Lu Shaoyong, Fu Zhong, Li Fu, Weng Kangkang, Zhou Likuan, Zhang Lipeng, Yang Yuchen, Qiu Hengwei, Liu Dan, Qing Wenyue, Ding He, Sheng Xing, Chen Menglu, Tang Xin, Duan Lian, Liu Wenyong, Wu Longjia, Yang Yixing, Zhang Hao, Li Jinghong
Department of Chemistry, Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology, Ministry of Education, Center for BioAnalytical Chemistry, Tsinghua University, Beijing, 100084, China.
TCL Research, No. 1001 Zhongshan Park Road, Shenzhen, Guangdong, 518067, China.
Angew Chem Int Ed Engl. 2022 Jun 7;61(23):e202202633. doi: 10.1002/anie.202202633. Epub 2022 Apr 5.
Surface chemistry mediated direct optical patterning represents an emerging strategy for incorporating colloidal nanocrystals (NCs) in integrated optoelectronic platforms including displays and image sensors. However, the role of photochemistry of crosslinkers and other photoactive species in patterning remains elusive. Here we show the design of nitrene- and carbene-based photocrosslinkers can strongly affect the patterning capabilities and photophysical properties of NCs, especially quantum dots (QDs). Their role beyond physical linkers stems from structure-dictated electronic configuration, energy alignment and associated reaction kinetics and thermodynamics. Patterned QD layers with designed carbene-based crosslinkers fully preserve their photoluminescent and electroluminescent properties. Patterned light emitting diodes (QLEDs) show a maximum external quantum efficiency of ≈12 % and lifetime over 4800 h, among the highest for reported patterned QLEDs. These results would guide the rational design of photoactive species in NC patterning and create new possibilities in the monolithic integration of NCs in high-performance device platforms.
表面化学介导的直接光学图案化是一种新兴策略，用于将胶体纳米晶体（NCs）整合到包括显示器和图像传感器在内的集成光电子平台中。然而，交联剂和其他光活性物种的光化学在图案化中的作用仍然难以捉摸。在此，我们表明基于氮烯和卡宾的光交联剂的设计可强烈影响NCs，尤其是量子点（QDs）的图案化能力和光物理性质。它们作为物理连接剂之外的作用源于结构决定的电子构型、能量匹配以及相关的反应动力学和热力学。具有设计的基于卡宾的交联剂的图案化量子点层完全保留了它们的光致发光和电致发光特性。图案化发光二极管（QLEDs）显示出最高约12%的最大外量子效率和超过4800小时的寿命，在已报道的图案化QLEDs中处于最高水平。这些结果将指导NC图案化中光活性物种的合理设计，并为NCs在高性能器件平台中的单片集成创造新的可能性。
