Thin Solid Films, Vol.330, No.2, 183-189, 1998
Thickness dependence of structural and ferroelectric properties of sol-gel Pb(Zr0.56Ti0.44)(0.90)(Mg1/3Nb2/3)(0.10)O-3 films
Sol-gel Pb(Zr0.56Ti0.44)(0.90)(Mg1/3Nb2/3)(0.10)O-3 (PZT-PMN) films were prepared onto the Ti/Pt/Ti bottom electrode by multilayer spin coating. The film thickness ranged from 0.22 to 0.88 mu m The Pt top electrodes were deposited on the PZT-PMN films by DC sputtering. The structural and ferroelectric properties of PZT-PMN films were investigated as a function of film thickness by X-ray diffraction (XRD), scanning electron microscopy (SEM), cross-sectional transmission electron microscopy (XTEM), and by measuring the relative permittivity. The film retains the tetragonal perovskite structure with the [111] and [100] preferred orientations perpendicular to the film surface independent of film thickness. The [100] texture increases with increasing film thickness although the [111] texture is always predominant. The film consists of columnar grains. The average grain size is nearly independent of film thickness. The surface layer containing fine grains about 30 nm in diameter is induced on the top of the film. As the film thickness exceeds 0.44 mu m, the number of the fine grains decreases remarkably. The crystalline interface layer about 10 nm thick is formed between the film and the bottom electrode. This interface layer is composed of Pt, Pb, Zr, Ti and O, while it is rich in Ti and deficient in Pb and O as compared with the inside of the film. The measured relative permittivity of the film increases with increasing film thickness, following the low permittivity interface model. On the basis of this model, the relative permittivity is estimated to be 3200 for the intrinsic PZT-PMN film, 750 for the surface layer and 50 for the interface layer.