Zhongxiong Sun, Jinjin Yang, Yifeng Han, Man-Rong Li
{"title":"负化学压力下 Ag2B(IV)B′(VI)O6 的数据驱动型高通量筛选和实验实现","authors":"Zhongxiong Sun, Jinjin Yang, Yifeng Han, Man-Rong Li","doi":"10.1021/acs.chemmater.4c00300","DOIUrl":null,"url":null,"abstract":"Harsh synthetic conditions and high cost seriously hinder the discoveries of metastable materials under extreme conditions. Extending the big-data-driven high-throughput calculation (HTC) to depict the chemically negative pressure (NP) zone enables the creation of efficient and accurate prediction models over the full pressure range. This approach significantly expedites the exploration and discovery of novel multifunctional metastable materials. Here, double perovskites Ag<sub>2</sub><i>B</i>(IV)<i>B</i><b>′</b>(VI)O<sub>6</sub> were adopted to illustrate the comprehensive process of big-data-mining, HTC, and experimental realization under chemically NP. High-throughput screening of 32 Ag<sub>2</sub><i>BB</i><b>′</b>O<sub>6</sub> compounds, encompassing 9 possible crystal structures and 23 derived magnetic structures, resulting in 1024 potential candidates. Ag<sub>2</sub>MnTeO<sub>6</sub> (AMTO) and Ag<sub>2</sub>TiTeO<sub>6</sub> (ATTO) were selected for the experimental validation. We captured a new polymorph of AMTO (<i>R</i>-3, 3<i>R</i>) at ambient pressure through ion-exchange reaction, a phase theoretically predicted to be stable under NP about −6.6 GPa. Moreover, as predicted by density functional theory calculations, the <i>P</i>-31<i>c</i> (2<i>H</i>) AMTO is an antiferromagnetic semiconductor with magnetic transition at 3 K and direct band gap ∼0.97 eV. This work is expected to guide the exploration of hidden metastable phase by providing a methodological framework and novel conceptual approach for future research.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":null,"pages":null},"PeriodicalIF":7.2000,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Data-Driven High-Throughput Screening and Experimental Realization of Ag2B(IV)B′(VI)O6 under Negative Chemical-Pressure\",\"authors\":\"Zhongxiong Sun, Jinjin Yang, Yifeng Han, Man-Rong Li\",\"doi\":\"10.1021/acs.chemmater.4c00300\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Harsh synthetic conditions and high cost seriously hinder the discoveries of metastable materials under extreme conditions. Extending the big-data-driven high-throughput calculation (HTC) to depict the chemically negative pressure (NP) zone enables the creation of efficient and accurate prediction models over the full pressure range. This approach significantly expedites the exploration and discovery of novel multifunctional metastable materials. Here, double perovskites Ag<sub>2</sub><i>B</i>(IV)<i>B</i><b>′</b>(VI)O<sub>6</sub> were adopted to illustrate the comprehensive process of big-data-mining, HTC, and experimental realization under chemically NP. High-throughput screening of 32 Ag<sub>2</sub><i>BB</i><b>′</b>O<sub>6</sub> compounds, encompassing 9 possible crystal structures and 23 derived magnetic structures, resulting in 1024 potential candidates. Ag<sub>2</sub>MnTeO<sub>6</sub> (AMTO) and Ag<sub>2</sub>TiTeO<sub>6</sub> (ATTO) were selected for the experimental validation. We captured a new polymorph of AMTO (<i>R</i>-3, 3<i>R</i>) at ambient pressure through ion-exchange reaction, a phase theoretically predicted to be stable under NP about −6.6 GPa. Moreover, as predicted by density functional theory calculations, the <i>P</i>-31<i>c</i> (2<i>H</i>) AMTO is an antiferromagnetic semiconductor with magnetic transition at 3 K and direct band gap ∼0.97 eV. This work is expected to guide the exploration of hidden metastable phase by providing a methodological framework and novel conceptual approach for future research.\",\"PeriodicalId\":33,\"journal\":{\"name\":\"Chemistry of Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":7.2000,\"publicationDate\":\"2024-07-09\",\"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.4c00300\",\"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.4c00300","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}
Data-Driven High-Throughput Screening and Experimental Realization of Ag2B(IV)B′(VI)O6 under Negative Chemical-Pressure
Harsh synthetic conditions and high cost seriously hinder the discoveries of metastable materials under extreme conditions. Extending the big-data-driven high-throughput calculation (HTC) to depict the chemically negative pressure (NP) zone enables the creation of efficient and accurate prediction models over the full pressure range. This approach significantly expedites the exploration and discovery of novel multifunctional metastable materials. Here, double perovskites Ag2B(IV)B′(VI)O6 were adopted to illustrate the comprehensive process of big-data-mining, HTC, and experimental realization under chemically NP. High-throughput screening of 32 Ag2BB′O6 compounds, encompassing 9 possible crystal structures and 23 derived magnetic structures, resulting in 1024 potential candidates. Ag2MnTeO6 (AMTO) and Ag2TiTeO6 (ATTO) were selected for the experimental validation. We captured a new polymorph of AMTO (R-3, 3R) at ambient pressure through ion-exchange reaction, a phase theoretically predicted to be stable under NP about −6.6 GPa. Moreover, as predicted by density functional theory calculations, the P-31c (2H) AMTO is an antiferromagnetic semiconductor with magnetic transition at 3 K and direct band gap ∼0.97 eV. This work is expected to guide the exploration of hidden metastable phase by providing a methodological framework and novel conceptual approach for future research.
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.