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

TL;DR

This paper introduces a grid-based implementation of the time-dependent configuration-interaction singles method for modeling strong-field ionization in small molecules, demonstrating its effectiveness through calculations on several molecules.

Contribution

It presents a novel grid-based computational approach for the time-dependent CI singles method applied to molecular ionization, expanding the toolset for strong-field molecular physics.

Findings

Successful implementation for small molecules

Accurate modeling of strong-field ionization processes

Demonstrated utility on multiple molecular systems

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 helium, lithium hydride, water, and ethylene that demonstrate the utility of our implementation. The following companion paper specializes to the case of spherical symmetry, which is applied to various atoms.