Abstract

We investigated the infrared multiphoton excitation of SO 2 in bulk samples and in a supersonic jet with the 9R(22), 9R(32), and 9P(32) CO 2-laser lines. Coherent anti-Stokes Raman spectra reveal unambiguously that only the ν 1-mode at 1151.3 cm −1 is actually pumped; no 2ν 2 overtone pumping at 1035.2 cm −1 is observed. From the spectra we directly determine the anharmonic constants χ 11 = −3.65 ± 0.06 cm −1 and χ 12 = −3.3 ± 0.3 cm −1.

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