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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...

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Autores principales: Lamaire, Aran, Cools-Ceuppens, Maarten, Bocus, Massimo, Verstraelen, Toon, Van Speybroeck, Veronique
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
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.
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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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