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1、560Chem.Mater.2005,17,560-565DepositionofCopperbytheH2-AssistedReductionofCu(tmod)2inSupercriticalCarbonDioxide:KineticsandReactionMechanismYinfengZongandJamesJ.WatkinsDepartmentofChemicalEngineering,UniVersityofMassachusetts,Amherst,Massachusetts01003ReceiVedAu
2、gust12,2004.ReVisedManuscriptReceiVedNoVember17,2004Thekineticsandreactionmechanismforcopperdepositionbythehydrogen-assistedreductionofbis-(2,2,7-trimethyloctane-3,5-dionato)copper(II),[Cu(tmod)2],insupercriticalcarbondioxidewasstudiedusingadifferentialcoldwallr
3、eactor.Atsubstratetemperaturesbetween220and270°C,themeasuredfilmgrowthraterangedbetween5and35nm/min.Theoverallapparentactivationenergywas51.9kJ/mol.Filmgrowthrateexhibitedzero-orderdependenceontheprecursoratprecursorconcentrationsbetween0.02and0.5wt%Cu(tmod)2inC
4、O2andazero-orderdependenceonhydrogenathydrogenconcentrationsgreaterthan0.06wt%inCO2.Zero-orderprecursordependenceoverlargeconcentrationrangespromotesexceptionalstepcoverage.Atlowerconcentrationsofeitherreagenta1/2-orderdependencewasobserved.Filmgrowthratewasnega
5、tiveorderwithrespecttoexcessquantitiesofthehydrogenatedligandbyproduct,(tmod)H,andfilmgrowthcouldbesuppressedcompletelyat(tmod)Hconcentrationsabove1wt%.Withuseoftheresultsoftheexperiments,aheterogeneousreactionmechanismisproposed.Protonationoftheadsorbedligand(t
6、mod)wasfoundtobetherate-determiningstep.ALangmuir-Hinshelwoodrateexpressionwasusedtocorrelatethedatawithgoodagreement.Introductionviscosity,highdiffusivity,andzerosurfacetensionarecloserCopperhasreplacedaluminumastheinterconnectmaterialtothoseofagas,facilitating
7、rapidmasstransferwithinofchoiceinadvancedintegratedcircuitsduetoitslowconfinedgeometries.Consequently,SFDisespeciallyca-electricalresistanceandsuperiorelectromigrationresistance.pableofachievingconformalstepcoverageanddefect-freeBy2010,theInternationalTechnology
8、RoadmapforSemi-fillinhighaspectratiofeatures.conductors(ITRS)predictsmicroprocessorswillenterpro-Todate,anumberofmetalfilms,suchasCu,Pt,Pd,Au,ductionatthe45nmtechnolo
