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Register a new userElectron correlation in two-photon double ionization of helium from attosecond to FEL pulses
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We investigate the role of electron correlation in the two-photon double ionization of helium for ultrashort XUV pulses with durations ranging from a hundred attoseconds to a few femtoseconds. We perform time-dependent ab initio calculations for pulses with mean frequencies in the so-called sequential regime (photon energy above 54.4 eV). Electron correlation induced by the time correlation between emission events manifests itself in the angular distribution of the ejected electrons, which strongly depends on the energy sharing between them. We show that for ultrashort pulses two-photon double ionization probabilities scale non-uniformly with pulse duration depending on the energy sharing between the electrons. Most interestingly we find evidence for an interference between direct (nonsequential) and indirect (sequential) double photo-ionization with intermediate shake-up states, the strength of which is controlled by the pulse duration. This observation may provide a route toward measuring the pulse duration of FEL pulses.
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We present accurate time-dependent ab initio calculations on fully differential and total integrated (generalized) cross sections for the nonsequential two-photon double ionization of helium at photon energies from 40 to 54 eV. Our computational method is based on the solution of the time-dependent Schroedinger equation and subsequent projection of the wave function onto Coulomb waves. We compare our results with other recent calculations and discuss the emerging similarities and differences. We investigate the role of electronic correlation in the representation of the two-electron continuum states, which are used to extract the ionization yields from the fully correlated final wave function. In addition, we study the influence of the pulse length and shape on the cross sections in time-dependent calculations and address convergence issues.
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.
We present the first demonstration of two-photon double ionization of neon using an intense extreme ultraviolet (XUV) attosecond pulse train (APT) in a photon energy regime where both direct and sequential mechanisms are allowed. For an APT generated through high-order harmonic generation (HHG) in argon we achieve a total pulse energy close to 1 $mu$J, a central energy of 35 eV and a total bandwidth of $sim30$ eV. The APT is focused by broadband optics in a neon gas target to an intensity of $3cdot10^{12} $W$cdot$cm$^{-2}$. By tuning the photon energy across the threshold for the sequential process the double ionization signal can be turned on and off, indicating that the two-photon double ionization predominantly occurs through a sequential process. The demonstrated performance opens up possibilities for future XUV-XUV pump-probe experiments with attosecond temporal resolution in a photon energy range where it is possible to unravel the dynamics behind direct vs. sequential double ionization and the associated electron correlation effects.
Triple-differential cross sections for two-photon double ionization of molecular hydrogen are presented for a central photon energy of 30 eV. The calculations are based on a fully {it ab initio}, nonperturbative, approach to the time-dependent Schroedinger equation in prolate spheroidal coordinates, discretized by a finite-element discrete-variable-representation. The wave function is propagated in time for a few femtoseconds using the short, iterative Lanczos method to study the correlated response of the two photoelectrons to short, intense laser radiation. The current results often lie in between those of Colgan {it et al} [J. Phys. B {bf 41} (2008) 121002] and Morales {it et al} [J. Phys. B {bf 41} (2009) 134013]. However, we argue that these individual predictions should not be compared directly to each other, but preferably to experimental data generated under well-defined conditions.
Phase-shift differences and amplitude ratios of the outgoing $s$ and $d$ continuum wave packets generated by two-photon ionization of helium atoms are determined from the photoelectron angular distributions obtained using velocity map imaging. Helium atoms are ionized with ultrashort extreme-ultraviolet free-electron laser pulses with a photon energy of 20.3, 21.3, 23.0, and 24.3 eV, produced by the SPring-8 Compact SASE Source test accelerator. The measured values of the phase-shift differences are distinct from scattering phase-shift differences when the photon energy is tuned to an excited level or Rydberg manifold. The difference stems from the competition between resonant and non-resonant paths in two-photon ionization by ultrashort pulses. Since the competition can be controlled in principle by the pulse shape, the present results illustrate a new way to tailor the continuum wave packet.
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