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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 segrega...

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Autores principales: Motti, Silvia G., Patel, Jay B., Oliver, Robert D. J., Snaith, Henry J., Johnston, Michael B., Herz, Laura M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8630172/
https://www.ncbi.nlm.nih.gov/pubmed/34845219
http://dx.doi.org/10.1038/s41467-021-26930-4
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author Motti, Silvia G.
Patel, Jay B.
Oliver, Robert D. J.
Snaith, Henry J.
Johnston, Michael B.
Herz, Laura M.
author_facet Motti, Silvia G.
Patel, Jay B.
Oliver, Robert D. J.
Snaith, Henry J.
Johnston, Michael B.
Herz, Laura M.
author_sort Motti, Silvia G.
collection PubMed
description 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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spelling pubmed-86301722021-12-01 Phase segregation in mixed-halide perovskites affects charge-carrier dynamics while preserving mobility Motti, Silvia G. Patel, Jay B. Oliver, Robert D. J. Snaith, Henry J. Johnston, Michael B. Herz, Laura M. Nat Commun Article 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. Nature Publishing Group UK 2021-11-29 /pmc/articles/PMC8630172/ /pubmed/34845219 http://dx.doi.org/10.1038/s41467-021-26930-4 Text en © The Author(s) 2021 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Motti, Silvia G.
Patel, Jay B.
Oliver, Robert D. J.
Snaith, Henry J.
Johnston, Michael B.
Herz, Laura M.
Phase segregation in mixed-halide perovskites affects charge-carrier dynamics while preserving mobility
title Phase segregation in mixed-halide perovskites affects charge-carrier dynamics while preserving mobility
title_full Phase segregation in mixed-halide perovskites affects charge-carrier dynamics while preserving mobility
title_fullStr Phase segregation in mixed-halide perovskites affects charge-carrier dynamics while preserving mobility
title_full_unstemmed Phase segregation in mixed-halide perovskites affects charge-carrier dynamics while preserving mobility
title_short Phase segregation in mixed-halide perovskites affects charge-carrier dynamics while preserving mobility
title_sort phase segregation in mixed-halide perovskites affects charge-carrier dynamics while preserving mobility
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8630172/
https://www.ncbi.nlm.nih.gov/pubmed/34845219
http://dx.doi.org/10.1038/s41467-021-26930-4
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