The observation of strong magnetoelectric (ME) coupling is reported in zinc-substituted layered composites of ferrites and lead zirconate titanate (PZT). Multilayer samples contained cobalt zinc ferrite ${\mathrm{Co}}_{1-x}{\mathrm{Zn}}_x{\mathrm{Fe}}_2{\mathrm{O}}_4$ (CZFO) $(x=0\mathrm{}–0.6)$ or nickel zinc ferrite ${\mathrm{Ni}}_{1-x}{\mathrm{Zn}}_x{\mathrm{Fe}}_2{\mathrm{O}}_4$ (NZFO) $(x=0\mathrm{}–0.5)$ and were prepared by laminating and sintering ferrite and PZT thick films obtained by tape casting. The ME voltage coefficient ${\alpha }_E$ was measured for transverse and longitudinal field orientations for frequencies 10–1000 Hz. A substantial enhancement in ${\alpha }_E$ is observed with the substitution of Zn. The largest increase, by about 500%, is observed in CZFO-PZT and the smallest increase of 60% is measured for NZFO-PZT. As the Zn concentration is increased, ${\alpha }_E$ increases and shows a maximum for $x=0.2\mathrm{}–0.4,$ depending on the ferrite. The data is analyzed based on a theoretical model for a ferrite-PZT bilayer, taking into consideration less than ideal coupling at the interface. The interface coupling parameter k is quite small for CZFO-PZT; it increases from 0 to 0.6 as Zn concentration is increased from 0% to 40%. Composites of NZFO-PZT, however, have a near perfect interface coupling. The Zn-assisted enhancement in the ME coefficient is discussed in terms of joule magnetostriction, initial permeability, and magnetomechanical coupling for the ferrites.

• Received 26 February 2002

DOI:https://doi.org/10.1103/PhysRevB.67.014418