Dielectric, magnetic and lattice dynamics properties of double perovskite (Ca0.5Mn1.5)MnWO6

Abstract

Recent dielectric and magnetic studies of (Ca0.5Mn1.5)MnWO6 ceramics [A.A. Belik, Chem. Mater. 36, 7604 (2024)] have classified this material as a rare hybrid multiferroic, with both antiferromagnetic and (anti)ferroelectric ordering occurring at the same temperature of 22 K. The pronounced dielectric anomaly observed at this temperature indicated that the structural change is primarily induced by a phonon soft mode and not by a spin arrangement, as is usually the case in type II multiferroics. However, our comprehensive investigation involving new ceramic samples as well as the sample from the above-mentioned reference does not support this conclusion. Low-temperature polarization measurements revealed no evidence of either ferroelectric or antiferroelectric order in both sample series. The dielectric permittivity exhibits only a slight change at the antiferromagnetic transition, and phonon modes observed in IR and Raman spectra show no indication of a symmetry change at low temperatures. In the new samples the Neel temperature is shifted to TN = 18 K. XRD, SEM, EDS and WDS analyses confirmed the composition (Ca0.5Mn1.5)MnWO6 of both ceramics, but also indicated a small amount (percentage points) of MnO and CaO impurities in the sample from the previous publication and Mn3O4, CaWO4 secondary phases (<4%) in the new ceramics. The differences in dielectric and magnetic properties of the two samples can therefore be explained by their different chemical purity. The small dielectric anomaly of the new sample at the antiferromagnetic transition temperature is explained by a spin-phonon coupling. We conclude that (Ca0.5Mn1.5)MnWO6 is not a multiferroic, but a paraelectric antiferromagnet.