Towards accessible quantum chemistry and automated photochemical design via machine learning and nonadiabatic dynamics simulation
Abstract/Contents
- Abstract
- The ability to reliably design molecular systems for targeted applications has the potential to revolutionize drug and material discovery. Quantum chemistry can now accurately predict useful chemical properties for a wide range of molecules and continues to enhance its predictive power as new algorithms and hardware come online. However, several major hurdles remain. In this work, I focus on two outstanding challenges: building accessible tools for the wider chemistry community to interact with quantum chemistry, and designing photochemical systems with nonadiabatic dynamics simulations. I develop ChemPix, a hand-drawn hydrocarbon structure recognition software to provide an almost barrierless molecule input method for computational chemistry software. ChemPix and other accessible molecular input tools are combined with cloud-based GPU- accelerated quantum chemistry and extended reality visualization to build a series of interactive quantum chemistry tools. These tools can compute quantum mechanical properties in real-time from hand-drawn structures or voice input. Photochemical systems can be modeled with nonadiabatic dynamics simulations. However, the complex multi-reference electronic structure calculations required for these simulations means that modelling even simple photochemical processes demands domain expertise and substantial human effort. Here, I employ cis-stilbene, a prototypical photo- switch, to explore the path towards automated photochemical design. First, nonadiabatic dynamics simulations of cis-stilbene are performed and analyzed to uncover the cis-trans photoisomerization and photocyclization mechanisms. Next, I propose the use of ensembled simulations to build stronger mechanistic predictors and link the predictions to the experimental ultrafast electron diffraction signal. Finally, a highly symmetric light- induced molecular motor is designed based on the simulations by photo-exciting cis- stilbene with circularly polarized light.
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 | Weir, Hayley Victoria |
|---|---|
| Degree supervisor | Martinez, Todd J. (Todd Joseph), 1968- |
| Thesis advisor | Martinez, Todd J. (Todd Joseph), 1968- |
| Thesis advisor | Markland, Thomas E |
| Thesis advisor | Rotskoff, Grant |
| Degree committee member | Markland, Thomas E |
| Degree committee member | Rotskoff, Grant |
| Associated with | Stanford University, Department of Chemistry |
Subjects
| Genre | Theses |
|---|---|
| Genre | Text |
Bibliographic information
| Statement of responsibility | Hayley Weir. |
|---|---|
| Note | Submitted to the Department of Chemistry. |
| Thesis | Thesis Ph.D. Stanford University 2022. |
| Location | https://purl.stanford.edu/bd879hw9651 |
Access conditions
- Copyright
- © 2022 by Hayley Victoria Weir
- License
- This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).
Also listed in
Loading usage metrics...