CASM Monte Carlo: Calculations of the thermodynamic and kinetic properties of complex multicomponent crystals

Puchala, Brian [University of Michigan Ann Arbor, MI (United States)] (ORCID:0000000224616614); Thomas, John C. [University of California, Santa Barbara, CA (United States)]; Van der Ven, Anton [University of California, Santa Barbara, CA (United States)]

doi:10.1016/j.commatsci.2025.114091

DOE OSTI · 2970757

CASM Monte Carlo: Calculations of the thermodynamic and kinetic properties of complex multicomponent crystals

Puchala, Brian [University of Michigan Ann Arbor, MI (United States)] (ORCID:0000000224616614)·Thomas, John C. [University of California, Santa Barbara, CA (United States)]·Van der Ven, Anton [University of California, Santa Barbara, CA (United States)]

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Abstract

Monte Carlo techniques play a central role in statistical mechanics approaches that connect macroscopic thermodynamic and kinetic properties to the electronic structure of a material. This paper describes the implementation of Monte Carlo techniques for the study of multicomponent crystalline materials within the Clusters Approach to Statistical Mechanics (CASM) software suite, and demonstrates their use in model systems to calculate free energies and kinetic coefficients, study phase transitions, and construct phase diagrams from first principles. Many crystal structures are complex, with multiple sublattices occupied by differing sets of chemical species, along with the presence of vacancies or interstitial species. This imposes constraints on concentration variables, the form of thermodynamic potentials, and the values of kinetic transport coefficients. The framework used by CASM to formulate thermodynamic potentials and kinetic transport coefficients accounting for arbitrarily complex crystal structures is presented and demonstrated with examples of increasing complexity. Additionally, an overview of the capabilities of the CASM software specific to Monte Carlo methods is given, and a new CASM software package is introduced, casm-flow, which helps automate the setup, submission, management, and analysis of Monte Carlo simulations.

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Puchala, Brian [University of Michigan Ann Arbor, MI (United States)] (ORCID:0000000224616614), Thomas, John C. [University of California, Santa Barbara, CA (United States)], Van der Ven, Anton [University of California, Santa Barbara, CA (United States)]. 2025-08-27. CASM Monte Carlo: Calculations of the thermodynamic and kinetic properties of complex multicomponent crystals. https://doi.org/10.1016/j.commatsci.2025.114091

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