DOI: https://doi.org/10.29363/nanoge.almips.2021.002
Publication date: 23rd September 2021
Wide bandgap mixed-halide perovskites as the top absorbers in tandem solar cells typically exhibit a larger voltage deficit in contrast to their corresponding tri-iodide-based perovskites. With this work we are tackling the challenge of directly correlating the multi-stage synthesis of bromide-containing perovskites with optoelectronic properties and consequently device performance. Our results show that the incorporation of bromide occurs via a halide homogenization process where the perovskite composition transitions from an initial bromide-rich phase to the final target stoichiometry. In situ photoluminescence measurements during synthesis reveal that bromide inclusion alters the formation dynamics. By combining experiments with first-principle calculations we suggest that the formation of FAMACsPb(I0.8Br0.2)3 starts with the nucleation of a bromide-rich phase from solution during supersaturation followed by a retarded growth stage. The retarded growth stage is associated with a halide homogenization process that brings the composition of crystallized material to the target stoichiometry. This homogenization process not only changes the formation dynamics of mixed-halide perovskites but also promotes defect formation, which consequently leads to increased non-radiative recombination losses in the final perovskite film and thus, could contribute to the larger voltage deficit.
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