Attosecond strobing of two-surface population dynamics in dissociating H2+

Using H2+ and D2+, we observe two-surface population dynamics by measuring the kinetic energy of the correlated ions that are created when H2+ (D2+) ionize in short (40-140 fs) and intense (10(14) W/cm2) infrared laser pulses. Experimentally, we find a modulation of the kinetic energy spectrum of the correlated fragments. The spectral progression arises from a hitherto unexpected spatial modulation on the excited state population, revealed by Coulomb explosion. By solving the two-level time-dependent Schr?dinger equation, we show that an interference between the net-two-photon and the one-photon transition creates localized electrons which subsequently ionize.