Extended Data for Dynamics of Intermittent Delayed Emission in Single CdSe CdS Quantum Dots - Hinterding et al. - Unknown - Unknown

《Extended Data for Dynamics of Intermittent Delayed Emission in Single CdSe CdS Quantum Dots - Hinterding et al. - Unknown - Unknown》由会员上传分享，免费在线阅读，更多相关内容在学术论文-天天文库。

ExtendedDataforDynamicsofIntermittentDelayedEmissioninSingleCdSe/CdSQuantumDotsStijnO.M.Hinterding1;2,SanderJ.W.Vonk1;2,EllekeJ.vanHarten1,FreddyT.Rabouw1;2;1SoftCondensedMatterand2InorganicChemistryandCatalysis,DebyeInstituteforNanomaterialsScience,UtrechtUniversity,P.O.Box80000,3508TAUtrecht,TheNetherlandsCorrespondingauthor.E-mail:f.t.rabouw@uu.nlE1

1FigureE1–E10—Resultsofdouble-APDexperimentsformorequantumdots.Belowweprovideanoverviewofresultsfromthedouble-APD(inHanburyBrown-Twissconfiguration)experiments.Aftereachoftheseexperiments,thesameindividualquantumdotswerestudiedbyasingleAPDandaspectrometersimultaneously(asdescribedinthemaintext).Fortheseresults,seeFigureE11–20.Thearrangementofeachofthesefiguresisasfollows:(A)Totalphotoluminescence(PL)intensity(Itot)asafunctionoftime.(B)DistributionofPLintensityvalues.Thereddottedline(atION)in(A,B)indicatesthethresholdusedtodistinguishtheONstate.(C)DelayedPLintensity(Idel),definedasthenumberofphotonsdetected200nsafteralaserpulse.(D)DistributionofIdel.(E)Fluorescence-lifetime-intensitydistribution,obtainedfromthePLintensityandaveragephotondelaytimeforeachindividual10msperiodintheexperiment.(F)Normalizedsecond-ordercorrelationfunction.Lightbluelineisexperimentaldata,darkbluelineisafittoabi-exponentialmodel.Thesmallareaofthezero-delaypeak,relativetotheside-peaks,indicatesasingleQDwasstudied.(G)Background-subtractedPLdecaycurvescorrespondingtothe(green)ONand(red)GRAYstates.Symbolsaredatapoints,solidlinesarefitstoabi-exponentialdecayfunction.TimeperiodswerecategorizedasGRAYwhentheintensitywasintherangeIGRAY.(H)Thesamedataasin(G),nowdisplayedondouble-logarithmicaxes.(I)2-dimensionalhistogramofthecorrelationbetweenIdelandItot,constructedfromthetotaldouble-APDexperiment,binnedat10ms.(J)2-dimensionalhistogramofthecorrelationbetweenIdelandthefollowingchangeinItot,i.e.offIdel;i;Itot;i+1Itot;ig.(K)SameasJ,butnowcorrelatingIdelandthepreceedingchangeinItot,i.e.,histogrammingfIdel;i;Itot;iItot;i1g.(L)DistributionsofIdel,correspondingto(blue)all10-mstimebinsduringwhichtheQDisON(ItotION),(red)binsdirectlyprecedinganON!GRAYswitch(i.e.,selectingallbinsiforwhichItot;i+1Itot;i70cts/10ms),and(green)binsdirectlyfollowingaGRAY!ONswitch(i.e.,Itot;iItot;i170cts/10ms).Here,ION,andIGRAYaretheON-statethresholdandGRAY-stateintensity-range,respectively.Thevaluesoftheseparameters,aswellastheestimatednumberofphotonsabsorbedperlaserpulse,p(determinedfromthelaserpowerusedintheexperiment,seeSectionS5),areprovidedinthefollowingtable:TableE1—Overviewofanalysisandacquisitionparametersofdouble-APDexperimentsQDnumberI(cts/10ms)I(cts/10ms)pONGRAY1100[25;60]0:32130[35;60]0:33110[15;50]0:34110[25;55]0:35230[15;40]16230[50;100]17230[70;120]18220[50;85]19210[40;85]110300[60;120]1E2

2(A)(B)250I=136.9±0.2200ON150100(cts/10ms)ItotI=42.1±1.250GRAY00100200(C)(D)403020(cts/10ms)Idel100100120140160180200010002000Time(s)Occurrence(E)(F)(G)(H)00250301010A/A=0.11A=0.32100centersideON−1200−1AGRAY=0.531010−2752010150(τ)−2−3(2)101010050g(cts/10ms)−4Occurrence10−310Itot251050τ=40.7ns−5ON10PLintensity(cts/ps/s)τ=4.7nsPLintensity(cts/ps/s)−4GRAY−60001010050100150−100001000050100100101102103®τ(ns)Lagtimeτ(ns)Delaytime(ns)Delaytime(ns)(I)(J)(K)(L)4040QDON2221010100.4BeforeturnOFF3030AfterturnON20201110.210(cts/10ms)1010(cts/10ms)iOccurrenceOccurrenceOccurrenceIdel10Idel,10Occurrence(norm.)0000.0010010100100200−1000100−100010002040I(cts/10ms)ΔI(cts/10ms)ΔI(cts/10ms)I(cts/10ms)toti+1idelFigureE1—Overviewofphotoluminescencepropertiesofquantumdot1(samequantumdotasdiscussedinmaintext).E3

3(A)(B)250I=171.6±0.4ON200150100(cts/10ms)ItotI=45.8±2.350GRAY00100200(C)(D)6040(cts/10ms)20Idel010012014016018020005001000Time(s)Occurrence(E)(F)(G)(H)002501002010A=0.3110Acenter/Aside=0.13ONA=0.56−1200−1GRAY10751510−210150(τ)−2−350(2)101010100g(cts/10ms)−4Occurrence−310Itot2551050τ=53.8ns−5ON10PLintensity(cts/ps/s)τ=1.7nsPLintensity(cts/ps/s)−4GRAY−60001010050100150−100001000050100100101102103®τ(ns)Lagtimeτ(ns)Delaytime(ns)Delaytime(ns)(I)(J)(K)(L)6060222101010QDONBeforeturnOFF0.2AfterturnON4040111101010(cts/10ms)0.1(cts/10ms)20Occurrencei20OccurrenceOccurrenceIdelIdel,Occurrence(norm.)0000.0010010100100200−1000100−10001000204060I(cts/10ms)ΔI(cts/10ms)ΔI(cts/10ms)I(cts/10ms)toti+1idelFigureE2—Overviewofphotoluminescencepropertiesofquantumdot2.E4

4(A)(B)250I=148.7±0.3ON200150100(cts/10ms)ItotI=33.3±0.550GRAY00100200(C)(D)403020(cts/10ms)Idel100100120140160180200010002000Time(s)Occurrence(E)(F)(G)(H)00250201010A/A=0.08A=0.35centersideON−1200100−1AGRAY=0.60101510−210150(τ)−2τON=40.2ns−3(2)1010τ=4.4ns1010050gGRAY(cts/10ms)−4Occurrence−310Itot51050−510PLintensity(cts/ps/s)PLintensity(cts/ps/s)−4−60001010050100150−100001000050100100101102103®τ(ns)Lagtimeτ(ns)Delaytime(ns)Delaytime(ns)(I)(J)(K)(L)404022QDON21010100.4BeforeturnOFF3030AfterturnON201201110(cts/10ms)10100.2(cts/10ms)iOccurrenceOccurrenceOccurrenceIdel10Idel,10Occurrence(norm.)0000.0010010100100200−1000100−100010002040I(cts/10ms)ΔI(cts/10ms)ΔI(cts/10ms)I(cts/10ms)toti+1idelFigureE3—Overviewofphotoluminescencepropertiesofquantumdot3.E5

5(A)(B)250I=138.9±0.6ON200150100(cts/10ms)ItotI=40.9±1.850GRAY00200400(C)(D)6040(cts/10ms)20Idel0100120140160180200010002000Time(s)Occurrence(E)(F)(G)(H)00250201010A/A=0.08A=0.32centersideON−1200100−1AGRAY=0.51101510−210150(τ)−2−3(2)10101010050g−4(cts/10ms)10Occurrence−3Itot51050τ=40.4ns−5ON10PLintensity(cts/ps/s)τ=5.3nsPLintensity(cts/ps/s)−4GRAY−60001010050100150−100001000050100100101102103®τ(ns)Lagtimeτ(ns)Delaytime(ns)Delaytime(ns)(I)(J)(K)(L)6060220.4QDON2101010BeforeturnOFFAfterturnON40400.31110.2101010(cts/10ms)20(cts/10ms)i20delOccurrenceOccurrenceOccurrence0.1IIdel,Occurrence(norm.)0000.0010010100100200−1000100−10001000204060I(cts/10ms)ΔI(cts/10ms)ΔI(cts/10ms)I(cts/10ms)toti+1idelFigureE4—Overviewofphotoluminescencepropertiesofquantumdot4.E6

6(A)(B)250I=164.2±0.7ON200150100(cts/10ms)ItotI=33.8±1.450GRAY00100(C)(D)403020(cts/10ms)Idel100100120140160180200010002000Time(s)Occurrence(E)(F)(G)(H)00250201010A/A=0.07A=0.4880centersideON−1200−1AGRAY=0.83101510−26010150(τ)−2τ=33.4ns−3(2)1010ON1010040gτGRAY=4.4ns(cts/10ms)−4Occurrence−310Itot5105020−510PLintensity(cts/ps/s)PLintensity(cts/ps/s)−4−60001010050100150−100001000050100100101102103®τ(ns)Lagtimeτ(ns)Delaytime(ns)Delaytime(ns)(I)(J)(K)(L)4040222QDON1010100.4BeforeturnOFF3030AfterturnON20120111010100.2(cts/10ms)(cts/10ms)iOccurrenceOccurrenceOccurrenceIdel10Idel,10Occurrence(norm.)0000.0010010100100200−1000100−100010002040I(cts/10ms)ΔI(cts/10ms)ΔI(cts/10ms)I(cts/10ms)toti+1idelFigureE5—Overviewofphotoluminescencepropertiesofquantumdot5.E7

7(A)(B)400I=274.1±3.3ON300200(cts/10ms)Itot100I=72.2±11.4GRAY0050100(C)(D)806040(cts/10ms)Idel20002040608010001000Time(s)Occurrence(E)(F)(G)(H)00400301010A/A=0.12A=0.62centersideON−1−1103001040−220A=0.8410GRAY(τ)−2−3200(2)1010g(cts/10ms)2010−4Occurrence−310Itot10010τ=39.8ns−5ON10PLintensity(cts/ps/s)τ=11.9nsPLintensity(cts/ps/s)−4GRAY−60001010050100150−100001000050100100101102103®τ(ns)Lagtimeτ(ns)Delaytime(ns)Delaytime(ns)(I)(J)(K)(L)8080QDONBeforeturnOFF60260110.10AfterturnON10101040401(cts/10ms)0.05(cts/10ms)10iOccurrenceOccurrenceOccurrenceIdel20Idel,20Occurrence(norm.)0000.00010010100100200300400−20000200050I(cts/10ms)ΔI(cts/10ms)ΔI(cts/10ms)I(cts/10ms)toti+1idelFigureE6—Overviewofphotoluminescencepropertiesofquantumdot6.E8

8(A)(B)400I=270.9±0.2ON300200(cts/10ms)Itot100I=89.9±0.9GRAY00100200(C)(D)403020(cts/10ms)Idel100020406080100010002000Time(s)Occurrence(E)(F)(G)(H)00400301010A/A=0.14A=0.91centersideON−1−11030010010−22010(τ)−2AGRAY=1.33−3200(2)101050g−4(cts/10ms)1010Occurrence−3Itot10010τ=28.7ns−5ON10PLintensity(cts/ps/s)τ=6.2nsPLintensity(cts/ps/s)−4GRAY−60001010050100150−100001000050100100101102103®τ(ns)Lagtimeτ(ns)Delaytime(ns)Delaytime(ns)(I)(J)(K)(L)40402221010QDON100.4BeforeturnOFF3030AfterturnON0.320120111010100.2(cts/10ms)(cts/10ms)iOccurrenceOccurrenceOccurrenceIdel10Idel,100.1Occurrence(norm.)0000.0010010100100200300400−2000020002040I(cts/10ms)ΔI(cts/10ms)ΔI(cts/10ms)I(cts/10ms)toti+1idelFigureE7—Overviewofphotoluminescencepropertiesofquantumdot7.E9

9(A)(B)300200I=252.3±0.6ON(cts/10ms)100ItotI=65.8±2.4GRAY00100200(C)(D)3020(cts/10ms)10Idel0160180200220240010002000Time(s)Occurrence(E)(F)(G)(H)00300301010A/A=0.09A=0.88centersideON−130010−110−22002010200(τ)−2A=1.21−3(2)10GRAY10g(cts/10ms)−4100100Occurrence10−310Itot10τ=27.3ns−5ON10PLintensity(cts/ps/s)τ=8.7nsPLintensity(cts/ps/s)−4GRAY−60001010050100150−100001000050100100101102103®τ(ns)Lagtimeτ(ns)Delaytime(ns)Delaytime(ns)(I)(J)(K)(L)2303010QDON0.4BeforeturnOFF2AfterturnON2010200.31110100.21(cts/10ms)(cts/10ms)1010Occurrencei10OccurrenceOccurrenceIdelIdel,0.1Occurrence(norm.)0000.0010010100100200300−200002000102030I(cts/10ms)ΔI(cts/10ms)ΔI(cts/10ms)I(cts/10ms)toti+1idelFigureE8—Overviewofphotoluminescencepropertiesofquantumdot8.E10

10(A)(B)400I=251.0±1.1ON300200(cts/10ms)Itot100I=56.2±1.1GRAY0050100(C)(D)806040(cts/10ms)Idel200100120140160180200010002000Time(s)Occurrence(E)(F)(G)(H)0040080301010A/A=0.12A=0.69centersideON−1−1AGRAY=1.08103006010−22010(τ)−2−320040(2)1010g(cts/10ms)−4Occurrence10−310Itot1002010τ=34.6ns−5ON10PLintensity(cts/ps/s)τ=9.8nsPLintensity(cts/ps/s)−4GRAY−60001010050100150−100001000050100100101102103®τ(ns)Lagtimeτ(ns)Delaytime(ns)Delaytime(ns)(I)(J)(K)(L)8080210QDON2BeforeturnOFF6010600.3AfterturnON4040110.210101(cts/10ms)10(cts/10ms)iOccurrenceOccurrenceOccurrence0.1Idel20Idel,20Occurrence(norm.)0000.0010010100100200300400−20000200050I(cts/10ms)ΔI(cts/10ms)ΔI(cts/10ms)I(cts/10ms)toti+1idelFigureE9—Overviewofphotoluminescencepropertiesofquantumdot9.E11

11(A)(B)500I=366.0±0.3ON400300200(cts/10ms)I=89.0±0.3ItotGRAY10000100(C)(D)100(cts/10ms)50Idel002040608010005001000Time(s)Occurrence(E)(F)(G)(H)0050060201010A/A=0.14A=0.73centersideON−1400−1101510−240A=1.5110300GRAY(τ)−2−3(2)101010200g(cts/10ms)−420Occurrence−310Itot510100τ=46.9ns−5ON10PLintensity(cts/ps/s)τ=6.9nsPLintensity(cts/ps/s)−4GRAY−60001010050100150−100001000050100100101102103®τ(ns)Lagtimeτ(ns)Delaytime(ns)Delaytime(ns)(I)(J)(K)(L)2100.20QDONBeforeturnOFF100100AfterturnON110.1510101100.10(cts/10ms)50(cts/10ms)i50OccurrenceOccurrenceOccurrenceIdelIdel,0.05Occurrence(norm.)0000.00010010100100200300400500−20000200050100I(cts/10ms)ΔI(cts/10ms)ΔI(cts/10ms)I(cts/10ms)toti+1idelFigureE10—Overviewofphotoluminescencepropertiesofquantumdot10.E12

12FigureE11–E20—Resultsofspectrometer-APDexperiments.BelowweprovideanoverviewofresultsfromexperimentsemployingsimultaneousdetectionbyasingleAPDandaspectrometer.Theseexperimentswereperformeddirectlyafterthedouble-APDexperimentsofFigureE1–E9.Thearrangementofeachofthesefiguresisasfollows:(A)Distributionofdelayedemissionintensity,Idel.Thecolors(blue,cyan,green,yellow,orange,red)indicatethesixdelayedemissioncategoriesusedinthiswork.(B)Pho-toluminescencedecaycurvesfromselectedperiodswithincreaseddelayedemissionintensity,correspondingtothesixdelayed-emissioncategoriesindicatedin(A).Symbolsrepresentexperimentaldata,linesaremono-exponentialfitsondelay-timerange50–150ns.(C)Thesameasin(B),butdisplayedindoublelogarithmicaxes.(D)Amplitudesanddecayratesobtainedfromfitsofexponentialdecaytotheexperimentaldecaycurvesdepictedin(B).Symbolsareexperimentaldata,colorsindicatethedelayed-emissioncategory(seeA).Thesolidlineisalinearfittothedatapoints.(E)Single-QDPLspectraasafunctionofIdel,correspondingtothesixdelayed-emissioncategoriesindicatedin(A).ThedottedlineisaguidetotheeyeandindicatesthePLpeakpositionofthe‘no-delayed-emission’spectrum.(F)PLpeakpositionand(G)full-width-at-half-maximumasafunctionofourselectionofIdel,displayedhereasthemeanstandarddeviationofLorentzianfitstotheselected18-msintegratedspectralframes.0(A)(D)(E)(F)100.2−1010−20.1−2010−310ΔE(meV)−40−4Occurrence(norm.)10Amplitude(cts/ps/s)0.001020300.000.02I(cts/18ms)Decayrate(1/ns)del(B)(C)(G)−1120−110PLintensity(arb.u.)10−210010−38010−2−4601010−5401020−6FWHM(meV)−310010PLintensity(cts/ps/s)PLintensity(cts/ps/s)01002001001011021032.01.80102030Delaytime(ns)Energy(eV)I(cts/18ms)Delaytime(ns)delFigureE11—Resultsofspectrometer-avalanchephotondiodeparallelmeasurements,quantumdot1(thequantumdotdiscussedinthemaintext).E13

130(A)(D)(E)(F)100.2−1010−20.1−2010−310ΔE(meV)−40−4Occurrence(norm.)10Amplitude(cts/ps/s)0.001020300.000.02I(cts/18ms)Decayrate(1/ns)del(B)(C)(G)−1120−110PLintensity(arb.u.)10−210010−38010−2−4601010−5401020−6FWHM(meV)−310010PLintensity(cts/ps/s)PLintensity(cts/ps/s)01002001001011021032.01.80102030Delaytime(ns)Energy(eV)I(cts/18ms)Delaytime(ns)delFigureE12—Resultsofspectrometer-avalanchephotondiodeparallelmeasurements,quantumdot2.0(A)(D)(E)(F)100.2−1010−20.1−2010−310ΔE(meV)−40−4Occurrence(norm.)10Amplitude(cts/ps/s)0.001020300.000.02I(cts/18ms)Decayrate(1/ns)del(B)(C)(G)−1120−110PLintensity(arb.u.)10−210010−3801060−2−4101040−510FWHM(meV)20−6−310010PLintensity(cts/ps/s)PLintensity(cts/ps/s)01002001001011021032.01.80102030Delaytime(ns)Energy(eV)I(cts/18ms)Delaytime(ns)delFigureE13—Resultsofspectrometer-avalanchephotondiodeparallelmeasurements,quantumdot3.E14

140(A)(D)(E)(F)100.20−110−2−20100.1−3−4010ΔE(meV)−4−60Occurrence(norm.)10Amplitude(cts/ps/s)0.001020300.000.02I(cts/18ms)Decayrate(1/ns)del(B)(C)(G)−1−110PLintensity(arb.u.)12010−210010−38010−2−4601010−54010FWHM(meV)20−6−310010PLintensity(cts/ps/s)PLintensity(cts/ps/s)01002001001011021032.01.80102030Delaytime(ns)Energy(eV)I(cts/18ms)Delaytime(ns)delFigureE14—Resultsofspectrometer-avalanchephotondiodeparallelmeasurements,quantumdot4.0(A)(D)(E)(F)100.4−1010−2100.2−20−310ΔE(meV)−4Occurrence(norm.)10Amplitude(cts/ps/s)0.0−4001020300.000.020.04I(cts/18ms)Decayrate(1/ns)del(B)(C)(G)00101080−1PLintensity(arb.u.)10−1−2601010−31040−2−41010−52010FWHM(meV)−6−310010PLintensity(cts/ps/s)PLintensity(cts/ps/s)01002001001011021032.01.80102030Delaytime(ns)Energy(eV)I(cts/18ms)Delaytime(ns)delFigureE15—Resultsofspectrometer-avalanchephotondiodeparallelmeasurements,quantumdot5.E15

150(A)(D)(E)(F)100.4−1010−2100.2−20−310ΔE(meV)−40−4Occurrence(norm.)10Amplitude(cts/ps/s)0.0010203040500.000.020.04I(cts/18ms)Decayrate(1/ns)del(B)(C)(G)001010100−1PLintensity(arb.u.)1080−1−2101060−310−2−4401010−52010FWHM(meV)−3−610100PLintensity(cts/ps/s)PLintensity(cts/ps/s)01002001001011021032.01.801020304050Delaytime(ns)Energy(eV)I(cts/18ms)Delaytime(ns)delFigureE16—Resultsofspectrometer-avalanchephotondiodeparallelmeasurements,quantumdot6.0(A)(D)(E)(F)100−10.410−20−2100.2−40−310ΔE(meV)−60−4Occurrence(norm.)10Amplitude(cts/ps/s)0.0010203040500.0000.0250.050I(cts/18ms)Decayrate(1/ns)del(B)(C)(G)001010100−1PLintensity(arb.u.)1080−1−2101060−310−2−4401010−52010FWHM(meV)−3−610100PLintensity(cts/ps/s)PLintensity(cts/ps/s)01002001001011021032.01.801020304050Delaytime(ns)Energy(eV)I(cts/18ms)Delaytime(ns)delFigureE17—Resultsofspectrometer-avalanchephotondiodeparallelmeasurements,quantumdot7.E16

160(A)(D)(E)(F)100.40−110−20−2100.2−40−3ΔE(meV)−6010−4−80Occurrence(norm.)10Amplitude(cts/ps/s)0.0010203040500.000.020.04I(cts/18ms)Decayrate(1/ns)del(B)(C)(G)001010120−1PLintensity(arb.u.)10100−1−2101080−31060−2−4101040−510FWHM(meV)20−3−610100PLintensity(cts/ps/s)PLintensity(cts/ps/s)01002001001011021032.01.801020304050Delaytime(ns)Energy(eV)I(cts/18ms)Delaytime(ns)delFigureE18—Resultsofspectrometer-avalanchephotondiodeparallelmeasurements,quantumdot8.0(A)(D)(E)(F)100.40−110−20−2100.2−40−3ΔE(meV)−6010−4−80Occurrence(norm.)10Amplitude(cts/ps/s)0.0010203040500.000.020.04I(cts/18ms)Decayrate(1/ns)del(B)(C)(G)001010120−1PLintensity(arb.u.)10100−1−2101080−31060−2−4101040−510FWHM(meV)20−3−610100PLintensity(cts/ps/s)PLintensity(cts/ps/s)01002001001011021032.01.801020304050Delaytime(ns)Energy(eV)I(cts/18ms)Delaytime(ns)delFigureE19—Resultsofspectrometer-avalanchephotondiodeparallelmeasurements,quantumdot9.E17

170(A)(D)(E)(F)100.40−110−20−2100.2−40−3ΔE(meV)−6010−4−80Occurrence(norm.)10Amplitude(cts/ps/s)0.0040800.000.020.04I(cts/18ms)Decayrate(1/ns)del(B)(C)(G)001010120−1PLintensity(arb.u.)10100−1−2101080−31060−2−4101040−510FWHM(meV)20−3−610100PLintensity(cts/ps/s)PLintensity(cts/ps/s)01002001001011021032.01.804080Delaytime(ns)Energy(eV)I(cts/18ms)Delaytime(ns)delFigureE20—Resultsofspectrometer-avalanchephotondiodeparallelmeasurements,quantumdot10.E18

18E19