We report herein the discovery of methylamine (CH3NH2) induced defect-healing (MIDH) of CH3NH3PbI3 perovskite thin films based on their ultrafast (seconds), reversible chemical reaction with CH3NH2 gas at room temperature. The key to this healing behavior is the formation and spreading of an intermediate CH3NH3PbI3⋅xCH3NH2 liquid phase during this unusual perovskite-gas interaction. We demonstrate the versatility and scalability of the MIDH process, and show dramatic enhancement in the performance of perovskite solar cells (PSCs) with MIDH. This study represents a new direction in the formation of defect-free films of hybrid perovskites.

Solution-processed perovskite (PSC) solar cells have achieved extremely high power conversion efficiencies (PCEs) over 20%, but practical application of this photovoltaic technology requires further advancements on both long-term stability and large-area device demonstration. Here, an additive-engineering strategy is developed to realize a facile and convenient fabrication method of large-area uniform perovskite films composed of large crystal size and low density of defects. The high crystalline quality of the perovskite is found to simultaneously enhance the PCE and the durability of PSCs. By using the simple and widely used methylammonium lead iodide (MAPbI ), a certified PCE of 19.19% is achieved for devices with an aperture area of 1.025 cm , and the high-performing devices can sustain over 80% of the initial PCE after 500 h of thermal aging at 85 °C, which are among the best results of MAPbI -based PSCs so far.

Perovskite solar cells (PSCs) emerging as a promising photovoltaic technology with high efficiency and low manufacturing cost have attracted the attention from all over the world. Both the efficiency and stability of PSCs have increased steadily in recent years, and the research on reducing lead leakage and developing eco-friendly lead-free perovskites pushes forward the commercialization of PSCs step by step. This review summarizes the main progress of PSCs in 2020 and 2021 from the aspects of efficiency, stability, perovskite-based tandem devices, and lead-free PSCs. Moreover, a brief discussion on the development of PSC modules and its challenges toward practical application is provided.

We demonstrate the feasibility of a nonsalt-based precursor pair--inorganic HPbI3 solid and organic CH3NH2 gas--for the deposition of uniform CH3NH3PbI3 perovskite thin films. The strong room-temperature solid-gas interaction between HPbI3 and CH3NH2 induces transformative evolution of ultrasmooth, full-coverage perovskite thin films at a rapid rate (in seconds) from nominally processed rough, partial-coverage HPbI3 thin films. The chemical origin of this behavior is elucidated via in situ experiments. Perovskite solar cells, fabricated using MAPbI3 thin films thus deposited, deliver power conversion efficiencies up to 18.2%, attesting to the high quality of the perovskite thin films deposited using this transformative process.