This thesis describes the first and second-order correlation measurements that were performed on a III-V self-assembled quantum dot weakly coupled to a H1 nanophotonic crystal cavity. The system has an exceptionally large Purcell factor, which enables new regimes of light-matter coupling to be explored. In particular, the Purcell effect enhances the radiative recombination rate by an unprecedented factor, allowing measurements to take advantage of the fast lifetime and broad, transform-limited linewidth of the excitons excited in the quantum dot. The main results of this thesis are presented in three chapters, which explore, respectively, the application of the system as a single-photon source, the interactions between the quantum dot excitons and their solid-state environment, and the effect of spectral filtering on resonance fluorescence photon statistics. None of these experiments would have been possible without the very large Purcell enhancement of the radiative emission from the quantum dot. In the first set of experiments, the emission properties of the cavity-coupled quantum dot under p-pulsed resonant excitation were investigated. Hanbury Brown and Twiss second-order correlation measurements were used to measure the single-photon purity of the quantum dot emission. Hong-Ou-Mandel measurements were performed to investigate the indistinguishability of the single-photons produced. The emission from the cavity-coupled dot was then investigated under continuous wave excitation. In the second set of experiments, first-order correlation measurements were made in conjunction with spectroscopic measurements to investigate the phonon sideband properties of the quantum dot, both under resonant and slightly detuned excitation. In the final set of measurements, spectral filtering was used to alter the photon statistics observed when measuring the resonance fluorescence from the cavity-coupled quantum dot. Here, the effect of filtering in both the weak and strong driving regimes was investigated by filtering both above and below the linewidth of the quantum dot.
This thesis describes the first and second-order correlation measurements that were performed on a III-V self-assembled quantum dot weakly coupled to a H1 nanophotonic crystal cavity. The system has an exceptionally large Purcell factor, which enables new regimes of light-matter coupling to be explored. In particular, the Purcell effect enhances the radiative recombination rate by an unprecedented factor, allowing measurements to take advantage of the fast lifetime and broad, transform-limited linewidth of the excitons excited in the quantum dot. The main results of this thesis are presented in three chapters, which explore, respectively, the application of the system as a single-photon source, the interactions between the quantum dot excitons and their solid-state environment, and the effect of spectral filtering on resonance fluorescence photon statistics. None of these experiments would have been possible without the very large Purcell enhancement of the radiative emission from the quantum dot. In the first set of experiments, the emission properties of the cavity-coupled quantum dot under p-pulsed resonant excitation were investigated. Hanbury Brown and Twiss second-order correlation measurements were used to measure the single-photon purity of the quantum dot emission. Hong-Ou-Mandel measurements were performed to investigate the indistinguishability of the single-photons produced. The emission from the cavity-coupled dot was then investigated under continuous wave excitation. In the second set of experiments, first-order correlation measurements were made in conjunction with spectroscopic measurements to investigate the phonon sideband properties of the quantum dot, both under resonant and slightly detuned excitation. In the final set of measurements, spectral filtering was used to alter the photon statistics observed when measuring the resonance fluorescence from the cavity-coupled quantum dot. Here, the effect of filtering in both the weak and strong driving regimes was investigated by filtering both above and below the linewidth of the quantum dot.
In the fields of quantum communications and quantum computing, the transmission of information using single photons guarantees the security of the communication and enables calculations that would be impossible with our "classical" computers. One of the key elements in implementing such protocols is the photon source. It must emit, on demand, one and only one photon with specific quantum properties.The aim of this project is to characterise a source of single and indistinguishable photons, designed and manufactured at CEA-Grenoble, and consisting of an indium arsenide (InAs) semiconductor quantum dot integrated into a gallium arsenide (GaAs) nanocavity. With its low quality factor, the nanocavity enables photons to be extracted efficiently over a wide range of wavelengths (30nm). In addition, thanks to its small mode volume, the spontaneous emission of quantum dots within it can be accelerated by Purcell effect (Purcell factor up to 6).In this manuscript, we first detail the implementation and the optimisation of the experimental setups used to characterise the photons emitted by our sample : microphotoluminescence, radiative lifetime measurement, Hanbury-Brown and Twiss (HBT) experiment and Hong-Ou-Mandel (HOM) experiment. Then, we present the experimental results obtained for photons emitted by two distinct quantum dots : One containing neutral exciton states, and the second, containing a charged exciton state. In order to photo-create these exciton states in the quantum dots, two pulsed optical excitation schemes were implemented: the two-photon resonant excitation of the neutral biexciton, and the phonon-assisted quasi-resonant excitation of the neutral and charged excitons. We present the measurement of the three figures of merit of a single photon source for these two quantum dots : the brightness, the single-photon purity and the indistinguishability of the emitted photons. In a second phase, we will focus on the charged exciton state and measure the profile of its emission line and its autocorrelation function under continuous resonant excitation. These results, achieved within the nano-photonics group of the University of Basel, constitute the first demonstration of continuous excitation on these nanostructures, which is a good surprise given their small size.Finally, we will look at the effects of the application of mechanical stress on the energy separation of the two neutral exciton states, known as the "fine structure splitting" (FSS). During the radiative cascade of the neutral biexciton state, the two photons emitted are entangled in polarisation, and the fidelity of the entanglement depends in particular on the FSS. Here, we will consider a second sample, where the InAs quantum dots are embedded in a GaAs photonic nanowire. By bending the nanowire, mechanical stresses are applied to the quantum dots, which will modify the energy of the exciton states. We will present an experimental study aimed at observing a possible effect on the fine structure splitting.In conclusion, we have developed and optimised various experimental setups for characterising photon sources for applications in the fields of quantum communications and quantum computing. For a first version of these photonic nanostructures, the brightness, the single-photon purity and the indistinguishability of the photons emitted by our quantum dots integrated into nanocavities are very encouraging for the future. The next objectives are to improve the nanocavities and to characterise the decoherence phenomena and the mechanical coupling between the quantum dots and these nanostructures.
Next-generation information technology is expected to rely on discrete two-state quantum systems that can deterministically emit single photons. Quantum dots are mesoscopic (~10,000 atoms large) semiconductor islands grown in a host crystal of larger band-gap that make well-defined two-level quantum systems and are very attractive due to stability, record coherence times, and the possibility of integrating them into larger structures, such as optical microcavities. This work presents experimental progress towards understanding the coherent optical processes that occur in single quantum dots, particularly such phenomena that might be one day utilized for quantum communication applications. High resolution low temperature optical spectroscopy is used in conjunction with first order (amplitude) and second-order (intensity) correlation measurements of the emitted field. A novel technique is introduced that is capable of harvesting the fluorescence of single dots at the same frequency as the laser, previously impossible due to insurmountable scattering. This technique enables the observation, for the first time, of single quantum dot resonance fluorescence, in both the weak and strong excitation regimes, which forms the basis for deterministic generation of single photons. Guided by the rich theoretical description available from quantum optics with atoms we obtain insight into the complex dynamics of this driven system. Quantum dots confined to novel optical microcavities were further investigated using micro photoluminescence. An optical microcavity properly coupled to a two-level system can profoundly modify its emission characteristics via quantum electrodynamical effects, which are highly attractive for single photon sources. The all-epitaxial structures we probe are distinguished by a bulk morphology that overcomes the fragility problems of existing approaches, and provides high quality factors as well as small mode volumes. Lasing is obtained with larger strucutres. Additionally, isolation of individual dots is further realized in smaller cavities and the Purcell effect observed in time-resolved photon counting experiments.
Abstract Inhibition and enhancement of spontaneous emission rate, first proposed by Purcell, is discussed in terms of altered density-of-modes in various types of solid-state cavities and the Purcell factor is derived for two-level atomic system. The conditions for observing Purcell factor and experimental findings in micropillars embedded with Quantum Dots (QD)s are discussed. The strong interaction between photons and matter in the form of QD excitons, dispersion relations for ground and excited states separated by Rabi splitting are discussed. Experimental photoluminescence spectra showing anticrossing of exciton lines and cavity lines by temperature and other tuning methods are used to illustrate the strong light-matter interaction. The Jayness–Cummins model based on second quantization is presented to point out Rabi oscillation, Purcell effect, and other novel features. Microcavity structures for observing cavity quantum electrodynamics effects are mentioned. Microcavity lasers predicting thresholdless operation for unity spontaneous emission coupling factors are discussed.
A single quantum dot embedded in a photonic crystal defect cavity allows for the investigation of cavity quantum electrodynamics effects in a solid-state environment. We present experiments demonstrating the quantum nature of this fundamental system in the strong coupling regime. Photon correlation measurements are used to characterize the fundamental properties of this unique system: through these experiments, we identify an unexpected, efficient sustaining mechanism that ensures strong cavity emission and is quantum correlated with the exciton resonance, even when all the quantum dot resonances are far detuned from the cavity mode.
This thesis presents work on a series of devices for the generation of photonic quantum states based on self-assembled InAs quantum dots, which are among the most technologically mature candidates for practical quantum photonic applications due to their high internal quantum efficiency, narrow linewidth, tunability and straightforward integration with photonic and electric components. The primary results presented concern sources of multi-photon entangled states and single-photon sources with high repetition rate, both of which are crucial components for emerging photonic quantum technologies. First, we propose a scheme for the sequential generation of entangled photon chains by resonant scattering of a laser field on a single charged particle in a cavity-enhanced quantum dot. The charge has an associated spin that can determine the time bin of a photon, allowing for information encoding in this degree of freedom. We demonstrate coherent operations on this spin and realize a proof-of-principle experiment of the proposed scheme by showing that the time bin of a single-photon is dependent on the measured state of the trapped spin. The second main avenue of work investigates the effects of a surface acoustic wave, a mechanical displacement wave confined to the surface of a substrate, on the optical properties of quantum dots. In particular, we exploit the dynamic acoustically-induced tuning of the emission energy to modulate the Purcell effect in a pillar microcavity. Under resonant optical excitation we demonstrate the conversion of the continuous wave laser into a pulsed single-photon stream inheriting the acoustic frequency of 1 GHz as the repetition rate. High resolution spectroscopy reveals the presence of narrow sidebands in the emission spectrum, whose relative intensity can be controlled by the acoustic power and laser detuning. Furthermore, we develop a platform for analogous in-plane experiments by transferring GaAs membranes hosting quantum dots onto LiNbO3 substrates and patterning them into whispering gallery mode optical resonators. In addition to Purcell enhancement and acoustic tuning of the emission, the devices exhibit strong localized mechanical resonances. Finally, we perform initial experiments on the effects of a surface acoustic wave on the spin of a charge trapped in a quantum dot. We integrate acoustic transducers with charge-tunable diodes, where the charge state of the dot can be precisely controlled by an applied bias voltage, and demonstrate the frustration of optical spin pumping by the acoustic wave.
Cavity quantum electrodynamic (cQED) systems have attracted extensive research interest in the past decades as the main driving force of quantum optics. First experimental demonstrations focused on the enhancement of spontaneous emission and optical nonlinearities related to a single quantum emitter confined in a microcavity. Major technological effort was needed to enter the strong coupling regime of single emitter cQED to study for instance the non-harmonicity of resulting Jaynes-Cummings ladder and to perform quantum non-demolition measurements at the heart of quantum optics. Corresponding milestone experiments paved the way towards the realization of a wide variety of non-classical light sources bringing the concept of photonic quantum networks to a practical level. cQED systems can be realized using atomic, superconducting and semiconductor platforms. In view of future applications in the quantum information technology, the solid state platform of microcavities with embedded quantum emitters is the most attractive one as it promises low-cost mass production as well as interoperability with the integrated electronic circuit technology of today. Therefore, quantum dot (QD)-microcavity systems are very attractive for further investigations in this field. Indeed, even though cQED effects have been studied for many years now, there are still fundamental aspects remaining to be explored. One example is the exploration of a strongly coupled cQED system under coherent optical excitation which is one of the primary goals of this work. The work presented in this thesis aims at a deeper understanding of cQED effects in semiconductor based implementations of this central topic of quantum optics. It includes comprehensive spatially-resolved studies of the QD-micropillar system in the both weak and strong coupling regime. For this purpose an advanced 90 degree excitation and detection scheme, suitable for efficient wavelength-independent driving of the coupled exciton (X) and cavity mode (C) system, was implemented. This flexible and powerful technique enables access to the three-dimensional emission characteristics of QD-micropillars providing important new insight into cQED effects which is the central aspect of the first part of this thesis. The performed studies show for instance a pronounced anticorrelation (correlation) of the directional emission characteristics down to the single emitter level in the weak (strong) coupling regime demonstrating directly their fundamentally different nature. Related investigations of the lasing regime present a straightforward characterization method to demonstrate lasing action in high-Beta microlasers without the need for time consuming studies employing photon statistics. The second part of the thesis addresses another very important yet unexplored fundamental aspect of cQED. The main focus is on coherently-driven strongly-coupled QD-microcavity systems. Of particular interest is the regime where the coherent excitation dresses the X-C polariton at high excitation powers. This regime is found at the crossover from a quantum (Jaynes Cummings) to a semi-classical (Mollow Triplet-like) system and can be observed between the limiting cases of an anharmonic and a harmonic ladder solely by varying the excitation strength. An indispensable condition for the first observation of this transitory regime is driving the system through the matter (X) component, which distinguishes this work from previous studies. Counterintuitively, significant cavity losses with respect to the coupling strength are required to create the highly coherent state of the laser-dressed polariton. Moreover, this work pioneers in resonance fluorescence (RF) studies of strongly-coupled QD-microcavity systems and reveals that strong X-C coupling suppresses the RF substantially. Additionally, injection pulling of a single polariton is observed for the first time in the QD-microcavity system, which links this classical effect of injection locking, which is also found in macroscopic lasers, to the quantum regime. Complementary studies on long range off-resonant X-C coupling, mutual coupling of two QD Xs as well as temperature stability of the coherent coupling regime deepen the fundamental understanding of the strong light-matter interaction in semiconductor systems.