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Among various types of perovskite-based tandem solar cells (TSCs), all-perovskite TSCs are of particular attractiveness for building- and vehicle-integrated photovoltaics, or space energy areas as they can be fabricated on flexible and lightweight substrates with a very high power-to-weight ratio. However, the efficiency of flexible all-perovskite tandems is lagging far behind their rigid counterparts primarily due to the challenges in developing efficient wide-bandgap (WBG) perovskite solar cells on the flexible substrates as well as their low open-circuit voltage (V-OC). Here, it is reported that the use of self-assembled monolayers as hole-selective contact effectively suppresses the interfacial recombination and allows the subsequent uniform growth of a 1.77 eV WBG perovskite with superior optoelectronic quality. In addition, a postdeposition treatment with 2-thiopheneethylammonium chloride is employed to further suppress the bulk and interfacial recombination, boosting the V-OC of the WBG top cell to 1.29 V. Based on this, the first proof-of-concept four-terminal all-perovskite flexible TSC with a power conversion efficiency of 22.6% is presented. When integrating into two-terminal flexible tandems, 23.8% flexible all-perovskite TSCs with a superior V-OC of 2.1 V is achieved, which is on par with the V-OC reported on the 28% all-perovskite tandems grown on the rigid substrate.
Perovskite semiconductors differ from most inorganic and organic semiconductors due to the presence of mobile ions in the material. Although the phenomenon is intensively investigated, important questions such as the exact impact of the mobile ions on the steady-state power conversion efficiency (PCE) and stability remain. Herein, a simple method is proposed to estimate the efficiency loss due to mobile ions via "fast-hysteresis" measurements by preventing the perturbation of mobile ions out of their equilibrium position at fast scan speeds (approximate to 1000 V s(-1)). The "ion-free" PCE is between 1% and 3% higher than the steady-state PCE, demonstrating the importance of ion-induced losses, even in cells with low levels of hysteresis at typical scan speeds (approximate to 100mv s(-1)). The hysteresis over many orders of magnitude in scan speed provides important information on the effective ion diffusion constant from the peak hysteresis position. The fast-hysteresis measurements are corroborated by transient charge extraction and capacitance measurements and numerical simulations, which confirm the experimental findings and provide important insights into the charge carrier dynamics. The proposed method to quantify PCE losses due to field screening induced by mobile ions clarifies several important experimental observations and opens up a large range of future experiments.