1 3688435

A review and analysis of microwave absorption in polymer composites filled with
carbonaceous particles
F. Qin and C. Brosseau
Citation: Journal of Applied Physics 111, 061301 (2012); doi: 10.1063/1.3688435
View online: http://dx.doi.org/10.1063/1.3688435
View Table of Contents: http://scitation.aip.org/content/aip/journal/jap/111/6?ver=pdfcov
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131.180.140.56 On: Tue, 30 Dec 2014 20:12:48
JOURNAL OF APPLIED PHYSICS 111, 061301 (2012)
APPLIED PHYSICS REVIEWS
A review and analysis of microwave absorption in polymer composites

filled with carbonaceous particles
F. Qin and C. Brosseaua)
Universite Europeenne de Bretagne, Lab-STICC, Universite de Brest, CS 93837, 6 avenue Le Gorgeu,
29238 Brest Cedex 3, France
(Received 30 November 2011; accepted 27 January 2012; published online 16 March 2012)
Carbon (C) is a crucial material for many branches of modern technology. A growing number of
demanding applications in electronics and telecommunications rely on the unique properties of C
allotropes. The need for microwave absorbers and radar-absorbing materials is ever growing in
military applications (reduction of radar signature of aircraft, ships, tanks, and targets) as well as in
civilian applications (reduction of electromagnetic interference among components and circuits,
reduction of the back-radiation of microstrip radiators). Whatever the application for which
the absorber is intended, weight reduction and optimization of the operating bandwidth are two
important issues. A composite absorber that uses carbonaceous particles in combination with a
polymer matrix offers a large flexibility for design and properties control, as the composite can be
tuned and optimized via changes in both the carbonaceous inclusions (C black, C nanotube, C fiber,
graphene) and the embedding matrix (rubber, thermoplastic). This paper offers a perspective on the
experimental efforts toward the development of microwave absorbers composed of carbonaceous
inclusions in a polymer matrix. The absorption properties of such composites can be tailored
through changes in geometry, composition, morphology, and volume fraction of the filler particles.
Polymer composites filled with carbonaceous particles provide a versatile system to probe
physical properties at the nanoscale of fundamental interest and of relevance to a wide range
of potential applications that span radar absorption, electromagnetic protection from natural
phenomena (lightning), shielding for particle accelerators in nuclear physics, nuclear electromagnetic pulse protection, electromagnetic compatibility for electronic devices, high-intensity radiated
field protection, anechoic chambers, and human exposure mitigation. Carbonaceous particles are
also relevant to future applications that require environmentally benign and mechanically flexible
C 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.3688435]
materials. V
TABLE OF CONTENTS
I. INTRODUCTION . . . . . . . . . . . . . . . . . . . . . . . . . . . .
A. Carbonaceous materials . . . . . . . . . . . . . . . . . .
B. Filled polymers . . . . . . . . . . . . . . . . . . . . . . . . .
C. Microwave absorbers . . . . . . . . . . . . . . . . . . . .
D. Objectives and outline . . . . . . . . . . . . . . . . . . .
II. MA THEORY. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
A. Microwave interaction with absorbers. . . . . .
B. A birds eye view on dielectric
heterostructures theory . . . . . . . . . . . . . . . . . . .
1. Mixture laws and effective medium
approaches . . . . . . . . . . . . . . . . . . . . . . . . . .
2. Computational approaches . . . . . . . . . . . . .
III. CF-BASED POLYMER COMPOSITES. . . . . . . .
A. Continuous-fiber composites. . . . . . . . . . . . . .
B. Short-fiber composites . . . . . . . . . . . . . . . . . . .
a)
2
2
2
3
4
4
5
6
6
8
9
9
12
Author to whom correspondence should be addressed. Electronic mail:

brosseau@univ-brest.fr.
0021-8979/2012/111(6)/061301/24/$30.00
IV. CNT-BASED POLYMER COMPOSITES . . . . . .

A. MA properties of CNT-based materials . . . .
1. CNT loading dependence . . . . . . . . . . . . . .
2. Geometry of particles . . . . . . . . . . . . . . . . .
3. Dispersion of particles . . . . . . . . . . . . . . . .
4. Interfacial properties . . . . . . . . . . . . . . . . . .
B. Magnetically filled or decorated CNTs . . . . .
V. CB-BASED POLYMER COMPOSITES . . . . . . . .
A. Single layer microwave absorber . . . . . . . . . .
B. Multilayer microwave absorbers. . . . . . . . . . .
VI. OTHER TYPES OF C-BASED POLYMER
COMPOSITES . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
A. C micro-/nano-coils . . . . . . . . . . . . . . . . . . . . .
B. Onion-like C . . . . . . . . . . . . . . . . . . . . . . . . . . .
C. C nanofibers. . . . . . . . . . . . . . . . . . . . . . . . . . . .
D. Graphite . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
VII. SUMMARY AND FUTURE PROSPECTS . . . .
A. Future prospects . . . . . . . . . . . . . . . . . . . . . . . .
B. Final thoughts . . . . . . . . . . . . . . . . . . . . . . . . . .
111, 061301-1
13
13
13
14
14
15
15
16
16
16
17
17
18
18
19
19
19
19
C 2012 American Institute of Physics

V
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I. INTRODUCTION
A. Carbonaceous materials
Carbon (C) is the fourth most abundant chemical element

in the universe by mass after hydrogen, helium, and oxygen. It
is the element that is natures choice as a basis for life under
conditions corresponding to those of Earths surface. Pure C
occurs in several ways (see Fig. 1) including diamond, graphite
(carbon black (CB)), graphene, buckminsterfullerene (nanosized spheres of rolled-up graphene) and nanotube, each of
which has been a star material at one time, e.g., diamond, the
sp3 allotrope, was Science magazines molecule of the year in
1988 because for the first time it could be synthesized as thin
films by chemical vapor deposition.1,336 The inherent charge
transport characteristics and the factors that limit the charge
carrier mobility differ significantly between the various C
nanostructures reflecting, on the one hand, the electronic
dimensionality of the structures, and, on the other hand, the
achievable dimensions of the respective p-systems. Bonding
between C and other elements can easily be changed by chemi-
J. Appl. Phys. 111, 061301 (2012)
cal reactions and physical interactions. Ever since the development of plastic electronics, there has been tremendous interest
in the properties of C-based materials owing to the substantial
p-electron delocalization of fullerenes and C nanotubes
(CNTs). The motivation for the miniaturization of electronics
has continuously pushed the research via the top-down
approach into nanostructures. As one of the most promising
candidates, C nanostructures, either 2D graphene57 or quasi1D CNTs,8,9 have opened entirely new perspectives toward the
C-based electronics. In many respect CNTs resemble the polymer chains used as composite matrices: both have covalently
bonded structures, similar dimensions, and mechanical flexibility. However, despite considerable interest in adding small
concentrations of CNTs to polymeric materials, what unquestionably matters is the ability to disperse them in the polymer
matrix. The difficulty to separate bundled tubes, the strong dependence of the conductivity on the CNT structure, and the
lack of techniques for observing their dynamics in molten suspensions, have slowed fundamental progress on their use in
nanotechnology. Over the last decade, through recent technological advances in nanoplasticsthe fusion of traditional
plastics and the developing field of nanotechnologymany
exciting results have demonstrated that polymers filled with
C-based materials possess unique properties, including
improved strength and durability, electrical conductivity,
flame resistance, UV absorption, and reduced permeability. In
addition to these properties, the rapid progress in the fabrication of CNTs and large area 1 cm2 graphene flakes10
makes these C structures promising for microwave absorption
(MA) applications, e.g., shielding materials for protection of
electronic devices, reduction in electromagnetic exposure, and
camouflage materials for radar and defense projects.
B. Filled polymers
FIG. 1. (Color) Some allotropes of C: (a) diamond; (b) graphite; (c) lonsdaleite; (df) fullerenes (C60, C540, C70); (g) amorphous carbon; (h) carbon
nanotube (Courtesy of Michael Strock, reprinted from http://en.wikipedia.org/wiki/Carbon); (i) graphene (reprinted with permission from Ref.
338, copyright 2009 Wiley and Sons).
The study of the electromagnetic properties of an ensemble of filler particles embedded in a polymer matrix requires
the determination of not only the intrinsic electromagnetic
properties of the individual particles but also the type and
strength of interparticle interactions, e.g., long-range dipoledipole interactions, clustering, and matrix-particle interactions, such as multicontact chain adsorption to the surface of
the filler. It has been well established that spatial inhomogeneities, i.e., clusters of filler particles, give rise to polarization
phenomena and therefore to a frequency dependence of the
effective permittivity.11 However, understanding how electrons are distributed in these filler aggregates remains one outstanding unresolved problem in mesoscopics of disordered
materials, making it difficult to know which theoretical framework is most appropriate for understanding these compounds,
e.g., localization by disorder is a common cause of insulating
behavior in condensed matter systems.
Among the broad variety of polymers suitable for embedding carbonaceous particles for MA applications, epoxy resins
are good candidates due to their low cost, ease of mixing with
different types of fillers, resistance to oxidative photodegradation, and stability in sunlight. An epoxy polymer chain
is made up of alternating single and double carbon bonds,
which enables the formation of a spatially delocalized electron
131.180.140.56 On: Tue, 30 Dec 2014 20:12:48
061301-3
system. This electronic distribution is strongly affected

by selective chain adsorption on the CB aggregates providing charge trapping sites.1116 This effect has previously
been experimentally studied in the context of CB-filled
polymers.1719 The conductivity of these systems relies on
two distinct carrier types within the CB aggregates and
agglomerates. Such a separation of carriers has been recently
predicted by Brosseau et al.1719 on the basis of electron spin
resonance experiments. Their results suggest that the majority
of the carriers are confined to the aggregate and agglomerate
surfaces. Localization by disorder is a common cause of insulating behavior in these systems. Yet, some open questions
remain. For instance, it would be desirable to know how
aggregation effects of the filler particles create microstructures
with multiscale and hierarchical structures formed when the
filler particles are immersed in the complex fluid environment
formed by polymer chains.337 The heart of the problem lies in
the strength of the van der Waals attraction among the particles. Once they come into contact, they form irregular clusters the morphology of which is determined by the kinetics of
aggregation. Another relevant question is how aggregation
and agglomeration of filler particles influence the conductivity
and the polarization mechanisms. The experimental characterization of filler particle clusters polarization and conduction is
a nontrivial task. The experimental determination of the 3D
detailed structure of this filler phase can be complicated
because it requires a difficult tomography analysis, which is
often restricted in spatial resolution. Most data available is either very limited or performed in extremely diluted systems
where the average dipolar interaction is very weak. In addition, most conventional analysis do not take spatial confinement factors into consideration. In this regard, important
information of the electrical connection among the filler
aggregates can be obtained by using local probes, e.g., electric
force microscopy, capacitance probe microscopy, or atomic
force microscopy.2227
C. Microwave absorbers
To a large extent, the theoretical and experimental

efforts designed to provide microwave absorbers are associated with two important features of their electromagnetic
properties. The first is based on enhanced magnetic losses
due to, for example, resonance phenomenon in the higher
frequency region (> 300 MHz). Additionally, it has been
argued that the second feature is related to enhanced dielectric losses. The magnetic losses of the spinel ferrites become
small in accordance with Snoeks limit and, thus, these materials are not adequate in the GHz frequency range. However,
considerable research has been devoted to developing artificial composite media using a wide range of polymers filled
with M-type hexaferrites posessing large tunable anisotropy
field.2840 Advances in ferrite technology have given experimentalists unprecedented control over gyromagnetic resonance characteristics for selective frequencies or over a
narrow frequency range, paving the way to fabrication of radar absorbers.41 Many recent experiments and simulations
investigated the behavior of ferromagnetic nanoparticles in
combination with a dielectric matrix material for MA.33,42
J. Appl. Phys. 111, 061301 (2012)
MA has also been discussed in the context of aluminum (Al)

flakes and CB-filled polymers.4354 Variations of the content
of the Al and CB constituents allow the real and imaginary
parts of the effective permittivity of the composite to be
tuned independently to match some absorption requirement
at a given frequency. One significant advantage of these
(lightweight) polymeric composites is that, depending on the
filler particles incorporation-mixing process and by an
adjustment of the nature and geometry of the filler particles,
they offer multiple degrees of freedom to tune the particles
aggregation state and the overall effective permittivity.
There has been a long history for research into C-based
absorbers.5559 The first use of C particles into absorber dates
back to 1936 when an absorber based on CB and TiO2 was
patented in the Netherlands.60 During World War II (WWII),
the United States developed an absorbing material known as
Halpern anti radiation paint (HARP) based on rubber filled
with CB and Al flakes. It was then successfully implemented
in airborne and seaborne vehicles for radar absorption with a
1520 dB absorption at the X-band.61,62 Broadband absorbers grabbed the attention in the post-WWII period. C-loaded
plaster and graphite were among the most intensively investigated absorbing materials. In the 1950s, C-based absorbers
started to find commercial use. For example, Spongex made
of C-coated animal hair, developed by the Sponge Products
Company, was able to give 20 dB attenuation in the range
2.410 GHz with a thickness of 50.8 mm and normal incidence. With the development of absorbers of particular structures in the 1960s and 1970s, particulate or fibrous C, among
other materials, were used to fill or coat on the netlike structures, knitted structures, or honeycomb structures.63 CB and
graphite remained the favorite absorbing candidates until the
discovery of CNTs in the 1990s, which have been exploited
to a wide range of potential industrial applications, including
MA.64102 Since the beginning of this millennium, other
forms of C-based absorbers with good absorption characteristics have appeared, due to advances in synthesis techniques
and optimized design approaches.103112 Most recently, graphene joined the C family for MA applications.113115
The characterization of absorbers can be done via standard measurement methods, i.e., direct measurement of the
reflection in free space with transmission eliminated by a
metal substrate attached on the absorbers, or indirect measurements of their electromagnetic parameters. The main
requirements for the absorbers are as follows: (i) it should
minimize the front-face reflection and impedance matching
at the air to absorber interface, (ii) it should increase the
absorption of electromagnetic waves through high values of
dielectric and magnetic losses, (iii) it is expected to be
applied in a wide frequency range, and (iv) it does not
require the use of an external magnetic field.116121 Microwave absorbing materials, including Salisbury screens, Jaumann absorbers, particle laden polymeric layers, and paints
are generally passive systems, although there is some work
dealing with active surfaces, such as variable impedance
surfaces.
Over the last decade, through recent technological
advances in nanoplasticsthe fusion of traditional plastics
and the developing field of nanotechnologymany exciting
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061301-4
results have demonstrated that polymers filled with C-based

materials have unique properties including improved
strength and durability, electrical conductivity, flame resistance, UV absorption, and reduced permeability. Excellent
absorbing materials are expected to have not only a strong
MA and a wide absorption bandwidth, but also to be lightweight, have a fine thickness, and be cost-effective.122 For
these reasons, C-based polymer materials are useful to materials scientists in guiding their ongoing efforts to design MA
materials. Since the early 2000s, a number of researchers in
academia and industry have investigated the possibility of
realizing flexible electronic device technologies, e.g., artificially structured soft materials with tunable electric and electromagnetic properties.123 Flexible circuit technology
attracts much attention in the electronics industry for portable applications because the flexible substrate can be rolled,
bent, and folded to fit a limited space where required. To
achieve the control required for technology will require a far
more complete understanding. Of particular interest is the
observation of unexpected physical effects, which emerge as
the size of carbonaceous fillers reaches a few nanometers. As
well as the fundamental nature of such question, this issue is
clearly of much interest to experimentalists who try to
explore multifunctionalities in nanostructures.
D. Objectives and outline
In the pursuit of technological advances at the nanoscale, MA of polymer composites with different allotropes
of C continues to draw substantial research interests both as
a fundamental subject and as a serious reliability concern in
nanoelectronics materials and devices. By controlling the
microstructural heterogeneities in these composites, unique
absorption responses at the macroscale can be achieved. This
necessitates developing systematic fabrication procedures to
optimize the MA. In what follows, we review the MA properties of polymer composites with C-based particles, including carbon fibers (CFs), CNTs, CB, graphene, and other
C-based materials. To our knowledge, no dedicated review
paper is available on this topic. We have endeavored to bring
together in one place diverse results so as to provide the
readers a fairly comprehensive panorama of our current
knowledge in terms of the influence of the carbonaceous
component in their composites on MA. Each of the results is
briefly described and, whenever possible, accompanied by
its implications for MA. While the descriptions here are not
extensive for reasons of space, we have provided relevant
pointers to the literature for a more in-depth study. Such a
review will be of much interest to the scientific and engineering communities, notably those working on nanocomposite
science and technology. We believe it is thus a sensible and
opportune time to revisit the claims made for high MA and
also make a comparison with other microwave absorbent
materials.
In spite of the recent advances, this research program still
presents quite a few challenges related to the following questions, such as what C-based filler properties determine the
MA features in polymer composites? How does one design
and optimize the C component to obtain the best absorption
J. Appl. Phys. 111, 061301 (2012)
characteristics of these composites? Some indications for the

possible answers stem from key experimental observations
that have motivated this review paper. However, despite the
substantial empirical literature on MA, the mechanism by
which various carbonaceous particles inhibit or exalt MA
remains largely unsolved.
The rest of the review is organized as follows. In Sec. II
we provide a brief description of the theoretical methods
most commonly employed to describe MA and dielectric
heterostructures with an eye on their strengths and limitations. Secs. III to VI survey the research to date on MA of
polymer nanocomposites with different types of C-based filler particles. The review is then concluded in Sec. VII with
some prospects given.
II. MA THEORY
Although the phenomenon of MA has been known for

many decades and the cause of the absorption is well formulated, the design of absorbers has occupied the minds of
many materials scientists and engineers for centuries.
Recently, the problem has garnered even more attention and
has become more important than ever. In addition to academic reasons, its practical impact on society has been recognized. The growing public concern about possible human
health effects in relation to weak radio frequency (RF) fields,
i.e., health hazards from environmental fields,124126 motivate the relevant research.
In this section, fundamental knowledge of microwave
absorption will be presented as well as an overview of mixture law theory. These two together provide a theoretical
route to an optimized design of absorbers. Microwave
energy, when incident on a lossy dispersive material, creates
heating within the material through the interactions of the
electromagnetic field with the materials molecular and electronic structure. Homogeneous and heterogeneous media analyzed within an effective medium approach are described
by two material parameters: the complex (relative) permittivity e e0 je00 and the magnetic permeability (relative)
l l0 jl00 . The terms e0 (and l0 ) are associated with
energy storage and e00 (and l00 ) are associated with dielectric
loss or energy dissipation within a material resulting from
conduction, resonance, and relaxation mechanisms. The loss
tangent of the dielectric material is tan d e00 =e0 , where d is
the dielectric loss angle of the material. Energy loss in a material illuminated by electromagnetic waves comes about
through damping forces acting on polarized atoms and molecules and through the finite conductivity of a material. It is
common knowledge in electromagnetism that the Poynting
theorem governs our understanding of the conservation of
power in linear, dispersive media.127 It states that the total
power (for a harmonic electromagnetic field of angular frequency x) entering a volume V through the surface S goes
partially into increasing the field energy stored inside V and
partially is lost into heat, i.e.,
D
E
D
E
@u
r:S j:E 2xIm e jEj2 l jHj2 ;
@t
(2.1)
where,
131.180.140.56 On: Tue, 30 Dec 2014 20:12:48
061301-5

dxe D 2 E
d xl D 2 E
;
u Re e0
jEj l0
jH j
dx
dx
J. Appl. Phys. 111, 061301 (2012)
(2.2)
h i denotes the time average over the period of the carrier

frequency, and S E H is the Poynting vector. The quantities e0 and l0 are the permittivity and the magnetic permeability of vacuum, respectively. The quantities E and H are
the electric and magnetic field intensities, respectively. The
quantity j accounts for both conductive and dielectric losses.
We observe that the conductive and dielectric losses are
indistinguishable with respect to the heat generated. Applying external electromagnetic fields to a composite material
implies that the electromagnetic waves come across a variety
of microscopic boundary conditions due to the inclusions
making the heterostructure. The resulting local field variations can have a very strong effect on energy absorption at
such boundaries because absorption depends quadratically
on the electric field intensity.
Figure 2 shows a multilayer microwave absorber that

consists of n layers of different materials backed by a perfect
electric conductor (PEC). For simplicity, we consider that
the electromagnetic wave is normally incident. Here di , gi
and ci denote the thickness, the complex intrinsic impedance,
and the propagation constant of the ith layer, respectively.
The conductivity for each individual layer of the absorber is
assumed to be zero. According to the transmission-line
theory,58,128,129 the wave impedance Zi of the ith layer is
given by,
Zi1 gi tanhci di
;
gi Zi1 tanhci di
(2.3)
p
p
where gi g0 li =e, ci j2pf le=c, g0 is the characteristic impedance of the free space; and li and ei are the relative
complex permeability and permittivity of the ith layer,
respectively. Considering that the metal plate is a PEC,
g0 0, the impedance of first layer reads as:
Z1 g1 tanhc1 d1 :
(2.5)
where C is the reflection coefficient. Through Eqs. (2.3) to

(2.5), we can see that the combination of the magnetic permeability and the permittivity (of both absorbing and substrate layers) satisfying the impedance matching condition
is the key to producing a high-performance microwave
absorber.
Specifically, for a single layer of absorber backed by a
PEC, which is a common situation in many studies discussed
above, the reflection loss is given as,
r

l

2pfd p

le 1
tanh j

c
e

RL 20 logr

:
l

p
2pfd

le 1
e tanh j c
(2.6)
The attenuation constant a (real part of the propagation

factor c), in nepers/m, is defined by,58,130
A. Microwave interaction with absorbers
Zi gi

Zn g0

;
RL 20 logjCj 20 log
Zn g0
(2.4)
The reflection loss (RL) of normal incident electromagnetic

wave at the absorber surface is given by,
a Rec
p
jx le
Re
c
q
p
x
l00 e00 l0 e0 l02 l002 e02 e002 ;
p
2c
(2.7)
where c is the speed of light in free space. Here we can see

that the attenuation constant is dependent on complex magnetic permeability, permittivity, and frequency. If we consider diamagnetic carbonaceous materials, MA is due to
dielectric losses. Before we proceed to consider the case of
pure dielectrics with l 1 j0, we first consider for the
purpose of comparison the case of ferrites with strong magnetic losses; their absorption being mainly due to the ferromagnetic resonance. To satisfy the minimum reflection loss,
according to Eq. (2.6) the perfect matching condition is,
r

l
2pfd p
tanh j
le 1:
e
c
(2.8)
p
Usually, 2pfd
le 1, as the thickness d is much smaller
c
than the wavelength and e is also small. It follows from
Eq. (2.8) that,
2pfd 0
l jl00 1;
(2.9)
j
c
which can be reduced to,
l0 0 and
l00
c
:
2pfd
We find that the matching frequency fm is,

c
:
fm
2pdl00
FIG. 2. Schematic of a multilayer microwave absorber with a normally incident wave. di, li, and ei denotes the thickness, relative magnetic permeability
and permittivity of the ith layer, respectively.
(2.10)
(2.11)
The matching frequency should be generally the same as the

natural resonance frequency, which can be given by,131133
131.180.140.56 On: Tue, 30 Dec 2014 20:12:48
061301-6
J. Appl. Phys. 111, 061301 (2012)
r
Ha ;
2p
(2.12)
where c=2p 2:8 MHz/Oe is the gyromagnetic ratio. The

anisotropy field Ha is given by,134
Ha
2jK1 j
;
l0 Ms
(2.13)
where K1 is the anisotropy constant and Ms is the saturation

magnetization. Larger saturation magnetization or smaller
anisotropy field will redshift the resonance frequency, which
also means an improved absorption bandwidth, because there
exists a trade-off between resonance frequency and absorption bandwidth.135
We now turn to the case of a dielectric absorbent.
Assuming that l 1 j0, Eq. (2.6) can be written as,
r

1

2pfd p

tanh j
e 1

c
e

RL 20 logr
(2.14)
:

1

p
2pfd

e 1
e tanh j c
FIG. 3. (Color online) Dielectric loss dependence of the maximum reflection loss for different values of e.
After some transformation, we obtain,

v
r!
u
x u
1
1
a p te00
1 2
:
tan d tan d
2c
(2.20)
p
e < 1, the best possible matching, i.e.,
As 1=e tanh j 2pfd
c
p
2pfd p
p
1=e tanh j c e , achieves maximum. As 2pfd
e 1,
c
the best possible matching condition is,
r
1
2pfd p
j
e:
(2.15)
e
c
At the matching frequency, the attenuation constant reads as,

v
r!
u
x u
1
1
1
:
(2.21)
1 2
a p t 00
tan d tan d
2d e
This can be reduced to,
B. A birds eye view on dielectric heterostructures

theory
e0 0;
e00
c
:
2pfd
(2.16)
This is quite similar to Eq. (2.10). At the best matching condition, we can calculate the maximum reflection loss as
follows:

1

1
e

RLmax 20 log
(2.17)
:
1

1
e
After some transformation, we obtain,
0
4

RLmax 20 log@1
2 e00 tan d
1
1
A:
(2.18)
tan d
Note that tan d tan1 d is monotonically decreasing,

8 tan d < 1. Thus, maximum reflection loss should be evaluated by considering both e00 and loss tangent. The usual case
is that larger e00 give rise to larger loss tangents, thus an optimized e00 and associated loss tangent can be expected to
achieve the maximum absorption condition (too small or too
large e00 will not be in favor of absorption), as shown in Fig. 3.
This is further confirmed by the attenuation constant,
x
a p
2c
q
p
0
e e02 e002 :
One long-standing issue and rich area of research in the

theory of composite materials is the determination of their
effective transport properties that relate average flux fields to
average gradient fields. See, e.g., Ref. 136 for a review. A principal question with these materials is how the effective permittivity of a composite medium can be evaluated as a function of
the intrinsic permittivity of the phases, their volume fraction,
their shape and size, and their geometrical arrangement associated with the material mixture. As far as is known, theories and
experiments have been able to highlight some facets of this
issue but not reveal the complete physical picture. The recent
reviews of Sahimi,137 Milton,138 and Sihvola139 summarized a
broad range of theoretical techniques which have, by now, been
applied to solve this central challenge. Complementary to semiempirical analytical approaches, accurate computer simulations
(reviewed in, e.g., Ref. 140) have produced a full electromagnetic description of a suspension of inclusions having arbitrary
shape and size, subject to a complex dielectric environment
as explicit function of the volume fraction of inclusion. The
physical parameters characterizing these systems are numerically tunable so that it is viable for one to do the theoretical
design and optimization of novel optimized multifunctional
materials.141
1. Mixture laws and effective medium approaches
(2.19)
It is well known that the filler particles volume fraction

dependence of permittivity exhibits nonlinearity at relatively
131.180.140.56 On: Tue, 30 Dec 2014 20:12:48
061301-7
J. Appl. Phys. 111, 061301 (2012)
low filler particle contents, i.e., / 10 15 vol. %. One

common approach to permittivity calculations is based on
mixing laws. For the rest of this section, we consider two
(popular ones) of them among many that have been suggested in the literature; first, the Maxwell Garnett (MG) law,
e e1
e2 e1
/
:
e 2e1
e2 2e1
(2.22)
However, this is a special case dealing with spherical monodisperse particles. A second, alternative to the MG mixing
law, i.e., Lichteneker and Rothers law,
ek / e2 k 1 / e1 k ;
(2.23)
where k is within the range [1,1], is often found in the literature. Their validity, though widely accepted in the dilute
limit, is sometimes debated on theoretical grounds. In previous literature, mixing laws have sometimes produced (quantitatively) incorrect results in evaluating permittivity.140 The
advantages as well as the effectiveness of different mixing
laws have been discussed by Brosseau and Beroual.140
Effective medium analysis (EMA) is widely known for
being an alternate formulation of phenomenological mixing
laws, and appears in many review papers and textbooks as a
useful calculational tool for various statistical dielectric and
mechanical problems within the long-wavelength description
of the wave propagation.136,137,140,141 Once an order parameter, the CB volume fraction / in the host matrix, has been
identified, one constructs a permittivity functional
ee1 ; e2 ; / that satisfies the self-consistency requirement in
the long-wavelength physics description. Generally speaking, these approaches make use of the idea that a medium
containing inclusions of another phase can be approximated
as a homogeneous material. The underlying assumption, i.e.,
effective properties depend only on the materials constants
of the pure phases and their volume fractions, is of course an
approximation, and the quality of the theoretical predictions
can hardly be controlled.136142 A classic example of an
effective model is the Bruggeman symmetric equation which
can be written, for spherical particles, in the form,
1 /
e e1
e e2
/
0:
e 2e1
e 2e2
(2.24)
There are reasons to doubt the validity of the Bruggeman

prediction over a large range of / values. Despite its generality, Eq. (2.1) hinges on certain implicit assumptions. One is
that the typical inhomogeneity length scale in the heterostructure is much smaller than the wavelength of the electromagnetic wave probing the system. Another one is that only
dipolar interactions contribute to the polarization. All details
of the microstructure are encoded in the order parameter /.
Another assumption is that a continuum representation of the
system is effective. However, incorporation of CB nanoparticles into a polymer material can lead to large property
changes that are difficult to comprehend by extension of the
effects of macroscopic filler additives. Notably, this is due to
the much larger density of interface between the two phases
of different electromagnetic parameters. The nature of the
relations between these interfaces, of nanometric extension,

and macroscopic (effective) properties, such as permittivity,
is not completely understood.
The theory of percolation (critical) phenomena is relevant to a very large number of physics problems. These
include, on the condensed-matter side, the insulatorconductor transition.141143 Going back to the critical behavior of percolative heterostructures can give rise to a
bewildering array of physical effects,141,144148 especially
when they are combined with finite-size effects.143,149153
The experimental activity141,143,153 has been steady. To
describe how the effective conductivity versus inclusion volume fraction behaves close to the isotropic percolation
threshold /c of the conducting constituent, the following
formulas can be employed,143,153155
r r1 /c /s
for / < /c ;
(2.25)
r r2 r2 =r1 st ;
r r2 / /c t
for / > /c ;
(2.26)
(2.27)
where s and t are critical exponents having the so-called universal values, i.e., s 0:7 and t 2 in 3D, r1 is the electrical
conductivity of the insulator matrix and r2 is the electrical
conductivity of the conductive fillers. Because the percolation
model is independent of the nature of the filler particles and
the nature of the insulating host matrix, it is possible to apply
to most polymers filled with powdery materials. At this stage
it is worthwhile stressing the fact that while such an approach
can give valuable insights into the CB volume fraction dependence of the effective conductivity, the intrinsic value of
the filling phase is generally unknown. Scher and Zallen predicted that the percolation threshold is close to 17 vol. % for
conducting spherical particles distributed randomly within a
3D dielectric matrix.156158 However, it is well established
that the CB particles form aggregates with more or less irregular and tenuous shapes. For low structure CB the aggregates
are small and regular, while for high structure CB the aggregates typically contain a few hundreds of particles. Because of
their often somewhat elongated shapes the probability of
aggregate-aggregate contact is larger than it would have been
had the aggregate been a compact sphere. Hence, the conduction threshold is usually lower than the 17 vol. % of filler particles, as is the case of the composites investigated here. In
addition, the insulator-conductor transition width is often large
due to variations in the particle aggregate size, geometry, and
orientation.158
During the past decade, different prescriptions to deal
with the problem of modeling the dielectric behavior in multicomponent percolative materials over the entire range of
phase concentration have been proposed in the literature.
Each of these methods improves one failing or another in the
EMA, but they often bear a semiempirical character, and none
can be considered universal and parameter-free. In particular,
McLachlan and co-workers159163 made an important contribution by proposing a simple two exponent phenomenological
percolation equation (TEPPE) that depends on s and t for
characterizing the effective complex permittivity e/,
131.180.140.56 On: Tue, 30 Dec 2014 20:12:48
061301-8

1 /
1=~
s
J. Appl. Phys. 111, 061301 (2012)
1=~
s
e1 e1
1=~
s
1=~
s
e1 1 /c =/c e1

1=~t
e2 e1=~t
1=~t
e2 1 /c =/c e1=~t
0;
(2.28)
where e1 denotes the permittivity of the host matrix.

With regard to Eq. (2.28), several remarks are appropriate. First, because in practice e1 , e2 , /c , s~, and ~t can be determined from experimental measurements, the proposed
method requires no empirical fit parameters making it ideal
for predicting e/2 . However, from recent experimental evidence it has become clear that much earlier modeling of
composites is based on values of many quantities that are
difficult to obtain. For example, any attempt to determine
the absolute value of the permittivity of powder materials
can be seriously challenged depending on the experimental conditions and the technique employed in the
measurement.12,164169 Second, it is worth observing that the
TEPPE is not a mean-field theory analogous to Eq. (2.24)
that neglects order-parameter fluctuations. One attribute of
this equation is that the two behaviors (mean-field Bruggeman model for / /c and if one sets s~ ~t 1), and critical percolation model for / /c and if one sets s~ s and
~t t) are recovered as limiting cases of Eq. (2.28). It is also
important to remark that while in principle it is possible to
observe a singularity at /c 1=3 within the symmetric
Bruggeman model as the ratio e2 =e1 ! 1, in practice /c in
Eq. (2.28) can be varied between 0 and 1. Third, another feature of Eq. (2.28) is that it only depends on the volume (surface) fractions, or particle number densities, of constituents
in the mixture. This originates from the important fact that
Bruggemans formulation is based on a dipolar analysis, and
does not take into account the multipole correlations, i.e.,
many-body problem inherent in the electromagnetics of the
particular system. It is now well accepted that for dispersed
two-phase mixtures other interface descriptors (local structure) should appear in the averaged equation for the permittivity. Furthermore, it turns out that no reference to any
internal length scale is explicitly included. Fourth, in a series
of papers, McLachlan and co-workers explored the validity
of this equation and analyzed many experiments.159163 To
match the experimental data an appropriate choice of the
unspecified constants s~ and ~t in Eq. (2.28) were used and
treated as fit parameters. However, while this approach has
been found capable of reproducing the salient trends of
e/ e0 / ie00 /, the empirical nature of the TEPPE
restricts its predictive power.
2. Computational approaches
Note that the present-day numerical techniques allow us

to deal directly with the experimentally relevant range of the
model parameters. The electromagnetic response of composite
materials should be circumvented by the use of validated theoretical methods.144,146,147,149,170173 As both computing power
and the efficiency of computational methods are steadily
increasing, it is becoming possible to investigate new compos-
ite materials through computer simulations, before they have

even been synthesized. Many theorists have examined this
subject by performing ab initio calculations, e.g., densityfunctional theory (DFT),174176 or finite element method
(FEM).177 The finite element method (FEM) has considerable
flexibility because arbitrary shapes can be modeled. The FEM
takes much more time and memory than the finite-differencetime-domain (FDTD) because it is required to solve linear
equations in each time step. Consequently, the FEM is mainly
used in the frequency domain and eigenmode analysis. For a
general presentation of the finite element modeling of nondestructive material evaluation, we refer the interested reader
to Ref. 178. There is a vast literature on the FEM in the context of engineering. It is also worth noting that FEM software
with flexible mesh generators, robust equation solvers, and
versatile post-processors have become available in recent
years. Interested readers are referred to Refs. 179183 for a
general introduction of FEM. Other relevant numerical techniques include the different variants of boundary integral equation (BIE),140,184 first-principles molecular dynamics,185187
finite integration algorithm,187189 Monte Carlo (MC),190 multipole moments,191,192 differential evolution (DE),193 genetic
algorithm (GA),194 or FDTD.195197 The widespread use of
the World Wide Web (www) offers the unprecedented opportunity of delivering information through an easy-to-use and
easy-to-learn interface. Nowadays, the front-end provided by
popular www browsers is known and available to millions of
users, and has become a de-facto standard for the dissemination of information. Complementary and up to date information on the FDTD methods is available at http://www.fdtd.org,
and fast Fourier transform (FFT) method198,199 on a variety of
systems where only two phases are present. Related to the
problem at hand, the notions of random close packing (RCP)
and maximally random jamming have been discussed by Torquato and co-workers.141,200 The main problem is that real
calculations are not easy, and the challenge is to find a reasonable balance between the choice of method, desired accuracy,
and computational expense. The most desirable approach for
fully harnessing the dielectric properties of heterostructures at
the macroscale must be inherently multiscale (both in time
and space) because its evolution is mediated by a combination
of atomic level dynamics, defect physics, nonequilibrium thermodynamics, and transport kinetics. Most numerical analyses
reported thus far have fallen short of this goal for a variety of
reasons. While numerical approaches may be exact in principle, the true form of the randomness is unknown. The high
computational cost of averaging over a large set of system
configurations makes it difficult to obtain well-converged estimates of the observables. Current research is pushing available approximations toward the description of fluctuations on
the hierarchy of length scales that are relevant to the problem.
Actually, the cross-fertilization between computational and
analytical work in the area of composite materials is rapidly
growing. Unfortunately, current feasible representations for
the a priori knowledge of the microstructure of the composite,
such as the correlation functions that specify the average microscopic arrangement of the constituents, require significant
experience in the construction of reliable and solvable microstructures. The primary reason for the limitation of exact
131.180.140.56 On: Tue, 30 Dec 2014 20:12:48
061301-9
calculations of the property of interest, especially for continuum models, has been the lack of efficient algorithms suited
to generate collections of random packings of particles (disks,
spheres). It is perhaps fair to observe that theories that start
with similar algorithms may arrive at different descriptions of
their properties. Yet even if this disorder representation problem were solved in its entirety, the would-be composite designer would still face the formidable tasks of (i) finding the
starting entities that will maintain their structural integrity
throughout the synthesis process, and (ii) controlling the morphology he or she wished to engineer. As testimony to these
difficulties, it is not uncommon to find in the literature disagreements over the predictions of the porosity, mean coordination number, and radial distribution function.201,202
With the guidance of absorption and dielectric heterostructures theories detailed in Sec. II, we will discuss in
detail the polymer absorber with each kind of C filler. The
emphasis is placed on the description and analysis of absorption features, i.e., maximum absorption, absorption bandwidth with respect to the thickness and filler content. The
methods of tailoring the C fillers and the design of macroscopic structure are also presented. In addition to providing
the readers sufficient information for choosing and designing
C-based absorbers for a targeted MA application, an overall
evaluation of the C-filler loaded polymer composites is also
given to clearly identify their practical value. In view of the
rich class of C-based fillers that have been discovered and
produced, we lay out the following discussion in a sequence
conforming to the significance from the application point of
view. As such, we start from CF-based composites which
have been identified as the core engineering material superseding conventional metals and alloys as critical structural
components. This is followed with CNT-based polymer
composites and then with CB-filled materials. Finally, we
complete this presentation by giving a flavor of other forms
of C-based polymer materials containing C coils, C onions,
and C nanofibers. To make this review easier to follow, Table I summarizes the absorption properties for the various
composite materials discussed in this review paper.
III. CF-BASED POLYMER COMPOSITES
Carbon fiber reinforced polymer composites (CFRP)

have been the focus of many fundamental and engineering
studies due to their unique mechanical performance compared
with their low density. It was reported that 28000 tons of CF
with an estimated price of US$50200/kg were produced in
2006, yet still cannot meet the demand.203,204 An increasing
amount of CF is used in the aircraft industry to reduce weight
and, hence, improve the performance of aircraft, although
some issues such as in-flight structural health monitoring
remain unresolved.204 It is also desirable to know if CF-filled
polymer composites can absorb electromagnetic waves to
reduce interference and radar backscattering. Unfortunately,
CFRP containing large concentrations ( 6070 vol. %) of
CFs having typical dc conductivity (105106 Xm at microwave frequency) are quasi-reflective when they interact with
electromagnetic waves. It is generally believed that
CFRP-polymer composites can be used for electromagnetic
J. Appl. Phys. 111, 061301 (2012)
interference shielding application,205 but these materials are

not fully adapted for MA.
A. Continuous-fiber composites
One of the key aspects in materials engineering is to tailor materials in terms of morphology and structure to modify
their macroscopic properties and meet the requirements of a
specific application. If the material is intrinsically nonapplicable, one can transform it to be applicable via appropriate tailoring approaches. In this regard, it is possible to
modify CFs to make them applicable for MA applications.
For example, Zhu et al.206 coated pitch-based CF (PCF)
using amino-modified polyorganosiloxane with low conductivity and surface area to increase the contact resistance.
Nonwovens with various PCF contents up to 100 vol. %
were characterized from 8 to 18 GHz. A complicated dependence of the electromagnetic characteristics depending
on PCF content was observed. For small PCF concentrations,
the absorption dominates the attenuation (reflection is rather
small), while at larger concentrations, the reflection dominates the attenuation. Quantitatively, a maximum absorption
of 18 dB was achieved at 18 GHz for a PCF concentration of
2 wt. %, with a large absorption bandwidth (818 GHz). In
this paper, absorption or reflection losses are presented in
absolute values. This absorption level is larger than that of
nonwovens containing CB, such as reported by Lopes and
co-workers,207 i.e., a 4 GHz (812 GHz) absorption bandwidth was obtained for the sample containing 33 wt. % CB.
Wu et al.208 pointed out that activated CF (ACF) is an effective way to increase MA because ACF can significantly exalt
multiple reflections with a longer propagation distance inside
the composites. This was later confirmed by Zou et al.209
who reported an enhanced absorption of 16.6 dB for composites containing ACF with a 12 GHz absorption bandwidth
(618 GHz). Because wasted CF can be regenerated for the
production of ACF,210 the excellent microwave properties of
ACF make them materials of choice for MA materials. Other
work worth mentioning is that of Zeng et al.,211 who showed
that a CuO/Co layer on the surface of CF has a significant
effect on MA, the maximum absorption is 23.0 dB for CuO/CF
and equal to 42.7 dB for CuO/Co/CF at matching thickness of
2 mm. The decoration of CFs surface by magnetic nanoparticles has also a profound impact on MA, arising from the
additional absorption mechanism introduced by these particles, such as Neel relaxation, and the interface created
between the particles and CF, which can promote interfacial
polarization. Most important, the improvement of impedance
matching when magnetic particles are present leads to an
enhanced absorption as compared to the case of pure CFs.
ACFs can also be structured in a specific design termed CFfelt screens,212 in analogy to traditional metallic frequency
selective surface, in either cross-linked (Fig. 4(a)) or vertical
manners, and embedded into an epoxy matrix. When interacting with an incident microwave field the CF-felt screens
behave as a waveguide when they are cross-linked or as an
antenna when they are vertically aligned. The MA characteristics are found to be strongly dependent on the geometric
parameters of the fiber array, such as the spacing between
131.180.140.56 On: Tue, 30 Dec 2014 20:12:48
Matrix
PAN-based CF (activated)
Pitch-based CF (activated)
CF (activated)
CF
Cuo/CF
Cuo/Co/CF
CF
Filler fraction, wt%
MT, mm
[MA]max, dB
F, GHz
A, GHz
Ref.
55.5%
2%
0.43 %
0.43 %
18.7%
4.0
10.0
4.0
4.0
1.7
2.0
18.0
30.6
18
26.8
10.2
23
42.7
31.6
12.4
18
8.2
11.9
8.2
10.8
16.5
10 (8-18)
10 (818)
12 (618)
0
2.4 (7.69)
2.7 (9.312)
10 (818)
[212]
[206]
[209]
[209]
[211]
[211]
[213]
60 %
5.0
38
6.9
4.7 (4.5-9.2)
[214]
30%
2.0
1.2 (4.35.5)
and 2.4 (15.417.8)
[217]
18.6
32.5
16
11
5.2 (12.818)
4.2 (8.212.4)
[129]
[41]
22
13.8
24.27
17
27.5
8.8
13.5
15.36
7.6
10.9
2.6 (7.510.1)
3.1 (12.015.1)
4.8 (13.218)
2.7 (6.59.2)
4 (9.513.5)
[76]
[76]
[233]
[233]
[269]
17.9
25.78
26.39
14
16
24.8
18
16
17.5
21.9
22.7
12.5
27.7
21.5
19.2
22.9
21.8
28.7
18
7.18
7.71
8
8
11
9
9
11
8.5
15.6
9
10
9.4
7.8
11.4
12.2
10
2 (16.018.0)
14 (418)
2.2 (6.89)
3 (69)
4 (59)
16 (218)
7 (6.513.5)
16 (218)
16 (218)
6 (612)
4.2 (13.417.6)
2.4 (8.110.5)
2.3 (911.3)
1.6 (8.710.3)
1.8 (7.29.0)
3 (10.113.1)
3.4 (10.814.2)
1.4 (9.711.1)
[269]
[90]
[90]
[83]
[83]
[66]
[68]
[72]
[72]
[230]
[274]
[268]
[264]
[263]
[265]
[265]
[261]
[308]
Epoxy
CF
Linear low density polyethylene

(LLDPE)/Ethyleneoctene
copolymer (POE)
Epoxy
Polyurathane (PU)
SCF
Single-layer, Felt screen

Single-layer, Non-woven
Single-layer
Single-layer
Multilayer structure
CFRC foam,
Double layer: absorbing
layer(ferrites)
substrate layer (CFRP)
Single layer
SCF
SCF
Double layer: ferrite SCF

Graded double layer
0.2%
0.39%
SWCNT
SWCNT
MWCNT
MWCNT
Ni/MWCNT
Single layer
Single layer
Single layer
Single layer
Single layer
5%
2%
20%
4%
15%
1.5 (ferrite) 0.5 (SCF)

3.35 (1 g paste) 0.65
(11.1 g paste)
2
2
1
2
0.9 6 0.07
MWCNT
Low helicity MWCNT
Worm-like MWCNTs
MWCNT
MWCNT/Co
MWCNT/Fe
MWCNT/CoFe2O4
MWCNxNT/Fe
MWCNT/Fe
MWCNT ferrite
Fe/MWCNT
Fe/Fe3C-MWCNT
MWCNTs/Er2O3
MWCNTs/ Sm2O3
MWCNT/Ag
MWCNT
CNT/Co
MWCNT
Single layer
Single layer
Single layer
Single layer
Single layer
Single layer
Single layer
Single layer
Single layer
Single layer
15%
30%
30%
16.7%
16.7%
16.7%
16.7%
40% ferrite 18.6% CNT
10%
5%
10%
5%
0.9 6 0.07
3
2.8
2
2
1.2
1.4
2
2
2
3.5
2
2
2
1
1
1
12.9 (0.7 11.5 0.7)
Cross-linked PU
Cross-linked PU
Varnish
Polyethylene terephthalate (PET)
Phthalazinone ethersulfone
ketone (PPESK)
PPESK
Paraffin
Paraffin
Olefin
Olefin
Epoxy
Epoxy
Epoxy
Epoxy
Paraffin
-c
Epoxy
Epoxy
Epoxy
PU
Single layer
Single layer
Single layer
Sandwich, GFRC PU
foam CFRC
15.66 and 17.37 4.6 and 16.4 GHz
J. Appl. Phys. 111, 061301 (2012)
Configuration of composite
Epoxy
Polyester
Epoxy
Epoxy
Epoxy
Filler
061301-10
TABLE 1. Summary of the absorption properties for the various polymer composites filled with carbonaceous particles discussed in this review paper.a
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Filler
MWCNT
PU
MWCNT
Epoxy
GFRP
Rubber
Natural Rubber
Paraffin
Epoxy
poly-(ethylene oxide) (PEO)
Phenol-formaldehyde
cement (PFC)
Nomex honeycomb sandwich
composites
Epoxy
Epoxy
Filler fraction, wt%

5%
MT, mm
12.5 (1 10.5 0.8 0.2)
[MA]max, dB
28.5
F, GHz
9.9
A, GHz
1.2 (9.610.8)
Ref.
[308]
5%
9.9 (1 2.7 1 5 0.2)
24
9.5
3 (8.711.7)
[308]
30%
7% (1st layer),
5% (2nd layer)
10%
50% CI, 40% CB
11.1%
5% CB 50% SiC
2.6%
2
0.65 mm 1.9 mm
40
37.5
11.3
9.8
2.9 (10.113)
2.8 (8.611.4),
[294]
[128]
25%
1.9
22
6
3
1.8
1.5
2
22
23.3
22
41.5
38.8
16.5
12.7
11.6
14.5
16.2
9
16.5
12
14.5
3.9(9.613.5)
5.5 (4.56.5, 12.716.2)
5.6, 12.418
6 (713)
4.1 (13.918)
5 (1015)
4.4 (13.618)
[295]
[310]
[305]
[299]
[113]
[114]
[324]
Polyaniline (PANI)/CB
CB
Configuration of composite
Sandwich GFRC PU foam
GFRC CFRC
Sandwich GFRC PU
foam GFRC
PU foam CFRC
Single layer
Double layer
CB
CB Carbonyl iron (CI)
heat-treated carbon black
CB SiC
Chemically reduced graphene
Ni coated graphene
graphite flakes
Single layer
Double layer
Single layer
Single layer
Single layer
Single layer
Single layer
Carbon microcoil
(A type, Fig. 11(a))
Carbon microcoil
(B type, Fig. 11(b))
Carbon nanocoil
Sandwich
0.007%
9.6 (0.58 7.34 0.58)
18
12.4
3.2 (10.814)
[108]
Sandwich
0.007%
9.6 (0.58 7.34 0.58)
13
12.2
3.3 (1114.3)
[108]
Sandwich
0.007%
9.6 (0.58 7.34 0.58)
32.23
12
9.1 (8.918)
[111]
CNF (type 1)d

CNF (type 2)
Single layer
Single layer
4%
4%
4
4
26
22
18.4
16
1.8 (1819.8)
1.6 (15.216.8)
[107]
[107]
Matrix
PU
061301-11
TABLE 1. Continued.
a
The results summarized here concern primarily the maximum of the MA, the corresponding frequency, and the absorption bandwidth. The table includes results available from the literature up to August 2011.
MT: matching thickness, [MA]max: maximum of MA, F: frequency at [MA]max, A: absorption bandwidth over 10 dB.
b
The activation procedure is detailed in the corresponding reference.
c
Information on the matrix is missing here because the absorption results are calculated from the permittivity and magnetic permeability rather than direct measurement on planar samples.
d
Type 1 is different from type 2 in terms of dispersion techniques, which are detailed in the corresponding reference.
J. Appl. Phys. 111, 061301 (2012)
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061301-12
J. Appl. Phys. 111, 061301 (2012)
FIG. 5. Smith chart input impedance for a ferrite-epoxy absorber with a

metal plate and CFRP plate as the substrate, respectively (reprinted with permission from Ref. 214, copyright 2007 Wiley and Sons).
enhanced. On the other hand, sandwich structure with mesophase pitch C foams215,216 and glass-fiber composite (matching layer) exhibit excellent MA.
B. Short-fiber composites
FIG. 4. (a) Geometry of the inductive activated CF felt screens (IACFFSs);

(b) Effect of a/b on the microwave absorbing properties of the composites
containing IACFFSs (reprinted with permission from Ref. 212, copyright
2006 Elsevier).
the fibers and width of the fiber strips (see Fig. 4(b)). For an
optimized configuration, 30 dB maximum absorption and
10 GHz (818) bandwidth can be achieved.212 The combination of different types of screens is shown to improve the
absorption. It should be noted that although CFs link together
to form a network, such layering of screens will not make
the composite reflective but instead will enhance MA. A
similar design concept can be found in a CFRP grid
absorber, consisting of a CFRP grid and absorbing foam.213
MA characteristics are driven by thickness and geometry of
the unit cell. An optimal geometry has been suggested and
yields a maximum absorption of 31.63 dB with a wide
absorption bandwidth, 818 GHz. Note that although the
absorber shows strong absorption, its relatively large thickness of 18 mm compromises its performance and limits its
applications.
Two final comments are in order. In Ref. 214, it has
been observed that the double layer absorber containing CF
can achieve impedance match (Fig. 5), whereas the metalbacked absorber cannot. Thus the absorption is greatly
Different from continuous fibers, short fibers can be

sparsely dispersed as filler particles in the polymeric
matrix and have been extensively explored for MA
applications.217221 Two main advantages of these materials
are that they allow broadband MA along with significant
decrease of the absorbers thickness,41,222 and they have a
high permittivity even at low volume fractions of inclusion.223
Different approaches to use short CFs for designing
absorbers have been reported. One method is to randomly
disperse them into the host material. Ling et al.217 reported a
double absorption peak (4.6 and 16.4 GHz) for composites
containing 30 vol. % short CFs, with diameter 5 mm and average length 60 mm, and respective absorbing peak values
of 15.66 dB and 17.37 dB. However, the corresponding
absorption bandwidths, which are respectively of 1.2 and
2.4 GHz, are narrow. Another method is to integrate them
into multilayer structures, such as Salisbury or Jaumann
structures. Shen et al.129,218 designed a double layer
absorber consisting of composites containing ferrites and
short CFs, yielding an improved absorption performance as
compared with single layer structures. Furthermore, twolayer absorbers have a significantly enhanced absorption
bandwidth. Neo et al.41,219 analyzed the dielectric properties
of CF-filled polymer composites, based on Lichteneker and
Rothers law (Eq. (2.23) with k ! 0), and managed to optimize the absorption properties of multilayered structures
containing these materials in terms of the number of layers
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and the thickness of each layer. They found, both experimentally and theoretically, that a 4 mm double-layer structure shows the best absorption features with maximum
absorption at 32.5 dB and absorption bandwidth covering the
whole X-band. Within this perspective, another study which
should be highlighted here is that of Mitrano and co-workers:222 They suggested a model based on genetic algorithm
techniques and the MG formula (Eq. (2.22)) for designing a
Jaumann-type CFRP-based multilayer structure to obtain a
broadband absorption.222 The third approach is to fabricate
hybrid multilayered composite structures by mixing short
CFs and other types of filler particles. In this way, double
layer structures with lossy layers containing mixtures of ferrites and short CFs were developed.218,221,224 For relatively
small loadings of CFs, the absorption performance is significantly improved. The possibility that short CFs can act like
bridges to link the ferrite particles was suggested to explain
these observations.
The absorption behavior of composites containing short
CFs can be modeled by an appropriate effective medium
analysis, such as those described in Sec. II. In addition,
recent studies have demonstrated the ability of numerical
techniques225,226 for the design of single layer and multilayered absorbers containing short CFs.
IV. CNT-BASED POLYMER COMPOSITES
As previously mentioned, an important consideration for

the designer of microwave absorbers concerns the absorption
efficiency with respect to weight. In this sense, it goes without question that the composite consists of non-corrosive,
lightweight polymer and the nano-scale particles have absolute advantage. Carbon nanotubes (CNTs) meet the criterion
essentially. Compared with CB-filled polymers, they have
stronger mechanical properties with typical values of the
elastic modulus of the order of 1 TPa, and tensile strength
within the range 50500 GPa.227 More important, CNTs can
be fabricated to yield good semiconducting properties with
charge carrier mobility as high as 105 cm2/Vs, and current
carrying capacity over 109 A/cm.228,229 An immediate benefit
associated with loading a polymer matrix with CNT is that
much smaller CNT content 0:35% is needed to obtain
the same conductivity level than for CB particles 20%.
This is of particular attraction for one to realize costeffective and lightweight absorbers. As CNTs are nonmagnetic materials, their MA originates either from polarization,
Ohmic losses, or multiple scattering due to the large specific
surface area. We shall note here that the different types of
CNTs have been graded for their use in MA.230 Compared
with single-walled CNTs (SWCNTs), multi-walled CNTs
(MWCNTs) have more defects due to their complicated
structure and higher permittivity, and their absorption is
mainly due to dielectric relaxation. In a series of papers,71,231
it has been shown that defects and impurities of CNTs have
become impediments to properly describing the polarization
mechanisms and Ohmic losses of the composite materials.71,231 The microwave absorption of CNT composites
depends on multiple factors, which will be discussed at
length in what follows.
J. Appl. Phys. 111, 061301 (2012)
A. MA properties of CNT-based materials

1. CNT loading dependence
As the amount of CNT increases from below to above the

percolation threshold of composite samples there will be a
significant impact on their effective dielectric properties and,
hence, their MA characteristics. Such behavior may be
regarded as arising from passage of an insulating state through
a conducting state, as described by Eq. (2.27). However, the
CNT concentration dependence of the permittivity and conductivity data is generally not consistent with the universal
value of t in Eq. (2.27). The role of aggregates143 and the thermal activation of electrons232 have been suggested as possible
mechanisms for explaining this discrepancy. Liu et al.76 found
that the MA can be optimized at a given concentration close
to the percolation threshold and that the absorption peak shifts
with CNT content. These observations are consistent with
other studies.233 From the published experimental studies it
appears that the loss tangent increases slightly when the CNT
content is below the threshold. With increasing CNT content
in the sample the dielectric losses rapidly increase due to
wave reflection rather than absorption. Some experimental
reports234,235 claim a correlation of the electrical (geometrical) percolation threshold and mechanical (rheological) percolation. Of particular interest is that the dielectric relaxation of
CNT composites is closely associated with the mechanical
damping properties. We shall note that the CNT content dependence of the dielectric loss tangent resembles that of the
elastic modulus loss tangent.236 As the typical aspect ratio of
CNTs is usually between 100 and 1000, the percolation
threshold is within the range 0.11 vol. %: this corresponds to
maximum tensile strength and Youngs modulus observed for
CNT/epoxy composites.237239
The observed redshift of the absorption peak with
increasing CNT content can be explained by the increase of
the dielectric losses240243 according to Eq. (2.16). Few
papers have quantitatively discussed the dependence of the
absorption resonance frequency with CNT content. As
shown in Fig. 6, fitting the experimental data of Ref. 76
FIG. 6. (Color online) Dielectric loss dependence of matching frequency.

The solid (red) line is a fit of experimental data76 to Eq. (2.16).
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J. Appl. Phys. 111, 061301 (2012)
yields a reasonable agreement with the behavior predicted

by Eq. (2.16). Clearly, the larger is the dielectric loss, the
lower is the matching frequency. Size and thickness polydispersity of the CNTs, as well as the experimental uncertainty
related to the microwave characterization can contribute to
discrepancies of the experimental data with Eq. (2.16).
In addition, CNT concentration can be varied to manipulate the absorption bandwidth. For example, Liu et al.76
showed that the absorption bandwidth broadens from 6.48.2
(1.8 GHz) to 7.510.1 (2.6 GHz) to 12.015.1 GHz (3.1 GHz)
for SWCNTs/PU nanocomposites. Thus, a multilayer structure with optimized wire concentration in each layer is likely
to realize a broadband MA.
2. Geometry of particles
The aspect ratio of CNTs is a crucial parameter in determining the charge and wave transport mechanisms in such
composite materials. It is generally understood that a large
aspect ratio implies a large excluded volume, defined as the
volume around an object into which the center of another
similar object is not allowed to enter if overlapping of the
two objects is to be avoided. A smaller percolation threshold
/c is expected if the aspect ratio is increased. Despite CNT
being an archetypal material, interpretations of the percolation characteristics in CNT-filled polymers vary dramatically
in the literature depending on which theoretical model is
used. The abundance of literature makes it hard to describe
universal features of the percolation characteristics, which
depend on the details of the model and/or material. Specifically, for stick-shaped fillers with large aspect ratio (l
a),
where a is the radius of the stick, and l denotes its length, the
standard EMA theory predicts that,244
/c / a=l2 ;
(4.1)
whereas the MG formula suggests that,
/c / a=l1=2 :
However, computational studies244247 revealed that,
/c / a=l:
(4.2)
(4.3)
Equation (4.3) was verified over a wide range of aspect ratios

for various CF- and CNT-polymer composites.240,243,248 The
proportionality constant in Eq. (4.3) was found to be equal to
1,249,250 or to 1.4.245,249 However, the theoretical prediction
fails in many real nanocomposite systems by either being too
big250252 (see Fig. 7) or too small.253,254 The latter can be
conveniently explained by the poor dispersion of the particles.255 The former case is worth some discussion. As the
model does not take into account the inter-particle or
the matrix-particle interactions or kinetic effects such as the
Brownian motion of particles, it is a purely statistical percolation. A kinetic theory of percolation was introduced to
take into account these effects.255 Thus, it is not surprising to
find out that, due to the increasing mobility of shorter wires,
the (kinetic) percolation threshold decreases with decreasing
aspect ratio.256 Unfortunately, data were obtained over a
limited range of aspect ratios and a precise understanding
of the relationship between the CNT aspect ratio and the
FIG. 7. Theoretical prediction of upper and lower bounds for the percolation
threshold (in wt%) as a function of the particle aspect ratio determined from
the excluded volume approach. As a comparison, the experimentally determined percolation threshold for CVD-grown MWCNTs in an epoxy resin is
shown (reprinted with permission from Ref. 25, copyright 2004 Elsevier).
percolation threshold of the composite material is lacking.

The rationale behind these studies is that by uncovering the
detailed influence of the aspect ratio of CNT on percolation
threshold, theory may provide guidance to experiments and
even suggest new materials with minimum percolation
thresholds at which maximum absorption can be achieved.
The aspect ratio also plays an important role for CNTs
decorated with filled magnetic particles, i.e., a larger aspect
ratio can increase the magnetic anisotropy field of filled
CNTs, and consequently influence the absorption features
induced by natural ferromagnetic resonance as inferred by
Eq. (2.11) and Eq. (2.13). Thinner wires will shift the matching frequency higher. However, thin wires will also have
small content of magnetic nanoparticles. This will decrease
the saturation magnetization and shift the matching frequency lower. The overall absorption characteristic is determined by the competition between these two mechanisms.
The consensus among computational studies suggests
that MA is favored by large tunneling conduction. Hence,
the contact resistance should be minimized. For example,
Kovacs et al.234 modeled the contact resistance in CNTfilled composites as,
r
l U2x1
;
2p2 R Rc
(4.4)
where r is the dc conductivity, l is the length of the CNT

particle, r and R denote respectively the radius and resistance
of a single particle, Rc is the contact resistance, x is an empirical numerical constant, and U is the filler volume fraction.
Within this modeling approach, increasing the diameter of
CNTs has the effect of lowering the contact resistance.
3. Dispersion of particles
It is likely that the morphology of the composite material is largely dependent on the dispersion procedure of the
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J. Appl. Phys. 111, 061301 (2012)
CNTs. For low CNT content (smaller than the threshold concentration predicted by the kinetic theory of percolation),
dispersion is easily realized. For larger concentrations, the
aggregation mechanism will be of paramount importance to
determine the percolation transition and, hence, the maximum absorption, which is expected to occur at percolation
threshold. The best dispersion conditions do not necessarily
lead to the maximum tunneling conductivity, because it is
well recognized that a good dispersion leads to the formation
of an insulating polymer layer between the CNTs. This
absorption layer will eventually reduce the conductivity. To
minimize this polymer sheath effect, various processing
techniques, e.g., solvent processing,235 have been suggested.
The dependence of the MA characteristics on the dispersion
of particles has been reported in many experimental works;
see, e.g., Refs. 107, 233, 236, and 257. Pre-treatment258 and
stirring rate234 were found to be important steps of the dispersion process. Generally speaking, a good dispersion is
also crucial for the mechanical performance of CNT-based
polymer composites. This and recent research in stretchable
C nanoelectronics has indicated that further progress requires
multidisciplinary programs, incorporating nearly every field
of traditional study, from chemistry, materials science,
computation, and physics, to mechanical and electrical
engineering.
4. Interfacial properties
From the published theoretical and experimental studies

on polymer composites it is clear that the interphase and
interface properties are governed by the properties of the
polymer, the type of filler particles, and the fabrication process. These interface properties will eventually influence the
MA characteristics. For example, Fan et al.233 measured the
microwave absorption spectra of CNT/polyethylene terephthalate (PET) and CNT/varnish composite samples with the
same kind of CNTs and very similar fabrication process.
Larger maximum MA was evidenced for the latter. These
observations led to the suggestion that a large density of
boundaries at the interface is essential for a strong interfacial
polarization. The effect of interfacial polarization was also
demonstrated by comparing the MA characteristics of CNT/
polymer and decorated CNT/polymer composites.87,99,259
B. Magnetically filled or decorated CNTs
Previous publications have considered magnetized

CNTs by filling66,68,87,97,259268 or coating100,101,269272 hollow
CNTs with nanoparticles or nanowires, or unpurified CNTs
with Fe catalyst.65,257,273 Some of these publications have
indicated that MA is greatly enhanced because of the contributions of magnetic losses and impedance match (see
Fig. 8).66,68,87,271,273 For instance, Lin and co-workers274
reported an enhanced absorption for Fe-filled CNTs compared
with unfilled CNTs. It is worth asking if this larger absorption
is due to the magnetic phase. From Eqs. (2.11) and (2.16) one
can show that the answer is that this is not due to the contribution of the magnetic losses but rather to the increased dielectric
losses. The magnetic particles content is so small that the magnetic effects are weak.83,259,275277 A similar conclusion was
FIG. 8. MA characteristics over the 218 GHz band of CoFe2O4 particles,

pure CNTs and CNTs/CoFe2O4 nanocomposites (a) and the high-resolution
transmission electron microscopy (HRTEM) image of the CNT shows
graphite shells and lattice fringes of CoFe2O4 (b) (reprinted with permission
from Ref. 68, copyright 2006 American Institute of Physics).
arrived at by Naab and co-workers278 for similar materials. The

increase of the static magnetization saturation279,280 and the
dielectric/magnetic losses as the concentration of filled or
coated magnetic particles is increased highlights the complex
interplay between dielectric and magnetic properties and disorder.281 Another area where this interplay has a profound impact
is the significant increase of coercivity for polymers containing
magnetically loaded CNTs compared with polymers containing
only magnetic particles;279,280 this has potential for MA
because larger hysteresis losses have been reported.35,263 Other
mechanisms that could contribute to MA with filled CNTs
include defects that are introduced during the filling process,
which will be the source of multiple scattering and induce interfacial polarization;231,259,282 and the local properties of nanoparticles, which are greatly modified by the quantum confinement
effect. Kubo theory283 predicts that the discrete energy levels of
the encapsulated nanoparticles in the CNTs will absorb the
microwave energy through electrons hopping. It is worth noting
that because these effects are not limited to magnetic nanoparticles, various experiments were performed on CNTs filled with
different kinds of nanoparticles including Ag,265 Sn,94,
Sm2O3,263 and Er2O3,264 and interesting phenomena such as
enhanced absorption bandwidth94,263 were observed. However,
it should be noted that the resultant MA performances can be
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degraded due to the destruction of the CNT integrity during the

filling and decoration processes.265
Today, our knowledge of the impact of magnetically filled
or decorated CNTs on MA remains limited. Little is known
about the nature of the transition between a situation for which
the absorption mechanism is driven by magnetic losses to its
counterpart, for which dielectric losses are the main contributor
for MA. In the former, the Landau-Lifshitz-Gilbert formalism,284 Snoeks law,135 the Kittel equation,132 and the effective
medium theory dealing with magnetic permeability should be
considered to evaluate the electromagnetic properties of such
absorbents.285289 It is also beneficial to ask if there is an alternative way to circumvent the complex chemical process of doping CNTs but still be able to take advantage of magnetic
absorbents in order to increase the MA of CNTs. Polymer matrices with embedded ceramic or inorganic filler particles, e.g.,
ZnO (Ref. 290) or TiO2,82 are widely explored materials for
dielectric and magnetic applications.291 However, a better solution is to design multilayer structures. Within this context, Park
et al.292 showed that a sandwich structure (see Fig. 9) with front
layer containing CB particles and several layers of foam containing CNTs achieves excellent MA performances.
V. CB-BASED POLYMER COMPOSITES
Carbon black (CB) particles are common filler particles

used for modifying the mechanical, electrical, and optical
properties of a polymer matrix into which they are dispersed.15,43,293 MA is another important application. Compared with magnetic ferrites, CB particles will lead to a
broader frequency range of application up to the THz (infrared) due to their very fine primary particle size (typically,
10 nm) and much smaller density ( 2 g/cm3). However, their
J. Appl. Phys. 111, 061301 (2012)
narrow absorption bandwidth is unfavorable. Then, one has

to resort to multilayer structures in order to broaden the
absorption band. In what follows, we shall discuss MA of
CB composites with single layer and multilayer structures
separately.
A. Single layer microwave absorber
Wu et al.294 fabricated core-shell polyaniline/CB nanocomposites and found that the maximum absorption of 40 dB
is observed within the X-band with CB concentration of
30 wt. %. However, the absorption bandwidth is quite narrow
(3 GHz). Adding 6 vol. % CB into a glass/epoxy matrix
yields a sample with a maximum absorption of 32 dB within
the X-band and 2.7 GHz absorption bandwidth.128 Kwon295
showed that CB/silicone rubber exhibits a 24 dB minimum
reflection loss within the X-band and 3.9 GHz absorption
bandwidth. Of particular interest is the observation that these
measurements concern supercolative CB-filled polymer samples for X-band absorption. These measurements can be
understood by considering that, for low CB volume fractions,
an increase of CB will increase the conductivity by tunneling, which favors MA. A large CB concentration will prevent the wave from propagating into the absorber due to the
front surface reflection. As evident from these measurements, the observed percolation threshold in CB-based
absorbers can be very rich and, as discussed in many
places,143,155,296,297 the corresponding mechanical, electronic, and transport properties of percolating networks are
strongly affected by the system percolation. It is well established that the filler dispersion becomes difficult for CB concentrations well away from the percolation threshold and this
is detrimental to the improvement of the mechanical properties observed at low CB volume fractions.298300 From a
practical perspective, we note that our work123 and recent
results by other groups indicated that improving the MA of
CB-filled composites can be realized by catalyzing the CB
particles with SiC,301 BaTiO3,302 Fe(Co)5,220,301304 nanosized Fe,305 and ferrite304,306 particles, which have better
MA performance and larger percolation threshold. On the
other hand, some experiments also showed that that the
absorption features of these composites can be precisely controlled with mechanical stress.307 The ability to control
the CB mesostructure will be instrumental in developing
CB-based polymer materials for MA.
B. Multilayer microwave absorbers
FIG. 9. Schematic designs of sandwich structured absorbers. The surface

layer consists of glass fabric with carbon black. CB6 and CB5 represents
6 wt% and 5 wt% carbon black, respectively. The main absorbing layer is
PU foam containing MWCNT. The substrate is carbon fibre reinforced polymer (CFRP). The sequence and thickness of each model is labelled in the
graph (reprinted with permission from Ref. 308, copyright 2006 Elsevier).
In general, a multilayer microwave absorber is characterized by a set of layers with different MA materials in
order to enhance the overall absorption features. As was
briefly mentioned in Sec. II A, one of the main issues for the
design of such absorbers lies in the minimization of the overall reflection coefficient in a specific frequency range and a
specific range of incidence angles. The front layer is
expected to give the best impedance match, while the
absorbing layer is supposed to dissipate the microwave
energy as much as possible, and the substrate layer is
expected to be reflective to prevent any escape of the microwave. In Ref. 128 (CB2), Oh et al. proposed a double-layer
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structure with the same CB/glass/epoxy composite but with

different CB contents. However, it failed to exhibit better
absorption properties than the single layer of the same thickness at optimized content. A multilayer structure consisting
of a thermosetting resin-impregnated fibrous sheet (such as
glass fiber reinforced polymer (GFRC)), a rubber sheet with
CB, and a reinforced resin sheet (such as CFRP) was also
suggested as an efficient microwave absorber.308 The two
main advantages of these structures are as follows: (i) the
surface layer can act as a matching layer to improve the
absorption as well as to reduce the total thickness of the
absorber;309 and (ii) more possibilities are available to optimize the MA characteristics. For example, with a double
layer structure containing carbonyl-iron and CB, respectively, we can tune the microwave absorption feature by
varying the parameters of each layer, such as the thickness
ratio and filler content310 (see Fig. 10). As was found similarly for the case of single layers, other type of fillers, e.g.,
SnO2,311 can be exploited to modulate the electromagnetic
parameters of double-layer structures.
VI. OTHER TYPES OF C-BASED POLYMER

COMPOSITES
As previously noted, recent experiments on polymers

filled with conducting components structured at the nano-
FIG. 10. (Color) RL curves of double-layer absorber containing CB particles and carbonyl iron (CI) particles #1#6, of which the thickness of the
matching layer and the absorbing layer is uniform 2 mm. (a) The mass fraction of CI in the matching layer is set to 50%, the mass fraction of CB in the
absorbing layer of samples #1, #2 and #3 are 40%, 50% and 60%, respectively. (b) The mass fraction of CI in the matching layer is set to 70%, the
mass fraction of CB in the absorbing layer of samples #4, #5 and #6 are
40%, 50% and 60%, respectively (reprinted with permission from Ref. 310,
copyright 2009 Elsevier).
J. Appl. Phys. 111, 061301 (2012)
scale have shown that these materials form an interesting

class of broadband microwave absorbers.312 Compared with
absorbents that are structured at larger length scales,
nanocarbon-based composites involve complex absorption
mechanisms related to a hierarchy of scale.313,314 This is for
many reasons. First, quasi-particles, such as plasmons or
polaritons, rather than the free electrons, are responsible for
the charge transport mechanisms. Second, the macroscopic
(effective) behavior of the composite should be analyzed
within the framework of nano-electromagnetism rather than
based on classical electromagnetism. Third, the tunneling
effect can be important due to the formation of multichannels. However, the difficulty in dispersing these fillers
in polymers can be detrimental to their expected MA performance. All these characteristics distinguish nanocarbon
particles from the micro- and macro-carbonaceous particle
fillers. In the following, we discuss some salient features of
the MA properties of such materials.
A. C micro-/nano-coils
Carbon coils (see, e.g., Fig. 11) can be fabricated by the

CVD technique at the micro- or nanoscale. Various electromagnetic and MA experiments were performed on C microcoils.108,315,316 These experiments suggested that the absorption properties depend on the chirality of the micro-coils,
which influences their dielectric behavior. However, the MA
FIG. 11. SEM images of C micro-coils with different chiralities, obtained by a

vapor phase catalytic cracking process with different gas flow rate. (a) the coil
diameter is 4 mm, pitch is about 0.5-0.8 l/mm. It was produced with gas flow
rate of 150 ml/min. (b) the coil diameter is 20 mm, pitch is about 1-4 l/m. It
was produced with gas flow rate of 200 ml/min (reprinted with permission
from Ref. 108, copyright 2005 Chinese Academy of Sciences).
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properties are not impressive, with a small bandwidth of

1015 GHz and a maximum absorption of 18 dB. Nano-coils
were also explored for MA application.109111 These studies
revealed that they exhibit superior MA than micro-coils. For
example, Zhao et al.111 measured the microwave properties
of Nomex honeycomb sandwich composites filled with C
nano-coils and found that their reflection loss has the absorption bandwidth of 8.918 GHz and a maximum absorption of
32.23 dB at 12 GHz. The substrate and front layer of this
composite structure contain glass fibers. The absorption
could be enhanced if glass fibers are substituted with CFs for
the substrate layer. Because C coil is a dielectrically lossy
material, coating or catalyzing it with magnetic particles represents an effective method to improve the MA performance
of polymer composites containing such filler particles.109,112
B. Onion-like C
Soon after the discovery of onion-like C (OLC) by Kuznetsov et al.,317 electromagnetic studies were performed for
shielding and MA application. OLCs are quasi-spherical
nanoparticles consisting of fullerene-like C layers enclosed
by concentric graphitic shells (Fig. 12). They are predicted
to have different properties from other C nanostructures,
such as graphite, nano-diamond, or CNTs, due to their highly
symmetric structure and may serve uses in different applications. OLCs can even serve as nanocapsules for drug
delivery systemsthe external graphite layers providing
protection to substances contained within and possibly serving as a template for the attachment of desirable functional
groups. Until recently the investigation of the unique chemical and physical properties of OLCs was limited by the lack
of a method that produced them with well-ordered structures
and in sufficiently large quantities. Several recent publications have shown that magnetic nanoparticles encapsulated
within graphite-like layers may find applications as microwave absorption materials,318 particularly in the Ka band
which covers the frequencies of 26.540 GHz.104,319 From
FIG. 12. HRTEM image of onion-like C powder, which was produced by

annealing of nanodiamonds powder in vacuum at 1800 K (reprinted with
permission from Ref. 318, copyright 2009 Elsevier).
J. Appl. Phys. 111, 061301 (2012)
the published experimental studies it is clear that OLCs are

characterized by complex frequency dispersion consistent
with their structure. It was suggested that the MA depends
on a variety of parameters. For instance, increasing the nanodiamond annealing temperature will promote the extent of
graphitization and the amount of conductive channels within
OLC aggregates, i.e., with annealing temperature increased
from 1400 K to 1800 K, the transmission minimum at
28 GHz decreased from 3 to 13 dB.314 These experiments
also suggest that aggregate size plays a key role. That is,
larger sizes result in larger polarization,320 and consequently
larger absorption, e.g., the maximum attenuation at Ka band
was found to increase by 20% when the aggregate size is
increased from 85 to 180 nm.104 Other observations reveal
that metallic admixtures such as Cr or Fe have strong
impacts on MA. At the Ka band, it was reported319 that OLC
powders with Fe admixtures present larger attenuation
( 4050 dB) than pure OLCs, or OLCs containing other
admixtures. Compared with conventional absorbents such as
iron carbonyl, OLCs present superior MA performances in
the Ka band. Now, what happens when OLCs are embedded
in a polymer matrix? It was reported that when the OLC
concentration is sufficiently large ( 20 wt. %), smaller
aggregates reduce the percolation threshold,104 and increase
the MA.314 It can be drawn from these experimental results
that the electromagnetic response of OLCs and their composites with polymers can be modulated by annealing temperature, aggregate size, and of course the types of the initial
diamonds and polymer matrix.
C. C nanofibers
In analogy to CNTs, C nanofibers (CNFs) are a onedimensional nanocarbon material, characterized with a large
aspect ratio, high mechanical properties, and excellent electrical and thermal properties.321 However, because CNFs
have a higher density of defects compared to CNTs, their
mechanical properties are reduced. However, one major
advantages of CNFs is their availability and cheaper production cost relative to CNTs. The large aspect ratio of the
CNFs promotes larger conductivity and permittivity and a
smaller percolation threshold compared with CNTs. Over the
frequency range 0.518 GHz, a maximum absorption of
18 dB was found close to 10 GHz for CNF/epoxy composites.322 This is not as good as for CNT/epoxy and CB/epoxy
composites fabricated in the same conditions, but they
achieve equal absorption bandwidth of 3 GHz for smaller filler loading and matching thickness. As with other types of
nanoparticles, some experimental reports claim that the MA
features of CNF-filled composites are related to the filler
content and dispersion quality. For instance, Nanni et al.107
reported an improvement of the maximum absorption,
increasing from 0.2 to 18.3 dB over the 820 GHz bandwidth
when the CNF content is increased from 1 wt. % to 4 wt. %
for CNF/epoxy composites. Additionally, these authors
showed that a better dispersion of CNFs into the polymer
permits obtainment of a higher permittivity and a larger MA.
To improve the absorption efficiency of CNFs, researchers
also tried to mix them with magnetic absorbents.323 Both
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J. Appl. Phys. 111, 061301 (2012)
absorption maximum and bandwidth were found to be significantly enhanced for a specific mixing ratio. In view of the
likely economic feasibility of CNFs, these materials are viable solutions for microwave absorbers.
D. Graphite
A couple of studies have been devoted to flaky graphite.

In the first one, Fan et al.324 prepared a phenol-formaldehyde
cement based absorber using ball-milled flaky graphite. This
leads to a maximum absorption of 25.5 dB at 14.5 GHz and
absorption bandwidth of 2.9 GHz. A longer ball-milling time
along with a good dispersion of graphite increased the MA. In
the second study, expanded graphite flake/novalac-phenolic
resin was explored.325 It was shown that this composite material exhibits a dielectric loss tangent larger than unity and
absorption smaller than 10 dB in the whole X-band range.
VII. SUMMARY AND FUTURE PROSPECTS
In this review, we have discussed fundamentals of MA and

reported on the development of C-based microwave absorbers.
The development of polymers filled with carbonaceous nanostructures with tailored dielectric, magnetic, and MA properties
represents a key issue in many technological fields. We have
critically examined both theoretical and experimental aspects
of these topics. On the experimental side we have reviewed
state-of-the-art experiments and stressed the difficulty and open
questions in analyzing such experiments. Four interesting features of polymer composites filled with carbonaceous particles
are their lightweight structures, their moldability, their thin
matching thickness, and their broad bandwidth; however, most
of the experimental results point out that the carbonaceous material needs to be doped or surface modified, for example,
CNTs decorated by magnetic particles, in order to have strong
MA. Even if these smart materials are promising electromagnetic wave absorbers in the laboratory, it remains a challenge to
develop suitable techniques for mass production of these
polymer-filled nanocomposites.
A. Future prospects
We note that active development in this field has already

successfully demonstrated the great promise of graphenepolymer composites for a range of technological advances,
from electronic devices to biosensors.326330 Of particular interest to us is that researchers have found applications of graphene in microwave absorption. For example, the authors of
Ref. 113 reported a 38.8 dB absorption at 16 GHz with 2.6
vol. % graphene content. Another, more recent, batch of
microwave experiments was conducted on nickel-coated graphene114 It was demonstrated that MA is due to dielectric
losses, and that nickel coating transforms the graphene from
paramagnetic to ferromagnetic, thus improving the maximum
absorption from 6.5 dB to 16.5 dB at 118 GHz. Zhang
et al.115 fabricated PMMA/graphene composites (see Figure
13) and found that when the matching thickness is 1.5 mm
and graphene content is 1.8 vol. %, the maximum absorption
is 18 dB at 9.25 GHz and the frequency region in which the
maximum reflection loss is more than 10 dB is 9.514.6 GHz.
FIG. 13. (a) SEM image of the cross-section of PMMA nanocomposite

microcellular foam with 1.8 vol % graphene sheets; (b) TEM image of welldispersed graphene sheets in a cell wall of the PMMA nanocomposite
micro-cellular foam with 0.8 vol % graphene sheets. The arrows point to the
cell wall surfaces (reprinted with permission from Ref. 115, copyright 2011
American Chemical Society).
These experiments that have appeared recently are certainly a

good start, but more are needed in order to have a good mechanistic understanding in terms of absorption process and to
optimize the absorption performance.
Other interesting applications such as microwaveassisted purification and functionalization of CNT particles,231,331 or microwave curing of composites,78,332 add to
the importance and interest of this research field. Similarly,
multilayer structures offer us unlimited possibilities by introducing more degrees of freedom for controlling and eventually fine-tuning the MA characteristics. As commented by
Hirsch,3 it is likely many novel forms of C will be discovered. Synthetic C allotropes represent a family of fascinating
and esthetically pleasing architectures with outstanding
materials properties.
B. Final thoughts
These last few examplesand what we have discussed

in this reviewshow that the quest to understand MA in
polymer composites filled with carbonaceous materials is far
131.180.140.56 On: Tue, 30 Dec 2014 20:12:48
061301-20
from over. One of the characteristics of these soft materials

is that they have developed in the hands of scientists with
backgrounds in organic chemistry and materials science; this
group is particularly inclined philosophically to mixing. A
characteristic of this work has been its focus on the function
rather than on structure. Regarding technological applications, finding materials that show either very good MA (for
camouflage applications) or very poor MA (for invisibility
cloaks)333 is needed. There is clearly a need to advance our
theoretical tools substantially. Parallel to the experimental
achievements and insights, the community of plastic nanoelectronics should develop powerful ab initio multifunctional
computational approaches that capture the underlying
physics. On the basis of our longtime experience with the
computational analysis of dielectric heterostructures,334 we
consider that it is a major undertaking to examine the modeling of the effects of strain of carbonaceous materials filled
polymers by multiscale numerical simulation, e.g., Monte
Carlo and molecular dynamics techniques. The multiscale
geometry of these materials is expected to have a significant
effect on their transport properties. The formation of cracks
under tension, or of bending fatigue tests, eventually affect
the electrical and electromagnetic properties.307,335 Systematic ageing studies on polymeric materials are especially informative because the failure mechanisms can be tracked.
The damage and fracture behavior of materials characterized
by microscopic structural disorder is determined by the distribution properties at the scale of the microstructure. Accurate predicting of the collective chain dynamics of the
elasticity networkthe local strain field produced by the
external stressis key to predictive modeling of physical
aging in C-filled polymers.
Because of the rapid developments in fundamental science and technology and interdisciplinary nature of the field,
it is formidable to give an exact prediction of future directions. However, there is no doubt that ingenious ideas will be
put forth and lead to, say, novel nanostructures with optimized MA.
ACKNOWLEDGMENTS
Lab-STICC is UMR CNRS 6185. We acknowledge support from the Conseil General du Finiste`re post-doctoral fellowship program.
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The isolated C atom has a 1s22s22p2 configuration with filled 1s and 2s states
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forms of sp2 C. Through sp2 hybridization of the atomic orbitals, two neighboring atoms can bond strongly via both s- and p-states. As a result of the
high p-bonding energy, graphite is energetically slightly more stable than
sp3-bonded diamond-like structures under ambient temperature and pressure.
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the most exciting form of C, ever since it was made by the mechanical exfoliation of graphite. Its unique band structure of mass-less fermions due to the
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(Ref. 4).
337
There are three main approaches for introducing particle fillers into a
polymer matrix. The first one is the mechanical mixing of the molten
polymer phase with the particles. A second one is based on the in situ formation of the particles in the presence of the already formed polymer matrix. The third strategy consists in dispersing the particles in a monomer
solution (precursor of the host matrix), which is then polymerized
(Ref. 20). The effective utilization of particles in composite applications
depends strongly on the ability to disperse the particles homogeneously
throughout the matrix without destroying the integrity of the particles.
Rational design of any device requires a fundamental understanding of
the physical properties of these materials, and how they depend on the
way in which filler particles and polymer chains are connected, fillerfiller interactions, and the state of dispersion of filler particles. Modern
technologies aim to tailor such properties for specific applications in the
aforementioned industries enabling composites to be cost-effectively
manufactured by injection molding or extrusion techniques. On the other
hand, these materials have also proved to be model systems to examine
the underlying molecular level underpinnings of the mesostructure and
macroscopic properties of confined polymer systems. Essential to understanding these issues is a clear delineation of the intrinsic vs extrinsic
properties of the filler particles. However, studies of interactions between
polymer chains and filler particles are influenced by complex factors
including particle size, surface area, aggregate structure and surface activity that have precluded the development of a first-principles understanding of particle-filled composite materials. For example, Obrzut and
co-workers (Ref. 21) have shown that the blending of CNTs into
polymer matrices leads to composite materials whose properties can
depend strongly on the flow history to which the materials have been
subjected.
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A review and analysis of microwave absorption in polymer composites filled with

JOURNAL OF APPLIED PHYSICS 111, 061301 (2012)

APPLIED PHYSICS REVIEWS

A review and analysis of microwave absorption in polymer composites

Author to whom correspondence should be addressed. Electronic mail:

IV. CNT-BASED POLYMER COMPOSITES . . . . . .

C 2012 American Institute of Physics

F. Qin and C. Brosseau

Carbon (C) is the fourth most abundant chemical element

J. Appl. Phys. 111, 061301 (2012)

F. Qin and C. Brosseau

system. This electronic distribution is strongly affected

To a large extent, the theoretical and experimental

J. Appl. Phys. 111, 061301 (2012)

MA has also been discussed in the context of aluminum (Al)

F. Qin and C. Brosseau

results have demonstrated that polymers filled with C-based

J. Appl. Phys. 111, 061301 (2012)

characteristics of these composites? Some indications for the

Although the phenomenon of MA has been known for

F. Qin and C. Brosseau

J. Appl. Phys. 111, 061301 (2012)

h i denotes the time average over the period of the carrier

Figure 2 shows a multilayer microwave absorber that

where C is the reflection coefficient. Through Eqs. (2.3) to

The attenuation constant a (real part of the propagation

A. Microwave interaction with absorbers

The reflection loss (RL) of normal incident electromagnetic

where c is the speed of light in free space. Here we can see

We find that the matching frequency fm is,

The matching frequency should be generally the same as the

F. Qin and C. Brosseau

J. Appl. Phys. 111, 061301 (2012)

where c=2p 2:8 MHz/Oe is the gyromagnetic ratio. The

where K1 is the anisotropy constant and Ms is the saturation

After some transformation, we obtain,

At the matching frequency, the attenuation constant reads as,

This can be reduced to,

B. A birds eye view on dielectric heterostructures

Note that tan d tan1 d is monotonically decreasing,

One long-standing issue and rich area of research in the

It is well known that the filler particles volume fraction

F. Qin and C. Brosseau

J. Appl. Phys. 111, 061301 (2012)

low filler particle contents, i.e., / 10 15 vol. %. One

There are reasons to doubt the validity of the Bruggeman

relations between these interfaces, of nanometric extension,

F. Qin and C. Brosseau

J. Appl. Phys. 111, 061301 (2012)

where e1 denotes the permittivity of the host matrix.

Note that the present-day numerical techniques allow us

ite materials through computer simulations, before they have

F. Qin and C. Brosseau

Carbon fiber reinforced polymer composites (CFRP)

J. Appl. Phys. 111, 061301 (2012)

interference shielding application,205 but these materials are

Filler fraction, wt%

Linear low density polyethylene

Single-layer, Felt screen

Double layer: ferrite SCF

1.5 (ferrite) 0.5 (SCF)

15.66 and 17.37 4.6 and 16.4 GHz

J. Appl. Phys. 111, 061301 (2012)