Sub-10-fs control of dissociation pathways in the hydrogen molecular ion with a few-pulse attosecond pulse train

The control of the electronic states of a hydrogen molecular ion by photoexcitation is considerably difficult because it requires multiple sub-10 fs light pulses in the extreme ultraviolet (XUV) wavelength region with a sufficiently high intensity. Here, we demonstrate the control of the dissociation pathway originating from the 2 pσ u electronic state against that originating from the 2 pπ u electronic state in a hydrogen molecular ion by using a pair of attosecond pulse trains in the XUV wavelength region with a train-envelope duration of ∼4 fs. The switching time from the peak to the valley in the oscillation caused by the vibrational wavepacket motion in the 1 sσ g ground electronic state is only 8 fs. This result can be classified as the fastest control, to the best of our knowledge, of a molecular reaction in the simplest molecule on the basis of the XUV-pump and XUV-probe scheme. Attosecond laser pulses allow to explore the ultrafast atomic or molecular processes occurring in chemical reactions. Here the authors utilize a sequence of two XUV pump-probe pulses to control the dissociation dynamics of the hydrogen molecular ion.