Ellipticity dependence of anticorrelation in the nonsequential double ionization of Ar.

Within the framework of the improved quantitative rescattering (QRS) model, we simulate the correlated two-electron momentum distributions (CMDs) for nonsequential double ionization (NSDI) of Ar by elliptically polarized laser pulses with a wavelength of 788 nm at an intensity of 0.7 × 1014 W/cm2 for the ellipticities ranging from 0 to 0.3. Only the CMDs for recollision excitation with subsequent ionization (RESI) are calculated and the contribution from recollision direct ionization is neglected. According to the QRS model, the CMD for RESI can be factorized as a product of the parallel momentum distribution (PMD) for the first released electron after recollision and the PMD for the second electron ionized from an excited state of the parent ion. The PMD for the first electron is obtained from the laser-free differential cross sections for electron impact excitation of Ar+ calculated using state-of-the-art many-electron R-matrix theory while that for the second electron is evaluated by solving the time-dependent Schrödinger equation. The results show that the CMDs for all the ellipticities considered here exhibit distinct anticorrelated back-to-back emission of the electrons along the major polarization direction, and the anticorrelation is more pronounced with increasing ellipticity. It is found that anticorrelation is attributed to the pattern of the PMD for the second electron ionized from the excited state that, in turn, is caused by the delayed recollision time with respect to the instant of the external field crossing. Our work shows that both the ionization potential of the excited parent ion and the laser intensity play important roles in the process.

Nonsequential double ionization of Ar in near-single-cycle laser pulses.

Using the improved quantitative rescattering (QRS) model, we simulate the correlated two-electron momentum distributions (CMD) for nonsequential double ionization (NSDI) of Ar by near-single-cycle laser pulses with a wavelength of 750 nm at an intensity of 2.8 × 1014 W/cm2. With the accurate cross sections obtained from fully quantum mechanical calculations for both electron impact excitation and electron impact ionization of Ar+, we unambiguously identify the contributions from recollision direct ionization (RDI) and recollision excitation with subsequent ionization (RESI). Our analysis reveals that RESI constitutes the main contribution to NSDI of Ar under the conditions considered here. The simulated results are directly compared with experimental measurements [Bergues et al., Nature Commun. 3, 813 (2012)] in which each NSDI event is tagged with the carrier-envelope phase (CEP). It is found that the overall pattern of both the CEP-resolved and the CEP-averaged CMDs measured in experiment are well reproduced by the QRS model, and the cross-shaped structure in the CEP-averaged CMD is attributed to the strong forward scattering of the recolliding electron as well as the depletion effect in tunneling ionization of the electron from an excited state of the parent ion.

Intensity dependence in nonsequential double ionization of helium.

Using the quantitative rescattering model, we simulate the correlated two-electron momentum distributions for nonsequential double ionization of helium by 800 nm laser pulses at intensities in the range of (2 - 15) × 1014 W/cm2. The experimentally observed V-shaped structure at high intensities [A. Rudenko et al., Phys. Rev. Lett. 99, 263003 (2007)] is attributed to the strong forward scattering in laser-induced recollision excitation and the asymmetric momentum distribution of electrons that are tunneling-ionized from the excited states. The final-state electron repulsion also plays an important role in forming the V-shaped structure.

Unraveling nonadiabatic ionization and Coulomb potential effect in strong-field photoelectron holography.

Strong field photoelectron holography has been proposed as a means for interrogating the spatial and temporal information of electrons and ions in a dynamic system. After ionization, part of the electron wave packet may directly go to the detector (the reference wave), while another part may be driven back and scatters off the ion(the signal wave). The interference hologram of the two waves may be used to extract target information embedded in the collision process. Unlike conventional optical holography, however, propagation of the electron wave packet is affected by the Coulomb potential as well as by the laser field. In addition, electrons are emitted over the whole laser pulse duration, thus multiple interferences may occur. In this work, we used a generalized quantum-trajectory Monte Carlo method to investigate the effect of Coulomb potential and the nonadiabatic subcycle ionization on the photoelectron hologram. We showed that photoelectron hologram can be well described only when the effect of nonadiabatic ionization is accounted for, and Coulomb potential can be neglected only in the tunnel ionization regime. Our results help paving the way for establishing photoelectron holography for probing spatial and dynamic properties of atoms and molecules.

Molecular photoelectron holography with circularly polarized laser pulses.

We investigate the photoelectron momentum distribution of molecular-ion H2+driven by ultrashort intense circularly polarized laser pulses. Both numerical solutions of the time-dependent Schrödinger equation (TDSE) and a quasiclassical model indicate that the photoelectron holography (PH) with circularly polarized pulses can occur in molecule. It is demonstrated that the interference between the direct electron wave and rescattered electron wave from one core to its neighboring core induces the PH. Moreover, the results of the TDSE predict that there is a tilt angle between the interference pattern of the PH and the direction perpendicular to the molecular axis. Furthermore, the tilt angle is sensitively dependent on the wavelength of the driven circularly polarized pulse, which is confirmed by the quasiclassical calculations. The PH induced by circularly polarized laser pulses provides a tool to resolve the electron dynamics and explore the spatial information of molecular structures.

Phase-dependent above-barrier ionization of excited-state electrons.

The carrier-envelope phase (CEP)-dependent above-barrier ionization (ABI) has been investigated in order to probe the bound-state electron dynamics. It is found that when the system is initially prepared in the excited state, the ionization yield asymmetry between left and right sides can occur both in low-energy and high-energy parts of the photoelectron spectra. Moreover, in electron momentum map, a new interference effect along the direction perpendicular to the laser polarization is found. We show that this interference is related to the competition among different excited states. The interference effect is dependent on CEPs of few-cycle probe pulses, which can be used to trace the superposition information and control the electron wave packet of low excited states.

Laser-induced electron diffraction for probing rare gas atoms.

Recently, using midinfrared laser-induced electron diffraction (LIED), snapshots of a vibrating diatomic molecule on a femtosecond time scale have been captured [C.I. Blaga et al., Nature (London) 483, 194 (2012)]. In this Letter, a comprehensive treatment for the atomic LIED response is reported, a critical step in generalizing this imaging method. Electron-ion differential cross sections (DCSs) of rare gas atoms are extracted from measured angular-resolved, high-energy electron momentum distributions generated by intense midinfrared lasers. Following strong-field ionization, the high-energy electrons result from elastic rescattering of a field-driven wave packet with the parent ion. For recollision energies ≥100 eV, the measured DCSs are indistinguishable for the neutral atoms and ions, illustrating the close collision nature of this interaction. The extracted DCSs are found to be independent of laser parameters, in agreement with theory. This study establishes the key ingredients for applying LIED to femtosecond molecular imaging.

Quantum theory of recollisional (e, 2e) process in strong field nonsequential double ionization of helium.

Based on the full quantal recollision model and field-free electron impact ionization theory, we calculate the correlated momentum spectra of the two outgoing electrons in strong field nonsequential double ionization (NSDI) of helium to compare with recent experiments. By analyzing the relative strength of binary versus recoil collisions exhibited in the photoelectron spectra, we confirm that the observed fingerlike structure in the experiment is a consequence of the Coulomb interaction between the two emitted electrons. Our result supports the recollision mechanism of strong field NSDI at the most fundamental level.

Accurate retrieval of target structures and laser parameters of few-cycle pulses from photoelectron momentum spectra.

We illustrate a new method of analyzing three-dimensional momentum images of high-energy photoelectrons generated by intense phase-stabilized few-cycle laser pulses. Using photoelectron momentum spectra that were obtained by velocity-map imaging of above-threshold ionization of xenon and argon targets, we show that the absolute carrier-envelope phase, the laser peak intensity, and pulse duration can be accurately determined simultaneously (with an error of a few percent). We also show that the target structure, in the form of electron-target ion elastic differential cross sections, can be retrieved over a range of energies. The latter offers the promise of using laser-generated electron spectra for probing dynamic changes in molecular targets with subfemtosecond resolution.

Accurate retrieval of structural information from laser-induced photoelectron and high-order harmonic spectra by few-cycle laser pulses.

By analyzing accurate theoretical results from solving the time-dependent Schrödinger equation of atoms in few-cycle laser pulses, we established the general conclusion that laser-generated high-energy electron momentum spectra and high-order harmonic spectra can be used to extract accurate differential elastic scattering and photo-recombination cross sections of the target ion with free electrons, respectively. Since both electron scattering and photoionization (the inverse of photo-recombination) are the conventional means for interrogating the structure of atoms and molecules, this result implies that existing few-cycle infrared lasers can be implemented for ultrafast imaging of transient molecules with temporal resolution of a few femtoseconds.

Unexpected higher-order effects in charged particle impact ionization at high energies.

Most of the experimental and theoretical studies of electron-impact ionization of atoms, referred to as (e, 2e), have concentrated on the scattering plane. The assumption has been that all the important physical effects will be observable in the scattering plane. However, very recently it has been shown that, for C6+-helium ionization, experiment and theory are in nice agreement in the scattering plane and in very bad agreement out of the scattering plane. This lack of agreement between experiment and theory has been explained in terms of higher-order scattering effects between the projectile and target ion. We have examined electron-impact ionization of magnesium and have observed similar higher-order effects. The results of the electron-impact ionization of magnesium indicate the possible deficiencies in the calculation of fully differential cross sections in previous heavy particle ionization work.