Vertically aligned nanocomposite (VAN) thin films have recently stimulated significant research interest to achieve better material functionality or multifunctionalities. In VAN thin films, both phases grow epitaxially in parallel on given substrates and form a unique nano-checkerboard structure. Multiple strains, including the vertical strain which along the vertical interface and the substrate induced strain which along the film and substrate interface, exist in VAN thin films. The competition of these strains gives a promise to tune the material lattice structure and future more the nanocomposite film physical properties. Those two phases in the VAN thin films are selected based on their growth kinetics, thermodynamic stability and epitaxial growth ability on given substrates. In the present work, we investigated unique epitaxial two-phase VAN (BiFeO3)x:(Sm2O3)1-x and (La0.7Sr0.3MnO3)x:(Mn3O4)1-x thin film systems by pulsed laser deposition. These VAN thin films exhibit a highly ordered vertical columnar structure with good epitaxial quality. The strain of the two phases can be tuned by deposition parameters, e.g. deposition frequency and film composition. Their strain tunability is found to be related directly to the systematic variation of the column widths and domain structures. Their physical properties, such as dielectric loss and ferromagnetisms can be tuned systematically by this variation. The growth morphology, microstructure and material functionalities of VAN thin films can be varied by modifying the phase ratio, substrate orientation or deposition conditions. Systematic study has been done on growing (SrTiO3)0.5:(MgO)0.5 VAN thin films on SrTiO3 and MgO substrates, respectively. The variation of column width demonstrates the substrate induced strain plays another important role in the VAN thin film growth. The VAN thin films also hold promise in achieving porous thin films with ordered nanopores by thermal treatment. We selected (BiFeO3)0.5:(Sm2O3)0.5 VAN thin films as a template and get uniformly distributed bi-layered nanopores. Controllable porosity can be achieved by adjusting the microstructure of VAN (BiFeO3):(Sm2O3) thin films and the annealing parameters. In situ heating experiments within a transmission electron microscope column provide direct observations into the phases transformation, evaporation and structure reconstruction during the annealing. Systematic study in this dissertation demonstrate that the vertically aligned nanocomposite microstructure is a brand new architecture in thin films and an exciting approach that promises tunable material functionalities as well as novel nanostructures.

Afin de développer de nouvelles applications aux couches minces d’oxydes fonctionnels, il est nécessaire de comprendre les corrélations entre leurs modes de croissance, leur microstructure, leur structure à l’interface avec le substrat, et leurs contraintes et propriétés physiques. Pour cela, une étude par spectroscopie infrarouge et THz des systèmes modèles films/substrats a été exécutée, et confrontée à des calculs théoriques, en particulier sur des couches épitaxiales de SrTiO3/Si(001), VO2/Gd2O3/Si(111) et des couches d’alumine sur alliage d’aluminium. Les caractéristiques vibrationnelles des couches minces sont ici étudiées dans l’infrarouge moyen et lointain sur la ligne AILES du Synchrotron SOLEIL, et simulées à l’aide de la Théorie de la Fonctionnelle de la Densité (DFT), permettant ainsi la première détermination de la structure cristalline de ces couches. Ainsi, une comparaison entre la structure bidimensionnelle et tridimensionnelle des matériaux est effectuée. L’effet des contraintes dans les couches est évalué grâce aux variations des énergies de vibration par rapport au matériau massif. L’influence des conditions expérimentales de l’épitaxie dans la structure locale interatomique de couches minces de SrTiO3/Si(001) est évaluée. D’autre part, la nature de l’interface STO-Si peut être caractérisée par les modes de vibration du réseau cristallin. Enfin, la transition métal-isolant (MIT) des couches minces de VO2 sur des substrats de Gd2O3/Si(111) est étudié par spectroscopie IR ; les variations de propriétés optiques et diélectriques pendant la transition, ainsi que les changements d’intensité des modes de vibration, indiquent que la transition est entraînée par une corrélation électronique et une basse température. La phase monoclinique M1 de VO2 est un isolant de Mott. Ce résultat peut aider à un meilleur contrôle des MIT de couches minces de VO2 pour de futures applications. / In order to understand the relations between growth, microstructure, interface structure, strain, and physical properties in functional oxide thin films for further applications, a study of infrared and THz spectroscopy combined with theoretical calculation has been performed on the films/substrates model systems, in particular epitaxial SrTiO3/Si(001), VO2/Gd2O3/Si(111) films and alumina/alloy films. The vibrational characteristics of the crystal structure of films have been investigated in the mid and far infrared ranges on the AILES beamline at Synchrotron SOLEIL. This experimental vibrational study has been combined with Density Functional Theory (DFT) simulation to allow for the first measure of the crystalline structure of these thin films. The 2-dimensional lattice modification compared with the bulk materials has been discussed. The strain effect in the films can be evaluated on the phonon shifts compared with the crystal spectrum. The influences of epitaxial conditions on the local interatomic structure of SrTiO3/Si(001) thin films have been estimated. The nature of STO-Si interface can be characterized by the phonon modes. The metal–insulator transition (MIT) of VO2 thin films on Gd2O3/Si(111) substrate have been studied by IR spectroscopy. The variations of optical and dielectric properties during the MIT, as well as the phonon intensities, indicate that the MIT is driven by electron correlation and the low temperature M1 monoclinic phase of VO2 is a Mott insulator. This result may help to better understand and control the MITs of VO2 thin films in the device applications.