The dielectric behavior of Zn1−xNixO/NiO two-phase composites

Abstract

The effect of nickel content on the dielectric permittivity ‘εr’ and the ac-electrical conductivity of Zn1−xNixO/NiO (0 ≤ x ≤ 0.55) two-phase composites were investigated. The antiferro to the paramagnetic Néel temperature TN (~ 523 K) of the NiO associated with the structural phase transition from the rhombohedral to the cubic phase has been exploited to realize a dielectric anomaly across 523–541 K in the Zn1−xNixO/NiO composite system. Also, a giant dielectric peak across 410 °C in pure NiO was observed together with an anomaly across TN. The formation of tiny polar clusters due to the compositional heterogeneity for the samples with x ≥ 0.16 drove the system to exhibit a weakly coupled relaxor-like behavior with a locally varying maximum temperature of T* (~ 530 K at 106 Hz), obeying the Vogel–Fulcher law and the Uchino–Nomura criteria. The values of the diffuseness-exponent ‘γ’ (1.91) and the shape-parameter ‘δ’ (88 °C) were determined by using the empirical scaling relation (εA/εr = 1 + 0.5 (T − TA)2/ δ2), which is often used to describe relaxor-like behavior. Our results provide strong evidence for the variable-range-hopping of charge carriers between the localized states. The effects of non-ohmic sample-electrode contact impedance and negative-capacitance on the global dielectric behavior of a Zn1−xNixO/NiO composite system are discussed.