Two novel halogeno(cyano)argentates(I), [Et4N]3[Ag6(CN)3.39Br5.61] (1) and [Pp4N]3[Ag8(CN)4I7] (2) (Et4N = tetra-ethylammonium, Pp4N = tetra-n-propylammonium), were obtained by the solvothermal reaction of silver(I) cyanide with tetraalkylammonium salts in anhydrous THF. Complex 1 presents a 2-D grid-like sheet built by [Ag6Br5]+ clusters bridged by cyanide groups. Complex 2 is the first example of 3-D halogeno(cyano)argentates(I), and displays a porous framework with fluorite (flu) topology based on [Ag4I4] and an unprecedented [Ag8I6]2+ cluster, respectively, as 4-connected and 8-connected nodes. The optical and luminescent properties of the two complexes have been investigated. On the basis of Time-dependent Density Functional Theory calculations, the emission spectrum of 1 can be assigned as metal-centred (MC) transitions, while the luminescence behavior for 2 is assumed to arise from metal-to-ligand charge-transfer (MLCT) transitions.
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