Calculation of Zn, Cd, Hg adsorption on graphene with incremental CCSD(T) and range-separated hybrid DFT*

ABSTRACT

At the hand of the adsorption of the metal atoms Zn, Cd and Hg on a graphene sheet, we propose a combination of range-separated hybrid density-functional theory in combination with the incremental scheme in localised orbitals and extrapolation procedures for the description of this type of extended systems. Using only dispersion terms for the long-range part, we were able to obtain results comparable to incremental coupled-cluster calculations with singles, doubles and perturbative triples (CCSD(T)). Repulsive three-centre increments reduce the overall correlation contribution to the binding energy by 20 %.

GRAPHICAL ABSTRACT

Keywords:

• Localised orbitals
• density functional theory
• adsorption
• correlation energy
• dispersion interaction

PACS numbers:

• 31.15.ae
• 31.15.vq
• 34.35.+a

Acknowledgments

The calculations have been carried out in the laboratory of theoretical chemistry in Paris and ZeDat in Berlin. Additional computing resources, furnished by the computing platform jarvis@IP2CT of the research federation IP2CT in Paris, are gratefully acknowledged. Peter Reinhardt expresses his gratitude and warmest regards for numerous outstanding discussions with A. Savin in Paris and elsewhere. For the present project, the advice and practical help of J. Toulouse and B. Mussard in Paris were of great value, as well as discussions with H. Stoll in Stuttgart about recently published work [11]. The stay of Fabian Weber in Paris was possible through a grant of the FU Berlin via the PROMOS program. Carsten Müller acknowledges support by the DFG GRK 1582 “Fluorine as a key element”.

Disclosure statement

No potential conflict of interest was reported by the authors.

Additional information

Funding

FU Berlin, Promos program: Fabian Weber; DFG GRK “Fluorine as a key element”: Carsten Müller.