Retrosynthetic topological synthesis of two-dimensional inorganic crystals with record solar-blind nonlinear optical performance

Retrosynthetic topological synthesis of two-dimensional inorganic crystals with record solar-blind nonlinear optical performance | 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 Retrosynthetic topological synthesis of two-dimensional inorganic crystals with record solar-blind nonlinear optical performance Kang Min Ok, Wei Zeng, Yao Tian, Yalan Deng, Ying Long, Huixian Chen, and 5 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-9296902/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 The rational synthesis of high-performance inorganic two-dimensional (2D) nonlinear optical (NLO) crystals remains challenging because wide bandgaps, large birefringence, and strong second-harmonic generation (SHG) responses are difficult to optimize simultaneously. Here, we introduce retrosynthetic crystal topological chemistry (RCTC) as a predictive, topology-driven strategy for designing advanced 2D optical materials. Guided by this approach, five new inorganic layered crystals were synthesized as designed. Among them, (NH4)As2O3Br exhibits outstanding optical performance arising from densely packed and highly ordered [As2O3]∞ layers composed of [AsO3] units, delivering a large birefringence of 0.24 at 546 nm and, to the best of our knowledge, the strongest SHG response reported for solar-blind ultraviolet NLO materials (23.3 × KDP at 1064 nm). Theoretical calculations reveal that this exceptional performance originates from the high density and cooperative alignment of stereochemically active lone-pair-rich anionic groups, establishing RCTC as a versatile framework for designing next-generation 2D functional photonic materials. Physical sciences/Chemistry/Inorganic chemistry/Solid-state chemistry Physical sciences/Optics and photonics/Optical materials and structures/Photonic crystals Full Text Additional Declarations There is NO Competing Interest. Supplementary Files RCTCSI.docx Supplementary Information CombinedCIFs.cif CIF 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. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. 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