Edge-Pinning Effect of Graphene Nanoflakes Sliding Atop Graphene

Abstract

Edge effect is one of the detrimental factors preventing superlubricity in laminar solid lubricants. Separating the friction contribution from the edge atom and inner atom is of paramount importance for rational design of ultralow friction across scales in van der Waals heterostructures. To decouple these contributions and provide the underlying microscopic origin at the atomistic level, we considered two contrast models, namely, graphene nanoflakes with dimerized and pristine edges sliding on graphene monolayer based on extensive ab initio calculations. We found the edge contribution to friction is lattice orientation dependence. In particular, edge pinning effect by dimerization is obvious for misaligned contact but suppressed in aligned lattice orientation. The former case providing local commensuration along edges is reminiscent of     Aubry’s pinned phase and the contribution of per edge carbon atom to the sliding potential energy corrugation is even 1.5 times more than that of an atom in bilayer graphene under commensurate contact. Furthermore, we demonstrated that the dimerized edges as high frictional pinning sites are robust to strain engineering and even enhanced by fluorination. Both structural and chemical modification in the tribological system constructed here offers the atomic physics details to dissect the undesirable edge pinning effect in layered materials which would give rise to the marked discrepancies in measured friction parameters from the same superlubric sample or different samples with the same size and identical preparation.

Keywords: Edge-pinning effect, Structural lubricity, Dimerized edge, Aubry's pinned phase, Misaligned contact