{"title":"Dimensionality and strain-dependent properties of Orthorhombic (100) NaTaO3 thin films: A comprehensive DFT investigation","authors":"","doi":"10.1016/j.commatsci.2024.113335","DOIUrl":null,"url":null,"abstract":"<div><p>The modulation of perovskite oxide thin films’ properties, through both intrinsic and extrinsic methods, has been extensively studied to enhance their photocatalytic performance. We employed <em>ab initio</em> density functional theory calculations to investigate the layer-dependent structural and electronic properties of orthorhombic NaTaO<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span> thin films. Our findings reveal that slabs comprising five, four, and three layers retain the non-magnetic and semiconducting characteristics of the bulk material, with their properties progressively converging towards those of an infinite-surface slab as the number of layers increases. Biaxial in-plane strain induces a linear change in the structure of surface TaO<span><math><msub><mrow></mrow><mrow><mn>4</mn></mrow></msub></math></span> tetrahedra, thereby altering the film’s band gap. Notably, the two-layer slab exhibits a transitional behavior between the bulk-like nature of thicker films and the unique features of a NaTaO<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span> monolayer, showing heightened sensitivity to strain. Under compression, this bilayered system acquires bulk-like properties, whereas its strain-free state is magnetic and metallic akin to the monolayer. Similar transitions are observed in the latter, though under higher compression values. We provide an in-depth discussion of the structural and electronic mechanisms underlying these transitions. Additionally, the relative band-edge alignment with water-splitting photocatalytic potentials underscores the complex interplay between strain and dimensionality. This work offers valuable insights towards the design of more efficient photocatalysts, highlighting the potential of engineered NaTaO<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span> thin-film structures for advancing photocatalytic applications.</p></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":null,"pages":null},"PeriodicalIF":3.1000,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Computational Materials Science","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0927025624005561","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
The modulation of perovskite oxide thin films’ properties, through both intrinsic and extrinsic methods, has been extensively studied to enhance their photocatalytic performance. We employed ab initio density functional theory calculations to investigate the layer-dependent structural and electronic properties of orthorhombic NaTaO thin films. Our findings reveal that slabs comprising five, four, and three layers retain the non-magnetic and semiconducting characteristics of the bulk material, with their properties progressively converging towards those of an infinite-surface slab as the number of layers increases. Biaxial in-plane strain induces a linear change in the structure of surface TaO tetrahedra, thereby altering the film’s band gap. Notably, the two-layer slab exhibits a transitional behavior between the bulk-like nature of thicker films and the unique features of a NaTaO monolayer, showing heightened sensitivity to strain. Under compression, this bilayered system acquires bulk-like properties, whereas its strain-free state is magnetic and metallic akin to the monolayer. Similar transitions are observed in the latter, though under higher compression values. We provide an in-depth discussion of the structural and electronic mechanisms underlying these transitions. Additionally, the relative band-edge alignment with water-splitting photocatalytic potentials underscores the complex interplay between strain and dimensionality. This work offers valuable insights towards the design of more efficient photocatalysts, highlighting the potential of engineered NaTaO thin-film structures for advancing photocatalytic applications.
期刊介绍:
The goal of Computational Materials Science is to report on results that provide new or unique insights into, or significantly expand our understanding of, the properties of materials or phenomena associated with their design, synthesis, processing, characterization, and utilization. To be relevant to the journal, the results should be applied or applicable to specific material systems that are discussed within the submission.