Role of the single-particle dynamics in the transverse current autocorrelation function of a liquid metal

TL;DR

This study investigates the transverse current autocorrelation in liquid gold using ab initio molecular dynamics, revealing that a second oscillatory component originates from longitudinal dynamics and is reflected in the self part of the correlation.

Contribution

It demonstrates that the second oscillatory component in the transverse current autocorrelation arises from longitudinal processes, challenging previous assumptions about mode coupling.

Findings

The second oscillatory component is linked to longitudinal dynamics.

The signature of longitudinal processes appears in the self part of the autocorrelation.

The behavior is consistent across a wide range of wavevectors.

Abstract

A very recent simulation study of the transverse current autocorrelation of the Lennard-Jones fluid revealed, as expected, that this function can be perfectly described within the exponential expansion theory. However, above a certain wavevector $Q$, not only transverse collective excitations are found to propagate in the fluid, but a second oscillatory component of unclear origin (thereby called X) must be considered to properly account for the time behavior of the correlation. Here we present an extended investigation of the transverse current autocorrelation of liquid Au as obtained by ab initio molecular dynamics in the very wide range 5.7 nm$^{-1}$ $\le Q \le$ 32.8 nm$^{-1}$ in order to follow the behavior of the X component, if present, also at large $Q$ values. By combining the study of the transverse current autocorrelation with the analogous analysis of its self part, we show that the second oscillatory component originates from the longitudinal dynamics and appears in the same form as a collective excitation is represented in the single-particle behavior. Therefore, the signature of the longitudinal processes (sound waves) in the transverse current autocorrelation is not due to often conjectured couplings of longitudinal and trasverse modes, but descends from the self part of the function, which contains the traces of all processes acting in the fluid as the density of states, that is the spectrum of the velocity autocorrelation function, does.