Diffusion Monte Carlo Study of the O${}_2$ Adsorption on a Single Layer Graphene

Abstract

Diffusion Monte Carlo (DMC) calculations were performed for an accurate description of the nature of the O${}_2$ adsorption on a single layer graphene. We investigated the stable orientation of O${}_2$ at a specific adsorption site as well as its equilibrium adsorption energy. At equilibrium adsorption distances, an O${}_2$ molecule was found to prefer a horizontal orientation, where the O-O bond is parallel to the graphene surface, to the vertical orientation. However, the vertical orientation is favored at the O${}_2$-graphene distances shorter than the equilibrium distance, which could be understood by the steric repulsion between O and C atoms. Contrary to previous DFT calculations, our DMC calculations show that the midpoint of a C-C bond (a bridge site) is energetically preferred for the O${}_2$ adsorption to a center of a hexagonal ring (a hollow site). The lowest DMC adsorption energy was found at an intermediate point between a hollow and a bridge site, where the O${}_2$ adsorption energy was estimated to be -0.142(4) eV that was in very good agreement with the recently-reported experimental value. Finally, we have found that O${}_2$ is very diffusive on the surface of graphene with the diffusion barrier along a bridge-hollow-bridge path being as small as ~ 11 meV.

arXiv comment19 pages, 7 figures

References in corpus (17)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Two-Dimensional Gas of Massless Dirac Fermions in Graphene
• Graphene: Status and Prospects
• Experimental Observation of Quantum Hall Effect and Berry's Phase in Graphene
• Detection of Individual Gas Molecules Absorbed on Graphene
• Van der Waals Density Functional for General Geometries
• A Higher-Accuracy van der Waals Density Functional
• Molecular Doping of Graphene
• Twist-averaged Boundary Conditions in Continuum Quantum Monte Carlo
• The Nature of the Interlayer Interaction in Bulk and Few-Layer Phosphorus
• QMCPACK : An open source ab initio Quantum Monte Carlo package for the electronic structure of atoms, molecules, and solids
• Quantum Monte Carlo Calculation of the Binding Energy of Bilayer Graphene
• Cohesion Energetics of Carbon Allotropes : Quantum Monte Carlo Study
• Size-consistent variational approaches to non-local pseudopotentials: standard and lattice regularized diffusion Monte Carlo methods revisited
• Phase Stability of TiO${}_2$ Polymorphs from Diffusion Quantum Monte Carlo
• Quantum Monte Carlo analysis of a charge ordered insulating antiferromagnet: the Ti${}_4$O${}_7$ Magnéli phase
• Temperature induced inversion of oxygen response in CVD graphene on SiO2

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