Signatures of magnetic field effects in non-sequential double ionization manifesting as back-scattering for molecules versus forward-scattering for atoms
Georgios Petros Katsoulis, Matthew Benjamin Peters, André Staudte, Ravi Bhardwaj, Agapi Emmanouilidou
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. This is in striking contrast to strongly-driven atoms where the recolliding electron forward-scatters along the direction of light propagation. We attribute these distinct signatures to the different gate that the magnetic field creates jointly with a soft recollision in molecules compared to a hard recollision in atoms. These two different gates give rise, shortly before recollision, to different momenta and positions of the recolliding electron along the direction of light propagation. As a result, we show that the Coulomb forces from the nuclei act to back-scatter the recolliding electron in molecules and forward-scatter it in atoms along the direction of light propagation.
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.
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 $U_{p}$…
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…
We present a theoretical model for atomic hydrogen ionization by electron impact in the instantaneous approximation and the more accurate non-instantaneous approach using the methods of Quantum Electrodynamics, for the binary coplanar and the coplanar asymmetric geometries. All electrons are described by plane wave functions in the coplanar binary geometry but in the asymmetric geometry the ejected electron is described by a Sommerfeld-Maue wave function. It is shown that the two models give the same results in the non relativistic limit for the binary coplanar geometry where the interactions …
We study double ionization (DI) dynamics of vibrating HeH$^+$ versus its isotopic variant HeT$^+$ in strong laser fields numerically. Our simulations show that for both cases, these two electrons in DI prefer to release together along the H(T) side. At the same time, however, the single ionization (SI) is preferred when the first electron escapes along the He side. This potential mechanism is attributed to the interplay of the rescattering of the first electron and the Coulomb induced large ionization time lag. On the other hand, the nuclear motion increases the contributions of these two elec…
In this paper we present Classical Trajectory Monte Carlo (CTMC) calculations for single and multiple electron ionization of Argon atoms and ions in the threshold region. We are able to recover the Wannier exponents a for the power-law behavior of the cross section s versus excess energy: the exact value of the exponent as well as the existence of its saturation for multiple ionization appear to be related to how the total binding energy is shared between target electrons.
We analyze the dynamical processes behind delayed double ionization of atoms subjected to strong laser pulses. Using reduced models, we show that these processes are a signature of Hamiltonian chaos which results from the competition between the laser field and the Coulomb attraction to the nucleus. In particular, we exhibit the paramount role of the unstable manifold of selected periodic orbits which lead to a delay in these double ionizations. Among delayed double ionizations, we consider the case of "Recollision Excitation with Subsequent Ionization" (RESI) and, as a hallmark of this mechan…
We revisit the stabilization of ionization of atoms subjected to a superintense laser pulse using nonlinear dynamics. We provide an explanation for the lack of complete ionization at high intensity and for the decrease of the ionization probability as intensity is increased. We investigate the role of each part of the laser pulse (ramp-up, plateau, ramp-down) in this process. We emphasize the role of the choice for the ionization criterion, energy versus distance criterion.
The measurement of the tunneling time in attosecond experiments, termed attoclock, triggered a hot debate about the tunneling time, the role of time in quantum mechanics, where the interaction with the laser pulse involves two regimes of a different character, the multiphoton and the tunneling (field-) ionization. In the adiabatic field calibration, one of us (O. K.) developed in earlier works a real tunneling time model and showed that the model fits well to the experimental data of Landsmann et al. (Optica {\bf 1}, 343 2014). In the present work, it is shown that the model explains the exper…
We describe the influence of electron-impact multiple ionization (EIMI) on the ionization balance of collisionally ionized plasmas. We are unaware of any previous ionization balance calculations that have included EIMI, which is usually assumed to be unimportant. Here, we incorporate EIMI cross-section data into calculations of both equilibrium and non-equilibrium charge-state distributions (CSDs). For equilibrium CSDs, we find that EIMI has only a small effect and can usually be ignored. However, for non-equilibrium plasmas the influence of EIMI can be important. In particular, we find that f…
Few-photon induced breakup of helium is studied using a newly developed ab initio numerical framework for solving the six-dimensional time-dependent Schroedinger equation. We present details of the method and calculate (generalized) cross sections for the process of two-photon nonsequential (direct) double ionization at photon energies ranging from 39.4 to 54.4 eV, a process that has been very much debated in recent years and is not yet fully understood. In particular, we have studied the convergence property of the total cross section in the vicinity of the upper threshold (54.4 eV), versus t…
We study the behavior of reduced models for the propagation of intense laser pulses in atomic gases. The models we consider incorporate ionization, blueshifting, and other nonlinear propagation effects in an ab initio manner, by explicitly taking into account the microscopic electron dynamics. Numerical simulations of the propagation of ultrashort linearly-polarized and elliptically-polarized laser pulses over experimentally-relevant propagation distances are presented. We compare the behavior of models where the electrons are treated classically with those where they are treated quantum-mecha…
Using a semiclassical model which incorporates tunneling and Coulomb field effects, the origin of the unexpected low-energy structure (LES) in above-threshold ionization spectrum observed in recent experiments [C. I. Blaga et al., Nature Phys. {\bf 5}, 335 (2009) and W. Quanet al., Phys. Rev. Lett. {\bf 103}, 093001 (2009)] is identified. We show that the LES arises due to an interplay between multiple forward scattering of an ionized electron and the electron momentum disturbance by the Coulomb field immediately after the ionization. The multiple forward scattering is mainly responsible for t…
The charge transfer (ionization) of hydrogen Rydberg atoms (principal quantum number $n=25-34$) incident at a Cu(100) surface is investigated. Unlike fully metallic surfaces, where the Rydberg electron energy is degenerate with the conduction band of the metal, the Cu(100) surface has a projected bandgap at these energies, and only discrete image states are available through which charge transfer can take place. Resonant enhancement of charge transfer is observed at hydrogen principal quantum numbers for which the Rydberg energy matches the energy of one of the image states. The integrated sur…
To measure the mass of the electron neutrino, the "Electron Capture in Holmium-163" (ECHo) collaboration aims at calorimetrically measuring the spectrum following electron capture in $^{163}$Ho. The success of the ECHo experiment depends critically on the radiochemical purity of the $^{163}$Ho sample, which is ion-implanted into the calorimeters. For this, a $30 \, \textrm{kV}$ high transmission magnetic mass separator equipped with a resonance ionization laser ion source is used. To meet the ECHo requirements, the ion source unit was optimized with respect to its thermal characteristics and m…
We study the photoionization properties of the C_60 versus C_240 molecule in a spherical jellium frame of density functional method. Two different approximations to the exchange-correlation (xc) functional are used: (i) The Gunnerson-Lundqvist parametrization [Phys. Rev. B 13, 4274 (1976)] with an explicit correction for the electron self-interaction (SIC) and (ii) a gradient-dependent augmentation of (i) by using the van Leeuwen and Baerends model potential [Phys. Rev. A 49, 2421 (1994)], in lieu of SIC, to implicitly restore electrons' asymptotic properties. Ground state results from the two…
The directional control of molecular dissociation with the laser electric field waveform is a paradigm and was demonstrated for a variety of molecules. In most cases, the directional control occurs via a dissociative ionization pathway. The role of laser-induced coupling of electronic states in the dissociating ion versus selective ionization of oriented neutral molecules, however, could not be distinguished for even small heteronuclear molecules such as CO. Here, we introduce a technique, using elliptically polarized pump and linearly polarized two-color probe pulses that unambiguously distin…
Transition of an electron from a free to a bound state is critical in determining the qualitative shape of the spectrum in high-order harmonic generation (HHG), and in tomographic imaging of orbitals. We calculate and compare the recombination amplitude, from a continuum state described by a plane wave and an outgoing scattering eigenstate, to the bound state for the noble gases that are commonly used in HHG. These calculations are based on the single active electron model and the Hartree-Fock-Slater method, using both the length form and the acceleration form of the dipole matrix element. We …
