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"status_changed": "2019-01-30 17:43:32", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "aileenhui@gmail.com", "id": "Hui-Aileen-Oyama-Ah-Yee", "name": { "family": "Hui", "given": "Aileen Oyama Ah Yee" }, "orcid": "0000-0003-4217-2698", "show_email": "NO" } ] }, "title": "Atmospheric Peroxy Radical Chemistry Studied by Infrared Kinetic Spectroscopy", "ispublished": "unpub", "full_text_status": "public", "keywords": "Chemical physics, kinetics, atmospheric chemistry, spectroscopy", "abstract": "
Peroxy radical (RO2) chemistry plays a central role in atmospheric science. RO2 radicals control the oxidative capacity of the atmosphere and are key intermediates in the cycling of ozone in the troposphere in regions where levels of nitrogen oxides (NOx ≡ NO + NO2) are high. In more remote regions of the Earth where NOx concentrations are low, RO2 loss is dominated by reaction with hydroperoxy (HO2) and other peroxy radicals, leading to removal of reactive radicals from the troposphere. However, for certain species of RO2, reaction with HO2 can also propagate radical chemistry by recycling hydroxyl (OH) radicals, a primary oxidant in the atmosphere. Both HO2 and OH radicals play important roles in atmospheric oxidation reactions. Accurate characterization of various RO2 reactions that contribute to consuming and recycling HOx (HOx ≡ HO2 + OH) are instrumental for understanding the effects of atmospheric composition on climate forcing, air quality, and the global ozone budget.
\r\n\r\nMy thesis work used laboratory studies to characterize gas phase organic peroxy radical (RO2) reactions that are relevant to atmospheric chemistry. The main body of my work focused on studying the self reactions of HO2 and RO2 as well as their cross reactions (HO2 + RO2) using a time-resolved experimental technique called Infrared Kinetic Spectroscopy (IRKS), which combines infrared (IR) and ultraviolet (UV) absorption spectroscopy. Perfect isolation of one specific reaction is generally difficult or impossible due to radical recycling and secondary chemistry, which leads to numerous reactions occurring simultaneously. Thus, although laboratory studies provide controlled environments to study these reactions, the accuracy of the results are highly dependent on the experiment's selectivity and sensitivity to specific transient species. In this work, a new mid-IR (MIR) laser was implemented into the existing apparatus for measuring OH radicals. In addition to UV absorption spectroscopy, the IRKS apparatus was equipped for selective detection of HO2 and OH radicals in the near-IR (NIR) and MIR, respectively.
\r\n\r\nThe kinetics and product yields of a reaction are two important factors for assessing the impact of these reactions on the atmosphere. IRKS was used to study the kinetics of the self reactions of acetylperoxy (CH3C(O)O2) and acetonylperoxy (CH3C(O)CH2O2), as well as their reactions with HO2. The OH and O3 yields from the reaction of HO2 + CH3C(O)O2 were also measured, providing the first parametrization of the temperature dependence of the OH product channel. The temperature dependence of the HO2 self reaction kinetics was re-investigated to resolve discrepancies in the results previously reported in the literature. Furthermore, this work identified and characterized rate enhancement effects on the HO2 self reaction by the adducts of HO2 formed from the reaction of HO2 with methanol (CH3OH), acetaldehyde (CH3CHO), and acetone (CH3C(O)CH3), which were used as radical precursors for HO2, CH3C(O)O2, and CH3C(O)CH2O2, respectively.
\r\n\r\nFinally, the improved sensitivity of the IRKS apparatus enabled the investigation of fast reaction kinetics. The rate constants of Cl atoms with CH3OH and CH3CHO were measured over a wide range of temperatures. The results were consistent with previously reported values in the literature and additionally validated assumptions that had been made regarding the temperature independence of these reactions. The temperature and pressure dependences of the OH yield from the reaction of CH3CO with O2 were also studied to resolve current discrepancies in the literature. The yield of HO2 from this reaction was also directly measured for the first time.
", "date": "2019", "date_type": "degree", "id_number": "CaltechTHESIS:01172019-135430092", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:01172019-135430092", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "NSF", "grant_number": "CHE-1413712" }, { "agency": "NASA", "grant_number": "NNX12AE01G" } ] }, "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "deposited_by": "Aileen Hui", "deposited_on": "2019-01-30 17:43:32", "doi": "10.7907/Z9H0-1H20", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "mo@caltech.edu", "id": "Okumura-M", "name": { "family": "Okumura", "given": "Mitchio" }, "role": "advisor" }, { "email": "stanley.p.sander@jpl.nasa.gov", "id": "Sander-S-P", "name": { "family": "Sander", "given": "Stanley P." }, "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "tfm@caltech.edu", "id": "Miller-T-F", "name": { "family": "Miller", "given": "Thomas F." }, "role": "chair" }, { "email": "gab@gps.caltech.edu", "id": "Blake-G-A", "name": { "family": "Blake", "given": "Geoffrey A." }, "role": "member" }, { "email": "ram@caltech.edu", "id": "Marcus-R-A", "name": { "family": "Marcus", "given": "Rudolph A." }, "role": "member" }, { "email": "mo@caltech.edu", "id": "Okumura-M", "name": { "family": "Okumura", "given": "Mitchio" }, "role": "member" }, { "email": "stanley.p.sander@jpl.nasa.gov", "id": "Sander-S-P", "name": { "family": "Sander", "given": "Stanley P." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2018-11-29", "gradofc_approval_date": "2019-01-29", "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": "2019", "author_list": "Hui, Aileen Oyama Ah Yee", "advisor_list": "Okumura, Mitchio and Sander, Stanley P.", "comittee_list": "Miller, Thomas F.; Blake, Geoffrey A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/7086", "eprint_id": 7086, "rev_number": 168, "documents": [ { "id": "/id/document/14942", "doc_id": 14942, "rev_number": 8, "files": [ { "id": "/id/file/97137", "fileid": 97137, "datasetid": "document", "objectid": 14942, "filename": "Sprague_Matthew_Thesis_Front_Matter.pdf", "mime_type": "application/pdf", "filesize": 139471, "mtime": "2012-12-26 04:43:41", "url": "/7086/23/Sprague_Matthew_Thesis_Front_Matter.pdf" } ], "eprint_id": 7086, "pos": 23, "placement": 2, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Title, Acknowledgements, TOC", "language": 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"disk0/00/00/70/86", "datestamp": "2012-05-30 15:44:48", "lastmod": "2019-10-03 23:56:11", "status_changed": "2012-05-30 15:44:48", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "matthew.sprague@gmail.com", "id": "Sprague-Matthew-Kiran", "name": { "family": "Sprague", "given": "Matthew Kiran" }, "show_email": "YES" } ] }, "title": "Cavity Ringdown Spectroscopy, Kinetics, and Quantum Chemistry of Atmospherically Relevant Reactions", "ispublished": "unpub", "full_text_status": "public", "keywords": "cavity ringdown; spectroscopy; kinetics; quantum chemistry; CRDS; atmospheric; radicals; HOONO; peroxynitrous acid; hydroxymethylperoxy; alkoxy; butoxy; pentoxy; hydroxybutylperoxy; hydroxypentylperoxy", "abstract": "This thesis describes laboratory experiments and electronic structure calculations on three chemical systems relevant to tropospheric ozone chemistry: peroxynitrous acid (HOONO), hydroxymethylperoxy radical formed from HO2 + HCHO (R1), and products of alkoxy isomerization (R2). R1 and R2 were studied experimentally using a gas flow cell that combined UV photolysis with cavity ringdown spectroscopy (CRDS). All chemical systems were studied using electronic structure calculations and kinetics modeling.
\r\n\r\nHOONO is one of the products of the reaction OH + NO2, and acts as a temporary reservoir for HOx and NOx in the atmosphere. Torsional excitation of HOONO will break its internal hydrogen bond, leading to sequence band formation in the OH stretch spectrum. Chapter 3 describes a calculated 3-dimensional potential energy surface to examine torsional mode coupling and sequence band formation. We apply these results to previous CRDS kinetics studies of HOONO.
\r\n\r\nThe reaction of HO2 with carbonyls is believed to be a major sink of HOx and carbonyl compounds at reduced temperatures. R1 is the simplest of these reactions. Despite numerous previous studies, considerable uncertainty exists on the activation energy and rate constant of R1. Chapters 4-6 describe CRDS and electronic structure studies on the isomerization product, hydroxymethylperoxy. CRDS was used to make the first measurements of the OH stretch and A-X electronic spectra, and the kinetics of hydroxymethylperoxy chemistry. Electronic structure calculations were used to simulate the spectroscopic bands and examine the conformers of hydroxymethylperoxy and 2-hydroxyisopropylperoxy.
\r\n\r\nAtmospheric alkoxy radicals can isomerize or react with O2, and each pathway has a different impact on ozone chemistry. Chapters 7-10 describe cavity ringdown spectroscopy, kinetics, and electronic structure calculations on the n-butoxy and 2-pentoxy isomerization products, specifically δ-HOC4H8\u2022, δ-HOC4H8OO\u2022, δ-HO-1-C5H10\u2022, and δ-HO-1-C5H10OO\u2022. CRDS was used to make the first measurements of the A-X electronic spectrum of δ-HOC4H8OO\u2022 and clean OH stretch spectra of all four radicals. Relative kinetics data previously obtained using CRDS were reanalyzed to include the effects of additional alkoxy reactions. Electronic structure calculations were performed to explain the observations that the OH stretch absorption cross section differs between HOR\u2022 and HOROO\u2022.
", "date": "2012", "date_type": "degree", "id_number": "CaltechTHESIS:05282012-184532561", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:05282012-184532561", "related_url": { "items": [ { "type": "doi", "url": "http://dx.doi.org/10.1021/jp905731h" }, { "type": "doi", "url": "http://dx.doi.org/10.1021/jp212136r" }, { "type": "doi", "url": "http://dx.doi.org/10.1126/science.1193030 " } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "Department of Defense", "grant_number": "National Defense Science and Engineering Graduate Fellowship" }, { "agency": "NASA Upper Atmospheric Research Program", "grant_number": "NAG5-11657" }, { "agency": "NASA Upper Atmospheric Research Program", "grant_number": "NNG06GD88G" }, { "agency": "NASA Upper Atmospheric Research Program", "grant_number": "NNX09AE21G" }, { "agency": "California Air Resources Board", "grant_number": "03-333" }, { "agency": "California Air Resources Board", "grant_number": "07-730" }, { "agency": "National Science Foundation", "grant_number": "CHE-0515627" } ] }, "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Matthew Sprague", "deposited_on": "2012-05-30 15:44:48", "doi": "10.7907/T8BQ-D871", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "mo@caltech.edu", "id": "Okumura-M", "name": { "family": "Okumura", "given": "Mitchio" }, "role": "advisor" }, { "email": "stanley.p.sander@jpl.nasa.gov", "id": "Sander-S-P", "name": { "family": "Sander", "given": "Stanley P." }, "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "gab@gps.caltech.edu", "id": "Blake-G-A", "name": { "family": "Blake", "given": "Geoffrey A." }, "role": "chair" }, { "email": "mo@caltech.edu", "id": "Okumura-M", "name": { "family": "Okumura", "given": "Mitchio" }, "role": "member" }, { "email": "stanley.p.sander@jpl.nasa.gov", "id": "Sander-S-P", "name": { "family": "Sander", "given": "Stanley P." }, "role": "member" }, { "email": "wennberg@gps.caltech.edu", "id": "Wennberg-P-O", "name": { "family": "Wennberg", "given": "Paul O." }, "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_defense_date": "2012-05-18", "gradofc_approval_date": "2012-05-29", "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": "2012", "author_list": "Sprague, Matthew Kiran", "advisor_list": "Okumura, Mitchio and Sander, Stanley P.", "comittee_list": "Blake, Geoffrey A.; Okumura, Mitchio; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/5540", "eprint_id": 5540, "rev_number": 73, "documents": [ { "id": "/id/document/9324", "doc_id": 9324, "rev_number": 11, "files": [ { "id": "/id/file/58892", "fileid": 58892, "datasetid": "document", "objectid": 9324, "filename": "ACN_Experimental_Ch5_final.pdf", "mime_type": "application/pdf", "filesize": 766577, "mtime": "2012-12-26 03:21:29", "url": "/5540/1/ACN_Experimental_Ch5_final.pdf" } ], "eprint_id": 5540, "pos": 1, "placement": 7, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Chapter 5 (Experimental)", "language": "en", "security": "public", 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codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/9330" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/9330" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/9330" } ] } } ], "eprint_status": "archive", "userid": 39, "dir": "disk0/00/00/55/40", "datestamp": "2010-03-19 17:06:54", "lastmod": "2019-11-08 18:08:19", "status_changed": "2010-03-19 17:06:54", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "anoell@jpl.nasa.gov", "id": "Noell-Aaron-Craig", "name": { "family": "Noell", "given": "Aaron Craig" }, "orcid": "0000-0001-6244-174X", "show_email": "YES" } ] }, "title": "Laboratory Studies of the Self and Cross Reactions of Atmospheric Peroxy Radicals", "ispublished": "unpub", "full_text_status": "public", "keywords": "Atmospheric Chemistry; Peroxy Radical; HO2; Ethyl Peroxy; C2H5O2; Photoinduced Nucleation", "abstract": "My studies focused on the self and cross reactions of peroxy radicals (RO\u2082). These are important gas phase reactions in the atmosphere when concentrations of nitrogen oxides are low. Hydroperoxide products of these reactions can undergo further reaction to form aerosol precursors, making RO\u2082 reactions critical to aerosol formation as well. The occurrence of multiple simultaneous reactions is frequently unavoidable when working with radical reactions. Self reactions of RO\u2082 further complicate matters by producing another peroxy radical (HO\u2082) through one of their product channels. Time resolved spectroscopic probes in the ultraviolet and near-infrared, specifically targeting each reactant, were used to measure the rate coefficients for the self and cross reactions of HO\u2082 and ethyl peroxy radicals (C\u2082H\u2085O\u2082). In addition the product branching fraction leading to HO\u2082 was determined for the C\u2082H\u2085O\u2082 self reaction with results very different from the literature.
\r\n\r\nFurther work on the self reaction branching fractions of methyl peroxy, ethyl peroxy, and propyl peroxy was done to try and resolve the discrepancy with the literature. A photoionization mass spectrometry technique was used to monitor all of the stable reaction products on the timescale of the reaction. The literature work had used end product studies after the reactions had completed to measure all of the stable products. Results from the photoionization studies appear to agree with the spectroscopic work for the C\u2082H\u2085O\u2082 self reaction, indicating that additional secondary chemistry may have skewed the results in the literature.
\r\n\r\nAerosol nucleation observed in low temperature experiments on the HO\u2082 self reaction was another area of work. Radical chemistry is the main driver of gas phase atmospheric cycles, but is not currently thought to be at the center of new particle formation. Radical-molecule complexes between HO\u2082 and a number of species including methanol, water, and acetone could act as particle seeds at low temperature due to the stability of their hydrogen bonds. Most of the nucleation work described is on the HO\u2082 - methanol complex, but all three were investigated. Lastly, the experimental calibrations and general procedures that went on throughout all this work are described.
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K.;" ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Gayle Hammer", "deposited_by": "Aaron Noell", "deposited_on": "2010-03-19 17:06:54", "doi": "10.7907/B844-DA56", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "mo@caltech.edu", "id": "Okumura-M", "name": { "family": "Okumura", "given": "Mitchio" }, "role": "advisor" }, { "email": "stan.sander@jpl.nasa.gov", "id": "Sander-S-P", "name": { "family": "Sander", "given": "Stanley P." }, "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "gab@gps.caltech.edu", "id": "Blake-G-A", "name": { "family": "Blake", "given": "Geoffrey A." }, "role": "chair" }, { "email": "ram@caltech.edu", "id": "Marcus-R-A", "name": { "family": "Marcus", "given": "Rudolph A." }, "role": "member" }, { "email": "jlbchamp@caltech.edu", "id": "Beauchamp-J-L", "name": { "family": "Beauchamp", "given": "Jesse L." }, "role": "member" }, { "email": "mo@caltech.edu", "id": "Okumura-M", "name": { "family": "Okumura", "given": "Mitchio" }, "role": "member" }, { "email": "stan.sander@jpl.nasa.gov", "id": "Sander-S-P", "name": { "family": "Sander", "given": "Stanley P." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2009-11-18", "gradofc_approval_date": "2010-03-16", "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": "2010", "author_list": "Noell, Aaron Craig", "advisor_list": "Okumura, Mitchio and Sander, Stanley P.", "comittee_list": "Blake, Geoffrey A.; Marcus, Rudolph A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/2019", "eprint_id": 2019, "rev_number": 39, "documents": [ { "id": "/id/document/3568", "doc_id": 3568, "rev_number": 3, "files": [ { "id": "/id/file/21075", "fileid": 21075, "datasetid": "document", "objectid": 3568, "filename": "AKMollnerThesis2007Abstract_TOC.pdf", "mime_type": "application/pdf", "filesize": 224869, "mtime": "2012-12-26 02:45:38", "url": "/2019/1/AKMollnerThesis2007Abstract_TOC.pdf" } ], "eprint_id": 2019, "pos": 1, "placement": 2, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "AKMollnerThesis2007Abstract_TOC.pdf", "language": "en", 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"mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/3574" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/3574" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/3574" } ] } }, { "id": "/id/document/121854", "doc_id": 121854, "rev_number": 1, "files": [ { "id": "/id/file/367247", "fileid": 367247, "datasetid": "document", "objectid": 121854, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "2844fcf57ddb2229af51442f6fe60161", "hash_type": "MD5", "filesize": 6067, "mtime": "2021-06-23 21:39:10", "url": "/2019/25/indexcodes.txt" } ], "eprint_id": 2019, "pos": 25, "placement": 25, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/3575" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/3575" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/3575" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/20/19", "datestamp": "2007-05-31", "lastmod": "2020-03-03 19:20:05", "status_changed": "2009-09-25 02:23:26", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "Andrew.K.Mollner@aero.org", "id": "Mollner-Andrew-Keeler", "name": { "family": "Mollner", "given": "Andrew Keeler" }, "show_email": "YES" } ] }, "title": "Cavity Ringdown Spectroscopy Studies of Atmospheric Reactions: Peroxynitrous Acid Formation and Alkoxy Radical Isomerization", "ispublished": "unpub", "full_text_status": "public", "keywords": "alkoxy; butoxy; cavity ringdown; CRDS; HOONO; isomerization; nitric acid; pentoxy; peroxynitrous acid", "abstract": "This thesis describes laboratory experiments investigating atmospheric reactions using cavity ringdown spectroscopy (CRDS). The reactions studied were the formation of peroxynitrous acid (HOONO) in the termolecular association reaction OH + NO\u2082 (R1) and the isomerization of alkoxy radicals. Experiments were conducted in a gas flow cell combining UV photolysis to initiate reactions with infrared CRDS for the detection of products.
\r\n\r\nFormation of the weakly bound HOONO in the atmosphere reduces the yield of nitric acid (HONO\u2082) from R1 and lowers the efficiency of R1 as a sink for radicals. The cis-cis conformer of HOONO was detected through its fundamental \u03bd\u2081(OH stretch) spectrum centered at 3306 cm\u207b\u00b9. The integrated absorbance of the \u03bd\u2081 bands for HOONO and HONO\u2082 were measured with CRDS and used to calculate the branching ratio (BR = kHOONO / kHONO2) of R1. Initial experiments using a microwave discharge to initiate R1 measured BR at 298 K and 14 torr, but were limited to low pressures by the discharge. BR was then reinvestigated using pulsed laser photolysis to initiate R1. BR was measured over the range 20\u2013760 torr at 298 K.
\r\n\r\nIn support of these branching ratio measurements, a detailed study of the spectroscopy of HONO\u2082 was conducted. CRDS experiments with moderate resolution (1 cm\u207b\u00b9) are known to give incorrect absorbances and line shaes when measuring spectral features with much narrower linewidths. However, the magnitude of these CRDS errors when probing a highly congested spectrum such as that of HONO\u2082 was unknown. We observed reductions in the HONO\u2082 integrated intensity up to 60% and quantified these errors as a function of concentration and pressure.
\r\n\r\nAlkoxy radicals (RO) are an important class of intermediates in the oxidation of hydrocarbons, and they react via several mechanisms. For longer chain RO isomerization (forming HOR) becomes a major pathway, but isomerization rates have never been directly measured. Continuing work described in Eva Garland\u2019s thesis, we measured the infrared spectrum of alkoxy radical isomerization products (HOR and HORO2) formed within 100 \u00b5s. We then used this spectrum to measure the relative rate of isomerization to reaction with oxygen for n-butoxy and 2-pentoxy radicals.
", "date": "2007", "date_type": "degree", "id_number": "CaltechETD:etd-05242007-095914", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05242007-095914", "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": "2007-05-31", "doi": "10.7907/HSF6-WM41", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "mo@caltech.edu", "id": "Okumura-M", "name": { "family": "Okumura", "given": "Mitchio" }, "role": "advisor" }, { "email": "stanley.p.sander@jpl.nasa.gov", "id": "Sander-S-P", "name": { "family": "Sander", "given": "Stanley P." }, "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "collier@caltech.edu", "id": "Collier-C-P", "name": { "family": "Collier", "given": "C. Patrick" }, "role": "chair" }, { "email": "mo@caltech.edu", "id": "Okumura-M", "name": { "family": "Okumura", "given": "Mitchio" }, "role": "member" }, { "email": "nslewis@caltech.edu", "id": "Lewis-N-S", "name": { "family": "Lewis", "given": "Nathan Saul" }, "role": "member" }, { "email": "wennberg@gps.caltech.edu", "id": "Wennberg-P-O", "name": { "family": "Wennberg", "given": "Paul O." }, "role": "member" }, { "email": "stanley.p.sander@jpl.nasa.gov", "id": "Sander-S-P", "name": { "family": "Sander", "given": "Stanley P." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2007-05-24", "thesis_defense_date": "2007-05-18", "thesis_approved_date": "2007-05-31", "gradofc_approval_date": "2007-05-30", "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": "2007", "author_list": "Mollner, Andrew Keeler", "advisor_list": "Okumura, Mitchio and Sander, Stanley P.", "comittee_list": "Collier, C. Patrick; Okumura, Mitchio; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/6804", "eprint_id": 6804, "rev_number": 21, "documents": [ { "id": "/id/document/14170", "doc_id": 14170, "rev_number": 5, "files": [ { "id": "/id/file/91234", "fileid": 91234, "datasetid": "document", "objectid": 14170, "filename": "Rosario-Ortiz_fl_2002.pdf", "mime_type": "application/pdf", "filesize": 15406967, "mtime": "2012-12-26 04:40:07", "url": "/6804/1/Rosario-Ortiz_fl_2002.pdf" } ], "eprint_id": 6804, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": "Rosario-Ortiz_fl_2002.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/27789" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/27789" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/27789" } ] } }, { "id": "/id/document/14171", "doc_id": 14171, "rev_number": 3, "files": [ { "id": "/id/file/207714", "fileid": 207714, "datasetid": "document", "objectid": 14171, "filename": "Rosario-Ortiz_fl_2002.zip", "mime_type": "application/zip", "filesize": 48620046, "mtime": "2016-08-22 21:23:33", "url": "/6804/2/Rosario-Ortiz_fl_2002.zip" } ], "eprint_id": 6804, "pos": 2, "format": "application/zip", "format_desc": "TIFF", "language": "en", "security": "internal", "license": "other", "main": "Rosario-Ortiz_fl_2002.zip", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final" }, { "id": "/id/document/27789", "doc_id": 27789, "rev_number": 3, "files": [ { "id": "/id/file/91232", "fileid": 91232, "datasetid": "document", "objectid": 27789, "filename": "preview.png", "mime_type": "image/png", "hash": "e5a1e0cd5fdae3278bdf1313021bc23c", "hash_type": "MD5", "filesize": 28807, "mtime": "2012-12-26 04:40:07", "url": "/6804/3/preview.png" } ], "eprint_id": 6804, "pos": 3, "placement": 3, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "public", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/14170" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/14170" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/14170" } ] } }, { "id": "/id/document/127184", "doc_id": 127184, "rev_number": 1, "files": [ { "id": "/id/file/372618", "fileid": 372618, "datasetid": "document", "objectid": 127184, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "18333deff64746aa546e0195af311ab0", "hash_type": "MD5", "filesize": 17083, "mtime": "2021-06-24 01:31:42", "url": "/6804/4/indexcodes.txt" } ], "eprint_id": 6804, "pos": 4, "placement": 4, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/14170" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/14170" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/14170" } ] } } ], "eprint_status": "archive", "userid": 87, "dir": "disk0/00/00/68/04", "datestamp": "2012-02-02 17:59:10", "lastmod": "2022-08-18 22:47:44", "status_changed": "2012-02-02 17:59:10", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Rosario-Ortiz-Fernando-L", "name": { "family": "Rosario-Ortiz", "given": "Fernando L." }, "show_email": "NO" } ] }, "title": "Determination of the Relative Line Strengths of the A\u00b2A' \u2190 X\u00b2A\" and (200)\u2190(000) transitions of HO\u2082", "ispublished": "unpub", "full_text_status": "public", "keywords": "Chemistry", "abstract": "The hydroperoxyl radical (HO\u2082) has been one of the most studied triatomic radicals during the past few decades. Its roles in atmospheric chemistry through the HO\u2093 cycle as well as in processes such as combustion have made the study of this radical extremely important. In the past three decades the interest in the spectroscopy of this molecule has increased due in part by the need of detecting this radical in several different environments. Although its UV, mid- and far-IR transitions have been studied extensively, its near-IR transitions have not received much attention until recently. Among the transitions observed in this region, the A\u00b2A' \u2190 X\u00b2A\" first electronic transition and the (200)\u2190(000) first OH overtone transition are two of the most important. These bands offer many advantages for detection of HO\u2082 in kinetic experiments and possibly in situ. Due to the importance of these two bands, information on their intensity is needed to measure accurately the concentration of HO\u2082. An apparatus has been constructed to measure the line strengths of the A \u2190 X electronic transition at 1.43 \u00b5m and the (200)\u2190(000) first OH overtone transition at 1.51 \u00b5m by diode laser absorption spectroscopy.", "date": "2002", "date_type": "degree", "id_number": "CaltechTHESIS:02022012-093757351", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:02022012-093757351", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Tony Diaz", "deposited_by": "Benjamin Perez", "deposited_on": "2012-02-02 17:59:10", "doi": "10.7907/vh44-fh68", "divisions": { "items": [ "div_chem" ] }, "institution": "California Institute of Technology", "thesis_type": "masters", "thesis_advisor": { "items": [ { "id": "Okumura-M", "name": { "family": "Okumura", "given": "Mitchio" }, "orcid": "0000-0001-6874-1137", "role": "advisor" }, { "id": "Sander-S-P", "name": { "family": "Sander", "given": "Stanley P." }, "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "name": { "family": "Unknown", "given": "Unknown" } } ] }, "thesis_degree": "MS", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2001-09-28", "review_status": "approved", "option_major": { "items": [ "chemistry" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2002", "author_list": "Rosario-Ortiz, Fernando L.", "advisor_list": "Okumura, Mitchio and Sander, Stanley P.", "comittee_list": "Unknown, Unknown" } ]