This thesis deals with various functional materials from first-principles methods and is divided into two major parts according to the underlying atomic structure of the system under study. The first part of the thesis deals with the temperature-induced structural phase transitions in metallic  β'-AuZn and perovskite oxide LiOsO3. The former one, i.e. binary AuZn, belongs to a class of shape-memory alloys that regain their initial shape due to a reversible martensitic phase transformation. Here, by means of density functional and density functional perturbation theories, we show that the martensitic transition is due to coupling between the Fermi surface nesting and anomalies in the phonon dispersion relations. The other metallic system, perovskite LiOsO3, exhibits a ferroelectric-like transition and is currently the first and sole realization of the Anderson and Blount idea. By means of ab initio molecular dynamics simulations, we investigate the mechanism behind this structural phase transformation. Another part of the thesis is dedicated to modelling and characterization of topologically disordered materials on atomic level. The structural and electronic properties of amorphous W-S-N are addressed regarding its outstanding tribological properties, i.e. almost vanishing friction coefficient. Molecular dynamics “melt-and-quench” technique has been employed in order to construct a model structure of amorphous W-S-N. Further analysis of the atomic structure revealed a formation of quasi-free N2 molecules trapped in S cages, which, together with the complex atomic structure of W-S-N, is the key to ultra-low-friction in this functional material. In the last chapter of the thesis a magnetic class of amorphous materials is addressed. Magnetic order in amorphous Gd-Fe ferrimagnet has been shown to undergo magnezation switching driven by a femtosecond laser pulse. Here, we combine first-principles density functional theory and atomistic spin dynamics simulations to explore this phenomena. A possible mechanism behind magnetization reversal in Gd-Fe based on a combination of the Dzyaloshinskii-Moriya interaction and exchange frustration is proposed.

Dans cette thèse, on s’intéresse à l'étude théorique et à la simulation numérique de la dynamique de charges et de spins dans des nano-structures métalliques. Ces dernières années la physique des nano-structures métalliques à connu un intérêt croissant, aussi bien d'un point de vue de la physique fondamental que d'un point de vue des applications technologiques. Il est donc essentiel d'avoir des modèles théoriques nous permettant de décrire correctement ce type d'objets. Cette thèse comporte deux études distinctes. Dans un premier temps on utilise un modèle semi-classique dans l'espace des phases afin d'étudier la dynamique de charges et de spins dans des films ferromagnétiques(Nickel). On décrit dans le même modèle le magnétisme itinérant et le magnétisme localisé. On montre qu'il est possible, en excitant le système avec un laser pulsé femtoseconde dans le domaine du visible, de créer un courant de spin oscillant dans la direction normal du film sur des temps ultrarapides(femtoseconde). Dans un second temps on s’intéresse à la dynamique de charge d'électrons confinés dans des nano-particules d'Or ou bien encore par des potentiels anisotropes. On montre que de telles systèmes sont des candidats intéressant pour faire de la génération d'harmoniques. / In this thesis we focus on the theoritical description and on the numerical simulation of the charge and spin dynamics in metallic nano-structures. The physics of metallic nano-structures has stimulated a huge amount of scientific interest in the last two decades, both for fundamental research and for potential technological applications. The thesis is divided in two parts. In the first part we use a semiclassical phase-space model to study the ultrafast charge and spin dynamics in thin ferromagnetic films (Nickel). Both itinerant and localized magnetism are taken into account. It is shown that an oscillating spin current can be generated in the film via the application of a femtosecond laser pulse in the visible range. In the second part we focus on the charge dynamics of electrons confined in metallic nano-particles (Gold) or anisotropic wells. We show that such systems can be used for high harmonic generation.