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

Author

Listed:
  • 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
    Karlsruhe Institute of Technology)

  • Karolina Słowik

    (Nicolaus Copernicus University)

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.

Suggested Citation

  • Evgenia Rusak & Jakob Straubel & Piotr Gładysz & Mirko Göddel & Andrzej Kędziorski & Michael Kühn & Florian Weigend & Carsten Rockstuhl & Karolina Słowik, 2019. "Enhancement of and interference among higher order multipole transitions in molecules near a plasmonic nanoantenna," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-13748-4
    DOI: 10.1038/s41467-019-13748-4
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