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A Universal Strategy of Perovskite Ink - Substrate Interaction to Overcome the Poor Wettability of a Self-Assembled Monolayer for Reproducible Perovskite Solar Cells
Authors:Ashish Kulkarni  Ranjini Sarkar  Samah Akel  Maria Häser  Benjamin Klingebiel  Matthias Wuttig  Simone Wiegand  Sudip Chakraborty  Michael Saliba  Thomas Kirchartz
Affiliation:1. Helmholtz Young Investigator Group FRONTRUNNER, IEK5-Photovoltaik, Forschungszentrum Jülich, Wilhelm-Johnen-Straße, 52428 Jülich, Germany;2. Materials Theory for Energy Scavenging (MATES) Lab, Department of Physics, Harish-Chandra Research Institute (HRI), A C.I. of Homi Bhabha National Institute (HBNI), Chhatnag Road, Jhunsi, Prayagraj, 211019 India

Ceramic Technologies Group – Center of Excellence in Materials and Manufacturing for Futuristic Mobility, Indian Institute of Technology (IIT) Madras, Chennai, 600036 India;3. IEK-5 Photovoltaik, Forschungszentrum Jülich, Wilhelm-Johnen-Straße, 52428 Jülich, Germany;4. I. Physikalisches Institut, RWTH Aachen University, 52074 Aachen, Germany;5. I. Physikalisches Institut, RWTH Aachen University, 52074 Aachen, Germany

Peter Grünberg Institute – JARA-Institute Energy-Efficient Information Technology (PGI-10), Forschungszentrum Jülich GmbH, 52425 Jülich, Germany;6. Institute of Biological Information Processing (IBI-4:Biomacromolecular Systems and Processes), Forschungszentrum Jülich, Wilhelm-Johnen-Straße, 52428 Jülich, Germany

Chemistry Department – Physical Chemistry, University Cologne, D-50939 Cologne, Germany;7. Materials Theory for Energy Scavenging (MATES) Lab, Department of Physics, Harish-Chandra Research Institute (HRI), A C.I. of Homi Bhabha National Institute (HBNI), Chhatnag Road, Jhunsi, Prayagraj, 211019 India

Abstract:Perovskite solar cells employing [4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz) self-assembled monolayer as the hole transport layer have been reported to demonstrate a high device efficiency. However, the poor perovskite wetting on Me-4PACz caused by poor perovskite ink interaction with the underlying Me-4PACz presents significant challenges for fabricating efficient perovskite devices. A triple co-solvent system comprising dimethylformamide (DMF), dimethyl sulfoxide (DMSO), and N-methyl-2-pyrrolidone (NMP) is employed to improve the perovskite ink - Me-4PACz coated substrate interaction and obtain a uniform perovskite layer. In comparison to DMF- and DMSO-based inks, the inclusion of NMP shows considerably higher binding energies of the perovskite ink with Me-4PACz as revealed by density-functional theory calculations. With the optimized triple co-solvent ratio, the perovskite devices deliver high power conversion efficiencies of >20%, 19.5%, and ≈18.5% for active areas of 0.16, 0.72, and 1.08 cm2, respectively. Importantly, this perovskite ink–substrate interaction approach is universal and helps in obtaining a uniform layer and high photovoltaic device performance for other perovskite compositions such as MAPbI3, FA1−xMAxPbI3–yBry, and MA-free FA1−xCsxPbI3–yBry.
Keywords:hydrophobicity  large areas  perovskite inks  self-assembled monolayers  solar cells  solvent interactions
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