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Abstract The development of vacuum‐deposited perovskite materials and devices is partially slowed down by the minor research effort in this direction, due to the high cost of the required research tools. But there is also another factor, thermal co‐deposition in high vacuum involves the simultaneous sublimation of several precursors with an overall deposition rate in the range of few Å s−1. This leads to a deposition time of hours with only a single set of process parameters per batch, hence to a long timeframe to optimize even a single perovskite composition. Here we report the combinatorial vacuum deposition of wide bandgap perovskites using 4 sources and a non‐rotating sample holder. By using small pixel substrates, more than 100 solar cells can be produced with different perovskite absorbers in a single deposition run. The materials are characterized by spatially resolved methods, including optical, morphological, and structural techniques. By fine‐tuning of the deposition rates, the gradient can be altered and the best‐performing formulations in standard depositions with rotation can be reproduced. This is viewed as an approach that can serve as a basis to prototype other compositions, overcoming the current limitations of vacuum deposition as a research tool for perovskite films.

Herein, the long‐term stability of vacuum‐deposited methylammonium lead iodide (MAPbI3) perovskite solar cells (PSCs) with power conversion efficiencies (PCEs) of around 19% is evaluated. A low‐temperature atomic layer deposition (ALD) Al2O3 coating is developed and used to protect the MAPbI3 layers and the solar cells from environmental agents. The ALD encapsulation enables the MAPbI3 to be exposed to temperatures as high as 150 °C for several hours without change in color. It also improves the thermal stability of the solar cells, which maintain 80% of the initial PCEs after aging for ≈40 and 37 days at 65 and 85 °C, respectively. However, room‐temperature operation of the solar cells under 1 sun illumination leads to a loss of 20% of their initial PCE in 230 h. Due to the very thin ALD Al2O3 encapsulation, X‐ray diffraction can be performed on the MAPbI3 films and completed solar cells before and after the different stress conditions. Surprisingly, it is found that the main effect of light soaking and thermal stress is a crystal reorientation with respect to the substrate from (002) to (202) of the perovskite layer, and that this reorientation is accelerated under illumination.