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Title: Real-Time Observation of Order-Disorder Transformation of Organic Cations Induced Phase Transition and Anomalous Photoluminescence in Hybrid Perovskites

A fundamental understanding of the interplay between the microscopic structure and macroscopic optoelectronic properties of organic-inorganic hybrid perovskite materials is essential to design new materials and improve device performance. However, how exactly the organic cations affect the structural phase transition and optoelectronic properties of the materials is not well understood. Here, real-time, in situ temperature-dependent neutron/X-ray diffraction and photoluminescence (PL) measurements reveal a transformation of the organic cation CH 3NH 3 + from order to disorder with increasing temperature in CH 3NH 3PbBr 3 perovskites. The molecular-level order-to-disorder transformation of CH 3NH 3 + not only leads to an anomalous increase in PL intensity, but also results in a multidomain to single-domain structural transition. Lastly, this discovery establishes the important role that organic cation ordering has in dictating structural order and anomalous optoelectronic phenomenon in hybrid perovskites.
Authors:
 [1] ;  [2] ;  [2] ;  [3] ;  [4] ;  [4] ;  [5] ;  [4] ;  [6] ;  [4]
  1. Hunan Univ., Changsha (China). College of Materials Science and Engineering, Key Lab. for Micro-Nano Physics and Technology of Hunan Province; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  5. Univ. of Nebraska, Lincoln, NE (United States). Dept. of Mechanical and Materials Engineering
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 22; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; optoelectronic properties; organohalide perovskites; phase transitions; single crystal neutron diffraction; solar cells
OSTI Identifier:
1458381
Alternate Identifier(s):
OSTI ID: 1433297

Yang, Bin, Ming, Wenmei, Du, Mao-Hua, Keum, Jong K., Puretzky, Alexander A., Rouleau, Christopher M., Huang, Jinsong, Geohegan, David B., Wang, Xiaoping, and Xiao, Kai. Real-Time Observation of Order-Disorder Transformation of Organic Cations Induced Phase Transition and Anomalous Photoluminescence in Hybrid Perovskites. United States: N. p., Web. doi:10.1002/adma.201705801.
Yang, Bin, Ming, Wenmei, Du, Mao-Hua, Keum, Jong K., Puretzky, Alexander A., Rouleau, Christopher M., Huang, Jinsong, Geohegan, David B., Wang, Xiaoping, & Xiao, Kai. Real-Time Observation of Order-Disorder Transformation of Organic Cations Induced Phase Transition and Anomalous Photoluminescence in Hybrid Perovskites. United States. doi:10.1002/adma.201705801.
Yang, Bin, Ming, Wenmei, Du, Mao-Hua, Keum, Jong K., Puretzky, Alexander A., Rouleau, Christopher M., Huang, Jinsong, Geohegan, David B., Wang, Xiaoping, and Xiao, Kai. 2018. "Real-Time Observation of Order-Disorder Transformation of Organic Cations Induced Phase Transition and Anomalous Photoluminescence in Hybrid Perovskites". United States. doi:10.1002/adma.201705801.
@article{osti_1458381,
title = {Real-Time Observation of Order-Disorder Transformation of Organic Cations Induced Phase Transition and Anomalous Photoluminescence in Hybrid Perovskites},
author = {Yang, Bin and Ming, Wenmei and Du, Mao-Hua and Keum, Jong K. and Puretzky, Alexander A. and Rouleau, Christopher M. and Huang, Jinsong and Geohegan, David B. and Wang, Xiaoping and Xiao, Kai},
abstractNote = {A fundamental understanding of the interplay between the microscopic structure and macroscopic optoelectronic properties of organic-inorganic hybrid perovskite materials is essential to design new materials and improve device performance. However, how exactly the organic cations affect the structural phase transition and optoelectronic properties of the materials is not well understood. Here, real-time, in situ temperature-dependent neutron/X-ray diffraction and photoluminescence (PL) measurements reveal a transformation of the organic cation CH3NH3 + from order to disorder with increasing temperature in CH3NH3PbBr3 perovskites. The molecular-level order-to-disorder transformation of CH3NH3 + not only leads to an anomalous increase in PL intensity, but also results in a multidomain to single-domain structural transition. Lastly, this discovery establishes the important role that organic cation ordering has in dictating structural order and anomalous optoelectronic phenomenon in hybrid perovskites.},
doi = {10.1002/adma.201705801},
journal = {Advanced Materials},
number = 22,
volume = 30,
place = {United States},
year = {2018},
month = {4}
}

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