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Two-dimensional bipolar magnetic semiconductors with high Curie-temperature and electrically controllable spin polarization realized in exfoliated Cr(pyrazine)2 monolayers

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Abstract

Exploring two-dimensional (2D) magnetic semiconductors with room-temperature magnetic ordering and electrically controllable spin-polarization is a highly desirable but challenging task for nano-spintronics. Here, through first-principles calculations, we propose to realize such a material by exfoliating the recently synthesized organometallic layered crystal Li0.7[Cr(pyz)2]Cl0.7·0.25(THF) (pyz=pyrazine, THF=tetrahydrofuran). The feasibility of exfoliation is confirmed by the rather low exfoliation energy of 0.27 J m−2, even smaller than that of graphite. In exfoliated Cr(pyz)2 monolayers, each pyrazine ring grabs one electron from the Cr atom to become a radical anion, and then a strong d-p direct-exchange magnetic interaction emerges between Cr cations and pyrazine radicals, resulting in room-temperature ferrimagnetism with a Curie temperature of 342 K. Moreover, the Cr(pyz)2 monolayer is revealed to be an intrinsic bipolar magnetic semiconductor where electrical doping can induce half-metallic conduction with controllable spin-polarization direction.

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Acknowledgements

This work is supported by the National Natural Science Foundation of China (21688102), by the National Key Research & Development Program of China (2016YFA0200604), by Anhui Initiative in Quantum Information Technologies (AHY090400), by the Youth Innovation Promotion Association CAS (2019441), and by USTC Research Funds of the Double First-Class Initiative (YD2060002011). The computational resources are provided by the Supercomputing Center of University of Science and Technology of China, Supercomputing Center of Chinese Academy of Sciences, and Tianjin and Shanghai Supercomputer Centers.

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Hefei National Laboratory of Physical Science at the Microscale, Department of Chemical Physics, Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, 230026, China

    Xiangyang Li, Haifeng Lv, Xiaofeng Liu, Xiaojun Wu, Xingxing Li & Jinlong Yang

  2. Department of Chemistry, Key Laboratory of Functional Inorganic Materials of Anhui Province, Anhui University, Hefei, 230601, China

    Tong Jin

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  1. Xiangyang Li
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  2. Haifeng Lv
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  3. Xiaofeng Liu
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  4. Tong Jin
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  5. Xiaojun Wu
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  6. Xingxing Li
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  7. Jinlong Yang
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Correspondence to Xiaojun Wu, Xingxing Li or Jinlong Yang.

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11426_2021_1160_MOESM1_ESM.docx

Two-Dimensional Bipolar Magnetic Semiconductor with High Curie Temperature and Electrically Controllable Spin Polarization Realized in Exfoliated Cr(pyrazine)2 Monolayer

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Li, X., Lv, H., Liu, X. et al. Two-dimensional bipolar magnetic semiconductors with high Curie-temperature and electrically controllable spin polarization realized in exfoliated Cr(pyrazine)2 monolayers. Sci. China Chem. 64, 2212–2217 (2021). https://doi.org/10.1007/s11426-021-1160-7

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  • DOI: https://doi.org/10.1007/s11426-021-1160-7

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