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.
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.
Controlling quantum emitters (atoms, molecules, quantum dots, etc.), light, and its interactionsis a key issue for implementing all-optical devices and information processing at thequantum level. This generally necessitates a strong coupling of emitters to photonic modes,as achieved by a high-Q cavity, for efficient manipulation of the atoms and field dynamicsthrough cavity quantum electrodynamics (cQED).The integration of the principles of quantum optics at the nanoscale in a plasmonic platformhas been envisioned, on the basis of a possible strong coupling between a quantum emitter andthe surface plasmon polaritons (SPPs) via their strong mode confinement. Recent progressshowed the possibility to reach such a strong coupling regime, allowing the development ofquantum plasmonics where a SPP mode takes the role of the cavity mode. However, its applicationappears notoriously limited in practical situations due to the intrinsic presence ofnumerous and lossy modes, which complicates the description and the interpretation of theinteraction, and introduces strong decoherence in the system, in particular for strong coupling.In this work, a detailed overview of quantum control applied to ion trapping, cQED, and plasmonics,is presented. The first part of the thesis is a study of adiabatic processes in trappedion systems and cQED:- We summarize quantum computation processes using quantum gates, and control usingadiabatic laser pulses with atomic systems.- We design arbitrary quantum gates with ions manipulated with laser pulses.- Models for cQED are derived and applied for the production of photon states leakingfrom a cavity.In the second part, we develop a formalism to describe the quantum dynamics of emitters closeto nanoscale structures, and numerics showing the strong coupling regime and the couplingof emitters via plasmon modes. More specifically:- We provide a general field quantization procedure for spherically layered systems.- Effective models using the field quantization are derived, and we show they are analogousto cQED models.- We describe the interaction of localized plasmons (LSPs) with quantum emitters.- The coupling/entanglement of emitters by adiabatic passage through lossy plasmonicmodes of a nanosphere is shown.
We develop a microscopic quantum theory of surface plasmon polaritons valid for arbitrary metal-dielectric geometries. Our framework is based on the Power-Zienau-Woolley representation of quantum electrodynamics, which provides an optimal separation between electronic and photonic degrees of freedom and is therefore particularly well suited for constructing quantum descriptions of polaritonic excitations in strongly dispersive media. Within this formulation, the fundamental electronic oscillator is identified as the bulk plasmon mode, which is nonperturbatively coupled to the radiative continuum of free photon modes. This coupling induces a geometry-dependent renormalization of the bulk plasma frequency, giving rise to confined plasmonic resonances. As specific applications, we recover the localized surface plasmon modes of metallic nanoparticles, including radiative frequency shifts and decay, as well as the exact dispersion relation of propagating surface plasmon polaritons at planar interfaces. Our quantum treatment further reveals that light-matter interactions at metal-dielectric interfaces are inherently in the ultrastrong coupling regime. As a result, in the quasistatic limit, the system exhibits unconventional ground-state quantum fluctuations that can be controlled through the refractive index. These results open new intriguing perspectives in the field of quantum plasmonics.
Strong light-matter coupling gives rise to polaritons - hybrid excitations whose mixed photonic and matter character enables control over optical, electronic and chemical properties. This Feature Article surveys the main architectures supporting polariton formation, including photonic microcavities, plasmonic nanostructures, open cavities and metasurfaces, and outlines how inorganic semiconductors, organic aggregates and hybrid systems access strong and ultrastrong coupling. Key phenomena such as coherent dynamics, vibronic interactions, dark-state reservoirs and polariton-mediated energy and electron transport are discussed, together with the experimental and theoretical tools used to study them. We highlight examples where strong coupling modifies charge transport, energy flow and chemical reactivity, and we summarize emerging regimes, including intermediate and dark-strong coupling, that broaden the landscape of hybrid light-matter physics.
Rabi oscillations characterize light-matter hybridization in the waveguide quantum electrodynamics~(WQED) framework, with their associated decay rates reflecting excitation damping, yet their behavior remains unresolved when collective emitters are coupled to a collective waveguide mode. This scenario reveals a conceptually novel collective-light-collective-matter interaction, realizable when a timed-Dicke state~(TDS) of subwavelength emitters couples to a slow, delocalized surface-plasmon mode, forming a hybridized plasmon-polariton~(HPP). The HPP acquires its directionality from the TDS via momentum matching. It also exhibits plasmonic characteristics, with excitation frequencies following the surface-plasmon dispersion relation. We obtain a Rabi oscillation and a long-time decay that describe the HPP and use them to reveal weak- and strong-coupling regimes through the emergence of normal-mode splitting. By performing a finite-time Lyapunov-exponent analysis, we show that the HPP also exhibits instantaneous decay and identify three distinct decay regimes: early-time rapid, transient-time oscillatory, and long-time classical. Finally, by analyzing the emission spectrum, we observe an anticrossing of the peak doublets~(a feature also seen in cavity QED setups) which originates from quantum vacuum effects and the resulting non-Markovian HPP evolution in our WQED.
Frontier quantum engineering tasks require reliable control over light-matter interaction dynamics, which could be obtained by introducing electromagnetic structuring. Initiated by the Purcell's discovery of spontaneous emission acceleration in a cavity, the concept of electromagnetic modes' design have gained a considerable amount of attention due to development of photonic crystals, micro-resonators, plasmonic nanostructures and metamaterials. Those approaches, however, offer qualitatively different strategies for tailoring light-matter interactions and are based on either high quality factor modes shaping, near field control, or both. Remarkably, rigorous quantum mechanical description might address those processes in a different fashion. While traditional cavity quantum electrodynamics tools are commonly based on mode decomposition approach, few challenges rise once dispersive and lossy nanostructures, such as noble metals (plasmonic) antennas or metamaterials, are involved. The primary objective of this review is to introduce key methods and techniques while aiming to obtain comprehensive quantum mechanical description of spontaneous, stimulated and higher order emission and interaction processes, tailored by nanostructured material environment. The main challenge and the complexity here are set by the level of rigorousity, up to which materials should be treated. While relatively big nanostructured features (10 nm and larger) could be addressed by applying fluctuation–dissipation theorem and corresponding Green functions' analysis, smaller objects will require individual approach. Effects of material granularity, spatial dispersion, tunneling over small gaps, material memory and others will be reviewed. Quantum phenomena, inspired and tailored by nanostructured environment, plays a key role in development of quantum information devices and related technologies. Rigorous analysis is required for both examination of experimental observations and prediction of new effects.
Surface plasmon polaritons are charge density waves of electrons in a metal, which are coupled to an electromagnetic field at a metal-dielectric interface. The electro- magnetic field associated with surface plasmons is confined, resulting in increased field intensities near the interface. Optical emitters placed near a metal film interact strongly with the surface plasmon modes present, not only modifying the radiation rates, but also the radiation profile. These emitters may be used to store and process information, and understanding their behaviour in the presence of a lossy metal film is important in determining the advantages and limitations of using surface plasmons. In this thesis, we wish to understand how we can optically control atoms by exploring two physical phenomena: first, the influence of surface plasmons on collective effects in an ensemble of emitters. Secondly, the single photon excitation of an emitter near a metal film. In the first case, we analyze the collective radiative behaviour of multiple classical emitters near a metal film that radiatively couple to the far-field through surface plasmon modes. We demonstrate that the contributions of dipolar image charges within the metal film significantly affect the cooperative emission of nearby sources, generating sub- and super-radiant emission that can be controlled with a suitably detuned external driving field. In the second case, we determine the excitation probability of an atom near a metal film by a single photon pulse that is time reversed. Using a quantum electro- dynamic description of absorbing dielectrics, we show that non-radiative decay will limit the excitation probability to about half of the maximum that could be achieved in the absence of losses.