Topic:
Theory and simulations reveal routes to eliminate competing impurities and pave the way for the synthesis of novel multi-component oxides. This method for predicting impurity phases and cation disorder as a function of oxygen partial pressure and temperature enables future synthesis of metastable phases with tailored ion and thermal transport.
First principles calculations are used to generate binary mixing maps for different crystal structures including oxygen vacancies. Monte Carlo simulations use these maps to predict impurity fractions as a function of synthesis conditions. Iterative loops with synthesis efforts refine out impurities to achieve phase pure La- and Nd-based pyrochlores. Initial failures in synthesis were corrected with theory insights of phase diagrams that support pure metastable phases. DOI: 10.1021/acs.chemmater.1c02361
