Extraordinarily large intrinsic magnetodielectric coupling of Tb member within the Haldane spin-chain family, R2BaNiO5

The Haldane spin-chain compound, Tb2BaNiO5, has been known to order antiferromagnetically below (T_N= ) 63 K. The present magnetic studies on the polycrystals bring out that there is another magnetic transition at a lower temperature (T_2= ) 25 K, with a pronounced magnetic-field induced metamagnetic and metaelectric behavior. Multiferroic features are found below T_2 only, and not at T_N. The most intriguing observation is that the observed change of dielectric constant is intrinsic and largest (e.g., about 18% at 15 K) within this Haldane spin-chain family, R2BaNiO5. Taking into account that this trend (the largest change for Tb case within this family) correlates with a similar trend in T_N (with the values of T_N being about 55, 58, 53 and 32 K for Gd, Dy, Ho and Er cases), we believe that an explanation usually offered for this T_N behavior in rare-earth systems is applicable for this behavior as well . That is, single-ion anisotropy following crystal-field splitting is responsible for this extraordinary magnetodielectric effect in this Tb case. To our knowledge, such an observation was not made in the past literature of multiferroics.