The physical properties of two-dimensional van der Waals crystals can be sensitive to interlayer coupling. For two-dimensional magnets1–3, 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 state4–10. Here, we demonstrate pressure tuning of magnetic order in the two-dimensional magnet CrI3. We probe the magnetic states using tunnelling8,11–13 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. Pressure-induced changes in the magnetic order of bilayer and trilayer van der Waals crystals are revealed and attributed to changes in the stacking arrangement.

Switching 2D magnetic states via pressure tuning of layer stacking