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61Ni Nuclear Forward Scattering Study of Magnetic Hyperfine Interactions in Double Perovskites A2NiMnO6 (A = Sc, In, Tl)

The relationship between hyperfine interactions, local structure and magnetism in ordered double perovskites A2NiMnO6 (A = Sc, In and Tl) is investigated by nuclear forward scattering (NFS) with the 61Ni nuclear transition. Special attention is given to a quantitative determination of on-site and transferred hyperfine fields on the 61Ni nuclei. The anomalous small value of the saturated hyperfine magnetic field Hhf(0) in antiferromagnetic Sc2NiMnO6 is explained by spin-orbital coupling and strong Ni-3d and O-2p hybridization. The temperature evolution of Hhf(T) is reproduced with Neel temperature TN1 ≈ 37 K, that is incompatible with the earlier assumption that magnetic ordering in Ni sublattice takes place below TN2 ≈ 17 K. Significantly reduced fields Hhf(0) in In2NiMnO6 (∼21 kOe) with a cycloidal magnetic structure and Tl2NiMnO6 (∼18 kOe) with collinear ferromagnetic ordering are related to the supertransferred hyperfine field (HSTHF) induced by the nearest Mn4+ neighbors. Taking into account the angul...