Spectral/Spatial Tensor Atomic Cluster Expansion with Universal Embeddings in Cartesian Space

Abstract

Equivariant atomistic machine learning models have largely been built on spherical-tensor representations, where explicit angular-momentum coupling introduces substantial complexity and systematic extensions beyond energies and forces remain challenging, often requires problem-specific architectural choices. Here we introduce the Tensor Atomic Cluster Expansion (TACE), which unifies scalar and tensorial modeling in Cartesian and space by decomposing local environments into irreducible Cartesian tensors (ICT) constructing a controlled many-body hierarchy with atomic cluster expansion (ACE). In addition to performing ACE in the frequency domain, we propose an efficient Clebsch-Gordan-free alternative in the spatial domain. TACE provides universal invariant (e.g., fidelity tags and charges) and equivariant (e.g., external electric fields and non-collinear magnetic moments) embeddings and predicted tensorial observables are handled on equal footing and enabling explicit control at inference. We demonstrate the accuracy, stability, and efficiency across finite molecules and extended materials, including in-domain and out-of-domain benchmarks, spectra, Hessian, external-field responses, charged systems, and multi-fidelity/head training. We further show its robustness on nonequilibrium/reactive datasets and controlled scaling when extending to large foundation model datasets.