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Title: | Plasmonic enhancement and polarization dependence of nonlinear upconversion emissions from single gold nanorod@SiO2@CaF2 : Yb3+,Er3+ hybrid core-shell-satellite nanostructures | Authors: | He, JJ Zheng, W Ligmajer, FL Chan, CF Bao, ZY Wong, KL Chen, XY Hao, JH Dai, JY Yu, SF Lei, DY |
Issue Date: | 2017 | Source: | Light : science & applications, 2017, v. 6, e16217 | Abstract: | Lanthanide-doped upconversion nanocrystals (UCNCs) have recently become an attractive nonlinear fluorescence material for use in bioimaging because of their tunable spectral characteristics and exceptional photostability. Plasmonic materials are often introduced into the vicinity of UCNCs to increase their emission intensity by means of enlarging the absorption cross-section and accelerating the radiative decay rate. Moreover, plasmonic nanostructures (e.g., gold nanorods, GNRs) can also influence the polarization state of the UC fluorescence-an effect that is of fundamental importance for fluorescence polarization-based imaging methods yet has not been discussed previously. To study this effect, we synthesized GNR@SiO2@CaF2:Yb3+,Er3+ hybrid core-shell-satellite nanostructures with precise control over the thickness of the SiO2 shell. We evaluated the shell thickness-dependent plasmonic enhancement of the emission intensity in ensemble and studied the plasmonic modulation of the emission polarization at the single-particle level. The hybrid plasmonic UC nanostructures with an optimal shell thickness exhibit an improved bioimaging performance compared with bare UCNCs, and we observed a polarized nature of the light at both UC emission bands, which stems from the relationship between the excitation polarization and GNR orientation. We used electrodynamic simulations combined with Forster resonance energy transfer theory to fully explain the observed effect. Our results provide extensive insights into how the coherent interaction between the emission dipoles of UCNCs and the plasmonic dipoles of the GNR determines the emission polarization state in various situations and thus open the way to the accurate control of the UC emission anisotropy for a wide range of bioimaging and biosensing applications. | Keywords: | Forster resonance energy transfer Gold nanorods Lanthanide-doped upconversion nanocrystals Plasmon-enhanced nonlinear fluorescence Polarization modulation |
Publisher: | Chinese Academy of Sciences, ChangChun Institute of Optics Fine Mechanics and Physics | Journal: | Light : science & applications | ISSN: | 2095-5545 | EISSN: | 2047-7538 | DOI: | 10.1038/lsa.2016.217 | Rights: | This work is licensed under a Creative Commons AttributionNonCommercial-ShareAlike 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under
the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by-nc-sa/4.0/ ©The Author(s) 2017 The following publication He, J., Zheng, W., Ligmajer, F., Chan, C. F., Bao, Z., Wong, K. L., ... & Lei, D. Y. (2017). Plasmonic enhancement and polarization dependence of nonlinear upconversion emissions from single gold nanorod@ SiO 2@ CaF 2: Yb 3+, Er 3+ hybrid core–shell–satellite nanostructures. Light: Science & Applications, 6(5), e16217 is available at https://doi.org/10.1038/lsa.2016.217 |
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