We introduce a unified and simplified theory of atomic double ionization. Our results show that at high laser intensities ($I \ge 10^{14}$ watts/cm$^2$) purely classical correlation is strong enough to account for all of the main features observed in experiments to date.
This is a Reply on the proceeding comment on our paper titled "Classical Simulations Including Electron Correlations for Sequential Double Ionization".
Multielectron double ionization with elliptically polarized light is examined theoretically using a classical ensemble method going beyond the single-active-electron approximation. A knee structure in the ion signal is found. Our analysis provides an explanation for newly observed SDI phenomena.
Above 54.4 eV, two-photon double ionization of helium is dominated by a sequential absorption process, producing characteristic behavior in the single and triple differential cross sections. We show that the signature of this process is visible in the nuclear recoil cross section, integrated over all energy sharings of the ejected electrons, even below the threshold for the sequential process. Since nuclear recoil momentum imaging does not require coincident photoelectron measurement, the predicted images present a viable target for future experiments with new short-pulse VUV and soft X-ray so…
We take advantage of the information provided by use of elliptical polarization in a recent two-electron release time experiment [A.N. Pfeiffer et al., Nature Physics 7, 428 (2011)]. This allows a comparative test of the currently dominant conjectures regarding independent-electron tunneling theory vs. fully electron-correlated classical release theory to describe electron release in strong-field double ionization.
With a classical ensemble model that including electron correlations during the whole ionization process, we investigated strong-field sequential double ionization of Ar by elliptically polarized pulses at the quantitative level. The experimentally observed intensity-dependent three-band or four-band structures in the ion momentum distributions are well reproduced with this classical model. More importantly, the experimentally measured ionization time of the second electrons [A. N. Pfeiffer et al., Nature Phys. 7, 428 (2011)], which can not be predicted by the standard independent-electron mod…
A simple model for sequential multiphoton ionization by ultra-intense x-rays is presented. The derived scaling of the ion yield with pulse energy quantitatively reproduces the experimental data, which shows that the ion yield increases according to the "power law" behavior typical of multiphoton ionization, followed by saturation at high pulse energies. The calculated average time interval between ionizations for producing ions at a certain charge state is found to be proportional to the pulse duration and independent of all other x-ray pulse parameters. This agrees with previous studies where…
We report full-dimensionality quantum and classical calculations for double ionization of laser-driven helium at 390 nm. Good qualitative agreement is observed. We show that the classical double ionization trajectories can be divided into two distinct pathways: direct and delayed. The direct pathway, with an almost simultaneous ejection of both electrons, emerges from small laser intensities. With increasing intensity its relative importance, compared to the delayed ionization pathway, increases until it becomes the predominant pathway for total electron escape energy below around 5.25 $U_{p}$…
Owing to its numerical simplicity, a two-dimensional two-electron model atom, with each electron moving in one direction, is an ideal system to study non-perturbatively a fully correlated atom exposed to a laser field. Frequently made assumptions, such as the ``single active electron''- approach and calculational approximations, e.g. time dependent density functional theory or (semi-) classical techniques, can be tested. In this paper we examine the multiphoton short pulse-regime. We observe ``non-sequential'' ionization, i.e.\ double ionization at lower field strengths as expected from a sequ…
The experimental observations of sequential double ionization (SDI) of Ar [A. N. Pfeiffer {\it et al.}, Nature Phys. {\bf 7}, 428 (2011)], such as the four-peak momentum distribution and the ionization time of the first and second electrons, are investigated and reproduced with a quantum model by including and excluding the $e$-$e$ correlation effect. Based on the comparison of experiment and simulation, the role of $e$-$e$ correlation in SDI is discussed. It is shown that the inclusion of $e$-$e$ correlation is necessary to reproduce the momentum distribution of electrons.
We report on non-sequential double ionization of Ar by a laser pulse consisting of two counter rotating circularly polarized fields (390 nm and 780 nm). The double ionization probability depends strongly on the relative intensity of the two fields and shows a "knee"-like structure as function of intensity. We conclude that double ionization is driven by a beam of nearly monoenergetic recolliding electrons, which can be controlled in intensity and energy by the field parameters. The electron momentum distributions show the recolliding electron as well as a second electron which escapes from an …
Breakdown of sequential tunnel ionization in ultrashort electromagnetic pulses
National Research Nuclear University MEPhI(国立研究核大学);P.N. Lebedev Physical Institute of the Russian Academy of Sciences(俄罗斯科学院列别捷夫物理研究所);Prokhorov General Physics Institute of the Russian Academy of Sciences(俄罗斯科学院普罗霍罗夫普通物理研究所)
We consider the final stage of double ionization of $\rm O_2$ molecules by short linearly polarized laser pulses. The saddles of the effective adiabatic potential energy close to which simultaneous escape of electrons from a molecule takes place are identified. The analysis of the saddles and numerical simulations of the ionization indicate that to observe clear signatures of simultaneous electron escape in double ionization of $\rm O_2$ molecules stronger and much shorter laser pulses than those used in the recent experiment [E. Eremina, {\it et al}, Phys. Rev. Lett. {\bf 92}, 173001 (2004)] …
Double ionization in intense laser fields can comprise electron correlations, which manifest in the non-independent emission of two electrons from an atom or molecule. However, experimental methods that directly access the electron emission times have been scarce. Here, we explore the application of an all-optical streaking technique to strong-field double ionization both theoretically and experimentally. We show that both sequential and non-sequential double ionization processes lead to streaking delays that are distinct from each other and single ionization. Moreover, coincidence detection o…
At intensities below-the-recollision threshold, we show that re-collision-induced excitation with one electron escaping fast after re-collision and the other electron escaping with a time delay via a Coulomb slingshot motion is one of the most important mechanisms of non-sequential double ionization, for strongly-driven He at 400 nm. Slingshot-NSDI is a general mechanism present for a wide range of low intensities and pulse durations. Anti-correlated two-electron escape is its striking hallmark. This mechanism offers an alternative explanation of anti-correlated two-electron escape obtained in…
We study double ionization of He driven by a near-single-cycle laser pulse at low intensities at 400 nm. Using a three-dimensional semiclassical model, we identify the pathways that prevail non-sequential double ionization (NSDI). We focus mostly on the delayed pathway, where one electron ionizes with a time-delay after recollision. We have recently shown that the mechanism that prevails the delayed pathway depends on intensity. For low intensities slingshot-NSDI is the mechanism that prevails. Here, we identify the differences in two-electron probability distributions of the prevailing NSDI p…
We study the resonant sequential two-photon ionization of neutral atoms by a combination of twisted- and plane-wave light within a fully relativistic framework. In particular, the ionization of an isotropic ensemble of neutral sodium atoms ($Z = 11$) from their ground $3^{2}S_{1/2}$ state via the $3^{2}P_{3/2}$ level is considered. We investigate in details the influence of the kinematic parameters of incoming twisted radiation on the photoelectron angular distribution and the circular dichroism. Moreover we study the influence of the geometry of the process on these quantities. This is perfor…
We perform high-resolution measurements of momentum distribution on Rb$^{n+}$ recoil ions up to charge state $n=4$, where laser-cooled rubidium atoms are ionized by femtosecond elliptically polarized lasers with the pulse duration of 35 fs and the intensity of 3.3$\times$10$^{15}$ W/cm$^2$ in the over-barrier ionization (OBI) regime. The momentum distributions of the recoil ions are found to exhibit multi-band structures as the ellipticity varies from the linear to circular polarizations. The origin of these band structures can be explained quantitatively by the classical OBI model and dedicat…
Fully accounting for non-dipole effects in the electron dynamics, double ionization is studied for He driven by a near-infrared laser field and for Xe driven by a mid-infrared laser field. Using a three-dimensional semiclassical model, the average sum of the electron momenta along the propagation direction of the laser field is computed. This sum is found to be an order of magnitude larger than twice the average electron momentum along the propagation direction of the laser field in single ionization. Moreover, the average sum of the electron momenta in double ionization is found to be maximum…
Two-electron correlated spectra of non-sequential double ionization below laser-intensity threshold are known to exhibit back-to-back scattering of the electrons, viz., the anticorrelation of the electrons. Currently, the widely accepted interpretation of the anticorrelation is recollision-induced excitation of the ion plus subsequent field ionization of the second electron. We argue that another mechanism, namely simultaneous electron emission, when the time of return of the rescattered electron is equal to the time of liberation of the bounded electron (the ion has no time for excitation), c…
Exchange correlation plays an important role in double-ionization of complex atoms by ultrashort laser pulse. In this work, we investigate two-photon double inner-shell electron ionization of neon induced by an attosecond extreme ultraviolent pulse in the framework of the quantum master equation. Our simulations reveal a distinct non-sequential effect via broadened double peaks, as a result of energy sharing between the two ionized electrons. When dissipation is included to show the interplay of coherence and decoherence, the two-photon double-ionization scaling law breaks down. We further stu…
Double ionization of diatomic molecules by short linearly polarized laser pulses is analyzed. We consider the final stage of the ionization process, that is the decay of a highly excited two electron molecule, which is formed after re-scattering. The saddles of the effective adiabatic potential energy close to which simultaneous escape of electrons takes place are identified. Numerical simulations of the ionization of molecules show that the process can be dominated by either sequential or non-sequential events. In order to increase the ratio of non-sequential to sequential ionizations very sh…
We predict new end-of-pulse behavior in high-field atomic double ionization. Calculations of atomic electron trajectories in short intense laser pulses confirm our analysis of elliptical polarization. We exhibit a four-band structure in ion momentum distributions under various ellipticities, and predict that sequential and non-sequential double ionization can be cleanly distinguished under elliptical polarization.
We investigate the possibility to deduce momentum space properties from time-dependent density functional calculations. Electron and ion momentum distributions after double ionization of a model Helium atom in a strong few-cycle laser pulse are studied. We show that, in this case, the choice of suitable functionals for the observables is considerably more important than the choice of the correlation potential in the time-dependent Kohn-Sham equations. By comparison with the solution of the time-dependent Schroedinger equation, the insufficiency of functionals neglecting electron correlation is…
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 $μ$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 $3\cdot10^{12} $W$\cdot$cm$^{-2}$. By tuning the photon energy across the threshold for the sequential …
A three-dimensional semiclassical model is used to study double ionization of Ar when driven by a near-infrared and near-single-cycle laser pulse for intensities ranging from 0.85$\times$10$^{14}$ W/cm$^{2}$ to 5$\times$10$^{14}$ W/cm$^{2}$. Asymmetry parameters, distributions of the sum of the two electron momentum components along the direction of the polarization of the laser field and correlated momenta are computed as a function of intensity and of the carrier envelope phase. A very good agreement is found with recently obtained results in kinematically complete experiments employing near…
We demonstrate kinematically complete measurements on frustrated double ionization of argon atoms in strong laser fields with a reaction microscope. We found that the electron trapping probability after strong field double ionization is much higher than that after strong field single ionization, especially in case of high laser intensity. The retrieved electron momentum distributions of frustrated double ionization show a clear transition from the nonsequential to the sequential regime, similar to those of strong field double ionization. The dependence of electron momentum width on the laser i…
Quantum calculations of a 1+1-dimensional model for double ionization in strong laser fields are used to trace the time evolution from the ground state through ionization and rescattering to the two electron escape. The subspace of symmetric escape, a prime characteristic of nonsequential double ionization, remains accessible by a judicious choice of 1-d coordinates for the electrons. The time resolved ionization fluxes show the onset of single and double ionization, the sequence of events during the pulse, and the influences of pulse duration, and reveal the relative importance of sequential …
We examine the nature and statistical properties of electron-electron collisions in the recollision process in a strong laser field. The separation of the double ionization yield into sequential and nonsequential components leads to a bell-shaped curve for the nonsequential probability and a monotonically rising one for the sequential process. We identify key features of the nonsequential process and connect our findings in a simplified model which reproduces the knee shape for the probability of double ionization with laser intensity and associated trends.
We describe first-principles in-plane calculations of non-sequential triple ionization (NSTI) of atoms in a linearly polarized intense laser pulse. In a fully classically correlated description, all three electrons respond dynamically to the nuclear attraction, the pairwise e-e repulsions and the laser force throughout the duration of a 780nm laser pulse. Nonsequential ejection is shown to occur in a multi-electron, possibly multi-cycle and multi-dimensional, rescattering sequence that is coordinated by a number of sharp transverse recollimation impacts.
For two-electron diatomic molecules, we investigate magnetic field effects in non-sequential double ionization where recollisions prevail. We do so by formulating a three-dimensional semi-classical model that fully accounts for the Coulomb singularities and for magnetic field effects during time propagation. Using this model, we identify a prominent signature of non-dipole effects. Namely, we demonstrate that the recolliding electron back-scatters along the direction of light propagation. Hence, this electron escapes opposite to the direction of change in momentum due to the magnetic field. Th…
We explore the influence of elliptical polarization on the (non)sequential two-photon double ionization of atomic helium with ultrashort extreme ultraviolet (XUV) light fields using time-dependent full ab-initio simulations. The energy and angular distributions of photoelectrons are found to be strongly dependent on the ellipticity. The correlation minimum in the joint angular distribution becomes more prominently visible with increasing ellipticity. In a pump-probe sequence of two subsequent XUV pulses with varying ellipticities, polarization tagging allows to discriminate between sequential …
Electron-electron correlation effects play an instrumental role in our understanding of sequential (SDI) and non-sequential double ionization (NSDI) mechanisms. Here, we present a theoretical study of NSDI driven by plasmonic-enhanced spatial inhomogeneous fields. By numerically solving the time-dependent Schrödinger equation for a linear reduced model of He and a double-electron time-evolution probability analysis, we provide evidence for the enhancement effects in NSDI showing that the double ionization yield at lower laser peak intensities is increased due to the inhomogeneity of the laser …
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 the first theoretical treatment of the formation of highly excited neutral H atoms (H$^{*}$) for strongly driven H$_{2}$. This process, with one electron ionizing and one captured in a Rydberg state, was recently reported in an experimental study in Phys. Rev. Lett {\bf 102} 113002 (2009). We show that two mechanisms underlie this process: a non-sequential one resembling non-sequential double ionization, and a sequential one resembling double ionization through enhanced ionization. We also predict a new feature, asymmetric energy sharing between H$^{*}$ and H$^{+}$ with increasing i…
The degree of elliptical polarization of intense short laser pulses is shown to be related to the timing of strong-field non-sequential double ionization. Higher ellipticity is predicted to force the initiation of double ionization into a narrower time window, and this "pins" the ionizing field strength in an unexpected way, leading to the first experimentally testable formula for double ionization probability as a function of ellipticity.
We study ab initio computations of the interaction of Lithium with a strong laser field. Numerical solutions of the time-dependent fully-correlated three-particle Schroedinger equation restricted to the one-dimensional soft-core approximation are presented. Our results show a clear transition from non-sequential to sequential double ionization for increasing intensities. Non sequential double ionization is found to be sensitive to the spin configuration of the ionized pair. This asymmetry, also found in experiments of photoionization of Li with synchrotron radiation, shows the evidence of the …
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 modern Free-Electron-Lasers generate a highly intense polarized radiation which initiate a sequence of ionization and decay events. Their probability depends on the polarization of each state as function of time. Its complete accounting is limited by the fact that a state can be formed in various ways. Here we present the equivalent of rate equations for population that completely accounts polarization of radiation and formulated in terms of the statistical tensors. To illustrate our approach we theoretically consider sequential photoionization of krypton by an intense extreme ultraviolet …
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…
The multiconfigurational time-dependent Hartree-Fock method (MCTDHF) is applied for simulations of the two-photon ionization of Helium. We present results for the single- and double ionization from the groundstate for photon energies in the non-sequential regime, and compare them to direct solutions of the Schrödinger equation using the time-dependent (full) Configuration Interaction method (TDCI). We find that the single-ionization is accurately reproduced by MCTDHF, whereas the double ionization results correctly capture the main trends of TDCI.
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…
We explore the dependence of the double ionization of the He atom on the frequency of a strong laser field while keeping the ponderomotive energy constant. As we increase the frequency we find that the remarkable "finger-like" structure for high momenta recently found for $ω=0.055$ a.u. \cite{Staudte, Rudenko} persists for higher frequencies. At the same time, at $ω=0.187$ a.u. a new X-shape structure emerges for small momenta that prevails in the correlated momenta distribution. The role of this structure as a signature of the frequency dependence of non-sequential double ionization is discus…
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 show the details of the pathway for dissociative ionization process of ground electronic state of aligned D$^{+}_{2}$ due to first ionization of D$_2$ in short ($\thicksim$100 fs) and intense ($4.0\times10^{14}$ W cm$^{-2}$) 480 nm laser pulses. The initial vibrational state of D$^{+}_{2}$ comes from the vertical transformation of the ground state of D$_{2}$. The initial wavepacket in the ground electronic state of D$_{2}^{+}$ is outgoing through dissociation-ionization channel accompanied by a strong coupling between $1s σ_{g}$ and $2p σ_{u}$ electronic states. We show explicitly that the …
For a model atom with the $p^3$ valence shell we construct consistent three- and two-active electrons models enabling their direct comparison. Within these models, we study the influence of the third active electron on the double ionization yield in strong femtosecond laser fields. We reveal proportionality between double ionization signals obtained with both models in the field intensity region where non-sequential ionization dominates. We derive analytically a correspondence rule connecting the double ionization yields obtained within the three- and two-active electrons models.
A molecular rotation assisted non-sequential double ionization (MR-NSDI) mechanism is identified in the breakup of rotational H$_2$ molecules in a few-cycle intense laser pulse using a semi-classical trajectory Monte Carlo method. Applying a molecular source in an appropriate rotational state could intensively boost NSDI probability, and conclude with an additional small anti-correlated electron momentum distribution. It reveals the critical role of the continuous dynamics of molecular rotation, which assists the recollision process and subsequently releases the excited electron from the poten…
We show through simulation that quantum interference in non-sequential double ionization can be used to control the recollision with subsequent ionization (RESI) mechanism. This includes the shape, localization and symmetry of RESI electron-momentum distributions, which may be shifted from a correlated to an anti-correlated distribution or vice versa, far below the direct ionization threshold intensity. As a testing ground, we reproduce recent experimental results by employing specific coherent superpositions of excitation channels. We examine two types of interference, from electron indisting…
Longitudinal momentum spectra and electron drift directions are considered for several laser wavelengths in Non-Sequential Double Ionization of helium using three dimensional classical ensembles. In this model, the familiar doublet for wavelength 800 nm and intensities of order 0.5 PW/cm^2, becomes a triplet for wavelength 1314 nm, then a doublet with plateau for 2017 nm. The results are explained based on whether the post-ionization impulse from the laser results in backward drift for one or both electrons.
We report on the observation of discrete structures in the electron energy distribution for strong field double ionization of Argon at 394 nm. The experimental conditions were chosen in order to ensure a non-sequential ejection of both electrons with an intermediate rescattering step. We have found discrete ATI (above-threshold ionization) like peaks in the sum energy of both electrons, as predicted by all quantum mechanical calculations. More surprisingly however is the observation of two ATI combs in the energy distribution of the individual electrons.
It has been recently predicted theoretically that due to nuclear motion light and heavy hydrogen molecules exposed to strong electric field should exhibit substantially different tunneling ionization rates (O.I. Tolstikhin, H.J. Worner and T. Morishita, Phys. Rev. A 87, 041401(R) (2013) [1]). We studied that isotope effect experimentally by measuring relative ionization yields for each species in a mixed H2/D2 gas jet interacting with intense femtosecond laser pulses. In a reaction microscope apparatus we detected ionic fragments from all contributing channels (single ionization, dissociation,…
We study the double ionization of atoms subjected to circularly polarized (CP) laser pulses. We analyze two fundamental ionization processes: the sequential (SDI) and non-sequential (NSDI) double ionization in the light of the rotating frame (RF) which naturally embeds nonadiabatic effects in CP pulses. We use and compare two adiabatic approximations: The adiabatic approximation in the laboratory frame (LF) and the adiabatic approximation in the RF. The adiabatic approximation in the RF encapsulates the energy variations of the electrons on subcycle timescales happening in the LF and this, by …
We report the observation of multiple ionization of Argon through multi-XUV-photon absorption induced by an unprecedentedly powerful laser driven high-harmonic-generation source. Comparing the measured intensity dependence of the yield of the different Argon charge states with numerical calculations we can infer the different channels -direct and sequential- underlying the interaction. While such studies were feasible so far only with FEL sources, this work connects highly-non-linear-XUV-processes with the ultra-short time scales, inherent to the harmonic pulses, and highlights the advanced pe…
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…