No Arabic abstract
Ferroelectric and dielectric properties of polydomain (twinned) single-crystal Pb(Zr1-xTix)O3 thin films are described with the aid of a nonlinear thermodynamic theory, which has been developed recently for epitaxial ferroelectric films with dense laminar domain structures. For Pb(Zr1-xTix)O3 (PZT) films with compositions x = 0.9, 0.8, 0.7, 0.6, 0.5, and 0.4, the misfit strain-temperature phase diagrams are calculated and compared with each other. It is found that the equilibrium diagrams of PZT films with x > 0.7 are similar to the diagram of PbTiO3 films. They consist of only four different stability ranges, which correspond to the paraelectric phase, single-domain tetragonal ferroelectric phase, and two pseudo-tetragonal domain patterns. In contrast, at x = 0.4, 0.5, and 0.6, the equilibrium diagram displays a rich variety of stable polarization states, involving at least one monoclinic polydomain state. Using the developed phase diagrams, the mean out-of-plane polarization of a poled PZT film is calculated as a function of the misfit strain and composition. Theoretical results are compared with the measured remanent polarizations of PZT films grown on SrTiO3. Dependence of the out-of-plane dielectric response of PZT films on the misfit strain in the heterostructure is also reported.
A thermodynamic theory is developed for dense laminar domain structures in epitaxial ferrolectric films. It is found that, at some critical misfit strain between the film and substrate, the 90 degrees c/a/c/a domain structure becomes unstable with respect to the appearance of the polarization component parallel to domain walls, which results in the formation of a heterophase structure. For PbTiO_3 and BaTiO_3 films, the stability ranges of polydomain and heterophase states are determined using misfit strain - temperature diagrams. Dielectric anomalies accompanying misfit-strain-driven structural transformations are described.
Ferroelectric switching and nanoscale domain dynamics were investigated using atomic force microscopy on monocrystalline Pb(Zr0.2Ti0.8)O3 thin films. Measurements of domain size versus writing time reveal a two-step domain growth mechanism, in which initial nucleation is followed by radial domain wall motion perpendicular to the polarization direction. The electric field dependence of the domain wall velocity demonstrates that domain wall motion in ferroelectric thin films is a creep process, with the critical exponent mu close to 1. The dimensionality of the films suggests that disorder is at the origin of the observed creep behavior.
The strain dependence of electric and magnetic properties has been widely investigated, both from a fundamental science perspective and an applications point of view. Electromechanical coupling through field-induced polarization rotation (PRO) and polarization reorientation (PRE) in piezoelectric single crystals can provide an effective strain in film/substrate epitaxial heterostructures. However, the specific pathway of PRO and PRE is a complex thermodynamic process, depending on chemical composition, temperature, electric field and mechanical load. Here, systematic studies of the temperature-dependent field-induced phase transitions in Pb(Mg,Nb)O3-PbTiO3 single crystals with different initial phase and orientation configurations have been performed. Different types of strains, volatile/nonvolatile and biaxial/uniaxial, have been measured by both macroscopic and in-situ X-ray diffraction techniques. In addition, the strain state of epitaxial Mn-doped CoFe2O4 thin films was examined by magnetic anisotropy measurements, where a giant magnetoelectric coupling has been demonstrated.
The dielectric properties of NiO thin films grown by pulsed laser deposition have been studied as a function of strain at temperature from 10 to 300 K. Above 150 K, the contribution of space-charge polarization to the dielectric permittivity of NiO films becomes dominant and the more defective films, which were grown at low temperatures show a drastical increase in the dielectric constant up to room temperature. While the atomically-ordered film, which was grown at high temperature doesnt show any considerable change in the dielectric constant in the range from 10 to 300 K. Below 100 K, the effect of strain on the dielectric constant becomes clear. An increase in dielectric permittivity is observed in the strained films while the relaxed film doesnt show any remarkable deviation from its bulk value. The low-temperature dielectric behavior of NiO thin film can be interpreted based on the effect of strain on the lattice dynamics of rocksalt binary oxides.
Metastable manganite perovskites displaying the antiferromagnetic so-called E-phase are predicted to be multiferroic. Due to the need of high-pressures for the synthesis of this phase, this prediction has only been confirmed in bulk HoMnO3. Here we report on the growth and characterization of YbMnO3 perovskite thin films grown under epitaxial strain. Highly-oriented thin films, with thickness down to ~30nm, can be obtained showing magneto-dielectric coupling and magnetic responses as those expected for the E-phase. We observe that the magnetic properties depart from the bulk behavior only in the case of ultrathin films (d< 30nm), which display a glassy magnetic behavior. We show that strain effects alone cannot account for this difference and that the film morphology plays, instead, a crucial role.