Ti-Alloying of BaZrS₃ Chalcogenide Perovskite for Photovoltaics

BaZrS₃, a prototypical chalcogenide perovskite, has been shown to possess a direct band gap, an exceptionally strong near band edge light absorption, and good carrier transport. Coupled with its great stability, nontoxicity with earth-abundant elements, it is thus a promising candidate for thin film solar cells. However, its reported band gap in the range of 1.7-1.8 eV is larger than the optimal value required to reach the Shockley-Queisser limit of a single-junction solar cell. Here, we report the synthesis of Ba(Zr_1- Ti )S₃ perovskite compounds with a reduced band gap. It is found that Ti-alloying is extremely effective in band gap reduction of BaZrS₃: a mere 4 atom % alloying decreases the band gap from 1.78 to 1.51 eV, resulting in a theoretical maximum power conversion efficiency of 32%. Higher Ti-alloying concentration is found to destabilize the distorted chalcogenide perovskite phase.