Stabilizing the Efficiency Beyond 20% with a Mixed Cation Perovskite Solar Cell Fabricated in Ambient Air under Controlled Humidity

Perovskite solar cells have evolved to have compatible high efficiency and stability by employing mixed cation/halide type perovskite crystals as pinhole‐free large grain absorbers. The cesium (Cs)–formamidium–methylammonium triple cation‐based perovskite device fabricated in a glove box enables reproducible high‐voltage performance. This study explores the method to reproduce stable and high power conversion efficiency (PCE) of a triple cation perovskite prepared using a one‐step solution deposition and low‐temperature annealing fully conducted in controlled ambient humidity conditions. Optimizing the perovskite grain size by Cs concentration and solution processes, a route is created to obtain highly uniform, pinhole‐free large grain perovskite films that work with reproducible PCE up to 20.8% and high preservation stability without cell encapsulation for more than 18 weeks. This study further investigates the light intensity characteristics of open‐circuit voltage (Voc) of small (5 × 5 mm2, PCE > 20%) and large (10 × 10 mm2, PCE of 18%) devices. Intensity dependence of Voc shows an ideality factor in the range of 1.7‐1.9 for both devices, implying that the triple cation perovskite involves trap‐assisted recombination loss at the hetero junction interfaces that influences Voc. Despite relatively high ideality factor, perovskite device is capable of supplying high power conversion efficiency under low light intensity (0.01 Sun) whereas maintaining Voc over 0.9 V. The reproducible high performance of a triple‐cation‐based mixed halide perovskite cell fabricated by appropriate control of crystal growth and post‐annealing under controlled relative humidity (R.H. < 25%) and in ambient air conditions is demonstrated. The device fabrication shows high yield in producing power conversion efficiencies up to 20.8% with a cell aperture size of 25 mm2.