Hybridized decaying oscillations in a nanosystem of two coupled elements—a quantum emitter and a plasmonic nanoantenna—are considered as a classical effect. The circuit model of the nanosystem extends beyond the assumption of inductive or elastic coupling and implies the near-field dipole-dipole interaction. Its results fit those of the previously developed classical model of Rabi splitting, however going much farther. Using this model, we show that the hybridized oscillations depending on the relationships between design parameters of the nanosystem correspond to several characteristic regimes of spontaneous emission. These regimes were previously revealed in the literature and explained involving semiclassical theory. Our original classical model is much simpler: it results in a closed-form solution for the emission spectra. It allows fast prediction of the regime for different distances and locations of the emitter with respect to the nanoantenna (of a given geometry) if the dipole moment of the emitter optical transition and its field coupling constant are known.
Hybridized decaying oscillations in a nanosystem of two coupled elements—a quantum emitter and a plasmonic nanoantenna—are considered as a classical effect. The circuit model of the nanosystem extends beyond the assumption of inductive or elastic coupling and implies the near-field dipole-dipole interaction. Its results fit those of the previously developed classical model of Rabi splitting, however going much farther. Using this model, we show that the hybridized oscillations depending on the relationships between design parameters of the nanosystem correspond to several characteristic regimes of spontaneous emission. These regimes were previously revealed in the literature and explained involving semiclassical theory. Our original classical model is much simpler: it results in a closed-form solution for the emission spectra. It allows fast prediction of the regime for different distances and locations of the emitter with respect to the nanoantenna (of a given geometry) if the dipole moment of the emitter optical transition and its field coupling constant are known.
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.
We develop a theory of cooperative emission of light by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, located near a metal nanostructure supporting surface plasmon. The primary mechanism of cooperative emission in such systems is resonant energy transfer between emitters and plasmons rather than the Dicke radiative coupling between emitters. We identify two types of plasmonic coupling between the emitters, (i) plasmon-enhanced radiative coupling and (ii) plasmon-assisted nonradiative energy transfer, the competition between them governing the structure of system eigenstates. Specifically, when emitters are removed by more than several nm from the metal surface, the emission is dominated by three superradiant states with the same quantum yield as a single emitter, resulting in a drastic reduction of ensemble radiated energy, while at smaller distances cooperative behavior is destroyed by nonradiative transitions. The crossover between two regimes can be observed in distance dependence of ensemble quantum efficiency. Our numerical calculations incorporating direct and plasmon-assisted interactions between the emitters indicate that they do not destroy the plasmonic Dicke effect.
We develop a theory of cooperative emission of light by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, located near a metal nanostructure supporting surface plasmon. The primary mechanism of cooperative emission in such systems is resonant energy transfer between emitters and plasmons rather than the Dicke radiative coupling between emitters. We identify two types of plasmonic coupling between the emitters, (i) plasmon-enhanced radiative coupling and (ii) plasmon-assisted nonradiative energy transfer, the competition between them governing the structure of system eigenstates. Specifically, when emitters are removed by more than several nanometers from the metal surface, the emission is dominated by three superradiant states with the same quantum yield as a single emitter, resulting in a drastic reduction of ensemble radiated energy, while at smaller distances cooperative behavior is destroyed by nonradiative transitions. The crossover between two regimes can be observed in distance dependence of ensemble quantum efficiency. Our numerical calculations incorporating direct and plasmon-assisted interactions between the emitters indicate that they do not destroy the plasmonic Dicke effect.
Highly integrated single-photon sources are key components in future quantum-optical circuits. Whereas the probabilistic generation of single photons can routinely be done by now, their triggered generation is a much greater challenge. Here, we describe the triggered generation of single photons in a hybrid plasmonic device. It consists of a lambda-type quantum emitter coupled to a multimode optical nanoantenna. For moderate interaction strengths between the subsystems, the description of the quantum optical evolution can be simplified by an adiabatic elimination of the electromagnetic fields of the nanoantenna modes. This leads to an insightful analysis of the emitter's dynamics, entails the opportunity to understand the physics of the device, and to identify parameter regimes for a desired operation. Even though the approach presented in this work is general, we consider a simple exemplary design of a plasmonic nanoantenna, made of two silver nanorods, suitable for triggered generation of single photons. The investigated device realizes single photons, triggered, potentially at high rates, and using low device volumes.
We propose an efficient numerical method to study the emission dynamics of a two-level quantum system placed in the vicinity of plasmonic nano-structures. All parameters of an inhomogeneous environment relevant for the evolution of the quantum system are appropriately included via the classical Green's function calculated with three-dimensional finite element method. Numerical solution for the emission dynamics of a two-level system near a gold nano-cylinder demonstrates excellent agreement with the available analytical solution in the limit of the Lorenzian-shaped local density of states. We show numerically that the strong coupling regime can be realized for realistic strength of the dipole moment for a quantum emitter in the gap of a gold bowtie nano-antenna.
We have studied a mathematical framework of higher-order multipole fields in the vicinity of optical nanoantennas. We have exemplified at suitably chosen Nanoantennas i.e. a Nano antenna which strongly enhances the quadruple field. The modification of excitation rates in quantum mechanical systems due to this quadrupolar enhancement was studied. The hybrid system consisting of an optical Nano antenna and a quantum mechanical three level system was studied in detail. A properly designed Nano-antenna can excite dipole for bidden transitions in three level systems due to the enhanced higher order multipole fields. The dynamics of the system is strongly altered by the presence of the nanoantenna and cannot be done by the quadrupolar enhancement alone. This can be achieved by enhancing higher order multipole fields near the antenna. A quadrupole transition as the dominant excitation channel in a three level system was considered. It was found that the enhancement of this transition significantly intensify subsequent emission processes with respect to altered emission characteristics. The effects depend on geometrical parameters; the properties of the optical nanoantenna can be tailored and hence allowed for direct implementations in spectroscopies schemes. The obtained results were found in good agreement with previously obtained results.