Coherent lattice and molecular dynamics in ultrafast single-shot spectroscopy

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.

Department dc:contributor.department

Massachusetts Institute of Technology. Dept. of Chemistry.

Grantor dc:publisher

Massachusetts Institute of Technology

Year dc:date.issued

2005

Author dc:creator

• Poulin, Peter Roland, 1973-

Advisor dc:contributor.advisor

• Keith A. Nelson.

• Chemistry.

Statement dc:rights

• 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.

Licence dc:rights.uri

• http://dspace.mit.edu/handle/1721.1/7582

Language dc:language.iso

eng

Handle dc:identifier.uri

http://hdl.handle.net/1721.1/32430

OAI identifier oai:identifier

oai:dspace.mit.edu:1721.1/32430