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The laser induced dispersed fluorescence spectra (LIDFS) of CH 3 N radical from five different vibronic excited levels were recorded and assigned. The anharmonic constants of the ν″ 3 (CN stretching) mode were determined to be ω 0 = 1049 ± 2 cm −1 , ω 0 ξ 0 = 9 ± 0.5 cm −1 . The previous tentative assignment of 1 0 1 band in the excitation spectrum [J. Chem. Phys. 103 (1995) 4418] was confirmed by LIDFS. The lifetimes of different vibrational levels of the A 3 E state were measured and the radiative lifetimes of ν ′ = 0, ν ′ 3 = 1, ν ′ 2 = 1, ν ′ 3 = 2, ν ′ 3 = 3 and ν ′ 1 = 1 states were extrapolated as 415 ± 8, 341 ± 10, 231 ± 18, 219 ± 9, 170 ± 3 and 166 ± 7 ns, respectively.

The photolysis of methylazide around 313 nm is studied experimentally by laser Raman spectroscopy. The emission spectrum with a resolution of 50 cm−1 is reported. Based on our experiments, the photodissociation of methylazide on its first excited singlet surface is proposed to be a concerted N2 elimination and 1,2-H shift process.