Quasi 2D electronic states with high spin-polarization in centrosymmetric MoS₂ bulk crystals

Time reversal dictates that nonmagnetic, centrosymmetric crystals cannot be spin-polarized as a whole. However, it has been recently shown that the electronic structure in these crystals can in fact show regions of high spin-polarization, as long as it is probed locally in real and in reciprocal space. In this article we present the first observation of this type of compensated polarization in MoS$_2$ bulk crystals. Using spin- and angle-resolved photoemission spectroscopy (ARPES) we directly observed a spin-polarization of more than 65% for distinct valleys in the electronic band structure. By additionally evaluating the probing depth of our method we find that these valence band states at the $\overline{\text{K}}$ point in the Brillouin zone are close to fully polarized for the individual atomic trilayers of MoS$_2$, which is confirmed by our density functional theory calculations. Furthermore, we show that this spin-layer locking leads to the observation of highly spin-polarized bands in ARPES since these states are almost completely confined within two dimensions. Our findings prove that these highly desired properties of MoS$_2$ can be accessed without thinning it down to the monolayer limit.