Low field permittivity of ferroelectric-ferrite ceramic composites: Experiment

and modeling
Cristina Elena Ciomaga, Cristina Stefania Olariu, Leontin Padurariu, Andrei Victor Sandu, Carmen Galassi et al.

Citation: J. Appl. Phys. 112, 094103 (2012); doi: 10.1063/1.4764037

View online: http://dx.doi.org/10.1063/1.4764037
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 JOURNAL OF APPLIED PHYSICS 112, 094103 (2012)

Low field permittivity of ferroelectric-ferrite ceramic composites: Experiment

and modeling
Cristina Elena Ciomaga,1,a) Cristina Stefania Olariu,1 Leontin Padurariu,1
Andrei Victor Sandu,2 Carmen Galassi,3 and Liliana Mitoseriu1,a)
1
Faculty of Physics, Alexandru Ioan Cuza University Iasi, Blvd. Carol I, No. 11, 700506, Romania
2
Romanian Inventors Forum, Iasi 700089, Romania
3
ISTEC-CNR, Via Granarolo, No. 64, I-48018 Faenza, Italy
(Received 21 May 2012; accepted 9 October 2012; published online 2 November 2012)
The dielectric properties of xNiFe2O4-(1x)Pb0.988(Zr0.52Ti0.48)0.976Nb0.024O3 ceramic composites with
different volume filling factors (x ¼ 2, 5, 10, 20, 30, 40, 50, 60, 70 wt. %) prepared by sol-gel method
have been investigated in the frequency range (106  109) Hz. A reducing effective permittivity with
increasing the ferrite amount was observed as result of the “sum property.” The experimental results
have been compared with the effective permittivity values predicted by effective medium
approximation (EMA) models and finite element method (FEM) calculations. The comparison was
aimed to evaluate the appropriateness of the results of the two approaches in describing the effective
dielectric properties of the composite with contrasting permittivities and to understand the role of
microstructural characteristics on the dielectric response in a broad filling factor range. The best
description of the experimental data in overall filling factor range is given by the results of FEM
calculations which used realistic microstructures and among the EMA models, by the Lichtenecker’s
formula. VC 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4764037]

I. INTRODUCTION different compositions and microstructures remain an active

area in basic and applied material science research.9–12
Modern science and technology applications demand for
The spinel ferrites and perovskite ferroelectrics show a
new properties that rarely can be accomplished in single phase
good phase compatibility and the interconnectivity of the phases
structures. Therefore, various combinations of di-similar
which can be controlled by their relative amount and processing
materials in composites are designed, produced, and investi-
methods. Ferrites present ferrimagnetic behavior and possess a
gated, while the simulation techniques able to predict their
unique combination of moderate permittivity, spontaneous mag-
functional properties have been continuously developed. The
netization, and low dc-conductivity. The ferroelectric materials
composite electroceramics have a remarkably wide variety of
with perovskite structure, e.g., PZT doped with donor ions of
practical applications, including their use for: microwave
Nb5þ, normally have superior dielectric, elastic, and piezoelec-
antennas, sensors, resonators, oscillators, filters, phase shifters,
tric properties and a good electromechanical coupling factor.
attenuators and amplifiers, microwave resonance devices,
The study of the effective permittivity of composites has
micro/nanoelectromechanical systems, etc.1–8
been the subject of many discussion over several decades.
Due to their dielectric and magnetic properties, the
However, it is generally difficult to conclude because there
ferrite-ferroelectric composites are suitable for microwave
are not enough experimental data in a wide frequency range
devices and components. By modifying the dielectric permit-
and concentration of the phases in conjunction with the micro-
tivity or/and the magnetic permeability, these composites
structural characterization.11 Despite large research effort, the
can be easily used to adjust the output/input impedances, the
composite materials have a number of striking fundamental
resonance frequencies, the quality factor (losses) and the
properties which are not fully understood. There are many the-
attenuation or the amplification. The behavior of the material
oretical approaches for the description of electric and mag-
composite can be often dramatically altered by the variation
netic properties of the magnetoelectric composite materials,
of the relative volume fractions of the composite constitu-
related to the particular mixing degree and the volume fraction
ents, while for a given composition, the phase interconnec-
of the component phases.13,14 The effective medium theories
tivity can completely modify the functional properties.
take into consideration the effects of inclusions in the bulk
These changes in the properties of composites with composi-
material in order to deduce the effective macroscopic response
tional variations and phase interconnectivity cannot usually
of the composite mixtures. The most common effective me-
be described using a simple formalism in overall composi-
dium approximations (EMA) models for predicting the dielec-
tional range. Therefore, studies to compare the effective con-
tric properties in composites are: (a) Maxwell-Garnett (MG)
stants with the experimental values in composites with
approximation corresponding to isolated spherical inclusions
embedded in a continuous background matrix,15,16 (b) Brug-
geman (BG) approximation that consider the properties of ma-
a)
Authors to whom correspondence should be addressed. Electronic trix or host the same as of the effective medium itself and
addresses: cristina.ciomaga@uaic.ro and lmtsr@uaic.ro. assumes a symmetry between inclusion and background

0021-8979/2012/112(9)/094103/7/$30.00 112, 094103-1 C 2012 American Institute of Physics

V
094103-2 Ciomaga et al.
phases,17–19 while (c) Lichtenecker (LI) mixing formulae are
derived by differential analysis and is considered appropriate
for inhomogeneous microstructures.20–22
The finite element method (FEM) is another approach
allowing to calculate the electric field distribution inside the
composite and the effective dielectric constant. By compari-
son with EMA approximations, FEM takes into consideration
the shape of composites, the local permittivity, and performs a
more rigorous calculation of the local potential without sup-
plementary approximations. The effective permittivity as a
function of the volume fraction of inclusions can be calculated
using this method in all the compositional range, by consider-
ing realistic microstructures. For any type of approximation, it
is important to consider the intrinsic value of the dielectric pa-
rameters of the two phases (if available), since permittivity
and conductivity of the two phases and mainly of the compos-
ite are frequency dependent and might be strongly affected by
extrinsic phenomena, making thus a comparison of the experi-
mental data with model predictions difficult.22
In this paper, we have studied the frequency-dependent
complex permittivity of xNiFe2O4-(1x)Pb0.988(Zr0.52
Ti0.48)0.976Nb0.024O3 composites with x ¼ 2, 5, 10, 20, 30, 40,
50, 60, 70 wt. % compositions, by using impedance spectros-
copy in the range of frequency (1 MHz–1 GHz). The
obtained results were discussed in terms of the particular
mixing degree and volume fraction of constituent phases.
The experimental dielectric constant values on xNiFe2O4-
(1x)Pb0.988(Zr0.52Ti0.48)0.976Nb0.024O3 (xNF-(1x)PZTN)
ceramic composites with various compositions at higher
frequency have been compared with the results of EMA and
FEM models. The prediction of intrinsic properties of the
composite materials with various concentrations of the con-
stituent phases and with different types of microstructures is
an important tool for understanding their properties and for
their use in microwave electronic devices.
II. EXPERIMENTAL DETAILS
The xNiFe2O4-(1x)Pb0.988(Zr0.52Ti0.48)0.976Nb0.024O3
(NF-PZTN) composites with x ¼ 2, 5, 10, 20, 30, 40, 50, 60,
FIG. 1. Backscattering SEM-images of the polished surface of xNF-(1  x)PZTN ceramic composites with: (a) x ¼ 10 wt. %, (b) x ¼ 30 wt. %, and (c) x ¼ 70 wt. %
(black contrast: NF, white contrast: PZTN).
J. Appl. Phys. 112, 094103 (2012)
70 wt. % were synthesized by in situ processing based on a
sol-gel method presented in Ref. 24. Di-phase composites
containing only ferrite and perovskite phase in the nominal
amounts were densified as ceramics by sintering the pow-
ders at temperatures of 1200  C/1 h. Using the sol-gel
method, we have tried to control trough the microstructural
characteristics the functional properties of the studied sys-
tem, by preserving both the intrinsic properties of the parent
phases (i.e., ferroelectric and magnetic order) and to
ensure optimum conditions for the coupling between them
(in this case, to have a good mechanical coupling). The
microstructures have been studied by using a scanning elec-
tron microscope (SEM) (VEGA/TESCAN instrument) in
backscattering mode on the polished surfaces of the com-
posite ceramics.
The electrical properties at room temperature in the fre-
quency range of 1 MHz to 3 GHz were determined by using
an E4991A-RF impedance/Material Analyzer. The electrical
measurements were performed on parallel-plate capacitor
configuration, by applying Pd–Ag electrodes on the polished
surfaces of the sintered ceramic disks.
A. Microstructural analysis
The dielectric and magnetic properties of the
ferroelectric-magnetic composites depend strongly on their
microstructure. The backscattering SEM analysis for the NF-
PZTN ceramics with compositions x ¼ 10, 30, and 70 wt. %
are shown in Figures 1(a)–1(c). Dense and homogeneous
composites with a good dispersion of the ferrite spinel phase
(dark contrast) into the PZTN ferroelectric matrix (light con-
trast). Figure 1 shows that a good phase intermixing, with
0–3 connectivity resulted in all the compositions, with well-
defined clean interfaces between the two phases and a good
densification with (90–95)% relative density. Both at small
(Fig. 1(a)) and large (Fig. 1(c)) ferrite concentrations, both
fine (grain size about 1–2 lm) and large faceted ferrite grains
(average sizes of 2–4 lm) are present, while PZTN has finer
ceramic grains of 0.5–1 lm and forms a quasi-continuous
matrix at small ferrite concentrations.
094103-3 Ciomaga et al.
B. Dielectric properties
The real and imaginary part of permittivity vs. frequency
obtained at room temperature for the xNF-(1  x)PZTN
ceramic composites with x ¼ 2, 5, 10, 20, 30, 40, 50, 60,
70 wt. % are shown in Figures 2(a) and 2(b). The real part of
permittivity remains almost constant in the frequency range of
106 Hz  108 Hz, followed by an increase towards higher fre-
quencies above 5  108 Hz. Above this frequency, microwave
resonances characterized by a jump from positive to negative
values of the real part of permittivity (e0 ) accompanied by max-
ima of the imaginary part of permittivity, as shown in the inset
windows of the Figs. 2(a) and 2(b). These resonances shift to
higher frequencies when the real permittivity decreases with
the NF addition, due to the fact that the resonance frequencies
scale with the inverse of the real part of permittivity values.
These phenomena are extrinsic in nature and not related to a
functional property characteristic to the composite materials
and were explained within the dielectric resonant cavity and
perturbed dielectric resonant cavity models.25,26 For the analy-
sis related to the role of composition and microstructures on
the dielectric properties of the xNF-(1  x)PZTN composites,
the stationary permittivity values around the frequency of
107 Hz were considered as being intrinsic to the material.
These permittivity values scales with the addition of low-
permittivity ferrite phase, according to a “dilution effect”
FIG. 2. Frequency dependence of the (a) real part and (b) imaginary part of
permittivity of xNF-(1  x)PZTN ceramic composites with different addi-
tions of ferrite phase x.
J. Appl. Phys. 112, 094103 (2012)
(or “sum property”) and reduces from e0 r  1047 for
x ¼ 2 wt. % e0 r  47 for x ¼ 70 wt. % at the frequency of 107
Hz. The dielectric properties of the composites are not only
determined by the composition x but also by their microstruc-
tural characteristics. In order to describe such effects and to
compare with experimental data, various modeling approaches
have been proposed in the literature.
III. THEORETICAL BACKGROUND
A. Effective medium approximation models
The prediction of the effective electrical properties of
composites is still one of the challenging problems in material
science. The EMA considers that each inclusion grain is sur-
rounded by a continuous mixture which has the assumed ho-
mogeneous media properties. There were proposed many
approximations and empirical formulae which are insensitive
to the detailed microstructural characteristics as the connect-
edness and clustering of one phase in a binary-phase random
composite.27–29 The most used approximations were
Maxwell-Garnet, Bruggeman, and Lichtenecker equations22,23
which will be also employed in the present discussions.
MG formula was proposed for composites with a small
volume fraction f of inclusion grains randomly distributed
into a continuous host matrix and is suitable to describe elec-
trical properties in composites below the percolation
limit.15,16 It assumes that the inclusions are small spheres
not-connected each other (0-3 phase connectivity), randomly
distributed inside the host matrix. The dimensions of the em-
bedded spheres are considered much smaller that the dis-
tance between them. The complex effective permittivity of
such system is
~e 2  ~e 1
~e eff ¼ ~e 1 þ 3 f~e 1 ; (1)
~e 2 þ 2~e 1  f ð~e 2  ~e 1 Þ
where ~e eff ; ~e 1 and ~e 2 are the complex effective permittivity
of the composite medium, of the embedded matrix and the
inclusion phases (guest) and f is the inclusions volume filling
factor.
The BG approximation evaluates the dielectric proper-
ties of randomly inhomogeneous materials and treats both
phases on a completely symmetrical basis.17–19 Both parent
phases should have similar morphologies and are randomly
distributed through the whole system. The dielectric proper-
ties of the composite respect the self-consistency condition,
according to which the net polarization induced in material
is zero in the long-wavelength limit. The complex effective
permittivity is a solution of the symmetric equation with
respect of the embedded matrix and guest phase (3-3
connectivity)
~e 1  ~e eff ~e 2  ~e eff
ð1  f Þ þf ¼ 0: (2)
~e 1 þ 2~e eff ~e 2 þ 2~e eff
The LI’s formula was derived by employing differential
analysis onto the Maxwell’s equations and the principle of
local charge conservation. This formula approximates the per-
mittivity of a mixture formed by randomly spatial distribution
094103-4 Ciomaga et al.
of shapes and orientations of the inclusion phase into an effec-
tive matrix20–22,30
log ~e eff ¼ f1 log ~e 1 þ f2 log ~e 2 : (3)
The Lichtenecker’s equation was commonly proposed
to characterize composite systems that have complex local
microstructural characteristics that cannot be reduced to a
simple previously described microstructure.31
B. Finite element model approach
Using finite element model, randomly different types of
microstructures similar to ones observed by SEM in our com-
posites and with various compositions (filling factors 0 < f < 1)
have been numerically generated. For example, the numeri-
cally generated microstructure represented in Figure 3(a)
shows a good dispersion of the ferrite grains with different
dimensions and shapes (dark regions), placed inside the ferro-
electric PZTN matrix, similar to a 0-3 connectivity as observed
by the SEM analysis for low filling factor. Similar type of
phase connectivity will also result at high filling factor close to
1 (ferroelectric PZTN embedded into the ferrite NF matrix).
For intermediate filling factors, more complex types of micro-
structures were generated, as represented in Figures 3(c) and
3(e), as also resulted in the SEM analysis (Figs. 1(b) and 1(c)).
For all the compositions, the simulated microstructures modify
with filling factor, but the space homogeneity in the samples is
maintained. The complex permittivity of the ferroelectric and
ferrite phases were considered as being e1 ¼ 1129  i  49 and
e2 ¼ 23  i  0:26, respectively.
Taking into account the microstructures, the local
field was computed by solving the Poisson’s equation:
r  ðeðrÞrVðrÞÞ ¼ 0 with boundary conditions as shown in
Figs. 3(a), 3(c), and 3(e).32–34 eðrÞ ¼ e0 ðrÞ  ie00 ðrÞ is the local
complex permittivity and VðrÞ is the amplitude of the local
harmonically oscillating potential: Vðr; tÞ ¼ VðrÞ  ei2pvt ,
where v is the frequency of the applied voltage. The system
was meshed in discrete triangle elements according to the
FEM procedure and the local field was computed for each ele-
ment, as shown in the Figs. 3(b), 3(d), and 3(f) for the virtual
microstructures of Figs. 3(a), 3(c), and 3(e). The real part of
the effective permittivity was then derived by summation the
total electrostatic energy of the all Ne discrete elements35,36
 
1 0 DV 2 1X Ne
eeff At ¼ ee 0 E e 2 A e ; (4)
2 d 2 e¼1
where DV is the applied voltage, d is distance between elec-
trodes, At is the total area of the system; ee 0 is the real part of
permittivity, Ee is the local electric field, and Ae is the area
of the eth element.
In a similar way, the dielectric losses can be evaluated by
summing the local losses of the all elements and expressed as
a function of an effective imaginary part of the permittivity36
 2
1 DV 1X Ne
xeeff 00 At ¼ xee 00 Ee 2 Ae ; (5)
2 d 2 e¼1
J. Appl. Phys. 112, 094103 (2012)
where ee 00 is the imaginary part of the local permittivity of
the eth element.
The simulations show that local field became inhomo-
geneous in the composite structures, as a consequence of
the interfaces between phases with contrasting permittiv-
ities. Consequently, higher fields will concentrate in low-
permittivity regions (Figs. 3(b), 3(d), and 3(f)). Since the
electric field energy per volume element is proportional to
the local square field, the low-permittivity phase will con-
tribute to a higher extent to the composite effective permit-
tivity and a faster nonlinear decrease of the composite
permittivity with increasing NF filling factor is expected
from calculations.
In this way, a realistic effective permittivity of the compo-
sites ceramics with various concentrations of the ferrite phase
can be computed and compared with the experimental values
of permittivity in the xNF-(1  x)PZTN ceramic composites.
IV. COMPARISON OF THE EXPERIMENTAL DATA
WITH RESULTS OF EMA AND FEM MODEL
The experimental complex permittivity values of xNF-
(1  x)PZTN ceramic composites with x ¼ 2, 5, 10, 20, 30,
40, 50, 60, 70 wt. % (corresponding to the volume filling fac-
tors of f ¼ 2.9%, 7.3%, 14.3%, 28%, 39%, 50%, 60%, 70%,
and 79%) at v ¼ 108 Hz and the EMA and FEM model results
are comparatively shown in Figs. 4(a) and 4(b). Dielectric
data at 100 MHz were considered in the comparison because
the measured complex permittivity data show stationary
intrinsic values at this frequency.
The comparison shown in Figures 4(a) and 4(b) demon-
strates that not all the model results describe the experimen-
tal permittivity data. The most elaborated method, the FEM
approach resulted in an excellent agreement with the experi-
mental data in overall composition range (filling factor
0 < f < 1). This is due to the fact that FEM calculations were
performed in systems that simulated realistic virtual micro-
structures, which are similar with the experimentally
observed one and considers the computed local field distribu-
tions in evaluating the effective field permittivity without
using any additional approximation or property averaging.
The FEM also gives the possibility to predict local phenom-
ena generated in a real composite ceramic by the high/low
field values, e.g., possible breakdown, interface phenomena
related to the presence of uncompensated charges, etc.
Among the EMA equations, the comparison from
Figures 4(a) and 4(b) shows that the MG and BG approxima-
tions are close to the experimental data only for small (NF
inclusions inside PZTN matrix) or high volume filling factor
f (PZTN islands inside the NF matrix) and does not describe
at all the intermediate filling factor values: while MG under-
estimate, the BG formula highly overestimate the experimen-
tal permittivity values of the xNF-(1  x)PZTN composite in
intermediate filling factor range (Fig. 4). The reasons for this
discrepancy are related to the simplified hypothesis of spher-
ical fillers and of the 0-3 type of phase connectivity. In real-
ity, the ceramic grains (particularly, the ferrite ones) are
irregular in shape and size and they satisfy the condition to
have much smaller dimension than the distances among
094103-5 Ciomaga et al. J. Appl. Phys. 112, 094103 (2012)

FIG. 3. Generated composite ceramic microstructures with different volume filling factors of Ni ferrite phase: (a) f ¼ 10 vol. %, (c) f ¼ 30 vol. %, and (e) f ¼ 70
vol. %, in PZTN matrix (NF-dark color; PZTN-light color); and (b), (d), and (f)—the corresponding local field maps. The intensity of the local electric field is rep-
resented with colors, and the field direction is perpendicular on the isopotential lines (black lines), DV=25 is the difference between two successive lines. Note
that the isopotential lines are agglomerated in high field regions.

them, imposed by the MG approximation for small or high
filling factor, only. The BG approximation is in very good
correlation with the experimental data for higher concentra-
tion of the magnetic phase (x ¼ 60, 70, 100 wt. % corre-
sponding to f ¼ 70%, 77%, and 100%). For smaller filling
factor of the ferrite phase in composites (x < 60%, f < 70%),
the BG approximation cannot explain the experimental data
because the composite mixing is not perfect and the two
phases have not a symmetrical contribution (Fig. 1(b)).
Among the EMA models, the Lichtenecker’s approximation
gave the best prediction for the effective permittivity of com-
posite in overall compositional range. This result can be
094103-6 Ciomaga et al. J. Appl. Phys. 112, 094103 (2012)

range is given by the results of finite element model calcula-

tions which used realistic microstructures and among the
effective field approximations, by the Lichtenecker’s formula.
On limited ranges of small or high filling factor, the Brugge-
mann and Maxwell-Garnet equations also can satisfactory
describe the experimental data of the xNF-(1  x)PZTN com-
posite ceramics. The present study emphasis the role of the
microstructure in determining the effective material dielectric
properties in composites and the appropriateness of using
models which consider realistic microstructures (in terms of
phase interconnectivity, phase distributions, size, and shapes
of the parent phases in the mixture) for predicting the func-
tional properties of the composite.

ACKNOWLEDGMENTS
This work was financial supported by the Romanian
CNCSIS-UEFISCSU project number PN II-RU TE code
187/2010. One of the authors (C. S. Olariu) acknowledges
the financial supported by POSDRU/89/1.5/S/63663 grant.

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