LAUSR

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. Here, the authors study the interference effects between different multipole transition channels by coupling a molecule to a plasmonic nanoantenna. Controlling different emission pathways of quantum emitters allows selective enhancement or suppression of the transition rate through devoted illumination schemes.