{
  "abstract": "Machine-learned interatomic potentials have greatly expanded the reach of molecular dynamics simulations, but complex chemical environments often require explicit treatment of long-range electronic response, including charge transfer and polarization. Physics-based flexible-charge models capture these effects but require global nonlinear charge equilibration at every time step to obtain Born-Oppenheimer energies and forces. This process is computationally expensive and can lead to instabilities unless tightly converged. Here, we introduce a shadow molecular dynamics framework for flexible-charge models with arbitrary local nonlinearities and long-range multipolar electrostatics. We replace the exact Born-Oppenheimer potential with a nearby shadow potential obtained by exactly equilibrating a partially linearized electronic energy functional. This provides conservative forces and reduces the global nonlinear equilibration to a quasi-diagonal linear problem that can be solved directly at low cost. Auxiliary dynamical electronic degrees of freedom, propagated through an extended-Lagrangian dynamics, capture the long-range electronic response and define the reference state for the linearization of the energy functional. GPU-accelerated simulations with over 100,000 atoms demonstrate that the shadow potential closely follows the tightly converged Born-Oppenheimer surface, while maintaining long-term stability at a computational cost approaching that of a fixed-charge model. These advances establish an efficient and broadly applicable framework for machine-learned interatomic potentials that explicitly incorporate long-range electrostatic interactions and environment-dependent electronic response.",
  "abstract_shown": true,
  "affiliations": [],
  "article_type": null,
  "arxiv": "2611.03499",
  "author_total": 13,
  "authors": [
    {
      "name": "Jos Thomas"
    },
    {
      "name": "Anthony P. Baldo"
    },
    {
      "name": "Rae A. Corrigan Grove"
    },
    {
      "name": "Mehmet Cagri Kaymak"
    },
    {
      "name": "Joshua Finkelstein"
    },
    {
      "name": "James Goff"
    },
    {
      "name": "Maksim Kulichenko"
    },
    {
      "name": "Sergei Tretiak"
    },
    {
      "name": "Nicholas Lubbers"
    },
    {
      "name": "Vishikh Athavale"
    },
    {
      "name": "Christian F. A. Negre"
    },
    {
      "name": "Michael Wall"
    },
    {
      "name": "Anders M. N. Niklasson"
    }
  ],
  "bibtex": "https://research.draconitic.com/paper/3s3mkgbdgf152.bib",
  "cited_by": 0,
  "doi": "10.48550/arxiv.2611.03499",
  "fulltext_url": null,
  "id": "3s3mkgbdgf152",
  "issns": [],
  "landing_url": "https://arxiv.org/abs/2611.03499",
  "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",
      "physics.chem-ph"
    ]
  ],
  "openalex": null,
  "pdf_url": "https://arxiv.org/pdf/2611.03499",
  "pmcid": null,
  "pmid": null,
  "published": "2026-11-02",
  "publisher": null,
  "ris": "https://research.draconitic.com/paper/3s3mkgbdgf152.ris",
  "sources": [
    {
      "first_seen": "2026-11-03T12:21:04Z",
      "native_id": "2611.03499",
      "source": "arxiv",
      "url": "https://arxiv.org/abs/2611.03499"
    }
  ],
  "subjects": [
    {
      "field": "chemistry",
      "origin": "arxiv:physics.chem-ph",
      "subfield": "physical"
    }
  ],
  "title": "Shadow Molecular Dynamics for General Nonlinear Flexible-Charge Models",
  "title_text": "Shadow Molecular Dynamics for General Nonlinear Flexible-Charge Models",
  "type": "preprint",
  "updated_at": "2026-11-03T12:21:04Z",
  "url": "https://research.draconitic.com/paper/3s3mkgbdgf152",
  "venue": "arXiv",
  "versions": []
}