Momentum-resolved linear dichroism in bilayerMoS2

In solid state photoemission experiments it is possible to extract information about the symmetry and orbital character of the electronic wave functions via the photoemission selection rules that shape the measured intensity. This approach can be expanded in a pump-probe experiment where the intensity contains additional information about interband excitations induced by an ultrafast laser pulse with tunable polarization. Here, we find an unexpected strong linear dichroism effect (up to 42.4%) in the conduction band of bilayer ${\mathrm{MoS}}₂$, when measuring energy- and momentum-resolved snapshots of excited electrons by time- and angle-resolved photoemission spectroscopy. We model the polarization-dependent photoemission intensity in the transiently populated conduction band using the semiconductor Bloch equations. Our theoretical analysis reveals a strongly anisotropic momentum dependence of the optical excitations due to intralayer single-particle hopping, which explains the observed linear dichroism.