Liquid-liquid-solid transition in viscoelastic liquids

Abstract

Liquid-liquid-solid transitions (LLST) are known to occur in confined liquids, exist in supercooled liquids and emerge in liquids driven from equilibrium. Molecular dynamics (MD) simulations claim many successes in forecasting the phenomena. The transitions are also studied in the framework of thermodynamics based methods and minimalistic models. In here, the proposed approach is derived in the framework of continuum and includes spatial and temporal dynamic heterogeneities; the approach is meant to capture the material behavior at small scales. We conjecture that the liquid-like and solid-like behaviors are dissimilar enough for the two to be governed by different constitutive relations. In this way, we gain additional degree of freedom, which is found essential when predicting the transitional phenomena. As a result, we derive the LLST criteria for liquids in equilibrium, during steady flow and at transient conditions. Lastly, we forecast short-lived LLSTs in human blood during cardiac cycle.