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Register a new userStudying the universality of field induced tunnel ionization times via high-order harmonic spectroscopy
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Hadas Soifer
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High-harmonics generation spectroscopy is a promising tool for resolving electron dynamics and structure in atomic and molecular systems. This scheme, commonly described by the strong field approximation, requires a deep insight into the basic mechanism that leads to the harmonics generation. Recently, we have demonstrated the ability to resolve the first stage of the process -- field induced tunnel ionization -- by adding a weak perturbation to the strong fundamental field. Here we generalize this approach and show that the assumptions behind the strong field approximation are valid over a wide range of tunnel ionization conditions. Performing a systematic study -- modifying the fundamental wavelength, intensity and atomic system -- we observed a good agreement with quantum path analysis over a range of Keldysh parameters. The generality of this scheme opens new perspectives in high harmonics spectroscopy, holding the potential of probing large, complex molecular systems.
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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.
We illustrate an iterative method for retrieving the internuclear separations of N$_2$, O$_2$ and CO$_2$ molecules using the high-order harmonics generated from these molecules by intense infrared laser pulses. We show that accurate results can be retrieved with a small set of harmonics and with one or few alignment angles of the molecules. For linear molecules the internuclear separations can also be retrieved from harmonics generated using isotropically distributed molecules. By extracting the transition dipole moment from the high-order harmonic spectra, we further demonstrated that it is preferable to retrieve the interatomic separation iteratively by fitting the extracted dipole moment. Our results show that time-resolved chemical imaging of molecules using infrared laser pulses with femtosecond temporal resolutions is possible.
We report the observation of multiple ionization of Argon through multi-XUV-photon absorption induced by an unprecedentedly powerful laser driven high-harmonic-generation source. Comparing the measured intensity dependence of the yield of the different Argon charge states with numerical calculations we can infer the different channels -direct and sequential- underlying the interaction. While such studies were feasible so far only with FEL sources, this work connects highly-non-linear-XUV-processes with the ultra-short time scales, inherent to the harmonic pulses, and highlights the advanced perspectives of emerging large scale laser research infrastructures.
We present an experimental study on the photoionization dynamics of non-resonant one-color two-photon single valence ionization of neutral argon atoms. Using 9.3 eV photons produced via high harmonic generation and a 3-D momentum imaging spectrometer, we detect the photoelectrons and ions produced from non-resonant two-photon ionization in coincidence. Photoionization from the $3p$ orbital produces a photoelectron scattering wave function with $p$ and $f$ partial wave components, which interfere and result in a photoelectron angular distribution with peak amplitude perpendicular to the VUV polarization. The comparison between the present results and two previous sets of theoretical calculations [Pan, C. & Starace, A. F. (1991). $textit{Physical Review A}$, 44(1), 324., and Moccia, R., Rahman, N. K., & Rizzo, A. (1983). $textit{Journal of Physics B: Atomic and Molecular Physics}$, 16(15), 2737.] indicates that electron-electron correlation contributes appreciably to the two-photon ionization dynamics.
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.
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