Vapor deposition of halide perovskites presents high potential for scalability and industrial processing of perovskite solar cells. It prevents the use of toxic solvents, allows thickness control, and yields conformal and uniform coating over large areas. However, the distinct volatility of the perovskite organic and inorganic components currently requires the use of multiple thermal sources or two‐step deposition to achieve the perovskite phase. In this work, single‐source, single‐step MA1–xFAxPbI3 thin film deposition with tunable stoichiometry by pulsed laser deposition is demostrated. By controlling the laser ablation of a solid target containing adjustable MAI:FAI:PbI2 ratios, the room temperature formation of cubic α‐phase MA1–xFAxPbI3 thin films is demonstrated. The target‐to‐film transfer of the ablated species, including the integrity of the organic molecules and the desired MA+:FA+ ratio, is confirmed by x‐ray photoelectron spectroscopy and solid‐state NMR. Photoluminescence analysis further confirms the shift of the bandgap with varying the MA+:FA+ ratio. Finally, proof‐of‐concept n‐i‐p solar cells with 14% efficiency are demonstrated with as‐deposited non‐passivated pulsed laser deposition (PLD)‐MA1–xFAxPbI3. This study opens the path for future developments in industry‐compatible vapor‐deposition methods for perovskite solar cells.

As the employment of halide perovskite films in single-junction and tandem solar cells continues to soar, there is a strong drive -from academia to industry-to produce these films using dry processes, avoiding the use of toxic solvents. Vapor deposition methods such as co-evaporation have shown advantages of solvent-free approaches to produce high-efficiency solar cells. However, co-evaporation requires the use of multiple sources that challenge the deposition rate control of complex halide perovskite compositions. Here, Pulsed Laser Deposition (PLD) is proposed as an alternative method to deposit hybrid halide perovskites films from a single-source and following a fully dry approach. We use the archetypical methylammonium lead iodide (MAPbI3) to demonstrate the formation of high-quality films with optimal optoelectronic properties by PLD on various substrates for single-junction and tandem devices. Furthermore, the important role of the PLD target composition and deposition parameters to achieve control over film microstructure and optoelectronic properties is discussed. The controlled conformal growth provided by PLD demonstrated in this work with MAPbI3 on device-relevant substrates will broaden opportunities to explore PLD of more complex hybrid halide perovskite compositions for efficient, stable, and scalable solar cell devices.