Coupled sawtooth chain exchange network in olivine Mn$_2$GeO$_4$

Abstract

Sawtooth chain magnets have been a subject of historical interest in the field of frustrated magnetism, with classical olivine family $M_2TX_4$, ($M$ - 3d, $T$ - 4p, $X$ - chalcogen elements) typically realizing simple $\mathbf{k} = (000)$ states. The magnetism of the Mn$_2$GeO$_4$ olivine is surprisingly complex, proceeding from commensurate states to a multiferroic commensurate + incommensurate phase. Here we report inelastic neutron scattering results from a Mn$_2$GeO$_4$ single crystal and develop an effective Hamiltonian including long-distance bilinear and dipolar interactions. The magnetic interactions are predominantly antiferromagnetic and span a three-dimensional exchange network consisting of coupled sawtooth chains. Based on the determined strength of the couplings, the dominant sawtooth chains appear at third- and fourth- rather than next-nearest-neighbor. However the next-nearest-neighbor interaction is, along with a modest Dzyaloshinskii-Moriya interaction, important for modeling the observed incommensurability. We use the best-fit Hamiltonian as the basis for Langevin dynamics simulations and Luttinger-Tisza calculations of the high-temperature commensurate transition.