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Aqueous Synthesis of DNA-Functionalized Near-Infrared AgInS2/ZnS Core/Shell Quantum Dots

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    Functional Nanostructured Materials (including low-D carbon)

    Aqueous Synthesis of DNA-Functionalized Near-Infrared AgInS2/ZnS Core/Shell Quantum Dots
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    • Annette Delices
      Annette Delices
      Université Grenoble Alpes, CEA, CNRS, IRIG, PHELIQS, Grenoble F-38000, France
      Université Grenoble Alpes, CEA, CNRS, IRIG, SyMMES, UMR 5819, Grenoble F-38000, France
      More by Annette Delices
    • Davina Moodelly
      Davina Moodelly
      Université Grenoble Alpes, CEA, CNRS, IRIG, SyMMES, UMR 5819, Grenoble F-38000, France
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    • Charlotte Hurot
      Charlotte Hurot
      Université Grenoble Alpes, CEA, CNRS, IRIG, SyMMES, UMR 5819, Grenoble F-38000, France
      More by Charlotte Hurot
    • Yanxia Hou
      Yanxia Hou
      Université Grenoble Alpes, CEA, CNRS, IRIG, SyMMES, UMR 5819, Grenoble F-38000, France
      More by Yanxia Hou
      Orcidhttp://orcid.org/0000-0002-2991-1030
    • Wai Li Ling
      Wai Li Ling
      Université Grenoble Alpes, CEA, CNRS, IBS, Grenoble F-38000, France
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      Orcidhttp://orcid.org/0000-0002-4264-5750
    • Christine Saint-Pierre
      Christine Saint-Pierre
      Université Grenoble Alpes, CEA, CNRS, IRIG, SyMMES, UMR 5819, Grenoble F-38000, France
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    • Didier Gasparutto
      Didier Gasparutto
      Université Grenoble Alpes, CEA, CNRS, IRIG, SyMMES, UMR 5819, Grenoble F-38000, France
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    • Gilles Nogues
      Gilles Nogues
      University Grenoble Alpes, CNRS, Institut Néel, Grenoble F-38000, France
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    • Peter Reiss*
      Peter Reiss
      Université Grenoble Alpes, CEA, CNRS, IRIG, SyMMES, UMR 5819, Grenoble F-38000, France
      *Email: [email protected]
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      Orcidhttp://orcid.org/0000-0002-9563-238X
    • Kuntheak Kheng*
      Kuntheak Kheng
      Université Grenoble Alpes, CEA, CNRS, IRIG, PHELIQS, Grenoble F-38000, France
      *Email: [email protected]
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    Other Access OptionsSupporting Information (1)

    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2020, 12, 39, 44026–44038
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    https://doi.org/10.1021/acsami.0c11337
    Published August 25, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    Biocompatibility, biofunctionality, and chemical stability are essential criteria to be fulfilled by quantum dot (QD) emitters for bio-imaging and -sensing applications. In addition to these criteria, achieving efficient near-infrared (NIR) emission with nontoxic QDs remains very challenging. In this perspective, we developed water-soluble NIR-emitting AgInS2/ZnS core/shell (AIS/ZnS) QDs functionalized with DNA. The newly established aqueous route relying on a two-step hot-injection synthesis led to highly luminescent chalcopyrite-type AIS/ZnS core/shell QDs with an unprecedented photoluminescence quantum yield (PLQY) of 55% at 700 nm and a long photoluminescence (PL) decay time of 900 ns. Fast and slow hot injection of the precursors were compared for the AIS core QD synthesis, yielding a completely different behavior in terms of size, size distribution, stoichiometry, and crystal structure. The PL peak positions of both types of core QDs were 710 (fast) and 760 nm (slow injection) with PLQYs of 36 and 8%, respectively. The slow and successive incorporation of the Zn and S precursors during the subsequent shell growth step on the stronger emitting cores promoted the formation of a three-monolayer thick ZnS shell, evidenced by the increase of the average QD size from 3.0 to 4.8 nm. Bioconjugation of the AIS/ZnS QDs with hexylthiol-modified DNA was achieved during the ZnS shell growth, resulting in a grafting level of 5–6 DNA single strands per QD. The successful chemical conjugation of DNA was attested by UV–vis spectroscopy and agarose gel electrophoresis. Importantly, surface plasmon resonance imaging experiments using complementary DNA strands further corroborated the successful coupling and the stability of the AIS/ZnS-DNA QD conjugates as well as the preservation of the biological activity of the anchored DNA. The strong NIR emission and biocompatibility of these AIS/ZnS-DNA QDs provide a high potential for their use in biomedical applications.

    Copyright © 2020 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.0c11337.

    • PL decay curves of cQDs obtained from fast- and slow-injection fitted with two and three exponentials; associated time-resolved PL data of cQDs; absorption and PL spectra of cQDs and csQDs obtained from “slow injection”; PL decay curves at short times of csQDs fitted with two and three exponentials; associated time-resolved PL data of csQDs; absorption spectra of nonpurified csQD-DNA, purified csQD-DNA, and the different supernatant after each centrifugation; estimation of the cQDs and csQD-DNA concentration; estimation of the ssDNA QD concentration; and SPRi differential images for the biochip exposed to csQDs and ssDNAQD (PDF)

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    Cited By

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    This article is cited by 30 publications.

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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2020, 12, 39, 44026–44038
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.0c11337
    Published August 25, 2020
    Copyright © 2020 American Chemical Society
    Request reuse permissions

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