Professor Miller is supported by the Experimental Physical Chemistry Program in experimental investigations on both the dynamics and spectroscopy of a variety of neutral binary, tertiary, and higher order molecular complexes. Information is obtained on the structures of these complexes and on the flow of energy between various internal and translational (dissociative) degrees of freedom for vibrationally-excited complexes. Opto-thermal detection techniques are used to measure photofragment angular distributions and obtain state-to-state photodissociation cross sections following vibrational excitation of one molecule in a complex. Results are yielding insight into rotational state correlations between two departing photofragment molecules and also give accurate values for the complex dissociation energies. Extensions are planned that will allow probing of higher vibrational states of both these complexes and stable molecules through a two laser IR-IR double resonance experiment. For the complexes, the double resonance technique will also allow measurements of predissociation lifetimes in real time.
