ELSEVIER

Journal of Magnetism

and Magnetic Materials

164 (1996) I87- 196

Dielectric behavior and ac electrical conductivity of Zn-substituted Ni-Mg ferrites

M.A. El Hiti

Abstract
The effect of temperature, frequency and composition on the dielectric behavior and ac electrical conductivity were studied for a series of Zn-substituted Ni-Mg ferrite samples prepared using the usual ceramic technique. The experimental results indicated that the real dielectric constant 6, dielectric loss tan 6 and real ac electrical conductivity u, increase with , increasing temperature. The activation energy E, for electric conduction in the ferrimagnetic region, E and tan 6 decrease while the ac conductivity g&w) increases as the frequency increases. E has high values and tan 6 shows dielectric relaxation processes (or peaks) at relatively higher temperatures. The relaxation frequency ,fo shifts to higher values as the temperature increases. Us tan 8 and E increase while the Curie temperature T,, the activ-ation energy for electric ,, conduction Er, E, (in the paramagnetic region) and E, for the dielectric relaxation decrease as Zn ion substitution were found to be temperature and composition increases. The parameters II and B for the electrical conductivity Us dependent. Both 11and B increase as Zn ion addition increases. B increases while n decreases as the temperature increases; II is zero above the Curie temperature. Empirical formulae are suggested for the temperature and composition dependencies of both parameters n and B. K~~KwY/.Y: Ferrites: Electrical conductivity;
Dielectric behavior

1. Introduction Polycrystalline ferrites have high dielectric constants which makes them very useful for microwave applications. Ferrites remain the best magnetic material and cannot be replaced by any other magnetic element because they are inexpensive, more stable and have a wide range of technological applications in transformer cores, high quality filters. radio wave circuits and operating devices [I]. The electrical conductivity and dielectric behavior of ferrites markedly depend on the sintering time and tempera03048853/96/$15.00 Copyright PI/ SO304X853(96)00368-X

ture, chemical composition, preparation conditions, and the quantity and type of additives. Study of the effect of temperature, composition and frequency on the dielectric behavior and ac electrical conductivity offers much valuable information on the behavior of the localized electric charge carriers which can lead to a good explanation and understanding of the mechanism of electric conduction and dielectric polarization in ferrite systems. AC electrical conductivity studies have been performed for Co-Zn ferrites [2], Ni-Mg ferrites [3], Cu-Cr ferrites [4], Co-SbNi ferrites [5] and Ni-Zn ferrites [6-81. Dielectric be-

0 1996 Elvevier Science B.V. All rights reserved.

havior has been studied for Co-Zn ferriten [2]. Ni-Zn ferrites [8-IO], Cu-Cr ferrites [I I] and Mg-Zn ferrites [12]. The electric and dielectric properties of ferrites have been studied extensively, but the ZnNiMg ferrite system has rarely been treated in the literature. Only the dc electrical conductivity [ 131. structure [ 141 and thermoelectric power [IS] have been studied for Zn-NiMg ferrites. while the ac electrical conductivity and dielectric behavior have not been studied at all. Therefore. the present paper is a study of the effect of temperature. frequency and Zn ion substitution on the dielectric and ac electrical properties of the Zn , Mg,,, , Ni ,) 2 FelO, ferrite system prepared using the usual ceramic technique. The effect of Zn ion substitution on the activation energy (for the electric conduction and dielectric relaxation) and Curie temperature was also studied.

from which the real (q,:, 1 and imaginary (w,:) ac electrical conductivities were calculated using the expressions: CT,:. ( h/A) = I cos 4, (I) (2) q,: itself consists of two

c-,: = ( /r/A) 1 sin 4. The real ac conductivity terms [ 161: q,: = a,(T) + o?( w).

(3)

The first term, (r,(T), which is frequency independent and temperature dependent, is due to the drift mobility of electric charge carriers: it is actually the dc electrical conductivity and follows an Arrhenius form. The second term. cr.,(w). is frequency and temperature dependent. and is related to the dielectric relaxation caused by the localized electric charge carriers: it can be written in the power law form [16.17] as: rr?( W) = Bw. (4)

2. Experimental A series of samples of the Zn , ME,).~_ , Ni0.2 Fe,O, ferrite system (with s = 0. 0.2. 0.4, 0.6 and 0.8) were prepared in the form of discs of thickness h and cross-sectional area A using the usual ceramic technique [ 141. Analysis of X-ray diffraction patterns indicated that the studied samples have a single phase cubic spine1 structure [ 141. The surfaces of the samples were well polished and rubbed with silver paste as the contact material for the electrical measurements. The discs were placed between two electrodes inside the evacuated cell of a silica tube to avoid moisture absorption on the surface. The silica tube was supported within a furnace and a Ni-NiCr thermocouple to control and measure the temperature. An ac signal of V= I V and frequency in the range IO -IO Hz was applied to the circuit. The complex impedance measuring technique (lock-in amplifier SR 510 type, USA) was used to measure the ac voltage drop V, developed across a standard resistance R. frequency ,f and phase angle 4 between the voltage V, and current I simultaneously. The standard resistance R value was adjusted co make V, very small with respect to V. i.e. V,/V< 1%. The current I passing through the sample was calculated using Ohm law (I = V,/R). s This current consists of two terms, the in-phase component ( I cos I$) and the out-of phase component (I sin 4)

where w = 2~,f is the angular frequency, B and II are composition and temperature dependent parameters. the exponent 11 is dimensionless while B has conductivity units (0-l cm- The capacitance C ). of the sample (in picofarad) was calculated from the imaginary part of the ac electrical conductivity as follows: C = I sin d/w. The real dielectric C values as: E ll..iC(h, = A). The dielectric tan 6= l/tan loss. tan 6, was calculated 4. using: (7) constant E was calculated (5) from

(6)

where 6 = 90 - d. This experimental work was carried out at the Physics Department. Faculty of Science. Tanta University. Tanta, Egypt.

3. Results and discussion

The frequency dependence of the ac electrical conductivity a,(w), real dielectric constant E and

calculated for all samples at the designated temperatures. Fig. I indicates that a,(w) increases as the frequency increases in the ferrimagnetic region of

i
. ._

644 .K _.. ... . .. .I.

. ..

...

. .. . . . . ..
....

5. :::.: ..... :::;_ i

-2
-3

K 512

-4

106 :: -..,_ x-0 4 ., 105 ,,y:::: : ....1,?_ ... 104 ; :_::::::;,, : :::y+, . I , o3 :..pi; ;; j]l:: j+i. :::: I soih : :.... :::;i .a., i -lc

Fig.

I.

Frequency

dependence of oz( w) kitvarious

tcmperaturer.

dielectric loss tan 6 is illustrated in Figs. l-3, respectively. at selected temperatures. CT?(W), as shown in Fig. I. increases while E (Fig. 2) and tan 6 (Fig. 3) decrease as the frequency increases. According to Eq. (4), the logarithmic relation between (T?(W) and angular frequency w represents a straight line with a slope equal to the exponent n and intercepts a part equal to log B on the vertical axis at log w = 0 for each sample at the designated temperature, as shown in Fig. I. From Fig. I, the values of II and B were

106 :;z:::,.:: xmo.8 :: __ K t s,p1,:;;:;.. . .._ ma

> (.I,

*a*

. . ,..

. r-4

lo3

Id

105

f [Hz1

Fig. 2. Frequency dependence of E at various temperatures

190

cies. The dispersion or decrease in e and tan 6 as frequency increases takes place when the electron exchange interaction (or hopping) between the ferrous and ferric ions at the octahedral (B) sites cannot follow the alternation of the applied ac electric field beyond a certain critical frequency [IO]. All samples have abnormally high dielectric values in the range from IO up to 107. This result is in accordance with that observed earlier of the order of 10 for Mn-Mg ferrites [ 181 and of the order of IO for Ni-Zn ferrites [&l&19], Li-Ni ferrites [20] and Cu-Zn ferrites [9]. The effect of frequency on a,: and E has been studied theoretically and verified successfully experimentally [8,9,21] for various ferrite systems. Many theoretical relationships were derived. but the simplest expression predicted that the real ac electrical conductivity ok,: is directly proportional to the angular frequency w while E and tan 6 are inversely proportional to w [22]: E= 47ra,:./( w tan 6). (8)

Fig. 3. Frequency

dependence

of tan 6 at various temperatures.

ordered states and becomes frequency independent in the paramagnetic region of disordered states above the Curie temperature. E and tan 6 decrease rapidly at lower frequencies and slowly at higher frequen-

The derivation of the theoretical expressions [8,9,2 1,221 was based on the inhomogeneous nature of the dielectric structure which was considered as a double-layer dielectric model (Koops theory) [8]. In this model it was assumed that the polycrystalline sintered ferrite consists of two layers. The first layer consists of large grains of fairly well conducting material which are separated by the second layer which is a thin layer of grain boundaries of relatively poorly conducting substance. These grain boundaries could be formed by the superficial reduction or oxidation of the crystallites in the porous material as a result of their direct contact with the firing atmosphere [20]. The grain boundaries are effective at lower frequencies while the ferrite grains are effective at higher frequencies [4,8,23]. In addition, Eqs. (4) and (8) explain th e increase in a?(o) as shown in Fig. 1, while Eq. (8) explains the decrease in E (Fig. 2) and tan 6 (Fig. 3) as frequency increases. Fig. 3 for tan 6 shows abnormal behavior or dielectric relaxation processes which take place at relatively higher temperatures: these relaxation peaks were shifted to higher frequency values on increasing the temperature. The relaxation in dielectric loss tan 6 has been observed previously for Mn-Mg ferrites [18], Li-Ni ferrites [20], Co-Zn ferrites [24]

M.A. El Hiti/Joumal

qfMagnetism

and Magnetic

Materials

I64 119961 187~106

and Li-Zn ferrites [25]. The dielectric relaxation (peak) takes place when the jumping frequency of the electric charge carrier becomes approximately equal to that of the external applied ac electric field [lo]. The relaxation frequency .f,, was determined from Fig. 3 for all samples as a function of temperature. 3.2. Temperuture dependence

The temperature dependence of the real ac electrical conductivity a.:, real dielectric constant E and dielectric loss tan 6 is shown in Figs. 4-6, respectively, at selected frequencies. Figs. 4-6 indicate that a, E and tan 6 increase on increasing the tempera,, ture; this is the natural character of semiconductor ferrites. This result is in accordance with those observed earlier for Cu-Cr ferrites [4,11]. Ni-Mg ferrites [3], Sb-CoNi ferrites [5], Ni-Zn ferrites [9] and Mn-Zn ferrites [9]. The effect of temperature on E , tan 6 and a.: was studied theoretically and experimentally for Ni-Zn ferrites, Mn-Zn ferrites and hexagonal Ba-ferrites [9]; good agreement was found between the results. Study of the thermoelectric power of the present samples 1151 showed that the majority of the electric charge carriers are electrons above room temperature and the rise in the dc [13] and the present ac electrical conductivity for these samples as temperature increases could be related to the increase in the drift mobility of the thermally activated electrons according to the hopping conduction mechanism in the studied samples. The electron hopping (exchange) between the ferrous Fe + and ferric Fe3 ions on the octahedral sites (which is responsible for electric conduction) is thermally activated by increasing the temperature. This electron hopping causes local displacements in the direction of the external applied electric field; this includes the dielectric polarization in ferrites. As the temperature increases, the dc [13] and present ac electrical conductivities increase due to the increase in the drift mobility of thermally activated electrons [ 151. As a result, the dielectric polarization increases causing an increase in E and tan 6. The semilogarithmic relation in Fig. 4 indicates that the real ac electrical conductivity aaL is frequency dependent in the ferrimagnetic region (from room temperature up to about the Curie temperature

-0

L
C

-2.5. -3 1.4

(
2
2.6

3.2

103/T

IK- I

Fig. 4. Temperature dependence of Us: at selected frequencies: (1) 100 kHz, (2) 50 kHz, (3) 10 kHz and (4) 1 kHz.

T,) for all samples. U~: becomes frequency independent above the Curie or transition temperature in the paramagnetic region. It was reported that. on passing through the Curie point, a change in the gradient of the straight line or slope (Fig. 4) must take place [22], the magnitude of this effect (slope) depending on the exchange interaction between the outer and inner electrons which changes at the Curie point T,. The samples transform from the ferrimagnetic (ordered state) to the paramagnetic state (disordered state) at the Curie temperature. The Curie temperature T, and activation energy for electric conduction E, in the ferrimagnetic and ED im the paramagnetic

region were calculated from Fig. 4 as a function 01 composition. The relaxation frequency ,jn (determined from Fig. 3) was used to calculate the corresponding relaxation time 5-o using the relations: wo7r) = 1, WD = 2T,fl. time is controlled (9) by the relation

This relaxation [26]:

ho = T(, exp( -l&/U),

(IO)

where T(, is the pre-exponential constant. k the Boltzmann constant and E. the activation energy for dielectric relaxation. The semilogarithmic relation in Fig. 7 for relaxation time and temperature gives a straight line of slope -ED/k. The values of E,,

Fig. 6. Temperature ah in Fig. 5.

dependence

01tan 6 at the same t requencie~

So0

500
T WI

700

Fig. 5. Temperature dependence of e at selected frequencies: 100kHr, (2) 50 kHz. (3) IO hHz. (1) I kHr and (5) 100 Hr.

(1)

were calculated from Fig. 7 as a function of composition. The parameters II and B for the electrical conductivity u~( w) (calculated from Fig. I) were found to be temperature and composition dependent. II decreases while B increases as the temperature increases. n becomes negligible or nearly zero above the Curie temperature, because the power law for a,(w) in Eq. (4) becomes invalid and the conductivity becomes frequency independent where the ferrimagnetic samples transform to paramagnetic samples. It was reported that II has values between 0 and I [ 161. For II = 0. the electric conduction is frequency independent. or dc conductivity and frequency dependent for 1 > II > 0. In this study II lies

studied Zn , Mg s ~_,Ni Ij z Fe,O, samples could empirically suggested in the following forms:
(I

be

f2( 7) = ST , B(T) = NT,

(11)
(12)

1.4

1.5

16

17 10sf T [c 1

1.6

1.9

Fig. 7. Temperature
\ = 0, (b) .k- = 0.2.

dependence Cc) .t- = 0.1.

of the relaxation

time

7,). for (a)

Cd) .Y = 0.6 and (e) _k-= 0.8.

where dimensionless constants tn = -2.8 and g = 4.8 for the ferrite system Zn, Mg,, s_, Ni,, ,Fe,O,. S has units of Km- while N has units of a- cm- Km The expression in Eq. (I I) for the . temperature dependence of the exponent II has been suggested previously for Ni-Mg ferrites [3] and Co-SbNi ferrites [4]. Before setting up general theoretical formulae for the temperature dependence of the parameters t7 and B in the power law for a,(~), more extensive studies have to be performed for different ferrite systems.

between 0.005 and 0.1. The electrical conductivity increases as the temperature increases, which increases the value of B in conductivity units (Eq. (4)). To determine the real temperature dependence of both II and B. the logarithmic relation has been drawn as illustrated in Fig. 8a,b, respectively. The logarithmic relation shows parallel straight lines with a slope of -2.8 for 17 (Fig. &I> and of 4.8 for B (Fig. 8b) for all the studied samples. Therefore, the temperature dependence of both 17 and B for the
-0

The compositional dependence of c$,. tan 6 and E is shown Fig. 9a,b.c. respectively, at selected

-E

-1

-1 a g -2

-3

-4.

-5. 51 2.4

2.5

2.6 Loci T

2.7

Fig. 8. Temperature

dependence

of (a) II and (b) B

Fig. 9. Compwitional dependence of (a) c-c; at 300 K for various frequencies. (b) tan 6 and (c) E at (1) I kHz, 600 K: (2) IO kHz. SO0 K: (3) SO kHz. 100 K; (3) 100 kHlr, 300 K.

194

M.A. El Hiti/ Journal ofMugnetian

und Magnetic Mutrridc

164 (IYY61 187-196

frequencies and temperatures. a,:, E and tan 6 increase as Zn ion substitution increases. This result is explained on the basis that the conduction mechanism could be expressed in terms of electron hopping between ferrous and ferric ions on octahedral sites for n-type semiconductor ferrites and in terms of hole hopping for p-type ferrites [27,28]. The cation distribution shows that Zn ions strongly prefer the occupation of tetrahedral sites (A sites) [29], Ni ions prefer the occupation of B sites [29,30] while Mg and Fe ions partially occupy A sites as well as B sites [3 1,321. The increase of Zn ion substitution at A sites replaces some Mg ions. As a result, other Mg and Fe ions will migrate from A sites to B sites [32] to replace the reduction in Mg ions. Then, the number of ferrous Fe and ferric Fe?+ ions between which the electron exchange interaction (hopping conduction mechanism) takes place at the B sites increases, therefore the electrical conductivity increases. Since the mechanism of dielectric polarization in ferrites is similar to that for electric conduction [33], the increase in the number of electrons

Table I A comparison between the values of r, E, and Ei for present ac and previous dc [ 131 electrical conductivity studies .x Composition r, (10
X

E p (eV) ac 0.17 0.15 0.12 0.11 0.10 dc 0.18 0.16 0.14 0.13 0.12

E, ac

(eV)

dc 667 641 603 570 453

dc 0.16 0.14 0.12 0.10 0.08

0.0 0.2 0.4 0.6 0.X

Mg,, xN~,, *Fe,O, MgohZn,?NiozFezO, Mg,,,ZnO,Ni,,FezO, Mg,lZn,bNi,lFe,O, Zn,, 8Ni, zFezO,

670 645 606 561 460

0.14 0.13 0.10 0.08 0.06

00

z
00

t-u

\ .
_ 41 00

0.06

Fig. IO. Compositional dependence (c) E, at selected frequencies

of (a) E,,

(b) E, and T, and

exchanged between Fe and Fe3+ ions results in + local displacements in the direction of the applied external electric field which determines the dielectric polarization. This explains the increase in a,:, E and tan S with increasing Zn ion substitution. Experimentally, it was found that E is directly proportional to the root mean square of the electrical conductivity for Ni-Zn ferrites [8]. Zn-NiMg ferrites [13] and Ni-Mg ferrites [34]. This is another reason supporting the increase of E and a,: as Zn ion addition increases. The effect of Zn ion substitution on the activation energy E, for dielectric relaxation, the Curie temperature T, and the activation energy for electric conduction E,, in the paramagnetic region and Et in the ferrimagnetic region is shown in Fig. IOa,b,c, respectively. Fig. 10 shows that T,, E,, Ef and E, decrease on increasing the Zn ion substitution. This result agrees well with the conclusion that the lower activation energies and Curie temperatures are associated with a higher electrical conductivity [8,22]. The activation energy for electric conduction in the paramagnetic region Ep is higher than that in the ferrimagnetic region E1. This could be related to the disordered state in the paramagnetic region (of higher activation energy and lower conductivity) with respect to the ordered state in the ferrimagnetic region (of lower activation energy and higher conductivity). This result is in accordance with those observed for Co-Zn ferrites [35], Zn-MgNi ferrites [ 131, Mn-Zn ferrites [21], Li-Ti ferrites [36] and Ni-Zn ferrites [37]. This result is also in agreement with the theory developed by Irkhin and Turov [38]. In the paramagnetic region of disordered states, the increase of the frequency independent conductivity with increasing temperature corresponds to thermally activated elec-

M.A. El Hiti / Joumcrl ~j Mugnrtism

nnd Magnetic Mutrrials

164 (1996) 187-196

195

tric charge carriers (band conduction mechanism) [4] and the activation energy is constant (or frequency independent). The activation energy Er for electric conduction in the ferrimagnetic region decreases as the frequency increases. In the ferrimagnetic region of ordered states, the frequency dependent conductivity and activation energy vary with frequency. corresponding to the thermally activated mobility (hopping conduction model) [4]. The values of Tc. E, and E, as compared with the published results of dc conductivity for the same samples [13] are listed in Table 1 and indicate that the results of the present ac and previous dc [ 131 conductivity measurements are in good agreement. The values of the parameters n and B (calculated from Fig. I) were found to be composition dependent, with both IZ and B increasing with increasing Zn ion substitution. When Zn ion addition increases, the electrical conductivity (Fig. 9a) increases and, according to Eq. (4), the values of the exponents 11 and B (which has conductivity units) must also increase. To determine the exact composition dependence relation (befor both n and B, a semilogarithmic tween In y1and In B versus x) was drawn at selected temperatures, as indicated in Fig. 11a,b, respectively. This relation represents parallel straight lines with a

slope equal to 1.34 for n (Fig. 1 1a> and 4.15 for B (Fig. 1 lb) and intercept parts on the vertical axes at x = 0. As a result, the empirical composition dependence of n and B can be suggested in the following form: n(x) B(x) =Ae . =A e, ( 3) ( 4) a are dimensionless constants, A units (K cm- ) and a = 1.34 all samples. These suggested emhave to be studied extensively them as general formulae.

where A. u and has conductivity and a = 4.15 for pirical expressions before considering

4. Conclusion The results of this study can be summarized as follows. (1) The real ac electrical conductivity increases while the dielectric loss, real dielectric constant and activation energy for electric conduction in the ferrimagnetic region decrease as frequency increases. (2) The real dielectric constant has abnormally high values and the dielectric loss exhibits a dielectric relaxation process or peaks at relatively higher temperatures. The relaxation frequency shifts to higher frequency as the temperature increases. (3) The real ac electrical conductivity, real dielectric constant, dielectric loss and dielectric relaxation frequency increase as the temperature increases. (4) The real ac electrical conductivity, real dielectric constant and dielectric loss increase as Zn ion substitution increases. (5) The Curie temperature and activation energy for electric conduction in both the paramagnetic and ferrimagnetic regions and for dielectric relaxation decrease as the Zn ion substitution increases. (6) The activation energy in the paramagnetic region is higher than that in the ferrimagnetic region. (7) The parameters II and B for the electrical conductivity cr2( w) were found to be composition and temperature dependent. Both n and B increase as Zn ion addition increases. n decreases while B increases as the temperature increases. (8) Empirical formulae were suggested for both the temperature and composition dependence of n and B.

0.2

0.4 X

0.6

0.0

Fig.

11. Compositional

dependence

of (a) II and (b) B.

(9) The electric conduction is similar to the dielectric polarization and are related to the electron exchange interaction between the ferrous and ferric ions on the octahedral sites.

63. FIXI P. Reddy and T. Rae, J. Leawxmmon Metals 105 ( 19X5) iI91 C. Prakash and J. Bi.jal. J. Lc\s-common Metal\ 107 (14X.5)
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don.

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[II El Dl [Jl