{
  "abstract": "Hybrid interfaces formed by push-pull organic molecules physisorbed on two-dimensional (2D) semiconductors provide a structurally tunable platform for engineering second-harmonic generation (SHG). However, predicting and optimizing their macroscopic response remains a formidable challenge due to the phase-sensitive interference between the nonlinear responses of the adlayer and substrate. Here, we develop a physics-informed computational screening framework that decomposes the effective second-order susceptibility into its constituent substrate, molecular, and electric-field-induced SHG channels. Validated by fully atomistic first-principles calculations across representative interface structures, this model maps the complete orientation-resolved tensor landscape of chemically modulated carbon-conjugated polar molecules on 2D substrates with distinct symmetry. Crucially, our findings dismantle the conventional reliance on static polar descriptors, demonstrating that the ground-state permanent dipole magnitude is a fundamentally unreliable proxy for macroscopic nonlinear response. Instead, we show that the ultimate criterion for SHG maximization is encoded in the phase-resolved projection of the full anisotropic molecular hyperpolarizability tensor. On non-centrosymmetric substrates, the coherent interference between the physisorbed adlayer and the underlying 2D matrix induces a characteristic Fano-like asymmetry and ranking reversals that are entirely absent on centrosymmetric platforms. By establishing that functionalization topology, dynamic spatial orientation, and substrate point-group symmetry constitute a single, non-separable parameter space, this work provides a systematic blueprint for the rational assembly, predictive discovery, and non-invasive characterization of next-generation low-dimensional hybrid materials for nonlinear optoelectronics.",
  "abstract_shown": true,
  "affiliations": [],
  "article_type": null,
  "arxiv": "2609.29255",
  "author_total": 3,
  "authors": [
    {
      "name": "Michele Guerrini"
    },
    {
      "name": "Muhammad Sufyan Ramzan"
    },
    {
      "name": "Caterina Cocchi"
    }
  ],
  "bibtex": "https://research.draconitic.com/paper/6tbye9bd1r4ry.bib",
  "cited_by": 0,
  "doi": "10.48550/arxiv.2609.29255",
  "fulltext_url": null,
  "id": "6tbye9bd1r4ry",
  "issns": [],
  "landing_url": "https://arxiv.org/abs/2609.29255",
  "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",
      "2504|Nonlinear Optical Materials Research"
    ]
  ],
  "openalex": "W7214337791",
  "pdf_url": "https://arxiv.org/pdf/2609.29255",
  "pmcid": null,
  "pmid": null,
  "published": "2026-09-24",
  "publisher": null,
  "ris": "https://research.draconitic.com/paper/6tbye9bd1r4ry.ris",
  "sources": [
    {
      "first_seen": "2026-10-30T12:24:11Z",
      "native_id": "2609.29255",
      "source": "arxiv",
      "url": "https://arxiv.org/abs/2609.29255"
    }
  ],
  "subjects": [
    {
      "field": "physics",
      "origin": "arxiv:cond-mat.mtrl-sci",
      "subfield": "condensed-matter"
    }
  ],
  "title": "Rational Design of Low-Dimensional Hybrid Organic/Inorganic Interfaces for Enhanced Second-Harmonic Generation",
  "title_text": "Rational Design of Low-Dimensional Hybrid Organic/Inorganic Interfaces for Enhanced Second-Harmonic Generation",
  "type": "preprint",
  "updated_at": "2026-10-30T12:24:11Z",
  "url": "https://research.draconitic.com/paper/6tbye9bd1r4ry",
  "venue": "arXiv",
  "versions": []
}