Realizing room-temperature strong coupling of single-exciton with plasmons by controlling quantum exceptional point

Realizing room-temperature strong coupling of single-exciton with plasmons by controlling quantum exceptional point | 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 Realizing room-temperature strong coupling of single-exciton with plasmons by controlling quantum exceptional point Wei Li, Renming Liu, Junyu Li, Jie Zhong, Huanjun Chen, Xue-Hua Wang This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-228136/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 Single-exciton strong coupling with plasmons is highly desirable for exploiting room-temperature quantum devices and applications. However, the large plasmon decay makes the realization of such strong coupling extremely difficult. To overcome this challenge, here we propose an effective approach to easily achieve the single-exciton strong coupling at room temperature by controlling quantum exceptional point (QEP) of the coupling system via matching the decay between the localized plasmon mode (LPM) and exciton. The good match can be reached by suppressing the LPM’s decay with the use of a leaky Fabry-Perot cavity. Experimental results show that the LPM’s decay linewidth is greatly compressed from ~ 45 nm to ~ 15 nm, which is close to the excitonic linewidth (~ 10 nm), pushing their interaction from the Fano interference into the strong coupling. Our work opens a new way to flexibly control the QEP and more easily realize the single-exciton strong coupling in ambient conditions. Photonics/optics single-exciton plasmon room-temperature quantum exceptional point strong coupling Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Full Text Due to technical limitations, full-text HTML conversion of this manuscript could not be completed. However, the latest manuscript can be downloaded and accessed as a PDF. Additional Declarations There is NO Competing Interest. Supplementary Files SupplementaryMaterials.doc Supplementary Materials 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-228136","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":13867262,"identity":"fc0d294c-7113-4006-a1ef-6cc5b2684d82","order_by":0,"name":"Wei Li","email":"","orcid":"","institution":"State Key Laboratory of Optoelectronic Materials and Technologies, School of Physics, Sun Yat-sen University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Wei","middleName":"","lastName":"Li","suffix":""},{"id":13867263,"identity":"7c63b653-48bb-444e-b9d0-ca2603857bf4","order_by":1,"name":"Renming Liu","email":"","orcid":"","institution":"School of Physics and Electronics, Henan University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Renming","middleName":"","lastName":"Liu","suffix":""},{"id":13867264,"identity":"d521cea7-d8e3-451d-9035-656b1cefcef4","order_by":2,"name":"Junyu Li","email":"","orcid":"","institution":"State Key Laboratory of Optoelectronic Materials and Technologies, School of Physics, Sun Yat-sen University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Junyu","middleName":"","lastName":"Li","suffix":""},{"id":13867265,"identity":"7e0c67ee-2b77-4651-a018-de8cbc8c2bfa","order_by":3,"name":"Jie Zhong","email":"","orcid":"","institution":"State Key Laboratory of Optoelectronic Materials and Technologies, School of Physics, Sun Yat-sen University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Jie","middleName":"","lastName":"Zhong","suffix":""},{"id":13867266,"identity":"59408422-dfe5-4bef-9b49-9897f84942e3","order_by":4,"name":"Huanjun Chen","email":"","orcid":"https://orcid.org/0000-0003-4699-009X","institution":"Guangdong Province Key Laboratory of Display Material and Technology, Sun Yat-sen University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Huanjun","middleName":"","lastName":"Chen","suffix":""},{"id":13867267,"identity":"b6a0e73c-a92c-46be-b98f-4647ee13df15","order_by":5,"name":"Xue-Hua Wang","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAABC0lEQVRIiWNgGAWjYBCDBH4gceABjMtDjBbJBqCWBJK0GBwAkcRoMTh+9vBr3jabPONrhx8CbalLnD8jgfHB2zYGeXNcWs7kpVnObEsrNrudZgDUcjhxw40EZsO5bQyGOxuwazE7kGNm8LHtcOK22wkgLQcSN0gksEnztkGdik3L+TdmBolt/xM3z07/AHMY+2+8Wm7kGD/42AY0XDoHZAtzYsONBDZmfFrsb7wxY5xxLjlxxu2cggMJBoeNN5x52Cw555yE4QYcWiT7c4w/85TZJfbPTt/84UNFnez89uSDH96U2cjjsgUI2CQQbAMGxwYGxgYgSwKXchBg/oDiUnxKR8EoGAWjYGQCAPQrZfkyxNzaAAAAAElFTkSuQmCC","orcid":"https://orcid.org/0000-0003-1324-1471","institution":"State Key Laboratory of Optoelectronic Materials and Technologies, School of Physics, Sun Yat-sen University","correspondingAuthor":true,"submittingAuthor":false,"prefix":"","firstName":"Xue-Hua","middleName":"","lastName":"Wang","suffix":""}],"badges":[],"createdAt":"2021-02-10 01:01:03","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-228136/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-228136/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":6487071,"identity":"6afc5c4c-a0b0-4024-9b9d-5ad225074300","added_by":"auto","created_at":"2021-03-01 21:36:26","extension":"jpg","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":617848,"visible":true,"origin":"","legend":"LPM-exciton couplings in single Au@Ag NR/J-aggregate hybrids on ITO substrate. a Normalized scattering of a bare Au@Ag NR resonant to the exciton absorption (dashed green curve) with εc 2.11 meV. b Normalized scattering spectra of a strongly coupled Au@Ag NR/J-aggregate hybrid at resonance condition. The dotted black line is the theoretical result calculated using Eq. (3) with N = 1. c Normalized scattering spectra of the individual Au@Ag NR/J-aggregate hybrids isolated from the ensembles treated with 1.0-μΜdye solution, and ordered according to the detuning. d Extinction spectra calculated using Eq. (3) with N = 1 for the same samples as in (c). e, f Quantum step statistics of the effective coupling strength (√Ng) extracted (using the method proposed in ref. 37.) from the measured individual hybrids isolated from the ensembles treated with (e) 1.0-μΜ and (f) 3.0-μΜ dye solution, respectively. The insets in (a), (b) are SEM images of the measured nanostructures, and the scale bar is 50 nm.","description":"","filename":"Fig.1.jpg","url":"https://assets-eu.researchsquare.com/files/rs-228136/v1/8985f76ead2f0deed9ed1077.jpg"},{"id":6487900,"identity":"e28c50e5-c03f-4803-82a6-87f929266984","added_by":"auto","created_at":"2021-03-01 21:45:26","extension":"jpg","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":467298,"visible":true,"origin":"","legend":"Synergistic nanoantenna-microcavity hybrid for plasmonic decay suppression and local EF enhancement. a Schematic diagram of the synergistic Au NR/FP-cavity hybrid system. b Normalized scattering calculated for the Au NRs with different aspect ratios localized on the surface of the leaky FP cavity. The solid and dashed color curve represents the normalized scattering of the Au NRs on the FP cavity and on the bulk Si3N4 substrate, respectively. The dashed gray curve is the reflectivity of the bare FP cavity. Here, the length l and radius r of the Au NR are 45.2, 54.0, 61.8 and 12 nm, respectively; c Simulated total EF through the middle of the bare FP cavity. d Simulated x-component of the total EF, Ex, through the middle of the Au NR (l =54 nm) on the bulk Si3N4 substrate (i) and the FP cavity (ii), respectively. e Average near-field intensity 〈ΙEΙ2〉on the surface of the Au NR (l = 54 nm) as functions of wavelength for the NR located on the bulk Si3N4 substrate and the FP cavity, respectively. In simulations, tSi3N4 = 200 nm, tSiO2 = 4035 nm, silica is the substrate.","description":"","filename":"Fig.2.jpg","url":"https://assets-eu.researchsquare.com/files/rs-228136/v1/517de35489b244f0ec0bb1da.jpg"},{"id":6487369,"identity":"d1fa3157-b556-4060-a085-9e590bf7fad9","added_by":"auto","created_at":"2021-03-01 21:39:26","extension":"jpg","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":697976,"visible":true,"origin":"","legend":"Scattering measurements of the bare Au@Ag NRs in the EM environments engineered by the leaky FP cavity. a Schematic diagram of dark-field scattering measurement for a single cuboid Au@Ag NR on a leaky FP cavity. b Simulated (solid cyan curve) and measured (dashed grey line) reflectance for the leaky FP cavity with tSi3N4 = 216.9 nm and tSiO2 = 3008 nm. The silicon is set as a semi-infinite substrate. c, d Normalized scattering (solid color curves) for Au@Ag NRs located on (c) the FP cavity (with tSi3N4 = 216.9 nm and tSiO2 =3008 nm) and (d) the ITO-coated glass substrate, respectively. Dashed color curves are corresponding theoretical results calculated using the structural parameters extracted from the measurements. The dashed gray curves represent the experimental reflectance of bare FP cavity. The inserts are corresponding SEM images for the measured cuboid Au@Ag NRs, the scale bar is 50 nm. e Statistics of decay linewidths for (i) the ELPMs for the NRs on the FP cavity and (ii) bare LPMs for the NRs on the ITO substrate, note that the statistical wavelength range is TM1’ ± 8, TM2’ ± 8 and TM3’ ± 8 nm, respectively.","description":"","filename":"Fig.3.jpg","url":"https://assets-eu.researchsquare.com/files/rs-228136/v1/c8fbda6ab44237e5bf57e1f3.jpg"},{"id":6487371,"identity":"c712a100-2ddc-42ec-bf32-f5abea33c318","added_by":"auto","created_at":"2021-03-01 21:39:26","extension":"jpg","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":1195694,"visible":true,"origin":"","legend":"Single-exciton strong coupling in single-exciton-coupled NRs located on the leaky FP cavity. a A strongly coupled Au @ Ag NR/J-aggregate hybrid, measured on FP cavity (Si/SiO2/Si3N4). b Extinction spectra of J-aggregate (dashed green curve) solution and Scattering spectra (orange solid curve) of bare Au @ Ag NR with the size of 62×34 nm located on FP cavity. c, d Real (solid curve) and imaginary (dashed curve) parts of the eigenenergies in Eq. (1) as a function of g at resonance δ = 0 with (c) γd = 159 meV, γc = 36 meV; and (d) γd = 54 meV, γc = 36 meV. WC: Weak coupling; SC: Strong coupling. e Normalized scattering of the individual Au@Ag NR/J-aggregate hybrids isolated from the sample treated 1.0-μΜ dye solution, and ordered according to detuning. The dashed white lines are theoretical results calculated using Eq. (3) with N = 1, γd ~55 meV (Supplementary Fig. 8b), γc ~36 meV and g ~28.8 meV. f Quantum steps for the effective coupling coefficient, √Ng, observed as one, two and three-exciton coupling cases for the hybrid NRs isolated from the sample treated with the 1.0-μΜ dye solution. The scale bar in the insets of (a) and (b) is 50 nm.","description":"","filename":"Fig.4.jpg","url":"https://assets-eu.researchsquare.com/files/rs-228136/v1/1e9f8ca71d05f893c93716e6.jpg"},{"id":6487739,"identity":"e2fa4ebb-2773-46ad-b489-884884086cc8","added_by":"auto","created_at":"2021-03-01 21:42:26","extension":"jpg","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":219359,"visible":true,"origin":"","legend":"Influence of controlling gQEP on coherence properties in plasmon-exciton coupling systems. a Plasmonic and exciton fractions for the UPB and LPB of the single-exciton-coupled NRs located on the FP cavity (solid color curves) and the ITO substrate (dashed color curves), In the calculations, the parameters are the same as what have been used in Figs. 1d and 4e. b Cooperativities of the individual single-exciton-coupled NRs located on the FP cavity (red stars) and the ITO substrate (green triangles), which are calculated from the experimental data in Fig. 1c and Fig. 4e, respectively.","description":"","filename":"Fig.5.jpg","url":"https://assets-eu.researchsquare.com/files/rs-228136/v1/4f6556042663c9fad6231130.jpg"},{"id":13598427,"identity":"a57ce6ac-7f26-4806-b28e-4d458960a312","added_by":"auto","created_at":"2021-09-17 05:35:35","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":3320887,"visible":true,"origin":"","legend":"","description":"","filename":"Realizingroomtemperaturestrongcouplingofsingleexcitonwithplasmonsbycontrollingquantumexceptionalpoint.pdf","url":"https://assets-eu.researchsquare.com/files/rs-228136/v1_covered.pdf"},{"id":6488179,"identity":"2039b200-442f-4035-937c-ebca4beb53c1","added_by":"auto","created_at":"2021-03-01 21:48:30","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":3681044,"visible":true,"origin":"","legend":"","description":"","filename":"Realizingroomtemperaturestrongcouplingofsingleexcitonwithplasmonsbycontrollingquantumexceptionalpoint.pdf","url":"https://assets-eu.researchsquare.com/files/rs-228136/v1_stamped.pdf"},{"id":6487373,"identity":"c7bf03a4-023a-4a0d-bf7d-6d5111124517","added_by":"auto","created_at":"2021-03-01 21:39:26","extension":"doc","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":12312576,"visible":true,"origin":"","legend":"Supplementary Materials","description":"","filename":"SupplementaryMaterials.doc","url":"https://assets-eu.researchsquare.com/files/rs-228136/v1/ce74f65186ca5c936995ae26.doc"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Realizing room-temperature strong coupling of single-exciton with plasmons by controlling quantum exceptional point","fulltext":[{"header":"Full Text","content":"Due to technical limitations, full-text HTML conversion of this manuscript could not be completed. However, the latest manuscript can be downloaded and \u003ca href='/article/rs-228136/latest.pdf' target='_blank'\u003e accessed as a PDF.\u003c/a\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":false,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":true,"highlight":"","institution":"","isAcceptedByJournal":false,"isAuthorSuppliedPdf":true,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true},"keywords":"single-exciton, plasmon, room-temperature, quantum exceptional point, strong coupling","lastPublishedDoi":"10.21203/rs.3.rs-228136/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-228136/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"Single-exciton strong coupling with plasmons is highly desirable for exploiting room-temperature quantum devices and applications. However, the large plasmon decay makes the realization of such strong coupling extremely difficult. To overcome this challenge, here we propose an effective approach to easily achieve the single-exciton strong coupling at room temperature by controlling quantum exceptional point (QEP) of the coupling system via matching the decay between the localized plasmon mode (LPM) and exciton. The good match can be reached by suppressing the LPM’s decay with the use of a leaky Fabry-Perot cavity. Experimental results show that the LPM’s decay linewidth is greatly compressed from ~ 45 nm to ~ 15 nm, which is close to the excitonic linewidth (~ 10 nm), pushing their interaction from the Fano interference into the strong coupling. Our work opens a new way to flexibly control the QEP and more easily realize the single-exciton strong coupling in ambient conditions.","manuscriptTitle":"Realizing room-temperature strong coupling of single-exciton with plasmons by controlling quantum exceptional point","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2021-03-01 21:36:24","doi":"10.21203/rs.3.rs-228136/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"81fcc405-6219-404d-bed9-df6cb7b251c2","owner":[],"postedDate":"March 1st, 2021","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[{"id":2699024,"name":"Photonics/optics"}],"tags":[],"updatedAt":"2021-12-21T10:55:58+00:00","versionOfRecord":[],"versionCreatedAt":"2021-03-01 21:36:24","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-228136","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-228136","identity":"rs-228136","version":["v1"]},"buildId":"cBFmMYwuxLRRLfASyISRj","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}