Black phase CsPbI, naturally possessing the superiority of high radiative recombination efficiency and narrow emission line width, shows promise for commercial applications of red perovskite light-emitting diodes (PeLEDs). However, the metastable black phase CsPbI with a marginal tolerance factor () of 0.81 would easily convert to the nonoptical yellow phase. Herein, we demonstrate the strategy of partial substitution of larger dimethylammonium cation (DMA) for Cs to achieve the stable tolerance factor of 0.903 for greatly improved CsDMAPbI nanocrystals. These NCs present a superior ultraviolet (UV) irradiation stability by retaining 80% of the initial photoluminescence intensity after 5 h, which is much better than that of its counterparts (retaining 30%). Based on this, the as-developed red PeLEDs demonstrate remarkable luminance of 1258 cd/m and external quantum efficiency of 3.39%, which are almost 6 times and 3 times that of its counterparts, respectively (203 cd/m and 1.28%). This strategy may pave the way to improving the stability and efficiency of PeLEDs.
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