Spectroscopy and Dynamics of Open-Shell Complexes

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In this project supported by the Experimental Physical Chemistry Program of the Chemistry Division, Heaven will continue his studies of the spectroscopy and dynamics of the pre-reactive van der Waals complexes H2-CN and CN-HCl. He will use fluorescence excitation and optical-optical double resonance techniques to probe the ro-vibronic structures of H2(D2)-CN(A) and -N(B). In particular, he will examine the predissociation dynamics of the A state complex. In addition, Heaven will investigate vibrationally excited levels of H2(D2)-CN(X) using stimulated emission pumping (SEP) and stimulated Raman excitation (SRE) techniques. In collaboration with Morokuma and Bowman, Heaven proposes to calculate ab initio potential energy surfaces for the ground and excited states of CN-H2. Finally, he proposes studies of the predissociation dynamics of CN-Rg and (N2+)-Rg (Rg= Ne or Ar). The study of weakly bound van der Waals complexes is one of the frontier areas of contemporary physical chemistry. While numerous van der Waals complexes formed by stable (called `closed shell`) molecules have been investigated, the study of such complexes in which one of the component members is a radical (molecular fragment or `open shell` system) is still in its early stages. Theoretical models developed for the bonding interactions in closed shell van der Waals complexes are not applicable to open shell systems. This research provides an important data base for open shell van der Waals complexes that aids the development of theoretical models of these systems. The results of this research are of direct relevance to work on collisional processes involving open shell diatomics which is currently pursued in several laboratories and have applications in atmospheric and industrial processes.