Phase segregation in mixed-halide perovskites affects charge-carrier dynamics while preserving mobility
Phase segregation in mixed-halide perovskites affects charge-carrier dynamics while preserving mobility
Mixed halide perovskites can provide optimal bandgaps for tandem solar cells which are key to improved cost-efficiencies, but can still suffer from detrimental illumination-induced phase segregation. Here we employ optical-pump terahertz-probe spectroscopy to investigate the impact of halide segregation on the charge-carrier dynamics and transport properties of mixed halide perovskite films. We reveal that, surprisingly, halide segregation results in negligible impact to the THz charge-carrier mobilities, and that charge carriers within the I-rich phase are not strongly localised. We further demonstrate enhanced lattice anharmonicity in the segregated I-rich domains, which is likely to support ionic migration. These phonon anharmonicity effects also serve as evidence of a remarkably fast, picosecond charge funnelling into the narrow-bandgap I-rich domains. Our analysis demonstrates how minimal structural transformations during phase segregation have a dramatic effect on the charge-carrier dynamics as a result of charge funnelling. We suggest that because such enhanced recombination is radiative, performance losses may be mitigated by deployment of careful light management strategies in solar cells.
Motti, Silvia G.
17e505d8-5c5f-43e9-a5d3-370a0593e8f4
Patel, Jay B.
391ccce8-4447-4389-a03d-816ebc7c85ad
Oliver, Robert D. J.
ca304331-2963-4479-8b2f-4ec3f091e869
Snaith, Henry J.
12799605-fd5f-4333-8c8c-270e2d291015
Johnston, Michael B.
2ec1a478-9acd-44cf-89e6-be97586f5d44
Herz, Laura M.
61d69096-5062-489f-b608-685166bc48f5
29 November 2021
Motti, Silvia G.
17e505d8-5c5f-43e9-a5d3-370a0593e8f4
Patel, Jay B.
391ccce8-4447-4389-a03d-816ebc7c85ad
Oliver, Robert D. J.
ca304331-2963-4479-8b2f-4ec3f091e869
Snaith, Henry J.
12799605-fd5f-4333-8c8c-270e2d291015
Johnston, Michael B.
2ec1a478-9acd-44cf-89e6-be97586f5d44
Herz, Laura M.
61d69096-5062-489f-b608-685166bc48f5
Motti, Silvia G., Patel, Jay B., Oliver, Robert D. J., Snaith, Henry J., Johnston, Michael B. and Herz, Laura M.
(2021)
Phase segregation in mixed-halide perovskites affects charge-carrier dynamics while preserving mobility.
Nature Communications, 12, [6955].
(doi:10.1038/s41467-021-26930-4).
Abstract
Mixed halide perovskites can provide optimal bandgaps for tandem solar cells which are key to improved cost-efficiencies, but can still suffer from detrimental illumination-induced phase segregation. Here we employ optical-pump terahertz-probe spectroscopy to investigate the impact of halide segregation on the charge-carrier dynamics and transport properties of mixed halide perovskite films. We reveal that, surprisingly, halide segregation results in negligible impact to the THz charge-carrier mobilities, and that charge carriers within the I-rich phase are not strongly localised. We further demonstrate enhanced lattice anharmonicity in the segregated I-rich domains, which is likely to support ionic migration. These phonon anharmonicity effects also serve as evidence of a remarkably fast, picosecond charge funnelling into the narrow-bandgap I-rich domains. Our analysis demonstrates how minimal structural transformations during phase segregation have a dramatic effect on the charge-carrier dynamics as a result of charge funnelling. We suggest that because such enhanced recombination is radiative, performance losses may be mitigated by deployment of careful light management strategies in solar cells.
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Accepted/In Press date: 26 October 2021
e-pub ahead of print date: 29 November 2021
Published date: 29 November 2021
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Local EPrints ID: 481327
URI: http://eprints.soton.ac.uk/id/eprint/481327
ISSN: 2041-1723
PURE UUID: c65d4b93-5ab9-4170-9d44-3ab6114b2146
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Date deposited: 23 Aug 2023 16:51
Last modified: 17 Mar 2024 04:17
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Author:
Silvia G. Motti
Author:
Jay B. Patel
Author:
Robert D. J. Oliver
Author:
Henry J. Snaith
Author:
Michael B. Johnston
Author:
Laura M. Herz
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