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Register a new userImproved Lewenstein model for high-order harmonic generation of atoms and molecules with scattering wavefunctions
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We demonstrate a simple method to improve the Lewenstein model for the description of high-order harmonic generation (HHG). It is shown that HHG spectra can be expressed as the product of a returning electron wave packet and the photo-recombination cross sections, where the former can be extracted from the Lewenstein model. By replacing plane waves with scattering waves in the calculation of recombination matrix elements, we showed that the resulting HHG spectra agree well with those from solving the time-dependent Schrodinger equation. The improved model can be used for quantitative calculations of high harmonics generated by molecules.
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We show that the dependence of high-order harmonic generation (HHG) on the molecular orientation can be understood within a theoretical treatment that does not involve the strong field of the laser. The results for H_2 show excellent agreement with time-dependent strong field calculations for model molecules, and this motivates a prediction for the orientation dependence of HHG from the N_2 3s_g valence orbital. For both molecules, we find that the polarization of recombination photons is influenced by the molecular orientation. The variations are particularly pronounced for the N_2 valence orbital, which can be explained by the presence of atomic p-orbitals.
Using dynamical Hartree-Fock mean-field theory, we study the high-harmonic generation (HHG) in the fullerene molecules C$_{60}$ and C$_{70}$ under strong pump wave driving. We consider a strong-field regime and show that the output harmonic radiation exhibits multiple plateaus, whose borders are defined by the molecular excitonic lines and cutoff energies within each plateau scale linearly with the field strength amplitude. In contrast to atomic cases for the fullerene molecule, with the increase of the pump wave photon energy the cutoff harmonic energy is increased. We also show that with the increase of the electron-electron interaction energy overall the HHG rate is suppressed. We demonstrate that the C$_{70}$ molecule shows richer HHG spectra and a stronger high-harmonic intensity than the C$_{60}$.
We show that high-order harmonics generated from molecules by intense laser pulses can be expressed as the product of a returning electron wave packet and the photo-recombination cross section (PRCS) where the electron wave packet can be obtained from simple strong-field approximation (SFA) or from a companion atomic target. Using these wave packets but replacing the PRCS obtained from SFA or from the atomic target by the accurate PRCS from molecules, the resulting HHG spectra are shown to agree well with the benchmark results from direct numerical solution of the time-dependent Schrodinger equation, for the case of H$_2^+$ in laser fields. The result illustrates that these powerful theoretical tools can be used for obtaining high-order harmonic spectra from molecules. More importantly, the results imply that the PRCS extracted from laser-induced HHG spectra can be used for time-resolved dynamic chemical imaging of transient molecules with temporal resolutions down to a few femtoseconds.
Electron quantum path interferences in strongly laser-driven aligned molecules and their dependence on the molecular alignment is an essential open problem in strong-field molecular physics. Here, we demonstrate an approach which provides direct access to the observation of these interference processes. The approach is based on the combination of the time-gated-ion-microscopy technique with a pump-probe arrangement used to align the molecules and generate high-order harmonics. By spatially resolving the interference pattern produced by the spatiotemporal overlap of the harmonics emitted by the short and long electron quantum paths, we have succeeded in measuring in situ their phase difference and disclose their dependence on molecular alignment. The findings constitute a vital step towards an understanding of strong-field molecular physics and the development of attosecond spectroscopy approaches without the use of auxiliary atomic references.
We study high-order harmonic generation in aligned molecules close to the ionization threshold. Two distinct contributions to the harmonic signal are observed, which show very different responses to molecular alignment and ellipticity of the driving field. We perform a classical electron trajectory analysis, taking into account the significant influence of the Coulomb potential on the strong-field-driven electron dynamics. The two contributions are related to primary ionization and excitation processes, offering a deeper understanding of the origin of high harmonics near the ionization threshold. This work shows that high harmonic spectroscopy can be extended to the near-threshold spectral range, which is in general spectroscopically rich.
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