Single Particle Cathodoluminescence Spectroscopy with Sub-20 nm, Electron-Stable Phosphors

Dayne F. Swearer, Stefan Fischer, Daniel K. Angell, Chris Siefe, A. Paul Alivisatos, Steven Chu, Jennifer A. Dionne*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

Lanthanide-doped nanophosphors have emerged as promising optical labels for high-resolution, "multicolor"electron microscopy. Here, we develop a library of 11 unique lanthanide-doped nanophosphors with average edge lengths of 15.2 ± 2.0 nm (N = 4284). These nanophosphors consist of an electron-stable BaYF5 host lattice doped at 25% atomic concentration with the lanthanides Pr3+, Nd3+, Sm3+, Eu3+, Tb3+, Dy3+, Ce3+, Ho3+, Er3+, Tm3+, and Yb3+. Under â 100 pA/nm2 beam current in a transmission electron microscope, each nanophosphor species exhibits strong cathodoluminescence spectra with sharp characteristic emission lines for each lanthanide. The bright emission and stability of these nanoparticles enable not only ensemble, but also single-particle cathodoluminescence spectroscopy, which we demonstrate with BaYF5:Ln3+, where Ln3+ = Tb3+, Ho3+, Er3+, Sm3+, Eu3+, or Pr3+. Single-particle cathodoluminescence corresponds directly with HAADF intensity across nanoparticles, confirming high spatial localization of the measured cathodoluminescence signal of lanthanide-doped nanophosphors. Our synthesis and characterization of sub-20 nm, electron-stable nanophosphors provides a robust material platform to achieve single-molecule labeled correlative cathodoluminescence electron microscopy, a critical foundation for high-resolution correlation of single molecules within the context of cellular ultrastructure.

Original languageEnglish (US)
Pages (from-to)1539-1547
Number of pages9
JournalACS Photonics
Volume8
Issue number6
DOIs
StatePublished - Jun 16 2021
Externally publishedYes

Keywords

  • cathodoluminescence
  • nanophosphors
  • scanning transmission electron microscopy (STEM)
  • single particle spectroscopy

ASJC Scopus subject areas

  • Biotechnology
  • Electronic, Optical and Magnetic Materials
  • Atomic and Molecular Physics, and Optics
  • Electrical and Electronic Engineering

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