Abstract
The notion that strong laser light can intervene and modify the dynamical processes of matter has been demonstrated and exploited both in gas and condensed phases. The central objective of laser control schemes has been the modification of branching ratios in chemical processes, under the philosophy that conveniently tailored light can steer the dynamics of a chemical mechanism towards desired targets. Less explored is the role that strong laser control can play on chemical stereodynamics, i.e. the angular distribution of the products of a chemical reaction in space. This work demonstrates for the case of methyl iodide that when a molecular bond breaking process takes place in the presence of an intense infrared laser field, its stereodynamics is profoundly affected, and that the intensity of this laser field can be used as an external knob to control it.
Highlights
The notion that strong laser light can intervene and modify the dynamical processes of matter has been demonstrated and exploited both in gas and condensed phases
When a light field of high intensity is added, the matter states become “dressed by light” and we move into the field of laser control, or, from an alternative view, the dynamics in the presence of strong laser fields, a theme that has experienced tremendous advances over recent years
CH3 ion images, as a function of time delay, which reveals the exponential growth derived from the 1.5 ± 0.1 ps lifetime[35] of the initially populated Rydberg state. 3D plot insets correspond to a polar representation of the angular distribution at positions A
Summary
The notion that strong laser light can intervene and modify the dynamical processes of matter has been demonstrated and exploited both in gas and condensed phases. The angular distribution of fragments resulting from a molecular bond breaking process induced by linearly polarized light reveals the preferential directions of fragment ejection in the laboratory frame These are only a faithful reflection of the nature of the transition that causes dissociation in the axial recoil limit and in the absence of fragment alignment. The three mentioned ingredients (preferential molecular excitation due to the nature of the transition, loss of anisotropy due to rotation of the molecular axis during dissociation, and fragment alignment) contribute to the observed reaction stereodynamics Even though these complex molecular processes are lightinduced, the description of their dynamics is essentially field-free, in the sense that they are governed by the molecular Hamiltonian. Significant work has been devoted to create asymmetries in the fragment spatial distributions by the introduction of asymmetric laser fields, either few-cycle carrier envelope phase (CEP)-stabilized fields[25], or bichromatic fields with relative phase control[26, 27]
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