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Controlling light–matter interaction at the nanoscale with cavities and nanoantennas

H. Benisty, Jean‐Jacques Greffet, Philippe Lalanne

Published Apr 12, 2022• 0 citations
Publisher

Abstract

Abstract We consider light-matter interaction processes such as emission, absorption, elastic or inelastic scattering and fluorescence by a quantum object such as an atom, a molecule or a quantum dot. The idea of controlling these processes with a resonator (a cavity or a resonant nanoantenna) is to use an intermediate structure which is coupled both to plane waves in vacuum and to the emitters. In this chapter we use a unified approach to discuss any type of resonator using the concept of Green tensor. We review different models to deal with spontaneous emission with the aim of clarifying the connection between classical and quantum points of view. After this analysis of spontaneous emission, we discuss different light-matter interaction processes such as Raman Scattering and Fluorescence both in the linear regime and in the saturation regime. Finally, we discuss how to optimize absorption and introduce the concept of impedance for an optical nanoantenna.

DOI
10.1093/oso/9780198786139.003.0019

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Abstract We consider light-matter interaction processes such as emission, absorption, elastic or inelastic scattering and fluorescence by a quantum object such as an atom, a molecule or a quantum dot. The idea of controlling these processes with a resonator (a cavity or a resonant nanoantenna) is to use an intermediate structure which is coupled both to plane waves in vacuum and to the emitters. In this chapter we use a unified approach to discuss any type of resonator using the concept of Green tensor. We review different models to deal with spontaneous emission with the aim of clarifying the connection between classical and quantum points of view. After this analysis of spontaneous emission, we discuss different light-matter interaction processes such as Raman Scattering and Fluorescence both in the linear regime and in the saturation regime. Finally, we discuss how to optimize absorption and introduce the concept of impedance for an optical nanoantenna.
This chapter considers electron–photon interaction, i.e., light–matter coupling. It introduces the theoretical treatment of electron–photon interaction for different and mostly strongly simplified cases. In resonator structures, calculation of the appropriate photon modes is required to allow access to the strength of electron–photon coupling. The general guideline is that light may be treated as a wave when propagating in vacuum, yet it has to be quantized in the case of the interaction with matter. In any ensemble of atoms or molecules in interaction with an electromagnetic field, there are three processes occurring: spontaneous emission, absorption, and stimulated emission. In order to get a flavor of a many-body treatment of electron–photon interaction, the derivation of the semiconductor Bloch equations will be discussed briefly. The strength of the light field at the location of the electron determines the interaction strength between light and matter.
Single quantum emitters are critical components for many future quantum information technologies. Novel active material systems have been developed and transitioned into engineering efforts at nanoscale. Here, we review recent progress of diverse quantum emitters and their optical properties, including fluorescent point defect in bulk and single nanocrystal, two-dimensional materials, and quantum dots (QDs). Remarkable progress has also been made in controlling spontaneous emission by utilizing the local density of optical states in dielectric photonic nanostructures. We focus on the enhanced light–matter interaction between the emitter and cavity, enabling the realization of efficient and fast single photon sources.
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.
In this chapter, we discuss a purely quantum approach to the interaction between an atom and the electromagnetic field. In this treatment, the atom and electromagnetic field form a single quantum system, whose evolution is handled globally within a unified formalism. This will thus have the merit of being fully consistent from the theoretical standpoint. But the main advantage in an entirely quantum approach is that it can treat the full range of matter–radiation interaction phenomena. In particular, it provides a rigorous description of the spontaneous emission of light by an excited atom , something that falls outside the scope of the semi-classical framework applied in Chapters 2 and 3, where the lifetime of an excited atomic state had to be fed in phenomenologically. It can describe other phenomena of the same type, such as parametric fluorescence by a nonlinear crystal subjected to pumping radiation (see Chapter 7), which underlies many recent developments in quantum optics. The fully quantum approach also has the merit of allowing a simple interpretation in terms of photons for the various matter–radiation interaction processes, such as absorption, stimulated emission, scattering, and also the basic processes of nonlinear optics. Indeed, it provides a unified framework for both stimulated and spontaneous processes. Finally, it can be used to tackle completely new situations where matter and radiation interact, which lie outside the scope of any semi-classical description, such as cavity quantum electrodynamics or the production of single-photon or entangled-photons states .
The fundamental processes of absorption, stimulated and spontaneous emission, and elastic as well as inelastic scattering involving light and atoms, molecules, and nano-particles have been studied for decades using both classical and quantum theories. While providing an overview of the subject, this paper presents a streamlined approach to studying atom-photon interactions in the context of modern quantum optics in the hope of providing guidance for applications in the general area of molecular and nano-photonic machines.
The interaction of light with nanoscale structures is at the core of nano-optics. As the structures become smaller and smaller the laws of quantum mechanics will become apparent. In this limit, the discrete nature of atomic states gives rise to resonant light-matter interactions. In atoms, molecules, and nanoparticles, such as semiconductor nanocrystals and other “quantum confined” systems, these resonances occur when the photon energy matches the energy difference of discrete internal (electronic) energy levels. Owing to the resonant character, light-matter interaction can often be approximated by treating these quantum emitters as effective two-level systems, i.e. by considering only those two (electronic) levels whose difference in energy is close to the interacting photon energy ħω 0 . In this chapter we discuss quantum emitters that are used in optical experiments. We will discuss their use as single-photon sources and analyze their photon statistics. While the radiative properties of quantum emitters have been discussed in Chapter 8, this chapter focuses on the properties of the quantum emitters themselves. We adopt a rather practical perspective since more detailed accounts can be found elsewhere (see e.g. [1–4]). Types of quantum emitters The possibility of detecting single quantum emitters optically relies mostly on the fact that redshifted emission can be very efficiently discriminated against excitation light [5, 6]. This opens the road for experiments in which the properties of these emitters are studied or in which they are used as discrete light sources.