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Multifunctional Phosphorusa??Containing Lewis Acid and Base Passivation Enabling Efficient and Moisturea??Stable Perovskite Solar Cells
摘要： Multiple-cation lead mixed-halide perovskites (MLMPs) have been recognized as ideal candidates in perovskite solar cells in terms of high efficiency and stability due to decreased open-circuit voltage loss and suppressed yellow phase formation. However, they still suffer from an unsatisfactory long-term moisture stability. In this study, phosphorus-containing Lewis acid and base molecules are employed to improve device efficiency and stability based on their multifunction including recombination reduction, phase segregation suppression, and moisture resistance. The strong fluorine-containing Lewis acid treatment can achieve a champion PCE of 22.02%. Unencapsulated and encapsulated devices retain 63% and 80% of the initial efficiency after 14 days of aging under 75% and 85% relative humidity, respectively. The better passivation of Lewis acid implies more halide defects than Pb defects at the MLMP surface. This unbalanced defect type results from phase segregation that is the synergistic effect of Cs and halide ion migrations. Identifying defect type based on different passivation effects is beneficial to not only choose suitable passivators to boost the efficiency and slow down the moisture degradation of MLMP solar cells, but also to understand the mechanism of defect-assisted moisture degradation.
关键词： lewis acids,trap passivation,moisture stable solar cells,multiple-cation lead mixed-halide perovskites,phase segregation,lewis bases
更新于2025-09-23 15:19:57
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Electronic Traps and Phase Segregation in Lead Mixed-Halide Perovskite
摘要： An understanding of the factors driving halide segregation in lead mixed-halide perovskites is required for their implementation in tandem solar cells with existing silicon technology. Here we report that the halide segregation dynamics observed in the photoluminescence from CH3NH3Pb(Br0.5I0.5)3 is strongly influenced by the atmospheric environment, and that encapsulation of films with a layer of poly(methyl methacrylate) allows for halide segregation dynamics to be fully reversible and repeatable. We further establish an empirical model directly linking the amount of halide segregation observed in the photoluminescence to the fraction of charge-carriers recombining through trap-mediated channels, and the photon flux absorbed. From such quantitative analysis we show that under pulsed illumination, the frequency of the modulation alone has no influence on the segregation dynamics. Additionally, we extrapolate that working CH3NH3Pb(Br0.5I0.5)3 perovskite cells would require a reduction of the trap-related charge-carrier recombination rate to (cid:46) 105 s?1 in order for halide segregation to be sufficiently suppressed.
关键词： photoluminescence,lead mixed-halide perovskites,halide segregation,charge-carrier dynamics,trap-mediated recombination
更新于2025-09-09 09:28:46