Upconversion luminescence with tunable lifetime in NaYF4

Yb,Er nanocrystals: role of nanocrystal size

Jiangbo Zhao, Zhenda Lu, Yadong Yin, Christopher McRae, James A. Piper, Judith M. Dawes, Dayong Jin*, Ewa M. Goldys

*Corresponding author for this work

Research output: Contribution to journalArticle

243 Citations (Scopus)

Abstract

Despite recent achievements to reduce surface quenching in NaYF 4:Yb,Er nanocrystals, a complete understanding of how the nanocrystal size affects the brightness of upconversion luminescence is still incomplete. Here we investigated upconversion luminescence of Yb,Er-doped nanocrystals in a broad range of sizes from 6 nm to 45 nm (cubic or hexagonal phases), displaying an increasing red-to-green luminescence intensity ratio and reduced luminescence lifetimes with decreasing size. By analyzing the upconversion process with a set of rate equations, we found that their asymptotic analytic solutions explain lower decay rates of red compared to green upconversion luminescence. Furthermore, we quantified the effect of the surface on luminescence lifetime in a model where nanocrystal emitters are divided between the near-surface and inside regions of each nanocrystal. We clarify the influence of the four nonradiative recombination mechanisms (intrinsic phonon modes, vibration energy of surface ligands, solvent-mediated quenching, and surface defects) on the decay rates for different-size nanocrystals, and find that the defect density dominates decay rates for small (below 15 nm) nanocrystals. Our results indicate that a defect-reduction strategy is a key step in producing small upconversion nanocrystals with increased brightness for a variety of bioimaging and biosensing applications.

Original languageEnglish
Pages (from-to)944-952
Number of pages9
JournalNanoscale
Volume5
Issue number3
DOIs
Publication statusPublished - 7 Feb 2013

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