arXiv subjects

Thierry Ruchon

Publications and source records attributed to Thierry Ruchon.

16 recordsLinked to original sources

arXiv2026

Optical design for implementing non-collinear circularly polarized high harmonic generation in an enhancement cavity

We introduce an original optical cavity design intended to efficiently output-couple extreme ultraviolet (XUV) light produced via cavity-enhanced high harmonic generation (CE-HHG). It supports the amplification of oppositely circularly polarized modes, crossing with a small angle in the high finesse cavity, where circularly polarized HHG scheme (NCP-HHG) will be implemented. We present an analytical model, numerical simulations, and experimental results obtained with a low-power continuous (CW) laser, demonstrating the strong potential of the cavity as an efficient XUV output coupling method. In particular, it is well suited for producing the 7th harmonic (H7) from an Ytterbium frequency comb at 8.4 eV, which is of particular interest for precision nuclear spectroscopy of Thorium.

physics.optics↗

arXiv2026

Controlled generation of high-harmonic spatiotemporal optical vortices

Spatiotemporal optical vortex (STOV) pulses are puzzling states of light, which see their transverse orbital angular momentum being debated in spite of possessing a topological charge. Thus far studied at conventional optical wavelengths, we herein demonstrate their upconversion to extreme ultraviolet (XUV) frequencies via high-harmonic generation (HHG). Circularly-symmetric infrared STOV pulses of topological charges $\ell=\pm1$ and $\pm2$ from a bespoke pulse shaper are focused in argon to drive harmonics, each order $q$ forming a spatiospectral ring in the far-field. Dependence of their radii on $q$ and $\ell$ indicates XUV vortices of charge ${\ell}_{q} = q \times \ell$, and sensitivity of these modes to the focus position further establishes control over their production. The availability of XUV STOVs unlocks investigations and applications of their elusive angular momentum in the context of photoionization and other ultrafast spectroscopies.

physics.optics↗

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↗

arXiv2025

Soft x-rays with Orbital Angular Momentum for resonant scattering experiments at the SOLEIL synchrotron

The paper presents a comprehensive description of a new setup implemented and commissioned at the SEXTANTS beamline of the SOLEIL synchrotron for absorption and scattering experiments with x-ray beams carrying an orbital angular momentum, also known as twisted x-ray beams. Two alternative methods have been implemented, based on the use of either spiral zone plates or fork gratings devices, and we show how they can be used for both defining and assessing the orbital angular momentum of an x-ray beam. We show also how multiple devices can be used in sequence to define an integer arithmetic of the orbital angular momentum of the final x-ray beam. Finally, we report the results of the first resonant scattering pilot experiments in transmission and reflection mode, intended to assess the feasibility of future users measurements. The availability of twisted soft x-rays complements the range of experimental techniques in elastic, resonant and coherent scattering available at the SEXTANTS beamline of the SOLEIL synchrotron.

cond-mat.mtrl-sci↗

arXiv2025

Optical spin-orbit interaction induced by magnetic textures

Contrary to the optical spin angular momentum (SAM), the role played by the orbital angular momentum (OAM) of light in magneto-optics remains largely unexplored. However, the SAM and OAM are known to be coupled when light interacts with non-homogeneous and non-isotropic materials. Here we predict that the OAM carried by each photon in a light beam is modified upon reflection on magnetic textures like skyrmions, and that the sign of this variation is governed by the SAM of the incident field. Our predictions can be readily tested by performing circular dichroism measurements, and may provide new routes to shape light's angular momentum with magnetism.

physics.optics↗

arXiv2025

Energy and photon centroids of spatiotemporal light pulses and consequences for their intrinsic orbital angular momentum

An ongoing debate surrounding the intrinsic transverse orbital angular momentum (OAM) attributed to spatiotemporal optical vortex (STOV) light pulses has raised the energy and photon-density centroids as two alternative frameworks to define the center of a free electromagnetic wavepacket. We herein derive, within a single formalism, lowest-order expressions for the positions and velocities of both centroids, directly applicable to an arbitrary scalar, near-paraxial and quasi-monochromatic pulse envelope formulated in space-time. Examining pulses with structures including temporal chirp, wavefront rotation, Gaussian-type STOVs and tilted lobulated profiles, we illustrate general principles underlying the shifts and propagation dynamics of the two centroids, and discuss how these properties underpin the value and conservation of intrinsic OAM referenced to either centroid. Finally, despite widespread use of the notion of intrinsic OAM "per photon", we argue that in neither framework could individual STOV photons be said to carry a well-defined quantum of intrinsic transverse OAM, as such quantities do not write as expectation values of a single operator for which STOV states could form a basis of orthogonal eigenmodes. This contrasts with the well-established quantization scheme for the total longitudinal OAM of light in spatial vortex beams, bearing implications for the interpretation of future experiments involving STOV pulses in quantum optics, nonlinear wave-mixing or light-matter interactions.

physics.optics↗

arXiv2023

Ultrafast Hidden Spin Polarization Dynamics of Bright and Dark Excitons in 2H-WSe$_2$

We performed spin-, time- and angle-resolved extreme ultraviolet photoemission spectroscopy (STARPES) of excitons prepared by photoexcitation of inversion-symmetric 2H-WSe$_2$ with circularly polarized light. The very short probing depth of XUV photoemission permits selective measurement of photoelectrons originating from the top-most WSe$_2$ layer, allowing for direct measurement of hidden spin polarization of bright and momentum-forbidden dark excitons. Our results reveal efficient chiroptical control of bright excitons' hidden spin polarization. Following optical photoexcitation, intervalley scattering between nonequivalent K-K' valleys leads to a decay of bright excitons' hidden spin polarization. Conversely, the ultrafast formation of momentum-forbidden dark excitons acts as a local spin polarization reservoir, which could be used for spin injection in van der Waals heterostructures involving multilayer transition metal dichalcogenides.

cond-mat.mes-hall↗

arXiv2022

Conservation of a Half-Integer Angular Momentum in Nonlinear Optics with a Polarization Möbius Strip

Symmetries and conservation laws of energy, linear momentum and angular momentum play a central role in physics, in particular in nonlinear optics. Recently, light fields with non trivial topology, such as polarization Möbius strips or torus-knot beams, have been unveiled. They cannot be associated to well-defined values of orbital and spin angular momenta (OAM and SAM), but are invariant under coordinated rotations, i.e. rotational symmetries that are generated by the generalized angular momentum (GAM) operator, a mixture of the OAM and SAM operators. The discovery of the GAM, which at variance with integer-valued OAM and SAM, can have arbitrary value, and raises the question of its conservation in nonlinear optical processes. By driving high harmonic generation with a polarization Möbius strip and implementing novel OAM characterization methods in the XUV range, we experimentally observe the conservation of the GAM, each harmonic carrying a precise half-integer GAM charge equal to that of the fundamental field multiplied by the harmonic order. The GAM is thus revealed as the appropriate quantum number to describe nonlinear processes driven by light fields containing topological polarization singularities.

physics.optics↗

arXiv2021

Observation of magnetic helicoidal dichroism with extreme ultraviolet light vortices

We report on the experimental evidence of magnetic helicoidal dichroism, observed in the interaction of an extreme ultraviolet vortex beam carrying orbital angular momentum with a magnetic vortex. Numerical simulations based on classical electromagnetic theory show that this dichroism is based on the interference of light modes with different orbital angular momenta, which are populated after the interaction between the light phase chirality and the magnetic topology. This observation gives insight into the interplay between orbital angular momentum and magnetism, and sets the framework for the development of new analytical tools to investigate ultrafast magnetization dynamics.

physics.optics↗

arXiv2020

In situ sub-50 attosecond active stabilization of the delay between infrared and extreme ultraviolet light pulses

The blooming of attosecond science (1 as = $10^{-18}$ s) has raised the need to exquisitely control the delay between two ultrashort light pulses, one of them being intense and in the visible spectral range, while the second is weak and in the Extreme Ultra-Violet spectral range. Here we introduce a robust technique, named LIZARD (Laser-dressed IoniZation for the Adjustment of the pump-pRobe Delay), allowing an active stabilization of this pump-probe delay. The originality of the method lies in an error signal calculated from a two-photon photoelectron signal obtained by photoionizing a gas target in an electronic spectrometer with the two superimposed beams. The modulation of sidebands in phase quadrature allows us to perform an \textit{in situ} measurement of the pump-probe phase, and to compensate for fluctuations with an uniform noise sensitivity over a large range of delays. Despite an interferometer length of several meters, we achieved a long term stability of 28 as RMS over hours. This method could be applied to the stabilization of other types of two-color interferometers, provided that one of the propagating beams is capable of photoionizing a target.

physics.atom-ph↗

arXiv2020

Magnetic helicoidal dichroism in reflection by magnetic vortices

Identifying and imaging spin textures of ever more complex magnetic structures has become a major challenge in the past decade, especially at ultrashort timescales. Most of current approaches are based on the analysis of their polarization and magnetization-dependent reflectivities. Based on our joint publication XXX XX XXXXXX, we introduce a different concept, centered on the coupling of magnetic structures with light beams carrying orbital angular momentum (OAM). Upon reflection by a magnetic vortex, an incoming beam with a unique value $\ell$ of OAM gets enriched in the neighboring OAM modes $\ell\pm 1$. It results in anisotropic far-field images, which are identified as a Magnetic Helicoidal Dichroism (MHD) signal. Their analysis allow to retrieve the complex magneto-optical constants with excellent precision. This method, which does not require any polarization-resolved analysis, is promising for a quick identification of spin textures, including with attosecond to femtosecond time resolutions.

physics.optics↗

arXiv2020

Electromagnetic theory of Helicoidal Dichroism in reflection from magnetic structures

We present the classical electromagnetic theory framework of reflection of a light beam carrying Orbital Angular Momentum (OAM) by an in-plane magnetic structure with generic symmetry. Depending on the magnetization symmetry, we find a change in the OAM content of the reflected beam due to magneto-optic interaction and an asymmetric far-field intensity profile. This leads to three types of Magnetic Helicoidal Dichroism (MHD), observed when switching the OAM of the incoming beam, the magnetization sign, or both. In cases of sufficient symmetries, we establish analytical formulas which link an experimentally accessible MHD signal up to $10\%$ to the Magneto-Optical Kerr Effect (MOKE) constants. Magnetic vortices are particularly enlightening and promising targets, for which we explore the implications of our theory in the joint publication XX XXX XXXXXX.

physics.optics↗

arXiv2020

Attosecond-resolved photoionization of chiral molecules

Chiral light-matter interactions have been investigated for two centuries, leading to the discovery of many chiroptical processes used for discrimination of enantiomers. Whereas most chiroptical effects result from a response of bound electrons, photoionization can produce much stronger chiral signals that manifest as asymmetries in the angular distribution of the photoelectrons along the light propagation axis. Here we implement a self-referenced attosecond photoelectron interferometry to measure the temporal profile of the forward and backward electron wavepackets emitted upon photoionization of camphor by circularly polarized laser pulses. We found a delay between electrons ejected forward and backward, which depends on the ejection angle and reaches 24 attoseconds. The asymmetric temporal shape of electron wavepackets emitted through an autoionizing state further reveals the chiral character of strongly-correlated electronic dynamics.

physics.chem-ph↗

arXiv2019

Spin-, time- and angle-resolved photoemission spectroscopy on WTe$_2$

We combined a spin-resolved photoemission spectrometer with a high-harmonic generation (HHG) laser source in order to perform spin-, time- and angle-resolved photoemission spectroscopy (STARPES) experiments on the transition metal dichalcogenide bulk WTe$_2$, a possible Weyl type-II semimetal. Measurements at different femtosecond pump-probe delays and comparison with spin-resolved one-step photoemission calculations provide insight into the spin polarization of electrons above the Fermi level in the region where Weyl points of WTe$_2$ are expected. We observe a spin accumulation above the Weyl points region, that is consistent with a spin-selective bottleneck effect due to the presence of spin polarized cone-like electronic structure. Our results support the feasibility of STARPES with HHG, which despite being experimentally challenging provides a unique way to study spin dynamics in photoemission.

cond-mat.mtrl-sci↗

arXiv2019

Time-resolved inner-shell photoelectron spectroscopy: from a bound molecule to an isolated atom

Due to its element- and site-specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (CH$_3$I) is investigated by ionization above the iodine 4d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.

physics.chem-ph↗

arXiv2017

Coulomb explosion imaging of concurrent CH$_{2}$BrI photodissociation dynamics

The dynamics following laser-induced molecular photodissociation of gas-phase CH$_{2}$BrI at 271.6 nm were investigated by time-resolved Coulomb explosion imaging using intense near-IR femtosecond laser pulses. The observed delay-dependent photofragment momenta reveal that CH$_{2}$BrI undergoes C-I cleavage, depositing 65.6% of the available energy into internal product states, and that absorption of a second UV photon breaks the C-Br bond of CH$_{2}$Br. Simulations confirm that this mechanism is consistent with previous data recorded at 248 nm, demonstrating the sensitivity of Coulomb explosion imaging as a real-time probe of chemical dynamics.

physics.chem-ph↗