Non-equilibrium Kinetics of the Transformation of Liquids into Physical Gels

TL;DR

This paper discusses the NE-SCGLE theory's ability to predict the kinetics of liquid-to-gel transformations, highlighting its universality and agreement with experimental and simulation data.

Contribution

It applies the NE-SCGLE theory to describe gel formation kinetics, providing a universal framework for understanding non-equilibrium amorphous states.

Findings

The theory predicts structural arrest during gelation.

Simulation and experimental data support the universality of the scenario.

Structural parameters show arrested spinodal decomposition.

Abstract

A major stumbling block for statistical physics and materials science has been the lack of a uni- versal principle that allows us to understand and predict elementary structural, morphological, and dynamical properties of non-equilibrium amorphous states of matter. The recently-developed non- equilibrium self-consistent generalized Langevin equation (NE-SCGLE) theory, however, has been shown to provide a fundamental tool for the understanding of the most essential features of the transformation of liquids into amorphous solids, such as their aging kinetics or their dependence on the protocol of fabrication. In this work we focus on the predicted kinetics of one of the main fingerprints of the formation of gels by arrested spinodal decomposition of suddenly and deeply quenched simple liquids, namely, the arrest of structural parameters associated with the morpho- logical evolution from the initially uniform fluid, to the dynamically arrested sponge-like amorphous material. The comparison of the theoretical predictions (based on a simple specific model system), with simulation and experimental data measured on similar but more complex materials, suggests the universality of the predicted scenario.