Homogeneous solid solutions of sol−gel-prepared R 2 NiMnO 6 (R = La, Pr, Nd, Sm, Gd, Tb, Dy, Y, and Ho) double perovskites crystallize in a B-site-ordered monoclinic structure (P2 1 /n space group). Monoclinic distortion enhances with decreasing R 3+ ionic radii (r R 3+ ). The magnetic ordering temperature (T C ) decreases from 270 K for La 2 NiMnO 6 to 80 K for Ho 2 NiMnO 6 as r R 3+ decreases from 1.16 Å (La 3+ ) to 1.02 Å (Ho 3+ ). An additional magnetic anomaly is observed in Nd 2 NiMnO 6 , Sm 2 NiMnO 6 , Tb 2 NiMnO 6 , and Dy 2 NiMnO 6 at lower temperatures, which originates from the 3d−4f coupling between Mn−Ni and Nd 3+ /Sm 3+ /Tb 3+ /Dy 3+ magnetic moments. Further, high saturation magnetization is achieved for all samples, indicating that they are atomically ordered and have less antisite disorders. Upon a decrease in the size of R 3+ , the local structure shows an expansion of NiO 6 octahedra and almost unchanged of MnO 6 octahedra. X-ray-absorption near-edge spectroscopy reveals a majority of Ni 2+ and Mn 4+ ions in all samples. Softening of phonon modes results in the elongation of the Ni/Mn−O bond length. Finally, a correlation among lattice parameters, structural distortion, octahedral tilting, superexchange angle, electronic band gap, Curie temperature, and the rare-earth ionic radius is established.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.