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Twist engineering of the two-dimensional magnetism in double bilayer chromium triiodide homostructures

Nature Physics volume 18, pages 30–36 (2022)Cite this article

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Abstract

Twist engineering—the alignment of two-dimensional (2D) crystalline layers with a specific orientation—has led to tremendous success in controlling the charge degree of freedom, particularly in producing correlated and topological electronic phases in moiré crystals1,2. However, although pioneering theoretical efforts have predicted that non-trivial magnetism3,4,5 and magnons6,7 can be made by twisting 2D magnets, the experimental realization of engineering the spin degree of freedom by twisting remains elusive. Here we fabricate twisted double bilayers of a 2D magnet, namely, chromium triiodide (CrI3), and demonstrate the successful twist engineering of 2D magnetism in them. We identify signatures of a new magnetic ground state that is distinct from those in natural two-layer (2L) and four-layer (4L) CrI3. We show that for a very small twist angle, this emergent magnetism can be well approximated by a weighted linear superposition of those of 2L and 4L CrI3, whereas for a large twist angle, it mostly resembles that of isolated 2L CrI3. However, at an intermediate twist angle, there is a finite net magnetization that cannot be simply inferred from any homogeneous stacking configuration, but emerges because spin frustrations are introduced by competition between ferromagnetic and antiferromagnetic exchange coupling within individual moiré supercells.

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Fig. 1: Sample fabrication, TEM and magneto-Raman characterizations of tDB CrI3.
Fig. 2: Twist-angle dependence of the magneto-Raman spectra of tDB CrI3.
Fig. 3: Magnetic-field dependence of the magneto-Raman spectra of tDB CrI3 at selected twist angles.
Fig. 4: Raman circular dichroism and magnetic circular dichroism for 1.1° tDB CrI3.

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Source data are provided with this paper. All other data that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request.

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Acknowledgements

L.Z. acknowledges support by NSF CAREER grant no. DMR-174774 and AFOSR YIP grant no. FA9550-21-1-0065. R. He acknowledges support by NSF CAREER grant no. DMR-1760668. K.S. acknowledges support by NSF grant no. NSF-EFMA-1741618. R. Hovden acknowledges support from the W. M. Keck Foundation. This work made use of facilities at the Michigan Center for Materials Characterization. H.L. acknowledges support by the National Key R&D Program of China (grant nos. 2018YFE0202600 and 2016YFA0300504), the National Natural Science Foundation of China (nos. 11774423 and 11822412), the Beijing Natural Science Foundation (grant no. Z200005), and the Fundamental Research Funds for the Central Universities and Research Funds of Renmin University of China (RUC) (grant nos. 18XNLG14, 19XNLG17 and 20XNH062).

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Author notes

  1. These authors contributed equally: Hongchao Xie, Xiangpeng Luo, Gaihua Ye.

Authors and Affiliations

  1. Department of Physics, University of Michigan, Ann Arbor, MI, USA

    Hongchao Xie, Xiangpeng Luo, Kai Sun & Liuyan Zhao

  2. Department of Electrical and Computer Engineering, Texas Tech University, Lubbock, TX, USA

    Gaihua Ye, Zhipeng Ye & Rui He

  3. Department of Mechanical Engineering, Texas Tech University, Lubbock, TX, USA

    Haiwen Ge

  4. Department of Materials Science and Engineering, University of Michigan, Ann Arbor, MI, USA

    Suk Hyun Sung & Robert Hovden

  5. Department of Mechanical Engineering, University of Michigan, Ann Arbor, MI, USA

    Emily Rennich

  6. Department of Physics and Beijing Key Laboratory of Opto-electronic Functional Materials & Micro-Nano Devices, Renmin University of China, Beijing, China

    Shaohua Yan, Yang Fu, Shangjie Tian & Hechang Lei

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  1. Hongchao Xie
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Contributions

L.Z., H.X. and X.L. conceived the idea and initiated this project. H.X. fabricated the 4L and 2L CrI3 and tDB CrI3 homostructures. H.X., X.L., G.Y., Z.Y. and H.G. carried out the Raman experiments under the supervision of L.Z. and R. He. S.H.S., E.R. and R. Hovden performed the TEM characterizations. S.Y., Y.F., S.T. and H.L. grew the van der Waals CrI3 bulk single crystals. K.S. performed the theoretical analysis. H.X., X.L., R. He and L.Z. analysed the data and wrote the manuscript. All the authors participated in the discussion of the results.

Corresponding authors

Correspondence to Rui He or Liuyan Zhao.

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Xie, H., Luo, X., Ye, G. et al. Twist engineering of the two-dimensional magnetism in double bilayer chromium triiodide homostructures. Nat. Phys. 18, 30–36 (2022). https://doi.org/10.1038/s41567-021-01408-8

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