Work

Time-Dependent Gaussian Basis Sets for Many-Body Systems Using Rothe’s Method: A Mean-Field Study

Year: 2025

Type: article

Abstract: High Resolution Image Download MS PowerPoint Slide A challenge in modeling time-dependent strong-field processes such as high-harmonic generation for many-body systems is how to effectively represent the electronic continuum. We apply Rothe’s method to the time-dependent Hartree–Fock (TDHF) and density functional theory (TDDFT) equations of motion for the orbitals, which reformulate them as an optimization problem. We show that thawed, complex-valued Gaussian basis sets can be propagated efficiently for these orbital-based approaches, removing the need for grids. In particular, we illustrate that qualitatively correct results can often be obtained by using just a few fully flexible Gaussians that describe the unbound dynamics for both TDHF and TDDFT. Grid calculations can be reproduced quantitatively using 30–100 Gaussians for intensities up to 4 × 10 14 W/cm 2 for the one-dimensional molecular systems considered in this work.

Source: Journal of Chemical Theory and Computation

DOI: 10.1021/acs.jctc.5c00970

Authors: Simon Elias Schrader, Håkon Emil Kristiansen, Thomas Bondo Pedersen, Simen Kvaal

Institution: University of Oslo

Language: English

Topic: Laser-Matter Interactions and Applications

Subfield: Atomic and Molecular Physics, and Optics

Field: Physics and Astronomy

Domain: Physical Sciences

Open Access status: hybrid

Estimated APC paid: $4,500

Funder: Norges Forskningsråd