Nuclear Interference in the Coulomb Explosion of H2+ in Short vuv Laser Fields

We report ab initio calculations of H-2(+) three-photon ionization by vuv/fs 10(12) W/cm(2) laser pulses including electronic and vibrational degrees of freedom in the Born-Oppenheimer approximation. The initial nuclear wave packet of H-2(+)(1s sigma(g)) is assumed to be equal to the H-2 vibrational ground state. For pulse durations longer than 10 fs, we find an unexpected modulation in the kinetic energy spectra of the correlated fragments (H++H+). It is shown that the structures in the spectra originate from the interference between a direct and a sequential dissociation channel. While the first channel is open even for relatively short pulses, the sequential one only opens for pulse durations longer than 10 fs. In the latter case we show that interference between the two components results in a modulated kinetic energy release spectrum in the dissociation channel 3d sigma(g), which is reflected in the ionization spectrum.