RESUMO
Quasi-2D perovskites are enchanting alternative materials for solar cells due to their intrinsic stability. The manipulation of crystal orientation of quasi-2D perovskites is indispensable to target efficient devices, however, the origin of orientation during the film fabrication process still lacks in-depth understanding and convincing evidence yet, which hinders further boosting the performance of photovoltaic devices. Herein, the crystallizing processes during spin-coating and annealing are probed by in situ grazing-incidence wide-angle X-ray scattering (GIWAXS), and the incident-angle-dependent GIWAXS is conducted to unveil the phase distribution in the films. It is found that undesirable lead iodide sol-gel formed intermediate phase would disturb oriented crystalline growth, resulting in random crystal orientation in poor quasi-2D films. A general strategy is developed via simple additive agent incorporation to suppress the formation of the intermediate phase. Accordingly, highly oriented perovskite films with reduced trap density and higher carrier mobility are obtained, which enables the demonstration of optimized quasi-2D perovskite solar cells with a power conversion efficiency of 15.2% as well as improved stability. This work paves a promising way to manipulate the quasi-2D perovskites nucleation and crystallization processes via tuning nucleation stage.
RESUMO
A considerable efficiency gap exists between large-area perovskite solar modules and small-area perovskite solar cells. The control of forming uniform and large-area film and perovskite crystallization is still the main obstacle restricting the efficiency of PSMs. In this work, we adopted a solid-liquid two-step film formation technique, which involved the evaporation of a lead iodide film and blade coating of an organic ammonium halide solution to prepare perovskite films. This method possesses the advantages of integrating vapor deposition and solution methods, which could apply to substrates with different roughness and avoid using toxic solvents to achieve a more uniform, large-area perovskite film. Furthermore, modification of the NiOx/perovskite buried interface and introduction of Urea additives were utilized to reduce interface recombination and regulate perovskite crystallization. As a result, a large-area perovskite film possessing larger grains, fewer pinholes, and reduced defects could be achieved. The inverted PSM with an active area of 61.56 cm2 (10 × 10 cm2 substrate) achieved a champion power conversion efficiency of 20.56% and significantly improved stability. This method suggests an innovative approach to resolving the uniformity issue associated with large-area film fabrication.
RESUMO
Despite tremendous developments in the luminescene performance of perovskite light-emitting diodes (PeLEDs), the brittle nature of perovskite crystals and their poor crystallinity on flexible substrates inevitably lead to inferior performance. Inspired by pangolins' combination of rigid scales and soft flesh, we propose a bionic structure design for self-healing flexible PeLEDs by employing a polymer-assisted crystal regulation method with a soft elastomer of diphenylmethane diisocyanate polyurethane (MDI-PU). The crystallinity and flexural strain resistance of such perovskite films on plastics with silver-nanowire-based flexible transparent electrodes are highly enhanced. The detrimental cracks induced during repeated deformation can be effectively self-healed under heat treatment via intramolecular/intermolecular hydrogen bonds with MDI-PU. Upon collective optimization of the perovskite films and device architecture, the blue-emitting flexible PeLEDs can achieve a record external quantum efficiency of 13.5% and high resistance to flexural strain, which retain 87.8 and 80.7% of their initial efficiency after repeated bending and twisting operations of 2000 cycles, respectively.