Le travail de thèse présenté dans ce manuscrit traite du développement de dispositifs à base de dioxyde de vanadium VO₂ et de méta-surfaces dans le moyen infrarouge pour des applications passives et une intégration sur des lasers à cascade quantique (QCL). Ce travail a permis l'élaboration de nouvelles conditions de dépôt du matériau à changement de phase VO₂ par ablation laser pulsé à des températures compatibles avec les hétérostructures de III-V utilisées en optoélectronique. Les caractérisations des couches minces déposées montrent un changement de la réflectivité et de la conductivité électrique entre l'état isolant à basse température et l'état métallique à haute température autour de 68°C (341 K). Des développements ont ensuite été menés sur l'emploi d'un réseau de méta-surfaces permettant d'obtenir une couche homogène d'indice de réfraction effectif résonnant. Ces méta-surfaces sont constituées de résonateurs à anneau fendu dont la fréquence de résonance peut être ajustée par le choix de leurs paramètres géométriques et des matériaux les constituant. Une modulation optique de plus de 100cm-1 du pic de la résonance a été obtenue lors de la transition de phase avec des méta-surfaces déposées sur un film de VO₂. Ce résultat est très prometteur pour la conception de dispositifs monolithiques, robustes, compacts, accordables en fréquence et dont les propriétés optiques ne dépendent que de la température de la couche de VO₂.Enfin, ce travail étudie la fonctionnalisation des QCL dans le moyen infrarouge (7-8 µm) par des couches de VO₂ et de méta-surfaces. Il vise à comprendre l’influence des couches intégrées sur les propriétés d’émission. Afin de garantir une bonne interaction entre ces couches et le mode guidé du laser tout en ayant des pertes optiques faibles, des nouveaux guides d'onde ont été modélisés, puis les premiers QCL à base de VO₂ ont été démontrés et une température maximale de fonctionnement de 334 K a été mesurée. / The thesis work presented in this manuscript deals with the development of vanadium dioxide VO₂ and meta-surfaces based devices in the mid-infrared for passive applications and an integration on quantum cascade lasers (QCL).This work enabled the elaboration of new deposition conditions for the VO₂ phase change material by pulsed laser ablation at temperatures compatible with III-V heterostructures used in optoelectronics. The characterizations of the VO₂ coated thin films show a change in reflectivity and in electric conductivity between the insulating state at low temperature and the metallic state at high temperature around 68°C (341 K).Developments were then carried out on the use of a meta-surfaces array in order to obtain an homogeneous layer of resonant effective refractive index. These meta-surfaces are constituted by split-ring resonators, whose resonance frequency can be adjusted by choosing their geometric parameters and the materials they are made of. An optical modulation of more than 100cm-1 of the resonance peak has been obtained during the phase transition with meta-surfaces deposited on a VO₂ layer. This result is very promising for the conception of monolithic, robust, compact, frequency tunable devices and whose optical properties only depend on the VO₂ layer temperature.Finally, this work studies the functionalization of mid-infrared QCL (7-8 µm) with VO₂ and meta-surfaces layers. It aims at understanding the influence of the integrated layers on the emission properties. In order to ensure a good interaction between these layers and the laser guided mode while having low optical losses, new waveguides were modeled, then the first VO₂ based QCL have been demonstrated and a maximum operating temperature of 334 K has been measured.

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<p>This dissertation presents research work related to laser micro sintering, laser micro machining and laser-induced plasma. Firstly, we present extensive experimental studies of double-pulse laser micro sintering (DP-LMS), which typically utilizes the high pressure generated by laser-induced plasma over the powder bed surface to promote molten flow and enhance densification. Chapter 2 shows a single-track experimental study of the DP-LMS process using cobalt powder. The related fundamental mechanisms and effects of different laser parameters on the sintering results are analyzed with the help of <em>in-situ</em> time-resolved temperature measurements. Chapter 3 shows a multi-track experimental study of the DP-LMS process using iron powder. The sintered materials are characterized via the top surface porosity, elemental composition, grain microstructure, nanohardness and metal phase. Three strategic guidelines for laser parameter selection are summarized in the end. Chapter 4 shows time-resolved imaging and OES measurements for plasma induced during DP-LMS. The plasma temperature and free electron number density are deduced by its optical emission spectra (OES). These three chapters have clearly demonstrated DP-LMS can produce much more continuous and densified materials than LMS only using the sintering or pressing laser pulses.</p> <p><br></p> <p>Then, we present laser micro grooving of silicon carbide (SiC) in Chapter 5 by ultrasound-assisted water-confined laser micromachining (UWLM), in comparison with laser machining in water without ultrasound and laser machining in air. UWLM applies <em>in-situ</em> ultrasound to the water-immersed workpiece surface to improve the machining quality and/or productivity. Time-resolved water pressure measurements are carried out to help analyze relevant mechanisms. It has been demonstrated UWLM can be a competitive approach to produce high-quality micro grooves on SiC. The crack problem appears to be effectively solved using a high pulse repetition rate.</p> <p><br></p> <p>Finally, we report a double-front phenomenon for plasma induced by high-intensity nanosecond laser ablation of aluminum in Chapter 6. An additional plasma front is observed via an intensified CCD (ICCD) camera, which propagates very fast at the beginning but stops propagating soon after the laser pulse mostly ends. Its formation could be caused by the inverse bremsstrahlung absorption of laser energy by the ionized ambient gas. Three possible mechanisms on how the ambient gas breakdown is initiated are proposed. </p>

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<p dir="ltr">Metamaterials are artificially engineered nanoscale systems with a three-dimensional repetitive arrangement of certain components, and present exceptional optical properties for applications in nanophotonics, solar cells, plasmonic devices, and more. Self-assembled oxide-metal vertically aligned nanocomposites (VANs), with metallic phase as nanopillars embedded in the matrix oxide, have been recently proposed as a promising candidate for metamaterial applications. However, precise microstructural control and the structure-property relationships in VANs are still in high demand. Thus, by employing multiple approaches for structural design, this dissertation attempts to investigate the mechanisms of nanostructure evolutions and the corresponding optical responses.</p><p dir="ltr">In this dissertation, the precise control over the nanostructures has been demonstrated through morphology tuning, nanopillar orderings, and strain engineering. Firstly, Au, a well-known plasmonic mediator, has been selected as the metallic phase that forms nanopillars. Based on the previously proposed strain compensation model which describes the basic formation mechanism of VAN morphology, two oxides were then considered: La_0.7Sr_0.3MnO₃(LSMO) and CeO₂. In the first two chapters of this dissertation, LSMO was considered due to its similar lattice (a_LSMO= 3.87 Å, a_Au= 4.08 Å) and its enormous potential in nanoelectronics and spintronics. Deposited on SrTiO₃ (001) substrate through pulsed laser deposition (PLD), LSMO-Au nanocomposites exhibit ideal VAN morphology as well as promising hyperbolic dispersions in response to the incident illuminations. By substrate surface treatment of annealing at 1000°C, and variation of STO substate orientations from (001), to (111) and (110), the improved and tunable in-plan orderings of Au nanopillars have been successfully achieved. In the third chapter, a new oxide-metal VAN system of <a href="" target="_blank">CeO₂</a>-Au (a_CeO2= 5.411 Å, and a_CeO2/= 3.83 Å) has been deposited. The intriguing 45° rotated in-plan epitaxy presents an unexpected update to the strain compensation model, and tuning of Au morphology from nanopillars, nanoantennas, to nanoparticles also shows an effective modulation of the LSPR responses. COMSOL simulations have been exploited to reveal the relationships between Au morphologies and optical responses. In the last chapter, the two VAN systems of LSMO-Au and CeO₂-Au have been combined to form a complex layered VAN thin film. Investigations into the strain states, the nature of complex interfaces, and the according hybrid properties, show dramatic possibilities for further strain engineering. In summary, this dissertation has provided multiple routes for highly tailorable oxide-metal nanocomposite designs. And the two proposed material systems present great potential in optical metamaterial applications including biosensors, photovoltaics, super lenses, and more.</p>

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Within the framework of this thesis, the influence of non equilibrium post growth thermal treatments of ion implanted and epitaxially grown Ge1-xSnx and Si1-x-yGeySnx layers for nano and optoelectronic devices has been investigated. The main focus has been placed on the study and development of thermal treatment conditions to improve the as grown layer quality and the fabrication of Ge1-xSnx and Si1-x-yGeySnx on SOI JNTs. In addition, through layer characterization, exhaustive analysis has provided deep insight into key material properties and the alloy´s response to the thermal treatment. For instance, (i) the conversion of as grown in plane compressive strained Ge1-xSnx into in-plane tensile strained Ge1-xSnx after PLA that is required for high mobility n-type transistors and (ii) the evolution of monovacancies to larger vacancy clusters due to post growth thermal treatments. Moreover, the adaption of CMOS compatible fabrication approaches to the novel Ge1-xSnx and Si1-x-yGeySnx alloys allowed the successful fabrication of first lateral n-type JNTs on SOI with remarkable Ion/Ioff ratios of up to 10^8 to benchmark the alloy performance.:I. Table of contents II. Abstract III. Kurzfassung (Abstract in German) IV. List of Abbreviations V. List of Symbols VI. List of Figures VII. List of Tables 1 Introduction 2 Fabrication and properties of Ge1 xSnx and Si1 x yGeySnx alloys 2.1 Alloy formation 2.2 Strain and defects 2.3 Electrical and optical properties 2.3.1 Band structure of strain relaxed alloys 2.3.2 Band structure of strained alloys 2.3.3 Doping influenced properties 2.3.4 Electrical properties 2.4 Thermal treatments 2.4.1 Rapid thermal annealing 2.4.2 Flash lamp annealing 2.4.3 Pulsed laser annealing 2.5 Summary 3 Experimental setups 3.1 Molecular beam epitaxy (MBE) 3.2 Ion beam implantation 3.3 Pulsed laser annealing (PLA) 3.4 Flash lamp annealing (FLA) 3.5 Micro Raman spectroscopy 3.6 Rutherford backscattering spectrometry (RBS) 3.7 X ray diffraction (XRD) 3.8 Secondary ion mass spectrometry (SIMS) 3.9 Hall effect measurement 3.10 Transmission electron microscopy (TEM) 3.11 Positron annihilation spectroscopy (PAS) 3.12 Cleanroom 4 Post growth thermal treatments of Ge1-xSnx alloys 4.1 Post growth pulsed laser annealing 4.1.1 Material fabrication and PLA annealing 4.1.2 Microstructural investigation 4.1.3 Strain relaxation and optical properties 4.1.4 Electrical properties and defect analysis 4.1.5 Strain relaxed Ge1-xSnx as virtual substrates 4.1.6 Conclusion 4.2 Post growth flash lamp annealing 4.2.1 Material fabrication and r FLA annealing 4.2.2 Alloy composition and strain analysis 4.2.3 Defect investigation 4.2.4 Dopant distribution and activation 4.2.5 Conclusion 5 Fabrication of Ge1-xSnx and Si1-x-yGeySnx alloys on SOI 5.1 Alloy fabrication with ion beam implantation and FLA 5.1.1 Si1-x-yGeySnx formation via implantation and FLA 5.1.2 Si1-x-yGeySnx on SOI fabrication via implantation and FLA 5.1.3 Recrystallization of Si1-x-yGeySnx on SOI by FLA 5.1.4 P and Ga doping of Si1 x yGeySnxOI via implantation and FLA 5.1.5 Conclusion 5.2 MBE and post growth thermal treatments of Ge1-xSnx and Si1-x-yGeySnx on SOI 5.2.1 MBE growth of Ge0.94Sn0.06 and Si0.14Ge0.80Sn0.06 on SOI 5.2.2 Microstructure of as grown Ge0.94Sn0.06 and Si0.14Ge0.80Sn0.06 5.2.3 Microstructure after post growth thermal treatments 5.2.4 Dopant concentration and distribution 5.2.5 Conclusion 6 Ge1-xSnx and Si1-x-yGeySnx on SOI junctionless transistors 6.1 Operation principle of n type JLFETs 6.2 Fabrication of n-type JNTs 6.3 Electrical characterization 6.3.1 JNT performance evolution during processing 6.3.2 JNT performance in dependence on post growth PLA 6.3.3 Gate configuration of Ge1-xSnx JNTs 6.3.4 Influence of post fabrication FLA on Ge1-xSnx JNTs 6.4 Conclusion 7 Conclusion and future prospects References 8 Appendix 8.1 Sample list and fabrication details for Chapter 4 8.2 Extended RBS information 8.3 Extended TEM analysis for section 4.1.2 8.4 Strain calculation based on (224) RSM 8.5 Strain calculation by µ Raman 8.6 Analysis of Hall effect measurements 8.7 VEPFit and ATSUP simulations 8.8 Strain relaxation of Ge0.89Sn0.11 for section 4.1.5 8.9 COMSOL simulation of FLA temperature 8.10 ECV measurement setup 8.11 Datasheet of the SOI wafers 8.12 Sample list of Chapter 5 8.13 Calculation of the ion beam implantation parameter by SRIM 8.14 RBS simulation results for section 5.1 8.15 GI XRD and (224) XRD RSM results for section 5.1 8.16 SIMS limitations for section 5.1.4 8.17 RBS of Ge1-xSnx on SOI for section 5.2.3 8.18 Fit procedure for SOI RSM peak positions 8.19 Supporting µ Raman results for section 5.2.3 8.20 Process details for n-JNT fabrication 8.21 Flat band voltage VFB and on current Ion of JNTs 8.22 Ioff, Imax, Ion/Ioff and Imax/Ioff ratio of JNTs 8.23 Subthreshold swing SS calculation of JNTs 8.24 Threshold voltage Vth of JNTs 187 8.25 Gate configuration of Si1-x-yGeySnx JNTs 8.26 n-type transistors compared in Chapter 7 8.27 Annealing setup description

Die vorliegende Arbeit befasst sich mit der Untersuchung von Schottky-Kontakten auf halbleitenden Zinkoxid- und β-Galliumoxid-Dünnfilmen. Nach einer kurzen Einführung in die verwendeten Materialsysteme und die Theorie von Schottky-Kontakten werden die Eigenschaften von verschiedenartig hergestellten Schottky-Kontakten auf Zinkoxid aufgezeigt. Dazu werden typischerweise Strom-Spannungs- und Kapazitäts-Spannungs-Messungen genutzt. Für die Zinkoxid-basierten Schottky-Kontakte konnte anhand verschiedenartig hergestellter Schottky-Kontakte gezeigt werden, dass deren Barrierenformation maßgeblich von Sauerstoffvakanzen nahe der Metall-Halbleiter-Grenzfläche beeinflusst wird. Zur Realisierung von Galliumoxid-basierten Schottky-Kontakten wurden zunächst die Eigenschaften von undotierten und Silizium-dotierten Galliumoxid-Dünnfilmen untersucht. Diese Dünnfilme sind mittels gepulster Laserabscheidung auf c-plane Saphir hergestellt. Als Prozessparameter sind in dieser Arbeit die Wachstumstemperatur, der Sauerstoffpartialdruck in der Kammer und der Silizumgehalt bspw. in Bezug auf Leitfähigkeit, Oberflächenmorphologie oder Kristallinität zur Realisierung von Schottky-Kontakten optimiert. Auf diesen Dünnfilmen wurden mit verschiedenen Herstellungsverfahren, wie thermischer Verdampfung, (reaktiver) Kathodenzerstäubung oder (reaktiver) Distanz-Kathodenzerstäubung, Metall- bzw. Metalloxid-Schottky-Kontakte aufgebracht. Dabei werden unter anderem die elektrischen Eigenschaften direkt nach der Herstellung und deren Entwicklung im weiteren zeitlichen Verlauf untersucht. Des Weiteren werden die Temperaturstabilität oder aber die Spannungsstabilität der Schottky-Kontakte studiert. Ein Vergleich zu Schottky-Kontakten auf β-Galliumoxid-Volumenmaterial wird anhand mittels reaktiver Distanz-Kathodenzerstäubung hergestellter Platinoxid-Dioden durchgeführt.

Conventional computing faces a huge technical challenge as traditional transistors will soon reach their size limitations. This will halt progress in reaching faster processing speeds and to overcome this problem, require an entirely new approach. Quantum computing (QC) is a natural solution offering a route to miniaturisation by, for example, storing information in electron or nuclear spin states, whilst harnessing the power of quantum physics to perform certain calculations exponentially faster than its classical counterpart. However, QCs face many difficulties, such as, protecting the quantum-bit (qubit) from the environment and its irreversible loss through the process of decoherence. Hybrid systems provide a route to harnessing the benefits of multiple degrees of freedom through the coherent transfer of quantum information between them. In this thesis I show coherent qubit transfer between electron and nuclear spin states in a ¹⁵N@C₆₀ molecular system (comprising a nitrogen atom encapsulated in a carbon cage) and a solid state system, using phosphorous donors in silicon (Si:P). The propagation uses a series of resonant mi- crowave and radiofrequency pulses and is shown with a two-way fidelity of around 90% for an arbitrary qubit state. The transfer allows quantum information to be held in the nuclear spin for up to 3 orders of magnitude longer than in the electron spin, producing a ¹⁵N@C₆₀ and Si:P ‘quantum memory’ of up to 130 ms and 1.75 s, respectively. I show electron and nuclear spin relaxation (T₁), in both systems, is dominated by a two-phonon process resonant with an excited state, with a constant electron/nuclear T₁ ratio. The thesis further investigates the decoherence and relaxation properties of metal atoms encapsulated in a carbon cage, termed metallofullerenes, discovering that exceptionally long electron spin decoherence times are possible, such that these can be considered a viable QC candidate.