A. Ferré

Inhomogeneous high harmonic generation in krypton clusters.

High order harmonic generation from clusters is a controversial topic: conflicting theories exist, with different explanations for similar experimental observations. From an experimental point of view, separating the contributions from monomers and clusters is challenging. By performing a spectrally and spatially resolved study in a controlled mixture of clusters and monomers, we are able to isolate a region of the spectrum where the emission purely originates from clusters. Surprisingly, the emission from clusters is depolarized, which is the signature of statistical inhomogeneous emission from a low-density source. The harmonic response to laser ellipticity shows that this generation is produced by a new recollisional mechanism, which opens the way to future theoretical studies.

Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation

High-order harmonic generation in polyatomic molecules generally involves multiple channels of ionization. Their relative contribution can be strongly influenced by the presence of resonances, whose assignment remains a major challenge for high-harmonic spectroscopy. Here we present a multi-modal approach for the investigation of unaligned polyatomic molecules, using SF6 as an example. We combine methods from extreme-ultraviolet spectroscopy, above-threshold ionization and attosecond metrology. Fragment-resolved above-threshold ionization measurements reveal that strong-field ionization opens at least three channels. A shape resonance in one of them is found to dominate the signal in the 20–26 eV range. This resonance induces a phase jump in the harmonic emission, a switch in the polarization state and different dynamical responses to molecular vibrations. This study demonstrates a method for extending high-harmonic spectroscopy to polyatomic molecules, where complex attosecond dynamics are expected.

Universality of photoelectron circular dichroism in the photoionization of chiral molecules

Photoionization of chiral molecules by circularly polarized radiation gives rise to a strong forward/backward asymmetry in the photoelectron angular distribution, referred to as photoelectron circular dichroism (PECD). Here we show that PECD is a universal effect that reveals the inherent chirality of the target in all ionization regimes: single photon, multiphoton, above-threshold and tunnel ionization. These different regimes provide complementary spectroscopic information at electronic and vibrational levels. The universality of the PECD can be understood in terms of a classical picture of the ionizing process, in which electron scattering on the chiral potential under the influence of a circularly polarized electric field results in a strong forward/backward asymmetry.

High-harmonic transient grating spectroscopy of NO2 electronic relaxation.

We study theoretically and experimentally the electronic relaxation of NO(2) molecules excited by absorption of one ∼400 nm pump photon. Semiclassical simulations based on trajectory surface hopping calculations are performed. They predict fast oscillations of the electronic character around the intersection of the ground and first excited diabatic states. An experiment based on high-order harmonic transient grating spectroscopy reveals dynamics occurring on the same time scale. A systematic study of the detected transient is conducted to investigate the possible influence of the pump intensity, pump wavelength, and rotational temperature of the molecules. The quantitative agreement between measured and predicted dynamics shows that, in NO(2), high harmonic transient grating spectroscopy encodes vibrational dynamics underlying the electronic relaxation.

Two-Dimensional Frequency Resolved Optomolecular Gating of High-Order Harmonic Generation.

Probing electronic wave functions of polyatomic molecules is one of the major challenges in high-harmonic spectroscopy. The extremely nonlinear nature of the laser-molecule interaction couples the multiple degrees of freedom of the probed system. We combine two-dimensional control of the electron trajectories and vibrational control of the molecules to disentangle the two main steps in high-harmonic generation-ionization and recombination. We introduce a new measurement scheme, frequency-resolved optomolecular gating, which resolves the temporal amplitude and phase of the harmonic emission from excited molecules. Focusing on the study of vibrational motion in N_{2}O_{4}, we show that such advanced schemes provide a unique insight into the structural and dynamical properties of the underlying mechanism.

Combined high-harmonic interferometries for vectorial spectroscopy

We present a new method to characterize transverse vectorial light produced by high-harmonic generation (HHG). The incoherent sum of the two components of the electric field is measured using a bi-dimensional transient grating while one of the components is simultaneously characterized using two-source interferometry. The combination of these two interferometric setups enables the amplitude and phase measurement of the two vectorial components of the extreme ultraviolet radiation. We demonstrate the potential of this technique in the case of HHG in aligned nitrogen, revealing the vectorial properties of harmonics 9-17 of a Ti:sapphire laser.

Entropy production of a Rayleigh piston separating gases of different temperature

For thermodiffusion of polymers, it was shown that the transport coefficient has two contributions of different origins: first, dispersion forces between solvent and solute that grow it to cold areas, and secondly, a gradient of chemical potential of the solvent that acts as generalized force on the solute and promotes to hot areas. The competition of these opposite effects explains the variation with the molecular weight of polymer diffusion coefficient, which can change sign. As a toy model for this problem, we looked at the example of the Rayleigh piston: in a cylinder, a piston, assumed adiabatic (representing the solute as a macro particle without internal structure) fluctuates because of collisions with the two gases which it separates. Even if the pressures in the two semiinfinite reservoirs are equal, i.e., even if there is macroscopic equilibrium, when the temperatures are different, the system is out of equilibrium and acquires a nonzero average velocity, proportional to temperature gradient. The piston thus acts as a rectifier of fluctuations of Brownian motion. Therefore, there is a heat transfer between the two gases, causing a flow of entropy that we have calculated, together with the work of the ”generalized force”.

On the complex structures of spatially resolved XUV high-order-harmonic spectra

We study the far field spatial profiles of high order harmonics generated in gases with a high spectral resolution. It allows us to observe simultaneously several harmonics under diverse conditions including single shot imaging with spatio-spectral resolution at low and high intensities. This study gives access to the origin of the spatiospectral coupling appearing in the far field spatially resolved high-order-harmonic spectra.

Probing Ultrafast Molecular Chirality

We investigate the photoionization of chiral molecules in different ionization regimes : one photon-, multiphoton above threshold-, and tunnel-ionization. We use the photoelectron circular dichroism to track the ultrafast relaxation of a chiral molecule.