General Time-Dependent Configuration-Interaction Singles II: The Atomic Case

TL;DR

This paper adapts a grid-based time-dependent configuration-interaction singles method to spherical symmetry, enabling detailed simulations of photoionization processes and matching experimental results.

Contribution

It provides a specialized implementation for spherical symmetry, detailing the time propagator and demonstrating its effectiveness with example calculations.

Findings

Accurate photoelectron spectra near Fano resonances in neon

Spin-polarized photoelectron results in xenon match experiments

Enhanced understanding of time-dependent photoionization processes

Abstract

We present a specialization of the grid-based implementation of the time-dependent configuration-interaction singles described in the preceding paper (arXiv:2204.09966) to the case of spherical symmetry. We describe the intricate time propagator in detail, and conclude with a few example calculations. Among these, of note are high-resolution photoelectron spectra in the vicinity of the Fano resonances in photoionization of neon, and spin-polarized photoelectrons from xenon, in agreement with recent experiments.