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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.

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.

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.

We demonstrate the simultaneous generation of more than four harmonics from individual dielectric nanoparticles excited by a telecom fiber laser at 1560. We discuss the possibility to control their relative intensities by the laser polarization.

We use Hyper Rayleigh Scattering and polarization resolved multiphoton microscopy to investigate simultaneously the second and third-order nonlinear response of Potassium Niobate and Bismuth Ferrite harmonic nanoparticles. We first derive the second-to-third harmonic intensity ratio for colloidal ensembles and estimate the average third-order efficiency of these two materials. Successively, we explore the orientation dependent tensorial response of individual nanoparticles fixed on a substrate. The multi-order polarization resolved emission curves are globally fitted with an analytical model to retrieve individual elements of susceptibility tensors.

International audience; Charge transfer mechanisms lay at the heart of chemistry and biochemistry. Proton coupled electron transfers (PCET) are central in biological processes such as photosynthesis and in the respiratory chain, where they mediate long-range charge transfers. These mechanisms are normally difficult to harness experimentally due to the intrinsic complexity of the associated biological systems. Metal-peptide cations experience both electron and proton transfers upon photoexcitation, proving an amenable model system to study PCET. We report on a time-resolved experiment designed to follow this dual charge transfer kinetics in [HG3W+Ag]+ (H = histidine, G = glycine, W = tryptophan) on time scales ranging from femtoseconds to milliseconds. While electron transfer completes in less than 4 ps, it triggers a proton transfer lasting over hundreds of microseconds. Molecular dynamics simulations show that conformational dynamic plays an important role in slowing down this reaction. This combined experimental and computational approach provides a view of PCET as a single phenomenon despite its very wide time-domain span.

Bismuth Ferrite (BFO) nanoparticles (BFO-NP) display interesting optical (nonlinear response) and magnetic properties which make them amenable for bio-oriented applications as intra- and extra membrane contrast agents. Due to the relatively recent availability of this material in well dispersed nanometric form, its biocompatibility was not known to date. In this study, we present a thorough assessment of the effects of in vitro exposure of human adenocarcinoma (A549), lung squamous carcinoma (NCI-H520), and acute monocytic leukemia (THP-1) cell lines to uncoated and poly(ethylene glycol)-coated BFO-NP in the form of cytotoxicity, haemolytic response and biocompatibility. Our results support the attractiveness of the functional-BFO towards biomedical applications focused on advanced diagnostic imaging., Word Count: 109 Complete Word Count (body text and figure legends) : 4886 Number of Figures: 6 Number of Tables: 0 Number of reference: 45

Second Harmonic Generation (SHG) from BiFeO3 nanocrystals is investigated for the first time to determine their potential as biomarkers for multiphoton imaging. Nanocrystals are produced by an auto-combustion method with 2-amino-2-hydroxymethyl-propane-1,3-diol as a fuel. Stable colloidal suspensions with mean particle diameters in the range 100–120 nm are then obtained after wet-milling and sonication steps. SHG properties are determined using two complementary experimental techniques, Hyper Rayleigh Scattering and nonlinear polarization microscopy. BiFeO3 shows a very high second harmonic efficiency with an averaged hdi coefficient of 79612 pm/V. From the nonlinear polarization response of individual nanocrystals, relative values of the independent dij coefficients are also determined and compared with recent theoretical and experimental studies. Additionally, the particles show a moderate magnetic response, which is attributed to gamma-Fe2O3 impurities. A combination of high nonlinear optical efficiency and magnetic response within the same particle is of great interest for future bio-imaging and diagnostic applications.

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.

International audience; Nonlinear optical nanocrystals have been recently introduced as a promising alternative to fluorescent probes for multiphoton microscopy. We present for the first time a complete survey of the properties of five nanomaterials (KNbO3, LiNbO3, BaTiO3, KTP, and ZnO), describing their preparation and stabilization and providing quantitative estimations of their nonlinear optical response. In the light of their prospective use as biological and clinical markers, we assess their biocompatibility on human healthy and cancerous cell lines. Finally, we demonstrate the great potential for cell imaging of these inherently nonlinear probes in terms of optical contrast, wavelength flexibility, and signal photostability.

Fundamental molecular selectivity limits are probed by exploiting laser-controlled quantum interferences for the creation of distinct spectral signatures in two flavin molecules, erstwhile nearly indistinguishable via steady-state methods. Optimal dynamic discrimination (ODD) uses optimally shaped laser fields to transiently amplify minute molecular variations that would otherwise go unnoticed with linear absorption and fluorescence techniques. ODD is experimentally demonstrated by combining an optimally shaped UV pump pulse with a time-delayed, fluorescence-depleting IR pulse for discrimination amongst riboflavin and flavin mononucleotide in aqueous solution, which are structurally and spectroscopically very similar. Closed-loop, adaptive pulse shaping discovers a set of UV pulses that induce disparate responses from the two flavins and allows for concomitant flavin discrimination of ∼16σ. Additionally, attainment of ODD permits quantitative, analytical detection of the individual constituents in a flavin mixture. The successful implementation of ODD on quantum systems of such high complexity bodes well for the future development of the field and the use of ODD techniques in a variety of demanding practical applications.

5 pags, 4 figs.-- PACS number(s): 42.65.Jx, 42.65.Tg, 78.20.Ci. -- Publisher error corrected 27 September 2010, Erratum Phys. Rev. A 82, 039905 (2010): https://doi.org/10.1103/PhysRevA.82.033826, Based on numerical simulations, we show that higher-order nonlinear indices (up to n8 and n10, respectively) of air and argon have a dominant contribution to both focusing and defocusing in the self-guiding of ultrashort laser pulses over most of the spectrum. Plasma generation and filamentation are therefore decoupled. As a consequence, ultraviolet wavelength may not be the optimal wavelength for applications requiring to maximize ionization. © 2010 The American Physical Society., This work was supported by the Conseil Régional de Bourgogne, the ANR COMOC, the FASTQUAST ITN Program of the 7th FP, and the Swiss NSF (Contracts No. 200021-116198 and No. 200021-125315).

International audience; We numerically investigate the pulse compression mechanism in the infrared spectral range based on the successive action of nonlinear pulse propagation in a hollow-core fiber (HCF) followed by linear propagation through bulk material. We found an excellent agreement of simulated pulse properties with experimental results at 1.8 µm in the two optical-cycle regime close to the Fourier limit (FL). In particular, the spectral phase asymmetry attributable to self-steepening combined with self-phase modulation (SPM) is a necessary prerequisite for subsequent compensation by the phase introduced by glass material in the anomalous dispersion regime. The excellent agreement of the model enabled simulating pressure and wavelength tunability of sub-two cycles in the range from 1.5-4 µm with this cost-efficient and robust approach.

Fundamental selectivity limits of quantum control are pushed by introducing laser driven optimal dynamic discrimination to create distinguishing excitations on two nearly identical flavin molecules. Even with modest spectral resources, significant specificity is achieved with optimal pulse shapes, which amplify small molecular differences to create distinct, identifying signals. Rather than being a hindrance, system complexity appears to aid the control process and augments control field capability, which bodes well for implementation of quantum control in a variety of demanding applications.

We demonstrate the possibility to excite second-harmonic (SH) active Fe(IO(3))(3) nanocrystals with two distinct laser sources at 800 and 1550 nm, and we show, by a complementary experimental and numerical study, how the wavelength flexibility inherent to non-phase-matched SH nanoparticles can be efficiently exploited to increase imaging penetration depth of markers embedded in biological samples.

International audience; We present a technique to characterize ultrashort pulses at the focal plane of a high numerical aperture objective with unprecedented spatial resolution, by performing a FROG measurement with a single nanocrystal as nonlinear medium. This approach can be extended to develop novel phase-sensitive techniques in laser scanning microscopy, probing the microscopic environment by monitoring phase and amplitude distortions of femtosecond laser pulses.

We measured the angular distribution of the near-backward multiphoton-excited fluorescence emission by ellipsoidal-shaped, dye-doped ethanol microdroplets deformed perpendicularly to the direction of the incident laser beam. The high-intensity region in the backward direction is elongated in the same direction as the emitting microdroplet. Simulations based on ray tracing agree well with the experimental pattern and show that the droplet aspect ratio ϱ may be deduced from the fluorescence pattern of both oblate and prolate microparticles with ϱ varying from 0.9 to 1.3.

International audience; Femtosecond pump-probe experiments are performed on flavin biomolecules isolated in an ion trap. Mass spectra of the photoinduced fragments show that the fragmentation pathways can be modified using two-color two-photon excitation. In particular, when an infrared probe pulse (810 nm) is added subsequent to the first excitation step (excitation of the S(1) state of flavin mononucleotide at 405 nm), branching ratios between lumichrome and lumiflavin production are inverted relative to the single excitation case.

Distortions of ultrashort laser pulses propagating through turbulence are investigated both experimentally and numerically. As expected, a strong correlation is found between temporal distortions and local intensity on the speckle pattern. We suggest that the localization of distortions in low-intensity regions may favor remote control strategies based on nonlinear interactions with respect to those based on linear schemes.

International audience; BACKGROUND: Moderately cold head-out water immersion stimulates both baro- and cold-receptors, and triggers complex and contradictory effects on the cardiovascular system and its autonomic nervous control. OBJECTIVES: To assess the effects of water immersion and cold on cardiovascular status and related autonomic nervous activity. METHODS: Hemodynamic variables and indexes of autonomic nervous activity (analysis of heart rate and blood pressure variability) were evaluated in 12 healthy subjects during 3 exposures of 20 min each in the upright position, i.e., in air (AIR, 24-25 degrees C), and during head-out water immersion at 35-36 degrees C (WIn) and 26-27 degrees C (WIc). RESULTS: Plasma noradrenaline, systolic and diastolic blood pressure, and total peripheral resistances were reduced during WIn compared to AIR (263.9 +/- 39.4 vs. 492.5 +/- 35.7 pg x ml(-1), 116.5 +/- 3.7 and 65.4 +/- 1.7 mmHg vs. 140.8 +/- 4.7 and 89.8 +/- 2.8 mmHg, 14.1 +/- 1.0 vs. 16.3 +/- 0.9 mmHg x L(-1) x min, respectively) while they were increased during WIc (530.8 +/- 84.7 pg ml(-1), 148.0 +/- 7.0 mmHg, 80.8 +/- 3.0 mmHg, and 25.8 +/- 1.9 mmHg x L(-1) x min, respectively). The blood pressure variability was reduced to the same extent during WIc and Win compared to AIR. Heart rate decreased during WIn (67.8 +/- 2.7 vs. 81.2 +/- 2.7 bpm during AIR), in parallel with an increased cardiac parasympathetic activity. This pattern was strengthened during WIc (55.3 +/- 2.2 bpm). CONCLUSIONS: Thermoneutral WI lowered sympathetic activity and arterial tone, while moderate whole-body skin cooling triggered vascular sympathetic activation. Conversely, both WI and cold triggered cardiac parasympathetic activation, highlighting a complex autonomic control of the cardiovascular system.

International audience; Multiple filamentation in a high concentration solution of coumarin 153 in ethanol is studied. It is shown that the output filament pattern may be controlled by placing diffractive elements (circular aperture, edge) in the input beam path. These filaments are formed in highly reproducible arrays along diffraction maxima corresponding to the element used. Experimental results are supported by numerical simulations. They confirm that diffraction-induced intensity gradients swamp modulational instability on the wavefront, forcing filaments to form along diffraction maxima. The effect of two-photon absorption by coumarin molecules on filament patterns is also investigated over a range of dye concentrations. Control results are finally exploited in the production of arrays of localized lasing filaments, which should open novel applications. The resultant lasing sources are mutually coherent and highly repeatable from shot-to-shot, as is shown by their far-field interference patterns.

International audience; The present study was aimed at investigating the autonomic nervous system influences on the fractal organization of human heart rate during sympathovagal interactions, with special emphasize on the short-term fractal organization in heart rate variability (HRV), as assessed by the scaling exponent (alpha(1)) of the detrended fluctuation analysis. Linear and non-linear HRV analyses were used to study the sympathetic and vagal modulation of heart rate in ten healthy men (mean +/- SEM; age 26 +/- 1 years) during conditions of 1) increased sympathetic activity and vagal withdrawal (head-up tilt), 2) decreased sympathetic activity and increased vagal outflow (thermoneutral upright head-out water immersion, WIn), and 3) simultaneous activation of the two arms of the autonomic nervous activity (upright head-out immersion in cold water, WIc). Hemodynamic and linear HRV results were consistent with previous reports during similar physiological conditions. alpha(1) increased significantly during head-up tilt (from 0.71 +/- 0.13 supine to 0.90 +/- 0.15 upright) and WIn (0.86 +/- 0.10) and was significantly decreased during WIc (0.61 +/- 0.15). Thus, alpha(1) increased when the cardiac autonomic interplay was altered in a reciprocal fashion, whatever the direction of the balance change. Conversely, alpha(1) decreased during the concomitant activation of both vagal and sympathetic activities. The results of linear analysis were necessary to precisely define the direction of change in autonomic control revealed by an increase in alpha(1), while the direction of change in alpha(1) indicated whether an increased vagal activity is coupled with a decreased or increased sympathetic activation. Using both linear and non-linear analysis of HRV may increase the understanding of changes in cardiac autonomic status.

International audience; We present the most powerful white light femtosecond Lidar experiment to date using a 30J-30TW laser. We also discuss the applicability of coherent control to femtosecond Lidar experiments, in order to identify bioagents in air.

The present study was designed to assess the cardiac changes induced by cold water immersion compared with dry conditions during a prolonged hyperbaric and hyperoxic exposure (ambient pressure between 1.6 and 3 ATA and PiO(2) between 1.2 and 2.8 ATA). Ten healthy volunteers were studied during a 6 h compression in a hyperbaric chamber with immersion up to the neck in cold water while wearing wet suits. Results were compared with measurements obtained in dry conditions. Echocardiography and Doppler examinations were performed after 15 min and 5 h. Stroke volume, left atrial and left ventricular (LV) diameters remained unchanged during immersion, whereas they significantly fell during the dry session. As an index of LV contractility, percentage fractional shortening remained unchanged, in contrast to a decrease during dry experiment. Heart rate (HR) significantly decreased after 5 h, although it had not changed during the dry session. The changes in the total arterial compliance were similar during the immersed and dry sessions, with a significant decrease after 5 h. In immersed and dry conditions, cardiac output was unchanged after 15 min but decreased by almost 20% after 5 h. This decrease was related to a decrease in HR during immersion and to a decrease in stroke volume in dry conditions. The hydrostatic pressure exerted by water immersion on the systemic vessels could explain these differences. Indeed, the redistribution of blood volume towards the compliant thoracic bed may conceal a part of hypovolaemia that developed in the course of the session.

International audience; We have applied a multiobjective genetic algorithm to the optimization of multiphoton-excited fluorescence. Our study shows the advantages that this approach can offer to experiments based on adaptive shaping of femtosecond pulses. The algorithm outperforms single-objective optimizations, being totally independent from the bias of user defined parameters and giving simultaneous access to a large set of feasible solutions. The global inspection of their ensemble represents a powerful support to unravel the connections between pulse spectral field features and excitation dynamics of the sample.

International audience; We investigated femtosecond pump-repump depletion schemes in biological fluorophors (tryptophan and riboflavin) in order to discriminate bioaerosols from organic interferents emitted by combustion (traffic related urban aerosols). Although fluorescence depletion is significative for riboflavin (Rbf, Vitamin B2), the most striking results have been obtained for the amino acid tryptophan (Trp). By using a 270 nm-pump 810 nm-repump fermosecond excitation, we showed that Trp exhibits fluorescence depletion up to 50%, contrary to naphthalene (< 2%), despite almost identical absorption/emission spectra. We demonstrate that this process in Trp is so robust that it still occurs in living bacteria (Bacillus subtilis, Escherechia coli and Enterococcus f ae calis) but is absent for pure diesel fuel. This remarkable difference between biological and organic aerosols can be exploited to discriminate among them.

International audience; The triggering and guiding of negative discharges using filaments induced by a femtosecond-terawatt laser pulse have been studied in sphere-plane gaps up to 4.5 meters. Fast-frame camera pictures allow the evaluation of the influence of the negative leader propagation on the triggering and guiding process. We show that the plasma channel can either trigger a space-leader discharge or act as a guiding path for the negative leader head. For the latter case the results suggest a linear dependence of the guided lengths up to 2.4 m, while the formation of a space-leader reduces this guided length by up to 50%. This effect is explained by the limited plasma lifetime of the filament that is measured to be about 1 μs.

International audience; Using femtosecond laser-induced breakdown spectroscopy, the authors have analyzed five different species of bacterium. Line emissions from six trace mineral elements, Na, Mg, P, K, Ca, and Fe, have been clearly detected. Their intensities correspond to relative concentrations of these elements contained in the analyzed samples. The authors demonstrate that the concentration profile of trace elements allows unambiguous discrimination of different bacteria. Quantitative differentiation has been made by representing bacteria in a six-dimension hyperspace with each of its axis representing a detected trace element. In such hyperspace, representative points of different species of bacterium are gathered in different and distinct volumes.

International audience; We demonstrate that the capacity of ultrashort high-power laser pulses to trigger and guide high-voltage discharges can be significantly enhanced by a subsequent visible nanosecond laser pulse. The femtosecond pulse induces a bundle of filaments, which creates a conducting channel of low density and cold plasma connecting the electrodes. The subsequent laser pulse photodetaches electrons from O2- ions in the electrode leader. The resulting electrons allow efficient heating by Joule effect in a retroaction loop, resulting in a 5% reduction of the breakdown voltage.

International audience; A sample of Escherichia coli has been analyzed by laser-induced breakdown spectroscopy (LIBS) using femtosecond pulses. The spectrum shows strong CN molecular bands due to the direct ablation of native CN molecular bonds from the bacteria in contrast with weak atomic lines from carbon. The native nature of the observed CN bonds is supported by the kinetic behavior of the CN band head which rapidly decays with a time constant of 94 ns, while for a pure graphite sample the CN band head increases with a delay of 450 ns due to recombination with the ambient air. Moreover, about hundred resolved lines belonging to 12 atomic or molecular species are recorded, providing a valuable spectral signature to identify the bacterium.

International audience; The propagation of femtosecond terawatt laser pulses at reduced pressure (0.7 atm) is investigated experimentally. In such conditions, the non-linear refractive index n 2 is reduced by 30%, resulting in a slightly farther filamentation onset and a reduction of the filament number. However, the filamentation process, especially the filament length, is not qualitatively affected. We also show that drizzle does not prevent the filaments from forming and propagating.

International audience; We demonstrate remote elemental analysis at distances up to 90 m, using a laser-induced breakdown spectroscopy scheme based on filamentation induced by the nonlinear propagation of unfocused ultrashort laser pulses. A detailed signal analysis suggests that this technique, remote filament-induced breakdown spectroscopy, can be extended up to the kilometer range.

International audience; The filamentation of femtosecond light pulses in air is numerically and experimentally investigated for beam powers reaching several TW. Beam propagation is shown to be driven by the interplay between intense, robust spikes created by the defects of the input beam and random nucleation of light cells. Evolution of the filament patterns can be qualitatively reproduced by an averaged-in-time (2D+1)-dimensional model derived from the propagation equations for ultrashort pulses.

International audience; Ultrashort, high-power laser pulses propagating vertically in the atmosphere have been observed over more than 20 km using an imaging 2-m astronomical telescope. This direct observation in several wavelength bands shows indications for filament formation at distances as far as 2 km in the atmosphere. Moreover, the beam divergence at 5 km altitude is smaller than expected, bearing evidence for whole-beam parallelization about the nonlinear focus. We discuss implications for white-light Lidar applications.

International audience; We demonstrate experimentally the first range-resolved detection and identification of biological aerosols in the air by non-linear lidar. Ultra-short terawatt laser pulses are used to induce two-photon-excited fluorescence (2PEF) in riboflavin-containing particles at a remote location. We show that, in the case of amino acid detection, 2PEF-lidar should be more efficient than linear 1PEF-lidar beyond a typical distance of 2 km, because it takes advantage of the higher atmospheric transmission at the excitation wavelengths. 2PEF-lidar moreover allows size measurement by pump-probe schemes, and pulse shaping may improve the detection selectivity.

International audience

In this paper, we present a new methodology for urban aerosol survey, coupling Lidar measurements and numerical models. The aim of this study is build a continuous survey of aerosol impact on the local and regional scale.

Lidar signals were obtained for the first time in the near-infrared using the supercontinuum generated by the terawatt femtosecond laser of the Teramobile system. A signal up to 4 km in altitude, in the band 1–1.7 μm, was collected using a 2 m astronomical telescope. We observed a 10-fold enhancement of the infrared signal backscattered from the atmosphere compared with that expected using a previously measured laboratory spectrum. This suggests a more efficient frequency conversion into the infrared (typically 7% into the 1–1.5 μm band) under long-distance propagation conditions.

International audience; We describe the Teramobile system, a new mobile femtosecond multi-terawatt laser and detection system based on a state-of-the art CPA laser system embedded in a standard freight container, as well as a mobile detection unit allowing a characterization of the nonlinear propagation of high power laser pulses over long horizontal distances. The unique mobility feature of the whole system opens the way to previously unreachable applications for high-power laser pulses in the field of atmospheric research (lidar, laser-triggered lightning), which are also briefly reviewed.

International audience; This paper reports on a model investigation of a particular episode of tropospheric ozone formation in the city of Lyon, France. A large-scale measurement campaign involving ground-based analyzers, sampling, Sodars and Lidars has been used to validate the model results. Based on validated meteorological data and primary pollutant concentrations, the numerical model has been run to obtain 3D ozone concentration profiles during the whole campaign (22-25 June 1999). The results are compared to the ozone Lidar vertical profiles. Good agreement between Lidar data and model predictions is first obtained on 22 June (but not on the following days). On 23 and 24 June, ozone concentrations are significantly underestimated by the model. The ozone Lidar measurements allowed identifying large import processes from high altitudes that explain the difference. In a second model simulation, these imports are taken into account as new boundary conditions. This yielded good agreement between the experimental data and the predicted ozone concentrations over the whole period. The evidence of high altitude ozone intrusion is confirmed by back-trajectories calculations.

This paper is devoted to two photons excited fluorescence in a spherical micro-cavity. We describe the internal fields created when two ultra-short pulses of light illuminate a spherical micro-cavity, with the time delay between the two pulses as a parameter.

National audience; All solid-state laser based Lidar systems allow today a direct access to the air pollution physico-chemistry. As an example, we present the characterization of an ozone episode in Paris in summer 1999, using Lidar 3D-mappings over 33 hours.; Les systèmes Lidar actuels, basés sur des lasers solides, permettent un accès direct à la physico chimie de la pollution atmosphérique. Nous présentons, en exemple, la caractérisation d'un épisode d'ozone à Paris durant l'été 1999, en utilisant les cartographies 3D obtenues sur 33 heures.

International audience; Lidar measurements of stratospheric aerosols were made at several Arctic and mid-latitude stations as part of the European Arctic Stratospheric Ozone Experiment (EASOE) in 1991/92. Volcanic aerosols were observed throughout the winter at all stations. High latitude stations observed an aerosol-free stratosphere during most of the winter at altitudes above 450 K potential temperature (above 16 km). An even latitudinal distribution of volcanic aerosols was observed below this level. This is interpreted as indicative of latitudinal transport into the polar region throughout the winter.

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Lithium clusters up to Li 100 are produced in a seeded molecular beam using a special oven able tu sustain temperature up to 1800 K. Optical spectra were recorded by two photon ionization spectroscopy for Li 3 and dy depletion for larger clusters because of fast dissociation in excited states. For Li 3 , clear vibronic and rotational structures have been measured leading to a complete determination of the geometry and potential surfaces of the ground state of the two observed excited states. For larger clusters, no vibronic structure was observed except in Li 4 for which a residual vibronic pattern was obtained. Optical spectra have been compared to SCF-CI calculations [1]. Since the calculated spectra strongly depend on the ground state geometry, it is possible to determine the cluster geometry. In Li 4 , the experimental absorption spectrum is in complete agreement with the theoretical spectrum obtained for the planar rhombus geometry while the theoretical spectrum calculated for the other isomer slightly higher in energy (deformed tetrahedron) is completely different. This is the first confirmation of the planar rhombus geometry of Li 4 . For Li 7 and Li 8 , the experimental results are also in agreement with the geometries calculated by the SCF-CI method. In Li 6 , the calculations lead to three isomers having very similar energy [2] : the planar D 3h structure, the quasi planar C 5v pentagonal pyramid and the 3D trypyramidal C 2v geometry. Only this last geometry gives a theoretical absorption spectrum in agreement with the experimental one. The two other structures lead mainly to a hyge peak at 2.1 eV in complete contradiction with the experimental results. Experiments are in progress to extend our measurements up to Li 40

Non-centrosymetric nanocrystals show promising nonlinear optical properties for being used as optical labels in bio-imaging applications, with significant interest for observations of long duration and for penetration depth into biological tissues. The development of such biomarkers requires the determination of their nonlinear optical properties to select the best potential markers. In this thesis, Hyper-Rayleigh Scattering (HRS) technique is used to determine nonlinear efficiencies of several nanocystals (BaTiO3, KNbO3, KTP, LiNbO3, ZnO and BiFeO3). These ensemble measurements have been performed on nanocrystals suspensions, for which the influence of parameters such as size, concentration and aggregation state was discussed. BiFeO3nanocrystals offer the best nonlinear optical efficiency compared to other particles, showing their potential as efficient optical biomarkers. Polarisation-resolved measurements have also been performed to retrieve individual coefficients of the nonlinear tensor of the investigated materials and influent parameters such as nanocrystals shape have been identified.; Les nanocristaux à structure non-centrosymétrique présentent des propriétés optiques non linéaires prometteuses pour une utilisation en tant que marqueurs optiques en imagerie biomédicale, avec un intérêt significatif en termes de suivi sur de longues durées et de profondeur de pénétration dans les tissus biologiques. Le développement de ces marqueurs nécessite la détermination de leurs efficacités optiques non linéaires afin de pouvoir sélectionner les nanocristaux les plus prometteurs. Pour cela, la technique de diffusion Hyper-Rayleigh a été adaptée à la caractérisation de suspensions de nanoparticules (BaTiO3, KNbO3, KTP, LiNbO3 et ZnO, BiFeO3) pour lesquelles l’influence de paramètres comme la taille, la concentration ou l’état d’agrégation a été analysée et discutée. Les nanocristaux de BiFeO3 possèdent une efficacité optique non linéaire largement supérieure aux autres particules, démontrant leur potentiel pour la réalisation de nano-sondes optiques particulièrement performantes. Des mesures résolues en polarisation ont également été mises en œuvre pour déterminer les coefficients optiques non linéaires indépendants des particules étudiées. Dans ce cadre, une étude a permis de mettre en évidence l’influence de la forme des nanocristaux sur cette réponse.

Non-centrosymetric nanocrystals show promising nonlinear optical properties for being used as optical labels in bio-imaging applications, with significant interest for observations of long duration and for penetration depth into biological tissues. The development of such biomarkers requires the determination of their nonlinear optical properties to select the best potential markers. In this thesis, Hyper-Rayleigh Scattering (HRS) technique is used to determine nonlinear efficiencies of several nanocystals (BaTiO3, KNbO3, KTP, LiNbO3, ZnO and BiFeO3). These ensemble measurements have been performed on nanocrystals suspensions, for which the influence of parameters such as size, concentration and aggregation state was discussed. BiFeO3nanocrystals offer the best nonlinear optical efficiency compared to other particles, showing their potential as efficient optical biomarkers. Polarisation-resolved measurements have also been performed to retrieve individual coefficients of the nonlinear tensor of the investigated materials and influent parameters such as nanocrystals shape have been identified., Les nanocristaux à structure non-centrosymétrique présentent des propriétés optiques non linéaires prometteuses pour une utilisation en tant que marqueurs optiques en imagerie biomédicale, avec un intérêt significatif en termes de suivi sur de longues durées et de profondeur de pénétration dans les tissus biologiques. Le développement de ces marqueurs nécessite la détermination de leurs efficacités optiques non linéaires afin de pouvoir sélectionner les nanocristaux les plus prometteurs. Pour cela, la technique de diffusion Hyper-Rayleigh a été adaptée à la caractérisation de suspensions de nanoparticules (BaTiO3, KNbO3, KTP, LiNbO3 et ZnO, BiFeO3) pour lesquelles l’influence de paramètres comme la taille, la concentration ou l’état d’agrégation a été analysée et discutée. Les nanocristaux de BiFeO3 possèdent une efficacité optique non linéaire largement supérieure aux autres particules, démontrant leur potentiel pour la réalisation de nano-sondes optiques particulièrement performantes. Des mesures résolues en polarisation ont également été mises en œuvre pour déterminer les coefficients optiques non linéaires indépendants des particules étudiées. Dans ce cadre, une étude a permis de mettre en évidence l’influence de la forme des nanocristaux sur cette réponse.

Ultrashort laser pulses propagate in the air in the form of structures of one hundredmicrons of diameter called “filaments”, which have the properties of self-guiding, propagatingfor hundreds of meters, white light generation, etc. These original properties find severalapplications in the domain of remote sensing of pollutants by non-linear Lidar measurements,lightning control, remote LIBS, etc.During my PhD work we have performed several laboratory experiments and field campaignwithin the context of Teramobile project. In particular we have studied the geometry offilamentation, its robustness in an extended region of turbulent air, the propagation ofultrashort pulses beam in multijoules regime, and atmospheric applications of filamentation.For example, we have characterized the angular distribution of the conical emission in thevisible and ultraviolet spectral bands. In another series of experiments, we have proved thatatmospheric turbulence is not a limiting factor of filaments propagation, which also keep theirspectral properties useful for atmospheric applications. Finally, we have illustrated a methodof laser triggering and guiding of lightning and realized laser induced condensation of waterdroplets in laboratory as well as in a reel atmosphere.; La propagation des impulsions laser ultra brèves dans l’air se fait sous la forme de structures d’une centaine de micromètres de diamètre appelées filaments, qui ont entre autres les propriétés d’être autoguidées, de se propager sur plusieurs centaines de mètres, de générer un continuum de lumière blanche, etc. Ces propriétés originales trouvent de nombreuses applications dans le domaine de la télédétection des polluants par mesures lidar, le déclenchement et le guidage de la foudre par laser, le LIBS à distance, etc.Au cours de mon travail de thèse, nous avons mené de nombreuses expériences de laboratoire et sur terrain dans le cadre du projet Tera mobile. Nous avons en particulier étudié la géométrie de la filamentation, sa robustesse dans une région de turbulence étendue, la propagation verticale d’un faisceau d’impulsions ultra brèves dans un régime multi joules, et des applications atmosphériques de la filamentation. Nous avons par exemple caractérisé la distribution angulaire de l’émission conique dans le visible et dans l’ultraviolet. Nous avons également prouvé que la turbulence atmosphérique n’est pas un facteur limitant de la propagation des filaments qui arrivent même à garder leurs propriétés spectrales nécessaires aux applications atmosphériques. Enfin nous avons illustré une méthode de déclenchement et de guidage de foudre par laser et réalisé une expérience de condensation de gouttelettes d’eau assistée par laser en laboratoire ainsi que dans une atmosphère réelle.