STATE-TO-STATE DYNAMICS IN THE HIGH RYDBERG STATES OF POLYATOMIC-MOLECULES

Rydberg states in polyatomic molecules exhibit dynamics that bear on i ssues of longstanding importance for theory. Coupling is made complica ted, however, by the presence of many rovibrational degrees of freedom and the existence of multiple pathways for intramolecular relaxation. In work on vibrationally autoionizing states of HCO and NO2, we have applied multiple resonance excitation strategies to isolate single rov ibrational Rydberg-Rydberg transition, the positions, lineshapes and i ntensities of which reflect coupling strengths for state-detailed rela xation processes.