Dielectric loss, conductivity relaxation process and magnetic properties of Mg substituted Ni–Cu ferrites

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Abstract

The dielectric properties, dc and ac electrical resistivities of Mg substituted Ni–Cu ferrites with general formula Ni0.5Cu0.5−xMgxFe2O4 (0.0≤x≤0.5) have been investigated as a function of frequency, temperature and composition. ac resistivity of all the samples decreases with increase in the frequency exhibiting normal ferrimagnetic behavior. The frequency dependence of dielectric loss tangent showed a maximum in between 10 Hz and 1 kHz in all the ferrites. The conductivity relaxation of the charge carriers was examined using the electrical modulus formulism, and the results indicate the presence of the non-Debye type of relaxation in the prepared ferrites. Similar values of activation energies for dc conduction and for conductivity relaxation reveal that the mechanism of electrical conduction and dielectric polarization is the same in these ferrites. A single ‘master curve’ for normalized plots of all the modulus isotherms observed for a given composition indicates that the distribution of relaxation time is temperature independent. The saturation magnetization and coercivity as calculated from the hysteresis loop measurement show striking dependence on composition.

Highlights

► The crystalline size as well as the lattice parameter of the Ni–Cu ferrites increases with Mg2+ ion content. ► Similar values of activation energies for dc conduction and for conductivity relaxation reveal that the mechanism of electrical conduction and dielectric polarization is the same in these ferrites. ► A single ‘master curve’ for normalized plots of all the modulus isotherms observed for a given composition indicates that the distribution of relaxation time is temperature independent. ► Saturation magnetization first increases with Mg composition and then decreases. ► Coercivity values are found to decrease with the substitution of Mg in Ni–Cu ferrite.

Introduction

Spinel ferrites with general formulae AB2O4 are the most important materials for fundamental as well as for applied research point of view due to their high electrical resistivity and sufficient low dielectric losses [1], [2], [3]. Polycrystalline ferrites are supposed to be very good dielectric materials with low conductivity and have a wide field of technological applications in the range from microwave to radio wave frequencies [4], [5], [6], [7]. The distribution of cations over tetrahedral and octahedral sites in ferrites has a remarkable effect on the electrical and magnetic behavior [8], [9], [10], [11]. Spinel ferrites have been shown to exhibit interesting dielectric and magnetic properties in the nanocrystalline form compared with those of bulk form, because the cation distribution is distinctly different in ferrite nanoparticles compared with the bulk ferrites [12], [13]. The physical properties of ferrites are also dependent on synthesis technique, chemical composition, the quantity and type of additives [14], [15], [16]. Interesting results have been reported on the electrical and magnetic behavior of Ni–Cu ferrites substituted with different metal ions such as Zn, Al and Co [9], [17], [18]. All these factors play a major role in deciding the overall electrical properties of the ferrites. The sol–gel auto-combustion synthesis [19] provides an easy alternative for the preparation of nano-size particles that require low annealing temperature. Therefore, in the present work Mg substituted Ni–Cu ferrites of different compositions prepared by the sol–gel technique for the first time have been reported. Further, the electrical and magnetic properties of Ni–Cu ferrites have been studied as a function of Mg2+ ions concentration for widening its range of applications. A detailed investigation on the transport properties of the ferrites belonging to a series of type Ni0.5Cu0.5−xMgxFe2O4 can throw light on the mechanism of electric conduction studied over a wide range of frequencies.

Section snippets

Experimental

Ferrite samples with the chemical formula Ni0.5Cu0.5−xMgxFe2O4 (0.0≤x≤0.5) were prepared by the sol–gel auto-combustion technique. The chemicals used for their synthesis were analytical grade ferric nitrate, nickel nitrate, copper nitrate, magnesium nitrate and citric acid. Deionized water was used to form a sol of the chemical reagents and the ratio of metal nitrates to citric acid was 1:1 (mol%). The pH of the sol was adjusted at 7 using ammonia solution. The sol was heated for 4–5 h with

XRD analysis

The X-ray diffraction patterns of Ni0.5Cu0.5−xMgxFe2O4 ferrites annealed at 1073 K are shown in Fig. 1. The XRD patterns reveal that the annealed ferrites are of spinel structure and there is no extra phase in the structure [22], [23]. The average crystalline size is calculated from the most intense peak, i.e., (311) peak, using the Scherrer formulaD=kλ/(βcosθ)where D is the average crystalline size, k is a constant, λ is the X-ray wavelength, β is the full width at half maximum of the most

Conclusions

The crystalline size (D) as well as the lattice parameter (a) of the present Ni–Cu ferrites increases with Mg2+ ion content. Dielectric loss (tan δ) decreases with the frequency of external electric field and increase with temperature. Magnesium substitution increases the loss tan δ even at very low frequency in Ni–Cu ferrites. Resistivity is found to decrease slowly at low frequency and abruptly at high frequency due to hopping of electrons in Fe2+ –Fe3+ ion pairs. The linear variation of dc

Acknowledgments

Authors are thankful to CSIR and DST (FIST scheme), New Delhi for providing financial support.

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