Adaptive Elastic Networks as models of supercooled liquids

TL;DR

This paper introduces adaptive elastic network models where the network's geometry can evolve with temperature, providing insights into the thermodynamics and structure of supercooled liquids near the rigidity transition.

Contribution

It extends previous elastic network models by allowing the network to adapt dynamically, and offers analytical predictions aligning with real material behaviors.

Findings

Structure-thermodynamics relationship holds in adaptive models

Redundant constraints behave like an ideal gas in the model

Distance to rigidity transition controls specific heat and phase space directions

Abstract

The thermodynamics and dynamics of supercooled liquids correlate with their elasticity. In particular for covalent networks, the jump of specific heat is small and the liquid is {\it strong} near the threshold valence where the network acquires rigidity. By contrast, the jump of specific heat and the fragility are large away from this threshold valence. In a previous work [Proc. Natl. Acad. Sci. U.S.A., 110, 6307 (2013)], we could explain these behaviors by introducing a model of supercooled liquids in which local rearrangements interact via elasticity. However, in that model the disorder characterizing elasticity was frozen, whereas it is itself a dynamic variable in supercooled liquids. Here we study numerically and theoretically adaptive elastic network models where polydisperse springs can move on a lattice, thus allowing for the geometry of the elastic network to fluctuate and evolve with temperature. We show numerically that our previous results on the relationship between structure and thermodynamics hold in these models. We introduce an approximation where redundant constraints (highly coordinated regions where the frustration is large) are treated as an ideal gas, leading to analytical predictions that are accurate in the range of parameters relevant for real materials. Overall, these results lead to a description of supercooled liquids, in which the distance to the rigidity transition controls the number of directions in phase space that cost energy and the specific heat.