We demonstrate how the evolution of a bound vibrational wave packet can be controlled by a strong field laser pulse. We consider two different control schemes within the same molecule (CH(2)BrI): reshaping of the wave packet via strong field population transfer ("hole burning"), and redirecting its trajectory by dressing the potential energy surface on which the wave packet evolves ("photon locking"). Our measurements are compared with calculations using wave packet propagation on ab initio potential energy surfaces.
We follow the evolution of a vibrational wave packet in a highly excited state of the halogenated methane CH 2 I 2. We observe how the wave packet modulates both dissociation and concerted elimination to form CH 2 I + and I 2 + , respectively. We present a simple and intuitive interpretation of the molecular dynamics leading to the formation of the products.
We explore strong field molecular ionization with velocity map imaging of fragment ions produced by dissociation following ionization. Our measurements and ab initio electronic structure calculations allow us to identify various electronic states of the molecular cation populated during ionization, with multiple pathways to individual states highlighted by the pulse shape dependence. In addition, we show that relative populations can be reconstructed from our measurements. The results illustrate how strong field molecular ionization can be complicated by the presence and interaction of multiple cationic states during ionization.
We use ultrafast laser pulse shaping to discriminate between different pathways to multiple continua in strong field molecular ionization. Shaping the laser pulse which ionizes the molecule allows us to control the photoelectron spectrum, which we interpret using a newly developed model of resonantly enhanced multiphoton ionization. Our measurements and calculations allow us to distinguish between a single intermediate resonance leading to multiple continua and multiple intermediate resonances each leading to a separate continuum.
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