Asynchronous Photoexcited Electronic and Structural Relaxation in Lead-Free Perovskites

Journal of the American Chemical Society
Cunming LiuXiaoyi Zhang

Abstract

Vacancy-ordered lead-free perovskites with more-stable crystalline structures have been intensively explored as the alternatives for resolving the toxic and long-term stability issues of lead halide perovskites (LHPs). The dispersive energy bands produced by the closely packed halide octahedral sublattice in these perovskites are meanwhile anticipated to facility the mobility of charge carriers. However, these perovskites suffer from unexpectedly poor charge carrier transport. To tackle this issue, we have employed the ultrafast, elemental-specific X-ray transient absorption (XTA) spectroscopy to directly probe the photoexcited electronic and structural dynamics of a prototypical vacancy-ordered lead-free perovskite (Cs3Bi2Br9). We have discovered that the photogenerated holes quickly self-trapped at Br centers, simultaneously distorting the local lattice structure, likely forming small polarons in the configuration of Vk center (Br2- dimer). More significantly, we have found a surprisingly long-lived, structural distorted state with a lifetime of ∼59 μs, which is ∼3 orders of magnitude slower than that of the charge carrier recombination. Such long-lived structural distortion may produce a transient "background" under continuo...Continue Reading

References

Mar 1, 1989·Physical Review. B, Condensed Matter·N Nagaosa, T Ogawa
Sep 30, 2015·Advanced Materials·Byung-Wook ParkErik M J Johansson
Feb 26, 2016·Nature Materials·Aslihan BabayigitBert Conings
May 18, 2016·Nature Communications·Wanyi NieAditya D Mohite
Jun 11, 2016·Journal of the American Chemical Society·Annalise E MaughanJames R Neilson
Nov 2, 2016·The Journal of Physical Chemistry Letters·Kaibo ZhengSophie E Canton
Aug 19, 2017·Science Advances·Kiyoshi MiyataX-Y Zhu
Aug 23, 2017·Physical Chemistry Chemical Physics : PCCP·Byungkyun Kang, Koushik Biswas
Feb 21, 2018·Accounts of Chemical Research·Matthew D Smith, Hemamala I Karunadasa
Jun 30, 2018·Nature Communications·Myeongkee ParkRichard A Mathies

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Citations

Mar 31, 2021·The Journal of Physical Chemistry Letters·Adam D WrightLaura M Herz
Jun 3, 2021·Journal of the American Chemical Society·Oliviero CannelliGiulia F Mancini
Oct 31, 2019·Accounts of Chemical Research·Bin Yang, Keli Han
Aug 24, 2021·The Journal of Physical Chemistry Letters·Bin Yang, Keli Han
Jul 14, 2020·The Journal of Physical Chemistry Letters·Cunming LiuXiaoyi Zhang

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