Abstract
Configurational disorder can be compositionally engineered into mixed oxide by populating a single sublattice with many distinct cations. The formulations promote novel and entropy-stabilized forms of crystalline matter where metal cations are incorporated in new ways. Here, through rigorous experiments, a simple thermodynamic model, and a five-component oxide formulation, we demonstrate beyond reasonable doubt that entropy predominates the thermodynamic landscape, and drives a reversible solid-state transformation between a multiphase and single-phase state. In the latter, cation distributions are proven to be random and homogeneous. The findings validate the hypothesis that deliberate configurational disorder provides an orthogonal strategy to imagine and discover new phases of crystalline matter and untapped opportunities for property engineering.
Highlights
A grand challenge facing materials science is the continuous hunt for advanced materials with properties that satisfy the demands of rapidly evolving technology needs
As early as 1926 many of the technologically important materials that remain subjects of contemporary research were identified; BaTiO3, AlN, GaP, ZnO and GaAs are among that list
Inspired by research activities in the metal alloy communities and fundamental principles of thermodynamics we extend the entropy concept to five-component oxides
Summary
A grand challenge facing materials science is the continuous hunt for advanced materials with properties that satisfy the demands of rapidly evolving technology needs. To further expand the library of advanced materials and property opportunities, our community explores possibilities based on mechanical strain[5], artificial layering[6], external fields[7], combinatorial screening[8], interface engineering[9,10] and structuring at the nanoscale[6,11] In many of these efforts, computation and experiment are important companions. High-throughput methods emerged as a powerful engine to assess huge sections of composition space[12,13,14,15,16,17] and identified rapidly new Heusler alloys, extensive ion substitution schemes[18,19], new 18-electron ABX compounds[20] and new ferroic semiconductors[21]. There remains a potential section of discovery space at elevated temperatures where entropy predominates the free-energy landscape
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