Collective Excitations in Supercritical Fluids

Abstract

AbstractRecent progress in theoretical and simulation studies of collective excitations in supercritical fluid s is reviewed. We discuss a methodology of fit-free estimation of dispersion of longitudinal and transverse excitations in simple fluids. The issue of vanishing positive sound dispersion—a viscoelastic increase of the speed of sound from adiabatic one to its high-frequency (elastic) value—with reduction of density, as it was observed in inelastic X-ray scattering experiments on supercritical Ar, is discussed from the point of view of finding distinctions in collective dynamics of low—and high-density supercritical fluids. On the basis of several theoretical models within the extended hydrodynamic description of density-density correlations in liquids analytical expressions for positive sound dispersion are obtained and applied for analysis of time correlation function s obtained from molecular dynamics simulations. A location of a crossover from the liquid-like to gas-like types of collective dynamics is discussed based on general findings for spectra of collective excitations in supercritical Ar and soft sphere fluids.KeywordsCollective excitationsDispersiongeneralized hydrodynamicscomputer simulationssupercritical fluids