Perfect short-range ordered alloy with line-compound-like properties in the ZnSnN₂:ZnO system

Inorganic crystalline materials are either line compounds or solid solutions, and computational materials discovery has so far focused primarily on the former. We here present a new condensed-matter phase which is a disordered solid solution but offers many ordered line-compound features. The emergent physical phenomena are rooted in the perfect short-range order. We model the dual-sublattice mixed semiconductor alloy (ZnSnN2)1-x(ZnO)2x using first-principles calculations, Monte- Carlo simulations with a model Hamiltonian, and an extension of the regular solution model by incorporating short-range order. We demonstrate that this unique solid solution, occurring at a “magic” composition, can provide an electronically pristine character without disorder-induced charge localization and, therefore, a superior carrier transport similar to ordered phases. Interestingly, this phase shows singularities that are absent in the conventional solid-solution models, such as the regular solution and band-gap bowing model. Thermodynamically, this alloy phase has a sharply reduced enthalpy at its composition (like a line compound), but it still requires the entropy from long-range disorder to be stabilized at experimentally accessible temperatures.