《发光学报》英文论文投稿模板.docx

第X卷第X期发光学报VOLXNo.xXXXX年X月ChineSeJoUmalOfLUmineSCenCexxx.XXXX注：作者编排论文时，为了调整方便，页面布局可采用单栏排版。ArticleIDHighlyFlexibleGreenLight-emittingDiodeBasedonCsPbBr3PerovskiteQuantumDots（二号）GUOJie,LUMin,SUNSi-qi,HUQiang,ZHANGJia,BAIXue*（四号，需用*标明通信作者）（StateKeyLaboratoiyofIntegratedOptoelectronics,CollegeofElectronicScienceandEngineering,JilinUniversity,Changchun130012,China）*CorrespondingAuthor,E-mail:baix血.edM.cnAbstract:Flexibleinformationdisplayshavethepromisingpotentialforthefutureoptoelectronicapplication.However,achievingthehighlyefficientandstableflexiblelight-emittingdiodes（LEDs）isstillabigchallengeduetothelimitedchoicesofelectrodematerialsandflexiblesubstrates.Herein,theflexibleperovskitelight-emitting（Iiodes（Pe-LEDs）bycombiningtheflexiblesubstratebasedonaphotopolymerwiththeCsPbBr?quantumdots（QDs）emittinglayerwerefabricated.Inordertoimproveelectronsinjectionandtransport,Agwasusedasthecathode.Asaresult,thegreenlightemittingPe-LEDswithhighluminanceof10325cd,m-2andhighcolorpuritywiththefull-width-at-half-maximum（FWHM）of19nmwereobtained.Inaddition,thePe-LEDsexhibitgoodflexibilityandmechanicalductility,andtheas-preparedflexibledevicestillmaintainsitsoptoelectronicperformanceevenafterrepeatedbending100timesunderabendingangleofabout180o.Theresearchpresentsafurthersteptowardthefutureapplicationofflexibledisplays.（小五号）（一般应包括：目的，方法，结果，结论）（全文所有的O都用全角）Keywords:CsPbBnQDs;photopolymer:Agelectrode;flexiblelight-emittingdiodeCLCnumber:0482.31Documentcode:A基于CSPbBn钙钛矿量子点的高柔性绿光发光二极管（二号）郭洁，陆敏，孙思琪，胡强，张佳，白雪*（四号，需用*标明通信作者）（吉林大学电子科学与工程学院，集成光电子学国家重点联合实验室，吉林长春130012）摘要：众所周知，柔性信息显示将在未来的光电应用中发挥重要作用。然而，由于电极材料和柔性衬底的选择有限，制备高效、稳定的柔性发光二极管仍然存在巨大的挑战。以光聚合物作为柔性衬底，CSPbBr3量子点作为发光层，成功制备柔性钙钛矿发光二极管。为了进一步改善电子的注入和传输，采用Ag作阴极。因此，得到具有高柔性的钙钛矿发光二极管，发光二极管的最高亮度为10325cdm2且有高色纯度(FWHM=I9nm)。此外，制备的钙钛矿发光二极管具有良好的柔性和机械延展性。在大约180°的弯曲角度下反复弯曲100次后，仍然保持着良好的器件性能。该研究为未来柔性显示器的应用奠定研究基础。关犍词，CSPbB门量子点；光聚合物；银电极：柔性发光二极管(文中若有公式，请用公式编辑器书写)1Introduction(四号)Overthepastfewyears,organic-inorganichybridperovskitematerialshaveattractedconsiderableresearchinterestduetotheirexcellentproperties,whichresultinthewideapplications,especiallyfortheflexibleoptoelectronicdevices1'(两个及以上连续参考文献,标号之间用连字符连接).Nevertheless,organic-inorganichybridperovskitematerialsexhibittheinferiorstabilitythatrestrictingtheirpracticalapplications.Comparedtothehybridorganic-inorganichalidecounterparts,allinorganiccesiumleadhalidePerOVSkite(CSPbX3,X=Cl,Br,Iormixed)quantumdots(QDs)exhibitanenhancedstability,andmeanwhiletheyalsodemonstratearemarkableopticalandoptoelectronicperformanceincludingtheexcellentphotoluminescencequantumyield(PLQY)levelsreaching90%,highcolorpurity,widecolorgamut,andhighcharge-carriermobility".Therefore,theyhavethehugepotentialasanidealemissivelayermaterialstofabricatehighlyefficientperovskitelight-emittingdiodes(Pe-LEDs)5.191Fordisplayapplications,flexible,curveddisplaysarekeyelementsinfutureoptoelectronicdevices1''.However,therearestillchallengesinthefabricationofflexiblePe-LEDsowningtothesophisticatedfabricatedsteps,includingthesolution-processedspin-coatingwithvariouschemicals,high-temperatureannealingandvacuumevaporation.Thesemultipleproceduresconsiderablylimitthedevicearchitecturedesignsaswellasthechoicesofappropriateflexiblesubstratesandelectrodes.Thesoftplasticsubstrateisgenerallyaproperalternativeforflexiblesubstrateduetoitslowcostandhighflexibility"".However,theycanbeeasilycorrodedbysomeacidicreagentandorganicsolvents(toluene,chloroform)duringthefabricationofLEDs.Fortheelectrodes,althoughtheIndium-TinOxide(ITO)hasbeenwidelyusedintheLEDs"",itisn,tsuitableforflexibleLEDsduetoitspoormechanicalrobustnessj.Therefore,toachievehigh-perfbrmanceflexiblePe-LEDs,weneedtochooseasuitableelectrodeandsubstratematerial.Here,wefabricatedaflexiblePe-LEDbasedonallinorganicCsPbBr?perovskiteQDsemissivelayers,inwhichtheperovskiteQDsexhibitanefficientgreenlightemissionwiththePLQYof75%.PhotopolymerNOA63wasusedasaflexiblesubstratebyspin-coatingitontheSisubstrateandbeingstrippedfromtheSi.Simultaneously,AgfilmwasusedasacathodebysimplethermalevaporationComparedwiththeITOelectrode,theAghashigherconductivityandbettermechanicalductility.Inaddition,Agascathodereducedenergybarrierbetweenthecathodeandelectrontransportlayer(ETL),whichismoreconducivetoelectroninjection.Consequently,theas-preparedgreenlightemittingPe-LEDsexhibitgoodflexibility,highbrightnessof10325cdm2,highcolorpuritywiththefull-width-at-half-maximum(FWHM)of19nmandlowthresholdvoltageabout2.6V.ThedeviceperformancestillmaintainedwhentheflexiblePe-LEDswererepeatedlybent100times.TheseresultsillustratethattheflexiblePe-LEDshaveagreatapplicationprospectinthefieldoftheflexibledisplays.2 Experiment(四号)2.1 Materials(五号)Cs2CO3,andPbBr2werepurchasedfromSigma-Aldrich.Oleicacid(OA,90%)and1-octadecene(ODE,90%)werepurchasedfromAlfaAesar.Oleylamine(OLA,80%-90%)waspurchasedfromAladdin.2.2 SynthesisofCsPbBr3QDsTheCsPbBr3perovskiteQDsweresynthesizedonthebaseofthepreviouslyreportedmethod.CesiumOleate(Cs-OA)waspreparedbymixingCs2CO3(O.8i4g),OA(2.5mL),andODE(30.0mL)ina100mLthree-neckedflask,whichwasdegassedanddriedundervacuumfor1hat120,thenheatedto150°CunderN2untilaclearsolutionwasobtained.ForthesynthesisofCsPbBr3QDs,10.0mLODE,0.138gPbBr2,1.0mLOAand1.0mLOLAwereloadedintoa50mLthree-neckedflask,degassedanddriedbyapplyingvacuumfor1hat120;afterthesolutionbecameclear,thetemperaturewasraisedto180and1mLofcesiumoleatesolutionwasquicklyinjected.5secondslater,thereactionmixturewascooleddowntoroomtemperatureinanice-waterbath.Thereactionmixtureneedstobecentrifugedfor10minat5000rmin,andtheobtainedprecipitatewasredispersedin5.0mLofhexane,centrifugeddownagainfor10minat10000rmin,andprecipitatewasredispersedin1.0mLofhexane.2.3 DeviceFabricationFirstly,photopolymer(NOA63,Norland)wasspin-coatedontoacleanedsiliconwaferataspeedof1500r/minfor40sandexposedtoanultravioletlampfor3min.Then,theAgelectrodewasgrownonthephotopolymerfilmviathermalevaporation.Subsequently,ZnOnanocrystals(NCs)solutionwasspin-coatedoniotheAgelectrodeataspeedofI000r/minfor40s,andannealedonthehotplateat150for10min,afterdowntoroomtemperature.Then,thesubstratewastransferredintoaglovebox.Asolutionofpolyethylenimine(PEI)(dissolvein2-methoxyethanolinamassfractionsof0.2%)wasspin-coatedontotheZnOfilmat3O(X)rpmfor40Sandannealedat125for10min.CSPbB门QDSwerespin-coatedataspeedof1000rpmfor40s.Next,4,4,-Bis(carbazole-9-yl)biphenyl(CBP),4.4',4'-IriS(carbazol-9-yl)-triphenylamine(TCTA),MOO3,andAuweresequentiallydepositedusingathermalevaporationunderabasepressureof7×104Pa.Atlast,theflexibleLEDswasstrippedfromthesilicontemplate.2.4 CharacterizationsAbsorptionspectraweremeasuredusingaShimadzuLJV-2550spectrophotometer.ThePLspectraweremeasuredusinganOceanOptics.X-raydiffraction(XRD)patternswereacquiredusingaBrukerD8AdvanceXdiffractometer(CuK,=0.15406nm)(文中变量用斜体，数字与单位之间空格).Thetransmissionelectronmicroscopy(TEM)andhigh-resolutionTEM(HRTEM)imageswereobtainedonaFEITecnaiF20microscope.Thecurrentdensity-voltage-luminanceofLEDwasmeasuredbyAKeithley2612Bsourcemeasureunit.TheLEDbrightnesswasdeterminedusingaPhotoResearchSpectraScanspectrometerPR650.Theelectroluminescence(EL)spectrawererecordedwithaMayaspectrometer(OceanOptics)coupledtoanopticalfiber.3 ResultsandDiscussionTheUV-visibleabsorptionandPLemissionspectraofCsPbBr?perovskiteQDsareshowninFig.1(a).ThefirstexcitonabsorptionpeakandPLemissionpeakarelocatedat500nmand513nm,respectively.TheCSPbB门perovskiteQDsexhibitasmallstokesdisplacementandanarrowFWHMabout18nm.TheinsetinFig.1(a)showsthephotographsoftheCSPbB门QDsolutionunderafluorescentlampandUVlamp(excitationwavelengthof365nm),respectively.AbrightgreenemissionoftheCSPbBr3QDsolutionespeciallyundertheUVirradiationwasobserved.TheseresultsindicatedthatCsPbBr3QDsarebenefittingforfabricatingthehighcolorpuritymonochromaticLEDs.FigureIbpresentstheXRDpatternofCsPbBrjQDpowder(JCPDSNo.PDF#75-412).The15.2°,21.5°,30.6°,34.4°,37.7°,43.8°,46.7°correspondto(100),(110),(200),(210),(211),(220),and(300)crystalplane,wellconsistingwiththecubiccrystalstructureintheliterature1131.TheTEMandHRTEMimagesofCSPbB门QDsareshowninFig.1(c)and1(d),respectively,fromwhichtheCsPbBr?QDsaremonodisperseandhaveacubestructurewithanaveragesizeof9nm.ThelatticespacingofCsPbBrjQDsis0.58nm,correspondingto(100)crystalplaneofcubiccrystalstructure,thusfurtherillustratingtheCsPbBr3QDsweresuccessfullysynthesized.Fig.l(a)UV-VisabsorptionandPLspectraofCsPbBr?QDsunderexcitationwavelengthof365nm,withinsetsshowingthephotographofQDsolutionsunderambientlight(left)andUVlight(right).(b)XRDpatternsofCsPbBr?QDspowder.(c)TEMimageOfCsPbBr3QDs.(d)HRTEMimageofCsPbBnQDs.ThefabricatedprocessesofflexiblephotopolymersubstrateareshowninFig.2(a).ThephotopolymerNOA63wasspin-coatedonSiwaferandcuredunderultravioletozonetoformafilm,andthenthefilmwaspeeledofffromSiwafer.InordertoachievethebalancedchargeinjectionandefficienttransportinLEDs,theinverteddevicearchitectureofAgZnOPEICsPbBr3QDsCBPTCTAMoO3Auwasdesigned,asshowninFig.2(b).Correspondingenergy-leveldiagramofeachlayerwithintheflexibledeviceisshowninFig.2(c),andalltheenergylevelsofthesematerialsusedinPe-LEDswereobtainedfromthepublishedstudies171.TheAgandZnOwereusedascathodeandETL,respectively.Herein,weutilizedtheAgascathodemainlybecausethatitisbeneficialforelectroninjectionduetothesmallenergybarrierbetweenAgcathodeandZnO,whichisdifferentfromtheconventionalreportsintheLEDwithinverteddevicestructurethatITOnormallyisusedascathode.ThePEIasinterfacelayernotonlycanmodifytheenergylevelofZnObutalsocanpassivateCSPbBr3films.Simultaneously,theZnO/PEIlayercanalsobeusedasholeblockIayer(HBL),becausethelargeenergybarrierbetweenthevalencebandmaximum(VBM)ofCsPbBnandthehighestoccupiedmolecularOrbital(HOMO)ofZnO/PEIlayercanblockthetransportofholesfromtheoppositedirection.TheCBPandTCTAasholetransportlayer(HTL)canformagradientlevelduetoproperHOMOlevelbetweenCBPandTCTA,whichcanfacilitateholestransportfromanodetoCBPlayerandinjectintoemissionlayer.Inaddition,theyalsowereusedaselectronblockIayer(EBL)toconfineelectronsintheCSPbBr3emissivelayerduetothehighlowestunoccupiedmolecularOrbital(LUMO)level.Whenelectronsfromcathodeandholesfromanoderecombineintheperovskiteemissionlayer,resultinginELemissionoftheflexiblePe-LED.2 3 4 5 6 H>)Ap8一!山Mo03AuTCTACBPPerovskiteZnO/PEIAgFg.2(a)Processoffabricatingaflexiblephotopolymersubstratebytemplate-strippingtechnique.(b)DevcestructureoftheCsPbBr?Pe-LED.(C)CorrespondingenergybanddiagramofthePe-LEDstructure.InordertoanalysistheperformancesofflexibleLEDs,currentdensity-voltage-luminance(7-V-L)characteristicswereperformedandshowninFig.3(a).Thedeviceturn-onvoltage(generallydefinedasthedrivingvoltageatwhichtheluminescenceof1cdm2isobtained)isaround2.6VnearthebandgapoftheCsPbBnQDs,whichillustratesthatanefficientandbarrier-freechargeinjectionintotheemissivelayersisaccomplished.Peakluminanceof10325cdm2isachievedundertheappliedvoltageof11V.Fig.3(b)showsthecurrentefficiency-currentdensity-externalquantumefficiency(CE-EQE)characteristicsoftheas-preparedflexiblePe-LEDs,whichdemonstrateamaximumCEof3.4cdA1andpeakEQEof1.25%atacurrentdensityof158mAcm'2.Moreover,theCEandEQEvaluesdisplaylittleroll-off,indicatingabalancedandefficientchargeinjectionintheas-prepareddevice.ThePLspectrumofCsPbBrjQDfilmsandELspectrumofthecorrespondingLEDdevicearegiveninFigure3c.Bothemissivepeaksarelocatedat513nm,andwithoutanyadditionalpeakfromthechargetransportmaterialsintheELspectrum,suggestingthatCsPbBr?QDsastheprimaryexcitonrecombinationcentersresultingfromthebalancedchargerecombinationduringthedeviceoperation.However,theELspectrumhasaslightbroadeningcomparedwiththePLspectrum,whichisattributedtotheenergytransferfromsmallertolargeQDsintheemissivelayersorthedielectricfunctionofthesurroundingmedium'".Thesymmetricemissionfromtheflexibledevice,correspondingtoCommissionInternationaldeEclairage(CIE)colorcoordinatesof(0.08,0.73)asshowninFig.3(d),whichrevealsthecolor-saturatedgreenemissionandhopefulapplicationprospectinthedisplay.68Voltage(V)OoOo42G.E3VUJ)A=SUaPcotn。(-<PsAoUaQypw4>hnoLUm三'ance(cdm.2)S0.e)3防UQc-Wavelength(nm)CIExA山QFg.3(a)CurrentdensityandluminancevsdvingvoltageofexblePe-LEDs.(b)ExiemalquantumefficiencyandcurrentefficiencyvscurrentdensityofflexiblePe-LEDs.(c)PLspectrumofCsPbBnQDfilms,andELspectrumofthePe-LEDs.(Cl)CorrespondingCIEcoordinatesfortheELspectrum.ThephotographsofthecurveddevicebeforeandafterlightingareshowninFig.4(a)and(b),respectively.Itisobservedthattherearenocracksordarkspotswhilethedevicewasoperating.InordertofurtherinvestigatethemechanicalrobustnessoftheflexiblePe-LEDs,wemeasuredtheJ-VandELcharacteristicsofthisdeviceafterrepeatedstretch-release100cycleswithabendingangleofabout180degrees.AsshowninFig.4(c)andd,theJ-VcurvesandELspectrahavenoobviousdeteriorationafterrepeatedbendingupto100cycles.TheseresultsillustratethattheflexiblePe-LEDsbasedonphotopolymersubstrateandAgcathodeownhighflexibility.Voltage(V)0.0440480520560600Wavelength(m)Fig.4Photographsof(heflexiblePe-LEDsbeforelighting(a),andoperateda(5V(b).(C)ComparisonofJ-Vcharacteristics.(d)ELspectrabeforeandafterrepeatedbending.4ConclusionInthiswork,wereportedaPe-LEDbasedonthegreenlightemittingCSPbBi3QDsthatactastheemissivelayers.ThePe-LEDmanifestahighlyflexibleperformancesbenefitingfromtheutilizationofaflexiblephotopolymersubstrate,whichcanavoidthecorrosionfromanorganicsolventinthesubsequentPe-LEDfabricationprocess.Furthermore,weusedAgasacathodetoensuretheconductivityandmechanicalductilityofflexibleelectrode,andmoreovertheAgcathodecanenhanceelectronsinjectionefficiency.Therefore,theflexiblePe-LEDsexhibitasaturatedcolorpuritywithgreenemission,lowturnonvoltageof2.6Vandhighbrightnessof10325cdm2.Inaddition,theblendingtestillustratesthatflexiblePe-LEDshaveexcellentflexibilityandhighmechanicalrobustness.ResponseLetterisavailableforthispaperat:http:CjLliHhlPubliS1.20220*(20220*为文章稿另).1 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