{
  "abstract": "Interlayer interactions in two-dimensional materials can generate emergent phenomena absent in their constituent monolayers, including unconventional magnetic order, multiferroicity, and topological magnetic phases. Predicting such emergent behavior requires simultaneously resolving long-range dispersion, short-range orbital hybridization, and electronic correlation interactions that are intrinsically nonlocal and many-body and remain challenging even for advanced density-functional approximations. Here we establish a systematically controlled many-body benchmark for diverse bilayer materials using diffusion Monte Carlo (DMC), spanning single-sheet materials, transition-metal dichalcogenides, and magnetic transition-metal halides. We obtain equilibrium separations, binding energetics, interlayer vibrational modes, and charge redistribution, finding excellent agreement with available experiments while revealing systematic and property-dependent failures across widely used semilocal, meta-GGA, and dispersion-corrected density functionals. Beyond energetics, DMC resolves subtle interlayer charge rearrangements, particularly leading to long-ranged dipolar tails in magnetic Cr trihalides that survive well beyond the regime where semilocal DFT predicts appreciable interlayer polarization, providing a many-body basis for understanding interlayer-coupled ferroic and magnetic phenomena. The resulting energies, response properties, and high-accuracy electron densities constitute a transferable benchmark for developing next-generation density functionals. Finally, we provide a scalable high-performance-computing workflow that enables systematic expansion of many-body benchmark datasets across emerging families of layered quantum materials by the scientific community.",
  "abstract_shown": true,
  "affiliations": [],
  "article_type": null,
  "arxiv": "2609.05845",
  "author_total": 6,
  "authors": [
    {
      "name": "Kayahan Saritas"
    },
    {
      "name": "Hyeonedok Shin"
    },
    {
      "name": "Jaron T. Krogel"
    },
    {
      "name": "Anouar Benali"
    },
    {
      "name": "P. Ganesh"
    },
    {
      "name": "Paul R. C. Kent"
    }
  ],
  "bibtex": "https://research.draconitic.com/paper/0r1eexzm6x057.bib",
  "cited_by": 0,
  "doi": "10.48550/arxiv.2609.05845",
  "fulltext_url": null,
  "id": "0r1eexzm6x057",
  "issns": [],
  "landing_url": "https://arxiv.org/abs/2609.05845",
  "language": null,
  "licence": "CC-BY-4.0",
  "licence_label": "CC BY 4.0",
  "licence_source": "article",
  "licence_url": "http://creativecommons.org/licenses/by/4.0/",
  "metadata_licence": "CC0-1.0",
  "native_subjects": [
    [
      "arxiv",
      "cond-mat.mtrl-sci"
    ],
    [
      "openalex",
      "3107|Advanced Chemical Physics Studies"
    ]
  ],
  "openalex": "W7212017445",
  "pdf_url": "https://arxiv.org/pdf/2609.05845",
  "pmcid": null,
  "pmid": null,
  "published": "2026-09-05",
  "publisher": null,
  "ris": "https://research.draconitic.com/paper/0r1eexzm6x057.ris",
  "sources": [
    {
      "first_seen": "2026-10-30T12:19:48Z",
      "native_id": "2609.05845",
      "source": "arxiv",
      "url": "https://arxiv.org/abs/2609.05845"
    }
  ],
  "subjects": [
    {
      "field": "physics",
      "origin": "arxiv:cond-mat.mtrl-sci",
      "subfield": "condensed-matter"
    }
  ],
  "title": "Diffusion Quantum Monte Carlo Benchmark of Interlayer Binding and Charge Redistribution in Chemically Distinct Two-Dimensional Van Der Waals Bilayers",
  "title_text": "Diffusion Quantum Monte Carlo Benchmark of Interlayer Binding and Charge Redistribution in Chemically Distinct Two-Dimensional Van Der Waals Bilayers",
  "type": "preprint",
  "updated_at": "2026-10-30T12:19:48Z",
  "url": "https://research.draconitic.com/paper/0r1eexzm6x057",
  "venue": "arXiv",
  "versions": []
}