Zhou Ding, Jing Pengtao, Wang Yi, Zhai Yuechen, Li Di, Xiong Yuan, Baranov Alexander V, Qu Songnan, Rogach Andrey L
State Key Laboratory of Luminescence and Applications, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, Changchun, 130033, P. R. China.
Nanoscale Horiz. 2019 Mar 1;4(2):388-395. doi: 10.1039/c8nh00247a. Epub 2018 Nov 13.
Aggregation-induced quenching (AIQ) of emission is an obstacle for the development of carbon dots (CDots) for solid-state luminescent devices. In this work, we introduce a method to avoid AIQ and to produce highly luminescent CDots through a space-confined vacuum heating synthesis. In the presence of CaCl, a mixture of citric acid and urea forms an inflated foam under vacuum heating at 120 °C. Upon gradually increasing the heating temperature to 250 °C, blue emissive molecular species are first formed, and are then transformed into uniform-sized green emissive CDots through dehydration and carbonization processes taking place in the confined ultrathin spaces of the foam walls. The green luminescence of these CDots originates from conjugated sp domains, and these CDots exhibit a high photoluminescence quantum yield (PLQY) of 72% in ethanol solution. Remarkably, due to the existence of only one type of recombination center in these nanoparticles, AIQ does not take place in CDot-based close-packed films, which show strong emission with a PLQY of 65%. Utilizing the differences in the emission properties of vacuum heating produced CDots, CDots synthesized through microwave-assisted heating, and commercial green fluorescent organic ink (namely, excitation-dependent vs. excitation-independent emission, and different stability against photobleaching), multilevel data encryption has been demonstrated.
发射的聚集诱导猝灭(AIQ)是固态发光器件用碳点(CDots)发展的一个障碍。在这项工作中,我们介绍了一种避免AIQ并通过空间受限的真空加热合成制备高发光性碳点的方法。在氯化钙存在下,柠檬酸和尿素的混合物在120℃真空加热下形成膨胀泡沫。随着加热温度逐渐升至250℃,首先形成蓝色发光分子物种,然后通过在泡沫壁的受限超薄空间中发生的脱水和碳化过程转化为尺寸均匀的绿色发光碳点。这些碳点的绿色发光源自共轭sp域,并且这些碳点在乙醇溶液中表现出72%的高光致发光量子产率(PLQY)。值得注意的是,由于这些纳米颗粒中仅存在一种类型的复合中心,基于碳点的紧密堆积薄膜中不会发生AIQ,其表现出强烈发射,PLQY为65%。利用真空加热制备的碳点、微波辅助加热合成的碳点以及商业绿色荧光有机墨水(即激发依赖与激发独立发射以及对光漂白的不同稳定性)的发射特性差异,已经证明了多级数据加密。