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First-principles predictions of new superhard magnetic clathrate material β-C3N2 through atom embeddedness

基于第一性原理的β-C3N2笼中原子嵌入引起的超硬 磁性新材料设计

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Abstract

Using first-principles calculations, we predict the coexistence of mechanical superhardness and the controllable magnetism in the clathrate material β-C3N2 through the implant of the external atom into the intrinsic cage structure. Taking hydrogen-doping (H@β-C3N2) and fluorine-doping (F@β-C3N2) as examples, our calculations indicate these two doped configurations are stable and discover that they belong to antiferromagnetic semiconductor and ferromagnetic semi-metal, respectively. These intriguing magnetic phase transitions originate from their distinctive band structures around the Fermi level and can be well understood by the three-dimensional Hubbard model with half-filling occupation and the Stoner model. Moreover, the high Vickers hardness of 49.0 GPa for H@β-C3N2 and 48.2 GPa for F@β-C3N2 are obtained, suggesting they are clathrate superhard materials as their host. Therefore, the incorporations of H and F in β-C3N2 give rise to new types of superhard antiferromagnetic semiconductor and superhard ferromagnetic semimetal, respectively, which could have potential applications in harsh conditions. Our work provides an effective strategy to design a new class of highly desirable multifunctional materials with excellent mechanical properties and magnetic properties, which may arouse spintronic applications in superhard materials in the future.

摘要

基于第一性原理计算, 我们通过将客体原子嵌入β-C3N2笼状结构 的内在空腔中, 预测了机械超硬和可控磁性的共存. 以氢掺杂(H@β-C3N2)和氟掺杂(F@β-C3N2)为例, 我们的研究表明两种掺杂构型是稳定 的, 并发现它们分别属于反铁磁半导体和铁磁半金属. 这些有趣的磁相 变源于它们在费米能级周围独特的能带结构, 并可通过具有半填充占 据的3D Hubbard模型和Stoner模型很好地解释. 此外, H@β-C3N2和 F@β-C3N2的高维氏硬度(49.0和48.2 GPa)表明它们具有笼状超硬材料 特征. 因此, 氢和氟在β-C3N2笼中的掺杂分别产生了一种新型的超硬反 铁磁半导体和超硬铁磁半金属, 这些材料在极端条件下具有潜在的应 用前景. 我们的工作为设计具有优异机械性能和磁性的新型高性能多 功能材料提供了一种有效的策略, 这可能会为超硬材料未来在自旋电 子学的应用提供理论依据.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (12204330) and Sichuan Normal University for financial support (341829001).

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Authors and Affiliations

  1. College of Physics and Electronic Engineering, Sichuan Normal University, Chengdu, 610068, China

    Liping Sun  (孙丽萍) & Jing Chang  (常景)

  2. College of Physics and Electronic Engineering, Center for Computational Sciences, Sichuan Normal University, Chengdu, 610068, China

    Botao Fu  (付波涛)

Authors
  1. Liping Sun  (孙丽萍)
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  2. Botao Fu  (付波涛)
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  3. Jing Chang  (常景)
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Contributions

Author contributions Chang J conceived this research. Sun L performed the investigation and the corresponding calculations. Fu B and Chang J contributed to the theoretical analysis. All authors contributed to the general discussion.

Corresponding author

Correspondence to Jing Chang  (常景).

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Conflict of interest The authors declare that they have no conflict of interest.

Additional information

Supplementary information Experimental details and supporting data are available in the online version of the paper.

Liping Sun is a master student at the School of Physics and Electronic Engineering, Sichuan Normal University. Her research interests mainly focus on the DFT calculations regarding superhard and magnetic materials and their applications.

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Sun, L., Fu, B. & Chang, J. First-principles predictions of new superhard magnetic clathrate material β-C3N2 through atom embeddedness. Sci. China Mater. (2024). https://doi.org/10.1007/s40843-024-2916-5

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