Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV22)
Publication date: 20th April 2022
Heteroatom alloying of lead-free perovskite derivates was shown to be a highly promising route to circumvent some of the problems this class of materials faces for application as optoelectronic material. Here, we demonstrate the first, facile solution-based synthesis of Sn-alloyed layered MA3Sb2I9 thin films by precursor engineering, combining acetate and halide sources. An increasing concentration of tin halides in different oxidation states leads to a boost in absorption over the whole visible spectrum. We demonstrate phase pure synthesis with homogeneous thin film morphologies and elucidate the heterovalent incorporation of Sn into the MA3Sb2I9 lattice, proving the formation of additional states in the bandgap by theoretical calculations. With this, we dissect the absorption increase into three singular components which we attribute to Sn intervalence and Sb-Sn “defect-to-band” transitions. Finally, we show the charge-stabilizing effect of the system through robustness towards precursors in mixed oxidation states, discussing the ambiguous formal oxidation state and trace the improved ambient stability of this material back to this property.
The authors acknowledge funding from the Bavarian Network “Solar Technologies Go Hybrid”, the German Science Foundation (DFG) focus program SPP 2196 and the DFG Excellence Cluster e-conversion (EXC 2089/1-390776260). The authors thank Dr. Steffen Schmidt for performing the SEM measurements.