Bilayer phosphine oxide modification toward efficient and large-area pure-blue perovskite quantum dot light-emitting diodes

Blue emissive halide perovskite light-emitting diodes (LEDs) are gaining increasing attention. Reducing defects in halide perovskites to improve the performance of the resulting LEDs is a main research direction, but there are limited passivation methods for achieving efficient and spectrally-stable pure-blue LEDs based on mixed-halide perovskites. In this work, double modification layers containing phosphine oxides, i.e., diphenyl[4-(triphenylsilyl)phenyl]phosphine oxide (TSPO1) and 2,7-bis(diphenylphosphoryl)-9,9'-spirobifluorene (SPPO13), are developed to passivate mixed-halide perovskite quantum dot (QD) films. The comprehensive spectroscopic and structural characterization results indicate the presence of strong interactions between TSPO1/SPPO13 and the QDs. Besides, the combination of the bilayer exhibits a synergistic hole-blocking effect, improving the charge balance of the LEDs. LEDs based on the QD/TSPO1/SPPO13 films deliver stable electroluminesence at 469 nm and present a maximum external quantum efficiency (EQE) and luminance of 4.87% and 560 cd m-2, respectively. Benefiting from the uniform QD/TSPO1/SPPO13 film over a large area, LEDs with an area of 64 mm2 show a maximum EQE of 3.91%, which represents the first efficient large-area mixed-halide perovskite LED with stable pure-blue emission. This work provides a method to improve the perovskite QDs-based film quality and optoelectronic properties, and is a step toward the fabrication of highly-efficient large-area blue perovskite LEDs.