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Quasi-2D perovskites are stable alternative materials for solar cells, but achieving high performance requires precise control over crystal orientation during film fabrication. Using real-time and angle-dependent X-ray scattering techniques, the crystallisation dynamics during spin-coating and annealing were investigated. The analysis reveals that an unwanted lead iodide sol-gel intermediate phase disrupts ordered crystal growth, leading to random crystal orientation that impairs film quality. By introducing a simple additive agent during processing, this disruptive intermediate phase is suppressed. This targeted intervention yields highly oriented perovskite films with fewer defects, lower trap density, and higher charge carrier mobility. Consequently, solar cell devices fabricated with these optimised films achieved an improved power conversion efficiency of 15.2% alongside enhanced operational stability, offering a clear pathway to control crystallisation in next-generation photovoltaic materials.
Perovskite solar cells promise cheaper, high-efficiency renewable energy, but instability and inconsistent film quality have slowed widespread adoption. By identifying the exact mechanism that causes structural defects during manufacturing and offering a straightforward chemical solution, this research helps make next-generation solar devices both more efficient and durable.
This method applies directly to perovskite solar cell manufacturing, offering photovoltaic hardware developers a practical additive strategy to boost efficiency and lifespan. Operating at laboratory device scale, the technology has reached a working cell efficiency of 15.2%, placing it at an early stage of applied research that requires further scale-up beyond spin-coating to reach commercial viability.
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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.
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DOI: 10.1002/smll.202100972
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