Photon Pathways and the Nonperturbative Scaling Law of High Harmonic Generation.

High harmonic generation (HHG) has become a core pillar of attosecond science. Traditionally described with field-based models, HHG can also be viewed in a parametric picture, which predicts all properties of the emitted photons, but not the nonperturbative efficiency of the process. Driving HHG with two noncollinear beams and deriving analytically the corresponding yield scaling laws for any intensity ratio, we herein reconcile the two interpretations, introducing a generalized photonic description of HHG. It is in full agreement with field-based simulations and experimental data, opening the route to smart engineering of HHG with multiple driving beams.

Pulsewidth-switchable ultrafast source at 114 nm.

Femtosecond laser sources with high repetition rate in the ultraviolet (UV) and vacuum UV (VUV) are fundamental tools enabling tabletop time-resolved and angle-resolved photoemission spectroscopy in solids. We describe a VUV source at 114 nm (10.8 eV) based on an industrial grade ytterbium-doped ultrafast laser, a nonlinear pulse width selection stage, and two cascaded frequency tripling stages, first in crystals, second in xenon. The role of ionization in gas-based perturbative third harmonic generation phase-matching is analyzed using a simple theory, numerical simulations, and experimental data. The source features high photon flux, high repetition rate, and adjustable time resolutions. Thereby, in combination with a state-of-the-art angle-resolved photoemission spectroscopy (ARPES) apparatus it enables the study of the electronic dynamics of the whole Brillouin zone in a large number of materials.

Polarization spectroscopy of high-order harmonic generation in gallium arsenide.

An interesting property of high harmonic generation in solids is its laser polarization dependent nature which in turn provides information about the crystal and band structure of the generation medium. Here we report on the linear polarization dependence of high-order harmonic generation from a gallium arsenide crystal. Interestingly, we observe a significant evolution of the anisotropic response of above bandgap harmonics as a function of the laser intensity. We attribute this change to fundamental microscopic effects of the emission process comprising a competition between intraband and interband dynamics. This intensity dependence of the anisotropic nature of the generation process offers the possibility to drive and control the electron current along preferred directions of the crystal, and could serve as a switching technique in an integrated all-solid-state petahertz optoelectronic device.

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.

Evidence of depolarization and ellipticity of high harmonics driven by ultrashort bichromatic circularly polarized fields.

High harmonics generated by counter-rotating laser fields at the fundamental and second harmonic frequencies have raised important interest as a table-top source of circularly polarized ultrashort extreme-ultraviolet light. However, this emission has not yet been fully characterized: in particular it was assumed to be fully polarized, leading to an uncertainty on the effective harmonic ellipticity. Here we show, through simulations, that ultrashort driving fields and ultrafast medium ionization lead to a breaking of the dynamical symmetry of the interaction, and consequently to deviations from perfectly circular and fully polarized harmonics, already at the single-atom level. We perform the complete experimental characterization of the polarization state of high harmonics generated along that scheme, giving direct access to the ellipticity absolute value and sign, as well as the degree of polarization of individual harmonic orders. This study allows defining optimal generation conditions of fully circularly polarized harmonics for advanced studies of ultrafast dichroisms.

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.

Isolated attosecond pulses using a detuned second-harmonic field.

Calculations are presented for the generation of an isolated attosecond pulse in a multicycle two-color strong-field regime. We show that the recollision of the electron wave packet can be confined to half an optical cycle using pulses of up to 40 fs in duration. The scheme is proven to be efficient using two intense beams, one producing a strong field at omega and the other a strong field detuned from 2omega. The slight detuning deltaomega of the second harmonic is used to break the symmetry of the electric field over many optical cycles and provides a coherent control for the formation of an isolated attosecond pulse.

High-efficiency, simple setup for pulse cleaning at the millijoule level by nonlinear induced birefringence.

Nonlinear elliptical polarization rotation is used to improve the contrast of femtosecond pulses by several orders of magnitude. Using nonlinear induced birefringence in air, we produced cleaned pulses with an energy of a few hundreds of microjoules. This technique presents several major advantages, such as convenience and stability of the setup. We investigated the phase profile required for obtaining high-energy pulses. No phase distortion is observed, and the spatial quality of the beam is preserved.