The generation of anti-Stokes emission through lanthanide-doped upconversion nanoparticles is of great importance for technological applications in energy harvesting, bioimaging and optical cryptography1,2,3. However, the weak absorption and long radiative lifetimes of upconversion nanoparticles may significantly limit their use in imaging and labelling applications in which a fast spontaneous emission rate is essential4,5,6. Here, we report the direct observation of upconversion superburst with directional, fast and ultrabright luminescence by coupling gap plasmon modes to nanoparticle emitters. Through precise control over the nanoparticle’s local density of state, we achieve emission amplification by four to five orders of magnitude and a 166-fold rate increase in spontaneous emission. We also demonstrate that tailoring the mode of the plasmonic cavity permits active control over the colour output of upconversion emission. These findings may benefit the future development of rapid nonlinear image scanning nanoscopy and open up the possibility of constructing high-frequency, single-photon emitters driven by telecommunication wavelengths.
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Qin, X., Xu, J., Wu, Y. & Liu, X. Energy-transfer editing in lanthanide-activated upconversion nanocrystals: a toolbox for emerging applications. ACS Cent. Sci. 5, 29–42 (2019).
Lu, Y. et al. Tunable lifetime multiplexing using luminescent nanocrystals. Nat. Photon. 8, 32–36 (2014).
Chen, S. et al. Near-infrared deep brain stimulation via upconversion nanoparticle-mediated optogenetics. Science 359, 679–684 (2018).
Chen, X. et al. Confining energy migration in upconversion nanoparticles towards deep ultraviolet lasing. Nat. Commun. 7, 10304 (2016).
Liu, Y. et al. Amplified stimulated emission in upconversion nanoparticles for super-resolution nanoscopy. Nature 543, 229–233 (2017).
Fan, Y. et al. Lifetime-engineered NIR-II nanoparticles unlock multiplexed in vivo imaging. Nat. Nanotechnol. 13, 941–946 (2018).
Wu, M. et al. Solid-state infrared-to-visible upconversion sensitized by colloidal nanocrystals. Nat. Photon. 10, 31–34 (2016).
Chen, C. K., De Castro, A. R. B. & Shen, Y. R. Surface-enhanced second-harmonic generation. Phys. Rev. Lett. 46, 145–148 (1981).
Chen, W. et al. Giant five-photon absorption from multidimensional core-shell halide perovskite colloidal nanocrystals. Nat. Commun. 8, 15198 (2017).
Liu, Q. et al. Single upconversion nanoparticle imaging at sub-10 W cm−2 irradiance. Nat. Photon. 12, 548–553 (2018).
Wu, S. et al. Non-blinking and photostable upconverted luminescence from single lanthanide-doped nanocrystals. Proc. Natl Acad. Sci. USA 106, 10917–10921 (2009).
Zhou, B., Shi, B., Jin, D. & Liu, X. Controlling upconversion nanocrystals for emerging applications. Nat. Nanotechnol. 10, 924–936 (2015).
Renero-Lecuna, C. et al. Origin of the high upconversion green luminescence efficiency in β-NaYF4:2%Er3+,20%Yb3+. Chem. Mater. 23, 3442–3448 (2011).
Zhao, J. et al. Single-nanocrystal sensitivity achieved by enhanced upconversion luminescence. Nat. Nanotechnol. 8, 729–734 (2013).
Laporte, O. & Meggers, W. F. Some rules of spectral structure. J. Opt. Soc. Am. 12, 459–463 (1925).
Malta, O. L. Mechanisms of non-radiative energy transfer involving lanthanide ions revisited. J. Non Cryst. Solids 354, 4770–4776 (2008).
Park, W., Lu, D. & Ahn, S. Plasmon enhancement of luminescence upconversion. Chem. Soc. Rev. 44, 2940–2962 (2015).
Das, A., Mao, C., Cho, S., Kim, K. & Park, W. Over 1,000-fold enhancement of upconversion luminescence using water-dispersible metal–insulator–metal nanostructures. Nat. Commun. 9, 4828 (2018).
Zhang, W., Ding, F. & Chou, S. Y. Large enhancement of upconversion luminescence of NaYF4:Yb3+/Er3+ nanocrystal by 3D plasmonic nano-antennas. Adv. Mater. 24, OP236–OP241 (2012).
Akselrod, G. M. et al. Probing the mechanisms of large Purcell enhancement in plasmonic nanoantennas. Nat. Photon. 8, 835–840 (2014).
Pelton, M. Modified spontaneous emission in nanophotonic structures. Nat. Photon. 9, 427–435 (2015).
Purcell, E., Torrey, H. & Pound, R. Resonance absorption by nuclear magnetic moments in a solid. Phys. Rev. 69, 37–38 (1946).
Song, J. H. et al. Fast and bright spontaneous emission of Er3+ ions in metallic nanocavity. Nat. Commun. 6, 7080 (2015).
Chikkaraddy, R. et al. Single-molecule strong coupling at room temperature in plasmonic nanocavities. Nature 535, 127–130 (2016).
Moreau, A. et al. Controlled-reflectance surfaces with film-coupled colloidal nanoantennas. Nature 492, 86–89 (2012).
Liang, L. et al. Upconversion amplification through dielectric superlensing modulation. Nat. Commun. 10, 1391 (2019).
Gargas, D. J. et al. Engineering bright sub-10-nm upconverting nanocrystals for single-molecule imaging. Nat. Nanotechnol. 9, 300–305 (2014).
Zhang, Q. et al. Seed-mediated synthesis of Ag nanocubes with controllable edge lengths in the range of 30–200 nm and comparison of their optical properties. J. Am. Chem. Soc. 132, 11372–11378 (2010).
Pollnau, M., Gamelin, D., Lüthi, S., Güdel, H. & Hehlen, M. Power dependence of upconversion luminescence in lanthanide and transition-metal-ion systems. Phys. Rev. B 61, 3337–3346 (2000).
Suyver, J., Aebischer, A., García-Revilla, S., Gerner, P. & Güdel, H. Anomalous power dependence of sensitized upconversion luminescence. Phys. Rev. B 71, 125123 (2005).
This work is supported by the Singapore Ministry of Education (MOE2017-T2-2-110), the Agency for Science, Technology and Research (A*STAR; grant no. A1883c0011), the National Research Foundation (NRF), the Prime Minister’s Office, Singapore under its Competitive Research Program (award no. NRF-CRP15-2015-03) and under the NRF Investigatorship Program (award no. NRF-NRFI05-2019-0003), and the National Natural Science Foundation of China (no. 21771135).
The authors declare no competing interests.
Peer review information Nature Nanotechnology thanks Oscar Loureiro and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Wu, Y., Xu, J., Poh, E.T. et al. Upconversion superburst with sub-2 μs lifetime. Nat. Nanotechnol. 14, 1110–1115 (2019). https://doi.org/10.1038/s41565-019-0560-5
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