摘要
Halide Perovskite light emitting diodes (LEDs) have attracted enormous attention due to their remarkable optoelectronic properties, facile bandgap tunability and low-cost. Here, we successfully synthesized the centimeter-sized pure non-emissive Cs 4 PbBr 6 , hybrid green-emitting Cs 4 PbBr 6 @CsPbBr 3 (H-Cs 4 PbBr 6 ) and ligand-induced H-Cs 4 PbBr 6 single crystals (SCs) via the precision-temperature-gradient crystallization method. The detailed formation process of H-Cs 4 PbBr 6 was detected by a real-time optical photograph and ultraviolet lamp during different growth stages ranged from colorless transparent to bright green. Notably, the H-Cs 4 PbBr 6 SC shows the behavior of excellent luminous properties (PLQY = 92 %) owing to the higher exciton binding energy, which is estimated to be ∼439.8 meV. The unusual intense green photoluminescence mechanism is evidenced by the various measurements, which can be attributed to the embedded CsPbBr 3 nanocrystals. Interestingly, the excellent long-term stabilities of as-prepared H-Cs 4 PbBr 6 SC against heat, and environment oxygen/moisture degradation are reported, which maintains high fluorescence brightness for 3 years in air, and then for more than 4 days under 80 °C and 80 % relative humidity without additional encapsulation. A larger activation energy of 461.1 meV exhibits the better thermal stability. Furthermore, an adjustment of the PL emission of H-Cs 4 PbBr 6 SCs is first achieved with the addition of ligands. Ultrapure green LED fabricated with the whole large Cs 4 PbBr 6 SC exhibits wonderful performance with luminous efficiency of 20.50 lm·W −1 , excellent color purity of ∼90.7 % and external quantum efficiency of 5.43 %, which demonstrate the immense potential and great prospect of H-Cs 4 PbBr 6 perovskite composites to replace conventional phosphors in lighting devices.
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