Thermodynamics and Dynamics of the Two-Scale Spherically-Symmetric Jagla Model of Anomalous Liquids

TL;DR

This study uses molecular dynamics to explore a two-scale Jagla potential model that exhibits water-like anomalies, a liquid-liquid phase transition, and differing glass transition behaviors in high and low density phases.

Contribution

It introduces a detailed analysis of the thermodynamics and dynamics of a Jagla model with two scales, revealing phase behavior and glass transition differences.

Findings

The model shows water-like anomalies such as expansion upon cooling.

A liquid-liquid phase transition with a positive slope coexistence line is observed.

Different glass transition behaviors are identified in HDL and LDL phases.

Abstract

Using molecular dynamics simulations, we study a liquid model which consists of particles interacting via a spherically-symmetric two-scale Jagla ramp potential with both repulsive and attractive ramps. The Jagla potential displays anomalies similar to those found in liquid water, namely expansion upon cooling and an increase of diffusivity upon compression, as well as a liquid-liquid (LL) phase transition in the region of the phase diagram accessible to simulations. The LL coexistence line, unlike in tetrahedrally-coordinated liquids, has a positive slope, because of the Clapeyron relation, corresponding to the fact that the high density phase (HDL) is more ordered than low density phase (LDL). When we cool the system at constant pressure above the critical pressure, the hydrodynamic properties rapidly change from those of LDL-like to those of HDL-like upon crossing the Widom line. The temperature dependence of the diffusivity also changes rapidly in the vicinity of the Widom line, namely the slope of the Arrhenius plot sharply increases upon entering the HDL domain. The properties of the glass transition are different in the two phases, suggesting that the less ordered phase (LDL) is fragile, while the more ordered phase (HDL) is strong, which is consistent with the behavior of tetrahedrally-coordinated liquids such as water silica, silicon, and BeF$_2$.