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One of the organic components in the perovskite photo-absorber, the methylammonium cation, has been suggested to be a roadblock to the long-term operation of organic–inorganic hybrid perovskite-based solar cells. In this work we systematically explore the crystallographic and optical properties of the compositional space of mixed cation and mixed halide lead perovskites, where formamidinium (FA+) is gradually replaced by cesium (Cs+), and iodide (I−) is substituted by bromide (Br−), i.e., CsyFA1−yPb(BrxI1−x)3. Higher tolerance factors lead to more cubic structures, whereas lower tolerance factors lead to more orthorhombic structures. We find that while some correlation exists between the tolerance factor and structure, the tolerance factor does not provide a holistic understanding of whether or not a perovskite structure will fully form. By screening 26 solar cells with different compositions, our results show that Cs1/6FA5/6PbI3 delivers the highest efficiency and long-term stability among the I-rich compositions. This work sheds light on the fundamental structure–property relationships in the CsyFA1−yPb(BrxI1−x)3 compositional space, providing vital insight to the design of durable perovskite materials. Our approach provides a library of structural and optoelectronic information for this compositional space.

This review focuses on the advancements in stability of perovskite solar cells under stress from ambient moisture, high temperatures, and UV light exposure. Moisture stability has been improved by utilizing several polymeric encapsulation methods, moisture-resistant hole transport layers (HTLs), CF4 plasma treatments, and perovskite grain crosslinking. Fluorinated encapsulation methods have proven especially successful, producing cells that maintained their PCE after 75 days at 50% RH and 5 mW cm−2 of UV radiation. Temperature destabilization has been hypothesized to occur as a result of perovskite phase transitions and the HTL dopant migration to the mesoporous TiO2 surface. Temperature-sensitive perovskites have been stabilized by tuning the Goldschmidt tolerance factor and introducing thermally resistant HTLs embedded in a polymeric matrix with polycarbonate acting as an effective thermal insulating matrix. UV light instabilities have also been shown to occur due to the photocatalysis of TiO2 and the TiO2 perovskite interface. The introduction of a Sb2S3 buffer or CsBr clusters as interface modifiers can stabilize the interface of TiO2 perovskite. Herein, we aim at highlighting the main processes that prevent perovskite degradation using polymers and interfacial modifiers.