M. J. J. Vrakking

Non-linear processes in the interaction of atoms and molecules with intense EUV and X-ray fields from SASE free electron lasers (FELs)

The advent of free electron laser (FEL) facilities capable of delivering high intensity pulses in the extreme-UV to X-ray spectral range has opened up a wide vista of opportunities to study and control light matter interactions in hitherto unexplored parameter regimes. In particular, current short wavelength FELs can uniquely drive non-linear processes mediated by inner shell electrons and in fields where the photon energy can be as high as 10 keV and so the corresponding optical period reaches below one attosecond. Combined with ultrafast optical lasers, or simply employing wavefront division, pump probe experiments can be performed with femtosecond time resolution. As single photon ionization of atoms and molecules is by now very well understood, they provide the ideal targets for early experiments by which not only FELs can be characterised and benchmarked but can also be the natural departure point in the hunt for non-linear behaviour of atomistic systems bathed in laser fields of ultrahigh photon energy. In this topical review we illustrate with specific examples the gamut of apposite experiments in atomic, molecular physics currently underway at the SCSS Test Accelerator (Japan), FLASH (Hamburg) and LCLS (Stanford).

Femtosecond x-ray photoelectron diffraction on gas-phase dibromobenzene molecules

We present time-resolved femtosecond photoelectron momentum images and angular distributions of dissociating, laser-aligned 1,4-dibromobenzene (C6H4Br2) molecules measured in a near-infrared pump, soft-x-ray probe experiment performed at an x-ray free-electron laser. The observed alignment dependence of the bromine 2p photoelectron angular distributions is compared to density functional theory calculations and interpreted in terms of photoelectron diffraction. While no clear time-dependent effects are observed in the angular distribution of the Br(2p) photoelectrons, other, low-energy electrons show a pronounced dependence on the time delay between the near-infrared laser and the x-ray pulse.

Coulomb explosion of diatomic molecules in intense XUV fields mapped by partial covariance

Single-shot time-of-flight spectra for Coulomb explosion of N2 and I2 molecules have been recorded at the Free Electron LASer in Hamburg (FLASH) and have been analysed using a partial covariance mapping technique. The partial covariance analysis unravels a detailed picture of all significant Coulomb explosion pathways, extending up to the N 4+ ‐N 5+ channel for nitrogen and up to the I 8+ ‐I 9+ channel for iodine. The observation of the latter channel is unexpected if only sequential ionization processes from the ground state ions are considered. The maximum kinetic energy release extracted from the covariance maps for each dissociation channel shows that Coulomb explosion of nitrogen molecules proceeds much faster than that of the iodine. The N2 ionization dynamics is modelled using classical trajectory simulations in good agreement with the outcome of the experiments. The results suggest that covariance mapping of the Coulomb explosion can be used to measure the intensity and pulse duration of free-electron lasers.

Electron angular distributions in near-threshold atomic ionization

We present angle- and energy-resolved measurements of photoelectrons produced in strong-field ionization of Xe using a tunable femtosecond laser. An occurrence of highly oscillatory patterns in the angular distribution at low photoelectron kinetic energy is observed that correlates with channel closing/opening over a wide range of laser parameters. The correlation is investigated both experimentally and by means of systematic analysis of numerical solutions of the time-dependent Schrodinger equation. Our experimental and numerical results are in quantitative agreement with the semi-classical model introduced by Arbo et al (2008 Phys. Rev. A 78 013406), which relates the oscillatory patterns to interference between photoelectrons produced during different cycles of the laser pulse in the course of non-resonant ionization of the atom. We observe that an increase of the laser intensity eventually leads to qualitative invariance of the pattern, defining a limit on the applicability of the semi-classical model.

Wavelength dependence of photoelectron spectra in above-threshold ionization

We present angle- and energy-resolved measurements of photoelectrons produced in strong-field ionization of Xe and Ar using a tunable femtosecond laser in the wavelength range between 600 and 800 nm. Systematic analysis of the experimental data that are quantitatively reproduced by numerical solutions of the time-dependent Schrodinger equation with integration over the laser focal volume demonstrates the dominance of resonance-enhanced ionization. Continuous variation of the laser wavelength allows the identification of a number of consecutive channel-switching effects with a reliable assignment of the intermediate Rydberg states involved. The appearance of the resonant sub-structure in the electron energy spectra is influenced by the presence of a non-resonant contribution. At relatively low laser intensity, a coherent addition of resonant and non-resonant ionization processes is observed. Due to the absence of an intensity dependence in the resonance-enhanced ionization, we observe the persistence of Freeman resonances at the transition to the tunnelling regime.

Photoelectron angular distributions for the two-photon sequential double ionization of xenon by ultrashort extreme ultraviolet free electron laser pulses

Xenon atoms are double-ionized by sequential two-photon absorption by ultrashort extreme ultraviolet free-electron laser pulses with a photon energy of 23.0 and 24.3 eV, produced by the SPring-8 Compact SASE Source test accelerator. The angular distributions of photoelectrons generated by two-photon double ionization are obtained using velocity map imaging. The results are reproduced reasonably well by the present theoretical calculations within the multi-configurational Dirac-Fock approach.

Photoelectron angular distributions for the two-photon ionization of helium by ultrashort extreme ultraviolet free-electron laser pulses

The two-photon ionization of helium atoms by ultrashort extreme-ultraviolet free-electron laser pulses, produced by the SPring-8 Compact SASE Source test accelerator, was investigated at photon energies of 20.3, 21.3, 23.0 and 24.3 eV. The angular distribution of photoelectrons generated by two-photon ionization is obtained using a velocity map imaging spectrometer. The phase-shift differences and amplitude ratios of the outgoing s and d continuum wave packets are extracted from the photoelectron angular distributions. The obtained values of the phase-shift differences are distinct from scattering phase-shift differences when the photon energy is tuned to a resonance with an excited level or Rydberg manifold. The difference stems from the co-presence of resonant and non-resonant path contributions in the two-photon ionization by femtosecond pulses. Since the relative contribution of both paths can be controlled in principle by the pulse shape, these results illustrate a new way to tailor the continuum wave packet.

Interference in the angular distribution of photoelectrons in superimposed XUV and optical laser fields

The angular distribution of photoelectrons ejected during the ionization of Ne atoms by extreme ultraviolet (XUV) free-electron laser radiation in the presence of an intense near infrared (NIR) dressing field was investigated experimentally and theoretically. A highly nonlinear process with absorption and emission of more than ten NIR photons results in the formation of numerous sidebands. The amplitude of the sidebands varies strongly with the emission angle and the angular distribution pattern reveals clear signatures of interferences between the different angular momenta for the outgoing electron in the multi-photon process. As a specific feature, the central photoelectron line is characterized at the highest NIR fields by an angular distribution, which is peaked perpendicularly to both the XUV and NIR polarization directions. Experimental results are reproduced by a theoretical model based on the strong field approximation.

Attosecond control of electron localization in one- and two-color dissociative ionization of H 2 and D 2

We present one-color (IR) and two-color (single attosecond XUV pulse + IR) experiments where the sub-cycle evolution of the electric field of light is used to control the dissociative ionization of hydrogen and deuterium molecules.

Mapping the dissociative ionization dynamics of molecular nitrogen with attosecond resolution

We wish to understand the processes underlying the ionization dynamics of N2 as experimentally induced and studied by recording the kinetic energy release (KER) in a XUV-pump/IR-probe setup. To this end a theoretical model was developed describing the ionization process using Dyson Orbitals and, subsequently, the dissociation process using a large set of diabatic potential energy surfaces (PES) on which to propagate. From said set of PES, a small subset is extracted allowing for the identification of one and two photon processes chiefly responsible for the experimentally observed features.