Topological Characterization of Rigid–Nonrigid Transition across the Frenkel Line

Abstract

The dynamics of supercritical fluids, a state of matter beyond the gas-liquid critical point, changes from diffusive to oscillatory motions at high pressure. This transition is believed to occur across a locus of thermodynamic states called the Frenkel line. The Frenkel line has been extensively investigated from the viewpoint of the dynamics, but its structural meaning is still not well-understood. This Letter interprets the mesoscopic picture of the Frenkel line entirely based on a topological and geometrical framework. This discovery makes it possible to understand the mechanism of rigid-nonrigid transition based not on the dynamics of individual atoms but on their instantaneous configurations. The topological classification method reveals that the percolation of solid-like structures occurs above the rigid-nonrigid crossover densities.