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The orthorhombic Haldane spin chain compound Tb2BaNiO5 (Neel order, TN1= 63K) has been shown to be an exotic multiferroic system below (TN2) 25 K due tovarious fascinating features, pointing to a strong potential for theadvancement of concepts in this field. In particular, the rare-earth ions playa direct decisive role unlike in many other well known multiferroic materialsand there appears to be a critical canting angle, developing below TN2,subtended by Tb 4f and Ni 3d moments to trigger this cross coupling phenomenon.However, for a small replacement of Sr for Ba, viz. in Tb2Ba0.9Sr0.1NiO5,ferroelectricity was reported to get destroyed, but retaining magnetic featuresat (TN1) 55 K and (TN2) 14 K. In this article, we address the origin ofsuppression of multiferrocity in this Sr doped system through neutrondiffraction studies and density functional theory calculations. We find that,unlike in Tb2BaNiO5, there is no pronounced change in the relative cantingangle of the magnetic moments around TN2 and that the absolute value of thisparameter down to 2 K fails to exceed the critical value noted for the parent,thereby explaining the origin of destruction of magnetoelectric coupling in theSr doped material. This finding renders strong support to the proposal ofpossible existence of critical canting angle, at least in some cases, to inducemultiferroicity, apart from serving as a route to engineer multiferroicmaterials for applications.

Origin of destruction of multiferroicity in Tb2BaNiO5 by Sr doping and its implications