High harmonic spectra computed using time-dependent Kohn-Sham theory with Gaussian orbitals and a complex absorbing potential

High harmonic spectra for H-2 and H-2(+) are simulated by solving the time-dependent Kohn-Sham equation in the presence of a strong laser field using an atom-centered Gaussian representation of the density and a complex absorbing potential. The latter serves to mitigate artifacts associated with the finite extent of the basis functions, including spurious reflection of the outgoing electronic wave packet. Interference between the outgoing and reflected waves manifests as peak broadening in the spectrum as well as the appearance of spurious high-energy peaks after the harmonic progression has terminated. We demonstrate that well-resolved spectra can be obtained through the use of an atom-centered absorbing potential. As compared to grid-based algorithms, the present approach is more readily extensible to larger molecules. Published under an exclusive license by AIP Publishing.

Automated summary

In this study, high harmonic spectra for H-2 and H-2(+) were simulated using an atom-centered Gaussian representation of the density and a complex absorbing potential. The results showed that this approach can achieve better resolution compared to grid-based algorithms.