# Single-photon double ionization: renormalized-natural-orbital theory vs multi-configurational Hartree-Fock

## TL;DR

This paper compares the effectiveness of the renormalized-natural-orbital theory (TDRNOT) with multi-configurational Hartree-Fock (MCTDHF) and the full Schrödinger equation in modeling single-photon double ionization, highlighting TDRNOT's potential for accurate, reduced-dimensionality simulations.

## Contribution

It demonstrates the relation between TDRNOT and MCTDHF and evaluates their performance against the full Schrödinger equation for a specific ionization process.

## Key findings

- TDRNOT closely relates to MCTDHF in describing electron dynamics.
- TDRNOT outperforms TDDFT in modeling correlated photoelectron spectra.
- Both TDRNOT and MCTDHF provide accurate results compared to the full Schrödinger solution.

## Abstract

The $N$-particle wavefunction has too many dimensions for a direct time propagation of a many-body system according to the time-dependent Schr\"odinger equation (TDSE). On the other hand, time-dependent density functional theory (TDDFT) tells us that the single-particle density is, in principle, sufficient. However, a practicable equation of motion (EOM) for the accurate time evolution of the single-particle density is unknown. It is thus an obvious idea to propagate a quantity which is not as reduced as the single-particle density but less dimensional than the $N$-body wavefunction. Recently, we have introduced time-dependent renormalized-natural-orbital theory (TDRNOT). TDRNOT is based on the propagation of the eigenfunctions of the one-body reduced density matrix (1-RDM), the so-called natural orbitals. In this paper we demonstrate how TDRNOT is related to the multi-configurational time-dependent Hartree-Fock (MCTDHF) approach. We also compare the performance of MCTDHF and TDRNOT vs the TDSE for single-photon double ionization (SPDI) of a 1D helium model atom. SPDI is one of the effects where TDDFT does not work in practice, especially if one is interested in correlated photoelectron spectra, for which no explicit density functional is known.