Abstract
Bulky organic cations exhibit significant roles in improving the phase stability of CsPbI3 by reducing its dimension with higher steric hindrance. However, the insulative properties of organic cations impede the carrier transition and damage the device performance. Herein, a new aromatic cation of 4‐fluorobenzenaminium (FPA+) in the 2D CsPbI3 to act as a spacer cation, is reported. Based on the theoretical simulation and experimental characterization for materials properties, film quality, and device performance, the large dipole moment and electronic inductive effect of FPA+ cations improve the hydrogen bond between H and I atoms, which is beneficial to realizing controllable crystallization quality. Therefore, the whole quality of 2D CsPbI3 film is improved with a larger grain size, compact morphology, and low trap density. As a result, the (FPA)2Cs4Pb5I16 perovskite solar cell delivers a power conversion efficiency of 15.18%, significantly higher than that of PA‐based (14.32%) perovskite solar cells. Herein, an in‐depth understanding of fluoro‐substituted organic cations is provided and is beneficial to the design and synthesis of new organic molecules in 2D perovskite.
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