Atomistic View of Homogeneous Nucleation of Water into Polymorphic Ices

TL;DR

This study uses atomistic simulations and enhanced sampling to explore the thermodynamics and nucleation mechanisms of various ice phases, providing insights consistent with experimental observations.

Contribution

It introduces a novel simulation approach combining MetaITS with X-ray diffraction peaks to map phase diagrams and explain ice stability.

Findings

Reversible water-ice phase transitions simulated at atomistic level

Phase diagrams of water, Ice Ih, and Ice Ic constructed

A simple physical model explains ice thermodynamic stability

Abstract

Water is one of the most abundant substances on Earth, and ice, i.e., solid water, has more than 18 known phases. Normally ice in nature exists only as Ice Ih, Ice Ic, or a stacking disordered mixture of both. Although many theoretical efforts have been devoted to understanding the thermodynamics of different ice phases at ambient temperature and pressure, there still remains many puzzles. We simulated the reversible transitions between water and different ice phases by performing full atom molecular dynamics simulations. Using the enhanced sampling method MetaITS with the two selected X-ray diffraction peak intensities as collective variables, the ternary phase diagrams of liquid water, ice Ih, ice Ic at multiple were obtained. We also present a simple physical model which successfully explains the thermodynamic stability of ice. Our results agree with experiments and leads to a deeper understanding of the ice nucleation mechanism.