Quantum and classical molecular dynamics for H atom scattering from graphene - Archive ouverte HAL
Article Dans Une Revue The Journal of Chemical Physics Année : 2023

Quantum and classical molecular dynamics for H atom scattering from graphene

Lei Shi
Université Paris-Saclay
Laboratoire de Mathématiques d'Orsay
Markus Schröder
Hans-Dieter Meyer
Daniel Peláez
Alec Wodtke
Kai Golibrzuch
Anna-Maria Schönemann
Alexander Kandratsenka
Fabien Gatti
CV

Résumé

This work presents systematic comparisons between classical molecular dynamics (cMD) and quantum dynamics (QD) simulations of 15-dimensional and 75-dimensional models in their description of H atom scattering from graphene. We use an experimentally validated full-dimensional neural network potential energy surface of a hydrogen atom interacting with a large cell of graphene containing 24 carbon atoms. For quantum dynamics simulations, we apply Monte Carlo canonical polyadic decomposition to transform the original potential energy surface (PES) into a sum of products form and use the multi-layer multi-configuration time-dependent Hartree method to simulate the quantum scattering of a hydrogen or deuterium atom with an initial kinetic energy of 1.96 or 0.96 eV and an incident angle of 0°, i.e., perpendicular to the graphene surface. The cMD and QD initial conditions have been carefully chosen in order to be as close as possible. Our results show little differences between cMD and QD simulations when the incident energy of the H atom is equal to 1.96 eV. However, a large difference in sticking probability is observed when the incident energy of the H atom is equal to 0.96 eV, indicating the predominance of quantum effects. To the best of our knowledge, our work provides the first benchmark of quantum against classical simulations for a system of this size with a realistic PES. Additionally, new projectors are implemented in the Heidelberg multi-configuration time-dependent Hartree package for the calculation of the atom scattering energy transfer distribution as a function of outgoing angles.

Domaines

Chimie théorique et/ou physique

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https://hal.science/hal-04351769

Soumis le : lundi 18 décembre 2023-19:25:32

Dernière modification le : mercredi 15 mai 2024-12:40:28

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Dates et versions

hal-04351769 , version 1 (18-12-2023)

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Lei Shi, Markus Schröder, Hans-Dieter Meyer, Daniel Peláez, Alec Wodtke, et al.. Quantum and classical molecular dynamics for H atom scattering from graphene. The Journal of Chemical Physics, 2023, 159 (19), ⟨10.1063/5.0176655⟩. ⟨hal-04351769⟩

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