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A new statistical analysis of spatially resolved photocurrent and electroluminescence images has been developed and applied to Cu2ZnSn(SxSe1−x)4 (CZTSSe) monograin solar cells. CZTSSe as an absorber material has the potential to significantly reduce manufacturing costs and develop new application fields in photovoltaics. Deep understanding of the performance related parameters in various production steps is crucial for further development of the technology. In this paper we show that by a thorough investigation by means of a combination of opto‐electrical measurement methods such as light beam induced current mapping, scanning electron microscopy, optical microscopy, photoluminescence, and electroluminescence measurements a correlation with different current‐voltage (j/V) measurement parameters can be established. Hereby, we clearly identify barrier variations at the active interface as the main reason for current variations across the cell, which for record cells can largely be avoided. These variations show up clearly in the microscopic spatial analysis developed. The detailed analysis of the homogeneity of the solar cell photocurrent presented in this study is relevant for all kinds of solar cells including thin‐film and wafer‐based cells.

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Although photovoltaic is one the most promising solution for the future power supply in the world, the issue of storing it is still an open problem. Photoelectrochemical (PEC) cells, which convert solar energy into storable chemical energy directly, is one of the solutions of the storage problem in photovoltaics. In this paper the preparation of freestanding monograin membranes for use in PECs and their characterization is described. The manufacturing process in terms of reproducibility semiconductor particle densities and accessibility for contact formation is optimized. Here especially the etching process reducing the thickness of the polymer film and thereby exposing more of the monograin particles required attention since the etching temperature plays an important role determining the thickness of the. Whereas monograin layer solar cells as yet require particles of at least 45 m diameter, the monograin membrane process developed here allows to produce such membranes from particles as yet down to 38-45 m diameter, open and accessible from both sides.