Abstract
Abstract The isotypic title compounds ate obtained from reactions of stoichiometric mixtures of the elements in welded Ta containers at 700–800 °C. The structure of Na 2 BaSi 4 was determined by single-crystal X-ray diffraction (orthorhombic, Ima2 (No. 46), Z = 8, a = 9.524, b = 17.980(3), c = 8.570(3) A). The compound crystallizes in a novel structure type with Na + and Ba 2+ cations and two crystallographically-independent isolated Si 4 4− anions. The anions are nearly regular tetrahedra with bond distances of 2.385(3) to 2.448(4) A and bond angles between 59.2 and 61.7°. The overall structure may be described as a distorted face-centered-cubic array of Si 4 4− anions in which Na + and Ba 2+ atoms occupy all tetrahedral and octahedral holes in an ordered way. The result is closely related to the topology of f.c.c. Li 3 Bi type but with ordering of the two cations. Magnetic measurements showed that Na 2 BaSi 4 is diamagnetic, and its family can be formulated in terms of oxidation states as Zintl phases (Na + ) 2 Ba 2+ (Tt 4 4− ).
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