In recent years, interest has grown in the research fields of semiconductor lasers and photonic crystals. This thesis looks at integrating photonic crystals into existing semiconductor laser technology to act as functional laser mirrors. The majority of the research is conducted on a quantum-dot material system. The surface recombination velocity of a GaAs based quantum-dot material is shown to be a similar value to InP material. This allows the creation of fine photonic crystal structures in the laser design without high threshold current penalties. The spectral reflection properties of a one dimensional photonic crystal is studied and found to be an unsuitable candidate for a stand-alone laser mirror, due to its low reflectivity. A two-dimensional photonic crystal W3 defect waveguide is successfully integrated as a quantum-dot laser mirror. Single fundamental mode output is achieved with a typically multi-mode 20 μm wide laser mesa, highlighting the mode selective property of the mirror. A similar two-dimensional mirror is studied for its potential as a dispersion compensating mirror for mode-locked lasers. Initial theoretical analysis shows pulse compression for a suitably designed mirror. Experimental continuous- wave results for the same mirror structure demonstrate the tuning of mirror reflectivity with photonic crystal hole radius. A hybrid silicon-organic photonic crystal laser is demonstrated with output in the visible spectrum. This design is a new type of silicon emitter.

Transparent oxide semiconducting films have continued to receive considerable attention, from a fundamental and application-based point of view, primarily because of their useful fundamental properties. Of particular interest is zinc oxide (ZnO), an n-type semiconductor that exhibits excellent optical, electrical, catalytic and gas-sensing properties, and has many applications in various fields. In this work, thin film transistor (TFT) arrays based on ZnO have been prepared by reactive radio frequency (RF) magnetron sputtering. Prior to the TFT fabrication, ZnO layers were sputtered on to glass and silicon substrates, and the deposition parameters optimised for electrical resistivities suitable for TFT applications. The sputtering process was carried out at room temperature with no intentional heating. The aim of this work is to prepare ZnO thin films with stable semiconducting electrical properties to be used as the active channel in TFTs; and to understand the role of intrinsic point defects in device performance and stability. The effect of oxygen (O2) adsorption on TFT device characteristics is also investigated. The structural quality of the material (defect type and concentration), electrical and optical properties (transmission/absorption) of semiconductor materials are usually closely correlated. Using the Vienna ab-initio simulation package (VASP), it is predicted that O2 adsorption may influence film transport properties only within a few atomic layers beneath the adsorption site. These findings were exploited to deposit thin films that are relatively stable in atmospheric ambient with improved TFT applications. TFTs incorporating the optimised layer were fabricated and demonstrated very impressive performance metrics, with effective channel mobilities as high as 30 cm2/V-1s-1, on-off current ratios of 107 and sub-threshold slopes of 0.9 – 3.2 V/dec. These were found to be dependent on film thickness (~15 – 60 nm) and the underlying dielectric (silicon dioxide (SiO2), gadolinium oxide (Gd2O3), yttrium oxide (Y2O3) and hafnium oxide (HfO2)). In this work, prior to sputtering the ZnO layer (using a ZnO target of 99.999 % purity), the sputtering chamber was evacuated to a base pressure ~4 x 10-6 Torr. Oxygen (O2) and argon (Ar) gas (with O2/Ar ratio of varying proportions) were then pumped into the chamber and the deposition process optimised by varying the RF power between 25 and 500 W and the O2/Ar ratio between 0.010 to 0.375. A two-level factorial design technique was implemented to test specific parameter combinations (i.e. RF power and O2/Ar ratio) and then statistical analysis was utilised to map out the responses. The ZnO films were sputtered on glass and silicon substrates for transparency and resistivity measurements, and TFT fabrication respectively. For TFT device fabrication, ZnO films were deposited onto thermally-grown silicon dioxide (SiO2) or a high-k dielectric layer (HfO2, Gd2O3 and Y2O3) deposited by a metal-organic chemical deposition (MOCVD) process. Also, by using ab initio simulation as implemented in the “Vienna ab initio simulation package (VASP)”, the role of oxygen adsorption on the electrical stability of ZnO thin film is also investigated. The results indicate that O2 adsorption on ZnO layers could modify both the electronic density of states in the vicinity of the Fermi level and the band gap of the film. This study is complemented by studying the effects of low temperature annealing in air on the properties of ZnO films. It is speculated that O2 adsorption/desorption at low temperatures (150 – 350 0C) induces variations in the electrical resistance, band gap and Urbach energy of the film, consistent with the trends predicted from DFT results.

Semiconductor nanostructures have attracted great interest owing to their unique physical properties and potential applications in nanoscale functional devices. The enhancement of the physical properties of semiconductor nanostructures and their performance in devices requires a deeper understanding of their fundamental microstructural properties. Thus this thesis is focused on the experimental and theoretical studies of the microstructural properties of two important semiconductor nanostructures: axial heterostructured silicon nanowires with varying doping and indium nitride colloidal nanoparticles. In this thesis, axial heterostructured silicon nanowires with varying doping were synthesized on an oxide-removed Si{111} substrate using a vapour-liquid-solid approach. Their fundamental microstructural properties, including the crystalline structure, wire growth direction and morphologies, were studied using various characterization techniques. It is found that a very small fraction of the silicon nanowires crystallize in a hexagonal (wurtzite) phase, which is thermodynamically unstable in bulk silicon under ambient conditions, while a large majority of the synthesized silicon nanowires exhibit the expected diamond cubic crystalline structure. About 75% of the diamond cubic silicon nanowires synthesized grow in a single <111> direction, while the rest contain growth-related kinks, where the nanowire switches to another direction during the growth. The ~109° silicon nanowire kinks are the most commonly observed, and the growth direction before and after such ~109° kink are both <111>. The sidewalls of silicon nanowires do not change abruptly at the ~109° kink, but exhibit an elbow-shaped structure. It is also found that the nanowire sidewalls exhibit periodic nanofaceting, which is strongly doping-dependent. The nanofaceting is found to occur during the enhanced sidewall growth that arises when the diborane dopant gas is introduced. A thermodynamic model predicting the dependence of nanofacet period on the wire diameter is developed. Another semiconductor nanostructure studied in this thesis is indium nitride colloidal nanoparticles, which were grown using a solution-phase chemical method. The formation of such indium nitride colloidal nanoparticles is confirmed by studying their compositions, crystalline structures and shape using various electron microscopy techniques. The size of the indium nitride colloidal nanoparticles was controlled by varying the time of solution-phase reactions. The most probable size of the colloidal nanoparticles increases and the size distribution broadens with the increase of reaction time. The crystalline structures of the indium nitride colloidal nanoparticles are found to be particle size dependent. The observed dependence of the band gap blueshift of the indium nitride colloidal nanoparticles on the reaction time (hence the particle size) is explained by the quantum-size effect.

La pollution actuelle des effluents hospitaliers par des médicaments, nécessite le développement de nouvelles techniques de traitement, la photocatalyse étant l’une des plus efficaces pour remédier à ce type de pollution. Cependant, les oxydes métalliques utilisés pour la photocatalyse (TiO2, ZnO, …) ne sont activables que sous irradiation UV. L’association de ces oxydes à des Quantum Dots (QDs), crée une hétérojonction qui étend la zone d’activation du photocatalyseur vers les rayonnements visibles et diminue les recombinaisons des porteurs de charges. La première partie de ce travail décrit le développement d’un photocatalyseur activable sous irradiation solaire pour la dégradation du colorant Orange II. Nous avons d’abord caractérisé l’hétérojonction créée entre ZnO et les QDs CuInS2/ZnS (ZCIS) puis étudié leur efficacité photocatalytique, en regardant notamment leurs capacités à générer des espèces réactives de l’oxygène. Dans la seconde partie, nous avons évalué la photodégradation d’un agent anticancéreux, l’Ifosfamide, présent dans les effluents hospitaliers. Pour cela, des réacteurs fermés agités et des microréacteurs ont été utilisés. Dans les deux cas, l’Ifosfamide, ainsi que ses intermédiaires de dégradation, sont photodégradés efficacement par le catalyseur ZnO/ZCIS sous une irradiation solaire de faible intensité (5 mW/cm2). Dans le cas des microréacteurs, le dépôt du catalyseur dans le microcanal a été optimisé et sa stabilité évaluée. Les résultats montrent que le catalyseur ZnO/ZCIS est réutilisable cinq fois sans perte d’activité, témoignant d’une bonne recyclabilité, ce qui en fait un bon candidat pour des applications photocatalytiques / The pollution of hospital effluents by pharmaceutical drugs, requires the development of new treatment techniques. Among these processes, photocatalysis is one of the most efficient one and allows the remediation of this kind of pollution. However, metal oxides used for photocatalysis (TiO2, ZnO, …) can only be activated by UV light. The association of these oxides with quantum dots (QDs) creates an heterojunction, which not only allows to extend the activation spectrum of the photocatalyst to the visible region but also decreases the charge carriers recombinations. The first part of this work describes the development of a catalyst responding to solar light irradiation for the degradation of the Orange II dye. First, we characterized the heterojunction created between ZnO and the CuInS2/ZnS (ZCIS) QDs and evaluated their photocatalytic efficiency. This work was undertaken by evaluating the capacity of the ZnO/ZCIS catalyst to produce reactive oxygen species (ROS). In the second part, we studied the photodegradation of the antineoplastic agent Ifosfamide commonly found in hospital effluents. For this purpose, closed and agitated reactors but also microreactors were used. In both cases, Ifosfamide, and the compounds originating from its degradation, can be fully photodegraded under simulated light of weak intensity (5 mW/cm2) using the ZnO/ZCIS catalyst. In the case of microreactors, the deposition of the catalyst was optimized and its stability evaluated. Results obtained demonstrate that the ZnO/ZCIS catalyst can be reused, at least five times, without significant loss in activity, thus demonstrating its ability to be used in real photocatalytic applications

This thesis describes electrical measurements performed on low dimensional p-type devices, fabricated from GaAs/AlGaAs heterostructures. The Coulomb interaction between holes is similar to that between electrons. However, the kinetic energy is suppressed, which makes interaction effects particularly important. Holes may also be used to study band structure effects which arise from spin-orbit coupling in the valence band. The effects of Coulomb interactions in low dimensional electron systems are currently being studied extensively. Experiments presented in this thesis indicate the possible importance of Coulomb exchange interactions in both one and two dimensional hole systems (1DHSs,2DHSs). Tilted magnetic field studies of 2DHSs in the quantum Hall regime indicate that Landau levels at even filling factors will not cross. For high filling factor, this is attributed to a spin-orbit mixing effect which arises from the low symmetry ofthe system. At lower filling factor, activation-energy measurements verify that the energy gaps decrease and then increase as the field is tilted. However, the energy gap versus field dependences do not exhibit the curvature that might be expected from a perturbative anticrossing. It is speculated that the origin of this effect is a phase transition driven by the exchange interaction. Balanced arguments contrasting the relative strengths of the mixing and interactions theories are provided. The second part of this thesis describes a new method for the fabrication ofballistic 1DHSs, which exhibit clear conductance quantization. The quantization changes from even to odd multiples of e2/h as a function of the magnetic field in the plane of the heterostructure, as 'spin splitting' causes the 1D subbands to cross. Measurements of the 1D subband energy spacings are used together with the magnetic fields at which the crossings occur to calculate the in-plane g factors of the 1D subbands. These are found to increase as the number of occupied 1D subbands decreases. This enhancement of the g factor is attributed to exchange interactions; possible mixing explanations are also discussed. At higher magnetic fields, the pattern of quantization features shows that the subbands have crossed many times, and that the 1DHS can be strongly magnetized.

Στη διπλωματική εργασία αυτή μελετάμε αναλυτικά και υπολογιστικά το φαινόμενο της μίξης τεσσάρων κυμάτων σε δια-υποζωνικές μεταβάσεις ενός συστήματος που αποτελείται από δομές συμμετρικών ημιαγώγιμων κβαντικών πηγαδιών. Στο θεωρητικό μοντέλο παίρνουμε υπόψη δύο υποζώνες ενός ημιαγώγιμου κβαντικού πηγαδιού που αλληλεπιδρούν ταυτόχρονα με ένα ισχυρό ηλεκτρομαγνητικό πεδίο (πεδίο σύζευξης) καθορισμένης συχνότητας και ένα ασθενές ηλεκτρομαγνητικό πεδίο (πεδίο ιχνηθέτη) μεταβλητής συχνότητας. Περά από τη σύμφωνη αλληλεπίδραση των ηλεκτρομαγνητικών πεδίων με τα κβαντικά πηγάδια στη θεωρία μας συμπεριλαμβάνουμε και τα φαινόμενα των αλληλεπιδράσεων ηλεκτρονίου-ηλεκτρονίου. Για την περιγραφή της δυναμικής του συστήματος χρησιμοποιούμε τις εξισώσεις του πίνακα πυκνότητας που προκύπτουν, κάτω από κατάλληλες παραδοχές, από τις γενικευμένες μη-γραμμικές εξισώσεις Bloch. Οι εξισώσεις αυτές επιλύονται αριθμητικά για μια συγκεκριμένη δομή διπλού ημιαγώγιμου κβαντικού πηγαδιού GaAs/AlGaAs στην οποία μεταβάλλουμε την επιφανειακή πυκνότητα ηλεκτρονίων. Παρουσιάζουμε αποτελέσματα και για συνεχή και για παλμικά ηλεκτρομαγνητικά πεδία και δείχνουμε ότι τόσο η ένταση όσο και η μορφή του φάσματος της μίξης τεσσάρων κυμάτων εξαρτάται σημαντικά από την επιφανειακή πυκνότητα ηλεκτρονίων, τη συχνότητα και την ένταση του πεδίου σύζευξης, και στην περίπτωση των παλμικών πεδίων από τη σειρά της χρονικής επιβολής των παλμών. / In this diploma thesis we study analytically and numerically the phenomenon of four-wave mixing in intersubband transitions of a symmetric double quantum well structure. In the theoretical model we consider two quantum well subbands that are coupled by a strong coupling electromagnetic field with fixed frequency and a weak probe electromagnetic field with varying frequency. We consider the coherent interaction of the electromagnetic fields with the quantum wells taking into account the effects of electron-electron interactions. For the description of the system dynamics we use the density matrix equations obtained from the generalized nonlinear Bloch equations. These equations are solved numerically for a realistic semiconductor quantum well structure GaAs/AlGaAs with varying electron sheet density. We present results for both continuous and pulsed electromagnetic fields and show that both the intensity and the shape of the four-wave mixing spectrum can be significantly dependent on electron sheet density, on the frequency and the intensity of the coupling field, and in the case of pulsed fields on the delay between the fields.

The construction of a high-resolution optical microscope system for micro-photoluminescence (µ-PL) spectroscopy is described, and a range of time-integrated and time-resolved experimental work on single InGaN quantum dots (QDs) is presented. Time-integrated measurements demonstrate the existence of InGaN QDs in three different samples via the presence of sharp exciton recombination lines in the µ-PL spectra. The narrowest peaks display a linewidth Γ of ~230 µeV, implying a decoherence time T2 ≥5.7 ps. Time-resolved measurements on exciton recombination lines from single self-assembled InGaN QDs reveal typical lifetimes of ~2.0 ns (which decrease with increasing temperature), while typical lifetimes for excitons in single selectively-grown micropyramidal InGaN QDs are found to be ~0.4 ns. The shorter exciton recombination lifetime in selectively-grown QDs is believed to be due to a stronger coupling of these QDs to the underlying quantum well. Temporal fluctuations (on a timescale of seconds) in the energy, intensity and FWHM of µ-PL peaks arising from the recombination of excitons in single self-assembled InGaN QDs are observed. These are attributed to transient Stark shifts induced by a fluctuating local charge distribution as carriers become trapped in defect states in the vicinity of the QDs. Time-integrated power-dependent measurements are used to demonstrate the presence of biexciton states in single self-assembled InGaN QDs. The exciton–biexciton energy splitting is found to be ~41 meV, in agreement with values predicted by theoretical calculations. Time-resolved studies of the biexciton and exciton decay curves reveal a coupling as the exciton population is refilled by biexciton decays. The biexciton lifetime is found to be ~1.4 ns, compared to an exciton lifetime of ~1.0 ns. Lateral electric fields are applied to a single self-assembled InGaN QD using aluminium electrodes lithographically defined on the sample surface. Application of fields of the order of ~0.17 MVcm-1 is found to cause both a red-shift and a reduction in the intensity of the exciton recombination peak in the µ-PL spectrum.

Magnetic exchange spring systems are multi-layers or composites of magnetically hard and soft materials that are exchange-coupled across their interfaces. In recent years, research into exchange spring systems has flourished, with potential for application in high-performance permanent magnets, GMR spin devices, magnetic MEMS technology, and in magnetic data storage. We investigate the magnetic properties of MBE grown superlattices with alternating layers of magnetically hard rare earth-iron (DyFe2, ErFe2) and soft yttriumiron (YFe2) compounds. They are ideal model systems to study exchange spring phenomena. We develop numerical models of the investigated systems and apply micromagnetic simulations. The simulation code OOMMF is extended and used to solve Landau-Lifshitz-Gilbert and Brown’s equations. This allows us to determine the microscopic configuration of the magnetisation that is not directly accessible by experiment. Magnetic field-sweep measurements of a multilayered DyFe2/YFe2 system show an unexpected triple switching of the magnetically hard DyFe2 layers. The magnetisation of the hard magnetic layers reverse before the soft magnetic layers. We reproduce the experimental hysteresis loops of the net and compound-specific magnetisation by means of simulations and explain the switching behaviour. Using similar numerical methods, we interpret experimental data on ErFe2/YFe2 multilayers. At sufficiently high fields, applied perpendicular to the multilayer film plane, the energy is minimised by a multilayer spin flop. This is a particular spin configuration where the magnetisation aligns with a direction perpendicular to the applied field. Taking the preceding findings further, we investigate multilayers of ErFe2/YFe2/ DyFe2/YFe2. We gain insight in the complex spin configurations in systems of different magnetically hard materials, with a pre-strung domain wall in the soft YFe2 layers. Varying the thickness of the YFe2 layers, we study the changing mutual interference of the switching patterns in the ErFe2 and DyFe2 layers.

Le contexte de cette thèse se situe dans les nombreuses applications de sources UV tels que la stérilisation et la purification. Comparés aux sources conventionnelles, les dispositifs à base de semiconducteur présentent la fiabilité, l'efficacité élevée, et les effets minimaux sur l'environnement. Sur l'aspect des matériaux, III-Nitrures (BAlGaInN) sont les candidats prometteurs car ils sont stables chimiquement et physiquement, et ils présentent les bandes interdites couvrant le spectre visible à l'UV profond. Sur l'aspect des structures, le laser à cavité vertical émettant par la surface (VCSEL) est l'une des configurations les plus attrayantes, et il offre des avantages tels que le seuil bas, le haut rendement, la possibilité d'intégration des réseaux 2D et les tests au niveau de la plaquette. Néanmoins, il n'existe aucun VCSEL fonctionnant en dessous de 300 nm. Des défis importants concernent l'efficacité de MQWs et la réflectivité de réflecteur de Bragg distribué (DBR), qui sont limitées par la qualité des matériaux, les propriétés optiques des MQWs, le contraste faible d'indice de réfraction pour les couches dans les DBRs à des longueurs d'onde courtes, etc. L'objectif de cette thèse est de répondre aux défis relevés auparavant en étudiant la croissance de BAlGaN par épitaxie en phase vapeur aux organométalliques (MOVPE), en développant les MQWs d'AlGaN avec l'augmentation des émissions par la surface, et en explorant les DBRs en BAlN/AlGaN, en vue du développement de VCSEL à pompage optique fonctionnant dans DUV / The context of this thesis falls in the wide applications of UV light sources such as sterilization and purification. Compared to the conventional UV sources (excimer lasers, Nd: YAG lasers or mercury lamps), the semiconductor devices have advantages in reliability, compactness, high efficiency and minimum environmental effects. On the material aspect, III-nitrides (BAlGaInN) are promising candidates since they are chemically and physically stable with direct bandgaps covering from visible to DUV spectrum. On the structure aspect, vertical-cavity surface-emitting laser (VCSEL) is one of the most attractive configurations considering its low threshold, high efficiency, and the possibility for the integration of 2D arrays and the wafer-level tests. It constitutes a multiple-quantum-well (MQW) active region sandwiched by a top and a bottom distributed Bragg reflector (DBR). However, no VCSELs can operate below 300 nm until now. The major challenges lie in the two main blocks: the emission efficiency of MQWs and the reflectivity of DBRs, which are limited by the quality of the substrates and epitaxial layers, optical-polarization properties of the MQW emission, small refractive index contrast of the layers used for DBRs at short wavelengths, etc. The objective of this thesis is to address this need by studying metal-organic vapor-phase epitaxy (MOVPE) growth of BAlGaN materials, developing AlGaN MQWs with enhanced surface emission and exploring BAlN/AlGaN DBRs, for the future development of optically-pumped VCSELs operating below 300 nm

Les boîtes quantiques semiconductrices, confiné dans les trois directions de l’espace, ont une structure électronique proche de celle d’un atome. Une excitation lumineuse y crée des états hors équilibre entraînant l’émission des différents états de charge. Ce travail porte sur l’étude de boîtes quantiques GaAs/AlGaAs produites par une méthode d’épitaxie par jet moléculaire modifiée sur un substrat de GaAs (111) insérées dans une structure de type diode. La première partie porte sur la séparation des différents états de charge dans une boîte unique par la tension appliquée puis leur identification compte tenu de l’échange coulombien et de leurs propriétés magnéto-optiques. Une deuxième partie porte sur l’interaction hyperfine des trous avec le champ nucléaire. Un modèle d’Hamiltonien effectif est proposé pour cette interaction. Des phénomènes de bistabilité, en champ magnétique, de la polarisation des spins nucléaire et électronique sont mis en évidence. / The electronic structure of a semiconductor quantum dot, with 3D carrier confinement on the nano-scale, is close to an atom with discrete state. Above-gap laser excitation creates different exciton state that show very rich emission patterns. This work studies GaAs/AlGaAs quantum dots grown droplet epitaxy on (111)A GaAs substrate embedded in a diode structure. The first part of this thesis presents the spectral separation of exciton complexes due to the bias applied to the sample; the different charge states are identified by analyzing the Coulomb exchange interaction and magneto-optics behavior. The second part studies the hyperfine interaction of the hole spin confined to a dot with the nuclear spins of the atoms that form the dot. An effective Hamiltonian model is proposed for this interaction. Bistable nuclear and also carrier spin polarization states are uncovered in magnetic field dependent measurements.