Implementation of the multiconfiguration time-dependent Hatree-Fock method for general molecules on a multi-resolution Cartesian grid

TL;DR

This paper presents a 3D numerical implementation of the multiconfiguration time-dependent Hartree-Fock method on a multi-resolution Cartesian grid, enabling first-principles studies of ultrafast phenomena in general molecules without symmetry assumptions.

Contribution

The paper introduces a novel 3D implementation of MCTDHF on a multi-resolution grid that does not require molecular symmetry, expanding computational capabilities for complex molecules.

Findings

Successfully computed high-harmonic generation in H2 and H2O

Demonstrated feasibility of first-principles ultrafast molecular simulations

Enabled study of intense-field phenomena in general molecules

Abstract

We report a three-dimensional numerical implementation of multiconfiguration time-dependent Hartree-Fock (MCTDHF) based on a multi-resolution Cartesian grid, with no need to assume any symmetry of molecular structure. We successfully compute high-harmonic generation (HHG) of H2 and H2O. The present implementation will open a way to the first-principle theoretical study of intense-field and attosecond-pulse induced ultrafast phenomena in general molecules.