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Copyright 2013 by American Scientic Publishers
All rights reserved.
Printed in the United States of America
Advanced Science Focus
Vol. 1, pp. 225230, 2013
(www.aspbs.com/asfo)
The Electrical Resistivity and ac Conductivity of
Co Substituted LiNiZn Nanocrystalline
Ferrites Prepared by a Chemical Method
A. T. Pathan
1,
and A. M. Shaikh
2
1
Department of Physics, M. H. Saboo Siddik College of Engineering, Mumbai 400008, India
2
Department of Electronics, The New College, Kolhapur 416014, India
The dc electrical resistivity measurements of the ferrites Li
0.5
Ni
0.25x,2
Co
x,2
Zn
0.5
Fe
2
O
4
(x = 0, 0.1, 0.2, 0.3,
0.4 and 0.5), were performed as a function of temperature and composition, in the temperature range from
room temperature to 500

C. A break in the plot of ln j against 1/T has been observed around Tc (Curie
temperature). This break is associated with the change in activation energy around the Curie temperature. The
composition dependence of the dc electrical resistivity is found to support the hopping conduction mechanism.
The activation energy and drift mobility were calculated from the temperature-dependent dc electrical resistivity
measurements. AC conductivity of the samples was measured in the frequency range 20 Hz1 MHz. The
electrical conduction mechanism could be explained with the help of an electron hopping model. The nano
crystalline nature of ferrites was also conrmed by Transmission Electron Microscopy (TEM).
KEYWORDS: Ferrites, Activation Energy, Resistivity, Polaron Hopping, TEM.
1. INTRODUCTION
High resistivity ferrites with low eddy current losses are
required from the technological applications point of view.
The electrical resistivity of ferrites has been normally
found to increase on doping or substituting with other
oxides. In the last few years several studies have been
reported with addition of divalent, trivalent and tetrava-
lent ions to study various parameters depending on the
intended applications of the ferrites. With a view to under-
stand the effect of Co substitution on the electrical prop-
erties a series of Co substituted lithium nickel zinc ferrites
were synthesized and studied.
Cobalt ferrite possesses an inverse spinel structure and
the degree of inversion depends upon the heat treatment. It
is reported that cobalt ferrites are in demand due to these
properties for magnetic recording, magneto optical record-
ing and other electronic devices.
12
Li-ferrites emerged
as good microwave device materials due to their high
Curie temperature, high squareness ratio, superior temper-
ature stability of saturation magnetization, low intrinsic
linewidth and low magnetic losses. The physical properties
of spinel ferrites are attributed to the distribution of cations
among the tetrahedral (A) site and the octahedral (B) sites.

Author to whom correspondence should be addressed.

Email: asrar.pathan@rediffmail.com
Received: 29 September 2013
Accepted: 21 October 2013
The dielectric properties and the conductivity of the fer-
rites depend on the preparation method, chemical compo-
sition, grain size, frequency and temperature.
34
Abdeen
et al.
5
studied structural, electrical and transport phenom-
ena of CdCo ferrites and reported an increase of lattice
parameter and X-ray density with Cd
2+
contents and a
decrease of porosity. Vasambekar et al.
6
have reported the
resistivity of Co ferrites to be higher than that of Cd fer-
rites. It is found to be dependent on the saturation mag-
netic moments of the samples. Ghatage et al.
7
measured
electrical resistivity and seebeck coefcient as a func-
tion of temperature for the system (Ni
0.5+x
Zn
0.5
Ti
x
Fe
2

xO
4
) with x = 0.0, 0.2, 0.4 and 0.5. Iftimie et al.
8
have
studied the possibility of the use of nickel ferrite as semi-
conducting gas sensor. Their results of the sensitivity stud-
ies of (Ni
0.94
Co
0.01
Mn
0.02
Fe
1.98
O
4
) ferrite revealed that the
electrical resistivity of ferrites prepared by self combus-
tion is more sensitive to acetone and its sensitivity depends
on the temperature. Ahmed et al.
9
studied the conductiv-
ity improvement of LiCoYb ferrites. The temperature
dependence of the polarization and resistance was studied
in the range 300 K to 700 K. Soibam et al.
10
prepared
and studied the electrical properties of Cobalt substituted
LiZn ferrites. Their result shows that the substitution of
Co
2+
greatly affects certain properties of LiZn ferrites
like the increase in lattice parameter, the samples are den-
sied as is indicated by the decrease in porosity, the dielec-
tric constant decreases. However the divalent Co
2+
ion
Adv. Sci. Focus, Vol. 1, No. 3, 2013 2330-0760/2013/1/225/006 doi:10.1166/asfo.2013.1043 225
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substitution enhances the dc resistivity of the basic LiZn
ferrites. Sattar et al.
11
have reported that the compositional
dependence of the dc electrical resistivity is found to sup-
port the hopping conduction mechanism in Zr
4+
substi-
tuted LiZn ferrite. Maisnam et al.
12
have reported that the
room temperature dc resistivity as a function of composi-
tion showed an increasing trend with increase in Co
2+
ion
concentration for x > 0.2 in CoLiNiMn ferrites pre-
pared by the ceramic route. Kapse et al.
13
showed that
the activation energy calculated from the dc electrical con-
ductivity versus temperature for all the samples ranges
from 0.6156 to 0.4714 eV. The dc electrical conductiv-
ity increases while the activation energy was found to
decrease with Zn content in Ni
1x
Zn
x
Fe
2
O
4
(0 x 0.5).
dc resistivity of ferrites as a function of temperature
and drift mobility and activation energy was reported by
different authors.
1415
However there is almost no report on the studies of
mixed Cobalt substituted LiNiZn nanostructured fer-
rites. In the present communication, we report on dc
electrical resistivity and ac conductivity of LiNiCoZn
nanostructured ferrites prepared by chemical method.
2. EXPERIMENTAL DETAILS
Ferrite samples with the chemical formula
Li
0.5
Ni
0.25x,2
Co
x,2
Zn
0.5
Fe
2
O
4
(x = 0.0, 0.1, 0.2, 0.3, 0.4
and 0.5) were prepared by the usual chemical method.
16
The advantages of the wet chemical method over the
conventional ceramic method is given as follows.
Limitations of the ceramic method
Possibility of a chemical inhomogneity due to evap-
oration of certain metals at elevated temperature.
It gives a relatively higher porosity, a lower density
and a higher particle size.
Relatively high sintering temperature and time is
required.
Due to the high temperature there is the possibility
of formation of Fe
2+
ions that may affect the properties of
the samples.
In comparison to ceramic methods, wet chemical methods
are based on the principle of co-precipitation. Generally
these methods have been employed to avoid a lengthy and
tedious milling process involved in the dry methods and to
achieve higher density samples with small grains. Exam-
ples are
(a) the hydroxide co-precipitation method,
(b) the oxalate-co-precipitation method,
(c) the solgel method and
(d) the auto-combustion method.
Conrmation of single phase formation of the sam-
ples was carried out using a Philips X-ray diffractometer
(Philips Model PW 3710) operated at 40 KV and 30 mA
(\ = 1.542 ). The 20 angle was varied from 20

to 80

.
The nanoparticle morphologies were investigated by using
transmission electron microscopy (TEM Model Philips
CM 200 super twin STEM). The dc electrical resistiv-
ity of the disc shaped samples of an average thickness of
23 mm was measured as a function of temperature by
using the two probe method. InHg was used as a contact
material. A small constant current (-10 mA) was passed
through the sample to avoid the Joule heating. A constant
voltage of 10 V was applied across the series combina-
tion of the sample holder containing the sample and a
standard resistance whose value was always less than the
sample resistance. The voltage developed across the stan-
dard resistance was measured with the help of a Keithley
Electrometer from which the current in the in circuit could
be readily obtained. Knowing the current owing through
the circuit and voltage across the sample, resistivity of the
sample could be calculated by using the following equa-
tion
j = (rJ
2
,4t)R (1)
where, R is resistance of the pellet, t is the thickness of
the pellet and J denotes the diameter of the pellet. The d.c
resistivity has been measured at various temperatures from
room temperature to about 773 K. According to Wilsons
law the resistivity values are given by the equation
j = j
0
exp(AE,kT ) (2)
wheren j is the resistivity in ohm cm, AE is the activation
energy in eV, k denotes the Boltzmann constant, and T the
absolute temperatutre in K.
The plots of the log j versus 1000,T were plotted for
all the samples under investigation and activation energy
values (AE) were calculated using the relation
AE = 1.98310
4
|Alog
10
j,A(1,T )] eV (3)
The drift mobility j of the charge carrier in the syn-
thesized sample is calculated by following equation
j = 1,nej (4)
where n is number of charge carriers, e the charge on
electron and j is the resistivity at a given temperature.
The AC conductivity (u
ac
) is related to the dielectric
relaxation caused by localized electric charge carriers. The
frequency dependent AC conductivity was calculated from
the dielectric constant and the loss tangent (tan o) using
the relation
u
ac
= wa

a
o
tan o (5)
where, a

is the real dielectric constant, a

o
is the permit-
tivity of free space, tan o is the loss tangent at real a

and
w is the angular frequency (i.e., = 2r] ).
The frequency response of the dielectric behavior and
the AC conductivity are known as the relaxation spectrum
or the dispersion curve, respectively, which gives the infor-
mation about the conduction mechanism in the ferrite.
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The u
ac
is temperature and frequency dependent and
it is attributed to the dielectric relaxation caused by the
localized electric charge carriers which obey the law,
u
ac
(wT ) = Bwn (6)
where B and n are composition and temperature dependent
parameters.
3. RESULTS AND DISCUSSION
3.1. XRD Analysis
The X-ray diffraction patterns reveal that all the samples
are having single phase cubic structure. The lattice con-
stants are listed in Table I. The variation of X-ray den-
sity and porosity with cobalt composition is shown in
Figure 1. The details about the method of preparation,
variation of lattice parameter, X-ray density and poros-
ity with cobalt composition were reported in our earlier
communication.
1617
3.2. TEM Analysis
The Transmission Electron Microscopy was used to record
the size of the ferrite particles. Typical TEM images of the
synthesized powder captured at different magnications of
the sample are shown in Figures 2(a) and (b), which con-
rm their nano crystalline nature. Most of the particles
appear spherical in shape, however some elongated parti-
cles are also present. More agglomerated particles of low
polydispersity in size than separated particles are present
in the images. Agglomeration appears unavoidable due the
absence of a surfactant. The average particle size is found
to be around 30 nm. The size of the particles as observed
by TEM is consistent with the average particle size of 17 to
24 nm as estimated from XRD analysis, which is reported
in our earlier communication.
25
3.3. DC Electrical Resistivity
The plots of logj versus 1000/T for the samples
Li
0.5
Ni
0.25x,2
Co
x,2
Zn
0.5
Fe
2
O
4
ferrites where x = 0, 0.1,
0.2, 0.3, 0.4 and 0.5 are shown in Figure 3. From the
plots it can be concluded that as the temperature increases
the resistivity decreases linearly, and shows transition near
the Curie temperature. At this temperature the material
Table I. Data on lattice constant (a), X-ray density (dx), porosity for
Li
0.5
Ni
0.25x,2
Co
x,2
Zn
0.5
Fe
2
O
4
ferrites.
Composition Lattice X-ray Porosity
(x) constant, a, () density (g/cc) P (%)
x = 0 8.352 5.167 27.09
x = 0.1 8.364 5.145 22.80
x = 0.2 8.376 5.123 19.32
x = 0.3 8.389 5.100 16.66
x = 0.4 8.410 5.035 14.39
x = 0.5 8.438 5.018 12.97
0.00 0.05 0.10 0.15 0.20 0.25
5.00
5.02
5.04
5.06
5.08
5.10
5.12
5.14
5.16
5.18
Cobalt content (x)
X
-
r
a
y

d
e
n
s
i
t
y
(
g
/
c
c
)
12
14
16
18
20
22
24
26
28
P
o
r
o
s
i
t
y
,

P

(
%
)
Fig. 1. Variation of X-ray density (j
x
), porosity (P) with cobalt content.
changes from the ferromagnetic to the paramagnetic state.
The change in slope is observed in the case of all fer-
rites. The activation energies were calculated for the two
different regions.
The DC electrical resistivity of the samples was found
to decrease with increasing Co
2+
content from x = 0 to
x = 0.3 (Table II) and thereafter the resistivity sharply
increases at x =0.4. This increase in resistivity may be due
to the hindrance of the hopping mechanism between Fe
2+
and Fe
3+
and then it decreases rapidly at x = 0.5. It may
be due to the substitution of Co
2+
ions, which decreases
the concentration of Fe
3+
and Ni
2+
ions and correspond-
ingly the formation of Fe
2+
ions, thus restricting the Ver-
way mechanism of electron hopping. This leads to a slight
increase in the DC resistivity at x = 0.4. A similar type
of trend of variation of DC resistivity with composition
was reported earlier.
10, 12, 18
The variation of the resistivity
with composition is shown in the Figure 4. The decrease in
resistivity may be due to the presence of Fe
2+
ions, which
were produced during the sintering on cobalt addition.
19
Another reason for the decrease of j on increasing cobalt
composition is that Co
2+
ions prefer to occupy tetrahedral
(A) sites and Ni ions to occupy octahedral (B) sites., while
Fe
2+
ions partially occupy A and B sites. On increasing
the Co
2+
concentration at A sites, the Ni
2+
ions concentra-
tion at the B sites decreases. This leads to the migration of
some Fe ions from the A sites to the B sites in order to bal-
ance the reduction in Ni ions concentration at the B sites.
As a result the number of ferric and ferrous ions at the
B sites, which are responsible for the electrical conductiv-
ity in the ferrites increases thereby reducing the resistivity
with increasing Co
2+
ion concentration.
20
A similar trend
of resistivity has been reported earlier.
21
3.4. Activation Energy
The activation energies of the samples are given in Table I
along with the other parameters. The activation energy
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Fig. 2. (a) TEM micrograph for the sample with x = 0 and (b) SAD pattern.
1.4 1.6 1.8 2.0 2.2 2.4 2.6 2.8 3.0 3.2 3.4
0.0
0.5
1.0
1.5
2.0
2.5
3.0
3.5
4.0
L
o
g

1000/ T(K
1
)
X=0.0
X=0.1
X=0.2
X=0.3
X=0.4
X=0.5
Fig. 3. Variation of dc resistivity with temperature for
Li
0.5
Ni
0.25x,2
Co
x,2
Zn
0.5
Fe
2
O
4
ferrites.
decreases from 0.329 eV to 0.131 eV as the Co
2+
con-
centration increases from x = 0 to 0.5. The variation
of the activation energy with composition is shown in
the Figure 5. The decrease in activation energy may
be due to the creation of a smaller number of oxygen
vacancies.
21
It may be also due to a decrease in resistivity
with increase of Co
2+
concentration because the activation
energy behaves in the same as that of the DC electrical
resistivity.
Table II. DC resistivity, activation energy, charge carrier concentration
and drift mobility for Li
0.5
Ni
0.25x,2
Co
x,2
Zn
0.5
Fe
2
O
4
ferrites.
Cobalt Activation Carrier Drift mobility
Sr. content Resistivity energy concentration, (j
d
) 10
13
no. (x) j
dc
10
6
D cm (eV) n (cm) Cm
2
/V S
1 0 710.20 0.329 2.19910
23
0.400
2 0.05 332.79 0.35 2.186510
23
0.835
3 0.1 209.58 0.349 2.18010
23
1.366
4 0.15 202.96 0.343 2.17010
23
1.392
5 0.2 292.60 0.254 2.14210
23
0.996
6 0.25 90.48 0.131 2.13510
23
3.235
0.00 0.05 0.10 0.15 0.20 0.25
0
100
200
300
400
500
600
700
800

d
c

x

1
0
6
(

c
m
)
Cobalt content(x)
Fig. 4. Variation of room temperature dc resistivity with cobalt content.
0.00 0.05 0.10 0.15 0.20 0.25
0.22
0.24
0.26
0.28
0.30
0.32
0.34
0.36
A
c
t
i
v
a
t
i
o
n

E
n
e
r
g
y

E
p

(
e
V
)
Co content (x)
Fig. 5. Variation of activation energy with Cobalt content.
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0.00 0.05 0.10 0.15 0.20 0.25
0.0
0.5
1.0
1.5
2.0
2.5
3.0
3.5

d

x

1
0

1
3

c
m
2
/
V
.
s
e
c
.
Cobalt content(x)
Fig. 6. Variation of drift mobility with Cobalt content.
The variation of the drift mobility with cobalt
concentration is shown in Figure 6. It is noted that the drift
mobility increases with increasing cobalt content. The tem-
perature variation of charge carrier concentration is shown
in Figure 7. It can be seen from the gure that the charge
carrier concentration decreases with increase in tempera-
ture continuously.
22
3.5. The Electrical Conductivity
The electrical conductivity in ferrites can be explained
on the basis of Verwey-de-Boer mechanism, involving
electron exchange between ions of the same element,
which are present in more than one valence state and are
distributed randomly over crystallographically equivalent
lattice sites. The number of such ions depends upon the
400 420 440 460 480 500
2.13
2.14
2.15
2.16
2.17
2.18
2.19
2.20
n

1
0
2
3
(
c
m
3
)
T (K)
Fig. 7. Variation of charge carrier concentration with temperature for
Li
0.5
Ni
0.25x,2
Co
x,2
Zn
0.5
Fe
2
O
4
ferrites.
4 5 6 7 8 9 10 11 12
7.4
7.5
7.6
7.7
7.8
7.9
8.0
8.1
8.2
8.3
8.4
L
o
g
(

a
c
)
Log(
2
)
X=0.0
X=0.1
x=0.2
x=0.3
Fig. 8. Variation of AC conductivity for Li
0.5
Ni
0.25x,2
Co
x,2
Zn
0.5
Fe
2
O
4
ferrites (for x = 0, 0.1, 0.2 and 0.3) as a function of frequency.
sintering conditions, evaporation of ions and a reduction
of Fe
3+
and Fe
2+
ions at elevated temperature.
To understand the conduction mechanism and the
hopping of charge carriers responsible for the con-
duction mechanism, the variation of the AC con-
ductivity as a function of frequency was studied.
Figure 8. shows the variation of log u
ac
with logw
2
for
Li
0.5
Ni
0.25x,2
Co
x,2
Zn
0.5
Fe
2
O
4
ferrites, where x = 0, 0.1,
0.2 and 0.3. The plots are almost linear indicating that the
conductivity increases with increase in frequency, which
conrms the polaron type of conduction. In a few cases
the conductivity slightly decreases, which is attributed to
the conduction by mixed polarons. It is well known that
the AC conductivity in disordered solids is directly propor-
tional to the frequency. The electrical conduction mecha-
nism in terms of the electron and polaron hopping model
has been discussed by Austin and Mott.
24
4. CONCLUSION
A series of Co substituted lithium nickel zinc ferrites were
successfully prepared by the auto combustion method. The
XRD study shows that the lattice parameter increases. The
particle size obtained from XRD data is found to be around
1724 nm, which is in close agreement with the aver-
age particle size of 30 nm obtained from TEM studies.
However the divalent Co
2+
ion substitution decreases the
DC resistivity of the basic lithium nickel zinc ferrites,
whereas the drift mobility increases with increasing Co
content. The conductivity of the investigated composition
Li
0.5
Ni
0.25x,2
Co
x,2
Zn
0.5
Fe
2
O
4
increases with increasing
temperature, which is the characteristics of semiconductor
ferrites. The activation energy for electrical conduction in
the paramagnetic region is higher than that in the ferri-
magnetic region.
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Acknowledgment: The authors are thankful to IIT,
Bombay and USIC, Shivaji University, Kolhapur for pro-
viding experimental facilities.
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