Structure and Dynamics of the Magnetite(001)/Water Interface from Molecular Dynamics Simulations Based on a Neural Network Potential.

Abstract

The magnetite/water interface is commonly found in nature and plays a crucial role in various technological applications. However, our understanding of its structural and dynamical properties at the molecular scale remains still limited. In this study, we developed an efficient Behler-Parrinello neural network potential (NNP) for the magnetite/water system, paying particular attention to the accurate generation of reference data with density functional theory. Using this NNP, we performed extensive molecular dynamics simulations of the magnetite (001) surface across a wide range of water coverages, from single molecules to bulk water. Our simulations revealed several new ground states of low coverage water on the Subsurface Cation Vacancy (SCV) model and yielded a density profile of water at the surface that exhibits marked layering. By calculating mean square displacements, we obtained quantitative information on the diffusion of water molecules on the SCV for different coverages, revealing significant anisotropy. Additionally, our simulations provided qualitative insights into the dissociation mechanisms of water molecules at the surface.