Optical magnetoelectric effect in the polar honeycomb antiferromagnet Fe2Mo3O8

The lack of both time-reversal and spatial inversion symmetry in polar magnets is a prerequisite for the occurrence of optical magnetoelectric effects such as nonreciprocal directional dichroism, i.e., a difference in refractive index and absorption for two counter-propagating electromagnetic waves, which has the potential for the realization of optical diodes. In particular, antiferromagnetic materials with magnetic excitations in the THz range such as Fe₂Mo₃O₈ are promising candidates for next-generation spintronic applications. In a combined experimental and theoretical effort we investigated the THz excitations of the polar honeycomb antiferromagnet Fe₂Mo₃O₈ in external magnetic fields and their nonreciprocal directional dichroism, together with the temperature dependence of the electronic transitions in the mid- and near-infrared frequency range. Using an advanced single-ion approach for the Fe ions, we are able to describe optical excitations from the THz to the near-infrared frequency range quantitatively and model the observed nonreciprocal directional dichroism in the THz regime successfully.