Does Stochastic Disorder Conform to Configurational Disorder?

Abstract

In alloy thermodynamics, stochastically disordered state (SDS), where each lattice point is stochastically occupied by constituents according to given composition, is typically referred to investigating physical properties for homogeneously substitutional state: The so-called special quasirandom structure (SQS) of a single microscopic structure, that mimics multisite correlation function for SDS, is amply, widely used for bulk, surface, interface and nano-cluster properties. Despite the widely-used concept for SDS, it has not been clear whether the SDS should conform to configurationally disordered state (CDS) for discrete system, i.e., average over all possible configuration. Here we quantitatively discuss the difference between SDS and CDS for multisite correlation, and show the condition where SDS conforms to CDS. The results show that when practical system size contains below around 100,000 atoms, differences in multisite correlation between SDS and CDS remains few percent depending on the geometry of lattice as well as of figure, indicating that SQS for subsystem of surface and interface, and for isolated clusters, should be carefully applied to investigate high-temperature properties as CDS.