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The binary Ru 4 Si 3  remained the only compound in its structure type for more than 60 years. Herein, we report the synthesis and crystal structure of the first ternary silicide (Ir 4− x  CuSi 2 ) in the Ru 4 Si 3 -type structure, which can be derived from RuSi by unit cell twinning. According to single-crystal X-ray diffraction, Ir vacancies exist along the twin boundary. Ir 4− x  CuSi 2  exhibits a distorted structure compared to Ru 4 Si 3 , as the larger Cu selectively replaces Si on only one of three possible sites, leading to zigzag chains with short Cu–Cu distances. Furthermore, DFT calculations show that the rigid band approximation does not apply to this structure type, but the similarities of electronic structures of the ideal binary and ternary compositions suggest that this structure type can accommodate a large variety of elemental substitutions without a significant change of its electronic structure if a similar valence electron count is maintained, hinting at a potentially rich substitutional chemistry.

Site-preferential copper substitution for silicon leads to Cu-chains in the new ternary silicide Ir 4− x CuSi 2