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Trans-glyoxal molecules in a seeded pulsed jet were laser-excited into selected vibrational levels of the T 1  and S 1  states. In the latter case, those specific rovibrational levels were chosen which exhibit S 1 /T 1  gateway coupling. In each case, the long-lived emission into the S 0  state was observed employing a spectrograph/CCD combination, covering 5000 cm -1  at 60 cm -1  FWHM resolution. A model Franck–Condon calculation of the relative ν 5  band intensities demonstrates the structural similarities of  the S 1  and T 1  states. However, there are some distinct differences, despite the almost identical S 1  and T 1  vibrational frequencies. The S 1 ← S 0  excitation distorts the molecule significantly more in the ν 5  dimension than does T 1 ← S 0 .

Spectrally Resolved Phosphorescence and Slow Fluorescence from Selected Vibronic Levels of Jet-Cooled Glyoxal