Amplified stimulated emission in upconversion nanoparticles for super-resolution nanoscopy

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, JA; Xi, P; Jin, D

Amplified stimulated emission in upconversion nanoparticles for super-resolution nanoscopy

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, JA Xi, P Jin, D

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Publication Type:: Journal Article
Citation:: Nature, 2017, 543 (7644), pp. 229 - 233
Issue Date:: 2017-03-09

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Field	Value	Language
dc.contributor.author	Liu, Y	en_US
dc.contributor.author	Lu, Y	en_US
dc.contributor.author	Yang, X	en_US
dc.contributor.author	Zheng, X	en_US
dc.contributor.author	Wen, S https://orcid.org/0000-0002-4670-4658	en_US
dc.contributor.author	Wang, F https://orcid.org/0000-0001-7403-3305	en_US
dc.contributor.author	Vidal, X	en_US
dc.contributor.author	Zhao, J	en_US
dc.contributor.author	Liu, D	en_US
dc.contributor.author	Zhou, Z https://orcid.org/0000-0002-9648-1325	en_US
dc.contributor.author	Ma, C	en_US
dc.contributor.author	Zhou, J https://orcid.org/0000-0002-0605-5745	en_US
dc.contributor.author	Piper, JA	en_US
dc.contributor.author	Xi, P	en_US
dc.contributor.author	Jin, D https://orcid.org/0000-0003-1046-2666	en_US
dc.date.available	2017-01-04	en_US
dc.date.issued	2017-03-09	en_US
dc.identifier.citation	Nature, 2017, 543 (7644), pp. 229 - 233	en_US
dc.identifier.issn	0028-0836	en_US
dc.identifier.uri	http://hdl.handle.net/10453/112909
dc.description.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.	en_US
dc.relation	http://purl.org/au-research/grants/arc/IH150100028
dc.relation	http://purl.org/au-research/grants/arc/FT130100517
dc.relation.ispartof	Nature	en_US
dc.relation.isbasedon	10.1038/nature21366	en_US
dc.subject.classification	General Science & Technology	en_US
dc.title	Amplified stimulated emission in upconversion nanoparticles for super-resolution nanoscopy	en_US
dc.type	Journal Article
utslib.citation.volume	7644	en_US
utslib.citation.volume	543	en_US
utslib.for	0904 Chemical Engineering	en_US
utslib.for	MD Multidisciplinary	en_US
pubs.embargo.period	Not known	en_US
pubs.organisational-group	/University of Technology Sydney
pubs.organisational-group	/University of Technology Sydney/Faculty of Science
pubs.organisational-group	/University of Technology Sydney/Faculty of Science/School of Mathematical and Physical Sciences
pubs.organisational-group	/University of Technology Sydney/Strength - IBMD - Initiative for Biomedical Devices
pubs.organisational-group	/University of Technology Sydney/Students
utslib.copyright.status	closed_access
pubs.issue	7644	en_US
pubs.publication-status	Published	en_US
pubs.volume	543	en_US

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.

Please use this identifier to cite or link to this item:

http://hdl.handle.net/10453/112909