Abstract

Upconversion nanocrystals that converted near-infrared radiation into emission in the ultraviolet spectral region offer many exciting opportunities for drug release, photocatalysis, photodynamic therapy, and solid-state lasing. However, a key challenge is the development of lanthanide-doped nanocrystals with efficient ultraviolet emission, due to low conversion efficiency. Here, we develop a dye-sensitized, heterogeneous core–multishelled lanthanide nanoparticle for ultraviolet upconversion enhancement. We systematically study the main influencing factors on ultraviolet upconversion emission, including dye concentration, excitation wavelength, and dye-sensitizer distance. Interestingly, our experimental results demonstrate a largely promoted multiphoton upconversion. The underlying mechanism and detailed energy transfer pathway are illustrated. These findings offer insights into future developments of highly ultraviolet-emissive nanohybrids and provide more opportunities for applications in photo-catalysis, biomedicine, and environmental science.

Highlights

  • Lanthanide-doped upconversion nanoparticles can absorb near-infrared (NIR) laser light and emit visible and ultraviolet light, with potential applications in bioimaging [1,2,3,4,5], biotherapy [6,7,8,9,10,11,12], and so on

  • We developed a dye‐sensitized heterogeneous lanthanide nanoparticle to regulate the energy transfer pathway for UV enhancement by 808 nm excitation

  • We systematically studied the influence of dye concentration, excitation wavelength, and dis‐

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Summary

Introduction

Lanthanide-doped upconversion nanoparticles can absorb near-infrared (NIR) laser light and emit visible and ultraviolet light, with potential applications in bioimaging [1,2,3,4,5], biotherapy [6,7,8,9,10,11,12], and so on. UV light can be obtained by Nd3+ - and Yb3+ -sensitized upconversion [17,18,20,21], it is challenging to realize the high luminescence intensity needed to satisfy the minimum requirement of biological applications. This obstacle can be addressed in several ways: by controlling dopant composition [22], nanoparticle phase and size [23], excitation beam pulse width [24], and nanoparticle core–shell design [21,25,26,27,28,29].

Methods
Characterization
Method
Preparation of Dye-Sensitized Upconversion Nanoparticles
Synthesis of Core–Multishell Upconversion Nanoparticles
Remarkable UV Enhancement
Optimum Weight Ratio between IR-806 and Nanoparticles
The Effect of Excitation Wavelength on UV Upconversion Emission
The Effect of IR-806 Sensitizer Distance on UV Upconversion
Y 3 4 ties of
Energy Transfer Mechanism
Back Energy Transfer from Nanoparticles to IR-806
Back Energy Transfer from Nanoparticles to IR‐806
Discussion
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