Attosecond angular streaking and tunnelling time in atomic hydrogen.

The tunnelling of a particle through a potential barrier is a key feature of quantum mechanics that goes to the core of wave-particle duality. The phenomenon has no counterpart in classical physics, and there are no well constructed dynamical observables that could be used to determine 'tunnelling times'. The resulting debate1-5 about whether a tunnelling quantum particle spends a finite and measurable time under a potential barrier was reignited in recent years by the advent of ultrafast lasers and attosecond metrology6. Particularly important is the attosecond angular streaking ('attoclock') technique7, which can time the release of electrons in strong-field ionization with a precision of a few attoseconds. Initial measurements7-10 confirmed the prevailing view that tunnelling is instantaneous, but later studies11,12 involving multi-electron atoms-which cannot be accurately modelled, complicating interpretation of the ionization dynamics-claimed evidence for finite tunnelling times. By contrast, the simplicity of the hydrogen atom enables precise experimental measurements and calculations13-15 and makes it a convenient benchmark. Here we report attoclock and momentum-space imaging16 experiments on atomic hydrogen and compare these results with accurate simulations based on the three-dimensional time-dependent Schrödinger equation and our experimental laser pulse parameters. We find excellent agreement between measured and simulated data, confirming the conclusions of an earlier theoretical study17 of the attoclock technique in atomic hydrogen that presented a compelling argument for instantaneous tunnelling. In addition, we identify the Coulomb potential as the sole cause of the measured angle between the directions of electron emission and peak electric field: this angle had been attributed11,12 to finite tunnelling times. We put an upper limit of 1.8 attoseconds on any tunnelling delay, in agreement with recent theoretical findings18 and ruling out the interpretation of all commonly used 'tunnelling times'19 as 'time spent by an electron under the potential barrier'20.

Author Correction: Attosecond angular streaking and tunnelling time in atomic hydrogen.

In this Letter, the statement 'I.I. and A.B. performed computations at the NCI Australia' was missing from the Acknowledgements section. This has been corrected online.

Strong-Field Ionization Phenomena Revealed by Quantum Trajectories.

We investigate the photoionization dynamics of atoms subjected to intense, ultrashort laser pulses through the use of quantum trajectories. This method provides a unique and consistent framework for examining electron dynamics within a time-dependent potential barrier. Our findings demonstrate that quantum trajectories offer additional insights into several key aspects of strong-field ionization, including the transition between ionization regimes, nonadiabatic effects under the barrier, the impact of the shape of the electronic potential, and the efficiency of over-the-barrier ionization.

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.

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.

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.

Electron collisions with atoms, ions, molecules, and surfaces: Fundamental science empowering advances in technology.

Electron collisions with atoms, ions, molecules, and surfaces are critically important to the understanding and modeling of low-temperature plasmas (LTPs), and so in the development of technologies based on LTPs. Recent progress in obtaining experimental benchmark data and the development of highly sophisticated computational methods is highlighted. With the cesium-based diode-pumped alkali laser and remote plasma etching of Si3N4 as examples, we demonstrate how accurate and comprehensive datasets for electron collisions enable complex modeling of plasma-using technologies that empower our high-technology-based society.

A few selected contributions to electron and photon collisions with H2 and H 2 + .

We discuss a number of aspects regarding the physics of H 2 + and H2. This includes low-energy electron scattering processes and the interaction of both weak (perturbative) and strong (ultrafast/intense) electromagnetic radiation with those systems.

Electron-impact ionization of neon at low projectile energy: an internormalized experiment and theory for a complex target.

As a fundamental test for state-of-the-art theoretical approaches, we have studied the single ionization (2p) of neon at a projectile energy of 100 eV. The experimental data were acquired using an advanced reaction microscope that benefits from high efficiency and a large solid-angle acceptance of almost 4π. We put special emphasis on the ability to measure internormalized triple-differential cross sections over a large part of the phase space. The data are compared to predictions from a second-order hybrid distorted-wave plus R-matrix model and a fully nonperturbative B-spline R-matrix (BSR) with pseudostates approach. For a target of this complexity and the low-energy regime, unprecedented agreement between experiment and the BSR model is found. This represents a significant step forward in the investigation of complex targets.

Nonperturbative treatment of ionization with excitation of helium by electron impact.

We present cross sections for electron-impact ionization and simultaneous ionization plus excitation of helium by electron impact. The results are obtained from a fully nonperturbative close-coupling formalism using our B-spline R-matrix approach. A large number of pseudostates in the expansion of the wave function represent the coupling to the ionization continuum. We obtain excellent agreement with the directly measured experimental cross section ratios (Bellm et al., Phys. Rev. A 75, 042704 (2007)) for ionization leaving the residual He⁺ ion in either the 1s ground state or the n = 2 (2s + 2p) excited states.

Complete breakup of the helium atom by proton and antiproton impact.

We present a fully ab initio, nonperturbative, time-dependent approach to describe single and double ionization of helium by proton and antiproton impact. The problem is discretized by a flexible finite-element discrete-variable representation on the radial grid. Good agreement with the most recent experimental data for absolute angle-integrated cross sections is obtained for projectile energies between 3 keV and 6 MeV. Also, angle-differential cross sections for two-electron ejection are predicted for a proton impact energy of 6 MeV. The time evaluation of the ionization process is portrayed by displaying the electron density as a function of the projectile location.

Coherent control schemes for the photoionization of neon and helium in the Extreme Ultraviolet spectral region.

The seeded Free-Electron Laser (FEL) FERMI is the first source of short-wavelength light possessing the full coherence of optical lasers, together with the extreme power available from FELs. FERMI provides longitudinally coherent radiation in the Extreme Ultraviolet and soft x-ray spectral regions, and therefore opens up wide new fields of investigation in physics. We first propose experiments exploiting this property to provide coherent control of the photoionization of neon and helium, carry out numerical calculations to find optimum experimental parameters, and then describe how these experiments may be realized. The approach uses bichromatic illumination of a target and measurement of the products of the interaction, analogous to previous Brumer-Shapiro-type experiments in the optical spectral range. We describe operational schemes for the FERMI FEL, and simulate the conditions necessary to produce light at the fundamental and second or third harmonic frequencies, and to control the phase with respect to the fundamental. We conclude that a quantitative description of the phenomena is extremely challenging for present state-of-the-art theoretical and computational methods, and further development is necessary. Furthermore, the intensity available may already be excessive for the experiments proposed on helium. Perspectives for further development are discussed.