Monte Carlo simulation of borosilicate glass dissolution using molecular dynamics-generated glass structures

Abstract Atomic-scale insights into borosilicate glass dissolution are critical to the development of waste form corrosion models. While Monte Carlo (MC) simulations have been instrumental in advancing the state of knowledge, all simulations to date have relied on lattices to represent the glass structure, potentially introducing artifacts. A new approach (amorphous MC approach) was developed whereby glass structures generated from molecular dynamics simulations were used as starting points for MC simulations. Correlations between dissolution rate and structural features were revealed in MC simulations of sodium borosilicate glasses that covered a wide compositional range. Notably, the lattice MC approach predicted the fraction of tetrahedral boron to have a lesser influence on the dissolution rate than computed with the amorphous MC approach. The lattice MC simulations also overestimated the dissolution rate for a given glass composition. These findings highlight the importance of using truly amorphous structures in MC simulations of glass corrosion.