Upper efficiency limit of Sb2Se3 solar cells

Abstract: Antimony selenide (Sb2Se3) is at the forefront of an emerging class of sustainable photovoltaic materials. Despite notable developments over the past decade, the light-to-electricity conversion efficiency of Sb2Se3 has reached a plateau of ~10%. Is this an intrinsic limitation of the material or is there scope to rival the success of metal halide perovskite solar cells? Here we assess the trap-limited conversion efficiency of Sb2Se3. First-principles defect analysis of the hole and electron capture rates for point defects demonstrates the critical role of vacancies as active recombination centres. We predict an upper limit of 25% efficiency in Sb2Se3 grown under optimal equilibrium conditions where the concentrations of charged vacancies are minimised. We further reveal how the detrimental effect of Se vacancies can be reduced by extrinsic oxygen passivation, highlighting a pathway to achieve high-performance metal selenide solar cells close to the thermodynamic limit.