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Misfit layer compounds (MLCs) are heterostructures composed of rocksalt units stacked with few-layers transition metal dichalcogenides (TMDs). They host Ising superconductivity, charge density waves, and good thermoelectricity. However, research has mostly focused on specific compounds and trial-and-error synthesis, making the design of misfits’ emergent properties hindered by a lack of a global picture. Our work offers an original perspective by deriving misfits’ properties from those of their constituent layers. We identify the fundamental mechanism governing charge transfer and demonstrate how charge injection into the TMD layers can be effectively controlled through chemical alloying in the rocksalt unit. We show that misfits behave as a periodic arrangement of ultra-tunable field-effect transistors, allowing for massive chargings. We establish a strategy to study the electronic and vibrational properties of MLCs, highlighting the two-dimensional nature of the lattice dynamics of TMDs in these three-dimensional hetrostructures. Finally, we present an in-depth study of superconductivity in MLCs, estimating critical temperatures and comparing with existent experimental data. Our work provides a complete characterization of these heterostructures, aiming to guide the design of materials with targeted emergent properties for future device applications.

Increased interest in the field of sensor technology stems from the availability of an inexpensive and robust sensor to detect and quantify the presence of a specific gas. Bulk p-CuO/n-ZnO heterocontact based gas sensors have been shown to exhibit the necessary sensitivity and selectivity characteristics, however, low interfacial CuO/ZnO contact area and poor CuO/ZnO connectivity limits their effective use as gas sensors. The phase equilibria between CuO and ZnO exhibits limited solubility. By exploiting this concept, a CuO/ZnO mixed solution is formed by combining CuO and ZnO precursors using wet chemical (sol-gel) techniques. Thin films fabricated using this mixed solution exhibit a unique CuO/ZnO microstructure such that ZnO grains are surrounded by a network of CuO grains. This is highly beneficial in gas sensing applications since the CuO/ZnO heterostructure interfacial area is considerably increased and is expected to enhance sensing characteristics. This work builds on previous research by Dandeneau et al. (Thin film chemical sensors based on p-CuO/n-ZnO heterocontacts, Thin Solid Films, 2008). CuO/ZnO mixed solution thin films are fabricated using the sol-gel technique and subsequently characterized. X-ray diffraction (XRD) data confirms the phase separation between ZnO and CuO grains. Scanning electron microscopy (SEM) as well as energy dispersive spectroscopy (EDS) reveal a network of ZnO grains amidst a matrix of CuO grains. Optical and electrical characterization provide material parameters used to construct an energy band diagram for the CuO/ZnO heterostructure. Aluminum interdigitated electrodes (IDEs) are patterned on the thin film and gas sensing characteristics in the presence of oxygen and hydrogen are investigated. Optimization of the electrode geometry is explored with the aim of increasing the sensitivity of the sensor in the presence of hydrogen gas. / Graduation date: 2010

Les dernières années montrent des nombreuses applications de la spectroscopie Teraheretz (THz) dans le domaine de sécurité postale, contrôle de la qualité, médecine et biologie. Après les premières expériences de l'imagerie avec un seul élément / détecteur, l'étape suivante est l'utilisation de matrices de détecteurs. Par conséquent, la nécessité de détecteurs THz sensibles, très rapides, opérant à température ambiante et intégrable facilement en matrice est devenue crucial. Les transistors à effet de champ semblaient être les candidats les plus appropriés pour la construction du première matrice pour l'imagerie THz. Ce travail présente les études des transistors à effet de champ à base de GaAs et GaN en vue de leur application comme imageurs THz. Dans la première partie, nous présentons les études de FET à base de GaAs sur une plage de fréquence très large (0,25 _2.54 THz). Nous étudions également les moyens d'accroître leur sensibilité et d'optimiser leurs puissance équivalente de bruit. Dans la deuxième partie nous étudions les transistors à base de GaN. Ce matériau , avec un grand bande interdite, pourrait être un candidat potentiel comme imageur THz travaillant à des températures élevées et / ou dans des environnements difficiles. Leur sensibilité a été étudiée en fonction de différents paramètres physiques, tels que la tension de grille, la longueur de grille, le courant de fuite de grille, la température et la direction de polarisation du rayonnement THz incidente. Nous avons étudié également l'influence de l'application de courant de drain. Les comportements observés ont été interprété / compris en utilisant des simulations numériques basées sur les modèles théoriques existants. Enfin, nous avons étudié des transistors à base de GaAs avec une structure de couplage spécifique réseaux de grille périodiques. La présence de la structure périodique permet d'améliorer le couplage entre l'onde THz incidente et le transistor. Une estimation théorique de la longueur caractéristique de détection, combinée à des calculs de l'intensité des champs THz locaux ont été utilisés pour interpréter nos résultats expérimentaux. Un bon accord avec le modèle théorique a été obtenue montrant que la détection a lieu principalement dans les zones appauvri du canal. / Last years clearly show many emerging applications of Teraheretz spectroscopy in postal and airport security, quality control, medicine and biology. After first demonstrations of imaging with a single element/detector the evident next step is use of detector matrixes. Therefore , the need for sensitive, rapid, room temperature operating, and easily integrable THz detectors became critical. Field effect transistors appeared to be the most suitable candidates for building the first matrixes focal plane arrays. This work presents the studies of different GaAs and GaN based field effect transistors in view of they application in Terahertz imagers. In the first part we present the studies of GaAs based FETs over a very wide frequency range (0.25 _2.54 THz). We study also the ways to increase their sensitivity and optimize their Noise Equivalent Power. In the second part we study the transistors based on GaN technology. This wide gap material can be a potential candidate for Terahertz imagers working at elevated temperatures or/and harsh environments. Their sensitivity has been studied as a function of various physical parameters, such as the gate voltage, gate length, the gate leakage current, temperature and direction of polarization of the incident THz radiation. We studied also the influence of a drain current. The observed behaviour was interpreted/understood using numerical simulations based on existing theoretical models. Finally, we studied GaAs based transistors with a specific coupling structure - periodic double-granting gate. The presence of periodic structure allows to improve the coupling between incident THz wave and a transistor. A theoretical estimate of the characteristic length of detection, combined with calculations of the intensity of THz local fields were used to interpret our experimental results. Good agreement with theoretical model was obtained showing that the detection takes place mainly in depleted portions of the channel.

Thin films of Strontium Ruthenate have been grown on Strontium Titanate and Lanthanum Aluminate (100) substrates by pulsed laser deposition. X-ray diffraction results show that the films grown on the Strontium Titanate are amorphous and polycrystalline on the Lanthanum Aluminate. Resistances versus temperature measurements show that the films exhibit semiconducting characteristics. In addition to the growth of Strontium Ruthenate thin films, multilayer heterostructures of Terfenol-D thin films on polycrystalline Lead Titanate thin films were grown by pulsed laser deposition. By using a novel experimental technique called magnetic field assisted piezoelectric force microscopy it is possible to investigate the magnetoelectric coupling between the electrostrictive Lead Titanate and magnetostrictive Terfenol-D thin film. Upon examination of the produced thin films the phase and amplitude components of the piezoelectric signal experience changes in response to an applied in-plane magnetic field. These changes provide experimental evidence of a magnetoelectric coupling between the Terfenol-D and Lead Titanate layers.

Le contrôle de la polarisation et de l’aimantation par le biais de champs magnétiques et électriques respectifs font des systèmes magnétoélectriques des candidats prometteurs à de nombreuses applications, parmi lesquelles les dispositifs micro-ondes, les dispositifs de stockage de données à haute densité, etc. L’élaboration d’hétérostructures toujours plus innovantes reste un défi majeur dans le but d’optimiser les densités d’interfaces entre les phases ferroélectriques et ferromagnétiques,et ainsi promouvoir les interactions de couplage mécaniques. Au cours de ce projet de thèse, deux stratégies sont mises en oeuvre pour la conception des matériaux : i) une structure coeur-écorce de type (1-1) composée de nanofils ferromagnétiques (1) dans des nanotubes ferroélectriques (1) àl’intérieur d’une membrane nanoporeuse tridimensionnelle auto supportée etii) une structure en couche mince de type (1-3) constituée de nanofils ferromagnétiques (1) supportés sur un substrat rigide et encapsulés dans une matrice ferroélectrique (3). / Controlling polarization or magnetization by an applied magneticand electric field respectively make magnetoelectric systems promisingcandidates for applications in microwave devices, high density data storagedevices, etc. Designing innovative magnetoelectric heterostructures is thus achallenge to optimize interface density between both ferroelectric andferromagnetic phases, and promote mechanical coupling interactions. In thisthesis project, two strategies are followed for material design: i) 1-1 coreshellstructure with ferromagnetic nanowires (1) inside ferroelectricnanotubes in a self-supported tridimensionnal porous template (1) and ii) 1-3structure where ferromagnetic nanowires (1) are supported on a substrateand embedded in a ferroelectric matrix (3).

Neste trabalho e apresentado um estudo, via teoria de massa efetiva multibanda autoconsistente de heteroestruturas de semicondutores magnéticos diluídos, generalizada para incluir parâmetros de diferentes materiais. A interacao magnética e descrita por um modelo de campo médio baseado no mecanismo de troca indireta, com a possibilidade de inclusão de diferentes íons magnéticos. As equacoes de massa efetiva são resolvidas de forma autoconsistente com o auxílio da equacao de Poisson. As interacoes de spin-órbita e de troca-correlacao, na aproximacao de densidade local, são incluídas no cálculo. O método e aplicado para o estudo das estruturas de bandas e densidades de carga com separacao por spin do portador de heteroestruturas com dopagem tipo-n e tipo-p, variando a geometria dos pocos magnéticos e também o período da super-rede, as densidades de portadores e as concentracoes de íons magnéticos. Solucoes autoconsistentes da equacao de massa efetiva são encontradas para o oxido semicondutor (Zn,Co)O. Será mostrada a separacao de portadores por spin em funcao dos parâmetros variados, simulando diversas concentracoes possíveis, utilizadas em sistemas descritos na literatura, e será analisado o comportamento dos perfis de potencial. Usando os dados obtidos, um diagrama de fases será traçado com base na polarizacao total ou parcial dos portadores, e o seu comportamento será discutido. Também serão mostradas as estruturas de bandas, os perfis de potencial e as distribuicoes de carga do semicondutor (GaMn)As, variando as densidades de portadores e a direcao do campo magnético intrínseco, gerado pela dopagem com íons magnéticos. Os resultados obtidos neste trabalho podem servir de guia para futuras experiências e para o desenvolvimento de dispositivos com semicondutores magnéticos diluídos baseados em (Zn,Co)O e (Ga,Mn)As. Os métodos aqui descritos são gerais e podem ser utilizados para outros materiais. / This work presents a self-consistent multiband effective mass theory applied to diluted magnetic semiconductor heterostructures, generalized to include parameters of different ma- terials. The magnetic interaction is described by a mean-field approximation based on indirect- exchange mecanism, with the possibility of inclusion of different magnetic ions. The effective mass equations are solved self-consistently with the help of the Poisson equation. Spin-orbit and exchange-correlation interactions are included in the simulation in the local density appro- ximation. The method is used to study band structures and charge densities separated by spin in n- and p-type heterostructures. The magnetic well\'s geometry, the superlattice period, the carrier density and the magnetic ion concentration are changed. Self-consistent solutions of the effective mass equation are found for the semiconductor oxide (Zn,Co)O. Charge separation by spin will be show in function of the variation of the simulation parameters, simulating several ion concentrations and charge densities used in systems described in literature, and the potenti- als profiles will be analised. Using the data obtained a phase diagram will be plotted, based on the carrier total or partial carrier polarization, and a model for the behavior of the phase diagram will be discussed. It will also be shown band structures, potential profiles and charge densities of the (Ga,Mn)As semiconductor, varying it carrier density and the direction of the intrinsic magnetic field, generated by the magnetic ions that doped the heterostructure. The results ob- tained in this work can be used as a guide in future experiences and development of devices with diluted magnetic semiconductors based on (Zn,Co)O and (Ga,Mn)As. The methods here described are general and can be used for other materials.

Este estudo propôs uma avaliação do papel dos três principais parâmetros clássicos da síntese do nitreto de carbono grafítico: temperatura final, tempo de permanência na temperatura final e taxa de aquecimento. Realizou-se a otimização da síntese, via metodologia de superfície de resposta, usando-se como variável-resposta a degradação fotocatalítica de um poluente-modelo (tartrazina). A significância estatística dos fatores foi confirmada, com 95% de confiança. Em seguida, um modelo de segunda ordem foi ajustado às melhores respostas e, no ponto de máxima degradação, as condições foram: 605oC por 183 min, com taxa de aquecimento de 5oC min-1. A taxa de degradação com o fotocatalisador sintetizado foi aproximadamente três vezes maior que a da fotólise. As amostras da região de melhores respostas foram analisadas em uma série de experimentos de caracterização, sendo eles: difratometria de raios X, espectroscopia na região do infravermelho médio, área superficial específica, microscopias de varredura (MEV e MEV-FEG), potencial zeta e espectroscopia de reflectância difusa na região do ultravioleta-visível. O fotocatalisador com maior atividade apresentou menor energia de band gap e maior área superficial especifica do que as relatadas na literatura (2,59 eV e 29,5 m2 g-1, respectivamente). Foram criadas heteroestruturas entre o fotocatalisador sintetizado e o trióxido de tungstênio. A partir de uma série de caracterizações básicas, confirmou-se a formação da heteroestrutura. Com essa heteroestrutura, a taxa de degradação foi aproximadamente cinco vezes maior que a com o nitreto de carbono grafítico. / This study proposed an assessment of the role of the three major classical parameters for synthesizing graphitic carbon nitride: final temperature, residence time at the final temperature and heating rate. The synthesis was optimized, via response surface methodology, using the photocatalytic degradation of a model pollutant (tatrazine) as the response-variable. The statistical significance of the factors was confirmed, within 95% confidence level. Afterwards, a second-order model was adjusted to the better responses and, at the maximum degradation point, the conditions were: 605oC for 183 min, with heating rate of 5oC min-1. The degradation rate with the synthetized photocatalyst was approximately three times greater than the photolytic one. The samples from the better response region were analyzed in a series of characterization experiments: X ray diffractometry, mid-infrared spectrometry, specific surface area, scanning electron microscopy (SEM and FEG-SEM), zeta potential, and ultraviolet-visible diffuse reflectance spectroscopy. The most active photocatalyst showed smaller band gap energy and greater specific surface area than the ones reported in literature (2.59 eV and 29.5 m2 g-1, respectively). Heterostructures were formed between the synthetized photocatalyst and tungsten trioxide. A series of basic characterization techniques confirmed the heterostructure formation. Using this heterostructure, the degradation rate was approximately five times greater than the one with graphitic carbon nitride.

Graphene has emerged as an appealing material for a variety of optoelectronic applications due to its unique electrical and optical characteristics. In this thesis, I will present recent advances in integrating graphene and graphene-boron nitride (BN) heterostructures with confined optical architectures, e.g. planar photonic crystal (PPC) nanocavities and silicon channel waveguides, to make this otherwise weakly absorbing material optically opaque. Based on these integrations, I will further demonstrate the resulting chip-integrated optoelectronic devices for optical interconnects. After transferring a layer of graphene onto PPC nanocavities, spectral selectivity at the resonance frequency and orders-of-magnitude enhancement of optical coupling with graphene have been observed in infrared spectrum. By applying electrostatic potential to graphene, electro-optic modulation of the cavity reflection is possible with contrast in excess of 10 dB. And furthermore, a novel and complex modulator device structure based on the cavity-coupled and BN-encapsulated dual-layer graphene capacitor is demonstrated to operate at a speed of 1.2 GHz. On the other hand, an enhanced broad-spectrum light-graphene interaction coupled with silicon channel waveguides is also demonstrated with ∼0.1 dB/μm transmission attenuation due to graphene absorption. A waveguide-integrated graphene photodetector is fabricated and shown 0.1 A/W photoresponsivity and 20 GHz operation speed. An improved version of a similar photodetector using graphene-BN heterostructure exhibits 0.36 A/W photoresponsivity and 42 GHz response speed. The integration of graphene and graphene-BN heterostructures with nanophotonic architectures promises a new generation of compact, energy-efficient, high-speed optoelectronic device concepts for on-chip optical communications that are not yet feasible or very difficult to realize using traditional bulk semiconductors.