Laser Spectroscopy of Excited States in Atmospheric Molecules

Abstract : The principal objectives of this project were to systematically investigate the structure and dynamics of molecular Rydberg states using high resolution laser spectroscopy. We have established a new laser facility for this purpose, and have used it to accomplish several initial projects. Using laser double resonance, we have made a systematic study of Rydberg state energy level structure and autoionization in the NO molecule, particularly in the nf states. A simple theoretical model was devised, based on the long-range interaction between the molecular ion core and the excited Rydberg electron, that accurately describes both electronic structure and autoionization rates in nonpenetrating Rydberg states. We have also obtained double resonance spectra of previously unknown excited states in CO, and have been able to characterize the 3 so state of O2 using photo-electron spectroscopy.