Graph Atomic Cluster Expansion for Semilocal Interactions beyond Equivariant Message Passing

Abstract

The atomic cluster expansion provides local, complete basis functions that enable efficient parametrization of many-atom interactions. We extend the atomic cluster expansion to incorporate graph basis functions. This naturally leads to representations that enable the efficient description of semilocal interactions in physically and chemically transparent form. Simplification of the graph expansion by tensor decomposition results in an iterative procedure that comprises current message-passing machine learning interatomic potentials. We demonstrate the accuracy and efficiency of the graph atomic cluster expansion for a number of small molecules, clusters, and a general-purpose model for carbon. We further show that the graph atomic cluster expansion scales linearly with the number of neighbors and layer depth of the graph basis functions. Published by the American Physical Society 2024