Ambient stability remains a critical hurdle for commercialization of perovskite solar cells. Two-dimensional Ruddlesden–Popper (RP) perovskite solar cells exhibit excellent stability but suffer from low photovoltaic performance so far. Herein, a RP/3D heterostructure passivated by semiconducting molecules is reported, which systematically addresses both charge dynamics and degradation mechanisms in concert for cesium-free FAPbI₃ solar cells, delivering a power-conversion efficiency as high as 20.62% and remarkable long-term ambient stability with a t₈₀ lifetime exceeding 2880 hours without encapsulation. In situ characterizations were carried out to gain insight into structural evolution and crystal growth mechanisms during spin coating. Comprehensive film and device characterizations were performed to understand the influences of the RP perovskite and molecule passivation on the film quality, photovoltaic performance and degradation mechanisms. This enables fabrication of a superior quality film with significantly improved optoelectronic properties, which lead to higher charge collection efficiency. The underlying mitigated degradation mechanisms of the passivated RP/3D devices were further elucidated. The understanding of the necessity of addressing both the charge dynamics and degradation mechanisms of solar cells will guide the future design and fabrication of chemically stable, high-efficiency photovoltaic devices.

中文翻译：

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具有分子钝化的Ruddlesden–Popper / 3D异质结构膜的 高性能环境空气稳定FAPbI ₃钙钛矿太阳能电池†

环境稳定性仍然是钙钛矿太阳能电池商业化的关键障碍。二维Ruddlesden-Popper（RP）钙钛矿型太阳能电池具有出色的稳定性，但迄今为止其光伏性能较低。本文报道了一种由半导体分子钝化的RP / 3D异质结构，该体系系统地解决了无铯FAPbI ₃太阳能电池的电荷动力学和降解机理，提供了高达20.62％的功率转换效率和出色的长期性能无封装的t ₈₀寿命超过2880小时具有良好的环境稳定性。原位进行表征以了解旋涂过程中的结构演变和晶体生长机理。进行了全面的膜和器件表征，以了解RP钙钛矿和分子钝化对膜质量，光伏性能和降解机理的影响。这使得能够制造具有显着改善的光电性能的高质量薄膜，从而导致更高的电荷收集效率。进一步阐明了钝化RP / 3D设备的潜在缓解机制。对解决太阳能电池的电荷动力学和降解机理的必要性的理解将指导化学稳定，高效的光伏器件的未来设计和制造。