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Local electrical conduction behaviors of polycrystalline La-doped BiFeO3 thin films have been investigated by combining conductive atomic force microscopy and piezoelectric force microscopy. Nanoscale current measurements were performed as a function of bias voltage for different crystal grains. Completely distinct conducting processes and resistive switching effects were observed in the grain boundary and grain interior. We have revealed that local electric conduction in a grain is dominated by both the grain boundary and ferroelectric domain, and is closely related to the applied electric field and the as-grown state of the grain. At lower voltages the electrical conduction is dominated by the grain boundary and is associated with the redistribution of oxygen vacancies in the grain boundary under external electric fields. At higher voltages both the grain boundary and ferroelectric domain are responsible for the electrical conduction of grains, and the electrical conduction gradually extends from the grain boundary into the grain interior due to the extension of the ferroelectric domain towards the grain interior. We have also demonstrated that the conduction dominated by the grain boundary exhibits a much small switching voltage, while the conduction of the ferroelectric domain causes a much high switching voltage in the grain interior.

The heterostructural film combining multiferroic CoFe2O4/Pb(Zr0.52Ti0.48)O3 bilayer with semiconductor ZnO layer was prepared. Three-state resistive switching was demonstrated by time-dependent current measurements under different stimuli combination of voltage pulse and magnetic bias. The asymmetry diodelike current-voltage, capacitance-voltage, and polarization-voltage loops, which seriously depend on magnetic bias, were observed. We revealed that three-state resistive switching was dominated by the changes in the charge carriers in the heterostructure, which were modulated by the magnetoelectric coupling between ferromagnetic and ferroelectric layers and interface polarization coupling between ferroelectric and semiconductor layers. This work provides promising candidates for developing advanced switchable devices with multifunctional memory.

Graded particulate composite films in which ferromagnetic CoFe 2 O 4 nanoparticles are gradedly distributed in the ferroelectric Pb(Zr 0.52 Ti 0.48 )O 3 matrix along the thickness direction have been prepared on Pt/Ti/SiO 2 /Si wafers via sol-gel spincoating method and rapid annealing process. Compared with the homogenous films, the graded ones not only exhibited magnetic anisotropy, but also showed evident increase in both ferroelectric polarization and dielectric tunability. Moreover, great enhancement of magnetodielectric effect was observed in such graded films. We elucidated the origin of enhanced magnetodielectric coupling and attributed it to the combined influence of two factors, that is, the enhanced ferroelectric polarization caused by CoFe 2 O 4 distribution gradient and flexoelectric polarization induced by strain gradient under external magnetic field. This work presents a feasible way to modulate the magnetoelectric coupling in ferromagnetic-ferroelectric composite films for developing high-performance multiferroic materials at nanoscale.

Multiferroic La-doped BiFeO3 thin films have been prepared by a sol-gel plus spin-coating process, and the local magnetoelectric coupling effect has been investigated by the magnetic-field-assisted scanning probe microscopy connected with a ferroelectric analyzer. The local ferroelectric polarization response to external magnetic fields is observed and a so-called optimized magnetic field of ~40 Oe is obtained, at which the ferroelectric polarization reaches the maximum. Moreover, we carry out the magnetic-field-dependent surface conductivity measurements and illustrate the origin of local magnetoresistance in the La-doped BiFeO3 thin films, which is closely related to the local ferroelectric polarization response to external magnetic fields. This work not only provides a useful technique to characterize the local magnetoelectric coupling for a wide range of multiferroic materials but also is significant for deeply understanding the local multiferroic behaviors in the BiFeO3-based systems.