No abstract

Transition‐metal dichalcogenides (TMDCs) are an aspiring class of materials with unique electronic and optical properties and potential applications in spin‐based electronics. Here, terahertz emission spectroscopy is used to study spin‐to‐charge current conversion (S2C) in the TMDC NbSe2 in ultra‐high‐vacuum‐grown F|NbSe2 thin‐film stacks, where F is a layer of ferromagnetic Fe or Ni. Ultrafast laser excitation triggers an ultrafast spin current that is converted into an in‐plane charge current and, thus, a measurable THz electromagnetic pulse. The THz signal amplitude as a function of the NbSe2 thickness shows that the measured signals are fully consistent with an ultrafast optically driven injection of an in‐plane‐polarized spin current into NbSe2. Modeling of the spin‐current dynamics reveals that a sizable fraction of the total S2C originates from the bulk of NbSe2 with the opposite, negative sign of the spin Hall angle as compared to Pt. By a quantitative comparison of the emitted THz radiation from F|NbSe2 to F|Pt reference samples and the results of ab initio calculations, it is estimated that the spin Hall angle of NbSe2 for an in‐plane polarized spin current lies between ‐0.2% and ‐1.1%, while the THz spin‐current relaxation length is of the order of a few nanometers.

We perform first-principles calculations to determine the electronic, magnetic and transport properties of rare-earth dichalcogenides taking a monolayer of the H-phase EuS2 as a representative. We predict that the H-phase of the EuS2 monolayer exhibits a half-metallic behavior upon doping with a very high magnetic moment. We find that the electronic structure of EuS2 is very sensitive to the value of Coulomb repulsion U , which effectively controls the degree of hybridization between Eu-f and S-p states. We further predict that the non-trivial electronic structure of EuS2 directly results in a pronounced anomalous Hall effect with non-trivial band topology. Moreover, while we find that the spin Hall effect closely follows the anomalous Hall effect in the system, the orbital complexity of the system results in a very large orbital Hall effect, whose properties depend very sensitively on the strength of correlations. Our findings thus promote rare-earth based dichalcogenides as a promising platform for topological spintronics and orbitronics.