Interface-regulated vapour crystallization for ultrapure perovskite LEDs

Achieving ultranarrow spectral linewidth and broad spectral tunability in light-emitting diodes (LEDs) remains challenging due to linewidth broadening from compositional and size heterogeneities. Here we report an interface-regulated vapour crystallization strategy that enables precise control over the spectral linewidth of solution-processed halide perovskite thin films. Underlying materials that exhibit minimal molecular interactions with perovskite precursors, exemplified by poly(9-vinylcarbazole), facilitate smooth ion diffusion and crystallization assisted by dimethylformamide vapour. This mechanism leads to perovskite films with both horizontal and vertical homogeneity and low inhomogeneous broadening comparable to that of perovskite single crystals. We demonstrate perovskite films with ultranarrow photoluminescence linewidths of 13.6 nm, 13.7 nm, 13.8 nm and 14.4 nm for emissions at 464 nm, 474 nm, 483 nm and 522 nm, respectively. This enables us to achieve sky-blue perovskite LEDs with narrow electroluminescence linewidths of 14.7 nm and a peak external quantum efficiency of 24.6%, with comparable linewidths and performance in LEDs spanning the pure blue to pure green. This work offers a practical and scalable strategy to realize narrow spectral linewidth, broad spectral tunability and high performance in thin film LEDs. (Figure presented.)