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Decoherence and Its Role in Electronically Nonadiabatic Dynamics
[Image: see text] Decoherence is the tendency of a time-evolved reduced density matrix for a subsystem to assume a form corresponding to a statistical ensemble of states rather than a coherent combination of pure-state wave functions. When a molecular process involves changes in the electronic state...
Autores principales: | , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2023
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9878713/ https://www.ncbi.nlm.nih.gov/pubmed/36622843 http://dx.doi.org/10.1021/acs.jctc.2c00988 |
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author | Shu, Yinan Truhlar, Donald G. |
author_facet | Shu, Yinan Truhlar, Donald G. |
author_sort | Shu, Yinan |
collection | PubMed |
description | [Image: see text] Decoherence is the tendency of a time-evolved reduced density matrix for a subsystem to assume a form corresponding to a statistical ensemble of states rather than a coherent combination of pure-state wave functions. When a molecular process involves changes in the electronic state and the coordinates of the nuclei, as in ultraviolet or visible light photochemistry or electronically inelastic collisions, the reduced density matrix of the electronic subsystem suffers decoherence, due to its interaction with the nuclear subsystem. We present the background necessary to conceptualize this decoherence; in particular, we discuss the density matrix description of pure states and mixed states, and we discuss pointer states and decoherence time. We then discuss how decoherence is treated in the coherent switching with decay of mixing algorithm and the trajectory surface hopping method for semiclassical calculations of electronically nonadiabatic processes. |
format | Online Article Text |
id | pubmed-9878713 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-98787132023-01-27 Decoherence and Its Role in Electronically Nonadiabatic Dynamics Shu, Yinan Truhlar, Donald G. J Chem Theory Comput [Image: see text] Decoherence is the tendency of a time-evolved reduced density matrix for a subsystem to assume a form corresponding to a statistical ensemble of states rather than a coherent combination of pure-state wave functions. When a molecular process involves changes in the electronic state and the coordinates of the nuclei, as in ultraviolet or visible light photochemistry or electronically inelastic collisions, the reduced density matrix of the electronic subsystem suffers decoherence, due to its interaction with the nuclear subsystem. We present the background necessary to conceptualize this decoherence; in particular, we discuss the density matrix description of pure states and mixed states, and we discuss pointer states and decoherence time. We then discuss how decoherence is treated in the coherent switching with decay of mixing algorithm and the trajectory surface hopping method for semiclassical calculations of electronically nonadiabatic processes. American Chemical Society 2023-01-09 /pmc/articles/PMC9878713/ /pubmed/36622843 http://dx.doi.org/10.1021/acs.jctc.2c00988 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by-nc-nd/4.0/Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works (https://creativecommons.org/licenses/by-nc-nd/4.0/). |
spellingShingle | Shu, Yinan Truhlar, Donald G. Decoherence and Its Role in Electronically Nonadiabatic Dynamics |
title | Decoherence and Its Role in Electronically Nonadiabatic
Dynamics |
title_full | Decoherence and Its Role in Electronically Nonadiabatic
Dynamics |
title_fullStr | Decoherence and Its Role in Electronically Nonadiabatic
Dynamics |
title_full_unstemmed | Decoherence and Its Role in Electronically Nonadiabatic
Dynamics |
title_short | Decoherence and Its Role in Electronically Nonadiabatic
Dynamics |
title_sort | decoherence and its role in electronically nonadiabatic
dynamics |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9878713/ https://www.ncbi.nlm.nih.gov/pubmed/36622843 http://dx.doi.org/10.1021/acs.jctc.2c00988 |
work_keys_str_mv | AT shuyinan decoherenceanditsroleinelectronicallynonadiabaticdynamics AT truhlardonaldg decoherenceanditsroleinelectronicallynonadiabaticdynamics |