Lead-free double perovskites Cs₂InCuCl₆ and (CH₃NH₃)₂InCuCl₆: electronic, optical, and electrical properties

Searching for alternatives to lead-containing metal halide perovskites, we explored the properties of indium-based inorganic double perovskites Cs₂InMX₆ with M = Cu, Ag, Au and X = Cl, Br, I, and of its organic-inorganic hybrid derivative MA₂InCuCl₆ (MA = CH₃NH₃⁺) using computation within Kohn-Sham density functional theory. Among these compounds, Cs₂InCuCl₆ and MA₂InCuCl₆ were found to be potentially promising candidates for solar cells. Calculations with different functionals provided the direct band gap of Cs₂InCuCl₆ between 1.05 and 1.73 eV. In contrast, MA₂InCuCl₆ exhibits an indirect band gap between 1.31 and 2.09 eV depending on the choice of exchange-correlation functional. Cs₂InCuCl₆ exhibits a much higher absorption coefficient than that calculated for c-Si and CdTe, common semiconductors for solar cells. Even MA₂InCuCl₆ is predicted to have a higher absorption coefficient than c-Si and CdTe across the visible spectrum despite the fact that it is an indirect band gap material. The intrinsic charge carrier mobilities for Cs₂InCuCl₆ along the L-Γ path are predicted to be comparable to those for MAPbI₃. Finally, we carried out calculations of the band edge positions for MA₂InCuCl₆ and Cs₂InCuCl₆ to offer guidance for solar cell heterojunction design and optimization. We conclude that Cs₂InCuCl₆ and MA₂InCuCl₆ are promising semiconductors for photovoltaic and optoelectronic applications.