Cargando…

Enhancement of and interference among higher order multipole transitions in molecules near a plasmonic nanoantenna

Spontaneous emission of quantum emitters can be modified by their optical environment, such as a resonant nanoantenna. This impact is usually evaluated under assumption that each molecular transition is dominated only by one multipolar channel, commonly the electric dipole. In this article, we go be...

Descripción completa

Detalles Bibliográficos
Autores principales: Rusak, Evgenia, Straubel, Jakob, Gładysz, Piotr, Göddel, Mirko, Kędziorski, Andrzej, Kühn, Michael, Weigend, Florian, Rockstuhl, Carsten, Słowik, Karolina
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6920377/
https://www.ncbi.nlm.nih.gov/pubmed/31852897
http://dx.doi.org/10.1038/s41467-019-13748-4
_version_ 1783480940835635200
author Rusak, Evgenia
Straubel, Jakob
Gładysz, Piotr
Göddel, Mirko
Kędziorski, Andrzej
Kühn, Michael
Weigend, Florian
Rockstuhl, Carsten
Słowik, Karolina
author_facet Rusak, Evgenia
Straubel, Jakob
Gładysz, Piotr
Göddel, Mirko
Kędziorski, Andrzej
Kühn, Michael
Weigend, Florian
Rockstuhl, Carsten
Słowik, Karolina
author_sort Rusak, Evgenia
collection PubMed
description Spontaneous emission of quantum emitters can be modified by their optical environment, such as a resonant nanoantenna. This impact is usually evaluated under assumption that each molecular transition is dominated only by one multipolar channel, commonly the electric dipole. In this article, we go beyond the electric dipole approximation and take light-matter coupling through higher-order multipoles into account. We investigate a strong enhancement of the magnetic dipole and electric quadrupole emission channels of a molecule adjacent to a plasmonic nanoantenna. Additionally, we introduce a framework to study interference effects between various transition channels in molecules by rigorous quantum-chemical calculations of their multipolar moments and a consecutive investigation of the transition rate upon coupling to a nanoantenna. We predict interference effects between these transition channels, which allow in principle for a full suppression of radiation by exploiting destructive interference, waiving limitations imposed on the emitter’s coherence time by spontaneous emission.
format Online
Article
Text
id pubmed-6920377
institution National Center for Biotechnology Information
language English
publishDate 2019
publisher Nature Publishing Group UK
record_format MEDLINE/PubMed
spelling pubmed-69203772019-12-20 Enhancement of and interference among higher order multipole transitions in molecules near a plasmonic nanoantenna Rusak, Evgenia Straubel, Jakob Gładysz, Piotr Göddel, Mirko Kędziorski, Andrzej Kühn, Michael Weigend, Florian Rockstuhl, Carsten Słowik, Karolina Nat Commun Article Spontaneous emission of quantum emitters can be modified by their optical environment, such as a resonant nanoantenna. This impact is usually evaluated under assumption that each molecular transition is dominated only by one multipolar channel, commonly the electric dipole. In this article, we go beyond the electric dipole approximation and take light-matter coupling through higher-order multipoles into account. We investigate a strong enhancement of the magnetic dipole and electric quadrupole emission channels of a molecule adjacent to a plasmonic nanoantenna. Additionally, we introduce a framework to study interference effects between various transition channels in molecules by rigorous quantum-chemical calculations of their multipolar moments and a consecutive investigation of the transition rate upon coupling to a nanoantenna. We predict interference effects between these transition channels, which allow in principle for a full suppression of radiation by exploiting destructive interference, waiving limitations imposed on the emitter’s coherence time by spontaneous emission. Nature Publishing Group UK 2019-12-18 /pmc/articles/PMC6920377/ /pubmed/31852897 http://dx.doi.org/10.1038/s41467-019-13748-4 Text en © The Author(s) 2019, corrected publication 2022 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Rusak, Evgenia
Straubel, Jakob
Gładysz, Piotr
Göddel, Mirko
Kędziorski, Andrzej
Kühn, Michael
Weigend, Florian
Rockstuhl, Carsten
Słowik, Karolina
Enhancement of and interference among higher order multipole transitions in molecules near a plasmonic nanoantenna
title Enhancement of and interference among higher order multipole transitions in molecules near a plasmonic nanoantenna
title_full Enhancement of and interference among higher order multipole transitions in molecules near a plasmonic nanoantenna
title_fullStr Enhancement of and interference among higher order multipole transitions in molecules near a plasmonic nanoantenna
title_full_unstemmed Enhancement of and interference among higher order multipole transitions in molecules near a plasmonic nanoantenna
title_short Enhancement of and interference among higher order multipole transitions in molecules near a plasmonic nanoantenna
title_sort enhancement of and interference among higher order multipole transitions in molecules near a plasmonic nanoantenna
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6920377/
https://www.ncbi.nlm.nih.gov/pubmed/31852897
http://dx.doi.org/10.1038/s41467-019-13748-4
work_keys_str_mv AT rusakevgenia enhancementofandinterferenceamonghigherordermultipoletransitionsinmoleculesnearaplasmonicnanoantenna
AT straubeljakob enhancementofandinterferenceamonghigherordermultipoletransitionsinmoleculesnearaplasmonicnanoantenna
AT gładyszpiotr enhancementofandinterferenceamonghigherordermultipoletransitionsinmoleculesnearaplasmonicnanoantenna
AT goddelmirko enhancementofandinterferenceamonghigherordermultipoletransitionsinmoleculesnearaplasmonicnanoantenna
AT kedziorskiandrzej enhancementofandinterferenceamonghigherordermultipoletransitionsinmoleculesnearaplasmonicnanoantenna
AT kuhnmichael enhancementofandinterferenceamonghigherordermultipoletransitionsinmoleculesnearaplasmonicnanoantenna
AT weigendflorian enhancementofandinterferenceamonghigherordermultipoletransitionsinmoleculesnearaplasmonicnanoantenna
AT rockstuhlcarsten enhancementofandinterferenceamonghigherordermultipoletransitionsinmoleculesnearaplasmonicnanoantenna
AT słowikkarolina enhancementofandinterferenceamonghigherordermultipoletransitionsinmoleculesnearaplasmonicnanoantenna