Articles | Volume 16, issue 4
https://doi.org/10.5194/acp-16-2659-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Special issue:
https://doi.org/10.5194/acp-16-2659-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
03 Mar 2016
Research article |
| 03 Mar 2016
Oxygen isotope mass balance of atmospheric nitrate at Dome C, East Antarctica, during the OPALE campaign
Joël Savarino
CORRESPONDING AUTHOR
Université Grenoble Alpes, Laboratoire de Glaciologie et
Géophysique de l'Environnement (LGGE), 38000 Grenoble, France
CNRS, Laboratoire de Glaciologie et Géophysique de l'Environnement
(LGGE), 38000 Grenoble, France
William C. Vicars
Université Grenoble Alpes, Laboratoire de Glaciologie et
Géophysique de l'Environnement (LGGE), 38000 Grenoble, France
CNRS, Laboratoire de Glaciologie et Géophysique de l'Environnement
(LGGE), 38000 Grenoble, France
now at: Technical Services Program, Air Pollution Control
Division, Colorado Department of Public Health and Environment, Denver, CO,
USA
Michel Legrand
Université Grenoble Alpes, Laboratoire de Glaciologie et
Géophysique de l'Environnement (LGGE), 38000 Grenoble, France
CNRS, Laboratoire de Glaciologie et Géophysique de l'Environnement
(LGGE), 38000 Grenoble, France
Suzanne Preunkert
Université Grenoble Alpes, Laboratoire de Glaciologie et
Géophysique de l'Environnement (LGGE), 38000 Grenoble, France
CNRS, Laboratoire de Glaciologie et Géophysique de l'Environnement
(LGGE), 38000 Grenoble, France
Bruno Jourdain
Université Grenoble Alpes, Laboratoire de Glaciologie et
Géophysique de l'Environnement (LGGE), 38000 Grenoble, France
CNRS, Laboratoire de Glaciologie et Géophysique de l'Environnement
(LGGE), 38000 Grenoble, France
Markus M. Frey
British Antarctic Survey, Natural Environment Research Council,
Cambridge, UK
Alexandre Kukui
Laboratoire Atmosphère, Milieux et Observations Spatiales
(LATMOS), UMR8190, CNRS-Université de Versailles Saint Quentin,
Université Pierre et Marie Curie, Paris, France
Laboratoire de Physique et Chimie de l'Environnement et de l'Espace
(LPC2E), UMR6115 CNRS-Université d'Orléans, 45071 Orléans CEDEX
2, France
Nicolas Caillon
Université Grenoble Alpes, Laboratoire de Glaciologie et
Géophysique de l'Environnement (LGGE), 38000 Grenoble, France
CNRS, Laboratoire de Glaciologie et Géophysique de l'Environnement
(LGGE), 38000 Grenoble, France
Jaime Gil Roca
Laboratoire Atmosphère, Milieux et Observations Spatiales
(LATMOS), UMR8190, CNRS-Université de Versailles Saint Quentin,
Université Pierre et Marie Curie, Paris, France
Laboratoire de Physique et Chimie de l'Environnement et de l'Espace
(LPC2E), UMR6115 CNRS-Université d'Orléans, 45071 Orléans CEDEX
2, France
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EGUsphere, https://doi.org/10.5194/egusphere-2024-1381, https://doi.org/10.5194/egusphere-2024-1381, 2024
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A record of ammonium covering the years 1750 to 2008 was extracted from a 182-meter-long ice core drilled in 2009 at Mt. Elbrus in the Caucasus, Russia. Changes in ammonia emissions in southeastern Europe during the pre-industrial and industrial periods were investigated. The level of ammonium in 1750 indicates a significant contribution of natural sources to the ammonia budget, contrasting with present-day conditions, where agricultural emissions outweigh those from biogenic sources in Europe.
Benjamin Heutte, Nora Bergner, Hélène Angot, Jakob B. Pernov, Lubna Dada, Jessica A. Mirrielees, Ivo Beck, Andrea Baccarini, Matthew Boyer, Jessie M. Creamean, Kaspar R. Daellenbach, Imad El Haddad, Markus M. Frey, Silvia Henning, Tiaa Laurila, Vaios Moschos, Tuukka Petäjä, Kerri A. Pratt, Lauriane L. J. Quéléver, Matthew D. Shupe, Paul Zieger, Tuija Jokinen, and Julia Schmale
EGUsphere, https://doi.org/10.5194/egusphere-2024-1912, https://doi.org/10.5194/egusphere-2024-1912, 2024
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Limited aerosol measurements in the central Arctic hinder our understanding of aerosol-climate interactions in the region. Our year-long observations of aerosol physicochemical properties during the MOSAiC expedition reveal strong seasonal variations in aerosol chemical composition, where the short-term variability is heavily affected by storms in the Arctic. Locally wind-generated particles are shown to be an important source of cloud seeds, especially in autumn.
V. Holly L. Winton, Robert Mulvaney, Joel Savarino, Kyle R. Clem, and Markus M. Frey
Clim. Past, 20, 1213–1232, https://doi.org/10.5194/cp-20-1213-2024, https://doi.org/10.5194/cp-20-1213-2024, 2024
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In 2018, a new 120 m ice core was drilled in a region located under the Antarctic ozone hole. We present the first results including a 1300-year record of snow accumulation and aerosol chemistry. We investigate the aerosol and moisture source regions and atmospheric processes related to the ice core record and discuss what this means for developing a record of past ultraviolet radiation and ozone depletion using the stable isotopic composition of nitrate measured in the same ice core.
James Brean, David C. S. Beddows, Eija Asmi, Ari Virkkula, Lauriane L. J. Quéléver, Mikko Sipilä, Floortje Van Den Heuvel, Thomas Lachlan-Cope, Anna Jones, Markus Frey, Angelo Lupi, Jiyeon Park, Young Jun Yoon, Ralf Weller, Giselle L. Marincovich, Gabriela C. Mulena, Roy M. Harrison, and Manuel Dall´Osto
EGUsphere, https://doi.org/10.5194/egusphere-2024-987, https://doi.org/10.5194/egusphere-2024-987, 2024
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Our results emphasize how understanding the geographical variation in surface types across the Antarctic is key to understanding secondary aerosol sources.
Susanne Preunkert, Pascal Bohleber, Michel Legrand, Adrien Gilbert, Tobias Erhardt, Roland Purtschert, Lars Zipf, Astrid Waldner, Joseph R. McConnell, and Hubertus Fischer
The Cryosphere, 18, 2177–2194, https://doi.org/10.5194/tc-18-2177-2024, https://doi.org/10.5194/tc-18-2177-2024, 2024
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Ice cores from high-elevation Alpine glaciers are an important tool to reconstruct the past atmosphere. However, since crevasses are common at these glacier sites, rigorous investigations of glaciological conditions upstream of drill sites are needed before interpreting such ice cores. On the basis of three ice cores extracted at Col du Dôme (4250 m a.s.l; French Alps), an overall picture of a dynamic crevasse formation is drawn, which disturbs the depth–age relation of two of the three cores.
Vladimir Mikhalenko, Stanislav Kutuzov, Pavel Toropov, Michel Legrand, Sergey Sokratov, Gleb Chernyakov, Ivan Lavrentiev, Susanne Preunkert, Anna Kozachek, Mstislav Vorobiev, Aleksandra Khairedinova, and Vladimir Lipenkov
Clim. Past, 20, 237–255, https://doi.org/10.5194/cp-20-237-2024, https://doi.org/10.5194/cp-20-237-2024, 2024
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In this paper, we present a reconstruction of snow accumulation for both summer and winter over the past 260 years using ice-core records obtained from Mt. Elbrus in the Caucasus region. The accumulation record represents the historical precipitation patterns in a vast region encompassing the northern Caucasus, Black Sea, and southeastern Europe. Our findings show that the North Atlantic plays a crucial role in determining precipitation levels in this region.
Anja Eichler, Michel Legrand, Theo M. Jenk, Susanne Preunkert, Camilla Andersson, Sabine Eckhardt, Magnuz Engardt, Andreas Plach, and Margit Schwikowski
The Cryosphere, 17, 2119–2137, https://doi.org/10.5194/tc-17-2119-2023, https://doi.org/10.5194/tc-17-2119-2023, 2023
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We investigate how a 250-year history of the emission of air pollutants (major inorganic aerosol constituents, black carbon, and trace species) is preserved in ice cores from four sites in the European Alps. The observed uniform timing in species-dependent longer-term concentration changes reveals that the different ice-core records provide a consistent, spatially representative signal of the pollution history from western European countries.
Amelia M. H. Bond, Markus M. Frey, Jan Kaiser, Jörg Kleffmann, Anna E. Jones, and Freya A. Squires
Atmos. Chem. Phys., 23, 5533–5550, https://doi.org/10.5194/acp-23-5533-2023, https://doi.org/10.5194/acp-23-5533-2023, 2023
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Atmospheric nitrous acid (HONO) amount fractions measured at Halley Research Station, Antarctica, were found to be low. Vertical fluxes of HONO from the snow were also measured and agree with the estimated HONO production rate from photolysis of snow nitrate. In a simple box model of HONO sources and sinks, there was good agreement between the measured flux and amount fraction. HONO was found to be an important OH radical source at Halley.
Albane Barbero, Roberto Grilli, Markus M. Frey, Camille Blouzon, Detlev Helmig, Nicolas Caillon, and Joël Savarino
Atmos. Chem. Phys., 22, 12025–12054, https://doi.org/10.5194/acp-22-12025-2022, https://doi.org/10.5194/acp-22-12025-2022, 2022
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The high reactivity of the summer Antarctic boundary layer results in part from the emissions of nitrogen oxides produced during photo-denitrification of the snowpack, but its underlying mechanisms are not yet fully understood. The results of this study suggest that more NO2 is produced from the snowpack early in the photolytic season, possibly due to stronger UV irradiance caused by a smaller solar zenith angle near the solstice.
Silvia Becagli, Elena Barbaro, Simone Bonamano, Laura Caiazzo, Alcide di Sarra, Matteo Feltracco, Paolo Grigioni, Jost Heintzenberg, Luigi Lazzara, Michel Legrand, Alice Madonia, Marco Marcelli, Chiara Melillo, Daniela Meloni, Caterina Nuccio, Giandomenico Pace, Ki-Tae Park, Suzanne Preunkert, Mirko Severi, Marco Vecchiato, Roberta Zangrando, and Rita Traversi
Atmos. Chem. Phys., 22, 9245–9263, https://doi.org/10.5194/acp-22-9245-2022, https://doi.org/10.5194/acp-22-9245-2022, 2022
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Measurements of phytoplanktonic dimethylsulfide and its oxidation products in the Antarctic atmosphere allow us to understand the role of the oceanic (sea ice melting, Chl α and dimethylsulfoniopropionate) and atmospheric (wind direction and speed, humidity, solar radiation and transport processes) factors in the biogenic aerosol formation, concentration and characteristic ratio between components in an Antarctic coastal site facing the polynya of the Ross Sea.
David N. Wagner, Matthew D. Shupe, Christopher Cox, Ola G. Persson, Taneil Uttal, Markus M. Frey, Amélie Kirchgaessner, Martin Schneebeli, Matthias Jaggi, Amy R. Macfarlane, Polona Itkin, Stefanie Arndt, Stefan Hendricks, Daniela Krampe, Marcel Nicolaus, Robert Ricker, Julia Regnery, Nikolai Kolabutin, Egor Shimanshuck, Marc Oggier, Ian Raphael, Julienne Stroeve, and Michael Lehning
The Cryosphere, 16, 2373–2402, https://doi.org/10.5194/tc-16-2373-2022, https://doi.org/10.5194/tc-16-2373-2022, 2022
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Based on measurements of the snow cover over sea ice and atmospheric measurements, we estimate snowfall and snow accumulation for the MOSAiC ice floe, between November 2019 and May 2020. For this period, we estimate 98–114 mm of precipitation. We suggest that about 34 mm of snow water equivalent accumulated until the end of April 2020 and that at least about 50 % of the precipitated snow was eroded or sublimated. Further, we suggest explanations for potential snowfall overestimation.
Xavier Faïn, Rachael H. Rhodes, Philip Place, Vasilii V. Petrenko, Kévin Fourteau, Nathan Chellman, Edward Crosier, Joseph R. McConnell, Edward J. Brook, Thomas Blunier, Michel Legrand, and Jérôme Chappellaz
Clim. Past, 18, 631–647, https://doi.org/10.5194/cp-18-631-2022, https://doi.org/10.5194/cp-18-631-2022, 2022
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Carbon monoxide (CO) is a regulated pollutant and one of the key components determining the oxidizing capacity of the atmosphere. In this study, we analyzed five ice cores from Greenland at high resolution for CO concentrations by coupling laser spectrometry with continuous melting. By combining these new datasets, we produced an upper-bound estimate of past atmospheric CO abundance since preindustrial times for the Northern Hemisphere high latitudes, covering the period from 1700 to 1957 CE.
V. Holly L. Winton, Alison Ming, Nicolas Caillon, Lisa Hauge, Anna E. Jones, Joel Savarino, Xin Yang, and Markus M. Frey
Atmos. Chem. Phys., 20, 5861–5885, https://doi.org/10.5194/acp-20-5861-2020, https://doi.org/10.5194/acp-20-5861-2020, 2020
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The transfer of the nitrogen stable isotopic composition in nitrate between the air and snow at low accumulation sites in Antarctica leaves an UV imprint in the snow. Quantifying how nitrate isotope values change allows us to interpret longer ice core records. Based on nitrate observations and modelling at Kohnen, East Antarctica, the dominant factors controlling the nitrate isotope signature in deep snow layers are the depth of light penetration into the snowpack and the snow accumulation rate.
Markus M. Frey, Sarah J. Norris, Ian M. Brooks, Philip S. Anderson, Kouichi Nishimura, Xin Yang, Anna E. Jones, Michelle G. Nerentorp Mastromonaco, David H. Jones, and Eric W. Wolff
Atmos. Chem. Phys., 20, 2549–2578, https://doi.org/10.5194/acp-20-2549-2020, https://doi.org/10.5194/acp-20-2549-2020, 2020
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A winter sea ice expedition to Antarctica provided the first direct observations of sea salt aerosol (SSA) production during snow storms above sea ice, thereby validating a model hypothesis to account for winter time SSA maxima in Antarctica not explained otherwise. Defining SSA sources is important given the critical roles that aerosol plays for climate, for air quality and as a potential ice core proxy for sea ice conditions in the past.
Susanne Preunkert, Michel Legrand, Stanislav Kutuzov, Patrick Ginot, Vladimir Mikhalenko, and Ronny Friedrich
Atmos. Chem. Phys., 19, 14119–14132, https://doi.org/10.5194/acp-19-14119-2019, https://doi.org/10.5194/acp-19-14119-2019, 2019
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This paper reports on an ice core drilled to bedrock at Mt Elbrus (5115 m a.s.l., Russia) to reconstruct the atmospheric pollution since the 19th century in south-eastern Europe. The annual dust-free sulfate record indicates a 7-fold increase from prior to 1900 to 1980–1995. Consistent with past SO2 emission inventories, a much earlier onset and a more pronounced decrease in the sulfur pollution over the last 3 decades are observed in western Europe than in south-eastern and eastern Europe.
Stanislav Kutuzov, Michel Legrand, Susanne Preunkert, Patrick Ginot, Vladimir Mikhalenko, Karim Shukurov, Aleksei Poliukhov, and Pavel Toropov
Atmos. Chem. Phys., 19, 14133–14148, https://doi.org/10.5194/acp-19-14133-2019, https://doi.org/10.5194/acp-19-14133-2019, 2019
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Ice cores are one of the most valuable paleo-archives. Here we present analysis of the concentrations of calcium, recorded in ice core from the Caucasus over the past 240 years. We found a correlation between dust in ice and precipitation and soil moisture content in the Middle East and North Africa. The prominent increase in dust concentration in the ice core confirms that the recent droughts in the Fertile Crescent were most severe at least for the past two centuries.
Xin Yang, Markus M. Frey, Rachael H. Rhodes, Sarah J. Norris, Ian M. Brooks, Philip S. Anderson, Kouichi Nishimura, Anna E. Jones, and Eric W. Wolff
Atmos. Chem. Phys., 19, 8407–8424, https://doi.org/10.5194/acp-19-8407-2019, https://doi.org/10.5194/acp-19-8407-2019, 2019
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This is a comprehensive model–data comparison aiming to evaluate the proposed mechanism of sea salt aerosol (SSA) production from blowing snow on sea ice. Some key parameters such as snow salinity and blowing-snow size distribution were constrained by data collected in the Weddell Sea. The good agreement between modelled SSA and the cruise data strongly indicates that sea ice surface is a large SSA source in polar regions, a process which has not been considered in current climate models.
Sentia Goursaud, Valérie Masson-Delmotte, Vincent Favier, Suzanne Preunkert, Michel Legrand, Bénédicte Minster, and Martin Werner
The Cryosphere, 13, 1297–1324, https://doi.org/10.5194/tc-13-1297-2019, https://doi.org/10.5194/tc-13-1297-2019, 2019
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We report new water stable isotope records from the first highly resolved firn core drilled in Adélie Land and covering 1998–2014. Using an updated database, we show that mean values are in line with the range of coastal values. Statistical analyses show no relationship between our record and local surface air temperature. Atmospheric back trajectories and isotopic simulations suggest that water stable isotopes in Adélie provide a fingerprint of the variability of atmospheric dynamics.
Rolf Weller, Michel Legrand, and Susanne Preunkert
Atmos. Chem. Phys., 18, 2413–2430, https://doi.org/10.5194/acp-18-2413-2018, https://doi.org/10.5194/acp-18-2413-2018, 2018
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We measured aerosol size distributions and the composition of summer aerosol at the continental Antarctic station Kohnen. Two different weather conditions mediated the transport of aerosol: (1) the intermittent impact of cyclones associated with outstanding marine aerosol concentrations and new particle formation and (2) steady long-range transport under prevailing clear sky conditions. The latter air masses were characterized by aged aerosol and less aerosol load.
Hoi Ga Chan, Markus M. Frey, and Martin D. King
Atmos. Chem. Phys., 18, 1507–1534, https://doi.org/10.5194/acp-18-1507-2018, https://doi.org/10.5194/acp-18-1507-2018, 2018
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Emissions of reactive nitrogen from snowpacks influence remote air quality. Two physical air–snow models for nitrate were developed. One assumes that below a threshold temperature the air–snow grain interface is pure ice and above it a disordered interface emerges. The other assumes an air–ice interface below melting and that any liquid present is concentrated in micropockets. Only the latter matches observations at two Antarctic lcoations covering a wide range of environmental conditions.
Michel Legrand, Susanne Preunkert, Eric Wolff, Rolf Weller, Bruno Jourdain, and Dietmar Wagenbach
Atmos. Chem. Phys., 17, 14039–14054, https://doi.org/10.5194/acp-17-14039-2017, https://doi.org/10.5194/acp-17-14039-2017, 2017
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Multiple year-round records of bulk and size-segregated composition of sea-salt aerosol and acidic gases (HCl and HNO3) were obtained at inland Antarctica. Both acidic sulfur particles and nitric acid are involved in the observed sea-salt dechlorination in spring/summer. The observed sulfate to sodium mass ratio of sea-salt aerosol in winter (0.16 ± 0.05) suggests on average a similar contribution of sea-ice and open-ocean emissions to the sea-salt load over inland Antarctica at that season.
Michel Legrand, Susanne Preunkert, Rolf Weller, Lars Zipf, Christoph Elsässer, Silke Merchel, Georg Rugel, and Dietmar Wagenbach
Atmos. Chem. Phys., 17, 14055–14073, https://doi.org/10.5194/acp-17-14055-2017, https://doi.org/10.5194/acp-17-14055-2017, 2017
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Levels of MSA and sulfate at inland Antarctica are documented from multiple year-round records of bulk and size-segregated aerosol samplings. A striking difference in the seasonality of sulfur aerosol composition, characterized by a MSA to nssSO4 ratio reaching a minimum in summer over the Antarctic plateau (0.05) and a maximum at the coast (up to 0.40), is clearly established. An efficient chemical destruction of MSA is suggested to take place over the Antarctic plateau in summer.
Rachael H. Rhodes, Xin Yang, Eric W. Wolff, Joseph R. McConnell, and Markus M. Frey
Atmos. Chem. Phys., 17, 9417–9433, https://doi.org/10.5194/acp-17-9417-2017, https://doi.org/10.5194/acp-17-9417-2017, 2017
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Sea salt aerosol comes from the open ocean or the sea ice surface. In the polar regions, this opens up the possibility of reconstructing sea ice history using sea salt recorded in ice cores. We use a chemical transport model to demonstrate that the sea ice source of aerosol is important in the Arctic. For the first time, we simulate realistic Greenland ice core sea salt in a process-based model. The importance of the sea ice source increases from south to north across the Greenland ice sheet.
Anna Kozachek, Vladimir Mikhalenko, Valérie Masson-Delmotte, Alexey Ekaykin, Patrick Ginot, Stanislav Kutuzov, Michel Legrand, Vladimir Lipenkov, and Susanne Preunkert
Clim. Past, 13, 473–489, https://doi.org/10.5194/cp-13-473-2017, https://doi.org/10.5194/cp-13-473-2017, 2017
Sakiko Ishino, Shohei Hattori, Joel Savarino, Bruno Jourdain, Susanne Preunkert, Michel Legrand, Nicolas Caillon, Albane Barbero, Kota Kuribayashi, and Naohiro Yoshida
Atmos. Chem. Phys., 17, 3713–3727, https://doi.org/10.5194/acp-17-3713-2017, https://doi.org/10.5194/acp-17-3713-2017, 2017
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We show the first simultaneous observations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal Antarctica. The contrasting seasonal trends between oxygen isotopes of ozone and those of sulfate and nitrate indicate that these signatures in sulfate and nitrate are mainly controlled by changes in oxidation chemistry. We also discuss the specific oxidation chemistry induced by the unique phenomena at the site.
Sentia Goursaud, Valérie Masson-Delmotte, Vincent Favier, Susanne Preunkert, Michel Fily, Hubert Gallée, Bruno Jourdain, Michel Legrand, Olivier Magand, Bénédicte Minster, and Martin Werner
The Cryosphere, 11, 343–362, https://doi.org/10.5194/tc-11-343-2017, https://doi.org/10.5194/tc-11-343-2017, 2017
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Uncertainty of sea level changes is a challenge. As Antarctica is the biggest water reservoir, it is necessary to know how it will contribute. To be able to simulate it, an understanding of past climate is to be achieved, for instance, by studying the ice cores. As climate change is different in different regions, observations are needed all over the continent. Studying an ice core in Adélie Land, we can conclude that there are no changes there at decadal scale over the period 1947–2007.
Michel Legrand, Joseph McConnell, Hubertus Fischer, Eric W. Wolff, Susanne Preunkert, Monica Arienzo, Nathan Chellman, Daiana Leuenberger, Olivia Maselli, Philip Place, Michael Sigl, Simon Schüpbach, and Mike Flannigan
Clim. Past, 12, 2033–2059, https://doi.org/10.5194/cp-12-2033-2016, https://doi.org/10.5194/cp-12-2033-2016, 2016
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Here, we review previous attempts made to reconstruct past forest fire using chemical signals recorded in Greenland ice. We showed that the Greenland ice records of ammonium, found to be a good fire proxy, consistently indicate changing fire activity in Canada in response to past climatic conditions that occurred since the last 15 000 years, including the Little Ice Age and the last large climatic transition.
Hélène Angot, Iris Dion, Nicolas Vogel, Michel Legrand, Olivier Magand, and Aurélien Dommergue
Atmos. Chem. Phys., 16, 8265–8279, https://doi.org/10.5194/acp-16-8265-2016, https://doi.org/10.5194/acp-16-8265-2016, 2016
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This paper presents a multi-year record of atmospheric gaseous elemental mercury (Hg(0)) at Dumont d’Urville (DDU) on the East Antarctic coast. This record reveals particularities that are not seen at other coastal Antarctic sites, likely due to the more frequent arrival of inland air masses at DDU than at other coastal sites, and to the influence of oceanic air masses. This study confirms the influence of processes observed inland on the cycle of atmospheric mercury at a continental scale.
Michel Legrand, Susanne Preunkert, Joël Savarino, Markus M. Frey, Alexandre Kukui, Detlev Helmig, Bruno Jourdain, Anna E. Jones, Rolf Weller, Neil Brough, and Hubert Gallée
Atmos. Chem. Phys., 16, 8053–8069, https://doi.org/10.5194/acp-16-8053-2016, https://doi.org/10.5194/acp-16-8053-2016, 2016
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Surface ozone, the most abundant atmospheric oxidant, has been measured since 2004 at the coastal East Antarctic site of Dumont d’Urville, and since 2007 at the Concordia station located on the high East Antarctic plateau. Long-term changes, seasonal and diurnal cycles, as well as inter-annual summer variability observed at these two East Antarctic sites are discussed. Influences like sea ice extent and outflow from inland Antarctica are discussed.
N. Zannoni, V. Gros, M. Lanza, R. Sarda, B. Bonsang, C. Kalogridis, S. Preunkert, M. Legrand, C. Jambert, C. Boissard, and J. Lathiere
Atmos. Chem. Phys., 16, 1619–1636, https://doi.org/10.5194/acp-16-1619-2016, https://doi.org/10.5194/acp-16-1619-2016, 2016
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Our manuscript shows results of OH reactivity and Biogenic Volatile Organic Compounds (BVOCs) concentration during a field experiment conducted in late spring 2014 at the Observatoire de Haute Provence (OHP) site. We found that OH reactivity is among the highest measured in forests globally (69 s−1) and it is mainly due to isoprene. No missing reactivity was present during daytime inside or above the canopy, while 50 % missing reactivity was found by night at both heights.
V. Mikhalenko, S. Sokratov, S. Kutuzov, P. Ginot, M. Legrand, S. Preunkert, I. Lavrentiev, A. Kozachek, A. Ekaykin, X. Faïn, S. Lim, U. Schotterer, V. Lipenkov, and P. Toropov
The Cryosphere, 9, 2253–2270, https://doi.org/10.5194/tc-9-2253-2015, https://doi.org/10.5194/tc-9-2253-2015, 2015
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For the first time an ice core unaffected by melting was recovered from the western Elbrus plateau in the Caucasus. The preserved chemical and isotopic data are considered a source of paleo-climate information for southern/eastern Europe. Considerable snow accumulation (about 1500mm w.e.) and high sampling resolution allowed seasonal variability to be obtained in climate signals, covering a time period of about 200 years. Ice flow models suggest that the basal ice age can be more than 600 years.
J. Erbland, J. Savarino, S. Morin, J. L. France, M. M. Frey, and M. D. King
Atmos. Chem. Phys., 15, 12079–12113, https://doi.org/10.5194/acp-15-12079-2015, https://doi.org/10.5194/acp-15-12079-2015, 2015
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In this paper, we describe the development of a numerical model which aims at representing nitrate recycling at the air-snow interface on the East Antarctic Plateau. Stable isotopes are used as diagnostic and evaluation tools by comparing the model's results to recent field measurements of nitrate and key atmospheric species at Dome C, Antarctica. From sensitivity tests conducted with the model, we propose a framework for the interpretation of the nitrate isotope record in deep ice cores.
T. A. Berhanu, J. Savarino, J. Erbland, W. C. Vicars, S. Preunkert, J. F. Martins, and M. S. Johnson
Atmos. Chem. Phys., 15, 11243–11256, https://doi.org/10.5194/acp-15-11243-2015, https://doi.org/10.5194/acp-15-11243-2015, 2015
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In this field study at Dome C, Antarctica, we investigated the effect of solar UV photolysis on the stable isotopes of nitrate in snow via comparison of two identical snow pits while exposing only one to solar UV. From the difference between the average isotopic fractionations calculated for each pit, we determined a purely photolytic nitrogen isotopic fractionation of -55.8‰, in good agreement with what has been recently determined in a laboratory study.
M. M. Frey, H. K. Roscoe, A. Kukui, J. Savarino, J. L. France, M. D. King, M. Legrand, and S. Preunkert
Atmos. Chem. Phys., 15, 7859–7875, https://doi.org/10.5194/acp-15-7859-2015, https://doi.org/10.5194/acp-15-7859-2015, 2015
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Surprisingly large concentrations and flux of atmospheric nitrogen oxides were measured at Dome C, East Antarctica. It was found that the surface snow holds a significant reservoir of photochemically produced NOx and is a sink of gas-phase ozone. Main drivers of NOx snow emissions were large snow nitrate concentrations, with contributions of increased UV from decreases in stratospheric ozone. Observed halogen and hydroxyl radical concentrations were too low to explain large NO2:NO ratios.
H. G. Chan, M. D. King, and M. M. Frey
Atmos. Chem. Phys., 15, 7913–7927, https://doi.org/10.5194/acp-15-7913-2015, https://doi.org/10.5194/acp-15-7913-2015, 2015
S. Preunkert, M. Legrand, M. M. Frey, A. Kukui, J. Savarino, H. Gallée, M. King, B. Jourdain, W. Vicars, and D. Helmig
Atmos. Chem. Phys., 15, 6689–6705, https://doi.org/10.5194/acp-15-6689-2015, https://doi.org/10.5194/acp-15-6689-2015, 2015
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During two austral summers HCHO was investigated in air, snow, and interstitial air at the Concordia site located on the East Antarctic Plateau. Snow emission fluxes were estimated to be around 1 to 2 and 3 to 5 x 10^12 molecules m-2 s-1 at night and at noon, respectively. Shading experiments suggest that the photochemical HCHO production in the snowpack at Concordia remains negligible. The mean HCHO level of 130pptv observed at 1m above the surface is quite well reproduced by 1-D simulations.
H. Gallée, S. Preunkert, S. Argentini, M. M. Frey, C. Genthon, B. Jourdain, I. Pietroni, G. Casasanta, H. Barral, E. Vignon, C. Amory, and M. Legrand
Atmos. Chem. Phys., 15, 6225–6236, https://doi.org/10.5194/acp-15-6225-2015, https://doi.org/10.5194/acp-15-6225-2015, 2015
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Regional climate model MAR was run for the region of Dome C located on the East Antarctic plateau, during summer 2011–2012, with a high vertical resolution in the lower troposphere. MAR is generally in very good agreement with the observations and provides sufficiently reliable information about surface turbulent fluxes and vertical profiles of vertical diffusion coefficients when discussing the representativeness of chemical measurements made nearby the ground surface at Dome C.
A. Kukui, M. Legrand, S. Preunkert, M. M. Frey, R. Loisil, J. Gil Roca, B. Jourdain, M. D. King, J. L. France, and G. Ancellet
Atmos. Chem. Phys., 14, 12373–12392, https://doi.org/10.5194/acp-14-12373-2014, https://doi.org/10.5194/acp-14-12373-2014, 2014
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Concentrations of OH radicals and the sum of peroxy radicals, RO2, were measured in the boundary layer for the first time on the East Antarctic Plateau at the Concordia Station during the austral summer 2011/2012. The concentrations of radicals were comparable to those observed at the South Pole, confirming that the elevated oxidative capacity of the Antarctic atmospheric boundary layer found at the South Pole is not restricted to the South Pole but common over the high Antarctic plateau.
M. Legrand, S. Preunkert, M. Frey, Th. Bartels-Rausch, A. Kukui, M. D. King, J. Savarino, M. Kerbrat, and B. Jourdain
Atmos. Chem. Phys., 14, 9963–9976, https://doi.org/10.5194/acp-14-9963-2014, https://doi.org/10.5194/acp-14-9963-2014, 2014
X. Faïn, J. Chappellaz, R. H. Rhodes, C. Stowasser, T. Blunier, J. R. McConnell, E. J. Brook, S. Preunkert, M. Legrand, T. Debois, and D. Romanini
Clim. Past, 10, 987–1000, https://doi.org/10.5194/cp-10-987-2014, https://doi.org/10.5194/cp-10-987-2014, 2014
M. Legrand, S. Preunkert, B. Jourdain, J. Guilhermet, X. Fa{ï}n, I. Alekhina, and J. R. Petit
Clim. Past, 9, 2195–2211, https://doi.org/10.5194/cp-9-2195-2013, https://doi.org/10.5194/cp-9-2195-2013, 2013
S. Masclin, M. M. Frey, W. F. Rogge, and R. C. Bales
Atmos. Chem. Phys., 13, 8857–8877, https://doi.org/10.5194/acp-13-8857-2013, https://doi.org/10.5194/acp-13-8857-2013, 2013
J. Erbland, W. C. Vicars, J. Savarino, S. Morin, M. M. Frey, D. Frosini, E. Vince, and J. M. F. Martins
Atmos. Chem. Phys., 13, 6403–6419, https://doi.org/10.5194/acp-13-6403-2013, https://doi.org/10.5194/acp-13-6403-2013, 2013
S. Preunkert and M. Legrand
Clim. Past, 9, 1403–1416, https://doi.org/10.5194/cp-9-1403-2013, https://doi.org/10.5194/cp-9-1403-2013, 2013
M. M. Frey, N. Brough, J. L. France, P. S. Anderson, O. Traulle, M. D. King, A. E. Jones, E. W. Wolff, and J. Savarino
Atmos. Chem. Phys., 13, 3045–3062, https://doi.org/10.5194/acp-13-3045-2013, https://doi.org/10.5194/acp-13-3045-2013, 2013
Related subject area
Subject: Isotopes | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
A seasonal analysis of aerosol NO3− sources and NOx oxidation pathways in the Southern Ocean marine boundary layer
Nitrate chemistry in the northeast US – Part 1: Nitrogen isotope seasonality tracks nitrate formation chemistry
Nitrate chemistry in the northeast US – Part 2: Oxygen isotopes reveal differences in particulate and gas-phase formation
Photolytic modification of seasonal nitrate isotope cycles in East Antarctica
Atmospheric methane isotopes identify inventory knowledge gaps in the Surat Basin, Australia, coal seam gas and agricultural regions
Methane (CH4) sources in Krakow, Poland: insights from isotope analysis
Isotopic signatures of major methane sources in the coal seam gas fields and adjacent agricultural districts, Queensland, Australia
Measurement report: Nitrogen isotopes (δ15N) and first quantification of oxygen isotope anomalies (Δ17O, δ18O) in atmospheric nitrogen dioxide
Measurement report: Spatial variability of northern Iberian rainfall stable isotope values – investigating atmospheric controls on daily and monthly timescales
Isotopic constraints on atmospheric sulfate formation pathways in the Mt. Everest region, southern Tibetan Plateau
Baffin Bay sea ice extent and synoptic moisture transport drive water vapor isotope (δ18O, δ2H, and deuterium excess) variability in coastal northwest Greenland
New evidence for atmospheric mercury transformations in the marine boundary layer from stable mercury isotopes
The isotopic composition of atmospheric nitrous oxide observed at the high-altitude research station Jungfraujoch, Switzerland
Deposition, recycling, and archival of nitrate stable isotopes between the air–snow interface: comparison between Dronning Maud Land and Dome C, Antarctica
Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative Δ33S reservoir of sulfate aerosols?
Atmospheric radiocarbon measurements to quantify CO2 emissions in the UK from 2014 to 2015
An improved estimate for the δ13C and δ18O signatures of carbon monoxide produced from atmospheric oxidation of volatile organic compounds
Seasonality in the Δ33S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO2
The Δ17O and δ18O values of atmospheric nitrates simultaneously collected downwind of anthropogenic sources – implications for polluted air masses
A very limited role of tropospheric chlorine as a sink of the greenhouse gas methane
Detection and variability of combustion-derived vapor in an urban basin
Stable sulfur isotope measurements to trace the fate of SO2 in the Athabasca oil sands region
Triple oxygen isotopes indicate urbanization affects sources of nitrate in wet and dry atmospheric deposition
Isotopic constraints on heterogeneous sulfate production in Beijing haze
Estimation of the fossil fuel component in atmospheric CO2 based on radiocarbon measurements at the Beromünster tall tower, Switzerland
Constraining N2O emissions since 1940 using firn air isotope measurements in both hemispheres
Seasonal variations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal Antarctica
Carbon isotopic signature of coal-derived methane emissions to the atmosphere: from coalification to alteration
Isotopic composition for source identification of mercury in atmospheric fine particles
Isotopic constraints on the role of hypohalous acids in sulfate aerosol formation in the remote marine boundary layer
In situ observations of the isotopic composition of methane at the Cabauw tall tower site
Isotopic effects of nitrate photochemistry in snow: a field study at Dome C, Antarctica
Stable carbon isotope ratios of ambient secondary organic aerosols in Toronto
WAIS Divide ice core suggests sustained changes in the atmospheric formation pathways of sulfate and nitrate since the 19th century in the extratropical Southern Hemisphere
Stable carbon isotope ratios of toluene in the boundary layer and the lower free troposphere
Emission ratio and isotopic signatures of molecular hydrogen emissions from tropical biomass burning
Can the carbon isotopic composition of methane be reconstructed from multi-site firn air measurements?
Air–snow transfer of nitrate on the East Antarctic Plateau – Part 1: Isotopic evidence for a photolytically driven dynamic equilibrium in summer
Chemical characterization and stable carbon isotopic composition of particulate Polycyclic Aromatic Hydrocarbons issued from combustion of 10 Mediterranean woods
Quantification of the carbonaceous matter origin in submicron marine aerosol by 13C and 14C isotope analysis
Temporal and spatial variability of the stable isotopic composition of atmospheric molecular hydrogen: observations at six EUROHYDROS stations
Continuous isotopic composition measurements of tropospheric CO2 at Jungfraujoch (3580 m a.s.l.), Switzerland: real-time observation of regional pollution events
Anthropogenic imprints on nitrogen and oxygen isotopic composition of precipitation nitrate in a nitrogen-polluted city in southern China
Analysis of 13C and 18O isotope data of CO2 in CARIBIC aircraft samples as tracers of upper troposphere/lower stratosphere mixing and the global carbon cycle
Tracing the fate of atmospheric nitrate deposited onto a forest ecosystem in Eastern Asia using Δ17O
Photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling
Sources and transport of Δ14C in CO2 within the Mexico City Basin and vicinity
Jessica M. Burger, Emily Joyce, Meredith G. Hastings, Kurt A. M. Spence, and Katye E. Altieri
Atmos. Chem. Phys., 23, 5605–5622, https://doi.org/10.5194/acp-23-5605-2023, https://doi.org/10.5194/acp-23-5605-2023, 2023
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A seasonal analysis of the nitrogen isotopes of atmospheric nitrate over the remote Southern Ocean reveals that similar natural NOx sources dominate in spring and summer, while winter is representative of background-level conditions. The oxygen isotopes suggest that similar oxidation pathways involving more ozone occur in spring and winter, while the hydroxyl radical is the main oxidant in summer. This work helps to constrain NOx cycling and oxidant budgets in a data-sparse remote marine region.
Claire Bekker, Wendell W. Walters, Lee T. Murray, and Meredith G. Hastings
Atmos. Chem. Phys., 23, 4185–4201, https://doi.org/10.5194/acp-23-4185-2023, https://doi.org/10.5194/acp-23-4185-2023, 2023
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Nitrate is a critical component of the atmosphere that degrades air quality and ecosystem health. We have investigated the nitrogen isotope compositions of nitrate from deposition samples collected across the northeastern United States. Spatiotemporal variability in the nitrogen isotope compositions was found to track with nitrate formation chemistry. Our results highlight that nitrogen isotope compositions may be a robust tool for improving model representation of nitrate chemistry.
Heejeong Kim, Wendell W. Walters, Claire Bekker, Lee T. Murray, and Meredith G. Hastings
Atmos. Chem. Phys., 23, 4203–4219, https://doi.org/10.5194/acp-23-4203-2023, https://doi.org/10.5194/acp-23-4203-2023, 2023
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Atmospheric nitrate has an important impact on human and ecosystem health. We evaluated atmospheric nitrate formation pathways in the northeastern US utilizing oxygen isotope compositions, which indicated a significant difference between the phases of nitrate (i.e., gas vs. particle). Comparing the observations with model simulations indicated that N2O5 hydrolysis chemistry was overpredicted. Our study has important implications for improving atmospheric chemistry model representation.
Pete D. Akers, Joël Savarino, Nicolas Caillon, Olivier Magand, and Emmanuel Le Meur
Atmos. Chem. Phys., 22, 15637–15657, https://doi.org/10.5194/acp-22-15637-2022, https://doi.org/10.5194/acp-22-15637-2022, 2022
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Nitrate isotopes in Antarctic ice do not preserve the seasonal isotopic cycles of the atmosphere, which limits their use to study the past. We studied nitrate along an 850 km Antarctic transect to learn how these cycles are changed by sunlight-driven chemistry in the snow. Our findings suggest that the snow accumulation rate and other environmental signals can be extracted from nitrate with the right sampling and analytical approaches.
Bryce F. J. Kelly, Xinyi Lu, Stephen J. Harris, Bruno G. Neininger, Jorg M. Hacker, Stefan Schwietzke, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Carina van der Veen, Malika Menoud, and Thomas Röckmann
Atmos. Chem. Phys., 22, 15527–15558, https://doi.org/10.5194/acp-22-15527-2022, https://doi.org/10.5194/acp-22-15527-2022, 2022
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This study explores using the composition of methane of in-flight atmospheric air samples for greenhouse gas inventory verification. The air samples were collected above one of the largest coal seam gas production regions in the world. Adjacent to these gas fields are coal mines, Australia's largest cattle feedlot, and over 1 million grazing cattle. The results are also used to identify methane mitigation opportunities.
Malika Menoud, Carina van der Veen, Jaroslaw Necki, Jakub Bartyzel, Barbara Szénási, Mila Stanisavljević, Isabelle Pison, Philippe Bousquet, and Thomas Röckmann
Atmos. Chem. Phys., 21, 13167–13185, https://doi.org/10.5194/acp-21-13167-2021, https://doi.org/10.5194/acp-21-13167-2021, 2021
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Using measurements of methane isotopes in ambient air and a 3D atmospheric transport model, in Krakow, Poland, we mainly detected fossil-fuel-related sources, coming from coal mining in Silesia and from the use of natural gas in the city. Emission inventories report large emissions from coal mine activity in Silesia, which is in agreement with our measurements. However, methane sources in the urban area of Krakow related to the use of fossil fuels might be underestimated in the inventories.
Xinyi Lu, Stephen J. Harris, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Thomas Röckmann, Carina van der Veen, Malika Menoud, Stefan Schwietzke, and Bryce F. J. Kelly
Atmos. Chem. Phys., 21, 10527–10555, https://doi.org/10.5194/acp-21-10527-2021, https://doi.org/10.5194/acp-21-10527-2021, 2021
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Many coal seam gas (CSG) facilities in the Surat Basin, Australia, are adjacent to other sources of methane, including agricultural, urban, and natural seeps. This makes it challenging to estimate the amount of methane being emitted into the atmosphere from CSG facilities. This research demonstrates that measurements of the carbon and hydrogen stable isotopic composition of methane can distinguish between and apportion methane emissions from CSG facilities, cattle, and many other sources.
Sarah Albertin, Joël Savarino, Slimane Bekki, Albane Barbero, and Nicolas Caillon
Atmos. Chem. Phys., 21, 10477–10497, https://doi.org/10.5194/acp-21-10477-2021, https://doi.org/10.5194/acp-21-10477-2021, 2021
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We report an efficient method to collect atmospheric NO2 adapted for multi-isotopic analysis and present the first NO2 triple oxygen and double nitrogen isotope measurements. Atmospheric samplings carried out in Grenoble, France, highlight the NO2 isotopic signature sensitivity to the local NOx emissions and chemical regimes. These preliminary results are very promising for using the combination of Δ17O and δ15N of NO2 as a probe of the atmospheric NOx emissions and chemistry.
Ana Moreno, Miguel Iglesias, Cesar Azorin-Molina, Carlos Pérez-Mejías, Miguel Bartolomé, Carlos Sancho, Heather Stoll, Isabel Cacho, Jaime Frigola, Cinta Osácar, Arsenio Muñoz, Antonio Delgado-Huertas, Ileana Bladé, and Françoise Vimeux
Atmos. Chem. Phys., 21, 10159–10177, https://doi.org/10.5194/acp-21-10159-2021, https://doi.org/10.5194/acp-21-10159-2021, 2021
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We present a large and unique dataset of the rainfall isotopic composition at seven sites from northern Iberia to characterize their variability at daily and monthly timescales and to assess the role of climate and geographic factors in the modulation of δ18O values. We found that the origin, moisture uptake along the trajectory and type of precipitation play a key role. These results will help to improve the interpretation of δ18O paleorecords from lacustrine carbonates or speleothems.
Kun Wang, Shohei Hattori, Mang Lin, Sakiko Ishino, Becky Alexander, Kazuki Kamezaki, Naohiro Yoshida, and Shichang Kang
Atmos. Chem. Phys., 21, 8357–8376, https://doi.org/10.5194/acp-21-8357-2021, https://doi.org/10.5194/acp-21-8357-2021, 2021
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Sulfate aerosols play an important climatic role and exert adverse effects on the ecological environment and human health. In this study, we present the triple oxygen isotopic composition of sulfate from the Mt. Everest region, southern Tibetan Plateau, and decipher the formation mechanisms of atmospheric sulfate in this pristine environment. The results indicate the important role of the S(IV) + O3 pathway in atmospheric sulfate formation promoted by conditions of high cloud water pH.
Pete D. Akers, Ben G. Kopec, Kyle S. Mattingly, Eric S. Klein, Douglas Causey, and Jeffrey M. Welker
Atmos. Chem. Phys., 20, 13929–13955, https://doi.org/10.5194/acp-20-13929-2020, https://doi.org/10.5194/acp-20-13929-2020, 2020
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Water vapor isotopes recorded for 2 years in coastal northern Greenland largely reflect changes in sea ice cover, with distinct values when Baffin Bay is ice covered in winter vs. open in summer. Resulting changes in moisture transport, surface winds, and air temperature also modify the isotopes. Local glacial ice may thus preserve past changes in the Baffin Bay sea ice extent, and this will help us better understand how the Arctic environment and water cycle responds to global climate change.
Ben Yu, Lin Yang, Linlin Wang, Hongwei Liu, Cailing Xiao, Yong Liang, Qian Liu, Yongguang Yin, Ligang Hu, Jianbo Shi, and Guibin Jiang
Atmos. Chem. Phys., 20, 9713–9723, https://doi.org/10.5194/acp-20-9713-2020, https://doi.org/10.5194/acp-20-9713-2020, 2020
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We found that Br atoms in the marine boundary layer are the most probable oxidizer that transform gaseous elemental mercury into gaseous oxidized mercury, according to the mercury isotopes in the total gaseous mercury. On the other hand, Br or Cl atoms are not the primary oxidizers that produced oxidized mercury on particles. This study showed that mercury isotopes can provide new evidence that help us to fully understand the transformations of atmospheric mercury.
Longfei Yu, Eliza Harris, Stephan Henne, Sarah Eggleston, Martin Steinbacher, Lukas Emmenegger, Christoph Zellweger, and Joachim Mohn
Atmos. Chem. Phys., 20, 6495–6519, https://doi.org/10.5194/acp-20-6495-2020, https://doi.org/10.5194/acp-20-6495-2020, 2020
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We observed the isotopic composition of nitrous oxide in the unpolluted air at Jungfraujoch for 5 years. Our results indicate a clear seasonal pattern in the isotopic composition, corresponding with that in atmospheric nitrous oxide levels. This is most likely due to temporal variations in both emission processes and air mass sources for Jungfraujoch. Our findings are of importance to global nitrous oxide modelling and to better understanding of long-term trends in atmospheric nitrous oxide.
V. Holly L. Winton, Alison Ming, Nicolas Caillon, Lisa Hauge, Anna E. Jones, Joel Savarino, Xin Yang, and Markus M. Frey
Atmos. Chem. Phys., 20, 5861–5885, https://doi.org/10.5194/acp-20-5861-2020, https://doi.org/10.5194/acp-20-5861-2020, 2020
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The transfer of the nitrogen stable isotopic composition in nitrate between the air and snow at low accumulation sites in Antarctica leaves an UV imprint in the snow. Quantifying how nitrate isotope values change allows us to interpret longer ice core records. Based on nitrate observations and modelling at Kohnen, East Antarctica, the dominant factors controlling the nitrate isotope signature in deep snow layers are the depth of light penetration into the snowpack and the snow accumulation rate.
Isabelle Genot, David Au Yang, Erwan Martin, Pierre Cartigny, Erwann Legendre, and Marc De Rafelis
Atmos. Chem. Phys., 20, 4255–4273, https://doi.org/10.5194/acp-20-4255-2020, https://doi.org/10.5194/acp-20-4255-2020, 2020
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Given their critical impact on radiative forcing, sulfate aerosols have been extensively studied using their isotope signatures (δ34S, ∆33S, ∆36S, δ18O, and ∆17O). A striking observation is that ∆33S > 0 ‰, implying a missing reservoir in the sulfur cycle. Here, we measured ∆33S < 0 ‰ in black crust sulfates (i.e., formed on carbonate walls) that must therefore result from distinct chemical pathway(s) compared to sulfate aerosols, and they may well represent this complementary reservoir.
Angelina Wenger, Katherine Pugsley, Simon O'Doherty, Matt Rigby, Alistair J. Manning, Mark F. Lunt, and Emily D. White
Atmos. Chem. Phys., 19, 14057–14070, https://doi.org/10.5194/acp-19-14057-2019, https://doi.org/10.5194/acp-19-14057-2019, 2019
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We present 14CO2 observations at a background site in Ireland and a tall tower site in the UK. These data have been used to calculate the contribution of fossil fuel sources to atmospheric CO2 mole fractions from the UK and Ireland. 14CO2 emissions from nuclear industry sites in the UK cause a higher uncertainty in the results compared to observations in other locations. The observed ffCO2 at the site was not significantly different from simulated values based on the bottom-up inventory.
Isaac J. Vimont, Jocelyn C. Turnbull, Vasilii V. Petrenko, Philip F. Place, Colm Sweeney, Natasha Miles, Scott Richardson, Bruce H. Vaughn, and James W. C. White
Atmos. Chem. Phys., 19, 8547–8562, https://doi.org/10.5194/acp-19-8547-2019, https://doi.org/10.5194/acp-19-8547-2019, 2019
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Stable isotopes of Carbon Monoxide (CO) and radiocarbon carbon dioxide were measured over three summers at Indianapolis, Indiana, US, and for 1 year at a site thought to be strongly influenced by CO from oxidized volatile organic compounds (VOCs) in South Carolina, US. The Indianapolis results were used to provide an estimate of the carbon and oxygen isotopic signatures of CO produced from oxidized VOCs. This updated estimate agrees well with the data from South Carolina during the summer.
David Au Yang, Pierre Cartigny, Karine Desboeufs, and David Widory
Atmos. Chem. Phys., 19, 3779–3796, https://doi.org/10.5194/acp-19-3779-2019, https://doi.org/10.5194/acp-19-3779-2019, 2019
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Sulfates present in urban aerosols collected worldwide usually exhibit 33S-anomalies whose origin remains unclear. Besides, the sulfate concentration is not very well modelled nowadays, which, coupled with the isotopic composition anomaly on the 33S, would highlight the presence of at least an additional oxidation pathway, different from O2+TMI, O3, OH, H2O2 and NO2. We suggest here the implication of two other possible oxidation pathways.
Martine M. Savard, Amanda S. Cole, Robert Vet, and Anna Smirnoff
Atmos. Chem. Phys., 18, 10373–10389, https://doi.org/10.5194/acp-18-10373-2018, https://doi.org/10.5194/acp-18-10373-2018, 2018
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Improving air quality requires understanding of the atmospheric processes transforming nitrous oxides emitted by human activities into nitrates, an N form that may degrade natural ecosystems. Isotopes (∆17O, δ18O) are characterized in separate wet, particulate and gaseous nitrates for the first time. The gas ranges are distinct from those of the other nitrates, and the plume dynamics emerge as crucial in interpreting the results, which unravel key processes behind the distribution of nitrates.
Sergey Gromov, Carl A. M. Brenninkmeijer, and Patrick Jöckel
Atmos. Chem. Phys., 18, 9831–9843, https://doi.org/10.5194/acp-18-9831-2018, https://doi.org/10.5194/acp-18-9831-2018, 2018
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Using the observational data on 13C (CO) and 13C (CH4) from the extra-tropical Southern Hemisphere (ETSH) and EMAC model we (1) provide an independent, observation-based evaluation of Cl atom concentration variations in the ETSH throughout 1994–2000, (2) show that the role of tropospheric Cl as a sink of CH4 is seriously overestimated in the literature, (3) demonstrate that the 13C/12C ratio of CO is a sensitive indicator for the isotopic composition of reacted CH4 and therefore for its sources.
Richard P. Fiorella, Ryan Bares, John C. Lin, James R. Ehleringer, and Gabriel J. Bowen
Atmos. Chem. Phys., 18, 8529–8547, https://doi.org/10.5194/acp-18-8529-2018, https://doi.org/10.5194/acp-18-8529-2018, 2018
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Fossil fuel combustion produces water; where fossil fuel combustion is concentrated in urban areas, this humidity source may represent ~ 10 % of total humidity. In turn, this water vapor addition may alter urban meteorology, though the contribution of combustion vapor is difficult to measure. Using stable water isotopes, we estimate that up to 16 % of urban humidity may arise from combustion when the atmosphere is stable during winter, and develop recommendations for application in other cities.
Neda Amiri, Roya Ghahreman, Ofelia Rempillo, Travis W. Tokarek, Charles A. Odame-Ankrah, Hans D. Osthoff, and Ann-Lise Norman
Atmos. Chem. Phys., 18, 7757–7780, https://doi.org/10.5194/acp-18-7757-2018, https://doi.org/10.5194/acp-18-7757-2018, 2018
David M. Nelson, Urumu Tsunogai, Dong Ding, Takuya Ohyama, Daisuke D. Komatsu, Fumiko Nakagawa, Izumi Noguchi, and Takashi Yamaguchi
Atmos. Chem. Phys., 18, 6381–6392, https://doi.org/10.5194/acp-18-6381-2018, https://doi.org/10.5194/acp-18-6381-2018, 2018
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Atmospheric nitrate may be produced locally and/or come from upwind regions. To address this issue we measured oxygen and nitrogen isotopes of wet and dry nitrate deposition at nearby urban and rural sites. Our results suggest that, relative to nitrate in wet deposition in urban environments and wet and dry deposition in rural environments, nitrate in dry deposition in urban environments results from local NOx emissions more so than wet deposition, which is transported longer distances.
Pengzhen He, Becky Alexander, Lei Geng, Xiyuan Chi, Shidong Fan, Haicong Zhan, Hui Kang, Guangjie Zheng, Yafang Cheng, Hang Su, Cheng Liu, and Zhouqing Xie
Atmos. Chem. Phys., 18, 5515–5528, https://doi.org/10.5194/acp-18-5515-2018, https://doi.org/10.5194/acp-18-5515-2018, 2018
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We use observations of the oxygen isotopic composition of sulfate aerosol as a fingerprint to quantify various sulfate formation mechanisms during pollution events in Beijing, China. We found that heterogeneous reactions on aerosols dominated sulfate production in general; however, in-cloud reactions would dominate haze sulfate production when cloud liquid water content was high. The findings also suggest the heterogeneity of aerosol acidity should be parameterized in models.
Tesfaye A. Berhanu, Sönke Szidat, Dominik Brunner, Ece Satar, Rüdiger Schanda, Peter Nyfeler, Michael Battaglia, Martin Steinbacher, Samuel Hammer, and Markus Leuenberger
Atmos. Chem. Phys., 17, 10753–10766, https://doi.org/10.5194/acp-17-10753-2017, https://doi.org/10.5194/acp-17-10753-2017, 2017
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Fossil fuel CO2 is the major contributor of anthropogenic CO2 in the atmosphere, and accurate quantification is essential to better understand the carbon cycle. Such accurate quantification can be conducted based on radiocarbon measurements. In this study, we present radiocarbon measurements from a tall tower site in Switzerland. From these measurements, we have observed seasonally varying fossil fuel CO2 contributions and a biospheric CO2 component that varies diurnally and seasonally.
Markella Prokopiou, Patricia Martinerie, Célia J. Sapart, Emmanuel Witrant, Guillaume Monteil, Kentaro Ishijima, Sophie Bernard, Jan Kaiser, Ingeborg Levin, Thomas Blunier, David Etheridge, Ed Dlugokencky, Roderik S. W. van de Wal, and Thomas Röckmann
Atmos. Chem. Phys., 17, 4539–4564, https://doi.org/10.5194/acp-17-4539-2017, https://doi.org/10.5194/acp-17-4539-2017, 2017
Short summary
Short summary
Nitrous oxide is the third most important anthropogenic greenhouse gas with an increasing mole fraction. To understand its natural and anthropogenic sources
we employ isotope measurements. Results show that while the N2O mole fraction increases, its heavy isotope content decreases. The isotopic changes observed underline the dominance of agricultural emissions especially at the early part of the record, whereas in the later decades the contribution from other anthropogenic sources increases.
Sakiko Ishino, Shohei Hattori, Joel Savarino, Bruno Jourdain, Susanne Preunkert, Michel Legrand, Nicolas Caillon, Albane Barbero, Kota Kuribayashi, and Naohiro Yoshida
Atmos. Chem. Phys., 17, 3713–3727, https://doi.org/10.5194/acp-17-3713-2017, https://doi.org/10.5194/acp-17-3713-2017, 2017
Short summary
Short summary
We show the first simultaneous observations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal Antarctica. The contrasting seasonal trends between oxygen isotopes of ozone and those of sulfate and nitrate indicate that these signatures in sulfate and nitrate are mainly controlled by changes in oxidation chemistry. We also discuss the specific oxidation chemistry induced by the unique phenomena at the site.
Giulia Zazzeri, Dave Lowry, Rebecca E. Fisher, James L. France, Mathias Lanoisellé, Bryce F. J. Kelly, Jaroslaw M. Necki, Charlotte P. Iverach, Elisa Ginty, Miroslaw Zimnoch, Alina Jasek, and Euan G. Nisbet
Atmos. Chem. Phys., 16, 13669–13680, https://doi.org/10.5194/acp-16-13669-2016, https://doi.org/10.5194/acp-16-13669-2016, 2016
Short summary
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Methane emissions estimates from the coal sector are highly uncertain. Precise δ13C isotopic signatures of methane sources can be used in atmospheric models for a methane budget assessment. Emissions from both underground and opencast coal mines in the UK, Australia and Poland were sampled and isotopically characterised using high-precision measurements of δ13C values. Representative isotopic signatures were provided, taking into account specific ranks of coal and mine type.
Qiang Huang, Jiubin Chen, Weilin Huang, Pingqing Fu, Benjamin Guinot, Xinbin Feng, Lihai Shang, Zhuhong Wang, Zhongwei Wang, Shengliu Yuan, Hongming Cai, Lianfang Wei, and Ben Yu
Atmos. Chem. Phys., 16, 11773–11786, https://doi.org/10.5194/acp-16-11773-2016, https://doi.org/10.5194/acp-16-11773-2016, 2016
Short summary
Short summary
Atmospheric airborne mercury is of particular concern because, once inhaled, both Hg and its vectors might have adverse effects on human beings. In this study, we attempted to identify the sources of PM2.5-Hg in Beijing, China, using Hg isotopic composition. Large range and seasonal variations in both mass-dependent and mass-independent fractionations of Hg isotopes in haze particles demonstrate the usefulness of Hg isotopes for directly tracing the sources and its vectors in the atmosphere.
Qianjie Chen, Lei Geng, Johan A. Schmidt, Zhouqing Xie, Hui Kang, Jordi Dachs, Jihong Cole-Dai, Andrew J. Schauer, Madeline G. Camp, and Becky Alexander
Atmos. Chem. Phys., 16, 11433–11450, https://doi.org/10.5194/acp-16-11433-2016, https://doi.org/10.5194/acp-16-11433-2016, 2016
Short summary
Short summary
The formation mechanisms of sulfate in the marine boundary layer are not well understood, which could result in large uncertainties in aerosol radiative forcing. We measure the oxygen isotopic composition (Δ17O) of sulfate collected in the MBL and analyze with a global transport model. Our results suggest that 33–50 % of MBL sulfate is formed via oxidation of S(IV) by hypohalous acids HOBr / HOCl in the aqueous phase, and the daily-mean HOBr/HOCl concentrations are on the order of 0.01–0.1 ppt.
Thomas Röckmann, Simon Eyer, Carina van der Veen, Maria E. Popa, Béla Tuzson, Guillaume Monteil, Sander Houweling, Eliza Harris, Dominik Brunner, Hubertus Fischer, Giulia Zazzeri, David Lowry, Euan G. Nisbet, Willi A. Brand, Jaroslav M. Necki, Lukas Emmenegger, and Joachim Mohn
Atmos. Chem. Phys., 16, 10469–10487, https://doi.org/10.5194/acp-16-10469-2016, https://doi.org/10.5194/acp-16-10469-2016, 2016
Short summary
Short summary
A dual isotope ratio mass spectrometric system (IRMS) and a quantum cascade laser absorption spectroscopy (QCLAS)-based technique were deployed at the Cabauw experimental site for atmospheric research (CESAR) in the Netherlands and performed in situ, high-frequency (approx. hourly) measurements for a period of more than 5 months, yielding a combined dataset with more than 2500 measurements of both δ13C and δD.
T. A. Berhanu, J. Savarino, J. Erbland, W. C. Vicars, S. Preunkert, J. F. Martins, and M. S. Johnson
Atmos. Chem. Phys., 15, 11243–11256, https://doi.org/10.5194/acp-15-11243-2015, https://doi.org/10.5194/acp-15-11243-2015, 2015
Short summary
Short summary
In this field study at Dome C, Antarctica, we investigated the effect of solar UV photolysis on the stable isotopes of nitrate in snow via comparison of two identical snow pits while exposing only one to solar UV. From the difference between the average isotopic fractionations calculated for each pit, we determined a purely photolytic nitrogen isotopic fractionation of -55.8‰, in good agreement with what has been recently determined in a laboratory study.
M. Saccon, A. Kornilova, L. Huang, S. Moukhtar, and J. Rudolph
Atmos. Chem. Phys., 15, 10825–10838, https://doi.org/10.5194/acp-15-10825-2015, https://doi.org/10.5194/acp-15-10825-2015, 2015
E. D. Sofen, B. Alexander, E. J. Steig, M. H. Thiemens, S. A. Kunasek, H. M. Amos, A. J. Schauer, M. G. Hastings, J. Bautista, T. L. Jackson, L. E. Vogel, J. R. McConnell, D. R. Pasteris, and E. S. Saltzman
Atmos. Chem. Phys., 14, 5749–5769, https://doi.org/10.5194/acp-14-5749-2014, https://doi.org/10.5194/acp-14-5749-2014, 2014
J. Wintel, E. Hösen, R. Koppmann, M. Krebsbach, A. Hofzumahaus, and F. Rohrer
Atmos. Chem. Phys., 13, 11059–11071, https://doi.org/10.5194/acp-13-11059-2013, https://doi.org/10.5194/acp-13-11059-2013, 2013
F. A. Haumann, A. M. Batenburg, G. Pieterse, C. Gerbig, M. C. Krol, and T. Röckmann
Atmos. Chem. Phys., 13, 9401–9413, https://doi.org/10.5194/acp-13-9401-2013, https://doi.org/10.5194/acp-13-9401-2013, 2013
C. J. Sapart, P. Martinerie, E. Witrant, J. Chappellaz, R. S. W. van de Wal, P. Sperlich, C. van der Veen, S. Bernard, W. T. Sturges, T. Blunier, J. Schwander, D. Etheridge, and T. Röckmann
Atmos. Chem. Phys., 13, 6993–7005, https://doi.org/10.5194/acp-13-6993-2013, https://doi.org/10.5194/acp-13-6993-2013, 2013
J. Erbland, W. C. Vicars, J. Savarino, S. Morin, M. M. Frey, D. Frosini, E. Vince, and J. M. F. Martins
Atmos. Chem. Phys., 13, 6403–6419, https://doi.org/10.5194/acp-13-6403-2013, https://doi.org/10.5194/acp-13-6403-2013, 2013
A. Guillon, K. Le Ménach, P.-M. Flaud, N. Marchand, H. Budzinski, and E. Villenave
Atmos. Chem. Phys., 13, 2703–2719, https://doi.org/10.5194/acp-13-2703-2013, https://doi.org/10.5194/acp-13-2703-2013, 2013
D. Ceburnis, A. Garbaras, S. Szidat, M. Rinaldi, S. Fahrni, N. Perron, L. Wacker, S. Leinert, V. Remeikis, M. C. Facchini, A. S. H. Prevot, S. G. Jennings, M. Ramonet, and C. D. O'Dowd
Atmos. Chem. Phys., 11, 8593–8606, https://doi.org/10.5194/acp-11-8593-2011, https://doi.org/10.5194/acp-11-8593-2011, 2011
A. M. Batenburg, S. Walter, G. Pieterse, I. Levin, M. Schmidt, A. Jordan, S. Hammer, C. Yver, and T. Röckmann
Atmos. Chem. Phys., 11, 6985–6999, https://doi.org/10.5194/acp-11-6985-2011, https://doi.org/10.5194/acp-11-6985-2011, 2011
B. Tuzson, S. Henne, D. Brunner, M. Steinbacher, J. Mohn, B. Buchmann, and L. Emmenegger
Atmos. Chem. Phys., 11, 1685–1696, https://doi.org/10.5194/acp-11-1685-2011, https://doi.org/10.5194/acp-11-1685-2011, 2011
Y. T. Fang, K. Koba, X. M. Wang, D. Z. Wen, J. Li, Y. Takebayashi, X. Y. Liu, and M. Yoh
Atmos. Chem. Phys., 11, 1313–1325, https://doi.org/10.5194/acp-11-1313-2011, https://doi.org/10.5194/acp-11-1313-2011, 2011
S. S. Assonov, C. A. M. Brenninkmeijer, T. J. Schuck, and P. Taylor
Atmos. Chem. Phys., 10, 8575–8599, https://doi.org/10.5194/acp-10-8575-2010, https://doi.org/10.5194/acp-10-8575-2010, 2010
U. Tsunogai, D. D. Komatsu, S. Daita, G. A. Kazemi, F. Nakagawa, I. Noguchi, and J. Zhang
Atmos. Chem. Phys., 10, 1809–1820, https://doi.org/10.5194/acp-10-1809-2010, https://doi.org/10.5194/acp-10-1809-2010, 2010
M. M. Frey, J. Savarino, S. Morin, J. Erbland, and J. M. F. Martins
Atmos. Chem. Phys., 9, 8681–8696, https://doi.org/10.5194/acp-9-8681-2009, https://doi.org/10.5194/acp-9-8681-2009, 2009
S. A. Vay, S. C. Tyler, Y. Choi, D. R. Blake, N. J. Blake, G. W. Sachse, G. S. Diskin, and H. B. Singh
Atmos. Chem. Phys., 9, 4973–4985, https://doi.org/10.5194/acp-9-4973-2009, https://doi.org/10.5194/acp-9-4973-2009, 2009
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Short summary
Atmospheric nitrate is collected on the East Antarctic ice sheet. Nitrogen and oxygen stable isotopes and concentrations of nitrate are measured. Using a box model, we show that there is s systematic discrepancy between observations and model results. We suggest that this discrepancy probably results from unknown NOx chemistry above the Antarctic ice sheet. However, possible misconception in the stable isotope mass balance is not completely excluded.
Atmospheric nitrate is collected on the East Antarctic ice sheet. Nitrogen and oxygen stable...
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