Accurate Surface and Finite-Temperature Bulk Properties of Lithium Metal at Large Scales Using Machine Learning Interaction Potentials

Abstract

The properties of lithium metal are key parameters in the design of lithium-ion and lithium-metal batteries. They are difficult to probe experimentally due to the high reactivity and low melting point of lithium as well as the microscopic scales at which lithium exists in batteries where it is found to have enhanced strength, with implications for dendrite suppression strategies. Computationally, there is a lack of empirical potentials that are consistently quantitatively accurate across all properties, and ab initio calculations are too costly. In this work, we train a machine learning interaction potential on density functional theory (DFT) data to state-of-the-art accuracy in reproducing experimental and ab initio results across a wide range of simulations at large length and time scales. We accurately predict thermodynamic properties, phonon spectra, temperature dependence of elastic constants, and various surface properties inaccessible using DFT. We establish that there exists a weak Bell-Evans-Polanyi relation correlating the self-adsorption energy and the minimum surface diffusion barrier for high Miller index facets.