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Vision in living mice is sensitive to femtosecond pulse shaping., Vision is usually assumed to be sensitive to the light intensity and spectrum but not to its spectral phase. However, experiments performed on retinal proteins in solution showed that the first step of vision consists in an ultrafast photoisomerization that can be coherently controlled by shaping the phase of femtosecond laser pulses, especially in the multiphoton interaction regime. The link between these experiments in solution and the biological process allowing vision was not demonstrated. Here, we measure the electric signals fired from the retina of living mice upon femtosecond multipulse and single-pulse light stimulation. Our results show that the electrophysiological signaling is sensitive to the manipulation of the light excitation on a femtosecond time scale. The mechanism relies on multiple interactions with the light pulses close to the conical intersection, like pump-dump (photoisomerization interruption) and pump-repump (reverse isomerization) processes. This interpretation is supported both experimentally and by dynamics simulations.

High intensity laser filamentation in air has recently demonstrated that, through plasma generation and its associated shockwave, fog can be cleared around the beam, leaving an optically transparent path to transmit light. However, for practical applications like free-space optical communication (FSO), channels of multi-centimeter diameters over kilometer ranges are required, which is extremely challenging for a plasma based method. Here we report a radically different approach, based on quantum control. We demonstrate that fog clearing can also be achieved by producing molecular quantum wakes in air, and that neither plasma generation nor filamentation are required. The effect is clearly associated with the rephasing time of the rotational wave packet in N2.Pump excitation provided in the form of resonant trains of 8 pulses separated by the revival time are able to transmit optical data through fog with initial extinction as much as −6 dB.

International audience; Lightning is highly destructive due to its high power density and unpredictable character. Directing lightning away would allow to protect sensitive sites from its direct and indirect impacts (electromagnetic perturbations). Up to now, lasers have been unable to guide lightning efficiently since they were not offering simultaneously terawatt peak powers and kHz repetition rates. In the framework of the Laser Lightning Rod project, we develop a laser system for lightning control, with J-range pulses of 1ps duration at 1kHz. The project aims at investigating its propagation in the multiple filamentation regime and its ability to control high-voltage discharges. In particular, a field campaign at the S ̈antis mountain will assess the laser ability to trigger upward lightning.

We present space and time resolved measurements of the air hydrodynamics induced by femtosecond laser pulse excitation of the air gap between two electrodes at high potential difference. We explore both plasma-based and plasma-free gap excitation. The former uses the plasma left in the wake of femtosecond filamentation, while the latter exploits air heating by multiple-pulse resonant excitation of quantum molecular wavepackets. We find that the cumulative electrode-driven air density depression channel plays the dominant role in the gap evolution leading to breakdown. Femtosecond laser heating serves mainly to initiate the depression channel; the presence of filament plasma only augments the early heating.

International audience; We study the use of frequency upconversion schemes of near-IR picosecond laser pulses and compare their ability to guide and trigger electric discharges through filamentation in air. Upconversion, such as Second Harmonic Generation, is favorable for triggering electric discharges for given amount of available laser energy, even taking into account the losses inherent to frequency conversion. We focus on the practical question of optimizing the use of energy from a given available laser system and the potential advantage to use frequency conversion schemes.

In this paper we examine the spectral changes in a white light laser filament due to different pulse shapes generated by a pulse shaping setup. We particularly explore how the properties of the filament spectra can be controlled by parametrically tailored white light pulses. The experiments are carried out in a gas cell with up to 9 bar of argon. Plasma generation and self-phase modulation strongly affect the pulse in the spectral and temporal domain. By exploiting these effects we show that the pulse spectrum can be modified in a desired way by either using second order parametric chirp functions to shift the filament spectrum to higher or lower wavelengths, or by optimizing pulse shapes with a genetic algorithm to generate more complex filament spectra. This paper is one of the first examples of the application of complex, parametrically shaped white light pulses., 14 pages, 7 figures

We propose the impingement of non-uniform wavefront curvature as a simple way to improve the longitudinal homogeneity of the plasma density along filaments generated by ultrashort laser pulses. We characterize multiple filamentation of a multiterawatt beam with different wavefront curvatures applied to specific regions in the transverse beam profile. In adequate conditions, the filamenting region is more homogeneously ionized, in the longitudinal direction, than in the case of uniform focusing. Moreover, the ionization maximum is located between the middle and the two thirds of the filaments in all investigated chirps and focus configurations.

We experimentally and numerically characterize multiple filamentation of laser pulses with incident intensities of a few TW/cm2. Propagating 100 TW laser pulses over 42 m in air, we observe a new propagation regime where the filament density saturates. As also evidenced by numerical simulations in the same intensity range, the total number of filaments is governed by geometric constraints and mutual interactions among filaments rather than by the available power in the beam.

Optics Express, 26 (9), ISSN:1094-4087

Filamentation of ultra-short TW-class lasers recently opened new perspectives in atmospheric research. Laser filaments are self-sustained light structures of 0.1-1 mm in diameter, spanning over hundreds of meters in length, and producing a low density plasma (1015-1017 cm-3) along their path. They stem from the dynamic balance between Kerr self-focusing and defocusing by the self-generated plasma and/or non-linear polarization saturation. While non-linearly propagating in air, these filamentary structures produce a coherent supercontinuum (from 230 nm to 4 µm, for a 800 nm laser wavelength) by self-phase modulation (SPM), which can be used for remote 3D-monitoring of atmospheric components by Lidar (Light Detection and Ranging). However, due to their high intensity (1013-1014 W cm-2), they also modify the chemical composition of the air via photo-ionization and photo-dissociation of the molecules and aerosols present in the laser path. These unique properties were recently exploited for investigating the capability of modulating some key atmospheric processes, like lightning from thunderclouds, water vapor condensation, fog formation and dissipation, and light scattering (albedo) from high altitude clouds for radiative forcing management. Here we review recent spectacular advances in this context, achieved both in the laboratory and in the field, reveal their underlying mechanisms, and discuss the applicability of using these new non-linear photonic catalysts for real scale weather control.

Time-resolved spectroscopy at element-specific absorption edges provides a powerful tool to study ultrafast phenomena of matter on the atomic scale in the gas, solid or liquid phase. Combining element sensitivity of core-to-valence transitions due to the very localized initial core state and femtosecond/attosecond time resolution of new soft X-ray sources based on high-harmonic generation from long-wavelength drivers, accurate electronic and structural information is now accessible.

The quantum concepts of entanglement and interaction-free measurements are applied to spectroscopy to successfully sense carbon dioxide in air.

We characterized the white-light supercontinuum emission by a sub-petawatt laser system in the atmosphere via light detection and ranging measurements. As much as 1 J of supercontinuum is generated in the atmosphere, corresponding to a conversion efficiency of 30 %. This generation occurs at altitudes below 100 m. The high initial beam intensity results in the saturation of the number of self-guided filaments. Therefore, the “photon bath” surrounding the filaments strongly contributes to the white-light generation. These finding is well reproduced by numerical simulations based on the experimental parameters.

We evaluate the linearity of three electric measurement techniques of the initial electron density in laser filaments by comparing their results for a pair of filaments and for the sum of each individual filament. The conductivity measured between two plane electrodes in a longitudinal configuration is linear within 2% provided the electric field is kept below 100 kV/m. Furthermore, simulations show that the signal behaves like the amount of generated free electrons. The slow ionic current measured with plane electrodes in a parallel configuration is representative of the ionic charge available in the filament, after several $\mu$s, when the free electrons have recombined. It is linear within 2% with the amount of ions and is insensitive to misalignment. Finally, the fast polarization signal in the same configuration deviates from linearity by up to 80% and can only be considered as a semi-qualitative indication of the presence of charges, e.g., to characterize the filament length., Comment: 17 pages, 7 figures

Ultrashort intense lasers are able to efficiently condensate water vapor in air into droplets, even with mid-IR laser pulses. In addition, existing droplets can be expelled from the beam to transmit information through fog.

The electric conductivity, HV discharge triggering and guiding capabilities of filaments at 3.9 micrometer in air are investigated in the perspective of lightning control applications, and compared to near-IR filaments in identical conditions

We study the triggering of single filaments due to turbulence in the beam path for a laser of power below the filamenting threshold. Turbulence can act as a switch between the beam not filamenting and producing single filaments. This 'positive' effect of turbulence on the filament probability, combined with our observation of off-axis filaments suggests the underlying mechanism is modulation instability caused by transverse perturbations. We hereby experimentally explore the interaction of modulation instability and turbulence, commonly associated with multiple-filaments, in the single-filament regime., 5 pages, 6 figures

Intense laser illumination of cirrus-like ice particles increases the amount of condensed water and modifies the particles’ albedo., We investigate the interaction of ultrashort laser filaments with individual 90-μm ice particles, representative of cirrus particles. The ice particles fragment under laser illumination. By monitoring the evolution of the corresponding ice/vapor system at up to 140,000 frames per second over 30 ms, we conclude that a shockwave vaporization supersaturates the neighboring region relative to ice, allowing the nucleation and growth of new ice particles, supported by laser-induced plasma photochemistry. This process constitutes the first direct observation of filament-induced secondary ice multiplication, a process that strongly modifies the particle size distribution and, thus, the albedo of typical cirrus clouds.

We report on the first study of live cell opto-poration by single temporally shaped femtosecond laser pulses. Based on an ad hoc developed cell staining protocol, we demonstrate the influence of the pulse temporal profile on the efficiency of poration and on cell viability at four hours comparing the results obtained for four different temporal pulse shapes: positive and negative temporal Airy, positively chirped, and 30 fs bandwidth limited pulses. Each pulse has been tested on a thousand cells. The most suitable pulses for opto-poration are the positive Temporal Airy Pulses (TAP+), likely because they enhance avalanche ionization compared to bandwidth-limited shorter pulses. We discuss the results in the context of previous studies, highlighting the differences between single and multi-pulse opto-poration strategies.

We demonstrate that a driving ultrashort laser pulse undergoing filamentation can induce a remarkably large birefringence in Argon, resulting in an ultrafast “half-wave plate” for a copropagating non-filamenting probe beam. Such femtosecond birefringence, which originates from the difference between the nonlinear refractive indices induced by the filament on the axes parallel and orthogonal to its own polarization, opens the way to potential ultrafast Kerr-gates whose ultimate time-duration is only restricted by the duration of the driving pulse. We also show that the induced birefringence is transversely inhomogeneous, resulting from to the intensity profile of the driving pulse.

Modern laser sources nowadays deliver ultrashort light pulses reaching few cycles in duration, high energies beyond the Joule level and peak powers exceeding several terawatt (TW). When such pulses propagate through optically-transparent media, they first self-focus in space and grow in intensity, until they generate a tenuous plasma by photo-ionization. For free electron densities and beam intensities below their breakdown limits, these pulses evolve as self-guided objects, resulting from successive equilibria between the Kerr focusing process, the chromatic dispersion of the medium, and the defocusing action of the electron plasma. Discovered one decade ago, this self-channeling mechanism reveals a new physics, widely extending the frontiers of nonlinear optics. Implications include long-distance propagation of TW beams in the atmosphere, supercontinuum emission, pulse shortening as well as high-order harmonic generation. This review presents the landmarks of the 10-odd-year progress in this field. Particular emphasis is laid to the theoretical modeling of the propagation equations, whose physical ingredients are discussed from numerical simulations. Differences between femtosecond pulses propagating in gaseous or condensed materials are underlined. Attention is also paid to the multifilamentation instability of broad, powerful beams, breaking up the energy distribution into small-scale cells along the optical path. The robustness of the resulting filaments in adverse weathers, their large conical emission exploited for multipollutant remote sensing, nonlinear spectroscopy, and the possibility to guide electric discharges in air are finally addressed on the basis of experimental results., Comment: 50 pages, 38 figures

International audience; We have investigated nanocrystals of Fe(IO3)3 by polarization-sensitive second harmonic generation (SHG) microscopy. As the nonlinear optical properties of this material were only poorly characterized, we have first determined the relative values of the elements of its second-order susceptibility tensor, by the global fitting of the polarization-resolved SHG response of an ensemble of nanocrystals. This information allows one to optically retrieve the orientation of individual particles in the sample. The high SHG efficiency measured for nanocrystals of Fe(IO3)3 and their polar nature could make them very attractive for nonlinear microscopy of biological samples.

Intensity correlations and noise reduction are observed and characterized in the broadband supercontinuum generated by spatio-temporal solitons propagating in air, i.e., in filamentation of ultrashort laser pulses. Large correlations and reduction of the laser noise are observed already at the first steps of the filamentation process, while further propagation results in cascaded χ(3) broadening processes and yield complex correlation maps. The spectral range yielding an optimal laser noise reduction of 3.6 dB is found to cover 10 nm around the fundamental wavelength.

We investigate the interaction of narrow plasma channels formed in the filamentation of ultrashort laser pulses, with a DC high voltage. The laser filaments prevent electrical arcs by triggering corona that neutralize the high-voltage electrodes. This phenomenon, due to the electric field modulation and free electron release around the filament, opens new prospects to lightning and over-voltage mitigation., Comment: 15 pages, 6 figures

International audience; We report new experimental and numerical results on supercontinuum generation at ultraviolet/visible wavelengths produced by the propagation of infrared femtosecond laser pulses in air. Spectral broadening is shown to similarly affect single filaments over laboratory distance scales, as well as broad beams over long-range propagation distances. Numerical simulations display evidence of the crucial role of third harmonic generation in the build-up of UV-visible wavelengths, by comparison with current single-envelope models including chromatic dispersion and self-steepening.

We demonstrate laser induced ablation and plasma line emission from a metallic target at distances up to 180 m from the laser, using filaments (self-guided propagation structures ¨100 Am in diameter and ¨5 � 10 13 W/cm 2 in intensity) appearing as femtosecond and terawatt laser pulses propagating in air. The remarkable property of filaments to propagate over a long distance independently of the diffraction limit opens the frontier to long range operation of the laser-induced breakdown spectroscopy technique. We call this special configuration of remote laser-induced breakdown spectroscopy ‘‘remote filament-induced breakdown spectroscopy’’. Our results show main features of filament-induced ablation on the surface of a metallic sample and associated plasma emission. Our experimental data allow us to estimate requirements for the detection system needed for kilometer-range remote filament-induced breakdown spectroscopy experiment. D 2005 Elsevier B.V. All rights reserved.

A new ray-tracing scheme is proposed to simulate the non-linear propagation of ultra-short pulses. The results are in good agreement with experimental data and numerical solving of the non-linear Schrodinger equation in both the self-focusing and the filamentation regions. In particular, they indicate a major contribution of the ‘photon bath’ in the self-guided propagation of ultra-short pulses. The model suggests that a pure-Kerr self-guiding mode can allow filamentation without ionization.

Using a container-integrated mobile femtosecond terawatt laser system with integrated detection unit (Teramobile), we have demonstrated remote laser-induced breakdown spectroscopy (R-LIBS) on copper and aluminium samples with targets located at 25 m away from the container. The ability of our laser system to generate pulses in the femtosecond, picosecond and nanosecond regimes allowed us to perform direct comparisons between these three pulse durations. The dependence of the fluorescence signal on laser pulse energy showed a nonlinear behavior with a threshold, which is consistent with the previous observations for laser ablation. Such nonlinear behavior leads to a dependence of the LIBS signal on the temporal-spectral shape of the laser pulse. We showed especially that the transform-limited pulse does not optimize the fluorescence. A properly applied chirp allows an increase of the LIBS signal. Understanding and optimization of the chirp effect would improve the detection limit of the LIBS using a femtosecond laser (Femto-LIBS) and lead to a larger detection distance. Furthermore the use of pulse shaping should enhance the detection specificity for the cases of spectral overlapping between several elements to be identified.

Strong deformation of ultrashort laser pulse shapes is unavoidable when delivering high intensities at remote distances due to non-linear effects taking place while propagating. Relying on the reversibility of laser filamentation, we propose to explicitly design laser pulse shapes so that propagation serves as a non-linear field synthesizer at a remote target location. Such an approach allows, for instance, coherent control of molecules at a remote distance, in the context of standoff detection of pathogens or explosives., Comment: 17 pages, 6 figures

We have investigated, both theoretically and experimentally, multiphoton-induced processes in aerosol particles using femtosecond laser pulses. More specifically, we have demonstrated that both multiphoton (1, 2 and 3 photon)-induced fluorescence (MPEF) and laser-induced breakdown (LIB) emissions are strongly enhanced in the backward direction. The backward enhancement increases from 1.8 to 35 (emission ratio between the backward direction and 90°) with increasing non-linear process order n. Application to non-linear lidar of biological aerosols is discussed.

A correction in the transit time of electrons between the filaments and the electrodes leads us to reattribute the remote unloading to ions rather than to electrons. The experimental results reported in [Opt. Express23, 286407 (2015)] about remote electrical unloading and discharge suppression, as well as the analogy with the analogy with a supercorona, remain valid.

An unexpected blue-fluorescence band (around 420 nm) from both micrometer-sized dried particles and aqueous droplets of riboflavin [7,8-dimethyl-10-(D-1′-ribityl)-isoalloxazine] is observed when the microparticles are irradiated with a pulsed UV (355- or 351-nm) laser. The intensity of the band increases quadratically with input laser energy density (fluence) and is attributable to a one-photon-excited fluorescence of lumichrome (7,8-dimethyl-alloxazine) that is produced by photo-degradation of riboflavin. The well-known greenish-yellow fluorescence band (at 560 nm for dried particles and 535 nm for aqueous droplets) from riboflavin increases sublinearly with UV-laser fluence. With a laser input fluence above 5 J/cm2 the riboflavin fluorescence decays earlier and the lumichrome fluorescence reaches a maximum later than the peak of the input laser pulse. The temporal dynamics of the 420- and 535-nm fluorescence peaks are consistent with a rate-equation simulation of photon-induced conversion of riboflavin to lumichrome and the subsequent fluorescence of lumichrome.

We have observed the second harmonic generation from a single crystal LiNbO3 fiber with a diameter of 63 μm. Femtosecond laser pulses form a modelocked oscillator was focused perpendicularly onto the fiber. Scattered second harmonic was analyzed in polarization and the conversion efficiency was estimated. Comparing to a bulk nonlinear crystal, the striking feature of the SHG from the microcylinder is that the nonlinear conversion takes place out off phase-matching condition. For the fundamental at 850 nm the phase-mismatching is negative, even so, a relative important conversion efficiency of 3.7 × 10 -4 was obtained for incident 1.1-nJ and 150-fs pulses (peak intensity of 1.0 x 10 9 W/cm 2 ) This conversion efficiency, independent to the phase matching, should not exhibit the sharp variation as for a bulk crystal when the incident fundamental is tuned across the phase-matched wavelength. The fiber provides then a wide bandwidth doubler. We applied this microdoubler in a second order autocorrelator.

We present simulations of transient stimulated Raman scattering processes (SRS) for aerosol distributions with particles larger than the spatial extent of the ultrashort pump laser pulse. It is shown that this can constitute a new analysis method for transparent spherical aerosol particles, yielding simultaneously size and composition. For the first time, nonlinear treatment of the lidar equation is derived in the general case as well. Our calculations show that application of transient SRS lidar could yield simultaneous remote size and composition measurements of cloud or haze droplets without a priori hypothesis about the microdroplets.

Very efficient and stable laser operation of Ce 3+ -doped LiLuF 4 (Ce:LLF) single crystals longitudinally pumped with a Ce:LiSAF pulsed laser is demonstrated for the first time. At the peak operating wavelength of 308 nm, laser thresholds as low as 250 mJ cm −2 and laser slope efficiencies and output energies as high as 55% and 2 mJ, respectively, have been obtained at a pulse repetition rate of 20 Hz.

We investigate the reversibility of laser filamentation, a self-sustained, non-linear propagation regime including dissipation and time-retarded effects. We show that even losses related to ionization marginally affect the possibility of reverse propagating ultrashort pulses back to the initial conditions, although they make it prone to finite-distance blow-up susceptible to prevent backward propagation., Comment: 12 pages, 3 figures

The consideration of the higher-order Kerr effect (HOKE) drastically improves the quantitative agreement between measured and simulated harmonic yield as well as intensity and electron density in laser filaments generated by pulses below a few hundreds of fs. In longer pulses, the plasma defocusing plays a much more important role.

Narrow bandwidth operation within 250 MHz of a flashlamp-pumped Ti:Al 2 O 3 laser is successfully demonstrated with injection seeding from a CW laser diode. Seeding is shown sensitive even to very small injected power. Typically, 70% energy of a 100 mJ and 50 ns pulse is locked into the narrow bandwidth. This seeding efficiency is essentially limited in our experiments by the spatial hole burning in a laser rod with linearly polarized laser beam. It is also limited by mode mismatching between slave laser and seeding laser due to thermal effect on the laser rod induced by short and intense pumping flash.

We demonstrate laser control of high-voltage discharges over a gap of 1.2 m filled with a dense water cloud. Self-guided filaments generated by ultrashort laser pulses are transmitted through the cloud and ionize a continuous plasma channel. The cloud typically reduces the discharge probability in given experimental conditions by 30%, but has almost no influence on the threshold required to trigger single discharge events, both in electrical field and laser energy. This result is favorable for real-scale lightning control applications.

We observed the filamentation of mid-infrared ultrashort laser pulses (3.9 μm, 80 fs) in molecular gases. It efficiently generates a broadband supercontinuum over two octaves in the 2.5–6 μm spectral range, with a red-shift up to 500 nm due to the Raman effect, which dominates over the blue shift induced by self-steepening and the gas ionization. As a result, the conversion efficiency into the Stokes region (4.3–6 μm) 65% is demonstrated.

We present a novel optical aerosol particle detector based on Xe flash lamp excitation and spectrally resolved fluorescence acquisition. We demonstrate its performances on three natural pollens acquiring in real-time scattering intensity at two wavelengths, sub-microsecond time-resolved scattering traces of the particles’ passage in the focus, and UV-excited fluorescence spectra. We show that the device gives access to a rather specific detection of the bioaerosol particles.

We experimentally demonstrate that the transmission of a 1030~nm, 1.3~ps laser beam of 100 mJ energy through fog increases when its repetition rate increases to the kHz range. Due to the efficient energy deposition by the laser filaments in the air, a shockwave ejects the fog droplets from a substantial volume of the beam, at a moderate energy cost. This process opens prospects for applications requiring the transmission of laser beams through fogs and clouds., 11 pages, 5 figures

We present the first lidar/DIAL system based on an Ultra Violet (UV) vibronic laser. A Nd:YAG-pumped Ce:LiSAF laser has been developed for this purpose, providing high pulse energy (5 mJ at 10 Hz), very high slope efficiency (33%), and a tuning range from 284 to 299 nm. Simultaneous measurements of SO2 and O3 concentration profiles are presented using this frequency-agile Ce:LiSAF-based lidar system.

We show that spectral phase shaping of fs-laser pulses can be used to optimize laser-cell membrane interactions in water environment. The energy and peak intensity thresholds required for cell poration with single pulse in the nJ range can be significantly reduced (25% reduction in energy and 88% reduction in peak intensity) by using temporal Airy pulses, controlled by positive third order dispersion, as compared to bandwidth limited pulses. Temporal Airy pulses are also effective to control the morphology of the induced pores, with prospective applications from cellular to tissue opto-surgery and transfection.

We demonstrate that ultrashort and ultraintense light filaments survive their interaction with water droplets as large as 95 μm and that they are transmitted through water clouds having an optical thickness as high as 3.2 (transmission 5%). In contrast with linear optics, this remarkable transmission through optically dense media results from a dynamic energy balance between the quasisolitonic structure and the surrounding laser photon bath, which acts as an energy reservoir. Implications for free-space laser communications, remote sensing, and telemetry are discussed.

Optics Express, 20 (23), ISSN:1094-4087

We propose a new technique for efficient generation of 6 THz near-single-cycle transients though optical rectification of 800 nm fs laser pulses in a DAST/SiO 2 multilayer structure. The use of such a composite material allows to obtain phase-matching and control cascaded nonlinear processes.

We present a novel concept for optical spectroscopy called nonlinear correlation spectroscopy (NLCS). NLCS analyses coherent field fluctuations of the second and third harmonic light generated by diffusing nanoparticles. Particles based on noncentrosymmetric nonlinear materials such as KNbO(3) show a strong second as well as third harmonic response. The method and the theory are introduced and experimental NLCS results in fetal calf serum are presented showing the promising selectivity of this technique for measurement in complex biological environments.

We report the first (to our knowledge) experimental results and numerical simulations on mid-IR femtosecond pulse filamentation in argon using 0.1 TW peak-power, 80 fs, 3.9 μm pulses. A broadband supercontinuum spanning the spectral range from 350 nm to 5 μm is generated, whereby about 4% of the mid-IR pulse energy is converted into the 350-1700 nm spectral region. These mid-IR-visible coherent continua offer a new, unique tool for time-resolved spectroscopy based on a mid-IR filamentation laser source.