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

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 approximate to 10-3 - 10-1s-1 for vacuum quenching, approximate to 10-5 - 10-3s-1 for static gas quenching, approximate to 10-2 - 100s-1 for dynamic gas quenching and approximate to 102s-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. Perovskite photovoltaics are very popular due to their excellent properties for commercial tandem photovoltaic applications. When printing these photovoltaics, quenching processes are pivotal for fabricating high-quality absorber layers. This work presents the first open-source software for quantitative modeling of mass transfer dynamics and determination of supersaturation rates in vacuum, gas, and antisolvent quenching-enabling a reproducible and scalable perovskite fabrication. image