Slow dynamics on the self-organization of intermediate-range orders in a supercooled liquid and their stability in a glass

Abstract

The nature of the glass transition is the self-organization of intermediate-range orders (IROs) in a supercooled liquid on cooling. This process was discussed on the basis of the three-step pathway for the nucleation and growth of crystalline solids such as IROs. The Suzuki scaling theory was applied to the nucleation process of a prenucleation cluster (PNC), the classical nucleation theory was applied to the nucleation process of primary particles and the classical crystal growth theory was applied to the growth process of a crystalline solid. The nucleation of PNCs in the first stage is a self-catalytic process, that is enhanced by boson peak modes in a supercooled liquid. The simulation of the crystal growth implies that the slow dynamics on cooling hinders a glass from becoming a crystal and permits IROs to coexist with an amorphous phase in a glass. The dissipative structure as the ultimate state of a glass is a thermodynamically stable state that is governed by the principle of Helmholtz free energy minimization as well as the equilibrium states of a liquid and crystal. This principle ensures the stable coexistence of IROs and an amorphous phase in a glass.