Transient Valence Charge Localization in Strong-Field Dissociative Ionization of HCl Molecules.

Probing transient charge localization in the innershell orbital of atoms and molecules has been made possible by the recent progress of advanced light sources. Here, we demonstrate that the ultrafast electron tunneling ionization by an intense femtosecond laser pulse could induce an asymmetric transient charge localization in the valence shell of the HCl molecule during the dissociative ionization process. The transient charge localization is encoded in the laser impulse acquired by the outgoing ionic fragments, and the asymmetry is revealed by carefully examining the electron tunneling-site distinguished momentum angular distribution of the ejected H^{+} fragments. Our work proposes a way to visualize the transient valence charge motion and will stimulate further investigations of the tunneling-site-sensitive ultrafast dynamics of molecules in strong laser fields.