Graphene on Ni(111): Strong interaction and weak adsorption

Abstract

The adsorption of graphene on Ni(111) has been investigated on the basis of the adiabatic-connection fluctuation-dissipation theorem in the random phase approximation (RPA). Although we find a significant hybridization between the graphene π orbitals and Ni d z 2 states at a binding distance of 2.17Å, the adsorption energy is still in the range of a typical physisorption (67 meV per carbon). An important contribution to the energy is related to a decrease in the exchange energy resulting from the adsorption-induced lower symmetry in the graphene layer. The energetics can be well reproduced using the computationally significantly cheaper van der Waals density functional theory with an appropriately chosen exchange-correlation functional.

Bottom-up approach for the low-cost synthesis of graphene-alumina nanosheet interfaces using bimetallic alloys

“…However, the coexistence of the two phases cannot be excluded. Finally, for the top-fcc structure, the calculated mean distance between the Gr layer and the substrate is 2.12 Å, similar to the Gr-Ni(111) system 20 .…”

The contact of graphene with Ni(111) surface: description by modern dispersive forces approaches

“…This is an indication for the failure of the non self-consistent treatment of graphene/Ni(111) within the RPA, yielding almost isoenergetic physisorbed and chemisorbed states [23,46].…”

“…Hybrid functionals, providing excellent description of the thermochemistry of main group molecules, are unadvised, because of their failure in treating largely delocalized systems, such as transition metals and graphene [22]. Calculations within the Random Phase Approximation (RPA) were suggested as a good choice [23] to model graphene-metal systems. However, on the one hand, these are computationally too expensive for many practical systems, and, on the other hand, RPA yields physisorbed and chemisorbed situations with similar adsorption energy, for which there is no experimental evidence, i.e.…”

Testing the Jacob's ladder of density functionals for electronic structure and magnetism of rutileVO2

“…In contrast, DFT+U and hybrid or fourth-rung functionals (PBE0 and HSE06) have already been applied to various strongly-correlated transition metal oxides [25,26]. Due to its extremely high computational cost, the RPA has only been applied to realistic systems very recently [27][28][29][30][31][32][33][34][35]. VO 2 is considered as a model system for studying the phase transition involving electron-electron correlation.…”