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An unprecedented pentanary chalcohalide with Mn atoms in two chemical environments: unique bonding characteristics and magnetic properties.

Mixed-anion chalcohalides have attracted significant attention lately, attributable to their unique structure compositions and captivating physicochemical properties. Herein, an unprecedented pentanary chalcohalide, Cs2[Mn2Ga3S7Cl] (1), was discovered by solid-state reaction at 1223 K. It is constructed by alternately stacked layers, each of which is made by a 2D [Ga3S9]9- ribbon embedded with 1D [Mn2S8Cl]13- chains. The coexistence of two Mn-coordinated polyhedra ([MnS6] octahedra and hetero-ligand [MnS3Cl] tetrahedra) in one material is surprisingly observed for the first time in the Mn-containing inorganic chalcogenides or chalcohalides. More interestingly, it exhibits ferrimagnetic (FIM) behaviour, which could be correlated to the magnetic sub-lattice sites with different coordination geometries. This work suggests a new route for designing and searching for unique functional chalcohalides with different chemical environments.