Multiferroic composite is an environmentally friendly material with the extraordinary multisusceptible and high storage properties. It is significant to find an effective way for designing and fabricating high-quality materials. In this context, the BTO/NZFO nanocrystalline multiferroic composite thin films with and without (100) oriented spinel ferrite were prepared by RF magnetron sputtering. The saturation magnetization, coercivity, and initial susceptibility of composite thin films with (100) oriented spinel NZFO phase are 1.05, 1.75 to 2.08, and 1.15 times as high as those of the composites without orientation, respectively. The dc conductivity and dielectric loss of the composite thin film with (100) oriented NZFO are 18 and 33.3% lower than those of composite without orientation, respectively. It is exhibited that the magnetic and dielectric properties of the BTO/NZFO multiferroic composite thin films are azimuthally controlled by distribution of the Zn/Fe−O−Ni/Fe superexchange coupling and charge hopping between Fe 2+ −Fe 3+ pair, respectively. Obviously, controlling the arrangement of magnetic couplings and charge hopping is an effective route to fabricate the multiferroic composite with the optimal or specific magnetic and dielectric properties.
■ INTRODUCTIONMultiferroic is an excellent environmentally friendly multifunctional material due to its potential applications in novel electronic devices, such as sensors, transducers, and memories with high storage capacity and low cost. 1−5 Recently, to further improve the performance of these devices and relieve the everincreasing pressure on energy and environment, more and more research on improvement of dielectric and magnetic properties of the material has been provoked. 6−18 It is known that the dielectric properties of the dielectrics, such as permittivity and tunability, of the dielectrics can be promoted to be optimal by the azimuthal control of dipoles. 19−21 Other than the common way that improves the dielectric properties through doping and controlling size, 22 the dipole azimuthal control motivates the intrinsic nature to the greatest extent and contributes the high dielectric properties to dielectric materials. Likewise, the magnetic moment of superexchange coupling and the direction of charge hopping in multiferroic also possesses the switchable characteristics. Therefore, it is significant to reveal that azimuthal control mechanism of the magnetic and dielectric properties by magnetic coupling and charge hopping and provide an effective way with distinct physical pictures to make the performance of multiferroic to be optimal.Herein, the multiferroic composite system of BaTiO 3 (BTO) − Ni 0.5 Zn 0.5 Fe 2 O 4 (NZFO) thin film deposited on singlecrystal silicon substrate with (100) and (111) orientation by RF magnetron sputtering is proposed. It is worth noting that BTO/NZFO is a typical multiferroic composite system with good dielectric and magnetic properties. 12−14,23,24 Single-crystal silicon is a chemically stable substrate without interac...