Multiferroic composite structures, i.e., composites of magnetostrictive and piezoelectric materials, can be envisioned to achieve the goal of strong room-temperature ME coupling for real practical device applications. Magnetic materials with high magnetostriction, high Néel temperature (T_N), high resistivity and large magnetization are required to observe high ME coupling in composite structures. In continuation of our investigations on suitable magnetic candidates for multiferroic composite structures, we have studied the crystal structure, dielectric, transport, and magnetic properties of Co_0.65Zn_0.35Fe₂O₄ (CZFO). Rietveld refinement of X-ray diffraction patterns confirms the phase purity with a cubic crystal structure with the (Fd3[combining macron]m) space group; however, we have found a surprisingly large magneto-dielectric anomaly at the Néel temperature, unexpected for a cubic structure. The presence of mixed valences of Fe²⁺/Fe³⁺ cations is probed by X-ray photoelectron spectroscopy (XPS), which supports the catonic ordering-mediated large dielectric response. Large dielectric permittivity dispersion with a broad anomaly is observed in the vicinity of the magnetic phase transition temperature (T_N) of CZFO suggesting a strong correlation between dielectric and magnetic properties. The evidence of strong spin-polaron coupling has been established from temperature dependent dielectric, ac conductivity and magnetization studies. The ferrimagnetic-paramagnetic phase transition of CZFO has been found at ∼640 K, which is well above room temperature. CZFO exhibits low loss tangent, a high dielectric constant, large magnetization with soft magnetic behavior and magnetodielectric coupling above room temperature, elucidating the possible potential candidates for multiferroic composite structures as well as for multifunctional and spintronics device applications.

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