Dredging the Charge‐Carrier Transfer Pathway for Efficient Low‐Dimensional Ruddlesden‐Popper Perovskite Solar Cells

Abstract Low‐dimensional Ruddlesden‐Popper (LDRP) perovskites still suffer from inferior carrier transport properties. Here, we demonstrate that efficient exciton dissociation and charge transfer can be achieved in LDRP perovskite by introducing γ‐aminobutyric acid (GABA) as a spacer. The hydrogen bonding links adjacent spacing sheets in (GABA) 2 MA 3 Pb 4 I 13 (MA=CH 3 NH 3 + ), leading to the charges localized in the van der Waals gap, thereby constructing “charged‐bridge” for charge transfer through the spacing region. Additionally, the polarized GABA weakens dielectric confinement, decreasing the (GABA) 2 MA 3 Pb 4 I 13 exciton binding energy as low as ≈73 meV. Benefiting from these merits, the resultant GABA‐based solar cell yields a champion power conversion efficiency (PCE) of 18.73 % with enhanced carrier transport properties. Furthermore, the unencapsulated device maintains 92.8 % of its initial PCE under continuous illumination after 1000 h and only lost 3 % of its initial PCE under 65 °C for 500 h.