Timing Dissociative Ionization of H2 Using a Polarization-Skewed Femtosecond Laser Pulse

We experimentally observe the bond stretching time of one-photon and net-two-photon dissociation pathways of singly ionized H2 molecules driven by a polarization-skewed femtosecond laser pulse. By measuring the angular distributions of the ejected photoelectron and nuclear fragments in coincidence, the cycle-changing polarization of the laser field enables us to clock the photon-ionization starting time and photon-dissociation stopping time, analogous to a stopwatch. After the single ionization of H2, our results show that the produced H2+ takes almost the same time in the one-photon and net-two-photon dissociation pathways to stretch to the internuclear distance of the one-photon coupled dipole-transition between the ground and excited electronic states. The spatiotemporal mapping character of the polarization-skewed laser field provides us a straightforward route to clock the ultrafast dynamics of molecules with sub-optical-cycle time resolution.