Pressure-controlled interlayer magnetism in atomically thin CrI3

Tingxin Li; Shengwei Jiang; Nikhil Sivadas; Zefang Wang; Yang Xu; Daniel Weber; Joshua E Goldberger; Kenji Watanabe; Takashi Taniguchi; Craig J Fennie; Kin Fai Mak; Jie Shan

doi:10.1038/s41563-019-0506-1

Pressure-controlled interlayer magnetism in atomically thin CrI₃

Nat Mater. 2019 Dec;18(12):1303-1308. doi: 10.1038/s41563-019-0506-1. Epub 2019 Oct 28.

Authors

Tingxin Li^#¹, Shengwei Jiang^#², Nikhil Sivadas¹, Zefang Wang¹, Yang Xu¹, Daniel Weber³, Joshua E Goldberger³, Kenji Watanabe⁴, Takashi Taniguchi⁴, Craig J Fennie¹, Kin Fai Mak^{5

6

7}, Jie Shan^{8

9

10}

Affiliations

¹ School of Applied and Engineering Physics, Cornell University, Ithaca, NY, USA.
² Laboratory of Atomic and Solid State Physics, Cornell University, Ithaca, NY, USA.
³ Department of Chemistry and Biochemistry, The Ohio State University, Columbus, OH, USA.
⁴ National Institute for Materials Science, Tsukuba, Japan.
⁵ School of Applied and Engineering Physics, Cornell University, Ithaca, NY, USA. [email protected].
⁶ Laboratory of Atomic and Solid State Physics, Cornell University, Ithaca, NY, USA. [email protected].
⁷ Kavli Institute at Cornell for Nanoscale Science, Ithaca, NY, USA. [email protected].
⁸ School of Applied and Engineering Physics, Cornell University, Ithaca, NY, USA. [email protected].
⁹ Laboratory of Atomic and Solid State Physics, Cornell University, Ithaca, NY, USA. [email protected].
¹⁰ Kavli Institute at Cornell for Nanoscale Science, Ithaca, NY, USA. [email protected].

^# Contributed equally.

PMID: 31659292
DOI: 10.1038/s41563-019-0506-1

Abstract

Stacking order can influence the physical properties of two-dimensional van der Waals materials^1,2. 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 calculations^3-8 and suggests a route towards nanoscale magnetic textures by moiré engineering^3,9.

Publication types

Research Support, Non-U.S. Gov't
Research Support, U.S. Gov't, Non-P.H.S.