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-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. Express26, 26444 (2018)].

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. We find that these light springs can rotate as they excite the twisted plasma wakefield, providing a new mechanism to control the twisted wakefield phase velocity and enhance energy gain and trapping efficiency beyond planar wakefields.

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. The physical effects determining the field mode content of the twisted harmonic beams are elucidated.

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. These measurements are used to validate analytical models of the harmonic spatial phase in different generation regimes, and to benchmark ultrahigh-order Maxwell solvers of particle-in-cell simulation codes.

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.

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. These spatio-temporal "light springs" will allow for the transfer of the orbital angular momentum to matter by stimulated Raman scattering.

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. The generic phase correction procedure implemented here can also be extended to other fiber optic device applications sensitive to phase fluctuations.

Optically controlled solid-density transient plasma gratings.

A general approach for optically controlled spatial structuring of overdense plasmas generated at the surface of initially plain solid targets is presented. We demonstrate it experimentally by creating sinusoidal plasma gratings of adjustable spatial periodicity and depth, and study the interaction of these transient structures with an ultraintense laser pulse to establish their usability at relativistically high intensities. We then show how these gratings can be used as a "spatial ruler" to determine the source size of the high-order harmonic beams produced at the surface of an overdense plasma. These results open new directions both for the metrology of laser-plasma interactions and the emerging field of ultrahigh intensity plasmonics.

Spectral characterization of laser-driven solid-based high harmonics in the coherent wake emission regime.

Laser-produced surface high-harmonic generation is an attractive source of extreme ultraviolet radiation due to its coherent properties and high peak power. By operating at subrelativistic laser intensities in the coherent wake emission regime, the harmonic spectrum was experimentally studied versus laser properties. At higher laser intensities (>10(17) W/cm(2)) a higher spectral cutoff was observed, with accompanying blueshifting and spectral broadening of the individual orders. A model based on an expanding critical surface provides qualitative agreement with the observations.

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. We demonstrate experimentally the key influence of the steepness of the plasma-vacuum interface on the interaction, by measuring the spectral and spatial properties of harmonics generated on a plasma mirror whose initial density gradient scale length L is continuously varied. Time-resolved interferometry is used to separately measure this scale length.

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. The X(2)Σ(+) and A(2)Π states of CaO(-) are energetically separated by <1 eV such that the first excited state is close to the electronic ground state of neutral CaO and unstable with respect to electron detachment. Using the potential energy curves and the spin-orbit coupling terms, the vibronic energy levels of these ions have been determined. The ionization energy and the electron affinity of CaO are calculated at 6.79 and 0.79 eV, respectively. The photoelectron spectra of CaO(-) and CaO have also been simulated.

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. Here, we explore an alternative and more intuitive path, which makes it possible to reduce the equations of motion of particles to rather simple and well-known physical systems such as Kapitza and gravity pendulums. Starting from these simple systems, we first show how to estimate chaos thresholds by deriving a model of the stretching and folding dynamics of the pendulum bob in phase space. Based on this first model, we then derive a random walk model for particle dynamics above the chaos threshold, which can predict major features of stochastic heating for any EM polarization and angle θ_{i}.

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., in gases or dense plasmas) enables the production of attosecond lighthouses, i.e., sources emitting a collection of angularly well-separated light beams, each consisting of an isolated attosecond pulse. This general effect opens the way to a new generation of light sources, particularly suitable for attosecond pump-probe experiments, and provides a new tool for ultrafast metrology, for instance, giving direct access to fluctuations of the carrier-envelope relative phase of even the most intense ultrashort lasers.

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 â† 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. The procedure leads to a repulsive (2)Π state reaching the first dissociation limit, Zn((1)S(g)) + F((2)P(u)), and a bound one associated with the second limit, Zn((3)P(u)) + F((2)P(u)). The adiabatic electronic potentials and coupling functions have been determined at the multi-reference-configuration-interaction level of theory. The vibrational energies and the spin-orbit splittings are in agreement with early experimental data. The wavepacket propagation approach, coupled with a Prony analysis, allowed also to analyze the resonances and the bound vibronic states of the (2)Π manifold. The (2)Π â† X(2)Σ(+) vibronic spectra have been determined for Ω = 1/2 and 3/2 originating to the v'' = 0 level of the X(2)Σ(+) state.

Complete characterization of a plasma mirror for the production of high-contrast ultraintense laser pulses.

Improving the temporal contrast of ultrashort and ultraintense laser pulses is a major technical issue for high-field experiments. This can be achieved using a so-called "plasma mirror." We present a detailed experimental and theoretical study of the plasma mirror that allows us to quantitatively assess the performances of this system. Our experimental results include time-resolved measurements of the plasma mirror reflectivity, and of the phase distortions it induces on the reflected beam. Using an antireflection coated plate as a target, an improvement of the contrast ratio by more than two orders of magnitude can be achieved with a single plasma mirror. We demonstrate that this system is very robust against changes in the pulse fluence and imperfections of the beam spatial profile, which is essential for applications.

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. Unfortunately, the considerable pressures exerted by the laser can deform the mirror surface, unfavourably affecting the reflected beam and complicating, or even preventing, the use of plasma mirrors at ultrahigh intensities. Here we derive a simple analytical model of the basic physics involved in laser-induced deformation of a plasma mirror. We validate this model numerically and experimentally, and use it to show how such deformation might be mitigated by appropriate control of the laser phase.

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.

Coherent wake emission of high-order harmonics from overdense plasmas.

We present a new mechanism for high-order harmonic generation by reflection of a laser beam from an overdense plasma, efficient even at moderate laser intensities (down to Igamma2 approximately 4x10(15) W cm-2 microm2). In this mechanism, a transient phase matching between the electromagnetic field and plasma oscillations within a density gradient leads to the emission of harmonics up to the plasma frequency. These plasma oscillations are periodically excited in the wake of attosecond electron bunches which sweep across the density gradient. This process leads to a train of unevenly spaced chirped attosecond pulses and, hence, to broadened and chirped harmonics. This last effect is confirmed experimentally.

A theoretical spectroscopic study of HeI and HeBr.

Highly accurate potential energy functions for the HeI and HeBr molecules have been calculated using an ab initio treatment that included basis set extrapolation to the complete basis set, as well as spin-orbit coupling in the ground 2sigma+ and first 2pi excited doublet states. The rovibronic bound state energies and resonance lifetimes were also evaluated by a Prony analysis of the autocorrelation function of the evolving wave packet.