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  1. Stabilizing perovskite solar cells requires consideration of all defective sites in the devices. Substantial efforts have been devoted to interfaces, while stabilization of grain boundaries received less attention. Here, we report on a molecule tributyl(methyl)phosphonium iodide (TPI), which can convert perovskite into a wide bandgap one-dimensional (1D) perovskite that is mechanically robust and water insoluble. Mixing TPI with perovskite precursor results in a wrapping of perovskite grains with both grain surfaces and grain boundaries converted into several nanometer-thick 1D perovskites during the grain formation process as observed by direct mapping. The grain wrapping passivates the grain boundaries, enhances their resistance to moisture, and reduces the iodine released during light soaking. The perovskite films with wrapped grains are more stable under heat and light. The best device with wrapped grains maintained 92.2% of its highest efficiency after light soaking under 1-sun illumination for 1900 hours at 55°C open-circuit condition.

     
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  2. Understanding carrier recombination processes in metal halide perovskites is fundamentally important to further improving the efficiency of perovskite solar cells, yet the accurate recombination velocity at grain boundaries (GBs) has not been determined. Here, we report the determination of carrier recombination velocities at GBs (SGB) of polycrystalline perovskites by mapping the transient photoluminescence pattern change induced by the nonradiative recombination of carriers at GBs. Charge recombination at GBs is revealed to be even stronger than at surfaces of unpassivated films, with averageSGBreaching 2200 to 3300 cm/s. Regular surface treatments do not passivate GBs because of the absence of contact at GBs. We find a surface treatment using tributyl(methyl)phosphonium dimethyl phosphate that can penetrate into GBs by partially dissolving GBs and converting it into one-dimensional perovskites. It reduces the averageSGBby four times, with the lowestSGBof 410 cm/s, which is comparable to surface recombination velocities after passivation.

     
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  3. Abstract

    High‐performance tin‐lead perovskite solar cells (PSCs) are needed for all‐perovskite‐tandem solar cells. However, iodide related fast photodegradation severely limits the operational stability of Sn‐Pb perovskites despite the demonstrated high efficiency and thermal stability. Herein, this work employs an alkylammonium pseudo‐halogen additive to enhance the power conversion efficiency (PCE) and photostability of methylammonium (MA)‐free, Sn‐Pb PSCs. Density functional theory (DFT) calculations reveal that the pseudo‐halogen tetrafluoroborate (BF4) has strong binding capacity with metal ions (Sn2+/Pb2+) in the Sn‐Pb perovskite lattice, which lowers iodine vacancy formation. Upon combining BF4with an octylammonium (OA+) cation, the PCE of the device with a built‐in light‐scattering layer is boosted to 23.7%, which represents a new record for Sn‐Pb PSCs. The improved efficiency benefits from the suppressed defect density. Under continuous 1 sun illumination, the OABF4embodied PSCs show slower generation of interstitial iodides and iodine, which greatly improves the device photostability under open‐circuit condition. Moreover, the device based on OABF4retains 88% of the initial PCE for 1000 h under the maximum‐power‐point tracking (MPPT) without cooling.

     
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  4. Abstract

    Layered perovskites have been employed for various optoelectronic devices including solar cells and light‐emitting diodes for improved stability, which need exciton transport along both the in‐plane and the out‐of‐plane directions. However, it is not clear yet what determines the exciton transport along the in‐plane direction, which is important to understand its impact toward electronic devices. Here, by employing both steady‐state and transient photoluminescence mapping, it is found that in‐plane exciton diffusivities in layered perovskites are sensitive to both the number of layers and organic cations. Apart from exciton–phonon coupling, the octahedral distortion is revealed to significantly affect the exciton diffusion process, determined by temperature‐dependent photoluminescence, light‐intensity‐dependent time‐resolved photoluminescence, and density function theory calculations. A simple fluorine substitution to phenethylammonium for the organic cations to tune the structural rigidity and octahedral distortion yields a record exciton diffusivity of 1.91 cm2s−1and a diffusion length of 405 nm along the in‐plane direction. This study provides guidance to manipulate exciton diffusion by modifying organic cations in layered perovskites.

     
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  5. Abstract

    Tailoring the doping of semiconductors in heterojunction solar cells shows tremendous success in enhancing the performance of many types of inorganic solar cells, while it is found challenging in perovskite solar cells because of the difficulty in doping perovskites in a controllable way. Here, a small molecule of 4,4′,4″,4″′‐(pyrazine‐2,3,5,6‐tetrayl) tetrakis (N,N‐bis(4‐methoxyphenyl) aniline) (PT‐TPA) which can effectively p‐dope the surface of FAxMA1−xPbI3(FA: HC(NH2)2; MA: CH3NH3) perovskite films is reported. The intermolecular charge transfer property of PT‐TPA forms a stabilized resonance structure to accept electrons from perovskites. The doping effect increases perovskite dark conductivity and carrier concentration by up to 4737 times. Computation shows that electrons in the first two layers of octahedral cages in perovskites are transferred to PT‐TPA. After applying PT‐TPA into perovskite solar cells, the doping‐induced band bending in perovskite effectively facilitates hole extraction to hole transport layer and expels electrons toward cathode side, which reduces the charge recombination there. The optimized devices demonstrate an increased photovoltage from 1.12 to 1.17 V and an efficiency of 23.4% from photocurrent scanning with a stabilized efficiency of 22.9%. The findings demonstrate that molecular doping is an effective route to control the interfacial charge recombination in perovskite solar cells which is in complimentary to broadly applied defect passivation techniques.

     
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