The binding of atomic hydrogen on graphene from density functional theory and diffusion Monte Carlo calculations

Amanda Dumi; Shiv Upadhyay; Leonardo Bernasconi; Hyeondeok Shin; Anouar Benali; Kenneth D Jordan

doi:10.1063/5.0085982

The binding of atomic hydrogen on graphene from density functional theory and diffusion Monte Carlo calculations

J Chem Phys. 2022 Apr 14;156(14):144702. doi: 10.1063/5.0085982.

Authors

Amanda Dumi¹, Shiv Upadhyay¹, Leonardo Bernasconi¹, Hyeondeok Shin², Anouar Benali², Kenneth D Jordan¹

Affiliations

¹ Department of Chemistry, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, USA.
² Computational Science Division, Argonne National Laboratory, Argonne, Illinois 60439, USA.

PMID: 35428395
DOI: 10.1063/5.0085982

Abstract

In this work, density functional theory (DFT) and diffusion Monte Carlo (DMC) methods are used to calculate the binding energy of a H atom chemisorbed on the graphene surface. The DMC value of the binding energy is about 16% smaller in magnitude than the Perdew-Burke-Ernzerhof (PBE) result. The inclusion of exact exchange through the use of the Heyd-Scuseria-Ernzerhof functional brings the DFT value of the binding energy closer in line with the DMC result. It is also found that there are significant differences in the charge distributions determined using PBE and DMC approaches.