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Hot-Hole cooling controls the initial ultrafast relaxation in methylammonium lead iodide perovskite

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Date
25/05/2018
Author
Hedley, Gordon James
Quarti, C
Harwell, Jonathon Robert
Prezhdo, O
Beljonne, D
Samuel, Ifor David William
Funder
EPSRC
European Research Council
EPSRC
Grant ID
ep/l017008/1
N/A
Keywords
QC Physics
TK Electrical engineering. Electronics Nuclear engineering
DAS
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Abstract
Understanding 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.
Citation
Hedley , 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/s41598-018-26207-9
Publication
Scientific Reports
Status
Peer reviewed
DOI
https://doi.org/10.1038/s41598-018-26207-9
ISSN
2045-2322
Type
Journal article
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/
Description
Funding: EPSRC (grants EP/J009016 and EP/L017008) and the European Research Council (grant 321305). IDWS acknowledges a Royal Society Wolfson Research Merit Award.
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  • University of St Andrews Research
URI
http://hdl.handle.net/10023/13547

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