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

Area of Science:

• Quantum chemistry
• Atomic and molecular physics
• Computational physics

Background:

• Time-domain quantum-chemistry methods using Gaussian basis sets are common for calculating high-harmonic generation (HHG) spectra.
• The accuracy of these methods is often limited by the ability of Gaussian basis sets to represent continuum states.

Purpose of the Study:

• To compare the performance of various proposed optimal-continuum Gaussian basis sets for simulating HHG spectra.
• To investigate strategies for balancing basis sets with continuum functions and the influence of angular momentum.
• To introduce novel local and global descriptors for quantifying HHG simulation performance.

Main Methods:

• Simulation of HHG spectra for a hydrogen atom using different Gaussian basis sets at varying laser intensities.
• Evaluation of basis set performance using introduced HHG descriptors.
• Comparison of results with grid-based and exact calculations.

Main Results:

• Performance variations were observed among different Gaussian basis sets in simulating HHG spectra.
• The choice of basis set and balancing strategies significantly impacts simulation accuracy.
• The introduced HHG descriptors effectively quantify the performance of the basis sets.

Conclusions:

• The study provides a comparative analysis of Gaussian basis sets for HHG simulations.
• The developed descriptors offer a reliable method for assessing basis set accuracy in quantum-chemistry calculations.
• Findings guide the selection of appropriate basis sets for accurate HHG spectral simulations.