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International audience; The study of complex reactive flows met in aeronautical engines is an experimental challenge that requires the development of noninvasive and precise measurement techniques. Coherent anti-Stokes Raman scattering (CARS) is a standard spectroscopic technique used for temperature measurements, which provides unmatched reliability and accuracy at high repetition rate thanks to its recent adaptation to femtosecond temporal regime. This paper reports the first demonstration of hybrid fs/ps-CARS thermometry in a representative aeronautical combustor (ONERA MICADO test bench, Reynolds number ≈105). Single-shot N2 CARS spectra have been recorded at 1 kHz, allowing temperature follow up, statistical and frequency (0.1–500 Hz) analysis of CH4/air flame at 0.34-MPa total pressure. The achieved results demonstrate the ability of the technique to be applied in representative engines conditions and its maturity for semi-industrial applications.

International audience; Non-invasive and accurate measurements are essential to study the reactive flows in aeronautical engines. This paper reports the results of a unique measurement campaign providing the temperature flowfield in a large scale facility turbomachine test rig using spontaneous rotational Raman scattering technique. Different planes of interest and operating conditions are probed, showing good agreement with thermocouple measurements. Fast temperature variations (>7.7 kHz) could be probed thanks to synchronization of the laser pulse with the rotor clock. Results outline the performance of in situ Raman technique to investigate steady and unsteady flows in turbine's conditions.

International audience; La combustion est un sujet d’intérêt pour une large variété de domaines d’applications civils ou militaires. Comprendre les phénomènes physico-chimiques à l’oeuvre dans ces milieux complexes, et les décrire à l’aide de modèles éprouvés, sont des enjeux majeurs qui requièrent des mesures fiables et quantitatives. La spectroscopie par diffusion Raman anti-Stokes cohérente (DRASC ou CARS en anglais) a démontré des performances inégalées pour la mesure de température. Cette technique a été implémentée avec de nombreuses architectures laser, et appliquée avec succès à un large éventail de milieux.

This paper demonstrates a new arrangement for wide-field CARS imaging. The setup using nanosecond dye lasers in a non-phase-matching illumination is presented. The chemical selectivity of the signal is demonstrated on polystyrene beads. Moreover, the experimental arrangement has enabled the acquisition of images of living cells in suspension with a satisfactory signal-to-background ratio by using only a single pair of laser shots. Therefore, each image can be acquired using a total duration of 3 ns, which is the pulse duration of the laser used in this study. Finally, lack of damage on cells has been demonstrated in conditions leading to strong CARS signal generation. In particular, no cell morphological changes were observed and cell membrane integrity (assessed by trypan blue test) was preserved. Copyright © 2012 John Wiley & Sons, Ltd.

A comparative study was made of sorted semi-conducting single walled carbon nanotube (SWCNT) films and unsorted SWCNT films for gas sensing applications. The transmission line method is used to monitor separately the SWCNTs film resistance and the contact resistance between electrodes and the SWCNTs, thus revealing that the sensing mechanism mainly relies on a modification of the tube conductivity during gas exposure. The fabricated sensors demonstrate a detection limit of 20 ppb NO2 and 600 ppb NH3 mainly attributed to experimental setup limitations. Moreover, semi-conducting nanotubes happened to be 2.5 times more sensitive to NH3 than unsorted ones, thus proving that selectivity can be improved by sorting the SWCNTs. The temperature dependence of the sensor sensitivity was studied, and a good agreement was found between experimental results and the Langmuir adsorption model.

The optoelectronic properties of hexagonal boron-nitride and boron-nitride nanotubes (BNNTs) are investigated by using photoconductivity experiments, associated to photoluminescence excitation analysis. By this way, excitations related to the conduction band of hexagonal boron-nitride have been experimentally determined, as well as the free excitonic level. Multiwalled boron-nitride nanotubes have also been lead by using these methods and the first results suggest some hypotheses about the band gap energy and the nature of the various absorptions, which occur under an UV excitation. These experimental results are presented and discussed and some perspectives are finally suggested.

In this paper we report the fabrication and characterization of single wall carbon nanotube film based devices. Carbon nanotubes (CNT) film is deposited on a silica substrate and usual clean room processes have been used to make Pt-electrodes on top of it and to pattern the CNT film. The obtained devices have been used to measure the evolution of the temperature coefficient of resistance (TCR) as a function of temperature. At room temperature the TCR is –0.2%K-1 and becomes even more important as the temperature goes down. Moreover the optical response in atmospheric band II and band III have been investigated at room temperature showing a variation of the device resistance up to 0.2% for an irradiance of ∼100 mW/cm2 in the 3–5 µm range. Such results are very promising for application of CNT films in bolometers for thermal infrared detection (© 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

International audience; Planar laser-induced fluorescence on atomic iron is investigated in this paper, and a measurement strategy is proposed to monitor the fluorescence of iron atoms with good sensitivity. A model is proposed to fit the experimental fluorescence spectra, and good agreement is found between simulated and experimental spectra. Emission and laser-induced fluorescence measurements are performed in the flames of ammonium perchlorate composite propellants containing iron-based catalysts. A fluorescence signal from iron atoms after excitation at 248 nm is observed for the first time in propellant flames. Images of the spatial distribution of iron atoms are recorded in the flame in which turbulent structures are generated. Iron fluorescence is detected up to 1.0 MPa, which opens the way to application in propellant combustion.; L'imagerie de fluorescence induite par laser est appliquée aux atomes de fer et une stratégie pour leurs mesurer avec une bonne sensibilité est présentée dans cet article. Un modèle est développé pour calculer les spectres de fluorescence et un bon accord est trouvé entre les spectres calculés et expérimentaux. Les mesures en émission et en fluorescence induite par laser sont effectuées dans des flammes de propergols composites à base de perchlorate d'ammonium dopés avec des catalyseurs ferriques.Le signal de fluorescence induit par l'excitation laser à 248 nm des atomes de fer est observé pour la première fois dans les flammes de propergol. La répartition spatiale des atomes de fer est visualisée en flamme dont les structures turbulentes sont forcées. La fluorescence du fer est détectée jusqu'à 1,0 MPa, ce qui ouvre des perspectives de visualisation d'écoulements de gaz de combustion de propergols solides.

Optical properties of multiwall boron nitride nanotubes are investigated by means of luminescence and absorption spectroscopies. Cathodoluminescence imaging shows that boron nitride nanotubes are highly UV luminescent materials and that the luminescence is located all along the nanotube. In comparison with the related bulk material, hexagonal boron nitride, luminescence and absorption experiments point out the role of excitonic effects in this nanoobject.

The main consequence of the interaction between cells and pulsed electric fields is the destabilization of the plasma membrane leading to its permeabilization. Previous vibrational spectroscopy studies (S.M. Gruenbaum et al., J. Chem. Phys., 135, 2011) have shown that interfacial water is highly organized around the phospholipids of the membrane. Moreover, various numerical studies (such as Molecular Dynamics simulations) have shown that the interfacial water is highly disturbed by the pulsed electric field. We detail here a study of the behavior of the interfacial water around biological objects, before and after exposition to intense pulsed electric fields, by Coherent Anti-stokes Raman Scattering (CARS) spectroscopy.

The temperature-induced changes in Raman spectra of two BN-based materials: a hexagonal boron nitride and soot with single-wall BN nanotubes, have been measured in temperature range 77-600 K in course of heating in the oven/cryostat cell. A nonlinear temperature dependence of the tangential Raman mode position (being at 1366 cm -1 at room temperature) has been observed for both materials. In the temperature range 350-600 K a linear approximation of the tangential Raman mode shifting was applicable. The measured rates were -0.014 cm -1 /K (for h-BN) and -0.027 cm -1 /K (for the nanotube-containing sample). The effects of the oven and laser heating have been compared. Under the laser heating with the same power density the nanotube-containing soot demonstrated much bigger shifts (up to 30 cm -1 ) than h-BN. The data obtained are useful for in-situ diagnostics of different BN-based phases in course of synthesis.

In situ measurements were executed in the continuous wave CO 2 -laser vaporization synthesis of single-walled carbon nanotubes (SWCNTs). The results were compared with the findings of the ex situ analysis of the product. Different catalysts (Co, Ni, Co/Ni, Ni/Y and Co/Y) were used and the temperature of the target surface (T s ) changed to compare the efficiency of the synthesis process. Our main results are related to the SWCNTs diameter which is depending on T, and on the catalysts nature. The targets containing Y with Co or Ni atoms produce more and larger SWCNTs than Co/Ni targets. The SWCNTs' diameter is seen to increase with T s .

International audience; Thin (0001) epitaxial aluminum nitride (AlN) layers were grown on c-plane sapphire using high temperature hydride vapor phase epitaxy. The experimental set-up consists of a vertical cold-wall quartz reactor working at low pressure in which the reactions take place on a susceptor heated by induction. The reactants used are ammonia and aluminum chlorides in situ formed via hydrogen chloride reaction with high purity aluminum pellets. As-grown AlN layers have been characterized by scanning electron microscopy, atomic force microscopy, X-ray diffraction, transmission electron microscopy, photoluminescence and Raman spectroscopies. The influence of the V/III ratio in the gas phase, from 1.5 to 15, on growth rate, surface morphology, roughness and crystalline quality is investigated in order to increase the quality of thin epitaxial AlN layers grown at high temperature. Typical growth rates of around 0.45 mu m/h were obtained for such thin epitaxial AlN layers. The growth rate was unaffected by the V/III ratio. An optimum for roughness, crystalline quality and optical properties seems to exist at V/III = 7.5. As a matter of fact, for a V/III ratio of 7.5, best root mean square roughness and crystalline quality-measured on 0002 symmetric reflection-as low as 6.9 nm and 898 arcsec were obtained, respectively.

The main consequence of the interaction between cells and pulsed electric fields is the destabilization of the plasma membrane leading to its permeabilization (allowing, for example, an uptake of external molecules by the biological cells). Electrochemotherapy [1,2] is one of the medical applications of this biophysical interaction. Although known for decades, the underlying mechanisms of cells electropermeabilization are still not fully understood [3]. One hypothesis explaining the membrane destabilization is the presence of chemically altered membrane phospholipids after the electrical excitation. We detail here a highly sensitive method coupling Raman Spectroscopy and CARS microscopy, to characterize the biochemical consequence of membranes electropermeabilization. An experimental setup of Raman spectroscope has been designed to probe the vibrational footprint of the membrane phospholipids. Comparing the vibrational footprint of biological samples before and after the application of pulsed electric fields can provide critical spectrum areas to characterize electropermeabilization. At UMR8203, a unique and homemade device [4] combines nanosecond electric pulses generator and wide-field CARS microscopy allowing to acquire images of living cells with a high time resolution. Based on the critical spectrum areas previously determined with Raman Spectroscopy, it will be possible to follow the evolution of the biochemical composition of the membrane during a pulsed electric field. The study is performed on two study systems: Giant Unilamellar Vesicles (GUV) of phospholipids which are a simple mimic of the cell membrane and DC-3F cells (Chinese hamster lung fibroblast cell) which are a classical cell line used to study electropermeabilization.

International audience; AlN layers were grown on c-plane sapphire substrates with AlN nucleation layers (NLs) using high temperature hydride vapor phase epitaxy (HT-HVPE). Insertion of low temperature NLs, as those typically used in MOVPE process, prior to the high temperature AlN (HT-AlN) layers has been investigated. The NLs surface morphology was studied by atomic force microscopy (AFM) and NLs thickness was measured by X-ray reflectivity. Increasing nucleation layer deposition temperature from 650 to 850 degrees C has been found to promote the growth of c-oriented epitaxial HT-AlN layers instead of polycrystalline layers. The growth of polycrystalline layers has been related to the formation of dis-oriented crystallites. The density of such disoriented crystallites has been found to decrease while increasing NLs deposition temperature. The HT-AlN layers have been characterized by X-ray diffraction theta - 2 theta scan and (0 0 0 2) rocking curve measurement, Raman and photoluminescence spectroscopies, AFM and field emission scanning electron microscopy. Increasing the growth temperature of HT-AlN layers from 1200 to 1400 degrees C using a NL grown at 850 degrees C improves the structural quality as well as the surface morphology. As a matter of fact, full-width at half-maximum (FWHM) of 0 0 0 2 reflections was improved from 1900 to 864 arcsec for 1200 degrees C and 1400 degrees C, respectively. Related RMS roughness also found to decrease from 10 to 5.6 nm. (C) 2012 Elsevier B. V. All rights reserved.

The boron nitride nanotubes (BNNTs) synthesis, using CO2-laser vaporization of a BN target under nitrogen gas, is investigated by UV-laser induced fluorescence (LIF) of the vapor phase and UV-Rayleigh scattering (RS) of the gas-suspended nanoparticles. The LIF signal from B atoms is mainly detected in the 1.5 mm-thick region above the BN target. It originates from a boron-rich vapor region confined near the hot boron droplet formed at the target surface. Then, recombination between hot boron and N2 gas occurs through a fast condensation process as revealed by both the depletion of B atoms from the vapor phase and the RS signal arising from the grown BN nanoparticles. Fluorescence spectra exhibit a strong peak at 250 nm due to boron fluorescence and mainly to nanoparticles Rayleigh scattering. A narrow peak is observed at 210 nm and a broader peak at 189 nm. These bands are tentatively assigned to fluorescence or photoluminescence (PL) from gaseous or solid BN species respectively since both gas and solid phases coexist in the plume due to the rapid cooling process. Two very weak bands occur at 308 nm and 350 nm. They are related to PL of defects bands from BN nanostructures on the basis of ex situ PL spectra of h-BN crystallites and multi-wall BNNTs. Detection of oxygen impurities is shown feasible through LIF from BO radical which is detected just above the BN target evaporated under vacuum pressure (∼1 mbar). An optical diagnosticstrategy is demonstrated from these first in situ observations during BNNTs synthesis.

The general expressions for rotationally resolved CARS transitions involving molecular electronic states of arbitrary electronic angular momentum and spin are derived. All possible types of resonances (triple, double, Raman) are considered and the explicit results are presented for Hund's coupling cases (a) and (b) and intermediate (a–b) coupling. The results given are applicable to arbitrary incident laser polarizations. Calculations of practical interest are performed for three diatomics, namely OH, C2 and CH, for the triple resonance. Complete sets of closed formulae are tabulated for Hund's cases (a) and (b) for 3Π ← 3Π and 2Σ ← 2Π type transitions. With minor modifications, these expressions are also applicable to resonant degenerate four wave mixing.

Individual multiwall boron nitride nanotubes with diameters from 30 nm to 110 nm are shown to be efficient UV emitters by cathodoluminescence. Their luminescence does not evolve much in this diameter range, with dominant UV recombinations at about 230 nm. As a result, single nanotube properties can be obtained from experiments performed on ensembles of nanotubes. Such ensembles are studied by photoluminescence as a function of temperature 5 K‐300 K and by photoluminescence excitation experiments at 9 K. The results are discussed and compared with the related bulk material, hexagonal boron nitride. The strong luminescence recorded around 230 nm is attributed to excitonic effects, more precisely to excitons bound to the structural defects: dislocations, facets, which are observed along the walls.

Cathodoluminescence imaging and spectroscopy experiments on a single bamboo-like boron nitride nanotube are reported. Imaging experiments show that the luminescence is located all along the nanotube. Spectroscopy experiments point out the important role of dimensionality in this one dimensional object.

M. G. Silly,1,2 P. Jaffrennou,1,2,4 J. Barjon,3 J.-S. Lauret,4 F. Ducastelle,1,* A. Loiseau,1 E. Obraztsova,5 B. Attal-Tretout,2 and E. Rosencher2 1Laboratoire d’Etude des Microstructures, ONERA-CNRS, Boite Postale 72, 92322 Châtillon Cedex, France 2Departement de Mesures Physiques, ONERA, Chemin de la Huniere, 91761 Palaiseau Cedex, France 3Groupe d’Etude de la Matiere Condensee, Universite de Versailles St. Quentin, CNRS Bellevue, 1 place Aristide Briand, 92195 Meudon Cedex, France 4Laboratoire de Photonique Quantique et Moleculaire, Institut d’Alembert, Ecole Normale Superieure de Cachan, 61 Avenue du President Wilson, 94235 Cachan Cedex, France 5A. M. Prokhorov General Physics Institute of Russian Academy of Sciences, 38 Vavilov Street, 119991 Moscow, Russia Received 27 July 2006; revised manuscript received 21 December 2006; published 12 February 2007

The excitonic recombinations in hexagonal boron nitride (hBN) are investigated with spatially resolved cathodoluminescence spectroscopy in the UV range. Cathodoluminescence images of an individual hBN crystallite reveals that the 215 nm free excitonic line is quite homogeneously emitted along the crystallite whereas the 220 nm and 227 nm excitonic emissions are located in specific regions of the crystallite. Transmission electron microscopy images show that these regions contain a high density of crystalline defects. This suggests that both the 220 nm and 227 nm emissions are produced by the recombination of excitons bound to structural defects.

BN nanotubes (BNNTs) are structurally similar to their carbon counterparts, though much less investigated. New synthesis methods have been recently reported, enabling the production of industrial quantities and stimulating the search of new applications for the BNNTs. In this paper, we investigate the luminescence of multiwall BNNTs. By performing cathodoluminescence experiments on single tubes at 10 K, we show that the tube luminescence is highly heterogeneous (i) from tube to tube and (ii) spatially along a single tube. By combining cathodoluminescence measurements with a nanometer excitation and transmission electron microscopy on the same tube, we correlate luminescence and structural features. We conclude that the near-band-edge luminescence of BNNTs (≈5.4 eV) is related to the presence of extended structural defects, such as dislocations or ruptures in the wall stacking.

Optical transitions in single-wall boron nitride nanotubes are investigated by means of optical absorption spectroscopy. Three absorption lines are observed. Two of them (at 4.45 and 5.5 eV) result from the quantification involved by the rolling up of the hexagonal boron nitride (h-BN) sheet. The nature of these lines is discussed, and two interpretations are proposed. A comparison with single-wall carbon nanotubes leads one to interpret these lines as transitions between pairs of van Hove singularities in the one-dimensional density of states of boron nitride single-wall nanotubes. But the confinement energy due to the rolling up of the h-BN sheet cannot explain a gap width of the boron nitride nanotubes below the h-BN gap. The low energy line is then attributed to the existence of a Frenkel exciton with a binding energy in the 1 eV range.

In this paper, we report about an application of the two-color laser-induced thermal gratings technique in the visible region to the detection of nitrogen dioxide in mixtures of nitrogen and argon at total pressure ranging up to 1 bar. We have investigated the dependence of the signal on the gas mixture parameters (pressure, NO 2 concentration, collision partners) and on the laser properties (beams polarization, pulse energy, bandwidth) at various instants during the temporal evolution of the thermal grating. Comparison of experimental results and theoretical predictions is performed. Finally, the detectivity of 4 ppm was obtained at normal conditions of pressure (1 bar) and temperature (300 K).

International audience; Laser-induced fluorescence (LIF) measurements of OH were performed in flat stoichiometric CH4/air flames burning at 1, 3, 5, 7, and 9.6 bar, which had previously been investigated using OH resonance CARS. In the LIF study, line shape information and temperatures were extracted from excitation spectra; in addition, OH profiles as a function of height above the burner surface and an estimate of the OH concentration for the different flames were obtained. The perspectives and feasibility of quantitative fluorescence measurements in high pressure flames are discussed, particularly in comparison with the application of resonance CARS.

During the PhD thesis, high-speed laser induced fluorescence (LIF) of two metallic atoms (Al and Fe) is presented, in order to use them as fluorescent markers in solid propellant flames, where they are naturally present. LIF measurements are first performed inside two different evaporation chambers used to generate aluminum vapors in controlled conditions over a broad pressure and temperature range. A theoretical model of the LIF process is elaborated and applied to both atoms in order to calculate the signal quenching rate as a function of pressure and temperature. Unavailable collisional data are determined theoretically for Fe and experimentally for Al.Energy transfer and collisional broadening coefficients are determined experimentally for the Al atom in pure nitrogen environment. Study of the signal level of Al as a function of laser intensity is undertaken to measure saturation thresholds in N₂, He and Ar as a function of pressure. The model is used to properly reproduce the temporal and spectral profiles, though some approximations and limitations remain. A first application of high-speed LIF imaging to the measurement of aluminum in a solid propellant flame (10 bar , 3000 K) is demonstrated. It allows us to clearly visualize reactive aluminum droplets in the flame and to follow their evolution in the flame., Cette thèse porte sur la méthode de Fluorescence Induite par Laser (LIF) à haute cadence développée sur deux atomes métalliques (Al et Fe) utilisés comme traceurs fluorescents dans les flammes de propergols solides où ils sont naturellement présents. Deux expériences d’évaporation de l’aluminium sont mises en œuvre pour mettre au point la technique dans des conditions contrôlées sur une large gamme de pressions et températures. Un modèle théorique du processus de fluorescence appliqué à ces deux atomes est élaboré pour calculer les taux de quenching du signal avec la pression et la température. Les données collisionnelles qui sont inconnues sont prédéterminées théoriquement pour Fe et expérimentalement pour Al. Les coefficients de transferts d’énergie et d’élargissements spectraux par collisions de l’atome Al sont déterminés expérimentalement en environnement d’azote pur. Une étude du comportement du signal de Al avec l’énergie laser est effectuée pour mesurer les seuils de saturation avec les gaz N₂, Ar et He en fonction de la pression. Le modèle permet de reproduire correctement les profils temporels et spectraux avec toutefois des approximations et des limitations qui sont explicitées. Une première application de l’imagerie LIF sur Al dans une flamme de propergol solide aluminisé (10 bar et 3000 K) permet de visualiser des gouttes d’aluminium réactives et observer leur évolution dans la flamme.