A "configurational-entropy-loss" law for the non-Arrhenius relaxation in disordered systems

TL;DR

This paper introduces a new configurational-entropy law based on Nowick's theory to better describe non-Arrhenius relaxation in disordered systems, connecting kinetics and thermodynamics more accurately than previous models.

Contribution

It develops a novel configurational-entropy relation that explicitly includes entropy loss and coupling interactions, extending beyond the Adam-Gibbs relation.

Findings

Provides more accurate estimates of activation enthalpy

Determines the systematic configurational entropy loss

Identifies the self-induced ordering temperature T_c

Abstract

Based on Nowick's self-induced ordering theory, we develop a new configurational-entropy relation to describe the non-Arrhenius temperature(T)-dependent relaxation in disordered systems. Both the configurational-entropy loss and the coupling interaction among relaxing units (RUs) are explicitly introduced in this relation; thus, it offers a novel connection between kinetics and thermodynamics that is different from the Adam-Gibbs (A-G) entropy relation, and it generalizes several well-known currently used relations. The present relation can provide direct and more accurate estimates of (i) the intrinsic activation enthalpy, (ii) the T-evolvement of the systematic configurational entropy loss and (iii) the self-induced ordering temperature Tc, which characterizes the coupling interaction among RUs. Application of the theory to experimental relaxation-time data for typical organic liquids demonstrates its validity.