Organolead trihalide perovskite films with a large grain size and excellent surface morphology are favored to good-performance solar cells. However, interstitial and antisite defects related trap-states are originated unavoidably on the surfaces of the perovskite films prepared by the solution deposition procedures. The development of post-growth treatment of defective films is an attractive method to reduce the defects to form good-quality perovskite layers. Herein, a post-treatment tactic is developed to optimize the perovskite crystallization by treating the surface of the one-step deposited CH 3 NH 3 PbI 3 (MAPbI 3 ) using formamidinium iodide (FAI). Charge carrier kinetics investigated via time-resolved photoluminescent, open-circuit photovoltage decay, and time-resolved charge extraction indicate that FAI post-treatment will boost the perovskite crystalline quality, and further result in the reduction of the defects or trap-states in the perovskite films. The photovoltaic devices by FAI treatment show much improved performance in comparison to the controlled solar cell. As a result, a champion solar cell with the best power conversion efficiency of 20.25% is obtained due to a noticeable improvement in fill factor. This finding exhibits a simple procedure to passivate the perovskite layer via regulating the crystallization and decreasing defect density.

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Two-dimensional (2D) perovskites, which have excellent stability compared with threedimensional (3D) perovskites owing to the effective protection of the hydrophobic organic ligands, have become a research hotspot and have made great developmental progress in recent years. Herein, an n-butylammonium iodide (BAI) post-treatment process was developed to fabricate a 2D-3D hybrid perovskite with a thin layer of 2D perovskite covered on the surface of the 3D CH 3 NH 3 PbI 3 perovskite. The growth process of 2D perovskite is formed through the chemical reaction between BAI and the residual PbI 2 , which improves stability and reduces the number of crystal defects of 3D perovskite by optimizing stoichiometry. Compared with the 3D counterpart, the 2D-3D hybrid perovskite shows outstanding light and air stability when exposed to external environments. Moreover, structure conversion from 3D to 2D-3D can induce the passivation of defects in the 3D films. The power conversion efficiency of the 2D-3D solar cell exceeds 18% and retains 80% of the initial value after more than 2000 h of storage without encapsulation.

Perovskite solar cells (PSCs) have been developed as a promising photovoltaic technology because of their excellent photovoltaic performance. However, interfacial recombination and charge carrier transport losses at the surface greatly limit the performance and stability of PSCs. In this work, the fabrication of high-quality PSCs based on methylammonium lead iodide with excellent ambient stability is reported. An anionic surfactant, sodium dodecylbenzene sulfonate (SDBS), is introduced to simultaneously passivate the defect states and stabilize the cubic phase of the perovskite film. The SDBS located at grain boundaries and the surface of the active layer can effectively passivate under-coordinated lead ions and protect the perovskite components from water-induced degradation. As a result, a champion power conversion efficiency (PCE) of 19.42% is achieved with an open-circuit voltage (V OC ) of 1.12 V, a short-circuit current (J SC ) of 23.23 mA cm −2 , and a fill factor (FF) of 74% in combination with superior moisture stability. The SDBS-passivated devices retain 80% of their initial average PCE after 2112 h of storage under ambient conditions.

Crystal orientations are closely related to the behavior of photogenerated charge carriers and are vital for controlling the optoelectronic properties of perovskite solar cells. Herein, we propose a facile approach to reveal the effect of lattice plane orientation distribution on the charge carrier kinetics via constructing CsBr-doped mixed cation perovskite phases. With grazing-incidence wide-angle X-ray scattering measurements, we investigate the crystallographic properties of mixed perovskite films at the microscopic scale and reveal the effect of the extrinsic CsBr doping on the stacking behavior of the lattice planes. Combined with transient photocurrent, transient photovoltage, and spacecharge-limited current measurements, the transport dynamics and recombination of the photogenerated charge carriers are characterized. It is demonstrated that CsBr compositional engineering can significantly affect the perovskite crystal structure in terms of the orientation distribution of crystal planes and passivation of trap-state densities, as well as simultaneously facilitate the photogenerated charge carrier transport across the absorber and its interfaces. This strategy provides unique insight into the underlying relationship between the stacking pattern of crystal planes, photogenerated charge carrier transport, and optoelectronic properties of solar cells.