Combining Molecular Dynamics and Machine Learning to Analyze Shear Thinning for Alkane and Globular Lubricants in the Low Shear Regime.

Lubricants with desirable frictional properties are important in achieving an energy-saving society. Lubricants at the interfaces of mechanical components are confined under high shear rates and pressures and behave quite differently from the bulk material. Computational approaches such as nonequilibrium molecular dynamics (NEMD) simulations have been performed to probe the molecular behavior of lubricants. However, the low-shear-velocity regions of the materials have rarely been simulated owing to the expensive calculations necessary to do so, and the molecular dynamics under shear velocities comparable with that in the experiments are not clearly understood. In this study, we performed NEMD simulations of extremely confined lubricants, i.e., two molecular layers for four types of lubricants confined in mica walls, under shear velocities from 0.001 to 1 m/s. While we confirmed shear thinning, the velocity profiles could not show the flow behavior when the shear velocity was much slower than thermal fluctuations. Therefore, we used an unsupervised machine learning approach to detect molecular movements that contribute to shear thinning. First, we extracted the simple features of molecular movements from large amounts of MD data, which were found to correlate with the effective viscosity. Subsequently, the extracted features were interpreted by examining the trajectories contributing to these features. The magnitude of diffusion corresponded to the viscosity, and the location of slips that varied depending on the spherical and chain lubricants was irrelevant. Finally, we attempted to apply a modified Stokes-Einstein relation at equilibrium to the nonequilibrium and confined systems. While systems with low shear rates obeyed the relation sufficiently, large deviations were observed under large shear rates.