A novel difference between strong liquids and fragile liquids in their dynamics near the glass transition

TL;DR

This paper introduces a unified mean-field theory approach to distinguish the dynamics of strong and fragile liquids near the glass transition, supported by molecular dynamics simulations revealing fundamental differences in their cage region behaviors.

Contribution

It proposes a unified framework based on master curves for analyzing liquid dynamics, revealing distinct behaviors of strong and fragile liquids near the glass transition.

Findings

Master curves $H_n^{(F)}$ and $H_n^{(S)}$ differ in the cage region.

Strong and fragile liquids exhibit different dynamics despite similar diffusion coefficients.

A new type of strong liquid shows different cage dynamics from network glass formers.

Abstract

The systematic method to explore how the dynamics of strong liquids (S) is different from that of fragile liquids (F) near the glass transition is proposed from a unified point of view based on the mean-field theory discussed recently by Tokuyama. The extensive molecular-dynamics simulations are performed on different glass-forming materials. The simulation results for the mean-$n$th displacement $M_n(t)$ are then analyzed from the unified point of view, where $n$ is an even number. Thus, it is first shown that in each type of liquids there exists a master curve $H_n^{(i)}$ as $M_n(t)=R^nH_n^{(i)}(v_{th}t/R;D/Rv_{th})$ onto which any simulation results collapse at the same value of $D/Rv_{th}$, where $R$ is a characteristic length such as an interatomic distance, $D$ a long-time self-diffusion coefficient, $v_{th}$ a thermal velocity, and $i=$F and S. The master curves $H_n^{(F)}$ and $H_n^{(S)}$ are then shown not to coincide with each other in the so-called cage region even at the same value of $D/Rv_{th}$. Thus, it is emphasized that the dynamics of strong liquids is quite different from that of fragile liquids. A new type of strong liquids recently proposed is also tested systematically from this unified point of view. The dynamics of a new type is then shown to be different from that of well-known network glass formers in the cage region, although both liquids are classified as a strong liquid. Thus, it is suggested that a smaller grouping is further needed in strong liquids, depending on whether they have a network or not.