The influence of nanoscale roughness and substrate chemistry on the frictional properties of single and few layer graphene.

Nanoscale carbon lubricants such as graphene, have garnered increased interest as protective surface coatings for devices, but its tribological properties have been shown to depend on its interactions with the underlying substrate surface and its degree of surface conformity. This conformity is especially of interest as real interfaces exhibit roughness on the order of ∼10 nm that can dramatically impact the contact area between the graphene film and the substrate. To examine the combined effects of surface interaction strength and roughness on the frictional properties of graphene, a combination of Atomic Force Microscopy (AFM) and Raman microspectroscopy has been used to explore substrate interactions and the frictional properties of single and few-layer graphene as a coating on silica nanoparticle films, which yield surfaces that mimic the nanoscaled asperities found in realistic devices. The interactions between the graphene and the substrate have been controlled by comparing their binding to hydrophilic (silanol terminated) and hydrophobic (octadecyltrichlorosilane modified) silica surfaces. AFM measurements revealed that graphene only partially conforms to the rough surfaces, with decreasing conformity, as the number of layers increase. Under higher mechanical loading the graphene conformity could be reversibly increased, allowing for a local estimation of the out-of-plane bending modulus of the film. The frictional properties were also found to depend on the number of layers, with the largest friction observed on single layers, ultimately decreasing to that of bulk graphite. This trend however, was found to disappear, depending on the tip-sample contact area and interfacial shear strain of the graphene associated with its adhesion to the substrate.