Showing papers by "Marc J. J. Vrakking published in 2012"

The Multielectron Ionization Dynamics Underlying Attosecond Strong-Field Spectroscopies

Abstract: Subcycle strong-field ionization (SFI) underlies many emerging spectroscopic probes of atomic or molecular attosecond electronic dynamics. Extending methods such as attosecond high harmonic generation spectroscopy to complex polyatomic molecules requires an understanding of multielectronic excitations, already hinted at by theoretical modeling of experiments on atoms, diatomics, and triatomics. Here, we present a direct method which, independent of theory, experimentally probes the participation of multiple electronic continua in the SFI dynamics of polyatomic molecules. We use saturated (n-butane) and unsaturated (1,3-butadiene) linear hydrocarbons to show how subcycle SFI of polyatomics can be directly resolved into its distinct electronic-continuum channels by above-threshold ionization photoelectron spectroscopy. Our approach makes use of photoelectron-photofragment coincidences, suiting broad classes of polyatomic molecules.

Direct Visualization of Laser-Driven Electron Multiple Scattering and Tunneling Distance in Strong-Field Ionization

Abstract: Using a simple model of strong-field ionization of atoms that generalizes the well-known 3-step model from 1D to 3D, we show that the experimental photoelectron angular distributions resulting from laser ionization of xenon and argon display prominent structures that correspond to electrons that pass by their parent ion more than once before strongly scattering. The shape of these structures can be associated with the specific number of times the electron is driven past its parent ion in the laser field before scattering. Furthermore, a careful analysis of the cutoff energy of the structures allows us to experimentally measure the distance between the electron and ion at the moment of tunnel ionization. This work provides new physical insight into how atoms ionize in strong laser fields and has implications for further efforts to extract atomic and molecular dynamics from strong-field physics.

Subcycle controlled charge-directed reactivity with few-cycle midinfrared pulses.

Abstract: The steering of electron motion in molecules is accessible with waveform-controlled few-cycle laser light and may control the outcome of light-induced chemical reactions. An optical cycle of light, however, is much shorter than the duration of the fastest dissociation reactions, severely limiting the degree of control that can be achieved. To overcome this limitation, we extended the control metrology to the midinfrared studying the prototypical dissociative ionization of D(2) at 2.1 μm. Pronounced subcycle control of the directional D(+) ion emission from the fragmentation of D(2)(+) is observed, demonstrating unprecedented charge-directed reactivity. Two reaction pathways, showing directional ion emission, could be observed and controlled simultaneously for the first time. Quantum-dynamical calculations elucidate the dissociation channels, their observed phase relation, and the control mechanisms.

Scaling laws for photoelectron holography in the midinfrared wavelength regime

Abstract: Midinfrared strong-field laser ionization offers the promise of measuring holograms of atoms and molecules, which contain both spatial and temporal information of the ion and the photoelectron with subfemtosecond temporal and angstrom spatial resolution. We report on the scaling of photoelectron holographic interference patterns with the laser pulse duration, wavelength, and intensity. High-resolution holograms for the ionization of metastable xenon atoms by 7-16 μm light from the FELICE free electron laser are presented and compared to semiclassical calculations that provide analytical insight.

X-Ray photonics: X-rays inspire electron movies

Abstract: The advent of high-energy, short-pulse X-ray sources based on free-electron lasers, laser plasmas and high-harmonic generation is now making it possible to probe the dynamics of electrons within molecules.

Photoelectron kinetic and angular distributions for the ionization of aligned molecules using a HHG source

Abstract: We present an experimental and theoretical investigation of the angular distributions of electrons ejected in aligned molecules by extreme ultra-violet ionization using a high harmonic generation (HHG) source. Impulsive alignment in O2, N2 and CO molecules was achieved using a near-IR laser pulse and the photoelectron angular distribution after ionization by a fs harmonic comb composed of harmonic H11 to H29 (17.5–46 eV) was recorded at the maximum of both alignment and anti-alignment. The experiment reveals signatures that are specific for the electronic orbitals that are ionized as well as the onset of the influence of the molecular structure and is well reproduced by theoretical calculations based on the multichannel Schwinger configuration interaction method.

Attosecond Time-Resolved Electron Dynamics in the Hydrogen Molecule

Abstract: Recent advances in the generation and characterization of extreme-ultraviolet pulses, generated either by intense femtosecond lasers or by free electron lasers, are pushing the frontier of time-resolved investigations down to the attosecond domain, the relevant timescale for electron motion. The quantum nature of the intertwined electronic and nuclear motion requires theoretical models going beyond the Born-Oppenheimer approximation and taking into account electron correlation, representing a challenge for the computational power available nowadays. Understanding how the electron dynamics inside molecules can influence chemical reactions presents important implications in several fields and allows for the development of new technologies. In this paper, we report on experimental and theoretical results of an investigation in H2/D2, where for the first time control of molecular dynamics with attosecond resolution was achieved. The data represent the first evidence of the control of the electron motion in a molecule undergoing a chemical reaction on the subfemtosecond scale.

Trajectory-Based Coulomb-Corrected Strong Field Approximation

Abstract: The strong field approximation (SFA) is one of the most successful theoretical approaches to tackle the problem of atomic or molecular ionization in intense laser fields. In the semi-classical limit, the SFA possesses an appealing interpretation in terms of interfering quantum trajectories, which mathematically originate from the saddle point approximation to the SFA transition matrix element. The trajectories not only allow to interpret particular features in photoelectron spectra in an intuitive way in terms of possible electron pathways typical for a quantum mechanical “multi-slit experiment” but also serve as a starting point for adopting Coulomb corrections.

Time-Resolved Photoelectron Diffraction of Laser-Aligned Molecules

Abstract: Static and time-resolved photoelectron diffraction of laser-aligned polyatomic molecules photoionized by Free-Electron Laser pulses is presented. The results are a proof-of-principle for imaging dynamic structural changes in molecules with femtosecond temporal and Angstrom spatial resolution.

Competition of sequential and direct paths in two-photon ionization of He

Abstract: We study the photoelectron angular distribution (PAD) from the two-photon ionization (TPI) of He by femtosecond EUV pulses. The calculation with the time-dependent Schrodinger equation (TDSE) and the measurement at the SPring-8 EUV-FEL show reasonable agreement. The extracted relative phase δ between the s and d wave packets are distinct from that between the corresponding eigenstates, due to the competition between sequential and direct ionization paths. When the pulse is resonant with an excited level, the sequential and direct TPI compete with each other, and δ and the PAD depend on the pulse width. On the other hand, when the Ry-dberg manifold is coherently excited, δ does not vary with the pulse width.