Construction of Machine-Learning Interatomic Potential Under Heat Flux Regularization and Its Application to Power Spectrum Analysis for Silver Chalcogenides

Abstract

We propose a data-driven approach for constructing machine-learning interatomic potentials (MLIPs) trained under a regularization with the aim of avoiding nonphysical heat flux. Specifically, we introduce a regularization term for the heat flux into the cost function of MLIPs to be minimized. Since the treatment of heat flux using MLIPs with regularization can be decomposed into elemental contributions or conducted in frequency space, this approach is expected to be useful for investigating the origin of thermal conductivity obtained from the Green-Kubo formula. However, the strength of regularization needs to be appropriately set because it may reduce not only the nonphysical part but also the intrinsic heat flux one. To this end, we investigated the conditions for constructing MLIPs that can reproduce the power spectra of heat flux associated with the empirical interatomic potential of Ag$_2$Se, which consists of pairwise functions and do not contain a nonphysical heat flux. The appropriate strength could be estimated from the variation of the magnitude of regularization term as well as root mean square errors for total potential energy, atomic force, and virial stress with respect to the strengths, without reference spectrum data. As an application example, we explored the differences in power spectra between superionic and nonsuperionic conducting phases based on the heat flux regularization to MLIPs trained with the first-principles calculation data of Ag$_2$S. Furthermore, our results demonstrate that training with the regularization improves the robustness of MLIPs as well as the reduction of the nonphysical heat flux.