Efficient simulation of multielectron dynamics in molecules under intense laser pulses: Implementation of the multiconfiguration time-dependent Hartree-Fock method based on the adaptive finite element method

TL;DR

This paper introduces an efficient implementation of the multiconfiguration time-dependent Hartree-Fock method using adaptive finite elements, enabling faster multielectron molecular dynamics simulations under intense laser pulses.

Contribution

The paper develops a parallelized, stable propagator-based implementation of MCTDHF with adaptive finite elements, significantly reducing computational time for multielectron dynamics simulations.

Findings

Successful simulation of high-harmonic generation from water.

Achieved faster multielectron dynamics simulations compared to previous methods.

Demonstrated scalability with parallel computing.

Abstract

We present an implementation of the multiconfiguration time-dependent Hartree-Fock method based on the adaptive finite element method for molecules under intense laser pulses. For efficient simulations, orbital functions are propagated by a stable propagator using the short iterative Arnoldi scheme and our implementation is parallelized for distributed memory computing. This is demonstrated by simulating high-harmonic generation from a water molecule and achieves a simulation of multielectron dynamics with overwhelmingly less computational time, compared to our previous work.