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Van der Waals epitaxial growth of air-stable CrSe2 nanosheets with thickness-tunable magnetic order

Nature Materials volume 20, pages 818–825 (2021)Cite this article

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Abstract

The discovery of intrinsic ferromagnetism in ultrathin two-dimensional van der Waals crystals opens up exciting prospects for exploring magnetism in the ultimate two-dimensional limit. Here, we show that environmentally stable CrSe2 nanosheets can be readily grown on a dangling-bond-free WSe2 substrate with systematically tunable thickness down to the monolayer limit. These CrSe2/WSe2 heterostructures display high-quality van der Waals interfaces with well-resolved moiré superlattices and ferromagnetic behaviour. We find no apparent change in surface roughness or magnetic properties after months of exposure in air. Our calculations suggest that charge transfer from the WSe2 substrate and interlayer coupling within CrSe2 play a critical role in the magnetic order in few-layer CrSe2 nanosheets. The highly controllable growth of environmentally stable CrSe2 nanosheets with tunable thickness defines a robust two-dimensional magnet for fundamental studies and potential applications in magnetoelectronic and spintronic devices.

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Fig. 1: Thickness-tunable synthesis of CrSe2 nanosheets on WSe2 substrates.
Fig. 2: STEM characterization of CrSe2 nanosheets.
Fig. 3: Thickness-dependent magnetic properties.
Fig. 4: Magnetotransport measurements of the CrSe2 nanosheets with different thickness.
Fig. 5: Theoretical calculations of the magnetism in CrSe2.

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The data that support the findings of this study are available from the corresponding author on reasonable request.

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Acknowledgements

Xidong Duan acknowledges support by the National Key Research and Development Program of China (no. 2018YFA0703700), the National Natural Science Foundation of China (nos. 51991343, 51991340, 61804050 and 51872086), the Fundamental Research Funds of the Central Universities (no. 531107051078), the Double First-Class Initiative of Hunan University (no. 531109100004), and the Hunan Key Laboratory of Two-Dimensional Materials (no. 2018TP1010). W.J. acknowledges support by the National Key Research and Development Program of China (no. 2018YFE0202700), the National Natural Science Foundation of China (nos. 11622437, 61674171 and 11974422), and the Strategic Priority Research Program of the Chinese Academy of Sciences (no. XDB30000000). B.L. acknowledges support by the National Natural Science Foundation of China (no. 61804050), and the Fundamental Research Funds of the Central Universities (no. 531107051055). Calculations were performed at the Physics Lab of High-Performance Computing of Renmin University of China and the Shanghai Supercomputer Center. The work done at the University of Washington is mainly supported by the Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division (DE-SC0018171).

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Author notes

  1. These authors contributed equally: Bo Li, Zhong Wan, Cong Wang, Peng Chen.

Authors and Affiliations

  1. Hunan Key Laboratory of Two-Dimensional Materials, Key Laboratory for Micro/Nano-Optoelectronic Devices, Ministry of Education, State Key Laboratory for Chemo/Biosensing and Chemometrics, Department of Applied Physics, School of Physics and Electronics, Hunan University, Changsha, China

    Bo Li, Yuan Liu & Lei Liao

  2. Hunan Key Laboratory of Two-Dimensional Materials and State Key Laboratory for Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, China

    Bo Li, Peng Chen, Jia Li, Zhengwei Zhang, Bei Zhao, Huifang Ma, Ruixia Wu & Xidong Duan

  3. Department of Chemistry and Biochemistry, University of California, Los Angeles, CA, USA

    Zhong Wan, Peng Chen, Qi Qian & Xiangfeng Duan

  4. Department of Physics and Beijing Key Laboratory of Optoelectronic Functional Materials & Micro-Nano Devices, Renmin University of China, Beijing, China

    Cong Wang & Wei Ji

  5. Department of Physics, University of Washington, Seattle, WA, USA

    Bevin Huang & Xiaodong Xu

  6. State Key Laboratory for Artificial Microstructure & Mesoscopic Physics, School of Physics, Peking University, Beijing, China

    Xing Cheng & Yu Ye

  7. School of Electronic and Information Engineering, Chongqing Three Gorges University, Chongqing, China

    Guangzhuang Sun

  8. State Key Laboratory of Superlattices and Microstructures, Institute of Semiconductors, Chinese Academy of Sciences, Beijing, China

    Zhongming Wei

  9. Department of Materials Science and Engineering, University of California, Los Angeles, CA, USA

    Yu Huang

  10. California NanoSystems Institute, University of California, Los Angeles, CA, USA

    Yu Huang & Xiangfeng Duan

Authors
  1. Bo Li
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  2. Zhong Wan
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Contributions

B.L. synthesized the samples. B.L., J.L., Z.Z., G.S., B.Z., H.M., R.W., Z. Wei, Y.L. and L.L. performed material characterizations. B.H., X.C., Y.Y. and X.X. contributed to RMCD measurements and analyses. Z. Wan, Q.Q., P.C. and B.L. fabricated and measured the Hall bar devices. C.W. and W.J. conducted theoretical calculations. B.L., Z. Wan, C.W., Y.H., W.J., Xidong Duan and Xiangfeng Duan wrote the manuscript. All authors discussed the results and commented on the manuscript.

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Correspondence to Xidong Duan, Wei Ji or Xiangfeng Duan.

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Supplementary Figs. 1–16, Tables 1–4 and refs. 1–9.

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Li, B., Wan, Z., Wang, C. et al. Van der Waals epitaxial growth of air-stable CrSe2 nanosheets with thickness-tunable magnetic order. Nat. Mater. 20, 818–825 (2021). https://doi.org/10.1038/s41563-021-00927-2

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