Physica B 426 (2013) 137–143

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Physica B
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Magnetic behavior and dielectric properties of aluminum substituted

M-type barium hexaferrite
S.M. El-Sayed a,n, T.M. Meaz b,1, M.A. Amer b,2, H.A. El Shersaby a,3
a
National Center for Radiation Research and Technology, Nasr City, Cairo, Egypt
b
Physics Department, Faculty of Science, Tanta University, Tanta, Egypt

art ic l e i nf o a b s t r a c t

Article history: Various parameters in the structural features of the aluminum substituted barium hexagonal ferrite
Received 11 April 2013 particles BaAlxFe12−xO19 with 0≤x≤3.5 which were prepared by the solid state reaction method have been
Received in revised form studied. The infrared transmission spectrum was measured in the wave number region 5000–200 cm−1
31 May 2013
at room temperature. The results were interpreted in terms of the vibrations of the isolated molecular
Accepted 14 June 2013
units in such a way to preserve the tetrahedral and octahedral clusters of metal oxides in the barium
Available online 21 June 2013
aluminum hexagonal ferrites. The infrared features are assigned to Fe–O and Ba–O bonds in M-type
Keywords: hexagonal ferrite (BaFe12O19) molecules. Also, the results explain the structural model, based on the
Infrared spectrum effect of aluminum substitution “Al–O bond”. On the other hand, the magnetic behavior of the samples
Magnetic behavior
was studied using the vibrating sample magnetometer technique. The saturation magnetization (Ms) and
X-ray diffraction
magneton number (nB) decrease with increasing Al3+ substitution from 61.2 to 28.9 emu/g and from 12.2
Dielectric parameters
Ac conductivity to 5.3 mB respectively. Also, all samples were characterized using X-ray diffraction and the values of grain
size, microstrain and dislocation density of all samples were calculated. The dielectric parameters and ac
conductivity measurements were performed within a temperature range 293–493 K. The ac conductivity
showed a linear relation with the frequency power law with an exponent s≈0.69–0.14 for BaFe12O19.
It decreases with increasing temperature, indicating that the heterogeneous structures increase. While
the dielectric constant (ε′) and the dielectric loss (ε″) decrease with increasing Al substitution.
& 2013 Elsevier B.V. All rights reserved.

1. Introduction of metal oxides in ferrites, respectively. FTIR spectra showed the

Recently, ceramic materials were characterized by their high
resistivity and high permeability, allowing them and their derived
products to be used in numerous industrial applications including
technology electronic devices, communication equipments, high
density magnetic recording media, materials for permanent mag-
nets and microwave devices. M-type hexagonal ferrite are very
promising materials because of their potential applications in
infrared (IR) optics. As a result, new technologies and techniques
for the miniaturization of components have been developed,
including thin- and thick-film techniques. Such techniques, e.g.,
pulsed-laser deposition, sputtering, and spin coating require
individual and complex setups based on the product [1]. FTIR
frequency bands in the range 560–580 cm−1 and 430–470 cm−1
correspond to the formation of tetrahedral and octahedral clusters
n
Corresponding author. Tel.: +20 2 2287592; fax: +20 2 22876031.
E-mail addresses: smelsayed@hotmail.com,
sobhia11@yahoo.com (S.M. El-Sayed).
1
Tel.: +20 1227870465; fax: +20 222876031.
2
Tel.: +20 1002500461; fax: +20 222876031.
3
Tel.: +20 403040992; fax: +20 222876031.
formation of the corresponding M–O stretching bands in ferrites.
The authors suggested that the vibrational mode of tetrahedral
clusters is higher as compared to that of the octahedral clusters,
which may be caused by the shorter bond length of tetrahedral
clusters. The frequency bands in the range 3030–2860 cm−1 and
1470–1374 cm−1 are attributed to the interference of stretching
and bending vibrations of nujol peaks [2]. Fine particles of barium
hexaferrite (BaFe12O19) powder have been synthesized by the sol–
gel based combustion technique. Generally, the metal oxide
vibrations occur below 1000 cm−1. The presence of Ba–O stretch-
ing caused the appearance of a peak at 895 cm−1. In addition the
broad absorption around 585 cm−1 is caused by Fe–O (Fe–O4)
stretching. The peak at 440 cm−1 corresponds to bending of Fe–O
(Fe–O4) and stretching of Fe–O (Fe–O6) [3]. Infrared (IR) spectro-
scopy is largely complementary to X-ray diffraction measure-
ments. It points directly to the general nature of unknown
substances, where it is able to detect and characterize non-
crystalline compounds. Such information being obtainable from
the presence or absence of characteristic absorption bands [4]. The
saturation magnetization (Ms) increased with temperature and
time. The longer the reaction time, the less the oxygen vacancies in
the crystal, and thus the enhanced Fe–O–Fe superexchange

0921-4526/$ - see front matter & 2013 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.physb.2013.06.026
138 S.M. El-Sayed et al. / Physica B 426 (2013) 137–143

coupling which increases Ms. Also Hc is mainly affected by the
grain size and shape. The saturation magnetization decreases with
Al3+ ion doping in MFe12O19 (M ¼Sr, Ba and Pb) hexaferrites due to
the diamagnetic nature of Al3+ ion [5]. With the adoption of non-
ferromagnetic Al3+, Hc values were increased. Also saturation
magnetization Ms and coercivity Hc of BaAlxFe12−xO19 powders
increase with the increase of calcinations temperature which
should be explained by the enhancement in crystallinity of
BaAlxFe12−xO19 powders. Compared with BaAl1Fe11O19 and BaAl2-
Fe10O19 powders, the increase of Al contents clearly shows that Ms
decreases but Hc increases [6]. This may be due to the lack of full
saturation reached at the maximum applied field (9.6 kOe) and
small particles size. The saturation magnetization and coercivity
for BaAl1Fe11O19 after annealing at 1000 1C is 45.8 emu/g and
2940 Oe, respectively [7]. However, the coercivity decreases with
increasing temperature of annealing above 950 1C. This effect is
related to increasing the crystallite size at higher temperatures.
The optimum coercive force (Hc) for a mixture of powders
annealed at 950 1C for 10, 20 and 30 h is 349 kA/m, 366 kA/m
and 364 kA/m, respectively [8]. For BaMg2Fe10O19 the dielectric
loss arises, when the polarization lags behind the applied altering
field indicating the structural inhomogeneity of such a materials.
The dielectric loss decreases substantially with increasing fre-
quency and reaches a constant value later on [9].
The aim of this paper is to show the absorption bands of the
samples that were measured by using a FTIR-spectrometer and
study the dielectric properties of M-type BaAlxFe12−xO19 hexagonal
ferrite system. Therefore, in the present work, the magnetization
measurements were carried out for all the samples at room
temperature up to a maximum field of 20 kG. Also, the dielectric
properties of the M-type barium aluminum hexagonal ferrite
have been investigated as a function of both temperature and
BaAl3.5Fe8.5O19
frequency. The measurements were analyzed within dielectric
parameters (ε′ and ε″). Finally, sac over a limited range of frequency
was measured.
2. Experimental techniques
The samples were prepared by the solid state reaction method.
BaCO3, Al2O3 and Fe2O3 were mixed well in the correct ratios and
calcined at 1440 K for four hours to form the M-type hexagonal
ferrite system BaAlxFe12−xO19 with x ¼0, 0.5, 1.5, 2.5 and 3.5. The
FIR transmission spectra of different samples were recorded on a
Fourier transform IR (TENSOR-27-BRUKER) spectrophotometer in
conjunction with the KBr disc technique, over the spectral range of
5000–200 cm−1 at room temperature. Powdered samples were
thoroughly mixed and grounded with KBr; after which the
mixtures were pressed at 10 T. Magnetic measurements were
made on a vibrating sample magnetometer (VSM), Model (VSM
LDJ Electronics Inc. Troy, MI). The room temperature magnetic
properties, namely coercivity (Hc) and saturation magnetization
(Ms) were measured in a vibrating sample magnetometer with an
applied field up to a maximum field of 20 kA/m. Also, the X-ray
diffraction (XRD) technique has been used to investigate the
structure of the prepared samples using the Shimadzu XD-D1
diffractometer with Cu radiation. For electrical measurements, the
powder samples were pelletized into disc shaped pellets. Dielec-
tric measurements were performed using the complex impedance
measuring technique (lock-in amplifier, Stanford SR 510 type USA);
consequently the current passing through the sample could be
determined. To ensure the proper connection to the sample, the
indigenously designed sample holder with silver electrode has
been used. In this arrangement the samples are sandwiched
between two circular electrodes of silver. The dielectric constant
(ε′), loss tangent (tan δ), and ac conductivity (sac) behavior were
studied as a function of frequency at different temperatures.

3. Results and discussion

BaAl2.5Fe9.5O19
3.1. FTIR analysis
Transmittance (%)

BaAl1.5Fe10.5O19
Fig. 1 shows FT-IR spectra of AlxBaFe12−xO19 (x ¼0.0, 0.5, 1.5,
2.5 and 3.5) with different Al3+ ion contents. The characteristic
vibration frequencies υ1–υ4 for these samples are represented in
BaAl0.5Fe11.5O19 Table 1. From Fig. 1 and Table 1, all the characteristic peaks can be
assigned to the M-type barium ferrite. With the increase of Al3+
ion content, the values of υ1–υ4 shift to a higher wave number and
BaFe12O19 this can be related to two major facts. The first is that Al3+ ions is
of a lighter atomic weight than Fe3+ ions while the second is that
the wave number is inversely proportional to the atomic weight.
Ferrites bands usually occur due to tetrahedral and octahedral
1000 2000 3000 4000 5000 complexes. IR bands of ferrites are usually assigned to the vibra-
Wave number (Cm-1) tion of ions present in the crystal lattices, caused by the tetra-
Fig. 1. FTIR absorption spectra of M-type barium aluminum hexagonal ferrites
hedral and octahedral Fe3+–O2− distances. It is known that ferrites
which have the formula BaAlxFe12−xO19 with different substitutions, x¼ 0.0, 0.5,1.5, has four bands, ν1 band assigned to the tetrahedral complexes
2.5 and 3.5. with high wave number, the band ν2 is assigned to the octahedral

Table 1
FTIR characteristic frequencies for all samples of BaAlxFe12−xO19.

Samples υ1 (cm−1) I (%) υ2 (cm−1) I (%) υ3 (cm−1) I (%) υ4 (cm−1) I (%)

BaFe12O19 594.06 0.315 447.474 0.467 892.054 0.890 339.463 0.644

BaAl0.5Fe11.5O19 592.131 0.290 443.616 0.416 891.09 0.815 339.463 0.586
BaAl1.5Fe10.5O19 595.989 0.047 449.403 0.126 893.09 0.877 341.392 0.279
BaAl2.5Fe9.5O19 597.918 0.198 453.26 0.339 894.947 0.959 341.392 0.500
BaAl3.5Fe8.5O19 603.704 0.313 457.118 0.478 900.704 0.984 347.178 0.614
 S.M. El-Sayed et al. / Physica B 426 (2013) 137–143
complexes with lower wave number, weaker ν3 band assigned to
divalent octahedral metal ion–oxygen ion complexes and finally ν4
depends on the mass of the divalent tetrahedral cation which is
assigned to some types of vibrations involving a displacement of
the tetrahedral cation [10]. Very weak satellite peaks at 432 and
402 cm−1, these peaks are assigned to the vibrations of metal ion–
oxygen complexes in the tetrahedral (ν1) and octahedral (ν2) sites,
respectively such as Fe–O vibrations for BaFe12O19. As in case of
barium hexa-aluminates the majority of infrared active modes of
vibrations for Ba and Fe in BaFe12O19 appear below 400 cm−1. The
wave number bands in the range 594–603 cm−1 represent Al–O
bending vibrations in the tetrahedral sheet and 447–457 cm−1
show the presence of Fe–O stretching vibrations that corresponds
to the formation of tetrahedral and octahedral clusters, confirming
the presence of M–O stretching band in ferrites. Also, the bands
existing in the 891–900 cm−1 range (centered at 893 cm−1) repre-
sent Ba–O stretching. As for the FT-IR spectra, a broad absorption
peak centered at 3423 cm−1, corresponding to characteristic O–H
stretching band, can be seen for all the as-burnt samples. Assum-
ably, this is due to water molecules adsorbed to the very finely
dispersed as-burnt samples. The vibrational mode of tetrahedral
clusters is higher as compared to that of octahedral clusters, which
is due to the shorter bond length of tetrahedral clusters [11].
3.2. Saturation magnetization
The magnetic properties of aluminum substituted barium
hexaferrite were quantified with the help of the vibrating sample
magnetometer (VSM) technique at room temperature. The coer-
cive field (Hc), saturation magnetization (Ms) and remanent
magnetization (Mr) values were obtained from the hysteresis loops
registered with a maximum field of 20 kOe. The measured hyster-
esis loops for some of the BaAlxFe12−xO19 (x¼ 0.0, 0.5, 1.5, 2.5, and
3.5) samples as a function of applied magnetic field are shown in
Fig. 2. Doping of barium ferrite with aluminum leads to the
decrease in both remnant and saturation magnetization. The
decrease in magnetization is related to the magnetic moment of
the constituent ions. The behavior of these properties can be
60
Magnetization (emu/g)
50
40
30
20
10
0
-20000 -10000
Applied magntic field (Oe) -10
-20
-30
-40
-50
-60
Fig. 2. Hysteresis loops for some of the BaAlxFe12−xO19 samples as a function of applied magnetic field.
139
explained on the basis of hexagonal structure of the ferrite being
occupied by doped cations. The nonmagnetic Al3+ replaces Fe3+
ion which is responsible for the reduction in saturation magneti-
zation and thus the remanence of the synthesized materials. The
saturation magnetization of BaM is 61.2 emu/g and decreases with
increasing Al concentration as expected, due to the weakening of
the super exchange interaction of Fe3+–O–Fe3+.
On the other hand, the coercivity increases with increasing Al
concentration. This increase in coercivity is attributed to the
increase in anisotropy field Ha, since the coercivity is proportional
to the magnetic anisotropy field. The measured values of Hc, Ms
and Mr are given in Table 2. From our results it is confirmed that
the magnetic properties of barium hexaferrite are very much
affected by the substitution of Al3+ in the barium hexaferrite
matrix. Squareness is the ratio between remanent (Mr) and
saturation magnetization (Ms) and such results match with other
references [12].The magneton number nB is obtained using the
relation [13,14]
molecular weight  M s
nB ¼ ð1Þ
5585
The values of magneton number decrease with increasing the
Al3+ substitution x. This is caused by the substitution of Fe3+ ions
in the barium hexaferrite matrix with non-magnetic Al3+ ions. The
values of magneton numbers are shown in Table 3.
3.3. X-ray diffraction (XRD)
The X-ray diffraction pattern provides information about the
nature and structure of the material. A pattern showing sharp
peaks with various intensities is indicators of polycrystalline
nature of the material. The X-ray diffraction of the prepared
BaAlxFe12−xO19 samples desks (x¼ 0, 0.5,1.5, 2.5, and 3.5) are shown
in Fig. 3. Such a figure reveals the crystalline nature of the
BaAlxFe12−xO19 samples. By increasing the Al content in the
samples, the possibility of strain (stress) developed increases and
that affects the mechanical properties of such samples including
the microstructure properties stability. This is clearly shown in
Table 3. The crystallite size and the residual strain were calculated
BaFe 12O 19
BaAl0.5Fe11.5O19
O19
BaAl 1.5Fe 10.5
O
BaAl2.5Fe9.5 19
O
BaAl3.5Fe8.5 19
0 10000 20000
140 S.M. El-Sayed et al. / Physica B 426 (2013) 137–143

Table 2 The variation of the ionic radii caused by the substation is the
Saturation magnetization (Ms), remanent magnetization (Mr), coercivity (Hc) and reason behind the lattice straining. The values of dislocation
magneton number (nB) of BaAlxFe12−xO19 samples.
density and residual strain of pressed samples increase with
Samples Ms (emu/g) Mr (emu/g) Hc (KA/m) Squareness n
B increasing Al substitution ions as shown in Table 3. Such an
increase is observed as a result of chemical structure undergoing
BaFe12O19 61.204 31.534 1655.8 0.51523 12.18 strain that raises structure's internal energy.
BaAl0.5Fe11.5O19 57.587 29.874 1645.2 0.51877 11.311
BaAl1.5Fe10.5O19 49.739 25.8 1765.8 0.5187 9.641
BaAl2.5Fe9.5O19 42.213 22.388 2192.8 0.53036 7.964
BaAl3.5Fe8.5O19 28.933 16.102 2119.8 0.55654 5.309 4. Frequency dependence of dielectric constant

4.1. Permittivity formalism

Table 3
Crystallite size, dislocation density and residual strain of the prepared samples The variation of the dielectric constant and dielectric loss ε′ and
in disc shape. ε″ as a function of frequency at different temperatures were
estimated. If a capacitor consists of two parallel plates of area
Samples D (m) E−8 δ E+14 ε E−4
A (cm2) separated by a distance d (cm) in empty space its
BaFe12O19 4.658 4.609 11.985 capacitance is given by
BaAl0.5Fe11.5O19 3.586 7.775 15.541
A
BaAl1.5Fe10.5O19 2.339 18.27 23.727 C0 ¼ PF ð4Þ
BaAl2.5Fe9.5O19 1.603 38.92 34.508 11:3d
BaAl3.5Fe8.5O19 1.334 56.16 41.339
The real dielectric constant ε′, and loss factor tan δ have been
determined as functions of frequency f at different temperatures
for all the studied samples using the following expressions [15]:
 
C 11:3dV R sin ðfÞ
BaAl3.5Fe8.5O19 ε′ ¼ ¼  1012 ð5Þ
C0 2πf RA

1
tan δ ¼ ð6Þ
tan f
BaAl2.5Fe9.5O19
The dielectric loss, ε″, which represents the phase lag of the
------------ Intensity (a.u.)

dipole oscillations with respect to the applied electric field,

depends on the number and nature of ions present [16]. The
BaAl1.5Fe10.5O19
dielectric loss, ε″, can be calculated from the following expression:
ε″ ¼ ε′ tan δ ð7Þ

BaAl0.5Fe11.5O19
35
BaFe12O19
BaAl0.5Fe11.5O19
BaFe12O19 30 BaAl1.5Fe10.5O19
BaAl2.5Fe9.5O19
25 BaAl3.5Fe8.5O19

20 30 40 50 60 70 80 90
20
Dielectric constant ε` (ω)

2q (degree)
Fig. 3. X-Ray diffraction patterns for desk samples.
15
3.5 4.0 4.5 5.0 5.5 6.0
from full width at half maximum (β) FWHM using the relations (2) 140
and (3) for hexagonal phases
0:94λ 120
D¼ ð2Þ
β cos θ
100 T = 313 K
The strain (ε) was calculated from relation T = 353 K
80 T = 393 K
λ
β¼ −ε tan θ ð3Þ T = 433 K
D cos θ T = 473 K
60
The dislocation density (δ), defined as the length of dislocation
lines per unit volume of the crystal, was evaluated from the 40
equation δ ¼ 1=D2 .
The crystallite size seems to be affected by size of the 20
substitution ions; it decreases with increasing the Al substitution.
This decrease can be associated to the replacement of parent 3.5 4.0 4.5 5.0 5.5 6.0
atoms with substitution atoms in the lattice site. Since the ionic Log ω (Hz)
size of aluminum is small as compared to the other iron ions so Fig. 4. The behavior of ε′ as function of frequency (a) all samples at room
the unit cell dimension of Al substituted compound is the lowest. temperature and (b) BaFe12O19 at different temperatures.
 S.M. El-Sayed et al. / Physica B 426 (2013) 137–143 141

10 50
BaFe12O19
8 BaAl0.5Fe11.5O19
BaAl1.5Fe10.5O19 BaFe12O19
BaAl2.5Fe9.5O19 40 BaAl0.5Fe11.5O19
6
BaAl3.5Fe8.5O19 BaAl1.5Fe10.5O19
4 BaAl2.5Fe9.5O19
30 BaAl3.5Fe8.5O19
Dielectric Loss ε`` (ω)

Dielectric constant ε` (ω)

0
3.5 4.0 4.5 5.0 5.5 6.0 20
1000
300 350 400 450 500
800 T = 313 K
T = 353 K 120
600 T = 393 K
T = 433 K BaFe12O19
T = 473 K 100
BaAl0.5Fe11.5O19
400
BaAl1.5Fe10.5O19
80 BaAl2.5Fe9.5O19
200
BaAl3.5Fe8.5O19
60
0
3.5 4.0 4.5 5.0 5.5 6.0
Log ω (Hz) 40
Fig. 5. The behavior of ε″ as function of frequency (a) all samples at room
temperature and (b) show the behavior of ε″ at different temperatures for
BaFe12O19 sample.
20
300 350 400 450 500
Temperture (K)
Fig. 4(a) shows that, at room temperature the values of ε′
decrease with an increase in Al contents, as a result of the Fig. 6. Behavior of dielectric constant as function of temperature for all BaAlx
Fe12−xO19 samples with different substitutions (a) at high frequency and
reduction of Fe2+ ions at the octahedral sites. The behavior of ε′
"1,00,000 KHz"(b) at low frequency "800 Hz".
and tan δ towards composition changes can be explained in the
essence of an assumption that the mechanism of the dielectric
polarization is similar to the electrical conduction. It can be seen 50
from Fig. 5(a) shows that the values of the dielectric loss are high
at low frequency and decrease with increasing the frequency in all 40
samples. Fig. 4(b) shows that the dielectric constant for BaFe12O19
BaFe12O19
prepared sample increases with increasing temperature at low 30 BaAl0.5Fe11.5O19
frequency, whereas at high frequency the increase of dielectric BaAl1.5Fe10.5O19
constant with increasing temperature is less observable. The same 20 BaAl2.5Fe9.5O19
behavior was also observed for the other samples. Also, Fig. 5 BaAl3.5Fe8.5O19
(b) shows the behavior of ε″ as a function of frequency at different
Dielectric loss ε`` (ω)

10
temperatures for BaFe12O19 prepared sample. For all samples the
values of ε″ decrease with an increase in Al contents. The dielectric
loss causes energy loss within the material during conduction of 0
300 350 400 450 500
electrons. Hopping of electrons produces polarization that changes
with changes in the applied field. 1200
The dielectric loss appears clearly when polarization lags
behind the applied ac electric field is justified by the materials 1000
structural imperfections, defects and the presence of material
impurities. With the rise in temperature the electrons and ions 800 BaFe12O19
get thermally activated which increases the conduction and hence BaAl0.5Fe11.5O19
there is an increase in value of tan δ. As the temperature increases, 600 BaAl1.5Fe10.5O19
the degree of dipole orientation increases and therefore energy BaAl2.5Fe9.5O19
required to overcome the barrier of the medium is reduced. 400 BaAl3.5Fe8.5O19
Finally, the values of both ε′ and ε″ are decreased with
increasing aluminum at the frequency range of interests. Those 200
behaviors obscured for ε′ with temperature changes at low
frequency resulted from the semiconducting nature properties of 0
the materials. Whereas at high frequency such property are 300 350 400 450 500
obscured by the disability of the charges at boundaries to follow Temperture (K)
the variation of the field as shown in Figs. 6 and 7. The decrease in Fig. 7. The behavior of dielectric loss as function of temperature for all prepared
both quantities with frequency changes may be ascribed to the samples have the formula BaAlxFe12−xO19 with different substitutions (a) at high
role played by the additional energy given to the structure on frequency 1,00,000 KHz and (b) at low frequency "800 KHz".
142 S.M. El-Sayed et al. / Physica B 426 (2013) 137–143

increasing the frequency. This energy, along with the Al, allows the
ε′ and ε″ to pass through a maximum value at the lower value of
frequency. It was observed that ε′ had high values (∼102–103) at
lower frequency and it decreases beyond 100 kHz.
4.2. Frequency dependence of conductivity
Conductivity sac has been determined as functions of frequency
f at different temperatures for all the studied samples using the
following expression [15]:
 
VRd
s`ac ¼ cos ðfÞ ð8Þ
RA
where d (cm) is the thickness of the sample, and A (cm2) is the
horizontal cross sectional area of the disc-shaped sample. The
frequency, phase angle and the voltage drop developed across a
standard resistance connected in series with the sample were
measured simultaneously, and the ac conductivity (sac) was
calculated at varies temperatures. Generally, the total measured
conductivity at a given frequency (ω) is then separated into dc and
ac components, according to Almond–West type power law [17]
s′total ¼ sdc ðTÞ þ sac ðω; TÞ ð9Þ
The first term dc conductivity is temperature dependent and
frequency independent. This is due to the band conduction and is
related to the drift mobility of the free charge carriers. The second
term sac is pure ac conductivity, caused by the hopping processes
at the octahedral site and is a frequency dependent function. The
first term is predominant in low frequencies and at high tempera-
tures, while the second term is predominant in high frequencies
and at low temperatures. The frequency dependence of the second
term sac can be written as [18]
sac ðω; TÞ ¼ BðT ÞωS ðTÞ ð10Þ
where B is a constant having the units of conductivity and ω is the
angular frequency (ω¼2πf). The power law component S is a
constant which depends on both the composition and the tem-
perature and its value lies between 0 and 1 as shown in Table 3.
Moreover, the temperature dependence of S in HOB model should
follow this expression [19]:

6K B T
1−S ¼ ð11Þ
6e-8 Wm

BaFe12O19 where Wm is polaron binding energy, KB is Boltzman constant, T is

4e-8 BaAl0.5Fe11.5O19 absolute temperature and S is exponent factor of frequency
BaAl1.5Fe10.5O19 estimated from the slopes ln(sac) and ln(ω) curves. Fig. 8(a) and
BaAl2.5Fe9.5O19 (b) illustrates the behavior of the real part of the complex ac
BaAl3.5Fe8.5O19 conductivity s′ac with frequency at room temperature for all
2e-8
samples and the behavior of s′ at different temperatures for
Conductivity σac (Ω--1m-1)

BaFe12O19 in the range from 313 K to 473 K. The conduction

mechanism in ferrites is explained by the hopping of charge
0
8 9 10 11 12 13 carriers between the Fe ions at octahedral sites. The increase in
conductivity does not mean the increase in charge concentration
5e-7
but indicates the increase in the mobility of charge carriers. The
T = 313 K values of conductivity increase with increasing temperature, also
4e-7 T = 353 K decreases with increasing the Al content as a function of fre-
T = 393 K quency. According to Maxwell–Wagner model our results of ac
T = 433 K
T = 473 K conductivity at low frequencies describe the grain boundary
3e-7
behavior while the dispersion at high frequency may be attributed
to the conductivity of grains tending to be effective good con-
2e-7 ductors and also there is an increase in hopping of electrons
between Fe3+ and Fe2+ ions which increases conductivity. The
1e-7
logarithmic representation of the previous power law was plotted
in Fig. 8(a) and (b).
Both Wm and S quantities for Al metal-containing hexaferrite
0 material are of the same order of magnitude as those for the
8 9 10 11 12 13 (BaFe12O19) as shown in Table 4. This result predicts that the
Ln ω (kHz) conduction mechanisms increases as a function of Al metal
Fig. 8. Behavior of conductivity as function of frequency (a) all samples at room addition process indicating that the probability of quantum tunnel-
temperature and (b) show the behavior of s′ at different temperatures for BaFe12O19 ing increases with the metal addition which reflects that the
sample. probability of phonon assisted tunneling or hopping is reduced.

Table 4
Frequency exponent (S) and polaron binding energy (Wm) for all BaAlxFe12−xO19 samples.

T (K) Prepared samples

BaFe12O19 BaAl0.5Fe11.5O19 BaAl1.5Fe10.5O19 BaAl2.5Fe9.5O19 BaAl3.5Fe8.5O19

S W S W S W S W S W

313 0.687 0.518 0.751 0.648 0.7791 0.732 0.818 0.855 0.832 0.964
353 0.501 0.365 0.614 0.472 0.675 0.568 0.716 0.642 0.758 0.756
393 0.362 0.318 0.3954 0.335 0.432 0.357 0.475 0.387 0.538 0.440
433 0.233 0.291 0.266 0.304 0.312 0.325 0.386 0.365 0.441 0.401
473 0.146 0.286 0.181 0.298 0.211 0.309 0.253 0.327 0.326 0.363
 S.M. El-Sayed et al. / Physica B 426 (2013) 137–143
5. Conclusions
Aluminum substituted barium hexaferrite particles have been
synthesized successfully by the solid state reaction method.
1. The structural measurements of the all samples by the X-ray
diffraction showed that the samples are polycrystalline.
2. Phase formation of BaAlxFe12−xO19 ferrite spectra reveals that
metal oxide vibrations are present which corresponds to the
tetrahedral and octahedral clusters.
3. Barium ferrites are well known hard magnetic materials and
cannot be easily replaced by any other magnetic materials.
Hc of intrinsic barium ferrite is high due to strong uniaxial
anisotropy along the c-axis.
4. The saturation magnetization (Ms) and remanent magnetiza-
tion of BaAlxFe12−xO19 decreased with increasing Al3+ substitu-
tion (0≤x≤3.5) and coercivity field (Hc) increases with increasing
Al3+ substitution.
5. Dielectric constant and dielectric loss increase with increas-
ing temperature at low frequency, whereas at high frequency
their increase with increasing temperature was less
observable.
6. The conductivity values decreased as the Al content was
increased for BaAlxFe12−xO19, while it increased with tempera-
ture for all sample. Also, it is observed that sac ðωÞ value was
frequency dependent.
143
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