Green-Kubo stress correlation function at the atomic scale and a long-range bond-orientational ordering in a model liquid

TL;DR

This paper investigates the Green-Kubo stress correlation function at the atomic scale using pairwise stress tensors, revealing long-range bond-orientational order in a model liquid and its relation to viscosity, with implications for understanding stress wave propagation.

Contribution

It introduces a microscopic approach based on pair stress tensors, highlighting the long-range bond-orientational order and its clearer manifestation in pair stress correlation functions compared to atomic ones.

Findings

Long-range bond-orientational order exists in the model liquid.

Bond-orientational order is more evident in pair stress correlations.

Stress waves are better observed in atomic stress correlation functions.

Abstract

Recently there have been several considerations by different authors of viscosity and the Green-Kubo stress correlation function from the microscopic perspective. In most of these and earlier works the atomic level stress is the minimal element of stress. It is also possible to consider, for pairwise interaction potentials, as the minimal elements of stress, the stress tensors associated with the pairs of interacting particles. From this perspective, the atomic level stress is not the minimal stress element, but a sum of all pair stress elements in which involved a selected particle. In this paper, we consider the Green-Kubo stress correlation function from a microscopic perspective using the stress tensors of interacting pairs as the basic stress elements. The obtained results show the presence of a long-range bond-orientational order in the studied model liquid and naturally elucidate the connection of the bond-orientational order with viscosity. It turns out that the long-range bond-orientational order is more clearly expressed in the pairs' stress correlation function than in the atomic stress correlation function. On the other hand, previously observed stress waves are much better expressed in the atomic stress correlation functions. We also address the close connection of our approach with the previous bond-orientational order considerations. Finally, we consider the probability distributions for the bond-stress and atomic stress correlation products at selected distances. The character of the obtained probability distributions raises questions about the meaning of the average correlation functions at large distances.