A Gaussian process coarse-grained potential for Na-montmorillonite

Abstract

Hydraulic transport in compacted bentonite is diffusion-controlled and governed by the hydration and microstructure of sodium montmorillonite (Na-MMT). Experiments cannot resolve how platelet interactions govern pore structure, transport and stiffness, while existing coarse-grained models smooth hydration oscillations or require manual corrections. We develop a tabulated potential combining Morse interactions between platelet centre and edge sites with a Gaussian process regression correction trained on all-atom potentials of mean force. It captures the hydration-induced complexity of the potential-of-mean-force profiles, including the three-water (3-W) hydration minimum and transfers across geometries, layer-charge variants and unseen configurations. Applied to monodisperse and polydisperse Na-MMT assemblies at dry densities of 0.8-1.3 g cm^-3, the model captures the 3-W to 1-W transition, loss of non-interlayer porosity and evolution of pore structure, random-walk tortuosity, diffusion and stiffness. Predicted diffusion agrees with compacted Na-bentonite measurements.