Abstract
Electron–ion coincidence detection allows one to visualize the ultrafast chemical reactions of molecules in strong laser fields. Here, by measuring the photoelectron angular distribution (PAD) of H2 in strong laser fields correlated to different pathways, i.e., direct ionization when the internuclear distance is small, or ionization after the molecular bond stretches to a large internuclear distance, we uncover the roles of the molecular orientation and internuclear distance in the dissociative ionization of H2. As compared to the first dissociation pathway, the regular nodal structures on the concentric above-threshold ionization circles vanish for the second pathway, which are numerically validated by the quantum simulations. Pathway-resolved PADs assisted by electron–ion coincidence detection open new possibilities to probe the rich dynamics of molecules in strong laser fields, in particular to image the instantaneous geometry of molecules.
Highlights
Single- and multiphoton-ionization of atoms and molecules in external fields have been well studied to probe the electronic and nuclear dynamics [1,2,3]
The photoelectron angular distribution (PAD) [4] of the above threshold ionization (ATI) in the multiphoton ionization regime manifests itself as multiple concentric circles shaped with regular nodal structures [5,6,7,8]
In this Letter, by resolving the multiphoton ATI of H2 into various dissociation pathways, we observe distinct PADs driven by an intense femtosecond laser pulse
Summary
Single- and multiphoton-ionization of atoms and molecules in external fields have been well studied to probe the electronic and nuclear dynamics [1,2,3]. We observe distinct PADs correlated to the post-ionization dissociation and stretched-bond ionization pathways.
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