Abstract
After an initial discussion of ergodicity-breaking in different types of relaxing systems we consider how relaxation can be characterized and how differences in system responses to different stresses can be interpreted in structural terms. The more general case of systems which respond similarly to different stresses is then considered, with emphasis on the temperature dependence of the relaxation time, its connection to the “ideal” glass transition, to thermodynamics, and to the topology of the potential energy hypersurface each system must explore at low temperatures. With this picture as background we turn to the conundrum presented by the behavior of supercooled water. After a brief review of power law divergences in supercooled water, we show how it is profitable—following Speedy—to study the relation of supercooled to superheated behavior. This leads us to a consideration of the spinodal boundary on liquid stability, and the existence of mechanically stable liquid states of tension. We bring reality to the discussion by presenting new experimental techniques and results which extend the existence of stretched water to pressures of −1400 bars. Based on the excellent agreement of our data with prior superheated water results and Fisher’s theory for the tensile strength of liquids, we argue that we have reached the homogeneous nucleation boundary for stretched water. Since nucleation ceases below 35°C we appear to have identified the tension maximum predicted by equation of state extrapolations, hence indirectly to have confirmed Speedy’s re-entrant spinodal conjecture which accounts for supercooled water anomalies in terms of pre-spinodal fluctuations. On this basis we identify alternative theoretical endpoints for supercooling liquids and identify a crossover between them in the case of water. Finally we consider, using molecular dynamic experiments, the consequences of “jumping” glassy systems across the spinodal. The process of rupture, and the structures produced, are analyzed, and the structures shown to be fractal in both structure and dynamics, with fractal dimensions which vary systematically with final density.
Manuscript prepared with the assistance of J. L. Green.
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Angell, C.A. (1990). Relaxation, Glass Formation, Nucleation, & Rupture in Normal and “Water-Like” Liquids at Low Temperatures and/or Negative Pressures. In: Stanley, H.E., Ostrowsky, N. (eds) Correlations and Connectivity. NATO ASI Series, vol 188. Springer, Dordrecht. https://doi.org/10.1007/978-94-009-2157-3_12
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DOI: https://doi.org/10.1007/978-94-009-2157-3_12
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