Over 20% Efficiency in Methylammonium Lead Iodide Perovskite Solar Cells with Enhanced Stability via "in Situ Solidification" of the TiO₂ Compact Layer

In methylammonium lead iodide (MAPbI₃) perovskite solar cells (PSCs), the device performance is strongly influenced by the TiO₂ electron transport layer (ETL). Typically, the ETL needs to simultaneously be thin and pinhole-free to have high transmittance and avoid shunting. In this work, we develop an "in situ solidification" process following spin coating in which the titanium-based precursor (titanium(diisopropoxide) bis(2,4-pentanedionate)) is dried under vacuum to rapidly achieve continuous TiO₂ layers. We refer to this as "gas-phase quenching". This results in thin (60 ± 10 nm), uniform, and pinhole-free TiO₂ films. The PSCs based on the gas-phase quenched TiO₂ exhibits improved power conversion efficiency, with a median value of 18.23% (champion value of 20.43%), compared to 9.03 and 14.09% for the untreated devices. Gas-phase quenching is further shown to be effective in enabling efficient charge transfer at the MAPbI₃/TiO₂ heterointerface. Furthermore, the stability of the gas-phase quenched devices is enhanced in ambient air as well as under 1 sun illumination. In addition, we achieve 12.1% efficiency in upscaled devices (1.1 cm² active area).