Magnetic ground state and crystal structure of the giant dielectric constant material Ba(Fe1/2Nb1/2)O3

Abstract

The room temperature crystal structure as well as the magnetic ground state of Ba(Fe1/2Nb1/2)O3 (BFN) are controversial. The results of Rietveld refinements using high-resolution synchrotron x-ray powder diffraction (SXRPD) data are presented to show that BFN belongs to cubic perovskite structure in the Pm3¯m space group and not in the cubic Fm3¯m or monoclinic symmetries, proposed by some earlier workers based on the analysis of the laboratory source XRD data. The temperature dependent specific heat measurements in the 1.8 to 300 K range on well characterized BFN samples are presented to show the absence of any long-range ordered (LRO) antiferromagnetic (AFM) transition, proposed by some earlier workers based on the observation of a peak in the temperature dependence of zero-field cooled (ZFC) DC magnetization around 25 to 32 K. Results of temperature dependent magnetization measurements during warming cycle on ZFC and field cooled (FC) BFN samples reveal history dependent bifurcation with a peak in the ZFC M (T) curve at Tf ~ 29 K, in agreement with some previous results where it was attributed to a spin-glass transition even though such an irreversibility can result from superparamagnetic (SPM) blocking as well. The appearance of a short plateau in our FC M (T) curve below Tf suggests a cluster spin-glass phase of BFN below Tf. This was confirmed by us through the ac susceptibility χ' (T, ω) studies which reveal divergence of spin dynamics at the spin-glass transition temperature TSG ~ (28 ± 1) K with a large characteristic spin relaxation time τ0 ~ 10−6 s following Vogel-Fulcher as well as power-law type critical dynamics. The existence of the magnetic glassy state in BFN is further supported by the observation of (1) magnetic field dependent shift of Tf with increasing magnetic field along the de Almeida-Thouless line in the T-H plane with a characteristic exponent of m = 2/3, (2) weak remanent magnetization Mr below Tf with exponentially decreasing Mr on approaching Tf, (3) extremely slow decay of the thermoremanent magnetization below Tf with time as per a stretched exponential function, and (4) characteristic aging, rejuvenation and memory effects below Tf. These results provide the first unambiguous confirmation of the cluster spin-glass state of BFN and settle the existing controversies related to its magnetic ground state.