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.
ABSTRACT
Monolayer molybdenum diselenide (MoSe2), a member of the TMDCs family, is an appealing candidate for coupling to gold plasmonic nanostructures as it has smaller bandgap and higher electron mobility in comparison to frequently studied molybdenum disulfide (MoS2). The PL of MoSe2 occurs in the near-infrared spectral range where the emissive properties do not suffer from the enhanced dissipation in the gold due to inter-band transitions. Here, we study the interaction between monolayer MoSe2 and plasmonic dipolar antennas in resonance with the PL emission of MoSe2. By varying the thickness of the spacer between the MoSe2 layer and nanoantenna, we demonstrate manipulation of the PL intensity from nearly fourfold quenching to approximately threefold enhancement. Furthermore, we show that the coupled TMDC-nanoantenna system exhibits strong polarization-dependent PL, thus offering the possibility of polarization-based emission control. Our experimental results are supported by numerical simulations as well. To the best of our knowledge, this is the first study of Au-MoSe2 plasmonic hybrid structures realizing flexible PL manipulation.
ABSTRACT
The standard hydrodynamic Drude model with hard-wall boundary conditions can give accurate quantitative predictions for the optical response of noble-metal nanoparticles. However, it is less accurate for other metallic nanosystems, where surface effects due to electron density spill-out in free space cannot be neglected. Here we address the fundamental question whether the description of surface effects in plasmonics necessarily requires a fully quantum-mechanical ab initio approach. We present a self-consistent hydrodynamic model (SC-HDM), where both the ground state and the excited state properties of an inhomogeneous electron gas can be determined. With this method we are able to explain the size-dependent surface resonance shifts of Na and Ag nanowires and nanospheres. The results we obtain are in good agreement with experiments and more advanced quantum methods. The SC-HDM gives accurate results with modest computational effort, and can be applied to arbitrary nanoplasmonic systems of much larger sizes than accessible with ab initio methods.
ABSTRACT
We propose to use nanoantennas (NAs) coupled to incoherently pumped quantum dots for ultrabright single photon emission. Besides fully quantum calculations, we analyze an analytical expression for the emitted photon rate. From these analytical considerations, it turns out that the Purcell factor and the pumping rate are the main quantities of interest. We also disclose a trade-off between the emitted photon rate and the nonclassical nature of the emitted light. This trade-off has to be considered while designing suitable NAs, which we also discuss in depth.
