Articles | Volume 18, issue 21
https://doi.org/10.5194/acp-18-15825-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-18-15825-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Understanding mercury oxidation and air–snow exchange on the East Antarctic Plateau: a modeling study
Department of Earth, Atmospheric and Planetary Sciences, Massachusetts
Institute of Technology, Cambridge, MA, USA
now at: School of Engineering and Applied Sciences, Harvard
University, Cambridge, MA, USA
Hélène Angot
Institute for Data, Systems and Society, Massachusetts Institute of
Technology, Cambridge, MA, USA
Noelle E. Selin
Department of Earth, Atmospheric and Planetary Sciences, Massachusetts
Institute of Technology, Cambridge, MA, USA
Institute for Data, Systems and Society, Massachusetts Institute of
Technology, Cambridge, MA, USA
Hubert Gallée
Univ. Grenoble Alpes, CNRS, IRD, Grenoble INP, Institut des
Géosciences de l'Environnement (IGE), Grenoble, France
Francesca Sprovieri
CNR-Institute of Atmospheric Pollution Research, Rende,
Italy
Nicola Pirrone
CNR-Institute of Atmospheric Pollution Research, Montelibretti, Rome,
Italy
Detlev Helmig
Institute of Arctic and Alpine Research (INSTAAR), University of
Colorado, Boulder, CO, USA
Joël Savarino
Univ. Grenoble Alpes, CNRS, IRD, Grenoble INP, Institut des
Géosciences de l'Environnement (IGE), Grenoble, France
Olivier Magand
Univ. Grenoble Alpes, CNRS, IRD, Grenoble INP, Institut des
Géosciences de l'Environnement (IGE), Grenoble, France
Aurélien Dommergue
Univ. Grenoble Alpes, CNRS, IRD, Grenoble INP, Institut des
Géosciences de l'Environnement (IGE), Grenoble, France
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This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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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
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Brandon Bottorff, Michelle M. Lew, Youngjun Woo, Pamela Rickly, Matthew D. Rollings, Benjamin Deming, Daniel C. Anderson, Ezra Wood, Hariprasad D. Alwe, Dylan B. Millet, Andrew Weinheimer, Geoff Tyndall, John Ortega, Sebastien Dusanter, Thierry Leonardis, James Flynn, Matt Erickson, Sergio Alvarez, Jean C. Rivera-Rios, Joshua D. Shutter, Frank Keutsch, Detlev Helmig, Wei Wang, Hannah M. Allen, Steven Bertman, and Philip S. Stevens
EGUsphere, https://doi.org/10.5194/egusphere-2023-790, https://doi.org/10.5194/egusphere-2023-790, 2023
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Inès N. Otosaka, Andrew Shepherd, Erik R. Ivins, Nicole-Jeanne Schlegel, Charles Amory, Michiel R. van den Broeke, Martin Horwath, Ian Joughin, Michalea D. King, Gerhard Krinner, Sophie Nowicki, Anthony J. Payne, Eric Rignot, Ted Scambos, Karen M. Simon, Benjamin E. Smith, Louise S. Sørensen, Isabella Velicogna, Pippa L. Whitehouse, Geruo A, Cécile Agosta, Andreas P. Ahlstrøm, Alejandro Blazquez, William Colgan, Marcus E. Engdahl, Xavier Fettweis, Rene Forsberg, Hubert Gallée, Alex Gardner, Lin Gilbert, Noel Gourmelen, Andreas Groh, Brian C. Gunter, Christopher Harig, Veit Helm, Shfaqat Abbas Khan, Christoph Kittel, Hannes Konrad, Peter L. Langen, Benoit S. Lecavalier, Chia-Chun Liang, Bryant D. Loomis, Malcolm McMillan, Daniele Melini, Sebastian H. Mernild, Ruth Mottram, Jeremie Mouginot, Johan Nilsson, Brice Noël, Mark E. Pattle, William R. Peltier, Nadege Pie, Mònica Roca, Ingo Sasgen, Himanshu V. Save, Ki-Weon Seo, Bernd Scheuchl, Ernst J. O. Schrama, Ludwig Schröder, Sebastian B. Simonsen, Thomas Slater, Giorgio Spada, Tyler C. Sutterley, Bramha Dutt Vishwakarma, Jan Melchior van Wessem, David Wiese, Wouter van der Wal, and Bert Wouters
Earth Syst. Sci. Data, 15, 1597–1616, https://doi.org/10.5194/essd-15-1597-2023, https://doi.org/10.5194/essd-15-1597-2023, 2023
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Alkuin M. Koenig, Olivier Magand, Bert Verreyken, Jerome Brioude, Crist Amelynck, Niels Schoon, Aurélie Colomb, Beatriz Ferreira Araujo, Michel Ramonet, Mahesh K. Sha, Jean-Pierre Cammas, Jeroen E. Sonke, and Aurélien Dommergue
Atmos. Chem. Phys., 23, 1309–1328, https://doi.org/10.5194/acp-23-1309-2023, https://doi.org/10.5194/acp-23-1309-2023, 2023
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Matthew Boyer, Diego Aliaga, Jakob Boyd Pernov, Hélène Angot, Lauriane L. J. Quéléver, Lubna Dada, Benjamin Heutte, Manuel Dall'Osto, David C. S. Beddows, Zoé Brasseur, Ivo Beck, Silvia Bucci, Marina Duetsch, Andreas Stohl, Tiia Laurila, Eija Asmi, Andreas Massling, Daniel Charles Thomas, Jakob Klenø Nøjgaard, Tak Chan, Sangeeta Sharma, Peter Tunved, Radovan Krejci, Hans Christen Hansson, Federico Bianchi, Katrianne Lehtipalo, Alfred Wiedensohler, Kay Weinhold, Markku Kulmala, Tuukka Petäjä, Mikko Sipilä, Julia Schmale, and Tuija Jokinen
Atmos. Chem. Phys., 23, 389–415, https://doi.org/10.5194/acp-23-389-2023, https://doi.org/10.5194/acp-23-389-2023, 2023
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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.
Vanessa Selimovic, Damien Ketcherside, Sreelekha Chaliyakunnel, Catherine Wielgasz, Wade Permar, Hélène Angot, Dylan B. Millet, Alan Fried, Detlev Helmig, and Lu Hu
Atmos. Chem. Phys., 22, 14037–14058, https://doi.org/10.5194/acp-22-14037-2022, https://doi.org/10.5194/acp-22-14037-2022, 2022
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Arctic warming has led to an increase in plants that emit gases in response to stress, but how these gases affect regional chemistry is largely unknown due to lack of observational data. Here we present the most comprehensive gas-phase measurements for this area to date and compare them to predictions from a global transport model. We report 78 gas-phase species and investigate their importance to atmospheric chemistry in the area, with broader implications for similar plant types.
William Atkinson, Sebastian D. Eastham, Y.-H. Henry Chen, Jennifer Morris, Sergey Paltsev, C. Adam Schlosser, and Noelle E. Selin
Geosci. Model Dev., 15, 7767–7789, https://doi.org/10.5194/gmd-15-7767-2022, https://doi.org/10.5194/gmd-15-7767-2022, 2022
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Understanding policy effects on human-caused air pollutant emissions is key for assessing related health impacts. We develop a flexible scenario tool that combines updated emissions data sets, long-term economic modeling, and comprehensive technology pathways to clarify the impacts of climate and air quality policies. Results show the importance of both policy levers in the future to prevent long-term emission increases from offsetting near-term air quality improvements from existing policies.
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.
Detlev Helmig, Alex Guenther, Jacques Hueber, Ryan Daly, Wei Wang, Jeong-Hoo Park, Anssi Liikanen, and Arnaud P. Praplan
Atmos. Meas. Tech., 15, 5439–5454, https://doi.org/10.5194/amt-15-5439-2022, https://doi.org/10.5194/amt-15-5439-2022, 2022
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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.
Minghao Qiu, Corwin Zigler, and Noelle E. Selin
Atmos. Chem. Phys., 22, 10551–10566, https://doi.org/10.5194/acp-22-10551-2022, https://doi.org/10.5194/acp-22-10551-2022, 2022
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Evaluating impacts of emission changes on air quality requires accounting for meteorological variability. Many studies use simple regression methods to correct for meteorology, but little is known about their performance. Using cases in the US and China, we show that widely used regression models do not perform well and can lead to biased estimates of emission-driven trends. We propose a novel machine learning method with lower bias and provide recommendations to policymakers and researchers.
Ivo Beck, Hélène Angot, Andrea Baccarini, Lubna Dada, Lauriane Quéléver, Tuija Jokinen, Tiia Laurila, Markus Lampimäki, Nicolas Bukowiecki, Matthew Boyer, Xianda Gong, Martin Gysel-Beer, Tuukka Petäjä, Jian Wang, and Julia Schmale
Atmos. Meas. Tech., 15, 4195–4224, https://doi.org/10.5194/amt-15-4195-2022, https://doi.org/10.5194/amt-15-4195-2022, 2022
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We present the pollution detection algorithm (PDA), a new method to identify local primary pollution in remote atmospheric aerosol and trace gas time series. The PDA identifies periods of contaminated data and relies only on the target dataset itself; i.e., it is independent of ancillary data such as meteorological variables. The parameters of all pollution identification steps are adjustable so that the PDA can be tuned to different locations and situations. It is available as open-access code.
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.
Christoph Kittel, Charles Amory, Stefan Hofer, Cécile Agosta, Nicolas C. Jourdain, Ella Gilbert, Louis Le Toumelin, Étienne Vignon, Hubert Gallée, and Xavier Fettweis
The Cryosphere, 16, 2655–2669, https://doi.org/10.5194/tc-16-2655-2022, https://doi.org/10.5194/tc-16-2655-2022, 2022
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Model projections suggest large differences in future Antarctic surface melting even for similar greenhouse gas scenarios and warming rates. We show that clouds containing a larger amount of liquid water lead to stronger melt. As surface melt can trigger the collapse of the ice shelves (the safety band of the Antarctic Ice Sheet), clouds could be a major source of uncertainties in projections of sea level rise.
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.
Sara Bacer, Fatima Jomaa, Julien Beaumet, Hubert Gallée, Enzo Le Bouëdec, Martin Ménégoz, and Chantal Staquet
Weather Clim. Dynam., 3, 377–389, https://doi.org/10.5194/wcd-3-377-2022, https://doi.org/10.5194/wcd-3-377-2022, 2022
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We study the impact of climate change on wintertime atmospheric blocking over Europe. We focus on the frequency, duration, and size of blocking events. The blocking events are identified via the weather type decomposition methodology. We find that blocking frequency, duration, and size are mostly stationary over the 21st century. Additionally, we compare the blocking size results with the size of the blocking events identified via a different approach using a blocking index.
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.
Hélène Angot, Connor Davel, Christine Wiedinmyer, Gabrielle Pétron, Jashan Chopra, Jacques Hueber, Brendan Blanchard, Ilann Bourgeois, Isaac Vimont, Stephen A. Montzka, Ben R. Miller, James W. Elkins, and Detlev Helmig
Atmos. Chem. Phys., 21, 15153–15170, https://doi.org/10.5194/acp-21-15153-2021, https://doi.org/10.5194/acp-21-15153-2021, 2021
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After a multidecadal global decline in atmospheric abundance of ethane and propane (precursors of tropospheric ozone and aerosols), previous work showed a reversal of this trend in 2009–2015 in the Northern Hemisphere due to the growth in oil and natural gas production in North America. Here we show a temporary pause in the growth of atmospheric ethane and propane in 2015–2018 and highlight the critical need for additional top-down studies to further constrain ethane and propane emissions.
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.
Louis Le Toumelin, Charles Amory, Vincent Favier, Christoph Kittel, Stefan Hofer, Xavier Fettweis, Hubert Gallée, and Vinay Kayetha
The Cryosphere, 15, 3595–3614, https://doi.org/10.5194/tc-15-3595-2021, https://doi.org/10.5194/tc-15-3595-2021, 2021
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Snow is frequently eroded from the surface by the wind in Adelie Land (Antarctica) and suspended in the lower atmosphere. By performing model simulations, we show firstly that suspended snow layers interact with incoming radiation similarly to a near-surface cloud. Secondly, suspended snow modifies the atmosphere's thermodynamic structure and energy exchanges with the surface. Our results suggest snow transport by the wind should be taken into account in future model studies over the region.
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.
Attilio Naccarato, Antonella Tassone, Maria Martino, Sacha Moretti, Antonella Macagnano, Emiliano Zampetti, Paolo Papa, Joshua Avossa, Nicola Pirrone, Michelle Nerentorp, John Munthe, Ingvar Wängberg, Geoff W. Stupple, Carl P. J. Mitchell, Adam R. Martin, Alexandra Steffen, Diana Babi, Eric M. Prestbo, Francesca Sprovieri, and Frank Wania
Atmos. Meas. Tech., 14, 3657–3672, https://doi.org/10.5194/amt-14-3657-2021, https://doi.org/10.5194/amt-14-3657-2021, 2021
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Mercury monitoring in support of the Minamata Convention requires effective and reliable analytical tools. Passive sampling is a promising approach for creating a sustainable long-term network for atmospheric mercury with improved spatial resolution and global coverage. In this study the analytical performance of three passive air samplers (CNR-PAS, IVL-PAS, and MerPAS) was assessed over extended deployment periods and the accuracy of concentrations was judged by comparison with active sampling.
Athanasios Nenes, Spyros N. Pandis, Maria Kanakidou, Armistead G. Russell, Shaojie Song, Petros Vasilakos, and Rodney J. Weber
Atmos. Chem. Phys., 21, 6023–6033, https://doi.org/10.5194/acp-21-6023-2021, https://doi.org/10.5194/acp-21-6023-2021, 2021
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Ecosystems and air quality are affected by the dry deposition of inorganic reactive nitrogen (Nr, the sum of ammonium and nitrate). Its large variability is driven by the large difference in deposition velocity of N when in the gas or particle phase. Here we show that aerosol liquid water and acidity, by affecting gas–particle partitioning, modulate the dry deposition velocity of NH3, HNO3, and Nr worldwide. These effects explain the rapid accumulation of nitrate aerosol during haze events.
Peter Sherman, Meng Gao, Shaojie Song, Alex T. Archibald, Nathan Luke Abraham, Jean-François Lamarque, Drew Shindell, Gregory Faluvegi, and Michael B. McElroy
Atmos. Chem. Phys., 21, 3593–3605, https://doi.org/10.5194/acp-21-3593-2021, https://doi.org/10.5194/acp-21-3593-2021, 2021
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The aims here are to assess the role of aerosols in India's monsoon precipitation and to determine the relative contributions from Chinese and Indian emissions using CMIP6 models. We find that increased sulfur emissions reduce precipitation, which is primarily dynamically driven due to spatial shifts in convection over the region. A significant increase in precipitation (up to ~ 20 %) is found only when both Indian and Chinese sulfate emissions are regulated.
Alkuin Maximilian Koenig, Olivier Magand, Paolo Laj, Marcos Andrade, Isabel Moreno, Fernando Velarde, Grover Salvatierra, René Gutierrez, Luis Blacutt, Diego Aliaga, Thomas Reichler, Karine Sellegri, Olivier Laurent, Michel Ramonet, and Aurélien Dommergue
Atmos. Chem. Phys., 21, 3447–3472, https://doi.org/10.5194/acp-21-3447-2021, https://doi.org/10.5194/acp-21-3447-2021, 2021
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The environmental cycling of atmospheric mercury, a harmful global contaminant, is still not sufficiently constrained, partly due to missing data in remote regions. Here, we address this issue by presenting 20 months of atmospheric mercury measurements, sampled in the Bolivian Andes. We observe a significant seasonal pattern, whose key features we explore. Moreover, we deduce ratios to constrain South American biomass burning mercury emissions and the mercury uptake by the Amazon rainforest.
Marion Donat-Magnin, Nicolas C. Jourdain, Christoph Kittel, Cécile Agosta, Charles Amory, Hubert Gallée, Gerhard Krinner, and Mondher Chekki
The Cryosphere, 15, 571–593, https://doi.org/10.5194/tc-15-571-2021, https://doi.org/10.5194/tc-15-571-2021, 2021
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We simulate the West Antarctic climate in 2100 under increasing greenhouse gases. Future accumulation over the ice sheet increases, which reduces sea level changing rate. Surface ice-shelf melt rates increase until 2100. Some ice shelves experience a lot of liquid water at their surface, which indicates potential ice-shelf collapse. In contrast, no liquid water is found over other ice shelves due to huge amounts of snowfall that bury liquid water, favouring refreezing and ice-shelf stability.
Shaojie Song, Tao Ma, Yuzhong Zhang, Lu Shen, Pengfei Liu, Ke Li, Shixian Zhai, Haotian Zheng, Meng Gao, Jonathan M. Moch, Fengkui Duan, Kebin He, and Michael B. McElroy
Atmos. Chem. Phys., 21, 457–481, https://doi.org/10.5194/acp-21-457-2021, https://doi.org/10.5194/acp-21-457-2021, 2021
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We simulate the atmospheric chemical processes of an important sulfur-containing organic aerosol species, which is produced by the reaction between sulfur dioxide and formaldehyde. We can predict its distribution on a global scale. We find it is particularly rich in East Asia. This aerosol species is more abundant in the colder season partly because of weaker sunlight.
Hélène Angot, Katelyn McErlean, Lu Hu, Dylan B. Millet, Jacques Hueber, Kaixin Cui, Jacob Moss, Catherine Wielgasz, Tyler Milligan, Damien Ketcherside, M. Syndonia Bret-Harte, and Detlev Helmig
Biogeosciences, 17, 6219–6236, https://doi.org/10.5194/bg-17-6219-2020, https://doi.org/10.5194/bg-17-6219-2020, 2020
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We report biogenic volatile organic compounds (BVOCs) ambient levels and emission rates from key vegetation species in the Alaskan arctic tundra, providing a new data set to further constrain isoprene chemistry under low NOx conditions in models. We add to the growing body of evidence that climate-induced changes in the vegetation composition will significantly affect the BVOC emission potential of the tundra, with implications for atmospheric oxidation processes and climate feedbacks.
Romie Tignat-Perrier, Aurélien Dommergue, Alban Thollot, Olivier Magand, Timothy M. Vogel, and Catherine Larose
Biogeosciences, 17, 6081–6095, https://doi.org/10.5194/bg-17-6081-2020, https://doi.org/10.5194/bg-17-6081-2020, 2020
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The adverse atmospheric environmental conditions do not appear suited for microbial life. We conducted the first global comparative metagenomic analysis to find out if airborne microbial communities might be selected by their ability to resist these adverse conditions. The relatively higher concentration of fungi led to the observation of higher proportions of stress-related functions in air. Fungi might likely resist and survive atmospheric physical stress better than bacteria.
Jingsha Xu, Shaojie Song, Roy M. Harrison, Congbo Song, Lianfang Wei, Qiang Zhang, Yele Sun, Lu Lei, Chao Zhang, Xiaohong Yao, Dihui Chen, Weijun Li, Miaomiao Wu, Hezhong Tian, Lining Luo, Shengrui Tong, Weiran Li, Junling Wang, Guoliang Shi, Yanqi Huangfu, Yingze Tian, Baozhu Ge, Shaoli Su, Chao Peng, Yang Chen, Fumo Yang, Aleksandra Mihajlidi-Zelić, Dragana Đorđević, Stefan J. Swift, Imogen Andrews, Jacqueline F. Hamilton, Ye Sun, Agung Kramawijaya, Jinxiu Han, Supattarachai Saksakulkrai, Clarissa Baldo, Siqi Hou, Feixue Zheng, Kaspar R. Daellenbach, Chao Yan, Yongchun Liu, Markku Kulmala, Pingqing Fu, and Zongbo Shi
Atmos. Meas. Tech., 13, 6325–6341, https://doi.org/10.5194/amt-13-6325-2020, https://doi.org/10.5194/amt-13-6325-2020, 2020
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An interlaboratory comparison was conducted for the first time to examine differences in water-soluble inorganic ions (WSIIs) measured by 10 labs using ion chromatography (IC) and by two online aerosol chemical speciation monitor (ACSM) methods. Major ions including SO42−, NO3− and NH4+ agreed well in 10 IC labs and correlated well with ACSM data. WSII interlab variability strongly affected aerosol acidity results based on ion balance, but aerosol pH computed by ISORROPIA II was very similar.
Martin Ménégoz, Evgenia Valla, Nicolas C. Jourdain, Juliette Blanchet, Julien Beaumet, Bruno Wilhelm, Hubert Gallée, Xavier Fettweis, Samuel Morin, and Sandrine Anquetin
Hydrol. Earth Syst. Sci., 24, 5355–5377, https://doi.org/10.5194/hess-24-5355-2020, https://doi.org/10.5194/hess-24-5355-2020, 2020
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The study investigates precipitation changes in the Alps, using observations and a 7 km resolution climate simulation over 1900–2010. An increase in mean precipitation is found in winter over the Alps, whereas a drying occurred in summer in the surrounding plains. A general increase in the daily annual maximum of precipitation is evidenced (20 to 40 % per century), suggesting an increase in extreme events that is significant only when considering long time series, typically 50 to 80 years.
Wei Wang, Laurens Ganzeveld, Samuel Rossabi, Jacques Hueber, and Detlev Helmig
Atmos. Chem. Phys., 20, 11287–11304, https://doi.org/10.5194/acp-20-11287-2020, https://doi.org/10.5194/acp-20-11287-2020, 2020
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Trees exchange with the atmosphere nitrogen oxides and ozone, affecting the tropospheric composition and consequently air quality and ecosystem health. We examined the leaf-level gas exchanges for four typical tree species (pine, maple, oak, aspen) found in northern Michigan, US. The leaves largely absorb the gases, showing little evidence of emission. We measured the uptake rates that can be used to improve model studies of the source and sink processes controlling these gases in forests.
Johannes Bieser, Hélène Angot, Franz Slemr, and Lynwill Martin
Atmos. Chem. Phys., 20, 10427–10439, https://doi.org/10.5194/acp-20-10427-2020, https://doi.org/10.5194/acp-20-10427-2020, 2020
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We use numerical models to determine the origin of air masses measured for elemental gaseous mercury (GEM) at Cape Point (CPT), South Africa. Our analysis is based on 10 years of hourly GEM measurements at CPT from 2007 to 2016. Based on GEM concentration and the origin of the air mass, we identify source and sink regions at CPT. We find, that the warm Agulhas Current to the south-east is the major Hg source and the continent the major sink.
Florentin Lemonnier, Alizée Chemison, Hubert Gallée, Gerhard Krinner, Jean-Baptiste Madeleine, Chantal Claud, and Christophe Genthon
The Cryosphere Discuss., https://doi.org/10.5194/tc-2020-167, https://doi.org/10.5194/tc-2020-167, 2020
Manuscript not accepted for further review
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This study presents the first evaluation from snowfall observations in Antarctica of the general circulation model LMDz (global), the atmospheric component of the coupled IPSL Climate Model that is part of CMIP6 (IPCC). We also present an evaluation of the new version of the MAR model (regional), considered as a reference in terms of polar climate modelling. Both models show satisfying results for the modelling of precipitation in Antarctica.
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.
Dean Howard, Yannick Agnan, Detlev Helmig, Yu Yang, and Daniel Obrist
Biogeosciences, 17, 4025–4042, https://doi.org/10.5194/bg-17-4025-2020, https://doi.org/10.5194/bg-17-4025-2020, 2020
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The Arctic tundra represents a vast store of carbon that may be broken down by microbial activity into greenhouse gases such as CO2 and CH4. Though microbes are less active in winter, the long duration of the cold season makes this period very important for carbon cycling. We show that, under conditions of warmer winter air temperatures and greater snowfall, deeper soils can remain warm enough to sustain significantly enhanced CH4 emission. This could have large implications for future climates.
Tuukka Petäjä, Ella-Maria Duplissy, Ksenia Tabakova, Julia Schmale, Barbara Altstädter, Gerard Ancellet, Mikhail Arshinov, Yurii Balin, Urs Baltensperger, Jens Bange, Alison Beamish, Boris Belan, Antoine Berchet, Rossana Bossi, Warren R. L. Cairns, Ralf Ebinghaus, Imad El Haddad, Beatriz Ferreira-Araujo, Anna Franck, Lin Huang, Antti Hyvärinen, Angelika Humbert, Athina-Cerise Kalogridis, Pavel Konstantinov, Astrid Lampert, Matthew MacLeod, Olivier Magand, Alexander Mahura, Louis Marelle, Vladimir Masloboev, Dmitri Moisseev, Vaios Moschos, Niklas Neckel, Tatsuo Onishi, Stefan Osterwalder, Aino Ovaska, Pauli Paasonen, Mikhail Panchenko, Fidel Pankratov, Jakob B. Pernov, Andreas Platis, Olga Popovicheva, Jean-Christophe Raut, Aurélie Riandet, Torsten Sachs, Rosamaria Salvatori, Roberto Salzano, Ludwig Schröder, Martin Schön, Vladimir Shevchenko, Henrik Skov, Jeroen E. Sonke, Andrea Spolaor, Vasileios K. Stathopoulos, Mikko Strahlendorff, Jennie L. Thomas, Vito Vitale, Sterios Vratolis, Carlo Barbante, Sabine Chabrillat, Aurélien Dommergue, Konstantinos Eleftheriadis, Jyri Heilimo, Kathy S. Law, Andreas Massling, Steffen M. Noe, Jean-Daniel Paris, André S. H. Prévôt, Ilona Riipinen, Birgit Wehner, Zhiyong Xie, and Hanna K. Lappalainen
Atmos. Chem. Phys., 20, 8551–8592, https://doi.org/10.5194/acp-20-8551-2020, https://doi.org/10.5194/acp-20-8551-2020, 2020
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The role of polar regions is increasing in terms of megatrends such as globalization, new transport routes, demography, and the use of natural resources with consequent effects on regional and transported pollutant concentrations. Here we summarize initial results from our integrative project exploring the Arctic environment and pollution to deliver data products, metrics, and indicators for stakeholders.
Franz Slemr, Lynwill Martin, Casper Labuschagne, Thumeka Mkololo, Hélène Angot, Olivier Magand, Aurélien Dommergue, Philippe Garat, Michel Ramonet, and Johannes Bieser
Atmos. Chem. Phys., 20, 7683–7692, https://doi.org/10.5194/acp-20-7683-2020, https://doi.org/10.5194/acp-20-7683-2020, 2020
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Monitoring of atmospheric mercury (Hg) concentrations is an important part of the effectiveness evaluation of the Minamata Convention on Hg. Hg concentrations in 2012–2017 at Cape Point, South Africa, and at Amsterdam Island in the remote Indian Ocean are comparable, and no trend or a slightly downward trend was observed at both stations. Over the 2007–2017 period an upward trend was observed at CPT which was driven mainly by the 2007–2014 data. The trend and its change are discussed.
Tao Ma, Hiroshi Furutani, Fengkui Duan, Takashi Kimoto, Jingkun Jiang, Qiang Zhang, Xiaobin Xu, Ying Wang, Jian Gao, Guannan Geng, Meng Li, Shaojie Song, Yongliang Ma, Fei Che, Jie Wang, Lidan Zhu, Tao Huang, Michisato Toyoda, and Kebin He
Atmos. Chem. Phys., 20, 5887–5897, https://doi.org/10.5194/acp-20-5887-2020, https://doi.org/10.5194/acp-20-5887-2020, 2020
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The formation mechanisms of organic matter and sulfate in winter haze in the North China Plain remain unclear. This paper presents the identification and quantification of hydroxymethanesulfonate (HMS) in PM2.5 in Beijing winter and elucidates the heterogeneous HMS chemistry in favorable winter haze conditions. We show that the HMS not only contributes a substantial mass of organic matter, but also leads to an overestimation of sulfate in conventional measurements.
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.
Meng Gao, Jinhui Gao, Bin Zhu, Rajesh Kumar, Xiao Lu, Shaojie Song, Yuzhong Zhang, Beixi Jia, Peng Wang, Gufran Beig, Jianlin Hu, Qi Ying, Hongliang Zhang, Peter Sherman, and Michael B. McElroy
Atmos. Chem. Phys., 20, 4399–4414, https://doi.org/10.5194/acp-20-4399-2020, https://doi.org/10.5194/acp-20-4399-2020, 2020
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A regional fully coupled meteorology–chemistry model, Weather Research and Forecasting model with Chemistry (WRF-Chem), was employed to study the seasonality of ozone (O3) pollution and its sources in both China and India.
Ryan J. Pound, Tomás Sherwen, Detlev Helmig, Lucy J. Carpenter, and Mat J. Evans
Atmos. Chem. Phys., 20, 4227–4239, https://doi.org/10.5194/acp-20-4227-2020, https://doi.org/10.5194/acp-20-4227-2020, 2020
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Ozone is an important pollutant with impacts on health and the environment. Ozone is lost to plants, land and the oceans. Loss to the ocean is slow compared to all other types of land cover and has not received as much attention. We build on previous work to more accurately model ozone loss to the ocean. We find changes in the concentration of ozone over the oceans, notably the Southern Ocean, which improves model performance.
Meng Gao, Zirui Liu, Bo Zheng, Dongsheng Ji, Peter Sherman, Shaojie Song, Jinyuan Xin, Cheng Liu, Yuesi Wang, Qiang Zhang, Jia Xing, Jingkun Jiang, Zifa Wang, Gregory R. Carmichael, and Michael B. McElroy
Atmos. Chem. Phys., 20, 1497–1505, https://doi.org/10.5194/acp-20-1497-2020, https://doi.org/10.5194/acp-20-1497-2020, 2020
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We quantified the relative influences of anthropogenic emissions and meteorological conditions on PM2.5 concentrations in Beijing over the winters of 2002–2016. Meteorological conditions over the study period would have led to an increase of haze in Beijing, but the strict emission control measures have suppressed the unfavorable influences of the recent climate.
Marion Donat-Magnin, Nicolas C. Jourdain, Hubert Gallée, Charles Amory, Christoph Kittel, Xavier Fettweis, Jonathan D. Wille, Vincent Favier, Amine Drira, and Cécile Agosta
The Cryosphere, 14, 229–249, https://doi.org/10.5194/tc-14-229-2020, https://doi.org/10.5194/tc-14-229-2020, 2020
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Modeling the interannual variability of the surface conditions over Antarctic glaciers is important for the identification of climate trends and climate predictions and to assess models. We simulate snow accumulation and surface melting in the Amundsen sector (West Antarctica) over 1979–2017. For all the glaciers, the interannual variability of summer snow accumulation and surface melting is driven by two distinct mechanisms related to variations in the Amundsen Sea Low strength and position.
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.
Andrea Spolaor, Elena Barbaro, David Cappelletti, Clara Turetta, Mauro Mazzola, Fabio Giardi, Mats P. Björkman, Federico Lucchetta, Federico Dallo, Katrine Aspmo Pfaffhuber, Hélène Angot, Aurelien Dommergue, Marion Maturilli, Alfonso Saiz-Lopez, Carlo Barbante, and Warren R. L. Cairns
Atmos. Chem. Phys., 19, 13325–13339, https://doi.org/10.5194/acp-19-13325-2019, https://doi.org/10.5194/acp-19-13325-2019, 2019
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The main aims of the study are to (a) detect whether mercury in the surface snow undergoes a daily cycle as determined in the atmosphere, (b) compare the mercury concentration in surface snow with the concentration in the atmosphere, (c) evaluate the effect of snow depositions, (d) detect whether iodine and bromine in the surface snow undergo a daily cycle, and (e) evaluate the role of metereological and atmospheric conditions. Different behaviours were determined during different seasons.
Martin Jiskra, Jeroen E. Sonke, Yannick Agnan, Detlev Helmig, and Daniel Obrist
Biogeosciences, 16, 4051–4064, https://doi.org/10.5194/bg-16-4051-2019, https://doi.org/10.5194/bg-16-4051-2019, 2019
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The tundra plays a pivotal role in Arctic mercury cycling by storing atmospheric mercury deposition and shuttling it to the Arctic Ocean. We used the isotopic fingerprint of mercury to investigate the processes controlling atmospheric mercury deposition. We found that the uptake of atmospheric mercury by vegetation was the major deposition source. Direct deposition to snow or soils only played a minor role. These results improve our understanding of Arctic mercury cycling.
Xiaoxiao Li, Shaojie Song, Wei Zhou, Jiming Hao, Douglas R. Worsnop, and Jingkun Jiang
Atmos. Chem. Phys., 19, 12163–12174, https://doi.org/10.5194/acp-19-12163-2019, https://doi.org/10.5194/acp-19-12163-2019, 2019
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Aerosol liquid water is ubiquitous in ambient aerosol. Using long-term aerosol chemical composition to model the aerosol water in Beijing, we found that water absorbed by organics contributes a significant fraction to the total aerosol water. We emphasize the hygroscopicity of organics is highly variable and should be taken into consideration in modelling. A positive feedback loop between organic hygroscopicity and aerosol water was found as one of the driving factors of severe haze in Beijing.
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.
Shaojie Song, Meng Gao, Weiqi Xu, Yele Sun, Douglas R. Worsnop, John T. Jayne, Yuzhong Zhang, Lei Zhu, Mei Li, Zhen Zhou, Chunlei Cheng, Yibing Lv, Ying Wang, Wei Peng, Xiaobin Xu, Nan Lin, Yuxuan Wang, Shuxiao Wang, J. William Munger, Daniel J. Jacob, and Michael B. McElroy
Atmos. Chem. Phys., 19, 1357–1371, https://doi.org/10.5194/acp-19-1357-2019, https://doi.org/10.5194/acp-19-1357-2019, 2019
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Chemistry responsible for sulfate production in northern China winter haze remains mysterious. We propose a potentially key pathway through the reaction of formaldehyde and sulfur dioxide that has not been accounted for in previous studies. The special atmospheric conditions favor the formation and existence of their complex, hydroxymethanesulfonate (HMS).
Cécile Agosta, Charles Amory, Christoph Kittel, Anais Orsi, Vincent Favier, Hubert Gallée, Michiel R. van den Broeke, Jan T. M. Lenaerts, Jan Melchior van Wessem, Willem Jan van de Berg, and Xavier Fettweis
The Cryosphere, 13, 281–296, https://doi.org/10.5194/tc-13-281-2019, https://doi.org/10.5194/tc-13-281-2019, 2019
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Antarctic surface mass balance (ASMB), a component of the sea level budget, is commonly estimated through modelling as observations are scarce. The polar-oriented regional climate model MAR performs well in simulating the observed ASMB. MAR and RACMO2 share common biases we relate to drifting snow transport, with a 3 times larger magnitude than in previous estimates. Sublimation of precipitation in the katabatic layer modelled by MAR is of a magnitude similar to an observation-based estimate.
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.
Benjamin Brown-Steiner, Noelle E. Selin, Ronald Prinn, Simone Tilmes, Louisa Emmons, Jean-François Lamarque, and Philip Cameron-Smith
Geosci. Model Dev., 11, 4155–4174, https://doi.org/10.5194/gmd-11-4155-2018, https://doi.org/10.5194/gmd-11-4155-2018, 2018
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We conduct three simulations of atmospheric chemistry using chemical mechanisms of different levels of complexity and compare their results to observations. We explore situations in which the simplified mechanisms match the output of the most complex mechanism, as well as when they diverge. We investigate how concurrent utilization of chemical mechanisms of different complexities can further our atmospheric-chemistry understanding at various scales and give some strategies for future research.
Luca Naitza, Davide Putero, Angela Marinoni, Francescopiero Calzolari, Fabrizio Roccato, Maurizio Busetto, Damiano Sferlazzo, Eleonora Aruffo, Piero Di Carlo, Mariantonia Bencardino, Francesco D'Amore, Francesca Sprovieri, Nicola Pirrone, Federico Dallo, Jacopo Gabrieli, Massimiliano Vardè, Carlo Barbante, Paolo Bonasoni, and Paolo Cristofanelli
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2018-245, https://doi.org/10.5194/amt-2018-245, 2018
Revised manuscript not accepted
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We implemented a prototype of a centralized system to support atmospheric observatories in data production and submission. By using the “R” Language, for several near-surface ECVs, we developed specific routines for data filtering, flagging, formatting, and creation of data products for detecting instrumental problems or special atmospheric events. Our effort would improve atmospheric data quality, accelerate the process of data submission and make the data flagging more “objective".
Benjamin Brown-Steiner, Noelle E. Selin, Ronald G. Prinn, Erwan Monier, Simone Tilmes, Louisa Emmons, and Fernando Garcia-Menendez
Atmos. Chem. Phys., 18, 8373–8388, https://doi.org/10.5194/acp-18-8373-2018, https://doi.org/10.5194/acp-18-8373-2018, 2018
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Detecting signals in observations and simulations of atmospheric chemistry is difficult due to the underlying variability in the chemistry, meteorology, and climatology. Here we examine the scale dependence of ozone variability and explore strategies for reducing or averaging this variability and thereby enhancing ozone signal detection capabilities. We find that 10–15 years of temporal averaging, and some level of spatial averaging, reduces the risk of overconfidence in ozone signals.
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.
Shaojie Song, Meng Gao, Weiqi Xu, Jingyuan Shao, Guoliang Shi, Shuxiao Wang, Yuxuan Wang, Yele Sun, and Michael B. McElroy
Atmos. Chem. Phys., 18, 7423–7438, https://doi.org/10.5194/acp-18-7423-2018, https://doi.org/10.5194/acp-18-7423-2018, 2018
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Severe haze events occur frequently over northern China, especially in winter. Acidity plays a critical role in the formation of secondary PM2.5 and its toxicity. Using field measurements of gases and particles to critically evaluate two thermodynamic models routinely employed to determine particle acidity, we found that China's winter haze particles are generally within a moderately acidic range (pH 4–5) and not highly acidic (0) or neutral (7) as has been previously reported in the literature.
Yaoxian Huang, Shiliang Wu, Louisa J. Kramer, Detlev Helmig, and Richard E. Honrath
Atmos. Chem. Phys., 17, 14661–14674, https://doi.org/10.5194/acp-17-14661-2017, https://doi.org/10.5194/acp-17-14661-2017, 2017
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A global chemical transport model (GEOS-Chem) was employed to simulate surface ozone and its precursors at Summit, Greenland in the Arctic and compare them with 2-year in situ surface observations. The model performed well in simulating certain species (such as carbon monoxide and propane), but some significant discrepancies were identified for other species (e.g., nitrogen oxides, ethane, PAN, and ozone). We further investigated the exact causes for model–data biases.
Mike J. Newland, Patricia Martinerie, Emmanuel Witrant, Detlev Helmig, David R. Worton, Chris Hogan, William T. Sturges, and Claire E. Reeves
Atmos. Chem. Phys., 17, 8269–8283, https://doi.org/10.5194/acp-17-8269-2017, https://doi.org/10.5194/acp-17-8269-2017, 2017
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We report increasing levels of alkyl nitrates in the Northern Hemisphere atmosphere between 1960 and the mid-1990s. These increases are symptomatic of large-scale changes to the chemical composition of the atmosphere, particularly with regards to the amounts of short-lived, reactive species. The observed increases are likely driven by increasing levels of nitrogen oxides. These changes have direct implications for the lifetimes of climate-relevant species in the atmosphere, such as methane.
Johannes Bieser, Franz Slemr, Jesse Ambrose, Carl Brenninkmeijer, Steve Brooks, Ashu Dastoor, Francesco DeSimone, Ralf Ebinghaus, Christian N. Gencarelli, Beate Geyer, Lynne E. Gratz, Ian M. Hedgecock, Daniel Jaffe, Paul Kelley, Che-Jen Lin, Lyatt Jaegle, Volker Matthias, Andrei Ryjkov, Noelle E. Selin, Shaojie Song, Oleg Travnikov, Andreas Weigelt, Winston Luke, Xinrong Ren, Andreas Zahn, Xin Yang, Yun Zhu, and Nicola Pirrone
Atmos. Chem. Phys., 17, 6925–6955, https://doi.org/10.5194/acp-17-6925-2017, https://doi.org/10.5194/acp-17-6925-2017, 2017
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We conducted a multi model study to investigate our ability to reproduce the vertical distribution of mercury in the atmosphere. For this, we used observational data from over 40 aircraft flights in EU and US. We compared observations to the results of seven chemistry transport models and found that the models are able to reproduce vertical gradients of total and elemental Hg. Finally, we found that different chemical reactions seem responsible for the oxidation of Hg depending on altitude.
Antonella Macagnano, Viviana Perri, Emiliano Zampetti, Andrea Bearzotti, Fabrizio De Cesare, Francesca Sprovieri, and Nicola Pirrone
Atmos. Chem. Phys., 17, 6883–6893, https://doi.org/10.5194/acp-17-6883-2017, https://doi.org/10.5194/acp-17-6883-2017, 2017
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By exploiting the photocatalytic properties of electrospun titania nanofibers, a novel conductometric sensor was designed and fabricated to entrap and detect GEM in air. Such a sensor was able to work at room temperature and was highly sensitive to elemental mercury. Since it is composed of titania and gold nanoparticles, it seems to be robust and resistant to common solvents and VOCs in the air.
Oleg Travnikov, Hélène Angot, Paulo Artaxo, Mariantonia Bencardino, Johannes Bieser, Francesco D'Amore, Ashu Dastoor, Francesco De Simone, María del Carmen Diéguez, Aurélien Dommergue, Ralf Ebinghaus, Xin Bin Feng, Christian N. Gencarelli, Ian M. Hedgecock, Olivier Magand, Lynwill Martin, Volker Matthias, Nikolay Mashyanov, Nicola Pirrone, Ramesh Ramachandran, Katie Alana Read, Andrei Ryjkov, Noelle E. Selin, Fabrizio Sena, Shaojie Song, Francesca Sprovieri, Dennis Wip, Ingvar Wängberg, and Xin Yang
Atmos. Chem. Phys., 17, 5271–5295, https://doi.org/10.5194/acp-17-5271-2017, https://doi.org/10.5194/acp-17-5271-2017, 2017
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The study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measurement data and simulation results of chemical transport models. Evaluation of the model simulations and numerical experiments against observations allows explaining spatial and temporal variations of Hg concentration in the near-surface atmospheric layer and shows possibility of multiple pathways of Hg oxidation occurring concurrently in various parts of the atmosphere.
Colin P. Thackray and Noelle E. Selin
Atmos. Chem. Phys., 17, 4585–4597, https://doi.org/10.5194/acp-17-4585-2017, https://doi.org/10.5194/acp-17-4585-2017, 2017
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PFCAs are toxic contaminants that can form in the atmosphere when precursor chemicals are released and degrade. We calculate the capacity of different atmospheric environments to form PFCAs this way. Different environments have very different capacities to form PFCAs, with the atmosphere far from sources of pollution being much better able to make the more toxic PFCAs. While the chemistry involved has uncertainties, they are small compared to the differences between environments.
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.
Francesca Sprovieri, Nicola Pirrone, Mariantonia Bencardino, Francesco D'Amore, Helene Angot, Carlo Barbante, Ernst-Günther Brunke, Flor Arcega-Cabrera, Warren Cairns, Sara Comero, María del Carmen Diéguez, Aurélien Dommergue, Ralf Ebinghaus, Xin Bin Feng, Xuewu Fu, Patricia Elizabeth Garcia, Bernd Manfred Gawlik, Ulla Hageström, Katarina Hansson, Milena Horvat, Jože Kotnik, Casper Labuschagne, Olivier Magand, Lynwill Martin, Nikolay Mashyanov, Thumeka Mkololo, John Munthe, Vladimir Obolkin, Martha Ramirez Islas, Fabrizio Sena, Vernon Somerset, Pia Spandow, Massimiliano Vardè, Chavon Walters, Ingvar Wängberg, Andreas Weigelt, Xu Yang, and Hui Zhang
Atmos. Chem. Phys., 17, 2689–2708, https://doi.org/10.5194/acp-17-2689-2017, https://doi.org/10.5194/acp-17-2689-2017, 2017
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The results on total mercury (THg) wet deposition flux obtained within the GMOS network have been presented and discussed to understand the atmospheric Hg cycling and its seasonal depositional patterns over the 2011–2015 period. The data set provides new insight into baseline concentrations of THg concentrations in precipitation particularly in regions where wet deposition and atmospheric Hg species were not investigated before, opening the way for additional measurements and modeling studies.
Francesco De Simone, Paulo Artaxo, Mariantonia Bencardino, Sergio Cinnirella, Francesco Carbone, Francesco D'Amore, Aurélien Dommergue, Xin Bin Feng, Christian N. Gencarelli, Ian M. Hedgecock, Matthew S. Landis, Francesca Sprovieri, Noriuki Suzuki, Ingvar Wängberg, and Nicola Pirrone
Atmos. Chem. Phys., 17, 1881–1899, https://doi.org/10.5194/acp-17-1881-2017, https://doi.org/10.5194/acp-17-1881-2017, 2017
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Biomass burning (BB) releases of Hg, usually considered to be Hg(0), are a significant global source of atmospheric Hg. However there is experimental evidence that a fraction of this Hg is bound to particulate matter, Hg(P). This modelling study shows how increasing fractions of Hg(P) reduce the availability of Hg to the global pool, raising Hg exposure for those regions characterized by high BB, with implications for the sub-Arctic and also rice-growing areas in South-East Asia.
Christophe Genthon, Luc Piard, Etienne Vignon, Jean-Baptiste Madeleine, Mathieu Casado, and Hubert Gallée
Atmos. Chem. Phys., 17, 691–704, https://doi.org/10.5194/acp-17-691-2017, https://doi.org/10.5194/acp-17-691-2017, 2017
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Natural atmospheric supersaturation is a norm rather than an exception at the surface of Dome C on the Antarctic Plateau. This is reported by hygrometers adapted to perform in extreme cold environments and avoid release of excess moisture before it is measured. One year of observation shows that atmospheric models with cold microphysics parameterizations designed for high altitude cirrus reproduce frequently but fail with the detailed statistics of supersaturation at the surface of Dome C.
Maria C. Diéguez, Patricia E. Garcia, Mariantonia Bencardino, Francesco D'Amore, Jessica Castagna, Sergio Ribeiro Guevara, and Francesca Sprovieri
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-1076, https://doi.org/10.5194/acp-2016-1076, 2017
Preprint withdrawn
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First continuous records of gaseous elemental Hg (GEM) concentrations monitored at the GMOS EMMA monitoring station in Nahuel Huapi National Park (Northwestern Patagonia, Argentina) showed seasonal and daily variation with mean values higher during spring and winter (ca. 0.92 ng m−3) and higher day-time levels across all seasons. GEM levels were determined by the westerly winds and backward trajectory analysis highlighted the influence of clean oceanic air masses and volcanoes in the Andes.
Andreas Weigelt, Franz Slemr, Ralf Ebinghaus, Nicola Pirrone, Johannes Bieser, Jan Bödewadt, Giulio Esposito, and Peter F. J. van Velthoven
Atmos. Chem. Phys., 16, 13653–13668, https://doi.org/10.5194/acp-16-13653-2016, https://doi.org/10.5194/acp-16-13653-2016, 2016
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Hg ∕ SO2, Hg ∕ CO, and NOx ∕ SO2 emission ratios (ERs) in the plume of the coal-fired power plant (CFPP), Lippendorf, near Leipzig in Germany, were determined in August 2013. GOM fraction of mercury emissions was also assessed. Measured Hg ∕ SO2 and Hg ∕ CO ERs were consistent with the ratios calculated from annual emissions in 2013 reported by the CFPP operator. The NOx ∕ SO2 ER was somewhat lower. GOM fractions of ~ 40 % of CFPP mercury emissions in current emission inventories are overestimated.
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.
Jozef M. Pacyna, Oleg Travnikov, Francesco De Simone, Ian M. Hedgecock, Kyrre Sundseth, Elisabeth G. Pacyna, Frits Steenhuisen, Nicola Pirrone, John Munthe, and Karin Kindbom
Atmos. Chem. Phys., 16, 12495–12511, https://doi.org/10.5194/acp-16-12495-2016, https://doi.org/10.5194/acp-16-12495-2016, 2016
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An assessment of current and future emissions, air concentrations and atmospheric deposition of mercury worldwide is presented on the basis of results obtained during the performance of the EU GMOS (Global Mercury Observation System) project. Emission estimates for mercury were prepared with the main goal of applying them in models to assess current (2013) and future (2035) air concentrations and atmospheric deposition of this contaminant.
Francesca Sprovieri, Nicola Pirrone, Mariantonia Bencardino, Francesco D'Amore, Francesco Carbone, Sergio Cinnirella, Valentino Mannarino, Matthew Landis, Ralf Ebinghaus, Andreas Weigelt, Ernst-Günther Brunke, Casper Labuschagne, Lynwill Martin, John Munthe, Ingvar Wängberg, Paulo Artaxo, Fernando Morais, Henrique de Melo Jorge Barbosa, Joel Brito, Warren Cairns, Carlo Barbante, María del Carmen Diéguez, Patricia Elizabeth Garcia, Aurélien Dommergue, Helene Angot, Olivier Magand, Henrik Skov, Milena Horvat, Jože Kotnik, Katie Alana Read, Luis Mendes Neves, Bernd Manfred Gawlik, Fabrizio Sena, Nikolay Mashyanov, Vladimir Obolkin, Dennis Wip, Xin Bin Feng, Hui Zhang, Xuewu Fu, Ramesh Ramachandran, Daniel Cossa, Joël Knoery, Nicolas Marusczak, Michelle Nerentorp, and Claus Norstrom
Atmos. Chem. Phys., 16, 11915–11935, https://doi.org/10.5194/acp-16-11915-2016, https://doi.org/10.5194/acp-16-11915-2016, 2016
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This work presents atmospheric Hg concentrations recorded within the GMOS global network analyzing Hg measurement results in terms of temporal trends, seasonality and comparability within the network. The over-arching benefit of this coordinated Hg monitoring network would clearly be the production of high-quality measurement datasets on a global scale useful in developing and validating models on different spatial and temporal scales.
Hélène Angot, Ashu Dastoor, Francesco De Simone, Katarina Gårdfeldt, Christian N. Gencarelli, Ian M. Hedgecock, Sarka Langer, Olivier Magand, Michelle N. Mastromonaco, Claus Nordstrøm, Katrine A. Pfaffhuber, Nicola Pirrone, Andrei Ryjkov, Noelle E. Selin, Henrik Skov, Shaojie Song, Francesca Sprovieri, Alexandra Steffen, Kenjiro Toyota, Oleg Travnikov, Xin Yang, and Aurélien Dommergue
Atmos. Chem. Phys., 16, 10735–10763, https://doi.org/10.5194/acp-16-10735-2016, https://doi.org/10.5194/acp-16-10735-2016, 2016
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This is a synthesis of the atmospheric mercury (Hg) monitoring data available in recent years (2011–2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. Based on this comparison, we discuss whether the processes that affect atmospheric Hg seasonality and interannual variability are appropriately represented in the models, and identify remaining research gaps.
Hélène Angot, Olivier Magand, Detlev Helmig, Philippe Ricaud, Boris Quennehen, Hubert Gallée, Massimo Del Guasta, Francesca Sprovieri, Nicola Pirrone, Joël Savarino, and Aurélien Dommergue
Atmos. Chem. Phys., 16, 8249–8264, https://doi.org/10.5194/acp-16-8249-2016, https://doi.org/10.5194/acp-16-8249-2016, 2016
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While the Arctic has been extensively monitored, there is still much to be learned from the Antarctic continent regarding the processes that govern the budget of atmospheric mercury species. We report here the first year-round measurements of gaseous elemental mercury (Hg(0)) in the atmosphere and in snowpack interstitial air on the East Antarctic ice sheet. The striking reactivity observed on the Antarctic plateau most likely influences the cycle of atmospheric mercury on a continental scale.
Hélène Angot, Iris Dion, Nicolas Vogel, Michel Legrand, Olivier Magand, and Aurélien Dommergue
Atmos. Chem. Phys., 16, 8265–8279, https://doi.org/10.5194/acp-16-8265-2016, https://doi.org/10.5194/acp-16-8265-2016, 2016
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This paper presents a multi-year record of atmospheric gaseous elemental mercury (Hg(0)) at Dumont d’Urville (DDU) on the East Antarctic coast. This record reveals particularities that are not seen at other coastal Antarctic sites, likely due to the more frequent arrival of inland air masses at DDU than at other coastal sites, and to the influence of oceanic air masses. This study confirms the influence of processes observed inland on the cycle of atmospheric mercury at a continental scale.
Michel Legrand, Susanne Preunkert, Joël Savarino, Markus M. Frey, Alexandre Kukui, Detlev Helmig, Bruno Jourdain, Anna E. Jones, Rolf Weller, Neil Brough, and Hubert Gallée
Atmos. Chem. Phys., 16, 8053–8069, https://doi.org/10.5194/acp-16-8053-2016, https://doi.org/10.5194/acp-16-8053-2016, 2016
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Surface ozone, the most abundant atmospheric oxidant, has been measured since 2004 at the coastal East Antarctic site of Dumont d’Urville, and since 2007 at the Concordia station located on the high East Antarctic plateau. Long-term changes, seasonal and diurnal cycles, as well as inter-annual summer variability observed at these two East Antarctic sites are discussed. Influences like sea ice extent and outflow from inland Antarctica are discussed.
N. Pirrone, S. Cinnirella, S. Nativi, F. Sprovieri, and I. M. Hedgecock
Int. Arch. Photogramm. Remote Sens. Spatial Inf. Sci., XLI-B8, 1349–1355, https://doi.org/10.5194/isprs-archives-XLI-B8-1349-2016, https://doi.org/10.5194/isprs-archives-XLI-B8-1349-2016, 2016
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.
Carey L. Friedman and Noelle E. Selin
Atmos. Chem. Phys., 16, 3433–3448, https://doi.org/10.5194/acp-16-3433-2016, https://doi.org/10.5194/acp-16-3433-2016, 2016
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We present a new global model to simulate the atmospheric transport of toxic contaminants (PCBs). We evaluate the model against PCB observations in the northern hemisphere midlatitude and Arctic atmosphere. We then use the model to calculate global budgets of PCBs and to examine the influence of climate- and emissions-driven processes on Arctic atmospheric concentrations. We find that processes occurring outside the Arctic have a greater influence on Arctic PCBs than those occurring within.
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.
V. Shah, L. Jaeglé, L. E. Gratz, J. L. Ambrose, D. A. Jaffe, N. E. Selin, S. Song, T. L. Campos, F. M. Flocke, M. Reeves, D. Stechman, M. Stell, J. Festa, J. Stutz, A. J. Weinheimer, D. J. Knapp, D. D. Montzka, G. S. Tyndall, E. C. Apel, R. S. Hornbrook, A. J. Hills, D. D. Riemer, N. J. Blake, C. A. Cantrell, and R. L. Mauldin III
Atmos. Chem. Phys., 16, 1511–1530, https://doi.org/10.5194/acp-16-1511-2016, https://doi.org/10.5194/acp-16-1511-2016, 2016
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We present airborne observations of mercury over the southeastern USA during summer. Higher concentrations of oxidized mercury were observed in clean, dry air masses descending in the subtropical anti-cyclones. We used an atmospheric model to simulate the chemistry and transport of mercury. We found reasonable agreement with the observations when the modeled oxidation of elemental mercury was increased, suggesting fast cycling between elemental and oxidized mercury.
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.
S. Song, N. E. Selin, A. L. Soerensen, H. Angot, R. Artz, S. Brooks, E.-G. Brunke, G. Conley, A. Dommergue, R. Ebinghaus, T. M. Holsen, D. A. Jaffe, S. Kang, P. Kelley, W. T. Luke, O. Magand, K. Marumoto, K. A. Pfaffhuber, X. Ren, G.-R. Sheu, F. Slemr, T. Warneke, A. Weigelt, P. Weiss-Penzias, D. C. Wip, and Q. Zhang
Atmos. Chem. Phys., 15, 7103–7125, https://doi.org/10.5194/acp-15-7103-2015, https://doi.org/10.5194/acp-15-7103-2015, 2015
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A better knowledge of mercury (Hg) emission fluxes into the global atmosphere is important for assessing its human health impacts and evaluating the effectiveness of corresponding policy actions. We for the first time apply a top-down approach at a global scale to quantitatively estimate present-day mercury emission sources as well as key parameters in a chemical transport model, in order to better constrain the global biogeochemical cycle of mercury.
L. J. Kramer, D. Helmig, J. F. Burkhart, A. Stohl, S. Oltmans, and R. E. Honrath
Atmos. Chem. Phys., 15, 6827–6849, https://doi.org/10.5194/acp-15-6827-2015, https://doi.org/10.5194/acp-15-6827-2015, 2015
L. K. Emmons, S. R. Arnold, S. A. Monks, V. Huijnen, S. Tilmes, K. S. Law, J. L. Thomas, J.-C. Raut, I. Bouarar, S. Turquety, Y. Long, B. Duncan, S. Steenrod, S. Strode, J. Flemming, J. Mao, J. Langner, A. M. Thompson, D. Tarasick, E. C. Apel, D. R. Blake, R. C. Cohen, J. Dibb, G. S. Diskin, A. Fried, S. R. Hall, L. G. Huey, A. J. Weinheimer, A. Wisthaler, T. Mikoviny, J. Nowak, J. Peischl, J. M. Roberts, T. Ryerson, C. Warneke, and D. Helmig
Atmos. Chem. Phys., 15, 6721–6744, https://doi.org/10.5194/acp-15-6721-2015, https://doi.org/10.5194/acp-15-6721-2015, 2015
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Eleven 3-D tropospheric chemistry models have been compared and evaluated with observations in the Arctic during the International Polar Year (IPY 2008). Large differences are seen among the models, particularly related to the model chemistry of volatile organic compounds (VOCs) and reactive nitrogen (NOx, PAN, HNO3) partitioning. Consistency among the models in the underestimation of CO, ethane and propane indicates the emission inventory is too low for these compounds.
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.
K. Dzepina, C. Mazzoleni, P. Fialho, S. China, B. Zhang, R. C. Owen, D. Helmig, J. Hueber, S. Kumar, J. A. Perlinger, L. J. Kramer, M. P. Dziobak, M. T. Ampadu, S. Olsen, D. J. Wuebbles, and L. R. Mazzoleni
Atmos. Chem. Phys., 15, 5047–5068, https://doi.org/10.5194/acp-15-5047-2015, https://doi.org/10.5194/acp-15-5047-2015, 2015
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Aerosol was sampled at the Pico Mountain Observatory located at 2.2km amsl on Pico Island of the North Atlantic Azores archipelago. Two aerosol samples characterized by ultrahigh resolution mass spectrometry had biomass burning and marine emissions origins, as corroborated by collocated gas- and particle-phase measurements, air masses analyses and satellites. The paper presents the first molecular characterization of aged and processed aerosol intercepted at a remote lower free troposphere
F. Slemr, H. Angot, A. Dommergue, O. Magand, M. Barret, A. Weigelt, R. Ebinghaus, E.-G. Brunke, K. A. Pfaffhuber, G. Edwards, D. Howard, J. Powell, M. Keywood, and F. Wang
Atmos. Chem. Phys., 15, 3125–3133, https://doi.org/10.5194/acp-15-3125-2015, https://doi.org/10.5194/acp-15-3125-2015, 2015
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• Longer-term mercury measurement in the Southern Hemisphere is compared.
• Mercury, in terms of monthly and annual medians and averages, is more evenly distributed than hitherto believed.
• Consequently, trends observed at one or a few sites are likely to be representative of the whole hemisphere, and smaller trends can be detected in shorter time periods.
• We report a change in the trend sign at Cape Point from decreasing mercury concentrations in 1996-2004 to increasing ones since 2007.
P. Weiss-Penzias, H. M. Amos, N. E. Selin, M. S. Gustin, D. A. Jaffe, D. Obrist, G.-R. Sheu, and A. Giang
Atmos. Chem. Phys., 15, 1161–1173, https://doi.org/10.5194/acp-15-1161-2015, https://doi.org/10.5194/acp-15-1161-2015, 2015
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Speciated atmospheric Hg measurements from five high-elevation sites were compared with a global mercury model. The comparison confirmed that reactive mercury is formed in dry free tropospheric air from the oxidation of elemental Hg, more so in the summer than in other seasons. Simulations run with OH-O3 oxidation instead of the Br oxidation mechanism compared more closely with observations at desert sites, suggesting future simulations should include multiple reaction mechanisms simultaneously.
R. Ahmadov, S. McKeen, M. Trainer, R. Banta, A. Brewer, S. Brown, P. M. Edwards, J. A. de Gouw, G. J. Frost, J. Gilman, D. Helmig, B. Johnson, A. Karion, A. Koss, A. Langford, B. Lerner, J. Olson, S. Oltmans, J. Peischl, G. Pétron, Y. Pichugina, J. M. Roberts, T. Ryerson, R. Schnell, C. Senff, C. Sweeney, C. Thompson, P. R. Veres, C. Warneke, R. Wild, E. J. Williams, B. Yuan, and R. Zamora
Atmos. Chem. Phys., 15, 411–429, https://doi.org/10.5194/acp-15-411-2015, https://doi.org/10.5194/acp-15-411-2015, 2015
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High 2013 wintertime O3 pollution events associated with oil/gas production within the Uinta Basin are studied using a 3D model. It's able quantitatively to reproduce these events using emission estimates of O3 precursors based on ambient measurements (top-down approach), but unable to reproduce them using a recent bottom-up emission inventory for the oil/gas industry. The role of various physical and meteorological processes, chemical species and pathways contributing to high O3 are quantified.
S. J. Lawson, P. W. Selleck, I. E. Galbally, M. D. Keywood, M. J. Harvey, C. Lerot, D. Helmig, and Z. Ristovski
Atmos. Chem. Phys., 15, 223–240, https://doi.org/10.5194/acp-15-223-2015, https://doi.org/10.5194/acp-15-223-2015, 2015
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Glyoxal and methylglyoxal are short-lived organic trace gases and important precursors of secondary organic aerosol. Measurements over oceans are sparse. We present the first in situ glyoxal and methylglyoxal observations over remote temperate oceans, alongside observations of precursor gases. Precursor gases cannot explain observed mixing ratios, highlighting an unknown source. We show a large discrepancy between calculated vertical column densities of glyoxal and those retrieved by satellite.
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.
H. Angot, M. Barret, O. Magand, M. Ramonet, and A. Dommergue
Atmos. Chem. Phys., 14, 11461–11473, https://doi.org/10.5194/acp-14-11461-2014, https://doi.org/10.5194/acp-14-11461-2014, 2014
M. D. Mulder, A. Heil, P. Kukučka, J. Klánová, J. Kuta, R. Prokeš, F. Sprovieri, and G. Lammel
Atmos. Chem. Phys., 14, 8905–8915, https://doi.org/10.5194/acp-14-8905-2014, https://doi.org/10.5194/acp-14-8905-2014, 2014
S. J. Oltmans, A. Karion, R. C. Schnell, G. Pétron, C. Sweeney, S. Wolter, D. Neff, S. A. Montzka, B. R. Miller, D. Helmig, B. J. Johnson, and J. Hueber
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-20117-2014, https://doi.org/10.5194/acpd-14-20117-2014, 2014
Revised manuscript not accepted
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
P. Boylan, D. Helmig, and J.-H. Park
Atmos. Meas. Tech., 7, 1231–1244, https://doi.org/10.5194/amt-7-1231-2014, https://doi.org/10.5194/amt-7-1231-2014, 2014
B. Zhang, R. C. Owen, J. A. Perlinger, A. Kumar, S. Wu, M. Val Martin, L. Kramer, D. Helmig, and R. E. Honrath
Atmos. Chem. Phys., 14, 2267–2287, https://doi.org/10.5194/acp-14-2267-2014, https://doi.org/10.5194/acp-14-2267-2014, 2014
D. Helmig, V. Petrenko, P. Martinerie, E. Witrant, T. Röckmann, A. Zuiderweg, R. Holzinger, J. Hueber, C. Thompson, J. W. C. White, W. Sturges, A. Baker, T. Blunier, D. Etheridge, M. Rubino, and P. Tans
Atmos. Chem. Phys., 14, 1463–1483, https://doi.org/10.5194/acp-14-1463-2014, https://doi.org/10.5194/acp-14-1463-2014, 2014
T. M. Thompson, R. K. Saari, and N. E. Selin
Atmos. Chem. Phys., 14, 969–978, https://doi.org/10.5194/acp-14-969-2014, https://doi.org/10.5194/acp-14-969-2014, 2014
A. Kumar, S. Wu, M. F. Weise, R. Honrath, R. C. Owen, D. Helmig, L. Kramer, M. Val Martin, and Q. Li
Atmos. Chem. Phys., 13, 12537–12547, https://doi.org/10.5194/acp-13-12537-2013, https://doi.org/10.5194/acp-13-12537-2013, 2013
P. M. Edwards, C. J. Young, K. Aikin, J. deGouw, W. P. Dubé, F. Geiger, J. Gilman, D. Helmig, J. S. Holloway, J. Kercher, B. Lerner, R. Martin, R. McLaren, D. D. Parrish, J. Peischl, J. M. Roberts, T. B. Ryerson, J. Thornton, C. Warneke, E. J. Williams, and S. S. Brown
Atmos. Chem. Phys., 13, 8955–8971, https://doi.org/10.5194/acp-13-8955-2013, https://doi.org/10.5194/acp-13-8955-2013, 2013
P. I. Palmer, M. Parrington, J. D. Lee, A. C. Lewis, A. R. Rickard, P. F. Bernath, T. J. Duck, D. L. Waugh, D. W. Tarasick, S. Andrews, E. Aruffo, L. J. Bailey, E. Barrett, S. J.-B. Bauguitte, K. R. Curry, P. Di Carlo, L. Chisholm, L. Dan, G. Forster, J. E. Franklin, M. D. Gibson, D. Griffin, D. Helmig, J. R. Hopkins, J. T. Hopper, M. E. Jenkin, D. Kindred, J. Kliever, M. Le Breton, S. Matthiesen, M. Maurice, S. Moller, D. P. Moore, D. E. Oram, S. J. O'Shea, R. C. Owen, C. M. L. S. Pagniello, S. Pawson, C. J. Percival, J. R. Pierce, S. Punjabi, R. M. Purvis, J. J. Remedios, K. M. Rotermund, K. M. Sakamoto, A. M. da Silva, K. B. Strawbridge, K. Strong, J. Taylor, R. Trigwell, K. A. Tereszchuk, K. A. Walker, D. Weaver, C. Whaley, and J. C. Young
Atmos. Chem. Phys., 13, 6239–6261, https://doi.org/10.5194/acp-13-6239-2013, https://doi.org/10.5194/acp-13-6239-2013, 2013
L. Hu, D. B. Millet, S. Y. Kim, K. C. Wells, T. J. Griffis, E. V. Fischer, D. Helmig, J. Hueber, and A. J. Curtis
Atmos. Chem. Phys., 13, 3379–3392, https://doi.org/10.5194/acp-13-3379-2013, https://doi.org/10.5194/acp-13-3379-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Large simulated future changes in the nitrate radical under the CMIP6 SSP scenarios: implications for oxidation chemistry
Impact of HO2 aerosol uptake on radical levels and O3 production during summertime in Beijing
Source attribution of near-surface ozone trends in the United States during 1995–2019
Exploring the drivers of tropospheric hydroxyl radical trends in the Geophysical Fluid Dynamics Laboratory AM4.1 atmospheric chemistry–climate model
Impacts of land cover changes on biogenic emission and its contribution to ozone and secondary organic aerosol in China
High-resolution regional emission inventory contributes to the evaluation of policy effectiveness: a case study in Jiangsu Province, China
Why is ozone in South Korea and the Seoul metropolitan area so high and increasing?
Vehicular ammonia emissions: an underappreciated emission source in densely populated areas
Improving ozone simulations in Asia via multisource data assimilation: results from an observing system simulation experiment with GEMS geostationary satellite observations
A three-dimensional simulation and process analysis of tropospheric ozone depletion events (ODEs) during the springtime in the Arctic using CMAQ (Community Multiscale Air Quality Modeling System)
A high-resolution satellite-based map of global methane emissions reveals missing wetland, fossil fuel, and monsoon sources
Global impact of the COVID-19 lockdown on surface concentration and health risk of atmospheric benzene
Variable effects of spatial resolution on modeling of nitrogen oxides
Tropospheric NO2 vertical profiles over South Korea and their relation to oxidant chemistry: implications for geostationary satellite retrievals and the observation of NO2 diurnal variation from space
Potential impact of shipping on air pollution in the Mediterranean region – a multimodel evaluation: comparison of photooxidants NO2 and O3
Summertime ozone pollution in China affected by stratospheric quasi-biennial oscillation
Declining, seasonal-varying emissions of sulfur hexafluoride from the United States
Atmospheric CO2 inversion reveals the Amazon as a minor carbon source caused by fire emissions, with forest uptake offsetting about half of these emissions
Nitrogen oxides in the free troposphere: implications for tropospheric oxidants and the interpretation of satellite NO2 measurements
Climate-driven deterioration of future ozone pollution in Asia predicted by machine learning with multi-source data
Reconciling the bottom-up and top-down estimates of the methane chemical sink using multiple observations
Arctic tropospheric ozone: assessment of current knowledge and model performance
Estimating Methane Emissions in the Arctic nations using surface observations from 2008 to 2019
Chloride (HCl ∕ Cl−) dominates inorganic aerosol formation from ammonia in the Indo-Gangetic Plain during winter: modeling and comparison with observations
Inferring and evaluating satellite-based constraints on NOx emissions estimates in air quality simulations
How do Cl concentrations matter for the simulation of CH4 and δ13C(CH4) and estimation of the CH4 budget through atmospheric inversions?
Quantification of Oil and Gas Methane Emissions in the Delaware and Marcellus Basins Using a Network of Continuous Tower-Based Measurements
Cluster-based characterization of multi-dimensional tropospheric ozone variability in coastal regions: an analysis of lidar measurements and model results
Examining the implications of photochemical indicators for O3–NOx–VOC sensitivity and control strategies: a case study in the Yangtze River Delta (YRD), China
Evaluation of isoprene nitrate chemistry in detailed chemical mechanisms
Sixteen years of MOPITT satellite data strongly constrain Amazon CO fire emissions
Comparison of model and ground observations finds snowpack and blowing snow aerosols both contribute to Arctic tropospheric reactive bromine
Continuous weekly monitoring of methane emissions from the Permian Basin by inversion of TROPOMI satellite observations
Background nitrogen dioxide (NO2) over the United States and its implications for satellite observations and trends: effects of nitrate photolysis, aircraft, and open fires
Assimilation of S5P/TROPOMI carbon monoxide data with the global CAMS near-real-time system
COVID-19 lockdown emission reductions have the potential to explain over half of the coincident increase in global atmospheric methane
Transport patterns of global aviation NOx and their short-term O3 radiative forcing – a machine learning approach
Inverse modelling of Chinese NOx emissions using deep learning: integrating in situ observations with a satellite-based chemical reanalysis
Sources of surface O3 in the UK: tagging O3 within WRF-Chem
Global tropospheric ozone trends, attributions, and radiative impacts in 1995–2017: an integrated analysis using aircraft (IAGOS) observations, ozonesonde, and multi-decadal chemical model simulations
Global sensitivities of reactive N and S gas and particle concentrations and deposition to precursor emissions reductions
Ozone depletion events in the Arctic spring of 2019: a new modeling approach to bromine emissions
High-resolution inverse modelling of European CH4 emissions using the novel FLEXPART-COSMO TM5 4DVAR inverse modelling system
Four-dimensional variational assimilation for SO2 emission and its application around the COVID-19 lockdown in the spring 2020 over China
Changing ozone sensitivity in the South Coast Air Basin during the COVID-19 period
Modelling the growth of atmospheric nitrous oxide using a global hierarchical inversion
Long-term regional trends of nitrogen and sulfur deposition in the United States from 2002 to 2017
Impact of urbanization on gas-phase pollutant concentrations: a regional-scale, model-based analysis of the contributing factors
Correcting ozone biases in a global chemistry–climate model: implications for future ozone
Evaluating the contribution of the unexplored photochemistry of aldehydes on the tropospheric levels of molecular hydrogen (H2)
Scott Archer-Nicholls, Rachel Allen, Nathan L. Abraham, Paul T. Griffiths, and Alex T. Archibald
Atmos. Chem. Phys., 23, 5801–5813, https://doi.org/10.5194/acp-23-5801-2023, https://doi.org/10.5194/acp-23-5801-2023, 2023
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The nitrate radical is a major oxidant at nighttime, but much less is known about it than about the other oxidants ozone and OH. We use Earth system model calculations to show how the nitrate radical has changed in abundance from 1850–2014 and to 2100 under a range of different climate and emission scenarios. Depending on the emissions and climate scenario, significant increases are projected with implications for the oxidation of volatile organic compounds and the formation of fine aerosol.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
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The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Pengwei Li, Yang Yang, Hailong Wang, Su Li, Ke Li, Pinya Wang, Baojie Li, and Hong Liao
Atmos. Chem. Phys., 23, 5403–5417, https://doi.org/10.5194/acp-23-5403-2023, https://doi.org/10.5194/acp-23-5403-2023, 2023
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We use a novel technique that can attribute O3 to precursors to investigate O3 changes in the United States during 1995–2019. We found that the US domestic energy and surface transportation emission reductions are primarily responsible for the O3 decrease in summer. In winter, factors such as nitrogen oxide emission reduction in the context of its inhibition of ozone production, increased aviation and shipping activities, and large-scale circulation changes contribute to the O3 increases.
Glen Chua, Vaishali Naik, and Larry Wayne Horowitz
Atmos. Chem. Phys., 23, 4955–4975, https://doi.org/10.5194/acp-23-4955-2023, https://doi.org/10.5194/acp-23-4955-2023, 2023
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The hydroxyl radical (OH) is an atmospheric
detergent, removing air pollutants and greenhouse gases like methane from the atmosphere. Thus, understanding how it is changing and responding to its various drivers is important for air quality and climate. We found that OH has increased by about 5 % globally from 1980 to 2014 in our model, mostly driven by increasing nitrogen oxide (NOx) emissions. This suggests potential climate tradeoffs from air quality policies solely targeting NOx emissions.
Jinlong Ma, Shengqiang Zhu, Siyu Wang, Peng Wang, Jianmin Chen, and Hongliang Zhang
Atmos. Chem. Phys., 23, 4311–4325, https://doi.org/10.5194/acp-23-4311-2023, https://doi.org/10.5194/acp-23-4311-2023, 2023
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An updated version of the CMAQ model with biogenic volatile organic compound (BVOC) emissions from MEGAN was applied to study the impacts of different land cover inputs on O3 and secondary organic aerosol (SOA) in China. The estimated BVOC emissions ranged from 25.42 to 37.39 Tg using different leaf area index (LAI) and land cover (LC) inputs. Those differences further induced differences of 4.8–6.9 ppb in O3 concentrations and differences of 5.3–8.4 µg m−3 in SOA concentrations in China.
Chen Gu, Lei Zhang, Zidie Xu, Sijia Xia, Yutong Wang, Li Li, Zeren Wang, Qiuyue Zhao, Hanying Wang, and Yu Zhao
Atmos. Chem. Phys., 23, 4247–4269, https://doi.org/10.5194/acp-23-4247-2023, https://doi.org/10.5194/acp-23-4247-2023, 2023
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We demonstrated the development of a high-resolution emission inventory and its application to evaluate the effectiveness of emission control actions, by incorporating the improved methodology, the best available data, and air quality modeling. We show that substantial efforts for emission controls indeed played an important role in air quality improvement even with worsened meteorological conditions and that the contributions of individual measures to emission reduction were greatly changing.
Nadia K. Colombi, Daniel J. Jacob, Laura Hyesung Yang, Shixian Zhai, Viral Shah, Stuart K. Grange, Robert M. Yantosca, Soontae Kim, and Hong Liao
Atmos. Chem. Phys., 23, 4031–4044, https://doi.org/10.5194/acp-23-4031-2023, https://doi.org/10.5194/acp-23-4031-2023, 2023
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Surface ozone, detrimental to human and ecosystem health, is very high and increasing in South Korea. Using a global model of the atmosphere, we found that emissions from South Korea and China contribute equally to the high ozone observed. We found that in the absence of all anthropogenic emissions over East Asia, ozone is still very high, implying that the air quality standard in South Korea is not practically achievable unless this background external to East Asia can be decreased.
Yifan Wen, Shaojun Zhang, Ye Wu, and Jiming Hao
Atmos. Chem. Phys., 23, 3819–3828, https://doi.org/10.5194/acp-23-3819-2023, https://doi.org/10.5194/acp-23-3819-2023, 2023
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This study established a high-resolution vehicular NH3 emission inventory for mainland China to quantify the absolute value and relative importance of on-road NH3 emissions for different regions, seasons and population densities. Our results indicate that the significant role of on-road NH3 emissions in populated urban areas may have been underappreciated, suggesting the control of vehicular NH3 emission can be a feasible and cost-effective way of mitigating haze pollution in urban areas.
Lei Shu, Lei Zhu, Juseon Bak, Peter Zoogman, Han Han, Song Liu, Xicheng Li, Shuai Sun, Juan Li, Yuyang Chen, Dongchuan Pu, Xiaoxing Zuo, Weitao Fu, Xin Yang, and Tzung-May Fu
Atmos. Chem. Phys., 23, 3731–3748, https://doi.org/10.5194/acp-23-3731-2023, https://doi.org/10.5194/acp-23-3731-2023, 2023
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We quantify the benefit of multisource observations (GEMS, LEO satellite, and surface) on ozone simulations in Asia. Data assimilation improves the monitoring of exceedance, spatial pattern, and diurnal variation of surface ozone, with the regional mean bias reduced from −2.1 to −0.2 ppbv. Data assimilation also better represents ozone vertical distributions in the middle to upper troposphere at low latitudes. Our results offer a valuable reference for future ozone simulations.
Le Cao, Simeng Li, Yicheng Gu, and Yuhan Luo
Atmos. Chem. Phys., 23, 3363–3382, https://doi.org/10.5194/acp-23-3363-2023, https://doi.org/10.5194/acp-23-3363-2023, 2023
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We performed a 3-D mesoscale model study on ozone depletion events (ODEs) occurring in the spring of 2019 at Barrow using an air quality model, CMAQ. Many ODEs observed at Barrow were captured by the model, and the contribution from each physical or chemical process to ozone and bromine species during ODEs was quantitatively evaluated. We found the ODEs at Barrow to be strongly influenced by horizontal transport. In contrast, over the sea, local chemistry significantly reduced the surface ozone.
Xueying Yu, Dylan B. Millet, Daven K. Henze, Alexander J. Turner, Alba Lorente Delgado, A. Anthony Bloom, and Jianxiong Sheng
Atmos. Chem. Phys., 23, 3325–3346, https://doi.org/10.5194/acp-23-3325-2023, https://doi.org/10.5194/acp-23-3325-2023, 2023
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We combine satellite measurements with a novel downscaling method to map global methane emissions at 0.1°×0.1° resolution. These fine-scale emission estimates reveal unreported emission hotspots and shed light on the roles of agriculture, wetlands, and fossil fuels for regional methane budgets. The satellite-derived emissions point in particular to missing fossil fuel emissions in the Middle East and to a large emission underestimate in South Asia that appears to be tied to monsoon rainfall.
Chaohao Ling, Lulu Cui, and Rui Li
Atmos. Chem. Phys., 23, 3311–3324, https://doi.org/10.5194/acp-23-3311-2023, https://doi.org/10.5194/acp-23-3311-2023, 2023
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An ensemble machine-learning model coupled with chemical transport models (CTMs) was applied to assess the impact of COVID-19 on ambient benzene. The change ratio of the deweathered benzene concentration from the pre-lockdown to lockdown period was in the order of India (−23.6 %) > Europe (−21.9 %) > the United States (−16.2 %) > China (−15.6 %), which might be associated with local serious benzene pollution and substantial emission reduction in the industrial and transportation sectors.
Chi Li, Randall V. Martin, Ronald C. Cohen, Liam Bindle, Dandan Zhang, Deepangsu Chatterjee, Hongjian Weng, and Jintai Lin
Atmos. Chem. Phys., 23, 3031–3049, https://doi.org/10.5194/acp-23-3031-2023, https://doi.org/10.5194/acp-23-3031-2023, 2023
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Models are essential to diagnose the significant effects of nitrogen oxides (NOx) on air pollution. We use an air quality model to illustrate the variability of NOx resolution-dependent simulation biases; how these biases depend on specific chemical environments, driving mechanisms, and vertical variabilities; and how these biases affect the interpretation of satellite observations. High-resolution simulations are thus critical to accurately interpret NOx and its relevance to air quality.
Laura Hyesung Yang, Daniel J. Jacob, Nadia K. Colombi, Shixian Zhai, Kelvin H. Bates, Viral Shah, Ellie Beaudry, Robert M. Yantosca, Haipeng Lin, Jared F. Brewer, Heesung Chong, Katherine R. Travis, James H. Crawford, Lok N. Lamsal, Ja-Ho Koo, and Jhoon Kim
Atmos. Chem. Phys., 23, 2465–2481, https://doi.org/10.5194/acp-23-2465-2023, https://doi.org/10.5194/acp-23-2465-2023, 2023
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A geostationary satellite can now provide hourly NO2 vertical columns, and obtaining the NO2 vertical columns from space relies on NO2 vertical distribution from the chemical transport model (CTM). In this work, we update the CTM to better represent the chemistry environment so that the CTM can accurately provide NO2 vertical distribution. We also find that the changes in NO2 vertical distribution driven by a change in mixing depth play an important role in the NO2 column's diurnal variation.
Lea Fink, Matthias Karl, Volker Matthias, Sonia Oppo, Richard Kranenburg, Jeroen Kuenen, Jana Moldanova, Sara Jutterström, Jukka-Pekka Jalkanen, and Elisa Majamäki
Atmos. Chem. Phys., 23, 1825–1862, https://doi.org/10.5194/acp-23-1825-2023, https://doi.org/10.5194/acp-23-1825-2023, 2023
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Potential ship impact on air pollution in the Mediterranean Sea was simulated with five chemistry transport models. An evaluation of the results for NO2 and O3 air concentrations and dry deposition is presented. Emission data, modeled year and domain were the same. Model run outputs were compared to measurements from background stations. We focused on comparing model outputs regarding the concentration of regulatory pollutants and the relative ship impact on total air pollution concentrations.
Mengyun Li, Yang Yang, Hailong Wang, Huimin Li, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 23, 1533–1544, https://doi.org/10.5194/acp-23-1533-2023, https://doi.org/10.5194/acp-23-1533-2023, 2023
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Using the GEOS-Chem model, the impact of the quasi-biennial oscillation (QBO) on summertime tropospheric O3 in China is investigated. In the warm phases of sea surface temperature anomalies over the eastern tropical Pacific, the QBO has a significant positive correlation with near-surface O3 concentrations over central China. The QBO impacts on O3 pollution in China are mainly a result of changing vertical transport of O3.
Lei Hu, Deborah Ottinger, Stephanie Bogle, Stephen A. Montzka, Philip L. DeCola, Ed Dlugokencky, Arlyn Andrews, Kirk Thoning, Colm Sweeney, Geoff Dutton, Lauren Aepli, and Andrew Crotwell
Atmos. Chem. Phys., 23, 1437–1448, https://doi.org/10.5194/acp-23-1437-2023, https://doi.org/10.5194/acp-23-1437-2023, 2023
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Effective mitigation of greenhouse gas (GHG) emissions relies on an accurate understanding of emissions. Here we demonstrate the added value of using inventory- and atmosphere-based approaches for estimating US emissions of SF6, the most potent GHG known. The results suggest a large decline in US SF6 emissions, shed light on the possible processes causing the differences between the independent estimates, and identify opportunities for substantial additional emission reductions.
Luana S. Basso, Chris Wilson, Martyn P. Chipperfield, Graciela Tejada, Henrique L. G. Cassol, Egídio Arai, Mathew Williams, T. Luke Smallman, Wouter Peters, Stijn Naus, John B. Miller, and Manuel Gloor
EGUsphere, https://doi.org/10.5194/egusphere-2023-19, https://doi.org/10.5194/egusphere-2023-19, 2023
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Tropical forests like Amazon are historically an important carbon sink, helping to mitigate global climate change. Using an atmospheric model and regional and global atmospheric CO2 observations, we quantified Amazonian carbon emissions between 2010 and 2018. We estimated that Amazon acted as a small carbon source to the atmosphere, mostly due to fire emissions. However, the forest uptake compensated 50 % of these fire emissions. We do not find an increasing time trend of carbon emissions.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
Huimin Li, Yang Yang, Jianbing Jin, Hailong Wang, Ke Li, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 23, 1131–1145, https://doi.org/10.5194/acp-23-1131-2023, https://doi.org/10.5194/acp-23-1131-2023, 2023
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Future climate change will aggravate ozone pollution in Asia, especially in high-forcing scenarios. Ozone pollution in China will expand from North China to South China and extend into the cold season in a warmer future. The emphasis of this work is to quantify the impacts of future climate change on O3 pollution in Asia, which is of great significance for future O3 pollution mitigation strategies.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, and Bo Zheng
Atmos. Chem. Phys., 23, 789–807, https://doi.org/10.5194/acp-23-789-2023, https://doi.org/10.5194/acp-23-789-2023, 2023
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The large uncertainties in OH simulated by atmospheric chemistry models hinder accurate estimates of CH4 chemical loss through the bottom-up method. This study presents a new approach based on OH precursor observations and a chemical box model to improve the tropospheric OH distributions simulated by atmospheric chemistry models. Through this approach, both the global OH burden and the corresponding methane chemical loss reach consistency with the top-down method based on MCF inversions.
Cynthia H. Whaley, Kathy S. Law, Jens Liengaard Hjorth, Henrik Skov, Stephen R. Arnold, Joakim Langner, Jakob Boyd Pernov, Garance Bergeron, Ilann Bourgeois, Jesper H. Christensen, Rong-You Chien, Makoto Deushi, Xinyi Dong, Peter Effertz, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Greg Huey, Ulas Im, Rigel Kivi, Louis Marelle, Tatsuo Onishi, Naga Oshima, Irina Petropavlovskikh, Jeff Peischl, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Tom Ryerson, Ragnhild Skeie, Sverre Solberg, Manu A. Thomas, Chelsea Thompson, Kostas Tsigaridis, Svetlana Tsyro, Steven T. Turnock, Knut von Salzen, and David W. Tarasick
Atmos. Chem. Phys., 23, 637–661, https://doi.org/10.5194/acp-23-637-2023, https://doi.org/10.5194/acp-23-637-2023, 2023
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This study summarizes recent research on ozone in the Arctic, a sensitive and rapidly warming region. We find that the seasonal cycles of near-surface atmospheric ozone are variable depending on whether they are near the coast, inland, or at high altitude. Several global model simulations were evaluated, and we found that because models lack some of the ozone chemistry that is important for the coastal Arctic locations, they do not accurately simulate ozone there.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, Joël Thanwerdas, Adrien Martinez, Jean-Daniel Paris, Tochinobu Machida, Motoki Sasakawa, Douglas E. J. Worthy, Xin Lan, Rona L. Thompson, Espen Sollum, and Michael Arshinov
EGUsphere, https://doi.org/10.5194/egusphere-2022-1257, https://doi.org/10.5194/egusphere-2022-1257, 2023
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Here, an inverse modeling approach is applied to estimate CH4 sources and sinks in the Arctic from 2008 to 2019. We study the magnitude, seasonal patterns and trends from different sources during recent years. We also assess how the current observation network helps constraining fluxes. We find that constraints are only significant for North America and in a lesser extent West Siberia, where the observation network is relatively dense. We find not clear trend over the period of inversion.
Pooja V. Pawar, Sachin D. Ghude, Gaurav Govardhan, Prodip Acharja, Rachana Kulkarni, Rajesh Kumar, Baerbel Sinha, Vinayak Sinha, Chinmay Jena, Preeti Gunwani, Tapan Kumar Adhya, Eiko Nemitz, and Mark A. Sutton
Atmos. Chem. Phys., 23, 41–59, https://doi.org/10.5194/acp-23-41-2023, https://doi.org/10.5194/acp-23-41-2023, 2023
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In this study, for the first time in South Asia we compare simulated ammonia, ammonium, and total ammonia using the WRF-Chem model and MARGA measurements during winter in the Indo-Gangetic Plain region. Since observations show HCl promotes the fraction of high chlorides in Delhi, we added HCl / Cl emissions to the model. We conducted three sensitivity experiments with changes in HCl emissions, and improvements are reported in accurately simulating ammonia, ammonium, and total ammonia.
James D. East, Barron H. Henderson, Sergey L. Napelenok, Shannon N. Koplitz, Golam Sarwar, Robert Gilliam, Allen Lenzen, Daniel Q. Tong, R. Bradley Pierce, and Fernando Garcia-Menendez
Atmos. Chem. Phys., 22, 15981–16001, https://doi.org/10.5194/acp-22-15981-2022, https://doi.org/10.5194/acp-22-15981-2022, 2022
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We present a framework that uses a computer model of air quality, along with air pollution data from satellite instruments, to estimate emissions of nitrogen oxides (NOx) across the Northern Hemisphere. The framework, which advances current methods to infer emissions from satellite observations, provides observationally constrained NOx estimates, including in regions of the world where emissions are highly uncertain, and can improve simulations of air pollutants relevant for health and policy.
Joël Thanwerdas, Marielle Saunois, Isabelle Pison, Didier Hauglustaine, Antoine Berchet, Bianca Baier, Colm Sweeney, and Philippe Bousquet
Atmos. Chem. Phys., 22, 15489–15508, https://doi.org/10.5194/acp-22-15489-2022, https://doi.org/10.5194/acp-22-15489-2022, 2022
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Atmospheric methane (CH4) concentrations have been rising since 2007, resulting from an imbalance between CH4 sources and sinks. The CH4 budget is generally estimated through top-down approaches using CH4 and δ13C(CH4) observations as constraints. The oxidation by chlorine (Cl) contributes little to the total oxidation of CH4 but strongly influences δ13C(CH4). Here, we compare multiple recent Cl fields and quantify the influence of Cl concentrations on CH4, δ13C(CH4), and CH4 budget estimates.
Zachary Barkley, Kenneth Davis, Natasha Miles, Scott Richardson, Aijun Deng, Benjamin Hmiel, David Lyon, and Thomas Lauvaux
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-709, https://doi.org/10.5194/acp-2022-709, 2022
Revised manuscript accepted for ACP
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Using methane monitoring instruments attached to towers, we measure methane concentrations and quantify methane emissions coming from the Marcellus and Permian oil & gas basins. In the Marcellus, emissions were 3 times higher than the state inventory across the entire monitoring period. In the Permian, we see a sharp decline in emissions aligning with the onset of the COVID-19 pandemic. Tower observational networks can be utilized in other basins for long-term monitoring of emissions.
Claudia Bernier, Yuxuan Wang, Guillaume Gronoff, Timothy Berkoff, K. Emma Knowland, John T. Sullivan, Ruben Delgado, Vanessa Caicedo, and Brian Carroll
Atmos. Chem. Phys., 22, 15313–15331, https://doi.org/10.5194/acp-22-15313-2022, https://doi.org/10.5194/acp-22-15313-2022, 2022
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Coastal regions are susceptible to variable and high ozone which is difficult to simulate. We developed a method to characterize large datasets of multi-dimensional measurements from lidar instruments taken in coastal regions. Using the clustered ozone groups, we evaluated model performance in simulating the coastal ozone variability vertically and diurnally. The approach allowed us to pinpoint areas where the models succeed in simulating coastal ozone and areas where there are still gaps.
Xun Li, Momei Qin, Lin Li, Kangjia Gong, Huizhong Shen, Jingyi Li, and Jianlin Hu
Atmos. Chem. Phys., 22, 14799–14811, https://doi.org/10.5194/acp-22-14799-2022, https://doi.org/10.5194/acp-22-14799-2022, 2022
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Photochemical indicators have been widely used to predict O3–NOx–VOC sensitivity with given thresholds. Here we assessed the effectiveness of four indicators with a case study in the Yangtze River Delta, China. The overall performance was good, while some indicators showed inconsistencies with the O3 isopleths. The methodology used to determine the thresholds may produce uncertainties. These results would improve our understanding of the use of photochemical indicators in policy implications.
Alfred W. Mayhew, Ben H. Lee, Joel A. Thornton, Thomas J. Bannan, James Brean, James R. Hopkins, James D. Lee, Beth S. Nelson, Carl Percival, Andrew R. Rickard, Marvin D. Shaw, Peter M. Edwards, and Jaqueline F. Hamilton
Atmos. Chem. Phys., 22, 14783–14798, https://doi.org/10.5194/acp-22-14783-2022, https://doi.org/10.5194/acp-22-14783-2022, 2022
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Isoprene nitrates are chemical species commonly found in the atmosphere that are important for their impacts on air quality and climate. This paper compares 3 different representations of the chemistry of isoprene nitrates in computational models highlighting cases where the choice of chemistry included has significant impacts on the concentration and composition of the modelled nitrates. Calibration of mass spectrometers is also shown to be an important factor when analysing isoprene nitrates.
Stijn Naus, Lucas G. Domingues, Maarten Krol, Ingrid T. Luijkx, Luciana V. Gatti, John B. Miller, Emanuel Gloor, Sourish Basu, Caio Correia, Gerbrand Koren, Helen M. Worden, Johannes Flemming, Gabrielle Pétron, and Wouter Peters
Atmos. Chem. Phys., 22, 14735–14750, https://doi.org/10.5194/acp-22-14735-2022, https://doi.org/10.5194/acp-22-14735-2022, 2022
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We assimilate MOPITT CO satellite data in the TM5-4D-Var inverse modelling framework to estimate Amazon fire CO emissions for 2003–2018. We show that fire emissions have decreased over the analysis period, coincident with a decrease in deforestation rates. However, interannual variations in fire emissions are large, and they correlate strongly with soil moisture. Our results reveal an important role for robust, top-down fire CO emissions in quantifying and attributing Amazon fire intensity.
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.
Daniel J. Varon, Daniel J. Jacob, Benjamin Hmiel, Ritesh Gautam, David R. Lyon, Mark Omara, Melissa Sulprizio, Lu Shen, Drew Pendergrass, Hannah Nesser, Zhen Qu, Zachary R. Barkley, Natasha L. Miles, Scott J. Richardson, Kenneth J. Davis, Sudhanshu Pandey, Xiao Lu, Alba Lorente, Tobias Borsdorff, Joannes D. Maasakkers, and Ilse Aben
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-749, https://doi.org/10.5194/acp-2022-749, 2022
Revised manuscript accepted for ACP
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Over 100 countries plan to cut their methane emissions by 30 % this decade under the 2021 Global Methane Pledge. The oil and gas industry is a high priority for emission reductions, but the temporal variability of oil/gas methane emissions is poorly understood. We used satellite observations to quantify weekly oil/gas methane emissions from the U.S. Permian Basin. We find that Permian emissions are highly variable and stronger than previously known, with diverse economic and activity drivers.
Ruijun Dang, Daniel J. Jacob, Viral Shah, Sebastian D. Eastham, Thibaud M. Fritz, Loretta J. Mickley, Tianjia Liu, Yi Wang, and Jun Wang
EGUsphere, https://doi.org/10.5194/egusphere-2022-1198, https://doi.org/10.5194/egusphere-2022-1198, 2022
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Model underestimate of the background NO2 is largely corrected by considering aerosol nitrate photolysis. Increase in aircraft emissions not only increases the background NO2, but also affects the satellite retrieval by altering the NO2 vertical profile. Increase in wildfire emissions contributes to the flattening of post-2009 OMI NO2 trends in the western US. Our work shows the importance of properly accounting for the free tropospheric background in interpreting satellite NO2 observations.
Antje Inness, Ilse Aben, Melanie Ades, Tobias Borsdorff, Johannes Flemming, Luke Jones, Jochen Landgraf, Bavo Langerock, Philippe Nedelec, Mark Parrington, and Roberto Ribas
Atmos. Chem. Phys., 22, 14355–14376, https://doi.org/10.5194/acp-22-14355-2022, https://doi.org/10.5194/acp-22-14355-2022, 2022
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The Copernicus Atmosphere Monitoring Service (CAMS) provides daily global air quality forecasts to users worldwide. One of the species of interest is carbon monoxide (CO), an important trace gas in the atmosphere with anthropogenic and natural sources, produced by incomplete combustion, for example, by wildfires. This paper looks at how well CAMS can model CO in the atmosphere and shows that the fields can be improved when blending CO data from the TROPOMI instrument with the CAMS model.
David S. Stevenson, Richard G. Derwent, Oliver Wild, and William J. Collins
Atmos. Chem. Phys., 22, 14243–14252, https://doi.org/10.5194/acp-22-14243-2022, https://doi.org/10.5194/acp-22-14243-2022, 2022
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Atmospheric methane’s growth rate rose by 50 % in 2020 relative to 2019. Lower nitrogen oxide (NOx) emissions tend to increase methane’s atmospheric residence time; lower carbon monoxide (CO) and non-methane volatile organic compound (NMVOC) emissions decrease its lifetime. Combining model sensitivities with emission changes, we find that COVID-19 lockdown emission reductions can explain over half the observed increases in methane in 2020.
Jin Maruhashi, Volker Grewe, Christine Frömming, Patrick Jöckel, and Irene C. Dedoussi
Atmos. Chem. Phys., 22, 14253–14282, https://doi.org/10.5194/acp-22-14253-2022, https://doi.org/10.5194/acp-22-14253-2022, 2022
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Aviation NOx emissions lead to the formation of ozone in the atmosphere in the short term, which has a climate warming effect. This study uses global-scale simulations to characterize the transport patterns between NOx emissions at an altitude of ~ 10.4 km and the resulting ozone. Results show a strong spatial and temporal dependence of NOx in disturbing atmospheric O3 concentrations, with the location that is most impacted in terms of warming not necessarily coinciding with the emission region.
Tai-Long He, Dylan B. A. Jones, Kazuyuki Miyazaki, Kevin W. Bowman, Zhe Jiang, Xiaokang Chen, Rui Li, Yuxiang Zhang, and Kunna Li
Atmos. Chem. Phys., 22, 14059–14074, https://doi.org/10.5194/acp-22-14059-2022, https://doi.org/10.5194/acp-22-14059-2022, 2022
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We use a deep-learning (DL) model to estimate Chinese NOx emissions by combining satellite analysis and in situ measurements. Our results are consistent with conventional analyses of Chinese NOx emissions. Comparison with mobility data shows that the DL model has a better capability to capture changes in NOx. We analyse Chinese NOx emissions during the COVID-19 pandemic lockdown period. Our results illustrate the potential use of DL as a complementary tool for conventional air quality studies.
Johana Romero-Alvarez, Aurelia Lupaşcu, Douglas Lowe, Alba Badia, Scott Archer-Nicholls, Steve Dorling, Claire E. Reeves, and Tim Butler
Atmos. Chem. Phys., 22, 13797–13815, https://doi.org/10.5194/acp-22-13797-2022, https://doi.org/10.5194/acp-22-13797-2022, 2022
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As ozone can be transported across countries, efficient air quality management and regulatory policies rely on the assessment of local ozone production vs. transport. In our study, we investigate the origin of surface ozone in the UK and the contribution of the different source regions to regulatory ozone metrics. It is shown that emission controls would be necessary over western Europe to improve health-related metrics and over larger areas to reduce impacts on ecosystems.
Haolin Wang, Xiao Lu, Daniel J. Jacob, Owen R. Cooper, Kai-Lan Chang, Ke Li, Meng Gao, Yiming Liu, Bosi Sheng, Kai Wu, Tongwen Wu, Jie Zhang, Bastien Sauvage, Philippe Nédélec, Romain Blot, and Shaojia Fan
Atmos. Chem. Phys., 22, 13753–13782, https://doi.org/10.5194/acp-22-13753-2022, https://doi.org/10.5194/acp-22-13753-2022, 2022
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We report significant global tropospheric ozone increases in 1995–2017 based on extensive aircraft and ozonesonde observations. Using GEOS-Chem (Goddard Earth Observing System chemistry model) multi-decadal global simulations, we find that changes in global anthropogenic emissions, in particular the rapid increases in aircraft emissions, contribute significantly to the increases in tropospheric ozone and resulting radiative impact.
Yao Ge, Massimo Vieno, David S. Stevenson, Peter Wind, and Mathew R. Heal
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-657, https://doi.org/10.5194/acp-2022-657, 2022
Revised manuscript accepted for ACP
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The reduction of fine particles (PM2.5) and reactive N (Nr) and S (Sr) is a key air quality objective. The sensitivity of global Nr, Sr, and PM2.5 to reductions in precursors emissions is investigated using the EMEP MSC-W atmospheric chemistry transport model. This study reveals that the individual emissions reduction has multiple and geographically-varying co-benefits and small disbenefits on different species, demonstrating the importance of prioritising regional emissions controls.
Maximilian Herrmann, Moritz Schöne, Christian Borger, Simon Warnach, Thomas Wagner, Ulrich Platt, and Eva Gutheil
Atmos. Chem. Phys., 22, 13495–13526, https://doi.org/10.5194/acp-22-13495-2022, https://doi.org/10.5194/acp-22-13495-2022, 2022
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Ozone depletion events (ODEs) are a common occurrence in the boundary layer during Arctic spring. Ozone is depleted by bromine species in an autocatalytic reaction cycle. Previous modeling studies assumed an infinite bromine source at the ground. An alternative emission scheme is presented in which a finite amount of bromide in the snow is tracked over time. The Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) is used to study ODEs in the Arctic from February to May 2019.
Peter Bergamaschi, Arjo Segers, Dominik Brunner, Jean-Matthieu Haussaire, Stephan Henne, Michel Ramonet, Tim Arnold, Tobias Biermann, Huilin Chen, Sebastien Conil, Marc Delmotte, Grant Forster, Arnoud Frumau, Dagmar Kubistin, Xin Lan, Markus Leuenberger, Matthias Lindauer, Morgan Lopez, Giovanni Manca, Jennifer Müller-Williams, Simon O'Doherty, Bert Scheeren, Martin Steinbacher, Pamela Trisolino, Gabriela Vítková, and Camille Yver Kwok
Atmos. Chem. Phys., 22, 13243–13268, https://doi.org/10.5194/acp-22-13243-2022, https://doi.org/10.5194/acp-22-13243-2022, 2022
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We present a novel high-resolution inverse modelling system, "FLEXVAR", and its application for the inverse modelling of European CH4 emissions in 2018. The new system combines a high spatial resolution of 7 km x 7 km with a variational data assimilation technique, which allows CH4 emissions to be optimized from individual model grid cells. The high resolution allows the observations to be better reproduced, while the derived emissions show overall good consistency with two existing models.
Yiwen Hu, Zengliang Zang, Xiaoyan Ma, Yi Li, Yanfei Liang, Wei You, Xiaobin Pan, and Zhijin Li
Atmos. Chem. Phys., 22, 13183–13200, https://doi.org/10.5194/acp-22-13183-2022, https://doi.org/10.5194/acp-22-13183-2022, 2022
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This study developed a four-dimensional variational assimilation (4DVAR) system based on WRF–Chem to optimise SO2 emissions. The 4DVAR system was applied to obtain the SO2 emissions during the early period of the COVID-19 pandemic over China. The results showed that the 4DVAR system effectively optimised emissions to describe the actual changes in SO2 emissions related to the COVID lockdown, and it can thus be used to improve the accuracy of forecasts.
Jason R. Schroeder, Chenxia Cai, Jin Xu, David Ridley, Jin Lu, Nancy Bui, Fang Yan, and Jeremy Avise
Atmos. Chem. Phys., 22, 12985–13000, https://doi.org/10.5194/acp-22-12985-2022, https://doi.org/10.5194/acp-22-12985-2022, 2022
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Ozone, a key component of smog, has plagued the Los Angeles (LA) region for decades. Ozone is created by complex chemical reactions that can be greatly impacted by anthropogenic emissions. This study makes use of the COVID-19 period to study the sensitivity of ozone chemistry in LA to certain anthropogenic emissions, notably from vehicles. We find that vehicular emissions of key pollutants dropped by up to 25 % during COVID-19, which caused a fundamental shift in ozone chemistry in the region.
Angharad C. Stell, Michael Bertolacci, Andrew Zammit-Mangion, Matthew Rigby, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Xin Lan, Manfredi Manizza, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, and Anita L. Ganesan
Atmos. Chem. Phys., 22, 12945–12960, https://doi.org/10.5194/acp-22-12945-2022, https://doi.org/10.5194/acp-22-12945-2022, 2022
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Nitrous oxide is a potent greenhouse gas and ozone-depleting substance, whose atmospheric abundance has risen throughout the contemporary record. In this work, we carry out the first global hierarchical Bayesian inversion to solve for nitrous oxide emissions. We derive increasing global nitrous oxide emissions over 2011–2020, which are mainly driven by emissions between 0° and 30°N, with the highest emissions recorded in 2020.
Sarah E. Benish, Jesse O. Bash, Kristen M. Foley, K. Wyat Appel, Christian Hogrefe, Robert Gilliam, and George Pouliot
Atmos. Chem. Phys., 22, 12749–12767, https://doi.org/10.5194/acp-22-12749-2022, https://doi.org/10.5194/acp-22-12749-2022, 2022
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We assess Community Multiscale Air Quality (CMAQ) model simulations of nitrogen and sulfur deposition over US climate regions to evaluate the model ability to reproduce long-term deposition trends and total deposition budgets. A measurement–model fusion technique is found to improve estimates of wet deposition. Emission controls set by the Clean Air Act successfully decreased oxidized nitrogen deposition across the US; we find increasing amounts of reduced nitrogen to the total nitrogen budget.
Peter Huszar, Jan Karlický, Lukáš Bartík, Marina Liaskoni, Alvaro Patricio Prieto Perez, and Kateřina Šindelářová
Atmos. Chem. Phys., 22, 12647–12674, https://doi.org/10.5194/acp-22-12647-2022, https://doi.org/10.5194/acp-22-12647-2022, 2022
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Urbanization turns rural land cover into artificial land cover, while due to human activities, it introduces a great quantity of emissions. We attempt to quantify the impact of urbanization on the final air pollutant levels by looking not only at these emissions, but also the way urban land cover influences meteorological conditions, how the removal of pollutants changes due to urban land cover, and how biogenic emissions from vegetation change due to less vegetation in urban areas.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Fiona M. O'Connor, and Steven T. Turnock
Atmos. Chem. Phys., 22, 12543–12557, https://doi.org/10.5194/acp-22-12543-2022, https://doi.org/10.5194/acp-22-12543-2022, 2022
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Weaknesses in process representation in chemistry–climate models lead to biases in simulating surface ozone and to uncertainty in projections of future ozone change. We develop a deep learning model to demonstrate the feasibility of ozone bias correction and show its capability in providing improved assessments of the impacts of climate and emission changes on future air quality, along with valuable information to guide future model development.
Maria Paula Pérez-Peña, Jenny A. Fisher, Dylan B. Millet, Hisashi Yashiro, Ray L. Langenfelds, Paul B. Krummel, and Scott H. Kable
Atmos. Chem. Phys., 22, 12367–12386, https://doi.org/10.5194/acp-22-12367-2022, https://doi.org/10.5194/acp-22-12367-2022, 2022
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We used two atmospheric models to test the implications of previously unexplored aldehyde photochemistry on the atmospheric levels of molecular hydrogen (H2). We showed that the new photochemistry from aldehydes produces more H2 over densely forested areas. Compared to the rest of the world, it is over these forested regions where the produced H2 is more likely to be removed. The results highlight that other processes that contribute to atmospheric H2 levels should be studied further.
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Short summary
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.
Mercury is a trace metal with adverse health effects on human and wildlife. Its unique property...
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