Correlation effects in strong-field ionization of heteronuclear diatomic molecules

Abstract

We develop a time-dependent theory to investigate electron dynamics and photoionization processes of diatomic molecules interacting with strong laser fields including electron-electron correlation effects. We combine the recently formulated time-dependent generalized-active-space configuration interaction theory [D. Hochstuhl and M. Bonitz, Phys. Rev. A 86, 053424 (2012); S. Bauch, et al., Phys. Rev. A 90, 062508 (2014)] 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 strong-field ionization of the two-center four-electron lithium hydride molecule in different intensity regimes. By using single-cycle pulses, two orientations of the asymmetric heteronuclear molecule are investigated: Li-H, with the electrical field pointing from H to Li, and the opposite case of H-Li. The preferred orientation for ionization is determined and we find a transition from H-Li, for low intensity, to Li-H, 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.

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Cited by in corpus (8)

• A review on non-relativistic fully numerical electronic structure calculations on atoms and diatomic molecules
• Ultrafast Dynamics of Strongly Correlated Fermions -- Nonequilibrium Green Functions and Selfenergy Approximations
• Electron correlation effects in enhanced-ionization of molecules:A time-dependent generalized-active-space configuration-interaction study
• Electron correlation effects in enhanced-ionization of diatomic molecules in near-infrared fields
• Comparing real-time coupled cluster methods through simulation of collective Rabi oscillations
• Multielectron effects in strong-field ionization of benzene derivatives
• Simulating real-time molecular electron dynamics efficiently using the time-dependent density matrix renormalization group
• Control of concerted back-to-back double ionization dynamics in helium