Ferromagnetic, ferroelectric, and magnetoelectric properties in individual nanotube-based magnetoelectric films of CoFe2O4/BaTiO3 using electrically resistive core-shell magnetostrictive nanoparticles

Abstract Since 2010, two-phase magnetoelectric (ME) films consisting of magnetostrictive and piezoelectric phases have been continuously developed with regard to their promising ME responses, for potential applications such as ultra-sensitive magnetic sensing, magnetic-field induced energy harvesting, and nano-transduction. Generally, one-dimensional piezoelectric nanowires, nanorods, and nanotubes are used to enlarge the active area for strain transfer between the piezoelectric and magnetostrictive phases of ME films. In this study, we developed 1–2 type individual nanotube-based ME films of CoFe2O4/BaTiO3 with main considerations in the optimization of magnetostrictive phase, piezoelectric phase, and interface between the phases, respectively. First, core-shell magnetostrictive nanoparticles were improved with a high resistivity of 3.89 MΩ·cm and saturation magnetization of 20.8 emu/g via a sufficient TiO2 coating on the CoFe2O4 nanoparticles. Then, individually free-standing TiOx nanotubes were prepared with an optimal structure exhibiting a large pore size of 220 nm and high interspace distance of 80 nm. Final 1–2 type ME films of CoFe2O4/BaTiO3 were successfully prepared by magnetostrictive particle electrodeposition and perovskite conversion in sequence. Enhanced dipole moments through high amounts of BaTiO3 phase were achieved with a maximal remnant polarization (Pr) of 0.192 µC/cm2 from the AC-electrodeposited (AC-) ME films exhibiting a dense film structure. Maximal ME coefficient of the AC-ME films was achieved with magnitude of 27.39 mV/cm∙Oe at Hbias = 1000 Oe. As a result, considering the investigations, the 1–2 type ME films could be expected for possible applications such as high-sensitive magnetic sensors or low-power energy harvesters.