Homogeneous TIP4P/2005 ice nucleation at low supercooling

TL;DR

This study provides a detailed free energy profile for homogeneous ice nucleation at low supercooling using an all-atom water model, confirming classical nucleation theory and highlighting the entropic nature of the nucleation barrier.

Contribution

It offers the first detailed free energy profile for ice nucleation at low supercooling with an all-atom model, validating classical theory and estimating temperature effects.

Findings

Free energy profile aligns with classical nucleation theory

Nucleation barrier is primarily entropic

Estimated temperature dependence of interfacial free energy

Abstract

We present a partial free energy profile for the homogeneous nucleation of ice using an all-atom model of water at low supercooling, at which ice growth dynamics are reasonably accessible to simulation. We demonstrate that the free energy profile is well described by classical nucleation theory, and that the nucleation barrier is entropic in origin. We also estimate to first order the temperature dependence of the interfacial free energy.