Structural transformation, Griffiths phase and metal-insulator transition in polycrystalline Nd2-x Sr x NiMnO6 (x = 0, 0.2, 0.4, 0.5 and 1) compound

J Phys Condens Matter. 2018 Sep 5;30(35):355401. doi: 10.1088/1361-648X/aad573. Epub 2018 Jul 24.

Abstract

Polycrystalline double perovskite Nd2-x Sr x NiMnO6 (x = 0, 0.2, 0.4, 0.5 and 1) samples were synthesized using the solid state reaction method. There occurs a structural transformation from monoclinic (P21/n, for x = 0 to x = 0.5) to cubic (Fm [Formula: see text] m, for x = 1) with increasing Sr doping. Raman spectroscopy reveals the increase in static disorder with doping. The Curie temperature (T C) shows a small increase from x = 0 to 0.5 (T C ~ 200 K), but for x = 1, T C increases drastically upto ~264 K. The deviation of 1/χ(T) from Curie-Weiss behaviour for doped samples with exponent less than one, indicates a development of the Griffiths phase with doping. The systematic reduction in magnetic moment at 5 K suggests an increase in anti-site disorders with doping. Mn 3s x-ray photoemission spectra show an increase in exchange splitting, indicating a decrease in the valency of Mn. The x-ray absorption spectra at Ni and Mn 2p edges show that the formal valence remains 2+ (Ni) and 4+ (Mn) for all the samples, with changes in spectral weights. Ni 2p x-ray photoemission spectra show characteristic feature similar to Ni3+ systems, only for x = 1 sample. Our GGA-based calculations for the ordered supercell, predict half metallic character for doping (x > 0) samples due to delocalization of Ni eg orbitals. The calculations with anti-site disorders yield drastic reduction in Ni moments, with the disordered anti-ferromagnetic phase having lowest energy at maximum doping. Temperature dependent resistivity measurements exhibit a clear metallic region for x = 0.2 sample, while for higher dopings (x > 0.2), the metallicity gets suppressed due to increase in anti-site disorders in these samples.