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The degradation rate of CH3NH3PbI3 perovskite films, made by a known deposition method, is found to be roughly proportional to the grain size.

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Two-dimensional (2D) halide perovskites have recently been recognized as a promising avenue in perovskite solar cells (PSCs) in terms of encouraging stability and defect passivation effect. However, the efficiency (less than 15%) of ultra-stable 2D Ruddlesden-Popper PSCs still lag far behind their traditional three-dimensional (3D) perovskite counterparts. Here, we report a rationally designed 2D-3D perovskite stacking-layered architecture by in-situ growing 2D PEA 2 PbI 4 capping layers on top of 3D perovskite film, which drastically improved the stability of PSCs without compromising their high performance. Such 2D perovskite capping layer induces larger Fermi-level splitting in the 2D-3D perovskite film under light illumination, resulting in an enhanced open-circuit voltage (V oc ) and thus a higher efficiency of 18.51% in the 2D-3D PSCs. The time-resolved photoluminescence (TRPL) decay measurements indicate the facilitated hole-extraction in the This article is protected by copyright. All rights reserved. 22D-3D stacking-layered perovskite films, which is ascribed to the optimized energy band alignment and reduced non-radiative recombination at the sub gap states. Benefiting from the high moisture resistivity as well as suppressed ion migration of the 2D perovskite, the 2D-3D PSCs show significantly improved long-term stability, retaining nearly 90% of the initial PCE after 1000 h exposure in the ambient conditions with a high relative humidity level of 60±10%.

The mixed caesium and formamidinium lead triiodide perovskite system (Cs1-xFAxPbI3) in the form of quantum dots (QDs) offers a new pathway towards stable perovskite-based photovoltaics and optoelectronics. However, it remains challenging to synthesize such multinary QDs with desirable properties for high-performance QD solar cells (QDSCs). Here we report an effective ligand-assisted cation exchange strategy that enables controllable synthesis of Cs1-xFAxPbI3 QDs across the whole composition range (x: 0-1), which is inaccessible in large-grain polycrystalline thin films. The surface ligands play a key role in driving the cross-exchange of cations for the rapid formation of Cs1-xFAxPbI3 QDs with suppressed defect density. The hero Cs0.5FA0.5PbI3 QDSC achieves a certified record power conversion efficiency (PCE) of 16.6% with negligible hysteresis. We further demonstrate that QD devices exhibit substantially enhanced photostability compared to their thin film counterparts because of the suppressed phase segregation, retaining 94% of the original PCE under continuous 1-sun illumination for 600 hours.