Micromechanical modeling of the elasto-viscoplastic behavior of semi-crystalline polymers

A micromechanically based constitutive model for the elasto-viscoplastic deformation and texture evolution of semi-crystalline polymers is developed. The model idealizes the microstructure to consist of an aggregate of two-phase layered composite inclusions. A new framework for the composite inclusion model is formulated to facilitate the use of finite deformation elasto-viscoplastic constitutive models for each constituent phase. The crystalline lamellae are modeled as anisotropic elastic with plastic flow occurring via crystallographic slip. The amorphous phase is modeled as isotropic elastic with plastic flow being a rate-dependent process with strain hardening resulting from molecular orientation. The volume-averaged deformation and stress within the inclusions are related to the macroscopic fields by a hybrid interaction model. The uniaxial compression of initially isotropic high density polyethylene (HDPE) is taken as a case study. The ability of the model to capture the elasto-plastic stress-strain behavior of HDPE during monotonic and cyclic loading, the evolution of anisotropy, and the effect of crystallinity on initial modulus, yield stress, post-yield behavior and unloading-reloading cycles are presented.     

A physically-based constitutive model for anisotropic damage in rubber-toughened glassy polymers during finite deformation

The present work focuses on the development of a physically-based model for large deformation stress-strain response and anisotropic damage in rubber-toughened glassy polymers. The main features leading to a microstructural evolution (regarding cavitation, void aspect ratio, matrix plastic anisotropy and rubbery phase deformation) in rubber-toughened glassy polymers are introduced in the proposed constitutive model. The constitutive response of the glassy polymer matrix is modelled using the hyperelastic-viscoplastic model of [Boyce et al., 1988] and [Boyce et al., 2000]. The deformation mechanisms of the matrix material are accounted for by two resistances: an elastic-viscoplastic isotropic intermolecular resistance acting in parallel with a visco-hyperelastic anisotropic network resistance, each resistance being modified to account for damage effects by void growth with a variation of the void aspect ratio. The effective contribution of the hyperelastic particles to the overall composite behaviour is taken into account by treating the overall system in a composite scheme framework. The capabilities of the proposed constitutive model are checked by comparing experimental data with numerical simulations. The deformation behaviour of rubber-toughened poly(methyl methacrylate) was investigated experimentally in tension at a temperature of 80 °C and for different constant true strain rates monitored by a video-controlled technique. The reinforcing phase is of the soft core-hard shell type and its diameter is of the order of one hundred nanometers. The particle volume fraction was adjusted from 15% to 45% by increments of 5%. The stress-strain response and the inelastic volumetric strain are found to depend markedly on particle volume fraction. For a wide range of rubber volume fractions, the model simulations are in good agreement with the experimental results. Finally, a parametric analysis demonstrates the importance of accounting for void shape, matrix plastic anisotropy and rubber content.     

Homogenization-based constitutive models for porous elastomers and implications for macroscopic instabilities: II—Results

In Part I of this paper, we developed a homogenization-based constitutive model for the effective behavior of isotropic porous elastomers subjected to finite deformations. In this part, we make use of the proposed model to predict the overall response of porous elastomers with (compressible and incompressible) Gent matrix phases under a wide variety of loading conditions and initial values of porosity. The results indicate that the evolution of the underlying microstructure—which results from the finite changes in geometry that are induced by the applied loading—has a significant effect on the overall behavior of porous elastomers. Further, the model is in very good agreement with the exact and numerical results available from the literature for special loading conditions and generally improves on existing models for more general conditions. More specifically, we find that, in spite of the fact that Gent elastomers are strongly elliptic materials, the constitutive models for the porous elastomers are found to lose strong ellipticity at sufficiently large compressive deformations, corresponding to the possible onset of “macroscopic” (shear band-type) instabilities. This capability of the proposed model appears to be unique among theoretical models to date and is in agreement with numerical simulations and physical experience. The resulting elliptic and non-elliptic domains, which serve to define the macroscopic “failure surfaces” of these materials, are presented and discussed in both strain and stress space.     

Homogenization-based constitutive models for porous elastomers and implications for macroscopic instabilities: I—Analysis

The purpose of this paper is to provide homogenization-based constitutive models for the overall, finite-deformation response of isotropic porous rubbers with random microstructures. The proposed model is generated by means of the “second-order” homogenization method, which makes use of suitably designed variational principles utilizing the idea of a “linear comparison composite.” The constitutive model takes into account the evolution of the size, shape, orientation, and distribution of the underlying pores in the material, resulting from the finite changes in geometry that are induced by the applied loading. This point is key, as the evolution of the microstructure provides geometric softening/stiffening mechanisms that can have a very significant effect on the overall behavior and stability of porous rubbers. In this work, explicit results are generated for porous elastomers with isotropic, (in)compressible, strongly elliptic matrix phases. In spite of the strong ellipticity of the matrix phases, the derived constitutive model may lose strong ellipticity, indicating the possible development of shear/compaction band-type instabilities. The general model developed in this paper will be applied in Part II of this work to a special, but representative, class of isotropic porous elastomers with the objective of exploring the complex interplay between geometric and constitutive softening/stiffening in these materials.     

Thermally actuated shape-memory polymers: Experiments, theory, and numerical simulations

With the aim of developing a thermo-mechanically coupled large-deformation constitutive theory and a numerical-simulation capability for modeling the response of thermally actuated shape-memory polymers, we have (i) conducted large strain compression experiments on a representative shape-memory polymer to strains of approximately unity at strain rates of 10⁻³ and 10⁻¹ s⁻¹, and at temperatures ranging from room temperature to approximately 30 °C above the glass transition temperature of the polymer; (ii) formulated a thermo-mechanically coupled large-deformation constitutive theory; (iii) calibrated the material parameters appearing in the theory using the stress-strain data from the compression experiments; (iv) numerically implemented the theory by writing a user-material subroutine for a widely used finite element program; and (v) conducted representative experiments to validate the predictive capability of our theory and its numerical implementation in complex three-dimensional geometries. By comparing the numerically predicted response in these validation simulations against measurements from corresponding experiments, we show that our theory is capable of reasonably accurately reproducing the experimental results. As a demonstration of the robustness of the three-dimensional numerical capability, we also show results from a simulation of the shape-recovery response of a stent made from the polymer when it is inserted in an artery modeled as a compliant elastomeric tube.     

Necking in glassy polymers: Effects of intrinsic anisotropy and structural evolution kinetics in their viscoplastic flow

Two recently proposed developments of the Glass–Rubber constitutive model for glassy polymers treat the viscoplastic deformation as intrinsically anisotropic, and incorporate the kinetics of structural evolution. These features enable the model to capture better the distinctive features of glassy polymers’ constitutive response: post-yield strain-softening and strain-hardening and effects of pre-existing molecular orientation. They have been combined to form a new variant of the model, and the consequences for necking have been explored. Uniaxial extension of prismatic bars was simulated using the finite element method, employing a numerical implementation of the new model, with material parameters of polystyrene. Strain localization predicted with the new model was found to be systematically retarded as compared to predictions with the original (intrinsically isotropic) version of the model, for the same conditions. In particular, the effect of frozen-in molecular orientation was examined. This was found to retard strain localization for stretching parallel to the orientation direction, for both models. But the localization predicted with the new model was always significantly less pronounced than with the original model. Indeed, for sufficiently high pre-orientation (e.g. a uniaxial stretch of 2.2), localization could be effectively prevented with the new model, under conditions when otherwise failure by necking is predicted. Such results can all be explained in terms of a linear stability analysis. They suggest that all previous simulations of necking in glassy polymers made using intrinsically isotropic representations of polymer viscoplasticity may have over-predicted the rate of strain localization.     

Unusual plastic deformation and damage features in titanium: Experimental tests and constitutive modeling

In this paper, we present an experimental study on plastic deformation and damage of polycrystalline pure HCP Ti, as well as modeling of the observed behavior. Mechanical characterization data were conducted, which indicate that the material is orthotropic and displays tension-compression asymmetry. The ex-situ and in-situ X-ray tomography measurements conducted reveal that damage distribution and evolution in this HCP Ti material is markedly different than in a typical FCC material such as copper. Stewart and Cazacu (2011) anisotropic elastic/plastic damage model is used to describe the behavior. All the parameters involved in this model have a clear physical significance, being related to plastic properties, and are determined from very few simple mechanical tests. It is shown that this model predicts correctly the anisotropy in plastic deformation, and its strong influence on damage distribution and damage accumulation. Specifically, for a smooth axisymmetric specimen subject to uniaxial tension, damage initiates at the center of the specimen, and is diffuse; the level of damage close to failure being very low. On the other hand, for a notched specimen subject to the same loading the model predicts that damage initiates at the outer surface of the specimen, and further grows from the outer surface to the center of the specimen, which corroborates with the in-situ tomography data.     

Experimental investigation and modeling of non-monotonic creep behavior in polymers

The deformation behavior of two unfilled engineering thermoplastics, ultra high molecular weight polyethylene (UHMWPE) and polycarbonate (PC), has been investigated in creep test conditions. It has been found that a loading history (prior to the creep test) comprising of loading to a maximum stress or strain value followed by partial unloading to arrive at the target stress value can greatly modify the strain-time behavior. Under such a test protocol, while the expected increase in strain during creep (constant tensile load) is observed, at relatively low creep stresses specimens have also demonstrated a monotonic decrease in strain. In an intermediate stress range, specimens have demonstrated time dependent behavior comprising of a transition from decreasing to increasing strain during creep in tension. This paper presents experimental results to delineate these findings and explore the effect of prior strain rate on the qualitative and quantitative changes in the output (strain-time) behavior. Furthermore, modification of the viscoplasticity theory based on overstress (VBO) model into a double element configuration is introduced. These changes confer upon the model the ability to yield non-monotonic behavior in creep, and supporting simulation results have been included. These changes, therefore, allow the model to simulate strain rate sensitivity, creep, relaxation, and recovery behavior, but more importantly address the issue of non-monotonic changes in creep and relaxation when a loading history involves some degree of unloading.     

Three-dimensional micromechanical modeling of voided polymeric materials

A three-dimensional micromechanical unit cell model for particle-filled materials is presented. The cell model is based on a Voronoi tessellation of particles arranged on a body-centered cubic (BCC) array. The three-dimensionality of the present cell model enables the study of several deformation modes, including uniaxial, plane strain and simple shear deformations, as well as arbitrary principal stress states.The unit cell model is applied to studies on the micromechanical and macromechanical behavior of rubber-toughened polycarbonate. Different load cases are examined, including plane strain deformation, simple shear deformation and principal stress states. For a constant macroscopic strain rate, the different load cases show that the macroscopic flow strength of the blend decreases with an increase in void volume fraction, as expected. The main mechanism for plastic deformation is broad shear banding across inter-particle ligaments. The distributed nature of plastic straining acts to reduce the amount of macroscopic strain softening in the blend as the initial void volume fraction is increased. In the case of plane strain deformation, the plastic flow is observed to initiate across inter-particle ligaments in the direction of constraint. This particular mode of deformation could not have been captured using a two-dimensional, plane strain idealization of cylindrical voids in a matrix.The potential for localized crazing and/or cavitation in the matrix is addressed. It is observed that the introduction of voids acts to relieve hydrostatic stress in the matrix material, compared to the homopolymer. It is also seen that the predicted peak hydrostatic stress in the matrix is higher under plane strain deformation than under triaxial tension (with equal lateral stresses), for the same macroscopic stress triaxiality.The effect of void volume fraction on the macroscopic uniaxial tension behavior of the different blends is examined using a Considère construction for dilatant materials. The natural draw ratio was predicted to decrease with an increase in void volume fraction.     

Micromechanics and macromechanics of carbon nanotube-enhanced elastomers

The effects of carbon nanotubes on the mechanical behavior of elastomeric materials is investigated. The large deformation uniaxial tension and uniaxial compression stress-strain behaviors of a representative elastomer are first presented. This elastomer is then reinforced with multi-wall carbon nanotubes (MWNTs) and the influence of weight fraction of MWNTs on the large deformation behavior of the resulting composite is quantified. The initial stiffness and subsequent strain-induced stiffening at large strains are both found to increase with MWNT content. The MWNTs are also found to increase both the tensile strength and the tensile stretch at break. A systematic approach for reducing the experimental data to isolate the MWNT contribution to the strain energy of the composite is presented. A constitutive model for the large strain deformation behavior of MWNT-elastomer composites is then developed. The effects of carbon nanotubes are modeled via a constitutive element which tracks the stretching and rotation of a distribution of wavy carbon nanotubes. The MWNT strain energy contribution is due to the bending/unbending of the initial waviness and provides the increase in initial stiffness as well as the retention and further enhancement of the increase in stiffness with large strains. The model is shown to track the stretching and rotation of the CNTs with macroscopic strain as well as predict the dependence of the macroscopic stress-strain behavior on the MWNT content for both uniaxial tension and uniaxial compression.     

Self-consistent modeling of large plastic deformation, texture and morphology evolution in semi-crystalline polymers

A self-consistent model for semi-crystalline polymers is proposed to study their constitutive behavior, texture and morphology evolution during large plastic deformation. The material is considered as an aggregate of composite inclusions, each representing a stack of crystalline lamellae with their adjacent amorphous layers. The deformation within the inclusions is volume-averaged over the phases. The interlamellar shear is modeled as an additional slip system with a slip direction depending on the inclusion's stress. Hardening of the amorphous phase due to molecular orientation and, eventually, coarse slip, is introduced via Arruda-Boyce hardening law for the corresponding plastic resistance. The morphology evolution is accounted for through the change of shape of the inclusions under the applied deformation gradient. The overall behavior is obtained via a viscoplastic tangent self-consistent scheme. The model is applied to high density polyethylene (HDPE). The stress-strain response, texture and morphology changes are simulated under different modes of straining and compared to experimental data as well as to the predictions of other models.     

An Eulerian multiplicative constitutive model of finite elastoplasticity

An Eulerian rate-independent constitutive model for isotropic materials undergoing finite elastoplastic deformation is formulated. Entirely fulfilling the multiplicative decomposition of the deformation gradient, a constitutive equation and the coupled elastoplastic spin of the objective corotational rate therein are explicitly derived. For the purely elastic deformation, the model degenerates into a hypoelastic-type equation with the Green–Naghdi rate. For the small elastic- and rigid-plastic deformations, the model converges to the widely-used additive model where the Jaumann rate is used. Finally, as an illustration, using a combined exponential isotropic-nonlinear kinematic hardening pattern, the finite simple shear deformation is analyzed and a comparison is made with the experimental findings in the literature.     

Finite deformation thermo-mechanical behavior of thermally induced shape memory polymers

Shape memory polymers (SMPs) are polymers that can demonstrate programmable shape memory effects. Typically, an SMP is pre-deformed from an initial shape to a deformed shape by applying a mechanical load at the temperature T_H>T_g. It will maintain this deformed shape after subsequently lowering the temperature to T_L<T_g and removing the externally mechanical load. The shape memory effect is activated by increasing the temperature to T_D>T_g, where the initial shape is recovered. In this paper, the finite deformation thermo-mechanical behaviors of amorphous SMPs are experimentally investigated. Based on the experimental observations and an understanding of the underlying physical mechanism of the shape memory behavior, a three-dimensional (3D) constitutive model is developed to describe the finite deformation thermo-mechanical response of SMPs. The model in this paper has been implemented into an ABAQUS user material subroutine (UMAT) for finite element analysis, and numerical simulations of the thermo-mechanical experiments verify the efficiency of the model. This model will serve as a modeling tool for the design of more complicated SMP-based structures and devices.     

Disorder,pre-stress and non-affinity in polymer 8-chain models

To assess the role of single-chain elasticity, non-affine strain fields and pre-stressed reference states we present and discuss the results of numerical and analytical analyses of a modified 8-chain Arruda–Boyce model for cross-linked polymer networks. This class of models has proved highly successful in modeling the finite-strain response of flexible rubbers. We extend it to include the effects of spatial disorder and the associated non-affinity, and use it to assess the validity of replacing the constituent chain's nonlinear elastic response with equivalent linear, Hookean springs. Surprisingly, we find that even in the regime of linear response, the full polymer model gives very different results from its linearized counterpart, even though none of the chains are stretched beyond their linear regime. We demonstrate that this effect is due to the fact that the polymer models are under considerable pre-stress in their ground state. We show that pre-stress strongly suppresses non-affinity in these unit cell models, resulting in a marked stiffening of the bulk response. Polymer networks with some degree of flexibility are thus intrinsically prestressed, and one effect of such prestresses is to reduce non-affine deformations. Combined, these findings may help explain why fully affine mechanical models, in many cases, predict the bulk mechanical response of disordered polymer networks so well.     

Incorporation of yield surface distortion in finite deformation constitutive modeling of rigid-plastic hardening materials based on the Hencky logarithmic strain

In this paper a constitutive model for rigid-plastic hardening materials based on the Hencky logarithmic strain tensor and its corotational rates is introduced. The distortional hardening is incorporated in the model using a distortional yield function. The flow rule of this model relates the corotational rate of the logarithmic strain to the difference of the Cauchy stress and the back stress tensors employing deformation-induced anisotropy tensor. Based on the Armstrong–Fredrick evolution equation the kinematic hardening constitutive equation of the proposed model expresses the corotational rate of the back stress tensor in terms of the same corotational rate of the logarithmic strain. Using logarithmic, Green–Naghdi and Jaumann corotational rates in the proposed constitutive model, the Cauchy and back stress tensors as well as subsequent yield surfaces are determined for rigid-plastic kinematic, isotropic and distortional hardening materials in the simple shear deformation. The ability of the model to properly represent the sign and magnitude of the normal stress in the simple shear deformation as well as the flattening of yield surface at the loading point and its orientation towards the loading direction are investigated. It is shown that among the different cases of using corotational rates and plastic deformation parameters in the constitutive equations, the results of the model based on the logarithmic rate and accumulated logarithmic strain are in good agreement with anticipated response of the simple shear deformation.     

Experimental investigation and modeling of the tension behavior of polycarbonate with temperature effects from low to high strain rates

The effects of strain rate and temperature on the tension stress–strain responses of polycarbonate are experimentally investigated over a wide range of strain rates (0.001–1700 s⁻¹) and temperatures (0–120 °C). A modified split Hopkinson tension bar is used for high-rate uniaxial tension tests. Experimental results indicate that the stress–strain responses of polycarbonate at high strain rates exhibit the nonlinear characteristics including the obvious yielding and strain softening. The tension behavior is strongly dependent on the strain rate and temperature. The values of yield stress and strain at yield present a dramatic increase at higher strain rates and decrease with the increase in temperature. Moreover, there exists a significant rate-sensitivity transition in the polycarbonate tension yield behavior. Based on the experimental investigation, a physically based three-dimensional elastoplastic constitutive model for the finite deformation of glassy polymers is used to characterize the rate-temperature dependent yield and post-yield behavior of polycarbonate when subjected to tension loading. The model results are shown close to the experimental data within the investigated strain-rate and temperature ranges.     

On the shear and bending of a degrading polymer beam

In this paper we develop a model, within a general framework that has been developed to describe the response of dissipative systems, for the strain induced degradation of polymeric solids, due to scission. The theory can be generalized to include degradation due to ultraviolet radiation, oxygen diffusion etc., by incorporating an appropriate form for the rate of dissipation associated with these processes. We study the simple shear and pure bending of such degrading polymer beams.     

Multi-scale constitutive modeling of the small deformations of semi-crystalline polymers

A multi-scale constitutive model for the small deformations of semi-crystalline polymers such as high density Polyethylene is presented. Each macroscopic material point is supposed to be the center of a representative volume element which is an aggregate of randomly oriented composite inclusions. Each inclusion consists of a stack of parallel crystalline lamellae with their adjacent amorphous layers.Micro-mechanically based constitutive equations are developed for each phase. A viscoplastic model is used for the crystalline lamellae. A new nonlinear viscoelastic model for the amorphous phase behavior is proposed. The model takes into account the fact that the presence of crystallites confines the amorphous phase in extremely thin layers where the concentration of chain entanglements is very high. This gives rise to a stress contribution due to elastic distortion of the chains. It is shown that the introduction of chains’ elastic distortion can explain the viscoelastic behavior of crystalline polymers. The stress contribution from elastic stretching of the tie molecules linking the neighboring lamellae is also taken into account.Next, a constitutive model for a single inclusion considered as a laminated composite is proposed. The macroscopic stress-strain behavior for the whole RVE is found via a Sachs homogenization scheme (uniform stress throughout the material is assumed).Computational algorithms are developed based on fully implicit time-discretization schemes.     

Elasto-visco-plastic modeling of mild steels for sheet forming applications over a large range of strain rates

A physically based elasto-visco-plastic constitutive model is presented and compared to experimental results for three different mild steels. The experiments consist of tensile tests ranging from quasi-static conditions up to strain rates of 10³ s^?1 as well as quasi-static simple and reverse shear tests at different amounts of pre-strain. Additional two-step sequential mechanical tests (Bauschinger and orthogonal effects) have been performed to further evaluate the ability of the model to describe strain-path changes at moderate/large strains. The model requires significantly fewer material parameters compared to other visco-plasticity models from the literature, while being able to describe some of the main features of the strain-rate sensitivity of mild steels. Accordingly, the parameter identification is simple and intuitive, requiring a relatively small set of experiments. The strain-rate sensitivity modeling is not restricted to a particular hardening law and thus provides a general framework in which advanced hardening equations can be adopted.     

Modelling of the elasto-viscoplastic damage behaviour of glassy polymers

Constitutive equations are proposed in order to describe the elasto-viscoplastic damage behaviour of polymers. The behaviour is well accounted for by a modified Bodner–Partom model comprising hydrostatic and void evolution terms. The true stress–strain and volumetric strain behaviour of typical rubber-toughened glassy polymers (RTPMMA and HIPS) were experimentally determined at constant local true strain rate by using a video-controlled technique. Successful agreement is obtained between experimental results and the proposed model.