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Evidence of non-collinear spin texture in magnetic moiré superlattices

Nature Physics volume 19, pages 1150–1155 (2023)Cite this article

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Abstract

Moiré magnetism is emerging as a platform to design and control exotic magnetic phases in twisted magnetic two-dimensional crystals. Non-collinear spin texture emerging from twisted two-dimensional magnets with collinear spins is one of the most profound consequences of moiré magnetism and forms the basis for realizing non-trivial magnetic orders and excitations. However, no direct experimental observations of non-collinear spins in moiré magnets have been made, despite recent theoretical and experimental efforts. Here, we report evidence of non-collinear spin texture in two-dimensional twisted double bilayer CrI3. We distinguish the non-collinear spins with a gradual spin flop process from the collinear spins with sudden spin flip transitions and identify a net magnetization emerging from the collinear spins. We also demonstrate that both non-collinear spins and net magnetization are present at twist angles from 0.5° to 5° but are most prominent for 1.1°. We resolve a critical temperature of 25 K for the onset of the net magnetization and the softening of the non-collinear spins in the 1.1° samples. This is substantially lower than the Néel temperature of 45 K for natural few layers. Our results provide a platform to explore non-trivial magnetism with non-collinear spins.

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Fig. 1: Calculations of the magnetic ground states of tDB CrI3.
Fig. 2: SAED and DF-TEM of high-quality moiré superlattice in tDB CrI3.
Fig. 3: Magnetic field dependent MCD data, model fits and spin configurations for 1.1° tDB CrI3.
Fig. 4: Twist angle dependence of MCD data of tDB CrI3.
Fig. 5: Temperature dependence of the MCD and polarized Raman scattering data of 1.1° tDB CrI3.

Data availability

Raw data for SAED and DF-TEM data are images shown in the main text and Supplementary Information. Raw data for MCD and Raman results are provided as Source data provided with this paper.

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Acknowledgements

We thank N. Agarwal for helpful discussions and assistance in SAED and DF-TEM measurements. L.Z. acknowledges support from NSF career grant no. DMR-174774, AFOSR YIP grant no. FA9550-21-1-0065 and the Alfred P. Sloan Foundation. R. He acknowledges support from NSF grant no. DMR-2104036 and NSF career grant no. DMR-1760668. R. Hovden acknowledges support from ARO grant no. W911NF-22-1-0056. S.H.S. acknowledges support from the W.M. Keck Foundation. K.S. acknowledges support from NSF grant no. NSF-EFMA-1741618. H.L. acknowledges support from the National Key R&D Program of China (grant nos. 2018YFE0202600 and 2016YFA0300504), 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 (grant nos. 18XNLG14, 19XNLG17 and 20XNH062).

Author information

Author notes

  1. These authors contributed equally: Hongchao Xie, Xiangpeng Luo, Zhipeng Ye, Zeliang Sun.

Authors and Affiliations

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

    Hongchao Xie, Xiangpeng Luo, Zeliang Sun, Kai Sun & Liuyan Zhao

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

    Zhipeng Ye, Gaihua Ye & Rui He

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

    Suk Hyun Sung & Robert Hovden

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

    Haiwen Ge

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

    Shaohua Yan, Yang Fu, Shangjie Tian & Hechang Lei

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Contributions

L.Z., H.X. and X.L. conceived the idea and initiated this project. H.X. and Z.S. fabricated the 4L, 2L and tDB CrI3 samples. H.X., X.L., Z.Y., G.Y. and H.G. built the MCD setup and carried out the MCD measurements under the supervision of L.Z. and R. He. S.H.S. and R. Hovden performed the electron diffraction and TEM measurements. S.Y., Y.F., S.T. and H.L. grew the CrI3 bulk single crystals. X.L. and K.S. performed the theoretical computation and analysis. X.L. and L.Z. analysed the data, and X.L., R. He and L.Z. wrote the manuscript. All authors participated in the discussion of the results.

Corresponding authors

Correspondence to Rui He or Liuyan Zhao.

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Nature Physics thanks Bevin Huang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Sections 1–5.

Source data

Source Data Fig. 3

Raw data for MCD spectra and their fits.

Source Data Fig. 4

Raw data for MCD spectra and their fitted key parameters.

Source Data Fig. 5

Raw data for MCD and Raman spectra and their fits.

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Xie, H., Luo, X., Ye, Z. et al. Evidence of non-collinear spin texture in magnetic moiré superlattices. Nat. Phys. 19, 1150–1155 (2023). https://doi.org/10.1038/s41567-023-02061-z

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