Gustau Catalan

Magnetocapacitance without magnetoelectric coupling

The existence of a magnetodielectric (magnetocapacitance) effect is often used as a test for multiferroic behavior in new material systems. However, strong magnetodielectric effects can also be achieved through a combination of magnetoresistance and the Maxwell-Wagner effect, unrelated to true magnetoelectric coupling. The fact that this resistive magnetocapacitance does not require multiferroic materials may be advantageous for practical applications. Conversely, however, it also implies that magnetocapacitance per se is not sufficient to establish that a material is multiferroic.The existence of a magnetodielectric (magnetocapacitance) effect is often used as a test for multiferroic behavior in new material systems. However, strong magnetodielectric effects can also be achieved through a combination of magnetoresistance and the Maxwell-Wagner effect, unrelated to multiferroic coupling. The fact that this resistive magnetocapacitance does not require multiferroic materials may be advantageous for some practical applications. Conversely, it also implies that magnetocapacitance per se is not sufficient to establish multiferroic coupling.

Mechanical Writing of Ferroelectric Polarization

Changing Polarization with Applied Stress The direction of electric polarization in ferroelectric materials can be switched with an applied field, but mechanical stresses can also couple to the polarization, forming the basis for piezoelectric effects. In principle, it should be possible to change the polarization of a ferroelectric material mechanically through stress gradients. Lu et al. (p. 59; see the Perspective by Gregg) demonstrate such switching for nanoscale-sized regions created by the stress induced with an atomic force microscope. The substrates are single-crystalline barium titanate films that have a vertically aligned dipole moment created by compressive stresses in the film. This approach may lead to memory devices in which bits are written mechanically but read electrically. The stress gradient created with the tip of an atomic force microscope can locally change the polarization of a barium titanate film. Ferroelectric materials are characterized by a permanent electric dipole that can be reversed through the application of an external voltage, but a strong intrinsic coupling between polarization and deformation also causes all ferroelectrics to be piezoelectric, leading to applications in sensors and high-displacement actuators. A less explored property is flexoelectricity, the coupling between polarization and a strain gradient. We demonstrate that the stress gradient generated by the tip of an atomic force microscope can mechanically switch the polarization in the nanoscale volume of a ferroelectric film. Pure mechanical force can therefore be used as a dynamic tool for polarization control and may enable applications in which memory bits are written mechanically and read electrically.

Strain-gradient-induced polarization in SrTiO3 single crystals.

Piezoelectricity is inherent only in noncentrosymmetric materials, but a piezoelectric response can also be obtained in centrosymmetric crystals if subjected to inhomogeneous deformation. This phenomenon, known as flexoelectricity, can significantly affect the functional properties of insulators, particularly thin films of high permittivity materials. We have measured strain-gradient-induced polarization in single crystals of paraelectric SrTiO3 as a function of temperature and orientation down to and below the 105 K phase transition. Estimates were obtained for all the components of the flexoelectric tensor, and calculations based on these indicate that local polarization around defects in SrTiO3 may exceed the largest ferroelectric polarizations. A sign reversal of the flexoelectric response detected below the phase transition suggests that the ferroelastic domain walls of SrTiO3 may be polar.

Flexoelectric rotation of polarization in ferroelectric thin films

Strain engineering enables modification of the properties of thin films using the stress from the substrates on which they are grown. Strain may be relaxed, however, and this can also modify the properties thanks to the coupling between strain gradient and polarization known as flexoelectricity. Here we have studied the strain distribution inside epitaxial films of the archetypal ferroelectric PbTiO(3), where the mismatch with the substrate is relaxed through the formation of domains (twins). Synchrotron X-ray diffraction and high-resolution scanning transmission electron microscopy reveal an intricate strain distribution, with gradients in both the vertical and, unexpectedly, the horizontal direction. These gradients generate a horizontal flexoelectricity that forces the spontaneous polarization to rotate away from the normal. Polar rotations are a characteristic of compositionally engineered morphotropic phase boundary ferroelectrics with high piezoelectricity; flexoelectricity provides an alternative route for generating such rotations in standard ferroelectrics using purely physical means.

Fractal Dimension and Size Scaling of Domains in Thin Films of Multiferroic BiFeO 3

Domains in ferroelectric films are usually smooth, stripelike, very thin compared with magnetic ones, and satisfy the Landau-Lifshitz-Kittel scaling law (width proportional to square root of film thickness). However, the ferroelectric domains in very thin films of multiferroic BiFeO3 have irregular domain walls characterized by a roughness exponent 0.5-0.6 and in-plane fractal Hausdorff dimension H||=1.4+/-0.1, and the domain size scales with an exponent 0.59+/-0.08 rather than 1/2. The domains are significantly larger than those of other ferroelectrics of the same thickness, and closer in size to those of magnetic materials, which is consistent with a strong magnetoelectric coupling at the walls. A general model is proposed for ferroelectrics, ferroelastics or ferromagnetic domains which relates the fractal dimension of the walls to domain size scaling.

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.

Electric-Field Control of the Metal-Insulator Transition in Ultrathin NdNiO3 Films

Field-effect transistors (FETs) are ubiquitous in our everyday life. Applying the fi eld-effect technique to new materials can lead not only to a modulation of their conductivity, but also to electrostatically driven phase transitions. [ 1–3 ] This method is particularly appealing for complex oxides, which exhibit a wide range of functional properties including metal-insulator (MI) transitions, colossal magnetoresistance and highT c superconductivity, all very sensitive to the level of electronic doping. The electric fi eld-effect approach seems thus to be a natural tool to try controlling and modifying reversibly the ground states of these materials. However, the required changes in carrier densities, which typically exceed 10 14 cm − 2 , [ 1 , 4 ] are diffi cult to induce with standard dielectrics. Recently, electric double layer transistors (EDLT), in which an ionic liquid or an electrolyte is used as a gate dielectric, have been the subject of intense research and rapidly increasing interest owing to the considerable amount of charge which can be provided by this technique. [ 5–7 ]

Progress in perovskite nickelate research

Perovskite nickelates (RNiO3, where R is rare earth or a heavy metal such as Tl or Bi) display sharp metal–insulator transitions, unusual magnetic order, charge order and, perhaps, orbital order. Furthermore, there are strong reasons to believe that some of them may be magnetoelectric multiferroics. In this article the author reviews recent research perovskite nickelates, highlighting the important role that thin film research has contributed to our understanding of their properties. A special emphasis is placed on open questions and highly topical issues such as whether or not nickelates have orbital order, and whether or not (and why) some of them may be multiferroic.