Interface Spin-Orbit Coupling in a Non-centrosymmetric Thin-Film Superconductor

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We present a detailed study of the effects of interface spin-orbit coupling (ISOC) on the critical field behavior of non-centrosymmetric (NCS), ultra-thin superconducting Be/Au bilayers. Parallel field measurements were made in bilayers with Be thicknesses

InterfaceSpin-OrbitCouplinginaNon-centrosymmetricThin-FilmSuperconductor

X.S.WuandP.W.Adams

DepartmentofPhysicsandAstronomy

LouisianaStateUniversity

BatonRouge,Louisiana,70803

arXiv:cond-mat/0509385v2 [cond-mat.supr-con] 19 Sep 2005Y.YangandR.L.McCarleyDepartmentofChemistryandtheCenterforBiomodularMulti-scaleSystemsLouisianaStateUniversityBatonRouge,LA,70803(Dated:February2,2008)Wepresentadetailedstudyofthee ectsofinterfacespin-orbitcoupling(ISOC)onthecritical eldbehaviorofnon-centrosymmetric(NCS),ultra-thinsuperconductingBe/Aubilayers.Parallel eldmeasurementsweremadeinbilayerswithBethicknessesintherangeofd=2 30nmandAucoveragesof0.5nm.ThoughtheAuhadnosigni cante ectonthesuperconductinggap,itproducedprofoundchangesinthespinstatesofthesystem.Inparticular,theparallelcritical eldexceededtheClogstonlimitbyanorderofmagnitudeinthethinnest lmsstudied.Inaddition,theparallelcritical eldunexpectedlyscaledasHc||/ o∝1/dsuggestingthatthespin-orbitcouplingenergywasproportionalto o/d2.Tilted eldmeasurementsshowedthatcontrarytorecenttheory,theISOCinducesalargein-planesuperconductingsusceptibilitybutonlyaverysmalltransversesusceptibility.PACSnumbers:74.20.Rp,74.78.Db,73.40.JnOneofthemostfundamentalcharacteristicsofasuperconductoristhesymmetryofitscondensatewavefunction.Indeed,thishasproventobeacentralissueinthedescriptionofanumberofnon-conventionalsuperconductorssuchashigh-TcsystemsandtheruthenatesInconventionalBCSsuperconductivitythecondensateistimereversalinvariantandisformedfromCooperpairsconsistingofelectronsofoppositemomentumandoppositespinInnon-conventionalsuperconductors,however,thissimplesymmetrycanbemodi edbytheunderlyingcrystalstructureand/orthesymmetryofthepairinginteraction.AcompellingexampleoftheformeristherecentlydiscoveredheavyfermionsuperconductorCePt3Si,whosecrystalstructurelacksinversionsymmetryCePt3Siexhibitsalinenodegapstructure7,whichisbelievedtobe,inpart,aconsequenceofstrongspin-orbit(SO)couplinginanon-centrosymmetric(NCS)crystalsymmetry9,10].Thishasstimulatedrenewedinterestinthepossibilityofrealizingnon-conventionalpairingstatesfromtheconvolutionofbrokeninversionsymmetryandspinorbitcoupling,neitherofwhichviolatetimereversalinvariance.Recenttheoreticalworkontheproblemhassuggestedthatabilayercon guration,which,byde nition,lacksinversionsymmetry,consistingofalowatomicmassthin- lmsuperconductorcoatedwithahighatomicmassnon-superconductingelementsuchasAuorPtwouldbeamodelsystemforstudyingthee ectsofSOcouplinginaNCSsuperconductorInthepresentLetter,wepresentastudyofinterfaceSOcouplinginthinBe lmscoatedwith0.5nmofAuviacriticalmagnetic eldmeasurements.Contrarytorecenttheoreticalpredictions,we ndthattheSOinducedin-planesuperconductingspinsusceptibilityissigni cantlylargerthanthecorrespondingperpendicularsusceptibility.Furthermore,theSOcouplingcannotbedescribedintermsofAbrikosov-Gorkovimpurityformalism[4]inthatitappearstobeafunctionofthesuperconductinggap.Intheexperimentsdescribedbelowweusecritical eldmeasurementstodeterminetheSOcouplingstrengthinBe/Au lmsofvaryingBethickness.TheMakiequation15]isausefultoolforextractingthespinresponseofthesuperconductorfromtheorbitalresponse,particularlywhenthe lmisnotinthethin- lmlimitand/orthe eldisnotparalleltothe lmsurface.Ingeneralthecritical eldofathin lmisafunctionofthesuperconductinggap

o,the lmthicknessd,theelectrondi usivityD,andthespinorbitcouplingparameterb.Thecritical eldHcisdeterminedbytheimplicitfunction[15]:

Tα+ +2α 1ln (1)+ψ222γ4πkBT

where

21/2α±=b±γ,γ=(b2 µ2,BHc)

We present a detailed study of the effects of interface spin-orbit coupling (ISOC) on the critical field behavior of non-centrosymmetric (NCS), ultra-thin superconducting Be/Au bilayers. Parallel field measurements were made in bilayers with Be thicknesses

Tcisthecriticaltemperature,andψisthedigammafunction. isafunctionoftheanglebetweentheplaneofthe lmandthemagnetic eld,

(θ)=D[2eHcsin(θ)+1

o≈√

3b/ ob/ o

≥1,(3)whereEq.(2)isthefamiliarClogstonspin-paramagneticcritical eld[16,17,18].NotethatfromEq.(3)thecritical eldcanbearbitrarilyhighwithincreasingb.Incontrast,iftheZeemancouplingisneglectedthen,atany nitethicknessd<ξ,theparallelcritical eldislimitedbytheorbitalterm,

2µBHc||3 3

d(4)

Numerousstudiesofthespin-paramagnetictransitioninultra-thinAlandBe lmshaveshownthatthesetwolightelementshaveaverylowintrinsicSOscatteringrate[19,20,21]andaretruespin-singletsuperconductors.Consequently,theymakeidealcandidatesforsystematicstudiesofthee ectsofISOCinducedbyimpuritycoatings

[11,22].Notonlydoesthisbilayercon gurationbreakinversionsymmetry,butonecantreattheISOCasaboundaryconditiononthespincomponentofthesuperconductingwavefunction.Earlymeasurementsofthecritical eldbehaviorofAl lmscoatedwithlessthan0.2nmofPtrevealedthatthePt-inducedISOCcanproducesigni cantenhancementsoftheparallelcritical eldwithvirtuallynoe ectonthetransitiontemperature[19].ThoughthetemperatureandangulardependenciesoftheAl/Ptcritical eldswereinreasonableagreementwiththeMakiformula,theoverallmagnitudeofHc||wastypically~10 30%higherthancouldbeaccountedforbyreasonableestimatesofb.

Recentanalysisofthespinstatesoftwo-dimensionalNCSsuperconductors,and,inparticular,superconducting-normalmetalbilayers,predictsthatISOCwillintroduceananisotropicspintripletcomponentintosuperconductinggroundstate[12,13].Thetripletcomponentismostdirectlymanifestinthespinsusceptibilityofthesuperconductorχs.Ofcourse,conventionalspin-singletBSCsuperconductorshaveχs~0atT=0,butISOCisexpectedtoliftnsnsthespindegeneracy,andinthestrongcouplingl:χs ~χ/2,χ⊥~χ,whereχ isthein-planesuperconductingsusceptibilityandχnisthenormalstatesusceptibility.TheClogstoncritical eldgivenbyEq.(2)isderivedbyequatingthemagneticfreeenergydi erencebetweennormalandsuperconductingstateswiththecondensationenergyofthesuperconductingstate.Ifχs=0thenEq.(2)canbegeneralized,√2µBHc=1 χs/χn.(5)Thiswouldimplythattheparallelcritical eldofabilayer,suchastheAl/PtsamplesofRef.19,wouldneverbelargerthanHc||= o/µB.However,thecritical eldenhancementsobservedinthoseearlyexperimentsweresigni cantlygreaterthanthisupperlimit.Sincethelate1970’sverylittleworkhasbeendoneonSOcouplinginthin lmsuperconductors,thoughseveralfundamentalquestionsremainunanswered.Forinstance,theAl/PtmeasurementsweremadeatasingleAlthicknessandoveraverynarrowrangeofgapvalues.Clearly,onewouldliketodeterminethedepthtowhichtheISOCpenetratesintothesuperconducting lmandhowthespincomponentofcritical eldbehaviorscaleswith lmthicknessandgapmagnitude.Anotherimportantissueiswhetherornottheanisotropyinχsisobservableintheangulardependenceofthecritical eld.

Be/Aubilayer lmsofvaryingBethicknesswerepreparedbye-beamevaporationinainitialvacuumof~0.2µTorr.Allofthedepositionsweremadeon repolishedglasssubstratesheldat84K.FirstalayerofBe lmwiththicknessintherange2. 30.0nmwasdepositedatarateof0.14nm/s,thena0.5nmAu lmwasdepositedat0.01nm/swithoutbreakingthevacuum.BoththeBeandBe/Au lmswerefoundtobeverysmoothandhomogenous,withnoevidenceofislandingorgranularity,seeFig.1.The lmsweresubsequentlytrimmedinordertoeliminateedgee ects.Resistivemeasurementsweremadeinadilutionrefrigeratorwithabasetemperature50mKbyastandardfour-probelock-inmethod.The lmswerealignedwiththemagnetic eldviaaninsitumechanicalrotator.Inthedatapresentedbelowthetransitiontemperatureswerede nedbythetemperatureatwhichtheresistancefellto10%ofitsnormalstatevalueandthecritical eldwasdeterminedbythemidpointoftheresistivetransition.

We present a detailed study of the effects of interface spin-orbit coupling (ISOC) on the critical field behavior of non-centrosymmetric (NCS), ultra-thin superconducting Be/Au bilayers. Parallel field measurements were made in bilayers with Be thicknesses

ThetransitiontemperatureofthehomogeneouslydisorderedBe/Au lmsusedinthisstudyareplottedasafunctionofBethicknessinFig.2.Filmswithd<2nmareknowntodisplayanon-perturbativezerobiasanomalyintheirtunnelingdensityofstates,whichisassociatedwiththeemergenceoftheCoulombgap[23].AscanbeseeninFig.2,thisisalsothecriticalthicknessbelowwhichthezerotemperaturesuperconductingphaseislostandtheelectrondi usivitygoestozero.InordertomakeuseofEq.(1)itwasnecessaryto tthethicknessdependenceofTcandDwithanempiricalfunctionalform.Inparticular,thesolidlinesinthemainpanelandtheinsetofFig.2arethefunctions:

Tc(d)=Tcotanh[(d 1.35)/1.29)]

D(d)=Dotanh[d2/23.3],(6)(7)

whereTco=0.68KandDo~3 /m.Dowasdeterminedfrom lmswithd>10nmusingtherelation1/R=2e2ν0Dod,whereRisthesheetresistanceandν0isthedensityofstatesperspinofBe.TheBCScoherencelengthforaBe lmwithTc~0.7Kisξo~4µm.Fortherangeofdi usivitiesplottedintheinsetofFig.√2themeanfreepathisalwayslo<1nmandthecorrespondingPippardcoherencelengthsareintherangeξ=0.85

We present a detailed study of the effects of interface spin-orbit coupling (ISOC) on the critical field behavior of non-centrosymmetric (NCS), ultra-thin superconducting Be/Au bilayers. Parallel field measurements were made in bilayers with Be thicknesses

critical eldsofthetwo lms.Thisre ectsthefactthatitisalmostindistinguishablefromwhatonewouldobtainusingthephenomenologicalTinkhamformula[4,15]whichonlyinvolvesHc||andHc2.Incontrast,thedashedlinedepictsthesolutiontoEq.(1)assuminganexponentiallyattenuatedSOparameterb=1.85exp( θ/θo)mV,withacharacteristicangleθo=2.5 .ThedashedlinecapturesthedipstructureinthedatawhichindicatesthattheZeemancomponentofthecritical eldisangledependent.Thedipstructureisconsistentwithananisotropicsuperconductingsusceptibilityconsistingofalargein-planecomponent(oftheorderofthenormalstatesusceptibility)andasmalltransversecomponent.Thesenseofthisanisotropyisoftheoppositesignofthatcalculatedfornon-disordered2DNCSsuperconductors,wherethein-planecomponentisexpectedtobehalfthatofthetransversecomponent.Nevertheless,thefactthatISOCinducesapreferentiallylargein-planesusceptibilitywouldalsoaccountforearlierreportsofanomalouslyhighparallelcritical eldsinAl/Ptbilayers[19].

Insummary,wehaveusedcritical eldmeasurementstoprobethee ectsofinterfacespin-orbitcouplingonthespinstatesofsuperconductingBe lms.We ndthata~1monolayercoatingofAuontheBesurfaceproducesalarge,anisotropicenhancementtotheZeemancomponentofthecritical eld.Thenormalizedparallelcritical eldHc||/ oofBe/AubilayersscalesastheinverseoftheBethicknessandcanexceedtheClogstonlimitbyasmuchasanorderofmagnitude.Thecritical eldscalingwasobservedoverawiderangeof owhichisinconsistentwiththestandardimpurityscatteringmodelofSOcoupling.Webelievethatthescalingis,infact,amanifestationofthesuperconductor’sattempttoreconcileamixed-spinboundaryconditionattheAuinterfacewiththeintrinsicspin-singletgroundstateofBe.Naively,onewouldexpectthattheISOChealinglengthwouldbeoftheorderofξ,butitmaybesigni cantlyshorterinthepresenceofdisorder.Nevertheless,theanisotropicspinsusceptibilityisclearlyevidentinthetilted elddata.Ahigh eldstudyofthelocaltunnelingdensityofstatesattheBe/AuandtheBe/substrateinterfaces,respectively,shouldprovideanimportantlocalprobeoftheextentofspin-mixingatthetwoboundaries.

WegratefullyacknowledgeenlighteningdiscussionswithVictorEdelstein,GianluigiCatelani,IlyaVekhter,DanaBrowne,andDavidYoung.ThisworkwassupportedbytheNationalScienceFoundationunderGrantDMR02-04871.

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We present a detailed study of the effects of interface spin-orbit coupling (ISOC) on the critical field behavior of non-centrosymmetric (NCS), ultra-thin superconducting Be/Au bilayers. Parallel field measurements were made in bilayers with Be thicknesses

Figures

FIG.1:A)0.1x0.1µmatomicforcemicrographofa6nmthickBe lmevaporatedontoglassat84K.B)MicrographofaBe lmcoatedwith0.5nmofAu.

We present a detailed study of the effects of interface spin-orbit coupling (ISOC) on the critical field behavior of non-centrosymmetric (NCS), ultra-thin superconducting Be/Au bilayers. Parallel field measurements were made in bilayers with Be thicknesses

FIG.2:TransitiontemperatureofBe/AubilayersasafunctionofBethickness.TheAuthicknesswas0.5nmineachsample.Thesolidlineisabest ttothedatausingtheempiricalformofEq.(6).Inset:relativedi usivityofBe/AubilayersasafunctionofBethickness.Thesolidlineisa ttoEq.(7).

We present a detailed study of the effects of interface spin-orbit coupling (ISOC) on the critical field behavior of non-centrosymmetric (NCS), ultra-thin superconducting Be/Au bilayers. Parallel field measurements were made in bilayers with Be thicknesses

FIG.3:Normalizedparallelcritical eldsasafunctionofBethicknessforBe/Aubilayers(circles),Be/Pb(crossedbox),pureBe lms(triangles).Thelongdashedlinerepresentsthetheoreticalorbitallylimitedcritical eldgivenbyEq.(4).Thesolidlineisalinearleast ttothebilayerdata.ThehorizontaldashedlinerepresentstheClogstoncritical eld.

We present a detailed study of the effects of interface spin-orbit coupling (ISOC) on the critical field behavior of non-centrosymmetric (NCS), ultra-thin superconducting Be/Au bilayers. Parallel field measurements were made in bilayers with Be thicknesses

FIG.4:Ratioofthecritical eldofBe/AubilayersandBe lmsofequalBethicknessasafunctionoftiltangle,θ=0correspondstoparallel eld.triangles:d=7.4nm,circles:d=5.4nm,diamonds:d=2.9nm.Thesolidlinesareaguidetotheeye.

We present a detailed study of the effects of interface spin-orbit coupling (ISOC) on the critical field behavior of non-centrosymmetric (NCS), ultra-thin superconducting Be/Au bilayers. Parallel field measurements were made in bilayers with Be thicknesses

FIG.5:Ratioofthecritical eldofa5.4nmBe/Aubilayer(Tc=0.68K,Hc2=0.137T,R=240 )and5.4nmBe lm(Tc=0.505K,Hc2=0.048T,R=162 )asafunctionoftiltangle.SolidlineisthesolutionofEq.(1)assuminganisotropicSOcouplingparameterofb=1.85mVfortheBe/Aubilayerandb=0.0132mVfortheBe lm.ThedashedlineisthesolutionofEq.(1)assumingthattheBe/AuSOparameterisexponentiallyattenuatedwithincreasingtiltangle.Leftinset:FitofEq.(1)totheBe lmdata.Rightinset:Solidlineisa tofEq.(1)totheBe/Audatawithaconstantb.Thedashedlineisasomewhatbetter tusinganexponentiallyformb=boexp( θ/θo).

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