Attosecond channel-coupling in molecular photoionization delays
Abstract/Contents
- Abstract
- Molecular and chemical physics rely heavily on the use of approximations and simplifying models to deal with the complex reality of many-body electronic interactions. Although these models are essential, they have their limitations. One important area where simplifying models break down is in the examination of electronic channel-coupling. Photoionization channel-coupling is defined as mixing multiple continuum channels of the scattering photoelectron, caused by attosecond-scale multielectron interactions. Channel-coupling in photoionization is challenging to measure and model because it is a time-dependent phenomenon. Most models will simplify out the dynamic electronic environment, and experimental observables similarly cannot access the intermediate states at attosecond timescales. The photoionization time delay, an interferometric measurement of the group delay of the scattering electron wavepacket, offers a solution to this problem. Although it is not a time-dependent quantity, it is highly sensitive to the intermediate states and their interactions, since phase is accumulated throughout the entire half-scattering process of photoionization. This sensitivity can be leveraged to discriminate between models with various levels of electronic approximations, identifying the relevant electronic interactions and determining the correct level of detail needed to accurately describe the system. I measured the photoionization time delay in a variety of molecular systems that showcase different continuum channel-coupling phenomena. In each system, I show that analyzing the photoionization time delay in the context of models gives insight into the relevance of various interactions at the attosecond timescale. Through these experiments, I demonstrate that photoionization delays are an effective model discriminator for continuum channel-coupling induced by attosecond-scale electron interactions.
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 | 2022; ©2022 |
| Publication date | 2022; 2022 |
| Issuance | monographic |
| Language | English |
Creators/Contributors
| Author | Wang, Anna Li |
|---|---|
| Degree supervisor | Bucksbaum, Philip H |
| Thesis advisor | Bucksbaum, Philip H |
| Thesis advisor | Cryan, James |
| Thesis advisor | Reis, David A, 1970- |
| Thesis advisor | Schleier-Smith, Monika |
| Degree committee member | Cryan, James |
| Degree committee member | Reis, David A, 1970- |
| Degree committee member | Schleier-Smith, Monika |
| Associated with | Stanford University, Department of Applied Physics |
Subjects
| Genre | Theses |
|---|---|
| Genre | Text |
Bibliographic information
| Statement of responsibility | Anna Li Wang. |
|---|---|
| Note | Submitted to the Department of Applied Physics. |
| Thesis | Thesis Ph.D. Stanford University 2022. |
| Location | https://purl.stanford.edu/dz019nj9665 |
Access conditions
- Copyright
- © 2022 by Anna Li Wang
- License
- This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).
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