Light Scattering from Solid-State Quantum Emitters: Beyond the Atomic Picture
Alistair J. Brash, Jake Iles-Smith, Catherine L. Phillips, Dara P. S. McCutcheon, John O’Hara, Edmund Clarke, Benjamin Royall, Luke R. Wilson, Jesper Mørk, Maurice S. Skolnick, A. M. Fox, Ahsan Nazir
Coherent scattering of light by a single quantum emitter is a fundamental process at the heart of many proposed quantum technologies. Unlike atomic systems, solid-state emitters couple to their host lattice by phonons. Using a quantum dot in an optical nanocavity, we resolve these interactions in both time and frequency domains, going beyond the atomic picture to develop a comprehensive model of light scattering from solid-state emitters. We find that even in the presence of a low-Q cavity with high Purcell enhancement, phonon coupling leads to a sideband that is completely insensitive to excitation conditions and to a nonmonotonic relationship between laser detuning and coherent fraction, both of which are major deviations from atomlike behavior.
Coherent scattering of light by a single quantum emitter is a fundamental process at the heart of many proposed quantum technologies. Unlike atomic systems, solid-state emitters couple to their host lattice by phonons. Using a quantum dot in an optical nanocavity, we resolve these interactions in both time and frequency domains, going beyond the atomic picture to develop a comprehensive model of light scattering from solid-state emitters. We find that even in the presence of a low-Q cavity with high Purcell enhancement, phonon coupling leads to a sideband that is completely insensitive to excitation conditions and to a nonmonotonic relationship between laser detuning and coherent fraction, both of which are major deviations from atomlike behavior.
The desire to produce high-quality single photons for applications in quantum information science has lead to renewed interest in exploring solid-state emitters in the weak excitation regime. Under these conditions it is expected that photons are coherently scattered, and so benefit from a substantial suppression of detrimental interactions between the source and its surrounding environment. Nevertheless, we demonstrate here that this reasoning is incomplete, as phonon interactions continue to play a crucial role in determining solid-state emission characteristics even for very weak excitation. We find that the sideband resulting from non-Markovian relaxation of the phonon environment is excitation strength independent. It thus leads to an intrinsic limit to the fraction of coherently scattered light and to the visibility of two-photon coalescence at weak driving, both of which are absent for atomic systems or within simpler Markovian treatments.
The desire to produce high-quality single photons for applications in quantum information science has lead to renewed interest in exploring solid-state emitters in the weak excitation regime. Under these conditions it is expected that photons are coherently scattered, and so benefit from a substantial suppression of detrimental interactions between the source and its surrounding environment. Nevertheless, we demonstrate here that this reasoning is incomplete, as phonon interactions continue to play a crucial role in determining solid-state emission characteristics even for very weak excitation. We find that the sideband resulting from non-Markovian relaxation of the phonon environment is excitation strength independent. It thus leads to an intrinsic limit to the fraction of coherently scattered light and to the visibility of two-photon coalescence at weak driving, both of which are absent for atomic systems or within simpler Markovian treatments.
Semiconductor nanostructures such as quantum dots (QDs) have offered unique opportunities to investigate quantum optical effects in solid-state systems. These include quantum interference, Rabi oscillations, as well as photon antibunching, and were previously observable only in isolated atoms or ions. In addition, QDs can be integrated into optical microcavities, making them attractive for applications in quantum information processing and high efficiency quantum light sources. Despite much progress towards these goals, one area that was little explored is coherent control of such solid-state quantum emitters in cavities. The main technical hurdle lies in overcoming the laser background scattering. By using a sample structure in which QDs are embedded in a planar Fabry-Perot cavity and by using an orthogonal excitation geometry, we have achieved a nearly complete elimination of laser background scattering. This in turn allows us to show resonantly controlled light emission of quantum dots in the cavity including (a) Rabi flopping using pulse control, (b) direct observation of Mollow triplets in the frequency domain, and (c) simultaneously measured first-order and second order photon-photon correlations.
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.
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