A stable and efficient carrier transfer is a prerequisite for high-performance perovskite solar cells. With optimized additives, a significantly improved charge carrier transfer can be achieved at the interface of perovskite/2,2',7,7'-tetrakis-(,-di-4-methoxyphenylamino)-9,90-spirobifluorene (Spiro-OMeTAD) with significantly boosted photostability. Using time-dependent spectroscopic techniques, we investigated charge carrier and mobile-ion dynamics at the perovskite/Spiro-OMeTAD interface, where the Spiro-OMeTAD contains different bis(trifluoromethanesulfonyl)imide (TFSI) salts additives (Li-TFSI, Mg-TFSI, Ca-TFSI). The pristine response and the dynamic changes under continuous illuminations are presented, which is correlated to the different behaviors of mobile-ion accumulations at the perovskite/Spiro interface and ascribed to the improved hole mobilities in Spiro-OMeTAD, ultimately contributing to the favorable behaviors in solar cells. It is demonstrated that the hole mobility and conductivity of hole transport layers play an important role in suppressing mobile-ion accumulation at the interfaces of solar cells. With the engineering of mixed-cation mixed-halide perovskite, optimal engineering of additives in hole transport materials is an efficient strategy. Therefore, it should be emphasized for accelerating perovskite photovoltaic commercialization.
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