Zhang Shuai, Yang Linxiang, Liu Gaoyu, Zhang Shengli, Shan Qingsong, Zeng Haibo
MIIT Key Laboratory of Advanced Display Materials and Devices, Institute of Optoelectronics & Nanomaterials, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
ACS Appl Mater Interfaces. 2023 Nov 1;15(43):50254-50264. doi: 10.1021/acsami.3c10642. Epub 2023 Oct 17.
I-III-VI quantum dots (QDs) and derivatives (I, III, and VI are Ag/Cu, Ga/In, and S/Se, respectively) are the ideal candidates to replace II-VI (e.g., CdSe) and perovskite QDs due to their nontoxicity, pure color, high photoluminescence quantum yield (PLQY), and full visible coverage. However, the chaotic cation alignment in multielement systems can easily lead to the formation of multiple surface vacancies, highlighted as V and V, leading to nonradiative recombination and nonequilibrium carrier distribution, which severely limit the performance improvement of materials and devices. Here, based on Zn-Ag-In-Ga-S QDs, we construct an ultrathin indium sulfide shell that can passivate electron vacancies and convert donor/acceptor level concentrations. The optimized In-rich 2-layer indium sulfide structure not only enhances the radiative recombination rate by preventing further formation but also achieves the typical DAP emission enhancement, achieving a significant increase in PLQY to 86.2% at 628 nm. Moreover, the optimized structure can mitigate the lattice distortion and make the carrier distribution in the interior of the QDs more balanced. On this basis, red QD light-emitting diodes (QLEDs) with the highest external quantum efficiency (EQE; 5.32%) to date were obtained, providing a novel scheme for improving I-III-VI QD-based QLED efficiency.
I-III-VI族量子点(QDs)及其衍生物(I、III和VI分别为Ag/Cu、Ga/In和S/Se)由于其无毒、颜色纯净、高光致发光量子产率(PLQY)以及全可见光覆盖范围,是替代II-VI族(如CdSe)和钙钛矿量子点的理想候选材料。然而,多元素体系中混乱的阳离子排列很容易导致形成多个表面空位,标记为V和V,从而导致非辐射复合和非平衡载流子分布,这严重限制了材料和器件性能的提升。在此,基于Zn-Ag-In-Ga-S量子点,我们构建了一层超薄的硫化铟壳层,它可以钝化电子空位并改变施主/受主能级浓度。优化后的富铟双层硫化铟结构不仅通过阻止进一步形成来提高辐射复合率,还实现了典型的DAP发射增强,在628nm处使PLQY显著提高到86.2%。此外,优化后的结构可以减轻晶格畸变,使量子点内部的载流子分布更加平衡。在此基础上,获得了迄今为止具有最高外量子效率(EQE;5.32%)的红色量子点发光二极管(QLED),为提高基于I-III-VI族量子点的QLED效率提供了一种新方案。