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Room-temperature upconverted superfluorescence

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Abstract

Superfluorescence (SF) is a unique quantum optics phenomenon arising from the assembly of self-organized and cooperatively coupled emitters. SF produces a short and intense burst of light, ideal for various applications in nanophotonics and optical computing. However, due to the prerequisite for cooperative emitter coupling, SF was conventionally observed in a Stokes-shifted manner under cryogenic conditions in limited systems (for example, atomic gases and perovskite-nanocrystal superlattices). Here we show that room-temperature anti-Stokes-shift SF is achieved in a few randomly assembled or in a single lanthanide-doped upconversion nanoparticle. Moreover, upconverted SF has a 10,000-fold accelerated nanosecond lifetime (τ = 46 ns of SF versus τ = 455.8 μs for normal upconversion luminescence), overcoming the slow decay of conventional upconversion systems. Therefore, the conceptual room-temperature anti-Stokes-shift SF not only lays the foundation for ultrafast upconversion but it also paves a straightforward way to a wide variety of applications that have been limited by the existing SF system.

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Fig. 1: Anti-Stokes-shift upconverted SF in Nd3+-ion-compacted UCNPs.
Fig. 2: Anti-Stokes-shift upconverted SF in CSS UCNP assembly.
Fig. 3: Nd3+-ion cluster is the driving force for upconverted SF.
Fig. 4: Upconverted SF in a single UCNP nanocrystal.

Data availability

All data relating to the paper are provided in the Supplementary Information. Source data are provided with this paper.

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Acknowledgements

We acknowledge the Electron Microscopy Facility at the University of Massachusetts Chan Medical School for assistance on the transmission electron microscopy and SEM characterizations. This material is based on work supported, in part, by the US Army Research Laboratory and the US Army Research Office under W911NF2110283.

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Contributions

S.F.L. and G.H. conceived the study., S.F.L., G.H., K.H. and K.K.G. wrote the manuscript. All the authors provided feedback and helped with the research, data analysis and manuscript preparation.

Corresponding authors

Correspondence to Kory Kevin Green, Gang Han or Shuang Fang Lim.

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Nature Photonics thanks the anonymous reviewers for their contribution to the peer review of this work.

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Supplementary Information

Supplementary Figs. 1–12, Notes 1–3 and references.

Source data

Source Data Fig. 2

Statistical source data.

Source Data Fig. 3

Statistical source data.

Source Data Fig. 4

Statistical source data.

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Huang, K., Green, K.K., Huang, L. et al. Room-temperature upconverted superfluorescence. Nat. Photon. 16, 737–742 (2022). https://doi.org/10.1038/s41566-022-01060-5

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