Novel Lewis Base Cyclam Self-Passivation of Perovskites without an Anti-Solvent Process for Efficient Light-Emitting...

Metal halide perovskites have been focused as a candidate applied as a promising luminescent material for next-generation high-quality lighting and high-definition display. However, as perovskite films formed, high density of defects would be produced in solution processing inevitably, leading to low exciton recombination efficiency in light-emitting diodes (LEDs). Herein, a facile and novel self-passivation strategy to inhibit defect formation in perovskite films for constructing high-performance LEDs is developed. For the first time, we introduce 1,4,8,11-tetraazacyclotetradecane (cyclam) in perovskite precursor solution, and it spontaneously passivates defect states of CsPbBr₃-based perovskites by coaction between amine and uncoordinated lead ions during spin-coating without an anti-solvent process. Furthermore, as a delocalized system, cyclam also possesses chemical properties that facilitate exciton transportation. The proposed passivation strategy boosts the external quantum efficiency from 1.25% (control device) to 16.24% (cyclam-passivated device). Furthermore, defect passivation is also conductive to reduce LED degradation paths and improve device stability as the extrapolated lifetime (T₅₀) of LEDs at an initial brightness of 100 cd/m² is increased from 0.9 to 127 h. These findings indicate that the introduction of cyclam is highly effective to enhance the performance of LEDs, and such a strategy in effectively reducing the defects could be also applied in other perovskite-based devices, such as lasers, solar cells, and photodetectors.