Both Raman and Li-7 NMR spectroscopic data of 0.2 M LiAlCl4 and LiGaCl4 in liquid sulfur dioxide indicate that ionic structural changes occur near 25-degrees-C, thus supporting observations from conductivity and cyclic voltammetric studies. The solvation number of the lithium cation is 4 for both salts of interest. The activation energies of spin-lattice relaxation, the formation constants of lithium ion pairs, and the chemical shifts due to the free lithium ions and lithium ion pairs of LiAlCl4 and LiGaCl4 in sulfur dioxide are presented.
