ABSTRACT
A wide range of harmonics especially continuum harmonics is a prerequisite for attosecond pulse generation. One can use longer-wavelength lasers to push the cutoff to a higher order. However, this does not translate to the same amount of continuum range extension because multiple rescattering phenomena are also enhanced in the process, potentially affecting the lower end of the continuum harmonics. It is then important to understand exactly how multiple rescatterings affect the harmonic structure and their response to various laser parameters, which is the main theme of this paper. Particularly, by applying the synchrosqueezed time-frequency transform and classical electron trajectory analysis to the asymmetric molecule carbon monoxide (CO), we justify that the multiple rescatterings indeed influence the periodicity of the harmonic spectra and the stable periodicity is, in fact, bounded by the first- and third-order returns. Moreover, for the first time, we find that the high-order rescatterings are asymmetric regarding the molecular rotation of 180°, but always correlate with the first-order returns. Our last result is that by breaking the laser symmetry in an appropriate way, the contribution of multiple rescatterings is removed so that the continuum region is entirely defined by the first-order return energies.
ABSTRACT
The effects of vibrational motions on dynamic Stark-induced π-electron rotations in a low-symmetry aromatic ring molecule are theoretically studied in the adiabatic approximation. We adopt a simplified three-electronic state model with a few vibronic states. A pair of the lowest vibronic states in two electronic excited states is set degenerate by irradiation of two linearly polarized UV lasers. The resultant degenerate state is named the dynamic Stark-induced degenerate vibronic state (DSIDVS). The laser parameters (intensities and central frequencies) are determined under the conditions of DSIDVS formation. The aromatic ring molecules of interest are supposed to belong to the weak coupling case. The analytical expressions for the DSIDVS and coherent angular momentum LZ(t) are derived in the displaced harmonic oscillator (DHO) model. Two horizontal potential displacements (δα, δß) between the two electronic excited states (α and ß) and the ground state are the parameters in the DHO model. The LZ(t) calculated with δα = 뫧 is characterized by a regular sequence of the angular momentum pulses with a positive (or negative) constant. For a more general case with δα ≠ δß, the regular sequence is broken down because of the contribution of the first excited vibronic state in each electronic state to LZ(t).
ABSTRACT
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.
