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Asynchronous Photoexcited Electronic and Structural Relaxation in Lead-Free Perovskites

Liu, Cunming (author)
Argonne National Laboratory
Wang, Yingqi (author)
Center for High Pressure Science &Technology Advanced Research (HPSTAR)
Geng, Huifang (author)
ELI-HU Non-profit Ltd
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Zhu, Taishan (author)
University of Illinois at Urbana-Champaign
Ertekin, Elif (author)
University of Illinois at Urbana-Champaign
Gosztola, David (author)
Argonne National Laboratory
Yang, Sizhuo (author)
Marquette University
Huang, Jier (author)
Marquette University
Yang, Bin (author)
Dalian Institute of Chemical Physics Chinese Academy of Sciences
Han, Keli (author)
Dalian Institute of Chemical Physics Chinese Academy of Sciences
Canton, Sophie E. (author)
ELI-HU Non-profit Ltd,German Electron Synchrotron (DESY)
Kong, Qingyu (author)
Synchrotron SOLEIL
Zheng, Kaibo (author)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Technical University of Denmark
Zhang, Xiaoyi (author)
Argonne National Laboratory
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 (creator_code:org_t)
2019-07-30
2019
English.
In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 141:33, s. 13074-13080
Related links:
http://dx.doi.org/10...
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  • Journal article (peer-reviewed)
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  • 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 continuous light illumination, influencing the charge carrier transport along the lattice framework. ©

Subject headings

NATURVETENSKAP  -- Kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences (hsv//eng)

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