Francois Legare

Francois Legare
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Francois Legare

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Physics - Optics (6)
Physics - Chemical Physics (2)
Physics - Atomic Physics (2)
Physics - Biological Physics (1)

Publications Authored By Francois Legare

We demonstrate temporal measurements of subpicosecond optical pulses via time-to-frequency conversion in a 45cm long CMOS compatible high index glass spiral waveguide. The measurements are based on efficient four wave mixing in the C-band, using around 1W of peak pump power. We achieve a resolution of 400fs over a time window of 100ps, representing a time-bandwidth product > 250. Read More

We present a novel time- and phase-resolved, background-free scheme to study the extreme ultraviolet dipole emission of a bound electronic wavepacket, without the use of any extreme ultraviolet exciting pulse. Using multiphoton transitions, we populate a superposition of quantum states which coherently emit extreme ultraviolet radiation through free induction decay. This emission is probed and controlled, both in amplitude and phase, by a time-delayed infrared femtosecond pulse. Read More

Unravelling the main initial dynamics responsible for chiral recognition is a key stepin the understanding of many biological processes. However this challenging task requires a sensitive enantiospecic probe to investigate molecular dynamics on their natural femtosecond timescale. Here we show that, in the gas phase, the ultrafast relaxationdynamics of photoexcited chiral molecules can be tracked by recording Time-ResolvedPhotoElectron Circular Dichroism (TR-PECD) resulting from the photoionisation bya circularly polarized probe pulse. Read More

We generate high-order harmonics of a mid-infrared laser from a silicon single crystal and find their origin in the recollision of coherently accelerated electrons with their holes, analogously to the atomic and molecular case, and to ZnO [Vampa et al., Nature 522, 462-464 (2015)], a direct bandgap material. Therefore indirect bandgap materials are shown to sustain the recollision process as well as direct bandgap materials. Read More

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 XUV 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. Read More

In the framework of linear optics, light fields do not interact with each other in a medium. Yet, when their field amplitude becomes comparable to the electron binding energies of matter, the nonlinear motion of these electrons emits new dipole radiation whose amplitude, frequency and phase differ from the incoming fields. Such high fields are typically achieved with ultra-short, femtosecond (1fs = 10-15 sec. Read More

The introduction of femto-chemistry has made it a primary goal to follow the nuclear and electronic evolution of a molecule in time and space as it undergoes a chemical reaction. Using Coulomb Explosion Imaging we have shot the first high-resolution molecular movie of a to and fro isomerization process in the acetylene cation. So far, this kind of phenomenon could only be observed using VUV light from a Free Electron Laser [Phys. Read More

We investigate the spatially and temporally resolved four-wave mixing of terahertz fields and optical pulses in large band-gap dielectrics, such as diamond. We show that it is possible to perform beam profiling and space-time resolved mapping of terahertz fields with sub-wavelength THz resolution by encoding the spatial information into an optical signal, which can then be recorded by a standard CCD camera. Read More

We report the imaging of tendon, a connective tissue rich in collagen type I proteins, with Interferometric Second Harmonic Generation (I-SHG) microscopy. We observed that the noncentrosymmetric structural organization can be maintained along the fibrillar axis over more than 150 {\mu}m, while in the transverse direction it is ~1-15 {\mu}m. Those results are explained by modeling tendon as a heterogeneous distribution of noncentrosymmetric nanocylinders (collagen fibrils) oriented along the fibrillar axis. Read More

Laser-induced ionization is a fundamental tool for the frequency conversion of lasers into spectral regions so far inaccessible, including both extreme ultraviolet and terahertz. The low-frequency currents induced by laser-driven ionization generate extremely broadband, single-cycle terahertz pulses, with applications ranging from remote sensing to optical pulse diagnostic, yet strong limitations arise from the low conversion efficiencies of this mechanism. We show a remarkable increase of the radiated terahertz energy with the laser wavelength and we relate this observation to the stronger action of long-wavelength fields on ionization-induced free-carriers. Read More