Interpretation of negative birefringence observed in strong-field optical pump-probe experiments: High-order Kerr and plasma grating effects

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…

Field-free molecular alignment for probing collisional relaxation dynamics

International audience; We report the experimental study of field-free molecular alignment in CO2 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.

Probing ultrafast thermalization with field-free molecular alignment

International audience; The rotation-translation thermalization of CO2 gas is investigated 500 ps after its preheating by a nonresonant short and intense laser pulse. The temperature of thermalization is optically determined with two additional short laser pulses enabling a field-free molecular alignment process and its probing, respectively. The measurements are performed for various intensities of the preheat pulse, leading to the observation of different temperatures which are in very good agreement with classical molecular dynamics simulations. The results can be regarded as a step towards real-time tracking of ultrafast relaxation pathways in molecular motion.

Transverse chemical interface detection with coherent anti-Stokes Raman scattering microscopy

International audience; Transverse "chemical" interfaces are revealed with a conventional two beam narrowband coherent anti-Stokes Raman scattering microscopy setup in a collinear configuration. The exciting "pump" and "Stokes" beams are focused on the sample in two opposite directions. The subtraction of the two generated anti-Stokes signals gives rise to a signal that is directly proportional to the pure Raman spectrum of the resonant medium. This property is used to highlight an interface between glass and N,N-dimethylformamide (DMF) and recover the pure Raman spectrum of DMF around its 1408 cm−1 vibrational band.

Background-free nonlinear Raman microscopy and spectroscopy at interfaces

Gaussian focused beams exhibit specific properties that drive the emitted fields in nonlinear optical microscopy. We discuss here how the basic field and object symmetry properties can be favorably used to obtain background-free images and spectra in third-order nonlinear optical processes. We concentrate here on coherent anti-Stokes Raman scattering (CARS), the non-linear analogue of Raman scattering. In CARS microscopy, the vibrational related (“resonant”) signal is often overwhelmed by an electronic related (“nonresonant”) background. Various strategies have been implemented to circumvent the undesirable effects of this nonresonant background: picosecond pulse excitation, time resolved, …

Fiber laser mode locked through an evolutionary algorithm

Mode locking of fiber lasers generally involves adjusting several control parameters, in connection with a wide range of accessible short-pulse dynamics. In this Letter, we experimentally demonstrate the ability of an evolutionary algorithm to prescribe a set of cavity parameters entailing specific self-starting mode locking. The prescribed parameters are applied to electrically driven polarization controllers, thus shaping the effective nonlinear transfer function at play within the fiber cavity. According to the specifications of the objective function used for the optimization procedure, various short-pulse regimes are obtained. Our versatile method represents an effective novel avenue f…

Méthode pour la détection d'un signal optique non linéaire résonant et dispositif pour la mise en œuvre de ladite méthode (II)

L'invention concerne une méthode et un dispositif pour détecter un signal optique non linéaire résonant induit dans un échantillon, l'échantillon comprenant un milieu résonant et un milieu non résonant formant une interface, le dispositif comprenant : - une source d'émission d'au moins un premier faisceau lumineux d'excitation du milieu résonant, dit faisceau pompe, à une première pulsation omega_p donnée, ledit faisceau pompe étant incident sur l'échantillon selon un axe optique, et interceptant l'échantillon à une position donnée d'une interface transverse entre le milieu résonant et non résonant, - un premier module optique de détection du signal optique non linéaire résultant de l'inter…

Optical kerr effect in the strong field regime

The optical Kerr response of hydrogen atom submitted to a strong and short near infrared laser pulse excitation is studied by solving the full 3D time-dependent Schro¨dinger equation. The nonlinear polarization evaluated at the driving field frequency is compared to the canonical expression derived from perturbation theory. A discrepancy between the two models is observed at large intensity affecting the nonlinear propagation of short and intense laser pulses.

Using molecular alignment to track ultrafast collisional relaxation

Field-free molecular alignment has been used in order to track the collisional relaxation occurring in a molecular gas. CO${}_{2}$ 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…

Echo-assisted impulsive alignment of room-temperature acetone molecules

International audience; We experimentally and theoretically investigate the field-free alignment of the asymmetric-top acetone molecule. Our study shows that the production of postpulse aligned molecules in a dense sample (0.05-0.2 bar) of room-temperature acetone using a single-pulse excitation can be significantly improved by rotational alignment echoes induced in a two-pulse excitation scheme. We report the observation of fractional echoes that can be used to reveal the nonlinearity of the molecular system. In a proof-of-principle experiment, a pre-aligned sample of acetone is also used for third-harmonic generation. The analysis of the experimental data with numerical simulations based …

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 ${\mathrm{CO}}_{2}$ molecules excited by a pair of femtosecond laser pulses.

Mid-infrared supercontinuum generation from 2 to 14 μm in various chalcogenide glasses optical fibers

Chalcogenide glasses optical fibers with step index or microstructured profiles are drawn from low toxicity compositions. Supercontinuum generation lead to an infrared spectrum spanning from 2 to 14µm with a 10µm core fiber of 40mm length.

Microscopie non-linéaire vibrationnelle CARS affranchie de bruit non-résonant aux interfaces

L'effet CARS (acronyme anglais de “coherent anti-Stokes Raman scattering”) est un analogue non-linéaire de l'effet Raman. A ce titre, il donne une information vibrationnelle sur l'échantillon étudié. Utilisé en microscopie, c'est une technique résolue chimiquement et qui permet de s'affranchir de marquage fluorescent. CARS est un processus de mélange à quatre ondes dans lequel deux faisceaux laser décalés en fréquence optique dénotés « pompe » et « Stokes » interagissent avec l'échantillon d'étude pour générer un signal dénoté « anti-Stokes » et décalé vers le bleu. Le signal anti-Stokes est la somme cohérente de deux composantes : une composante vibrationnelle, dite « résonante », générée …

Filament-induced visible-to-mid-IR supercontinuum in a ZnSe crystal: Towards multi-octave supercontinuum absorption spectroscopy

Abstract We report on the generation of multiple-octave supercontinuum laser source spanning from 0.5 μm to 11 μm induced by multi-filamentation in a ZnSe crystal. The generated supercontinuum is both spatially and spectrally characterized. It is then exploited in a proof-of-principle experiment for methane spectroscopy measurements by means of the supercontinuum absorption spectroscopy technique. The entire absorption spectrum is successfully recorded within the whole spectral bandwidth of the supercontinuum. Experimental results are in fairly good agreement with the HITRAN database, confirming the reliability and stability over several hours of the generated supercontinuum.

Molecular quantum interface for storing and manipulating ultrashort optical vortex

Light beams carrying orbital angular momentum (OAM) have become over the past few years a subject of widespread interest with unprecedented applications in various fields such as optical communication, super-resolution imaging, optical tweezers, or quantum processing. We demonstrate in the present work that gas-phase molecules can be used as a quantum interface to store an OAM carried by an ultrashort laser pulse. The interplay between spin angular momentum and OAM is exploited to encode the spatial phase information of light beams into rotational coherences of molecules. The embedded spatial structure is restored on-demand with a reading beam by taking advantage of field-free molecular ali…

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 ultraintense 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 analyzing full three-dimensional ab initio quantum calculations describing the microscopic atomic optical response, we have identified a fundamental mechanism resulting from interfere…

DEVICE AND METHOD FOR CHARACTERISING A FEMTOSECOND LASER PULSE

The invention relates to a device for characterising a laser pulse (Pu), comprising at least: - a Fresnel biprism (BPF) that separates an incident laser beam; a detector (CAM) comprising at least one linear semiconductor detector disposed in an overlap zone in which the separated beams interfere and generate a trace by absorption of two photons of at least two beams separated by the Fresnel biprism, said generated trace comprising information characterising the laser pulse (Pu); and a computer (K) that processes a signal from the detector (CAM), produced by the generation of the trace, in order to deduce therefrom a laser pulse duration.

Observation of laser-induced field-free permanent planar alignment of molecules

International audience; 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…

Microscopie CARS : état des lieux et perspectives

International audience

Filamentation-induced spectral broadening and pulse shortening of infrared pulses in Tellurite glass

Abstract Filamentation of infrared femtosecond pulses in Tellurite glass is reported, leading to the generation of a supercontinuum generation spanning from the visible up to 4 μm. The angular distribution of the supercontinuum shows clear evidence of conical waves generation, in particular, in the visible region. Moreover, taking advantage of the spatio-temporal self-focusing effect occurring in the Tellurite glass, a twofold pulse shortening is demonstrated. Tellurite glass appears as a very convenient, versatile and promising medium for femtosecond nonlinear optics in the infrared region.

Visualizing coherent molecular rotation in a gaseous medium

Inducing and controlling the ultrafast molecular rotational dynamics using shaped laser fields is essential in numerous applications. Several approaches exist that allow following the coherent molecular motion in real-time, including Coulomb explosion-based techniques and recovering molecular orientation from the angular distribution of high harmonics. We theoretically consider a non-intrusive optical scheme for visualizing the rotational dynamics in an anisotropic molecular gas. The proposed method allows determining the instantaneous orientation of the principal optical axes of the gas. The method is based on probing the sample using ultra-short circularly polarized laser pulses and recor…

Coherent Anti-Stokes Raman Scattering (CARS) in a microcavity

Optical Imaging of Coherent Molecular Rotors

International audience; Short laser pulses are widely used for controlling molecular rotational degrees of freedom and inducing molecular alignment, orientation, unidirectional rotation and other types of coherent rotational motion. To follow the ultra-fast rotational dynamics in real time, several techniques for producing molecular movies have been proposed based on the Coulomb explosion of rotating molecules, or recovering molecular orientation from the angular distribution of high-harmonics. The present work offers and demonstrates a novel non-destructive optical method for direct visualization and recording of movies of coherent rotational dynamics in a molecular gas. The technique is b…

Ultrafast collisional dissipation of symmetric-top molecules probed by rotational alignment echoes

We experimentally and theoretically investigate the ultrafast collisional dynamics of a symmetric-top molecule (${\mathrm{C}}_{2}{\mathrm{H}}_{6}$) in pure gas and mixtures with He at high density by employing the rotational alignment echo created by a pair of time-delayed intense laser kicks. The decrease of the amplitude of the echo when increasing the delay between the two laser pulses, reflecting the collisional relaxation of the system, is measured by probing the transient birefringence induced in the medium. The theoretical predictions, carried using purely classical molecular dynamics simulations, reproduce well the observed features, as demonstrated previously for a linear molecule.…

CHARACTERISATION OF A RADIATION PULSE BY TIME-RESOLVED OPTICAL WINDOWING

The invention relates to a system (10) for characterising a pulse (I) of electromagnetic radiation by time-resolved optical windowing, which comprises an device (1) for forming an interference which is suitable for superimposing four parts of the pulse. The system also comprises a matrix image sensor (3) which selectively captures an interference pattern formed by the pulse from two-photon absorptions. Said system allows the pulse shape to be obtained completely and accurately, and is particularly suitable for characterising ultrashort pulses. In various embodiments, the two-photon absorption can be produced in the matrix image sensor, or replaced by optical frequency doubling which is prod…

Rotational echoes as a tool for investigating ultrafast collisional dynamics of molecules

We show that recently discovered rotational echoes of molecules provide an efficient tool for studying collisional molecular dynamics in high-pressure gases. Our study demonstrates that rotational echoes enable the observation of extremely fast collisional dissipation, at timescales of the order of a few picoseconds, and possibly shorter. The decay of the rotational alignment echoes in ${\mathrm{CO}}_{2}$ gas and ${\mathrm{CO}}_{2}\text{\ensuremath{-}}\mathrm{He}$ mixture up to 50 bar was studied experimentally, delivering collision rates that are in good agreement with the theoretical expectations. The suggested measurement protocol may be used in other high-density media, and potentially …

Dissipation of post-pulse laser-induced alignment of CO2through collisions with Ar

In this paper, laser-induced field-free alignment of CO2 in mixtures with Ar is investigated under dissipative conditions (up to 15 bars) at room temperature. The degree of alignment is temporally monitored by a polarization spectroscopy technique, where a weak probe pulse measures the transient birefringence resulting from the alignment. The data are analyzed with a quantum mechanical density matrix formalism using properly J-dependent and M-dependent state-to-state transfer rates, which was previously successfully tested on pure CO2 and CO2–He mixtures. The same consistency is obtained between experiments and calculations, in particular the decay times of both the transient revivals and t…

Polarization shaping for unidirectional rotational motion of molecules.

Control of the orientation of the angular momentum of linear molecules is demonstrated by means of laser polarization shaping. For this purpose, we combine two orthogonally polarized and partially time-overlapped femtosecond laser pulses so as to produce a spinning linear polarization which in turn induces unidirectional rotation of N2 molecules. The evolution of the rotational response is probed by a third laser beam that can be either linearly or circularly polarized. The physical observable is the frequency shift imparted to the probe beam as a manifestation of the angular Doppler effect. Our experimental results are confirmed by theoretical computations, which allow one to gain a deep p…

Selective excitation of bright and dark plasmonic resonances of single gold nanorods.

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-p…

Direct temporal reconstruction of picosecond pulse by cross-correlation in semiconductor device

Cross-correlation measurements using the two-photon absorption process in a semiconductor is experimentally demonstrated for two pulses of different wavelengths (shifted by ~200 nm) and durations (20 times ratio). These measurements were found to be highly repeatable and fully suitable for the determination of the temporal intensity profile of picosecond (ps) pulses.

Molecular alignment echoes probe collision-induced rotational-speed changes

International audience; We show that the decays with pressure of the rotational alignment echoes induced in N 2 O-He gas mixtures by two ultrashort laser pulses with various delays show detailed information about collision-induced changes of the rotational speed of the molecules. Measurements and classical calculations consistently 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 narrowing of the filaments with time. The above mentioned variation of the echo decay then reflects the ability of collisi…