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Fourfold coordination of trivalent metal ions by chlorines in molecular dimers changes from tetrahedral in Al 2  Cl 6  and Fe 2 Cl 6  to planar in Au 2 Cl 6 . Within an ionic model we interpret this transition in the stable molecular shape as due to the quadrupolar polarizability of the gold(III) ion. We also demonstrate within the same model that a mixed tetrahedral-planar coordination is stable in AUAlCl 6  and AuFeCl 6  clusters. Quantitative comparisons are presented for the calculated molecular structures and vibrational frequencies against the available experimental data from crystalline diffraction and from Raman spectra of the crystal and of vapours.

Static and Dynamic Structure of AU 2 Cl 6 , AUAlCl 6 and AuFeCl 6 Clusters