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Synthesis and extensive structural, pyroelectric, magnetic, dielectric andmagneto-electric characterizations are reported for polycrystalline Co4Nb2O9towards unraveling the multiferroic state especially in reference to themagnetic spin flop transition. Magnetic measurements confirm the Co4Nb2O9becomes antiferromagnetic (AFM) at around 28 K but no clear evidence forspin-flop effect was found. Associated with the magnetic phase transition, asharp peak in pyroelectric current indicates the appearance of the strongmagneto-electric coupling below Neel temperature (TN) with a large couplingconstant upto 17.8 uC/m^2T. Using temperature oscillation technique, weestablish Co4Nb2O9 to be a genuine multiferroic with spontaneous electricpolarization in the anti-ferromagnetic state.

Exceptional magneto-electric coupling and spontaneous electric polarization in anti-ferromagnet Co4Nb2O9