Abstract
The two-photon excitation spectrum of the 1Au(S1)–1Ag(S0) transition in trans-glyoxal is observed in the region of 21 800–25 400 cm−1. The excitation source is the H2 Raman shifted output of a pulsed dye laser. The source yields tunable output from 0.7 to 1.4 μm and enables both one- and two-color two-photon spectra to be observed. These spectra are complementary to the well known one-photon spectra for this transition. However, the two-photon selection rules cause much of the vibrational structure to be simplified. Many of the observed bands belong to the torsional mode, ν7, revealing vibrational quanta up to 12 in the excited state and 8 in the ground state. The two-photon rotational contours for a number of transitions are calculated for comparison with the observed spectra.
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