Abstract
Alloying different metal elements to form two-dimensional (2D) materials (metallenes) holds great significance for both fundamental research and practical applications in nanoelectronics, but few of them are semiconductors with intrinsic band gaps. Here, inspired by bond characteristics in ionic crystals, we report a family of lattice dynamically stable 2D alkali auride bimetallene semiconductors with ionic bonding between alkali and gold atoms by extensive structure search and bonding analysis via high-throughput first-principles calculations over 2500 bimetallenes. Among them, 32 2D alkali auride bimetallenes are semiconductors with large band gaps ranging from 0.97 to 5.20 eV due to the large difference in electronegativity between alkali and gold atoms. Exceptionally, 2D LiAu bimetallene is metallic due to the reduced electronegativity difference between Li and Au atoms. Born-Oppenheimer molecular dynamic simulations imply that 19 alkali auride bimetallenes are structurally stable at room temperature for practical applications. This study provides guidance for designing bimetallene semiconductors and deepens the understanding of the correlation between the bonding behavior and electronic properties of 2D metal alloys.
摘要
将不同金属元素通过合金化形成二维材料(金属烯)对基础研究 和纳米电子器件的实际应用具有重要意义, 但目前鲜有金属烯材料是 具有本征带隙的半导体. 受离子晶体成键特征的启发, 通过结构搜索、 成键分析和高通量第一性原理计算, 本文从2500多个双金属烯中筛选 出一系列具有晶格动力学稳定和碱金属-金离子键的二维碱金属金化 物双金属烯半导体. 由于碱金属和金之间的大电负性差, 其中32个碱金 属金化物双金属烯是带隙范围为0.97~5.20 eV的半导体材料, 而锂金双 金属烯由于电负性差减小呈现出金属性. Bohn-Oppenheimer分子动力 学模拟表明19个双金属烯在室温下结构稳定有利于实际应用. 这项研 究为设计双金属烯半导体提供了指导, 并揭示了二维金属合金中成键 行为和电子结构性质间的关联.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (22073087, 12147105 and 22321001), the National Natural Science Foundation for Distinguished Young Scholars (22225301), Anhui Provincial Natural Science Foundation (2308085QB51), the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB0450101), and the Fundamental Research Funds for the Central Universities (20720220007). We thank the support from the Super Computer Centre of University of Science and Technology of China and Supercomputing Center of Chinese Academy of Sciences.
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Author contributions Wu X conceived the project. Zhang K carried out theoretical calculations. All authors wrote the paper and contributed to the general discussion.
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Kai Zhang is a postdoctor at Hefei National Research Center for Physical Sciences at the Microscale. He received his PhD degree from the University of Science and Technology of China in 2021. His research interest mainly focuses on the theoretical design of low-dimensional functional materials.
Xiaojun Wu is a full professor at the Department of Materials Sciences and Engineering, University of Science and Technology of China. He received his BSc degree and PhD degree from the Department of Physical Chemistry, University of Science and Technology of China. His research interest includes the development of materials design method, the design and computational simulation of spintronics materials, (photo)catalytic materials for energy, and other low-dimensional functional materials.
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Zhang, K., Lv, H., Wu, X. et al. Two-dimensional alkali auride bimetallene semiconductors. Sci. China Mater. 67, 1209–1216 (2024). https://doi.org/10.1007/s40843-023-2818-6
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DOI: https://doi.org/10.1007/s40843-023-2818-6