We consider the final stage of triple ionization of atoms in a strong linearly polarized laser field. We propose that for intensities below the saturation value for triple ionization the process is dominated by the simultaneous escape of three electrons from a highly excited intermediate complex. We identify within a classical model two pathways to triple ionization, one with a triangular configuration of electrons and one with a more linear one. Both are saddles in phase space. A stability analysis indicates that the triangular configuration has the larger cross sections and should be the dominant one. Trajectory simulations within the dominant symmetry subspace reproduce the experimentally observed distribution of ion momenta parallel to the polarization axis.
The outgoing electrons in non-sequential multiple ionization in intense laser fields are strongly correlated. The correlations can be explained within a classical model for interacting electrons in the presence of the external field. Here we extend the previous analysis for two and three electrons to cases with up to eight electrons and identify the saddle configurations that guard the channels for non-sequential multiple ionization. For four and fewer electrons the electrons in the dominant configuration are equivalent, for six and more electrons this is no longer the case. The case of five e…
The interaction of strong pulsed femtosecond laser field with atoms having three equivalent electrons in the outer shell ($p^3$ configuration, e.g. nitrogen) is studied via numerical integration of a time-dependent Schrödinger equation on a grid approach. Single, double and triple ionization yields originating from a completely antisymmetric wave function are calculated and extracted using a restricted-geometry model with the soft-core potential and three active electrons. The direct triple ionization channel is found to produce a larger yield than the channel connected with single and then di…
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…
We present a joint experimental and theoretical study of non-sequential double ionization (NSDI) in argon driven by a 3100-nm laser source. The correlated photoelectron momentum distribution (PMD) shows a strong dependence on the pulse duration, and the evolution of the PMD can be explained by an envelope-induced intensity effect. Determined by the time difference between tunneling and rescattering, the laser vector potential at the ionization time of the bound electron will be influenced by the pulse duration, leading to different drift momenta. Such a mechanism is extracted through a classic…
We discuss the final stages of double ionization of atoms in a strong linearly polarized laser field within a classical model. We propose that all trajectories leading to non-sequential double ionization pass close to a saddle in phase space which we identify and characterize. The saddle lies in a two degree of freedom subspace of symmetrically escaping electrons. The distribution of longitudinal momenta of ions as calculated within the subspace shows the double hump structure observed in experiments. Including a symmetric bending mode of the electrons allows us to reproduce the transverse ion…
We demonstrate entanglement between the orbital angular momentum (OAM) of two photoelectrons ionized via the strongly correlated process of non-sequential double ionization (NSDI). Due to the quantization of OAM, this entanglement is easily quantified and has a simple physical interpretation in terms of conservation laws. We explore detection by an entanglement witness, decomposable into local measurements, which strongly reduces the difficulty of experimental implementation. We compute the logarithmic negativity measure, which is directly applicable to mixed states, to demonstrate that the en…
We discuss the final stages of the simultaneous ionization of two or more electrons due to a strong laser pulse. An analysis of the classical dynamics suggests that the dominant pathway for non-sequential escape has the electrons escaping in a symmetric arrangement. Classical trajectory models within and near to this symmetry subspace support the theoretical considerations and give final momentum distributions in close agreement with experiments.
Without a formal derivation, we propose a formula for the total and single-differential cross in the problem of one-photon double ionization of an atom. The formula is benchmarked against accurate experimental data for the total cross section of helium. Furthermore, a direct comparison with ab initio calculations for the double ionization of Li+ suggests that the framework is valid for the entire helium isoelectronic sequence. To this end, we introduce a formula for the double ionization of lithium, as well as for the triple ionization of lithium and beryllium.
We analytically compute, in the first Born approximation for symmetric and asymmetric coplanar geometries, the triple differential cross sections for electron-impact ionization of hydrogen atom in the metastable 2S-state at both low and high energies. The process is investigated by using the relativistic Dirac-formalism and it is also shown that the nonrelativistic limit is accurately reproduced when using low incident kinetic energies. At high energies, relativistic and spin effects significantly affect the triple differential cross sections. Our analytical approach which seems exact is compa…
Recently introduced time-dependent renormalized natural orbital theory (TDRNOT) is tested on non-sequential double ionization (NSDI) of a numerically exactly solvable one-dimensional model He atom subject to few-cycle, 800-nm laser pulses. NSDI of atoms in strong laser fields is a prime example of non-perturbative, highly correlated electron dynamics. As such, NSDI is an important "worst-case" benchmark for any time-dependent few and many-body technique beyond linear response. It is found that TDRNOT reproduces the celebrated NSDI "knee," i.e., a many-order-of-magnitude enhancement of the doub…
Electron wave function entanglement and spin reconfiguration as source of electron correlation are investigated. Properties of correlation function are shown to have the best concordance with experimental data under supposition that probability of change of electron state to triplet state is about 0.5 or more.
We review the main aspects of multiple photoionization processes in atoms exposed to intense, short wavelength radiation. The main focus is the theoretical framework for the description of such processes as well as the conditions under which direct multiphoton multiple ionization processes can dominate over the sequential ones. We discuss in detail the mechanisms available in different wavelength ranges from the infrared to the hard X-rays. The effect of field fluctuations, present at this stage in all SASE free-electron-laser (FEL) facilities, as well as the effect of the interaction volume i…
Visualizing intense laser field driven electron dynamics in a multielectron molecule: dynamic electron localization, bonding properties and multiple ionization bursts
In the first part of this paper, the different distinguishable pathways and regions of the single and sequential double ionization are determined and discussed. It is shown that there are two distinguishable pathways for the single ionization and four distinct pathways for the sequential double ionization. It is also shown that there are two and three different regions of space which are related to the single and double ionization respectively. In the second part of the paper, the time dependent Schrödinger and Newton equations are solved simultaneously for the electrons and the nuclei of H$_2…
