Two-dimensional van der Waals magnetic materials are intriguing for applications in the future spintronics devices, so it is crucial to explore strategy to control the magnetic properties. Here, we carried out first-principles calculations and Monte Carlo simulations to investigate the effect of biaxial strain and hydrostatic pressure on the magnetic properties of the bilayer CrI 3 . We found that the magnetic anisotropy, intralayer and interlayer exchange interactions, and Curie temperature can be tuned by biaxial strain and hydrostatic pressure. Large compressive biaxial strain may induce a ferromagneticto-antiferromagnetic transition in both CrI 3 layers. The hydrostatic pressure could enhance the intralayer exchange interaction significantly and hence largely boost the Curie temperature. The effect of the biaxial strain and hydrostatic pressure revealed in the bilayer CrI 3 may be generalized to other two-dimensional magnetic materials.
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