Thermal stability of nanoscale metallic multilayers

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ThermalstabilityofnanoscalemetallicmultilayersA.S.Ramosa,⁎,A.J.Cavaleiroa,M.T.Vieiraa,J.Morgielb,G.SafrancaCEMUC®,DepartamentodeEngenhariaMecânica,UniversidadedeCoimbra,3030-788Coimbra,Portugal

bInstituteofMetallurgyandMaterialsScience,PolishAcademyofSciences,Reymonta25,30-059Cracow,Poland

cResearchInstituteforTechnicalPhysicsandMaterialsScience,HungarianAcademyofSciences,H-1121Budapest,Hungary

abstractarticleinfoAvailableonline7June2014Keywords:MultilayersTi/AlNi/AlNi/TiPd/AlIntermetallicSputteringThermalstability

Metallicnanolayeredthinfilms/foils,inparticularNi/Almultilayers,havebeenusedtopromotejoining.Theob-jectiveofthisworkistoevaluatethethermalstabilityofnanoscalemetallicmultilayerswithpotentialforjoiningapplications.Multilayersthinfilmswithlow(Ti/AlandNi/Ti),medium(Ni/Al)andhigh(Pd/Al)enthalpiesofexothermicreactionwerepreparedbydualcathodemagnetronsputtering.Theirthermalstabilitywasstudiedby:i)differentialscanningcalorimetrycombinedwithX-raydiffraction(XRD),ii)in-situXRDusingcobaltradi-ation,andiii)in-situtransmissionelectronmicroscopy.Itwaspossibletodetecttracesofintermetallicoramor-phousphasesintheas-depositedshortperiod(bilayerthickness)multilayers,exceptfortheTi/Alfilmswherenoreactionproductsthatmightbeformedduringdepositionwereidentified.Forshortperiods(below20nm)theequilibriumphasesaredirectlyachieveduponannealing,whereasforhigherperiodsintermediatetrialuminidephasesarepresentforTi/AlandNi/Almultilayers.TheformationofB2-NiTifromNi/Timultilayersoccurswithouttheformationofintermediatephases.Onthecontrary,forthePd–Alsystemtheformationofintermediatephaseswasneveravoided.Theviabilityofnanoscalemultilayersas“filler”materialsforjoiningmacroormicroparts/deviceswasdemonstrated.©2014ElsevierB.V.Allrightsreserved.

1.IntroductionReactivemultilayer(ML)thinfilmsarecomposedoftens,hundreds,orthousandsofalternatingindividuallayersofreactantshavingalargenegativeenthalpyofmixing.Thelayeredstructureisrepeatedthrough-outthefilmwithamodulationperiod(Λ)consistinginthethicknessofonedoublelayer.Thenegativeenthalpyofmixingoftheconstituentsresultsinheatreleaseoncereactionisinitiated.Forcertainsystemsanddesigns,reactiveMLsexhibitfastexothermalreactions,attaininghightemperatures.Thereactionscouldbeignitedbyanexternalenergysourcesuchasanelectricsparkoramechanicalload[1].Afterreactionisinitiated,atomicmixinganddiffusiontakeplacegeneratingheatataveryfastrate.Heatisconducteddownthefilms,promotingatomicmixingandestablishingaself-propagatingchainreaction[1].Innano-scale/nanocrystallineMLsheatcanbegeneratedfaster,increasingthereactionvelocityandenablingexothermicreactionstobecomeself-sustained.Theexothermicandself-propagatingnatureofreactiveMLsmakethempromisingforseveralapplications,includingjoining[2].Infact,reactivenanoscaleMLfoilsandthinfilmshavealreadyfounduseasafillermaterial,beingparticularlypromisingfor

dissimilarjoining.ReactiveMLscanbeusedasstand-aloneheatsourcesorbyusingtheenergyreleasedtomeltsurroundingsolderorbrazealloys.Forsomeyearsnow,theheatreleasedbytheexo-thermicreactioninnanolayeredNi/AlreactiveMLfoilsisbeingusedtomeltbrazealloys,promotingjoining[3–5].Inaddition,reac-tiveMLscanbeusedtoenhancethediffusionbondingprocessbytakingadvantageoftheirimproveddiffusivity/reactivityandexo-thermiccharacter—reactionassisteddiffusionbonding[6–8].ThefeasibilityofthisprocedurehasalreadybeendemonstratedforsimilaranddissimilarjoiningusingmetallicMLthinfilmswithnanometricmodulationperiods(bilayerthickness)[9–14].TheadvantagesofthereactionassisteddiffusionbondingprocessusingreactiveMLthinfilmsasa“filler”materialinclude:i)an“internal”energysourcetoaidonthediffusionbondingprocess,ii)lowerdiffusionbondingtemperature/pressureorshorterholdingtimes,iii)excellentfiller/basematerialinterface,iv)highqualityandcon-trollabilityofthefillermaterial,andv)thepossibilityofprovidinganinterfacezonewithanintermediatethermalexpansioncoeffi-cient,avoidingcracksandfractureduringdissimilarjoining.Whatevertheapplicationenvisaged,itisextremelyimportanttostudythethermalstabilityoftheMLthinfilmsandhowtheyevolvewiththetemperature.Thephaseevolutionofdifferentmetallicmultilayerthinfilmshasbeenstudiedbytheauthorsusingdifferenttechniques[8,15–18].ThisresearchconcernsthephaseevolutionwithtemperatureofMe1/Me2(Me—metal)MLthinfilmswithpotentialforjoining

ThinSolidFilms571(2014)268–274⁎Correspondingauthorat:DepartamentodeEngenhariaMecânica,PóloII,UniversidadedeCoimbra,R.LuísReisSantos,3030Coimbra,Portugal.Tel.:+351239790700;fax:+351239790701.E-mailaddress:sofia.ramos@dem.uc.pt(A.S.Ramos).