Proceedings of 13th Conference on Hybrid and Organic Photovoltaics (HOPV21)
Publication date: 11th May 2021
Mixed halide perovskite semiconductors can provide optimal bandgaps for multi-junction solar cells which are key to improve cost-efficiencies. However, these materials can suffer from detrimental illumination-induced phase segregation. In this work 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. By modelling the charge-carrier dynamics and incorporating the charge funnelling, we show how although the high mobilities are preserved, the long-range transport can be hampered by the enhanced recombination rates resulting from the charge concentration. Our analysis demonstrates how minimal structural transformations during phase segregation have a dramatic effect on the charge-carrier dynamics as a result of the film heterogeneities. Given that the such an enhanced recombination is mainly radiative, we suggest that performance losses may be mitigated by deployment of careful light management strategies in solar cells.
The authors gratefully acknowledge support from the Engineering and Physical Sciences Research Council (EPSRC). L.M.H. thanks TUM-IAS for a Hans Fischer Senior Fellowship and Award. R.D.J.O. expresses his gratitude to the Penrose Scholarship for funding his studentship.
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