Theoretical Dissection of Cation-Deficient Layered Ruddlesden-Popper Oxysulfide Perovskites with a High-Efficiency Carrier Transport Channel

The search for lead-free perovskite materials has triggered intensive interest. Here, we study the electronic structures and optical properties of cation-deficient Ruddlesden-Popper oxysulfide perovskites Ln(2)Ti(2)O(5)S(2) (Ln = Sc, Y, or La), with a tunable band gap of 1.45-2.1 eV and a small exciton binding energy of similar to 0.1 eV, among which Y2Ti2O5S2 has been synthesized experimentally. Sc2Ti2O5S2 possesses the largest light absorbance in the visible region. We further rationalize the light absorption via the transition dipole moment and suggest potential applications of Sc2Ti2O5S2 in solar cells and Y2Ti2O5S2 and La2Ti2O5S2 in water splitting. In addition, this family exhibits small effective masses within the x-y plane and large ones along the z direction. Most importantly, electron gas-like carrier behaviors are observed within the Ti-O bond region, offering a diffusion channel for electron transport. These findings greatly advance our understanding of lead-free perovskites and offer a novel material platform for future optoelectronic devices.