Sulfur mass loading of the atmosphere from volcanic eruptions: Calibration of the ice core record on basis of sulfate aerosol deposition in polar regions from the 1982 El Chichon eruption

Major volcanic eruptions disperse large quantities of sulfur compound throughout the Earth's atmosphere. The sulfuric acid aerosols resulting from such eruptions are scavenged by snow within the polar regions and appear in polar ice cores as elevated acidity layers. Glacio-chemical studies of ice cores can, thus, provide a record of past volcanism, as well as the means for understanding the fate of volcanic sulfur in the atmosphere. The primary objectives of this project are to study the chemistry and physical properties of volcanic fallout in a Greenland Ice Core in order to evaluate the impact of the volcanic gases on the atmospheric chemistry and the total atmospheric mass of volcanic aerosols emitted by major volcanic eruptions. We propose to compare the ice core record to other atmospheric records performed during the last 10 years to investigate transport and deposition of volcanic materials

Cn to ccn relationships and cloud microphysical properties in different air masses at a free tropospheric site

International audienceThe fraction of aerosol particles activated to droplets (CCN) is often derived from semi-empirical relationships that commonly tend to overestimate droplet number concentration leading to major uncertainties in global climate models. One of the difficulties in relating aerosol concentration to cloud microphysics and cloud albedo lies in the necessity of working at a constant liquid water path (LWP), which is very difficult to control. In this study we observed the relationships between aerosol number concentration (NCN), cloud droplet concentration (Nd) and effective radius (Reff), at the Puy de Dôme (France). A total of 20 cloud events were sampled representing a period of more than 250 h of cloud sampling. Samples are classified first according to air mass origins (Modified Marine, Continental and Polluted) and then according to their liquid water content (Thin, Medium and Thick clouds). The CCN fraction of aerosols appears to vary significantly according to the air mass origin. It is maximum for Continental air masses and minimum for Polluted air masses. Surprisingly, the CCN fraction of Modified Marine air masses fraction is lower than the continental air mass and from expected from previous studies. The limited number of activated particles in Modified Marine air masses is most likely the result of the presence of hydrophobic organic compounds. The limited activation effect leads to a 0.5 to 1 µm increase in Reff with respect to an ideal Marine case. This is significant and implies that the dReff/dNCN of low-continental clouds is higher than expected

Sulfate alters aerosol absorption properties in East Asian outflow

Black carbon (BC) and brown carbon (BrC) aerosols that are released from the combustion of fossil fuels and biomass are of great concern because of their light-absorbing ability and great abundance associated with various anthropogenic sources, particularly in East Asia. However, the optical properties of ambient aerosols are dependent on the mixing state and the chemical composition of absorbing and non-absorbing aerosols. Here we examined how, in East Asian outflows, the parameters of the aerosol optical properties can be altered seasonally in conjunction with the mixing state and the chemical composition of aerosols, using 3-year aerosol measurements. Our findings highlight the important role played by sulfate in East Asia during the warm season in both enhancing single scattering albedo (SSA) and altering the absorption properties of aerosols-enhancing mass absorption cross section of BC (MAC(BC)) and reducing MAC of BrC (MAC(BrC),(370)). Therefore we suggest that in global radiative forcing models, particular attention should be paid to the consideration of the accurate treatment of the SO2 emission changes in the coming years in this region that will result from China's air quality policy.Peer reviewe

Evolution récente des glaciers du Pamir-Karakoram-Himalaya (apport de l'imagerie satellite)

La région du Pamir - Karakoram - Himalaya (PKH) constitue la plus grande réserve de glace terrestre après les régions polaires. Cependant, l'évolution récente de ces glaciers, indicateurs privilégiés du changement climatique en haute altitude, reste encore mal connue, du fait notamment de difficultés d'accès et de conditions climatiques qui rendent délicate l'acquisition de mesures in situ. L'objectif de cette thèse est de contribuer à l'amélioration des connaissances sur l'évolution globale des glaces du PKH au cours de la dernière décennie, en s'appuyant sur des images satellite et des modèles numériques de terrain (MNTs). Une premièreméthodologie a été développée pour assurer le suivi automatique de la distribution spatiale et de l'évolution temporelle des lacs glaciaires à partir d'images Landsat entre 1990 et 2009 sur sept zones d'études réparties le long du PKH. Ainsi, une certaine disparité des types, tailles et évolutions des lacs entre la partie orientale et occidentale du PKH a été mise en évidence. Sur la période de temps considérée, la superficie des lacs a légèrement diminué à l'ouest (Karakoram et Hindu Kush), a été en très nette augmentation à l'est (Népal et Bouthan) et relativement stable sur la partie centrale (Inde du nord-ouest). Le bilan de masse des glaciers a ensuite été calculé, à partir des variations d'épaisseurs mesurées en comparant deuxMNTs, acquis à deux dates différentes, et issus de lamission SRTM et du satellite SPOT5. Cette méthode implique un certain nombre de corrections et d'ajustements au préalable, afin de garantir des mesures les moins biaisées possible. Ainsi, la différence de résolution spatiale initiale des MNTs peut être à l'origine d'un biais fonction de l'altitude, de même que la pénétration des ondes radar de la mission SRTM dans la neige et la glace est à prendre en compte le cas échéant, pour ne pas sous-estimer les altitudes sur les glaciers. Là encore, on observe des disparités entre les différents bilans de masse régionaux sur la période 1999-2011, avec des pertes de masse modérées sur l'Himalaya central et oriental(-0.30+-0.08 m a-1 w.e.), plus accentuées sur l'Himalaya occidental (-0.43+-0.09 m a-1 w.e.) et des gains de masse plus à l'ouest, pour les glaciers des massifs du Pamir (+0.14+-0.11 m a-1 w.e.) et du Karakoram (+0.10+-0.20 m a-1 w.e.). Ces résultats confirment donc l'anomalie des glaciers du Karakoram et suggèrent des comportements similaires au Pamir. Le bilan de masse global des glaciers du PKH est estimé à -0.13+-0.06 m a-1 w.e.The Pamir - Karakoram - Himalaya (PKH) mountain range is considered to be the largest terrestrial ice reservoir outside polar regions. However, the recent evolution of these glaciers, recognized as valuable high-altitude climatic indicators, remains poorly known, mainly because of accessibility issues and harsh meteorologic conditions that hamper field work and in situ observations. The aim of this thesis is therefore to improve the knowledge of glacier changes in PKH and study their evolution over the past decade, based on satellite images and digital elevation models (DEMs). We first developed automatic classification algorithms to monitor the spatial distribution and temporal evolution of glacial lakes between 1990 and 2009 along the PKH, based on Landsat images. We thereby highlight different types, sizes and evolutions of glacial lakes between eastern and western PKH. During the study period the total glacial lake area slightly decreased in the west (Hindu Kush and Karakoram), greatly increased in the east (Nepal, Bhutan) and remained stable in the central part (north-west India). We then computed the mass balance of PKH glaciers from elevation changes measured by comparing two DEMs, acquired 10 years appart, by the SRTM mission and the SPOT5 satellite. This method relies on a precise relative adjustment (horizontal and vertical) of the DEMs to remove possible systematic biases within glacier elevation changes. The difference in the original spatial resolution of the DEMs can result in an elevation-dependent bias, as well as the radar penetration into snow and ice can seriously underestimate glacier elevation in the case of a DEM derived from radar data such as SRTM. The spatial pattern of regional glacier mass balances between 1999 and 2011 turns out to be contrasted, with moderatemass losses in eastern and central Himalaya (-0.30+-0.08m yr-1 w.e.), stronger in western Himalaya (-0.43+-0.09 m yr-1 w.e.) and mass gains further west, for Pamir(+0.14+-0.11 m yr-1 w.e.) and Karakoram glaciers (+0.10+-0.20 m yr-1 w.e.). The global mass balance of PKH glaciers is estimated at -0.13+-0.06 m yr-1 w.e.SAVOIE-SCD - Bib.électronique (730659901) / SudocGRENOBLE1/INP-Bib.électronique (384210012) / SudocGRENOBLE2/3-Bib.électronique (384219901) / SudocSudocFranceF

A fate for organic acids, formaldehyde and methanol in cloud water: their biotransformation by micro-organisms

International audienceThe interactions between microbial and chemical contents of cloud water were investigated. First, we observe that the bulk cloud water solution provides a substantial environment where bacteria can develop significantly. Then, a total number of 60 microbial strains originating from seven distinct samples of cloud water and affiliated to various taxonomic groups were looked for their ability to degrade some of the main atmospheric carboxylic compounds: formate, acetate, lactate, succinate, formaldehyde and methanol. Biodegradation tests show that all these compounds can be transformed when used as single carbonaceous substrates, with activities depending on both the strain and the compound. The highest capacities of biodegradation are observed towards formaldehyde, formate and acetate, which are also the more concentrated compounds typically measured in cloud water. Hence, analyses by 1H NMR permitted to establish for instance that compounds like pyruvate or fumarate can be produced and released in the media in relation to the transformation of lactate or succinate. In addition, utilization of 13C labelled formaldehyde showed that it can be transformed through many metabolic pathways, similar to those induced by photochemistry and leading to the production of formate and/or methanol. These results suggest that microorganisms of cloud water can have various behaviours towards the chemical compounds present in the atmosphere: they can represent either a sink or source for organic carbon, and may have to be considered as actors of cloud chemistry

Regional characteristics of fine aerosol mass increase elucidated from long-term observations and KORUS-AQ campaign at a Northeast Asian background site

Funding Information: This research was supported by the National Research Foundation of Korea (NRF), funded by the Ministry of Science and ICT (MSIT) (NRF2020M3G1A111499813). S. Lim was supported by the National Research Foundation of Korea (NRF) from the Ministry of Science and ICT (2018R1D1A1B07050849 and 2021R1C1C2011543). M. Lee thanks to the support by the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (NRF2020R1A2C301459213). S.-W. Kim was supported by the Basic Science Research Program through the National Research Foundation of Korea (NRF), funded by the Ministry of Education (2017R1D1A1B06032548). Funding to K.-S. Kang was provided by the National Institute of Environmental Research (NIER-RP2017-166). Funding Information: This research was supported by the National Research Foundation of Korea (NRF), funded by the Ministry of Science and ICT (MSIT) (NRF2020M3G1A111499813). S. Lim was supported by the National Research Foundation of Korea (NRF) from the Ministry of Science and ICT (2018R1D1A1B07050849 and 2021R1C1C2011543). M. Lee thanks to the support by the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (NRF2020R1A2C301459213). S.-W. Kim was supported by the Basic Science Research Program through the National Research Foundation of Korea (NRF), funded by the Ministry of Education (2017R1D1A1B06032548). Funding to K.-S. Kang was provided by the National Institute of Environmental Research (NIER-RP2017-166). Publisher Copyright: © 2022 The Author(s)Northeast Asia has suffered from severe PM2.5 pollution and the exact mechanisms have yet to be fully understood. Here, we investigated the transformation processes of submicron aerosols using a 4-year data set obtained at Jeju, a Northeast Asian background site. The diurnal-cycle constrained empirical orthogonal function analysis of nanoparticle size-number distribution distinguished 2 modes: burst of nucleation-Aitken particles and increase in accumulation mode particles, representing “new particle formation and growth” and “PM2.5 mass increase,” respectively. In these events, aerosol and meteorological characteristics changed progressively over several days, revealing that the PM2.5 mass increase is an episodic event occurring on a regional scale. The increase in PM2.5 mass was accompanied by an increase in aerosol liquid water content, which correlated well with SO4-2 and NO3, and a decrease in incoming solar radiation (-14.1 Wm-2 day-1) constituting a positive feedback. The “transport/haze” episode of KOREA-U.S. Air Quality campaign corresponds to “PM2.5 mass increase,” during which the vertical evolution of particles demonstrates that nanoparticles ≥3.5 nm were entrained into the shallow boundary layer upon vertical mixing and converted to accumulation-mode particles ≥0.3 mm at relative humidity (RH) exceeding the deliquescence RH of secondary inorganic aerosol (SIA). Coincidently, at ground, the coating thickness of refractory black carbon (rBC) (48 ± 39 nm) and SIA concentration increased. Furthermore, the diameter of rBC (180-220 nm)-containing particle in core-shell configuration linearly increased with PM2.5 mass, reaching 300-400 nm at PM2.5 ≥ 40 mg m-3.This observational evidence suggests that the thick coating of rBCs resulted from the active conversion of condensable gases into the particulate phase on the rBC surface, thereby increasing the mass of the accumulation-mode aerosol. Consequently, this result complies with the strategy to reduce primary emissions of gaseous precursors for SIA and particulates such as rBC as a way to effectively mitigate haze pollution as well as climate change in Northeast Asia.Peer reviewe

Microbial population in cloud water at the Puy de Dôme: implications for the chemistry of clouds

Airborne micro-organisms are ubiquitous in the atmosphere where they can remain alive and be transported over long distances, thus colonizing new environments. Despite their great importance in relation to ecological and socio-economical issues (bio-terrorism, health, etc.) very few studies have been carried out in this field. In this study, the structure of the microbial community present in atmospheric water samples from clouds at the Puy de Dôme (alt 1465 m, Massif Central, France) is described and the metabolic potential of some bacteria is investigated. The total microflora has been quantified by epifluorescence microscopy, while the cultivable aerobic micro-organisms were isolated. Bacteria were identified by 16S DNA sequencing and fungi by morphological criteria. The total bacterial count reached about 3×104 cells m−3 of cloud volume (1×105 cells mL−1 of cloud water), of which less than 1% are cultivable. Most of the isolated micro-organisms, including 12 fungal and 17 bacterial strains, are described here for the first time in atmospheric water. Many bacterial strains seem to be adapted to the extreme conditions found in cloud water (pH, T°, UV radiations, etc.). Comparison of the two samples (March 2003) shows that pH can be a major factor controlling the structure of this community: an acidic pH (Sample 1: pH=4, 9) favours the presence of fungi and spore-forming bacteria, while a more neutral pH (Sample 2: pH=5, 8) favours greater biodiversity. We have also shown, using in situ 1H NMR, that most of the isolated bacteria are able to degrade various organic substrates such as formate, acetate, lactate, methanol and formaldehyde which represent the major organic compounds present in cloud water. In addition, the detection of intermediates indicated preferential metabolic routes for some of the strains