F. Billard

Nanosecond Z-scan measurements of the nonlinear refractive index of fused silica

We present the results of Z-scan studies carried out on fused silica at 1064nm and 532nm with two different nanosecond pulse durations. Such measurements in silica and in the nanosecond regime are possible thanks to a high sensitivity setting up of the Z-scan method and in-situ characterizations of the spatio-temporal parameters of the beam. Besides, with the use of a newly adapted numerical simulation only the calibration errors of the measurement devices are significant. In these conditions, we found a higher value of the nonlinear refractive index than in the femtosecond regime and we show that these values depend on pulse duration, which indicates the contribution of nanosecond mechanisms like electrostriction.

Orientation and Alignment Echoes

We present one of the simplest classical systems featuring the echo phenomenon-a collection of randomly oriented free rotors with dispersed rotational velocities. Following excitation by a pair of time-delayed impulsive kicks, the mean orientation or alignment of the ensemble exhibits multiple echoes and fractional echoes. We elucidate the mechanism of the echo formation by the kick-induced filamentation of phase space, and provide the first experimental demonstration of classical alignment echoes in a thermal gas of CO_{2} molecules excited by a pair of femtosecond laser pulses.

Harmonic Generation and Nonlinear Propagation: When Secondary Radiations Have Primary Consequences

In this Letter, it is experimentally and theoretically shown that weak odd harmonics generated during the propagation of an infrared ultrashort ultra-intense pulse unexpectedly modify the nonlinear properties of the medium and lead to a strong modification of the propagation dynamics. This result is in contrast with all current state-of-the-art propagation model predictions, in which secondary radiations, such as third harmonic, are expected to have a negligible action upon the fundamental pulse propagation. By analysing full three-dimensional ab initio quantum calculations describing the microscopic atomic optical response, we have identified a fundamental mechanism resulting from interferences between a direct ionization channel and a channel involving one single ultraviolet photon. This mechanism is responsible for wide refractive index modifications in relation with significant variation of the ionization rate. This work paves the way to the full physical understanding of the filamentation mechanism and could lead to unexplored phenomena, such as coherent control of the filamentation by harmonic seeding.

Observation of the field-free orientation of a symmetric-top molecule by terahertz laser pulses at high temperature

We investigate experimentally and numerically the field-free orientation of the symmetric top molecule of methyl-iodide at high temperature using a terahertz radiation generated by a plasma induced by a two-color laser beam. The degree of orientation is measured from the free-induction decay emitted by the sample. The observed experimental signal is reproduced with a good accuracy by numerical simulations.

Dissipation dynamics of field-free molecular alignment for symmetric-top molecules: Ethane (C2H6)

The field-free molecular alignment of symmetric-top molecules, ethane, induced by intense non-resonant linearly polarized femtosecond laser pulses is investigated experimentally in the presence of collisional relaxation. The dissipation dynamics of field-free molecular alignment are measured by the balanced detection of ultrafast molecular birefringence of ethane gas samples at high pressures. By separating the molecular alignment into the permanent alignment and the transient alignment, the decay time-constants of both components are quantified at the same pressure. It is observed that the permanent alignment always decays slower compared to the transient alignment within the measured pressure range. This demonstrates that the propensity of molecules to conserve the orientation of angular momentum during collisions, previously observed for linear species, is also applicable to symmetric-top molecules. The results of this work provide valuable information for further theoretical understanding of collisional relaxation within nonlinear polyatomic molecules, which are expected to present interesting and nontrivial features due to an extra rotational degree of freedom.

Subpicosecond Z-scan measurements of the nonlinear refractive index of dense materials

We present the results of Z-scan studies on a new setup in the sub-picosecond regime (central wavelength 800nm) carried out on solid and liquid materials such as pure water and silica. These measurements are made possible thanks to a high sensitivity setting up of our Z-scan method and in-situ characterizations of the spatio-temporal parameters of the beam. Besides, with the use of a newly adapted numerical simulation, only calibration errors of measurement devices are significant. These measurements are then used to separate the different contributions to the nonlinear refractive index from nanosecond scale mechanisms like electrostriction and/or thermal relaxation.

Resonantly enhanced filamentation in gases

In this Letter, a low-loss Kerr-driven optical filament in Krypton gas is experimentally reported in the ultraviolet. The experimental findings are supported by ab initio quantum calculations describing the atomic optical response. Higher-order Kerr effect induced by three-photon resonant transitions is identified as the underlying physical mechanism responsible for the intensity stabilization during the filamentation process, while ionization plays only a minor role. This result goes beyond the commonly-admitted paradigm of filamentation, in which ionization is a necessary condition of the filament intensity clamping. At resonance, it is also experimentally demonstrated that the filament length is greatly extended because of a strong decrease of the optical losses.

Polarized all-normal dispersion supercontinuum reaching 2.5 µm generated in a birefringent microstructured silica fiber

We demonstrate a polarized all-normal dispersion supercontinuum generated in a birefringent silica microstructured fiber spanning beyond 2.5 µm. To our knowledge, this is the spectra reaching the furthest in mid-infrared ever generated in normal dispersion silica fibers. The generation process was studied experimentally and numerically with 70 fs pump pulses operating at different wavelengths on short propagation distances of 48 mm and 122 mm. The all-normal operation was limited by the zero-dispersion wavelength at 2.56 µm and spectral broadening was stopped by OH absorption peak at 2.72 µm. We identified the asymmetry between propagation in both polarization axes and showed that pumping along a slow fiber axis is beneficial for a higher degree of polarization. Numerical simulations of the generation process conducted by solving the generalized nonlinear Schrödinger equation (NLSE) and coupled NLSEs system showed good agreement with experimental spectra.

Subcycle engineering of laser filamentation in gas by harmonic seeding

Manipulating at will the propagation dynamics of high power laser pulses is a long-standing dream whose accomplishment would lead to the control of a plethora of fascinating physical phenomena emerging from laser-matter interaction. The present work represents a significant step towards such an ideal control by manipulating the nonlinear optical properties of the gas medium at the quantum level. This is accomplished by engineering the intense laser pulse experiencing filamentation at the subcycle level with a relatively weak (about 1%) third-harmonic radiation. The control results from quantum interferences between a single and a two-color (mixing the fundamental frequency with its 3rd harmonic) ionization channel. This mechanism, which depends on the relative phase between the two electric fields, is responsible for wide refractive index modifications in relation with significant enhancement or suppression of the ionization rate. As a first application, we demonstrate the production and control of an axially modulated plasma channel that could be used for quasi-phase matched laser wakefield acceleration.

Interpretation of negative birefringence observed in strong-field optical pump-probe experiments: High-order Kerr and plasma grating effects

The analysis of negative birefringence optically induced in major air components (Loriot et al., [1, 2]) is revisited in light of the recently reported plasma grating-induced phase-shift effect predicted for strong field pump-probe experiments (Wahlstrand and Milchberg, [3]). The nonlinear birefrin- gence induced by a short and intense laser pulse in argon is measured by femtosecond time-resolved polarimetry. The experiments are performed with degenerate colors, where the pump and probe beam share the same spectrum, or with two different colors and non-overlapping spectra. The in- terpretation of the experimental results is substantiated using a numerical 3D+1 model accounting for nonlinear propagation effects, cross-beam geometry of the interacting laser pulses, and detec- tion technique. The model also includes the ionization rate of argon and high-order Kerr indices introduced by Loriot et al. enabling to assess the contribution of both terms to the observed effect. The results show that the ionization-induced phase-shift has a minor contribution compared to the high-order Kerr effect formerly introduced, the latter allowing a reasonably good reproduction of the experimental data for the present conditions.