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Efficient electron transport layer–free perovskite solar cells (ETL‐free PSCs) with cost‐effective and simplified design can greatly promote the large area flexible application of PSCs. However, the absence of ETL usually leads to the mismatched indium tin oxide (ITO)/perovskite interface energy levels, which limits charge transfer and collection, and results in severe energy loss and poor device performance. To address this, a polar nonconjugated small‐molecule modifier is introduced to lower the work function of ITO and optimize interface energy level alignment by virtue of an inherent dipole, as verified by photoemission spectroscopy and Kelvin probe force microscopy measurements. The resultant barrier‐free ITO/perovskite contact favors efficient charge transfer and suppresses nonradiative recombination, endowing the device with enhanced open circuit voltage, short circuit current density, and fill factor, simultaneously. Accordingly, power conversion efficiency increases greatly from 12.81% to a record breaking 20.55%, comparable to state‐of‐the‐art PSCs with a sophisticated ETL. Also, the stability is enhanced with decreased hysteresis effect due to interface defect passivation and inhibited interface charge accumulation. This work facilitates the further development of highly efficient, flexible, and recyclable ETL‐free PSCs with simplified design and low cost by interface electronic structure engineering through facile electrode modification. [ABSTRACT FROM AUTHOR]

Device modeling of CH 3 NH 3 PbI 3−x Cl x based electron transport layer-free planar perovskite solar cells was performed. The simulation was conducted by the program SCAPS (Solar Cell Capacitance Simulator). With appropriate physical parameters, a high open-circuit voltage of 1.04 V close to results reported experimentally was successfully reproduced in the simulation. Simulation results revealed a great dependence of PCE on the thickness and defect density of the perovskite layer. An optimum perovskite thickness of about 500 nm was confirmed and it well consistent with the thickness range of real devices was derived. Meanwhile, parameters including the FTO/perovskite interface defect density as well as the doping concentration of the front contact (FTO) were identified to significantly influence the performance of the device. In particular, the interface quality at the FTO/perovskite interface has greater impact on the device parameters than that at the perovskite/HTL interface, which suggests that more attention should be paid to the front FTO/perovskite interface to further enhance the performance of electron transport layer-free device. Appropriate interface defect passivation to reduce the interface defect density to the order of ~10 15 cm −3 is necessary and urgently needed. Lastly, the effect of the electron and hole mobility and carrier diffusion length of CH 3 NH 3 PbI 3−x Cl x were also analyzed and the results revealed that the mobility and diffusion length experimentally reported (~1.0 µm) are large and long enough for high efficiency. [ABSTRACT FROM AUTHOR]