Variational Augmentation of Gaussian Continuum Basis Sets for Calculating Atomic Higher Harmonic Generation Spectra

We present a variational augmentation procedure to optimize the exponents of Gaussian continuum basis sets for simulating strong-field laser ionization phenomena such as higher harmonic generation (HHG) in atoms and ions using the time-dependent configuration interaction (TDCI) method. We report the distribution of the optimized exponents and discuss how efficiently the resulting basis functions span the variational space to describe the near-continuum states involved in HHG. Further, we calculated the higher harmonic spectra of three two-electron systems – H^-, He and Li^+ – generated by 800nm driving laser-pulses with pulse-width of 54fs and peak intensities in the tunnel ionization regime of each system. We analyze the performance of these basis sets with an increasing number of higher angular momentum functions and show that up to g-type functions are required to obtain qualitatively accurate harmonic spectra. Additionally, we also comment on the impact of electron correlation on the HHG spectra. Finally, we show that by systematically augmenting additional shells we model the strong-field dynamics at higher laser peak intensities.