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Metal hybrid halide perovskite solar cells (PSCs) are very sensitive to air, and it is challenging to obtain air-processed, air-stable, and highly crystalline perovskite films. Photovoltaic performance decays dramatically due to air humidity influence with power conversion efficiency (PCE) of most air-processed PSCs < 15%. In this work, we develop a facile method to air-processed, highly crystalline (MA0.2FA0.8PbI3)1.0(CsPbBr3)0.05 perovskite films in ambient air with large grain size and low trap density based on mix-cation single crystal engineering. This method shows 75% increase in grain size and 28% decrease in trap density than conventional molecule/ion solution mixing-processed method. The large grain, low trap density, andhigh crystalline perovskite films result in high-efficient and air-stable PSCs. Consequently, the PCE increases to 36.7% from 12.56% for conventional molecule/ion solution mixing-processed devices and to 17.17% for single crystal engineering-based ones. Furthermore, benefiting from high moisture resistance of mix-cation single crystal engineering-based films, the PSC air stability has been improved significantly and 72% of the initial performance retains after 40 days of storage in ambient environment with a relative humidity of 60% at 25 °C without any encapsulation, with a 26% slower degradation rate than conventional solution-mixing method. [ABSTRACT FROM AUTHOR]

High-performance perovskite solar cell processed in ambient air is a big challenge due to the sensitivity of perovskite films to air. Many defects are generated easily at grain boundaries and in the perovskite films by conventional molecular/ion precursor solution mixing methods (i.e., solution mixing-based method), which restrict its stability in air and photovoltaic performance with most power conversion efficiency less than 15%. In this work, we develop a facile method for air-processed, highly crystalline, quasi-3D perovskite film with large grain size (over 6.6 times bigger than that from control conventional method) and improved ambient air stability by phenylethylammonium (PEA)-doped MA1−xPEAxPbI3 perovskite crystal engineering. Furthermore, benefiting from PEA+ doping and crystal engineering, the trap density decreases 50% compared with control. Consequently, with the optimal concentration of PEA doping, the power conversion efficiency increases from 15.6% for conventional solution mixing-based perovskite solar cells to 17.6% for crystal engineering-based ones with significantly improved moisture stability. The perovskite crystal engineering-based solar cells without any encapsulation retain 75% of the initial performance after 30-day storage in ambient air under a relative humidity of 50 ± 10%, and two times faster degradation rate is observed for control, conventional solution mixing-based perovskite solar cells when compared with crystal engineering-based ones. [ABSTRACT FROM AUTHOR]