Articles | Volume 14, issue 3
Atmos. Chem. Phys., 14, 1463–1483, 2014
https://doi.org/10.5194/acp-14-1463-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Special issue: Firn air: archive of the recent atmosphere
Atmos. Chem. Phys., 14, 1463–1483, 2014
https://doi.org/10.5194/acp-14-1463-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
10 Feb 2014
Research article
| 10 Feb 2014
Reconstruction of Northern Hemisphere 1950–2010 atmospheric non-methane hydrocarbons
D. Helmig et al.
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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.
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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This research demonstrates a new method for determination of the chemical reactivity of volatile organic compounds that are emitted from the leaves and needles of trees. These measurements allow elucidating if and how much of these emissions and their associated reactivity are captured and quantified by currently applicable chemical analysis methods.
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.
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.
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.
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.
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.
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.
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.
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.
Shaojie Song, Hélène Angot, Noelle E. Selin, Hubert Gallée, Francesca Sprovieri, Nicola Pirrone, Detlev Helmig, Joël Savarino, Olivier Magand, and Aurélien Dommergue
Atmos. Chem. Phys., 18, 15825–15840, https://doi.org/10.5194/acp-18-15825-2018, https://doi.org/10.5194/acp-18-15825-2018, 2018
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Mercury is a trace metal with adverse health effects on human and wildlife. Its unique property makes it undergo long-range transport, and even remote Antarctica receives significant inputs. This paper presents the first model that aims to understand mercury behavior over the Antarctic Plateau. We find that mercury is quickly cycled between snow and air in the sunlit period, likely driven by bromine chemistry, and that several uncertain processes contribute to its behavior in the dark period.
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.
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.
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.
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.
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
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.
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
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
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
Bryce F. J. Kelly, Xinyi Lu, Stephen J. Harris, Bruno G. Neininger, Jorg M. Hacker, Stefan Schwietzke, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Carina van der Veen, Malika Menoud, and Thomas Röckmann
Atmos. Chem. Phys., 22, 15527–15558, https://doi.org/10.5194/acp-22-15527-2022, https://doi.org/10.5194/acp-22-15527-2022, 2022
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This study explores using the composition of methane of in-flight atmospheric air samples for greenhouse gas inventory verification. The air samples were collected above one of the largest coal seam gas production regions in the world. Adjacent to these gas fields are coal mines, Australia's largest cattle feedlot, and over 1 million grazing cattle. The results are also used to identify methane mitigation opportunities.
Andreas Forstmaier, Jia Chen, Florian Dietrich, Juan Bettinelli, Hossein Maazallahi, Carsten Schneider, Dominik Winkler, Xinxu Zhao, Taylor Jones, Carina van der Veen, Norman Wildmann, Moritz Makowski, Aydin Uzun, Friedrich Klappenbach, Hugo Denier van der Gon, Stefan Schwietzke, and Thomas Röckmann
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-710, https://doi.org/10.5194/acp-2022-710, 2022
Preprint under review for ACP
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Large cities emit greenhouse gases which contribute to global warming. In this study we measured the release of one important green house gas, methane in the Hamburg. Multiple sources that contribute to the methane emissions were located and quantified. Methane sources were found to be mainly caused by human activity, for example by the release from oil and gas refineries. Also potential natural sources have been located such as the Elbe river and lakes.
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.
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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This research demonstrates a new method for determination of the chemical reactivity of volatile organic compounds that are emitted from the leaves and needles of trees. These measurements allow elucidating if and how much of these emissions and their associated reactivity are captured and quantified by currently applicable chemical analysis methods.
Malika Menoud, Carina van der Veen, Dave Lowry, Julianne M. Fernandez, Semra Bakkaloglu, James L. France, Rebecca E. Fisher, Hossein Maazallahi, Mila Stanisavljević, Jarosław Nęcki, Katarina Vinkovic, Patryk Łakomiec, Janne Rinne, Piotr Korbeń, Martina Schmidt, Sara Defratyka, Camille Yver-Kwok, Truls Andersen, Huilin Chen, and Thomas Röckmann
Earth Syst. Sci. Data, 14, 4365–4386, https://doi.org/10.5194/essd-14-4365-2022, https://doi.org/10.5194/essd-14-4365-2022, 2022
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Emission sources of methane (CH4) can be distinguished with measurements of CH4 stable isotopes. We present new measurements of isotope signatures of various CH4 sources in Europe, mainly anthropogenic, sampled from 2017 to 2020. The present database also contains the most recent update of the global signature dataset from the literature. The dataset improves CH4 source attribution and the understanding of the global CH4 budget.
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.
Christo Buizert, Sarah Shackleton, Jeffrey P. Severinghaus, William H. G. Roberts, Alan Seltzer, Bernhard Bereiter, Kenji Kawamura, Daniel Baggenstos, Anaïs J. Orsi, Ikumi Oyabu, Benjamin Birner, Jacob D. Morgan, Edward J. Brook, David M. Etheridge, David Thornton, Nancy Bertler, Rebecca L. Pyne, Robert Mulvaney, Ellen Mosley-Thompson, Peter D. Neff, and Vasilii V. Petrenko
Clim. Past Discuss., https://doi.org/10.5194/cp-2022-65, https://doi.org/10.5194/cp-2022-65, 2022
Revised manuscript accepted for CP
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It is unclear how different components of the global atmospheric circulation, such as the El Niño effect, respond to large-scale climate change. We present a new ice core gas proxy, called Krypton-86 excess, that reflects past storminess in Antarctica. We present data from 11 ice cores that suggest the new proxy works. We present a reconstruction of changes in West Antarctic storminess over the last 24,000 years, and suggest these are caused by north-south movement of the tropical rain belt.
David Robert Worton, Sergi Moreno, Kieran O'Daly, and Rupert Holzinger
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2022-243, https://doi.org/10.5194/amt-2022-243, 2022
Preprint under review for AMT
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Proton transfer reaction mass spectrometry is widely used in the environmental, health and food and beverage sectors. As a result, there is a need for accurate and comparable measurements. In this work we have developed a 20 component gravimetrically prepared primary reference material (gas standard in a high pressure cylinder) to enable quantitative and comparable measurements. The accuracy of all components was better than 3–10 % with stabilities of more than 1–2 years.
Hossein Maazallahi, Antonio Delre, Charlotte Scheutz, Anders M. Fredenslund, Stefan Schwietzke, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2022-134, https://doi.org/10.5194/amt-2022-134, 2022
Revised manuscript under review for AMT
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Measurement methods are increasingly deployed to verify reported methane emissions of gas leaks. This study describes unique advantages and limitations of three methods. Two methods are rapidly deployed, but uncertainties and biases exist for some leak locations. In contrast, the suction method could accurately determine leak rates in principle. However, this method, which provides data for the German emission inventory, creates an overall low-bias in our study due to non-random site selection.
Xavier Faïn, Rachael H. Rhodes, Philip Place, Vasilii V. Petrenko, Kévin Fourteau, Nathan Chellman, Edward Crosier, Joseph R. McConnell, Edward J. Brook, Thomas Blunier, Michel Legrand, and Jérôme Chappellaz
Clim. Past, 18, 631–647, https://doi.org/10.5194/cp-18-631-2022, https://doi.org/10.5194/cp-18-631-2022, 2022
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Carbon monoxide (CO) is a regulated pollutant and one of the key components determining the oxidizing capacity of the atmosphere. In this study, we analyzed five ice cores from Greenland at high resolution for CO concentrations by coupling laser spectrometry with continuous melting. By combining these new datasets, we produced an upper-bound estimate of past atmospheric CO abundance since preindustrial times for the Northern Hemisphere high latitudes, covering the period from 1700 to 1957 CE.
Stephen M. Platt, Øystein Hov, Torunn Berg, Knut Breivik, Sabine Eckhardt, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Markus Fiebig, Rebecca Fisher, Georg Hansen, Hans-Christen Hansson, Jost Heintzenberg, Ove Hermansen, Dominic Heslin-Rees, Kim Holmén, Stephen Hudson, Roland Kallenborn, Radovan Krejci, Terje Krognes, Steinar Larssen, David Lowry, Cathrine Lund Myhre, Chris Lunder, Euan Nisbet, Pernilla B. Nizzetto, Ki-Tae Park, Christina A. Pedersen, Katrine Aspmo Pfaffhuber, Thomas Röckmann, Norbert Schmidbauer, Sverre Solberg, Andreas Stohl, Johan Ström, Tove Svendby, Peter Tunved, Kjersti Tørnkvist, Carina van der Veen, Stergios Vratolis, Young Jun Yoon, Karl Espen Yttri, Paul Zieger, Wenche Aas, and Kjetil Tørseth
Atmos. Chem. Phys., 22, 3321–3369, https://doi.org/10.5194/acp-22-3321-2022, https://doi.org/10.5194/acp-22-3321-2022, 2022
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Here we detail the history of the Zeppelin Observatory, a unique global background site and one of only a few in the high Arctic. We present long-term time series of up to 30 years of atmospheric components and atmospheric transport phenomena. Many of these time series are important to our understanding of Arctic and global atmospheric composition change. Finally, we discuss the future of the Zeppelin Observatory and emerging areas of future research on the Arctic atmosphere.
Charel Wohl, Anna E. Jones, William T. Sturges, Philip D. Nightingale, Brent Else, Brian J. Butterworth, and Mingxi Yang
Biogeosciences, 19, 1021–1045, https://doi.org/10.5194/bg-19-1021-2022, https://doi.org/10.5194/bg-19-1021-2022, 2022
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We measured concentrations of five different organic gases in seawater in the high Arctic during summer. We found higher concentrations near the surface of the water column (top 5–10 m) and in areas of partial ice cover. This suggests that sea ice influences the concentrations of these gases. These gases indirectly exert a slight cooling effect on the climate, and it is therefore important to measure the levels accurately for future climate predictions.
Rupert Holzinger, Oliver Eppers, Kouji Adachi, Heiko Bozem, Markus Hartmann, Andreas Herber, Makoto Koike, Dylan B. Millet, Nobuhiro Moteki, Sho Ohata, Frank Stratmann, and Atsushi Yoshida
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-95, https://doi.org/10.5194/acp-2022-95, 2022
Revised manuscript not accepted
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In spring 2018 the research aircraft Polar 5 conducted flights in the Arctic atmosphere. The flight operation was from Station Nord in Greenland, 1700 km north of the Arctic Circle (81°43'N, 17°47'W). Using a mass spectrometer we measured more than 100 organic compounds in the air. We found a clear signature of natural organic compounds that are transported from forests to the high Arctic. These compounds have the potential to change the cloud cover and energy budget of the Arctic region.
Juhi Nagori, Narcisa Nechita-Bândă, Sebastian Oscar Danielache, Masumi Shinkai, Thomas Röckmann, and Maarten Krol
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-68, https://doi.org/10.5194/acp-2022-68, 2022
Publication in ACP not foreseen
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The sulfur isotopes (32S and 34S) were studied to understand the sources, sinks and processes of carbonyl sulphide (COS) in the atmosphere. COS is an important source of sulfur aerosol in the stratosphere (SSA). Few measurements of COS and SSA exist, but with our 1D model, we were able to match them and show the importance of COS to sulfate formation. Moreover, we are able to highlight some important processes for the COS budget and where measurements may fill a gap in current knowledge.
Michael Dyonisius, Vasilii Petrenko, Andrew Smith, Benjamin Hmiel, Peter Neff, Bin Yang, Quan Hua, Jochen Schmitt, Sarah Shackleton, Christo Buizert, Philip Place, James Menking, Ross Beaudette, Christina Harth, Michael Kalk, Heidi Roop, Bernhard Bereiter, Casey Armanetti, Isaac Vimont, Sylvia Englund Michel, Edward Brook, Jeffrey Severinghaus, Ray Weiss, and Joseph McConnell
The Cryosphere Discuss., https://doi.org/10.5194/tc-2021-375, https://doi.org/10.5194/tc-2021-375, 2022
Revised manuscript accepted for TC
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Cosmic rays that enter the atmosphere produce secondary particles. These particles react with surface minerals to produce radioactive nuclides. Cosmogenic nuclides are often used to constrain Earth's surface processes. However, the production rates from muons are not well constrained. We measured 14C in ice with well-constrained exposure history to quantitatively constrain the production rates from muons. We find that the commonly used 14C production rates are overestimated.
Truls Andersen, Marcel de Vries, Jaroslaw Necki, Justyna Swolkien, Malika Menoud, Thomas Röckmann, Anke Roiger, Andreas Fix, Wouter Peters, and Huilin Chen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1061, https://doi.org/10.5194/acp-2021-1061, 2022
Revised manuscript under review for ACP
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The Upper Silesian Coal Basin, Poland is one of the hot spots of methane emissions in Europe. Using an unmanned aerial vehicle (UAV), we performed atmospheric measurements of methane concentrations downwind of five ventilation shafts in this region and determined the emission rates from the individual shafts. We found a strong correlation between quantified shaft-averaged emission rates and hourly inventory data, which also allows us to estimate the methane emissions from the entire region.
Sarah Shackleton, James A. Menking, Edward Brook, Christo Buizert, Michael N. Dyonisius, Vasilii V. Petrenko, Daniel Baggenstos, and Jeffrey P. Severinghaus
Clim. Past, 17, 2273–2289, https://doi.org/10.5194/cp-17-2273-2021, https://doi.org/10.5194/cp-17-2273-2021, 2021
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In this study, we measure atmospheric noble gases trapped in ice cores to reconstruct ocean temperature during the last glaciation. Comparing the new reconstruction to other climate records, we show that the ocean reached its coldest temperatures before ice sheets reached maximum volumes and atmospheric CO2 reached its lowest concentrations. Ocean cooling played a major role in lowering atmospheric CO2 early in the glaciation, but it only played a minor role later.
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.
Malika Menoud, Carina van der Veen, Jaroslaw Necki, Jakub Bartyzel, Barbara Szénási, Mila Stanisavljević, Isabelle Pison, Philippe Bousquet, and Thomas Röckmann
Atmos. Chem. Phys., 21, 13167–13185, https://doi.org/10.5194/acp-21-13167-2021, https://doi.org/10.5194/acp-21-13167-2021, 2021
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Using measurements of methane isotopes in ambient air and a 3D atmospheric transport model, in Krakow, Poland, we mainly detected fossil-fuel-related sources, coming from coal mining in Silesia and from the use of natural gas in the city. Emission inventories report large emissions from coal mine activity in Silesia, which is in agreement with our measurements. However, methane sources in the urban area of Krakow related to the use of fossil fuels might be underestimated in the inventories.
Xinyi Lu, Stephen J. Harris, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Thomas Röckmann, Carina van der Veen, Malika Menoud, Stefan Schwietzke, and Bryce F. J. Kelly
Atmos. Chem. Phys., 21, 10527–10555, https://doi.org/10.5194/acp-21-10527-2021, https://doi.org/10.5194/acp-21-10527-2021, 2021
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Many coal seam gas (CSG) facilities in the Surat Basin, Australia, are adjacent to other sources of methane, including agricultural, urban, and natural seeps. This makes it challenging to estimate the amount of methane being emitted into the atmosphere from CSG facilities. This research demonstrates that measurements of the carbon and hydrogen stable isotopic composition of methane can distinguish between and apportion methane emissions from CSG facilities, cattle, and many other sources.
Max Thomas, Johannes C. Laube, Jan Kaiser, Samuel Allin, Patricia Martinerie, Robert Mulvaney, Anna Ridley, Thomas Röckmann, William T. Sturges, and Emmanuel Witrant
Atmos. Chem. Phys., 21, 6857–6873, https://doi.org/10.5194/acp-21-6857-2021, https://doi.org/10.5194/acp-21-6857-2021, 2021
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CFC gases are destroying the Earth's life-protecting ozone layer. We improve understanding of CFC destruction by measuring the isotopic fingerprint of the carbon in the three most abundant CFCs. These are the first such measurements in the main region where CFCs are destroyed – the stratosphere. We reconstruct the atmospheric isotope histories of these CFCs back to the 1950s by measuring air extracted from deep snow and using a model. The model and the measurements are generally consistent.
Vasilii V. Petrenko, Andrew M. Smith, Edward M. Crosier, Roxana Kazemi, Philip Place, Aidan Colton, Bin Yang, Quan Hua, and Lee T. Murray
Atmos. Meas. Tech., 14, 2055–2063, https://doi.org/10.5194/amt-14-2055-2021, https://doi.org/10.5194/amt-14-2055-2021, 2021
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This paper presents an improved methodology for measurements of atmospheric concentration of carbon-14-containing carbon monoxide (14CO), as well as a 1-year dataset that demonstrates the methodology. Atmospheric 14CO concentration measurements are useful for improving the understanding of spatial and temporal variability of hydroxyl radical concentrations. Key improvements over prior methods include a greatly reduced air sample size and accurate procedural blank characterization.
Jakob B. Pernov, Rossana Bossi, Thibaut Lebourgeois, Jacob K. Nøjgaard, Rupert Holzinger, Jens L. Hjorth, and Henrik Skov
Atmos. Chem. Phys., 21, 2895–2916, https://doi.org/10.5194/acp-21-2895-2021, https://doi.org/10.5194/acp-21-2895-2021, 2021
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Volatile organic compounds (VOCs) are an important constituent in the Arctic atmosphere due to their effect on aerosol and ozone formation. However, an understanding of their sources is lacking. This research presents a multiseason high-time-resolution dataset of VOCs in the Arctic and details their temporal characteristics and source apportionment. Four sources were identified: biomass burning, marine cryosphere, background, and Arctic haze.
Ashok K. Luhar, David M. Etheridge, Zoë M. Loh, Julie Noonan, Darren Spencer, Lisa Smith, and Cindy Ong
Atmos. Chem. Phys., 20, 15487–15511, https://doi.org/10.5194/acp-20-15487-2020, https://doi.org/10.5194/acp-20-15487-2020, 2020
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With the sharp rise in coal seam gas (CSG) production in Queensland’s Surat Basin, there is much interest in quantifying methane emissions from this area and from unconventional gas production in general. We develop and apply a regional Bayesian inverse model that uses hourly methane concentration data from two sites and modelled backward dispersion to quantify emissions. The model requires a narrow prior and suggests that the emissions from the CSG areas are 33% larger than bottom-up estimates.
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.
Hossein Maazallahi, Julianne M. Fernandez, Malika Menoud, Daniel Zavala-Araiza, Zachary D. Weller, Stefan Schwietzke, Joseph C. von Fischer, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 14717–14740, https://doi.org/10.5194/acp-20-14717-2020, https://doi.org/10.5194/acp-20-14717-2020, 2020
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Methane accounts for ∼ 25 % of current climate warming. The current lack of methane measurements is a barrier for tracking major sources, which are key for near-term climate mitigation. We use mobile measurements to identify and quantify methane emission sources in Utrecht (NL) and Hamburg (DE) with a focus on natural gas pipeline leaks. The measurements resulted in fixing the major leaks by the local utility, but coordinated efforts are needed at national levels for further emission reductions.
Joram J. D. Hooghiem, Maria Elena Popa, Thomas Röckmann, Jens-Uwe Grooß, Ines Tritscher, Rolf Müller, Rigel Kivi, and Huilin Chen
Atmos. Chem. Phys., 20, 13985–14003, https://doi.org/10.5194/acp-20-13985-2020, https://doi.org/10.5194/acp-20-13985-2020, 2020
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Wildfires release a large quantity of pollutants that can reach the stratosphere through pyro-convection events. In September 2017, a stratospheric plume was accidentally sampled during balloon soundings in northern Finland. The source of the plume was identified to be wildfire smoke based on in situ measurements of carbon monoxide (CO) and stable isotope analysis of CO. Furthermore, the age of the plume was estimated using backwards transport modelling to be ~24 d, with its origin in Canada.
Alina Fiehn, Julian Kostinek, Maximilian Eckl, Theresa Klausner, Michał Gałkowski, Jinxuan Chen, Christoph Gerbig, Thomas Röckmann, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Pawel Jagoda, Norman Wildmann, Christian Mallaun, Rostyslav Bun, Anna-Leah Nickl, Patrick Jöckel, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 20, 12675–12695, https://doi.org/10.5194/acp-20-12675-2020, https://doi.org/10.5194/acp-20-12675-2020, 2020
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A severe reduction of greenhouse gas emissions is necessary to fulfill the Paris Agreement. We use aircraft- and ground-based in situ observations of trace gases and wind speed from two flights over the Upper Silesian Coal Basin, Poland, for independent emission estimation. The derived methane emission estimates are within the range of emission inventories, carbon dioxide estimates are in the lower range and carbon monoxide emission estimates are slightly higher than emission inventory values.
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.
Patrick Dewald, Jonathan M. Liebmann, Nils Friedrich, Justin Shenolikar, Jan Schuladen, Franz Rohrer, David Reimer, Ralf Tillmann, Anna Novelli, Changmin Cho, Kangming Xu, Rupert Holzinger, François Bernard, Li Zhou, Wahid Mellouki, Steven S. Brown, Hendrik Fuchs, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 10459–10475, https://doi.org/10.5194/acp-20-10459-2020, https://doi.org/10.5194/acp-20-10459-2020, 2020
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We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from non-steady-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account to ~ 50 % of overall NO3 losses.
Jordi Vilà-Guerau de Arellano, Patrizia Ney, Oscar Hartogensis, Hugo de Boer, Kevin van Diepen, Dzhaner Emin, Geiske de Groot, Anne Klosterhalfen, Matthias Langensiepen, Maria Matveeva, Gabriela Miranda-García, Arnold F. Moene, Uwe Rascher, Thomas Röckmann, Getachew Adnew, Nicolas Brüggemann, Youri Rothfuss, and Alexander Graf
Biogeosciences, 17, 4375–4404, https://doi.org/10.5194/bg-17-4375-2020, https://doi.org/10.5194/bg-17-4375-2020, 2020
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The CloudRoots field experiment has obtained an open comprehensive observational data set that includes soil, plant, and atmospheric variables to investigate the interactions between a heterogeneous land surface and its overlying atmospheric boundary layer, including the rapid perturbations of clouds in evapotranspiration. Our findings demonstrate that in order to understand and represent diurnal variability, we need to measure and model processes from the leaf to the landscape scales.
Johannes C. Laube, Emma C. Leedham Elvidge, Karina E. Adcock, Bianca Baier, Carl A. M. Brenninkmeijer, Huilin Chen, Elise S. Droste, Jens-Uwe Grooß, Pauli Heikkinen, Andrew J. Hind, Rigel Kivi, Alexander Lojko, Stephen A. Montzka, David E. Oram, Steve Randall, Thomas Röckmann, William T. Sturges, Colm Sweeney, Max Thomas, Elinor Tuffnell, and Felix Ploeger
Atmos. Chem. Phys., 20, 9771–9782, https://doi.org/10.5194/acp-20-9771-2020, https://doi.org/10.5194/acp-20-9771-2020, 2020
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We demonstrate that AirCore technology, which is based on small low-cost balloons, can provide access to trace gas measurements such as CFCs at ultra-low abundances. This is a new way to quantify ozone-depleting, and related, substances in the stratosphere, which is largely inaccessible to aircraft. We show two potential uses: (a) tracking the stratospheric circulation, which is predicted to change, and (b) assessing three common meteorological reanalyses driving a global stratospheric model.
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.
Getachew Agmuas Adnew, Thijs L. Pons, Gerbrand Koren, Wouter Peters, and Thomas Röckmann
Biogeosciences, 17, 3903–3922, https://doi.org/10.5194/bg-17-3903-2020, https://doi.org/10.5194/bg-17-3903-2020, 2020
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We measured the effect of photosynthesis, the largest flux in the carbon cycle, on the triple oxygen isotope composition of atmospheric CO2 at the leaf level during gas exchange using three plant species. The main factors that limit the impact of land vegetation on the triple oxygen isotope composition of atmospheric CO2 are identified, characterized and discussed. The effect of photosynthesis on the isotopic composition of CO2 is commonly quantified as discrimination (ΔA).
Kévin Fourteau, Laurent Arnaud, Xavier Faïn, Patricia Martinerie, David M. Etheridge, Vladimir Lipenkov, and Jean-Marc Barnola
Earth Syst. Sci. Data, 12, 1171–1177, https://doi.org/10.5194/essd-12-1171-2020, https://doi.org/10.5194/essd-12-1171-2020, 2020
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Measurements of the porosity of three polar firns were conducted in the 1990s by Jean-Marc Barnola using the method of gas pycnometry. From these data, a parametrization of firn pore closure was produced and used in different published articles. However, the data have not been published in their own right yet. We have made the data publicly accessible on the PANGAEA database and here propose describing how they were obtained and used to produce the pore closure parametrization.
Charel Wohl, Ian Brown, Vassilis Kitidis, Anna E. Jones, William T. Sturges, Philip D. Nightingale, and Mingxi Yang
Biogeosciences, 17, 2593–2619, https://doi.org/10.5194/bg-17-2593-2020, https://doi.org/10.5194/bg-17-2593-2020, 2020
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The oceans represent a poorly understood source of organic carbon to the atmosphere. In this paper, we present ship-based measurements of specific compounds in ambient air and seawater of the Southern Ocean. We present fluxes of these gases between air and sea at very high resolution. The data also contain evidence for day and night variations in some of these compounds. These measurements can be used to better understand the role of the Southern Ocean in the cycling of these compounds.
Elise S. Droste, Karina E. Adcock, Matthew J. Ashfold, Charles Chou, Zoë Fleming, Paul J. Fraser, Lauren J. Gooch, Andrew J. Hind, Ray L. Langenfelds, Emma C. Leedham Elvidge, Norfazrin Mohd Hanif, Simon O'Doherty, David E. Oram, Chang-Feng Ou-Yang, Marios Panagi, Claire E. Reeves, William T. Sturges, and Johannes C. Laube
Atmos. Chem. Phys., 20, 4787–4807, https://doi.org/10.5194/acp-20-4787-2020, https://doi.org/10.5194/acp-20-4787-2020, 2020
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We update the tropospheric trends and emissions of six perfluorocarbon (PFC) gases, including separate isomers. Trends for these strong greenhouse gases are still increasing, but at slower rates than previously. The lack of natural sinks results in the global accumulation of 833 million metric tonnes of CO2 equivalent for these six PFCs by 2017. Modelling results indicate potential source regions and types in East Asia, but we find that many emissions are unaccounted for in emission reports.
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.
Jia Chen, Florian Dietrich, Hossein Maazallahi, Andreas Forstmaier, Dominik Winkler, Magdalena E. G. Hofmann, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 3683–3696, https://doi.org/10.5194/acp-20-3683-2020, https://doi.org/10.5194/acp-20-3683-2020, 2020
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We demonstrate for the first time that large festivals can be significant methane sources, though they are not included in emission inventories. We combined in situ measurements with a Gaussian plume model to determine the Oktoberfest emissions and show that they are not due solely to human biogenic emissions, but are instead primarily fossil fuel related. Our study provides the foundation to develop reduction policies for such events and new pathways to mitigate fossil fuel methane emissions.
Kévin Fourteau, Patricia Martinerie, Xavier Faïn, Alexey A. Ekaykin, Jérôme Chappellaz, and Vladimir Lipenkov
Clim. Past, 16, 503–522, https://doi.org/10.5194/cp-16-503-2020, https://doi.org/10.5194/cp-16-503-2020, 2020
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We quantify how the greenhouse gas records of East Antarctic ice cores (which are the oldest ice cores) might differ from the actual atmosphere history. It is required to properly interpret ice core data. For this, we measured the methane of five new East Antarctic ice core sections using a high-resolution technique. We found that in these very old ice cores, one can retrieve concentration variations occurring in only a few centuries, allowing climatologists to study climate's fast dynamics.
Stefan Lossow, Charlotta Högberg, Farahnaz Khosrawi, Gabriele P. Stiller, Ralf Bauer, Kaley A. Walker, Sylvia Kellmann, Andrea Linden, Michael Kiefer, Norbert Glatthor, Thomas von Clarmann, Donal P. Murtagh, Jörg Steinwagner, Thomas Röckmann, and Roland Eichinger
Atmos. Meas. Tech., 13, 287–308, https://doi.org/10.5194/amt-13-287-2020, https://doi.org/10.5194/amt-13-287-2020, 2020
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.
Kévin Fourteau, Patricia Martinerie, Xavier Faïn, Christoph F. Schaller, Rebecca J. Tuckwell, Henning Löwe, Laurent Arnaud, Olivier Magand, Elizabeth R. Thomas, Johannes Freitag, Robert Mulvaney, Martin Schneebeli, and Vladimir Ya. Lipenkov
The Cryosphere, 13, 3383–3403, https://doi.org/10.5194/tc-13-3383-2019, https://doi.org/10.5194/tc-13-3383-2019, 2019
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Understanding gas trapping in polar ice is essential to study the relationship between greenhouse gases and past climates. New data of bubble closure, used in a simple gas-trapping model, show inconsistency with the final air content in ice. This suggests gas trapping is not fully understood. We also use a combination of high-resolution measurements to investigate the effect of polar snow stratification on gas trapping and find that all strata have similar pores, but that some close in advance.
Marco de Bruine, Maarten Krol, Jordi Vilà-Guerau de Arellano, and Thomas Röckmann
Geosci. Model Dev., 12, 5177–5196, https://doi.org/10.5194/gmd-12-5177-2019, https://doi.org/10.5194/gmd-12-5177-2019, 2019
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An aerosol scheme with multiple aerosol species is introduced in the Dutch Atmospheric Large-Eddy Simulation model (DALES) and focused to simulate the feedback of aerosol–cloud interaction (ACI) on the aerosol population. Cloud aerosol processing is found to be sensitive to the numerical method, while removal by precipitation is more stable. How ACI increases or decreases the mean aerosol size depends on the balance between the evaporation of clouds/rain and ultimate removal by precipitation.
Rupert Holzinger, W. Joe F. Acton, William J. Bloss, Martin Breitenlechner, Leigh R. Crilley, Sébastien Dusanter, Marc Gonin, Valerie Gros, Frank N. Keutsch, Astrid Kiendler-Scharr, Louisa J. Kramer, Jordan E. Krechmer, Baptiste Languille, Nadine Locoge, Felipe Lopez-Hilfiker, Dušan Materić, Sergi Moreno, Eiko Nemitz, Lauriane L. J. Quéléver, Roland Sarda Esteve, Stéphane Sauvage, Simon Schallhart, Roberto Sommariva, Ralf Tillmann, Sergej Wedel, David R. Worton, Kangming Xu, and Alexander Zaytsev
Atmos. Meas. Tech., 12, 6193–6208, https://doi.org/10.5194/amt-12-6193-2019, https://doi.org/10.5194/amt-12-6193-2019, 2019
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.
Jens Mühle, Cathy M. Trudinger, Luke M. Western, Matthew Rigby, Martin K. Vollmer, Sunyoung Park, Alistair J. Manning, Daniel Say, Anita Ganesan, L. Paul Steele, Diane J. Ivy, Tim Arnold, Shanlan Li, Andreas Stohl, Christina M. Harth, Peter K. Salameh, Archie McCulloch, Simon O'Doherty, Mi-Kyung Park, Chun Ok Jo, Dickon Young, Kieran M. Stanley, Paul B. Krummel, Blagoj Mitrevski, Ove Hermansen, Chris Lunder, Nikolaos Evangeliou, Bo Yao, Jooil Kim, Benjamin Hmiel, Christo Buizert, Vasilii V. Petrenko, Jgor Arduini, Michela Maione, David M. Etheridge, Eleni Michalopoulou, Mike Czerniak, Jeffrey P. Severinghaus, Stefan Reimann, Peter G. Simmonds, Paul J. Fraser, Ronald G. Prinn, and Ray F. Weiss
Atmos. Chem. Phys., 19, 10335–10359, https://doi.org/10.5194/acp-19-10335-2019, https://doi.org/10.5194/acp-19-10335-2019, 2019
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We discuss atmospheric concentrations and emissions of the strong greenhouse gas perfluorocyclobutane. A large fraction of recent emissions stem from China, India, and Russia, probably as a by-product from the production of fluoropolymers and fluorochemicals. Most historic emissions likely stem from developed countries. Total emissions are higher than what is being reported. Clearly, more measurements and better reporting are needed to understand emissions of this and other greenhouse gases.
James A. Menking, Edward J. Brook, Sarah A. Shackleton, Jeffrey P. Severinghaus, Michael N. Dyonisius, Vasilii Petrenko, Joseph R. McConnell, Rachael H. Rhodes, Thomas K. Bauska, Daniel Baggenstos, Shaun Marcott, and Stephen Barker
Clim. Past, 15, 1537–1556, https://doi.org/10.5194/cp-15-1537-2019, https://doi.org/10.5194/cp-15-1537-2019, 2019
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An ice core from Taylor Glacier, Antarctica, spans a period ~ 70 000 years ago when Earth entered the last ice age. Chemical analyses of the ice and air bubbles allow for an independent determination of the ages of the ice and gas bubbles. The difference between the age of the ice and the bubbles at any given depth, called ∆age, is unusually high in the Taylor Glacier core compared to the Taylor Dome ice core situated to the south. This implies a dramatic accumulation gradient between the sites.
Charel Wohl, David Capelle, Anna Jones, William T. Sturges, Philip D. Nightingale, Brent G. T. Else, and Mingxi Yang
Ocean Sci., 15, 925–940, https://doi.org/10.5194/os-15-925-2019, https://doi.org/10.5194/os-15-925-2019, 2019
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In this paper we present a gas equilibrator that can be used to equilibrate gases continuously or in discrete samples from seawater into a carrier gas. The headspace is analysed by a commercially available proton-transfer-reaction mass spectrometer. This allows for the measurement of a broad range of dissolved gases up to a very high solubility in seawater. The main advantage of this equilibrator is its unique design and ease of reproducibility.
Isaac J. Vimont, Jocelyn C. Turnbull, Vasilii V. Petrenko, Philip F. Place, Colm Sweeney, Natasha Miles, Scott Richardson, Bruce H. Vaughn, and James W. C. White
Atmos. Chem. Phys., 19, 8547–8562, https://doi.org/10.5194/acp-19-8547-2019, https://doi.org/10.5194/acp-19-8547-2019, 2019
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Stable isotopes of Carbon Monoxide (CO) and radiocarbon carbon dioxide were measured over three summers at Indianapolis, Indiana, US, and for 1 year at a site thought to be strongly influenced by CO from oxidized volatile organic compounds (VOCs) in South Carolina, US. The Indianapolis results were used to provide an estimate of the carbon and oxygen isotopic signatures of CO produced from oxidized VOCs. This updated estimate agrees well with the data from South Carolina during the summer.
Mauro Rubino, David M. Etheridge, David P. Thornton, Russell Howden, Colin E. Allison, Roger J. Francey, Ray L. Langenfelds, L. Paul Steele, Cathy M. Trudinger, Darren A. Spencer, Mark A. J. Curran, Tas D. van Ommen, and Andrew M. Smith
Earth Syst. Sci. Data, 11, 473–492, https://doi.org/10.5194/essd-11-473-2019, https://doi.org/10.5194/essd-11-473-2019, 2019
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The scientific community uses numerical models to predict future atmospheric levels of greenhouse gases causing global warming. This study presents the history of atmospheric concentration of the major greenhouse gases over the last 2000 years measured in ice core bubbles from the site of Law Dome (East Antarctica). The associated dataset is useful to test climate models and help provide accurate predictions of future climate change.
Martin K. Vollmer, François Bernard, Blagoj Mitrevski, L. Paul Steele, Cathy M. Trudinger, Stefan Reimann, Ray L. Langenfelds, Paul B. Krummel, Paul J. Fraser, David M. Etheridge, Mark A. J. Curran, and James B. Burkholder
Atmos. Chem. Phys., 19, 3481–3492, https://doi.org/10.5194/acp-19-3481-2019, https://doi.org/10.5194/acp-19-3481-2019, 2019
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We have discovered a new compound in the atmosphere, octafluorooxolane (c-C4F8O), from measurements in archived air samples. From our laboratory studies, we find that c-C4F8O is a very powerful greenhouse gas thereby contributing to global warming, and that it has a very long atmospheric lifetime of more than 3500 years. Based on our measurements we could reconstruct its atmospheric evolution over more than 4 decades. Based on this, we could estimate the global emissions of c-C4F8O.
Iris N. Dekker, Sander Houweling, Sudhanshu Pandey, Maarten Krol, Thomas Röckmann, Tobias Borsdorff, Jochen Landgraf, and Ilse Aben
Atmos. Chem. Phys., 19, 3433–3445, https://doi.org/10.5194/acp-19-3433-2019, https://doi.org/10.5194/acp-19-3433-2019, 2019
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During November 2017, very high pollution levels were measured in the northern part of India. In this study, satellite (TROPOMI) data and model (WRF) data on carbon monoxide (CO) are studied to investigate the main sources of the CO pollution over the Indo-Gangetic Plain. We found that residential and commercial combustion was a much more important source of CO than the post-monsoon crop burning during this period. Meteorology was found important in the accumulation and ventilation of CO.
Naomi J. Farren, Rachel E. Dunmore, Mohammed Iqbal Mead, Mohd Shahrul Mohd Nadzir, Azizan Abu Samah, Siew-Moi Phang, Brian J. Bandy, William T. Sturges, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 19, 1537–1553, https://doi.org/10.5194/acp-19-1537-2019, https://doi.org/10.5194/acp-19-1537-2019, 2019
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During the winter monsoon, air quality on the east coast of Peninsular Malaysia is influenced by local emissions and aged emissions transported from highly polluted East Asian regions. Atmospheric particulate matter has been sampled at a rural coastal location, and ion chromatography has been used to make time-resolved measurements of the major atmospheric ions present. Analysis of aerosol composition and back trajectories has provided an insight into common sources and formation pathways.
Dušan Materić, Elke Ludewig, Kangming Xu, Thomas Röckmann, and Rupert Holzinger
The Cryosphere, 13, 297–307, https://doi.org/10.5194/tc-13-297-2019, https://doi.org/10.5194/tc-13-297-2019, 2019
Shaojie Song, Hélène Angot, Noelle E. Selin, Hubert Gallée, Francesca Sprovieri, Nicola Pirrone, Detlev Helmig, Joël Savarino, Olivier Magand, and Aurélien Dommergue
Atmos. Chem. Phys., 18, 15825–15840, https://doi.org/10.5194/acp-18-15825-2018, https://doi.org/10.5194/acp-18-15825-2018, 2018
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Mercury is a trace metal with adverse health effects on human and wildlife. Its unique property makes it undergo long-range transport, and even remote Antarctica receives significant inputs. This paper presents the first model that aims to understand mercury behavior over the Antarctic Plateau. We find that mercury is quickly cycled between snow and air in the sunlit period, likely driven by bromine chemistry, and that several uncertain processes contribute to its behavior in the dark period.
Georgios I. Gkatzelis, Thorsten Hohaus, Ralf Tillmann, Iulia Gensch, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Zhujun Yu, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 18, 12969–12989, https://doi.org/10.5194/acp-18-12969-2018, https://doi.org/10.5194/acp-18-12969-2018, 2018
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Defining the fundamental parameters that distribute organic molecules between the gas and particle phases is essential to understand their impact on the atmosphere. In this work, gas to particle partitioning of major biogenic oxidation products from monoterpenes and real plant emissions was investigated. While measurement results and theoretical calculation for most semi-volatile compounds are in good agreement, significant deviations are found for intermediate volatile organic compounds.
Alexis Burr, Clément Ballot, Pierre Lhuissier, Patricia Martinerie, Christophe L. Martin, and Armelle Philip
The Cryosphere, 12, 2481–2500, https://doi.org/10.5194/tc-12-2481-2018, https://doi.org/10.5194/tc-12-2481-2018, 2018
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Three-dimensional imaging of the pore network of polar firn from Antarctica was realized in order to relate the morphological evolution of pores with their progressive closure with depth. Evaluating the closed porosity was found to be very dependent on the size of samples and image reconstructions. A connectivity index, which is a parameter less dependent on such issues, was proposed and proved to accurately predict the close-off depths and densities of two polar sites.
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.
Marco de Bruine, Maarten Krol, Twan van Noije, Philippe Le Sager, and Thomas Röckmann
Geosci. Model Dev., 11, 1443–1465, https://doi.org/10.5194/gmd-11-1443-2018, https://doi.org/10.5194/gmd-11-1443-2018, 2018
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Precipitation evaporation (PE) and subsequent aerosol resuspension (AR) are currently ignored or implemented only crudely in GCMs. This research introduces PE to Earth system model EC-Earth and explores ways to treat AR and the impact on global aerosol burden. Simple 1:1 scaling of AR with PE leads to an increase (+8 to 15.9 %). Taking into account raindrop size distribution and/or accounting for in-rain aerosol processing decreases aerosol burden -1.5 to 6.2 % and -10 to -11 %, respectively.
Karina E. Adcock, Claire E. Reeves, Lauren J. Gooch, Emma C. Leedham Elvidge, Matthew J. Ashfold, Carl A. M. Brenninkmeijer, Charles Chou, Paul J. Fraser, Ray L. Langenfelds, Norfazrin Mohd Hanif, Simon O'Doherty, David E. Oram, Chang-Feng Ou-Yang, Siew Moi Phang, Azizan Abu Samah, Thomas Röckmann, William T. Sturges, and Johannes C. Laube
Atmos. Chem. Phys., 18, 4737–4751, https://doi.org/10.5194/acp-18-4737-2018, https://doi.org/10.5194/acp-18-4737-2018, 2018
Peter G. Simmonds, Matthew Rigby, Archie McCulloch, Martin K. Vollmer, Stephan Henne, Jens Mühle, Simon O'Doherty, Alistair J. Manning, Paul B. Krummel, Paul J. Fraser, Dickon Young, Ray F. Weiss, Peter K. Salameh, Christina M. Harth, Stefan Reimann, Cathy M. Trudinger, L. Paul Steele, Ray H. J. Wang, Diane J. Ivy, Ronald G. Prinn, Blagoj Mitrevski, and David M. Etheridge
Atmos. Chem. Phys., 18, 4153–4169, https://doi.org/10.5194/acp-18-4153-2018, https://doi.org/10.5194/acp-18-4153-2018, 2018
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Recent measurements of the potent greenhouse gas HFC-23, a by-product of HCFC-22 production, show a 28 % increase in the atmospheric mole fraction from 2009 to 2016. A minimum in the atmospheric abundance of HFC-23 in 2009 was attributed to abatement of HFC-23 emissions by incineration under the Clean Development Mechanism (CDM). Our results indicate that the recent increase in HFC-23 emissions is driven by failure of mitigation under the CDM to keep pace with increased HCFC-22 production.
Georgios I. Gkatzelis, Ralf Tillmann, Thorsten Hohaus, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Meas. Tech., 11, 1481–1500, https://doi.org/10.5194/amt-11-1481-2018, https://doi.org/10.5194/amt-11-1481-2018, 2018
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This manuscript presents an intercomparison of state-of-the-art online and in situ particle sampling techniques connected to proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS). Collection and vaporization of aerosol combined with soft ionization mass spectrometry offers the advantage of detailed chemical characterization of SOA species. The benefits of these techniques are highlighted through their consistency in providing the chemical composition of biogenic SOA.
Kieran M. Stanley, Aoife Grant, Simon O'Doherty, Dickon Young, Alistair J. Manning, Ann R. Stavert, T. Gerard Spain, Peter K. Salameh, Christina M. Harth, Peter G. Simmonds, William T. Sturges, David E. Oram, and Richard G. Derwent
Atmos. Meas. Tech., 11, 1437–1458, https://doi.org/10.5194/amt-11-1437-2018, https://doi.org/10.5194/amt-11-1437-2018, 2018
Emma C. Leedham Elvidge, Harald Bönisch, Carl A. M. Brenninkmeijer, Andreas Engel, Paul J. Fraser, Eileen Gallacher, Ray Langenfelds, Jens Mühle, David E. Oram, Eric A. Ray, Anna R. Ridley, Thomas Röckmann, William T. Sturges, Ray F. Weiss, and Johannes C. Laube
Atmos. Chem. Phys., 18, 3369–3385, https://doi.org/10.5194/acp-18-3369-2018, https://doi.org/10.5194/acp-18-3369-2018, 2018
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Chemical species measured in stratospheric air can be used as proxies for stratospheric circulation changes which cannot be measured directly. A range of tracers is important to understand changing stratospheric dynamics. We demonstrate the suitability of PFCs and HFCs as tracers and support recent work that reduces the current stratospheric lifetime of SF6. Updates to policy-relevant parameters (e.g. stratospheric lifetime) linked to this change are provided for O3-depleting substances.
Taku Umezawa, Carl A. M. Brenninkmeijer, Thomas Röckmann, Carina van der Veen, Stanley C. Tyler, Ryo Fujita, Shinji Morimoto, Shuji Aoki, Todd Sowers, Jochen Schmitt, Michael Bock, Jonas Beck, Hubertus Fischer, Sylvia E. Michel, Bruce H. Vaughn, John B. Miller, James W. C. White, Gordon Brailsford, Hinrich Schaefer, Peter Sperlich, Willi A. Brand, Michael Rothe, Thomas Blunier, David Lowry, Rebecca E. Fisher, Euan G. Nisbet, Andrew L. Rice, Peter Bergamaschi, Cordelia Veidt, and Ingeborg Levin
Atmos. Meas. Tech., 11, 1207–1231, https://doi.org/10.5194/amt-11-1207-2018, https://doi.org/10.5194/amt-11-1207-2018, 2018
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Isotope measurements are useful for separating different methane sources. However, the lack of widely accepted standards and calibration methods for stable carbon and hydrogen isotopic ratios of methane in air has caused significant measurement offsets among laboratories. We conducted worldwide interlaboratory comparisons, surveyed the literature and assessed them systematically. This study may be of help in future attempts to harmonize data sets of isotopic composition of atmospheric methane.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Martin K. Vollmer, Dickon Young, Cathy M. Trudinger, Jens Mühle, Stephan Henne, Matthew Rigby, Sunyoung Park, Shanlan Li, Myriam Guillevic, Blagoj Mitrevski, Christina M. Harth, Benjamin R. Miller, Stefan Reimann, Bo Yao, L. Paul Steele, Simon A. Wyss, Chris R. Lunder, Jgor Arduini, Archie McCulloch, Songhao Wu, Tae Siek Rhee, Ray H. J. Wang, Peter K. Salameh, Ove Hermansen, Matthias Hill, Ray L. Langenfelds, Diane Ivy, Simon O'Doherty, Paul B. Krummel, Michela Maione, David M. Etheridge, Lingxi Zhou, Paul J. Fraser, Ronald G. Prinn, Ray F. Weiss, and Peter G. Simmonds
Atmos. Chem. Phys., 18, 979–1002, https://doi.org/10.5194/acp-18-979-2018, https://doi.org/10.5194/acp-18-979-2018, 2018
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We measured the three chlorofluorocarbons (CFCs) CFC-13, CFC-114, and CFC-115 in the atmosphere because they are important in stratospheric ozone depletion. These compounds should have decreased in the atmosphere because they are banned by the Montreal Protocol but we find the opposite. Emissions over the last decade have not declined on a global scale. We use inverse modeling and our observations to find that a large part of the emissions originate in the Asian region.
Kévin Fourteau, Xavier Faïn, Patricia Martinerie, Amaëlle Landais, Alexey A. Ekaykin, Vladimir Ya. Lipenkov, and Jérôme Chappellaz
Clim. Past, 13, 1815–1830, https://doi.org/10.5194/cp-13-1815-2017, https://doi.org/10.5194/cp-13-1815-2017, 2017
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We measured methane concentrations from a polar ice core to quantify the differences between the ice record and the past true atmospheric conditions. Two effects were investigated by combining data analysis and modeling: the stratification of polar snow before gas enclosure driving chronological hiatuses in the record and the gradual formation of bubbles in the ice attenuating fast atmospheric variations. This study will contribute to improving future climatic interpretations from ice archives.
Iris N. Dekker, Sander Houweling, Ilse Aben, Thomas Röckmann, Maarten Krol, Sara Martínez-Alonso, Merritt N. Deeter, and Helen M. Worden
Atmos. Chem. Phys., 17, 14675–14694, https://doi.org/10.5194/acp-17-14675-2017, https://doi.org/10.5194/acp-17-14675-2017, 2017
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This study estimates carbon monoxide emissions from the city of Madrid using MOPITT satellite data. There are two methods used and reviewed in this paper: a method that can only estimate a trend in the emission and a newly developed method that also includes model data from WRF to quantify the emissions. We find Madrid CO emissions to be lower by 48 % for 2002 and by 17 % for 2006 compared with the EdgarV4.2 emission inventory, but uncertainty (20 to 50 %) remains.
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.
Heather Graven, Colin E. Allison, David M. Etheridge, Samuel Hammer, Ralph F. Keeling, Ingeborg Levin, Harro A. J. Meijer, Mauro Rubino, Pieter P. Tans, Cathy M. Trudinger, Bruce H. Vaughn, and James W. C. White
Geosci. Model Dev., 10, 4405–4417, https://doi.org/10.5194/gmd-10-4405-2017, https://doi.org/10.5194/gmd-10-4405-2017, 2017
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Modelling of carbon isotopes 13C and 14C in land and ocean components of Earth system models provides opportunities for new insights and improved understanding of global carbon cycling, and for model evaluation. We compiled existing historical datasets to define the annual mean carbon isotopic composition of atmospheric CO2 for 1850–2015 that can be used in CMIP6 and other modelling activities.
David E. Oram, Matthew J. Ashfold, Johannes C. Laube, Lauren J. Gooch, Stephen Humphrey, William T. Sturges, Emma C. Leedham Elvidge, Grant L. Forster, Neil R. P. Harris, Mohammed Iqbal Mead, Azizan Abu Samah, Siew Moi Phang, Chang-Feng Ou-Yang, Neng-Huei Lin, Jia-Lin Wang, Angela K. Baker, Carl A. M. Brenninkmeijer, and David Sherry
Atmos. Chem. Phys., 17, 11929–11941, https://doi.org/10.5194/acp-17-11929-2017, https://doi.org/10.5194/acp-17-11929-2017, 2017
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We have observed large amounts of man-made chlorine compounds in E and SE Asia and in the upper tropical troposphere. These relatively short-lived compounds are not controlled by the Montreal Protocol, but if significant quantities were able to reach the stratosphere, the long-term recovery of stratospheric ozone would be delayed. We have also identified an important atmospheric transport mechanism that can rapidly transport these chemicals from E Asia to the upper troposphere via the tropics.
Jason Roberts, Andrew Moy, Christopher Plummer, Tas van Ommen, Mark Curran, Tessa Vance, Samuel Poynter, Yaping Liu, Joel Pedro, Adam Treverrow, Carly Tozer, Lenneke Jong, Pippa Whitehouse, Laetitia Loulergue, Jerome Chappellaz, Vin Morgan, Renato Spahni, Adrian Schilt, Cecilia MacFarling Meure, David Etheridge, and Thomas Stocker
Clim. Past Discuss., https://doi.org/10.5194/cp-2017-96, https://doi.org/10.5194/cp-2017-96, 2017
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Here we present a revised Law Dome, Dome Summit South (DSS) ice core age model (denoted LD2017) that significantly improves the chronology over the last 88 thousand years. An ensemble approach was used, allowing for the computation of both a median age and associated uncertainty as a function of depth. We use a non-linear interpolation between age ties and unlike previous studies, we made an independent estimate of the snow accumulation rate, where required, for the use of gas based age ties.
Daniel Baggenstos, Thomas K. Bauska, Jeffrey P. Severinghaus, James E. Lee, Hinrich Schaefer, Christo Buizert, Edward J. Brook, Sarah Shackleton, and Vasilii V. Petrenko
Clim. Past, 13, 943–958, https://doi.org/10.5194/cp-13-943-2017, https://doi.org/10.5194/cp-13-943-2017, 2017
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We present measurements of the gas composition in trapped air bubbles in ice samples taken from Taylor Glacier, Antarctica. We can show that ice from the entire last glacial cycle (125 000 years ago to the present) is exposed at the surface of this glacier and that the atmospheric record contained in the air bubbles is well preserved. Taylor Glacier therefore provides an easily accessible archive of ancient ice that allows for studies of trace components that require large ice volumes.
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.
Malte Meinshausen, Elisabeth Vogel, Alexander Nauels, Katja Lorbacher, Nicolai Meinshausen, David M. Etheridge, Paul J. Fraser, Stephen A. Montzka, Peter J. Rayner, Cathy M. Trudinger, Paul B. Krummel, Urs Beyerle, Josep G. Canadell, John S. Daniel, Ian G. Enting, Rachel M. Law, Chris R. Lunder, Simon O'Doherty, Ron G. Prinn, Stefan Reimann, Mauro Rubino, Guus J. M. Velders, Martin K. Vollmer, Ray H. J. Wang, and Ray Weiss
Geosci. Model Dev., 10, 2057–2116, https://doi.org/10.5194/gmd-10-2057-2017, https://doi.org/10.5194/gmd-10-2057-2017, 2017
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Climate change is primarily driven by human-induced increases of greenhouse gas (GHG) concentrations. Based on ongoing community efforts (e.g. AGAGE and NOAA networks, ice cores), this study presents historical concentrations of CO2, CH4, N2O and 40 other GHGs from year 0 to year 2014. The data is recommended as input for climate models for pre-industrial, historical runs under CMIP6. Global means, but also latitudinal by monthly surface concentration fields are provided.
Carl Meusinger, Ulrike Dusek, Stephanie M. King, Rupert Holzinger, Thomas Rosenørn, Peter Sperlich, Maxime Julien, Gerald S. Remaud, Merete Bilde, Thomas Röckmann, and Matthew S. Johnson
Atmos. Chem. Phys., 17, 6373–6391, https://doi.org/10.5194/acp-17-6373-2017, https://doi.org/10.5194/acp-17-6373-2017, 2017
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Isotope studies can constrain budgets of secondary organic aerosol (SOA) that is pivotal to air pollution and climate. SOA from α-pinene ozonolysis was found to be enriched in 13C relative to the precursor. The observed difference in 13C between the gas and particle phases may arise from isotope-dependent changes in branching ratios. Alternatively, some gas-phase products involve carbon atoms from highly enriched and depleted sites, giving a non-kinetic origin to the observed fractionations.
Célia J. Sapart, Natalia Shakhova, Igor Semiletov, Joachim Jansen, Sönke Szidat, Denis Kosmach, Oleg Dudarev, Carina van der Veen, Matthias Egger, Valentine Sergienko, Anatoly Salyuk, Vladimir Tumskoy, Jean-Louis Tison, and Thomas Röckmann
Biogeosciences, 14, 2283–2292, https://doi.org/10.5194/bg-14-2283-2017, https://doi.org/10.5194/bg-14-2283-2017, 2017
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The Arctic Ocean, especially the Siberian shelves, overlays large areas of subsea permafrost that is degrading. We show that methane with a biogenic origin is emitted from this permafrost. At locations where bubble plumes have been observed, methane can escape oxidation in the surface sediment and rapidly migrate through the very shallow water column of this region to escape to the atmosphere, generating a positive radiative feedback.
Markella Prokopiou, Patricia Martinerie, Célia J. Sapart, Emmanuel Witrant, Guillaume Monteil, Kentaro Ishijima, Sophie Bernard, Jan Kaiser, Ingeborg Levin, Thomas Blunier, David Etheridge, Ed Dlugokencky, Roderik S. W. van de Wal, and Thomas Röckmann
Atmos. Chem. Phys., 17, 4539–4564, https://doi.org/10.5194/acp-17-4539-2017, https://doi.org/10.5194/acp-17-4539-2017, 2017
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Nitrous oxide is the third most important anthropogenic greenhouse gas with an increasing mole fraction. To understand its natural and anthropogenic sources
we employ isotope measurements. Results show that while the N2O mole fraction increases, its heavy isotope content decreases. The isotopic changes observed underline the dominance of agricultural emissions especially at the early part of the record, whereas in the later decades the contribution from other anthropogenic sources increases.
Ulrike Dusek, Regina Hitzenberger, Anne Kasper-Giebl, Magdalena Kistler, Harro A. J. Meijer, Sönke Szidat, Lukas Wacker, Rupert Holzinger, and Thomas Röckmann
Atmos. Chem. Phys., 17, 3233–3251, https://doi.org/10.5194/acp-17-3233-2017, https://doi.org/10.5194/acp-17-3233-2017, 2017
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Measurements of the radioactive carbon isotope 14C allow to identify the sources of aerosol carbon. We report an extensive 14C source apportionment record in the Netherlands with samples covering a whole year. We discovered that long-range transport has a large influence on aerosol carbon levels. Fossil fuel carbon is least influenced by long-range transport and more regional in origin. Biomass burning seems to be a minor source of aerosol carbon in the Netherlands.
Pearse J. Buchanan, Richard J. Matear, Andrew Lenton, Steven J. Phipps, Zanna Chase, and David M. Etheridge
Clim. Past, 12, 2271–2295, https://doi.org/10.5194/cp-12-2271-2016, https://doi.org/10.5194/cp-12-2271-2016, 2016
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We quantify the contributions of physical and biogeochemical changes in the ocean to enhancing ocean carbon storage at the Last Glacial Maximum. We find that simulated circulation and surface conditions cannot explain changes in carbon storage or other major biogeochemical fields that existed during the glacial climate. Key modifications to the functioning of the biological pump are therefore required to explain the glacial climate and improve model–proxy agreement for all fields.
Bastiaan Jonkheid, Thomas Röckmann, Norbert Glatthor, Christof Janssen, Gabriele Stiller, and Thomas von Clarmann
Atmos. Meas. Tech., 9, 6069–6079, https://doi.org/10.5194/amt-9-6069-2016, https://doi.org/10.5194/amt-9-6069-2016, 2016
Johannes C. Laube, Norfazrin Mohd Hanif, Patricia Martinerie, Eileen Gallacher, Paul J. Fraser, Ray Langenfelds, Carl A. M. Brenninkmeijer, Jakob Schwander, Emmanuel Witrant, Jia-Lin Wang, Chang-Feng Ou-Yang, Lauren J. Gooch, Claire E. Reeves, William T. Sturges, and David E. Oram
Atmos. Chem. Phys., 16, 15347–15358, https://doi.org/10.5194/acp-16-15347-2016, https://doi.org/10.5194/acp-16-15347-2016, 2016
Dorota Janina Mrozek, Carina van der Veen, Magdalena E. G. Hofmann, Huilin Chen, Rigel Kivi, Pauli Heikkinen, and Thomas Röckmann
Atmos. Meas. Tech., 9, 5607–5620, https://doi.org/10.5194/amt-9-5607-2016, https://doi.org/10.5194/amt-9-5607-2016, 2016
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Stratospheric Air Sub-sampler (SAS) is a device to collect and to store the stratospheric profile of air collected with an AirCore (Karion et al., 2010) in numerous sub-samples. The sub-samples (each of 25 mL at ambient temperature and pressure) can be later introduced to the continuous flow systems to measure for example the isotopic composition of CO2. The performance of the coupled system is demonstrated for a set of air samples from an AirCore flight in November 2014 near Sodankylä, Finland.
Beatriz Sayuri Oyama, Maria de Fátima Andrade, Pierre Herckes, Ulrike Dusek, Thomas Röckmann, and Rupert Holzinger
Atmos. Chem. Phys., 16, 14397–14408, https://doi.org/10.5194/acp-16-14397-2016, https://doi.org/10.5194/acp-16-14397-2016, 2016
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Vehicular emissions have a strong impact on air pollution in big cities; hence, the study was performed in São Paulo city, where light- (LDVs) and heavy-duty vehicles (HDVs) run on different fuels. We find that organic aerosol emission from LDVs and HDVs is a complex process involving oxidation of fuel constituents, NOx chemistry, and condensation of unburned fuel hydrocarbons on new or existing particles. The obtained emission patterns can be used to study processing of young aerosol in Brazil.
Matthias Egger, Peter Kraal, Tom Jilbert, Fatimah Sulu-Gambari, Célia J. Sapart, Thomas Röckmann, and Caroline P. Slomp
Biogeosciences, 13, 5333–5355, https://doi.org/10.5194/bg-13-5333-2016, https://doi.org/10.5194/bg-13-5333-2016, 2016
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By combining detailed geochemical analyses with diagenetic modeling, we provide new insights into how methane dynamics may strongly overprint burial records of iron, sulfur and phosphorus in marine systems subject to changes in organic matter loading or water column salinity. A better understanding of these processes will improve our ability to read ancient sediment records and thus to predict the potential consequences of global warming and human-enhanced inputs of nutrients to the ocean.
Cathy M. Trudinger, Paul J. Fraser, David M. Etheridge, William T. Sturges, Martin K. Vollmer, Matt Rigby, Patricia Martinerie, Jens Mühle, David R. Worton, Paul B. Krummel, L. Paul Steele, Benjamin R. Miller, Johannes Laube, Francis S. Mani, Peter J. Rayner, Christina M. Harth, Emmanuel Witrant, Thomas Blunier, Jakob Schwander, Simon O'Doherty, and Mark Battle
Atmos. Chem. Phys., 16, 11733–11754, https://doi.org/10.5194/acp-16-11733-2016, https://doi.org/10.5194/acp-16-11733-2016, 2016
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Perfluorocarbons (PFCs) are potent, long-lived and mostly man-made greenhouse gases released to the atmosphere mainly during aluminium production and semiconductor manufacture. Here we present the first continuous histories of three PFCs from 1800 to 2014, derived from measurements of these PFCs in the atmosphere and in air bubbles in polar ice. The records show how human actions have affected these important greenhouse gases over the past century.
Thomas Röckmann, Simon Eyer, Carina van der Veen, Maria E. Popa, Béla Tuzson, Guillaume Monteil, Sander Houweling, Eliza Harris, Dominik Brunner, Hubertus Fischer, Giulia Zazzeri, David Lowry, Euan G. Nisbet, Willi A. Brand, Jaroslav M. Necki, Lukas Emmenegger, and Joachim Mohn
Atmos. Chem. Phys., 16, 10469–10487, https://doi.org/10.5194/acp-16-10469-2016, https://doi.org/10.5194/acp-16-10469-2016, 2016
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A dual isotope ratio mass spectrometric system (IRMS) and a quantum cascade laser absorption spectroscopy (QCLAS)-based technique were deployed at the Cabauw experimental site for atmospheric research (CESAR) in the Netherlands and performed in situ, high-frequency (approx. hourly) measurements for a period of more than 5 months, yielding a combined dataset with more than 2500 measurements of both δ13C and δD.
Peter Sperlich, Nelly A. M. Uitslag, Jürgen M. Richter, Michael Rothe, Heike Geilmann, Carina van der Veen, Thomas Röckmann, Thomas Blunier, and Willi A. Brand
Atmos. Meas. Tech., 9, 3717–3737, https://doi.org/10.5194/amt-9-3717-2016, https://doi.org/10.5194/amt-9-3717-2016, 2016
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Isotope measurements in atmospheric CH4 are performed since more than 3 decades. However, standard gases to harmonize global measurements are not available to this day. We designed two methods to calibrate a suite of 8 CH4 gases with a wide range in isotopic composition to the VPDB and VSMOW scales with high precision and accuracy. Synthetic air mixtures with ~2 ppm of calibrated CH4 can be provided to the community by the ISOLAB of the Max Planck Institute for Biogeochemistry in Jena, Germany.
Theo Manuel Jenk, Mauro Rubino, David Etheridge, Viorela Gabriela Ciobanu, and Thomas Blunier
Atmos. Meas. Tech., 9, 3687–3706, https://doi.org/10.5194/amt-9-3687-2016, https://doi.org/10.5194/amt-9-3687-2016, 2016
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Atmospheric CO2 and δ13C-CO2 records from polar ice cores provide important constraints on the natural carbon cycle variability. Still, data exist only from a limited number of sampling sites and time periods due to demanding analytical challenges. Additional analytical state-of-the-art resources are desirable. This study describes such a new facility. Its analytical performance and new approaches for dealing with procedural blank contribution and analytical outliers are discussed in detail.
Makoto Inoue, Isamu Morino, Osamu Uchino, Takahiro Nakatsuru, Yukio Yoshida, Tatsuya Yokota, Debra Wunch, Paul O. Wennberg, Coleen M. Roehl, David W. T. Griffith, Voltaire A. Velazco, Nicholas M. Deutscher, Thorsten Warneke, Justus Notholt, John Robinson, Vanessa Sherlock, Frank Hase, Thomas Blumenstock, Markus Rettinger, Ralf Sussmann, Esko Kyrö, Rigel Kivi, Kei Shiomi, Shuji Kawakami, Martine De Mazière, Sabrina G. Arnold, Dietrich G. Feist, Erica A. Barrow, James Barney, Manvendra Dubey, Matthias Schneider, Laura T. Iraci, James R. Podolske, Patrick W. Hillyard, Toshinobu Machida, Yousuke Sawa, Kazuhiro Tsuboi, Hidekazu Matsueda, Colm Sweeney, Pieter P. Tans, Arlyn E. Andrews, Sebastien C. Biraud, Yukio Fukuyama, Jasna V. Pittman, Eric A. Kort, and Tomoaki Tanaka
Atmos. Meas. Tech., 9, 3491–3512, https://doi.org/10.5194/amt-9-3491-2016, https://doi.org/10.5194/amt-9-3491-2016, 2016
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In this study, we correct the biases of GOSAT XCO2 and XCH4 using TCCON data. To evaluate the effectiveness of our correction method, uncorrected/corrected GOSAT data are compared to independent XCO2 and XCH4 data derived from aircraft measurements. Consequently, we suggest that this method is effective for reducing the biases of the GOSAT data. We consider that our work provides GOSAT data users with valuable information and contributes to the further development of studies on greenhouse gases.
Patrick Schlag, Astrid Kiendler-Scharr, Marcus Johannes Blom, Francesco Canonaco, Jeroen Sebastiaan Henzing, Marcel Moerman, André Stephan Henry Prévôt, and Rupert Holzinger
Atmos. Chem. Phys., 16, 8831–8847, https://doi.org/10.5194/acp-16-8831-2016, https://doi.org/10.5194/acp-16-8831-2016, 2016
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This work provides chemical composition data of atmospheric aerosols acquired during 1 year in the rural site of Cabauw, the Netherlands. In some periods, we found unexpected high particle mass concentrations exceeding the WHO limits. Using these composition data, we found that reducing ammonia emissions in this region would largely reduce the main aerosol component ammonium nitrate, whereas the local mitigation of the organics turned out to be difficult due to the lack of a designated source.
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.
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.
Anna Karion, Colm Sweeney, John B. Miller, Arlyn E. Andrews, Roisin Commane, Steven Dinardo, John M. Henderson, Jacob Lindaas, John C. Lin, Kristina A. Luus, Tim Newberger, Pieter Tans, Steven C. Wofsy, Sonja Wolter, and Charles E. Miller
Atmos. Chem. Phys., 16, 5383–5398, https://doi.org/10.5194/acp-16-5383-2016, https://doi.org/10.5194/acp-16-5383-2016, 2016
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Northern high-latitude carbon sources and sinks, including those resulting from degrading permafrost, are thought to be sensitive to the rapidly warming climate. Here we use carbon dioxide and methane measurements from a tower near Fairbanks AK to investigate regional Alaskan fluxes of CO2 and CH4 for 2012–2014.
Sudhanshu Pandey, Sander Houweling, Maarten Krol, Ilse Aben, Frédéric Chevallier, Edward J. Dlugokencky, Luciana V. Gatti, Emanuel Gloor, John B. Miller, Rob Detmers, Toshinobu Machida, and Thomas Röckmann
Atmos. Chem. Phys., 16, 5043–5062, https://doi.org/10.5194/acp-16-5043-2016, https://doi.org/10.5194/acp-16-5043-2016, 2016
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This study investigates the constraint provided by measurements of Xratio (XCH4/XCO2) from space on surface fluxes of CH4 and CO2. We apply the ratio inversion method described in Pandey et al. (2015) to Xratio retrievals from the GOSAT with the TM5-4DVAR inverse modeling system, to constrain the surface fluxes of CH4 and CO2 for 2009 and 2010. The results are compared to proxy CH4 inversions using model-derived-XCO2 mixing ratios from CarbonTracker and MACC.
Reinhard Drews, Joel Brown, Kenichi Matsuoka, Emmanuel Witrant, Morgane Philippe, Bryn Hubbard, and Frank Pattyn
The Cryosphere, 10, 811–823, https://doi.org/10.5194/tc-10-811-2016, https://doi.org/10.5194/tc-10-811-2016, 2016
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The thickness of ice shelves is typically inferred using hydrostatic equilibrium which requires knowledge of the firn density. Here, we infer density from wide-angle radar using a novel algorithm including traveltime inversion and ray tracing. We find that firn is denser inside a 2 km wide ice-shelf channel which is confirmed by optical televiewing of two boreholes. Such horizontal density variations must be accounted for when using the hydrostatic ice thickness for determining basal melt rate.
Armin Rauthe-Schöch, Angela K. Baker, Tanja J. Schuck, Carl A. M. Brenninkmeijer, Andreas Zahn, Markus Hermann, Greta Stratmann, Helmut Ziereis, Peter F. J. van Velthoven, and Jos Lelieveld
Atmos. Chem. Phys., 16, 3609–3629, https://doi.org/10.5194/acp-16-3609-2016, https://doi.org/10.5194/acp-16-3609-2016, 2016
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The flying laboratory CARIBIC onboard a passenger aircraft measured trace gases and aerosol particles in the upper tropospheric Indian summer monsoon anticyclone in summer 2008. We used the measurements together with meteorological analyses to investigate the chemical signature of the northern and southern part of the monsoon, the source regions from where the air was entrained into the monsoon and which parts of the world received polluted air that had been chemically processed in the monsoon.
Narendra Ojha, Andrea Pozzer, Armin Rauthe-Schöch, Angela K. Baker, Jongmin Yoon, Carl A. M. Brenninkmeijer, and Jos Lelieveld
Atmos. Chem. Phys., 16, 3013–3032, https://doi.org/10.5194/acp-16-3013-2016, https://doi.org/10.5194/acp-16-3013-2016, 2016
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We compare simulations of ozone and carbon monoxide using a regional chemistry transport model (WRF-Chem) with aircraft observations from CARIBIC program over India during monsoon period. Sensitivity simulations are conducted to assess the influences of regional emissions and long-range transport.
S. Eyer, B. Tuzson, M. E. Popa, C. van der Veen, T. Röckmann, M. Rothe, W. A. Brand, R. Fisher, D. Lowry, E. G. Nisbet, M. S. Brennwald, E. Harris, C. Zellweger, L. Emmenegger, H. Fischer, and J. Mohn
Atmos. Meas. Tech., 9, 263–280, https://doi.org/10.5194/amt-9-263-2016, https://doi.org/10.5194/amt-9-263-2016, 2016
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We present a newly developed field-deployable, autonomous platform simultaneously measuring the three most abundant isotopologues of methane using mid-infrared laser absorption spectroscopy.
The instrument consists of a compact quantum cascade laser absorption spectrometer (QCLAS) coupled to a preconcentration unit, called TRace gas EXtractor (TREX).
The performance of this new in situ technique was investigated during a 2-week measurement campaign and compared to other techniques.
N. Bândă, M. Krol, M. van Weele, T. van Noije, P. Le Sager, and T. Röckmann
Atmos. Chem. Phys., 16, 195–214, https://doi.org/10.5194/acp-16-195-2016, https://doi.org/10.5194/acp-16-195-2016, 2016
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We quantify the processes responsible for methane growth rate variability in the period 1990 to 1995, a period with variations in climate and radiation due to the Pinatubo eruption. We find significant contributions from changes in the methane emission from wetlands, and in the methane removal by OH caused by stratospheric aerosols, by the decrease in temperature and water vapour, by stratospheric ozone depletion and by changes in emissions of CO and NMVOC.
S. Walter, A. Kock, T. Steinhoff, B. Fiedler, P. Fietzek, J. Kaiser, M. Krol, M. E. Popa, Q. Chen, T. Tanhua, and T. Röckmann
Biogeosciences, 13, 323–340, https://doi.org/10.5194/bg-13-323-2016, https://doi.org/10.5194/bg-13-323-2016, 2016
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Oceans are a source of H2, an indirect greenhouse gas. Measurements constraining the temporal and spatial patterns of oceanic H2 emissions are sparse and although H2 is assumed to be produced mainly biologically, direct evidence for biogenic marine production was lacking. By analyzing the H2 isotopic composition (δD) we were able to constrain the global H2 budget in more detail, verify biogenic production and point to additional sources. We also showed that current models are reasonably working.
S. L. Pathirana, C. van der Veen, M. E. Popa, and T. Röckmann
Atmos. Meas. Tech., 8, 5315–5324, https://doi.org/10.5194/amt-8-5315-2015, https://doi.org/10.5194/amt-8-5315-2015, 2015
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CO is established as an important indirect greenhouse gas, as it is the major sink for the OH∙. We have developed a fully automated system for the determination of δ13C and δ18O in atmospheric CO. The blank signal of the Schütze reagent is 1-3 % of the typical sample size. The repeatability is 0.1 ‰ for δ13C and 0.2 ‰ for δ18O. The analytical repeatability for the mole fraction is ~0.7 nmol mol-1 for 100 mL of ambient air (185.4 nmol mol-1 of CO). A single measurement is performed in 18 min.
S. X. Fang, P. P. Tans, M. Steinbacher, L. X. Zhou, and T. Luan
Atmos. Meas. Tech., 8, 5301–5313, https://doi.org/10.5194/amt-8-5301-2015, https://doi.org/10.5194/amt-8-5301-2015, 2015
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The identification of atmospheric CO2 observation data which are minimally influenced by very local emissions/removals is essential for trend analysis and for the estimation of regional sources and sinks. We compared four data filtering regimes based on the observation records at Lin'an station in China, and found that the use of meteorological parameters was the most favorable. This conclusion will aid regional data selection at the Lin'an station.
J. M. Barlow, P. I. Palmer, L. M. Bruhwiler, and P. Tans
Atmos. Chem. Phys., 15, 13739–13758, https://doi.org/10.5194/acp-15-13739-2015, https://doi.org/10.5194/acp-15-13739-2015, 2015
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The major results from our analysis include (1) a significant revision to previously reported estimates of phase changes in the seasonal cycle atmospheric CO2, which are more closely related to changes in the terrestrial biosphere; and (2) an indirect observation that is consistent with high northern latitude ecosystems progressively taking up more CO2 during spring and early summer.
J. Timkovsky, A. W. H. Chan, T. Dorst, A. H. Goldstein, B. Oyama, and R. Holzinger
Atmos. Meas. Tech., 8, 5177–5187, https://doi.org/10.5194/amt-8-5177-2015, https://doi.org/10.5194/amt-8-5177-2015, 2015
C. Le Quéré, R. Moriarty, R. M. Andrew, J. G. Canadell, S. Sitch, J. I. Korsbakken, P. Friedlingstein, G. P. Peters, R. J. Andres, T. A. Boden, R. A. Houghton, J. I. House, R. F. Keeling, P. Tans, A. Arneth, D. C. E. Bakker, L. Barbero, L. Bopp, J. Chang, F. Chevallier, L. P. Chini, P. Ciais, M. Fader, R. A. Feely, T. Gkritzalis, I. Harris, J. Hauck, T. Ilyina, A. K. Jain, E. Kato, V. Kitidis, K. Klein Goldewijk, C. Koven, P. Landschützer, S. K. Lauvset, N. Lefèvre, A. Lenton, I. D. Lima, N. Metzl, F. Millero, D. R. Munro, A. Murata, J. E. M. S. Nabel, S. Nakaoka, Y. Nojiri, K. O'Brien, A. Olsen, T. Ono, F. F. Pérez, B. Pfeil, D. Pierrot, B. Poulter, G. Rehder, C. Rödenbeck, S. Saito, U. Schuster, J. Schwinger, R. Séférian, T. Steinhoff, B. D. Stocker, A. J. Sutton, T. Takahashi, B. Tilbrook, I. T. van der Laan-Luijkx, G. R. van der Werf, S. van Heuven, D. Vandemark, N. Viovy, A. Wiltshire, S. Zaehle, and N. Zeng
Earth Syst. Sci. Data, 7, 349–396, https://doi.org/10.5194/essd-7-349-2015, https://doi.org/10.5194/essd-7-349-2015, 2015
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Accurate assessment of anthropogenic carbon dioxide emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere is important to understand the global carbon cycle, support the development of climate policies, and project future climate change. We describe data sets and a methodology to quantify all major components of the global carbon budget, including their uncertainties, based on a range of data and models and their interpretation by a broad scientific community.
Q. Chen, M. E. Popa, A. M. Batenburg, and T. Röckmann
Atmos. Chem. Phys., 15, 13003–13021, https://doi.org/10.5194/acp-15-13003-2015, https://doi.org/10.5194/acp-15-13003-2015, 2015
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We investigated soil production and uptake of H2 and associated isotope effects. Uptake and emission of H2 occurred simultaneously at all sampling sites, with strongest emission where N2 fixing legume was present. The fractionation constant during soil uptake was about 0.945 and it did not show positive correlation with deposition velocity. The isotopic composition of H2 emitted from soil with legume was about -530‰, which is less deuterium-depleted than isotope equilibrium between H2O and H2.
R. Holzinger
Atmos. Meas. Tech., 8, 3903–3922, https://doi.org/10.5194/amt-8-3903-2015, https://doi.org/10.5194/amt-8-3903-2015, 2015
S. Pandey, S. Houweling, M. Krol, I. Aben, and T. Röckmann
Atmos. Chem. Phys., 15, 8615–8629, https://doi.org/10.5194/acp-15-8615-2015, https://doi.org/10.5194/acp-15-8615-2015, 2015
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This study attempts to determine the feasibility of a new assimilation method of satellite measurements of CH4 and CO2 for optimization of their surface fluxes in a synthetic environment. Instead of their absolute concentrations, we assimilate the ratios of their concentrations (CH4/CO2) in our inversion. Doing so helps us to reduce the effect of atmospheric scattering on the measurements in our system. However, assimilation of the ratios makes the inversion non-linear.
K. Ishijima, M. Takigawa, K. Sudo, S. Toyoda, N. Yoshida, T. Röckmann, J. Kaiser, S. Aoki, S. Morimoto, S. Sugawara, and T. Nakazawa
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-19947-2015, https://doi.org/10.5194/acpd-15-19947-2015, 2015
Revised manuscript not accepted
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We developed an atmospheric N2O isotopocule model based on a chemistry-coupled atmospheric general circulation model and a simple method to optimize the model, and estimated the isotopic signatures of surface sources at the hemispheric scale. Data obtained from ground-based observations, measurements of firn air, and balloon and aircraft flights were used to optimize the long-term trends, interhemispheric gradients, and photolytic fractionation, respectively, in the model.
B. Lemieux-Dudon, L. Bazin, A. Landais, H. Toyé Mahamadou Kele, M. Guillevic, P. Kindler, F. Parrenin, and P. Martinerie
Clim. Past, 11, 959–978, https://doi.org/10.5194/cp-11-959-2015, https://doi.org/10.5194/cp-11-959-2015, 2015
S. J. Allin, J. C. Laube, E. Witrant, J. Kaiser, E. McKenna, P. Dennis, R. Mulvaney, E. Capron, P. Martinerie, T. Röckmann, T. Blunier, J. Schwander, P. J. Fraser, R. L. Langenfelds, and W. T. Sturges
Atmos. Chem. Phys., 15, 6867–6877, https://doi.org/10.5194/acp-15-6867-2015, https://doi.org/10.5194/acp-15-6867-2015, 2015
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Stratospheric ozone protects life on Earth from harmful UV-B radiation. Chlorofluorocarbons (CFCs) are man-made compounds which act to destroy this barrier.
This paper presents (1) the first measurements of the stratospheric δ(37Cl) of CFCs -11 and -113; (2) the first quantification of long-term trends in the tropospheric δ(37Cl) of CFCs -11, -12 and -113.
This study provides a better understanding of source and sink processes associated with these destructive compounds.
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.
A. L. Ganesan, A. J. Manning, A. Grant, D. Young, D .E. Oram, W. T. Sturges, J. B. Moncrieff, and S. O'Doherty
Atmos. Chem. Phys., 15, 6393–6406, https://doi.org/10.5194/acp-15-6393-2015, https://doi.org/10.5194/acp-15-6393-2015, 2015
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The UK is one of several countries to enact legislation to reduce its greenhouse gas emissions. We present top-down emissions of methane and nitrous oxide for the UK and Ireland over 2012-2014. We inferred average UK emissions of 2.09Tg/yr CH4 and 0.101Tg/yr N2O and used sectoral distributions to determine whether these discrepancies can be attributed to specific source sectors. We found the agricultural sector likely to be overestimated in the bottom-up emissions inventories of both gases.
C. Le Quéré, R. Moriarty, R. M. Andrew, G. P. Peters, P. Ciais, P. Friedlingstein, S. D. Jones, S. Sitch, P. Tans, A. Arneth, T. A. Boden, L. Bopp, Y. Bozec, J. G. Canadell, L. P. Chini, F. Chevallier, C. E. Cosca, I. Harris, M. Hoppema, R. A. Houghton, J. I. House, A. K. Jain, T. Johannessen, E. Kato, R. F. Keeling, V. Kitidis, K. Klein Goldewijk, C. Koven, C. S. Landa, P. Landschützer, A. Lenton, I. D. Lima, G. Marland, J. T. Mathis, N. Metzl, Y. Nojiri, A. Olsen, T. Ono, S. Peng, W. Peters, B. Pfeil, B. Poulter, M. R. Raupach, P. Regnier, C. Rödenbeck, S. Saito, J. E. Salisbury, U. Schuster, J. Schwinger, R. Séférian, J. Segschneider, T. Steinhoff, B. D. Stocker, A. J. Sutton, T. Takahashi, B. Tilbrook, G. R. van der Werf, N. Viovy, Y.-P. Wang, R. Wanninkhof, A. Wiltshire, and N. Zeng
Earth Syst. Sci. Data, 7, 47–85, https://doi.org/10.5194/essd-7-47-2015, https://doi.org/10.5194/essd-7-47-2015, 2015
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Carbon dioxide (CO2) emissions from human activities (burning fossil fuels and cement production, deforestation and other land-use change) are set to rise again in 2014.
This study (updated yearly) makes an accurate assessment of anthropogenic CO2 emissions and their redistribution between the atmosphere, ocean, and terrestrial biosphere in order to better understand the global carbon cycle, support the development of climate policies, and project future climate change.
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
A. P. Ballantyne, R. Andres, R. Houghton, B. D. Stocker, R. Wanninkhof, W. Anderegg, L. A. Cooper, M. DeGrandpre, P. P. Tans, J. B. Miller, C. Alden, and J. W. C. White
Biogeosciences, 12, 2565–2584, https://doi.org/10.5194/bg-12-2565-2015, https://doi.org/10.5194/bg-12-2565-2015, 2015
R. J. Matear, A. Lenton, D. Etheridge, and S. J. Phipps
Clim. Past Discuss., https://doi.org/10.5194/cpd-11-1093-2015, https://doi.org/10.5194/cpd-11-1093-2015, 2015
Revised manuscript has not been submitted
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Global climate models provide an important tool for simulating the earth's climate. Here we present a simulation of the climate of the Last Glacial Maximum, which was obtained by setting atmospheric greenhouse gas concentrations and the earth's orbital parameters to the 21 000 years before present values. We simulate an ocean behaviour that agrees with paleoclimate reconstructions supporting our ability to model the climate system and use the model to explore the impacts on the carbon cycle.
F. A. Stap, O. P. Hasekamp, and T. Röckmann
Atmos. Meas. Tech., 8, 1287–1301, https://doi.org/10.5194/amt-8-1287-2015, https://doi.org/10.5194/amt-8-1287-2015, 2015
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We present the capability of an aerosol retrieval algorithm, intended for multi-angle, multi-wavelength photopolarimetric measurements, to intrinsically screen for sub-pixel liquid water cloud contamination.
The screening is based on goodness-of-fit criteria. The algorithm has been applied to a synthetic data set of partially clouded scenes and (non-cloud-screened) POLDER3/PARASOL observations.
A. Ghosh, P. K. Patra, K. Ishijima, T. Umezawa, A. Ito, D. M. Etheridge, S. Sugawara, K. Kawamura, J. B. Miller, E. J. Dlugokencky, P. B. Krummel, P. J. Fraser, L. P. Steele, R. L. Langenfelds, C. M. Trudinger, J. W. C. White, B. Vaughn, T. Saeki, S. Aoki, and T. Nakazawa
Atmos. Chem. Phys., 15, 2595–2612, https://doi.org/10.5194/acp-15-2595-2015, https://doi.org/10.5194/acp-15-2595-2015, 2015
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Atmospheric CH4 increased from 900ppb to 1800ppb during the period 1900–2010 at a rate unprecedented in any observational records. We use bottom-up emissions and a chemistry-transport model to simulate CH4. The optimized global total CH4 emission, estimated from the model–observation differences, increased at fastest rate during 1940–1990. Using δ13C of CH4 measurements we attribute this emission increase to biomass burning. Total CH4 lifetime is shortened by 4% over the simulation period.
S. J. Sutanto, G. Hoffmann, R. A. Scheepmaker, J. Worden, S. Houweling, K. Yoshimura, I. Aben, and T. Röckmann
Atmos. Meas. Tech., 8, 999–1019, https://doi.org/10.5194/amt-8-999-2015, https://doi.org/10.5194/amt-8-999-2015, 2015
Emma C. Leedham Elvidge, D. E. Oram, J. C. Laube, A. K. Baker, S. A. Montzka, S. Humphrey, D. A. O'Sullivan, and C. A. M. Brenninkmeijer
Atmos. Chem. Phys., 15, 1939–1958, https://doi.org/10.5194/acp-15-1939-2015, https://doi.org/10.5194/acp-15-1939-2015, 2015
D. J. Mrozek, C. van der Veen, M. Kliphuis, J. Kaiser, A. A. Wiegel, and T. Röckmann
Atmos. Meas. Tech., 8, 811–822, https://doi.org/10.5194/amt-8-811-2015, https://doi.org/10.5194/amt-8-811-2015, 2015
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Our analytical system is a promising tool for investigating the triple oxygen isotope composition of CO2 from stratospheric air samples of volumes 100ml and smaller. The method is designed for measuring air samples with CO2 mole fractions between 360 and 400ppm, and it is the first fully automated analytical system that uses CeO2 as the isotope exchange medium.
Emma C. Leedham Elvidge, S.-M. Phang, W. T. Sturges, and G. Malin
Biogeosciences, 12, 387–398, https://doi.org/10.5194/bg-12-387-2015, https://doi.org/10.5194/bg-12-387-2015, 2015
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.
K. A. Masarie, W. Peters, A. R. Jacobson, and P. P. Tans
Earth Syst. Sci. Data, 6, 375–384, https://doi.org/10.5194/essd-6-375-2014, https://doi.org/10.5194/essd-6-375-2014, 2014
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Observation Package (ObsPack) is a framework designed to bring together atmospheric greenhouse gas measurements from a variety of sampling platforms, prepare them with specific applications in mind, and package and distribute them in a self-consistent and well-documented product. The framework includes a unique distribution stategy designed to improve communication between product users and data providers. The concepts presented are general and may be easily applied to other scientific data.
M. Inoue, I. Morino, O. Uchino, Y. Miyamoto, T. Saeki, Y. Yoshida, T. Yokota, C. Sweeney, P. P. Tans, S. C. Biraud, T. Machida, J. V. Pittman, E. A. Kort, T. Tanaka, S. Kawakami, Y. Sawa, K. Tsuboi, and H. Matsueda
Atmos. Meas. Tech., 7, 2987–3005, https://doi.org/10.5194/amt-7-2987-2014, https://doi.org/10.5194/amt-7-2987-2014, 2014
L. Bruhwiler, E. Dlugokencky, K. Masarie, M. Ishizawa, A. Andrews, J. Miller, C. Sweeney, P. Tans, and D. Worthy
Atmos. Chem. Phys., 14, 8269–8293, https://doi.org/10.5194/acp-14-8269-2014, https://doi.org/10.5194/acp-14-8269-2014, 2014
M. S. Mohd Nadzir, S. M. Phang, M. R. Abas, N. Abdul Rahman, A. Abu Samah, W. T. Sturges, D. E. Oram, G. P. Mills, Emma C. Leedham Elvidge, J. A. Pyle, N. R. P. Harris, A. D. Robinson, M. J. Ashfold, M. I. Mead, M. T. Latif, M. F. Khan, A. M. Amiruddin, N. Banan, and M. M. Hanafiah
Atmos. Chem. Phys., 14, 8137–8148, https://doi.org/10.5194/acp-14-8137-2014, https://doi.org/10.5194/acp-14-8137-2014, 2014
S. J. Sutanto, B. van den Hurk, P. A. Dirmeyer, S. I. Seneviratne, T. Röckmann, K. E. Trenberth, E. M. Blyth, J. Wenninger, and G. Hoffmann
Hydrol. Earth Syst. Sci., 18, 2815–2827, https://doi.org/10.5194/hess-18-2815-2014, https://doi.org/10.5194/hess-18-2815-2014, 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
U. Dusek, M. Monaco, M. Prokopiou, F. Gongriep, R. Hitzenberger, H. A. J. Meijer, and T. Röckmann
Atmos. Meas. Tech., 7, 1943–1955, https://doi.org/10.5194/amt-7-1943-2014, https://doi.org/10.5194/amt-7-1943-2014, 2014
A. J. van Beelen, G. J. H. Roelofs, O. P. Hasekamp, J. S. Henzing, and T. Röckmann
Atmos. Chem. Phys., 14, 5969–5987, https://doi.org/10.5194/acp-14-5969-2014, https://doi.org/10.5194/acp-14-5969-2014, 2014
C. Le Quéré, G. P. Peters, R. J. Andres, R. M. Andrew, T. A. Boden, P. Ciais, P. Friedlingstein, R. A. Houghton, G. Marland, R. Moriarty, S. Sitch, P. Tans, A. Arneth, A. Arvanitis, D. C. E. Bakker, L. Bopp, J. G. Canadell, L. P. Chini, S. C. Doney, A. Harper, I. Harris, J. I. House, A. K. Jain, S. D. Jones, E. Kato, R. F. Keeling, K. Klein Goldewijk, A. Körtzinger, C. Koven, N. Lefèvre, F. Maignan, A. Omar, T. Ono, G.-H. Park, B. Pfeil, B. Poulter, M. R. Raupach, P. Regnier, C. Rödenbeck, S. Saito, J. Schwinger, J. Segschneider, B. D. Stocker, T. Takahashi, B. Tilbrook, S. van Heuven, N. Viovy, R. Wanninkhof, A. Wiltshire, and S. Zaehle
Earth Syst. Sci. Data, 6, 235–263, https://doi.org/10.5194/essd-6-235-2014, https://doi.org/10.5194/essd-6-235-2014, 2014
O. Peltola, A. Hensen, C. Helfter, L. Belelli Marchesini, F. C. Bosveld, W. C. M. van den Bulk, J. A. Elbers, S. Haapanala, J. Holst, T. Laurila, A. Lindroth, E. Nemitz, T. Röckmann, A. T. Vermeulen, and I. Mammarella
Biogeosciences, 11, 3163–3186, https://doi.org/10.5194/bg-11-3163-2014, https://doi.org/10.5194/bg-11-3163-2014, 2014
H. F. Zhang, B. Z. Chen, I. T. van der Laan-Luijk, T. Machida, H. Matsueda, Y. Sawa, Y. Fukuyama, R. Langenfelds, M. van der Schoot, G. Xu, J. W. Yan, M. L. Cheng, L. X. Zhou, P. P. Tans, and W. Peters
Atmos. Chem. Phys., 14, 5807–5824, https://doi.org/10.5194/acp-14-5807-2014, https://doi.org/10.5194/acp-14-5807-2014, 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
S. Houweling, M. Krol, P. Bergamaschi, C. Frankenberg, E. J. Dlugokencky, I. Morino, J. Notholt, V. Sherlock, D. Wunch, V. Beck, C. Gerbig, H. Chen, E. A. Kort, T. Röckmann, and I. Aben
Atmos. Chem. Phys., 14, 3991–4012, https://doi.org/10.5194/acp-14-3991-2014, https://doi.org/10.5194/acp-14-3991-2014, 2014
B. Ringeval, S. Houweling, P. M. van Bodegom, R. Spahni, R. van Beek, F. Joos, and T. Röckmann
Biogeosciences, 11, 1519–1558, https://doi.org/10.5194/bg-11-1519-2014, https://doi.org/10.5194/bg-11-1519-2014, 2014
S. X. Fang, L. X. Zhou, P. P. Tans, P. Ciais, M. Steinbacher, L. Xu, and T. Luan
Atmos. Chem. Phys., 14, 2541–2554, https://doi.org/10.5194/acp-14-2541-2014, https://doi.org/10.5194/acp-14-2541-2014, 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
A. E. Andrews, J. D. Kofler, M. E. Trudeau, J. C. Williams, D. H. Neff, K. A. Masarie, D. Y. Chao, D. R. Kitzis, P. C. Novelli, C. L. Zhao, E. J. Dlugokencky, P. M. Lang, M. J. Crotwell, M. L. Fischer, M. J. Parker, J. T. Lee, D. D. Baumann, A. R. Desai, C. O. Stanier, S. F. J. De Wekker, D. E. Wolfe, J. W. Munger, and P. P. Tans
Atmos. Meas. Tech., 7, 647–687, https://doi.org/10.5194/amt-7-647-2014, https://doi.org/10.5194/amt-7-647-2014, 2014
M. E. Popa, M. K. Vollmer, A. Jordan, W. A. Brand, S. L. Pathirana, M. Rothe, and T. Röckmann
Atmos. Chem. Phys., 14, 2105–2123, https://doi.org/10.5194/acp-14-2105-2014, https://doi.org/10.5194/acp-14-2105-2014, 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
B. W. LaFranchi, G. Pétron, J. B. Miller, S. J. Lehman, A. E. Andrews, E. J. Dlugokencky, B. Hall, B. R. Miller, S. A. Montzka, W. Neff, P. C. Novelli, C. Sweeney, J. C. Turnbull, D. E. Wolfe, P. P. Tans, K. R. Gurney, and T. P. Guilderson
Atmos. Chem. Phys., 13, 11101–11120, https://doi.org/10.5194/acp-13-11101-2013, https://doi.org/10.5194/acp-13-11101-2013, 2013
J. Timkovsky, P. Gankema, R. Pierik, and R. Holzinger
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amtd-6-9005-2013, https://doi.org/10.5194/amtd-6-9005-2013, 2013
Preprint withdrawn
R. Holzinger, A. H. Goldstein, P. L. Hayes, J. L. Jimenez, and J. Timkovsky
Atmos. Chem. Phys., 13, 10125–10141, https://doi.org/10.5194/acp-13-10125-2013, https://doi.org/10.5194/acp-13-10125-2013, 2013
M. Inoue, I. Morino, O. Uchino, Y. Miyamoto, Y. Yoshida, T. Yokota, T. Machida, Y. Sawa, H. Matsueda, C. Sweeney, P. P. Tans, A. E. Andrews, S. C. Biraud, T. Tanaka, S. Kawakami, and P. K. Patra
Atmos. Chem. Phys., 13, 9771–9788, https://doi.org/10.5194/acp-13-9771-2013, https://doi.org/10.5194/acp-13-9771-2013, 2013
F. A. Haumann, A. M. Batenburg, G. Pieterse, C. Gerbig, M. C. Krol, and T. Röckmann
Atmos. Chem. Phys., 13, 9401–9413, https://doi.org/10.5194/acp-13-9401-2013, https://doi.org/10.5194/acp-13-9401-2013, 2013
M. von Hobe, S. Bekki, S. Borrmann, F. Cairo, F. D'Amato, G. Di Donfrancesco, A. Dörnbrack, A. Ebersoldt, M. Ebert, C. Emde, I. Engel, M. Ern, W. Frey, S. Genco, S. Griessbach, J.-U. Grooß, T. Gulde, G. Günther, E. Hösen, L. Hoffmann, V. Homonnai, C. R. Hoyle, I. S. A. Isaksen, D. R. Jackson, I. M. Jánosi, R. L. Jones, K. Kandler, C. Kalicinsky, A. Keil, S. M. Khaykin, F. Khosrawi, R. Kivi, J. Kuttippurath, J. C. Laube, F. Lefèvre, R. Lehmann, S. Ludmann, B. P. Luo, M. Marchand, J. Meyer, V. Mitev, S. Molleker, R. Müller, H. Oelhaf, F. Olschewski, Y. Orsolini, T. Peter, K. Pfeilsticker, C. Piesch, M. C. Pitts, L. R. Poole, F. D. Pope, F. Ravegnani, M. Rex, M. Riese, T. Röckmann, B. Rognerud, A. Roiger, C. Rolf, M. L. Santee, M. Scheibe, C. Schiller, H. Schlager, M. Siciliani de Cumis, N. Sitnikov, O. A. Søvde, R. Spang, N. Spelten, F. Stordal, O. Sumińska-Ebersoldt, A. Ulanovski, J. Ungermann, S. Viciani, C. M. Volk, M. vom Scheidt, P. von der Gathen, K. Walker, T. Wegner, R. Weigel, S. Weinbruch, G. Wetzel, F. G. Wienhold, I. Wohltmann, W. Woiwode, I. A. K. Young, V. Yushkov, B. Zobrist, and F. Stroh
Atmos. Chem. Phys., 13, 9233–9268, https://doi.org/10.5194/acp-13-9233-2013, https://doi.org/10.5194/acp-13-9233-2013, 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. Sperlich, C. Buizert, T. M. Jenk, C. J. Sapart, M. Prokopiou, T. Röckmann, and T. Blunier
Atmos. Meas. Tech., 6, 2027–2041, https://doi.org/10.5194/amt-6-2027-2013, https://doi.org/10.5194/amt-6-2027-2013, 2013
V. V. Petrenko, P. Martinerie, P. Novelli, D. M. Etheridge, I. Levin, Z. Wang, T. Blunier, J. Chappellaz, J. Kaiser, P. Lang, L. P. Steele, S. Hammer, J. Mak, R. L. Langenfelds, J. Schwander, J. P. Severinghaus, E. Witrant, G. Petron, M. O. Battle, G. Forster, W. T. Sturges, J.-F. Lamarque, K. Steffen, and J. W. C. White
Atmos. Chem. Phys., 13, 7567–7585, https://doi.org/10.5194/acp-13-7567-2013, https://doi.org/10.5194/acp-13-7567-2013, 2013
L. Bazin, A. Landais, B. Lemieux-Dudon, H. Toyé Mahamadou Kele, D. Veres, F. Parrenin, P. Martinerie, C. Ritz, E. Capron, V. Lipenkov, M.-F. Loutre, D. Raynaud, B. Vinther, A. Svensson, S. O. Rasmussen, M. Severi, T. Blunier, M. Leuenberger, H. Fischer, V. Masson-Delmotte, J. Chappellaz, and E. Wolff
Clim. Past, 9, 1715–1731, https://doi.org/10.5194/cp-9-1715-2013, https://doi.org/10.5194/cp-9-1715-2013, 2013
D. Veres, L. Bazin, A. Landais, H. Toyé Mahamadou Kele, B. Lemieux-Dudon, F. Parrenin, P. Martinerie, E. Blayo, T. Blunier, E. Capron, J. Chappellaz, S. O. Rasmussen, M. Severi, A. Svensson, B. Vinther, and E. W. Wolff
Clim. Past, 9, 1733–1748, https://doi.org/10.5194/cp-9-1733-2013, https://doi.org/10.5194/cp-9-1733-2013, 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
X. Faïn, D. Helmig, J. Hueber, D. Obrist, and M. W. Williams
Biogeosciences, 10, 3793–3807, https://doi.org/10.5194/bg-10-3793-2013, https://doi.org/10.5194/bg-10-3793-2013, 2013
Emma C. Leedham Elvidge, C. Hughes, F. S. L. Keng, S.-M. Phang, G. Malin, and W. T. Sturges
Biogeosciences, 10, 3615–3633, https://doi.org/10.5194/bg-10-3615-2013, https://doi.org/10.5194/bg-10-3615-2013, 2013
Y. Miyamoto, M. Inoue, I. Morino, O. Uchino, T. Yokota, T. Machida, Y. Sawa, H. Matsueda, C. Sweeney, P. P. Tans, A. E. Andrews, and P. K. Patra
Atmos. Chem. Phys., 13, 5265–5275, https://doi.org/10.5194/acp-13-5265-2013, https://doi.org/10.5194/acp-13-5265-2013, 2013
J. Schmitt, B. Seth, M. Bock, C. van der Veen, L. Möller, C. J. Sapart, M. Prokopiou, T. Sowers, T. Röckmann, and H. Fischer
Atmos. Meas. Tech., 6, 1425–1445, https://doi.org/10.5194/amt-6-1425-2013, https://doi.org/10.5194/amt-6-1425-2013, 2013
S. Walter, A. Kock, and T. Röckmann
Biogeosciences, 10, 3391–3403, https://doi.org/10.5194/bg-10-3391-2013, https://doi.org/10.5194/bg-10-3391-2013, 2013
M. Guillevic, L. Bazin, A. Landais, P. Kindler, A. Orsi, V. Masson-Delmotte, T. Blunier, S. L. Buchardt, E. Capron, M. Leuenberger, P. Martinerie, F. Prié, and B. M. Vinther
Clim. Past, 9, 1029–1051, https://doi.org/10.5194/cp-9-1029-2013, https://doi.org/10.5194/cp-9-1029-2013, 2013
E. Capron, A. Landais, D. Buiron, A. Cauquoin, J. Chappellaz, M. Debret, J. Jouzel, M. Leuenberger, P. Martinerie, V. Masson-Delmotte, R. Mulvaney, F. Parrenin, and F. Prié
Clim. Past, 9, 983–999, https://doi.org/10.5194/cp-9-983-2013, https://doi.org/10.5194/cp-9-983-2013, 2013
H. Chen, A. Karion, C. W. Rella, J. Winderlich, C. Gerbig, A. Filges, T. Newberger, C. Sweeney, and P. P. Tans
Atmos. Meas. Tech., 6, 1031–1040, https://doi.org/10.5194/amt-6-1031-2013, https://doi.org/10.5194/amt-6-1031-2013, 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
S. C. Biraud, M. S. Torn, J. R. Smith, C. Sweeney, W. J. Riley, and P. P. Tans
Atmos. Meas. Tech., 6, 751–763, https://doi.org/10.5194/amt-6-751-2013, https://doi.org/10.5194/amt-6-751-2013, 2013
J. C. Laube, A. Keil, H. Bönisch, A. Engel, T. Röckmann, C. M. Volk, and W. T. Sturges
Atmos. Chem. Phys., 13, 2779–2791, https://doi.org/10.5194/acp-13-2779-2013, https://doi.org/10.5194/acp-13-2779-2013, 2013
A. Karion, C. Sweeney, S. Wolter, T. Newberger, H. Chen, A. Andrews, J. Kofler, D. Neff, and P. Tans
Atmos. Meas. Tech., 6, 511–526, https://doi.org/10.5194/amt-6-511-2013, https://doi.org/10.5194/amt-6-511-2013, 2013
N. Bândă, M. Krol, M. van Weele, T. van Noije, and T. Röckmann
Atmos. Chem. Phys., 13, 2267–2281, https://doi.org/10.5194/acp-13-2267-2013, https://doi.org/10.5194/acp-13-2267-2013, 2013
C. M. Trudinger, I. G. Enting, P. J. Rayner, D. M. Etheridge, C. Buizert, M. Rubino, P. B. Krummel, and T. Blunier
Atmos. Chem. Phys., 13, 1485–1510, https://doi.org/10.5194/acp-13-1485-2013, https://doi.org/10.5194/acp-13-1485-2013, 2013
J.-H. Park, A. H. Goldstein, J. Timkovsky, S. Fares, R. Weber, J. Karlik, and R. Holzinger
Atmos. Chem. Phys., 13, 1439–1456, https://doi.org/10.5194/acp-13-1439-2013, https://doi.org/10.5194/acp-13-1439-2013, 2013
Related subject area
Subject: Gases | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Flaring efficiencies and NOx emission ratios measured for offshore oil and gas facilities in the North Sea
Measurement report: Long-range transport and the fate of dimethyl sulfide oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes
Formaldehyde and hydroperoxide distribution around the Arabian Peninsula – evaluation of EMAC model results with ship-based measurements
Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements – corrected
Fundamental oxidation processes in the remote marine atmosphere investigated using the NO–NO2–O3 photostationary state
Emission factors and evolution of SO2 measured from biomass burning in wildfires and agricultural fires
The unexpected high frequency of nocturnal surface ozone enhancement events over China: characteristics and mechanisms
Source apportionment of VOCs, IVOCs and SVOCs by positive matrix factorization in suburban Livermore, California
Measurement report: Intra- and interannual variability and source apportionment of volatile organic compounds during 2018–2020 in Zhengzhou, central China
Formation and impacts of nitryl chloride in Pearl River Delta
Multidecadal increases in global tropospheric ozone derived from ozonesonde and surface site observations: can models reproduce ozone trends?
What caused ozone pollution during the 2022 Shanghai lockdown? Insights from ground and satellite observations
Ammonium adduct chemical ionization to investigate anthropogenic oxygenated gas-phase organic compounds in urban air
Atmospheric biogenic volatile organic compounds in the Alaskan Arctic tundra: constraints from measurements at Toolik Field Station
Are dense networks of low-cost nodes really useful for monitoring air pollution? A case study in Staffordshire
Pandemic Restrictions in 2020 highlight the significance of non-road NOx sources in central London
Technical note: Northern midlatitude baseline ozone – long-term changes and the COVID-19 impact
Quantifying the importance of vehicle ammonia emissions in an urban area of northeastern USA utilizing nitrogen isotopes
Seasonal variation in nitryl chloride and its relation to gas-phase precursors during the JULIAC campaign in Germany
O3-precursor relationship over multiple patterns of time scale: A case study in Zibo, Shandong Province, China
Radical chemistry in the Pearl River Delta: observations and modeling of OH and HO2 radicals in Shenzhen in 2018
Reconciling the total carbon budget for boreal forest wildfire emissions using airborne observations
Summer variability of the atmospheric NO2 : NO ratio at Dome C on the East Antarctic Plateau
Measurement report: Ambient volatile organic compound (VOC) pollution in urban Beijing: characteristics, sources, and implications for pollution control
Mass spectrometric measurements of ambient ions and estimation of gaseous sulfuric acid in the free troposphere and lowermost stratosphere during the CAFE-EU/BLUESKY campaign
Springtime nitrogen oxides and tropospheric ozone in Svalbard: results from the measurement station network
Measurement report: Observations of long-lived volatile organic compounds from the 2019–2020 Australian wildfires during the COALA campaign
Experimental chemical budgets of OH, HO2 and RO2 radicals in rural air in West-Germany during the JULIAC campaign 2019
Composition and reactivity of volatile organic compounds in the South Coast Air Basin and San Joaquin Valley of California
Analysis of regional CO2 contributions at the high Alpine observatory Jungfraujoch by means of atmospheric transport simulations and δ13C
Variations and sources of volatile organic compounds (VOCs) in urban region: insights from measurements on a tall tower
Elucidate the Formation Mechanism of Particulate Nitrate Based on Direct Radical Observations in Yangtze River Delta summer 2019
Tropical peat fire emissions: 2019 field measurements in Sumatra and Borneo and synthesis with previous studies
Sulfuric acid in the Amazon basin: measurements and evaluation of existing sulfuric acid proxies
Seasonal variation in oxygenated organic molecules in urban Beijing and their contribution to secondary organic aerosol
Oxygenated volatile organic compounds (VOCs) as significant but varied contributors to VOC emissions from vehicles
The impacts of wildfires on ozone production and boundary layer dynamics in California's Central Valley
Distribution of hydrogen peroxide over Europe during the BLUESKY aircraft campaign
Eddy covariance measurements highlight sources of nitrogen oxide emissions missing from inventories for central London
Chemical and dynamical identification of emission outflows during the HALO campaign EMeRGe in Europe and Asia
Budget of nitrous acid (HONO) at an urban site in the fall season of Guangzhou, China
Long-term trend of ozone pollution in China during 2014–2020: distinct seasonal and spatial characteristics and ozone sensitivity
Investigation of new particle formation mechanisms and aerosol processes at Marambio Station, Antarctic Peninsula
Measurement report: Variations in surface SO2 and NOx mixing ratios from 2004 to 2016 at a background site in the North China Plain
Fate of the nitrate radical at the summit of a semi-rural mountain site in Germany assessed with direct reactivity measurements
Spatiotemporal variations of the δ(O2 ∕ N2), CO2 and δ(APO) in the troposphere over the western North Pacific
OH and HO2 radical chemistry at a suburban site during the EXPLORE-YRD campaign in 2018
Towards reconstructing the Arctic atmospheric methane history over the 20th century: measurement and modelling results for the North Greenland Ice Core Project firn
Atmospheric gas-phase composition over the Indian Ocean
Joint occurrence of heatwaves and ozone pollution and increased health risks in Beijing, China: role of synoptic weather pattern and urbanization
Jacob T. Shaw, Amy Foulds, Shona Wilde, Patrick Barker, Freya A. Squires, James Lee, Ruth Purvis, Ralph Burton, Ioana Colfescu, Stephen Mobbs, Samuel Cliff, Stéphane J.-B. Bauguitte, Stuart Young, Stefan Schwietzke, and Grant Allen
Atmos. Chem. Phys., 23, 1491–1509, https://doi.org/10.5194/acp-23-1491-2023, https://doi.org/10.5194/acp-23-1491-2023, 2023
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Flaring is used by the oil and gas sector to dispose of unwanted natural gas or for safety. However, few studies have assessed the efficiency with which the gas is combusted. We sampled flaring emissions from offshore facilities in the North Sea. Average measured flaring efficiencies were ~ 98 % but with a skewed distribution, including many flares of lower efficiency. NOx and ethane emissions were also measured. Inefficient flaring practices could be a target for mitigating carbon emissions.
Wiebke Scholz, Jiali Shen, Diego Aliaga, Cheng Wu, Samara Carbone, Isabel Moreno, Qiaozhi Zha, Wei Huang, Liine Heikkinen, Jean Luc Jaffrezo, Gaelle Uzu, Eva Partoll, Markus Leiminger, Fernando Velarde, Paolo Laj, Patrick Ginot, Paolo Artaxo, Alfred Wiedensohler, Markku Kulmala, Claudia Mohr, Marcos Andrade, Victoria Sinclair, Federico Bianchi, and Armin Hansel
Atmos. Chem. Phys., 23, 895–920, https://doi.org/10.5194/acp-23-895-2023, https://doi.org/10.5194/acp-23-895-2023, 2023
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Dimethyl sulfide (DMS), emitted from the ocean, is the most abundant biogenic sulfur emission into the atmosphere. OH radicals, among others, can oxidize DMS to sulfuric and methanesulfonic acid, which are relevant for aerosol formation. We quantified DMS and nearly all DMS oxidation products with novel mass spectrometric instruments for gas and particle phase at the high mountain station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes in free tropospheric air after long-range transport.
Dirk Dienhart, Bettina Brendel, John N. Crowley, Philipp G. Eger, Hartwig Harder, Monica Martinez, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Sebastian Tauer, David Walter, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 119–142, https://doi.org/10.5194/acp-23-119-2023, https://doi.org/10.5194/acp-23-119-2023, 2023
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Formaldehyde and hydroperoxide measurements were performed in the marine boundary layer around the Arabian Peninsula and highlight the Suez Canal and Arabian (Persian) Gulf as a hotspot of photochemical air pollution. A comparison with the EMAC model shows that the formaldehyde results match within a factor of 2, while hydrogen peroxide was overestimated by more than a factor of 5, which revealed enhanced HOx (OH+HO2) radicals in the simulation and an underestimation of dry deposition velocites.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Simone T. Andersen, Beth S. Nelson, Katie A. Read, Shalini Punjabi, Luis Neves, Matthew J. Rowlinson, James Hopkins, Tomás Sherwen, Lisa K. Whalley, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 22, 15747–15765, https://doi.org/10.5194/acp-22-15747-2022, https://doi.org/10.5194/acp-22-15747-2022, 2022
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The cycling of NO and NO2 is important to understand to be able to predict O3 concentrations in the atmosphere. We have used long-term measurements from the Cape Verde Atmospheric Observatory together with model outputs to investigate the cycling of nitrogen oxide (NO) and nitrogen dioxide (NO2) in very clean marine air. This study shows that we understand the processes occurring in very clean air, but with small amounts of pollution in the air, known chemistry cannot explain what is observed.
Pamela S. Rickly, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Glenn M. Wolfe, Ryan Bennett, Ilann Bourgeois, John D. Crounse, Jack E. Dibb, Joshua P. DiGangi, Glenn S. Diskin, Maximilian Dollner, Emily M. Gargulinski, Samuel R. Hall, Hannah S. Halliday, Thomas F. Hanisco, Reem A. Hannun, Jin Liao, Richard Moore, Benjamin A. Nault, John B. Nowak, Jeff Peischl, Claire E. Robinson, Thomas Ryerson, Kevin J. Sanchez, Manuel Schöberl, Amber J. Soja, Jason M. St. Clair, Kenneth L. Thornhill, Kirk Ullmann, Paul O. Wennberg, Bernadett Weinzierl, Elizabeth B. Wiggins, Edward L. Winstead, and Andrew W. Rollins
Atmos. Chem. Phys., 22, 15603–15620, https://doi.org/10.5194/acp-22-15603-2022, https://doi.org/10.5194/acp-22-15603-2022, 2022
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Biomass burning sulfur dioxide (SO2) emission factors range from 0.27–1.1 g kg-1 C. Biomass burning SO2 can quickly form sulfate and organosulfur, but these pathways are dependent on liquid water content and pH. Hydroxymethanesulfonate (HMS) appears to be directly emitted from some fire sources but is not the sole contributor to the organosulfur signal. It is shown that HMS and organosulfur chemistry may be an important S(IV) reservoir with the fate dependent on the surrounding conditions.
Cheng He, Xiao Lu, Haolin Wang, Haichao Wang, Yan Li, Guowen He, Yuanping He, Yurun Wang, Youlang Zhang, Yiming Liu, Qi Fan, and Shaojia Fan
Atmos. Chem. Phys., 22, 15243–15261, https://doi.org/10.5194/acp-22-15243-2022, https://doi.org/10.5194/acp-22-15243-2022, 2022
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We report that nocturnal ozone enhancement (NOE) events are observed at a high annual frequency of 41 % over 800 sites in China in 2014–2019 (about 50 % higher than that over Europe or the US). High daytime ozone provides a rich ozone source in the nighttime residual layer, determining the overall high frequency of NOE events in China, and enhanced atmospheric mixing then triggers NOE events by allowing the ozone-rich air in the residual layer to be mixed into the nighttime boundary layer.
Rebecca A. Wernis, Nathan M. Kreisberg, Robert J. Weber, Greg T. Drozd, and Allen H. Goldstein
Atmos. Chem. Phys., 22, 14987–15019, https://doi.org/10.5194/acp-22-14987-2022, https://doi.org/10.5194/acp-22-14987-2022, 2022
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We measured volatile and intermediate-volatility gases and semivolatile gas- and particle-phase compounds in the atmosphere during an 11 d period in a Bay Area suburb. We separated compounds based on variability in time to arrive at 13 distinct sources. Some compounds emitted from plants are found in greater quantities as fragrance compounds in consumer products. The wide volatility range of these measurements enables the construction of more complete source profiles.
Shijie Yu, Shenbo Wang, Ruixin Xu, Dong Zhang, Meng Zhang, Fangcheng Su, Xuan Lu, Xiao Li, Ruiqin Zhang, and Lingling Wang
Atmos. Chem. Phys., 22, 14859–14878, https://doi.org/10.5194/acp-22-14859-2022, https://doi.org/10.5194/acp-22-14859-2022, 2022
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In this study, the hourly data of 57 VOC species were collected during 2018–2020 at an urban site in Zhengzhou, China. The research of concentrations, source apportionment, and atmospheric environmental implications clearly elucidated the differences in major reactants observed in different seasons and years. Therefore, the control strategy should focus on key species and sources among interannual and seasonal variations. The results can provide references to develop control strategies.
Haichao Wang, Bin Yuan, E Zheng, Xiaoxiao Zhang, Jie Wang, Keding Lu, Chenshuo Ye, Lei Yang, Shan Huang, Weiwei Hu, Suxia Yang, Yuwen Peng, Jipeng Qi, Sihang Wang, Xianjun He, Yubin Chen, Tiange Li, Wenjie Wang, Yibo Huangfu, Xiaobing Li, Mingfu Cai, Xuemei Wang, and Min Shao
Atmos. Chem. Phys., 22, 14837–14858, https://doi.org/10.5194/acp-22-14837-2022, https://doi.org/10.5194/acp-22-14837-2022, 2022
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We present intensive field measurement of ClNO2 in the Pearl River Delta in 2019. Large variation in the level, formation, and atmospheric impacts of ClNO2 was found in different air masses. ClNO2 formation was limited by the particulate chloride (Cl−) and aerosol surface area. Our results reveal that Cl− originated from various anthropogenic emissions rather than sea sources and show minor contribution to the O3 pollution and photochemistry.
Amy Christiansen, Loretta J. Mickley, Junhua Liu, Luke D. Oman, and Lu Hu
Atmos. Chem. Phys., 22, 14751–14782, https://doi.org/10.5194/acp-22-14751-2022, https://doi.org/10.5194/acp-22-14751-2022, 2022
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Understanding tropospheric ozone trends is crucial for accurate predictions of future air quality and climate, but drivers of trends are not well understood. We analyze global tropospheric ozone trends since 1980 using ozonesonde and surface measurements, and we evaluate two models for their ability to reproduce trends. We find observational evidence of increasing tropospheric ozone, but models underestimate these increases. This hinders our ability to estimate ozone radiative forcing.
Yue Tan and Tao Wang
Atmos. Chem. Phys., 22, 14455–14466, https://doi.org/10.5194/acp-22-14455-2022, https://doi.org/10.5194/acp-22-14455-2022, 2022
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We present a timely analysis of the effects of the recent lockdown in Shanghai on ground-level ozone (O3). Despite a huge reduction in human activity, O3 concentrations frequently exceeded the O3 air quality standard during the 2-month lockdown, implying that future emission reductions similar to those that occurred during the lockdown will not be sufficient to eliminate O3 pollution in many urban areas without the imposition of additional VOC controls or substantial decreases in NOx emissions.
Peeyush Khare, Jordan E. Krechmer, Jo E. Machesky, Tori Hass-Mitchell, Cong Cao, Junqi Wang, Francesca Majluf, Felipe Lopez-Hilfiker, Sonja Malek, Will Wang, Karl Seltzer, Havala O. T. Pye, Roisin Commane, Brian C. McDonald, Ricardo Toledo-Crow, John E. Mak, and Drew R. Gentner
Atmos. Chem. Phys., 22, 14377–14399, https://doi.org/10.5194/acp-22-14377-2022, https://doi.org/10.5194/acp-22-14377-2022, 2022
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Ammonium adduct chemical ionization is used to examine the atmospheric abundances of oxygenated volatile organic compounds associated with emissions from volatile chemical products, which are now key contributors of reactive precursors to ozone and secondary organic aerosols in urban areas. The application of this valuable measurement approach in densely populated New York City enables the evaluation of emissions inventories and thus the role these oxygenated compounds play in urban air quality.
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.
Louise Bøge Frederickson, Ruta Sidaraviciute, Johan Albrecht Schmidt, Ole Hertel, and Matthew Stanley Johnson
Atmos. Chem. Phys., 22, 13949–13965, https://doi.org/10.5194/acp-22-13949-2022, https://doi.org/10.5194/acp-22-13949-2022, 2022
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Low-cost sensors see additional pollution that is not seen with traditional regional air quality monitoring stations. This additional local pollution is sufficient to cause exceedance of the World Health Organization exposure thresholds. Analysis shows that a significant amount of the NO2 pollution we observe is local, mainly due to road traffic. This article demonstrates how networks of nodes containing low-cost pollution sensors can powerfully extend existing monitoring programmes.
Samuel J. Cliff, Will Drysdale, James D. Lee, Carole Helfter, Eiko Nemitz, Stefan Metzger, and Janet F. Barlow
EGUsphere, https://doi.org/10.5194/egusphere-2022-956, https://doi.org/10.5194/egusphere-2022-956, 2022
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Emissions of nitrogen oxides (NOx) to the atmosphere are an ongoing air quality issue. This study directly measures emissions of NOx and carbon dioxide from a tall tower in central London during the coronavirus pandemic. It was found that transport NOx emissions had reduced by > 75 % since 2017 as a result of air quality policy and reduced congestion during coronavirus restrictions. During this period, central London was thought to be dominated by point source heat and power generation emissions.
David D. Parrish, Richard G. Derwent, Ian C. Faloona, and Charles A. Mims
Atmos. Chem. Phys., 22, 13423–13430, https://doi.org/10.5194/acp-22-13423-2022, https://doi.org/10.5194/acp-22-13423-2022, 2022
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Accounting for the continuing long-term decrease of pollution ozone and the large 2020 Arctic stratospheric ozone depletion event improves estimates of background ozone changes caused by COVID-19-related emission reductions; they are smaller than reported earlier. Cooperative, international emission control efforts aimed at maximizing the ongoing decrease in hemisphere-wide background ozone may be the most effective approach to improving ozone pollution in northern midlatitude countries.
Wendell W. Walters, Madeline Karod, Emma Willcocks, Bok H. Baek, Danielle E. Blum, and Meredith G. Hastings
Atmos. Chem. Phys., 22, 13431–13448, https://doi.org/10.5194/acp-22-13431-2022, https://doi.org/10.5194/acp-22-13431-2022, 2022
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Atmospheric ammonia and its products are a significant source of urban haze and nitrogen deposition. We have investigated the seasonal source contributions to a mid-sized city in the northeastern US megalopolis utilizing geospatial statistical analysis and novel isotopic constraints, which indicate that vehicle emissions were significant components of the urban-reduced nitrogen budget. Reducing vehicle ammonia emissions should be considered to improve ecosystems and human health.
Zhaofeng Tan, Hendrik Fuchs, Andreas Hofzumahaus, William J. Bloss, Birger Bohn, Changmin Cho, Thorsten Hohaus, Frank Holland, Chandrakiran Lakshmisha, Lu Liu, Paul S. Monks, Anna Novelli, Doreen Niether, Franz Rohrer, Ralf Tillmann, Thalassa S. E. Valkenburg, Vaishali Vardhan, Astrid Kiendler-Scharr, Andreas Wahner, and Roberto Sommariva
Atmos. Chem. Phys., 22, 13137–13152, https://doi.org/10.5194/acp-22-13137-2022, https://doi.org/10.5194/acp-22-13137-2022, 2022
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During the 2019 JULIAC campaign, ClNO2 was measured at a rural site in Germany in different seasons. The highest ClNO2 level was 1.6 ppbv in September. ClNO2 production was more sensitive to the availability of NO2 than O3. The average ClNO2 production efficiency was up to 18 % in February and September and down to 3 % in December. These numbers are at the high end of the values reported in the literature, indicating the importance of ClNO2 chemistry in rural environments in midwestern Europe.
Zhensen Zheng, Kangwei Li, Bo Xu, Jianping Dou, Liming Li, Guotao Zhang, Shijie Li, Chunmei Geng, Wen Yang, Merched Azzi, and Zhipeng Bai
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-592, https://doi.org/10.5194/acp-2022-592, 2022
Revised manuscript accepted for ACP
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Previous box model studies applied different timescales of observational datasets to identify the O3-precursor relationship, but there is a lack of comparison among these different timescales upon the impact of O3 formation chemistry. Through a case study at Zibo of China, we find that the O3 formation regime showed overall consistency but non-negligible variability among various patterns of timescale. This would be complementary in developing more accurate O3 pollution control strategy.
Xinping Yang, Keding Lu, Xuefei Ma, Yue Gao, Zhaofeng Tan, Haichao Wang, Xiaorui Chen, Xin Li, Xiaofeng Huang, Lingyan He, Mengxue Tang, Bo Zhu, Shiyi Chen, Huabin Dong, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 22, 12525–12542, https://doi.org/10.5194/acp-22-12525-2022, https://doi.org/10.5194/acp-22-12525-2022, 2022
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We present the OH and HO2 radical observations at the Shenzhen site (Pearl River Delta, China) in the autumn of 2018. The diurnal maxima were 4.5 × 106 cm−3 for OH and 4.2 × 108 cm−3 for HO2 (including an estimated interference of 23 %–28 % from RO2 radicals during the daytime). The OH underestimation was identified again, and it was attributable to the missing OH sources. HO2 heterogeneous uptake, ROx sources and sinks, and the atmospheric oxidation capacity were evaluated as well.
Katherine L. Hayden, Shao-Meng Li, John Liggio, Michael J. Wheeler, Jeremy J. B. Wentzell, Amy Leithead, Peter Brickell, Richard L. Mittermeier, Zachary Oldham, Cristian M. Mihele, Ralf M. Staebler, Samar G. Moussa, Andrea Darlington, Mengistu Wolde, Daniel Thompson, Jack Chen, Debora Griffin, Ellen Eckert, Jenna C. Ditto, Megan He, and Drew R. Gentner
Atmos. Chem. Phys., 22, 12493–12523, https://doi.org/10.5194/acp-22-12493-2022, https://doi.org/10.5194/acp-22-12493-2022, 2022
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In this study, airborne measurements provided the most detailed characterization, to date, of boreal forest wildfire emissions. Measurements showed a large diversity of air pollutants expanding the volatility range typically reported. A large portion of organic species was unidentified, likely comprised of complex organic compounds. Aircraft-derived emissions improve wildfire chemical speciation and can support reliable model predictions of pollution from boreal forest wildfires.
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.
Lulu Cui, Di Wu, Shuxiao Wang, Qingcheng Xu, Ruolan Hu, and Jiming Hao
Atmos. Chem. Phys., 22, 11931–11944, https://doi.org/10.5194/acp-22-11931-2022, https://doi.org/10.5194/acp-22-11931-2022, 2022
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A 1-year campaign was conducted to characterize VOCs at a Beijing urban site during different episodes. VOCs from fuel evaporation and diesel exhaust, particularly toluene, xylenes, trans-2-butene, acrolein, methyl methacrylate, vinyl acetate, 1-butene, and 1-hexene, were the main contributors. VOCs from diesel exhaust as well as coal and biomass combustion were found to be the dominant contributors for SOAFP, particularly the VOC species toluene, 1-hexene, xylenes, ethylbenzene, and styrene.
Marcel Zauner-Wieczorek, Martin Heinritzi, Manuel Granzin, Timo Keber, Andreas Kürten, Katharina Kaiser, Johannes Schneider, and Joachim Curtius
Atmos. Chem. Phys., 22, 11781–11794, https://doi.org/10.5194/acp-22-11781-2022, https://doi.org/10.5194/acp-22-11781-2022, 2022
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We present measurements of ambient ions in the free troposphere and lower stratosphere over Europe in spring 2020. We observed nitrate and hydrogen sulfate, amongst others. From their ratio, the number concentrations of gaseous sulfuric acid were inferred. Nitrate increased towards the stratosphere, whilst sulfuric acid was slightly decreased there. The average values for sulfuric acid were 1.9 to 7.8 × 105 cm-3. Protonated pyridine was identified in an altitude range of 4.6 to 8.5 km.
Alena Dekhtyareva, Mark Hermanson, Anna Nikulina, Ove Hermansen, Tove Svendby, Kim Holmén, and Rune Grand Graversen
Atmos. Chem. Phys., 22, 11631–11656, https://doi.org/10.5194/acp-22-11631-2022, https://doi.org/10.5194/acp-22-11631-2022, 2022
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Despite decades of industrial activity in Svalbard, there is no continuous air pollution monitoring in the region’s settlements except Ny-Ålesund. The NOx and O3 observations from the three-station network have been compared for the first time in this study. It has been shown how the large-scale weather regimes control the synoptic meteorological conditions and determine the atmospheric long-range transport pathways and efficiency of local air pollution dispersion.
Asher P. Mouat, Clare Paton-Walsh, Jack B. Simmons, Jhonathan Ramirez-Gamboa, David W. T. Griffith, and Jennifer Kaiser
Atmos. Chem. Phys., 22, 11033–11047, https://doi.org/10.5194/acp-22-11033-2022, https://doi.org/10.5194/acp-22-11033-2022, 2022
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We examine emissions of volatile organic compounds from 2020 wildfires in forested regions of Australia (AU). We find that biomass burning in temperate regions of the US and AU emit similar species in similar proportion, both in natural and lab settings. This suggests studies of wildfires in one region may be used to help improve air quality models in other parts of the world. We observe time series of ozone and nitrogen dioxide. Last, we look at which compounds contribute most to OH reactivity.
Changmin Cho, Hendrik Fuchs, Andreas Hofzumahaus, Frank Holland, William J. Bloss, Birger Bohn, Hans-Peter Dorn, Marvin Glowania, Thorsten Hohaus, Lu Liu, Paul S. Monks, Doreen Niether, Franz Rohrer, Roberto Sommariva, Zhaofeng Tan, Ralf Tillmann, Astrid Kiendler-Scharr, Andreas Wahner, and Anna Novelli
EGUsphere, https://doi.org/10.5194/egusphere-2022-820, https://doi.org/10.5194/egusphere-2022-820, 2022
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With this study, we investigated the processes leading to the formation, destruction, and recycling of radicals for four seasons in a rural environment. A complete knowledge of their chemistry is needed if we are to predict the formation of secondary pollutants from primary emissions. The results highlighted an incomplete understanding of the paths leading to the formation of the OH radical and that has been observed in several different environments and that needs to be investigated further.
Shang Liu, Barbara Barletta, Rebecca S. Hornbrook, Alan Fried, Jeff Peischl, Simone Meinardi, Matthew Coggon, Aaron Lamplugh, Jessica B. Gilman, Georgios I. Gkatzelis, Carsten Warneke, Eric C. Apel, Alan J. Hills, Ilann Bourgeois, James Walega, Petter Weibring, Dirk Richter, Toshihiro Kuwayama, Michael FitzGibbon, and Donald Blake
Atmos. Chem. Phys., 22, 10937–10954, https://doi.org/10.5194/acp-22-10937-2022, https://doi.org/10.5194/acp-22-10937-2022, 2022
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California’s ozone persistently exceeds the air quality standards. We studied the spatial distribution of volatile organic compounds (VOCs) that produce ozone over the most polluted regions in California using aircraft measurements. We find that the oxygenated VOCs have the highest ozone formation potential. Spatially, biogenic VOCs are important during high ozone episodes in the South Coast Air Basin, while dairy emissions may be critical for ozone production in San Joaquin Valley.
Simone M. Pieber, Béla Tuzson, Stephan Henne, Ute Karstens, Christoph Gerbig, Frank-Thomas Koch, Dominik Brunner, Martin Steinbacher, and Lukas Emmenegger
Atmos. Chem. Phys., 22, 10721–10749, https://doi.org/10.5194/acp-22-10721-2022, https://doi.org/10.5194/acp-22-10721-2022, 2022
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Understanding regional greenhouse gas emissions into the atmosphere is a prerequisite to mitigate climate change. In this study, we investigated the regional contributions of carbon dioxide (CO2) at the location of the high Alpine observatory Jungfraujoch (JFJ, Switzerland, 3580 m a.s.l.). To this purpose, we combined receptor-oriented atmospheric transport simulations for CO2 concentration in the period 2009–2017 with stable carbon isotope (δ13C–CO2) information.
Xiao-Bing Li, Bin Yuan, Sihang Wang, Chunlin Wang, Jing Lan, Zhijie Liu, Yongxin Song, Xianjun He, Yibo Huangfu, Chenglei Pei, Peng Cheng, Suxia Yang, Jipeng Qi, Caihong Wu, Shan Huang, Yingchang You, Ming Chang, Huadan Zheng, Wenda Yang, Xuemei Wang, and Min Shao
Atmos. Chem. Phys., 22, 10567–10587, https://doi.org/10.5194/acp-22-10567-2022, https://doi.org/10.5194/acp-22-10567-2022, 2022
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High-time-resolution measurements of volatile organic compounds (VOCs) were made using an online mass spectrometer at a 600 m tall tower in urban region. Compositions, temporal variations, and sources of VOCs were quantitatively investigated in this study. We find that VOC measurements in urban regions aloft could better characterize source characteristics of anthropogenic emissions. Our results could provide important implications in making future strategies for control of VOCs.
Tianyu Zhai, Keding Lu, Haichao Wang, Shengrong Lou, Xiaorui Chen, Renzhi Hu, and Yuanhang Zhang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-548, https://doi.org/10.5194/acp-2022-548, 2022
Revised manuscript accepted for ACP
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Particulate nitrate is a growing issue in the air pollution. Based on a comprehensive field measurement, we show a heavy nitrate pollution in eastern China in summer. OH reacts with NO2 at daytime dominates nitrate formation on clean days while N2O5 hydrolysis largely enhanced and become comparable with that of OH reacts with O2 during polluted days (47.1 % and 52.9 %). Model simulation indicates that VOCs: NOx = 2:1 is effective to mitigate the O3 and nitrate pollution coordinately.
Robert J. Yokelson, Bambang H. Saharjo, Chelsea E. Stockwell, Erianto I. Putra, Thilina Jayarathne, Acep Akbar, Israr Albar, Donald R. Blake, Laura L. B. Graham, Agus Kurniawan, Simone Meinardi, Diah Ningrum, Ati D. Nurhayati, Asmadi Saad, Niken Sakuntaladewi, Eko Setianto, Isobel J. Simpson, Elizabeth A. Stone, Sigit Sutikno, Andri Thomas, Kevin C. Ryan, and Mark A. Cochrane
Atmos. Chem. Phys., 22, 10173–10194, https://doi.org/10.5194/acp-22-10173-2022, https://doi.org/10.5194/acp-22-10173-2022, 2022
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Fire plus non-fire GHG emissions associated with draining peatlands are the largest per area of any land use change considered by the IPCC. To characterize average and variability for tropical peat fire emissions, highly mobile smoke sampling teams were deployed across four Indonesian provinces to explore an extended interannual, climatic, and spatial range. Large adjustments to IPCC-recommended emissions are suggested. Lab data bolster an extensive emissions database for tropical peat fires.
Deanna C. Myers, Saewung Kim, Steven Sjostedt, Alex B. Guenther, Roger Seco, Oscar Vega Bustillos, Julio Tota, Rodrigo A. F. Souza, and James N. Smith
Atmos. Chem. Phys., 22, 10061–10076, https://doi.org/10.5194/acp-22-10061-2022, https://doi.org/10.5194/acp-22-10061-2022, 2022
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We present the first measurements of gas-phase sulfuric acid from the Amazon basin and evaluate the efficacy of existing sulfuric acid parameterizations in this understudied region. Sulfuric acid is produced during the daytime and nighttime, though current proxies underestimate nighttime production. These results illustrate the need for better parameterizations of sulfuric acid and its precursors that are informed by measurements across a broad range of locations.
Yishuo Guo, Chao Yan, Yuliang Liu, Xiaohui Qiao, Feixue Zheng, Ying Zhang, Ying Zhou, Chang Li, Xiaolong Fan, Zhuohui Lin, Zemin Feng, Yusheng Zhang, Penggang Zheng, Linhui Tian, Wei Nie, Zhe Wang, Dandan Huang, Kaspar R. Daellenbach, Lei Yao, Lubna Dada, Federico Bianchi, Jingkun Jiang, Yongchun Liu, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 22, 10077–10097, https://doi.org/10.5194/acp-22-10077-2022, https://doi.org/10.5194/acp-22-10077-2022, 2022
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Gaseous oxygenated organic molecules (OOMs) are able to form atmospheric aerosols, which will impact on human health and climate change. Here, we find that OOMs in urban Beijing are dominated by anthropogenic sources, i.e. aromatic (29 %–41 %) and aliphatic (26 %–41 %) OOMs. They are also the main contributors to the condensational growth of secondary organic aerosols (SOAs). Therefore, the restriction on anthropogenic VOCs is crucial for the reduction of SOAs and haze formation.
Sihang Wang, Bin Yuan, Caihong Wu, Chaomin Wang, Tiange Li, Xianjun He, Yibo Huangfu, Jipeng Qi, Xiao-Bing Li, Qing'e Sha, Manni Zhu, Shengrong Lou, Hongli Wang, Thomas Karl, Martin Graus, Zibing Yuan, and Min Shao
Atmos. Chem. Phys., 22, 9703–9720, https://doi.org/10.5194/acp-22-9703-2022, https://doi.org/10.5194/acp-22-9703-2022, 2022
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Volatile organic compound (VOC) emissions from vehicles are measured using online mass spectrometers. Differences between gasoline and diesel vehicles are observed with higher emission factors of most oxygenated VOCs (OVOCs) and heavier aromatics from diesel vehicles. A higher aromatics / toluene ratio could provide good indicators to distinguish emissions from both vehicle types. We show that OVOCs account for significant contributions to VOC emissions from vehicles, especially diesel vehicles.
Keming Pan and Ian C. Faloona
Atmos. Chem. Phys., 22, 9681–9702, https://doi.org/10.5194/acp-22-9681-2022, https://doi.org/10.5194/acp-22-9681-2022, 2022
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This work represents a unique analysis of 10 existing air quality network sites and meteorological sites, two AmeriFlux sites, and a radio acoustic sounding system in the Central Valley of California during five consecutive fire seasons, June through September, from 2016 to 2020. We find that the ozone production rate increases by ~ 50 % during wildfire influenced periods. Wildfire smoke also decreases the heat flux by 30 % and results in 12 % lower mixed-layer height.
Zaneta T. Hamryszczak, Andrea Pozzer, Florian Obersteiner, Birger Bohn, Benedikt Steil, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 9483–9497, https://doi.org/10.5194/acp-22-9483-2022, https://doi.org/10.5194/acp-22-9483-2022, 2022
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Hydrogen peroxide plays a pivotal role in the chemistry of the atmosphere. Together with organic hydroperoxides, it forms a reservoir for peroxy radicals, which are known to be the key contributors to the self-cleaning processes of the atmosphere. Hydroperoxides were measured over Europe during the BLUESKY campaign in May–June 2020. The paper gives an overview of the distribution of the species in the troposphere and investigates the impact of wet scavenging and deposition on the budget of H2O2.
Will S. Drysdale, Adam R. Vaughan, Freya A. Squires, Sam J. Cliff, Stefan Metzger, David Durden, Natchaya Pingintha-Durden, Carole Helfter, Eiko Nemitz, C. Sue B. Grimmond, Janet Barlow, Sean Beevers, Gregor Stewart, David Dajnak, Ruth M. Purvis, and James D. Lee
Atmos. Chem. Phys., 22, 9413–9433, https://doi.org/10.5194/acp-22-9413-2022, https://doi.org/10.5194/acp-22-9413-2022, 2022
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Measurements of NOx emissions are important for a good understanding of air quality. While there are many direct measurements of NOx concentration, there are very few measurements of its emission. Measurements of emissions provide constraints on emissions inventories and air quality models. This article presents measurements of NOx emission from the BT Tower in central London in 2017 and compares them with inventories, finding that they underestimate by a factor of ∼1.48.
Eric Förster, Harald Bönisch, Marco Neumaier, Florian Obersteiner, Andreas Zahn, Andreas Hilboll, Anna Beata Kalisz Hedegaard, Nikos Daskalakis, Alexandros Panagiotis Poulidis, Mihalis Vrekoussis, Michael Lichtenstern, and Peter Braesicke
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-455, https://doi.org/10.5194/acp-2022-455, 2022
Revised manuscript accepted for ACP
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The airborne megacity campaign EMeRGe provided an unprecedented amount of trace gas measurements. We combine measured volatile organic compounds (VOCs) with trajectory-modelled emission uptakes to identify potential source regions of pollution. We also characterise the chemical fingerprints (e.g. biomass burning and anthropogenic signatures) of the probed air-masses to corroborate the contributing source regions. Our approach is the first large-scale study of VOCs originating from megacities.
Yihang Yu, Peng Cheng, Huirong Li, Wenda Yang, Baobin Han, Wei Song, Weiwei Hu, Xinming Wang, Bin Yuan, Min Shao, Zhijiong Huang, Zhen Li, Junyu Zheng, Haichao Wang, and Xiaofang Yu
Atmos. Chem. Phys., 22, 8951–8971, https://doi.org/10.5194/acp-22-8951-2022, https://doi.org/10.5194/acp-22-8951-2022, 2022
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We have investigated the budget of HONO at an urban site in Guangzhou. Budget and comprehensive uncertainty analysis suggest that at such locations as ours, HONO direct emissions and NO + OH can become comparable or even surpass other HONO sources that typically receive greater attention and interest, such as the NO2 heterogeneous source and the unknown daytime photolytic source. Our findings emphasize the need to reduce the uncertainties of both conventional and novel HONO sources and sinks.
Wenjie Wang, David D. Parrish, Siwen Wang, Fengxia Bao, Ruijing Ni, Xin Li, Suding Yang, Hongli Wang, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 8935–8949, https://doi.org/10.5194/acp-22-8935-2022, https://doi.org/10.5194/acp-22-8935-2022, 2022
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Tropospheric ozone is an air pollutant that is detrimental to human health, vegetation and ecosystem productivity. A comprehensive characterisation of the spatial and temporal distribution of tropospheric ozone is critical to our understanding of these issues. Here we summarise this distribution over China from the available observational records to the extent possible. This study provides insights into efficient future ozone control strategies in China.
Lauriane L. J. Quéléver, Lubna Dada, Eija Asmi, Janne Lampilahti, Tommy Chan, Jonathan E. Ferrara, Gustavo E. Copes, German Pérez-Fogwill, Luis Barreira, Minna Aurela, Douglas R. Worsnop, Tuija Jokinen, and Mikko Sipilä
Atmos. Chem. Phys., 22, 8417–8437, https://doi.org/10.5194/acp-22-8417-2022, https://doi.org/10.5194/acp-22-8417-2022, 2022
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Understanding how aerosols form is crucial for correctly modeling the climate and improving future predictions. This work provides extensive analysis of aerosol particles and their precursors at Marambio Station, Antarctic Peninsula. We show that sulfuric acid, ammonia, and dimethylamine are key contributors to the frequent new particle formation events observed at the site. We discuss nucleation mechanisms and highlight the need for targeted measurement to fully understand these processes.
Xueli Liu, Liang Ran, Weili Lin, Xiaobin Xu, Zhiqiang Ma, Fan Dong, Di He, Liyan Zhou, Qingfeng Shi, and Yao Wang
Atmos. Chem. Phys., 22, 7071–7085, https://doi.org/10.5194/acp-22-7071-2022, https://doi.org/10.5194/acp-22-7071-2022, 2022
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Significant decreases in annual mean NOx from 2011 to 2016 and SO2 from 2008 to 2016 confirm the effectiveness of relevant control measures on the reduction in NOx and SO2 emissions in the North China Plain (NCP). NOx at SDZ had a weaker influence than SO2 on the emission reduction in Beijing and other areas in the NCP. An increase in the number of motor vehicles and weak traffic restrictions have caused vehicle emissions of NOx, which indicates that NOx emission control should be strengthened.
Patrick Dewald, Clara M. Nussbaumer, Jan Schuladen, Akima Ringsdorf, Achim Edtbauer, Horst Fischer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 7051–7069, https://doi.org/10.5194/acp-22-7051-2022, https://doi.org/10.5194/acp-22-7051-2022, 2022
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We measured the gas-phase reactivity of the NO3 radical on the summit (825 m a.s.l.) of a semi-rural mountain in southwestern Germany in July 2021. The impact of VOC-induced NO3 losses (mostly monoterpenes) competing with a loss by reaction with NO and photolysis throughout the diel cycle was estimated. Besides chemistry, boundary layer dynamics and plant-physiological processes presumably have a great impact on our observations, which were compared to previous NO3 measurements at the same site.
Shigeyuki Ishidoya, Kazuhiro Tsuboi, Yosuke Niwa, Hidekazu Matsueda, Shohei Murayama, Kentaro Ishijima, and Kazuyuki Saito
Atmos. Chem. Phys., 22, 6953–6970, https://doi.org/10.5194/acp-22-6953-2022, https://doi.org/10.5194/acp-22-6953-2022, 2022
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The atmospheric O2 / N2 ratio and CO2 concentration over the western North Pacific are presented. We found significant modification of the seasonal APO cycle in the middle troposphere due to the interhemispheric mixing of air. APO driven by the net marine biological activities indicated annual sea–air O2 flux during El Niño. Terrestrial biospheric and oceanic CO2 uptakes during 2012–2019 were estimated to be 1.8 and 2.8 Pg C a−1, respectively.
Xuefei Ma, Zhaofeng Tan, Keding Lu, Xinping Yang, Xiaorui Chen, Haichao Wang, Shiyi Chen, Xin Fang, Shule Li, Xin Li, Jingwei Liu, Ying Liu, Shengrong Lou, Wanyi Qiu, Hongli Wang, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 22, 7005–7028, https://doi.org/10.5194/acp-22-7005-2022, https://doi.org/10.5194/acp-22-7005-2022, 2022
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This paper presents the first OH and HO2 radical observations made in the Yangtze River Delta in China, and strong oxidation capacity is discovered based on direct measurements. The impacts of new OH regeneration mechanisms, monoterpene oxidation, and HO2 uptake processes are examined and discussed. The sources and the factors to sustain such strong oxidation are the key to understanding the ozone pollution formed in this area.
Taku Umezawa, Satoshi Sugawara, Kenji Kawamura, Ikumi Oyabu, Stephen J. Andrews, Takuya Saito, Shuji Aoki, and Takakiyo Nakazawa
Atmos. Chem. Phys., 22, 6899–6917, https://doi.org/10.5194/acp-22-6899-2022, https://doi.org/10.5194/acp-22-6899-2022, 2022
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Greenhouse gas methane in the Arctic atmosphere has not been accurately reported for 1900–1980 from either direct observations or ice core reconstructions. By using trace gas data from firn (compacted snow layers above ice sheet), air samples at two Greenland sites, and a firn air transport model, this study suggests a likely range of the Arctic methane reconstruction for the 20th century. Atmospheric scenarios from two previous studies are also evaluated for consistency with the firn data sets.
Susann Tegtmeier, Christa Marandino, Yue Jia, Birgit Quack, and Anoop S. Mahajan
Atmos. Chem. Phys., 22, 6625–6676, https://doi.org/10.5194/acp-22-6625-2022, https://doi.org/10.5194/acp-22-6625-2022, 2022
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In the atmosphere over the Indian Ocean, intense anthropogenic pollution from Southeast Asia mixes with pristine oceanic air. During the winter monsoon, high pollution levels are regularly observed over the entire northern Indian Ocean, while during the summer monsoon, clean air dominates. Here, we review current progress in detecting and understanding atmospheric gas-phase composition over the Indian Ocean and its impacts on the upper atmosphere, oceanic biogeochemistry, and marine ecosystems.
Lian Zong, Yuanjian Yang, Haiyun Xia, Meng Gao, Zhaobin Sun, Zuofang Zheng, Xianxiang Li, Guicai Ning, Yubin Li, and Simone Lolli
Atmos. Chem. Phys., 22, 6523–6538, https://doi.org/10.5194/acp-22-6523-2022, https://doi.org/10.5194/acp-22-6523-2022, 2022
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Heatwaves (HWs) paired with higher ozone (O3) concentration at surface level pose a serious threat to human health. Taking Beijing as an example, three unfavorable synoptic weather patterns were identified to dominate the compound HW and O3 pollution events. Under the synergistic stress of HWs and O3 pollution, public mortality risk increased, and synoptic patterns and urbanization enhanced the compound risk of events in Beijing by 33.09 % and 18.95 %, respectively.
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