Articles | Volume 16, issue 17
https://doi.org/10.5194/amt-16-4015-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-16-4015-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
06 Sep 2023
Research article |
| 06 Sep 2023
| 06 Sep 2023
An extraction method for nitrogen isotope measurement of ammonium in a low-concentration environment
Alexis Lamothe
CORRESPONDING AUTHOR
Univ. Grenoble Alpes, CNRS, IRD, INRAE, Grenoble INP (Institute of Engineering and Management), IGE, 38000 Grenoble, France
Univ. Grenoble Alpes, CNRS, IRD, INRAE, Grenoble INP (Institute of Engineering and Management), IGE, 38000 Grenoble, France
Patrick Ginot
Univ. Grenoble Alpes, CNRS, IRD, INRAE, Grenoble INP (Institute of Engineering and Management), IGE, 38000 Grenoble, France
Lison Soussaintjean
Climate and Environmental Physics, Physics Institute and Oeschger
Centre for Climate Change Research, University of Bern, 3012 Bern,
Switzerland
Elsa Gautier
Univ. Grenoble Alpes, CNRS, IRD, INRAE, Grenoble INP (Institute of Engineering and Management), IGE, 38000 Grenoble, France
Pete D. Akers
Discipline of Geography, School of Natural Sciences, Trinity College Dublin, Dublin, Ireland
Nicolas Caillon
Univ. Grenoble Alpes, CNRS, IRD, INRAE, Grenoble INP (Institute of Engineering and Management), IGE, 38000 Grenoble, France
Joseph Erbland
Univ. Grenoble Alpes, CNRS, IRD, INRAE, Grenoble INP (Institute of Engineering and Management), IGE, 38000 Grenoble, France
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Fairbanks is among the most polluted cities with the highest particulate matter (PM) levels in the US during winters. Highly time-resolved measurements of the sub-micron PM elucidated residential heating with wood and oil and hydrocarbon-like organics from traffic, as well as sulphur-containing organic aerosol, to be the key pollution sources. Remarkable differences existed between complementary instruments, warranting the deployment of multiple tools at sites with wide-ranging influences.
Valeria Mardoñez-Balderrama, Griša Močnik, Marco Pandolfi, Robin L. Modini, Fernando Velarde, Laura Renzi, Angela Marinoni, Jean-Luc Jaffrezo, Isabel Moreno R., Diego Aliaga, Federico Bianchi, Claudia Mohr, Martin Gysel-Beer, Patrick Ginot, Radovan Krejci, Alfred Wiedensohler, Gaëlle Uzu, Marcos Andrade, and Paolo Laj
Atmos. Chem. Phys., 24, 12055–12077, https://doi.org/10.5194/acp-24-12055-2024, https://doi.org/10.5194/acp-24-12055-2024, 2024
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Levels of black carbon (BC) are scarcely reported in the Southern Hemisphere, especially in high-altitude conditions. This study provides insight into the concentration level, variability, and optical properties of BC in La Paz and El Alto and at the Chacaltaya Global Atmosphere Watch Station. Two methods of source apportionment of absorption were tested and compared showing traffic as the main contributor to absorption in the urban area, in addition to biomass and open waste burning.
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.
Zhuang Jiang, Becky Alexander, Joel Savarino, and Lei Geng
Atmos. Chem. Phys., 24, 4895–4914, https://doi.org/10.5194/acp-24-4895-2024, https://doi.org/10.5194/acp-24-4895-2024, 2024
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Ice-core nitrate could track the past atmospheric NOx and oxidant level, but its interpretation is hampered by the post-depositional processing. In this work, an inverse model was developed and tested against two polar sites and was shown to well reproduce the observed nitrate signals in snow and atmosphere, suggesting that the model can properly correct for the effect of post-depositional processing. This model offers a very useful tool for future studies on ice-core nitrate records.
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.
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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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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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Preprint archived
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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.
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.
Zhuang Jiang, Joel Savarino, Becky Alexander, Joseph Erbland, Jean-Luc Jaffrezo, and Lei Geng
The Cryosphere, 16, 2709–2724, https://doi.org/10.5194/tc-16-2709-2022, https://doi.org/10.5194/tc-16-2709-2022, 2022
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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.
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.
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.
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.
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.
Filipe G. L. Lindau, Jefferson C. Simões, Barbara Delmonte, Patrick Ginot, Giovanni Baccolo, Chiara I. Paleari, Elena Di Stefano, Elena Korotkikh, Douglas S. Introne, Valter Maggi, Eduardo Garzanti, and Sergio Andò
The Cryosphere, 15, 1383–1397, https://doi.org/10.5194/tc-15-1383-2021, https://doi.org/10.5194/tc-15-1383-2021, 2021
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Information about the past climate variability in tropical South America is stored in the snow layers of the tropical Andean glaciers. Here we show evidence that the presence of very large aeolian mineral dust particles at Nevado Illimani (Bolivia) is strictly controlled by the occurrence of summer storms in the Bolivian Altiplano. Therefore, based on the snow dust content and its composition of stable water isotopes, we propose a new proxy for information on previous summer storms.
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.
Filipe Gaudie Ley Lindau, Jefferson Cardia Simões, Rafael da Rocha Ribeiro, Patrick Ginot, Barbara Delmonte, Giovanni Baccolo, Stanislav Kutuzov, Valter Maggi, and Edson Ramirez
Clim. Past Discuss., https://doi.org/10.5194/cp-2020-129, https://doi.org/10.5194/cp-2020-129, 2020
Manuscript not accepted for further review
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Glaciers are important freshwater sources in the Tropical Andes. Their retreat has been accelerating since the 1980s. This exposes fresh glacial sediments and facilitates the transport of coarse dust particles to the Nevado Illimani summit. Both the glacial area of Illimani and its ice core record of coarse dust particles respond to warmer conditions across the southern tropical Andes, and drier conditions over the Amazon basin.
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.
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.
Christian Vincent, Adrien Gilbert, Bruno Jourdain, Luc Piard, Patrick Ginot, Vladimir Mikhalenko, Philippe Possenti, Emmanuel Le Meur, Olivier Laarman, and Delphine Six
The Cryosphere, 14, 925–934, https://doi.org/10.5194/tc-14-925-2020, https://doi.org/10.5194/tc-14-925-2020, 2020
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We observed very low glacier thickness changes over the last decades at very-high-elevation glaciated areas on Mont Blanc. Conversely, measurements performed in deep boreholes since 1994 reveal strong changes in englacial temperature reaching 1.5 °C at a depth of 50 m. We conclude that at such very high elevations, current changes in climate do not lead to visible changes in glacier thickness but cause invisible changes within the glacier in terms of englacial temperatures.
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.
Aurélien Chauvigné, Diego Aliaga, Karine Sellegri, Nadège Montoux, Radovan Krejci, Griša Močnik, Isabel Moreno, Thomas Müller, Marco Pandolfi, Fernando Velarde, Kay Weinhold, Patrick Ginot, Alfred Wiedensohler, Marcos Andrade, and Paolo Laj
Atmos. Chem. Phys., 19, 14805–14824, https://doi.org/10.5194/acp-19-14805-2019, https://doi.org/10.5194/acp-19-14805-2019, 2019
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The study presents for the first time the analysis of aerosol optical properties at the unique high-altitude station of Chacaltaya, Bolivia. Ideally located, the station allows us to better understand influences of urban areas and the Amazon Forest on tropospheric properties. An emerging method is applied to characterize aerosol origins and permits us to illustrate evidence of natural and anthropogenic influences.
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.
Hans-Werner Jacobi, Friedrich Obleitner, Sophie Da Costa, Patrick Ginot, Konstantinos Eleftheriadis, Wenche Aas, and Marco Zanatta
Atmos. Chem. Phys., 19, 10361–10377, https://doi.org/10.5194/acp-19-10361-2019, https://doi.org/10.5194/acp-19-10361-2019, 2019
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By combining atmospheric, precipitation, and snow measurements with snowpack simulations for a high Arctic site in Svalbard, we find that during wintertime the transfer of sea salt components to the snowpack was largely dominated by wet deposition. However, dry deposition contributed significantly for nitrate, non-sea-salt sulfate, and black carbon. The comparison of monthly deposition and snow budgets indicates an important redistribution of the impurities in the snowpack even during winter.
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.
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.
Saehee Lim, Xavier Faïn, Patrick Ginot, Vladimir Mikhalenko, Stanislav Kutuzov, Jean-Daniel Paris, Anna Kozachek, and Paolo Laj
Atmos. Chem. Phys., 17, 3489–3505, https://doi.org/10.5194/acp-17-3489-2017, https://doi.org/10.5194/acp-17-3489-2017, 2017
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A record of light-absorbing refractory black carbon (rBC), emitted by fossil fuel combustion and biomass burning, was reconstructed from the ice cores drilled at a high-altitude eastern European site in Mt. Elbrus. This record reports for the first time the high-resolution rBC mass concentrations in the European outflows over the past 189 years. Our study suggests that the past changes in BC emissions of eastern Europe need to be considered in assessing ongoing air quality regulations.
Paolo Gabrielli, Carlo Barbante, Giuliano Bertagna, Michele Bertó, Daniel Binder, Alberto Carton, Luca Carturan, Federico Cazorzi, Giulio Cozzi, Giancarlo Dalla Fontana, Mary Davis, Fabrizio De Blasi, Roberto Dinale, Gianfranco Dragà, Giuliano Dreossi, Daniela Festi, Massimo Frezzotti, Jacopo Gabrieli, Stephan P. Galos, Patrick Ginot, Petra Heidenwolf, Theo M. Jenk, Natalie Kehrwald, Donald Kenny, Olivier Magand, Volkmar Mair, Vladimir Mikhalenko, Ping Nan Lin, Klaus Oeggl, Gianni Piffer, Mirko Rinaldi, Ulrich Schotterer, Margit Schwikowski, Roberto Seppi, Andrea Spolaor, Barbara Stenni, David Tonidandel, Chiara Uglietti, Victor Zagorodnov, Thomas Zanoner, and Piero Zennaro
The Cryosphere, 10, 2779–2797, https://doi.org/10.5194/tc-10-2779-2016, https://doi.org/10.5194/tc-10-2779-2016, 2016
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New ice cores were extracted from Alto dell'Ortles, the highest glacier of South Tyrol in the Italian Alps, to check whether prehistoric ice, which is coeval to the famous 5300-yr-old Tyrolean Iceman, is still preserved in this region. Dating of the ice cores confirms the hypothesis and indicates the drilling site has been glaciated since the end of the Northern Hemisphere Climatic Optimum (7000 yrs BP). We also infer that an unprecedented acceleration of the glacier flow has recently begun.
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.
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.
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 %.
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.
H.-W. Jacobi, S. Lim, M. Ménégoz, P. Ginot, P. Laj, P. Bonasoni, P. Stocchi, A. Marinoni, and Y. Arnaud
The Cryosphere, 9, 1685–1699, https://doi.org/10.5194/tc-9-1685-2015, https://doi.org/10.5194/tc-9-1685-2015, 2015
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We detected up to 70 ppb of black carbon (BC) in surface snow in the upper Khumbu Valley, Nepal. With an upgraded snowpack model, including radiative transfer inside the snow, we studied the impact of BC on snow albedo, melting and radiative forcing for the sensitive high altitude regions of the Himalayas. We found that due to BC, the melting of the snow can be shifted by several days up to several weeks depending on meteorological conditions. The impact of BC is larger in dirty snow.
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.
S. Lim, X. Faïn, M. Zanatta, J. Cozic, J.-L. Jaffrezo, P. Ginot, and P. Laj
Atmos. Meas. Tech., 7, 3307–3324, https://doi.org/10.5194/amt-7-3307-2014, https://doi.org/10.5194/amt-7-3307-2014, 2014
P. Ginot, M. Dumont, S. Lim, N. Patris, J.-D. Taupin, P. Wagnon, A. Gilbert, Y. Arnaud, A. Marinoni, P. Bonasoni, and P. Laj
The Cryosphere, 8, 1479–1496, https://doi.org/10.5194/tc-8-1479-2014, https://doi.org/10.5194/tc-8-1479-2014, 2014
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
M. Ménégoz, G. Krinner, Y. Balkanski, O. Boucher, A. Cozic, S. Lim, P. Ginot, P. Laj, H. Gallée, P. Wagnon, A. Marinoni, and H. W. Jacobi
Atmos. Chem. Phys., 14, 4237–4249, https://doi.org/10.5194/acp-14-4237-2014, https://doi.org/10.5194/acp-14-4237-2014, 2014
Related subject area
Subject: Aerosols | Technique: Laboratory Measurement | Topic: Data Processing and Information Retrieval
Estimating errors in vehicle secondary aerosol production factors due to oxidation flow reactor response time
Quantifying functional group compositions of household fuel-burning emissions
A new software toolkit for optical apportionment of carbonaceous aerosol
Theoretical derivation of aerosol lidar ratio using Mie theory for CALIOP-CALIPSO and OPAC aerosol models
Estimation of secondary organic aerosol formation parameters for the volatility basis set combining thermodenuder, isothermal dilution, and yield measurements
Characterization of offline analysis of particulate matter with FIGAERO-CIMS
Mass spectrometry-based Aerosolomics: a new approach to resolve sources, composition, and partitioning of secondary organic aerosol
A universally applicable method of calculating confidence bands for ice nucleation spectra derived from droplet freezing experiments
Thermal–optical analysis of quartz fiber filters loaded with snow samples – determination of iron based on interferences caused by mineral dust
Modelling ultrafine particle growth in a flow tube reactor
Substantial organic impurities at the surface of synthetic ammonium sulfate particles
Contrasting mineral dust abundances from X-ray diffraction and reflectance spectroscopy
Fragment ion–functional group relationships in organic aerosols using aerosol mass spectrometry and mid-infrared spectroscopy
Evolution under dark conditions of particles from old and modern diesel vehicles in a new environmental chamber characterized with fresh exhaust emissions
Quantification of isomer-resolved iodide chemical ionization mass spectrometry sensitivity and uncertainty using a voltage-scanning approach
Assessing the sources of particles at an urban background site using both regulatory instruments and low-cost sensors – a comparative study
High-resolution optical constants of crystalline ammonium nitrate for infrared remote sensing of the Asian Tropopause Aerosol Layer
Assessing the accuracy of low-cost optical particle sensors using a physics-based approach
Comparison of dimension reduction techniques in the analysis of mass spectrometry data
Development of a new correction algorithm applicable to any filter-based absorption photometer
Chemical discrimination of the particulate and gas phases of miniCAST exhausts using a two-filter collection method
External and internal cloud condensation nuclei (CCN) mixtures: controlled laboratory studies of varying mixing states
Classification of iron oxide aerosols by a single particle soot photometer using supervised machine learning
Method to measure the size-resolved real part of aerosol refractive index using differential mobility analyzer in tandem with single-particle soot photometer
Quantitative capabilities of STXM to measure spatially resolved organic volume fractions of mixed organic ∕ inorganic particles
Revisiting the differential freezing nucleus spectra derived from drop-freezing experiments: methods of calculation, applications, and confidence limits
Particle wall-loss correction methods in smog chamber experiments
Improved real-time bio-aerosol classification using artificial neural networks
Machine learning for improved data analysis of biological aerosol using the WIBS
A machine learning approach to aerosol classification for single-particle mass spectrometry
Evaluation of a hierarchical agglomerative clustering method applied to WIBS laboratory data for improved discrimination of biological particles by comparing data preparation techniques
Using depolarization to quantify ice nucleating particle concentrations: a new method
Real-time analysis of insoluble particles in glacial ice using single-particle mass spectrometry
Evaluation of machine learning algorithms for classification of primary biological aerosol using a new UV-LIF spectrometer
Size distribution of particle-associated polybrominated diphenyl ethers (PBDEs) and their implications for health
Predicting ambient aerosol thermal–optical reflectance (TOR) measurements from infrared spectra: extending the predictions to different years and different sites
Electrodynamic balance measurements of thermodynamic, kinetic, and optical aerosol properties inaccessible to bulk methods
Mass-specific optical absorption coefficients and imaginary part of the complex refractive indices of mineral dust components measured by a multi-wavelength photoacoustic spectrometer
An experiment to measure raindrop collection efficiencies: influence of rear capture
Quantitative single-particle analysis with the Aerodyne aerosol mass spectrometer: development of a new classification algorithm and its application to field data
A modeling approach to evaluate the uncertainty in estimating the evaporation behaviour and volatility of organic aerosols
A model of aerosol evaporation kinetics in a thermodenuder
Pauli Simonen, Miikka Dal Maso, Pinja Prauda, Anniina Hoilijoki, Anette Karppinen, Pekka Matilainen, Panu Karjalainen, and Jorma Keskinen
Atmos. Meas. Tech., 17, 3219–3236, https://doi.org/10.5194/amt-17-3219-2024, https://doi.org/10.5194/amt-17-3219-2024, 2024
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Secondary aerosol is formed in the atmosphere from gaseous emissions. Oxidation flow reactors used in secondary aerosol research do not immediately respond to changes in the inlet concentration of gases because of their broad transfer functions. This may result in incorrect secondary aerosol production factors determined for vehicles. We studied the extent of possible errors and found that oxidation flow reactors with faster responses result in smaller errors.
Emily Y. Li, Amir Yazdani, Ann M. Dillner, Guofeng Shen, Wyatt M. Champion, James J. Jetter, William T. Preston, Lynn M. Russell, Michael D. Hays, and Satoshi Takahama
Atmos. Meas. Tech., 17, 2401–2413, https://doi.org/10.5194/amt-17-2401-2024, https://doi.org/10.5194/amt-17-2401-2024, 2024
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Infrared spectroscopy is a cost-effective measurement technique to characterize the chemical composition of organic aerosol emissions. This technique differentiates the organic matter emission factor from different fuel sources by their characteristic functional groups. Comparison with collocated measurements suggests that polycyclic aromatic hydrocarbon concentrations in emissions estimated by conventional chromatography may be substantially underestimated.
Tommaso Isolabella, Vera Bernardoni, Alessandro Bigi, Marco Brunoldi, Federico Mazzei, Franco Parodi, Paolo Prati, Virginia Vernocchi, and Dario Massabò
Atmos. Meas. Tech., 17, 1363–1373, https://doi.org/10.5194/amt-17-1363-2024, https://doi.org/10.5194/amt-17-1363-2024, 2024
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We present an innovative software toolkit to differentiate sources of carbonaceous aerosol in the atmosphere. Our toolkit implements an upgraded mathematical model which allows for determination of fundamental optical properties of the aerosol, its sources, and the mass concentration of different carbonaceous species of particulate matter. We have tested the functionality of the software by re-analysing published data, and we obtained a compatible results with additional information.
Radhika A. Chipade and Mehul R. Pandya
Atmos. Meas. Tech., 16, 5443–5459, https://doi.org/10.5194/amt-16-5443-2023, https://doi.org/10.5194/amt-16-5443-2023, 2023
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The extinction-to-backscattering ratio, popularly known as lidar ratio of atmospheric aerosols, is an important optical property, which is essential to retrieve the extinction profiles of atmospheric aerosols. A physics-based theoretical approach is presented in the present paper that estimates lidar ratio values for CALIPSO and OPAC aerosol models, which can be used as inputs to determine the extinction profiles of aerosols using CALIPSO data.
Petro Uruci, Dontavious Sippial, Anthoula Drosatou, and Spyros N. Pandis
Atmos. Meas. Tech., 16, 3155–3172, https://doi.org/10.5194/amt-16-3155-2023, https://doi.org/10.5194/amt-16-3155-2023, 2023
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In this work we develop an algorithm for the synthesis of the measurements performed in atmospheric simulation chambers regarding the formation of secondary organic aerosol (SOA). Novel features of the algorithm are its ability to use measurements of SOA yields, thermodenuders, and isothermal dilution; its estimation of parameters that can be used directly in atmospheric chemical transport models; and finally its estimates of the uncertainty in SOA formation yields.
Jing Cai, Kaspar R. Daellenbach, Cheng Wu, Yan Zheng, Feixue Zheng, Wei Du, Sophie L. Haslett, Qi Chen, Markku Kulmala, and Claudia Mohr
Atmos. Meas. Tech., 16, 1147–1165, https://doi.org/10.5194/amt-16-1147-2023, https://doi.org/10.5194/amt-16-1147-2023, 2023
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We introduce the offline application of FIGAERO-CIMS by analyzing Teflon and quartz filter samples that were collected at a typical urban site in Beijing with the deposition time varying from 30 min to 24 h. This method provides a feasible, simple, and quantitative way to investigate the molecular composition and volatility of OA compounds by using FIGAERO-CIMS to analyze offline samples.
Markus Thoma, Franziska Bachmeier, Felix Leonard Gottwald, Mario Simon, and Alexander Lucas Vogel
Atmos. Meas. Tech., 15, 7137–7154, https://doi.org/10.5194/amt-15-7137-2022, https://doi.org/10.5194/amt-15-7137-2022, 2022
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We introduce the aerosolomics database and apply it to particulate matter samples. Nine VOCs were oxidized under various conditions in an oxidation flow reactor, and the formed SOA was measured using liquid chromatography mass spectrometry. With the database, an unambiguous top-down attribution of atmospheric oxidation products to their parent VOCs is now possible. Combining the database with hierarchical clustering enables a better understanding of sources, formation, and partitioning of SOA.
William D. Fahy, Cosma Rohilla Shalizi, and Ryan Christopher Sullivan
Atmos. Meas. Tech., 15, 6819–6836, https://doi.org/10.5194/amt-15-6819-2022, https://doi.org/10.5194/amt-15-6819-2022, 2022
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Heterogeneous ice nucleation (IN) alters cloud microphysics and climate, and droplet freezing assays are widely used to determine a material's IN ability. Existing statistical procedures require restrictive assumptions that may bias reported results, and there is no rigorous way to compare IN spectra. To improve the accuracy of reported IN data, we present a method for calculating statistics and confidence bands and testing statistical differences between IN activities in different materials.
Daniela Kau, Marion Greilinger, Bernadette Kirchsteiger, Aron Göndör, Christopher Herzig, Andreas Limbeck, Elisabeth Eitenberger, and Anne Kasper-Giebl
Atmos. Meas. Tech., 15, 5207–5217, https://doi.org/10.5194/amt-15-5207-2022, https://doi.org/10.5194/amt-15-5207-2022, 2022
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The use of thermal–optical analysis for the determination of elemental carbon (EC) and organic carbon (OC) can be biased by mineral dust (MD). We present a method that utilizes this interference to quantify iron contained in MD in snow samples. Possibilities and limitations of applying this method to particulate matter samples are presented. The influence of light-absorbing iron compounds in MD on the transmittance signal can be used to identify samples experiencing a bias of the OC / EC split.
Michael S. Taylor Jr., Devon N. Higgins, and Murray V. Johnston
Atmos. Meas. Tech., 15, 4663–4674, https://doi.org/10.5194/amt-15-4663-2022, https://doi.org/10.5194/amt-15-4663-2022, 2022
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This modelling study investigates the complex growth kinetics of ultrafine particles in a flow tube reactor. When both surface- and volume-limited growth processes occur, the particle diameter growth rate changes as a function of time in the flow tube. We show that this growth can be represented by a parameter (growth factor, GF) which can be obtained experimentally from the outlet-minus-inlet particle diameter change without foreknowledge of the chemical growth processes involved.
Junteng Wu, Nicolas Brun, Juan Miguel González-Sánchez, Badr R'Mili, Brice Temime Roussel, Sylvain Ravier, Jean-Louis Clément, and Anne Monod
Atmos. Meas. Tech., 15, 3859–3874, https://doi.org/10.5194/amt-15-3859-2022, https://doi.org/10.5194/amt-15-3859-2022, 2022
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This work quantified and tentatively identified the organic impurities on ammonium sulfate aerosols generated in the laboratory. They are likely low volatile and high mass molecules containing oxygen, nitrogen, and/or sulfur. Our results show that these organic impurities likely originate from the commercial AS crystals. It is recommended to use AS seeds with caution, especially when small particles are used, in terms of AS purity and water purity when aqueous solutions are used for atomization.
Mohammad R. Sadrian, Wendy M. Calvin, and John McCormack
Atmos. Meas. Tech., 15, 3053–3074, https://doi.org/10.5194/amt-15-3053-2022, https://doi.org/10.5194/amt-15-3053-2022, 2022
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Mineral dust particles originate from surface soils, primarily in arid regions. They can stay suspended in the atmosphere, impacting Earth's radiation budget. Dust particles will have different perturbation effects depending on their composition. We obtained compositional information on dust collected in an urban setting using two different techniques. We recommended using the combination of measurements to determine the variability in dust mineral abundances.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Meas. Tech., 15, 2857–2874, https://doi.org/10.5194/amt-15-2857-2022, https://doi.org/10.5194/amt-15-2857-2022, 2022
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While the aerosol mass spectrometer provides high-time-resolution characterization of the overall extent of oxidation, the extensive fragmentation of molecules and specificity of the technique have posed challenges toward deeper understanding of molecular structures in aerosols. This work demonstrates how functional group information can be extracted from a suite of commonly measured mass fragments using collocated infrared spectroscopy measurements.
Boris Vansevenant, Cédric Louis, Corinne Ferronato, Ludovic Fine, Patrick Tassel, Pascal Perret, Evangelia Kostenidou, Brice Temime-Roussel, Barbara D'Anna, Karine Sartelet, Véronique Cerezo, and Yao Liu
Atmos. Meas. Tech., 14, 7627–7655, https://doi.org/10.5194/amt-14-7627-2021, https://doi.org/10.5194/amt-14-7627-2021, 2021
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A new method was developed to correct wall losses of particles on Teflon walls using a new environmental chamber. It was applied to experiments with six diesel vehicles (Euro 3 to 6), tested on a chassis dynamometer. Emissions of particles and precursors were obtained under urban and motorway conditions. The chamber experiments help understand the role of physical processes in diesel particle evolutions in the dark. These results can be applied to situations such as tunnels or winter rush hours.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6835–6850, https://doi.org/10.5194/amt-14-6835-2021, https://doi.org/10.5194/amt-14-6835-2021, 2021
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Iodide-adduct chemical ionization mass spectrometry (I-CIMS) has been widely used to analyze airborne organics. In this study, I-CIMS sensitivities of isomers within a formula are found to generally vary by 1 and up to 2 orders of magnitude. Comparisons between measured and predicted moles, obtained using a voltage-scanning calibration approach, show that predictions for individual compounds or formulas might carry high uncertainty, yet the summed moles of analytes agree reasonably well.
Dimitrios Bousiotis, Ajit Singh, Molly Haugen, David C. S. Beddows, Sebastián Diez, Killian L. Murphy, Pete M. Edwards, Adam Boies, Roy M. Harrison, and Francis D. Pope
Atmos. Meas. Tech., 14, 4139–4155, https://doi.org/10.5194/amt-14-4139-2021, https://doi.org/10.5194/amt-14-4139-2021, 2021
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Measurement and source apportionment of atmospheric pollutants are crucial for the assessment of air quality and the implementation of policies for their improvement. This study highlights the current capability of low-cost sensors in source identification and differentiation using clustering approaches. Future directions towards particulate matter source apportionment using low-cost OPCs are highlighted.
Robert Wagner, Baptiste Testa, Michael Höpfner, Alexei Kiselev, Ottmar Möhler, Harald Saathoff, Jörn Ungermann, and Thomas Leisner
Atmos. Meas. Tech., 14, 1977–1991, https://doi.org/10.5194/amt-14-1977-2021, https://doi.org/10.5194/amt-14-1977-2021, 2021
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During the Asian summer monsoon period, air pollutants are transported from layers near the ground to high altitudes of 13 to 18 km in the atmosphere. Infrared measurements have shown that particles composed of solid ammonium nitrate are a major part of these pollutants. To enable the quantitative analysis of the infrared spectra, we have determined for the first time accurate optical constants of ammonium nitrate for the low-temperature conditions of the upper atmosphere.
David H. Hagan and Jesse H. Kroll
Atmos. Meas. Tech., 13, 6343–6355, https://doi.org/10.5194/amt-13-6343-2020, https://doi.org/10.5194/amt-13-6343-2020, 2020
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Assessing the error of low-cost particulate matter (PM) sensors has been difficult as each empirical study presents unique limitations. Here, we present a new, open-sourced, physics-based model (opcsim) and use it to understand how the properties of different particle sensors alter their accuracy. We offer a summary of likely sources of error for different sensor types, environmental conditions, and particle classes and offer recommendations for the choice of optimal calibrant.
Sini Isokääntä, Eetu Kari, Angela Buchholz, Liqing Hao, Siegfried Schobesberger, Annele Virtanen, and Santtu Mikkonen
Atmos. Meas. Tech., 13, 2995–3022, https://doi.org/10.5194/amt-13-2995-2020, https://doi.org/10.5194/amt-13-2995-2020, 2020
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Online mass spectrometry produces large amounts of data. These data can be interpreted with statistical methods, enabling scientists to more easily understand the underlying processes. We compared these techniques on car exhaust measurements. We show differences and similarities between the methods and give recommendations on applicability of the methods on certain types of data. We show that applying multiple methods leads to more robust results, thus increasing reliability of the findings.
Hanyang Li, Gavin R. McMeeking, and Andrew A. May
Atmos. Meas. Tech., 13, 2865–2886, https://doi.org/10.5194/amt-13-2865-2020, https://doi.org/10.5194/amt-13-2865-2020, 2020
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We present a new correction algorithm that addresses biases in measurements of aerosol light absorption by filter-based photometers, incorporating the transmission of light through the filter and some aerosol optical properties. It was developed using biomass burning aerosols and tested using rural ambient aerosols. This new algorithm is applicable to any filter-based photometer, resulting in good agreement between different colocated instruments in both the laboratory and the field.
Linh Dan Ngo, Dumitru Duca, Yvain Carpentier, Jennifer A. Noble, Raouf Ikhenazene, Marin Vojkovic, Cornelia Irimiea, Ismael K. Ortega, Guillaume Lefevre, Jérôme Yon, Alessandro Faccinetto, Eric Therssen, Michael Ziskind, Bertrand Chazallon, Claire Pirim, and Cristian Focsa
Atmos. Meas. Tech., 13, 951–967, https://doi.org/10.5194/amt-13-951-2020, https://doi.org/10.5194/amt-13-951-2020, 2020
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The partitioning of noxious chemical compounds between the particulate and gas phases in combustion emissions is key to delineate their exact impacts on atmospheric chemistry and human health. We developed a two-filter sampling system, a multi-technique analytical approach, and advanced statistical methods to fully characterize the composition of both phases in combustion emissions. We could successfully discriminate samples from a standard soot generator by their volatile–non-volatile species.
Diep Vu, Shaokai Gao, Tyler Berte, Mary Kacarab, Qi Yao, Kambiz Vafai, and Akua Asa-Awuku
Atmos. Meas. Tech., 12, 4277–4289, https://doi.org/10.5194/amt-12-4277-2019, https://doi.org/10.5194/amt-12-4277-2019, 2019
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Aerosol–cloud interactions contribute the greatest uncertainty to cloud formation. Aerosol composition is complex and can change quickly in the atmosphere. In this work, we recreate a transition in aerosol mixing state in the laboratory, which (to date) has only been observed in the ambient state. We then report the subsequent changes on cloud condensation nuclei (CCN) activation.
Kara D. Lamb
Atmos. Meas. Tech., 12, 3885–3906, https://doi.org/10.5194/amt-12-3885-2019, https://doi.org/10.5194/amt-12-3885-2019, 2019
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Recent atmospheric observations have indicated emissions of iron-oxide-containing aerosols from anthropogenic sources could be 8x higher than previous estimates, leading models to underestimate their climate impact. Previous studies have shown the single particle soot photometer (SP2) can quantify the atmospheric abundance of these aerosols. Here, I explore a machine learning approach to improve SP2 detection, significantly reducing misclassifications of other aerosols as iron oxide aerosols.
Gang Zhao, Weilun Zhao, and Chunsheng Zhao
Atmos. Meas. Tech., 12, 3541–3550, https://doi.org/10.5194/amt-12-3541-2019, https://doi.org/10.5194/amt-12-3541-2019, 2019
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A new method is proposed to retrieve the size-resolved real part of the refractive index (RRI). The main principle of deriving the RRI is measuring the scattering intensity by a single-particle soot photometer of a size-selected aerosol. This method is validated by a series of calibration experiments using the components of the known RI. The retrieved size-resolved RRI covers a wide range, from 200 nm to 450 nm, with uncertainty of less than 0.02.
Matthew Fraund, Tim Park, Lin Yao, Daniel Bonanno, Don Q. Pham, and Ryan C. Moffet
Atmos. Meas. Tech., 12, 1619–1633, https://doi.org/10.5194/amt-12-1619-2019, https://doi.org/10.5194/amt-12-1619-2019, 2019
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Scanning transmission X-ray microscopy (STXM) is a powerful tool which is able to determine the elemental and functional composition of aerosols on a subparticle level. The current work validates the use of STXM for quantitatively calculating the organic volume fraction of individual aerosols by applying the calculation to lab-prepared samples. The caveats and limitations for this calculation are shown as well.
Gabor Vali
Atmos. Meas. Tech., 12, 1219–1231, https://doi.org/10.5194/amt-12-1219-2019, https://doi.org/10.5194/amt-12-1219-2019, 2019
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The abundance of freezing nuclei in water samples is routinely determined by experiments involving the cooling of sample drops and observing the temperatures at which the drops freeze. This is used for characterizing the nucleating abilities of materials in laboratory preparations or to determine the numbers of nucleating particles in rain, snow, river water or other natural waters. The evaluation of drop-freezing experiments in terms of differential nucleus spectra is advocated in the paper.
Ningxin Wang, Spiro D. Jorga, Jeffery R. Pierce, Neil M. Donahue, and Spyros N. Pandis
Atmos. Meas. Tech., 11, 6577–6588, https://doi.org/10.5194/amt-11-6577-2018, https://doi.org/10.5194/amt-11-6577-2018, 2018
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The interaction of particles with the chamber walls has been a significant source of uncertainty when analyzing results of secondary organic aerosol formation experiments performed in Teflon chambers. We evaluated the performance of several particle wall-loss correction methods for aging experiments of α-pinene ozonolysis products. Experimental procedures are proposed for the characterization of particle losses during different stages of these experiments.
Maciej Leśkiewicz, Miron Kaliszewski, Maksymilian Włodarski, Jarosław Młyńczak, Zygmunt Mierczyk, and Krzysztof Kopczyński
Atmos. Meas. Tech., 11, 6259–6270, https://doi.org/10.5194/amt-11-6259-2018, https://doi.org/10.5194/amt-11-6259-2018, 2018
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In this study we demonstrate the application of artificial neural networks to the real-time analysis of single-particle fluorescence fingerprints acquired using BARDet (a BioAeRosol Detector). 48 different aerosols including pollens, bacteria, fungi, spores and nonbiological substances were characterized. An entirely new approach to data analysis using a decision tree comprising 22 independent neural networks was discussed. A very high accuracy of aerosol classification in real time resulted.
Simon Ruske, David O. Topping, Virginia E. Foot, Andrew P. Morse, and Martin W. Gallagher
Atmos. Meas. Tech., 11, 6203–6230, https://doi.org/10.5194/amt-11-6203-2018, https://doi.org/10.5194/amt-11-6203-2018, 2018
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Pollen, bacteria and fungal spores are common in the environment, can have very important implications for public health and may influence the weather. Biological sensors potentially could be used to monitor quantities of these types of particles. However, it is important to transform the measurements from these instruments into counts of these biological particles. The paper tests a variety of approaches for achieving this aim on data collected in a laboratory.
Costa D. Christopoulos, Sarvesh Garimella, Maria A. Zawadowicz, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Meas. Tech., 11, 5687–5699, https://doi.org/10.5194/amt-11-5687-2018, https://doi.org/10.5194/amt-11-5687-2018, 2018
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Compositional analysis of atmospheric and laboratory aerosols is often conducted with mass spectrometry. In this study, machine learning is used to automatically differentiate particles on the basis of chemistry and size. The ability of the machine learning algorithm was then tested on a data set for which the particles were not initially known to judge its ability.
Nicole J. Savage and J. Alex Huffman
Atmos. Meas. Tech., 11, 4929–4942, https://doi.org/10.5194/amt-11-4929-2018, https://doi.org/10.5194/amt-11-4929-2018, 2018
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We show the systematic application of hierarchical agglomerative clustering (HAC) to comprehensive bioaerosol and non-bioaerosol laboratory data collected with the wideband integrated bioaerosol sensor (WIBS-4A). This study investigated various input conditions and used individual matchups and computational mixtures of particles; it will help improve clustering results applied to data from the ultraviolet laser and light-induced fluorescence instruments commonly used for bioaerosol research.
Jake Zenker, Kristen N. Collier, Guanglang Xu, Ping Yang, Ezra J. T. Levin, Kaitlyn J. Suski, Paul J. DeMott, and Sarah D. Brooks
Atmos. Meas. Tech., 10, 4639–4657, https://doi.org/10.5194/amt-10-4639-2017, https://doi.org/10.5194/amt-10-4639-2017, 2017
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We have developed a new method which employs single particle depolarization to determine ice nucleating particle (INP) concentrations and to differentiate between ice crystals, water droplets, and aerosols. The method is used to interpret measurements collected using the Texas A&M Continuous Flow Diffusion Chamber (TAMU CFDC) coupled to a Cloud and Aerosol Spectrometer with Polarization (CASPOL). This new method extends the range of operating conditions for the CFDC to higher supersaturations.
Matthew Osman, Maria A. Zawadowicz, Sarah B. Das, and Daniel J. Cziczo
Atmos. Meas. Tech., 10, 4459–4477, https://doi.org/10.5194/amt-10-4459-2017, https://doi.org/10.5194/amt-10-4459-2017, 2017
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This study presents the first-time attempt at using time-of-flight single particle mass spectrometry (SPMS) as an emerging online technique for measuring insoluble particles in glacial snow and ice. Using samples from two Greenlandic ice cores, we show that SPMS can constrain the aerodynamic size, composition, and relative abundance of most particulate types on a per-particle basis, reducing the preparation time and resources required of conventional, filter-based particle retrieval methods.
Simon Ruske, David O. Topping, Virginia E. Foot, Paul H. Kaye, Warren R. Stanley, Ian Crawford, Andrew P. Morse, and Martin W. Gallagher
Atmos. Meas. Tech., 10, 695–708, https://doi.org/10.5194/amt-10-695-2017, https://doi.org/10.5194/amt-10-695-2017, 2017
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Particles such as bacteria, pollen and fungal spores have important implications within the environment and public health sectors. Here we evaluate the performance of various different methods for distinguishing between these different types of particles using a new instrument. We demonstrate that there may be better alternatives to the currently used methods which can be further investigated in future research.
Yan Lyu, Tingting Xu, Xiang Li, Tiantao Cheng, Xin Yang, Xiaomin Sun, and Jianmin Chen
Atmos. Meas. Tech., 9, 1025–1037, https://doi.org/10.5194/amt-9-1025-2016, https://doi.org/10.5194/amt-9-1025-2016, 2016
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This study presents the particle size distribution of PBDEs in the atmosphere of a megacity and evaluates the contribution of size-fractionated PBDEs' deposition in the human respiratory tract.
Matteo Reggente, Ann M. Dillner, and Satoshi Takahama
Atmos. Meas. Tech., 9, 441–454, https://doi.org/10.5194/amt-9-441-2016, https://doi.org/10.5194/amt-9-441-2016, 2016
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Organic carbon and elemental carbon are major components of atmospheric PM. Typically they are measured using destructive and relatively expensive methods (e.g., TOR). We aim to reduce the operating costs of large air quality monitoring networks using FT-IR spectra of ambient PTFE filters and PLS regression. We achieve accurate predictions for models (calibrated in 2011) that use samples collected at the same or different sites of the calibration data set and in a different year (2013).
S. S. Steimer, U. K. Krieger, Y.-F. Te, D. M. Lienhard, A. J. Huisman, B. P. Luo, M. Ammann, and T. Peter
Atmos. Meas. Tech., 8, 2397–2408, https://doi.org/10.5194/amt-8-2397-2015, https://doi.org/10.5194/amt-8-2397-2015, 2015
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Atmospheric aerosol is often subject to supersaturated or supercooled conditions where bulk measurements are not possible. Here we demonstrate how measurements using single particle electrodynamic levitation combined with light scattering spectroscopy allow the retrieval of thermodynamic data, optical properties and water diffusivity of such metastable particles even when auxiliary bulk data are not available due to lack of sufficient amounts of sample.
N. Utry, T. Ajtai, M. Pintér, E. Tombácz, E. Illés, Z. Bozóki, and G. Szabó
Atmos. Meas. Tech., 8, 401–410, https://doi.org/10.5194/amt-8-401-2015, https://doi.org/10.5194/amt-8-401-2015, 2015
A. Quérel, P. Lemaitre, M. Monier, E. Porcheron, A. I. Flossmann, and M. Hervo
Atmos. Meas. Tech., 7, 1321–1330, https://doi.org/10.5194/amt-7-1321-2014, https://doi.org/10.5194/amt-7-1321-2014, 2014
F. Freutel, F. Drewnick, J. Schneider, T. Klimach, and S. Borrmann
Atmos. Meas. Tech., 6, 3131–3145, https://doi.org/10.5194/amt-6-3131-2013, https://doi.org/10.5194/amt-6-3131-2013, 2013
E. Fuentes and G. McFiggans
Atmos. Meas. Tech., 5, 735–757, https://doi.org/10.5194/amt-5-735-2012, https://doi.org/10.5194/amt-5-735-2012, 2012
C. D. Cappa
Atmos. Meas. Tech., 3, 579–592, https://doi.org/10.5194/amt-3-579-2010, https://doi.org/10.5194/amt-3-579-2010, 2010
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Short summary
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.
Ammonia is a reactive gas in our atmosphere that is key in air quality issues. Assessing its...
