Preventing cation intermixing enables 50% quantum yield in sub-15 nm short-wave infrared-emitting rare-earth based core-shell nanocrystals

Fernando Arteaga Cardona, Noopur Jain, Radian Popescu, Dmitry Busko, Eduard Madirov, Bernardo A. Arús, Dagmar Gerthsen, Annick Backer, Sara Bals, Oliver T. Bruns, Andriy Chmyrov (), Sandra Aert (), Bryce S. Richards () and Damien Hudry ()
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Fernando Arteaga Cardona: Karlsruhe Institute of Technology
Noopur Jain: University of Antwerp
Radian Popescu: Karlsruhe Institute of Technology
Dmitry Busko: Karlsruhe Institute of Technology
Eduard Madirov: Karlsruhe Institute of Technology
Bernardo A. Arús: Helmholtz Center Munich
Dagmar Gerthsen: Karlsruhe Institute of Technology
Annick Backer: University of Antwerp
Sara Bals: University of Antwerp
Oliver T. Bruns: Helmholtz Center Munich
Andriy Chmyrov: Helmholtz Center Munich
Sandra Aert: University of Antwerp
Bryce S. Richards: Karlsruhe Institute of Technology
Damien Hudry: Karlsruhe Institute of Technology

Nature Communications, 2023, vol. 14, issue 1, 1-14

Abstract: Abstract Short-wave infrared (SWIR) fluorescence could become the new gold standard in optical imaging for biomedical applications due to important advantages such as lack of autofluorescence, weak photon absorption by blood and tissues, and reduced photon scattering coefficient. Therefore, contrary to the visible and NIR regions, tissues become translucent in the SWIR region. Nevertheless, the lack of bright and biocompatible probes is a key challenge that must be overcome to unlock the full potential of SWIR fluorescence. Although rare-earth-based core-shell nanocrystals appeared as promising SWIR probes, they suffer from limited photoluminescence quantum yield (PLQY). The lack of control over the atomic scale organization of such complex materials is one of the main barriers limiting their optical performance. Here, the growth of either homogeneous (α-NaYF4) or heterogeneous (CaF2) shell domains on optically-active α-NaYF4:Yb:Er (with and without Ce3+ co-doping) core nanocrystals is reported. The atomic scale organization can be controlled by preventing cation intermixing only in heterogeneous core-shell nanocrystals with a dramatic impact on the PLQY. The latter reached 50% at 60 mW/cm2; one of the highest reported PLQY values for sub-15 nm nanocrystals. The most efficient nanocrystals were utilized for in vivo imaging above 1450 nm.

Date: 2023
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DOI: 10.1038/s41467-023-40031-4

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