Phase field simulations on the interaction of ferroelectric domains with point defects

One of the suspected micro-mechanical mechanisms causing electric fatigue in ferroelectric materials is the hindering and blocking of domain wall movement. These blocking or pinning phenomena are thought to be due to point defects which interact with domain walls and applied external loads. A phase field model employing the spontaneous polarization as an order parameter is used to simulate the inhomogeneous material behavior. The coupled field equations are solved using the Finite Element Method. The influence of a stationary point defect on a domain wall is shown in a numerical simulation. (© 2008 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)     

On domain switching in deformable ferroelectrics, seen as continua with microstructure

We obtain a three-dimensional continuum model for deformable ferroelectric bodies in their polar phase characterized by a spontaneous polarization. This is accomplished by assuming the body as comprised of a continuum with vectorial microstructure: in each point of the body therefore a gross and a fine structure are superposed, the gross structure representing a non linear polarizable elastic body and the vectorial fine structure describing the spontaneous polarization.¶Among the distinctive features of ferroelectric materials, the most interesting is represented by the organization of spontaneous polarization into a domain structure, which minimizes electrostatic energy and which can be modified by the application of electric and deformation fields. This process, called "polarization reversal" or "domain switching", is associated with various hysteresis loops, the most typical being those between spontaneous polarization and electric field (dielectric hysteresis), and between strain and electric field ("butterfly" loop).¶From the balance laws of continua with vectorial microstructure and dissipation inequality we arrive at the evolution equation for the spontaneous polarization which allows for both inertial and dissipative terms and describes domain switching. We postulate a simple interaction mechanism between the spontaneous polarization and the pair electric field, deformation and arrive at, in the quasi-static case, to a minimization problem for a functional which reminds the micromagnetic energy of deformable ferromagnetics.¶For linearized kinematics we study, in the one-dimensional case, stable relative minimizers and give a simple justification for dielectric hysteresis and butterfly loops: under the hypothesis that the domain walls are sharp interfaces, the solutions we find explain the banded twin domains morphology which is typical of many ferroelectrics.     

A 1D constitutive law for hysteresis effects in piezoceramics

This paper is concerned with a macroscopic constitutive law for domain switching effects, which occur in piezoelectric ceramics. The thermodynamical framework of the law is based on two scalar valued functions: the Helmholtz free energy and a switching surface. In common usage, the remanent polarization and the remanent strain are employed as internal variables. The novel aspect of the present work is to introduce an irreversible electric field, which serves besides the irreversible strain as internal variable. The irreversible electric field has only theoretical meaning, but leads to advantages within the finite element implementation, where displacement and the electric potential are the nodal degrees of freedoms. A common assumption is a one-to-one relation between the irreversible strain and the polarization. This simplification is not employed in the present paper. To accomplish enough space for the polarization, resulting from an applied electric field, the irreversible strains are additively split and a special hardening function is introduced. This balances the amount of space and the domain switching due to polarization. The constitutive model reproduces the ferroelastic and the ferroelectric hysteresis as well as the butterfly hysteresis for piezoelectric ceramics and it accounts for the mechanical depolarization effect. (© 2006 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)     

Toughening effect of ferroelectric ceramics induced by domain switching and dislocations

The multi-scale analysis of fracture toughness of ferroelectric ceramics under complicate mechanical–electrical coupling effect is carried out in this paper. The generalized stress intensity factor (SIF) arising from spontaneous strains and polarization transformation in switching domain zones is accurately obtained by using an extended Eshelby theory. Taking BaTiO₃ ferroelectric ceramic for example, it is discovered that the crack propagation can be induced by domain switching arising from negative electrical field when the crack surface is parallel to the isotropic plane, and the obtained critical electric displacement intensity factor (EDIF) approximates closely to that obtained by the Green’s function method. Additionally, as pinning dislocations and slip dislocations can strongly influence properties of ferroelectric devices and induce the property degradation, it is necessary to investigate the dislocation toughening effects on fatigue and fracture mechanisms. The results show that the dislocation shielding and anti-shielding effects on mode II SIF, mode I SIF and EDIF are obviously different when a dislocation locates at a position near the crack tip. Through the calculation of the critical applied EDIF for crack propagation by using mechanical energy release rate (MERR) theory, it is discovered that the slip angles obviously influence fracture toughness, and the mode II SIF arising from dislocation has little influence on fracture toughness, however, the mode I SIF and EDIF arising from dislocation have great influences on fracture toughness.     

FEM-analysis of a multiferroic nanocomposite – comparison of experiment and numerical simulation

The combination of electric and magnetic materials opens new possibilities in the field of sensor technologies and data storage [1]. These magneto-electric (ME) materials have the property to change a physical ferroic quantity into another, i.e. a magnetic field can change the electric polarization and vice versa. The combination of multiple ferroic characteristics within materials is called multiferroic. Since magneto-electric single-phase materials are rare in nature and typically operate only at very low temperature, they are not favorable in technical applications. However, ME composites, consisting of ferroelectric and ferromagnetic phases, produce a strain-induced magneto-electric product property at room temperature [2]. In these composites, two different effects can be differentiated, the direct and the converse ME effect. The first one describes a polarization which is magnetically caused. In detail, a magnetic field is applied which produces a deformation of the magneto-active phase which is transferred to the electro-active phase and as a consequence this phase exhibits a polarization. Therefore, one can discover a strain-induced polarization. The second effect to observe is a magnetization caused by an electric field. In our contribution, we focus on a (1-3) composite, where cobalt ferrite nanopillars are embedded in a barium titanate matrix, see the experiments described in [3]. In the numerical simulations we compare the changes of the strain-induced inplane polarizations of the ferroelectric matrix with experimental measurements. Furthermore, we analyze the magneto-electric coupling coefficient. (© 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim)     

Second-harmonic generation in ferroelectric thin films on metal substrates for isotropic and cubic symmetries

The Landau–Ginzburg phenomenological theory of ferroelectrics and Landau–Khalatnikov equations of motion are used to model the interaction of electromagnetic radiation and a ferroelectric thin film on a metal substrate. The analysis starts with the minimization of a Gibb’s free energy functional that accounts for the free energy cost of the boundaries of the thin film through a gradient term that is non-zero when the polarization in the film varies. The minimization procedure leads to an Euler–Lagrange equation that can be solved to find the equilibrium polarization in the film. Next the nonlinear dynamical equations that describe the response to an incident electromagnetic field are solved by a perturbation expansion about the equilibrium polarization. The second-harmonic generation term from the expansion is selected. We then go on to calculate a reflection coefficient for the harmonic generation term and investigate how the finite thickness of the film influences the reflection coefficient. In Landau theory the symmetry of the crystal making up the film in the paraelectric phase is reflected in the free energy expression. The analysis here is done for an isotropic symmetry that is often used as an approximation to the actual crystal symmetry and which is mathematically easier to handle. However it is also indicated how the free energy expression can be changed so that it is appropriate for cubic symmetry, and a discussion of how the second harmonic term can be calculated for this case is given. The theory presented is relevant to experimental studies using far-infrared or terahertz reflection measurements because the ferroelectric film is resonant in the far infrared and terahertz ranges.     

Phenomenological theory of surface effects in ferroelectrics and its relationship with transverse Ising model

The relationship between the transverse field Ising model and the Landau phenomenological theory for ferroelectrics is analyzed, and the Landau free energy expression for ferroelectrics having surfaces is derived. It is pointed out that the traditional expression in which the surface integral has only a term of the square polarization is valid only for special cases, in general a term of the polarization to the four should be included as well. By use of the newly derived free energy expression, the thickness-dependence of the spontaneous polarization and Curie temperature of ferroelectric films is calculated; thereby some experimental results incompatible with the traditional phenomenological theory are successfully explained.     

Numerical methods for the modeling of the magnetization vector in multiferroic heterostructures

Multiferroic heterostructures are commonly used to obtain electro-magnetic coupling effects. Thereby, the ferroelectric layer is used to control the magnetization in the ferromagnetic layer. The coupling between the layers is obtained by the mechanical coupling between the layers, which have well-defined interfaces. Within this contribution we use phase field models to define the polarization and magnetization in the ferroelectric and ferromagnetic layers, respectively. A coupling between polarization/magnetization and strains in each layer in combination with coherent deformations at the interface yields an electromagnetic coupling within the entire heterostructure. Numerical formulations for the interpolation of the polarization vector are well-defined in the literature. However, the establishment of a consistent numerical formulation for the ferromagnetic layer, where the length of the magnetization vector has to be constant, remains a difficult task. We propose a new numerical approach for the consistent treatment of the ferromagnetic layer and provide numerical simulations which illustrate the electromagnetic coupling effect. (© 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim)     

Theory and Numerics of Rate-Dependent Incremental Variational Formulations in Ferroelectricity

This paper is concerned with macroscopic continuous and discrete variational formulations for domain switching effects at small strains, which occur in ferroelectric ceramics. The developed new three–dimensional model is thermodynamically–consistent and determined by two scalar–valued functions: the energy storage function (Helmholtz free energy) and the dissipation function, which is in particular rate–dependent. The constitutive model successfully reproduces the ferroelastic and the ferroelectric hysteresis as well as the butterfly hysteresis for ferroelectric ceramics. The rate–dependent character of the dissipation function allows us also to reproduce the experimentally observed rate dependency of the above mentioned hysteresis phenomena. An important aspect is the numerical implementation of the coupled problem. The discretization of the two–field problem appears, as a consequence of the proposed incremental variational principle, in a symmetric format. The performance of the proposed methods is demonstrated by means of a benchmark problem. (© 2008 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)     

畴极化转动对多晶铁电材料断裂特性的影响

主要基于细观力学方法揭示了畴极化转动对多晶铁电陶瓷的各向异性断裂特性的平均影响。首先,用Eshelby-Mori-Tanaka理论和统计模型分析了无穷大铁电材料体中一椭球夹杂的内、外电弹性场,得到畴极化转动对电弹性场的平均影响;其次,推导了等效多晶铁电陶瓷中含一钱币状裂纹的裂纹扩展力(能量释放率)G_ext,并用它估计了畴极化转动对多晶铁电陶瓷断裂特性的影响。对BaTiO₃陶瓷中裂纹扩展力的计算结果表明,对多晶铁电材料断裂特性分析必须考虑畴极化转动的影响。计算结果得出了与实验相一致的结论:在受较小的力时,外加电场对裂纹扩展产生较大的影响,而且在某种程度上能促进了裂纹扩展。     

Phase field modeling of domain evolution in ferroelectric materials in the context of size effects

Phase field modeling provides an efficient tool for the study of domain evolution in ferroelectric materials. Such models naturally introduce an inner length scale which represents the width of the interfaces between domains (domain walls). This inner length scale is of the order of a few unit cells, i.e. about 0.8 nm–2 nm. The focus of this contribution is on size effects in a) the switching behavior of ferroelectric thin films and b) the microstructure evolution in ferroelectric nanodots. (© 2014 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim)     

A finite element phase field model for relaxor ferroelectrics

A mechanically coupled phase field model is presented for the domain evolution and mesoscopic response of relaxor ferroelectrics. In the model the spontaneous polarization is treated as order parameter. The model is derived from thermodynamic analysis including the material force theory. Random field theory is adopted to take the disorder of relaxor ferroelectrics into account. Results show that the model is capable of reproducing relaxor features, such as domain miniaturization, small remnant polarization and large piezoelectric response. Dependence of these features on the random field strength is discussed. (© 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim)     

A Variational Homogenization Approach to Electromechanical Hystereses Caused by Domain Wall Movement

In recent years, increasing interest in so-called smart materials such as ferroelectric polymers and ceramics has been shown. Those materials are used in various actuators, sensors, and also in medical devices. In this paper, we outline a micro-macro approach to the modeling of macroscopic hystereses which directly takes into account the microstructural evolution of electrically poled domains. To this end, an incremental variational formulation for a gradient-type phase field model is developed and exploited for the simulation of electromechanically coupled problems. The formulation determines the hysteretic response of the material in terms of an energy-enthalpy and a dissipation function which both depend on the microscopic remanent polarization treated as an order parameter. The gradient-type balance law for the phase field can be considered as a generalization of Biot's equation for standard dissipative materials and may be related to the classical Ginzburg-Landau equation. Furthermore, the variational formulation serves as natural starting point for a compact and symmetric finite element implementation of the coupled micromechanical problem covering the displacement, the electric potential, and the microscopic polarization vector. For this three-field scenario we develop a variational-based homogenization method which determines the overall macroscopic hysteretic properties of a polycrystalline aggregate. The proposed computational method can be used as a numerical laboratory for the improvement of microstructural properties. (© 2010 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim)     

由上下电极覆盖的铁电薄膜中最小180度电畴尺寸

在较低的电压下,铁电畴发生反转的性能对于研发高密度铁电存储器是至关重要的．为了实现高密度存储,铁电畴必须做得愈小愈好．然而,当外加电场撤去后,很小的铁电畴是不稳定的,会发生缩小,直致消失,导致存储的信息消失．为解决此问题,发展了一种通用的方法用于决定避免反向反转的铁电畴的尺寸．做为一个例子,确定了由上下电极覆盖的铁电薄膜中最小180度电畴尺寸．该研究可以用于许多相似的问题．     

An atomistic scale analysis of ferroelectric nanodomain interfaces

We discuss numerical results of nanodomain interfaces using a new extended molecular statics algorithm for ferroelectric materials. The new algorithm is able to not only calculate the change of the polarization behavior caused by strain but also the influence on the polarization behavior due to mechanical stress. The size effects of 180° head to head and tail to tail nanodomains have already been investigated. This study also considers 90° domain walls and discusses the impact of mechanical stress on polarization patterns and system energies of nanodomain interfaces. (© 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim)     

A laminate-based modelling approach for rate-dependent switching in ferroelectric materials

This contribution focuses on the sequential laminate-based modelling approach for the numerical simulation of the complex electromechanical material behaviour of ferroelectric single crystals. The construction of engineered domain configurations by using the method of sequential lamination in order to study the domain evolution and polarisation switching in ferroelectric single crystals has recently been carried out in the works of [1–4]. By fulfilling the kinematic and polarisation compatibility conditions between the domain structures in a crystal, the proposed laminate-based formulation is governed by an energy-enthalpy function and by a dissipation potential. The mixed energy-enthalpy, written in terms of the total strains, electric field and a set of internal variables, here the multi-rank laminate volume fractions, governs the dissipative electromechanical response of the ferroelectric crystal, whereas the rate-dependent dissipation potential formulated in terms of the flux of the internal variables describes the time-dependent evolution of the multi-rank laminate volume fractions, subjected to inequality constraints. The model reproduces experimentally observed hysteresis and butterfly curves, characteristic for single crystal ferroelectric materials, when subjected to homogeneous electromechanical loading conditions. (© 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim)     

On molecular statics simulations of ferroelectric functional materials

The simulation of ferroelectric materials on the atomistic length scale is getting more and more important due to recent advancements in related manufacturing technologies. Therefore, we present an extended molecular statics algorithm in order to not only compute equilibrium configurations efficiently but also to consider the deformation of a discrete particle system due to macroscopic stress. Furthermore, we discuss the impact of mechanical stress and strain on the spontaneous polarization and the magnitude of the coercive field of a ferroelectric barium titanate system. (© 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim)     

Simulation of Size Effects in Ferroelectric Materials using a Phase Field Model

An electro-mechanically coupled phase field model for domain evolution in ferroelectric materials is presented. The inner length scale introduced by the model gives rise to size effects, especially in the context of the poling behavior of polycrystals. Such size effects are investigated by 2D numerical simulations for barium titanate polycrystals. Ferroelectric hysteresis curves and coercive fields are calculated for two different transition conditions for the order parameter at the grain boundaries. The results show that there is a significant size effect for the investigated polycrystal systems. (© 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim)     

A condensed microelectromechanical constitutive and damage model for tetragonal ferroelectrics

A condensed model for ferroelectric solids with tetragonal unit cells is presented. The approach is microelectromechanically and physically motivated, considering discrete switching processes on the level of unit cells and quasi-continuous evolution of inelastic fields on the domain wall level. To calculate multiple grain interactions an interaction tensor is introduced. Hysteresis loops are simulated for pure electric and electromechanical loading, demonstrating e.g. the influence of a compressive preload on the poling process and interaction between statistically arranged crystallits. The residual stresses and the corresponding principle stresses are used to simulate fatigue damage in ferroelectric materials. (© 2014 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim)     

Interpretation of parameters in phase field models for ferroelectrics

Ferroelectric ceramics have a complex micro–structure which is responsible for their non–linear behavior on the macroscopic scale. The presented model treats the spontaneous polarization as an order parameter, for which a Ginzburg–Landau type evolution is postulated. Contrary to sharp interface models this allows for the simulation of evolving domain structures. The equations are solved via the Finite Element Method, employing an implicit time integration scheme. Numerical simulations show the physical interpretability of the phase field parameters. (© 2008 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)