Stéphane Petit

Ultra-broad bandwidth parametric amplification at degeneracy

We report on a novel approach of ultra-broad bandwidth parametric amplification around degeneracy. A bandwidth of up to 400 nm centered around 800 nm is amplified in a BBO crystal by using chirped pump pulses with a bandwitdth as broad as 10 nm. A supercontinuum signal is generated in a microstructured fiber, having to first order a quadratic chirp, which is necessary to ensure temporal overlap of the interacting waves over this broad bandwidth. Furthermore, we discuss the potential of this approach for an octave-spanning parametric amplification.

High-order harmonic generation at a megahertz-level repetition rate directly driven by an ytterbium-doped-fiber chirped-pulse amplification system.

We report the first experimental demonstration (to our knowledge) of high-order harmonic generation in rare gases driven by a state-of-the-art high-power Yb-doped-fiber chirped-pulse amplification system. The fiber laser delivers 270 fs pulses in the 30-100 microJ energy range at repetition rates varying from 100 kHz to 1 MHz. A proper focalization allows reaching several 10(13) W/cm2 in a gas jet. We have been able to produce and detect harmonics up to order 31 (33.2 nm) in Ar at a 100 kHz repetition rate. High-order harmonic generation at 1 MHz is also demonstrated in Xe up to harmonic 15. The demonstrated extreme UV (XUV) source will bring ultrashort XUV coincidence experiments from synchrotron facilities to tabletop laboratories.

Post-compression of high-energy femtosecond pulses using gas ionization

We present a new optical post-compression technique designed for high-energy ultrashort pulses. A large spectral broadening is achieved through rapid ionization of helium by an intense pulse (>10(15) W/cm(2)) propagating in a capillary filled with low-pressure helium. The blueshifted pulses are re-compressed with chirped mirrors and silica plates. From a terawatt Ti:sapphire laser chain providing pulses of 40 fs, 70 mJ, we demonstrate the compression of pulses down to 11.4 fs (FWHM) with a total output energy of 13.7 mJ.

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.

Relaxation Dynamics in Photoexcited Chiral Molecules Studied by Time-Resolved Photoelectron Circular Dichroism: Toward Chiral Femtochemistry

Unravelling the main initial dynamics responsible for chiral recognition is a key step in the understanding of many biological processes. However, this challenging task requires a sensitive enantiospecific probe to investigate molecular dynamics on their natural femtosecond time scale. Here we show that, in the gas phase, the ultrafast relaxation dynamics of photoexcited chiral molecules can be tracked by recording time-resolved photoelectron circular dichroism (TR-PECD) resulting from the photoionization by a circularly polarized probe pulse. A large forward–backward asymmetry along the probe propagation axis is observed in the photoelectron angular distribution. Its evolution with pump–probe delay reveals ultrafast dynamics that are inaccessible in the angle-integrated photoelectron spectrum or via the usual electron emission anisotropy parameter (β). PECD, which originates from the electron scattering in the chiral molecular potential, appears as a new sensitive observable for ultrafast molecular dynamics in chiral systems.

Phase characterization of the reflection on an extreme UV multilayer: comparison between attosecond metrology and standing wave measurements.

We characterize the phase shift induced by reflection on a multilayer mirror in the extreme UV range (80-93 eV) using two techniques: one based on high order harmonic generation and attosecond metrology (reconstruction of attosecond beating by interference of two-photon transitions), and a second based on synchrotron radiation and measurements of standing waves (total electron yield). We find an excellent agreement between the results from the two measurements and a flat group delay shift (±40 as) over the main reflectivity peak of the mirror.

Role of Excited States In High-order Harmonic Generation.

We investigate the role of excited states in high-order harmonic generation by studying the spectral, spatial, and temporal characteristics of the radiation produced near the ionization threshold of argon by few-cycle laser pulses. We show that the population of excited states can lead either to direct extreme ultraviolet emission through free induction decay or to the generation of high-order harmonics through ionization from these states and recombination to the ground state. By using the attosecond lighthouse technique, we demonstrate that the high-harmonic emission from excited states is temporally delayed by a few femtoseconds compared to the usual harmonics, leading to a strong nonadiabatic spectral redshift.

Role of the ionic potential in high harmonic generation.

Recollision processes provide direct insight into the structure and dynamics of electronic wave functions. However, the strength of the process sets its basic limitations--the interaction couples numerous degrees of freedom. In this Letter we decouple the basic steps of the process and resolve the role of the ionic potential which is at the heart of a broad range of strong field phenomena. Specifically, we measure high harmonic generation from argon atoms. By manipulating the polarization of the laser field we resolve the vectorial properties of the interaction. Our study shows that the ionic core plays a significant role in all steps of the interaction. In particular, Coulomb focusing induces an angular deflection of the electrons before recombination. A complete spatiospectral analysis reveals the influence of the potential on the spatiotemporal properties of the emitted light.

Ultra-wide parametric amplification at 800 nm toward octave spanning

We report on a significant improvement of the total bandwidth amplified in an optical parametric process. By pumping a parametric amplifier with a broadband pump, we demonstrate amplification of a supercontinuum whose spectrum expands over nearly an octave ranging from less than 600 nm up to 1200 nm. Our amplifier stage is set to provide amplification at degeneracy in the quasi-collinear configuration with a temporally as well as angularly dispersed pump.

Picosecond pulses of variable duration from a high-power passively mode-locked Nd:YVO 4 laser free of spatial hole burning

We report on a high-power passively mode-locked TEM(00)Nd:YVO(4) oscillator, 888 nm diode-pumped, with pulse durations adjustable between 46 ps and 12 ps. The duration tunability was obtained by varying the output coupler (OC) transmission while avoiding resorting to spatial hole burning (SHB) for pulse shortening. At a repetition rate of 91 MHz and for an output power ranging from 15 Wto45 W, we produced SHB-free 12-ps-to32-ps-long pulses. Within this range of power, these are the shortest pulse durations obtained directly from Nd:YVO(4) oscillators.