Optimization of magneto-electric properties in lead-free (x)Co1.2Ti0.2Fe1.6O4 - (100-x)BaTiO3 based composites

This work presents a systematic study of lead-free multiferroic composites of (x)Co1.2Ti0.2Fe1.6O4 - (100-x)BaTiO3 (x = 10, 20, 30), which were synthesized by a solid-state reaction method to investigate the effects of composition and sintering temperature on their structural , electrical, magnetic, and magnetoelectric (ME) properties. X-ray diffraction along with Rietveld refinement confirms the coexistence of tetragonal BaTiO3 (BTO) and cubic spinel Co1.2Ti0.2Fe1.6O4 (CTFO) phases. Microstructural analysis shows that densification and grain growth are better at higher sintering temperatures, leading to better coupling between the two phases. Dielectric and ferroelectric studies indicate lossy polarization-electric field (P-E) behaviour due to leakage from the conductive phase, while magnetic properties show increased magnetization with increasing ferrite content. All composites exhibit ME coefficients, which depend on the composition and sintering conditions; the highest ME coefficient (~1.28 mV/cm.Oe) was observed for the 30CTFO - 70BTO composite sintered at 1200 °C. This improvement is due to the optimal balance between magnetostrictive and piezoelectric responses and improved interfacial strain transfer. These results demonstrate that simultaneous optimization of dopant-modified composition and sintering conditions is essential for achieving improved magnetoelectric coupling in bulk multiferroic composites. Moreover, the results demonstrate the potential of lead-free composites for multifunctional device applications in next-generation, low-power technologies, including high-density non-volatile memory (e.g. FeRAM/MRAM), magnetic field sensors, spintronic devices, and actuators.