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通过蒸汽辅助平面异质结钙钛矿太阳能电池溶液处理（PlanarHeterojunctionPerovskiteSolarCellsviaVapor-AssistedSolutionProcess）摘要：ABSTRACT:Hybridorganic/inorganicperovskites(e.g.,CH3NH3PbI3)aslightabsorbersarepromisingplayersinthefieldofthird-generationphotovoltaics.Herewedemonstratealow-temperaturevapor-assistedsolutionprocesstoconstructpolycrystallineperovskitethinfilmswithfullsurfacecoverage,smallsurfaceroughness,andgrainsizeuptomicroscale.Solarcellsbasedontheaspreparedfilmsachievehighpowerconversionefficiencyof12.1%,sofarthehighestefficiencybasedonCH3NH3PbI3withtheplanarheterojunctionconfiguration.Thismethodprovidesasimpleapproachtoperovskitefilmpreparationandpavesthewayforhighreproducibilityoffilmsanddevices.Theunderlyingkineticandthermodynamicparametersregardingtheperovskitefilmgrowtharediscussedaswell.摘要：有机/无机杂化材料（如，CH3NH3PbI3）吸收光线是一种很有前途的球员第三代光伏领域。我们在这里演示低温蒸汽辅助溶液方法构建多晶钙钛矿薄膜表面覆盖度，表面粗糙度小晶粒尺寸微尺度。基于aspreparedfilms实现高功率转换效率的太阳能电池12.1%，到目前为止，最高效率的基础上3NH3PbI3平面异质结结构。这种方法提供了一种简单的方法制备perovskitefilm为电影和高重现性的方式装置。潜在的动力学和热力学钙钛矿薄膜生长参数讨论了。Hybridorganic/inorganicperovskitematerials(e.g.,CH3NH3PbI3)arecurrentlyamongthemostcompetitivecandidatesforabsorbermaterialsforthin-filmphotovoltaic(PV)applications.Withinthepast4years,perovskitesolarcellshavebeenreportedtoachieveremarkablyhighefficiencyof∼15%.Thereasonforthisrapidincreaseinpowerconversionefficiency(PCE)ofsuchdevicesisthatperovskitematerialspossessmostofthepropertiesrequiredtobeexcellentabsorbers:appropriatedirectbandgap,highabsorptioncoefficient,excellentcarriertransport,andapparenttoleranceofdefects.有机/无机杂化材料（例如，CH3NH3PbI3）目前最有竞争力的薄膜光伏（光伏）吸收材料的候选人应用。在过去的4年中，钙钛矿太阳能电池有据报道，∼15%实现非常高的效率。这种快速提高功率转换效率的原因Besidestheirextremelylowcostandeaseoffabrication,perovskitematerialsofferawidetunabilityoncompositionandstructurebyadjustingthemetalhalideframeworkandtheintercalatedorganicspecies.Pioneeringworksuggestedthattheseperovskitefilmsexhibitcomposition-/structure-dependentproperties,whichcanbeaccessedbyvariousprocessingapproaches.Itisessentialtoachievefinecontroloverthereactionbetweentheinorganicandorganicspecies,resultinginperovskiteswithdesiredpropertiesanddeviceperformance除了他们极低的成本和易于制造，钙钛矿材料提供通过调整和结构组成一个广泛的可调性金属卤化物框架与插层有机物种类。开创性的工作建议，这些彼罗夫裙边films展览组成/结构相关特性，可各种处理方法访问。这是必要的Althoughfirstimplementedindye-sensitizedsolarcellsbasedonmesoporousstructures,theperovskiteshavebeengraduallyfoundtoassumealloftheprincipalrolesofPVoperation,andPVdeviceswithplanararchitecturehavebeendemonstrated.Planararchitecturepotentiallyprovidesenhancedflexibilityfordeviceoptimization,multijunctionconstruction,andinvestigationoftheunderlyingdevicephysics,butitrequirestremendousefforttofabricatehigh-qualityperovskitefilms.Similartootherthin-filmPVtechnologies(e.g.,α-Si,Cu(InGa)SandCdTe),vacuumevaporationisoneofthemostpromisingtechniquestoconstructperovskitethinfilmsforplanarjunctions.Theresultingperovskitespreparedbyco-evaporationoftwoprecursors(PbCl2andCH3NH3I)exhibitsatisfactoryfilmcoverageanduniformitywithinexpectations.However,thistechniquedemandshighvacuum,whichistooenergyconsumingandhindersmassproduction.Alternatively,solution-basedtechniqueshavealsobeenproposedtofabricatethinfilms,inwhichamixtureoftwoprecursorsisusedtoformthecompletedabsorber.Duetothelackofsuitablesolventsthatcandissolvebothcomponents,andthehighreactionrateoftheperovskitecomponent,thisprocessoftenresultsinthinfilmswithpinholeformationandincompletesurfacecoverage,whichdeterioratesthefilmqualityandhampersthedeviceperformance.Asavariationtothismethod,atwostepapproachwasdemonstratedtofabricateefficientPVdevicesbydippingpreviouslydepositedinorganicprecursorfilmsintosolutionscontainingorganicspecies.Unfortunately,thismethodhasbeenlargelysuccessfulinfilmswithnanostructuredTiO2scaffoldsbutisseldomreportedtobeapplicableforfabricatingplanarheterojunctions.ConstructingaCH3NH3PbI3filmwithathicknessofseveralhundrednanometersrequireslongreactiontimesduetothelimitedreactioninterfacearea.Thetwo-stepprocessalsooftenresultsinfilmswithstrikinglyenhancedsurfaceroughnessthatfrequentlypeelofffromthesubstrate.Assuch,thereisanurgetodevelopafacilesolutionapproachtoperovskitematerialswithenhancedcontrollabilityofthefilmqualitytoconstructplanarstructureddeviceswithcompetitiveperformance.InthisCommunication,wedemonstrateuseofthevaporassistedsolutionprocess(VASP)tofabricateperovskitethinfilmsandsubsequentlyPVdeviceswithplanargeometry.Thekeystepisfilmgrowthviainsitureactionoftheas-depositedfilmofPbI2withCH3NH3Ivapor(Scheme1).Thismethodisconceptuallydifferentfromthecurrentsolutionprocessandvacuumdeposition,byavoidingco-depositionoforganicandReceived:November12,2013Published:December20,2013althoughfirst实现在染料敏化太阳电池介孔结构，钙钛矿已逐渐发现光伏发电的主要作用，和具有平面结构的光伏器件已被证明。2B，平面体系结构提供了对潜在enhancedflexibility装置的优化多结结构，和调查潜在的物理装置，但它需要巨大的为了制备出高质量perovskitefilms。类似于其他薄膜光伏技术（例如，α-Si，Cu（InGa），和CdTe），真空蒸发是最有前途的技术之一构建平面结钙钛矿薄膜。由此产生的由两个前体共蒸发法制备钙钛矿（PbCl2和甲烷3nh3i）表现出satisfactoryfilm均匀覆盖内在的期望。然而，这种技术要求很高真空，这是太耗费精力和阻碍质量生产。另外，基于解决方案的技术也提出了制备薄膜，其中混合了两前体是用来形成完整的吸收剂。由于的缺乏合适的溶剂，可以溶解这两个组件，和钙钛矿组分的高反应速率结果往往与针孔形成的和不完整的薄膜表面覆盖，影响薄膜