One-Electron Ionization of Multielectron Systems in Strong Nonresonant Laser Fields

TL;DR

This paper introduces a new computational approach for modeling multielectron molecular ionization in strong laser fields, capturing complex electron dynamics and explaining experimental results.

Contribution

A novel multielectron wavefunction method based on coupled single-particle equations for strong field ionization of molecules.

Findings

Applied to CO₂, revealing the significance of core excitation.

Successfully explains discrepancies in experimental ionization yields.

Provides a versatile framework for multielectron strong field processes.

Abstract

We present a novel approach to calculating strong field ionization dynamics of multielectron molecular targets. Adopting a multielectron wavefunction ansatz based on field-free ab initio neutral and ionic multielectron states, a set of coupled time-dependent single-particle Schroedinger equations describing the neutral amplitude and continuum electron are constructed. These equations, amenable to direct numerical solution or further analytical treatment, allow one to study multielectron effects during strong field ionization, recollision, and high harmonic generation. We apply the method to strong field ionization of CO_2, and suggest the importance of intermediate core excitation to explain previous failure of analytical models to reproduce experimental ionization yields for this molecule.