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Sub-50-ns ultrafast upconversion luminescence of a rare-earth-doped nanoparticle

Abstract

Rare-earth-doped upconversion nanoparticles are attracting considerable attention because of their stable, coherent, narrowband and multi-colour luminescence, which features less dephasing effects, crosstalk, photo-blinking and photo-bleaching compared with quantum dots and organic dyes. However, due to the 4f–4f forbidden transitions of rare-earth ions, upconversion nanoparticles exhibit long luminescence decay times, ranging from microseconds to milliseconds, restricting their application in time-dependent nanophotonic devices. Here we fabricate a tilted plasmonic nanocavity to shorten the luminescence decay time of a rare-earth-doped nanoparticle to sub-50 ns while maintaining high quantum efficiency enhancement, tunable polarization-dependent and far-field directional emissions and selective polychromatic chirality. We expect this new type of ultrafast, directional and polarized luminescence of a rare-earth-doped nanoparticle to vigorously promote the development of coherent single-photon sources, quantum communications and nanolasers.

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Fig. 1: Design of a tilted-nanocavity-coupled UCNP for sub-50-ns, directional and polarized emission.
Fig. 2: The upconversion process is significantly accelerated and enhanced using the tilted-plasmonic nanocavity.
Fig. 3: Far-field directional, polarized and ESA-enhanced UCL.
Fig. 4: Chiral control for UCL.

Data availability

All the data that support the plots within this paper are available in the Zenodo repository48.

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Acknowledgements

We thank X. Gan (Northwestern Polytechnical University) for great assistance with FIB morphology characterization. This work was supported by the National Natural Science Foundation of China (grants nos. 92150110, 92050112, 12074237 and 12004233), the Natural Key R&D Program of China (grants nos. 2020YFA0211300 and 2021YFA1201500) and the Fundamental Research Funds for Central Universities (grants nos. GK202201012, GK202103018 and SYJS202222).

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Contributions

Z.Z. conceived the concept. Z.Z., H.Z. and H.X. supervised the work. H.C. conceived and performed the experiment. Z.J., B.K. and H.H. performed the FEM simulation. X.M. and L.G. contributed to chemical syntheses. B.Z., L.Y., C.Z. and J. Li contributed to spectroscopy measurements. J. Lu contributed to TEM characterizations. H.C., Z.Z., Z.F. and H.H. analysed the results. H.C. wrote the manuscript, and all authors revised the manuscript.

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Correspondence to Zhenglong Zhang or Hairong Zheng.

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Nature Photonics thanks Andries Meijerink, Markus Suta and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–28, Discussion and Tables 1–5.

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Chen, H., Jiang, Z., Hu, H. et al. Sub-50-ns ultrafast upconversion luminescence of a rare-earth-doped nanoparticle. Nat. Photon. 16, 651–657 (2022). https://doi.org/10.1038/s41566-022-01051-6

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