Alexander L. Roytburd

Dielectric properties in heteroepitaxial Ba0.6Sr0.4TiO3 thin films: Effect of internal stresses and dislocation-type defects

A series of heteroepitaxial Ba0.6Sr0.4TiO3 were grown on 0.29(LaAlO3):0.35(Sr2TaAlO6) substrates using pulsed-laser deposition. X-ray characterization revealed compressive in-plane stresses in the thinnest films, which were relaxed in a continuous fashion with increasing thickness. A theoretical treatment of the misfit strain was in good agreement with the measured out-of-plane lattice parameter. The low-frequency dielectric constant was measured to be significantly less than the bulk value and found to decrease rapidly for films less than 100 nm. A thermodynamic model was developed to understand the reduction in dielectric constant. By observing the microstructure using plan-view and cross-section transmission electron microscopy, we identified local strain associated with a threading dislocation density on the order of 1011 cm−2 as a possible mechanism for dielectric degradation in these films.

Thermodynamics of polydomain heterostructures. III. Domain stability map

A map showing regions of stability of possible domain structures and relative fractions of domains in a polytwin structure is developed for epitaxial heterostructures with active layers which undergo a cubic–tetragonal or a tetragonal–orthorhombic transformation. This map, which is also applicable to epitaxial film–substrate systems, shows the dependence of the polytwin structure on misfit strain, lattice parameters of the product phase, and mechanical stress. A uniaxial stress field applied during cooling down from the growth temperature strongly affects the domain structure selection and perfect single-domain structures may be obtained with such fields. For polytwin layers with thicknesses close to the critical thickness for domain formation, microstresses must be taken into consideration and the domain stability map is modified accordingly. Misfit dislocation generation at the deposition temperature is taken into account through a temperature dependent effective substrate lattice parameter. As examples...

Thickness dependence of structural and electrical properties in epitaxial lead zirconate titanate films

We have studied the effect of misfit strain on the microstructure and properties of ferroelectric lead zirconate titanate thin films. We have changed the misfit strain by varying the film thickness and studied the thickness effect on the domain formation of epitaxial PbZr0.2Ti0.8O3 (PZT) films grown by pulsed laser deposition on (001) LaAlO3 substrates with La0.5Sr0.5CoO3 (LSCO) electrodes. The nominal thickness of the PZT films was varied from 60 to 400 nm with the LSCO electrode thickness kept constant at 50 nm. X-ray diffraction experiments show that the films relax via the formation of a domains, the fraction of which increase with the ferroelectric film thickness. The c-axis lattice constant of PZT films calculated from the 002 reflection decreases with increasing film thickness and approaches the bulk value of ∼0.413 nm in the films thicker than 300 nm. Cross-sectional transmission electron microscopy images reveal that the a-domain fraction and period increase with increasing film thickness. The re...

Dielectric anomaly due to electrostatic coupling in ferroelectric-paraelectric bilayers and multilayers

A thermodynamic model is presented that describes the polarization and the dielectric response of ferroelectric-paraelectric bilayers and multilayers. It is shown that a strong electrostatic coupling between the layers results in the suppression of ferroelectricity at a critical paraelectric layer thickness. The bilayer is expected to have a gigantic dielectric response similar to the dielectric anomaly near Curie–Weiss temperature in homogeneous ferroelectrics at this critical thickness. A numerical analysis is carried out for a pseudomorphic (001) BaTiO3∕SrTiO3 heteroepitaxial bilayer on (001) SrTiO3 and a stress-free BaTiO3∕SrTiO3 bilayer. Complete polarization suppression and a dielectric peak are predicted to occur at approximately 66% and 14% of SrTiO3 in these two systems, respectively.

Imaging three-dimensional polarization in epitaxial polydomain ferroelectric thin films

Voltage-modulated scanning force microscopy (Piezoresponse microscopy) is applied to investigate the domain structure in epitaxial PbZr0.2Ti0.8O3 ferroelectric thin films grown on (001) SrTiO3. By monitoring the vertical and lateral differential signals from the photodetector of the atomic force microscope it is possible to separate out and observe the out-of-plane and in-plane polarization vectors in the thin film individually. The relative orientation of the polarization vectors across a 90° domain wall is observed. Nucleation of new reversed 180° domains at the 90° domain wall is studied and its impact on the rotation of polarization within the a domain is analyzed as a function of reversal time.

Dependence of dielectric properties on internal stresses in epitaxial barium strontium titanate thin films

A series of heteroepitaxial BaxSr1−xTiO3 thin films with composition x=0.50 were deposited on (001) MgO substrates by pulsed-laser deposition. The thickness of the films was varied from 14 to 500 nm to produce a systematically decreasing level of in-plane tensile stresses. The microstructural and crystallographic features of the films were determined via transmission electron microscopy and x-ray diffraction. A theoretical treatment of the in-plane misfit strain as a function of film thickness is in agreement with the measured out-of-plane lattice parameters. Electrical measurements indicate a drop in the dielectric constant from 2350 for highly stressed thin films to 1700 for relaxed thicker films. The variation in the dielectric constant with the misfit strain is in accordance with a thermodynamic model developed. The relationship between the dielectric constant and electric field is also described by extending the thermodynamic model and taking the effect of electric field into account. A new definitio...

Elastic domains and polydomain phases in solids

Abstract The discovery of polydomain phases has been one of the fundamental results of the experimental and theoretical studies of solid phase transformations. These phases consist of the alternation of domains: twins of a product phase or layers of different product phases. Elastic interactions between domains lead to the formation of the equilibrium polydomain structure corresponding to the free energy minimum. Thus these domains have been named “elastic domains”. The elastic domains form the polydomain phase whose average properties are dependent on its domain structure. Its basic element is a polytwin: a plane-parallel plate consisting of alternating plane-parallel domains or twins. The crystallographic orientation of the polytwin interfaces and its internal structure are equilibrium characteristics of the phase transition. Thus the parameters of the domain structure are the additional degrees of freedom of a polydomain phase. This fact considerably determines the properties of the polydomain phase, a...

Realizing intrinsic piezoresponse in epitaxial submicron lead zirconate titanate capacitors on Si

We report on the out-of-plane piezoelectric response (d33), measured via piezoresponse scanning force microscopy, of submicron capacitors fabricated from epitaxial PbZrxTi1−xO3 thin films. Investigations on 1 μm2 and smaller capacitors show that the substrate-induced constraint is dramatically reduced by nanostructuring. At zero field, the experimentally measured values of d33 for clamped as well as submicron capacitors are in good agreement with the predictions from thermodynamic theory. The theory also describes very well the field dependence of the piezoresponse of clamped capacitors of key compositions on the tetragonal side of the PbZrxTi1−xO3 phase diagram as well as the behavior of submicron PbZr0.2Ti0.8O3 (hard ferroelectric) capacitors. However, the field-dependent piezoresponse of submicron capacitors in compositions closer to the morphotropic phase boundary (soft ferroelectrics) is different from the behavior predicted by the theoretical calculations.

Role of substrate on the dielectric and piezoelectric behavior of epitaxial lead magnesium niobate-lead titanate relaxor thin films

The effect of various substrates on the electrical and electromechanical properties of 100-nm-thick epitaxial 0.9[Pb(Mg1/3Nb2/3)O3]–0.1[PbTiO3](0.9PMN–0.1PT) thin films is investigated. (001) 0.9PMN–0.1PT films are grown on (001)LaAlO3(LAO), (La, Sr)(Al, Ta)O3(LSAT), SrTiO3(STO), and MgO substrates with 40-nm-thick top and bottom La0.5Sr0.5CoO3 electrodes by pulsed laser deposition. X-ray diffraction results indicate that the films on LAO, LSAT, and STO are stressed biaxially in compression in the film-substrate interface whereas the films on MgO are stressed in tension. A decrease in the temperature of dielectric maximum (Tm) together with an increase in the dielectric constant and the longitudinal piezomodulus is observed with decreasing in-plane epitaxial stresses for LAO, LSAT, and STO substrates. The films on MgO substrates have the highest dielectric constant and piezomodulus with Tm below room temperature. The variation in Tm may be attributed to the shift in the transformation temperature from the...

Self-assembled multiferroic nanostructures in the CoFe2O4-PbTiO3 system

The effect of substrate orientation on the morphologies of epitaxial self-assembled nanostructures was demonstrated using multiferroic 0.67PbTiO3-0.33CoFe2O4 thin films. The two-phase composite films were grown by pulsed laser deposition on single crystal SrTiO3 substrates having (001) and (110) orientations. The nanostructures of both orientations consisted of vertical rod- or platelet-like columns of CoFe2O4 dispersed in a PbTiO3 matrix. For the (001) orientation the platelet habits were parallel to the {110} planes, whereas for the (110) orientation the platelets were parallel to the {111} planes. The differences were explained using a thermodynamic theory of heterophase structures.