The Effect of the Alkyl Chains of the Alkylammonium Pesudohalide Additives on the Performance of Dion Jacobson Perovskite Solar Cells

Abstract Dion‐Jacobson perovskite (DJP) films suffer from the high structural disorder and non‐compact morphology, leading to inefficient and unstable solar cells (SCs). Here, how the alkyl chains of alkylammonium pseudohalide additives including methylammonium thiocyanate (MASCN) and ethylammonium thiocyanate (EASCN), and propylammonium thiocyanate (PASCN), impact the microstructures, optoelectronic properties and the performance of the solar cells is investigated. These additives substantially improve the structural order and the morphology of the DJP films, yielding more efficient and stable solar cells than the control device. They behave quite differently in modifying the morphological features. Particularly, EASCN outstands the additives in terms of the superior morphology, which is compact and uniform and consists of the largest flaky grains. Consequently, the corresponding device delivers a power conversion efficiency (PCE) of 15.27% and maintains ≈86% of the initial PCE after aging in the air for 182 h. Conversely, MASCN as an additive produces uneven DJP film and the device maintains only 46% of the initial PCE. PASCN as an additive produces the finest grains in the DJP film, and the corresponding device yields a PCE of 11.95%. From the economical point of view, it costs 0.0025 yuan per device for the EASCN additive, allowing for cost‐effective perovskite solar cells.