J. Non-Newtonian Fluid Mech.

129 (2005) 7584

Re-examination of the approximate methods for interconversion

between frequency- and time-dependent material functions
I. Emri a, , B.S. von Bernstorff b , R. Cvelbar a , A. Nikonov a
a Center for Experimental Mechanics, University of Ljubljana, Cesta na Brdo 49, SI-1000 Ljubljana, Slovenia
b BASF, Carl-Bosch-Strasse 38, Ludwigshafen, Germany

Received 4 October 2004; received in revised form 28 May 2005; accepted 28 May 2005

Abstract

The paper examines the correctness of the best-known approximate methods of interconversion between the frequency- and the time-
dependent material functions. Approximate interconversions are compared to the close-form viscoelastic interrelations through the relaxation
and/or retardation spectra. The analysis showed that the simple method, G(t)  G ()|=1/t , should be avoided. The most successful was the
method of Schwarzl yielding results with maximum relative error within 2%. The magnitude of the error of interconversion is related to
the magnitude of the response function first derivative. When the first derivative = |d(log G ())/d(log())| < 0.5 all approximate methods
except the simple method furnish interconversions within the acceptable error, i.e., less than 5%.
2005 Elsevier B.V. All rights reserved.

Keywords: Interconversion; Material functions; Material characterization

1. Introduction excitation (displacement or force), are interrelated in a close

Polymers are becoming increasingly important materi-
als in mechanical-, electrical- and civil-engineering. In such
applications, materials are expected to carry loads over
extended period of time. This requires means of predict-
ing their long-term reliability, which furthermore demands
knowledge of viscoelastic material functions. To determine
material functions in time-domain we need, in general, six
independent experiments, three for force (or stress) excita-
tion and three when the excitation is displacement (or strain).
In addition, we need the same number of experiments to
determine material functions in frequency-domain (dynamic
material functions). These material functions are listed in
Table 1.
Measurements in frequency-domain are common for char-
acterization of melts, while the time-domain experiments are
usually used for characterization of solids. Material func-
tions in time and frequency-domain, within a given mode of
Corresponding author.
E-mail address: ie@siol.net (I. Emri).
form via the corresponding relaxation and retardation spec-
trum. The two spectra are not measurable directly; they must
be calculated from the appropriate response function, mea-
sured either in time or frequency-domain. These calculations
require solution of an inverse problem, which happens to be
ill-posed. Until recently, there was no appropriate solution
for these problems. Mainly for that reason several approx-
imate methods for the interconversion between frequency-
and time-dependent material functions have been developed
in the past. Many of these algorithms are still in use, usually
as part of the software packages supporting different appa-
ratuses for the viscoelastic material characterization, e.g.,
rheometers and DTMA apparatuses. Most of these com-
mercial apparatuses are dynamic, i.e., they measure mate-
rial functions in the frequency-domain. The time-domain
response is then predicted using one of the approximate algo-
rithms [1].
The interrelations between frequency- and time-domain
material functions are schematically presented in Fig. 1 [1].
The ultimate goal of this paper is to examine the correct-
ness of the approximate methods of interconversion between

0377-0257/$ see front matter 2005 Elsevier B.V. All rights reserved.
doi:10.1016/j.jnnfm.2005.05.008
76 I. Emri et al. / J. Non-Newtonian Fluid Mech. 129 (2005) 7584

Table 1
Time- and frequency-dependent viscoelastic material functions
Mode of loading Time-dependent Frequency-dependent

Modulus Compliance Modulus Compliance

Shear G(t) J(t) G () G () J () J ()
Volumetric K(t) B(t) K () K () B () B ()
Uniaxial E(t) D(t) E () E () D () D ()
Poissons ratio (t)  ()  ()

kind, which is an ill-posed problem. Until recently [214],

we had no stable solution for this group of problems. Thus,
for the interconversion between the frequency- and the time-
dependent material functions many approximate methods
have been developed in the past. Some of these methods are
still in use, mostly in the industrial laboratories. We examine
here some of the most popular algorithms.

2.1. Conversion from frequency- to time-dependent

functions

The simplest approximation to G(t) and J(t) using the real

part of the frequency-dependent modulus, G (), and com-
pliance, J (), is [16]:
Fig. 1. The interrelations between frequency- and time-dependent material
G(t)  G ()|=1/t , (1)
functions.

the frequency- and the time-dependent material functions. and

We therefore compare the approximate interconversions to
J(t)  J  ()|=1/t . (2)
the close-form viscoelastic interrelations through the discrete
relaxation and/or retardation spectra. The latter can be now For the compliances similar interrelation was proposed by
readily calculated using one of the algorithms for calcula- Riande and Markovitz [17] and by Koppelman [18]:
tion of mechanical spectra from the dynamic and/or static
response functions, e.g., [211]. J(t)  J()|
=1/t , (3)
We will first examine the approximate interrelations
between frequency- and time-dependent material functions where
[1225], using synthetic data generated from the known dis-

crete spectrum. We carefully examine the effect of the shape J()
= (J  ())2 + (J  ())2 . (4)
of the spectrum on the accuracy of the interconversion. Next,
we analyze the accuracy of approximate methods for four dif- Christensen [12] has proposed slightly modified algorithm
ferent materials, i.e., PVAc, NR, EPDM and PA66 [2628]. for prediction of G(t) and J(t) from the frequency-dependent
modulus, G (), and compliance, J (). He replaced fre-
quency by = 2/t to obtain:
2. Approximate interrelations G(t)  G ()|=2/t , (5)
Mechanical spectrum cannot be measured directly. It has and
to be calculated from one of the response functions, usu-
ally from the harmonic (dynamic) response functions, e.g., J(t)  J  ()|=2/t . (6)
G () and G (). Dynamic measurements are most widely
used in industry, because they are easily performed on one of Ninomiya and Ferry [19,29] developed an algorithm for cal-
the commercially available apparatuses.1 Calculation of the culating G(t) and J(t) that comprises contributions from the
relaxation and retardation spectra requires an inverse solu- real and the imaginary part of the dynamic modulus and
tion of the Fredholm integral equation of the first or second dynamic compliance, respectively,

1 G(t)  [G () 0.4G (0.4) + 0.014G (10)]=1/t , (7)

It has to be noted that due to the heat dissipation, the accuracy of these
measurements may be a weak point, particularly when experiments are per-
formed in the vicinity of glass-transition temperature. J(t)  [J  () + 0.4J  (0.4) 0.014J  (10)]=1/t . (8)
 I. Emri et al. / J. Non-Newtonian Fluid Mech. 129 (2005) 7584 77

Schwarzl and Struik [20] obtained several approximations of and

similar form. One, which is most often used, is:
G ()  0.470G(4t) 2.144G(2t) + 1.476G(t)
  t t t
G(t)  G () 0, 337G (0, 323)|=1/t . (9)
0.422G + 0.608G 0.160G
In the same paper, they proposed also an approximation to 2 4 8
 t 
G(t) derived solely from G ():
+ 0.172G |t=1/ . (16)
16
G(1.44t)  G () 0, 4[G (1, 59) G (0, 193)]|=1/t ,
Relations for J () and J () may be again obtained through
(10)
the substitutions (14). Similar relations were proposed by
which is however less precise. Schwarzl [22,31] developed Yagii and Maekawa [23,29]:
several approximations for calculation of time-dependent
G ()  G(t) + 1.080[G(1.585t) G(2.512t)]
material functions from the corresponding frequency-
dependent functions. For those cases when damping, tan , + 0.159[G(0.251t) G(0.398t)]|t=1/ , (17)
is small he proposed a simple formula:
and
G(t)  G () 0.566G (0.5) + 0.203G ()|=1/t ,
G ()  2.7[G(0.631t) G(t)]
(11)
and for all other cases, a more complex relation: + 0.794[G(0.1t) G(0.159t)]|t=1/ . (18)
 
G(t)  G () 0.00807G 0.00719G They have also proposed relations for the frequency-
16 8 dependent (dynamic) creep compliance functions:
 
+ 0.00616G 0.467G + 0.0918G () J  ()  J(t) + 1.08[J(1.585t) J(2.512t)] + 0.159
4 2
+ 0.0534G (2) 0.08G (4) + 0.0428G (8)|=1/t , [J(0.251t) J(0.398t)] + 0.025{f t}|t=1/ , (19)
(12) and
or
 J  ()  2.7[J(t) J(0.631t)] + 0.794[J(0.159t)
 
G(t)  G () 0.496G 0.0651
2 J(0.1t)] + 0.043{f t}|t=1/ . (20)
      
G G 0.0731 G G () The curly brackets in Eqs. (19) and (20) denote presence or
4 2 2
absence of the corresponding physical quantity, depending
0.111[G () G (2)] 0.03[G (8) G (16)] on the arrheodictic,2 or rheodictic behavior of the material
0.00683[G (32) G (64)]|=1/t . (13) [29].
Plazek and Raghupathi [25,29,30] proposed relations for
The relations for the creep functions in Eqs. (11)(13) may the frequency-dependent creep compliance, which takes into
be obtained through the substitutions: account the slope of the time-dependent creep compliance
G(t) J(t); G () J  (); function:

G () J  (). (14) J  ()  [1 m(2t)]0.8 Jr (t)|t=1/ , (21)

   0.8

There are of course many approximations in opposite direc-

2 1

tion, i.e., predictions of frequency-dependent material func- J  ()  m t Jr (t) + 0

, (22)
3

tions from the corresponding time-dependent ones. We t=1/

review those below. where
t
2.2. Conversion from time- to frequency-dependent Jr (t) = J(t) , (23)
functions 0
d(log Jr (t))
Let us start with one of the approximate relations proposed m= . (24)
d(log t)
by Schwarzl [22,31]:
It should be noted that when the slope of the creep compliance
G ()  0.142G(8t) 0.86G(4t) + 0.674G(2t) function, J(t), is small then the loss tangent, tan , becomes
t t
+ 0.942G(t) + 0.001G + 0.101G
2 4
t  t  2 The term rheodictic refers to a material showing steady-state flow and

0.00855G + 0.00855G |t=1/ , (15) arrheodictic denotes a material which does not ([29], p. 93).
8 16
78 I. Emri et al. / J. Non-Newtonian Fluid Mech. 129 (2005) 7584

independent of frequency, and may be approximated as:

d(log Jr (t))
tan  . (25)
2 d(log t)
Schapery and Park [15] recently developed new relations:

G ()   G(t)|=1/t , and G ()   G(t)|=1/t ,

(26)

where
 
 = (1 n) cos n , and Fig. 2. Schematics of the numerical experiments procedure.
2
 
 = (1 n) sin n , (27) on the arrheodictic,3 or rheodictic behavior of the material
2
[29].
with Next, we use the exact frequency response functions as
d(log G(t)) a starting point to predict the time-dependent response func-
n= , (28) tions, Gap (t), using the approximate relations (1), (5), (7), (9),
d(log t) (12) and (13). We used the subscripts ex and ap to indicate
which is a slowly varying function (1 < n < 1) and is a the so-called exact and approximate response functions,
Gamma function. respectively. The goodness of the approximate interconver-
sions we analyze by calculating the relative error:
Gap (t) Gex (t)
3. Numerical experiments = , (32)
Gex (t)
We first examine the approximate interrelations between and the average relative error:
frequency- and time-dependent material functions using syn- n

thetic data generated from the known discrete spectrum 1 

Gap (ti ) Gex (ti )

=



. (33)
Hex (). Next, we analyze the accuracy of the approxi- n Gex (ti )
i=1
mate methods using measured relaxation functions, G(t),
for four different materials. From them, we first calculate This scheme of analysis is schematically presented in Fig. 2.
discrete spectrum Hex () using EmriTschoegl algorithm
[610]. As in previous case, we consider that Hex () is the 3.1. Synthetic spectra
correct known spectrum. Using the spectra, we gener-
ate the exact response functions in the frequency-domain We start the accuracy analysis of the approximate inter-
[29]: conversions with known synthetic spectra with different
distributions: (i) box, HB (), (ii) wedge, HW (), (iii) ramp,
i=n
 i=n

2 i2 1 HR () and (iv) Lorentzian, HL (). In all four cases, we have
Gex () = {Ge } + Hi = G g Hi , generated 57 spectrum lines, ranging from log = 14 s to
i=1
1 + i
2 2
i=1
1 + 2 i2
log = 14 s, i.e., two lines per decade, using Gg = 109 Pa and
(29)
Ge = 99900.999 Pa as the glassy and the equilibrium modu-
lus, respectively. Strengths of the spectrum lines were in all
i=n
 i cases normalized according to:
Gex () = Hi , (30)
1 + 2 i2 i=57
i=1 
H i = Gg G e . (34)
and the time-domain, Gex (t): i=1
i=n
  
t According to this we have:
Gex (t) = {Ge } + Hi exp  
i
i=1 H
i
   H() = 57 (Gg Ge ), i ; i = 1, 2, 3, . . . , 57 ,
j=1 Hj
i=n

t
= Gg Hi 1 exp . (31) (35)
i
i=1

The curly brackets in Eqs. (29)(31) denote presence or 3 The term rheodictic refers to a material showing steady-state flow and

absence of the corresponding physical quantity depending arrheodictic denotes a material which does not ([29], p. 93).
 I. Emri et al. / J. Non-Newtonian Fluid Mech. 129 (2005) 7584 79

for the Lorentzian distribution. The envelopes of the four

spectra are shown in Fig. 3.
Using the four spectra we can now generate the exact
response functions in the frequency-, Gex () and Gex () and
the time-domain, Gex (t), using the Eqs. (29)(31) respec-
tively. The exact response functions corresponding to the
four spectra were calculated for the logarithmic frequency-
and time-span ranging from 12 to +12, which is two decades
shorter on both sides than the corresponding spectrum to
account for the truncation error. The exact response func-
tions are shown in Fig. 4.
Starting from the exact frequency-dependent response
Fig. 3. Envelopes of the four spectra: HB (), HW (), HR (), HL (). functions, G () and G (), we can now calculate the corre-
sponding time-dependent material functions, Gap (t), using
where six different approximate interrelations, which we named
Gg Ge as: Simple (1), Christensen (5), Ninomiya and Ferry (7),
H
i = HB (i ) = , for the box distribution, (36) Schwarzl and Struik (9), Schwarzl2 (12) and Schwarzl3 (13),
57
respectively. The goodness of the approximate predictions,
i = HW (i ) = 109 i0.5 ,
H for the wedge distribution, expressed as relative-error are presented in Fig. 5.
From each of the four diagrams, one may extract the max-
(37) imum relative error, which is shown as bar diagram in Fig. 6a.
In Fig. 6b, we also show the corresponding average relative
9 1.35
10 i ; for logi < 6

Hi = HR (i ) = 7.94328; for 6 logi 6 ,
for the ramp distribution, and (38)

9 1.35
10 i ; for logi > 6

error calculated from the Eq. (33). It is interesting to

i = HL (i ) =  r 2  r ,
H with 0 = 1 and r = 0.5, note that the shape of the response function affects the
i
0 + 0i maximal relative error and the averaged relative error
(39) differently.

Fig. 4. Stress relaxation functions, G(t), storage, G () and loss moduli, G (), corresponding to different spectra.
80 I. Emri et al. / J. Non-Newtonian Fluid Mech. 129 (2005) 7584

Fig. 5. Comparison of different approximate interconversions of the response functions in terms of the relative error .

3.2. Interconversion of experimental data
We now proceed with the analysis of the approximate
interconversions by using our own experimental data on
shear relaxation modulus, G(t), measured on four different
materials: PVAc, NR, EPDM and PA66. The time-dependent
response functions are displayed on the left-hand side in
Figs. 710. Details of the experimental procedures and data
reduction are presented and discussed elsewhere [2628].
From the time-dependent response functions, we first cal-
culate the corresponding relaxation spectra, H(), using the
algorithm proposed by Emri and Tschoegl [6,10]. The cor-
rectness of the calculated spectra was checked by calcu-
lating back the shear relaxation functions, G(t), using Eq.
(31). The maximum relative error was in all cases less than
0.5%. The four spectra are shown on the right-hand side in
Figs. 710.
From the calculated spectra, we now again calculate the
exact frequency-dependent material functions Gex () and
Gex (), using Eqs. (29) and (30), which are not shown. The
frequency-dependent response functions Gex () and Gex (),
served as a starting point to predict the time-dependent
response functions, Gap (t), using the approximate relations
(1), (5), (7), (9), (12) and (13), as schematically presented in
Fig. 2.
The relative errors of the approximate interconversions are
presented in Fig. 11. In the error analysis, we have skipped
one decade on both sides of the response function to avoid the
effect of the truncation error resulting from the calculation of
spectra.
From each of the four diagrams, we can again extract the
maximum relative error, which is shown as bar diagram in
Fig. 12a. In Fig. 12b, we show the corresponding average
relative error calculated from the Eq. (33).

Fig. 6. Comparison of approximate interconversions, in terms of the maximum relative error, max (a) and in terms of the average relative error,
(b).
 I. Emri et al. / J. Non-Newtonian Fluid Mech. 129 (2005) 7584 81

Fig. 7. The relaxation function, G(t,T), on PVAc (a) and the corresponding relaxation spectrum, H() (b).

Fig. 8. The relaxation function, G(t,T), on NR (a) and the corresponding relaxation spectrum, H() (b).

Fig. 9. The relaxation function, G(t,T), on EPDM (a) and the corresponding relaxation spectrum, H() (b).

Fig. 10. The relaxation function, G(t,T), on PA66 (a) and the corresponding relaxation spectrum, H() (b).
82 I. Emri et al. / J. Non-Newtonian Fluid Mech. 129 (2005) 7584

Fig. 11. Comparison of different approximate interconversions of the PVAc, NR, EPDM and PA66 frequency-response functions, in terms of the relative error
.

Fig. 12. Comparison of different approximate interconversions of the material response functions, presented with the maximum, max (a) and the average
relative error,
(b).

4. Discussion and conclusions
The first set of analysis was performed on synthetic data
generated from the four different synthetic spectra. In order
to minimize the truncation error, the time span of spectra
was chosen to be four decades broader than the correspond-
we have generated two additional response functions using
the wedge and the Lorentzian shaped spectra.
The analysis showed that the error of interconversion in
general corresponds to the first derivative of the response
function:

d(log G ())

ing response functions (see [6] for the detailed analysis of =

(40)
d(log())

this problem). The spectra have been selected such that the
corresponding response functions mimic the shape of the
most commonly used polymers in solid and molten state, i.e.,
very slowly and very rapidly decreasing response functions
in respect to the logarithmic time scale.
The slowest and the fastest response functions corre-
spond to the box and ramp shaped spectra. Between the two
The derivatives of the response functions are displayed in
Fig. 13.
Comparing Figs. 5 and 13 shows that the location of the
maximum error for each of the four response functions coin-
cides with the location of the maximum of the response
function derivative, max . The latter may be correlated with
 I. Emri et al. / J. Non-Newtonian Fluid Mech. 129 (2005) 7584 83

ative error in interconversions of experimental response

functions, as function of the corresponding first derivative
maximum.
Fig. 15 confirms that the error of interconversion for
all approximate methods except the simple method remains
within the acceptable range when, = |d(log G ())/
d(log())| < 0.5.
From the presented analysis, several useful conclusions
may be drawn:

(i) The so called simple method, G(t)  G ()|=1/t , should

Fig. 13. First derivatives of the response functions.
(iii) The location of the response function first derivative
(iv) The magnitude of the error of interconversion is
Fig. 14. Maximum relative error as function of the maximum first derivative
of the synthetic response functions.
the maximum relative error, max (see Fig. 6), as shown in
Fig. 14.
From Fig. 14, we may conclude that all analyzed approx-
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NR, EPDM and PA66. Fig. 15 shows the maximum rel-
Fig. 15. Maximum relative error as function of the maximum first derivative
of the experimental response functions.
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