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Quantum Free Energy Profiles for Molecular Proton Transfers
[Image: see text] Although many molecular dynamics simulations treat the atomic nuclei as classical particles, an adequate description of nuclear quantum effects (NQEs) is indispensable when studying proton transfer reactions. Herein, quantum free energy profiles are constructed for three typical pr...
Autores principales: | , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2022
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9835831/ https://www.ncbi.nlm.nih.gov/pubmed/36563337 http://dx.doi.org/10.1021/acs.jctc.2c00874 |
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author | Lamaire, Aran Cools-Ceuppens, Maarten Bocus, Massimo Verstraelen, Toon Van Speybroeck, Veronique |
author_facet | Lamaire, Aran Cools-Ceuppens, Maarten Bocus, Massimo Verstraelen, Toon Van Speybroeck, Veronique |
author_sort | Lamaire, Aran |
collection | PubMed |
description | [Image: see text] Although many molecular dynamics simulations treat the atomic nuclei as classical particles, an adequate description of nuclear quantum effects (NQEs) is indispensable when studying proton transfer reactions. Herein, quantum free energy profiles are constructed for three typical proton transfers, which properly take NQEs into account using the path integral formalism. The computational cost of the simulations is kept tractable by deriving machine learning potentials. It is shown that the classical and quasi-classical centroid free energy profiles of the proton transfers deviate substantially from the exact quantum free energy profile. |
format | Online Article Text |
id | pubmed-9835831 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-98358312023-01-13 Quantum Free Energy Profiles for Molecular Proton Transfers Lamaire, Aran Cools-Ceuppens, Maarten Bocus, Massimo Verstraelen, Toon Van Speybroeck, Veronique J Chem Theory Comput [Image: see text] Although many molecular dynamics simulations treat the atomic nuclei as classical particles, an adequate description of nuclear quantum effects (NQEs) is indispensable when studying proton transfer reactions. Herein, quantum free energy profiles are constructed for three typical proton transfers, which properly take NQEs into account using the path integral formalism. The computational cost of the simulations is kept tractable by deriving machine learning potentials. It is shown that the classical and quasi-classical centroid free energy profiles of the proton transfers deviate substantially from the exact quantum free energy profile. American Chemical Society 2022-12-23 /pmc/articles/PMC9835831/ /pubmed/36563337 http://dx.doi.org/10.1021/acs.jctc.2c00874 Text en © 2022 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 | Lamaire, Aran Cools-Ceuppens, Maarten Bocus, Massimo Verstraelen, Toon Van Speybroeck, Veronique Quantum Free Energy Profiles for Molecular Proton Transfers |
title | Quantum Free Energy
Profiles for Molecular Proton
Transfers |
title_full | Quantum Free Energy
Profiles for Molecular Proton
Transfers |
title_fullStr | Quantum Free Energy
Profiles for Molecular Proton
Transfers |
title_full_unstemmed | Quantum Free Energy
Profiles for Molecular Proton
Transfers |
title_short | Quantum Free Energy
Profiles for Molecular Proton
Transfers |
title_sort | quantum free energy
profiles for molecular proton
transfers |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9835831/ https://www.ncbi.nlm.nih.gov/pubmed/36563337 http://dx.doi.org/10.1021/acs.jctc.2c00874 |
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