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1、LETTERdoi:10.1038/nature10569Twotypesofluminescenceblinkingrevealedbyspectroelectrochemistryofsinglequantumdots1,233131,2ChristopheGalland,YagnaseniGhosh,AndreaSteinbru¨ck,MilanSykora,JenniferA.Hollingsworth,VictorI.Klimov1,2,3&HanHtoonPhotoluminescenceblinking—randomswitchingbetweenstatesofdis
2、tribution(FLID)representation.Inthisrepresentation,theprob-high(ON)andlow(OFF)emissivities—isauniversalpropertyofabilityofoccupyingagivenstateinthetwo-dimensionallifetime–123molecularemittersfoundindyes,polymers,biologicalmoleculesintensityspaceisshownbyfalsecolour,whichchangesfrombluetoandarti
3、ficialnanostructuressuchasnanocrystalquantumdots,redastheprobabilityincreases.AsillustratedintheinsetsofFigs1c,d,4–6theuseofFLIDsallowsreadyidentificationofdifferenttypesofchargecarbonnanotubesandnanowires.Forthepast15years,colloidalnanocrystalshavebeenusedasamodelsystemtostudythisphe-stateaswe
4、llasdifferenttypesofblinkingbehaviour(forexample5,6binaryblinkingversusflickering).nomenon.TheoccurrenceofOFFperiodsinnanocrystalemis-sionhasbeencommonlyattributedtothepresenceofanadditionalInourwork,toverifythevalidityofthechargingmodelofphoto-7charge,whichleadstophotoluminescencequenchingbyno
5、n-luminescenceintermittency,wecombinesingle-nanocrystalspectro-8scopywithanelectrochemicalapproachforcontrollingtheextentofradiativerecombination(theAugermechanism).However,this9,1015–17‘charging’modelwasrecentlychallengedinseveralreports.nanocrystalcharging.Specifically,weconductsingle-nanocry
6、stal,Herewereporttime-resolvedphotoluminescencestudiesoftime-tagged,time-resolved,single-photoncountingstudiesofsamplesindividualnanocrystalquantumdotsperformedwhileelectro-incorporatedintoathree-electrodeelectrochemicalcell(Fig.2a).Wechemicallycontrollingthedegreeoftheircharging,withthegoalinv
7、estigatecore–shellCdSe/CdSnanocrystalssynthesizedaccordingtoofclarifyingtheroleofcharginginblinking.Wefindthattworef.18.Inthecaseofexceptionallythick,16–19-monolayershells,they18distincttypesofblinkingarepossible:conventional(A-ty
