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Research Article | Open Access

Rationally designed synthesis of bright AgInS2/ZnS quantum dots with emission control

José X. Soares1, K. David Wegner2, David S. M. Ribeiro1, Armindo Melo3, Ines Häusler4, João L. M. Santos1, Ute Resch-Genger2( )
LAQV-REQUIMTE, Department of Chemical Sciences, Laboratory of Applied Chemistry, Faculty of Pharmacy, University of Porto, Rua de Jorge Viterbo Ferreira, 228, Porto, 4050-313, Portugal
Federal Institute for Materials Research and Testing (BAM), Division Biophotonics, Richard-Willstaetter-Strasse 11, 12489 Berlin, Germany
LAQV-REQUIMTE, Laboratório de Bromatologia e Hidrologia, Departamento de Ciências Químicas, Faculdade de Farmácia da Universidade do Porto, Rua de Jorge Viterbo Ferreira, 228, Porto, 4050-313, Portugal
Technische Universität Berlin, Institut für Optik und Atomare Physik, Straße des 17. Juni 135, 10623 Berlin, Germany
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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.

Keywords

design of experimentphotoluminescencequantum dotsilver indium sulfidecore/shell nanoparticlemicrowave-assisted synthesis

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Nano Research
Volume 13 Issue 9,
September 2020
Pages 2438-2450
DOI: 10.1007/s12274-020-2876-8
Cite this article:
Soares JX, Wegner KD, Ribeiro DSM, et al. Rationally designed synthesis of bright AgInS2/ZnS quantum dots with emission control. Nano Research, 2020, 13(9): 2438-2450. https://doi.org/10.1007/s12274-020-2876-8
Topics:
Infrared devices Nanocrystals

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Received: 26 August 2019
Revised: 11 May 2020
Accepted: 13 May 2020
Published: 19 June 2020
© The Author(s) 2020

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