The recent sky-rocketing performance of perovskite solar cells has triggered a strong interest in further upgrading the fabrication techniques to meet the scalability requirements of the photovoltaic industry. The integration of vapor-deposition into the solution process in a sequential fashion can boost the uniformity and reproducibility of the perovskite solar cells.Besides, mixed-halide perovskites have exhibited outstanding crystallinity as well as higher stability compared with iodide-only perovskite. An extensive study was carried out to identify a reproducible process leading to highly crystalline perovskite films that when integrated into solar cells exhibited high power conversion efficiency (max. 19.8%). This was achieved by optimizing the deposition rate of the PbI2 layer as well as by inserting small amounts of methylammonium (MA) bromide and chloride salts to the primary MAI salt in the solution-based conversion step. 3The optimum MABr/MAI molar ratio leading to the most efficient and stable solar cells was found to be 0.4. Stabilities were in excess of 90 hours for p-i-n type solar cells. This reproducible approach towards the fabrication of triple halide perovskites using a hybrid vapor-solution method is a promising method towards scalable production techniques.Recently, Rafizadeh et. al. used a hybrid vapor-solution method to fabricate planar MAPI-based devices with 18.9% efficiency in the n-i-p structure 26 . In that work, TiO2 was used as the Supporting Information.XRD, AFM, and, SEM of the PbI2 layer deposited at different rates, device statistical data depending on PbI2 deposition rate, XRD of MAPI-BrCl depending on MACl concentration, the effect of MABr/MAI ratio on the absorbance edge and on the Shockley-Queisser limit and average values of J-V parameters, stability analysis of the devices.
Vacuum processing of multicomponent perovskites is not straightforward, because the number of precursors is in principle limited by the number of available thermal sources. Herein, we present a process which allows increasing the complexity of the formulation of vacuum-deposited lead halide perovskite films by multisource deposition and premixing both inorganic and organic components. We apply it to the preparation of wide-bandgap CsMAFA triple-cation perovskite solar cells, which are found to be efficient but not thermally stable. With the aim of stabilizing the perovskite phase, we add guanidinium (GA + ) to the material formulation and obtained CsMAFAGA quadruple-cation perovskite films with enhanced thermal stability, as observed by X-ray diffraction and rationalized by microstructural analysis. The corresponding solar cells showed similar performance with improved thermal stability. This work paves the way toward the vacuum processing of complex perovskite formulations, with important implications not only for photovoltaics but also for other fields of application.
A series of copper(I) complexes of the type [Cu(HN‐xantphos)(N^N)][PF6] and [Cu(BnN‐xantphos)(N^N)][PF6], in which N^N = bpy, Mebpy, and Me2bpy, HN‐xantphos = 4,6‐bis(diphenylphosphanyl)‐10H‐phenoxazine and BnN‐xantphos = 10‐benzyl‐4,6‐bis(diphenylphosphanyl)‐10H‐phenoxazine is described. The single crystal structures of [Cu(HN‐xantphos)(Mebpy)][PF6] and [Cu(BnN‐xantphos)(Me2bpy)][PF6] confirm the presence of N^N and P^P chelating ligands with the copper(I) atoms in distorted coordination environments. Solution electrochemical and photophysical properties of the BnN‐xantphos‐containing compounds (for which the highest‐occupied molecular orbital is located on the phenoxazine moiety) are reported. The first oxidation of [Cu(BnN‐xantphos)(N^N)][PF6] occurs on the BnN‐xantphos ligand. Time‐dependent density functional theory (TD‐DFT) calculations have been used to analyze the solution absorption spectra of the [Cu(BnN‐xantphos)(N^N)][PF6] compounds. In the solid‐state, the compounds show photoluminescence in the range 518–555 nm for [Cu(HN‐xantphos)(N^N)][PF6] and 520–575 nm for [Cu(BnN‐xantphos)(N^N)][PF6] with a blue‐shift on going from bpy to Mebpy to Me2bpy. [Cu(BnN‐xantphos)(Me2bpy)][PF6] exhibits a solid‐state photoluminescence quantum yield of 55% with an excited state lifetime of 17.4 µs. Bright light‐emitting electrochemical cells are obtained using this complex, and it is shown that the electroluminescence quantum yield can be enhanced by using less conducting hole injection layers.
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