Non-degenerate valleys in the half-metallic ferromagnet Fe/WS${}_2$

We present a first principles investigation of the electronic properties of monolayer WS${}_2$ coated with an overlayer of Fe. Our ab initio calculations reveal that the system is a half-metallic ferromagnet with a gap of $\sim 1$ eV for the majority spin channel. Furthermore, the combined effect of time-reversal symmetry breaking due to the magnetic Fe overlayer and the large spin-orbit coupling induced by W gives rise to non-degenerate K and K${}^{\mathrm{\prime }}$ valleys. This has a tremendous impact on the excited state properties induced by externally applied circularly polarized light. Our analysis demonstrates that the latter induces a singular hot spot structure of the transition probability around the K and K${}^{\mathrm{\prime }}$ valleys for right and left circular polarization, respectively. We trace back the emergence of this remarkable effect to the strong momentum dependent spin-noncollinearity of the valence band involved. As a main consequence, a strong valley-selective magnetic circular dichroism is obtained, making this system a prime candidate for spintronics and photonics applications.