Lead-free halide double perovskite, as one of the promising candidates for lead halide perovskite materials, shows great potential in light-emitting diodes (LEDs), benefiting from its environmental friendliness and high chemical stability. However, the poor regulation of the emission spectra severely limits its application range. Herein, various lanthanide ions were successfully doped in Cs2NaScCl6 double perovskite single crystals (DPSCs) to yield effective and stable emissions spanning from visible to near-infrared (NIR) regions. Notably, efficient energy transfer from the host to the dopants enables tunable emissions with good chromaticity, which is rarely reported in the field of lead-free double perovskite. Moreover, density functional theory calculations reveal that the high local electron density around the [LnCl6]3– octahedron in DPSCs plays a key role in the improvement of photoluminescence quantum yields (PLQYs). The optimal PLQYs are up to 84%, which increases around 3 times over that of the undoped sample. Finally, multicolor and NIR LEDs based on Ln3+-doped Cs2NaScCl6 DPSCs were fabricated and had different application functions. Specifically, the single-composite white LED shows adjustable coordinates and correlated color temperatures, while the NIR LED shows good night vision imaging. This work provides new inspiration for the application of efficient multifunctional LEDs based on lead-free double perovskite materials.

Lead-free double perovskite materials with efficient and stable self-trapped exciton (STE) emissions show enormous potential for next-generation solid-state lighting. However, the low-emission efficiency and difficulty of spectral regulation are two major obstacles to their application. Here, all-inorganic rare-earth-based double perovskite Cs2NaYCl6 single crystals with strong blue emissions were reported as effective hosts to accommodate lanthanide ion doping. By controlling the introduction of Tb3 + ions and efficient energy transfer from the STEs to the dopants, the emission color of Cs2NaYCl6 single crystals was flexibly modulated from blue to green. The quantum yields were also significantly improved from 10% to 78.81% by optimizing the Tb3 + ion concentration. Further, stable light-emitting diode prototypes based on Cs2NaYCl6 color conversion materials were fabricated to demonstrate the practical applications of rare-earth-based double perovskite.

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