D. Mondelain

Infrared extension of the supercontinuum generated by femtosecond terawatt laser pulses propagating in the atmosphere

We investigated the spectral behavior of a white-light continuum generated in air by 2-TW femtosecond laser pulses at 800 nm. The spectrum extends at least from 300 nm to 4.5 mum. From 1 to 1.6 mum the continuums intensity increases strongly with the laser energy and depends on the initial chirp.

Backward supercontinuum emission from a filament generated by ultrashort laser pulses in air.

Backward emission of the supercontinuum from a light filament induced by high-intensity femtosecond laser pulses propagating in air has been observed to be enhanced compared with linear Rayleigh-Mie scattering. This enhancement is interpreted as a nonlinear scattering process onto longitudinal refractive-index changes induced by the laser pulse itself. The spectral dependence of the supercontinuum angular distribution is also investigated.

Sonographic probing of laser filaments in air

The acoustic wave emitted from the plasma channel associated with a filament induced by a femtosecond laser pulse in air was detected with a microphone. This sonographic detection provides a new method to determine the length and the spatial profile of the free-electron density of a filament. The acoustic wave is emitted owing to the expansion of the gas in the filament, which is heated through collisions with high-energy photoelectrons generated by multiphoton ionization. Compared with other methods, the acoustic detection is simpler, more sensitive, and with higher spatial resolution, making it suitable for field measurements over kilometer-range distances or laboratory-scale studies on the fine structure of a filament.

Velocity effects on the shape of pure H2O isolated lines: complementary tests of the partially correlated speed-dependent Keilson-Storer model.

Complementary tests of the partially correlated speed-dependent Keilson-Storer (pCSDKS) model for the shape of isolated transition of pure water vapor [N. H. Ngo et al., J. Chem. Phys. 136, 154310 (2012)] are made using new measurements. The latter have been recorded using a high sensitivity cavity ring down spectrometer, for seven self-broadened H(2)O lines in the 1.6 μm region at room temperature and for pressures from 0.5 to 15 Torr. Furthermore, the H(2) (18)O spectra of [M. D. De Vizia et al., Phys. Rev. A 83, 052506 (2011)] in the 1.38 μm region, measured at 273.15 K and for pressures from 0.3 to 3.75 Torr have also been used for comparison with the model. Recall that the pCSDKS model takes into account the collision-induced velocity changes, the speed dependences of the broadening and shifting coefficients as well as the partial correlation between velocity and rotational-state changes. All parameters of the model have been fixed at values previously determined, except for a scaling factor applied to the input speed-dependent line broadening. Comparisons between predictions and experiments have been made by looking at the results obtained when fitting the calculated and measured spectra by Voigt profiles. The good agreement obtained for all considered lines, at different temperature and pressure conditions, confirms the consistency and the robustness of the model. Limiting cases of the model have been then derived, showing the influence of different contributions to the line shape.

3D-air quality model evaluation using the Lidar technique

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.

Temperature dependence of the water vapor self-continuum by cavity ring-down spectroscopy in the 1.6 µm transparency window

The very weak water vapor self-continuum has been investigated by high-sensitivity cavity ring-down spectroscopy in the 1.6 µm window at five temperatures between 302 K and 340 K. The absorption cross sections, Cs(ν, T), were retrieved for 10 selected wave numbers from a fit of the absorption coefficients measured in real time during pressure ramps, after subtraction of the contributions of the local water monomer lines and of water adsorbed on the cell mirrors. The values measured between 5875 and 6665 cm−1 range between 1.5 × 10−25 and 2 × 10−24 cm2 mol−1 atm−1 with a minimum around 6300 cm−1. At 302 K, an agreement within 50% is observed over the whole window with the cross sections provided by the MT_CKD V2.5 model. Nevertheless, while our measurements show that the Cs(ν, T) decrease from 302 K to 340 K is no more than 50% for all our selected wave numbers, the MT_CKD V2.5 model predicts a much more pronounced temperature dependence in the center of the window, the agreement being better on the edges of the window. The obtained results are discussed in relation with theoretical modeling of the water vapor self-continuum as far wings of monomer lines or water dimer absorption. For potential atmospheric applications, cross sections are provided at each temperature with a sampling step of 10 cm−1 for the entire 5850–6700 cm−1 range.

Accurate measurements and temperature dependence of the water vapor self-continuum absorption in the 2.1 μm atmospheric window

In spite of its importance for the evaluation of the Earth radiative budget, thus for climate change, very few measurements of the water vapor continuum are available in the near infrared atmospheric windows especially at temperature conditions relevant for our atmosphere. In addition, as a result of the difficulty to measure weak broadband absorption signals, the few available measurements show large disagreements. We report here accurate measurements of the water vapor self-continuum absorption in the 2.1 μm window by Optical Feedback Cavity Enhanced Absorption Spectroscopy (OF-CEAS) for two spectral points located at the low energy edge and at the center of the 2.1 μm transparency window, at 4302 and 4723 cm(-1), respectively. Self-continuum cross sections, CS, were retrieved with a few % relative uncertainty, from the quadratic dependence of the spectrum base line level measured as a function of water vapor pressure, between 0 and 16 Torr. At 296 K, the CS value at 4302 cm(-1) is found 40% higher than predicted by the MT_CKD V2.5 model, while at 4723 cm(-1), our value is 5 times larger than the MT_CKD value. On the other hand, these OF-CEAS CS values are significantly smaller than recent measurements by Fourier transform spectroscopy at room temperature. The temperature dependence of the self-continuum cross sections was also investigated for temperatures between 296 K and 323 K (23-50 °C). The derived temperature variation is found to be similar to that derived from previous Fourier transform spectrometer (FTS) measurements performed at higher temperatures, between 350 K and 472 K. The whole set of measurements spanning the 296-472 K temperature range follows a simple exponential law in 1/T with a slope close to the dissociation energy of the water dimer, D0 ≈ 1100 cm(-1).

CRDS with a VECSEL for broad-band high sensitivity spectroscopy in the 2.3 μm window

The integration of an industry ready packaged Sb-based Vertical-External-Cavity Surface-Emitting-Laser (VECSEL) into a Cavity Ring Down Spectrometer (CRDS) is presented. The instrument operates in the important 2.3 μm atmospheric transparency window and provides a high sensitivity (minimum detectable absorption of 9 × 10(-11) cm(-1)) over a wide spectra range. The VECSEL performances combine a large continuous tunability over 120 cm(-1) around 4300 cm(-1) together with a powerful (∼5 mW) TEM00 diffraction limited beam and linewidth at MHz level (for 1 ms of integration time). The achieved performances are illustrated by high sensitivity recordings of the very weak absorption spectrum of water vapor in the region. The developed method gives potential access to the 2-2.7 μm range for CRDS.

Accurate laboratory determination of the near‐infrared water vapor self‐continuum: A test of the MT_CKD model

The semi empirical MT_CKD model of the absorption continuum of water vapor is widely used in atmospheric radiative transfer codes of the atmosphere of Earth and, recently, of exoplanets, but lacks of experimental validation in the atmospheric windows. Recent laboratory measurements by Fourier transform Spectroscopy led to self-continuum cross-sections much larger than the MT_CKD values in the near infrared transparency windows. We report on accurate measurements by Cavity Ring Down Spectroscopy (CRDS) and Optical-Feedback-Cavity Enhanced Laser Spectroscopy (OF-CEAS) at selected spectral points of the transparency windows centered around 4.0, 2.1 and 1.25 µm. The temperature dependence of the absorption continuum at 4.38 µm is measured in the 23-39 °C range. The self-continuum water vapor absorption is derived either from the baseline variation of water vapor spectra recorded for a series of pressure values over a small spectral interval or from baseline monitoring at fixed laser frequency during pressure ramps. After subtraction of the local water monomer lines contribution, self-continuum cross-sections, CS, are determined with an accuracy better than 10% from the pressure squared dependence of the continuum absorption measured up to about 15 Torr. Together with our previous measurements in the 2.1 and 1.6 µm windows, the present results provide a unique set of water vapor cross-sections for testing the MT_CKD model in four transparency windows. Although showing some important deviations of the absolute values (up to about a factor 4), our accurate measurements validate the overall frequency dependence of the most recent version (V2.8) of the MT_CKD model.

Highly excited vibrational states of 18O3 as a test of the ozone potential energy surface

This work is a part of our systematic investigation of the very weak absorption spectra of 16O3 and 18O3 by high sensitivity Cavity Ring Down Spectroscopy between 5850 and 7920 cm-1. In total, 29 vibrational bands of 16O3 and 24 bands of 18O3 have been assigned in this range. Here we present the recent results of analyses of highly excited states of 18O3 ozone, located near the dissociation energy (D0~8560 cm-1). The comparison of the vibrational band centers obtained from the analysis with the predictions based on the potential energy surface (PES) suggests that the hypothesis of the “reef structure” at the ozone transition state towards the dissociation is not confirmed by spectroscopic observations. In this work, we focus on the comparison between theoretical and experimental values of the 18O3 vibrational levels near the dissociation limit.