Odd-even harmonic generation from oriented CO molecules in linearly polarized laser fields and the influence of the dynamic core-electron polarization
We present a detailed theoretical study of the odd-even harmonics generated from the polar molecule CO by the method based on numerically solving the time-dependent Schrödinger equation within the single-active-electron approximation. First, we reproduce the pure even harmonic generation of CO predi...
Gespeichert in:
Veröffentlicht in: | Physical chemistry chemical physics : PCCP 2019-11, Vol.21 (43), p.24177-24186 |
---|---|
Hauptverfasser: | , , , |
Format: | Artikel |
Sprache: | eng |
Schlagworte: | |
Online-Zugang: | Volltext |
Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
Zusammenfassung: | We present a detailed theoretical study of the odd-even harmonics generated from the polar molecule CO by the method based on numerically solving the time-dependent Schrödinger equation within the single-active-electron approximation. First, we reproduce the pure even harmonic generation of CO predicted theoretically by Hu
et al.
using the time-dependent density functional theory [H. Hu
et al.
,
Phys. Rev. Lett.
, 2017,
119
, 173201]. Then, based on the Floquet approach, we are able to attribute this behavior to the half-cycle mirror symmetry of the molecule-field system when the polar molecule is perpendicular to the laser polarization. By numerical simulations, we show that this symmetry is broken at orientation angles other than 90° resulting in the odd-even harmonic generation and a non-trivial even-to-odd harmonics ratio strongly dependent on the molecular orientation. Furthermore, we investigate the influence of the dynamic core-electron polarization (DCeP) on the odd-even behavior near the cutoff of the high-order harmonic spectra. We emphasize that the DCeP effect is noticeable for the odd harmonics only.
We present a detailed theoretical study of the odd-even harmonics generated from the polar molecule CO by the method based on numerically solving the time-dependent Schrödinger equation within the single-active-electron approximation. |
---|---|
ISSN: | 1463-9076 1463-9084 |
DOI: | 10.1039/c9cp04064a |