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A Pseudo-Elastic Model For The Mullins Effect in Filled Rubber
A Pseudo-Elastic Model For The Mullins Effect in Filled Rubber
When a rubber test piece is loaded in simple tension from its virgin state, unloaded
and then reloaded, the stress required on reloading is less than that on the initial
loading for stretches up to the maximum stretch achieved on the initial loading. This
stress softening phenomenon is referred to as the Mullins effect. In this paper a sim-
ple phenomenological model is proposed to account for the Mullins effect observed in
filled rubber elastomers. The model is based on the theory of incompressible isotropic
elasticity amended by the incorporation of a single continuous parameter, interpreted
as a damage parameter. This parameter controls the material properties in the sense
that it enables the material response to be governed by a strain-energy function on
unloading and subsequent submaximal loading different from that on the primary
(initial) loading path from the virgin state. For this reason the model is referred
to as pseudo-elastic and a primary loading–unloading cycle involves energy dissipa-
tion. The dissipation is measured by a damage function which depends only on the
damage parameter and on the point of the primary loading path from which unload-
ing begins. A specific form of this function with two adjustable material constants,
coupled with standard forms of the (incompressible, isotropic) strain-energy func-
tion, is used to illustrate the qualitative features of the Mullins effect in both simple
tension and pure shear. For simple tension the model is then specialized further in
order to fit Mullins effect data. It is emphasized that the model developed here is
applicable to multiaxial states of stress and strain, not just the specific uniaxial tests
highlighted.
Keywords: pseudo-elasticity; rubber elasticity; Mullins effect;
stress softening; solid mechanics
1. Introduction
The theory of isotropic elasticity, in particular the incompressible theory, has been
used extensively for modelling the mechanical response of rubber-like materials, such
as vulcanized natural rubber and synthetic rubbers (see, for example, the reviews
by Ogden (1982, 1986)). The success of the theory is reflected in its widespread use
for engineering design calculations, based mainly on finite-element software packages
such as Abaqus and Marc into which specific material models have been incorpo-
rated. Elasticity theory has also been applied to many of the rubber-like materials
used in engineering components, notably rubbers hardened by the inclusion of fillers
† Present address: Department of Engineering Mathematics, University of Newcastle, Stephenson
Building, Newcastle upon Tyne NE1 7RU, UK.
Proc. R. Soc. Lond. A (1999) 455, 2861–2877 c 1999 The Royal Society
Printed in Great Britain 2861 TEX Paper
Downloaded from http://rspa.royalsocietypublishing.org/ on April 8, 2016
We assume that the material response of the body can be described in terms of
an energy function of the form W(F , η), defined per unit volume in Ω. This is the
prescription used in standard nonlinear elasticity theory except that an additional
scalar variable η has been included. Because of the interpretation and influence of
this variable, discussed below, it is no longer appropriate to regard W as a stored- (or
strain-) energy function and we therefore refer to it as a pseudo-energy function and
the ensuing constitutive theory as pseudo-elasticity, terminology used by Lazopoulos
& Ogden (1999). In this paper it suffices to take η to be a continuous variable. A
theory in which η is allowed to be discontinuous was discussed by Lazopoulos &
Ogden (1998, 1999) in the context of modelling phase-change phenomena.
The pseudo-energy function is required to satisfy the usual objectivity conditions,
for details of which we refer to Ogden (1984), for example. The material is taken to
be incompressible, so that F satisfies the constraint
det F = 1. (2.2)
The nominal and Cauchy stress tensors, S and σ, respectively, are then given by
∂W ∂W
S= (F , η) − pF −1 , σ=F (F , η) − pI, (2.3)
∂F ∂F
where p is a Lagrange multiplier associated with the constraint (2.2) and I is the
identity tensor.
From Lazopoulos & Ogden (1998), it follows that in equilibrium in the absence of
body forces,
Div S = 0 in Ω, (2.4)
∂W
(F , η) = 0 in Ω, (2.5)
∂η
where Div denotes the divergence operator in Ω. Equation (2.4) is the usual equi-
librium equation, while (2.5) is an additional equation arising from inclusion of the
variable η. Note that (2.5) is easily modified to account for more than one additional
variable. Moreover, if η is allowed to be discontinuous, then further equations (jump
conditions) are needed, as discussed in Lazopoulos & Ogden (1998, 1999).
The role of the parameter η can be interpreted as follows. During a deformation
process, η may be either active or inactive and may switch from inactive to active
and conversely provided it remains continuous in so doing. When it is not active, the
material behaves as an elastic material with strain-energy function W(F , η), η being
held constant. However, when η is active it is determined implicitly in terms of F
by equation (2.5); we write η = χ(F ) in this case. The material will again behave as
an elastic material, but with a different strain-energy function, namely W(F , χ(F )).
At a transition point where the parameter η switches on or off, as we see below, the
pseudo-energy function W and the associated stresses change continuously.
(a) Isotropy
Henceforth we restrict attention to isotropic materials. The pseudo-energy function
then depends on the deformation only through the (positive) principal stretches
λ1 , λ2 and λ3 , where λ2i (i = 1, 2, 3) are the eigenvalues of the right Cauchy–Green
c'
c
stress (t)
b'
b C
B
λ
Figure 1. Schematic loading–unloading curves in simple tension (Mullins effect).
is that the energy required to cause the damage is not recoverable, and the area
between, for example, the curves abb0 and aBb0 represents this energy for primary
loading up to b0 . These interpretations are embodied in the model discussed below.
in this case. This is the energy function of the perfectly elastic material for which
the primary loading path is also the unloading path. We therefore take W̃ (λ1 , λ2 )
to characterize any primary loading path in (λ1 , λ2 )-space, exemplified by the path
abb0 cc0 d in figure 1 in the simple tension specialization. Standard forms of the strain-
energy function, such as the neo-Hookean or Ogden forms (see, for example, Ogden
1984), may then be used as representative of W̃ (λ1 , λ2 ).
From (2.9) the specialization (3.1) yields the stresses
where a superposed tilde refers to a primary loading path and (2.10) is not operative.
We impose the usual requirements
where t̃ is the Biot stress on the primary loading path at the same value of λ. For
(3.11) to predict stress softening it is clear that we must have η 6 1 on the unloading
path. We also take η > 0, so that t remains positive on unloading until λ = 1 is
reached.
On substitution of (3.8) into equation (2.10), we obtain
−φ0 (η) = W̃ (λ1 , λ2 ), (3.12)
which, implicitly, defines the damage parameter η in terms of the deformation. The
simple tension specialization of (3.12) is
(c) Dissipation
When the damaged material is in a fully unloaded state the pseudo-energy function
(3.8) has the residual value
w(1, 1) = W (1, 1, ηm ) = φ(ηm ). (3.20)
Thus, the residual (non-recoverable) energy φ(ηm ) may be interpreted as a measure
of the energy required to cause the damage in the material. In a uniaxial test such as
simple tension, φ(ηm ) is the area between the primary loading curve and the relevant
unloading curve.
We recall that in view of the condition (3.14) the function φ depends, through
Wm , on the point at which unloading starts. We accommodate this by defining the
function f , independent of Wm , by
φ0 (η) + Wm = φ0 (η) − φ0 (1) = f (η). (3.21)
Specification of the form of the function f is then equivalent to specifying the con-
stitutive function φ subject to (3.9), (3.14) and (3.16). Note that we must have
f (1) = 0, f (ηm ) = Wm , (3.22)
and therefore, by the monotonicity of φ0 and hence of f , the second equation in (3.22)
gives ηm uniquely in terms of Wm .
Integration of equation (3.21) with respect to η followed by rearrangement leads
to
Z η
φ(η) = f (η) dη + (1 − η)Wm ≡ Φ(η, Wm ), (3.23)
1
where m and r are positive parameters (material constants) and erf −1 (·) is the inverse
of the error function, which has properties particularly well suited to our aims. It is
not necessary to integrate this equation in order to satisfy (3.9) explicitly, but we
note that (3.14) follows immediately from (3.26). The properties of the error function
ensure that the inequality (3.16) holds. On substitution of equation (3.26) into (3.12)
and after a little algebra the expression
1 1
η = 1 − erf (Wm − W̃ (λ1 , λ2 )) (3.27)
r m
for η is obtained.
Since m and r were defined to be positive and, by definition, W̃ (λ1 , λ2 ) 6 Wm ,
it follows that η 6 1, with equality only when W̃ (λ1 , λ2 ) = Wm . Moreover, taking
r > 1 ensures that η is positive. The minimum value ηm of η, corresponding to the
undeformed configuration, is given by
1 Wm
ηm = 1 − erf , (3.28)
r m
and the dissipation rate (3.25) is given explicitly by
1 Wm
φ̇(ηm ) = erf Ẇm . (3.29)
r m
The parameters r and m have the following physical interpretations. The parame-
ter r is a measure of the extent of the damage relative to the virgin state. In particular,
from (3.27) it follows that the larger the value of r the less the damage parameter
η can depart from unity and the less damage can occur. Note that if r < 1 were
allowed then η, which enters as a multiplicative factor in the pseudo-energy func-
tion (3.8), and hence the stress, would vanish before the undeformed configuration
is recovered. This possibility has been ruled out in our considerations in this paper.
In contrast, the parameter m controls the dependence of the damage on the extent
of deformation. For small values of m, significant damage is caused for small strains,
and the material response in the small strain region is not markedly affected by fur-
ther primary loading. For larger values of m there is relatively little damage for small
strains but the material response changes significantly in the small strain region after
subsequent primary loading. Figure 2 illustrates these observations in respect of a
neo-Hookean material undergoing pure shear with r and m varied independently.
The dashed curve in each of the figures in the right-hand column is, for fixed r, the
asymptotic unloading–reloading curve for large primary deformation.
4. Numerical results
In this section we consider first the example of pure shear to highlight the theory
developed heretofore, in particular to show the relative behaviour of the main and side
stresses with respect to stress softening. The theory is then used to fit the (somewhat
limited) experimental data obtained by Mullins from simple tension tests.
4
r = 1.2, m = 2.0 r = 2.0, m = 0.5
3
0
4
r = 2.0, m = 2.0 r = 2.0, m = 2.0
3
Biot stress (t)
0
4
r = 3.0, m = 2.0 r = 2.0, m = 4.0
3
Biot stress (t)
0
1 2 3 4 1 2 3 4
stretch (λ) stretch (λ)
Figure 2. Plots of the main Biot stress t in pure shear against the corresponding stretch λ for
the neo-Hookean material, showing the effect of changing the parameters r (left-hand column)
and m (right-hand column).
4 3.5
(a) (b)
3
3
Biot stress (t) 2.5
1 1
0.5
0 0
1 2 3 4 1 2 3 4
λ λ
Figure 3. Pure shear loading–unloading curves for (a) the neo-Hookean material and (b) the
Ogden material. The main Biot stresses t1 (continuous curves) and the side stresses t2 (broken
curves) are plotted against λ.
Similar expressions may be written down for the Ogden form of strain-energy
function
X3
µi αi
W̃ (λ1 , λ2 ) = µ (λ1 + λα −αi −αi
2 + λ1
i
λ2 − 3), (4.4)
i=1
αi
70
(a) (b)
60
50
Biot stress (t) 40
30
20
10
0
0 0.5 1 1.5 2 2.5 3 3.5 1 1.5 2 2.5 3 3.5 4 4.5
strain (ε ) λ
Figure 4. (a) Data obtained from Mullins & Tobin (1957); (b) best-fit curves from the model
developed here.
the first equation in (4.1). For the neo-Hookean material, we therefore have
σ1 = λt1 = ηµ(λ2 − λ−1 ), (4.5)
and similarly for (4.4).
In figure 4a we display data taken from Mullins & Tobin (1957, fig. 4) for a simple
tension experiment in which the stress t = t1 is plotted against the strain measure
= λ − 1. All the measurements were taken during loading. It should be noted that
the material used by Mullins & Tobin (1957) exhibited permanent set on removal of
the stress, so that a given sample was longer after the initial stretch than it was in
its virgin state. This meant that after the initial loading the raw data curves did not
pass through the origin, but intercepted the horizontal axis at some positive value.
In their original paper Mullins & Tobin (1957) adjusted their data by subtracting
the permanent set from length measurements to ensure that the stress–strain curves
passed through the origin. Consequently, the data points on the reloading curves
have been shifted to the left of their true positions by the amount of the ‘set’ strain
(which is different for each reloading). There must therefore be some uncertainty
about the precise interpretation of the data.
We do not discuss the nature of the permanent set here nor the extent to which it
is recoverable, but clearly it affects the ability of the theory discussed here to fit the
data. We note that previous models designed to describe the Mullins effect do not
take account of the permanent set either. The theory discussed here will be adapted
to incorporate permanent set in a subsequent paper.
Figure 4b shows the result of a nonlinear least-squares best-fit solution to the data
obtained from Mullins & Tobin (1957) based on a strain-energy function of the form
(4.4). Here, t is plotted against λ rather than . First, a best fit was carried out for
the primary loading curve to obtain the appropriate values for the material constants
in (4.4). These values are
µ1 = 8.00, µ2 = 0.76, µ3 = −4.50,
α1 = 1.25, α2 = 4.0, α3 = −2.0.
With the primary loading curve fitted, it was then a simple matter to find suitable
values of the parameters r and m in (3.27) to fit the reloading curves. The values
2 3
λ2
2
1
1
0 1 2 3 0 1 2 3 4 5
λ1 λ1
Figure 5. Constant energy contour curves in (λ1 , λ2 )-space for (a) the neo-Hookean
strain-energy function (4.2) and (b) the strain-energy function (5.2).
obtained are r = 2.104 and m = 22.45. The results are displayed as continuous curves
in figure 4b. The comparison between the theory and data is very good, especially
bearing in mind the reservations expressed above. Indeed, the fit of the theory to
the data shown in figure 4b is somewhat better than that achieved by Govindjee &
Simo (1992a), who, it should be noted, included only the second and third reloading
paths in their numerical simulation.
5. Discussion
In the examples of pure shear and simple tension considered above, the point at which
unloading began was identified by the value of the stretch at that point. However, it is
clear from the theory developed in § 3 that it is the associated energy on the primary
path, rather than the deformation, that is the key ingredient. In the case of general
biaxial deformations it is the value of the energy maximum Wm = W̃ (λ1m , λ2m )
on the primary loading path, rather than the specific (λ1m , λ2m ) pair, that governs
the unloading response. Thus, any other pair of (λ1 , λ2 ) values corresponding to the
same value of Wm could equally be taken as the starting point for unloading. The
collection of all such pairs satisfies the equation
W̃ (λ1 , λ2 ) = Wm , (5.1)
and, for given (constant) Wm , forms a closed contour in (λ1 , λ2 )-space. This is
depicted in figure 5a in respect of the neo-Hookean strain-energy function (4.2),
illustrated for Wm /µ = 1, 2, 3, 4.
The contour defined by the current maximum value Wm represents the current
damage threshold, and η = 1 at any point on this contour. For any deformation path
within this contour η < 1 and no further damage occurs. The energy required on
the initial loading path to cause the damage is not required on subsequent loading
up to the contour boundary. However, if the deformation path crosses the contour,
primary loading is again activated, η = 1 and further damage will occur. The value
of W̃ (λ1 , λ2 ) will increase until the next maximum value Wm is reached, at which
point loading terminates and a new threshold contour is established (which encloses
the previous one).
Note that if σ3 = 0, then at any point (λ1 , λ2 ) on the contour (5.1) the vector
(t̃1 , t̃2 ), being the gradient of W̃ , is the outward pointing normal. For the incremental
deformation vector (δλ1 , δλ2 ), the corresponding increment in W̃ is given by the
scalar product (t̃1 , t̃2 ) · (δλ1 , δλ2 ). This is positive if (δλ1 , δλ2 ) points out of the
region enclosed by the contour (primary loading) and negative if it is inward pointing
(unloading).
Note that the regions enclosed by the contours shown in figure 5a are convex and
hence W̃ increases on any straight-line path from (1, 1), as intimated in § 3 b. This
is also the case for many commonly used forms of W̃ including those described by
(4.4) with µi αi > 0 and |αi | > 1 for each i. By contrast, we note in passing that
for a single-term form of (4.4) with |α1 | < 1 and Wm sufficiently large the contours
are not convex but, nevertheless, W̃ increases on any straight-line path from (1, 1).
The non-convexity is illustrated in figure 5b for α1 = 12 , that is, for the strain-energy
function
1/2 1/2 −1/2 −1/2
W̃ (λ1 , λ2 ) = 8µ(λ1 + λ2 + λ1 λ2 − 3). (5.2)
It is important to emphasize that for the model developed in this paper the extent
of the damage sustained by the material is controlled by the maximum energy state
Wm attained. We therefore have an energy-based damage model, as distinct from the
strain-based models of Johnson & Beatty (1993a, b) and Govindjee & Simo (1991,
1992a, b). For this reason the model is readily applicable to three-dimensional (multi-
axial) states of deformation. Specifically, for computational purposes, the value Wm
may be stored and the current energy state may be compared with it to determine
if further damage is being caused. Within a finite-element code this comparison can
be carried out on an element-by-element basis.
D.G.R. was supported by a research grant awarded by the UK Engineering and Physical Sciences
Research Council. The authors thank the Tun Abdul Razak Research Centre for their technical
advice and support.
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