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Enhancement of strong field two-electron ionization via doubly excited states

Maxim Sukharev, Éric Charron, Annick Giusti-Suzor

Published Jan 1, 2003• 0 citations
OpenAlex

Abstract

We have performed nonperturbative time-dependent calculations of single and double ionization of atomic calcium by short and intense laser pulses using a two-active electron model (TAE). It is shown that the significant enhancement of the Ca 2+ yield observed in a recent experiment [1] using feedback control techniques originates from the time asymmetry of the pulse shape. The initial part of the pulse prepares a coherent superposition of doubly excited states which is transferred into the double electron continuum at later times. An asymmetric shape, with a slowly decreasing tail, therefore favors the production of Ca 2+ .

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We have performed nonperturbative time-dependent calculations of single and double ionization of atomic calcium by short and intense laser pulses using a two-active electron model (TAE). It is shown that the significant enhancement of the Ca 2+ yield observed in a recent experiment [1] using feedback control techniques originates from the time asymmetry of the pulse shape. The initial part of the pulse prepares a coherent superposition of doubly excited states which is transferred into the double electron continuum at later times. An asymmetric shape, with a slowly decreasing tail, therefore favors the production of Ca 2+ .
A model which describes the time evolution of strong-field photoionization of atoms is presented. Based on the numerical solution of the non-stationary Schrodinger equation, the model allows one to predict and to interpret the results of experiments on double photoionization of atoms by a combined action of a very short (attosecond) XUV pulse and a few-cycle IR pulse of a powerful laser at various delay times between the two pulses. Depending on the binding energy of the ionized electron, two types of processes are considered. If the electron is tightly bound (Ne case), the XUV pulse ionizes the atom and shakes up another (outer) electron to an excited state, which is subsequently ionized by the strong IR field. For an atom with a weakly bound outer electron (Li case), the IR field ionizes the latter, while the XUV pulse, ionizing the inner shell, terminates (or suppresses) the strong-field ionization. In both cases the yield of doubly ionized ions strongly depends on the delay time between the two pulses, revealing 'steps', oscillations and other features which characterize the time evolution of the ionization process. The presented model describes qualitatively the results of recent experiments on Ne.
Singly and doubly charged Ca ions have been produced by multiphoton excitation of Ca vapour with 5 ns, low intensity (⩽3 × 10 11 W cm −2 ) dye-laser pulses in the 675–685 nm wavelength range, including the four-photon 4s 2 1 S 0 → 4p 2 1 S 0 excitation. The intensity and wavelength dependence of the ion yields was recorded as well as the fluorescence emission from excited states of the Ca ion in an effort to identify the excitation pathways leading to single and double ionization. Unambiguous evidence for the absorption of at least two photons above the first ionization threshold was recorded, in agreement with earlier results for Mg and Sr obtained under similar conditions. However, certain characteristics of the process differ significantly from those of the earlier results, despite the apparent similarity in both the atomic structure and the excitation scheme. The most striking and unexpected finding is that for a certain wavelength, the Ca 2+ yield is observable well before the saturation intensity of Ca + and, moreover, it grows with intensity and saturates in parallel with the Ca + yield. Possible mechanisms behind this outcome are discussed in detail as well as their implications for the multiphoton multiple ionization of complex atoms. Our tentative conclusion is that the occurrence of doubly charged ion production before the singly charged ion saturation should not be considered as 'synonymous' with direct (or non-sequential) multiphoton double ionization.
We report on the experimental observation of a strong-field dressing of an autoionizing two-electron state in helium with intense extreme-ultraviolet laser pulses from a free-electron laser. The asymmetric Fano line shape of this transition is spectrally resolved, and we observe modifications of the resonance asymmetry structure for increasing free-electron-laser pulse energy on the order of few tens of Microjoules. A quantum-mechanical calculation of the time-dependent dipole response of this autoionizing state, driven by classical extreme-ultraviolet (XUV) electric fields, evidences strong-field-induced energy and phase shifts of the doubly excited state, which are extracted from the Fano line-shape asymmetry. The experimental results obtained at the Free-Electron Laser in Hamburg (FLASH) thus correspond to transient energy shifts on the order of a few meV, induced by strong XUV fields. These results open up a new way of performing nonperturbative XUV nonlinear optics for the light-matter interaction of resonant electronic transitions in atoms at short wavelengths.
The energy levels of atoms and molecules exposed to intense, short, high-frequency laser pulses undergo time-dependent distortion known as dynamic Stark shift (DSS). These level shifts are induced by the coupling with nonresonant (nonessential) states and follow the temporal intensity profile of the laser pulse. Owing to the different DSSs of the individual atomic levels, transient resonance suppressions and enhancements significantly modify the multiphoton ionization pathway, leaving clear fingerprints (asymmetry, splitting, and shifting) in the energy spectrum of emitted photoelectrons. Here we investigate this phenomenon by solving the time-dependent Schr\"odinger equation of the valence electron of Na and Li in increasing levels of complexity: (i) developing minimal models for two-photon transition and (2+12+12+1)-photon ionization, (ii) applying a spectral method without continuum-continuum couplings, and (iii) propagating the electron wave packet on a large spatial grid accounting for all possible couplings. We show that appropriately detuned transform limited pulses provide a high level of control in strong-field excitation, when the atomic levels are dynamically shifted. Furthermore, we demonstrate the role of DSSs in the multipeak structure of the Autler-Townes doublet, found when several Rabi oscillations are induced during the strong-field resonant ionization.
We present a simple model for calculating strong-field atomic and molecular ionization dominated by Freeman resonances. Our model combines multiphoton coupling between bound states, including dynamic Stark shifts, with coupling to a discretized continuum. The simplicity of the model allows us to interpret pulse-shape-dependent strong-field ionization yields and to demonstrate the relevance of strong-field atomic or molecular phase matching to ionization, as well as bound-state population transfer. Comparison with experimental measurements demonstrates that the calculations capture the essence of the pulse-shape-dependent ionization yields.