Large magnetoelectric response in lead-free (1−x)BCZTO+xMNZGF multiferroic composites

Multiferroic (1- x )Ba 0.83 Ca 0.17 Zr 0.12 Ti 0.88 O 3 + x Mn 0.5 Ni 0.1 Zn 0.4 Gd 0.03 Fe 1.97 O 4 composites [abbreviated as (1− x )BCZTO+ x MNZGF, with x = 0.0, 0.1, 0.2, 0.3, 0.4, 0.5 and 1.0] were fabricated, and their lattice structure, surface morphology, magnetoelectric, dielectric, ferroelectric and magnetic response were thoroughly examined and analyzed. The XRD spectra confirm the simultaneous presence of BCZTO and MNZGF phases in all composites, with no detectable impurity peaks, suggesting a structurally stable system that promotes robust magnetoelectric coupling through enhanced interphase interaction. The Rietveld refined XRD patterns for all compositions obtained goodness-of-fit ( χ 2 ) values close to 2, confirming a high degree of reliability and excellent fitting quality. The composite sample with x = 0.2 demonstrates the lowest porosity among all the studied composites. The FESEM micrographs of the composite samples display two distinctly identifiable grain types, indicating the coexistence of two separate phases with no indication of interphase reactions. The dielectric study reveals that samples containing a higher proportion of the BCZTO phase exhibit increased dielectric constants ( ε' ). Notably, the composite with x = 0.2 demonstrates the largest ac resistivity and the minimum dielectric loss among the investigated composites. The P–E loops of the samples with x > 0.2 become progressively more rounded as ferrite content rises, implying a deterioration in polarization behavior at higher ferrite concentrations. The composite sample with x = 0.2 achieved the largest magnetoelectric voltage coefficient ( α ME ) of 206 mV·cm⁻¹·Oe⁻¹, suggesting its viability for use in versatile technologies, including magnetoelectric sensors, spintronic devices, and energy harvesting systems.