Tailoring wetting properties of organic hole-transport interlayers for slot-die coated perovskite solar modules

The use of self-assembled monolayers (SAMs) with anchoring groups was considered as an effective approach for interface engineering in perovskite solar cells with metal oxide charge transporting layers. However, the coating of SAM layers in PSMs by means of a slot-die is a challenging process due to the low viscosity of the solutions and the low wettability of the films. In this study, we integrate a triphenylamine-based polymer, pTPA-TDP, blended with SAM based on 5-[4-[4-(diphenylamino) phenyl] thiophene-2-carboxylic acid (TPATC), to address the challenges of uniform slot-die coating and interface passivation in large-area modules. We fabricated p-i-n oriented PSMs on 50x50 mm2 substrates (12-sub-cells) with NiO hole transport layer (HTL) and organic interlayers for surface modification. Wetting angle mapping demonstrated that ununiform regions of the slot-die coated SAM have hydrophobicity with contact angle values up to 90{\deg}, causing fluctuations in absorber thickness and the presence of macro-defects at buried interfaces. The incorporation of the blended interlayer to NiO/perovskite junction homogenized the surface wettability (contact angle=40{\deg}) and mitigated lattice strain in the absorber. This enabled the effective use of SAM properties on a large-area surface, improving energy level alignment and enhancing the power conversion efficiency (PCE) of the modules from 13.98% to 15.83% and stability (ISOS-L-2, T80 period) from 500-1000 hours to 1630 hours. Investigation of PSMs upon cooling till -5 {\deg}C showed that the PCE increased by +0.19%/{\deg}C for samples with NiO HTL, while using SAM and blended interlayers raised the coefficient to ~0.40%/{\deg}C due to changes in activation energy and trap contributions to device performance across a wide temperature range.