Liu Yongfeng, Shao Xiuwen, Gao Zhaoju, Xie Qingyu, Ying Yupeng, Zhu Xiaolin, Pan Zhangcheng, Yang Jinpeng, Lin Hao, Tang Xiaosheng, Chen Weiwei, Pei Wei, Tu Yusong
College of Physical Science and Technology & Microelectronics Industry Research Institute, Yangzhou University, Yangzhou, 225002, P. R. China.
College of Optoelectronic Engineering, Chongqing University, Chongqing, 400044, P. R. China.
Small. 2024 Jan;20(3):e2305664. doi: 10.1002/smll.202305664. Epub 2023 Sep 10.
Inorganic CsPbX perovskite quantum dots (PeQDs) show great potential in white light-emitting diodes (WLEDs) due to excellent optoelectronic properties, but their practical application is hampered by low photoluminescence quantum yield (PLQY) and especially poor stability. Herein, we developed an in-situ and general multidentate ligand passivation strategy that allows for CsPbX PeQDs not only near-unit PLQY, but significantly improved stability against storage, heat, and polar solvent. The enhanced optical property arises from high effectiveness of the multidentate ligand, diethylenetriaminepentaacetic acid (DTPA) with five carboxyl groups, in passivating uncoordinated Pb defects and suppressing nonradiative recombination. First-principles calculations reveal that the excellent stability is attributed to tridentate binding mode of DTPA that remarkably boosts the adsorption capacity to PeQD core. Finally, combining the green and red PeQDs with blue chip, we demonstrated highly luminous WLEDs with distinctly enhanced operation stability, a wide color gamut of 121.3% of national television system committee, standard white light of (0.33,0.33) in CIE 1931, and tunable color temperatures from warm to cold white light readily by emitters' ratio. This study provides an operando yet general approach to achieve efficient and stable PeQDs for WLEDs and accelerates their progress to commercialization.
无机CsPbX钙钛矿量子点(PeQDs)由于其优异的光电性能,在白光发光二极管(WLEDs)中显示出巨大的潜力,但其实际应用受到低光致发光量子产率(PLQY)的阻碍,尤其是稳定性较差。在此,我们开发了一种原位且通用的多齿配体钝化策略,该策略不仅能使CsPbX PeQDs具有接近单位的PLQY,还能显著提高其在储存、热和极性溶剂方面的稳定性。增强的光学性能源于具有五个羧基的多齿配体二乙烯三胺五乙酸(DTPA)在钝化未配位的Pb缺陷和抑制非辐射复合方面的高效性。第一性原理计算表明,优异的稳定性归因于DTPA的三齿结合模式,该模式显著提高了对PeQD核的吸附能力。最后,将绿色和红色PeQDs与蓝色芯片相结合,我们展示了具有明显增强的工作稳定性、121.3%的国家电视系统委员会宽色域、CIE 1931标准白光(0.33,0.33)以及通过发射体比例可轻松从暖白光调节到冷白光的色温的高发光WLEDs。这项研究提供了一种可操作且通用的方法来实现用于WLEDs的高效稳定的PeQDs,并加速其商业化进程。