Quantitative prediction of rate constants and its application to organic emitters

Quantitative prediction of rate constants and its application to organic emitters | 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 Physical Sciences - Article Quantitative prediction of rate constants and its application to organic emitters Hironori Kaji, Katsuyuki Shizu This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-3387334/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 03 Jun, 2024 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Abstract Many phenomena in nature consist of multiple elementary processes. If we can predict all the rate constants of each process quantitatively, we can comprehensively predict and understand various phenomena in nature. Here, we report that it is possible to quantitatively predict all related rate constants and quantum yields without conducting experiments, using multiple-resonance thermally activated delayed fluorescence (MR–TADF) as an example. MR–TADF is desirable for practical application in organic light-emitting diodes (OLEDs) because of their narrow emission spectra, high luminescence efficiency, and chemical stability. However, MR–TADF emitters have one drawback: slow reverse intersystem crossing (RISC), leading to efficiency roll-off and reduced device lifetime. We first showed a quantum chemical calculation method for quantitatively reproducing all experimentally obtained rate constants and quantum yields for previously synthesized MR–TADF emitters. Next, this method was applied to presently unsynthesised molecules. This study reveals a strategy to improve RISC without compromising other important factors: rate constant of radiative decay, photoluminescence quantum yields, and emission linewidth. Our method is robust and can be applied in a wide range of research fields—not only for quantitative prediction of rate constants and quantum yields but also for a comprehensive understanding of the mechanism including the time evolution of excitons. Physical sciences/Materials science/Materials for devices Physical sciences/Chemistry/Materials chemistry Full Text Additional Declarations There is NO Competing Interest. Supplementary Files 20230826NatureSI.pdf Supplementary Information Cite Share Download PDF Status: Published Journal Publication published 03 Jun, 2024 Read the published version in Nature Communications → 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-3387334","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Physical Sciences - Article","associatedPublications":[],"authors":[{"id":237852916,"identity":"0a257d7b-a0ef-4569-a009-cb7de47b65a1","order_by":0,"name":"Hironori Kaji","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA9klEQVRIie3RsWoCMRzH8Z8Uzg5/yZpg6zNEhGKh+CyRAyc7udx407lYuvoa3RxzBDoF+goRwanDdXM4aHNiHVpMOwrmuyQEPvyTOyAWO8M4oHQF3IB+HAdJuYQHDdH/JLiiXySUmOu1eahHntj+psowztvG4X51mnRJKfNYpITOYiC19YQmEsKeJj00JNcERne8LD7HOaZ+eBEgzCkzrI/ET2HvYdLlfgoS3VzsQPgfU8TSqfLJvyWh15m0FoOCb6UOvYW/TdNqV496jNIXl2W4fWbpeiMCX8z/EbVfElzLwwYwIg+Rtv7euONZ6yNIYrFY7ML6AhKCTCxJA1KMAAAAAElFTkSuQmCC","orcid":"https://orcid.org/0000-0002-5111-3852","institution":"Kyoto University","correspondingAuthor":true,"submittingAuthor":false,"prefix":"","firstName":"Hironori","middleName":"","lastName":"Kaji","suffix":""},{"id":237852917,"identity":"982d985d-65a5-4efd-87a8-f545cc21a702","order_by":1,"name":"Katsuyuki Shizu","email":"","orcid":"","institution":"Kyoto University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Katsuyuki","middleName":"","lastName":"Shizu","suffix":""}],"badges":[],"createdAt":"2023-09-26 06:40:20","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-3387334/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-3387334/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1038/s41467-024-49069-4","type":"published","date":"2024-06-03T04:00:00+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":57709835,"identity":"efb910e4-2f34-4ea8-8bb4-9a1d47236994","added_by":"auto","created_at":"2024-06-04 15:40:56","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":982255,"visible":true,"origin":"","legend":"","description":"","filename":"20230926Naturemaintext.pdf","url":"https://assets-eu.researchsquare.com/files/rs-3387334/v1_covered_2e97960e-3964-4c1f-a46b-aba41b83ec19.pdf"},{"id":45065298,"identity":"c3a848b5-fd0a-4788-8229-131b3bf13762","added_by":"auto","created_at":"2023-10-23 06:44:28","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":2540579,"visible":true,"origin":"","legend":"Supplementary Information","description":"","filename":"20230826NatureSI.pdf","url":"https://assets-eu.researchsquare.com/files/rs-3387334/v1/df7558f50bad1d42f2af3c43.pdf"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Quantitative prediction of rate constants and its application to organic emitters","fulltext":[],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":false,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":true,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":true,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"nature-portfolio","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"","title":"Nature Portfolio","twitterHandle":"","acdcEnabled":false,"dfaEnabled":false,"editorialSystem":"ejp","reportingPortfolio":"","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"","lastPublishedDoi":"10.21203/rs.3.rs-3387334/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-3387334/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eMany phenomena in nature consist of multiple elementary processes. 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