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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
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.
2041-1723
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.
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).

Record type: Article

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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More information

Accepted/In Press date: 26 October 2021
e-pub ahead of print date: 29 November 2021
Published date: 29 November 2021

Identifiers

Local EPrints ID: 481327
URI: http://eprints.soton.ac.uk/id/eprint/481327
ISSN: 2041-1723
PURE UUID: c65d4b93-5ab9-4170-9d44-3ab6114b2146
ORCID for Silvia G. Motti: ORCID iD orcid.org/0000-0002-8088-3485

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Date deposited: 23 Aug 2023 16:51
Last modified: 17 Mar 2024 04:17

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Contributors

Author: Silvia G. Motti ORCID iD
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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