Tunable Polaron Distortions Control the Extent of Halide Demixing in Lead Halide Perovskites
Abstract
Photoinduced phase separation in mixed halide perovskites emerges from their electro-mechanical properties and high ionic conductivities, resulting in photoinduced I$^-$ rich charge carrier traps that diminish photovoltaic performance. Whether photoinduced phase separation stems from the polycrystalline microstructure or is an intrinsic material property has been an open question. We investigate the nanoscale photoinduced behavior of single-crystal mixed Br$^-$/I$^-$ methylammonium (MA+) lead halide perovskite (MAPb(BrxI1- x)3) nanoplates, eliminating effects from extended structural defects. Even in these nanoplates, we find that phase separation occurs, resulting in I$^-$rich clusters that are nucleated stochastically and stabilized by polarons. Upon lowering the electron-phonon coupling strength by partially exchanging MA+ for Cs+, a phase-separated steady state is not reached, nevertheless transient I$^-$ clustering still occurs. Our results, supported by multiscale modeling, demonstrate that photoinduced phase separation is an intrinsic property of mixed halide perovskites, the extent and dynamics of which depends on the electron-phonon coupling strength.
- Authors:
-
- Univ. of California, Berkeley, CA (United States)
- Univ. of California, Berkeley, CA (United States). Kavli Energy NanoScience Inst.; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1601185
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry Letters
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 14; Journal ID: ISSN 1948-7185
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Phase separation; Inorganic compounds; Cluster chemistry; Perovskites; Halogens
Citation Formats
Bischak, Connor G., Wong, Andrew B., Lin, Elbert, Limmer, David T., Yang, Peidong, and Ginsberg, Naomi S. Tunable Polaron Distortions Control the Extent of Halide Demixing in Lead Halide Perovskites. United States: N. p., 2018.
Web. doi:10.1021/acs.jpclett.8b01512.
Bischak, Connor G., Wong, Andrew B., Lin, Elbert, Limmer, David T., Yang, Peidong, & Ginsberg, Naomi S. Tunable Polaron Distortions Control the Extent of Halide Demixing in Lead Halide Perovskites. United States. https://doi.org/10.1021/acs.jpclett.8b01512
Bischak, Connor G., Wong, Andrew B., Lin, Elbert, Limmer, David T., Yang, Peidong, and Ginsberg, Naomi S. Fri .
"Tunable Polaron Distortions Control the Extent of Halide Demixing in Lead Halide Perovskites". United States. https://doi.org/10.1021/acs.jpclett.8b01512. https://www.osti.gov/servlets/purl/1601185.
@article{osti_1601185,
title = {Tunable Polaron Distortions Control the Extent of Halide Demixing in Lead Halide Perovskites},
author = {Bischak, Connor G. and Wong, Andrew B. and Lin, Elbert and Limmer, David T. and Yang, Peidong and Ginsberg, Naomi S.},
abstractNote = {Photoinduced phase separation in mixed halide perovskites emerges from their electro-mechanical properties and high ionic conductivities, resulting in photoinduced I$^-$ rich charge carrier traps that diminish photovoltaic performance. Whether photoinduced phase separation stems from the polycrystalline microstructure or is an intrinsic material property has been an open question. We investigate the nanoscale photoinduced behavior of single-crystal mixed Br$^-$/I$^-$ methylammonium (MA+) lead halide perovskite (MAPb(BrxI1- x)3) nanoplates, eliminating effects from extended structural defects. Even in these nanoplates, we find that phase separation occurs, resulting in I$^-$rich clusters that are nucleated stochastically and stabilized by polarons. Upon lowering the electron-phonon coupling strength by partially exchanging MA+ for Cs+, a phase-separated steady state is not reached, nevertheless transient I$^-$ clustering still occurs. Our results, supported by multiscale modeling, demonstrate that photoinduced phase separation is an intrinsic property of mixed halide perovskites, the extent and dynamics of which depends on the electron-phonon coupling strength.},
doi = {10.1021/acs.jpclett.8b01512},
journal = {Journal of Physical Chemistry Letters},
number = 14,
volume = 9,
place = {United States},
year = {Fri Jul 06 00:00:00 EDT 2018},
month = {Fri Jul 06 00:00:00 EDT 2018}
}
Web of Science
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