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Simulating Quantum Vibronic Dynamics at Finite Temperatures With Many Body Wave Functions at 0 K
For complex molecules, nuclear degrees of freedom can act as an environment for the electronic “system” variables, allowing the theory and concepts of open quantum systems to be applied. However, when molecular system-environment interactions are non-perturbative and non-Markovian, numerical simulat...
Autores principales: | , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Frontiers Media S.A.
2021
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7831969/ https://www.ncbi.nlm.nih.gov/pubmed/33505954 http://dx.doi.org/10.3389/fchem.2020.600731 |
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author | Dunnett, Angus J. Chin, Alex W. |
author_facet | Dunnett, Angus J. Chin, Alex W. |
author_sort | Dunnett, Angus J. |
collection | PubMed |
description | For complex molecules, nuclear degrees of freedom can act as an environment for the electronic “system” variables, allowing the theory and concepts of open quantum systems to be applied. However, when molecular system-environment interactions are non-perturbative and non-Markovian, numerical simulations of the complete system-environment wave function become necessary. These many body dynamics can be very expensive to simulate, and extracting finite-temperature results—which require running and averaging over many such simulations—becomes especially challenging. Here, we present numerical simulations that exploit a recent theoretical result that allows dissipative environmental effects at finite temperature to be extracted efficiently from a single, zero-temperature wave function simulation. Using numerically exact time-dependent variational matrix product states, we verify that this approach can be applied to vibronic tunneling systems and provide insight into the practical problems lurking behind the elegance of the theory, such as the rapidly growing numerical demands that can appear for high temperatures over the length of computations. |
format | Online Article Text |
id | pubmed-7831969 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | Frontiers Media S.A. |
record_format | MEDLINE/PubMed |
spelling | pubmed-78319692021-01-26 Simulating Quantum Vibronic Dynamics at Finite Temperatures With Many Body Wave Functions at 0 K Dunnett, Angus J. Chin, Alex W. Front Chem Chemistry For complex molecules, nuclear degrees of freedom can act as an environment for the electronic “system” variables, allowing the theory and concepts of open quantum systems to be applied. However, when molecular system-environment interactions are non-perturbative and non-Markovian, numerical simulations of the complete system-environment wave function become necessary. These many body dynamics can be very expensive to simulate, and extracting finite-temperature results—which require running and averaging over many such simulations—becomes especially challenging. Here, we present numerical simulations that exploit a recent theoretical result that allows dissipative environmental effects at finite temperature to be extracted efficiently from a single, zero-temperature wave function simulation. Using numerically exact time-dependent variational matrix product states, we verify that this approach can be applied to vibronic tunneling systems and provide insight into the practical problems lurking behind the elegance of the theory, such as the rapidly growing numerical demands that can appear for high temperatures over the length of computations. Frontiers Media S.A. 2021-01-07 /pmc/articles/PMC7831969/ /pubmed/33505954 http://dx.doi.org/10.3389/fchem.2020.600731 Text en Copyright © 2021 Dunnett and Chin. http://creativecommons.org/licenses/by/4.0/ This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use, distribution or reproduction in other forums is permitted, provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these terms. |
spellingShingle | Chemistry Dunnett, Angus J. Chin, Alex W. Simulating Quantum Vibronic Dynamics at Finite Temperatures With Many Body Wave Functions at 0 K |
title | Simulating Quantum Vibronic Dynamics at Finite Temperatures With Many Body Wave Functions at 0 K |
title_full | Simulating Quantum Vibronic Dynamics at Finite Temperatures With Many Body Wave Functions at 0 K |
title_fullStr | Simulating Quantum Vibronic Dynamics at Finite Temperatures With Many Body Wave Functions at 0 K |
title_full_unstemmed | Simulating Quantum Vibronic Dynamics at Finite Temperatures With Many Body Wave Functions at 0 K |
title_short | Simulating Quantum Vibronic Dynamics at Finite Temperatures With Many Body Wave Functions at 0 K |
title_sort | simulating quantum vibronic dynamics at finite temperatures with many body wave functions at 0 k |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7831969/ https://www.ncbi.nlm.nih.gov/pubmed/33505954 http://dx.doi.org/10.3389/fchem.2020.600731 |
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