Colorful Perovskite Solar Cells Progress, Strategies, and Potentials - Wang et al. - 2021 - Unknown

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pubs.acs.org/JPCLPerspectiveColorfulPerovskiteSolarCells:Progress,Strategies,andPotentialsHaoWang,JiaLi,HerlinaArianitaDewi,NripanMathews,SubodhMhaisalkar,andAnnalisaBruno*CiteThis:J.Phys.Chem.Lett.2021,12,1321−1329ReadOnlineACCESSMetrics&MoreArticleRecommendationsABSTRACT:Inthepastfewyears,alargevarietyofperovskitesolarcells(PSCs)withvividandwell-distinguishedcolorhueshavebeendemonstrated.InthisPerspective,wecomparedifferentstrategiesemployedtorealizecolorfulPSCsbothinopaqueandsemitransparentdesigns.TheapproachesusedtomodulatethePSCs’colorfulappearancecanbedividedintotwomaincategories:thefirstonebasedonthemodificationsoftheirinternallayers(i.e.,absorber,electron-and/orhole-transportinglayers,andelectrodes),whilethesecondisbasedontheadditionofexternalcoloredornanostructuredfilmstothestandardPSCs.TheadvantagesandbottlenecksofeachstrategyarediscussedintermsofPSCs’colortunability,transparency,photovoltaicperformances,fabricationprocessesfeasibility,andscalability,inviewofsuitableapplicationsinanurbancontextforbuilding-integratedphotovoltaics.6olarcell(SC)integrationintourbanspacesisbeneficialtofrom3.8%to25.5%overadecade.PSCs,fabricatedbyS6−89−11bothenlargetheexploitablelandandmaximizethesolutionandlow-temperaturevacuumprocesses,are1electricityproductionclosetothepointsofdemand.High-compatiblewithflexiblesubstrates.ConventionalPSCsareperformingSCswithkeyfeaturesofsemitransparencyandopaque,althoughmanysemitransparentPSCs(ST-PSCs)havebroadcolortunabilityaredesirable.Theconventionalrigidandbeendemonstrated.12−14opaquecrystallinesiliconmodulesareintegratedonbuildingThemainrequirementsforefficientPSCintegrationinanroofsprovidinghighpowerconversionefficiencies(PCEs)andurbancontextincludethepossibilityofcolortunabilitylong-termstability,buttheiraestheticsandtheirtransparencymaintaininghighPCEs,thesimplicityandscalabilityoftherepresentthemainlimitationsforwiderintegrationinthecityfabricationprocesses,andtransparency(Scheme1).landscape.Indeed,theheavyandopaqueSi-SCscannotbePSCs’performancesandtheiraestheticpropertieshavebeenintegratedintowindowsorconformtocurvedsurfaces.ThetunedbycontrollingeitherthePSCs’internalinter-fewcoloredSimodulesdemonstratedreportedasignificativelayers1,11,15−23oraddingexternallayers24−29(Table1).InDownloadedviaBUTLERUNIVonMay15,2021at20:52:41(UTC).2,34PCEdrop.Lighterphotovoltaic(PV)technologieshavethisPerspective,wereviewthesedifferentstrategies.Wewill5emergedasalternativestoSi-SCs.Organicanddye-sensitizeddiscussthedesignprinciplestogetherwiththeadvantagesandSCsofferawiderangeofcolorandhightransparencyonrigidbottlenecksoftheseapproachesforurbanintegration,andweandflexiblesubstrates,butthelowPCEsoverlargeareasandSeehttps://pubs.acs.org/sharingguidelinesforoptionsonhowtolegitimatelysharepublishedarticles.5willprovidedesignpropositionsforcolorfulPSCs.poorstabilitylimittheirapplications.ThevarietyofcolorsachievableinPSCsisimportantforarchitecturalelements’design.TheperceptionofcolorsisThemainPSCs’requirementsforcreatedbymodulatingeitherthelighttransmittance(Schemetheirproficientintegrationin2A)orreflectance(Scheme2B)throughthePSCs.TheurbancontextsincludewidedesignsfortuningthePSCs’colorsbothintransmissionandreflectioncanbebasedoneither(i)internalor(ii)externalcolortunability,highPCEs,sim-modificationsofthePSCsstructure(Scheme2C).InternalplicityandscalabilityofthemodificationsincludetheapproachesbasedonthevariationoffabricationprocessesandhighthePSCsinternallayersastheperovskitelayer,theelectronopticaltransparency.Received:November19,2020Thehighlyefficient,cost-effective,andversatilemetalhalideAccepted:January15,2021perovskitesolarcells(PSCs)representapromisingPVPublished:January27,2021technologywiththepotentialtobeimplementedinurbansettings.Theypresentexcellentbandgaptunability(1.2−2.3eV)andhighabsorption.ThePSCs’PCEshaveskyrocketed©2021AmericanChemicalSocietyhttps://dx.doi.org/10.1021/acs.jpclett.0c034451321J.Phys.Chem.Lett.2021,12,1321−1329

1TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLPerspectiveaScheme1.KeyPropertiesofColorfulPerovskiteSolarCellsScheme2.ColorfulPSCSchematicStructuresandDesignaforIntegrationinUrbanContextsa(i)Widecolortunability,(ii)highpowerconversionefficiency,(iii)easyandlow-temperatureprocessing,(iv)scalability,and(v)transparencywhenrequiredforspecificapplications.transportlayer(ETL),holetransportlayers(HTL),ortheelectrodes.Incontrast,externalmodificationstrategiesmodifythePSCs’colorsbyaddingcoatingsordielectricmirrors.aThecolorfulappearanceisgeneratedbymodulatingtheincidentThereisanunavoidabletrade-offbetweentheaestheticlightin(A)transmissionmodeand(B)reflectionmode.(C)Designpropertiesandlight-harvestinginPSCs.approachestocreatecoloredPSCs.AstraightforwardwaytotunethePSCs’colorsisbymodifyingtheperovskitecoloreitherbycompositional33−3530engineeringorthroughtuningthefilmthickness.Bothdoesnotrequireadditionalprocessing,butthecolortunabilityPb-basedandlead-freeperovskitehavesimilarcolorpropertiesislimitedandthedifferentcolorsachievedifferentPCEs.asthecolorgenerationdependsonthebandgapratherthanUpamaetal.fabricatedPSCsintheshadesofbrownandPCEs36elementalcomposition.Yuanetal.demonstratedPSCsfrom3.5%to9.23%,forperovskitethicknessesbetween40and30exhibitingcolorsfromdarktolightredtuningthebandgapof100nm.Jungetal.showedPSCsofdifferentgradesofbrownMAPbI3−xBrx,yieldingPCEsrangingfrom14.15%toandPCEsbetween7.53%and10.73%employing140−240nm153110.03%.thickCH3NH3PbI3film(Figure1A).SimulationsbyQuirozPSCswithyellowtoredcolorshavebeendemonstratedetal.alsopredictedthedependenceofthePSCcolorsonthe30,3137throughtuningperovskitethickness.Thissimplemethodperovskitethickness.aTable1.ColorfulOpaquePSCandST-PSCCharacteristicsPCE(%)layermodifiedmethodadvantagesconstraintsopaqueST3031perovskiteperovskitebandgaporsimplefabrication;scalablelimitedcolortunability;thinabsorber3.5−9.23,7.53−10.73thicknesstuningprocessrequired;limitedPCE23perovskitemorphologydistinctivevividcolorfulcolorsarenotreproducible;strictprocess12.2%controlpatterncontrolrequirements17ETL/HTLpost-tintingsimplefabrication;scalablecolorsdependondyeavailability6.516nanostructureswidecolortunabilitysophisticateddesign;nanostructure19.6%fabrication1photoniccrystalwidecolortunabilitysophisticateddesign4.5−8.8%,3216.94%1819electrodemicrocavityincorporationwidecolortunabilityrequiresultrathinabsorber;limitedPCE;3.18−3.86,5.7−7.2,20sophisticateddesign10.47−11.182111electrodethicknesstuningwidecolortunability;11.6−13.8,15.1−16.8,22simplefabrication10.6−13.3262425externalmicrocavitiestuningwidecolortunability;requireultrathinabsorber;limitedPCE;18−18.9%3−3.610.2layersfabrication;scalablesophisticateddesign2728colorfulcoatingadditionsimplefabrication;scalablecolorsdependonpigment/inkavailability9.4%N.A.29plasmonicnanogratingwidecolortunabilitysophisticateddesign7.72−10.12additionaMethodsusedtotunethecolorfulappearanceandtheirrelativeadvantagesandconstraintstogetherwiththePCEs.1322https://dx.doi.org/10.1021/acs.jpclett.0c03445J.Phys.Chem.Lett.2021,12,1321−1329

2TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLPerspectiveFigure1.ColoredPSCsobtainedbymodulatingtheperovskiteactivelayer.(A)Left:DevicestructureofST-PSCsconsistingofglass/FTO/PEDOTorCuSCN/CH3NH3PbI3/PC61BM/Bis-C60/Ag.Middle:Devicephotographswithperovskitelayerofdifferentthickness.Right:PSCcolorcoordinatesonCIE1931chromaticitydiagram.Reprintedfromref31.Copyright2015Wiley-VCHVerlagGmbH&Co.KGaA.(B)Left:DevicestructureschematicofthecoloredopaquePSCs:consistingofglass/ITO/PTAA/perovskite/C60/BCP/Al.Middle:Microscopyimagesoftheas-preparedperovskitefilmspreparedatsubstratetemperature160,135,and100°C.Right:Photographsoftheperovskitefilm(left)andthecompletePSC(right).Reprintedfromref23.Copyright2015TheRoyalSocietyofChemistry.TheperovskitemorphologyalsoaffectsthePSCs’colors.coloredPSCs.Zhangetal.demonstratedopaquePSCswithEperonetal.demonstratedneutral-coloredPSCswithdistinctivecolorsbyincorporatingaporousphotoniccrystal17,38microstructured“islands”intheperovskite.Dengetal.(TiO2−SiO2nanoparticlesalternatedlayers)withinthefabricatedPSCswithvividnonhomogeneouscolorsbyformingphotoactivelayer,Figure2C.Thecolors,generatedinacoffee-ring-likephotonicstructures(bycontrollingtheperov-reflectionmode,covertheentirevisibleregion.ThePSCs1skitemorphology)duringdoctor-bladedeposition(FigureachievedPCEsof4.5%fortheredand8.8%fortheblue.The231B).Thedoctor-bladedcolorfulPSCsareeasilyscalable.keyadvantagesofthisapproacharethehighreproducibilityThealterationofETLand/orHTLbytintingorthicknessandthewidecolortunabilityachievablewithhuesthatarevariationornanostructuresincorporationisanotherinternalunlikelytobleachorfadewithtime.Themainlimitationofthemodificationapproach.photoniccrystaldesignisrelatedtothefabricationcomplexityEperonetal.demonstrated“rose-tinted”PSCsbyincorpo-aseachSiO2andTiO2layerneedstobewellcontrolledtonotratingdyeintheHTL,withoutaffectingthePCE(Figurecompromisethehinderingofchargetransportorthecolor172A).Thisisapromisingmethodforgoodreproducibilityandgeneration.Moreover,thetotalPSCfabricationprocesstimescalabilitywithoutsacrificingthePCEs.Thecolortunabilitybecomessignificantlylonger,andthespin-coatingpreparationconstraintsaredefinedbythedye’scolors.Wangetal.reportedprocessofthephotoniccrystalsmayrestrictthePSCs’opticalsimulationsforn-i-pPSCsshowingthatdistinctivescalability.22colorscanbeobtainedbyvaryingtheHTLthickness.Liuetal.designedanETLwithtwo-dimensionalphotonicDengetal.demonstratedcolorfulPSCsbyincorporatingincrystalstructuresconsistingofanopalstructuredSnO2−TiO2theETLdoublediffractiongratings,whichincludesa(IOST)compositefabricatedusingatemplate-assistedspin-nanostructuredTiO2scaffoldandastructuredPDMSfilmascoatingmethodbasedon550nmpolystyrene(PS)micro-39antireflectionlayer(Figure2B).Thisapproachgeneratedvividspheresasthepatternedmedium.TheIOSTlayerscoated16colorsandenhancedthePCEsfrom18.2%to19.6%.Indeed,withaperovskitefilmexhibitdifferentcolorsatvariousviewingthestructuredETLdidnotaffectthePSCs’performance,whileangles.ThePSCsachived16.8%PCE;however,thefinalthetexturedPDMSenhancedthelight-harvesting.AsthecolorcolorsgeneratedcanbeaffectedbythepresenceoftheHTLformationisinreflectivemode,thisapproachissuitablealsoandtopelectrode.Wangetal.nanostructuredtheETLlayersforST-PSCs.ThebottleneckisthereproducibilityandwithTiO2nanobowl(NB)arraysfabricatedbylithography32scalabilityofthepatternedETLfilmfabricatedbytheusingPSspheresasthepatternedmedium.Theperovskiteimprintingprocess.ThedesignofthediffractiongratinginfiltratedintheTiO2NBarrayshowedvividcolorsdependentwithintheETLisaneffectivewaytomodulatethecolorsofontheviewingangles.ThecolorfulPSCsreachedPCEofPSCs.16.94%.TheincorporationofphotoniccrystalsinETLhasalsobeenBesidesthenanostructuresandphotoniccrystalsdiscusseddemonstratedtobeanefficientstrategytocreatebright-here,othernanophotonicsdesignscouldalsobeexploredto1323https://dx.doi.org/10.1021/acs.jpclett.0c03445J.Phys.Chem.Lett.2021,12,1321−1329

3TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLPerspectiveFigure2.ColoredperovskitesolarcellswereobtainedbymodulatingtheETL/HTLlayers.(A)Left:ST-PSCsdevicestructureconsistingofglass/FTO/c-TiO2/perovskiteislands/Spiro-OMeTAD/thinAu.Middle:PhotographsofST-PSCswithout(left)andwith(right)D102dyeincorporatedintheSpiro-OMeTADlayer.Right:J−Vcurvesofthecolor-tintedST-PSCandcontrolPSCs.Reprintedfromref17.Copyright2013AmericanChemicalSociety(ACS).(B)Left:Fabricationprocessofgrating-patternedPDMSandtheTiO2scaffold,anddevicestructureofPSCswithflat,grating-TiO2,gratingTiO2+gratingPDMSconfiguration.Middle:PSCsJ−Vcurves.Right:PhotographsofthecolorfulPSCs(flatTiO2andgratingTiO2+gratingPDMS).Reprintedfromref16.Copyright2019Wiley-VCHVerlagGmbH&Co.KGaA.(C)Left:Devicestructureandphotographsofthecolorfulphotonic-crystal(PC)-basedopaquePSCconsistingofglass/FTO/TiO2−SiO2NPsalternatedlayers/CH3NH3PbI3−xClx/Spiro-OMeTAD/Au.Middle:Experimental(solidlines)andtheoretical(dashedlines)reflectanceofthecolorfulPSCs.Right:PSCcolorsCIE1931Chromaticityspace.Reprintedfromref1.Copyright2015ACS.formcolorfulPSCs.ThesimplicityandscalabilityofthewheretheopticaldielectricspacerWO3istunedtocreatenanophotonicstructure’sfabricationproceduresareimportantdifferentcolors.Thethinperovskiteabsorberemployed(∼8018factorsfortheirpracticalimplementation.nm)leadstolowlightabsorptionlimitingthePCEsto∼3%.Luetal.employedAg/ITO/AgmicrocavityastransparentThesimplicityandscalabilityofelectrodestocreatered,orange,yellow,green,andblueST-PSCs,bytuningtheITOopticalspacerthickness(Figure3A).thenanophotonicstructure’sThePSCsachievedrelativelylowPCEsrangingfrom5.7%tofabricationproceduresareim-197.2%becauseofthelimitedlightabsorptionintheultrathinportantfactorsfortheirpracticalperovskite.Leeetal.developedefficientmulticoloredST-PSCsimplementation.basedonphase-compensatedmicrocavities,Ag/SiO2/ZnS/Ag/ZnS,showinghighangularincidencetolerance.ThePSCsefficientlyutilizemostofthevisiblelight,throughimpedanceAnotherinternalmodificationapproachtotunethecolorsofmatching,providinghighlightharvesting.Witha∼100nm-thePSCsisbasedondesigningtransparentelectrodestothickperovskiteabsorber,PCEabove10%wasachievedfor20modulatethetransmissionorreflectionspectralpeaks.red,green,andblueST-PSCs.Recently,afewworkshaveshownthatawiderangeofcolorTheincorporationofopticalmicrocavitiesinthetransparent11,21,22electroderequiresultrathinperovskite(<100nm)absorber,huescanbeachievedwithoutsacrificingthePCEs.Leeetal.demonstratedthattheincorporationofopticalwhichcompromisesthePCE.microcavitiesinthetransparentelectrodesgeneratesdistinctiveTuningthetransparentelectrodethicknessisasimpleandtransmissivecolorsbycreatinglightinterferenceatspecificeffectiveapproachtocreatecolorswithoutrequiringextra18wavelengths.Thetransparentelectrodeisametal−fabrication.ThePSCs’colortuninghasbeendemonstratedindielectric−metalstructure(PTCBI/Ag/WO3/PTCBI/Ag)areflectivemode,whichhasnoconstraintsontheperovskite1324https://dx.doi.org/10.1021/acs.jpclett.0c03445J.Phys.Chem.Lett.2021,12,1321−1329

4TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLPerspectiveFigure3.ColoredPSCsobtainedbymodulatingthesemitransparentelectrodes.(A)Left:ColoredST-PSCconsistingofglass/ITO/PEDOT:PSS/perovskite(75nm)/PCBM/thinAg/ITO/thinAg.ThemicrocavityiscreatedbysandwichingtheITObetweentwothinmetallicAglayers.Middle:ST-PSCsSimulated(dashedlines)andexperimental(solidlines)transmittancecurves.Right:PhotographsofthecolorfulPSCs.Reprintedfromref19.Copyright2016ACS.(B)Left:DevicestructureofcoloredST-PSC.Middle:Photographsofacoloredschematic“H”assembledbycolorfulPSCs.Right:PSCcolorcoordinatesintheCIEdiagram.Reprintedfromref21.Copyright2016ACS.(C)Left:ColorfulST-PSC(glass/FTO/SnO2/PCBM/CH3NH3PbI3/Spiro-OMeTAD/Ag/ITO).Middle:PCEsandphotographsofthecoloredST-PSCsasafunctionoftheITOthicknesses.Right:PSCcolorcoordinatesintheCIEdiagram.Reprintedfromref11.Copyright2020ElsevierInc.(D)Left:SchematicofcolorfulST-PSC.Middle:PhotographsofcolorfulPSCwithdifferentITOelectrodethickness.Right:PSCcolorcoordinatesintheCIEdiagram.Reprintedfromref22.Copyright2019ACS.thickness.Jiangetal.reportedcolorfulST-PSCbyemployingLietal.reportedST-PSCswithdistinctivecolorsbytuningtransfer-printedPEDOT:PSSasatransparentelectrodethethicknessofthesputteredITOandPCEsrangingfrom11(Figure3B).Transparencyandthicknessweretunedto15%to16.8%(Figure3C).ThesecolorfulST-PSCsshowedgoodscalabilityoverlargeareasbyemployingcoevaporatedengineertheopticalinterference.DistinctivecolorsandPCEsperovskite,andcoloredSTmini-modules(14cm2)achieved21between11.6%and13.8%wereobtained.Themain11PCEsabove11%.limitationofthismethodistheST-PSCscalability,astheWangetal.reportedST-PSCswiththehighlytransparenttransfer-printingmethodisnoteasilytransferableoverlargeCuSCNasHTLinwhichtheITOthicknesswastunedto22areas.achievecolors(Figure3D).Distinctivevividcolorswere1325https://dx.doi.org/10.1021/acs.jpclett.0c03445J.Phys.Chem.Lett.2021,12,1321−1329

5TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLPerspectiveFigure4.ColoredPSCsobtainedbytheadditionofexternallayers.(A)Left:ST-PSCschematicconsistingofglass/ITO/PEDOT:PSS/perovskite/PCBM/ZnO/AgNWwithadielectricmirrorattherearside.Middle:PSCsbackandfrontimageswitha∼40nmthickperovskiteasabsorberlayer,fourbaredielectricmirrors.Right:ChromaticityofapristinePSCs.Reprintedfromref24.Copyright2016ACS.(B)Left:Diagramofthenarrow-bandwidthreflectivefilters(NBRF)formedbyperiodicstackingofhigh-refractive-index(TiO2)andlow-refractive-index(SiO2)layers.Middle:ReflectivespectraandimagesofthefabricatedRGB-NBRFs.Right:ColorcoordinatesoffabricatedandsimulatedRGB-NBRFsinCIEcolorcoordinatediagram.Reprintedfromref26.Copyright2019ACS.(C)Left:Schematicofaninkjet-printedluminescentdown-shifting(LDS)layercoatedonthesubstratesideofaPSC.Middle:TransmittancespectraofLDSlayers.Right:ColorcoordinatesoftheLDS,perovskitelayers,andcombinationofLDSandperovskiteinCIE-diagram.Inset:PhotographsofPSC.Reprintedfromref27.Copyright2018ACS.(D)Left:PSCschematicwithatopplasmoniccolorfilter.Middle:J−VcharacteristicsofthePSCsintegratedwiththeRGBplasmonicfilters.Right:ColoredPSCsincidentphoton-to-currentefficiency(IPCE)spectra.Reprintedfromref29.Copyright2017TheAuthors(openaccess).theoreticallypredictedandexperimentallydemonstratedbyelectrodecombinationenabledtheST-PSCstoachieveatuningtheITOthickness.ThehighlytransparentHTL/bifacialfactorof∼93.7%andbifacialPCEof22.1%.1326https://dx.doi.org/10.1021/acs.jpclett.0c03445J.Phys.Chem.Lett.2021,12,1321−1329

6TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLPerspectiveAsanexternalmodification,theadditionofdielectricmirrorsofcurvysurfaces,flexible,colorfulPSCsarerequired,andtheorcolorfulcoatingsinPSCsisastraightforwardmethodforfabricationprocessesbecomecritical.Besidesthesespecificcreatingcolors.However,itmayaffectthelightabsorptionandrequirements,thePSCs’scalability,reproducibility,andthePVperformance.stabilityareimportanttomakePSCscost-effectiveandsuitableQuirozetal.demonstratedthatmicrocavityintegrationinforurbanintegration.25ST-PSCimprovedlightharvesting.Thedoctor-bladedInconclusion,effectiveapproachestorealizeopaqueandSTdielectricmirrorswereplacedunderneaththeST-PSCsservingPSCswithdistinctcolorsandreasonablePCEscanbeasabacksidereflector.Themirrorscreatemultiple-coloredST-categorizedbymethodbasedonthemodificationsofinternalPSCandenhancetheirharvestedlight.ThePSCcolorisorexternalPSClayers.ThemainchallengetowardthePSCgeneratedinacombinationoftransmissiveandreflectiveimplementationininfrastructureisreachingcolortunabilityatmodes.PCEsaround3%weredemonstrated(Figure4A).littlecostofthePCE.Yooetal.investigatedtheuseofnarrow-bandwidthreflectiveAmongthedesignsbasedoninternalmodifications,tuningfilters(NBRFs)onthefrontoftheITO/glasstotunethethetransparentelectrodethicknessmightbethesimplest,mostPSCs’colors.NBRFsareformedbyhigh-indexTiO2/low-indexSiO2multinanolayers(Figure4B).PCEsof18.0%,Amongthedesignsbasedon18.6%,and18.9%wereachievedforred,green,andblueinternalmodifications,tuningthe26PSCs.ThesePCEsare2%lowerthanthenoncolorfulPSCbecauseofthereducedlightabsorptionwhereahighreflectiontransparentelectrodethicknesspeakiscreated.ThispromisingstrategyforcolorfulPSCscanmightbethesimplest,mostalsobetransferredtoST-PSCs.favorable,andeffectivewaytoThesimpledepositionofacolorfulcoatingontopofthetunethePSCscolorwithoutsurfaceofST-PSChasbeendemonstratedtobeeffectivetotunePSCcolors.Schlisskeetal.reportedthecoloringofPSCsadditionalfabricationprocesses.bydepositingluminescentdown-shifting(LDS)layersontheir27frontsurface(Figure4C).TheLDSprecursorswerefavorable,andeffectivewaytotunethePSCscolorwithoutpreparedbyinkjetprintingpoly(methylmethacrylate)additionalfabricationprocesses.ForthesePSCs,highly(PMMA)mixedwithdyes(Violet570,Yellow083,andRedtransparentelectrodesandcharge-transportinglayersare300Lumogen-Fseries)onaglasssubstrate.WithLDSthecrucialtomaximizePCEsanddistinctivecolorssimulta-PSCsdemonstratedwell-definedcolorsandreporteda17%neously.ThetransparentelectrodedepositioniscriticalforthereductionofPCE.Thered-coloredPSCsachievedthehighestPSCscalability,andsputteredTCOsaremorefavorablethanPCEof9.4%.thesolution-processedconductivepolymers.Guoetal.provedcoloredST-PSCs(PCEof5.36%)byspin-Amongthedesignsbasedonexternalmodifications,the28coatingpigmentsonthethin-AuSTelectrode.Leeetal.additionofcolorfulcoatingsisapromisingapproach,astheirdemonstratedthatasubwavelengthplasmonicnanoresonatorintegrationminimallyimpactsthePSCs’electronicproperties,29canbeintegratedontheglasstomodulatethePSCscolors.andthemainconstraintistheavailabilityofefficientandThegratingisanarrayofultrathinmetallicsubwavelengthtransparentdyestomodifythePSCs’colors.nanowiresfabricatedbynanoimprintlithography.ThePSCsexhibitangle-independent(upto60°)red,green,andblue■AUTHORINFORMATIONcolorsandPCEsof10.12%,8.17%,and7.72%,respectivelyCorrespondingAuthor29(Figure4D).AnnalisaBruno−EnergyResearchInstitute@NTU(ERI@TheexternalmodificationsleadtominimallimitationsontheN),NanyangTechnologicalUniversity,Singapore637553;reproducibility,fabrication,andstabilityofthePSCsorST-orcid.org/0000-0002-6963-1682;Email:Annalisa@PSCs.ThemainlimitationofthisapproachisthePSCs’ntu.edu.sgvariationofthelightabsorptionduetotheadditionalcoating.Accordingly,thecolorcoatingtransparencyandthelight-AuthorsharvestingreductioninPSCsneedtobeevaluatedfordifferentHaoWang−EnergyResearchInstitute@NTU(ERI@N),applications.NanyangTechnologicalUniversity,Singapore637553;ColorfulSCsareextremelyattractivearchitecturalsolutionsorcid.org/0000-0003-0037-4523becauseoftheirabilitytoaddthefunctionalityofconvertingJiaLi−EnergyResearchInstitute@NTU(ERI@N),solarenergyintoelectricityinareasthatcouldnotbeexploitedNanyangTechnologicalUniversity,Singapore637553otherwise.ThedesignconsiderationsforcolorfulPSCsmustHerlinaArianitaDewi−EnergyResearchInstitute@NTUincludetheapplication’sutility,location,andorientation(ERI@N),NanyangTechnologicalUniversity,SingaporetogetherwithPCEandtransparencyrequirementsforspecific637553applications.Forexample,ifthePSCsareintegratedasNripanMathews−EnergyResearchInstitute@NTU(ERI@windowsorskylights,thevisibletransparencyofthedevicewillN),NanyangTechnologicalUniversity,Singapore637553;determinetheamountofsunlightpenetratingthebuilding.ASchoolofMaterialsScience&Engineering,NanyangTechnologicalUniversity,Singapore639798;orcid.org/balanceamongPCEs,visiblecomfort,andaestheticappear-0000-0001-5234-0822anceneedstobeconsidered.DesignapproachesincludingSubodhMhaisalkar−EnergyResearchInstitute@NTUultrathinST-PSCs,generatingcolorsinthetransmissivemode,(ERI@N),NanyangTechnologicalUniversity,Singaporewillbeverysuitableforthisapplication.Incontrast,PSCscan637553;orcid.org/0000-0002-9895-2426beintegratedintobuildingfacadesasacontinuousbuildingenvelope.Inthiscase,hightransparencyisnotessentialwhileCompletecontactinformationisavailableat:highPCEanddistinctivecolorsbecomeessential.Inthecasehttps://pubs.acs.org/10.1021/acs.jpclett.0c034451327https://dx.doi.org/10.1021/acs.jpclett.0c03445J.Phys.Chem.Lett.2021,12,1321−1329

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