Abstract
Large single crystals of Li2(Ca3N)2[Ga4] and Li2(Sr3N)2[Ga4] up to several mm in size were grown from mixtures of the respective elements and binary alkaline‐earth metal nitrides in reactive lithium melts employing a modified high‐temperature centrifugation‐aided filtration (HTCAF) technique. The main structural features of these isotypic phases are stella quadrangula building units [Ga4]Li4/2 and octahedra (Nae6/2), which form two independent interpenetrating networks. The phases crystallize in the η‐carbide structure and represent diamagnetic small bandgap semiconductors. Real‐space chemical bonding analysis indicates predominantly ionic bonding.
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