Your search for "anne l'huillier" returned 16 results

We study phase-matching conditions for high-order harmonic generation as well as high-order sum- and difference-frequency mixing processes in strong laser fields, using a graphical approach described in Balcou et al (1997 Phys. Rev. A 55 3204-10). This method is based on the analysis of the different quantum paths that contribute, with different phase properties, to the single-atom response. We propose a simple numerical method to disentangle the quantum paths contributing to the generation process. We present graphical maps of the phase matching around the laser focus, which allow one to predict the geometries that optimize the conversion efficiency of the process considered. The method is applied to the study of sum- and difference-frequency mixing processes. The qualitative predictions of the graphical phase-matching approach are confirmed by numerical propagation calculations.

Ultrafast processes in matter can be captured and even controlled by using sequences of few-cycle optical pulses, which need to be well characterized, both in amplitude and phase. The same degree of control has not yet been achieved for few-cycle extreme ultraviolet pulses generated by high-order harmonic generation (HHG) in gases, with duration in the attosecond range. Here, we show that by varying the spectral phase and carrier-envelope phase (CEP) of a high-repetition rate laser, using dispersion in glass, we achieve a high degree of control of the relative phase and CEP between consecutive attosecond pulses. The experimental results are supported by a detailed theoretical analysis based upon the semi-classical three-step model for HHG.

We present efficient high-order harmonic generation (HHG) based on a high-repetition rate, few-cycle, near infrared (NIR), carrier-envelope phase stable, optical parametric chirped pulse amplifier (OPCPA), emitting 6 fs pulses with 9 μJ pulse energy. In krypton, we reach conversion efficiencies from the NIR to the extreme ultraviolet (XUV) radiation pulse energy on the order of ∼10⁻⁶ with less than 3 μJ driving pulse energy. This is achieved by optimizing the OPCPA for a spatially and temporally clean pulse and by a specially designed high-pressure gas target. In the future, the high efficiency of the HHG source will be beneficial for high-repetition rate two-colour (NIR-XUV) pump-probe experiments, where the available pulse energy from the laser has to be distributed economically between pump and probe pulses.

This review presents the technological infrastructure that will be available at the Extreme Light Infrastructure Attosecond Light Pulse Source (ELI-ALPS) international facility. ELI-ALPS will offer to the international scientific community ultrashort pulses in the femtosecond and attosecond domain for time-resolved investigations with unprecedented levels of high quality characteristics. The laser sources and the attosecond beamlines available at the facility will make attosecond technology accessible for scientists lacking access to these novel tools. Time-resolved investigation of systems of increasing complexity is envisaged using the end stations that will be provided at the facility.

Ionisation with ultrashort pulses in the extreme ultraviolet (XUV) regime can be used to prepare an ion in a superposition of spin–orbit substates. In this work, we study the coherence properties of such a superposition, created by ionising xenon atoms using two phase-locked XUV pulses at different frequencies. In general, if the duration of the driving pulse exceeds the quantum beat period, dephasing will occur. If however, the frequency difference of the two pulses matches the spin–orbit splitting, the coherence can be efficiently increased and dephasing does not occur.

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 Ångstrom, 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 Ångstroms) and the bond length in methane of ∼1 Ångstrom. 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 Ångstroms). 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 Ångstrom 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.

We study XUV generation with several-cycle laser pulses of intensity up to 10¹⁵ W cm⁻² using numerical solution of the 3D Schrödinger equation for a hydrogen atom. Ionization of the atom mainly takes place in a barrier-suppression regime for such driving intensities. We find that in this regime XUV yield stops growing with the laser intensity and then even essentially decreases. The calculated yield dependence on the laser intensity agrees well with predictions of our theory. The latter shows several factors that lead to the decrease of the XUV yield in the barrier-suppression regime. The calculated cut-off in the XUV spectrum is displaced to slightly lower energies than those predicted by the I_p + 3.17U_p law. The change in the cut-off can be due to the non-zero initial velocity of the electron detached under the barrier-suppression ionization. We find that essential population of both the free wave packet returning to the origin and the ground state at the instant of the return is required for effective XUV generation. Rapid ground state depopulation leads to shortening of the attopulse train generated by the two-cycle laser pulse when laser intensity increases. In particular, we find that the cut-off XUV generated under essential barrier-suppression with sine-like laser pulse provides an isolated attopulse, while two attopulses are generated for lower laser intensity.

This article addresses topics regarding time measurements performed on quantum systems. The motivation is linked to the advent of 'attophysics' which makes feasible to follow the motion of electrons in atoms and molecules, with time resolution at the attosecond (1 as = 10⁻¹⁸ s) level, i.e. at the natural scale for electronic processes in these systems. In this context, attosecond 'time-delays' have been recently measured in experiments on photoionization and the question arises if such advances could cast a new light on the still active discussion on the status of the time variable in quantum mechanics. One issue still debatable is how to decide whether one can define a quantum time operator with eigenvalues associated to measurable 'time-delays', or time is a parameter, as it is implicit in the Newtonian classical mechanics. One objective of this paper is to investigate if the recent attophysics-based measurements could shed light on this parameter–operator conundrum. To this end, we present here the main features of the theory background, followed by an analysis of the experimental schemes that have been used to evidence attosecond 'time-delays' in photoionization. Our conclusion is that these results reinforce the view that time is a parameter which cannot be defined without reference to classical mechanics.

Ultrashort, coherent light pulses in the extreme ultraviolet (XUV) wavelength region are excellent tools for a wide range of experiments. These XUV pulses are in particular used to characterize electron dynamics. Additionally, the high photon energy enables quantum control of short-lived transitions in atoms. These transitions are of interest for ultrafast quantum control as the bandwidth of the control pulses needs to be less than the transition frequency. Coherent XUV pulses would be even more useful if the tools to control and manipulate them existed. Presently, however, no modulators exist for these frequencies, which significantly reduces the number of possible ultrafast optics experiments and applications in the XUV regime. This Ph.D. tutorial addresses this problem and focuses on the control of XUV light in time and space. To enable control of XUV light we have developed a method for opto-optical modulation (OOM), which modulates the phase of XUV light emitted from a gas of atoms. The atoms are resonantly excited with a coherent XUV pulse generated through high order harmonic generation and emit light after the excitation pulse passed. By shifting the resonance frequencies through the AC Stark shift with a non-resonant infrared control pulse, the phase of the emitted light, and therefore its wavefront, is controlled. With OOM the direction of XUV light emitted from noble gases has been controlled, and the temporal dynamics of the emission studied. By varying the delay between the excitation and the control pulse, the time of redirection was controlled, which enabled high signal to noise study of the temporal dynamics of the emission. Furthermore, a proof-of-principle experiment with two control pulses was performed, resulting in a shaped XUV pulse with controlled duration. The technique of OOM presented in this article is still at a very early stage and in order to obtain complete control of the amplitude and phase of the XUV pulses further development is necessary. Such development would present new opportunities for ultrafast XUV quantum control.