Atomistic Machine Learning with Cartesian Natural Tensors

Abstract: Atomistic ML is a transformative tool for accurate and efficient investigation of material behavior at the atomic scale. While such models have been constructed within Cartesian space to harness geometric information and preserve intuitive physical representations, they face inherent challenges - primarily due to the lack of a systematic symmetry-preserving framework for representing arbitrary physical tensors. We address these challenges by proposing Cartesian Natural Tensor Networks (CarNet) as a general framework for atomistic ML. We first develop the theory of irreducible representations using Cartesian natural tensors (their creation, operation, as well as the decomposition and reconstruction of physical tensors such as the elastic constant tensor). Leveraging this machinery, we design an equivariant Cartesian model and demonstrate its exceptional performance across diverse atomistic ML tasks. CarNet enables the development of highly accurate and reliable interatomic potentials for both materials and molecular systems. Furthermore, structure-property relationships can be readily constructed for tensorial quantities ranging from simple properties like the dipole moment to arbitrary high-rank tensors with complex symmetries such as the elastic constant tensor -- capabilities that were previously inaccessible. This work removes theoretical barriers and unleashes the power of Cartesian approaches for advanced atomistic ML in the understanding and design of new materials.