Journal of the American Chemical Society
Journal of the American Chemical Society
5 years ago

A Selective Cation Exchange Strategy for the Synthesis of Colloidal Yb3+-Doped Chalcogenide Nanocrystals with Strong Broadband Visible Absorption and Long-Lived Near-Infrared Emission

A Selective Cation Exchange Strategy for the Synthesis of Colloidal Yb3+-Doped Chalcogenide Nanocrystals with Strong Broadband Visible Absorption and Long-Lived Near-Infrared Emission
Daniel R. Gamelin, Rachel Fainblat, Younghwan Kim, Sidney E. Creutz, Michael C. De Siena
Doping lanthanide ions into colloidal semiconductor nanocrystals is a promising strategy for combining their sharp and efficient 4f–4f emission with the strong broadband absorption and low-phonon-energy crystalline environment of semiconductors to make new solution-processable spectral-conversion nanophosphors, but synthesis of this class of materials has proven extraordinarily challenging because of fundamental chemical incompatibilities between lanthanides and most intermediate-gap semiconductors. Here, we present a new strategy for accessing lanthanide-doped visible-light-absorbing semiconductor nanocrystals by demonstrating selective cation exchange to convert precursor Yb3+-doped NaInS2 nanocrystals into Yb3+-doped PbIn2S4 nanocrystals. Excitation spectra and time-resolved photoluminescence measurements confirm that Yb3+ is both incorporated within the PbIn2S4 nanocrystals and sensitized by visible-light photoexcitation of these nanocrystals. This combination of strong broadband visible absorption, sharp near-infrared emission, and long (>400 μs) emission lifetimes in a colloidal nanocrystal system opens promising new opportunities for both fundamental-science and next-generation spectral-conversion applications such as luminescent solar concentrators.

Publisher URL: http://dx.doi.org/10.1021/jacs.7b04938

DOI: 10.1021/jacs.7b04938

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