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Pressure-controlled interlayer magnetism in atomically thin CrI3

Abstract

Stacking order can influence the physical properties of two-dimensional van der Waals materials1,2. Here we applied hydrostatic pressure up to 2 GPa to modify the stacking order in the van der Waals magnetic insulator CrI3. We observed an irreversible interlayer antiferromagnetic-to-ferromagnetic transition in atomically thin CrI3 by magnetic circular dichroism and electron tunnelling measurements. The effect was accompanied by a monoclinic-to-rhombohedral stacking-order change characterized by polarized Raman spectroscopy. Before the structural change, the interlayer antiferromagnetic coupling energy can be tuned up by nearly 100% with pressure. Our experiment reveals the interlayer ferromagnetic ground state, which is established in bulk CrI3 but not observed in native exfoliated thin films. The observed correlation between the magnetic ground state and the stacking order is in good agreement with first principles calculations3,4,5,6,7,8 and suggests a route towards nanoscale magnetic textures by moiré engineering3,9.

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Fig. 1: Crystal structure of CrI3.
Fig. 2: Pressure-induced interlayer AF–FM transition in atomically thin CrI3.
Fig. 3: Pressure-induced structural phase transition in atomically thin CrI3.
Fig. 4: Spin-filtering effect in atomically thin CrI3 as a function of pressure.

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The data supporting the plots within this paper and other findings of this study are available from the corresponding authors upon request.

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Acknowledgements

We thank D. Graf and K. Huang for fruitful discussions on high-pressure cell operation, and G. H. Olsen and Z. He on density functional theory calculations. This work was supported by the US Army Research Office (ARO) under award W911NF-17-1-0605 (high-pressure cell set-up), the Office of Naval Research (ONR) under award N00014-18-1-2368 (device fabrication) and the Center for Emergent Materials, an NSF MRSEC under award number DMR-1420451 (bulk CrI3 crystal growth and optical measurements). This work was also partially supported by the Cornell Center for Materials Research with funding from the NSF MRSEC program under DMR-1719875 (first principles calculations and transport measurements). The growth of hBN crystals was supported by the Elemental Strategy Initiative conducted by the MEXT, Japan, and the CREST(JPMJCR15F3), JST. D.W. gratefully acknowledges the financial support by the German Science Foundation (Deutsche Forschungsgemeinschaft, DFG) under the fellowship number WE6480/1. K.F.M. acknowledges support from a David and Lucille Packard Fellowship and a Sloan Fellowship.

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T.L., S.J., K.F.M. and J.S. designed the study. T.L. developed the high-pressure cell set-up. T.L. and S.J. fabricated the devices and performed the measurements with the assistance of Z.W. and Y.X. N.S. and C.J.F. performed the first principles calculations. D.W. and J.E.G. grew the bulk CrI3 crystals and K.W. and T.T. grew the bulk hBN crystals. T.L., K.F.M. and J.S. co-wrote the manuscript. All the authors discussed the results and commented on the manuscript.

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Correspondence to Kin Fai Mak or Jie Shan.

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Supplementary Figs. 1–7, Notes 1–5, References 1–11 and Table 1.

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Li, T., Jiang, S., Sivadas, N. et al. Pressure-controlled interlayer magnetism in atomically thin CrI3. Nat. Mater. 18, 1303–1308 (2019). https://doi.org/10.1038/s41563-019-0506-1

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