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Spontaneous exciton...
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Gillett, Alexander J.Univ Cambridge, England
(author)
Spontaneous exciton dissociation enables spin state interconversion in delayed fluorescence organic semiconductors
- Article/chapterEnglish2021
Publisher, publication year, extent ...
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2021-11-17
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Nature Portfolio,2021
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electronicrdacarrier
Numbers
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LIBRIS-ID:oai:DiVA.org:liu-181469
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https://urn.kb.se/resolve?urn=urn:nbn:se:liu:diva-181469URI
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https://doi.org/10.1038/s41467-021-26689-8DOI
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Language:English
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Summary in:English
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Subject category:ref swepub-contenttype
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Subject category:art swepub-publicationtype
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Funding Agencies|Simons Foundation [601946]; EPSRCUK Research & Innovation (UKRI)Engineering & Physical Sciences Research Council (EPSRC) [EP/M01083X/1, EP/M005143/1, EP/L01551X/1]; European Research Council (ERC) under the European Unions Horizon 2020 research and innovation programmeEuropean Research Council (ERC) [670405]; Swedish Energy AgencySwedish Energy AgencyMaterials & Energy Research Center (MERC) [EM-48594-1]; Swedish Research CouncilSwedish Research CouncilEuropean Commission [VR-2017-05285]; Aix Marseille Universite; CNRSCentre National de la Recherche Scientifique (CNRS)European Commission; Basque GovernmentBasque Government [PIBA19-0004]; Spanish Government MINECO/FEDERSpanish Government [PID2019-109555GB-I00]; European Unions Horizon 2020 research and innovation programme under Marie Skodowska Curie Grant [722651]; Fonds de la Recherche Scientifiques de Belgique (F.R.S.-FNRS)Fonds de la Recherche Scientifique - FNRS [2.5020.11]; Tier-1 supercomputer of the Federation Wallonie-Bruxelles; Walloon Region [1117545]; FRS-FNRSFonds de la Recherche Scientifique - FNRS [F.4534.21]; Fonds pour la formation a la Recherche dans lIndustrie et dans lAgriculture (F.R.I.A.) of the F.R.S.-F.N.R.S
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Engineering a low singlet-triplet energy gap (Delta E-ST) 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 x 10(5) cm(-1)) and a relatively large Delta E-ST of 0.2 eV. In isolated BF2 molecules, intramolecular rISC is slow (delayed lifetime = 260 mu s), 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 similar to 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 Delta E-ST in organic DF emitters.
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Tonnele, ClaireDonostia Int Phys Ctr DIPC, Spain
(author)
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Londi, GiacomoUniv Mons, Belgium
(author)
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Ricci, GaetanoUniv Namur, Belgium; Univ Namur, Belgium
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Catherin, ManonAix Marseille Univ, France
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Unson, Darcy M. L.Univ Cambridge, England
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Casanova, DavidDonostia Int Phys Ctr DIPC, Spain
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Castet, FredericUniv Bordeaux, France
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Olivier, YoannUniv Namur, Belgium; Univ Namur, Belgium
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Chen, WeiminLinköpings universitet,Elektroniska och fotoniska material,Tekniska fakulteten(Swepub:liu)weich55
(author)
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Zaborova, ElenaAix Marseille Univ, France
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Evans, Emrys W.Univ Cambridge, England; Swansea Univ, Wales
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Drummond, Bluebell H.Univ Cambridge, England
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Conaghan, Patrick J.Univ Cambridge, England; Univ Sydney, Australia
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Cui, Lin-SongUniv Cambridge, England; Univ Sci & Technol China, Peoples R China
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Greenham, Neil C.Univ Cambridge, England
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Puttisong, YuttapoomLinköpings universitet,Elektroniska och fotoniska material,Tekniska fakulteten(Swepub:liu)yutpu33
(author)
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Fages, FredericAix Marseille Univ, France
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Beljonne, DavidUniv Mons, Belgium
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Friend, Richard H.Univ Cambridge, England
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Univ Cambridge, EnglandDonostia Int Phys Ctr DIPC, Spain
(creator_code:org_t)
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In:Nature Communications: Nature Portfolio12:12041-1723
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Gillett, Alexand ...
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Tonnele, Claire
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Londi, Giacomo
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Ricci, Gaetano
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Catherin, Manon
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Unson, Darcy M. ...
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Casanova, David
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Castet, Frederic
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Olivier, Yoann
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Chen, Weimin
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Zaborova, Elena
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Evans, Emrys W.
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Drummond, Bluebe ...
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Conaghan, Patric ...
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Cui, Lin-Song
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Greenham, Neil C ...
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Fages, Frederic
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