High-Resolution Imaging of Photodissociation Dynamics in Ions and Neutral Molecules

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Arthur Suits and Oleg Vasyutinskii of Wayne State University are supported by the Experimental Physical Chemistry Program to carry out high-resolution ion imaging studies of photochemical processes in both ionic and neutral molecular systems. The objectives are to understand multi-surface dynamics and nonadiabatic processes in polyatomic systems; to examine coherent effects in photodissociation; to explore features of the ground and excited-state potential energy surfaces; to reveal unusual reaction mechanisms; to obtain accurate branching fractions for multi-channel processes and explore the dynamical issues controlling this branching; and to benchmark electronic structure and dynamical calculations for these challenging problems. These studies will exploit the recently developed reflectron multimass imaging apparatus to study conformationally- and vibrationally-mediated dissociation of ions, a new direction that promises insights into the light-driven dynamics of polyatomic systems. In parallel with the ion photodissociation studies, atomic orbital polarization in polyatomic systems will be used to investigate atomic and molecular interactions in unique detail. Detailed investigations of the complete angular momentum polarization, including contributions from higher moments, will be used to unravel the decay dynamics in cases were several excited electronic states play a role. Concurrently, new theoretical descriptions of these phenomena will be developed so that a direct connection can be made between the experiment and a complete quantum description of the polyatomic photodissociation process. Outcomes from this research are anticipated to lead to major insights into how chemical reactions occur at the highest detail, and may compel substantial changes in how presumably statistical molecular dissociations are described. This project will provide challenging research opportunities for a diverse group of students and postdocs. As well, the technological and software advances that result will be shared freely with numerous research groups.