Magnetic Interactions in the Polar Ferrimagnet with a Bipartite Structure

Abstract: The polar magnets A$2$Mo$_3$O$_8$ (A=Fe, Mn, Co, and Ni) feature a bipartite structure, where the magnetic A$^{2+}$ ions occupy two different sites with octahedral and tetrahedral oxygen coordinations. This bipartite structure provides a platform for the emergence of nontrivial magnetoelectric (ME) effects and intriguing excitation behaviors, and thus creates significant research interest. In this study, we conduct inelastic neutron scattering measurements on single crystals of Mn$_2$Mo$_3$O$_8$, an L-type ferrimagnet in the A$_2$Mo$_3$O$_8$ family, to investigate its spin dynamics. The obtained magnetic excitation spectra reveal two distinct magnon dispersions corresponding to the octahedral and tetrahedral spins in Mn$_2$Mo$_3$O$_8$. These magnon bands can be well described by a spin Hamiltonian including Heisenberg and single-ion anisotropy terms. Employing our effective spin model, we successfully reproduce the unusual temperature dependence of the L-type ferrimagnetic susceptibility through self-consistent mean-field theory. This research reveals the significance of the bipartite structure in determining the excitation properties of the polar magnets $\rm{A{2}Mo_{3}O_{8}}$ and provides valuable insights into the spin dynamics of L-type ferrimagnets.