A phase transition model in dual-amorphous water undergoing liquid–liquid transition

Abstract

Abstract An in-depth understanding of liquid–liquid phase transition (LLPT) in condensed water will gain insight into anomalous behaviors of dual-amorphous condensed water. Despite numerous experimental, molecular simulation, and theoretical studies, it is yet to achieve a widely accepted consensus with convinced evidence in the condensed matter physics for two-state liquid–liquid transition of water. In this work, a theoretical model is proposed based on the Avrami equation, commonly used to describe first-order phase transitions, to elucidate complex homogeneous and inhomogeneous condensation from high-density liquid (HDL) water to low-density liquid (LDL) water for both pure and ionic dual-amorphous condensed water. This model unifies the coupling effects of temperature and electrolyte concentration based on the new theoretical framework. The Adam–Gibbs theory is then introduced to characterize the synergistic motion and relaxation behavior of condensed water. Variations in the configurational entropy under electrostatic forces are further explored, and an analytical 2D cloud chart is developed to visualize the synergistic effect of temperature and electrolyte concentration on the configurational entropy of ionic water. The constitutive relationships among viscosity, temperature, and electrolyte concentration are derived to analyze their synergistic effects under different condensation fractions of LDL and HDL. The Stokes–Einstein relation and free volume theory are further used to analyze diffusion coefficients and densities (or apparent density) during both pure and ionic LLPT. Finally, theoretical results obtained from these models are compared with experimental results reported in literature to validate the accuracy and applicability of the proposed models, which offer significant benefits and advancements in effectively predicting physical property changes of dual-amorphous condensed water.