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Reversible Photo-Induced Phase Segregation and Origin of Long Carrier Lifetime in Mixed-Halide Perovskite Films

Abstract : Mixed-halide based hybrid perovskite semiconductors have attracted tremendous attention as a promising candidate for high efficient photovoltaic and light-emitting devices. However, these advanced perovskite materials may undergo phase segregation under light illumination due to halide ion migration, affecting their optoelectronic properties. Here, we report photo-excitation induced phase segregation in triple-cation mixed-halide perovskite films that yields to red-shift in photoluminescence response. We demonstrate that photo-excitation induced halide ion migration leads to the formation of smaller-bandgap iodide-rich and larger-bandgap bromide-rich domains in the perovskite film, where the phase segregation rate is found to follow the excitation power-density as a power law. Results confirm that charge carrier lifetime increases with redshift in photoluminescence due to the trapping of photo-excited carriers in the segregated smaller-bandgap iodide-rich domains. Interestingly, we found that these photo-induced changes are fully reversible and thermally activated when the excitation power is turned off. A significant difference in activation energies for halide ion migration is observed during phase segregation and recovery process under darkness. Additionally, we have investigated the emission linewidth broadening as a function of temperature which is governed by the exciton-optical phonon coupling. The mechanism of photo-induced phase segregation is interpreted based on excitonphonon coupling strength in both mixed and demixed (segregated) states of perovskite film.
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Submitted on : Monday, October 11, 2021 - 1:15:35 PM
Last modification on : Saturday, April 2, 2022 - 3:38:06 AM
Long-term archiving on: : Wednesday, January 12, 2022 - 7:44:11 PM

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Subodh K Gautam, Minjin Kim, Douglas R Miquita, Jean-Eric Bourée, Bernard Geffroy, et al.. Reversible Photo-Induced Phase Segregation and Origin of Long Carrier Lifetime in Mixed-Halide Perovskite Films. Advanced Functional Materials, Wiley, 2020, 30 (28), pp.2002622. ⟨10.1002/adfm.202002622⟩. ⟨hal-03373162⟩

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