E. Hertz

Measurement of high order Kerr refractive index of major air components

We measure the instantaneous electronic nonlinear refractive index of N(2), O(2) and Ar at room temperature for a 90 fs and 800 nm laser pulse. Measurements are calibrated by post-pulse molecular alignment through a polarization technique. At low intensity, quadratic coefficients n(2) are determined. At higher intensities, a strong negative contribution with a higher nonlinearity appears, which leads to an overall negative nonlinear Kerr refractive index in air above 26 TW/cm(2).

Measurement of high order Kerr refractive index of major air components: erratum

A clarification is missing concerning the high order Kerr non-linearities deduced from our experimental data published in [Opt. Express 17, 13429-13434 (2009)]. Here, we rectify this omission by making explicit the distinction between cross-Kerr and Kerr effects, and by extrapolating the value of the nonlinear refractive index for the last effect. Since the occurrence of sign inversion in the Kerr effect is not affected, the overall report in [Opt. Express 17, 13429-13434] remains valid.

Transition from Plasma-Driven to Kerr-Driven Laser Filamentation

While filaments are generally interpreted as a dynamic balance between Kerr focusing and plasma defocusing, the role of the higher-order Kerr effect (HOKE) is actively debated as a potentially dominant defocusing contribution to filament stabilization. In a pump-probe experiment supported by numerical simulations, we demonstrate the transition between two distinct filamentation regimes at 800 nm. For long pulses (1.2 ps), the plasma substantially contributes to filamentation, while this contribution vanishes for short pulses (70 fs). These results confirm the occurrence, in adequate conditions, of filamentation driven by the HOKE rather than by plasma.

Field-free two-direction alignment alternation of linear molecules by elliptic laser pulses.

We show that a linear molecule subjected to a short specific elliptically polarized laser field yields post-pulse revivals exhibiting alignment alternatively located along the orthogonal axis and the major axis of the ellipse. The effect is experimentally demonstrated by measuring the optical Kerr effect along two different axes. The conditions ensuring an optimal field-free alternation of high alignments along both directions are derived.

High-Field Quantum Calculation Reveals Time-Dependent Negative Kerr Contribution

The exact quantum time-dependent optical response of hydrogen under strong-field near-infrared excitation is investigated and compared to the perturbative model widely used for describing the effective atomic polarization induced by intense laser fields. By solving the full 3D time-dependent Schrödinger equation, we exhibit a supplementary, quasi-instantaneous defocusing contribution missing in the weak-field model of polarization. We show that this effect is far from being negligible, in particular when closures of ionization channels occur and stems from the interaction of electrons with their parent ions. It provides an interpretation of the higher-order Kerr effect recently observed in various gases.

On negative higher-order Kerr effect and filamentation

As a contribution to the ongoing controversy about the role of higher-order Kerr effect (HOKE) in laser filamentation, we first provide thorough details about the protocol that has been employed to infer the HOKE indices from the experiment. Next, we discuss potential sources of artifact in the experimental measurements of these terms and show that neither the value of the observed birefringence, nor its inversion, nor the intensity at which it is observed, appear to be flawed. Furthermore, we argue that, independently on our values, the principle of including HOKE is straightforward. Due to the different temporal and spectral dynamics, the respective efficiency of defocusing by the plasma and by the HOKE is expected to depend substantially on both incident wavelength and pulse duration. The discussion should therefore focus on defining the conditions where each filamentation regime dominates.

Spectral dependence of purely-Kerr-driven filamentation in air and argon

Based on numerical simulations, we show that higher-order nonlinear indices (up to n{sub 8} and n{sub 10}, respectively) of air and argon have a dominant contribution to both focusing and defocusing in the self-guiding of ultrashort laser pulses over most of the spectrum. Plasma generation and filamentation are therefore decoupled. As a consequence, ultraviolet wavelength may not be the optimal wavelength for applications requiring to maximize ionization.

Ultimate field-free molecular alignment by combined adiabatic-impulsive field design

We show that a laser pulse designed as an adiabatic ramp followed by a kick allows one to reach a perfect postpulse molecular alignment, free of saturation. The mechanism is based on an optimized distribution of the energy between a weakly efficient but non saturating adiabatic ramp and an efficient but saturating impulsive field. Unprecedent degrees of alignment are predicted using state-of-the-art pulse shaping techniques and non-destructive field intensities. The scheme can be extended to reach high degrees of orientation of polar molecules using designed half-cycle pulses.

Femtosecond polarization spectroscopy in molecular gas mixtures: Macroscopic interference and concentration measurements

Raman-induced polarization spectroscopy (RIPS) experiments combined with homodyne detection have been conducted with a femtosecond laser at room temperature and low pressure (p<2 atm) in CO2–N2 mixtures as well as in air (O2–N2 mixtures). Each molecule of the mixture produces its own time-dependent signal, measured as a series of recurring transients. Macroscopic interference is observed when transients of both molecules overlap in the time domain. This interference leads to a large modification of the signal, which is well reproduced by calculations. The total signal recorded in CO2–N2 or O2–N2 mixtures of known concentration is analyzed in order to measure the polarizability anisotropy ratio of the two components at 800 nm. The ratio measured in an O2–N2 (air) mixture is compared with values of previous works. The knowledge of the ratio for CO2/N2 allows us to determine the concentration of CO2–N2 unknown gas mixtures. The method is presented as a relevant technique for concentration measurements in the...

Towards the adaptive optimization of field-free molecular alignment

We theoretically report the optimization of field-free molecular alignment by spectral phase shaping of femtosecond laser pulses. Optimal pulse shapes are designed iteratively by an evolutionary algorithm in conjunction with a non-perturbative regime calculation. The investigation is conducted in O2 and N2 under realistic conditions of intensity, temperature and pulse shaping. We demonstrate that specific tailored pulses can provide significant maximization of field-free alignment compared to the Fourier transform limited pulses of the same energy. The underlying control mechanism is discussed. The effect of pulse energy and temperature is analysed leading to the identification of a general criteria for a successful optimization. Finally, the optimal spectral phase learned from the algorithm is rather smooth and can be described by a representation in terms of a sigmoidal function. We show that the use of a low-dimensional parametrization of the phase yields an efficient optimization of the alignment within a highly reduced convergence time.