Spatial‐Uniformity–Driven Bayesian Optimization for Rapid Development of Printed Perovskite Solar Cells

Abstract Printed metal halide perovskites can enable rapid, roll‐to‐roll manufacturing of a broad class of optoelectronics—flexible solar cells and imagers among them—while promising cost and speed advantages over incumbent silicon. However, though current methods offer high throughput and patterning capabilities, perovskite films’ spatial heterogeneity remains a challenge for large‐area devices. Here, a spatial‐uniformity‐driven Bayesian optimization (BO) approach is leveraged to accelerate the development of printed perovskite solar cells and improve large‐area device performance. Using a BO surrogate model, a 6D design space of ink chemistry and printing physics is explored via extensive iterative experimentation (≈100) informed by an objective function capturing spatial photoluminescence (PL) variance. It is discovered that optimizing for uniformity drives rapid advances in photovoltaic performance, yielding ≈20% power conversion efficiency (PCE) for small area (0.134 cm ² ) devices and > 16% for large area (1 cm ² ) devices. This machine‐learning approach simultaneously enables rheological comparison of ink formulations that accelerate the leveling of Saffman‐Taylor artifacts and improve film uniformity. This showcases uniformity‐driven BO as an efficient approach for uncovering the key printing physics and mitigating spatial heterogeneity to enable device scaling beyond small cell areas.