Microscopic Mechanisms Behind the High Friction and Failure Initiation of Graphene Wrinkles

Wrinkling occurs on the surfaces of large-area graphene ubiquitously. Despite that the wrinkled structures are found to degrade the lubricous property, the behind mechanisms remain less understood. Here, atomic force microscopy is adopted to characterize the friction and wear properties of graphene wrinkles (GWs) with different heights by nanoscratch tests. We verify the phenomena of high friction and reduced load-carrying capacity of wrinkles and report the observation of lubrication deterioration with increased heights. Using molecular dynamics simulations, we reveal that the contact quality at the interface is a dominant role in the friction evolution of wrinkles. The high friction of wrinkles is determined by the increased contact area and commensurability caused by the wrinkle deformation and topography changes. The wrinkle failure initiates near the root of the formed bilayer configuration due to the increased lateral stiffness and reduced atomic distance between the wrinkle layers. The increased interlocking effect results in a local shear stress of 91 GPa and induces the phase transitions of carbon atoms easily. As the wrinkle height decreases, the unstable local configuration weakens the interlocking effects and cannot fail even at a high load. This investigation sheds light on the microscopic frictional contact of GWs and provides guidance for tuning the tribological properties of graphene by controlling the wrinkle structures.