Das Wachstum von monolagen dünnen Schichten von InN und GaN/InN auf ZnO wurde untersucht. Ebenso der Einfluss der Verspannung, welche durch das Substrat bedingt ist, auf den Indiumgehalt von (In, Ga)N Heterostrukturen, welche auf GaN und ZnO gewachsen wurden. Alle Proben wurden mittels Molekularstrahlepitaxy gewachsen. Es wurde eine Prozedur entwickelt zum Glühen von ZnO Substraten, um glatte Oberflächen mit Stufenfluss-Morphologie zu erhalten, welche sich für das Wachstum von monolage-dünnen Heterostrukturen eignen. Solche Zn-ZnO und O-ZnO Oberflächen konnten produziert werden, wenn die Proben bei 1050 °C in einer O2 Atmosphäre bei 1 bar für eine Stunde geglüht wurden. Reflection high energy electron diffraction wurde eingesetzt, um in situ den Wachstumsmodus und die Entwicklung des a-Gitterabstandes zu untersuchen. Die kritische Schichtdicke, ab welcher ein Übergang im Wachstumsmodus von glattem zu rauhem Wachstum statt findet, war für das Wachstum von InN auf ZnO geringer als 2 ML und setzt gemeinsam mit dem Beginn der Relaxation ein. Für das Wachstum von GaN auf monolagen-dünnem InN/ZnO konnte gezeigt werden, dass höchstens wenige ML abgeschieden werden können, bevor Relaxation eintritt und/oder eine Vermischung zu (In, Ga)N stattfindet. Untersuchungen durch Röntgenbeugung und Raman Spektroskopie geben Hinweise darauf, dass das Abscheidung der nominalen Struktur 100x(1 ML InN/2 MLs GaN) vermutlich zum Wachstum von (In, Ga)N führte. Die chemische Zusammensetzung war für alle Proben sehr ähnlich mit einem indium Gehält von etwa x: 0.36 und einem Relaxationsgrad von 65% - 73% für Proben, die auf ZnO gewachsen wurde und 95% für Wachstum auf 300 nm In0.19Ga0.81N/GaN. Ein unbeabsichtigter Unterschied im V/III-Verhältnis während des Wachstums von (In, Ga)N Heterostrukturen, auf welchen die Anwesenheit von Metalltröpchen auf manchen Proben hinwies, lies auf einen möglichen Einfluss auf das Relaxationsverhalten und die Oberflächenrauhigkeit schließen. / Several thin InN and GaN/InN films and (In, Ga)N heterostructures were grown using molecular beam epitaxy to investigate their growth mode. InN and GaN/InN films were grown on ZnO substrates and (In, Ga)N heterostructures were grown on (In, Ga)N buffers and ZnO substrates. Fabricating the heterostructures on two different types of substrates was a means of strain engineering to possibly increase the indium content in the (In, Ga)N layers. An annealing procedure was established to treat ZnO substrate to gain smooth, stepped surfaces suitable for ML thin heterostructure devices. Reflection high energy electron diffraction was used to investigate in situ the growth mechanism and evolution of the a-lattice spacing. The critical layer thickness for growth mode transition of InN from smooth to rough is below 2 MLs and fairly coincides with the onset of main relaxation. The deposition of GaN on ML thin InN/ZnO shows that at best a few MLs can be deposited before relaxation and/or intermixing into (In, GaN) takes place. Investigations by X-ray diffraction and Raman spectroscopy indicate that the deposition of a nominal structure of 100x(1 ML InN/2 MLs GaN) seems to result in the growth of (In, Ga)N instead. The average chemical composition was similar for all samples with an indium content close to x: 0.36 and a degree of relaxation between 65%-73% for samples grown on ZnO and 95% for the sample grown on 300 nm In0.19Ga0.81N/GaN pseudo-substrate. The surface was probed with atomic force microscopy and showed that starting with smooth surfaces with root mean square roughness around 0.2 nm there was a considerable roughening during growth and surfaces with grain like morphology and a roughness around 2 to 3 nm was produced. Unintentional differences in V/III ratio during growth of (In, Ga)N heterostructures, indicated by the presence of droplets on some of the sample surfaces, were possible, impacting on the sample relaxation behavior and the surface roughness.

This thesis examines second-order optical nonlinear wave mixing processes in domain-disordered quasi-phase matching waveguides and evaluates their potential use in compact, monolithically integrated wavelength conversion devices. The devices are based on a GaAs/AlGaAs superlattice-core waveguide structure with an improved design over previous generations. Quantum-well intermixing by ion-implantation is used to create the quasi-phase matching gratings in which the nonlinear susceptibility is periodically suppressed. Photoluminescence experiments showed a large band gap energy blue shift around 70 nm after intermixing. Measured two-photon absorption coefficients showed a significant polarization dependence and suppression of up to 80% after intermixing. Similar polarization dependencies and suppression were observed in three-photon absorption and nonlinear refraction. Advanced modeling of second-harmonic generation showed reductions of over 50% in efficiency due to linear losses alone. Self-phase modulation was found to be the dominant parasitic nonlinear effect on the conversion efficiency, with reductions of over 60%. Simulations of group velocity mismatch showed modest reductions in efficiency of less than 10%. Experiments on second-harmonic generation showed improvements in efficiency over previous generations due to low linear loss and improved intermixing. The improvements permitted demonstration of continuous wave second-harmonic generation for the first time in such structures with output power exceeding 1 µW. Also, Type-II phase matching was demonstrated for the first time. Saturation was observed as the power was increased, which, as predicted, was the result of self-phase modulation when using 2 ps pulses. By using 20 ps pulses instead, saturation effects were avoided. Thermo-optically induced bistability was observed in continuous wave experiments. Difference frequency generation was demonstrated with wavelengths from the optical C-band being converted to the L- and U-bands with continuous waves. Conversion for Type-I phase matching was demonstrated over 20 nm with signal and idler wavelengths being separated by over 100 nm. Type-II phase matched conversion was also observed. Using the experimental data for analysis, self-pumped conversion devices were found to require external amplification to reach practical output powers. Threshold pump powers for optical parametric oscillators were calculated to be impractically large. Proposed improvements to the device design are predicted to allow more practical operation of integrated conversion devices based on quasi-phase matching superlattice waveguides.

The unique properties, such as large direct bandgap, excellent thermal stability, high μH × ns, of III-nitrides make them ideal candidates for both optoelectronic and high-speed electronic devices. In the past decades, great success has been achieved in commercialization of GaN based light emitting diodes (LEDs) and laser diodes (LDs). However, due to the lack of native substrates, thin films grown on sapphire or SiC substrates have high defect densities that degrade the device performance and reliability. Conventional epitaxy lateral overgrowth (ELO) can reduce dislocation densities down to ∼10-6 cm-2 in the lateral growth area, but requires ex situ photolithography steps. Hence, an in situ method using a SiNx interlayer (nano-scale ELOG) has emerged as a promising technique. The GaN templates prepared by this method exhibit a very low dislocation density (low-10-7 cm-2) and excellent optical and electrical properties. As a cost, such high quality GaN templates containing SiN, nanonetworks are not suitable for heterojunction field effect transistor (HFET) applications due to degenerate GaN:Si layer which serves as parallel conduction channel. This dissertation discusses the growth of low dislocation density GaN templates, by using the in situ SiNx nanonetwork for conductive templates, and the AIN buffer for semi-insulating templates. On SiN x nanonetwork templates, double-barrier RTD and superlattice (SL) exhibited negative differential resistances. Moreover, the injection current of Blue LEDs (450 nm) was improved ∼30%. On semi-insulating GaN templates, nearly lattice matched AlInN/AIN/GaN HFETs were successfully demonstrated and exhibited ∼ 1600 cm2/Vs and 17 600 cm2/Vs Hall mobilities at 300 K and 10 K, respectively. Those mobility values are much higher than literature reports and indicate that high quality HFETs can be realized in lattice matched AlInN/AIN/GaN, thereby solving the strain related issue. The attempt to use InGaN as the 2DEG channel has also been successfully implemented. A Hall mobility (1230 cm2/Vs) was achieved in a 12 nm InGaN channel HFET with AlInGaN barrier, which demonstrates the viability of InGaN channel HFETs.

Ce travail de thèse porte sur la conception et la réalisation de capteurs optiques ultracompacts et sensibles utilisant le mode d’interrogation en intensité pour la détection d’analytes chimiques et biologiques. Deux approches, l’intégration hybride et l’intégration monolithique, ont été explorées durant cette thèse. Après un descriptif des outils d’analyse et de conception de guides d’onde et de micro résonateurs en anneaux, le manuscrit présente l’intégration hybride d’un laser Fabry-Perot en semiconducteur III-V avec un résonateur en anneau basé sur du matériau SOI. Le laser Fabry-Perot à faible coût fonctionnant en multimode longitudinal a été utilisé comme peigne de référence pour le résonateur en anneau en contact avec un échantillon liquide. L’effet Vernier a été implanté dans le système de détection en utilisant le mode d’interrogation en intensité. La largeur spectrale étroite du laser avec sa densité de puissance élevée ont permis d’obtenir un capteur de plus haute sensitivité en comparaison avec le capteur en double anneaux réalisé précédemment. Une étude numérique d’un capteur composé d’un laser Fabry-Perot et deux résonateurs en anneaux permettant de compenser la fluctuation de température a été ensuite présentée. Concernant l'intégration monolithique, l'interface entre oxyde et non-oxyde après l’oxydation de AlGaAs a été étudiée au Central de Technologies du LPN/CNRS. Un phénomène d’oxydation verticale de GaAs ou AlGaAs avec une faible teneur en aluminium activée par une couche voisine oxydée de AlGaAs avec une forte teneur en aluminium a été identifié expérimentalement. Afin de limiter l’oxydation verticale et de réduire la rugosité des interfaces, des guides d’onde basés respectivement sur une structure intégrant un super-réseau et sur une structure standard ont été fabriqués et caractérisés. L’impact de l'hydrogène sur l'activation du processus d'oxydation de GaAs ou AlGaAs avec une faible teneur en Al a été mis en évidence. Enfin, ce manuscrit décrit la réalisation et la caractérisation d’un laser Fabry-Perot fonctionnant en mode TM. Ce laser constitue une brique important vers l’intégration monolithique d’un capteur extrêmement sensible. / The objective of the thesis is to realize the integrated optical sensors with high sensitivity using intensity interrogation method for chemical and biological analyte detection. For this purpose, two approaches, hybrid integration and monolithic integration, have been explored theoretically and experimentally during this thesis. After a review of the design and analysis tools of optical waveguide and micro-ring resonators, the manuscript reports an experimental demonstration of a highly-sensitive intensity-interrogated optical sensor based on cascaded III-V semiconductor Fabry-Perot laser and silicon-on-insulator ring resonator. The low-cost easy-to-fabricate Fabry-Perot laser serves as a reference comb for the sensing ring in contact with liquid sample. The Vernier effet has been exploited in the detection scheme using intensity interrogation mode. The sharp emission peaks of the FP laser with high spectral power density result in a high sensitivity for the sensor compared to previously investigated all-passive double-ring sensor. The temperature compensation method has also been investigated numerically to improve the performance of the sensor. Concerning the potential monolithic integration of laser and sensing waveguide, the interface between oxide and non-oxide after wet oxidation of buried AlGaAs has been investigated at the Technology Centre of LPN/CNRS. The vertical oxidation of GaAs or AlGaAs with low Al content activated by a neighbouring oxidized Al-rich AlGaAs layer has been discovered experimentally. To limit the vertical oxidation and reduce the roughness of the interface, the waveguides with buried oxide layer on superlattice sample and standard sample have been fabricated and characterised. The key role of hydrogen incorporation in the activation of the oxidation process for GaAs or AlGaAs materials with low Al content has been shown experimentally. Finally, this thesis reports the fabrication and the characterisation results of a Fabry-Perot laser working on TM mode which is an important building block for highly-sensitive monolithically-integrated circuit.

In schwach gekoppelten Halbleiterübergittern können die Elektronen resonant von dem untersten Subband eines Quantentopfes in verschiedene höhere Subbänder des benachbarten Topfes durch die Potenzialbarriere tunneln. In stark dotierten Übergittern kann sich eine Ladungsakkumulationsschicht im Übergitter ausbilden, die es in zwei Felddomänen mit verschiedenen Feldstärken teilt. Aus der detaillierten Untersuchung des Stromverhaltens bei schnellen Spannungsänderungen konnten wichtige Erkenntnisse über die Dynamik der Akkumulationsschicht gewonnen werden, die zum besseren Verständnis von selbstgenerierten Stromoszillationen beitragen. Die beobachteten Stromoszillationen liegen in einem Frequenzbereich von einigen hundert kHz bis zu einigen GHz. Es werden zwei Oszillationsmoden ausführlich beschrieben und gezeigt, wie man sie unterscheiden kann. Die erste Mode tritt bei Proben mit einer gut leitenden Kontaktschicht und moderater Dotierung auf, bei denen die Feldverteilung im Übergitter instabil ist. Die zweite Mode kann dagegen auch bei stark dotierten Übergittern auftreten. Die Voraussetzung ist, dass die Emitterkontaktschicht einen genügend großen spezifischen Widerstand besitzt. Mit dem dargestellten Escape-Time-Modell kann man aus den Übergitterparametern die Oszillationsfrequenzen und die zu erwartenden Stromdichten in den verschiedenen Plateaus abschätzen. Weiterhin wird gezeigt, wie sich die äußere Beschaltung auf die Eigenschaften auswirkt. Durch den Einbau des Übergitters in einen Resonator können diskrete Frequenzen mit einem konstanten Frequenzabstand erzeugt werden. In der Arbeit wird auch der Einfluss von DX-Zentren in den Kontaktschichten beschrieben, welche die Eigenschaften der Proben bei tiefen Temperaturen stark beeinträchtigen können. Durch die Verbesserung der Probeneigenschaften oszilliert der Strom in den Übergittern auch bei Raumtemperatur. Die Frequenz ist mit Hilfe der angelegten Spannung innerhalb eines Plateaus kontinuierlich um bis zu einem Faktor vier durchstimmbar. Es wird die Verwendung von Oszillatoren, basierend auf schwach gekoppelten Halbleiterübergittern, als Bauelement für die Nachrichtenübermittlung vorgeschlagen. / In weakly coupled semiconductor superlattices, the electrons can resonantly tunnel from the first subband of a quantum well into a higher subband of the adjacent well. In highly doped superlattices, a charge accumulation layer can be formed, which divides the superlattice in two field domains of different field strengths. From detailed investigations of the current transients after fast voltage switches, one can obtain important insights into the dynamics of the accumulation layer, which is important for the understanding of self-sustained current oscillations. The frequencies of the resulting current oscillations of the investigated samples are in the range between several hundred kHz and a few GHz. Two possible oscillation modes and their identification from the oscillation characteristics are described. The first mode is observed in samples with contacts with a small resistance and moderately doped superlattices with an unstable field distribution. The second mode appears, if the resistance of the emitter contact layer is sufficiently large and a depletion layer can be injected. A semiclassical model is introduced for the estimation of the oscillation frequencies and the current density in the different plateaus from the superlattice parameters. Finally, the influence of the electrical circuit on the properties of the oscillations will be shown. If the superlattice is put into a resonator, discrete frequencies with constant distances are observed. In this thesis also the influences of DX-centers in the contact layers are described, which can significantly alter the properties of the samples at low temperatures. By applying a larger voltage or by illumination, the contact resistance can be recovered to a common value. Due to the improvement of the sample parameters, the samples also oscillate at room temperature and above. The frequency within a plateau is continuously tunable by a factor of two to four. An application as a tunable oscillator device for wireless and optical communication is proposed.

This thesis, submitted to the University of Manchester, covers a range of topics related to current research in two-dimensional materials under the title: 'Investigations into the interfacial interaction of graphene with hexagonal boron nitride.'In the last decade, two-dimensional materials have become a rich source of original research and potential applications. The main advantage lies in the ability to produce novel composite structures, so-called 'layered heterostructures', which are only a few atomic layers thick. One can utilise the unique properties of several species of crystal separately, or how they interact to realise a diverse range of uses. Two such crystals are graphene and hexagonal boron nitride. Hexagonal boron nitride has, so far, been used primarily as a substrate for graphene, allowing researchers to get the most out of graphene's impressive individual properties. However, in this thesis, the non-trivial van der Waals interaction between graphene and hexagonal boron nitride is examined. The interface potential reveals itself as a relatively large-scale, orientation-dependant superlattice, which is described in chapters 1 and 2.I In Chapter 4, the effect of this superlattice is examined by measurement of its effect upon the electrons in graphene, where its modulation leads to the creation of second and third generation Dirac points, revealing Hofstadter's Butterfly. As well as an excellent example of the physics possible with graphene, it also presents a new tool with which to create novel devices possessing tailored electronic properties. II In chapter 5, the consequential effect of the superlattice potential on the structure of graphene is studied. Results are discussed within the framework of the Frenkel-Kontorova model for a chain of atoms on a static background potential. Results are consistent with relaxation of the graphene structure leading to the formation of a commensurate ground state. This has exciting consequences for the production of heterostructures by demonstrating that alignment angle can have large effects upon the physical properties of the crystals. III In chapter 6, the van der Waals potential is shown to be responsible for the self-alignment of the two crystals. This effect is important for the fabrication of perfectly aligned devices and may lead to new applications based on nanoscale motion.

Dans le domaine de la photodétection infrarouge (IR) haute performance refroidie, le photodétecteur à superréseaux (SR) InAs/GaSb est une filière émergente qui peut compléter les technologies déjà établies. Grâce à des années de recherche, l'Institut d'Electronique du Sud (IES) de l'Université de Montpellier a développé une expertise sur la croissance du matériau SR InAs/GaSb par épitaxie par jets moléculaires et sur la fabrication technologique des photodiodes pin dont les performances sont à l'état de l'art mondial dans le moyen IR (3-5µm). Au cours de cette thèse, nous avons étudié deux périodes différentes de SR comme zone active de photodiodes pin ayant une longueur d'onde de coupure à 5 µm à 80K : une riche en InAs (InAs-rich) et l'autre riche en GaSb (GaSb-rich). Ces structures SR présentent des caractéristiques électriques et électro-optiques très différentes. Notamment, les densités de courant de la structure InAs-rich sont très bonnes, de l'ordre de 10-8A/cm2 à 80K, alors que celles de la structure GaSb-rich sont deux décades plus élevées. L'objectif de cette thèse était donc d'analyser les performances de ces photodiodes. Pour cela, nous avons développé une méthode de simulation avec l'outil TCAD SILVACO. Appliquée tout d'abord aux structures InAs-rich, nous avons mis en évidence que ces diodes sont limitées à basse température (typiquement < 120K) par le courant de génération-recombinaison et/ou par le courant tunnel assisté par pièges. La durée de vie extraite de la simulation suit une variation en T-1/2, démontrant que les mécanismes limitant les photodiodes est la génération-recombinaison SRH. Appliquée aux structures GaSb-rich, l'approche SILVACO ne peut expliquer les résultats en courant. Nous démontrons que ces résultats sont fortement liés à la présence du champ électrique dans la zone d'absorption du composant. Cela génère à faible polarisation, un fort courant tunnel, au travers des états Wannier-Stark localisés, qui pénalise fortement le courant d'obscurité et cela malgré des améliorations obtenues au niveau du matériau. Pour finir, nous établissons des règles de dimensionnement de structures à barrière et nous proposons une structure à SR pour le lointain infrarouge. / Among the high performance cooled infrared (IR) photodetector systems, the InAs/GaSb superlattice (SL) is an emerging material which may complement the currently technologies already established. Over the last 10 years, the Institut d'Electronique du Sud (IES) of the University of Montpellier has developed skills in both the growth of SL materials by molecular beam epitaxy and the process fabrication of pin photodiodes. The photodiode fabricated by the IES group are at the state of the art in the mid IR (3 – 5 μm). During this thesis, we studied two structures with different SL periods for the pin active zone showing the same cut-off wavelength of 5 μm at 80K: the structure called InAs-rich structure presents InAs layer thicker than the GaSb layer in each SL period while this configuration is reversed in the case of the GaSb-rich structure. These SL structures have very different electrical and electro-optical characteristics. In particular, the current densities of the InAs-rich structure are very good, about 10-8 A/cm2 at 80K - two orders of magnitude greater than that of GaSb-rich. The aim of this thesis work was therefore to analyze the performance of these photodiodes. For this purpose, we developed a simulation method with the SILVACO TCAD tool. Using this tool, we found that the InAs-rich diodes are limited at low temperatures (typically under 120K) by generation recombination and/or by assisted tunneling currents. The lifetimes extracted from the simulation follows the T-1/2 law, which demonstrates that the limiting mechanism is SRH recombination. However, we found that we could not study the current densities of the GaSb-rich structure using the same procedure. We demonstrate that these results are strongly related to the presence of the electric field in the absorption zone of the device. This electric field generates, at low biases, a strong tunneling current through localized Wannier-Stark states, which strongly limits the overall current despite material improvements. Finally, we define the design conditions to achieve an optimized SL barrier structure and propose a design for SL structures targeting the long wavelength domain.

<p>In the first part of this work, the influence of hydrogen on the structural and magnetic properties of Fe/V(001) superlattices was studied. The local structure of the vanadium-hydride layers was determined by extended x-ray absorption fine structure (EXAFS) measurements. The magnetic ordering in a weakly coupled Fe/V(001) superlattice was investigated using the magneto-optical Kerr effect (MOKE). The interlayer exchange coupling is weakened upon alloying with hydrogen and a phase with short-range magnetic order was observed.</p><p>The second part is concerned with first-principles calculations of magnetic materials, with a focus on magnetic recording applications. The uniaxial magnetic anisotropy energy (MAE) of Fe, Co, and Ni was calculated for tetragonal and trigonal structures. Based on an analysis of the electronic states of tetragonal Fe and Co at the center of the Brillouin zone, tetragonal Fe-Co alloys were proposed as a material that combines a large uniaxial MAE with a large saturation magnetization. This was confirmed by experimental studies on (Fe,Co)/Pt superlattices. The large uniaxial MAE of L1₀ FePt is caused by the large spin-orbit interaction on the Pt sites in connection with a strong hybridization between Fe and Pt. Furthermore, it was shown that the uniaxial MAE can be increased by alloying the Fe sublattice with Mn. The combination of the high-moment rare-earth (RE) metals with the high-<i>T</i>_C 3<i>d</i> transition metals in RE/Cr/Fe multilayers (RE = Gd, Tb, Dy) gives rise to a strong ferromagnetic effective exchange interaction between the Fe layers and the RE layer. The MAE of hcp Gd was found to have two principal contributions, namely the dipole interaction of the large localized 4<i>f</i> spins and the band electron magnetic anisotropy due to the spin-orbit interaction. The peculiar temperature dependence of the easy axis of magnetization was reproduced on a qualitative level.</p>

Properties of magnetic thin film devices cannot be understood without detailed knowledge of their structure. For this purpose, a variety of thin film and multilayer systems have been studied. Both reciprocal space (low energy electron diffraction, reflection high energy electron diffraction, X-ray diffraction and reflectometry) and direct space (transmission electron microscopy) as well as Rutherford backscattering spectrometry have been applied. To gain understanding of an oxidation procedure for the growth of magnetite layers, thermal stability of iron layers on molybdenum seed layers has been investigated. Following the mosaicity and the out-of-plane coherence length over different ratios between the constituting layers allowed a deeper understanding of the limits of metallic superlattices. This, together with an approach to use hydrogen in the process gas during magnetron sputter epitaxy, opens routes for the growth of metallic superlattices of superior quality. A non-isostructural multilayer/superlattice system, Fe/MgO, has been investigated. In turn, this gave more understanding how superlattice diffraction patterns are suppressed by strain fields. As an alternative route to single-crystalline superlattices, amorphous multilayers present interesting opportunities. In this context, crystallization effects of iron/zirconium layers on alumiunium oxide were studied. Understanding these effects enables significant improvement in the quality of amorphous multilayers, and allows avoiding these, growing truly amorphous layers. Both the substantial improvement in quality of metallic superlattices, approaching true single-crystallinity, as well as the improvements in the growth of amorphous multilayers give rise to opportunities in the field of magnetic coupling and superconducting spin valves.

Mg-based alloys form a variety of interesting structures including stable and metastable crystalline, stable and metastable quasicrystalline, nanocrystalline and amorphous phases. Many of these phases can be made to coexist by suitable processing leading to an interesting combination of properties. Non-equilibrium processing in combination with suitable heat treatments can be used to control the scale and dispersion of these phases. Further thrust to Mg-based alloys is expected through the development of Mg-based bulk metallic glasses. Magnesium matrix composites are also gaining in prominence. The thesis has been divided into theoretical and experimental parts. The theoretical part focuses on understanding the structure of quasicrystals, rational approximants and related structures. The experimental work involves synthesis, non-equilibrium processing and characterization of specific Mg-based alloys. The structure of quasicrystals and related structures can be understood by working in three dimensions or by projection from higher dimensions. The projection formalism is used to generate quasicrystals and rational approximants in 2D and 3D. Approximants to the Penrose lattice are generated with directions of approximation oriented 90° and 72° apart. Rational approximants to the icosahedral quasilattice are generated and the systematics of lattice-centring in these approximants analysed. Two-dimensional quasiperiodic lattice with 5-fold symmetry, which is periodic along the third dimension, is generated as an approximant to the icosahedral lattice. Approximants are also considered wherein quasiperiodicity is retained along one or two directions. The concept of average lattices can be used to understand diverse structures including vacancy ordered phases (VOP) and orthorhombic approximants to the decagonal phase. VOP which lack incommensurate length scales should be considered as quasiperiodic superlattice (QPSL) approximants rather than as conventional rational approximants and hence have the average lattice scheme built into them. The average lattice approach is further used to unify Kuo’s and Anantharaman's models for orthorhombic approximants to the decagonal quasicrystal. A modified version of Anantharaman's model is also presented. Using the twinned icosahedron model, Robinson and Taylor approximants to the decagonal quasicrystal are generated by the twinning of Mackay and Little approximants to the icosahedral quasicrystal. An indexing scheme based on this model is developed which inherits the merits of the twinned icosahedron model. Further, using cluster of four icosahedra, in a distorted tetrahedral configuration, symmetries of the hexagonal phases, which are related to quasicrystals, are generated. Frank's ratio is brought out as a unifying thread connecting diverse kinds of structures including VOP and hexagonal phases related to quasicrystals, which have pseudocubic symmetry. Experimental work involves the synthesis and characterization of alloys in four systems: a) Mg-Zn-Y, b) Mg-Zn-La, c) Al-Mg-Cu and d) Mg-Cu-Y. Induction melting is used to prepare the alloys and melt-spinning is used as the primary non-equilibrium processing route. The focus in the Mg-Zn-RE systems is in the as cast condition while in the Al-Mg-Cu system it is in the melt-spun condition. Characterization techniques used are XRD, SEM and TEM. In the Mg-Zn-Y system face-centred icosahedral (FC1) phase with quasilattice parameter of 5.21 A is found to coexist with related crystalline phases in the Mg4Zn94Y2 and Mg23Zn5gY9 alloys. A series of crystalline phases with superlattice ordering are seen in the Mg-Zn-Y and Mg-Zn-La systems. These phases with a variety of ordering, many of which display interesting patterns of streaking in the SAD pattern, are related to one-another and to the FCI QC found in the Mg-Zn-Y system. No quasicrystal could be observed in the two alloys investigated in the Mg-Zn-La system with La = 5 and 8 %. Conventional rational approximants were conspicuous by there absence in both the rare-earth containing systems. This is understood in terms of the absence of large clusters in these systems. High Y alloys display a tendency to form nanocrystals in the as-cast condition and amorphous regions are observed in the as-cast alloys with Y > 20 %. Hence, high Y alloys are anticipated to be bulk glass formers. Melt-spinning of the alloys in both the RE containing systems lead to the formation of nanocrystalline regions. The e/a ratio plays an important role in the formation of phases in the Mg-Zn-Y system. An e/a ratio near 2.08 has a stabilising effect on a variety of phases including the FCI quasicrystal, ternary phases related to the quasicrystal and binary phases like YZn12 and Y2Zn17. Formation of quasicrystals in the Al-Mg binary and Mg-Al-Cu ternary seem to be very sensitive to processing conditions and were not observed in the present investigation in the melt-spun alloys. However, β-Al3Mg2 and Mg32(Al,Cu)49 phases with large lattice parameters, which are related to quasicrystals, are observed in as-cast and melt-spun conditions. The Mg32(Al,Cu)49 phase brings out the similarity between this system and the Mg-Al-Zn system. The glass formability of the alloys in the Al-Mg binary and in the Mg-Al-Cu ternary is limited. Except for the formation of amorphous phase in some regions, the alloys were crystalline even when melt-spun at 2800 rpm. The ability to form nanocrystals is also limited in this system as compared to the Mg-Zn-RE systems. Often melt-spun alloys showed a wide range of grain sizes coexisting together.