Publication date: 15th December 2025
Scaling high-performance perovskite solar cells (PSCs) into large-area photovoltaic modules remains a central challenge due to difficulties in achieving uniform crystallization, suppressing defect-mediated recombination, and ensuring long-term stability. We present a seed-primed and vacuum-assisted crystallization (S-VAC) strategy that enables the fabrication of highly uniform, monolithic perovskite films over 15×15 cm2 substrates without the use of anti-solvents. Oleylamine-induced α-phase nanocrystal seeds are formed directly in solution and preserved during low-pressure vacuum processing, which accelerates solvent extraction and drives vertically aligned (100)-oriented crystal growth. In situ GIWAXS measurements reveal a rapid α-phase transition under vacuum, while solution/solid-state NMR and particle-size analysis confirm controlled nanocrystal seed formation prior to film deposition. Cross-sectional TEM and nanoscale infrared PiFM further verify monolithic grain structures, enhanced vibrational ordering, and improved lattice coherence across the film thickness.
These structural advantages translate directly into enhanced optoelectronic performance. Optimized p-i-n devices achieve a power conversion efficiency (PCE) of 23.25% for 2.5×2.5 cm2 cells, with high external quantum efficiency across 350–850 nm. Scaled mini-modules fabricated using a laser-scribed P1–P2–P3 interconnection design deliver a certified PCE of 19.1% over a 15×15 cm2 aperture, establishing a new benchmark among anti-solvent-free perovskite modules. Electrochemical impedance spectroscopy and TRPL analyses indicate reduced trap-assisted recombination and enhanced carrier lifetimes in S-VAC films, while depth-profile XPS confirms more stable Br-rich surface compositions that mitigate light-induced halide migration.
Long-term operational assessments following ISOS protocols demonstrate excellent stability. Encapsulated modules retain over 94% of their initial efficiency after 500 h of indoor light soaking and maintain stable power output for more than one year of continuous outdoor exposure. Collectively, these results establish S-VAC as a scalable, industrially compatible crystallization route for high-efficiency and durable perovskite photovoltaic module manufacturing.
J-Y. Seo was supported by the Ministry of Trade, Industry and Energy (MOTIE) and Korea Institute for Advancement of Technology (KIAT) through the International Cooperative R&D program (P0026100) and the Association of Korean Woman Scientists and Engineers (KWSE) and funded by the Ministry of Science and ICT under the legal framework of the Act on Fostering and Supporting Women Scientists and Technicians. This work was supported by Korea Electric Power Corporation (R22XO02-03, R21EA07). J.V.M, G.A., and W.L. are grateful for the support of the Swiss National Science Foundation (project 193174) and Laura Pivetau (EPFL) for support with solid-state NMR spectroscopy. This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (NRF-2021R1A2C2010179, RS-2022-00154676, RS-2024- 00436187 and RS-2024-00406152).
