The effect of ultraviolet-ozone (UVO) irradiation on amorphous (am) SnO₂ and its impact on the photoconversion efficiency of MAPbI₃-based perovskite solar cells were investigated in detail. UVO treatment was found to increase the amount of chemisorbed oxygen on the am-SnO₂ surface, reducing the surface energy and contact angle. Physicochemical changes in the am-SnO₂ surface lowered the Gibbs free energy for the densification of perovskite films and facilitated the formation of homogeneous perovskite grains. In addition, the Fermi energy of the UVO-treated am-SnO₂ shifted upwards to achieve an ideal band offset for MAPbI₃, which was verified by theoretical calculations based on the density functional theory. We achieved a champion efficiency of 19.01 % with a statistical reproducibility of 17.01 ± 1.34 % owing to improved perovskite film densification and enhanced charge transport/extraction, which is considerably higher than the 13.78 ± 2.15 % of the counterpart. Furthermore, UVO-treated, am-SnO₂-based devices showed improved stability and less hysteresis, which is encouraging for the future application of up-scaled perovskite solar cells.

详细研究了紫外臭氧（UVO）辐照对非晶（am）SnO ₂的影响及其对基于MAPbI ₃的钙钛矿太阳能电池光转换效率的影响。发现UVO处理增加了am-SnO ₂表面上化学吸附的氧的量，从而降低了表面能和接触角。am-SnO ₂表面的物理化学变化降低了钙钛矿薄膜致密化的吉布斯自由能，并促进了均匀钙钛矿晶粒的形成。此外，经UVO处理的am-SnO ₂的费米能向上移动，以实现MAPbI ₃的理想带偏移，已通过基于密度泛函理论的理论计算得到验证。由于钙钛矿薄膜致密化的改善和电荷传输/萃取的增强，我们实现了19.01％的冠军效率和17.01±1.34％的统计可重复性，这大大高于同类产品的13.78±2.15％。此外，经UVO处理的基于am-SnO ₂的器件显示出更高的稳定性和更少的滞后性，这对于将来扩大规模的钙钛矿太阳能电池的应用是令人鼓舞的。