Design of Novel Highly E ffi cient Yellow-Orange Color-Tunable Luminescence in Rb 2 Sr 1 − - Zhang et al. - 2021 - Unknown

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pubs.acs.org/JPCLLetterDesignofNovelHighlyEfficientYellow-OrangeColor-Tunable2+LuminescenceinRb2Sr1−yCayP2O7:xEuSolidSolutionsforWhiteLight-EmittingDiodesQiangZhang,XichengWang,XiaopengZhou,andYuhuaWang*CiteThis:J.Phys.Chem.Lett.2021,12,1087−1092ReadOnlineACCESSMetrics&MoreArticleRecommendations*sıSupportingInformationABSTRACT:Traditionalwhitelight-emittingdiodes(WLEDs)arelimitedbytheenergylossduetoreabsorption.Integratingbinarycomplementarycolorphosphorswithnear-ultraviolet(n-UV)LEDchipscanbeagoodsolution,andthecoreofitistodevelopyellow-emittingphosphors.Inthiswork,wehavedesignedRbSrCaPO:xEu2+solidsolutionswithyellow-21−yy27orangecolor-tunableluminescence.Thecrystalstructure,luminescenceproperties,andpotentialapplicationsforWLEDswereexploredsystematically.Undern-UVlightexcitation,thephosphorsefficientlyemitbroadbandyellow-orangeemission.ThereasonsandmechanismsofthevariationofthePL/PLEspectrahavebeeninvestigated.TheoptimalRbSrPO:0.5%Eu2+227sampleexhibitsahighquantumefficiencyof72.96%withagoodcolorpurityof87.1%.UponcombinationoftheBAM:Eu2+andRbSrPO:0.5%Eu2+phosphorswitha380nmn-UVchip,a227WLEDdeviceisfabricatedandcanemitwhitelightwithgoodperformance.Comparedwithtraditionallightsources,whitelight-absorbn-UVtobluelightandefficientlytransformitintoemittingdiodes(WLEDs)havehighlymetthehumanvisiblelighteventothenear-infraredregion,andluminescencedemandforhigh-qualitywhitelightduetotheirhighefficiency,spectraltuningiseasilyfulfilledbythevariationofthehostenergyconservation,andenvironmentalfriendliness.1−3Whitestructure.17,18TosearchforaproperhostforEu2+iondoping,lightcanbeeasilyproducedviaasetupofabluechipwithawefocusmainlyonphosphatesbecauseoftheirgoodchemicalYAGphosphor,yettheabsenceofaredcomponentinsuchastability,moderatesynthesistemperatures,andhighluminouscasecangiverisetoalowcolorrenderingindex(CRI)andaefficiency.18Amongtheirabundantfamilymembers,the4highcorrelatedcolortemperature(CCT).Asanimprove-A2MP2O7(A=Li,Na,K,orRb;M=Mg,Ca,orSr)systemDownloadedviaBUTLERUNIVonMay16,2021at06:35:26(UTC).ment,anothermethodhasbeenintroducedbyfabricatingahasattractedthemostattentionandbeenthoroughlynear-ultraviolet(n-UV)chipwithRGBtricolorphosphors.519−22investigatedasahostmatrix.Intheirbasicstructure,However,therearestillsomeunsolvedproblems.Thefirstistwo[PO4]tetrahedraconnectasa[P2O7]groupviacorner-energylossduetoreabsorption.ThesecondisthecomplicatedsharingthesameOatoms.Thenthe[P2O7]groups6−8andcostlyproductionprocess.Toovercometheseconcatenatewith[MO]octahedratoformtheframework.Seehttps://pubs.acs.org/sharingguidelinesforoptionsonhowtolegitimatelysharepublishedarticles.6problems,aneotericsolutionhasbeenproposedbyusingaThealkalimetalionsfilltheintersticeswithdifferentblendofbinarycomplementarycolorphosphorswithn-UVcoordinationnumbers(CNs).Inthisstudy,weselectLEDchips.ThecoreofthisapproachistofindaphosphorthatRb2SrP2O7(RSP)asthehostmatrix,whichwasfirstreportedpossessesabroadyellowemissionwithmoreredcomponentsin1991.22Itcouldbesynthesizedatalowtemperature,anditsthatalsocanbeefficientlyexcitedbyn-UVlightratherthanrichcationicsitesarecapableofprovidingmultipleoccupied9,10bluelight.Sofar,manyyellow-emittingphosphorshavepositionsforthedopingions,whichisconducivetoobtainingabeendevelopedandevaluated.Nevertheless,theresultsarenottunableandefficientluminescence.satisfyingandtheobtainedphosphorssufferfromtheproblemsAccordingly,forthepurposeoffundamentalresearchandofweakabsorptioninthen-UVregion,lowluminescent2+11−13practicalapplications,wehavedevelopedaEu-dopedRSPefficiency,andpoorthermalstability.Hence,findingnoveloxide-basedyellow-emittingphosphorswithexcellentluminescentpropertieshasalwaysbeenapopularandarduousReceived:December20,2020task.Accepted:January18,2021AsuitablephosphorcomesfromparticularlyselectingthePublished:January20,2021hostandactivatorions.Amongthecommonlyusedactivators,weareparticularlyinterestedinobtainingatargetedphosphorwithEu2+ions.14−16TheEu2+ion-dopedphosphorscan©2021AmericanChemicalSocietyhttps://dx.doi.org/10.1021/acs.jpclett.0c037371087J.Phys.Chem.Lett.2021,12,1087−1092

1TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetterFigure1.(aandb)RietveldrefinementsofRSPandRSP:0.5%Eu2+,respectively.(c)CrystalstructureoftheRSPhost.(d)CoordinationenvironmentsofRbandSrsites.(e)XRDpatternsofRSP:xEu2+(0.25%≤x≤4%)samples.Figure2.(a)PLandPLEspectraoftheRSP:0.5%Eu2+sample.TheinsetshowsadigitalphotooftheRSP:0.5%Eu2+sampleunderann-UVlamp.(b)PLspectraoftheRSP:0.5%Eu2+sampleuponexcitationatdifferentwavelengths.phosphorwithyellowemission.Furthermore,withbridgingP−O−Plinkagesof128.553°isformedbytwoRb2Sr1−xCaxP2O7(0≤x≤1)solidsolutionsweredesigned[PO4]tetrahedrasharingthesameOatom.Bysharingatoachievecolor-tunableluminescenceandtooptimizethecorner,the[P2O7]groupsconnectwiththesurrounding[SrO]octahedratoformthebasicskeleton,andRb+ionsfillluminescentproperties.Thestructure,luminescentproperties,6andpotentialapplicationsforWLEDswereexploredsystem-itspores.Figure1dshowsthecoordinationenvironmentsofRbandSrsites.TheonlytypeofRb+ioniscoordinatedwithatically.PanelsaandbofFigure1illustratetheRietveldrefinementsnineOatoms,anditsradiusis1.63Å;theaveragebondlengthofRSPandRSP:0.5%Eu2+,respectively,toverifythephaseiscalculatedas3.0939Å.23Forthesix-coordinatedSr2+ionpurity.Forbothofthem,theobserveddatahighlymatchthewitharadiusof1.18Å,theaveragebondlengthis2.4853Å,23calculateddatabecausethedifferencesbetweenthemareverywhichismuchshorterthantheRb−Obondlength.Theslightandnoextraimpuritypeaksexist.Theresultsprovethatradiiforthesix-coordinatedandnine-coordinatedEu2+ions23thesinglephaseofRSPhasbeenobtained,andthedopingare1.17and1.30Å,respectively.WhentheshortestionicEu2+ionsintroducenoimpurityphases.Thedetailedradiiandthesamenumberofchargesareconsidered,thedopingEu2+ionscouldoccupyonlyonetypeofSr2+ionsites.informationaboutRietveldrefinementislistedinTableS1.Fromthestructuredata(TableS2),thecrystalstructureofAfterdopingwithEu2+ions,theXRDpatternsofRSP:xEu2+theRSPhostisshowninFigure1c.RSPisathree-dimensional(0.25%≤x≤4%)samplesweretestedandareshowninnetworkstructure,andinitsstructuralunit,a[P2O7]groupFigure1e.Allofthepeaksmatchwellwiththecalculateddata,1088https://dx.doi.org/10.1021/acs.jpclett.0c03737J.Phys.Chem.Lett.2021,12,1087−1092

2TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetterFigure3.Normalized(a)PLEand(b)PLspectraofRSP:0.5%Eu2+,yCa2+(0≤y≤1)phosphors.andtherearenoimpurityphasesevenathigherdopingweakenedduetotheconcentrationquenchingeffect,whichis26concentrations.Moreover,fromtherightpanelofFigure1e,duetotheenergytransferbetweenactivatorions.Thenthewecanobservethatthediffractionpeaksintherangeof28.3−quenchingmechanismisdeterminedasthedipole−dipole31.3°shifttolargerangleswithanincreaseinEu2+content.interaction,whichisdiscussedinFigureS3b.2+Meanwhile,theQEoftheoptimalRSP:0.5%Eu2+phosphorThisphenomenonoriginatesfromthelargerSrionsbeingsubstitutedwithsmallerEu2+ions.wasdeterminedtoreach72.96%,whichcansatisfytheTheSEMmicrograph,TEMimage,HRTEMimage,EDXcommercialrequirements.Inaddition,afteroptimizationofthespectrum,andEDSmappingoftheRSP:0.5%Eu2+sampleareprocessingconditionsandchemicalcomposition,thevalueof27investigatedsystematically(FigureS1).TheresultsprovethatQEcouldbelikelyestimatedtoincreaseevenfurther.ThecolorcoordinatesoftheRSP:0.5%Eu2+samplewerecalculatedthepowderedsamplehasgoodcrystallinityandalloftheelementsarehomogeneouslydistributed.Accordingtotheas(0.452,0.503),andthenthecolorpuritywascalculatedtorefinedcrystalstructure,thebandstructureoftheRSPhosthasbe87.1%(SupplementaryNote1),whichishigherthanthoseofsomeyellow-emittingphosphorssuchasLiBaPO:1%Bi3+beeninvestigatedandtheresultssuggestthatRSPhasadirect4(68.2%),ZnGeN(82%),SrZnSc(PO):Eu2+(75%),andbandgapof4.852eV(FigureS2a,b).Thenthetotalandpartial28473+13,28−30densitiesofstatesofRSParecalculatedandexhibited.TheRbCa7.95Mg7Si9N22:0.05Ce(84%),indicatingabetter4pandO2porbitalsmainlycontributedtotheCB,andtheVBperformanceforWLEDs.Tofurtherunderstandtheenergytransferprocess,thedecaycurvesofRSP:xEu2+(0.25%≤x≤isdominatedbytheSr3dorbital(FigureS2c).Moreover,theDRSoftheRSPhostismeasuredanddepictedinFigureS2d.4%)phosphorsexcitedat368nmandmonitoredat575nmweremeasuredandareshowninFigureS4.ThecurvescanbeTheopticalbandgapofRSPisestimatedbyextrapolatingthe31fitwellintothefollowingsingle-exponentialfunction:linearportionbasedonitsDRS(insetofFigureS2d),andthebandgapsobtainedbythesetwomethodsareconsistent.2+I()TA=−1exp(/)tτ(1)ThentheluminescentpropertiesofRSP:xEu(0.25%≤x≤4%)sampleswereevaluatedandinvestigated.Figure2a2+whereI(T)meanstheemissionintensityattimet,AisadisplaysthePLandPLEspectraoftheRSP:0.5%Eusampleconstant,andτreferstothelifetime.Thecalculatedlifetime(λex=368nm;λem=575nm).Asonecansee,under368nmdecreasesfrom1.32to0.635μswithanincreaseinEu2+lightexcitation,thephosphoryieldsintenseyellowemissioncontentfrom0.25%to4%.Astheconcentrationofactivatorspeakingat575nmwithafullwidthathalf-maximum(fwhm)increases,thedistancebetweenEu2+ionsbecomesshorter,of130nm.Thebroademissionbandisattributedtothe5d→whichwillincreasetheprobabilityofthenonradiative2+244ftransitionofEuions,andthesymmetricshapeofthetransitionbetweenEu2+ions.Thus,thefluorescencedecaycurveimpliesthatonlyoneluminescentcenterexistsinthelifetimesbecomefaster.32Moreover,thetime-resolvedphoto-2+RSP:0.5%Euphosphor,whichiscoincidentwiththeformerluminescence(TRPL)spectraoftheRSP:0.5%Eu2+sampleanalysisthatEu2+ionsoccupyonlySr2+sites.25Inaddition,wererecordedinFigureS5withdecaytimesfrom1992.2towhenmonitoredat575nm,astrongexcitationbandinthe3847.7ns.TheTRPLspectraareingoodagreementwiththerangeof300−430nmcanbeclearlydetectedwiththePLspectrumoftheRSP:0.5%Eu2+sample,andinaddition,amaximumat368nm.ThewideexcitationbandallowstheconstantshapeoftheTRPLspectraunderdifferentdecayphosphortoheightmatchn-UVLEDs.ThePLspectraofthetimescanbedetected.TheresultsprovidefurtherevidenceforRSP:0.5%Eu2+sampleuponexcitationatdifferentwavelengthsthesingleluminescencecenterinthecrystallattice.werealsomeasuredtoexplorethenumberofluminescentFurthermore,torealizecolor-tunableluminescenceandcenters(Figure2b).Theintensityofemissioncurvesvariesoptimizetheluminescentproperties,RSP:0.5%Eu2+,yCa2+(0withexcitationwavelength,yetboththeshapeandthepeak≤y≤1)solidsolutionsweredesignedandevaluated.Thepositionremainthesame,whichprovidesreasonableproofforXRDpatternsofRSP:0.5%Eu2+,yCa2+(0

3TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetterFigure4.(a)Temperature-dependentintegratedemissionintensityofRSP:0.5%Eu2+.(b)Emissionspectrumandaphotographoftheas-fabricatedpc-LED.≤y≤1)solidsolutionshadbeenachieved.ThecorrespondingEu2+andO2−ions.ThisphenomenoncausesalargerDandqcrystallographicdataandstructurerefinementparametersarealsolowersthelowest5dstateofEu2+,whichgeneratesaredlistedinTableS3.Moreover,theEDSmappingofselectedshiftofbothPLandPLEspectra.Onthecontrary,thevaluesRSP:0.5%Eu2+,yCa2+(y=0.6and1)samplesareshowninoftheStokesshiftforyvaluesof0,0.2,0.4,0.6,0.8,and1areFiguresS7andS8.Theimagescandemonstratethatallofthecalculatedas9783,9845,10005,10087,10198,and10425elementsarehomogeneouslydistributedintheparticles.cm−1,respectively.TheincreasedStokesshiftscouldoriginateThePLEandPLspectraofRSP:0.5%Eu2+,yCa2+(0≤y≤fromtheenhancedinteractionbetweenelectronsandphonons1)phosphorsaremeasuredanddisplayedinFigure3.Astheduringthetransitionandthuslosemuchenergy.35Inaddition,2+contentofCaincreases,aslightredshiftoccursattheboththePLintensityandtheQEdeclinegraduallyastheCa2+excitationprofilesandalsotheabsorptionnear400nmiscontentincreases(TableS4).Thisphenomenonisdiscussedenhanced(Figure3a),whichfavorsabettermatchbetweentheandexplainedinFigureS10.obtainedphosphorsand380−400nmn-UVchips.UponThetemperature-dependentPLspectraofexcitationofthemaximumvalue,allofthephosphorsemita2+Rb2Sr1−yCayP2O7:xEusamplesweremeasured;thebroadsymmetricbandintherangeof450−750nm(Figure2+RSP:0.5%Euphosphordisplaysthebestthermalstability,3b);however,themainpeakshiftstolongerwavelengthfromandthecorrespondingspectraaredepictedinFigure4a.With575to613nm,andthePLintensitydecreasesgraduallyfromyanincreasedtemperature,thePLintensityremainsat42.5%at=0to1.ThemainpeaksofPLEandPLspectra,Stokesshifts,2+2+150°C,whichisclosetothatofthecommercialfwhms,QEs,andPLintensitiesofRSP:0.5%Eu,yCa(0≤2+36y≤1)phosphorsaresummarizedinTableS4.ThentheCIE(Sr,Ba)2SiO4:Euphosphor(45%).ItcanbefurtherchromaticitydiagramsofRSP:0.5%Eu2+,yCa2+(0≤y≤1)improvedbyasurfacecoatingmethodinpractical37phosphorsareillustratedinFigureS9.Thecolorcoordinatesapplications.Thephosphorisstronglyexpectedtobechangefrom(0.452,0.503)aty=0to(0.547,0.443)aty=1,appliedinsolid-statelightingconsideringitsspecialperform-andthecolorshiftsfromyellowtoorange.Theresultsmanifestances.Asproof,thepc-WLEDwasfabricatedbycombiningtheBAM:Eu2+andRSP:0.5%Eu2+phosphorswitha380nmn-UVthattheexcitationandemissionspectracanbeadjustedeffectivelybythedesignofsolidsolutions.chip.Theemissionspectrumandaphotographoftheas-Fromtheliterature,fortheexcitationandemissionfabricatedpc-LEDaredepictedinFigure4b.TheexhibitedpropertiesofluminescentmaterialsdopedwithEu2+,bothofbrightwarmwhitelightshowsaCIEof(0.344,0.333),ahigh2+33themareassociatedwiththe4fand5denergylevelsofEu.CRIof88.4,alowCCTof4425K,andaluminousefficiencyAsthe5dorbitalstronglydependsonthecoordinationof29.23lm/Wunderacurrentof40mA,providingfurtherenvironment,theadjustmentofPLandPLEperformancescanevidencefortheRSP:Eu2+phosphortobeappliedforhigh-befulfilledbyalteringthecompositionandstructureofthequalityWLEDlighting.matrix.FortheRSP:0.5%Eu2+,yCa2+(0≤y≤1)system,the2+Insummary,thecolor-tunableEu-activatedtuningofthePLandPLEspectraisrelatedtothecrystalfieldRb2Sr1−xCaxP2O7solidsolutionhasbeenrealizedundersplitting(Dq)andStokesshift.Thefollowingformulaisusedmoderateconditions.Thecalculatedbandgaphasagoodfit34toestimateDq:withtheexperimentalvalueandsuppliesaproperbandgapforEu2+ionstobetheluminouscenter.Thephosphorscan412rDZq=e5absorbthen-UVlightandefficientlyemitbroadbandyellow-6R(2)orangelight.Accordingtotheneed,themainpeakcanshiftfrom575to613nmasthereplacedCa2+contentchanges.ThewhereZrepresentstheanioncharge,ereferstotheelectronQEfortheRSP:0.5%Eu2+sampleis72.96%,anditscolorcharge,rmeanstheradiusofthed-wavefunction,andRisthebondlength.Inthiscase,Disproportionaltoonly1/R.5Withpurityiscalculatedtopeakat87.1%.Moreover,ann-UVchip-qanincreaseiny,weknowfromtheresultsofRietveldbasedWLEDhasbeenachievedwithaCIEof(0.344,0.333),refinementfortheRSP:0.5%Eu2+,yCa2+(0≤y≤1)systemahighCRIof88.4,andalowCCTof4425Kbyfabricatingthe380nmchipwithRSP:0.5%Eu2+andBAM:Eu2+thatthelatticeparametersdecreaseandthematrixshrinkagewillleadtoadecreaseinthedistancebetweenthesurroundingphosphors.Alloftheresultspavethewayforconceiving1090https://dx.doi.org/10.1021/acs.jpclett.0c03737J.Phys.Chem.Lett.2021,12,1087−1092

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