Abstract

Controlling magnetism via electric fields addresses fundamental questions of magnetic phenomena and phase transitions1,2,3, and enables the development of electrically coupled spintronic devices, such as voltage-controlled magnetic memories with low operation energy4,5,6. Previous studies on dilute magnetic semiconductors such as (Ga,Mn)As and (In,Mn)Sb have demonstrated large modulations of the Curie temperatures and coercive fields by altering the magnetic anisotropy and exchange interaction2,4,7,8,9. Owing to their unique magnetic properties10,11,12,13,14, the recently reported two-dimensional magnets provide a new system for studying these features15,16,17,18,19. For instance, a bilayer of chromium triiodide (CrI3) behaves as a layered antiferromagnet with a magnetic field-driven metamagnetic transition15,16. Here, we demonstrate electrostatic gate control of magnetism in CrI3 bilayers, probed by magneto-optical Kerr effect (MOKE) microscopy. At fixed magnetic fields near the metamagnetic transition, we realize voltage-controlled switching between antiferromagnetic and ferromagnetic states. At zero magnetic field, we demonstrate a time-reversal pair of layered antiferromagnetic states that exhibit spin-layer locking, leading to a linear dependence of their MOKE signals on gate voltage with opposite slopes. Our results allow for the exploration of new magnetoelectric phenomena and van der Waals spintronics based on 2D materials.

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References

  1. 1.

    Chiba, D. et al. Electrical control of the ferromagnetic phase transition in cobalt at room temperature. Nat. Mater. 10, 853–856 (2011).

  2. 2.

    Chiba, D. et al. Magnetization vector manipulation by electric fields. Nature 455, 515–518 (2008).

  3. 3.

    Eerenstein, W., Mathur, N. D. & Scott, J. F. Multiferroic and magnetoelectric materials. Nature 442, 759–765 (2006).

  4. 4.

    Matsukura, F., Tokura, Y. & Ohno, H. Control of magnetism by electric fields. Nat. Nanotech. 10, 209–220 (2015).

  5. 5.

    Prinz, G. A. Magnetoelectronics. Science 282, 1660–1663 (1998).

  6. 6.

    Chu, Y. H. et al. Electric-field control of local ferromagnetism using a magnetoelectric multiferroic. Nat. Mater. 7, 478–482 (2008).

  7. 7.

    Ohno, H. et al. Electric-field control of ferromagnetism. Nature 408, 944–947 (2000).

  8. 8.

    Dietl, T., Ohno, H., Matsukura, F., Cibert, J. & Ferrand, D. Zener model description of ferromagnetism in zinc-blende magnetic semiconductors. Science 287, 1019–1022 (2000).

  9. 9.

    MacDonald, A. H., Schiffer, P. & Samarth, N. Ferromagnetic semiconductors: moving beyond (Ga,Mn)As. Nat. Mater. 4, 195–202 (2005).

  10. 10.

    Gong, C. et al. Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals. Nature 546, 265–269 (2017).

  11. 11.

    Tian, Y., Gray, M. J., Ji, H., Cava, R. J. & Burch, K. S. Magneto-elastic coupling in a potential ferromagnetic 2D atomic crystal. 2D Mater. 3, 25035 (2016).

  12. 12.

    Zhou, B. et al. Possible structural transformation and enhanced magnetic fluctuations in exfoliated α-RuCl3. J. Phys. Chem. Solids (in the press).

  13. 13.

    O’Hara, D. J. et al. Room temperature intrinsic ferromagnetism in epitaxial manganese selenide films in the monolayer limit. Preprint at https://arxiv.org/abs/1802.08152 (2018).

  14. 14.

    Wang, X. et al. Raman spectroscopy of atomically thin two-dimensional magnetic iron phosphorus trisulfide (FePS3) crystals. 2D Mater. 3, 31009 (2016).

  15. 15.

    Huang, B. et al. Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit. Nature 546, 270–273 (2017).

  16. 16.

    Seyler, K. L. et al. Ligand-field helical luminescence in a 2D ferromagnetic insulator. Nat. Phys. 14, 277–281 (2018).

  17. 17.

    Lee, J. U. et al. Ising-type magnetic ordering in atomically thin FePS3. Nano Lett. 16, 7433–7438 (2016).

  18. 18.

    Xing, W. et al. Electric field effect in multilayer Cr2Ge2Te6: a ferromagnetic two-dimensional material. 2D Mater. 4, 24009 (2017).

  19. 19.

    McGuire, M. A., Dixit, H., Cooper, V. R. & Sales, B. C. Coupling of crystal structure and magnetism in the layered, ferromagnetic insulator CrI3. Chem. Mater. 27, 612–620 (2015).

  20. 20.

    Song, T. et al. Giant tunneling magnetoresistance in spin-filter van der Waals heterostructures. Preprint at https://arxiv.org/abs/1801.08679 (2018).

  21. 21.

    Klein, D. R. et al. Probing magnetism in 2D van der Waals crystalline insulators via electron tunneling. Preprint at https://arxiv.org/abs/1801.10075 (2018).

  22. 22.

    Wang, L. et al. One-dimensional electrical contact to a two-dimensional material. Science 342, 614–617 (2013).

  23. 23.

    Sato, K. Measurement of magneto-optical Kerr effect using piezo-birefringent modulator. Jpn J. Appl. Phys. 20, 2403–2409 (1981).

  24. 24.

    Zhang, Y. et al. Direct observation of a widely tunable bandgap in bilayer graphene. Nature 459, 820–823 (2009).

  25. 25.

    Taychatanapat, T., Watanabe, K., Taniguchi, T. & Jarillo-Herrero, P. Quantum Hall effect and Landau-level crossing of Dirac fermions in trilayer graphene. Nat. Phys. 7, 621–625 (2011).

  26. 26.

    Dean, C. R. et al. Boron nitride substrates for high-quality graphene electronics. Nat. Nanotech. 5, 722–726 (2010).

  27. 27.

    Wang, Z. et al. Very large tunneling magnetoresistance in layered magnetic semiconductor CrI3. Preprint at https://arxiv.org/abs/1801.08188 (2018).

  28. 28.

    Weisheit, M. et al. Electric field-induced modification of magnetism in thin-film ferromagnets. Science 315, 349–351 (2007).

  29. 29.

    Duan, C. G. et al. Surface magnetoelectric effect in ferromagnetic metal films. Phys. Rev. Lett. 101, 137201 (2008).

  30. 30.

    Nakamura, K. et al. Giant modification of the magnetocrystalline anisotropy in transition-metal monolayers by an external electric field. Phys. Rev. Lett. 102, 187201 (2009).

  31. 31.

    Schmehl, A. et al. Epitaxial integration of the highly spin-polarized ferromagnetic semiconductor EuO with silicon and GaN. Nat. Mater. 6, 882–887 (2007).

  32. 32.

    Mairoser, T. et al. Is there an intrinsic limit to the charge-carrier-induced increase of the Curie temperature of EuO? Phys. Rev. Lett. 105, 257206 (2010).

  33. 33.

    Sivadas, N., Okamoto, S. & Xiao, D. Gate-controllable magneto-optic Kerr effect in layered collinear antiferromagnets. Phys. Rev. Lett. 117, 267203 (2016).

  34. 34.

    Gong, Z. et al. Magnetoelectric effects and valley-controlled spin quantum gates in transition metal dichalcogenide bilayers. Nat. Commun. 4, 2053 (2013).

  35. 35.

    Jones, A. M. et al. Spin-layer locking effects in optical orientation of exciton spin in bilayer WSe2. Nat. Phys. 10, 130–134 (2014).

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Acknowledgements

Work at the University of Washington was mainly supported by the Department of Energy, Basic Energy Sciences (DOE BES), Materials Sciences and Engineering Division (DE-SC0012509) and a University of Washington Innovation Award. Work at MIT was supported by the Center for Integrated Quantum Materials under National Science Foundation (NSF) grant DMR-1231319 as well as the Gordon and Betty Moore Foundation’s EPiQS Initiative through grant GBMF4541 to P.J.-H. D.R.K. was funded in part by a QuantEmX grant from ICAM and the Gordon and Betty Moore Foundation through grant GBMF5305 and from the NSF Graduate Research Fellowship Program (GRFP) under grant 1122374. Device fabrication has been partly supported by the Center for Excitonics, an Energy Frontier Research Center funded by the DOE BES under award DE-SC0001088. D.H.C.’s contribution was supported by DE-SC0002197. Work at CMU was also supported by DOE BES DE-SC0012509. W.Y. was supported by the Croucher Foundation (Croucher Innovation Award) and the HKU ORA. Work at ORNL (M.A.M.) was supported by the DOE BES Materials Sciences and Engineering Division. D.X. acknowledges the support of a Cottrell Scholar Award. X.X. acknowledges the support from the State of Washington funded Clean Energy Institute and from the Boeing Distinguished Professorship in Physics.

Author information

Author notes

  1. These authors contributed equally: Bevin Huang, Genevieve Clark and Dahlia R. Klein.

Affiliations

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

    • Bevin Huang
    • , Kyle L. Seyler
    • , Nathan Wilson
    • , David H. Cobden
    •  & Xiaodong Xu
  2. Department of Materials Science and Engineering, University of Washington, Seattle, WA, USA

    • Genevieve Clark
    •  & Xiaodong Xu
  3. Department of Physics, Massachusetts Institute of Technology, Cambridge, MA, USA

    • Dahlia R. Klein
    • , David MacNeill
    •  & Pablo Jarillo-Herrero
  4. Instituto de Ciencia Molecular, Universidad de Valencia, Paterna, Spain

    • Efrén Navarro-Moratalla
  5. Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN, USA

    • Michael A. McGuire
  6. Department of Physics, Carnegie Mellon University, Pittsburgh, PA, USA

    • Di Xiao
  7. Department of Physics and Center of Theoretical and Computational Physics, University of Hong Kong, Hong Kong, China

    • Wang Yao

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Contributions

X.X. and P.J.-H. supervised the project. E.N.-M. and M.A.M. synthesized and characterized the bulk CrI3 crystals. D.R.K. fabricated the devices, assisted by D.M., G.C. and B.H. G.C. built the set-up with help from B.H. and N.W. B.H. and G.C. performed the MOKE measurements, assisted by K.L.S. and D.R.K. W.Y. and D.X. provided the theoretical support. All authors contributed to writing the paper and discussed the results.

Competing interests

The authors declare no competing interests.

Corresponding authors

Correspondence to Pablo Jarillo-Herrero or Xiaodong Xu.

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DOI

https://doi.org/10.1038/s41565-018-0121-3