To grind or not to grind? The influence of mechanical and thermal treatments on the Cu/Zn disorder in Cu2ZnSn(SxSe1-x)4 monograins

Kesterite-type based thin film solar cell technologies are mainly based on polycrystalline absorber layers. A promising low cost alternative technology uses Cu2ZnSn(SxSe1-x)(4) (CZTSSe) monograins (single crystals of 20-100 mu m size) which are fixed in a polymer matrix to form a flexible solar cell. The Cu/Zn disorder is discussed as a possible reason for band tailing causing voltage losses limiting the efficiency of CZTSSe-based devices. The experimental determination of the order parameter Q which is a quantitative measure of Cu/Zn disorder, requires a differentiation between the isoelectronic cations Cu+ and Zn2+. An in-depth analysis of neutron diffraction data allows the determination of type and concentration of intrinsic point defects including a distinction between Cu and Zn. Neutron diffraction requires large sample volumes, thus monograins offer the unique possibility to correlate structural disorder in CZTSSe with device performance parameters. In this study we tackle the influence of grinding the monograins on stoichiometry deviations, the Cu/Zn disorder as well as intrinsic point defects and optoelectronic properties of CZTSSe monograins. Moreover, an easy methodology based on Raman scattering spectroscopy is proposed for the assessment of Cu/Zn disorder in the CZTSSe compounds.

Automated summary

Kesterite-type thin film solar cell technologies based on polycrystalline absorber layers are commonly used. However, the use of Cu2ZnSn(SxSe1-x)(4) (CZTSSe) monograins in a polymer matrix offers a promising low cost alternative. In this study, neutron diffraction and Raman scattering spectroscopy were used to analyze the influence of Cu/Zn disorder, stoichiometry deviations, and intrinsic point defects on CZTSSe monograins.