Ab Initio Modeling of CuGa1−xInxS2, CuGaS2(1−x)Se2x and Ag1−xCuxGaS2 Chalcopyrite Solid Solutions for Photovoltaic Applications

Chalcopyrites are ternary semiconductor compounds with successful applications in photovoltaics. Certain chalcopyrites are well researched, yet others remain understudied despite showing promise. In this study, we use ab initio methods to study CuGaS2, AgGaS2, and CuGaSe2 chalcopyrites with a focus on their less studied solid solutions. We use density functional theory (DFT) to study the effects that atomic configurations have on the properties of a solid solution and we calculate the optical absorption spectra using a many-body perturbation theory. Our theoretical simulations predict that excess of In and Se in the solid solutions leads to narrowing of the band gap and to the broadening of the absorption spectra. Obtained results show promise for possible photovoltaic applications, as well as developed methodology can be used for further study of other promising chalcopyritic compounds.