Inner valence contributions and phase-matching effects in high-harmonic spectroscopy
Abstract/Contents
- Abstract
- Laser driven high-order harmonics can be used to monitor electron dynamics in molecules with angstrom spatial resolution and sub-femtosecond time resolution. I will discuss experiments extending high harmonic spectroscopy on two fronts: phase-matching and multiple orbital effects. First, measurable harmonic yields require phase-matched emission from macroscopic numbers of molecules. Due to this, observed spectra contain both single molecule and macroscopic responses. We study phase-matching's influence on spectral information using the Cooper Minimum in Argon as a spectral marker. In addition, we develop a phase-matching-based highly dispersive transient Bragg gratings scheme, which shows that phase-matching can actively be used in high harmonic spectroscopy experiments. Second, high harmonics originating from several valence orbitals and their subsequent interferences offers dynamical information but complicates the interpretation of data. Using molecular nitrogen, we show that adjustment and control of the molecular axis can to some extent isolate the contribution of an inner valence orbital. Using water, we demonstrate a different scheme for isolating inner valence contributions based on isotopic substitution. This technique marks the ionizing orbitals by the vibrational motion during the first femtosecond following ionization. These results show that inner valence contributions are ubiquitous and can be isolated even without vibrational or rotational pre-excitation.
Description
| Type of resource | text |
|---|---|
| Form | electronic; electronic resource; remote |
| Extent | 1 online resource. |
| Publication date | 2012 |
| Issuance | monographic |
| Language | English |
Creators/Contributors
| Associated with | Farrell, Joseph Patrick |
|---|---|
| Associated with | Stanford University, Department of Physics |
| Primary advisor | Bucksbaum, Philip H |
| Thesis advisor | Bucksbaum, Philip H |
| Thesis advisor | Martinez, Todd J. (Todd Joseph), 1968- |
| Thesis advisor | Reis, David A, 1970- |
| Advisor | Martinez, Todd J. (Todd Joseph), 1968- |
| Advisor | Reis, David A, 1970- |
Subjects
| Genre | Theses |
|---|
Bibliographic information
| Statement of responsibility | Joe Farrell. |
|---|---|
| Note | Submitted to the Department of Physics. |
| Thesis | Thesis (Ph.D.)--Stanford University, 2012. |
| Location | electronic resource |
Access conditions
- Copyright
- © 2012 by Joseph Patrick Farrell
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