{
  "abstract": "In this work, we use spin-polarized density functional theory (DFT) to identify substantial third-order, nonadditive configurational energy contributions in lithium-rich oxyfluorides that quadratic unconstrained binary optimization (QUBO) models cannot represent. We test the extension from QUBO to higher-order unconstrained binary optimization (HUBO) in two disordered-rocksalt cathode materials, Li$_2$MnO$_2$F (LMOF) and Li$_2$Mn$_{0.5}$Ti$_{0.5}$O$_2$F (LMTiOF), using composition-preserving DFT energy maps. Using fixed-geometry energy maps, we show that cubic HUBO captures nonadditive contributions absent from QUBO models and substantially reduces fitting errors in both materials. Direct DFT energy differences confirm third-order nonadditivity, while comparisons of magnetic initializations reveal a strong dependence of the LMTiOF contribution on the converged electronic state. These results support the inclusion of higher-order terms when modeling configurational energetics and highlight the need to account for magnetic-state dependence in constructing DFT energy maps. The extracted terms describe effective couplings among composition-preserving exchange variables, rather than uniquely identified microscopic three-atom interactions.",
  "abstract_shown": true,
  "affiliations": [],
  "article_type": null,
  "arxiv": "2610.38321",
  "author_total": 1,
  "authors": [
    {
      "name": "Joonho Bae"
    }
  ],
  "bibtex": "https://research.draconitic.com/paper/3rcrk9j7mk6g5.bib",
  "cited_by": 0,
  "doi": "10.48550/arxiv.2610.38321",
  "fulltext_url": null,
  "id": "3rcrk9j7mk6g5",
  "issns": [],
  "landing_url": "https://arxiv.org/abs/2610.38321",
  "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"
    ]
  ],
  "openalex": null,
  "pdf_url": "https://arxiv.org/pdf/2610.38321",
  "pmcid": null,
  "pmid": null,
  "published": "2026-10-28",
  "publisher": null,
  "ris": "https://research.draconitic.com/paper/3rcrk9j7mk6g5.ris",
  "sources": [
    {
      "first_seen": "2026-10-30T12:36:23Z",
      "native_id": "2610.38321",
      "source": "arxiv",
      "url": "https://arxiv.org/abs/2610.38321"
    }
  ],
  "subjects": [
    {
      "field": "physics",
      "origin": "arxiv:cond-mat.mtrl-sci",
      "subfield": "condensed-matter"
    }
  ],
  "title": "First-Principles Identification of Higher-Order Configurational Energy Terms and Their Magnetic-State Dependence in Lithium-Rich Oxyfluorides: From QUBO to HUBO",
  "title_text": "First-Principles Identification of Higher-Order Configurational Energy Terms and Their Magnetic-State Dependence in Lithium-Rich Oxyfluorides: From QUBO to HUBO",
  "type": "preprint",
  "updated_at": "2026-11-01T12:20:44Z",
  "url": "https://research.draconitic.com/paper/3rcrk9j7mk6g5",
  "venue": "arXiv",
  "versions": []
}