Ferrimagnetism of the magnetoelectric compound Cu$_2$OSeO$_3$ probed by $^{77}$Se NMR

Abstract

We present a thorough $^{77}$Se NMR study of a single crystal of the magnetoelectric compound Cu$_2$OSeO$_3$. The temperature dependence of the local electronic moments extracted from the NMR data is fully consistent with a magnetic phase transition from the high-T paramagnetic phase to a low-T ferrimagnetic state with 3/4 of the Cu$^{2+}$ ions aligned parallel and 1/4 aligned antiparallel to the applied field of 14.09 T. The transition to this 3up-1down magnetic state is not accompanied by any splitting of the NMR lines or any abrupt modification in their broadening, hence there is no observable reduction of the crystalline symmetry from its high-T cubic \textit{P}2$_1$3 space group. These results are in agreement with high resolution x-ray diffraction and magnetization data on powder samples reported previously by Bos {\it et al.} [Phys. Rev. B, {\bf 78}, 094416 (2008)]. We also develop a mean field theory description of the problem based on a microscopic spin Hamiltonian with one antiferromagnetic ($J_\text{afm}\simeq 68$ K) and one ferromagnetic ($J_\text{fm}\simeq -50$ K) nearest-neighbor exchange interaction.