Great efforts have been made to further reduce friction of atomically thin two-dimensional (2D) materials as solid lubricants due to their exceptional tribological properties and mechanical strength. In this work, the friction of atomically thin graphene is extensively and controllably reduced through pre-rubbing under high stress, resulting in a reduction of the friction coefficient by up to a factor of six compared to the pristine graphene. Also, this reduction can be reversed by reciprocating friction under moderate stress. Furthermore, high-stress pre-rubbing allows for patterning intentionally lubricating features on atomically thin graphene, such as nanometer-sized letters. This reduction in friction is attributed to the decreased sliding potential barrier yet increased contact stiffness, induced by the enhanced strength of graphene adhesion to the substrate due to interfacial charge transfer, as revealed by density functional theory (DFT) calculations. These findings present a practical methodology for optimizing and controlling the performance of 2D materials.
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