Computing Gibbs free energy differences by interface pinning

TL;DR

This paper introduces a novel method to compute Gibbs free energy differences between material phases by analyzing interface forces, validated on models and real elements, showing high accuracy in melting temperature predictions.

Contribution

The paper presents a new interface pinning method for calculating Gibbs free energy differences, applicable to complex materials using density functional theory.

Findings

Accurately predicts melting temperatures for sodium, magnesium, and aluminum.

Successfully applies the method to silicon, with some underestimation.

Demonstrates the method's efficiency and practical applicability.

Abstract

We propose an approach for computing the Gibbs free energy difference between phases of a material. The method is based on the determination of the average force acting on interfaces that separate the two phases of interest. This force, which depends on the Gibbs free energy difference between the phases, is computed by applying an external harmonic field that couples to a parameter which specifies the two phases. Validated first for the Lennard-Jones model, we demonstrate the flexibility, efficiency and practical applicability of this approach by computing the melting temperatures of sodium, magnesium, aluminum and silicon at ambient pressure using density functional theory. Excellent agreement with experiment is found for all four elements, except for silicon, for which the melting temperature is, in agreement with previous simulations, seriously underestimated.