Decoupling absorption and emission processes in super-resolution localisation of emitters in a plasmonic hotspot

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Title: Decoupling absorption and emission processes in super-resolution localisation of emitters in a plasmonic hotspot
Authors: Mack
Cortes
Giannini
Torok
Roschuk
Maier, SA
Item Type: Journal Article
Abstract: The absorption process of an emitter close to a plasmonic antenna is enhanced due to strong local electromagnetic (EM) fields. The emission process, if resonant with the plasmonic system, re-radiates to the far-field by coupling with the antenna due to the availability of plasmonic states. This increases the local density of states (LDOS), effectively providing more, or alternate, pathways for emission. Through the mapping of localized emission events from single molecules close to plasmonic antennas – performed using far-field data – one gains combined information on both the local EM field strength and the LDOS available. The localization from these emission-coupled events generally do not, therefore, report the real position of the molecules, nor the EM enhancement distribution at the illuminating wavelength. Here we propose the use of a fluorescent molecule with a large Stokes shift in order to spectrally decouple the emission process of the dye from the plasmonic system, leaving only the absorption strongly in resonance with the enhanced EM field in the antenna’s vicinity. We demonstrate that this technique provides an effective way of exploring either the EM field or the LDOS with nanometre spatial resolution.
Issue Date: 17-Feb-2017
Date of Acceptance: 3-Jan-2017
URI: http://hdl.handle.net/10044/1/43753
DOI: https://dx.doi.org/10.1038/ncomms14513
ISSN: 2041-1723
Publisher: Nature Publishing Group
Journal / Book Title: Nature Communications
Volume: 8
Copyright Statement: © The Author(s) 2017. This work is licensed under a Creative Commons Attribution 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/4.0/
Sponsor/Funder: The Leverhulme Trust
Engineering & Physical Science Research Council (E
Funder's Grant Number: RPG-2014-018
EP/M013812/1
Keywords: Science & Technology
Multidisciplinary Sciences
Science & Technology - Other Topics
SINGLE-MOLECULE
NANOMETER-SCALE
NEAR-FIELD
FLUORESCENCE MICROSCOPY
METALLIC NANOSTRUCTURES
LOCAL-DENSITY
NANOANTENNA
ALUMINUM
ENHANCEMENT
NANOSCALE
MD Multidisciplinary
Publication Status: Published
Article Number: 14513
Appears in Collections:Condensed Matter Theory
Physics
Photonics
Experimental Solid State
Faculty of Natural Sciences



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