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Metathesis reactions designed to produce nominally the pseudo-ternary  A Tl[N(CN) 2 ] 2  compounds ( A  = Li, Na, K, Rb or Cs) either yielded solid solutions or separated pseudo-binary dicyanamides next to the new compounds LiTl[N(CN) 2 ] 2  and Tl 0.89(1) Cs 0.11(1) [N(CN) 2 ]. Tetragonal LiTl[N(CN) 2 ] 2  ( a  = 724.96(2),  c  = 1411.77(6) pm,  Z  = 4) is crystallizing isotypically with LiK[N(CN) 2 ] 2  in the space group  I 4/ mcm , while orthorhombic Tl 0.89(1) Cs 0.11(1) [N(CN) 2 ] ( a  = 858.19(4),  b  = 654.22(2),  c  = 738.94(4) pm,  Z  = 4) adopts the  α -K[N(CN) 2 ]-type structure in the space group  Pbcm , which Tl[N(CN) 2 ] itself also assumes, with the unique cationic position shared by Tl +  and Cs +  in an approximate 9:1 molar ratio. The Raman spectra of the new compounds are presented and compared to those of Tl[N(CN) 2 ], LiK[N(CN) 2 ] 2  and LiRb[N(CN) 2 ] 2 .

About the pseudo-ternary alkali metal-thallium(I) dicyanamide systems