Resolving the Hydrophobicity of Me-4PACz Hole Transport Layer for Inverted Perovskite Solar Cells

[4-(3,6-Dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz) self-assembled monolayer (SAM) has been employed in perovskite single junction and tandem devices demonstrating high efficiencies. However, a uniform perovskite layer does not form due to the hydrophobicity of Me-4PACz. Here, we tackle this challenge by adding a conjugated polyelectrolyte poly(9,9-bis(3’-(N,N-dimethyl)-N-ethylammonium-propyl-2,7-fluorene)-alt-2,7-(9,9dioctylfluorene))dibromide (PFN-Br) to the Me-4PACz in a specific ratio, defined as Pz:PFN. With this mixing engineering strategy of Pz:PFN, the PFN-Br interacts with the A-site cation is confirmed via solution-state nuclear magnetic resonance studies. The narrow full width at half maxima (FWHM) of diffraction peaks of perovskite film revealed improved crystallization on optimal mixing ratio of Pz:PFN. Interestingly, the mixing of PFN-Br additionally tunes the work function of the Me-4PACz as revealed by Kelvin probe force microscopy and built-in-voltage estimation in solar cells. Devices employing optimized Pz:PFN mixing ratio deliver open-circuit voltage (<i>V</i>_OC) of 1.16V and efficiency &gt;20% for perovskites with a bandgap of 1.6 eV with high reproducibility and concomitant stability. Considering significant research on Me-4PACz SAM, our work highlights the importance of obtaining a uniform perovskite layer with improved yield and performance.<br/><br/>Reference: <br/>Hossain, K.; Kulkarni, A.; Bothra, U.; Klingebiel, B.; Kirchartz, T.; Saliba, M.; Kabra, D. Resolving the Hydrophobicity of Me-4PACz Hole Transport Layer for High-Efficiency Inverted Perovskite Solar Cells. <i>arXiv Prepr. arXiv2304.13788</i> <b>2023</b>.