Abstract
Substitution of Ca2+ and Sr2+ at the A-site of multiferroic TbMnO3 bulk results in an increased average ionic radius and ionic-size mismatch, and was found to reduce the orthorhombic distortion. Signatures of long-range ferromagnetic-like ordering at 78 K in Tb0.67Ca0.33MnO3 and at 87 K in Tb0.67Sr0.33MnO3 samples are clearly observed in both the dc and ac susceptibility data. A compensation temperature is also observed in Tb0.67Ca0.33MnO3, indicating the antiparallel alignment of Tb3+ moments to the Mn3+–Mn4+ moments. The canted antiferromagnetic ordering coexists with antiferromagnetic clusters, resulting in spin-glass-like behavior at low temperatures. An increased average ionic radius and ionic-size mismatch at the A-site are determined to be critical factors in determining the magnetic properties of the hole-doped manganites.
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