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Real-Time Observation of Exciton-Phonon Coupling Dynamics in Self-Assembled Hybrid Perovskite Quantum Wells

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cam.issuedOnline2017-10-24
cam.orpheus.successThu Jan 30 13:04:41 GMT 2020 - The item has an open VoR version.
datacite.issupplementedby.urlhttps://doi.org/10.17863/CAM.13802
dc.contributor.authorNi, L
dc.contributor.authorHuynh, U
dc.contributor.authorCheminal, A
dc.contributor.authorThomas, T
dc.contributor.authorShivanna, R
dc.contributor.authorHinrichsen, T
dc.contributor.authorAhmad, S
dc.contributor.authorSadhanala, A
dc.contributor.authorRao, A
dc.contributor.orcidNi, Limeng [0000-0001-6604-7336]
dc.contributor.orcidCheminal, Alexandre [0000-0001-9969-672X]
dc.contributor.orcidShivanna, Ravichandran [0000-0002-0915-6066]
dc.contributor.orcidHinrichsen, Ture [0000-0001-7599-2436]
dc.contributor.orcidSadhanala, Aditya [0000-0003-2832-4894]
dc.contributor.orcidRao, Akshay [0000-0003-0320-2962]
dc.date.accessioned2018-09-14T12:52:16Z
dc.date.available2018-09-14T12:52:16Z
dc.description.abstractSelf-assembled hybrid perovskite quantum wells have attracted attention due to their tunable emission properties, ease of fabrication and device integration. However, the dynamics of excitons in these materials, especially how they couple to phonons remains an open question. Here, we investigate two widely used materials, namely butylammonium lead iodide (CH3(CH2)3NH3)2PbI4 and hexylammonium lead iodide (CH3(CH2)5NH3)2PbI4, both of which exhibit broad photoluminescence tails at room temperature. We performed femtosecond vibrational spectroscopy to obtain a real-time picture of the exciton phonon interaction and directly identified the vibrational modes that couple to excitons. We show that the choice of the organic cation controls which vibrational modes the exciton couples to. In butylammonium lead iodide, excitons dominantly couple to a 100 cm-1 phonon mode, whereas in hexylammonium lead iodide, excitons interact with phonons with frequencies of 88 cm-1 and 137 cm-1. Using the determined optical phonon energies, we analyzed PL broadening mechanisms. At low temperatures (<100 K), the broadening is due to acoustic phonon scattering, whereas at high temperatures, LO phonon-exciton coupling is the dominant mechanism. Our results help explain the broad photoluminescence lineshapes observed in hybrid perovskite quantum wells and provide insights into the mechanism of exciton-phonon coupling in these materials.
dc.identifier.doi10.17863/CAM.27641
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/280271
dc.languageeng
dc.language.isoeng
dc.publisherAmerican Chemical Society
dc.publisher.urlhttps://pubs.acs.org/doi/10.1021/acsnano.7b03984
dc.rightsAttribution 4.0 International
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/
dc.subject2D materials
dc.subjectperovskites
dc.subjectRaman spectroscopy
dc.subjecttemperature-dependent photoluminescence
dc.subjecttransient absorption dynamics
dc.subjectultrafast vibrational spectroscopy
dc.titleReal-Time Observation of Exciton-Phonon Coupling Dynamics in Self-Assembled Hybrid Perovskite Quantum Wells
dc.typeArticle
dcterms.dateAccepted2017-10-24
prism.endingPage10843
prism.issueIdentifier11
prism.publicationNameACS Nano
prism.startingPage10834
prism.volume11
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/M006360/1)
pubs.funder-project-idEPSRC (1591119)
rioxxterms.licenseref.startdate2017-10-24
rioxxterms.licenseref.urihttp://creativecommons.org/licenses/by/4.0/
rioxxterms.typeJournal Article/Review
rioxxterms.versionVoR
rioxxterms.versionofrecord10.1021/acsnano.7b03984

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