On the heterophase liquid thermodynamics and cooperative dynamics

Abstract

The thermodynamics and cooperative dynamics of heterophase liquid states is considered taking into account frustration and volumetric interaction of the solid-like fluctuons. It is found that the glass transition temperature range is scaled by difference of the frustration parameter and mean energy of the volumetric interaction. A model of the cooperative relaxation with finite cooperatively rearranging domains is considered. The fictitious Kauzmann and Vogel-Fulcher temperatures are determined. It is found that they are close to a proper accuracy. Correlation of the temperatures of glass transition, Vogel-Fulcher and "ideal" glass transition (as it is determined in the mode coupling model) is considered too.

Heterophase liquid states: Thermodynamics, structure, dynamics

“…Due to the above noted absence of the "entropy crisis" in the "ideal" glass, one can conclude that T K and T VFT should be considered as free parameters of the widely used phenomenological model [36]. The issue of proximity of T K and T VFT is considered and confirmed within the framework of HPFM in [37].…”

New paradigm for configurational entropy in glass-forming systems

“…is an essential thermodynamic characteristic of previtreous domain. [2][3][4][5]10,11,[13][14][15][16][17][18][19][20][21][22][23][24] formation. We also insisted that this is still a hypothesis but in no way a proven or necessary fact…'.…”

“…. 2,4,[16][17][18][19][20][21][22][23][24] One of the most inspiring models for glass transition was proposed by Adam and Gibbs (AG), five decades ago. 10 It links previtreous slowing-down to cooperatively rearranged regions (CRR), which influence configurational entropy, leading to following relation for previtreous changes of relaxation time: 10…”

“…2,10,14 Numerous reports empirically support such a coincidence between a 'dynamic' and 'thermodynamic' singular temperatures for glass-forming systems. 2,3,[9][10][11][12][13][14][21][22][23] Such an agreement also constitutes an essential reference for a set of theoretical models which link a finite temperature singularity in dynamics to a 'hidden' phase transition. 2,3,[9][10][11][12][13][14][21][22][23] These empirical and theoretical correlations between 'thermodynamic' and 'dynamic' characterizations of previtreous domain, matched to enormous popularity of the VFT Eq.…”