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High ellipticity of harmonics from molecules in strong laser fields of small ellipticity

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 Added by Yanjun Chen
 Publication date 2021
  fields Physics
and research's language is English




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We study high-order harmonic generation (HHG) from aligned molecules in strong elliptically polarized laser fields numerically and analytically. Our simulations show that the spectra and polarization of HHG depend strongly on the molecular alignment and the laser ellipticity. In particular, for small laser ellipticity, large ellipticity of harmonics with high intensity is observed for parallel alignment, with forming a striking ellipticity hump around the threshold. We show that the interplay of the molecular structure and two-dimensional electron motion plays an important role here. This phenomenon can be used to generate bright elliptically-polarized EUV pulses.

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The present work reports on the generation of short-pulse coherent extreme ultraviolet radiation of controlled polarization. The proposed strategy is based on high-order harmonics generated in pre-aligned molecules. Field-free molecular alignment produced by a short linearly-polarized infrared laser pulse is used to break the isotropy of a gas medium. Driving the aligned molecules by a circularly-polarized infrared pulse allows to transfer the anisotropy of the medium to the polarization of the generated harmonic light. The ellipticity of the latter is controlled by adjusting the angular distribution of the molecules at the time they interact with the driving pulse. Extreme ultraviolet radiation produced with high degree of ellipticity (close to circular) is demonstrated.
We consider second-order partial differential operators $H$ in divergence form on $Ri^d$ with a positive-semidefinite, symmetric, matrix $C$ of real $L_infty$-coefficients and establish that $H$ is strongly elliptic if and only if the associated semigroup kernel satisfies local lower bounds, or, if and only if the kernel satisfies Gaussian upper and lower bounds.
We perform high-resolution measurements of momentum distribution on Rb$^{n+}$ recoil ions up to charge state $n=4$, where laser-cooled rubidium atoms are ionized by femtosecond elliptically polarized lasers with the pulse duration of 35 fs and the intensity of 3.3$times$10$^{15}$ W/cm$^2$ in the over-barrier ionization (OBI) regime. The momentum distributions of the recoil ions are found to exhibit multi-band structures as the ellipticity varies from the linear to circular polarizations. The origin of these band structures can be explained quantitatively by the classical OBI model and dedicated classical trajectory Monte Carlo simulations with Heisenberg potential. Specifically, with back analysis of the classical trajectories, we reveal the ionization time and the OBI geometry of the sequentially released electrons, disentangling the mechanisms behind the tilted angle of the band structures. These results indicate that the classical treatment can describe the strong-field multiple ionization processes of alkali atoms.
The quasistatic limit of the velocity-gauge strong-field approximation describing the ionization rate of atomic or molecular systems exposed to linear polarized laser fields is derived. It is shown that in the low-frequency limit the ionization rate is proportional to the laser frequency, if a Coulombic long-range interaction is present. An expression for the corresponding proportionality coefficient is given. Since neither the saddle-point approximation nor the one of a small kinetic momentum is used in the derivation, the obtained expression represents the exact asymptotic limit. This result is used to propose a Coulomb correction factor. Finally, the applicability of the found asymptotic expression for non-vanishing laser frequencies is investigated.
The dependence of high-harmonic generation (HHG) on laser ellipticity is investigated using a modified ZnO model. In the driving of relatively weak field, we reproduce qualitatively the ellipticity dependence as observed in the HHG experiment of wurtzite ZnO. When increasing the field strength, the HHG shows an anomalous ellipticity dependence, similar to that observed experimentally in the single-crystal MgO. With the help of a semiclassical analysis, it is found that the key mechanism inducing the change of ellipticity dependence is the interplay between the dynamical Bloch oscillation and the anisotropic band structure. The dynamical Bloch oscillation contributes additional quantum paths, which are less sensitive to ellipticity. The anisotropic band-structure make the driving pulse with finite ellipticity be able to drive the pairs to the band positions with larger gap, which extends the harmonic cutoff. The combination of these two effects leads to the anomalous ellipticity dependence. The result reveals the importance of dynamical Bloch oscillations for the ellipticity dependence of HHG from bulk ZnO.
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