Experimental indication for liquid-liquid transition in aqueous solutions

Abstract

Contrary to the conventional wisdom that there exists only one unique liquid state for any material, there are growing experimental and numerical evidence for the existence of more than two liquid states in a single component substance. The transition between them is called liquid-liquid transition (LLT). LLT has attracted considerable attention because of its counterintuitive nature and its importance in the fundamental understanding of the liquid state. However, the physical nature of the transition has remained elusive. Particularly for water, the possible existence of LLT has special implications not only on its fundamental understanding, but also on a link of various thermodynamic and transport anomalies with critical anomaly associated with LLT. In this paper, we show experimental indications for a LLT in aqueous solutions of glycerol. We demonstrated that LLT proceeds through two types of kinetics characteristic of the first order transition: nucleation-growth (NG) and spinodal-decomposition (SD) type transformation. We also reveal that local tetrahedral ordering of water molecules play a key role, which is suggestive of the presence of LLT in pure water.