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dc.contributor.authorPandya, Rajen
dc.contributor.authorGu, Qen
dc.contributor.authorCheminal, Aen
dc.contributor.authorChen, RYSen
dc.contributor.authorBooker, EPen
dc.contributor.authorSoucek, Ren
dc.contributor.authorSchott, Men
dc.contributor.authorLegrand, Len
dc.contributor.authorMathevet, Fen
dc.contributor.authorGreenham, Neilen
dc.contributor.authorBarisien, Ten
dc.contributor.authorMusser, AJen
dc.contributor.authorChin, AWen
dc.contributor.authorRao, Akshayen
dc.date.accessioned2021-01-08T00:32:08Z
dc.date.available2021-01-08T00:32:08Z
dc.date.issued2020-10-08en
dc.identifier.issn2451-9308
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/315898
dc.description.abstractThe S1 (21Ag-) state is an optically dark state of natural and synthetic pi-conjugated materials that can play a critical role in optoelectronic processes such as, energy harvesting, photoprotection and singlet fission. Despite this widespread importance, direct experimental characterisations of the electronic structure of the S1 (21Ag-) wavefunction have remained scarce and uncertain, although advanced theory predicts it to have a rich multi-excitonic character. Here, studying an archetypal polymer, polydiacetylene, and carotenoids, we experimentally demonstrate that S1 (21Ag-) is a superposition state with strong contributions from spin-entangled pairs of triplet excitons (1(TT)). We further show that optical manipulation of the S1 (21Ag-) wavefunction using triplet absorption transitions allows selective projection of the 1(TT) component into a manifold of spatially separated triplet-pairs with lifetimes enhanced by up to one order of magnitude and whose yield is strongly dependent on the level of inter-chromophore coupling. Our results provide a unified picture of 21Ag-states in pi-conjugated materials and open new routes to exploit their dynamics in singlet fission, photobiology and for the generation of entangled (spin-1) particles for molecular quantum technologies.
dc.rightsAttribution 4.0 International
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/
dc.titleOptical Projection and Spatial Separation of Spin-Entangled Triplet Pairs from the S<inf>1</inf> (2<sup>1</sup> A<inf>g</inf><sup>–</sup>) State of Pi-Conjugated Systemsen
dc.typeArticle
prism.endingPage2851
prism.issueIdentifier10en
prism.publicationDate2020en
prism.publicationNameChemen
prism.startingPage2826
prism.volume6en
dc.identifier.doi10.17863/CAM.63009
dcterms.dateAccepted2020-10-01en
rioxxterms.versionofrecord10.1016/j.chempr.2020.09.011en
rioxxterms.versionVoR
rioxxterms.licenseref.urihttp://www.rioxx.net/licenses/all-rights-reserveden
rioxxterms.licenseref.startdate2020-10-08en
dc.contributor.orcidPandya, Raj [0000-0003-1108-9322]
dc.contributor.orcidGreenham, Neil [0000-0002-2155-2432]
dc.contributor.orcidRao, Akshay [0000-0003-0320-2962]
dc.identifier.eissn2451-9294
rioxxterms.typeJournal Article/Reviewen
pubs.funder-project-idEPSRC (1805376)


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Attribution 4.0 International
Except where otherwise noted, this item's licence is described as Attribution 4.0 International