K. J. Schafer

Theoretical aspects of intense field harmonic generation

The authors present theoretical studies of high-order harmonic generation in a rare-gas medium. The experimental results obtained at Saclay with a 1064 nm Nd-YAG laser in the 1013 W cm-2 intensity range are summarized. The harmonic emission strengths, first decrease rather steeply for the first orders, then form a long plateau up to the 21st harmonic in xenon, or up to the 33rd harmonic in argon, before decreasing again rather abruptly. The theoretical description of these experiments consists first in the calculation of the photoemission spectra emitted by a single atom. The spectra are obtained by numerically integrating a time dependent Schrodinger equation for the laser-excited rare-gas atom. Second, one must account for collective effects in the medium, described by Maxwells equations. A theoretical framework for describing the generation and propagation of harmonics in strong laser fields is developed. An numerical solution of the propagation equations for the harmonic fields in xenon at 1064 nm provides results which agree well with experimental data.

Time-Resolved Holography with Photoelectrons

The intefererence pattern produced by photoelectrons provides holographic snapshots of the photoionization process. Ionization is the dominant response of atoms and molecules to intense laser fields and is at the basis of several important techniques, such as the generation of attosecond pulses that allow the measurement of electron motion in real time. We present experiments in which metastable xenon atoms were ionized with intense 7-micrometer laser pulses from a free-electron laser. Holographic structures were observed that record underlying electron dynamics on a sublaser-cycle time scale, enabling photoelectron spectroscopy with a time resolution of almost two orders of magnitude higher than the duration of the ionizing pulse.

Attosecond Electron Spectroscopy Using a Novel Interferometric Pump-Probe Technique

We present an interferometric pump-probe technique for the characterization of attosecond electron wave packets (WPs) that uses a free WP as a reference to measure a bound WP. We demonstrate our method by exciting helium atoms using an attosecond pulse (AP) with a bandwidth centered near the ionization threshold, thus creating both a bound and a free WP simultaneously. After a variable delay, the bound WP is ionized by a few-cycle infrared laser precisely synchronized to the original AP. By measuring the delay-dependent photoelectron spectrum we obtain an interferogram that contains both quantum beats as well as multipath interference. Analysis of the interferogram allows us to determine the bound WP components with a spectral resolution much better than the inverse of the AP duration.

Attosecond control of ionization by wave-packet interference

Attosecond pulses [1, 2] can be used to initiate and control electron dynamics on a sub-femtosecond time scale. The first step in this process occurs when an atom absorbs an ultraviolet photon leading to the formation of an attosecond electron wave packet (EWP). Until now, attosecond pulses have been used to create free EWPs in the continuum, where they quickly disperse [3, 4, 5, 6, 7]. In this paper we use a train of attosecond pulses, synchronized to an infrared (IR) laser field, to create a series of EWPs that are below the ionization threshold in helium. We show that the ionization probability then becomes a function of the delay between the IR and attosecond fields. Calculations that reproduce the experimental results demonstrate that this ionization control results from interference between transiently bound EWPs created by different pulses in the train. In this way, we are able to observe, for the first time, wave packet interference in a strongly driven atomic system.

Phase Measurement of Resonant Two-Photon Ionization in Helium

We study resonant two-color two-photon ionization of helium via the 1s3p (1)P(1) state. The first color is the 15th harmonic of a tunable Ti:sapphire laser, while the second color is the fundamental laser radiation. Our method uses phase-locked high-order harmonics to determine the phase of the two-photon process by interferometry. The measurement of the two-photon ionization phase variation as a function of detuning from the resonance and intensity of the dressing field allows us to determine the intensity dependence of the transition energy.

Frequency chirp of harmonic and attosecond pulses

We study the phase of the atomic polarization in the process of high-order harmonic generation. Its dependence on the laser intensity and the harmonic order induce a frequency variation in time (chirp) respectively of the harmonic pulses and attosecond pulses. We review the recent experimental results on the temporal characterization of the harmonic emission and show that measurements performed using very different techniques (like XFROG and RABITT), probing the phase in different parameter spaces, can be connected through the mixed phase derivatives, demonstrating the common underlying physics.

Attosecond control of electron-ion recollision in high harmonic generation

We show that high harmonic generation driven by an intense near-infrared (IR) laser can be temporally controlled when an attosecond pulse train (APT) is used to ionize the generation medium, thereby replacing tunnel ionization as the first step in the well-known three-step model. New harmonics are formed when the ionization occurs at a well-defined time within the optical cycle of the IR field. The use of APT-created electron wave packets affords new avenues for the study and application of harmonic generation. In the present experiment, this makes it possible to study harmonic generation at IR intensities where tunnel ionization does not give a measurable signal.

Control of high-order harmonic emission using attosecond pulse trains

We show that attosecond pulse trains are a natural tool to control strong field processes such as high-order harmonic generation. Coherently combining an attosecond pulse train with an IR driving field, we predict and experimentally confirm enhancement and spectral narrowing of the harmonic yield at photon energies around 90 eV. The use of an attosecond pulse train to seed the harmonic generation process replaces tunneling ionization with a single-photon ionization step, therefore permitting the manipulation of the time–frequency properties of high-order harmonic generation already at the single-atom level.

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.

Intensity dependence of laser-assisted attosecond photoionization spectra

We study experimentally the influence of the intensity of the infrared (IR) probe field on attosecond pulse train (APT) phase measurements performed with the RABITT method (Reconstruction of Attosecond Beating by Interference in Two-Photon Transitions). We find that if a strong IR field is applied, the attosecond pulses will appear to have lower-than-actual chirp rates. We also observe the onset of the streaking regime in the breakdown of the weak-field RABITT conditions. We perform a Fourier-analysis of harmonic and sideband continuum states and show that the mutual phase relation of the harmonics can be extracted from higher Fourier components.