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Sulfur-vacancy-tunable interlayer magnetic coupling in centimeter-scale MoS2 bilayer

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Abstract

Endowing bilayer transition-metal dichalcogenides (TMDs) with tunable magnetism is significant to investigate the coupling of multiple electron degrees of freedom (DOFs). However, effectively inducing and tuning the magnetic interaction of bilayer TMDs are still challenges. Herein, we report a strategy to tune the interlayer exchange interaction of centimeter-scale MoS2 bilayer with substitutional doping of Co ion, by introducing sulfur vacancy (VS) to modulate the interlayer electronic coupling. This strategy could transform the interlayer exchange interaction from antiferromagnetism (AFM) to ferromagnetism (FM), as revealed by the magnetic measurements. Experimental characterizations and theoretical calculations indicate that the enhanced magnetization is mainly because the hybridization of Co 3d band and VS-induced impurity band alters the forms of interlayer orbital hybridizations between the partial Co atoms in upper and lower layers, and also enhances the intralayer FM. Our work paves the way for tuning the interlayer exchange interaction with defects and could be extended to other two-dimensional (2D) magnetic materials.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 11975234, 11775225, 12075243, 12005227, 51790491, U2032150 and U1732148), the Users with Excellence Program of Hefei Science Center CAS (Nos. 2019HSC-UE002, 2020HSC-UE002, 2020HSC-CIP013 and 2021HSC-UE002), the Postdoctoral Science Foundation of China (Nos. 2020M682041, 2020TQ0316 and 2019M662202), the National Key Research and Development Program of China (No. 2019YFA0307900), and partially carried out at the USTC Center for Micro and Nanoscale Research and Fabrication. The authors would like to thank SSRF, BSRF and NSRL for the synchrotron beamtime.

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  1. Hengli Duan and Guinan Li contributed equally to this work.

Authors and Affiliations

  1. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, China

    Hengli Duan, Guinan Li, Hao Tan, Chao Wang, Qian Li, Zeming Qi & Wensheng Yan

  2. Hefei National Laboratory for Physical Sciences at the Microscale, Department of Physics, and CAS Key Laboratory of Strongly-coupled Quantum Matter Physics, University of Science and Technology of China, Hefei, 230026, China

    Chuanchuan Liu, Yuewei Yin & Xiaoguang Li

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  1. Hengli Duan
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Correspondence to Chao Wang, Zeming Qi or Wensheng Yan.

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Duan, H., Li, G., Tan, H. et al. Sulfur-vacancy-tunable interlayer magnetic coupling in centimeter-scale MoS2 bilayer. Nano Res. 15, 881–888 (2022). https://doi.org/10.1007/s12274-021-3569-7

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