Atomic-scale defects restricting structural superlubricity: Ab initio study on the example of the twisted graphene bilayer

Abstract

The potential energy surface (PES) of interlayer interaction of twisted bilayer graphene with vacancies in one of the layers is investigated via density functional theory (DFT) calculations with van der Waals corrections. These calculations give a non-negligible magnitude of PES corrugation of 28 meV per vacancy and barriers for relative sliding of the layers of 7 - 8 meV per vacancy for the moir\'e pattern with coprime indices (2,1) (twist angle 21.8$^\circ$). At the same time, using the semiempirical potential fitted to the DFT results, we confirm that twisted bilayer graphene without defects exhibits superlubricity for the same moir\'e pattern and the magnitude of PES corrugation for the infinite bilayer is below the calculation accuracy. Our results imply that atomic-scale defects restrict the superlubricity of 2D layers and can determine static and dynamic tribological properties of these layers in a superlubric state. We also analyze computationally cheap approaches that can be used for modeling of tribological behavior of large-scale systems with defects. The adequacy of using state-of-the-art semiempirical potentials for interlayer interaction and approximations based on the first spatial Fourier harmonics for the description of interaction between graphene layers with defects is discussed.