Articles | Volume 14, issue 7
https://doi.org/10.5194/acp-14-3589-2014
© Author(s) 2014. 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-14-3589-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
09 Apr 2014
Research article |
| 09 Apr 2014
Factors controlling variability in the oxidative capacity of the troposphere since the Last Glacial Maximum
L. T. Murray
School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
now at: Lamont-Doherty Earth Observatory, Columbia University, Palisades, NY, USA
L. J. Mickley
School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
J. O. Kaplan
ARVE Group, École Polytechnique Fédérale de Lausanne, Lausanne, Switzerland
E. D. Sofen
Department of Atmospheric Sciences, University of Washington, Seattle, WA, USA
M. Pfeiffer
ARVE Group, École Polytechnique Fédérale de Lausanne, Lausanne, Switzerland
B. Alexander
Department of Atmospheric Sciences, University of Washington, Seattle, WA, USA
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Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonne, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
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This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Zhuang Jiang, Becky Alexander, Joel Savarino, and Lei Geng
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We use the GEOS-Chem model to better understand the magnitude and trend in free tropospheric NO2 over the contiguous US. Model underestimate of background NO2 is largely corrected by considering aerosol nitrate photolysis. Increase in aircraft emissions affects satellite retrievals by altering the NO2 shape factor, and this effect is expected to increase in future. We show the importance of properly accounting for the free tropospheric background in interpreting NO2 observations from space.
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Atmos. Chem. Phys., 23, 4203–4219, https://doi.org/10.5194/acp-23-4203-2023, https://doi.org/10.5194/acp-23-4203-2023, 2023
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Short summary
Atmospheric nitrate has an important impact on human and ecosystem health. We evaluated atmospheric nitrate formation pathways in the northeastern US utilizing oxygen isotope compositions, which indicated a significant difference between the phases of nitrate (i.e., gas vs. particle). Comparing the observations with model simulations indicated that N2O5 hydrolysis chemistry was overpredicted. Our study has important implications for improving atmospheric chemistry model representation.
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Atmos. Meas. Tech., 16, 1431–1441, https://doi.org/10.5194/amt-16-1431-2023, https://doi.org/10.5194/amt-16-1431-2023, 2023
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Short summary
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Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
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Global lightning strokes are recorded continuously by a network of ground-based stations. We consolidated these point observations into a map form and provide these as electronic datasets for research purposes. Here we extend our dataset to include lightning observations from 2021.
Amy Christiansen, Loretta J. Mickley, Junhua Liu, Luke D. Oman, and Lu Hu
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Understanding tropospheric ozone trends is crucial for accurate predictions of future air quality and climate, but drivers of trends are not well understood. We analyze global tropospheric ozone trends since 1980 using ozonesonde and surface measurements, and we evaluate two models for their ability to reproduce trends. We find observational evidence of increasing tropospheric ozone, but models underestimate these increases. This hinders our ability to estimate ozone radiative forcing.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
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Yanzhi Cao, Zhuang Jiang, Becky Alexander, Jihong Cole-Dai, Joel Savarino, Joseph Erbland, and Lei Geng
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We investigate the potential of ice-core preserved nitrate isotopes as proxies of stratospheric ozone variability by measuring nitrate isotopes in a shallow ice core from the South Pole. The large variability in the snow accumulation rate and its slight increase after the 1970s masked any signals caused by the ozone hole. Moreover, the nitrate oxygen isotope decrease may reflect changes in the atmospheric oxidation environment in the Southern Ocean.
Basil Andrew Stansfield Davis, Marc Fasel, Jed O. Kaplan, Emmanuele Russo, and Ariane Burke
Clim. Past Discuss., https://doi.org/10.5194/cp-2022-59, https://doi.org/10.5194/cp-2022-59, 2022
Revised manuscript accepted for CP
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During the last Ice Age 21 k BP, Northern Europe was covered in ice and steppe, and forests were restricted to sheltered regions to the south. However, the composition and extent of forest and its associated climate remains unclear, with models indicating more forest north of the Alps than suggested by the data. A new compilation of pollen records with improved dating suggests greater agreement with model climate, but still suggests models over estimate forest cover especially in the west.
Zhuang Jiang, Joel Savarino, Becky Alexander, Joseph Erbland, Jean-Luc Jaffrezo, and Lei Geng
The Cryosphere, 16, 2709–2724, https://doi.org/10.5194/tc-16-2709-2022, https://doi.org/10.5194/tc-16-2709-2022, 2022
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A record of year-round atmospheric nitrate isotopic composition along with snow nitrate isotopic data from Summit, Greenland, revealed apparent enrichments in nitrogen isotopes in snow nitrate compared to atmospheric nitrate, in addition to a relatively smaller degree of changes in oxygen isotopes. The results suggest that at this site post-depositional processing takes effect, which should be taken into account when interpreting ice-core nitrate isotope records.
Liam Bindle, Randall V. Martin, Matthew J. Cooper, Elizabeth W. Lundgren, Sebastian D. Eastham, Benjamin M. Auer, Thomas L. Clune, Hongjian Weng, Jintai Lin, Lee T. Murray, Jun Meng, Christoph A. Keller, William M. Putman, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 14, 5977–5997, https://doi.org/10.5194/gmd-14-5977-2021, https://doi.org/10.5194/gmd-14-5977-2021, 2021
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Atmospheric chemistry models like GEOS-Chem are versatile tools widely used in air pollution and climate studies. The simulations used in such studies can be very computationally demanding, and thus it is useful if the model can simulate a specific geographic region at a higher resolution than the rest of the globe. Here, we implement, test, and demonstrate a new variable-resolution capability in GEOS-Chem that is suitable for simulations conducted on supercomputers.
Lee T. Murray, Eric M. Leibensperger, Clara Orbe, Loretta J. Mickley, and Melissa Sulprizio
Geosci. Model Dev., 14, 5789–5823, https://doi.org/10.5194/gmd-14-5789-2021, https://doi.org/10.5194/gmd-14-5789-2021, 2021
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Chemical-transport models are tools used to study air pollution and inform public policy. However, they are limited by the availability of archived meteorology. Here, we describe how the GEOS-Chem chemical-transport model may now be driven by meteorology archived from a state-of-the-art general circulation model for past and future climates, allowing it to be used to explore the impact of climate change on air pollution and atmospheric composition.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Zhuang Jiang, Becky Alexander, Joel Savarino, Joseph Erbland, and Lei Geng
The Cryosphere, 15, 4207–4220, https://doi.org/10.5194/tc-15-4207-2021, https://doi.org/10.5194/tc-15-4207-2021, 2021
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We used a snow photochemistry model (TRANSITS) to simulate the seasonal nitrate snow profile at Summit, Greenland. Comparisons between model outputs and observations suggest that at Summit post-depositional processing is active and probably dominates the snowpack δ15N seasonality. We also used the model to assess the degree of snow nitrate loss and the consequences in its isotopes at present and in the past, which helps for quantitative interpretations of ice-core nitrate records.
Jed O. Kaplan and Katie Hong-Kiu Lau
Earth Syst. Sci. Data, 13, 3219–3237, https://doi.org/10.5194/essd-13-3219-2021, https://doi.org/10.5194/essd-13-3219-2021, 2021
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Lightning is an important atmospheric phenomenon and natural hazard, but few long-term data are freely available on lightning stroke location, timing, and power. Here, we present a new, open-access dataset of lightning strokes covering 2010–2020, based on a network of low-frequency radio detectors. The dataset is comprised of GIS maps and is intended for researchers, government, industry, and anyone for whom knowing when and where lightning is likely to strike is useful information.
Patricio Velasquez, Jed O. Kaplan, Martina Messmer, Patrick Ludwig, and Christoph C. Raible
Clim. Past, 17, 1161–1180, https://doi.org/10.5194/cp-17-1161-2021, https://doi.org/10.5194/cp-17-1161-2021, 2021
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This study assesses the importance of resolution and land–atmosphere feedbacks for European climate. We performed an asynchronously coupled experiment that combined a global climate model (~ 100 km), a regional climate model (18 km), and a dynamic vegetation model (18 km). Modelled climate and land cover agree reasonably well with independent reconstructions based on pollen and other paleoenvironmental proxies. The regional climate is significantly influenced by land cover.
Kun Wang, Shohei Hattori, Mang Lin, Sakiko Ishino, Becky Alexander, Kazuki Kamezaki, Naohiro Yoshida, and Shichang Kang
Atmos. Chem. Phys., 21, 8357–8376, https://doi.org/10.5194/acp-21-8357-2021, https://doi.org/10.5194/acp-21-8357-2021, 2021
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Sulfate aerosols play an important climatic role and exert adverse effects on the ecological environment and human health. In this study, we present the triple oxygen isotopic composition of sulfate from the Mt. Everest region, southern Tibetan Plateau, and decipher the formation mechanisms of atmospheric sulfate in this pristine environment. The results indicate the important role of the S(IV) + O3 pathway in atmospheric sulfate formation promoted by conditions of high cloud water pH.
Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, https://doi.org/10.5194/acp-21-4187-2021, 2021
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We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.
Vasilii V. Petrenko, Andrew M. Smith, Edward M. Crosier, Roxana Kazemi, Philip Place, Aidan Colton, Bin Yang, Quan Hua, and Lee T. Murray
Atmos. Meas. Tech., 14, 2055–2063, https://doi.org/10.5194/amt-14-2055-2021, https://doi.org/10.5194/amt-14-2055-2021, 2021
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This paper presents an improved methodology for measurements of atmospheric concentration of carbon-14-containing carbon monoxide (14CO), as well as a 1-year dataset that demonstrates the methodology. Atmospheric 14CO concentration measurements are useful for improving the understanding of spatial and temporal variability of hydroxyl radical concentrations. Key improvements over prior methods include a greatly reduced air sample size and accurate procedural blank characterization.
Yang Li, Loretta J. Mickley, and Jed O. Kaplan
Atmos. Chem. Phys., 21, 57–68, https://doi.org/10.5194/acp-21-57-2021, https://doi.org/10.5194/acp-21-57-2021, 2021
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Climate models predict a shift toward warmer, drier environments in southwestern North America. Under future climate, the two main drivers of dust trends play opposing roles: (1) CO2 fertilization enhances vegetation and, in turn, decreases dust, and (2) increasing land use enhances dust emissions from northern Mexico. In the worst-case scenario, elevated dust concentrations spread widely over the domain by 2100 in spring, suggesting a large climate penalty on air quality and human health.
George C. Hurtt, Louise Chini, Ritvik Sahajpal, Steve Frolking, Benjamin L. Bodirsky, Katherine Calvin, Jonathan C. Doelman, Justin Fisk, Shinichiro Fujimori, Kees Klein Goldewijk, Tomoko Hasegawa, Peter Havlik, Andreas Heinimann, Florian Humpenöder, Johan Jungclaus, Jed O. Kaplan, Jennifer Kennedy, Tamás Krisztin, David Lawrence, Peter Lawrence, Lei Ma, Ole Mertz, Julia Pongratz, Alexander Popp, Benjamin Poulter, Keywan Riahi, Elena Shevliakova, Elke Stehfest, Peter Thornton, Francesco N. Tubiello, Detlef P. van Vuuren, and Xin Zhang
Geosci. Model Dev., 13, 5425–5464, https://doi.org/10.5194/gmd-13-5425-2020, https://doi.org/10.5194/gmd-13-5425-2020, 2020
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To estimate the effects of human land use activities on the carbon–climate system, a new set of global gridded land use forcing datasets was developed to link historical land use data to eight future scenarios in a standard format required by climate models. This new generation of land use harmonization (LUH2) includes updated inputs, higher spatial resolution, more detailed land use transitions, and the addition of important agricultural management layers; it will be used for CMIP6 simulations.
David S. Stevenson, Alcide Zhao, Vaishali Naik, Fiona M. O'Connor, Simone Tilmes, Guang Zeng, Lee T. Murray, William J. Collins, Paul T. Griffiths, Sungbo Shim, Larry W. Horowitz, Lori T. Sentman, and Louisa Emmons
Atmos. Chem. Phys., 20, 12905–12920, https://doi.org/10.5194/acp-20-12905-2020, https://doi.org/10.5194/acp-20-12905-2020, 2020
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We present historical trends in atmospheric oxidizing capacity (OC) since 1850 from the latest generation of global climate models and compare these with estimates from measurements. OC controls levels of many key reactive gases, including methane (CH4). We find small model trends up to 1980, then increases of about 9 % up to 2014, disagreeing with (uncertain) measurement-based trends. Major drivers of OC trends are emissions of CH4, NOx, and CO; these will be important for future CH4 trends.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys., 20, 10937–10951, https://doi.org/10.5194/acp-20-10937-2020, https://doi.org/10.5194/acp-20-10937-2020, 2020
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Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
Yang Li, Loretta J. Mickley, Pengfei Liu, and Jed O. Kaplan
Atmos. Chem. Phys., 20, 8827–8838, https://doi.org/10.5194/acp-20-8827-2020, https://doi.org/10.5194/acp-20-8827-2020, 2020
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Using a coupled vegetation–fire–climate modeling framework, we show a northward shift in forests and increased lightning fire activity in northern US states, including Idaho, Montana, and Wyoming. Our findings suggest a large climate penalty on ecosystem, air quality, visibility, and human health in a region valued for its national forests and parks. The fine-scale smoke PM predictions provided in this study should prove useful to human health and environmental assessments.
Jiayue Huang, Lyatt Jaeglé, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mat J. Evans, Nicolas Theys, and Sungyeon Choi
Atmos. Chem. Phys., 20, 7335–7358, https://doi.org/10.5194/acp-20-7335-2020, https://doi.org/10.5194/acp-20-7335-2020, 2020
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Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often observed in the springtime Arctic. Here, we use a chemical transport model to examine the role of sea salt aerosol from blowing snow in explaining these phenomena. We find that our simulation can account for the spatiotemporal variability of satellite observations of BrO. However, the model has difficulty in producing the magnitude of observed ozone depletion events.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Sandy P. Harrison, Marie-José Gaillard, Benjamin D. Stocker, Marc Vander Linden, Kees Klein Goldewijk, Oliver Boles, Pascale Braconnot, Andria Dawson, Etienne Fluet-Chouinard, Jed O. Kaplan, Thomas Kastner, Francesco S. R. Pausata, Erick Robinson, Nicki J. Whitehouse, Marco Madella, and Kathleen D. Morrison
Geosci. Model Dev., 13, 805–824, https://doi.org/10.5194/gmd-13-805-2020, https://doi.org/10.5194/gmd-13-805-2020, 2020
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The Past Global Changes LandCover6k initiative will use archaeological records to refine scenarios of land use and land cover change through the Holocene to reduce the uncertainties about the impacts of human-induced changes before widespread industrialization. We describe how archaeological data are used to map land use change and how the maps can be evaluated using independent palaeoenvironmental data. We propose simulations to test land use and land cover change impacts on past climates.
Julie M. Nicely, Bryan N. Duncan, Thomas F. Hanisco, Glenn M. Wolfe, Ross J. Salawitch, Makoto Deushi, Amund S. Haslerud, Patrick Jöckel, Béatrice Josse, Douglas E. Kinnison, Andrew Klekociuk, Michael E. Manyin, Virginie Marécal, Olaf Morgenstern, Lee T. Murray, Gunnar Myhre, Luke D. Oman, Giovanni Pitari, Andrea Pozzer, Ilaria Quaglia, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Kane Stone, Susan Strahan, Simone Tilmes, Holger Tost, Daniel M. Westervelt, and Guang Zeng
Atmos. Chem. Phys., 20, 1341–1361, https://doi.org/10.5194/acp-20-1341-2020, https://doi.org/10.5194/acp-20-1341-2020, 2020
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Differences in methane lifetime among global models are large and poorly understood. We use a neural network method and simulations from the Chemistry Climate Model Initiative to quantify the factors influencing methane lifetime spread among models and variations over time. UV photolysis, tropospheric ozone, and nitrogen oxides drive large model differences, while the same factors plus specific humidity contribute to a decreasing trend in methane lifetime between 1980 and 2015.
Pierre Friedlingstein, Matthew W. Jones, Michael O'Sullivan, Robbie M. Andrew, Judith Hauck, Glen P. Peters, Wouter Peters, Julia Pongratz, Stephen Sitch, Corinne Le Quéré, Dorothee C. E. Bakker, Josep G. Canadell, Philippe Ciais, Robert B. Jackson, Peter Anthoni, Leticia Barbero, Ana Bastos, Vladislav Bastrikov, Meike Becker, Laurent Bopp, Erik Buitenhuis, Naveen Chandra, Frédéric Chevallier, Louise P. Chini, Kim I. Currie, Richard A. Feely, Marion Gehlen, Dennis Gilfillan, Thanos Gkritzalis, Daniel S. Goll, Nicolas Gruber, Sören Gutekunst, Ian Harris, Vanessa Haverd, Richard A. Houghton, George Hurtt, Tatiana Ilyina, Atul K. Jain, Emilie Joetzjer, Jed O. Kaplan, Etsushi Kato, Kees Klein Goldewijk, Jan Ivar Korsbakken, Peter Landschützer, Siv K. Lauvset, Nathalie Lefèvre, Andrew Lenton, Sebastian Lienert, Danica Lombardozzi, Gregg Marland, Patrick C. McGuire, Joe R. Melton, Nicolas Metzl, David R. Munro, Julia E. M. S. Nabel, Shin-Ichiro Nakaoka, Craig Neill, Abdirahman M. Omar, Tsuneo Ono, Anna Peregon, Denis Pierrot, Benjamin Poulter, Gregor Rehder, Laure Resplandy, Eddy Robertson, Christian Rödenbeck, Roland Séférian, Jörg Schwinger, Naomi Smith, Pieter P. Tans, Hanqin Tian, Bronte Tilbrook, Francesco N. Tubiello, Guido R. van der Werf, Andrew J. Wiltshire, and Sönke Zaehle
Earth Syst. Sci. Data, 11, 1783–1838, https://doi.org/10.5194/essd-11-1783-2019, https://doi.org/10.5194/essd-11-1783-2019, 2019
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The Global Carbon Budget 2019 describes the data sets and methodology used to quantify the emissions of carbon dioxide and their partitioning among the atmosphere, land, and ocean. These living data are updated every year to provide the highest transparency and traceability in the reporting of CO2, the key driver of climate change.
Anina Gilgen, Stiig Wilkenskjeld, Jed O. Kaplan, Thomas Kühn, and Ulrike Lohmann
Clim. Past, 15, 1885–1911, https://doi.org/10.5194/cp-15-1885-2019, https://doi.org/10.5194/cp-15-1885-2019, 2019
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Using the global aerosol–climate model ECHAM-HAM-SALSA, the effect of humans on European climate in the Roman Empire was quantified. Both land use and novel estimates of anthropogenic aerosol emissions were considered. We conducted simulations with fixed sea-surface temperatures to gain a first impression about the anthropogenic impact. While land use effects induced a regional warming for one of the reconstructions, aerosol emissions led to a cooling associated with aerosol–cloud interactions.
Rachel F. Silvern, Daniel J. Jacob, Loretta J. Mickley, Melissa P. Sulprizio, Katherine R. Travis, Eloise A. Marais, Ronald C. Cohen, Joshua L. Laughner, Sungyeon Choi, Joanna Joiner, and Lok N. Lamsal
Atmos. Chem. Phys., 19, 8863–8878, https://doi.org/10.5194/acp-19-8863-2019, https://doi.org/10.5194/acp-19-8863-2019, 2019
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The US EPA reports a steady decrease in nitrogen oxide (NOx) emissions from fuel combustion over the 2005–2017 period, while satellite observations show a leveling off after 2009, suggesting emission reductions and related air quality gains have halted. We show the sustained decrease in NOx emissions is in fact consistent with observed trends in surface NO2 and ozone concentrations and that the flattening of the satellite trend reflects a growing influence from the non-anthropogenic background.
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
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Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Lu Shen, Daniel J. Jacob, Loretta J. Mickley, Yuxuan Wang, and Qiang Zhang
Atmos. Chem. Phys., 18, 17489–17496, https://doi.org/10.5194/acp-18-17489-2018, https://doi.org/10.5194/acp-18-17489-2018, 2018
Eloise A. Marais, Daniel J. Jacob, Sungyeon Choi, Joanna Joiner, Maria Belmonte-Rivas, Ronald C. Cohen, Steffen Beirle, Lee T. Murray, Luke D. Schiferl, Viral Shah, and Lyatt Jaeglé
Atmos. Chem. Phys., 18, 17017–17027, https://doi.org/10.5194/acp-18-17017-2018, https://doi.org/10.5194/acp-18-17017-2018, 2018
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We intercompare two new products of global upper tropospheric nitrogen dioxide (NO2) retrieved from the Ozone Monitoring Instrument (OMI). We evaluate these products with aircraft observations from NASA DC8 aircraft campaigns and interpret the useful information these products can provide about nitrogen oxides (NOx) in the global upper troposphere using the GEOS-Chem chemical transport model.
Samuel R. Hall, Kirk Ullmann, Michael J. Prather, Clare M. Flynn, Lee T. Murray, Arlene M. Fiore, Gustavo Correa, Sarah A. Strode, Stephen D. Steenrod, Jean-Francois Lamarque, Jonathan Guth, Béatrice Josse, Johannes Flemming, Vincent Huijnen, N. Luke Abraham, and Alex T. Archibald
Atmos. Chem. Phys., 18, 16809–16828, https://doi.org/10.5194/acp-18-16809-2018, https://doi.org/10.5194/acp-18-16809-2018, 2018
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Photolysis (J rates) initiates and drives atmospheric chemistry, and Js are perturbed by factors of 2 by clouds. The NASA Atmospheric Tomography (ATom) Mission provides the first comprehensive observations on how clouds perturb Js through the remote Pacific and Atlantic basins. We compare these cloud-perturbation J statistics with those from nine global chemistry models. While basic patterns agree, there is a large spread across models, and all lack some basic features of the observations.
Qianjie Chen, Tomás Sherwen, Mathew Evans, and Becky Alexander
Atmos. Chem. Phys., 18, 13617–13637, https://doi.org/10.5194/acp-18-13617-2018, https://doi.org/10.5194/acp-18-13617-2018, 2018
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Uncertainty in the natural tropospheric sulfur cycle represents the largest source of uncertainty in radiative forcing estimates of sulfate aerosol. This study investigates the natural sulfur cycle in the marine troposphere using the GEOS-Chem model. We found that BrO is important for DMS oxidation and multiphase chemistry is important for MSA production and loss, which have implications for the yield of SO2 and MSA from DMS oxidation and the radiative effect of DMS-derived sulfate aerosol.
Jean J. Guo, Arlene M. Fiore, Lee T. Murray, Daniel A. Jaffe, Jordan L. Schnell, Charles T. Moore, and George P. Milly
Atmos. Chem. Phys., 18, 12123–12140, https://doi.org/10.5194/acp-18-12123-2018, https://doi.org/10.5194/acp-18-12123-2018, 2018
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We use the GEOS-Chem model to estimate the influence from anthropogenic and background sources to ozone over the USA. Novel findings include the point that year-to-year background variability on the 10 highest observed ozone days is driven mainly by natural sources and not international or intercontinental pollution transport. High positive model biases during summer are associated with regional ozone production. The EPA 3-year average metric falls short of its aim to remove natural variability.
Prasad Kasibhatla, Tomás Sherwen, Mathew J. Evans, Lucy J. Carpenter, Chris Reed, Becky Alexander, Qianjie Chen, Melissa P. Sulprizio, James D. Lee, Katie A. Read, William Bloss, Leigh R. Crilley, William C. Keene, Alexander A. P. Pszenny, and Alma Hodzic
Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, https://doi.org/10.5194/acp-18-11185-2018, 2018
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Recent measurements of NOx and HONO suggest that photolysis of particulate nitrate in sea-salt aerosols is important in terms of marine boundary layer oxidant chemistry. We present the first global-scale assessment of the significance of this new chemical pathway for NOx, O3, and OH in the marine boundary layer. We also present a preliminary assessment of the potential impact of photolysis of particulate nitrate associated with other aerosol types on continental boundary layer chemistry.
Danny M. Leung, Amos P. K. Tai, Loretta J. Mickley, Jonathan M. Moch, Aaron van Donkelaar, Lu Shen, and Randall V. Martin
Atmos. Chem. Phys., 18, 6733–6748, https://doi.org/10.5194/acp-18-6733-2018, https://doi.org/10.5194/acp-18-6733-2018, 2018
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This paper investigates how large-scale weather systems control fine particulate matter (PM2.5) air quality in China. We show that winter monsoons, onshore winds and frontal rains can drive daily PM2.5 variability in different regions of China. We further project future PM2.5 concentration change by 2050s due to climate change, and verify that climate change has little benefit on future PM2.5 in Beijing, implying cutting down emissions is necessary to mitigate pollutions in megacities of China.
Michael J. Prather, Clare M. Flynn, Xin Zhu, Stephen D. Steenrod, Sarah A. Strode, Arlene M. Fiore, Gustavo Correa, Lee T. Murray, and Jean-Francois Lamarque
Atmos. Meas. Tech., 11, 2653–2668, https://doi.org/10.5194/amt-11-2653-2018, https://doi.org/10.5194/amt-11-2653-2018, 2018
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A new protocol for merging in situ atmospheric chemistry measurements with 3-D models is developed. This technique can identify the most reactive air parcels in terms of tropospheric production/loss of O3 & CH4. This approach highlights differences in 6 global chemistry models even with composition specified. Thus in situ measurements from, e.g., NASA's ATom mission can be used to develop a chemical climatology of, not only the key species, but also the rates of key reactions in each air parcel.
Pengzhen He, Becky Alexander, Lei Geng, Xiyuan Chi, Shidong Fan, Haicong Zhan, Hui Kang, Guangjie Zheng, Yafang Cheng, Hang Su, Cheng Liu, and Zhouqing Xie
Atmos. Chem. Phys., 18, 5515–5528, https://doi.org/10.5194/acp-18-5515-2018, https://doi.org/10.5194/acp-18-5515-2018, 2018
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We use observations of the oxygen isotopic composition of sulfate aerosol as a fingerprint to quantify various sulfate formation mechanisms during pollution events in Beijing, China. We found that heterogeneous reactions on aerosols dominated sulfate production in general; however, in-cloud reactions would dominate haze sulfate production when cloud liquid water content was high. The findings also suggest the heterogeneity of aerosol acidity should be parameterized in models.
Emeline Chaste, Martin P. Girardin, Jed O. Kaplan, Jeanne Portier, Yves Bergeron, and Christelle Hély
Biogeosciences, 15, 1273–1292, https://doi.org/10.5194/bg-15-1273-2018, https://doi.org/10.5194/bg-15-1273-2018, 2018
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A vegetation model was used to reconstruct fire activity from 1901 to 2012 in relation to changes in lightning ignition, climate, and vegetation in eastern Canada's boreal forest. The model correctly simulated the history of fire activity. The results showed that fire activity is ignition limited but is also greatly affected by both climate and vegetation. This research aims to develop a vegetation model that could be used to predict the future impacts of climate changes on fire activity.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Daniel H. Cusworth, Loretta J. Mickley, Eric M. Leibensperger, and Michael J. Iacono
Atmos. Chem. Phys., 17, 13559–13572, https://doi.org/10.5194/acp-17-13559-2017, https://doi.org/10.5194/acp-17-13559-2017, 2017
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Since 1990, light-scattering pollution known as aerosols have declined as a result of tightening US air quality regulations. Our study finds that US surface solar radiation has increased simultaneously. We establish a link between aerosols and radiation through physical and statistical models. We find the strongest relationship between aerosols, radiation, and climate at a site in the Midwest. Our work underscores the importance of regional pollution on climate in the US and abroad.
Jenny A. Fisher, Lee T. Murray, Dylan B. A. Jones, and Nicholas M. Deutscher
Geosci. Model Dev., 10, 4129–4144, https://doi.org/10.5194/gmd-10-4129-2017, https://doi.org/10.5194/gmd-10-4129-2017, 2017
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Carbon monoxide (CO) simulation in atmospheric chemistry models is used for source–receptor analysis, emission inversion, and interpretation of observations. We introduce a major update to CO simulation in the GEOS-Chem chemical transport model that removes fundamental inconsistencies relative to the standard model, resolving biases of more than 100 ppb and errors in vertical structure. We also add source tagging of secondary CO and demonstrate it provides added value in low-emission regions.
Johann H. Jungclaus, Edouard Bard, Mélanie Baroni, Pascale Braconnot, Jian Cao, Louise P. Chini, Tania Egorova, Michael Evans, J. Fidel González-Rouco, Hugues Goosse, George C. Hurtt, Fortunat Joos, Jed O. Kaplan, Myriam Khodri, Kees Klein Goldewijk, Natalie Krivova, Allegra N. LeGrande, Stephan J. Lorenz, Jürg Luterbacher, Wenmin Man, Amanda C. Maycock, Malte Meinshausen, Anders Moberg, Raimund Muscheler, Christoph Nehrbass-Ahles, Bette I. Otto-Bliesner, Steven J. Phipps, Julia Pongratz, Eugene Rozanov, Gavin A. Schmidt, Hauke Schmidt, Werner Schmutz, Andrew Schurer, Alexander I. Shapiro, Michael Sigl, Jason E. Smerdon, Sami K. Solanki, Claudia Timmreck, Matthew Toohey, Ilya G. Usoskin, Sebastian Wagner, Chi-Ju Wu, Kok Leng Yeo, Davide Zanchettin, Qiong Zhang, and Eduardo Zorita
Geosci. Model Dev., 10, 4005–4033, https://doi.org/10.5194/gmd-10-4005-2017, https://doi.org/10.5194/gmd-10-4005-2017, 2017
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Climate model simulations covering the last millennium provide context for the evolution of the modern climate and for the expected changes during the coming centuries. They can help identify plausible mechanisms underlying palaeoclimatic reconstructions. Here, we describe the forcing boundary conditions and the experimental protocol for simulations covering the pre-industrial millennium. We describe the PMIP4 past1000 simulations as contributions to CMIP6 and additional sensitivity experiments.
Philipp S. Sommer and Jed O. Kaplan
Geosci. Model Dev., 10, 3771–3791, https://doi.org/10.5194/gmd-10-3771-2017, https://doi.org/10.5194/gmd-10-3771-2017, 2017
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We present GWGEN, a computer program for converting monthly climate data into estimates of daily weather, using statistical methods. The GWGEN weather generator program was developed using a global database of more than 5 million observations of daily weather, and it simulates daily values of minimum and maximum temperature, precipitation, cloud cover, and wind speed. GWGEN may be used in a range of applications, for example, in global vegetation, crop, soil erosion, or hydrological models.
Michael J. Prather, Xin Zhu, Clare M. Flynn, Sarah A. Strode, Jose M. Rodriguez, Stephen D. Steenrod, Junhua Liu, Jean-Francois Lamarque, Arlene M. Fiore, Larry W. Horowitz, Jingqiu Mao, Lee T. Murray, Drew T. Shindell, and Steven C. Wofsy
Atmos. Chem. Phys., 17, 9081–9102, https://doi.org/10.5194/acp-17-9081-2017, https://doi.org/10.5194/acp-17-9081-2017, 2017
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We present a new approach for comparing atmospheric chemistry models with measurements based on what these models are used to do, i.e., calculate changes in ozone and methane, prime greenhouse gases. This method anticipates a new type of measurements from the NASA Atmospheric Tomography (ATom) mission. In comparing the mixture of species within air parcels, we focus on those responsible for key chemical changes and weight these parcels by their chemical reactivity.
Lu Shen, Loretta J. Mickley, and Lee T. Murray
Atmos. Chem. Phys., 17, 4355–4367, https://doi.org/10.5194/acp-17-4355-2017, https://doi.org/10.5194/acp-17-4355-2017, 2017
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We introduce a new method to characterize the influence of atmospheric circulation on surface PM2.5 concentrations. Applying our statistical model to climate projections, we find a strong influence of 2000–2050 climate change on PM2.5 air quality in the United States. We find that current atmospheric chemistry models may underestimate the strong positive sensitivity of PM2.5 to temperature in the eastern United States in summer, and so may underestimate PM2.5 changes in a warmer climate.
Sam S. Rabin, Joe R. Melton, Gitta Lasslop, Dominique Bachelet, Matthew Forrest, Stijn Hantson, Jed O. Kaplan, Fang Li, Stéphane Mangeon, Daniel S. Ward, Chao Yue, Vivek K. Arora, Thomas Hickler, Silvia Kloster, Wolfgang Knorr, Lars Nieradzik, Allan Spessa, Gerd A. Folberth, Tim Sheehan, Apostolos Voulgarakis, Douglas I. Kelley, I. Colin Prentice, Stephen Sitch, Sandy Harrison, and Almut Arneth
Geosci. Model Dev., 10, 1175–1197, https://doi.org/10.5194/gmd-10-1175-2017, https://doi.org/10.5194/gmd-10-1175-2017, 2017
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Global vegetation models are important tools for understanding how the Earth system will change in the future, and fire is a critical process to include. A number of different methods have been developed to represent vegetation burning. This paper describes the protocol for the first systematic comparison of global fire models, which will allow the community to explore various drivers and evaluate what mechanisms are important for improving performance. It also includes equations for all models.
Tomás Sherwen, Mat J. Evans, Lucy J. Carpenter, Johan A. Schmidt, and Loretta J. Mickley
Atmos. Chem. Phys., 17, 1557–1569, https://doi.org/10.5194/acp-17-1557-2017, https://doi.org/10.5194/acp-17-1557-2017, 2017
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We model pre-industrial to present day changes using the GEOS-Chem global chemical transport model with halogens (Cl, Br, I). The model better captures pre-industrial O3 observations with halogens included. Halogens buffer the tropospheric forcing of O3 (RFTO3) from pre-industrial to present day, reducing RFTO3 by 0.087 Wm−2. This reduction is greater than that from halogens on stratospheric O3 (−0.05 Wm−2). This suggests that models that do not include halogens will overestimate RFTO3by ~ 25%.
Maria Zatko, Joseph Erbland, Joel Savarino, Lei Geng, Lauren Easley, Andrew Schauer, Timothy Bates, Patricia K. Quinn, Bonnie Light, David Morison, Hans D. Osthoff, Seth Lyman, William Neff, Bin Yuan, and Becky Alexander
Atmos. Chem. Phys., 16, 13837–13851, https://doi.org/10.5194/acp-16-13837-2016, https://doi.org/10.5194/acp-16-13837-2016, 2016
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This manuscript presents chemical and optical observations collected in the air and snow during UBWOS2014 in eastern Utah. These observations are used to calculate fluxes of reactive nitrogen associated with snow nitrate photolysis. Snow-sourced reactive nitrogen fluxes are compared to reactive nitrogen emission inventories to find that snow-sourced reactive nitrogen is a minor contributor to the reactive nitrogen budget, and thus wintertime ground-level ozone formation, in the Uintah Basin.
Lei Zhu, Daniel J. Jacob, Patrick S. Kim, Jenny A. Fisher, Karen Yu, Katherine R. Travis, Loretta J. Mickley, Robert M. Yantosca, Melissa P. Sulprizio, Isabelle De Smedt, Gonzalo González Abad, Kelly Chance, Can Li, Richard Ferrare, Alan Fried, Johnathan W. Hair, Thomas F. Hanisco, Dirk Richter, Amy Jo Scarino, James Walega, Petter Weibring, and Glenn M. Wolfe
Atmos. Chem. Phys., 16, 13477–13490, https://doi.org/10.5194/acp-16-13477-2016, https://doi.org/10.5194/acp-16-13477-2016, 2016
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HCHO column data are widely used as a proxy for VOCs emissions, but validation of the data has been extremely limited. We use accurate aircraft observations to validate and intercompare 6 HCHO retrievals with GEOS-Chem as the intercomparison platform. Retrievals are interconsistent in spatial variability over the SE US and in daily variability, but are biased low by 20–51 %. Our work supports the use of HCHO column as a quantitative proxy for isoprene emission after correction of the low bias.
Qianjie Chen, Lei Geng, Johan A. Schmidt, Zhouqing Xie, Hui Kang, Jordi Dachs, Jihong Cole-Dai, Andrew J. Schauer, Madeline G. Camp, and Becky Alexander
Atmos. Chem. Phys., 16, 11433–11450, https://doi.org/10.5194/acp-16-11433-2016, https://doi.org/10.5194/acp-16-11433-2016, 2016
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The formation mechanisms of sulfate in the marine boundary layer are not well understood, which could result in large uncertainties in aerosol radiative forcing. We measure the oxygen isotopic composition (Δ17O) of sulfate collected in the MBL and analyze with a global transport model. Our results suggest that 33–50 % of MBL sulfate is formed via oxidation of S(IV) by hypohalous acids HOBr / HOCl in the aqueous phase, and the daily-mean HOBr/HOCl concentrations are on the order of 0.01–0.1 ppt.
Stijn Hantson, Almut Arneth, Sandy P. Harrison, Douglas I. Kelley, I. Colin Prentice, Sam S. Rabin, Sally Archibald, Florent Mouillot, Steve R. Arnold, Paulo Artaxo, Dominique Bachelet, Philippe Ciais, Matthew Forrest, Pierre Friedlingstein, Thomas Hickler, Jed O. Kaplan, Silvia Kloster, Wolfgang Knorr, Gitta Lasslop, Fang Li, Stephane Mangeon, Joe R. Melton, Andrea Meyn, Stephen Sitch, Allan Spessa, Guido R. van der Werf, Apostolos Voulgarakis, and Chao Yue
Biogeosciences, 13, 3359–3375, https://doi.org/10.5194/bg-13-3359-2016, https://doi.org/10.5194/bg-13-3359-2016, 2016
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Our ability to predict the magnitude and geographic pattern of past and future fire impacts rests on our ability to model fire regimes. A large variety of models exist, and it is unclear which type of model or degree of complexity is required to model fire adequately at regional to global scales. In this paper we summarize the current state of the art in fire-regime modelling and model evaluation, and outline what lessons may be learned from the Fire Model Intercomparison Project – FireMIP.
M. Clare Smith, Joy S. Singarayer, Paul J. Valdes, Jed O. Kaplan, and Nicholas P. Branch
Clim. Past, 12, 923–941, https://doi.org/10.5194/cp-12-923-2016, https://doi.org/10.5194/cp-12-923-2016, 2016
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We used climate modelling to estimate the biogeophysical impacts of agriculture on the climate over the last 8000 years of the Holocene. Our results show statistically significant surface temperature changes (mainly cooling) from as early as 7000 BP in the JJA season and throughout the entire annual cycle by 2–3000 BP. The changes were greatest in the areas of land use change but were also seen in other areas. Precipitation was also affected, particularly in Europe, India, and the ITCZ region.
Maria Zatko, Lei Geng, Becky Alexander, Eric Sofen, and Katarina Klein
Atmos. Chem. Phys., 16, 2819–2842, https://doi.org/10.5194/acp-16-2819-2016, https://doi.org/10.5194/acp-16-2819-2016, 2016
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We have incorporated an idealized snowpack with a nitrate photolysis parameterization into a global chemical transport model (GEOS-Chem) to examine the implications of snow nitrate photolysis for boundary layer chemistry, the recycling and redistribution of reactive nitrogen, and the preservation of ice-core nitrate in ice cores across Antarctica and Greenland. We also examine the sensitivity of these processes to meteorological parameters and chemical, optical, and physical snow properties.
Zhen Zhang, Niklaus E. Zimmermann, Jed O. Kaplan, and Benjamin Poulter
Biogeosciences, 13, 1387–1408, https://doi.org/10.5194/bg-13-1387-2016, https://doi.org/10.5194/bg-13-1387-2016, 2016
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This study investigates improvements and uncertainties associated with estimating global inundated area and wetland CH4 emissions using TOPMODEL. Different topographic information and catchment aggregation schemes are evaluated against seasonal and permanently inundated wetland observations. Reducing uncertainty in prognostic wetland dynamics modeling must take into account forcing data as well as topographic scaling schemes.
L. Shen, L. J. Mickley, and A. P. K. Tai
Atmos. Chem. Phys., 15, 10925–10938, https://doi.org/10.5194/acp-15-10925-2015, https://doi.org/10.5194/acp-15-10925-2015, 2015
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In this study, we have examined the effect of polar jet and Bermuda High on ozone air quality in the eastern United States. In the Midwest and northeast, the poleward shift of jet wind leads to reduced polar jet frequency, resulting in increased ozone there. In the southeast, the influence of Bermuda High on ozone variability depends on the location of its west edge. Westward movement increases the ozone only when the JJA Bermuda High west edge is located west of 85.4°W.
X. Yue, L. J. Mickley, J. A. Logan, R. C. Hudman, M. V. Martin, and R. M. Yantosca
Atmos. Chem. Phys., 15, 10033–10055, https://doi.org/10.5194/acp-15-10033-2015, https://doi.org/10.5194/acp-15-10033-2015, 2015
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Based on simulated meteorology from 13 GCMs, we projected future wildfire activity in Alaskan and Canadian ecoregions by the mid-century. The most robust change is the increase of 150-390% in area burned over Alaska and western Canada. The models also predict an increase of 45-90% in the central and southern Canadian ecoregions, but a decrease of up to 50% in northern Canada. We further quantify how the changes in wildfire emissions may affect ozone concentrations in North America.
M. J. McGrath, S. Luyssaert, P. Meyfroidt, J. O. Kaplan, M. Bürgi, Y. Chen, K. Erb, U. Gimmi, D. McInerney, K. Naudts, J. Otto, F. Pasztor, J. Ryder, M.-J. Schelhaas, and A. Valade
Biogeosciences, 12, 4291–4316, https://doi.org/10.5194/bg-12-4291-2015, https://doi.org/10.5194/bg-12-4291-2015, 2015
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Studying century-scale ecological processes and their legacy effects requires taking forest management into account. In this study we produce spatially and temporally explicit maps of European forest management from 1600 to 2010. The most important changes between 1600 and 2010 are an increase of 593 000km2 in conifers at the expense of deciduous forest, a 612 000km2 decrease in unmanaged forest, a 152 000km2 decrease in coppice management and a 818 000km2 increase in high stand management.
P. Achakulwisut, L. J. Mickley, L. T. Murray, A. P. K. Tai, J. O. Kaplan, and B. Alexander
Atmos. Chem. Phys., 15, 7977–7998, https://doi.org/10.5194/acp-15-7977-2015, https://doi.org/10.5194/acp-15-7977-2015, 2015
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The atmosphere’s oxidative capacity determines the lifetime of many trace gases important to climate, chemistry, and human health. Yet uncertainties remain about its past variations, its controlling factors, and the radiative forcing of short-lived species it influences. To reduce these uncertainties, we must better quantify the natural emissions and chemical reaction mechanisms of organic compounds in the atmosphere, which play a role in governing the oxidative capacity.
T. J. Bohn, J. R. Melton, A. Ito, T. Kleinen, R. Spahni, B. D. Stocker, B. Zhang, X. Zhu, R. Schroeder, M. V. Glagolev, S. Maksyutov, V. Brovkin, G. Chen, S. N. Denisov, A. V. Eliseev, A. Gallego-Sala, K. C. McDonald, M.A. Rawlins, W. J. Riley, Z. M. Subin, H. Tian, Q. Zhuang, and J. O. Kaplan
Biogeosciences, 12, 3321–3349, https://doi.org/10.5194/bg-12-3321-2015, https://doi.org/10.5194/bg-12-3321-2015, 2015
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We evaluated 21 forward models and 5 inversions over western Siberia in terms of CH4 emissions and simulated wetland areas and compared these results to an intensive in situ CH4 flux data set, several wetland maps, and two satellite inundation products. In addition to assembling a definitive collection of methane emissions estimates for the region, we were able to identify the types of wetland maps and model features necessary for accurate simulations of high-latitude wetlands.
L. Geng, J. Cole-Dai, B. Alexander, J. Erbland, J. Savarino, A. J. Schauer, E. J. Steig, P. Lin, Q. Fu, and M. C. Zatko
Atmos. Chem. Phys., 14, 13361–13376, https://doi.org/10.5194/acp-14-13361-2014, https://doi.org/10.5194/acp-14-13361-2014, 2014
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Examinations on snowpit and firn core results from Summit, Greenland suggest that there are two mechanisms leading to the observed double nitrate peaks in some years in the industrial era: 1) long-rang transport of nitrate and 2) enhanced local photochemical production of nitrate. Both of these mechanisms are related to pollution transport, as the additional nitrate from either direct transport or enhanced local photochemistry requires enhanced nitrogen sources from anthropogenic emissions.
A. Mauri, B. A. S. Davis, P. M. Collins, and J. O. Kaplan
Clim. Past, 10, 1925–1938, https://doi.org/10.5194/cp-10-1925-2014, https://doi.org/10.5194/cp-10-1925-2014, 2014
E. D. Sofen, B. Alexander, E. J. Steig, M. H. Thiemens, S. A. Kunasek, H. M. Amos, A. J. Schauer, M. G. Hastings, J. Bautista, T. L. Jackson, L. E. Vogel, J. R. McConnell, D. R. Pasteris, and E. S. Saltzman
Atmos. Chem. Phys., 14, 5749–5769, https://doi.org/10.5194/acp-14-5749-2014, https://doi.org/10.5194/acp-14-5749-2014, 2014
G. Strandberg, E. Kjellström, A. Poska, S. Wagner, M.-J. Gaillard, A.-K. Trondman, A. Mauri, B. A. S. Davis, J. O. Kaplan, H. J. B. Birks, A. E. Bjune, R. Fyfe, T. Giesecke, L. Kalnina, M. Kangur, W. O. van der Knaap, U. Kokfelt, P. Kuneš, M. Lata\l owa, L. Marquer, F. Mazier, A. B. Nielsen, B. Smith, H. Seppä, and S. Sugita
Clim. Past, 10, 661–680, https://doi.org/10.5194/cp-10-661-2014, https://doi.org/10.5194/cp-10-661-2014, 2014
T. Hoffmann, S. M. Mudd, K. van Oost, G. Verstraeten, G. Erkens, A. Lang, H. Middelkoop, J. Boyle, J. O. Kaplan, J. Willenbring, and R. Aalto
Earth Surf. Dynam., 1, 45–52, https://doi.org/10.5194/esurf-1-45-2013, https://doi.org/10.5194/esurf-1-45-2013, 2013
M. Scherstjanoi, J. O. Kaplan, E. Thürig, and H. Lischke
Geosci. Model Dev., 6, 1517–1542, https://doi.org/10.5194/gmd-6-1517-2013, https://doi.org/10.5194/gmd-6-1517-2013, 2013
V. Beck, C. Gerbig, T. Koch, M. M. Bela, K. M. Longo, S. R. Freitas, J. O. Kaplan, C. Prigent, P. Bergamaschi, and M. Heimann
Atmos. Chem. Phys., 13, 7961–7982, https://doi.org/10.5194/acp-13-7961-2013, https://doi.org/10.5194/acp-13-7961-2013, 2013
H. Jiang, H. Liao, H. O. T. Pye, S. Wu, L. J. Mickley, J. H. Seinfeld, and X. Y. Zhang
Atmos. Chem. Phys., 13, 7937–7960, https://doi.org/10.5194/acp-13-7937-2013, https://doi.org/10.5194/acp-13-7937-2013, 2013
M. Pfeiffer, A. Spessa, and J. O. Kaplan
Geosci. Model Dev., 6, 643–685, https://doi.org/10.5194/gmd-6-643-2013, https://doi.org/10.5194/gmd-6-643-2013, 2013
R. Wania, J. R. Melton, E. L. Hodson, B. Poulter, B. Ringeval, R. Spahni, T. Bohn, C. A. Avis, G. Chen, A. V. Eliseev, P. O. Hopcroft, W. J. Riley, Z. M. Subin, H. Tian, P. M. van Bodegom, T. Kleinen, Z. C. Yu, J. S. Singarayer, S. Zürcher, D. P. Lettenmaier, D. J. Beerling, S. N. Denisov, C. Prigent, F. Papa, and J. O. Kaplan
Geosci. Model Dev., 6, 617–641, https://doi.org/10.5194/gmd-6-617-2013, https://doi.org/10.5194/gmd-6-617-2013, 2013
J. R. Melton, R. Wania, E. L. Hodson, B. Poulter, B. Ringeval, R. Spahni, T. Bohn, C. A. Avis, D. J. Beerling, G. Chen, A. V. Eliseev, S. N. Denisov, P. O. Hopcroft, D. P. Lettenmaier, W. J. Riley, J. S. Singarayer, Z. M. Subin, H. Tian, S. Zürcher, V. Brovkin, P. M. van Bodegom, T. Kleinen, Z. C. Yu, and J. O. Kaplan
Biogeosciences, 10, 753–788, https://doi.org/10.5194/bg-10-753-2013, https://doi.org/10.5194/bg-10-753-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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
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
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
Evaluation of modelled versus observed NMVOC compounds at EMEP sites in Europe
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
Constraint of non-methane volatile organic compound emissions with TROPOMI HCHO observations and its impact on summertime surface ozone simulation over China
The suitability of atmospheric oxygen measurements to constrain western European fossil-fuel CO2 emissions and their trends
Identifying decadal trends in deweathered concentrations of criteria air pollutants in Canadian urban atmospheres with machine learning approaches
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
Comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA: implications for atmospheric oxidative capacity
Insights into soil NO emissions and the contribution to surface ozone formation in China
Development, intercomparison, and evaluation of an improved mechanism for the oxidation of dimethyl sulfide in the UKCA model
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.
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.
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.
Yao Ge, Sverre Solberg, Mathew Heal, Stefan Reimann, Willem van Caspel, Bryan Hellack, Thérèse Salameh, and David Simpson
EGUsphere, https://doi.org/10.5194/egusphere-2023-3102, https://doi.org/10.5194/egusphere-2023-3102, 2024
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Atmospheric volatile organic compounds (VOC) 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.
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.
Shuzhuang Feng, Fei Jiang, Tianlu Qian, Nan Wang, Mengwei Jia, Songci Zheng, Jiansong Chen, Fang Ying, and Weimin Ju
EGUsphere, https://doi.org/10.5194/egusphere-2023-2654, https://doi.org/10.5194/egusphere-2023-2654, 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.
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.
Xiaohong Yao and Leiming Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2023-2968, https://doi.org/10.5194/egusphere-2023-2968, 2023
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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 ten Canadian cities during the last two to three decades and associated driving forces in terms of emission reductions, perturbations from varying weather conditions and large-scale wildfires, and changes in O3 sources and sinks.
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.
Meghna Soni, Rolf Sander, Lokesh K. Sahu, Domenico Taraborrelli, Pengfei Liu, Ankit Patel, Imran A. Girach, Andrea Pozzer, Sachin S. Gunthe, and Narendra Ojha
Atmos. Chem. Phys., 23, 15165–15180, https://doi.org/10.5194/acp-23-15165-2023, https://doi.org/10.5194/acp-23-15165-2023, 2023
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The study presents the implementation of comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA. Simulations for contrasting urban environments of Asia and Europe highlight the significant impacts of chlorine on atmospheric oxidation capacity and composition. Chemical processes governing the production and loss of chlorine-containing species has been discussed. The updated chemical mechanism will be useful to interpret field measurements and for future air quality studies.
Ling Huang, Jiong Fang, Jiaqiang Liao, Greg Yarwood, Hui Chen, Yangjun Wang, and Li Li
Atmos. Chem. Phys., 23, 14919–14932, https://doi.org/10.5194/acp-23-14919-2023, https://doi.org/10.5194/acp-23-14919-2023, 2023
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Surface ozone concentrations have emerged as a major environmental issue in China. Although control strategies aimed at reducing NOx emissions from conventional combustion sources are widely recognized, soil NOx emissions have received little attention. The impact of soil NO emissions on ground-level ozone concentration is yet to be evaluated. In this study, we estimated the soil NO emissions and evaluated its impact on ozone formation in China.
Ben A. Cala, Scott Archer-Nicholls, James Weber, N. Luke Abraham, Paul T. Griffiths, Lorrie Jacob, Y. Matthew Shin, Laura E. Revell, Matthew Woodhouse, and Alexander T. Archibald
Atmos. Chem. Phys., 23, 14735–14760, https://doi.org/10.5194/acp-23-14735-2023, https://doi.org/10.5194/acp-23-14735-2023, 2023
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Dimethyl sulfide (DMS) is an important trace gas emitted from the ocean recognised as setting the sulfate aerosol background, but its oxidation is complex. As a result representation in chemistry-climate models is greatly simplified. We develop and compare a new mechanism to existing mechanisms via a series of global and box model experiments. Our studies show our updated DMS scheme is a significant improvement but significant variance exists between mechanisms.
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