Quantitative performance analysis and comparison of optimal-continuum Gaussian basis sets for high-harmonic generation spectra.

Abstract

Quantum-chemistry methods in the time domain with Gaussian basis sets are increasingly used to compute high-harmonic generation (HHG) spectra of atomic and molecular systems. The quality of these approaches is limited by the accuracy of Gaussian basis sets to describe continuum energy states. In the literature, optimal-continuum Gaussian basis sets have been proposed: Kaufmann et al. [J. Phys. B: At., Mol. Opt. Phys. 22, 2223 (1989)], Woźniak et al. [J. Chem. Phys. 154, 094111 (2021)], Nestmann and Peyerimhoff [J. Phys. B: At., Mol. Opt. Phys. 23, L773 (1990)], Faure et al. [Comput. Phys. Commun. 144, 224 (2002)], and Krause et al. [J. Chem. Phys. 140, 174113 (2014)]. In this work, we have compared the performances of these basis sets to simulate HHG spectra of H atom at different laser intensities. We have also investigated different strategies to balance basis sets with these continuum functions, together with the role of angular momentum. To quantify the performance of the different basis sets, we introduce local and global HHG descriptors. Comparisons with the grid and exact calculations are also provided.