Hybrid-Protected Perovskite Quantum Dot Films with Ultra-High Efficiency and Stability for LED Backlighting.

Abstract

All-inorganic lead halide perovskite quantum dots (PQDs) have emerged as highly promising materials for photonic and optoelectronic devices, solar cells, and photocatalysts. However, PQDs encounter instability and color separation issues because of ion diffusion. Current strategies mainly address stability in green CsPbBr3 PQDs, with limited focus on the red-mixed halide PQDs because of their inferior stability compared with green PQDs. Our study provides a new dual-protection methodology for synthesizing high-efficiency green and red mixed-halide PQD films. Red CsPb(Br0.4I0.6)3 and green CsPbBr3 PQDs are embedded with silicone resin and then incorporated with poly(methyl methacrylate) (PMMA) matrix to form red and green PQDs@silicone/PMMA films. The high photoluminescence quantum yield (PLQY) and great stability are recorded for the pure-red PQD polymer film. The ultrabright green CsPbBr3 PQDs@silicone/PMMA film was also successfully fabricated with an outstanding PLQY beyond 94%. These films exhibited enhanced stability against thermal and environmental degradation, attributed to the dense protective layer of silicone resin and PMMA matrices by the formation of Si-halide and Pb-O bonds, thereby reducing surface defects. Theoretical calculations reveal that combining silicone resin and PMMA improves Pb-O interactions, eliminating uncoordinated Pb2+ and enhancing PQD stability. Applied to white light-emitting diodes (WLEDs), these films demonstrated a broad color gamut of 143.4%, indicating their potential for efficient WLED backlighting.