Solid-liquid coexistence in small systems: A statistical method to calculate melting temperatures

Abstract

We propose an efficient and accurate scheme to calculate the melting point (MP) of materials. This method is based on the statistical analysis of small-size coexistence molecular dynamics simulations. It eliminates the risk of metastable superheated solid in the fast-heating method, while also significantly reducing the computer cost relative to the traditional large-scale coexistence method. Using empirical potentials, we validate the method and systematically study the finite-size effect on the calculated MPs. The method converges to the exact result in the limit of large system size. An accuracy within 100 K in MP is usually achieved when simulation contains more than 100 atoms. Density functional theory examples of tantalum, high-pressure sodium, and ionic material NaCl are shown to demonstrate the accuracy and flexibility of the method in its practical applications. The method serves as a promising approach for large-scale automated material screening in which the MP is a design criterion.