Please use this identifier to cite or link to this item: https://hdl.handle.net/2440/105603
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Type: Journal article
Title: Amplified stimulated emission in upconversion nanoparticles for super-resolution nanoscopy
Author: Liu, Y.
Lu, Y.
Yang, X.
Zheng, X.
Wen, S.
Wang, F.
Vidal, X.
Zhao, J.
Liu, D.
Zhou, Z.
Ma, C.
Zhou, J.
Piper, J.
Xi, P.
Jin, D.
Citation: Nature, 2017; 543(7644):229-233
Publisher: Nature Publishing Group
Issue Date: 2017
ISSN: 0028-0836
1476-4687
Statement of
Responsibility: 
Yujia Liu, Yiqing Lu, Xusan Yang, Xianlin Zheng, Shihui Wen, Fan Wang, Xavier Vidal, Jiangbo Zhao, Deming Liu, Zhiguang Zhou, Chenshuo Ma, Jiajia Zhou, James A. Piper, Peng Xi, Dayong Jin
Abstract: Lanthanide-doped glasses and crystals are attractive for laser applications because the metastable energy levels of the trivalent lanthanide ions facilitate the establishment of population inversion and amplified stimulated emission at relatively low pump power. At the nanometre scale, lanthanide-doped upconversion nanoparticles (UCNPs) can now be made with precisely controlled phase, dimension and doping level. When excited in the near-infrared, these UCNPs emit stable, bright visible luminescence at a variety of selectable wavelengths, with single-nanoparticle sensitivity, which makes them suitable for advanced luminescence microscopy applications. Here we show that UCNPs doped with high concentrations of thulium ions (Tm³⁺), excited at a wavelength of 980 nanometres, can readily establish a population inversion on their intermediate metastable ³H₄ level: the reduced inter-emitter distance at high Tm³⁺ doping concentration leads to intense cross-relaxation, inducing a photon-avalanche-like effect that rapidly populates the metastable ³H₄ level, resulting in population inversion relative to the ³H₆ ground level within a single nanoparticle. As a result, illumination by a laser at 808 nanometres, matching the upconversion band of the ³H₄ → ³H₆ transition, can trigger amplified stimulated emission to discharge the ³H₄ intermediate level, so that the upconversion pathway to generate blue luminescence can be optically inhibited. We harness these properties to realize low-power super-resolution stimulated emission depletion (STED) microscopy and achieve nanometre-scale optical resolution (nanoscopy), imaging single UCNPs; the resolution is 28 nanometres, that is, 1/36th of the wavelength. These engineered nanocrystals offer saturation intensity two orders of magnitude lower than those of fluorescent probes currently employed in stimulated emission depletion microscopy, suggesting a new way of alleviating the square-root law that typically limits the resolution that can be practically achieved by such techniques.
Keywords: Nanoparticles, super-resolution microscopy, lasers, LEDs and light sources, imaging techniques
Rights: © 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
DOI: 10.1038/nature21366
Grant ID: http://purl.org/au-research/grants/arc/FT130100517
http://purl.org/au-research/grants/arc/CE140100003
Published version: http://dx.doi.org/10.1038/nature21366
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