Tailoring Phase Alignment and Interfaces via Polyelectrolyte Anchoring Enables Large-Area 2D Perovskite Solar Cells

Ruddlesden-Popper phase 2D perovskite solar cells (PSCs) exhibit improved lifetime while still facing challenges such as phase alignment and up-scaling to module-level devices. Herein, polyelectrolytes are explored to tackle this issue. The contact between perovskite and hole-transport layer (HTL) is important for decreasing interfacial non-radiative recombination and scalable fabrication of uniform 2D perovskite films. Through exploring compatible butylamine cations, we first demonstrate poly(3-(4-carboxybutyl)thiophene-2,5-diyl)-butylamine (P3CT-BA) as an efficient HTL for 2D PSCs due to its great hydrophilicity, relatively high hole mobility and uniform surface. More importantly, the tailored P3CT-BA has an anchoring effect and acts as the buried passivator for 2D perovskites. Consequently, a best efficiency approaching 18 % was achieved and we further first report large-area (2×3 cm² , 5×5 cm² ) 2D perovskite minimodules with an impressive efficiency of 14.81 % and 11.13 %, respectively.