Quantum-Path-Resolved Attosecond High-Harmonic Spectroscopy.

Strong-field ionization of molecules releases electrons which can be accelerated and driven back to recombine with their parent ion, emitting high-order harmonics. This ionization also initiates attosecond electronic and vibrational dynamics in the ion, evolving during the electron travel in the continuum. Revealing this subcycle dynamics from the emitted radiation usually requires advanced theoretical modeling. We show that this can be avoided by resolving the emission from two families of electronic quantum paths in the generation process. The corresponding electrons have the same kinetic energy, and thus the same structural sensitivity, but differ by the travel time between ionization and recombination-the pump-probe delay in this attosecond self-probing scheme. We measure the harmonic amplitude and phase in aligned CO_{2} and N_{2} molecules and observe a strong influence of laser-induced dynamics on two characteristic spectroscopic features: a shape resonance and multichannel interference. This quantum-path-resolved spectroscopy thus opens wide prospects for the investigation of ultrafast ionic dynamics, such as charge migration.

High complexity femtosecond pulse duplicator.

This paper presents a theoretical and numerical study of a 0-π fan-out phase grating placed in the Fourier plane of a spatio-spectral pulse shaper followed by a spherical focusing lens. It is shown that this device acts as a high complexity femtosecond pulse duplicator designed for two source interferometry. At the focus of the lens, the electric field displays two spatially separated intense spots in which relative delay can be continuously tuned over 4 orders of magnitude, typically from a few attoseconds to a few tens of femtoseconds. Because the two pulses do not spatially overlap, their intensity remains unchanged when the relative delay is smaller than the pulse duration. Detailed simulations of the shaped electric field are presented.

High relative-phase precision beam duplicator for mid-infrared femtosecond pulses.

In this Letter, we use a 0-π square-wave phase grating to shape 1350 nm and 1450 nm femtosecond pulses and create two intense lobes at the focus of a lens. We show that the relative phase between these two lobes (the 1st and -1st orders of diffraction of the grating) is controlled very simply and precisely by shifting the position of the grating in its plane. We generate high harmonic orders from the two bright lobes and record the beating between the two emissions for each harmonic order up to the 53rd harmonic order.

Disentangling Spectral Phases of Interfering Autoionizing States from Attosecond Interferometric Measurements.

We have determined spectral phases of Ne autoionizing states from extreme ultraviolet and midinfrared attosecond interferometric measurements and ab initio full-electron time-dependent theoretical calculations in an energy interval where several of these states are coherently populated. The retrieved phases exhibit a complex behavior as a function of photon energy, which is the consequence of the interference between paths involving various resonances. In spite of this complexity, we show that phases for individual resonances can still be obtained from experiment by using an extension of the Fano model of atomic resonances. As simultaneous excitation of several resonances is a common scenario in many-electron systems, the present work paves the way to reconstruct electron wave packets coherently generated by attosecond pulses in systems larger than helium.

Tunable mid-infrared source of light carrying orbital angular momentum in the femtosecond regime.

We report on a tunable intense femtosecond mid-infrared (mid-IR) light source carrying orbital angular momentum (OAM). Our setup is based on an optical parametric amplification system with an 800 nm pump shaped with a spiral phase plate. We confirm the anisotropic OAM transfer from the pump to the idler through stimulated difference frequency generation by measuring the diffraction patterns of a triangular aperture illuminated by the signal, pump, and idler beams. The tunability of the setup is demonstrated by performing measurements at 3.0 and 3.6 µm idler wavelengths. This result provides a robust method of controlling OAM in strong field physics and designing secondary sources carrying OAM in the extreme ultraviolet spectral range through high-order harmonics generation.

High-order harmonic generations in intense MIR fields by cascade three-wave mixing in a fractal-poled LiNbO3 photonic crystal.

We report on the generation of harmonic-like photon upconversion in a LiNbO3-based nonlinear photonic crystal by mid-infrared (MIR) femtosecond laser pulses. We study below bandgap harmonics of various driver wavelengths, reaching up to the 11th order at 4 µm driver with 13% efficiency. We compare our results to numerical simulations based on two mechanisms: cascade three-wave mixing and non-perturbative harmonic generation, both of which include quasi-phase matching. The cascade model reproduces well the general features of the observed spectrum, including a plateau-like harmonic distribution and the observed efficiency. This has the potential for providing a source of tabletop few femtosecond ultraviolet pulses.

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.

Self-Probing Spectroscopy of the SF6 Molecule: A Study of the Spectral Amplitude and Phase of the High Harmonic Emission.

We present characterizations of the attosecond pulse train produced in the high harmonic generation (HHG) from SF6 molecules irradiated by a strong pulsed laser field at 800 nm. At harmonic order 17, we observe a minimum in the amplitude of the emitted spectrum and a corresponding distortion in the phase. Our experimental results are compared to two models: a multicenter interference model focused on the effect of the structure of the SF6 molecule in HHG and a model focused on the interferences between multiple ionization channels in HHG. We find that the experimental results agree very well with the multiple ionization channels model, illustrating that HHG in molecules can be very complex and that it provides insights of the intramolecular electron dynamics during the interaction process.