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Stacking order can significantly influence the physical properties of two-dimensional (2D) van der Waals materials. The recent isolation of atomically thin magnetic materials opens the door for control and design of magnetism via stacking order. Here we apply hydrostatic pressure up to 2 GPa to modify the stacking order in a prototype van der Waals magnetic insulator CrI3. We observe an irreversible interlayer antiferromagnetic (AF) to ferromagnetic (FM) transition in atomically thin CrI3 by magnetic circular dichroism and electron tunneling measurements. The effect is accompanied by a monoclinic to a rhombohedral stacking order change characterized by polarized Raman spectroscopy. Before the structural change, the interlayer AF coupling energy can be tuned up by nearly 100% by pressure. Our experiment reveals interlayer FM coupling, which is the established ground state in bulk CrI3, but never 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 and suggests a route towards nanoscale magnetic textures by moire engineering.
Recently, two-dimensional (2D) materials with strong in-plane anisotropic properties such as black phosphorus have demonstrated great potential for developing new devices that can take advantage of its reduced lattice symmetry with potential applicat
Diverse interlayer tunability of physical properties of two-dimensional layers mostly lies in the covalent-like quasi-bonding that is significant in electronic structures but rather weak for energetics. Such characteristics result in various stacking
Electronic states in two-dimensional layered materials can exhibit a remarkable variety of correlated phases including Wigner-crystals, Mott insulators, charge density waves, and superconductivity. Recent experimental and theoretical research has ind
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We conduct a comprehensive study of three different magnetic semiconductors, CrI$_3$, CrBr$_3$, and CrCl$_3$, by incorporating both few- and bi-layer samples in van der Waals tunnel junctions. We find that the interlayer magnetic ordering, exchange g