We have synthesized piezomagnetic–piezoelectric composites thin films MnFe2O4/(Pb1−xSrx)TiO3, where x=0.1, 0.2, and 0.3, using the metalorganic deposition (MOD) reaction method. The structural and microstructural analysis using the X-ray diffraction (XRD), AFM, and SEM reveals the presence of homogenous growth of both pervoskite and spinel phases in the composite films. Our results show that all the composites films exhibit good multiferroic as well as considerable magnetoelectric coupling. The impedance (Z′ and Z″) and electrical modulus (M′ and M″) Nyquist plots show distinct electrical responses with the magnetic field. Our analyses suggest that this electrical response arises due to the coexistence of the high resistive phase and the comparatively conductive phase in the MFO/PST composite films. The maximum magnetoelectric coefficient (α) is found to be 4.29VOe−1cm−1 and 2.82VOe−1cm−1 for compositions x=0.1 and 0.2. These values are substantially larger than those reported for bilayer composites thin films in literature and make them interesting for room temperature device applications.
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