Magnetic-Field-Dependent Raman Scattering in Multiferroic Bilayer Films: Evidence for Stress-Mediated Magnetoelectric Coupling

We report the first magnetic-field-dependent Raman scattering studies on Pb(Zr,Ti)O3-CoFe2O4 bilayer multiferroic system. The phonon frequencies of the nano-bilayers obviously change with magnetic field, which is absent in the single Pb(Zr,Ti)O3 films. The magnetostriction of the CoFe2O4 layer generates stress mechanically transferred to the Pb(Zr,Ti)O3 layer, resulting in the mode changes. The observed magnetic-field-induced softening of the soft mode in the Pb(Zr,Ti)O3 layer bears a striking resemblance to direct magnetoelectric output in the bilayers, providing evidence for stress-mediated magnetoelectric coupling mechanism in the multiferroic bi-layers.