arXiv subjects

Yann Mairesse

Publications and source records attributed to Yann Mairesse.

At least 19 recordsLinked to original sources

arXiv2026

Direct Asymmetric Photochemistry with Synthetic Chiral Light

Circularly polarized light has long been used to distinguish the two mirror images of chiral molecules. Recently, a conceptual breakthrough has predicted that a new form of optical fields - synthetic chiral light - could usher in an 'electric-dipole revolution' in chiroptical interactions. We report the first experimental evidence for this prediction in the optical domain, using a three-dimensional laser electric field synthesized to trace a chiral pattern. The ionization and fragmentation of chiral molecules was found to depend on both the molecular handedness, and the handedness and geometry of the synthetic chiral field. Supported by two theoretical models, our results demonstrate that synthetic chiral light can induce strong chiroptical interactions, opening new horizons for asymmetric photochemistry and chiral analysis.

physics.chem-ph↗

arXiv2026

Enhanced Valley Polarization via Nonlinear Cascaded Quantum-Geometric Selection Rules

The quantum geometric properties of Bloch electrons fundamentally govern light-matter interactions and optical selection rules in solids. In semiconducting transition-metal dichalcogenides, circularly polarized excitation near the band edge enables valley-selective interband transitions, providing the basis for valleytronics. While nonlinear optical protocols are being developed to manipulate and probe valley selection rules, they largely rely on band-edge transitions that proceed via virtual intermediate states. Here, we demonstrate a doubly resonant cascaded nonlinear pathway from the valence band to high-lying states, mediated by a real intermediate state whose participation substantially reshapes the valley optical selection rules. Using time- and angle-resolved extreme-ultraviolet photoemission spectroscopy in combination with a time-dependent Lindblad master-equation formalism, we show that this cascaded nonlinear photoexcitation produces a substantially enhanced high-lying valley polarization compared to the conventional linear optical response near the band edge. The extension of the quantum-geometry-based selection rules to the nonlinear regime and high-lying bands offers new perspectives for ultrafast valleytronics and should play a determinant role in strong-field-driven phenomena in quantum materials.

cond-mat.mtrl-sci↗

arXiv2026

Dielectric Screening in Electromagnetic Dressing of Semiconductors

Nonequilibrium manipulation of quantum materials via electromagnetic dressing provides an on-demand route to tailoring electronic band structures through Floquet engineering. Time- and angle-resolved photoemission spectroscopy offers a direct means to probe these light-dressed electronic states. In such photoemission experiments, dressing can also occur for quasi-free electrons outside the material, giving rise to Volkov states. In certain cases, strong surface screening reduces the penetration of the driving field into the solid, resulting in Volkov contributions that dominate over Floquet ones. In this work, we systematically investigate the influence of materials' dielectric properties on Floquet-Volkov dressing of semiconductors, focusing on bulk layered van der Waals materials GeS, SnS, and 2H-WSe$_2$. First, by combining a simple model based on Fresnel equations with an electron-scattering description of Volkov amplitudes, we use polarization-dependent Volkov sideband intensities to extract a lower bound for the real part of the materials' dielectric functions, which typically lie between the reported dielectric constants for monolayer and bulk crystals. We demonstrate that increasing the fluence of the pump laser enables the generation of high-order Volkov sidebands which exhibit clear signatures of nonlinear light-matter interactions. Finally, we show that for our experimental geometry, the quasi-transparent nature of semiconductors in below-band-gap driving regime allows the optical pump to propagate within the sample and undergo multiple total internal reflections, producing temporally delayed Volkov replicas in pump-probe measurements via dressing of photoelectrons by evanescent fields. These systematic studies uncover previously unexplored aspects of Floquet-Volkov dressing in solids, highlighting the role of dielectric screening of the driving field.

cond-mat.mtrl-sci↗

arXiv2026

Electron-phonon-dominated charge-density-wave fluctuations in TiSe$_2$ accessed by ultrafast nonequilibrium dynamics

The complex phase diagram of 1T-TiSe2 consists of a charge density wave (CDW) below 200 K, and CDW fluctuations of still unknown origin at higher temperatures. Here, we use time-resolved extreme ultraviolet momentum microscopy and density functional perturbation theory to uncover the formation mechanism of CDW fluctuations and their spectral features at 295 K. We investigated the transient dynamics of fluctuations upon nonresonant ultrafast photoexcitation, and directly correlate it with the CDW soft-phonon hardening. Surprisingly, our results show that the coherent amplitude mode modulating ultrafast CDW recovery persists above TCDW, and reveal that CDW fluctuations are dominated by the electron-phonon interaction rather than excitonic correlations as commonly believed. Our findings on these microscopic CDW fluctuations clarify the complex interplay between electronic and lattice degrees of freedom at elevated temperatures and, therefore, could be useful in understanding the nature of the CDW phase transition in 1T-TiSe2 and similar quantum materials.

cond-mat.str-el↗

arXiv2025

Theory of Non-Dichroic Enantio-Sensitive Chiroptical Spectroscopy

We show that the photoelectron angular distributions produced by elliptical and cross-polarized two-color laser fields interacting with randomly oriented chiral molecules decompose into four irreducible representations of the $D_{2h}$ point group. One of these ($A_u$) corresponds to a non-dichroic enantiosensitive (NoDES) contribution. This NoDES contribution has opposite sign for opposite enantiomers but remains invariant under reversal of the field ellipticity, enabling chirality detection that is robust against variations of the relative phase between orthogonal field components. We propose a protocol to isolate this component using only two velocity-map imaging projections and validate it through numerical simulations. Our calculations, performed in the two-photon resonantly-enhanced ionization, multi-photon, and strong-field ionization regimes with cross-polarized two-color fields show that the NoDES signal reaches about 1\% of the energy-resolved ionization yield, comparable to photoelectron circular dichroism and much larger than standard magnetic-dipole chiroptical effects. NoDES spectroscopy thus provides a symmetry-protected and phase-robust route to probe molecular chirality on the ultrafast time scale. The experimental confirmation of our theory is presented in the companion paper [L. Fede et al., arXiv:2512.19062 (2025)].

physics.chem-ph↗

arXiv2025

Non-Dichroic Enantio-Sensitive Chiroptical Spectroscopy

Chiroptical effects using circularly polarized light produce signals that change sign when switching either molecular handedness (enantiosensitivity) or the light helicity (circular dichroism). Here, we break this enantiosensitive-and-dichroic paradigm by measuring a new type of chiroptical signal which is enantiosensitive but not dichroic. We photoionize chiral molecules using a strong laser field and detect the three-dimensional photoelectron momentum distribution. The non-dichroic, enantiosensitive asymmetry is encoded in octupolar and higher multipolar terms in the photoelectron angular distribution, which appear in multiphoton ionization with elliptically polarized fields or cross polarized two-color fields. The robustness of the enantiosensitivity with respect to the relative phase between the vectorial components of the ionizing field represents an example of symmetry protection, and opens unexplored opportunities for imaging ultrafast dynamics in chiral molecules, such as enantiosensitive photoelectron spectroscopy with bright squeezed vacuum states.

physics.chem-ph↗

arXiv2025

Excited States Band Mapping and Ultrafast Nonequilibrium Dynamics in Topological Dirac Semimetal 1T-ZrTe$_2$

We performed time- and polarization-resolved extreme ultraviolet momentum microscopy on topological Dirac semimetal candidate 1T-ZrTe$_2$. Excited states band mapping uncovers the previously inaccessible linear dispersion of the Dirac cone above the Fermi level. We study the orbital texture of bands using linear dichroism in photoelectron angular distributions. These observations provide hints on the topological character of 1T-ZrTe$_2$. Time-, energy- and momentum-resolved nonequilibrium carrier dynamics reveal that intra- and inter-band scattering processes play a capital role in the relaxation mechanism, leading to multivalley electron-hole accumulation near the Fermi level. We also show that electrons' inverse lifetime has a linear dependence on their binding energy. Our time- and polarization-resolved XUV photoemission results shed light on the excited state electronic structure of 1T-ZrTe$_2$ and provide valuable insights into the relatively unexplored field of quantum-state-resolved ultrafast dynamics in 3D topological Dirac semimetals.

cond-mat.mtrl-sci↗

arXiv2025

Time- and Polarization-Resolved Extreme Ultraviolet Momentum Microscopy

We report the development of an instrument combining an ultrafast, high-repetition-rate, polarization-tunable monochromatic extreme ultraviolet (XUV, 21.6 eV) beamline and a next-generation momentum microscope endstation. This setup enables time- and angle-resolved photoemission spectroscopy of quantum materials, offering multimodal photoemission dichroism capabilities. The momentum microscope simultaneously detects the full surface Brillouin zone over an extended binding energy range. It is equipped with advanced electron optics, including a new type of front lens that supports multiple operational modes. Enhanced spatial resolution is achieved by combining the small XUV beam footprint (33 $μ$m by 45 $μ$m) with the selection of small regions of interest using apertures positioned in the Gaussian plane of the momentum microscope. This instrument achieves an energy resolution of 44 meV and a temporal resolution of 144 fs. We demonstrate the capability to perform linear, Fourier, and circular dichroism in photoelectron angular distributions from photoexcited 2D materials. This functionality paves the way for time-, energy-, and momentum-resolved investigations of orbital and quantum geometrical properties underlying electronic structures of quantum materials driven out of equilibrium.

cond-mat.mtrl-sci↗

arXiv2025

Floquet-Bloch Valleytronics

Driving quantum materials out-of-equilibrium makes it possible to generate states of matter inaccessible through standard equilibrium tuning methods. Upon time-periodic coherent driving of electrons using electromagnetic fields, the emergence of Floquet-Bloch states enables the creation and control of exotic quantum phases. In transition metal dichalcogenides, broken inversion symmetry within each monolayer results in a non-zero Berry curvature at the K and K$^{\prime}$ valley extrema, giving rise to chiroptical selection rules that are fundamental to valleytronics. Here, we bridge the gap between these two concepts and introduce Floquet-Bloch valleytronics. Using time- and polarization-resolved extreme ultraviolet momentum microscopy combined with state-of-the-art ab initio theory, we demonstrate the formation of valley-polarized Floquet-Bloch states in 2H-WSe$_2$ upon below-bandgap coherent electron driving with chiral light pulses. We investigate quantum path interference between Floquet-Bloch and Volkov states, showing that this interferometric process depends on the valley pseudospin and light polarization-state. Conducting extreme ultraviolet photoemission circular dichroism in these nonequilibrium settings reveals the potential for controlling the orbital character of Floquet-engineered states. These findings link Floquet engineering and quantum geometric light-matter coupling in two-dimensional materials. They can serve as a guideline for reaching novel out-of-equilibrium phases of matter by dynamically breaking symmetries through coherent dressing of winding Bloch electrons with tailored light pulses.

cond-mat.mes-hall↗

arXiv2024

Strong-field ionization of chiral molecules with bicircular laser fields : sub-barrier dynamics, interference, and vortices

Strong-field ionization by counter-rotating two-color laser fields produces quantum interference between photoelectrons emitted on the leading and trailing edges of the laser field oscillations. We show that in chiral molecules, this interference is asymmetric along the light propagation direction and strongly enhances the sensitivity of the attoclock scheme to molecular chirality. Calculations in a toy-model molecule with a short-range chiral potential show that this enhanced sensitivity already emerges at the exit of the tunnel. We investigate the possible sources of chiral sensitivity in the tunneling process, and find that the interference between electron vortices plays a crucial role in the chiral response.

physics.atom-ph↗

arXiv2024

Capturing electron-driven chiral dynamics in UV-excited molecules

Molecular chirality is a key design property for many technologies including bioresponsive imaging, circularly polarized light detection and emission, molecular motors and switches. Imaging and manipulating the primary steps of transient chirality is therefore central for controlling numerous physical, chemical and biological properties that arise from chiral molecules in response to external stimuli. So far, the manifestation of electron-driven chiral dynamics in neutral molecules has not been demonstrated at their intrinsic timescale. Here, we use time-resolved photoelectron circular dichroism (TR-PECD) with an unprecedented instrument response function of 2.9 fs to image the dynamics of coherent electronic motion activated by prompt UV-excitation in neutral chiral molecules, disclosing its impact on the molecular chiral response. We find that electronic beatings between Rydberg states lead to periodic modulations of the chiroptical response on the few-femtosecond timescale, showing a sign inversion in less than 10 fs. Calculations including both the molecular UV-excitation and subsequent photoionization confirm this interpretation and provide further evidence that the combination of the resulting photoinduced chiral current with a circularly polarized probe pulse realizes an enantio-selective filter of molecular orientations upon photoionization, opening up a route towards enantio-selective charge-directed reactivity.

physics.chem-ph↗

arXiv2023

Role of Spin-Orbit Coupling in High-order Harmonic Generation Revealed by Super-Cycle Rydberg Trajectories

High-harmonic generation is typically thought of as a sub-laser-cycle process, with the electron's excursion in the continuum lasting a fraction of the optical cycle. However, it was recently suggested that long-lived Rydberg states can play a particularly important role in atoms driven by the combination of the counter-rotating circularly polarized fundamental light field and its second harmonic. Here we report direct experimental evidence of long and stable Rydberg trajectories contributing to high-harmonic generation. We confirm their effect on the harmonic emission via Time-Dependent Schr{ö}dinger Equation simulations and track their dynamics inside the laser pulse using the spin-orbit evolution in the ionic core, utilizing the spin-orbit Larmor clock. Our observations contrast sharply with the general view that long-lived Rydberg orbits should generate negligible contribution to the macroscopic far-field high harmonic response of the medium. Indeed, we show how and why radiation from such states can lead to well collimated macroscopic signal in the far field.

physics.atom-ph↗

arXiv2022

Ultrafast Polarization-Tunable Monochromatic Extreme Ultraviolet Source at High-Repetition-Rate

We report on the development of a high-order harmonic generation (HHG)-based ultrafast high-repetition-rate (250 kHz) monochromatic extreme ultraviolet (21.6 eV) source with polarization tunability, specifically designed for multi-modal dichroism in time- and angle-resolved photoemission spectroscopy. Driving HHG using an annular beam allows us to spatially separate the high-power 515 nm driving laser from the XUV beamlet while preserving the linear polarization axis angle tunability. This enables controlling the polarization state of the XUV radiation with a fixed all-reflective phase-shifter. This scheme leads to a source brightness of 5.7$\times$10$^{12}$ photons/s at 21.6 eV (up to 4$\times$10$^{11}$ photons/s on target) with ellipticities as high as 90$\%$.

physics.optics↗

arXiv2021

Photoionization of chiral molecules by counter-rotating bicircular laser fields: a chiral attoclock

Measuring and controlling the ionization dynamics by intense laser fields has recently led to important breakthroughs, from the investigation of tunneling time delays to attosecond molecular imaging by electron holography. In these experiments, extracting the subtle influence of the ionic potential on the departing electrons is of capital importance, and often challenging. Here we show that molecular chirality naturally provides a solution to this issue by breaking the symmetry of the photoionization process along the laser propagation direction. Using counter-rotating bicircular bichromatic laser fields, we produce two families of electrons with distinct ionization dynamics. Their overlap in momentum space results in quantum interferences, which are extremely sensitive to molecular chirality. The angular streaking of the electrons by the rotating laser field acts as an attoclock, encoding the ionization dynamics onto the electron ejection angle. Chirosensitive forward/backward asymmetries reveal the short and long spatial range influence of the ionic potential in the ionization process.

physics.atom-ph↗

arXiv2020

Bright, polarization-tunable high repetition rate extreme ultraviolet beamline for coincidence electron-ion imaging

After decades of supremacy of the Titanium:Sapphire technology, Ytterbium-based high-order harmonic sources are emerging as an interesting alternative for experiments requiring high flux of ultrashort extreme ultraviolet (XUV) radiation. In this article we describe a versatile experimental setup delivering XUV photons in the 10-50 eV range. The use of cascaded high-harmonic generation enables us to reach 1.8 mW of average power at 18 eV. Several spectral focusing schemes are presented, to select either a single harmonic or group of high-harmonics and thus an attosecond pulse train. In the perspective of circular dichroism experiments, we produce highly elliptical XUV radiation using resonant elliptical high-harmonic generation, and circularly polarized XUV by bichromatic bicircular high-harmonic generation. As a proof of principle experiment, we focus the XUV beam in a coincidence electron-ion imaging spectrometer, where we measure the photoelectron momentum angular distributions of xenon monomers and dimers.

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

Controlling Sub-Cycle Optical Chirality in the Photoionization of Chiral Molecules

Controlling the polarization state of electromagnetic radiation enables the investigation of fundamental symmetry properties of matter through chiroptical processes. Many strategies have been developed to reveal structural or dynamical information about chiral molecules, from the microwave to the extreme ultraviolet range. Most schemes employ circularly or elliptically polarized radiation, and more sophisticated configurations involve, for instance, light pulses with time-varying polarization states. In all these schemes, the polarization state of light is always considered as constant over one optical cycle. In this study, we zoom into the optical cycle in order to resolve and control a subcyle attosecond chiroptical process. We engineer an electric field whose instantaneous chirality can be controlled within the optical cycle, by combining two phase-locked orthogonally polarized fundamental and second harmonic fields. While the composite field has zero net ellipticity, it shows an instantaneous optical chirality which can be controlled via the two-color delay. We theoretically and experimentally investigate the photoionization of chiral molecules with this controlled chiral field. We find that electrons are preferentially ejected forward or backward relative to the laser propagation direction depending on the molecular handedness, similarly to the well-established photoelectron circular dichroism process. However, since the instantaneous chirality switches sign from one half cycle to the next, electrons ionized from two consecutive half cycles of the laser show opposite forward/backward asymmetries. This chiral signal provides a unique insight into the influence of instantaneous chirality in the dynamical photoionization process. Our results demonstrate the important role of sub-cycle polarization shaping of electric fields, as a new route to study and manipulate chiroptical processes.

physics.optics↗

arXiv2019

High-harmonics of harmonics of a fiber laser: a milliwatt XUV ultrashort source

Recent progresses in femtosecond ytterbium-doped fiber laser technology areopening new perspectives in strong field physics and attosecond science. Highorder harmonic generation from these systems is particularly interesting because it provides high flux beams of ultrashort extreme ultraviolet radiation. A lot of efforts have been devoted to optimize the macroscopic generation parameters. Here we investigate the possibility of enhancing the single-atom response by producing high-harmonics from the second, third and fourth harmonics of a turnkey Yb-fiber laser at 1030 nm. We show that the harmonic efficiency is optimal when the process is driven by the third harmonic, producing 4.4 1014 photon/s at 18 eV, which corresponds to 1.3 mW average power.

physics.optics↗