Magnetic Gap of Fe-Doped BiSbTe 2 Se Bulk Single Crystals Detected by Tunneling Spectroscopy and Gate-Controlled Transports - Yano et al

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pubs.acs.org/JPCLLetterMagneticGapofFe-DopedBiSbTe2SeBulkSingleCrystalsDetectedbyTunnelingSpectroscopyandGate-ControlledTransports,+RikizoYano,*AndreiKudriashov,HishiroT.Hirose,TaikiTsuda,HiromiKashiwaya,TakaoSasagawa,,+AlexanderA.Golubov,VasilyS.Stolyarov,*andSatoshiKashiwaya*CiteThis:J.Phys.Chem.Lett.2021,12,4180−4186ReadOnlineACCESSMetrics&MoreArticleRecommendations*sıSupportingInformationABSTRACT:Topologicalinsulatorswithbrokentime-reversalsymmetryandtheFermilevelwithinthemagneticgapattheDiracconeprovidesexotictopologicalmagneto-electronicphenomena.Here,weintroduceanimprovedmagneticallydopedtopologicalinsulator,Fe-dopedBiSbTe2Se(Fe-BSTS)bulksinglecrystal,withanidealFermilevel.Scanningtunnelingmicroscopyandspectroscopy(STM/STS)measurementsrevealedthatthesurfacestatepossessesaDiracconewiththeDiracpointjustbelowtheFermilevelby12meV.ThenormalizeddI/dVspectrasuggestagapopeningwithΔmag∼55meV,resultingintheFermilevelwithintheopenedgap.Ionic-liquidgated-transportmeasurementsalsosupporttheDiracpointjustbelowtheFermilevelandthepresenceofthemagneticgap.Thechemicalpotentialofthesurfacestatecanbefullytunedbyionic-liquidgating,andthustheFe-dopedBSTSprovidesanidealplatformtoinvestigateexoticquantumtopologicalphenomena.opologicalinsulators(TIs)possessauniquetime-reversaltetradymites.ThetetradymiteshavelayeredcrystalstructuresTinvariantsurface(edge)state,theso-calledmassless(Figure1a).WeshouldcareabouttheunintendedintergrowthDiraccone(e.g.,linearbanddispersion),whichoffershigh-ofmagneticimpuritiesofFe−SecompoundspromotedbyFe1−10doping.25−27Thisintergrowthmayoccuroveracertainmobilitycarriersandpromisingspinfunctionalities.Breakingtime-reversalsymmetryonTIsbyapplyingalargetemperaturerangeandbeeasilydrivenbyaninhomogeneousmagneticfieldormagnetizationannihilatesthetime-reversalFedistribution.Indeed,owingtospecialcaresuchasinvariantpoint(theDiracpoint:DP)andopensthemagnetichomogeneousmixingathightemperaturesandrapidgap,Δmag(theso-calledmassiveDiraccone).Themassivequenching,wegrewFe-dopedBi2Te2SeandFe-dopedDiracstateinducesremarkabletopologicalphenomena,suchasBiSbTe2Se(Fe-BSTS)ashighbulk-insulatingmagnetically28,29thequantumanomalousHall(QAH)effectandtheimagedopedTIsandreportedobservationofunusualproximity28DownloadedviaUNIVOFCONNECTICUTonMay16,2021at09:22:52(UTC).magneticmonopole.Besides,fabricatingheterostructureswitheffects.However,thedetailedelectronicstructure,inothermagneticinsulatorsorsuperconductors,thechiraledgeparticular,thelocationoftheDPandEF,isstillanopenstatesproducetopologicalelectromagnetic(ME)effectsandquestion.Seehttps://pubs.acs.org/sharingguidelinesforoptionsonhowtolegitimatelysharepublishedarticles.virtualexoticelementaryparticlestates,e.g.,axionMEtermsHere,wereportthedetailedelectronicbandstructureoftheandMajoranaFermions.2,11−13Fe-BSTS.ItsschematicbandstructuresaboveandbelowtheTherearetwokeyfactorsintheobservationofthesurface-Curietemperature(TCuri)aresummarizedinFigure1b,c,respectively.Weperformedinsitucleavagescanningtunnelingdrivenphenomena:idealFermilevelEF(withinthemagneticmicroscopyandspectroscopy(STM/STS)measurements.Fe-gapandthebulkbandgap)andhighbulkinsulatingnature.FornonmagneticTIs,tremendouseffortshavebeenputintoBSTShasahighbulkinsulatingnaturewithabandgapofΔbulk∼400meV,andtheFermilevelEFisfoundtobeclosetothealloyingappropriateBi−Sb−Te−Secompositionsconsideringdefectchemistry14−18toovercomethetwodrawbacks.OntheDP(EDP).Furthermore,wediscoveredamagneticgapΔmagattheDP.Thetransportmeasurementstunedwithelectric-otherhand,achievinghighbulkinsulatingmagneticTIisstilldouble-layertransistors(EDLTs)alsosupportthesesurfacechallenging.Thecommonapproachistoutilizeathinfilmof19−23magneticTIstoreducethebulkconductioncontribution.WhileCr-doped(Bi,Sb)Se19andMnBiTe24thinfilmsReceived:March17,20212324exhibittheQAHeffect,bulkmagneticTIswillprovideAccepted:April12,2021complicatedheterostructuredeviceswithahighdegreeofPublished:April26,2021freedom.Inthecontextofsearchingfordesirablebulkmaterials,wefocusonFeasadopantinto(Bi,Sb)sitesinBibased©2021AmericanChemicalSocietyhttps://doi.org/10.1021/acs.jpclett.1c008694180J.Phys.Chem.Lett.2021,12,4180−4186

1TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetter(QL)ofFe-BSTS,asshowninFigure1a.TheseQLsareweaklybondedbyvanderWaalsforcesandterminatedbychalcogenatoms(Se,Te).AlocalSTMstudyoftheflatterracesrevealedwell-orderedhexagonallatticeswithrandomlyarrangedatomicdefects,reflectingitshomogeneoussub-stitutionof(Bi,Sb,Fe)and(Te,Se)sites(seeFigure1a,theinset).Weconfirmedthatthespatialelectrondensitydistributionneardefects(notshownhere)showedatypical30−32spectrumforotherBibasedtetradymites.Theformoffingerprintsdependsonthetypeofdefectsandtheirdepthin33theQLs;e.g.,thesurfacehasbrighttriangulardotscorrespondingtothechalcogenvacanciesdescribedinref34.Figure2ashowstheaveragedSTSspectrameasuredat4.2K(blueline)and77K(red).TherapidrisearoundVT=−100mVand300mVcorrespondstothebulkvalenceband(BVB)andbulkconductionband(BCB),respectively,andthusthebulkbandgapisΔbulk≃400meV(markedasagreen-whitegradient).Thezero-biasvoltage(FermienergyEF)islocatedFigure1.SummarizedbandstructuresandscanningtunnelingclosetotheBVB,ahallmarkofap-typesemiconductor.Withinmicroscopy.(a)ThecrystalstructureofFe-BSTS.Theupperandbottomfiguresindicatethetopviewandthelayeredstructure,thebandgap,almostlinearspectraappearedregardlessoftherespectively.Thearrowindicatesasinglequintuplelayer(QL).Bandmeasurementspots(seetheinsetofFigure2a),whichisastructuresofFe-BSTS(b)aboveand(c)belowtheCurietopologicallyprotectedfeature,andthelinearbandrepresentstemperature.TheparametersweredeterminedbySTMandgate-thesurfacestates(theDiraccone).TheDPwasestimatedastunedtransports.Δmag=55meV,EDP=−12meV,andEact,b=33.3EDP∼−12meVfromtheextrapolationofthelinearpartofthemeV(seetextformoredetails).(d)A200nm×200nmSTMimagespectra(insetofFigure2a).Furthermore,thenormalized(biasvoltageVT=183mVandtunnelcurrentIT=104pA)ofthein35spectrumofdI/dV(4.2K)dividedbythedI/dV(77K)situcleavedcrystal.Atomicallyflatterracesareseparatedby1.03nmheightsteps(thebottomleftinsetdepictstheprofilealongthedashedrevealssomegapsaroundtheDP(seeFigure2b).Basedon28,36lineoftheSTMimage),andtheheightoftheterracescorrespondstopreviousreports(TCurri<50K)andothermagnetically22,23QL.Inthetop-rightinset,a10nm×10nmatomicallyresolvedimagedopedtetradymitesystems(TCurri∼10K),themeasure-withatypicalsetofdefects.menttemperaturesshouldcrosstheCurietemperatureofthepresentmaterial,andtheobservedgaprepresentsthemagneticstates.CombiningmicroscopicSTSandmacroscopictransportgapattheDPwithasizeofΔmag∼55meV,whichis36−38resultsconsistentlyensuresanidealEFpositionwithinΔmagatcomparabletoothermagneticTIs.Welinkthefactthataverylowtemperature.themagneticgapispartiallyfilledintheregionoftheDiracOwingtotheexcellentcleavagepropertyofFe-BSTS,sizablepointbecauseofthetemperaturefluctuationsandthelargecrystalswerecleavedinthechamber,andanatomicallyflatnumberofatomicdefectssaturatingthemagneticgapbysurfaceenablingSTM/STSmeasurementswasobtained.STMelectronsgivinganonzerobackground.Thegapatthetime-mappingwithaconstantcurrentof104pAandabiasvoltageconservedDPisahallmarkofthebrokentime-reversalof183mV(Figure1d)showclearatomicallyflatterraces.Thesymmetryduetoferromagneticordering,whereastypicalother39observedstepheightwas1.03nm(Figure1d,inset),whichorigins,e.g.,theKondoeffect,producethegapstructureatcorrespondstoafiveatomiclayer,theso-calledquintuplelayertheEF.Figure2.Scanningtunnellingspectroscopy.(a)Averagetunnellingspectraat4.2K(blueline)and77K(redline).Theinsetshowsahighlightaroundthezero-biasvoltage.Thedashedlinerepresentsalineardispersionapproximation,andthearrowindicatestheestimatedDiracpointat−12mV.(b)NormalizeddI/dVspectrumof4.2Kbythe77Kspectra.Aclear55mVgapappearsneartheDiracpoint.InsetsareschematicsurfacestructuresbelowtheCurietemperature.4181https://doi.org/10.1021/acs.jpclett.1c00869J.Phys.Chem.Lett.2021,12,4180−4186

2TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetterFigure3.ExperimentalsetupsandtransportpropertiesofaFe-BSTS.(a)Temperaturedependenceofresistivitywithandwithoutgatingvoltage.Thelabel“w/ogating”indicatesthemeasurementperformedjustafterloadingtheionic-liquid(IL)butwithoutapplyingexternalgatingvoltage.TheinsetistheschematicofatransportmeasurementsetupwithILgatingonabulksinglecrystal.(b)Hallresistivityforvariousgatingvoltagesat2K.Theinsetshowsazoomed-inplotforVG=+2V.Dashedlinesforeachplotrepresentthebestfittingresultsbythetwo-bandmodel.(c)ChangeinsheetmagnetoconductanceofNo-IL(withoutIL)withaperpendicularmagneticfieldatseveraltemperaturesrangingfrom2to50K.Thedashedblacklinesrepresentfittingresultsat2−30KbytheHLNmodel.TheinsetshowsapolarplotofthemagnetoresistanceoftheNo-ILcrystalwithamagneticfieldof8Tat2K.(d)Temperaturedependencesofthecarrier(toppanel)andmobility(bottompanel)forthebulkandsurfaceoftheas-grownFe-BSTScrystal(No-IL).TheinsetisthetemperaturedependenceofthephasecoherencelengthobtainedusingtheHLNmodel.ThedashedlineisafittingresultforT−1/2above20K.TheinsetofFigure2bshowstheschematicbandstructureobservedinnonmagneticTIs,e.g.,inrefs45and46.ThedeterminedfromtheSTSdI/dVspectra.Themostprominentmagnetotransportpropertiesalsochangearoundthistemper-featureisthatthelocationoftheFermilevelisjustabovetheature,asdiscussedlaterinthetransportsection.Therefore,weDPandwithinthemagneticgap,whichisanidealsituationtoclaimthisupturncanbeascribedtothegapopeningnear10K.observeexoticmagneticgap-originphenomenadescribedinThehigh-temperatureresistivityfollowedthree-dimensionaltheintroductionsection.variablerangehopping,whichiscommonlyobservedinTIs14,17,45,47Weinvestigatedthetransportpropertiesofthegate-withhighlyinsulationinthebulk.FromthestandardcontrolledFe-BSTSbulksinglecrystaltodeterminetheArrheniusplot,thevalueoftheactivationenergyforthebulklocationsoftheEFandtheEDP.Theionic-liquid(IL)gatinginwasdeterminedtoEact,b=33.3meV.ReferringtoFigure1b,c,EDLTenableseffectivecarriercontroljustnearthesurfacethevaluesofEDP,Δmag,andEact,bareconsistentwiththe(typicaleffectivedepth∼severalnanometers).40−43Ingeneral,estimatedbandstructure,i.e.,theFermilevelshouldbelocatedthistechniqueisappliedtothin-filmmaterialsnowadays,anditwithinthemagneticgapatlowtemperatures.isdifficulttoachieveambipolarconductionforbulkThedominantsurfacecontributionwasconfirmedfrommaterials.44Incontrast,weobservedtheambipolarsurfacemagnetoresistance(MR=(ρ(H)−ρ(0))/ρ(0)),magneto-carrierconductionofFe-BSTSevenusingabulkcrystal,owingconductance,andHallresistivity(Figure3b).DetailedMRtoitshighsurfacemobility.TheexperimentalsetupisshownindataaresummarizedintheSupportingInformation.The2-foldtheinsetofFigure3a.FurtherdetailsareprovidedintherotationalsymmetryintheMRisacharacteristicofthetwo-SupportingInformation.BecauseloadingtheILitselfaffectsdimensionalelectronnaturefromthesurfacestates(insetofcarrierdensity,welabeled“No-IL”and“w/ogating”astheFigure3c).Figure3cshowsthesheetmagnetoconductancestateoftheas-growncrystalwithoutILandjustafterloadingandfittingresults(blacklines)usingthesimpleHikami−46,48ILbutwithoutvoltage-control,respectively.ThepositivegateLarkin−Nagaoka(HLN)modelforweakantilocalizationvoltageprovideselectroncarrierdopingatthetopofthe(WAL):crystal.Allgate-voltagecontrollingtookplaceaftercoolingtoÄÅÅÉÑÑeB2ÅÅijj1yzzijjByzzÑÑ230Kinavacuumedchambertopreventchemicalreactions.GB()−≃G(0)αÅÅÅÅΨ+−jjzzlnjjzzÑÑÑÑAsafirststep,weevaluatedtheas-grownFe-BSTSbulk2π2ℏÅÅjj2BzzjjBzzÑÑÅÇkϕϕ{k{ÑÖcrystal(No-IL).Thetemperaturedependenceofresistivityshowedinsulatingabove50K,whereastheslopedecreasedwhereα,e,ℏ,andΨaretheWALcoefficient,electronicbelow25K,asshowninFigure3a.Interestingly,theresistivitycharge,reducedPlanckconstant,anddigammafunction,increasedagainbelow10Kanddidnotfollowthetypical−logrespectively.Theα∼−1wasobtainedatthelow-temperatureTdependenceexpectedfortheKondoeffectwhichisoftenregion.Fromthecharacteristicmagneticfield,Bϕ,the4182https://doi.org/10.1021/acs.jpclett.1c00869J.Phys.Chem.Lett.2021,12,4180−4186

3TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetterFigure4.SchematicbandstructureandanalyticalresultsforIL-gatedFe-BSTS.(a)Schematicbandstructureandtransfercharacteristics(RtotalvsVG)oftheEDLT-basedFe-BSTSbulkcrystalat230K.ThedottedlinescorrespondtotheestimatedBCB,BVB,andFermienergylevelofbulkbandsandVG.Voltagedependenceof(b)carrierand(c)mobilityforbulk(red)andsurface(blue).Thecircleandtrianglesymbolsrepresenttheaboveparametersofholesandelectrons,respectively.ThestarandsquaresymbolsareestimatedattheVGpositionfortheNo-ILandw/ogatingcases,respectively.ℏapproximately10KwheremostmagneticTIsshowacoherencelengthlϕcanbeevaluatedasBϕ=.Almost22,234elϕferromagnetictransition.TheHallresistivityshowedperfectfittingresultswereobtainedinthetemperaturerangeofgentlecurves,indicatingthatatleasttwocomponentsshould2−50K.Thepower-lawfitofthecoherencelengthabove20Kexist.Here,weappliedthestandardtwo-bandmodel(withinyieldedT−0.45∼T−1/2,indicatingtwo-dimensionaldecay46,49theDrudemodelinlow-field)fittingtotheHallresistivity,(insetofFigure3d).Interestingly,thecoherencelengthbelowassumingthesurfaceandbulkcontributionsdescribedinref10KdeviatesfromtheT−1/2curveandissuppressedat50.223()RRH,surfρρbulk++H,bulksurfBRH,surfRH,bulk(RH,surf+RH,bulk)Bρ()B=xy222()ρρsurf+++H,bulk(RRBH,surfH,bulk)whereRH(ρ)surf/bulkrepresentstheHallcoefficients(resistivity)holedoping.AlltheHallresistanceshowedgentlecurveslikeforsurface/bulk,respectively.Thismodeliswidelyappliedfor17,51theNo-ILcase,includingVG=+2and+1.2VwhichlookTIs.Usingthestandardrelation,wecanobtainthesamplelinear.AsshownintheinsetofFigure3b,theslopeofVG=+2t1parametersasfollows:R=,R=,andVwasnegative,indicatingsuccessfulelectrondopingbytheILH,surfensurfH,bulkenbulkRgating.MRwasalsochangedbygating(FigureS3d).TheseH,surf/bulkμsurf/bulk=ρ,wheret,nsurf,andnbulkarethesamplefactsindicatethattheILgatingontothebulkcrystalachievedsurf/bulkthicknessandcarrierdensitiesofthesurfaceandbulk,bipolartransport.Figure4a−cshowssummarizedfittingresultsfromthetwo-respectively.Asaresult,weobtainedanexcellentfit(dashedbandmodel.ThebulkholecarrierslightlydecreasedwithlinesinFigure3bandFigureS3cforthetemperatureelevatinggatevoltage,whilethesurfacecarriershowedthep−dependenceoftheNo-ILsample).Thefittingparametersncarrier-typetransitionaround+0.5V.ThesurfacemobilityobtainedaresummarizedinFigure3d.ThetemperaturedrasticallydroppedtothebulkvaluewhentheVG=+1.2Vdependenceofthecarrierdensityandmobilityshowedtypicaland−1V,indicatingthatthechemicalpotentialofVG=1.2p-typesemiconductingbehavior,ensuringthevalidityofthe2(−1)VislocatedneartheBCB(BVB).Theanalysesalsoanalyticalfitting.Thesurfacemobilityexceeded1500cm/(Vrevealedthatthesurfacecontributionalsochangedfrom26%s),whichmakestheplotofHallresistivitycurved.EDLT(No-IL)to60%(2V),comparabletopreviousreportsusingagatingmainlytunesthesesurfacestatesandthusenablesusto5345thin-filmsampleandnanowires.Consideringthetrendsofevaluatethesurfacestates,evenusingabulkcrystal.thegatedproperties,wecanestimatethelocationoftheFigure4ashowsthegate-voltagedependenceofresistanceatsurfacechemicalpotentialofNo-ILandw/ogating.The230K,wherethebulkcontributiondominatesalmosttheappropriatepositionsare−0.25VforNo-ILand−0.5Vforw/entiretransport.Despiteasmallchangeintheresistance,aogating,resultinginsmoothlyconnectedcarrierdensitylines.smallhystereticloopappeared.ThelooptracedthesamecyclicThehighestmobilityshouldreflectthenearestchemicalloopsatleastthreetimesevenatdifferentsweepspeeds(1−2potentialtotheDP,andthus,theFermienergyoftheas-mV/s).Thislooprepresentsonlyaunipolarnaturesimilartogrowncrystal(No-IL)isclosesttotheDP.Therefore,thisIL-4452thebulkMoS2and(Bi1−xSbx)2Te3thinfilmatthisgated-transportmeasurementalsoindicatesthatthelocationoftemperature.However,low-temperaturetransportdrasticallytheDPisjustbelowtheFermienergylevel.ToachievefineEFaffectedtheIL-gatingeffect.Figure3bshowstheHalltuningjustontotheDPusingILgating,thepromisinggateresistanceat2Kfordifferentgatevoltages.Notethat,evenvoltageisapproximately0.25V,wherethep−ncarrier-typeforjustloadingtheILontothesample,theresistancedrasticallythesurfacecarrierschanges.Theseanalyseswiththetwo-banddroppedatlowtemperatures(Figure3a),andtheslopeofthemodelconsistentlyexplainallthegated-transportmeasure-Hallresistancedecreased,meaningthattheILitselfleadstomentsandsupporttheSTM/STSconclusionoftheidealEF4183https://doi.org/10.1021/acs.jpclett.1c00869J.Phys.Chem.Lett.2021,12,4180−4186

4TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetterandDPpositions.Therefore,weconcludethatFe-BSTSisaTaikiTsuda−AppliedPhysics,NagoyaUniversity,Nagoyapromisingbulkmaterialforobservingquantumphenomena464-8603,JapandrivenbythemassiveDiracconeatverylowtemperaturesHiromiKashiwaya−NationalInstituteofAdvancedwhereintheexcitationiswellsuppressedbythesurroundingIndustrialScienceandTechnology(AIST),Tsukuba305-temperature.8568,JapanInsummary,weinvestigatedthesurfacebandstructuresofTakaoSasagawa−LaboratoryforMaterialsandStructures,Fe-BSTSviaSTS/STMandIL-gated-transportmeasurements.TokyoInstituteofTechnology,Yokohama226-8503,JapanThelocalSTSmeasurementshowedtwonotablefeaturesofAlexanderA.Golubov−TQPSSLab,CenterforPhotonicsthesurfacestate:theDPneartheFermilevelandthegappedand2DMaterials,MoscowInstituteofPhysicsandstatesattheDP(4Knormalizedspectra),implyingamagneticTechnology,Dolgoprudny,MoscowOblast141700,Russia;gapopening.TheIL-gated-transportmeasurementcombinedFacultyofScienceandTechnologyandMESA+Instituteofwiththetwo-bandanalysesalsosupportsthattheDPisnearNanotechnology,Enschede7500AE,TheNetherlandstheidealposition.BothresultscanconsistentlybeunderstoodCompletecontactinformationisavailableat:withintheframeworkofthebandstructureofFigure1b,c,https://pubs.acs.org/10.1021/acs.jpclett.1c00869ensuringthemagneticgapandtheFermienergyabovetheDP.Therefore,theFe-BSTSbulksinglecrystalisapromisingAuthorContributionsplatformfordetectingexoticphenomenasuchastheQAH+R.Y.andV.S.S.contributedequallytothiswork.effect.Notes■Theauthorsdeclarenocompetingfinancialinterest.METHODSWegrewsinglecrystalsofFe-BSTSusingamodifiedBridgman36methodreferredtoasFe-orMn-dopedBi2Se3,Fe-doped■ACKNOWLEDGMENTS2829Bi2Te2Se,andFe-dopedBSbT2Se.ThedetailsofcrystalTheauthorsthankProf.YukioTanakaandDr.KoheiTsumuragrowthandsamplecharacterizationaredescribedintheforfruitfuldiscussions.ThisstudywassupportedbyJSTSupportingInformation.STM/STSmeasurementswereCREST(GrantNo.JPMJCR16F2)andKAKENHI(GrantperformedusingJT-SPM(SPECS).ThecrystalswereNos.JP15H05851,15H05853,16H03847,18H01243,mechanicallycleavedinanultrahighvacuum(UHV,∼10−1020H00131,21H04652,and21K13854),ResearcherExchangembar).ThetransportpropertieswereevaluatedusingaPPMSProgrambetweenJSPSandRFBR(JPJSBP120194816),and(QuantumDesignInc.)withanexternalgate-voltagesource/JSPSCore-to-Coreprogram“OxideSuperspin”(OSS)currentmonitorR6244(Advantest).DetailsoftheIL-gatinginternationalnetwork(GrantJPJSCCA20170002).CrystalconfigurationareprovidedintheSupportingInformation.growthwassupportedbyCollaborativeResearchProjectsinMSL-TokyoTech.,Japan.A.A.G.andV.S.S.acknowledgethe■ASSOCIATEDCONTENTGrantRSF-ANR20-42-09033.*sıSupportingInformationTheSupportingInformationisavailablefreeofchargeat■REFERENCEShttps://pubs.acs.org/doi/10.1021/acs.jpclett.1c00869.(1)Hasan,M.Z.;Kane,C.L.Colloquium:TopologicalInsulators.Crystalpreparationandcharacterization,EDLTdeviceRev.Mod.Phys.2010,82,3045−3067.fabricationprocess,anddetailedmagnetotransport(2)Qi,X.-L.;Zhang,S.-C.TopologicalInsulatorsandSuper-propertiesoftheas-growncrystal(PDF)conductors.Rev.Mod.Phys.2011,83,1057−1110.(3)Kou,L.;Ma,Y.;Sun,Z.;Heine,T.;Chen,C.TwoDimensionalTopologicalInsulators:ProgressandProspects.J.Phys.Chem.Lett.■AUTHORINFORMATION2017,8,1905−1919.CorrespondingAuthors(4)Ando,Y.TopologicalInsulatorMaterials.J.Phys.Soc.Jpn.2013,RikizoYano−InstituteofMaterialsandSystemsfor82,102001.(5)Si,N.;Yao,Q.;Jiang,Y.;Li,H.;Zhou,D.;Ji,Q.;Huang,H.;Li,SustainabilityandAppliedPhysics,NagoyaUniversity,H.;Niu,T.RecentAdvancesinTin:FromTwo-DimensionalNagoya464-8603,Japan;orcid.org/0000-0003-1959-QuantumSpinHallInsulatortoBulkDiracSemimetal.J.Phys.Chem.311X;Email:yano-rikizo@nagoya-u.jpLett.2020,11,1317−1329.VasilyS.Stolyarov−TQPSSLab,CenterforPhotonicsand(6)Kane,C.L.;Mele,E.J.Z2TopologicalOrderandtheQuantum2DMaterials,MoscowInstituteofPhysicsandTechnology,SpinHallEffect.Phys.Rev.Lett.2005,95,146802.Dolgoprudny,MoscowOblast141700,Russia;Dukhov(7)Xue,H.;Lv,W.;Wu,D.;Cai,J.;Ji,Z.;Zhang,Y.;Zeng,Z.;Jin,ResearchInstituteofAutomatics(VNIIA),Moscow127055,Q.;Zhang,Z.TemperatureDependenceofSpin−OrbitTorquesinRussia;orcid.org/0000-0002-5317-0818;NearlyCompensatedTb21Co79FilmsbyaTopologicalInsulatorEmail:vasiliy.stoliarov@gmail.comSb2Te3.J.Phys.Chem.Lett.2021,12,2394−2399.SatoshiKashiwaya−AppliedPhysics,NagoyaUniversity,(8)Fu,L.;Kane,C.L.;Mele,E.J.TopologicalInsulatorsinThreeDimensions.Phys.Rev.Lett.2007,98,106803.Nagoya464-8603,Japan;Email:s.kashiwaya@nagoya-u.jp(9)Pi,S.-T.;Wang,H.;Kim,J.;Wu,R.;Wang,Y.;Lu,C.-K.NewAuthorsClassof3DTopologicalInsulatorinDoublePerovskite.J.Phys.Chem.Lett.2017,8,332−339.AndreiKudriashov−TQPSSLab,CenterforPhotonicsand(10)Tian,L.;Liu,Y.;Meng,W.;Zhang,X.;Dai,X.;Liu,G.Spin-2DMaterials,MoscowInstituteofPhysicsandTechnology,OrbitCoupling-DeterminedTopologicalPhase:TopologicalInsulatorDolgoprudny,MoscowOblast141700,RussiaandQuadraticDiracSemimetals.J.Phys.Chem.Lett.2020,11,HishiroT.Hirose−LaboratoryforMaterialsandStructures,10340−10347.TokyoInstituteofTechnology,Yokohama226-8503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