Robustness of the cluster expansion: Assessing the roles of relaxation and numerical error

AH Nguyen and CW Rosenbrock and CS Reese and GLW Hart, PHYSICAL REVIEW B, 96, 014107 (2017).

DOI: 10.1103/PhysRevB.96.014107

Cluster expansion (CE) is effective in modeling the stability of metallic alloys, but sometimes cluster expansions fail. Failures are often attributed to atomic relaxation in the DFT-calculated data, but there is no metric for quantifying the degree of relaxation. Additionally, numerical errors can also be responsible for slow CE convergence. We studied over one hundred different Hamiltonians and identified a heuristic, based on a normalized mean-squared displacement of atomic positions in a crystal, to determine if the effects of relaxation in CE data are too severe to build a reliable CE model. Using this heuristic, CE practitioners can determine a priori whether or not an alloy system can be reliably expanded in the cluster basis. We also examined the error distributions of the fitting data. We find no clear relationship between the type of error distribution and CE prediction ability, but there are clear correlations between CE formalism reliability, model complexity, and the number of significant terms in the model. Our results show that the size of the errors is much more important than their distribution.

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