Exploring new perovskite-related solid-state materials and the investigating composition-dependent structural and physical properties are highly important for advanced functional material development. Herein, we present the successful hydrothermal synthesis of tetragonal CsPbCl and the anion-exchange phase formation of CsPb(ClBr ) ( x = 0-1) solid solutions. The CsPb(ClBr ) crystal structures, which crystallize in the tetragonal system, space group I4/ mcm, with parameters similar to those of CsPbCl, have been determined by Rietveld analysis. The optical band gap was obtained by UV-vis spectroscopy, and the band structure was further calculated by the full-potential method within the generalized gradient approximation. It was revealed that the band gap in CsPb(ClBr ) solid solutions can be tuned over the range of 4.5-3.8 eV by anion substitution.
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