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1 Supporting Information A Completely Benign Food Additive Solution Enables Air Processing of Organic Solar Cells with High Performance and Hierarchical Morphology Long Ye, Yuan Xiong, Huifeng Yao, Abay Gadisa, Hao Zhang, Sunsun Li, Masoud Ghasemi, Nrup Balar, Adrian Hunt, Brendan T. O Connor, Jianhui Hou, * and Harald Ade, * Department of Physics and Organic and Carbon Electronics Laboratory, North Carolina State University, Raleigh, NC 27695, USA Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing , China Department of Mechanical and Aerospace Engineering, North Carolina State University, Raleigh, NC 27695, USA Basic Information of o-ma [S1-S3] Full Name: ortho-methyl anisole; 2-Methylanisole; 1-methoxy-2-methylbenzene CAS Number: Appearance: colorless Chemical formula: C 8 H 10 O Molecular Weight: g/mol Density: g/cm 3 Boiling Points: C Alfa Aesar S1

2 Flash Points: 51 C Alfa Aesar Safety: GHS02 Category: flavor and fragrance agents Function used in food: Flavoring ingredient [S3] 2. DSC thermogram of PBDT-TSR Figure S1. DSC heat-cool-heat trace of pure PBDT-TSR. No apparent peak of melting or crystallization transition was observed during the heating and cooling process, so PBDT-TSR is a low crystalline polymer. 3. 2D GIXRD patterns of spin-coated and blade-coated films. S2

3 Figure S2. 2D GXRD patterns of spin-coated PBDT-TSR:PC 71 BM film using (a) CB/DIO and (b) o-ma. Both films show similar amphous rings and exhibit a low degree of molecular order, as evidenced by weak (100) and (010) reflection peaks. Some extra features (sharp rings around ~1.7 Å -1 ) are from substrate scattering. GIXRD characterizations was carried out at Beamline [S4], ALS, Berkeley National Lab. 4. Materials Contrast of PBDT-TSR and PC 71 BM 10 6 Contrast Function PCBM Vac PBDT-TSR Vac Material Contrast 295 Photon Energy [ev] 300 Figure S3. PBDT-TSR:PC 71 BM material contrast and vacuum/mass-thickness contrast functions. 5. Multipeak Fit of R-SoXS profiles of spin-coated films. S3

4 Figure S4. Log-normal multipeak Fit of R-SoXS profiles of spin-coated PBDT- TSR:PC 71 BM films processed by o-ma (a) and CB/DIO (b). Both profiles can be fitted with two peaks, with q around 0.15 nm -1 and 0.3 nm AFM height image of blade coated PBDT-TSR:PC 71 BM film. Figure S5 AFM height image of blade coated PBDT-TSR:PC 71 BM film. 7. FFT analysis of AFM phase image of blade coated PBDT-TSR:PC 71 BM film. S4

5 Figure S6. PSD from AFM phase image of blade coated PBDT-TSR:PC 71 BM film. The multi-length scale features are roughly consistent with the R-SoXS observation as ahown in Figure 4b. 8. Blade fabrication and EQE curve of all-polymer OPV device featuring PBDT- TS1:PPDIODT Blade fabrication of all-polymer OPV [S5] : Equal weight amounts of PBDT-TS1 and PPDIODT were dissolved in o-ma with a total concentration of 14 mg/ml and then stirred at 110 C for 8 h. For the inverted devices, a thin layer of ZnO (~30 nm) was spin-coated onto precleaned ITO-coated glass substrates and then annealed at 180 C for 1 h in air. The ZnO precursor solution were prepared according to a previous report [S6] by the H. Yan group. Subsequently, all-polymer blend film layer was blade-coated at a speed of 40 mm/s on the top of ZnO. Finally, 10 nm thick MoO 3 film and 90 nm thick Al layers were deposited sequentially to complete the inverted device. S5

6 EQE curve (left) and PSD of AFM phase image (right) of blade-coated all-polymer OPV device based on PBDT-TS1:PPDIODT. All-polymer blend film blade coated in air also exhibits a multiple length scale morphology. 9. Comparison of our result with the previous results in literatures. Table S1. PCEs of the state-of-the-art blade-coated OPV devices. Materials Solvent Single Green Processed PCE Solvent Solvent in air (%) Ref. POD2T-DTBT:PCBM CB Yes 6.69 [S7] PBDTTT-C-T:PCBM Xylene Yes Yes 5.98 [S8] PDPP5T-2:PCBM CF+DCB 6.3 [S9] PIDT-PhanQ:PCBM DCB Yes Yes 7.08 [S10] PiI-tT-PS5:P(TP) CB Yes 3.2 [S11] PTB7-Th:PC 71BM CB+DIO Yes 8.35 [S12] N(Ph-2T-DCN-Et)3:PC 71BM Benzaldehyde +Mesitylene Yes Yes 3.74 [S13] PBDT-TSR:PC 71BM o-ma Yes Yes Yes 8.38 This work 10. Blade Coater Experimental Setup (a) (b) (b) S6

7 Figure S7. (a) Blade coater setup integrated with a variable angle ellipsometer (b) Components of the blade coater setup: (1) linear translation stage, (2) stepper motor, (3) XY translation stage, (4) vertical translation stage, (5) tip-tilt and rotation stage. The experimental setup was based upon the design reported by Stafford et al [S14]. The blade coater in integrated with a spectroscopic ellipsometer (M2000, J A Woollam Co) as shown in the Figure S7a. This required movement of the blade, as apposed to movement of the substrate as reported by Stafford et al. The components of the blade coater are pictured in Figure S7b. The blade coater consists of a translation stage (404XR-150, Parker Automation) driven by a computer controlled stepper motor (DMX UMD 23, Arcus Technology) that controls the motion of the blade. An XY translation stage is mounted on top of the linear actuator to adjust the position of the blade in the horizontal plane. The set-up also includes a vertical linear translation stage to adjust the blade gap, and a tip-tilt-rotation stage is used to ensure that the blade edge is horizontal and well aligned with the edges of the substrate. The substrate is placed on a custom heating stage module, which was supplied with the ellipsometer, so that the temperature of the substrate can also be controlled which eventually enables us to control the rate of evaporation of solvent. The substrate is held stationary with vacuum. References: [S1] Sigma-Aldrich (website accessed by June 2016) [S2] Alfa Aesar (website accessed by June 2016) https://www.alfa.com/en/catalog/a13897/ [S3] Encyclopedia of Food and Color Additives, Volume 1, By George A. Burdock, Page 1715, CRC Press. [S4] Hexemer, A.; Bras, W.; Glossinger, J.; Schaible, E.; Gann, E.; Kirian, R.; MacDowell, A.; Church, M.; Rude, B.; Padmore, H. A SAXS/WAXS/GISAXS Beamline with Multilayer Monochromator. J. Phys.: Conf. Ser. 2010, 247, S7

8 [S5] Li, S.; Zhang, H.; Zhao, W.; Ye, L.; Yao, H.; Yang, B.; Zhang, S.; Hou, J., Green- Solvent-Processed All-Polymer Solar Cells Containing a Perylene Diimide-Based Acceptor with an Efficiency over 6.5%. Adv. Energy Mater. 2016, 6, [S6] Liu, Y.; Zhao, J.; Li, Z.; Mu, C.; Ma, W.; Hu, H.; Jiang, K.; Lin, H.; Ade, H.; Yan, H. Aggregation and morphology control enables multiple cases of high-efficiency polymer solar cells. Nat. Commun. 2014, 5, [S7] Lim, S.-L.; Chen, E.-C.; Chen, C.-Y.; Ong, K.-H.; Chen, Z.-K.; Meng, H.-F. High performance organic photovoltaic cells with blade-coated active layers. Sol. Energy Mater. Sol. Cells 2012, 107, [S8] Tsai, P.-T.; Tsai, C.-Y.; Wang, C.-M.; Chang, Y.-F.; Meng, H.-F.; Chen, Z.-K.; Lin, H.- W.; Zan, H.-W.; Horng, S.-F.; Lai, Y.-C.; Yu, P. High-efficiency polymer solar cells by blade coating in chlorine-free solvents. Organic Electronics 2014, 15, [S9] Tait, J. G.; Merckx, T.; Li, W.; Wong, C.; Gehlhaar, R.; Cheyns, D.; Turbiez, M.; Heremans, P. Determination of Solvent Systems for Blade Coating Thin Film Photovoltaics. Adv. Funct. Mater. 2015, 25, [S10] Kim, J. H.; Jung, J. W.; Williams, S. T.; Liu, F.; Russell, T. P.; Jen, A. K. Y. Enhanced crystalline morphology of a ladder-type polymer bulk-heterojunction device by blade-coating. Nanoscale 2015, 7, [S11] Diao, Y.; Zhou, Y.; Kurosawa, T.; Shaw, L.; Wang, C.; Park, S.; Guo, Y.; Reinspach, J. A.; Gu, K.; Gu, X.; Tee, B. C.; Pang, C.; Yan, H.; Zhao, D.; Toney, M. F.; Mannsfeld, S. C.; Bao, Z., Flow-enhanced Solution Printing of All-polymer Solar Cells. Nat. Commun. 2015, 6, [S12] Li, N.; Brabec, C. J. Air-processed polymer tandem solar cells with power conversion efficiency exceeding 10%. Energy Environ. Sci. 2015, 8, [S13] Burgués-Ceballos, I.; Machui, F.; Min, J.; Ameri, T.; Voigt, M. M.; Luponosov, Y. N.; Ponomarenko, S. A.; Lacharmoise, P. D.; Campoy-Quiles, M.; Brabec, C. J. Solubility Based S8

9 Identification of Green Solvents for Small Molecule Organic Solar Cells. Adv. Funct. Mater. 2014, 24, [S14] Stafford, C. M.; Roskov, K. E.; Epps, T. H.; Fasolka, M. J. Generating thickness gradients of thin polymer films via flow coating. Rev. Sci. Instrum. 2006, 77, S9

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