UniHam: A Large-Scale SOC-Complete Dataset and Benchmark for Hamiltonian Learning in Materials
Yuewen Huang, Pin Chen, Yutong Lu
原文摘要
Accurate prediction of electronic Hamiltonians would enable broad property inference while avoiding the high computational cost of Density Functional Theory (DFT). However, progress toward general-purpose materials foundation models is limited by a data bottleneck: existing Hamiltonian datasets are typically small, lack structural diversity, and often omit essential relativistic physics such as spin--orbit coupling (SOC). We therefore construct UniHam, a large-scale Hamiltonian dataset and benchmark suite comprising 100,000+ DFT-computed complex-valued Hermitian Hamiltonians with full SOC, covering 72 elements and a wide range of crystal geometries and symmetries (spanning diverse lattice types and space-group families). Building on UniHam, we benchmark two representative state-of-the-art models under a standardized protocol and introduce complementary evaluation metrics that jointly assess three dimensions: (i) Hamiltonian reconstruction accuracy, (ii) out-of-distribution (OOD) generalization across composition/symmetry shifts, and (iii) the ability to support downstream property prediction from the predicted Hamiltonians. Experiments on UniHam demonstrate that the proposed benchmark and metrics effectively differentiate model capabilities, revealing intrinsic SOC- and element-dependent failure modes, large variations in compositional OOD robustness, and the necessity of spectral-level evaluation to assess whether Hamiltonian predictions reliably support downstream electronic-structure properties. Overall, UniHam provides a reproducible, SOC-complete benchmark that can sharpen model comparisons and accelerate the development of next-generation foundation models for quantum materials.
cs.LG · cond-mat.mtrl-sci