Exciton footprint of self-assembled AlGaAs quantum dots in core-shell nanowires

Quantum-dot-in-nanowire systems constitute building blocks for advanced photonics and sensing applications. The electronic symmetry of the emitters impacts their function capabilities. Here we study the fine structure of gallium-rich quantum dots nested in the shell of GaAs-Al-0.51 Ga-0.49 As core-shell nanowires. We used optical spectroscopy to resolve the splitting resulting from the exchange terms and extract the main parameters of the emitters. Our results indicate that the quantum dots can host neutral as well as charged excitonic complexes and that the excitons exhibit a slightly elongated footprint, with the main axis tilted with respect to the long axis of the host nanowire. GaAs-AlxGa1-xAs emitters in a nanowire are particularly promising for overcoming the limitations set by strain in other systems, with the benefit of being integrated in a versatile photonic structure.

Realization and study of InAs/GaAs quantum dot superluminescent diodes emitting at 1.3µm

Marco Rossetti

A quantum dot is a semiconductor nanostructure that confines the motion of conduction band electrons and valence band holes in all three spatial directions, thus creating fully discrete energy levels. The confinement in the InAs/GaAs material system is generated by the bandgap difference for the two materials (∼ 0.4 eV for InAs, and ∼ 1.4 eV for GaAs) which provides a minimum of potential energy for both electrons and holes inside the InAs nanoparticle. The appearance of new nanoscale effects modifies the electro-optical properties of such a system which makes possible the improvement of existing device performance or even fascinating novel device applications. For the creation of coherent structures with very high purity and high density, as it is required for application in light emitting devices, self-assembling is a very important pathway. The quantum dot creation mostly relies on the relaxation of the strain accumulated during the growth of lattice mismatched materials, which happens in a non-equlibrium condition. This results in a statistical distribution of all the parameters characterizing the InAs nanocrystals as size, composition and strain, whose direct manifestation is the inhomogeneously broadened light emission deriving from quantum dot ensembles. At the dawning of the quantum dot development the broadening was considered as a limiting factor for application in semiconductor lasers. Today, it is considered favorably for all the applications where a broad gain spectrum is required as optical amplifiers, monolithic and external-cavity tunable lasers, and superluminescent diodes. The objective of this thesis is the application of InAs/GaAs self-assembled quantum dots to the active region of high power and broad-band superluminescent diodes emitting in the 1.3 μm wavelength region. Superluminescent diodes are edge-emitting semiconductor light sources based on the amplification of spontaneous emission along a waveguide where optical gain is achieved through current injection. They combine the high power and brightness of laser diodes with the low coherence of LEDs. The latter is a fundamental feature for the application in optical coherence tomography medical imaging, where the image resolution is related to the spectral bandwidth of the light source used. The achievement of bandwidths larger than 100 nm are demonstrated in this work through the optimization of molecular beam epitaxy growth conditions. This may be done optimizing the statistical size-dispersion of the dot ensemble, or through the use of different dot layers emitting at slightly different wavelengths. The large bandwidth emission is obtained also due to the peculiar energy structure of this material, for which a multi-state emission appears under particular injection conditions. As a term of comparison, best commercial single-chip superluminescent diodes for the imaging application at 1.3 μm show bandwidths around 60 nm. Moreover, the discrete nature of the energy levels in InAs quantum dots together with the implementation of a GaAs-based technology can be beneficial for the device temperature stability (the competing technology, based on InP, suffers from strong thermal degradation). The analysis and understanding of the device temperature characteristics will be detailed in the last chapter of the manuscript. Even though standard devices show an important temperature dependence, a better stability may be achieved through the use of p-doped active regions. In the last few years quantum dot devices have shown outstanding properties if compared to the competing quantum well technology. Low threshold currents, high temperature stability and low chirp in lasers, large bandwidths and low gain saturation in amplifiers have been demonstrated. However, in spite of the large interest among the scientific community, many of the microscopic processes at the origin of the electro-optical characteristics of this material are not completely understood yet. The physics of the quantum dot active material, will be modeled in this work through the use of systems of rate equations with different complexity depending on the system they are applied to. We will provide a mean-field rate equation model allowing to get insights about carrier dynamics in QD lasers. Also, we will develop two different traveling-wave rate equation models, one for the modeling of the L-I characteristics and the other for the modeling of the spectral characteristics of quantum dot superluminescent diodes. Considering the carrier and photon density distributions across the device cavity is essential in superluminescent diodes, where the high single pass gain results in large non-homogeneities of photon and carrier distributions. The work is motivated by an industrial cooperation with EXALOS AG, a leading company in the development, manufacturing, and sales of broadband superluminescent diodes.

EPFL2007

Electronic and Optical Properties of Semiconductor Quantum Dots

Guillaume Jean Tarel

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.

EPFL2011

Optically active quantum dots in bottom-up nanowires

Yannik Fontana

This thesis is dedicated to the discovery and progressive study of quantum emitters embedded in the shell of coaxial gallium arsenide/ aluminum gallium arsenide nanowires. The bottom-up core/shell nanowires were grown in a molecular beam epitaxy machine. During the shell growth, diffusion-driven phenomena lead to segregation effects. Gallium-rich regions are formed at the nanoscopic scale. The observation has been made that the reduced dimensionality of these regions provides true tridimensional confinement for the carriers. The recombination spectra of the electrons with the holes in what was coined shell quantum dots (shell-QDs) thus appear as sets of narrow, intense peaks. The formation of shell quantum dots is taking place on a large range of growth temperatures and nominal alloy fractions, giving freedom to engineer the growth process. The shell thickness plays an important role in the quantum dot density and total ensemble spectrum. In addition, the adjunction of an aluminum arsenide predeposition layer increasing the local curvature has been seen to foster the quantum dots formation. Single emitter spectroscopy reveals the few-particles electronic structure of quantum dots, with systematic signatures for the different degrees of occupation of the quantum dot. The shape anisotropy of the quantum dots leads to observable spin-spin interactions, which lift the degeneracy of the exciton level (one hole and one electron). Generally undesirable, this effect allows here to find that the orientation of the quantum dots in the nanowire is not hard-wired to the growth direction or to the nanowire long axis. This observation is confirmed by magneto-photoluminescence experiments. The energetic splitting and shift of the spin sublevels when an external magnetic field is applied also confirms the small size of the quantum dots. It is found that for GaAs in the strong confinement regime, the Landé coefficients of the electron and hole take opposite signs and are dependent on the angle at which the field is applied. These effects allow to tune the exciton composite Landé coefficient and could be used to reduce the splitting between the exciton spin sublevels or create optically degenerate coupled systems. Finally, the sub-nanosecond dynamics happening in the quantum dots are probed with time-correlated photon counting. It is shown that the carriers in the shell are quickly captured by the quantum dots. In addition, it is proposed that the electron population is reduced due to diffusion-assisted mechanisms or through electron-donor recombination.

EPFL2015