Physical Chemistry

DFT Accurate Interatomic Potential for Molten NaCl from Machine Learning

Abstract

Molten alkali chloride salts are a critical component in concentrated solar power and nuclear applications. Despite their ubiquity, the extreme chemical reactivity of molten alkali chlorides at high temperatures has presented a significant challenge in characterizing atomic structures and dynamic properties experimentally. Here we investigate

molten NaCl by performing high temperature molecular dynamics simulations using a Gaussian Approximation Potential (GAP) trained on Density Functional Theory (DFT) datasets. Our GAP model, trained with a meager 1000 atomic configurations, arrives at near DFT accuracy with a mean absolute error of 1.5 meV/atom, thus enabling fast analysis of high temperature salt properties on large length (5000 ion pairs) and time (> 1ns) scales, currently inaccessible to ab initio simulations. Calculated structure factors and diffusion constants from our GAP model simulations show excellent agreement with experiments. Our results indicate that GAP models are able to capture the many-body interactions required to accurately model ionic-systems.

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