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Register a new userPhotoelectron Angular Distributions for Two-photon Ionization of Helium by Ultrashort Extreme Ultraviolet Free Electron Laser Pulses
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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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We analyzed the two-dimensional (2D) electron momentum distributions of high-energy photoelectrons of atoms in an intense laser field using the second-order strong field approximation (SFA2). The SFA2 accounts for the rescattering of the returning electron with the target ion to first order and its validity is established by comparing with results obtained by solving the time-dependent Schr{o}dinger equation (TDSE) for short pulses. By analyzing the SFA2 theory, we confirmed that the yield along the back rescattered ridge (BRR) in the 2D momentum spectra can be interpreted as due to the elastic scattering in the backward directions by the returning electron wave packet. The characteristics of the extracted electron wave packets for different laser parameters are analyzed, including their dependence on the laser intensity and pulse duration. For long pulses we also studied the wave packets from the first and the later returns.
In conditions where the interaction betweeen an atom and a short high-frequency extreme ultraviolet laser pulse is a perturbation, we show that a simple theoretical approach, based on Coulomb-Volkov-type states, can make reliable predictions for ionization. To avoid any additional approximation, we consider here a standard case : the ionization of hydrogen atoms initially in their ground state. For any field parameter, we show that the method provides accurate energy spectra of ejected electrons, including many above threshold ionization peaks, as long as the two following conditions are simultaneously fulfilled : (i) the photon energy is greater than or equal to the ionization potential ; (ii) the ionization process is not saturated. Thus, ionization of atoms or molecules by the high order harmonic laser pulses which are generated at present may be addressed through this Coulomb-Volkov treatment.
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.
We describe the results of experiments and simulations performed with the aim of extending photoelectron spectroscopy with intense laser pulses to the case of molecular compounds. Dimer frame photoelectron angular distributions generated by double ionization of N$_2$-N$_2$ and N$_2$-O$_2$ van der Waals dimers with ultrashort, intense laser pulses are measured using four-body coincidence imaging with a reaction microscope. To study the influence of the first-generated molecular ion on the ionization behavior of the remaining neutral molecule we employ a two-pulse sequence comprising of a linearly polarized and a delayed elliptically polarized laser pulse that allows distinguishing the two ionization steps. By analysis of the obtained electron momentum distributions we show that scattering of the photoelectron on the neighbouring molecular potential leads to a deformation and rotation of the photoelectron angular distribution as compared to that measured for an isolated molecule. Based on this result we demonstrate that the electron momentum space in the dimer case can be separated, allowing to extract information about the ionization pathway from the photoelectron angular distributions. Our work, when implemented with variable pulse delay, opens up the possibility of investigating light-induced electronic dynamics in molecular dimers using angularly resolved photoelectron spectroscopy with intense laser pulses.
We analyze the photoelectron angular distribution in two-pathway interference between non-resonant one-photon and resonant two-photon ionization of neon. We consider a bichromatic femtosecond XUV pulse whose fundamental frequency is tuned near the $2p^5 3s$ atomic states of neon. The time-dependent Schrodinger equation is solved and the results are employed to compute the angular distribution and the associated anisotropy parameters at the main photoelectron line. We also employ a time-dependent perturbative approach, which allows obtaining information on the process for a large range of pulse parameters, including the steady-state case of continuous radiation, i.e., an infinitely long pulse. The results from the two methods are in relatively good agreement over the domain of applicability of perturbation theory.
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