2D semiconductors are one of the most promising materials for next-generation electronics. Realizing continuous 2D monolayer semiconductors with single-crystalline structure at the wafer scale is still a challenge. We developed an epitaxial phase conversion (EPC) process to meet these requirements. The EPC process is a two-step process, where the sulfurization process was carried out on pre-deposited Mo-containing films. Traditionally, two-step processes for 2D MoS2 and other chalcogenides have suffered low-quality film and non-discontinuity at monolayer thickness. The reason was regarded as the low lattice quality of precursor film. The EPC process solves these problems by carefully preparing the precursor film and carefully controlling the sulfurization process. The precursor film in the EPC process is epitaxial MoO2 grown on 2″ diameter sapphire substrate by pulsed laser deposition. This epitaxial precursor contains significantly fewer defects compared to amorphous precursor films. Thus fewer defects are inherited by the EPC MoS2 film. Therefore, EPC MoS2 film quality is much better. The EPC prepared monolayer MoS2 devices to show field-effect mobility between 10 ~ 30 cm2·V-1s-1, which is the best among the two-step process. We also developed a CLAP method further to reduce the defects in the precursor oxide film; thus, in-plane texture in the thicker MoS2 film was eliminated, and a single-crystalline structure was obtained in the wafer-scale MoS2 films. The potentially feasible technique to further improve the 2D film quality is pointed out for our next research plan. Meanwhile, the epitaxial phase conversion process was proposed to be as a universal growth method. Last but not least, we demonstrate several potential applications of the wafer-scale single-crystalline MoS2 film we developed, such as logic circuits, flexible electronics, and seeding layer of van der Waal or remote epitaxial growth.

L’énergie photovoltaïque jouera un rôle déterminant dans la transition énergétique future. Bien que les cellules solaires à base de silicium dominent encore le marché, leur coût de fabrication et le poids des modules limitent leur développement. Depuis quelques années, les industriels s’intéressent de plus en plus aux dispositifs à base de couches minces en raison de leurs procédés de fabrication rapides et peu onéreux sur de larges substrats. Cette technologie utilise une large variété de matériaux; les chalcopyrites tels que Cu(In,Ga)Se2 sont les plus prometteurs. Le procédé de fabrication de couches chalcopyrites le plus répandu est la coévaporation mais l’utilisation de vides très poussés rende cette technique peu adaptée à la production à grande échelle de modules bon marché. La solution alternative décrite dans ce travail est un procédé en deux étapes basé sur le recuit sous atmosphère réactive de précurseurs métalliques électrodéposés. Le développement de cette technologie passe par une meilleure compréhension des mécanismes d’incorporation et d’homogénéisation du gallium dans les couches formées et par une optimisation des étapes de recuit. Le premier objectif de ce travail de thèse est une étude des mécanismes réactionnels mis en jeu lors du procédé de recuit à travers l’étude de différents types de précurseur. Par la suite ces connaissances sont utilisées pour modéliser et optimiser un recuit industriel innovant. Ce travail est réalisé à l’aide de plans d’expérience (DOE) où l’influence de certains paramètres, les plus critiques est mise en évidence. Des voies d’optimisation sont proposées et des hypothèses faites afin d’expliquer les phénomènes observés. / Solar energy is promised to be a major actor in the future of energy production. Even if silicon based solar cells remain the main product their fabrication is energy consuming and requires heavy cover glass for protection, which reduce their development. For several years, commercial interest has shifted towards thin-film cells for which manufacturing time, large scale production, fabrication costs and weight savings are the main advantages. For thin film technology, a wide variety of materials can be used but chalcopyrite such as Cu(In,Ga)Se2 is one of the most promising. The most current method used for chalcopyrite formation is co- evaporation but this process is very expensive and not well suitable for large scale production due to high vacuum requirements. One alternative solution described in this work consists of a two-step technology based on the sequential electro-deposition of a metallic precursor followed by a rapid reactive annealing. However to reach its full potential this technology needs a better understanding of the Ga incorporation mechanism and of the selenization/sulfurization step. This work focuses first on formation mechanisms through the study of several kinds of precursor. This knowledge is then used to explain and to optimize innovative annealing processes. This study is achieved by observing the impact of some process parameters using designs of experiment (DOE). A link between process parameters and properties of these thin films is obtained using electrical, structural and diffusion characterization of the devices. Finally we propose hypothesis to explain observed phenomena and also some improvements to meet the challenges of this process.

Recently, Zn-XAl-YMg coatings have emerged as lighter-weight substitutes for traditional Zn-based coatings for the corrosion protection of steels; however, little is currently known concerning the interactions between the oxides present on advanced high strength steel (AHSS) surfaces and the Zn-Al-Mg bath. In the current contri- bution, the selective oxidation and reactive wetting of a series of C-Mn AHSS were determined with the objective of providing a quantitative description of this pro- cess. The process atmosphere pO2 was varied using dew points of −50◦C, −30◦C and −5◦C. The surface oxide chemistry and morphology were analysed by means of SEM and XPS techniques. Reactive wetting of the selectively oxidized surfaces using a Zn-1.6 wt.% Al-1.6 wt.% Mg bath was monitored as a function of annealing time at 60 s, 100 s and 140 s at 800◦C. The resulting bare spot defects in the Zn-1.6 wt.% Al-1.6 wt.% Mg coating were assessed by means of SAM-AES and FIB, while coating adhesion was analysed by 180◦ bend tests. Annealing the steel substrates resulted in the formation of surface MnO, which varied based on pO2 and Mn alloy content, and that this MnO greatly reduced the wettability of the steel by the Zn-1.6 wt.% Al- 1.6 wt.% Mg bath, resulting in bare spot defects. It was determined that the reactive wetting of the steel substrate was dependant on the oxide morphology and oxidation mode, which was a function of both alloying content of Mn in the steel and annealing pO2 process atmosphere (dew point). Finally, it was concluded that the bare spot area percentage on the coated panels was statistically invariant for annealing times of between 60 s and 140 s at 800◦C. / Thesis / Master of Applied Science (MASc) / Metallic coatings are applied to steels that are not naturally corrosion resistant. The aim of this research was to determine how well a coating containing zinc, aluminum and magnesium adhered to high strength automotive steel. It was deter- mined that manganese oxides formed on the steel during heating prior to applying the metallic coating. The manganese oxides prevented good adhesion between the steel and the coating, resulting in bare spot defects in the coating. The bare spot defects are undesirable as they leave the steel exposed and therefore susceptible to corrosion and are unsightly when painted.