Rationally designed synthesis of bright AgInS2/ZnS quantum dots with emission control
Rationally designed synthesis of bright AgInS2/ZnS quantum dots with emission control
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合理设计合成明亮的 AgInS2/ZnS 量子点并控制发射
DOI：
10.1007/s12274-020-2876-8
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发表时间：
2020
期刊：
影响因子：
9.9
通讯作者：
Resch-Genger
中科院分区：
文献类型：
--
作者：
Soares;Wegner;Ribeiro;D. S. M;Santos;J. L. M;Resch-Genger
在无镉半导体量子点（QD）的蓬勃发展领域中，三元I-III-VI QD由于易于在水中环境友好地合成高质量材料、其在红色和近红外（NIR）区域的高光致发光（PL）量子产率（QY）以及其固有的低毒性而受到越来越多的关注。此外，其氧不敏感的长PL寿命高达几百纳秒关闭的应用程序利用化合物的特定参数PL寿命的差距。为了克服缺乏可重复的合成方法，并使其PL性能的设计为基础的控制，我们评估和模拟高品质的MPA封端的AgInS 2/ZnS（AIS/ZnS）量子点的合成。使用实验设计方法，系统地改进的参数包括反应时间、温度、Ag：In比率、S：In比率、Zn：In比率、MPA：In比率和pH。优化的指导提供了数学模型开发的应用相关的PL参数，最大PL波长，QY，PL寿命，以及元素组成的Ag：In：Zn的比例。通过这些基于实验数据的模型，MPA：In和Ag：In的比例和pH值被确定为PL控制的最重要的合成参数，并且可以获得对这些参数之间的连接的洞察。在此基础上，预测了制备具有可调谐发射和高量子产率的量子点的实验条件。预测和实验发现的PL功能之间的良好协议证实了我们的方法的可靠性，为高品质的AIS/ZnS量子点的合理设计与定义的PL功能。这种方法可以直接扩展到其他三元和四元量子点和掺杂量子点。
In the blossoming field of Cd-free semiconductor quantum dots (QDs), ternary I-III-VI QDs have received increasing attention due to the ease of the environmentally friendly synthesis of high-quality materials in water, their high photoluminescence (PL) quantum yields (QYs) in the red and near infrared (NIR) region, and their inherently low toxicity. Moreover, their oxygen-insensitive long PL lifetimes of up to several hundreds of nanoseconds close a gap for applications exploiting the compound-specific parameter PL lifetime. To overcome the lack of reproducible synthetic methodologies and to enable a design-based control of their PL properties, we assessed and modelled the synthesis of high-quality MPA-capped AgInS2/ZnS (AIS/ZnS) QDs. Systematically refined parameters included reaction time, temperature, Ag:In ratio, S:In ratio, Zn:In ratio, MPA:In ratio, and pH using a design-of-experiment approach. Guidance for the optimization was provided by mathematical models developed for the application-relevant PL parameters, maximum PL wavelength, QY, and PL lifetime as well as the elemental composition in terms of Ag:In:Zn ratio. With these experimental data-based models, MPA:In and Ag:In ratios and pH values were identified as the most important synthesis parameters for PL control and an insight into the connection of these parameters could be gained. Subsequently, the experimental conditions to synthetize QDs with tunable emission and high QY were predicted. The excellent agreement between the predicted and experimentally found PL features confirmed the reliability of our methodology for the rational design of high quality AIS/ZnS QDs with defined PL features. This approach can be straightforwardly extended to other ternary and quaternary QDs and to doped QDs.