Accurate Multiscale Simulation of Frictional Interfaces by Quantum Mechanics/Green’s Function Molecular Dynamics

[Image: see text] Understanding frictional phenomena is a fascinating fundamental problem with huge potential impact on energy saving. Such an understanding requires monitoring what happens at the sliding buried interface, which is almost inaccessible by experiments. Simulations represent powerful tools in this context, yet a methodological step forward is needed to fully capture the multiscale nature of the frictional phenomena. Here, we present a multiscale approach based on linked ab initio and Green’s function molecular dynamics, which is above the state-of-the-art techniques used in computational tribology as it allows for a realistic description of both the interfacial chemistry and energy dissipation due to bulk phonons in nonequilibrium conditions. By considering a technologically relevant system composed of two diamond surfaces with different degrees of passivation, we show that the presented method can be used not only for monitoring in real-time tribolochemical phenomena such as the tribologically induced surface graphitization and passivation effects but also for estimating realistic friction coefficients. This opens the way to in silico experiments of tribology to test materials to reduce friction prior to that in real labs.