Lanthanide-Doped CaS and SrS Luminescent Nanocrystals: A Single-Source Precursor Approach for Doping

Yiming Zhou, Freddy Rabouw, Tim van Puffelen, Cornelis Van Walree, Daniel Gamelin, Celso de Mello Donega, Andries Meijerink

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    41 Citations (Scopus)

    Abstract

    The incorporation of dopants with optical or magnetic functionalities into colloidal nanocrystals (NCs) has been a longstanding challenge for nanomaterial research. A deeper understanding of the doping kinetics will aid a better control of the doping process. In particular, alkaline-earth sulfides are an important class of host materials for a range of luminescent dopants, including transition-metal and lanthanide ions. Their nanocrystalline analogues have many potential applications. However, the lack of synthetic methodologies hampers their development. Here we introduce a single-source precursor approach that successfully leads to Ce3+- and Eu2+-doped CaS and SrS luminescent NCs with diameters of ∼10 nm and with luminescent properties similar to those of the bulk analogues. The characteristic absorption and luminescence of Ce3+ and Eu2+ depend on the local coordination and are applied to probe dopant ion internalization. We demonstrate that controlling the reactivity of the precursors is crucial for achieving effective doping. By designing the chemical structure of the dopant precursor to vary the reactivity relative to that of the host precursor, the doping efficiency can be controlled. In addition, we have applied a growth doping strategy to further improve internalization of the dopants. Finally, we demonstrate nucleation doping as an alternative method to achieve lanthanide NC doping for dopant and host precursors with strongly different reactivities. The single-source precursor approaches proposed here allow for a flexible design of synthesis strategies and have the potential to be widely applicable to the doping of colloidal chalcogenide NCs with transition-metal and lanthanide dopant ions.

    Original languageEnglish
    Pages (from-to)16533-16543
    Number of pages11
    JournalJournal of The American Chemical Society
    Volume136
    Issue number47
    DOIs
    Publication statusPublished - 26 Nov 2014

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  • Cite this

    Zhou, Y., Rabouw, F., van Puffelen, T., Van Walree, C., Gamelin, D., de Mello Donega, C., & Meijerink, A. (2014). Lanthanide-Doped CaS and SrS Luminescent Nanocrystals: A Single-Source Precursor Approach for Doping. Journal of The American Chemical Society, 136(47), 16533-16543. https://doi.org/10.1021/ja5076663