Continuum percolation and the liquid-solid coexistence line of simple fluids

TL;DR

This study compares chemical and physical cluster percolation lines with the liquid-solid transition in Lennard-Jones fluids, revealing that chemical clusters do not form stable structures in the fluid phase, unlike physical clusters.

Contribution

It introduces a detailed comparison of chemical and physical cluster percolation lines with phase transitions in simple fluids using molecular dynamics simulations.

Findings

Chemical cluster percolation lines shift rapidly with tau

Chemical clusters do not form stable structures in the fluid phase

Physical cluster percolation lines differ from the liquid-solid transition line

Abstract

We compare the percolation loci for chemical clusters with the liquid-solid transition in the temperature-density phase diagram. Chemical clusters are defined as sets of particles connected through particle-particle bonds that last for a given time tau. By using molecular dynamics simulations of a Lennard-Jones system we obtain the percolation loci at different values of tau as the lines in the temperature-density plane at which the system presents a spanning cluster in 50 percent of the configurations. We find that the percolation loci for chemical clusters shifts rapidly towards high densities as tau is increased. For moderate values of tau this line coincides with the low-density branch of the liquid-solid coexistence curve. This implies that no stable chemical clusters can be found in the fluid phase. In contrast, the percolation loci for physical clusters -sets of particles that remain close together at every instant for a given period tau- tends to a limiting line, as tau tends to infinity, which is far from the liquid-solid transition line.