Abstract

An overview of theoretical results and experimental data on the thermodynamics, structure and dynamics of the heterophase glass-forming liquids is presented. The theoretical approach is based on the mesoscopic heterophase fluctuations model (HPFM) developed within the framework of the bounded partition function approach. The Fischer cluster phenomenon, glass transition, liquid-liquid transformations, parametric phase diagram, cooperative dynamics and fragility of the glass-forming liquids is considered.

Highlights

  • Structure of a glass-forming liquid and glass possesses a short-range and medium-range order (SRO and MRO) rather than a long-range order (LRO)

  • The liquid is nonequilibrium and unstable at the glass transition. For this reason a description of the glass transition cannot be based on the canonic Gibbs statistics

  • A palliative approach based on the bounded statistics can be formulated as follows

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Summary

Introduction

Structure of a glass-forming liquid and glass possesses a short-range and medium-range order (SRO and MRO) rather than a long-range order (LRO). The liquid or glass, which is equilibrated on the scale r ∼ ξSRO without considerable correlations on larger scales, is the minimally ordered amorphous state which can be considered using the bounded statistics method For this reason, as the first step, the bounded partition function should be considered taking into account the states with equilibrated SRO. Parameters of the mesoscopic Hamiltonian can be considered as phenomenological coefficients with averaged out microscopic details of molecular interaction These ideas are in the base of the heterophase fluctuation model (HPFM) [10, 21,22,23,24,25,26,27] which is considered in sections 2–6 and in appendixes A and B.

Hetrophase fluctuations and the order parameter
The quasi-equilibrium glass transition and “ideal” glass
Mesoscopic free energy of the heterophase liquid
The fluctuon-fluctuon interaction and the frustration parameter
Equations of the liquid state equilibrium
Two-state approximation
Phase transition in the solid-like fraction
The Fischer cluster
Parametric phase diagram
Static structure factor and the order parameter restoration
Dynamics
Ultra-slow modes and the Fischer cluster equilibration time
Fragility
Concluding remarks
The bounded phase space and efficient mesoscopic Hamiltonian
Solutions of the equations of state
Thermodynamics and structure of the Fischer cluster
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