Switching 2D magnetic states via pressure tuning of layer stacking

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Abstract

The physical properties of two-dimensional van der Waals crystals can be sensitive to interlayer coupling. For two-dimensional magnets1,2,3, theory suggests that interlayer exchange coupling is strongly dependent on layer separation while the stacking arrangement can even change the sign of the interlayer magnetic exchange, thus drastically modifying the ground state4,5,6,7,8,9,10. Here, we demonstrate pressure tuning of magnetic order in the two-dimensional magnet CrI3. We probe the magnetic states using tunnelling8,11,12,13 and scanning magnetic circular dichroism microscopy measurements2. We find that interlayer magnetic coupling can be more than doubled by hydrostatic pressure. In bilayer CrI3, pressure induces a transition from layered antiferromagnetic to ferromagnetic phase. In trilayer CrI3, pressure can create coexisting domains of three phases, one ferromagnetic and two antiferromagnetic. The observed changes in magnetic order can be explained by changes in the stacking arrangement. Such coupling between stacking order and magnetism provides ample opportunities for designer magnetic phases and functionalities.

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Fig. 1: Stacking-order determined 2D magnetism and tunnelling measurements of bilayer CrI3 under pressure.
Fig. 2: Effect of pressure on the magnetic properties of bilayer CrI3.
Fig. 3: New pressure-induced magnetic states in trilayer CrI3.
Fig. 4: Magnetic and layer stacking phase map of a trilayer CrI3 flake.

Data availability

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

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Acknowledgements

We thank S. Wu and W. Wu for the insightful discussion. This work was mainly supported by the Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division, Pro-QM EFRC (grant no. DE-SC0019443). Device fabrication and quantum tunnelling measurement were partially supported by NSF MRSEC (grant no. 1719797), and magnetic circular dichroism measurement was partially supported by the Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division (grant no. E-SC0018171). The material synthesis performed at the University of Washington was partially supported by the Gordon and Betty Moore Foundation’s EPiQS Initiative (grant no. GBMF6759 to J.-H.C.). M.A.M. was supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by MEXT, Japan, A3 Foresight by JSPS and CREST (grant no. JPMJCR15F3) and JST. A portion of this work was performed at the National High Magnetic Field Laboratory, which is supported by National Science Foundation Cooperative Agreement (no. DMR-1644779) and the State of Florida. X.X. and J.-H.C. acknowledge support from the State of Washington-funded Clean Energy Institute. X.X. also acknowledges support from the Boeing Distinguished Professorship in Physics.

Author information

X.X., T.S., M.Y., C.R.D. and D.X. conceived the experiment. T.S. and Z.F. fabricated and characterized the devices, assisted by M.Y. and B.S. T.S., Z.F. and M.Y. performed the high-pressure measurements, assisted by D.G. T.S. performed magnetic circular dichroism and Raman measurements. K.H. and Q.Z. assisted in Raman measurement. T.S., Z.F., X.X., D.X., T.C. and D.H.C. analysed and interpreted the results. M.M., Z.L., Q.J. and J.-H.C. independently synthesized and characterized the bulk CrI3 crystals. T.S., X.X., D.H.C., D.X. and Z.F. wrote the paper with input from all authors. All authors discussed the results.

Correspondence to Xiaodong Xu.

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Song, T., Fei, Z., Yankowitz, M. et al. Switching 2D magnetic states via pressure tuning of layer stacking. Nat. Mater. (2019) doi:10.1038/s41563-019-0505-2

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