Amorphous and crystalline functional materials from first principles

Abstract: 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  ?'-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.