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We report fluorescence-dip as well as ion-dip spectra of single rovibronic one-photon states of benzene with a linewidth as narrow as 0.14 cm'1. The selective excitation of the rovibronic states was achieved through the combination of a frequency-doubled pulsed amplified cw dye laser (Avuv 100 MHz) and a collimated molecu- lar beam. The detailed analysis of the dip spectra shows that the observed spectral features correspond to single rovibronic transitions if suitable states are excited. From the spectra, precise harmonic frequencies and anharmonic constants for the So state are determined. A hitherto unknown Darling-Dennison resonance of the overtones of v, with the 52 state is found. In molecular spectroscopy the many rotational lines are assigned according to a given zero-order Hamiltonian to the various quantum numbers that are associated with ro- tation, and the spectroscopic parameters are then ex- tracted. In many cases deviations from line positions predicted by the Hamiltonian are seen as perturbations in the spectrum, and analyses of these can sometimes yield higher-order corrections to the Hamiltonian. These cor- rections or couplings between the different zero-order states of the molecule are also responsible for the redistri- bution of the vibrational or electronic energy of the molecule and give rise to the dynamics observed in time- resolved experiments. The interesting instances of the dynamics in the intermediate case or at the statistical limit leads to a completely perturbed spectrum, and a de- tailed analysis of the spectrum is nearly impossible. This is because the couplings between the zero-order states lead to a mixture of the wave functions, and therefore many more lines are observed in the spectrum than would be expected from considerations of regular selection rules. To identify the various lines in the spectrum according to the quantum numbers and to eliminate the many contri- butions from sequence congestion additional information are the purposes of the experiment.

Rotationally resolved fluorescence-dip and ion-dip spectra of single rovibronic states of benzene