Supporting Information

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1 Supporting Information Modulation of PEDOT:PSS ph for Efficient Inverted Perovskite Solar Cells with Reduced Potential Loss and Enhanced Stability Qin Wang 1,2, Chu-Chen Chueh 1, Morteza Eslamian 2 * and Alex K.-Y. Jen 1 * 1 Q. Wang, Dr. C.-C. Chueh, Prof. A. K.-Y. Jen Department of Materials Science and Engineering, University of Washington, Seattle, WA, 98105, USA. ajen@u.washington.edu 2 Q. Wang, Prof. M. Eslamian University of Michigan Shanghai Jiao Tong University Joint Institute, Shanghai, , China. Morteza.Eslamian@sjtu.edu.cn KEYWORDS: PEDOT:PSS, ph, potential loss, environmental stability, perovskite solar cells S-1

2 Figure S1. Contact angle images of a-, n-, and b-pedot:pss solution droplets on glass substrate. Figure S2. SEM images of a-, n-, and b-pedot:pss films at two magnifications: (a) 20,000X and (b) 50,000X. S-2

3 Figure S3. (a) N(1s) spectrum, (b) S(2p) spectrum and (c) O(1s) spectrum of a-, n-, and b-pedot:pss films. S-3

4 Figure S4. UV-vis absorption spectra of CH 3 NH 3 PbI 3 deposited on a-, n-, and b-pedot:pss films. Figure S5. Steady-state PL spectra of perovskite layers deposited on a-, n-, and b-pedot:pss films. S-4

5 Figure S6. J-V curves of b-pedot:pss PVSC device measured under forward scan (0 V~ 1.1 V) and reverse scan (1.1 V~0 V) at a scan rate of 0.1 V s -1. S-5

6 Figure S7. Illustration of the data in Table S1, summary of literature data on the performance of inverted PVSCs using PEDOT:PSS HTLs. The black square symbols represent the MAPbI 3 system, while the green circles represent the MAPbI 3-x Cl x system. In this work, MAPbI 3 system was used (Star shape). Devices fell in the hatched area show superior performance with a low potential loss (< 0.5V) and a high efficiency (>15%). MA stands for methylammonium.. S-6

7 Table S1. Literature summary of the perofrmance of inverted PVSCs using PEDOT:PSS HTLs. The (*) behind the device architechture represents the MAPbI 3-x Cl x system while the structure without (*) represents MAPbI 3 system. Our work is shown last one which belongs to MAPbI 3 system. Device architecture V oc (V) J sc [ma cm -2 ] FF (%) PCE (%) Remarks Referenc e ITO/PEDOT: PSS/HSL/MAPbI 3-xCl x/pcb M/PN4N/Ag (*) ITO/SOHEL/ MAPbI 3/PCBM/Al ITO/PEDOT: PSS-g-PANI:PFI/ MAPbI 3/PCBM/Al ITO/SOHEL4/ MAPbI 3/PCBM/Al ITO/PEDOT: PSS (1:20)/ MAPbI 3/PCBM/Ag ITO/1%PEDOT: PSS+NiO x/ MAPbI 3/PCBM/Ag Synthesizing new polymeric hole selective layer; Bilayer HTL; Self-organized HTL with high work function by tuning PFI/PEDOT: PSS weight ratio Self-doped HTL Universal energy level tailoring of a self-organized HTL Tuning the work function of HTL by tuning the ratio of PEDOT and PSS Hybrid layer for the HTL [1] [2] [3] [4] [5] [6] ITO/PEDOT: PSS-H(high conductivity) / MAPbI 3/PCBM/Al ITO/ 1%MoO 3+PEDOT: PSS/ MAPbI 3/C 60/Bphen/Ag Tuning the conductivity of HTL Using bilayer to increase the stability [7] [8] ITO/Sulfonated Lignin Doped PEDOT/MAPbI 3/PCBM/Ag ITO/PEDOT: PSS+0.05%wt Ag NPs/ MAPbI 3-xCl x/pcbm/bphen/a g (*) ITO/PEO doped PEDOT: PSS/ MAPbI 3/PCBM/Al Using high-value-added lignin to replace the PSS part Applying Ag NPs to improve the conductivity Improve the HTL conductivity by doping [9] [10] [11] ITO/PEDOT: PSS/perylene/MAPbI 3-xCl x/ PCBM/Bphen/Ag (*) ITO/ultrasonic treated PEDOT: PSS/MAPbI 3-xCl x/rhodamine 101/C 60/LiF/Ag (*) ITO/b-PEDOT: PSS/ MAPbI 3/PCBM/bis-C 60/Ag Perylene-Induced crystallization Physical method to increase the ph of PEDOT: PSS ph induced potential loss minimization and stability and efficiency enhancement [12] [13] Our work S-7

8 Figure S8. XPS spectra of a-pedot: PSS, n-pedot: PSS and b-pedot: PSS thin films after three days. Table S2. Atomic concentration of indium diffused into PEDOT:PSS with different ph. Measurement were performed after three days. HTLs a-pedot: PSS n-pedot: PSS b-pedot: PSS Indium atomic concentration (%) S-8

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10 MoO3/PEDOT:PSS Hole Transporting Layer. Nanoscale 2015, 7 (21), Wu, Y.; Wang, J.; Qiu, X.; Yang, R.; Lou, H.; Bao, X.; Li, Y., Highly Efficient Inverted Perovskite Solar Cells With Sulfonated Lignin Doped PEDOT as Hole Extract Layer. ACS Appl. Mater. Interfaces 2016, 8 (19), Qian, M.; Li, M.; Shi, X.-B.; Ma, H.; Wang, Z.-K.; Liao, L.-S., Planar Perovskite Solar Cells with 15.75% Power Conversion Efficiency by Cathode and Anode Interfacial Modification. J. Mater. Chem. A 2015, 3 (25), Huang, X.; Wang, K.; Yi, C.; Meng, T.; Gong, X., Efficient Perovskite Hybrid Solar Cells by Highly Electrical Conductive PEDOT:PSS Hole Transport Layer. Adv. Energy Mater. 2016, 6 (3), (1-8). 12. Wang, Z. K.; Gong, X.; Li, M.; Hu, Y.; Wang, J. M.; Ma, H.; Liao, L. S., Induced Crystallization of Perovskites by a Perylene Underlayer for High-Performance Solar Cells. ACS Nano 2016, 10 (5), Zhang, S.; Yu, Z.; Li, P.; Li, B.; Isikgor, F. H.; Du, D.; Sun, K.; Xia, Y.; Ouyang, J., Poly(3,4-ethylenedioxythiophene):polystyrene Sulfonate Films with Low Conductivity and Low Acidity through A Treatment of Their Solutions with Probe Ultrasonication and Their Application as Hole Transport Layer in Polymer Solar Cells and Perovskite Solar Cells. Org. Electron. 2016, 32, S-10