Flexoelectric Tensor Research Articles

Surface polar states and pyroelectricity in ferroelastics induced by flexo-roto field

Theoretical analysis based on the Landau-Ginzburg-Devonshire theory is used to show that the joint action of flexoelectric effect and rotostriction leads to a large spontaneous in-plane polarization (∼1-5 μC/cm2) and pyroelectric coefficient (∼10−3 C/m2K) in the vicinity of surfaces of otherwise non-ferroelectric ferroelastics, such as SrTiO3, with static octahedral rotations. The origin of the improper polarization and pyroelectricity is an electric field we name flexo-roto field whose strength is proportional to the convolution of the flexoelectric and rotostriction tensors with octahedral tilts and their gradients. Flexo-roto field should exist at surfaces and interfaces in all structures with static octahedral rotations, and thus, it can induce surface polar states and pyroelectricity in a large class of otherwise nonpolar materials.

Finite-temperature flexoelectricity in ferroelectric thin films from first principles

A first-principles-based effective Hamiltonian technique is developed to study flexoelectricity in (Ba${}_{0.5}$Sr${}_{0.5}$)TiO${}_{3}$ thin films of different thicknesses in their paraelectric phase. The magnitude as well as sign of individual components of the flexoelectric tensor are reported, which provides answers to existing controversies. The use of this numerical tool also allows us to show that flexoelectric coefficients depend strongly on the film's thickness and temperature. Such dependence is explained using the relationship between the flexoelectric coefficients and the dielectric susceptibility.

Linear magnetoelectric coupling and ferroelectricity induced by the flexomagnetic effect in ferroics

Using the symmetry theory we analyze of the flexomagnetic effect in all 90 magnetic classes and showed that 69 of them are flexomagnetic. Then we explore how the symmetry breaking, inevitably present in the vicinity of the surface, changes the local symmetry and thus the form of the flexomagnetic tensors. All possible surface magnetic classes (in the number of 19) were obtained from the 90 bulk magnetic classes for the surface cuts 001, 010 and 100 types. It appeared that all 90 bulk magnetic classes become flexomagnetic, piezomagnetic and piezoelectric in the vicinity of surface. Using the free energy approach, we show that the flexomagnetic effect leads to a new type of flexo-magnetoelectric (FME) coupling in nanosized and bulk materials, in all spatial regions, where the polarization and (anti)magnetization vectors are spatially inhomogeneous due to external or internal forces. The linear FME coupling, proportional to the product of the gradients of (anti)magnetization and polarization, flexoelectric and flexomagnetic tensors, is significant in nanosized ferroelectrics-(anti)ferromagnetics, where gradients of the polarization and magnetization obligatory exist. The spontaneous FME coupling induced by the spatial confinement give rise to the size-dependent linear magnetoelectric coupling in nanosized ferroelectrics-(anti)ferromagnetics. We show that the flexomagnetic effect may lead to improper ferroelectricity in bulk (anti)ferromagnetics via the linear and nonlinear FME coupling. Inhomogeneous spontaneous polarization is induced by the (anti)magnetization gradient, which exists in all spatial regions, where polarization varies and (anti)magnetization vector changes its direction. The gradient can be induced by the surface influence as well as by external strain via e.g. the sample bending.

The number and types of all possible rotational symmetries for flexoelectric tensors

Flexoelectricity is due to the electric polarization generated by a non-zero strain gradient in a dielectric material without or with centrosymmetric microstructure. It is characterized by a fourth-order tensor, referred to as flexoelectric tensor, which relates the electric polarization vector to the gradient of the second-order strain tensor. This paper solves the fundamental problem of determining the number and types of all possible rotational symmetries for flexoelectric tensors and specifies the number of independent material parameters contained in a flexoelectric tensor belonging to a given symmetry class. These results are useful and even indispensable for experimentally identifying or theoretically/numerically estimating the flexoelectric coefficients of a dielectric material.

Towards a Bulk Theory of Flexoelectricity

Flexoelectricity is the linear response of polarization to a strain gradient. Here we address the simplest class of dielectrics, namely, elemental cubic crystals, and we prove that therein there is no extrinsic (i.e., surface) contribution to flexoelectricity in the thermodynamic limit. The flexoelectric tensor is expressed as a bulk response of the solid, manifestly independent of surface configurations. Furthermore, we prove that the flexoelectric responses induced by a long-wavelength phonon and by a uniform strain gradient are identical.

Atomistic determination of flexoelectric properties of crystalline dielectrics

Upon application of a uniform strain, internal sublattice shifts within the unit cell of a noncentrosymmetric dielectric crystal result in the appearance of a net dipole moment: a phenomenon well known as piezoelectricity. A macroscopic strain gradient on the other hand can induce polarization in dielectrics of any crystal structure, even those which possess a centrosymmetric lattice. This phenomenon, called flexoelectricity, has both bulk and surface contributions: the strength of the bulk contribution can be characterized by means of a material property tensor called the bulk flexoelectric tensor. Several recent studies suggest that strain-gradient induced polarization may be responsible for a variety of interesting and anomalous electromechanical phenomena in materials including electromechanical coupling effects in nonuniformly strained nanostructures, ``dead layer'' effects in nanocapacitor systems, and ``giant'' piezoelectricity in perovskite nanostructures among others. In this work, adopting a lattice dynamics based microscopic approach we provide estimates of the flexoelectric tensor for certain cubic crystalline ionic salts, perovskite dielectrics, $III\text{\ensuremath{-}}V$ and $II\text{\ensuremath{-}}VI$ semiconductors. We compare our estimates with experimental/theoretical values wherever available and also revisit the validity of an existing empirical scaling relationship for the magnitude of flexoelectric coefficients in terms of material parameters. It is interesting to note that two independent groups report values of flexoelectric properties for perovskite dielectrics that are orders of magnitude apart: Cross and co-workers from Penn State have carried out experimental studies on a variety of materials including barium titanate while Catalan and co-workers from Cambridge used theoretical ab initio techniques as well as experimental techniques to study paraelectric strontium titanate as well as ferroelectric barium titanate and lead titanate. We find that, in the case of perovskite dielectrics, our estimates agree to an order of magnitude with the experimental and theoretical estimates for strontium titanate. For barium titanate however, while our estimates agree to an order of magnitude with existing ab initio calculations, there exists a large discrepancy with experimental estimates. The possible reasons for the observed deviations are discussed.

Strain-Gradient-Induced Polarization inSrTiO3Single 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.