Multiferroic response and conductivity features in CoFe2O4/65BiFeO3-35PbTiO3 heterostructure composite thin films

Magnetoelectric composite materials, which exhibit both ferroelectric and ferromagnetic properties simultaneously, have attracted considerable interest for their potential in various applications such as microelectronics, memory devices, and spintronics. In this study, we investigated the synthesis, structural, morphological, electrical, and magnetic properties of multiferroic CoFe 2 O 4 /0.65BiFeO 3 -0.35PbTiO 3 (CFO/65BF-35PT) composite thin films. These films were prepared using a high ferroelectric, morphotropic phase boundary (MPB) composition, 65BF-35PT, combined with a high magnetostrictive compound, CFO. Multilayered CFO/65BF-35PT composite films were spin-coated onto fluorine-doped tin oxide (FTO)/glass substrates using the sol-gel method, with variation in the solution molarity to achieve different layer thicknesses. Structural analysis revealed a perovskite phase for 65BF-35PT and a spinal structure for CFO, with the presence of rhombohedral and tetragonal polymorphs confirming MPB composition. Scanning electron microscope images demonstrated uniform growth of 1 μm thick composite films. Ferroelectric hysteresis loops exhibited considerable leakage current at room temperature, increasing with higher CFO content, while current versus voltage plots revealed ohmic conduction at low applied fields and space charge limited current (SCLC) conduction at high fields in all composite films. The crossover field between ohmic and SCLC conduction decreased with increasing CFO content. Moreover, room-temperature magnetic hysteresis loops showed a decrease in saturation and coercive field with increasing CFO concentration, and the temperature-dependent magnetization response indicated a monotonic decrease, with magnetization vanishing around 800 K, confirming the magnetic order of CFO. Our findings demonstrate that stable ferroelectric and ferromagnetic phases can be achieved at low temperatures by depositing composite films containing CFO/MPB on a low-cost FTO substrate.