Development of potentials for molecular dynamics simulations of dry and hydrated calcium aluminosilicate glasses by force matching and refinement

Abstract

Potential development and refinement to improve the applicability and transferability of the forcefield is important to atomistic simulations of glass materials and their interactions with the environment. In this paper, we demonstrate potential development of calcium aluminosilicate glasses with and without water using a reactive potential framework by adopting the force matching technique and subsequent refinement. Accordingly, we have reproduced the forces on atoms of the system from a DFT based ab-initio molecular dynamics (AIMD) simulations by adjusting the potential parameters. We chose the diffuse charge reactive potential (DCRP) as the classical potential as it has been previously demonstrated to accurately and efficiently simulate interactions between water and silicate-glasses. The obtained force matched parameters were further refined to accurately reproduce the structures and dynamics of dry and hydrated calcium alumino silicate glass and gel structures. The Ca2+ behavior in solution was correctly reproduced with an average local coordination equal to 6.12 and a diffusion coefficient close to the experimental values. This force field also correctly reproduces the local environment of Al3+ in glass, but it falls short in describing Al3+ ion coordination in solutions as compared to AIMD results, suggesting a direction of future improvement. This set of potential can thus be used for simulations of calcium aluminosilicate glasses with various technological applications and hydrated gel structures resulted from corrosions of boroaluminosilicate glasses.