Unraveling Multiferroic Properties and Phase Stability of Bismuth Ferrite (BiFeO₃)–Calcium Titanate (CaTiO₃) Solid Solution Ceramics Synthesized via the Flux‐Assisted Preparative Route

Bismuth ferrite (BiFeO 3 , BFO) is a classical multiferroic compound associated with high leakage current density, low resistivity, and instability to obtain the pure phase of this material, which limits its practical applicability. To improve BFO's structural stability, dielectric and magnetic properties combined with calcium titanate (CaTiO 3 , CTO), a lead‐free material, exhibit high dielectric constant with improved multiferroic properties of BFO. This work describes the solid solution formation of (1‐ x )BFO– x CTO (0.1 ≤ x ≤ 0.4) ceramics using a low‐temperature NaCl‐based molten salt synthesis route. X‐ray diffraction patterns reveal a distorted rhombohedral perovskite structure of pure BFO phase at lower CTO compositions, merging diffraction peaks (1 0 4) and (1 1 0) as CTO content increases. Field‐emission scanning electron microscope micrographs show uniform granular‐shaped morphology of these substitutional BFO ceramics. Interestingly, the 0.6BFO–0.4CTO composition exhibits a higher dielectric constant (~ 162) and low loss tangent factor (≈0.09) at 300 K. M–H hysteresis curves display saturated loops for all samples, with 0.8BFO–0.2CTO composition achieving 2M s of ≈8.2 emu gm −1 , attributed to increased spin canting due to higher surface‐to‐volume ratio of BFO nanoparticles. These findings provide insight into the structure–property correlation phenomenon, making the BFO–CTO solid solutions promising for capacitors and magnetic random access memory storage device applications.