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European Polymer Journal 48 (2012) 79–85

Contents lists available at SciVerse ScienceDirect

European Polymer Journal

journal homepage: www.elsevier.com/locate/europolj

Dielectric spectroscopy of biodegradable

poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) films
Yi Yang a,b, Shanming Ke b, Li Ren a,⇑, Yingjun Wang a, Yiyang Li c, Haitao Huang a,b,⇑
a
National Engineering Research Center for Tissue Regeneration and Reconstruction, School of Materials Science and Engineering,
South China University of Technology, Guangzhou 510641, China
b
Department of Applied Physics and Materials Research Center, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong
c
Department of Mechanical and Automation Engineering, The Chinese University of Hong Kong, Sha Tin, New Territories, Hong Kong

a r t i c l e i n f o a b s t r a c t

Article history: In this paper, we report a systematic study of the dielectric relaxation spectroscopy of bio-
Received 21 June 2011 degradable poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) (PHBHHx) polyester which
Received in revised form 15 August 2011 has potential applications as a ‘‘green’’ dielectric material in electronic devices. The dielec-
Accepted 7 October 2011
tric spectra was measured over a wide frequency range (100  107 Hz) from 100 to 60 °C.
Available online 15 October 2011
A glass and a sub-glass transition relaxations were observed in the dielectric spectra of
PHBHHx. In addition, a nearly constant loss behavior was found by analyzing the dielectric
Keywords:
and conductivity spectra.
Dielectric spectroscopy
PHBHHx
Ó 2011 Elsevier Ltd. All rights reserved.
Biodegradable polyester
Green dielectric materials
Nearly constant loss

1. Introduction
Polyhydroxyalkanoates (PHA) are a bio-polyester family
which is produced by bacteria under unbalanced growth [1].
This family of materials has attracted more and more atten-
tion in tissue engineering and other biomedical applications
due to their microbial synthesis [2], good biocompatibility,
biodegradability and promoting cell growth [3–5]. Poly(3-
hydroxybutyrate-co-3-hydroxyhexanoate) (PHBHHx) is a
kind of copolyesters consisting of 3-hydroxybutyrate (HB)
and randomly distributed 3-hydroxyhexanoate (HHx) units
[6]. As a common member of the PHA family, PHBHHx
shows better thermal and mechanical properties, such as
flexibility and thermoplasticity, than those of many other
PHAs. For instance, PHBHHx (with 12 mol% HHx) has an
elongation at break of 500% and maintains an applicable
⇑ Corresponding authors at: Department of Applied Physics and Mate-
rials Research Center, The Hong Kong Polytechnic University, Hung Hom,
Kowloon, Hong Kong (H. Huang).
E-mail addresses: psliren@scut.edu.cn (L. Ren), aphhuang@polyu.
edu.hk (H. Huang).
tensile strength of 20 MPa, while PHB film only has an elon-
gation at break of less than 10% [7,8]. Previous studies also
showed that PHBHHx has better biocompatibilities with
fibroblast, chondrocyte and nerve cells than PHB [5,9].
The glass transition temperature (Tg  0 °C for PHBHHx
with 12 mol% HHx) and melting temperature (Tm) of
PHBHHx vary with the number of the HHx units, which have
been well investigated by differential scanning calorimeter
(DSC) and thermogravimetric analysis (TGA) [10,11]. Re-
cently, PHBHHx has been produced in a large scale [12],
which is very important for practical applications. Apart
from a variety of biological and medical applications,
PHBHHx may find its potential applications as a ‘‘green’’
dielectric material for capacitors [13]. Capacitors with high
energy storage density are becoming increasingly important
to a broad range of applications, especially in pulsed power
circuit applications, such as implantable medical devices.
The term ‘‘green’’ in electronics actually refers to lead- and
halogen-free materials. To meet the ever rising require-
ments on environment protection, a new generation of
‘‘green’’ dielectrics has to be composed of biodegradable
polymers which can be decomposed when buried, without

0014-3057/$ - see front matter Ó 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.eurpolymj.2011.10.002
 Author's personal copy

80 Y. Yang et al. / European Polymer Journal 48 (2012) 79–85

affecting the environment and ecosystem. PHBHHx is
biodegradable and it is worthwhile to study its dielectric
properties for potential applications as ‘‘green’’ dielectric
material. Our previous study [13] on PHBV has shown that
PHBV has a higher dielectric constant (e0 = 8.5 for 10 KHz
at room temperature) than that of the conventional dielec-
tric polymer, such as polypropylene (PP, e0 = 2 for 10 KHz
at room temperature) and polycarbonate (PC, e0 = 2.5 for
10 KHz at room temperature). The electrical energy density
stored in PHBV is also much higher than that stored in PP
and PC. This leads us to give the first detailed study on the
dielectric properties of PHBHHx by using the dielectric
relaxation spectroscopy (DRS) which is one of the most
suitable and versatile techniques to assess the dynamics of
polymer materials in various time and length scales.
2. Experimental
2.1. Materials and film preparation
Poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) (PHB
HHx, with HHx content of 12%) raw powders were used as
received from Jiangmen Center for Biotechnology Develop-
ment, Guangdong, China. The PHBHHx films were fabricated
by hot-pressing. The raw powders were compression-
molded directly under a pressure of 20 MPa at 120 °C for
2 h. The PHBHHx films with a thickness of 0.05 mm were
then obtained and cut into 10  10 mm2 pieces for dielectric
measurements.
2.2. Nuclear magnetic resonance spectroscopy (NMR)
1H Nuclear magnetic resonance (1H NMR) spectroscopy
of PHBHHx was recorded on a Bruker AG 300 NMR Spec-
trometer in CDCl3 at room temperature. Tetramethylsilane
was used as the internal reference.
2.3. Scanning electron microscopy (SEM)
The morphology of the obtained films was examined
under a scanning electron microscope (SEM, JEOL JSM-
6490). Before observation, the specimen was fractured in
liquid nitrogen and coated with gold. The acceleration volt-
age of the SEM apparatus was controlled at 20 kV. Thick-
ness of the PHBHHx film was measured from the SEM
image and also by a vernier caliper.
2.5. Dynamic mechanical analysis (DMA)
The glass transition temperature (Tg) of the pure PHBHHx
polymer was determined by dynamic mechanical analysis
(DMA). A Perkin Elmer Diamond DMA was used in tensile
mode at a frequency of 1 Hz. The sample was heated from
100 to 100 °C at a rate of 5 °C/min.
3. Results and discussion
3.1. 1H NMR and SEM
The chemical structure of PHBHHx, as shown in the in-
set of Fig. 1, contains [–O–CH(CH3)–CH2–CO–] for HB and
[–O–CH(C3H7)–CH2–CO–] for HHx. As characterized by
the 1H NMR spectrum in Fig. 1, a strong proton signal at
1.26 ppm can be attributed to –CH3 in HB while another
methyl group in HHx appeared at 0.91 ppm. The signal
appearing at 1.57 ppm can be assigned to the H atom res-
onances of the –CH2–CH2– unit in HHx. All these results
are consistent with previous reports [2,14], indicating that
pure PHBHHx was obtained.
3.2. DMA
Similar to PHB, PHBHHx is a semi-crystalline polymer
with a melting point Tm  124 °C [15]. From the X-ray
diffraction patterns (not shown here), the crystallinity (Xc)
of the PHBHHx films was estimated to be 7.6%. The low de-
gree of crystallinity will leads to some interesting relaxation
processes which different from the crystalline polymers
[16,17]. DMA was also performed to investigate the
thermomechanical properties of PHBHHx films. The storage
modulus (G0 ), loss modulus (G00 ) and tan d plots over a wide
temperature range are presented in Fig. 2. At temperatures
higher than 0 °C, the storage modulus decreases, manifest-
ing a rubbery state of the PHBHHx polyester. The accompa-
nied relaxation is associated to the apparent glass transition
and Tg can be defined as the temperature corresponding to

2.4. Dielectric relaxation spectroscopy (DRS)

For dielectric measurements, silver was sputtered on

both surfaces of the specimens. The dielectric properties
and ac conductivity were measured by using a broadband
frequency-response analyzer (Alpha analyzer, Novocontrol
Technologies) over a frequency range of 100–107 Hz at var-
ious temperatures. The temperature was controlled by a
Novocontrol Quatro Cryosystem with high accuracy
(±0.1 K). The real and imaginary parts of dielectric permit-
tivity [e⁄(f) = e0 (f)  ie00 (f), where f is the probe frequency]
were collected isothermally in the order of increasing Fig. 1. 300 MHz 1H NMR spectrum of PHBHHx in CDCl3. The inset shows
temperatures. the chemical structure of PHBHHx.
 Author's personal copy
Y. Yang et al. / European Polymer Journal 48 (2012) 79–85
Fig. 2. Dynamical mechanical analysis results: storage (G0 ) and loss (G00 )
modulus, and tan d of the PHBHHx film.
the maximum of either the loss modulus or the tan d. The
values of Tg are 8.9 and 12 °C, respectively, as determined
from the loss modulus and the tan d. A weak cold crystalliza-
tion peak could be observed at Tcc  87.8 °C. These are con-
sistent with previous reports [15].
3.3. Dielectric relaxation spectroscopy
As a new member of the PHA family, PHBHHx still has
many properties that are interesting for a wide range of
applications. In this section, we provide detailed dielectric
studies to extend the research area of biodegradable poly-
esters and to give a deeper understanding on the dielectric
properties of PHBHHx.
Depending on the structure, polymer molecules may
show different kinds of molecular motions leading to dif-
ferent relaxations. The temperature dependences of the
real (e0 ) and the imaginary (e00 ) parts of the relative dielec-
tric permittivity of PHBHHx films at selected frequencies
are shown in Fig. 3. Similar to other biodegradable polyes-
ter (such as Poly(butylene succinate), PBS) [18,19], three
types of dielectric relaxation processes can be observed:
region I (at low temperatures, 100 to 50 °C), region II
(at intermediate temperatures, 50 to 60 °C), and region
III (at high temperatures, 20–60 °C). In region I, a broad
relaxation peak in e00 (T) can be seen to move toward higher
frequencies as the temperature increases, which is accom-
panied by a slow transition step in the e0 curve. This has
been identified as a sub-glass b transition process similar
to that in many other hyperbranched polymersexplored
by using dielectric relaxation spectroscopy [19,20] and dy-
namic mechanical analysis [21]. The origin of such sub-
81
Fig. 3. Temperature dependence of the (a) real and (b) imaginary parts of
the relative dielectric permittivity of PHBHHx at selected frequencies.
glass transition is still an open question and it has been
assigned to the reorientation of the ester groups [22] or re-
lated to the torsional vibrations of main chains in the
neighborhood of its local equilibrium conformation [23].
It should be noted that the b process in PHBHHx merges
into an extremely broad peak with increasing probe fre-
quency and there is no well-defined peak maximum above
1 KHz, as shown in Fig. 3b. This result implies that there
should be other contributions to PHBHHx in this tempera-
tures range, which dominates the high frequency DRS.
At temperatures above 50 °C (region II), another relax-
ation process becomes evident. This process is very similar
to a relaxation which is related to the glass transition in
polymers and the segmental mobility. The peak height of
the a relaxation in PHBHHx seems unchanged with
increasing frequencies. It is interesting that this relaxation
process took place over a wide temperature range, cover-
ing the glass transition temperature obtained from the
DMA results (Tg  8.9–12 °C) [16]. The a relaxation peak
in PHBHHx became broader and the peak height was al-
most unchanged with increasing frequencies. This is quite
different from PBS, whose peak height shows an intense
rising trend with increasing frequencies. This implies that
the segmental mobility in PHBHHx is much lower than
that in PBS which reflects its viscous nature. The space
charge effect [24] is evident in region III, where e0 and e00 in-
crease dramatically at low frequencies with increasing
temperatures (Fig. 3).
The frequency dependences of the relative dielectric
permittivity (both e0 and e00 ) for a and b relaxations are
 Author's personal copy
82 Y. Yang et al. / European Polymer Journal 48 (2012) 79–85
Fig. 4. Frequency dependence of the (a) real and (b) imaginary parts of
the relative dielectric permittivity of PHBHHx at around the a glass
transition temperature. The dots are experimental data and the solid
curves are the best-fitted curves according to Eqs. (2) and (3).
plotted in Figs. 4 and 5, respectively. For quantitative eval-
uation of the relaxation time s(T) and other relaxation
parameters, the data were fitted by a Cole–Cole dielectric
equation [25,26],
 De
e ðxÞ ¼ e1 þ ; 0 < a P 1; ð1Þ
1 þ ðixsc Þ1a
 
De sinhðbuÞ
e0 ðxÞ ¼ e1 þ 1 ð2Þ
2 coshðbuÞ þ cosðbp=2Þ
De sinðbp=2Þ
e00 ðxÞ ¼ ; b ¼ 1  a; ð3Þ
2 coshðbuÞ þ cosðbp=2Þ
where u = ln(xsc), x is the angular frequency, sc is the
characteristic time, a is the shape parameter, De = es  e1
is the dielectric relaxation strength with es and e1 defined
as the low and high frequency limits of the relative dielec-
tric permittivity. It can be seen from Figs. 4 and 5 that the
low frequency permittivity (i.e. <100 Hz) at 0 °C does not
follow the fitting curves, which was probably due to the
space charge polarization [24]. For the b relaxation, which
is visible at relatively low frequency (Fig. 3), the corre-
sponding e00 (f) becomes almost frequency independent at
higher frequencies (as shown in Fig. 5b), similar to a
‘‘nearly constant loss’’ (NCL) process [27]. This ‘‘NCL’’
behavior will be discussed in Section 3.5 and is obviously
the main reason for the flattening of the high frequency
Fig. 5. Frequency dependence of the (a) real and (b) imaginary parts of
the relative dielectric permittivity of PHBHHx at around the b sub-glass
transition temperature. The dots are experimental data and the solid
curves are the best-fitted curves according to Eqs. (2) and (3).
dielectric loss peak corresponding to the b relaxation, as
shown in Fig. 3(b).
3.4. Mapping of the relaxation parameters
The relaxation shape parameter a and the characteristic
time sc were evaluated from the frequency spectra of the
dielectric permittivity by using the Cole–Cole functions
(Eqs. (1)–(3)). The evolution of a and the distribution of
sc (for both the a and b relaxations) are shown in Figs. 6
and 7 as a function of temperature. Clearly, the shape
parameter a associated with the a relaxation increases
from 0.4 to 0.7 with decreasing temperatures, while it
maintains at a fixed value of around 0.7 for the b relaxa-
tion. Larger a means a much broader distribution of relax-
ation times [25]. For a relaxations, the distribution of
relaxation time becomes broader upon cooling, which
can be better viewed from Fig. 6b. Here, the distribution
of relaxation time derived from the Cole–Cole relation
can be expressed as [25],
sinðapÞ
f ðsÞ ¼ ð4Þ
2p½coshðð1  aÞ lnðsc =sÞÞ  cosðapÞ
where f(s) can be calculated from the fitting parameters of
the dielectric permittivity.
It can also be seen from Fig. 6b that the distribution of
relaxation times for b relaxation is nearly temperature
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Y. Yang et al. / European Polymer Journal 48 (2012) 79–85
Fig. 6. (a) Temperature dependence of a obtained from the fitting of data
shown in Figs. 4 and 5. (b) Cole–Cole distribution of relaxation times at
selected temperatures.
independent. This feature is helpful to understanding the
origin of the b sub-glass transition process. However, it
cannot lead to the conclusion that the b sub-glass transi-
tion process is related to the torsional vibrations of main
chains in the neighborhood of its local equilibrium confor-
mation [23], or to the reorientation of the ester groups
Fig. 7. Temperature dependence of the characteristic relaxation time sc (obtained from the fitting of data shown in Figs. 4 and 5) for the a and b transitions.
(a) and (c) represent the Arrhenius plots. Also shown in (b) is the relation between the probe frequency and the temperature corresponding to the
maximum dielectric permittivity (imaginary part) of the a relaxation in PHBHHx. The short dashed lines in (a) just guide the eyes. The solid and dashed
lines in (b) are fitted by the Vögel–Fulcher law. The solid line in (c) is fitted by the Arrhenius law.
83
[22]. Due to the large free spaces in polymers, the freezing
of ester groups may not influence the distribution of relax-
ation times.
The temperature dependences of the characteristic time
sc for the a and b relaxations are shown in Fig. 7. Generally,
the relaxation for a sub-glass transition process always fol-
lows an Arrhenius law. The characteristic time for the
relaxation process in region II of Fig. 3 does not follow an
Arrhenius law exactly (Fig. 7a), but can be well described
by the Vögel–Fulcher (VF) equation [26,28]:
1 Ea
sc ¼ exp ð5Þ
x0 kB ðT  T f Þ
where Ea is the activation energy, x0 is the attempt fre-
quency of a molecule and Tf is the static freezing tempera-
ture at which x goes to zero. This behavior indicates that
the relaxation process in region II is a genuine a process.
The large difference between the viscoelastic and dielectric
peak may be understood by its semi-crystalline structure
with very low degree of crystallinity [16,17]. It should be
emphasized that Ea obtained from VF relation is a parame-
ter corresponding to the hindering barrier of the Arrhenius
case (i.e. the case for Tf = 0 K), but it does not represent a
real activation process. The calculated activation energy
Ea for the a relaxation is 91.9 meV, while the freezing tem-
perature Tf is 212 K. Besides, the relationship between the
probe frequency f and the peak temperature Tm obtained
from Fig. 3b for the glass transition a is also shown in
Fig. 7 and can be described by the following VF equation,
Ea
f ¼ f0 exp ð6Þ
kB ðT  T f Þ
The obtained activation energy and freezing tempera-
ture are 90.2 meV and 211 K, respectively, and are in good
agreement with the results obtained from the sc–T relation.
Fig. 7c shows the Arrhenius plot for the b relaxation. The
activation energy for this process is 679 meV.
3.5. Nearly constant loss-like behavior
At low temperatures, there are two obvious contribu-
tions to DRS of PHBHHx (Fig. 6): one is the sub-glass tran-
sition at low frequency and the other is the ‘‘nearly
 Author's personal copy
84 Y. Yang et al. / European Polymer Journal 48 (2012) 79–85
constant loss’’-like (NCL) process. Actually, NCL is a univer-
sal behavior in disordered materials (such as glasses, poly-
mers and highly doped crystals) [29–31]. At sufficiently
low temperatures and/or high frequencies, the conductiv-
ity r0 (f) for NCL response depends linearly on frequency,
which implying a negligible frequency dependence of the
imaginary part of dielectric permittivity [e00 (f) = r0 (f)/2pf].
The frequency dependence of the conductivity is given by
r0 ðf Þ ¼ Af s ð7Þ
where the exponent s is nearly equal to 1 and A is a con-
stant with weak temperature dependence [29].
Fig. 8a–c show the frequency dependence of the con-
ductivity r0 (f) and imaginary part of permittivity e00 (f) at se-
lected temperatures. At low temperature (95 °C), r0 (f)
exhibits a linear frequency dependence above 200 Hz (with
an exponent s = 1 following Eq. (7)) and therefore a negli-
gible frequency dependence of e00 , an NCL-like behavior.
At 45 °C, the right wing of b process is absolutely covered
by the NCL-like response and meanwhile the a process sets
in at low frequencies. The span of the NCL-like regime
becomes narrower with increasing temperatures.
By fitting Eq. (7), the exponent s can be obtained and its
temperature dependence is shown in Fig. 8d. Two regions
can be clearly identified. Below 25 °C, the exponent s
reaches a plateau value of 1, while at a higher temperature
(25  5 °C), s decreases quickly with increasing
Fig. 8. (a, b, c) Frequency dependence of the conductivity and the imaginary part of the dielectric permittivity at selected temperatures for PHBHHx. The
solid lines are the best fits according to Eq. (7). (d) Temperature dependence of the exponent s from the fitting data.
temperature. (It should be noted that the NCL-like response
above 5 °C is out of our experimental frequency window.)
This behavior is very similar to that of ionic conducting
glasses, such as CeO2:Gd2O3 [27], but is quite different from
that of ferroelectric ceramics [32] and some other biode-
gradable polyester, such as poly(butylene succinate) [18],
whose s increases linearly with increasing temperature
leading to a superlinear power-law behavior [33].
From the Kramers–Krönig relation [26,32,34], it is
known that the power law (2pf)n of the ac conductivity will
lead to a (2pf)n1 behavior for the real part of the dielectric
permittivity, e.g.,
e0 ðf Þ ¼ Bð2pf Þn1 ð8Þ
0
We plotted the frequency dependence of e (f) at selected
temperatures in Fig. 9a. Clearly, the e0 (f) at the NCL-like re-
gime could be described well by Eq. (8), which again
reflecting a genuine NCL behavior. The temperature depen-
dence of the exponent n displays a very similar behavior to
that of exponent s, as shown in Fig. 9(b).
Although the apparent dielectric response behaves as
constant loss, it should be emphasized that we cannot con-
clude here an unambiguous NCL behavior in PHBHHx.
Overlapping of two or several relaxation processes could
also give rise to a ‘‘nearly constant loss’’. Further experi-
mental investigation is needed to confirm our finding is a
real NCL response or multi relaxation overlapping.
 Author's personal copy
Y. Yang et al. / European Polymer Journal 48 (2012) 79–85
Fig. 9. (a) Frequency dependence of the real part of the relative dielectric
permittivity at selected temperatures. Dots are experimental values and
the solid lines are the best fits according to Eq. (8). (b) Temperature
dependence of the exponent n and constant B fitted according to Eq. (8).
4. Conclusions
In summary, we have performed a systematic dielectric
study on the biodegradable polyester PHBHHx. The sub-
glass transition relaxation (a and b) and nearly constant
dielectric loss behavior in PHBHHx have been addressed
and discussed. The a process shows a Vögel–Fulcher tem-
perature dependence, while the b relaxation follows the
Arrhenius law. The distribution of relaxation times is sym-
metric for both a and b processes. However, the width of
distribution is temperature independent for b process,
but becomes broader upon cooling for a process. The cou-
pling between the b relaxation and NCL-like response in
PHBHHx is interesting and is may be useful for a plausible
explanation of NCL.
85
Acknowledgements
This work was supported by National Natural Science
Foundation of China (Grant Nos. 50732003, 50803018
and U0834003), National Science and Technology Support
Programme of China (Grant No. 2006BAI16B06), the Hong
Kong Polytechnic University (Project Nos. A-PK30 and A-
PJ46) and Endowment Fund Research Grant of United Col-
lege, The Chinese University of Hong Kong (Project No.
CA11168).
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