A Machine Learning Approach for the Prediction of Formability and Thermodynamic Stability of Single and Double Perovskite Oxides

• Published in: Chemistry of materials 2021-02, Vol.33 (3), p.845-858
• Main Authors: Talapatra, Anjana, Uberuaga, Blas P, Stanek, Christopher R, Pilania, Ghanshyam
• Format: Article
• Language: English
• Subjects: cations; energy; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Machine learning, perovskites, high-throughput screening; oxides; perovskites; stability
• ISSN: 0897-4756; 1520-5002
• DOI: 10.1021/acs.chemmater.0c03402

Perovskite oxides continue to attract huge interest due to their fascinating and wide-ranging properties for diverse applications. The tunability of these properties may be further enhanced by increasing their compositional complexity via double perovskite-ordered configurations containing multiple cations. In this work, we focus on an exhaustive chemical space of single and double oxide perovskites and optimally explore this space to identify novel compositions that are likely to form stable compounds. Critically, we examine the relationship between formability, the practical ability to synthesize a compound, and stability, the thermodynamic preference to form the structure. Our formability and stability training data sets were enumerated from the available experimental literature and in-house density functional theory computations and contained 1505 and 3469 examples, respectively, representing state-of-the-art in the current open literature in perovskite and double perovskite compounds. Subsequently, cross-validated and highly accurate machine learning classification models are built using these training data sets and employed to screen for novel stable oxide perovskites. The study identifies (1) atomic features relevant to prediction of formability and stability in perovskite and double perovskite compounds, (2) the importance of including energy contributions due to local structural relaxations going beyond the high symmetry perovskite phase, and (3) 437,828 double perovskite compounds that are likely to be stable and 891,188 compounds that are likely to be formable. From the intersection of this large chemical space of formable and stable oxide perovskites, 414 compositions are identified as the most promising candidates for future experimental synthesis of novel oxide perovskites. The developed models may be generalized and have implications beyond perovskite discovery if applied to other families of compounds.