ApplPhysLett_88_062502
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ApplPhysLett_88_062502
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内容需要下载文档才能查看 内容需要下载文档才能查看Combining half-metals and multiferroics into epitaxial heterostructures forspintronics
H. Béa, M. Bibes, M. Sirena, G. Herranz, K. Bouzehouane et al.
Citation: Appl. Phys. Lett. 88, 062502 (2006); doi: 10.1063/1.2170432
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APPLIEDPHYSICSLETTERS88,062502?2006?
Combininghalf-metalsandmultiferroicsintoepitaxialheterostructuresforspintronics
H.Béa
UnitéMixtedePhysiqueCNRS-Thales,RouteDépartementale128,91767Palaiseau,France
M.Bibesa?
Institutd’ElectroniqueFondamentale,UniversitéParis-Sud,91405Orsay,France
M.Sirena,G.Herranz,K.Bouzehouane,andE.Jacquet
UnitéMixtedePhysiqueCNRS-Thales,RouteDépartementale128,91767Palaiseau,France
S.Fusil
Universitéd’Evry,BâtimentdesSciences,ruedupèreJarlan,91025Evry,France
P.ParuchandM.Dawber
DPMC,UniversityofGeneva,24QuaiE.Ansermet,1211Geneva4,Switzerland
J.-P.ContourandA.Barthélémy
UnitéMixtedePhysiqueCNRS-Thales,RouteDépartementale128,91767Palaiseau,France
?Received4August2005;accepted9December2005;publishedonline6February2006?WereportonthegrowthofepitaxialbilayersoftheLa2/3Sr1/3MnO3?LSMO?half-metallicferromagnetandtheBiFeO3?BFO?multiferroic,onSrTiO3?001?bypulsedlaserdeposition.Thegrowthmodeofbothlayersistwodimensional,whichresultsinunit-cellsmoothsurfaces.Weshowthatbothmaterialskeeptheirpropertiesinsidetheheterostructures,i.e.,theLSMOlayer?11nmthick?isferromagneticwithaCurietemperatureof?330K,whiletheBFO?lmsshowsferroelectricitydowntoverylowthicknesses?5nm?.Conductive-tipatomicforcemicroscopemappingsofBFO/LSMObilayersfordifferentBFOthicknessesrevealahighandhomogeneousresistivestatefortheBFO?lmthatcanthusbeusedasaferroelectrictunnelbarrierintunneljunctionsbasedonahalf-metal.©2006AmericanInstituteofPhysics.?DOI:10.1063/1.2170432?
Toagreatextent,today’sresearchinspintronicsfocusesonthedevelopmentofmaterialsanddevicesconcepts.1Inmanycases,theformerarerequisitestothelatter.Recently,severalfamiliesofmaterialshavebeendevelopedinthissense,atypicalexamplebeingthatofdilutedmagneticsemiconductors.2Asspintronicseffectsrelyonthespinpolarizationoftheelectricalcurrent,materialswithlarge,ideallytotal,spin-polarizationhavealsobeenextensivelyinvestigated.Withtheseso-calledhalf-metals,3aconsider-ableincreaseinthetunnelmagnetoresistanceofmagnetictunneljunctions4hasindeedbeenachieved,atleastatlowtemperatures.5
Anotheremergingfamilyofmagneticmaterialsaremultiferroics.6Inthesecompounds,severalferroicorders?e.g.,magneticandelectric?coexist,withsomecouplingbetweenthem?themagnetoelectriceffect?.7Mostareferroelectricandantiferromagnetic,anotableexceptionbeingBiMnO3thatisferromagnetic.8ApropotypicalmultiferroicthathasattractedalotofattentionlatelyisBiFeO3?BFO?.9,10Itisaferroelectricandweaklyferromagneticrhombohedralperovskitewithordertem-peraturesfaraboveroomtemperature?TC=1043K,11TN=647K?.12BFOthuscrystallizesinthesamestructureasseveralknownhalf-metallicferromagnets?suchasLa2/3Sr1/3MnO3,La2/3Ca1/3MnO3,orSr2FeMoO6?,whichmakesitpossibletocombineitwiththesematerialsinmul-tifunctionalepitaxialheterostructures.Severalpromisingtypesofdevicescanbeimaginedfromthiscombination,as
a?
Electronicmail:manuel.bibes@ief.u-psud.fr
discussed,forinstance,byBineketal.13,14Inparticular,onecanthinkofusingverythinlayersofBiFeO3asmultiferroictunnelbarriers.Ifferroelectric,theselayersshouldhavethesamefunctionalitiesasthoseofrecentlydeveloped15andmodeled16,17ferroelectrictunnelbarriers,combinedwithamagneticorderingandapossiblemagnetoelectriccoupling.
Inthisletter,wedescribethegrowthandpropertiesofbilayersoftheLa2/3Sr1/3MnO3?LSMO?half-metalcombinedwithBFOandepitaxiallygrownontoSrTiO3?001?substratesbypulsedlaserdeposition.Westudythemorphological,structural,electrical,andmagneticpropertiesofBFO/LSMObilayers.WeshowthatthemagneticpropertiesofLSMOarepreservedandthattheBFOlayersareinsulatingandferro-electric,downtothicknessesoftBFO=5nm.BFOultrathinlayersthusful?llsomeimportantcriteriaforbeingusedasferroelectrictunnelbarriers.
ThesamplesusedinthisstudyhavebeengrownbypulsedlaserdepositionusingaNd:yttrium–aluminium–garnet?YAG?laser,atafrequencyof2.5Hz.TheLSMOtargetwasstoichiometricwhileforBFO,atargetwithnomi-nalcompositionBi1.15FeO3wasused,inordertocompensateforthehighvolatilityofBi.?001?-orientedSrTiO3?STO?substrateswereused.Inthepseudo-cubicrepresentation,BFOhasaunit-cellparameterof3.96Å,LSMOof3.88Å,andSTOof3.905Å,sothattheSTOsubstrateinducesatensilestrainonLSMOandacompressivestrainonBFO.TheoptimalgrowthconditionsforLSMOwerepreviouslydeterminedtobeofadepositiontemperatureTdep=720°CandanoxygenpressureofPdep=0.41mbar,18withapostan-nealingat300mbarofO2.Werecentlydeterminedthe
©2006AmericanInstituteofPhysics
0003-6951/2006/88?6?/062502/3/$23.0088,062502-1
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062502-2Beaetal.Appl.Phys.Lett.88,062502?2006?
FIG.2.?a?MagnetichysteresisloopsoftheBFO/LSMO//STObilayerwithtBFO=5nmmeasuredbySQUIDat10K.?b?Temperaturedependenceofthemagnetizationina?eldof1kOe,normalizedtothemagnetizationat10K?M10K?forthesamesample.
FIG.1.RHEEDpatternsinthe?100?directionofthesamplewithtBFO=20nm?a?oftheSTOsubstratebeforedeposition,?b?afterdepositionoftheLSMOlayer,and?c?afterdepositionoftheBFO.Thepatternismorediffusein?b?becausethepressureofmeasurementwas6?10?3mbarcom-paredto10?6mbarfor?a?and?c?.?d?X-raydiffractionspectraofBFO/LSMO//STObilayerswithtLSMO=11nmandtBFO=5nmand70nm.S,L,andBlabelpeaksofSTO,LSMO,andBFO,respectively.?e?RSMofthe?103?re?ectionsoftheBFO?70nm?/LSMO//STObilayer;r.l.u.isforre-ciprocalspace
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Pdep-TdepphasestabilitydiagramforBFO?lmsandfoundthatoptimalconditionsarearoundTdep=580°CandPdep=6?10?3mbar.19Inthepresentsamples,theLSMOlayer?11nmthickforallsamples?wasgrown?rst,andtheBFO?lm?tBFO=1–70nm?afterward.Tolimitapossibledeoxygenationofthemanganite,afterthegrowthoftheLSMO?lm,thepressurewaskeptattheLSMOdepositionpressurewhiledecreasingTdepto580°C.Then,thepressurewasrapidlydecreasedto6?10?3mbar,togrowtheBFOlayer.Thesamplewas?nallycooledtoroomtemperaturein300mbarofoxygen.
Re?ectionhigh-energyelectrondiffraction?RHEED?patternswerecollected?atanaccelerationvoltageof25kV?beforegrowth,andafterdepositingeachlayer.Imagesforthe?100?directionareshowninFigs.1?a?–1?c?,andindicateatwo-dimensionalgrowthfortheLSMOandtheBFOlayer?uptoatleasttBFO=35nm?.Anazimuthalanalysisrevealedanin-planeepitaxyforbothlayers.
X-raydiffraction?-2?spectra?inthe15°–115°2?range?werecollectedforallsamplesandonlyshowedpeakscorrespondingto?00??re?ections?pseudo-cubicindexation?ofSTO,LSMO,andBFO.Figure1?d?showsthespectrafortBFO=5nmand70nm.Fromtheangularpositionofthe?003?re?ectionsofBFO,wecalculatedtheout-of-planepa-rametercBFO?4.10Åthatwasfoundtovaryonlyslightlywiththickness.Areciprocalspacemap?RSM?ofthe?103?re?ections?seeFig.1?e??fora70nm?lmshowsthatboththeLSMOandBFOlayersareveryheavilystrainedontheSTOsubstrate.NotethatnosplittingoftheBFO?103?peakisdetected,suggestingatetragonalratherthanmonoclinicorrhombohedralsymmetryfortheBFOlayer,incontrasttotheresultsofXuetal.20orQietal.,21respectively.
Figure2?a?showsamagnetizationhysteresiscycleofaBFO?5nm?/LSMObilayermeasuredat10Kwiththe?eldappliedin-planealong?100?afterzero-?eldcooling,mea-suredinasuperconductingquantuminterferencedevice?SQUID?.Thesaturationmagnetization?MS?fortBFO=5nmisabout580emucm?3,closetothemagnetizationof
bulkLSMO?590emucm?3?.22EvenforlargerBFOthick-nessvalues,thecontributionoftheBFOlayertothemagne-tizationwasnotvisible,asexpectedfromtheverysmallmagnetizationvaluesobtainedforoptimizedBFOsingle?lmsgrowninthesameconditions.19Wemeasuredtheevo-lutionofthemagnetizationwiththetemperatureinordertocheckthequalityoftheLSMOlayer?seeFig.2?b??.TheCurietemperature?TC?is330K,somehowsmallerthanthebulkTC=370K,22butingoodagreementwiththeTCofthinsingle?lms23ofsimilarthickness.
TheBFO/LSMObilayerswereimagedwithaconductive-tipatomicforcemicroscope?CTAFM?.Inthesetypeofexperiments,themorphologyofthesamplesurfaceandtheresistancebetweenthebottomelectrodeandthetiparemeasuredsimultaneously,andcoupledheight-resistancemapsarerecorded.24Examplesofsuchmaps3?3?m2areshowninFigs.3?a?and3?b?foraBFO?5nm?/LSMObi-layer.Theleftimagerevealsavery?atsurface?inagreementwiththetwo-dimensionalgrowthmodeinferredfromtheRHEEDpatterns?withterracesseparatedby?4Åhighsteps,i.e.,aperovskiteunitcell.Thecorrespondingresis-tancemap?Fig.3?b??showsahighresistancelevel?averagevalue?1G??,witharemarkablehomogeneity.SimilarcoupledmapswerecollectedforsampleswithdifferentBFOthicknesses.Identicalunit-cellstepswereobserveduptotBFO=20nm.ResistancemapscouldbecollectedforthetBFO=1,2,and5nmsamples,withoutsaturatingthecapabil-ityoftheCTAFMelectronics.TheaverageresistanceofthemapsisplottedasafunctionoftheBFOthicknessinFig.3?c?.ThedataattBFO=0correspondtoasingleLSMO?lm.AnexponentialincreaseoftheresistancewithtBFOisob-tained,whichindicatesthattransportoccursthroughtheBFO?lmbytunneling.Thisobservation,togetherwiththe?atnessandthehomogeneityoftheBFOontheLSMObuff-ers,quali?esBFOverythin?lmsaspotentialbarriersintunneljunctions.
Piezoelectricatomicforcemicroscopy?PFM?wasusedtoprobetheferroelectricityoftheBFO?lmsinBFO/LSMObilayers,25forseveralvaluesoftBFO.Analternativelyposi-tiveandnegativevoltagewasappliedbetweentheconduc-tivetipoftheAFMandthebottomelectrode?LSMO?topoletheBFOlayerinto“up”and“down”stripes.PFMwasthenusedtodetectthedomainstructure.Figure4?a?showsthetopography,andFigs.4?b?and4?c?thePFMimagesofthe5nm?lmafterwriting.WeobserveaclearcontrastinFig.4?b?thatrevealsthepresenceofupanddownferroelectricdo-mainsinthis?lm.Notethatthispatternisnotobserved
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062502-3Beaetal.Appl.Phys.Lett.88,062502?2006?
?lmsgivevirtuallynosignal,asexpectedforaweakferro-magnet.ThroughacombinedCTAFMandPFMstudyontheseBFO/LSMOheterostructures,wehaveshownthatBFOlayersasthinas5nmareferroelectricandcanbeusedastunnelbarriers.Thisopensthewayfortherealizationofseveraltypesofdevices,suchasferroelectrictunneljunctions15ormagnetictunneljunctions4withferroelectrictunnelbarriers.Inthislattertypeofstructure,acontroloftheferroelectricpolarizationbyanexternalmagnetic?eldcanbeenvisaged,viathemagnetoelectriceffect.
TheauthorsareverygratefultoM.ViretandD.ColsonforprovidingtheBFOtargetandtoJ.-M.Trisconeforfruit-fuldiscussions.Twooftheauthors?G.H.andM.S.?acknowledge?nancialsupportfromtheMinistèredel’EducationNationale,del’EnseignementSupérieuretdelaRecherche?France?.Anotherauthor?H.B.?acknowledges?nancialsupportfromtheConseilGénéraldel’Essone?France?.
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1
FIG.3.3?3?m2morphology?a?andresistance?b?mapsoftheBFO?5nm?/LSMObilayermeasuredsimultaneouslybyaCTAFM.?c?LogarithmoftheaverageresistanceofthesemapsfordifferentBFOthicknesses.Theerrorbarscorrespondtothefullwidthathalfmaximumoftheresistance
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thetopography.Figure4?c?,collectedafterwritingtwowiderstripesperpendicularlytothe?rstpatternofFig.4?b?,showsthatthePFMresponsecanbeswitched.ThesePFMmeasurementsarenotquantitative;sothatwecannotconcludeonapossibledecreaseofthepolarizationoftheBFO?lmwhenthicknessdecreases,asreportedforPbTiO3,forinstance.26However,theydemonstratethattheferroelec-triccharacterispreservedinBFOlayersdowntoathicknessof5nm.
Insummary,wehavesuccessfullygrownepitaxialhet-erostructuresintegratingaLSMObottomelectrodeandaBFOlayer.Thegrowthofbothlayersistwodimensional;theyareheavilystrainedandthesurfaceofthestructureisunit-cell?at.SQUIDmeasurementsindicatethattheLSMOlayerisferromagneticwithaTCof330K,whiletheBFO
FIG.4.Topography?a?andPFMimage?b?afterwritingstripedomainsusingtheAFMtipasatopelectrodeofthe5nmBFOlayer.PFMimage?c?afterwritingtwowiderstripesperpendicularlytothepatternseenin?b?.
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