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Author Angot, H., Magand, O., Helmig, D., Ricaud, P., Quennehen, B., Gallée, H., Del Guasta, M., Sprovieri, F., Pirrone, N., Savarino, J., Dommergue, A. doi  openurl
  Title New insights into the atmospheric mercury cycling in central Antarctica and implications on a continental scale Type Journal Article
  Year 2016 Publication Atmospheric chemistry and physics Abbreviated Journal  
  Volume 16 Issue 13 Pages 8249-8264  
  Keywords  
  Abstract Under the framework of the GMOS project (Global Mercury Observation System) atmospheric mercury monitoring has been implemented at Concordia Station on the high-altitude Antarctic plateau (75°06′ S, 123°20′ E, 3220 m above sea level). We report here the first year-round measurements of gaseous elemental mercury (Hg(0)) in the atmosphere and in snowpack interstitial air on the East Antarctic ice sheet. This unique data set shows evidence of an intense oxidation of atmospheric Hg(0) in summer (24-hour daylight) due to the high oxidative capacity of the Antarctic plateau atmosphere in this period of the year. Summertime Hg(0) concentrations exhibited a pronounced daily cycle in ambient air with maximal concentrations around midday. Photochemical reactions and chemical exchange at the air–snow interface were prominent, highlighting the role of the snowpack on the atmospheric mercury cycle. Our observations reveal a 20 to 30 % decrease of atmospheric Hg(0) concentrations from May to mid-August (winter, 24 h darkness). This phenomenon has not been reported elsewhere and possibly results from the dry deposition of Hg(0) onto the snowpack. We also reveal the occurrence of multi-day to weeklong atmospheric Hg(0) depletion events in summer, not associated with depletions of ozone, and likely due to a stagnation of air masses above the plateau triggering an accumulation of oxidants within the shallow boundary layer. Our observations suggest that the inland atmospheric reservoir is depleted in Hg(0) in summer. Due to katabatic winds flowing out from the Antarctic plateau down the steep vertical drops along the coast and according to observations at coastal Antarctic stations, the striking reactivity observed on the plateau most likely influences the cycle of atmospheric mercury on a continental scale.  
  Programme 1028  
  Campaign  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Summary Language Original Title  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1680-7316 ISBN Medium  
  Area Expedition Conference  
  Notes Approved yes  
  Call Number Serial 6561  
Permanent link to this record
 

 
Author H. Angot, O. Magand, D. Helmig, P. Ricaud, B. Quennehen, H. Gallée, M. Del Guasta, F. Sprovieri, N. Pirrone, J. Savarino, A. Dommergue doi  isbn
openurl 
  Title New insights into the atmospheric mercury cycling in central Antarctica and implications on a continental scale Type Journal
  Year 2016 Publication Atmos. chem. phys. Abbreviated Journal  
  Volume 16 Issue 13 Pages 8249-8264  
  Keywords  
  Abstract Under the framework of the GMOS project (Global Mercury Observation System) atmospheric mercury monitoring has been implemented at Concordia Station on the high-altitude Antarctic plateau (75°06′ S, 123°20′ E, 3220 m above sea level). We report here the first year-round measurements of gaseous elemental mercury (Hg(0)) in the atmosphere and in snowpack interstitial air on the East Antarctic ice sheet. This unique data set shows evidence of an intense oxidation of atmospheric Hg(0) in summer (24-hour daylight) due to the high oxidative capacity of the Antarctic plateau atmosphere in this period of the year. Summertime Hg(0) concentrations exhibited a pronounced daily cycle in ambient air with maximal concentrations around midday. Photochemical reactions and chemical exchange at the air–snow interface were prominent, highlighting the role of the snowpack on the atmospheric mercury cycle. Our observations reveal a 20 to 30 % decrease of atmospheric Hg(0) concentrations from May to mid-August (winter, 24 h darkness). This phenomenon has not been reported elsewhere and possibly results from the dry deposition of Hg(0) onto the snowpack. We also reveal the occurrence of multi-day to weeklong atmospheric Hg(0) depletion events in summer, not associated with depletions of ozone, and likely due to a stagnation of air masses above the plateau triggering an accumulation of oxidants within the shallow boundary layer. Our observations suggest that the inland atmospheric reservoir is depleted in Hg(0) in summer. Due to katabatic winds flowing out from the Antarctic plateau down the steep vertical drops along the coast and according to observations at coastal Antarctic stations, the striking reactivity observed on the plateau most likely influences the cycle of atmospheric mercury on a continental scale.  
  Programme 1028  
  Campaign  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Summary Language Original Title  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1680-7324 ISBN 1680-7324 Medium  
  Area Expedition Conference  
  Notes Approved yes  
  Call Number Serial 6591  
Permanent link to this record
 

 
Author Legrand, M., Preunkert, S., Savarino, J., Frey, M. M., Kukui, A., Helmig, D., Jourdain, B., Jones, A., Weller, R., Brough, N., and Gallée, H doi  openurl
  Title Inter-annual variability of surface ozone at coastal (Dumont d’Urville, 2004-014) and inland (Concordia, 2007-2014) sites in East Antarctica Type Journal Article
  Year 2016 Publication Atmospheric chemistry and physics Abbreviated Journal  
  Volume 16 Issue 12 Pages 8053-8069  
  Keywords  
  Abstract Surface ozone has been measured since 2004 at the coastal East Antarctic site of Dumont d'Urville (DDU), and since 2007 at the Concordia station located on the high East Antarctic plateau. This paper discusses long-term changes, seasonal and diurnal cycles, as well as inter-annual summer variability observed at these two East Antarctic sites. At Concordia, near-surface ozone data were complemented by balloon soundings and compared to similar measurements done at the South Pole. The DDU record is compared to those obtained at the coastal site of Syowa, also located in East Antarctica, as well as the coastal sites of Neumayer and Halley, both located on the coast of the Weddell Sea in West Antarctica. Surface ozone mixing ratios exhibit very similar seasonal cycles at Concordia and the South Pole. However, in summer the diurnal cycle of ozone is different at the two sites with a drop of ozone in the afternoon at Concordia but not at the South Pole. The vertical distribution of ozone above the snow surface also differs. When present, the ozone-rich layer located near the ground is better mixed and deeper at Concordia (up to 400 m) than at the South Pole during sunlight hours. These differences are related to different solar radiation and wind regimes encountered at these two inland sites. DDU appears to be the coastal site where the impact of the late winter/spring bromine chemistry is the weakest, but where the impact of elevated ozone levels caused by NOx snow emissions from the high Antarctic plateau is the highest. The highest impact of the bromine chemistry is seen at Halley and Neumayer, and to a lesser extent at Syowa. These three sites are only weakly impacted by the NOx chemistry and the net ozone production occurring on the high Antarctic plateau. The differences in late winter/spring are attributed to the abundance of sea ice offshore from the sites, whereas those in summer are related to the topography of East Antarctica that promotes the katabatic flow bringing oxidant-rich inland air masses to the site. There appears to be a decreasing change in summer surface ozone at the two East Antarctic sites of Concordia and DDU over the most recent period (2004–2014 and 2007–2014). Further research, including continued monitoring, is needed at these two sites to better separate the effect of synoptic transport from possible change of NOx snow emissions in response to recovery of the stratospheric ozone layer leading to penetration of more UV radiation to the surface.  
  Programme 414  
  Campaign  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Summary Language Original Title  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1680-7316 ISBN Medium  
  Area Expedition Conference  
  Notes Approved yes  
  Call Number Serial 6542  
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Author T. Dinh, A. Podglajen, A. Hertzog, B. Legras, R. Plougonven doi  openurl
  Title Effect of gravity wave temperature fluctuations on homogeneous ice nucleation in the tropical tropopause layer Type Journal
  Year 2016 Publication Atmospheric Chemistry and Physics Abbreviated Journal  
  Volume 16 Issue 1 Pages 35-46  
  Keywords  
  Abstract The impact of high-frequency fluctuations of temperature on homogeneous nucleation of ice crystals in the vicinity of the tropical tropopause is investigated using a bin microphysics scheme for air parcels. The imposed temperature fluctuations come from measurements during isopycnic balloon flights near the tropical tropopause. The balloons collected data at high frequency, guaranteeing that gravity wave signals are well resolved.

With the observed temperature time series, the numerical simulations with homogeneous freezing show a full range of ice number concentration (INC) as previously observed in the tropical upper troposphere. In particular, a low INC may be obtained if the gravity wave perturbations produce a non-persistent cooling rate (even with large magnitude) such that the absolute change in temperature remains small during nucleation. This result is explained analytically by a dependence of the INC on the absolute drop in temperature (and not on the cooling rate). This work suggests that homogeneous ice nucleation is not necessarily inconsistent with observations of low INCs.

 
  Programme 914  
  Campaign  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Summary Language Original Title  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1680-7316 ISBN Medium  
  Area Expedition Conference  
  Notes Approved yes  
  Call Number Serial 8280  
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Author J. Bock, J. Savarino, G. Picard doi  isbn
openurl 
  Title Air–snow exchange of nitrate: a modelling approach to investigate physicochemical processes in surface snow at Dome C, Antarctica Type Journal
  Year 2016 Publication Atmos. Chem. Phys. Abbreviated Journal  
  Volume 16 Issue 19 Pages 12531-12550  
  Keywords  
  Abstract Snowpack is a multiphase (photo)chemical reactor that strongly influences the air composition in polar and snow-covered regions. Snowpack plays a special role in the nitrogen cycle, as it has been shown that nitrate undergoes numerous recycling stages (including photolysis) in the snow before being permanently buried in the ice. However, the current understanding of these physicochemical processes remains very poor. Several modelling studies have attempted to reproduce (photo)chemical reactions inside snow grains, but these have relied on strong assumptions to characterise snow reactive properties, which are not well defined. Air–snow exchange processes such as adsorption, solid-state diffusion, or co-condensation also affect snow chemical composition. Here, we present a physically based model of these processes for nitrate. Using as input a 1-year-long time series of atmospheric nitrate concentration measured at Dome C, Antarctica, our model reproduces with good agreement the nitrate measurements in the surface snow. By investigating the relative importance of the main exchange processes, this study shows that, on the one hand, the combination of bulk diffusion and co-condensation allows a good reproduction of the measurements (correlation coefficient r = 0.95), with a correct amplitude and timing of summer peak concentration of nitrate in snow. During winter, nitrate concentration in surface snow is mainly driven by thermodynamic equilibrium, whilst the peak observed in summer is explained by the kinetic process of co-condensation. On the other hand, the adsorption of nitric acid on the surface of the snow grains, constrained by an already existing parameterisation for the isotherm, fails to fit the observed variations. During winter and spring, the modelled concentration of adsorbed nitrate is respectively 2.5 and 8.3-fold higher than the measured one. A strong diurnal variation driven by the temperature cycle and a peak occurring in early spring are two other major features that do not match the measurements. This study clearly demonstrates that co-condensation is the most important process to explain nitrate incorporation in snow undergoing temperature gradient metamorphism. The parameterisation developed for this process can now be used as a foundation piece in snowpack models to predict the inter-relationship between snow physical evolution and snow nitrate chemistry.  
  Programme 1110  
  Campaign  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Summary Language Original Title  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1680-7324 ISBN 1680-7324 Medium  
  Area Expedition Conference  
  Notes Approved yes  
  Call Number Serial 6776  
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Author F. Sprovieri, N. Pirrone, M. Bencardino, F. D'Amore, F. Carbone, S. Cinnirella, V. Mannarino, M. Landis, R. Ebinghaus, A. Weigelt, E.-G. Brunke, C. Labuschagne, L. Martin, J. Munthe, I. Wängberg, P. Artaxo, F. Morais, H. D. M. J. Barbosa, J. Brito, W. Cairns, C. Barbante, M. D. C. Diéguez, P. E. Garcia, A. Dommergue, H. Angot, O. Magand, H. Skov, M. Horvat, J. Kotnik, K. A. Read, L. M. Neves, B. M. Gawlik, F. Sena, N. Mashyanov, V. Obolkin, D. Wip, X. B. Feng, H. Zhang, X. Fu, R. Ramachandran, D. Cossa, J. Knoery, N. Marusczak, M. Nerentorp, C. Norstrom doi  isbn
openurl 
  Title Atmospheric mercury concentrations observed at ground-based monitoring sites globally distributed in the framework of the GMOS network Type Journal
  Year 2016 Publication Atmos. chem. phys. Abbreviated Journal  
  Volume 16 Issue 18 Pages 11915-11935  
  Keywords  
  Abstract Long-term monitoring of data of ambient mercury (Hg) on a global scale to assess its emission, transport, atmospheric chemistry, and deposition processes is vital to understanding the impact of Hg pollution on the environment. The Global Mercury Observation System (GMOS) project was funded by the European Commission (http://www.gmos.eu) and started in November 2010 with the overall goal to develop a coordinated global observing system to monitor Hg on a global scale, including a large network of ground-based monitoring stations, ad hoc periodic oceanographic cruises and measurement flights in the lower and upper troposphere as well as in the lower stratosphere. To date, more than 40 ground-based monitoring sites constitute the global network covering many regions where little to no observational data were available before GMOS. This work presents atmospheric Hg concentrations recorded worldwide in the framework of the GMOS project (2010–2015), analyzing Hg measurement results in terms of temporal trends, seasonality and comparability within the network. Major findings highlighted in this paper include a clear gradient of Hg concentrations between the Northern and Southern hemispheres, confirming that the gradient observed is mostly driven by local and regional sources, which can be anthropogenic, natural or a combination of both.  
  Programme 1028  
  Campaign  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Summary Language Original Title  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1680-7324 ISBN 1680-7324 Medium  
  Area Expedition Conference  
  Notes Approved yes  
  Call Number Serial 6596  
Permanent link to this record
 

 
Author H. Angot, A. Dastoor, F. De Simone, K. Gårdfeldt, C. N. Gencarelli, I. M. Hedgecock, S. Langer, O. Magand, M. N. Mastromonaco, C. Nordstrøm, K. A. Pfaffhuber, N. Pirrone, A. Ryjkov, N. E. Selin, H. Skov, S. Song, F. Sprovieri, A. Steffen, K. Toyota, O. Travnikov, X. Yang, A. Dommergue doi  isbn
openurl 
  Title Chemical cycling and deposition of atmospheric mercury in polar regions: review of recent measurements and comparison with models Type Journal
  Year 2016 Publication Atmos. chem. phys. Abbreviated Journal  
  Volume 16 Issue 16 Pages 10735-10763  
  Keywords  
  Abstract Mercury (Hg) is a worldwide contaminant that can cause adverse health effects to wildlife and humans. While atmospheric modeling traces the link from emissions to deposition of Hg onto environmental surfaces, large uncertainties arise from our incomplete understanding of atmospheric processes (oxidation pathways, deposition, and re-emission). Atmospheric Hg reactivity is exacerbated in high latitudes and there is still much to be learned from polar regions in terms of atmospheric processes. This paper provides a synthesis of the atmospheric Hg monitoring data available in recent years (2011–2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. The cycle of atmospheric Hg in the Arctic and in Antarctica presents both similarities and differences. Coastal sites in the two regions are both influenced by springtime atmospheric Hg depletion events and by summertime snowpack re-emission and oceanic evasion of Hg. The cycle of atmospheric Hg differs between the two regions primarily because of their different geography. While Arctic sites are significantly influenced by northern hemispheric Hg emissions especially in winter, coastal Antarctic sites are significantly influenced by the reactivity observed on the East Antarctic ice sheet due to katabatic winds. Based on the comparison of multi-model simulations with observations, this paper discusses whether the processes that affect atmospheric Hg seasonality and interannual variability are appropriately represented in the models and identifies research gaps in our understanding of the atmospheric Hg cycling in high latitudes.  
  Programme 1028  
  Campaign  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Summary Language Original Title  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1680-7324 ISBN 1680-7324 Medium  
  Area Expedition Conference  
  Notes Approved yes  
  Call Number Serial 6592  
Permanent link to this record
 

 
Author Frey M M, Roscoe H K, Kukui A, Savarino J, France J L, King M D, Legrand M, Preunkert S, doi  openurl
  Title Atmospheric nitrogen oxides (NO and NO2) at Dome C, East Antarctica, during the OPALE campaign Type Journal Article
  Year 2015 Publication Atmospheric Chemistry and Physics Abbreviated Journal  
  Volume 15 Issue 14 Pages 7859-7875  
  Keywords  
  Abstract Mixing ratios of the atmospheric nitrogen oxides NO and NO2 were measured as part of the OPALE (Oxidant Production in Antarctic Lands & Export) campaign at Dome C, East Antarctica (75.1° S, 123.3° E, 3233 m), during December 2011 to January 2012. Profiles of NOx mixing ratios of the lower 100 m of the atmosphere confirm that, in contrast to the South Pole, air chemistry at Dome C is strongly influenced by large diurnal cycles in solar irradiance and a sudden collapse of the atmospheric boundary layer in the early evening. Depth profiles of mixing ratios in firn air suggest that the upper snowpack at Dome C holds a significant reservoir of photolytically produced NO2 and is a sink of gas-phase ozone (O3). First-time observations of bromine oxide (BrO) at Dome C show that mixing ratios of BrO near the ground are low, certainly less than 5 pptv, with higher levels in the free troposphere. Assuming steady state, observed mixing ratios of BrO and RO2 radicals are too low to explain the large NO2 : NO ratios found in ambient air, possibly indicating the existence of an unknown process contributing to the atmospheric chemistry of reactive nitrogen above the Antarctic Plateau. During 2011–2012, NOx mixing ratios and flux were larger than in 2009–2010, consistent with also larger surface O3 mixing ratios resulting from increased net O3 production. Large NOx mixing ratios at Dome C arise from a combination of continuous sunlight, shallow mixing height and significant NOx emissions by surface snow (FNOx). During 23 December 2011–12 January 2012, median FNOx was twice that during the same period in 2009–2010 due to significantly larger atmospheric turbulence and a slightly stronger snowpack source. A tripling of FNOx in December 2011 was largely due to changes in snowpack source strength caused primarily by changes in NO3- concentrations in the snow skin layer, and only to a secondary order by decrease of total column O3 and associated increase in NO3- photolysis rates. A source of uncertainty in model estimates of FNOx is the quantum yield of NO3- photolysis in natural snow, which may change over time as the snow ages.  
  Programme 903  
  Campaign  
  Address  
  Corporate Author Thesis  
  Publisher Copernicus GmbH Place of Publication Editor  
  Language Summary Language Original Title  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1680-7316 ISBN Medium  
  Area Expedition Conference  
  Notes Approved yes  
  Call Number Serial 6156  
Permanent link to this record
 

 
Author Song S, Selin N E, Soerensen A L, Angot H, Artz R, Brooks S, Brunke E-G, Conley G, Dommergue A, Ebinghaus R, Holsen T M, Jaffe D A, Kang S, Kelley P, Luke W T, Magand O, Marumoto K, Pfaffhuber K A, Ren X, Sheu G-R, Slemr F, Warneke T, Weigelt A, Weiss-Penzias P, Wip D C, Zhang Q, doi  openurl
  Title Top-down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling Type Journal Article
  Year 2015 Publication Atmospheric Chemistry and Physics Abbreviated Journal  
  Volume 15 Issue 12 Pages 7103-7125  
  Keywords  
  Abstract  
  Programme 1028  
  Campaign  
  Address  
  Corporate Author Thesis  
  Publisher Copernicus GmbH Place of Publication Editor  
  Language Summary Language Original Title  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1680-7316 ISBN Medium  
  Area Expedition Conference  
  Notes Approved yes  
  Call Number Serial 6219  
Permanent link to this record
 

 
Author Preunkert S, Legrand M, Frey M M, Kukui A, Savarino J, Gallée H, King M, Jourdain B, Vicars W, Helmig D, doi  openurl
  Title Formaldehyde (HCHO) in air, snow, and interstitial air at Concordia (East Antarctic Plateau) in summer Type Journal Article
  Year 2015 Publication Atmospheric Chemistry and Physics Abbreviated Journal  
  Volume 15 Issue 12 Pages 6689-6705  
  Keywords  
  Abstract During the 2011/12 and 2012/13 austral summers, HCHO was investigated for the first time in ambient air, snow, and interstitial air at the Concordia site, located near Dome C on the East Antarctic Plateau, by deploying an Aerolaser AL-4021 analyzer. Snow emission fluxes were estimated from vertical gradients of mixing ratios observed at 1 cm and 1 m above the snow surface as well as in interstitial air a few centimeters below the surface and in air just above the snowpack. Typical flux values range between 1 and 2 × 1012 molecules m-2 s-1 at night and 3 and 5 × 1012 molecules m-2 s-1 at noon. Shading experiments suggest that the photochemical HCHO production in the snowpack at Concordia remains negligible compared to temperature-driven air–snow exchanges. At 1 m above the snow surface, the observed mean mixing ratio of 130 pptv and its diurnal cycle characterized by a slight decrease around noon are quite well reproduced by 1-D simulations that include snow emissions and gas-phase methane oxidation chemistry. Simulations indicate that the gas-phase production from CH4 oxidation largely contributes (66%) to the observed HCHO mixing ratios. In addition, HCHO snow emissions account for ~ 30% at night and ~ 10% at noon to the observed HCHO levels.  
  Programme 903  
  Campaign  
  Address  
  Corporate Author Thesis  
  Publisher Copernicus GmbH Place of Publication Editor  
  Language Summary Language Original Title  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1680-7316 ISBN Medium  
  Area Expedition Conference  
  Notes Approved yes  
  Call Number Serial 6158  
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