Nuclear Quantum Effects in Scattering of H and D from Graphene

TL;DR

This paper investigates how nuclear quantum effects influence hydrogen and deuterium scattering on graphene, demonstrating improved agreement with experiments when quantum effects are included, and highlighting the importance of phonon dynamics.

Contribution

It introduces a detailed comparison of classical, quantum, and mixed simulations for H/D scattering on graphene, emphasizing the role of nuclear quantum effects and phonon dynamics.

Findings

Quantum effects increase sticking probabilities.

Inclusion of phonon dynamics improves experimental agreement.

An inverse isotope effect is observed from Newtonian mechanics.

Abstract

We present a detailed study of the nuclear quantum effects in H/D sticking to graphene, comparing classical, quantum and mixed quantum/classical simulations to results of scattering experiments. Agreement with experimentally derived sticking probabilities is improved when nuclear quantum effects are included using ring polymer molecular dynamics. Specifically, the quantum motion of the carbon atoms enhances sticking, showing that an accurate description of graphene phonons is important to capturing the adsorption dynamics. We also find an inverse H/D isotope effect arising from Newtonian mechanics.