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dc.contributor.authorBooker, Edwarden
dc.contributor.authorThomas, Tudoren
dc.contributor.authorQuarti, Claudioen
dc.contributor.authorStanton, Michaelen
dc.contributor.authorDashwood, Cameron Den
dc.contributor.authorGillett, Alexen
dc.contributor.authorRichter, Johannesen
dc.contributor.authorPearson, Andrewen
dc.contributor.authorDavis, Nathaniel JLKen
dc.contributor.authorSirringhaus, Henningen
dc.contributor.authorPrice, Michaelen
dc.contributor.authorGreenham, Neilen
dc.contributor.authorBeljonne, Daviden
dc.contributor.authorDutton, Sianen
dc.contributor.authorDeschler, Felixen
dc.date.accessioned2018-02-07T09:44:00Z
dc.date.available2018-02-07T09:44:00Z
dc.date.issued2017-12-15en
dc.identifier.issn0002-7863
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/271757
dc.description.abstractWe investigate the origin of the broadband visible emission in layered hybrid lead-halide perovskites and its connection with structural and photophysical properties. We study <001> oriented thin films of hexylammonium (HA) lead iodide, (C6H16N)2PbI4, and dodecylammonium (DA) lead iodide, (C12H28N)2PbI4 by combining first-principles simulations with time-resolved photoluminescence, steady-state absorption and X-ray diffraction measurements on cooling from 300 K to 4 K. Ultrafast transient absorption and photoluminescence measurements are used to track the formation and recombination of emissive states. In addition to the excitonic photoluminescence near the absorption edge, we find a red-shifted, broadband (full-width at half maximum of about 0.4 eV), emission band below 200 K, similar to emission from <110> oriented bromide 2D perovskites at room temperature. The lifetime of this sub-bandgap emission exceeds that of the excitonic transition by orders of magnitude. We use X-ray diffraction measurements to study the changes in crystal lattice with temperature. We report changes in the octahedral tilt and lattice spacing in both materials, together with a phase change around 200 K in DA2PbI4. DFT simulations of the HA2PbI4 crystal structure indicate that the low-energy emission is due to interstitial iodide and related Frenkel defects. Our results demonstrate that white-light emission is not limited to <110> oriented bromide 2D perovskites but a general property of this class of system and highlight the importance of defect control for the formation of low-energy emissive sites, which can provide a pathway to design tailored white-light emitters.
dc.format.mediumPrint-Electronicen
dc.languageengen
dc.publisherAmerican Chemical Society
dc.rightsAttribution 4.0 International*
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/*
dc.titleFormation of Long-Lived Color Centers for Broadband Visible Light Emission in Low-Dimensional Layered Perovskites.en
dc.typeArticle
prism.endingPage18639
prism.issueIdentifier51en
prism.publicationDate2017en
prism.publicationNameJournal of the American Chemical Societyen
prism.startingPage18632
prism.volume139en
dc.identifier.doi10.17863/CAM.18749
dcterms.dateAccepted2017-11-20en
rioxxterms.versionofrecord10.1021/jacs.7b10223en
rioxxterms.versionVoR*
rioxxterms.licenseref.urihttp://www.rioxx.net/licenses/all-rights-reserveden
rioxxterms.licenseref.startdate2017-12-15en
dc.contributor.orcidBooker, Edward [0000-0001-8155-8206]
dc.contributor.orcidQuarti, Claudio [0000-0002-5488-1216]
dc.contributor.orcidDashwood, Cameron D [0000-0002-1582-3945]
dc.contributor.orcidPearson, Andrew [0000-0003-3634-4748]
dc.contributor.orcidDavis, Nathaniel JLK [0000-0003-2535-8968]
dc.contributor.orcidSirringhaus, Henning [0000-0001-9827-6061]
dc.contributor.orcidPrice, Michael [0000-0003-2227-0514]
dc.contributor.orcidGreenham, Neil [0000-0002-2155-2432]
dc.contributor.orcidDutton, Sian [0000-0003-0984-5504]
dc.contributor.orcidDeschler, Felix [0000-0002-0771-3324]
dc.identifier.eissn1520-5126
rioxxterms.typeJournal Article/Reviewen
pubs.funder-project-idEPSRC (EP/M005143/1)
pubs.funder-project-idEPSRC (via University of Liverpool) (unknown)
pubs.funder-project-idUNIVERSITY OF LIVERPOOL (FB EPSRC) (EP/L01551X/1)
pubs.funder-project-idEPSRC (EP/L015978/1)
cam.orpheus.successThu Jan 30 13:04:42 GMT 2020 - The item has an open VoR version.*
rioxxterms.freetoread.startdate2100-01-01


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