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We report cooperative magnetic orderings in a 6H-perovskite multiferroicsystem, Ba3HoRu2O9, via comprehensive neutron powder diffraction measurements.This system undergoes long-range antiferromagnetic ordering at TN1 ~ 50 K witha propagation wave vector of K1 = (0.5 0 0), a transition temperature muchhigher than the previously reported one at ~10 K (TN2). Both Ru and Ho-momentsorder simultaneously below TN1, followed by spin-reorientations at lowertemperatures, demonstrating strong Ru(4d)-Ho(4f) magnetic correlation. BelowTN1 another magnetic phase with a propagation wave vector K2 = (0.25 0.25 0)emerges and coexists with the one associated with K1, which is rarely observedand suggests complex magnetism due to phase competition in the magnetic groundstate. We argue that the exchange-striction arising from the up-up-down-downspin structure associated with K2-wave vector below TN2 may be responsible forthe small ferroelectric polarization reported previously in this compound.

Cooperative Ru(4d)-Ho(4f) magnetic orderings and phase coexistence in the 6H-perovskite multiferroic Ba3HoRu2O9