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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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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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.
The authors declare no competing interests.
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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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