Towards 3D molecular movies : electron orbital signatures in asymmetric tops
Abstract/Contents
- Abstract
- High-order harmonic generation in atoms or linear molecules offers valuable information about valence electrons. When combined with molecular alignment, high harmonic generation is sensitive to both Angstrom-scale structure and sub-femtosecond dynamics, and can even create very simple movies of molecules in motion. Extending these techniques to more complex molecules with three distinct dimensions is hindered, however, by the interference of radiation from random molecular orientations. In this dissertation, I demonstrate a solution to this dilemma by making use of the full-scale molecular revival pattern of a three-dimensional asymmetric top. I present an alignment-decomposition approach based on methods derived from rotational coherence spectroscopy and test them on the asymmetric-top molecule sulfur dioxide. I then apply this approach to experimental results from the full sulfur dioxide high-harmonic spectrum and show that prominent spectral features must be due to ionization and recombination from multiple molecular orbitals. These results simplify the task of spectral analysis and extend the usefulness of high harmonic generation to increasingly complicated molecules. They provide a first step towards constructing real, three-dimensional molecular movies.
Description
| Type of resource | text |
|---|---|
| Form | electronic; electronic resource; remote |
| Extent | 1 online resource. |
| Publication date | 2013 |
| Issuance | monographic |
| Language | English |
Creators/Contributors
| Associated with | Spector, Limor Shoshana |
|---|---|
| Associated with | Stanford University, Department of Applied Physics. |
| Primary advisor | Bucksbaum, Philip H |
| Thesis advisor | Bucksbaum, Philip H |
| Thesis advisor | Kasevich, Mark A |
| Thesis advisor | Martinez, Todd J. (Todd Joseph), 1968- |
| Advisor | Kasevich, Mark A |
| Advisor | Martinez, Todd J. (Todd Joseph), 1968- |
Subjects
| Genre | Theses |
|---|
Bibliographic information
| Statement of responsibility | Limor Shoshana Spector. |
|---|---|
| Note | Submitted to the Department of Applied Physics. |
| Thesis | Thesis (Ph.D.)--Stanford University, 2013. |
| Location | electronic resource |
Access conditions
- Copyright
- © 2013 by Limor Shoshana Spector
- License
- This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).
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