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Rapid Aqueous Spray Fabrication of Robust NiOx: A Simple and Scalable Platform for Efficient Perovskite Solar Cells

Organometal halide perovskites have powerful intrinsic potential to drive next‐generation solar technology, but their insufficient thermomechanical reliability and unproven large‐area manufacturability limit competition with incumbent silicon photovoltaics. This work addresses these limitations by leveraging large‐area processing and robust inorganic hole transport layers (HTLs). Inverted perovskite solar cells utilizing NiOx HTLs deposited by rapid aqueous spray‐coating that outperform spin‐coated NiOx and lead to a 5× improvement in the fracture energy (Gc), a primary metric of thermomechanical stability, are presented. The morphology, chemical composition, and optoelectronic properties of the NiOx films are characterized to understand and optimize compatibility with an archetypal double cation perovskite, Cs.17FA.83Pb(Br.17I.83)3. Perovskite solar cells with sprayed NiOx show higher photovoltaic performance, exhibiting up to 82% fill factor and 17.7% power conversion efficiency (PCE)—the highest PCE reported for inverted cell with scalable charge transport layers—as well as excellent stability under full illumination and after 4000 h aging in inert conditions at room temperature. By utilizing open‐air techniques and aqueous precursors, this combination of robust materials and low‐cost processing provides a platform for scaling perovskite modules with long‐term reliability.