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Dielectric control of reverse intersystem crossing in thermally activated delayed fluorescence emitters.

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cam.depositDate2023-01-09
cam.issuedOnline2022-08-04
cam.orpheus.success2023-01-11 - Embargo set during processing via Fast-track
datacite.issupplementedby.urlhttps://doi.org/10.17863/CAM.85068
dc.contributor.authorGillett, Alexander J
dc.contributor.authorPershin, Anton
dc.contributor.authorPandya, Raj
dc.contributor.authorFeldmann, Sascha
dc.contributor.authorSneyd, Alexander J
dc.contributor.authorAlvertis, Antonios M
dc.contributor.authorEvans, Emrys W
dc.contributor.authorThomas, Tudor H
dc.contributor.authorCui, Lin-Song
dc.contributor.authorDrummond, Bluebell H
dc.contributor.authorScholes, Gregory D
dc.contributor.authorOlivier, Yoann
dc.contributor.authorRao, Akshay
dc.contributor.authorFriend, Richard H
dc.contributor.authorBeljonne, David
dc.contributor.orcidGillett, Alexander J [0000-0001-7572-7333]
dc.contributor.orcidPershin, Anton [0000-0002-2414-6405]
dc.contributor.orcidFeldmann, Sascha [0000-0002-6583-5354]
dc.contributor.orcidSneyd, Alexander J [0000-0002-4205-0554]
dc.contributor.orcidEvans, Emrys W [0000-0002-9092-3938]
dc.contributor.orcidCui, Lin-Song [0000-0001-6577-3432]
dc.contributor.orcidDrummond, Bluebell H [0000-0001-5940-8631]
dc.contributor.orcidScholes, Gregory D [0000-0003-3336-7960]
dc.contributor.orcidRao, Akshay [0000-0003-4261-0766]
dc.contributor.orcidFriend, Richard H [0000-0001-6565-6308]
dc.contributor.orcidBeljonne, David [0000-0001-5082-9990]
dc.date.accessioned2023-01-12T00:30:22Z
dc.date.available2023-01-12T00:30:22Z
dc.date.issued2022-10
dc.date.updated2023-01-09T14:36:57Z
dc.description.abstractThermally activated delayed fluorescence enables organic semiconductors with charge transfer-type excitons to convert dark triplet states into bright singlets via reverse intersystem crossing. However, thus far, the contribution from the dielectric environment has received insufficient attention. Here we study the role of the dielectric environment in a range of thermally activated delayed fluorescence materials with varying changes in dipole moment upon optical excitation. In dipolar emitters, we observe how environmental reorganization after excitation triggers the full charge transfer exciton formation, minimizing the singlet-triplet energy gap, with the emergence of two (reactant-inactive) modes acting as a vibrational fingerprint of the charge transfer product. In contrast, the dielectric environment plays a smaller role in less dipolar materials. The analysis of energy-time trajectories and their free-energy functions reveals that the dielectric environment substantially reduces the activation energy for reverse intersystem crossing in dipolar thermally activated delayed fluorescence emitters, increasing the reverse intersystem crossing rate by three orders of magnitude versus the isolated molecule.
dc.format.mediumPrint-Electronic
dc.identifier.doi10.17863/CAM.92692
dc.identifier.eissn1476-4660
dc.identifier.issn1476-1122
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/345270
dc.language.isoeng
dc.publisherSpringer Science and Business Media LLC
dc.publisher.urlhttp://dx.doi.org/10.1038/s41563-022-01321-2
dc.rightsAll Rights Reserved
dc.rights.urihttp://www.rioxx.net/licenses/all-rights-reserved
dc.subjectFluorescence
dc.subjectSemiconductors
dc.titleDielectric control of reverse intersystem crossing in thermally activated delayed fluorescence emitters.
dc.typeArticle
dcterms.dateAccepted2022-06-13
prism.endingPage1157
prism.issueIdentifier10
prism.publicationDate2022
prism.publicationNameNat Mater
prism.startingPage1150
prism.volume21
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/M006360/1)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/M005143/1)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/M01083X/1)
pubs.funder-project-idEuropean Research Council (670405)
pubs.funder-project-idEuropean Research Council (758826)
pubs.licence-display-nameApollo Repository Deposit Licence Agreement
pubs.licence-identifierapollo-deposit-licence-2-1
rioxxterms.typeJournal Article/Review
rioxxterms.versionAM
rioxxterms.versionofrecord10.1038/s41563-022-01321-2

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