CAREER: Investigating Ultrafast Electronic and Structural Dynamics During Light-Driven Chemical Reactions

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This project will develop new experimental tools for imaging ultrafast dynamics during photochemical reactions in molecules. This will enable new studies of light-induced reactions that are important in several scientific areas. For example, photochemical dissociation reactions play a major role in atmospheric chemistry. Light-induced molecular ring-opening and isomerization reactions also serve as prototypes for understanding biosynthesis of vitamin D, controlling the dynamics of organic molecular switches, and engineering novel light-harvesting materials. Imaging and controlling such reactions at the electronic level can therefore lead to the development of new technologies with potential benefits to society. This project will engage students from diverse backgrounds and foster their interest in basic science and technology disciplines by introducing them early in their academic career to scientific research. Students will benefit from a variety of research environments ranging from a state-of-the-art laser laboratory at a university to large-scale user facilities operated at national laboratories.To further the understanding of the ultrafast electronic and structural dynamics occurring during light-driven reactions, this project will use femtosecond light sources combined with powerful detection techniques such as coincident electron and ion momentum imaging and time-resolved photoelectron spectroscopy. These tools will be used to study isomerization and ring-opening reactions in organic molecules with chemical relevance. Femtosecond pump-probe techniques with laboratory-based femtosecond lasers and high-order harmonic generation sources will be complemented by experiments with free-electron lasers. Being able to record "molecular movies" of benchmark photochemical reactions will allow for a more direct comparison to quantum chemistry calculations. The aim is to provide a better understanding of the underlying reaction mechanism and to develop and optimize schemes for controlling the dynamics and outcome of such reactions.This project is jointly funded by the Atomic, Molecular, and Optical Physics Experiment program in the Division of Physics and the Chemical Measurement and Imaging program in the Division of Chemistry (both Divisions are in the NSF Directorate for Mathematical and Physical Sciences) as well as the Established Program to Stimulate Competitive Research.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.