Atomistic characterization of the SiO2 high-density liquid/low-density liquid interface

TL;DR

This study uses molecular dynamics simulations to analyze the structure, thermodynamics, and dynamics of the silica HDL-LDL liquid-liquid interface, revealing complex heterogeneities and phase coexistence features.

Contribution

It provides detailed atomistic insights into the silica HDL-LDL interface, highlighting heterogeneity and phase transition characteristics not previously characterized.

Findings

Identification of a fragile-to-strong transition across the interface.

Observation of three types of dynamical heterogeneity.

Detection of a significant Si/O coordination ratio jump indicating mixing.

Abstract

The equilibrium silica liquid-liquid interface between the high-density liquid (HDL) phase and the low-density liquid (LDL) phase is examined using molecular-dynamics simulation. The structure, thermodynamics, and dynamics within the interfacial region are characterized in detail and compared with previous studies on the liquid-liquid phase transition (LLPT) in bulk silica, as well as traditional crystal-melt interfaces. We find that the silica HDL-LDL interface exhibits a spatial fragile-to-strong transition across the interface. Calculations of dynamics properties reveal three types of dynamical heterogeneity hybridizing within the silica HDL-LDL interface. We also observe that as the interface is traversed from HDL to LDL, the Si/O coordination number ratio jumps to an unexpectedly large value, defining a thin region of the interface where HDL and LDL exhibit significant mixing. In addition, the LLPT phase coexistence is interpreted in the framework of the traditional thermodynamics of alloys and phase equilibria.