General Time-Dependent Configuration-Interaction Singles I: The Molecular Case

Abstract

We present a grid-based implementation of the time-dependent configuration-interaction singles method suitable for computing the strong-field ionization of small gas-phase molecules. After outlining the general equations of motion used in our treatment of this method, we present example calculations of strong-field ionization of He, LiH, H2O, and C2H4 that demonstrate the utility of our implementation. The following paper [S. Carlström et al., following paper, Phys. Rev. A 106, 042806 (2022)] specializes to the case of spherical symmetry, which is applied to various atoms.