Quasi-static models of barrier suppression have played a major role in our understanding of the ionization of atoms and molecules in strong laser fields. Despite their success, in the case of diatomic molecules these studies have so far been restricted to fields aligned with the molecular axis. In this paper we investigate the locations and heights of the potential barriers in the hydrogen molecular ion in an electric field of arbitrary orientation. We find that the barriers undergo bifurcations as the external field strength and direction are varied. This phenomenon represents an unexpected level of intricacy even on this most elementary level of the dynamics. We describe the dynamics of tunnelling ionization through the barriers semiclassically and use our results to shed new light on the success of a recent theory of molecular tunnelling ionization as well as earlier theories that restrict the electric field to be aligned with the molecular axis.
We review the semiclassical two-step model for strong-field ionization. The semiclassical two-step model describes quantum interference and accounts for the ionic potential beyond the semiclassical perturbation theory. We discuss formulation and implementation of this model, its further developments, as well as some of the applications. The reviewed applications of the model include strong-field holography with photoelectrons, multielectron polarization effects in ionization by an intense laser pulse, and strong-field ionization of the hydrogen molecule.
We present a mixed quantum-classical approach to strong-field ionization - a semiclassical two-step model with quantum input. In this model the initial conditions for classical trajectories that simulate electron wave packet after ionization are determined by the exact quantum dynamics. As a result, the model allows to overcome deficiencies of standard semiclassical approaches in describing the ionization step. The comparison with the exact numerical solution of the time-dependent Schrödinger equation shows that for ionization of a one-dimensional atom the model yields quantitative agreement w…
Fully differential cross sections are calculated for the ionization of H$_2$ by fast charged projectiles using a semiclassical model developed previously for the ionization of atoms. The method is tested in case of 4 keV electron and 6 MeV proton projectiles. The obtained results show good agreement with the available experimental data. Interference effects due to the two-center character of the target are also observed and analyzed.
We extend the semiclassical two-step model for strong-field ionization that describes quantum interference and accounts for the Coulomb potential beyond the semiclassical perturbation theory to the hydrogen molecule. In the simplest case of the molecule oriented along the polarization direction of a linearly polarized laser field, we predict significant deviations of the two-dimensional photoelectron momentum distributions and the energy spectra from the case of atomic hydrogen. Specifically, for the hydrogen molecule the electron energy spectrum falls off slower with increasing energy, and th…
We present a semiclassical two-step model for strong-field ionization that accounts for path interferences of tunnel-ionized electrons in the ionic potential beyond perturbation theory. Within the framework of a classical trajectory Monte-Carlo representation of the phase-space dynamics, the model employs the semiclassical approximation to the phase of the full quantum propagator in the exit channel. By comparison with the exact numerical solution of the time-dependent Schrödinger equation for strong-field ionization of hydrogen, we show that for suitable choices of the momentum distribution a…
In the semiclassical picture of photoionization process in intense laser fields, the ionization rate solely depends on the amplitude of the electric field and the final photoelectron momentum corresponds to the instant of ionization of the photoelectron, however, this picture has never been checked rigorously. Recently an attosecond angular streaking technique based on this semiclassical perspective has been widely applied to temporal measurement of the atomic and molecular dynamics in intense laser fields. We use a Wigner-distribution-like function to calculate the time-emission angle distrib…
The electron impact ionization of atomic hydrogen is calculated for incident elrctron energy 76.46 eV. The Hartree-Fock approximation is used to calculate the initial state which includes both bound and continum wave functions. The final state continuum electron wave functions are obtained in the potential of hydrogen ion. The interaction between the two final state continuum electrons is approximated with the screening potential determined variationally.
A new relativistic method based on the Dirac equation for calculating fully differential cross sections for ionization in ion-atom collisions is developed. The method is applied to ionization of the atomic hydrogen by antiproton impact, as a non-relativistic benchmark. The fully differential, as well as various doubly and singly differential cross sections for ionization are presented. The role of the interaction between the projectile and the target nucleus is discussed. Several discrepancies in available theoretical predictions are resolved. The relativistic effects are studied for ionizatio…
We present both full quantum mechanical and semiclassical calculations of above threshold ionization (ATI) of a hydrogen atom in the tunneling regime by a few-cycle linearly polarized infrared laser pulse. As a quantum treatment, we applied the direct integration of the time dependent Schrödinger equation (TDSE). In the semiclassical approximation (SCA), it is assumed that wavepacket propagation in the post-tunneling process can be well described within the classical framework. With these two methods, we analyze the similarities and deviations for ionization of the hydrogen atom. We found that…
We have implemented the paraxial approximation followed by the time-dependent Hartree-Fock method with frozen core for the single impact ionization of atoms and two-atomic molecules. It reduces the original scattering problem to the five-dimensional time-dependent Schrödinger equation solution. By using this method we calculated the multi-fold differential cross section of the impact single ionization of the helium atom, the hydrogen molecule and the nitrogen molecule by the intermediate energy electrons. Our results for the helium and the hydrogen are quite close to experimental data, but for…
We studied nonrelativistic collision of antiproton with hydrogen atom by solving time-dependent Schrodinger equation numerically. Coulomb wave function discrete variable method (CWDVR) had been used to calculate electron wave function evolution, while projectile defined classically, moving along the straight line trajectories with constant velocity. The ionization amplitude calculated by projection of the wave function into continuum wave function of the hydrogen electron. The fully differential cross sections calculated depending on projectile impact energy, scattering angle and electron ejec…
Experiments have shown that the microwave ionization probability of a highly excited almost monodimensional hydrogen atom subjected to a microwave pulse sometimes grows in steps when the peak electric field of the pulse is increased. Classical pulsed simulations display the same steps, which have been traced to phase-space metamorphoses. Quantum numerical calculations again exhibit the same ionization steps. I show that the time-sequence of two level interactions, responsible for the observed steps in the quantum picture, is strictly related to the classical phase space structures generated by…
Relativistic strong-field ionization of hydrogen-like atoms or ions in a constant crossed electromagnetic field is studied. The transition amplitude is formulated within the strong-field approximation in Göppert-Mayer gauge, with initial and final electron states being described by the corresponding Dirac-Coulomb and Dirac-Volkov wave functions, respectively. Coulomb corrections to the electron motion during tunneling are taken into account by adjusting an established method to the present situation. Total and energy-differential ionization rates are calculated and compared with predictions fr…
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 investigate the strong-field ionization of atomic hydrogen in a few-cycle elliptically polarized infrared pulse by solving the time-dependent Schrödinger equation. The dependence of the photoelectron momentum distribution on the pulse intensity, ellipticity, length, envelope, and carrier envelope phase is analyzed. In particular, we explain the variation of the electron offset angle with asymptotic electron energy through the combined action of the field and the Coulomb potential, and demonstrate that low-ellipticity pulses make it possible to access the electron release time.
In this paper a 4-component Dirac theory of ionization of hydrogen molecular ion in a super-intense laser field is developed. Simple analytic expressions for the spin specific as well as the total ionization currents emitted from the ground state of the ion are derived. The results are given for all polarization and finite propagation vectors of the field. They apply for inner-shell ionization of analogous heavier molecular ions as well. The presence of molecular two-slit interference effect, first found in the non-relativistic case, and the spin-flip ionization current, and an asymmetry of th…
We present a theoretical study of the ionization dynamics of a hydrogen atom exposed to attosecond laser pulses in the extreme ultra violet region at very high intensities. The pulses are such that the electron is expected to reach relativistic velocities, thus necessitating a fully relativistic treatment. We solve the time dependent Dirac equation and compare its predictions with those of the corresponding non-relativistic Schr{ö}dinger equation. We find that as the electron is expected to reach about 20% of the speed of light, relativistic corrections introduces a finite yet small decrease i…
We calculate ionization energies and fundamental vibrational transitions for H$_2^+$, D$_2^+$, and HD$^+$ molecular ions. The NRQED expansion for the energy in terms of the fine structure constant $α$ is used. Previous calculations of orders $mα^6$ and $mα^7$ are improved by including second-order contributions due to the vibrational motion of nuclei. Furthermore, we evaluate the largest corrections at the order $mα^8$. That allows to reduce the fractional uncertainty to the level of $7\cdot10^{-12}$ for fundamental transitions and to $4\cdot10^{-12}$ for the ionization energies.
Electron-impact ionization of atomic hydrogen with the electron's anomalous mag- netic moment (AMM) effects are examined. The formulas for the laser-assisted relativis- tic triple differential cross section (TDCS) in the coplanar binary geometry developed earlier by Y. Attaourti and S. Taj [Phys. Rev. A 69, 063411 (2004)] are used to check the consistency of our computations when the anomaly $κ$ is taken to be zero. We show that the contribution of the terms containing the AMM effects even in the first Born approximation has an important contribution, so it must be included in any reliable ana…
Approximate scaling laws with respect to the nuclear charge are introduced for the time-dependent Dirac equation describing hydrogen-like ions subject to laser fields within the dipole approximation. In particular, scaling relations with respect to the laser wavelengths and peak intensities are discussed. The validity of the scaling relations is investigated for two-, three-, four-, and five-photon ionization of hydrogen-like ions with the nuclear charges ranging from $Z=1$ to $92$ by solving the corresponding time-dependent Dirac equations adopting the properly scaled laser parameters. Good a…
The tunneling ionization of a hydrogen atom excited in the presence of a static electric field is investigated for the case where, before being extracted, the electron has an orbital angular momentum L perpendicular to the field E. The escaping electron has a nonzero mean transverse velocity <vT> in the direction of E cross <L>. This asymmetry is similar to the Collins effect in the fragmentation into hadrons of a transversely polarized quark. In addition, the linear Stark effect make <L> and <vT> oscillate in time. The degree of asymmetry is calculated at leading order in E for an initial sta…
The alignment- and internuclear-distance dependent ionization of H$_2$ exposed to intense, ultrashort laser fields is studied by solving the time-dependent two-electron Schrödinger equation. In the regime of perturbative few-photon ionization, a strong dependence of the ionization yield on the internuclear distance is found. While this finding confirms a previously reported breakdown of the fixed-nuclei approximation for parallel alignment, a simpler explanation is provided and it is demonstrated that this breakdown is not due to vibrational dynamics during the laser pulse. The persistence of …
We present experimental data on the non-adiabatic strong field ionization of atomic hydrogen using elliptically polarized femtosecond laser pulses at a central wavelength of 390 nm. Our measured results are in very good agreement with a numerical solution of the time-dependent Schrödinger equation (TDSE). Experiment and TDSE show four above-threshold ionization (ATI) peaks in the electron's energy spectrum. The most probable emission angle (also known as 'attoclock-offset angle' or 'streaking angle') is found to increase with energy, a trend that is opposite to standard predictions based on Co…
We have implemented three variants of the exterior complex scaling procedure in prolate spheroidal coordinates (PS-ECS) to study the dissociative electron impact ionization-excitation of hydrogen molecule, where the emerging electrons and one of the protons are detected in coincidence for the first time in a recent experiment. In the first variant, designated PSECS-1B, the two target electrons are treated ab initio while the interaction of the incident-scattered electron is taken into account using the first term of the Born series. In the second, PSECS-2BCD, the second Born term is introduced…
We study the formation of highly excited neutral atoms during the break-up of strongly-driven molecules. Past work on this significant phenomenon has shown that during the formation of highly excited neutral atoms ($\mathrm{H^{*}}$) during the break-up of H$_{2}$ in a linear laser field the electron that escapes does so either very quickly or after remaining bound for a few periods of the laser field. Here, we address the electron-nuclear dynamics in $\mathrm{H^{*}}$ formation in elliptical laser fields, through Coulomb explosion. We show that with increasing ellipticity two-electron effects a…
In the recent work of Herath et al. [Phys. Rev. Lett. 109, 043004 (2012)] the first experimental observation of a dependence of strong-field ionization rate on the sign of the magnetic quantum number m (of the initial bound state (n,l.m)) was reported. The experiment with nearly circularly polarized light could not distinguish which sign of m favors faster ionization. We perform ab initio calculations for the hydrogen atom initially in one of the four bound sub states with the principal quantum number n=2 and irradiated by a short circularly polarized laser pulse of 800nm. In the intensity ran…
Optical vortex beams have an extensive history in terms of both theory and experiment, but only recently have electron vortex beams been proposed and realized. The possible applications of these matter vortex waves are numerous, but a fundamental understanding of their interactions with atoms and molecules has not yet been developed. In this work, fully differential cross sections for fast (e,2e) collisions using electron vortex projectiles with small amounts of quantized orbital angular momentum are presented. A comparison is made with the fully differential cross sections using plane wave pr…
The three-body dynamics of the ionization of the atomic hydrogen by 30 keV antiproton impact has been investigated by calculation of fully differential cross sections (FDCS) using the classical trajectory Monte Carlo (CTMC) method. The results of the calculations are compared with the predictions of quantum mechanical descriptions: The semi-classical time-dependent close-coupling theory, the fully quantal, time-independent close-coupling theory, and the continuum-distorted-wave-eikonal-initial-state model. In the analysis particular emphasis was put on the role of the nucleus-nucleus (NN) inte…
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…
Wavefunction-splitting or mask method, widely used in the non-relativistic calculations of the photoelectron angular distributions, is extended to the relativistic domain within the dipole approximation. Since the closed-form expressions for the relativistic Volkov states are not available within the dipole approximation, we build such states numerically solving a single second-order differential equation. We calculate the photoelectron energy spectra and angular distributions for highly charged ions under different ionization regimes with both the direct and the relativistic mask methods. We …
The existence of periodic orbit bunches is proven for the diamagnetic Kepler problem. Members of each bunch are reconnected differently at self-encounters in phase space but have nearly equal classical action and stability parameters. Orbits can be grouped already on the level of the symbolic dynamics by application of appropriate reconnection rules to the symbolic code in the ternary alphabet. The periodic orbit bunches can significantly improve the efficiency of semiclassical quantization methods for classically chaotic systems, which suffer from the exponential proliferation of orbits. For …
Positronium breakup versus hydrogen ionization in collisions with fast charged projectiles: a comparative study
Institute of Modern Physics, Chinese Academy of Sciences（中国科学院近代物理研究所）；Heinrich-Heine-University of Düsseldorf（杜塞尔多夫大学）；University of Chinese Academy of Sciences（中国科学院大学）
Time-dependent close-coupling calculations of the ionization and excitation cross section for antiproton collisions with molecular hydrogen ions are performed in an impact-energy range from 0.5 keV to 10 MeV. The Born-Oppenheimer and Franck-Condon approximations as well as the impact parameter method are applied in order to describe the target molecule and the collision process. It is shown that three perpendicular orientations of the molecular axis with respect to the trajectory are sufficient to accurately reproduce the ionization cross section calculated by [Sakimoto, Phys. Rev. A 71, 06270…
We perform ab initio calculations for the hydrogen atom initially in one of the six circular bound states with the principal quantum numbers n = 2, 3 and 4, irradiated by a short circularly polarized laser pulse of 400 nm. The field propagates in the direction parallel to the z-component of the angular momentum of the atom. We investigate probabilities for the atom to ionize or to get on some bound (excited) state or to remain in the initial state after the end of the laser pulse. In most cases, we find pronounced differences in ionization probabilities for atoms in states having different sig…
