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

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.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ; ORCiD logo [5] ;  [5] ;  [3] ; ORCiD logo [3] ;  [6] ;  [7] ;  [3] ;  [3] ;  [3] ;  [3] ;  [8] ;  [1] ;  [8] ;  [3] ; ORCiD logo [5] ;  [7] more »;  [2] ; ORCiD logo [9] « less
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
  2. Univ. of Pennsylvania, Philadelphia, PA (United States). Makineni Theoretical Lab., Dept. of Chemistry
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
  5. Columbia Univ., New York, NY (United States). Dept. of Chemistry
  6. Carnegie Inst. for Science, Washington, DC (United States). Extreme Materials Initiative, Geophysical Lab.
  7. Weizmann Inst. of Science, Rehovoth (Israel). Dept. of Materials and Interfaces
  8. Stanford Univ., CA (United States). Dept. of Chemistry
  9. 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)
Publication Date:
Grant/Contract Number:
AC02-76SF00515; ER46980; N00014-17-1-2574; DGE-114747; ECCS-1542152
Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 3; Journal Issue: 7; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); Austrian Science Fund (FWF)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
OSTI Identifier:
1380107

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., and Lindenberg, Aaron M.. Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites. United States: N. p., Web. doi:10.1126/sciadv.1602388.
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.. Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites. United States. doi:10.1126/sciadv.1602388.
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., and Lindenberg, Aaron M.. 2017. "Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites". United States. doi:10.1126/sciadv.1602388. https://www.osti.gov/servlets/purl/1380107.
@article{osti_1380107,
title = {Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites},
author = {Wu, Xiaoxi and Tan, Liang Z. and Shen, Xiaozhe and Hu, Te and Miyata, Kiyoshi and Trinh, M. Tuan and Li, Renkai and Coffee, Ryan and Liu, Shi and Egger, David A. and Makasyuk, Igor and Zheng, Qiang and Fry, Alan and Robinson, Joseph S. and Smith, Matthew D. and Guzelturk, Burak and Karunadasa, Hemamala I. and Wang, Xijie and Zhu, Xiaoyang and Kronik, Leeor and Rappe, Andrew M. and Lindenberg, Aaron M.},
abstractNote = {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.},
doi = {10.1126/sciadv.1602388},
journal = {Science Advances},
number = 7,
volume = 3,
place = {United States},
year = {2017},
month = {7}
}

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