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Received 6 March 2015; Revised 19 April 2015; Accepted 22 April 2015; Published 28 May 2015
0-3 dielectric composites with high dielectric constants have received great interest for various technological applications. Great
achievements have been made in the development of high performance of 0-3 composites, which can be classified into dielectric–
dielectric (DDCs) and conductor–dielectric composites (CDCs). However, predicting the dielectric properties of a composite is still
a challenging problem of both theoretical and practical importance. Here, the physical aspects of 0-3 dielectric composites are
reviewed. The limitation of current understanding and new developments in the physics of dielectric properties for dielectric
composites are discussed. It is indicated that the current models cannot explain well the physical aspects for the dielectric properties
of 0-3 dielectric composites. For the CDCs, experimental results show that there is a need to find new equations/models to predict
the percolative behavior incorporating more parameters to describe the behavior of these materials. For the DDCs, it is indicated that
J. Adv. Dielect. 2015.05. Downloaded from www.worldscientific.com
the dielectric loss of each constituent has to be considered, and that it plays a critical role in the determination of the dielectric
response of these types of composites. The differences in the loss of the constituents can result in a higher dielectric constant than
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1. Introduction of Dielectric Composites defined as 0-0, 0-1, 0-2, 0-3, 1-1, 2-1, 3-1, 2-2, 3-2, and 3-3,
Dielectric materials, which have a high dielectric constant ("), where 0/1/2/3 represent the number of dimensions in conti-
a low dielectric loss (tan ), and a high breakdown field (i.e., nuity for each constitute in the composite.12–15 For example,
a 0-3 composite is defined as having a 0-dimension (i.e.,
dielectric strength, Eb ) have received a great deal of interest
isolated) particle embedded in 3-dimensions of a continuous
from various technological applications, such as energy-
media (i.e., a polymer matrix).6–8 Dielectric composites, es-
storage capacitors, electroactive devices, gate dielectrics,
pecially 0-3 composites using a dielectric polymer as matrix,
electric powered vehicles and pulse-power applications.1–5
have been widely studied in last three decades. Based on the
Dielectrics can be inorganic and organic. In general, the in-
fillers used, the dielectric 0-3 composites using a dielectric
organic dielectrics, such as metal oxides and ceramics (es-
polymer matrix can be classified into: (a) dielectric–dielectric
pecially ferroelectric ceramics), can exhibit a high dielectric
composites (DDCs), in which the filler is a dielectric; (b)
constant, but they are brittle, exhibit a low Eb, and require a
conductor-dielectric composites (CDCs), in which the filler is
high processing temperature. Organic dielectrics, such as
a conductor.7
polymers, are flexible, exhibit a high Eb , and can be pro-
Mathematically, it is impossible to determine the dielectric
cessed at a low temperature, but exhibit a low dielectric
response of a composite even with the detailed information
constant.6,7 Therefore, it is of interest to develop organic–
about the exact microstructure of the composite. However,
inorganic composites in order to optimize the dielectric
it is of theoretical and practical importance to know the re-
properties for different applications. Great strides have been
made in the development of dielectric composites.8–10 lationship between the dielectric properties and the compo-
A composite is a mixture of materials with significantly sition of a composite. Therefore, different assumptions and
different physical or chemical properties in an attempt to approximations have been used to establish the relationship
obtain some advanced properties. The physical properties of a between the dielectric response and composition of the
composite can be the sum, combination, or the product of composites. The current understanding of the physical aspects
the properties of its constituents dependent on the property for the dielectric 0-3 composites and the recent achievements
and connectivity. It is known that the connectivity of a in the development of the dielectric 0-3 composites are briefly
composite plays a key role in its properties. The connectivity discussed here. The limitation of the current understanding is
for composites was first classified by Newnham et al.11 For reviewed and new developments in the physics behind the
composites with two constituents, their connectivity can be properties of dielectric composites are discussed.
This is an Open Access article published by World Scientific Publishing Company. It is distributed under the terms of the Creative Commons Attribution 3.0
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1550012-1
L. Zhang, P. Bass & Z.-Y. Cheng J. Adv. Dielect. 5, 1550012 (2015)
εeff
600 Yamada Model
ferroelectrics, such as BaTiO3 (BT), Pb(Mg1∕3 Nb2∕3 )O3
400
(PMN), Pb(Zr,Ti)O3 (PZT), (Ba,Sr)TiO3 (BST), have been
200
widely used in the development of DDCs.16–25 Unfortunately,
the dielectric constant of a ferroelectric or relaxor ferroelec- 0
tric is strongly dependent on the temperature.26 The discovery 0.0 0.2 0.4 0.6 0.8 1.0
of CaCu3Ti4O12 (CCTO) provides new opportunities/avenues Volume fraction of filler (ϕ)
to develop high performance composites due to the facts that
Fig. 1. Composition dependence of the effective dielectric constant
CCTO exhibits a very high dielectric constant (> 104) that is
("eff ) calculated using different models for 0-3 DDCs.
also weakly dependent on the temperature.27–29 Composites
using CCTO have been widely studied.30–45 It should be
mentioned that, in most of DDCs using nanosized ceramic Lichtenecker's logarithmic law and 10 for the Yamada
fillers, the dielectric constant can only reach the value around Model.7 Based on all of the models/equations introduced so
50 even for the composites with a volume fraction of filler up far as illustrated in Fig. 1, it is concluded that: (1) "eff
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to 50 vol.%.7 It is well known that the high filler content increases with increasing ’, in other words, "eff monotoni-
reduces the composite flexibility and results in weak me- cally changes with ’; (2) "eff falls in between the two extreme
by 200.132.111.137 on 03/07/18. For personal use only.
chanical properties, which can limit its applications. Re- curves for parallel and series connections. Actually, the sec-
garding polymers used as the matrix for the development of ond conclusion is the well-known Wiener limits which was
DDCs, polyvinylidene fluoride (PVDF)-based ferroelectric introduced by Wiener in 19217,46:
polymers have been used since they exhibit a higher dielectric
"seri "eff "para or
constant ( 10). However, these polymers exhibit a relative ð1Þ
high loss (tan 10%). Some other nonpolar polymers, such ð’1 " 1 1 1
1 þ ’2 " 2 Þ "eff ’1 "1 þ ’2 "2 :
as epoxy, polyethylene (PE), polyester (PS), poly(methyl
methacrylate) (PMMA), poly(vinyl chloride) (PVC), and
polyurethanes (PU) are also used as matrix materials for di- 2.2. Conductor–dielectric composites
electric composites.7 These polymers exhibit a low dielectric The dielectric response of a CDC is determined by the per-
constant (< 5) with a very small loss.7,8 colation phenomenon.7 As shown in Fig. 2, if the filler
Understanding the dielectric response of a composite (or content is higher than a certain value (i.e., the percolation
heterogeneous dielectrics) has been an interesting topic for threshold ’c Þ, the composite is a conductor. When the vol-
fundamental research and applications. The first study of the umetric content of conducting filler is lower than the ’c , the
dielectric response of a 0-3 composite was done by Rayleigh composite is an insulator/dielectric and its dielectric constant
in 1890s.7 Based on different assumptions and approxima- increases with increasing ’. As the filler content approaches
tions, various models/equations have been introduced to
simulate the relationship between the effective dielectric
constant ("eff ) of a composite and its composition by using
the dielectric constant ("f ) of the filler and the dielectric
constant ("m ) of the matrix.7 In these models/equations, the
composition of a composite is usually represented by the
volume fraction of fillers (’). In some of the models/equa-
tions, an additional parameter is used to modify the rela-
tionship in order to include the influence of the filler particle
shape or the microstructure on the "eff . The most used
models/equations have been discussed in a previous review.7
The "eff of a composite was simulated using different
models/equations as shown in Fig. 1, where "f ¼ 1000 and
"m ¼ 10 are used. There are eight curves in Fig. 1, among
which two characterize extreme cases: the parallel (black) and
series (red) connection. The other six include four without the Fig. 2. Composition dependence (i.e., volume fraction of conduct-
additional parameter and two (modified Lichtenecker's log- ing filler, ’) of the effective dielectric constant ("eff ) of 0-3 CDCs,
arithmic law and Yamada Model) with the additional pa- where ’c is the percolation threshold (dashed blue line). The insets
rameter. The additional parameter used is 0.3 for the modified show the microstructure of the composites.
1550012-2
L. Zhang, P. Bass & Z.-Y. Cheng J. Adv. Dielect. 5, 1550012 (2015)
’c , the dielectric constant increases with increasing filler strongly dependent on the frequency as:
content very rapidly so that a giant dielectric constant may be
"eff / ! 1 ; ð4Þ
obtained in the composites close to ’c . This provides an
approach to develop composites with a high dielectric con- where (< 1) is a constant and ! is the angular frequency.
stant. This approach was first used to prepare composites
with a high dielectric constant in 1970s.47,48 Therefore, var-
ious conducting fillers have been used in the development of 3. New Physical Aspects for Dielectric Composites
CDCs in recent years. Conductor fillers with various shapes
3.1. Dielectric–dielectric composites
(spherical, core-shell, tube, and bar/wire/fiber-like) ranging in
size from micrometers to nanometers have been studied, such As more and more experimental results are being reported,
as with metals,49–54 carbon/carbon nanotubes,55–60 and con- some results have been shown that contradict the current un-
ducting polymers. 6164 These composites can exhibit a high derstanding. There are two different phenomena: (1) "eff does
dielectric constant (up to 1000) for the composites with a not increase with ’ monotonically, and (2) "eff is larger than
small ’. This is the major advantage of CDCs over DDCs the dielectric constant of both constituents. For example, three
since a composite with low ’ would be more flexible. different ceramic–polymer composites prepared by different
The ’c is an intrinsic parameter for a composite system research groups are shown in Fig. 3, where the dielectric
and is a very critical point for a CDC. The ’c is strongly constants at 100 Hz for composites at room temperature are
plotted versus the volume fraction of ceramic fillers. Shan
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1550012-3
L. Zhang, P. Bass & Z.-Y. Cheng J. Adv. Dielect. 5, 1550012 (2015)
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L. Zhang, P. Bass & Z.-Y. Cheng J. Adv. Dielect. 5, 1550012 (2015)
79
Ni-P(VDF-CTFE), Zhang et. al
0.2 PANI-PVDF, Yuan et. al 80
CF-PVDF, Dang et. al 55 1 : ε 's=10, ε oo
" =1, τ0 =10-2
MWNT-PVDF, Dang et. al 57 2
0.1 100 2 : ε 's=100, ε "oo=1, τ0 =10-3
ϕ = 0.1
ϕ = 0.3
0.0 ϕ = 0.5
ε 'eff
100 1k 10k 100k 1M ϕ = 0.7
Frequency (Hz) 10 ϕ = 0.8
1 ϕ = 0.9
Fig. 5. Frequency dependence of the fitting constants ’c by fitting ϕ = 0.95
dielectric constant using Eq. (3) for different nanocomposites at ϕ = 0.98
room temperature. The dielectric constant used in the fitting was
J. Adv. Dielect. 2015.05. Downloaded from www.worldscientific.com
ϕ = 0.8
composite, the simple series connection is considered here. ϕ = 0.9
2
That is, two dielectric layers are connected in series to form an ϕ = 0.95
ϕ = 0.98
extremely simple composite. To make the simulation simple, 1 1
the two dielectric layers are considered as two ideal Debye
media with a zero electrical conductivity. That is, for each 0
dielectric layer, its dielectric properties can be written as1,2:
1 10 100 1k 10k 100k 1M
" "1 " "
" ð!Þ ¼ "1 þ s ; " 0 ¼ "1 þ s 212 ; Frequency (Hz)
1 þ j!0 1 þ ! 0
(c)
ð" "1 Þ!0 " 00 ð" "1 Þ!0
" 00 ¼ s ; tan ¼ 0 ¼ s ; Fig. 6. Frequency dependence of the dielectric response of two
1 þ ! 0
2 2 " "s þ "1 ! 2 02
Debye media in the series connection: (a) real part (i.e., dielectric
ð5Þ constant), (b) imaginary part and (c) loss.
1550012-5
L. Zhang, P. Bass & Z.-Y. Cheng J. Adv. Dielect. 5, 1550012 (2015)
constant and is also termed as the permittivity strength of the dielectric loss of two is different. In other words, when the
relaxation process. dielectric loss of the constituents in a composite is different, a
For a series connection of two dielectric layers, the " eff peak-like curve is expected for "eff and ’. Therefore, the
would be: reported results shown in Figs. 3 and 4 can be explained due
1 1’ ’ to the difference in the loss of their constituents. It should be
¼ þ ; ð6Þ mentioned that the simulation above is based on the dielectric
"eff ð!Þ "1 ð!Þ "2 ð!Þ
loss due to the relaxation. If a dielectric has a nonzero elec-
where ’ is the volumetric fraction of the dielectric layer trical conductivity, the conductivity will contribute to the
(constituent) 2, and "1 ð!Þ and "2 ð!Þ are the dielectric dielectric loss. In this case, above conclusion is valid.
responses of the two dielectric layers and can be written using
Eq. (5) with corresponding "s , "1 and 0 . For further illus-
tration, numerical calculation is carried out using follow- 5. Summary
ing parameters: "s1 ¼ 10, "11 ¼ 1, 01 ¼ 10 2 , "s2 ¼ 100, In this work, the physical aspect of 0-3 dielectric composites
"12 ¼ 1, 02 ¼ 10 3 . Figure 6 shows the results for the is examined. The limitation of the current understanding and
composites with different compositions. the new development of physics for explaining the dielectric
From the data shown in Fig. 6(a), one can find that when properties of dielectric composites are discussed. It is found
the frequency is very low (i.e., the loss of both dielectric that the current models of both DDCs and CDCs cannot
layers is almost zero), the "eff increases with the ’ mono-
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L. Zhang, P. Bass & Z.-Y. Cheng J. Adv. Dielect. 5, 1550012 (2015)
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