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Title: Lattice dynamics and the nature of structural transitions in organolead halide perovskites

Abstract

Organolead halide perovskites are a family of hybrid organic-inorganic compounds whose remark- able optoelectronic properties have been under intensive scrutiny in recent years. Here we use inelastic X-ray scattering to study low-energy lattice excitations in single crystals of methylammonium lead iodide and bromide perovskites. Our ndings conrm the displacive nature of the cubic-to- tetragonal phase transition, which is further shown, using neutron and x-ray diraction, to be close to a tricritical point. The experimental sound speed, around 100-200 m/s, suggests that electron- phonon scattering is likely a limiting factor for further improvements in carrier mobility. Lastly, we detect quasistatic symmetry-breaking nanodomains persisting well into the high-temperature cubic phase, possibly stabilized by local defects. These ndings reveal key structural properties of these materials, but also bear important implications for carrier dynamics across an extended temperature range relevant for photovoltaic applications.

Authors:
 [1];  [2];  [3];  [4];  [5];  [6];  [6];  [1];  [1];  [7];  [1]
+ Show Author Affiliations
  1. Univ. of Toronto, ON (Canada). Dept. of Electrical and Computer Engineering
  2. DuPont Central Research and Development, Wilmington, DE (United States); Univ. of Delaware, Newark, DE (United States). Dept. of Physics and Astronomy
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  4. DuPont Electronics and Communication Technologies, Wilmington, DE (United States)
  5. DuPont Central Research and Development, Wilmington, DE (United States)
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division
  7. Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Mechanical Engineering
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Org.:
Natural Sciences and Engineering Research Council of Canada (NSERC); USDOE Office of Science (SC)
OSTI Identifier:
1328290
Alternate Identifier(s):
OSTI ID: 1323583
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 94; Journal Issue: 9; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Comin, Riccardo, Crawford, Michael K., Said, Ayman H., Herron, Norman, Guise, William E., Wang, Xiaoping, Whitfield, Pamela S., Jain, Ankit, Gong, Xiwen, McGaughey, Alan J. H., and Sargent, Edward H. Lattice dynamics and the nature of structural transitions in organolead halide perovskites. United States: N. p., 2016. Web. doi:10.1103/PhysRevB.94.094301.
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Comin, Riccardo, Crawford, Michael K., Said, Ayman H., Herron, Norman, Guise, William E., Wang, Xiaoping, Whitfield, Pamela S., Jain, Ankit, Gong, Xiwen, McGaughey, Alan J. H., & Sargent, Edward H. Lattice dynamics and the nature of structural transitions in organolead halide perovskites. United States. https://doi.org/10.1103/PhysRevB.94.094301
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Comin, Riccardo, Crawford, Michael K., Said, Ayman H., Herron, Norman, Guise, William E., Wang, Xiaoping, Whitfield, Pamela S., Jain, Ankit, Gong, Xiwen, McGaughey, Alan J. H., and Sargent, Edward H. Fri . "Lattice dynamics and the nature of structural transitions in organolead halide perovskites". United States. https://doi.org/10.1103/PhysRevB.94.094301. https://www.osti.gov/servlets/purl/1328290.
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@article{osti_1328290,
title = {Lattice dynamics and the nature of structural transitions in organolead halide perovskites},
author = {Comin, Riccardo and Crawford, Michael K. and Said, Ayman H. and Herron, Norman and Guise, William E. and Wang, Xiaoping and Whitfield, Pamela S. and Jain, Ankit and Gong, Xiwen and McGaughey, Alan J. H. and Sargent, Edward H.},
abstractNote = {Organolead halide perovskites are a family of hybrid organic-inorganic compounds whose remark- able optoelectronic properties have been under intensive scrutiny in recent years. Here we use inelastic X-ray scattering to study low-energy lattice excitations in single crystals of methylammonium lead iodide and bromide perovskites. Our ndings conrm the displacive nature of the cubic-to- tetragonal phase transition, which is further shown, using neutron and x-ray diraction, to be close to a tricritical point. The experimental sound speed, around 100-200 m/s, suggests that electron- phonon scattering is likely a limiting factor for further improvements in carrier mobility. Lastly, we detect quasistatic symmetry-breaking nanodomains persisting well into the high-temperature cubic phase, possibly stabilized by local defects. These ndings reveal key structural properties of these materials, but also bear important implications for carrier dynamics across an extended temperature range relevant for photovoltaic applications.},
doi = {10.1103/PhysRevB.94.094301},
journal = {Physical Review B},
number = 9,
volume = 94,
place = {United States},
year = {Fri Sep 09 00:00:00 EDT 2016},
month = {Fri Sep 09 00:00:00 EDT 2016}
}
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https://doi.org/10.1103/PhysRevB.94.094301
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    Works referencing / citing this record:

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    Assessment of dynamic structural instabilities across 24 cubic inorganic halide perovskites
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    Phonon anharmonicity, lifetimes, and thermal transport in CH 3 NH 3 PbI 3 from many-body perturbation theory
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