Abstract
Following photodissociation of dimethyl disulfide (CH3SSCH3) in a supersonic jet with a KrF excimer laser at 248 nm, degenerate four-wave mixing spectra of the A 2A1←X 2E3/2 transition of CH3S in a spectral region 317–377 nm are recorded using a dye laser. Observed features extend to 5020 cm−1 above the origin, much greater than 1490 cm−1 for fluorescence spectra and 2979 cm−1 for fluorescence depletion spectra. In addition to extension to higher members of the known progressions 3v and 213v associated with C–S stretching (ν3) and CH3 umbrella (ν2) modes, three new progressions 113v, 3v41, and 213v41 (or 11213v) involving the symmetric CH3 stretching (ν1) and asymmetric CH3 (ν4) stretching modes of the A 2A1 state of CH3S are tentatively assigned, yielding values of ν1=2966 cm−1 and ν4=3006 cm−1 that are consistent with theoretical predictions. Vibrational spectral parameters for ν1, ν2, ν3, and ν4 modes of the A 2A1 state of CH3S are derived.
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