Efficient sub-15 nm cubic-phase core/shell upconversion nanoparticles as reporters for ensemble and single particle studies

This is the authors' abstract. We don't add key points for this paper.

Single particle imaging of upconversion nanoparticles (UCNPs) has typically been realized using hexagonal (β) phase lanthanide-doped sodium yttrium fluoride (NaYF4) materials, the upconversion luminescence (UCL) of which saturates at power densities (P) of several hundred W cm-2 under 980 nm near-infrared (NIR) excitation. Cubic (α) phase UCNPs have been mostly neglected because of their commonly observed lower UCL efficiency at comparable P in ensemble level studies. Here, we describe a set of sub-15 nm ytterbium-enriched α-NaYbF4:Er3+@CaF2 core/shell UCNPs doped with varying Er3+ concentrations (5-25%), studied over a wide P range of ∼8-105 W cm-2, which emit intense UCL even at a low P of 10 W cm-2 and also saturate at relatively low P. The highest upconversion quantum yield (ΦUC) and the highest particle brightness were obtained for an Er3+ dopant concentration of 12%, reaching the highest ΦUC of 0.77% at a saturation power density (Psat) of 110 W cm-2. These 12%Er3+-doped core/shell UCNPs were also the brightest UCNPs among this series under microscopic conditions at high P of ∼102-105 W cm-2 as demonstrated by imaging studies at the single particle level. Our results underline the potential applicability of the described sub-15 nm cubic-phase core/shell UCNPs for ensemble- and single particle-level bioimaging.