Unraveling the Interfacial Properties of Twisted Single‐Crystal Au(111)/MoS₂ Heterostructures: A Pathway to Robust Superlubricity

Abstract A comprehensive study of monolayer MoS₂ on a single‐crystal Au(111) surface is reported, combining ultra‐high vacuum scanning probe microscopy with advanced computational methods. Kelvin probe force microscopy precisely quantified the work function of the heterointerface, while topographic analysis by contact and non‐contact atomic force microscopy revealed a moiré superlattice with an interfacial twist angle of 0.45° between MoS₂ and Au(111). To accurately model and predict the twist angle and out‐of‐plane corrugation of these moiré superlattices, a semi‐anisotropic interlayer force field based on density functional theory is developed. This avoids the limitations of conventional pairwise potentials, and our results show excellent agreement with experiments. Furthermore, friction simulations revealed a non‐monotonic dependence on the interfacial twist angle, with small angles exhibiting unexpectedly large shear stress, suggesting that MoS₂ could serve as an effective superlubric coating for gold. This work establishes a robust framework for the investigation of van der Waals heterostructures, bridging nanoscale experimental observations with first‐principles calculations, and providing insights for the design of novel nanoscale devices with tailored electronic, mechanical, and tribological properties.