Coherent lattice and molecular dynamics in ultrafast single-shot spectroscopy
Name
61717974-MIT.pdf
Description
Full printable version
Size
17.81 MB
Format
Adobe PDF
Checksum (MD5)
a80c78d78cf81055fd73efddc7bb524e
Author(s)
Poulin, Peter Roland, 1973-
Advisor(s)
Keith A. Nelson.
Date Issued
2005
Publisher
Massachusetts Institute of Technology
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.
Description
Thesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Chemistry, 2005.
Includes bibliographical references.
Subjects
Chemistry.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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