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Vibronically coherent ultrafast triplet-pair formation and subsequent thermally activated dissociation control efficient endothermic singlet fission.

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cam.issuedOnline2017-09-11
dc.contributor.authorStern, Hannah L
dc.contributor.authorCheminal, Alexandre
dc.contributor.authorYost, Shane R
dc.contributor.authorBroch, Katharina
dc.contributor.authorBayliss, Sam L
dc.contributor.authorChen, Kai
dc.contributor.authorTabachnyk, Maxim
dc.contributor.authorThorley, Karl
dc.contributor.authorGreenham, Neil
dc.contributor.authorHodgkiss, Justin M
dc.contributor.authorAnthony, John
dc.contributor.authorHead-Gordon, Martin
dc.contributor.authorMusser, Andrew J
dc.contributor.authorRao, Akshay
dc.contributor.authorFriend, Richard H
dc.contributor.orcidCheminal, Alexandre [0000-0001-9969-672X]
dc.contributor.orcidTabachnyk, Maxim [0000-0001-9390-3791]
dc.contributor.orcidAnthony, John [0000-0002-8972-1888]
dc.contributor.orcidRao, Akshay [0000-0003-0320-2962]
dc.contributor.orcidFriend, Richard H [0000-0001-6565-6308]
dc.date.accessioned2018-09-27T14:10:20Z
dc.date.available2018-09-27T14:10:20Z
dc.date.issued2017-12
dc.description.abstractSinglet exciton fission (SF), the conversion of one spin-singlet exciton (S1) into two spin-triplet excitons (T1), could provide a means to overcome the Shockley-Queisser limit in photovoltaics. SF as measured by the decay of S1 has been shown to occur efficiently and independently of temperature, even when the energy of S1 is as much as 200 meV less than that of 2T1. Here we study films of triisopropylsilyltetracene using transient optical spectroscopy and show that the triplet pair state (TT), which has been proposed to mediate singlet fission, forms on ultrafast timescales (in 300 fs) and that its formation is mediated by the strong coupling of electronic and vibrational degrees of freedom. This is followed by a slower loss of singlet character as the excitation evolves to become only TT. We observe the TT to be thermally dissociated on 10-100 ns timescales to form free triplets. This provides a model for 'temperature-independent' efficient TT formation and thermally activated TT separation.
dc.format.mediumPrint-Electronic
dc.identifier.doi10.17863/CAM.30165
dc.identifier.eissn1755-4349
dc.identifier.issn1755-4330
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/282801
dc.languageeng
dc.language.isoeng
dc.publisherSpringer Science and Business Media LLC
dc.publisher.urlhttp://dx.doi.org/10.1038/nchem.2856
dc.subject34 Chemical Sciences
dc.subject3406 Physical Chemistry
dc.subject3407 Theoretical and Computational Chemistry
dc.titleVibronically coherent ultrafast triplet-pair formation and subsequent thermally activated dissociation control efficient endothermic singlet fission.
dc.typeArticle
dcterms.dateAccepted2017-07-28
prism.endingPage1212
prism.issueIdentifier12
prism.publicationDate2017
prism.publicationNameNat Chem
prism.startingPage1205
prism.volume9
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/M024873/1)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/P027741/1)
rioxxterms.licenseref.startdate2017-12
rioxxterms.licenseref.urihttp://www.rioxx.net/licenses/all-rights-reserved
rioxxterms.typeJournal Article/Review
rioxxterms.versionAM
rioxxterms.versionofrecord10.1038/nchem.2856

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