Compositional asymmetry of disordered structure: Role of spatial constraint

TL;DR

This paper reveals that the compositional asymmetry in disordered structures under spatial constraints can be universally characterized by specific microscopic structures, independent of interactions or temperature, with practical predictive applications.

Contribution

It introduces a universal framework to characterize compositional asymmetry in disordered systems based solely on spatial constraints, without requiring interaction or temperature data.

Findings

Analytical expression for temperature dependence of disordered structures.

Validation through prediction of short-range order parameters in alloys.

Demonstration of applicability without interaction or temperature information.

Abstract

When spatial constraint for the constituents (e.g., atom or particle) of system is once given, disordered structure for non-interacting system in equilibrium states is symmetric with respect to equiatomic composition. Meanwhile, when the interaction between constituents is introduced, this symmetry is typically broken, naturally appearing compositional asymmetry. Although this asymmetry, depending on temperature, comes from multibody interactions in the system, we here clarify that the asymmetry near equiatomic composition can be universally well-characterized by two specially selected microscopic structure, which can be known a priori without any information about interactions or temperature: The key role is the class of spatial constraint. Based on the facts, we provide analytical expression of temperature dependence of disordered structure, and demonstrate its validity and applicability by predicting short-range order parameters of practical alloys compared with full thermodynamic simulation.