<p>Lanthanide-doped upconversion nanoparticles are attractive single-molecule imaging probes due to their high photostability and anti-Stokes luminescence. However, achieving both small particle size and strong brightness has remained a major challenge, as reducing size often leads to dimmer emission. Herein, we fabricate a sub-10 nm cascade actively protected upconversion nanoparticles, which shows a 33-fold enhanced upconversion efficiency at the single-particle level compared to larger ~19 nm conventional&#xa0;nanoparticles. Theoretical modeling and time-resolved measurements show that emission loss mainly comes from energy leakage of Er<sup>3+</sup> ions to surface defects. By introducing a NaYbF<sub>4</sub> layer as photon-harvesting and protective intermediate layer, we minimize this energy loss and significantly boost brightness. A monolayer of inert NaLuF<sub>4</sub> can effectively suppress the surface quenching to Yb<sup>3+</sup>. Using these ultra-small bright probes, we successfully tracked single epidermal growth factor receptor molecules on live cells for up to one hour, revealing dynamic switching between different diffusion modes.</p>

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Sub-10 nm upconversion nanocrystals for long-term single-particle tracking

  • Xiaochen Qiu,
  • Daoming Guan,
  • Xiaojing Xia,
  • Huan Ling,
  • Jialing Hu,
  • Yunxiang Zhang,
  • Emory Chan,
  • Fuyou Li,
  • Qian Liu

摘要

Lanthanide-doped upconversion nanoparticles are attractive single-molecule imaging probes due to their high photostability and anti-Stokes luminescence. However, achieving both small particle size and strong brightness has remained a major challenge, as reducing size often leads to dimmer emission. Herein, we fabricate a sub-10 nm cascade actively protected upconversion nanoparticles, which shows a 33-fold enhanced upconversion efficiency at the single-particle level compared to larger ~19 nm conventional nanoparticles. Theoretical modeling and time-resolved measurements show that emission loss mainly comes from energy leakage of Er3+ ions to surface defects. By introducing a NaYbF4 layer as photon-harvesting and protective intermediate layer, we minimize this energy loss and significantly boost brightness. A monolayer of inert NaLuF4 can effectively suppress the surface quenching to Yb3+. Using these ultra-small bright probes, we successfully tracked single epidermal growth factor receptor molecules on live cells for up to one hour, revealing dynamic switching between different diffusion modes.