Phase segregation in mixed-halide perovskites affects charge-carrier dynamics while preserving mobility

Silvia G. Motti, Jay B. Patel, Robert D. J. Oliver, Henry J. Snaith, Michael B. Johnston and Laura M. Herz ()
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Silvia G. Motti: University of Oxford, Clarendon Laboratory
Jay B. Patel: University of Oxford, Clarendon Laboratory
Robert D. J. Oliver: University of Oxford, Clarendon Laboratory
Henry J. Snaith: University of Oxford, Clarendon Laboratory
Michael B. Johnston: University of Oxford, Clarendon Laboratory
Laura M. Herz: University of Oxford, Clarendon Laboratory

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-021-26930-4

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