Polar Fluctuations in Metal Halide Perovskites Uncovered by Acoustic Phonon Anomalies
Abstract
Solution-processable metal-halide perovskites (MHPs) offer great promise for efficient light harvesting and emitting devices due to their long carrier lifetime and superior carrier transport characteristics. Ferroelectric effects, a hallmark of traditional oxide perovskites, was proposed to be a mechanism to suppress carrier recombination and enhance charge transport in MHPs, but the existence and influence of such polar order is still of considerable debate. Here we performed transient reflection measurements on single crystals of both inorganic and organic-inorganic (hybrid) MHPs over a range of temperatures, and demonstrate significant phonon softening in the cubic phases close to the cubic-to-tetragonal phase transition temperatures. Such phonon softening indicates the formation of polar domains, which grow in size upon cooling and can persist in the low-temperature tetragonal and orthorhombic phases. Our results link the extraordinary electronic properties of MHPs to the spontaneous polarizations which can contribute to more efficient charge separation and characteristics of an indirect bandgap.
- Authors:
-
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Northern Illinois Univ., DeKalb, IL (United States)
- Northwestern Univ., Evanston, IL (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States); Northwestern Univ., Evanston, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Scientific User Facilities Division
- OSTI Identifier:
- 1402074
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- ACS Energy Letters
- Additional Journal Information:
- Journal Volume: 2; Journal Issue: 10; Journal ID: ISSN 2380-8195
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
Citation Formats
Guo, Peijun, Xia, Yi, Gong, Jue, Stoumpos, Constantinos C., McCall, Kyle M., Alexander, Grant C. B., Ma, Zhiyuan, Zhou, Hua, Gosztola, David J., Ketterson, John B., Kanatzidis, Mercouri G., Xu, Tao, Chan, Maria K. Y., and Schaller, Richard D. Polar Fluctuations in Metal Halide Perovskites Uncovered by Acoustic Phonon Anomalies. United States: N. p., 2017.
Web. doi:10.1021/acsenergylett.7b00790.
Guo, Peijun, Xia, Yi, Gong, Jue, Stoumpos, Constantinos C., McCall, Kyle M., Alexander, Grant C. B., Ma, Zhiyuan, Zhou, Hua, Gosztola, David J., Ketterson, John B., Kanatzidis, Mercouri G., Xu, Tao, Chan, Maria K. Y., & Schaller, Richard D. Polar Fluctuations in Metal Halide Perovskites Uncovered by Acoustic Phonon Anomalies. United States. https://doi.org/10.1021/acsenergylett.7b00790
Guo, Peijun, Xia, Yi, Gong, Jue, Stoumpos, Constantinos C., McCall, Kyle M., Alexander, Grant C. B., Ma, Zhiyuan, Zhou, Hua, Gosztola, David J., Ketterson, John B., Kanatzidis, Mercouri G., Xu, Tao, Chan, Maria K. Y., and Schaller, Richard D. 2017.
"Polar Fluctuations in Metal Halide Perovskites Uncovered by Acoustic Phonon Anomalies". United States. https://doi.org/10.1021/acsenergylett.7b00790. https://www.osti.gov/servlets/purl/1402074.
@article{osti_1402074,
title = {Polar Fluctuations in Metal Halide Perovskites Uncovered by Acoustic Phonon Anomalies},
author = {Guo, Peijun and Xia, Yi and Gong, Jue and Stoumpos, Constantinos C. and McCall, Kyle M. and Alexander, Grant C. B. and Ma, Zhiyuan and Zhou, Hua and Gosztola, David J. and Ketterson, John B. and Kanatzidis, Mercouri G. and Xu, Tao and Chan, Maria K. Y. and Schaller, Richard D.},
abstractNote = {Solution-processable metal-halide perovskites (MHPs) offer great promise for efficient light harvesting and emitting devices due to their long carrier lifetime and superior carrier transport characteristics. Ferroelectric effects, a hallmark of traditional oxide perovskites, was proposed to be a mechanism to suppress carrier recombination and enhance charge transport in MHPs, but the existence and influence of such polar order is still of considerable debate. Here we performed transient reflection measurements on single crystals of both inorganic and organic-inorganic (hybrid) MHPs over a range of temperatures, and demonstrate significant phonon softening in the cubic phases close to the cubic-to-tetragonal phase transition temperatures. Such phonon softening indicates the formation of polar domains, which grow in size upon cooling and can persist in the low-temperature tetragonal and orthorhombic phases. Our results link the extraordinary electronic properties of MHPs to the spontaneous polarizations which can contribute to more efficient charge separation and characteristics of an indirect bandgap.},
doi = {10.1021/acsenergylett.7b00790},
url = {https://www.osti.gov/biblio/1402074},
journal = {ACS Energy Letters},
issn = {2380-8195},
number = 10,
volume = 2,
place = {United States},
year = {Thu Sep 28 00:00:00 EDT 2017},
month = {Thu Sep 28 00:00:00 EDT 2017}
}
Web of Science
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