Abstract

The quality of perovskite light‐harvesting layer is known to be the most critical factor for the performance of perovskite solar cells (PSCs). We herein adopt a facile ambient air‐aging process (AAP, 20‐30% RH) to realize the fabrication of high‐quality Cs0.15FA0.75MA0.1PbI3 perovskite films, thereby upgrading device performance. We find that the perovskite crystallinity after AAP for 10 d is greatly intensified, with large grain size and preferred crystal orientation along (110) and (220) planes. Comparative studies on the Ag‐based devices employing the perovskite films upon exposing to different atmospheres i.e. dry N2, dry O2, N2 & H2O (20‐30% RH), and ambient air (20‐30% RH) demonstrate that H2O molecules in air rather than O2 molecules induce an effective defect‐passivation that holds the multiple functions in enhancing the quality of perovskite film, inhibiting the nonradiative recombination, prolonging the carrier lifetime and improving the energy level matching, etc. Moreover, the positive effect of H2O in ambient atmosphere on cell performance is irreversible and remains even if moisture escapes. Finally, the average PCE of device based on the AAP‐induced film is increased from 18.24±1.49 to 21.34±0.76, with the champion PCE up to 22.60%. Also, the device with AAP exhibits better moisture resistance capability. This work offers a viable AAP‐induced route for the perovskite films with superb optoelectronic properties that can be subsequently extend to the design and construction of other photovoltaic devices for practical application.This article is protected by copyright. All rights reserved.

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