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Assessment of Optimal Control Mechanism Complexity by Experimental Landscape Hessian Analysis: Fragmentation of CH2BrI

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Journal Article - Open Access

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Department of Chemistry, Princeton University Princeton United States

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Optimally shaped femtosecond laser pulses can often be effectively identified inadaptive feedback quantum control experiments, but elucidating the underlyingcontrol mechanism can be a difficult task requiring significant additional analysis.We introduce landscape Hessian analysis LHA as a practical experimentaltool to aid in elucidating control mechanism insights. This technique isapplied to the dissociative ionization of CH2BrI using shaped fs laser pulses foroptimization of the absolute yields of ionic fragments as well as their ratios forthe competing processes of breaking the CBr and CI bonds. The experimentalresults suggest that these nominally complex problems can be reduced to a lowdimensionalcontrol space with insights into the control mechanisms. While theoptimal yield for some fragments is dominated by a non-resonant intensitydrivenprocess, the optimal generation of other fragments maa difficult taskrequiring significant additionaly be explained by a non-resonant process coupledto few level resonant dynamics. Theoretical analysis and modeling is consistentwith the experimental observations.

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  • Quantum Theory and Relativity

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