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Two-order-parameter model of the liquid-glass transition. II. Structural relaxation and dynamic heterogeneity

by: Hajime Tanaka
Journal of Non-Crystalline Solids, Vol. 351, No. 43-45. (1 November 2005), pp. 3385-3395.


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We propose that there exist two key temperatures relevant to glass transition: (i) a transition from the ordinary-liquid to the frustrated metastable-liquid (the Griffiths-phase-like) state at , which is characterized by the appearance of metastable high-density solid-like islands and the resulting appearance of the cooperative nature of [alpha] relaxation, and (ii) another transition into the spin-glass-like state and the resulting divergence of the [alpha] relaxation time at T0. is a density-ordering (melting) point of the corresponding hypothetical pure system that is free from disorder effects. Below , a system has a complex free-energy landscape characteristic of the frustrated metastable-liquid state; metastable solid-like islands with different densities coexist and fluctuate dynamically. In our model, the [alpha] mode is associated with dynamics of creation and annihilation of metastable islands below . The metastable solid-like islands are the origin of dynamic heterogeneity. We propose a modified Vogel-Fulcher law, which can phenomenologically describe the Arrhenius/Vogel-Fulcher crossover induced by a transition from the ordinary-liquid to the frustrated metastable-liquid state around . We also argue that the hidden crystalline ordering in metastable islands may cause the change in the structure factor of a supercooled liquid below , which is more enhanced upon cooling.


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