Simultaneously Magnetic- and Electric-dipole Active Spin Excitations Govern the Static Magnetoelectric Effect in Multiferroic Materials

We derive a sum rule to demonstrate that the static magnetoelectric (ME) effect is governed by optical transitions that are simultaneously excited via the electric and magnetic components of light. By a systematic analysis of magnetic point groups, we show that the ME sum rule is applicable to a broad variety of non-centrosymmetric magnets including ME multiferroic compounds. Due to the dynamical ME effect, the optical excitations in these materials can exhibit directional dichroism, i.e. the absorption coefficient can be different for counter-propagating light beams. According to the ME sum rule, the magnitude of the linear ME effect of a material is mainly determined by the directional dichroism of its low-energy optical excitations. Application of the sum rule to the multiferroic Ba$_2$CoGe$_2$O$_7$, Sr$_2$CoSi$_2$O$_7$ and Ca$_2$CoSi$_2$O$_7$ shows that in these compounds the static ME effect is mostly governed by the directional dichroism of the spin-wave excitations in the GHz-THz spectral range. On this basis, we argue that the studies of directional dichroism and the application of ME sum rule can promote the synthesis of new materials with large static ME effect.