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Physical Review A

Impact of nonradiative line broadening on emission in photonic and plasmonic cavities

Pavel Ginzburg, Alexey V. Krasavin, David R. Richards, Anatoly V. Zayats

Published Oct 20, 2014• 10 citations
Publisher

Abstract

A light-matter interaction modified by the material environment is one of the central topics in quantum electrodynamics. While a strong coupling between a single emitter and a cavity and the Markovian (exponential) relaxation regime are most straightforwardly covered by theory, real physical systems that include also various line broadening effects may possess a much more complicated behavior. Here we propose a theoretical framework to account for nonradiative interaction effects in emission in photonic and plasmonic cavities. The quantum electrodynamics model formulated via a stochastic Hamiltonian approach has been developed with nonradiative line broadening introduced via the Kubo oscillator model. The impact of competing radiative and nonradiative processes on the emitter dynamics has been studied, showing that nonradiative relaxations, having significant impact on processes in high-$Q$ photonic cavities, are much less influential in the plasmonic regime. The developed theoretical framework is not restricted to the emitter in a cavity example, but represents a general tool for multiple stochastic Hamiltonian evolution, important for various types of interactions where either classical or quantum noise is present.

DOI
10.1103/physreva.90.043836

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A light-matter interaction modified by the material environment is one of the central topics in quantum electrodynamics. While a strong coupling between a single emitter and a cavity and the Markovian (exponential) relaxation regime are most straightforwardly covered by theory, real physical systems that include also various line broadening effects may possess a much more complicated behavior. Here we propose a theoretical framework to account for nonradiative interaction effects in emission in photonic and plasmonic cavities. The quantum electrodynamics model formulated via a stochastic Hamiltonian approach has been developed with nonradiative line broadening introduced via the Kubo oscillator model. The impact of competing radiative and nonradiative processes on the emitter dynamics has been studied, showing that nonradiative relaxations, having significant impact on processes in high-QQQ photonic cavities, are much less influential in the plasmonic regime. The developed theoretical framework is not restricted to the emitter in a cavity example, but represents a general tool for multiple stochastic Hamiltonian evolution, important for various types of interactions where either classical or quantum noise is present.
Plasmons in nanostructured metals are widely utilized to trigger strong light-matter interactions with quantum light sources. While the nonclassical behavior of such quantum emitters (QEs) is well understood in this context, the role of quantum and surface effects in the plasmonic resonator is usually neglected. Here, we combine the Green's tensor approach with the Feibelman ddd-parameter formalism to theoretically explore the influence of quantum surface effects in metal-dielectric layered nanostructures on the relaxation dynamics of a proximal two-level QE. Having identified electron spill-out as the dominant source of quantum effects in jellium-like metals, we focus our study on sodium. Our results reveal a clear splitting in the emission spectrum, indicative of having reached the strong coupling regime, and, more importantly, non-Markovian relaxation dynamics of the emitter. Our findings establish that strong light-matter coupling is not suppressed by the emergence of nonclassical surface effects in the optical response of the metal.
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Summary form only given. In the pioneering work of Purcell, the possibility to control spontaneous emission lifetimes of quantum emitters by tailoring their electromagnetic surroundings was widely investigated and verified in various types of cavities or band-gap environments. This includes semiconductor microstructures, photonic crystals, and plasmonic nanoparticles. Due to the extraordinary ability of plasmonic nanostructures to confine light into subwavelength spatial domains, steps beyond the paradigmatic electric dipole approximation in the theoretical description of this process may be necessary. In this contribution, we focus on the case of multiple in general nonidentical two-level emitters, sharing the same electromagnetic surroundings, whose local density of states could be tailored by a neighbouring nanostructure. In this case, the surroundings may serve as a long-distance emitter-emitter interaction carrier, or it may trigger collective emission processes, in analogy to Dicke superradiance. We describe these phenomena taking into account the electric dipole, magnetic dipole and electric quadrupole components of light-matter interaction Hamiltonian.
Abstract In the light–matter strong coupling regime, the excited state of quantum emitters is inextricably linked to a photonic mode, leading to hybrid states that are part light and part matter. Recently, there has been a huge effort to realize strong coupling with nanoplasmonics, since it provides a versatile environment to study and control molecules in ambient conditions. Among the most promising designs are plasmonic nanocavities that confine light to unprecedentedly small volumes. Such nanocavities, though, support multiple types of modes, with different field profiles and radiative decay rates (bright and dark modes). Here, we show theoretically that the different nature of these modes leads to mode beating within the nanocavity and the Rabi oscillations, which alters the spatiotemporal dynamics of the hybrid system. By specifically designing the illumination setup, we decompose and control the dark and bright plasmon mode excitation and therefore their coupling with quantum emitters. Hence, this work opens new routes for dynamically dressing emitters, to tailor their hybrid states with external radiation.
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.