Raman spectra of Mg(CIO,),-NaNCS-H,O mixtures were analysed as a function of the concentration ratio of the components at ambient and elevated temperatures. The strong perturbation of the thiocyanate spectrum observed in the regions of the v, and v3 vibrations is interpreted in terms of complex formation. Band intensity measurements of resolved bands gave evidence for two complex species: (MgNCS]' and [Mg(NCS),], the former being discernible over the whole concentration range studied. The variations in the spectrum of the Td perchlorate ion at very low water-to-salt molar ratios are explained as indicating a coordination of C10,-unit and lowering of the symmetry of C,, .

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