Below- and near-threshold harmonic generation provides a potential approach to achieve a high conversion efficiency of vacuum-ultraviolet and extreme-ultraviolet sources for the advancement of spectroscopy. Here, we perform a time-dependent density functional theory study for the nonperturbative treatment of below- and near-threshold harmonic generation of CO and N2 diatomic molecules subject to short near-infrared laser pulses and aligned parallel to the laser field polarization. We find that with the use of different driving laser pulse shapes, we can control and enhance harmonic generation through the excited-state resonance structures. Depending on the pulse shape, the enhancement can reach five to seven orders of magnitude as compared to the reference sine-squared laser pulse of the same duration. The results for different driving laser intensities are also presented and discussed in detail.

Original languageEnglish
Article number063401
Number of pages11
JournalPhysical Review A - Atomic, Molecular, and Optical Physics
Volume93
Issue number6
DOIs
StatePublished - 1 Jun 2016

    Scopus subject areas

  • Atomic and Molecular Physics, and Optics

ID: 7569250