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Abstract Renewable energy sources, in particular, photovoltaic solar cells and hydrogen fuel, are expected to be the pillars of a sustainable society. Chalcopyrite CuGaSe 2 (CGSe) has potential for using in such applications. This article presents efficient solar cells suitable as top cells for tandem devices and highly active photocathodes for solar hydrogen evolution using CGSe photoabsorber layers with modified p–n heterointerfaces. Rb‐doping during the last stage of CGSe film growth effectively improves the photovoltaic performance, and solar cell efficiency of >10% with a high fill factor (FF) of 74.6% is obtained. The half‐cell solar‐to‐hydrogen conversion efficiency reaches 8% with the use of a photocathode composed of a CGSe film grown in an identical growth batch. Interface modification with i) a Cu‐deficient layer, ii) alkali‐metal doping, and iii) an n‐type buffer layer formed on the CGSe film surface is found to a be key to control the energy conversion device parameters, such as the FF and open circuit voltage of solar cells and the onset potential of photoelectrochemical cells, due to the suppression of interface recombination.
Ishizuka et al. (2022) studied this question.