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In-situ Determination of Indium Segregation in

InGaAs/GaAs Quantum Wells Grown by

Moleular Beam Epitaxy

S. Martiniand A.A. Quivy

InstitutodeFsiadaUniversidadede S~ao Paulo,Laboratorio deNovosMateriais Semiondutores,

CP66318, 05315-970S~aoPaulo,SP, Brazil

Reeivedon23April,2001

Thesurfaesegregation ofindiumatomsduringthegrowthofInGaAs/GaAsheterostrutureshas

beeninvestigatedin situby reetionhigh-energy eletrondiration(RHEED).We pointedout

thatthestrongdampingoftheRHEEDosillationsduringthedepositionofInGaAsonGaAswas

relatedtothesegregationstrengthofindiumatomsintheInGaAslayer. Asimplemodelshowsthat

thedeayonstantoftheRHEEDosillationsmaybeusedtodetermineauratelythesegregation

oeÆient R,asonrmedbyphotoluminesene(PL)measurements.

I Introdution

Sineitsdisovery[1,2℄,surfaesegregationin

III-V semiondutor alloys has been the subjet of

nu-merous studies, in partiular in InGaAs/GaAs

quan-tum wells (QWs) [3, 4℄ beause of their importane

to theoptoeletronis and mirowaveindustries. It is

nowwellestablishedthatsegregationrepresentsthe

ul-timate limitation to obtainperfetly abrupt interfaes

neessary for the prodution of high-performane

de-vies [5℄. This phenomenon has already been

investi-gated by various surfae-sensitivemethods suh as

x-rayphotoeletronspetrosopy(XPS) [6℄, Auger

ele-tron spetrosopy (AES) and RHEED [7, 8℄, ormore

indiretly throughthetof QWoptial-transition

en-ergies from omposition-prole models [3℄. However,

untilnownoneofthephysialtheoriesreportedin the

literature was able to explain the origin of the eet

in asatisfatorywayforallthedierentmaterialsand

systemsinvestigated.

Inthiswork,weproposeasimpleandveryeÆient

wayto determine,insituand inreal time,thesurfae

segregationofindium(In)atoms duringthegrowthof

InGaAs layersonGaAs(001)substrates. Ourmethod,

thatisbasedontheinterpretationoftheintensity

vari-ationoftheRHEEDosillations,diersfromtheother

fewRHEEDstudiesbythefatthattheyonlyprovide

qualitativeresults[7℄orarerestritedtoaspei

ma-terialor growthtehnique[8℄.

II Experimental Details

Thesampleinvestigatedherewasgrownin aMod.

Gen. II moleular beam epitaxy (MBE) systemfrom

Varian and onsisted of a 0.25m-thik GaAs buer

grown at 570 o

C and a QW struture grown at 520

o

C.AftertheGaAsbuerlayer,thesubstrate

temper-ature was ramped up to 610 o

C during 2 minutes to

smooth the GaAs surfae and then ramped down to

520 o

C to deposit the 50

A-thik In

0:14 Ga

0:86

As layer.

Agrowthinterruptionof20swasrealizedattheseond

interfaeand, nally, a50

A-thik GaAs layerwas

de-posited at520 o

C,followedby450

AofGaAsgrownat

570 o

C. Thegrowthratesof thematerialswere

deter-minedby RHEED measurements that yielded avalue

of0.79and 0.68monolayerperseond (ML/s) forthe

In

0:14 Ga

0:86

AsandGaAslayers,respetively. The

sam-plewasnotrotatedduring thegrowthofthestruture

inordertoallowRHEEDmeasurementsduringthe

de-positionoftheInGaAslayerandtheseondGaAs

bar-rier. TheRHEEDmeasurementswerearriedoutwith

a8kVeletrongunand aglaning angleof 1.0 o

along

the[110℄diretionoftheGaAs(001)surfae. Afterthe

growth, thesample wasanalyzed by PL spetrosopy

at1.4Kusingonventionallok-intehniques,aooled

GaAsPhotomultiplier andthe 5145

Aline of anargon

laser.

III Results and Disussion

(2)

0

5

10

15

20

25

30

35

40

45

90

100

110

120

130

140

150

GaAs on GaAs

R

H

E

E

D

In

ten

sity

(arb

. u

n

its)

Time (s)

Figure1. TypialRHEEDosillationsduringthedeposition

ofGaAsonaGaAs(001)substrateat570 o

C.

Sine,underonventionalgrowthonditions,

homoepi-taxy proeeds in the layer-by-layer growth mode, the

osillationsareusuallyexplainedintermsofthe

rough-ening of the growth front by the nuleation of small

two-dimensional(2D) islands that merge to omplete

thelayersoneaftertheotherone. Thisperiodi

rough-eningofthesurfaeinduesaperiodisatteringofthe

eletronbeamthat yieldsaminimum reetionofthe

speularbeamwhen half ofthelayeris deposited and

a maximum reetion when the layer is omplete, as

showninFig. 1. However,asthetotalroughnessofthe

growthfrontinreasesslowlywithtime,theamplitude

oftheosillationsdereasesas thegrowthproeeds.

Fig. 2a shows the RHEED osillations when the

In

0:14 Ga

0:86

As layers of the 50

A-wide QW were

de-posited onthe rst GaAs barrier at 520 o

C.A strong

andasymmetridampingoftheosillationsisobserved

(unlikeinFig. 1)andisusuallyrelatedintheliterature

tothestrainedgrowthoriginatingfromthelattie

mis-mathbetweenGaAsandInAs[9℄. Intheseonditions,

the initial stage of the deposition ours under strain

and the InAs layeradopts the lateral lattie

parame-teroftheGaAssubstrate,storingelastienergyinthe

45

50

55

60

65

70

150

180

210

GaAs on InGaAs

(b)

R

H

E

E

D

In

ten

sity

(arb

. u

n

its)

Time (s)

160

200

240

0

5

10

15

20

25

InGaAs on GaAs

(a)

Figure 2. RHEED osillations (solid lines) deteted a) at

therst interfaeofthe InGaAsQW;b)at theseond

in-terfaeoftheInGaAsQW.Thedottedlinesshowthebest

tofthedampingusingequation1.

manner, but nownuleationof newislandson thetop

layer before the ompletion of the underlying layeris

energetially morefavorable, unlike in the ase of

ho-moepitaxy, beause they allow a partial relaxationof

thestrainattheislandedgeandontributetoderease

the totalenergy of thesurfae. As aonsequene the

surfaebeomesroughfaster,yieldingastronger

damp-ingoftheosillations. However,suhargumentsarenot

totallysatisfatorybeausetheydonotexplainwhythe

damping varies with temperatureand why it still

ap-pearsduringthegrowthoflattie-mathed

heterostru-tures[8℄.

Inordertobetterunderstandtheoriginofthe

phe-nomenon, we investigated the inuene of the growth

onditionson thebehaviorof theRHEED osillations

during deposition of InGaAs on GaAs and observed

thattheirdampingwasstrongerathighertemperature

andat lowergrowthrateandV/III ux ratio.

Coini-dentally,Insegregationisknowntobeveryeetivein

this ternaryalloyandstrongly depends onthesurfae

mobility of the group-III adatoms that varies exatly

in the samewaywith respetto these growth

(3)

parameter that ould be related to the strength of In

segregationintheInGaAslayers. Theexpression

I =I

0 +I

1

exp(n=) (1)

wasused, where n is the number of osillations (i: e:

of MLs)and thedeayonstantthat is therelevant

ttingparameterexpressedinMLs. Thebesttofthe

experimental datais shownin Fig. 1a. Thereal

phys-ial meaning of an be betterunderstood when the

segregationoeÆientRisexpressedas [3℄

R=exp( 1=Æ) (2)

where Æ is a harateristi length (expressed in MLs)

over whih segregation is eetive. If the dampingof

theRHEEDosillationsisamanifestationofIn

segrega-tion(aswesuggest),weshouldbeallowedtosubstitute

Æby andalulateR.Usingtheexperimentaldataof

Fig. 2aandtheirbesttfromequation1,weobtained

R=0.83,whihisatypialvalueforthegrowth

ondi-tionsused here[10℄. Whentheseond GaAsbarrieris

depositedontopoftheInGaAslayers,thelargenumber

ofInatomsaumulatedonthesurfaeisprogressively

inorporated into the GaAs barrier and the envelope

oftheRHEEDosillationsreoversitsnormalintensity

as shown in Fig. 2b. Sine this behavior also results

from thesegregationofInatoms,wealulatedR

(us-ingthe+signinequation1)andobtained0.84,avalue

that isin exellent agreementwith the other one

pre-viously determined at the rst interfae, showing the

onsistenyofourmodel. OthersimilarRHEED

stud-ies were arried out hanging the growth parameters

(growthtemperature, growthrate,V/IIIux ratio)in

ordertoverifytheirinueneonthenumerialvalueof

R.Inalltheases,weobtainedextremelyoherentand

reproduibleresultsompatiblewiththedataavailable

in theliterature[11℄.

To rosshekthe validity ofour model, PL

mea-surements were arried out on the same sample. In

segregationgenerally produesa blueshiftof the

opti-alQWemissionwithrespettotheexpetedeletroni

transition of a square QW beause of the non-ideal

potential prole at both interfaes. Using the

ee-tivemassesofeletronandheavyholesfora

biaxially-strained InGaAs layer, we ould obtain their

onne-mentpotentialsandsolvetheShrodingerequation.

As-suminganexitonbindingenergyof7meV,theoptial

transition of the square QW was estimated in 1.4229

meV, showing a redshift of 5.3 meV with respet to

the experimental PLenergy(1.4282meV)[11℄. To

de-termine R, we used the omposition-prole model of

Muraki[3℄aordingtowhihtheInompositionx

n of

thenthlayeris

x =x (1 R n

) nN (3)

wherex

0

andNarethenominalInomposition(0.14)

andthewellwidthin MLs(18),respetively. The

seg-regation oeÆient R is adjusted in order to provide

therightvalueoftheInontentthathastobeused to

alulatetheeletronandheavy-holeonnement

ener-giesthatwill ttheexperimental PLdata[4℄. Forthe

optialemissiondetetedinoursample,weobtaineda

valueofR=0.83,whihisinperfetagreementwiththe

previousresultsprovidedbytheRHEEDtehnique.

IV Conlusion

We showed that the damping of the RHEED

os-illations during theMBE growthof InGaAs layersis

related to the strength of In segregation that an be

quantitativelyestimated in averyaurate way. This

powerfulandversatilemethodallowsreal-timeand

in-situ investigations of the phenomenon and will surely

providenewinterestingdatain thiseld.

Aknowledgments

WearegratefultoFAPESPforpartialnanial

sup-port(grants97/07974-6and98/14489-0).

Referenes

[1℄ J.M.Moison,C.Guille,F.Houzay,F.Barhte,andM.

VanRompay,Phys.Rev.B40,6149(1989).

[2℄ J.Massies,F.Turo,A.Salletes,andJ.P.Contour, J.

Cryst.Growth80,307(1987).

[3℄ K.Muraki,S.Fukatsu,andY.Shiraki,Appl.Phys.Lett.

61,557(1992).

[4℄ S.Martini,A. A.Quivy,A.Tabata, and J.R.Leite, J.

Va.Si. Tehnol.B18,1991(2000).

[5℄ J.F.Zheng, J.D. Walker, M. B.Salmeron, andE. R.

Weber,Phys.Rev.Lett.72,2414(1994).

[6℄ G.Grenet,E.Bergignat,M.Gendry,M.Lapeyrade,and

G.Hollinger,Surf.Si.352/354,734(1996).

[7℄ J.M.Gerard,Appl.Phys.Lett.61,2096 (1992).

[8℄ M.Mesrine,J.Massies, C.Deparis,N.Grandjean, and

E.Vanelle,Appl.Phys.Lett.68,3579(1996).

[9℄ C.W.Snyder,B.G.Orr,D.Kessler,andL.M.Sander,

Phys.Rev.Lett.66,3032(1991).

[10℄ R.Kaspiand K.R. Evans, Appl. Phys.Lett67, 819

(1995).

[11℄ S.Martini,A. A.Quivy,andE. Abramof,X th

Brazil-ian Workshop onSemiondutor Physis, April 22-27,

Imagem

Figure 1. Typial RHEED osillations during the deposition

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