Development and application of a machine learning potential for diamond surfaces and their sliding interfaces with silicon nitride and silica: effect of passivation, orientation and load

Abstract

Friction and wear of diamond are controlled by its surface chemistry, which determines whether covalent bonds form across the sliding interface. First-principles simulations have explored the role of surface orientation and passivation, but are limited to a few hundred atoms and tens of picoseconds. To bridge this gap, we develop a reactive machine learning interatomic potential for the C/H/N/O/Si chemical space, covering diamond, silicon nitride, silicon oxide, their surfaces, interfaces, and environmental molecules. The potential is trained on a large dataset of diverse structures and is tested on multiple physical properties, including ab initio reaction barriers on diamond surfaces, and structural/mechanical properties of amorphous Si$_3$N$_4$ and SiO$_2$. We then simulate sliding of diamond-Si$_3$N$_4$ interfaces with four surface orientations, clean and H/OH-passivated terminations, and normal loads from 0.1 to 23 GPa. We identify two different regimes: one where sliding is localized at the interface, and shear stress is proportional to the interfacial bond density, and another where shear is distributed inside the softer material, and adhesion due to full interfacial bonding dominates. These results show how passivation, surface orientation and load together determine interfacial bonding and friction, with implications for the environmental sensitivity of diamond wear. More broadly, the potential enables reactive simulations of diamond, silicon nitride and silica with near-ab initio accuracy at length and time scales beyond first-principles methods, providing a useful tool for future studies of wear at plowing asperities, chemical-mechanical polishing, and properties of amorphous ceramic films.