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Amplified Plasmonic Forces from DNA Origami-Scaffolded Single Dyes in Nanogaps
[Image: see text] Developing highly enhanced plasmonic nanocavities allows direct observation of light–matter interactions at the nanoscale. With DNA origami, the ability to precisely nanoposition single-quantum emitters in ultranarrow plasmonic gaps enables detailed study of their modified light em...
Autores principales: | , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2023
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10347698/ https://www.ncbi.nlm.nih.gov/pubmed/37364270 http://dx.doi.org/10.1021/acs.nanolett.3c01016 |
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author | Rocchetti, Sara Ohmann, Alexander Chikkaraddy, Rohit Kang, Gyeongwon Keyser, Ulrich F. Baumberg, Jeremy J. |
author_facet | Rocchetti, Sara Ohmann, Alexander Chikkaraddy, Rohit Kang, Gyeongwon Keyser, Ulrich F. Baumberg, Jeremy J. |
author_sort | Rocchetti, Sara |
collection | PubMed |
description | [Image: see text] Developing highly enhanced plasmonic nanocavities allows direct observation of light–matter interactions at the nanoscale. With DNA origami, the ability to precisely nanoposition single-quantum emitters in ultranarrow plasmonic gaps enables detailed study of their modified light emission. By developing protocols for creating nanoparticle-on-mirror constructs in which DNA nanostructures act as reliable and customizable spacers for nanoparticle binding, we reveal that the simple picture of Purcell-enhanced molecular dye emission is misleading. Instead, we show that the enhanced dipolar dye polarizability greatly amplifies optical forces acting on the facet Au atoms, leading to their rapid destabilization. Using different dyes, we find that emission spectra are dominated by inelastic (Raman) scattering from molecules and metals, instead of fluorescence, with molecular bleaching also not evident despite the large structural rearrangements. This implies that the competition between recombination pathways demands a rethink of routes to quantum optics using plasmonics. |
format | Online Article Text |
id | pubmed-10347698 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-103476982023-07-15 Amplified Plasmonic Forces from DNA Origami-Scaffolded Single Dyes in Nanogaps Rocchetti, Sara Ohmann, Alexander Chikkaraddy, Rohit Kang, Gyeongwon Keyser, Ulrich F. Baumberg, Jeremy J. Nano Lett [Image: see text] Developing highly enhanced plasmonic nanocavities allows direct observation of light–matter interactions at the nanoscale. With DNA origami, the ability to precisely nanoposition single-quantum emitters in ultranarrow plasmonic gaps enables detailed study of their modified light emission. By developing protocols for creating nanoparticle-on-mirror constructs in which DNA nanostructures act as reliable and customizable spacers for nanoparticle binding, we reveal that the simple picture of Purcell-enhanced molecular dye emission is misleading. Instead, we show that the enhanced dipolar dye polarizability greatly amplifies optical forces acting on the facet Au atoms, leading to their rapid destabilization. Using different dyes, we find that emission spectra are dominated by inelastic (Raman) scattering from molecules and metals, instead of fluorescence, with molecular bleaching also not evident despite the large structural rearrangements. This implies that the competition between recombination pathways demands a rethink of routes to quantum optics using plasmonics. American Chemical Society 2023-06-26 /pmc/articles/PMC10347698/ /pubmed/37364270 http://dx.doi.org/10.1021/acs.nanolett.3c01016 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Rocchetti, Sara Ohmann, Alexander Chikkaraddy, Rohit Kang, Gyeongwon Keyser, Ulrich F. Baumberg, Jeremy J. Amplified Plasmonic Forces from DNA Origami-Scaffolded Single Dyes in Nanogaps |
title | Amplified Plasmonic
Forces from DNA Origami-Scaffolded
Single Dyes in Nanogaps |
title_full | Amplified Plasmonic
Forces from DNA Origami-Scaffolded
Single Dyes in Nanogaps |
title_fullStr | Amplified Plasmonic
Forces from DNA Origami-Scaffolded
Single Dyes in Nanogaps |
title_full_unstemmed | Amplified Plasmonic
Forces from DNA Origami-Scaffolded
Single Dyes in Nanogaps |
title_short | Amplified Plasmonic
Forces from DNA Origami-Scaffolded
Single Dyes in Nanogaps |
title_sort | amplified plasmonic
forces from dna origami-scaffolded
single dyes in nanogaps |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10347698/ https://www.ncbi.nlm.nih.gov/pubmed/37364270 http://dx.doi.org/10.1021/acs.nanolett.3c01016 |
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