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A large spin-orbit coupling is a way to control strong magnetodielectric (MD)coupling in a higher d-orbital materials. However reports are rare on suchcompounds due to often leaky conductive behavior. Here, we demonstrate MDcoupling in a Ru-based 6H-perovskite system, Ba3NdRu2O9. The rare-earth ion ina 6H-perovskite makes the system insulating enough to carry out MDinvestigation. The compound is ferromagnetically ordered below 24 K (TC),followed by another magnetic feature at T~ 17 K (T2). The dielectric constantclearly traces the magnetic ordering, manifesting a peak at the onset of TC,which is suppressed by the application of an external magnetic field (H). Theresults indicate the presence of MD coupling in this compound, which is furtherconfirmed by the H-dependence of the dielectric constant. Interestingly, across-over of the sign of MD coupling is observed at T ~ T2. We conclude thattwo different mechanism controls the MD coupling which yields positive andnegative coupling, respectively. Both mechanisms are competing as a function oftemperature and magnetic field. This brings us a step closer to design andcontrol the magnetodielectric effect in 6H-perovskites containing higherd-orbital elements.

Magnetodielectric coupling in a Ru-based 6H-perovskite, Ba3NdRu2O9