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Methane plays an important role in the radiative balance of the Earth climate: about 20% of the manmade global warming is related to methane emissions. To contribute to the study of CH trends, we have developed a compact lightweight spectrometer (2.5 kg) by combining an antimonide laser diode at 3.24 µm with an 8 m optical multipass path cell open to the atmosphere. This laser sensor is to be operated from weather balloons to provide with regular in situ methane soundings from ground level up to ~ 25 km. In this paper, the laser sensor is described as well as the processing of the absorption spectra and the calibration of the instrument. The concentration data obtained from recent stratospheric balloon flights are reported and discussed. [ABSTRACT FROM AUTHOR]

In this paper, we discuss the interest of the singular value decomposition (SVD) data processing method applied to the in situ monitoring of gases (NO) b mid-infrared quantum cascade laser absorption spectroscopy. An approach by simulation is used to determine the most appropriate parameters of the SVD treatment for this specific laser sensing application. The simulation is further used to estimate the effectiveness of the SVD in terms of improvement of the concentration data precision. Finally, the proposed SVD method is applied to experimental NO measurements achieved in the laboratory with calibrated gas samples and with NO flux measurements yielded during a field campaign in farm parcels. [ABSTRACT FROM AUTHOR]

The main characteristics that a sensor must possess for trace gas detection and pollution monitoring are high sensitivity, high selectivity and the capability to perform in situ measurements. The photacoustic Helmholtz sensor developed in Reims, used in conjunction with powerful Quantum Cascade Lasers (QCLs), fulfils all these requirements. The best cell response is # 1200 V W−1 cm and the corresponding ultimate sensitivity is j 3.3 × 10−10 W cm−11 Hz−11/2. This efficient sensor is used with mid-infrared QCLs from Alpes Lasers to reach the strong fundamental absorption bands of some atmospheric gases. A first cryogenic QCL emitting at 7.9 μm demonstrates the detection of methane in air with a detection limit of 3 ppb. A detection limit of 20 ppb of NO in air is demonstrated using another cryogenic QCL emitting in the 5.4 μm region. Real in-situ measurements can be achieved only with room-temperature QCLs. A room-temperature QCL emitting in the 7.9 μm region demonstrates the simultaneous detection of methane and nitrous oxide in air (17 and 7 ppb detection limit, respectively). All these reliable measurements allow the estimated detection limit for various atmospheric gases using quantum cascade lasers to be obtained. Each gas absorbing in the infrared may be detected at a detection limit in the ppb or low-ppb range. [ABSTRACT FROM AUTHOR]

A network of remote and in-situ sensors was deployed in a Paris suburb in order to evaluate the mesoscale evolution of the daily cycle of CO2 and related tracers in the atmospheric boundary layer (ABL) and its relation to ABL dynamics and nearby natural and anthropogenic sources and sinks. A 2-μm heterodyne Doppler differential absorption lidar, which combines measurements of, (1) structure of the atmosphere, (2) radial velocity, and (3) CO2 differential absorption was a particularly unique element of the observational array. We analyse the differences in the diurnal cycle of CO, CO2, lidar reflectivity (a proxy for aerosol content) and H2O using the lidar, airborne measurements in the free troposphere and ground-based measurements made at two sites located few kilometres apart. We demonstrate that vertical mixing dominates the early morning drawdown of CO and aerosol content trapped in the former nocturnal layer but not the H2O and CO2 mixing ratio variations. Surface fluxes, vertical mixing and advection all contribute to the ABL CO2 mixing ratio decrease during the morning transition, with the relative importance depending on the rate and timing of ABL rise. We also show evidence that when the ABL is stable, small-scale (0.1-km vertical and 1-km horizontal) gradients of CO2 and CO are large. The results illustrate the complexity of inferring surface fluxes of CO2 from atmospheric budgets in the stable boundary layer. [ABSTRACT FROM AUTHOR]