Crystallization and Orientation Modulation Enable Highly Efficient Doctor-Bladed Perovskite Solar Cells

With the rapid rise in perovskite solar cells (PSCs) performance, it is imperative to develop scalable fabrication techniques to accelerate potential commercialization. However, the power conversion efficiencies (PCEs) of PSCs fabricated via scalable two-step sequential deposition lag far behind the state-of-the-art spin-coated ones. Herein, the additive methylammonium chloride (MACl) is introduced to modulate the crystallization and orientation of a two-step sequential doctor-bladed perovskite film in ambient conditions. MACl can significantly improve perovskite film quality and increase grain size and crystallinity, thus decreasing trap density and suppressing nonradiative recombination. Meanwhile, MACl also promotes the preferred face-up orientation of the (100) plane of perovskite film, which is more conducive to the transport and collection of carriers, thereby significantly improving the fill factor. As a result, a champion PCE of 23.14% and excellent long-term stability are achieved for PSCs based on the structure of ITO/SnO₂/FA_1-xMA_xPb(I_1-yBr_y)₃/Spiro-OMeTAD/Ag. The superior PCEs of 21.20% and 17.54% are achieved for 1.03 cm² PSC and 10.93 cm² mini-module, respectively. These results represent substantial progress in large-scale two-step sequential deposition of high-performance PSCs for practical applications.