Atomistic Mechanisms of Sliding in Few-Layer and Bulk Doped MoS₂

Sliding of two-dimensional materials is critical for their application as solid lubricants for space, and also relevant for strain engineering and device fabrication. Dopants such as Ni surprisingly improve lubrication in MoS$_2$, despite formation of interlayer bonds by intercalated Ni, and the mechanism has remained unclear. While sliding on the atomistic level has been theoretically investigated in pristine 2D materials, there has been little work on doped forms, especially for the complicated case of intercalation. We use density functional theory to study sliding of Ni-doped MoS$_2$, considering Mo/S substitution and octahedral/tetrahedral intercalation. We find that bulk and trilayers are well described by pairwise bilayer interactions. Tetrahedral intercalation between layers dramatically increases their sliding barrier, but minimally affects sliding between adjacent undoped layers, thus preserving effective lubrication. We provide an atomistic view of how sliding occurs in doped transition-metal dichalcogenides, and a general methodology to analyze doped sliding.