The interaction of light with nanometer-sized structures is at the core of nano-optics. It is obvious that as the particles become smaller and smaller the laws of quantum mechanics will become apparent in their interaction with light. In this limit, continuous scattering and absorption of light will be supplemented or replaced by resonant interactions if the photon energy hits the energy difference of discrete internal (electronic) energy levels. In atoms, molecules and nanoparticles, like semiconductor nanocrystals and other “quantum confined” systems, these resonances are found at optical frequencies. Due to the resonant character, the light–matter interaction can often be approximated by treating the quantum system as an effective two-level system, i.e. by considering only those two (electronic) levels whose difference in energy is close to the interacting photon energy ħ ω 0 . In this chapter we consider single-quantum systems that are fixed in space, either by deposition to a surface or by being embedded into a solid matrix. The material to be covered should familiarize the reader with single-photon emitters and with concepts developed in the field of quantum optics. While various theoretical aspects related to the fields emitted by a quantum system have been discussed in Chapter 8, the current chapter focuses more on the nature of the quantum system itself. We adopt a rather practical perspective since more rigorous accounts can be found elsewhere (see e.g. [1–4]).
The interaction of light with nanometer-sized structures is at the core of nano-optics. It is obvious that as the particles become smaller and smaller the laws of quantum mechanics will become apparent in their interaction with light. In this limit, continuous scattering and absorption of light will be supplemented or replaced by resonant interactions if the photon energy hits the energy difference of discrete internal (electronic) energy levels. In atoms, molecules and nanoparticles, like semiconductor nanocrystals and other “quantum confined” systems, these resonances are found at optical frequencies. Due to the resonant character, the light–matter interaction can often be approximated by treating the quantum system as an effective two-level system, i.e. by considering only those two (electronic) levels whose difference in energy is close to the interacting photon energy ħ ω 0 . In this chapter we consider single-quantum systems that are fixed in space, either by deposition to a surface or by being embedded into a solid matrix. The material to be covered should familiarize the reader with single-photon emitters and with concepts developed in the field of quantum optics. While various theoretical aspects related to the fields emitted by a quantum system have been discussed in Chapter 8, the current chapter focuses more on the nature of the quantum system itself. We adopt a rather practical perspective since more rigorous accounts can be found elsewhere (see e.g. [1–4]).
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.
Even though the quantized interaction between light and matter in the photoelectric effect is considered one of the cornerstones in the development of quantum mechanics, it was long thought impossible to directly observe the quantized nature of light itself. The advent of light-intensity autocorrelation techniques in the 1950s, first developed to study the size of stars, changed little in this perception, until true single-photon correlation spectroscopy from trapped ions was proven to be possible in the late 1970s: Photons from a single quantum emitter tend to arrive in bunches, but each light quantum is spaced apart in time—it is antibunched. Initially considered only as the workhorse of atomic quantum optics, over the past two decades, photon correlation techniques have become a standard in fields as diverse as quantum-information processing, biological imaging, polymer physics, and materials science, in general. The technique is particularly useful for probing materials that are specifically designed to emit or absorb light in optoelectronic devices, such as light-emitting diodes, solar cells, or lasers. The central question in such studies is how large a mesoscopic piece of material can become and still behave as an atom-like source of single photons. What interactions may arise between multiple excitations within a material, and what sort of dark states may give rise to intermittency in the stream of photons? We review the many different classes of optoelectronic materials for which photon-correlation spectroscopy has proven to offer useful insight into excited-state dynamics, ranging from molecular, over semiconductor to metallic nanostructures. The technique is particularly suited to probing mesoscopic aggregates of organic semiconductors since each single molecule acts as a quantum emitter itself.
This thesis is devoted to theoretically study the systems of single quantum dots (QDs) embedded in various photonic nanostructures, in close relation with experimental data. The word single is essential: due to their nanometer size, QDs have mainly been studied as ensembles. It is only recently that the experimental progress, in particular in the domain of QDs growth, has allowed to address single QDs. This helped to observe that the confined states in a QD resemble those of an atom, leading in turn to the macro-atom picture for QDs. It opened the path to the study of cavity quantum electrodynamics (CQED) in the solid state, as the analogous of a system of an atom in an electromagnetic cavity. However, already at the level of the QD (i.e. without a solid state cavity), the macro-atom picture has been proven to be oversimplified. Various effects related to the solid state environment of the QD have been experimentally and theoretically evidenced, like the influence of acoustic and optical phonons. These are channels of decoherence for the otherwise well isolated and confined QD levels. When adding the cavity, these effects are possibly enhanced, which can lead to very large deviations from the CQED ideal picture. Therefore the clear understanding of these effects is of essential importance, especially in view of the application of solid state systems to quantum information science. In Chapter 2, we address the radiation-matter coupling between two QDs in a nanocavity. This field of research combines the high quality of light resonators to the nonlinearities of the semiconductor material. It is promising in view of manipulating and transferring single long-lived excitations, an essential goal for quantum information science. Then, we study the deviations of a QD from the idealized macroatom picture. First, in Chapter 3, we include the influence of acoustic phonons on the light emitted by a QD-cavity system. We show that the QD modified susceptibility leads to the qualitative explanation of the cavity feeding effects, which is one of the most striking deviations of the QD-cavity system from the ideal CQED picture. In addition to phonons are extended two-dimensional states populated by the non resonant pumping laser in the QD's wetting layer (WL). In Chapters 4 and 5 we build a Monte-Carlo model of the excitation-decay mechanism in a QD-cavity system. We use it to describe the influence of WL states on the dynamics of the QD, leading in turn to a non-CQED behavior. This approach is particularly successful in the case of large QD-cavity detuning, where it predicts both time-dependent and spectral characteristics of the emitted light. Finally, in Chapter 6, we discuss our conclusions, emphasizing in particular that the knowledge of the actual solid state environment of the QD leads to a better control over the parameters allowing to reach the CQED regime. We also discuss the possible extensions of this work, in particular in relation to the analysis of the stimulated emission regime.
Small optical microresonators are structures which confine light to volumes with dimensions on the order of one wavelength and provide an important means for controlling light-matter interaction in integrated optics. In this Paper, we would like to present our work on the study of the interaction of single quantum emitters or nanoparticles located in the confined optical field of a single-mode microresonator. The interaction possibilities between a general photonic system and a quantum system are discussed, with special focus on the effect of resonant microcavities. For the case of the optical microresonator used in our experiments, we present a model based on the transfer matrix method which can analytically describe the radiative enhancement of even complex resonator geometries. This allows not only the optimization of resonator geometries, but gives accurate information on the radiative processes occurring in the cavity, allowing the extraction of information normally inaccessible in optical measurements.
The interaction of light with matter is at the heart of quantum optics, which itself enables insight into the fundamental aspects of quantum mechanics. First experimental access to this research field has been realized by coupling atoms to light. Here, the transition between discrete energy states of the atom is associated with the absorption and emission of a photon, a single quantum of the electromagnetic field. As a central aspect of quantum optics, the light-emitter interaction can be significantly enhanced by placing the emitter in optical cavity that is on resonance with the emitter. In recent years, this has led to a rapidly evolving research field known as cavity quantum electrodynamics (CQED). In CQED two different regimes are distinguished: the strong and the weak coupling regimes. In the strong coupling regime, the emitted photon is reflected from the cavity mirrors and eventually reabsorbed by the emitter. In contrast, the weak coupling regime describes the irreversible emission, where the photon leaks out of the cavity before it can be reabsorbed. Both the weak and strong coupling regimes enabled fundamental experiments for a better understanding of quantum optical phenomena. \n \n \n \nCQED grants access to the quantum world and hence offers potentially revolutionizing applications, particularly in the field of quantum information processing. A central aspect for the successful implementation of quantum applications is the system's scalability. Unfortunately, placing atoms deterministically inside a cavity remains technologically elaborate and hence minimizes the prospect of scaling a atom-CQED system. \n \nA possibility to address this issue is to implement CQED in the solid state, where sophisticated fabrication strategies allow miniaturization and scalability of the system. Particularly the development of self-assembled quantum dots (QD) in semiconductors represent a promising route. QDs can be considered as artificial atoms that mimic the atomic two-level system. These structures interact strongly with light and therefore have the potential for replacing atoms in CQED. As a central advantage, QDs are naturally trapped, which greatly simplifies the deterministic incorporation into the cavity. \n \nIn recent years, many efforts have been made to couple self-assembled QDs to microcavities. Generally, the successful implementation of CQED requires a cavity with a high quality factor Q and a low mode volume. In a majority of the approaches, the high Q/small mode volume cavities were monolithically defined around the QD, embedding the QD at a fixed position inside the cavity. Both the weak and strong coupling regimes have been reached with these systems. However, for future applications they suffer from several disadvantages. The fixed position of the QD inside the cavity minimizes the prospects for spectral tunability and spatial positioning the QD inside the cavity. Furthermore, prospects for further increasing of the cavity Q-factor and minimization of the mode volume remain limited in these systems. \n \nIn this thesis the mentioned disadvantages are addressed by developing a fully tunable miniaturized Fabry-Pérot microcavity with low mode volume. The design enables both spatial positioning of the emitter inside the cavity and spectral tunability. Successful coupling of a single QD to the microcavity is demonstrated including the strong coupling regime. Further a new approach to decrease the cavity mode volume is presented, where we demonstrate weak coupling is achieved
The discussions in the previous chapters show that already the spontaneous emission, i.e., the simplest manifestation of the quantum-optical fluctuations, exhibits highly nontrivial features as soon as the quantum light is coupled to interacting many-body systems. We have seen, for example, that pronounced resonances in the semiconductor luminescence originate from a nontrivial mixture of exciton and plasma contributions in contrast to the simple transitions between the eigenstates of isolated atomic systems. As a consequence of the conservation laws inherent to the light–matter coupling, the photon emission induces rearrangements in the entire many-body system leading, e.g., to pronounced hole burning in the exciton distribution. As discussed in Chapter 29, this depletion of the optically active excitons leads to a reduction of the total radiative recombination and the appearance of nonthermal luminescence even when the electron–hole system is in quasiequilibrium. Already these observations show that the coupled quantum-optical and many-body interactions induce new intriguing phenomena that are not explainable by the concepts of traditional quantum optics or classical semiconductor physics alone. The foundations of quantum optics are based on systematic investigations of simple systems interacting with few quantized light modes. In this context, one can evaluate and even measure the exact eigenstates or the density matrix with respect to both the photonic and the atomic degrees of freedom. In semiconductor systems, currently the investigations using one or a few quantum dots (QD) are closest to the atomic studies because, due to their discrete eigenstates, one can treat strongly confined quantum dots to some extent like artificial atoms.