Evidence of self-biased magnetoelectric coupling in eco-friendly (Na0.41K0.09Bi0.5TiO3-Ba0.85Ca0.15Zr0.1Ti0.9O3)-(CoFe2O4) particulate composites

The magnetoelectric (ME) properties of eco-friendly 1-x(0.94Na0.41K0.09Bi0.5TiO3-0.06Ba0.85Ca0.15Zr0.1Ti0.9O3)-x (CoFe2O4) (NKBCZT-CFO) with x = 0, 0.1, 0.2, 0.3 and 0.4 particulate composites were investigated. The X-ray diffraction studies provided evidence for the simultaneous existence of constituent phases (ferroelectric and ferromagnetic) in the composite. The structural and surface morphology analysis of the composite affirmed the homogeneous and densely packed distribution of CFO grains within the NKBCZT matrix. The composite's multiferroic behavior at room temperature was confirmed through the characterization of P vs E and M vs H hysteresis loops. The observed values of remnant polarization (Pr) and coercive field (Ec) are 26.7 μC/cm2 and 35.5 kV/cm, respectively, for 10 mol% of CFO. The increase in CFO content resulted in a decrease in the ferroelectric properties, possibly due to the conductive behaviour exhibited by CFO, and correlated with leakage current measurement. For the composite containing 40 mol% of CFO, the estimated values of remanent (Mr), saturation (Ms) magnetization, coercive field (Hc), and magnetic moment (µB) are 2.35 emu/g, 21.85 emu/g, 104.2 Oe, and 0.86 µB, respectively. The non-Debye type dielectric relaxation processes have been observed in the composites, and the electron hopping mechanism resulted in a higher dielectric constant (εʹ). Enhancement in relaxor nature had been observed through Vogel-Fulcher analysis with CFO content. The evidence of ME coupling was revealed through the direct ME voltage coefficient (αME) and magnetocapacitance (MC) measurement. The observed maximum value of MC measured at 1 kHz for the 20 mol% CFO is ∼5.6 %. Self-biased ME coupling (non-zero αME at HDC = 0 Oe) was observed in 20 and 30 mol% of CFO composite. The highest measured value of αME for 20 and 30 mol% CFO is 3.63 mV/cm.Oe and 4.09 mV/cm.Oe at HDC = 0 Oe respectively. The strong ME interaction and significant value of self-biased ME αME suggest that these composites can be explored for magnetic sensor and ME memory device applications.