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<p>Ferroelectrics are a group of advanced electronic materialswith a wide variety of properties useful in applications suchas memory devices, resonators and filters, infrared sensors,microelectromechanical systems, and optical waveguides andmodulators. Among the oxide perovskite-structured ferroelectricthin film materials sodium potassium niobate or Na0.5K0.5NbO3(NKN) has recently emerged as one of the most promisingmaterials in microwave applications due to high dielectrictunability and low dielectric loss. This licentiate thesispresents results on growth and structural, optical, andelectrical characterization of Na0.5K0.5NbO3 thin films. Thefilms were deposited by rf-magnetron sputtering of astoichiometric, high density, ceramic Na0.5K0.5NbO3 target ontosingle crystal LaAlO3 and Al2O3, and polycrystalline Pt80Ir20substrates. By x-ray diffractometry, NKN films on c-axisoriented LaAlO3 substrates were found to grow epitaxially,whereas films on hexagonal sapphire and polycrystallinePt80Ir20 substrates were found to be preferentially (00l)oriented. Optical and waveguiding properties of theNa0.5K0.5NbO3/Al2O3 heterostructure were characterized using aprism-coupling technique. Sharp and distinguishable transversemagnetic (TM) and electric (TE) propagation modes wereobserved. The extraordinary and ordinary refractive indiceswere calculated to ne = 2.216±0.003 and no =2.247±0.002 for a 2.0 μm thick film at λ = 632.8nm. This implies a birefringence Δn = ne - no =-0.031±0.003 in the film. The ferroelectric state inNKN/Pt80Ir20 films at room temperature was indicated by apolarization loop with polarization as high as 33.4 μC/cm2at 700 kV/cm, remnant polarization of 9.9 μC/cm2 andcoercive field of 91 kV/cm. Current-voltage characteristics ofvertical Au/NKN/Pt80Ir20 capacitive cells and planar Au/NKN/LaAlO3 interdigital capacitors (IDCs) showed very goodinsulating properties, with the leakage current density for anNKN IDC on the order of 30 nA/cm2 at 400 kV/cm. Rf dielectricspectroscopy demonstrated low loss, low frequency dispersion,and high voltage tunability. At 1 MHz NKN/LaAlO3 showed adissipation factor tan δ of 0.010 and a tunability of 16.5% at 200 kV/cm. For the same structure the frequencydispersion, Δεr, between 1 kHz and 1 MHz was 8.5%.</p><p><b>Key words:</b>ferroelectrics, sodium potassium niobates,thin films, rf-magnetron sputtering, waveguiding, refractiveindex, prism coupling, dielectric tunability</p>

Owing to the large electric-field-dependent permittivity, ferroelectric thin films have attracted a great deal of attention on applications in miniature tunable microwave components with high performance and cost reduction, such as phase shifters, tunable oscillators, delay lines, and antennas. These tunable devices require large change in the dielectric constant with applied field and a low loss at microwave frequencies. As one of the promising ferroelectric materials, barium strontium titanate thin film, especially Ba0.5Sr0.5TiO3 (BST) films, have raises great research interests due to its high dielectric constant, which is tunable in an external electric field, combined with relative low loss at microwave frequencies. Tunable microwave components, such as phase shifter, based on the BST films have been widely investigated. Since the polarization, the significant characterization of ferroelectrics, is very sensitive to distortion in crystal structure of ferroelectrics, strain can be effectively utilized to tailor the dielectric properties of BST films. Due to the lattice-mismatch from the substrate and various deposition conditions, epitaxial BST thin film usually contains residual strain generated during film growth. Strain control by improved deposition technique and implementing thermal treatment as well as choosing suitable substrate has attracted intensive attentions in ferroelectric film fabrication. Theory predicts that high dielectric properties can be achieved when free strain or slightly tensile strain left in the BST thin film at room temperature. Microwave application, such as phase shifter, also expects the enhanced tunability by an applied electric field. In this dissertation, single crystalline BST thin films deposited by radio frequency magnetron sputtering on SrTiO3 and DyScO3 substrates were studied. The crystal structure characteristics, including lattice parameters and film strain, were determined using X-ray diffraction. A new growth technique, three-step technique, was introduced and implemented into BST thin film deposition. The application of this new technique in deposition dramatically reduced the compressive strain in the films. We use microwave measurements on coplanar waveguides to evidence the improvement on dielectric properties achieved by tailoring the film strain. Additionally, we studied the BST film deposited by pulsed laser deposition (PLD) with introducing a sputtered seed layer of BST thin film. Compared with the BST film directly deposited on the substrate by PLD deposition, the films with a seed layer showed a large enhancement on the dielectric constant and tunability. The discussion on the change in film strain and dielectric performance of the PLD deposited films further proved the influence of film strain on dielectric properties. We discussed the design, fabrication, and measurement of coplanar waveguide transmission lines as phase shifters fabricated BST films. The thin BST films (~700 nm) on DyScO3 substrates deposited by sputtering demonstrated that the three-step deposition technique improved differential phase shift and microwave figure of merit to a great extent. The introduction of the sputtered seed layer into the PLD deposition of a thicker BST film (~2.15 μm) showed a dramatically enhancement on differential phase shift and microwave figure of merit. The enhanced performance on different series of BST films in microwave frequencies is consistent with the improvement on crystal structure, especially with the change in film strain.

Ferroelectrics are a group of advanced electronic materialswith a wide variety of properties useful in applications suchas memory devices, resonators and filters, infrared sensors,microelectromechanical systems, and optical waveguides andmodulators. Among the oxide perovskite-structured ferroelectricthin film materials sodium potassium niobate or Na0.5K0.5NbO3(NKN) has recently emerged as one of the most promisingmaterials in microwave applications due to high dielectrictunability and low dielectric loss. This licentiate thesispresents results on growth and structural, optical, andelectrical characterization of Na0.5K0.5NbO3 thin films. Thefilms were deposited by rf-magnetron sputtering of astoichiometric, high density, ceramic Na0.5K0.5NbO3 target ontosingle crystal LaAlO3 and Al2O3, and polycrystalline Pt80Ir20substrates. By x-ray diffractometry, NKN films on c-axisoriented LaAlO3 substrates were found to grow epitaxially,whereas films on hexagonal sapphire and polycrystallinePt80Ir20 substrates were found to be preferentially (00l)oriented. Optical and waveguiding properties of theNa0.5K0.5NbO3/Al2O3 heterostructure were characterized using aprism-coupling technique. Sharp and distinguishable transversemagnetic (TM) and electric (TE) propagation modes wereobserved. The extraordinary and ordinary refractive indiceswere calculated to ne = 2.216±0.003 and no =2.247±0.002 for a 2.0 μm thick film at λ = 632.8nm. This implies a birefringence Δn = ne - no =-0.031±0.003 in the film. The ferroelectric state inNKN/Pt80Ir20 films at room temperature was indicated by apolarization loop with polarization as high as 33.4 μC/cm2at 700 kV/cm, remnant polarization of 9.9 μC/cm2 andcoercive field of 91 kV/cm. Current-voltage characteristics ofvertical Au/NKN/Pt80Ir20 capacitive cells and planar Au/NKN/LaAlO3 interdigital capacitors (IDCs) showed very goodinsulating properties, with the leakage current density for anNKN IDC on the order of 30 nA/cm2 at 400 kV/cm. Rf dielectricspectroscopy demonstrated low loss, low frequency dispersion,and high voltage tunability. At 1 MHz NKN/LaAlO3 showed adissipation factor tan δ of 0.010 and a tunability of 16.5% at 200 kV/cm. For the same structure the frequencydispersion, Δεr, between 1 kHz and 1 MHz was 8.5%. <b>Key words:</b>ferroelectrics, sodium potassium niobates,thin films, rf-magnetron sputtering, waveguiding, refractiveindex, prism coupling, dielectric tunability / NR 20140805

To date, the search efforts have shifted from the toxic II-VI, III-V and IV-VI semiconductors to more environmentally friendly materials. Among Group II-V semiconductors, Zn3P2 has shown to be a more benign option, similar to Group IV (Ge, Si) materials, for future applications in photovoltaics and optoelectronics. This work is dedicated to the development of wet-chemical synthetic routes of (1) Zn3P2 and (2) Group IV (Ge, Si, Si1-xGex) nanocrystals with precise control over composition, crystal structure, size and dispersity by adjusting different reaction parameters such as temperature, time and solvent composition. Different characterizations will also be employed to probe the size- and composition-dependent physical and optical properties of resulting products. The first part of this work illustrates the synthesis of luminescent Zn3P2 nanocrystals, an earth-abundant and a direct-gap semiconductor possessing high absorption coefficient and long carrier diffusion length, which uphold promising potential in many optoelectronic applications. A hot injection method by using highly reactive P and Zn precursors (P[Si(CH3)3]3 and diethyl zinc) in hexadecylamine and octadecene was developed to prepare a series of alkyl-amine-passivated tetragonal Zn3P2 crystallites with varying size sizes. Substantial blue shifts in the absorption onsets (2.11−2.73 eV) in comparison to the bulk counterpart (1.4−1.5 eV) and a clear red shift with increasing particle size indicates the quantum confinement effects. This is also consistent with the photoluminescent studies with the size-tunable maxima in the visible region (469−545 nm) as a function of growth temperature and time. The phase purity and alkyl-amine passivation of the nanocrystals were determined by structural and surface analysis, confirming the presence of N–Zn and N–P bonds on the tetragonal Zn3P2 crystallites. The second part of this works focuses on the development of a colloidal synthetic strategy of alkyl-amine capped Si1-xGex nanocrystals with control over size- and composition-dependent optical properties. Despite their high miscibility at all compositions, developing a wet-chemical synthesis of Si1-xGex alloys in the nanoscale remains a challenging task, owing to the difference of their crystallization temperatures and the high surface oxidation of Si. Thus an adapted colloidal method is utilized to fabricate single-element Ge and Si nanocrystals. Powder X-ray diffraction indicates successful production of cubic crystalline Ge and amorphous Si nanoparticles individually in oleylamine/octadecene (surfactant/solvent) mixture at 300°C. Absorption onset values of 1.28 eV and 3.11 eV are obtained for resulting Ge and Si colloids, respectively. By alloying these two materials in their nano-regime, tunable optical properties can be achieved throughout the visible to the near IR region by simply varying their elemental compositions. The success of this bandgap engineering process offers more options for new material design by taking advantage of unique properties from each component material.

Cette thèse a pour but d’étudier le principe d’un multiplexeur de sortie accordable pour la charge utile d’un satellite de télécommunication. La première étape consiste à analyser les principales topologies de multiplexeur de sortie utilisables et les comparer pour en retirer le meilleur candidat pour cette application. Par la suite, diverses études ont été menées sur des composants passifs imprimés en 3D plastique et métallisés de diverses manières, en cherchant à comprendre comment améliorer au mieux les résultats de ces prototypes. La dernière partie de ce manuscrit détaille la conception d’un multiplexeur à deux canaux pouvant être utilisé sur trois états différents en large bande à 19 GHz. Ces états sont créés par des bandes passantes relatives variant de 1,6 à 4,8 % et une réalisation de deux maquettes sert de preuves de concept et de performance (une en plastique métallisé et la seconde en aluminium usiné). / This thesis is about study of tunable output multiplexer principle for telecommunication satellite payload. The first step is analysis of the main topologies of output multiplexers and to compare them to conclude with the best candidate. Then, several studies were conducted on 3D plastic printed passive components with specific metallizations, searching how to improve results in term of losses and precision. Last part detailed two channels multiplexer design which can be used on three different states of relative bandwidth from 1.6 to 4.8 % at 19 GHz, and realization of two concept proof prototypes (one in metallized 3D printed plastic and another one in machined aluminum).

Compte tenu de la multiplication des standards dans le domaine des télécommunications,l’accordabilité au sein des systèmes est devenue une priorité en termes d’intégration et de coût.Un seul circuit accordable doit ainsi permettre d’adresser plusieurs normes. Dans la gamme deshyperfréquences, en technologie planaire, la fonction accordable (filtre ou antenne) estactuellement un dispositif passif distribué sur lequel sont reportés un ou plusieurs élémentsd’accords. Il est ainsi possible de faire varier au moins une des caractéristiques du dispositif(fréquence centrale et/ou bande passante pour les filtres et fréquence de résonance, diagrammede rayonnement ou mode de polarisation pour les antennes). Le circuit passif étant distribué, pourassurer la propagation de l’onde, un matériau diélectrique faible pertes est généralement utilisé.Cependant, l’ajout d’éléments d’accord engendre des pertes et des perturbations liées au report ducomposant (éléments parasites au niveau de l’interconnexion et des discontinuités composantd’accord-dispositif passif, et de la mise en boitier du composant reporté). Enfin, cette manière deréaliser des fonctions accordables rend peu flexible la conception (dimensions et localisation ducomposant d’accord) et la fabrication (perçage et métallisation pour les vias).Dans ce contexte, nous proposons de co-concevoir des fonctions hyperfréquences accordablessur un substrat semi-conducteur sur lequel il est à la fois possible de réaliser le composantd’accord et le dispositif passif distribué. Cette co-conception du circuit passif et de son élémentd’accord permet d’éliminer toutes les contraintes liées au report de composant, au perçage de viamétallique et apporte une grande flexibilité au niveau du dimensionnement de la zone dopée. Eneffet, elles peuvent être soit localisées soit distribuées. Toutefois, ce concept nécessite que lesupport semi-conducteur soit à la fois compatible à la propagation de l’onde et à la réalisation del’élément d’accord. Ces travaux de thèse ont permis de lever ce verrou en proposant descompromis permettant la réalisation de composants accordables validés par des démonstrateurssur technologie silicium.Au cours de ces travaux, une ligne de transmission micro-ruban et un composant d’accord de typeswitch ont été co-conçus. De très bonnes performances, validées par la mesure, ont été obtenues.De plus, une démarche de co-simulation a été proposée pour prendre en compte les effets semiconducteursdans la simulation électromagnétique.Le concept ayant été validé, il a été ensuite appliqué à des dispositifs accordables relativementsimples afin de montrer le potentiel de cette démarche (en termes de performances et de flexibilitéde conception), tels que des filtres accordables, des guides d’ondes de type SIW (SubstrateIntegrated Waveguide) reconfigurables ou encore des antennes accordables en fréquence. Cestravaux font également apparaître de nombreuses perspectives pour la réalisation de nouvellestopologies de filtres accordables (filtres SIW, interdigités…), d’antennes accordables (enfréquence, en diagramme de rayonnement…) ou de déphaseurs. Enfin, un potentiel a été identifiépour de nouvelles topologies de fonctions accordables en continu à base de jonction de typediodes varactors (composants à capacités variables). / Given the proliferation of standards in telecommunication systems, tunability is becoming a priorityboth in terms of integration and cost. A single tunable circuit needs to be able to work according toseveral different standards. Nowadays, a tunable function (filter or antenna) in planar technology isa passive distributed device to which some active tuning elements are soldered. At least onecharacteristic of the device can therefore be varied (the central frequency and/or the bandwidth inthe case of a filter; or the resonant frequency, radiating pattern or polarization mode in the case ofan antenna). Because passive devices are distributed in order to propagate the electromagneticwave, they are often designed on a dielectric substrate to minimize losses. However, the additionof tuning elements causes some additional losses and disturbances (some parasitic effects canarise due to the packaging or the interconnection and discontinuities between active and passiveparts). Finally, these tunable functions reduce the flexibility of the design (due to the size andlocalization of the active tuning elements) and manufacturing (due to drilling and via metallization).In this context, we propose to co-design tunable microwave functions on a semiconductorsubstrate on which it is possible to build both the tunable element and the passive distributedcomponent. This co-design between the passive and active parts removes the constraints relatedto the tuning elements and drilling of via holes. The concept offers a greater flexibility with regard tothe size of doped areas, allowing them to be either localized or distributed. However, this approachrequires the substrate to be compatible with the propagation of the electromagnetic field and withthe design of the tunable element. The work of this thesis makes it possible to overcome suchobstacles by proposing some tradeoffs allowing the design and the manufacture of tunablemicrowave components in silicon technology, which have been validated by demonstrator circuits.During this work, a microstrip transmission line and a switch were co-designed. Goodperformances were obtained both in simulations and measurements. Moreover, a co-simulationapproach is proposed to take into account the semiconductor effects in electromagneticsimulations.Once validated, this concept was applied to other relatively simple tunable devices to show thepotential of this approach (in terms of performances and design flexibility). Applications includedtunable filters, reconfigurable waveguides (such as SIW: Substrate Integrated Waveguides) andfrequency-tunable antennas. This study showed promising results for the design of new tunablefilter topologies (SIW filters, coupled-line filters), tunable antennas (in resonant frequency orradiation pattern) and phase shifters. Finally, the approach shows potential for continuous tunablefunctions based on varactor diodes (with capacitance variation).

Au cours de dix dernières années la science aux attoseconde ou Physique au champ-fort a été l’objet d’un fort développement. La production d’impulsions laser énergétiques de courte durée à haute cadence et stabilisées en CEP constitue la première étape pour accéder aux dynamiques ultra-rapides caractérisant l’interaction de la matière avec une source de lumière cohérente, intense et ultra-rapide. Le travail de cette thèse consiste à améliorer globalement les performances d’un système laser Ti:Sa à haute cadence optimisé pour la génération des impulsions attoseconde. Nous avons développé une nouvelle configuration de cavité régénérative fonctionnant à 10 kHz qui permet une meilleure gestion des effets thermiques dans le cristal. En sortie de l’amplificateur les impulsions atteignent des valeurs de puissance de 5 W en bande étroite (35 fs), ou 2.7 W en bande spectrale large permettant une compression des impulsions proche de 17 fs. La CEP des impulsions en sortie d’amplificateur a été stabilisée ; le bruit résiduel mesuré tir-à-tir est de 210 mrad pendant trois heures.L’amplificateur peut supporter également le fonctionnement en mode accordable, en sélectionnant des spectres de 30 à 40 nm de largeur à mi-hauteur et en accordant leur longueur d’onde centrale dans une gamme de 80 nm autour de 800 nm. Nous avons conçu et mis en fonctionnement un amplificateur multi-passages non-cryogéné à imagerie par lentille thermique pour accroître la puissance des impulsions jusqu’à 10 W à une cadence de 1 kHz. Le régime de forte saturation d’amplificateur garantit une variation négligeable (±3% pic à pic) de la puissance des impulsions en sortie du module, face à une variation importante de la puissance en entrée (±25% pic à pic) sur la bande spectrale accordable. L’amplification peut encore être plus importante grâce à une ligne d’amplification à refroidissement cryogénique, qui permet d’atteindre des puissances au niveau TW, à la cadence de 1 kHz, tout en maintenant un régime de courte durée (17.5 fs) et stabilité en CEP (350 mrad de bruit résiduel tir-à-tir). Nous proposons aussi une étude des sources de bruit de CEP dans les modules hautement dispersifs: nous avons conçu une nouvelle approche numérique sur la base d’un logiciel de tracé de rayon commercial (Zemax) pour évaluer les variations de CEP dans les modules contenant réseaux de diffraction. / The last decade has seen a lot of progress in attosecond science or in strong field physics. Generating energetic, few-cycle laser pulses with stabilized Carrier-Envelope Phase at high repetition rate constitutes the first step to access the ultra-fast dynamics underlying the interaction of matter with intense, ultrashort coherent light source. The work of this thesis consists in globally improving the performances of a high repetition rate Ti:Sa laser system optimized for attosecond science. We present an original 10 kHz Ti:Sa CPA laser based on an newlydesigneddouble-crystal cavity for thermal lensing management. The amplifier delivers up to 5 W in narrow band mode (35 fs pulses), or 2.7 W in broad band mode, supporting 17 fs pulses after temporal compression. We demonstrate shot-to-shot CEP stabilization with a remaining noise of 210 mrad over three hours at the front-end output. In parallel to the short pulse duration operation mode, it is possible to use the front end in a wavelength tunability mode within a 80 nm range around 800 nm, with a resolution of 1 nm and 30 to 40 nm of bandwidth. We designed and demonstrated a complete water-cooled lens-less multipass amplifier using thermal lensing for modeadaptation boosting the pulse energy up to 10mJ at 1 kHz repetition rate (up to 10 W). The saturation regime of the amplifier ensures negligible variation (±3% peak to peak) of the output power for significant variation of the input power (±25% peak to peak) over the tunability range. The energy scalability of the front-end is demonstrated by coupling its output to cryogenically cooled amplifier, delivering 1 kHz, TW-class pulses at 17.5 fs and CEP stabilized with a residual noise of 350 mrad. A study of CEP noise sources in high dispersive module is also addressed, proposing a numerical approach based on a commercial ray-tracing software (Zemax) for predicting CEP fluctuation in grating based modules.

La photoisomérisation de la molécule d’azobenzène entre ses formes trans et cis génère un travail mécanique qui peut déformer la matrice solide environnante et provoquer un déplacement de matière. Il est en particulier possible de contrôler optiquement la formation de motifs de taille micro- et nanométrique à la surface d’un matériau de type polymère ou verre. Ces phénomènes ont été étudiés en détails ces dernières années et de nombreuses approches ont été proposées pour réaliser des dispositifs ajustables qui exploitent les propriétés photomécaniques des azo-matériaux.L’objectif de ce doctorat était de réaliser des réseaux de micro- et nanostructures hybrides métal/diélectrique contenant des matériaux à base de dérivés d’azobenzène, et d’étudier, d’une part, la réponse photomécanique de ces structures et, d’autre part, la variation des propriétés optiques des réseaux associée à la photo-déformation des structures.La première partie de ce travail a consisté au développement d’une méthode de structuration de polymères photo-actifs à base d’azobenzène en réseaux de piliers par embossage en voie liquide. L’étude des déformations des micro- et nanostructures induites par photo-stimulation dans la bande d’absorption des molécules d’azobenzène montre en particulier que les déformations sont dirigées par la polarisation de la lumière et que certaines déformations peuvent être réversibles. Les propriétés optiques (diffraction, transmission) des réseaux de micro- et nanostructures sont alors ajustables en fonction de la déformation du motif.Dans un second temps, les motifs d’azo-matériaux sont recouverts par une fine couche d’or d’une dizaine de nanomètres. Il a été montré que les propriétés photomécaniques de l’azo-matériau sont conservées malgré la métallisation. Dans la gamme du spectre visible, les interférences présentes dans le spectre de réflexion sont annulées par la déformation du motif du réseau. En lumière infrarouge, cette déformation permet de modifier les conditions de couplages entre les modes localisés et les modes propagatifs présents dans la structure métallisée. Le contrôle de la forme des motifs qui composent le réseau permet donc de moduler avec précision les propriétés optiques et plasmoniques du système hybride. / Trans-cis photo-isomerization of azobenzene units generate mechanical work on its hosting matrice, allowing matter migration inside. This property allows to optically pattern micro and nanometric structures at the surface of azobenzene-containing materials (polymer, glass). Such phenomena were widely investigated and exploited to produce tunable devices exploiting photo-mechanical properties of azobenzene molecules.The purpose of this thesis were to fabricate metal-dielectric azobenzene-containing micro and nanostructured gratings and study the evolution of their optical and plasmonic properties under light stimulation.First, we developped a structuration methode inspired from solvent-assisted nanoimprint lithography to generate 2D azobenzene-gratings of pillars. Type and direction of the deformation induced in the structures were directly associated with the stimulation light polarization. Reversibility of the deformation were observed for a certain type of illumination cycle. Modification of the optical properties (transmission, diffraction) was investigated during the deformation of the pillars.Then, gratings were covered with tens of nanometers of gold. Metallization did not affect the deformation of the structures. Study in the visible range shows that interferences in the reflection spectra vanishes during the photo-deformation. In the infrared domain, the deformation leads to a strong modification of the plasmonic properties, enhancing particular plasmonic modes in favor of others. Control of the grating pillars shape allows a precise tenability of optical and plasmonic properties of the hybrid device.

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