J. M. Gregg

Dielectric enhancement and Maxwell–Wagner effects in ferroelectric superlattice structures

In an attempt to reproduce the functional properties associated with relaxor electroceramics, pulsed laser deposition has been used to fabricate thin-film capacitor structures in which the dielectric layer is composed of a superlattice of Ba0.8Sr0.2TiO3 and Ba0.2Sr0.8TiO3. The properties of the capacitors were investigated as a function of superlattice periodicity. The dielectric constant was significantly enhanced at stacking periodicities of a few unit cells, consistent with relaxor behavior. However, enhancement in dielectric constant was generally associated with high dielectric loss. Analysis of the imaginary permittivity as a function of frequency shows that fine-scale superlattices conform to Maxwell–Wagner behavior. This suggests that the observed enhancement of the real part of the dielectric constant is an artifact produced by carrier migration to interfaces within the dielectric. A comparison of this data with that already published on dielectric superlattices suggests that previous claims of a...

Strain gradients in epitaxial ferroelectrics

X-ray analysis of ferroelectric thin layers of Ba1/2Sr1/2TiO3 with different thicknesses reveals the presence of strain gradients across the films and allows us to propose a functional form for the internal strain profile. We use this to calculate the influence of strain gradient, through flexoelectric coupling, on the degradation of the ferroelectric properties of films with decreasing thickness, in excellent agreement with the observed behavior. This paper shows that strain relaxation can lead to smooth, continuous gradients across hundreds of nanometers, and it highlights the pressing need to avoid such strain gradients in order to obtain ferroelectric films with bulklike properties.

The effect of flexoelectricity on the dielectric properties of inhomogeneously strained ferroelectric thin films

Recent experimental measurements of large flexoelectric coefficients in ferroelectric ceramics suggest that strain gradients can affect the polarization and permittivity behaviour of inhomogeneously strained ferroelectrics. Here we present a phenomenological model of the effect of flexoelectricity on the dielectric constant, polarization, Curie temperature (TC), temperature of maximum dielectric constant (Tm) and temperature of the onset of reversible polarization (Tferro) for ferroelectric thin films subject to substrate-induced epitaxial strains that are allowed to relax with thickness, and the qualitative and quantitative predictions of the model are compared with experimental results for (Ba0.5Sr0.5)TiO3 thin films on SrRuO3 electrodes. It is shown that flexoelectricity can play an important role in decreasing the maximum dielectric constant of ferroelectric thin films under inhomogeneous in-plane strain, regardless of the sign of the strain gradient.

Relaxor features in ferroelectric superlattices: A Maxwell–Wagner approach

A Maxwell–Wagner series capacitor model is proposed to explain anomalous dielectric properties of ferroelectric superlattices. The results of the model show that a superlattice consisting of normal ferroelectric layers separated by low-resistivity interfacial regions can account for most experimental results reported to date, namely: dielectric enhancement for certain stacking periodicities, giant permittivities, and temperature migration of dielectric maxima as a function of frequency. The predictions of the model are discussed and compared to our own experimental results from thin film superlattice capacitors made by pulsed-laser deposition.

Magnetic switching of ferroelectric domains at room temperature in multiferroic PZTFT

Single-phase magnetoelectric multiferroics are ferroelectric materials that display some form of magnetism. In addition, magnetic and ferroelectric order parameters are not independent of one another. Thus, the application of either an electric or magnetic field simultaneously alters both the electrical dipole configuration and the magnetic state of the material. The technological possibilities that could arise from magnetoelectric multiferroics are considerable and a range of functional devices has already been envisioned. Realising these devices, however, requires coupling effects to be significant and to occur at room temperature. Although such characteristics can be created in piezoelectric-magnetostrictive composites, to date they have only been weakly evident in single-phase multiferroics. Here in a newly discovered room temperature multiferroic, we demonstrate significant room temperature coupling by monitoring changes in ferroelectric domain patterns induced by magnetic fields. An order of magnitude estimate of the effective coupling coefficient suggests a value of ~1 × 10−7 sm−1.

Mesoscale flux-closure domain formation in single-crystal BaTiO3.

Over 60 years ago, Charles Kittel predicted that quadrant domains should spontaneously form in small ferromagnetic platelets. He expected that the direction of magnetization within each quadrant should lie parallel to the platelet surface, minimizing demagnetizing fields,and that magnetic moments should be configured into an overall closed loop, or flux-closure arrangement. Although now a ubiquitous observation in ferromagnets, obvious flux-closure patterns have been somewhat elusive in ferroelectric materials. This is despite the analogous behaviour between these two ferroic subgroups and the recent prediction of dipole closure states by atomistic simulations research. Here we show Piezoresponse Force Microscopy images of mesoscopic dipole closure patterns in free-standing, single-crystal lamellae of BaTiO3. Formation of these patterns is a dynamical process resulting from system relaxation after the BaTiO3 has been poled with a uniform electric field. The flux-closure states are composed of shape conserving 90° stripe domains which minimize disclination stresses.

Domain Bundle Boundaries in Single Crystal BaTiO3 Lamellae: Searching for Naturally Forming Dipole Flux-Closure / Quadrupole Chains

Naturally occurring boundaries between bundles of 90° stripe domains, which form in BaTiO(3) lamellae on cooling through the Curie Temperature, have been characterized using both piezoresponse force microscopy (PFM) and scanning transmission electron microscopy (STEM). Detailed interpretation of the dipole configurations present at these boundaries (using data taken from PFM) shows that in the vast majority of cases they are composed of simple zigzag 180° domain walls. Topological information from STEM shows that occasionally domain bundle boundaries can support chains of dipole flux closure and quadrupole nanostructures, but these kinds of boundaries are comparatively rare; when such chains do exist, it is notable that singularities at the cores of the dipole structures are avoided. The symmetry of the boundary shows that diads and centers of inversion exist at positions where core singularities should have been expected.

Room-temperature single phase multiferroic magnetoelectrics: Pb(Fe,M)x(Zr,Ti)(1−x)O3 [M=Ta, Nb]

We describe extensive studies on a family of perovskite oxides that are ferroelectric and ferromagnetic at ambient temperatures. The data include x-ray diffraction, Raman spectroscopy, measurements of ferroelectric and magnetic hysteresis, dielectric constants, Curie temperatures, electron microscopy (both scanning electron microscope and transmission electron microscopy (TEM)) studies, and both longitudinal and transverse magnetoelectric constants α33 and α31. The study extends earlier work to lower Fe, Ta, and Nb concentrations at the B-site (from 15%–20% down to 5%). The magnetoelectric constants increase supralinearly with Fe concentrations, supporting the earlier conclusions of a key role for Fe spin clustering. The room-temperature orthorhombic C2v point group symmetry inferred from earlier x-ray diffraction studies is confirmed via TEM, and the primitive unit cell size is found to be the basic perovskite Z = 1 structure of BaTiO3, also the sequence of phase transitions with increasing temperature f...

Wall thickness dependence of the scaling law for ferroic stripe domains

The periodicity of 180° stripe domains as a function of crystal thickness scales with the width of the domain walls, both for ferroelectric and for ferromagnetic materials. Here we derive an analytical expression for the generalized ferroic scaling factor and use this to calculate the domain wall thickness and gradient coefficients (exchange constants) in some ferroelectric and ferromagnetic materials. We then use these to discuss some of the wider implications for the physics of ferroelectric nanodevices and periodically poled photonic crystals.We show how the periodicity of 180 ◦ domains as a function of crystal thickness scales with the thickness of the domain walls both for ferroelectric and for ferromagnetic materials. We derive an analytical expression for the universal scaling factor and use this to calculate domain wall thickness and gradient coefficients (exchange constants) in some ferroic materials. We then use these to discuss some of the wider implications for the physics of ferroelectric nano-devices and periodically poled photonic crystals.

Thickness independence of true phase transition temperatures in barium strontium titanate films

The functional properties of two types of barium strontium titanate (BST) thin film capacitor structures were studied: one set of structures was made using pulsed-laser deposition (PLD) and the other using chemical solution deposition. While initial observations on PLD films looking at the behavior of Tm (the temperature at which the maximum dielectric constant was observed) and Tc* (from Curie-Weiss analysis) suggested that the paraelectric-ferroelectric phase transition was progressively depressed in temperature as BST film thickness was reduced, further work suggested that this was not the case. Rather, it appears that the temperatures at which phase transitions occur in the thin films are independent of film thickness. Further, the fact that in many cases three transitions are observable, suggests that the sequence of symmetry transitions that occur in the thin films are the same as in bulk single crystals. This new observation could have implications for the validity of the theoretically produced thi...