Role of ferroelectric/ferromagnetic layers on the ferroelectric properties of magnetoelectric composite films derived by chemical solution deposition

Highlights: • Multiferroic composite films with different components were prepared. • Individual layer effect on the properties of composite films was studied. • BTO-CFO film shows bigger ferroelectric polarization than BTO-BFO film. • Leakage current curves show BTO-CFO film has the smallest leakage current. • Leakage current is dominated by the space-charges-limited mechanisms. - Abstract: Composite thin films with BiFeO₃ (BFO), CoFeO₄ (CFO) and/or BaTiO₃ (BTO) layers as the components are fabricated via CSD method. XRD and Raman patterns show all the composite films can be indexed to perovskite and spinel structures. Except the interfaces between BTO and CFO layers, the other two-phase interfaces can be clearly observed. Interestingly, the BTO-CFO film has bigger polarization than BTO-BFO, especially the thickness of CFO layer is smaller than the BFO layer, implying the ferromagnetic layer has a significant impact on the ferroelectric properties of the composite films, which is too thin to be fully polarized. The variation of leakage currents show BTO-CFO film has the smallest value, corroborating the results of ferroelectric measurements. The leakage current is dominated by the space-charges-limited mechanisms according to the fitting results, and the oxygen vacancies in the BFO layers play an important role for the variations of E_SCL and E_TFL voltages.