Ying Li , Guangyao Li , Xiaoxin Xu , Xiaofang Peng , Shihua Tan , Yabei Wu
{"title":"HfRu1.5Sb中空位有序-无序跃迁和能带收敛的第一性原理研究","authors":"Ying Li , Guangyao Li , Xiaoxin Xu , Xiaofang Peng , Shihua Tan , Yabei Wu","doi":"10.1016/j.mtphys.2025.101848","DOIUrl":null,"url":null,"abstract":"<div><div>The discovery of vacancy-driven short-range order in the half-Heusler-like HfRu<sub>1.5</sub>Sb is reported, along with its quantified impact on the electronic structure. By integrating density-functional total energies with cluster expansion and large-cell Monte-Carlo annealing simulation, it was found that the order-disorder phase transition occurred at 1100K, which is consistent with the experimental 1170K. And two nearly degenerate ground-state configurations (GS1 and GS2) are identified at room temperature, distinguished by the spatial arrangement of Ru vacancies on the 4d sub-lattice. Although short-range order parameters reveal similar ordering tendencies in both GS1 and GS2, it is specifically in GS2 that Ru vacancies form tetrahedral configurations encapsulating Hf atoms, thereby weakening adjacent Hf–Ru bonding interaction. These tetrahedral motifs introduce additional valence band valleys, whose weight scales with the degree of disordering, enhancing the band convergence effects. This study systematically reveals the formation mechanism of the order-disorder transition of vacancies in HfRu<sub>1+x</sub>Sb and its effect on the electronic structure, providing theoretical guidance for optimizing thermoelectric performance and designing advanced half-Heusler-like materials.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"58 ","pages":"Article 101848"},"PeriodicalIF":9.7000,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Vacancy order–disorder transition and band convergence in HfRu1.5Sb: A first-principles study\",\"authors\":\"Ying Li , Guangyao Li , Xiaoxin Xu , Xiaofang Peng , Shihua Tan , Yabei Wu\",\"doi\":\"10.1016/j.mtphys.2025.101848\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The discovery of vacancy-driven short-range order in the half-Heusler-like HfRu<sub>1.5</sub>Sb is reported, along with its quantified impact on the electronic structure. By integrating density-functional total energies with cluster expansion and large-cell Monte-Carlo annealing simulation, it was found that the order-disorder phase transition occurred at 1100K, which is consistent with the experimental 1170K. And two nearly degenerate ground-state configurations (GS1 and GS2) are identified at room temperature, distinguished by the spatial arrangement of Ru vacancies on the 4d sub-lattice. Although short-range order parameters reveal similar ordering tendencies in both GS1 and GS2, it is specifically in GS2 that Ru vacancies form tetrahedral configurations encapsulating Hf atoms, thereby weakening adjacent Hf–Ru bonding interaction. These tetrahedral motifs introduce additional valence band valleys, whose weight scales with the degree of disordering, enhancing the band convergence effects. This study systematically reveals the formation mechanism of the order-disorder transition of vacancies in HfRu<sub>1+x</sub>Sb and its effect on the electronic structure, providing theoretical guidance for optimizing thermoelectric performance and designing advanced half-Heusler-like materials.</div></div>\",\"PeriodicalId\":18253,\"journal\":{\"name\":\"Materials Today Physics\",\"volume\":\"58 \",\"pages\":\"Article 101848\"},\"PeriodicalIF\":9.7000,\"publicationDate\":\"2025-08-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Materials Today Physics\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2542529325002044\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Materials Today Physics","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2542529325002044","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
Vacancy order–disorder transition and band convergence in HfRu1.5Sb: A first-principles study
The discovery of vacancy-driven short-range order in the half-Heusler-like HfRu1.5Sb is reported, along with its quantified impact on the electronic structure. By integrating density-functional total energies with cluster expansion and large-cell Monte-Carlo annealing simulation, it was found that the order-disorder phase transition occurred at 1100K, which is consistent with the experimental 1170K. And two nearly degenerate ground-state configurations (GS1 and GS2) are identified at room temperature, distinguished by the spatial arrangement of Ru vacancies on the 4d sub-lattice. Although short-range order parameters reveal similar ordering tendencies in both GS1 and GS2, it is specifically in GS2 that Ru vacancies form tetrahedral configurations encapsulating Hf atoms, thereby weakening adjacent Hf–Ru bonding interaction. These tetrahedral motifs introduce additional valence band valleys, whose weight scales with the degree of disordering, enhancing the band convergence effects. This study systematically reveals the formation mechanism of the order-disorder transition of vacancies in HfRu1+xSb and its effect on the electronic structure, providing theoretical guidance for optimizing thermoelectric performance and designing advanced half-Heusler-like materials.
期刊介绍:
Materials Today Physics is a multi-disciplinary journal focused on the physics of materials, encompassing both the physical properties and materials synthesis. Operating at the interface of physics and materials science, this journal covers one of the largest and most dynamic fields within physical science. The forefront research in materials physics is driving advancements in new materials, uncovering new physics, and fostering novel applications at an unprecedented pace.