Abstract
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.
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Acknowledgements
The authors acknowledge fruitful discussions with Irina V. Martynenko and Lorena Dhamo from division Biophotonics. The authors thank André Gardei from the division 7.1 Building Materials (BAM) for the XRD measurements. The TEM images were carried out as part of the DFG core facility project “Berlin Electron Microscopy Network (Berlin EM Network)”. This work received financial support from the European Union (FEDER funds POCI/01/0145/FEDER/007265) and National Funds (FCT/MEC, Fundação para a Ciência e Tecnologia and Ministério da Educação e Ciência) under the Partnership Agreement PT2020 UID/QUI/50006/2013 and through the FCT PhD Programmes and by Programa Operacional Potencial Humano (POCH), specifically by the BiotechHealth Programme (Doctoral Programme on Cellular and Molecular Biotechnology Applied to Health Sciences), reference PD/00016/2012. J. X. S. thanks FCT and POPH for his PhD grant (SFRH/BD/98105/2013). K. D. W. acknowledges the European Union’s Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement No. 846764. URG gratefully acknowledges financial support by the German Research Council (DFG; grant RE1203/12-3).
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Soares, J.X., Wegner, K.D., Ribeiro, D.S.M. et al. Rationally designed synthesis of bright AgInS2/ZnS quantum dots with emission control. Nano Res. 13, 2438–2450 (2020). https://doi.org/10.1007/s12274-020-2876-8
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DOI: https://doi.org/10.1007/s12274-020-2876-8