Abstract
<title>Abstract</title> <p>Ultrahigh-resolution quantum dot light-emitting diodes (QLEDs) are promising building blocks for next-generation near-eye micro-displays, yet pixel-edge electric field distortion induces an intrinsic efficiency-resolution trade-off that severely hinders their practical deployment. Tandem architectures enable prominent electroluminescence enhancement, but their implementation in high-resolution patterned QLEDs remains largely unexplored, limited by the inferior charge-generation capability and high operating voltage of conventional charge generation layers (CGLs). Herein, we demonstrate the first dual-function molecularly engineered CGL for high-resolution tandem QLEDs, realizing synergistic defect passivation and electronic band modulation of ZnO using fluorinated 4,4'-(hexafluoroisopropylidene)diphenol (BPAF). BPAF strongly coordinates with defective sites to passivate oxygen-vacancy-derived deep-level traps, while triggering spontaneous downward band bending to optimize interfacial energy alignment, thereby suppressing non-radiative recombination and lowering the interfacial charge-generation barrier. Benefiting from this dual-functional modulation, the all-solution-processed patterned QLEDs deliver a record-high external quantum efficiency of 42.82% at an ultrahigh pixel density of 10,160 PPI, fundamentally breaking the long-standing efficiency-resolution trade-off. Importantly, the high-resolution QLEDs achieve an ultra-low turn-on voltage of 2.0 V and a state-of-the-art power efficiency of 62.7 lm W-1. This work opens a universal pathway toward the design of high-performance, ultrahigh-resolution QLEDs for low-power wearable near-eye display applications.</p>