Perovskite light-emitting diodes (PeLEDs) provide excellent opportunities for low-cost, color-saturated, and large-area displays. However, the performance of blue PeLEDs lags far behind that of their green and red counterparts. Here, we show that the external quantum efficiencies (EQEs) of blue PeLEDs scale linearly with the photoluminescence quantum yields (PL QYs) of CsPb(Br x Cl
1−
x ) 3 nanocrystals emitting at 460 to 480 nm. The recombination efficiency of carriers is highly sensitive to the chlorine content and the related deep-level defects in nanocrystals, causing notable EQE drops even with minor increases in chlorine defects. Minor adjustments of chlorine content through rubidium compensation on the A-site effectively suppress the formation of nonradiative defects, improving PL QYs while retaining desirable bandgaps for blue-emitting nanocrystals. Our PeLEDs with record-high efficiencies span the blue spectrum, achieving peak EQEs of 12.0% (460 nm), 16.7% (465 nm), 21.3% (470 nm), 24.3% (475 nm), and 26.4% (480 nm). This work exemplifies chlorine-defect control as a key design principle for high-efficiency blue PeLEDs.
Organolead trihalide perovskites have attracted great attention due to the stunning advances in both photovoltaic and light-emitting devices. However, the photophysical properties, especially the recombination dynamics of photogenerated carriers, of this class of materials are controversial. Here we report that under an excitation level close to the working regime of solar cells, the recombination of photogenerated carriers in solution-processed methylammonium–lead–halide films is dominated by excitons weakly localized in band tail states. This scenario is evidenced by experiments of spectral-dependent luminescence decay, excitation density-dependent luminescence and frequency-dependent terahertz photoconductivity. The exciton localization effect is found to be general for several solution-processed hybrid perovskite films prepared by different methods. Our results provide insights into the charge transport and recombination mechanism in perovskite films and help to unravel their potential for high-performance optoelectronic devices.