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Manipulating at will the propagation dynamics of high power laser pulses is a long-standing dream whose accomplishment would lead to the control of fascinating physical phenomena emerging from laser-matter interaction. The present work represents a significant step towards such a control by manipulating the nonlinear optical response of the gas medium. This is accomplished by shaping an intense laser pulse experiencing filamentation at the subcycle level with a relatively weak (...) third-harmonic radiation. The control results from quantum interference between a single- and a two-color (mixing the fundamental frequency with its third-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. [ABSTRACT FROM AUTHOR]

Field-free molecular alignment has been used in order to track the collisional relaxation occurring in a molecular gas. CO2 molecules were initially irradiated by a short linearly polarized laser pulse resulting in the increase of their rotational energy. The evolution of the subsequent ultrafast relaxation process was optically probed after irradiating the sample with a second, weaker, short pulse leading to the alignment of the preheated molecules. Using classical molecular dynamic simulations, we were able to quantitatively reproduce the experimental shapes and amplitudes of the recorded revival transients for a time interval extending from 25 to 500 ps until thermalization of the gas sample is reached. [ABSTRACT FROM AUTHOR]

The analysis of negative birefringence optically induced in major air components [Loriot et al., Opt. Express 17, 13429 (2009); Loriot et al., Opt. Express 18, 3011 (2010)] is revisited in light of the recently reported plasma grating-induced phase-shift effect predicted for strong-field pump-probe experiments [Wahlstrand and Milchberg, Opt. Lett. 36, 3822 (2011)]. The nonlinear birefringence 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 nonoverlapping spectra. The interpretation 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 detection technique. The model also includes the ionization rate of argon and high-order Kerr indices introduced by Loriot et al., enabling one 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. [ABSTRACT FROM AUTHOR]

We experimentally investigate odd-order harmonic generation in molecular gases produced by circularly polarized laser fields. While forbidden in isotropic medium, this effect is allowed by symmetry breaking resulting from nonadiabatic laser-induced molecular alignment. The demonstration is provided by generating the third harmonic in CO2 molecules. Attractive properties and challenging potential applications are discussed in the context of higher-order harmonic generation. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

We report the experimental study of field-free molecular alignment in C02 gas mixtures induced by intense femtosecond laser pulses in the presence of collisional processes. We demonstrate that the alignment signals exhibit specific features due to nontrivial collisional propensity rules that tend to preserve the orientation of the rotational angular momentum of the molecules. The analysis is performed with a quantum approach based on the modeling of rotational J- and M-dependent state-to-state transfer rates. The present work paves the way for strong-field spectroscopy of collisional dynamics. [ABSTRACT FROM AUTHOR]

Permanent planar alignment of gas-phase linear molecules is achieved by a pair of delayed perpendicularly polarized short laser pulses. The experiment is performed in a supersonic jet, ensuring a relatively high number density of molecules with moderately low rotational temperature. The effect is optically probed on a femtosecond time scale by the use of a third short pulse, enabling a time-resolved birefringence detection performed successively in two perpendicular planes of the laboratory frame. The technique allows for an unambiguous estimation of the molecular planar delocalization produced within the polarization plane of the pulse pair after the turn-off of the field. The measurements are supported by numerical simulations which lead to the quantification of the observed effect and provide more physical insights into the phenomenon. [ABSTRACT FROM AUTHOR]

In this article, we derive the general exact solution of the modulation instability gain. The solution described here is valid for 1-D, 2-D, and 3-D cases considering any temporal response function of the medium and with possible higher order Kerr nonlinearities. In particular, we show that the gain induced by modulation instability is initial condition dependent, while the usual calculations do not lead to such a dependence. Applications for current and high-interest nonlinear propagation problems, such as 1-D optical fiber propagation with delayed Raman response and 2-D filamentation in gases, are investigated in detail. More specifically, we demonstrate that the 2-D model of filamentation based on the balance between higher order Kerr terms leads to a modulation instability window. The impact of both self-steepening and space-time defocusing effects is also highlighted. Finally, we discuss the influence of the finite-time response of the different order electronic Kerr effects on the growth of the expected modulation instability bands. [ABSTRACT FROM AUTHOR]

We present an observation of the rotational Doppler shift in the frequency of optical harmonic generated in fast rotating molecules. Conservation of energy and angular momentum in the light-molecule interaction suggests four different kinds of shifts depending on the mutual handedness of the circularly polarized fundamental and harmonic fields, as well as the handedness of the molecular rotation. All four types of the frequency shifts were observed in our experiments on third-harmonic generation in a gas of fast spinning O2 molecules. [ABSTRACT FROM AUTHOR]

We investigate experimentally and numerically the field-free orientation of the symmetric-top molecule of methyl iodide at high temperatures 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 good accuracy by numerical simulations. [ABSTRACT FROM AUTHOR]

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 multiples 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 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. [ABSTRACT FROM AUTHOR]