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Continuous-wave upconverting nanoparticle microlasers

Abstract

Reducing the size of lasers to microscale dimensions enables new technologies1 that are specifically tailored for operation in confined spaces ranging from ultra-high-speed microprocessors2 to live brain tissue3. However, reduced cavity sizes increase optical losses and require greater input powers to reach lasing thresholds. Multiphoton-pumped lasers4,5,6,7 that have been miniaturized using nanomaterials such as lanthanide-doped upconverting nanoparticles (UCNPs)8 as lasing media require high pump intensities to achieve ultraviolet and visible emission and therefore operate under pulsed excitation schemes. Here, we make use of the recently described energy-looping excitation mechanism in Tm3+-doped UCNPs9 to achieve continuous-wave upconverted lasing action in stand-alone microcavities at excitation fluences as low as 14 kW cm−2. Continuous-wave lasing is uninterrupted, maximizing signal and enabling modulation of optical interactions10. By coupling energy-looping nanoparticles to whispering-gallery modes of polystyrene microspheres, we induce stable lasing for more than 5 h at blue and near-infrared wavelengths simultaneously. These microcavities are excited in the biologically transmissive second near-infrared (NIR-II) window and are small enough to be embedded in organisms, tissues or devices. The ability to produce continuous-wave lasing in microcavities immersed in blood serum highlights practical applications of these microscale lasers for sensing and illumination in complex biological environments.

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Fig. 1: Use of microsphere cavity modes and ELNPs for achieving CW, upconverting lasing at low powers.
Fig. 2: Upconverting microlaser structure and WGM properties.
Fig. 3: Upconverting microlaser characterization.
Fig. 4: ELNP energy transfer and emission mechanisms.
Fig. 5: Lasing in aqueous environments, temperature sensing calibration, characterization of microlaser temperature versus pump power, and evaluation of laser stability.

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Acknowledgements

The authors thank E. Wong for technical support. This work was performed at the Molecular Foundry and was supported by the Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under contract no. DE-AC02-05CH11231. This research was in part funded under the target program no. 0115РК03029 “NU-Berkeley strategic initiative in warm-dense matter, advanced materials and energy sources for 2014-2018” from the Ministry of Education and Science of the Republic of Kazakhstan. Portions of this research were supported by the Global Research Laboratory (GRL) Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (no. 2016911815).

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The scientific concepts, ideas and experimental designs were the result of interactions and discussions between A.F.B., N.J.B., E.S.L, L.M., F.S., B.E.C., P.J.S. and E.M.C. E.M.C., E.S.L, C.A.T. and B.T. synthesized the nanoparticles, and A.F.B., E.S.L., L.M., B.E.C. and E.M.C. fabricated the microlasers. A.F.B., K.Y., E.S.B, N.J.B., E.S.L., L.M. and F.S. conducted the spectroscopic measurements. K.Y., K.B. and E.M.C. performed the theoretical modelling. M.V.A., A.F.B. and S.A. conducted the electron microscopy. A.F.B., B.E.C., E.M.C. and P.J.S. wrote the paper, in coordination with all the authors.

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Correspondence to Bruce E. Cohen, Emory M. Chan or P. James Schuck.

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Supplementary Information

Supplementary Figures 1–15, Supplementary Tables 1–2, Supplementary References.

Supplementary Video 1

Description: A 5 μm UCNP microlaser operating in blood serum. The lasing emission is at 800 nm, with the 1,064 nm excitation laser being filtered out in this video. The laser emission illuminates protein globules in the blood serum as they approach and pass by the optical field of the resonator.

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Fernandez-Bravo, A., Yao, K., Barnard, E.S. et al. Continuous-wave upconverting nanoparticle microlasers. Nature Nanotech 13, 572–577 (2018). https://doi.org/10.1038/s41565-018-0161-8

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