Theoretical and Computational Chemistry

On the role of long-range electrostatics in machine-learned interatomic potentials for complex battery materials



Modeling complex energy materials such as solid-state electrolytes (SSEs) realistically at the atomistic level strains the capabilities of state-of-the-art theoretical approaches. On one hand, the system sizes and simulation time scales required are prohibitive for first-principles methods like density functional theory (DFT). On the other hand, parameterizations for empirical potentials are often not available and these potentials may ultimately lack the desired predictive accuracy. Fortunately, modern machine learning (ML) potentials are increasingly able to bridge this gap, promising first-principles accuracy at a much reduced computational cost. However, the local nature of these ML potentials typically means that long-range contributions arising, e.g., from electrostatic interactions are neglected. Clearly, such interactions can be large in polar materials like electrolytes, however. Herein, we investigate the effect that the locality assumption of ML potentials has on lithium mobility and defect formation energies in the SSE Li$_7$P$_3$S$_{11}$. We find that neglecting long-range electrostatics is unproblematic for the description of lithium transport in the isotropic bulk. In contrast (field-dependent) defect formation energies are only adequately captured by a hybrid potential combining ML and a physical model of electrostatic interactions. Broader implications for ML based modelling of energy materials are discussed.


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