Vibronic structure of CCS in the à [sup 3]Π[sub i] state studied by laser-induced fluorescence spectroscopy

Nakajima, Masakazu; Sumiyoshi, Yoshihiro; Endo, Yasuki
November 2002
Journal of Chemical Physics;11/22/2002, Vol. 117 Issue 20, p9327
Academic Journal
Laser-induced fluorescence spectrum of the Ã[SUP3]π[SUBi]←&Xtilde;[SUP3]Σ[SUP-] transition of the CCS radical has been studied in a discharged supersonic jet of a mixture gas, carbon disulfide and acetylene diluted in Ar. More than 40 vibronic bands in the 600-925 nm region have been assigned to the transitions from the ground vibronic level of the CCS radical. The progression of the C-C stretching mode was identified for v[SUB1] = 1-4, and the harmonic frequency of the mode was determined to be 1840.13(1) cm[SUP-1]. In addition to the perpendicular bands, Σ-Σ parallel-type bands have been observed and assigned to vibronically forbidden transitions, Ã(v[SUB1],0,1 )←&Xtilde;(0,0,0). Based on the positions of the bands, the harmonic frequency and the Renner parameter of the bending mode in the Ã[SUP3]π[SUBi] state were determined to be 399.00(3) cm[SUP-1] and -0.23467(7), respectively. High-level ab initio calculations were performed to compare the results with the experimentally determined vibronic parameters. Since the band at 778 nm has a complicated rotational structure due to the overlap of vibronic levels, a microwave-optical double-resonance method using a Fourier-transform microwave spectrometer and a pulsed laser was applied to obtain a definite rotational assignment.


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