Abstract
The dissociative ionization of N2O by near-single-cycle laser pulses is studied using phase-tagged ion–ion coincidence momentum imaging. Carrier–envelope phase (CEP) dependences are observed in the absolute ion yields and the emission direction of nearly all ionization and dissociation pathways of the triatomic molecule. We find that laser-field-driven electron recollision has a significant impact on the dissociative ionization dynamics and results in pronounced CEP modulations in the dication yields, which are observed in the product ion yields after dissociation. The results indicate that the directional emission of coincident and ions in the denitrogenation of the dication can be explained by selective ionization of oriented molecules. The deoxygenation of the dication with the formation of coincident + ions exhibits an additional shift in its CEP dependence, suggesting that this channel is further influenced by laser interaction with the dissociating dication. The experimental results demonstrate how few-femtosecond dynamics can drive and steer molecular reactions taking place on (much) longer time scales.
Highlights
The interplay between electronic and nuclear motion is at the heart of chemical reactions
The carrier–envelope phase (CEP) control of molecular dynamics has been predominantly investigated for diatomic molecules in both experiment and theory [5, 8]
These studies have established that the control may involve the following CEP-dependent processes: (1) the laser ionization and excitation of the molecule, (2) field-driven electron recollision dynamics leading to further ionization and excitation, and (3) the laser dressing and laser-induced coupling of states
Summary
The interplay between electronic and nuclear motion is at the heart of chemical reactions. We extend the studies on complex systems and investigate the CEP dependence of the dissociative ionization of N2O molecules in strong, near-single-cycle laser fields. The enhancement of the double ionization of N2O after the formation of highly excited, autoionizing states of the cation by an extreme ultraviolet pulse through a timedelayed infrared pulse was investigated by Zhou et al [33] They found that the highly excited, inner–valence ionized N2O+* molecular ions decay rapidly through autoionization or dissociation in about 20 fs. We directly compare the dynamics of N+ formation to that of the competing O+ channel, taking advantage of our coincident detection scheme
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