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1、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,CollegeofElectroni
2、cScienceandEngineering,JilinUniversity,Changchun130012,China）*CorrespondingAuthor,E-mail:baix血.edM.cnAbstract:Flexibleinformationdisplayshavethepromisingpotentialforthefutureoptoelectronicapplication.However,achievingthehighlyefficientandstableflexiblelight-emittingdiodes（LEDs）isstillabigchallengedu
3、etothelimitedchoicesofelectrodematerialsandflexiblesubstrates.Herein,theflexibleperovskitelight-emitting（Iiodes（Pe-LEDs）bycombiningtheflexiblesubstratebasedonaphotopolymerwiththeCsPbBr?quantumdots（QDs）emittinglayerwerefabricated.Inordertoimproveelectronsinjectionandtransport,Agwasusedasthecathode.As
4、aresult,thegreenlightemittingPe-LEDswithhighluminanceof10325cd,m-2andhighcolorpuritywiththefull-width-at-half-maximum（FWHM）of19nmwereobtained.Inaddition,thePe-LEDsexhibitgoodflexibilityandmechanicalductility,andtheas-preparedflexibledevicestillmaintainsitsoptoelectronicperformanceevenafterrepeatedbe
5、nding100timesunderabendingangleofabout180o.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
6、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
7、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,especiallyfortheflexibl
8、eoptoelectronicdevices1(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)quantumdot
9、s(QDs)exhibitanenhancedstability,andmeanwhiletheyalsodemonstratearemarkableopticalandoptoelectronicperformanceincludingtheexcellentphotoluminescencequantumyield(PLQY)levelsreaching90%,highcolorpurity,widecolorgamut,andhighcharge-carriermobility.Therefore,theyhavethehugepotentialasanidealemissivelaye
10、rmaterialstofabricatehighlyefficientperovskitelight-emittingdiodes(Pe-LEDs)5.191Fordisplayapplications,flexible,curveddisplaysarekeyelementsinfutureoptoelectronicdevices1.However,therearestillchallengesinthefabricationofflexiblePe-LEDsowningtothesophisticatedfabricatedsteps,includingthesolution-proc
11、essedspin-coatingwithvariouschemicals,high-temperatureannealingandvacuumevaporation.Thesemultipleproceduresconsiderablylimitthedevicearchitecturedesignsaswellasthechoicesofappropriateflexiblesubstratesandelectrodes.Thesoftplasticsubstrateisgenerallyaproperalternativeforflexiblesubstrateduetoitslowco
12、standhighflexibility.However,theycanbeeasilycorrodedbysomeacidicreagentandorganicsolvents(toluene,chloroform)duringthefabricationofLEDs.Fortheelectrodes,althoughtheIndium-TinOxide(ITO)hasbeenwidelyusedintheLEDs,itisn,tsuitableforflexibleLEDsduetoitspoormechanicalrobustnessj.Therefore,toachievehigh-p
13、erfbrmanceflexiblePe-LEDs,weneedtochooseasuitableelectrodeandsubstratematerial.Here,wefabricatedaflexiblePe-LEDbasedonallinorganicCsPbBr?perovskiteQDsemissivelayers,inwhichtheperovskiteQDsexhibitanefficientgreenlightemissionwiththePLQYof75%.PhotopolymerNOA63wasusedasaflexiblesubstratebyspin-coatingi
14、tontheSisubstrateandbeingstrippedfromtheSi.Simultaneously,AgfilmwasusedasacathodebysimplethermalevaporationComparedwiththeITOelectrode,theAghashigherconductivityandbettermechanicalductility.Inaddition,Agascathodereducedenergybarrierbetweenthecathodeandelectrontransportlayer(ETL),whichismoreconducive
15、toelectroninjection.Consequently,theas-preparedgreenlightemittingPe-LEDsexhibitgoodflexibility,highbrightnessof10325cdm2,highcolorpuritywiththefull-width-at-half-maximum(FWHM)of19nmandlowthresholdvoltageabout2.6V.ThedeviceperformancestillmaintainedwhentheflexiblePe-LEDswererepeatedlybent100times.The
16、seresultsillustratethattheflexiblePe-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
17、SynthesisofCsPbBr3QDsTheCsPbBr3perovskiteQDsweresynthesizedonthebaseofthepreviouslyreportedmethod.CesiumOleate(Cs-OA)waspreparedbymixingCs2CO3(O.8i4g),OA(2.5mL),andODE(30.0mL)ina100mLthree-neckedflask,whichwasdegassedanddriedundervacuumfor1hat120,thenheatedto150CunderN2untilaclearsolutionwasobtained
18、.ForthesynthesisofCsPbBr3QDs,10.0mLODE,0.138gPbBr2,1.0mLOAand1.0mLOLAwereloadedintoa50mLthree-neckedflask,degassedanddriedbyapplyingvacuumfor1hat120;afterthesolutionbecameclear,thetemperaturewasraisedto180and1mLofcesiumoleatesolutionwasquicklyinjected.5secondslater,thereactionmixturewascooleddowntor
19、oomtemperatureinanice-waterbath.Thereactionmixtureneedstobecentrifugedfor10minat5000rmin,andtheobtainedprecipitatewasredispersedin5.0mLofhexane,centrifugeddownagainfor10minat10000rmin,andprecipitatewasredispersedin1.0mLofhexane.2.3 DeviceFabricationFirstly,photopolymer(NOA63,Norland)wasspin-coatedon
20、toacleanedsiliconwaferataspeedof1500r/minfor40sandexposedtoanultravioletlampfor3min.Then,theAgelectrodewasgrownonthephotopolymerfilmviathermalevaporation.Subsequently,ZnOnanocrystals(NCs)solutionwasspin-coatedoniotheAgelectrodeataspeedofI000r/minfor40s,andannealedonthehotplateat150for10min,afterdown
21、toroomtemperature.Then,thesubstratewastransferredintoaglovebox.Asolutionofpolyethylenimine(PEI)(dissolvein2-methoxyethanolinamassfractionsof0.2%)wasspin-coatedontotheZnOfilmat3O(X)rpmfor40Sandannealedat125for10min.CSPbB门QDSwerespin-coatedataspeedof1000rpmfor40s.Next,4,4,-Bis(carbazole-9-yl)biphenyl(
22、CBP),4.4,4-IriS(carbazol-9-yl)-triphenylamine(TCTA),MOO3,andAuweresequentiallydepositedusingathermalevaporationunderabasepressureof7104Pa.Atlast,theflexibleLEDswasstrippedfromthesilicontemplate.2.4 CharacterizationsAbsorptionspectraweremeasuredusingaShimadzuLJV-2550spectrophotometer.ThePLspectrawere
23、measuredusinganOceanOptics.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-luminanceofLEDwasmeasure
24、dbyAKeithley2612Bsourcemeasureunit.TheLEDbrightnesswasdeterminedusingaPhotoResearchSpectraScanspectrometerPR650.Theelectroluminescence(EL)spectrawererecordedwithaMayaspectrometer(OceanOptics)coupledtoanopticalfiber.3 ResultsandDiscussionTheUV-visibleabsorptionandPLemissionspectraofCsPbBr?perovskiteQ
25、DsareshowninFig.1(a).ThefirstexcitonabsorptionpeakandPLemissionpeakarelocatedat500nmand513nm,respectively.TheCSPbB门perovskiteQDsexhibitasmallstokesdisplacementandanarrowFWHMabout18nm.TheinsetinFig.1(a)showsthephotographsoftheCSPbB门QDsolutionunderafluorescentlampandUVlamp(excitationwavelengthof365nm)
26、,respectively.AbrightgreenemissionoftheCSPbBr3QDsolutionespeciallyundertheUVirradiationwasobserved.TheseresultsindicatedthatCsPbBr3QDsarebenefittingforfabricatingthehighcolorpuritymonochromaticLEDs.FigureIbpresentstheXRDpatternofCsPbBrjQDpowder(JCPDSNo.PDF#75-412).The15.2,21.5,30.6,34.4,37.7,43.8,46
27、.7correspondto(100),(110),(200),(210),(211),(220),and(300)crystalplane,wellconsistingwiththecubiccrystalstructureintheliterature1131.TheTEMandHRTEMimagesofCSPbB门QDsareshowninFig.1(c)and1(d),respectively,fromwhichtheCsPbBr?QDsaremonodisperseandhaveacubestructurewithanaveragesizeof9nm.Thelatticespacin
28、gofCsPbBrjQDsis0.58nm,correspondingto(100)crystalplaneofcubiccrystalstructure,thusfurtherillustratingtheCsPbBr3QDsweresuccessfullysynthesized.Fig.l(a)UV-VisabsorptionandPLspectraofCsPbBr?QDsunderexcitationwavelengthof365nm,withinsetsshowingthephotographofQDsolutionsunderambientlight(left)andUVlight(
29、right).(b)XRDpatternsofCsPbBr?QDspowder.(c)TEMimageOfCsPbBr3QDs.(d)HRTEMimageofCsPbBnQDs.ThefabricatedprocessesofflexiblephotopolymersubstrateareshowninFig.2(a).ThephotopolymerNOA63wasspin-coatedonSiwaferandcuredunderultravioletozonetoformafilm,andthenthefilmwaspeeledofffromSiwafer.Inordertoachievet
30、hebalancedchargeinjectionandefficienttransportinLEDs,theinverteddevicearchitectureofAgZnOPEICsPbBr3QDsCBPTCTAMoO3Auwasdesigned,asshowninFig.2(b).Correspondingenergy-leveldiagramofeachlayerwithintheflexibledeviceisshowninFig.2(c),andalltheenergylevelsofthesematerialsusedinPe-LEDswereobtainedfromthepu
31、blishedstudies171.TheAgandZnOwereusedascathodeandETL,respectively.Herein,weutilizedtheAgascathodemainlybecausethatitisbeneficialforelectroninjectionduetothesmallenergybarrierbetweenAgcathodeandZnO,whichisdifferentfromtheconventionalreportsintheLEDwithinverteddevicestructurethatITOnormallyisusedascat
32、hode.ThePEIasinterfacelayernotonlycanmodifytheenergylevelofZnObutalsocanpassivateCSPbBr3films.Simultaneously,theZnO/PEIlayercanalsobeusedasholeblockIayer(HBL),becausethelargeenergybarrierbetweenthevalencebandmaximum(VBM)ofCsPbBnandthehighestoccupiedmolecularOrbital(HOMO)ofZnO/PEIlayercanblockthetran
33、sportofholesfromtheoppositedirection.TheCBPandTCTAasholetransportlayer(HTL)canformagradientlevelduetoproperHOMOlevelbetweenCBPandTCTA,whichcanfacilitateholestransportfromanodetoCBPlayerandinjectintoemissionlayer.Inaddition,theyalsowereusedaselectronblockIayer(EBL)toconfineelectronsintheCSPbBr3emissi
34、velayerduetothehighlowestunoccupiedmolecularOrbital(LUMO)level.Whenelectronsfromcathodeandholesfromanoderecombineintheperovskiteemissionlayer,resultinginELemissionoftheflexiblePe-LED.2 3 4 5 6 H)Ap8一!山Mo03AuTCTACBPPerovskiteZnO/PEIAgFg.2(a)Processoffabricatingaflexiblephotopolymersubstratebytemplate
35、-strippingtechnique.(b)DevcestructureoftheCsPbBr?Pe-LED.(C)CorrespondingenergybanddiagramofthePe-LEDstructure.InordertoanalysistheperformancesofflexibleLEDs,currentdensity-voltage-luminance(7-V-L)characteristicswereperformedandshowninFig.3(a).Thedeviceturn-onvoltage(generallydefinedasthedrivingvolta
36、geatwhichtheluminescenceof1cdm2isobtained)isaround2.6VnearthebandgapoftheCsPbBnQDs,whichillustratesthatanefficientandbarrier-freechargeinjectionintotheemissivelayersisaccomplished.Peakluminanceof10325cdm2isachievedundertheappliedvoltageof11V.Fig.3(b)showsthecurrentefficiency-currentdensity-externalq
37、uantumefficiency(CE-EQE)characteristicsoftheas-preparedflexiblePe-LEDs,whichdemonstrateamaximumCEof3.4cdA1andpeakEQEof1.25%atacurrentdensityof158mAcm2.Moreover,theCEandEQEvaluesdisplaylittleroll-off,indicatingabalancedandefficientchargeinjectionintheas-prepareddevice.ThePLspectrumofCsPbBrjQDfilmsand
38、ELspectrumofthecorrespondingLEDdevicearegiveninFigure3c.Bothemissivepeaksarelocatedat513nm,andwithoutanyadditionalpeakfromthechargetransportmaterialsintheELspectrum,suggestingthatCsPbBr?QDsastheprimaryexcitonrecombinationcentersresultingfromthebalancedchargerecombinationduringthedeviceoperation.Howe
39、ver,theELspectrumhasaslightbroadeningcomparedwiththePLspectrum,whichisattributedtotheenergytransferfromsmallertolargeQDsintheemissivelayersorthedielectricfunctionofthesurroundingmedium.Thesymmetricemissionfromtheflexibledevice,correspondingtoCommissionInternationaldeEclairage(CIE)colorcoordinatesof(
40、0.08,0.73)asshowninFig.3(d),whichrevealsthecolor-saturatedgreenemissionandhopefulapplicationprospectinthedisplay.68Voltage(V)OoOo42G.E3VUJ)A=SUaPcotn。(-hnoLUm三ance(cdm.2)S0.e)3防UQc-Wavelength(nm)CIExA山QFg.3(a)CurrentdensityandluminancevsdvingvoltageofexblePe-LEDs.(b)Exiemalquantumefficiencyandcurren
41、tefficiencyvscurrentdensityofflexiblePe-LEDs.(c)PLspectrumofCsPbBnQDfilms,andELspectrumofthePe-LEDs.(Cl)CorrespondingCIEcoordinatesfortheELspectrum.ThephotographsofthecurveddevicebeforeandafterlightingareshowninFig.4(a)and(b),respectively.Itisobservedthattherearenocracksordarkspotswhilethedevicewaso
42、perating.InordertofurtherinvestigatethemechanicalrobustnessoftheflexiblePe-LEDs,wemeasuredtheJ-VandELcharacteristicsofthisdeviceafterrepeatedstretch-release100cycleswithabendingangleofabout180degrees.AsshowninFig.4(c)andd,theJ-VcurvesandELspectrahavenoobviousdeteriorationafterrepeatedbendingupto100c
43、ycles.TheseresultsillustratethattheflexiblePe-LEDsbasedonphotopolymersubstrateandAgcathodeownhighflexibility.Voltage(V)0.0440480520560600Wavelength(m)Fig.4Photographsof(heflexiblePe-LEDsbeforelighting(a),andoperateda(5V(b).(C)ComparisonofJ-Vcharacteristics.(d)ELspectrabeforeandafterrepeatedbending.4
44、ConclusionInthiswork,wereportedaPe-LEDbasedonthegreenlightemittingCSPbBi3QDsthatactastheemissivelayers.ThePe-LEDmanifestahighlyflexibleperformancesbenefitingfromtheutilizationofaflexiblephotopolymersubstrate,whichcanavoidthecorrosionfromanorganicsolventinthesubsequentPe-LEDfabricationprocess.Further
45、more,weusedAgasacathodetoensuretheconductivityandmechanicalductilityofflexibleelectrode,andmoreovertheAgcathodecanenhanceelectronsinjectionefficiency.Therefore,theflexiblePe-LEDsexhibitasaturatedcolorpuritywithgreenemission,lowturnonvoltageof2.6Vandhighbrightnessof10325cdm2.Inaddition,theblendingtes
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