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To cite this article: Harish Lambadi & C. Lakshmana Rao (2019) Monotonic uniaxial and biaxial
electromechanical experiments and modeling of uniaxial stretched polyvinylidene fluoride (PVDF),
Ferroelectrics, 540:1, 41-53, DOI: 10.1080/00150193.2019.1611105
1. Introduction
Piezoelectric materials are a special class of materials that can convert mechanical loads
into free electric charges and vice-versa. Observing electricity when applying mechanical
stretch is called direct piezoelectricity (sensor effect). The direct piezoelectricity was first
discovered in quartz crystals by Jaques and Perry Query in 1880. Later piezoelectricity
was also observed in polymers by Kawai [1]. Kawai investigated the direct piezoelectri-
city in different polymers. Among them, Polyvinylidene fluoride (PVDF) had shown
high direct piezoelectric constant in stretch direction. Piezo polymers which involve
mechanical or electrical stimuli as input, find use in industries for sensing and actuat-
ing purposes.
PVDF is a semi-crystalline polymer and has a basic building block of CH 2 CF 2
monomer. PVDF sheets are extracted from melt extraction of PVDF resin pellets.
Stretching of PVDF sheets at a temperature below the melting point of the PVDF can
change chain packing of the molecules structure (a phase) into the parallel crystal
planes (b phase) [2]. The Beta phase is a dipole-oriented microstructure, the Fluorine
and Hydrogen atoms are negatively and positively charged with respect to the carbon
atoms. Due to this, electric dipoles would form and this look like lamellar crystals in
amorphous background. The net dipole moment becomes zero due to random dipole
directions. To achieve high piezoelectricity, the sheets are conditioned at high tempera-
ture and electric field (electric polling).
Due to the amorphous background and crystal phases, PVDF undergoes large
deformation with the stimuli of mechanical loads. There are two different forms of
PVDF available in the literature [3], uniaxially stretched and biaxially stretched form.
Uniaxially stretched PVDF shows stronger mechanical and electrical properties (along
with the stretch direction) compared to biaxially stretched PVDF.
Uniaxial PVDF film sheets are known to be anisotropic in both mechanical and elec-
tromechanical response. Higher mechanical and electrical properties are reported in
stretched direction compared to orthogonal to stretch direction. Vinogradov et al. [4],
Satyanarayana et al. [5], did experiments on uniaxial and biaxial stretched PVDF, they
observed strong anisotropy in uniaxial stretch directions. Recently, Harish and
Lakshmana Rao [6] have done uniaxial and biaxial tests on dog bone shape and cruci-
form shape specimens respectively. They also reported a strong anisotropy in mechan-
ical response in uniaxially stretched PVDF, found the local strains using speckle
monitoring method and reported the stiffer stress-strain plots compared to the cross-
head movement of the machine. For mechanical response of the PVDF, the slope of the
stress-strain plot (Youngs Modulus) was taken as a property of PVDF for an instantan-
eous elastic response. Harish and Lakshmana Rao [6] attempted to use the polynomial
hyperelastic model to model the nonlinear elastic response of uniaxial PVDF by consid-
ering the anisotropic effects. Boltzmann superposition principle based viscoelastic model
[7] was used to model the time-dependent response of the PVDF. However,
Satyanarayana et al., used the 1D three parameter solid model to model the time-
dependent response of the PVDF.
r ¼ Ce eE;
DE ¼ rE þ ee (1)
Linear coupled piezoelectric equations of the type shown in equation one and are
used for modeling the piezoelectric materials [8]. Here r; D; e; E; C; e; r are stress
and electric displacement, strain, electric field vector, elastic matrix, and material con-
stants respectively. Since the models are to capture only the linear response, same linear
coupled models were used for the PVDF also [9]. The linear piezoelectricity coefficients
(d31 and d32) for PVDF are well archived Dargahi et al. [9]. However, the nonlinear
anisotropic piezoelectric response of direct piezoelectricity is not yet done. In literature,
Richards and Odegard [10], Anna ask et al. [11], developed hyperelastic models for elec-
troactive polymers and electrostrictive polymers for electro-mechanical response predic-
tions. A coupled strain energy density function (which can be additively split into
mechanical and electrical parts) was used to model the coupled electro-mechanical
fields, Piezo polymers like electroactive polymers, and polyurethane were modeled using
strain energy function to fit into their experimental plots. In this paper, we have pro-
posed a similar approach to model an anisotropic electromechanical response of a pie-
zopolymer, when the polymer is subjected to finite deformation.
The nonlinear mechanical and electromechanical response of PVDF is obtained from
the tests using quasi-static charge integration technique. Non-contact speckle monitor-
ing method was used to get local strains. The details of this experimental procedure are
described in Section 2 of this paper. A hyperelastic based approach has been used in
this study to model the non-linear electromechanical response. Model predictions are in
FERROELECTRICS 43
good agreement with the electromechanical test data. Section 3 describes the details of
this model and its usage.
2. Experiments
There are different methods available in the literature to do direct piezoelectricity
experiments. Piezoelectric strain coefficients can be measured using both direct and
converse piezoelectric measurement technique. In the direct method, uniaxial stress is
applied to the piezoelectric sheet and the associated electric charges due to stress is
measured. This method is popular and was adopted to measure the piezoelectric con-
stants of equation 1 by several researchers [12, 13]. In the indirect method, the electric
field is applied to the specimen, and the associated deformation due to the electric field
is measured. Several researchers [13] adopted this method to capture the piezoelectric
constants of equation 1.
Kunstler et al. [14], suggested a quasi-static charge integration technique to conduct
direct piezoelectric experiments and to obtain piezo strain parameters. To achieve stable
electro-mechanical test results for PVDF, Mohammad Shahid et al. [15] had done a
parametric study from 1 mF to 1000 mF and found the threshold capacitance for the
PVDF as 100 mF. The same capacitance value is used in this study for direct electro-
mechanical tests. The Quasi-static charge integration technique as described in Section
2.1 of this paper, is adopted in the current study to perform electromechanical tests.
Figure 2. PVDF specimens (a) uniaxial dimension (b) during the uniaxial experiment (c) biaxial dimen-
sion (d) during the biaxial test.
Figure 3. (a) Biaxial test setup (b) Schematic view of the connection.
FERROELECTRICS 45
the capability to load 1kN on thin films. Black speckle markers were applied on the
sample to find strains using the stingray camera (F125 C). The camera was fixed
orthogonally to the sample as shown in Figure 3b. Electrodes were attached on top and
bottom of the sample and connected to Agilent digital multimeter along with 100mF
capacitor in parallel to observe the voltage variations. As shown in Figure 4, the sample
is connected to the multimeter through the 100 mF capacitor. The charge accumulation
on top and bottom of the films are stored in the capacitor. The represented voltage on
the multimeter is the potential difference between the two plates of the capacitor. In
order to obtain the real charge(Q) of the PVDF, we need to multiply the voltage (V)
with the capacitance (C) of the capacitor, and the same as shown in the equation 2.
Q¼CV (2)
Uni-axial and biaxial direct piezoelectricity experiments performed. Loads were
obtained from machine output, strain were calculated from image data of the camera,
and voltage variations were obtained from Agilent digital multimeter. Speckle dot track-
ing algorithm was developed in Matlab code [6] and image viewer tool (for cropping
the images) were used to process the image data to obtain the strains from raw image
data. Nominal stress values found from loads with original cross-sectional area.
I. More stretch (12%), and high mechanical strength (260 MPa) can be seen in the
stretch direction compared to orthogonal to stretch direction.
II. A similar trend is observed in the electromechanical plots.
46 H. LAMBADI AND C. LAKSHMANA RAO
Figure 5. Uniaxial experiment in stretch direction (a) Stress-strain plot (b) Electric displacement-
stress plot.
Figure 6. Uniaxial experiment in orthogonal to stretch direction (a) Stress-strain plot (b) Electric dis-
placement-stress plot.
Equi-Biaxial experiments were also carried out using cruciform shaped specimen, and
the results are showed in Figure 7. The following observations may be made in Figure 7.
I. The mechanical stresses induced for given strains along the stretch direction in
biaxial experiments are marginally higher than the corresponding response of
orthogonal to stretch direction.
II. In bi-axial tests, the material failed after immediate elastic response in stretch
direction and elastic strain limits are also less compared to the uniaxial tests.
III. The mechanical response in stretch direction shows a marginal softening at
higher stretches. The softening of mechanical response after stretching is more
FERROELECTRICS 47
Figure 7. Bi-axial experiment in stretch direction (a) Stress-strain plot (b) Voltage-stress plot; in
orthogonal to stretch direction (a) Stress-strain plot (b) Electric displacement-stress plot.
The model prediction of the mechanical part has already shown in the recent litera-
ture [3], the model prediction of the electromechanical part is discussed in the
next section.
However, these models are applicable only for isotropic piezo-materials. In this study,
we have used this model and extending it to observed anisotropic electromechan-
ical response.
This modal has been adopted in the current study to capture the mechanical response
of PVDF.
b. Piezoelectric response
We observe in the literature that several authors [11, 16] have developed and used a
quasi-static invariant (Iq ) for modeling the electromechanical response of electroactive
polymers. This quasi-static invariant, for an isotropic electromechanical response, can
be written as [16]
Iqi ¼ Ci : ðE EÞ i ¼ 1; 2 (7)
Where Ci refers to Cauchy green tensor to a pure stretch in direction i only.
For in-plane stretches (either uniaxial or biaxial tests), having an electric field in dir-
ection 3 alone, E can be written as
2 3
0
E¼4 0 5 (8)
E3
Similarly, for the stretch matrix for mechanically anisotropic is given by
2 3
I4 1 0 0
C¼ 4 0 I6 1 05 (9)
0 0 0
We postulate that the anisotropic electromechanical response is given as a linear
combination of isotropic response in two different directions as
W2 ¼ C6 Iq1 þ C7 Iq2 (10)
Where Iq1 and Iq2 (defined in equation 7) are assumed in isotropic response functions
for direction 1 and 2 respectively.
Below expression can be obtained by substituting the 7 and 9 in the equation 10
W2 ¼ C6 E32 ðI4 1Þ C7 E32 ðI6 1Þ (11)
Here C6 and C7 are electromechanical coefficients represent electromechan-
ical response.
A dominant piezoelectric response in PVDF sheets is in stretch direction (direction 1
in Figure 1), which signifies a voltage induced in direction three due to a stretch along
direction 1. The constants (C6 and C7 ) can be obtained by observing voltage variation
in the thickness direction (direction 3). The piezoelectric response corresponding to this
phenomenon can be evaluated with the above expression.
c. Dielectric response
PVDF is a dielectric cum ferroelectric material. PVDF exhibits the spontaneous polar-
ization due to ferroelectric property. PVDF generates internal energy due to the applica-
tion of electric field E. This internal energy due to electric fields for electroactive
polymer [11] is given by
50 H. LAMBADI AND C. LAKSHMANA RAO
Equation 12 has been adapted to capture the pure dielectric response of PVDF.
However, since this paper focuses only on the electromechanical response, this aspect is
not elaborated in this paper.
Q V
D3 ¼ ; E3 ¼ (13)
A t
Here A is surface area (20 45mm) and t is thickness of the film (28mm), and Q is
the charge of PVDF, calculated using equation 2 in section 2.
The modal predictions of electric displacement components can be found directly
using equation 3 after substituting W from equation 11 and 12; the following are the
expression for electric displacement components D3 (computed from equation 3) for
different loading conditions encountered in the experiments.
Expression given in Table 1 for D3 functions are used to find an error in equation 14
in section 4 below.
Levenberg Marquart algorithm has been used to optimize the parameters. The coeffi-
cients of the modal as obtained by this procedure are shown in Table 2.
The model parameters shown in Table 2 are used to reproduce the experimental
graphs in Figure 8 using modal equations from Table 1. The modal shows good correl-
ation with experiments.
FERROELECTRICS 51
Figure 8. Model prediction of direct piezoelectricity experiment in stretch direction for (a) uniaxial
case and (b) biaxial case.
5. Discussion
The manufacturers quoted d31 and d32 coefficient as a ratio of electric displacement
(D3) to the stress, as shown below
D3
d3i ¼ i ¼ 1; 2 (15)
ri
d3i can be calculated for various loadings using the values of stresses at different strains.
These values have been calculated for a given sample of PVDF, and its variation with
strain is plotted in Figure 9. From Figure 9, it may be observed that there is a nonlinear
variation of d3i with finite strains. The strain independent value of d3i as quoted from
manufacturer is also plotted in the same Figure for comparison. It is clear from graph
that d3i is over estimated in lower strain region and underestimated in higer
strain regions.
6. Conclusions
Monotonic uniaxial and biaxial electromechanical experiments were conducted on uni-
axially stretched PVDF film. Stress and voltage responses are observed high in stretch
direction and in the orthogonal to stretch direction for both uniaxial and biaxial tests.
Hyperelastic based constitutive model was developed to predict non-linear electromech-
anical plots from the experiments. Model predictions fit well with experimental plots.
Significant observations from this study are:
References
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[2] S. F. Mendes et al., Effect of the ceramic grain size and concentration on the dynamical
mechanical and dielectric behavior of poly (vinilidene fluoride)/pb (Zr0.53Ti0.47)O3 compo-
sites, Appl. Phys. A. 96 (4), 899 (2009).
[3] S. Sokhanvar, A. Zabihollah, and R. Sedaghati, Investigating the effect of the orthotropic
property of piezoelectric PVDF, Trans. Can. Soc. Mech. Eng. 31 (1), 111 (2007). DOI:
10.1139/tcsme-2007-0007.
[4] A. Vinogradov, and F. Holloway, Electro-mechanical properties of the piezoelectric polymer
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FERROELECTRICS 53