Order evolution from a high-entropy matrix: Understanding and predicting paths to low-temperature equilibrium

Saeed S.I. Almishal, Leixin Miao, Yueze Tan, George N. Kotsonis, Jacob T. Sivak, Nasim Alem, Long Qing Chen, Vincent H. Crespi, Ismaila Dabo, Christina M. Rost, Susan B. Sinnott, Jon Paul Maria

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

Interest in high-entropy inorganic compounds originates from their ability to stabilize cations and anions in local environments that rarely occur at standard temperature and pressure. This leads to new crystalline phases in many-cation formulations with structures and properties that depart from conventional trends. The highest-entropy homogeneous and random solid solution is a parent structure from which a continuum of lower-entropy offspring can originate by adopting chemical and/or structural order. This report demonstrates how synthesis conditions, thermal history, and elastic and chemical boundary conditions conspire to regulate this process in Mg0.2Co0.2Ni0.2Cu0.2Zn0.2O, during which coherent CuO nanotweeds and spinel nanocuboids evolve. We do so by combining structured synthesis routes, atomic-resolution microscopy and spectroscopy, density functional theory, and a phase field modeling framework that accurately predicts the emergent structure and local chemistry. This establishes a framework to appreciate, understand, and predict the macrostate spectrum available to a high-entropy system that is critical to rationalizing property engineering opportunities.

Original languageEnglish (US)
Article numbere20223
JournalJournal of the American Ceramic Society
Volume108
Issue number2
DOIs
StatePublished - Feb 2025

All Science Journal Classification (ASJC) codes

  • Ceramics and Composites
  • Materials Chemistry

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