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dc.contributor.authorHedley, Gordon James
dc.contributor.authorQuarti, C
dc.contributor.authorHarwell, Jonathon Robert
dc.contributor.authorPrezhdo, O
dc.contributor.authorBeljonne, D
dc.contributor.authorSamuel, Ifor David William
dc.date.accessioned2018-05-25T16:30:05Z
dc.date.available2018-05-25T16:30:05Z
dc.date.issued2018-05-25
dc.identifier.citationHedley , G J , Quarti , C , Harwell , J R , Prezhdo , O , Beljonne , D & Samuel , I D W 2018 , ' Hot-Hole cooling controls the initial ultrafast relaxation in methylammonium lead iodide perovskite ' , Scientific Reports , vol. 8 , 8115 . https://doi.org/10.1038/s41598-018-26207-9en
dc.identifier.issn2045-2322
dc.identifier.otherPURE: 253036442
dc.identifier.otherPURE UUID: 927c150b-4b51-4a43-8222-750fa3b3016e
dc.identifier.otherScopus: 85047833693
dc.identifier.otherWOS: 000433059900025
dc.identifier.otherORCID: /0000-0002-2508-1965/work/90952158
dc.identifier.urihttps://hdl.handle.net/10023/13547
dc.descriptionFunding: EPSRC (grants EP/J009016 and EP/L017008) and the European Research Council (grant 321305). IDWS acknowledges a Royal Society Wolfson Research Merit Award.en
dc.description.abstractUnderstanding the initial ultrafast excited state dynamics of methylammonium lead iodide (MAPI) perovskite is of vital importance to enable its fullest utilisation in optoelectronic devices and the design of improved materials. Here we have combined advanced measurements of the ultrafast photoluminescence from MAPI films up to 0.6 eV above the relaxed excited state with cutting-edge advanced non-adiabatic quantum dynamics simulations, to provide a powerful unique insight into the earliest time behaviour in MAPI. Our joint experimental-theoretical approach highlights that the cooling of holes from deep in the valence band to the valence band edge is fast, occurring on a 100-500 fs timescale. Cooling of electrons from high in the conduction band to the conduction band edge, however, is much slower, on the order of 1-10 ps. Density of states calculations indicate that excited states with holes deep in the valence band are greatly favoured upon photoexcitation, and this matches well with the fast (100-500 fs) formation time for the relaxed excited state observed in our ultrafast PL measurements. Consequently we are able to provide a complete observation of the initial excited state evolution in this important prototypical material.
dc.format.extent9
dc.language.isoeng
dc.relation.ispartofScientific Reportsen
dc.rights© 2018, the Author(s). This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/en
dc.subjectQC Physicsen
dc.subjectTK Electrical engineering. Electronics Nuclear engineeringen
dc.subjectDASen
dc.subject.lccQCen
dc.subject.lccTKen
dc.titleHot-Hole cooling controls the initial ultrafast relaxation in methylammonium lead iodide perovskiteen
dc.typeJournal articleen
dc.contributor.sponsorEPSRCen
dc.contributor.sponsorEuropean Research Councilen
dc.contributor.sponsorEPSRCen
dc.description.versionPublisher PDFen
dc.contributor.institutionUniversity of St Andrews. School of Physics and Astronomyen
dc.contributor.institutionUniversity of St Andrews. Condensed Matter Physicsen
dc.identifier.doihttps://doi.org/10.1038/s41598-018-26207-9
dc.description.statusPeer revieweden
dc.identifier.grantnumberep/l017008/1en
dc.identifier.grantnumberen
dc.identifier.grantnumberN/Aen


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