Efficient Planar Structured Perovskite Solar Cells with Enhanced Open-Circuit Voltage and Suppressed Charge Recombination Based on a Slow Grown Perovskite Layer from Lead Acetate Precursor

For planar structured organic–inorganic hybrid perovskite solar cells (PerSCs) with the poly­(3,4-ethylenedioxythiophene:polystyrene sulfonate) (PEDOT:PSS) hole transport layer, the open-circuit voltage (<i>V</i>_oc) of the device is limited to be about 1.0 V, resulting in inferior performance in comparison with TiO₂-based planar counterparts. Therefore, increasing <i>V</i>_oc of the PEDOT:PSS-based planar device is an important way to enhance the efficiency of the PerSCs. Herein, we demonstrate a novel approach for perovskite film formation and the film is formed by slow growth from lead acetate precursor via a one-step spin-coating process without the thermal annealing (TA) process. Because the perovskite layer grows slowly and naturally, high-quality perovskite film can be achieved with larger crystalline particles, less defects, and smoother surface morphology. Ultraviolet absorption, X-ray diffraction, scanning electron microscopy, steady-state fluorescence spectroscopy (photoluminescence), and time-resolved fluorescence spectroscopy are used to clarify the crystallinity, morphology, and internal defects of perovskite thin films. The power conversion efficiency of p–i–n PerSCs based on slow-grown film (16.33%) shows greatly enhanced performance compared to that of the control device based on traditional thermally annealed perovskite film (14.33%). Furthermore, the <i>V</i>_oc of the slow-growing device reaches 1.12 V, which is 0.1 V higher than that of the TA device. These findings indicate that slow growth of the perovskite layer from lead acetate precursor is a promising approach to achieve high-quality perovskite film for high-performance PerSCs