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Defects play an important role in the degradation processes of hybrid halide perovskite absorbers, impeding their application for solar cells. Among all defects, halide anion and organic cation vacancies are ubiquitous, promoting ion diffusion and leading to thin-film decomposition at surfaces and grain boundaries. Here, we employ fluoride to simultaneously passivate both anion and cation vacancies, by taking advantage of the extremely high electronegativity of fluoride. We obtain a power conversion efficiency of 21.46% (and a certified 21.3%-efficient cell) in a device based on the caesium, methylammonium (MA) and formamidinium (FA) triple-cation perovskite (Cs0.05FA0.54MA0.41)Pb(I0.98Br0.02)3 treated with sodium fluoride. The device retains 90% of its original power conversion efficiency after 1,000 h of operation at the maximum power point. With the help of first-principles density functional theory calculations, we argue that the fluoride ions suppress the formation of halide anion and organic cation vacancies, through a unique strengthening of the chemical bonds with the surrounding lead and organic cations. Defects and defect migration are detrimental for perovskite solar cell efficiency and long-term stability. Li et al. show that fluoride is able to suppress the formation of halide anion and organic cation vacancy defects by restraining the relative ions via ionic and hydrogen bonds.

Blending perovskite with different cations has been successful in improving performance of perovskite solar cells, but the complex pathway of perovskite crystal formation remains a mystery, hindering its further development. In this paper, the detailed crystallization process of formamidinium lead iodide (FAPbI3) perovskite films doped by methylammonium lead bromide (MAPbBr3) additive was investigated by in situ grazing incident wide-angle X-ray scattering measurements during both spin coating and annealing. During spin-coating, it was found that the FAPbI3 perovskite precursor easily formed a mixture of black perovskite phase (α phase) and non-perovskite yellow phase (δ phase) after the addition of MAPbBr3, whereas only δ phase formed without MAPbBr3. The δ phase gradually converted to α phase during annealing and there was only α phase left in both films with and without MAPbBr3. However, the doped films presented high film quality without PbI2 residue in contrast to the undoped films. These findings imply that the MAPbBr3 additive can effectively suppress the formation of the unfavorable δ phase and trigger the formation of the optically active α phase even during spin-coating, which enhances the film quality possibly by removing the energy barriers from δ phase to α phase at room temperature. Finally, PSCs based on MAPbBr3-doped FAPbI3 were fabricated with a champion efficiency as high as 19.4% from 14.2% for the PSCs based on undoped FAPbI3.

Bandgap tuning through mixing halide anions is one of the most attractive features for metal halide perovskites. However, mixed halide perovskites usually suffer from phase segregation under electrical biases. Herein, we obtain high-performance and color-stable blue perovskite LEDs (PeLEDs) based on mixed bromide/ chloride three-dimensional (3D) structures. We demonstrate that the color instability of CsPb(Br1-xClx)(3) PeLEDs results from surface defects at perovskite grain boundaries. By effective defect passivation, we achieve color-stable blue electroluminescence from CsPb(Br1-xClx)(3) PeLEDs, with maximum external quantum efficiencies of up to 4.5% and high luminance of up to 5351 cd m(-2) in the sky-blue region (489 nm). Our work provides new insights into the color instability issue of mixed halide perovskites and can spur new development of high-performance and color-stable blue PeLEDs. Funding Agencies|ERC Starting GrantEuropean Research Council (ERC) [717026]; Swedish Energy Agency EnergimyndighetenSwedish Energy Agency [48758-1, 44651-1]; Swedish Foundation for International Cooperation in Research and Higher Education [CH2018-7736]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [200900971]; China Scholarship CouncilChina Scholarship Council

Crystal orientations in multiple orders correlate to the properties of polycrystalline materials, and it is critical to manipulate these microstructural arrangements to enhance device performance. Herein, we report a controllable approach to manipulate the facet orientation within the ABX3 hybrid perovskites polycrystalline films by cation cascade doping at A-site. Two-dimensional synchrotron radiation grazing incidence wide-angle X-ray scattering is employed to probe the crystal orientations in multiple orders in mixed perovskites thin films, revealing a general pattern to guide crystal planes stacking upon extrinsic doping during crystallization. Different from previous studies, this method enables to adjust the crystal stacking mode of certain crystallographic planes in polycrystalline perovskites. Moreover, the preferred facet orientation is found to facilitate photocarrier transport across the absorber and pertaining interface in the resultant PV device, which provides an exemplary paradigm for further explorations that relate to the microstructures of hybrid perovskite materials and relevant optoelectronics., Crystal facet orientations of the polycrystalline hybrid lead halide perovskite thin films play a crucial role in determining the device performance. Here Zheng et al. demonstrate effective control of the crystal stacking mode by cation cascade doping, which promotes the charge transport in the photovoltaic device.