P. Béjot

From higher-order Kerr nonlinearities to quantitative modeling of third and fifth harmonic generation in argon

The recent measurement of negative higher-order Kerr effect (HOKE) terms in gases has given rise to a controversial debate, fed by its impact on short laser pulse propagation. By comparing the experimentally measured yield of the third and fifth harmonics, with both an analytical and a full comprehensive numerical propagation model, we confirm the absolute and relative values of the reported HOKE indices.

Molecular alignment and filamentation: Comparison between weak- and strong-field models

The impact of nonadiabatic laser-induced molecular alignment on filamentation is numerically studied. Weak and strong field model of impulsive molecular alignment are compared in the context of nonlinear pulse propagation. It is shown that the widely used weak field model describing the refractive index modification induced by impulsive molecular alignment accurately reproduces the propagation dynamics providing that only a single pulse is involved during the experiment. On the contrary, it fails at reproducing the nonlinear propagation experienced by an intense laser pulse traveling in the wake of a second strong laser pulse. The discrepancy depends on the relative delay between the two pulses and is maximal for delays corresponding to half the rotational period of the molecule.

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.

Coherent supercontinuum generation beyond 2.6 μm in all-normal dispersion silica microstructured fibers

Femtosecond pumping in an anomalous chromatic dispersion results in the generation of ultra-broad supercontinuum (SC) spectrum [1, 2]. However, such SC is associated with many pulses in the time domain and it is not flat in the spectral domain. Heidt et al. have shown that SC generated by pumping all-normal dispersion (ANDi) fiber is single pulse, has high coherence and spectral flatness [3-5]. Such all-normal dispersion supercontinuum is well suited for applications in an ultrafast spectroscopy. Mid-infrared SC is of particular interest since strong absorption lines of numerous chemical compounds are located in this spectral range. Unfortunately, long wavelength range of ANDi SC generated in silica microstructured fibers was limited so far to only 1.5 μm [4]. It means that full transparency window of silica glass was not covered. ANDi SC in mid-infrared was generated in more exotic glasses like soft-glass [6], ZBLAN-chalcogenide [7] and chalcogenide [8].

Revisiting interferences for measuring and optimizing optical nonlinearities

A method based on optical interferences for measuring optical nonlinearities is presented. In a proof-of-principle experiment, the technique is applied to the experimental determination of the intensity dependence of the photoionization process. It is shown that it can also be used to control and optimize the nonlinear process itself at constant input energy. The presented strategy leads to enhancements that can reach several orders of magnitude for highly nonlinear processes.