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Spontaneous exciton dissociation enables spin state interconversion in delayed fluorescence organic semiconductors

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datacite.issupplementedby.urlhttps://doi.org/10.17863/CAM.76085
dc.contributor.authorGillett, Alexander J.
dc.contributor.authorTonnelé, Claire
dc.contributor.authorLondi, Giacomo
dc.contributor.authorRicci, Gaetano
dc.contributor.authorCatherin, Manon
dc.contributor.authorUnson, Darcy M. L.
dc.contributor.authorCasanova, David
dc.contributor.authorCastet, Frédéric
dc.contributor.authorOlivier, Yoann
dc.contributor.authorChen, Weimin M.
dc.contributor.authorZaborova, Elena
dc.contributor.authorEvans, Emrys W.
dc.contributor.authorDrummond, Bluebell H.
dc.contributor.authorConaghan, Patrick J.
dc.contributor.authorCui, Lin-Song
dc.contributor.authorGreenham, Neil C.
dc.contributor.authorPuttisong, Yuttapoom
dc.contributor.authorFages, Frédéric
dc.contributor.authorBeljonne, David
dc.contributor.authorFriend, Richard H.
dc.contributor.orcidGillett, Alexander J. [0000-0001-7572-7333]
dc.contributor.orcidTonnelé, Claire [0000-0003-0791-8239]
dc.contributor.orcidLondi, Giacomo [0000-0001-7777-9161]
dc.contributor.orcidCasanova, David [0000-0002-8893-7089]
dc.contributor.orcidCastet, Frédéric [0000-0002-6622-2402]
dc.contributor.orcidChen, Weimin M. [0000-0002-6405-9509]
dc.contributor.orcidEvans, Emrys W. [0000-0002-9092-3938]
dc.contributor.orcidDrummond, Bluebell H. [0000-0001-5940-8631]
dc.contributor.orcidGreenham, Neil C. [0000-0002-2155-2432]
dc.contributor.orcidPuttisong, Yuttapoom [0000-0002-9690-6231]
dc.contributor.orcidFages, Frédéric [0000-0003-2013-0710]
dc.contributor.orcidBeljonne, David [0000-0001-5082-9990]
dc.contributor.orcidFriend, Richard H. [0000-0001-6565-6308]
dc.date.accessioned2021-11-22T14:43:05Z
dc.date.available2021-11-22T14:43:05Z
dc.date.issued2021-11-17
dc.date.submitted2021-06-29
dc.date.updated2021-11-22T14:43:04Z
dc.description.abstractAbstract: Engineering a low singlet-triplet energy gap (ΔEST) is necessary for efficient reverse intersystem crossing (rISC) in delayed fluorescence (DF) organic semiconductors but results in a small radiative rate that limits performance in LEDs. Here, we study a model DF material, BF2, that exhibits a strong optical absorption (absorption coefficient = 3.8 × 105 cm−1) and a relatively large ΔEST of 0.2 eV. In isolated BF2 molecules, intramolecular rISC is slow (delayed lifetime = 260 μs), but in aggregated films, BF2 generates intermolecular charge transfer (inter-CT) states on picosecond timescales. In contrast to the microsecond intramolecular rISC that is promoted by spin-orbit interactions in most isolated DF molecules, photoluminescence-detected magnetic resonance shows that these inter-CT states undergo rISC mediated by hyperfine interactions on a ~24 ns timescale and have an average electron-hole separation of ≥1.5 nm. Transfer back to the emissive singlet exciton then enables efficient DF and LED operation. Thus, access to these inter-CT states, which is possible even at low BF2 doping concentrations of 4 wt%, resolves the conflicting requirements of fast radiative emission and low ΔEST in organic DF emitters.
dc.identifier.doi10.17863/CAM.78307
dc.identifier.eissn2041-1723
dc.identifier.others41467-021-26689-8
dc.identifier.other26689
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/330864
dc.languageen
dc.publisherNature Publishing Group UK
dc.subjectArticle
dc.subject/639/301/1019/1020/1091
dc.subject/639/624/1020/1091
dc.subject/132
dc.subject/140/125
dc.subject/120
dc.subjectarticle
dc.titleSpontaneous exciton dissociation enables spin state interconversion in delayed fluorescence organic semiconductors
dc.typeArticle
dcterms.dateAccepted2021-10-14
prism.issueIdentifier1
prism.publicationNameNature Communications
prism.volume12
pubs.funder-project-idEC | EU Framework Programme for Research and Innovation H2020 | H2020 Priority Excellent Science | H2020 European Research Council (H2020 Excellent Science - European Research Council) (670405)
pubs.funder-project-idRCUK | Engineering and Physical Sciences Research Council (EPSRC) (EP/M01083X/1, EP/M005143/1)
pubs.funder-project-idSimons Foundation (601946)
rioxxterms.licenseref.urihttp://creativecommons.org/licenses/by/4.0/
rioxxterms.versionVoR
rioxxterms.versionofrecord10.1038/s41467-021-26689-8

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