Interfacial dipolar interactions drive giant second-harmonic generation in 2D organic–inorganic heterostructures

Interfacial dipolar interactions drive giant second-harmonic generation in 2D organic–inorganic heterostructures | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Interfacial dipolar interactions drive giant second-harmonic generation in 2D organic–inorganic heterostructures Jun Yi, Ye-Tao Chen, Shi-Yi Yuan, Xiu-Bin Liu, Xiu-Qi Shi, Xi Xu, and 7 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8303381/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted You are reading this latest preprint version Abstract Interfacial coupling governs the emergent functionality of two-dimensional (2D) organic–inorganic heterostructures, underpinning advances in linear optoelectronics such as photovoltaics. However, extending this control to the nonlinear optical regime remains elusive, as it requires driving the coherent nonlinear polarization of the inorganic lattice using molecular states, which is distinct from the incoherent charge transfer exploited in linear devices. Here we report a giant second-harmonic generation (SHG) response driven purely by long-range interfacial dipolar interactions in an α-perylene organic crystal (α-Pe)/WS2 heterostructure. We show that the specific crystalline anisotropy of the organic layer creates a polarization-tunable antenna, where anisotropic dipole–dipole coupling efficiently channels excitation energy into the WS2 layer to drive the nonlinear process. This mechanism yields a spatially uniform, giant effective second-order susceptibility χ eff (2) approaching ~20 nm V -1 in monolayers and, notably, induces interfacial symmetry breaking to activate robust SHG in nominally centrosymmetric bilayer WS2. Our results establish organic–inorganic interfacial coupling as a generalizable lever for engineering nonlinear optical responses; given the vast abundance of molecular crystals with distinct dipolar symmetries, this strategy offers a scalable route to compact, chemically designable on-chip nonlinear photonic systems. Physical sciences/Optics and photonics/Other photonics Physical sciences/Materials science/Materials for optics/Nonlinear optics Full Text Additional Declarations There is NO Competing Interest. Supplementary Files Supplementary20251208f.docx Supplementary Materials Cite Share Download PDF Status: Under Review Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-8303381","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":556686780,"identity":"f3fb9c5c-04ed-4df1-a6f3-cf680553c0a4","order_by":0,"name":"Jun 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