Time-dependent Gaussian basis sets for many-body systems using Rothe's method: A mean-field study
arXiv:2506.10701 · doi:10.1021/acs.jctc.5c00970
Abstract
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 reformulates 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 -- Gaussians for intensities up to W/cm for the one-dimensional molecular systems considered in this work.
22 pages, 10 figures
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