Rheologica Acta Rheol Acta 30:151-158 (1991)

Relaxation and retardation functions of the Maxwell model

with fractional derivatives
Chr. Friedrich

Institut ftir Makromolekulare Chemie, Albert-Ludwigs-Universit~tt Freiburg, FRG

Abstract: A four-parameter Maxwell model is formulated with fractional

derivatives of different orders of the stress and strain using the Riemann-
Liouville definition, This model is used to determine the relaxation and retarda-
tion functions. The relaxation function was found in the time domain with the
help of a power law series; a direct solution was used in the Laplace domain. The
solution can be presented as a product of a power law term and the Mittag-Lef-
tier function. The retardation function is determined via Laplace transformation
and is solely a power law type.
The investigation of the relaxation function shows that it is strongly
monotonic. This explains why the model with fractional derivatives is consistent
with thermodynamic principles.
This type of rheological constitutive equation shows fluid behavior only in the
case of a fractional derivative of the stress and a first order derivative of the
strain. In all other cases the viscosity does not reach a stationary value.
In a comparison with other relaxation functions like the exponential function
or the Kohlrausch-Williams-Watts function, the investigated model has no ter-
minal relaxation time. The time parameter of the fractional Maxwell model is
determined by the intersection point of the short- and long-rime asymptotes of
the relaxation function.

Key words: Fractional _derivative; _Maxwell _model; r_elaxation and _retardation

functions; _Mittag-Leffler _functions; time c_onstants

L Introduction In [4] an operator f o r m of the constitutive equation

Rheological constitutive equations with fractional
derivatives have long played an important role in the
description of the properties of polymer solutions and
melts [ 1 - 6]. These equations are derived f r o m well
known models (e.g., the Maxwell model) by
substituting the ordinary derivatives of first, second
and higher order by fractional derivatives of any
noninteger order a. With this scheme, the order of the
derivative relates to a material parameter which can
be associated with degree of conversion as, for exam-
ple, for a sol-gel transition [7, 8]. In other cases, it has
been shown that constitutive equations employing
fractional derivatives are linked to molecular theories
[31 or are associated with system theory in general or
with Cole-Cole behavior in particular [4, 9]. The ar-
rangement of these models within the frame of linear
theory of viscoelasticity is given in part by Tschoegl
[9].
containing fractional derivatives was derived and led
to the complex modulus.
In [6] a general three-dimensional constitutive
equation applying fractional derivatives to linear
viscoelasticity has been developed. The use of such an
equation is limited because of its mathematical intrac-
tability in the time domain. For a five-parameter
model with a fractional derivative of the stress and of
the strain, the sinusoidal response and ther-
modynamic admissibility was investigated. Attempts
to calculate the relaxation and retardation functions
failed insofar as a less instructive numerical solution
was given.
Usually, the usefulness of these models with frac-
tional derivatives will be tested with the help of dy-
namic experimental investigations. The complex
modulus G* can be calculated easily because the
Fourier transform of a fractional derivative of order
a is the product of (ie)) a and the Fourier transform
152 Rheologica Acta, Vol. 30, No. 2 (1991)

of the function itself. This is correct for functions DV=I-V=Dn~n-~]] n>v>0 (2)
which vanish for negative time, as do the stress and
strain to be considered in this paper. Comparison D n is the usual n-th order (n = 1,2, 3 . . . . ) derivative.
with experiments show that constitutive equations An equivalent presentation of this formula is the
with fractional derivatives can be used in describing following:
the rheological behavior of polymer melts and solu-
tions. n-I (x_a)k-v k)
In contrast, the determination of the relaxation or ovtjl--f0rW 5) (a)
retardation functions is more complicated. Their
analytical determination via Laplace transform is
hindered by the problems arising from the inverse r(n - v~ ~ ( x - ~ - v ) dy ; (3)
Laplace transform [6].
The attempt to find the relaxation function in the in this equation f(") designates the n-th (usual)
time domain by solving the appropriate differential derivative.
equations with fractional derivatives has not yet been From Eq. (3), it can be seen that the fractional
made. Examples of solving these types of differential derivative depends on the lower limit, a, and on the
equations are contained in [10], where some solutions integer derivatives at this lower limit. Further
of diffusion equation are presented. simplifications can be introduced without leading to a
Within this paper the analytic solution of the prob- loss of generality. First of all, the lower limit a is set
lem of relaxation and retardation function determina- to zero. This is possible, because we restrict our atten-
tion are given. These functions are calculated for a tion to strain and stress histories which vanish for all
four-parameter Maxwell model with fractional non-positive times. This form of presentation is
derivatives of different orders for stress and strain. equivalent to the case a = -oo which is closer to the
The obtained solutions are compared with other formulation of a rheological constitutive equation,
relaxation functions to demonstrate its behavior. but which would lead to the mathematically more
complicated Weyl's definition of a fractional deriva-
tive [10]. Further, it is advantageous to set the first
derivatives of stress and strain at the lower limit to
2. I n t e g r a t i o n and d i f f e r e n t i a t i o n to f r a c t i o n a l zero. These quantities will be chosen here to be zero
order and the relaxation and retardation functions will be
calculated for times greater than zero.
Integration to fractional order can be introduced by
In addition, it is-necessary to introduce the Laplace
generalizing the Cauchy equation of repeated integra-
transform of a function f , L ~
tion. If we turn the integer n to values/2 lying in the
interval 0 </2 < 1 and use the Gamma function F in-
stead of the factorial the equation of definition for L{f] = f f ( t ) e - S t dt (4)
the operation of fractional integration can be in-
troduced as follows:
to calculate the Laplace transform of a fractional
1 x f(y) , derivative. Following [10], and under the above-made
U [ f l = r(~----) ~1(x_y)-------I It ay ; (1) assumptions, the following useful relationship is ob-
tained.
I ~ denotes the operator of fractional integration of
order/2. Equation (1) was designated as the Riemann-
LtDV[f]l = sVLU'l . (5)
Liouville definition of such an operator [10]. The
At this point, the important example of the fractional
generalization of Eq. (1) to intervals between 1 and 2,
derivative of the power-law function cx" is given. It
or 2 and 3, etc. is given in [10] as well.
yields
The definition of the operation of fractional dif-
ferentiation, i.e., the inverse operation to the frac-
tional integration, can be arrived at in several ways. F(v + 1)
D a [cx v] = c x v-u , (6)
Here, we will follow [10] and expand the range of/2 F ( v - / 2 + 1)
to negative values and, therefore, introduce the
operator of fractional differentiation D v. 0</2~l,v>-i .
Friedrich, Relaxation and retardation functions of the Maxwell model with fractional derivatives 153

From this it can be seen that the derivative of order tion and retardation functions are next to be deter-
a of a constant is not zero, but gives a power of x. mined.

c
D u[c]=cD u[1]--x-u . (7)
v(1 - ~ )
3. Generalized M a x w e l l m o d e l
The generalized Maxwell model is obtained as a
superposition of Maxwell elements connected in
parallel. However, here generalizations of the single
mode Maxwell model
z + A D [ z ] = AGoD[y] (8)
are considered where z is the stress tensor, y is the
strain tensor, ,~ is the relaxation time, and G O is the
modulus. For deformation histories in which a critical
value (limit of linear viscoelastic behavior) will not be
reached this model is used for the determination of
the complex modulus. A good agreement between
theory and experiment is obtained in the range of low
frequencies. To obtain a good fit at high frequencies
it is necessary to superimpose many Maxwell elements
in the above-described manner. This will not be ex-
amined here.
To enlarge the field of application for a mono-
modal Maxwell model, many modifications were car-
ried out. The introduction of a power law time mea-
sure, according to T = (t/,~) ~, and a deformation-
dependent modulus G = G(y) leads to an enormous
change in behavior although the form of the equation
does not change [11].
Within the framework of this paper, Eq. (8) will be
modified by introducing fractional derivatives, as was
also done in [6]. Using a fractional derivative of order
a instead of the first order derivative of stress, and a
fractional derivative of order fl instead of the first
order derivative of strain, the following four-parame-
ter Maxwell model with fractional derivatives is ob-
tained.
4. D e t e r m i n a t i o n of the relaxation function
4.1 Determination in the time domain
In this part of the paper the relaxation function
G(t) = r/Y0 shall be determined in the time domain
as the solution of the differential equation with a frac-
tional derivative arising from the history y = Y0 for
t > 0. Here r is the shear stress component of the stress
tensor and )'0 is the strain amplitude of the strain
jump history. With this history, we obtain from
Eq. (9), with the help of Eq. (6), the following dif-
ferential equation for the dimensionless relaxation
function g = G(t)/Go in dependence of the dimen-
sionless time x = t/2.
x-~
g+D~[g] - - - (10)
r(i -/~)
For this equation, where x = t/,~ is the dimensionless
time, we attempt to find a solution in the form of a
power series.
g = x a ~ ak xak . (11)
k=O
The coefficients in this equation must fulfill the con-
ditions: % > 0 and fi> - 1. This series is a generaliza-
tion of the "diffintegrable series" given in [10], where
a is restricted to the following form: a = 1/k,
k = 1,2, etc. Without p r o o f that this series fulfills the
conditions of the class o f functions of diffintegrable
series, we use Eq. (11) to find the solution of Eq. (10).
In Sect. 4.2 it is indirectly shown that the series in
Eq. (i l) fulfills these conditions (as expected from
[10]).
Putting Eq. (1 l) in Eq. (10), we arrive at Eq. (12).
xa ~ akx~k+xa_a ~ bkakx~k - X -~ , (12)
k=0 k=0 V(1 - t)

r + 2 a D a [ r ] =)J~GoD/~[y] and 0 < a , f l < l . (9) F ( a k + f i + 1)

with bk -
F(ak+~+ l-a)
In the case a = fl = 0, we get a Hookean element, even
though the case a = fl = 1 gives the Maxwell element. By means of comparison of coefficients the
The formal introduction of two different time con- unknowns ak and fi can be determined. The compari-
stants ~ = 2 and ~ does not lead to further son of the coefficients at the lowest order gives
generalization, because choosing 2 r = b~ gives a
modified modulus bEG. Thus, Eq. (9) represents the 1
fi=a-fl and ao- (13)
Maxwell model with fractional derivatives. Its relaxa- F(1 -fl)bo
154 Rheologica Acta, Vol. 30, No. 2 (1991)

All other coefficients will be chosen so that they are t/2 > 0. This inverse transformation immediately
zero according to Eq. (12). This yields the general for- yields the same result as obtained by Eq. (15):
mula for all other coefficients:
oo ( _ 1)k (t/2) a-~+~k
(-1)k (19)
g(t) = k ~ _ o F ( a k + a ~ f l + 1)
ak - , K=a-fl+l . (14)
F ( a k + tc)
(t/)~ ) > 0
Inserting these conditions in Eq. (11), we obtain the a-fl> -1 .
solution in the following manner.
oo (- 1) k
g(t) = ( t / 2 ) a-~ ~ (t/2) ak . (15)
k=oF(ak+x)
5. Determination of the retardation function
The behavior of this solution will be investigated
The determination of the retardation function J(t)
under Sect. 6.
for the Maxwell model with fractional derivatives is
easily done in the Laplace domain. Starting with the
well-known equation about the relationship between
4.2 Determination in the Laplace domain the Laplace transform of the dimensionless relaxation
function, g, and the dimensionless retardation func-
In this section, we try to obtain the solution in the
Laplace domain. Here, we make use of the abbrevia- tion, j = Go J,
tion L{f} = f . If we build the Laplace transform of
Eq. (9) under the above-made assumptions, term-
sQy= 1 , (20)
by-term, it yields the following equation in the
the following equation is used to transform to the
Laplace domain:
time domain:

f + ( £ s ) a f = Go(2S)~y . (16) 1 + (2s) a

f= 2 - - (21)
(As)P +1
The dimensionless relaxation function, g, is the in-
verse Laplace transform of g = f / ( y s ) . Thus, we have This tabulated inverse Laplace transform, for a :~ fl,
to transform in the time domain the following irra- yields
tionale function
(t/)O ~ (t/~.) ~-a
(~.S) fl-1 j - - - ~ (t//l) > 0 , (22)
g = A- - (17) rq~+ l) rq~-a+l)
1 + (2s) a
and in the case a = fl
For this function no tabulated transform exists and
we must determine another way to infer the solution. (t/2) ~
j - - - ~-1 . (23)
There exists a lemma about the term-wise inverse rq~+ 1)
transformation o f a series in the Laplace domain (see,
e.g., [12]). Since the function [1 + ( s ) O - ~ ] -~ can be Equations (22) and (23) are easy to interpret, and
developed in a series with decreasing powers and hav- show that the retardation function is solely of power
ing a radius of convergence different from zero, law type. It is also easy to see that for the whole a and
Eq. (15) can also be developed in such a series, fulfill- fl parameter range the retardation function is strongly
ing these conditions: increasing if only the condition f l - a - > 0 is fulfilled.
The appropriate assertion about the monotonicly
g=)~ ~ (--1)k(2s) ~ - l - a - a k fl-a-l<0. (18) decreasing character of the relaxation function is not
k=0 as easily made, as will be seen in the next section.
The behavior of the relaxation function is not so
For such a series a term-wise inverse transformation obvious and explains why this function will be ex-
is possible and converges in the time domain for amined in more detail.
Friedrich, Relaxation and retardation functions of the Maxwell model with fractional derivatives
6. Behavior of the relaxation function and the
comparison with other types of relaxation functions
Here the relaxation function o f the Maxwell model
with fractional derivatives is investigated and com-
pared with another function. This other function is a
product of the power-law function x ~-~ and a cut-
o f f function, coff. In the case of the cut-off function
two different types will be examined: a) the strong ex-
ponential cut-off coff (x) = exp ( - x), and b) the soft
cut-off of the Kohlrausch-Williams-Watts type
coff ( x ) = exp ( - x a ) . These functions were used for
material function calculations in [15].
In the relaxation function of the fractional Maxwell
model the term F ( x ) will be introduced to guarantee
the identity of these different functions in the short-
time range. This introduction is equivalent to a
decomposition of the modulus in the following way:
Go = GooF(K). This relaxation function will be in-
vestigated in more detail. Before doing so, some
special cases for the parameters a and fl will be gi,¢en.
For the parameters a = fl = 1/2, we get the result
obtained in [6],
g = exp (x) erfc (X 1/2) , (24)
whereby erfc is the complementary error function.
In the case fl = 1 and a = 1/2 the following result is
obtained:
g = X-1/2 [1 --I'(1/2)X 1/2 exp (x) erfc (x1/2)] , (25)
whereas a = fl = 1 yields the well-known result of the
ordinary Maxwell model.
g = exp ( - x ) . (26)
Now we turn our attention to Eq. (15) or (19). The
sum contained in the relaxation function is the
generalized Mittag-Leffier (GML) function which was
investigated in the 1950s by several authors (see [13]).
With the notation introduced in [13], this function
reads
Ea,z(x) = ~ a,fl>O, (27)
k = o F ( a k + fl)
and
E~, ~(x) = E~ ( x ) , (28)
the latter being the Mittag-Leffler function in-
vestigated by those authors almost a century ago.
155
Nevertheless, these functions remain rather unknown.
Under certain conditions, they yield a generalized ex-
ponential function like the Kohlrausch-Williams-
Watts function.
With this notation, the relaxation function of the
fractional Maxwell model can be presented as
g = F(x)xa-BEa,x(-x a) x = t/2 . (29)
A special case (fl = 1) of this function is known in the
Russian literature as the fractional exponential func-
tion or the Rabotnov function [14]. This function was
obtained by Rabotnov as he inverted a Volterra in-
tegral equation of second kind with a kernel of the
type t a / F ( a + 1). The asymptotic expansion he gave
is certainly incorrect. This expansion is verY impor-
tant in understanding the type of investigated relaxa-
tion function with which we are working.
The designation of this type of function as a frac-
tional exponential function is also known in the
English-speaking countries. This is a consequence of
the fact that the asymptotic expansion for x ~ oo of
the Mittag-Leffler function for non-negative
arguments leads to the following relationship:
Ea(x)= l/aexpxlm+O(lx] -1) 0<a<2. (30)
For the function Ea,~ a similar expansion is obtained
(see [13]).
For negative arguments the expansion must be
developed from the formulas given in [13]. A presen-
tation of the generalized Mittag-Leffler function in
the following form is helpful.
E a , x ( - x ) = E2a,x(x 2) - x E 2 a , x+a(X 2) . (31)
With the aid of this equation and the expansion for
positive arguments it can be concluded that for fl = 1:
Ea, a ( - x) oc 6~ X- 2 a ¢ 1 , (32)
r(1 - a)
and in all other cases:
Ea,~(_x)¢¢ 1 x -~ Kg=a . (33)
F(x - a)
With these functions the asymptotic behavior of the
relaxation function for short and long times can be
established. For Eqs. (32) and (33), we have to look
for different conditions. The first occurs as fl equals
156
1 (an ordinary first order derivative of the strain). The
asymptotes for fl = l , O < a _ 1 0 c = a ) are:
F ( a ) x a - l E a , a ( - x a)
as x~0
o:f xa-1
F(l+a)x_(l+a) as x-~ oo .
r(I - a)
In all other cases different parameters appear in the
parameter list of the G M L function, and for the
asymptotes we get:
F ( K ) xa - PEa,K ( - x a)
I Xa-B as x--'0
o: , r ( K------L~ x - ~
as x ~ oo .
r(1 -Z)
If a rheological constitutive equation is formulated,
the thermodynamic behavior of this "model material"
is also prescribed. Because the second law of ther-
modynamics imposes restrictions on physically realiz-
able processes, it is necessary to consider the ther-
modynamic compatibility of a given rheological con-
stitutive equation. That means, we have to look for
conditions under which the constitutive equation in
general or the parameter functions or parameters in
special in it guarantee non-negative rates of
mechanical energy dissipation tim. This can be for-
mulated [161 by the following equation
fim=qS-~f>_o , with ~=r12~)~2,
where ~ is the stress power which is, in the case of
relaxation after a step-strain experiment, equal to
zero; fis the rate of change of the free energy, and Q
the density. It can be seen that in the case of relaxa-
tion, the demand for non-negative mechanical
dissipation rates is equivalent to the non-positive rate
of free energy. This means that relaxation is associat-
ed with the release of free energy stored during the
jump.
Investigations concerning the energy storage during
harmonic excitations [6] or arbitrary deformation
histories [14] demand that the relaxation and retarda-
tion functions should be positive definite functions.
This means in detail [14] that
Rheologica Acta, Vol. 30, No. 2 (1991)
- G(t),J(t)>_O for all t;
- G ( t ) is monotonic non-increasing, and (37)
- J ( t ) is monotonic non-decreasing.
If Eqs. (22) and (23) are to be analyzed for ther-
modynamic compatibility, we see that the conditions
(37) are fulfilled if the relations fl>_a>O and ; t > 0
(34) hold.
This analysis is more complicated for Eq. (29). It
follows for the power law term that: ~ > 0 and
a-fl<_O. For the G M L F it can be deduced (without
proof) from the results of monotonicity of MLF [13]
that this function is non-increasing if ) . > 0 and
fl_> a > 0. For both functions it follows that the ther-
modynamic compatibility is guaranteed if conditions
(35) are fulfilled:
G0>0, X>0, fl>_a>O. (38)
(35)
For a more detailed study of thermodynamic com-
patibility in connection with other rheological con-
stitutive equations see [17].
The analysis of Eqs. (34) and (35) shows that the
G M L function is not of fractional-exponential type,
but of a power-law type. This is also seen from Figs. 1
and 2. Figure 1 shows the dimensionless relaxation
functions of a fractional Maxwell model with one
fractional derivative of the stress only (fl--- I). For
a = 1, we get the well-known exponential relaxation
of the ordinary Maxwell equation. In all other cases,
we have, at large t, a power law behavior according
to Eq. (34). Figure 2 shows the dimensionless relaxa-
tion functions of the fractional Maxwell model with
fractional derivatives of the stress (a = 0.2, 0.35, 0.5)
and strain 66 = 0.5). Here, we also have power law
behavior at long times, but with a much weaker
dependence on the time as in the case for fl = 1. The
(36) slope of these curves at large t does not depend on a.
This means that the behavior of the relaxation func-
tion for large t is controlled mainly by the order of
fractional differentiation of the strain.
From the asymptotic behavior of the relaxation
function it can also be deduced that under certain cir-
cumstances the fractional Maxwell model shows
solid-like behavior. This means that the stationary
viscosity is infinity. From the equation for the dimen-
sionless viscosity, q, of a stationary flow:
~l = ~ g ( x ) d x , (39)
o
the existence of the integral can be shown with help
the of Eqs. (34) and (35) in the case fl = 1. This means
Friedrich, Relaxation and retardation functions of the Maxwell model with fractional derivatives 157

3 I I I I I I I 4 i [ i i i i i i i

a=0.2

~
2 2
a = 0,5

a = 0,7 0
) X-0.5 Eo5.o.5( x )
0.5
1

a= 1.0
0 -2
a = 0.5 /
b~O em
-1 -4
o # = ~.o

-2 6

-3 -8
-0.5 -x
X e
-0.5 -x °5
-4 -10 X e

I I I [ I 12 r I I I I I I F [
-5 [
-5 -4 -3 -2 -1 0 2 3 -5 -2 -I 0 I 2 3 4 5

log x log t/X

Fig. 1. Dimensionless relaxation function g of the fractional Fig. 3. Comparison of different types of relaxation func-
Maxwell model vs dimensionless time for different orders a tions. The type is given by the corresponding equation
of the fractional derivative of stress. The fractional
derivative of strain is of the order fl = 1 (usual first order
derivative)

1.0 I I I I I I I
Now we turn our attention to Fig. 3. In this figure
a = 0.2 the comparison is given between the relaxation func-
"x tion for a = 0.5, f l = 1 and the above-mentioned,
0.5-a = 0.35
~ ~ ~=o.5 well-known relaxation functions. We recognize once
more the power-law behavior of the relaxation func-
0.0 o( 05 ~ ~ tion of the fractional model, and the cut-off behavior

em
-0.5
"x \
of the other relaxation functions. Obviously, the
relaxation function, according to Eq. (29) shows no
cut-off. For that reason, the time-constant of this
model cannot play the role of a terminal relaxation
asymptotes accor- ~ - ~ k time, as is the case for the other functions. Here it is
-1.o di g to Eq. / X\ a characteristic time, determined by the intersection
point of the short- and long-time asymptotes, as can
-- o.; / N\
-1.5 a = 0.35 / / be seen f r o m Figs. 1 and 2.
a=05 / " To conclude this section, it m a y be suggested that
the three compared relaxation functions can be cast
--2.0 I t I I I I I into one equation by the following procedure:
-5 -4 -3 -2 -1 0 1 2

log x

Fig. 2. Dimensionless relaxation function g of the fractional x °'5 exp ( - x ) with b=0.5,
Maxwell model vs dimensionless time for different orders a c=d=e=l ;
of the fractional derivative of stress. The fractional
derivative of strain is of the order fl = 0.5 x -°'5 exp ( - x °'s) = ~ . x - b Ec, d ( - x e ) with
b=0.5, c=d=l,
that the fractional Maxwell model, with only the frac- e = 0.5; and
tional derivative for the stress, shows fluid behavior.
- 0.5 X0.5) with
In all other cases the integral in Eq. (39) diverges, X E0.5,0.5 ( - =
which is equivalent to solid-like behavior. J
b=c=d=e=0.5 .
158 Rheologica Acta, Vol. 30, No. 2 (1991)

It must be mentioned that the function xbEc, d( - X e) Acknowledgement

with arbitrary b, c, d, e-values is not a solution of a The author would like to express his gratitude to Mary
fractional Maxwell model. Krenceski for improving the English.

7. Conclusions

The generalization of the Maxwell model in the References

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Torvik [6] on the basis of an analysis o f the functions 16. Astarita G, Marrucci G (1974) Principles of Non-
Newtonian Fluid Mechanics. McGraw Hill, London
G ' and G " . New York
3) The investigated Maxwell model shows only in the 17. Friedrich C (1991) to appear in Lecture Notes in Phys-
case fl = 1, and a variable, fluid-like behavior. All the ics. Springer, Berlin Heidelberg New York
other parameter combinations give a divergent viscos-
(Received September 7, 1990;
ity in stationary flow.
in revised form January 7, 1991)
4) The found relaxation function with the G M L F
term can be further generalized to include Kohlrausch
behavior. This generalized relaxation function is not
Author's address:
a solution of the fractional Maxwell model.
This general f o r m of a relaxation function provides Chr. Friedrich
hope that m a t e r i a l s with a supra structure like filled Inst. f. Macromolekulare Chemie
Hermann-Staudinger-Haus
polymers or polymer blends can be described Albert-Ludwigs-Universit~it Freiburg
phenomenologically. Further investigations in this Stefan-Meier-Str. 31
direction are under way. 7800 Freiburg, FRG