Articles | Volume 16, issue 7
https://doi.org/10.5194/tc-16-2709-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/tc-16-2709-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
12 Jul 2022
Research article |
| 12 Jul 2022
| 12 Jul 2022
Impacts of post-depositional processing on nitrate isotopes in the snow and the overlying atmosphere at Summit, Greenland
Zhuang Jiang
School of Earth and Space Sciences, University of Science and Technology of
China, Hefei, Anhui, China
Joel Savarino
Univ. Grenoble Alpes, CNRS, IRD, G-INP, Institut des Géosciences
de l'Environnement, Grenoble, France
Becky Alexander
Department of Atmospheric Sciences, University of Washington, Seattle,
WA, USA
Joseph Erbland
Univ. Grenoble Alpes, CNRS, IRD, G-INP, Institut des Géosciences
de l'Environnement, Grenoble, France
Jean-Luc Jaffrezo
Univ. Grenoble Alpes, CNRS, IRD, G-INP, Institut des Géosciences
de l'Environnement, Grenoble, France
School of Earth and Space Sciences, University of Science and Technology of
China, Hefei, Anhui, China
Laboratory for Ocean Dynamics and Climate, Pilot National
Laboratory for Marine Science and Technology (Qingdao), Qingdao, Shandong, China
CAS Center for Excellence in Comparative Planetology, University of
Science and Technology of China, Hefei, Anhui, China
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Dimethyl sulfide (DMS) is mostly emitted from ocean surfaces and represents the largest natural source of sulfur for the atmosphere. Once in the atmosphere, DMS forms stable oxidation products such as SO2 and H2SO4, which can subsequently contribute to airborne particle formation and growth. In this study, we update the DMS oxidation mechanism in the chemical transport model GEOS-Chem and describe resulting changes in particle growth as well as the overall global sulfur budget.
Julie Camman, Benjamin Chazeau, Nicolas Marchand, Amandine Durand, Grégory Gille, Ludovic Lanzi, Jean-Luc Jaffrezo, Henri Wortham, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 3257–3278, https://doi.org/10.5194/acp-24-3257-2024, https://doi.org/10.5194/acp-24-3257-2024, 2024
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Fine particle (PM1) pollution is a major health issue in the city of Marseille, which is subject to numerous pollution sources. Sampling carried out during the summer enabled a fine characterization of the PM1 sources and their oxidative potential, a promising new metric as a proxy for health impact. PM1 came mainly from combustion sources, secondary ammonium sulfate, and organic nitrate, while the oxidative potential of PM1 came from these sources and from resuspended dust in the atmosphere.
C. Isabel Moreno, Radovan Krejci, Jean-Luc Jaffrezo, Gaëlle Uzu, Andrés Alastuey, Marcos F. Andrade, Valeria Mardóñez, Alkuin Maximilian Koenig, Diego Aliaga, Claudia Mohr, Laura Ticona, Fernando Velarde, Luis Blacutt, Ricardo Forno, David N. Whiteman, Alfred Wiedensohler, Patrick Ginot, and Paolo Laj
Atmos. Chem. Phys., 24, 2837–2860, https://doi.org/10.5194/acp-24-2837-2024, https://doi.org/10.5194/acp-24-2837-2024, 2024
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Aerosol chemical composition (ions, sugars, carbonaceous matter) from 2011 to 2020 was studied at Mt. Chacaltaya (5380 m a.s.l., Bolivian Andes). Minimum concentrations occur in the rainy season with maxima in the dry and transition seasons. The origins of the aerosol are located in a radius of hundreds of kilometers: nearby urban and rural areas, natural biogenic emissions, vegetation burning from Amazonia and Chaco, Pacific Ocean emissions, soil dust, and Peruvian volcanism.
Sarah Albertin, Joël Savarino, Slimane Bekki, Albane Barbero, Roberto Grilli, Quentin Fournier, Irène Ventrillard, Nicolas Caillon, and Kathy Law
Atmos. Chem. Phys., 24, 1361–1388, https://doi.org/10.5194/acp-24-1361-2024, https://doi.org/10.5194/acp-24-1361-2024, 2024
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This study reports the first simultaneous records of oxygen (Δ17O) and nitrogen (δ15N) isotopes in nitrogen dioxide (NO2) and nitrate (NO3−). These data are combined with atmospheric observations to explore sub-daily N reactive chemistry and quantify N fractionation effects in an Alpine winter city. The results highlight the necessity of using Δ17O and δ15N in both NO2 and NO3− to avoid biased estimations of NOx sources and fates from NO3− isotopic records in urban winter environments.
Máté Vörösmarty, Gaëlle Uzu, Jean-Luc Jaffrezo, Pamela Dominutti, Zsófia Kertész, Enikő Papp, and Imre Salma
Atmos. Chem. Phys., 23, 14255–14269, https://doi.org/10.5194/acp-23-14255-2023, https://doi.org/10.5194/acp-23-14255-2023, 2023
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Poor air quality caused by high concentrations of particulate matter is one of the most severe public health concerns for humans worldwide. One of the most important biological mechanisms inducing adverse health effects is the oxidant–antioxidant imbalance. We showed that the oxidative stress changed substantially and in a complex manner with location and season. Biomass burning exhibited the dominant influence, while motor vehicles played an important role in the non-heating period.
Valeria Mardoñez, Marco Pandolfi, Lucille Joanna S. Borlaza, Jean-Luc Jaffrezo, Andrés Alastuey, Jean-Luc Besombes, Isabel Moreno R., Noemi Perez, Griša Močnik, Patrick Ginot, Radovan Krejci, Vladislav Chrastny, Alfred Wiedensohler, Paolo Laj, Marcos Andrade, and Gaëlle Uzu
Atmos. Chem. Phys., 23, 10325–10347, https://doi.org/10.5194/acp-23-10325-2023, https://doi.org/10.5194/acp-23-10325-2023, 2023
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La Paz and El Alto are two fast-growing, high-altitude Bolivian cities forming the second-largest metropolitan area in the country. The sources of particulate matter (PM) in this conurbation were not previously investigated. This study identified 11 main sources of PM, of which dust and vehicular emissions stand out as the main ones. The influence of regional biomass combustion and local waste combustion was also observed, with the latter being a major source of hazardous compounds.
Alexis Lamothe, Joel Savarino, Patrick Ginot, Lison Soussaintjean, Elsa Gautier, Pete D. Akers, Nicolas Caillon, and Joseph Erbland
Atmos. Meas. Tech., 16, 4015–4030, https://doi.org/10.5194/amt-16-4015-2023, https://doi.org/10.5194/amt-16-4015-2023, 2023
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Ammonia is a reactive gas in our atmosphere that is key in air quality issues. Assessing its emissions and how it reacts is a hot topic that can be addressed from the past. Stable isotopes (the mass of the molecule) measured in ice cores (glacial archives) can teach us a lot. However, the concentrations in ice cores are very small. We propose a protocol to limit the contamination and apply it to one ice core drilled in Mont Blanc, describing the opportunities our method brings.
Simone Ventisette, Samuele Baldini, Claudio Artoni, Silvia Becagli, Laura Caiazzo, Barbara Delmonte, Massimo Frezzotti, Raffaello Nardin, Joel Savarino, Mirko Severi, Andrea Spolaor, Barbara Stenni, and Rita Traversi
EGUsphere, https://doi.org/10.5194/egusphere-2023-393, https://doi.org/10.5194/egusphere-2023-393, 2023
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The paper reports the spatial variability of concentration and fluxes of chemical impurities in superficial snow over unexplored area of the East Antarctic ice sheet. Pinatubo and Puyehue-Cordón Caulle volcanic eruptions in non-sea salt sulfate and dust snow pits record were used to achieve the accumulation rates. Deposition (wet, dry and uptake from snow surface) and post deposition processes are constrained. These knowledges are fundamental in Antarctic ice cores stratigraphies interpretation.
Wiebke Scholz, Jiali Shen, Diego Aliaga, Cheng Wu, Samara Carbone, Isabel Moreno, Qiaozhi Zha, Wei Huang, Liine Heikkinen, Jean Luc Jaffrezo, Gaelle Uzu, Eva Partoll, Markus Leiminger, Fernando Velarde, Paolo Laj, Patrick Ginot, Paolo Artaxo, Alfred Wiedensohler, Markku Kulmala, Claudia Mohr, Marcos Andrade, Victoria Sinclair, Federico Bianchi, and Armin Hansel
Atmos. Chem. Phys., 23, 895–920, https://doi.org/10.5194/acp-23-895-2023, https://doi.org/10.5194/acp-23-895-2023, 2023
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Dimethyl sulfide (DMS), emitted from the ocean, is the most abundant biogenic sulfur emission into the atmosphere. OH radicals, among others, can oxidize DMS to sulfuric and methanesulfonic acid, which are relevant for aerosol formation. We quantified DMS and nearly all DMS oxidation products with novel mass spectrometric instruments for gas and particle phase at the high mountain station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes in free tropospheric air after long-range transport.
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.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
Atmos. Chem. Phys., 22, 14467–14488, https://doi.org/10.5194/acp-22-14467-2022, https://doi.org/10.5194/acp-22-14467-2022, 2022
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Radical bromine molecules are seen at higher concentrations during the Arctic spring. We use the global model GEOS-Chem to test whether snowpack and wind-blown snow sources can explain high bromine concentrations. We run this model for the entire year of 2015 and compare results to observations of bromine from floating platforms on the Arctic Ocean and at Utqiaġvik. We find that the model performs best when both sources are enabled but may overestimate bromine production in summer and fall.
Yanzhi Cao, Zhuang Jiang, Becky Alexander, Jihong Cole-Dai, Joel Savarino, Joseph Erbland, and Lei Geng
Atmos. Chem. Phys., 22, 13407–13422, https://doi.org/10.5194/acp-22-13407-2022, https://doi.org/10.5194/acp-22-13407-2022, 2022
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We investigate the potential of ice-core preserved nitrate isotopes as proxies of stratospheric ozone variability by measuring nitrate isotopes in a shallow ice core from the South Pole. The large variability in the snow accumulation rate and its slight increase after the 1970s masked any signals caused by the ozone hole. Moreover, the nitrate oxygen isotope decrease may reflect changes in the atmospheric oxidation environment in the Southern Ocean.
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.
Xueyin Ruan, Chun Zhao, Rahul A. Zaveri, Pengzhen He, Xinming Wang, Jingyuan Shao, and Lei Geng
Geosci. Model Dev., 15, 6143–6164, https://doi.org/10.5194/gmd-15-6143-2022, https://doi.org/10.5194/gmd-15-6143-2022, 2022
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Accurate prediction of aerosol pH in chemical transport models is essential to aerosol modeling. This study examines the performance of the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) on aerosol pH predictions and the sensitivities to emissions of nonvolatile cations and NH3, aerosol-phase state assumption, and heterogeneous sulfate production. Temporal evolution of aerosol pH during haze cycles in Beijing and the driving factors are also presented and discussed.
Lucille Joanna Borlaza, Samuël Weber, Anouk Marsal, Gaëlle Uzu, Véronique Jacob, Jean-Luc Besombes, Mélodie Chatain, Sébastien Conil, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 22, 8701–8723, https://doi.org/10.5194/acp-22-8701-2022, https://doi.org/10.5194/acp-22-8701-2022, 2022
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A 9-year dataset of the chemical and oxidative potential (OP) of PM10 was investigated at a rural background site. Extensive source apportionment led to identification of differences in source impacts between mass and OP, underlining the importance of PM redox activity when considering health effects. The influence of mixing and ageing processes was also tackled. Traffic contributions have decreased here over the years, attributed to regulations limiting vehicular emissions in bigger cities.
Stuart K. Grange, Gaëlle Uzu, Samuël Weber, Jean-Luc Jaffrezo, and Christoph Hueglin
Atmos. Chem. Phys., 22, 7029–7050, https://doi.org/10.5194/acp-22-7029-2022, https://doi.org/10.5194/acp-22-7029-2022, 2022
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Oxidative potential (OP), a biologically relevant metric for particulate matter (PM), was linked to PM10 and PM2.5 sources and constituents across Switzerland between 2018 and 2019. Wood burning and non-exhaust traffic emissions were identified as key processes that led to enhanced OP. Therefore, the make-up of the PM mix was very important for OP. The results highlight the importance of the management of wood burning and non-exhaust emissions to reduce OP, and presumably biological harm.
Adam Brighty, Véronique Jacob, Gaëlle Uzu, Lucille Borlaza, Sébastien Conil, Christoph Hueglin, Stuart K. Grange, Olivier Favez, Cécile Trébuchon, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 22, 6021–6043, https://doi.org/10.5194/acp-22-6021-2022, https://doi.org/10.5194/acp-22-6021-2022, 2022
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With an revised analytical method and long-term sampling strategy, we have been able to elucidate much more information about atmospheric plant debris, a poorly understood class of particulate matter. We found weaker seasonal patterns at urban locations compared to rural locations and significant interannual variability in concentrations between previous years and 2020, during the COVID-19 pandemic. This suggests a possible man-made influence on plant debris concentration and source strength.
Saehee Lim, Meehye Lee, Joel Savarino, and Paolo Laj
Atmos. Chem. Phys., 22, 5099–5115, https://doi.org/10.5194/acp-22-5099-2022, https://doi.org/10.5194/acp-22-5099-2022, 2022
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We determined δ15N(NO3−) and Δ17O(NO3−) of PM2.5 in Seoul during 2018–2019 and estimated quantitatively the contribution of oxidation pathways to NO3− formation and NOx emission sources. The nighttime pathway played a significant role in NO3− formation during the winter, and its contribution further increased up to 70 % on haze days when PM2.5 was greater than 75 µg m−3. Vehicle emissions were confirmed as a main NO3− source with an increasing contribution from coal combustion in winter.
Pamela A. Dominutti, Pascal Renard, Mickaël Vaïtilingom, Angelica Bianco, Jean-Luc Baray, Agnès Borbon, Thierry Bourianne, Frédéric Burnet, Aurélie Colomb, Anne-Marie Delort, Valentin Duflot, Stephan Houdier, Jean-Luc Jaffrezo, Muriel Joly, Martin Leremboure, Jean-Marc Metzger, Jean-Marc Pichon, Mickaël Ribeiro, Manon Rocco, Pierre Tulet, Anthony Vella, Maud Leriche, and Laurent Deguillaume
Atmos. Chem. Phys., 22, 505–533, https://doi.org/10.5194/acp-22-505-2022, https://doi.org/10.5194/acp-22-505-2022, 2022
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We present here the results obtained during an intensive field campaign conducted in March to April 2019 in Reunion. Our study integrates a comprehensive chemical and microphysical characterization of cloud water. Our investigations reveal that air mass history and cloud microphysical properties do not fully explain the variability observed in their chemical composition. This highlights the complexity of emission sources, multiphasic exchanges, and transformations in clouds.
Laura Crick, Andrea Burke, William Hutchison, Mika Kohno, Kathryn A. Moore, Joel Savarino, Emily A. Doyle, Sue Mahony, Sepp Kipfstuhl, James W. B. Rae, Robert C. J. Steele, R. Stephen J. Sparks, and Eric W. Wolff
Clim. Past, 17, 2119–2137, https://doi.org/10.5194/cp-17-2119-2021, https://doi.org/10.5194/cp-17-2119-2021, 2021
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The ~ 74 ka eruption of Toba was one of the largest eruptions of the last 100 ka. We have measured the sulfur isotopic composition for 11 Toba eruption candidates in two Antarctic ice cores. Sulfur isotopes allow us to distinguish between large eruptions that have erupted material into the stratosphere and smaller ones that reach lower altitudes. Using this we have identified the events most likely to be Toba and place the eruption on the transition into a cold period in the Northern Hemisphere.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Zhuang Jiang, Becky Alexander, Joel Savarino, Joseph Erbland, and Lei Geng
The Cryosphere, 15, 4207–4220, https://doi.org/10.5194/tc-15-4207-2021, https://doi.org/10.5194/tc-15-4207-2021, 2021
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We used a snow photochemistry model (TRANSITS) to simulate the seasonal nitrate snow profile at Summit, Greenland. Comparisons between model outputs and observations suggest that at Summit post-depositional processing is active and probably dominates the snowpack δ15N seasonality. We also used the model to assess the degree of snow nitrate loss and the consequences in its isotopes at present and in the past, which helps for quantitative interpretations of ice-core nitrate records.
Samuël Weber, Gaëlle Uzu, Olivier Favez, Lucille Joanna S. Borlaza, Aude Calas, Dalia Salameh, Florie Chevrier, Julie Allard, Jean-Luc Besombes, Alexandre Albinet, Sabrina Pontet, Boualem Mesbah, Grégory Gille, Shouwen Zhang, Cyril Pallares, Eva Leoz-Garziandia, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 21, 11353–11378, https://doi.org/10.5194/acp-21-11353-2021, https://doi.org/10.5194/acp-21-11353-2021, 2021
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Oxidative potential (OP) of aerosols is apportioned to the main PM sources found in 15 sites over France. The sources present clear distinct intrinsic OPs at a large geographic scale, and a drastic redistribution between the mass concentration and OP measured by both ascorbic acid and dithiothreitol is highlighted. Moreover, the high discrepancy between the mean and median contributions of the sources to the given metrics raises some important questions when dealing with health endpoints.
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.
Lucille Joanna S. Borlaza, Samuël Weber, Jean-Luc Jaffrezo, Stephan Houdier, Rémy Slama, Camille Rieux, Alexandre Albinet, Steve Micallef, Cécile Trébluchon, and Gaëlle Uzu
Atmos. Chem. Phys., 21, 9719–9739, https://doi.org/10.5194/acp-21-9719-2021, https://doi.org/10.5194/acp-21-9719-2021, 2021
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With an enhanced source apportionment obtained in a companion paper, this paper acquires more understanding of the spatiotemporal associations of the sources of PM to oxidative potential (OP), an emerging health-based metric. Multilayer perceptron neural network analysis was used to apportion OP from PM sources. Results showed that such a methodology is as robust as the linear classical inversion and permits an improvement in the OP prediction when local features or non-linear effects occur.
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.
Vincent Michoud, Elise Hallemans, Laura Chiappini, Eva Leoz-Garziandia, Aurélie Colomb, Sébastien Dusanter, Isabelle Fronval, François Gheusi, Jean-Luc Jaffrezo, Thierry Léonardis, Nadine Locoge, Nicolas Marchand, Stéphane Sauvage, Jean Sciare, and Jean-François Doussin
Atmos. Chem. Phys., 21, 8067–8088, https://doi.org/10.5194/acp-21-8067-2021, https://doi.org/10.5194/acp-21-8067-2021, 2021
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A multiphasic molecular characterization of oxygenated compounds has been carried out during the ChArMEx field campaign using offline analysis. It leads to the identification of 97 different compounds in the gas and aerosol phases and reveals the important contribution of organic acids to organic aerosol. In addition, comparison between experimental and theoretical partitioning coefficients revealed in most cases a large underestimation by the theory reaching 1 to 7 orders of magnitude.
Lucille Joanna S. Borlaza, Samuël Weber, Gaëlle Uzu, Véronique Jacob, Trishalee Cañete, Steve Micallef, Cécile Trébuchon, Rémy Slama, Olivier Favez, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 21, 5415–5437, https://doi.org/10.5194/acp-21-5415-2021, https://doi.org/10.5194/acp-21-5415-2021, 2021
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This study focuses on fully discriminating the origins of particulates by tackling specific secondary organic aerosol (SOA) sources that are difficult to resolve using traditional datasets, especially at a city scale. This is done through the use of additional fit-for-purpose tracers in the Positive Matrix Factorization (PMF) model, which can be obtained using simpler and more targeted techniques, and the comparison of the PMF models from sites in close range but with different urban typologies.
Martin Rigler, Luka Drinovec, Gašper Lavrič, Athanasia Vlachou, André S. H. Prévôt, Jean Luc Jaffrezo, Iasonas Stavroulas, Jean Sciare, Judita Burger, Irena Kranjc, Janja Turšič, Anthony D. A. Hansen, and Griša Močnik
Atmos. Meas. Tech., 13, 4333–4351, https://doi.org/10.5194/amt-13-4333-2020, https://doi.org/10.5194/amt-13-4333-2020, 2020
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Carbonaceous aerosols are a large fraction of fine particulate matter. They are extremely diverse, and they directly impact air quality, visibility, cloud formation and public health. In this paper we present a new instrument and new method to measure carbon content in particulate matter in real time and at a high time resolution. The new method was validated in a 1-month winter field campaign in Ljubljana, Slovenia.
Albane Barbero, Camille Blouzon, Joël Savarino, Nicolas Caillon, Aurélien Dommergue, and Roberto Grilli
Atmos. Meas. Tech., 13, 4317–4331, https://doi.org/10.5194/amt-13-4317-2020, https://doi.org/10.5194/amt-13-4317-2020, 2020
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In this paper, we present a compact, affordable and robust instrument for in situ measurements of different trace gases: NOx, IO, CHOCHO and O3 with very low detection limits. The device weighs 15 kg and has a total electrical power consumption of < 300 W. Its very low detection limits and its design make it suitable for field applications to address different questions such as how to better constrain the oxidative capacity of the atmosphere and study the chemistry of highly reactive species.
Lu Qi, Alexander L. Vogel, Sepideh Esmaeilirad, Liming Cao, Jing Zheng, Jean-Luc Jaffrezo, Paola Fermo, Anne Kasper-Giebl, Kaspar R. Daellenbach, Mindong Chen, Xinlei Ge, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 20, 7875–7893, https://doi.org/10.5194/acp-20-7875-2020, https://doi.org/10.5194/acp-20-7875-2020, 2020
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We present the first application of this online and offline strategy using the new extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF), which achieves increased chemical specificity relative to other online techniques. Measurement and source apportionment of 1 year of filter samples collected in Zurich, Switzerland, show seasonal contributions from fresh and aged wood combustion in winter and biogenic emission-derived SOA in summer, as well as other sources.
Jiayue Huang, Lyatt Jaeglé, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mat J. Evans, Nicolas Theys, and Sungyeon Choi
Atmos. Chem. Phys., 20, 7335–7358, https://doi.org/10.5194/acp-20-7335-2020, https://doi.org/10.5194/acp-20-7335-2020, 2020
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Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often observed in the springtime Arctic. Here, we use a chemical transport model to examine the role of sea salt aerosol from blowing snow in explaining these phenomena. We find that our simulation can account for the spatiotemporal variability of satellite observations of BrO. However, the model has difficulty in producing the magnitude of observed ozone depletion events.
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.
Abdoulaye Samaké, Aurélie Bonin, Jean-Luc Jaffrezo, Pierre Taberlet, Samuël Weber, Gaëlle Uzu, Véronique Jacob, Sébastien Conil, and Jean M. F. Martins
Atmos. Chem. Phys., 20, 5609–5628, https://doi.org/10.5194/acp-20-5609-2020, https://doi.org/10.5194/acp-20-5609-2020, 2020
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Despite being a major source of coarse organic matter, primary biogenic organic aerosols (PBOAs) remain poorly implemented in source-resolved chemical transport models. This study, based on an intensive field sampling of aerosols, combined physicochemical characterizations of PM10 with DNA high-throughput sequencing to provide a comprehensive understanding of the microbial fingerprints associated with primary sugar compounds (tracers of PBOAs) and their main surrounding environmental sources.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Detlev Helmig, Daniel Liptzin, Jacques Hueber, and Joel Savarino
The Cryosphere, 14, 199–209, https://doi.org/10.5194/tc-14-199-2020, https://doi.org/10.5194/tc-14-199-2020, 2020
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We present 15 months of trace gas observations from air withdrawn within the snowpack and from above the snow at Concordia Station in Antarctica. The data show occasional positive spikes, indicative of pollution from the station generator. The pollution signal can be seen in snowpack air shortly after it is observed above the snow surface, and lasting for up to several days, much longer than above the surface.
Abdoulaye Samaké, Jean-Luc Jaffrezo, Olivier Favez, Samuël Weber, Véronique Jacob, Trishalee Canete, Alexandre Albinet, Aurélie Charron, Véronique Riffault, Esperanza Perdrix, Antoine Waked, Benjamin Golly, Dalia Salameh, Florie Chevrier, Diogo Miguel Oliveira, Jean-Luc Besombes, Jean M. F. Martins, Nicolas Bonnaire, Sébastien Conil, Géraldine Guillaud, Boualem Mesbah, Benoit Rocq, Pierre-Yves Robic, Agnès Hulin, Sébastien Le Meur, Maxence Descheemaecker, Eve Chretien, Nicolas Marchand, and Gaëlle Uzu
Atmos. Chem. Phys., 19, 11013–11030, https://doi.org/10.5194/acp-19-11013-2019, https://doi.org/10.5194/acp-19-11013-2019, 2019
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We conducted a large study focusing on the daily (24 h) PM10 sugar compound (SC) concentrations for 16 increasing space-scale sites in France (local to nationwide) over at least 1 complete year. Our main results clearly show distance-dependent covariation patterns, with SC concentrations being highly synchronous at an urban city scale and remaining well correlated throughout the same geographic regions. However, sampling sites located in two distinct geographic areas are poorly correlated.
Athanasia Vlachou, Anna Tobler, Houssni Lamkaddam, Francesco Canonaco, Kaspar R. Daellenbach, Jean-Luc Jaffrezo, María Cruz Minguillón, Marek Maasikmets, Erik Teinemaa, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 7279–7295, https://doi.org/10.5194/acp-19-7279-2019, https://doi.org/10.5194/acp-19-7279-2019, 2019
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The resolution of rotational ambiguity in positive matrix factorization (PMF) models is a major challenge. Here, we developed a method based on bootstrapping and correlations to extract environmentally meaningful solutions from PMF analysis based on offline aerosol mass spectrometry data. The method has been tested on a dataset that covers 1 full year of filter samples collected at three different sites in Estonia.
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
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Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
Kaspar R. Daellenbach, Ivan Kourtchev, Alexander L. Vogel, Emily A. Bruns, Jianhui Jiang, Tuukka Petäjä, Jean-Luc Jaffrezo, Sebnem Aksoyoglu, Markus Kalberer, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 5973–5991, https://doi.org/10.5194/acp-19-5973-2019, https://doi.org/10.5194/acp-19-5973-2019, 2019
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Here we present the molecular composition of the organic aerosol (OA) at an urban site in Central Europe (Zurich, Switzerland) and compare it to smog chamber wood smoke and ambient biogenic secondary OA (SOA) (Orbitrap analyses). Accordingly, we are able to explain the strong seasonality of the molecular composition by aged wood smoke and biogenic SOA during winter and summer. Our results could also explain the predominance of non-fossil organic carbon at European locations throughout the year.
Aurélie Charron, Lucie Polo-Rehn, Jean-Luc Besombes, Benjamin Golly, Christine Buisson, Hervé Chanut, Nicolas Marchand, Géraldine Guillaud, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 19, 5187–5207, https://doi.org/10.5194/acp-19-5187-2019, https://doi.org/10.5194/acp-19-5187-2019, 2019
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This research quantified particulate species that could be used to trace non-exhaust and exhaust traffic emissions. Results showed the important contribution of heavy metals from brake wear to total particulate traffic emissions. In France the traffic largely dominated by diesel vehicles led to important emissions of elemental carbon, as well as significant emissions of low-molecular-weight polycyclic aromatic compounds.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Abdoulaye Samaké, Jean-Luc Jaffrezo, Olivier Favez, Samuël Weber, Véronique Jacob, Alexandre Albinet, Véronique Riffault, Esperanza Perdrix, Antoine Waked, Benjamin Golly, Dalia Salameh, Florie Chevrier, Diogo Miguel Oliveira, Nicolas Bonnaire, Jean-Luc Besombes, Jean M. F. Martins, Sébastien Conil, Géraldine Guillaud, Boualem Mesbah, Benoit Rocq, Pierre-Yves Robic, Agnès Hulin, Sébastien Le Meur, Maxence Descheemaecker, Eve Chretien, Nicolas Marchand, and Gaëlle Uzu
Atmos. Chem. Phys., 19, 3357–3374, https://doi.org/10.5194/acp-19-3357-2019, https://doi.org/10.5194/acp-19-3357-2019, 2019
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The contribution of primary biogenic organic aerosols to PM is barely documented. This work provides a broad overview of the spatiotemporal evolution of concentrations and contributions to OM of dominant primary sugar alcohols and saccharides for a large selection of environmental conditions in France (28 sites and more than 5 340 samples). These chemicals are ubiquitous, and are associated with coarse aerosols. Their concentrations display site-to-site and clear seasonal variations.
Tommaso Galeazzo, Slimane Bekki, Erwan Martin, Joël Savarino, and Stephen R. Arnold
Atmos. Chem. Phys., 18, 17909–17931, https://doi.org/10.5194/acp-18-17909-2018, https://doi.org/10.5194/acp-18-17909-2018, 2018
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Volcanic sulfur can have climatic impacts for the planet via sulfate aerosol formation, leading also to pollution events. We provide model constraints on tropospheric volcanic sulfate formation, with implications for its lifetime and impacts on regional air quality. Oxygen isotope investigations from our model suggest that in the poor tropospheric plumes of halogens, the O2/TMI sulfur oxidation pathway might significantly control sulfate production. The produced sulfate has no isotopic anomaly.
Shaojie Song, Hélène Angot, Noelle E. Selin, Hubert Gallée, Francesca Sprovieri, Nicola Pirrone, Detlev Helmig, Joël Savarino, Olivier Magand, and Aurélien Dommergue
Atmos. Chem. Phys., 18, 15825–15840, https://doi.org/10.5194/acp-18-15825-2018, https://doi.org/10.5194/acp-18-15825-2018, 2018
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Mercury is a trace metal with adverse health effects on human and wildlife. Its unique property makes it undergo long-range transport, and even remote Antarctica receives significant inputs. This paper presents the first model that aims to understand mercury behavior over the Antarctic Plateau. We find that mercury is quickly cycled between snow and air in the sunlit period, likely driven by bromine chemistry, and that several uncertain processes contribute to its behavior in the dark period.
Qianjie Chen, Tomás Sherwen, Mathew Evans, and Becky Alexander
Atmos. Chem. Phys., 18, 13617–13637, https://doi.org/10.5194/acp-18-13617-2018, https://doi.org/10.5194/acp-18-13617-2018, 2018
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Uncertainty in the natural tropospheric sulfur cycle represents the largest source of uncertainty in radiative forcing estimates of sulfate aerosol. This study investigates the natural sulfur cycle in the marine troposphere using the GEOS-Chem model. We found that BrO is important for DMS oxidation and multiphase chemistry is important for MSA production and loss, which have implications for the yield of SO2 and MSA from DMS oxidation and the radiative effect of DMS-derived sulfate aerosol.
Prasad Kasibhatla, Tomás Sherwen, Mathew J. Evans, Lucy J. Carpenter, Chris Reed, Becky Alexander, Qianjie Chen, Melissa P. Sulprizio, James D. Lee, Katie A. Read, William Bloss, Leigh R. Crilley, William C. Keene, Alexander A. P. Pszenny, and Alma Hodzic
Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, https://doi.org/10.5194/acp-18-11185-2018, 2018
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Recent measurements of NOx and HONO suggest that photolysis of particulate nitrate in sea-salt aerosols is important in terms of marine boundary layer oxidant chemistry. We present the first global-scale assessment of the significance of this new chemical pathway for NOx, O3, and OH in the marine boundary layer. We also present a preliminary assessment of the potential impact of photolysis of particulate nitrate associated with other aerosol types on continental boundary layer chemistry.
Samuël Weber, Gaëlle Uzu, Aude Calas, Florie Chevrier, Jean-Luc Besombes, Aurélie Charron, Dalia Salameh, Irena Ježek, Griša Močnik, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 18, 9617–9629, https://doi.org/10.5194/acp-18-9617-2018, https://doi.org/10.5194/acp-18-9617-2018, 2018
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The oxidative potential (OP) of the PM appears to be a relevant proxy of health outcomes from PM exposure. We developed a new statistical model using a coupled approach with positive matrix factorization (PMF) and multiple linear regressions to attribute a redox activity per PM sources. Our results highlight the importance of biomass burning and vehicular sources to explain the observed OP of PM. A different contribution of the sources is observed when considering OP or the mass of the PM10.
Aude Calas, Gaëlle Uzu, Frank J. Kelly, Stephan Houdier, Jean M. F. Martins, Fabrice Thomas, Florian Molton, Aurélie Charron, Christina Dunster, Ana Oliete, Véronique Jacob, Jean-Luc Besombes, Florie Chevrier, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 18, 7863–7875, https://doi.org/10.5194/acp-18-7863-2018, https://doi.org/10.5194/acp-18-7863-2018, 2018
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This study reports on seasonal variations of five oxidative potential (OP) assays of PM from the city of Chamonix over a 1-year period. A detailed PM10 characterization allowed univariate and multivariate regression analyses in order to obtain further insight into groups of chemical species that drive OP measurements. Evidence is presented of intercorrelation assays and seasonal contrasts.
Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Benjamin Chazeau, Gary A. Salazar, Soenke Szidat, Jean-Luc Jaffrezo, Christoph Hueglin, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 6187–6206, https://doi.org/10.5194/acp-18-6187-2018, https://doi.org/10.5194/acp-18-6187-2018, 2018
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Carbonaceous aerosols are related to adverse human health effects, which depend on the aerosol chemical composition and size. Here, we combine aerosol mass spectrometry and radiocarbon measurements of size-resolved samples collected over a long term to identify the origins of primary and secondary carbonaceous aerosols in the fine and coarse modes.
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.
Kaspar R. Daellenbach, Imad El-Haddad, Lassi Karvonen, Athanasia Vlachou, Joel C. Corbin, Jay G. Slowik, Maarten F. Heringa, Emily A. Bruns, Samuel M. Luedin, Jean-Luc Jaffrezo, Sönke Szidat, Andrea Piazzalunga, Raquel Gonzalez, Paola Fermo, Valentin Pflueger, Guido Vogel, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 2155–2174, https://doi.org/10.5194/acp-18-2155-2018, https://doi.org/10.5194/acp-18-2155-2018, 2018
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A novel offline LDI-MS method was developed to analyse particulate matter (PM) collected at multiple sites in central Europe during the entire year of 2013. PM sources were identified by positive matrix factorization. Wood burning emissions were separated according to the burning conditions; inefficient burns had a larger impact on air quality in southern Alpine valleys than in northern Switzerland. Moreover, primary tailpipe exhaust was distinguished from aged/secondary traffic emissions.
Allison N. Schwier, Karine Sellegri, Sébastien Mas, Bruno Charrière, Jorge Pey, Clémence Rose, Brice Temime-Roussel, Jean-Luc Jaffrezo, David Parin, David Picard, Mickael Ribeiro, Greg Roberts, Richard Sempéré, Nicolas Marchand, and Barbara D'Anna
Atmos. Chem. Phys., 17, 14645–14660, https://doi.org/10.5194/acp-17-14645-2017, https://doi.org/10.5194/acp-17-14645-2017, 2017
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In the present paper, we quantify sea-to-air emission fluxes of aerosol to the atmosphere and characterize their physical and chemical properties as a function of the seawater biochemical and physical properties. Fluxes are evaluated with an original approach, a "lab in the field" experiment that preserves the seawater and atmospheric complexity while isolating air-to-sea exchanges from their surroundings. We show different features of the aerosol emission fluxes compared to previous findings.
Kaspar R. Daellenbach, Giulia Stefenelli, Carlo Bozzetti, Athanasia Vlachou, Paola Fermo, Raquel Gonzalez, Andrea Piazzalunga, Cristina Colombi, Francesco Canonaco, Christoph Hueglin, Anne Kasper-Giebl, Jean-Luc Jaffrezo, Federico Bianchi, Jay G. Slowik, Urs Baltensperger, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 13265–13282, https://doi.org/10.5194/acp-17-13265-2017, https://doi.org/10.5194/acp-17-13265-2017, 2017
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We present offline AMS analyses for the organic aerosol (OA) in PM10 at nine sites in central Europe for 2013. Primary OA is separated into traffic, cooking, and wood-burning components. A factor explaining sulfur-containing ions, with an event-driven time series, is also separated. We observe enhanced production of secondary OA (SOA) in summer, following biogenic emissions with temperature. In winter a SOA component is dominant, which correlates with anthropogenic inorganic species.
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.
Carlo Bozzetti, Yuliya Sosedova, Mao Xiao, Kaspar R. Daellenbach, Vidmantas Ulevicius, Vadimas Dudoitis, Genrik Mordas, Steigvilė Byčenkienė, Kristina Plauškaitė, Athanasia Vlachou, Benjamin Golly, Benjamin Chazeau, Jean-Luc Besombes, Urs Baltensperger, Jean-Luc Jaffrezo, Jay G. Slowik, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 117–141, https://doi.org/10.5194/acp-17-117-2017, https://doi.org/10.5194/acp-17-117-2017, 2017
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In this study we present the offline-AMS source apportionment of the submicron organic aerosol (OA) sources conducted over 1 year at three locations in the south east Baltic region, which has so far received small attention. Offline-AMS enabled broadening the AMS spatial and temporal coverage, and provided a full characterization of the OA sources. Source apportionment results revealed that biomass burning and biogenic secondary emissions were the major OA sources during winter and summer.
Maria Zatko, Joseph Erbland, Joel Savarino, Lei Geng, Lauren Easley, Andrew Schauer, Timothy Bates, Patricia K. Quinn, Bonnie Light, David Morison, Hans D. Osthoff, Seth Lyman, William Neff, Bin Yuan, and Becky Alexander
Atmos. Chem. Phys., 16, 13837–13851, https://doi.org/10.5194/acp-16-13837-2016, https://doi.org/10.5194/acp-16-13837-2016, 2016
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This manuscript presents chemical and optical observations collected in the air and snow during UBWOS2014 in eastern Utah. These observations are used to calculate fluxes of reactive nitrogen associated with snow nitrate photolysis. Snow-sourced reactive nitrogen fluxes are compared to reactive nitrogen emission inventories to find that snow-sourced reactive nitrogen is a minor contributor to the reactive nitrogen budget, and thus wintertime ground-level ozone formation, in the Uintah Basin.
Josué Bock, Joël Savarino, and Ghislain Picard
Atmos. Chem. Phys., 16, 12531–12550, https://doi.org/10.5194/acp-16-12531-2016, https://doi.org/10.5194/acp-16-12531-2016, 2016
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We develop a physically based parameterisation of the co-condensation process. Our model includes solid-state diffusion within a snow grain. It reproduces with good agreement the nitrate measurement in surface snow. Winter and summer concentrations are driven respectively by thermodynamic equilibrium and co-condensation. Adsorbed nitrate likely accounts for a minor part. This work shows that co-condensation is required to explain the chemical composition of snow undergoing temperature gradient.
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
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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.
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.
Alexandra Touzeau, Amaëlle Landais, Barbara Stenni, Ryu Uemura, Kotaro Fukui, Shuji Fujita, Sarah Guilbaud, Alexey Ekaykin, Mathieu Casado, Eugeni Barkan, Boaz Luz, Olivier Magand, Grégory Teste, Emmanuel Le Meur, Mélanie Baroni, Joël Savarino, Ilann Bourgeois, and Camille Risi
The Cryosphere, 10, 837–852, https://doi.org/10.5194/tc-10-837-2016, https://doi.org/10.5194/tc-10-837-2016, 2016
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The relationship between water isotope ratios and temperature is investigated in precipitation snow at Vostok and Dome C, as well as in surface snow along traverses. The temporal slope of the linear regression for the precipitation is smaller than the geographical slope. Thus, using the latter could lead to an underestimation of past temperature changes. The processes active at remote sites (best glacial analogs) are explored through a combination of water isotopes in short snow pits.
Michael Sigl, Tyler J. Fudge, Mai Winstrup, Jihong Cole-Dai, David Ferris, Joseph R. McConnell, Ken C. Taylor, Kees C. Welten, Thomas E. Woodruff, Florian Adolphi, Marion Bisiaux, Edward J. Brook, Christo Buizert, Marc W. Caffee, Nelia W. Dunbar, Ross Edwards, Lei Geng, Nels Iverson, Bess Koffman, Lawrence Layman, Olivia J. Maselli, Kenneth McGwire, Raimund Muscheler, Kunihiko Nishiizumi, Daniel R. Pasteris, Rachael H. Rhodes, and Todd A. Sowers
Clim. Past, 12, 769–786, https://doi.org/10.5194/cp-12-769-2016, https://doi.org/10.5194/cp-12-769-2016, 2016
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Here we present a chronology (WD2014) for the upper part (0–2850 m; 31.2 ka BP) of the West Antarctic Ice Sheet (WAIS) Divide ice core, which is based on layer counting of distinctive annual cycles preserved in the elemental, chemical and electrical conductivity records. We validated the chronology by comparing it to independent high-accuracy, absolutely dated chronologies. Given its demonstrated high accuracy, WD2014 can become a reference chronology for the Southern Hemisphere.
Maria Zatko, Lei Geng, Becky Alexander, Eric Sofen, and Katarina Klein
Atmos. Chem. Phys., 16, 2819–2842, https://doi.org/10.5194/acp-16-2819-2016, https://doi.org/10.5194/acp-16-2819-2016, 2016
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We have incorporated an idealized snowpack with a nitrate photolysis parameterization into a global chemical transport model (GEOS-Chem) to examine the implications of snow nitrate photolysis for boundary layer chemistry, the recycling and redistribution of reactive nitrogen, and the preservation of ice-core nitrate in ice cores across Antarctica and Greenland. We also examine the sensitivity of these processes to meteorological parameters and chemical, optical, and physical snow properties.
Joël Savarino, William C. Vicars, Michel Legrand, Suzanne Preunkert, Bruno Jourdain, Markus M. Frey, Alexandre Kukui, Nicolas Caillon, and Jaime Gil Roca
Atmos. Chem. Phys., 16, 2659–2673, https://doi.org/10.5194/acp-16-2659-2016, https://doi.org/10.5194/acp-16-2659-2016, 2016
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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.
E. Gautier, J. Savarino, J. Erbland, A. Lanciki, and P. Possenti
Clim. Past, 12, 103–113, https://doi.org/10.5194/cp-12-103-2016, https://doi.org/10.5194/cp-12-103-2016, 2016
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We evaluate the local-scale variability of a sulfate profile at a low-accumulation site (Dome C, Antarctica) to assess the representativeness of one ice core for volcanic reconstructions. Peak statistical occurrence, depth and flux variability are evaluated from five cores. Due to local-scale variability, 64 volcanic peaks can be identified by a five-cores analysis, while only half of them can be assessed from two cores. Using five cores, the uncertainty of the mean flux is reduced to 29 %.
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.
P. Achakulwisut, L. J. Mickley, L. T. Murray, A. P. K. Tai, J. O. Kaplan, and B. Alexander
Atmos. Chem. Phys., 15, 7977–7998, https://doi.org/10.5194/acp-15-7977-2015, https://doi.org/10.5194/acp-15-7977-2015, 2015
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The atmosphere’s oxidative capacity determines the lifetime of many trace gases important to climate, chemistry, and human health. Yet uncertainties remain about its past variations, its controlling factors, and the radiative forcing of short-lived species it influences. To reduce these uncertainties, we must better quantify the natural emissions and chemical reaction mechanisms of organic compounds in the atmosphere, which play a role in governing the oxidative capacity.
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.
L. Geng, J. Cole-Dai, B. Alexander, J. Erbland, J. Savarino, A. J. Schauer, E. J. Steig, P. Lin, Q. Fu, and M. C. Zatko
Atmos. Chem. Phys., 14, 13361–13376, https://doi.org/10.5194/acp-14-13361-2014, https://doi.org/10.5194/acp-14-13361-2014, 2014
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Examinations on snowpit and firn core results from Summit, Greenland suggest that there are two mechanisms leading to the observed double nitrate peaks in some years in the industrial era: 1) long-rang transport of nitrate and 2) enhanced local photochemical production of nitrate. Both of these mechanisms are related to pollution transport, as the additional nitrate from either direct transport or enhanced local photochemistry requires enhanced nitrogen sources from anthropogenic emissions.
J.-C. Gallet, F. Domine, J. Savarino, M. Dumont, and E. Brun
The Cryosphere, 8, 1205–1215, https://doi.org/10.5194/tc-8-1205-2014, https://doi.org/10.5194/tc-8-1205-2014, 2014
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
L. T. Murray, L. J. Mickley, J. O. Kaplan, E. D. Sofen, M. Pfeiffer, and B. Alexander
Atmos. Chem. Phys., 14, 3589–3622, https://doi.org/10.5194/acp-14-3589-2014, https://doi.org/10.5194/acp-14-3589-2014, 2014
Related subject area
Discipline: Snow | Subject: Snow Chemistry
200-year ice core bromine reconstruction at Dome C (Antarctica): observational and modelling results
Temporal variation of bacterial community and nutrients in Tibetan glacier snowpack
Impacts of the photo-driven post-depositional processing on snow nitrate and its isotopes at Summit, Greenland: a model-based study
Brief communication: Spatial and temporal variations in surface snow chemistry along a traverse from coastal East Antarctica to the ice sheet summit (Dome A)
Brief communication: An alternative method for estimating the scavenging efficiency of black carbon by meltwater over sea ice
Quantifying the light absorption and source attribution of insoluble light-absorbing particles on Tibetan Plateau glaciers between 2013 and 2015
Mercury in the Arctic tundra snowpack: temporal and spatial concentration patterns and trace gas exchanges
Variability of sea salts in ice and firn cores from Fimbul Ice Shelf, Dronning Maud Land, Antarctica
François Burgay, Rafael Pedro Fernández, Delia Segato, Clara Turetta, Christopher S. Blaszczak-Boxe, Rachael H. Rhodes, Claudio Scarchilli, Virginia Ciardini, Carlo Barbante, Alfonso Saiz-Lopez, and Andrea Spolaor
The Cryosphere, 17, 391–405, https://doi.org/10.5194/tc-17-391-2023, https://doi.org/10.5194/tc-17-391-2023, 2023
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The paper presents the first ice-core record of bromine (Br) in the Antarctic plateau. By the observation of the ice core and the application of atmospheric chemical models, we investigate the behaviour of bromine after its deposition into the snowpack, with interest in the effect of UV radiation change connected to the formation of the ozone hole, the role of volcanic deposition, and the possible use of Br to reconstruct past sea ice changes from ice core collect in the inner Antarctic plateau.
Yuying Chen, Keshao Liu, Yongqin Liu, Trista J. Vick-Majors, Feng Wang, and Mukan Ji
The Cryosphere, 16, 1265–1280, https://doi.org/10.5194/tc-16-1265-2022, https://doi.org/10.5194/tc-16-1265-2022, 2022
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We investigated the bacterial communities in surface and subsurface snow samples in a Tibetan Plateau glacier using 16S rRNA gene sequences. Our results revealed rapid temporal changes in nitrogen (including nitrate and ammonium) and bacterial communities in both surface and subsurface snow. These findings advance our understanding of bacterial community variations and bacterial interactions after snow deposition and provide a possible biological explanation for nitrogen dynamics in snow.
Zhuang Jiang, Becky Alexander, Joel Savarino, Joseph Erbland, and Lei Geng
The Cryosphere, 15, 4207–4220, https://doi.org/10.5194/tc-15-4207-2021, https://doi.org/10.5194/tc-15-4207-2021, 2021
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We used a snow photochemistry model (TRANSITS) to simulate the seasonal nitrate snow profile at Summit, Greenland. Comparisons between model outputs and observations suggest that at Summit post-depositional processing is active and probably dominates the snowpack δ15N seasonality. We also used the model to assess the degree of snow nitrate loss and the consequences in its isotopes at present and in the past, which helps for quantitative interpretations of ice-core nitrate records.
Guitao Shi, Hongmei Ma, Zhengyi Hu, Zhenlou Chen, Chunlei An, Su Jiang, Yuansheng Li, Tianming Ma, Jinhai Yu, Danhe Wang, Siyu Lu, Bo Sun, and Meredith G. Hastings
The Cryosphere, 15, 1087–1095, https://doi.org/10.5194/tc-15-1087-2021, https://doi.org/10.5194/tc-15-1087-2021, 2021
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It is important to understand atmospheric chemistry over Antarctica under a changing climate. Thus snow collected on a traverse from the coast to Dome A was used to investigate variations in snow chemistry. The non-sea-salt fractions of K+, Mg2+, and Ca2+ are associated with terrestrial inputs, and nssCl− is from HCl. In general, proportions of non-sea-salt fractions of ions to the totals are higher in the interior areas than on the coast, and the proportions are higher in summer than in winter.
Tingfeng Dou, Zhiheng Du, Shutong Li, Yulan Zhang, Qi Zhang, Mingju Hao, Chuanjin Li, Biao Tian, Minghu Ding, and Cunde Xiao
The Cryosphere, 13, 3309–3316, https://doi.org/10.5194/tc-13-3309-2019, https://doi.org/10.5194/tc-13-3309-2019, 2019
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The meltwater scavenging coefficient (MSC) determines the BC enrichment in the surface layer of melting snow and therefore modulates the BC-snow-albedo feedbacks. This study presents a new method for MSC estimation over the sea-ice area in Arctic. Using this new method, we analyze the spatial variability of MSC in the western Arctic and demonstrate that the value in Canada Basin (23.6 % ± 2.1 %) ≈ that in Greenland (23.0 % ± 12.5 %) > that in Chukchi Sea (17.9 % ± 5.0 %) > that in Elson Lagoon (14.5 % ± 2.6 %).
Xin Wang, Hailun Wei, Jun Liu, Baiqing Xu, Mo Wang, Mingxia Ji, and Hongchun Jin
The Cryosphere, 13, 309–324, https://doi.org/10.5194/tc-13-309-2019, https://doi.org/10.5194/tc-13-309-2019, 2019
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A large survey on measuring optical and chemical properties of insoluble light-absorbing impurities (ILAPs) from seven glaciers was conducted on the Tibetan Plateau (TP) during 2013–2015. The results indicated that the mixing ratios of black carbon (BC), organic carbon (OC), and iron (Fe) all showed a tendency to decrease from north to south, and the industrial pollution (33.1 %), biomass and biofuel burning (29.4 %), and soil dust (37.5 %) were the major sources of the ILAPs on the TP.
Yannick Agnan, Thomas A. Douglas, Detlev Helmig, Jacques Hueber, and Daniel Obrist
The Cryosphere, 12, 1939–1956, https://doi.org/10.5194/tc-12-1939-2018, https://doi.org/10.5194/tc-12-1939-2018, 2018
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In this study, we investigated mercury dynamics in an interior arctic tundra at Toolik Field Station (200 km from the Arctic Ocean) during two full snow seasons. We continuously measured atmospheric, snow gas phase, and soil pores mercury concentrations. We observed consistent concentration declines from the atmosphere to snowpack to soils, indicating that soils are continuous sinks of mercury. We suggest that interior arctic snowpacks may be negligible sources of mercury.
Carmen Paulina Vega, Elisabeth Isaksson, Elisabeth Schlosser, Dmitry Divine, Tõnu Martma, Robert Mulvaney, Anja Eichler, and Margit Schwikowski-Gigar
The Cryosphere, 12, 1681–1697, https://doi.org/10.5194/tc-12-1681-2018, https://doi.org/10.5194/tc-12-1681-2018, 2018
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Ions were measured in firn and ice cores from Fimbul Ice Shelf, Antarctica, to evaluate sea-salt loads. A significant sixfold increase in sea salts was found in the S100 core after 1950s which suggests that it contains a more local sea-salt signal, dominated by processes during sea-ice formation in the neighbouring waters. In contrast, firn cores from three ice rises register the larger-scale signal of atmospheric flow conditions and transport of sea-salt aerosols produced over open water.
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Sofen, E. D., Alexander, B., Steig, E. J., Thiemens, M. H., Kunasek, S. A.,
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Short summary
A record of year-round atmospheric nitrate isotopic composition along with snow nitrate isotopic data from Summit, Greenland, revealed apparent enrichments in nitrogen isotopes in snow nitrate compared to atmospheric nitrate, in addition to a relatively smaller degree of changes in oxygen isotopes. The results suggest that at this site post-depositional processing takes effect, which should be taken into account when interpreting ice-core nitrate isotope records.
A record of year-round atmospheric nitrate isotopic composition along with snow nitrate isotopic...
