From time-resolved to frequency-resolved x-ray scattering
Abstract/Contents
- Abstract
- Gas-phase time-resolved x-ray scattering (TRXS) measures internuclear separations in a molecule following laser-induced photoexcitation. TRXS constitutes an indirect measurement of the molecular motion because it captures information in reciprocal-space and real-time, which then must be inverted to recover the charge density as it changes in time. The spatial resolution of the recovered charge density is fundamentally restricted by the x-ray wavelength used in the experiment. There is no corresponding technical restriction on the ability to scan the delay between the pump-laser pulse and the x-ray-probe pulses, and thus no lower limit on the ability to resolve beat frequencies from TRXS measurements. This observation motivates transforming the measured TRXS in reciprocal-space and real-time into its reciprocal-space and reciprocal-time representation through a temporal Fourier transform. This representation is called frequency-resolved x-ray scattering (FRXS). The novel aspect of this approach is that an interpretable and compact representation of the experimental measurement may be obtained in reciprocal-space and reciprocal-time without the difficulty of inverting the measurement to the traditional real-space and time representation, and thus FRXS presents an alternative to traditional analyses of TRXS. The traditional approach based on pair correlation functions is limited by the range of momentum transfer, Q, that is accessible at x-ray free electron lasers (FELs). FRXS does not suffer this limitation, and in fact, FRXS leverages the strengths of FELs, namely fine time resolution and (relatively) fast data accumulation. This enables a long range of pump-probe delays to be measured in an experiment, thus improving the frequency resolution of an experiment, while maintaining sufficient temporal resolution to measure high beat frequencies. These advantages have been used to obtain compact representations of bound states and dissociations along lines in reciprocal-space and reciprocal-time, demonstrating an alternative to traditional analyses of time-resolved x-ray scattering for gas-phase photochemistry.
Description
| Type of resource | text |
|---|---|
| Form | electronic resource; remote; computer; online resource |
| Extent | 1 online resource. |
| Place | California |
| Place | [Stanford, California] |
| Publisher | [Stanford University] |
| Copyright date | 2019; ©2019 |
| Publication date | 2019; 2019 |
| Issuance | monographic |
| Language | English |
Creators/Contributors
| Author | Ware, Matthew Robert | |
|---|---|---|
| Degree supervisor | Bucksbaum, Philip H | |
| Thesis advisor | Bucksbaum, Philip H | |
| Thesis advisor | Martinez, Todd J. (Todd Joseph), 1968- | |
| Thesis advisor | Reis, David A, 1970- | |
| Degree committee member | Martinez, Todd J. (Todd Joseph), 1968- | |
| Degree committee member | Reis, David A, 1970- | |
| Associated with | Stanford University, Department of Physics. |
Subjects
| Genre | Theses |
|---|---|
| Genre | Text |
Bibliographic information
| Statement of responsibility | Matthew Robert Ware. |
|---|---|
| Note | Submitted to the Department of Physics. |
| Thesis | Thesis Ph.D. Stanford University 2019. |
| Location | electronic resource |
Access conditions
- Copyright
- © 2019 by Matthew Robert Ware
- License
- This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).
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