Energy cascades in polaritonic systems with energetic disorder observed by ultrafast two-dimensional white-light spectroscopy

Energy cascades in polaritonic systems with energetic disorder observed by ultrafast two-dimensional white-light spectroscopy | 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 Energy cascades in polaritonic systems with energetic disorder observed by ultrafast two-dimensional white-light spectroscopy Minjung Son, Zachary Armstrong, Ryan Allen, Abitha Dhavamani, and 2 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-1582812/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 27 Nov, 2022 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Abstract Exciton-polaritons are hybrid states formed when molecular excitons are strongly coupled to photons trapped in an optical cavity. These systems have many attractive properties, including large delocalization lengths, but questions regarding the role of energetic disorder remain unanswered. Here, we fabricate microcavities with two different layers of semiconducting carbon nanotubes as a way of controlling the energetic disorder and exploring its impact on energy transfer. Using ultrafast two-dimensional white-light spectroscopy, we observe a delayed growth of a cross peak between the upper- and lower-polariton states. Using Redfield theory, we assign the growth to cascading energy transfer down a manifold of new electronic states created by energetic disorder that is of comparable magnitude to the light-matter coupling. These results broaden our understanding of energy transfer dynamics in exciton-polariton systems beyond the Rabi contraction picture and enable control over how energy is transported in polaritonic systems. Full Text Additional Declarations Yes there is potential Competing Interest. Martin T. Zanni is a co-owner of PhaseTech Spectroscopy, which sells ultrafast pulse shapers and multidimensional spectrometers. Supplementary Files SupplementaryInformation.pdf Cite Share Download PDF Status: Published Journal Publication published 27 Nov, 2022 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-1582812","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":103495243,"identity":"93465649-233f-4437-a2d7-ce5b020c759e","order_by":0,"name":"Minjung Son","email":"","orcid":"https://orcid.org/0000-0002-8385-062X","institution":"University of Wisconsin-Madison","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Minjung","middleName":"","lastName":"Son","suffix":""},{"id":103495244,"identity":"bdac04f7-a152-43b8-83e2-bd5eff46ea77","order_by":1,"name":"Zachary Armstrong","email":"","orcid":"","institution":"University of Wisconsin-Madison","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Zachary","middleName":"","lastName":"Armstrong","suffix":""},{"id":103495245,"identity":"5e9a6e0d-1854-4c64-9e7b-2cfc2311e8bc","order_by":2,"name":"Ryan Allen","email":"","orcid":"","institution":"University of Wisconsin-Madison","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Ryan","middleName":"","lastName":"Allen","suffix":""},{"id":103495246,"identity":"3e98f93a-9fdf-4014-a27a-edaaf070acc5","order_by":3,"name":"Abitha Dhavamani","email":"","orcid":"","institution":"University of Wisconsin-Madison","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Abitha","middleName":"","lastName":"Dhavamani","suffix":""},{"id":103495247,"identity":"517f7038-0bf4-488a-8d54-b3b90aee2452","order_by":4,"name":"Michael Arnold","email":"","orcid":"https://orcid.org/0000-0002-2044-7032","institution":"University of Wisconsin-Madison","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Michael","middleName":"","lastName":"Arnold","suffix":""},{"id":103495248,"identity":"deab3fdd-53cb-4cd1-b0bb-c5d2c07f70bf","order_by":5,"name":"Martin Zanni","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA0ElEQVRIiWNgGAWjYLCChAqGBAgDiSSg5QzJWhjbUJQR0CLffvbYg4fz7PL4xQ6wSTz4Y8fAz55jgN+Cnrx0g8RtycWSsxPYJBLbkhkke97g18LMkGMmkbjtQOKG2wlsNxIbDjAY3CBgCxv/G6CWOQcS94O0JPw5wGBPSAuPBMiWBqAt0iAtbEBbJAhokZAA2pJwLDlxxu3E9h9Av/BInHlWgFeLfH+OmeSPGrvE/tnJhw1//LGT429P3oBXCxJgbAC7lFjlo2AUjIJRMArwAACvakUfYfAu8wAAAABJRU5ErkJggg==","orcid":"https://orcid.org/0000-0001-7191-9768","institution":"University of Wisconsin-Madison","correspondingAuthor":true,"submittingAuthor":false,"prefix":"","firstName":"Martin","middleName":"","lastName":"Zanni","suffix":""}],"badges":[],"createdAt":"2022-04-22 04:30:42","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-1582812/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-1582812/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1038/s41467-022-35046-2","type":"published","date":"2022-11-27T05:00:00+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":29554885,"identity":"6e163049-6ffa-4915-b4da-1068e43b648a","added_by":"auto","created_at":"2022-11-27 08:10:05","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2845653,"visible":true,"origin":"","legend":"","description":"","filename":"MainTextlineno.pdf","url":"https://assets-eu.researchsquare.com/files/rs-1582812/v1_covered.pdf"},{"id":21073840,"identity":"27c1110f-1af7-4067-873c-125961d86698","added_by":"auto","created_at":"2022-05-04 16:15:57","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2833880,"visible":true,"origin":"","legend":"","description":"","filename":"MainTextlineno.pdf","url":"https://assets-eu.researchsquare.com/files/rs-1582812/v1_covered.pdf"},{"id":21073838,"identity":"a90bfc6d-a8eb-4121-8836-ec075e6e1b8a","added_by":"auto","created_at":"2022-05-04 16:15:45","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":11608845,"visible":true,"origin":"","legend":"","description":"","filename":"SupplementaryInformation.pdf","url":"https://assets-eu.researchsquare.com/files/rs-1582812/v1/6c73eada3bd2dfda8866be48.pdf"}],"financialInterests":"\u003cb\u003eYes\u003c/b\u003e there is potential Competing Interest.\nMartin T. Zanni is a co-owner of PhaseTech Spectroscopy, which sells ultrafast pulse shapers and multidimensional spectrometers.","formattedTitle":"Energy cascades in polaritonic systems with energetic disorder observed by ultrafast two-dimensional white-light spectroscopy","fulltext":[{"header":"Full Text","content":"This preprint is available for \u003ca href='/article/rs-1582812/latest.pdf' target='_blank'\u003edownload as a PDF\u003c/a\u003e."}],"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":false,"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-1582812/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-1582812/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"Exciton-polaritons are hybrid states formed when molecular excitons are strongly coupled to photons trapped in an optical cavity. These systems have many attractive properties, including large delocalization lengths, but questions regarding the role of energetic disorder remain unanswered. Here, we fabricate microcavities with two different layers of semiconducting carbon nanotubes as a way of controlling the energetic disorder and exploring its impact on energy transfer. Using ultrafast two-dimensional white-light spectroscopy, we observe a delayed growth of a cross peak between the upper- and lower-polariton states. Using Redfield theory, we assign the growth to cascading energy transfer down a manifold of new electronic states created by energetic disorder that is of comparable magnitude to the light-matter coupling. 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