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Solution-Processed Highly Conductive PEDOTPSS/AgNW/GOTransparent Film for E cient Organic-Si Hybrid Solar CellsQiaojing Xu, Tao Song,* Wei Cui, YuqiangLiu, WeidongXu, Shuit-TongLee,and BaoquanSun*JiangsuKey Laboratoryfor Carbon-BasedFunctionalMaterials silvergrid electrode;andpristine AgNW TCE with aconcentrationof 3.5 mg/mL. The short-circuitcurrent densityJsc, the open-circuitvoltageVoc, the ll factor FF, andthePCE of solarcellswith dierenttop anodesaresummarizedinTable 1 and Table S2 in the Supporting Information. Thedevicesbasedon PEDOTPSS/AgNW/GO TCEs showhigherPCE than those based on either conventionalAg grids orPEDOTPSS/AgNW TCEs without GO. With the GO layer,the PCEof the hybrid devicesis enhancedfrom ~ 11 to ~ 12on average.In particular,the FF is signicantly improved byintegrationof GO becauseof reducedseriesresistanceof thedevicesTable 1 andTableS2in the SupportingInformation.Seriesresistancewasextractedfrom slopeof J- V curvesat J 0.40 Seriesresistanceof the deviceswith PEDOTPSS/AgNW/GO TCEs is much lower than that of the devicewithout GOand the Ag grids device. Seriesresistanceof solar cells isinuencedby the lateralRs aswell asthe contactresistance.41Lateral resistanceof PEDOTPSS lms was reducedby thepercolatedAgNW networks.Meanwhile,contact resistanceofthe “ sandwich” structure of PEDOTPSS/AgNW/GO is lowbecauseof the strong electrostaticadhesionbetween hydro-philic PEDOTPSSand GO.By analyzingthe device performance,we found that GOtendedto takea more prominentrole in the sparsedistributedAgNW network than the denselypackedone.Specically,forthe GO-covereddevicefabricatedfrom 1.5 mg/mL AgNWs,the FF and the PCE were improved by 12.2 and 11.8,respectively.While for the GO-covereddevice with a higherAgNW concentrationof 5 mg/mL, the correspondingFF andthe PCE wereslightly increasedby 5.4 and 3.4,respectively.This phenomenoncanbeexplainedasfollowsdueto the loosemorphology of the AgNW mesh, the sparseAgNW networkcannot provide enough conducting paths to deliver chargecarriersgeneratedby light; it could be readilycompensatedbyincreasingthe amount of contactingjunctionsand decreasingthe junction resistancein AgNW network by the GO sheetscoating.For the denseAgNW network, the Rs is alreadyverylow and the space for further improvementsby the GOcoverageis ratherlimited. Asa resultof abalancebetweenlightabsorptionand chargecarriercollection,a remarkablePCE of13.3with a Jsc of 28.4mA/cm2, a Voc of 0.601V, anda FF of78.4wasachievedemployingthe PEDOTPSS/AgNW/GOcompositeTCEs with a AgNW suspensionconcentrationof 3.5mg/mL. It is worth noting that thisresultis alsoconsistentwiththe maximum Φ TC value of the PEDOTPSS/AgNW/GOcomposite TCEs fabricated from 3.5 mg/mL AgNWconcentration. The reference device based on the PE-DOTPSS/AgNW TCE with the sameAgNW concentrationexhibiteda lower PCE of 11.6with a Jsc of 28.3 mA/cm2, aVoc of 0.579 V and a FF of 70.9,which may be partiallycausedby the largeroughnessof thepristine AgNW mesh.Theperformanceof the referencedeviceswas consistentwith thepreviousresultswhere nanostructuredsilicon substrateswereemployed as photoactive layers and PEDOTPSS/AgNWsacted as TCEs.8 We believethat the higher e ciency of thehybrid solarcell basedon PEDOTPSS/AgNW/GO compositeTCE can be attributed to the more e cient chargecarriercollection and transfer, wherein the AgNW networks wereeectivelyweldedby GO nanosheets.Though electrical conductivity has been improved usingcompositeelectrodewith and without GO coverage,similarJscwasobtainedfor those two typesof devices.Accordingto theEQE spectraof hybrid solar cells as shown in Figure 3c, thecalculatedJsc was27.8and 27.7mA/cm2 for the deviceswithPEDOTPSS/AgNWelectrodesandPEDOTPSS/AgNW/GOcompositeelectrodes,respectively.The integratedJsc valuesarein good accordance with those extracted from the J- Vcharacteristics.EQE spectraare closely correlatedwith bothoptical and electricalcharacteristicsof the solar cells,suchaslight trapping and electrode conductivity, as well as chargeseparationandtransferin the devices.As shownin FigureS2din the SupportingInformation,reectanceis almostthe samefor the PEDOTPSS/AgNW lms with or without GO,indicating that light reection is not the main reasonfor PVperformancedierence.On the other hand,we comparedlighttransmittance of the PEDOTPSS/AgNW lms and thePEDOTPSS/AgNW/GO ones, as shown in Figure S2c inthe SupportingInformation.This analysisconrmsthat for thedeviceswith PEDOTPSS/AgNW/GO composite TCEs, theslightdecreaseof EQE at the wavelengthsshorterthan600nmis causedby the light absorptionof GO. The improvementatlonger wavelengthsis ascribedto enhancedchargetransportand collection in the GO-coveredTCEs. Finally, almost thesamephotocurrentsareachievedin the both cases.In addition, the Voc of the hybrid solar cells withPEDOTPSS/AgNWelectrodesis slightly improvedwith GOcoating.We speculatedthat PEDOTPSSWF wasrelatedwithFigure 4. a Surfacepotential prole of the PEDOTPSSlm with left part and without right part GO. b 1/ C2- V plots of the hybrid solarcells basedon AgNW and AgNW/GO TCEs with 3.5 mg/mL AgNWs.ACS Applied Materials Nowlan, M. J. CrystallineSilicon PhotovoltaicstheHurdle for Thin Films. Prog.Photovolt.Res.Appl. 1997, 5, 309- 315.2 Fthenakis,V. M.; Kim, H. C. PhotovoltaicsLife-Cycle Analyses.Sol.Energy2011, 85, 1609- 1628.3 Chen, T. G.; Huang, B. Y.; Chen, E. C.; Yu, P.; Meng, H. F.Micro-Textured Conductive Polymer/Silicon Heterojunction Photo-voltaic Devices with High Efficiency. Appl. Phys.Lett. 2012, 101,033301.4 Avasthi,S.; Lee,S.;Loo, Y. L.; Sturm, J.C. Role of Majority andMinority Carrier Barriers Silicon/Organic Hybrid HeterojunctionSolar Cells. Adv. Mater.2011, 23, 5762- 5766.5 He, L.; Jiang,C.; Wang,H.; Lai, D. Rusli.High EfficiencyPlanarSi/Organic Heterojunction Hybrid Solar Cells.Appl. Phys.Lett. 2012,100, 073503.6 Zhang,F.; Sun,B.; Song,T.; Zhu, X.; Lee,S.Air Stable,EfficientHybrid Photovoltaic Devices Basedon Poly3-hexylthiophene andSilicon Nanostructures.Chem.Mater. 2011, 23, 2084- 2090.7 Shiu, S.-C.; Chao, J.-J.; Hung, S.-C.; Yeh, C.-L.; Lin, C.-F.Morphology Dependence of Silicon Nanowire/Poly3,4-ethylenedioxythiophenePolystyrenesulfonateHeterojunction SolarCells. Chem.Mater. 2010, 22, 3108- 3113.8 Chen, T. G.; Huang, B. Y.; Liu, H. W.; Huang, Y. Y.; Pan,H. T.;Meng, H. F.; Yu, P. Flexible Silver Nanowire Meshes for High-efficiency Microtextured Organic-Silicon Hybrid Photovoltaics. ACSAppl. Mater. Interfaces2012, 4, 6857- 6864.9 Liu, Q.; Ono, M.; Tang, Z.; Ishikawa, R.; Ueno, K.; Shirai, H.Highly Efficient Crystalline Silicon/Zonyl Fluorosurfactant-TreatedOrganic Heterojunction Solar Cells. Appl. Phys. Lett. 2012, 100,183901.10 Jeong,S.;Garnett, E. C.; Wang, S.;Yu,Z.; Fan,S.; Brongersma,M. L.; McGehee,M. D.; Cui, Y. Hybrid Silicon Nanocone-PolymerSolar Cells. Nano Lett. 2012, 12, 2971- 2976.11 Yu, P.; Tsai, C.-Y.; Chang,J.-K.;Lai, C.-C.; Chen, P.-H.; Lai, Y.-C.; Tsai, P.-T.; Li, M.-C.; Pan,H.-T.; Huang, Y.-Y.;Wu, C.-I.; Chueh,Y.-L.; Chen, S.-W.; Du, C.-H.; Horng, S.-F.; Meng, H.-F. 13Efficiency Hybrid Organic/Silicon-Nanowire Heterojunction SolarCell via Interface Engineering.ACS Nano 2013, 7, 10780- 10787.12 Liu, R.; Lee,S. T.; Sun, B. 13.8EfficiencyHybrid Si/OrganicHeterojunction Solar Cells with MoO 3 Film as Antireflection andInversion Induced Layer. Adv. Mater. 2014, 26, 6007- 6012.13 Liu, Z.; Wang,H.; Fung,M.-K.; Lee, C.-S.;Zhang, X.-H. Low-Cost Solar Cell Basedon a Composite of Silicon Nanowires and aHighly ConductiveNonphotoactive Polymer.Chem. Eur. J.2013, 19,17273- 17276.14 Pudasaini,P. R.; Ruiz-Zepeda,F.; Sharma,M.; Elam,D.; Ponce,A.; Ayon, A. A. High Efficiency Hybrid Silicon Nanopillar-PolymerSolar Cells.ACS Appl. Mater.Interfaces2013, 5, 9620- 9627.15 Liu, Q.; Khatri, I.; Ishikawa,R.; Fujimori, A.; Ueno, K.; Manabe,K.; Nishino, H.; Shirai, H. Improved Photovoltaic PerformanceofCrystalline-Si/Organic Schottky Junction Solar Cells Using Ferro-electric Polymers.Appl. Phys.Lett. 2013, 103, 163503.16 Wu, Z.; Chen, Z.; Du, X.; Logan,J. M.; Sippel,J.;Nikolou, M.;Kamaras,K.; Reynolds,J. R.; Tanner, D. B.; Hebard,A. F.; Rinzler,A.G. Transparent, Conductive Carbon Nanotube Films. Science2004,305, 1273- 1276.17 Ham, H. T.; Choi, Y. S.; Chee,M. G.; Cha, M. H.; Chung, I. J.PEDOT-PSS/SinglewallCarbon Nanotubes Composites.Polym.Eng.Sci.2008, 48, 1- 10.18 Matyba, P.; Yamaguchi,H.; Chhowalla, M.; Robinson, N. D.;Edman, L. Flexible and Metal-Free Light-Emitting ElectrochemicalCells Basedon GrapheneandPEDOT-PSSasthe ElectrodeMaterials.ACS Nano 2010, 5, 574- 580.19 Hong, W.; Xu, Y.; Lu, G.; Li, C.; Shi,G. TransparentGraphene/PEDOT- PSS Composite Films as Counter Electrodes of Dye-SensitizedSolarCells. Electrochem.Commun.2008, 10, 1555- 1558.20 Lee, J.-Y.; Connor, S. T.; Cui, Y.; Peumans, P. Solution-ProcessedMetal Nanowire Mesh Transparent Electrodes.Nano Lett.2008, 8, 689- 692.21 Gaynor, W.; Lee, J.-Y.; Peumans,P. Fully Solution-ProcessedInverted Polymer Solar Cells with Laminated Nanowire Electrodes.ACS Nano 2009, 4, 30- 34.22 Krantz, J.;Stubhan,T.; Richter,M.; Spallek,S.;Litzov, I.; Matt,G. J.;Spiecker,E.; Brabec,C. J.Spray-CoatedSilverNanowiresasTopElectrode Layer in Semitransparent P3HTPCBM-Based OrganicSolar Cell Devices.Adv. Funct.Mater. 2013, 23, 1711- 1717.23 Rathmell,A. R.; Bergin,S.M.; Hua, Y. L.; Li, Z. Y.; Wiley, B. 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