Search

We report in this paper the development of an embedded ultralight spectrometer (<3 kg) based on tuneable diode laser absorption spectroscopy (with a sampling rate of 24 Hz) in the mid-infrared spectral region. This instrument is dedicated to in situ measurements of the vertical profile concentrations of three main greenhouse gases – carbon dioxide (CO2), methane (CH4) and water vapour (H2O) – via standard weather and tethered balloons. The plug and play instrument is compact, robust, cost-effective, and autonomous. The instrument also has low power consumption and is non-intrusive. It was first calibrated during an in situ experiment on an ICOS (Integrated Carbon Observation System) site for several days, then used in two experiments with several balloon flights of up to 30 km altitude in the Reims region of France in 2017–2018 in collaboration with Météo-France CNRM (Centre National de Recherches Météorologiques). This paper shows the valuable interest of the data measured by the AMULSE (Atmospheric Measurements by Ultra-Light Spectrometer) instrument during the APOGEE (Atmospheric Profiles of Greenhouse Gases) measurement experiment, specifically for the vertical profiles of CO2 and CH4 , measurements of which remain very sparse. We have carried out several experiments showing that the measured profiles have several applications: the validation of simulations of infrared satellite observations, evaluating the quality of chemical profiles from chemistry transport models (CTMs) and evaluating the quality of retrieved chemical profiles from the assimilation of infrared satellite observations. The results show that the simulations of infrared satellite observations from IASI (Infrared Atmospheric Sounding Interferometer) and CrIS (Cross-track Infrared Sounder) instruments performed in operational mode for numerical weather prediction (NWP) by the radiative transfer model (RTM) RTTOV (Radiative Transfer for the TIROS Operational Vertical Sounder) are of good quality. We also show that the MOCAGE (Modèle de Chimie Atmosphérique de Grande Echelle) and CAMS (Copernicus Atmospheric Monitoring Service) CTMs modelled ozone profiles fairly accurately and that the CAMS CTM represents the methane in the troposphere well compared to MOCAGE. Finally, the measured in situ ozone profiles allowed us to show the good quality of the retrieved ozone profiles by assimilating ozone-sensitive infrared spectral radiances from the IASI and CrIS. [ABSTRACT FROM AUTHOR]

Atmospheric aerosol optical, physical, and chemical properties play a fundamental role in the Earth's climate system. A better understanding of the processes involved in their formation, evolution, and interaction with radiation and the water cycle is critical. We report the analysis of atmospheric molecules/particles collected with a new sampling system that flew under regular weather balloons for the first time. The flight took place on January 18, 2022 from Reims (France). The samples were subsequently analyzed by high-resolution mass spectrometry (Orbitrap) to specifically infer hundreds of organic components present in 4 different layers from the troposphere to the stratosphere (up to 20 km). Additional measurements of O 3 , CO, and aerosol concentrations a few hours before this flight took place to contextualize the sampling. After separating common species found on each filter that might be common to atmospheric layers or residuals for contaminations, we found that each sample yields significant differences in the number and size of organic species detected that should reflect the unique composition of atmospheric layers. While tropospheric samples yield significantly oxidized and saturated components, with carbon numbers below 30 that might be explained by complex organics chemistry from local and distant source emissions, the upper tropospheric and stratospheric samples were associated with increased carbon numbers (C > 30), with a significantly reduced unsaturation number for the stratosphere, that might be induced by strong UV radiations. The multimodal distributions of carbon numbers in chemical formulas observed between 15 and 20 km suggest that oligomerization and growth of organic molecules may take place in aged air masses of tropical origin that are known to carry organic compounds even several km above the tropopause where their lifetime significantly increases. In addition, the presence of organics may also reflect the extended influence of wildfires smoke injected during the spring and summer in the NH hemisphere before the in situ observations and their long-lifetime in the upper troposphere and stratosphere. Photographic credit: Marc Fourmentin - Laboratoire de PhysicoChimie de l'Atmosphère. [Display omitted] • Unique launching infrastructure in Europe (Reims/France) to operate state-of-the art atmospheric instruments • New balloon-borne sampling device to characterize the chemical composition of organics (troposphere to stratosphere) • Offline analysis reveals the growth of organics aerosol in the stratosphere • Organics aerosol could derive from oligomerization processes along transport from the tropics and/or influenced by wildfires [ABSTRACT FROM AUTHOR]