEC to come.
\r\n", "date": "2009", "date_type": "degree", "id_number": "CaltechETD:etd-05082009-170032", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05082009-170032", "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": "2009-05-14", "doi": "10.7907/Y61P-2B24", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "mckoy@caltech.edu", "id": "McKoy-B-V", "name": { "family": "McKoy", "given": "Basil Vincent" }, "role": "chair" }, { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "member" }, { "email": "dcrees@caltech.edu", "id": "Rees-D-C", "name": { "family": "Rees", "given": "Douglas C." }, "role": "member" }, { "email": "ncyeh@caltech.edu", "id": "Yeh-Nai-Chang", "name": { "family": "Yeh", "given": "Nai-Chang" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2009-05-08", "thesis_defense_date": "2009-05-05", "thesis_approved_date": "2009-05-14", "gradofc_approval_date": "2009-05-12", "thesis_awards": "The Herbert Newby McCoy Award, 2009", "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": "2009", "author_list": "Yang, Ding-Shyue (Jerry)", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "McKoy, Basil Vincent; Zewail, Ahmed H.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/409", "eprint_id": 409, "rev_number": 49, "documents": [ { "id": "/id/document/617", "doc_id": 617, "rev_number": 4, "files": [ { "id": "/id/file/3909", "fileid": 3909, "datasetid": "document", "objectid": 617, "filename": "01TitlePages.pdf", "mime_type": "application/pdf", "filesize": 34518, "mtime": "2012-12-26 02:29:37", "url": "/409/1/01TitlePages.pdf" } ], "eprint_id": 409, "pos": 1, "placement": 2, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "01TitlePages.pdf", "language": "en", "security": "public", "license": "other", "main": "01TitlePages.pdf", "media_duration": 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"dir": "disk0/00/00/04/09", "datestamp": "2007-02-12", "lastmod": "2020-02-26 19:16:12", "status_changed": "2009-09-25 01:36:56", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "songyech@caltech.edu", "id": "Chen-Songye", "name": { "family": "Chen", "given": "Songye" }, "orcid": "0000-0001-5407-5049", "show_email": "YES" } ] }, "title": "Structural Dynamics by Ultrafast Electron Crystallography", "ispublished": "unpub", "full_text_status": "public", "keywords": "diffraction; fatty acid; Langmuir-Blodgett film; phospholipids; surfaces and interfaces", "abstract": "Ultrafast electron crystallography (UEC), combining the ultrafast time resolution with femtosecond lasers and the atomic spacial resolution with electron crystallography, is developed and applied to elucidate the structural dynamics in solids, surfaces and macromolecular systems. The UEC experiments for surface studies were first demonstrated on semiconductor surfaces. Coherent nonthermal motions of atoms following ultrafast laser irradiation were shown with the timescales in picoseconds, and the amplitude of the motions was determined in picometer. Using Langmuir-Blodgett films, two-dimensional crystalline monolayer, bilayers and multilayers of fatty acids and phospholipids were also studied by UEC. The atomic structures under different preparation conditions were determined. The structural dynamics following a temperature jump induced by femtosecond laser on the substrates were obtained and compared to the equilibrium temperature dependence. It was observed that a coherent anisotropic expansion solely along the aliphatic chains happens at picosecond timescale, followed by nonequilibrium contraction and restructuring at longer times. The effects of different molecules, layer thickness and substrate on the dynamics were examined. Unlike monotonic disordering in the equilibrium heating, a transient structural ordering was revealed on the picosecond timescale.", "date": "2007", "date_type": "degree", "id_number": "CaltechETD:etd-01302007-102801", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-01302007-102801", "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/PE9B-7R72", "divisions": { "items": [ "div_pma" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "chair" }, { "email": "etcher@caltech.edu", "id": "Scherer-A", "name": { "family": "Scherer", "given": "Axel" }, "role": "member" }, { "email": "ncyeh@caltech.edu", "id": "Yeh-Nai-Chang", "name": { "family": "Yeh", "given": "Nai-Chang" }, "role": "member" }, { "email": "mckoy@caltech.edu", "id": "McKoy-B-V", "name": { "family": "McKoy", "given": "Basil Vincent" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2007-01-30", "thesis_defense_date": "2006-11-30", "thesis_approved_date": "2007-02-12", "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. 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"uri": "/id/document/3464" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/3464" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/3464" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/19/78", "datestamp": "2006-05-30", "lastmod": "2019-12-21 04:19:09", "status_changed": "2009-09-25 02:21:48", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "feenstra@alumni.caltech.edu", "id": "Feenstra-Jonathan-Stuart", "name": { "family": "Feenstra", "given": "Jonathan Stuart" }, "show_email": "NO" } ] }, "title": "Ultrafast Electron Diffraction: Direct Determination of Structural Dynamics of Molecular Excited States", "ispublished": "unpub", "full_text_status": "public", "keywords": "excited state dynamics; transient structure; ultrafast electron diffraction", "note": "Thesis in Commencement Program (2006) entitled: Ultrafast Electron Diffraction: The Development of Methodology for the Direct Determination of Structural Dynamics of Molecular Excited States", "abstract": "Ultrafast electron diffraction (UED) has been applied to determine the structures of isolated molecules and the dynamics of their excited states. Preceding the experimental accounts is a detailed discussion of the theoretical methodology behind UED in the Caltech labs. The procedure is explained by which electron scattering signal is measured and processed to allow the direct determination of structural dynamics (the signature feature of this experiment). The apparatus itself is also broken down into its component parts and discussed.
\r\n\r\nUED has the capability of studying both ground and excited state systems, which will be demonstrated by example. A number of molecules were studied in their ground states (chlorobenzene, bromobenzene, iodobenzene, 2-fluoropyridine, acetylacetone, benzaldehyde, acetophenone, and methylbenzoate). The structures were determined and compared with structures derived by theoretical calculations and with the results of previous gas electron diffraction inquiries. The molecular structures of 2-fluoropyridine, acetophenone, and methylbenzoate had not been previously experimentally determined. The structure of ground-state acetylacetone is discussed in detail as it represents an old problem involving the influence of intramolecular hydrogen bonding.
\r\n\r\nAcetylacetone, benzaldehyde, and acetophenone were also studied after excitation by a femtosecond laser pulse. Acetylacetone was observed to fragment \u2013 losing the hydroxyl radical. Calculations were performed to further explore the dynamics and mechanism. For excited benzaldehyde and acetophenone, a bifurcation of pathways was structurally resolved. Both molecules have photophysical and photochemical channels from the excited state. The photophysical channels result in the formation of a structure possessing a quinoid ring. The photochemical channels differed \u2013 for benzaldehyde, molecular dissociation resulting in benzene and carbon monoxide, and for acetophenone, homolytic bond cleavage resulting in methyl and benzoyl radicals. The structures of all species were determined as were the time scales involved. Calculations were used to assist in the determination of the excited state decay mechanisms.
", "date": "2006", "date_type": "degree", "id_number": "CaltechETD:etd-05232006-084250", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05232006-084250", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "Blanche Mowrer Fellowship" }, { "agency": "NSF" }, { "agency": "U.S. Air Force Office of Scientific Research" } ] }, "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2006-05-30", "doi": "10.7907/QCFT-AK63", "alt_title": { "items": [ "Ultrafast Electron Diffraction: The Development of Methodology for the Direct Determination of Structural Dynamics of Molecular Excited States" ] }, "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "dcrees@caltech.edu", "id": "Rees-D-C", "name": { "family": "Rees", "given": "Douglas C." }, "role": "chair" }, { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "member" }, { "email": "collier@caltech.edu", "id": "Collier-C-P", "name": { "family": "Collier", "given": "C. Patrick" }, "role": "member" }, { "email": "mckoy@caltech.edu", "id": "McKoy-B-V", "name": { "family": "McKoy", "given": "Basil Vincent" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2006-05-23", "thesis_defense_date": "2006-05-23", "thesis_approved_date": "2006-05-30", "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": "Feenstra, Jonathan Stuart", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Rees, Douglas C.; Zewail, Ahmed H.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1749", "eprint_id": 1749, "rev_number": 55, "documents": [ { "id": "/id/document/2829", "doc_id": 2829, "rev_number": 5, "files": [ { "id": "/id/file/17250", "fileid": 17250, "datasetid": "document", "objectid": 2829, "filename": "00_TOC.pdf", "mime_type": "application/pdf", "filesize": 1006976, "mtime": "2012-12-26 02:41:34", "url": "/1749/1/00_TOC.pdf" } ], "eprint_id": 1749, "pos": 1, "placement": 2, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "00_TOC.pdf", "language": "en", "security": "public", "license": "other", "main": "00_TOC.pdf", "media_duration": "0", 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"0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/11759" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/11759" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/11759" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/17/49", "datestamp": "2005-05-13", "lastmod": "2020-07-23 22:02:51", "status_changed": "2009-09-25 02:14:23", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "ramesh@alumni.caltech.edu", "id": "Srinivasan-Ramesh", "name": { "family": "Srinivasan", "given": "Ramesh" }, "show_email": "YES" } ] }, "title": "Structural Dynamics of Complex Molecules by Ultrafast Electron Diffraction : Concepts, Methodology and Applications", "ispublished": "unpub", "full_text_status": "public", "keywords": "complex molecules; femtochemistry; femtoscience; structural dynamics; ultrafast electron crystallography; ultrafast electron diffraction; ultrafast electron microscopy", "abstract": "The central theme in ultrafast electron diffraction (UED) is the elucidation of the structural dynamics of transient molecular entities. With properly timed sequences of ultrafast electron pulses, it is now possible to image complex molecular structures in the four dimensions of space and time with resolutions approaching 0.01 [angstroms] and 1 ps, respectively. Reaching this spatiotemporal resolution on the atomic scale has been the driving force behind the development and application of the third generation UED instrument\u2013-the subject of this dissertation. The current state-of-the-art in resolutions and sensitivity, together with theoretical advances, has made possible the direct determination of transient structures, leading to studies of diverse molecular phenomena hitherto not accessible to other techniques. By freezing structures on the ultrafast timescale, we are able to develop concepts that correlate structure with dynamics. Examples include structure-driven radiationless processes, dynamics-driven reaction stereochemistry, and non-equilibrium structures exhibiting negative temperature, bifurcation, or selective energy localization in bonds. These successes in the studies of complex molecular systems, even without heavy atoms, establish UED as a powerful method for mapping out temporally changing molecular structures in chemistry, and potentially, in biology.", "date": "2005", "date_type": "degree", "id_number": "CaltechETD:etd-05122005-083103", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05122005-083103", "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": "2005-05-13", "doi": "10.7907/DTG2-5932", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "chair" }, { "email": "tirrell@caltech.edu", "id": "Tirrell-D-A", "name": { "family": "Tirrell", "given": "David A." }, "role": "member" }, { "email": "dcrees@caltech.edu", "id": "Rees-D-C", "name": { "family": "Rees", "given": "Douglas C." }, "role": "member" }, { "email": "jak@cheme.caltech.edu", "id": "Kornfield-J-A", "name": { "family": "Kornfield", "given": "Julia A." }, "role": "member" }, { "email": "mckoy@its.caltech.edu", "id": "McKoy-B-V", "name": { "family": "McKoy", "given": "Basil Vincent" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2005-05-12", "thesis_defense_date": "2004-12-01", "thesis_approved_date": "2005-05-13", "thesis_awards": "Everhart Distinguished Graduate Student Lecturer Award, 2002.", "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": "2005", "author_list": "Srinivasan, Ramesh", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Zewail, Ahmed H.; Tirrell, David A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/2140", "eprint_id": 2140, "rev_number": 9, "documents": [ { "id": "/id/document/3888", "doc_id": 3888, "rev_number": 3, "files": [ { "id": "/id/file/22766", "fileid": 22766, "datasetid": "document", "objectid": 3888, "filename": "THESIS.pdf", "mime_type": "application/pdf", "filesize": 14968159, "mtime": "2012-12-26 02:47:24", "url": "/2140/1/THESIS.pdf" } ], "eprint_id": 2140, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": "THESIS.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", 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"eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/21/40", "datestamp": "2004-06-09", "lastmod": "2021-02-02 23:26:06", "status_changed": "2009-09-25 02:27:53", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "paikd@jilau1.Colorado.EDU", "id": "Paik-Daniel-Hern", "name": { "family": "Paik", "given": "Daniel Hern" }, "show_email": "NO" } ] }, "title": "Femtosecond Time-Resolved Spectroscopy of Anionic Systems: Dynamics of Mesoscopic Solvation and Gas-Phase Organic Reactions", "ispublished": "unpub", "full_text_status": "public", "keywords": "anionic clusters; femtosecond spectroscopy; transition state dynamics", "abstract": "This thesis work presents the femtosecond time-resolved spectroscopy of anionic systems ranging from gas-phase organic molecules to the finite-sized molecular clusters. The subject matter in this thesis is twofold: Mesoscopic solvation of anionic clusters and transition state dynamics of neutral organic molecules.
\r\n\r\nSolvation dynamics in the finite sized clusters were investigated at the molecular level of details. The main objective of the cluster study was to follow the evolution of cluster properties as function of cluster size. Ultrafast processes exhibited in the cluster systems were investigated by utilizing the femtosecond time-resolved anion photoelectron spectroscopy. The bond rupture and solvent evaporation of homogeneous and heterogeneous clusters were studied, and the correlation between the dissociation rates and the cluster size is obtained. Gas-phase analogues of solvated systems were studied, and the key steps involved in the solvation dynamics are highlighted.
\r\n\r\nDirect probing of the transition state dynamics in the ground state is studied with femtosecond time resolution. The transition state of the ring inversion reaction of cyclooctatetraene was directly accessed by the vertical detachment from the planar anion. The subsequent nuclear motion was then probed by ionization mass spectrometry. The oscillatory feature observed in the transients reflects trajectories of motion (resonance) along the reaction coordinate, and comparison with theory is reported. This work demonstrated the applicability of the charge reversal scheme to a complex organic system and suggests the possibility of studying ground-state thermal organic reactions with their transition states resolved in real time.
", "date": "2004", "date_type": "degree", "id_number": "CaltechETD:etd-05272004-213231", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05272004-213231", "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": "2004-06-09", "doi": "10.7907/W687-V550", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "mckoy@caltech.edu", "id": "McKoy-B-V", "name": { "family": "McKoy", "given": "Basil Vincent" }, "role": "chair" }, { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "member" }, { "email": "collier@caltech.edu", "id": "Collier-C-P", "name": { "family": "Collier", "given": "C. Patrick" }, "role": "member" }, { "email": "jkbarton@caltech.edu", "id": "Barton-J-K", "name": { "family": "Barton", "given": "Jacqueline K." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2004-05-27", "thesis_defense_date": "2004-05-26", "thesis_approved_date": "2004-06-09", "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": "2004", "author_list": "Paik, Daniel Hern", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "McKoy, Basil Vincent; Zewail, Ahmed H.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1292", "eprint_id": 1292, "rev_number": 22, "documents": [ { "id": "/id/document/1959", "doc_id": 1959, "rev_number": 4, "files": [ { "id": "/id/file/12258", "fileid": 12258, "datasetid": "document", "objectid": 1959, "filename": "Ihee_h_2001.pdf", "mime_type": "application/pdf", "filesize": 24711254, "mtime": "2012-12-26 02:36:56", "url": "/1292/1/Ihee_h_2001.pdf" } ], "eprint_id": 1292, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": "Ihee_h_2001.pdf", "media_duration": "0", "media_aspect_ratio": "0", 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"media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/92669" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/92669" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/92669" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/12/92", "datestamp": "2008-04-08", "lastmod": "2022-09-13 21:39:54", "status_changed": "2009-09-25 02:00:30", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "ihee57@gmail.com", "id": "Ihee-Hyotcherl", "name": { "family": "Ihee", "given": "Hyotcherl" }, "orcid": "0000-0003-0397-5965", "show_email": "YES" } ] }, "title": "Ultrafast Electron Diffraction", "ispublished": "unpub", "full_text_status": "public", "keywords": "Chemistry", "abstract": "Molecular dynamics is now routinely studied on femtosecond time scales using various spectroscopies. However, direct structural information of all nuclear coordinates involved in such dynamical processes requires resolution in time by x-ray or electron diffraction. The focus of this laboratory has been the development of ultrafast electron diffraction (UED) for recording structures in motion, which exploits the six-orders-of-magnitude higher scattering cross section of electrons compared with x-rays. Conventional electron diffraction has been developed over the last several decades to become an enormously powerful technique for determining the static structures of molecules in the gas phase; the subsequent plementation of pulsed electron sources has added a temporal dimension to such studies. In UED, a femtosecond (fs) laser pulse is used to initiate a reaction, but unlike other ultrafast spectroscopies, the subsequent laser pulses normally used to probe the progress of the reaction are replaced with ultrashort pulses of electrons. Time-resolved diffraction patterns are then recorded at fixed time delays relative to the zero-of-time. This directly reflects the changing internuclear distances in the species under study.
\r\n\r\nFor these UED studies, there exist a number of significant experimental challenges, including: (i) the problem of independently determining the temporal overlap (zero-of-time) of the pump and probe pulses in situ for clocking the change; (ii) the problem of low electron flux required to minimize space-charge induced temporal broadening of electron pulses; and (iii) the problem of low scattering and sensitivity caused by the absence of long-range order present in solids, and the low density of molecules in gases. These challenges to the realization of UED have been surmounted over the last decade, and UED now approaches the combined spatial and temporal resolution necessary for tracking all nuclear coordinates during the making and breaking of chemical bonds, thereby permitting the direct observation of molecular structural dynamics in real time. In addition, the diffraction-difference method\u2014which employs the subtraction of a reference diffraction signal from the signals recorded over the course of the reaction\u2014can be used to select the contributions resulting only from changes in structure in the species under study, thereby enhancing the sensitivity of UED to chemical change. Contributions only from the products can be also isolated by adding the appropriately scaled parent diffraction signal at negative time to the difference curves, thus canceling out the parent contribution in each curve.
\r\n\r\nThe first reaction studied by UED was the dissociation of CH2I2 into CH2I and I with fs laser pulses. The second-generation apparatus allowed us to see the amplitude change in the scattering intensity on the picosecond time scale resulting from dissociation. Since this work, UED experiments have successfully investigated the course of several prototypical chemical reactions. For example, the molecular structures and branching ratios of the final products were determined in the dissociation of Fe(CO)5 upon two-photon excitation at 310 nm. A simple intermediate, CF2, was generated by fragmentation of CF2I2 and its molecular structure was precisely determined and compared with other experiments and theoretical calculations. Furthermore, the molecular structure of the transient Fe(CO)4 species was elucidated and compared with available theoretical predictions, permitting identification of the specific electronic energy state of the intermediate and the primary reaction pathway. UED was applied to another organometallic compound, namely (C5H5)Co(CO)2 and the molecular structures of the intermediate and final products were observed. A preliminary analysis showed that either C5H5 and other species can be selectively generated depending on the excitation wavelength. Further analysis will elucidate their molecular structures. The elimination of iodine from 1,2-diiodotetrafluoroethane (C2F4I2) was also studied with the second-generation apparatus, providing early results which suggested that the molecular structure of the C2F4I radical intermediate is not bridged in nature, but instead is \"classical,\" resembling the structure of the parent species.
\r\n\r\nThe need for greater sensitivity and resolution, as well as the desire to study more complex reactions, led to the development of our third-generation UED apparatus. This new machine, with vast improvements in pulsed electron flux, repetition rate, detection sensitivity, and experimental stability, permits the direct imaging of complex chemical reactions with unprecedented spatial and temporal resolution. The spatial and temporal resolution of UED approached ~0.01 \u00c5 and ~1 ps, respectively, and we were sensitive to ~1% changes in the mole fractions of the various chemical species over the course of the reaction. In its first application, the non-concerted elimination of iodine from a haloethane (C2F4I2) was re-visited and the molecular structure of the transient (C2F4I) radical was determined for the first time. Two prototypical cyclic hydrocarbons, 1,3,5-cycloheptatriene (CHT) and 1,3-cyclohexadiene (CHD), were also studied with temporal and spatial resolution of ~5 ps and ~0.04 \u00c5 respectively. At high internal energies of ~4 eV, these molecules displayed markedly different behavior. For CHT, wherein excitation resulted in the reformation of the parent, the observed diffraction change was explained with an equipartitioned model of hot structures\u2014indicating rapid energy redistribution (within a few picoseconds). For CHD, photo-induced ring opening was shown to result in hot but highly non-equilibrium structures even up to 400 ps, with energy trapped in large-amplitude motions comprised of torsion and asymmetric stretching. These studies promise a new direction of research for studying transient structural changes both in equilibrium and non-equilibrium complex systems. The results presented here provide the new limit of improved detection sensitivity, versatility, and resolution of UED, as well as the potential for its diverse applications. The extension to even more complex systems, a process that has already begun in our laboratory, represents our next challenge in UED.
\r\n", "date": "2001", "date_type": "degree", "id_number": "CaltechETD:etd-04072008-112244", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04072008-112244", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "NSF" }, { "agency": "U.S. Air Force Office of Scientific Research" }, { "agency": "U.S. Office of Naval Research" } ] }, "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-04-08", "doi": "10.7907/AZ0P-H612", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "id": "McKoy-B-V", "name": { "family": "McKoy", "given": "Basil Vincent" }, "role": "chair" }, { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "member" }, { "id": "Stoltz-B-M", "name": { "family": "Stoltz", "given": "Brian M." }, "orcid": "0000-0001-9837-1528", "role": "member" }, { "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_submitted_date": "2008-04-07", "thesis_defense_date": "2001-04-30", "thesis_approved_date": "2008-04-08", "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": "2001", "author_list": "Ihee, Hyotcherl", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "McKoy, Basil Vincent; Zewail, Ahmed H.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1296", "eprint_id": 1296, "rev_number": 13, "documents": [ { "id": "/id/document/1963", "doc_id": 1963, "rev_number": 4, "files": [ { "id": "/id/file/12290", "fileid": 12290, "datasetid": "document", "objectid": 1963, "filename": "Chong_sh_2001.pdf", "mime_type": "application/pdf", "filesize": 4476745, "mtime": "2012-12-26 02:36:57", "url": "/1296/1/Chong_sh_2001.pdf" } ], "eprint_id": 1296, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": "Chong_sh_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/18733" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/18733" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/18733" } ] } }, { "id": "/id/document/18733", "doc_id": 18733, "rev_number": 3, "files": [ { "id": "/id/file/12288", "fileid": 12288, "datasetid": "document", "objectid": 18733, "filename": "preview.png", "mime_type": "image/png", "hash": "15a2b67b209bc94ecedbe61c33f5438c", "hash_type": "MD5", "filesize": 13772, "mtime": "2012-12-26 02:36:57", "url": "/1296/2/preview.png" } ], "eprint_id": 1296, "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/1963" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/1963" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/1963" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/12/96", "datestamp": "2008-04-08", "lastmod": "2022-09-13 20:53:51", "status_changed": "2009-09-25 02:00:35", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Chong-Sing-Hwa", "name": { "family": "Chong", "given": "Sing Hwa" }, "show_email": "NO" } ] }, "title": "Ultrafast Dynamics of Barrier Crossing: Step-Wise Solvation Effect on Isomerization of Trans-Stilbene in Alkane Clusters", "ispublished": "unpub", "full_text_status": "public", "keywords": "(Chemistry)", "abstract": "The ultrafast spectroscopic study of molecular clusters in supersonic beams can provide valuable information on the structure, energetics and dynamics of molecular aggregates in gas phase and in solution. This information will shed light on important issues such as how molecules interact, how energy flows in solvated systems, and how chemical reactions progress.
\r\n\r\nAlthough microscopic friction and solvation in barrier crossing reactions is of fundamental importance in molecular dynamics, their roles are not well understood. This is mainly due to the fact that few comprehensive investigations of this subject have been performed. In this thesis, the detail studies of a prototypical barrier crossing reaction\u2014the photoisomerization of jet-cooled trans-stilbene\u2014in size-selected n-alkane clusters, using the picosecond pump-probe ionization TOF mass spectrometry and transient technique, are reported. The microcanonical nonradiative decay rate constants at the S1 manifold for trans-stilbene-hexanen and trans-stilbene-octanen (n = 1, 2) complexes, including certain deuterated variants, were measured as a function of excitation energy, with the energy range defined by tuning the pump wavelength from the 0-0 transition of trans-stilbene to ~3200 cm-1 higher in energy. The experimental results were modeled with standard RRKM theory, nonadiabatic RRKM theory and Kramers-type theory for microcanonical systems. It was found that the excess energy dependence results could be accounted for very well by the nonadiabatic RRKM theory, from which analysis the barriers to isomerization for all of the trans-stilbene n-alkane clusters were found to be lower than that of the parent molecule by ~50%. The analysis revealed that not only can the differences in the rates among the four trans-stilbene-hexane1 isotopic species studied (combinations of trans-stilbene-h12 and -d12 with n-hexane-h14 and -d14) be attributed to energy friction, a term describing how energy is \"drained away\" from the reaction coordinate as a result of the change in the vibrational density of states, but the reduction in the nonradiative rates of the 1:2 complexes, relative to that of the 1:1 complexes, can also be attributed to the same energy friction.
\r\n\r\nFinally, in the same studies, the cluster binding energies of trans-stilbene-hexanen and trans-stilbene-octanen were also determined.
", "date": "2001", "date_type": "degree", "id_number": "CaltechETD:etd-04072008-151825", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04072008-151825", "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": "2008-04-08", "doi": "10.7907/5m8y-hz17", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" }, { "id": "Bercaw-J-E", "name": { "family": "Bercaw", "given": "John E." }, "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "id": "Okumura-M", "name": { "family": "Okumura", "given": "Mitchio" }, "orcid": "0000-0001-6874-1137", "role": "chair" }, { "id": "Barton-J-K", "name": { "family": "Barton", "given": "Jacqueline K." }, "orcid": "0000-0001-9883-1600", "role": "member" }, { "id": "McKoy-B-V", "name": { "family": "McKoy", "given": "Basil Vincent" }, "role": "member" }, { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-04-07", "thesis_defense_date": "1999-08-09", "thesis_approved_date": "2008-04-08", "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": "2001", "author_list": "Chong, Sing Hwa", "advisor_list": "Zewail, Ahmed H. and Bercaw, John E.", "comittee_list": "Okumura, Mitchio; Barton, Jacqueline K.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1294", "eprint_id": 1294, "rev_number": 14, "documents": [ { "id": "/id/document/1961", "doc_id": 1961, "rev_number": 3, "files": [ { "id": "/id/file/12275", "fileid": 12275, "datasetid": "document", "objectid": 1961, "filename": "Zhong_d_1999.pdf", "mime_type": "application/pdf", "filesize": 14523102, "mtime": "2012-12-26 02:36:57", "url": "/1294/1/Zhong_d_1999.pdf" } ], "eprint_id": 1294, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Zhong_d_1999.pdf", "language": "en", "security": "public", "license": "other", "main": "Zhong_d_1999.pdf", 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provides new challenges because the reactions evolve along multiple pathways. New techniques are needed to dissect these complex systems into the elementary reactions. In this thesis, femtosecond-resolved mass spectrometry is successfully developed to achieve temporal, speed, angular and state resolution(s) of the reaction dynamics. With these capabilities, the mechanism and dynamics of the complex reactions are able to be microscopically elucidated for each elementary step by monitoring the temporal evolution of the transition state and final products, measuring the energy deposition among the translational and internal motions of the final products, and resolving the correlation between the structural changes and the energy release.
\r\n\r\nThe complex reactions studied range from unimolecular dissociation, to bimolecular reactions, to cluster solvation, and to nonradiative dynamics. For unimolecular reactions, the level of complexity varies from diatomics to polyatomics, from direct-mode to complex-mode, from one-bond breakage to multi-bond fission. The six different systems were examined and a variety of dynamic behaviors have been revealed, including product rotational and vibrational excitation, electronic and vibrational predissociation, and saddle-point transition-state dynamics.
\r\n\r\nMany kinds of bimolecular reactions were studied, consisting of the major contributions of this thesis. For the first time, the famous electron-donor-acceptor charge-transfer reactions are fully understood. More than ten systems were examined with the different charge-transfer characters and all elementary steps involved are microscopically resolved. Several concepts have been addressed including the reversibility of electron transfer, the nonconcertedness of reverse electron transfer and the bond breakage, the energy dissipation, and the reaction coherence. The reversible electron transfer is found as a general reaction mechanism. The system has been considered as a benchmark textbook example and provides insights into biological charge-transfer processes.
\r\n\r\nThe aromatic nucleophilic substitution reaction was studied. The reaction is involved with many elementary steps and the rate-determining step was identified. The first atom-molecule inelastic collision was clocked in fs resolution and a novel method is presented by femtosecond detachment. The collision complexes are observed and quantum resonance may play a role. The first four-center covalent-covalent bimolecular reaction was studied and the cooperative motion of four centers was observed. The method presented is general and very important, and should be applied to study a variety of covalent-covalent bimolecular reactions.
\r\n\r\nThe solvation ultrafast dynamics were systematically studied for many systems from small to lager clusters by monitoring the temporal evolution and translational energy distributions of the escaped solute. Different solvent structures are identified based on the dramatic temporal behaviors of the exited solute. Finally, the nonradiative dynamics of big organic molecules, using azines as examples, were studied. Different isomers of the valance-bond azines are observed. The conical intersection was found to play a key role on the ultrafast nonradiative dynamics and seems to be a general phenomenon, consistent with the recent ab initio predictions.
\r\n", "date": "1999", "date_type": "degree", "id_number": "CaltechETD:etd-04072008-130657", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04072008-130657", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-04-08", "doi": "10.7907/7GR2-YW91", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "chair" }, { "id": "Richards-J-H", "name": { "family": "Richards", "given": "John H." }, "role": "member" }, { "id": "Okumura-M", "name": { "family": "Okumura", "given": "Mitchio" }, "role": "member" }, { "id": "McKoy-B-V", "name": { "family": "McKoy", "given": "Basil Vincent" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-04-07", "thesis_defense_date": "1999-05-05", "thesis_approved_date": "2008-04-08", "thesis_awards": "The Herbert Newby McCoy Award, 1999.\r\nMilton and Francis Clauser Doctoral Prize, 1999.", "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": "1999", "author_list": "Zhong, Dongping", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Zewail, Ahmed H.; Richards, John H.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1291", "eprint_id": 1291, "rev_number": 9, "documents": [ { "id": "/id/document/1958", "doc_id": 1958, "rev_number": 3, "files": [ { "id": "/id/file/12249", "fileid": 12249, "datasetid": "document", "objectid": 1958, "filename": "Liu_q_1997.pdf", "mime_type": "application/pdf", "filesize": 8193923, "mtime": "2012-12-26 02:36:56", "url": "/1291/1/Liu_q_1997.pdf" } ], "eprint_id": 1291, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Liu_q_1997.pdf", "language": "en", "security": "public", "license": "other", "main": "Liu_q_1997.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/18728" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/18728" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/18728" } ] } }, { "id": "/id/document/18728", "doc_id": 18728, "rev_number": 3, "files": [ { "id": "/id/file/12247", "fileid": 12247, "datasetid": "document", "objectid": 18728, "filename": "preview.png", "mime_type": "image/png", "hash": "a5e1ea35153767b1981868d2d53e8cf5", "hash_type": "MD5", "filesize": 10784, "mtime": "2012-12-26 02:36:56", "url": "/1291/2/preview.png" } ], "eprint_id": 1291, "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/1958" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/1958" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/1958" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/12/91", "datestamp": "2008-04-08", "lastmod": "2021-04-16 22:55:51", "status_changed": "2009-09-25 02:00:29", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Liu-Q", "name": { "family": "Liu", "given": "Qianli" }, "show_email": "NO" } ] }, "title": "Femtosecond real-time dynamics of solvation : molecular reactions in clusters and supercritical fluids", "ispublished": "unpub", "full_text_status": "public", "abstract": "This thesis presents two distinct applications of femtosecond laser spectroscopy combined with molecular dynamics (MD) simulations. The first application is the study of the dissociation and geminate recombination dynamics of iodine in argon clusters. By using different size distributions of the clusters in a molecular beam, and tuning the central frequencies of the pump and probe beams, the dynamics over a wide range of energies, states and reaction coordinates have been resolved. A microscopic picture of solvation has been established. The MD simulations in this study have covered the femtosecond to picosecond time scales which are essential for characterizing the evolution of solvation and its equilibration in clusters. The second application is the study of vibrational energy and phase relaxation dynamics of iodine in the gas-to-liquid transition region of rare gases (He, Ne, and Ar). The pressure of the system has been continuously varied from 0 to 4000 bar, allowing the relaxation dynamics to be examined across a wide dynamic range. The usual near-linear density dependence has been found for the energy relaxation rate, while a striking non-linear behavior with density has been discovered for the dephasing rate. The MD simulations in this study adopted both a classical model and a semi-classical model, and have reproduced the experimental observations. The novel density dependence of the dephasing rate is attributed to the combined influence of the solute-solvent forces and the vibration-rotation couplings which have opposite trends with density in the intermediate and high density regimes.\n", "date": "1997", "date_type": "degree", "id_number": "CaltechETD:etd-04072008-091702", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04072008-091702", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-04-08", "doi": "10.7907/adkg-dg69", "divisions": { "items": [ "div_pma" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "chair" }, { "id": "Tombrello-T-A", "name": { "family": "Tombrello", "given": "Thomas A." }, "role": "member" }, { "id": "McKoy-B-V", "name": { "family": "McKoy", "given": "Basil Vincent" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-04-07", "thesis_defense_date": "1996-08-12", "thesis_approved_date": "2008-04-08", "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": "1997", "author_list": "Liu, Qianli", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Zewail, Ahmed H.; Tombrello, Thomas A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1311", "eprint_id": 1311, "rev_number": 11, "documents": [ { "id": "/id/document/1996", "doc_id": 1996, "rev_number": 3, "files": [ { "id": "/id/file/12477", "fileid": 12477, "datasetid": "document", "objectid": 1996, "filename": "Herek_jl_1996.pdf", "mime_type": "application/pdf", "filesize": 7629447, "mtime": "2012-12-26 02:37:08", "url": "/1311/1/Herek_jl_1996.pdf" } ], "eprint_id": 1311, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Herek_jl_1996.pdf", "language": "en", "security": "public", "license": "other", "main": "Herek_jl_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/18766" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/18766" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/18766" } ] } }, { "id": "/id/document/18766", "doc_id": 18766, "rev_number": 3, "files": [ { "id": "/id/file/12475", "fileid": 12475, "datasetid": "document", "objectid": 18766, "filename": "preview.png", "mime_type": "image/png", "hash": "bb8d57559ffa0433145b3dad5b519f90", "hash_type": "MD5", "filesize": 11434, "mtime": "2012-12-26 02:37:08", "url": "/1311/2/preview.png" } ], "eprint_id": 1311, "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/1996" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/1996" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/1996" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/13/11", "datestamp": "2008-04-08", "lastmod": "2021-04-16 23:09:03", "status_changed": "2009-09-25 02:01:01", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Herek-J-L", "name": { "family": "Herek", "given": "Jennifer Lynn" }, "show_email": "NO" } ] }, "title": "Femtochemistry and reactive intermediates : application to atmospheric and organic chemistry", "ispublished": "unpub", "full_text_status": "public", "keywords": "chemistry", "abstract": "The logical sequence of primary steps in a reaction mechanism is governed by the reactive intermediates which are postulated to ensure smooth transformations between stable species. Historically, such constructs were merely hypothetical as their (assumed) extreme reactivity and/or unstable nature precluded their observation. The introduction of femtosecond lasers to chemistry has allowed insight and understanding to many fundamental processes in reaction dynamics. This thesis presents applications of femtosecond spectroscopy to atmospheric and organic chemistry, specifically probing the reactive intermediates mediating various chemical transformations. Direct observation of these fleeting species can validate previously proposed mechanisms as well as offer new perspectives to their reaction dynamics.\r\n\r\nStudies of diradicals, the molecular species hypothesized to be archetypal of chemical bond transformations in many reactions in organic chemistry, have been made using femtosecond laser techniques combined with mass spectrometry in a molecular beam. Evolution of the diradical intermediate is monitored in real time throughout the course of the chemical reaction. These studies offer the first direct evidence of singlet 1,3- and 1,4-diradicals.\r\n\r\nHydrogen-atom transfer processes are fundamental to many reactions in organic chemistry. The dynamics of the motion may be localized, with little nuclear motion aside from the H-atom transfer between two \"anchors,\" or may be global, involving a multidimensional potential. Using methyl salicylate as a prototype system, direct studies of the nuclear motion in this important transformation are made with femtosecond resolution.\r\n\r\nMany reactive intermediates have been linked to stratospheric ozone depletion in recent years. In particular, catalytic cycles involving halogens are considered critical to establishing the overall mechanism for ozone depletion. Direct studies of the photochemically-activated dissociation of key species in atmospheric chemistry can offer insight to the global dynamics by providing important rate constants and branching ratios. Femtosecond reaction dynamics of OClO in a supersonic molecular beam are reported. The observations reveal the nuclear motions and couplings between potential energy surfaces relevant to the dissociation process. Comparisons with results of ab initio calculations are made.\r\n", "date": "1996", "date_type": "degree", "id_number": "CaltechETD:etd-04082008-084916", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04082008-084916", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-04-08", "doi": "10.7907/qj6m-w225", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "name": { "family": "Unknown", "given": "Unknown" } } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-04-08", "thesis_defense_date": "1996-06-06", "thesis_approved_date": "2008-04-08", "thesis_awards": "The Herbert Newby McCoy Award, 1996", "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": "1996", "author_list": "Herek, Jennifer Lynn", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Unknown, Unknown" }, { "id": "https://thesis.library.caltech.edu/id/eprint/1293", "eprint_id": 1293, "rev_number": 10, "documents": [ { "id": "/id/document/1960", "doc_id": 1960, "rev_number": 3, "files": [ { "id": "/id/file/12266", "fileid": 12266, "datasetid": "document", "objectid": 1960, "filename": "Pedersen_s_1996.pdf", "mime_type": "application/pdf", "filesize": 13247794, "mtime": "2012-12-26 02:36:56", "url": "/1293/1/Pedersen_s_1996.pdf" } ], "eprint_id": 1293, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Pedersen_s_1996.pdf", "language": "en", "security": "public", "license": "other", "main": "Pedersen_s_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/18730" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/18730" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/18730" } ] } }, { "id": "/id/document/18730", "doc_id": 18730, "rev_number": 3, "files": [ { "id": "/id/file/12264", "fileid": 12264, "datasetid": "document", "objectid": 18730, "filename": "preview.png", "mime_type": "image/png", "hash": "c43b1918ef2eca67ccc749a5461bd4f8", "hash_type": "MD5", "filesize": 9199, "mtime": "2012-12-26 02:36:56", "url": "/1293/2/preview.png" } ], "eprint_id": 1293, "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/1960" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/1960" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/1960" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/12/93", "datestamp": "2008-04-08", "lastmod": "2021-04-20 22:18:51", "status_changed": "2009-09-25 02:00:32", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Pedersen-S\u00f8ren", "name": { "family": "Pedersen", "given": "S\u00f8ren" }, "show_email": "NO" } ] }, "title": "Development and Applications of Techniques in Laser Femtochemistry", "ispublished": "unpub", "full_text_status": "public", "keywords": "Physics ; Femtochemistry", "abstract": "Femtosecond laser pulses provide the necessary time resolution to study fundamental dynamics of chemical reactions at the temporal scale of atomic resolution. New experimental techniques are introduced to the field of laser femtochemistry to generalize the range of accessible systems and further the understanding of molecular dynamics. In addition, theoretical models are developed that complement the experimental results and form the required basis for the interpretation of ultrafast measurements. The combination of multiphoton ionization with mass spectrometry and femtosecond lasers is introduced to isolate the elementary steps of reactions, differentiating parent and intermediate species and establishing the time scale for their dynamics. In two examples, using this approach, the direct real-time detection of diradical intermediates was made, and in another study the stepwise nature of a process initiated by the Norrish Type-I alfa-cleavage of acetone was revealed. This technique was also employed in the direct observation of vibrational motion in the transition state of a reaction (stilbene isomerization). The kinetic-energy time-of-flight (KETOF) method is developed to describe anisotropy and rotational alignment in the transition-state region and is applied to the dissociation of HgI2. An extension of the pump-probe scheme is made using the non-linear optical technique of femtosecond degenerate four-wave-mixing (DFWM) and application is made to the study of gas phase reaction dynamics of uni-(NaI) and bi-molecular (NaH2) systems. A detailed theoretical description of femtosecond transition-state dynamics is provided and illustrated via numerous examples. A kinetic model is developed, describing molecular response functions for ionization, fluorescence, depletion and absorption measurements. Effects of pulse width and saturation are discussed and comparison is made to classical and quantum mechanical models.", "date": "1996", "date_type": "degree", "id_number": "CaltechETD:etd-04072008-130051", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04072008-130051", "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": "2008-04-08", "doi": "10.7907/7q2y-1p50", "divisions": { "items": [ "div_pma" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "name": { "family": "Unknown", "given": "Unknown" } } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-04-07", "thesis_defense_date": "1996-02-05", "thesis_approved_date": "2008-04-08", "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": "Pedersen, S\u00f8ren", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Unknown, Unknown" }, { "id": "https://thesis.library.caltech.edu/id/eprint/5072", "eprint_id": 5072, "rev_number": 10, "documents": [ { "id": "/id/document/8044", "doc_id": 8044, "rev_number": 3, "files": [ { "id": "/id/file/49502", "fileid": 49502, "datasetid": "document", "objectid": 8044, "filename": "Heikal_aa_1996.pdf", "mime_type": "application/pdf", "filesize": 10725002, "mtime": "2012-12-26 03:14:31", "url": "/5072/1/Heikal_aa_1996.pdf" } ], "eprint_id": 5072, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Heikal_aa_1996.pdf", "language": "en", "security": "public", "license": "other", "main": "Heikal_aa_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/24551" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/24551" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/24551" } ] } }, { "id": "/id/document/24551", "doc_id": 24551, "rev_number": 3, "files": [ { "id": "/id/file/49500", "fileid": 49500, "datasetid": "document", "objectid": 24551, "filename": "preview.png", "mime_type": "image/png", "hash": "5cda467579aa52a1440391518efb166a", "hash_type": "MD5", "filesize": 8412, "mtime": "2012-12-26 03:14:31", "url": "/5072/2/preview.png" } ], "eprint_id": 5072, "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/8044" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/8044" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/8044" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/50/72", "datestamp": "2008-01-23", "lastmod": "2021-04-19 22:33:40", "status_changed": "2009-09-25 03:32:18", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Heikal-A-A", "name": { "family": "Heikal", "given": "Ahmed Abdou" }, "show_email": "NO" } ] }, "title": "Ultrafast molecular dynamics in complexed trans-stilbene", "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.\n\nUltrafast molecular dynamics in large molecular systems have been studied using either pump/probe time-of-flight mass spectrometry, or laser-induced fluorescence with time-correlated single photon counting technique. Intramolecular vibrational energy redistribution (IVR) and photoisomerization reaction in alkane-solvated and substituted trans-stilbenes are presented. Absent, restricted, and dissipative IVR were identified in stilbene-hexane[...] van der Waals complex. The dramatic increase of the density of states upon hexane solvation shifts the threshold for an efficient IVR to much lower excess-energy (~300 [...] for the dissipative regime) in comparison with the bare molecule (~1170 [...]). The effects of symmetry, density of states, and number of atoms on IVR were studied by using 4-methoxystilbene, 4,4'-dimethoxystilbene, and 2-phenylindene as model systems. The solvation and structural effects on the isomerization reaction in trans-stilbene is even more dramatic. For the first time, the lowering of the isomerization barrier (~700\u00b1100 [...]) in trans-stilbene upon one-hexane complexation is observed experimentally upon and compared with that in the bare molecule (~1250\u00b1100 [...]). Furthermore, the isomerization rate above the barrier in stilbene-(hexane)[...] complex is slightly slower than that in bare trans-stilbene. As the excess-vibrational energy exceeds the calculated binding energy of the (1:1) complex, the vibrational predissociation channel become open and was accounted for by using a simple kinetic model. Further decrease in the isomerization rate in stilbene-hexane[...] clusters was observed as the number of solvent molecules [...] increases. As the cluster size increases, the rate becomes less dependent on the excess energy in the [...]-state and the separation of the barrier must await theoretical calculations. The solvent polarity (in stilbene-hexanenitrile[...] complexes) and isotope effects (in stilbene-hexane-[...] complex) on the overall isomerization reaction were also examined. Similar studies were carried out on stilbene-(ethane)[...] clusters which has a lower binding energy than stilbene-(hexane)[...] clusters which, in turn, make the fragmentation of the cluster more severe. On the other hand, interesting observations were made on the reaction dynamics in a designed set of substituted stilbenes. 4-Methoxystilbene, 4,4'-dimethoxystilbene, 4,4'-dihydroxystilbene, trans-[beta]-1-cyclohexene-styrene and 2-phenylindene were used as model systems to study the role of electron conjugation and the torsional motion around [...]-[...] single bond in the isomerization reaction in trans-stilbene.\n", "date": "1996", "date_type": "degree", "id_number": "CaltechETD:etd-12192007-150129", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-12192007-150129", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-01-23", "doi": "10.7907/p3gz-kj57", "divisions": { "items": [ "div_eng" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "chair" }, { "id": "Culick-F-E-C", "name": { "family": "Culick", "given": "Fred E. C." }, "role": "member" }, { "id": "Corngold-N-R", "name": { "family": "Corngold", "given": "Noel Robert" }, "role": "member" }, { "id": "Marcus-R-A", "name": { "family": "Marcus", "given": "Rudolph A." }, "role": "member" }, { "id": "McKoy-B-V", "name": { "family": "McKoy", "given": "Basil Vincent" }, "role": "member" }, { "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": "2007-12-19", "thesis_defense_date": "1995-08-28", "thesis_approved_date": "2008-01-23", "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": "1996", "author_list": "Heikal, Ahmed Abdou", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Zewail, Ahmed H.; Culick, Fred E. C.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1270", "eprint_id": 1270, "rev_number": 8, "documents": [ { "id": "/id/document/1930", "doc_id": 1930, "rev_number": 3, "files": [ { "id": "/id/file/12056", "fileid": 12056, "datasetid": "document", "objectid": 1930, "filename": "Willberg_dm_1994.pdf", "mime_type": "application/pdf", "filesize": 7193657, "mtime": "2012-12-26 02:36:47", "url": "/1270/1/Willberg_dm_1994.pdf" } ], "eprint_id": 1270, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Willberg_dm_1994.pdf", "language": "en", "security": "public", "license": "other", "main": "Willberg_dm_1994.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/18700" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/18700" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/18700" } ] } }, { "id": "/id/document/18700", "doc_id": 18700, "rev_number": 3, "files": [ { "id": "/id/file/12054", "fileid": 12054, "datasetid": "document", "objectid": 18700, "filename": "preview.png", "mime_type": "image/png", "hash": "cf3c0abadbd7441d7fec8b8c679e9095", "hash_type": "MD5", "filesize": 8345, "mtime": "2012-12-26 02:36:47", "url": "/1270/2/preview.png" } ], "eprint_id": 1270, "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/1930" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/1930" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/1930" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/12/70", "datestamp": "2008-04-04", "lastmod": "2021-04-16 23:11:38", "status_changed": "2009-09-25 02:00:02", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Willberg-D-M", "name": { "family": "Willberg", "given": "Dean Michael" }, "show_email": "NO" } ] }, "title": "Picosecond spectroscopy of van der Waals clusters", "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.\n\nThis thesis presents pump/probe picosecond spectroscopic investigations of the dynamics of van der Waals clusters. The first phase of these investigations was the construction of a laboratory specifically designed for van der Waals cluster research consisting of a molecular beam apparatus and a two-color picosecond laser system. It is possible to perform both time resolved laser induced fluorescence (LE), and multi-photon ionization (MPI) experiments in this laboratory. A description of the construction and operation of the laboratory, focusing on the laser system, is presented. A full account of the real-time studies of the vibrational predissociation of [...] clusters where [...] is given. The first set of experiments described is the measurement of the rates of vibrational predissociation for [...] clusters. The results for [...] are compared with a number of theoretical models of vibrational predissociation, specifically focusing on the dependence of the rates on the initially prepared vibrational state of the cluster. The results for the [...] cluster are described in terms of the competition between two relaxation channels: vibrational predissociation of the van der Waals cluster, and electronic predissociation of the [...] moiety. The second set of experiments are the analogous measurements of the rates of vibrational predissociation of [...] clusters. These results are compared with the [...] results, as well as with lifetime estimates available from high resolution spectroscopy. The final chapter in this series describes our investigation of vibrational predissociation and intramolecular vibrational energy relaxation in [...] clusters. The dynamics of these larger clusters are inherently more complicated than when n = 1, however, a quantitative model for the fragmentation of n = 2 clusters is presented. This thesis also presents a preliminary description of an ongoing MPI experiment on the dynamics of t-stilbene clusters.", "date": "1994", "date_type": "degree", "id_number": "CaltechETD:etd-04042008-110156", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04042008-110156", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-04-04", "doi": "10.7907/605h-j578", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "name": { "family": "Unknown", "given": "Unknown" } } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-04-04", "thesis_defense_date": "1993-07-09", "thesis_approved_date": "2008-04-04", "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": "1994", "author_list": "Willberg, Dean Michael", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Unknown, Unknown" }, { "id": "https://thesis.library.caltech.edu/id/eprint/1271", "eprint_id": 1271, "rev_number": 8, "documents": [ { "id": "/id/document/1931", "doc_id": 1931, "rev_number": 3, "files": [ { "id": "/id/file/12063", "fileid": 12063, "datasetid": "document", "objectid": 1931, "filename": "Potter_ed_1993.pdf", "mime_type": "application/pdf", "filesize": 9974696, "mtime": "2012-12-26 02:36:47", "url": "/1271/1/Potter_ed_1993.pdf" } ], "eprint_id": 1271, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Potter_ed_1993.pdf", "language": "en", "security": "public", "license": "other", "main": "Potter_ed_1993.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/18701" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/18701" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/18701" } ] } }, { "id": "/id/document/18701", "doc_id": 18701, "rev_number": 3, "files": [ { "id": "/id/file/12061", "fileid": 12061, "datasetid": "document", "objectid": 18701, "filename": "preview.png", "mime_type": "image/png", "hash": "8617597b26dd6b79c1a69907199688a0", "hash_type": "MD5", "filesize": 8852, "mtime": "2012-12-26 02:36:47", "url": "/1271/2/preview.png" } ], "eprint_id": 1271, "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/1931" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/1931" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/1931" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/12/71", "datestamp": "2008-04-04", "lastmod": "2021-04-16 23:10:59", "status_changed": "2009-09-25 02:00:02", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Potter-E-D", "name": { "family": "Potter", "given": "Earl Douglas" }, "show_email": "NO" } ] }, "title": "Ultrafast control and dynamics of chemical reactions", "ispublished": "unpub", "full_text_status": "public", "abstract": "This thesis presents four distinct applications of ultrafast laser spectroscopy. Unimolecular photodissociation was one of the early applications of this technique and proved to be invaluable in furthering the understanding of unimolecular dissociation mechanisms. As such, the photodissociation of ketene represents one of the two systems where micro-canonical, state-to-state reaction rates, have been measured. Clocking of bimolecular reactions, while still in its infancy, provides a means of measuring the rate at which an elementary reaction actually occurs--isolated from other molecules. The rate at which the bimolecular reaction of bromine atoms with molecular iodine to form iodine monobromide has been measured at two collision energies. An area where ultrafast techniques are just now seeing application, is control of chemical reactions. This thesis illustrates an initial study, albeit limited, of how ultrashort light pulses can be used to \"control\" the outcome of a chemical reaction. The experiments here show how the natural wave-packet motion of the initially prepared B state iodine can be used to \"control\" whether or not xenon iodide is formed even when the necessary photons are available. Finally, cluster science is becoming a mature field within physical chemistry, but one of the goals of such work has been to make a connection between gas-phase studies and condensed-phase work. Small clusters, those not large enough to bridge this gap, have proven sufficiently interesting to monopolize the efforts of many groups. Again in a limited way, we have begun to study large clusters in the hope that these systems will truly show characteristics that are somehow intermediate to the gas-phase and condensed-phase characteristics. A dissociating iodine molecule surrounded by many argon atoms encounters an environment that significantly alters the time scales and overall mechanism for separation of the two iodine atoms.\n\nWork done under the direction of Professor Ahmed H. Zewail.\n", "date": "1993", "date_type": "degree", "id_number": "CaltechETD:etd-04042008-113817", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04042008-113817", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-04-04", "doi": "10.7907/k9hx-hh19", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "name": { "family": "Unknown", "given": "Unknown" } } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-04-04", "thesis_defense_date": "1993-03-10", "thesis_approved_date": "2008-04-04", "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": "1993", "author_list": "Potter, Earl Douglas", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Unknown, Unknown" }, { "id": "https://thesis.library.caltech.edu/id/eprint/1262", "eprint_id": 1262, "rev_number": 8, "documents": [ { "id": "/id/document/1908", "doc_id": 1908, "rev_number": 3, "files": [ { "id": "/id/file/11969", "fileid": 11969, "datasetid": "document", "objectid": 1908, "filename": "Cong_p_1992.pdf", "mime_type": "application/pdf", "filesize": 5226807, "mtime": "2012-12-26 02:36:43", "url": "/1262/1/Cong_p_1992.pdf" } ], "eprint_id": 1262, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Cong_p_1992.pdf", "language": "en", "security": "public", "license": "other", "main": "Cong_p_1992.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/18687" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/18687" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/18687" } ] } }, { "id": "/id/document/18687", "doc_id": 18687, "rev_number": 3, "files": [ { "id": "/id/file/11967", "fileid": 11967, "datasetid": "document", "objectid": 18687, "filename": "preview.png", "mime_type": "image/png", "hash": "d719f1ed37bb4cefc9fd14cc8ec4b6ac", "hash_type": "MD5", "filesize": 8080, "mtime": "2012-12-26 02:36:43", "url": "/1262/2/preview.png" } ], "eprint_id": 1262, "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/1908" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/1908" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/1908" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/12/62", "datestamp": "2008-04-08", "lastmod": "2021-04-16 23:22:25", "status_changed": "2009-09-25 01:59:43", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Cong-P", "name": { "family": "Cong", "given": "Peijun" }, "show_email": "NO" } ] }, "title": "Femtosecond photodissociation dynamics of alkali halides", "ispublished": "unpub", "full_text_status": "public", "abstract": "Femtosecond transition-state spectroscopy (I. S) is a time-resolved spectroscopic technique by which the real time dynamics of the transition state of a chemical reaction can be studied with femtosecond resolution. This technique has been applied to study a number of chemical reactions. This thesis presents one such system, the photodissociation of alkali halides, and that of NaI in particular.\n\nUpon excitation to the covalent state, the alkali halide molecule will encounter a curve crossing during its way to dissociation. This curve-crossing phenomenon manifests itself in the dynamics of the photodissociation process. Experimentally, wave-packet trapping and leaking that are due to the curve crossing are observed. Taking full advantage of the femtosecond resolution offered by the FTS technique, the wave-packet dephasing dynamics is separated from the population decay. The Landau-Zener coupling-matrix element is also obtained from the time-resolved data, which is in close agreement with previous literature values. Furthermore, the combination of the temporal resolution and the spectral resolution of the FTS methodology allows the wave-packet motion to be monitored at a specific internuclear separation, which covers a wide range of distances. This feature of the FTS technique makes the mapping of reaction trajectories possible. A classical mechanics-based inversion procedure is then developed to obtain the relevant potential- energy curves involved in the photodissociation reaction from the results of such trajectory mapping experiments. The potentials inverted this way are tested by quantum dynamical simulation and compared with those obtained by other workers from different techniques. The long-time behavior of the wave-packet motion after many oscillations is also discussed.", "date": "1992", "date_type": "degree", "id_number": "CaltechETD:etd-04032008-154309", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04032008-154309", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-04-08", "doi": "10.7907/w8dq-ee77", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "name": { "family": "Unknown", "given": "Unknown" } } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-04-03", "thesis_defense_date": "1991-09-17", "thesis_approved_date": "2008-04-08", "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": "1992", "author_list": "Cong, Peijun", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Unknown, Unknown" }, { "id": "https://thesis.library.caltech.edu/id/eprint/1272", "eprint_id": 1272, "rev_number": 8, "documents": [ { "id": "/id/document/1932", "doc_id": 1932, "rev_number": 3, "files": [ { "id": "/id/file/12070", "fileid": 12070, "datasetid": "document", "objectid": 1932, "filename": "Peng_lw_1991.pdf", "mime_type": "application/pdf", "filesize": 13522821, "mtime": "2012-12-26 02:36:47", "url": "/1272/1/Peng_lw_1991.pdf" } ], "eprint_id": 1272, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Peng_lw_1991.pdf", "language": "en", "security": "public", "license": "other", "main": "Peng_lw_1991.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/18702" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/18702" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/18702" } ] } }, { "id": "/id/document/18702", "doc_id": 18702, "rev_number": 3, "files": [ { "id": "/id/file/12068", "fileid": 12068, "datasetid": "document", "objectid": 18702, "filename": "preview.png", "mime_type": "image/png", "hash": "cd85d0eceace5f86223ca14acc424f76", "hash_type": "MD5", "filesize": 10459, "mtime": "2012-12-26 02:36:47", "url": "/1272/2/preview.png" } ], "eprint_id": 1272, "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/1932" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/1932" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/1932" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/12/72", "datestamp": "2008-04-04", "lastmod": "2021-04-16 23:16:36", "status_changed": "2009-09-25 02:00:03", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Peng-L-W", "name": { "family": "Peng", "given": "Lawrence Weiman" }, "show_email": "NO" } ] }, "title": "Reactions in small clusters studied by time-resolved laser spectroscopy", "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.\n\nMolecular solute/solvent clusters are an ideal medium for studying solvent effects from the van der Waals complex to the solution bulk limit. Such clusters are conveniently produced using molecular beams. Thus, a new apparatus for making time-resolved measurements of large neutral clusters was constructed and is described in detail herein. The apparatus consists of a molecular beam interrogated by two picosecond lasers. Detection is by laser-induced fluorescence and resonance-enhanced multiphoton ionization. The laser and molecular beam combination permits the study of the role of solvation on the solute's excited electronic-state dynamics for a specific cluster size.\n\nPicosecond time-resolved laser spectroscopy is applied to neutral solute/solvent clusters to study the effect of solvation on charge-transfer reactions in real-time. p(Dimethylamino)benzonitrile (4-DMABN) and [...]-naphthol ([...]-NpOH) are used as model systems since the charge-transfer is solvent dependent. The S[...] excited state dynamics of gas-phase 4-DMABN has been studied both in a supersonic jet expansion and in a thermalized vapor. The jet studies show that 1:1 complexes with water, ammonia, methanol, and acetonitrile do not undergo charge-transfer. At higher jet temperatures, emission is observed from 4-DMABN self-complexes. Charge-transfer fluorescence from 4-DMABN self-complexes is observed in a thermalized vapor. Studies have been done on the S[...] excited state dynamics of gas phase [...]-NpOH clustered with ammonia, piperidine and water. The measurements reveal cluster-size dependent dynamics for [...]-NpOH clustered with ammonia and piperidine, but not with water. The fast-time dynamics in the ammonia and piperidine clusters indicates the occurrence of proton-transfer reactions in these solute/solvent clusters. The cluster size, solvent dependence and the timescale for the reactions serve to emphasize the importance of the local solvent environment.\n", "date": "1991", "date_type": "degree", "id_number": "CaltechETD:etd-04042008-130407", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04042008-130407", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-04-04", "doi": "10.7907/3cw7-7w07", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "name": { "family": "Unknown", "given": "Unknown" } } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-04-04", "thesis_defense_date": "1990-10-01", "thesis_approved_date": "2008-04-04", "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": "1991", "author_list": "Peng, Lawrence Weiman", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Unknown, Unknown" }, { "id": "https://thesis.library.caltech.edu/id/eprint/2661", "eprint_id": 2661, "rev_number": 9, "documents": [ { "id": "/id/document/4961", "doc_id": 4961, "rev_number": 3, "files": [ { "id": "/id/file/28801", "fileid": 28801, "datasetid": "document", "objectid": 4961, "filename": "Dantus_m_1991.pdf", "mime_type": "application/pdf", "filesize": 11301013, "mtime": "2012-12-26 02:53:26", "url": "/2661/1/Dantus_m_1991.pdf" } ], "eprint_id": 2661, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Dantus_m_1991.pdf", "language": "en", "security": "public", "license": "other", "main": "Dantus_m_1991.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/21511" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/21511" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/21511" } ] } }, { "id": "/id/document/21511", "doc_id": 21511, "rev_number": 3, "files": [ { "id": "/id/file/28799", "fileid": 28799, "datasetid": "document", "objectid": 21511, "filename": "preview.png", "mime_type": "image/png", "hash": "9fa5dc855126ab005cdfa4ff6dd88980", "hash_type": "MD5", "filesize": 9110, "mtime": "2012-12-26 02:53:26", "url": "/2661/2/preview.png" } ], "eprint_id": 2661, "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/4961" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/4961" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/4961" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/26/61", "datestamp": "2007-07-16", "lastmod": "2021-04-16 22:23:26", "status_changed": "2009-09-25 02:42:40", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Dantus-M", "name": { "family": "Dantus", "given": "Marcos" }, "show_email": "NO" } ] }, "title": "Femtosecond transition-state spectroscopy of chemical reactions", "ispublished": "unpub", "full_text_status": "public", "keywords": "chemistry", "abstract": "The field of molecular dynamics emerged in the beginning of this century with the goal of understanding chemical reactions at the molecular level. The main interest was to study elementary processes such as bond rupture and bond formation as they occur on isolated molecules. Progress in that field has been directly related to technological advances. The development of the cross molecular beam techniques, for example, allowed the first observations of single molecule reactive collisions. Since the early experiments, it was recognized that the elementary steps in chemistry occurred on the time scale of a single vibration, many thought they might be unmeasurably fast. This thesis presents the first real-time observations of elementary chemical processes occurring on dissociative and bound potentials with a time resolution of 10(-14) s.\r\n\r\nThe technique for achieving real-time monitoring of chemical reactions is Femtosecond Transition-State Spectroscopy (FTS). In essence, it involves two femtosecond (10(-15) s) laser pulses; one to initiate the reaction and the second to probe the progress at subsequent times. In addition to the time delay between the two pulses, the experiments include different wavelengths for the pump and probe pulses. The collection of data scans as a function of time delay for each combination of pump and probe wavelengths provides sufficient information about the dynamics to allow inversion to the potential energy surface of the reaction. The potential energy surface then contains all information about the reaction.\r\n\r\nThe FTS technique has been applied with success to several systems. For repulsive states, such as the dissociation reaction of ICN, it has yielded a direct clocking of the bond rupture process and the real-time observation of transition states. For bound and quasi-bound states, the technique has allowed the real-time observation of wave packet oscillation in alkali-halides, halogens and inter-halogens. The technique has been applied to more than one dimensional systems such as HgI2. In addition to the scalar quantities, FTS has also been successful in the measurement of vectorial quantities such as the angular momentum and torque during dissociation reactions. Of all these, and many other measurements under different conditions, only a few representative examples are discussed here. The technique is now well established and it has become an important tool for the study of molecular dynamics on bound and repulsive potential energy surfaces.", "date": "1991", "date_type": "degree", "id_number": "CaltechETD:etd-06202007-112232", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-06202007-112232", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2007-07-16", "doi": "10.7907/6aam-8f30", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "name": { "family": "Unknown", "given": "Unknown" } } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2007-06-20", "thesis_defense_date": "1990-12-07", "thesis_approved_date": "2007-07-16", "thesis_awards": "The Herbert Newby McCoy Award, 1991", "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": "1991", "author_list": "Dantus, Marcos", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Unknown, Unknown" }, { "id": "https://thesis.library.caltech.edu/id/eprint/4660", "eprint_id": 4660, "rev_number": 18, "documents": [ { "id": "/id/document/7523", "doc_id": 7523, "rev_number": 3, "files": [ { "id": "/id/file/45994", "fileid": 45994, "datasetid": "document", "objectid": 7523, "filename": "Baskin_js_1990.pdf", "mime_type": "application/pdf", "filesize": 13957065, "mtime": "2012-12-26 03:10:45", "url": "/4660/1/Baskin_js_1990.pdf" } ], "eprint_id": 4660, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Original (no OCR) Baskin_js_1990.pdf", "language": "en", "security": "internal", "license": "other", "main": "Baskin_js_1990.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/24042" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/24042" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/24042" } ] } }, { "id": "/id/document/15685", "doc_id": 15685, "rev_number": 5, "files": [ { "id": "/id/file/204409", "fileid": 204409, "datasetid": "document", "objectid": 15685, "filename": "Baskin_John_Spencer_1990.txt", "mime_type": "text/plain", "filesize": 1946, "mtime": "2016-08-22 21:17:30", "url": "/4660/2/Baskin_John_Spencer_1990.txt" } ], "eprint_id": 4660, "pos": 2, "format": "text/plain", "language": "en", "security": "internal", "license": "other", "main": "Baskin_John_Spencer_1990.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", 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"thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "baskin@caltech.edu", "id": "Baskin-John-Spencer", "name": { "family": "Baskin", "given": "John Spencer" }, "show_email": "YES" } ] }, "title": "Real-Time Observation and Analysis of Coherence and Alignment in Molecular Systems: Isolated Molecules and Chemical Reactions", "ispublished": "unpub", "full_text_status": "public", "keywords": "Applied Physics", "abstract": "Picosecond time-resolved rotational coherence spectroscopy is developed as a probe of excited state rotational level structure and alignment. The measurement technique employs a combination of supersonic cooling by molecular beam expansion, coherent picosecond pulsed laser excitation, and time-resolved and polarization-analyzed detection of spectrally dispersed fluorescence. The requisite measurement system response time of approximately 50 picoseconds is attained using time-correlated single photon counting and a microchannel plate detector.
\r\n\r\nIn the case of purely rotational coherence (PRC), i.e., when rotation may be treated in the rigid rotor approximation, analysis of the polarization-analyzed fluorescence provides direct information about the rotational constants and structure of the molecule's excited vibronic state. This method of structural determination of excited states has the inherent advantages over conventional frequency-domain spectroscopy of sub-Doppler resolution and insensitivity to ground state structure. As a result, it is particularly valuable in investigations of large molecules and complexes. Analyses of PRC measurements on eight different molecular systems are detailed in this thesis. These provide illustrative examples of various aspects of the technique while permitting the derivation of new information about the excited states of six of the eight molecules or complexes studied. Principal among the findings are values of the sum of rotational constants B' and C' of the t-stilbene S\u2081 electronic state (B'+ C' = 0.5132 \u00b1 .0008 GHz) and of all three S\u2081 rotational constants of anthracene.
\r\n\r\nWe also report measurements of time-resolved and polarization-analyzed fluorescence as a function of excess vibrational energy in the S\u2081 electronic states of both t-stilbene and anthracene. We are able to distinguish the contribution of purely rotational coherence from the contributions of purely vibrational (or rovibrational) coherence to the evolution of fluorescence from the vibrationally excited molecule. Our results provide a test of the extent of coupling between vibrational and rotational motion and its influence on intramolecular vibrational energy redistribution.
\r\n\r\nMeasurements of polarization-analyzed fluorescence of dissociation products demonstrate that rotational coherence of the reagent can be transferred to its fragments. In order to interpret the results of these and related experiments, a classical model of fluorescence anisotropy in prompt, impulsive dissociation reactions is developed.
", "date": "1990", "date_type": "degree", "id_number": "CaltechETD:etd-11252003-112746", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-11252003-112746", "related_url": { "items": [ { "description": "Article adapted for Chapter 2, 3, 4, 5.", "type": "doi", "url": "https://doi.org/10.1063/1.452100" }, { "description": "Article adapted for Chapter 2, 3, 4, 5.", "type": "doi", "url": "https://doi.org/10.1021/j100352a014" }, { "description": "Article adapted for Appendix I.", "type": "doi", "url": "https://doi.org/10.1063/1.449998" } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "NSF", "grant_number": "DMR-8521191" }, { "agency": "ARCS Foundation" } ] }, "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "deposited_by": "Imported from ETD-db", "deposited_on": "2003-11-26", "doi": "10.7907/H8TF-EE69", "divisions": { "items": [ "div_eng" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" }, { "email": "pbellan@caltech.edu", "id": "Bellan-P-M", "name": { "family": "Bellan", "given": "Paul Murray" }, "orcid": "0000-0002-0886-8782", "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "zewail@caltech.edu", "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "chair" }, { "email": "nrdc@cco.caltech.edu", "id": "Corngold-N-R", "name": { "family": "Corngold", "given": "Noel Robert" }, "role": "member" }, { "email": "ram@caltech.edu", "id": "Marcus-R-A", "name": { "family": "Marcus", "given": "Rudolph A." }, "orcid": "0000-0001-6547-1469", "role": "member" }, { "email": "rwgould@caltech.edu", "id": "Gould-R-W", "name": { "family": "Gould", "given": "Roy Walter" }, "role": "member" }, { "email": "wag@wag.caltech.edu", "id": "Goddard-W-A-III", "name": { "family": "Goddard", "given": "William A., III" }, "orcid": "0000-0003-0097-5716", "role": "member" }, { "email": "pbellan@caltech.edu", "id": "Bellan-P-M", "name": { "family": "Bellan", "given": "Paul Murray" }, "orcid": "0000-0002-0886-8782", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2003-11-25", "thesis_defense_date": "1989-09-28", "thesis_approved_date": "2003-11-26", "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": "1990", "author_list": "Baskin, John Spencer", "advisor_list": "Zewail, Ahmed H. and Bellan, Paul Murray", "comittee_list": "Zewail, Ahmed H.; Corngold, Noel Robert; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1261", "eprint_id": 1261, "rev_number": 10, "documents": [ { "id": "/id/document/1907", "doc_id": 1907, "rev_number": 3, "files": [ { "id": "/id/file/11962", "fileid": 11962, "datasetid": "document", "objectid": 1907, "filename": "Semmes_dh_1990.pdf", "mime_type": "application/pdf", "filesize": 5532702, "mtime": "2012-12-26 02:36:42", "url": "/1261/1/Semmes_dh_1990.pdf" } ], "eprint_id": 1261, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Semmes_dh_1990.pdf", "language": "en", "security": "public", "license": "other", "main": "Semmes_dh_1990.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/18686" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/18686" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/18686" } ] } }, { "id": "/id/document/18686", "doc_id": 18686, "rev_number": 3, "files": [ { "id": "/id/file/11960", "fileid": 11960, "datasetid": "document", "objectid": 18686, "filename": "preview.png", "mime_type": "image/png", "hash": "3d15d492d0b8eaa46f3cf61cc70bc2b4", "hash_type": "MD5", "filesize": 9644, "mtime": "2012-12-26 02:36:42", "url": "/1261/2/preview.png" } ], "eprint_id": 1261, "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/1907" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/1907" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/1907" } ] } }, { "id": "/id/document/41323", "doc_id": 41323, "rev_number": 3, "files": [ { "id": "/id/file/125067", "fileid": 125067, "datasetid": "document", "objectid": 41323, "filename": "Semmes author permission to release june2013.txt", "mime_type": "message/rfc822\\0117bit", "hash": "e52b7edb27edfbb42e496b73695284a7", "hash_type": "MD5", "filesize": 2848, "mtime": "2013-06-07 21:08:21", "url": "/1261/3/Semmes author permission to release june2013.txt" } ], "eprint_id": 1261, "pos": 3, "placement": 3, "mime_type": "message/rfc822\\0117bit", "format": "text/plain", "format_desc": "author permission to release june 2013", "language": "en", "security": "internal", "license": "other", "main": "Semmes author permission to release june2013.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "release" } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/12/61", "datestamp": "2008-04-08", "lastmod": "2019-12-21 04:01:01", "status_changed": "2009-09-25 01:59:42", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "DSemmes@gmail.com", "id": "Semmes-D-H", "name": { "family": "Semmes", "given": "David Haynes" }, "show_email": "NO" } ] }, "title": "Picosecond studies of the vibrational predissociation of van der Waals complexes", "ispublished": "unpub", "full_text_status": "public", "keywords": "van der Waals complexes ; chemistry", "abstract": "The vibrational predissociation of several van der Waals complexes of aromatic molecules with rare gas atoms, isolated in a free-jet molecular beam expansion, has been studied using time-resolved spectroscopy. Direct measurements have been made, on a picosecond time scale, of the fluorescence intensity from the initially excited single vibrational level and from the various final vibrational states formed in the dissociation of the complexes. The time-resolved data is analyzed with the aid of different kinetic models and can distinguish between parallel decay paths, sequential paths with intramolecular vibrational redistribution (IVR) preceding vibrational predissociation, and sequential paths with reversible IVR preceding vibrational predissociation. The contribution of the van der Waals modes to the total vibrational state density induces dissipative IVR in the complexes at much lower energies than in the bare aromatic molecule. The measured predissociation rates are compared with rates calculated according to the statistical RRKM theory of unimolecular reactions. Some of the experimental results show mode-selective behavior, while other results suggest statistical behavior.", "date": "1990", "date_type": "degree", "id_number": "CaltechETD:etd-04032008-144110", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04032008-144110", "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": "2008-04-08", "doi": "10.7907/NTP7-RS50", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "name": { "family": "Unknown", "given": "Unknown" } } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-04-03", "thesis_defense_date": "1989-09-27", "thesis_approved_date": "2008-04-08", "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": "1990", "author_list": "Semmes, David Haynes", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Unknown, Unknown" }, { "id": "https://thesis.library.caltech.edu/id/eprint/4693", "eprint_id": 4693, "rev_number": 18, "documents": [ { "id": "/id/document/10724", "doc_id": 10724, "rev_number": 4, "files": [ { "id": "/id/file/204420", "fileid": 204420, "datasetid": "document", "objectid": 10724, "filename": "Scherer_nf_1989_no_UMI.pdf", "mime_type": "application/pdf", "filesize": 36336, "mtime": "2016-08-22 21:17:32", "url": "/4693/2/Scherer_nf_1989_no_UMI.pdf" } ], "eprint_id": 4693, "pos": 2, "format": "application/pdf", "format_desc": "NO UMI, per division", "language": "en", "security": "internal", "license": "other", "main": "Scherer_nf_1989_no_UMI.pdf", "media_duration": "0", "media_aspect_ratio": "0", 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"Scherer-Norbert-Franz", "name": { "family": "Scherer", "given": "Norbert Franz" }, "show_email": "YES" } ] }, "title": "Time-Resolved Studies of Molecular Reaction Dynamics and Development of Experimental Methodology", "ispublished": "unpub", "full_text_status": "public", "keywords": "Chemistry", "note": "Thesis file (PDF) missing pp. 157 and 170 (or original pagination incorrect); two pages labeled pp. 167.", "abstract": "The six research topics presented in the following chapters are concerned with several diverse problems of molecular reaction dynamics in isolated gas-phase environments. The scope of the studies ranges from performing direct measurements of bond-breakage on electronically dissociative potential energy surfaces, to monitoring the time-course of a restricted geometry bimolecular reaction. The common experimental method used in all of the studies has been a variant of pump-probe time-resolved spectroscopy. The underlying theme of the endeavors has been threefold: 1) To gain a better understanding of the role of intramolecular dynamics that precede or are commensurate with the reaction dynamics; 2) To begin to appreciatiate the observable manifestations of specific features of the reactive potential energy surface; and 3) To utilize the specific temporal behavior to elucidate quantitative information for the said potential surface.
\r\n\r\nThe studies of molecular dissociation on repulsive electronic surfaces has lead to a quantification of the timescale for primary steps in reaction processes. Moreover, transform limited temporal/spectral studies have begun to focus on specific long-range reaction fragment interactions in a state-specific manner. The latter endeavor has identified a mechanism for the reaction-fragment(s) interaction in the near-asymptotic product region.
\r\n\r\nPredissociative reaction and intramolecular dynamical behavior has been studied on ground potential energy surfaces. Overtone excitation of the OH-stretch mode of hydrogen peroxide enables molecular ground state excitation and state-specific detection of the OH reaction product. These investigations point out the potential of this picosecond pump-probe method for directly elucidating the intramolecular energy redistribution process and the possibility for direct investigation of the long-range tail region of the free-radical recombination potential surface.
\r\n\r\nThe investigation of a spatially oriented bimolecular reaction has conclusively shown that the IH-OCO reaction proceeds by way of the [HOCO]\u2020 reaction complex species. The close proximity of the van der Waals bound reactants produces unique multi-body interactions not found in the gas phase but which may arise in condensed phases. Moreover, these investigations have obtained evidence for a unique reaction reasonance (which is analogous to a shape-resonance) feature. The presence of such a resonance in the reaction entrance channel region affects the temporal behavior and yield of product formation.
", "date": "1989", "date_type": "degree", "id_number": "CaltechETD:etd-11302006-091037", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-11302006-091037", "related_url": { "items": [ { "description": "Article adapted for Chapter III.", "type": "doi", "url": "https://doi.org/10.1021/j100270a001" }, { "description": "Article adapted for Chapter V.", "type": "doi", "url": "https://doi.org/10.1063/1.453529" }, { "description": "Article adapted for Appendix A.", "type": "doi", "url": "https://doi.org/10.1021/j100310a012" } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "deposited_by": "Imported from ETD-db", "deposited_on": "2006-12-18", "doi": "10.7907/5JGV-E964", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "ram@caltech.edu", "id": "Marcus-R-A", "name": { "family": "Marcus", "given": "Rudolph A." }, "orcid": "0000-0001-6547-1469", "role": "chair" }, { "email": "chans@its.caltech.edu", "id": "Chan-S-I", "name": { "family": "Chan", "given": "Sunney I." }, "orcid": "0000-0002-5348-2723", "role": "member" }, { "email": "weitekamp@caltech.edu", "id": "Weitekamp-D-P", "name": { "family": "Weitekamp", "given": "Daniel P." }, "role": "member" }, { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2006-11-30", "thesis_defense_date": "1989-01-23", "thesis_approved_date": "2006-12-18", "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": "1989", "author_list": "Scherer, Norbert Franz", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Marcus, Rudolph A.; Chan, Sunney I.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1269", "eprint_id": 1269, "rev_number": 16, "documents": [ { "id": "/id/document/1929", "doc_id": 1929, "rev_number": 3, "files": [ { "id": "/id/file/12049", "fileid": 12049, "datasetid": "document", "objectid": 1929, "filename": "Khundkar_lr_1988.pdf", "mime_type": "application/pdf", "filesize": 10292654, "mtime": "2012-12-26 02:36:46", "url": "/1269/1/Khundkar_lr_1988.pdf" } ], "eprint_id": 1269, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Original (no OCR) Khundkar_lr_1988.pdf", "language": "en", "security": "internal", "license": "other", "main": 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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/105801" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/105801" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/105801" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/12/69", "datestamp": "2008-04-04", "lastmod": "2021-04-16 23:05:51", "status_changed": "2009-09-25 02:00:01", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Khundkar-Lutfur-Rahman", "name": { "family": "Khundkar", "given": "Lutfur Rahman" }, "show_email": "NO" } ] }, "title": "Microcanonical Rates of Unimolecular Reactions Studied by Time-Resolved Photofragment Spectroscopy", "ispublished": "unpub", "full_text_status": "public", "keywords": "Chemistry", "abstract": "The use of modern technology in the study of classic problems in chemistry has afforded researchers the opportunity to understand the dynamics of reactions on a molecular level. This thesis represents one such instance, where the combination of pulsed lasers and molecular beams has made the study of ultrafast reactions of isolated molecules possible.
\r\n\r\nThe optical technique is, in essence, a two pulse pump-probe method. One of the pulses resonantly excites the molecule to be studied, while the second one, delayed in time, measures the population in either the excited parent state or some quantum state of the product. The sample is cooled in a supersonic expansion and observed under collisionless conditions. Atomic and molecular species may be detected by laser-induced fluorescence (LIF) or resonantly-enhanced multiphoton ionization (REMPI), followed by mass-selective detection. The temporal evolution of the state being probed is mapped out as the delay between the pulses is varied. The resolution of this method is determined by the temporal widths of the two pulses, typically ~ 8 picoseconds in the studies presented here.
\r\n\r\nThe technique, termed Time-Resolved Photofragment Spectroscopy (TRPS), has been used to study a number of unimolecular reactions under collisionless conditions. Microcanonical rates of the reaction NCNO \u2192 CN + NO have been measured for excitation energies near threshold. The rates are compared with predictions of various statistical theories, including a recently proposed variational method. State-selected studies of the production of iodine atoms in the UV photodissociation of 1,2\u2014diiodotetrafluoroethane indicate the existence of a bound intermediate, the iodoperfluoroethyl radical. Energy dependent rates show that the amount of internal energy in the intermediate may be varied by changing excitation conditions, thereby affecting the rate of its decomposition. Time and frequency-resolved studies of the photodissociation of methyl iodide show evidence that perturbed species in a dissociating system (so-called transition-state species) may be observed by this technique.
", "date": "1988", "date_type": "degree", "id_number": "CaltechETD:etd-04042008-083918", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04042008-083918", "related_url": { "items": [ { "description": "Article adapted for Chapter 5A.", "type": "doi", "url": "https://doi.org/10.1063/1.453527" }, { "description": "Article adapted for Chapter 7A.", "type": "doi", "url": "https://doi.org/10.1016/0009-2614(87)85137-0" }, { "description": "Article adapted for Appendix I.", "type": "doi", "url": "https://doi.org/10.1063/1.453608" }, { "description": "Article adapted for Appendix II.", "type": "doi", "url": "https://doi.org/10.1063/1.453280" } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-04-04", "doi": "10.7907/zfwr-rk30", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "ram@caltech.edu", "id": "Marcus-R-A", "name": { "family": "Marcus", "given": "Rudolph A." }, "role": "chair" }, { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "member" }, { "email": "dervan@caltech.edu", "id": "Dervan-P-B", "name": { "family": "Dervan", "given": "Peter B." }, "role": "member" }, { "email": "jhopfiel@caltech.edu", "id": "Hopfield-J-J", "name": { "family": "Hopfield", "given": "John J." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-04-04", "thesis_defense_date": "1988-05-06", "thesis_approved_date": "2008-04-04", "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": "1988", "author_list": "Khundkar, Lutfur Rahman", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Marcus, Rudolph A.; Zewail, Ahmed H.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1258", "eprint_id": 1258, "rev_number": 15, "documents": [ { "id": "/id/document/1904", "doc_id": 1904, "rev_number": 3, "files": [ { "id": "/id/file/11942", "fileid": 11942, "datasetid": "document", "objectid": 1904, "filename": "Keelan_bw_1986.pdf", "mime_type": "application/pdf", "filesize": 9037162, "mtime": "2012-12-26 02:36:42", "url": "/1258/1/Keelan_bw_1986.pdf" } ], "eprint_id": 1258, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Keelan_bw_1986.pdf", "language": "en", "security": "public", "license": "other", "main": "Keelan_bw_1986.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/18683" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/18683" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/18683" } ] } }, { "id": "/id/document/18683", "doc_id": 18683, "rev_number": 3, "files": [ { "id": "/id/file/11940", "fileid": 11940, "datasetid": "document", "objectid": 18683, "filename": "preview.png", "mime_type": "image/png", "hash": "310ecb8aebef2cb3e81920cf6c0bcafd", "hash_type": "MD5", "filesize": 8769, "mtime": "2012-12-26 02:36:42", "url": "/1258/2/preview.png" } ], "eprint_id": 1258, "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/1904" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/1904" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/1904" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/12/58", "datestamp": "2008-04-08", "lastmod": "2021-04-16 23:11:28", "status_changed": "2009-09-25 01:59:39", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Keelan-Brian-William", "name": { "family": "Keelan", "given": "Brian William" }, "show_email": "NO" } ] }, "title": "High Resolution Laser Spectroscopy of Supersonic Jet-Cooled Molecules", "ispublished": "unpub", "full_text_status": "public", "keywords": "Chemistry", "abstract": "The phenomenon of intramolecular vibrational redistribution (IVR) is currently of significant theoretical and practical interest. Consideration of a simple model raises several important questions about the coupling mechanisms responsible for NR. A review of recent work indicates that these questions are best addressed using complimentary high resolution spectral and temporal experiments, as have been reported elsewhere for only two large molecules. Thus, a tunable laser - free jet apparatus capable of producing fluorescence excitation, dispersed fluorescence, and rotational band contour spectra was constructed and is described in detail herein. High resolution spectral. data obtained using this apparatus is presented for five molecules for which complimentary temporal data is now available: stilbene, diphenylbutadiene, anthracene\u2014h10, anthracene-9d1, and anthracene\u2014d10. Analysis of the spectral data yields information about coupling mechanisms which is relevant to the questions proposed initially.
\r\n\r\nThe results obtained support the following conclusions for these molecules: (1) anharmonic coupling predominates at ranges of \u2248 1 - 10 cm-1, but Coriolis coupling may also be important at shorter ranges; (2) molecular symmetry influences coupling by limiting the number of nearby levels with which a given level may interact; and (3) coupling is more extensive at higher vibrational densities of states due .to the increased number of levels of the appropriate symmetry lying within the effective coupling range of a given level.
", "date": "1986", "date_type": "degree", "id_number": "CaltechETD:etd-04032008-111202", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04032008-111202", "related_url": { "items": [ { "description": "Article adapted for Chapter 5.", "type": "doi", "url": "https://doi.org/10.1016/0009-2614(83)87064-x" }, { "description": "Article adapted for Chapter 6.", "type": "doi", "url": "https://doi.org/10.1021/j100269a011" }, { "description": "Article adapted for Chapter 7.", "type": "doi", "url": "https://doi.org/10.1063/1.448250" } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "NSF", "grant_number": "CHE-8211356" }, { "agency": "NSF", "grant_number": "DMR-8105034" }, { "agency": "Atlantic Richfield Company" } ] }, "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "suggestions": "Student listed in 1986 commencement program despite 1987 degree date on PDF.", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-04-08", "doi": "10.7907/n788-xq67", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "chair" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-04-03", "thesis_defense_date": "1986-06-03", "thesis_approved_date": "2008-04-08", "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": "1986", "author_list": "Keelan, Brian William", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Zewail, Ahmed H." }, { "id": "https://thesis.library.caltech.edu/id/eprint/11756", "eprint_id": 11756, "rev_number": 18, "documents": [ { "id": "/id/document/102421", "doc_id": 102421, "rev_number": 3, "files": [ { "id": "/id/file/295131", "fileid": 295131, "datasetid": "document", "objectid": 102421, "filename": "Siders_PD_1983.pdf", "mime_type": "application/pdf", "hash": "ffb883d371f25e99d89a7ff044d2f0ab", "hash_type": "MD5", "filesize": 44881491, "mtime": "2019-08-01 23:02:05", "url": "/11756/1/Siders_PD_1983.pdf" } ], "eprint_id": 11756, "pos": 1, "placement": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": 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"http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/102421" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/102421" } ] } } ], "eprint_status": "archive", "userid": 1660, "dir": "disk0/00/01/17/56", "datestamp": "2019-08-02 17:45:16", "lastmod": "2021-04-19 22:31:57", "status_changed": "2019-08-02 17:45:16", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Siders-Paul-David", "name": { "family": "Siders", "given": "Paul David" }, "show_email": "NO" } ] }, "title": "Theory of Outer-Sphere Electron-Transfer Reactions", "ispublished": "unpub", "full_text_status": "public", "keywords": "Chemistry", "abstract": "Classical, semiclassical and quantum theories of outer-sphere electron-transfer reactions in polar media are discussed. For each, the Franck-Condon overlap factors for the hexaamminecobalt, hexaaquoiron and hexaammineruthenium self-exchange rates and for the cross-reaction of hexaaquoiron(II) with tris(2,2\u2019-bipyridine)ruthenium(III) are evaluated and compared. The quantum effect on the rates is small in the region of moderate driving force; the \"normal\" \u0394Go region. Direct-sum and saddle-point evaluations of the quantum Franck-Condon factors are made and compared. The saddle-point approximation is shown to be an excellent approximation in the cases considered.
\r\n\r\nQuantum effects in homogeneous outer-sphere electron transfer reactions in the region of large negative \u0394Go (the \"inverted\" region) are considered. The results of quantum, semiclassical and classical calculations on model systems are presented. A sequence of highly exothermic photoinduced reactions of tris(2,2'-bipyridyl) complexes is discussed with regard to the possible importance of quantum effects and of alternate reaction pathways in understanding the failure of the sequence of reactions to exhibit pronounced \"inverted\" behavior. A mechanism leading to electronically excited products provides a possible explanation for the large discrepancy.
\r\n\r\nThe theory of highly exothermic homogeneous outersphere electron-transfer reactions is discussed for transfers occurring over a range of distances. A finite rate of diffusion of reactants and their long-range force are treated by solving the reaction-diffusion equation numerically for the reactant pair distribution function. Steady-state solutions are compared with experimental data. On the basis of short-time solutions it is proposed that experiments which measure electron-transfer rates at short times following the onset of reaction improve the possibility of observing the inverted effect in bimolecular systems.
\r\n\r\nThe effect of the reactants' relative orientation on the electron-transfer rate is considered. Reactants are modeled as oblate-spheroidal potential wells of constant, finite depth. Energy levels and wavefunctions are obtained for an electron localized in such a well. The electronic matrix elements that govern electron transfer within a nonadiabatic quantum theory are evaluated. Significant orientational preferences are predicted for electron transfer between nonspherical donor and acceptor sites.
", "date": "1983", "date_type": "degree", "id_number": "CaltechTHESIS:08012019-155724801", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:08012019-155724801", "related_url": { "items": [ { "description": "Article adapted for Chapter 1.", "type": "doi", "url": "https://doi.org/10.1021/ja00394a003" }, { "description": "Article adapted for Chapter 2.", "type": "doi", "url": "https://doi.org/10.1021/ja00394a004" }, { "description": "Article adapted for Chapter 3.", "type": "doi", "url": "https://doi.org/10.1021/bk-1982-0198.ch010" }, { "description": "Article adapted for Chapter 4.", "type": "doi", "url": "https://doi.org/10.1021/j100394a009" } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "deposited_by": "Bianca Rios", "deposited_on": "2019-08-02 17:45:16", "doi": "10.7907/mgjj-rj90", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "ram@caltech.edu", "id": "Marcus-R-A", "name": { "family": "Marcus", "given": "Rudolph A." }, "role": "chair" }, { "email": "mckoy@caltech.edu", "id": "McKoy-B-V", "name": { "family": "McKoy", "given": "Basil Vincent" }, "role": "member" }, { "email": "chans@its.caltech.edu", "id": "Chan-S-I", "name": { "family": "Chan", "given": "Sunney I." }, "role": "member" }, { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "1983-05-16", "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": "1983", "author_list": "Siders, Paul David", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Marcus, Rudolph A.; McKoy, Basil Vincent; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/4566", "eprint_id": 4566, "rev_number": 14, "documents": [ { "id": "/id/document/7389", "doc_id": 7389, "rev_number": 4, "files": [ { "id": "/id/file/45144", "fileid": 45144, "datasetid": "document", "objectid": 7389, "filename": "Batchelder_js_1982.pdf", "mime_type": "application/pdf", "filesize": 6945202, "mtime": "2012-12-26 03:09:47", "url": "/4566/1/Batchelder_js_1982.pdf" } ], "eprint_id": 4566, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Original (no OCR) Batchelder_js_1982.pdf", "language": "en", "security": "internal", "license": "other", "main": 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"http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/107933" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/45/66", "datestamp": "2004-11-17", "lastmod": "2020-05-14 00:04:28", "status_changed": "2009-09-25 03:21:02", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "jsbatchelder@conveytechnology.com", "id": "Batchelder-John-Samuel", "name": { "family": "Batchelder", "given": "John Samuel" }, "show_email": "NO" } ] }, "title": "The Luminescent Solar Concentrator", "ispublished": "unpub", "full_text_status": "public", "keywords": "Applied Physics", "abstract": "The Luminescent Solar Concentrator (LSC) allows sunlight to be concentrated through the use of light pipe trapping of luminescence. Such concentrators do not require tracking, and they can reduce the cost of solar energy conversion by reducing the required area of photovoltaic cells. We have conducted the following experimental and theoretical investigations in order to optimize the LSC's performance.
\r\n\r\nThe spectral characteristics of 18 organic laser dyes are studied for their applicability as luminescing centers. The spectral homogeneity and self-absorption characteristics of representative dyes are examined in detail. The relative spectral homogeneity of such dyes is shown to depend upon the surrounding material using narrow band laser excitation. We develop three independent techniques for measuring self-absorption rates; these are time-resolved emission, steady state polarization anisotropy, and spectral convolution. Prototype devices are tested for performance, and the componant dyes are tested for stability to solar exposure.
\r\n\r\nA model is developed which predicts the efficiency and gain of and LSC from the spectroscopic characteristics of its components. A critical optical density (CODE) is assigned to the dyes surveyed which predicts the self-absorption limited performance for a particular dye. The maximum efficiency of an LSC is found using a simple model and the experimentally measured Stokes shift required to minimize self-absorption.
\r\n\r\nWe find that the performance of LSCs which achieve high light concentration is primarily limited by self-absorption and by photodegradation. The maximum efficiency possible is about 9% in such systems, and present devices can achieve about 3%. A typical lifetime for an LSC using organic laser dyes due to photodegradation is on the order of a month.
", "date": "1982", "date_type": "degree", "id_number": "CaltechETD:etd-11152004-162115", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-11152004-162115", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "Caltech" }, { "agency": "Department of Energy (DOE)" } ] }, "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "deposited_by": "Imported from ETD-db", "deposited_on": "2004-11-17", "doi": "10.7907/W5W7-9660", "divisions": { "items": [ "div_eng" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "chair" }, { "email": "w6fa@caltech.edu", "id": "Bridges-W-B", "name": { "family": "Bridges", "given": "William B." }, "role": "member" }, { "id": "McCaldin-J-O", "name": { "family": "McCaldin", "given": "James Oeland" }, "role": "member" }, { "id": "Murray-B-C", "name": { "family": "Murray", "given": "Bruce C." }, "role": "member" }, { "email": "rutledge@caltech.edu", "id": "Rutledge-D-B", "name": { "family": "Rutledge", "given": "David B." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2004-11-15", "thesis_defense_date": "1981-08-04", "thesis_approved_date": "2004-11-17", "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": "1982", "author_list": "Batchelder, John Samuel", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Zewail, Ahmed H.; Bridges, William B.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/911", "eprint_id": 911, "rev_number": 18, "documents": [ { "id": "/id/document/1395", "doc_id": 1395, "rev_number": 3, "files": [ { "id": "/id/file/8703", "fileid": 8703, "datasetid": "document", "objectid": 1395, "filename": "Rice_sf_1982.pdf", "mime_type": "application/pdf", "filesize": 5068588, "mtime": "2012-12-26 02:33:36", "url": "/911/1/Rice_sf_1982.pdf" } ], "eprint_id": 911, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Original (no OCR) Rice_sf_1982.pdf", "language": "en", "security": "internal", "license": "other", "main": "Rice_sf_1982.pdf", 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2, "dir": "disk0/00/00/09/11", "datestamp": "2005-03-14", "lastmod": "2020-06-25 23:29:32", "status_changed": "2009-09-25 01:50:09", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "sfrice@sandia.gov", "id": "Rice-Steven-Frederick", "name": { "family": "Rice", "given": "Steven Frederick" }, "show_email": "NO" } ] }, "title": "Optical Spectroscopic Studies of Square Planar d\u2078 Dimers", "ispublished": "unpub", "full_text_status": "public", "keywords": "Chemistry", "abstract": "The single crystal polarized absorption spectra of rhodium(I) diisocyanide dimers presented confirm the assignment of Mann and Gray for the intense visible absorption band as 1A1g \u2192 1A2u. The structured 1A1g \u2192 3A2u absorption band in RH2(b)4(Bph4)2 shows the 3A2u excited state to have a metal-metal vibrational frequency of 149 cm-1. This is compared to the 85 cm-1 ground state frequency which results in the orbital assignment of this transition as d z2\u03c3* \u2192 pz\u03c3. The excited state has an internuclear bond distance .31 \u00c5 shorter than that of the ground state. The bonding description obtained through the analysis of the spectra depicts a ground state that is formally nonbonding stabilized through configurational interaction with a low lying, strongly bonded excited state.
\r\n\r\nThe 3A2u state in these dimers has a pronounced phosphorescence with a 77K lifetime of 20 \u03bcsec. The quantum yields and lifetimes are very temperature sensitive with several 300K lifetimes of about 10 nsec. This temperature dependence, characteristic of a strong coupling limit, is interpreted in terms of a nonradiative pathway depopulating the 3A2u through another excited state associated with a dz2 \u2192 dx2-y2 transition.
\r\n\r\nA compound isoelectronic with these rhodium diisocyanides, Pt2(H2P2O5)4-4, is shown to have a similar metal-metal interaction in both the ground and lowest excited states. Recent results regarding the low temperature photophysics of this compound have been verified and extended through an analysis of the vibronically structured 3A2u \u2192 1A1g luminescence. The 3A2u state is demonstrated to have an internuclear distance of 2.71 \u00c5, .21 \u00c5 shorter than that of the ground state. The metal-metal vibrational frequency in the 3A2u is 155 cm-1, distinctly higher than the 110 cm-1 of the ground state.
\r\n", "date": "1982", "date_type": "degree", "id_number": "CaltechETD:etd-03102005-155606", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-03102005-155606", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "Fannie and John Hertz Foundation" } ] }, "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "deposited_by": "Imported from ETD-db", "deposited_on": "2005-03-14", "doi": "10.7907/Z2CJ-J714", "alt_title": { "items": [ "Optical Spectroscopic Studies of Square Planar d8 Dimers", "Optical Spectroscopic Studies of Square Planar d^8 Dimers" ] }, "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "hbgray@caltech.edu", "id": "Gray-H-B", "name": { "family": "Gray", "given": "Harry B." }, "role": "chair" }, { "email": "bercaw@caltech.edu", "id": "Bercaw-J-E", "name": { "family": "Bercaw", "given": "John E." }, "role": "member" }, { "id": "Janda-K-C", "name": { "family": "Janda", "given": "Kenneth C." }, "role": "member" }, { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2005-03-10", "thesis_defense_date": "1982-02-03", "thesis_approved_date": "2005-03-14", "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": "1982", "author_list": "Rice, Steven Frederick", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Gray, Harry B.; Bercaw, John E.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1295", "eprint_id": 1295, "rev_number": 9, "documents": [ { "id": "/id/document/1962", "doc_id": 1962, "rev_number": 3, "files": [ { "id": "/id/file/12283", "fileid": 12283, "datasetid": "document", "objectid": 1962, "filename": "Smith_dd_1981.pdf", "mime_type": "application/pdf", "filesize": 9934247, "mtime": "2012-12-26 02:36:57", "url": "/1295/1/Smith_dd_1981.pdf" } ], "eprint_id": 1295, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Smith_dd_1981.pdf", "language": "en", "security": "public", "license": "other", "main": "Smith_dd_1981.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/18732" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/18732" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/18732" } ] } }, { "id": "/id/document/18732", "doc_id": 18732, "rev_number": 3, "files": [ { "id": "/id/file/12281", "fileid": 12281, "datasetid": "document", "objectid": 18732, "filename": "preview.png", "mime_type": "image/png", "hash": "c5c9687fe20eb652c1c4bf8861e75630", "hash_type": "MD5", "filesize": 9978, "mtime": "2012-12-26 02:36:57", "url": "/1295/2/preview.png" } ], "eprint_id": 1295, "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/1962" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/1962" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/1962" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/12/95", "datestamp": "2008-04-08", "lastmod": "2021-04-16 22:59:34", "status_changed": "2009-09-25 02:00:34", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Smith-D-D", "name": { "family": "Smith", "given": "Duane D." }, "show_email": "NO" } ] }, "title": "Optical dephasing and energy transfer in ordered and disordered solids : studies by laser spectroscopy and optical-microwave double resonance", "ispublished": "unpub", "full_text_status": "public", "keywords": "chemistry", "abstract": "NOTE: Text or symbols not renderable in plain ASCII are indicated by [...]. Abstract is included in .pdf document.\r\n\r\nElectronic energy transfer and optical dephasing of ordered and disordered molecular crystals is studied theoretically and experimentally. Data on impurity band transport are presented which are consistent with the Anderson transition. The effect of dimensionality on trap-trap energy transfer thresholds is experimentally measured and modeled.\r\n\r\nExperiments focus on 1,4-dibromonaphthalene whose lowest triplet exciton is quasi-one-dimensional. Steady state and transient line narrowing laser spectroscopy provide the first unequivocal measurement of the inelastic scattering rate amongst the band states. The inelastic scattering rate (intraband exchange rate) is slow and of the order of 10 [...]sec at 20 K. Further, the elastic scattering rate is ~10 psec at 20 K and is describable as Raman scattering by ~ a 42 cm[...] phonon. It is significant that there is a six order of magnitude separation of time scales for the elastic and inelastic scattering, demonstrating that pure dephasing dominates the intraband exchange. From the broadening and the lack of a relative shift of the two sublattice [...] absorptions, it is concluded that the interband exchange rate is negligible compared to the pure dephasing. It is found that disordering [...] DBN with up to 16% [...] DBN, the inelastic scattering rate is unaltered, being 10 gsec at 20 K! Pumping the [...] state of the upper sublattice, relaxation is exclusively to the [...] state of the lower sublattice, implicating single phonon resonant relaxation.\r\n\r\nFor heavily trap-disordered DBN (up to 24% [...]/[...]) it is found that (1) excitation migration is step-wise incoherent, (2) energy transfer to deep traps is best fit with a [...] energy transfer rate, (3) there are no mobility edges in the trap inhomogeneous profile and (4) an upper limit for the trap homogeneous linewidth at 1.3 K is 9 Ghz.\r\n\r\nUsing lifetimes and temperature-dependent lineshapes, optical dephasing of F and [...] center triplet states in CaO is is consistent with Raman scattering by effective oscillators of 89 and 151 cm[...], respectively.\r\n\r\nVibrational dephasing of the CO stretch for benzophenone matrix-isolated in 4,4'-dibromodiphenyl ether at 2.1 K was investigated with a novel application of emission spectroscopy. It was found that the total dephasing rate of the CO stretch was linear in the CO quantum number, consistent with recent theoretical predictions for carbonyl moieties.\r\n", "date": "1981", "date_type": "degree", "id_number": "CaltechETD:etd-04072008-141328", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04072008-141328", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-04-08", "doi": "10.7907/1gza-t381", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "name": { "family": "Unknown", "given": "Unknown" } } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-04-07", "thesis_defense_date": "1981-03-02", "thesis_approved_date": "2008-04-08", "thesis_awards": "The Herbert Newby McCoy Award, 1980", "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": "1981", "author_list": "Smith, Duane D.", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Unknown, Unknown" }, { "id": "https://thesis.library.caltech.edu/id/eprint/10755", "eprint_id": 10755, "rev_number": 17, "documents": [ { "id": "/id/document/87006", "doc_id": 87006, "rev_number": 3, "files": [ { "id": "/id/file/246546", "fileid": 246546, "datasetid": "document", "objectid": 87006, "filename": "Highe_AJ_1981.pdf", "mime_type": "application/pdf", "hash": "9f41ea8424ca57252c00dfdb3dadc669", "hash_type": "MD5", "filesize": 50340096, "mtime": "2018-03-06 20:25:59", "url": "/10755/1/Highe_AJ_1981.pdf" } ], "eprint_id": 10755, "pos": 1, "placement": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": "Highe_AJ_1981.pdf", 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"http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/87006" } ] } } ], "eprint_status": "archive", "userid": 8820, "dir": "disk0/00/01/07/55", "datestamp": "2018-03-06 22:07:51", "lastmod": "2021-04-16 23:01:43", "status_changed": "2018-03-06 22:07:51", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Highe-Albert-John", "name": { "family": "Highe", "given": "Albert John" } } ] }, "title": "Ionic Motion in Solid Electrolytes: A Solid State NMR Study of Sodium and Lithium in \u03b2-Alumina", "ispublished": "unpub", "full_text_status": "public", "keywords": "Chemistry", "abstract": "Solid state NMR techniques have been used as a microscopic probe of the structural and dynamical properties of the mobile cations in the solid electrolyte \u03b2-alumina. The first order quadrupole shifts in the (\u00b13/2 \u2194 \u00b11/2) transitions in the spin 3/2 nuclei sodium and lithium have allowed the electric field gradients (EFG) for the nominal Beevers and Ross (BR) and mid-oxygen (MO) sites to be characterized. The details of the EFG's for and the distribution of cations among BR and MO sites reflect the differences in the potential wells for lithium and sodium in \u03b2-alumina. In particular, unlike sodium, the MO site for lithium is lower in energy than the BR site which results in a different structural arrangement of lithium ions. In sodium \u03b2-alumina, the equilibrium position for sodium in the BR site is displaced from the three-fold symmetry axis. It is believed that this is due to the presence of nearby MO-MO pairs. Furthermore, an activation energy of 0.04 eV is observed for the motion of sodium ions among the displaced BR sites which is associated with the correlated motion of MO-MO pairs. The effects of a second motional process with an activation energy of 0.08 eV are observed in both lithium and sodium spectra which are associated with the motion of cations among BR and MO sites. The interaction of cations in MO-MO pairs was further investigated by observing the effect of varying the ratio of lithium and sodium in mixed lithium-sodium \u03b2-alumina on the distribution of cations among the available sites. The results were interpreted using a theory previously developed to explain the mixed-alkali effect in glasses and indicate that there is a strong interaction between unlike MO-MO pairs which governs the cation site distribution and raises the activation energy for conduction.
", "date": "1981", "date_type": "degree", "id_number": "CaltechTHESIS:03062018-120827730", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:03062018-120827730", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Mel Ray", "deposited_on": "2018-03-06 22:07:51", "doi": "10.7907/w0cr-8h87", "alt_title": { "items": [ "Ionic Motion in Solid Electrolytes: A Solid State NMR Study of Sodium and Lithium in beta-Alumina", "Solid State NMR Study of Sodium and Lithium in \u03b2-Alumina", "Solid State NMR Study of Sodium and Lithium in beta-Alumina" ] }, "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "chair" }, { "email": "chans@its.caltech.edu", "id": "Chan-S-I", "name": { "family": "Chan", "given": "Sunney I." }, "role": "member" }, { "email": "wag@wag.caltech.edu", "id": "Goddard-W-A-III", "name": { "family": "Goddard", "given": "William A., III" }, "role": "member" }, { "id": "Cole-Terry", "name": { "family": "Cole", "given": "Terry" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "1980-11-18", "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": "1981", "author_list": "Highe, Albert John", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Zewail, Ahmed H.; Chan, Sunney I.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1310", "eprint_id": 1310, "rev_number": 10, "documents": [ { "id": "/id/document/1995", "doc_id": 1995, "rev_number": 3, "files": [ { "id": "/id/file/12468", "fileid": 12468, "datasetid": "document", "objectid": 1995, "filename": "Orlowski_te_1979.pdf", "mime_type": "application/pdf", "filesize": 13116909, "mtime": "2012-12-26 02:37:07", "url": "/1310/1/Orlowski_te_1979.pdf" } ], "eprint_id": 1310, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Orlowski_te_1979.pdf", "language": "en", "security": "public", "license": "other", "main": "Orlowski_te_1979.pdf", "media_duration": 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Abstract is included in .pdf document.\r\n\r\nThe objectives of this thesis are to develop new high-resolution (\u00b1 3 MHz) coherent nonlinear optical spectroscopic techniques and to utilize them to examine the nature of line broadening processes in optical transitions of isolated large and small molecules. By measuring the coherent and incoherent transients observed either in the forward direction along the laser beam (absorption) or at right-angles to the exciting beam (emission), these techniques allow one to determine optical [...] (the longitudinal relaxation time) and optical [...] (the transverse relaxation time). From [...] and [...] one can obtain under certain circumstances, both the radiative and nonradiative [...] contributions as well as the pure dephasing [...] contribution to the total homogeneous linewidth [...] of the optical transition.\r\n\r\nTwo molecules are examined in detail. Iodine was chosen to demonstrate the new techniques because its conventional spectroscopy is well-known and to examine dephasing and decay processes important for small molecules. It was studied in the gas phase and in a molecular beam. Condensed phase experiments were performed on single crystals of pentacene isolated in a p-terphenyl host to obtain information about the nature of radiationless transitions and dephasing processes important in this large molecule.\r\n\r\nThe optical transition that was studied in iodine is [...]. Using LADS (Laser Acoustic Diffraction Spectroscopy) for obtaining nanosecond time resolution with a narrowband single-mode dye laser and the IRD (Incoherent Resonance Decay) method whereby population dynamics and the coherence in the system can be obtained by monitoring the spontaneous emission, the following Stern-Volmer relationship was obtained for iodine:\r\n\r\n[...] = (0.783 \u00b1 0.032) + (0.0143 \u00b1 0.0005) P(mtorr).\r\n\r\nThis relationship provides a zero-pressure radiative lifetime of 1.28 \u00b1 0.05 [...]sec and a nonradiative collisional quenching cross section of [...] = 70 \u00b1 2 [...]. These results agree with those obtained in previous studies with broadband excitation indicating that excitation bandwidth is unimportant for [...] processes in small molecules. Using the electrooptic method of laser frequency switching, an optical nutation was observed in iodine whose Rabi oscillation frequency [...] provided the dipole moment for the transition ([mu] = 0.05 Debye) after determining the laser field amplitude [...]. The Rabi frequency was also obtained from a coherent oscillation observed on top of the IRD signal in iodine at low pressure. This oscillation decayed by [...] and the overall IRD signal provided [...] such that both the coherence and decay of the system were obtained simply by monitoring the spontaneous emission. The homogeneous linewidth of the transition was measured using the 3-pulse photon echo method. At 10 mtorr pressure it was found to be 579 kHz. This is almost three orders of magnitude less than the inhomogeneous (Doppler) linewidth of ca. 400 MHz. Molecular beam experiments provided the radiative lifetime (1.24 \u00b1 0.02 [...]sec) of iodine in a collisionless environment from which the radiative contribution (22%, 128 kHz) to the total homogeneous linewidth was obtained. Assuming that radiative losses from the lower level of the system can be neglected it was also determined that 38 kHz (7%) of the homogeneous linewidth is due to non-radiative relaxation (inelastic scattering) and a dramatic 413 kHz (71%) is due to pure dephasing [...] as a result of elastic scattering processes. Finally an OFID (optical free induction decay) was observed in the molecular beam whose decay indicated that [...]. Therefore, in a collisionless environment, the only dephasing process for iodine is spontaneous emission (i.e., no intramolecular dephasing processes exist).\r\n\r\nThe optical transition that was studied in pentacene [...] exhibits four sites in a p-terphenyl host. The lowest energy site at 16,887 cm[...] has the following characteristics at 1.8[...]K:\r\n\r\n[...] = 24.9 \u00b1 2 nsec; [...] = 44 \u00b1 2 nsec, and [mu] = 0.7 \u00b1 0.1 Debye.\r\n\r\nExperiments in this system are categorized into two time regimes for theoretical analysis: a transient coherence regime where the observed decay is comparable with [...] and [...], and a steady-state coherence regime where transient dephasing is complete and the off-diagonal elements of the density matrix have decayed to their steady-state values in the presence of the laser field. The Wilcox-Lamb method is used to derive rate equations ([...] dependent) from the density matrix equations of motion. These equations describe the population dynamics in the pentacene level structure ([...] = ground state, [...] = excited singlet state and [...] = triplet manifold) and upon averaging them over the inhomogeneous linewidth of the transition and then using them to fit experimental decay curves one obtains:\r\n\r\n[...] = 24.9 \u00b1 2 nsec and [...] = 15.7 [...]sec,\r\n\r\nthe time constants for spontaneous emission to [...] and crossing into [...], respectively. OFID and nutation expressions are presented for the pentacene level structure and when appropriate averaging is done over both the inhomogeneous linewidth and the laser beam spatial profile, good fits can be obtained for the experimental transients. At 1.8[...]K it was determined that [...] = [...]. Therefore, as in iodine at zero pressure, spontaneous emission is the only dephasing process in pentacene at low temperature. At higher temperature, however, a strongly temperature dependent dephasing process takes place with an onset at 3.7[...]K. A theoretical treatment of the various dephasing channels is presented that explains the observed temperature dependence of [...] in pentacene and attributes pure dephasing to an anisotropy in the scattering amplitudes between the ground and excited states. Optical site selection of the pentacene transitions has been observed and is related to vibrational relaxation and homogeneous and inhomogeneous broadening in this system. Studies of the homogeneous broadening of the vibronic line 267 cm[...] above the lowest energy site indicate that vibrational relaxation is fast (psec) in the excited singlet manifold of pentacene. Finally from more than ten independent experiments including narrow and broad band excitation, on- and off-resonance scattering, Zeeman effect measurements and the transient decay as a function of excess energy in the molecule, a more complete picture of the pentacene level structure is given. It is proposed that the slow decay\t[...] observed during narrowband excitation represents intersystem crossing to nearby triplet manifolds after the transient coherence of the \"two-level\" system [...] has decayed. Furthermore, the decay of the primary state prepared in these experiments is not sensitive to the bandwidth or the coherence properties of the excitation source.\r\n", "date": "1979", "date_type": "degree", "id_number": "CaltechETD:etd-04082008-084228", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-04082008-084228", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-04-08", "doi": "10.7907/1KE1-7557", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "id": "Zewail-A-H", "name": { "family": "Zewail", "given": "Ahmed H." }, "role": "chair" }, { "id": "Anson-F-C", "name": { "family": "Anson", "given": "Fred C." }, "role": "member" }, { "id": "Robinson-G-W", "name": { "family": "Robinson", "given": "G. Wilse" }, "role": "member" }, { "id": "Beauchamp-J-L", "name": { "family": "Beauchamp", "given": "Jesse L." }, "role": "member" }, { "id": "McKoy-B-V", "name": { "family": "McKoy", "given": "Basil Vincent" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-04-08", "thesis_defense_date": "1978-08-14", "thesis_approved_date": "2008-04-08", "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": "1979", "author_list": "Orlowski, Thomas Edward", "advisor_list": "Zewail, Ahmed H.", "comittee_list": "Zewail, Ahmed H.; Anson, Fred C.; et el." } ]