RUI: Momentum Imaging Studies of Controlled Molecular Fragmentation

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A variety of chemical processes have been controlled in recent years using closed loop schemes involving shaped laser pulses. For all but the most basic systems, however, it has proved challenging to deconstruct the optimal laser pulse to recover information about the molecular dynamics involved in the laser-molecule interaction. On the other hand, momentum imaging techniques can produce rich, correlated, multi-dimensional data that has led to significant advances in our understanding of many photon- and ion-molecule interactions. The program of research described in this proposal would use momentum imaging to probe the molecular fragmentation dynamics arising from optimized laser pulses. By combining numerical analysis capable of reducing the optimal pulse shape to its essential features with a posteriori reconstruction of the dynamics afforded by momentum imaging, we hope to deduce the control mechanism(s). Specifically, the PI proposes to identify interesting "optimal" pulses for selective molecular fragmentation using closed-loop control and then use momentum imaging to investigate the control mechanisms produced by these pulses. Information gleaned from the imaging measurements will also be used to explore the interesting topology of the multidimensional surface that defines the optimal control parameters.