Effect of deposition rate on the characteristics

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EffectofdepositionrateonthecharacteristicsofGequantumdotsonSi(001)substrates

KazuhiroGotoha,⁎,RyujiOshimab,TakeyoshiSugayab,IsaoSakatab,KojiMatsubarab,MichioKondoa,baDepartmentofInnovativeandEngineeredMaterials,InterdisciplinaryGraduateSchoolofScienceandEngineering,TokyoInstituteofTechnology,4259Nagatsuta-cho,Midori-ku,Yokohama,

Kanagawa226-8503,JapanbNationalInstituteofAdvancedIndustrialScienceandTechnology,1-1-1Umezono,Tsukuba,Ibaraki305-8568,Japan

abstractarticleinfoAvailableonline26October2013Keywords:GermaniumSiliconQuantumdotsMolecularbeamepitaxySelf-assembly

Wehavestudiedtheeffectofthedepositionrateonthestructuralandopticalcharacteristicsoffive-layer-stackedGeself-assembledquantumdots(QDs)onaSi(001)substrategrownbymolecularbeamepitaxy.GeQDswereformedusingapulsegrowthtechnique,whichconsistsofhigh-rateGedepositionandaninterruptioningrowth.Inthiswork,thedepositionratewasvariedfrom1.1Å/sto2.8Å/s.Pyramid-shapedQDswithamonomodalsizedistributionwereobtainedat2.8Å/s,whileabimodalsizedistributionincludingpyramid-shapedQDsandmulti-faceteddome-shapedQDswasobservedbetween1.1Å/sand2.2Å/s.Asaresult,animprovedsizefluctuationof11.1%andhighestsheetdensityof5.6×1010cm−2wereachievedfortheQDsamplegrownat2.8Å/s.Asforthe

opticalcharacteristics,asinglephotoluminescence(PL)emissionlineat0.825eVwithawidthof86.1meVwasob-servedat12K.Furthermore,wefoundthatthePLemissionfromtheGeQDsshowstype-IIemissioncharacteristics,i.e.,theshiftofthePLpeakenergywithrespecttothePLexcitationpower(Pexc)wasproportionaltoPexc

1/3.

©2013ElsevierB.V.Allrightsreserved.

1.IntroductionSelf-assembledquantumdots(QDs)formedusingtheStranski–Krastanovmodeofhetero-epitaxialgrowthhavemuchpotentialforoptoelectronicdevicessuchasQDintermediatebandsolarcells(QD-IBSCs)[1–3].IBSCsareexpectedtoachievehighconversioneffi-cienciesbytakingadvantageoftwo-stepopticaltransitionsviaIBstatesinadditiontotheconventionalopticaltransitionsfromthevalencebandtotheconductionband.Recently,QDSCsbasedonIII–Vcompoundsemiconductorshavebeenintensivelystudiedbecauseoftheirwell-establishedself-assemblingprocessaswellastheiropticalcharacteris-tics[4,5].Incomparison,self-assembledGeQDsinaSimatrixareexpectedtoimprovethecarriercollectionefficiencyinsolarcellsthroughtheirtype-IIheterointerfaceandindirectbandstructure[6].Inordertorealizehigh-efficiencyQDSCs,theGeQDsshouldbesmall,dense,highlyuniform,andalignedinthegrowthdirectiontoformelec-tricallycoupledQDs,leadingtotheformationofminibandsorIBstates.Especially,theinterdotspacingshouldbelessthan3nmtoformminibandsinGe/Simatrices[7].Furthermore,theGeQDsmustbefreeofcontaminationanddefectstoavoidundesirablenonradiativere-combinationlosses.SeveralapproacheshavebeenexploitedtotunethemorphologyandstructuralpropertiesofGeQDsonSisubstrates,suchasantimony-surfactant-mediatedgrowth[8]andlow-temperaturegrowth[9],althoughthesetechniquestendtoleadtounexpectedmodulationofthecarrierconcentration.Ontheotherhand,wehave

recentlyproposedapulsegrowthtechniquethatconsistsofGedeposi-tionatahighrateof2.8Å/sandashortgrowthinterruptiontoallowtheformationofhigh-densitypyramid-shapedGeQDs[10].Furthermore,wehavefoundthatthepulsegrowthtechniqueisadvantageousforobtaininghigh-qualitymultiple-layer-stackedGeQDswithoutanydis-locations,especiallyincomparisontothewell-studiedcontinuousgrowthtechniqueusingalowdepositionrateof0.2Å/s.Inthispaper,wefurtherstudythestructuralandopticalcharacteristicsofGeQDsgrownusingapulsegrowthtechniquewithvariousdepositionrates.

2.ExperimentsAllsamplesweregrownbysolid-sourcemolecularbeamepitaxy(MBE)usingasystemequippedwithtwoelectrongunsforSiandGesolidsources.Theequilibriumback-pressureinthegrowthchamberwasoftheorderof10−8Pa.First,Si(001)substrateswerecleaned

usingastandardRCAprocedure.Afterathermalcleaningat850°Cfor5min,a150-nm-thickSibufferlayerwasgrownat600°Ctoobtainanatomicallyflatsurface.Then,five-layer-stackedGeQDsweregrownat500°C.Thedepositionthicknessandthedurationofgrowthinterruptionafterthedepositionwerefixedto5.0monolayersand30s,respectively.ThedepositionrateforGewasvariedfrom1.1Å/sto2.8Å/s,andthethicknessoftheSispacerlayerwas40nm.ThetopmostQDlayerwasnotcappedinordertocharacterizethesurfacemorphology.Thestructuralpropertieswerecharacterizedusingatappingmodeatomicforcemicroscope(AFM)equippedwithatipof10nmtipradius.Foropticalcharacterization,photoluminescence(PL)wasmeasuredusinga532-nmgreenlaserwithaspotdiameterofabout500μmfor

ThinSolidFilms557(2014)80–83⁎Correspondingauthor.Tel./fax:+81459245567.E-mailaddress:gotou.k.ab@m.titech.ac.jp(K.Gotoh).