Date of Award
Doctor of Philosophy (PhD)
The glass transition remains one of the great open problems of modern physics. This dissertation aims to increase understanding of this topic by studying the rich phenomenology of supercooled liquids, the metastable precursors to the glassy state. Principally, we aim to discover what underlying physics leads to the dramatic, non-Arrhenius increase of the viscosity and relaxation time of supercooled liquids, and what thermodynamic properties govern this physics. We propose a novel framework and associated viscosity function applicable to all supercooled liquids/glassy systems, and rigorously assess both the performance and implications of this model. We demonstrate that the theoretical framework uncovers an underlying universality in the dynamics of supercooled liquids over as much as 16 decades. We extend the model to describe the thermodynamics of supercooled liquids, as well as dynamical features outside of the viscosity/relaxation time. We conclude by discussing a micro structural link, and investigate a growing length scale associated with local rigidity, and percolating clusters of mid range order.
Chair and Committee
Jonathan I. Katz, Kenneth F. Kelton, Kater Murch, David S. Wisbey,
Weingartner, Nicholas Bryan, "Supercooled: An Equilibrium, Melting-Based, Energy Distribution Approach for Describing the Phenomenology of Metastable Liquids" (2017). Arts & Sciences Electronic Theses and Dissertations. 1154.