D. Descamps’s research while affiliated with Université Bordeaux-I and other places

• LIDT of Yb:YAG crystals with antireflection coatings is as high underwater as in air. • One sample exhibited higher LIDT underwater. • The LIDT reaches the Yb:YAG saturation intensity at room temperature. • Water permeation into the coating may lead to reduced field intensities on defects.

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.

We performed time- and polarization-resolved extreme ultraviolet momentum microscopy on the topological Dirac semimetal candidate 1T-ZrTe2. Excited state 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 about the topological character of 1T-ZrTe2. Time-, energy-, and momentum-resolved nonequilibrium carrier dynamics reveal that intra- and interband scattering processes play a major 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 as a function of their excess energy. Our time- and polarization-resolved XUV photoemission results shed light on the excited state electronic structure of 1T-ZrTe2 and provide valuable insights into the relatively unexplored field of quantum-state-resolved ultrafast dynamics in 3D topological Dirac semimetals.

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.

Strong-field ionization by counterrotating 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.

The performance of time-resolved photoelectron spectroscopy for the study of subpicosecond dynamics of laser-heated solids is often limited by space charge effects. The consequent shift and distortion of the photoelectron spectrum induced by electrons emitted by the ultrashort pump pulse is studied here using a fully coherent approach based on experimental measurements and space charge calculations. The temporal dynamics of the valence band of a copper sample is recorded before and after an 800 nm laser pump excitation at a fluence of 750mJ/cm2. The probe pulse is produced using a laboratory-based high-harmonics source delivering 25 fs pulses up to 100 eV photon energy. We extract the laser-heating contribution by comparing these measurements with space charge calculations based on particle-in-cell simulations of the pump and probe electron clouds mutual interaction on their way to the detector. The deduced picosecond dynamics associated to the electronic density of states shift is attributed to lattice changes with the help of hydrodynamic simulations including the two-temperature model.

Strong laser pulses enable probing molecules with their own electrons. The oscillating electric field tears electrons off a molecule, accelerates them, and drives them back toward their parent ion within a few femtoseconds. The electrons are then diffracted by the molecular potential, encoding its structure and dynamics with angstrom and attosecond resolutions. Using elliptically polarized laser pulses, we show that laser-induced electron diffraction is sensitive to the chirality of the target. The field selectively ionizes molecules of a given orientation and drives the electrons along different sets of trajectories, leading them to recollide from different directions. Depending on the handedness of the molecule, the electrons are preferentially diffracted forward or backward along the light propagation axis. This asymmetry, reaching several percent, can be reversed for electrons recolliding from two ends of the molecule. The chiral sensitivity of laser-induced electron diffraction opens a new path to resolve ultrafast chiral dynamics. Published by the American Physical Society 2024

We demonstrate nonlinear temporal compression of a vortex beam by propagation in a gas-filled capillary. Starting from an ytterbium-based laser delivering 700 μJ 640 fs pulses at a 100 kHz repetition rate, the vortex beam is generated using a spiral phase plate and coupled to a capillary where it excites a set of four modes that have an overlap integral of 97% with a Laguerre–Gauss LG10 mode. Nonlinear propagation of this hybrid, orbital angular momentum (OAM)-carrying mode results in temporal compression down to 74 fs at the output. Beam and pulse characterizations are carried out to determine the spatial profile and temporal duration of compressed pulses. This result in multimode nonlinear optics paves the way towards the generation of OAM-carrying few-cycle pulses, isolated attosecond XUV pulses, and tunable UV pulses through resonant dispersive wave emission.