Correlation effects in strongfield ionization of heteronuclear diatomic molecules
Abstract
We develop a timedependent theory to investigate electron dynamics and photoionization processes of diatomic molecules interacting with strong laser fields including electronelectron correlation effects. We combine the recently formulated timedependent generalizedactivespace configuration interaction theory [D. Hochstuhl and M. Bonitz, Phys. Rev. A 86, 053424 (2012), 10.1103/PhysRevA.86.053424; S. Bauch et al., Phys. Rev. A 90, 062508 (2014), 10.1103/PhysRevA.90.062508] with a prolate spheroidal basis set including localized orbitals and continuum states to describe the bound electrons and the outgoing photoelectron. As an example, we study the strongfield ionization of the twocenter fourelectron lithium hydride molecule in different intensity regimes. By using singlecycle pulses, two orientations of the asymmetric heteronuclear molecule are investigated: LiH, with the electrical field pointing from H to Li, and the opposite case of HLi. The preferred orientation for ionization is determined and we find a transition from HLi, for low intensity, to LiH, for high intensity. The influence of electron correlations is studied at different levels of approximation, and we find a significant change in the preferred orientation. For certain intensity regimes, even an interchange of the preferred configuration is observed, relative to the uncorrelated simulations. Further insight is provided by detailed comparisons of photoelectron angular distributions with and without correlation effects taken into account.
 Publication:

Physical Review A
 Pub Date:
 January 2016
 DOI:
 10.1103/PhysRevA.93.013426
 arXiv:
 arXiv:1507.04107
 Bibcode:
 2016PhRvA..93a3426L
 Keywords:

 Physics  Chemical Physics;
 Physics  Computational Physics;
 Quantum Physics;
 8108
 EPrint:
 Phys. Rev. A 93, 013426 (2016)