Cartesian atomic cluster expansion for machine learning interatomic potentials (2402.07472v3)

Abstract: Machine learning interatomic potentials are revolutionizing large-scale, accurate atomistic modelling in material science and chemistry. Many potentials use atomic cluster expansion or equivariant message passing frameworks. Such frameworks typically use spherical harmonics as angular basis functions, and then use Clebsch-Gordan contraction to maintain rotational symmetry, which may introduce redundancies in representations and computational overhead. We propose an alternative: a Cartesian-coordinates-based atomic density expansion. This approach provides a complete set of polynormially indepedent features of atomic environments while maintaining interaction body orders. Additionally, we integrate low-dimensional embeddings of various chemical elements and inter-atomic message passing. The resulting potential, named Cartesian Atomic Cluster Expansion (CACE), exhibits good accuracy, stability, and generalizability. We validate its performance in diverse systems, including bulk water, small molecules, and 25-element high-entropy alloys.