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Title: Chemical nature of ferroelastic twin domains in CH 3NH 3PbI 3 perovskite

The extraordinary optoelectronic performance of hybrid organic–inorganic perovskites has resulted in extensive efforts to unravel their properties. Recently, observations of ferroic twin domains in methylammonium lead triiodide drew significant attention as a possible explanation for the current–voltage hysteretic behaviour in these materials. However, the properties of the twin domains, their local chemistry and the chemical impact on optoelectronic performance remain unclear. Here, using multimodal chemical and functional imaging methods, we unveil the mechanical origin of the twin domain contrast observed with piezoresponse force microscopy in methylammonium lead triiodide. By combining experimental results with first principles simulations we reveal an inherent coupling between ferroelastic twin domains and chemical segregation. Furthermore, these results reveal an interplay of ferroic properties and chemical segregation on the optoelectronic performance of hybrid organic–inorganic perovskites, and offer an exploratory path to improving functional devices.
Authors:
ORCiD logo [1] ; ORCiD logo [2] ;  [3] ; ORCiD logo [4] ;  [5] ; ORCiD logo [2] ;  [5] ;  [5] ; ORCiD logo [2] ; ORCiD logo [2] ; ORCiD logo [2] ; ORCiD logo [2] ; ORCiD logo [2] ; ORCiD logo [2] ; ORCiD logo [2] ; ORCiD logo [2] ;  [5] ; ORCiD logo [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Asylum Research an Oxford Instruments Co., Santa Barbara, CA (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Pusan National Univ., Busan (South Korea)
  5. Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 17; Journal Issue: 11; Journal ID: ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing Group
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
OSTI Identifier:
1486954

Liu, Yongtao, Collins, Liam F., Proksch, Roger, Kim, Songkil, Watson, Brianna R., Doughty, Benjamin, Calhoun, Tessa R., Ahmadi, Mahshid, Ievlev, Anton V., Jesse, Stephen, Retterer, Scott T., Belianinov, Alex, Xiao, Kai, Huang, Jingsong, Sumpter, Bobby G., Kalinin, Sergei V., Hu, Bin, and Ovchinnikova, Olga S.. Chemical nature of ferroelastic twin domains in CH3NH3PbI3 perovskite. United States: N. p., Web. doi:10.1038/s41563-018-0152-z.
Liu, Yongtao, Collins, Liam F., Proksch, Roger, Kim, Songkil, Watson, Brianna R., Doughty, Benjamin, Calhoun, Tessa R., Ahmadi, Mahshid, Ievlev, Anton V., Jesse, Stephen, Retterer, Scott T., Belianinov, Alex, Xiao, Kai, Huang, Jingsong, Sumpter, Bobby G., Kalinin, Sergei V., Hu, Bin, & Ovchinnikova, Olga S.. Chemical nature of ferroelastic twin domains in CH3NH3PbI3 perovskite. United States. doi:10.1038/s41563-018-0152-z.
Liu, Yongtao, Collins, Liam F., Proksch, Roger, Kim, Songkil, Watson, Brianna R., Doughty, Benjamin, Calhoun, Tessa R., Ahmadi, Mahshid, Ievlev, Anton V., Jesse, Stephen, Retterer, Scott T., Belianinov, Alex, Xiao, Kai, Huang, Jingsong, Sumpter, Bobby G., Kalinin, Sergei V., Hu, Bin, and Ovchinnikova, Olga S.. 2018. "Chemical nature of ferroelastic twin domains in CH3NH3PbI3 perovskite". United States. doi:10.1038/s41563-018-0152-z.
@article{osti_1486954,
title = {Chemical nature of ferroelastic twin domains in CH3NH3PbI3 perovskite},
author = {Liu, Yongtao and Collins, Liam F. and Proksch, Roger and Kim, Songkil and Watson, Brianna R. and Doughty, Benjamin and Calhoun, Tessa R. and Ahmadi, Mahshid and Ievlev, Anton V. and Jesse, Stephen and Retterer, Scott T. and Belianinov, Alex and Xiao, Kai and Huang, Jingsong and Sumpter, Bobby G. and Kalinin, Sergei V. and Hu, Bin and Ovchinnikova, Olga S.},
abstractNote = {The extraordinary optoelectronic performance of hybrid organic–inorganic perovskites has resulted in extensive efforts to unravel their properties. Recently, observations of ferroic twin domains in methylammonium lead triiodide drew significant attention as a possible explanation for the current–voltage hysteretic behaviour in these materials. However, the properties of the twin domains, their local chemistry and the chemical impact on optoelectronic performance remain unclear. Here, using multimodal chemical and functional imaging methods, we unveil the mechanical origin of the twin domain contrast observed with piezoresponse force microscopy in methylammonium lead triiodide. By combining experimental results with first principles simulations we reveal an inherent coupling between ferroelastic twin domains and chemical segregation. Furthermore, these results reveal an interplay of ferroic properties and chemical segregation on the optoelectronic performance of hybrid organic–inorganic perovskites, and offer an exploratory path to improving functional devices.},
doi = {10.1038/s41563-018-0152-z},
journal = {Nature Materials},
number = 11,
volume = 17,
place = {United States},
year = {2018},
month = {8}
}

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