Is the mechanism of "fast sound" the same in liquids with long-range interactions and disparate mass metallic alloys?

Abstract

We present ab initio simulations of a large system of 2400 particles of molten NaCl to investigate the behavior of collective mode dispersion beyond the hydrodynamic regime. In particular, we aim to explain the unusually strong increase in the apparent speed of sound with wave number, which significantly exceeds the typical positive sound dispersion of 10%-25% observed in simple liquids. We compare dispersions of "bare" acoustic and optic modes in NaCl with ab initio simulations of other ionic melts such as CuCl and LiBr, metallic liquid alloys such as Pb44Bi56 and Li4Tl, and the regular Lennard-Jones KrAr liquid simulated by classical molecular dynamics. Analytical expressions for the "bare" acoustic and optic branches of collective excitations help us to identify the impact of the high-frequency optic branch on the emergence of "fast sound" in binary melts. Our findings show that in ionic melts, the high-frequency speed of sound is much larger than in the simple Lennard-Jones liquids and metallic melts, leading to an observed strong viscoelastic increase in the apparent speed of sound-more than double its adiabatic value.