Highly Efficient and Stable Sn-Rich Perovskite Solar Cells by Introducing Bromine.

Compositional engineering of recently arising methylammonium (MA) lead (Pb) halide based perovskites is an essential approach for finding better perovskite compositions to resolve still remaining issues of toxic Pb, long-term instability, etc. In this work, we carried out crystallographic, morphological, optical, and photovoltaic characterization of compositional MASn0.6Pb0.4I3-xBrx by gradually introducing bromine (Br) into parental Pb-Sn binary perovskite (MASn0.6Pb0.4I3) to elucidate its function in Sn-rich (Sn:Pb = 6:4) perovskites. We found significant advances in crystallinity and dense coverage of the perovskite films by inserting the Br into Sn-rich perovskite lattice. Furthermore, light-intensity-dependent open circuit voltage (Voc) measurement revealed much suppressed trap-assisted recombination for a proper Br-added (x = 0.4) device. These contributed to attaining the unprecedented power conversion efficiency of 12.1% and Voc of 0.78 V, which are, to the best of our knowledge, the highest performance in the Sn-rich (≥60%) perovskite solar cells reported so far. In addition, impressive enhancement of photocurrent-output stability and little hysteresis were found, which paves the way for the development of environmentally benign (Pb reduction), stable monolithic tandem cells using the developed low band gap (1.24-1.26 eV) MASn0.6Pb0.4I3-xBrx with suggested composition (x = 0.2-0.4).