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(1)

Spae-Charge-Limited Condution in Thin Film

Al/Sb

2 Pb

1 Se

7

/Al Devies

ShailaWagle and Vinay Shirodkar

SolidState EletronisLaboratory, DepartmentofPhysis,

TheInstituteof Siene,15,MadamCamaRoad,

Mumbai-400032. India

Reeivedon20June,1999. Revisedversionreeivedon10November1999

Thin lm Al/Sb2Pb1Se7/Al, MGM, sandwihed strutures, prepared using thermal evaporation

tehniquehavebeenstudied. TheDCmeasurementsatloweletrieldsuggestthattheeletrial

transportisgovernedbyspaehargelimitedondution(SCLC)mehanism. Thedetailedanalysis

of urrent-voltage limited ondution (SCLC) mehanism harateristis on the basis of SCLC

theory reveals thepresene of uniformlydistributed trap densityof the orderof 10 23

m 3

eV 1

withaverage ativationenergy0.48eV.

I Introdution

Thinlmtehnologyiswellestablishedandwidelyused

in thefabriating ofeletroni devies. Thetehnique

hasbeen suessfullyused to fabriate thin lm

resis-tors, apaitors, photoeletroni devies et.[1,2℄. The

use of this tehnique in fabriating eletroni devies

makesitneessarytounderstandtheeletrial

proper-tiesofthematerialin thinlmform.

In the devie appliations of thin lms, new and

omplex materials are being used and developed and

theireletrialpropertiesarebeingstudied. The

disor-dered materials. partiularly amorphous

semiondu-tors, overing a wide range of ompositions and with

interesting eletrial properties, have been studied in

greater detail[3-5℄. A good amount of work on the

DCondution ofhalogenide/glassymaterialsinthe

form of metal-glass-metal (MGM) struture has been

reported by many researhers[3,6℄. Sine these

mate-rialsare weilknownfor their property to swith from

oneimpedanestatetoanother,whensubjetedtohigh

eld of the order Of 10 6

V/m, most of the reported

work pertains to the eletrial measurements arried

outat highelds. However,itis equallyimportantto

know the behaviour of these materials at low eletri

eldsuptoabout10 4

V/m.

Tothebest ofourknowledgenoattempt hasbeen

madeto studytheloweld DCondution ofvauum

evaporated Sb

2 Pb

1 Se

7

thin lms. In the present

pa-pertherefore, wereport onthe loweld DC

measure-tionmehanisminvauumdepositedSb

2 Pb

1 Se

7 lms.

II Experimental

TheSb

2 Pb

1 Se

7

ompoundusedtofabriatethe

metal-glass-metal, MGM, devies was prepared as follows.

Initially,theweighedquantitiesofhighpurity(5N)Sb,

Pb and Se, taken in their atomi proportions, to give

Sb

2 Pb

1 Se

7

omposition, were rushed and mixed

to-gether. Themixturewasthenintroduedinahigh

pu-rityquartztubelosedatoneendandmadeintoanek

withonstritionattheotherend. Thequartzampoule

wasevauatedto 10 5

mbarandlledagain withdry

argontoinreaseitspressuretoabout10 3

mbar. The

ampoulewassealedatthepointofonstritionand

in-troduedinarokingfurnae. Thetemperatureofthe

furnae wasraisedto 1100 Æ

C and maintainedat that

levelforaboutvehours. Therokingfurnae helped

thoroughly to mix the onstituents in thequartz

am-pouleto form theompound. After ompletion of the

reationthequartzampoulewasallowedtofalldiretly

intoaliquidnitrogenontainer. Theampoulewasthen

brokeopenandglassymassthusobtainedwasrushed

into nepowderandstoredseurelyin adessiator.

The MGM devies were fabriated, on thoroughly

leaned mirosope glass slides, using Edwards Co.

(UK) Turbomoleular pumping station. The working

hamber was tted with Maxtek (USA) lm

deposi-tionontrollermodelFDC-440,whihandisplaylm

(2)

parame-and many suh parameters are fed into the program.

The thiknessof lm wasalso measuredusingDektek

thiknessprolometerand wasfound to be within 1%

ofthedisplayedvaluebytheFDC-440. Thebaseplate

housed aneightsoure turret,while thetopplate was

ttedwithmaskhangerassembly,bothofwhihould

bemonitoredexternallywithoutrequiringtobreakthe

vauum. Theultimateworkingpressureduringthe

de-positionwas510 6

mbar. Initially,aluminiummetal

wasevaporatedand deposited onthe substrate in the

form oftwoparallelstripseah60mmlong,2mm wide

and separated by5mm from eah other. These strips

formed a pair of lower eletrodes. The material was

deposited on the strips through an appropriate mask

to over area of 50mm 15mm, leaving 5mm of the

endportionsofeahaluminiumstrip. Sixounter

ele-trodes,eah2mm wideand20mmlong,perpendiular

to thelowereletrodesweredepositedonthe material

toobtain12MGMdevieseahofarea4mm 2

(seeFigs.

1a and 1b). The entiredeposition sequene was

om-pletedwithoutbreakingthevauumatanystage.This

madeitonvenientrepeatedlytoarryoutallthe

ele-trial measurementsonalm,ofanypartiular

thik-ness, using twelve devies prepared essentially under

idential deposition onditions.

Figure 1. a. Shemativiewof metal-glass-metal devies.

b. Crosssetionalviewofthedevies.

The eletrial measurements on the devies were

arriedoutin vauumusingaryostatwhihouldbe

evauatedto 10 2

mbar pressureduring the

measure-ments. The substratetemperatureinside theryostat

ould be varied from 150 K to 500 K. The

urrent-voltage, I-V, measurements were arried out using a

regulatedpowersupplyonnetedinserieswiththe

de-vie under investigation and astandard resistor. The

urrentthroughthedeviewasalulatedbyaurately

monitoringthepotentialdroparossthestandard

resis-voltage arossthe devie was obtainedasa dierene

between supply voltage and drop arossthe standard

resistor. The seriesresistoralso helpedto preventthe

ow ofexessiveurrentthroughthe devie when the

supplyvoltagewouldovershootaidentally.

III Results and disussion

Fig. 2,urve'a',showsatypialroomtemperatureI-V

urveof Al/Sb

2 Pb

1 Se

7

/AI sample with lm thikness

270nm. Itisseenthattheurveexhibitsahighly

non-linearfeature. Thenon-linearityoftheI-V

harateris-tisindiatesthattheprevalentondutionmehanism

isnon-ohmiinnature.

Figure2. RoomtemperatureI-V.urvea,andlogI V 1=2

,

urveb,harateristisofanMGMdevie withlm

thik-nesses270nm.

It wasobserved during themeasurementsthat the

reported I-V harateristis were reproduible when

ountereletrodewasbiasedwitheitherpolarity. This

indiatedthatthemetal-glassinterfaesatbottomand

topeletrodeswereidentialin nature.

The results shown in gure 2 need to be

are-fullyanalysed,toidentify thepredominantondution

mehanism,sinedierenttypesofondution

meha-nismsan give rise to non-linear harateristis. One

an rst explain observed non-linearity in terms of

Rihardson-Shottky[7℄orPoole-Frenkel[8℄typeof

on-dutionmehanisms. Shottkyemission ours due to

thermalativationofeletronsoverthemetal-insulator

or metal-semiondutor interfae barrier beause of

loweringofbarrierheightduetotheappliedeld. The

(3)

eletrons from traps into the ondution band of the

insulator. In boththeaseslog I vs. v 1=2

harateris-tisareexpetedto belinearin nature. InFig. 2the

urve'b',showslogIvs. v 1=2

harateristisofa

typi-alrepresentativesamplewithlmthikness270nm. It

is seenthat theharateristiurveisstill non- linear

in nature, whih rules out the possibility of existene

of Rihardson Shottky or Poole- Frenkel as possible

ondutionmehanisms.

Theother ondution mehanism,whih gives rise

toahighlynon-linearI-Vharateristis,isthe

spae-harge-limited ondution (SCLC)[9℄, whih is

inu-enedby the traps. However,the exatnature of the

traps presentin thematerial under study depends on

the type of the traps and their position with respet

to the Fermi-level. It is therefore, neessary to apply

this theory veryarefully to explain the experimental

results. In aseof SCLC proessthe detailed features

ofthe non-linearI -V harateristisarerevealed in

log I - log V plot. Fig. 3 shows logarithmi plot of

the I - V harateristis of the devies with dierent

lm thikneses. It is observed that, the urrent

ow-ing throughthe devie dereases with inreasein lm

thikness. However, the natures of theurvesremain

the same. It is seen that the harateristis are

dis-tributedinfourregions(markedAB,BC,CDandDE)

havingdierentslopes,whihimpliesthattheI-V

re-lationisofthetypeI /V n

wherenistheslopeofthe

urve.

Figure3. Log I -log V harateristisof thedevieswith

dierentlmthiknessesat294K.

For verylow voltages (i.e. urveAB) the slope is

equal to unity indiating that the ondution

meha-that in this regionthe urrent isdiretly proportional

totheappliedvoltage.

Intheregion2,urveBC,thevalueof exponentn

is found to be nearly equal to 2.5. This region starts

atapartiularvoltage,V

x

,whihistheendoftherst

region. Thus,atV

x

,theondutionmehanismisboth

OhmiandSCLC.ItisalsonotedfromtheFig. 3that

V

x

inreasesasthiknessinreases.

In the third region, urve CD, the slope inreases

to thevaluemuhlargerthan2. Thisregionisalmost

paralleltotheurrentaxis,indiatingthattheurrent

-voltagerelationfollowsamuh higherpowerlaw. The

transition voltage from seond region to the third

re-gionisdenoted byVTFL,whih inreasesasthikness

inreases.

In the region 4, urve DE, the exponent is again

foundtobe2,indiatingatraPlledSCLC proess.

It is also notied that the slopesof all the regions

areindependentoftheselmthikness.

Fig. 4 shows the log I - log V harateristis at

ve dierent temperatures of a typial representative

sample of lm thikness 270 nm. It is seen that the

natureoftheurvesisessentiallysameasthat,in Fig.

3. It is also seen that as the temperature inreases

urrentthroughthedevieinreasesbutVxandVTFI

derease.

Figure 4. Log I -log Vharateristis ofthedevieswith

thikness270nmatdierenttemperatures.

Itisalsonotiedthattheslopesoftheurvesin

re-gionBCare temperaturedependentsuhthat as

tem-peratureinreasestheslopesdereaseslightly;but the

slopesofregionsAB,CDand DEarepratially

inde-pendentoftemperature.

(4)

sug-MGM devies under present study is governedby the

SCLC mehanism. Therefore, the results of the

mea-surementsonthedevieswithvariousglassthiknesses

andtemperaturesareanalysedonsimillarlinesandare

showntobeonsistentwiththeSCLCmehanism.

Sinevauumevaporatedlmstendtobeamixture

ofamorphousandrystallineregions,oneanexpeta

large onentration of traps distributed in the energy

band-gap [10℄. Therefore, the SCLC phenomenon

ap-propriatetosuhdistributionanbeappliedtodesribe

theondutionintheselms. Astheexatdistribution

oftrapsisdiÆulttopredit,anapproximationstothe

real distributionwasattempted.

TheFigs. 3and4showthattheI-Vharateristis

are governedby the relation I /V n

. Also the plot

showstwodistintross-overvoltages,V

x

representing

transition from Ohmi ondution to the SCLC with

traps, and the V

TFL

, whih is transition from SCLC

with traps to the trap lling level. This implies that

the traps, in the present ase, are situated at energy

levelhigherthanthatoftheFermi-levelofthematerial.

Hene traps are expeted to behave like donors [11℄.

Also, the temperature dependene of the region

sug-gestsapossibilityofexponentialdistributionoftraps.

Lampert hasshown [9℄that the urrent density in

theseondregionisgivenby,

J =

9

8

(K

0 )

V 2

S 3

(1)

where

J =urrentdensityintheseondregion

K =dieletrionstantofthematerial

0

=permittivityoffreespae

=ratiooffreehargearrierstothetrapped

ar-riers

S =thiknessof thelm

=mobilityofthearriers

V =applied bias

Eq. (1) suggeststhat to establishthe existeneof

SCLCaplotoflogIversuslogSshouldyieldastraight

linewithslopeequalto-3. Theurve'a'inFig. 5shows

logI-logSurvegeneratedusingdataofFig. 3

orre-spondingto aonstantvoltagebiasof 0.8V.Itis seen

Figure5. Curvea: Log I-log Sharateristisof the

de-vies.Curveb:LogVx-logSharateristisofthedevies.

Curve : Log VTFI- log S harateristis of the devies.

Temperatureofthedevie=294K.

The transition voltages, V

x and V

TFL

, transition

from Ohmi region to the ondution with tras and

transitionfrom ondution with traps to thetrapfree

ondutionrespetively,aregivenby,

V

x =

8

9

en

0

S 2

(2)

V

TFL =

eQ

TFL S

C =

eQ

TFL

AK

0

S 2

(3)

where

Q

TFL

=hargearriersinjeted atV

TFL

e=eletroni harge

C =apaitaneatV

TFL

A=areaofthedevie

n

0

=freearrierdensity

Eqs. 2and3suggestthattheplotsoflogV

x versus

logS and logV

TFL

versuslog S should yieldstraight

lineswith slope2. Fig. 5,urve'b'giveslog V

X - log

S urve, while urve '' gives log V

TFL

versus log S

plot. Theslopesoftheurvesbandarerespetively,

2.17and1.97whihprovideadditionalsupportforthe

existeneofSCL ondution.

Thetemperaturedependeneoftheurrentdensity,

J,in theseondregionisgivenby[11℄,

j=en

0 Fexp

F

0 K

eN

t kTS

(4)

where

F =eletrield= V

S

N

t

(5)

J

V =

en

0

S

exp

V

0 K

eN

t kTS

2

(5)

) J

V =A

0 exp

V

V

0

(6)

with

A

0 =

en

0

S

(7)

V

0 =

eN

t kTS

2

0 K

(8)

Thus, a plot of log (I=V) versus V should yield a

straightline with slope(1=V

0

) and intereptA

0 . Fig.

6showsthelog (I=V)versusV plots, generatedusmg

thedata of Fig. 3,for thesamples with dierentlm

thiknesses. Fig. 7 shows simillar plots, for various

temperaturesgeneratedusingdataofFig. 4. Itisseen

that, while the slopes of the urves in the Fig. 6

re-main thesame,they dereaseslightlywith inreasein

temperature, as revealed from Fig. 7. The derease

inslope(1=V

o

)withtemperatureimpliesthattheRose

model, [12℄ whih preditsthe natureof trap

distribu-tion anbe applied in the present ase. Using Eq. 7

and interepts of plots in Figs. 6 and 7, trap

densi-ties for various lm thiknesses and temperatures are

omputed. These values are shown in table 1a and

1b respetively. It It is seen that the trap densities

oftheorderof10 23

m 3

eV 1

exist forthepresent

sys-tem. These values are in lose agreement with those

reported for thesimillar disordermaterials.[13,14℄For

highly disorderedmaterialthemagnitude oftrap

den-sity isashigh as10 27

m 3

eV 1

hasbeenobservedfor

vauumdepositedCdSlms.[15℄

Figure6. Log(I/V)-V harateristisofthe devieswith

Figure 7. Log (I/V) - V harateristis of the devies at

dierenttemperatures,lmthikness=270nm.

Table1. Variationoftrapdensitywiththikness,

table(a), andtemperature,table(b).

(a)

Temperature=294K

Thikness N

t (m

3

eV 1

)

nm 10

23

150 6.299

108 4.374

204 3.405

230 2.679

270 1.944

(b)

Thikness=270nm

Temperature N

t (m

3

eV 1

)

K 10

23

294 1.944

304 1.640

309 1.347

319 1.172

329 1.055

Itisfurther seenthat usingequation 7and the

in-tereptsthevaluesforn

0

anbealulatedfrom the

interepts. The interept, log A

0

, is also found to be

a funtion of the mobility of arriers, free eletron

density andthe thiknessof thedevie. Themobility

(6)

=

0 exp

E

t

kT

(9)

where E

t

istheativationenergyofthetraps

Eq. (9)anberewrittenas

n

0 =n

0

0 exp

E

t

kT

(10)

Thus,itispossibletoextratinformationaboutthe

a-tivation energyofthetraps byplottinglog n

0

versus

1/T(Fig. 8). Itisseenthattheplotislinearand,from

the slope, the value of E

t

is alulated to be 0.48eV,

whihistheativationenergyoftraps. Thisvalueisin

loseagreementwiththereportedoneforsimillartype

ofhalogenidematerials[17℄.

Figure 8. Log (n0) -(1/T) harateristis of the devie

withlmthikness270nm.

The distribution of the traps in the devie ould

be either disrete or exponential. Rose [12℄ gives the

urrent voltage relation, whih is in the form I /

V

[(T=T)+1℄

,whereTistheharateristitemperature.

Thus [(T=T)+1℄ isthe slopeof theseond regionof

Fig. 3 whih givesT as 600K. Thus, kT beomes

0.05eV,whihisverysmallomparedtotheaverage

a-tivationenergyofthetrapsdeterminedas0.48eV.This

suggeststhatthedistributionoftrapsisuniformwhih

isexpetedforamorphousorpolyrystallinelms[12℄

IV Conlusions

InthispaperloweldDC harateristisof theMGM

deviesareanalysed. Thedominantondution

meha-nismisidentiedasSCLCproess. Itisfurthershowed

thatthe traps aredistributed uniformly in the

forbid-den band-gap. The ativation energy of the traps is

estimatedas0.48eV. Thetrapdensityisfoundto

de-rease for inrease in both the lm thikness and the

temperature.

Aknowledgement

The authors wish to thank Prof A.P. Sathe, for

stimulating disussions and for ritially reading the

manusript.

Referenes

[1℄ L. Kasturi, Thin Film Phenomena, Mgraw-Hill Book

Company.

[2℄ N.F.Mott andE.A. Davis, Eletroni Proess In

Non-rystallineMaterials,ClarendonPress,Oxford2nd

edi-tion(1978).

[3℄ G.S. Nadkarni and V.S. Shirodkar, Thin Solid Films

105,115(1983).

[4℄ V.K. Dhavan, A. Mansingh and M. Sayer, J.

Non-rystallineSolids51,87(1982).

[5℄ K.NassauandD.W.Murphy,J.Non-rystallineSolids

44,297(1981).

[6℄ A.ServiniandA.K.Jonsher,Thin SolidFilms3,341

(1965).

[7℄ W.Z.Shottky,Phys.15,872(1914).

[8℄ Frenkel,J.Phys.Rev.54,647(1938).

[9℄ M.A. Lampert, RCA Teh. Report No. PTR., p 1445

(1963).

[10℄ J.G.Simmon,J.Phys.D4,613(1971).

[11℄ M.A. Lampert and P. Mark, Current injetions in

solids,NY.Lond.(1970).

[12℄ A.Rose,Phys.Rev.97,1538(1955).

[13℄ S.P.BodhaneandV.S.Shirodkar,J.Apply.Poly.Si.

Inpress(Publiationno.6700).

[14℄ T.Budinas,P.Makus,A. Smilga,J.Vivvakas,Phys.

Sol.Stat.31,375(1969).

[15℄ J.DresnerandF.V.Shallross,Sol.Stat.Eletr.5,205

(1962).

[16℄ I. Solomon, R. Benferhat and H. Tran-Quo, Phys.

Rev.B30,3422 (1984).

[17℄ N.KenshiroandC.K.KwanJpn.Appl.Phys.18,1161

Imagem

Figure 1. a. Shemati view of metal-glass-metal devies.
Figure 3. Log I - log V harateristis of the devies with
Figure 5. Curve a: Log I - log S harateristis of the de-
Figure 7. Log (I/V) - V harateristis of the devies at
+2

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