Yateng Wang, Bianca Baldassarri, Jiahong Shen, Jiangang He, Chris Wolverton
{"title":"A2BB′O6 化合物的热力学稳定性景观","authors":"Yateng Wang, Bianca Baldassarri, Jiahong Shen, Jiangang He, Chris Wolverton","doi":"10.1021/acs.chemmater.4c00576","DOIUrl":null,"url":null,"abstract":"Perovskite oxides have been extensively studied for their wide range of compositions and structures, as well as their valuable properties for various applications. Expanding from single-perovskite <i>AB</i>O<sub>3</sub> to double-perovskite <i>A</i><sub>2</sub><i>BB</i>′O<sub>6</sub> significantly enhances the ability to tailor specific physical and chemical properties. However, the vast number of potential compositions of <i>A</i><sub>2</sub><i>BB</i>′O<sub>6</sub> makes it impractical to explore all of them experimentally. In this study, we conducted high-throughput calculations to systematically investigate the structures and stabilities of 4900 <i>A</i><sub>2</sub><i>BB</i>′O<sub>6</sub> compositions (with <i>A</i> = Ca, Sr, Ba, and La; <i>B</i> and <i>B</i>′ representing metal elements) through over 42 000 density functional theory (DFT) calculations. Our analysis lead to the discovery of more than 1500 new <i>A</i><sub>2</sub><i>BB</i>′O<sub>6</sub> compounds, with over 1100 of them exhibiting double perovskite structures, predominantly in the space group. By leveraging the high-throughput dataset, we developed machine learning models that achieved mean absolute errors of 0.0422 and 0.0329 eV/atom for formation energy and decomposition energy, respectively. Using these models, we identified 803 stable or metastable compositions beyond the chemical space covered in our initial calculations, with 612 of them having DFT-validated decomposition energies below 0.1 eV/atom, resulting in a success rate of 76.2%. This study delineates the stability landscape of <i>A</i><sub>2</sub><i>BB</i>′O<sub>6</sub> compounds and offers new insights for exploration of these materials.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":null,"pages":null},"PeriodicalIF":7.2000,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Landscape of Thermodynamic Stabilities of A2BB′O6 Compounds\",\"authors\":\"Yateng Wang, Bianca Baldassarri, Jiahong Shen, Jiangang He, Chris Wolverton\",\"doi\":\"10.1021/acs.chemmater.4c00576\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Perovskite oxides have been extensively studied for their wide range of compositions and structures, as well as their valuable properties for various applications. Expanding from single-perovskite <i>AB</i>O<sub>3</sub> to double-perovskite <i>A</i><sub>2</sub><i>BB</i>′O<sub>6</sub> significantly enhances the ability to tailor specific physical and chemical properties. However, the vast number of potential compositions of <i>A</i><sub>2</sub><i>BB</i>′O<sub>6</sub> makes it impractical to explore all of them experimentally. In this study, we conducted high-throughput calculations to systematically investigate the structures and stabilities of 4900 <i>A</i><sub>2</sub><i>BB</i>′O<sub>6</sub> compositions (with <i>A</i> = Ca, Sr, Ba, and La; <i>B</i> and <i>B</i>′ representing metal elements) through over 42 000 density functional theory (DFT) calculations. Our analysis lead to the discovery of more than 1500 new <i>A</i><sub>2</sub><i>BB</i>′O<sub>6</sub> compounds, with over 1100 of them exhibiting double perovskite structures, predominantly in the space group. By leveraging the high-throughput dataset, we developed machine learning models that achieved mean absolute errors of 0.0422 and 0.0329 eV/atom for formation energy and decomposition energy, respectively. Using these models, we identified 803 stable or metastable compositions beyond the chemical space covered in our initial calculations, with 612 of them having DFT-validated decomposition energies below 0.1 eV/atom, resulting in a success rate of 76.2%. This study delineates the stability landscape of <i>A</i><sub>2</sub><i>BB</i>′O<sub>6</sub> compounds and offers new insights for exploration of these materials.\",\"PeriodicalId\":33,\"journal\":{\"name\":\"Chemistry of Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":7.2000,\"publicationDate\":\"2024-06-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemistry of Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.chemmater.4c00576\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemistry of Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acs.chemmater.4c00576","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Landscape of Thermodynamic Stabilities of A2BB′O6 Compounds
Perovskite oxides have been extensively studied for their wide range of compositions and structures, as well as their valuable properties for various applications. Expanding from single-perovskite ABO3 to double-perovskite A2BB′O6 significantly enhances the ability to tailor specific physical and chemical properties. However, the vast number of potential compositions of A2BB′O6 makes it impractical to explore all of them experimentally. In this study, we conducted high-throughput calculations to systematically investigate the structures and stabilities of 4900 A2BB′O6 compositions (with A = Ca, Sr, Ba, and La; B and B′ representing metal elements) through over 42 000 density functional theory (DFT) calculations. Our analysis lead to the discovery of more than 1500 new A2BB′O6 compounds, with over 1100 of them exhibiting double perovskite structures, predominantly in the space group. By leveraging the high-throughput dataset, we developed machine learning models that achieved mean absolute errors of 0.0422 and 0.0329 eV/atom for formation energy and decomposition energy, respectively. Using these models, we identified 803 stable or metastable compositions beyond the chemical space covered in our initial calculations, with 612 of them having DFT-validated decomposition energies below 0.1 eV/atom, resulting in a success rate of 76.2%. This study delineates the stability landscape of A2BB′O6 compounds and offers new insights for exploration of these materials.
期刊介绍:
The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.