Triplet Envelope Functions for increasing machine learning interatomic potential efficiency and stability

Abstract

Central to interatomic potential efficiency is the radial envelope function that enables linear scaling with computational cost by defining a local neighborhood of atoms. This has enabled MLIPs to revolutionize materials science over the past decade by providing DFT accuracy with linear scaling computational cost in molecular dynamics workflows. However, MLIPs still have a relatively high computational cost compared to empirical interatomic potentials, preventing them from transforming molecular dynamics workflows. A central issue is that MLIPs use relatively large cutoff radii, converging to 6A over the last few years. The large cutoffs prioritize accuracy of any material over efficiency in any particular region of phase space, capturing dispersion effects and low density materials at the expense of increased computational cost in higher density materials. Past work has aimed to address this with KNN graph sparsification, which, while significantly reducing cost, has the drawback of breaking energy conservation. In this work, we propose higher-order envelope functions that prune local atomic neighborhoods through physically inspired geometric functions to provide the memory and efficiency benefits of KNN graph sparsification while eliminating non-conservative energy dynamics. Through numerical experiments on solids and liquids with 5-8A cutoffs, we show that triplet envelope functions complement radial envelope functions by doubling training and inference speed, tripling memory efficiency, and increasing simulation stability while not impacting accuracy or data efficiency for the most common 6A cutoff. Moreover, experiments with 8A radial cutoffs show triplet envelope functions create a pathway to larger cutoff radii for efficiently and accurately modeling open structures with large interatomic distances, showing a promising new direction for engineering MLIP efficiency.