Hidden spontaneous polarisation in the chalcohalide photovoltaic absorber Sn2SbS2I3

Perovskite-inspired materials aim to replicate the optoelectronic performance of lead-halide perovskites, while eliminating issues with stability and toxicity. Chalcohalides of group IV/V elements have attracted attention due to enhanced stability provided by stronger metal-chalcogen bonds, alongside compositional flexibility and ns(2) lone pair cations - a performance-defining feature of halide perovskites. Following the experimental report of solution-grown tin-antimony sulfoiodide (Sn2SbS2I3) solar cells, with power conversion efficiencies above 4%, we assess the structural and electronic properties of this emerging photovoltaic material. We find that the reported centrosymmetric Cmcm crystal structure represents an average over multiple polar Cmc2(1) configurations. The instability is confirmed through a combination of lattice dynamics and molecular dynamics simulations. We predict a large spontaneous polarisation of 37 mu C cm(-2) that could be active for electron-hole separation in operating solar cells. We further assess the radiative efficiency limit of this material, calculating eta(max) > 30% for film thicknesses t > 0.5 mu m.

Automated summary

Perovskite-inspired materials aim to replicate the optoelectronic performance of lead-halide perovskites, while eliminating issues with stability and toxicity. Experimental results show that Sn2SbS2I3 solar cells have power conversion efficiencies above 4% and a large spontaneous polarization value, which could be active for electron-hole separation in operating solar cells.