Marc J. J. Vrakking

Bio: Marc J. J. Vrakking is an academic researcher from Fundamental Research on Matter Institute for Atomic and Molecular Physics. The author has contributed to research in topics: Attosecond & Ionization. The author has an hindex of 45, co-authored 267 publications receiving 8129 citations. Previous affiliations of Marc J. J. Vrakking include University of Rostock & VU University Amsterdam.

Attosecond real-time observation of electron tunnelling in atoms

Abstract: Atoms exposed to intense light lose one or more electrons and become ions. In strong fields, the process is predicted to occur via tunnelling through the binding potential that is suppressed by the light field near the peaks of its oscillations. Here we report the real-time observation of this most elementary step in strong-field interactions: light-induced electron tunnelling. The process is found to deplete atomic bound states in sharp steps lasting several hundred attoseconds. This suggests a new technique, attosecond tunnelling, for probing short-lived, transient states of atoms or molecules with high temporal resolution. The utility of attosecond tunnelling is demonstrated by capturing multi-electron excitation (shake-up) and relaxation (cascaded Auger decay) processes with subfemtosecond resolution.

Attosecond molecular dynamics: fact or fiction?

Abstract: The emerging application of attosecond techniques to molecular systems allows the role of electronic coherence in the control of chemical reactions to be investigated. Prompt ionization of molecules by an attosecond pulse may induce charge migration across a molecular structure on attosecond to few-femtosecond timescales, thereby possibly determining the subsequent relaxation pathways that a molecule may take. We discuss how proposals for this 'charge-directed reactivity' fit within the current understanding of quantum control and review the current state of the art of attosecond molecular science. Specifically, we review the role of electronic coherence and coupling of the electronic and nuclear degrees of freedom in high-harmonic spectroscopy and in the first attosecond pump–probe experiments on molecular systems. Attosecond science allows the role of electronic coherence in the control of chemical reactions in molecular systems to be investigated. This article reviews recent activities in attosecond molecular science and identifies some promising directions for further development.

Attosecond Electron Dynamics

Abstract: We describe the recent emergence of attosecond science, assessing the present state of the art and discussing several recent examples where attosecond electron dynamics has been studied in atomic and molecular systems. After introducing the generation and characterization of attosecond laser pulses, we describe the use of isolated attosecond pulses in a pump-probe experiment revealing the subcycle time dependence of a multiphoton ionization process and an experiment using the interference from a train of attosecond pulses to extract amplitude and phase information for electronic wave functions. We furthermore discuss experiments where ultrashort laser pulses with a reproducible waveform control electron dynamics in the D2+ molecular ion on attosecond timescales. Attosecond science is coming of age and presently is reaching a level of maturity and sophistication that allows detailed investigations of the role of multielectron dynamics in physics and chemistry.

An iterative procedure for the inversion of two-dimensional ion/photoelectron imaging experiments

Abstract: We present an iterative method for the extraction of velocity and angular distributions from two-dimensional (2D) ion/photoelectron imaging experiments. This method is based on the close relationship which exists between the initial 3D angular and velocity distribution and the measured 2D angular and radial distributions, and gives significantly better results than other inversion procedures which are commonly used today. Particularly, the procedure gets rid of the center-line noise which is one of the main artifacts in many current ion/photoelectron imaging experiments.

Roadmap of ultrafast x-ray atomic and molecular physics

Abstract: X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (1020 W cm-2) of x-rays at wavelengths down to ∼1 Angstrom, and HHG provides unprecedented time resolution (∼50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of ∼280 eV (44 Angstroms) and the bond length in methane of ∼1 Angstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Angstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Angstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.

Theory of Bose-Einstein condensation in trapped gases

Abstract: The phenomenon of Bose-Einstein condensation of dilute gases in traps is reviewed from a theoretical perspective. Mean-field theory provides a framework to understand the main features of the condensation and the role of interactions between particles. Various properties of these systems are discussed, including the density profiles and the energy of the ground-state configurations, the collective oscillations and the dynamics of the expansion, the condensate fraction and the thermodynamic functions. The thermodynamic limit exhibits a scaling behavior in the relevant length and energy scales. Despite the dilute nature of the gases, interactions profoundly modify the static as well as the dynamic properties of the system; the predictions of mean-field theory are in excellent agreement with available experimental results. Effects of superfluidity including the existence of quantized vortices and the reduction of the moment of inertia are discussed, as well as the consequences of coherence such as the Josephson effect and interference phenomena. The review also assesses the accuracy and limitations of the mean-field approach.

Fourier-transform method of fringe-pattern analysis for computer-based topography and interferometry

Abstract: A fast-Fourier-transform method of topography and interferometry is proposed. By computer processing of a noncontour type of fringe pattern, automatic discrimination is achieved between elevation and depression of the object or wave-front form, which has not been possible by the fringe-contour-generation techniques. The method has advantages over moire topography and conventional fringe-contour interferometry in both accuracy and sensitivity. Unlike fringe-scanning techniques, the method is easy to apply because it uses no moving components.

Progress and Perspectives of Electrochemical CO2 Reduction on Copper in Aqueous Electrolyte

Abstract: To date, copper is the only heterogeneous catalyst that has shown a propensity to produce valuable hydrocarbons and alcohols, such as ethylene and ethanol, from electrochemical CO2 reduction (CO2R). There are variety of factors that impact CO2R activity and selectivity, including the catalyst surface structure, morphology, composition, the choice of electrolyte ions and pH, and the electrochemical cell design. Many of these factors are often intertwined, which can complicate catalyst discovery and design efforts. Here we take a broad and historical view of these different aspects and their complex interplay in CO2R catalysis on Cu, with the purpose of providing new insights, critical evaluations, and guidance to the field with regard to research directions and best practices. First, we describe the various experimental probes and complementary theoretical methods that have been used to discern the mechanisms by which products are formed, and next we present our current understanding of the complex reaction networks for CO2R on Cu. We then analyze two key methods that have been used in attempts to alter the activity and selectivity of Cu: nanostructuring and the formation of bimetallic electrodes. Finally, we offer some perspectives on the future outlook for electrochemical CO2R.

Ab initio calculation of vibrational absorption and circular dichroism spectra using density functional force fields

Abstract: : The unpolarized absorption and circular dichroism spectra of the fundamental vibrational transitions of the chiral molecule, 4-methyl-2-oxetanone, are calculated ab initio. Harmonic force fields are obtained using Density Functional Theory (DFT), MP2, and SCF methodologies and a 5S4P2D/3S2P (TZ2P) basis set. DFT calculations use the Local Spin Density Approximation (LSDA), BLYP, and Becke3LYP (B3LYP) density functionals. Mid-IR spectra predicted using LSDA, BLYP, and B3LYP force fields are of significantly different quality, the B3LYP force field yielding spectra in clearly superior, and overall excellent, agreement with experiment. The MP2 force field yields spectra in slightly worse agreement with experiment than the B3LYP force field. The SCF force field yields spectra in poor agreement with experiment.The basis set dependence of B3LYP force fields is also explored: the 6-31G* and TZ2P basis sets give very similar results while the 3-21G basis set yields spectra in substantially worse agreements with experiment. jg

Attosecond Physics

Abstract: Summary form only given. Fundamental processes in atoms, molecules, as well as condensed matter are triggered or mediated by the motion of electrons inside or between atoms. Electronic dynamics on atomic length scales tends to unfold within tens to thousands of attoseconds (1 attosecond [as] = 10-18 s). Recent breakthroughs in laser science are now opening the door to watching and controlling these hitherto inaccessible microscopic dynamics. The key to accessing the attosecond time domain is the control of the electric field of (visible) light, which varies its strength and direction within less than a femtosecond (1 femtosecond = 1000 attoseconds). Atoms exposed to a few oscillations cycles of intense laser light are able to emit a single extreme ultraviolet (XUV) burst lasting less than one femtosecond. Full control of the evolution of the electromagnetic field in laser pulses comprising a few wave cycles have recently allowed the reproducible generation and measurement of isolated sub-femtosecond XUV pulses, demonstrating the control of microscopic processes (electron motion and photon emission) on an attosecond time scale. These tools have enabled us to visualize the oscillating electric field of visible light with an attosecond "oscilloscope", to control single-electron and probe multi-electron dynamics in atoms, molecules and solids. Recent experiments hold promise for the development of an attosecond X-ray source, which may pave the way towards 4D electron imaging with sub-atomic resolution in space and time.