A Novel Class of Organic SERS-Active Materials from Bioinspired Supramolecular Frenkel Excitonic Nanoassemblies

A Novel Class of Organic SERS-Active Materials from Bioinspired Supramolecular Frenkel Excitonic Nanoassemblies | 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 Research Article A Novel Class of Organic SERS-Active Materials from Bioinspired Supramolecular Frenkel Excitonic Nanoassemblies Kara Ng, Seda Kelestemur, Hua Deng, William P Carbery, Piyali Maity, and 4 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-9396896/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 While Surface-enhanced Raman Spectroscopy (SERS) is one of the most sensitive techniques for non-destructive analysis for molecular analytes at ultra-low concentrations, the development of SERS-based devices operating in real-life conditions have been restricted by current SERS substrates. Here, we overcome these limitations by providing proof-of- concept for an entirely new class of SERS-active materials: aqueous solution-based supramolecular Frenkel excitonic nanoassemblies. We found inter-molecular photon- induced charge-transfer from a model analyte—Rhodamine 6G (R6G)—adsorbed to cyanine dye based supramolecular nanotubes (b-NTs). Near-field Scanning Optical Microscopy (NSOM), time-resolved fluorescence spectroscopy and SERS revealed that the energy-level alignment between R6G and b-NT’s exciton band led to efficient Herzberg- Teller coupling, resulting in high degree of charge-transfer ( ρ =0.72) and significant plasmon-free SERS enhancement factor (3.0x104). Our results demonstrate how Frenkel excitonic nanoassemblies can serve as breakthrough materials allowing for rational design of efficient, tunable, and flexible substrates for charge-transport and resonant, aqueous solution-based plasmon-free SERS substrates. Raman Spectroscopy Surface-enhanced Raman Spectroscopy Frenkel Excitonic Nanoassemblies J-aggregates Supramolecular assemblies Full Text Additional Declarations The authors declare no competing interests. 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. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. 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-9396896","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":621810530,"identity":"0f212955-2618-40e7-954f-60d902057eef","order_by":0,"name":"Kara Ng","email":"","orcid":"","institution":"Department of Chemistry and Biochemistry, The City College of New York of the City University of New York, New York, USA ; Ph.D. Program in Chemistry, The Graduate Center of the City University of New York, New York, USA","correspondingAuthor":false,"prefix":"","firstName":"Kara","middleName":"","lastName":"Ng","suffix":""},{"id":621810531,"identity":"1ff4fb02-40e2-4b23-a6a3-57a081e67fdf","order_by":1,"name":"Seda Kelestemur","email":"","orcid":"","institution":"Department of Chemistry and Biochemistry, The City College of New York of the City University of New York, New York, USA; Biotechnology Department, Institute of Health Sciences, University of Health Sciences, Istanbul, Turkey","correspondingAuthor":false,"prefix":"","firstName":"Seda","middleName":"","lastName":"Kelestemur","suffix":""},{"id":621810532,"identity":"261000d4-f88d-4acb-a656-a197663aa4a9","order_by":2,"name":"Hua Deng","email":"","orcid":"","institution":"Department of Chemistry and Biochemistry, The City College of New York of the City University of New York, New York, USA ; Ph.D. Program in Chemistry, The Graduate Center of the City University of New York, New York, USA","correspondingAuthor":false,"prefix":"","firstName":"Hua","middleName":"","lastName":"Deng","suffix":""},{"id":621810533,"identity":"2638a235-9979-483e-ab28-7b6c2daaf74d","order_by":3,"name":"William P Carbery","email":"","orcid":"","institution":"Department of Chemistry and Biochemistry, The City College of New York of the City University of New York, New York, USA","correspondingAuthor":false,"prefix":"","firstName":"William","middleName":"P","lastName":"Carbery","suffix":""},{"id":621810534,"identity":"1ebe4613-2786-45dc-b29b-157c3a0a6c88","order_by":4,"name":"Piyali Maity","email":"","orcid":"","institution":"Department of Chemistry and Biochemistry, The City College of New York of the City University of New York, New York, USA","correspondingAuthor":false,"prefix":"","firstName":"Piyali","middleName":"","lastName":"Maity","suffix":""},{"id":621810535,"identity":"8f214134-1653-4019-bbf9-1b67dc6dee44","order_by":5,"name":"Ahamed Jubair","email":"","orcid":"","institution":"Department of Physics, The City College of New York of the City University of New York, New York, USA; Ph.D. Program in Physics, The Graduate Center of the City University of New York, New York, USA","correspondingAuthor":false,"prefix":"","firstName":"Ahamed","middleName":"","lastName":"Jubair","suffix":""},{"id":621810536,"identity":"aa2b513c-f64e-4462-810d-1f3173706b43","order_by":6,"name":"Swapan K. 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Here, we overcome these limitations by providing proof-of- concept for an entirely new class of SERS-active materials: aqueous solution-based supramolecular Frenkel excitonic nanoassemblies. We found inter-molecular photon- induced charge-transfer from a model analyte—Rhodamine 6G (R6G)—adsorbed to cyanine dye based supramolecular nanotubes (b-NTs). Near-field Scanning Optical Microscopy (NSOM), time-resolved fluorescence spectroscopy and SERS revealed that the energy-level alignment between R6G and b-NT’s exciton band led to efficient Herzberg- Teller coupling, resulting in high degree of charge-transfer (\u003c/strong\u003e\u003cem\u003e\u003cstrong\u003eρ\u003c/strong\u003e\u003c/em\u003e\u003cstrong\u003e=0.72) and significant plasmon-free SERS enhancement factor (3.0x104). 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