No abstract

We report the observation of a very large negative magnetoresistance effect in a van der Waals tunnel junction incorporating a thin magnetic semiconductor, CrI, as the active layer. At constant voltage bias, current increases by nearly one million percent upon application of a 2 T field. The effect arises from a change between antiparallel to parallel alignment of spins across the different CrI layers. Our results elucidate the nature of the magnetic state in ultrathin CrI and present new opportunities for spintronics based on two-dimensional materials.

We conduct a comprehensive study of three different magnetic semiconductors, CrI3, CrBr3, and CrCl3, by incorporating both few-and bi-layer samples in van der Waals tunnel junctions. We find that the interlayer magnetic ordering, exchange gap, magnetic anisotropy, as well as magnon excitations evolve systematically with changing halogen atom. By fitting to a spin wave theory that accounts for nearest neighbor exchange interactions, we are able to further determine a simple spin Hamiltonian describing all three systems. These results extend the 2D magnetism platform to Ising, Heisenberg, and XY spin classes in a single material family. Using magneto-optical measurements, we additionally demonstrate that ferromagnetism can be stabilized down to monolayer in more isotropic CrBr3, with transition temperature still close to that of the bulk.

We report structural properties, physical properties, and the electronic structure of van der Waals (vdW) crystal VI3. Detailed analysis reveals that VI3 exhibits a structural transition from monoclinic C2/m to rhombohedral R3̅ at T s ≈ 79 K, similar to CrX3 (X = Cl, Br, I). Below T s, a long-range ferromagnetic (FM) transition emerges at T c ≈ 50 K. The local moment of V in VI3 is close to the high-spin state V3+ ion (S = 1). Theoretical calculations suggest that VI3 may be a Mott insulator with a band gap of about 0.90 eV. In addition, VI3 has a relatively small interlayer binding energy and can be exfoliated easily down to a few layers experimentally. Therefore, VI3 is a candidate for two-dimensional FM semiconductors. It also provides a novel platform to explore 2D magnetism and vdW heterostructures in S = 1 system.

Two-dimensional (2D) magnetism has been long sought-after and only very recently realized in atomic crystals of magnetic van der Waals materials. So far, a comprehensive understanding of the magnetic excitations in such 2D magnets remains missing. Here we report polarized micro-Raman spectroscopy studies on a 2D honeycomb ferromagnet CrI3. We show the definitive evidence of two sets of zero-momentum spin waves at frequencies of 2.28 terahertz (THz) and 3.75 THz, respectively, that are three orders of magnitude higher than those of conventional ferromagnets. By tracking the thickness dependence of both spin waves, we reveal that both are surface spin waves with lifetimes an order of magnitude longer than their temporal periods. Our results of two branches of high-frequency, long-lived surface spin waves in 2D CrI3 demonstrate intriguing spin dynamics and intricate interplay with fluctuations in the 2D limit, thus opening up opportunities for ultrafast spintronics incorporating 2D magnets.