Articles | Volume 15, issue 20
https://doi.org/10.5194/acp-15-11753-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-15-11753-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
22 Oct 2015
Research article |
| 22 Oct 2015
Modelling marine emissions and atmospheric distributions of halocarbons and dimethyl sulfide: the influence of prescribed water concentration vs. prescribed emissions
GEOMAR Helmholtz-Centre for Ocean Research Kiel, Kiel, Germany
G. Krysztofiak
Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, Karlsruhe, Germany
now at: LPC2E, UMR 7328, CNRS-Université d'Orléans, 45071 Orléans CEDEX 2, France
C. A. Marandino
GEOMAR Helmholtz-Centre for Ocean Research Kiel, Kiel, Germany
B.-M. Sinnhuber
Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, Karlsruhe, Germany
S. Tegtmeier
GEOMAR Helmholtz-Centre for Ocean Research Kiel, Kiel, Germany
F. Ziska
GEOMAR Helmholtz-Centre for Ocean Research Kiel, Kiel, Germany
R. Hossaini
School of Earth and Environment, University of Leeds, Leeds, UK
K. Krüger
University of Oslo, Department of Geosciences, Oslo, Norway
S. A. Montzka
NOAA/CMDL, Boulder, CO, USA
RSMAS/MAC, University of Miami, Florida, USA
D. E. Oram
National Centre for Atmospheric Science, Centre for Oceanography and Atmospheric Science, University of East Anglia, Norwich, UK
T. Keber
Goethe University Frankfurt a. M., Institute for Atmospheric and Environmental Sciences, Frankfurt, Germany
H. Bönisch
Goethe University Frankfurt a. M., Institute for Atmospheric and Environmental Sciences, Frankfurt, Germany
B. Quack
GEOMAR Helmholtz-Centre for Ocean Research Kiel, Kiel, Germany
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Daniel Zawada, Kimberlee Dubé, Taran Warnock, Adam Bourassa, Susann Tegtmeier, and Douglas Degenstein
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There remain large uncertainties in long-term changes of stratospheric–atmospheric temperatures. We have produced a time series of more than 20 years of satellite-based temperature measurements from the OSIRIS instrument in the upper–middle stratosphere. The dataset is publicly available and intended to be used for a better understanding of changes in stratospheric temperatures.
Lily Gouldsbrough, Ryan Hossaini, Emma Eastoe, Paul J. Young, and Massimo Vieno
Atmos. Chem. Phys., 24, 3163–3196, https://doi.org/10.5194/acp-24-3163-2024, https://doi.org/10.5194/acp-24-3163-2024, 2024
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High-resolution spatial fields of surface ozone are used to understand spikes in ozone concentration and predict their impact on public health. Such fields are routinely output from complex mathematical models for atmospheric conditions. These outputs are on a coarse spatial resolution and the highest concentrations tend to be biased. Using a novel data-driven machine learning methodology, we show how such output can be corrected to produce fields with both lower bias and higher resolution.
Ryan Hossaini, David Sherry, Zihao Wang, Martyn Chipperfield, Wuhu Feng, David Oram, Karina Adcock, Stephen Montzka, Isobel Simpson, Andrea Mazzeo, Amber Leeson, Elliot Atlas, and Charles C.-K. Chou
EGUsphere, https://doi.org/10.5194/egusphere-2024-560, https://doi.org/10.5194/egusphere-2024-560, 2024
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Ethylene dichloride (EDC) is an industrial chemical used to produce polyvinyl chloride (PVC). We analysed EDC production data to estimate global EDC emissions (2002 to 2020). The emissions were included in an atmospheric model and evaluated by comparing simulated EDC to EDC measurements in the troposphere. We show EDC contributes ozone-depleting chlorine to the stratosphere and this has increased with increasing EDC emissions. EDC’s impact on stratospheric ozone is currently small, but non-zero.
Sankirna D. Joge, Anoop Sharad Mahajan, Shrivardhan Hulswar, Christa Marandino, Martí Galí, Thomas Bell, and Rafel Simo
EGUsphere, https://doi.org/10.5194/egusphere-2024-173, https://doi.org/10.5194/egusphere-2024-173, 2024
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Dimethyl sulfide (DMS) is the largest natural source of sulfur into the atmosphere and leads to the formation of CCN. DMS emissions, and hence the quantification of its impacts, have large uncertainties, but a detailed study on the range of emissions and drivers of their uncertainty is missing to date. The emissions are usually calculated from the seawater DMS concentrations and a flux parameterization. Here we quantify the differences in DMS seawater products, which can affect the DMS fluxes.
Sankirna D. Joge, Anoop Sharad Mahajan, Shrivardhan Hulswar, Christa Marandino, Marti Gali, Thomas Bell, Mingxi Yang, and Rafel Simo
EGUsphere, https://doi.org/10.5194/egusphere-2024-175, https://doi.org/10.5194/egusphere-2024-175, 2024
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Dimethyl sulfide (DMS) is the largest natural source of sulfur into the atmosphere and leads to the formation of CCN. DMS emissions, and hence the quantification of its impacts, have large uncertainties, but a detailed study on the range of emissions and drivers of their uncertainty is missing to date. The emissions are usually calculated from the seawater DMS concentrations and a flux parameterization. Here we quantify the differences in the effect of flux parameterisations used in models.
Gabrielle B. Dreyfus, Stephen A. Montzka, Stephen O. Andersen, and Richard Ferris
Atmos. Chem. Phys., 24, 2023–2032, https://doi.org/10.5194/acp-24-2023-2024, https://doi.org/10.5194/acp-24-2023-2024, 2024
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The Montreal Protocol has put the ozone layer on a path to recovery by phasing out 99 % of banned ozone-damaging substances. Most of these substances are also potent greenhouse gases. Atmospheric monitoring has detected unexpected increases in emissions in several of these banned substances. Here we present an approach for quantifying damage to ozone, climate and health for these emissions and offset by preventing the equivalent emissions of ozone-damaging substances.
Rona L. Thompson, Stephen A. Montzka, Martin K. Vollmer, Jgor Arduini, Molly Crotwell, Paul B. Krummel, Chris Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Stefan Reimann, Isaac Vimont, Hsiang Wang, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 24, 1415–1427, https://doi.org/10.5194/acp-24-1415-2024, https://doi.org/10.5194/acp-24-1415-2024, 2024
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The hydroxyl radical determines the atmospheric lifetimes of numerous species including methane. Since OH is very short-lived, it is not possible to directly measure its concentration on scales relevant for understanding its effect on other species. Here, OH is inferred by looking at changes in hydrofluorocarbons (HFCs). We find that OH levels have been fairly stable over our study period (2004 to 2021), suggesting that OH is not the main driver of the recent increase in atmospheric methane.
Sören Johansson, Michael Höpfner, Felix Friedl-Vallon, Norbert Glatthor, Thomas Gulde, Vincent Huijnen, Anne Kleinert, Erik Kretschmer, Guido Maucher, Tom Neubert, Hans Nordmeyer, Christof Piesch, Peter Preusse, Martin Riese, Björn-Martin Sinnhuber, Jörn Ungermann, Gerald Wetzel, and Wolfgang Woiwode
EGUsphere, https://doi.org/10.5194/egusphere-2024-77, https://doi.org/10.5194/egusphere-2024-77, 2024
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We present airborne infra red limb sounding GLORIA measurements of ammonia in the upper troposphere of air masses within the Asian Monsoon, and of air masses connected with biomass burning. In comparisons with CAMS model data, we find that the model is well reproducing the measured enhanced ammonia within the Asian Monsoon, but not within biomass burning plumes, where no enhanced ammonia is measured in the upper troposphere, but considerable amounts of ammonia are simulated by CAMS.
Tanja J. Schuck, Johannes Degen, Eric Hintsa, Peter Hoor, Markus Jesswein, Timo Keber, Daniel Kunkel, Fred Moore, Florian Obersteiner, Matt Rigby, Thomas Wagenhäuser, Luke M. Western, Andreas Zahn, and Andreas Engel
Atmos. Chem. Phys., 24, 689–705, https://doi.org/10.5194/acp-24-689-2024, https://doi.org/10.5194/acp-24-689-2024, 2024
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We study the interhemispheric gradient of sulfur hexafluoride (SF6), a strong long-lived greenhouse gas. Its emissions are stronger in the Northern Hemisphere; therefore, mixing ratios in the Southern Hemisphere lag behind. Comparing the observations to a box model, the model predicts air in the Southern Hemisphere to be older. For a better agreement, the emissions used as model input need to be increased (and their spatial pattern changed), and we need to modify north–south transport.
Karolin Voss, Philip Holzbeck, Klaus Pfeilsticker, Ralph Kleinschek, Gerald Wetzel, Blanca Fuentes Andrade, Michael Höpfner, Jörn Ungermann, Björn-Martin Sinnhuber, and André Butz
EGUsphere, https://doi.org/10.5194/egusphere-2023-2912, https://doi.org/10.5194/egusphere-2023-2912, 2024
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A novel balloon-borne instrument for direct sun and solar occultation measurements of several UV/vis absorbing gases (e.g. O3, NO2, BrO, IO, HONO, ..) is described. Major design features as well as its performance during two stratospheric deployments are discussed. From the measured overhead BrO concentration and a suitable photochemical correction, total stratospheric bromine is inferred to (17.5 ± 2.2) ppt in air masses which entered the stratosphere around early 2017±1 yr.
Ewa M. Bednarz, Ryan Hossaini, and Martyn P. Chipperfield
Atmos. Chem. Phys., 23, 13701–13711, https://doi.org/10.5194/acp-23-13701-2023, https://doi.org/10.5194/acp-23-13701-2023, 2023
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We quantify, for the first time, the time-varying impact of uncontrolled emissions of chlorinated very short-lived substances (Cl-VSLSs) on stratospheric ozone using a state-of-the-art chemistry-climate model. We demonstrate that Cl-VSLSs already have a non-negligible impact on stratospheric ozone, including a local reduction of up to ~7 DU in Arctic ozone in the cold winter of 2019/20, and any so future growth in emissions will continue to offset some of the benefits of the Montreal Protocol.
Ewa M. Bednarz, Ryan Hossaini, N. Luke Abraham, and Martyn P. Chipperfield
Geosci. Model Dev., 16, 6187–6209, https://doi.org/10.5194/gmd-16-6187-2023, https://doi.org/10.5194/gmd-16-6187-2023, 2023
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Development and performance of the new DEST chemistry scheme of UM–UKCA is described. The scheme extends the standard StratTrop scheme by including important updates to the halogen chemistry, thus allowing process-oriented studies of stratospheric ozone depletion and recovery, including impacts from both controlled long-lived ozone-depleting substances and emerging issues around uncontrolled, very short-lived substances. It will thus aid studies in support of future ozone assessment reports.
Kimberlee Dubé, Susann Tegtmeier, Adam Bourassa, Daniel Zawada, Douglas Degenstein, Patrick E. Sheese, Kaley A. Walker, and William Randel
Atmos. Chem. Phys., 23, 13283–13300, https://doi.org/10.5194/acp-23-13283-2023, https://doi.org/10.5194/acp-23-13283-2023, 2023
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This paper presents a technique for understanding the causes of long-term changes in stratospheric composition. By using N2O as a proxy for stratospheric circulation in the model used to calculated trends, it is possible to separate the effects of dynamics and chemistry on observed trace gas trends. We find that observed HCl increases are due to changes in the stratospheric circulation, as are O3 decreases above 30 hPa in the Northern Hemisphere.
Chaoyang Xue, Gisèle Krysztofiak, Vanessa Brocchi, Stéphane Chevrier, Michel Chartier, Patrick Jacquet, Claude Robert, and Valéry Catoire
Earth Syst. Sci. Data, 15, 4553–4569, https://doi.org/10.5194/essd-15-4553-2023, https://doi.org/10.5194/essd-15-4553-2023, 2023
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To understand tropospheric air pollution at regional and global scales, an infrared laser spectrometer called SPIRIT was used on aircraft to rapidly and accurately measure carbon monoxide (CO), an important indicator of air pollution, during the last decade. Measurements were taken for more than 200 flight hours over three continents. Levels of CO are mapped with 3D trajectories for each flight. Additionally, this can be used to validate model performance and satellite measurements.
Frederik Harzer, Hella Garny, Felix Ploeger, Harald Bönisch, Peter Hoor, and Thomas Birner
Atmos. Chem. Phys., 23, 10661–10675, https://doi.org/10.5194/acp-23-10661-2023, https://doi.org/10.5194/acp-23-10661-2023, 2023
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We study the statistical relation between year-by-year fluctuations in winter-mean ozone and the strength of the stratospheric polar vortex. In the latitude–pressure plane, regression analysis shows that anomalously weak polar vortex years are associated with three pronounced local ozone maxima over the polar cap relative to the winter climatology. These response maxima primarily reflect the non-trivial combination of different ozone transport processes with varying relative contributions.
Luis F. Millán, Gloria L. Manney, Harald Boenisch, Michaela I. Hegglin, Peter Hoor, Daniel Kunkel, Thierry Leblanc, Irina Petropavlovskikh, Kaley Walker, Krzysztof Wargan, and Andreas Zahn
Atmos. Meas. Tech., 16, 2957–2988, https://doi.org/10.5194/amt-16-2957-2023, https://doi.org/10.5194/amt-16-2957-2023, 2023
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The determination of atmospheric composition trends in the upper troposphere and lower stratosphere (UTLS) is still highly uncertain. We present the creation of dynamical diagnostics to map several ozone datasets (ozonesondes, lidars, aircraft, and satellite measurements) in geophysically based coordinate systems. The diagnostics can also be used to analyze other greenhouse gases relevant to surface climate and UTLS chemistry.
Marc von Hobe, Christoph Brühl, Sinikka T. Lennartz, Mary E. Whelan, and Aleya Kaushik
Atmos. Chem. Phys., 23, 6591–6598, https://doi.org/10.5194/acp-23-6591-2023, https://doi.org/10.5194/acp-23-6591-2023, 2023
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Carbonyl sulfide plays a role in the climate system as a greenhouse gas and as the major non-volcanic precursor of particles reflecting sunlight. Here, we comment on a proposal to increase the number of particles by emitting extra carbonyl sulfide at the surface. We show that the balance between aerosol cooling and greenhouse gas warming may not be as favorable as suggested and also that much of the carbonyl sulfide emissions will actually be taken up by the biosphere and the oceans.
Thomas Wagenhäuser, Markus Jesswein, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 23, 3887–3903, https://doi.org/10.5194/acp-23-3887-2023, https://doi.org/10.5194/acp-23-3887-2023, 2023
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A common assumption to derive mean age from trace gas observations is that all air enters the stratosphere through the tropical tropopause. Using SF6 as an age tracer, this leads to negative mean age values close to the Northern Hemispheric extra-tropical tropopause. Our improved method also considers extra-tropical input into the stratosphere. More realistic values are derived using this method. Interhemispheric differences in mean age are found when comparing data from two aircraft campaigns.
Evelien van Dijk, Ingar Mørkestøl Gundersen, Anna de Bode, Helge Høeg, Kjetil Loftsgarden, Frode Iversen, Claudia Timmreck, Johann Jungclaus, and Kirstin Krüger
Clim. Past, 19, 357–398, https://doi.org/10.5194/cp-19-357-2023, https://doi.org/10.5194/cp-19-357-2023, 2023
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The mid-6th century was one of the coldest periods of the last 2000 years as characterized by great societal changes. Here, we study the effect of the volcanic double event in 536 CE and 540 CE on climate and society in southern Norway. The combined climate and growing degree day models and high-resolution pollen and archaeological records reveal that the northern and western sites are vulnerable to crop failure with possible abandonment of farms, whereas the southeastern site is more resilient.
Eric Förster, Harald Bönisch, Marco Neumaier, Florian Obersteiner, Andreas Zahn, Andreas Hilboll, Anna B. Kalisz Hedegaard, Nikos Daskalakis, Alexandros Panagiotis Poulidis, Mihalis Vrekoussis, Michael Lichtenstern, and Peter Braesicke
Atmos. Chem. Phys., 23, 1893–1918, https://doi.org/10.5194/acp-23-1893-2023, https://doi.org/10.5194/acp-23-1893-2023, 2023
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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.
Lei Hu, Deborah Ottinger, Stephanie Bogle, Stephen A. Montzka, Philip L. DeCola, Ed Dlugokencky, Arlyn Andrews, Kirk Thoning, Colm Sweeney, Geoff Dutton, Lauren Aepli, and Andrew Crotwell
Atmos. Chem. Phys., 23, 1437–1448, https://doi.org/10.5194/acp-23-1437-2023, https://doi.org/10.5194/acp-23-1437-2023, 2023
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Effective mitigation of greenhouse gas (GHG) emissions relies on an accurate understanding of emissions. Here we demonstrate the added value of using inventory- and atmosphere-based approaches for estimating US emissions of SF6, the most potent GHG known. The results suggest a large decline in US SF6 emissions, shed light on the possible processes causing the differences between the independent estimates, and identify opportunities for substantial additional emission reductions.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
Shih-Wei Fang, Claudia Timmreck, Johann Jungclaus, Kirstin Krüger, and Hauke Schmidt
Earth Syst. Dynam., 13, 1535–1555, https://doi.org/10.5194/esd-13-1535-2022, https://doi.org/10.5194/esd-13-1535-2022, 2022
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The early 19th century was the coldest period over the past 500 years, when strong tropical volcanic events and a solar minimum coincided. This study quantifies potential surface cooling from the solar and volcanic forcing in the early 19th century with large ensemble simulations, and identifies the regions that their impacts cannot be simply additive. The cooling perspective of Arctic amplification exists in both solar and post-volcano period with the albedo feedback as the main contribution.
Li Zhou, Dennis Booge, Miming Zhang, and Christa A. Marandino
Biogeosciences, 19, 5021–5040, https://doi.org/10.5194/bg-19-5021-2022, https://doi.org/10.5194/bg-19-5021-2022, 2022
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Trace gas air–sea exchange exerts an important control on air quality and climate, especially in the Southern Ocean (SO). Almost all of the measurements there are skewed to summer, but it is essential to expand our measurement database over greater temporal and spatial scales. Therefore, we report measured concentrations of dimethylsulfide (DMS, as well as related sulfur compounds) and isoprene in the Atlantic sector of the SO. The observations of isoprene are the first in the winter in the SO.
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.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, https://doi.org/10.5194/acp-22-10657-2022, 2022
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Atmospheric impacts of chlorinated very short-lived substances (Cl-VSLS) over the first two decades of the 21st century are assessed using the UM-UKCA chemistry–climate model. Stratospheric input of Cl from Cl-VSLS is estimated at ~130 ppt in 2019. The use of model set-up with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running set-up. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
Praveen Kumar Pothapakula, Amelie Hoff, Anika Obermann-Hellhund, Timo Keber, and Bodo Ahrens
Earth Syst. Dynam. Discuss., https://doi.org/10.5194/esd-2022-24, https://doi.org/10.5194/esd-2022-24, 2022
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The Vb-cyclones simulated with a coupled regional climate model with two different driving data sets are compared against each other in historical period, thereafter the future climate predictions were analyzed. The Vb-cyclones in two simulations agree well in terms of their occurrence, intensity and track in two simulations, though there are discrepancies in seasonal cycles and their process linking Mediterranean Sea in historical period. So significant changes were observed in the future.
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616, https://doi.org/10.5194/acp-22-9601-2022, https://doi.org/10.5194/acp-22-9601-2022, 2022
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The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
Kristof Bognar, Susann Tegtmeier, Adam Bourassa, Chris Roth, Taran Warnock, Daniel Zawada, and Doug Degenstein
Atmos. Chem. Phys., 22, 9553–9569, https://doi.org/10.5194/acp-22-9553-2022, https://doi.org/10.5194/acp-22-9553-2022, 2022
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We quantify recent changes in stratospheric ozone (outside the polar regions) using a combination of three satellite datasets. We find that upper stratospheric ozone have increased significantly since 2000, although the recovery shows an unexpected pause in the Northern Hemisphere. Combined with the likely decrease in ozone in the lower stratosphere, this presents an interesting challenge for predicting the future of the ozone layer.
Evelien van Dijk, Johann Jungclaus, Stephan Lorenz, Claudia Timmreck, and Kirstin Krüger
Clim. Past, 18, 1601–1623, https://doi.org/10.5194/cp-18-1601-2022, https://doi.org/10.5194/cp-18-1601-2022, 2022
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A double volcanic eruption in 536 and 540 CE caused one of the coldest decades during the last 2000 years. We analyzed new climate model simulations from that period and found a cooling of up to 2°C and a sea-ice extent up to 200 km further south. Complex interactions between sea ice and ocean circulation lead to a reduction in the northward ocean heat transport, which makes the sea ice extend further south; this in turn leads to a surface cooling up to 20 years after the eruptions.
Yue Jia, Birgit Quack, Robert D. Kinley, Ignacio Pisso, and Susann Tegtmeier
Atmos. Chem. Phys., 22, 7631–7646, https://doi.org/10.5194/acp-22-7631-2022, https://doi.org/10.5194/acp-22-7631-2022, 2022
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In this study, we assessed the potential risks of bromoform released from Asparagopsis farming near Australia for the stratospheric ozone layer by analyzing different cultivation scenarios. We conclude that the intended operation of Asparagopsis seaweed cultivation farms with an annual yield to meet the needs of 50 % of feedlots and cattle in either open-ocean or terrestrial cultures in Australia will not impact the ozone layer under normal operating conditions.
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.
Eric A. Ray, Elliot L. Atlas, Sue Schauffler, Sofia Chelpon, Laura Pan, Harald Bönisch, and Karen H. Rosenlof
Atmos. Chem. Phys., 22, 6539–6558, https://doi.org/10.5194/acp-22-6539-2022, https://doi.org/10.5194/acp-22-6539-2022, 2022
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The movement of air masses and the trace gases they contain from the Earth’s surface into the upper troposphere and lower stratosphere (UTLS) can have important implications for the radiative and chemical balance of the atmosphere. In this study we build on recent techniques and use new ones to estimate a range of transport diagnostics based on simultaneously measured trace gases in the UTLS during the monsoon season in North America.
Camille Abadie, Fabienne Maignan, Marine Remaud, Jérôme Ogée, J. Elliott Campbell, Mary E. Whelan, Florian Kitz, Felix M. Spielmann, Georg Wohlfahrt, Richard Wehr, Wu Sun, Nina Raoult, Ulli Seibt, Didier Hauglustaine, Sinikka T. Lennartz, Sauveur Belviso, David Montagne, and Philippe Peylin
Biogeosciences, 19, 2427–2463, https://doi.org/10.5194/bg-19-2427-2022, https://doi.org/10.5194/bg-19-2427-2022, 2022
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A better constraint of the components of the carbonyl sulfide (COS) global budget is needed to exploit its potential as a proxy of gross primary productivity. In this study, we compare two representations of oxic soil COS fluxes, and we develop an approach to represent anoxic soil COS fluxes in a land surface model. We show the importance of atmospheric COS concentration variations on oxic soil COS fluxes and provide new estimates for oxic and anoxic soil contributions to the COS global budget.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 22, 6087–6101, https://doi.org/10.5194/acp-22-6087-2022, https://doi.org/10.5194/acp-22-6087-2022, 2022
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The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result of the phasing out of ozone-depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
M. Dolores Andrés Hernández, Andreas Hilboll, Helmut Ziereis, Eric Förster, Ovid O. Krüger, Katharina Kaiser, Johannes Schneider, Francesca Barnaba, Mihalis Vrekoussis, Jörg Schmidt, Heidi Huntrieser, Anne-Marlene Blechschmidt, Midhun George, Vladyslav Nenakhov, Theresa Harlass, Bruna A. Holanda, Jennifer Wolf, Lisa Eirenschmalz, Marc Krebsbach, Mira L. Pöhlker, Anna B. Kalisz Hedegaard, Linlu Mei, Klaus Pfeilsticker, Yangzhuoran Liu, Ralf Koppmann, Hans Schlager, Birger Bohn, Ulrich Schumann, Andreas Richter, Benjamin Schreiner, Daniel Sauer, Robert Baumann, Mariano Mertens, Patrick Jöckel, Markus Kilian, Greta Stratmann, Christopher Pöhlker, Monica Campanelli, Marco Pandolfi, Michael Sicard, José L. Gómez-Amo, Manuel Pujadas, Katja Bigge, Flora Kluge, Anja Schwarz, Nikos Daskalakis, David Walter, Andreas Zahn, Ulrich Pöschl, Harald Bönisch, Stephan Borrmann, Ulrich Platt, and John P. Burrows
Atmos. Chem. Phys., 22, 5877–5924, https://doi.org/10.5194/acp-22-5877-2022, https://doi.org/10.5194/acp-22-5877-2022, 2022
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EMeRGe provides a unique set of in situ and remote sensing airborne measurements of trace gases and aerosol particles along selected flight routes in the lower troposphere over Europe. The interpretation uses also complementary collocated ground-based and satellite measurements. The collected data help to improve the current understanding of the complex spatial distribution of trace gases and aerosol particles resulting from mixing, transport, and transformation of pollution plumes over Europe.
Helmut Ziereis, Peter Hoor, Jens-Uwe Grooß, Andreas Zahn, Greta Stratmann, Paul Stock, Michael Lichtenstern, Jens Krause, Vera Bense, Armin Afchine, Christian Rolf, Wolfgang Woiwode, Marleen Braun, Jörn Ungermann, Andreas Marsing, Christiane Voigt, Andreas Engel, Björn-Martin Sinnhuber, and Hermann Oelhaf
Atmos. Chem. Phys., 22, 3631–3654, https://doi.org/10.5194/acp-22-3631-2022, https://doi.org/10.5194/acp-22-3631-2022, 2022
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Airborne observations were conducted in the lowermost Arctic stratosphere during the winter of 2015/2016. The observed distribution of reactive nitrogen shows clear indications of nitrification in mid-winter and denitrification in late winter. This was caused by the formation of polar stratospheric cloud particles, which were observed during several flights. The sedimentation and evaporation of these particles and the descent of air masses cause a redistribution of reactive nitrogen.
Sören Johansson, Gerald Wetzel, Felix Friedl-Vallon, Norbert Glatthor, Michael Höpfner, Anne Kleinert, Tom Neubert, Björn-Martin Sinnhuber, and Jörn Ungermann
Atmos. Chem. Phys., 22, 3675–3691, https://doi.org/10.5194/acp-22-3675-2022, https://doi.org/10.5194/acp-22-3675-2022, 2022
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We present GLORIA airborne cross sections of PAN, C2H6, HCOOH, CH3OH, and C2H4 in the South Atlantic UTLS in September/October 2019. Filamentary structures and a large plume were observed. Backward trajectories indicate that measured pollutants come from South America and central Africa. Comparisons to CAMS show structural agreement of the measured distributions. PAN absolute VMRs agree with the GLORIA measurements, C2H6 and HCOOH are simulated too low, and CH3OH and C2H4 are too high.
Guangyu Liu, Toshihiko Hirooka, Nawo Eguchi, and Kirstin Krüger
Atmos. Chem. Phys., 22, 3493–3505, https://doi.org/10.5194/acp-22-3493-2022, https://doi.org/10.5194/acp-22-3493-2022, 2022
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The sudden stratospheric warming (SSW) event that occurred in September 2019 in the Southern Hemisphere was analyzed. A large warming and decelerated westerly winds were observed in the southern polar region. Since a reversal from westerly to easterly winds did not take place SSW2019 was classified as a minor SSW. The total wave forcing and the contribution from PW1 were larger in 2019. The strong and long-lasting planetary-scale waves with zonal wavenumber 1 played a role in SSW2019.
Florian Haenel, Wolfgang Woiwode, Jennifer Buchmüller, Felix Friedl-Vallon, Michael Höpfner, Sören Johansson, Farahnaz Khosrawi, Oliver Kirner, Anne Kleinert, Hermann Oelhaf, Johannes Orphal, Roland Ruhnke, Björn-Martin Sinnhuber, Jörn Ungermann, Michael Weimer, and Peter Braesicke
Atmos. Chem. Phys., 22, 2843–2870, https://doi.org/10.5194/acp-22-2843-2022, https://doi.org/10.5194/acp-22-2843-2022, 2022
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We compare remote sensing observations of H2O, O3, HNO3 and clouds in the upper troposphere–lowermost stratosphere during an Arctic winter long-range research flight with simulations by two different state-of-the-art model systems. We find good agreement for dynamical structures, trace gas distributions and clouds. We investigate model biases and sensitivities, with the goal of aiding model development and improving our understanding of processes in the upper troposphere–lowermost stratosphere.
Lei Hu, Stephen A. Montzka, Fred Moore, Eric Hintsa, Geoff Dutton, M. Carolina Siso, Kirk Thoning, Robert W. Portmann, Kathryn McKain, Colm Sweeney, Isaac Vimont, David Nance, Bradley Hall, and Steven Wofsy
Atmos. Chem. Phys., 22, 2891–2907, https://doi.org/10.5194/acp-22-2891-2022, https://doi.org/10.5194/acp-22-2891-2022, 2022
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The unexpected increase in CFC-11 emissions between 2012 and 2017 resulted in concerns about delaying the stratospheric ozone recovery. Although the subsequent decline of CFC-11 emissions indicated a mitigation in part to this problem, the regions fully responsible for these large emission changes were unclear. Here, our new estimate, based on atmospheric measurements from two global campaigns and from NOAA, suggests Asia primarily contributed to the global CFC-11 emission rise during 2012–2017.
Marine Remaud, Frédéric Chevallier, Fabienne Maignan, Sauveur Belviso, Antoine Berchet, Alexandra Parouffe, Camille Abadie, Cédric Bacour, Sinikka Lennartz, and Philippe Peylin
Atmos. Chem. Phys., 22, 2525–2552, https://doi.org/10.5194/acp-22-2525-2022, https://doi.org/10.5194/acp-22-2525-2022, 2022
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Carbonyl sulfide (COS) has been recognized as a promising indicator of the plant gross primary production (GPP). Here, we assimilate both COS and CO2 measurements into an atmospheric transport model to obtain information on GPP, plant respiration and COS budget. A possible scenario for the period 2008–2019 leads to a global COS biospheric sink of 800 GgS yr−1 and higher oceanic emissions between 400 and 600 GgS yr−1.
Yanan Zhao, Dennis Booge, Christa A. Marandino, Cathleen Schlundt, Astrid Bracher, Elliot L. Atlas, Jonathan Williams, and Hermann W. Bange
Biogeosciences, 19, 701–714, https://doi.org/10.5194/bg-19-701-2022, https://doi.org/10.5194/bg-19-701-2022, 2022
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We present here, for the first time, simultaneously measured dimethylsulfide (DMS) seawater concentrations and DMS atmospheric mole fractions from the Peruvian upwelling region during two cruises in December 2012 and October 2015. Our results indicate low oceanic DMS concentrations and atmospheric DMS molar fractions in surface waters and the atmosphere, respectively. In addition, the Peruvian upwelling region was identified as an insignificant source of DMS emissions during both periods.
Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Ryan Hossaini, Graham W. Mann, Michelle L. Santee, and Mark Weber
Atmos. Chem. Phys., 22, 903–916, https://doi.org/10.5194/acp-22-903-2022, https://doi.org/10.5194/acp-22-903-2022, 2022
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Solar flux variations associated with 11-year sunspot cycle is believed to exert important external climate forcing. As largest variations occur at shorter wavelengths such as ultra-violet part of the solar spectrum, associated changes in stratospheric ozone are thought to provide direct evidence for solar climate interaction. Until now, most of the studies reported double-peak structured solar cycle signal (SCS), but relatively new satellite data suggest only single-peak-structured SCS.
Michael Höpfner, Oliver Kirner, Gerald Wetzel, Björn-Martin Sinnhuber, Florian Haenel, Sören Johansson, Johannes Orphal, Roland Ruhnke, Gabriele Stiller, and Thomas von Clarmann
Atmos. Chem. Phys., 21, 18433–18464, https://doi.org/10.5194/acp-21-18433-2021, https://doi.org/10.5194/acp-21-18433-2021, 2021
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BrONO2 is an important reservoir gas for inorganic stratospheric bromine linked to the chemical cycles of stratospheric ozone depletion. Presently infrared limb sounding is the only way to measure BrONO2 in the atmosphere. We provide global distributions of BrONO2 derived from MIPAS observations 2002–2012. Comparisons with EMAC atmospheric modelling show an overall agreement and enable us to derive an independent estimate of stratospheric bromine of 21.2±1.4pptv based on the BrONO2 measurements.
Markus Jesswein, Heiko Bozem, Hans-Christoph Lachnitt, Peter Hoor, Thomas Wagenhäuser, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 21, 17225–17241, https://doi.org/10.5194/acp-21-17225-2021, https://doi.org/10.5194/acp-21-17225-2021, 2021
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This study presents and compares inorganic chlorine (Cly) derived from observations with the HALO research aircraft in the Antarctic late winter–early fall 2019 and the Arctic winter 2015–2016. Trend-corrected correlations from the Northern Hemisphere show excellent agreement with those from the Southern Hemisphere. After observation allocation inside and outside the vortex based on N2O measurements, results of the two campaigns reveal substantial differences in Cly within the respective vortex.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Eric J. Hintsa, Fred L. Moore, Dale F. Hurst, Geoff S. Dutton, Bradley D. Hall, J. David Nance, Ben R. Miller, Stephen A. Montzka, Laura P. Wolton, Audra McClure-Begley, James W. Elkins, Emrys G. Hall, Allen F. Jordan, Andrew W. Rollins, Troy D. Thornberry, Laurel A. Watts, Chelsea R. Thompson, Jeff Peischl, Ilann Bourgeois, Thomas B. Ryerson, Bruce C. Daube, Yenny Gonzalez Ramos, Roisin Commane, Gregory W. Santoni, Jasna V. Pittman, Steven C. Wofsy, Eric Kort, Glenn S. Diskin, and T. Paul Bui
Atmos. Meas. Tech., 14, 6795–6819, https://doi.org/10.5194/amt-14-6795-2021, https://doi.org/10.5194/amt-14-6795-2021, 2021
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We built UCATS to study atmospheric chemistry and transport. It has measured trace gases including CFCs, N2O, SF6, CH4, CO, and H2 with gas chromatography, as well as ozone and water vapor. UCATS has been part of missions to study the tropical tropopause; transport of air into the stratosphere; greenhouse gases, transport, and chemistry in the troposphere; and ozone chemistry, on both piloted and unmanned aircraft. Its design, capabilities, and some results are shown and described here.
Meike K. Rotermund, Vera Bense, Martyn P. Chipperfield, Andreas Engel, Jens-Uwe Grooß, Peter Hoor, Tilman Hüneke, Timo Keber, Flora Kluge, Benjamin Schreiner, Tanja Schuck, Bärbel Vogel, Andreas Zahn, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 15375–15407, https://doi.org/10.5194/acp-21-15375-2021, https://doi.org/10.5194/acp-21-15375-2021, 2021
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Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses persistently protruded into the lower stratosphere (LS), creating a high Brtot region over the North Atlantic in fall 2017. The main source is via isentropic transport by the Asian monsoon and to a lesser extent transport across the extratropical tropopause as quantified by a Lagrange model. The transport of Brtot via Central American hurricanes is also observed. Lastly, the impact of Brtot on LS O3 is assessed.
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.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke D. Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul A. Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 11113–11132, https://doi.org/10.5194/acp-21-11113-2021, https://doi.org/10.5194/acp-21-11113-2021, 2021
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected nearly from pole to pole over the oceans during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigated their impact on the variability of tropospheric N2O.
Stefanie Kremser, Mike Harvey, Peter Kuma, Sean Hartery, Alexia Saint-Macary, John McGregor, Alex Schuddeboom, Marc von Hobe, Sinikka T. Lennartz, Alex Geddes, Richard Querel, Adrian McDonald, Maija Peltola, Karine Sellegri, Israel Silber, Cliff S. Law, Connor J. Flynn, Andrew Marriner, Thomas C. J. Hill, Paul J. DeMott, Carson C. Hume, Graeme Plank, Geoffrey Graham, and Simon Parsons
Earth Syst. Sci. Data, 13, 3115–3153, https://doi.org/10.5194/essd-13-3115-2021, https://doi.org/10.5194/essd-13-3115-2021, 2021
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Aerosol–cloud interactions over the Southern Ocean are poorly understood and remain a major source of uncertainty in climate models. This study presents ship-borne measurements, collected during a 6-week voyage into the Southern Ocean in 2018, that are an important supplement to satellite-based measurements. For example, these measurements include data on low-level clouds and aerosol composition in the marine boundary layer, which can be used in climate model evaluation efforts.
Gerald Wetzel, Felix Friedl-Vallon, Norbert Glatthor, Jens-Uwe Grooß, Thomas Gulde, Michael Höpfner, Sören Johansson, Farahnaz Khosrawi, Oliver Kirner, Anne Kleinert, Erik Kretschmer, Guido Maucher, Hans Nordmeyer, Hermann Oelhaf, Johannes Orphal, Christof Piesch, Björn-Martin Sinnhuber, Jörn Ungermann, and Bärbel Vogel
Atmos. Chem. Phys., 21, 8213–8232, https://doi.org/10.5194/acp-21-8213-2021, https://doi.org/10.5194/acp-21-8213-2021, 2021
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Measurements of the pollutants C2H6, C2H2, HCOOH, and PAN were performed in the North Atlantic UTLS region with the airborne limb imager GLORIA in 2017. Enhanced amounts of these species were detected in the upper troposphere and even in the lowermost stratosphere (PAN). Main sources of these gases are forest fires in North America and anthropogenic pollution in South Asia. Simulations of EMAC and CAMS are qualitatively able to reproduce the measured data but underestimate the absolute amounts.
Sinikka T. Lennartz, Michael Gauss, Marc von Hobe, and Christa A. Marandino
Earth Syst. Sci. Data, 13, 2095–2110, https://doi.org/10.5194/essd-13-2095-2021, https://doi.org/10.5194/essd-13-2095-2021, 2021
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This study provides a marine emission inventory for the sulphur gases carbonyl sulphide (OCS) and carbon disulphide (CS2), derived from a numerical model of the surface ocean at monthly resolution for the period 2000–2019. Comparison with a database of seaborne observations reveals very good agreement for OCS. Interannual variability in both gases seems to be mainly driven by the amount of chromophoric dissolved organic matter present in surface water.
Fabienne Maignan, Camille Abadie, Marine Remaud, Linda M. J. Kooijmans, Kukka-Maaria Kohonen, Róisín Commane, Richard Wehr, J. Elliott Campbell, Sauveur Belviso, Stephen A. Montzka, Nina Raoult, Ulli Seibt, Yoichi P. Shiga, Nicolas Vuichard, Mary E. Whelan, and Philippe Peylin
Biogeosciences, 18, 2917–2955, https://doi.org/10.5194/bg-18-2917-2021, https://doi.org/10.5194/bg-18-2917-2021, 2021
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The assimilation of carbonyl sulfide (COS) by continental vegetation has been proposed as a proxy for gross primary production (GPP). Using a land surface and a transport model, we compare a mechanistic representation of the plant COS uptake (Berry et al., 2013) to the classical leaf relative uptake (LRU) approach linking GPP and vegetation COS fluxes. We show that at high temporal resolutions a mechanistic approach is mandatory, but at large scales the LRU approach compares similarly.
Michaela I. Hegglin, Susann Tegtmeier, John Anderson, Adam E. Bourassa, Samuel Brohede, Doug Degenstein, Lucien Froidevaux, Bernd Funke, John Gille, Yasuko Kasai, Erkki T. Kyrölä, Jerry Lumpe, Donal Murtagh, Jessica L. Neu, Kristell Pérot, Ellis E. Remsberg, Alexei Rozanov, Matthew Toohey, Joachim Urban, Thomas von Clarmann, Kaley A. Walker, Hsiang-Jui Wang, Carlo Arosio, Robert Damadeo, Ryan A. Fuller, Gretchen Lingenfelser, Christopher McLinden, Diane Pendlebury, Chris Roth, Niall J. Ryan, Christopher Sioris, Lesley Smith, and Katja Weigel
Earth Syst. Sci. Data, 13, 1855–1903, https://doi.org/10.5194/essd-13-1855-2021, https://doi.org/10.5194/essd-13-1855-2021, 2021
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An overview of the SPARC Data Initiative is presented, to date the most comprehensive assessment of stratospheric composition measurements spanning 1979–2018. Measurements of 26 chemical constituents obtained from an international suite of space-based limb sounders were compiled into vertically resolved, zonal monthly mean time series. The quality and consistency of these gridded datasets are then evaluated using a climatological validation approach and a range of diagnostics.
Stijn Naus, Stephen A. Montzka, Prabir K. Patra, and Maarten C. Krol
Atmos. Chem. Phys., 21, 4809–4824, https://doi.org/10.5194/acp-21-4809-2021, https://doi.org/10.5194/acp-21-4809-2021, 2021
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Following up on previous box model studies, we employ a 3D transport model to estimate variations in the hydroxyl radical (OH) from observations of methyl chloroform (MCF). We derive small interannual OH variations that are consistent with variations in the El Niño–Southern Oscillation. We also find evidence for the release of MCF from oceans in atmospheric gradients of MCF. Both findings highlight the added value of a 3D transport model since box model studies did not identify these effects.
Josefine Maas, Susann Tegtmeier, Yue Jia, Birgit Quack, Jonathan V. Durgadoo, and Arne Biastoch
Atmos. Chem. Phys., 21, 4103–4121, https://doi.org/10.5194/acp-21-4103-2021, https://doi.org/10.5194/acp-21-4103-2021, 2021
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Cooling-water disinfection at coastal power plants is a known source of atmospheric bromoform. A large source of anthropogenic bromoform is the industrial regions in East Asia. In current bottom-up flux estimates, these anthropogenic emissions are missing, underestimating the global air–sea flux of bromoform. With transport simulations, we show that by including anthropogenic bromoform from cooling-water treatment, the bottom-up flux estimates significantly improve in East and Southeast Asia.
Jin Ma, Linda M. J. Kooijmans, Ara Cho, Stephen A. Montzka, Norbert Glatthor, John R. Worden, Le Kuai, Elliot L. Atlas, and Maarten C. Krol
Atmos. Chem. Phys., 21, 3507–3529, https://doi.org/10.5194/acp-21-3507-2021, https://doi.org/10.5194/acp-21-3507-2021, 2021
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Carbonyl sulfide is an important trace gas in the atmosphere and useful to estimating gross primary productivity in ecosystems, but its sources and sinks remain highly uncertain. Therefore, we applied inverse model system TM5-4DVAR to better constrain the global budget. Our finding is in line with earlier studies, pointing to missing sources in the tropics and more uptake in high latitudes. We also stress the necessity of more ground-based observations and satellite data assimilation in future.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
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.
Malte Meinshausen, Zebedee R. J. Nicholls, Jared Lewis, Matthew J. Gidden, Elisabeth Vogel, Mandy Freund, Urs Beyerle, Claudia Gessner, Alexander Nauels, Nico Bauer, Josep G. Canadell, John S. Daniel, Andrew John, Paul B. Krummel, Gunnar Luderer, Nicolai Meinshausen, Stephen A. Montzka, Peter J. Rayner, Stefan Reimann, Steven J. Smith, Marten van den Berg, Guus J. M. Velders, Martin K. Vollmer, and Ray H. J. Wang
Geosci. Model Dev., 13, 3571–3605, https://doi.org/10.5194/gmd-13-3571-2020, https://doi.org/10.5194/gmd-13-3571-2020, 2020
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This study provides the future greenhouse gas (GHG) concentrations under the new set of so-called SSP scenarios (the successors of the IPCC SRES and previous representative concentration pathway (RCP) scenarios). The projected CO2 concentrations range from 350 ppm for low-emission scenarios by 2150 to more than 2000 ppm under the high-emission scenarios. We also provide concentrations, latitudinal gradients, and seasonality for most of the other 42 considered GHGs.
Jonathon S. Wright, Xiaoyi Sun, Paul Konopka, Kirstin Krüger, Bernard Legras, Andrea M. Molod, Susann Tegtmeier, Guang J. Zhang, and Xi Zhao
Atmos. Chem. Phys., 20, 8989–9030, https://doi.org/10.5194/acp-20-8989-2020, https://doi.org/10.5194/acp-20-8989-2020, 2020
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High clouds are influential in tropical climate. Although reanalysis cloud fields are essentially model products, they are indirectly constrained by observations and offer global coverage with direct links to advanced water and energy cycle metrics, giving them many useful applications. We describe how high cloud fields are generated in reanalyses, assess their realism and reliability in the tropics, and evaluate how differences in these fields affect other aspects of the reanalysis state.
Marius Hauck, Harald Bönisch, Peter Hoor, Timo Keber, Felix Ploeger, Tanja J. Schuck, and Andreas Engel
Atmos. Chem. Phys., 20, 8763–8785, https://doi.org/10.5194/acp-20-8763-2020, https://doi.org/10.5194/acp-20-8763-2020, 2020
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This study features an extended inversion method that includes transport across the extratropical tropopause to derive age spectra in the lowermost stratosphere from in situ trace gas measurements. The refined method is validated in a model setup and applied to data gained with the HALO research aircraft. Results are congruent with the findings of previous studies so that the method provides a promising toolset for the analysis of stratospheric dynamics based on observations in the future.
Frauke Fritsch, Hella Garny, Andreas Engel, Harald Bönisch, and Roland Eichinger
Atmos. Chem. Phys., 20, 8709–8725, https://doi.org/10.5194/acp-20-8709-2020, https://doi.org/10.5194/acp-20-8709-2020, 2020
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We test two methods to derive age of air as a diagnostic of the Brewer–Dobson circulation from non-linear increasing trace gases such as SF6 using a chemistry-climate model and observations. Both the model and the observations show systematic variation of the age of air trend dependent on the chosen assumptions that are required when deriving age of air from measurements. This provides insight into the differences in age of air trends of observations and models.
Sarah A. Strode, James S. Wang, Michael Manyin, Bryan Duncan, Ryan Hossaini, Christoph A. Keller, Sylvia E. Michel, and James W. C. White
Atmos. Chem. Phys., 20, 8405–8419, https://doi.org/10.5194/acp-20-8405-2020, https://doi.org/10.5194/acp-20-8405-2020, 2020
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The 13C : 12C isotopic ratio in methane (CH4) provides information about CH4 sources, but loss of CH4 by reaction with OH and chlorine (Cl) also affects this ratio. Tropospheric Cl provides a small and uncertain sink for CH4 but has a large effect on its isotopic ratio. We use the GEOS model with several different Cl fields to test the sensitivity of methane's isotopic composition to tropospheric Cl. Cl affects the global mean, hemispheric gradient, and seasonal cycle of the isotopic ratio.
Xiao Ma, Mingshuang Sun, Sinikka T. Lennartz, and Hermann W. Bange
Biogeosciences, 17, 3427–3438, https://doi.org/10.5194/bg-17-3427-2020, https://doi.org/10.5194/bg-17-3427-2020, 2020
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Monthly measurements of dissolved methane (CH4), a potent greenhouse gas, were conducted at Boknis Eck (BE), a time-series station in the southwestern Baltic Sea, from June 2006. In general CH4 concentrations increased with depth. High concentrations in the upper layer were linked to saline water inflow. Eckernförde Bay emitted CH4 to the atmosphere throughout the monitoring period. No significant trend was detected in CH4 concentrations or emissions during 2006–2017.
Susann Tegtmeier, Elliot Atlas, Birgit Quack, Franziska Ziska, and Kirstin Krüger
Atmos. Chem. Phys., 20, 7103–7123, https://doi.org/10.5194/acp-20-7103-2020, https://doi.org/10.5194/acp-20-7103-2020, 2020
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We investigate emissions of brominated gases from the ocean and their contribution to stratospheric ozone depletion. Once in the atmosphere, these gases usually break down in less than 6 months. Their impact on the ozone layer depends on the prevailing atmospheric circulation, since transport to the stratosphere requires uplift. We combine aircraft and ship observations with atmospheric modelling to analyse how, where, and when these gases are transported from the ocean into the stratosphere.
Hans Brenna, Steffen Kutterolf, Michael J. Mills, and Kirstin Krüger
Atmos. Chem. Phys., 20, 6521–6539, https://doi.org/10.5194/acp-20-6521-2020, https://doi.org/10.5194/acp-20-6521-2020, 2020
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The Los Chocoyos supereruption (84 000 years ago) in Guatemala was one of the largest volcanic events of the last 100 000 years. This eruption released enormous amounts of sulfur, which cooled the climate, as well as chlorine and bromine, which destroyed the ozone in the stratosphere. We have simulated this eruption by using an advanced chemistry–climate model. We found a collapse in the ozone layer lasting more than 10 years, increased surface–UV radiation, and a 30-year climate-cooling period.
Timo Keber, Harald Bönisch, Carl Hartick, Marius Hauck, Fides Lefrancois, Florian Obersteiner, Akima Ringsdorf, Nils Schohl, Tanja Schuck, Ryan Hossaini, Phoebe Graf, Patrick Jöckel, and Andreas Engel
Atmos. Chem. Phys., 20, 4105–4132, https://doi.org/10.5194/acp-20-4105-2020, https://doi.org/10.5194/acp-20-4105-2020, 2020
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In this paper we summarize observations of short-lived halocarbons in the tropopause region. We show that, especially during winter, the levels of short-lived bromine gases at the extratropical tropopause are higher than at the tropical tropopause. We discuss the impact of the distributions on stratospheric bromine levels and compare our observations to two models with four different emission scenarios.
Sinikka T. Lennartz, Christa A. Marandino, Marc von Hobe, Meinrat O. Andreae, Kazushi Aranami, Elliot Atlas, Max Berkelhammer, Heinz Bingemer, Dennis Booge, Gregory Cutter, Pau Cortes, Stefanie Kremser, Cliff S. Law, Andrew Marriner, Rafel Simó, Birgit Quack, Günther Uher, Huixiang Xie, and Xiaobin Xu
Earth Syst. Sci. Data, 12, 591–609, https://doi.org/10.5194/essd-12-591-2020, https://doi.org/10.5194/essd-12-591-2020, 2020
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Sulfur-containing trace gases in the atmosphere influence atmospheric chemistry and the energy budget of the Earth by forming aerosols. The ocean is an important source of the most abundant sulfur gas in the atmosphere, carbonyl sulfide (OCS) and its most important precursor carbon disulfide (CS2). In order to assess global variability of the sea surface concentrations of both gases to calculate their oceanic emissions, we have compiled a database of existing shipborne measurements.
Susann Tegtmeier, James Anstey, Sean Davis, Rossana Dragani, Yayoi Harada, Ioana Ivanciu, Robin Pilch Kedzierski, Kirstin Krüger, Bernard Legras, Craig Long, James S. Wang, Krzysztof Wargan, and Jonathon S. Wright
Atmos. Chem. Phys., 20, 753–770, https://doi.org/10.5194/acp-20-753-2020, https://doi.org/10.5194/acp-20-753-2020, 2020
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The tropical tropopause layer is an important atmospheric region right in between the troposphere and the stratosphere. We evaluate the representation of this layer in reanalyses data sets, which create a complete picture of the state of Earth's atmosphere using atmospheric modeling and available observations. The recent reanalyses show realistic temperatures in the tropical tropopause layer. However, where the temperature is lowest, the so-called cold point, the reanalyses are too cold.
Elizabeth Asher, Rebecca S. Hornbrook, Britton B. Stephens, Doug Kinnison, Eric J. Morgan, Ralph F. Keeling, Elliot L. Atlas, Sue M. Schauffler, Simone Tilmes, Eric A. Kort, Martin S. Hoecker-Martínez, Matt C. Long, Jean-François Lamarque, Alfonso Saiz-Lopez, Kathryn McKain, Colm Sweeney, Alan J. Hills, and Eric C. Apel
Atmos. Chem. Phys., 19, 14071–14090, https://doi.org/10.5194/acp-19-14071-2019, https://doi.org/10.5194/acp-19-14071-2019, 2019
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Halogenated organic trace gases, which are a source of reactive halogens to the atmosphere, exert a disproportionately large influence on atmospheric chemistry and climate. This paper reports novel aircraft observations of halogenated compounds over the Southern Ocean in summer and evaluates hypothesized regional sources and emissions of these trace gases through their relationships to additional aircraft observations.
Marleen Braun, Jens-Uwe Grooß, Wolfgang Woiwode, Sören Johansson, Michael Höpfner, Felix Friedl-Vallon, Hermann Oelhaf, Peter Preusse, Jörn Ungermann, Björn-Martin Sinnhuber, Helmut Ziereis, and Peter Braesicke
Atmos. Chem. Phys., 19, 13681–13699, https://doi.org/10.5194/acp-19-13681-2019, https://doi.org/10.5194/acp-19-13681-2019, 2019
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We analyse nitrification of the LMS in the Arctic winter 2015–2016 based on GLORIA measurements. Vertical cross sections of HNO3 for several flights show complex fine–scale structures and enhanced values down to 9 km. The extent of overall nitrification is quantified based on HNO3–O3 correlations and reaches between 5 ppbv and 7 ppbv at potential temperature levels between 350 and 380 K. Further, we compare our result with the atmospheric model CLaMS.
Xiao Ma, Sinikka T. Lennartz, and Hermann W. Bange
Biogeosciences, 16, 4097–4111, https://doi.org/10.5194/bg-16-4097-2019, https://doi.org/10.5194/bg-16-4097-2019, 2019
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Monthly measurements of nitrous oxide (N2O), a potent greenhouse gas and ozone depletion agent, were conducted at Boknis Eck (BE), a time series station in the southwestern Baltic Sea, since July 2005. Low N2O concentrations were observed in autumn and high in winter and early spring. Dissolved nutrients and oxygen played important roles in N2O distribution. Although we did not observe a significant N2O trend during 2005–2017, a decrease in N2O concentration and emission seems likely in future.
Vanessa Brocchi, Gisèle Krysztofiak, Adrien Deroubaix, Greta Stratmann, Daniel Sauer, Hans Schlager, Konrad Deetz, Guillaume Dayma, Claude Robert, Stéphane Chevrier, and Valéry Catoire
Atmos. Chem. Phys., 19, 11401–11411, https://doi.org/10.5194/acp-19-11401-2019, https://doi.org/10.5194/acp-19-11401-2019, 2019
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This study reports the first flaring in situ measurements in southern West Africa. According to the measurements, oil rig flaring plumes in Ghana lead to increases in NO2 and aerosols but not always in CO and not in SO2. Flaring measurements can be reproduced using FLEXPART model, adjusting both the emission flux and the injection height. The DACCIWA satellite flaring inventory provides a reasonable estimate of flaring emission.
Yue Jia, Susann Tegtmeier, Elliot Atlas, and Birgit Quack
Atmos. Chem. Phys., 19, 11089–11103, https://doi.org/10.5194/acp-19-11089-2019, https://doi.org/10.5194/acp-19-11089-2019, 2019
Ulrike Niemeier, Claudia Timmreck, and Kirstin Krüger
Atmos. Chem. Phys., 19, 10379–10390, https://doi.org/10.5194/acp-19-10379-2019, https://doi.org/10.5194/acp-19-10379-2019, 2019
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In 1963 Mt. Agung, Indonesia, showed unrest for several months. During this period,
two medium-sized eruptions injected SO2 into the stratosphere. Recent volcanic emission datasets include only one large eruption phase. Therefore, we compared model experiments, with (a) one larger eruption and (b) two eruptions as observed. The evolution of the volcanic cloud differs significantly between the two experiments. Both climatic eruptions should be taken into account.
Sinikka T. Lennartz, Marc von Hobe, Dennis Booge, Henry C. Bittig, Tim Fischer, Rafael Gonçalves-Araujo, Kerstin B. Ksionzek, Boris P. Koch, Astrid Bracher, Rüdiger Röttgers, Birgit Quack, and Christa A. Marandino
Ocean Sci., 15, 1071–1090, https://doi.org/10.5194/os-15-1071-2019, https://doi.org/10.5194/os-15-1071-2019, 2019
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The ocean emits the gases carbonyl sulfide (OCS) and carbon disulfide (CS2), which affect our climate. The goal of this study was to quantify the rates at which both gases are produced in the eastern tropical South Pacific (ETSP), one of the most productive oceanic regions worldwide. Both gases are produced by reactions triggered by sunlight, but we found that the amount produced depends on different factors. Our results improve numerical models to predict oceanic concentrations of both gases.
Xin Chen, Dylan B. Millet, Hanwant B. Singh, Armin Wisthaler, Eric C. Apel, Elliot L. Atlas, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, John D. Crounse, Joost A. de Gouw, Frank M. Flocke, Alan Fried, Brian G. Heikes, Rebecca S. Hornbrook, Tomas Mikoviny, Kyung-Eun Min, Markus Müller, J. Andrew Neuman, Daniel W. O'Sullivan, Jeff Peischl, Gabriele G. Pfister, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Stephen R. Shertz, Chelsea R. Thompson, Victoria Treadaway, Patrick R. Veres, James Walega, Carsten Warneke, Rebecca A. Washenfelder, Petter Weibring, and Bin Yuan
Atmos. Chem. Phys., 19, 9097–9123, https://doi.org/10.5194/acp-19-9097-2019, https://doi.org/10.5194/acp-19-9097-2019, 2019
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Volatile organic compounds (VOCs) affect air quality and modify the lifetimes of other pollutants. We combine a high-resolution 3-D atmospheric model with an ensemble of aircraft observations to perform an integrated analysis of the VOC budget over North America. We find that biogenic emissions provide the main source of VOC reactivity even in most major cities. Our findings point to key gaps in current models related to oxygenated VOCs and to the distribution of VOCs in the free troposphere.
Josefine Maas, Susann Tegtmeier, Birgit Quack, Arne Biastoch, Jonathan V. Durgadoo, Siren Rühs, Stephan Gollasch, and Matej David
Ocean Sci., 15, 891–904, https://doi.org/10.5194/os-15-891-2019, https://doi.org/10.5194/os-15-891-2019, 2019
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In a large-scale analysis, the spread of disinfection by-products from oxidative ballast water treatment is investigated, with a focus on Southeast Asia where major ports are located. Halogenated compounds such as bromoform (CHBr3) are produced in the ballast water and, once emitted into the environment, can participate in ozone depletion. Anthropogenic bromoform is rapidly emitted into the atmosphere and can locally double around large ports. A large-scale impact cannot be found.
Sören Johansson, Michelle L. Santee, Jens-Uwe Grooß, Michael Höpfner, Marleen Braun, Felix Friedl-Vallon, Farahnaz Khosrawi, Oliver Kirner, Erik Kretschmer, Hermann Oelhaf, Johannes Orphal, Björn-Martin Sinnhuber, Ines Tritscher, Jörn Ungermann, Kaley A. Walker, and Wolfgang Woiwode
Atmos. Chem. Phys., 19, 8311–8338, https://doi.org/10.5194/acp-19-8311-2019, https://doi.org/10.5194/acp-19-8311-2019, 2019
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We present a study based on GLORIA aircraft and MLS/ACE-FTS/CALIOP satellite measurements during the Arctic winter 2015/16, which demonstrate (for the Arctic) unusual chlorine deactivation into HCl instead of ClONO2 due to low ozone abundances in the lowermost stratosphere, with a focus at 380 K potential temperature. The atmospheric models CLaMS and EMAC are evaluated, and measured ClONO2 is linked with transport and in situ deactivation in the lowermost stratosphere.
Alexander Zavarsky and Christa A. Marandino
Atmos. Chem. Phys., 19, 1819–1834, https://doi.org/10.5194/acp-19-1819-2019, https://doi.org/10.5194/acp-19-1819-2019, 2019
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Wind–wave interaction can suppress gas transfer between the atmosphere and the ocean. Using a global wave model we investigate the impact of this interaction on the global gas transfer of CO2 and DMS. We also investigate the impact on of gas transfer limitation on two commonly used gas transfer velocity parameterizations.
Roland Eichinger, Simone Dietmüller, Hella Garny, Petr Šácha, Thomas Birner, Harald Bönisch, Giovanni Pitari, Daniele Visioni, Andrea Stenke, Eugene Rozanov, Laura Revell, David A. Plummer, Patrick Jöckel, Luke Oman, Makoto Deushi, Douglas E. Kinnison, Rolando Garcia, Olaf Morgenstern, Guang Zeng, Kane Adam Stone, and Robyn Schofield
Atmos. Chem. Phys., 19, 921–940, https://doi.org/10.5194/acp-19-921-2019, https://doi.org/10.5194/acp-19-921-2019, 2019
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To shed more light upon the changes in stratospheric circulation in the 21st century, climate projection simulations of 10 state-of-the-art global climate models, spanning from 1960 to 2100, are analyzed. The study shows that in addition to changes in transport, mixing also plays an important role in stratospheric circulation and that the properties of mixing vary over time. Furthermore, the influence of mixing is quantified and a dynamical framework is provided to understand the changes.
Pingyang Li, Jens Mühle, Stephen A. Montzka, David E. Oram, Benjamin R. Miller, Ray F. Weiss, Paul J. Fraser, and Toste Tanhua
Ocean Sci., 15, 33–60, https://doi.org/10.5194/os-15-33-2019, https://doi.org/10.5194/os-15-33-2019, 2019
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Use of CFCs as oceanic transient tracers is difficult for recently ventilated water masses as their atmospheric mole fractions have been decreasing. To explore novel tracers, we synthesized consistent annual mean atmospheric histories of HCFC-22, HCFC-141b, HCFC-142b, HFC-134a, HFC-125, HFC-23, PFC-14 (CF4) and PFC-116 in both hemispheres and reconstructed their solubility functions in water and seawater. This work is also potentially useful for tracer studies in a range of natural waters.
Stijn Naus, Stephen A. Montzka, Sudhanshu Pandey, Sourish Basu, Ed J. Dlugokencky, and Maarten Krol
Atmos. Chem. Phys., 19, 407–424, https://doi.org/10.5194/acp-19-407-2019, https://doi.org/10.5194/acp-19-407-2019, 2019
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We investigate how the use of a two-box model to describe the troposphere can impact derived results, relative to more complex models. For this, we use a 3-D transport model to tune a two-box model of OH, CH4, and MCF. By comparing the tuned two-box model with a standard model run, we can diagnose and quantify biases inherent to a two-box model. We find strong biases, but these have only a small impact on our final conclusions. However, it is not obvious that this should hold for future studies.
Joe McNorton, Chris Wilson, Manuel Gloor, Rob J. Parker, Hartmut Boesch, Wuhu Feng, Ryan Hossaini, and Martyn P. Chipperfield
Atmos. Chem. Phys., 18, 18149–18168, https://doi.org/10.5194/acp-18-18149-2018, https://doi.org/10.5194/acp-18-18149-2018, 2018
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Since 2007 atmospheric methane (CH4) has been unexpectedly increasing following a 6-year hiatus. We have used an atmospheric model to attribute regional sources and global sinks of CH4 using observations for the 2003–2015 period. Model results show the renewed growth is best explained by decreased atmospheric removal, decreased biomass burning emissions, and an increased energy sector (mainly from Africa–Middle East and Southern Asia–Oceania) and wetland emissions (mainly from northern Eurasia).
Tanja J. Schuck, Fides Lefrancois, Franziska Gallmann, Danrong Wang, Markus Jesswein, Jesica Hoker, Harald Bönisch, and Andreas Engel
Atmos. Chem. Phys., 18, 16553–16569, https://doi.org/10.5194/acp-18-16553-2018, https://doi.org/10.5194/acp-18-16553-2018, 2018
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We present the first results of regular halocarbon measurements at Taunus Observatory, Germany. Halogenated gases contribute to stratospheric ozone depletion and to radiative forcing. Time-of-flight mass spectrometry allows one to assess a large number of compounds; the measurements are expected to provide better constraints for European emission estimates. CFC-11 and CFC-12 show small unexpected differences regarding outlier occurrence and seasonality, indicating ongoing emissions of CFC-11.
Christiane Voigt, Andreas Dörnbrack, Martin Wirth, Silke M. Groß, Michael C. Pitts, Lamont R. Poole, Robert Baumann, Benedikt Ehard, Björn-Martin Sinnhuber, Wolfgang Woiwode, and Hermann Oelhaf
Atmos. Chem. Phys., 18, 15623–15641, https://doi.org/10.5194/acp-18-15623-2018, https://doi.org/10.5194/acp-18-15623-2018, 2018
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The 2015–2016 stratospheric winter was the coldest in the 36-year climatological data record. The extreme conditions promoted the formation of persistent Arctic polar stratospheric ice clouds. An extended ice PSC detected by airborne lidar in January 2016 shows a second mode with higher particle depolarization ratios. Back-trajectories from the high-depol ice matched to CALIOP PSC curtains provide evidence for ice nucleation on NAT. The novel data consolidate our understanding of PSC formation.
Wolfgang Woiwode, Andreas Dörnbrack, Martina Bramberger, Felix Friedl-Vallon, Florian Haenel, Michael Höpfner, Sören Johansson, Erik Kretschmer, Isabell Krisch, Thomas Latzko, Hermann Oelhaf, Johannes Orphal, Peter Preusse, Björn-Martin Sinnhuber, and Jörn Ungermann
Atmos. Chem. Phys., 18, 15643–15667, https://doi.org/10.5194/acp-18-15643-2018, https://doi.org/10.5194/acp-18-15643-2018, 2018
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GLORIA observations during two crossings of the polar front jet stream resolve the fine mesoscale structure of a tropopause fold in high detail. Tracer–tracer correlations of H2O and O3 are presented as a function of potential temperature and reveal an active mixing region. Our study confirms conceptual models of tropopause folds, validates the high quality of ECMWF IFS forecasts, and suggests that mountain waves are capable of modulating exchange processes in the vicinity of tropopause folds.
Robyn Butler, Paul I. Palmer, Liang Feng, Stephen J. Andrews, Elliot L. Atlas, Lucy J. Carpenter, Valeria Donets, Neil R. P. Harris, Stephen A. Montzka, Laura L. Pan, Ross J. Salawitch, and Sue M. Schauffler
Atmos. Chem. Phys., 18, 13135–13153, https://doi.org/10.5194/acp-18-13135-2018, https://doi.org/10.5194/acp-18-13135-2018, 2018
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Natural sources of short-lived bromoform and dibromomethane are important for determining the inorganic bromine budget in the stratosphere that drives ozone loss. Two new modelling techniques describe how different geographical source regions influence their atmospheric variability over the western Pacific. We find that it is driven primarily by open ocean sources, and we use atmospheric observations to help estimate their contributions to the upper tropospheric inorganic bromine budget.
Franz Slemr, Andreas Weigelt, Ralf Ebinghaus, Johannes Bieser, Carl A. M. Brenninkmeijer, Armin Rauthe-Schöch, Markus Hermann, Bengt G. Martinsson, Peter van Velthoven, Harald Bönisch, Marco Neumaier, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 18, 12329–12343, https://doi.org/10.5194/acp-18-12329-2018, https://doi.org/10.5194/acp-18-12329-2018, 2018
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Total and elemental mercury were measured in the upper troposphere and lower stratosphere onboard a passenger aircraft. Their concentrations in the upper troposphere were comparable implying low concentrations of oxidized mercury in this region. Large scale seasonally dependent influence of emissions from biomass burning was also observed. Their distributions in the lower stratosphere implies a long stratospheric lifetime, which precludes significant mercury oxidation by ozone.
Alina Fiehn, Birgit Quack, Irene Stemmler, Franziska Ziska, and Kirstin Krüger
Atmos. Chem. Phys., 18, 11973–11990, https://doi.org/10.5194/acp-18-11973-2018, https://doi.org/10.5194/acp-18-11973-2018, 2018
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Oceanic very short-lived substances, VSLS, contribute to stratospheric halogen loading and ozone depletion. We created bromoform emission inventories with monthly resolution for the tropical Indian Ocean and west Pacific and modeled the atmospheric transport of bromoform with the particle dispersion model FLEXPART/ERA-Interim. Results underline that the seasonal and regional stratospheric bromine entrainment critically depends on the seasonality and spatial distribution of the VSLS emissions.
Sören Johansson, Wolfgang Woiwode, Michael Höpfner, Felix Friedl-Vallon, Anne Kleinert, Erik Kretschmer, Thomas Latzko, Johannes Orphal, Peter Preusse, Jörn Ungermann, Michelle L. Santee, Tina Jurkat-Witschas, Andreas Marsing, Christiane Voigt, Andreas Giez, Martina Krämer, Christian Rolf, Andreas Zahn, Andreas Engel, Björn-Martin Sinnhuber, and Hermann Oelhaf
Atmos. Meas. Tech., 11, 4737–4756, https://doi.org/10.5194/amt-11-4737-2018, https://doi.org/10.5194/amt-11-4737-2018, 2018
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We present two-dimensional cross sections of temperature, HNO3, O3, ClONO2, H2O and CFC-12 from measurements of the GLORIA infrared limb imager during the POLSTRACC/GW-LCYCLE/SALSA aircraft campaigns in the Arctic winter 2015/2016. GLORIA sounded the atmosphere between 5 and 14 km with vertical resolutions of 0.4–1 km. Estimated errors are in the range of 1–2 K (temperature) and 10 %–20 % (trace gases). Comparisons to in situ instruments onboard the aircraft and to Aura/MLS are shown.
Amanda C. Maycock, Katja Matthes, Susann Tegtmeier, Hauke Schmidt, Rémi Thiéblemont, Lon Hood, Hideharu Akiyoshi, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Oliver Kirner, Markus Kunze, Marion Marchand, Daniel R. Marsh, Martine Michou, David Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Yousuke Yamashita, and Kohei Yoshida
Atmos. Chem. Phys., 18, 11323–11343, https://doi.org/10.5194/acp-18-11323-2018, https://doi.org/10.5194/acp-18-11323-2018, 2018
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The 11-year solar cycle is an important driver of climate variability. Changes in incoming solar ultraviolet radiation affect atmospheric ozone, which in turn influences atmospheric temperatures. Constraining the impact of the solar cycle on ozone is therefore important for understanding climate variability. This study examines the representation of the solar influence on ozone in numerical models used to simulate past and future climate. We highlight important differences among model datasets.
Mary E. Whelan, Sinikka T. Lennartz, Teresa E. Gimeno, Richard Wehr, Georg Wohlfahrt, Yuting Wang, Linda M. J. Kooijmans, Timothy W. Hilton, Sauveur Belviso, Philippe Peylin, Róisín Commane, Wu Sun, Huilin Chen, Le Kuai, Ivan Mammarella, Kadmiel Maseyk, Max Berkelhammer, King-Fai Li, Dan Yakir, Andrew Zumkehr, Yoko Katayama, Jérôme Ogée, Felix M. Spielmann, Florian Kitz, Bharat Rastogi, Jürgen Kesselmeier, Julia Marshall, Kukka-Maaria Erkkilä, Lisa Wingate, Laura K. Meredith, Wei He, Rüdiger Bunk, Thomas Launois, Timo Vesala, Johan A. Schmidt, Cédric G. Fichot, Ulli Seibt, Scott Saleska, Eric S. Saltzman, Stephen A. Montzka, Joseph A. Berry, and J. Elliott Campbell
Biogeosciences, 15, 3625–3657, https://doi.org/10.5194/bg-15-3625-2018, https://doi.org/10.5194/bg-15-3625-2018, 2018
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Measurements of the trace gas carbonyl sulfide (OCS) are helpful in quantifying photosynthesis at previously unknowable temporal and spatial scales. While CO2 is both consumed and produced within ecosystems, OCS is mostly produced in the oceans or from specific industries, and destroyed in plant leaves in proportion to CO2. This review summarizes the advancements we have made in the understanding of OCS exchange and applications to vital ecosystem water and carbon cycle questions.
Richard Hyde, Ryan Hossaini, and Amber A. Leeson
Geosci. Model Dev., 11, 2033–2048, https://doi.org/10.5194/gmd-11-2033-2018, https://doi.org/10.5194/gmd-11-2033-2018, 2018
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Clustering, the automated grouping of similar data, can provide powerful insight into large/complex data. We demonstrate the benefits of clustering applied to output from climate model inter-comparison initiatives. We focus on modelled tropospheric ozone from the ACCMIP project. Cluster-based subsampling of the model ensemble can (i) remove outlier data on a grid-cell basis, reducing model–observation bias and (ii) provide a useful framework in which to investigate and visualise model diversity.
Vanessa Brocchi, Gisèle Krysztofiak, Valéry Catoire, Jonathan Guth, Virginie Marécal, Régina Zbinden, Laaziz El Amraoui, François Dulac, and Philippe Ricaud
Atmos. Chem. Phys., 18, 6887–6906, https://doi.org/10.5194/acp-18-6887-2018, https://doi.org/10.5194/acp-18-6887-2018, 2018
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The Mediterranean Basin still suffers from a limited amount of in situ measurements for a good characterization of its environmental state. This study shows that intercontinental transport of very high CO concentrations can affect the upper Mediterranean Basin troposphere. By using modeling, 5- to 12-day eastward transport of biomass burning starting from North America and Siberia impacts the mid-troposphere of the Mediterranean Basin.
Simone Dietmüller, Roland Eichinger, Hella Garny, Thomas Birner, Harald Boenisch, Giovanni Pitari, Eva Mancini, Daniele Visioni, Andrea Stenke, Laura Revell, Eugene Rozanov, David A. Plummer, John Scinocca, Patrick Jöckel, Luke Oman, Makoto Deushi, Shibata Kiyotaka, Douglas E. Kinnison, Rolando Garcia, Olaf Morgenstern, Guang Zeng, Kane Adam Stone, and Robyn Schofield
Atmos. Chem. Phys., 18, 6699–6720, https://doi.org/10.5194/acp-18-6699-2018, https://doi.org/10.5194/acp-18-6699-2018, 2018
Jens Krause, Peter Hoor, Andreas Engel, Felix Plöger, Jens-Uwe Grooß, Harald Bönisch, Timo Keber, Björn-Martin Sinnhuber, Wolfgang Woiwode, and Hermann Oelhaf
Atmos. Chem. Phys., 18, 6057–6073, https://doi.org/10.5194/acp-18-6057-2018, https://doi.org/10.5194/acp-18-6057-2018, 2018
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We present tracer measurements of CO and N2O measured during the POLSTRACC aircraft campaign in winter 2015–2016. We found enhanced CO values relative to N2O in the polar lower stratosphere in addition to the ageing of this region during winter. By using model simulations it was possible to link this enhancement to an increased mixing of the tropical tropopause. We thus conclude that the polar lower stratosphere in late winter is strongly influenced by quasi-isentropic mixing from the tropics.
Richard Newton, Geraint Vaughan, Eric Hintsa, Michal T. Filus, Laura L. Pan, Shawn Honomichl, Elliot Atlas, Stephen J. Andrews, and Lucy J. Carpenter
Atmos. Chem. Phys., 18, 5157–5171, https://doi.org/10.5194/acp-18-5157-2018, https://doi.org/10.5194/acp-18-5157-2018, 2018
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We consider the ozone measurements from aircraft during the CAST/CONTRAST/ATTREX campaigns of 2014. Low concentrations of ozone were found in the layer of 10–15 km altitude, which is indicative of uplift of ozone-poor air from near the sea surface to 10–15 km altitude. Chemicals that have origins in the sea were found in greater abundance when ozone concentrations were low compared to when ozone concentrations were high. The lowest ozone concentrations were found in the Southern Hemisphere.
Stefanie Falk and Björn-Martin Sinnhuber
Geosci. Model Dev., 11, 1115–1131, https://doi.org/10.5194/gmd-11-1115-2018, https://doi.org/10.5194/gmd-11-1115-2018, 2018
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Ozone depletion events (ODEs) in the polar boundary layer are observed frequently in spring. ODEs serve as a source of tropospheric BrO at high latitudes. A treatment of bromine release and recycling on sea-ice- and snow-covered surfaces is implemented in global chemistry–climate model EMAC based on a scheme of Toyota et al. (2011). Many aspects of bromine enhancement and associated ODEs are reproduced in both polar regions. Further bromine release mechanisms can now be tested in a global model.
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.
Dennis Booge, Cathleen Schlundt, Astrid Bracher, Sonja Endres, Birthe Zäncker, and Christa A. Marandino
Biogeosciences, 15, 649–667, https://doi.org/10.5194/bg-15-649-2018, https://doi.org/10.5194/bg-15-649-2018, 2018
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Our isoprene data from field measurements in the mixed layer from the Indian Ocean and the eastern Pacific Ocean show that the ability of different phytoplankton functional types to produce isoprene seems to be mainly influenced by light, ocean temperature, salinity, and nutrients. By calculating in-field isoprene production rates, we demonstrate that an additional loss is needed to explain the measured isoprene concentration, which is potentially due to degradation or consumption by bacteria.
Annika Günther, Michael Höpfner, Björn-Martin Sinnhuber, Sabine Griessbach, Terry Deshler, Thomas von Clarmann, and Gabriele Stiller
Atmos. Chem. Phys., 18, 1217–1239, https://doi.org/10.5194/acp-18-1217-2018, https://doi.org/10.5194/acp-18-1217-2018, 2018
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Satellite-borne data of sulfur dioxide and a new data set of sulfate aerosol volume densities, as retrieved from MIPAS measurements, are studied in the upper-troposphere–lower-stratosphere region. General patterns of enhanced aerosol are in agreement with SO2. Via chemical transport model simulations for two volcanic eruptions in the Northern Hemisphere midlatitudes, we show that the volcanic enhancements in MIPAS SO2 and sulfate aerosol are consistent in terms of mass and transport patterns.
Andreas Engel, Harald Bönisch, Jennifer Ostermöller, Martyn P. Chipperfield, Sandip Dhomse, and Patrick Jöckel
Atmos. Chem. Phys., 18, 601–619, https://doi.org/10.5194/acp-18-601-2018, https://doi.org/10.5194/acp-18-601-2018, 2018
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We present a new method to derive equivalent effective stratospheric chlorine (EESC), which is based on an improved formulation of the propagation of trends of species with chemical loss from the troposphere to the stratosphere. EESC calculated with the new method shows much better agreement with model-derived ESC. Based on this new formulation, we expect the halogen impact on midlatitude stratospheric ozone to return to 1980 values about 10 years later, then using the current formulation.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Gerald Wetzel, Hermann Oelhaf, Michael Höpfner, Felix Friedl-Vallon, Andreas Ebersoldt, Thomas Gulde, Sebastian Kazarski, Oliver Kirner, Anne Kleinert, Guido Maucher, Hans Nordmeyer, Johannes Orphal, Roland Ruhnke, and Björn-Martin Sinnhuber
Atmos. Chem. Phys., 17, 14631–14643, https://doi.org/10.5194/acp-17-14631-2017, https://doi.org/10.5194/acp-17-14631-2017, 2017
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We report the first stratospheric measurements of the diurnal variation in the inorganic bromine (Bry) reservoir species BrONO2 around sunrise and sunset. The main goal of these observations was to check the current understanding of stratospheric bromine chemistry and to estimate the amount of lower-stratospheric Bry. The calculated temporal variation in BrONO2 largely reproduces the balloon-borne observations. The amount of Bry was estimated to be about 21–25 pptv in the lower stratosphere.
Farahnaz Khosrawi, Oliver Kirner, Björn-Martin Sinnhuber, Sören Johansson, Michael Höpfner, Michelle L. Santee, Lucien Froidevaux, Jörn Ungermann, Roland Ruhnke, Wolfgang Woiwode, Hermann Oelhaf, and Peter Braesicke
Atmos. Chem. Phys., 17, 12893–12910, https://doi.org/10.5194/acp-17-12893-2017, https://doi.org/10.5194/acp-17-12893-2017, 2017
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The 2015/2016 Arctic winter was one of the coldest winters in recent years, allowing extensive PSC formation and chlorine activation. Model simulations of the 2015/2016 Arctic winter were performed with the atmospheric chemistry–climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC). We find that ozone loss was quite strong but not as strong as in 2010/2011; denitrification and dehydration were so far the strongest observed in the Arctic stratosphere in at least the past 10 years.
Sean M. Davis, Michaela I. Hegglin, Masatomo Fujiwara, Rossana Dragani, Yayoi Harada, Chiaki Kobayashi, Craig Long, Gloria L. Manney, Eric R. Nash, Gerald L. Potter, Susann Tegtmeier, Tao Wang, Krzysztof Wargan, and Jonathon S. Wright
Atmos. Chem. Phys., 17, 12743–12778, https://doi.org/10.5194/acp-17-12743-2017, https://doi.org/10.5194/acp-17-12743-2017, 2017
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Ozone and water vapor in the stratosphere are important gases that affect surface climate and absorb incoming solar ultraviolet radiation. These gases are represented in reanalyses, which create a complete picture of the state of Earth's atmosphere using limited observations. We evaluate reanalysis water vapor and ozone fidelity by intercomparing them, and comparing them to independent observations. Generally reanalyses do a good job at representing ozone, but have problems with water vapor.
Stefanie Falk, Björn-Martin Sinnhuber, Gisèle Krysztofiak, Patrick Jöckel, Phoebe Graf, and Sinikka T. Lennartz
Atmos. Chem. Phys., 17, 11313–11329, https://doi.org/10.5194/acp-17-11313-2017, https://doi.org/10.5194/acp-17-11313-2017, 2017
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Brominated very short-lived source gases (VSLS) contribute significantly to the tropospheric and stratospheric bromine loading. We find an increase of future ocean–atmosphere flux of brominated VSLS of 8–10 % compared to present day. A decrease in the tropospheric mixing ratios of VSLS and an increase in the lower stratosphere are attributed to changes in atmospheric chemistry and transport. Bromine impact on stratospheric ozone at the end of the 21st century is reduced compared to present day.
Cathleen Schlundt, Susann Tegtmeier, Sinikka T. Lennartz, Astrid Bracher, Wee Cheah, Kirstin Krüger, Birgit Quack, and Christa A. Marandino
Atmos. Chem. Phys., 17, 10837–10854, https://doi.org/10.5194/acp-17-10837-2017, https://doi.org/10.5194/acp-17-10837-2017, 2017
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For the first time, oxygenated volatile organic carbon (OVOC) in the ocean and overlaying atmosphere in the western Pacific Ocean has been measured. OVOCs are important for atmospheric chemistry. They are involved in ozone production in the upper troposphere (UT), and they have a climate cooling effect. We showed that phytoplankton was an important source for OVOCs in the surface ocean, and when OVOCs are emitted into the atmosphere, they could reach the UT and might influence ozone formation.
Maria A. Navarro, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Elliot Atlas, Xavier Rodriguez-Lloveras, Douglas Kinnison, Jean-Francois Lamarque, Simone Tilmes, Troy Thornberry, Andrew Rollins, James W. Elkins, Eric J. Hintsa, and Fred L. Moore
Atmos. Chem. Phys., 17, 9917–9930, https://doi.org/10.5194/acp-17-9917-2017, https://doi.org/10.5194/acp-17-9917-2017, 2017
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Inorganic bromine (Bry) plays an important role in ozone layer depletion. Based on aircraft observations of organic bromine species and chemistry simulations, we model the Bry abundances over the Pacific tropical tropopause. Our results show BrO and Br as the dominant species during daytime hours, and BrCl and BrONO2 as the nighttime dominant species over the western and eastern Pacific, respectively. The difference in the partitioning is due to changes in the abundance of O3, NO2, and Cly.
Olivier Membrive, Cyril Crevoisier, Colm Sweeney, François Danis, Albert Hertzog, Andreas Engel, Harald Bönisch, and Laurence Picon
Atmos. Meas. Tech., 10, 2163–2181, https://doi.org/10.5194/amt-10-2163-2017, https://doi.org/10.5194/amt-10-2163-2017, 2017
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A new high-resolution AirCore system is presented. This system flown with stratospheric balloons allows us to sample atmospheric air during the descent. The analysis of trace gases (CO2 and CH4 in this case) in the collected air sample provides information on the vertical distribution along the atmospheric column. The continuous vertical profiles retrieved may contribute to several research topics concerning the observation of greenhouse gases and, more generally, carbon cycle studies.
Andreas Engel, Harald Bönisch, Markus Ullrich, Robert Sitals, Olivier Membrive, Francois Danis, and Cyril Crevoisier
Atmos. Chem. Phys., 17, 6825–6838, https://doi.org/10.5194/acp-17-6825-2017, https://doi.org/10.5194/acp-17-6825-2017, 2017
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AirCore is new technique for sampling stratospheric air. We present new observations of CO2 and CH4 using AirCore and derive stratospheric transport time, called the mean age of air. The purpose of using AirCore is to provide a cost-effective tool for deriving mean age. Mean age may serve as a proxy to investigate changes in stratospheric circulation. We show that there is no statistically significant trend in our 40-year time series of mean age, which is now extended using AirCore.
Alina Fiehn, Birgit Quack, Helmke Hepach, Steffen Fuhlbrügge, Susann Tegtmeier, Matthew Toohey, Elliot Atlas, and Kirstin Krüger
Atmos. Chem. Phys., 17, 6723–6741, https://doi.org/10.5194/acp-17-6723-2017, https://doi.org/10.5194/acp-17-6723-2017, 2017
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Halogenated very short-lived substances (VSLSs) are naturally produced in the ocean and emitted to the atmosphere. In the stratosphere, these compounds can have a significant influence on the ozone layer and climate. During a research cruise in the west Indian Ocean, we found an important source region of halogenated VSLSs during the Asian summer monsoon. Modeling the transport from the ocean to the stratosphere we found two main pathways, one over the Indian Ocean and one over northern India.
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.
Jennifer Ostermöller, Harald Bönisch, Patrick Jöckel, and Andreas Engel
Atmos. Chem. Phys., 17, 3785–3797, https://doi.org/10.5194/acp-17-3785-2017, https://doi.org/10.5194/acp-17-3785-2017, 2017
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We analysed the temporal evolution of fractional release factors (FRFs) from EMAC model simulations for several halocarbons and nitrous oxide. The current formulation of FRFs yields values that depend on the tropospheric trend of the species. This is a problematic issue for the application of FRF in the calculation of steady-state quantities (e.g. ODP). Including a loss term in the calculation, we develop a new formulation of FRF and find that the time dependence can almost be compensated.
Jochen Stutz, Bodo Werner, Max Spolaor, Lisa Scalone, James Festa, Catalina Tsai, Ross Cheung, Santo F. Colosimo, Ugo Tricoli, Rasmus Raecke, Ryan Hossaini, Martyn P. Chipperfield, Wuhu Feng, Ru-Shan Gao, Eric J. Hintsa, James W. Elkins, Fred L. Moore, Bruce Daube, Jasna Pittman, Steven Wofsy, and Klaus Pfeilsticker
Atmos. Meas. Tech., 10, 1017–1042, https://doi.org/10.5194/amt-10-1017-2017, https://doi.org/10.5194/amt-10-1017-2017, 2017
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A new limb-scanning Differential Optical Absorption Spectroscopy (DOAS) instrument was developed for NASA’s Global Hawk unmanned aerial system during the Airborne Tropical TRopopause EXperiment to study trace gases in the tropical tropopause layer. A new technique that uses in situ and DOAS O3 observations together with radiative transfer calculations allows the retrieval of mixing ratios from the slant column densities of BrO and NO2 at high accuracies of 0.5 ppt and 15 ppt, respectively.
Norbert Glatthor, Michael Höpfner, Adrian Leyser, Gabriele P. Stiller, Thomas von Clarmann, Udo Grabowski, Sylvia Kellmann, Andrea Linden, Björn-Martin Sinnhuber, Gisèle Krysztofiak, and Kaley A. Walker
Atmos. Chem. Phys., 17, 2631–2652, https://doi.org/10.5194/acp-17-2631-2017, https://doi.org/10.5194/acp-17-2631-2017, 2017
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To date, information on the global distribution of atmospheric carbonyl sulfide (OCS) is still rather sparse.
However, detailed knowledge of the OCS distribution is of scientific interest, because this trace gas is on one of the major sources of atmospheric sulfur, which is a prerequisite of the stratospheric aerosol layer. Under this aspect we present a comprehensive space-borne data set of global OCS concentrations covering the period from June 2002 to April 2012.
Gwenaël Berthet, Fabrice Jégou, Valéry Catoire, Gisèle Krysztofiak, Jean-Baptiste Renard, Adam E. Bourassa, Doug A. Degenstein, Colette Brogniez, Marcel Dorf, Sebastian Kreycy, Klaus Pfeilsticker, Bodo Werner, Franck Lefèvre, Tjarda J. Roberts, Thibaut Lurton, Damien Vignelles, Nelson Bègue, Quentin Bourgeois, Daniel Daugeron, Michel Chartier, Claude Robert, Bertrand Gaubicher, and Christophe Guimbaud
Atmos. Chem. Phys., 17, 2229–2253, https://doi.org/10.5194/acp-17-2229-2017, https://doi.org/10.5194/acp-17-2229-2017, 2017
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Since the last major volcanic event, i.e. the Pinatubo eruption in 1991, only
moderateeruptions have regularly injected sulfur into the stratosphere, typically enhancing the aerosol loading for several months. We investigate here for the first time the chemical perturbation associated with the Sarychev eruption in June 2009, using balloon-borne instruments and model calculations. Some chemical compounds are significantly affected by the aerosols, but the impact on stratospheric ozone is weak.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Garlich Fischbeck, Harald Bönisch, Marco Neumaier, Carl A. M. Brenninkmeijer, Johannes Orphal, Joel Brito, Julia Becker, Detlev Sprung, Peter F. J. van Velthoven, and Andreas Zahn
Atmos. Chem. Phys., 17, 1985–2008, https://doi.org/10.5194/acp-17-1985-2017, https://doi.org/10.5194/acp-17-1985-2017, 2017
Masatomo Fujiwara, Jonathon S. Wright, Gloria L. Manney, Lesley J. Gray, James Anstey, Thomas Birner, Sean Davis, Edwin P. Gerber, V. Lynn Harvey, Michaela I. Hegglin, Cameron R. Homeyer, John A. Knox, Kirstin Krüger, Alyn Lambert, Craig S. Long, Patrick Martineau, Andrea Molod, Beatriz M. Monge-Sanz, Michelle L. Santee, Susann Tegtmeier, Simon Chabrillat, David G. H. Tan, David R. Jackson, Saroja Polavarapu, Gilbert P. Compo, Rossana Dragani, Wesley Ebisuzaki, Yayoi Harada, Chiaki Kobayashi, Will McCarty, Kazutoshi Onogi, Steven Pawson, Adrian Simmons, Krzysztof Wargan, Jeffrey S. Whitaker, and Cheng-Zhi Zou
Atmos. Chem. Phys., 17, 1417–1452, https://doi.org/10.5194/acp-17-1417-2017, https://doi.org/10.5194/acp-17-1417-2017, 2017
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We introduce the SPARC Reanalysis Intercomparison Project (S-RIP), review key concepts and elements of atmospheric reanalysis systems, and summarize the technical details of and differences among 11 of these systems. This work supports scientific studies and intercomparisons of reanalysis products by collecting these background materials and technical details into a single reference. We also address several common misunderstandings and points of confusion regarding reanalyses.
Brian M. Lerner, Jessica B. Gilman, Kenneth C. Aikin, Elliot L. Atlas, Paul D. Goldan, Martin Graus, Roger Hendershot, Gabriel A. Isaacman-VanWertz, Abigail Koss, William C. Kuster, Richard A. Lueb, Richard J. McLaughlin, Jeff Peischl, Donna Sueper, Thomas B. Ryerson, Travis W. Tokarek, Carsten Warneke, Bin Yuan, and Joost A. de Gouw
Atmos. Meas. Tech., 10, 291–313, https://doi.org/10.5194/amt-10-291-2017, https://doi.org/10.5194/amt-10-291-2017, 2017
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Whole air sampling followed by analysis by gas chromatography is a common technique for characterization of trace volatile organic compounds in the atmosphere. We describe a new automated gas chromatograph–mass spectrograph which uses a Stirling cooler for sample preconcentration at −165 °C without the need for a cryogen such as liquid nitrogen. We also discuss potential sources of artifacts from our electropolished stainless steel sampling system and present results from two field campaigns.
Bodo Werner, Jochen Stutz, Max Spolaor, Lisa Scalone, Rasmus Raecke, James Festa, Santo Fedele Colosimo, Ross Cheung, Catalina Tsai, Ryan Hossaini, Martyn P. Chipperfield, Giorgio S. Taverna, Wuhu Feng, James W. Elkins, David W. Fahey, Ru-Shan Gao, Erik J. Hintsa, Troy D. Thornberry, Free Lee Moore, Maria A. Navarro, Elliot Atlas, Bruce C. Daube, Jasna Pittman, Steve Wofsy, and Klaus Pfeilsticker
Atmos. Chem. Phys., 17, 1161–1186, https://doi.org/10.5194/acp-17-1161-2017, https://doi.org/10.5194/acp-17-1161-2017, 2017
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The paper reports on inorganic and organic bromine measured in the tropical tropopause layer (TTL) over the eastern Pacific in early 2013. Bryinorg is found to increase from a mean of 2.63 ± 1.04 ppt for θ in the range of 350–360 K to 5.11 ± 1.57 ppt for θ=390 ± 400 K, whereas in the subtropical lower stratosphere, it reaches 7.66 ± 2.95 ppt for θ in the range of 390–400 K. Within the TTL, total bromine is found to range from 20.3 ppt to 22.3 ppt.
Sinikka T. Lennartz, Christa A. Marandino, Marc von Hobe, Pau Cortes, Birgit Quack, Rafel Simo, Dennis Booge, Andrea Pozzer, Tobias Steinhoff, Damian L. Arevalo-Martinez, Corinna Kloss, Astrid Bracher, Rüdiger Röttgers, Elliot Atlas, and Kirstin Krüger
Atmos. Chem. Phys., 17, 385–402, https://doi.org/10.5194/acp-17-385-2017, https://doi.org/10.5194/acp-17-385-2017, 2017
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We present new sea surface and marine boundary layer measurements of carbonyl sulfide, the most abundant sulfur gas in the atmosphere, and calculate an oceanic emission estimate. Our results imply that oceanic emissions are very unlikely to account for the missing source in the atmospheric budget that is currently discussed for OCS.
Martyn P. Chipperfield, Qing Liang, Matthew Rigby, Ryan Hossaini, Stephen A. Montzka, Sandip Dhomse, Wuhu Feng, Ronald G. Prinn, Ray F. Weiss, Christina M. Harth, Peter K. Salameh, Jens Mühle, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Paul B. Krummel, Paul J. Fraser, L. Paul Steele, James D. Happell, Robert C. Rhew, James Butler, Shari A. Yvon-Lewis, Bradley Hall, David Nance, Fred Moore, Ben R. Miller, James W. Elkins, Jeremy J. Harrison, Chris D. Boone, Elliot L. Atlas, and Emmanuel Mahieu
Atmos. Chem. Phys., 16, 15741–15754, https://doi.org/10.5194/acp-16-15741-2016, https://doi.org/10.5194/acp-16-15741-2016, 2016
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Carbon tetrachloride (CCl4) is a compound which, when released into the atmosphere, can cause depletion of the stratospheric ozone layer. Its emissions are controlled under the Montreal Protocol, and its atmospheric abundance is slowly decreasing. However, this decrease is not as fast as expected based on estimates of its emissions and its atmospheric lifetime. We have used an atmospheric model to look at the uncertainties in the CCl4 lifetime and to examine the impact on its atmospheric decay.
Christiane Voigt, Andreas Dörnbrack, Martin Wirth, Silke M. Groß, Robert Baumann, Benedikt Ehard, Michael C. Pitts, Lamont R. Poole, Björn-Martin Sinnhuber, and Hermann Oelhaf
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-1082, https://doi.org/10.5194/acp-2016-1082, 2016
Revised manuscript not accepted
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The letter describes unprecedented observations of widespread and persistent polar stratospheric ice clouds (ice PSCs) in the exceptionally cold Arctic stratospheric winter 2015/16. The unique observations are of global relevance because trends in Arctic ozone loss and in polar temperatures are highly uncertain. The new observations at cold conditions serve to enhance our knowledge on ice PSC formation, Arctic ozone loss and polar stratrospheric temperatures in a changing climate.
Elisa Castelli, Marco Ridolfi, Massimo Carlotti, Björn-Martin Sinnhuber, Oliver Kirner, Michael Kiefer, and Bianca Maria Dinelli
Atmos. Meas. Tech., 9, 5499–5508, https://doi.org/10.5194/amt-9-5499-2016, https://doi.org/10.5194/amt-9-5499-2016, 2016
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MIPAS is a satellite-borne limb emission sounder. The algorithm used to infer atmospheric composition from its measurements exploits the assumption that the atmosphere is horizontally homogeneous. This assumption can cause significant errors. We use synthetic observations to quantify these errors. Furthermore we show that the inclusion of any kind of horizontal variability model improves all the retrieval targets and that the two-dimensional approach implies the smallest errors.
Linda M. J. Kooijmans, Nelly A. M. Uitslag, Mark S. Zahniser, David D. Nelson, Stephen A. Montzka, and Huilin Chen
Atmos. Meas. Tech., 9, 5293–5314, https://doi.org/10.5194/amt-9-5293-2016, https://doi.org/10.5194/amt-9-5293-2016, 2016
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The accuracy of carbon models, used for the prediction of global climate change, is limited by the knowledge of the uptake of carbon by plants through photosynthesis. Carbonyl sulfide (COS) has been suggested as a tracer for this process. To be able to further explore and verify the application of this novel tracer we have tested a laser spectrometer for its suitability to obtain accurate and high precision measurements of COS and CO2 with both laboratory experiments and field measurements.
Florian Obersteiner, Harald Bönisch, Timo Keber, Simon O'Doherty, and Andreas Engel
Atmos. Meas. Tech., 9, 5265–5279, https://doi.org/10.5194/amt-9-5265-2016, https://doi.org/10.5194/amt-9-5265-2016, 2016
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The analysis of trace gases in ambient air requires a preconcentration technique, in many cases to make the species of interest detectable and quantifiable. In this paper, such a preconcentration set-up is presented. Target species are trapped on adsorptive material cooled by a Stirling cooler which allows for a very low adsorption temperature but only requires electrical power. A simple and lightweight mechanical design guarantees very good suitability for remote-site field operation.
Stephen J. Andrews, Lucy J. Carpenter, Eric C. Apel, Elliot Atlas, Valeria Donets, James R. Hopkins, Rebecca S. Hornbrook, Alastair C. Lewis, Richard T. Lidster, Richard Lueb, Jamie Minaeian, Maria Navarro, Shalini Punjabi, Daniel Riemer, and Sue Schauffler
Atmos. Meas. Tech., 9, 5213–5225, https://doi.org/10.5194/amt-9-5213-2016, https://doi.org/10.5194/amt-9-5213-2016, 2016
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We present a comparison of aircraft measurements of important trace gases from a co-ordinated campaign in Jan–Feb 2014 in the tropical west Pacific involving the NASA Global Hawk, NCAR GV and FAAM BAe-146 aircraft.
The paper studies the comparability of separate measurements across platforms and demonstrates that aircraft measurements are relevant for characterising the vertical uplift of important gases, such as those with ozone-depleting potential, to the upper troposphere–lower stratosphere.
Steffen Fuhlbrügge, Birgit Quack, Elliot Atlas, Alina Fiehn, Helmke Hepach, and Kirstin Krüger
Atmos. Chem. Phys., 16, 12205–12217, https://doi.org/10.5194/acp-16-12205-2016, https://doi.org/10.5194/acp-16-12205-2016, 2016
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This study presents novel observations of the very short lived substances (VSLSs) bromoform, dibromomethane and methyl iodide with high-resolution meteorological measurements and Lagrangian transport in the Peruvian upwelling. With a simple source–loss estimate we identified VSLS abundances below the trade inversion to be significantly influenced by advection of regional sources, underscoring the importance of oceanic upwelling and trade winds on the atmospheric distribution of VSLS emission.
Helmke Hepach, Birgit Quack, Susann Tegtmeier, Anja Engel, Astrid Bracher, Steffen Fuhlbrügge, Luisa Galgani, Elliot L. Atlas, Johannes Lampel, Udo Frieß, and Kirstin Krüger
Atmos. Chem. Phys., 16, 12219–12237, https://doi.org/10.5194/acp-16-12219-2016, https://doi.org/10.5194/acp-16-12219-2016, 2016
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We present surface seawater measurements of bromo- and iodocarbons, which are involved in numerous atmospheric processes such as tropospheric and stratospheric ozone chemistry, from the highly productive Peruvian upwelling. By combining trace gas measurements, characterization of organic matter and phytoplankton species, and tropospheric modelling, we show that large amounts of iodocarbons produced from the pool of organic matter may contribute strongly to local tropospheric iodine loading.
Dennis Booge, Christa A. Marandino, Cathleen Schlundt, Paul I. Palmer, Michael Schlundt, Elliot L. Atlas, Astrid Bracher, Eric S. Saltzman, and Douglas W. R. Wallace
Atmos. Chem. Phys., 16, 11807–11821, https://doi.org/10.5194/acp-16-11807-2016, https://doi.org/10.5194/acp-16-11807-2016, 2016
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Isoprene, a biogenic trace gas, is an important precursor of secondary organic aerosol/cloud condensation nuclei. Here, we use isoprene and related field measurements from three different ocean data sets together with remotely sensed satellite data to model global marine isoprene emissions. Our findings suggest that there is at least one missing oceanic source of isoprene and possibly other unknown factors in the ocean or atmosphere influencing the atmospheric values.
James H. Butler, Shari A. Yvon-Lewis, Jurgen M. Lobert, Daniel B. King, Stephen A. Montzka, John L. Bullister, Valentin Koropalov, James W. Elkins, Bradley D. Hall, Lei Hu, and Yina Liu
Atmos. Chem. Phys., 16, 10899–10910, https://doi.org/10.5194/acp-16-10899-2016, https://doi.org/10.5194/acp-16-10899-2016, 2016
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This study was conducted to understand the influence of the ocean on the lifetime of atmospheric carbon tetrachloride, a strong, ozone-depleting gas. Data from 16 research cruises conducted between 1987 and 2010 show that, unlike the unreactive chlorofluorocarbons, carbon tetrachloride is undersaturated in surface waters regardless of temperature, wind, or biological regime, but with larger undersaturations with upwelling. Results suggest that the ocean consumes about 18 % of atmospheric CCl4.
Stefan Müller, Peter Hoor, Heiko Bozem, Ellen Gute, Bärbel Vogel, Andreas Zahn, Harald Bönisch, Timo Keber, Martina Krämer, Christian Rolf, Martin Riese, Hans Schlager, and Andreas Engel
Atmos. Chem. Phys., 16, 10573–10589, https://doi.org/10.5194/acp-16-10573-2016, https://doi.org/10.5194/acp-16-10573-2016, 2016
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In situ airborne measurements performed during TACTS/ESMVal 2012 were analysed to investigate the chemical compostion of the upper troposphere and lower stratosphere. N2O, CO and O3 data show an increase in tropospherically affected air masses within the extratropical stratosphere from August to September 2012, which originate from the Asian monsoon region. Thus, the Asian monsoon anticyclone significantly affected the chemical composition of the extratropical stratosphere during summer 2012.
Amanda C. Maycock, Katja Matthes, Susann Tegtmeier, Rémi Thiéblemont, and Lon Hood
Atmos. Chem. Phys., 16, 10021–10043, https://doi.org/10.5194/acp-16-10021-2016, https://doi.org/10.5194/acp-16-10021-2016, 2016
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The impact of changes in incoming solar radiation on stratospheric ozone has important impacts on the atmosphere. Understanding this ozone response is crucial for constraining how solar activity affects climate. This study analyses the solar ozone response (SOR) in satellite datasets and shows that there are substantial differences in the magnitude and spatial structure across different records. In particular, the SOR in the new SAGE v7.0 mixing ratio data is smaller than in the previous v6.2.
R. Hossaini, P. K. Patra, A. A. Leeson, G. Krysztofiak, N. L. Abraham, S. J. Andrews, A. T. Archibald, J. Aschmann, E. L. Atlas, D. A. Belikov, H. Bönisch, L. J. Carpenter, S. Dhomse, M. Dorf, A. Engel, W. Feng, S. Fuhlbrügge, P. T. Griffiths, N. R. P. Harris, R. Hommel, T. Keber, K. Krüger, S. T. Lennartz, S. Maksyutov, H. Mantle, G. P. Mills, B. Miller, S. A. Montzka, F. Moore, M. A. Navarro, D. E. Oram, K. Pfeilsticker, J. A. Pyle, B. Quack, A. D. Robinson, E. Saikawa, A. Saiz-Lopez, S. Sala, B.-M. Sinnhuber, S. Taguchi, S. Tegtmeier, R. T. Lidster, C. Wilson, and F. Ziska
Atmos. Chem. Phys., 16, 9163–9187, https://doi.org/10.5194/acp-16-9163-2016, https://doi.org/10.5194/acp-16-9163-2016, 2016
Lothar Stramma, Tim Fischer, Damian S. Grundle, Gerd Krahmann, Hermann W. Bange, and Christa A. Marandino
Ocean Sci., 12, 861–873, https://doi.org/10.5194/os-12-861-2016, https://doi.org/10.5194/os-12-861-2016, 2016
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Results from a research cruise on R/V Sonne to the eastern tropical Pacific in October 2015 during the 2015–2016 El Niño show the transition of current, hydrographic, and nutrient conditions to El Niño conditions in the eastern tropical Pacific in October 2015. Although in early 2015 the El Niño was strong and in October 2015 showed a clear El Niño influence on the EUC, in the eastern tropical Pacific the measurements only showed developing El Niño water mass distributions.
Joe McNorton, Martyn P. Chipperfield, Manuel Gloor, Chris Wilson, Wuhu Feng, Garry D. Hayman, Matt Rigby, Paul B. Krummel, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, Ed Dlugokencky, and Steve A. Montzka
Atmos. Chem. Phys., 16, 7943–7956, https://doi.org/10.5194/acp-16-7943-2016, https://doi.org/10.5194/acp-16-7943-2016, 2016
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Methane (CH4) is an important greenhouse gas. The growth of atmospheric CH4 stalled from 1999 to 2006, with current explanations focussed mainly on changing surface fluxes. We combine models with observations and meteorological data to assess the atmospheric contribution to CH4 changes. We find that variations in mean atmospheric hydroxyl concentration can explain part of the stall in growth. Our study highlights the role of multi-annual variability in atmospheric chemistry in global CH4 trends.
Steffen Fuhlbrügge, Birgit Quack, Susann Tegtmeier, Elliot Atlas, Helmke Hepach, Qiang Shi, Stefan Raimund, and Kirstin Krüger
Atmos. Chem. Phys., 16, 7569–7585, https://doi.org/10.5194/acp-16-7569-2016, https://doi.org/10.5194/acp-16-7569-2016, 2016
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This study presents a novel estimate for the contribution of oceanic VSLS emissions to the atmospheric boundary layer and free troposphere during the SHIVA-Sonne cruise in the South China and Sulu seas in 2011. While oceanic emissions of CHBr3 and CH3I showed a significant contribution to their atmospheric abundances, atmospheric CH2Br2 appeared to be largely advected. Convective activity in the region can furthermore lead to low VSLS boundary layer mixing ratios despite high oceanic emissions.
M. Chirkov, G. P. Stiller, A. Laeng, S. Kellmann, T. von Clarmann, C. D. Boone, J. W. Elkins, A. Engel, N. Glatthor, U. Grabowski, C. M. Harth, M. Kiefer, F. Kolonjari, P. B. Krummel, A. Linden, C. R. Lunder, B. R. Miller, S. A. Montzka, J. Mühle, S. O'Doherty, J. Orphal, R. G. Prinn, G. Toon, M. K. Vollmer, K. A. Walker, R. F. Weiss, A. Wiegele, and D. Young
Atmos. Chem. Phys., 16, 3345–3368, https://doi.org/10.5194/acp-16-3345-2016, https://doi.org/10.5194/acp-16-3345-2016, 2016
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HCFC-22 global distributions from MIPAS measurements for 2005 to 2012 are presented. Tropospheric trends are in good agreement with ground-based observations. A layer of enhanced HCFC-22 in the upper tropospheric tropics and northern subtropics is identified to come from Asian sources uplifted in the Asian monsoon. Stratospheric distributions provide show seasonal, semi-annual, and QBO-related variations. Hemispheric asymmetries of trends hint towards a change in the stratospheric circulation.
Andreas Engel, Harald Bönisch, Tim Schwarzenberger, Hans-Peter Haase, Katja Grunow, Jana Abalichin, and Stephan Sala
Atmos. Meas. Tech., 9, 1051–1062, https://doi.org/10.5194/amt-9-1051-2016, https://doi.org/10.5194/amt-9-1051-2016, 2016
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We present a validation of MIPAS-ENVISAT vertical profiles (ESA operational retrieval version 6.0) of N2O, CH4, CFC-12, and CFC-11. The geophysical validation is performed using data from a balloon-borne cryogenic whole air sampler and trajectory matching. We show that the validation results are different for the period prior to 2005 compared to the post 2005 period. N2O, CH4, and CFC-12 show partly good agreement while CFC-11 data from this retrieval cannot be used for scientific studies.
S. Tegtmeier, M. I. Hegglin, J. Anderson, B. Funke, J. Gille, A. Jones, L. Smith, T. von Clarmann, and K. A. Walker
Earth Syst. Sci. Data, 8, 61–78, https://doi.org/10.5194/essd-8-61-2016, https://doi.org/10.5194/essd-8-61-2016, 2016
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The first comprehensive intercomparison of CFC-11, CFC-12, HF, and SF6 satellite data was performed as part of the SPARC Data Initiative following a new "top-down" concept of satellite measurement validation and thus providing a global picture of the data characteristics. The comparisons will provide basic information on quality and consistency of the various data sets and will serve as a guide for their use in empirical studies of climate and variability, and in model-measurement comparisons.
F. Obersteiner, H. Bönisch, and A. Engel
Atmos. Meas. Tech., 9, 179–194, https://doi.org/10.5194/amt-9-179-2016, https://doi.org/10.5194/amt-9-179-2016, 2016
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We present the characterization and application of a new gas chromatography time-of-flight mass spectrometry instrument, with focus on quantitative analysis of halocarbons in air samples. The applicability of the TOFMS technique, e.g. to form the basis of a "digital air archieve", is supported by the findings of this work: very high sensitivity, high measurement precision, a large dynamical range and an open data format which allows in-depth analysis of the data.
S. Tegtmeier, F. Ziska, I. Pisso, B. Quack, G. J. M. Velders, X. Yang, and K. Krüger
Atmos. Chem. Phys., 15, 13647–13663, https://doi.org/10.5194/acp-15-13647-2015, https://doi.org/10.5194/acp-15-13647-2015, 2015
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At present, man-made halogens and natural oceanic substances both contribute to the observed ozone depletion. Emissions of the anthropogenic halogens have been reduced, whereas emissions of the natural substances are expected to increase in future climate due to anthropogenic activities affecting oceanic processes. We assess the impact of these oceanic substances on ozone by weighting their emissions with their potential to destroy ozone for current conditions and future projections.
H. Hepach, B. Quack, S. Raimund, T. Fischer, E. L. Atlas, and A. Bracher
Biogeosciences, 12, 6369–6387, https://doi.org/10.5194/bg-12-6369-2015, https://doi.org/10.5194/bg-12-6369-2015, 2015
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This manuscript covers the first measurements of CHBr3, CH2Br2 and CH3I from the equatorial Atlantic during the Cold Tongue season, identifying this region and season as a source for these compounds. For the first time, we calculated diapycnal fluxes, and showed that the fluxes from below the mixed layer to the surface are not sufficient to balance the mixed layer budget. Hence, we conclude that mixed layer production has to take place despite a pronounced sub-mixed-layer-maximum.
J. G. Levine, A. R. MacKenzie, O. J. Squire, A. T. Archibald, P. T. Griffiths, N. L. Abraham, J. A. Pyle, D. E. Oram, G. Forster, J. F. Brito, J. D. Lee, J. R. Hopkins, A. C. Lewis, S. J. B. Bauguitte, C. F. Demarco, P. Artaxo, P. Messina, J. Lathière, D. A. Hauglustaine, E. House, C. N. Hewitt, and E. Nemitz
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-24251-2015, https://doi.org/10.5194/acpd-15-24251-2015, 2015
Revised manuscript has not been submitted
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This study explores our ability to simulate atmospheric chemistry stemming from isoprene emissions—a reactive gas emitted from vegetation—in pristine and polluted regions of the Amazon basin. We explore how two contrasting models fare in reproducing recent airborne measurements in the region. Their differing treatments of transport and mixing are found to: profoundly affect their performance; and yield very different pictures of the exposure of the rainforest to harmful ozone concentrations.
V. Catoire, G. Krysztofiak, C. Robert, M. Chartier, P. Jacquet, C. Guimbaud, P. D. Hamer, and V. Marécal
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amtd-8-9165-2015, https://doi.org/10.5194/amtd-8-9165-2015, 2015
Preprint withdrawn
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A three-channel infrared laser absorption spectrometer has been developed for airborne measurements of trace gases up to the upper troposphere. More than three different species can be measured simultaneously with high time resolution using three individual Continuous Wave Quantum Cascade Lasers coupled to a single Robert multipass optical cell. The first deployment of this spectrometer was realized in convective outflows over South China Sea where enhancements of CO were detected.
G. Wetzel, H. Oelhaf, M. Birk, A. de Lange, A. Engel, F. Friedl-Vallon, O. Kirner, A. Kleinert, G. Maucher, H. Nordmeyer, J. Orphal, R. Ruhnke, B.-M. Sinnhuber, and P. Vogt
Atmos. Chem. Phys., 15, 8065–8076, https://doi.org/10.5194/acp-15-8065-2015, https://doi.org/10.5194/acp-15-8065-2015, 2015
Fuqing Zhang, Junhong Wei, Meng Zhang, K. P. Bowman, L. L. Pan, E. Atlas, and S. C. Wofsy
Atmos. Chem. Phys., 15, 7667–7684, https://doi.org/10.5194/acp-15-7667-2015, https://doi.org/10.5194/acp-15-7667-2015, 2015
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Based on spectral and wavelet analyses, along with a diagnosis of the polarization relations, this study analyzes in situ airborne measurements from the 2008 Stratosphere-Troposphere Analyses of Regional Transport (START08) experiment to characterize gravity waves in the extratropical upper troposphere and lower stratosphere (ExUTLS) region. The focus is on the second research flight (RF02), which was dedicated to probing gravity waves associated with strong upper-tropospheric jet-front systems.
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.
J. Hoker, F. Obersteiner, H. Bönisch, and A. Engel
Atmos. Meas. Tech., 8, 2195–2206, https://doi.org/10.5194/amt-8-2195-2015, https://doi.org/10.5194/amt-8-2195-2015, 2015
I. Stemmler, I. Hense, and B. Quack
Biogeosciences, 12, 1967–1981, https://doi.org/10.5194/bg-12-1967-2015, https://doi.org/10.5194/bg-12-1967-2015, 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
T. G. Bell, W. De Bruyn, C. A. Marandino, S. D. Miller, C. S. Law, M. J. Smith, and E. S. Saltzman
Atmos. Chem. Phys., 15, 1783–1794, https://doi.org/10.5194/acp-15-1783-2015, https://doi.org/10.5194/acp-15-1783-2015, 2015
M. Toohey, K. Krüger, M. Bittner, C. Timmreck, and H. Schmidt
Atmos. Chem. Phys., 14, 13063–13079, https://doi.org/10.5194/acp-14-13063-2014, https://doi.org/10.5194/acp-14-13063-2014, 2014
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Earth system model simulations are used to investigate the impact of volcanic aerosol forcing on stratospheric dynamics, e.g. the Northern Hemisphere (NH) polar vortex. We find that mechanisms linking aerosol heating and high-latitude dynamics are not as direct as often assumed; high-latitude effects result from changes in stratospheric circulation and related vertical motions. The simulated responses also show evidence of being sensitive to the structure of the volcanic forcing used.
A. Ostler, R. Sussmann, M. Rettinger, N. M. Deutscher, S. Dohe, F. Hase, N. Jones, M. Palm, and B.-M. Sinnhuber
Atmos. Meas. Tech., 7, 4081–4101, https://doi.org/10.5194/amt-7-4081-2014, https://doi.org/10.5194/amt-7-4081-2014, 2014
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Ground-based FTIR soundings of column-average methane from NDACC and TCCON can be combined without the need to apply an overall calibration factor. NDACC and TCCON measurements complement one another and provide valuable information for satellite validation, evaluation of chemical-transport models, and source-sink inversions. The impact of dynamical variability on NDACC and TCCON retrievals of column-average methane is reflected in different smoothing effects.
S. T. Lennartz, A. Lehmann, J. Herrford, F. Malien, H.-P. Hansen, H. Biester, and H. W. Bange
Biogeosciences, 11, 6323–6339, https://doi.org/10.5194/bg-11-6323-2014, https://doi.org/10.5194/bg-11-6323-2014, 2014
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A time series of nine oceanic parameters from the coastal time series station Boknis Eck (BE, southwestern Baltic Sea) in the period of 1957-2013 is analysed with respect to seasonal cycles and long-term trends. Most striking was a paradoxical decreasing trend in oxygen with a simultaneous decline in eutrophication. Possible reasons for this paradox, e.g. processes related to warming temperatures such as increased decomposition of organic matter or altered ventilation, are discussed.
L. Kritten, A. Butz, M. P. Chipperfield, M. Dorf, S. Dhomse, R. Hossaini, H. Oelhaf, C. Prados-Roman, G. Wetzel, and K. Pfeilsticker
Atmos. Chem. Phys., 14, 9555–9566, https://doi.org/10.5194/acp-14-9555-2014, https://doi.org/10.5194/acp-14-9555-2014, 2014
M. Maione, F. Graziosi, J. Arduini, F. Furlani, U. Giostra, D. R. Blake, P. Bonasoni, X. Fang, S. A. Montzka, S. J. O'Doherty, S. Reimann, A. Stohl, and M. K. Vollmer
Atmos. Chem. Phys., 14, 9755–9770, https://doi.org/10.5194/acp-14-9755-2014, https://doi.org/10.5194/acp-14-9755-2014, 2014
I. Stemmler, I. Hense, B. Quack, and E. Maier-Reimer
Biogeosciences, 11, 4459–4476, https://doi.org/10.5194/bg-11-4459-2014, https://doi.org/10.5194/bg-11-4459-2014, 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
S. Sala, H. Bönisch, T. Keber, D. E. Oram, G. Mills, and A. Engel
Atmos. Chem. Phys., 14, 6903–6923, https://doi.org/10.5194/acp-14-6903-2014, https://doi.org/10.5194/acp-14-6903-2014, 2014
Q. Liang, E. Atlas, D. Blake, M. Dorf, K. Pfeilsticker, and S. Schauffler
Atmos. Chem. Phys., 14, 5781–5792, https://doi.org/10.5194/acp-14-5781-2014, https://doi.org/10.5194/acp-14-5781-2014, 2014
D. R. Gentner, T. B. Ford, A. Guha, K. Boulanger, J. Brioude, W. M. Angevine, J. A. de Gouw, C. Warneke, J. B. Gilman, T. B. Ryerson, J. Peischl, S. Meinardi, D. R. Blake, E. Atlas, W. A. Lonneman, T. E. Kleindienst, M. R. Beaver, J. M. St. Clair, P. O. Wennberg, T. C. VandenBoer, M. Z. Markovic, J. G. Murphy, R. A. Harley, and A. H. Goldstein
Atmos. Chem. Phys., 14, 4955–4978, https://doi.org/10.5194/acp-14-4955-2014, https://doi.org/10.5194/acp-14-4955-2014, 2014
M. Rex, I. Wohltmann, T. Ridder, R. Lehmann, K. Rosenlof, P. Wennberg, D. Weisenstein, J. Notholt, K. Krüger, V. Mohr, and S. Tegtmeier
Atmos. Chem. Phys., 14, 4827–4841, https://doi.org/10.5194/acp-14-4827-2014, https://doi.org/10.5194/acp-14-4827-2014, 2014
C. J. Young, R. A. Washenfelder, P. M. Edwards, D. D. Parrish, J. B. Gilman, W. C. Kuster, L. H. Mielke, H. D. Osthoff, C. Tsai, O. Pikelnaya, J. Stutz, P. R. Veres, J. M. Roberts, S. Griffith, S. Dusanter, P. S. Stevens, J. Flynn, N. Grossberg, B. Lefer, J. S. Holloway, J. Peischl, T. B. Ryerson, E. L. Atlas, D. R. Blake, and S. S. Brown
Atmos. Chem. Phys., 14, 3427–3440, https://doi.org/10.5194/acp-14-3427-2014, https://doi.org/10.5194/acp-14-3427-2014, 2014
P. Bohlinger, B.-M. Sinnhuber, R. Ruhnke, and O. Kirner
Atmos. Chem. Phys., 14, 1679–1688, https://doi.org/10.5194/acp-14-1679-2014, https://doi.org/10.5194/acp-14-1679-2014, 2014
B. D. Hall, A. Engel, J. Mühle, J. W. Elkins, F. Artuso, E. Atlas, M. Aydin, D. Blake, E.-G. Brunke, S. Chiavarini, P. J. Fraser, J. Happell, P. B. Krummel, I. Levin, M. Loewenstein, M. Maione, S. A. Montzka, S. O'Doherty, S. Reimann, G. Rhoderick, E. S. Saltzman, H. E. Scheel, L. P. Steele, M. K. Vollmer, R. F. Weiss, D. Worthy, and Y. Yokouchi
Atmos. Meas. Tech., 7, 469–490, https://doi.org/10.5194/amt-7-469-2014, https://doi.org/10.5194/amt-7-469-2014, 2014
H. Hepach, B. Quack, F. Ziska, S. Fuhlbrügge, E. L. Atlas, K. Krüger, I. Peeken, and D. W. R. Wallace
Atmos. Chem. Phys., 14, 1255–1275, https://doi.org/10.5194/acp-14-1255-2014, https://doi.org/10.5194/acp-14-1255-2014, 2014
L. Kuai, J. Worden, S. S. Kulawik, S. A. Montzka, and J. Liu
Atmos. Meas. Tech., 7, 163–172, https://doi.org/10.5194/amt-7-163-2014, https://doi.org/10.5194/amt-7-163-2014, 2014
C. Cressot, F. Chevallier, P. Bousquet, C. Crevoisier, E. J. Dlugokencky, A. Fortems-Cheiney, C. Frankenberg, R. Parker, I. Pison, R. A. Scheepmaker, S. A. Montzka, P. B. Krummel, L. P. Steele, and R. L. Langenfelds
Atmos. Chem. Phys., 14, 577–592, https://doi.org/10.5194/acp-14-577-2014, https://doi.org/10.5194/acp-14-577-2014, 2014
S. J. O'Shea, G. Allen, M. W. Gallagher, S. J.-B. Bauguitte, S. M. Illingworth, M. Le Breton, J. B. A. Muller, C. J. Percival, A. T. Archibald, D. E. Oram, M. Parrington, P. I. Palmer, and A. C. Lewis
Atmos. Chem. Phys., 13, 12451–12467, https://doi.org/10.5194/acp-13-12451-2013, https://doi.org/10.5194/acp-13-12451-2013, 2013
S. Tegtmeier, K. Krüger, B. Quack, E. Atlas, D. R. Blake, H. Boenisch, A. Engel, H. Hepach, R. Hossaini, M. A. Navarro, S. Raimund, S. Sala, Q. Shi, and F. Ziska
Atmos. Chem. Phys., 13, 11869–11886, https://doi.org/10.5194/acp-13-11869-2013, https://doi.org/10.5194/acp-13-11869-2013, 2013
R. Hossaini, H. Mantle, M. P. Chipperfield, S. A. Montzka, P. Hamer, F. Ziska, B. Quack, K. Krüger, S. Tegtmeier, E. Atlas, S. Sala, A. Engel, H. Bönisch, T. Keber, D. Oram, G. Mills, C. Ordóñez, A. Saiz-Lopez, N. Warwick, Q. Liang, W. Feng, F. Moore, B. R. Miller, V. Marécal, N. A. D. Richards, M. Dorf, and K. Pfeilsticker
Atmos. Chem. Phys., 13, 11819–11838, https://doi.org/10.5194/acp-13-11819-2013, https://doi.org/10.5194/acp-13-11819-2013, 2013
S. S. Brown, W. P. Dubé, R. Bahreini, A. M. Middlebrook, C. A. Brock, C. Warneke, J. A. de Gouw, R. A. Washenfelder, E. Atlas, J. Peischl, T. B. Ryerson, J. S. Holloway, J. P. Schwarz, R. Spackman, M. Trainer, D. D. Parrish, F. C. Fehshenfeld, and A. R. Ravishankara
Atmos. Chem. Phys., 13, 11317–11337, https://doi.org/10.5194/acp-13-11317-2013, https://doi.org/10.5194/acp-13-11317-2013, 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
M. Le Breton, A. Bacak, J. B. A. Muller, S. J. O'Shea, P. Xiao, M. N. R. Ashfold, M. C. Cooke, R. Batt, D. E. Shallcross, D. E. Oram, G. Forster, S. J.-B. Bauguitte, P. I. Palmer, M. Parrington, A. C. Lewis, J. D. Lee, and C. J. Percival
Atmos. Chem. Phys., 13, 9217–9232, https://doi.org/10.5194/acp-13-9217-2013, https://doi.org/10.5194/acp-13-9217-2013, 2013
F. Ziska, B. Quack, K. Abrahamsson, S. D. Archer, E. Atlas, T. Bell, J. H. Butler, L. J. Carpenter, C. E. Jones, N. R. P. Harris, H. Hepach, K. G. Heumann, C. Hughes, J. Kuss, K. Krüger, P. Liss, R. M. Moore, A. Orlikowska, S. Raimund, C. E. Reeves, W. Reifenhäuser, A. D. Robinson, C. Schall, T. Tanhua, S. Tegtmeier, S. Turner, L. Wang, D. Wallace, J. Williams, H. Yamamoto, S. Yvon-Lewis, and Y. Yokouchi
Atmos. Chem. Phys., 13, 8915–8934, https://doi.org/10.5194/acp-13-8915-2013, https://doi.org/10.5194/acp-13-8915-2013, 2013
C. A. Marandino, S. Tegtmeier, K. Krüger, C. Zindler, E. L. Atlas, F. Moore, and H. W. Bange
Atmos. Chem. Phys., 13, 8427–8437, https://doi.org/10.5194/acp-13-8427-2013, https://doi.org/10.5194/acp-13-8427-2013, 2013
P. D. Hamer, V. Marécal, R. Hossaini, M. Pirre, N. Warwick, M. Chipperfield, A. A. Samah, N. Harris, A. Robinson, B. Quack, A. Engel, K. Krüger, E. Atlas, K. Subramaniam, D. Oram, Emma C. Leedham Elvidge, G. Mills, K. Pfeilsticker, S. Sala, T. Keber, H. Bönisch, L. K. Peng, M. S. M. Nadzir, P. T. Lim, A. Mujahid, A. Anton, H. Schlager, V. Catoire, G. Krysztofiak, S. Fühlbrügge, M. Dorf, and W. T. Sturges
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-20611-2013, https://doi.org/10.5194/acpd-13-20611-2013, 2013
Revised manuscript not accepted
W. Cheah, B. B. Taylor, S. Wiegmann, S. Raimund, G. Krahmann, B. Quack, and A. Bracher
Biogeosciences Discuss., https://doi.org/10.5194/bgd-10-12115-2013, https://doi.org/10.5194/bgd-10-12115-2013, 2013
Revised manuscript not accepted
S. Fuhlbrügge, K. Krüger, B. Quack, E. Atlas, H. Hepach, and F. Ziska
Atmos. Chem. Phys., 13, 6345–6357, https://doi.org/10.5194/acp-13-6345-2013, https://doi.org/10.5194/acp-13-6345-2013, 2013
C. Zindler, A. Bracher, C. A. Marandino, B. Taylor, E. Torrecilla, A. Kock, and H. W. Bange
Biogeosciences, 10, 3297–3311, https://doi.org/10.5194/bg-10-3297-2013, https://doi.org/10.5194/bg-10-3297-2013, 2013
K. Großmann, U. Frieß, E. Peters, F. Wittrock, J. Lampel, S. Yilmaz, J. Tschritter, R. Sommariva, R. von Glasow, B. Quack, K. Krüger, K. Pfeilsticker, and U. Platt
Atmos. Chem. Phys., 13, 3363–3378, https://doi.org/10.5194/acp-13-3363-2013, https://doi.org/10.5194/acp-13-3363-2013, 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
J. Aschmann and B.-M. Sinnhuber
Atmos. Chem. Phys., 13, 1203–1219, https://doi.org/10.5194/acp-13-1203-2013, https://doi.org/10.5194/acp-13-1203-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Aggravated surface O3 pollution primarily driven by meteorological variations in China during the 2020 COVID-19 pandemic lockdown period
Identifying decadal trends in deweathered concentrations of criteria air pollutants in Canadian urban atmospheres with machine learning approaches
Evaluation of modelled versus observed non-methane volatile organic compounds at European Monitoring and Evaluation Programme sites in Europe
Constraining non-methane VOC emissions with TROPOMI HCHO observations: impact on summertime ozone simulation in August 2022 in China
Revealing the significant acceleration of hydrofluorocarbon (HFC) emissions in eastern Asia through long-term atmospheric observations
Interpreting Geostationary Environment Monitoring Spectrometer (GEMS) geostationary satellite observations of the diurnal variation in nitrogen dioxide (NO2) over East Asia
An intercomparison of satellite, airborne, and ground-level observations with WRF–CAMx simulations of NO2 columns over Houston, Texas, during the September 2021 TRACER-AQ campaign
Interannual variability of summertime formaldehyde (HCHO) vertical column density and its main drivers at northern high latitudes
The impact of multi-decadal changes in VOC speciation on urban ozone chemistry: a case study in Birmingham, United Kingdom
Technical note: Challenges in detecting free tropospheric ozone trends in a sparsely sampled environment
Combined assimilation of NOAA surface and MIPAS satellite observations to constrain the global budget of carbonyl sulfide
The impact of gaseous degradation on the gas–particle partitioning of methylated polycyclic aromatic hydrocarbons
Technical note: An assessment of the performance of statistical bias correction techniques for global chemistry–climate model surface ozone fields
A better representation of volatile organic compound chemistry in WRF-Chem and its impact on ozone over Los Angeles
High-resolution US methane emissions inferred from an inversion of 2019 TROPOMI satellite data: contributions from individual states, urban areas, and landfills
Summertime tropospheric ozone source apportionment study in the Madrid region (Spain)
CO anthropogenic emissions in Europe from 2011 to 2021: insights from Measurement of Pollution in the Troposphere (MOPITT) satellite data
Constraining long-term NOx emissions over the United States and Europe using nitrate wet deposition monitoring networks
Analysis of an intense O3 pollution episode on the Atlantic coast of the Iberian Peninsula using photochemical modeling: characterization of transport pathways and accumulation processes
Atmospheric oxygen as a tracer for fossil fuel carbon dioxide: a sensitivity study in the UK
Impact of improved representation of VOC emissions and production of NOx reservoirs on modeled urban ozone production
MIXv2: a long-term mosaic emission inventory for Asia (2010–2017)
Organosulfate produced from consumption of SO3 speeds up sulfuric acid–dimethylamine atmospheric nucleation
Contribution of expanded marine sulfur chemistry to the seasonal variability of dimethyl sulfide oxidation products and size-resolved sulfate aerosol
Development of a detailed gaseous oxidation scheme of naphthalene for SOA formation and speciation
Spatial disparities of ozone pollution in the Sichuan Basin spurred by extreme, hot weather
Global impacts of aviation on air quality evaluated at high resolution
Enhancing Long-Term Trend Simulation of Global Tropospheric OH and Its Drivers from 2005–2019: A Synergistic Integration of Model Simulations and Satellite Observations
Large contribution of soil emissions to the atmospheric nitrogen budget and their impacts on air quality and temperature rise in North China
Bias correction of OMI HCHO columns based on FTIR and aircraft measurements and impact on top-down emission estimates
Intercomparison of GEOS-Chem and CAM-chem tropospheric oxidant chemistry within the Community Earth System Model version 2 (CESM2)
Investigation of the renewed methane growth post-2007 with high-resolution 3-D variational inverse modeling and isotopic constraints
NOx emissions in France in 2019–2021 as estimated by the high spatial resolution assimilation of TROPOMI NO2 observations
Estimating NOx emissions of stack plumes using a high-resolution atmospheric chemistry model and satellite-derived NO2 columns
Revisiting day-of-week ozone patterns in an era of evolving US air quality
Changes in South American Surface Ozone Trends: Exploring the Influences of Precursors and Extreme Events
Air quality and radiative impacts of downward-propagating sudden stratospheric warmings (SSWs)
Estimation of the atmospheric hydroxyl radical oxidative capacity using multiple hydrofluorocarbons (HFCs)
Investigating the differences in calculating global mean surface CO2 abundance: the impact of analysis methodologies and site selection
The effect of different Climate and Air Quality policies in China on in situ Ozone production in Beijing
Meteorological characteristics of extreme ozone pollution events in China and their future predictions
Evaluating modelled tropospheric columns of CH4, CO, and O3 in the Arctic using ground-based Fourier transform infrared (FTIR) measurements
The high-resolution Global Aviation emissions Inventory based on ADS-B (GAIA) for 2019–2021
Zonal variability of methane trends derived from satellite data
Weekly derived top-down volatile-organic-compound fluxes over Europe from TROPOMI HCHO data from 2018 to 2021
Current status of model predictions of volatile organic compounds and impacts on surface ozone predictions during summer in China
Utility of Geostationary Lightning Mapper-derived lightning NO emission estimates in air quality modeling studies
The suitability of atmospheric oxygen measurements to constrain western European fossil-fuel CO2 emissions and their trends
Future tropospheric ozone budget and distribution over east Asia under a net-zero scenario
Why Did Ozone Concentrations Increase During Shanghai’s Static Management? A Statistical and Radical Chemistry Perspective
Zhendong Lu, Jun Wang, Yi Wang, Daven K. Henze, Xi Chen, Tong Sha, and Kang Sun
Atmos. Chem. Phys., 24, 7793–7813, https://doi.org/10.5194/acp-24-7793-2024, https://doi.org/10.5194/acp-24-7793-2024, 2024
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In contrast with past work showing that the reduction of emissions was the dominant factor for the nationwide increase of surface O3 during the lockdown in China, this study finds that the variation in meteorology (temperature and other parameters) plays a more important role. This result is obtained through sensitivity simulations using a chemical transport model constrained by satellite (TROPOMI) data and calibrated with surface observations.
Xiaohong Yao and Leiming Zhang
Atmos. Chem. Phys., 24, 7773–7791, https://doi.org/10.5194/acp-24-7773-2024, https://doi.org/10.5194/acp-24-7773-2024, 2024
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This study investigates long-term trends of criteria air pollutants, including NO2, CO, SO2, O3 and PM2.5, and NO2+O3 measured in 10 Canadian cities during the last 2 to 3 decades. We also investigate associated driving forces in terms of emission reductions, perturbations from varying weather conditions and large-scale wildfires, as well as changes in O3 sources and sinks.
Yao Ge, Sverre Solberg, Mathew R. Heal, Stefan Reimann, Willem van Caspel, Bryan Hellack, Thérèse Salameh, and David Simpson
Atmos. Chem. Phys., 24, 7699–7729, https://doi.org/10.5194/acp-24-7699-2024, https://doi.org/10.5194/acp-24-7699-2024, 2024
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Atmospheric volatile organic compounds (VOCs) constitute many species, acting as precursors to ozone and aerosol. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the EMEP MSC-W to evaluate emission inventories in Europe. We focus on the varying agreement between modelled and measured VOCs across different species and underscore potential inaccuracies in total and sector-specific emission estimates.
Shuzhuang Feng, Fei Jiang, Tianlu Qian, Nan Wang, Mengwei Jia, Songci Zheng, Jiansong Chen, Fang Ying, and Weimin Ju
Atmos. Chem. Phys., 24, 7481–7498, https://doi.org/10.5194/acp-24-7481-2024, https://doi.org/10.5194/acp-24-7481-2024, 2024
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We developed a multi-air-pollutant inversion system to estimate non-methane volatile organic compound (NMVOC) emissions using TROPOMI formaldehyde retrievals. We found that the inversion significantly improved formaldehyde simulations and reduced NMVOC emission uncertainties. The optimized NMVOC emissions effectively corrected the overestimation of O3 levels, mainly by decreasing the rate of the RO2 + NO reaction and increasing the rate of the NO2 + OH reaction.
Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, and Sunyoung Park
Atmos. Chem. Phys., 24, 7309–7330, https://doi.org/10.5194/acp-24-7309-2024, https://doi.org/10.5194/acp-24-7309-2024, 2024
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We analyzed with an inversion model the atmospheric abundance of hydrofluorocarbons (HFCs), potent greenhouse gases, from 2008 to 2020 at Gosan station in South Korea and revealed a significant increase in emissions, especially from eastern China and Japan. This increase contradicts reported data, underscoring the need for accurate monitoring and reporting. Our findings are crucial for understanding and managing global HFCs emissions, highlighting the importance of efforts to reduce HFCs.
Laura Hyesung Yang, Daniel J. Jacob, Ruijun Dang, Yujin J. Oak, Haipeng Lin, Jhoon Kim, Shixian Zhai, Nadia K. Colombi, Drew C. Pendergrass, Ellie Beaudry, Viral Shah, Xu Feng, Robert M. Yantosca, Heesung Chong, Junsung Park, Hanlim Lee, Won-Jin Lee, Soontae Kim, Eunhye Kim, Katherine R. Travis, James H. Crawford, and Hong Liao
Atmos. Chem. Phys., 24, 7027–7039, https://doi.org/10.5194/acp-24-7027-2024, https://doi.org/10.5194/acp-24-7027-2024, 2024
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The Geostationary Environment Monitoring Spectrometer (GEMS) provides hourly measurements of NO2. We use the chemical transport model to find how emissions, chemistry, and transport drive the changes in NO2 observed by GEMS at different times of the day. In winter, the chemistry plays a minor role, and high daytime emissions dominate the diurnal variation in NO2, balanced by transport. In summer, emissions, chemistry, and transport play an important role in shaping the diurnal variation in NO2.
M. Omar Nawaz, Jeremiah Johnson, Greg Yarwood, Benjamin de Foy, Laura Judd, and Daniel L. Goldberg
Atmos. Chem. Phys., 24, 6719–6741, https://doi.org/10.5194/acp-24-6719-2024, https://doi.org/10.5194/acp-24-6719-2024, 2024
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NO2 is a gas with implications for air pollution. A campaign conducted in Houston provided an opportunity to compare NO2 from different instruments and a model. Aircraft and satellite observations agreed well with measurements on the ground; however, the latter estimated lower values. We find that model-simulated NO2 was lower than observations, especially downtown, suggesting that NO2 sources associated with the urban core of Houston, such as vehicle emissions, may be underestimated.
Tianlang Zhao, Jingqiu Mao, Zolal Ayazpour, Gonzalo González Abad, Caroline R. Nowlan, and Yiqi Zheng
Atmos. Chem. Phys., 24, 6105–6121, https://doi.org/10.5194/acp-24-6105-2024, https://doi.org/10.5194/acp-24-6105-2024, 2024
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HCHO variability is a key tracer in understanding VOC emissions in response to climate change. We investigate the role of methane oxidation and biogenic and wildfire emissions in HCHO interannual variability over northern high latitudes in summer, emphasizing wildfires as a key driver of HCHO interannual variability in Alaska, Siberia and northern Canada using satellite HCHO and SIF retrievals and then GEOS-Chem model. We show SIF is a tool to understand biogenic HCHO variability in this region.
Jianghao Li, Alastair C. Lewis, Jim R. Hopkins, Stephen J. Andrews, Tim Murrells, Neil Passant, Ben Richmond, Siqi Hou, William J. Bloss, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 24, 6219–6231, https://doi.org/10.5194/acp-24-6219-2024, https://doi.org/10.5194/acp-24-6219-2024, 2024
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A summertime ozone event at an urban site in Birmingham is sensitive to volatile organic compounds (VOCs) – particularly those of oxygenated VOCs. The roles of anthropogenic VOC sources in urban ozone chemistry are examined by integrating the 1990–2019 national atmospheric emission inventory into model scenarios. Road transport remains the most powerful means of further reducing ozone in this case study, but the benefits may be offset if solvent emissions of VOCs continue to increase.
Kai-Lan Chang, Owen R. Cooper, Audrey Gaudel, Irina Petropavlovskikh, Peter Effertz, Gary Morris, and Brian C. McDonald
Atmos. Chem. Phys., 24, 6197–6218, https://doi.org/10.5194/acp-24-6197-2024, https://doi.org/10.5194/acp-24-6197-2024, 2024
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A great majority of observational trend studies of free tropospheric ozone use sparsely sampled ozonesonde and aircraft measurements as reference data sets. A ubiquitous assumption is that trends are accurate and reliable so long as long-term records are available. We show that sampling bias due to sparse samples can persistently reduce the trend accuracy, and we highlight the importance of maintaining adequate frequency and continuity of observations.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Fu-Jie Zhu, Zi-Feng Zhang, Li-Yan Liu, Pu-Fei Yang, Peng-Tuan Hu, Geng-Bo Ren, Meng Qin, and Wan-Li Ma
Atmos. Chem. Phys., 24, 6095–6103, https://doi.org/10.5194/acp-24-6095-2024, https://doi.org/10.5194/acp-24-6095-2024, 2024
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Gas–particle (G–P) partitioning is an important atmospheric behavior for semi-volatile organic compounds (SVOCs). Diurnal variation in G–P partitioning of methylated polycyclic aromatic hydrocarbons (Me-PAHs) demonstrates the possible influence of gaseous degradation; the enhancement of gaseous degradation (1.10–5.58 times) on G–P partitioning is verified by a steady-state G–P partitioning model. The effect of gaseous degradation on G–P partitioning of (especially light) SVOCs is important.
Christoph Staehle, Harald E. Rieder, Arlene M. Fiore, and Jordan L. Schnell
Atmos. Chem. Phys., 24, 5953–5969, https://doi.org/10.5194/acp-24-5953-2024, https://doi.org/10.5194/acp-24-5953-2024, 2024
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Chemistry–climate models show biases compared to surface ozone observations and thus require bias correction for impact studies and the assessment of air quality changes. We compare the performance of commonly used correction techniques for model outputs available via CMIP6. While all methods can reduce model biases, better results are obtained from more complex approaches. Thus, our study suggests broader use of these techniques in studies seeking to inform air quality management and policy.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, J. Andrew Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
Atmos. Chem. Phys., 24, 5265–5286, https://doi.org/10.5194/acp-24-5265-2024, https://doi.org/10.5194/acp-24-5265-2024, 2024
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Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represents VOC chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from volatile chemical products and other anthropogenic sources to total VOC reactivity and O3.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Alba Lorente, Zichong Chen, Xiao Lu, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Margaux Winter, Shuang Ma, A. Anthony Bloom, John R. Worden, Robert N. Stavins, and Cynthia A. Randles
Atmos. Chem. Phys., 24, 5069–5091, https://doi.org/10.5194/acp-24-5069-2024, https://doi.org/10.5194/acp-24-5069-2024, 2024
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We quantify 2019 methane emissions in the contiguous US (CONUS) at a ≈ 25 km × 25 km resolution using satellite methane observations. We find a 13 % upward correction to the 2023 US Environmental Protection Agency (EPA) Greenhouse Gas Emissions Inventory (GHGI) for 2019, with large corrections to individual states, urban areas, and landfills. This may present a challenge for US climate policies and goals, many of which target significant reductions in methane emissions.
David de la Paz, Rafael Borge, Juan Manuel de Andrés, Luis Tovar, Golam Sarwar, and Sergey L. Napelenok
Atmos. Chem. Phys., 24, 4949–4972, https://doi.org/10.5194/acp-24-4949-2024, https://doi.org/10.5194/acp-24-4949-2024, 2024
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This source apportionment modeling study shows that around 70 % of ground-level O3 in Madrid (Spain) is transported from other regions. Nonetheless, emissions from local sources, mainly road traffic, play a significant role, especially under atmospheric stagnation. Local measures during those conditions may be able to reduce O3 peaks by up to 30 % and, thus, lessen impacts from high-O3 episodes in the Madrid metropolitan area.
Audrey Fortems-Cheiney, Gregoire Broquet, Elise Potier, Robin Plauchu, Antoine Berchet, Isabelle Pison, Hugo Denier van der Gon, and Stijn Dellaert
Atmos. Chem. Phys., 24, 4635–4649, https://doi.org/10.5194/acp-24-4635-2024, https://doi.org/10.5194/acp-24-4635-2024, 2024
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We have estimated the carbon monixide (CO) European emissions from satellite observations of the MOPITT instrument at the relatively high resolution of 0.5° for a period of over 10 years from 2011 to 2021. The analysis of the inversion results reveals the challenges associated with the inversion of CO emissions at the regional scale over Europe.
Amy Christiansen, Loretta J. Mickley, and Lu Hu
Atmos. Chem. Phys., 24, 4569–4589, https://doi.org/10.5194/acp-24-4569-2024, https://doi.org/10.5194/acp-24-4569-2024, 2024
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In this work, we provide an additional constraint on emissions and trends of nitrogen oxides using nitrate wet deposition (NWD) fluxes over the United States and Europe from 1980–2020. We find that NWD measurements constrain total NOx emissions well. We also find evidence of NOx emission overestimates in both domains, but especially over Europe, where NOx emissions are overestimated by a factor of 2. Reducing NOx emissions over Europe improves model representation of ozone at the surface.
Eduardo Torre-Pascual, Gotzon Gangoiti, Ana Rodríguez-García, Estibaliz Sáez de Cámara, Joana Ferreira, Carla Gama, María Carmen Gómez, Iñaki Zuazo, Jose Antonio García, and Maite de Blas
Atmos. Chem. Phys., 24, 4305–4329, https://doi.org/10.5194/acp-24-4305-2024, https://doi.org/10.5194/acp-24-4305-2024, 2024
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We present an analysis of an intense air pollution episode of tropospheric ozone (O3) along the Atlantic coast of the Iberian Peninsula, incorporating both measured and simulated parameters. Our study extends beyond surface-level factors to include altitude-related parameters. These episodes stem from upper-atmosphere O3 accumulation in preceding days, transported to surface layers, causing rapid O3 concentration increase.
Hannah Chawner, Eric Saboya, Karina E. Adcock, Tim Arnold, Yuri Artioli, Caroline Dylag, Grant L. Forster, Anita Ganesan, Heather Graven, Gennadi Lessin, Peter Levy, Ingrid T. Luijkx, Alistair Manning, Penelope A. Pickers, Chris Rennick, Christian Rödenbeck, and Matthew Rigby
Atmos. Chem. Phys., 24, 4231–4252, https://doi.org/10.5194/acp-24-4231-2024, https://doi.org/10.5194/acp-24-4231-2024, 2024
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The quantity of atmospheric potential oxygen (APO), derived from coincident measurements of carbon dioxide (CO2) and oxygen (O2), has been proposed as a tracer for fossil fuel CO2 emissions. In this model sensitivity study, we examine the use of APO for this purpose in the UK and compare our model to observations. We find that our model simulations are most sensitive to uncertainties relating to ocean fluxes and boundary conditions.
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Greg Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
EGUsphere, https://doi.org/10.5194/egusphere-2024-951, https://doi.org/10.5194/egusphere-2024-951, 2024
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Human activities result in the emission of many volatile organic compounds (VOCs) into the atmosphere that contribute to ozone air pollution. Detailed measurements were taken of VOCs during a field study in South Korea. When compared to models using current VOC emissions, large discrepancies pointed to underestimated emissions from chemical products, liquified petroleum gas, and long-range transport. We improved emissions and chemistry of these VOCs to better describe urban ozone pollution.
Meng Li, Junichi Kurokawa, Qiang Zhang, Jung-Hun Woo, Tazuko Morikawa, Satoru Chatani, Zifeng Lu, Yu Song, Guannan Geng, Hanwen Hu, Jinseok Kim, Owen R. Cooper, and Brian C. McDonald
Atmos. Chem. Phys., 24, 3925–3952, https://doi.org/10.5194/acp-24-3925-2024, https://doi.org/10.5194/acp-24-3925-2024, 2024
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In this work, we developed MIXv2, a mosaic Asian emission inventory for 2010–2017. With high spatial (0.1°) and monthly temporal resolution, MIXv2 integrates anthropogenic and open biomass burning emissions across seven sectors following a mosaic methodology. It provides CO2 emissions data alongside nine key pollutants and three chemical mechanisms. Our publicly accessible gridded monthly emissions data can facilitate long-term atmospheric and climate model analyses.
Xiaomeng Zhang, Yongjian Lian, Shendong Tan, and Shi Yin
Atmos. Chem. Phys., 24, 3593–3612, https://doi.org/10.5194/acp-24-3593-2024, https://doi.org/10.5194/acp-24-3593-2024, 2024
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Atmospheric new particle formation (NPF) has a significant influence on the global climate, local air quality and human health. Using a combination of quantum chemical calculations and kinetics modeling, we find that thhe gas-phase organosulfate produced from consumption of SO3 can significantly enhance SA–DMA nucleation in the polluted boundary layer, resulting in non-negligible contributions to NPF. Our findings provide important insights into organic sulfur in atmospheric aerosol formation.
Linia Tashmim, William C. Porter, Qianjie Chen, Becky Alexander, Charles H. Fite, Christopher D. Holmes, Jeffrey R. Pierce, Betty Croft, and Sakiko Ishino
Atmos. Chem. Phys., 24, 3379–3403, https://doi.org/10.5194/acp-24-3379-2024, https://doi.org/10.5194/acp-24-3379-2024, 2024
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Dimethyl sulfide (DMS) is mostly emitted from ocean surfaces and represents the largest natural source of sulfur for the atmosphere. Once in the atmosphere, DMS forms stable oxidation products such as SO2 and H2SO4, which can subsequently contribute to airborne particle formation and growth. In this study, we update the DMS oxidation mechanism in the chemical transport model GEOS-Chem and describe resulting changes in particle growth as well as the overall global sulfur budget.
Victor Lannuque and Karine Sartelet
EGUsphere, https://doi.org/10.5194/egusphere-2024-711, https://doi.org/10.5194/egusphere-2024-711, 2024
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation and speciation from naphthalene oxidation. This study details the development of the first near-explicit chemical scheme for naphthalene oxidation by OH including kinetic and mechanistic data and able to reproduce most of the experimentally identified products in both gas and particle phases.
Nan Wang, Yunsong Du, Dongyang Chen, Haiyan Meng, Xi Chen, Li Zhou, Guangming Shi, Yu Zhan, Miao Feng, Wei Li, Mulan Chen, Zhenliang Li, and Fumo Yang
Atmos. Chem. Phys., 24, 3029–3042, https://doi.org/10.5194/acp-24-3029-2024, https://doi.org/10.5194/acp-24-3029-2024, 2024
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In the scorching August 2022 heatwave, China's Sichuan Basin saw a stark contrast in ozone (O3) levels between Chengdu and Chongqing. The regional disparities were studied considering meteorology, precursors, photochemistry, and transportation. The study highlighted the importance of tailored pollution control measures and underlined the necessity for region-specific strategies to combat O3 pollution on a regional scale.
Sebastian D. Eastham, Guillaume P. Chossière, Raymond L. Speth, Daniel J. Jacob, and Steven R. H. Barrett
Atmos. Chem. Phys., 24, 2687–2703, https://doi.org/10.5194/acp-24-2687-2024, https://doi.org/10.5194/acp-24-2687-2024, 2024
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Emissions from aircraft are known to cause air quality impacts worldwide, but the scale and mechanisms of this impact are not well understood. This work uses high-resolution computational modeling of the atmosphere to show that air pollution changes from aviation are mostly the result of emissions during cruise (high-altitude) operations, that these impacts are related to how much non-aviation pollution is present, and that prior regional assessments have underestimated these impacts.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
EGUsphere, https://doi.org/10.5194/egusphere-2024-410, https://doi.org/10.5194/egusphere-2024-410, 2024
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We explore a new method to make use of the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, along with MERRA2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Tong Sha, Siyu Yang, Qingcai Chen, Liangqing Li, Xiaoyan Ma, Yan-Lin Zhang, Zhaozhong Feng, K. Folkert Boersma, and Jun Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-359, https://doi.org/10.5194/egusphere-2024-359, 2024
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By using an updated soil reactive nitrogen emission scheme in the UI-WRF-Chem model, we investigate the underappreciated role of soil NO and HONO (Nr) emissions on air quality and temperature rise in North China. The significant contributions of soil Nr emissions to O3 and secondary pollutants, exceeding the effects of soil NOx or HONO emission alone. And soil Nr emissions play an important role in mitigating O3 pollution and addressing climate change.
Jean-François Müller, Trissevgeni Stavrakou, Glenn-Michael Oomen, Beata Opacka, Isabelle De Smedt, Alex Guenther, Corinne Vigouroux, Bavo Langerock, Carlos Augusto Bauer Aquino, Michel Grutter, James Hannigan, Frank Hase, Rigel Kivi, Erik Lutsch, Emmanuel Mahieu, Maria Makarova, Jean-Marc Metzger, Isamu Morino, Isao Murata, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Amelie Röhling, Wolfgang Stremme, Kimberly Strong, Ralf Sussmann, Yao Té, and Alan Fried
Atmos. Chem. Phys., 24, 2207–2237, https://doi.org/10.5194/acp-24-2207-2024, https://doi.org/10.5194/acp-24-2207-2024, 2024
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Formaldehyde observations from satellites can be used to constrain the emissions of volatile organic compounds, but those observations have biases. Using an atmospheric model, aircraft and ground-based remote sensing data, we quantify these biases, propose a correction to the data, and assess the consequence of this correction for the evaluation of emissions.
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
EGUsphere, https://doi.org/10.5194/egusphere-2024-470, https://doi.org/10.5194/egusphere-2024-470, 2024
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Tropospheric ozone is a major air pollutant, greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side-by-side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
Joël Thanwerdas, Marielle Saunois, Antoine Berchet, Isabelle Pison, and Philippe Bousquet
Atmos. Chem. Phys., 24, 2129–2167, https://doi.org/10.5194/acp-24-2129-2024, https://doi.org/10.5194/acp-24-2129-2024, 2024
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We investigate the causes of the renewed growth of atmospheric methane (CH4) after 2007 using inverse modeling. We use the additional information provided by observations of CH4 isotopic compositions to better differentiate between the emission categories. Accounting for the large uncertainties in source signatures, our results suggest that the post-2007 increase in atmospheric CH4 was caused by similar increases in emissions from (1) fossil fuels and (2) agriculture and waste.
Robin Plauchu, Audrey Fortems-Cheiney, Grégoire Broquet, Isabelle Pison, Antoine Berchet, Elise Potier, Gaëlle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, and Henk Eskes
EGUsphere, https://doi.org/10.5194/egusphere-2024-103, https://doi.org/10.5194/egusphere-2024-103, 2024
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Over 2019–2021, our study used satellite data to assess NOx emissions in France. National budgets decreased due to effective policies, but COVID-19 lockdowns in 2020 didn't uniformly reduce emissions. Focusing on urban areas revealed varied impacts, with challenges like cloud coverage and model errors limiting precision. These findings contribute valuable insights into factors influencing emission assessments, informing future research.
Maarten Krol, Bart van Stratum, Isidora Anglou, and Klaas Folkert Boersma
EGUsphere, https://doi.org/10.5194/egusphere-2023-2519, https://doi.org/10.5194/egusphere-2023-2519, 2024
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This paper presents detailed plume simulations of nitrogen oxides and carbon dioxide that are emitted from four large industrial facilities world-wide. Results from the high-resolution simulations that include atmospheric chemistry are compared to nitrogen-dioxide observations from satellites. We find good performance of the model and show that common assumptions that are used in simplified models need revision. This work is important for the monitoring of emissions using satellite data.
Heather Simon, Christian Hogrefe, Andrew Whitehill, Kristen M. Foley, Jennifer Liljegren, Norm Possiel, Benjamin Wells, Barron H. Henderson, Lukas C. Valin, Gail Tonnesen, K. Wyat Appel, and Shannon Koplitz
Atmos. Chem. Phys., 24, 1855–1871, https://doi.org/10.5194/acp-24-1855-2024, https://doi.org/10.5194/acp-24-1855-2024, 2024
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We assess observed and modeled ozone weekend–weekday differences in the USA from 2002–2019. A subset of urban areas that were NOx-saturated at the beginning of the period transitioned to NOx-limited conditions. Multiple rural areas of California were NOx-limited for the entire period but become less influenced by local day-of-week emission patterns in more recent years. The model produces more NOx-saturated conditions than the observations but captures trends in weekend–weekday ozone patterns.
Rodrigo J. Seguel, Lucas Castillo, Charlie Opazo, Néstor Y. Rojas, Thiago Nogueira, María Cazorla, Mario Gavidia-Calderón, Laura Gallardo, René Garreaud, Tomás Carrasco-Escaff, and Yasin Elshorbany
EGUsphere, https://doi.org/10.5194/egusphere-2024-328, https://doi.org/10.5194/egusphere-2024-328, 2024
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Our research found that surface ozone trends in major South American cities increase or remain steady but show no signs of decreasing. Extra-tropical cities (Santiago and São Paulo), in particular, face the highest risk of ozone exposure. Furthermore, we found that prolonged heat waves and large fires explain many of the most extreme ozone values.
Ryan S. Williams, Michaela I. Hegglin, Patrick Jöckel, Hella Garny, and Keith P. Shine
Atmos. Chem. Phys., 24, 1389–1413, https://doi.org/10.5194/acp-24-1389-2024, https://doi.org/10.5194/acp-24-1389-2024, 2024
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During winter, a brief but abrupt reversal of the mean stratospheric westerly flow (~30 km high) around the Arctic occurs ~6 times a decade. Using a chemistry–climate model, about half of these events are shown to induce large anomalies in Arctic ozone (>25 %) and water vapour (>±25 %) around ~8–12 km altitude for up to 2–3 months, important for weather forecasting. We also calculate a doubling to trebling of the risk in breaches of mid-latitude surface air quality (ozone) standards (~60 ppbv).
Rona L. Thompson, Stephen A. Montzka, Martin K. Vollmer, Jgor Arduini, Molly Crotwell, Paul B. Krummel, Chris Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Stefan Reimann, Isaac Vimont, Hsiang Wang, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 24, 1415–1427, https://doi.org/10.5194/acp-24-1415-2024, https://doi.org/10.5194/acp-24-1415-2024, 2024
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The hydroxyl radical determines the atmospheric lifetimes of numerous species including methane. Since OH is very short-lived, it is not possible to directly measure its concentration on scales relevant for understanding its effect on other species. Here, OH is inferred by looking at changes in hydrofluorocarbons (HFCs). We find that OH levels have been fairly stable over our study period (2004 to 2021), suggesting that OH is not the main driver of the recent increase in atmospheric methane.
Zhendong Wu, Alex Vermeulen, Yousuke Sawa, Ute Karstens, Wouter Peters, Remco de Kok, Xin Lan, Yasuyuki Nagai, Akinori Ogi, and Oksana Tarasova
Atmos. Chem. Phys., 24, 1249–1264, https://doi.org/10.5194/acp-24-1249-2024, https://doi.org/10.5194/acp-24-1249-2024, 2024
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This study focuses on exploring the differences in calculating global surface CO2 and its growth rate, considering the impact of analysis methodologies and site selection. Our study reveals that the current global CO2 network has a good capacity to represent global surface CO2 and its growth rate, as well as trends in atmospheric CO2 mass changes. However, small differences exist in different analyses due to the impact of methodology and site selection.
Beth S. Nelson, Zhenze Liu, Freya A. Squires, Marvin Shaw, James R. Hopkins, Jacqueline F. Hamilton, Andrew R. Rickard, Alastair C. Lewis, Zongbo Shi, and James D. Lee
EGUsphere, https://doi.org/10.5194/egusphere-2023-2910, https://doi.org/10.5194/egusphere-2023-2910, 2024
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The impact of combined air quality and carbon neutrality policies on O3 formation in Beijing were investigated. Emissions inventory data was used to estimate future pollutant mixing ratios, relative to ground-level observations. O3 production was found to be most sensitive to changes in alkenes but large reductions in less reactive compounds led to larger reductions in future O3 production. This study highlights the importance of understanding the emission trajectories of organic pollutants.
Yang Yang, Yang Zhou, Hailong Wang, Mengyun Li, Huimin Li, Pinya Wang, Xu Yue, Ke Li, Jia Zhu, and Hong Liao
Atmos. Chem. Phys., 24, 1177–1191, https://doi.org/10.5194/acp-24-1177-2024, https://doi.org/10.5194/acp-24-1177-2024, 2024
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This study reveals that extreme ozone pollution over the North China Plain and Yangtze River Delta is due to the chemical production related to hot and dry conditions, and the regional transport explains the ozone pollution over the Sichuan Basin and Pearl River Delta. The frequency of meteorological conditions of the extreme ozone pollution increases from the past to the future. The sustainable scenario is the optimal path to retaining clean air in China in the future.
Victoria A. Flood, Kimberly Strong, Cynthia H. Whaley, Kaley A. Walker, Thomas Blumenstock, James W. Hannigan, Johan Mellqvist, Justus Notholt, Mathias Palm, Amelie N. Röhling, Stephen Arnold, Stephen Beagley, Rong-You Chien, Jesper Christensen, Makoto Deushi, Srdjan Dobricic, Xinyi Dong, Joshua S. Fu, Michael Gauss, Wanmin Gong, Joakim Langner, Kathy S. Law, Louis Marelle, Tatsuo Onishi, Naga Oshima, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Manu A. Thomas, Svetlana Tsyro, and Steven Turnock
Atmos. Chem. Phys., 24, 1079–1118, https://doi.org/10.5194/acp-24-1079-2024, https://doi.org/10.5194/acp-24-1079-2024, 2024
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It is important to understand the composition of the Arctic atmosphere and how it is changing. Atmospheric models provide simulations that can inform policy. This study examines simulations of CH4, CO, and O3 by 11 models. Model performance is assessed by comparing results matched in space and time to measurements from five high-latitude ground-based infrared spectrometers. This work finds that models generally underpredict the concentrations of these gases in the Arctic troposphere.
Roger Teoh, Zebediah Engberg, Marc Shapiro, Lynnette Dray, and Marc E. J. Stettler
Atmos. Chem. Phys., 24, 725–744, https://doi.org/10.5194/acp-24-725-2024, https://doi.org/10.5194/acp-24-725-2024, 2024
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Emissions from aircraft contribute to climate change and degrade air quality. We describe an up-to-date 4D emissions inventory of global aviation from 2019 to 2021 based on actual flown trajectories. In 2019, 40.2 million flights collectively travelled 61 billion kilometres using 283 Tg of fuel. Long-haul flights were responsible for 43 % of CO2. The emissions inventory is made available for use in future studies to evaluate the negative externalities arising from global aviation.
Jonas Hachmeister, Oliver Schneising, Michael Buchwitz, John P. Burrows, Justus Notholt, and Matthias Buschmann
Atmos. Chem. Phys., 24, 577–595, https://doi.org/10.5194/acp-24-577-2024, https://doi.org/10.5194/acp-24-577-2024, 2024
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We quantified changes in atmospheric methane concentrations using satellite data and a dynamic linear model approach. We calculated global annual methane increases for the years 2019–2022, which are in good agreement with other sources. For zonal methane growth rates, we identified strong inter-hemispheric differences in 2019 and 2022. For 2022, we could attribute decreases in the global growth rate to the Northern Hemisphere, possibly related to a reduction in anthropogenic emissions.
Glenn-Michael Oomen, Jean-François Müller, Trissevgeni Stavrakou, Isabelle De Smedt, Thomas Blumenstock, Rigel Kivi, Maria Makarova, Mathias Palm, Amelie Röhling, Yao Té, Corinne Vigouroux, Martina M. Friedrich, Udo Frieß, François Hendrick, Alexis Merlaud, Ankie Piters, Andreas Richter, Michel Van Roozendael, and Thomas Wagner
Atmos. Chem. Phys., 24, 449–474, https://doi.org/10.5194/acp-24-449-2024, https://doi.org/10.5194/acp-24-449-2024, 2024
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Natural emissions from vegetation have a profound impact on air quality for their role in the formation of harmful tropospheric ozone and organic aerosols, yet these emissions are highly uncertain. In this study, we quantify emissions of organic gases over Europe using high-quality satellite measurements of formaldehyde. These satellite observations suggest that emissions from vegetation are much higher than predicted by models, especially in southern Europe.
Yongliang She, Jingyi Li, Xiaopu Lyu, Hai Guo, Momei Qin, Xiaodong Xie, Kangjia Gong, Fei Ye, Jianjiong Mao, Lin Huang, and Jianlin Hu
Atmos. Chem. Phys., 24, 219–233, https://doi.org/10.5194/acp-24-219-2024, https://doi.org/10.5194/acp-24-219-2024, 2024
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In this study, we use multi-site volatile organic compound (VOC) measurements to evaluate the CMAQ-model-predicted VOCs and assess the impacts of VOC bias on O3 simulation. Our results demonstrate that current modeling setups and emission inventories are likely to underpredict VOC concentrations, and this underprediction of VOCs contributes to lower O3 predictions in China.
Peiyang Cheng, Arastoo Pour-Biazar, Yuling Wu, Shi Kuang, Richard T. McNider, and William J. Koshak
Atmos. Chem. Phys., 24, 41–63, https://doi.org/10.5194/acp-24-41-2024, https://doi.org/10.5194/acp-24-41-2024, 2024
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Lightning-induced nitrogen monoxide (LNO) emission can be estimated from geostationary satellite observations. The present study uses the LNO emission estimates derived from geostationary satellite observations in an air quality modeling system to investigate the impact of LNO on air quality. Results indicate that significant ozone increase could be due to long-distance chemical transport, lightning activity in the upwind direction, and the mixing of high LNO (or ozone) plumes.
Christian Rödenbeck, Karina E. Adcock, Markus Eritt, Maksym Gachkivskyi, Christoph Gerbig, Samuel Hammer, Armin Jordan, Ralph F. Keeling, Ingeborg Levin, Fabian Maier, Andrew C. Manning, Heiko Moossen, Saqr Munassar, Penelope A. Pickers, Michael Rothe, Yasunori Tohjima, and Sönke Zaehle
Atmos. Chem. Phys., 23, 15767–15782, https://doi.org/10.5194/acp-23-15767-2023, https://doi.org/10.5194/acp-23-15767-2023, 2023
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The carbon dioxide content of the Earth atmosphere is increasing due to human emissions from burning of fossil fuels, causing global climate change. The strength of the fossil-fuel emissions is estimated by inventories based on energy data, but independent validation of these inventories has been recommended by the Intergovernmental Panel on Climate Change. Here we investigate the potential to validate inventories based on measurements of small changes in the atmospheric oxygen content.
Xuewei Hou, Oliver Wild, Bin Zhu, and James Lee
Atmos. Chem. Phys., 23, 15395–15411, https://doi.org/10.5194/acp-23-15395-2023, https://doi.org/10.5194/acp-23-15395-2023, 2023
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In response to the climate crisis, many countries have committed to net zero in a certain future year. The impacts of net-zero scenarios on tropospheric O3 are less well studied and remain unclear. In this study, we quantified the changes of tropospheric O3 budgets, spatiotemporal distributions of future surface O3 in east Asia and regional O3 source contributions for 2060 under a net-zero scenario using the NCAR Community Earth System Model (CESM) and online O3-tagging methods.
Jian Zhu, Shanshan Wang, Chuanqi Gu, Zhiwen Jiang, Sanbao Zhang, Ruibin Xue, Yuhao Yan, and Bin Zhou
EGUsphere, https://doi.org/10.5194/egusphere-2023-2142, https://doi.org/10.5194/egusphere-2023-2142, 2023
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In 2022, Shanghai implemented city-wide static management measures during the high-ozone season in April and May, providing a change to study ozone pollution control. Despite significant emissions reductions, ozone levels increased by 23 %. Statistically, the number of days with higher ozone diurnal variation types increased during the lockdown period. The uneven decline in VOC and NO2 emissions led to heightened photochemical processes, resulting in the observed ozone level rise.
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Short summary
Marine-produced short-lived trace gases such as halocarbons and DMS significantly impact atmospheric chemistry. To assess this impact on ozone depletion and the radiative budget, it is critical that their marine emissions in atmospheric chemistry models are quantified as accurately as possible. We show that calculating emissions online with an interactive atmosphere improves the agreement with current observations and should be employed regularly in models where marine sources are important.
Marine-produced short-lived trace gases such as halocarbons and DMS significantly impact...
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