Investigating isomorphs with the topological cluster classification

TL;DR

This study explores higher-order structural and dynamical correlations along isomorphs in Lennard-Jones liquids, revealing significant differences in local structure populations but similar relaxation times compared to inverse power law systems.

Contribution

It demonstrates the variation in higher-order structural populations along isomorphs and compares these with inverse power law reference systems using topological cluster classification.

Findings

Locally favored structures are up to 80% more prevalent in Lennard-Jones systems.

Structural relaxation times are nearly identical between Lennard-Jones and inverse power law systems.

Lifetime of locally favored structures is up to 40% longer in Lennard-Jones systems upon cooling.

Abstract

Isomorphs are lines in the density-temperature plane of certain "strongly-correlating" or "Roskilde simple" liquids where two-point structure and dynamics have been shown to be close to identical up to a scale transformation. Here we consider such a liquid, a Lennard-Jones glassformer, and investigate the behavior along isomorphs of higher-order structural and dynamical correlations. We then consider an inverse power law reference system mapped to the Lennard-Jones system [Pedersen et al., Phys. Rev. Lett. 105, 157801 (2010)]. Using the topological cluster classification to identify higher-order structures, in both systems we find bicapped square anti-prisms, which are known to be a locally favored structure in the Lennard-Jones glassformer. The population of these locally favored structures is up to 80% higher in the Lennard-Jones system than the equivalent inverse power law system. The structural relaxation time of the two systems, on the other hand, is almost identical, and the four-point dynamical susceptibility is marginally higher in the inverse power law system. Upon cooling the lifetime of the locally favored structures in the Lennard-Jones system are up to 40% higher relative to the reference system.