Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites

Wu, Xiaoxi; Tan, Liang Z.; Shen, Xiaozhe; Hu, Te; Miyata, Kiyoshi; Trinh, M. Tuan; Li, Renkai; Coffee, Ryan; Liu, Shi; Egger, David A.; Makasyuk, Igor; Zheng, Qiang; Fry, Alan; Robinson, Joseph S.; Smith, Matthew D.; Guzelturk, Burak; Karunadasa, Hemamala I.; Wang, Xijie; Zhu, Xiaoyang; Kronik, Leeor; Rappe, Andrew M.; Lindenberg, Aaron M.

doi:10.1126/sciadv.1602388

Title: Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites

Journal Article · Wed Jul 26 00:00:00 EDT 2017 · Science Advances

DOI:https://doi.org/10.1126/sciadv.1602388· OSTI ID:1380107

Wu, Xiaoxi ^[1]; Tan, Liang Z. ^[2]; Shen, Xiaozhe ^[3]; Hu, Te ^[4];

^[5]; Trinh, M. Tuan ^[5]; Li, Renkai ^[3];

^[3]; Liu, Shi ^[6]; Egger, David A. ^[7]; Makasyuk, Igor ^[3]; Zheng, Qiang ^[3]; Fry, Alan ^[3]; Robinson, Joseph S. ^[3]; Smith, Matthew D. ^[8]; Guzelturk, Burak ^[1]; Karunadasa, Hemamala I. ^[8]; Wang, Xijie ^[3];

^[5]; Kronik, Leeor ^[7] more »

SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
Univ. of Pennsylvania, Philadelphia, PA (United States). Makineni Theoretical Lab., Dept. of Chemistry
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
Columbia Univ., New York, NY (United States). Dept. of Chemistry
Carnegie Inst. for Science, Washington, DC (United States). Extreme Materials Initiative, Geophysical Lab.
Weizmann Inst. of Science, Rehovoth (Israel). Dept. of Materials and Interfaces
Stanford Univ., CA (United States). Dept. of Chemistry
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES); Stanford Univ., CA (United States). Dept. of Materials Science and Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)

Femtosecond resolution electron scattering techniques are applied to resolve the first atomic-scale steps following absorption of a photon in the prototypical hybrid perovskite methylammonium lead iodide. Following above-gap photoexcitation, we directly resolve the transfer of energy from hot carriers to the lattice by recording changes in the mean square atomic displacements on 10-ps time scales. Measurements of the time-dependent pair distribution function show an unexpected broadening of the iodine-iodine correlation function while preserving the Pb-I distance. This indicates the formation of a rotationally disordered halide octahedral structure developing on picosecond time scales. Here, this work shows the important role of light-induced structural deformations within the inorganic sublattice in elucidating the unique optoelectronic functionality exhibited by hybrid perovskites and provides new understanding of hot carrier-lattice interactions, which fundamentally determine solar cell efficiencies.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Austrian Science Fund (FWF)

Grant/Contract Number:: AC02-76SF00515; ER46980; N00014-17-1-2574; DGE-114747; ECCS-1542152

OSTI ID:: 1380107

Journal Information:: Science Advances, Vol. 3, Issue 7; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 128 works

Citation information provided by
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Large electrostrictive response in lead halide perovskites E., Mosconi,; B., Chen,; J., Song, The University of North Carolina at Chapel Hill University Libraries https://doi.org/10.17615/fjfy-8b57	text	January 2018
Hot Electron Injection into Semiconducting Polymers in Polymer Based-Perovskite Solar Cells and Their Fate Jiménez-López, Jesús; Puscher, Bianka M. D.; Cambarau, Werther SSRN Electronic Journal https://doi.org/10.2139/ssrn.3305584	journal	January 2018
Unraveling exciton-phonon coupling in individual FAPbI(3) nanocrystals emitting near-infrared single photons Fu, Ming; Tamarat, Philippe; Trebbia, Jean-Baptiste ETH Zurich https://doi.org/10.3929/ethz-b-000285895	text	January 2018
Incorporating Large A Cations into Lead Iodide Perovskite Cages: Relaxed Goldschmidt Tolerance Factor and Impact on Exciton–Phonon Interaction Fu, Yongping; Hautzinger, Matthew P.; Luo, Ziyu ACS Central Science, Vol. 5, Issue 8 https://doi.org/10.1021/acscentsci.9b00367	journal	July 2019
Slow cooling of hot polarons in halide perovskite solar cells Frost, Jarvist Moore; Whalley, Lucy D.; Walsh, Aron arXiv https://doi.org/10.48550/arxiv.1708.04158	text	January 2017

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