Publication date: 5th November 2025
Organo–lead iodide perovskites (PVSKs) have attracted extensive attention owing to their tunable optoelectronic properties, facile fabrication, and low cost. However, incomplete conversion of PbI₂ precursors remains a persistent issue in solution-processed PVSK films, leading to undesirable PbI₂ residues that compromise long-term device stability. In this work, we present a novel precursor engineering strategy in which pre-synthesized MAPbI₃ single-crystal powders are dissolved into conventional coating solvents to form a stoichiometrically balanced precursor solution. This single-crystal-derived approach effectively eliminates residual PbI₂, producing PbI2-free, morphologically uniform and chemically homogeneous MAPbI₃ films with low defect densities. Devices fabricated from these films exhibit a champion power conversion efficiency (PCE) of 21.01%, while 5 × 5 cm² mini-modules achieve 19.8% under AM 1.5G illumination and 39.7% under indoor LED light. In comparison, conventional precursor-based devices deliver lower PCEs of 18.61% (cell) and 17.2% (mini-module) under AM 1.5G illumination, and 34.5% under LED light. Furthermore, single-crystal-derived devices retain 99% of their initial efficiency after 1000 hours of operation in ambient dry-room conditions without encapsulation, whereas conventional devices show significant degradation.
Beyond pure MAPbI₃, this strategy also enables convenient preparation of mixed-halide perovskite films by simply combining different PVSK single-crystal powders in designed proportions. The resulting films remain PbI₂-free and exhibit superior halide uniformity compared with those derived from conventional precursor methods. Consequently, single-crystal-derived mixed-halide PVSK films effectively suppress photoinduced I/Br segregation, leading to enhanced optoelectronic stability and improved device performance.
This project has received funding from the Ministry of Science and Technology, Taiwan (108-2221-E-007-102-MY3) and (112-2222-E-011-002-MY3), the Ministry of Economic Affairs, Taiwan (E111-EC-17-A-08-S6-013), and a grant from National Tsing-Hua University (111B0124J2).
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