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arXiv · 2306.06200

A generalized approach to photon avalanche upconversion in luminescent nanocrystals

Artiom Skripka·Minji Lee·Xiao Qi·Jia-Ahn Pan·Haoran Yang·Changhwan Lee·P. James Schuck·Bruce E. Cohen·Daniel Jaque·Emory M. Chan
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Abstract

Photon avalanching nanoparticles (ANPs) exhibit extremely nonlinear upconverted emission valuable for sub-diffraction imaging, nanoscale sensing, and optical computing. Avalanching has been demonstrated with Tm3+, Nd3+ or Pr3+-doped nanocrystals, but their emission is limited to 600 and 800 nm, restricting applications. Here, we utilize Gd3+-assisted energy migration to tune the emission wavelengths of Tm3+-sensitized ANPs and generate highly nonlinear emission of Eu3+, Tb3+, Ho3+, and Er3+ ions. The upconversion intensities of these spectrally discrete ANPs scale with the nonlinearity factor s = 10-17 under 1064 nm excitation at power densities as low as 6 kW/cm2. This strategy for imprinting avalanche behavior on remote emitters can be extended to fluorophores adjacent to ANPs, as we demonstrate with CdS/CdSe/CdS core/shell/shell quantum dots. ANPs with rationally designed energy transfer networks provide the means to transform conventional linear emitters into a highly nonlinear ones, expanding the use of photon avalanching in biological, chemical, and photonic applications.

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Artiom Skripka, Minji Lee, Xiao Qi, Jia-Ahn Pan, Haoran Yang, Changhwan Lee, P. James Schuck, Bruce E. Cohen, Daniel Jaque, Emory M. Chan. 2023-06-09. A generalized approach to photon avalanche upconversion in luminescent nanocrystals. https://doi.org/10.1021/acs.nanolett.3c01955

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