arXiv subjects

Anne L'Huillier

Publications and source records attributed to Anne L'Huillier.

At least 19 recordsLinked to original sources

arXiv2026

Quantum optical photoelectron interferometry

We present a general theoretical framework for multiphoton processes driven by quantum light fields, establishing a direct link between photon statistics and photoelectron observables. Our results show that the autocorrelation and cross-correlation functions, which quantify the underlying photon statistics, are directly mapped onto the resulting photoelectron spectra. Although our framework is broadly applicable, we demonstrate specifically in the example of reconstruction of attosecond beating by interference of two-photon transitions (RABBIT) the influence of the light statistical properties. In this approach, the amplitude, contrast and phase of the oscillations of the sideband signal as a function of pump-probe delay reveal the quantum nature of light. We analyze these observables across several quantum configurations, including correlated infrared and harmonic modes, as well as the uncorrelated case with non-classical harmonic statistics, thereby establishing a general framework for quantum-light RABBIT spectroscopy. We compare the analytical theory with numerical simulations for the case of classical harmonics and an infrared field in a squeezed coherent state, obtaining excellent agreement. Our results reveal how the interplay between classical and quantum correlations dictates the coherence of the photoemission process, providing a new window into the quantum-optical foundations of attosecond science.

quant-ph↗

arXiv2026

Roadmap on Attosecond Science

Twenty-five years have passed since the first experimental demonstration of attosecond pulses, marking the advent of our ability to resolve and control electron motion in real time. What began as a technological breakthrough - generating the shortest flashes ever produced - has evolved into a powerful approach for probing and steering electronic dynamics in atoms, molecules, and solids. This roadmap, authored by leading experts in the field, surveys the recent rapid progress in the generation and characterization of attosecond pulses, emerging attosecond measurement and control techniques, and their expanding range of applications. It reviews current and future developments in attosecond light sources, including novel laser technologies, waveform synthesizers, new schemes for high-order harmonic generation, attosecond pulse generation at free-electron lasers, and structured light. Advances in attosecond measurement methodologies are also discussed, encompassing all-attosecond pump-probe spectroscopy, attosecond four-wave mixing, attosecond microscopy, spectroscopy with light transients, and attosecond interferometry. Furthermore, the roadmap addresses applications of attosecond spectroscopy to reveal electron dynamics in molecules and condensed matter systems from both theoretical and experimental perspectives, and highlights emerging directions at the interface with quantum optics and quantum entanglement. Overall, this work aims to serve as a comprehensive resource for navigating the evolving landscape of attosecond science.

physics.optics↗

arXiv2026

High intensity attosecond beamline for XUV pump XUV probe measurements with photon energies up to 150 eV

The field of attosecond physics has expanded significantly in recent years, yet experimental facilities supporting attosecond pump attosecond probe spectroscopy remain rare. Here, we present a newly constructed beamline for the generation and application of energetic, isolated extreme ultraviolet (XUV) and soft X-ray attosecond pulses via upscaling of high-harmonic generation (HHG) in a gas medium. The fundamental properties of the HHG radiation energy, beam profile, spectrum, and divergence are characterized and optimized. The source delivers up to 55 nJ of pulse energy within the Zr window (65-150 eV) with high stability (~5-10) and a divergence of 0.1 mrad. Numerical simulations identify optimal operating conditions consistent with experimental results. Temporal super-resolution of the driving laser is applied, resulting in a broadened spectral continuum. Furthermore, the beamline includes a split-and-delay stage before focusing the HHG radiation to a <6 um spot for pump-probe experiments using two distinct focusing optics. Spatially resolved ion microscopy is employed to trace the generated ions at the focus. The presented beamline is designed for nonlinear XUV studies with attosecond isolated pulses.

physics.optics↗

arXiv2025

Compact, intense attosecond sources driven by hollow Gaussian beams

High-order harmonic generation (HHG) enables the up-conversion of intense infrared or visible femtosecond laser pulses into extreme-ultraviolet attosecond pulses. However, the highly nonlinear nature of the process results in low conversion efficiency, which can be a limitation for applications requiring substantial pulse energy, such as nonlinear attosecond time-resolved spectroscopy or single-shot diffractive imaging. Refocusing of the attosecond pulses is also essential to achieve a high intensity, but difficult in practice due to strong chromatic aberrations. In this work, we address both the generation and the refocusing of attosecond pulses by sculpting the driving beam into a ring-shaped intensity profile with no spatial phase variations, referred to as a Hollow Gaussian beam (HGB). Our experimental and theoretical results reveal that HGBs efficiently redistribute the driving laser energy in the focus, where the harmonics are generated on a ring with low divergence, which furthermore decreases with increasing order. Although generated as a ring, the attosecond pulses can be refocused with greatly reduced chromatic spread, therefore reaching higher intensity. This approach enhances the intensity of refocused attosecond pulses and enables significantly higher energy to be delivered in the driving beam without altering the focusing conditions. These combined advantages open pathways for compact, powerful, tabletop, laser-driven attosecond light sources.

physics.optics↗

arXiv2025

Photoionization time delays probe electron correlations

The photoelectric effect, explained by Einstein in 1905, is often regarded as a one-electron phenomenon. However, in multi-electron systems, the interaction of the escaping electron with other electrons, referred to as electron correlation, plays an important role. For example, electron correlations in photoionization of the outer $s$-subshells of rare gas atoms lead to a substantial minimum in the ionization probability, which was theoretically predicted in 1972 and experimentally confirmed using synchrotron radiation. However, recent attosecond photoionization time delay measurements in argon strongly disagree with theory, thus raising questions on the nature of electron correlations leading to this minimum. In this work, combining high-spectral resolution attosecond interferometry experiments and novel theoretical calculations allows us to identify the most essential electron correlations affecting the photoemission. The measurement of time delays gives unprecedented insight into the photoionization process, unraveling details of the atomic potential experienced by the escaping electron and capturing its dynamics.

physics.atom-ph↗

arXiv2025

Influence of the laser pulse duration in high-order harmonic generation

High-order harmonic generation (HHG) in gases has been studied for almost 40 years in many different conditions, varying the laser wavelength, intensity, focusing geometry, target design, gas species, etc. However, no systematic investigation of the effect of the pulse duration has been performed in spite of its expected impact on phase-matching of the high-order harmonics. Here, we develop a compact post-compression method based on a bulk multi-pass cell enabling tunable Fourier-limited pulse durations. We examine the HHG yield as a function of the pulse duration, ranging from 42 fs to 180 fs, while maintaining identical focusing conditions and generating medium. Our findings reveal that, for a given intensity, there exists an optimum pulse duration - not necessarily the shortest - that maximizes conversion efficiency. This optimum pulse duration increases as the intensity decreases. The experimental results are corroborated by numerical simulations, which show the dependence of HHG yield on the duration and peak intensity of the driving laser and underscore the importance of the interplay between light-matter interaction and phase-matching in the non-linear medium. Our conclusion explains why HHG could be demonstrated in 1988 with pulses as long as 40 ps and intensities of just a few $10^{13}$ W/cm${^2}$.

physics.optics↗

arXiv2024

XUV yield optimization of two-color high-order harmonic generation in gases

We perform an experimental two-color high-order harmonic generation study in argon with the fundamental of an ytterbium ultrashort pulse laser and its second harmonic. The intensity of the second harmonic and its phase relative to the fundamental are varied, in a large range compared to earlier works, while keeping the total intensity constant. We extract the optimum values for the relative phase and ratio of the two colors which lead to a maximum yield enhancement for each harmonic order in the extreme ultraviolet spectrum. Within the semi-classical three-step model, the yield maximum can be associated with a flat electron return time vs. return energy distribution. An analysis of different distributions allows to predict the required relative two-color phase and ratio for a given harmonic order, total laser intensity, fundamental wavelength, and ionization potential.

physics.atom-ph↗

arXiv2024

A multidimensional approach to quantum state tomography of photoelectron wavepackets

There is a growing interest in reconstructing the density matrix of photoelectron wavepackets, in particular in complex systems where decoherence can be introduced either by a partial measurement of the system or through coupling with a stochastic environment. To this end, several methods to reconstruct the density matrix, quantum state tomography protocols, have been developed and tested on photoelectrons ejected from noble gases following absorption of extreme ultraviolet (XUV) photons from attosecond pulses. It remains a challenge to obtain model-free, single scan protocols that can reconstruct the density matrix with high fidelities. Current methods require extensive measurements or involve complex fitting of the signal. Efficient single-scan reconstructions would be of great help to increase the number of systems that can be studied. We propose a new and more efficient protocol that is able to reconstruct the continuous variable density matrix of a photoelectron in a single time delay scan. It is based on measuring the coherences of a photoelectron created by absorption of an XUV pulse using a broadband infrared (IR) probe that is scanned in time and a narrowband IR reference that is temporally fixed to the XUV pulse. We illustrate its performance for a Fano resonance in He as well as mixed states in Ar arising from spin-orbit splitting. We show that the protocol results in excellent fidelities and near-perfect estimation of the purity.

quant-ph↗

arXiv2024

The influence of final state interactions in attosecond photoelectron interferometry

Fano resonances are ubiquitous phenomena appearing in many fields of physics, e.g. atomic or molecular photoionization, or electron transport in quantum dots. Recently, attosecond interferometric techniques have been used to measure the amplitude and phase of photoelectron wavepackets close to Fano resonances in argon and helium, allowing for the retrieval of the temporal dynamics of the photoionization process. In this work, we study the photoionization of argon atoms close to the $3s^13p^64p$ autoionizing state using an interferometric technique with high spectral resolution. The phase shows a monotonic $2π$ increase across the resonance or a sigmoïdal less than $π$ variation depending on experimental conditions, e.g. the probe laser bandwidth. Using three different, state-of-the-art calculations, we show that the measured phase is influenced by the interaction between final states reached by two-photon transitions.

physics.atom-ph↗

arXiv2024

Highly versatile, two-color setup for high-order harmonic generation using spatial light modulators

We present a novel, interferometric, two-color, high-order harmonic generation setup, based on a turn-key Ytterbium-doped femtosecond laser source and its second harmonic. Each interferometer arm contains a spatial light modulator, with individual capabilities to manipulate the spatial beam profiles and to stabilize the relative delay between the fundamental and the second harmonic. Additionally, separate control of the relative power and focusing geometries of the two color beams is implemented to conveniently perform automatized scans of multiple parameters. A live diagnostics system gives continuous information during ongoing measurements.

physics.optics↗

arXiv2023

Time-resolved photoemission electron microscopy on a ZnO surface using an extreme ultraviolet attosecond pulse pair

Electrons photoemitted by extreme ultraviolet attosecond pulses derive spatially from the first few atomic surface layers and energetically from the valence band and highest atomic orbitals. As a result, it is possible to probe the emission dynamics from a narrow two-dimensional region in the presence of optical fields as well as obtain elemental specific information. However, combining this with spatially-resolved imaging is a long-standing challenge because of the large inherent spectral width of attosecond pulses as well as the difficulty of making them at high repetition rates. Here we demonstrate an attosecond interferometry experiment on a zinc oxide (ZnO) surface using spatially and energetically resolved photoelectrons. We combine photoemission electron microscopy with near-infrared pump - extreme ultraviolet probe laser spectroscopy and resolve the instantaneous phase of an infrared field with high spatial resolution. Our results show how the core level states with low binding energy of ZnO are well suited to perform spatially resolved attosecond interferometry experiments. We observe a distinct phase shift of the attosecond beat signal across the laser focus which we attribute to wavefront differences between the pump and the probe fields at the surface. Our work demonstrates a clear pathway for attosecond interferometry with high spatial resolution at atomic scale surface regions opening up for a detailed understanding of nanometric light-matter interaction.

physics.optics↗

arXiv2023

Measuring the quantum state of photoelectrons

A photoelectron, emitted due to the absorption of light quanta as described by the photoelectric effect, is often characterized experimentally by a classical quantity, its momentum. However, since the photoelectron is a quantum object, its rigorous characterization requires the reconstruction of the complete quantum state, the photoelectron's density matrix. Here, we use quantum state tomography to fully characterize photoelectrons emitted from helium and argon atoms upon absorption of ultrashort, extreme ultraviolet light pulses. While in helium we measure a pure photoelectronic state, in argon, spin-orbit interaction induces entanglement between the ion and the photoelectron, leading to a reduced purity of the photoelectron state. Our work shows how state tomography gives new insights into the fundamental quantum aspects of light-induced electronic processes in matter, bridging the fields of photoelectron spectroscopy and quantum information, and offering new spectroscopic possibilities for quantum technology.

quant-ph↗

arXiv2023

Measurement of Ultrashort Laser Pulses With a Time-Dependent Polarization State Using the D-Scan Technique

The dispersion scan (d-scan) technique is extended to measurement of the timedependent polarization state of ultrashort laser pulses. In the simplest implementation for linearly polarized ultrashort pulses, the d-scan technique records the second harmonic generation (SHG) spectrum as a function of a known spectral phase manipulation. By applying this method to two orthogonally polarized projections of an arbitrary polarized electric field and by measuring the spectrum at an intermediate angle, we can reconstruct the evolution over time of the polarization state. We demonstrate the method by measuring a polarization gate generated from 6 fs pulses with a combination of waveplates. The measurements are compared to simulations, showing an excellent agreement.

physics.optics↗

arXiv2023

Spatial aberrations in high-order harmonic generation

We investigate the spatial characteristics of high-order harmonic radiation generated in argon, and observe cross-like patterns in the far field. An analytical model describing harmonics from an astigmatic driving beam reveals that these patterns result from the order and generation position dependent divergence of harmonics. Even small amounts of driving field astigmatism may result in cross-like patterns, coming from the superposition of individual harmonics with spatial profiles elongated in different directions. By correcting the aberrations using a deformable mirror, we show that fine-tuning the driving wavefront is essential for optimal spatial quality of the harmonics.

physics.optics↗

arXiv2023

Ultra-stable and versatile high-energy resolution setup for attosecond photoelectron spectroscopy

Attosecond photoelectron spectroscopy is often performed with interferometric experimental setups that require outstanding stability. We demonstrate and characterize in detail an actively stabilized, versatile, high spectral resolution attosecond beamline. The active-stabilization system can remain ultra-stable for several hours with an RMS stability of 13 as and a total pump-probe delay scanning range of \sim 400 fs. A tunable femtosecond laser source to drive high-order harmonic generation allows for precisely addressing atomic and molecular resonances. Furthermore, the interferometer includes a spectral shaper in 4f-geometry in the probe arm as well as a tunable bandpass filter in the pump arm, which offer additional high flexibility in terms of tunability as well as narrowband or polychromatic probe pulses. We show that spectral phase measurements of photoelectron wavepackets with the rainbow RABBIT technique (reconstruction of attosecond beating by two photon transitions) with narrowband probe pulses can significantly improve the photoelectron energy resolution. In this setup, the temporal-spectral resolution of photoelectron spectroscopy can reach a new level of accuracy and precision.

physics.atom-ph↗

arXiv2022

Multi-gigawatt peak power post-compression in a bulk multi-pass cell at high repetition rate

The output of a 200 kHz, 34 W, 300 fs Yb amplifier is compressed to 31 fs with > 88 % efficiency to reach a peak power of 2.5 GW, which to date is a record for a single-stage bulk multi-pass cell. Despite operation 80 times above the critical power for self-focusing in bulk material, the setup demonstrates excellent preservation of the input beam quality. Extensive beam and pulse characterizations are performed to show that the compressed pulses are promising drivers for high harmonic generation and nonlinear optics in gases or solids.

physics.optics↗

arXiv2022

Resonant two-photon ionization of helium atoms studied by attosecond interferometry

We study resonant two-photon ionization of helium atoms via the $1s3p$, $1s4p$ and $1s5p^1$P$_1$ states using the 15$^\mathrm{th}$ harmonic of a titanium-sapphire laser for the excitation and a weak fraction of the laser field for the ionization. The phase of the photoelectron wavepackets is measured by an attosecond interferometric technique, using the 17$^\mathrm{th}$ harmonic. We perform experiments with angular resolution using a velocity map imaging spectrometer and with high energy resolution using a magnetic bottle electron spectrometer. Our results are compared to calculations using the two-photon random phase approximation with exchange to account for electron correlation effects. We give an interpretation for the multiple $π$-rad phase jumps observed, both at and away from resonance, as well as their dependence on the emission angle.

physics.atom-ph↗

arXiv2022

Continuous variable quantum state tomography of photoelectrons

We propose a continuous variable quantum state tomography protocol of electrons which result from the ionization of atoms or molecules by the absorption of extreme ultraviolet light pulses. Our protocol is benchmarked against a direct calculation of the quantum state of photoelectrons ejected from helium and argon in the vicinity of a Fano resonance. In the latter case, we furthermore distill ion-photoelectron entanglement due to spin-orbit splitting. This opens new routes towards the investigation of quantum coherence and entanglement properties on the ultrafast timescale.

physics.atom-ph↗