Advanced Optical Materials 11, 16

Recently, the mixed-dimensional (3D/2D or 3D/1D) perovskite solar cells using small organic spacers have attracted interest due to their outstanding long-term stability. Here, a new type of thiophene-based organic cation 2-(thiophene-2yl-)pyridine-1-ium iodide (ThPyI), which is used to fabricate mixed-dimensional 3D/1D perovskite solar cells, is presented. The ThPyI-based 1D perovskitoid is applied as a passivator on top of a 3D methyl ammonium lead iodide (MAPI) to fabricate surface-passivated 3D/1D perovskite films or added alone into the 3D perovskite precursor to generate bulk-passivated 3D MAPI. The 1D perovskitoid acts as a passivating agent at the grain boundaries of surface-passivated 3D/1D, which improves the power conversion efficiency (PCE) of the solar cells. Grazing incidence wide-angle X-ray scattering (GIWAXS) studies confirm that ThPyI triggers the preferential orientation of the bulk MAPI slabs, which is essential to enhance charge transport. Champion bulk-passivated 3D and surface-passivated 3D/1D devices yield 14.10% and 19.60% PCE, respectively. The bulk-passivated 3D offers favorable stability, with 84% PCE retained after 2000 h without encapsulation. This study brings a new perspective to the design of organic spacers having a different binding motif and a passivation strategy to mitigate the impact of defects in hybrid 3D/1D perovskite solar cells.