Power conversion efficiencies of lead halide perovskite solar cells have rapidly increased in the decade since their emergence, reaching 25% this year. However, reliable film uniformity and device stability remain hard to achieve and often require precise compliance with complicated protocols, which hampers upscaling towards industrial applications. Here, we explore the potential of an alternative route towards high-quality perovskite films: The reaction between a pre-existing perovskite film and methylamine (MA) gas has been shown to possess the striking ability to both improve film morphology and increase grain size drastically, boosting device performance. This post-deposition treatment could provide the means to decouple film quality from the initial deposition process, thus promising to facilitate upscaling and lowering production costs. Furthermore, such MA gas treatments show great promise regarding the stability of fabricated devices, as they open up the opportunity to reduce or even eliminate the adverse role of grain boundaries in film degradation.
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Considerable efforts have been devoted to optimizing and controlling the morphology and electronic properties of lead halide perovskites. The defect density of a perovskite layer strongly depends on the processing conditions. Consequently, the fabrication process of high-quality films is often complex, and reproducibility is a challenge. In this work, we present a methylamine gas-based method to recrystallize perovskite layers of any given quality in a controlled way, leading to millimeter-sized domains. Crystallinity significantly increases upon methylamine treatment, and crystal growth follows a preferred orientation. Photoluminescence- and space-charge limited current measurements show that the trap density halves after recrystallization. Conductive atomic force microscopy measurements show a higher surface conductivity and an improved spatial homogeneity after methylamine treatment. When applied in photodetectors, the improved film quality of the recrystallized films leads to increased detectivities of ≈4 × 1011 Jones compared to 3 × 109 Jones of a reference device. The response time falls from 0.1 to 10−5 s upon methylamine treatment. Our work, thus, presents a promising route to fabricating reproducible, high-quality perovskite films through well-controllable recrystallization.
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