Additive-Assisted Hydrothermal Growth Enabling Defect Passivation and Void Remedy in Antimony Selenosulfide Solar Cells.

Antimony selenosulfide (Sb2(S,Se)3) has recently emerged as a promising light-absorbing material, attributed to its tunable photovoltaic properties, low toxicity, and robust environmental stability. However, despite these advantages, the current record efficiency for Sb2(S,Se)3 solar cells significantly lags behind their Shockley-Queisser limit, especially when compared to other well-established chalcogenide-based thin-film solar cells, such as CdTe and Cu(In,Ga)Se2. This underperformance primarily arises from the formation of unfavorable defects, predominately located at deep energy levels, which act as recombination centers, thereby limiting the potential for performance enhancement in Sb2(S,Se)3 solar cells. Specifically, deep-level defects, such as sulfur vacancy (VS), have a lower formation energy, leading to severe non-radiative recombination and compromising device performance. To address this challenge, thioacetamide (TA), a sulfur-containing additive is introduced, into the precursor solution for the hydrothermal deposition of Sb2(S,Se)3. This results indicate that the incorporation of TA helps in passivating deep-level defects such as sulfur vacancies and in suppressing the formation of large voids within the Sb2(S,Se)3 absorber. Consequently, Sb2(S,Se)3 solar cells, with reduced carrier recombination and improved film quality, achieved a power conversion efficiency of 9.04%, with notable improvements in open-circuit voltage and fill factor. This work provides deeper insights into the passivation of deep-level donor-like VS defects through the incorporation of a sulfur-containing additive, highlighting pathways to enhance the photovoltaic performance of Sb2(S,Se)3 solar cells.

Comprehensive rear surface passivation of superstrate Sb2Se3 solar cells via post-deposition selenium annealing treatments and the application of an electron blocking layer.

Sb2Se3, a quasi-1D structured binary chalcogenide, has great potential as a solar cell light absorber owing to its anisotropic carrier transport and benign grain boundaries when the absorber layer is properly aligned along the [hk1] direction perpendicular to the substrate. A growth technique with a high deposition rate, such as vapor transport deposition, is preferred to form an [hk1]-oriented Sb2Se3 film. However, the possible decomposition of Sb2Se3 during cooling after the high-temperature deposition appears to result in Se deficiency, accompanied by the formation of deep-level donor-like defects, such as Se vacancies and Sb on Se antisite defects. Here, we present comprehensive passivation strategies for the rear interface of Sb2Se3 solar cells in a superstrate configuration, namely a post-deposition annealing treatment (PAT) under Se, and the introduction of an electron-blocking layer between Sb2Se3 and the rear metal contact. The PAT effectively passivated the defects associated with Se deficiency and greatly improved the open-circuit voltage and fill factor of Sb2Se3 solar cells. With the further introduction of a poly(N,N-bis(4-butylphenyl)-N,N-bis(phenyl)benzidine) electron-blocking layer, the Sb2Se3 solar cell achieved an efficiency of 7.0%.