Search

Technological advances in femtosecond laser sources call for the development of increasingly refined characterization tools implying to enrich the existing panel of operable nonlinear interactions. The present paper describes a novel characterization method based on spectral-shearing interferometry which exploits the non-standard rotational Doppler effect for producing the frequency shear. This original approach, called DEER "Doppler Effect for Electric field Reconstruction", provides a spectral-shearing in the absence of frequency conversion and features multiple benefits as for instance the ability of operation in the ultraviolet spectral range or the characterization of ultra-broadband laser pulses., Comment: 7 pages, 3 figures

We show that the decays with pressure of the alignment echoes induced in N2O-He gas mixtures by two laser pulses with various delays bring detailed information on collision-induced changes of the rotational speed. Measurements and calculations demonstrate that collisions reduce the echo amplitude all the more efficiently when the echo appears late. We quantitatively explain this behavior by the filamentation of the classical rotational phase space induced by the first pulse and the progressive narrowing of the filaments with time. The variation of the echo decay thus reflects the ability of collisions to change the molecules' rotational speed by various amounts, enabling refined tests of models for the dissipation induced by intermolecular forces.

Energy transfer through quantum coherences plays an essential role in diverse natural phenomena and technological applications, such as human vision, light-harvesting complexes, quantum heat engines, and quantum information and computing. The understanding of the long-lived coherence involved in these phenomena requires a detailed modeling of the system-bath interactions beyond the so-called secular and/or Markovian approximations. Despite continuous theoretical progress on understanding nonsecular dynamics in the last decades, convincing experimental observations are still lacking. By using the laser-kicked molecular rotor as a model system, we here experimentally unveil the nonsecular dynamics in the rotational relaxation of molecules due to thermal collisions. Specifically, the rotational coherence in gas-phase molecules is systematically probed and characterized by the recently discovered rotational alignment echoes featuring a decoherence and dissipation process which can only be explained by the nonsecular quantum master equations for modeling molecular collisions.

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., Comment: 16 pages, 7 figures

We report the observation of fractional echoes in a double-pulse excited nonlinear system. Unlike standard echoes which appear periodically at delays which are integer multiple of the delay between the two exciting pulses, the fractional echoes appear at rational fractions of this delay. We discuss the mechanism leading to this phenomenon, and provide the first experimental demonstration of fractional echoes by measuring third harmonic generation in a thermal gas of CO2 molecules excited by a pair of femtosecond laser pulses.

We present what is probably the simplest classical system 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/alignment of the ensemble exhibits multiple echoes and fractional echoes. We elucidate the mechanism of the echo formation by 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.

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., Comment: 7 pages, 4 figures

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., Comment: 7 pages, 5 figures

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., Comment: 10 pages, 11 figures

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., Comment: 6 pages, 5 figures

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., Comment: 3 pages, 2 figures

We show that higher-order nonlinear indices ($n_4$, $n_6$, $n_8$, $n_{10}$) provide the main defocusing contribution to self-channeling of ultrashort laser pulses in air and Argon at 800 nm, in contrast with the previously accepted mechanism of filamentation where plasma was considered as the dominant defocusing process. Their consideration allows to reproduce experimentally observed intensities and plasma densities in self-guided filaments., Comment: 11 pages, 6 figures (11 panels)

Based on numerical simulations, we show that higher-order nonlinear indices (up to $n_8$ and $n_{10}$, 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 wavelengths for applications requiring to maximize ionization., Comment: 14 pages, 4 figures (14 panels)

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., Comment: 22 pages, 11 figures. Submitted to Laser physics as proceedings of the Laser Physics 2010 conference

An investigation of field-free molecular alignment produced by elliptically polarized laser pulses is reported. Experiments are conducted in CO$_2$ at room temperature. A non invasive all-optical technique, based on the cross defocusing of a probe pulse, is used to measure the alignment along two orthogonal directions that is sufficient to provide a 3 dimensional characterization. The field-free molecular alignment produced by a laser of elliptical polarization is in good agreement in terms of amplitude and shape with theoretical predictions. It turns out to be almost equivalent to the superposition of the effects that one would obtain with two individual cross-polarized pulses. The investigation highlights notably the occurrence of field-free two-direction alignment alternation for a suitably chosen degree of ellipticity. The analogy between this specific ellipticity and the well known "magic angle" used in time resolved spectroscopy to prevent rotational contributions is discussed., Comment: 6 pages, 4 figures

We show that a linear molecule subjected to a short specific elliptically polarized laser field yields postpulse 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., Comment: 5 pages, 4 color figures

Self- and argon-broadening coefficients are reported for a number of Raman Q-branch transitions in the nu(1) and nu(2) + nu(4) bands of (C-12)D4 at room temperature (296 K). The coefficients display a variation with j and with C exp n (symmetry species A, E, F) that is essentially independent of collision partner and which is similar to the j- and C exp n-dependence found in previous measurements of the IR line-broadening coefficients. The rotationally inelastic collision rates previously measured by Foy et al. (1988) for (C-13)D4 (V4 = 0, 1) in collision with (C-13)D4 or Ar account for only a part of the Raman broadening rate, suggesting possibly significant contributions to the linewidths from efficient V-V transfer or elastic dephasing collisions.

Self-, argon-, and helium-broadening coefficients have been measured for 13 lines in the 2nu2 Raman Q branch of CH4 using stimulated inverse Raman spectroscopy. The linewidths clearly show the symmetry-state dependence characteristic of pressure broadening, and inelastic processes in general, involving spherical-top molecules. Pressure-induced line shifts have also been measured for these features in pure methane. The pressure-shift coefficients do not display the symmetry-state dependence found for the linewidths. By applying the Rosenkranz perturbation treatment to a pair of collisionally mixed lines, an estimate of individual state-to-state contributions to the overall linewidth has been obtained.