Title: van der Waals Correction to the Physisorption of Graphene on Metal Surfaces

Abstract

Adsorption is a scientifically and technologically important interfacial phenomenon, which however presents challenges to conventional density functional theory (DFT) due to the long-range van der Waals (vdW) interactions. We have developed a model of long-range vdW correction for physisorption of graphene (G) on metals with the Lifshitz–Zaremba–Kohn second-order perturbation theory, by incorporating dipole- and quadrupole-surface interactions and screening effects. The physisorption energies calculated by the model between graphene and eight metal surfaces (Al, Ni, Co, Pd, Pt, Cu, Ag, and Au), and the adsorption energies for the same G/metal structures from self-consistent DFT PBE (Perdew–Burke–Ernzerhof) calculations, are obtained in a range of distances between G and the metal surfaces. The sum of these two parts is the total adsorption energy as a function of the distance, from which the equilibrium distance and the binding energy are determined simultaneously. The results show high accuracy, with the mean absolute error (MAE) of binding energy of 7 meV and the MAE of equilibrium distance of 0.2 Å, significantly improving upon other vdW methods. Here, the PBE + vdW binding energy curves give better fits to the random phase approximation curves around the equilibrium distances than do the curves of other methods considered here.more » The higher-order quadrupole-surface correction is important and accounts for about 30% of the total vdW correction.« less

Authors:

Tang, Hong  ^[1];

• Search DOE PAGES for author "Tang, Hong"
• Search DOE PAGES for ORCID "0000-0002-6221-0922"

Tao, Jianmin ^[1]; Ruzsinszky, Adrienn ^[1]; Perdew, John P. ^[1]

---

+ Show Author Affiliations

1. Temple Univ., Philadelphia, PA (United States)

Publication Date:

Wed May 08 00:00:00 EDT 2019

Research Org.:

Energy Frontier Research Centers (EFRC) (United States). Center for Complex Materials from First Principles (CCM); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Temple Univ., Philadelphia, PA (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

OSTI Identifier:

1577506

Grant/Contract Number:  

SC0012575; SC0018194; W911NF-16-2-0189; 1625061; CHE 1760814

Resource Type:

Accepted Manuscript

Journal Name:

Journal of Physical Chemistry. C

Additional Journal Information:

Journal Volume: 123; Journal Issue: 22; Journal ID: ISSN 1932-7447

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemistry; science & technology; other topics; materials science; metals; binding energy; adsorption; equilibrium; two dimensional materials