AbstractInfrared spectra of reaction mixtures of methyl methacrylate or methacrylonitrile with an equimolar amount of organometallic compounds were investigated in relation to the stereoregulating ability of the catalysts in polymerization. It was found that the carbonyl or nitrile stretching frequency correlated with the stereoregularity of polymers prepared with the corresponding catalysts; i.e., the higher the frequency, the higher the isotacticity. From these results a mechanism of isotactic polymer formation was proposed, in which catalyst counterion was located near the carbonyl group in polymer terminal and that of monomer to be reacted, and consequently the isotactic polymerization is facilitated.