Acta Mech 232, 2347–2359 (2021)

https://doi.org/10.1007/s00707-021-02946-1

O R I G I NA L PA P E R

Teng Su · Hongwei Zhou · Jiawei Zhao · Zelin Liu ·

Daniel Dias

A fractional derivative-based numerical approach

to rate-dependent stress–strain relationship for viscoelastic
materials

Received: 7 August 2020 / Revised: 9 January 2021 / Accepted: 20 January 2021 / Published online: 29 March 2021
© The Author(s), under exclusive licence to Springer-Verlag GmbH, AT part of Springer Nature 2021

Abstract Strain/stress-controlled loading, loading–unloading, loading-relaxation (or creep), and correspond-

ing cyclic tests are essential for characterizing the viscoelastic materials’ rate-dependent stress–strain relation-
ship. A three-parameter model is proposed based on the basic definition of fractional derivative viscoelasticity
and time-varying viscosity. This model is applied to many complex loading conditions. The solutions for three
monocyclic loading conditions are given and then further generalized to arbitrary linear loading conditions,
which are assumed to be first-order functions of time. The generalized solution for the arbitrary linear loading
path is validated by modelling the mechanical response of cyclic loading–unloading and loading–relaxation (or
creep) tests. Four sets of experimental data for polymer materials are employed to demonstrate the proposed
fractional derivative model’s efficiency. The results show that it can accurately model strain/ stress-controlled
response under various loading conditions using only three parameters. The model is then implemented in
numerical software to explore its capacity further, and the simulation results show that it also succeeds in
simulating cyclic loading–unloading tests.

1 Introduction

Experimental tests are usually carried out to understand the material properties better, and prediction models
based on experimental data are proposed. Classical mechanics classified materials into categories according
to the observed behaviours. Haupt [1] suggests a classification based on the material properties such as strain
rate dependency, hysteresis effect, and equilibrium relation. First, using tests loaded at different constant
strain rates, two categories can be distinguished: materials that are rate-independent or rate-dependent. If
the material stress–strain relationships are rate-independent, loading–unloading tests should be performed to
examine the existence of a hysteresis. The material with rate-independent hysteresis has a persistent memory
of its loading history that remains after the transients disappear [2]. In the case of rate-dependent materials,
they must possess hysteresis. It may be caused by the friction inside the material combined with persistent
deformations. According to the cause of hysteresis, there are two further possibilities for the rate-dependent
T. Su · J. Zhao · Z. Liu
School of Mechanics and Civil Engineering, China University of Mining and Technology,
Beijing 100083, People’s Republic of China
H. Zhou (B)
School of Energy and Mining Engineering, China University of Mining and Technology,
Beijing 100083, People’s Republic of China
e-mail: zhw@cumtb.edu.cn
T. Su · D. Dias
Laboratory 3SR, Grenoble Alpes University, Grenoble, France
D. Dias
Antea Group, Antony, France
2348 T. Su et al.

materials: an equilibrium hysteresis can exist or not. Equilibrium curves can be obtained only when the input
process is infinitely slow, which is rigorously not possible. The loading with intermediate holding times is
the alternative method to obtain the equilibrium curve in practical experiments. Thus, it can be concluded
that linear loading, loading–unloading, loading-holding tests, and their corresponding cyclic tests are the most
common and necessary experiments to characterize materials.
According to experimental observations, four categories can be recognized: (1) elasticity able to represent
the rate-independent materials without a hysteresis; (2) plasticity referring to materials possessing time inde-
pendency and hysteresis; (3) rate-dependent viscoelastic materials where no equilibrium hysteresis occurs;
(4) rate-dependent viscoplastic materials with a hysteresis. These four different categories motivate four dif-
ferent corresponding mathematical modelling theories. Although many tests were already done, it is still
challenging to characterize the observed behaviours accurately and systematically, especially for viscoelastic
and viscoplastic materials. Based on the mechanical model theory, the compression behaviour of high-density
polyethene (HDPE) was modelled by Bodner’s model [3]. The results showed that even though the loading,
creep, and relaxation behaviour were captured well, Bodner’s model could not accurately predict the unloading
behaviour. The difficulty in modelling the unloading path was also emphasized by Brusselle-Dupend et al.
[4], whose visco–elastoplastic model used 23 parameters to capture the unloading path. Modifying the Zener
model, a nine-parameter model was proposed, capable of correctly fitting the whole tensile curve, including the
loading–unloading path and loading–relaxation–unloading path [5]. A ten-parameters hyper-visco-hysteresis
model was proposed by Zrida et al. [6]. The comparison results with experimental data showed that it could
be adequate to describe the stress–strain evolution of polymers under various mechanical loadings such as
loading–unloading and torsion tests.
Obviously, in the modelling process, two problems gradually emerge. The first one is that many models can
be used but only under certain loading conditions and fail to model complex loading conditions. The second
one concerns the fact that more parameters are often introduced to obtain a better fitting effect, resulting in an
unclear physical meaning for these parameters and difficulties in obtaining analytical solutions or numerical
calculations. Considering rheology, researchers like Gemant [7], Scott-Blair [8], Slonimsky [9], Smit and
de Vries [10], Bagley and Torvik [11, 12], Koeller [13], Schiessel et al. [14], Schmidt and Gaul [15], and
Jiang [16] used fractional operators to frame the viscoelastic problem. Ref. [17] claimed that the fractional
calculus could capture complex phenomena with very few parameters. Xu and Jiang [18] considered that
the fractional operators are powerful tools for modelling viscoelastic behaviours, particularly for the time-
dependent constitutive model, because of the long history dependency or so-called memory effects. Obviously,
as mentioned above, the time-dependent mechanical responses (i.e., creep and relaxation) can be categorized
as special cases of the rate-dependent stress–strain relationship. However, to our knowledge, the fractional
operators have not been applied into the modelling of rate-dependent stress–strain relation. Motivated by the
advantage of the fractional operator in describing time-strain and time-stress relationships, this research work
further explores its capability in modelling the time-stress–strain relationship.
This paper uses a fractional operator to model the loading-rate-dependent stress–strain relationship of
viscoelastic materials based on the basic definition of viscoelasticity. A fractional constitutive model with time-
varying viscosity is proposed considering the thixotropy and rheopexy of viscoelastic materials. The analytical
solutions of various stress (strain)-controlled loading conditions are presented. Four sets of experimental data
for polymers are employed to demonstrate the proposed fractional derivative model’s efficiency. The model’s
capacity is further studied by simulating material behaviour under cyclic loading–unloading conditions using
a numerical method.

2 Definitions

2.1 Definition of viscoelasticity from the fractional perspective

The aforementioned classification under constant strain rate loading is qualitatively sketched in Fig. 1. When
|ε̇| > 0, the stresses of viscoelastic materials are related to both the strain and strain rates. In the linear
viscoelastic theory, the mechanical properties of a purely elastic solid can be expressed as a spring element,
and a dashpot can express the mechanical properties of a purely viscous fluid. The relation between stress σ
and strain ε for these two mechanical elements can be described as follows:

σ Eε, spring,
(1)
σ με̇, dashpot.
A fractional derivative-based numerical approach to rate-dependent stress–strain relationship for viscoelastic materials 2349

Fig. 1 Four different classes of material response

where E is the spring elastic modulus and μ is the dashpot viscous modulus.
From the integral-based differential aspect, Eq. (1) can be rewritten as
⎧
⎪
⎪ d 0 ε(t)
⎨ σ E , spring,
dt 0 (2)
⎪
⎩ σ μ d ε(t) , dashpot.
1
⎪
dt 1
As shown in Eq. (2), the stress of elastic solid is proportional to the zeroth-order derivative of strain. The
stress of Newtonian fluid is proportional to the first-order derivative of strain. It can be concluded that the stress
of the viscoelastic material is proportional to the non-integer strain. Based on Eq. (2), the general constitutive
equation of viscoelasticity can be written as
dγ ε(t)
σ (t)  η , 0 <γ < 1, (3)
dtγ
where σ (t) and ε(t) are, respectively, the time-dependent stress and strain; γ is the fractional derivative order,
and η is the modulus for viscoelasticity, which influences the strain or stress response magnitude.

2.2 Definitions of fractional integrals and derivatives

There are several definitions for fractional integrals and derivatives. The Riemann–Liouville and the Caputo
ones are the most commonly used.
Let   [a, b] (0 < a < b < ∞) be a finite interval on the real axis R+ . The Riemann- Liouville fractional
γ
integral a+ It y of order γ ∈ C ( (a) > 0) is defined as
 γ  1 t y(τ )
a+ It y (t)  dτ, (t > a), (4)
(γ ) a (t − τ )1−γ
γ
and the Riemann–Liouville fractional derivatives a+ Dt y of order γ ∈ C ( (a) > 0) is defined by
 γ  d m m−γ 1 dm t y(τ )
a+ Dt y (t)  a+ It y (t)  dτ, (t > a). (5)
dx (m − γ ) dt a (t − τ )1+γ −m
m

γ
a+ Dt y of order γ ∈ C ( (a) > 0) is defined by
The Caputo’s fractional derivative C
γ 1 t y (m) (τ )
C
a+ Dt y (t)  dτ, (t > a), (6)
(m − γ ) a (t − τ )1+γ −m
where t  a is the starting
 +∞ x−1point, m is the integer satisfying m − 1 ≤ γ < m and  is the Euler gamma function
defined by (x)  0 t e−t dt for x > 0.
2350 T. Su et al.

Fig. 2 Loading patterns: a Monotonic loading b loading-holding c loading–unloading experiments

3 Fractional derivative constitutive models and analytical solutions

Experiments on viscoelastic materials (e.g. cellulose, epoxy resin, semisolid food, and salt) exhibited time-
varying non-Newtonian viscous characteristics, namely, thixotropy and rheopexy [19, 20]. Thixotropy means
a viscosity that decreases with time, while rheopectic materials show an opposite characteristic [21]. Yin [22]
indicated that some predictive results of fractional models are not ideal. The model supposes the invariability
of materials’ mechanical properties while these features are changing during the deformation or loading.
To solve this problem, a few researchers carried out some studies on time-varying viscosity. Buckingham
[23] proposed a modified Maxwell model with a linear time-varying viscosity to explain the strain hardening
mechanism within the grains. Pandey and Holm [24] extended the work of Buckingham. They found that
the modified Maxwell model’s relaxation modulus and creep compliance are similar to a fractional dashpot’s
stress response and the Lomnitz’s creep law. Based on experimental observations of salt rock, Zhou et al. [25]
introduced exponentially time-varying viscosity into the Scott-Blair model to model viscoplastic deformation
of salt rocks. Using the Boltzmann superposition, the exponentially time-varying viscosity Scott-Blair model
can model the nonlinear viscoelastic and viscoplastic properties of various materials [26–29]. Yang et al. [21]
proposed a power-law viscosity and compared it with linearly varying viscosity and exponentially varying
viscosity. The comparison results showed that the power-law viscosity and exponentially varying viscosities
are more universal and capable of characterizing both thixotropy and rheopexy. Due to the exponential law’s
excellent characteristic in the solving process, the exponentially time-varying viscosity η(t)  e−wt η0 is
introduced into Eq. (3), which can then be formulated as
dγ ε(t)
σ (t)  e−wt η0 , 0 <γ < 1, (7)
dtγ
where γ ∈ [0, 1] denotes the material viscoelasticity, and w is an empirical parameter controlling the viscosity
monotonicity and variation rate. For γ , the material is more elastic for γ → 0 and more viscous for γ → 1.
When w is positive, the viscosity decreases with time, representing thixotropy; when w is negative, viscosity
is positively correlated with time, referring to rheopexy.
Following the material classification, loading conditions such as constant loading rate, loading–unloading,
loading-relaxation (or creep), and their corresponding cyclic tests are employed to test the model’s capacity
of characterizing viscoelastic materials’ rate-dependent stress–strain relationships. The analytical solutions of
Eq. (7) are given by substituting various conditions.

3.1 Constant-rate loading

Constant strain rate compression and tension are the most common tests. Monotonic tests at multiple constant
strain rates are performed, and any differences between the stress–strain curves are obtained, indicating the
strain rate dependence of the material behaviour. For constant strain rate loadings, as shown in Fig. 2a, the
strain applied increases linearly with the strain rate c,
ε(t)  ct, t ≥ 0. (8)
Substituting Eq. (8) into (7), one can obtain
η0 c d t η0 ct 1−γ
σ (t)  e−wt (t − τ )−γ τ dτ  e−wt , t ≥ 0. (9a)
(1 − γ ) dt 0 (2 − γ )
A fractional derivative-based numerical approach to rate-dependent stress–strain relationship for viscoelastic materials 2351

Equation (9a) can also be rewritten as stress–strain form as follows:

η0 cγ ε(t)1−γ
σ (t)  e−wt , t ≥ 0. (9b)
(2 − γ )
Constant-stress rate tests are also discussed, though stress-controlled loading is only commonly performed
on strain hardening materials. The loading path can be expressed as
σ (t)  ct, t ≥ 0. (10)
Substituting Eq. (10) into (7) leads to
c t c 1+γ 2
ε(t)  (t − τ )γ −1 τ ewt dτ  t E 1,2+γ (wt), t ≥ 0, (11a)
η0 (γ ) 0 η0
and the stress–strain form of Eq. (11a) is
c−γ σ (t)
ε(t)  σ (t)1+γ E 1,2+γ
2
w , t ≥ 0. (11b)
η0 t

3.2 Loading-relaxation (or creep)

The characterization of the strain rate or stress rate dependence is then accomplished by holding the load
(relaxation or creep), which is used to obtain equilibrium points. Relaxation and creep are also two critical
rheological behaviours. In real experiments, the input of relaxation or creep is also a constant-rate loading ramp
followed by a constant strain or stress because the experimental set-up limits the loading velocity. Figure 2b
shows that the input of this loading mode can be divided into two segments: an initial ramp at a constant
loading rate c during [0, t 1 ] and the creep or relaxation, which is expressed as

ε(t)  ct, 0 ≤ t ≤ t1 ,
(12)
ε(t)  ct1 , t1 <t.
or

σ (t)  ct, 0 ≤ t ≤ t1 ,
(13)
σ (t)  ct1 , t1 <t.
Substituting Eq. (12) into (7), one can obtain
⎧
⎪ η0 c d t
⎪
⎪ σ (t)  e−wt (t − τ )−γ τ dτ
⎪
⎪ (1 − γ ) dt
⎪
⎪
0
⎪
⎪ η 1−γ
⎪
⎪ ct
 e−wt
0
⎨ , 0 < t ≤ t1 ,
(2 − γ ) (14)
⎪
⎪ η0 c d t1 t
⎪
⎪ σ (t)  e−wt (t − τ )−γ τ dτ + (t − τ )−γ t1 dτ
⎪
⎪ (1 − γ )
⎪
⎪ dt 0 t
⎪
⎪ η0 c
1
⎪
⎩  e−wt (t 1−γ − (t − t1 )1−γ ), t > t1 .
(2 − γ )
Substituting Eq. (13) into (7) yields
⎧ t
⎪ c
⎪ ε(t) 
⎪ (t − τ )γ −1 ewτ τ dτ
⎪
⎪ η (γ )
⎪
⎪
0 0
⎪
⎪ c
⎪
⎪  t 1+γ E 1,2+γ2
(wt), 0 < t ≤ t1 ,
⎨ η0
t1 t (15)
⎪
⎪ c γ −1 wτ ct1
⎪
⎪ ε(t)  (t − τ ) e τ dτ + (t − τ )γ −1 ewτ dτ
⎪
⎪ η (γ ) η (γ )
⎪
⎪
0 0 0 t 1
⎪
⎪ 1+γ wt1
⎪
⎩ ct ce
 2
E 1,2+γ (wt) − (t − t1 )1+γ E 1,2+γ
2
(w(t − t1 )), t > t1 .
η0 η0
Equations (14) and (15) are the solutions for strain- and stress-controlled inputs, respectively.
2352 T. Su et al.

3.3 Loading and then unloading

The first two loading paths are used to obtain the strain or stress rate dependency of materials. Then, the
loading–unloading is usually performed to examine the existence of a hysteresis. With a strain rate c1 for the
loading stage and c2 for the unloading stage, as shown in Fig. 2c, the strain–time relationship is

ε(t)  c1 t, 0 ≤ t ≤ t1 ,
(16)
ε(t)  c1 t1 + c2 t1 − c2 t, t1 <t,

where c1 and c2 are the absolute values of the loading rate.

According to the loading path in Eq. (16), one can obtain the analytical equations of Eq. (7) as
⎧
⎪ η0 c1 t
⎪
⎪ σ (t)  e−wt (t − τ )−γ dτ
⎪
⎪ (1 − γ )
⎪
⎪
0
⎪
⎪ η0 c1 t 1−γ
⎪
⎪
⎨  e−wt , 0 ≤ t ≤ t1 ,
(2 − γ ) (17)
⎪
⎪ η0 t0 t
⎪
⎪ σ  −wt
(t − τ )−γ
(t − τ )−γ (−c2 )dτ
⎪
⎪
(t) e
(1 − γ )
c1 dτ +
⎪
⎪ 0 t
⎪
⎪ η0
0
⎪
⎩ e −wt
(c1 t 1−γ
− (c1 + c2 )(t − t0 )1−γ ), t > t1 .
(2 − γ )

Similarly, the loading condition of the first loading at a stress rate of c1 during [0, t 1 ] and then unloading
at c2 can be expressed as

σ (t)  c1 t, 0 <t ≤ t1 ,
(18)
σ (t)  c1 t1 + c2 t1 − c2 t, t1 <t.

Inserting the loading condition of Eq. (18) into Eq. (7), one obtains
⎧ t
⎪
⎪ c1
⎪
⎪ ε(t)  (t − τ )γ −1 τ ewt dτ
⎪
⎪ η0 (γ ) 0
⎪
⎪
⎪
⎪ c1
⎪
⎪  t 1+γ E 1,2+γ
2
(wt), 0 ≤ t ≤ t1 ,
⎪
⎪ η
⎪
⎪
0
⎪
⎨ 1 t1 t
ε(t)  (t − τ )γ −1 c1 τ ewt dτ + (t − τ )γ −1 (c1 t1 + c2 t1 − c2 τ )ewt dτ
⎪ η0 (γ ) 0 t1
(19)
⎪
⎪  
⎪
⎪ ∞
(k k c t γ +k + 1 − (c + c )(t − t )γ +k + 1 ewt1
⎪
⎪
+ 1)w 1 1 2 1
⎪
⎪ 
⎪
⎪ (k + γ + 2)
⎪
⎪ k0
⎪
⎪
⎪
⎪ c1 (c1 + c2 ) wt1
⎩ = t 1 + γ E 1,2+γ
2
(wt) − e (t − t1 )1 + γ E 1,2+γ
2
(w(t − t1 )), t > t1 .
η0 η0
Equations (17) and (19) are the solutions for strain- and stress-controlled loading–unloading inputs, respec-
tively. The stress–strain equations can be easily obtained by substituting back Eqs. (16) and (18).

3.4 Cyclic loading

The cyclic paths of loading-relaxation or creep are generally used to obtain the equilibrium curves. The cyclic
experiments of loading–unloading inputs are commonly used to study the hysteresis evolution. From the
loading paths mentioned above, defining a generalized loading function for an arbitrary linear loading mode
is essential. It is assumed that the loading path is a first-order function of time, which defined by

n
Fn (t)  cn (t − tn−1 ) + ci−1 (ti−1 − ti−2 ), (20)
i1
A fractional derivative-based numerical approach to rate-dependent stress–strain relationship for viscoelastic materials 2353

where n is the number of changing loads Fn (t) and ci ∈ R is the function of the nth changing load rates.
The value of t -1 , t 0 , c0 is equal to zero. Equation (20) is an arbitrary loading function for both strain- and
stress-controlled inputs.
Substituting Eq. (20) into (7), the generalized stress response expression of arbitrary strain-controlled
loading can be expressed by

⎛ t1 t2 ⎞
⎜ (t − τ )−γ F1 (τ )m dτ + (t − τ )−γ F2 (τ )m dτ + · · ·⎟
η0 ⎜ ⎟
σn (t)  e−wt
0 t1
⎜ ⎟ (21)
(1 − γ ) ⎝ t
−γ ⎠
+ (t − τ ) m
Fn (τ ) dτ
tn−1

where m  1 and Fn (t) is the input function of strain-controlled loading. Thus, the generalized solution for
arbitrary strain-controlled loading is presented by

η0 t1 t2 t
σn (t)  e−wt (t − τ )−γ c1 dτ + (t − τ )−γ c2 dτ + ... + (t − τ )−γ cn dτ
(1 − γ ) 0 t1 tn−1
η0 n−1 ti t
 e−wt (t − τ )−γ ci dτ + (t − τ )−γ cn dτ
(1 − γ ) i1 ti−1 tn−1

η0 
n
 e−wt (ci − ci−1 )(t − ti−1 )1−γ , t > t0 . (22)
(2 − γ )
i1

Substituting Eq. (20) into (7), the generalized strain-response expression of arbitrary stress-controlled
loading can be formulated by

⎛ t1 t2 ⎞
(t − τ )γ −1 F1 (τ )m ewτ dτ + (t − τ )γ −1 F2 (τ )m ewτ dτ...⎟
1 ⎜ ⎜ 0 t1 ⎟
εn (t)  ⎜ ⎟, (23)
η0 (γ ) ⎝ t ⎠
+ (t − τ )γ −1 Fn (τ )m ewτ dτ
tn−1

where m  0 and Fn (t) is the input function of strain-controlled loading. The generalized solution for arbitrary
stress-controlled loading can be presented as

⎛ t1 t2 ⎞
(t − τ )γ −1 F1 (τ )ewτ dτ + (t − τ )γ −1
F2 (τ )e
wτ
dτ...
1 ⎜ ⎜ 0 t1
⎟
⎟
εn (t)  ⎜ ⎟
η0 (γ ) ⎝ t ⎠
+ (t − τ )γ −1 Fn (τ )ewτ dτ
tn−1
 n 

∞ (k + 1)w k (ci − ci−1 )ewti−1 (t − ti−1 )γ +k+1
 i1

(k + γ + 2)η0
k0

1 
n
 (ci − ci−1 )ewti−1 (t − ti−1 )γ +1 E 1,2+γ
2
(w(t − ti−1 )), t > t0 . (24)
η0
i1

The generalized solutions (22) and (24) can be used to model the mechanical responses of cyclic load-
ing–unloading and loading-relaxation or creep tests, where each cycle consists of two segments, namely, a
relationship 2N  n for a cycle number N and a load changing number n.
2354 T. Su et al.

4 Experimental validation and numerical simulation

To systematically validate the analytical solutions for various loading conditions, four sets of experimental
data in Refs. [6, 30–32] for polymers are employed, and all previously mentioned loading conditions are
included. The Lsqcurvefit function using the Levenberg–Marquardt algorithm in MATLAB is employed to fit
the experimental data. Lsqcurvefit function can solve nonlinear curve-fitting (data-fitting) problems in the least-
squares sense. For further details on this function, interested readers are invited to refer to [33]. Besides, the
expressions are programed into MATLAB, and the response of cyclic loading–unloading inputs are simulated.
The corresponding fitting and simulation results are given in the following subsections.

4.1 Validation of constant-rate loading

In Refs. [6], monotonic tensile tests are carried out on copolymer polypropylene (PPC7712). The inputs of
tests are strain-controlled loading at rates of 0.001/s, 0.01/s, 0.1/s, respectively. Another strain-controlled
experiment case is a compression test on HDPE [30], carried out at three strain rates: 0.00001/s, 0.0001/s, and
0.001/s. Equation (9) is used to fit these test results. Besides, the compression tests of HDPE were performed
under a stress-controlled loading at a rate of 26.5 N/s and 3.0 N/s, respectively. Equation (11) is used to fit
these test results. Figure 3 shows that the fitting curves using Eqs. (9) and (11) agree reasonably well with
the experimental data under the constant-rate loading. Zhang et al. [30] indicated that HDPE’s maximum test
strains range from 1.8 to 20.7%, but no geometric nonlinearity was observed. Moreover, Zhang et al. [30] and
Colak et al. [34] later modelled the experimental data assuming it is geometrically linear.

4.2 Validation of the loading and then relaxation or creep

In the extension study on PPC7712 [6], a strain rate of 0.001/s was imposed, followed by a relaxation time of
12 h, and stress decreasing with time was shown. In [31], a creep test preceded by an uninterrupted loading (at
a constant stress rate of 1 MPa/s) to 45 MPa was performed on BMI 5250–4 Neat Resin. Equation (14) and
Eq. (15) are used to fit these test results. Figure 4 shows that Eqs. (14) and (15) result in better fitting accuracy
than results in researches [6, 31].

4.3 Validation of loading and then unloading

Strain reversals with the same rate magnitude were conducted after the specimens were compressed to about
15% axial strain at a constant strain rate [30]. The nonlinear behaviours were observed under unloading
conditions. Equation (17) is used to simulate this process. The effect of loading rate was also explored in
loading–unloading tests conducted with constant stress rate magnitudes of 1.0 MPa/s and 0.01 MPa/s at 19 °C
[31]. Equation (19) is used to fit the results. Figure 5 shows that Eqs. (17) and (19) agree well with experimental
data.

4.4 Validation of cyclic loading

A strain-controlled cyclic experiment was carried out on HDPE at the same rate of 0.0001/s during each
loading–unloading-reloading cycle [30]. In this study [6], a three-cycle test was performed on PPC7712. The
specimens were loaded up to a maximum strain of 0.023 with a strain rate of 0.001/s, unloaded down to
null stress with the same strain rate, reloaded up to the maximum strain, etc. Besides, a two-cycle loading-
relaxation test with a preceding rate of 0.001/s was done. Equation (22) is used to fit the results. Besides, the
stress-controlled cyclic experiment is carried out on ultra-high molecular weight polyethene (UHMWPE) in
[32]. The UHMWPE was tested under a uniaxial stress-controlled cyclic loading condition with a stress level
of 6 ± 10 MPa (i.e. the applied mean stress was equal to 6 MPa and stress amplitude was 10 MPa) and at the
stress rate of 5 MPa/s. Equation (24) is used to fit the results. Figure 6 shows that the model behaves correctly
for cyclic loading–unloading experiments. For the loading-relaxation test, it gets excellent fitting accuracy
during the loading stage.
A fractional derivative-based numerical approach to rate-dependent stress–strain relationship for viscoelastic materials 2355

(a) 30 (b) 30

25 25

20 20
Stress (MPa)

Stress (MPa)
15 15
Loading rate Loading rate
0.001/s test simulation 0.00001/s test simulation
10 10
0.01/s test simulation 0.0001/s test simulation
0.1/s test simulation 0.001/s test simulation
5 5

0 0
0.00 0.02 0.04 0.06 0.00 0.02 0.04 0.06 0.08 0.10 0.12 0.14 0.16
Strain Strain

(c) 30

25

20
Stress (MPa)

15

Loading rate
10
26.5 N/s test simulation
3 N/s test simulation
5

0
0.00 0.02 0.04 0.06 0.08 0.10 0.12 0.14 0.16
Strain

Fig. 3 Comparison between experiments and fitting curves for constant-rate loading a Strain-controlled loading on PPC7712 [6].
b Strain-controlled loading on HDPE [30]. c Stress-controlled loading on HDPE [30]

(a) 1.0 (b) 0.030

Prior loading rate 0.001/s 0.028

0.8
Strain level 2.3%
test simulation 0.026
Normalized stress

0.6
0.024
Strain

0.022 Prior loading rate 1MPa/s

0.4
Strain level 45MPa
0.020 test simulation
0.2
0.018

0.0 0.016
0 10000 20000 30000 40000 0 1000 2000 3000 4000
Time (s) Time (s)

Fig. 4 Comparison between experiments and fitting curves for loading-relaxation and creep. a Relaxation on PPC7712 [6].
b Creep on BMI 5250–4 [31]
2356 T. Su et al.

(a) 35 (b) 50
Loading rate Loading rate
30 0.001/s test simulation 1MPa/s test simulation
0.0001/s test simulation 40 0.01MPa/s test simulation
0.00001/s test simulation
25
30
Stress (MPa)

Stress (MPa)
20

20
15

10 10

5
0

0
0.00 0.02 0.04 0.06 0.08 0.10 0.12 0.14 0.16 0.000 0.005 0.010 0.015 0.020
Strain (%) Time (s)

Fig. 5 Comparison between experiments and fitting curves for loading and then unloading. a Strain-controlled loading–unloading
on HDPE [30]. b Stress-controlled loading–unloading on BMI 5250–4 [31]

(a) 25 (b) 20
strain VS stress time VS stress
Loading rate 0.0001/s
test simulation test
20
15 simulation
Stress (MPa)
Stress (MPa)

15
10

10 Loading rate
0.001/s
5

0
0
0.00 0.02 0.04 0.06 0.08 0.000 0.005 0.010 0.015 0.020 0.025 0 30 60 90 120 150
Strain (%) Strain (%) Time (s)

(c) 25 (d) 20 3.0

strain VS stress time VS strain
2.5
20 15 test
simulation
2.0
15
Stress (MPa)

Stress (MPa)

10
Strain (%)

1.5

10
1.0
5
Prior loading rate 0.001/s
Loading rate
5 Strain level 2.3%, 4.8% 0.5
5MPa/s
test simulation
0
0.0
0

-5 -0.5
0 500 1000 1500 2000 0 1 2 3 0 10 20 30 40
Time (s) Strain (%) Time (s)

Cyclic strain loading/relaxation on PPC7712.

Fig. 6 Comparison between experimental and fitting curves for cyclic inputs. (a) Cyclic strain loading/unloading on HDPE
[30]. (b) Cyclic strain loading/unloading on PPC7712 [6]. (c) Cyclic strain loading/relaxation on PPC7712. (d) Cyclic stress
loading/unloading on UHMWPE [32]
A fractional derivative-based numerical approach to rate-dependent stress–strain relationship for viscoelastic materials 2357

Table 1 Model parameters identified from the first cycle of the cyclic strain-controlled experiment

γ (%) w η0 (MPa·sγ )

23.45 1.0710−3 19.835

(a) 40 1-5th 10th 50th

(b) 30
test simulation simulation simulation Experimrntal data Predicted data
30 20
1st
Loading rate
20 0.02/s 10 Loading rate 0.02/s
Stress (MPa)

Stress (MPa)
10
0

0 1-5th
-10 10th
-10 50th

-20
-20

-30 -30
0 1000 2000 3000 4000 7000 8000 39000 40000 -4 -2 0 2 4 -4 -2 0 2 4

Time(s) Strain (%) Strain (%)

Fig. 7 Comparison between experimental and simulation curves for cyclic strain-controlled inputs. a Stress-time relationship.
b Stress–strain relationship

Table 2 Model parameters identified from the first cycle of the cyclic stress-controlled experiment

γ (%) w η0 (MPa·sγ )

17.34 3.8·10–3 8.6637

4.5 Numerical simulations of a cyclic loading

The results show that the constitutive model agrees well with the cyclic loading–unloading data. To further
explore the formulated model’s capabilities, a curve of the N cycles is simulated using the parameters obtained
from the first cycle.
In [32], the cyclic softening/hardening feature of the UHMWPE is shown. The samples were first tested
under strain-controlled cyclic loading conditions with zero mean strain, a strain amplitude of 4%, and a strain
rate of 0.02/s. Equation (22) is used for the simulation. In the first step, the parameters are identified by the
data of the first cycle. The results are presented in Table 1.
Using parameters in Table 1, the strain–time relationships of the 1–5th, 10th, and 50th cycles are simulated.
A comparison between the obtained strain–time curves and experimental results is shown in Fig. 7a. The
strain–time curves are converted to stress–strain curves and re-plotted in Fig. 7b. It is found that simulation
and experiment are in a good overall agreement.
In addition to the strain-controlled cyclic experiments, the UHMWPE was also tested under uniaxial
stress-controlled cyclic loading conditions with a stress level of 10 ± 6 MPa and a stress rate of 5 MPa/s. The
experimental curve of the first cycle is fitted, and the results are shown in Table 2. The parameters are then used
to simulate the stress-time relationship of the 1–5th, 10th, and 50th cycles. In Fig. 8, the stress–time curve for a
cyclic test is compared with experimental observations. The converted stress–strain curve is also plotted. The
comparison in Fig. 8 shows that the overall behaviour can be well reproduced. However, the derived hysteresis
of the rheological model is larger than the one observed in the test, which may lead to prediction errors when
the number of loading cycles increases to a certain value.

5 Conclusions

In this work, a three-parameter fractional model is used to model the time-dependent stress–strain relationship
of the viscoelasticity under constant loading, loading–unloading, and loading-relaxation (or creep) paths.
Considering the thixotropy or rheopexy property of materials, an exponentially varying viscosity is introduced
2358 T. Su et al.

(a) 4.5 (b) 20

Experimrntal data Predicted data
4.0
test simulation simulation simulation Loading rate 5 MPa/s
3.5
Loading rate 5 MPa/s 15
1-5th
3.0 10th

Stress (MPa)
50th
Strain (%)

2.5
1st 10
2.0

1.5

1.0 5
1-5th 10th 50th
0.5

0.0 0
-5 0 5 10 15 20 25 40 45 220 225 0 2 4 0 2 4
Time(s) Strain (%) Strain (%)

Fig. 8 Comparison between experimental and simulation curves for cyclic stress-controlled inputs. a Strain–time relationship.
b Stress–strain relationship

into a fractional viscoelastic model. The rate-dependent stress–strain relationship is first converted into stress-
time or strain–time one by substituting the specific input functions. Then, the solution can be obtained using the
Riemann–Liouville and Caputo definitions. Substituting back the input function, the stress-time or strain–time
solution can be converted back into stress–strain ones. Using this method, the new model’s solutions under
three monocyclic loading conditions are first given and then generalized to an arbitrary linear loading, which is
assumed as a first-order function of time. Four sets of experiments for the polymer are employed, and both stress
and strain-controlled inputs are concluded. The experimental data are fitted and simulated by the proposed
model. It allows showing that the fractional derivative model, with three parameters, can reproduce behaviours
under various loading conditions. Compared with the existing models [3–6], the proposed fractional derivative
model’s main advantage is that it enables to model the mechanical responses of viscoelastic materials under
arbitrary linear loading paths using only three parameters with precise physical meanings.
However, it is noted that the model agrees badly with the second part of each cycle for the cyclic loading-
holding test. It may be because the order here is considered as a constant, which means that the material
viscoelasticity is not variable. This is contrary to lots of experimental observations, which indicated that
viscoelasticity could change with time. Future research will focus on the variable fractional-order model,
which may better fit cyclic loading-relaxation or creep conditions.

Acknowledgements The present work is supported by the National Natural Science Foundation of China 51674266, the State
Key Research Development Program of China 2016YFC0600704, and the Yueqi Outstanding Scholar Program of CUMTB
2017A03.

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