Preferred Film Orientation to Achieve Stable and Efficient Sn-Pb Binary Perovskite Solar Cells

The preferred orientation of crystalline films in hybrid perovskite materials is known to influence the performance of perovskite solar cells (PSCs). Although the preferred growth along the (112) directions has been reported to promote charge transport within the Pb-based polycrystalline perovskite films, the preferred orientation growth of this facet is still difficult to be achieved due to the higher formation energy compared with the (110) plane. Herein, Sn-Pb binary perovskite films with a well-controlled orientation along the (224) plane were achieved by introducing a simple ultrasonic treatment (UST) into the additive engineering fabricated method. UST is used to process the perovskite precursor solutions of tartaric acid (TA) modified Sn-Pb binary polycrystalline perovskite films to regulate the interactions between PbI₂/SnI₂ and TA in the intermediate phases. Meanwhile, TA-modulated MA_0.9Cs_0.1Pb_0.75Sn_0.25I₃-based perovskite films with a preferred orientation of (224) crystal plane were obtained by precisely controlling the UST time to 15 min. The highest power conversion efficiency (PCE) of 15.59% with less hysteresis and improved stability was achieved, while realizing 8.64 and 25.32% enhancements of PCE compared with that of TA-based and control counterparts with (110) preferred orientation, respectively. Our work provides a promising route to obtain preferred orientation growth of polycrystalline perovskite films. In particular, we have shown that this approach improves the performance of Sn-Pb binary PSCs, while such methodology is quite flexible and could also be applied to other low-/non-toxic PSCs.