Contribution of space charges to the polarization of ferroelectric superlattices and its effect on dielectric properties

Official URL: http://dx.doi.org/10.1103/PhysRevB.82.094115

A theoretical model is developed for ferroelectric bilayers and multilayer heterostructures that employs a nonlinear Landau-Devonshire formalism coupled with a detailed analysis of the depolarizing fields arising from the polarization mismatch across interlayer interfaces and the electrical fields of localized space charges at such interfaces. We first present how space charges alter the free-energy curves of ferroelectrics and then proceed with a numerical analysis for heteroepitaxial (001) PbTiO3-SrTiO3 (PTO-STO) bilayers and (001) superlattice structures on (001) STO substrates. The switchable (ferroelectric) and nonswitchable (built-in) polarizations and the dielectric properties of PTO-STO bilayers and superlattices are calculated as a function of the planar space-charge density and the volume fraction of the PTO layer. Similar to the temperature dependence of a monolithic ferroelectric, there exists a critical volume fraction PTO below which the bilayer or the superlattice is in the paraelectric state. This critical volume fraction is strongly dependent on the density of trapped charges at the interlayer interfaces. For charge-free (001) PTO-STO heteroepitaxial bilayer and superlattices, the critical fraction is 0.40 for both constructs but increases to 0.6 and 0.72, for the bilayer and the superlattice, respectively, for a planar space-charge density of 0.05 C/m(2). Furthermore, our results show that close to the vicinity of ferroelectric-paraelectric phase transition, there is a recovery in ferroelectric polarization. The dielectric-response calculations verify that there is sharp ferroelectric phase transformation for charge-free bilayers and superlattices whereas it is progressively smeared out with an increase in the charge density. Furthermore, our analysis shows that the dielectric constant of these multilayers at a given volume fraction of PTO decreases significantly in the presence of space charges.