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Rationally designed synthesis of bright AgInS 2 /ZnS quantum dots with emission control
Nano Research ( IF 9.5 ) Pub Date : 2020-06-19 , DOI: 10.1007/s12274-020-2876-8
José X. Soares , K. David Wegner , David S. M. Ribeiro , Armindo Melo , Ines Häusler , João L. M. Santos , Ute Resch-Genger

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.



中文翻译:

合理设计的带有发射控制的亮AgInS 2 / ZnS量子点合成

在无镉半导体量子点(QD)蓬勃发展的领域,三元I-III-VI量子点由于在水中容易合成环境友好的高质量材料,其高光致发光(PL)量子而受到越来越多的关注。在红色和近红外(NIR)区域产生的QYs及其固有的低毒性。此外,它们对氧气不敏感的长达数百纳秒的长PL寿命为利用化合物特定参数PL寿命的应用程序填补了一个空白。为了克服可重复使用的合成方法的不足,并使其能够基于设计控制其PL特性,我们评估和建模了高质量MPA封端的AgInS 2的合成/ ZnS(AIS / ZnS)QD。使用实验设计方法,系统优化的参数包括反应时间,温度,Ag:In比,S:In比,Zn:In比,MPA:In比和pH。通过为与应用相关的PL参数,最大PL波长,QY和PL寿命以及以Ag:In:Zn比例表示的元素组成开发的数学模型,为优化提供了指导。使用这些基于实验数据的模型,MPA:In和Ag:In的比率和pH值被确定为PL控制的最重要合成参数,并且可以深入了解这些参数之间的联系。随后,预测了合成具有可调发射和高QY的QD的实验条件。预测的和实验发现的PL特征之间的极好的一致性证实了我们用于合理设计具有定义PL特征的高质量AIS / ZnS QD的方法的可靠性。这种方法可以直接扩展到其他三元和四元QD以及掺杂QD。

更新日期:2020-06-19
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