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Thermodynamic multi-component solution solidification approach toliquid-to-glass transition is proposed and actual mechanisms underlyingvitrification, other than viscous slowdown, are identified. Due to polydisperseaggregation in liquid state, glass-forming liquids, irrespective of chemicalcomposition, appear to be mixtures of various quasi-components whosethermodynamic quantities shall be expressed not in terms of molarconcentrations of actual chemical components, but in terms of relativeconcentrations of dominant structural units. Thermodynamically, anyglass-former is expected to behave as multi-component solution and solidify incontinuous temperature range between apparent liquidus and solidus temperaturesthat can be identified as glass-transition range. Using extended irreversiblethermodynamics of polydisperse solutions it is demonstrated that uponquenching, diffusional and Brownian mass transport in such solutions is negatedwithin heat removal timescale, which results in dynamical arrest of nucleationand growth in clusters and solid-liquid phase separation. Rapid solutionsolidification proceeds via successive cluster freezing in continuoustemperature range, in line with cluster size dispersity, which can be describedin terms of percolation in static polydisperse fractal ensemble where glasstransition temperature naturally emerges as percolation threshold.Multi-component solution solidification framework is shown to be reconcilablequalitatively and quantitatively with the Mode Coupling - Random First OrderTransition scenario. Finally, it is demonstrated that liquid-to-glasstransformation is thermodynamic liquid-to-solid phase transition, glassy stateof matter appears to be solid supersaturated solution of defects in otherwiseperfect matrix, and the true equilibrium structure which glass is unable accessis a crystalline one.

Thermodynamic approach to liquid-to-glass transformation as an arrest transition in polydisperse solution