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We present a novel self-referenced method for the complete temporal characterization (phase and amplitude) of ultrashort optical laser pulses. The technique, called TIme-Gated Electric field Reconstruction (TIGER), measures a second-order nonlinear signal (namely, second harmonic generation or two-photon absorption) produced by four time-delayed replicas of the input pulse. The delays are spatially encoded in the beam profile using a four-faced pyramid-like optical element. The presented technique enables single shot measurement and does not require any spectral measurements, in contrast with well-known self-referenced characterization methods. Depending on the chosen geometry, the recorded TIGER signal can be either interferometric (i.e., carrier frequency resolved) or intensimetric. This paper describes the principle operation of the device together with a detailed theoretical analysis. TIGER measurements of various laser pulse shapes with their reconstructions are then presented demonstrating the relevance of this original approach., Comment: 10 pages, 14 figures

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

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.

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 employ nonlinear autocorrelation measurements to investigate plasmon-assisted hot carrier dynamics generated in optical gold antennas. We demonstrate that surface plasmons enable a nonlinear formation of hot carriers, providing thus a unique lever to optimize the energy distribution and generation efficiency of the photo-excited charges. The temporal response of the carriers' relaxation can be controlled within a range extending from 500~fs to 2.5~ps. By conducting a quantitative analysis of the dynamics, we determine the nonlinear absorption cross-section of individual optical antennas. As such, this work provides strong insights on the understanding of plasmon-induced hot carrier generation, especially in the view of applications where the time response plays a preponderant role.

Plasmonic dark modes are pure near-field resonances since their dipole moments are vanishing in far field. These modes are particularly interesting to enhance nonlinear light-matter interaction at the nanometer scale because radiative losses are mitigated therefore increasing the intrinsic lifetime of the resonances. However, the excitation of dark modes by standard far field approaches is generally inefficient because the symmetry of the electromagnetic near-field distribution has a poor overlap with the excitation field. Here, we demonstrate the selective optical excitation of bright and dark plasmonic modes of single gold nanorods by spatial phase-shaping the excitation beam. Using two-photon luminescence measurements, we unambiguously identify the symmetry and the order of the emitting modes and analyze their angular distribution by Fourier-space imaging.

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