Magneto-optical anisotropies of two-dimensional antiferromagnetic MPX3 from first principles

Here we systematically investigate the impact of the spin direction on the electronic and optical properties of transition metal phosphorus trichalcogenides (MPX3, M=Mn, Ni, Fe; X=S, Se) exhibiting various antiferromagnetic arrangements within the 2D limit. Our analysis based on the density functional theory and versatile formalism of Bethe-Salpeter equation reveals larger exciton binding energies for MPS3 (up to 1.1 eV in air) than MPSe3 (up to 0.8 eV in air), exceeding the values of transition metal dichalcogenides (TMDs). For the (Mn,Fe)PX3, we determine the optically active band-edge transitions, revealing that they are sensitive to in-plane magnetic order, irrespective of the type of chalcogen atom. We predict the anistropic effective masses and the type of linear polarization as important fingerprints for sensing the type of magnetic AFM arrangements. Furthermore, we identify the spin-orientation-dependent features such as the valley splitting, the effective mass of holes, and the exciton binding energy. In particular, we demonstrate that for MnPX3 (X=S, Se), a pair of nonequivalent K+ and K− points exists yielding the valley splittings that strongly depend on the direction of AFM aligned spins. Notably, for the out-of-plane direction of spins, two distinct peaks are expected to be visible below the absorption onset, whereas one peak should emerge for the in-plane configuration of spins. These spin-dependent features provide an insight into spin flop transitions of 2D materials. Finally, we propose a strategy for how the spin valley polarization can be realized in 2D AFM within a honeycomb lattice. Published by the American Physical Society 2024