dc.contributor.author Richter, Johannes en dc.contributor.author Branchi, F en dc.contributor.author Valduga de Almeida Camargo, F en dc.contributor.author Zhao, Baodan en dc.contributor.author Friend, Richard en dc.contributor.author Cerullo, G en dc.contributor.author Deschler, Felix en dc.date.accessioned 2017-07-20T10:14:20Z dc.date.available 2017-07-20T10:14:20Z dc.identifier.issn 2041-1723 dc.identifier.uri https://www.repository.cam.ac.uk/handle/1810/265674 dc.description.abstract In band-like semiconductors, charge carriers form a thermal energy distribution rapidly after optical excitation. In hybrid perovskites, the cooling of such thermal carrier distributions occurs on timescales of about 300 fs via carrier-phonon scattering. However, the initial build-up of the thermal distribution proved difficult to resolve with pump–probe techniques due to the requirement of high resolution, both in time and pump energy. Here, we use two-dimensional electronic spectroscopy with sub-10 fs resolution to directly observe the carrier interactions that lead to a thermal carrier distribution. We find that thermalization occurs dominantly via carrier-carrier scattering under the investigated fluences and report the dependence of carrier scattering rates on excess energy and carrier density. We extract characteristic carrier thermalization times from below 10 to 85 fs. These values allow for mobilities of 500 cm$^2$ V$^{−1}$s$^{−1}$ at carrier densities lower than 2 × 10$^{19}$ cm$^{−3}$ and limit the time for carrier extraction in hot carrier solar cells. dc.description.sponsorship This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement no 654148 Laserlab-Europe (CUSBO 002151). We acknowledge further financial support from the Engineering and Physical Sciences Research Council of the UK (EPSRC). G.C. acknowledges support by the European Union Horizon 2020 Programme under Grant Agreement No. 696656 Graphene Flagship and by the European Research Council Advanced Grant STRATUS (ERC-2011-AdG No. 291198). J.M.R. and F.D. thank the Winton Programme for the Physics of Sustainability (University of Cambridge). J.M.R. thanks the Cambridge Home European Scheme for financial support. F.D. acknowledges funding from a Herchel Smith Research Fellowship and a Winton Advanced Research Fellowship. We thank Cristian Manzoni for fruitful discussions. dc.language.iso en en dc.publisher Nature Publishing Group dc.rights Attribution 4.0 International en dc.rights.uri http://creativecommons.org/licenses/by/4.0/ en dc.title Ultrafast carrier thermalization in lead iodide perovskite probed with two-dimensional electronic spectroscopy en dc.type Article prism.number 376 en prism.publicationName Nature Communications en prism.volume 8 en dc.identifier.doi 10.17863/CAM.11191 dcterms.dateAccepted 2017-07-07 en rioxxterms.versionofrecord 10.1038/s41467-017-00546-z en rioxxterms.version VoR en rioxxterms.licenseref.uri http://creativecommons.org/licenses/by/4.0/ en rioxxterms.licenseref.startdate 2017-07-07 en dc.contributor.orcid Friend, Richard [0000-0001-6565-6308] dc.contributor.orcid Deschler, Felix [0000-0002-0771-3324] dc.identifier.eissn 2041-1723 rioxxterms.type Journal Article/Review en pubs.funder-project-id EPSRC (EP/M005143/1) pubs.funder-project-id EPSRC (1492283) pubs.funder-project-id European Commission Horizon 2020 (H2020) Future and Emerging Technologies (FET) (696656) cam.issuedOnline 2017-08-29 en datacite.issupplementedby.doi 10.17863/CAM.11883 en cam.orpheus.success Thu Jan 30 12:53:38 GMT 2020 - The item has an open VoR version. * rioxxterms.freetoread.startdate 2100-01-01
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