Stochastic heating of free electrons in multiple electromagnetic waves: A simple physical analysis.

It is established that charged particles crossing the interference field of two colliding electromagnetic (EM) waves can behave chaotically, leading to a stochastic heating of the particle distribution. A fine understanding of the stochastic heating process is crucial to the optimization of many physical applications requiring a high EM energy deposition to these charged particles. Predicting key stochastic heating features (particle distribution, chaos threshold) is usually achieved using a heavy Hamiltonian formalism required to model particle dynamics in chaotic regimes.

Survey of spatio-temporal couplings throughout high-power ultrashort lasers.

The investigation of spatio-temporal couplings (STCs) of broadband light beams is becoming a key topic for the optimization as well as applications of ultrashort laser systems. This calls for accurate measurements of STCs. Yet, it is only recently that such complete spatio-temporal or spatio-spectral characterization has become possible, and it has so far mostly been implemented at the output of the laser systems, where experiments take place.

Probing Strong-Field QED with Doppler-Boosted Petawatt-Class Lasers.

We propose a scheme to explore regimes of strong-field quantum electrodynamics (SF QED) otherwise unattainable with the currently available laser technology. The scheme relies on relativistic plasma mirrors curved by radiation pressure to boost the intensity of petawatt-class laser pulses by Doppler effect and focus them to extreme field intensities. We show that very clear SF QED signatures could be observed by placing a secondary target where the boosted beam is focused.

Spatio-temporal characterization of attosecond pulses from plasma mirrors.

Reaching light intensities above 10 W/cm and up to the Schwinger limit of the order of 10 W/cm would enable testing fundamental predictions of quantum electrodynamics. A promising - yet challenging - approach to achieve such extreme fields consists in reflecting a high-power femtosecond laser pulse off a curved relativistic mirror. This enhances the intensity of the reflected beam by simultaneously compressing it in time down to the attosecond range, and focusing it to sub-micrometre focal spots.

Spectrally resolved point-spread-function engineering using a complex medium.

Propagation of an ultrashort pulse of light through strongly scattering media generates an intricate spatio-spectral speckle that can be described by means of the multi-spectral transmission matrix (MSTM). In conjunction with a spatial light modulator, the MSTM enables the manipulation of the pulse leaving the medium; in particular focusing it at any desired spatial position and/or time. Here, we demonstrate how to engineer the point-spread-function of the focused beam both spatially and spectrally, from the measured MSTM.

Oxidation of Silver Cyanide Ag(CN) by the OH Radical: From Calculation to Molecular Simulation and to Experiment.

We investigate the oxidation of silver cyanide in water by the OH radical in order to compare this complex with the free cation Ag and to measure the influence of the ligands. High-level calculations of the model species enable the calibration of molecular simulations and the prediction of the oxidized species: and its absorption spectrum, with an intense band at 292 nm and a weaker one at 390 nm. Pulse radiolysis measurements of the oxidation of by the OH radical in water yields a transient species with a broad, intense band at 290 nm and a weaker band at 410 nm at short times after the pulse and a blue shift of the spectrum at longer times.

Spatio-spectral metrology at focus of ultrashort lasers: a phase-retrieval approach: erratum.

This is an erratum on the manuscript entitled 'Spatio-spectral metrology at focus of ultrashort lasers: a phase-retrieval approach', by A. Borot and F. Quéré [Opt.

Controlling the velocity of a femtosecond laser pulse using refractive lenses.

The combination of temporal chirp with a simple chromatic aberration known as longitudinal chromatism leads to extensive control over the velocity of laser intensity in the focal region of an ultrashort laser beam. We present the first implementation of this effect on a femtosecond laser. We demonstrate that by using a specially designed and characterized lens doublet to induce longitudinal chromatism, this velocity control can be implemented independent of the parameters of the focusing optic, thus allowing for great flexibility in experimental applications.

Spatio-spectral metrology at focus of ultrashort lasers: a phase-retrieval approach.

The complete characterization of an ultrashort laser beam ultimately requires the determination of its spatio-temporal electric field E(x, y, t), or its spatio-spectral counterpart Ẽ(x, y, ω). We describe a new measurement technique called INSIGHT, which determines Ẽ(x, y, ω), up to an unknown spatially-homogeneous spectral phase. Combining this information with a temporal measurement at a single point of the beam then enables the determination of the spatio-temporal field E(x, y, t).

Optical Control of the Topology of Laser-Plasma Accelerators.

We propose a twisted plasma accelerator capable of generating relativistic electron vortex beams with helical current profiles. The angular momentum of these vortex bunches is quantized, dominates their transverse motion, and results in spiraling particle trajectories around the twisted wakefield. We focus on a laser wakefield acceleration scenario, driven by a laser beam with a helical spatiotemporal intensity profile, also known as a light spring.

Different Time Scales in the Dissociation Dynamics of Core-Excited CF_{4} by Two Internal Clocks.

Fragmentation processes following C 1s→lowest unoccupied molecular orbital core excitations in CF_{4} have been analyzed on the ground of the angular distribution of the CF_{3}^{+} emitted fragments by means of Auger electron-photoion coincidences. Different time scales have been enlightened, which correspond to either ultrafast fragmentation, on the few-femtosecond scale, where the molecule has no time to rotate and the fragments are emitted according to the maintained orientation of the core-excited species, or dissociation after resonant Auger decay, where the molecule still keeps some memory of the excitation process before reassuming random orientation. Potential energy surfaces of the ground, core-excited, and final states have been calculated at the ab initio level, which show the dissociative nature of the neutral excited state, leading to ultrafast dissociation, as well as the also dissociative nature of some of the final ionic states reached after resonant Auger decay, yielding the same fragments on a much longer time scale.

Spatial Properties of High-Order Harmonic Beams from Plasma Mirrors: A Ptychographic Study.

Spatial properties of high-order harmonic beams produced by high-intensity laser-matter interactions carry rich information on the physics of the generation process, and their detailed understanding is essential for applications of these light beams. We present a thorough study of these properties in the case of harmonic generation from plasma mirrors, up to the relativistic interaction regime. In situ ptychographic measurements of the amplitude and phase spatial profiles of the different harmonic orders in the target plane are presented, as a function of the key interaction parameters.

Interaction of Ultraintense Laser Vortices with Plasma Mirrors.

Laser beams carrying orbital angular momentum (OAM) have found major applications in a variety of scientific fields, and their potential for ultrahigh-intensity laser-matter interactions has since recently been considered theoretically. We present an experiment where such beams interact with plasma mirrors up to laser intensities such that the motion of electrons in the laser field is relativistic. By measuring the spatial intensity and phase profiles of the high-order harmonics generated in the reflected beam, we obtain evidence for the helical wavefronts of the high-intensity laser at focus, and study the conservation of OAM in highly nonlinear optical processes at extreme laser intensities.

Spatio-temporal light springs: extended encoding of orbital angular momentum in ultrashort pulses.

We introduce a new class of spatio-temporally coupled ultrashort laser beams, which are obtained by superimposing Laguerre-Gauss beams whose azimuthal mode index is correlated to their frequency. These beams are characterized by helical structures for their phase and intensity profiles, which both encode the orbital angular momentum carried by the light. They can easily be engineered in the optical range, and are naturally produced at shorter wavelengths when attosecond pulses are generated by intense femtosecond Laguerre-Gauss laser beams.

Dual spectral-band interferometry for spatio-temporal characterization of high-power femtosecond lasers.

We present and demonstrate a technique called RED-SEA TADPOLE for the spatio-temporal characterization of high peak power femtosecond lasers. It retains the basic principle of an existing method, where a scanning monomode fiber is utilized in an interferometric scheme to measure the spectral amplitude and phase at all points across an ultrashort laser beam. We combine this approach with dual spectral-band interferometry, to correct for all phase errors occurring in this interferometer, thus allowing for the simultaneous measurement of the beam wavefront and pulse front in a collimated beam of large diameter.

Optical properties of relativistic plasma mirrors.

The advent of ultrahigh-power femtosecond lasers creates a need for an entirely new class of optical components based on plasmas. The most promising of these are known as plasma mirrors, formed when an intense femtosecond laser ionizes a solid surface. These mirrors specularly reflect the main part of a laser pulse and can be used as active optical elements to manipulate its temporal and spatial properties.

Theoretical investigations on CaO ions: vibronic states and photoelectron spectroscopy.

The low-lying electronic states, X(2)Π and A(2)Σ(+) of CaO(+) and X(2)Σ(+) and A(2)Π of CaO(-), have been determined at the MRCI+Q level of theory with the aug-cc-pV5Z(O) and cc-pCV5Z(Ca) basis sets. The two states of CaO(+) are close within <0.1 eV and coupled via spin-orbit effect.

Direct observation of density-gradient effects in harmonic generation from plasma mirrors.

High-order harmonics and attosecond pulses of light can be generated when ultraintense, ultrashort laser pulses reflect off a solid-density plasma with a sharp vacuum interface, i.e., a plasma mirror.

Theoretical study of the predissociation of the A2Π state of ZnF including quasi-diabatisation of the spin-orbit coupling.

The excited (2)Π electronic states of ZnF have been diabatized in order to simulate the (2)Π ← X(2)Σ(+) vibronic spectrum using a wavepacket propagation technique. The spin-orbit coupling functions within the (2)Π states and between the (2)Π and B(2)Σ(+) states have also been diabatized, as well as the dipole and transition moment functions. As the adiabatic electronic (2)Π states are strongly multi-configurational, the quasi-diabatisation scheme was based on the electronic wavefunction overlap along the reaction coordinate.

Attosecond lighthouses: how to use spatiotemporally coupled light fields to generate isolated attosecond pulses.

Under the effect of even simple optical components, the spatial properties of femtosecond laser beams can vary over the duration of the light pulse. We show how using such spatiotemporally coupled light fields in high harmonic generation experiments (e.g.

Full-dimensional quantum dynamics of vibrationally highly excited NHD2.

We report on full-dimensional vibrational quantum dynamics of the highly excited ammonia isotopologue NHD(2) using a newly developed potential energy surface and the MCTDH program package. The calculations allow to realistically simulate an infrared laser induced stereomutation reaction at the pyramidal nitrogen atom in the femtosecond time domain. Our results allow for a thorough qualitative and quantitative understanding of infrared photoinduced stereomutation kinetics, the underlying quantum dynamics, and the reaction mechanisms.

Phase properties of laser high-order harmonics generated on plasma mirrors.

As a high-intensity laser-pulse reflects on a plasma mirror, high-order harmonics of the incident frequency can be generated in the reflected beam. We present a numerical study of the phase properties of these individual harmonics, and demonstrate experimentally that they can be coherently controlled through the phase of the driving laser field. The harmonic intrinsic phase, resulting from the generation process, is directly related to the coherent sub-laser-cycle dynamics of plasma electrons, and thus constitutes a new experimental probe of these dynamics.