Reply to: On the ferroelectricity of CH3NH3PbI3 perovskites

Liu, Yongtao; Collins, Liam; Proksch, Roger; Kim, Songkil; Watson, Brianna R.; Doughty, Benjamin L.; Calhoun, Tessa R.; Ahmadi, Mahshid; Ievlev, Anton; Jesse, Stephen; Retterer, Scott; Belianinov, Alex; Xiao, Kai; Huang, Jingsong; Sumpter, Bobby G.; Kalinin, Sergei V.; Hu, Bin; Ovchinnikova, Olga S.

doi:10.1038/s41563-019-0481-6

Title: Reply to: On the ferroelectricity of CH₃NH₃PbI₃ perovskites

Journal Article · Mon Sep 16 00:00:00 EDT 2019 · Nature Materials

DOI:https://doi.org/10.1038/s41563-019-0481-6· OSTI ID:1606956

^[1];

^[2]; Proksch, Roger ^[3];

^[4]; Watson, Brianna R. ^[5];

^[6];

^[5]; Ahmadi, Mahshid ^[5];

^[2];

^[7];

^[2]; Hu, Bin ^[5];

^[2]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS); Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Asylum Research, Santa Barbara, CA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS); Pusan National Univ., Busan (South Korea)
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS) and Computational Sciences and Engineering Division

First, we thank Schulz et al.¹ for their response to our Article². Schulz et al. raise a few concerns regarding the piezoresponse force microscopy (PFM) measurements and their interpretation, as well as the crystal orientation, which they claim brings into question our central conclusions. Accordingly, Schulz et al. conclude that ferroelectricity is responsible for the origin of the PFM signal. However, we do not agree with this conclusion as there is no measurable electromechanical contrast above 1 pm V^-1 and there are strong mechanical and chemical variations inside the twin domains that, in our opinion, are behind the measured PFM signal.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1606956

Journal Information:: Nature Materials, Vol. 18, Issue 10; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (14)

Differentiating Ferroelectric and Nonferroelectric Electromechanical Effects with Scanning Probe Microscopy Balke, Nina; Maksymovych, Petro; Jesse, Stephen ACS Nano, Vol. 9, Issue 6 https://doi.org/10.1021/acsnano.5b02227	journal	May 2015
Ferroelectric or non-ferroelectric: Why so many materials exhibit “ferroelectricity” on the nanoscale Vasudevan, Rama K.; Balke, Nina; Maksymovych, Peter Applied Physics Reviews, Vol. 4, Issue 2 https://doi.org/10.1063/1.4979015	journal	June 2017
Chemical nature of ferroelastic twin domains in CH3NH3PbI3 perovskite Liu, Yongtao; Collins, Liam; Proksch, Roger Nature Materials, Vol. 17, Issue 11 https://doi.org/10.1038/s41563-018-0152-z	journal	August 2018
Electrostrictive and electrostatic responses in contact mode voltage modulated scanning probe microscopies Eliseev, Eugene A.; Morozovska, Anna N.; Ievlev, Anton V. Applied Physics Letters, Vol. 104, Issue 23 https://doi.org/10.1063/1.4882861	journal	June 2014
Ferroelectricity-free lead halide perovskites Gómez, Andrés; Wang, Qiong; Goñi, Alejandro R. Energy & Environmental Science, Vol. 12, Issue 8 https://doi.org/10.1039/C9EE00884E	journal	January 2019
On the ferroelectricity of CH3NH3PbI3 perovskites Schulz, Alexander D.; Röhm, Holger; Leonhard, Tobias Nature Materials, Vol. 18, Issue 10 https://doi.org/10.1038/s41563-019-0480-7	journal	September 2019
Scanning force microscopy for the study of domain structure in ferroelectric thin films Gruverman, A. Journal of Vacuum Science & Technology B: Microelectronics and Nanometer Structures, Vol. 14, Issue 2 https://doi.org/10.1116/1.589143	journal	March 1996
Quantitative Electromechanical Atomic Force Microscopy Collins, Liam; Liu, Yongtao; Ovchinnikova, Olga S. ACS Nano, Vol. 13, Issue 7 https://doi.org/10.1021/acsnano.9b02883	journal	July 2019
Dynamic behaviour in piezoresponse force microscopy Jesse, Stephen; Baddorf, Arthur P.; Kalinin, Sergei V. Nanotechnology, Vol. 17, Issue 6 https://doi.org/10.1088/0957-4484/17/6/014	journal	February 2006
Orientation of Ferroelectric Domains and Disappearance upon Heating Methylammonium Lead Triiodide Perovskite from Tetragonal to Cubic Phase Vorpahl, Sarah M.; Giridharagopal, Rajiv; Eperon, Giles E. ACS Applied Energy Materials, Vol. 1, Issue 4 https://doi.org/10.1021/acsaem.7b00330	journal	March 2018
Electrostrictive and electrostatic responses in contact mode voltage modulated Scanning Probe Microscopies Eliseev, Eugene A.; Morozovska, Anna N.; Ievlev, Anton V. arXiv https://doi.org/10.48550/arxiv.1403.1225	text	January 2014
Ferroelectric or non-ferroelectric: why so many materials exhibit ferroelectricity on the nanoscale Vasudevan, Rama K.; Balke, Nina; Maksymovych, Peter arXiv https://doi.org/10.48550/arxiv.1701.01128	preprint	January 2017
Quantitative Electromechanical Atomic Force Microscopy Collins, Liam; Liu, Yongtao; Ovchinnikova, Olga arXiv https://doi.org/10.48550/arxiv.1904.06776	preprint	January 2019
Dynamic Behavior in Piezoresponse Force Microscopy Jesse, Stephen; Baddorf, Arthur P.; Kalinin, Sergei V. arXiv https://doi.org/10.48550/arxiv.cond-mat/0509427	text	January 2005

Cited By (4)

Ferroelectric Poling of Methylammonium Lead Iodide Thin Films Röhm, Holger; Leonhard, Tobias; Hoffmann, Michael J. Advanced Functional Materials, Vol. 30, Issue 5 https://doi.org/10.1002/adfm.201908657	journal	November 2019
Strain–Chemical Gradient and Polarization in Metal Halide Perovskites Liu, Yongtao; Ievlev, Anton V.; Collins, Liam Advanced Electronic Materials, Vol. 6, Issue 4 https://doi.org/10.1002/aelm.201901235	journal	April 2020
Imaging Metal Halide Perovskites Material and Properties at the Nanoscale Howard, John M.; Lahoti, Richa; Leite, Marina S. Advanced Energy Materials https://doi.org/10.1002/aenm.201903161	journal	December 2019
Twin domains modulate light-matter interactions in metal halide perovskites Liu, Yongtao; Li, Mingxing; Wang, Miaosheng APL Materials, Vol. 8, Issue 1 https://doi.org/10.1063/1.5127866	journal	January 2020

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Title: Reply to: On the ferroelectricity of CH3NH3PbI3 perovskites

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Title: Reply to: On the ferroelectricity of CH₃NH₃PbI₃ perovskites