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Register a new userTransition from non-sequential to sequential double ionisation in many-electron systems
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Obtaining a detailed understanding of strong-field double ionisation of many-electron systems (heavy atoms and molecules) remains a challenging task. By comparing experimental and theoretical results in the mid-IR regime, we have unambiguously identified the transition from non-sequential (e,2e) to sequential double ionisation in Xe and shown that it occurs at an intensity below $10^{14}$ Wcm$^{-2}$. In addition, our data demonstrate that ionisation from the Xe 5s orbital is decisive at low intensities. Moreover, using the acetylene molecule, we propose how sequential double ionisation in the mid-IR can be used to study molecular dynamics and fragmentation on unprecedented few-femtosecond timescales.
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At intensities below-the-recollision threshold, we show that re-collision-induced excitation with one electron escaping fast after re-collision and the other electron escaping with a time delay via a Coulomb slingshot motion is one of the most important mechanisms of non-sequential double ionization, for strongly-driven He at 400 nm. Slingshot-NSDI is a general mechanism present for a wide range of low intensities and pulse durations. Anti-correlated two-electron escape is its striking hallmark. This mechanism offers an alternative explanation of anti-correlated two-electron escape obtained in previous studies.
Fully accounting for non-dipole effects in the electron dynamics, double ionization is studied for He driven by a near-infrared laser field and for Xe driven by a mid-infrared laser field. Using a three-dimensional semiclassical model, the average sum of the electron momenta along the propagation direction of the laser field is computed. This sum is found to be an order of magnitude larger than twice the average electron momentum along the propagation direction of the laser field in single ionization. Moreover, the average sum of the electron momenta in double ionization is found to be maximum at intensities smaller than the intensities satisfying previously predicted criteria for the onset of magnetic field effects. It is shown that strong recollisions are the reason for this unexpectedly large value of the sum of the momenta along the direction of the magnetic component of the Lorentz force.
We report on non-sequential double ionization of Ar by a laser pulse consisting of two counter rotating circularly polarized fields (390 nm and 780 nm). The double ionization probability depends strongly on the relative intensity of the two fields and shows a knee-like structure as function of intensity. We conclude that double ionization is driven by a beam of nearly monoenergetic recolliding electrons, which can be controlled in intensity and energy by the field parameters. The electron momentum distributions show the recolliding electron as well as a second electron which escapes from an intermediate excited state of Ar$^+$.
We describe first-principles in-plane calculations of non-sequential triple ionization (NSTI) of atoms in a linearly polarized intense laser pulse. In a fully classically correlated description, all three electrons respond dynamically to the nuclear attraction, the pairwise e-e repulsions and the laser force throughout the duration of a 780nm laser pulse. Nonsequential ejection is shown to occur in a multi-electron, possibly multi-cycle and multi-dimensional, rescattering sequence that is coordinated by a number of sharp transverse recollimation impacts.
We analyze two-photon double ionization of helium in both the nonsequential and sequential regime. We show that the energy spacing between the two emitted electrons provides the key parameter that controls both the energy and the angular distribution and reveals the universal features present in both the nonsequential and sequential regime. This universality, i.e., independence of photon energy, is a manifestation of the continuity across the threshold for sequential double ionization. For all photon energies, the energy distribution can be described by a universal shape function that contains only the spectral and temporal information entering second-order time-dependent perturbation theory. Angular correlations and distributions are found to be more sensitive to the photon energy. In particular, shake-up interferences have a large effect on the angular distribution. Energy spectra, angular distributions parameterized by the anisotropy parameters, and total cross sections presented in this paper are obtained by fully correlated time-dependent ab initio calculations.
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