Effects of Sr substitution at A-site in ordered perovskite Ba3-xSrxMnNb2O9 (x = 1 and 3) have been investigated using X-ray diffraction, magnetization, dielectric/magnetodielectric and neutron diffraction measurements. The parent compound Ba3MnNb2O9 having a large spin (S=5/2) is known to exhibit type-II multiferroic properties with quasi 2D triangular lattice antiferromagnetic ground state. A slight perturbation in exchange interaction due to substitution of smaller size isovalent ion at the A-site in Ba3-xSrxMnNb2O9 (x = 1 and 3) has been found to alter the ground states drastically and hence the multiferroicity. The crucial role of various fluctuations (quantum and/or thermal), weak lattice distortion induced by Sr-substitution and slight imbalance between different fluctuations in determining the ground states and the multiferroicity is discussed and compared with the results of smaller spin compounds (S = 1/2 or 1).
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