Direct Visualization of Trimerized States in 1T

Transition-metal dichalcogenides containing tellurium anions show remarkable charge-lattice modulated structures and prominent interlayer character. Using cryogenic scanning transmission electron microscopy (STEM), we map the atomic-scale structures of the high temperature (HT) and low temperature (LT) modulated phases in 1T^{'}-TaTe_{2}. At HT, we directly show in-plane metal distortions which form trimerized clusters and staggered, three-layer stacking. In the LT phase at 93 K, we visualize an additional trimerization of Ta sites and subtle distortions of Te sites by extracting structural information from contrast modulations in plan-view STEM data. Coupled with density functional theory calculations and image simulations, this approach opens the door for atomic-scale visualizations of low temperature phase transitions and complex displacements in a variety of layered systems.

Pressure-controlled interlayer magnetism in atomically thin CrI3.

Stacking order can influence the physical properties of two-dimensional van der Waals materials1,2. 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 calculations3-8 and suggests a route towards nanoscale magnetic textures by moiré engineering3,9.

Current-Induced Torques with Dresselhaus Symmetry Due to Resistance Anisotropy in 2D Materials.

We report measurements of current-induced torques in heterostructures of Permalloy (Py) with TaTe2, a transition-metal dichalcogenide (TMD) material possessing low crystal symmetry, and observe a torque component with Dresselhaus symmetry. We suggest that the dominant mechanism for this Dresselhaus component is not a spin-orbit torque but rather the Oersted field arising from a component of current that flows perpendicular to the applied voltage due to resistance anisotropy within the TaTe2. This type of transverse current is not present in wires made from a single uniform layer of a material with resistance anisotropy but will result whenever a material with resistance anisotropy is integrated into a heterostructure with materials having different resistivities, thereby producing a spatially nonuniform pattern of current flow. This effect will therefore influence measurements in a wide variety of heterostructures incorporating 2D TMD materials and other materials with low crystal symmetries.

Stacking-Dependent Magnetism in Bilayer CrI3.

We report the connection between the stacking order and magnetic properties of bilayer CrI3 using first-principles calculations. We show that the stacking order defines the magnetic ground state. By changing the interlayer stacking order, one can tune the interlayer exchange interaction between antiferromagnetic and ferromagnetic. To measure the predicted stacking-dependent magnetism, we propose using linear magnetoelectric effect. Our results not only gives a possible explanation for the observed antiferromagnetism in bilayer CrI3 but also have direct implications in heterostructures made of two-dimensional magnets.

Tuning Ising superconductivity with layer and spin-orbit coupling in two-dimensional transition-metal dichalcogenides.

Systems simultaneously exhibiting superconductivity and spin-orbit coupling are predicted to provide a route toward topological superconductivity and unconventional electron pairing, driving significant contemporary interest in these materials. Monolayer transition-metal dichalcogenide (TMD) superconductors in particular lack inversion symmetry, yielding an antisymmetric form of spin-orbit coupling that admits both spin-singlet and spin-triplet components of the superconducting wavefunction. Here, we present an experimental and theoretical study of two intrinsic TMD superconductors with large spin-orbit coupling in the atomic layer limit, metallic 2H-TaS2 and 2H-NbSe2. We investigate the superconducting properties as the material is reduced to monolayer thickness and show that high-field measurements point to the largest upper critical field thus reported for an intrinsic TMD superconductor. In few-layer samples, we find the enhancement of the upper critical field is sustained by the dominance of spin-orbit coupling over weak interlayer coupling, providing additional candidate systems for supporting unconventional superconducting states in two dimensions.

Van der Waals engineering of ferromagnetic semiconductor heterostructures for spin and valleytronics.

The integration of magnetic material with semiconductors has been fertile ground for fundamental science as well as of great practical interest toward the seamless integration of information processing and storage. We create van der Waals heterostructures formed by an ultrathin ferromagnetic semiconductor CrI3 and a monolayer of WSe2. We observe unprecedented control of the spin and valley pseudospin in WSe2, where we detect a large magnetic exchange field of nearly 13 T and rapid switching of the WSe2 valley splitting and polarization via flipping of the CrI3 magnetization. The WSe2 photoluminescence intensity strongly depends on the relative alignment between photoexcited spins in WSe2 and the CrI3 magnetization, because of ultrafast spin-dependent charge hopping across the heterostructure interface. The photoluminescence detection of valley pseudospin provides a simple and sensitive method to probe the intriguing domain dynamics in the ultrathin magnet, as well as the rich spin interactions within the heterostructure.

Gate-Controllable Magneto-optic Kerr Effect in Layered Collinear Antiferromagnets.

Using symmetry arguments and a tight-binding model, we show that for layered collinear antiferromagnets, magneto-optic effects can be generated and manipulated by controlling crystal symmetries through a gate voltage. This provides a promising route for electric field manipulation of the magneto-optic effects without modifying the underlying magnetic structure. We further demonstrate the gate control of the magneto-optic Kerr effect (MOKE) in bilayer MnPSe_{3} using first-principles calculations. The field-induced inversion symmetry breaking effect leads to gate-controllable MOKE, whose direction of rotation can be switched by the reversal of the gate voltage.