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Keith A. Nelson. Poulin, Peter Roland, 1973- Massachusetts Institute of Technology. Dept. of Chemistry. Massachusetts Institute of Technology. Department of Chemistry 2006-03-29T18:43:57Z 2006-03-29T18:43:57Z 2005 2005 http://hdl.handle.net/1721.1/32430 61717974 Thesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Chemistry, 2005. Includes bibliographical references. This thesis focuses on the development, refinement, and application of dual- echelon single-shot ultrafast spectroscopy to the study of coherent nuclear motion in condensed phase systems. The general principles of the single-shot method are described, and particular emphasis is given to the general applicability and shortcomings of this technique and the extraction of data from raw laboratory images. Coupled to the single-shot system is a synchronously pumped dual-beam noncollinear optical parametric amplifier which was developed to provide independently tunable pump and probe beams in the visible and UV regions of the electromagnetic spectrum. The second part of the thesis concerns the application of this technique to the study of atomic motions in liquids and solids. Single-shot nonresonant impulsive stimulated Raman scattering (ISRS) measurements in m-iodoanisole and bismuth germanate reveal the existence of transient coherent behavior. High-field resonant excitation of the semimetals bismuth, antimony and tellurium, as well as the semiconductor germanium telluride, reveals dramatic lattice anharmoniticity as a function of pump fluence. Finally, ultrafast photodissociation of the triiodide ion both in solution and in the solid state gives considerable insight regarding the role of the local environment in mediating chemical reaction dynamics. by Peter Roland Poulin. Ph.D. 413 p. 18648321 bytes 18678804 bytes application/pdf application/pdf eng Massachusetts Institute of Technology M.I.T. theses are protected by copyright. They may be viewed from this source for any purpose, but reproduction or distribution in any format is prohibited without written permission. See provided URL for inquiries about permission. http://dspace.mit.edu/handle/1721.1/7582 Chemistry. Coherent lattice and molecular dynamics in ultrafast single-shot spectroscopy Thesis application/pdf Publication unknown unknown <Publication xmlns="https://www.openaire.eu/cerif-profile/1.1/" id="ec2301fd-4c8f-42c5-8a24-696e7a6c7814"> <Type xmlns="https://www.openaire.eu/cerif-profile/vocab/COAR_Publication_Types">http://purl.org/coar/resource_type/c_1843</Type> <Language>eng</Language> <Title>Coherent lattice and molecular dynamics in ultrafast single-shot spectroscopy</Title> <PublishedIn> <Publication> </Publication> </PublishedIn> <PublicationDate>2005</PublicationDate> <Authors> <Author> <DisplayName>Poulin, Peter Roland, 1973-</DisplayName> <Affiliation> <OrgUnit> </OrgUnit> </Affiliation> </Author> </Authors> <Editors> </Editors> <Publishers> <Publisher> <DisplayName>Massachusetts Institute of Technology</DisplayName> <OrgUnit /> </Publisher> </Publishers> <License>http://dspace.mit.edu/handle/1721.1/7582</License> <Keyword>Chemistry.</Keyword> <Abstract>This thesis focuses on the development, refinement, and application of dual- echelon single-shot ultrafast spectroscopy to the study of coherent nuclear motion in condensed phase systems. The general principles of the single-shot method are described, and particular emphasis is given to the general applicability and shortcomings of this technique and the extraction of data from raw laboratory images. Coupled to the single-shot system is a synchronously pumped dual-beam noncollinear optical parametric amplifier which was developed to provide independently tunable pump and probe beams in the visible and UV regions of the electromagnetic spectrum. The second part of the thesis concerns the application of this technique to the study of atomic motions in liquids and solids. Single-shot nonresonant impulsive stimulated Raman scattering (ISRS) measurements in m-iodoanisole and bismuth germanate reveal the existence of transient coherent behavior. High-field resonant excitation of the semimetals bismuth, antimony and tellurium, as well as the semiconductor germanium telluride, reveals dramatic lattice anharmoniticity as a function of pump fluence. Finally, ultrafast photodissociation of the triiodide ion both in solution and in the solid state gives considerable insight regarding the role of the local environment in mediating chemical reaction dynamics.</Abstract> <Access xmlns="http://purl.org/coar/access_right" > </Access> </Publication>