{
  "abstract": "Coupled-cluster theory defines the accuracy standard for molecular electronic-structure properties but scales too steeply for routine application, whereas density-functional theory is affordable yet systematically biased. We resolve this trade-off with a single equivariant network, HARP (Hamiltonian Read-out for Properties), that predicts an effective one-electron Hamiltonian from one inexpensive B3LYP/def2-SVP calculation and derives a broad suite of properties from it (energy, optical gap, dipole, quadrupole, polarizability, Mulliken atomic charges, and Mayer bond orders) at coupled-cluster accuracy across nine main-group elements, including the under-served phosphorus, sulfur, and chlorine chemistries. The model is trained on a new in-house dataset of multi-property labels computed at the CCSD(T) level for all nine elements. On a held-out test set, it reduces the error of every property by a factor of 3.8 to 270 relative to semi-local, hybrid, and double-hybrid DFT (referenced to composite CCSD(T)/cc-pVTZ), while adding only ~0.1 s wall time per molecule, delivering coupled-cluster-quality predictions at the cost of a single DFT calculation. Critically, deriving every property from a predicted Hamiltonian rather than pooling per-atom features builds the correct size-scaling into the model architecture: on pi-conjugated oligothiophenes it matches finite-field CCSD polarizability to ~1% and the EOM-CCSD optical gap to ~3% at the largest sizes where those references remain affordable (44 and 37 atoms, where a single CCSD field point already costs ~500x the model's entire inference) and extrapolates the corrected trends to 58-atom chains, a regime where pooling-based architectures fail by construction. Accurate extrapolation is therefore set by the model's inductive bias rather than by the training data.",
  "abstract_shown": true,
  "affiliations": [],
  "article_type": null,
  "arxiv": "2608.18346",
  "author_total": 13,
  "authors": [
    {
      "name": "Wenhao He"
    },
    {
      "name": "Xu Chen"
    },
    {
      "name": "Noah Song"
    },
    {
      "name": "Haowei Xu"
    },
    {
      "name": "Tim S. Hindges"
    },
    {
      "name": "Bohan Li"
    },
    {
      "name": "Zihan Lin"
    },
    {
      "name": "Yu Yao"
    },
    {
      "name": "Avetik R. Harutyunyan"
    },
    {
      "name": "Fang Liu"
    },
    {
      "name": "Yao Wang"
    },
    {
      "name": "Hao Tang"
    },
    {
      "name": "Ju Li"
    }
  ],
  "bibtex": "https://research.draconitic.com/paper/584tbrvqwqajs.bib",
  "cited_by": 0,
  "doi": "10.48550/arxiv.2608.18346",
  "fulltext_url": null,
  "id": "584tbrvqwqajs",
  "issns": [],
  "landing_url": "https://arxiv.org/abs/2608.18346",
  "language": null,
  "licence": "LicenseRef-arXiv-nonexclusive-1.0",
  "licence_label": "arXiv licence",
  "licence_source": "article",
  "licence_url": "http://arxiv.org/licenses/nonexclusive-distrib/1.0/",
  "metadata_licence": "CC0-1.0",
  "native_subjects": [
    [
      "arxiv",
      "cond-mat.mtrl-sci"
    ],
    [
      "arxiv",
      "cs.AI"
    ],
    [
      "arxiv",
      "cs.LG"
    ],
    [
      "arxiv",
      "physics.chem-ph"
    ],
    [
      "arxiv",
      "physics.comp-ph"
    ],
    [
      "openalex",
      "3107|Advanced Chemical Physics Studies"
    ]
  ],
  "openalex": "W7203936690",
  "pdf_url": "https://arxiv.org/pdf/2608.18346",
  "pmcid": null,
  "pmid": null,
  "published": "2026-10-01",
  "publisher": null,
  "ris": "https://research.draconitic.com/paper/584tbrvqwqajs.ris",
  "sources": [
    {
      "first_seen": "2026-10-30T12:26:03Z",
      "native_id": "2608.18346",
      "source": "arxiv",
      "url": "https://arxiv.org/abs/2608.18346"
    }
  ],
  "subjects": [
    {
      "field": "chemistry",
      "origin": "arxiv:physics.chem-ph",
      "subfield": "physical"
    },
    {
      "field": "physics",
      "origin": "arxiv:physics.comp-ph",
      "subfield": "computational"
    },
    {
      "field": "physics",
      "origin": "arxiv:cond-mat.mtrl-sci",
      "subfield": "condensed-matter"
    }
  ],
  "title": "Coupled-cluster molecular properties across the main group that extrapolate beyond training size",
  "title_text": "Coupled-cluster molecular properties across the main group that extrapolate beyond training size",
  "type": "preprint",
  "updated_at": "2026-10-30T12:26:03Z",
  "url": "https://research.draconitic.com/paper/584tbrvqwqajs",
  "venue": "arXiv",
  "versions": []
}