arXiv subjects

A. L'Huillier

Publications and source records attributed to A. L'Huillier.

At least 19 recordsLinked to original sources

arXiv2026

Photoelectron interferometry with spectrally shaped polychromatic infrared pulses

Laser-assisted photoelectron interferometry is a cornerstone of attosecond science, first used to characterize attosecond pulse trains and later to study photoionization dynamics. Extending this method to spectrally shaped polychromatic infrared probe fields enables encoding of information across multiple interferometric pathways within the photoelectron spectrum. Here, we experimentally demonstrate laser-assisted photoelectron interferometry using a spectrally shaped polychromatic infrared probe field composed of five distinct spectral components forming a Golomb ruler in the frequency domain. The measured interferograms exhibit multiple beating frequencies that agree with theoretical calculations, demonstrating the simultaneous encoding of multiple laser-assisted quantum beats in a single measurement. A quantitative analysis of the beating amplitudes shows that the strongly modulated temporal profile of the polychromatic probe introduces intensity- and delay-dependent distortions of the quantum beats that cannot be explained by second-order perturbation theory. These results establish the conditions required for the quantitative interpretation of polychromatic photoelectron interferometry and highlight the opportunities offered by spectro-temporal engineering of the probe field for future developments in attosecond science.

physics.atom-ph↗

arXiv2026

Parity-mixing interference in laser-assisted photoionization

Photoionization of atoms by high-order harmonics in the presence of a laser may lead to quantum interference from which information about the photoionization dynamics or the light fields can be extracted. Traditionally, this interference arises from two-photon transitions involving the absorption of consecutive harmonics combined with the absorption and stimulated emission of a laser photon. In this process, parity is conserved. Here, we investigate interference between one- and two-photon transitions in helium using high-order harmonics generated by a few-cycle laser and three-dimensional electron detection. In this case, parity is not conserved. We identify four parity-mixing interference pathways, involving two different harmonic fields or a single harmonic, together with absorption or emission of a probe photon.

physics.atom-ph↗

arXiv2026

Subcycle phase matching effects in short attosecond pulse trains

Attosecond pulses produced by High-order Harmonic Generation (HHG) in gases driven by intense laser fields have become a cornerstone technique for probing ultrafast electronic motion in matter. These applications require a good knowledge of the temporal and spectral properties of the emitted radiation. In this work, we generate a train of two to three attosecond pulses that we characterize using two-color laser-assisted photoionization. \textcolor{black}{An unexpected spectral behavior, with more pulses at high energies than at low energies, is observed when the carrier-to-envelope phase of the laser field is changed by 90$^\circ$.} HHG simulations indicate that the time-dependent phase matching of the harmonics contributes in a non-trivial way to the structure of the pulse train. Two-color laser-assisted photoionization enables us to unravel the dynamical influence of subcycle phase matching on the spectral properties of the attosecond pulse train, going beyond the predictions of the response of a single atom to a strong laser field.

physics.atom-ph↗

arXiv2022

Efficient generation of high-order harmonics in gases

High-order harmonic generation (HHG) in gases leads to short-pulse extreme ultraviolet (XUV) radiation useful in a number of applications, for example, attosecond science and nanoscale imaging. However, this process depends on many parameters and there is still no consensus on how to choose the target geometry to optimize the source efficiency. Here, we review the physics of HHG with emphasis on the macroscopic aspects of the nonlinear interaction. We analyze the influence of medium length, pressure, position of the medium and intensity of the driving laser on the HHG conversion efficiency (CE), using both numerical modelling and analytical expressions. We find that efficient high-order harmonic generation can be realized over a large range of pressures and medium lengths, if these follow a certain hyperbolic equation. The spatial and temporal properties of the generated radiation are, however, strongly dependent on the choice of pressure and medium length. Our results explain the large versatility in gas target design for efficient HHG and provide design guidance for future high-flux XUV sources.

physics.optics↗

arXiv2020

Attosecond timing of electron emission from a molecular shape resonance

Shape resonances in physics and chemistry arise from the spatial confinement of a particle by a potential barrier. In molecular photoionization, these barriers prevent the electron from escaping instantaneously, so that nuclei may move and modify the potential, thereby affecting the ionization process. By using an attosecond two-color interferometric approach in combination with high spectral resolution, we have captured the changes induced by the nuclear motion on the centrifugal barrier that sustains the well-known shape resonance in valence-ionized N$_2$. We show that despite the nuclear motion altering the bond length by only $2\%$, which leads to tiny changes in the potential barrier, the corresponding change in the ionization time can be as large as $200$ attoseconds. This result poses limits to the concept of instantaneous electronic transitions in molecules, which is at the basis of the Franck-Condon principle of molecular spectroscopy.

physics.chem-ph↗

arXiv2020

Attosecond photoionization dynamics in the vicinity of the Cooper minima in argon

Using a spectrally resolved electron interferometry technique, we measure photoionization time delays between the $3s$ and $3p$ subshells of argon over a large 34-eV energy range covering the Cooper minima in both subshells. The observed strong variations of the $3s-3p$ delay difference, including a sign change, are well reproduced by theoretical calculations using the Two-Photon Two-Color Random Phase Approximation with Exchange. Strong shake-up channels lead to photoelectrons spectrally overlapping with those emitted from the $3s$ subshell. These channels need to be included in our analysis to reproduce the experimental data. Our measurements provide a stringent test for multielectronic theoretical models aiming at an accurate description of inter-channel correlation.

physics.atom-ph↗

arXiv2019

Compact 200 kHz HHG source driven by a few-cycle OPCPA

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 6fs pulses with 9μJ pulse energy at 200kHz repetition rate. 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 3μJ 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) pumpprobe experiments, where the available pulse energy from the laser has to be distributed economically between pump and probe pulses.

physics.atom-ph↗

arXiv2018

Temporal Resolution of the RABBITT technique

One of the most ubiquitous techniques within attosecond science is the so-called Reconstruction of Attosecond Bursts by Interference of Two-Photon Transitions (RABBITT). Originally proposed for the characterization of attosecond pulses, it has been successfully applied to accurate determinations of time delays in photoemission. Here, we examine in detail, using numerical simulations, the effect of the spatial and temporal properties of the light fields and of the experimental procedure on the accuracy of the method. This allows us to identify the necessary conditions to achieve the best temporal resolution in RABBITT measurements.

physics.atom-ph↗

arXiv2017

Time-frequency representations of autoionization dynamics in helium

Autoionization, which results from the interference between direct photoionization and photoexcitation to a discrete state decaying to the continuum by configuration interaction, is a well known example of the important role of electron correlation in light-matter interaction. Information on this process can be obtained by studying the spectral, or equivalently, temporal complex amplitude of the ionized electron wavepacket. Using an energy-resolved interferometric technique, we measure the spectral amplitude and phase of autoionized wavepackets emitted via the sp2+ and sp3+ resonances in helium. These measurements allow us to reconstruct the corresponding temporal profiles by Fourier transform. In addition, applying various time-frequency representations, we observe the build up of the wavepackets in the continuum, monitor the instantaneous frequencies emitted at any time and disentangle the dynamics of the direct and resonant ionization channels.

physics.atom-ph↗

arXiv2017

Photoionization in the time and frequency domain

Ultrafast processes in matter, such as the electron emission following light absorption, can now be studied using ultrashort light pulses of attosecond duration ($10^{-18}$s) in the extreme ultraviolet spectral range. The lack of spectral resolution due to the use of short light pulses may raise serious issues in the interpretation of the experimental results and the comparison with detailed theoretical calculations. Here, we determine photoionization time delays in neon atoms over a 40 eV energy range with an interferometric technique combining high temporal and spectral resolution. We spectrally disentangle direct ionization from ionization with shake up, where a second electron is left in an excited state, thus obtaining excellent agreement with theoretical calculations and thereby solving a puzzle raised by seven-year-old measurements. Our experimental approach does not have conceptual limits, allowing us to foresee, with the help of upcoming laser technology, ultra-high resolution time-frequency studies from the visible to the x-ray range.

physics.atom-ph↗

arXiv2016

Sub-cycle ionization dynamics revealed by trajectory resolved, elliptically-driven high-order harmonic generation

The sub-cycle dynamics of electrons driven by strong laser fields is central to the emerging field of attosecond science. We demonstrate how the dynamics can be probed through high-order harmonic generation, where different trajectories leading to the same harmonic order are initiated at different times, thereby probing different field strengths. We find large differences between the trajectories with respect to both their sensitivity to driving field ellipticity and resonant enhancement. To accurately describe the ellipticity dependence of the long trajectory harmonics we must include a sub-cycle change of the initial velocity distribution of the electron and its excursion time. The resonant enhancement is observed only for the long trajectory contribution of a particular harmonic when a window resonance in argon, which is off-resonant in the field-free case, is shifted into resonance due to a large dynamic Stark shift.

physics.atom-ph↗

arXiv2016

Two-photon double ionization of neon using an intense attosecond pulse train

We present the first demonstration of two-photon double ionization of neon using an intense extreme ultraviolet (XUV) attosecond pulse train (APT) in a photon energy regime where both direct and sequential mechanisms are allowed. For an APT generated through high-order harmonic generation (HHG) in argon we achieve a total pulse energy close to 1 $μ$J, a central energy of 35 eV and a total bandwidth of $\sim30$ eV. The APT is focused by broadband optics in a neon gas target to an intensity of $3\cdot10^{12} $W$\cdot$cm$^{-2}$. By tuning the photon energy across the threshold for the sequential process the double ionization signal can be turned on and off, indicating that the two-photon double ionization predominantly occurs through a sequential process. The demonstrated performance opens up possibilities for future XUV-XUV pump-probe experiments with attosecond temporal resolution in a photon energy range where it is possible to unravel the dynamics behind direct vs. sequential double ionization and the associated electron correlation effects.

physics.atom-ph↗

arXiv2015

Scale-invariant nonlinear optics in gases

Nonlinear optical methods are becoming ubiquitous in many areas of modern photonics. They are, however, often limited to a certain range of input parameters, such as pulse energy and average power, since restrictions arise from, for example, parasitic nonlinear effects, damage problems and geometrical considerations. Here, we show that many nonlinear optics phenomena in gaseous media are scale-invariant if spatial coordinates, gas density and laser pulse energy are scaled appropriately. We develop a general scaling model for (3+1)-dimensional wave equations, demonstrating the invariant scaling of nonlinear pulse propagation in gases. Our model is numerically applied to high-order harmonic generation and filamentation as well as experimentally verified using the example of pulse post-compression via filamentation. Our results provide a simple recipe for up-or downscaling of nonlinear processes in gases with numerous applications in many areas of science.

physics.optics↗

arXiv2015

Phase measurement of a Fano window resonance using tunable attosecond pulses

We study the photoionization of argon atoms close to the 3s$^2$3p$^6$ $\rightarrow$ 3s$^1$3p$^6$4p $\leftrightarrow$ 3s$^2$3p$^5$ $\varepsilon \ell$, $\ell$=s,d Fano window resonance. An interferometric technique using an attosecond pulse train, i.e. a frequency comb in the extreme ultraviolet range, and a weak infrared probe field allows us to study both amplitude and phase of the photoionization probability amplitude as a function of photon energy. A theoretical calculation of the ionization process accounting for several continuum channels and bandwidth effects reproduces well the experimental observations and shows that the phase variation of the resonant two-photon amplitude depends on the interaction between the channels involved in the autoionization process.

physics.atom-ph↗

arXiv2012

Introduction to attosecond time-delays in photoionization

This tutorial presents an introduction to the interaction of light and matter on the attosecond timescale. Our aim is to detail the theoretical description of ultra-short time-delays, and to relate these to the phase of extreme ultraviolet (XUV) light pulses and to the asymptotic phase-shifts of photoelectron wave packets. Special emphasis is laid on time-delay experiments, where attosecond XUV pulses are used to photoionize target atoms at well-defined times, followed by a probing process in real time by a phase-locked, infrared laser field. In this way, the laser field serves as a "clock" to monitor the ionization event, but the observable delays do not correspond directly to the delay associated with single-photon ionization. Instead, a significant part of the observed delay originates from a measurement induced process, which obscures the single-photon ionization dynamics. This artifact is traced back to a phase-shift of the above-threshold ionization transition matrix element, which we call the continuum-continuum phase. It arises due to the laser-stimulated transitions between Coulomb continuum states. As we shall show here, these measurement-induced effects can be separated from the single-photon ionization process, using analytical expressions of universal character, so that eventually the attosecond time-delays in photoionization can be accessed.

physics.atom-ph↗

arXiv2012

Photoemission time-delay measurements and calculations close to the 3s ionization minimum in Ar

We present experimental measurements and theoretical calculations of photoionization time delays from the $3s$ and $3p$ shells in Ar in the photon energy range of 32-42 eV. The experimental measurements are performed by interferometry using attosecond pulse trains and the infrared laser used for their generation. The theoretical approach includes intershell correlation effects between the 3s and 3p shells within the framework of the random phase approximation with exchange (RPAE). The connection between single-photon ionization and the two-color two-photon ionization process used in the measurement is established using the recently developed asymptotic approximation for the complex transition amplitudes of laser-assisted photoionization. We compare and discuss the theoretical and experimental results especially in the region where strong intershell correlations in the 3s to kp channel lead to an induced "Cooper" minimum in the 3s ionization cross-section.

physics.atom-ph↗

arXiv2012

Theory of attosecond delays in laser-assisted photoionization

We study the temporal aspects of laser-assisted extreme ultraviolet (XUV) photoionization using attosecond pulses of harmonic radiation. The aim of this paper is to establish the general form of the phase of the relevant transition amplitudes and to make the connection with the time-delays that have been recently measured in experiments. We find that the overall phase contains two distinct types of contributions: one is expressed in terms of the phase-shifts of the photoelectron continuum wavefunction while the other is linked to continuum--continuum transitions induced by the infrared (IR) laser probe. Our formalism applies to both kinds of measurements reported so far, namely the ones using attosecond pulse trains of XUV harmonics and the others based on the use of isolated attosecond pulses (streaking). The connection between the phases and the time-delays is established with the help of finite difference approximations to the energy derivatives of the phases. This makes clear that the observed time-delays is a sum of two components: a one-photon Wigner-like delay and an universal delay that originates from the probing process itself.

physics.atom-ph↗

arXiv2011

Quantum mechanical approach to probing the birth of attosecond pulses using a two-color field

We investigate the generation of even and odd harmonics using an intense laser and a weak second harmonic field. Our theoretical approach is based on solving the saddle-point equations within the Strong Field Approximation. The phase of the even harmonic oscillation as a function of the delay between fundamental and second harmonic field is calculated and its variation with energy is found to be in good agreement with recent experimental results. We also find that the relationship between this phase variation and the group delay of the attosecond pulses, depends on the intensity and wavelength of the fundamental field as well as the ionization potential of the atom.

quant-ph↗