Supplementary Information

Printing-friendly sequential deposition via intra-

additive approach for roll-to-roll process of perovskite

solar cells

Youn-Jung Heo1,2, Jueng-Eun Kim1,2, Hasitha Weerasinghe1, Dechan Angmo1, Tianshi Qin1, Kallista Sears1, Kyeongil Hwang1,2, Yen-Sook

Jung1,2, Jegadesan Subbiah3, David J. Jones3, Mei Gao2, Dong-Yu Kim2* and Doojin Vak1*

1Flexible Electronics Lab, CSIRO Manufacturing, Clayton South, Victoria 3168, Australia

2School of Materials Science and Engineering (MSE), Gwangju Institute of Science and Technology (GIST), Gwangju 61005, Republic of Korea3School of Chemistry Bio21 Institute, University of Melbourne Victoria

3010, Australia

Figure S1. SEM images of slot-die coated PbI2 films (a) without MAI additive and (b) with MAI additive system. Films were formed without external drying system (i.e. N2 gas blowing)

Figure S2. J-V curve of a slot die coated perovskite solar cells on ITO glass using FAI additive in printing-friendly sequential deposition process.

Figure S3. Sequential slot die coating setup on a roll-to-roll coater used for initial trial for printing-friendly sequential deposition

Figure S4. A device layout developed for small scale roll-to-roll experiments

Figure S5 J-V curves of a roll-to-roll slot die coated devices prepared using previously published sequential slot die coating. [Hwang et al. Advanced Materials, 2015, 27, 1241.] The new device layout shown in Figure S5 was used with previously reported procedure and compared with published results.

Figure S6 PCEs of roll-to-roll slot die coated perovskite devices with various solution flow of PbI2 + 40 mol% FAI. The experiment was

carried out before optimization of other layers. PET/TCE/ZnO/FA0.4:MA0.6:PbI3/P3HT/Ag device configuration was used.

Figure S7 PCE of roll-to-roll slot die coated perovskite devices with ZnO layer condition. PET/TCE/ZnO/FA0.4:MA0.6:PbI3/neutral PEDOT:PSS/Ag device configuration was used.

Figure S8 PCE of roll-to-roll slot die coated perovskite devices with different HTLs. PET/TCE/ZnO/FA0.4:MA0.6:PbI3/HTLs/Ag device configuration was used.

Figure S9 SEM cross-section of R2R processed perovskite cells with a configuration of PET/TCO/perovskite/PEDOT:PSS/MoO3/Ag.