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

Evgenia Rusak, Jakob Straubel, Piotr Gładysz, Mirko Göddel, Andrzej Kędziorski, Michael Kühn, Florian Weigend, Carsten Rockstuhl and Karolina Słowik ()
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Evgenia Rusak: Karlsruhe Institute of Technology
Jakob Straubel: Karlsruhe Institute of Technology
Piotr Gładysz: Nicolaus Copernicus University
Mirko Göddel: Karlsruhe Institute of Technology
Andrzej Kędziorski: Nicolaus Copernicus University
Michael Kühn: Karlsruhe Institute of Technology
Florian Weigend: Karlsruhe Institute of Technology
Carsten Rockstuhl: Karlsruhe Institute of Technology
Karolina Słowik: Nicolaus Copernicus University

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: Abstract 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.

Date: 2019
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DOI: 10.1038/s41467-019-13748-4

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