Very large dielectric response from ferroelectric nanocapacitor films due to collective surface and strain relaxation effects

Official URL: http://dx.doi.org/10.1063/1.4831939

Dependence of the dielectric response of ferroelectrics on defect types, particularly those with long range strain fields in confined geometries have been often mentioned, especially in interpreting experimental results in films. However, detailed discussions on the mechanisms with which defects alter properties, particularly in the presence of interfaces imposing certain boundary conditions, are seldom made. Here, we studied the thickness dependence of transition temperatures and dielectric response of Metal/BaTiO3/Metal ferroelectric nanocapacitor structures grown on SrTiO3 using a phenomenological approach accounting for the equations of electrostatics and semiconductors. Relaxation of the misfit strain via misfit dislocations amplify the surface effects in films below a critical thickness and favor electrical domains leading to very large dielectric responses in this regime. Thin film structures with relaxed misfit strain in this work are fully-depleted in the presence of moderate densities of impurities (~1025 m-3). This is due to the reduction of polarization amplitude parallel to the film normal and its mplications for near-micron thick films are discussed. Consequently, the misfit dislocation sites have nearly no free carrier localization, making the role of these sites on leakage currents highly questionable. Dielectric response of intrinsic thicker films (>40 nm) are mostly under the influence of strain relaxation only with minimal interface impact in the limit of ideal electrodes. Our results point out that control of the dislocation density can lead to non-conventional functionalities in ferroelectric thin film capacitors via electromechanical coupling of properties to structure and domain stabilization.