arXiv subjects

Mathieu Gisselbrecht

Publications and source records attributed to Mathieu Gisselbrecht.

At least 19 recordsLinked to original sources

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↗

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 $2{\pi}$ increase across the resonance or a sigmo\"idal less than ${\pi}$ 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

Controlled molecule injector for cold, dense, and pure molecular beams at the European x-ray free-electron laser

A permanently available molecular-beam injection setup for controlled molecules (COMO) was installed and commissioned at the small quantum systems (SQS) instrument at the European x-ray free-electron laser (EuXFEL). A $b$-type electrostatic deflector allows for pure state-, size-, and isomer-selected samples of polar molecules and clusters. The source provides a rotationally cold ($T\approx1$~K) and dense ($\rho\approx10^8$~cm$^{-3}$) molecular beam with pulse durations up to 100~\us generated by a new version of the Even-Lavie valve. Here, a performance overview of the COMO setup is presented along with characterization experiments performed both, with an optical laser at the Center for Free-Electron-Laser Science and with x-rays at EuXFEL under burst-mode operation. COMO was designed to be attached to different instruments at the EuXFEL, in particular at the small quantum systems (SQS) and single particles, clusters, and biomolecules (SPB) instruments. This advanced controlled-molecules injection setup enables XFEL studies using highly defined samples with soft and hard x-ray FEL radiation for applications ranging from atomic, molecular, and cluster physics to elementary processes in chemistry and biology.

physics.chem-ph↗

arXiv2023

Generation of entanglement using a short-wavelength seeded free-electron laser

Quantum entanglement between the degrees of freedom encountered in the classical world is challenging to observe due to the surrounding environment. To elucidate this issue, we investigate the entanglement generated over ultrafast timescales in a bipartite quantum system comprising two massive particles: a free-moving photoelectron, which expands to a mesoscopic length-scale, and a light-dressed atomic ion, which represents a hybrid state of light and matter. Although the photoelectron spectra are measured classically, the entanglement allows us to reveal information about the dressed-state dynamics of the ion and the femtosecond extreme ultraviolet pulses delivered by a seeded free-electron laser. The observed generation of entanglement is interpreted using the time-dependent von Neumann entropy. Our results unveil the potential for using short-wavelength coherent light pulses from free-electron lasers to generate entangled photoelectron and ion systems for studying spooky action at a distance.

quant-ph↗

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

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

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 $\pi$-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↗

arXiv2022

Studying ultrafast Rabi dynamics with a short-wavelength seeded free-electron laser

Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field. They are ubiquitous in physics with applications in different areas such as photonics, nano-electronics, electron microscopy, and quantum information. While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light-matter interaction within the rotating wave approximation\cite. Although intense nanometer-wavelength light-sources have been available for more than a decade, Rabi dynamics at such short wavelengths have not been observed directly. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser can drive Rabi oscillations between the ground state and an excited state in helium atoms. The measured photoemission signal revealed an Autler-Townes doublet as well as an avoided crossing, phenomena that are both trademarks of quantum optics. Using theoretical analyses that go beyond the strong-field approximation, we found that the ultrafast build-up of the doublet structure follows from a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond and few-femtosecond extreme-ultraviolet pulses, our results offer opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.

quant-ph↗

arXiv2021

Probing electronic decoherence with high-resolution attosecond photoelectron interferometry

Quantum coherence plays a fundamental role in the study and control of ultrafast dynamics in matter. In the case of photoionization, entanglement of the photoelectron with the ion is a well known source of decoherence when only one of the particles is measured. Here we investigate decoherence due to entanglement of the radial and angular degrees of freedom of the photoelectron. We study two-photon ionization via the 2s2p autoionizing state in He using high spectral resolution photoelectron interferometry. Combining experiment and theory, we show that the strong dipole coupling of the 2s2p and 2p$^2$ states results in the entanglement of the angular and radial degrees of freedom. This translates, in angle integrated measurements, into a dynamic loss of coherence during autoionization.

physics.atom-ph↗

arXiv2021

Complete characterization of multi-channel single photon ionization

Ionization of atoms and molecules by absorption of a light pulse results in electron wavepackets carrying information on the atomic or molecular structure as well as on the dynamics of the ionization process. These wavepackets can be described as a coherent sum of waves of given angular momentum, called partial waves, each characterized by an amplitude and a phase. The complete characterization of the individual angular momentum components is experimentally challenging, requiring the analysis of the interference between partial waves both in energy and angle. Using a two-photon interferometry technique based on extreme ultraviolet attosecond and infrared femtosecond pulses, we characterize the individual partial wave components in the photoionization of the 2p shell in neon. The study of the phases of the angular momentum channels allows us to unravel the influence of short-range, correlation and centrifugal effects. This approach enables the complete reconstruction of photoionization electron wavepackets in time and space, providing insight into the photoionization dynamics.

physics.atom-ph↗

arXiv2021

Fission of charged nano-hydrated ammonia clusters -- microscopic insights on the nucleation processes

While largely studied on the macroscopic scale, the dynamics leading to nucleation and fission processes in atmospheric aerosols are still poorly understood at the molecular level. Here, we present a joint experimental-theoretical study of a model system consisting of hydrogen-bonded ammonia and water molecules. Experimentally, the clusters were produced via adiabatic co-expansion. Double ionization ionic products were prepared using synchrotron radiation and analyzed with coincident mass- and 3D momentum spectroscopy. Calculations were carried out using ab initio molecular dynamics to understand the fragmentation within the first 500 fs. Further exploration of the potential energy surfaces were performed at a DFT level of theory to gain information on the energetics of the processes. Water was identified as an efficient nano-droplet stabilizer, and is found to have a significant effect even at low water content. On the molecular level, the stabilizing role of water can be related to an increase in the dissociation energy between ammonia molecules and the water enriched environment at the cluster surface. Furthermore, our results support the role of ammonium as a charge carrier in the solution, preferentially bound to surrounding ammonia molecules, which can influence atmospheric nucleation process.

physics.atm-clus↗

arXiv2020

A high-repetition rate attosecond light source for time-resolved coincidencespectroscopy

Attosecond pulses, produced through high-order harmonic generation in gases, have been successfully used for observing ultrafast, sub-femtosecond electron dynamics in atoms, molecules and solid state systems. Today's typical attosecond sources, however, are often impaired by their low repetition rate and the resulting insufficient statistics, especially when the number of detectable events per shot is limited. This is the case for experiments where several reaction products must be detected in coincidence, and for surface science applications where space-charge effects compromise spectral and spatial resolution. In this work, we present an attosecond light source operating at 200 kHz, which opens up the exploration of phenomena previously inaccessible to attosecond interferometric and spectroscopic techniques. Key to our approach is the combination of a high repetition rate, few-cycle laser source, a specially designed gas target for efficient high harmonic generation, a passively and actively stabilized pump-probe interferometer and an advanced 3D photoelectron/ion momentum detector. While most experiments in the field of attosecond science so far have been performed with either single attosecond pulses or long trains of pulses, we explore the hitherto mostly overlooked intermediate regime with short trains consisting of only a few attosecond pulses.e also present the first coincidence measurement of single-photon double ionization of helium with full angular resolution, using an attosecond source. This opens up for future studies of the dynamic evolution of strongly correlated electrons.

physics.atom-ph↗

arXiv2020

Attosecond electron-spin dynamics in Xe 4d photoionization

The photoionization of xenon atoms in the 70-100 eV range reveals several fascinating physical phenomena such as a giant resonance induced by the dynamic rearrangement of the electron cloud after photon absorption, an anomalous branching ratio between intermediate Xe$^+$ states separated by the spin-orbit interaction and multiple Auger decay processes. These phenomena have been studied in the past, using in particular synchrotron radiation, but without access to real-time dynamics. Here, we study the dynamics of Xe 4d photoionization on its natural time scale combining attosecond interferometry and coincidence spectroscopy. A time-frequency analysis of the involved transitions allows us to identify two interfering ionization mechanisms: the broad giant dipole resonance with a fast decay time less than 50 as and a narrow resonance at threshold induced by spin-flip transitions, with much longer decay times of several hundred as. Our results provide new insight into the complex electron-spin dynamics of photo-induced phenomena.

physics.atom-ph↗

arXiv2019

Controlling the Photoelectric Effect in the Time Domain

When an atom or molecule absorbs a high-energy photon, an electron is emitted with a well-defined energy and a highly-symmetric angular distribution, ruled by energy quantization and parity conservation. These rules seemingly break down when small quantum systems are exposed to short and intense light pulses, which raise the question of their universality for the simplest case of the photoelectric effect. Here we investigate the photoionization of helium by a sequence of attosecond pulses in the presence of a weak infrared dressing field. We continuously control the energy and introduce an asymmetry in the emission direction of the photoelectrons, thus contradicting well established quantum-mechanical predictions. This control is possible due to an extreme temporal confinement of the light-matter interaction. Our work extends time-domain coherent control schemes to one of the fastest processes in nature, the photoelectric effect.

physics.atom-ph↗

arXiv2019

Phase Control of Attosecond Pulses in a Train

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 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 semiclassical three-step model for high-order harmonic generation.

physics.atom-ph↗

arXiv2019

A Versatile Velocity Map Ion-Electron Covariance Imaging Spectrometer for High-Intensity XUV Experiments

We report on the design and performance of a velocity map imaging (VMI) spectrometer optimized for experiments using high-intensity extreme ultraviolet (XUV) sources such as laser-driven high-order harmonic generation (HHG) sources and free-electron lasers (FELs). Typically exhibiting low repetition rates and high single-shot count rates, such~experiments do not easily lend themselves to coincident detection of photo-electrons and -ions. In order to obtain molecular frame or reaction channel-specific information, one has to rely on other correlation techniques, such as covariant detection schemes. Our device allows for combining different photo-electron and -ion detection modes for covariance analysis. We present the expected performance in the different detection modes and present the first results using an intense high-order harmonic generation (HHG) source.

physics.atom-ph↗

arXiv2018

Fano's propensity rule in angle-resolved attosecond pump-probe photoionization

In a seminal article, Fano predicts that absorption of light occurs preferably with increase of angular momentum. Here we generalize Fano's propensity rule to laser-assisted photoionization, consisting of absorption of an extreme-ultraviolet photon followed by absorption or emission of an infrared photon. The predicted asymmetry between absorption and emission leads to incomplete quantum interference in attosecond photoelectron interferometry. It explains both the angular-dependence of the photoionization time delays and the delay-dependence of the photoelectron angular distributions. Our theory is verified by experimental results in Ar in the 20-40 eV range.

physics.atom-ph↗