Computationally accelerated discovery of high entropy pyrochlore oxides [post]

Krishna Chaitanya Pitike, Antonio Macias, Markus Eisenbach, Craig Bridges, Valentino Cooper
2021 unpublished
High entropy ceramics provide enhanced flexibility for tailoring a wide range of physical properties, emerging from the diverse chemical and configurational degrees of freedom. Expanding upon the endeavors of recently synthesized high entropy ceramics in rock salt, fluorite, spinel and perovskite structures, we explore the relative feasibility of formation of high entropy pyrochlore oxides, A2B2O7, with multi-cation occupancy of the B-site, estimated from first principles based thermodynamic
more » ... ed thermodynamic descriptors. Subsequently, we used Monte Carlo simulations to estimate the phase composition, oxygen vacancy concentration and local ionic segregation as a function of temperature and oxygen partial pressure. In parallel, we have investigated the synthesis of several multicomponent oxides with a pyrochlore composition, related to our computational investigations, resulting in several high purity pyrochlore oxides, in some cases with minor impurity phases. Ultimately, our approach allows us to evaluate potential impurity phases, ionic disorder and oxygen vacancy concentration in response to the experimental variables, thereby making realistic predictions that can direct and accelerate experimental synthesis of novel multicomponent ceramics.
doi:10.21203/rs.3.rs-405947/v1 fatcat:7lffcp3qa5ftjoj3phezucbs3m