In this research work, the room-temperature multiferroic behavior resulting from the inclusion of transition metal ions (Ni2+ and Fe3+) in lead-free \({Ba}_{0.7}{Sr}_{0.3}Ti{O}_{3}\) [ \({Ba}_{0.7}{Sr}_{0.3}({Fe}_{x/2}{Ni}_{x/2}){Ti}_{1-x}{O}_{3}; x = 0.00, 0.01, 0.03, 0.05, 0.07\) ] ceramics synthesized via the solid-state reaction (SSR) technique has been extensively examined. The study consistently investigated the structural, ferroelectric, dielectric, magnetic, and magnetodielectric properties with the increasing co-doping content of transition metal ions. The X-ray diffraction (XRD) results for all ceramic compositions clearly showed the development of a single-phase crystalline structure exhibiting P4mm space group symmetry. The Raman investigation confirmed the existence of multiple modes, all of which are related to the presence of the single phase, thus providing robust confirmation for the X-ray diffraction findings. SEM micrographs demonstrate that the incorporation of transition metal ions leads to a reduction in grain size. The frequency-reliant dielectric properties were illustrated across a frequency range from 103 to 106 Hz. The hysteresis curves for polarization vs. electric field (P–E) consistently depict a decrease in both Ps and Pr values, while the magnetization (M–H) hysteresis curve indicates an enhancement in the magnetic properties as doping levels increase. The magnetodielectric (MD) analysis validated the coupling between ferromagnetic and ferroelectric ordering. The BST-1FN sample demonstrated the most significant MC % value of 1.82% and a magnetoelectric coupling coefficient \({\prime}\gamma {\prime}\) of \(-3.64\times {10}^{-1}{(memu/g)}^{-2}\) , establishing it as a promising contender for the development of cutting-edge non-volatile multiferroic memory devices.
