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Quantum Free Energy Profiles for Molecular Proton Transfers

Aran Lamaire, Maarten Cools‐Ceuppens, Massimo Bocus, Toon Verstraelen, Véronique Van Speybroeck

2022Journal of Chemical Theory and Computation12 citationsDOIOpen Access PDF

Abstract

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.

Topics & Concepts

Path integral formulationCentroidQuantumFormalism (music)Molecular dynamicsProtonPhysicsStatistical physicsQuantum simulatorQuantum mechanicsQuantum computerComputer scienceVisual artsArtMusicalArtificial intelligenceAdvanced Chemical Physics StudiesSpectroscopy and Quantum Chemical StudiesPhotochemistry and Electron Transfer Studies
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