Controlling the multi-electron dynamics in the high harmonic spectrum from N2O molecule using TDDFT

• Published in: The Journal of chemical physics 2018-06, Vol.148 (23), p.234303-234303
• Main Authors: Monfared, M., Irani, E., Sadighi-Bonabi, R.
• Format: Article
• Language: English
• Subjects: Attosecond pulses; Broadband; Density functional theory; Electron trajectories; Electrons; Frequency shift; Harmonic generations; Molecular dynamics; Nitrous oxide; Physics; Time dependence; Wavelet transforms
• ISSN: 0021-9606; 1089-7690
• DOI: 10.1063/1.5025155

In this study, high harmonic generation from a multi-atomic nitrous oxide molecule was investigated. A comprehensive three-dimensional calculation of the molecular dynamics and electron trajectories through an accurate time-dependent density functional theory was conducted to efficiently explore a broad harmonic plateau. The effects of multi-electron and inner orbitals on the harmonic spectrum and generated coherent attosecond pulses were analyzed. The role of the valence electrons in controlling the process and extending the harmonic plateau was investigated. The main issue of producing a super-continuum harmonic spectrum via a frequency shift was considered. The time-frequency representation by means of a wavelet transform of the induced dipole acceleration provided a good insight into the distorted effects from the nonlinear processes in high harmonic emission. The effect of the chirped laser pulse on the production of broadband amplitude was justified in this model. By adjusting the optimal laser parameters to an input intensity of 2.5 × 1014 W cm−2, an isolated 68 as pulse was generated.