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Title: Large Thermal Motion in Halide Perovskites

Abstract

Solar cells based on hybrid perovskites have shown high efficiency while possessing simple processing methods. To gain a fundamental understanding of their properties on an atomic level, we investigate single crystals of CH 3NH 3PbI 3 with a narrow transition (~5 K) near 327 K. Temperature dependent structural measurements reveal a persistent tetragonal structure with smooth changes in the atomic displacement parameters (ADPs) on crossing T*. We show that the ADPs for I ions yield extended flat regions in the potential wells consistent with the measured large thermal expansion parameter. Molecular dynamics simulations reveal that this material exhibits significant asymmetries in the Pb-I pair distribution functions. We also show that the intrinsically enhanced freedom of motion of the iodine atoms enables large deformations. This flexibility (softness) of the atomic structure results in highly localized atomic relaxation about defects and hence accounts for both the high carrier mobility as well as the structural instability.

Authors:
 [1]; ORCiD logo [2];  [3];  [4];  [1]
  1. New Jersey Inst. of Technology, Newark, NJ (United States)
  2. Univ. of South Florida, Tampa, FL (United States)
  3. Univ. of Chicago, IL (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1413908
Report Number(s):
BNL-114284-2017-JA
Journal ID: ISSN 2045-2322
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Tyson, T. A., Gao, W., Chen, Y. -S., Ghose, S., and Yan, Y. Large Thermal Motion in Halide Perovskites. United States: N. p., 2017. Web. doi:10.1038/s41598-017-09220-2.
Tyson, T. A., Gao, W., Chen, Y. -S., Ghose, S., & Yan, Y. Large Thermal Motion in Halide Perovskites. United States. doi:10.1038/s41598-017-09220-2.
Tyson, T. A., Gao, W., Chen, Y. -S., Ghose, S., and Yan, Y. Thu . "Large Thermal Motion in Halide Perovskites". United States. doi:10.1038/s41598-017-09220-2. https://www.osti.gov/servlets/purl/1413908.
@article{osti_1413908,
title = {Large Thermal Motion in Halide Perovskites},
author = {Tyson, T. A. and Gao, W. and Chen, Y. -S. and Ghose, S. and Yan, Y.},
abstractNote = {Solar cells based on hybrid perovskites have shown high efficiency while possessing simple processing methods. To gain a fundamental understanding of their properties on an atomic level, we investigate single crystals of CH3NH3PbI3 with a narrow transition (~5 K) near 327 K. Temperature dependent structural measurements reveal a persistent tetragonal structure with smooth changes in the atomic displacement parameters (ADPs) on crossing T*. We show that the ADPs for I ions yield extended flat regions in the potential wells consistent with the measured large thermal expansion parameter. Molecular dynamics simulations reveal that this material exhibits significant asymmetries in the Pb-I pair distribution functions. We also show that the intrinsically enhanced freedom of motion of the iodine atoms enables large deformations. This flexibility (softness) of the atomic structure results in highly localized atomic relaxation about defects and hence accounts for both the high carrier mobility as well as the structural instability.},
doi = {10.1038/s41598-017-09220-2},
journal = {Scientific Reports},
number = 1,
volume = 7,
place = {United States},
year = {Thu Aug 24 00:00:00 EDT 2017},
month = {Thu Aug 24 00:00:00 EDT 2017}
}

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Works referenced in this record:

Efficient Hybrid Solar Cells Based on Meso-Superstructured Organometal Halide Perovskites
journal, October 2012


Semiconducting Tin and Lead Iodide Perovskites with Organic Cations: Phase Transitions, High Mobilities, and Near-Infrared Photoluminescent Properties
journal, July 2013

  • Stoumpos, Constantinos C.; Malliakas, Christos D.; Kanatzidis, Mercouri G.
  • Inorganic Chemistry, Vol. 52, Issue 15, p. 9019-9038
  • DOI: 10.1021/ic401215x