research article structural and electrical properties of...
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Research ArticleStructural and Electrical Properties of LindashNi NanoferritesSynthesised by Citrate Gel Autocombustion Method
G Aravind1 D Ravinder1 and V Nathanial2
1 Department of Physics Osmania University Hyderabad Telangana 500007 India2Department of Physics University College of Science Osmania University Saifabad Telangana 500044 India
Correspondence should be addressed to D Ravinder ravindergupta28rediffmailcom
Received 9 July 2014 Revised 19 September 2014 Accepted 21 September 2014 Published 20 October 2014
Academic Editor Israel Felner
Copyright copy 2014 G Aravind et al This is an open access article distributed under the Creative Commons Attribution Licensewhich permits unrestricted use distribution and reproduction in any medium provided the original work is properly cited
An attempt has been made to synthesize nanocrystalline lithium-nickel ferrites with a compositional formulaLi05minus05xNixFe25minus05xO4 (where 119909 = 00 to 10 with step of 02) by a low temperature citrate gel autocombustion method
Single phase cubic structure is confirmed by X-ray diffraction analysis This result demonstrates that the prepared samples arehomogeneous and the sharp peaks reveal that the samples are in good crystalline form As the Ni concentration is increasedvarious interesting changes in the values of the structural parameters like lattice parameter X-ray density bulk density andporosity have been observed The surface morphology of the prepared samples was studied using scanning electron microscopy(SEM) The DC resistivity measurements were carried out using two-probe method from 200∘C to 600∘C The variation oflog(120590119879) with reciprocal of temperature shows a discontinuity at Curie temperature log(120590119879) versus 1119879 plot of the pure lithiumferrites is almost linear which indicates the Curie temperature of the pure lithium ferrites was beyond our measured temperatureThe dielectric properties of these ferrites have been studied using a LCR meter from the room temperature to 700K at variousfrequencies up to 5MHz which reveals that all the prepared samples have dielectric transition temperature around 600K
1 Introduction
The spinel magnetic ferrites have generated considerableinterest among the researchers all across the world due totheir unique and versatile properties Novel electrical andmagnetic behaviors are observed for the nanosized magneticparticles when compared to that of the bulk counterparts [1]In the early days garnets were used for microwave deviceswhere they have high value of electrical resistivity and lowdielectric losses But because of low Curie temperature highstress sensitivity and high cost of the garnets they are rarelyused Recently spinel ferrites are often used in place ofgarnets Lithium ferrites and substituted lithium ferrites havebecome important materials for the microwave applicationssuch as in circulators isolators and phase shifters due to theirhigh resistivity low dielectric losses high Curie temperaturesquare hysteresis loop and low cost [2ndash6]
In the inverse spinel lithium ferrite structure Li05Fe25O4
Li+ and 35th of the Fe+3 ions occupy octahedral sites (B-sites)
of cubic spinel structure AB2O4 The distribution of cations
in the inverse spinel structure of lithium ferrite is given by(Fe+3)[Li+1
05Fe+305Fe+3]O
4 where parentheses and square
brackets indicate the ion distribution on tetrahedral (A-site)and octahedral (B-site) sites respectively [7 8]
The diverse properties of spinel lithium ferrites originatefrom their ability to incorporate a variety of transition metalcations into their lattice causing a subsequent change intheir structural optical magnetic and electrical properties[9 10] The observed changes in these properties are broughtabout by a redistribution of cations among the tetrahedraland octahedral sites of the ferrite sublattice The substitutionof various metal ions into the lattice of the lithium ferritegives rise to materials with new and interesting propertiesThis is because the degree of inversion in the substitutedlithium ferrites and therefore their properties are found to bestrongly dependent on the preparation conditions (method ofpreparation sintering time sintering temperature pH valueetc) amount of the substituent and type of substitution and
Hindawi Publishing CorporationPhysics Research InternationalVolume 2014 Article ID 672739 11 pageshttpdxdoiorg1011552014672739
2 Physics Research International
+Mixing and
stirring
Continuous stirring
Heating to
Grinding
Homogeneous solution of
metal nitratesCitric acid
pH 7 maintained byadding ammonia
Viscous gelDry gelAutocombustion
Burnt ash
GrindingCalcination at Nanoferrite
powder
and heating to 100∘C
200∘C
500∘C for 4hr
Figure 1 Schematic diagram representing preparation of nanoferrites
so forthTheDCelectrical conductivity of ferrites is one of theimportant properties which gives the valuable informationabout the conduction mechanism Moreover electrical con-ductivity has a significant effect on the dielectric polarizationin the spinel ferrites
Several methods are used for synthesizing nanosizedspinel ferrites such as coprecipitation sol-gel microemul-sion hydrothermal citrate gel and reverse micelle methods[11ndash13] In the preparation of lithium based ferrites low tem-perature sintering is needed to suppress lithium volatility andoxygen loss during sintering Many researchers proposed thecitrate gel method is a simple route to synthesize materials inthe nanocrystalline form due to lower sintering temperatureSeveral investigations on the properties of the LindashCd [14] LindashZn [15] and LindashMg [16] ferrites have been reported Mazenand Elmosalami [17] and Bhatu et al [18] have synthesizednickel substituted lithium ferrites by ceramic method withhigh sintering temperature However there are no detailreports on Ni substituted lithium nanoferrites prepared bycitrate gel autocombustion method with low sintering tem-perature
In the present study we report the synthesis of nickel sub-stituted lithium nanoferrites by nonconventional citrate gelautocombustion method XRD studies of prepared samplesSEM micrographs temperature dependent DC conductivitystudies and the dielectric properties of these ferrites from theroom temperature to 700K at various selected frequencies upto 5MHz have been studied
2 Experimental Techniques
Nanocrystalline nickel substituted lithium ferrites having thechemical formula Li
05minus05xNixFe25minus05xO4 (where 119909 = 00to 10 with step of 02) were synthesized using citrate gelautocombustion method This method has certain inherentadvantages like low processing temperature (200∘C) goodstoichiometric control and homogeneous distribution ofreactants and production of ultrafine particles with narrowsize distribution In this citrate gel autocombustion method
metal nitrates act as oxidizing agents and organic fuels asreducing agents [19 20] The various powder propertiescan be systematically tuned by altering the oxidant to fuelratios In present study fuel to oxidizing ratio was maintainedat unity The detailed synthesis process is represented inFigure 1
The stoichiometric amounts of ferric nitrate (Fe(NO3)2
9H2O) Nickel nitrate (Ni(NO
3)26H2O) lithium nitrate
(LiNO3) and citric acid (C
6H8O7sdotH2O) (all chemicals are
SD Fine-Chem Limited) were weighed and dissolved sep-arately in minimum amount of distilled water All the indi-vidual solutions were mixed together and then the ammoniasolutionwas slowly added to adjust the pH value at 7The pro-liferation of nitrate ions at low pH value is likely to decreasethe enthalpy of exothermic reaction by decreasing the fuelto oxidizing ratio Thus the rate of combustion reactiondecreases and particles agglomerate [21] so the pH value ofthe solution was maintained at 7 to avoid the agglomerationand preserve the stoichiometry The resultant solution waskept on a hot plate magnetic stirrer at 100∘C till gels wereformed after that increasing the temperature up to 200∘Cthe gels self-ignited in an autocombustion manner till wholecitrate complex was consumed to yield nanoferrite powdersThe as synthesized ferrite powders were annealed at 500∘C for4 hours in a muffle furnace [22]
The structural characterization of the synthesized sam-ples was carried out by Philips X-ray diffractometer (Model3710) using Cu K
120572radiation of wavelength 15405 A at room
temperature by continuous scanning in the range of Braggrsquosangles 5∘ to 80∘ in steps of 2∘min to investigate the phase andcrystalline size
The average crystalline size of the ferrites was determinedfrom the measured width of their diffraction pattern usingDebye Schererrsquos formula
119863 =
091120582
120573 cos 120579 (1)
where 120582 is the wavelength of the X-ray used for diffractionand 120573 is the full width half maximum (FWHM) in radians
Physics Research International 3
The lattice constant was calculated using the followingrelation
2119889 sin 120579 = 119899120582 (2)
where 119889 = 119886(ℎ2 + 1198962 + 1198972)12 for Fcc systemThe X-ray density (119889
119909) has been calculated according to
the relation
119889119909=
8119872
1198863119873
[gmcm3] (3)
where 119872 = molecular weight of the sample 119886 is the latticeparameter and119873 is the Avogadro number
The volume of the unit cell 119881 = 1198863The experimental density of the prepared sample was
calculated by Archimedesrsquo principle with xylene media usingfollowing relation
119889119864=
119908air119908air minus 119908xylene
times density of xylene (4)
where 119908air is weight of the sample in air 119908xylene is the weightof the sample in xylene
Porosity 119875 of the ferrite sample was then determined byemploying the relation
119875 = 119889119909minus
119889119864
119889119909
(5)
The powders of different compositions were pressed intodisc shaped pellets of 13mm diameter by applying a pressureof 25 times 108Nm2 Silver coating was done on adjacent facesof circular disc shaped pellets to have good ohmic contactand also tomake parallel plate capacitor geometrywith ferritematerial as a dielectric medium
The DC electrical conductivities of nanoferrite materialswere measured by two-probe technique in the temperaturerange 473ndash873K The measurements were recorded in thesteps of 10 K
The dielectric parameters like dielectric constant (1205761015840)and dielectric loss tangent (tan 120575) were measured usingAgilent E4986A precession LCR meter in the temperaturerange 313 Kndash723K at selected frequencies (75 kHz 30 kHz600 kHz 1MHz 3MHz and 5MHz) up to 5MHz frequency
The dielectric constant of prepared sample was calculatedusing the following relation
1205761015840=
119862119905
120576119900119860
(6)
where 119862 is the capacitance of the pellet 119905 is the thickness ofthe sample pellet 119860 is the cross section area of pellet and 120576
119900
is the free space permittivity
Inte
nsity
(AU
)
(440
)
(511
)(4
22)
(400
)
(311
)
(220
)
x = 10
x = 08
x = 06
x = 04
x = 02
x = 00
20 30 40 50 60 70 80
2120579 (deg)
Figure 2 XRD pattern of the Li05minus05xNixFe25minus05xO4 nanoferrites
3 Results and Discussion
31 Structural Analysis The structural study is essential foroptimizing the properties needed for various applicationsThe phase identification and lattice constant determinationof the prepared samples were performed on the X-ray diffrac-tion analysis The obtained XRD pattern of the nickel substi-tuted lithium nanoferrites samples having chemical formulaLi05minus05xNixFe25minus05xO4 (where 119909 = 00 to 10 with step of 02)
sintered at 500∘ for 4 hours was shown in Figure 2 The XRDpatterns of the calcined LindashNi nanoferrite powders (shown inFigure 2) confirm the formation of a single phase cubic spinelstructure with no extra impurity diffraction lines The strongdiffraction from the (220) (311) (400) (422) (511) and (440)planes confirms the pure spinel phase of the annealed ferrites[23 24]TheXRDpattern perfectlymatcheswith the standardpattern with JCPDS reference code 00-013-0207
The average crystallite size of the prepared nanoferritesamples was in the ranges from 39 to 49 nm for different dop-ing levels of the Ni+2 ions (Table 1) The lattice constant (119886) isfound to be increased with the increasing of the Ni+2 ion con-centration (Table 1) This is obvious because Ni+2 ions havethe larger ionic radii (078 A) than that of Li+1 ion (076 A)and Fe+3 ion (067 A) and obey Vegardrsquos law [25 26]The sub-stitution by the larger ions results in expansion of lattice Anincrease in the lattice parameterwhenLi and Fewere replacedby Ni as observed in the present work is therefore expectedThe observed deviation in the value of lattice parameter canbe attributed to the rearrangement of cations in the nanosizedLindashNi ferrites consequent to the sintering process
X-ray density values of the LindashNi nanoferrites wereincreased with increasing the Ni concentration becausemolecular weight of the samples increases with increasing theNi composition It is noted that X-ray density of each sample(119889119909) is greater than the corresponding bulk density (119889
119890)which
is an evidence of the presence of pores in the samplesThe surface morphology of the LindashNi nanoferrite parti-
cles sintered at 500∘C was examined by scanning electron
4 Physics Research International
Table 1 Crystalline size lattice parameter X-ray density bulk density and porosity of LindashNi nanoferrites obtained from XRD analysis
S No Composition Mol wt(gmmole)
Crystallitesize (nm)
Lattice parameter(A∘)
X-ray density (119889119909)
(gmcc)Expt density (119889
119890)
(gmcc) Porosity (119875)
1 Li05Fe25O4 207079 4190 8356 4713 4286 9012 Li04Ni02Fe24O4 212538 3954 8356 4839 4319 10703 Li03Ni04Fe23O4 217998 4535 8358 4957 4329 12664 Li02Ni06Fe22O4 223458 4990 8361 5076 4553 10315 Li01Ni08Fe21O4 228918 4130 8368 5206 4568 12226 NiFe2O4 234379 4301 8374 5334 4742 1107
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
(a)
x = 02 x = 04
(b)
Figure 3 (a) SEM images of the Li05minus05xNixFe25minus05xO4 nanoferrites (b) SEM images with grain size of the samples at 119909 = 02 and 119909 = 04
microscopy (SEM) shown in Figure 3(a) which indicatesthe agglomerated nanoparticles which is attributed to themagnetic exchange interaction between the nanoparticles Itis observed that the average grain size of the prepared samplesgoes on increasing on substitution of Ni in the place of Li andFe in ferrites The average grain size of all the prepared sam-ples directly calculated from SEM instrument is in the range
of 50ndash130 nm only The SEM images of samples 119909 = 02 and119909 = 04 with grain size were shown in Figure 3(b) and grainsize of remaining samples is also in the same range (the figuresare not shown)
32 Electrical Properties The DC electrical conductivity ofthe prepared samples was measured by two-probe method
Physics Research International 5
Table 2 Electrical resistivity and activation energies of the Li05minus05119909
Ni119909Fe25minus05119909
O4system
S No Composition Resistivity(Ω-cm) Curie temp (∘C) 119864
119886in paramagneticregion (eV)
119864119886in Ferromagneticregion (eV)
1 Li05Fe25O4 921 times 108 mdash mdash mdash2 Li04Ni02Fe24O4 917 times 108 567 161 0823 Li03Ni04Fe23O4 573 times 108 560 127 0934 Li02Ni06Fe22O4 273 times 108 540 095 0835 Li01Ni08Fe21O4 124 times 107 535 090 0736 NiFe2O4 682 times 107 528 081 071
in the temperature range from 473K to 873K The ferritesample is pressed into circular pellets The measurementswere recorded in the steps of 10 K
The temperature dependence of the prepared ferritesconductivity is plotted in accordance with the followingArrhenius type equation
log120590 = log120590119900minus
119864119886
119870119861119879
(7)
where 120590 is the conductivity 120590119900is the conductivity at abso-
lute temperature 119870119861is Boltzmannrsquos constant and 119879 is the
temperature The phenomenon of phase transition cationmigration cation reordering the presence of impurities andmagnetotransport effects are considered to be responsible forthe temperature dependence on the electrical conductivity ofthe prepared ferrite samples
The variations of the electrical conductivity (log120590119879) withinverse of temperature (1000119879) were shown in Figure 4Theconductivity of the ferrite samples increases with increasingthe temperatureThat is temperature increases and resistivityof the ferrites was decreased indicating the semiconductingbehaviour All the plots (except pure lithium ferrites) of elec-trical conductivity (log120590119879) versus 1000119879 yield a change inslope at a particular temperatureThis change in slope occurswhile crossing the Curie temperature (the temperature atwhich the ferromagnetic material changed to paramagnetic)The discontinuity at the Curie temperature was attributedto the magnetic transition from well-ordered ferromagneticstate to disordered paramagnetic state which involves differ-ent activation energies The values of the electrical resistivityand thermal activation energies of the prepared samples atferromagnetic region and paramagnetic region were given inTable 2
It is observed that the activation energy in the ferromag-netic region is smaller than the paramagnetic region this isdue to the effect of spin disordering
Someworkers have reported three regions of conductivity[26ndash29] of which the first region has been attributed to thepresence of impurities second region was due to the phasetransition from tetragonal structure to cubic structure andthe third one was due to the ferromagnetic to paramag-netic change The electrical conductivity of ferrites can beexplained on the basis of the Verwey and de Boer mechanism[30] which involves the exchange of charge carriers thatis electrons between the ions of the same element that are
present in more than one valence state (Fe+2 Fe+3) dis-tributed randomly over the crystallographic lattice sites TheFe+2 ion concentration is a characteristic property of nanofer-rites and it depends on several factors such as sintering tem-peraturetime and atmosphere and annealing time includingthe grain structure Some amount of Fe+2 ions is also formeddue to possible evaporation of Li ions during the sintering[28] Sintering of lithium ferrites is therefore carried out atrelatively lower temperature (500∘C) in order to avoid lithiumloss during sintering
The variation of DC electrical resistivity at 200∘C withNi composition in the Li ferrites is given in Table 2 The DCresistivity of the all the samples was observed to be in therange 124 times 107ndash921 times 108Ω-cm Compositionally decreasein the DC resistivity of LindashNi ferrites with increasing theNi concentration was observed The overall higher valuesof resistivity obtained for the ferrites can be attributed tothe small grain size and better compositional stoichiometrywith reduced Fe+2 formation as a result of low temperatureprocessing by the citrate gel method [31 32]
33 Dielectric Properties The dielectric constant and DCelectrical resistivity of ferrites are very important parametersfrom the application point of view These two parametersare electrical properties and exchange of electrons betweenthe Fe+2 and Fe+3 ions is responsible for these mechanismswhich results in local displacement of charges responsible forthe polarisation in ferrites The dielectric constant (1205761015840) anddielectric loss tangent (tan 120575) were found to be dependenton the variation of external factors such as temperature andfrequencyThe variation of dielectric constant (1205761015840) and dielec-tric loss tangent (tan 120575) with respect to selected frequenciesand temperature in the range of 300K to 700K has beeninvestigated
The variation of dielectric constant (1205761015840) and dielectricloss tangent (tan 120575) for all prepared ferrite samples withtemperature has been studied at different frequencies asshown in Figures 5(a) and 5(b)
It is observed that the dielectric constant (1205761015840) and dielec-tric loss tangent (tan 120575) of prepared samples were increasedwith increase in temperature for all selected frequencies Theincrease in temperature of the sample thermally activates thecharge carrier increasing the electron exchange interactionwhich results in increasing the dielectric constant values of
6 Physics Research International
minus5
minus4
minus3
minus2
minus1
0
1
minus5
minus4
minus3
minus2
minus1
0
1
2
minus5
minus4
minus3
minus2
minus1
0
1
minus4
minus3
minus2
minus1
0
1
minus25
minus20
minus15
minus10
minus05
00
05
10
15
minus30
minus25
minus20
minus15
minus10
minus05
00
05
10
15
x = 00 x = 02
x = 04 x = 06
x = 08 x = 10
161 eV
082 eV
127 eV
093 eV
095 eV
083 eV
090 eV
073 eV
081 ev
071 eV
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
Figure 4 Arrhenius plots for electrical conductivities of Li05minus05xNixFe25minus05xO4 nanoferrites
Physics Research International 7
510152025303540
Temperature (K)
5
10
15
20
25
30
0
20
40
60
80
100
120
020406080
100120140
0
20
40
60
80
100
020406080
100120140
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
75 kHz
75 kHz75 kHz 75 kHz
75 kHz
75 kHz
30kHz
30kHz30kHz 30kHz
30kHz
30kHz600kHz
600kHz600kHz
600kHz
600kHz
600kHz1MHz
1MHz1MHz
1MHz
1MHz
1MHz3MHz
3MHz 3MHz3MHz
3MHz
3MHz5MHz
5MHz5MHz
5MHz
5MHz
5MHz
300 400 500 600 700 800
Temperature (K) Temperature (K)300 400 500 600 700 800 300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
(a)
minus0100010203040506070809
Temperature (K)
0005101520253035
minus02000204060810121416
minus02000204060810121416
0002040608101214161820
minus0200020406081012
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
750Hz
750Hz 750Hz
750Hz
750Hz 750Hz
3kHz
3kHz3kHz
3kHz
3kHz
3kHz
100 kHz
100 kHz100 kHz
100 kHz
100 kHz
100 kHz
1MHz
1MHz1MHz
1MHz
1MHz
1MHz
3MHz
3MHz3MHz
3MHz
3MHz
3MHz
5MHz
5MHz
5MHz
5MHz
5MHz
5MHz
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 5 (a)Variation of dielectric constant (1205761015840)with temperature at different frequencies of Li05minus05xNixFe25minus05xO4 nanoferrites (b)Variation
of loss tangent (tan 120575) with temperature at different frequencies of Li05minus05xNixFe25minus05xO4 nanoferrites
the ferrites It is observed that there are four major con-tributions for polarisation in ferrites They are electronicatomic dipolar and interfacial polarisations [33] Electronicand atomic polarisations are important at high frequenciesand are independent of temperature while remaining two are
important at lower frequencies and dependent on tempera-ture By increasing the temperature interfacial polarisationis increased and dipolar polarisation decreases The increasein dielectric constant with increase in temperature at lowfrequency may be due to the interfacial polarisation
8 Physics Research International
6
7
8
9
10
11
12
13
14
Ni composition
750Hz and 323K
Die
lect
ric co
nsta
nt (120576
998400 )times10
2
00 02 04 06 08 10
(a)
000
002
004
006
008
010 750Hz and 323K
Ni composition00 02 04 06 08 10
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 6 Variation of dielectric constant (1205761015840) and tan 120575 with Ni concentration
From Figure 5(a) it can be noticed that the dielectricconstant (1205761015840) values increase rapidly in the low temperaturerange (119879 lt 600K) whereas in the high temperaturerange (119879 gt 600K) dielectric constant (1205761015840) reaches a stablevalue (Resonance peak) after that it starts to decrease withincreasing the temperature For the low temperature range(119879 lt 600K) the polarisation is increased by the electricfield and also by increasing the number of charge carriers(electrons) which are increased with temperature hence theincrease in the dielectric constant (1205761015840) at low temperaturerange (119879 lt 600K) is due to increase in both temperatureand frequency For the high temperature range (119879 gt 600K)the saturation in the generation of charge carriers is reachedTherefore the electron exchange between the ions of the sameelement that are present in more than one valence state (Fe+2Fe+3 orNi+2 Ni+1) cannot follow the field variation and hencedielectric constant decreases [34] The temperature at whichthe resonance peak appeared is observed to be shifted towardsthe higher temperature as the frequency is increased [35]The variation of loss angle tangent (tan 120575) of the preparedsample as a function temperature at different frequencies hasalso been investigated and an increase is observed just as thedielectric constant (1205761015840) curve This variation of loss tangentwith temperature curve can be understood on the basis ofDebyersquos equation for loss given as [33]
The compositional dependence (Ni concentration) of thedielectric constant (1205761015840) and dielectric loss tangent (tan 120575) ofprepared samples at 323K and at 75 kHz is shown in Figure 6It can be observed that the dielectric constant (1205761015840) value ofthe prepared samples was increased from 119909 = 00 to 119909 =06 and then decreased It can be attributed to the effect ofsimultaneous contributions of different factors such as grainsize density porosity and cation distribution The initialincrease in dielectric constant (1205761015840) when Ni content increasesfrom 119909 = 00 to 119909 = 06 coincides with the increase ofgrain size from Table 1 [36] After that the cation distribution
becomes the predominant factor in decreasing the dielectricconstant (1205761015840) with Ni content since the decrease of holehoping becomes greater than the increase of electron hopingin the B-sites For the same reasons it can be observed thatthe variation of loss tangent of the prepared samples withNi content has almost the same trend in inverse mannerFrom all these results it can be concluded that doping ofLi nanoferrites with Ni ions leads to improvement in theirdielectrical properties especially in the sample at 119909 = 06 andthese compositions make promising materials for microwaveapplications
The variation of dielectric constant (1205761015840) and dielectric losstangent (tan 120575) of prepared samples at 119909 = 04with frequencyat different temperatures has been investigated in Figure 7
It is observed that dielectric constant (1205761015840) of preparedsamples was decreased rapidly in the low frequency regionand decrease is quite slow in the high frequency regionthat is dielectric constant is almost independent of fre-quency (shown in Figure 7(a)) This dielectric behaviour offerrites was explained by Koopsrsquo theory [37] According tothis model dielectric medium is assumed to be made upof highly conducting grains surrounded by nonconductinggrain boundaries The grain boundaries are more effectiveat low frequencies and grains are more effective at thehigher frequencies As the grain boundaries having the largeresistance the charge carriers (electrons) pile up there andproduce large space charge polarisation which results in largevalue of dielectric constant at low frequency region Andfurther increasing the frequency the charge carriers (elec-trons) change their direction of motion due to the factthat this accumulation of charge at the grain boundarydecreases which results in the decrease of dielectric constantFrom the figures it is also observed that dielectric constantvalues increase with increase in the temperature in the lowfrequency region because electron exchange between the Fe+2and Fe+3 ions at octahedral sites was thermally activated
Physics Research International 9
15
30
45
60
75
90
105
120x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Log f (Hz)
(a)
00
02
04
06
08
10
12
14
16x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric lo
ss (t
an 120575)
Log f (Hz)
(b)
Figure 7 The variation of dielectric constant (1205761015840) and (tan 120575) with frequency at different temperatures of the LindashNi ferrite system at 119909 = 04
Figure 7(b) shows the variation dielectric loss tangent(tan 120575) with frequencies at different temperatures for 119909 = 04It is observed that the dielectric loss decreases with frequencybecause the jumping frequency of charge carriers cannot fol-low the frequency of the applied field after certain frequency
This figure also shows that the dielectric loss of the pre-pared samples increases with increasing the temperaturebecause of the enhanced hopping of thermally energized elec-trons
Figure 8 shows the variation of dielectric constant at75 kHz with temperature range 323Kndash723K for all ferritesamples It can be observed that the dielectric constant ofall the ferrite samples increases with increasing temperatureup to certain temperature after this temperature dielectricconstant of the prepared samples is going to decrease thattemperature is known as dielectric transition temperature119879119889[38] The decrease in the value of dielectric constant
takes place when the jumping frequency of the electronscannot follow the frequency of the applied electric field FromFigure 8 it is observed that dielectric transition temperature119879119889range is found to be in the 600Kndash680K for all prepared
samples of Li05minus05xNixFe25minus05xO4 system [39] It is also
observed that the slope variation in theArrhenius plots (otherthan Curie point) was in the same temperature range only forall samples
4 Conclusions
All the LindashNi ferrites samples prepared by low temperatureautocombustion method and single phase were confirmedthroughXRD analysisThe experimental results revealed thatthe lattice parameter X-ray density of the prepared ferrite
0
20
40
60
80
100
120
140
Temperature (K)
Data1 ln00Data1 LN02
Data1 LN04
Data1 LN06
Data1 LN08
Data1 LN10
300 400 500 600 700 800
120576998400times10
2
Figure 8 The variation of dielectric constant with temp forLi05minus05xNixFe25minus05xO4 nanoferrites
samples increases with increase in Ni-substituted concen-tration and the grain size is also in the nm range only DCelectrical resistivity of the prepared samples decreases withincreasing in the temperature which shows the semiconduct-ing behaviour of nanoferrites It is observed that the dis-continuity in the log(120590119879) versus 1000119879 graph shows Curiepoint of the prepared ferrite samples Curie temperature of
10 Physics Research International
the prepared LindashNi ferrites decreases with the increase ofthe Ni concentration The variation of DC conductivity withtemperature can be explained using the hopping mechanismof electrons between the Fe+2 and Fe+3 The dielectric con-stant of the prepared ferrite samples increases with increasein temperature up to certain temperature and afterwardsdecreases with increase in temperature
Conflict of Interests
The authors declare that there is no conflict of interestsregarding the publication of this paper
Acknowledgments
The authors are very grateful to Professor K Venu GopalReddy Head Department of Physics University College ofScience Osmania University Hyderabad The authors arevery thankful to UGC New Delhi for their financial assis-tance through Major Research Project (MRP)
References
[1] N S Gajbhiye and G Balaji ldquoMossbaur studies of nanosizeCuFe2O4ferritesrdquo in Advances in Nanoscience and Nano Tech
A Sharma Ed NISCAIR 2003[2] S A Jadhav ldquoMagnetic properties of Zn-substituted LindashCu
ferritesrdquo Journal of Magnetism andMagnetic Materials vol 224no 2 pp 167ndash172 2001
[3] M F Al-Hilli S Li and K S Kassim ldquoGadolinium substitutionand sintering temperature dependent electronic properties ofLindashNi ferriterdquo Journal ofMagnetism andMagneticMaterials vol324 pp 873ndash879 2012
[4] AM A El AtaM K El Nimr SM Attia D El Kony andAHAl-Hammadi ldquoStudies of AC electrical conductivity and initialmagnetic permeability of rare-earth-substituted LindashCo ferritesrdquoJournal of Magnetism andMagnetic Materials vol 297 no 1 pp33ndash43 2006
[5] AM A El Ata S M Attia D El Kony and A H Al-HammadildquoSpectral initial magnetic permeability and transport studies ofLi05minus05xCoxFe25minus05xO4 spinel ferriterdquo Journal ofMagnetism and
Magnetic Materials vol 295 no 1 pp 28ndash36 2005[6] S A Jadhav ldquoStructural and magnetic properties of Zn substi-
tuted LindashCu ferritesrdquo Materials Chemistry and Physics vol 65no 1 pp 120ndash123 2000
[7] H Kawazoe and K Ueda ldquoTransparent conducting oxidesbased on the spinel structurerdquo Journal of the American CeramicSociety vol 82 no 12 pp 3330ndash3336 1999
[8] P V Reddy and T S Rao ldquoX-ray studies on lithium-nickeland manganese-magnesiummixed ferritesrdquo Journal of the Less-Common Metals vol 75 no 2 pp 255ndash260 1980
[9] R S Devan Y D Kolekar and B K Chougule ldquoTransitionmetal-doped rare earth vanadates a regenerable catalytic mate-rial for SOFC anodesrdquo Journal of Physics CondensedMatter vol18 no 43 pp 9809ndash9821 2006
[10] M A Gabal and S S Ata-Allah ldquoEffect of diamagnetic substi-tution on the structural electrical and magnetic properties ofCoFe2O4rdquo Materials Chemistry and Physics vol 85 no 1 pp
104ndash112 2004
[11] E VeenaGopalan I A Al-Omari K AMalini et al ldquoImpact ofzinc substitution on the structural and magnetic properties ofchemically derived nanosized manganese zinc mixed ferritesrdquoJournal of Magnetism andMagnetic Materials vol 321 no 8 pp1092ndash1099 2009
[12] E Veena Gopalan K A Malini S Saravanan D Sakthi KumarY Yoshida and M R Anantharaman ldquoEvidence for polaronconduction in nanostructured manganese ferriterdquo Journal ofPhysics D Applied Physics vol 41 no 18 Article ID 1850052008
[13] M Srivastava S Chaubey andAKOjha ldquoInvestigation on sizedependent structural and magnetic behavior of nickel ferritenanoparticles prepared by sol-gel and hydrothermal methodsrdquoMaterials Chemistry and Physics vol 118 no 1 pp 174ndash1802009
[14] S S Bellad R B Pujar and B K Chougule ldquoStructural andmagnetic properties of some mixed LindashCd ferritesrdquo MaterialsChemistry and Physics vol 52 no 2 pp 166ndash169 1998
[15] D Ravinder ldquoDielectric behaviour of mixed lithium-zinc fer-ritesrdquo Journal of Materials Science Letters vol 11 no 22 pp1498ndash1500 1992
[16] Y Purushotham M B Reddy P Kishan D R Sagar and PV Reddy ldquoElectrical conductivity and thermopower studiesof titanium-substituted lithium-magnesium ferritesrdquoMaterialsLetters vol 17 no 6 pp 341ndash345 1993
[17] S A Mazen and T A Elmosalami ldquoStructural and elasticproperties of LindashNi ferritesrdquo ISRN Condensed Matter Physicsvol 2011 Article ID 820726 9 pages 2011
[18] S S Bhatu V K Lakhani A R Tanna et al ldquoEffect of nickelsubstitution on structural infrared and elastic properties oflithium ferriterdquo Indian Journal of Pure and Applied Physics vol45 no 7 pp 596ndash608 2007
[19] L Vijayan R Cheruku G Govindaraj and S Rajagopan ldquoIondynamics in combustion synthesized Na
3Cr2(PO4)3crystal-
litesrdquoMaterials Chemistry and Physics vol 125 no 1-2 pp 184ndash190 2011
[20] R Cheruku L Vijayan and G Govindaraj ldquoElectrical relax-ation studies of solution combustion synthesized nanocrys-talline Li
2NiZrO
4materialrdquo Materials Science and Engineering
B Solid-State Materials for Advanced Technology vol 177 no 11pp 771ndash779 2012
[21] L C Pathak T B Singh S Das A K Verma and P Ramachan-drarao ldquoEffect of pH on the combustion synthesis of nano-crystalline alumina powderrdquoMaterials Letters vol 57 no 2 pp380ndash385 2002
[22] J ChandradassM Balasubramanian andKHKim ldquoSynthesisand characterization of LaAlO
3nanopowders by various fuelsrdquo
Materials andManufacturing Processes vol 25 no 12 pp 1449ndash1453 2010
[23] J Jing L Liangchao and X Feng ldquoStructural analysis andmagnetic properties of Gd-doped LindashNi ferrites prepared usingrheological phase reaction methodrdquo Journal of Rare Earths vol25 no 1 pp 79ndash83 2007
[24] R G Kharabe R S Devan C M Kanamadi and B KChougule ldquoDielectric properties of mixed LindashNindashCd ferritesrdquoSmart Materials and Structures vol 15 no 2 pp N36ndashN392006
[25] F F Y Wang Treatise on Material Science and Technology vol2 Academic Press New York NY USA 1973
[26] R W Cahn Physical Mettaliurgy vol 1 North Holland Ams-terdam The Netherlands 1985
Physics Research International 11
[27] S B Patil R P Patil and B K Chougale ldquoDC electrical andthermo electric power measurement studies of NindashMgndashZnndashCoferritesrdquo Journal of Magnetism andMagnetic Materials vol 335pp 109ndash113 2013
[28] M A El Hiti ldquoStudies of structural electric andmagnetic prop-erties of some mixed ferritesrdquo Journal of Magnetism andMagnetic Materials vol 136 p 138 1994
[29] A N Patil R P Mahajan K K Patankar A K Ghatake andS A Patil ldquoMagnetic and Optical properties of conductionmechanism in Copper ferritesrdquo Indian Journal of Pure andApplied Physics vol 38 article 651 2000
[30] E J W Verwey and J H de Boer ldquoCation arrangement in afew oxides with crystal structures of the spinel typerdquo Recueildes Travaux Chimiques des Pays-Bas vol 55 no 6 pp 531ndash5401936
[31] A Verma T C Goel R GMendiratta and R G Gupta ldquoHigh-resistivity nickel-zinc ferrites by the citrate precursor methodrdquoJournal of Magnetism andMagneticMaterials vol 192 no 2 pp271ndash276 1999
[32] W D Kingery H K Bowen and P R Uhlum Introduction toCeramics Wiley New York NY USA 1975
[33] L L Hench and J K West Principles of Electronic CeramicsJohn Wiley amp Sons New York NY USA 1990
[34] S AMazen andH A Dawoud ldquoTemperature and compositiondependence of dielectric properties in LindashCu ferriterdquoMaterialsChemistry and Physics vol 82 no 3 pp 557ndash566 2003
[35] I Soibam S Phanjoubam H B Sharma H N K SarmaR Laishram and C Prakash ldquoEffects of Cobalt substitutionon the dielectric properties of LindashZn ferritesrdquo Solid StateCommunications vol 148 no 9-10 pp 399ndash402 2008
[36] S T Assar and H F Aboshiesha ldquoStructure and magneticproperties of CondashNindashLi ferrites synthesized by citrate precursormethodrdquo Journal ofMagnetism andMagneticMaterials vol 324no 22 pp 3846ndash3852 2012
[37] C G Koops ldquoOn the dispersion of resistivity and dielectricconstant of some semiconductors at audiofrequenciesrdquo PhysicalReview vol 83 article 121 1951
[38] K L Yadav andRN P Choudary ldquoStudy of structural electricaland optical properties of lead free based ceramic systemrdquoJournal of Materials Science Letters vol 19 p 61 1994
[39] V Verma V Pandey V N Shukla S Annapoorni and R KKotnala ldquoRemarkable influence on the dielectric and magneticproperties of lithium ferrite by Ti and Zn substitutionrdquo SolidState Communications vol 149 no 39-40 pp 1726ndash1730 2009
Submit your manuscripts athttpwwwhindawicom
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
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Superconductivity
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Physics Research International
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ThermodynamicsJournal of
2 Physics Research International
+Mixing and
stirring
Continuous stirring
Heating to
Grinding
Homogeneous solution of
metal nitratesCitric acid
pH 7 maintained byadding ammonia
Viscous gelDry gelAutocombustion
Burnt ash
GrindingCalcination at Nanoferrite
powder
and heating to 100∘C
200∘C
500∘C for 4hr
Figure 1 Schematic diagram representing preparation of nanoferrites
so forthTheDCelectrical conductivity of ferrites is one of theimportant properties which gives the valuable informationabout the conduction mechanism Moreover electrical con-ductivity has a significant effect on the dielectric polarizationin the spinel ferrites
Several methods are used for synthesizing nanosizedspinel ferrites such as coprecipitation sol-gel microemul-sion hydrothermal citrate gel and reverse micelle methods[11ndash13] In the preparation of lithium based ferrites low tem-perature sintering is needed to suppress lithium volatility andoxygen loss during sintering Many researchers proposed thecitrate gel method is a simple route to synthesize materials inthe nanocrystalline form due to lower sintering temperatureSeveral investigations on the properties of the LindashCd [14] LindashZn [15] and LindashMg [16] ferrites have been reported Mazenand Elmosalami [17] and Bhatu et al [18] have synthesizednickel substituted lithium ferrites by ceramic method withhigh sintering temperature However there are no detailreports on Ni substituted lithium nanoferrites prepared bycitrate gel autocombustion method with low sintering tem-perature
In the present study we report the synthesis of nickel sub-stituted lithium nanoferrites by nonconventional citrate gelautocombustion method XRD studies of prepared samplesSEM micrographs temperature dependent DC conductivitystudies and the dielectric properties of these ferrites from theroom temperature to 700K at various selected frequencies upto 5MHz have been studied
2 Experimental Techniques
Nanocrystalline nickel substituted lithium ferrites having thechemical formula Li
05minus05xNixFe25minus05xO4 (where 119909 = 00to 10 with step of 02) were synthesized using citrate gelautocombustion method This method has certain inherentadvantages like low processing temperature (200∘C) goodstoichiometric control and homogeneous distribution ofreactants and production of ultrafine particles with narrowsize distribution In this citrate gel autocombustion method
metal nitrates act as oxidizing agents and organic fuels asreducing agents [19 20] The various powder propertiescan be systematically tuned by altering the oxidant to fuelratios In present study fuel to oxidizing ratio was maintainedat unity The detailed synthesis process is represented inFigure 1
The stoichiometric amounts of ferric nitrate (Fe(NO3)2
9H2O) Nickel nitrate (Ni(NO
3)26H2O) lithium nitrate
(LiNO3) and citric acid (C
6H8O7sdotH2O) (all chemicals are
SD Fine-Chem Limited) were weighed and dissolved sep-arately in minimum amount of distilled water All the indi-vidual solutions were mixed together and then the ammoniasolutionwas slowly added to adjust the pH value at 7The pro-liferation of nitrate ions at low pH value is likely to decreasethe enthalpy of exothermic reaction by decreasing the fuelto oxidizing ratio Thus the rate of combustion reactiondecreases and particles agglomerate [21] so the pH value ofthe solution was maintained at 7 to avoid the agglomerationand preserve the stoichiometry The resultant solution waskept on a hot plate magnetic stirrer at 100∘C till gels wereformed after that increasing the temperature up to 200∘Cthe gels self-ignited in an autocombustion manner till wholecitrate complex was consumed to yield nanoferrite powdersThe as synthesized ferrite powders were annealed at 500∘C for4 hours in a muffle furnace [22]
The structural characterization of the synthesized sam-ples was carried out by Philips X-ray diffractometer (Model3710) using Cu K
120572radiation of wavelength 15405 A at room
temperature by continuous scanning in the range of Braggrsquosangles 5∘ to 80∘ in steps of 2∘min to investigate the phase andcrystalline size
The average crystalline size of the ferrites was determinedfrom the measured width of their diffraction pattern usingDebye Schererrsquos formula
119863 =
091120582
120573 cos 120579 (1)
where 120582 is the wavelength of the X-ray used for diffractionand 120573 is the full width half maximum (FWHM) in radians
Physics Research International 3
The lattice constant was calculated using the followingrelation
2119889 sin 120579 = 119899120582 (2)
where 119889 = 119886(ℎ2 + 1198962 + 1198972)12 for Fcc systemThe X-ray density (119889
119909) has been calculated according to
the relation
119889119909=
8119872
1198863119873
[gmcm3] (3)
where 119872 = molecular weight of the sample 119886 is the latticeparameter and119873 is the Avogadro number
The volume of the unit cell 119881 = 1198863The experimental density of the prepared sample was
calculated by Archimedesrsquo principle with xylene media usingfollowing relation
119889119864=
119908air119908air minus 119908xylene
times density of xylene (4)
where 119908air is weight of the sample in air 119908xylene is the weightof the sample in xylene
Porosity 119875 of the ferrite sample was then determined byemploying the relation
119875 = 119889119909minus
119889119864
119889119909
(5)
The powders of different compositions were pressed intodisc shaped pellets of 13mm diameter by applying a pressureof 25 times 108Nm2 Silver coating was done on adjacent facesof circular disc shaped pellets to have good ohmic contactand also tomake parallel plate capacitor geometrywith ferritematerial as a dielectric medium
The DC electrical conductivities of nanoferrite materialswere measured by two-probe technique in the temperaturerange 473ndash873K The measurements were recorded in thesteps of 10 K
The dielectric parameters like dielectric constant (1205761015840)and dielectric loss tangent (tan 120575) were measured usingAgilent E4986A precession LCR meter in the temperaturerange 313 Kndash723K at selected frequencies (75 kHz 30 kHz600 kHz 1MHz 3MHz and 5MHz) up to 5MHz frequency
The dielectric constant of prepared sample was calculatedusing the following relation
1205761015840=
119862119905
120576119900119860
(6)
where 119862 is the capacitance of the pellet 119905 is the thickness ofthe sample pellet 119860 is the cross section area of pellet and 120576
119900
is the free space permittivity
Inte
nsity
(AU
)
(440
)
(511
)(4
22)
(400
)
(311
)
(220
)
x = 10
x = 08
x = 06
x = 04
x = 02
x = 00
20 30 40 50 60 70 80
2120579 (deg)
Figure 2 XRD pattern of the Li05minus05xNixFe25minus05xO4 nanoferrites
3 Results and Discussion
31 Structural Analysis The structural study is essential foroptimizing the properties needed for various applicationsThe phase identification and lattice constant determinationof the prepared samples were performed on the X-ray diffrac-tion analysis The obtained XRD pattern of the nickel substi-tuted lithium nanoferrites samples having chemical formulaLi05minus05xNixFe25minus05xO4 (where 119909 = 00 to 10 with step of 02)
sintered at 500∘ for 4 hours was shown in Figure 2 The XRDpatterns of the calcined LindashNi nanoferrite powders (shown inFigure 2) confirm the formation of a single phase cubic spinelstructure with no extra impurity diffraction lines The strongdiffraction from the (220) (311) (400) (422) (511) and (440)planes confirms the pure spinel phase of the annealed ferrites[23 24]TheXRDpattern perfectlymatcheswith the standardpattern with JCPDS reference code 00-013-0207
The average crystallite size of the prepared nanoferritesamples was in the ranges from 39 to 49 nm for different dop-ing levels of the Ni+2 ions (Table 1) The lattice constant (119886) isfound to be increased with the increasing of the Ni+2 ion con-centration (Table 1) This is obvious because Ni+2 ions havethe larger ionic radii (078 A) than that of Li+1 ion (076 A)and Fe+3 ion (067 A) and obey Vegardrsquos law [25 26]The sub-stitution by the larger ions results in expansion of lattice Anincrease in the lattice parameterwhenLi and Fewere replacedby Ni as observed in the present work is therefore expectedThe observed deviation in the value of lattice parameter canbe attributed to the rearrangement of cations in the nanosizedLindashNi ferrites consequent to the sintering process
X-ray density values of the LindashNi nanoferrites wereincreased with increasing the Ni concentration becausemolecular weight of the samples increases with increasing theNi composition It is noted that X-ray density of each sample(119889119909) is greater than the corresponding bulk density (119889
119890)which
is an evidence of the presence of pores in the samplesThe surface morphology of the LindashNi nanoferrite parti-
cles sintered at 500∘C was examined by scanning electron
4 Physics Research International
Table 1 Crystalline size lattice parameter X-ray density bulk density and porosity of LindashNi nanoferrites obtained from XRD analysis
S No Composition Mol wt(gmmole)
Crystallitesize (nm)
Lattice parameter(A∘)
X-ray density (119889119909)
(gmcc)Expt density (119889
119890)
(gmcc) Porosity (119875)
1 Li05Fe25O4 207079 4190 8356 4713 4286 9012 Li04Ni02Fe24O4 212538 3954 8356 4839 4319 10703 Li03Ni04Fe23O4 217998 4535 8358 4957 4329 12664 Li02Ni06Fe22O4 223458 4990 8361 5076 4553 10315 Li01Ni08Fe21O4 228918 4130 8368 5206 4568 12226 NiFe2O4 234379 4301 8374 5334 4742 1107
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
(a)
x = 02 x = 04
(b)
Figure 3 (a) SEM images of the Li05minus05xNixFe25minus05xO4 nanoferrites (b) SEM images with grain size of the samples at 119909 = 02 and 119909 = 04
microscopy (SEM) shown in Figure 3(a) which indicatesthe agglomerated nanoparticles which is attributed to themagnetic exchange interaction between the nanoparticles Itis observed that the average grain size of the prepared samplesgoes on increasing on substitution of Ni in the place of Li andFe in ferrites The average grain size of all the prepared sam-ples directly calculated from SEM instrument is in the range
of 50ndash130 nm only The SEM images of samples 119909 = 02 and119909 = 04 with grain size were shown in Figure 3(b) and grainsize of remaining samples is also in the same range (the figuresare not shown)
32 Electrical Properties The DC electrical conductivity ofthe prepared samples was measured by two-probe method
Physics Research International 5
Table 2 Electrical resistivity and activation energies of the Li05minus05119909
Ni119909Fe25minus05119909
O4system
S No Composition Resistivity(Ω-cm) Curie temp (∘C) 119864
119886in paramagneticregion (eV)
119864119886in Ferromagneticregion (eV)
1 Li05Fe25O4 921 times 108 mdash mdash mdash2 Li04Ni02Fe24O4 917 times 108 567 161 0823 Li03Ni04Fe23O4 573 times 108 560 127 0934 Li02Ni06Fe22O4 273 times 108 540 095 0835 Li01Ni08Fe21O4 124 times 107 535 090 0736 NiFe2O4 682 times 107 528 081 071
in the temperature range from 473K to 873K The ferritesample is pressed into circular pellets The measurementswere recorded in the steps of 10 K
The temperature dependence of the prepared ferritesconductivity is plotted in accordance with the followingArrhenius type equation
log120590 = log120590119900minus
119864119886
119870119861119879
(7)
where 120590 is the conductivity 120590119900is the conductivity at abso-
lute temperature 119870119861is Boltzmannrsquos constant and 119879 is the
temperature The phenomenon of phase transition cationmigration cation reordering the presence of impurities andmagnetotransport effects are considered to be responsible forthe temperature dependence on the electrical conductivity ofthe prepared ferrite samples
The variations of the electrical conductivity (log120590119879) withinverse of temperature (1000119879) were shown in Figure 4Theconductivity of the ferrite samples increases with increasingthe temperatureThat is temperature increases and resistivityof the ferrites was decreased indicating the semiconductingbehaviour All the plots (except pure lithium ferrites) of elec-trical conductivity (log120590119879) versus 1000119879 yield a change inslope at a particular temperatureThis change in slope occurswhile crossing the Curie temperature (the temperature atwhich the ferromagnetic material changed to paramagnetic)The discontinuity at the Curie temperature was attributedto the magnetic transition from well-ordered ferromagneticstate to disordered paramagnetic state which involves differ-ent activation energies The values of the electrical resistivityand thermal activation energies of the prepared samples atferromagnetic region and paramagnetic region were given inTable 2
It is observed that the activation energy in the ferromag-netic region is smaller than the paramagnetic region this isdue to the effect of spin disordering
Someworkers have reported three regions of conductivity[26ndash29] of which the first region has been attributed to thepresence of impurities second region was due to the phasetransition from tetragonal structure to cubic structure andthe third one was due to the ferromagnetic to paramag-netic change The electrical conductivity of ferrites can beexplained on the basis of the Verwey and de Boer mechanism[30] which involves the exchange of charge carriers thatis electrons between the ions of the same element that are
present in more than one valence state (Fe+2 Fe+3) dis-tributed randomly over the crystallographic lattice sites TheFe+2 ion concentration is a characteristic property of nanofer-rites and it depends on several factors such as sintering tem-peraturetime and atmosphere and annealing time includingthe grain structure Some amount of Fe+2 ions is also formeddue to possible evaporation of Li ions during the sintering[28] Sintering of lithium ferrites is therefore carried out atrelatively lower temperature (500∘C) in order to avoid lithiumloss during sintering
The variation of DC electrical resistivity at 200∘C withNi composition in the Li ferrites is given in Table 2 The DCresistivity of the all the samples was observed to be in therange 124 times 107ndash921 times 108Ω-cm Compositionally decreasein the DC resistivity of LindashNi ferrites with increasing theNi concentration was observed The overall higher valuesof resistivity obtained for the ferrites can be attributed tothe small grain size and better compositional stoichiometrywith reduced Fe+2 formation as a result of low temperatureprocessing by the citrate gel method [31 32]
33 Dielectric Properties The dielectric constant and DCelectrical resistivity of ferrites are very important parametersfrom the application point of view These two parametersare electrical properties and exchange of electrons betweenthe Fe+2 and Fe+3 ions is responsible for these mechanismswhich results in local displacement of charges responsible forthe polarisation in ferrites The dielectric constant (1205761015840) anddielectric loss tangent (tan 120575) were found to be dependenton the variation of external factors such as temperature andfrequencyThe variation of dielectric constant (1205761015840) and dielec-tric loss tangent (tan 120575) with respect to selected frequenciesand temperature in the range of 300K to 700K has beeninvestigated
The variation of dielectric constant (1205761015840) and dielectricloss tangent (tan 120575) for all prepared ferrite samples withtemperature has been studied at different frequencies asshown in Figures 5(a) and 5(b)
It is observed that the dielectric constant (1205761015840) and dielec-tric loss tangent (tan 120575) of prepared samples were increasedwith increase in temperature for all selected frequencies Theincrease in temperature of the sample thermally activates thecharge carrier increasing the electron exchange interactionwhich results in increasing the dielectric constant values of
6 Physics Research International
minus5
minus4
minus3
minus2
minus1
0
1
minus5
minus4
minus3
minus2
minus1
0
1
2
minus5
minus4
minus3
minus2
minus1
0
1
minus4
minus3
minus2
minus1
0
1
minus25
minus20
minus15
minus10
minus05
00
05
10
15
minus30
minus25
minus20
minus15
minus10
minus05
00
05
10
15
x = 00 x = 02
x = 04 x = 06
x = 08 x = 10
161 eV
082 eV
127 eV
093 eV
095 eV
083 eV
090 eV
073 eV
081 ev
071 eV
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
Figure 4 Arrhenius plots for electrical conductivities of Li05minus05xNixFe25minus05xO4 nanoferrites
Physics Research International 7
510152025303540
Temperature (K)
5
10
15
20
25
30
0
20
40
60
80
100
120
020406080
100120140
0
20
40
60
80
100
020406080
100120140
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
75 kHz
75 kHz75 kHz 75 kHz
75 kHz
75 kHz
30kHz
30kHz30kHz 30kHz
30kHz
30kHz600kHz
600kHz600kHz
600kHz
600kHz
600kHz1MHz
1MHz1MHz
1MHz
1MHz
1MHz3MHz
3MHz 3MHz3MHz
3MHz
3MHz5MHz
5MHz5MHz
5MHz
5MHz
5MHz
300 400 500 600 700 800
Temperature (K) Temperature (K)300 400 500 600 700 800 300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
(a)
minus0100010203040506070809
Temperature (K)
0005101520253035
minus02000204060810121416
minus02000204060810121416
0002040608101214161820
minus0200020406081012
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
750Hz
750Hz 750Hz
750Hz
750Hz 750Hz
3kHz
3kHz3kHz
3kHz
3kHz
3kHz
100 kHz
100 kHz100 kHz
100 kHz
100 kHz
100 kHz
1MHz
1MHz1MHz
1MHz
1MHz
1MHz
3MHz
3MHz3MHz
3MHz
3MHz
3MHz
5MHz
5MHz
5MHz
5MHz
5MHz
5MHz
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 5 (a)Variation of dielectric constant (1205761015840)with temperature at different frequencies of Li05minus05xNixFe25minus05xO4 nanoferrites (b)Variation
of loss tangent (tan 120575) with temperature at different frequencies of Li05minus05xNixFe25minus05xO4 nanoferrites
the ferrites It is observed that there are four major con-tributions for polarisation in ferrites They are electronicatomic dipolar and interfacial polarisations [33] Electronicand atomic polarisations are important at high frequenciesand are independent of temperature while remaining two are
important at lower frequencies and dependent on tempera-ture By increasing the temperature interfacial polarisationis increased and dipolar polarisation decreases The increasein dielectric constant with increase in temperature at lowfrequency may be due to the interfacial polarisation
8 Physics Research International
6
7
8
9
10
11
12
13
14
Ni composition
750Hz and 323K
Die
lect
ric co
nsta
nt (120576
998400 )times10
2
00 02 04 06 08 10
(a)
000
002
004
006
008
010 750Hz and 323K
Ni composition00 02 04 06 08 10
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 6 Variation of dielectric constant (1205761015840) and tan 120575 with Ni concentration
From Figure 5(a) it can be noticed that the dielectricconstant (1205761015840) values increase rapidly in the low temperaturerange (119879 lt 600K) whereas in the high temperaturerange (119879 gt 600K) dielectric constant (1205761015840) reaches a stablevalue (Resonance peak) after that it starts to decrease withincreasing the temperature For the low temperature range(119879 lt 600K) the polarisation is increased by the electricfield and also by increasing the number of charge carriers(electrons) which are increased with temperature hence theincrease in the dielectric constant (1205761015840) at low temperaturerange (119879 lt 600K) is due to increase in both temperatureand frequency For the high temperature range (119879 gt 600K)the saturation in the generation of charge carriers is reachedTherefore the electron exchange between the ions of the sameelement that are present in more than one valence state (Fe+2Fe+3 orNi+2 Ni+1) cannot follow the field variation and hencedielectric constant decreases [34] The temperature at whichthe resonance peak appeared is observed to be shifted towardsthe higher temperature as the frequency is increased [35]The variation of loss angle tangent (tan 120575) of the preparedsample as a function temperature at different frequencies hasalso been investigated and an increase is observed just as thedielectric constant (1205761015840) curve This variation of loss tangentwith temperature curve can be understood on the basis ofDebyersquos equation for loss given as [33]
The compositional dependence (Ni concentration) of thedielectric constant (1205761015840) and dielectric loss tangent (tan 120575) ofprepared samples at 323K and at 75 kHz is shown in Figure 6It can be observed that the dielectric constant (1205761015840) value ofthe prepared samples was increased from 119909 = 00 to 119909 =06 and then decreased It can be attributed to the effect ofsimultaneous contributions of different factors such as grainsize density porosity and cation distribution The initialincrease in dielectric constant (1205761015840) when Ni content increasesfrom 119909 = 00 to 119909 = 06 coincides with the increase ofgrain size from Table 1 [36] After that the cation distribution
becomes the predominant factor in decreasing the dielectricconstant (1205761015840) with Ni content since the decrease of holehoping becomes greater than the increase of electron hopingin the B-sites For the same reasons it can be observed thatthe variation of loss tangent of the prepared samples withNi content has almost the same trend in inverse mannerFrom all these results it can be concluded that doping ofLi nanoferrites with Ni ions leads to improvement in theirdielectrical properties especially in the sample at 119909 = 06 andthese compositions make promising materials for microwaveapplications
The variation of dielectric constant (1205761015840) and dielectric losstangent (tan 120575) of prepared samples at 119909 = 04with frequencyat different temperatures has been investigated in Figure 7
It is observed that dielectric constant (1205761015840) of preparedsamples was decreased rapidly in the low frequency regionand decrease is quite slow in the high frequency regionthat is dielectric constant is almost independent of fre-quency (shown in Figure 7(a)) This dielectric behaviour offerrites was explained by Koopsrsquo theory [37] According tothis model dielectric medium is assumed to be made upof highly conducting grains surrounded by nonconductinggrain boundaries The grain boundaries are more effectiveat low frequencies and grains are more effective at thehigher frequencies As the grain boundaries having the largeresistance the charge carriers (electrons) pile up there andproduce large space charge polarisation which results in largevalue of dielectric constant at low frequency region Andfurther increasing the frequency the charge carriers (elec-trons) change their direction of motion due to the factthat this accumulation of charge at the grain boundarydecreases which results in the decrease of dielectric constantFrom the figures it is also observed that dielectric constantvalues increase with increase in the temperature in the lowfrequency region because electron exchange between the Fe+2and Fe+3 ions at octahedral sites was thermally activated
Physics Research International 9
15
30
45
60
75
90
105
120x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Log f (Hz)
(a)
00
02
04
06
08
10
12
14
16x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric lo
ss (t
an 120575)
Log f (Hz)
(b)
Figure 7 The variation of dielectric constant (1205761015840) and (tan 120575) with frequency at different temperatures of the LindashNi ferrite system at 119909 = 04
Figure 7(b) shows the variation dielectric loss tangent(tan 120575) with frequencies at different temperatures for 119909 = 04It is observed that the dielectric loss decreases with frequencybecause the jumping frequency of charge carriers cannot fol-low the frequency of the applied field after certain frequency
This figure also shows that the dielectric loss of the pre-pared samples increases with increasing the temperaturebecause of the enhanced hopping of thermally energized elec-trons
Figure 8 shows the variation of dielectric constant at75 kHz with temperature range 323Kndash723K for all ferritesamples It can be observed that the dielectric constant ofall the ferrite samples increases with increasing temperatureup to certain temperature after this temperature dielectricconstant of the prepared samples is going to decrease thattemperature is known as dielectric transition temperature119879119889[38] The decrease in the value of dielectric constant
takes place when the jumping frequency of the electronscannot follow the frequency of the applied electric field FromFigure 8 it is observed that dielectric transition temperature119879119889range is found to be in the 600Kndash680K for all prepared
samples of Li05minus05xNixFe25minus05xO4 system [39] It is also
observed that the slope variation in theArrhenius plots (otherthan Curie point) was in the same temperature range only forall samples
4 Conclusions
All the LindashNi ferrites samples prepared by low temperatureautocombustion method and single phase were confirmedthroughXRD analysisThe experimental results revealed thatthe lattice parameter X-ray density of the prepared ferrite
0
20
40
60
80
100
120
140
Temperature (K)
Data1 ln00Data1 LN02
Data1 LN04
Data1 LN06
Data1 LN08
Data1 LN10
300 400 500 600 700 800
120576998400times10
2
Figure 8 The variation of dielectric constant with temp forLi05minus05xNixFe25minus05xO4 nanoferrites
samples increases with increase in Ni-substituted concen-tration and the grain size is also in the nm range only DCelectrical resistivity of the prepared samples decreases withincreasing in the temperature which shows the semiconduct-ing behaviour of nanoferrites It is observed that the dis-continuity in the log(120590119879) versus 1000119879 graph shows Curiepoint of the prepared ferrite samples Curie temperature of
10 Physics Research International
the prepared LindashNi ferrites decreases with the increase ofthe Ni concentration The variation of DC conductivity withtemperature can be explained using the hopping mechanismof electrons between the Fe+2 and Fe+3 The dielectric con-stant of the prepared ferrite samples increases with increasein temperature up to certain temperature and afterwardsdecreases with increase in temperature
Conflict of Interests
The authors declare that there is no conflict of interestsregarding the publication of this paper
Acknowledgments
The authors are very grateful to Professor K Venu GopalReddy Head Department of Physics University College ofScience Osmania University Hyderabad The authors arevery thankful to UGC New Delhi for their financial assis-tance through Major Research Project (MRP)
References
[1] N S Gajbhiye and G Balaji ldquoMossbaur studies of nanosizeCuFe2O4ferritesrdquo in Advances in Nanoscience and Nano Tech
A Sharma Ed NISCAIR 2003[2] S A Jadhav ldquoMagnetic properties of Zn-substituted LindashCu
ferritesrdquo Journal of Magnetism andMagnetic Materials vol 224no 2 pp 167ndash172 2001
[3] M F Al-Hilli S Li and K S Kassim ldquoGadolinium substitutionand sintering temperature dependent electronic properties ofLindashNi ferriterdquo Journal ofMagnetism andMagneticMaterials vol324 pp 873ndash879 2012
[4] AM A El AtaM K El Nimr SM Attia D El Kony andAHAl-Hammadi ldquoStudies of AC electrical conductivity and initialmagnetic permeability of rare-earth-substituted LindashCo ferritesrdquoJournal of Magnetism andMagnetic Materials vol 297 no 1 pp33ndash43 2006
[5] AM A El Ata S M Attia D El Kony and A H Al-HammadildquoSpectral initial magnetic permeability and transport studies ofLi05minus05xCoxFe25minus05xO4 spinel ferriterdquo Journal ofMagnetism and
Magnetic Materials vol 295 no 1 pp 28ndash36 2005[6] S A Jadhav ldquoStructural and magnetic properties of Zn substi-
tuted LindashCu ferritesrdquo Materials Chemistry and Physics vol 65no 1 pp 120ndash123 2000
[7] H Kawazoe and K Ueda ldquoTransparent conducting oxidesbased on the spinel structurerdquo Journal of the American CeramicSociety vol 82 no 12 pp 3330ndash3336 1999
[8] P V Reddy and T S Rao ldquoX-ray studies on lithium-nickeland manganese-magnesiummixed ferritesrdquo Journal of the Less-Common Metals vol 75 no 2 pp 255ndash260 1980
[9] R S Devan Y D Kolekar and B K Chougule ldquoTransitionmetal-doped rare earth vanadates a regenerable catalytic mate-rial for SOFC anodesrdquo Journal of Physics CondensedMatter vol18 no 43 pp 9809ndash9821 2006
[10] M A Gabal and S S Ata-Allah ldquoEffect of diamagnetic substi-tution on the structural electrical and magnetic properties ofCoFe2O4rdquo Materials Chemistry and Physics vol 85 no 1 pp
104ndash112 2004
[11] E VeenaGopalan I A Al-Omari K AMalini et al ldquoImpact ofzinc substitution on the structural and magnetic properties ofchemically derived nanosized manganese zinc mixed ferritesrdquoJournal of Magnetism andMagnetic Materials vol 321 no 8 pp1092ndash1099 2009
[12] E Veena Gopalan K A Malini S Saravanan D Sakthi KumarY Yoshida and M R Anantharaman ldquoEvidence for polaronconduction in nanostructured manganese ferriterdquo Journal ofPhysics D Applied Physics vol 41 no 18 Article ID 1850052008
[13] M Srivastava S Chaubey andAKOjha ldquoInvestigation on sizedependent structural and magnetic behavior of nickel ferritenanoparticles prepared by sol-gel and hydrothermal methodsrdquoMaterials Chemistry and Physics vol 118 no 1 pp 174ndash1802009
[14] S S Bellad R B Pujar and B K Chougule ldquoStructural andmagnetic properties of some mixed LindashCd ferritesrdquo MaterialsChemistry and Physics vol 52 no 2 pp 166ndash169 1998
[15] D Ravinder ldquoDielectric behaviour of mixed lithium-zinc fer-ritesrdquo Journal of Materials Science Letters vol 11 no 22 pp1498ndash1500 1992
[16] Y Purushotham M B Reddy P Kishan D R Sagar and PV Reddy ldquoElectrical conductivity and thermopower studiesof titanium-substituted lithium-magnesium ferritesrdquoMaterialsLetters vol 17 no 6 pp 341ndash345 1993
[17] S A Mazen and T A Elmosalami ldquoStructural and elasticproperties of LindashNi ferritesrdquo ISRN Condensed Matter Physicsvol 2011 Article ID 820726 9 pages 2011
[18] S S Bhatu V K Lakhani A R Tanna et al ldquoEffect of nickelsubstitution on structural infrared and elastic properties oflithium ferriterdquo Indian Journal of Pure and Applied Physics vol45 no 7 pp 596ndash608 2007
[19] L Vijayan R Cheruku G Govindaraj and S Rajagopan ldquoIondynamics in combustion synthesized Na
3Cr2(PO4)3crystal-
litesrdquoMaterials Chemistry and Physics vol 125 no 1-2 pp 184ndash190 2011
[20] R Cheruku L Vijayan and G Govindaraj ldquoElectrical relax-ation studies of solution combustion synthesized nanocrys-talline Li
2NiZrO
4materialrdquo Materials Science and Engineering
B Solid-State Materials for Advanced Technology vol 177 no 11pp 771ndash779 2012
[21] L C Pathak T B Singh S Das A K Verma and P Ramachan-drarao ldquoEffect of pH on the combustion synthesis of nano-crystalline alumina powderrdquoMaterials Letters vol 57 no 2 pp380ndash385 2002
[22] J ChandradassM Balasubramanian andKHKim ldquoSynthesisand characterization of LaAlO
3nanopowders by various fuelsrdquo
Materials andManufacturing Processes vol 25 no 12 pp 1449ndash1453 2010
[23] J Jing L Liangchao and X Feng ldquoStructural analysis andmagnetic properties of Gd-doped LindashNi ferrites prepared usingrheological phase reaction methodrdquo Journal of Rare Earths vol25 no 1 pp 79ndash83 2007
[24] R G Kharabe R S Devan C M Kanamadi and B KChougule ldquoDielectric properties of mixed LindashNindashCd ferritesrdquoSmart Materials and Structures vol 15 no 2 pp N36ndashN392006
[25] F F Y Wang Treatise on Material Science and Technology vol2 Academic Press New York NY USA 1973
[26] R W Cahn Physical Mettaliurgy vol 1 North Holland Ams-terdam The Netherlands 1985
Physics Research International 11
[27] S B Patil R P Patil and B K Chougale ldquoDC electrical andthermo electric power measurement studies of NindashMgndashZnndashCoferritesrdquo Journal of Magnetism andMagnetic Materials vol 335pp 109ndash113 2013
[28] M A El Hiti ldquoStudies of structural electric andmagnetic prop-erties of some mixed ferritesrdquo Journal of Magnetism andMagnetic Materials vol 136 p 138 1994
[29] A N Patil R P Mahajan K K Patankar A K Ghatake andS A Patil ldquoMagnetic and Optical properties of conductionmechanism in Copper ferritesrdquo Indian Journal of Pure andApplied Physics vol 38 article 651 2000
[30] E J W Verwey and J H de Boer ldquoCation arrangement in afew oxides with crystal structures of the spinel typerdquo Recueildes Travaux Chimiques des Pays-Bas vol 55 no 6 pp 531ndash5401936
[31] A Verma T C Goel R GMendiratta and R G Gupta ldquoHigh-resistivity nickel-zinc ferrites by the citrate precursor methodrdquoJournal of Magnetism andMagneticMaterials vol 192 no 2 pp271ndash276 1999
[32] W D Kingery H K Bowen and P R Uhlum Introduction toCeramics Wiley New York NY USA 1975
[33] L L Hench and J K West Principles of Electronic CeramicsJohn Wiley amp Sons New York NY USA 1990
[34] S AMazen andH A Dawoud ldquoTemperature and compositiondependence of dielectric properties in LindashCu ferriterdquoMaterialsChemistry and Physics vol 82 no 3 pp 557ndash566 2003
[35] I Soibam S Phanjoubam H B Sharma H N K SarmaR Laishram and C Prakash ldquoEffects of Cobalt substitutionon the dielectric properties of LindashZn ferritesrdquo Solid StateCommunications vol 148 no 9-10 pp 399ndash402 2008
[36] S T Assar and H F Aboshiesha ldquoStructure and magneticproperties of CondashNindashLi ferrites synthesized by citrate precursormethodrdquo Journal ofMagnetism andMagneticMaterials vol 324no 22 pp 3846ndash3852 2012
[37] C G Koops ldquoOn the dispersion of resistivity and dielectricconstant of some semiconductors at audiofrequenciesrdquo PhysicalReview vol 83 article 121 1951
[38] K L Yadav andRN P Choudary ldquoStudy of structural electricaland optical properties of lead free based ceramic systemrdquoJournal of Materials Science Letters vol 19 p 61 1994
[39] V Verma V Pandey V N Shukla S Annapoorni and R KKotnala ldquoRemarkable influence on the dielectric and magneticproperties of lithium ferrite by Ti and Zn substitutionrdquo SolidState Communications vol 149 no 39-40 pp 1726ndash1730 2009
Submit your manuscripts athttpwwwhindawicom
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
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FluidsJournal of
Atomic and Molecular Physics
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Advances in Condensed Matter Physics
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Superconductivity
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Physics Research International
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ThermodynamicsJournal of
Physics Research International 3
The lattice constant was calculated using the followingrelation
2119889 sin 120579 = 119899120582 (2)
where 119889 = 119886(ℎ2 + 1198962 + 1198972)12 for Fcc systemThe X-ray density (119889
119909) has been calculated according to
the relation
119889119909=
8119872
1198863119873
[gmcm3] (3)
where 119872 = molecular weight of the sample 119886 is the latticeparameter and119873 is the Avogadro number
The volume of the unit cell 119881 = 1198863The experimental density of the prepared sample was
calculated by Archimedesrsquo principle with xylene media usingfollowing relation
119889119864=
119908air119908air minus 119908xylene
times density of xylene (4)
where 119908air is weight of the sample in air 119908xylene is the weightof the sample in xylene
Porosity 119875 of the ferrite sample was then determined byemploying the relation
119875 = 119889119909minus
119889119864
119889119909
(5)
The powders of different compositions were pressed intodisc shaped pellets of 13mm diameter by applying a pressureof 25 times 108Nm2 Silver coating was done on adjacent facesof circular disc shaped pellets to have good ohmic contactand also tomake parallel plate capacitor geometrywith ferritematerial as a dielectric medium
The DC electrical conductivities of nanoferrite materialswere measured by two-probe technique in the temperaturerange 473ndash873K The measurements were recorded in thesteps of 10 K
The dielectric parameters like dielectric constant (1205761015840)and dielectric loss tangent (tan 120575) were measured usingAgilent E4986A precession LCR meter in the temperaturerange 313 Kndash723K at selected frequencies (75 kHz 30 kHz600 kHz 1MHz 3MHz and 5MHz) up to 5MHz frequency
The dielectric constant of prepared sample was calculatedusing the following relation
1205761015840=
119862119905
120576119900119860
(6)
where 119862 is the capacitance of the pellet 119905 is the thickness ofthe sample pellet 119860 is the cross section area of pellet and 120576
119900
is the free space permittivity
Inte
nsity
(AU
)
(440
)
(511
)(4
22)
(400
)
(311
)
(220
)
x = 10
x = 08
x = 06
x = 04
x = 02
x = 00
20 30 40 50 60 70 80
2120579 (deg)
Figure 2 XRD pattern of the Li05minus05xNixFe25minus05xO4 nanoferrites
3 Results and Discussion
31 Structural Analysis The structural study is essential foroptimizing the properties needed for various applicationsThe phase identification and lattice constant determinationof the prepared samples were performed on the X-ray diffrac-tion analysis The obtained XRD pattern of the nickel substi-tuted lithium nanoferrites samples having chemical formulaLi05minus05xNixFe25minus05xO4 (where 119909 = 00 to 10 with step of 02)
sintered at 500∘ for 4 hours was shown in Figure 2 The XRDpatterns of the calcined LindashNi nanoferrite powders (shown inFigure 2) confirm the formation of a single phase cubic spinelstructure with no extra impurity diffraction lines The strongdiffraction from the (220) (311) (400) (422) (511) and (440)planes confirms the pure spinel phase of the annealed ferrites[23 24]TheXRDpattern perfectlymatcheswith the standardpattern with JCPDS reference code 00-013-0207
The average crystallite size of the prepared nanoferritesamples was in the ranges from 39 to 49 nm for different dop-ing levels of the Ni+2 ions (Table 1) The lattice constant (119886) isfound to be increased with the increasing of the Ni+2 ion con-centration (Table 1) This is obvious because Ni+2 ions havethe larger ionic radii (078 A) than that of Li+1 ion (076 A)and Fe+3 ion (067 A) and obey Vegardrsquos law [25 26]The sub-stitution by the larger ions results in expansion of lattice Anincrease in the lattice parameterwhenLi and Fewere replacedby Ni as observed in the present work is therefore expectedThe observed deviation in the value of lattice parameter canbe attributed to the rearrangement of cations in the nanosizedLindashNi ferrites consequent to the sintering process
X-ray density values of the LindashNi nanoferrites wereincreased with increasing the Ni concentration becausemolecular weight of the samples increases with increasing theNi composition It is noted that X-ray density of each sample(119889119909) is greater than the corresponding bulk density (119889
119890)which
is an evidence of the presence of pores in the samplesThe surface morphology of the LindashNi nanoferrite parti-
cles sintered at 500∘C was examined by scanning electron
4 Physics Research International
Table 1 Crystalline size lattice parameter X-ray density bulk density and porosity of LindashNi nanoferrites obtained from XRD analysis
S No Composition Mol wt(gmmole)
Crystallitesize (nm)
Lattice parameter(A∘)
X-ray density (119889119909)
(gmcc)Expt density (119889
119890)
(gmcc) Porosity (119875)
1 Li05Fe25O4 207079 4190 8356 4713 4286 9012 Li04Ni02Fe24O4 212538 3954 8356 4839 4319 10703 Li03Ni04Fe23O4 217998 4535 8358 4957 4329 12664 Li02Ni06Fe22O4 223458 4990 8361 5076 4553 10315 Li01Ni08Fe21O4 228918 4130 8368 5206 4568 12226 NiFe2O4 234379 4301 8374 5334 4742 1107
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
(a)
x = 02 x = 04
(b)
Figure 3 (a) SEM images of the Li05minus05xNixFe25minus05xO4 nanoferrites (b) SEM images with grain size of the samples at 119909 = 02 and 119909 = 04
microscopy (SEM) shown in Figure 3(a) which indicatesthe agglomerated nanoparticles which is attributed to themagnetic exchange interaction between the nanoparticles Itis observed that the average grain size of the prepared samplesgoes on increasing on substitution of Ni in the place of Li andFe in ferrites The average grain size of all the prepared sam-ples directly calculated from SEM instrument is in the range
of 50ndash130 nm only The SEM images of samples 119909 = 02 and119909 = 04 with grain size were shown in Figure 3(b) and grainsize of remaining samples is also in the same range (the figuresare not shown)
32 Electrical Properties The DC electrical conductivity ofthe prepared samples was measured by two-probe method
Physics Research International 5
Table 2 Electrical resistivity and activation energies of the Li05minus05119909
Ni119909Fe25minus05119909
O4system
S No Composition Resistivity(Ω-cm) Curie temp (∘C) 119864
119886in paramagneticregion (eV)
119864119886in Ferromagneticregion (eV)
1 Li05Fe25O4 921 times 108 mdash mdash mdash2 Li04Ni02Fe24O4 917 times 108 567 161 0823 Li03Ni04Fe23O4 573 times 108 560 127 0934 Li02Ni06Fe22O4 273 times 108 540 095 0835 Li01Ni08Fe21O4 124 times 107 535 090 0736 NiFe2O4 682 times 107 528 081 071
in the temperature range from 473K to 873K The ferritesample is pressed into circular pellets The measurementswere recorded in the steps of 10 K
The temperature dependence of the prepared ferritesconductivity is plotted in accordance with the followingArrhenius type equation
log120590 = log120590119900minus
119864119886
119870119861119879
(7)
where 120590 is the conductivity 120590119900is the conductivity at abso-
lute temperature 119870119861is Boltzmannrsquos constant and 119879 is the
temperature The phenomenon of phase transition cationmigration cation reordering the presence of impurities andmagnetotransport effects are considered to be responsible forthe temperature dependence on the electrical conductivity ofthe prepared ferrite samples
The variations of the electrical conductivity (log120590119879) withinverse of temperature (1000119879) were shown in Figure 4Theconductivity of the ferrite samples increases with increasingthe temperatureThat is temperature increases and resistivityof the ferrites was decreased indicating the semiconductingbehaviour All the plots (except pure lithium ferrites) of elec-trical conductivity (log120590119879) versus 1000119879 yield a change inslope at a particular temperatureThis change in slope occurswhile crossing the Curie temperature (the temperature atwhich the ferromagnetic material changed to paramagnetic)The discontinuity at the Curie temperature was attributedto the magnetic transition from well-ordered ferromagneticstate to disordered paramagnetic state which involves differ-ent activation energies The values of the electrical resistivityand thermal activation energies of the prepared samples atferromagnetic region and paramagnetic region were given inTable 2
It is observed that the activation energy in the ferromag-netic region is smaller than the paramagnetic region this isdue to the effect of spin disordering
Someworkers have reported three regions of conductivity[26ndash29] of which the first region has been attributed to thepresence of impurities second region was due to the phasetransition from tetragonal structure to cubic structure andthe third one was due to the ferromagnetic to paramag-netic change The electrical conductivity of ferrites can beexplained on the basis of the Verwey and de Boer mechanism[30] which involves the exchange of charge carriers thatis electrons between the ions of the same element that are
present in more than one valence state (Fe+2 Fe+3) dis-tributed randomly over the crystallographic lattice sites TheFe+2 ion concentration is a characteristic property of nanofer-rites and it depends on several factors such as sintering tem-peraturetime and atmosphere and annealing time includingthe grain structure Some amount of Fe+2 ions is also formeddue to possible evaporation of Li ions during the sintering[28] Sintering of lithium ferrites is therefore carried out atrelatively lower temperature (500∘C) in order to avoid lithiumloss during sintering
The variation of DC electrical resistivity at 200∘C withNi composition in the Li ferrites is given in Table 2 The DCresistivity of the all the samples was observed to be in therange 124 times 107ndash921 times 108Ω-cm Compositionally decreasein the DC resistivity of LindashNi ferrites with increasing theNi concentration was observed The overall higher valuesof resistivity obtained for the ferrites can be attributed tothe small grain size and better compositional stoichiometrywith reduced Fe+2 formation as a result of low temperatureprocessing by the citrate gel method [31 32]
33 Dielectric Properties The dielectric constant and DCelectrical resistivity of ferrites are very important parametersfrom the application point of view These two parametersare electrical properties and exchange of electrons betweenthe Fe+2 and Fe+3 ions is responsible for these mechanismswhich results in local displacement of charges responsible forthe polarisation in ferrites The dielectric constant (1205761015840) anddielectric loss tangent (tan 120575) were found to be dependenton the variation of external factors such as temperature andfrequencyThe variation of dielectric constant (1205761015840) and dielec-tric loss tangent (tan 120575) with respect to selected frequenciesand temperature in the range of 300K to 700K has beeninvestigated
The variation of dielectric constant (1205761015840) and dielectricloss tangent (tan 120575) for all prepared ferrite samples withtemperature has been studied at different frequencies asshown in Figures 5(a) and 5(b)
It is observed that the dielectric constant (1205761015840) and dielec-tric loss tangent (tan 120575) of prepared samples were increasedwith increase in temperature for all selected frequencies Theincrease in temperature of the sample thermally activates thecharge carrier increasing the electron exchange interactionwhich results in increasing the dielectric constant values of
6 Physics Research International
minus5
minus4
minus3
minus2
minus1
0
1
minus5
minus4
minus3
minus2
minus1
0
1
2
minus5
minus4
minus3
minus2
minus1
0
1
minus4
minus3
minus2
minus1
0
1
minus25
minus20
minus15
minus10
minus05
00
05
10
15
minus30
minus25
minus20
minus15
minus10
minus05
00
05
10
15
x = 00 x = 02
x = 04 x = 06
x = 08 x = 10
161 eV
082 eV
127 eV
093 eV
095 eV
083 eV
090 eV
073 eV
081 ev
071 eV
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
Figure 4 Arrhenius plots for electrical conductivities of Li05minus05xNixFe25minus05xO4 nanoferrites
Physics Research International 7
510152025303540
Temperature (K)
5
10
15
20
25
30
0
20
40
60
80
100
120
020406080
100120140
0
20
40
60
80
100
020406080
100120140
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
75 kHz
75 kHz75 kHz 75 kHz
75 kHz
75 kHz
30kHz
30kHz30kHz 30kHz
30kHz
30kHz600kHz
600kHz600kHz
600kHz
600kHz
600kHz1MHz
1MHz1MHz
1MHz
1MHz
1MHz3MHz
3MHz 3MHz3MHz
3MHz
3MHz5MHz
5MHz5MHz
5MHz
5MHz
5MHz
300 400 500 600 700 800
Temperature (K) Temperature (K)300 400 500 600 700 800 300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
(a)
minus0100010203040506070809
Temperature (K)
0005101520253035
minus02000204060810121416
minus02000204060810121416
0002040608101214161820
minus0200020406081012
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
750Hz
750Hz 750Hz
750Hz
750Hz 750Hz
3kHz
3kHz3kHz
3kHz
3kHz
3kHz
100 kHz
100 kHz100 kHz
100 kHz
100 kHz
100 kHz
1MHz
1MHz1MHz
1MHz
1MHz
1MHz
3MHz
3MHz3MHz
3MHz
3MHz
3MHz
5MHz
5MHz
5MHz
5MHz
5MHz
5MHz
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 5 (a)Variation of dielectric constant (1205761015840)with temperature at different frequencies of Li05minus05xNixFe25minus05xO4 nanoferrites (b)Variation
of loss tangent (tan 120575) with temperature at different frequencies of Li05minus05xNixFe25minus05xO4 nanoferrites
the ferrites It is observed that there are four major con-tributions for polarisation in ferrites They are electronicatomic dipolar and interfacial polarisations [33] Electronicand atomic polarisations are important at high frequenciesand are independent of temperature while remaining two are
important at lower frequencies and dependent on tempera-ture By increasing the temperature interfacial polarisationis increased and dipolar polarisation decreases The increasein dielectric constant with increase in temperature at lowfrequency may be due to the interfacial polarisation
8 Physics Research International
6
7
8
9
10
11
12
13
14
Ni composition
750Hz and 323K
Die
lect
ric co
nsta
nt (120576
998400 )times10
2
00 02 04 06 08 10
(a)
000
002
004
006
008
010 750Hz and 323K
Ni composition00 02 04 06 08 10
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 6 Variation of dielectric constant (1205761015840) and tan 120575 with Ni concentration
From Figure 5(a) it can be noticed that the dielectricconstant (1205761015840) values increase rapidly in the low temperaturerange (119879 lt 600K) whereas in the high temperaturerange (119879 gt 600K) dielectric constant (1205761015840) reaches a stablevalue (Resonance peak) after that it starts to decrease withincreasing the temperature For the low temperature range(119879 lt 600K) the polarisation is increased by the electricfield and also by increasing the number of charge carriers(electrons) which are increased with temperature hence theincrease in the dielectric constant (1205761015840) at low temperaturerange (119879 lt 600K) is due to increase in both temperatureand frequency For the high temperature range (119879 gt 600K)the saturation in the generation of charge carriers is reachedTherefore the electron exchange between the ions of the sameelement that are present in more than one valence state (Fe+2Fe+3 orNi+2 Ni+1) cannot follow the field variation and hencedielectric constant decreases [34] The temperature at whichthe resonance peak appeared is observed to be shifted towardsthe higher temperature as the frequency is increased [35]The variation of loss angle tangent (tan 120575) of the preparedsample as a function temperature at different frequencies hasalso been investigated and an increase is observed just as thedielectric constant (1205761015840) curve This variation of loss tangentwith temperature curve can be understood on the basis ofDebyersquos equation for loss given as [33]
The compositional dependence (Ni concentration) of thedielectric constant (1205761015840) and dielectric loss tangent (tan 120575) ofprepared samples at 323K and at 75 kHz is shown in Figure 6It can be observed that the dielectric constant (1205761015840) value ofthe prepared samples was increased from 119909 = 00 to 119909 =06 and then decreased It can be attributed to the effect ofsimultaneous contributions of different factors such as grainsize density porosity and cation distribution The initialincrease in dielectric constant (1205761015840) when Ni content increasesfrom 119909 = 00 to 119909 = 06 coincides with the increase ofgrain size from Table 1 [36] After that the cation distribution
becomes the predominant factor in decreasing the dielectricconstant (1205761015840) with Ni content since the decrease of holehoping becomes greater than the increase of electron hopingin the B-sites For the same reasons it can be observed thatthe variation of loss tangent of the prepared samples withNi content has almost the same trend in inverse mannerFrom all these results it can be concluded that doping ofLi nanoferrites with Ni ions leads to improvement in theirdielectrical properties especially in the sample at 119909 = 06 andthese compositions make promising materials for microwaveapplications
The variation of dielectric constant (1205761015840) and dielectric losstangent (tan 120575) of prepared samples at 119909 = 04with frequencyat different temperatures has been investigated in Figure 7
It is observed that dielectric constant (1205761015840) of preparedsamples was decreased rapidly in the low frequency regionand decrease is quite slow in the high frequency regionthat is dielectric constant is almost independent of fre-quency (shown in Figure 7(a)) This dielectric behaviour offerrites was explained by Koopsrsquo theory [37] According tothis model dielectric medium is assumed to be made upof highly conducting grains surrounded by nonconductinggrain boundaries The grain boundaries are more effectiveat low frequencies and grains are more effective at thehigher frequencies As the grain boundaries having the largeresistance the charge carriers (electrons) pile up there andproduce large space charge polarisation which results in largevalue of dielectric constant at low frequency region Andfurther increasing the frequency the charge carriers (elec-trons) change their direction of motion due to the factthat this accumulation of charge at the grain boundarydecreases which results in the decrease of dielectric constantFrom the figures it is also observed that dielectric constantvalues increase with increase in the temperature in the lowfrequency region because electron exchange between the Fe+2and Fe+3 ions at octahedral sites was thermally activated
Physics Research International 9
15
30
45
60
75
90
105
120x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Log f (Hz)
(a)
00
02
04
06
08
10
12
14
16x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric lo
ss (t
an 120575)
Log f (Hz)
(b)
Figure 7 The variation of dielectric constant (1205761015840) and (tan 120575) with frequency at different temperatures of the LindashNi ferrite system at 119909 = 04
Figure 7(b) shows the variation dielectric loss tangent(tan 120575) with frequencies at different temperatures for 119909 = 04It is observed that the dielectric loss decreases with frequencybecause the jumping frequency of charge carriers cannot fol-low the frequency of the applied field after certain frequency
This figure also shows that the dielectric loss of the pre-pared samples increases with increasing the temperaturebecause of the enhanced hopping of thermally energized elec-trons
Figure 8 shows the variation of dielectric constant at75 kHz with temperature range 323Kndash723K for all ferritesamples It can be observed that the dielectric constant ofall the ferrite samples increases with increasing temperatureup to certain temperature after this temperature dielectricconstant of the prepared samples is going to decrease thattemperature is known as dielectric transition temperature119879119889[38] The decrease in the value of dielectric constant
takes place when the jumping frequency of the electronscannot follow the frequency of the applied electric field FromFigure 8 it is observed that dielectric transition temperature119879119889range is found to be in the 600Kndash680K for all prepared
samples of Li05minus05xNixFe25minus05xO4 system [39] It is also
observed that the slope variation in theArrhenius plots (otherthan Curie point) was in the same temperature range only forall samples
4 Conclusions
All the LindashNi ferrites samples prepared by low temperatureautocombustion method and single phase were confirmedthroughXRD analysisThe experimental results revealed thatthe lattice parameter X-ray density of the prepared ferrite
0
20
40
60
80
100
120
140
Temperature (K)
Data1 ln00Data1 LN02
Data1 LN04
Data1 LN06
Data1 LN08
Data1 LN10
300 400 500 600 700 800
120576998400times10
2
Figure 8 The variation of dielectric constant with temp forLi05minus05xNixFe25minus05xO4 nanoferrites
samples increases with increase in Ni-substituted concen-tration and the grain size is also in the nm range only DCelectrical resistivity of the prepared samples decreases withincreasing in the temperature which shows the semiconduct-ing behaviour of nanoferrites It is observed that the dis-continuity in the log(120590119879) versus 1000119879 graph shows Curiepoint of the prepared ferrite samples Curie temperature of
10 Physics Research International
the prepared LindashNi ferrites decreases with the increase ofthe Ni concentration The variation of DC conductivity withtemperature can be explained using the hopping mechanismof electrons between the Fe+2 and Fe+3 The dielectric con-stant of the prepared ferrite samples increases with increasein temperature up to certain temperature and afterwardsdecreases with increase in temperature
Conflict of Interests
The authors declare that there is no conflict of interestsregarding the publication of this paper
Acknowledgments
The authors are very grateful to Professor K Venu GopalReddy Head Department of Physics University College ofScience Osmania University Hyderabad The authors arevery thankful to UGC New Delhi for their financial assis-tance through Major Research Project (MRP)
References
[1] N S Gajbhiye and G Balaji ldquoMossbaur studies of nanosizeCuFe2O4ferritesrdquo in Advances in Nanoscience and Nano Tech
A Sharma Ed NISCAIR 2003[2] S A Jadhav ldquoMagnetic properties of Zn-substituted LindashCu
ferritesrdquo Journal of Magnetism andMagnetic Materials vol 224no 2 pp 167ndash172 2001
[3] M F Al-Hilli S Li and K S Kassim ldquoGadolinium substitutionand sintering temperature dependent electronic properties ofLindashNi ferriterdquo Journal ofMagnetism andMagneticMaterials vol324 pp 873ndash879 2012
[4] AM A El AtaM K El Nimr SM Attia D El Kony andAHAl-Hammadi ldquoStudies of AC electrical conductivity and initialmagnetic permeability of rare-earth-substituted LindashCo ferritesrdquoJournal of Magnetism andMagnetic Materials vol 297 no 1 pp33ndash43 2006
[5] AM A El Ata S M Attia D El Kony and A H Al-HammadildquoSpectral initial magnetic permeability and transport studies ofLi05minus05xCoxFe25minus05xO4 spinel ferriterdquo Journal ofMagnetism and
Magnetic Materials vol 295 no 1 pp 28ndash36 2005[6] S A Jadhav ldquoStructural and magnetic properties of Zn substi-
tuted LindashCu ferritesrdquo Materials Chemistry and Physics vol 65no 1 pp 120ndash123 2000
[7] H Kawazoe and K Ueda ldquoTransparent conducting oxidesbased on the spinel structurerdquo Journal of the American CeramicSociety vol 82 no 12 pp 3330ndash3336 1999
[8] P V Reddy and T S Rao ldquoX-ray studies on lithium-nickeland manganese-magnesiummixed ferritesrdquo Journal of the Less-Common Metals vol 75 no 2 pp 255ndash260 1980
[9] R S Devan Y D Kolekar and B K Chougule ldquoTransitionmetal-doped rare earth vanadates a regenerable catalytic mate-rial for SOFC anodesrdquo Journal of Physics CondensedMatter vol18 no 43 pp 9809ndash9821 2006
[10] M A Gabal and S S Ata-Allah ldquoEffect of diamagnetic substi-tution on the structural electrical and magnetic properties ofCoFe2O4rdquo Materials Chemistry and Physics vol 85 no 1 pp
104ndash112 2004
[11] E VeenaGopalan I A Al-Omari K AMalini et al ldquoImpact ofzinc substitution on the structural and magnetic properties ofchemically derived nanosized manganese zinc mixed ferritesrdquoJournal of Magnetism andMagnetic Materials vol 321 no 8 pp1092ndash1099 2009
[12] E Veena Gopalan K A Malini S Saravanan D Sakthi KumarY Yoshida and M R Anantharaman ldquoEvidence for polaronconduction in nanostructured manganese ferriterdquo Journal ofPhysics D Applied Physics vol 41 no 18 Article ID 1850052008
[13] M Srivastava S Chaubey andAKOjha ldquoInvestigation on sizedependent structural and magnetic behavior of nickel ferritenanoparticles prepared by sol-gel and hydrothermal methodsrdquoMaterials Chemistry and Physics vol 118 no 1 pp 174ndash1802009
[14] S S Bellad R B Pujar and B K Chougule ldquoStructural andmagnetic properties of some mixed LindashCd ferritesrdquo MaterialsChemistry and Physics vol 52 no 2 pp 166ndash169 1998
[15] D Ravinder ldquoDielectric behaviour of mixed lithium-zinc fer-ritesrdquo Journal of Materials Science Letters vol 11 no 22 pp1498ndash1500 1992
[16] Y Purushotham M B Reddy P Kishan D R Sagar and PV Reddy ldquoElectrical conductivity and thermopower studiesof titanium-substituted lithium-magnesium ferritesrdquoMaterialsLetters vol 17 no 6 pp 341ndash345 1993
[17] S A Mazen and T A Elmosalami ldquoStructural and elasticproperties of LindashNi ferritesrdquo ISRN Condensed Matter Physicsvol 2011 Article ID 820726 9 pages 2011
[18] S S Bhatu V K Lakhani A R Tanna et al ldquoEffect of nickelsubstitution on structural infrared and elastic properties oflithium ferriterdquo Indian Journal of Pure and Applied Physics vol45 no 7 pp 596ndash608 2007
[19] L Vijayan R Cheruku G Govindaraj and S Rajagopan ldquoIondynamics in combustion synthesized Na
3Cr2(PO4)3crystal-
litesrdquoMaterials Chemistry and Physics vol 125 no 1-2 pp 184ndash190 2011
[20] R Cheruku L Vijayan and G Govindaraj ldquoElectrical relax-ation studies of solution combustion synthesized nanocrys-talline Li
2NiZrO
4materialrdquo Materials Science and Engineering
B Solid-State Materials for Advanced Technology vol 177 no 11pp 771ndash779 2012
[21] L C Pathak T B Singh S Das A K Verma and P Ramachan-drarao ldquoEffect of pH on the combustion synthesis of nano-crystalline alumina powderrdquoMaterials Letters vol 57 no 2 pp380ndash385 2002
[22] J ChandradassM Balasubramanian andKHKim ldquoSynthesisand characterization of LaAlO
3nanopowders by various fuelsrdquo
Materials andManufacturing Processes vol 25 no 12 pp 1449ndash1453 2010
[23] J Jing L Liangchao and X Feng ldquoStructural analysis andmagnetic properties of Gd-doped LindashNi ferrites prepared usingrheological phase reaction methodrdquo Journal of Rare Earths vol25 no 1 pp 79ndash83 2007
[24] R G Kharabe R S Devan C M Kanamadi and B KChougule ldquoDielectric properties of mixed LindashNindashCd ferritesrdquoSmart Materials and Structures vol 15 no 2 pp N36ndashN392006
[25] F F Y Wang Treatise on Material Science and Technology vol2 Academic Press New York NY USA 1973
[26] R W Cahn Physical Mettaliurgy vol 1 North Holland Ams-terdam The Netherlands 1985
Physics Research International 11
[27] S B Patil R P Patil and B K Chougale ldquoDC electrical andthermo electric power measurement studies of NindashMgndashZnndashCoferritesrdquo Journal of Magnetism andMagnetic Materials vol 335pp 109ndash113 2013
[28] M A El Hiti ldquoStudies of structural electric andmagnetic prop-erties of some mixed ferritesrdquo Journal of Magnetism andMagnetic Materials vol 136 p 138 1994
[29] A N Patil R P Mahajan K K Patankar A K Ghatake andS A Patil ldquoMagnetic and Optical properties of conductionmechanism in Copper ferritesrdquo Indian Journal of Pure andApplied Physics vol 38 article 651 2000
[30] E J W Verwey and J H de Boer ldquoCation arrangement in afew oxides with crystal structures of the spinel typerdquo Recueildes Travaux Chimiques des Pays-Bas vol 55 no 6 pp 531ndash5401936
[31] A Verma T C Goel R GMendiratta and R G Gupta ldquoHigh-resistivity nickel-zinc ferrites by the citrate precursor methodrdquoJournal of Magnetism andMagneticMaterials vol 192 no 2 pp271ndash276 1999
[32] W D Kingery H K Bowen and P R Uhlum Introduction toCeramics Wiley New York NY USA 1975
[33] L L Hench and J K West Principles of Electronic CeramicsJohn Wiley amp Sons New York NY USA 1990
[34] S AMazen andH A Dawoud ldquoTemperature and compositiondependence of dielectric properties in LindashCu ferriterdquoMaterialsChemistry and Physics vol 82 no 3 pp 557ndash566 2003
[35] I Soibam S Phanjoubam H B Sharma H N K SarmaR Laishram and C Prakash ldquoEffects of Cobalt substitutionon the dielectric properties of LindashZn ferritesrdquo Solid StateCommunications vol 148 no 9-10 pp 399ndash402 2008
[36] S T Assar and H F Aboshiesha ldquoStructure and magneticproperties of CondashNindashLi ferrites synthesized by citrate precursormethodrdquo Journal ofMagnetism andMagneticMaterials vol 324no 22 pp 3846ndash3852 2012
[37] C G Koops ldquoOn the dispersion of resistivity and dielectricconstant of some semiconductors at audiofrequenciesrdquo PhysicalReview vol 83 article 121 1951
[38] K L Yadav andRN P Choudary ldquoStudy of structural electricaland optical properties of lead free based ceramic systemrdquoJournal of Materials Science Letters vol 19 p 61 1994
[39] V Verma V Pandey V N Shukla S Annapoorni and R KKotnala ldquoRemarkable influence on the dielectric and magneticproperties of lithium ferrite by Ti and Zn substitutionrdquo SolidState Communications vol 149 no 39-40 pp 1726ndash1730 2009
Submit your manuscripts athttpwwwhindawicom
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Superconductivity
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Physics Research International
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ThermodynamicsJournal of
4 Physics Research International
Table 1 Crystalline size lattice parameter X-ray density bulk density and porosity of LindashNi nanoferrites obtained from XRD analysis
S No Composition Mol wt(gmmole)
Crystallitesize (nm)
Lattice parameter(A∘)
X-ray density (119889119909)
(gmcc)Expt density (119889
119890)
(gmcc) Porosity (119875)
1 Li05Fe25O4 207079 4190 8356 4713 4286 9012 Li04Ni02Fe24O4 212538 3954 8356 4839 4319 10703 Li03Ni04Fe23O4 217998 4535 8358 4957 4329 12664 Li02Ni06Fe22O4 223458 4990 8361 5076 4553 10315 Li01Ni08Fe21O4 228918 4130 8368 5206 4568 12226 NiFe2O4 234379 4301 8374 5334 4742 1107
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
(a)
x = 02 x = 04
(b)
Figure 3 (a) SEM images of the Li05minus05xNixFe25minus05xO4 nanoferrites (b) SEM images with grain size of the samples at 119909 = 02 and 119909 = 04
microscopy (SEM) shown in Figure 3(a) which indicatesthe agglomerated nanoparticles which is attributed to themagnetic exchange interaction between the nanoparticles Itis observed that the average grain size of the prepared samplesgoes on increasing on substitution of Ni in the place of Li andFe in ferrites The average grain size of all the prepared sam-ples directly calculated from SEM instrument is in the range
of 50ndash130 nm only The SEM images of samples 119909 = 02 and119909 = 04 with grain size were shown in Figure 3(b) and grainsize of remaining samples is also in the same range (the figuresare not shown)
32 Electrical Properties The DC electrical conductivity ofthe prepared samples was measured by two-probe method
Physics Research International 5
Table 2 Electrical resistivity and activation energies of the Li05minus05119909
Ni119909Fe25minus05119909
O4system
S No Composition Resistivity(Ω-cm) Curie temp (∘C) 119864
119886in paramagneticregion (eV)
119864119886in Ferromagneticregion (eV)
1 Li05Fe25O4 921 times 108 mdash mdash mdash2 Li04Ni02Fe24O4 917 times 108 567 161 0823 Li03Ni04Fe23O4 573 times 108 560 127 0934 Li02Ni06Fe22O4 273 times 108 540 095 0835 Li01Ni08Fe21O4 124 times 107 535 090 0736 NiFe2O4 682 times 107 528 081 071
in the temperature range from 473K to 873K The ferritesample is pressed into circular pellets The measurementswere recorded in the steps of 10 K
The temperature dependence of the prepared ferritesconductivity is plotted in accordance with the followingArrhenius type equation
log120590 = log120590119900minus
119864119886
119870119861119879
(7)
where 120590 is the conductivity 120590119900is the conductivity at abso-
lute temperature 119870119861is Boltzmannrsquos constant and 119879 is the
temperature The phenomenon of phase transition cationmigration cation reordering the presence of impurities andmagnetotransport effects are considered to be responsible forthe temperature dependence on the electrical conductivity ofthe prepared ferrite samples
The variations of the electrical conductivity (log120590119879) withinverse of temperature (1000119879) were shown in Figure 4Theconductivity of the ferrite samples increases with increasingthe temperatureThat is temperature increases and resistivityof the ferrites was decreased indicating the semiconductingbehaviour All the plots (except pure lithium ferrites) of elec-trical conductivity (log120590119879) versus 1000119879 yield a change inslope at a particular temperatureThis change in slope occurswhile crossing the Curie temperature (the temperature atwhich the ferromagnetic material changed to paramagnetic)The discontinuity at the Curie temperature was attributedto the magnetic transition from well-ordered ferromagneticstate to disordered paramagnetic state which involves differ-ent activation energies The values of the electrical resistivityand thermal activation energies of the prepared samples atferromagnetic region and paramagnetic region were given inTable 2
It is observed that the activation energy in the ferromag-netic region is smaller than the paramagnetic region this isdue to the effect of spin disordering
Someworkers have reported three regions of conductivity[26ndash29] of which the first region has been attributed to thepresence of impurities second region was due to the phasetransition from tetragonal structure to cubic structure andthe third one was due to the ferromagnetic to paramag-netic change The electrical conductivity of ferrites can beexplained on the basis of the Verwey and de Boer mechanism[30] which involves the exchange of charge carriers thatis electrons between the ions of the same element that are
present in more than one valence state (Fe+2 Fe+3) dis-tributed randomly over the crystallographic lattice sites TheFe+2 ion concentration is a characteristic property of nanofer-rites and it depends on several factors such as sintering tem-peraturetime and atmosphere and annealing time includingthe grain structure Some amount of Fe+2 ions is also formeddue to possible evaporation of Li ions during the sintering[28] Sintering of lithium ferrites is therefore carried out atrelatively lower temperature (500∘C) in order to avoid lithiumloss during sintering
The variation of DC electrical resistivity at 200∘C withNi composition in the Li ferrites is given in Table 2 The DCresistivity of the all the samples was observed to be in therange 124 times 107ndash921 times 108Ω-cm Compositionally decreasein the DC resistivity of LindashNi ferrites with increasing theNi concentration was observed The overall higher valuesof resistivity obtained for the ferrites can be attributed tothe small grain size and better compositional stoichiometrywith reduced Fe+2 formation as a result of low temperatureprocessing by the citrate gel method [31 32]
33 Dielectric Properties The dielectric constant and DCelectrical resistivity of ferrites are very important parametersfrom the application point of view These two parametersare electrical properties and exchange of electrons betweenthe Fe+2 and Fe+3 ions is responsible for these mechanismswhich results in local displacement of charges responsible forthe polarisation in ferrites The dielectric constant (1205761015840) anddielectric loss tangent (tan 120575) were found to be dependenton the variation of external factors such as temperature andfrequencyThe variation of dielectric constant (1205761015840) and dielec-tric loss tangent (tan 120575) with respect to selected frequenciesand temperature in the range of 300K to 700K has beeninvestigated
The variation of dielectric constant (1205761015840) and dielectricloss tangent (tan 120575) for all prepared ferrite samples withtemperature has been studied at different frequencies asshown in Figures 5(a) and 5(b)
It is observed that the dielectric constant (1205761015840) and dielec-tric loss tangent (tan 120575) of prepared samples were increasedwith increase in temperature for all selected frequencies Theincrease in temperature of the sample thermally activates thecharge carrier increasing the electron exchange interactionwhich results in increasing the dielectric constant values of
6 Physics Research International
minus5
minus4
minus3
minus2
minus1
0
1
minus5
minus4
minus3
minus2
minus1
0
1
2
minus5
minus4
minus3
minus2
minus1
0
1
minus4
minus3
minus2
minus1
0
1
minus25
minus20
minus15
minus10
minus05
00
05
10
15
minus30
minus25
minus20
minus15
minus10
minus05
00
05
10
15
x = 00 x = 02
x = 04 x = 06
x = 08 x = 10
161 eV
082 eV
127 eV
093 eV
095 eV
083 eV
090 eV
073 eV
081 ev
071 eV
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
Figure 4 Arrhenius plots for electrical conductivities of Li05minus05xNixFe25minus05xO4 nanoferrites
Physics Research International 7
510152025303540
Temperature (K)
5
10
15
20
25
30
0
20
40
60
80
100
120
020406080
100120140
0
20
40
60
80
100
020406080
100120140
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
75 kHz
75 kHz75 kHz 75 kHz
75 kHz
75 kHz
30kHz
30kHz30kHz 30kHz
30kHz
30kHz600kHz
600kHz600kHz
600kHz
600kHz
600kHz1MHz
1MHz1MHz
1MHz
1MHz
1MHz3MHz
3MHz 3MHz3MHz
3MHz
3MHz5MHz
5MHz5MHz
5MHz
5MHz
5MHz
300 400 500 600 700 800
Temperature (K) Temperature (K)300 400 500 600 700 800 300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
(a)
minus0100010203040506070809
Temperature (K)
0005101520253035
minus02000204060810121416
minus02000204060810121416
0002040608101214161820
minus0200020406081012
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
750Hz
750Hz 750Hz
750Hz
750Hz 750Hz
3kHz
3kHz3kHz
3kHz
3kHz
3kHz
100 kHz
100 kHz100 kHz
100 kHz
100 kHz
100 kHz
1MHz
1MHz1MHz
1MHz
1MHz
1MHz
3MHz
3MHz3MHz
3MHz
3MHz
3MHz
5MHz
5MHz
5MHz
5MHz
5MHz
5MHz
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 5 (a)Variation of dielectric constant (1205761015840)with temperature at different frequencies of Li05minus05xNixFe25minus05xO4 nanoferrites (b)Variation
of loss tangent (tan 120575) with temperature at different frequencies of Li05minus05xNixFe25minus05xO4 nanoferrites
the ferrites It is observed that there are four major con-tributions for polarisation in ferrites They are electronicatomic dipolar and interfacial polarisations [33] Electronicand atomic polarisations are important at high frequenciesand are independent of temperature while remaining two are
important at lower frequencies and dependent on tempera-ture By increasing the temperature interfacial polarisationis increased and dipolar polarisation decreases The increasein dielectric constant with increase in temperature at lowfrequency may be due to the interfacial polarisation
8 Physics Research International
6
7
8
9
10
11
12
13
14
Ni composition
750Hz and 323K
Die
lect
ric co
nsta
nt (120576
998400 )times10
2
00 02 04 06 08 10
(a)
000
002
004
006
008
010 750Hz and 323K
Ni composition00 02 04 06 08 10
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 6 Variation of dielectric constant (1205761015840) and tan 120575 with Ni concentration
From Figure 5(a) it can be noticed that the dielectricconstant (1205761015840) values increase rapidly in the low temperaturerange (119879 lt 600K) whereas in the high temperaturerange (119879 gt 600K) dielectric constant (1205761015840) reaches a stablevalue (Resonance peak) after that it starts to decrease withincreasing the temperature For the low temperature range(119879 lt 600K) the polarisation is increased by the electricfield and also by increasing the number of charge carriers(electrons) which are increased with temperature hence theincrease in the dielectric constant (1205761015840) at low temperaturerange (119879 lt 600K) is due to increase in both temperatureand frequency For the high temperature range (119879 gt 600K)the saturation in the generation of charge carriers is reachedTherefore the electron exchange between the ions of the sameelement that are present in more than one valence state (Fe+2Fe+3 orNi+2 Ni+1) cannot follow the field variation and hencedielectric constant decreases [34] The temperature at whichthe resonance peak appeared is observed to be shifted towardsthe higher temperature as the frequency is increased [35]The variation of loss angle tangent (tan 120575) of the preparedsample as a function temperature at different frequencies hasalso been investigated and an increase is observed just as thedielectric constant (1205761015840) curve This variation of loss tangentwith temperature curve can be understood on the basis ofDebyersquos equation for loss given as [33]
The compositional dependence (Ni concentration) of thedielectric constant (1205761015840) and dielectric loss tangent (tan 120575) ofprepared samples at 323K and at 75 kHz is shown in Figure 6It can be observed that the dielectric constant (1205761015840) value ofthe prepared samples was increased from 119909 = 00 to 119909 =06 and then decreased It can be attributed to the effect ofsimultaneous contributions of different factors such as grainsize density porosity and cation distribution The initialincrease in dielectric constant (1205761015840) when Ni content increasesfrom 119909 = 00 to 119909 = 06 coincides with the increase ofgrain size from Table 1 [36] After that the cation distribution
becomes the predominant factor in decreasing the dielectricconstant (1205761015840) with Ni content since the decrease of holehoping becomes greater than the increase of electron hopingin the B-sites For the same reasons it can be observed thatthe variation of loss tangent of the prepared samples withNi content has almost the same trend in inverse mannerFrom all these results it can be concluded that doping ofLi nanoferrites with Ni ions leads to improvement in theirdielectrical properties especially in the sample at 119909 = 06 andthese compositions make promising materials for microwaveapplications
The variation of dielectric constant (1205761015840) and dielectric losstangent (tan 120575) of prepared samples at 119909 = 04with frequencyat different temperatures has been investigated in Figure 7
It is observed that dielectric constant (1205761015840) of preparedsamples was decreased rapidly in the low frequency regionand decrease is quite slow in the high frequency regionthat is dielectric constant is almost independent of fre-quency (shown in Figure 7(a)) This dielectric behaviour offerrites was explained by Koopsrsquo theory [37] According tothis model dielectric medium is assumed to be made upof highly conducting grains surrounded by nonconductinggrain boundaries The grain boundaries are more effectiveat low frequencies and grains are more effective at thehigher frequencies As the grain boundaries having the largeresistance the charge carriers (electrons) pile up there andproduce large space charge polarisation which results in largevalue of dielectric constant at low frequency region Andfurther increasing the frequency the charge carriers (elec-trons) change their direction of motion due to the factthat this accumulation of charge at the grain boundarydecreases which results in the decrease of dielectric constantFrom the figures it is also observed that dielectric constantvalues increase with increase in the temperature in the lowfrequency region because electron exchange between the Fe+2and Fe+3 ions at octahedral sites was thermally activated
Physics Research International 9
15
30
45
60
75
90
105
120x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Log f (Hz)
(a)
00
02
04
06
08
10
12
14
16x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric lo
ss (t
an 120575)
Log f (Hz)
(b)
Figure 7 The variation of dielectric constant (1205761015840) and (tan 120575) with frequency at different temperatures of the LindashNi ferrite system at 119909 = 04
Figure 7(b) shows the variation dielectric loss tangent(tan 120575) with frequencies at different temperatures for 119909 = 04It is observed that the dielectric loss decreases with frequencybecause the jumping frequency of charge carriers cannot fol-low the frequency of the applied field after certain frequency
This figure also shows that the dielectric loss of the pre-pared samples increases with increasing the temperaturebecause of the enhanced hopping of thermally energized elec-trons
Figure 8 shows the variation of dielectric constant at75 kHz with temperature range 323Kndash723K for all ferritesamples It can be observed that the dielectric constant ofall the ferrite samples increases with increasing temperatureup to certain temperature after this temperature dielectricconstant of the prepared samples is going to decrease thattemperature is known as dielectric transition temperature119879119889[38] The decrease in the value of dielectric constant
takes place when the jumping frequency of the electronscannot follow the frequency of the applied electric field FromFigure 8 it is observed that dielectric transition temperature119879119889range is found to be in the 600Kndash680K for all prepared
samples of Li05minus05xNixFe25minus05xO4 system [39] It is also
observed that the slope variation in theArrhenius plots (otherthan Curie point) was in the same temperature range only forall samples
4 Conclusions
All the LindashNi ferrites samples prepared by low temperatureautocombustion method and single phase were confirmedthroughXRD analysisThe experimental results revealed thatthe lattice parameter X-ray density of the prepared ferrite
0
20
40
60
80
100
120
140
Temperature (K)
Data1 ln00Data1 LN02
Data1 LN04
Data1 LN06
Data1 LN08
Data1 LN10
300 400 500 600 700 800
120576998400times10
2
Figure 8 The variation of dielectric constant with temp forLi05minus05xNixFe25minus05xO4 nanoferrites
samples increases with increase in Ni-substituted concen-tration and the grain size is also in the nm range only DCelectrical resistivity of the prepared samples decreases withincreasing in the temperature which shows the semiconduct-ing behaviour of nanoferrites It is observed that the dis-continuity in the log(120590119879) versus 1000119879 graph shows Curiepoint of the prepared ferrite samples Curie temperature of
10 Physics Research International
the prepared LindashNi ferrites decreases with the increase ofthe Ni concentration The variation of DC conductivity withtemperature can be explained using the hopping mechanismof electrons between the Fe+2 and Fe+3 The dielectric con-stant of the prepared ferrite samples increases with increasein temperature up to certain temperature and afterwardsdecreases with increase in temperature
Conflict of Interests
The authors declare that there is no conflict of interestsregarding the publication of this paper
Acknowledgments
The authors are very grateful to Professor K Venu GopalReddy Head Department of Physics University College ofScience Osmania University Hyderabad The authors arevery thankful to UGC New Delhi for their financial assis-tance through Major Research Project (MRP)
References
[1] N S Gajbhiye and G Balaji ldquoMossbaur studies of nanosizeCuFe2O4ferritesrdquo in Advances in Nanoscience and Nano Tech
A Sharma Ed NISCAIR 2003[2] S A Jadhav ldquoMagnetic properties of Zn-substituted LindashCu
ferritesrdquo Journal of Magnetism andMagnetic Materials vol 224no 2 pp 167ndash172 2001
[3] M F Al-Hilli S Li and K S Kassim ldquoGadolinium substitutionand sintering temperature dependent electronic properties ofLindashNi ferriterdquo Journal ofMagnetism andMagneticMaterials vol324 pp 873ndash879 2012
[4] AM A El AtaM K El Nimr SM Attia D El Kony andAHAl-Hammadi ldquoStudies of AC electrical conductivity and initialmagnetic permeability of rare-earth-substituted LindashCo ferritesrdquoJournal of Magnetism andMagnetic Materials vol 297 no 1 pp33ndash43 2006
[5] AM A El Ata S M Attia D El Kony and A H Al-HammadildquoSpectral initial magnetic permeability and transport studies ofLi05minus05xCoxFe25minus05xO4 spinel ferriterdquo Journal ofMagnetism and
Magnetic Materials vol 295 no 1 pp 28ndash36 2005[6] S A Jadhav ldquoStructural and magnetic properties of Zn substi-
tuted LindashCu ferritesrdquo Materials Chemistry and Physics vol 65no 1 pp 120ndash123 2000
[7] H Kawazoe and K Ueda ldquoTransparent conducting oxidesbased on the spinel structurerdquo Journal of the American CeramicSociety vol 82 no 12 pp 3330ndash3336 1999
[8] P V Reddy and T S Rao ldquoX-ray studies on lithium-nickeland manganese-magnesiummixed ferritesrdquo Journal of the Less-Common Metals vol 75 no 2 pp 255ndash260 1980
[9] R S Devan Y D Kolekar and B K Chougule ldquoTransitionmetal-doped rare earth vanadates a regenerable catalytic mate-rial for SOFC anodesrdquo Journal of Physics CondensedMatter vol18 no 43 pp 9809ndash9821 2006
[10] M A Gabal and S S Ata-Allah ldquoEffect of diamagnetic substi-tution on the structural electrical and magnetic properties ofCoFe2O4rdquo Materials Chemistry and Physics vol 85 no 1 pp
104ndash112 2004
[11] E VeenaGopalan I A Al-Omari K AMalini et al ldquoImpact ofzinc substitution on the structural and magnetic properties ofchemically derived nanosized manganese zinc mixed ferritesrdquoJournal of Magnetism andMagnetic Materials vol 321 no 8 pp1092ndash1099 2009
[12] E Veena Gopalan K A Malini S Saravanan D Sakthi KumarY Yoshida and M R Anantharaman ldquoEvidence for polaronconduction in nanostructured manganese ferriterdquo Journal ofPhysics D Applied Physics vol 41 no 18 Article ID 1850052008
[13] M Srivastava S Chaubey andAKOjha ldquoInvestigation on sizedependent structural and magnetic behavior of nickel ferritenanoparticles prepared by sol-gel and hydrothermal methodsrdquoMaterials Chemistry and Physics vol 118 no 1 pp 174ndash1802009
[14] S S Bellad R B Pujar and B K Chougule ldquoStructural andmagnetic properties of some mixed LindashCd ferritesrdquo MaterialsChemistry and Physics vol 52 no 2 pp 166ndash169 1998
[15] D Ravinder ldquoDielectric behaviour of mixed lithium-zinc fer-ritesrdquo Journal of Materials Science Letters vol 11 no 22 pp1498ndash1500 1992
[16] Y Purushotham M B Reddy P Kishan D R Sagar and PV Reddy ldquoElectrical conductivity and thermopower studiesof titanium-substituted lithium-magnesium ferritesrdquoMaterialsLetters vol 17 no 6 pp 341ndash345 1993
[17] S A Mazen and T A Elmosalami ldquoStructural and elasticproperties of LindashNi ferritesrdquo ISRN Condensed Matter Physicsvol 2011 Article ID 820726 9 pages 2011
[18] S S Bhatu V K Lakhani A R Tanna et al ldquoEffect of nickelsubstitution on structural infrared and elastic properties oflithium ferriterdquo Indian Journal of Pure and Applied Physics vol45 no 7 pp 596ndash608 2007
[19] L Vijayan R Cheruku G Govindaraj and S Rajagopan ldquoIondynamics in combustion synthesized Na
3Cr2(PO4)3crystal-
litesrdquoMaterials Chemistry and Physics vol 125 no 1-2 pp 184ndash190 2011
[20] R Cheruku L Vijayan and G Govindaraj ldquoElectrical relax-ation studies of solution combustion synthesized nanocrys-talline Li
2NiZrO
4materialrdquo Materials Science and Engineering
B Solid-State Materials for Advanced Technology vol 177 no 11pp 771ndash779 2012
[21] L C Pathak T B Singh S Das A K Verma and P Ramachan-drarao ldquoEffect of pH on the combustion synthesis of nano-crystalline alumina powderrdquoMaterials Letters vol 57 no 2 pp380ndash385 2002
[22] J ChandradassM Balasubramanian andKHKim ldquoSynthesisand characterization of LaAlO
3nanopowders by various fuelsrdquo
Materials andManufacturing Processes vol 25 no 12 pp 1449ndash1453 2010
[23] J Jing L Liangchao and X Feng ldquoStructural analysis andmagnetic properties of Gd-doped LindashNi ferrites prepared usingrheological phase reaction methodrdquo Journal of Rare Earths vol25 no 1 pp 79ndash83 2007
[24] R G Kharabe R S Devan C M Kanamadi and B KChougule ldquoDielectric properties of mixed LindashNindashCd ferritesrdquoSmart Materials and Structures vol 15 no 2 pp N36ndashN392006
[25] F F Y Wang Treatise on Material Science and Technology vol2 Academic Press New York NY USA 1973
[26] R W Cahn Physical Mettaliurgy vol 1 North Holland Ams-terdam The Netherlands 1985
Physics Research International 11
[27] S B Patil R P Patil and B K Chougale ldquoDC electrical andthermo electric power measurement studies of NindashMgndashZnndashCoferritesrdquo Journal of Magnetism andMagnetic Materials vol 335pp 109ndash113 2013
[28] M A El Hiti ldquoStudies of structural electric andmagnetic prop-erties of some mixed ferritesrdquo Journal of Magnetism andMagnetic Materials vol 136 p 138 1994
[29] A N Patil R P Mahajan K K Patankar A K Ghatake andS A Patil ldquoMagnetic and Optical properties of conductionmechanism in Copper ferritesrdquo Indian Journal of Pure andApplied Physics vol 38 article 651 2000
[30] E J W Verwey and J H de Boer ldquoCation arrangement in afew oxides with crystal structures of the spinel typerdquo Recueildes Travaux Chimiques des Pays-Bas vol 55 no 6 pp 531ndash5401936
[31] A Verma T C Goel R GMendiratta and R G Gupta ldquoHigh-resistivity nickel-zinc ferrites by the citrate precursor methodrdquoJournal of Magnetism andMagneticMaterials vol 192 no 2 pp271ndash276 1999
[32] W D Kingery H K Bowen and P R Uhlum Introduction toCeramics Wiley New York NY USA 1975
[33] L L Hench and J K West Principles of Electronic CeramicsJohn Wiley amp Sons New York NY USA 1990
[34] S AMazen andH A Dawoud ldquoTemperature and compositiondependence of dielectric properties in LindashCu ferriterdquoMaterialsChemistry and Physics vol 82 no 3 pp 557ndash566 2003
[35] I Soibam S Phanjoubam H B Sharma H N K SarmaR Laishram and C Prakash ldquoEffects of Cobalt substitutionon the dielectric properties of LindashZn ferritesrdquo Solid StateCommunications vol 148 no 9-10 pp 399ndash402 2008
[36] S T Assar and H F Aboshiesha ldquoStructure and magneticproperties of CondashNindashLi ferrites synthesized by citrate precursormethodrdquo Journal ofMagnetism andMagneticMaterials vol 324no 22 pp 3846ndash3852 2012
[37] C G Koops ldquoOn the dispersion of resistivity and dielectricconstant of some semiconductors at audiofrequenciesrdquo PhysicalReview vol 83 article 121 1951
[38] K L Yadav andRN P Choudary ldquoStudy of structural electricaland optical properties of lead free based ceramic systemrdquoJournal of Materials Science Letters vol 19 p 61 1994
[39] V Verma V Pandey V N Shukla S Annapoorni and R KKotnala ldquoRemarkable influence on the dielectric and magneticproperties of lithium ferrite by Ti and Zn substitutionrdquo SolidState Communications vol 149 no 39-40 pp 1726ndash1730 2009
Submit your manuscripts athttpwwwhindawicom
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
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FluidsJournal of
Atomic and Molecular Physics
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Advances in Condensed Matter Physics
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Superconductivity
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Statistical MechanicsInternational Journal of
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GravityJournal of
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Physics Research International
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Solid State PhysicsJournal of
Computational Methods in Physics
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Soft MatterJournal of
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PhotonicsJournal of
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ThermodynamicsJournal of
Physics Research International 5
Table 2 Electrical resistivity and activation energies of the Li05minus05119909
Ni119909Fe25minus05119909
O4system
S No Composition Resistivity(Ω-cm) Curie temp (∘C) 119864
119886in paramagneticregion (eV)
119864119886in Ferromagneticregion (eV)
1 Li05Fe25O4 921 times 108 mdash mdash mdash2 Li04Ni02Fe24O4 917 times 108 567 161 0823 Li03Ni04Fe23O4 573 times 108 560 127 0934 Li02Ni06Fe22O4 273 times 108 540 095 0835 Li01Ni08Fe21O4 124 times 107 535 090 0736 NiFe2O4 682 times 107 528 081 071
in the temperature range from 473K to 873K The ferritesample is pressed into circular pellets The measurementswere recorded in the steps of 10 K
The temperature dependence of the prepared ferritesconductivity is plotted in accordance with the followingArrhenius type equation
log120590 = log120590119900minus
119864119886
119870119861119879
(7)
where 120590 is the conductivity 120590119900is the conductivity at abso-
lute temperature 119870119861is Boltzmannrsquos constant and 119879 is the
temperature The phenomenon of phase transition cationmigration cation reordering the presence of impurities andmagnetotransport effects are considered to be responsible forthe temperature dependence on the electrical conductivity ofthe prepared ferrite samples
The variations of the electrical conductivity (log120590119879) withinverse of temperature (1000119879) were shown in Figure 4Theconductivity of the ferrite samples increases with increasingthe temperatureThat is temperature increases and resistivityof the ferrites was decreased indicating the semiconductingbehaviour All the plots (except pure lithium ferrites) of elec-trical conductivity (log120590119879) versus 1000119879 yield a change inslope at a particular temperatureThis change in slope occurswhile crossing the Curie temperature (the temperature atwhich the ferromagnetic material changed to paramagnetic)The discontinuity at the Curie temperature was attributedto the magnetic transition from well-ordered ferromagneticstate to disordered paramagnetic state which involves differ-ent activation energies The values of the electrical resistivityand thermal activation energies of the prepared samples atferromagnetic region and paramagnetic region were given inTable 2
It is observed that the activation energy in the ferromag-netic region is smaller than the paramagnetic region this isdue to the effect of spin disordering
Someworkers have reported three regions of conductivity[26ndash29] of which the first region has been attributed to thepresence of impurities second region was due to the phasetransition from tetragonal structure to cubic structure andthe third one was due to the ferromagnetic to paramag-netic change The electrical conductivity of ferrites can beexplained on the basis of the Verwey and de Boer mechanism[30] which involves the exchange of charge carriers thatis electrons between the ions of the same element that are
present in more than one valence state (Fe+2 Fe+3) dis-tributed randomly over the crystallographic lattice sites TheFe+2 ion concentration is a characteristic property of nanofer-rites and it depends on several factors such as sintering tem-peraturetime and atmosphere and annealing time includingthe grain structure Some amount of Fe+2 ions is also formeddue to possible evaporation of Li ions during the sintering[28] Sintering of lithium ferrites is therefore carried out atrelatively lower temperature (500∘C) in order to avoid lithiumloss during sintering
The variation of DC electrical resistivity at 200∘C withNi composition in the Li ferrites is given in Table 2 The DCresistivity of the all the samples was observed to be in therange 124 times 107ndash921 times 108Ω-cm Compositionally decreasein the DC resistivity of LindashNi ferrites with increasing theNi concentration was observed The overall higher valuesof resistivity obtained for the ferrites can be attributed tothe small grain size and better compositional stoichiometrywith reduced Fe+2 formation as a result of low temperatureprocessing by the citrate gel method [31 32]
33 Dielectric Properties The dielectric constant and DCelectrical resistivity of ferrites are very important parametersfrom the application point of view These two parametersare electrical properties and exchange of electrons betweenthe Fe+2 and Fe+3 ions is responsible for these mechanismswhich results in local displacement of charges responsible forthe polarisation in ferrites The dielectric constant (1205761015840) anddielectric loss tangent (tan 120575) were found to be dependenton the variation of external factors such as temperature andfrequencyThe variation of dielectric constant (1205761015840) and dielec-tric loss tangent (tan 120575) with respect to selected frequenciesand temperature in the range of 300K to 700K has beeninvestigated
The variation of dielectric constant (1205761015840) and dielectricloss tangent (tan 120575) for all prepared ferrite samples withtemperature has been studied at different frequencies asshown in Figures 5(a) and 5(b)
It is observed that the dielectric constant (1205761015840) and dielec-tric loss tangent (tan 120575) of prepared samples were increasedwith increase in temperature for all selected frequencies Theincrease in temperature of the sample thermally activates thecharge carrier increasing the electron exchange interactionwhich results in increasing the dielectric constant values of
6 Physics Research International
minus5
minus4
minus3
minus2
minus1
0
1
minus5
minus4
minus3
minus2
minus1
0
1
2
minus5
minus4
minus3
minus2
minus1
0
1
minus4
minus3
minus2
minus1
0
1
minus25
minus20
minus15
minus10
minus05
00
05
10
15
minus30
minus25
minus20
minus15
minus10
minus05
00
05
10
15
x = 00 x = 02
x = 04 x = 06
x = 08 x = 10
161 eV
082 eV
127 eV
093 eV
095 eV
083 eV
090 eV
073 eV
081 ev
071 eV
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
Figure 4 Arrhenius plots for electrical conductivities of Li05minus05xNixFe25minus05xO4 nanoferrites
Physics Research International 7
510152025303540
Temperature (K)
5
10
15
20
25
30
0
20
40
60
80
100
120
020406080
100120140
0
20
40
60
80
100
020406080
100120140
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
75 kHz
75 kHz75 kHz 75 kHz
75 kHz
75 kHz
30kHz
30kHz30kHz 30kHz
30kHz
30kHz600kHz
600kHz600kHz
600kHz
600kHz
600kHz1MHz
1MHz1MHz
1MHz
1MHz
1MHz3MHz
3MHz 3MHz3MHz
3MHz
3MHz5MHz
5MHz5MHz
5MHz
5MHz
5MHz
300 400 500 600 700 800
Temperature (K) Temperature (K)300 400 500 600 700 800 300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
(a)
minus0100010203040506070809
Temperature (K)
0005101520253035
minus02000204060810121416
minus02000204060810121416
0002040608101214161820
minus0200020406081012
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
750Hz
750Hz 750Hz
750Hz
750Hz 750Hz
3kHz
3kHz3kHz
3kHz
3kHz
3kHz
100 kHz
100 kHz100 kHz
100 kHz
100 kHz
100 kHz
1MHz
1MHz1MHz
1MHz
1MHz
1MHz
3MHz
3MHz3MHz
3MHz
3MHz
3MHz
5MHz
5MHz
5MHz
5MHz
5MHz
5MHz
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 5 (a)Variation of dielectric constant (1205761015840)with temperature at different frequencies of Li05minus05xNixFe25minus05xO4 nanoferrites (b)Variation
of loss tangent (tan 120575) with temperature at different frequencies of Li05minus05xNixFe25minus05xO4 nanoferrites
the ferrites It is observed that there are four major con-tributions for polarisation in ferrites They are electronicatomic dipolar and interfacial polarisations [33] Electronicand atomic polarisations are important at high frequenciesand are independent of temperature while remaining two are
important at lower frequencies and dependent on tempera-ture By increasing the temperature interfacial polarisationis increased and dipolar polarisation decreases The increasein dielectric constant with increase in temperature at lowfrequency may be due to the interfacial polarisation
8 Physics Research International
6
7
8
9
10
11
12
13
14
Ni composition
750Hz and 323K
Die
lect
ric co
nsta
nt (120576
998400 )times10
2
00 02 04 06 08 10
(a)
000
002
004
006
008
010 750Hz and 323K
Ni composition00 02 04 06 08 10
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 6 Variation of dielectric constant (1205761015840) and tan 120575 with Ni concentration
From Figure 5(a) it can be noticed that the dielectricconstant (1205761015840) values increase rapidly in the low temperaturerange (119879 lt 600K) whereas in the high temperaturerange (119879 gt 600K) dielectric constant (1205761015840) reaches a stablevalue (Resonance peak) after that it starts to decrease withincreasing the temperature For the low temperature range(119879 lt 600K) the polarisation is increased by the electricfield and also by increasing the number of charge carriers(electrons) which are increased with temperature hence theincrease in the dielectric constant (1205761015840) at low temperaturerange (119879 lt 600K) is due to increase in both temperatureand frequency For the high temperature range (119879 gt 600K)the saturation in the generation of charge carriers is reachedTherefore the electron exchange between the ions of the sameelement that are present in more than one valence state (Fe+2Fe+3 orNi+2 Ni+1) cannot follow the field variation and hencedielectric constant decreases [34] The temperature at whichthe resonance peak appeared is observed to be shifted towardsthe higher temperature as the frequency is increased [35]The variation of loss angle tangent (tan 120575) of the preparedsample as a function temperature at different frequencies hasalso been investigated and an increase is observed just as thedielectric constant (1205761015840) curve This variation of loss tangentwith temperature curve can be understood on the basis ofDebyersquos equation for loss given as [33]
The compositional dependence (Ni concentration) of thedielectric constant (1205761015840) and dielectric loss tangent (tan 120575) ofprepared samples at 323K and at 75 kHz is shown in Figure 6It can be observed that the dielectric constant (1205761015840) value ofthe prepared samples was increased from 119909 = 00 to 119909 =06 and then decreased It can be attributed to the effect ofsimultaneous contributions of different factors such as grainsize density porosity and cation distribution The initialincrease in dielectric constant (1205761015840) when Ni content increasesfrom 119909 = 00 to 119909 = 06 coincides with the increase ofgrain size from Table 1 [36] After that the cation distribution
becomes the predominant factor in decreasing the dielectricconstant (1205761015840) with Ni content since the decrease of holehoping becomes greater than the increase of electron hopingin the B-sites For the same reasons it can be observed thatthe variation of loss tangent of the prepared samples withNi content has almost the same trend in inverse mannerFrom all these results it can be concluded that doping ofLi nanoferrites with Ni ions leads to improvement in theirdielectrical properties especially in the sample at 119909 = 06 andthese compositions make promising materials for microwaveapplications
The variation of dielectric constant (1205761015840) and dielectric losstangent (tan 120575) of prepared samples at 119909 = 04with frequencyat different temperatures has been investigated in Figure 7
It is observed that dielectric constant (1205761015840) of preparedsamples was decreased rapidly in the low frequency regionand decrease is quite slow in the high frequency regionthat is dielectric constant is almost independent of fre-quency (shown in Figure 7(a)) This dielectric behaviour offerrites was explained by Koopsrsquo theory [37] According tothis model dielectric medium is assumed to be made upof highly conducting grains surrounded by nonconductinggrain boundaries The grain boundaries are more effectiveat low frequencies and grains are more effective at thehigher frequencies As the grain boundaries having the largeresistance the charge carriers (electrons) pile up there andproduce large space charge polarisation which results in largevalue of dielectric constant at low frequency region Andfurther increasing the frequency the charge carriers (elec-trons) change their direction of motion due to the factthat this accumulation of charge at the grain boundarydecreases which results in the decrease of dielectric constantFrom the figures it is also observed that dielectric constantvalues increase with increase in the temperature in the lowfrequency region because electron exchange between the Fe+2and Fe+3 ions at octahedral sites was thermally activated
Physics Research International 9
15
30
45
60
75
90
105
120x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Log f (Hz)
(a)
00
02
04
06
08
10
12
14
16x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric lo
ss (t
an 120575)
Log f (Hz)
(b)
Figure 7 The variation of dielectric constant (1205761015840) and (tan 120575) with frequency at different temperatures of the LindashNi ferrite system at 119909 = 04
Figure 7(b) shows the variation dielectric loss tangent(tan 120575) with frequencies at different temperatures for 119909 = 04It is observed that the dielectric loss decreases with frequencybecause the jumping frequency of charge carriers cannot fol-low the frequency of the applied field after certain frequency
This figure also shows that the dielectric loss of the pre-pared samples increases with increasing the temperaturebecause of the enhanced hopping of thermally energized elec-trons
Figure 8 shows the variation of dielectric constant at75 kHz with temperature range 323Kndash723K for all ferritesamples It can be observed that the dielectric constant ofall the ferrite samples increases with increasing temperatureup to certain temperature after this temperature dielectricconstant of the prepared samples is going to decrease thattemperature is known as dielectric transition temperature119879119889[38] The decrease in the value of dielectric constant
takes place when the jumping frequency of the electronscannot follow the frequency of the applied electric field FromFigure 8 it is observed that dielectric transition temperature119879119889range is found to be in the 600Kndash680K for all prepared
samples of Li05minus05xNixFe25minus05xO4 system [39] It is also
observed that the slope variation in theArrhenius plots (otherthan Curie point) was in the same temperature range only forall samples
4 Conclusions
All the LindashNi ferrites samples prepared by low temperatureautocombustion method and single phase were confirmedthroughXRD analysisThe experimental results revealed thatthe lattice parameter X-ray density of the prepared ferrite
0
20
40
60
80
100
120
140
Temperature (K)
Data1 ln00Data1 LN02
Data1 LN04
Data1 LN06
Data1 LN08
Data1 LN10
300 400 500 600 700 800
120576998400times10
2
Figure 8 The variation of dielectric constant with temp forLi05minus05xNixFe25minus05xO4 nanoferrites
samples increases with increase in Ni-substituted concen-tration and the grain size is also in the nm range only DCelectrical resistivity of the prepared samples decreases withincreasing in the temperature which shows the semiconduct-ing behaviour of nanoferrites It is observed that the dis-continuity in the log(120590119879) versus 1000119879 graph shows Curiepoint of the prepared ferrite samples Curie temperature of
10 Physics Research International
the prepared LindashNi ferrites decreases with the increase ofthe Ni concentration The variation of DC conductivity withtemperature can be explained using the hopping mechanismof electrons between the Fe+2 and Fe+3 The dielectric con-stant of the prepared ferrite samples increases with increasein temperature up to certain temperature and afterwardsdecreases with increase in temperature
Conflict of Interests
The authors declare that there is no conflict of interestsregarding the publication of this paper
Acknowledgments
The authors are very grateful to Professor K Venu GopalReddy Head Department of Physics University College ofScience Osmania University Hyderabad The authors arevery thankful to UGC New Delhi for their financial assis-tance through Major Research Project (MRP)
References
[1] N S Gajbhiye and G Balaji ldquoMossbaur studies of nanosizeCuFe2O4ferritesrdquo in Advances in Nanoscience and Nano Tech
A Sharma Ed NISCAIR 2003[2] S A Jadhav ldquoMagnetic properties of Zn-substituted LindashCu
ferritesrdquo Journal of Magnetism andMagnetic Materials vol 224no 2 pp 167ndash172 2001
[3] M F Al-Hilli S Li and K S Kassim ldquoGadolinium substitutionand sintering temperature dependent electronic properties ofLindashNi ferriterdquo Journal ofMagnetism andMagneticMaterials vol324 pp 873ndash879 2012
[4] AM A El AtaM K El Nimr SM Attia D El Kony andAHAl-Hammadi ldquoStudies of AC electrical conductivity and initialmagnetic permeability of rare-earth-substituted LindashCo ferritesrdquoJournal of Magnetism andMagnetic Materials vol 297 no 1 pp33ndash43 2006
[5] AM A El Ata S M Attia D El Kony and A H Al-HammadildquoSpectral initial magnetic permeability and transport studies ofLi05minus05xCoxFe25minus05xO4 spinel ferriterdquo Journal ofMagnetism and
Magnetic Materials vol 295 no 1 pp 28ndash36 2005[6] S A Jadhav ldquoStructural and magnetic properties of Zn substi-
tuted LindashCu ferritesrdquo Materials Chemistry and Physics vol 65no 1 pp 120ndash123 2000
[7] H Kawazoe and K Ueda ldquoTransparent conducting oxidesbased on the spinel structurerdquo Journal of the American CeramicSociety vol 82 no 12 pp 3330ndash3336 1999
[8] P V Reddy and T S Rao ldquoX-ray studies on lithium-nickeland manganese-magnesiummixed ferritesrdquo Journal of the Less-Common Metals vol 75 no 2 pp 255ndash260 1980
[9] R S Devan Y D Kolekar and B K Chougule ldquoTransitionmetal-doped rare earth vanadates a regenerable catalytic mate-rial for SOFC anodesrdquo Journal of Physics CondensedMatter vol18 no 43 pp 9809ndash9821 2006
[10] M A Gabal and S S Ata-Allah ldquoEffect of diamagnetic substi-tution on the structural electrical and magnetic properties ofCoFe2O4rdquo Materials Chemistry and Physics vol 85 no 1 pp
104ndash112 2004
[11] E VeenaGopalan I A Al-Omari K AMalini et al ldquoImpact ofzinc substitution on the structural and magnetic properties ofchemically derived nanosized manganese zinc mixed ferritesrdquoJournal of Magnetism andMagnetic Materials vol 321 no 8 pp1092ndash1099 2009
[12] E Veena Gopalan K A Malini S Saravanan D Sakthi KumarY Yoshida and M R Anantharaman ldquoEvidence for polaronconduction in nanostructured manganese ferriterdquo Journal ofPhysics D Applied Physics vol 41 no 18 Article ID 1850052008
[13] M Srivastava S Chaubey andAKOjha ldquoInvestigation on sizedependent structural and magnetic behavior of nickel ferritenanoparticles prepared by sol-gel and hydrothermal methodsrdquoMaterials Chemistry and Physics vol 118 no 1 pp 174ndash1802009
[14] S S Bellad R B Pujar and B K Chougule ldquoStructural andmagnetic properties of some mixed LindashCd ferritesrdquo MaterialsChemistry and Physics vol 52 no 2 pp 166ndash169 1998
[15] D Ravinder ldquoDielectric behaviour of mixed lithium-zinc fer-ritesrdquo Journal of Materials Science Letters vol 11 no 22 pp1498ndash1500 1992
[16] Y Purushotham M B Reddy P Kishan D R Sagar and PV Reddy ldquoElectrical conductivity and thermopower studiesof titanium-substituted lithium-magnesium ferritesrdquoMaterialsLetters vol 17 no 6 pp 341ndash345 1993
[17] S A Mazen and T A Elmosalami ldquoStructural and elasticproperties of LindashNi ferritesrdquo ISRN Condensed Matter Physicsvol 2011 Article ID 820726 9 pages 2011
[18] S S Bhatu V K Lakhani A R Tanna et al ldquoEffect of nickelsubstitution on structural infrared and elastic properties oflithium ferriterdquo Indian Journal of Pure and Applied Physics vol45 no 7 pp 596ndash608 2007
[19] L Vijayan R Cheruku G Govindaraj and S Rajagopan ldquoIondynamics in combustion synthesized Na
3Cr2(PO4)3crystal-
litesrdquoMaterials Chemistry and Physics vol 125 no 1-2 pp 184ndash190 2011
[20] R Cheruku L Vijayan and G Govindaraj ldquoElectrical relax-ation studies of solution combustion synthesized nanocrys-talline Li
2NiZrO
4materialrdquo Materials Science and Engineering
B Solid-State Materials for Advanced Technology vol 177 no 11pp 771ndash779 2012
[21] L C Pathak T B Singh S Das A K Verma and P Ramachan-drarao ldquoEffect of pH on the combustion synthesis of nano-crystalline alumina powderrdquoMaterials Letters vol 57 no 2 pp380ndash385 2002
[22] J ChandradassM Balasubramanian andKHKim ldquoSynthesisand characterization of LaAlO
3nanopowders by various fuelsrdquo
Materials andManufacturing Processes vol 25 no 12 pp 1449ndash1453 2010
[23] J Jing L Liangchao and X Feng ldquoStructural analysis andmagnetic properties of Gd-doped LindashNi ferrites prepared usingrheological phase reaction methodrdquo Journal of Rare Earths vol25 no 1 pp 79ndash83 2007
[24] R G Kharabe R S Devan C M Kanamadi and B KChougule ldquoDielectric properties of mixed LindashNindashCd ferritesrdquoSmart Materials and Structures vol 15 no 2 pp N36ndashN392006
[25] F F Y Wang Treatise on Material Science and Technology vol2 Academic Press New York NY USA 1973
[26] R W Cahn Physical Mettaliurgy vol 1 North Holland Ams-terdam The Netherlands 1985
Physics Research International 11
[27] S B Patil R P Patil and B K Chougale ldquoDC electrical andthermo electric power measurement studies of NindashMgndashZnndashCoferritesrdquo Journal of Magnetism andMagnetic Materials vol 335pp 109ndash113 2013
[28] M A El Hiti ldquoStudies of structural electric andmagnetic prop-erties of some mixed ferritesrdquo Journal of Magnetism andMagnetic Materials vol 136 p 138 1994
[29] A N Patil R P Mahajan K K Patankar A K Ghatake andS A Patil ldquoMagnetic and Optical properties of conductionmechanism in Copper ferritesrdquo Indian Journal of Pure andApplied Physics vol 38 article 651 2000
[30] E J W Verwey and J H de Boer ldquoCation arrangement in afew oxides with crystal structures of the spinel typerdquo Recueildes Travaux Chimiques des Pays-Bas vol 55 no 6 pp 531ndash5401936
[31] A Verma T C Goel R GMendiratta and R G Gupta ldquoHigh-resistivity nickel-zinc ferrites by the citrate precursor methodrdquoJournal of Magnetism andMagneticMaterials vol 192 no 2 pp271ndash276 1999
[32] W D Kingery H K Bowen and P R Uhlum Introduction toCeramics Wiley New York NY USA 1975
[33] L L Hench and J K West Principles of Electronic CeramicsJohn Wiley amp Sons New York NY USA 1990
[34] S AMazen andH A Dawoud ldquoTemperature and compositiondependence of dielectric properties in LindashCu ferriterdquoMaterialsChemistry and Physics vol 82 no 3 pp 557ndash566 2003
[35] I Soibam S Phanjoubam H B Sharma H N K SarmaR Laishram and C Prakash ldquoEffects of Cobalt substitutionon the dielectric properties of LindashZn ferritesrdquo Solid StateCommunications vol 148 no 9-10 pp 399ndash402 2008
[36] S T Assar and H F Aboshiesha ldquoStructure and magneticproperties of CondashNindashLi ferrites synthesized by citrate precursormethodrdquo Journal ofMagnetism andMagneticMaterials vol 324no 22 pp 3846ndash3852 2012
[37] C G Koops ldquoOn the dispersion of resistivity and dielectricconstant of some semiconductors at audiofrequenciesrdquo PhysicalReview vol 83 article 121 1951
[38] K L Yadav andRN P Choudary ldquoStudy of structural electricaland optical properties of lead free based ceramic systemrdquoJournal of Materials Science Letters vol 19 p 61 1994
[39] V Verma V Pandey V N Shukla S Annapoorni and R KKotnala ldquoRemarkable influence on the dielectric and magneticproperties of lithium ferrite by Ti and Zn substitutionrdquo SolidState Communications vol 149 no 39-40 pp 1726ndash1730 2009
Submit your manuscripts athttpwwwhindawicom
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
High Energy PhysicsAdvances in
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FluidsJournal of
Atomic and Molecular Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Advances in Condensed Matter Physics
OpticsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstronomyAdvances in
International Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Superconductivity
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Statistical MechanicsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
GravityJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstrophysicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Physics Research International
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Solid State PhysicsJournal of
Computational Methods in Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Soft MatterJournal of
Hindawi Publishing Corporationhttpwwwhindawicom
AerodynamicsJournal of
Volume 2014
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PhotonicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Journal of
Biophysics
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
ThermodynamicsJournal of
6 Physics Research International
minus5
minus4
minus3
minus2
minus1
0
1
minus5
minus4
minus3
minus2
minus1
0
1
2
minus5
minus4
minus3
minus2
minus1
0
1
minus4
minus3
minus2
minus1
0
1
minus25
minus20
minus15
minus10
minus05
00
05
10
15
minus30
minus25
minus20
minus15
minus10
minus05
00
05
10
15
x = 00 x = 02
x = 04 x = 06
x = 08 x = 10
161 eV
082 eV
127 eV
093 eV
095 eV
083 eV
090 eV
073 eV
081 ev
071 eV
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
log(120590T)
(Sm
T)
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
1000T (Kminus1)
10 12 14 16 18 20 22
Figure 4 Arrhenius plots for electrical conductivities of Li05minus05xNixFe25minus05xO4 nanoferrites
Physics Research International 7
510152025303540
Temperature (K)
5
10
15
20
25
30
0
20
40
60
80
100
120
020406080
100120140
0
20
40
60
80
100
020406080
100120140
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
75 kHz
75 kHz75 kHz 75 kHz
75 kHz
75 kHz
30kHz
30kHz30kHz 30kHz
30kHz
30kHz600kHz
600kHz600kHz
600kHz
600kHz
600kHz1MHz
1MHz1MHz
1MHz
1MHz
1MHz3MHz
3MHz 3MHz3MHz
3MHz
3MHz5MHz
5MHz5MHz
5MHz
5MHz
5MHz
300 400 500 600 700 800
Temperature (K) Temperature (K)300 400 500 600 700 800 300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
(a)
minus0100010203040506070809
Temperature (K)
0005101520253035
minus02000204060810121416
minus02000204060810121416
0002040608101214161820
minus0200020406081012
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
750Hz
750Hz 750Hz
750Hz
750Hz 750Hz
3kHz
3kHz3kHz
3kHz
3kHz
3kHz
100 kHz
100 kHz100 kHz
100 kHz
100 kHz
100 kHz
1MHz
1MHz1MHz
1MHz
1MHz
1MHz
3MHz
3MHz3MHz
3MHz
3MHz
3MHz
5MHz
5MHz
5MHz
5MHz
5MHz
5MHz
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 5 (a)Variation of dielectric constant (1205761015840)with temperature at different frequencies of Li05minus05xNixFe25minus05xO4 nanoferrites (b)Variation
of loss tangent (tan 120575) with temperature at different frequencies of Li05minus05xNixFe25minus05xO4 nanoferrites
the ferrites It is observed that there are four major con-tributions for polarisation in ferrites They are electronicatomic dipolar and interfacial polarisations [33] Electronicand atomic polarisations are important at high frequenciesand are independent of temperature while remaining two are
important at lower frequencies and dependent on tempera-ture By increasing the temperature interfacial polarisationis increased and dipolar polarisation decreases The increasein dielectric constant with increase in temperature at lowfrequency may be due to the interfacial polarisation
8 Physics Research International
6
7
8
9
10
11
12
13
14
Ni composition
750Hz and 323K
Die
lect
ric co
nsta
nt (120576
998400 )times10
2
00 02 04 06 08 10
(a)
000
002
004
006
008
010 750Hz and 323K
Ni composition00 02 04 06 08 10
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 6 Variation of dielectric constant (1205761015840) and tan 120575 with Ni concentration
From Figure 5(a) it can be noticed that the dielectricconstant (1205761015840) values increase rapidly in the low temperaturerange (119879 lt 600K) whereas in the high temperaturerange (119879 gt 600K) dielectric constant (1205761015840) reaches a stablevalue (Resonance peak) after that it starts to decrease withincreasing the temperature For the low temperature range(119879 lt 600K) the polarisation is increased by the electricfield and also by increasing the number of charge carriers(electrons) which are increased with temperature hence theincrease in the dielectric constant (1205761015840) at low temperaturerange (119879 lt 600K) is due to increase in both temperatureand frequency For the high temperature range (119879 gt 600K)the saturation in the generation of charge carriers is reachedTherefore the electron exchange between the ions of the sameelement that are present in more than one valence state (Fe+2Fe+3 orNi+2 Ni+1) cannot follow the field variation and hencedielectric constant decreases [34] The temperature at whichthe resonance peak appeared is observed to be shifted towardsthe higher temperature as the frequency is increased [35]The variation of loss angle tangent (tan 120575) of the preparedsample as a function temperature at different frequencies hasalso been investigated and an increase is observed just as thedielectric constant (1205761015840) curve This variation of loss tangentwith temperature curve can be understood on the basis ofDebyersquos equation for loss given as [33]
The compositional dependence (Ni concentration) of thedielectric constant (1205761015840) and dielectric loss tangent (tan 120575) ofprepared samples at 323K and at 75 kHz is shown in Figure 6It can be observed that the dielectric constant (1205761015840) value ofthe prepared samples was increased from 119909 = 00 to 119909 =06 and then decreased It can be attributed to the effect ofsimultaneous contributions of different factors such as grainsize density porosity and cation distribution The initialincrease in dielectric constant (1205761015840) when Ni content increasesfrom 119909 = 00 to 119909 = 06 coincides with the increase ofgrain size from Table 1 [36] After that the cation distribution
becomes the predominant factor in decreasing the dielectricconstant (1205761015840) with Ni content since the decrease of holehoping becomes greater than the increase of electron hopingin the B-sites For the same reasons it can be observed thatthe variation of loss tangent of the prepared samples withNi content has almost the same trend in inverse mannerFrom all these results it can be concluded that doping ofLi nanoferrites with Ni ions leads to improvement in theirdielectrical properties especially in the sample at 119909 = 06 andthese compositions make promising materials for microwaveapplications
The variation of dielectric constant (1205761015840) and dielectric losstangent (tan 120575) of prepared samples at 119909 = 04with frequencyat different temperatures has been investigated in Figure 7
It is observed that dielectric constant (1205761015840) of preparedsamples was decreased rapidly in the low frequency regionand decrease is quite slow in the high frequency regionthat is dielectric constant is almost independent of fre-quency (shown in Figure 7(a)) This dielectric behaviour offerrites was explained by Koopsrsquo theory [37] According tothis model dielectric medium is assumed to be made upof highly conducting grains surrounded by nonconductinggrain boundaries The grain boundaries are more effectiveat low frequencies and grains are more effective at thehigher frequencies As the grain boundaries having the largeresistance the charge carriers (electrons) pile up there andproduce large space charge polarisation which results in largevalue of dielectric constant at low frequency region Andfurther increasing the frequency the charge carriers (elec-trons) change their direction of motion due to the factthat this accumulation of charge at the grain boundarydecreases which results in the decrease of dielectric constantFrom the figures it is also observed that dielectric constantvalues increase with increase in the temperature in the lowfrequency region because electron exchange between the Fe+2and Fe+3 ions at octahedral sites was thermally activated
Physics Research International 9
15
30
45
60
75
90
105
120x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Log f (Hz)
(a)
00
02
04
06
08
10
12
14
16x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric lo
ss (t
an 120575)
Log f (Hz)
(b)
Figure 7 The variation of dielectric constant (1205761015840) and (tan 120575) with frequency at different temperatures of the LindashNi ferrite system at 119909 = 04
Figure 7(b) shows the variation dielectric loss tangent(tan 120575) with frequencies at different temperatures for 119909 = 04It is observed that the dielectric loss decreases with frequencybecause the jumping frequency of charge carriers cannot fol-low the frequency of the applied field after certain frequency
This figure also shows that the dielectric loss of the pre-pared samples increases with increasing the temperaturebecause of the enhanced hopping of thermally energized elec-trons
Figure 8 shows the variation of dielectric constant at75 kHz with temperature range 323Kndash723K for all ferritesamples It can be observed that the dielectric constant ofall the ferrite samples increases with increasing temperatureup to certain temperature after this temperature dielectricconstant of the prepared samples is going to decrease thattemperature is known as dielectric transition temperature119879119889[38] The decrease in the value of dielectric constant
takes place when the jumping frequency of the electronscannot follow the frequency of the applied electric field FromFigure 8 it is observed that dielectric transition temperature119879119889range is found to be in the 600Kndash680K for all prepared
samples of Li05minus05xNixFe25minus05xO4 system [39] It is also
observed that the slope variation in theArrhenius plots (otherthan Curie point) was in the same temperature range only forall samples
4 Conclusions
All the LindashNi ferrites samples prepared by low temperatureautocombustion method and single phase were confirmedthroughXRD analysisThe experimental results revealed thatthe lattice parameter X-ray density of the prepared ferrite
0
20
40
60
80
100
120
140
Temperature (K)
Data1 ln00Data1 LN02
Data1 LN04
Data1 LN06
Data1 LN08
Data1 LN10
300 400 500 600 700 800
120576998400times10
2
Figure 8 The variation of dielectric constant with temp forLi05minus05xNixFe25minus05xO4 nanoferrites
samples increases with increase in Ni-substituted concen-tration and the grain size is also in the nm range only DCelectrical resistivity of the prepared samples decreases withincreasing in the temperature which shows the semiconduct-ing behaviour of nanoferrites It is observed that the dis-continuity in the log(120590119879) versus 1000119879 graph shows Curiepoint of the prepared ferrite samples Curie temperature of
10 Physics Research International
the prepared LindashNi ferrites decreases with the increase ofthe Ni concentration The variation of DC conductivity withtemperature can be explained using the hopping mechanismof electrons between the Fe+2 and Fe+3 The dielectric con-stant of the prepared ferrite samples increases with increasein temperature up to certain temperature and afterwardsdecreases with increase in temperature
Conflict of Interests
The authors declare that there is no conflict of interestsregarding the publication of this paper
Acknowledgments
The authors are very grateful to Professor K Venu GopalReddy Head Department of Physics University College ofScience Osmania University Hyderabad The authors arevery thankful to UGC New Delhi for their financial assis-tance through Major Research Project (MRP)
References
[1] N S Gajbhiye and G Balaji ldquoMossbaur studies of nanosizeCuFe2O4ferritesrdquo in Advances in Nanoscience and Nano Tech
A Sharma Ed NISCAIR 2003[2] S A Jadhav ldquoMagnetic properties of Zn-substituted LindashCu
ferritesrdquo Journal of Magnetism andMagnetic Materials vol 224no 2 pp 167ndash172 2001
[3] M F Al-Hilli S Li and K S Kassim ldquoGadolinium substitutionand sintering temperature dependent electronic properties ofLindashNi ferriterdquo Journal ofMagnetism andMagneticMaterials vol324 pp 873ndash879 2012
[4] AM A El AtaM K El Nimr SM Attia D El Kony andAHAl-Hammadi ldquoStudies of AC electrical conductivity and initialmagnetic permeability of rare-earth-substituted LindashCo ferritesrdquoJournal of Magnetism andMagnetic Materials vol 297 no 1 pp33ndash43 2006
[5] AM A El Ata S M Attia D El Kony and A H Al-HammadildquoSpectral initial magnetic permeability and transport studies ofLi05minus05xCoxFe25minus05xO4 spinel ferriterdquo Journal ofMagnetism and
Magnetic Materials vol 295 no 1 pp 28ndash36 2005[6] S A Jadhav ldquoStructural and magnetic properties of Zn substi-
tuted LindashCu ferritesrdquo Materials Chemistry and Physics vol 65no 1 pp 120ndash123 2000
[7] H Kawazoe and K Ueda ldquoTransparent conducting oxidesbased on the spinel structurerdquo Journal of the American CeramicSociety vol 82 no 12 pp 3330ndash3336 1999
[8] P V Reddy and T S Rao ldquoX-ray studies on lithium-nickeland manganese-magnesiummixed ferritesrdquo Journal of the Less-Common Metals vol 75 no 2 pp 255ndash260 1980
[9] R S Devan Y D Kolekar and B K Chougule ldquoTransitionmetal-doped rare earth vanadates a regenerable catalytic mate-rial for SOFC anodesrdquo Journal of Physics CondensedMatter vol18 no 43 pp 9809ndash9821 2006
[10] M A Gabal and S S Ata-Allah ldquoEffect of diamagnetic substi-tution on the structural electrical and magnetic properties ofCoFe2O4rdquo Materials Chemistry and Physics vol 85 no 1 pp
104ndash112 2004
[11] E VeenaGopalan I A Al-Omari K AMalini et al ldquoImpact ofzinc substitution on the structural and magnetic properties ofchemically derived nanosized manganese zinc mixed ferritesrdquoJournal of Magnetism andMagnetic Materials vol 321 no 8 pp1092ndash1099 2009
[12] E Veena Gopalan K A Malini S Saravanan D Sakthi KumarY Yoshida and M R Anantharaman ldquoEvidence for polaronconduction in nanostructured manganese ferriterdquo Journal ofPhysics D Applied Physics vol 41 no 18 Article ID 1850052008
[13] M Srivastava S Chaubey andAKOjha ldquoInvestigation on sizedependent structural and magnetic behavior of nickel ferritenanoparticles prepared by sol-gel and hydrothermal methodsrdquoMaterials Chemistry and Physics vol 118 no 1 pp 174ndash1802009
[14] S S Bellad R B Pujar and B K Chougule ldquoStructural andmagnetic properties of some mixed LindashCd ferritesrdquo MaterialsChemistry and Physics vol 52 no 2 pp 166ndash169 1998
[15] D Ravinder ldquoDielectric behaviour of mixed lithium-zinc fer-ritesrdquo Journal of Materials Science Letters vol 11 no 22 pp1498ndash1500 1992
[16] Y Purushotham M B Reddy P Kishan D R Sagar and PV Reddy ldquoElectrical conductivity and thermopower studiesof titanium-substituted lithium-magnesium ferritesrdquoMaterialsLetters vol 17 no 6 pp 341ndash345 1993
[17] S A Mazen and T A Elmosalami ldquoStructural and elasticproperties of LindashNi ferritesrdquo ISRN Condensed Matter Physicsvol 2011 Article ID 820726 9 pages 2011
[18] S S Bhatu V K Lakhani A R Tanna et al ldquoEffect of nickelsubstitution on structural infrared and elastic properties oflithium ferriterdquo Indian Journal of Pure and Applied Physics vol45 no 7 pp 596ndash608 2007
[19] L Vijayan R Cheruku G Govindaraj and S Rajagopan ldquoIondynamics in combustion synthesized Na
3Cr2(PO4)3crystal-
litesrdquoMaterials Chemistry and Physics vol 125 no 1-2 pp 184ndash190 2011
[20] R Cheruku L Vijayan and G Govindaraj ldquoElectrical relax-ation studies of solution combustion synthesized nanocrys-talline Li
2NiZrO
4materialrdquo Materials Science and Engineering
B Solid-State Materials for Advanced Technology vol 177 no 11pp 771ndash779 2012
[21] L C Pathak T B Singh S Das A K Verma and P Ramachan-drarao ldquoEffect of pH on the combustion synthesis of nano-crystalline alumina powderrdquoMaterials Letters vol 57 no 2 pp380ndash385 2002
[22] J ChandradassM Balasubramanian andKHKim ldquoSynthesisand characterization of LaAlO
3nanopowders by various fuelsrdquo
Materials andManufacturing Processes vol 25 no 12 pp 1449ndash1453 2010
[23] J Jing L Liangchao and X Feng ldquoStructural analysis andmagnetic properties of Gd-doped LindashNi ferrites prepared usingrheological phase reaction methodrdquo Journal of Rare Earths vol25 no 1 pp 79ndash83 2007
[24] R G Kharabe R S Devan C M Kanamadi and B KChougule ldquoDielectric properties of mixed LindashNindashCd ferritesrdquoSmart Materials and Structures vol 15 no 2 pp N36ndashN392006
[25] F F Y Wang Treatise on Material Science and Technology vol2 Academic Press New York NY USA 1973
[26] R W Cahn Physical Mettaliurgy vol 1 North Holland Ams-terdam The Netherlands 1985
Physics Research International 11
[27] S B Patil R P Patil and B K Chougale ldquoDC electrical andthermo electric power measurement studies of NindashMgndashZnndashCoferritesrdquo Journal of Magnetism andMagnetic Materials vol 335pp 109ndash113 2013
[28] M A El Hiti ldquoStudies of structural electric andmagnetic prop-erties of some mixed ferritesrdquo Journal of Magnetism andMagnetic Materials vol 136 p 138 1994
[29] A N Patil R P Mahajan K K Patankar A K Ghatake andS A Patil ldquoMagnetic and Optical properties of conductionmechanism in Copper ferritesrdquo Indian Journal of Pure andApplied Physics vol 38 article 651 2000
[30] E J W Verwey and J H de Boer ldquoCation arrangement in afew oxides with crystal structures of the spinel typerdquo Recueildes Travaux Chimiques des Pays-Bas vol 55 no 6 pp 531ndash5401936
[31] A Verma T C Goel R GMendiratta and R G Gupta ldquoHigh-resistivity nickel-zinc ferrites by the citrate precursor methodrdquoJournal of Magnetism andMagneticMaterials vol 192 no 2 pp271ndash276 1999
[32] W D Kingery H K Bowen and P R Uhlum Introduction toCeramics Wiley New York NY USA 1975
[33] L L Hench and J K West Principles of Electronic CeramicsJohn Wiley amp Sons New York NY USA 1990
[34] S AMazen andH A Dawoud ldquoTemperature and compositiondependence of dielectric properties in LindashCu ferriterdquoMaterialsChemistry and Physics vol 82 no 3 pp 557ndash566 2003
[35] I Soibam S Phanjoubam H B Sharma H N K SarmaR Laishram and C Prakash ldquoEffects of Cobalt substitutionon the dielectric properties of LindashZn ferritesrdquo Solid StateCommunications vol 148 no 9-10 pp 399ndash402 2008
[36] S T Assar and H F Aboshiesha ldquoStructure and magneticproperties of CondashNindashLi ferrites synthesized by citrate precursormethodrdquo Journal ofMagnetism andMagneticMaterials vol 324no 22 pp 3846ndash3852 2012
[37] C G Koops ldquoOn the dispersion of resistivity and dielectricconstant of some semiconductors at audiofrequenciesrdquo PhysicalReview vol 83 article 121 1951
[38] K L Yadav andRN P Choudary ldquoStudy of structural electricaland optical properties of lead free based ceramic systemrdquoJournal of Materials Science Letters vol 19 p 61 1994
[39] V Verma V Pandey V N Shukla S Annapoorni and R KKotnala ldquoRemarkable influence on the dielectric and magneticproperties of lithium ferrite by Ti and Zn substitutionrdquo SolidState Communications vol 149 no 39-40 pp 1726ndash1730 2009
Submit your manuscripts athttpwwwhindawicom
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
High Energy PhysicsAdvances in
The Scientific World JournalHindawi Publishing Corporation httpwwwhindawicom Volume 2014
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FluidsJournal of
Atomic and Molecular Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Advances in Condensed Matter Physics
OpticsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstronomyAdvances in
International Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Superconductivity
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Statistical MechanicsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
GravityJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstrophysicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Physics Research International
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Solid State PhysicsJournal of
Computational Methods in Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Soft MatterJournal of
Hindawi Publishing Corporationhttpwwwhindawicom
AerodynamicsJournal of
Volume 2014
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PhotonicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Journal of
Biophysics
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
ThermodynamicsJournal of
Physics Research International 7
510152025303540
Temperature (K)
5
10
15
20
25
30
0
20
40
60
80
100
120
020406080
100120140
0
20
40
60
80
100
020406080
100120140
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Die
lect
ric co
nsta
nt (120576
998400times10
2)
75 kHz
75 kHz75 kHz 75 kHz
75 kHz
75 kHz
30kHz
30kHz30kHz 30kHz
30kHz
30kHz600kHz
600kHz600kHz
600kHz
600kHz
600kHz1MHz
1MHz1MHz
1MHz
1MHz
1MHz3MHz
3MHz 3MHz3MHz
3MHz
3MHz5MHz
5MHz5MHz
5MHz
5MHz
5MHz
300 400 500 600 700 800
Temperature (K) Temperature (K)300 400 500 600 700 800 300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
(a)
minus0100010203040506070809
Temperature (K)
0005101520253035
minus02000204060810121416
minus02000204060810121416
0002040608101214161820
minus0200020406081012
x = 00 x = 02 x = 04
x = 06 x = 08 x = 10
300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
Temperature (K)300 400 500 600 700 800
750Hz
750Hz 750Hz
750Hz
750Hz 750Hz
3kHz
3kHz3kHz
3kHz
3kHz
3kHz
100 kHz
100 kHz100 kHz
100 kHz
100 kHz
100 kHz
1MHz
1MHz1MHz
1MHz
1MHz
1MHz
3MHz
3MHz3MHz
3MHz
3MHz
3MHz
5MHz
5MHz
5MHz
5MHz
5MHz
5MHz
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 5 (a)Variation of dielectric constant (1205761015840)with temperature at different frequencies of Li05minus05xNixFe25minus05xO4 nanoferrites (b)Variation
of loss tangent (tan 120575) with temperature at different frequencies of Li05minus05xNixFe25minus05xO4 nanoferrites
the ferrites It is observed that there are four major con-tributions for polarisation in ferrites They are electronicatomic dipolar and interfacial polarisations [33] Electronicand atomic polarisations are important at high frequenciesand are independent of temperature while remaining two are
important at lower frequencies and dependent on tempera-ture By increasing the temperature interfacial polarisationis increased and dipolar polarisation decreases The increasein dielectric constant with increase in temperature at lowfrequency may be due to the interfacial polarisation
8 Physics Research International
6
7
8
9
10
11
12
13
14
Ni composition
750Hz and 323K
Die
lect
ric co
nsta
nt (120576
998400 )times10
2
00 02 04 06 08 10
(a)
000
002
004
006
008
010 750Hz and 323K
Ni composition00 02 04 06 08 10
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 6 Variation of dielectric constant (1205761015840) and tan 120575 with Ni concentration
From Figure 5(a) it can be noticed that the dielectricconstant (1205761015840) values increase rapidly in the low temperaturerange (119879 lt 600K) whereas in the high temperaturerange (119879 gt 600K) dielectric constant (1205761015840) reaches a stablevalue (Resonance peak) after that it starts to decrease withincreasing the temperature For the low temperature range(119879 lt 600K) the polarisation is increased by the electricfield and also by increasing the number of charge carriers(electrons) which are increased with temperature hence theincrease in the dielectric constant (1205761015840) at low temperaturerange (119879 lt 600K) is due to increase in both temperatureand frequency For the high temperature range (119879 gt 600K)the saturation in the generation of charge carriers is reachedTherefore the electron exchange between the ions of the sameelement that are present in more than one valence state (Fe+2Fe+3 orNi+2 Ni+1) cannot follow the field variation and hencedielectric constant decreases [34] The temperature at whichthe resonance peak appeared is observed to be shifted towardsthe higher temperature as the frequency is increased [35]The variation of loss angle tangent (tan 120575) of the preparedsample as a function temperature at different frequencies hasalso been investigated and an increase is observed just as thedielectric constant (1205761015840) curve This variation of loss tangentwith temperature curve can be understood on the basis ofDebyersquos equation for loss given as [33]
The compositional dependence (Ni concentration) of thedielectric constant (1205761015840) and dielectric loss tangent (tan 120575) ofprepared samples at 323K and at 75 kHz is shown in Figure 6It can be observed that the dielectric constant (1205761015840) value ofthe prepared samples was increased from 119909 = 00 to 119909 =06 and then decreased It can be attributed to the effect ofsimultaneous contributions of different factors such as grainsize density porosity and cation distribution The initialincrease in dielectric constant (1205761015840) when Ni content increasesfrom 119909 = 00 to 119909 = 06 coincides with the increase ofgrain size from Table 1 [36] After that the cation distribution
becomes the predominant factor in decreasing the dielectricconstant (1205761015840) with Ni content since the decrease of holehoping becomes greater than the increase of electron hopingin the B-sites For the same reasons it can be observed thatthe variation of loss tangent of the prepared samples withNi content has almost the same trend in inverse mannerFrom all these results it can be concluded that doping ofLi nanoferrites with Ni ions leads to improvement in theirdielectrical properties especially in the sample at 119909 = 06 andthese compositions make promising materials for microwaveapplications
The variation of dielectric constant (1205761015840) and dielectric losstangent (tan 120575) of prepared samples at 119909 = 04with frequencyat different temperatures has been investigated in Figure 7
It is observed that dielectric constant (1205761015840) of preparedsamples was decreased rapidly in the low frequency regionand decrease is quite slow in the high frequency regionthat is dielectric constant is almost independent of fre-quency (shown in Figure 7(a)) This dielectric behaviour offerrites was explained by Koopsrsquo theory [37] According tothis model dielectric medium is assumed to be made upof highly conducting grains surrounded by nonconductinggrain boundaries The grain boundaries are more effectiveat low frequencies and grains are more effective at thehigher frequencies As the grain boundaries having the largeresistance the charge carriers (electrons) pile up there andproduce large space charge polarisation which results in largevalue of dielectric constant at low frequency region Andfurther increasing the frequency the charge carriers (elec-trons) change their direction of motion due to the factthat this accumulation of charge at the grain boundarydecreases which results in the decrease of dielectric constantFrom the figures it is also observed that dielectric constantvalues increase with increase in the temperature in the lowfrequency region because electron exchange between the Fe+2and Fe+3 ions at octahedral sites was thermally activated
Physics Research International 9
15
30
45
60
75
90
105
120x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Log f (Hz)
(a)
00
02
04
06
08
10
12
14
16x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric lo
ss (t
an 120575)
Log f (Hz)
(b)
Figure 7 The variation of dielectric constant (1205761015840) and (tan 120575) with frequency at different temperatures of the LindashNi ferrite system at 119909 = 04
Figure 7(b) shows the variation dielectric loss tangent(tan 120575) with frequencies at different temperatures for 119909 = 04It is observed that the dielectric loss decreases with frequencybecause the jumping frequency of charge carriers cannot fol-low the frequency of the applied field after certain frequency
This figure also shows that the dielectric loss of the pre-pared samples increases with increasing the temperaturebecause of the enhanced hopping of thermally energized elec-trons
Figure 8 shows the variation of dielectric constant at75 kHz with temperature range 323Kndash723K for all ferritesamples It can be observed that the dielectric constant ofall the ferrite samples increases with increasing temperatureup to certain temperature after this temperature dielectricconstant of the prepared samples is going to decrease thattemperature is known as dielectric transition temperature119879119889[38] The decrease in the value of dielectric constant
takes place when the jumping frequency of the electronscannot follow the frequency of the applied electric field FromFigure 8 it is observed that dielectric transition temperature119879119889range is found to be in the 600Kndash680K for all prepared
samples of Li05minus05xNixFe25minus05xO4 system [39] It is also
observed that the slope variation in theArrhenius plots (otherthan Curie point) was in the same temperature range only forall samples
4 Conclusions
All the LindashNi ferrites samples prepared by low temperatureautocombustion method and single phase were confirmedthroughXRD analysisThe experimental results revealed thatthe lattice parameter X-ray density of the prepared ferrite
0
20
40
60
80
100
120
140
Temperature (K)
Data1 ln00Data1 LN02
Data1 LN04
Data1 LN06
Data1 LN08
Data1 LN10
300 400 500 600 700 800
120576998400times10
2
Figure 8 The variation of dielectric constant with temp forLi05minus05xNixFe25minus05xO4 nanoferrites
samples increases with increase in Ni-substituted concen-tration and the grain size is also in the nm range only DCelectrical resistivity of the prepared samples decreases withincreasing in the temperature which shows the semiconduct-ing behaviour of nanoferrites It is observed that the dis-continuity in the log(120590119879) versus 1000119879 graph shows Curiepoint of the prepared ferrite samples Curie temperature of
10 Physics Research International
the prepared LindashNi ferrites decreases with the increase ofthe Ni concentration The variation of DC conductivity withtemperature can be explained using the hopping mechanismof electrons between the Fe+2 and Fe+3 The dielectric con-stant of the prepared ferrite samples increases with increasein temperature up to certain temperature and afterwardsdecreases with increase in temperature
Conflict of Interests
The authors declare that there is no conflict of interestsregarding the publication of this paper
Acknowledgments
The authors are very grateful to Professor K Venu GopalReddy Head Department of Physics University College ofScience Osmania University Hyderabad The authors arevery thankful to UGC New Delhi for their financial assis-tance through Major Research Project (MRP)
References
[1] N S Gajbhiye and G Balaji ldquoMossbaur studies of nanosizeCuFe2O4ferritesrdquo in Advances in Nanoscience and Nano Tech
A Sharma Ed NISCAIR 2003[2] S A Jadhav ldquoMagnetic properties of Zn-substituted LindashCu
ferritesrdquo Journal of Magnetism andMagnetic Materials vol 224no 2 pp 167ndash172 2001
[3] M F Al-Hilli S Li and K S Kassim ldquoGadolinium substitutionand sintering temperature dependent electronic properties ofLindashNi ferriterdquo Journal ofMagnetism andMagneticMaterials vol324 pp 873ndash879 2012
[4] AM A El AtaM K El Nimr SM Attia D El Kony andAHAl-Hammadi ldquoStudies of AC electrical conductivity and initialmagnetic permeability of rare-earth-substituted LindashCo ferritesrdquoJournal of Magnetism andMagnetic Materials vol 297 no 1 pp33ndash43 2006
[5] AM A El Ata S M Attia D El Kony and A H Al-HammadildquoSpectral initial magnetic permeability and transport studies ofLi05minus05xCoxFe25minus05xO4 spinel ferriterdquo Journal ofMagnetism and
Magnetic Materials vol 295 no 1 pp 28ndash36 2005[6] S A Jadhav ldquoStructural and magnetic properties of Zn substi-
tuted LindashCu ferritesrdquo Materials Chemistry and Physics vol 65no 1 pp 120ndash123 2000
[7] H Kawazoe and K Ueda ldquoTransparent conducting oxidesbased on the spinel structurerdquo Journal of the American CeramicSociety vol 82 no 12 pp 3330ndash3336 1999
[8] P V Reddy and T S Rao ldquoX-ray studies on lithium-nickeland manganese-magnesiummixed ferritesrdquo Journal of the Less-Common Metals vol 75 no 2 pp 255ndash260 1980
[9] R S Devan Y D Kolekar and B K Chougule ldquoTransitionmetal-doped rare earth vanadates a regenerable catalytic mate-rial for SOFC anodesrdquo Journal of Physics CondensedMatter vol18 no 43 pp 9809ndash9821 2006
[10] M A Gabal and S S Ata-Allah ldquoEffect of diamagnetic substi-tution on the structural electrical and magnetic properties ofCoFe2O4rdquo Materials Chemistry and Physics vol 85 no 1 pp
104ndash112 2004
[11] E VeenaGopalan I A Al-Omari K AMalini et al ldquoImpact ofzinc substitution on the structural and magnetic properties ofchemically derived nanosized manganese zinc mixed ferritesrdquoJournal of Magnetism andMagnetic Materials vol 321 no 8 pp1092ndash1099 2009
[12] E Veena Gopalan K A Malini S Saravanan D Sakthi KumarY Yoshida and M R Anantharaman ldquoEvidence for polaronconduction in nanostructured manganese ferriterdquo Journal ofPhysics D Applied Physics vol 41 no 18 Article ID 1850052008
[13] M Srivastava S Chaubey andAKOjha ldquoInvestigation on sizedependent structural and magnetic behavior of nickel ferritenanoparticles prepared by sol-gel and hydrothermal methodsrdquoMaterials Chemistry and Physics vol 118 no 1 pp 174ndash1802009
[14] S S Bellad R B Pujar and B K Chougule ldquoStructural andmagnetic properties of some mixed LindashCd ferritesrdquo MaterialsChemistry and Physics vol 52 no 2 pp 166ndash169 1998
[15] D Ravinder ldquoDielectric behaviour of mixed lithium-zinc fer-ritesrdquo Journal of Materials Science Letters vol 11 no 22 pp1498ndash1500 1992
[16] Y Purushotham M B Reddy P Kishan D R Sagar and PV Reddy ldquoElectrical conductivity and thermopower studiesof titanium-substituted lithium-magnesium ferritesrdquoMaterialsLetters vol 17 no 6 pp 341ndash345 1993
[17] S A Mazen and T A Elmosalami ldquoStructural and elasticproperties of LindashNi ferritesrdquo ISRN Condensed Matter Physicsvol 2011 Article ID 820726 9 pages 2011
[18] S S Bhatu V K Lakhani A R Tanna et al ldquoEffect of nickelsubstitution on structural infrared and elastic properties oflithium ferriterdquo Indian Journal of Pure and Applied Physics vol45 no 7 pp 596ndash608 2007
[19] L Vijayan R Cheruku G Govindaraj and S Rajagopan ldquoIondynamics in combustion synthesized Na
3Cr2(PO4)3crystal-
litesrdquoMaterials Chemistry and Physics vol 125 no 1-2 pp 184ndash190 2011
[20] R Cheruku L Vijayan and G Govindaraj ldquoElectrical relax-ation studies of solution combustion synthesized nanocrys-talline Li
2NiZrO
4materialrdquo Materials Science and Engineering
B Solid-State Materials for Advanced Technology vol 177 no 11pp 771ndash779 2012
[21] L C Pathak T B Singh S Das A K Verma and P Ramachan-drarao ldquoEffect of pH on the combustion synthesis of nano-crystalline alumina powderrdquoMaterials Letters vol 57 no 2 pp380ndash385 2002
[22] J ChandradassM Balasubramanian andKHKim ldquoSynthesisand characterization of LaAlO
3nanopowders by various fuelsrdquo
Materials andManufacturing Processes vol 25 no 12 pp 1449ndash1453 2010
[23] J Jing L Liangchao and X Feng ldquoStructural analysis andmagnetic properties of Gd-doped LindashNi ferrites prepared usingrheological phase reaction methodrdquo Journal of Rare Earths vol25 no 1 pp 79ndash83 2007
[24] R G Kharabe R S Devan C M Kanamadi and B KChougule ldquoDielectric properties of mixed LindashNindashCd ferritesrdquoSmart Materials and Structures vol 15 no 2 pp N36ndashN392006
[25] F F Y Wang Treatise on Material Science and Technology vol2 Academic Press New York NY USA 1973
[26] R W Cahn Physical Mettaliurgy vol 1 North Holland Ams-terdam The Netherlands 1985
Physics Research International 11
[27] S B Patil R P Patil and B K Chougale ldquoDC electrical andthermo electric power measurement studies of NindashMgndashZnndashCoferritesrdquo Journal of Magnetism andMagnetic Materials vol 335pp 109ndash113 2013
[28] M A El Hiti ldquoStudies of structural electric andmagnetic prop-erties of some mixed ferritesrdquo Journal of Magnetism andMagnetic Materials vol 136 p 138 1994
[29] A N Patil R P Mahajan K K Patankar A K Ghatake andS A Patil ldquoMagnetic and Optical properties of conductionmechanism in Copper ferritesrdquo Indian Journal of Pure andApplied Physics vol 38 article 651 2000
[30] E J W Verwey and J H de Boer ldquoCation arrangement in afew oxides with crystal structures of the spinel typerdquo Recueildes Travaux Chimiques des Pays-Bas vol 55 no 6 pp 531ndash5401936
[31] A Verma T C Goel R GMendiratta and R G Gupta ldquoHigh-resistivity nickel-zinc ferrites by the citrate precursor methodrdquoJournal of Magnetism andMagneticMaterials vol 192 no 2 pp271ndash276 1999
[32] W D Kingery H K Bowen and P R Uhlum Introduction toCeramics Wiley New York NY USA 1975
[33] L L Hench and J K West Principles of Electronic CeramicsJohn Wiley amp Sons New York NY USA 1990
[34] S AMazen andH A Dawoud ldquoTemperature and compositiondependence of dielectric properties in LindashCu ferriterdquoMaterialsChemistry and Physics vol 82 no 3 pp 557ndash566 2003
[35] I Soibam S Phanjoubam H B Sharma H N K SarmaR Laishram and C Prakash ldquoEffects of Cobalt substitutionon the dielectric properties of LindashZn ferritesrdquo Solid StateCommunications vol 148 no 9-10 pp 399ndash402 2008
[36] S T Assar and H F Aboshiesha ldquoStructure and magneticproperties of CondashNindashLi ferrites synthesized by citrate precursormethodrdquo Journal ofMagnetism andMagneticMaterials vol 324no 22 pp 3846ndash3852 2012
[37] C G Koops ldquoOn the dispersion of resistivity and dielectricconstant of some semiconductors at audiofrequenciesrdquo PhysicalReview vol 83 article 121 1951
[38] K L Yadav andRN P Choudary ldquoStudy of structural electricaland optical properties of lead free based ceramic systemrdquoJournal of Materials Science Letters vol 19 p 61 1994
[39] V Verma V Pandey V N Shukla S Annapoorni and R KKotnala ldquoRemarkable influence on the dielectric and magneticproperties of lithium ferrite by Ti and Zn substitutionrdquo SolidState Communications vol 149 no 39-40 pp 1726ndash1730 2009
Submit your manuscripts athttpwwwhindawicom
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
High Energy PhysicsAdvances in
The Scientific World JournalHindawi Publishing Corporation httpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
FluidsJournal of
Atomic and Molecular Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Advances in Condensed Matter Physics
OpticsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstronomyAdvances in
International Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Superconductivity
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Statistical MechanicsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
GravityJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstrophysicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Physics Research International
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Solid State PhysicsJournal of
Computational Methods in Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Soft MatterJournal of
Hindawi Publishing Corporationhttpwwwhindawicom
AerodynamicsJournal of
Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
PhotonicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Journal of
Biophysics
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
ThermodynamicsJournal of
8 Physics Research International
6
7
8
9
10
11
12
13
14
Ni composition
750Hz and 323K
Die
lect
ric co
nsta
nt (120576
998400 )times10
2
00 02 04 06 08 10
(a)
000
002
004
006
008
010 750Hz and 323K
Ni composition00 02 04 06 08 10
Die
lect
ric lo
ss (t
an 120575)
(b)
Figure 6 Variation of dielectric constant (1205761015840) and tan 120575 with Ni concentration
From Figure 5(a) it can be noticed that the dielectricconstant (1205761015840) values increase rapidly in the low temperaturerange (119879 lt 600K) whereas in the high temperaturerange (119879 gt 600K) dielectric constant (1205761015840) reaches a stablevalue (Resonance peak) after that it starts to decrease withincreasing the temperature For the low temperature range(119879 lt 600K) the polarisation is increased by the electricfield and also by increasing the number of charge carriers(electrons) which are increased with temperature hence theincrease in the dielectric constant (1205761015840) at low temperaturerange (119879 lt 600K) is due to increase in both temperatureand frequency For the high temperature range (119879 gt 600K)the saturation in the generation of charge carriers is reachedTherefore the electron exchange between the ions of the sameelement that are present in more than one valence state (Fe+2Fe+3 orNi+2 Ni+1) cannot follow the field variation and hencedielectric constant decreases [34] The temperature at whichthe resonance peak appeared is observed to be shifted towardsthe higher temperature as the frequency is increased [35]The variation of loss angle tangent (tan 120575) of the preparedsample as a function temperature at different frequencies hasalso been investigated and an increase is observed just as thedielectric constant (1205761015840) curve This variation of loss tangentwith temperature curve can be understood on the basis ofDebyersquos equation for loss given as [33]
The compositional dependence (Ni concentration) of thedielectric constant (1205761015840) and dielectric loss tangent (tan 120575) ofprepared samples at 323K and at 75 kHz is shown in Figure 6It can be observed that the dielectric constant (1205761015840) value ofthe prepared samples was increased from 119909 = 00 to 119909 =06 and then decreased It can be attributed to the effect ofsimultaneous contributions of different factors such as grainsize density porosity and cation distribution The initialincrease in dielectric constant (1205761015840) when Ni content increasesfrom 119909 = 00 to 119909 = 06 coincides with the increase ofgrain size from Table 1 [36] After that the cation distribution
becomes the predominant factor in decreasing the dielectricconstant (1205761015840) with Ni content since the decrease of holehoping becomes greater than the increase of electron hopingin the B-sites For the same reasons it can be observed thatthe variation of loss tangent of the prepared samples withNi content has almost the same trend in inverse mannerFrom all these results it can be concluded that doping ofLi nanoferrites with Ni ions leads to improvement in theirdielectrical properties especially in the sample at 119909 = 06 andthese compositions make promising materials for microwaveapplications
The variation of dielectric constant (1205761015840) and dielectric losstangent (tan 120575) of prepared samples at 119909 = 04with frequencyat different temperatures has been investigated in Figure 7
It is observed that dielectric constant (1205761015840) of preparedsamples was decreased rapidly in the low frequency regionand decrease is quite slow in the high frequency regionthat is dielectric constant is almost independent of fre-quency (shown in Figure 7(a)) This dielectric behaviour offerrites was explained by Koopsrsquo theory [37] According tothis model dielectric medium is assumed to be made upof highly conducting grains surrounded by nonconductinggrain boundaries The grain boundaries are more effectiveat low frequencies and grains are more effective at thehigher frequencies As the grain boundaries having the largeresistance the charge carriers (electrons) pile up there andproduce large space charge polarisation which results in largevalue of dielectric constant at low frequency region Andfurther increasing the frequency the charge carriers (elec-trons) change their direction of motion due to the factthat this accumulation of charge at the grain boundarydecreases which results in the decrease of dielectric constantFrom the figures it is also observed that dielectric constantvalues increase with increase in the temperature in the lowfrequency region because electron exchange between the Fe+2and Fe+3 ions at octahedral sites was thermally activated
Physics Research International 9
15
30
45
60
75
90
105
120x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Log f (Hz)
(a)
00
02
04
06
08
10
12
14
16x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric lo
ss (t
an 120575)
Log f (Hz)
(b)
Figure 7 The variation of dielectric constant (1205761015840) and (tan 120575) with frequency at different temperatures of the LindashNi ferrite system at 119909 = 04
Figure 7(b) shows the variation dielectric loss tangent(tan 120575) with frequencies at different temperatures for 119909 = 04It is observed that the dielectric loss decreases with frequencybecause the jumping frequency of charge carriers cannot fol-low the frequency of the applied field after certain frequency
This figure also shows that the dielectric loss of the pre-pared samples increases with increasing the temperaturebecause of the enhanced hopping of thermally energized elec-trons
Figure 8 shows the variation of dielectric constant at75 kHz with temperature range 323Kndash723K for all ferritesamples It can be observed that the dielectric constant ofall the ferrite samples increases with increasing temperatureup to certain temperature after this temperature dielectricconstant of the prepared samples is going to decrease thattemperature is known as dielectric transition temperature119879119889[38] The decrease in the value of dielectric constant
takes place when the jumping frequency of the electronscannot follow the frequency of the applied electric field FromFigure 8 it is observed that dielectric transition temperature119879119889range is found to be in the 600Kndash680K for all prepared
samples of Li05minus05xNixFe25minus05xO4 system [39] It is also
observed that the slope variation in theArrhenius plots (otherthan Curie point) was in the same temperature range only forall samples
4 Conclusions
All the LindashNi ferrites samples prepared by low temperatureautocombustion method and single phase were confirmedthroughXRD analysisThe experimental results revealed thatthe lattice parameter X-ray density of the prepared ferrite
0
20
40
60
80
100
120
140
Temperature (K)
Data1 ln00Data1 LN02
Data1 LN04
Data1 LN06
Data1 LN08
Data1 LN10
300 400 500 600 700 800
120576998400times10
2
Figure 8 The variation of dielectric constant with temp forLi05minus05xNixFe25minus05xO4 nanoferrites
samples increases with increase in Ni-substituted concen-tration and the grain size is also in the nm range only DCelectrical resistivity of the prepared samples decreases withincreasing in the temperature which shows the semiconduct-ing behaviour of nanoferrites It is observed that the dis-continuity in the log(120590119879) versus 1000119879 graph shows Curiepoint of the prepared ferrite samples Curie temperature of
10 Physics Research International
the prepared LindashNi ferrites decreases with the increase ofthe Ni concentration The variation of DC conductivity withtemperature can be explained using the hopping mechanismof electrons between the Fe+2 and Fe+3 The dielectric con-stant of the prepared ferrite samples increases with increasein temperature up to certain temperature and afterwardsdecreases with increase in temperature
Conflict of Interests
The authors declare that there is no conflict of interestsregarding the publication of this paper
Acknowledgments
The authors are very grateful to Professor K Venu GopalReddy Head Department of Physics University College ofScience Osmania University Hyderabad The authors arevery thankful to UGC New Delhi for their financial assis-tance through Major Research Project (MRP)
References
[1] N S Gajbhiye and G Balaji ldquoMossbaur studies of nanosizeCuFe2O4ferritesrdquo in Advances in Nanoscience and Nano Tech
A Sharma Ed NISCAIR 2003[2] S A Jadhav ldquoMagnetic properties of Zn-substituted LindashCu
ferritesrdquo Journal of Magnetism andMagnetic Materials vol 224no 2 pp 167ndash172 2001
[3] M F Al-Hilli S Li and K S Kassim ldquoGadolinium substitutionand sintering temperature dependent electronic properties ofLindashNi ferriterdquo Journal ofMagnetism andMagneticMaterials vol324 pp 873ndash879 2012
[4] AM A El AtaM K El Nimr SM Attia D El Kony andAHAl-Hammadi ldquoStudies of AC electrical conductivity and initialmagnetic permeability of rare-earth-substituted LindashCo ferritesrdquoJournal of Magnetism andMagnetic Materials vol 297 no 1 pp33ndash43 2006
[5] AM A El Ata S M Attia D El Kony and A H Al-HammadildquoSpectral initial magnetic permeability and transport studies ofLi05minus05xCoxFe25minus05xO4 spinel ferriterdquo Journal ofMagnetism and
Magnetic Materials vol 295 no 1 pp 28ndash36 2005[6] S A Jadhav ldquoStructural and magnetic properties of Zn substi-
tuted LindashCu ferritesrdquo Materials Chemistry and Physics vol 65no 1 pp 120ndash123 2000
[7] H Kawazoe and K Ueda ldquoTransparent conducting oxidesbased on the spinel structurerdquo Journal of the American CeramicSociety vol 82 no 12 pp 3330ndash3336 1999
[8] P V Reddy and T S Rao ldquoX-ray studies on lithium-nickeland manganese-magnesiummixed ferritesrdquo Journal of the Less-Common Metals vol 75 no 2 pp 255ndash260 1980
[9] R S Devan Y D Kolekar and B K Chougule ldquoTransitionmetal-doped rare earth vanadates a regenerable catalytic mate-rial for SOFC anodesrdquo Journal of Physics CondensedMatter vol18 no 43 pp 9809ndash9821 2006
[10] M A Gabal and S S Ata-Allah ldquoEffect of diamagnetic substi-tution on the structural electrical and magnetic properties ofCoFe2O4rdquo Materials Chemistry and Physics vol 85 no 1 pp
104ndash112 2004
[11] E VeenaGopalan I A Al-Omari K AMalini et al ldquoImpact ofzinc substitution on the structural and magnetic properties ofchemically derived nanosized manganese zinc mixed ferritesrdquoJournal of Magnetism andMagnetic Materials vol 321 no 8 pp1092ndash1099 2009
[12] E Veena Gopalan K A Malini S Saravanan D Sakthi KumarY Yoshida and M R Anantharaman ldquoEvidence for polaronconduction in nanostructured manganese ferriterdquo Journal ofPhysics D Applied Physics vol 41 no 18 Article ID 1850052008
[13] M Srivastava S Chaubey andAKOjha ldquoInvestigation on sizedependent structural and magnetic behavior of nickel ferritenanoparticles prepared by sol-gel and hydrothermal methodsrdquoMaterials Chemistry and Physics vol 118 no 1 pp 174ndash1802009
[14] S S Bellad R B Pujar and B K Chougule ldquoStructural andmagnetic properties of some mixed LindashCd ferritesrdquo MaterialsChemistry and Physics vol 52 no 2 pp 166ndash169 1998
[15] D Ravinder ldquoDielectric behaviour of mixed lithium-zinc fer-ritesrdquo Journal of Materials Science Letters vol 11 no 22 pp1498ndash1500 1992
[16] Y Purushotham M B Reddy P Kishan D R Sagar and PV Reddy ldquoElectrical conductivity and thermopower studiesof titanium-substituted lithium-magnesium ferritesrdquoMaterialsLetters vol 17 no 6 pp 341ndash345 1993
[17] S A Mazen and T A Elmosalami ldquoStructural and elasticproperties of LindashNi ferritesrdquo ISRN Condensed Matter Physicsvol 2011 Article ID 820726 9 pages 2011
[18] S S Bhatu V K Lakhani A R Tanna et al ldquoEffect of nickelsubstitution on structural infrared and elastic properties oflithium ferriterdquo Indian Journal of Pure and Applied Physics vol45 no 7 pp 596ndash608 2007
[19] L Vijayan R Cheruku G Govindaraj and S Rajagopan ldquoIondynamics in combustion synthesized Na
3Cr2(PO4)3crystal-
litesrdquoMaterials Chemistry and Physics vol 125 no 1-2 pp 184ndash190 2011
[20] R Cheruku L Vijayan and G Govindaraj ldquoElectrical relax-ation studies of solution combustion synthesized nanocrys-talline Li
2NiZrO
4materialrdquo Materials Science and Engineering
B Solid-State Materials for Advanced Technology vol 177 no 11pp 771ndash779 2012
[21] L C Pathak T B Singh S Das A K Verma and P Ramachan-drarao ldquoEffect of pH on the combustion synthesis of nano-crystalline alumina powderrdquoMaterials Letters vol 57 no 2 pp380ndash385 2002
[22] J ChandradassM Balasubramanian andKHKim ldquoSynthesisand characterization of LaAlO
3nanopowders by various fuelsrdquo
Materials andManufacturing Processes vol 25 no 12 pp 1449ndash1453 2010
[23] J Jing L Liangchao and X Feng ldquoStructural analysis andmagnetic properties of Gd-doped LindashNi ferrites prepared usingrheological phase reaction methodrdquo Journal of Rare Earths vol25 no 1 pp 79ndash83 2007
[24] R G Kharabe R S Devan C M Kanamadi and B KChougule ldquoDielectric properties of mixed LindashNindashCd ferritesrdquoSmart Materials and Structures vol 15 no 2 pp N36ndashN392006
[25] F F Y Wang Treatise on Material Science and Technology vol2 Academic Press New York NY USA 1973
[26] R W Cahn Physical Mettaliurgy vol 1 North Holland Ams-terdam The Netherlands 1985
Physics Research International 11
[27] S B Patil R P Patil and B K Chougale ldquoDC electrical andthermo electric power measurement studies of NindashMgndashZnndashCoferritesrdquo Journal of Magnetism andMagnetic Materials vol 335pp 109ndash113 2013
[28] M A El Hiti ldquoStudies of structural electric andmagnetic prop-erties of some mixed ferritesrdquo Journal of Magnetism andMagnetic Materials vol 136 p 138 1994
[29] A N Patil R P Mahajan K K Patankar A K Ghatake andS A Patil ldquoMagnetic and Optical properties of conductionmechanism in Copper ferritesrdquo Indian Journal of Pure andApplied Physics vol 38 article 651 2000
[30] E J W Verwey and J H de Boer ldquoCation arrangement in afew oxides with crystal structures of the spinel typerdquo Recueildes Travaux Chimiques des Pays-Bas vol 55 no 6 pp 531ndash5401936
[31] A Verma T C Goel R GMendiratta and R G Gupta ldquoHigh-resistivity nickel-zinc ferrites by the citrate precursor methodrdquoJournal of Magnetism andMagneticMaterials vol 192 no 2 pp271ndash276 1999
[32] W D Kingery H K Bowen and P R Uhlum Introduction toCeramics Wiley New York NY USA 1975
[33] L L Hench and J K West Principles of Electronic CeramicsJohn Wiley amp Sons New York NY USA 1990
[34] S AMazen andH A Dawoud ldquoTemperature and compositiondependence of dielectric properties in LindashCu ferriterdquoMaterialsChemistry and Physics vol 82 no 3 pp 557ndash566 2003
[35] I Soibam S Phanjoubam H B Sharma H N K SarmaR Laishram and C Prakash ldquoEffects of Cobalt substitutionon the dielectric properties of LindashZn ferritesrdquo Solid StateCommunications vol 148 no 9-10 pp 399ndash402 2008
[36] S T Assar and H F Aboshiesha ldquoStructure and magneticproperties of CondashNindashLi ferrites synthesized by citrate precursormethodrdquo Journal ofMagnetism andMagneticMaterials vol 324no 22 pp 3846ndash3852 2012
[37] C G Koops ldquoOn the dispersion of resistivity and dielectricconstant of some semiconductors at audiofrequenciesrdquo PhysicalReview vol 83 article 121 1951
[38] K L Yadav andRN P Choudary ldquoStudy of structural electricaland optical properties of lead free based ceramic systemrdquoJournal of Materials Science Letters vol 19 p 61 1994
[39] V Verma V Pandey V N Shukla S Annapoorni and R KKotnala ldquoRemarkable influence on the dielectric and magneticproperties of lithium ferrite by Ti and Zn substitutionrdquo SolidState Communications vol 149 no 39-40 pp 1726ndash1730 2009
Submit your manuscripts athttpwwwhindawicom
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
High Energy PhysicsAdvances in
The Scientific World JournalHindawi Publishing Corporation httpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
FluidsJournal of
Atomic and Molecular Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Advances in Condensed Matter Physics
OpticsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstronomyAdvances in
International Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Superconductivity
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Statistical MechanicsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
GravityJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstrophysicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Physics Research International
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Solid State PhysicsJournal of
Computational Methods in Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Soft MatterJournal of
Hindawi Publishing Corporationhttpwwwhindawicom
AerodynamicsJournal of
Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
PhotonicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Journal of
Biophysics
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
ThermodynamicsJournal of
Physics Research International 9
15
30
45
60
75
90
105
120x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric co
nsta
nt (120576
998400times10
2)
Log f (Hz)
(a)
00
02
04
06
08
10
12
14
16x = 04
T100
T200T300
T350
T400
T450
100 k 1M
Die
lect
ric lo
ss (t
an 120575)
Log f (Hz)
(b)
Figure 7 The variation of dielectric constant (1205761015840) and (tan 120575) with frequency at different temperatures of the LindashNi ferrite system at 119909 = 04
Figure 7(b) shows the variation dielectric loss tangent(tan 120575) with frequencies at different temperatures for 119909 = 04It is observed that the dielectric loss decreases with frequencybecause the jumping frequency of charge carriers cannot fol-low the frequency of the applied field after certain frequency
This figure also shows that the dielectric loss of the pre-pared samples increases with increasing the temperaturebecause of the enhanced hopping of thermally energized elec-trons
Figure 8 shows the variation of dielectric constant at75 kHz with temperature range 323Kndash723K for all ferritesamples It can be observed that the dielectric constant ofall the ferrite samples increases with increasing temperatureup to certain temperature after this temperature dielectricconstant of the prepared samples is going to decrease thattemperature is known as dielectric transition temperature119879119889[38] The decrease in the value of dielectric constant
takes place when the jumping frequency of the electronscannot follow the frequency of the applied electric field FromFigure 8 it is observed that dielectric transition temperature119879119889range is found to be in the 600Kndash680K for all prepared
samples of Li05minus05xNixFe25minus05xO4 system [39] It is also
observed that the slope variation in theArrhenius plots (otherthan Curie point) was in the same temperature range only forall samples
4 Conclusions
All the LindashNi ferrites samples prepared by low temperatureautocombustion method and single phase were confirmedthroughXRD analysisThe experimental results revealed thatthe lattice parameter X-ray density of the prepared ferrite
0
20
40
60
80
100
120
140
Temperature (K)
Data1 ln00Data1 LN02
Data1 LN04
Data1 LN06
Data1 LN08
Data1 LN10
300 400 500 600 700 800
120576998400times10
2
Figure 8 The variation of dielectric constant with temp forLi05minus05xNixFe25minus05xO4 nanoferrites
samples increases with increase in Ni-substituted concen-tration and the grain size is also in the nm range only DCelectrical resistivity of the prepared samples decreases withincreasing in the temperature which shows the semiconduct-ing behaviour of nanoferrites It is observed that the dis-continuity in the log(120590119879) versus 1000119879 graph shows Curiepoint of the prepared ferrite samples Curie temperature of
10 Physics Research International
the prepared LindashNi ferrites decreases with the increase ofthe Ni concentration The variation of DC conductivity withtemperature can be explained using the hopping mechanismof electrons between the Fe+2 and Fe+3 The dielectric con-stant of the prepared ferrite samples increases with increasein temperature up to certain temperature and afterwardsdecreases with increase in temperature
Conflict of Interests
The authors declare that there is no conflict of interestsregarding the publication of this paper
Acknowledgments
The authors are very grateful to Professor K Venu GopalReddy Head Department of Physics University College ofScience Osmania University Hyderabad The authors arevery thankful to UGC New Delhi for their financial assis-tance through Major Research Project (MRP)
References
[1] N S Gajbhiye and G Balaji ldquoMossbaur studies of nanosizeCuFe2O4ferritesrdquo in Advances in Nanoscience and Nano Tech
A Sharma Ed NISCAIR 2003[2] S A Jadhav ldquoMagnetic properties of Zn-substituted LindashCu
ferritesrdquo Journal of Magnetism andMagnetic Materials vol 224no 2 pp 167ndash172 2001
[3] M F Al-Hilli S Li and K S Kassim ldquoGadolinium substitutionand sintering temperature dependent electronic properties ofLindashNi ferriterdquo Journal ofMagnetism andMagneticMaterials vol324 pp 873ndash879 2012
[4] AM A El AtaM K El Nimr SM Attia D El Kony andAHAl-Hammadi ldquoStudies of AC electrical conductivity and initialmagnetic permeability of rare-earth-substituted LindashCo ferritesrdquoJournal of Magnetism andMagnetic Materials vol 297 no 1 pp33ndash43 2006
[5] AM A El Ata S M Attia D El Kony and A H Al-HammadildquoSpectral initial magnetic permeability and transport studies ofLi05minus05xCoxFe25minus05xO4 spinel ferriterdquo Journal ofMagnetism and
Magnetic Materials vol 295 no 1 pp 28ndash36 2005[6] S A Jadhav ldquoStructural and magnetic properties of Zn substi-
tuted LindashCu ferritesrdquo Materials Chemistry and Physics vol 65no 1 pp 120ndash123 2000
[7] H Kawazoe and K Ueda ldquoTransparent conducting oxidesbased on the spinel structurerdquo Journal of the American CeramicSociety vol 82 no 12 pp 3330ndash3336 1999
[8] P V Reddy and T S Rao ldquoX-ray studies on lithium-nickeland manganese-magnesiummixed ferritesrdquo Journal of the Less-Common Metals vol 75 no 2 pp 255ndash260 1980
[9] R S Devan Y D Kolekar and B K Chougule ldquoTransitionmetal-doped rare earth vanadates a regenerable catalytic mate-rial for SOFC anodesrdquo Journal of Physics CondensedMatter vol18 no 43 pp 9809ndash9821 2006
[10] M A Gabal and S S Ata-Allah ldquoEffect of diamagnetic substi-tution on the structural electrical and magnetic properties ofCoFe2O4rdquo Materials Chemistry and Physics vol 85 no 1 pp
104ndash112 2004
[11] E VeenaGopalan I A Al-Omari K AMalini et al ldquoImpact ofzinc substitution on the structural and magnetic properties ofchemically derived nanosized manganese zinc mixed ferritesrdquoJournal of Magnetism andMagnetic Materials vol 321 no 8 pp1092ndash1099 2009
[12] E Veena Gopalan K A Malini S Saravanan D Sakthi KumarY Yoshida and M R Anantharaman ldquoEvidence for polaronconduction in nanostructured manganese ferriterdquo Journal ofPhysics D Applied Physics vol 41 no 18 Article ID 1850052008
[13] M Srivastava S Chaubey andAKOjha ldquoInvestigation on sizedependent structural and magnetic behavior of nickel ferritenanoparticles prepared by sol-gel and hydrothermal methodsrdquoMaterials Chemistry and Physics vol 118 no 1 pp 174ndash1802009
[14] S S Bellad R B Pujar and B K Chougule ldquoStructural andmagnetic properties of some mixed LindashCd ferritesrdquo MaterialsChemistry and Physics vol 52 no 2 pp 166ndash169 1998
[15] D Ravinder ldquoDielectric behaviour of mixed lithium-zinc fer-ritesrdquo Journal of Materials Science Letters vol 11 no 22 pp1498ndash1500 1992
[16] Y Purushotham M B Reddy P Kishan D R Sagar and PV Reddy ldquoElectrical conductivity and thermopower studiesof titanium-substituted lithium-magnesium ferritesrdquoMaterialsLetters vol 17 no 6 pp 341ndash345 1993
[17] S A Mazen and T A Elmosalami ldquoStructural and elasticproperties of LindashNi ferritesrdquo ISRN Condensed Matter Physicsvol 2011 Article ID 820726 9 pages 2011
[18] S S Bhatu V K Lakhani A R Tanna et al ldquoEffect of nickelsubstitution on structural infrared and elastic properties oflithium ferriterdquo Indian Journal of Pure and Applied Physics vol45 no 7 pp 596ndash608 2007
[19] L Vijayan R Cheruku G Govindaraj and S Rajagopan ldquoIondynamics in combustion synthesized Na
3Cr2(PO4)3crystal-
litesrdquoMaterials Chemistry and Physics vol 125 no 1-2 pp 184ndash190 2011
[20] R Cheruku L Vijayan and G Govindaraj ldquoElectrical relax-ation studies of solution combustion synthesized nanocrys-talline Li
2NiZrO
4materialrdquo Materials Science and Engineering
B Solid-State Materials for Advanced Technology vol 177 no 11pp 771ndash779 2012
[21] L C Pathak T B Singh S Das A K Verma and P Ramachan-drarao ldquoEffect of pH on the combustion synthesis of nano-crystalline alumina powderrdquoMaterials Letters vol 57 no 2 pp380ndash385 2002
[22] J ChandradassM Balasubramanian andKHKim ldquoSynthesisand characterization of LaAlO
3nanopowders by various fuelsrdquo
Materials andManufacturing Processes vol 25 no 12 pp 1449ndash1453 2010
[23] J Jing L Liangchao and X Feng ldquoStructural analysis andmagnetic properties of Gd-doped LindashNi ferrites prepared usingrheological phase reaction methodrdquo Journal of Rare Earths vol25 no 1 pp 79ndash83 2007
[24] R G Kharabe R S Devan C M Kanamadi and B KChougule ldquoDielectric properties of mixed LindashNindashCd ferritesrdquoSmart Materials and Structures vol 15 no 2 pp N36ndashN392006
[25] F F Y Wang Treatise on Material Science and Technology vol2 Academic Press New York NY USA 1973
[26] R W Cahn Physical Mettaliurgy vol 1 North Holland Ams-terdam The Netherlands 1985
Physics Research International 11
[27] S B Patil R P Patil and B K Chougale ldquoDC electrical andthermo electric power measurement studies of NindashMgndashZnndashCoferritesrdquo Journal of Magnetism andMagnetic Materials vol 335pp 109ndash113 2013
[28] M A El Hiti ldquoStudies of structural electric andmagnetic prop-erties of some mixed ferritesrdquo Journal of Magnetism andMagnetic Materials vol 136 p 138 1994
[29] A N Patil R P Mahajan K K Patankar A K Ghatake andS A Patil ldquoMagnetic and Optical properties of conductionmechanism in Copper ferritesrdquo Indian Journal of Pure andApplied Physics vol 38 article 651 2000
[30] E J W Verwey and J H de Boer ldquoCation arrangement in afew oxides with crystal structures of the spinel typerdquo Recueildes Travaux Chimiques des Pays-Bas vol 55 no 6 pp 531ndash5401936
[31] A Verma T C Goel R GMendiratta and R G Gupta ldquoHigh-resistivity nickel-zinc ferrites by the citrate precursor methodrdquoJournal of Magnetism andMagneticMaterials vol 192 no 2 pp271ndash276 1999
[32] W D Kingery H K Bowen and P R Uhlum Introduction toCeramics Wiley New York NY USA 1975
[33] L L Hench and J K West Principles of Electronic CeramicsJohn Wiley amp Sons New York NY USA 1990
[34] S AMazen andH A Dawoud ldquoTemperature and compositiondependence of dielectric properties in LindashCu ferriterdquoMaterialsChemistry and Physics vol 82 no 3 pp 557ndash566 2003
[35] I Soibam S Phanjoubam H B Sharma H N K SarmaR Laishram and C Prakash ldquoEffects of Cobalt substitutionon the dielectric properties of LindashZn ferritesrdquo Solid StateCommunications vol 148 no 9-10 pp 399ndash402 2008
[36] S T Assar and H F Aboshiesha ldquoStructure and magneticproperties of CondashNindashLi ferrites synthesized by citrate precursormethodrdquo Journal ofMagnetism andMagneticMaterials vol 324no 22 pp 3846ndash3852 2012
[37] C G Koops ldquoOn the dispersion of resistivity and dielectricconstant of some semiconductors at audiofrequenciesrdquo PhysicalReview vol 83 article 121 1951
[38] K L Yadav andRN P Choudary ldquoStudy of structural electricaland optical properties of lead free based ceramic systemrdquoJournal of Materials Science Letters vol 19 p 61 1994
[39] V Verma V Pandey V N Shukla S Annapoorni and R KKotnala ldquoRemarkable influence on the dielectric and magneticproperties of lithium ferrite by Ti and Zn substitutionrdquo SolidState Communications vol 149 no 39-40 pp 1726ndash1730 2009
Submit your manuscripts athttpwwwhindawicom
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
High Energy PhysicsAdvances in
The Scientific World JournalHindawi Publishing Corporation httpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
FluidsJournal of
Atomic and Molecular Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Advances in Condensed Matter Physics
OpticsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstronomyAdvances in
International Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Superconductivity
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Statistical MechanicsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
GravityJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstrophysicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Physics Research International
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Solid State PhysicsJournal of
Computational Methods in Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Soft MatterJournal of
Hindawi Publishing Corporationhttpwwwhindawicom
AerodynamicsJournal of
Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
PhotonicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Journal of
Biophysics
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
ThermodynamicsJournal of
10 Physics Research International
the prepared LindashNi ferrites decreases with the increase ofthe Ni concentration The variation of DC conductivity withtemperature can be explained using the hopping mechanismof electrons between the Fe+2 and Fe+3 The dielectric con-stant of the prepared ferrite samples increases with increasein temperature up to certain temperature and afterwardsdecreases with increase in temperature
Conflict of Interests
The authors declare that there is no conflict of interestsregarding the publication of this paper
Acknowledgments
The authors are very grateful to Professor K Venu GopalReddy Head Department of Physics University College ofScience Osmania University Hyderabad The authors arevery thankful to UGC New Delhi for their financial assis-tance through Major Research Project (MRP)
References
[1] N S Gajbhiye and G Balaji ldquoMossbaur studies of nanosizeCuFe2O4ferritesrdquo in Advances in Nanoscience and Nano Tech
A Sharma Ed NISCAIR 2003[2] S A Jadhav ldquoMagnetic properties of Zn-substituted LindashCu
ferritesrdquo Journal of Magnetism andMagnetic Materials vol 224no 2 pp 167ndash172 2001
[3] M F Al-Hilli S Li and K S Kassim ldquoGadolinium substitutionand sintering temperature dependent electronic properties ofLindashNi ferriterdquo Journal ofMagnetism andMagneticMaterials vol324 pp 873ndash879 2012
[4] AM A El AtaM K El Nimr SM Attia D El Kony andAHAl-Hammadi ldquoStudies of AC electrical conductivity and initialmagnetic permeability of rare-earth-substituted LindashCo ferritesrdquoJournal of Magnetism andMagnetic Materials vol 297 no 1 pp33ndash43 2006
[5] AM A El Ata S M Attia D El Kony and A H Al-HammadildquoSpectral initial magnetic permeability and transport studies ofLi05minus05xCoxFe25minus05xO4 spinel ferriterdquo Journal ofMagnetism and
Magnetic Materials vol 295 no 1 pp 28ndash36 2005[6] S A Jadhav ldquoStructural and magnetic properties of Zn substi-
tuted LindashCu ferritesrdquo Materials Chemistry and Physics vol 65no 1 pp 120ndash123 2000
[7] H Kawazoe and K Ueda ldquoTransparent conducting oxidesbased on the spinel structurerdquo Journal of the American CeramicSociety vol 82 no 12 pp 3330ndash3336 1999
[8] P V Reddy and T S Rao ldquoX-ray studies on lithium-nickeland manganese-magnesiummixed ferritesrdquo Journal of the Less-Common Metals vol 75 no 2 pp 255ndash260 1980
[9] R S Devan Y D Kolekar and B K Chougule ldquoTransitionmetal-doped rare earth vanadates a regenerable catalytic mate-rial for SOFC anodesrdquo Journal of Physics CondensedMatter vol18 no 43 pp 9809ndash9821 2006
[10] M A Gabal and S S Ata-Allah ldquoEffect of diamagnetic substi-tution on the structural electrical and magnetic properties ofCoFe2O4rdquo Materials Chemistry and Physics vol 85 no 1 pp
104ndash112 2004
[11] E VeenaGopalan I A Al-Omari K AMalini et al ldquoImpact ofzinc substitution on the structural and magnetic properties ofchemically derived nanosized manganese zinc mixed ferritesrdquoJournal of Magnetism andMagnetic Materials vol 321 no 8 pp1092ndash1099 2009
[12] E Veena Gopalan K A Malini S Saravanan D Sakthi KumarY Yoshida and M R Anantharaman ldquoEvidence for polaronconduction in nanostructured manganese ferriterdquo Journal ofPhysics D Applied Physics vol 41 no 18 Article ID 1850052008
[13] M Srivastava S Chaubey andAKOjha ldquoInvestigation on sizedependent structural and magnetic behavior of nickel ferritenanoparticles prepared by sol-gel and hydrothermal methodsrdquoMaterials Chemistry and Physics vol 118 no 1 pp 174ndash1802009
[14] S S Bellad R B Pujar and B K Chougule ldquoStructural andmagnetic properties of some mixed LindashCd ferritesrdquo MaterialsChemistry and Physics vol 52 no 2 pp 166ndash169 1998
[15] D Ravinder ldquoDielectric behaviour of mixed lithium-zinc fer-ritesrdquo Journal of Materials Science Letters vol 11 no 22 pp1498ndash1500 1992
[16] Y Purushotham M B Reddy P Kishan D R Sagar and PV Reddy ldquoElectrical conductivity and thermopower studiesof titanium-substituted lithium-magnesium ferritesrdquoMaterialsLetters vol 17 no 6 pp 341ndash345 1993
[17] S A Mazen and T A Elmosalami ldquoStructural and elasticproperties of LindashNi ferritesrdquo ISRN Condensed Matter Physicsvol 2011 Article ID 820726 9 pages 2011
[18] S S Bhatu V K Lakhani A R Tanna et al ldquoEffect of nickelsubstitution on structural infrared and elastic properties oflithium ferriterdquo Indian Journal of Pure and Applied Physics vol45 no 7 pp 596ndash608 2007
[19] L Vijayan R Cheruku G Govindaraj and S Rajagopan ldquoIondynamics in combustion synthesized Na
3Cr2(PO4)3crystal-
litesrdquoMaterials Chemistry and Physics vol 125 no 1-2 pp 184ndash190 2011
[20] R Cheruku L Vijayan and G Govindaraj ldquoElectrical relax-ation studies of solution combustion synthesized nanocrys-talline Li
2NiZrO
4materialrdquo Materials Science and Engineering
B Solid-State Materials for Advanced Technology vol 177 no 11pp 771ndash779 2012
[21] L C Pathak T B Singh S Das A K Verma and P Ramachan-drarao ldquoEffect of pH on the combustion synthesis of nano-crystalline alumina powderrdquoMaterials Letters vol 57 no 2 pp380ndash385 2002
[22] J ChandradassM Balasubramanian andKHKim ldquoSynthesisand characterization of LaAlO
3nanopowders by various fuelsrdquo
Materials andManufacturing Processes vol 25 no 12 pp 1449ndash1453 2010
[23] J Jing L Liangchao and X Feng ldquoStructural analysis andmagnetic properties of Gd-doped LindashNi ferrites prepared usingrheological phase reaction methodrdquo Journal of Rare Earths vol25 no 1 pp 79ndash83 2007
[24] R G Kharabe R S Devan C M Kanamadi and B KChougule ldquoDielectric properties of mixed LindashNindashCd ferritesrdquoSmart Materials and Structures vol 15 no 2 pp N36ndashN392006
[25] F F Y Wang Treatise on Material Science and Technology vol2 Academic Press New York NY USA 1973
[26] R W Cahn Physical Mettaliurgy vol 1 North Holland Ams-terdam The Netherlands 1985
Physics Research International 11
[27] S B Patil R P Patil and B K Chougale ldquoDC electrical andthermo electric power measurement studies of NindashMgndashZnndashCoferritesrdquo Journal of Magnetism andMagnetic Materials vol 335pp 109ndash113 2013
[28] M A El Hiti ldquoStudies of structural electric andmagnetic prop-erties of some mixed ferritesrdquo Journal of Magnetism andMagnetic Materials vol 136 p 138 1994
[29] A N Patil R P Mahajan K K Patankar A K Ghatake andS A Patil ldquoMagnetic and Optical properties of conductionmechanism in Copper ferritesrdquo Indian Journal of Pure andApplied Physics vol 38 article 651 2000
[30] E J W Verwey and J H de Boer ldquoCation arrangement in afew oxides with crystal structures of the spinel typerdquo Recueildes Travaux Chimiques des Pays-Bas vol 55 no 6 pp 531ndash5401936
[31] A Verma T C Goel R GMendiratta and R G Gupta ldquoHigh-resistivity nickel-zinc ferrites by the citrate precursor methodrdquoJournal of Magnetism andMagneticMaterials vol 192 no 2 pp271ndash276 1999
[32] W D Kingery H K Bowen and P R Uhlum Introduction toCeramics Wiley New York NY USA 1975
[33] L L Hench and J K West Principles of Electronic CeramicsJohn Wiley amp Sons New York NY USA 1990
[34] S AMazen andH A Dawoud ldquoTemperature and compositiondependence of dielectric properties in LindashCu ferriterdquoMaterialsChemistry and Physics vol 82 no 3 pp 557ndash566 2003
[35] I Soibam S Phanjoubam H B Sharma H N K SarmaR Laishram and C Prakash ldquoEffects of Cobalt substitutionon the dielectric properties of LindashZn ferritesrdquo Solid StateCommunications vol 148 no 9-10 pp 399ndash402 2008
[36] S T Assar and H F Aboshiesha ldquoStructure and magneticproperties of CondashNindashLi ferrites synthesized by citrate precursormethodrdquo Journal ofMagnetism andMagneticMaterials vol 324no 22 pp 3846ndash3852 2012
[37] C G Koops ldquoOn the dispersion of resistivity and dielectricconstant of some semiconductors at audiofrequenciesrdquo PhysicalReview vol 83 article 121 1951
[38] K L Yadav andRN P Choudary ldquoStudy of structural electricaland optical properties of lead free based ceramic systemrdquoJournal of Materials Science Letters vol 19 p 61 1994
[39] V Verma V Pandey V N Shukla S Annapoorni and R KKotnala ldquoRemarkable influence on the dielectric and magneticproperties of lithium ferrite by Ti and Zn substitutionrdquo SolidState Communications vol 149 no 39-40 pp 1726ndash1730 2009
Submit your manuscripts athttpwwwhindawicom
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
High Energy PhysicsAdvances in
The Scientific World JournalHindawi Publishing Corporation httpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
FluidsJournal of
Atomic and Molecular Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Advances in Condensed Matter Physics
OpticsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstronomyAdvances in
International Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Superconductivity
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Statistical MechanicsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
GravityJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstrophysicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Physics Research International
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Solid State PhysicsJournal of
Computational Methods in Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Soft MatterJournal of
Hindawi Publishing Corporationhttpwwwhindawicom
AerodynamicsJournal of
Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
PhotonicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Journal of
Biophysics
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
ThermodynamicsJournal of
Physics Research International 11
[27] S B Patil R P Patil and B K Chougale ldquoDC electrical andthermo electric power measurement studies of NindashMgndashZnndashCoferritesrdquo Journal of Magnetism andMagnetic Materials vol 335pp 109ndash113 2013
[28] M A El Hiti ldquoStudies of structural electric andmagnetic prop-erties of some mixed ferritesrdquo Journal of Magnetism andMagnetic Materials vol 136 p 138 1994
[29] A N Patil R P Mahajan K K Patankar A K Ghatake andS A Patil ldquoMagnetic and Optical properties of conductionmechanism in Copper ferritesrdquo Indian Journal of Pure andApplied Physics vol 38 article 651 2000
[30] E J W Verwey and J H de Boer ldquoCation arrangement in afew oxides with crystal structures of the spinel typerdquo Recueildes Travaux Chimiques des Pays-Bas vol 55 no 6 pp 531ndash5401936
[31] A Verma T C Goel R GMendiratta and R G Gupta ldquoHigh-resistivity nickel-zinc ferrites by the citrate precursor methodrdquoJournal of Magnetism andMagneticMaterials vol 192 no 2 pp271ndash276 1999
[32] W D Kingery H K Bowen and P R Uhlum Introduction toCeramics Wiley New York NY USA 1975
[33] L L Hench and J K West Principles of Electronic CeramicsJohn Wiley amp Sons New York NY USA 1990
[34] S AMazen andH A Dawoud ldquoTemperature and compositiondependence of dielectric properties in LindashCu ferriterdquoMaterialsChemistry and Physics vol 82 no 3 pp 557ndash566 2003
[35] I Soibam S Phanjoubam H B Sharma H N K SarmaR Laishram and C Prakash ldquoEffects of Cobalt substitutionon the dielectric properties of LindashZn ferritesrdquo Solid StateCommunications vol 148 no 9-10 pp 399ndash402 2008
[36] S T Assar and H F Aboshiesha ldquoStructure and magneticproperties of CondashNindashLi ferrites synthesized by citrate precursormethodrdquo Journal ofMagnetism andMagneticMaterials vol 324no 22 pp 3846ndash3852 2012
[37] C G Koops ldquoOn the dispersion of resistivity and dielectricconstant of some semiconductors at audiofrequenciesrdquo PhysicalReview vol 83 article 121 1951
[38] K L Yadav andRN P Choudary ldquoStudy of structural electricaland optical properties of lead free based ceramic systemrdquoJournal of Materials Science Letters vol 19 p 61 1994
[39] V Verma V Pandey V N Shukla S Annapoorni and R KKotnala ldquoRemarkable influence on the dielectric and magneticproperties of lithium ferrite by Ti and Zn substitutionrdquo SolidState Communications vol 149 no 39-40 pp 1726ndash1730 2009
Submit your manuscripts athttpwwwhindawicom
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
High Energy PhysicsAdvances in
The Scientific World JournalHindawi Publishing Corporation httpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
FluidsJournal of
Atomic and Molecular Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Advances in Condensed Matter Physics
OpticsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstronomyAdvances in
International Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Superconductivity
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Statistical MechanicsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
GravityJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstrophysicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Physics Research International
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Solid State PhysicsJournal of
Computational Methods in Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Soft MatterJournal of
Hindawi Publishing Corporationhttpwwwhindawicom
AerodynamicsJournal of
Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
PhotonicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Journal of
Biophysics
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
ThermodynamicsJournal of
Submit your manuscripts athttpwwwhindawicom
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
High Energy PhysicsAdvances in
The Scientific World JournalHindawi Publishing Corporation httpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
FluidsJournal of
Atomic and Molecular Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Advances in Condensed Matter Physics
OpticsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstronomyAdvances in
International Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Superconductivity
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Statistical MechanicsInternational Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
GravityJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
AstrophysicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Physics Research International
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Solid State PhysicsJournal of
Computational Methods in Physics
Journal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Soft MatterJournal of
Hindawi Publishing Corporationhttpwwwhindawicom
AerodynamicsJournal of
Volume 2014
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
PhotonicsJournal of
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
Journal of
Biophysics
Hindawi Publishing Corporationhttpwwwhindawicom Volume 2014
ThermodynamicsJournal of