Light-Matter Interaction in Hybrid Quantum Plasmonic Systems

Attempting to implement quantum information related applications utilizing atoms and photons, as they naturally form quantum systems supporting superposition states, hybrid quantum plasmonic systems emerged in the past as a platform to study and engineer light-matter interaction. This platform combines the unrivaled electromagnetic field localization of surface plasmon polaritons, boosting the light-matter coupling rate, with the tremendous integration potential of truly nanoscale structures, and both the significant emission rates of nanoantennas and photonic transmission velocities. In this work, a classical description of surface plasmon polaritons is combined with a light-matter interaction model based on a cavity quantum electrodynamical formalism. The resulting composite semi-classical method, introduced and described in this thesis, provides efficient and versatile means to simulate the dynamical behavior of radiative atomic transitions coupled to plasmonic cavity modes in the weak incoherent coupling regime. Both the emission into the far field and various dissipation mechanisms are included by expanding the model to an open quantum system. The variety of light-matter interaction applications that can be modeled with the outlined method is indicated by the four different exemplary scenarios detailed in the application chapter of this thesis. The classical description of localized surface plasmon polaritons is benchmarked by reproducing the experimental measurements of the molecular fluorescence manipulation through optical nanoantennas in a collaborative effort with experimental partners. Furthermore, in the weak light-matter coupling regime, the potential of achieving a higher nanoantenna functionality and simultaneously realizing more elaborate quantum dynamics is revealed by the three remaining applications. Each pivotally involving a bimodal nanoantenna and demonstrating different quantum optical phenomena, the implementation of cavity radiation mode conversion, non-classical cavity emission statistics, and non-classical cavity emission properties is shown and described in the application chapter

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

Spontaneous emission of quantum emitters can be modified by engineering their optical environment. This allows a resonant nanoantenna to significantly modify the radiative properties of a quantum emitter. In this article, we go beyond the common electric dipole approximation for the molecular electronic transition and take light-matter coupling through higher order multipoles into account. We investigate, by means of theory and numerical simulations, a strong enhancement of the magnetic dipole and electric quadrupole emission channels of a molecule adjacent to a plasmonic patch nanoantenna. While this on its own had been considered, the assumption in prior work usually has been that each molecular transition is dominated only by one of those multipolar emission channels. This leads naturally to the notion of discussing the modified emission in terms of a modified local density of states defined for each specific multipolar transition. In reality, this restricts the applicability of the approach, since specific molecular transitions occur via multiple multipolar pathways that have to be considered all at once. Here, we introduce a framework to study interference effects between higher order transitions in molecules by (a) a rigorous quantum-chemical calculation of their multipolar moments and (b) by a consecutive investigation of the transition rate upon coupling to an arbitrarily shaped nanoantenna. Based on that formalism we predict interference effects between these transition channels. This allows for a strong suppression of radiation by exploiting destructive interference. Our work suggests that placing a suitably chosen molecule at a well defined position and at a well defined orientation relative to a nanoantenna can fully suppress the transition probability.Comment: 30 pages, 8 figure

Resonance shifts and spill-out effects in self-consistent hydrodynamic nanoplasmonics

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 approach, such as time-dependent density-functional theory (TD-DFT), that goes beyond an effective Drude-type model. We present a more general formulation of the hydrodynamic model for the inhomogeneous electron gas, which additionally includes gradients of the electron density in the energy functional. In doing so, we arrive at a Self-Consistent Hydrodynamic Model (SC-HDM), where spill-out emerges naturally. We find a redshift for the optical response of Na nanowires, and a blueshift for Ag nanowires, which are both in quantitative 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 TD-DFT methods. Moreover, while the latter typically neglect retardation effects due to time-varying magnetic fields, our SC-HDM takes retardation fully into account.Comment: 27 pages, including 4 figures. Supplemental Material is available upon request to author

Manipulation of photoluminescence of two-dimensional MoSe₂ by gold nanoantennas

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

Subwavelength Focusing of Bloch Surface Waves

Microsized spheres can focus light into subwavelength spatial domains, a phenomenon called photonic nanojet. Even though well studied in three-dimensional (3D) configurations, only a few attempts have been reported to observe similar phenomena in two-dimensional (2D) systems. This, however, is important to take advantage of photonic nanojets in planar optical systems. Usually, surface plasmon polaritons are suggested for this purpose, but they suffer notoriously from rather low propagation lengths due to 2 3 4 5 6 7 8 9 intrinsic absorption. Here, we solve this problem and explore, numerically and experimentally, the use of Bloch surface waves sustained by a suitably structured all-dielectric media to enable subwavelength focusing in a planar optical system. Since only a low-index contrast can be achieved while relying on Bloch surface waves, we perceive a new functional element that allows a tight focusing and the observation of a photonic nanojet on top of the surface. We experimentally demonstrate a spot size of 0.662 lambda in the effective medium. Our approach paves the way to 2D all-dielectric photonic chips for nanoparticle manipulation in fluidic devices and sensing applications

Manipulation of photoluminescence of two-dimensional MoSe2 by gold nanoantennas

stract 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