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Riedle, Eberhard ORCID logoORCID: https://orcid.org/0000-0002-2672-5718; Neusser, H. J. and Schlag, E. W. (1983): Sub-Doppler Spectroscopy of Benzene in the "Channel-three" Region. In: Faraday Discussions of the Chemical Society, Vol. 75: pp. 387-394 [PDF, 657kB]


In addition to an increased accuracy in the determination of structural parameters sub- Doppler spectroscopy of large molecules is shown to render valuable information about intramolecular processes and relaxation mechanisms. As an example we have measured the Doppler-free rotationally resolved two-photon spectrum of two vibronic bands of CsHs, 1461; and 14i1;. Compared with the 14i1: band (EcxE :,:=css 2492 cm-') a drastically reduced number of sharp lines is observed in the 14i1; band (Eence=ss 3 412 cm-I). The X = 0 rotational lines are still seen, while K # 0 lines disappear. This can be understood in terms of Coriolis coupling between the 14'1' state and other vibrational states within S1 and a subsequent om-radiative process. This coupling might be the explanation for the drastic onset of line broadening in C6H6 at an excess energy of 3000 cm-', " channel three." The line broadening is then due to a different process from that responsible for the population lifetime of s1.

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