Universal Hamiltonian learning with rotational and basis equivariance
arXiv:2401.17015
Abstract
Deep learning has the potential to transform computational materials research by making electronic-structure calculations more efficient and scalable. The Hamiltonian matrix in the localized atomic-orbital basis is a promising target for deep-learning electronic structure, yet enforcing rotational equivariance can be computationally costly, and the matrix depends on the choice of basis set. Here we introduce DeepH-2, a physics-guided neural-network framework that reduces the computational cost of enforcing rotational equivariance through a local-coordinate formulation and incorporates basis equivariance by mapping a shared latent Hamiltonian to the target atomic-orbital basis. DeepH-2 achieves sub-meV test-set error on a diverse materials dataset and demonstrates transferability across material dimensions. These results highlight the value of encoding physics priors into deep-learning electronic structure models, and pave the way for developing the electronic-structure foundation models.