Search

Whereas most of the reports on the nonlinear properties of micro- and nanostructures address the generation of distinct signals, such as second or third harmonic, we recently demonstrated that the novel generation of dual output lasers developed for microscopy can readily increase the accessible parameter space and enable the simultaneous excitation and detection of multiple emission orders such as several harmonics and signals stemming from various sum and difference frequency mixing processes. [1] This rich response, which in our case features 10 distinct emissions and encompasses the whole spectral range from the deep ultraviolet to the short-wave infrared region, is demonstrated using various nonlinear oxide nanomaterials while being characterized and simulated temporally and spectrally.

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.

International audience; Whereas most of the reports on the nonlinear properties of micro- and nanostructures address the generation of distinct signals, such as second or third harmonic, here we demonstrate that the novel generation of dual output lasers recently developed for microscopy can readily increase the accessible parameter space and enable the simultaneous excitation and detection of multiple emission orders such as several harmonics and signals stemming from various sum and difference frequency mixing processes. This rich response, which in our case features 10 distinct emissions and encompasses the whole spectral range from the deep ultraviolet to the short-wave infrared region, is demonstrated using various nonlinear oxide nanomaterials while being characterized and simulated temporally and spectrally. Notably, we show that the response is conserved when the particles are embedded in biological media opening the way to novel biolabeling and phototriggering strategies.

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.

Femtosecond X-ray absorption spectroscopy (XAS) is a powerful method to investigate the dynamical behavior of a system after photoabsorption in real time. So far, the application of this technique has remained limited to large-scale facilities, such as femtosliced synchrotrons and free-electron lasers (FEL). In this work, we demonstrate femtosecond time-resolved soft-X-ray absorption spectroscopy of liquid samples by combining a sub-micrometer-thin flat liquid jet with a high-harmonic tabletop source covering the entire water-window range (284–538 eV). Our work represents the first extension of tabletop XAS to the oxygen edge of a chemical sample in the liquid phase. In the time domain, our measurements resolve the gradual appearance of absorption features below the carbon K-edge of ethanol and methanol during strong-field ionization and trace the valence-shell ionization dynamics of the liquid alcohols with a temporal resolution of ∼30 fs. This technique opens unique opportunities to study molecular dynamics of chemical systems in the liquid phase with elemental, orbital, and site sensitivity. ISSN:1948-7185

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.

We couple the full 3D ab initio quantum evolution of the light pulse polarization in interaction with an atom with a propagation model to simulate the propagation of ultrashort laser pulses over macroscopic dimensions, in the presence of self-generated harmonics up to order 11. We evidence a clear feedback of the generated harmonics on propagation, with an influence on the ionization probability as well as the yield of the harmonic generation itself., Comment: 9 pages, 4 figures

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 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.

We present high flux table-top 220eV HHG source (>109 photons/s/1% bandwidth) driven directly by a

Light can be used to modify and control properties of media, as in the case of electromagnetically induced transparency or, more recently, for the generation of slow light or bright coherent XUV and X-ray radiation. Particularly unusual states of matter can be created by light fields with strengths comparable to the Coulomb field that binds valence electrons in atoms, leading to nearly-free electrons oscillating in the laser field and yet still loosely bound to the core [1,2]. These are known as Kramers-Henneberger states [3], a specific example of laser-dressed states [2]. Here, we demonstrate that these states arise not only in isolated atoms [4,5], but also in rare gases, at and above atmospheric pressure, where they can act as a gain medium during laser filamentation. Using shaped laser pulses, gain in these states is achieved within just a few cycles of the guided field. The corresponding lasing emission is a signature of population inversion in these states and of their stability against ionization. Our work demonstrates that these unusual states of neutral atoms can be exploited to create a general ultrafast gain mechanism during laser filamentation., Comment: 9 pages, 4 figures, 10 pages supplementary material, 8 supplementary figures

Atmospheric clearness is a key issue for free space optical communications (FSO). We present the first active method to achieve FSO through clouds and fog, using ultrashort high intensity laser filaments. The laser filaments opto-mechanically expel the droplets out of the beam and create a cleared channel for transmitting high bit rate telecom data at 1.55 microns. The low energy required for the process allows considering applications to Earth-satellite FSO and secure ground based optical communication, with classical or quantum protocols., 4 pages + 2 pages supplementary text and movies

We present laser-induced condensation as a method for detecting of ultra-low concentrations of volatile organic compounds featuring a detection threshold well below 1 ppb. The method was tested in lab scale experiments and compared with quantitative photo-ionization detection measurements. The method was shown to be sensitive to the laser excitation wavelength between 1.6’2.0 um range.

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.

Light is used to modify or control properties in many quantum systems, leading to phenomena such as electromagnetically induced transparency, the generation of slow light or bright coherent XUV radiation. Using light fields, with strengths comparable to the Coulomb field which binds valence electrons in atoms, particularly unusual quantum states can be created which describe a nearly free electron oscillating in the laser field yet still loosely bound to the core1, 2. We demonstrate that such states can arise not only in isolated atoms3, but also in gases at a few atmospheric pressures, guiding intense laser pulses, where they can act as a gain medium. This gain is created within just a few cycles of the guided field. Using shaped pulses4 with 5–10 fs risetimes, we create pulse conditions, within a laser filament, where these states can persist, and we observe in the corresponding emission, the signatures of these states. This work demonstrates a general, new, ultrafast gain mechanism during filamentation, in which any driven atom can achieve inversion intra-pulse, using pulse shaping techniques.

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.

While propagating in transparent media, near-infrared multiterawatt (TW) laser beams break up in a multitude of filaments of typically 100-200 um diameter with peak intensities as high as 10 to 100 TW/cm^{2}. We observe a phase transition at incident beam intensities of 0.4 TW/cm^{2}, where the interaction between filaments induce solidlike two-dimensional crystals with a 2.7 mm lattice constant, independent of the initial beam diameter. Below 0.4 TW/cm^{2}, we evidence a mixed phase state in which some filaments are closely packed in localized clusters, nucleated on inhomogeneities (seeds) in the transverse intensity profile of the beam, and other are sparse with almost no interaction with their neighbors, similar to a gas. This analogy with a thermodynamic gas-solid phase transition is confirmed by calculating the interaction Hamiltonian between neighboring filaments, which takes into account the effect of diffraction, Kerr self-focusing, and plasma generation. The shape of the effective potential is close to a Morse potential with an equilibrium bond length close to the observed value.

In the quest for the next generation of imaging bio-markers, successful probes have to prove to be non toxic, bright, stable against long term excitation, and able to generate a sharp contrast against background fluorescence. Harmonics-generating Nanocrystals (HN) appeared recently as a novel labelling method with unprecedented wavelength flexibility, enabled by the non-resonant nature of the harmonics generation process. In particular, imaging using frequency doubling nanocrystals (i.e. nanodoublers), such as iron iodate, potassium niobate, barium ferrite (BFO) and KTP, has been demonstrated with laser sources in the near-infrared (800 nm) and infrared (1.55 μm) regions. The latter allows deeper penetration depth in tissues, thus especially promising for in vivo applications. The phase-coherent optical response of HN can also be exploited to fully characterize the excitation laser pulse in the focal spot of a high-NA objective with nanometric resolution.

We investigate the influence of ultrashort laser filaments on high-voltage discharges and spark-free unloading at various repetition rates and wind conditions. For electric fields well below, close to and above the threshold for discharges, we respectively observe remote spark-free unloading, discharge suppression, and discharge guiding. These effects rely on an indirect consequence of the thermal deposition, namely the fast dilution of the ions by the shockwave triggered by the filament at each laser shot. This dilution drastically limits recombination and increases the plasma channel conductivity that can still be non-negligible after tens or hundreds of milliseconds. As a result, the charge flow per pulse is higher at low repetition rates., Comment: 8 pages, 4 figures

We investigate the triggering and guiding of DC high-voltage discharges over a distance of 37 cm by filaments produced by ultraviolet (266 nm) laser pulses of 200 ps duration. The latter reduce the breakdown electric field by half and allow up to 80% discharge probability in an electric field of 920 kV/m. This high efficiency is not further increased by adding nanosecond pulses in the Joule range at 532 nm and 1064 nm. However, the latter statistically increases the guiding length, thereby accelerating the discharge by a factor of 2. This effect is due both to photodetachment and to the heating of the plasma channel, that increases the efficiency of avalanche ionization and reduces electron attachment and recombination., Comment: 12 pages, 6 figures

In the present review, laser fields are so strong that they become part of the electronic potential, and sometimes even dominate the Coulomb contribution. This manipulation of atomic potentials and of the associated states and bands finds fascinating applications in gases and solids, both in the bulk and at the surface. We present some recent spectacular examples obtained within the NCCR MUST in Switzerland., Structural Dynamics, 4 (6), ISSN:2329-7778

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 investigate the pulse partitioning of a 6.3 mJ, 450 fs pulse at 1030 nm to produce plasma channels. At such moderate energies, splitting the energy into several sub-pulses reduces the ionization efficiency and thus does not extend the plasma lifetime. We numerically show that when sufficient energy to produce multifilamentation is available, splitting the pulse temporally in a pulse train increases the gas temperature compared to a filament bundle of the same energy. This could improve the mean free path of the free electrons, therefore enhancing the efficiency of discharge triggering., Correcting typo in Eq. (12) and unit of $\beta_{ep}$ in Table I

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.

Study Type – Therapy (case series) Level of Evidence 4 OBJECTIVE • To assess the residual power delivered at the tip of a high-power (80 W) potassium-titanyl-phosphate (KTP) laser (80 W Green Light PVTM, Laserscope®; American Medical Systems, Minnetonka, MN, USA) at the end of a photoselective vaporization of the prostate (PVP) procedure, as well as the deflection angle of the laser beam. MATERIALS AND METHODS • In total, 65 laser fibres were collected at the end of PVP procedures indicated for symptomatic benign prostatic hyperplasia over a period of 17 months. PVP was performed by two senior urologists. • The power of laser beam at tip exit was measured for each fibre at the end of the procedures using a photodiode whose signal was amplified, and then quantified by a volt multimeter. • The deflection angle was measured using a graduated sphere. RESULTS • Approximately 70% of fibres delivered less than 40 W at the end of the procedure, which is less than the vaporization threshold. • Some 9% of fibres had lost their diffraction capacity with a significant alteration of laser beam angulation. These values were not operator dependent. CONCLUSIONS • The data show that a large proportion of laser fibers deliver a significantly underpowered beam at the end of the procedures. • This seems to be caused by peroperative destruction of the fibers, which results in a progressive loss of efficacy of PVP during procedures.

We studied the nonlinear optical properties of single layer graphene using high terahertz (THz) fields. With the use of a back gate and cooling down the sample to cryogenic temperatures we are able to spectrally probe the nonlinear THz properties of intrinsic to highly doped graphene. The carrier density strongly affects the nonlinear properties of graphene; in the low doping and high THz field regime, an increase of the transmission on the order of 4% is found in our experiments. At higher doping levels we observe a larger relative nonlinear response: the larger the doping in the single layer the larger the relative field induced increase in transmission becomes. In all experiments, the THz field is opposing the effect of the gate, but field effects are never larger than the doping effects. We use the thermodynamical model for a hot electron gas also used by Mics et al (2015 Nat. Commun.. 6 7655) to simulate our data and study the effects of doping on the nonlinear properties of single layer graphene. We find that the highest carrier temperatures are obtained in low doped graphene. The model shows a good qualitative agreement with our data for high doping levels. Nevertheless our results demonstrate the limitation of the model for low doping levels. Our results are a road map for further explorations for the control of nonlinear light-matter interaction and functionalization of graphene layers in active THz devices in which carrier temperature and saturable absorption play a role.

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

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

We measured the chemical composition and the size distribution of aerosols generated by femtosecond-Terawatt laser pulses in the atmosphere using an aerosol mass spectrometer (AMS). We show that nitric acid condenses in the form of ammonium nitrate and that oxidized volatile organics also contribute to particle growth. These two components account for two thirds and one third, respectively, of the dry laser-condensed mass. They appear in two different modes centred at 380 nm and 150 nm. The number concentration of particles between 25 and 300 nm increases by a factor of 15. Pre-existing water droplets strongly increase the oxidative properties of the laser-activated atmosphere, substantially enhancing the condensation of organics under laser illumination.

We show that multiple filamentation patterns in high-power laser beams, can be described by means of two statistical physics concepts, namely self-similarity of the patterns over two nested scales, and nearest-neighbor interactions of classical rotators. The resulting lattice spin model perfectly reproduces the evolution of intense laser pulses as simulated by the Non-Linear Schr\"odinger Equation, shedding a new light on multiple filamentation. As a side benefit, this approach drastically reduces the computing time by two orders of magnitude as compared to the standard simulation methods of laser filamentation., Comment: 8 pages, 4 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.

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.

The impact of nonadiabatic laser-induced molecular alignment on filamentation is numerically studied. Weak and strong field model of impulsive molecular alignment are compared in the context of nonlinear pulse propagation. It is shown that the widely used weak field model describing the refractive index modification induced by impulsive molecular alignment accurately reproduces the propagation dynamics providing that only a single pulse is involved during the experiment. On the contrary, it fails at reproducing the nonlinear propagation experienced by an intense laser pulse traveling in the wake of a second strong laser pulse. The discrepancy depends on the relative delay between the two pulses and is maximal for delays corresponding to half the rotational period of the molecule.

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.

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

A novel bio-photonics approach based on the nonlinear optical process of second harmonic generation by non-centrosymmetric nanoparticles is presented and demonstrated on malignant human cell lines. The proposed method allows to directly interact with DNA in absence of photosensitizing molecules, to enable independent imaging and therapeutic modalities switching between the two modes of operation by simply tuning the excitation laser wavelength, and to avoid any risk of spontaneous activation by any natural or artificial light source.