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 electrons is marginal, with two almost degenerate transition configurations. The total number of configurations increases rapidly, from 2 configurations for three electrons up to 26 configurations for eight electrons.
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 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 dom…
The problem of Freeman resonances [R. R. Freeman \textit{et al.}, Phys. Rev. Lett. \textbf{59}, 1092 (1987)] when strong field ionization is enhanced due to the transient population of excited states during the ionization, is revisited. An intuitive model is put forward which explains the mechanism of the intermediate population of excited states during nonadiabatic tunneling ionization via the under-the-barrier recollision and recombination. The theoretical model is based on perturbative strong-field approximation (SFA), where the sub-barrier bound-continuum-bound pathway is described in the …
The two- and three-body Coulomb explosion of carbonyl sulfide (OCS) by 790 nm, 50 fs laser pulses focussed to $\approx $ 10$^{16}$ Wcm$^{-2}$ has been investigated by three-dimensional covariance mapping technique. For the first time in a triatomic molecule, a single charge state, in this case the trication, has been observed to dissociate into two distinct energy channels. With the aid of a three dimensional visualization technique to reveal the ionization hierarchy, evidence is presented for the existence of two sets of ionization pathways resulting from these two initial states. While one g…
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 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.
The attosecond ultrafast ionization dynamics of correlated two- or many-electron systems have, so far, been mainly addressed investigating atomic systems. In the case of single ionization, it is well known that electron-electron correlation modifies the ionization dynamics and observables beyond the single active electron picture, resulting in effects such as the Auger effect or shake-up/down and knock-up/down processes. Here, we extend these works by investigating the attosecond ionization of a molecular system involving correlated two-electron dynamics, as well as non-adiabatic nuclear dynam…
We present a multichannel photoelectron interferometry technique based on trichromatic pulse shaping for unambiguous determination of quantum phases in multiphoton ionization (MPI) of potassium atoms. The colors of the laser field are chosen to produce three energetically separated photoelectron interferograms in the continuum. While the red pulse is two-photon resonant with the $3d$-state resulting in a (2+1) resonance-enhanced MPI (REMPI), a (1+2) REMPI occurs via the non-resonant intermediate $4p$-state with an initial green or blue pulse. We show that ionization via a non-resonant intermed…
D$_2$ molecules, excited by linearly cross-polarized femtosecond extreme ultraviolet (XUV) and near-infrared (NIR) light pulses, reveal highly structured D$^+$ ion fragment momenta and angular distributions that originate from two different 4-step dissociative ionization pathways after four photon absorption (1 XUV + 3 NIR). We show that, even for very low dissociation kinetic energy release $\le$~240~meV, specific electronic excitation pathways can be identified and isolated in the final ion momentum distributions. With the aid of {\it ab initio} electronic structure and time-dependent Schröd…
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…
We address the concept of direct multiphoton multiple ionization in atoms exposed to intense, short wavelength radiation and explore the conditions under which such processes dominate over the sequential. Their contribution is shown to be quite robust, even under intensity fluctuations and interaction volume integration, and reasonable agreement with experimental data is also found.
We present a joint experimental and theoretical study on strong-field photo-ionization of sodium atoms using chirped femtosecond laser pulses. By tuning the chirp parameter, selectivity among the population in the highly excited states 5p, 6p, 7p and 5f, 6f is achieved. Different excitation pathways enabling control are identified by simultaneous ionization and measurement of photoelectron angular distributions employing the velocity map imaging technique. Free electron wave packets at an energy of around 1 eV are observed. These photoelectrons originate from two channels. The predominant 2+1+…
Selective field ionization is used to determine the state or distribution of states to which a Rydberg atom is excited. By evolving a small perturbation to the ramped electric field using a genetic algorithm, the shape of the time-resolved ionization signal can be controlled. This allows for separation of signals from pairs of states that would be indistinguishable with unperturbed selective field ionization. Measurements and calculations are presented that demonstrate this technique and shed light on how the perturbation directs the pathway of the electron to ionization. Pseudocode for the ge…
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…
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…
We present a rather elaborate theoretical model describing the dynamics of Neon under radiation of photon energies $\sim 93$ eV and pulse duration in the range of 15 fs, within the framework of Lowest non-vanishing Order of Perturbation Theory (LOPT), cast in terms of rate equations. Our model includes sequential as well as direct multiple ionization channels from the 2s and 2p atomic shells, including aspects of fine structure, whereas the stochastic nature of SASE-FEL light pulses is also taken into account. Our predictions for the ionization yields of the different ionic species are in exce…
Interferometrically Enhanced Asymmetry in Strong-field Ionization with Bright Squeezed Vacuum
Perimeter Institute for Theoretical Physics（Perimeter理论物理研究所）；University of Waterloo（滑铁卢大学）；University of Oxford（牛津大学）；University College London（伦敦大学学院）；ICFO – Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology（ICFO-光子科学研究所，巴塞罗那科技研究所）
We perform theoretical investigations of laser-induced nonsequential double ionization with few cycle pulses, with particular emphasis on the dependence of the electron-momentum distributions on the carrier-envelope phase. We focus on the recollision-excitation with subsequent tunneling ionization (RESI) pathway, in which a released electron, upon return to its parent ion, gives part of its kinetic energy to promote a second electron to an excited state. At a subsequent time, the second electron is freed through tunneling ionization. We show that the RESI electron-momentum distributions vary d…
We investigate the liberation of an atomic electron by a linearly polarized single-cycle near-infrared laser pulse having a peak intensity that ensures tunneling. Based on phase space analysis and energy distribution in the instantaneous potential, we reveal the importance of quantum interference between tunneling and over-the-barrier pathways of escape. Tunneling is blurred both in space and time, and the contribution of tunneling at the mean energy is almost negligible. We suggest and justify improved initial conditions for a classical particle approximation of strong-field ionization, based…
We propose an extension of coherent control using laser-synthesized free-electron matter waves. In contrast to coherent control schemes exploiting optical coherences to steer the dynamics of matter waves, we analyze the opposite and investigate the control of quantum light emission driven by laser-sculpted coherent free-electron matter waves. We apply this concept to the control of entangled photon-pair emission in electron-atom collisions, in which the incident electron wave packet, colliding with a target atom $B$, is engineered by interferometric resonantly-enhanced multiphoton ionization o…
