Multidimensional Bidirectional Functional Ordering Strategy for Deep-Ultraviolet Nonlinear Optical Crystals

Multidimensional Bidirectional Functional Ordering Strategy for Deep-Ultraviolet Nonlinear Optical Crystals | 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 Multidimensional Bidirectional Functional Ordering Strategy for Deep-Ultraviolet Nonlinear Optical Crystals Shilie Pan, Meng Cheng, Linlin Liu, Abudukadi Tudi, Chenxu Li, and 2 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8612296/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract Spatial ordering of functional units is a central yet poorly controllable factor in the chemical design of deep-ultraviolet (deep-UV) nonlinear optical (NLO) crystals, where wide bandgaps often compromise structural anisotropy. Here we introduce a bidirectional functional ordering strategy that couples zero-dimensional π-conjugated cations with two-dimensional fluorooxoborate layers, allowing weak directional interactions to actively regulate layer topology and stacking coherence. In crystal [C(NH)]BOF (GBOF), the guanidinium cations simultaneously adapt and reshape the [BOF] layer. Crystal exhibits deep-UV transparency (6.66 eV), enhanced birefringence (0.133 @ 1064 nm), and phase matching wavelength to 196 nm. Systematic modulation of interlayer stacking further reveals functional ordering as an independent chemical variable, enabling continuous tuning of optical properties across a GBOF-i (i=1-30) family of low-energy structures. This work establishes sequence-controlled functional ordering as a general design principle for deep-UV NLO crystals. Physical sciences/Chemistry/Materials chemistry/Optical materials Physical sciences/Chemistry/Chemical synthesis/Solid-phase synthesis Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupportingInformation.docx Multidimensional Bidirectional Functional Ordering Strategy for Deep-Ultraviolet Nonlinear Optical Crystals Cite Share Download PDF Status: Posted 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. 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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-8612296","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":577985519,"identity":"8436b3e7-2261-4fa0-be61-c4ef21d9d98b","order_by":0,"name":"Shilie 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Here we introduce a bidirectional functional ordering strategy that couples zero-dimensional π-conjugated cations with two-dimensional fluorooxoborate layers, allowing weak directional interactions to actively regulate layer topology and stacking coherence. In crystal [C(NH\u003c2\u003c/sub\u003esub\u003e)\u003c3\u003c/sub\u003esub\u003e]B\u003c6\u003c/sub\u003esub\u003eO\u003c9\u003c/sub\u003esub\u003eF (GBOF), the guanidinium cations simultaneously adapt and reshape the [B\u003c6\u003c/sub\u003esub\u003eO\u003c9\u003c/sub\u003esub\u003eF] layer. Crystal exhibits deep-UV transparency (6.66 eV), enhanced birefringence (0.133 @ 1064 nm), and phase matching wavelength to 196 nm. Systematic modulation of interlayer stacking further reveals functional ordering as an independent chemical variable, enabling continuous tuning of optical properties across a GBOF-i (i=1-30) family of low-energy structures. 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