B. Lavorel

Measurement of laser-induced alignment of molecules by cross defocusing.

The field-free alignment of CO2 produced in response to the excitation of a molecule by a high-intensity femtosecond pump pulse is measured with a simple coronography-like technique. The technique is based on the defocusing of a time-delayed probe pulse produced by the spatial distribution of aligned molecules. In the intensity regime explored here, the technique is shown to give valuable information about dynamic alignment. With the help of simulations, the degree of alignment is extracted from the data.

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.

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.

Dissipation of alignment in CO2 gas: A comparison between ab initio predictions and experiments

We present comparisons between measurements and ab initio calculations of the dissipation of the nonadiabatic laser-induced alignment in pure CO2 and CO2-He gas mixtures. The experiments were made for pressures between 2 and 20 bars at 295 K by using short non-resonant linearly polarized laser pulses for alignment and probe. The calculations are carried, free of any adjusted parameter, using refined intermolecular potentials and a requantized Classical Molecular Dynamics Simulations approach presented previously but not yet confronted to experiments. The results demonstrate that the model accurately reproduces the decays with time of both the transient revivals and permanent component of the alignment. The significant differences observed between the behaviors resulting from CO2-CO2 and CO2-He collisions are also well predicted by the model.

Collisional Raman linewidths of nitrogen at high temperature (1700–2400 K)

New high-temperature measurements of collisional linewidths of the Raman Q branch of nitrogen have been performed at 1700-2400 K with stimulated Raman spectroscopy in a tungsten filament. We fitted these data together with previous data obtained in the 295-1500-K range to redetermine the parameters of the relaxation models used in coherent anti-Stokes Raman spectroscopy thermometry. The improvement in the accuracy of the temperature measurement has been checked. Semiclassical calculations of linewidths in the 1700-2400-K range agree with the experimental data and have been extended to even higher temperatures.

Controlling molecular alignment rephasing through interference of Raman-induced rotational coherence

Quantum control over molecular alignment rephasing is experimentally investigated in gaseous CO2. The control process is achieved by illuminating the medium with a pair of pump-pulses separated in time by approximately an integer value of T0=1/8B0, where B0 is the rotational constant. Through a Raman-type process, each pulse alone produces rotational coherence leading to a periodic orientational anisotropy. It is the combination of the two pulses that yields to quantum interference, resulting in a modification of this anisotropy probed by a third delayed pulse. The effect is accurately analyzed for different time delays between the two pulses. A theoretical analysis supplies a clear understanding of the role played by the different rotational motions involved in the overall process. The relative orientation of the electric field vector for the two pulses is discussed in terms of an additional control parameter.

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.

Characterization of self-phase modulated ultrashort optical pulses by spectral phase interferometry

We present the procedure for measuring self-phase modulation of ultrashort laser pulses focused in gases by use of the spectral phase interferometry for direct electric-field reconstruction (SPIDER) technique. We tested the device, which employs a noncollinear type I frequency mixing scheme, by measuring the phase induced by group-velocity dispersion either in a piece of glass or in the compressor of the laser system. Both results were validated by comparison with the expected values. The phase that resulted from self-phase modulation in H2 gas or atmospheric air was then measured and compared with calculations based on a Gaussian beam assumption. A new estimate of the nonlinear index of refraction of H2 at 800 nm was deduced. The data recorded in atmospheric air are in good agreement with the reported value of the nonlinear index measured with spectral methods.

Shaping of a ground state rotational wavepacket by frequency-chirped pulses

A coherent rotational superposition state is produced in the ground vibronic level of N2 through the interaction of the molecule with the electric field vector of a nonresonant laser pulse. This rotational wavepacket is shaped with a linear frequency chirp of the laser field. The structural shape of the rotational coherences shows a strong dependence with the frequency-chirp amplitude. A comparison with a theoretical model allows the interpretation of the observed effects in terms of dephasing of the wavepacket induced by the laser phase distortion. Application of the presented results to the phase characterization of short XUV pulses is suggested.