Anisotropic Interlayer Force Field for Heterogeneous Interfaces of Graphene and h-BN with Transition Metal Dichalcogenides

An anisotropic interlayer potential (ILP), designed to describe the interlayer interaction in graphene/MX2 and h-BN/MX2 (M = Mo, W; X = S, Se) heterostructures, is presented. The ILP is parametrized against density functional theory (DFT) calculations within the Perdew–Burke–Ernzerhof (PBE) generalized-gradient approximation, augmented by nonlocal many-body dispersive (MBD-NL) interactions. The parametrized force field demonstrates excellent agreement with the DFT reference data of binding energy curves and sliding energy surfaces across all heterostructures considered. The transferability of the developed ILP is demonstrated for the phenalenyl (C13H9)/MoS2 and B7N6H9/MoS2 interfaces, which are outside the training set. The force field is then used to study equilibrium interlayer distances, bulk moduli, and phonon spectra by means of molecular dynamics simulations.