Odd-even harmonic generation from oriented CO molecules in linearly polarized laser fields and the influence of the dynamic core-electron polarization

• Published in: Physical chemistry chemical physics : PCCP 2019-11, Vol.21 (43), p.24177-24186
• Main Authors: Phan, Ngoc-Loan, Le, Cam-Tu, Hoang, Van-Hung, Le, Van-Hoang
• Format: Article
• Language: English
• Subjects: Computer simulation; Density functional theory; Electrons; Harmonic generations; Linear polarization; Schrodinger equation; Symmetry; Time dependence
• ISSN: 1463-9076; 1463-9084
• DOI: 10.1039/c9cp04064a

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.