A phenomenological constitutive model for ferroelastic and ferroelectric hysteresis effects in ferroelectric ceramics

This paper is concerned with a macroscopic constitutive law for domain switching effects, which occur in ferroelectric ceramics. The three-dimensional model is thermodynamically consistent and is determined by two scalar valued functions: the Helmholtz free energy and a switching surface. In a kinematic hardening process the movement of the center of the switching surface is controlled by internal variables. In common usage, the remanent polarization and the irreversible strain are employed as internal variables. The novel aspect of the present work is to introduce an irreversible electric field, which serves instead of the remanent polarization as internal variable. The irreversible electric field has only theoretical meaning, but it makes the formulation very suitable for a finite element implementation, where displacements and the electric potential are the nodal degrees of freedom. The paper presents an appropriate implementation into a hexahedral finite brick element. The uni-axial constitutive model successfully reproduces the ferroelastic and the ferroelectric hysteresis as well as the butterfly hysteresis for ferroelectric ceramics. Furthermore it accounts for the mechanical depolarization effect, which occurs if the polarized ferroelectric ceramic is subjected to a compression stress.     

Macroscopical non-linear material model for ferroelectric materials inside a hybrid finite element formulation

A new approach for modeling hysteretic non-linear ferroelectric ceramics is presented, based on a fully ferroelectric/ferroelastic coupled macroscopic material model. The material behavior is described by a set of yield functions and the history dependence is stored in internal state variables representing the remanent polarization and the remanent strain. For the solution of the electromechanical coupled boundary value problem, a hybrid finite element formulation is used. Inside this formulation the electric displacement is available as nodal quantity (i.e. degree of freedom) which is used instead of the electric field to determine the evolution of remanent polarization. This involves naturally the electromechanical coupling. A highly efficient integration technique of the constitutive equations, defining a system of ordinary differential equations, is obtained by a customized return mapping algorithm. Due to some simplifications of the algorithm, an analytical solution can be calculated. The automatic differentiation technique is used to obtain the consistent tangent operator. Altogether this has been implemented into the finite element code FEAP via a user element. Extensive verification tests are performed in this work to evaluate the behavior of the material model under pure electrical and mechanical as well as coupled and multi-axial loading conditions.     

State dependent linear moduli in ferroelectrics

A novel experimental method is used to measure the evolution of the linear elastic, dielectric and piezoelectric moduli of a soft ferroelectric ceramic during loading. The applied loading states are combinations of uniaxial compressive stress and electric field. Short pulses of electric field and stress are used to increment the remanent strain and polarization state of the material, while the rates of change of electric displacement and strain during unloading are used to assess the moduli. The remanent quantities are treated as state variables, with a view to expressing the moduli as functions of the material state. The piezoelectric moduli are found to vary approximately linearly with polarization, regardless of the remanent strain state, whilst the dielectric moduli and elastic compliances show more complex behaviour. A simple model of the state dependence of the moduli, based on varying the volume fractions of six crystal variants in the tetragonal system, is used to interpret the results.     

A ferroelectric and ferroelastic 3D hexahedral curvilinear finite element

An isoparametric 3D electromechanical hexahedral finite element integrating a 3D phenomenological ferroelectric and ferroelastic constitutive law for domain switching effects is proposed. The model presents two internal variables which are the ferroelectric polarization (related to the electric field) and the ferroelastic strain (related to the mechanical stress). An implicit integration technique of the constitutive equations based on the return-mapping algorithm is developed. The mechanical strain tensor and the electric field vector are expressed in a curvilinear coordinate system in order to handle the transverse isotropy behavior of ferroelectric ceramics. The hexahedral finite element is implemented into the commercial finite element code Abaqus® via the subroutine user element. Some linear (piezoelectric) and non linear (ferroelectric and ferroelastic) benchmarks are considered as validation tests.     

A finite element model for rate-dependent behavior of ferroelectric ceramics

In this article, materials within a crystallite are modeled by continuum particles consisting of various types of ferroelectric variants which are characterized by their mass fractions. The constitutive behavior of each type of variant is characterized by a proposed Helmholtz free energy potential. Polarization switching is modeled by continuous changes of mass fractions which are governed by a onset criterion and a kinetic relation. A finite element algorithm is developed using the virtual work principle. The simulated results on the rate dependence in the polarization and strain responses to applied alternating electric field of different frequencies are in qualitative consistence with experimental observations. The rate-dependent behavior is explained in terms of changes of mass fractions of the variants that polarization switching involves, in response to the loading programs of different loading rates.     

Shape memory behaviour: modelling within continuum thermomechanics

A phenomenological material model to represent the multiaxial material behaviour of shape memory alloys is proposed. The material model is able to represent the main effects of shape memory alloys: the one-way shape memory effect, the two-way shape memory effect due to external loads, the pseudoelastic and pseudoplastic behaviour as well as the transition range between pseudoelasticity and pseudoplasticity.The material model is based on a free energy function and evolution equations for internal variables. By means of the free energy function, the energy storage during thermomechanical processes is described. Evolution equations for internal variables, e.g. the inelastic strain tensor or the fraction of martensite are formulated to represent the dissipative material behaviour. In order to distinguish between different deformation mechanisms, case distinctions are introduced into the evolution equations. Thermomechanical consistency is ensured in the sense that the constitutive model satisfies the Clausius–Duhem inequality.Finally, some numerical solutions of the constitutive equations for isothermal and non-isothermal strain and stress processes demonstrate that the various phenomena of the material behaviour are well represented. This applies for uniaxial processes and for non-proportional loadings as well.     

Representation of the glass-transition in mechanical and thermal properties of glass-forming materials: A three-dimensional theory based on thermodynamics with internal state variables

In the vicinity of the glass transition, glass-forming materials exhibit pronounced frequency-dependent changes in the mechanical material properties, the thermal expansion behaviour and the specific heat. The frequency dependence becomes apparent under harmonic stress, strain or temperature excitations. The Prigogine-Defay ratio is a characteristic number which connects the changes in magnitude of these quantities at the glass transition. In order to represent the thermoviscoelastic properties of glass-forming materials in continuum mechanics, a three-dimensional approach which is based on the Gibbs free energy as thermodynamic potential is developed in this article. The Gibbs free energy depends on the stress tensor, the temperature and a set of internal variables which is introduced to take history-dependent phenomena into account. In the vicinity of an equilibrium reference state, the specific Gibbs free energy is approximated up to second order terms. Evaluating the Clausius-Duhem inequality, the constitutive relations for the strain tensor, the entropy and the internal variables are derived. In comparison with other approaches, the entropy, the strain tensor and the internal variables are functionals not only of the stress tensor but also of the temperature. Applying harmonic temperature- or stress-controlled excitations, complex frequency-dependent relations for the specific heat under constant stress, for the thermal expansion coefficients as well as for the dynamic mechanical compliance are obtained. The frequency-dependence of these quantities depicts the experimentally observed behaviour of glass-forming materials as published in literature. Under the assumption of isotropic material behaviour, it is shown that the developed theory is compatible with the Prigogine-Defay inequality for arbitrary values of the material parameters.     

Electroelastic field concentrations and polarization switching induced by circular electrode at the interface of piezoelectric disk composites

The electromechanical field concentrations due to circular electrode at the interface of piezoelectric disk composites have been discussed. This paper consists of two parts. In the first part, the problem of an internal electrode embedded at the interface of two dissimilar semi-infinite piezoelectric solids was formulated by means of Hankel transforms, and the solution was solved exactly. In the second part, finite element analysis was carried out to study electromechanical response in piezoelectric disk composites containing a circular electrode at the interface by introducing a model for polarization switching in local areas of field concentrations. A nonlinear behavior induced by localized polarization switching was observed between the strain and the voltage applied to the electrode.     

Cracks with surface charge in poled ferroelectrics

A solution is developed for a prismatic elliptical cavity inserted into an infinite, poled, ferroelectric body subjected to uniform mechanical and electrical loading at infinity consistent with planar fields. The surface of the cavity is also permitted to attract free charge in such a way that the electric field in the cavity remains uniform. The solution is used to develop the mechanical and electrical intensity factors at the tip of the crack obtained by allowing the minor axis of the ellipse to become very small. The energy release rate upon propagation of the crack is also derived. It is found that both the polarization of the ferroelectric and the free charge on the surface of the crack can have a very substantial effect on the magnitudes of both the intensity factors and the energy release rate. The reality of remanent polarization in common ferroelectrics means that it cannot be neglected in the fracture mechanics of such materials. Furthermore, it is likely that remanent polarization leads to free charge being attracted to crack surfaces, so consideration of the latter would also seem to be of importance in the fracture mechanics of ferroelectrics.     

On the evolution of the linear material properties of PZT during loading history—an experimental study

Ferroelectrics exhibit material behavior which is strongly affected by its loading history. Among other phenomena, the coefficients describing the linear material behavior are known to change when the state of polarization is altered. There are several approaches to modeling ferroelectric/ferroelastic behavior. However, with all models, assumptions have to be made on how the linear coefficients depend on the state of polarization. Often the elastic and dielectric coefficients are defined to be constant for the sake of simplicity. Alternatively, their evolution and that of the piezoelectric constants are described rather intuitively, while systematic experimental data are sparse. The present study explores the impact of large signal mechanical and electrical loading on the low frequency linear response of a soft PZT ceramic. This is accomplished via cyclic tests with progressively increasing maximum electrical or mechanical load. Upon load reversal, the quasi-linear response is measured. Remanent polarization and remanent strain are used as internal variables to describe the material behavior as a function of loading history. While the dielectric permittivity κ₃₃ is shown to exhibit only minor variation, Young’s modulus and the piezoelectric coefficient d₃₃ change significantly in the course of loading.     

Time dependent behavior of ferroelectric materials undergoing changes in their material properties with electric field and temperature

This paper presents a time dependent polarization constitutive model suitable for predicting nonlinear polarization and electro-mechanical strain responses of ferroelectric materials subject to various histories of electric fields. The constitutive model is derived based on a single integral form with nonlinear (electric field and temperature dependent) integrand. The total polarization consists of the time-dependent and residual components. The residual component of the polarization is due to polarization switching in the ferroelectric materials. We use an ‘internal clock’ concept to incorporate the effect of electric field on the rate of polarization. The corresponding strain response is determined through the use of third order piezoelectric constant and/or fourth order electrostrictive constant that vary with polarization stage. It is assumed that in absence of polarization, both piezoelectric and electrostrictive constants are zero. To incorporate the effect of temperature on the overall polarization behavior all material parameters in the constitutive model are allowed to change with the ambient temperature. We present numerical studies on the effect of time, temperature, and electric field on the response of ferroelectric material followed by verification of the constitutive model. Experimental data on lead zirconate titanate (PZT) materials available in the literature are used to verify the model.     

A constitutive model for magnetostrictive and piezoelectric materials

This paper is concerned with a macroscopic nonlinear constitutive law for magnetostrictive alloys and ferroelectric ceramics. It accounts for the hysteresis effects which occur in the considered class of materials. The uniaxial model is thermodynamically motivated and based on the definition of a specific free energy function and a switching criterion. Furthermore, an additive split of the strains and the magnetic or electric field strength into a reversible and an irreversible part is suggested. Analog to plasticity, the irreversible quantities serve as internal variables. A one-to-one-relation between the two internal variables provides conservation of volume for the irreversible strains. The material model is able to approximate the ferromagnetic or ferroelectric hysteresis curves and the related butterfly hysteresis curves. Furthermore, an extended approach for ferrimagnetic behavior which occurs in magnetostrictive materials is presented. A main aspect of the constitutive model is its numerical treatment. The finite element method is employed to solve the coupled field problem. Here the usage of the irreversible field strength permits the application of algorithms of computational inelasticity. The algorithmic consistent tangent moduli are developed in closed form. Hence, quadratic convergence in the iterative solution scheme of governing balance equations is obtained.     

Phenomenological model for the macroscopical material behavior of ferroelectric ceramics

A thermodynamically consistent phenomenological model for the simulation of the macroscopic behavior of ferroelectric polycrystalline ceramics is presented. It is based on the choice of microscopically motivated internal state variables, which describe the texture and the polarization state of the polycrystal. Saturation states are defined for the internal state variables. The linear material behavior is modelled by a transversely isotropic piezoelectric constitutive law, where the anisotropy is history dependent. For non-linear irreversible processes, a switching function and associated evolution rules are applied, satisfying the principle of maximum ferroelectric dissipation. Saturation is modelled by the use of energy-barrier functions in the electric enthalpy density function. Numerical examples demonstrate the capability of the proposed model, to predict the typical experimental results.     

Thermomechanical material modelling based on a hybrid free energy density depending on pressure,isochoric deformation and temperature

In order to represent temperature-dependent mechanical material properties in a thermomechanical consistent manner it is common practice to start with the definition of a model for the specific Helmholtz free energy. Its canonical independent variables are the Green strain tensor and the temperature. But to represent calorimetric material properties under isobaric conditions, for example the exothermal behaviour of a curing process or the dependence of the specific heat on the temperature history, the temperature and the pressure should be taken as independent variables. Thus, in the field of calorimetry the Gibbs free energy is usually used as thermodynamic potential whereas in continuum mechanics the Helmholtz free energy is normally applied. In order to simplify the representation of calorimetric phenomena in continuum mechanics a hybrid free energy density is introduced. Its canonical independent variables are the isochoric Green strain tensor, the pressure and the temperature. It is related to the Helmholtz free energy density by a Legendre transformation. In combination with the additive split of the stress power into the sum of isochoric and volumetric terms this approach leads to thermomechanical consistent constitutive models for large deformations. The article closes with applications of this approach to finite thermoelasticity, curing adhesives and the glass transition.     

Fully coupled, multi-axial, symmetric constitutive laws for polycrystalline ferroelectric ceramics

In this paper, a general form for multi-axial constitutive laws for ferroelectric ceramics is constructed. The foundation of the theory is an assumed form for the Helmholtz free energy of the material. Switching surfaces and associated flow rules are postulated in a modified stress and electric field space such that a positive dissipation rate during switching is guaranteed. The resulting tangent moduli relating increments of stress and electric field to increments of strain and electric displacement are symmetric since changes in the linear elastic, dielectric and piezoelectric properties of the material are included in the switching surface. Finally, parameters of the model are determined for two uncoupled cases, namely non-remanent straining ferroelectrics and purely ferroelastic switching, and then for the fully coupled ferroelectric case.     

On thermodynamic potentials in thermoelasticity under small strain and finite thermal perturbation assumptions

Expressions for thermodynamic potentials (internal energy, Helmholtz energy, Gibbs energy and enthalpy) of a thermoelastic material are developed under the assumption of small strains and finite changes in the thermal variable (temperature or entropy). The literature provides expressions for the Helmholtz energy in terms of strain and temperature, most often as expansions to the second order in strain and to a higher order in temperature changes, which ensures an affine stress–strain relation and a certain temperature dependence of the moduli of the material. Expressions are here developed for the four potentials in terms of all four possible pairs of independent variables. First, an expression is obtained for each potential as a quadratic function of its natural mechanical variable with coefficients depending on its natural thermal variable that are identified in terms of the moduli of the material. The form of the coefficients’ dependence on the thermal variable is not specified beforehand so as to obtain the most general expressions compatible with an affine stress–strain relation. Then, from each potential expressed in terms of its natural variables, expressions are derived for the other three potentials in terms of these same variables using the Gibbs–Helmholtz equations. The paper provides a thermodynamic framework for the constitutive modeling of thermoelastic materials undergoing small strains but finite changes in the thermal variables, the properties of which are liable to depend on the thermal variables.     

Elasto-plasticity of paper

We develop a constitutive model of paper's in-plane biaxial tensile response accounting for the elastic–plastic hardening behavior, and its orthotropic character. The latter aspect is motivated by machine-made papers, which, in contrast to isotropic laboratory handsheets, are strongly oriented. We focus on modeling paper's response under monotonic loading, this restriction allowing us to treat the elastic-plastic response as a physically nonlinear elastic one. A strain energy function of a hyperbolic tangent form is developed so as to fit the entire range of biaxial and uniaxial experiments on a commercial grade paper. This function may then be introduced as the free energy function into a model based on thermomechanics with internal variables.     

A finite element model of ferroelastic polycrystals

A finite element model of switching in polycrystalline ferroelastic ceramics is developed. It is assumed that a crystallite switches if the reduction in mechanically driven potential energy of the system exceeds a critical value per unit volume of switching material. Stress induced (i.e. ferroelastic) switching is a change of permanent strain in characteristic crystallographic directions. Martensitic twinning is one example, but the strain response of ferroelectric materials has the same characteristics. The model is suitable for representing ferroelastic systems such as shape memory alloys and as a preliminary model for ferroelectric/ferroelastic materials such as perovskite piezoelectrics. In the simulations, each crystallite is represented by a finite element and the crystallographic principal direction for each crystallite is assigned randomly. Different critical values for the energy barrier to switching are selected to simulate stress vs strain hysteresis loops of a ceramic lead lanthanum zirconate titanate (PLZT) at room temperature. The measured stress versus strain curves of polycrystalline ceramics designated PZT-A and PZT-B are also reproduced by the model.     

Size-effects on yield surfaces for micro reinforced composites

Size effects in heterogeneous materials are studied using a rate independent higher order strain gradient plasticity theory, where strain gradient effects are incorporated in the free energy of the material. Numerical studies are carried out using a finite element method, where the components of the plastic strain tensor appear as free variables in addition to the displacement variables. Non-conventional boundary conditions are applied at material interfaces to model a constraint on plastic flow due to dislocation blocking. Unit cell calculations are carried out under generalized plane strain conditions. The homogenized response of a material with cylindrical reinforcing fibers is analyzed for different values of the internal material length scale and homogenized yield surfaces are presented. While the main focus is on initial yield surfaces, subsequent yield surfaces are also presented. The center of the yield surface is tracked under uniaxial loading both in the transverse and longitudinal directions and an anisotropic Bauschinger effect is shown to depend on the size of the fibers. Results are compared to conventional predictions, and size-effects on the kinematic hardening are accentuated.     

Strain tunability of dielectric and ferroelectric properties in epitaxial lead titanate thin films

Many distinguished properties of epitaxial ferroelectric thin films can be tunable through the misfit strain. The strain tunability of ferroelectric and dielectric properties in epitaxial lead titanate ultrathin films is numerically investigated by using a phase field model, in which the surface effect of polarization is taken into account. The response of polarization to the applied electric field in the thickness direction is examined with different misfit strains at room temperature. It is found that a compressive misfit strain increases the coercive field and the remanent polarization while a tensile misfit strain decreases both of them. The nonlinear dielectric constants of the thin films with tensile misfit strains are much larger than those of the thin films without misfit strains, which are attributed to the existence of the a/c/a/c multiple domains in the thin films under tensile misfit strains.