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A series of complexes of ruthenium(II) with the strong -acceptor ligand 2-(phenylazo)pyridine (Azpy), [Ru(Azpy)2(AB)]"+, have been prepared. The coligands (AB) include Azpy, 2,2'-bipyridyl, 4,4'-bithiazole, 1,2-diaminoethane, 2,4-pentanedione anion, and X2 (X = N02", CN", Br", N3", and thiourea). Infrared spectra show the Azpy azo stretching mode to be diagnostic of the coligand (AB) -accepting behavior, with strongly -accepting coligands giving the highest Azpy y(N=N). Visible spectra of the complexes consist of intense charge-transfer bands; the first CT band is not found to be a valid criterion for Ru-ligand bonding. It is proposed that both and effects are important, causing the observed nonlinear behavior. Emission spectra could be obtained for three of the compounds, one compound appearing to give multiple emissions. Cyclic voltammetry data support the strong stabilization. Oxidation to Ru(III) could be observed in only a few complexes.However, all reduce at relatively high potentials, with RuAzpy32+ reducing near 0 V (vs.SCE). A new thin-layer chromatography technique for cationic ruthenium complexes has been developed.