Two-photon double photoionization of atomic Mg by ultrashort pulses: Variation of angular distributions with pulse length

Abstract

We investigate the two-photon double ionization of atomic magnesium induced by ultrashort pulses. Though the initial and final state symmetries are comparable to the same process in helium, in stark contrast the range of photon energies for which non-sequential ionization is the only open pathway is narrow (less than 1 eV) in magnesium. Thus, several sequential ionization pathways feature heavily in these processes. Nonetheless it is found that for pulse durations between 0.25 and 2.0 femtoseconds, the joint angular dependence of the ejected electrons can depend sensitively on pulse length, varying between the strictly back-to-back ejection characteristic of nonsequential ionization to other distributions. The significance of excited-state correlating configurations in representing the initial state of magnesium is discussed in the light of their consequences for the resulting angular distributions at photon energies where sequential ionization can access intermediate states that lie nearby in energy, particularly for longer pulses.