"Liquid-gas" transition in the supercritical region: Fundamental changes in the particle dynamics

Abstract

Recently, we have proposed a new dynamic line on the phase diagram in the supercritical region. Crossing this line corresponds to the radical changes of the fluid properties. Here, we focus on the dynamics of model Lennard-Jones and Soft-Sphere fluids. We show that the change of the dynamics from the liquid-like to gas-like can be established on the basis of the velocity autocorrelation function and mean-square displacement. Using the rigorous criterion, we show that the crossover of particle dynamics and key liquid properties occurs at the same line. We further show that positive sound dispersion disappears in the vicinity of this line in both kinds of systems. The dynamic line bears no relationship to the existence of the critical point. We find that the region of existence of liquid-like dynamics narrows with the increase of the exponent of the repulsive part of inter-particle potential.

15 pages, 7 figures, accepted to Physical Review Letters

References in corpus (3)

• Thermodynamic behavior of supercritical matter
• Liquid-like behavior of supercritical fluids
• Heat capacity of liquids: an approach from the solid phase

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