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Title: Re-entrant relaxor ferroelectricity of methylammonium lead iodide

Abstract

In this paper, we have performed a piezoresponse force microscopy (PFM) study on methylammonium lead iodide (MAPbI 3) thin films in normal (non-resonance, non-band-excitation) contact mode. In contrast to the ferroelectric Pb 0.76Ca 0.24TiO 3 (PCT) control sample, a typical ferroelectric response was not observed. However, a nonlinear electric field dependence of the local PFM amplitude was found in MAPbI 3, similar to PCT. An analysis combining results on structure, dielectric dispersion, and weak ferroelectricity demonstrates that MAPbI 3 is actually a re-entrant relaxor ferroelectric which, upon cooling, enters into a relaxor phase below its ferroelectric phase transition at ~327 K, due to the balance between the long range ferroelectric order and structural methylammonium group orientational disorder. The ferroelectricity at room temperature is compromised due to the re-entrant relaxor behavior, causing the poor polarization retention or weak ferroelectricity. Finally, our findings essentially conciliate the conflicting experimental results on MAPbI 3's ferroelectricity and are beneficial both for basic understanding as well as for device applications.

Authors:
 [1];  [2];  [2];  [2];  [2];  [3]
  1. Qingdao Huanghai Univ., Qingdao (China). College of Electromechanical Engineering; Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Semiconductors. Key Lab. of Semiconductor Materials Science
  2. Qingdao Huanghai Univ., Qingdao (China). College of Electromechanical Engineering
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Korea Advanced Inst. Science and Technology (KAIST), Daejeon (Korea, Republic of). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Qingdao Huanghai Univ., Qingdao (China)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Research Grants Council (RGC) of Hong Kong (China); Chinese Univ. of Hong Kong (China)
Contributing Org.:
Chinese Academy of Sciences (CAS), Beijing (China); Korea Advanced Inst. Science and Technology (KAIST), Daejeon (Korea, Republic of)
OSTI Identifier:
1352670
Alternate Identifier(s):
OSTI ID: 1358871
Grant/Contract Number:
AC02-06CH11357; T23-407/13-N; AoE/P-03/08
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Current Applied Physics
Additional Journal Information:
Journal Volume: 16; Journal Issue: 12; Journal ID: ISSN 1567-1739
Publisher:
Korean Physical Society
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Atomic force microscopy; Electronic materials; Ferroelectrics; Piezoresponse force microscopy; Relaxor

Citation Formats

Guo, Haiyan, Liu, Peixue, Zheng, Shichao, Zeng, Shixian, Liu, Na, and Hong, Seungbum. Re-entrant relaxor ferroelectricity of methylammonium lead iodide. United States: N. p., 2016. Web. doi:10.1016/j.cap.2016.09.016.
Guo, Haiyan, Liu, Peixue, Zheng, Shichao, Zeng, Shixian, Liu, Na, & Hong, Seungbum. Re-entrant relaxor ferroelectricity of methylammonium lead iodide. United States. doi:10.1016/j.cap.2016.09.016.
Guo, Haiyan, Liu, Peixue, Zheng, Shichao, Zeng, Shixian, Liu, Na, and Hong, Seungbum. Sat . "Re-entrant relaxor ferroelectricity of methylammonium lead iodide". United States. doi:10.1016/j.cap.2016.09.016. https://www.osti.gov/servlets/purl/1352670.
@article{osti_1352670,
title = {Re-entrant relaxor ferroelectricity of methylammonium lead iodide},
author = {Guo, Haiyan and Liu, Peixue and Zheng, Shichao and Zeng, Shixian and Liu, Na and Hong, Seungbum},
abstractNote = {In this paper, we have performed a piezoresponse force microscopy (PFM) study on methylammonium lead iodide (MAPbI3) thin films in normal (non-resonance, non-band-excitation) contact mode. In contrast to the ferroelectric Pb0.76Ca0.24TiO3 (PCT) control sample, a typical ferroelectric response was not observed. However, a nonlinear electric field dependence of the local PFM amplitude was found in MAPbI3, similar to PCT. An analysis combining results on structure, dielectric dispersion, and weak ferroelectricity demonstrates that MAPbI3 is actually a re-entrant relaxor ferroelectric which, upon cooling, enters into a relaxor phase below its ferroelectric phase transition at ~327 K, due to the balance between the long range ferroelectric order and structural methylammonium group orientational disorder. The ferroelectricity at room temperature is compromised due to the re-entrant relaxor behavior, causing the poor polarization retention or weak ferroelectricity. Finally, our findings essentially conciliate the conflicting experimental results on MAPbI3's ferroelectricity and are beneficial both for basic understanding as well as for device applications.},
doi = {10.1016/j.cap.2016.09.016},
journal = {Current Applied Physics},
number = 12,
volume = 16,
place = {United States},
year = {Sat Sep 24 00:00:00 EDT 2016},
month = {Sat Sep 24 00:00:00 EDT 2016}
}

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  • Cited by 1
  • Ba{sub 5}RTi{sub 3}Nb{sub 7}O{sub 30} (R = La, Nd, Sm) tungsten bronze ceramics were prepared, and the dielectric and ferroelectric properties were investigated over a broad temperature range. The relaxor nature was determined for all compositions in their permittivity curves, and a second anomaly of the dielectric loss (tan {delta}) was observed around 250 K in Ba{sub 5}NdTi{sub 3}Nb{sub 7}O{sub 30} and around 275 K in Ba{sub 5}SmTi{sub 3}Nb{sub 7}O{sub 30}. Both the maximum and remanent polarization tended to decrease and vanish at low temperatures in the ferroelectric phase for all compositions, which was referred to as the low temperaturemore » re-entrant relaxor behavior. The remanent polarization increased with decreasing temperature first and then reached the maximum value at the re-entrant temperature (T{sub r}). For Ba{sub 5}RTi{sub 3}Nb{sub 7}O{sub 30} (R = La, Nd, Sm), T{sub r} decreased with the radius of R{sup 3+} cations and the applied field amplitude.« less
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  • Here, mixed tin (Sn) and lead (Pb) based perovskite thin films have been prepared by solution processing combining methylammonium lead iodide (MAPbI 3) and formamidinium tin iodide (FASnI 3) precursors. Optical response in the form of complex dielectric function (ε = ε 1 + iε 2) spectra and absorption coefficient (α) spectra of (FASnI 3) 1-x(MAPbI 3) x based perovskite films have been extracted over a spectral range 0.74 to 5.89 eV using spectroscopic ellipsometry. Absorption band edge energy changes as a function of composition for films including FASnI 3, MAPbI 3, and mixed x = 0.20, 0.35, 0.40, andmore » 0.6 (FASnI 3) 1-x(MAPbI 3) x perovskites. (FASnI 3) 0.60(MAPbI 3) 0.4 is found to have the minimum absorption band edge energy near ~1.2 eV.« less