The smallest ketenimine and hydrogen cyanide N-methylide (CH 2 CNH and CH 2 NCH) are provided from the argon/acetonitrile matrix samples exposed to radiation from laser ablation of transition-metals. New infrared bands are observed in addition to better determination of the vibrational characteristics for the previously reported bands, and the 13 C substituted isotopomers ( 13 CH 2 13 CNH and 13 CH 2 N 13 CH) are also generated. Density functional frequency calculations and the D and 13 C

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... ic shifts substantiate the vibrational assignments. CH 2 CNH is probably produced through single-step conversion of CH 3 CN, whereas CH 2 NCH through two-step conversion via 2H-azirine. Inter-conversions between these two products evidently do not occur during photolysis and annealing.