Hydrazine solution processed Sb2S3, Sb2Se3 and Sb2(S1−xSex)3 film: molecular precursor identification, film fabrication and band gap tuning

Sb2(S(1-x)Se(x))3 (0 ≤ x ≤ 1) compounds have been proposed as promising light-absorbing materials for photovoltaic device applications. However, no systematic study on the synthesis and characterization of polycrystalline Sb2(S(1-x)Se(x))3 thin films has been reported. Here, using a hydrazine based solution process, single-phase Sb2(S(1-x)Se(x))3 films were successfully obtained. Through Raman spectroscopy, we have investigated the dissolution mechanism of Sb in hydrazine: 1) the reaction between Sb and S/Se yields [Sb4S7](2-)/[Sb4Se7](2-) ions within their respective solutions; 2) in the Sb-S-Se precursor solutions, Sb, S, and Se were mixed on a molecular level, facilitating the formation of highly uniform polycrystalline Sb2(S(1-x)Se(x))3 thin films at a relatively low temperature. UV-vis-NIR transmission spectroscopy revealed that the band gap of Sb2(S(1-x)Se(x))3 alloy films had a quadratical relationship with the Se concentration x and it followed the equation Eg(x) = 0.118x(2) - 0.662x + 1.621eV, where the bowing parameter was 0.118 eV. Our study provides a valuable guidance for the adjustment and optimization of the band gap in hydrazine solution processed Sb2(S(1-x)Se(x))3 alloy films for the future fabrication of improved photovoltaic devices.