Static and Dynamic Properties of a Viscous Silica Melt Molecular Dynamics Computer Simulations

TL;DR

This study uses large-scale molecular dynamics simulations to analyze the static and dynamic properties of silica melts across a wide temperature range, revealing structural similarities at high temperatures and a transition in diffusion behavior.

Contribution

It provides new insights into the temperature-dependent structural and dynamic properties of silica melts, including a crossover in diffusion mechanisms and validation against experimental data.

Findings

Structural similarity to low-temperature silica networks at high temperatures

Arrhenius behavior of defect concentration and diffusion constants at low T

Crossover from flow-like to hopping-like motion near T_c=3330 K

Abstract

We present the results of a large scale molecular dynamics computer simulation in which we investigated the static and dynamic properties of a silica melt in the temperature range in which the viscosity of the system changes from O(10^-2) Poise to O(10^2) Poise. We show that even at temperatures as high as 4000 K the structure of this system is very similar to the random tetrahedral network found in silica at lower temperatures. The temperature dependence of the concentration of the defects in this network shows an Arrhenius law. From the partial structure factors we calculate the neutron scattering function and find that it agrees very well with experimental neutron scattering data. At low temperatures the temperature dependence of the diffusion constants $D$ shows an Arrhenius law with activation energies which are in very good agreement with the experimental values. With increasing temperature we find that this dependence shows a cross-over to one which can be described well by a power-law, D\propto (T-T_c)^gamma. The critical temperature T_c is 3330 K and the exponent gamma is close to 2.1. Since we find a similar cross-over in the viscosity we have evidence that the relaxation dynamics of the system changes from a flow-like motion of the particles, as described by the ideal version of mode-coupling theory, to a hopping like motion. We show that such a change of the transport mechanism is also observed in the product of the diffusion constant and the life time of a Si-O bond, or the space and time dependence of the van Hove correlation functions.