Complex singularities of the fluid velocity autocorrelation function

Abstract

There are intensive debates regarding the nature of supercritical fluids: if their evolution from liquid-like to gas-like behavior is a continuous multistage process or there is a sharp well-defined crossover. Velocity auto-correlation function Z is the established detector of evolution of fluid particles dynamics. Usually, complex singularities of correlation functions give more information. For this reason, we investigate Z in complex plane of frequencies using numerical analytic continuation. We have found that naive picture with few isolated poles fails describing Z(ω) of one-component Lennard-Jones (LJ) fluid. Instead, we see the singularity manifold forming branch cuts extending approximately parallel to the real frequency axis. That suggests LJ velocity autocorrelation function is a multivalued function of complex frequency. The branch cuts are separated from the real axis by the well-defined “gap” whose width corresponds to an important time scale of a fluid characterizing crossover of system dynamics from kinetic to hydrodynamic regime. Our working hypothesis is that the branch cut origin is related to competition between one-particle dynamics and hydrodynamics. The observed analytic structure of Z is very stable under changes in the temperature; it survives at temperatures two orders of magnitude higher than the critical one.