Machine learning electronic structure and atomistic properties from the external potential
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arXiv
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| Format: | Preprint |
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2026
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| author | Nigam, Jigyasa Smidt, Tess Dusson, Geneviève |
| author_facet | Nigam, Jigyasa Smidt, Tess Dusson, Geneviève |
| contents | Electronic structure calculations remain a major bottleneck in atomistic simulations and, not surprisingly, have attracted significant attention in machine learning (ML). Most existing approaches learn a direct map from molecular geometries, typically represented as graphs or encoded local environments, to molecular properties or use ML as a surrogate for electronic structure theory by targeting quantities such as Fock or density matrices expressed in an atomic orbital (AO) basis.
Inspired by the Hohenberg-Kohn theorem, in this work, we propose an operator-centered framework in which the external (nuclear) potential, expressed in an AO basis, serves as the model input. From this operator, we construct hierarchical, body-ordered representations of atomic configurations that closely mirror the principles underlying several popular atom-centered descriptors. At the same time, the matrix-valued nature of the external potential provides a natural connection to equivariant message-passing neural networks. In particular, we show that successive products of the external potential provide a scalable route to equivariant message passing and enable an efficient description of long-range effects. We demonstrate that this approach can be used to model molecular properties, such as energies and dipole moments, from the external potential, or learn effective operator-to-operator maps, including mappings to the Fock matrix and the reduced density matrix from which multiple molecular observables can be simultaneously derived. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2602_15345 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Machine learning electronic structure and atomistic properties from the external potential Nigam, Jigyasa Smidt, Tess Dusson, Geneviève Chemical Physics Computational Physics Electronic structure calculations remain a major bottleneck in atomistic simulations and, not surprisingly, have attracted significant attention in machine learning (ML). Most existing approaches learn a direct map from molecular geometries, typically represented as graphs or encoded local environments, to molecular properties or use ML as a surrogate for electronic structure theory by targeting quantities such as Fock or density matrices expressed in an atomic orbital (AO) basis. Inspired by the Hohenberg-Kohn theorem, in this work, we propose an operator-centered framework in which the external (nuclear) potential, expressed in an AO basis, serves as the model input. From this operator, we construct hierarchical, body-ordered representations of atomic configurations that closely mirror the principles underlying several popular atom-centered descriptors. At the same time, the matrix-valued nature of the external potential provides a natural connection to equivariant message-passing neural networks. In particular, we show that successive products of the external potential provide a scalable route to equivariant message passing and enable an efficient description of long-range effects. We demonstrate that this approach can be used to model molecular properties, such as energies and dipole moments, from the external potential, or learn effective operator-to-operator maps, including mappings to the Fock matrix and the reduced density matrix from which multiple molecular observables can be simultaneously derived. |
| title | Machine learning electronic structure and atomistic properties from the external potential |
| topic | Chemical Physics Computational Physics |
| url | https://arxiv.org/abs/2602.15345 |