CARACTERISATION D'UN LASER Nd : YAG CONTINU A MODES COUPLES

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Imaging orbitals with attosecond and Ångström resolutions: toward attochemistry? Imaging orbitals with attosecond and Ångström resolutions: toward attochemistry?

International audienceThe recently developed attosecond light sources make the investigation of ultrafast processes in matter possible with unprecedented time resolution. It has been proposed that the very mechanism underlying the attosecond emission allows the imaging of valence orbitals with Ångström space resolution. This controversial idea together with the possibility of combining attosecond and Ångström resolutions in the same measurements has become a hot topic in strong-field science. Indeed , this could provide a new way to image the evolution of the molecular electron cloud during , e. g. a chemical reaction in ' real time '. Here we review both experimental and theoretical challenges raised by the implementation of these prospects. In particular , we show how the valence orbital structure is encoded in the spectral phase of the recombination dipole moment calculated for Coulomb scattering states , which allows a tomographic reconstruction of the orbital using first-order corrections to the plane-wave approach. The possibility of disentangling multi-channel contributions to the attosecond emission is discussed as well as the necessary compromise between the temporal and spatial resolutions. (Some figures may appear in colour only in the online journal

Photoionization time delays

International audienceThe material presented in this chapter is based on important advances realized in " attophysics " which make feasible to follow the motion of electrons in atoms and molecules with attosecond-level time resolution. In this context, time-delays have been recently determined in the process of photoionization by extreme-ultraviolet (xuv) pulses and the question of the significance of these measured delays arises. As we shall outline here, numerical experiments show that they are intimately related to the structure of the ionized species' continuous spectrum. Another point addressed here is that, in experiments, the measurements have the common characteristic to be performed in the presence of an auxiliary infra-red (IR) field, used to " clock " the timing of the process. This implies to adapt the theory treatment to handle such " two-color " photoionization processes. We review a systematic analysis of these features that are characteristic of this class of electronic transitions, when viewed in the time domain

Phase distortions of attosecond pulses produced by resonance-enhanced high harmonic generation

Resonant enhancement of high harmonic generation can be obtained in plasmas containing ions with strong radiative transitions resonant with harmonic orders. The mechanism for this enhancement is still debated. We perform the first temporal characterization of the attosecond emission from a tin plasma under near-resonant conditions for two different resonance detunings. We show that the resonance considerably changes the relative phase of neighbouring harmonics. For very small detunings, their phase locking may even be lost, evidencing strong phase distortions in the emission process and a modified attosecond structure. These features are well reproduced by our simulations, allowing their interpretation in terms of the phase of the recombination dipole moment

Optimisation of Quantum Trajectories Driven by Strong-field Waveforms

Quasi-free field-driven electron trajectories are a key element of strong-field dynamics. Upon recollision with the parent ion, the energy transferred from the field to the electron may be released as attosecond duration XUV emission in the process of high harmonic generation (HHG). The conventional sinusoidal driver fields set limitations on the maximum value of this energy transfer, and it has been predicted that this limit can be significantly exceeded by an appropriately ramped-up cycleshape. Here, we present an experimental realization of such cycle-shaped waveforms and demonstrate control of the HHG process on the single-atom quantum level via attosecond steering of the electron trajectories. With our optimized optical cycles, we boost the field-ionization launching the electron trajectories, increase the subsequent field-to-electron energy transfer, and reduce the trajectory duration. We demonstrate, in realistic experimental conditions, two orders of magnitude enhancement of the generated XUV flux together with an increased spectral cutoff. This application, which is only one example of what can be achieved with cycle-shaped high-field light-waves, has farreaching implications for attosecond spectroscopy and molecular self-probing

CEP-stable Tunable THz-Emission Originating from Laser-Waveform-Controlled Sub-Cycle Plasma-Electron Bursts

We study THz-emission from a plasma driven by an incommensurate-frequency two-colour laser field. A semi-classical transient electron current model is derived from a fully quantum-mechanical description of the emission process in terms of sub-cycle field-ionization followed by continuum-continuum electron transitions. For the experiment, a CEP-locked laser and a near-degenerate optical parametric amplifier are used to produce two-colour pulses that consist of the fundamental and its near-half frequency. By choosing two incommensurate frequencies, the frequency of the CEP-stable THz-emission can be continuously tuned into the mid-IR range. This measured frequency dependence of the THz-emission is found to be consistent with the semi-classical transient electron current model, similar to the Brunel mechanism of harmonic generation

Attosecond emission from chromium plasma

International audienceWe present the first measurement of the attosecond emission generated from underdense plasma produced on a solid target. We generate high-order harmonics of a femtosecond Ti:sapphire laser focused in a weakly ionized underdense chromium plasma. Using the " Reconstruction of Attosecond Beating by Interference of Two-photon Transitions " (RABITT) technique, we show that the 11 th to the 19 th harmonic orders form in the time domain an attosecond pulse train with each pulse having 300 as duration, which is only 1.05 times the theoretical Fourier transform limit. Measurements reveal a very low positive group delay dispersion of 4200 as 2. Beside its fundamental interest, high-order harmonic generation in plasma plumes could thus provide an intense source of attosecond pulses for applications

Spectrally resolved multi-channel contributions to the harmonic emission in N 2

International audienceWhen generated in molecules, high-order harmonics can be emitted through different ionization channels. The coherent and ultrafast electron dynamics occurring in the ion during the generation process is directly imprinted in the harmonic signal, i.e. in its amplitude and spectral phase. In aligned N2 molecules, we find evidence for a fast variation of this phase as a function of the harmonic order when varying the driving laser intensity. Basing our analysis on a three-step model, we find that this phase variation is a signature of transitions from a single- to a multi-channel regime. In particular, we show that significant nuclear dynamics may occur in the ionization channels on the attosecond timescale, affecting both the amplitude and the phase of the harmonic signal

Molecular orbital tomography from multi-channel harmonic emission in N2

International audienceHigh-order harmonic generation in aligned molecules can be used as an ultrafast probe of molecular structure and dynamics. By characterizing the emitted signal , one can retrieve information about electronic and nuclear dynamics occurring in the molecule at the attosecond timescale. In this paper , we discuss the theoretical and experimental aspects of molecular orbital tomography in N 2 and investigate the influence of multi-channel ionization on the orbital imaging. By analyzing the spectral phase of the harmonic emission as a function of the driving laser intensity , we address two distinct cases , which in principle allow the orbital reconstruction. First , the contributions from two molecular orbitals could be disentangled in the real and imaginary parts of the measured dipole , making it possible to reconstruct both orbitals. Second , by decreasing the driving laser intensity , the transition from a multi-channel to a single-channel ionization regime is shown. The highest occupied molecular orbital may then be selected as the only one contributing efficiently to the harmonic emission. The latter approach paves the way towards the generalization of tomography to more complex systems

Attosecond chirp-encoded dynamics of light nuclei Attosecond chirp-encoded dynamics of light nuclei

International audienceWe study the spectral phase of high-order harmonic emission as an observable for probing ultrafast nuclear dynamics after the ionization of a molecule. Using a strong-field approximation theory that includes nuclear dynamics, we relate the harmonic phase to the phase of the overlap integral of the nuclear wavefunctions of the initial neutral molecule and the molecular ion after an attosecond probe delay. We determine experimentally the group delay of the high harmonic emission from D 2 and H 2 molecules, which allows us to verify the relation between harmonic frequency and the attosecond delay. The small difference in the harmonic phase between H 2 and D 2 calculated theoretically is consistent with our experimental results