The first balloon-borne sample analysis of atmospheric carbonaceous components reveals new insights into formation processes.

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 O3, 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.

Vertical distribution of aerosols in dust storms during the Arctic winter.

High Latitude Dust (HLD) contributes 5% to the global dust budget, but HLD measurements are sparse. Dust observations from Iceland provide dust aerosol distributions during the Arctic winter for the first time, profiling dust storms as well as clean air conditions. Five winter dust storms were captured during harsh conditions. Mean number concentrations during the non-dust flights were <5 particles cm-3 for the particles 0.2-100 µm in diameter and >40 particles cm-3 during dust storms. A moderate dust storm with >250 particles cm-3 (2 km altitude) was captured on 10th January 2016 as a result of sediments suspended from glacial outburst flood Skaftahlaup in 2015. Similar concentrations were reported previously in the Saharan air layer. Detected particle sizes were up to 20 µm close to the surface, up to 10 µm at 900 m altitude, up to 5 µm at 5 km altitude, and submicron at altitudes >6 km. Dust sources in the Arctic are active during the winter and produce large amounts of particulate matter dispersed over long distances and high altitudes. HLD contributes to Arctic air pollution and has the potential to influence ice nucleation in mixed-phase clouds and Arctic amplification.

Optical and physical properties of stratospheric aerosols from balloon measurements in the visible and near-infrared domains. III. Presence of aerosols in the middle stratosphere.

The aerosol extinction measurements in the ultraviolet and visible wavelengths by the balloonborne spectrometer Spectroscopie d'Absorption Lunaire pour l'Observation des Minoritaires Ozone et NOx (SALOMON) show that aerosols are present in the middle stratosphere, above 25-km altitude. These observations are confirmed by the extinction measurements performed by a solar occultation radiometer. The balloonborne Laboratoire de Météorologie Dynamique (LMD) counter instrument also confirms the presence of aerosol around 30-km altitude, with an unrealistic excess of micronic particles assuming that only liquid sulfate aerosols are present. An unexpected spectral structure around 640-nm observed by SALOMON is also detectable in extinction measurements by the satellite instrument Stratospheric Aerosols and Gas Experiment III. This set of measurements could indicate that solid aerosols were detected at these altitude ranges. The amount of soot detected up to now in the lower stratosphere is too low to explain these measurements. Thus, the presence of interplanetary dust grains and micrometeorites may need to be invoked. Moreover, it seems that these grains fill the stratosphere in stratified layers.

Optical and physical properties of stratospheric aerosols from balloon measurements in the visible and near-infrared domains. 1. Analysis of aerosol extinction spectra from the AMON and SALOMON balloonborne spectrometers.

Aerosol extinction coefficients have been derived in the 375-700-nm spectral domain from measurement in the stratosphere since 1992, at night, at mid- and high latitudes from 15 to 40 km, by two balloonborne spectrometers, Absorption par les Minoritaires Ozone et NO(chi) (AMON) and Spectroscopie d'Absorption Lunaire pour l'Observation des Minoritaires Ozone et NO(chi) (SALOMON). Log-normal size distributions associated with the Mie-computed extinction spectra that best fit the measurements permit calculation of integrated properties of the distributions. Although measured extinction spectra that correspond to background aerosols can be reproduced by the Mie scattering model by use of monomodal log-normal size distributions, each flight reveals some large discrepancies between measurement and theory at several altitudes. The agreement between measured and Mie-calculated extinction spectra is significantly improved by use of bimodal log-normal distributions. Nevertheless, neither monomodal nor bimodal distributions permit correct reproduction of some of the measured extinction shapes, especially for the 26 February 1997 AMON flight, which exhibited spectral behavior attributed to particles from a polar stratospheric cloud event.

Optical and physical properties of stratospheric aerosols from balloon measurements in the visible and near-infrared domains. II. Comparison of extinction, reflectance, polarization, and counting measurements.

The physical properties of stratospheric aerosols can be retrieved from optical measurements involving extinction, radiance, polarization, and counting. We present here the results of measurements from the balloonborne instruments AMON, SALOMON, and RADIBAL, and from the French Laboratoire de Météorologie Dynamique and the University of Wyoming balloonborne particle counters. A cross comparison of the measurements was made for observations of background aerosols conducted during the polar winters of February 1997 and January-February 2000 for various altitudes from 13 to 19 km. On the one band, the effective radius and the total amount of background aerosols derived from the various sets of data are similar and are in agreement with pre-Pinatubo values. On the other hand, strong discrepancies occur in the shapes of the bimodal size distributions obtained from analysis of the raw measurement of the various instruments. It seems then that the log-normal assumption cannot fully reproduce the size distribution of background aerosols. The effect ofthe presence of particular aerosols on the measurements is discussed, and a new strategy for observations is proposed.