Highly In-Plane Polarization-Sensitive Photodetection in CsPbBr 3 Single Crystal - Wang et al. - 2021 - Unknown

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pubs.acs.org/JPCLLetterHighlyIn-PlanePolarization-SensitivePhotodetectioninCsPbBr3SingleCrystalKaiyuWang,LinJing,QingYao,JieZhang,XiaohuaCheng,YeYuan,ChenyuShang,JianxuDing,*TianliangZhou,*HaiqingSun,WeiweiZhang,andHuipingLi*CiteThis:J.Phys.Chem.Lett.2021,12,1904−1910ReadOnlineACCESSMetrics&MoreArticleRecommendations*sıSupportingInformationABSTRACT:Thefullyinorganicperovskiteleadcesiumbromidesinglecrystal(CsPbBr3SC)isconsideredasanexcellentcandidatesemiconductorforphotodetectorsbecauseofitssuperiorhumidityresistance,thermalstability,andlightstabilitycomparedwithorganic−inorganichybridperovskitesaswellasitsphotoelectricpropertiessuchaslargelightabsorptioncoefficientandultralongcarriermigrationdistance.InthisLetter,weutilizetheinversetemperaturesolubilityofCsPbBr3internarysolventstogrowlarge-sizedCsPbBr3SCs.Bytheuseofthe(101)plane,CsPbBr3SC-basedphotodetectorsarefabricated,whichexhibitexcellentpolarizedlightresponsecharacteristics.Thephotocurrentreliesonthepolarizationangleinasinusoidalfashionandshowsstronganisotropicoptoelectronicproperties.Thephotodetectionperformanceperpendiculartotheyaxisissignificantlyhigherthanthatparalleltotheyaxis,andthedichroicratiounder405nmilluminationatabiasvoltageof1Vreaches2.65.Theexperimentalresultsareconsistentwiththeresultsoffirst-principlescalculations.ecently,leadhalideperovskiteswiththeABX3stoichio-comparedwithCsPbBr3SCsgrownbytheBridgmanmethod,Rmetricratio(A=CHNH+,CH(NH)+,Cs;B=Pb2+,3322singlecrystalsgrownbythesolutionmethodhavelowertrapSn2+;X=I−,Br−,Cl−)havebeenwidelystudiedbecauseofdensity,lowercarrierdensity,moderatecarriermobility,andtheirexcellentoptoelectronicproperties,suchaslarge1718higherγphotonabsorptionrate.Xuetal.grewCsPbBr312absorbancecoefficient,longcarrierdiffusiondistance,highSCsdirectlyonITOglassandfabricatedtheAg/CsPbBr3/ITO345carriermobility,highdefecttolerance,lowcost,andsoon.sandwichstructuralX-raydetectorwithSchottkycontact.TheTheseexcellentpropertiespromoteitsapplicationinsolardevicehaslowdark-currentdensity(∼5−27nA/cm2)andcells,6,7light-emittingdiodes,8,9lasers,10photodetectors,andhighsensitivity(770μC·Gy−1·cm−2)at8Vvoltage.The11,12soon.However,fororganic−inorganichybridperovskiteaboveresearchprogressontheopticaldetectionpropertiesofmaterials,theirpoormoistureresistanceandhightemperatureCsPbBr3SCshaveevokedmoreresearcherstoexploretheirresistanceoforganicmoleculesinhibittheirdevelopmentinapplicationsinthefieldofphotodetectors.theoptoelectronicfield.Comparedwithorganic−inorganicOneoftheimportanttopicsforsingle-crystalphotodetectorsDownloadedviaUNIVOFCALIFORNIASANTABARBARAonMay16,2021at11:48:08(UTC).Seehttps://pubs.acs.org/sharingguidelinesforoptionsonhowtolegitimatelysharepublishedarticles.hybridperovskitematerials,fullyinorganicCsPbBr3hasbetterisphotoelectronicanisotropy.Recently,muchefforthasbeenthermalstabilityandhumiditystability,anditsoptoelectronicmadetorevealthephotoelectronicanisotropyforbothhybridperformancedoesnotdeteriorateforalongtime.13Besides,19,2021andfullyinorganicperovskitesinglecrystals.Lietal.theexistencestateoftheCsPbBr3isalsoanimportantcriterionusedatemplate-constrainedmethodtopreparethestabletwo-forapplicationsinthefieldofoptoelectronicdevices,especiallydimensionallayeredperovskite(BA)2(MA)n−1PbnX3n+1intoforphotodetectors.Forinstance,intheassemblednano-anisotropicmicrofilamentationarrays.Withthisanisotropicparticles,microcrystals,andfilms,thematerialcrystallinityandstructure,thedarkcurrentisaslowas10−12A,theresponseis14stoichiometrycangreatlyaffectsurfacestates,suchasshallowhighat3.5A·W−1,andthedetectivityexceeds1×1015Jones.ordeeptraps,whichcanplayamajorroleincarrierThismaterialhasbeensuccessfullyappliedtohigh-perform-recombinationandextractiondynamics.Therefore,CsPbBr3ancepolarizationdetection.Yan22usedMAPbIsingle-crystal3SChasbeenpaidmoreattentioninphotodetectors.Forinstance,CsPbBr3microrodSCsgrownbytheantisolventmethodwereusedtopreparephotodetectors,andtheReceived:January14,2021detectivityandon−offratioofCsPbBr3microrodSCsreachedAccepted:February8,20213.67×1012Jonesand988,respectively.15Kanatzidisetal.Published:February16,2021grewCsPbBr3SCsbytheBridgmanmethodandpreparedplanarphotodetectorswithlowdark-currentdensity(∼100nA/cm2)andtimestability.16Dirinetal.confirmedthat©2021AmericanChemicalSocietyhttps://doi.org/10.1021/acs.jpclett.1c001271904J.Phys.Chem.Lett.2021,12,1904−1910

1TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetterFigure1.(a)PowderandplaneXRDpatternsofCsPbBr3SC.(b)Photosoftheas-grownCsPbBr3SC.(c)EDScharacterizationofCsPbBr3SC.Figure2.(a)AbsorptionandphotoluminescencespectraofaCsPbBr3SC.TheinsetshowstheTaucplot.(b)Time-resolvedPLforaCsPbBr3SC.(c,d)FluorescencemicroscopyofaCsPbBr3SCunderbright-fieldandultravioletlight,respectively.26thinfilmswithdifferentorientationstoconstructaverticalnoncentrosymmetriccharacter.Thus,itsphysicalproperties,structureoffield-effecttransistors,observedanisotropiccarriersuchasphotoelectronicproperties,arepronetoexhibitstrongtransportinaMAPbI3singlecrystal,anddeducedthattheanisotropy.Inthiswork,wereportthatlarge-sizedCsPbBr3anisotropyofcarriertransportwasattributedtothemigrationSCscanbegrownviathesimpleinversetemperatureofMAunderanelectricfield.Ourgroupreportedthathighercrystallizationmethodindimethylsulfoxide(DMSO)/N,N-MA+and[PbBr]4−densitiesonthe(111)surfaceofadimethylformamide(DMF)/g-butyrolactone(GBL)ternary6MAPbBr3singlecrystalresultedinhigherinternalelectricfieldsolvents.Thein-planepolarization-sensitivephotodetectioncomparedwiththe(100)surface,whichultimatelyaffectedthepropertiesarerevealedviaaplanarmetal−semiconductor−ionicconductance,darkcurrent,photocurrent,andon−offmetalphotodetector,whichclearlydemonstratesthephoto-23ratio.TheabovestudiesindicatethattheperovskitematerialselectronicanisotropyinCsPbBr3SCs.havecrystalorientationandanisotropy,whichstronglyaffectFigure1adisplaysthepowderandplaneXRDpatternsof24thematerialpropertiesofhalideperovskites.Zhangetal.theCsPbBr3SC.ComparisonofthepowderXRDdatawithstudiedtheanisotropicphotoelectricpropertiesofCsPbBr3thecalculateddatashowsthatallofthediffractionpeakscrystalsforthefirsttimeandfoundthattheelectronmobilitybelongtoorthorhombic-phaseperovskite,andthespacegroupalongthebaxis(11.61cm2·V−1·s−1)was1orderofmagnitudeisassignedasPnma.Nootherimpurities,suchasCsPbBrand25higherthanthatalongtheaandcaxes.However,thereisstillaCs4PbBr6,weredetected.Forasinglecrystal,thedetermi-lackofsystematicresearchonthephotoelectronicanisotropynationofthespontaneouslyexposedfacetsiscrucial.Theas-ofperovskitesinglecrystals.grownorangeCsPbBr3SCsexhibitacuboidmorphology,asAnothermethodologytorevealphotoelectronicanisotropyillustratedinFigure1b.ThecuboidCsPbBr3SCisgenerallyofperovskitesinglecrystalphotodetectorsisdetectionunderassembledthrough(101)and(020)facets.Theirsimilar(101)polarizedlight,whichishelpfulforfurtherapplicationasand(020)interplanardistances(5.8074Åvs5.88647Å)make25polarizedlightdetectors.ItisknownthatCsPbBr3belongstoitdifficulttodistinguishtheplanesbecausethediffractiontheorthorhombicsystemandthatitscrystalstructurehaspeaksconstantlyaccompanyeachother.BymicrobeamXRD1905https://doi.org/10.1021/acs.jpclett.1c00127J.Phys.Chem.Lett.2021,12,1904−1910

2TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetterFigure3.(a)SchematicdiagramoftheplanarphotodetectorandphotocurrentmeasurementsontheCsPbBr3SCunderbothunpolarizedandlinearlypolarizedlight.(b)Photocurrentsofthedeviceunderunpolarizedlightatvariousilluminationpowers.(c)DarkI−VcurveoftheCsPbBr3SCforspace-charge-limitedcurrent(SCLC)analysis.(d)Photocurrentsofthedeviceunderpolarizedlightatdifferentpolarizationangleswithanilluminationpowerof0.5mW.(e,f)Photocurrentsofthedeviceunder0.5mWpolarizedilluminationatvariousbiasvoltages.analysis,thetoplargefacetoftheCsPbBr3SCisidentifiedasdynamicsofCsPbBr3SCwasfittedbyabiexponentialthe(101)plane,andthesidefacetisconfirmedasthe(020)function,asshowninFigure2b.Thefastandslowcomponentsplane(Figure1a).Theenergy-dispersiveX-rayspectroscopyofPLlifetimecanbeextractedasτ1=5.5nsandτ2=31.5ns.(EDS)datainFigure1cindicatethattheCs:Pb:BrelementThelongerPLlifetimeofτ2comparedwiththereportedvaluesratioisclosetothestoichiometricratioofCsPbBr3,implyingimpliesthatphotogeneratedelectronsorholeshaveamuchthehighpurityofourCsPbBr3SC.higherlikelihoodtoreachtheinterfacebetweenthesingle29Theopticalabsorptionandphotoluminescence(PL)spectracrystalandelectrodes.Ontheotherhand,wephotographedofCsPbBr3SCareshowninFigure2a.Thesharpabsorptionthecrystalusingafluorescencemicroscope.Figure2c,donsetislocatedataround567nm,correspondingtoadirectcorrespondstothephotosunderbright-fieldandultravioletopticalbandgapof2.19eV,whichissimilartothereportedlightsources,respectively.Itcanbeseenthattheluminescent26,27values.Incontrasttonanocrystals,noconspicuousUrbachcolorofthecrystalisrelativelyuniform,whichindicatesthattailoccursintheTaucfittingplotforourCsPbBr3SC,thePLofCsPbBr3SCishomogeneousandinaccordancewithsuggestingnegligiblephononparticipationinphotonabsorp-thenarrowfwhmofthePLdata.tionandweakself-dopingoftheCsPbBr3SCsemiconductorFigure3ashowsaschematicdiagramofthe(101)-facet-28byvacancyandinterstitialdefects.ThePLspectrumisbasedplanarphotodetectorwithAuinterdigitalelectrodes.Tocenteredat517nmwithastandardGaussianprofileandarevealtheanisotropicphotoelectronicproperties,theinter-narrowfullwidthathalf-maximum(fwhm)of17nm.SuchadigitalelectrodesweredesignedtobeperpendiculartothenarrowfwhmofPLisattributedtodirectelectron−hole[010]orientation.Thezerolinearlypolarizedincidentlightradiativerecombinationinthesinglecrystal.Besides,thebroadwasfixedperpendiculartotheinterdigitalelectrodes.First,theemissionwidthfrom484to575nmsuggeststhatnear-edgephotodetectionwascarriedoutunderunpolarizedlight,anddefectlevelsparticipateincarrierexcitation.ThePLdecaytheresultsaredisplayedinFigure3b.Undertheunpolarized1906https://doi.org/10.1021/acs.jpclett.1c00127J.Phys.Chem.Lett.2021,12,1904−1910

3TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetterlight,boththedarkcurrentandphotocurrentsexhibitrigidphotocurrentreachesthemaximum.Whenthepolarizationlinearfeatures,implyingOhmiccontactbetweentheAuangleis>90°,thecurrentbeginstodecrease.ThesymmetricalelectrodesandCsPbBr3SC.Thedarkcurrentisaslowas8.57angle-relatedphotocurrentssuggestthattheperiodis180°,nA@6V,whichissimilartothatreportedpreviouslyforawhichimpliesthatCsPbBr3SCisapromisingcandidatefor15planarphotodetectorbasedonaCsPbBr3SC.Whenthepolarization-sensitivephotodetectors.Thepolarization-angle-illuminationpoweris1mW,thephotocurrentreaches2000dependentdetailedphotocurrentsatbiasvoltagesof1,3,and5nA@6V,implyingthatsensitivephotodetectionbytheVareplottedinFigure3e,f.TheyshowthatthephotocurrentsCsPbBr3SCoccurs.Thetrap-statedensity(ntrap)iscrucialat90°and270°arelargerthanthoseatotherpolarizationtoevaluatethesemiconductorcrystalqualityandcanbeangles,whichisinaccordwiththecontinuousI−VdeterminedbymeasuringtheI−Vcurvethroughahole-onlymeasurements.Therelationshipbetweenphotocurrentanddeviceusingawell-polishedCsPbBr3SCwafer(0.5mminpolarizationanglecanbefittedbyasinusoidalfunction.Inthedepth),asshowninFigure3c.Thelineardependenceofthepolarization-sensitivephotodetectorbasedonCsPbBr3SCs,currentonthebiasvoltagedemonstratesanOhmicresponsethedeviceshowsexcellentanisotropicpropertieswithanforthehole-onlydevice.Accordingtotherelationshipbetweenultrahighdichroicratioof∼2.65under405nmilluminationcurrentandappliedvoltage,theconductivity(σ)oftheandabiasvoltageof1V,whicharecomparabletothoseoftheCsPbBrSCiscalculatedas5.3×10−8Ω−1·cm−1.Onthe423GeAspolarizedphotodetector.Hereitshouldbementionedotherhand,fromthetrap-filled-limitvoltage(Vtfl),whereallofthatthedichroicratiowascomparedthroughthemaximumthetrapstatesarefilledbyinjectedcarriers,thetrapdensityphotocurrent(IPmax)at90°totheminimumphotocurrent30(nt)canbecalculatedaccordingtotheformula(IPmin)at0°.Ontheotherhand,thedecayofthephotocurrentsunder2enLtcontinuousilluminationatvariouspolarizationanglesisVtfl=2εε0(1)anothercrucialparametertoevaluatethesensitiveresponse.Figure4adisplaystheI−tcurvesofthedeviceunderwhereListhedepthofthecrystal,εistherelativedielectriccontinuous0.5mWilluminationandabiasvoltageof1Vat31constantofCsPbBr3(22),andε0isthevacuumpermittivity.variouspolarizationangles.Undercontinuousillumination,theThetrapdensityisthereforecalculatedas7.45×109cm−3.optical-injection-inducednonequilibriumexcesscarriersmakeMoreover,theholemobility(μ)canbeestimatedaccordingtothephotocurrentsreachthemaximumandthenbegintodecay32theMott−Gurneyequation:toasteadystatethroughelasticscatteringandelectron−3phononinteractions.AsforCsPbBr3semiconductor,the8JLDcurrentdecayinFigure4aisprincipallyattributedtothefactμ=9εεV2thattheCsPbBrSCisamixedconductivesemiconductor,0(2)3withthetotalconductance(Gtotal)attheinitialstagebeingwhereJDandVstandforthecurrentdensityandappliedbiascontributedbyions(Gion)andelectrons(Gelectron),respec-43voltage,respectively.Table1liststheintrinsicoptoelectronictively.Thebias-drivenmigrationofionstoboththeanodepropertiesoftheCsPbBr3SCandfilms.andcathodewillestablishareversebuilt-inelectricfieldandThepolarization-dependentI−VcurvesfortheCsPbBr3SC-depressthefurthermigrationofions.Therefore,thebasedphotodetectorareshowninFigure3d.Underthesamephotocurrentscouldtrendtoasteadystate.Fromthesteadyilluminationpowersof0.5mW,thephotocurrentsatvariouscurrentsperspective,thesteadyphotocurrentateachpolar-polarizationanglesareinpairs(e.g.,0°vs180°,30°vs150°,izationangleisdrawninFigure4b.Thecontinuouscurrents60°vs120°).Whenthepolarizationangleis90°,theduringthetestsimilarlydemonstratethatthesensitiveresponseisrelatedtothepolarizationangleandthattheTable1.ComparisonsofTrapDensitiesandCarrieroptimum-sensitivityanglesare90°and270°,whichverifiestheaMobilitiesofCsPbBr3sinusoidalresponseagain.Furthermore,bycomparingthecurrentdecayamplitudeandthefirstdecaytime(τ1standsfortrapdensitycarriermobility(cm−3)(cm2·V−1·s−1)refthetimefordiffusionofionstotheelectrodes)at0°and90°,10thelargerdecayamplitudeandlongerdecaytimesuggestthataCsPbBr3SC4.2×1011(SCLC)3110largerbuilt-inelectricfieldisestablishedunderthe90°CsPbBr3SC2.84×1013.6(SCLC)3310polarizationillumination.CsPbBr3SC(a)1.65×103.54(SCLC)2410ThecalculatedbandstructureoforthorhombicCsPbBr3isCsPbBr3SC(b)6.31×1011.61(SCLC)249illuminatedinFigure5a.ThebandgapiscalculatedtobeCsPbBr3SC(c)1.08×101.62(SCLC)24about2.22eV,whichisslightlylargerthantheexperimentalCsPbBr3SC143(Hall)3444valueof2.19eV.AccordingtotheliteratureandtheCsPbBr3SC10.1±0.3(TOF)359calculateddensityofstatesinFigure5b,thevalence-bandCsPbBr3SC1.9×102060(SCLC)36CsPbBr3FL1.5×1012518(SCLC)37maximum(VBM)ofCsPbBr3canberegardedasthecontributionofBr4porbitals,andtheconductionbandCsPbBr3SC1000(TOF)38minimum(CBM)ismainlydeterminedbytheinteractionofCsPbBr3SC52±1(TOF)39Pb6porbitals.Ontheotherhand,theabsorptioncoefficientisCsPbBr3FL149.2(Hall)40proportionaltotheimaginarypartoftherelativedielectricCsPbBr3SC41.3(SCLC)419function,whichreflectsthatthelightabsorptionanisotropy.CsPbBr3SC7.45×101.06(SCLC)OurworkFigure5cshowstheimaginarypartsofthepolarizeddielectricaHall,TOF,andSCLCstandforHall,time-of-flight,andspace-functionsunderilluminationbothparalleltoandperpendicularcharge-limitedcurrentmeasurements,respectively.SCandFLstandtothe[010]directions.Whenthepolarizationangleincreasesforsinglecrystalandthinfilm,respectively.from0°to90°,thedeformationoftheelectroncloud1907https://doi.org/10.1021/acs.jpclett.1c00127J.Phys.Chem.Lett.2021,12,1904−1910

4TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetterFigure4.(a)I−tcurvesofthedeviceundercontinuous0.5mWilluminationandabiasvoltageof1Vatvariouspolarizationangles.(b)Timedependenceofsteadyphotocurrentsatdifferentpolarizationanglesatabiasvoltageof5V.Figure5.(a)BandstructureoforthorhombicCsPbBr3calculatedusingtheCASTEPcodebasedonDFT.(b)Totaldensityofstates(TDOS)andBr4pandPb6ppartialdensityofstates(PDOS)oforthorhombicCsPbBr3.(c)ImaginarypartsofthepolarizeddielectricfunctionsofCsPbBr3.(d)2Delectrondensitydifferencemapinthe(101)plane.(e)Bondlengthsandanglesinthe[PbBr]6octahedron.increases,andtheenergyrequiredfortheelectrictransitioncrystal,thecompactoctahedralarrayishelpfultoenhancedecreases,resultingintheredshiftoftheabsorptionedge.Theelectronexcitationanddiffusiontowardthecrystalboundary.90°polarizationlight,showninFigure5c,exhibitsanapparentInsummary,withtheaidofGBLandDMF,thesolubilityshifttolowerenergy,correspondingtoaredshiftoftheandtemperaturesensitivityofCsPbBr3inDMSOcanbeabsorptionedge.Ontheotherhand,theelectrondensitysignificantlyimproved.Therefore,CsPbBr3singlecrystalsweresuccessfullygrownfromtheDMSO/DMF/GBLternarydifferenceofthe(101)planeshowninFigure5ddemonstratessolventsystem.Thetrapdensityofsinglecrystalsgrownbythattheelectrondensityalong90°polarizedlightislargerthan9−3thismethodisaslowas7.45×10cm.Throughthe(101)thatalong0°(equivalenttotheyaxis).Thehigherelectronplanephotodetector,thelightdetectionperformanceunderdensityhelpstoincreasetheinjection-inducedcarrierpolarizedlightwasinvestigated,anditwasfoundthattheconcentration,andtherefore,thephotoelectricresponsedetectionperformanceoftheplaneperpendiculartotheyaxisunder90°polarizedlightishigher.Measuringandcomparingwassignificantlyhigherthanthatparalleltotheyaxis.thebondlengthsandanglesinthe[PbBr]6octahedrashowedthatthe[PbBr]6octahedrarenotstrictlysymmetrical,as■ASSOCIATEDCONTENTshowninFigure5e.ThePb−Brbondlengthsinthey-axis*sıSupportingInformationdirectionareslightlyshorterthanthePb−BrbondlengthsinTheSupportingInformationisavailablefreeofchargeatthexzplane,andthus,the[PbBr]6octahedraarearrangedhttps://pubs.acs.org/doi/10.1021/acs.jpclett.1c00127.morecompactlyalongtheyaxis.Inthexzplane,theBr−Pb−Single-crystalgrowthprocess,XRDpatternsofpowdersBrangleis180°,whereasitis179.97°alongtheyaxis.and(101)planes,opticalpropertycharacterizationsAccordingtothecalculationresultsinFigure5b,theVBMand(includingUV−vis,PL,andfluorescencelifetime),CBMoftheCsPbBr3semiconductoraredeterminedbytheBrfabricationofthephotodetectors,andfirst-principles4pandPb6porbitals,respectively.IntheCsPbBr3singlecalculations(PDF)1908https://doi.org/10.1021/acs.jpclett.1c00127J.Phys.Chem.Lett.2021,12,1904−1910

5TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetter■μmDespiteTrap-LimitedTransportinHalideDoublePerovskites.AUTHORINFORMATIONACSEnergyLett.2020,5,1337−1345.CorrespondingAuthors(4)Kang,J.;Wang,L.HighDefectToleranceinLeadHalideJianxuDing−CollegeofMaterialsScienceandEngineering,PerovskiteCsPbBr3.J.Phys.Chem.Lett.2017,8,489−493.ShandongUniversityofScienceandTechnology,Qingdao(5)Snaith,H.Perovskites:TheEmergenceofaNewEraforLow266590,China;orcid.org/0000-0001-5662-2683;Cost,High-EfficiencySolarCells.J.Phys.Chem.Lett.2013,4,3623−Email:dingjianxu@sdust.edu.cn3630.TianliangZhou−CollegeofMaterials,XiamenUniversity,(6)Kim,J.Y.;Lee,J.W.;Jung,H.S.;Shin,H.;Park,N.G.High-Xiamen361005,China;Email:bible2@163.comEfficiencyPerovskiteSolarCells.Chem.Rev.2020,120,7867−7918.HuipingLi−CollegeofMaterialsScienceandEngineering,(7)Jeon,N.J.;Na,H.;Jung,E.H.;Yang,T.Y.;Lee,Y.G.;Kim,G.;ShandongUniversityofScienceandTechnology,QingdaoShin,H.W.;IlSeok,S.;Lee,J.;Seo,J.AFluorene-TerminatedHole266590,China;Email:lihuiping99@163.comTransportingMaterialforHighlyEfficientandStablePerovskiteSolarCells.Nat.Energy2018,3,682−689.Authors(8)Futscher,M.;Gangishetty,M.;Congreve,D.;Ehrler,B.KaiyuWang−CollegeofMaterialsScienceandEngineering,ManganeseDopingStabilizesPerovskiteLight-EmittingDiodesbyReducingIonMigration.ACSAppl.Electron.Mater.2020,2,1522−ShandongUniversityofScienceandTechnology,Qingdao1528.266590,China(9)Liu,Y.;Yu,Z.;Chen,S.;Park,J.;Jung,E.;Lee,S.;Kang,K.;Ko,LinJing−CollegeofMaterialsScienceandEngineering,S.;Lim,J.;Song,M.;etal.BoostingtheEfficiencyofQuasi-2DShandongUniversityofScienceandTechnology,QingdaoPerovskitesLight-EmittingDiodesbyUsingEncapsulationGrowth266590,ChinaMethod.NanoEnergy2021,80,105511.QingYao−CollegeofMaterialsScienceandEngineering,(10)Shang,Q.;Li,M.;Zhao,L.;Chen,D.;Zhang,S.;Gao,P.;Shen,ShandongUniversityofScienceandTechnology,QingdaoC.;Xing,J.;Shen,B.;Liu,X.;etal.RoleoftheExciton-Polaritonina266590,ChinaContinuous-WaveOpticallyPumpedCsPbBr3PerovskiteLaser.NanoJieZhang−CollegeofMaterialsScienceandEngineering,Lett.2020,20,6636−6643.ShandongUniversityofScienceandTechnology,Qingdao(11)Cheng,X.;Jing,L.;Zhao,Y.;Du,S.;Ding,J.;Zhou,T.Crystal266590,ChinaOrientation-DependentOptoelectronicPropertiesofMAPbCl3XiaohuaCheng−CollegeofMaterialsScienceandSingle.J.Mater.Chem.C2018,6,1579−1586.Engineering,ShandongUniversityofScienceandTechnology,(12)Maculan,G.;Sheikh,A.D.;Abdelhady,A.L.;Saidaminov,M.Qingdao266590,ChinaI.;Haque,M.A.;Murali,B.;Alarousu,E.;Mohammed,O.F.;Wu,T.;YeYuan−CollegeofMaterialsScienceandEngineering,Bakr,O.M.CH3NH3PbCl3SingleCrystals:InverseTemperatureShandongUniversityofScienceandTechnology,QingdaoCrystallizationandVisible-BlindUV-Photodetector.J.Phys.Chem.266590,ChinaLett.2015,6,3781−3786.(13)Gao,Y.;Wu,Y.;Lu,H.;Chen,C.;Liu,Y.;Bai,X.;Yang,L.;Yu,ChenyuShang−CollegeofMaterialsScienceandEngineering,W.W.;Dai,Q.;Zhang,Y.CsPbBr3PerovskiteNanoparticlesasShandongUniversityofScienceandTechnology,QingdaoAdditiveforEnvironmentallyStablePerovskiteSolarCellswith266590,China20.46%Efficiency.NanoEnergy2019,59,517−526.HaiqingSun−CollegeofMaterialsScienceandEngineering,(14)Xie,L.;Chen,L.;Nan,Z.;Lin,H.;Wang,T.;Zhan,D.;Yan,J.;ShandongUniversityofScienceandTechnology,QingdaoMao,B.;Tian,Z.UnderstandingtheCubicPhaseStabilizationand266590,ChinaCrystallizationKineticsinMixedCationsandHalidesPerovskiteWeiweiZhang−CollegeofMaterialsScienceandEngineering,SingleCrystals.J.Am.Chem.Soc.2017,139,3320−3323.ShandongUniversityofScienceandTechnology,Qingdao(15)Cheng,X.;Yuan,Y.;Jing,L.;Zhou,T.;Li,Z.;Peng,Z.;Yao,266590,ChinaQ.;Zhang,J.;Ding,J.Nucleation-ControlledGrowthofSuperiorCompletecontactinformationisavailableat:LongOrientedCsPbBr3MicrorodSingleCrystalsforHighhttps://pubs.acs.org/10.1021/acs.jpclett.1c00127DetectivityPhoto-Detectors.J.Mater.Chem.C2019,7,14188−14197.(16)He,Y.;Liu,Z.;McCall,K.M.;Lin,W.;Chung,D.;Wessels,B.NotesW.;Kanatzidis,M.G.PerovskiteCsPbBr3SingleCrystalDetectorforTheauthorsdeclarenocompetingfinancialinterest.Alpha-ParticleSpectroscopy.Nucl.Instrum.MethodsPhys.Res.,Sect.A2019,922,217−221.■ACKNOWLEDGMENTS(17)Dirin,D.N.;Cherniukh,I.;Yakunin,S.;Shynkarenko,Y.;Kovalenko,M.Solution-GrownCsPbBr3PerovskiteSingleCrystalsThisworkwasfinanciallysupportedbytheNationalNaturalforPhotonDetection.Chem.Mater.2016,28,8470−8474.ScienceFoundationofChina(52072225)andtheNational(18)Xu,Q.;Wang,X.;Zhang,H.;Shao,W.;Nie,J.;Guo,Y.;Wang,ScienceFoundationofShandongProvinceJ.;Ouyang,X.CsPbBr3SingleCrystalX-rayDetectorwithSchottky(2019GGX104009).BarrierforX-rayImagingApplication.ACSAppl.Electron.Mater.2020,2,879−884.■REFERENCES(19)Li,M.;Han,S.;Liu,Y.;Luo,J.;Hong,M.;Sun,Z.Soft(1)Kojima,A.;Teshima,K.;Shirai,Y.;Miyasaka,T.OrganometalPerovskite-TypeAntiferroelectricwithGiantElectrocaloricStrengthHalidePerovskitesasVisible-LightSensitizersforPhotovoltaicCells.nearRoomTemperature.J.Am.Chem.Soc.2020,142,20744−20751.J.Am.Chem.Soc.2009,131,6050−6051.(20)Han,S.;Liu,X.;Liu,Y.;Xu,Z.;Li,Y.;Hong,M.;Luo,J.;Sun,(2)Shi,D.;Adinolfi,V.;Comin,R.;Yuan,M.J.;Alarousu,E.;Buin,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