Modeling and Fundamental Dynamics of Vacuum, Gas, and Antisolvent Quenching for Scalable Perovskite Processes

Abstract Hybrid perovskite photovoltaics (PVs) promise cost‐effective fabrication with large‐scale solution‐based manufacturing processes as well as high power conversion efficiencies. Almost all of today's high‐performance solution‐processed perovskite absorber films rely on so‐called quenching techniques that rapidly increase supersaturation to induce a prompt crystallization. However, to date, there are no metrics for comparing results obtained with different quenching methods. In response, the first quantitative modeling framework for gas quenching, anti‐solvent quenching, and vacuum quenching is developed herein. Based on dynamic thickness measurements in a vacuum chamber, previous works on drying dynamics, and commonly known material properties, a detailed analysis of mass transfer dynamics is performed for each quenching technique. The derived models are delivered along with an open‐source software framework that is modular and extensible. Thereby, a deep understanding of the impact of each process parameter on mass transfer dynamics is provided. Moreover, the supersaturation rate at critical concentration is proposed as a decisive benchmark of quenching effectiveness, yielding ≈ 10 −3 − 10 −1 s −1 for vacuum quenching, ≈ 10 −5 − 10 −3 s −1 for static gas quenching, ≈ 10 −2 − 10 0 s −1 for dynamic gas quenching and ≈ 10 2 s −1 for antisolvent quenching. This benchmark fosters transferability and scalability of hybrid perovskite fabrication, transforming the “art of device making” to well‐defined process engineering.