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Title: Connections between structure,dynamics and energy landscape in simple models of glass-forming liquids.
Authors: Coslovich, Daniele
Supervisore/Tutore: Pastore, Giorgio
Issue Date: 7-Apr-2008
Publisher: Università degli studi di Trieste
The microscopic origin of the glass-transition represents a long-standing open problem in condensed matter physics. Recent theoretical advances and the increasing amount of experimental and simulation data demonstrate the activity of this field of research. In this thesis we address, through molecular dynamics simulations of model glass-forming liquids, a key and yet unsolved issue concerning the description of the glass-transition: the connection between the unusual dynamical properties of glass-formers, their structural properties, and the features of the intermolecular interactions. Toward this end, we consider a broad range of models based on pair interactions. Such models are able to describe both fragile and strong glass-formers and to reproduce different types of local order, including icosahedral and prismatic structures (typical of metallic glasses) as well as tetrahedral ones (typical of network glasses). For these models we provide a systematic characterization of the structure, dynamics, and potential energy surface.

The first part of the thesis briefly introduces the theoretical framework concerning the connection between structure and dynamics in fragile and strong glass-formers, as well as the main experimental and simulation results. The state of the art of the description in terms of the potential energy surface is critically reviewed on the basis of recent simulation results. The simulation methods and the optimization algorithms employed in the thesis are then presented, focusing on the stage of object-oriented analysis of the problem of molecular simulations of classical interacting systems. Such analysis constitutes an original aspect of the thesis and provided a unified and effective framework for the development of simulation software.

The second part focuses on the main results obtained. The variations of dynamical properties in different systems, with particular reference to the Angell's fragility and to dynamic heterogeneities, are traced back first to the features of the locally preferred structures, then to the properties of the potential energy surface. In particular, we show that the variation of fragility in the models considered can be rationalized in terms of the formation of stable domains formed by locally preferred structures. The analysis of the properties of stationary points (local minima and saddle points) in the potential energy surface allows us to establish a direct connection between fragility, structurally stable domains and energy barriers. On the other hand, the spatial localization features of the unstable modes display qualitative variations in the models considered. The study of the correlation between the spatial localization of the unstable modes and the propensity of motion reveals that the dynamical influence of such modes is typical of the late beta-relaxation - time scale within which the effect of dynamic heterogeneity is maximum. It appears to be easier to identify such connection in fragile, rather than strong, systems. This provides indications on the possible qualitative differences concerning the metabasin structure of the potential energy surface in fragile and strong glass-formers.
Ciclo di dottorato: XX Ciclo
metadata.dc.subject.classification: FISICA
Keywords: supercooled liquidspotential energy surfacelennard-jones mixturesmolecular dynamics simulationsobject-oriented fortran
Type: Doctoral
Language: en
Settore scientifico-disciplinare: FIS/03 FISICA DELLA MATERIA
NBN: urn:nbn:it:units-7211
Appears in Collections:Scienze fisiche

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