We theoretically demonstrated that helical-photon-dressed states determine the rotational directions of the π-electrons of aromatic ring molecules formed by a circularly polarized or an elliptically polarized laser. This theory was verified using a minimal three-electronic-state model under the frozen nuclei condition. The model consists of the ground state and either a doubly degenerate electronic excited state or two quasi-degenerate excited states.
View Article and Find Full Text PDFA 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.
View Article and Find Full Text PDFThe 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.
View Article and Find Full Text PDFWe 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.
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