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Control over the instantaneous electric field via e.g. the carrier-envelope phase (CEP) allows to directly access the complex electronic and subsequent nuclear dynamics of molecules. Very recently, we have demonstrated efficient control over fragmentation of polyatomic molecules via tuning the CEP of the few-cycle laser pulse [1]. The mechanism of control was based on fine tuning of electron impact energy of, resulting in ionization of the outermost or an inner valence electron.
In this talk, new experimental and theoretical data will be presented, extending the approach towards achieving channel-selective fragmentation, utilizing the alignment of the molecule relative to the polarization axis of the laser as an additional control tool [2]. Here, control is mainly introduced in the ionization step, as different molecular orbitals feature alignment-dependent contributions to the ionization. Results of our theoretical modeling, where not only the angular dependence of the molecular strong-field ionization step, but also the angular dependence of the re-collisional ionization step are addressed, will be presented.
[1] X. Xie, et al., "Attosecond recollision-controlled selective fragmentation of polyatomic molecules", Phys. Rev. Lett. 2012, 109, 243001.
[2] X. Xie, et al., "Selective control over fragmentation reactions in polyatomic molecules using impulsive laser alignment", Phys. Rev. Lett. 2014, 112, 163003
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