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Synthesis, structural characterization and chemical bonding peculiarities of two new quaternary selenides of the Tl 4 Sb 8 Sn 5 Se 24  and Tl 5 Sb 2 Sn 4 Se 14−x  (x = 0.5) are reported. The crystal structures of these compounds were determined by single crystal X-ray diffraction analysis. The Tl 4 Sb 8 Sn 5 Se 24  phase is a new structure type and crystallizes in the triclinic  P  1̅ space group ( a =  7.9061(13) Å,  b =  13.9035(16) Å,  c =  21.4665(17) Å, α = 80.058(8)°, β = 84.727(10)°, γ = 73.542(12)°, w R  2  = 0.0258, 8200  F  2  values, 373 variables). The Tl 5 Sb 2 Sn 4 Se 14−x  (x = 0.5) phase represents a new structure type with a tetragonal unit cell ( P  4 /mbm ,  a =  8.1570(10) Å,  c =  21.946(3) Å, w R  2  = 0.0346, 1953  F  2  values, 44 variables). Crystallographic analysis together with linear muffin-tin orbital band structure calculations reveals that both structures we conform to the concept of Zintl-Klemm and exhibit semiconductor properties.

New quaternary selenides Tl 4 Sb 8 Sn 5 Se 24 and Tl 5 Sb 2 Sn 4 Se 14−x (x=0.5)