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The determination of the semiconducting materials performance heavily relies on the diffusion coefficient and length of the carrier. Recently, significant progress is made in enhancing solar cell efficiency through improved carrier diffusion in perovskite thin films. However, the spatial‐temporal mechanisms underlying carrier transport remain unclear. Recent advancements in utilizing transient absorption microscopy (TAM) offer promising opportunities to directly visualize the carrier transport dynamics within perovskite films. Here, the wide‐field imaging TAM combined with X‐ray diffraction and scanning electron microscopy is employed to investigate the spatial‐temporal carrier transport dynamics in FA1−xCsxPbI3 perovskites with varying Cs doping ratios. The experimental results indicate that the diffusion constant remains consistent regardless of the excitation power. Moreover, a decrease in the Cs doping ratio leads to an increase in the diffusion length within FA1−xCsxPbI3 perovskites. The measurements reveal a highest diffusion coefficient of up to 0.085 cm2 s−1 and a maximum diffusion length of ≈1.4 µm in FA0.97Cs0.03PbI3. Comparative analysis of short‐circuit current density, open‐circuit voltage, fill factor, and power conversion efficiency demonstrates that FA0.97Cs0.03PbI3 exhibits superior device efficiency. The TAM visualizes spatial/ temporal carrier diffusion dynamics, showing a significant correlation with device efficiency and thus providing valuable insights for further enhancing device performance. [ABSTRACT FROM AUTHOR]

The combination of comprehensive surface passivation and effective interface carriers transfer plays a critical role in high-performance perovskite solar cells. A 2D structure is an important approach for surface passivation of perovskite film, however, its large band gap could compromise carrier transfer. Herein, we synthesize a new molecule 2-thiopheneethylamine thiocyanate (TEASCN) for the construction of bilayer quasi-2D structure precisely on a tin-lead mixed perovskite surface. This bilayer structure can passivate the perovskite surface and ensure effective carriers transfer simultaneously. As a result, the open-circuit voltage (V oc ) of the device is increased without sacrificing short-circuit current density (J sc ), giving rise to a high certified efficiency from a credible third-party certification of narrow band gap perovskite solar cells. Furthermore, theoretical simulation indicates that the inclusion of TEASCN makes the bilayer structure thermodynamically more stable, which provides a strategy to tailor the number of layers of quasi-2D perovskite structures., (© 2022 Wiley-VCH GmbH.)