arXiv subjects

J. Caillat

Publications and source records attributed to J. Caillat.

7 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↗

arXiv2023

Production of positronium chloride: A study of the charge exchange reaction between Ps and Cl$^{-}$

We present cross sections for the formation of positronium chloride (PsCl) in its ground state from the charge exchange between positronium (Ps) and chloride (Cl$^-$) in the range of 10 meV - 100 eV Ps energy. We have used theoretical models based on the first Born approximation in its three-body formulation. We simulated the collisions between Ps and Cl$^-$ using ab-initio methods at both mean-field and correlated levels extrapolated to the complete basis set limit. We have investigated Ps excited states up to ${n=4}$. The results suggest that the channel Ps(${n=2}$) is of particular interest for the production of PsCl in the ground state, and shows that an accurate treatment of the electronic correlation leads to a significant change in the global shape of the PsCl production cross section with respect to the mean-field level.

physics.chem-ph↗

arXiv2022

Phase-resolved attosecond near-threshold photoionization of molecular nitrogen

We photoionize nitrogen molecules with a train of extreme ultraviolet attosecond pulses together with a weak infrared field. We measure the phase of the two-color two-photon ionization transition (molecular phase) for different states of the ion. We observe a 0.76 $π$ shift for the electrons produced in the ionization channels leading to the X$^2 Σ_g^+$, $v'=1$ and $v'=2$ states. We relate this phase shift to the presence of a complex resonance in the continuum. By providing both a high spectral and temporal resolution, this general approach gives access to the evolution of extremely short lived states, which is hardly accessible otherwise.

physics.atom-ph↗

arXiv2019

Attosecond dynamics through a Fano resonance: Monitoring the birth of a photoelectron

Amplitude and phase of wavepackets encode the dynamics of quantum systems. However, the rapidity of electron dynamics on the attosecond timescale has precluded their complete measurement in the time domain. Here, we demonstrate that spectrally-resolved electron interferometry reveals the amplitude and phase of a photoelectron wavepacket created through a Fano autoionizing resonance in helium. Replicas obtained by two-photon transitions interfere with reference wavepackets formed through smooth continua, allowing the full temporal reconstruction, purely from experimental data, of the resonant wavepacket released in the continuum. This in turn resolves the buildup of the autoionizing resonance on attosecond timescale. Our results, in excellent agreement with ab initio time-dependent calculations, raise prospects for both detailed investigations of ultrafast photoemission dynamics governed by electron correlation, as well as coherent control over structured electron wave-packets.

physics.atom-ph↗

arXiv2017

Laser-induced distortion of structural interferences in high harmonic generation

We study theoretically the two-center interferences occurring in high harmonic generation from diatomic molecules. By solving the time-dependent Schroedinger equation, either numerically or with the molecular strong-field approximation, we show that the electron dynamics results in a strong spectral smoothing of the interference, depending on the value and sign of the driving laser field at recombination. Strikingly, the associated phase-jumps are in opposite directions for the short and long trajectories. In these conditions, the harmonic emission is not simply proportional to the recombination dipole any more. This has important consequences in high harmonic spectroscopy, e.g., for accessing the molecular-frame recombination dipole in amplitude and phase.

physics.optics↗

arXiv2016

Synthesis and characterization of attosecond light vortices in the extreme ultraviolet

Infrared and visible light beams carrying orbital angular momentum (OAM) are currently thoroughly studied for their extremely broad applicative prospects, among which are quantum information, micromachining and diagnostic tools. Here we extend these prospects, presenting a comprehensive study for the synthesis and full characterization of optical vortices carrying OAM in the extreme ultraviolet (XUV) domain. We confirm the upconversion rules of a femtosecond infrared helically phased beam into its high-order harmonics, showing that each harmonic order carries the total number of OAM units absorbed in the process up to very high orders (57). This allows us to synthesize and characterize helically shaped XUV trains of attosecond pulses. To demonstrate a typical use of these new XUV light beams, we show our ability to generate and control, through photoionization, attosecond electron beams carrying OAM. These breakthroughs pave the route for the study of a series of fundamental phenomena and the development of new ultrafast diagnosis tools using either photonic or electronic vortices.

physics.optics↗

arXiv2010

Probing single-photon ionization on the attosecond time scale

We study photoionization of argon atoms excited by attosecond pulses using an interferometric measurement technique. We measure the difference in time delays between electrons emitted from the $3s^2$ and from the $3p^6$ shell, at different excitation energies ranging from 32 to 42 eV. The determination of single photoemission time delays requires to take into account the measurement process, involving the interaction with a probing infrared field. This contribution can be estimated using an universal formula and is found to account for a substantial fraction of the measured delay.

physics.atom-ph↗