Structural, magnetic and electronic structure studies of NdFe1-xNixO3 (0 ≤ x ≤ 0.3)

We present here the structural, electronic structure, magnetic and Mossbauer studies of NdFe1-xNixO3 (0 <= x <= 0.3) samples. All the samples exhibit a single-phase orthorhombic structure with space group Pbnm. The near-edge x-ray absorption fine structure (NEXAFS) studies reveal that, with the Ni substitution at Fe sites, a new spectral feature about 1.5 eV lower than the pre-edge structure of NdFeO3 in the O K edge is observed due to the 3d contraction effect and is growing monotonically with the increase of Ni concentration. The Fe L-3,L-2, Ni L-3,L-2 and Nd M-5,M-4 edges confirm the trivalent state of Fe, Ni and Nd ions. The Mossbauer spectra fitted with two Zeeman sextets confirm the different surroundings of Ni around Fe ions. With the increase in Ni concentration, the sextets are broadened. The increase of quadrupole splitting and the decrease of the hyperfine field suggest the change in the ordered regime of the system. The magnetic behaviour at low temperatures is explained in the context of competition among moments of rare earth (Nd) and transition metal ions (Fe/Ni). The strong paramagnetic contribution of the Nd magnetic sublattice and spin flip phenomenon is observed from the temperature dependence of zero-field-cooled and field-cooled magnetization where spin crossover is observed. The isothermal hysteresis loops show a decrease of magnetization and increase of coercivity with the increase in temperature and complements magnetization versus temperature. The results are explained on the basis of the spin reorientation phenomenon.