Relation between the Liquid-Liquid Phase Transition and Dynamic Behavior in the Jagla Model

TL;DR

This study uses molecular dynamics simulations to explore how the liquid-liquid phase transition in the Jagla model influences the dynamic behavior of the system, revealing a correlation between phase states and molecular mobility.

Contribution

It demonstrates a connection between liquid-liquid phase transitions and changes in dynamics, highlighting the behavior near the critical point and Widom line in the Jagla model.

Findings

High density phase exhibits slower dynamics than low density phase.

Diffusion constant and relaxation time follow Arrhenius behavior in HDL.

Dynamic crossover occurs near the Widom line, linking phase transition to dynamic change.

Abstract

Using molecular dynamics simulations, we study a spherically-symmetric ``two-scale'' Jagla potential with both repulsive and attractive ramps. This potential displays a liquid-liquid phase transition with a positively sloped coexistence line ending at critical point well above the equilibrium melting line. We study the dynamic behavior in the vicinity of this liquid-liquid critical point. We find that the dynamics in the more ordered high density phase (HDL) are much slower then the dynamics in the less ordered low density phase (LDL). Moreover, the behavior of the diffusion constant and relaxation time in the HDL phase follows approximately an Arrhenius law, while in the LDL phase the slope of the Arrhenius fit increases upon cooling. On the other hand, if we cool the system at constant pressure above the critical pressure behavior of the dynamics smoothly changes with temperature. It resembles the behavior of the LDL at high temperatures and resembles the behavior of the HDL at low temperatures. This dynamic crossover happens in the vicinity of the Widom line (the extension of the coexistence line into the one-phase region) which also has a positive slope. Our work suggests a possible general relation between a liquid-liquid phase transition and the change in dynamics.