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arxiv 2305.01806 v1 pith:O75RUPN5 submitted 2023-05-02 cond-mat.mtrl-sci physics.chem-ph

Data-Driven, Physics-Informed Descriptors of Cation Ordering in Multicomponent Oxides

classification cond-mat.mtrl-sci physics.chem-ph
keywords orderingoxidesdescriptorsmulticomponentcationdata-drivendisorderedexperimental
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The structural tunability and compositional diversity of multicomponent perovskite oxides have enabled their various applications, including catalysis and electronics. The cation ordering in these oxides, ranging from disordered (i.e., high-entropy) to ordered (e.g., rocksalt), profoundly influences their properties. While computational design tools can typically predict properties associated with a particular ordering, inferring which ordering -- if any -- will be observed in synthesized oxides remains challenging. Here, we leveraged first-principles simulations and machine learning to develop data-driven, physics-informed descriptors of experimental ordering in multicomponent perovskites and compared them with traditional physicochemical descriptors, e.g., ionic radii and oxidation states. The fitted low-dimensional classification models correctly rank up to 93% of compositions in an experimental dataset of 190 perovskites between cation-ordered and disordered, offering a rigorous benchmark between theory and experiments. Furthermore, these descriptors accelerate high-throughput virtual screening of multicomponent oxides by predicting their dominant ordering to avoid costly, exhaustive simulations of cation arrangements.

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