The stable crystal structures of two cuprous chalcogenides of ${\mathrm{Cu}}_{2}X$ ($X=\mathrm{Te}$ or Se) are predicted using an adaptive genetic algorithm in combination with first-principles density functional theory calculations. Both systems are found to prefer a unique and previously unrecognized layered structure, with the total energies much lower than all structures proposed in the literature so far. The newly discovered structures are further shown to be dynamically and mechanically stable, and possess electronic properties consistent with existing experimental observations. In particular, their layered nature is expected to prevail over other structural forms at the interfaces of thin-film solar cells, and knowledge about the precise atomic structures of the interfaces is a prerequisite for achieving long-term stability and high efficiency of CdTe and $\mathrm{Cu}(\mathrm{In},\mathrm{Ga}){\mathrm{Se}}_2$ solar cells.

• Received 27 March 2013

DOI:https://doi.org/10.1103/PhysRevLett.111.165502