Pulsed Laser Deposited CsPbBr ₃ Perovskite Solar Cells Achieving 10.71% Efficiency With Exceptional Long‐Term Stability via Target Engineering

ABSTRACT All‐inorganic perovskite CsPbBr ₃ has emerged as a promising candidate for stable and cost‐effective photovoltaic applications. Pulsed laser deposition (PLD), as a solvent‐free, material‐efficient, and highly controllable thin‐film growth technique, holds tremendous promise for the fabrication of photovoltaic devices. However, during the deposition process, the loose structure, poor thermal conductivity, and microstructural defects of conventional CsPbBr ₃ targets give rise to the generation of large neutral particles in the ablation plume, deteriorating film quality, and consequently limit device performance. In this work, these bottlenecks are addressed by introducing melt‐quenched CsPbBr ₃ targets to replace conventional powder‐pressed ones. Comprehensive analyses reveal that the emission of large neutral particles from the melt‐quenched targets and the kinetic energy of species in the ablation plume are both suppressed during deposition, which mitigates the formation of deep‐level defects, improves the quality of the thin films, and precludes band misalignment caused by surface dipoles. Ultimately, perovskite solar cells (PSCs) fabricated with the aforementioned target engineering achieve a maximum power conversion efficiency (PCE) of 10.71% and retaining a 93% of initial PCE over 150 days under ambient conditions without any encapsulation. This work presenting a compelling route toward large‐area, inline manufacturing and large‐scale commercialization for CsPbBr ₃ PSCs.