Abstract

Adding functionalities to existing ferroelectric/ferromagnetic materials showed promising results with exciting physical mechanisms. Pure and bilayer films of strong ferromagnetic oxides, viz, BaFe12O19 (BaM) and La0.67Sr0.33MnO3 (LSMO), were fabricated by pulsed laser deposition. Polycrystalline samples of dense structure, uniform thickness, and monodispersed grain distributions were used to form capacitor-like stack geometry for dielectric and magneto-dielectric (MD) measurements. High dielectric constants at moderately high frequencies with increased relaxation times were observed for the bilayer film and are attributed to the BaM/LSMO strained interface, while Maxwell–Wagner polarization plays an insignificant role. Modeling of dielectric loss tangents and AC conductivity revealed localized carrier hopping between Fe ions in the bilayer film. Pronounced hysteresis loops with a small coercive field and increased saturation magnetization values of BaM/LSMO bilayers, as compared with BaM/Pt, are demonstrated at 300 K; where the role of mixed valence Mn ions in +3 and +4 states at the bottom LSMO electrode is highlighted. MD measurements with varying magnetic fields showed magnetically tunable, large MD coupling values (∼287%) for BaM/LSMO/Pt. The phenomenally high MD values are discussed based on ionic polarization, colossal magnetoresistance of LSMO, and magnetostriction at the BaM/LSMO interface. Our findings propose significant applications of ferromagnetic oxide bilayers in the emerging field of magneto-dielectric coupling devices.

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