Articles | Volume 18, issue 18
https://doi.org/10.5194/acp-18-13617-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-18-13617-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
27 Sep 2018
Research article |
| 27 Sep 2018
| 27 Sep 2018
DMS oxidation and sulfur aerosol formation in the marine troposphere: a focus on reactive halogen and multiphase chemistry
Qianjie Chen
Department of Atmospheric Sciences, University of Washington, Seattle, WA, USA
now at: Department of Chemistry, University of Michigan, Ann Arbor, MI, USA
Tomás Sherwen
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK
National Centre for Atmospheric Science (NCAS), University of York, York, UK
Mathew Evans
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK
National Centre for Atmospheric Science (NCAS), University of York, York, UK
Becky Alexander
CORRESPONDING AUTHOR
Department of Atmospheric Sciences, University of Washington, Seattle, WA, USA
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Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles A. Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
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Zhouxing Zou, Qianjie Chen, Men Xia, Qi Yuan, Yi Chen, Yanan Wang, Enyu Xiong, Zhe Wang, and Tao Wang
Atmos. Chem. Phys., 23, 7057–7074, https://doi.org/10.5194/acp-23-7057-2023, https://doi.org/10.5194/acp-23-7057-2023, 2023
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Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
Simone T. Andersen, Beth S. Nelson, Katie A. Read, Shalini Punjabi, Luis Neves, Matthew J. Rowlinson, James Hopkins, Tomás Sherwen, Lisa K. Whalley, James D. Lee, and Lucy J. Carpenter
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During a spring field campaign in the coastal Arctic, ultrafine particles were enhanced during high wind speeds, and coarse-mode particles were reduced during blowing snow. Calculated periods blowing snow were overpredicted compared to observations. Sea spray aerosols produced by sea ice leads affected the composition of aerosols and snowpack. An improved understanding of aerosol emissions from leads and blowing snow is critical for predicting the future climate of the rapidly warming Arctic.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
Atmos. Chem. Phys., 22, 14467–14488, https://doi.org/10.5194/acp-22-14467-2022, https://doi.org/10.5194/acp-22-14467-2022, 2022
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Radical bromine molecules are seen at higher concentrations during the Arctic spring. We use the global model GEOS-Chem to test whether snowpack and wind-blown snow sources can explain high bromine concentrations. We run this model for the entire year of 2015 and compare results to observations of bromine from floating platforms on the Arctic Ocean and at Utqiaġvik. We find that the model performs best when both sources are enabled but may overestimate bromine production in summer and fall.
Yanzhi Cao, Zhuang Jiang, Becky Alexander, Jihong Cole-Dai, Joel Savarino, Joseph Erbland, and Lei Geng
Atmos. Chem. Phys., 22, 13407–13422, https://doi.org/10.5194/acp-22-13407-2022, https://doi.org/10.5194/acp-22-13407-2022, 2022
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We investigate the potential of ice-core preserved nitrate isotopes as proxies of stratospheric ozone variability by measuring nitrate isotopes in a shallow ice core from the South Pole. The large variability in the snow accumulation rate and its slight increase after the 1970s masked any signals caused by the ozone hole. Moreover, the nitrate oxygen isotope decrease may reflect changes in the atmospheric oxidation environment in the Southern Ocean.
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.
Kathryn D. Kulju, Stephen M. McNamara, Qianjie Chen, Hannah S. Kenagy, Jacinta Edebeli, Jose D. Fuentes, Steven B. Bertman, and Kerri A. Pratt
Atmos. Chem. Phys., 22, 2553–2568, https://doi.org/10.5194/acp-22-2553-2022, https://doi.org/10.5194/acp-22-2553-2022, 2022
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N2O5 uptake by chloride-containing surfaces produces ClNO2, which photolyzes, producing NO2 and highly reactive Cl radicals that impact air quality. In the inland urban atmosphere, ClNO2 was elevated during lower air turbulence and over snow-covered ground, from snowpack ClNO2 production. N2O5 and ClNO2 levels were lowest, on average, during rainfall and fog because of scavenging, with N2O5 scavenging by fog droplets likely contributing to observed increased particulate nitrate concentrations.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Tomás Sherwen, Rainer Volkamer, Theodore K. Koenig, Tanguy Giroud, and Thomas Peter
Geosci. Model Dev., 14, 6623–6645, https://doi.org/10.5194/gmd-14-6623-2021, https://doi.org/10.5194/gmd-14-6623-2021, 2021
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Here, we present the iodine chemistry module in the SOCOL-AERv2 model. The obtained iodine distribution demonstrated a good agreement when validated against other simulations and available observations. We also estimated the iodine influence on ozone in the case of present-day iodine emissions, the sensitivity of ozone to doubled iodine emissions, and when considering only organic or inorganic iodine sources. The new model can be used as a tool for further studies of iodine effects on ozone.
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 %.
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.
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.
Christoph A. Keller, Mathew J. Evans, K. Emma Knowland, Christa A. Hasenkopf, Sruti Modekurty, Robert A. Lucchesi, Tomohiro Oda, Bruno B. Franca, Felipe C. Mandarino, M. Valeria Díaz Suárez, Robert G. Ryan, Luke H. Fakes, and Steven Pawson
Atmos. Chem. Phys., 21, 3555–3592, https://doi.org/10.5194/acp-21-3555-2021, https://doi.org/10.5194/acp-21-3555-2021, 2021
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This study combines surface observations and model simulations to quantify the impact of COVID-19 restrictions on air quality across the world. The presented methodology removes the confounding impacts of meteorology on air pollution. Our results indicate that surface concentrations of nitrogen dioxide, an important air pollutant emitted during the combustion of fossil fuels, declined by up to 60 % following the implementation of COVID-19 containment measures.
Angharad C. Stell, Luke M. Western, Tomás Sherwen, and Matthew Rigby
Atmos. Chem. Phys., 21, 1717–1736, https://doi.org/10.5194/acp-21-1717-2021, https://doi.org/10.5194/acp-21-1717-2021, 2021
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Although it is the second-most important greenhouse gas, our understanding of the atmospheric-methane budget is limited. The uncertainty highlights the need for new tools to investigate sources and sinks. Here, we use a Gaussian process emulator to efficiently approximate the response of atmospheric-methane observations to changes in the most uncertain emission or loss processes. With this new method, we rigorously quantify the sensitivity of atmospheric observations to budget uncertainties.
Mike J. Newland, Daniel J. Bryant, Rachel E. Dunmore, Thomas J. Bannan, W. Joe F. Acton, Ben Langford, James R. Hopkins, Freya A. Squires, William Dixon, William S. Drysdale, Peter D. Ivatt, Mathew J. Evans, Peter M. Edwards, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, C. Nicholas Hewitt, James D. Lee, Tianqu Cui, Jason D. Surratt, Xinming Wang, Alastair C. Lewis, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 1613–1625, https://doi.org/10.5194/acp-21-1613-2021, https://doi.org/10.5194/acp-21-1613-2021, 2021
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We report the formation of secondary pollutants in the urban megacity of Beijing that are typically associated with remote regions such as rainforests. This is caused by extremely low levels of nitric oxide (NO), typically expected to be high in urban areas, observed in the afternoon. This work has significant implications for how we understand atmospheric chemistry in the urban environment and thus for how to implement effective policies to improve urban air quality.
Swaleha Inamdar, Liselotte Tinel, Rosie Chance, Lucy J. Carpenter, Prabhakaran Sabu, Racheal Chacko, Sarat C. Tripathy, Anvita U. Kerkar, Alok K. Sinha, Parli Venkateswaran Bhaskar, Amit Sarkar, Rajdeep Roy, Tomás Sherwen, Carlos Cuevas, Alfonso Saiz-Lopez, Kirpa Ram, and Anoop S. Mahajan
Atmos. Chem. Phys., 20, 12093–12114, https://doi.org/10.5194/acp-20-12093-2020, https://doi.org/10.5194/acp-20-12093-2020, 2020
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Iodine chemistry is generating a lot of interest because of its impacts on the oxidising capacity of the marine boundary and depletion of ozone. However, one of the challenges has been predicting the right levels of iodine in the models, which depend on parameterisations for emissions from the sea surface. This paper discusses the different parameterisations available and compares them with observations, showing that our current knowledge is still insufficient, especially on a regional scale.
Peter D. Ivatt and Mathew J. Evans
Atmos. Chem. Phys., 20, 8063–8082, https://doi.org/10.5194/acp-20-8063-2020, https://doi.org/10.5194/acp-20-8063-2020, 2020
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We investigate the potential of using a decision tree algorithm to identify and correct the tropospheric ozone bias in a chemical transport model. We train the algorithm on 2010–2015 ground and column observation data and test the algorithm on the 2016–2017 data using the ground data as well as independent flight data. We find the algorithm is successfully able to identify and correct the bias, improving the model performance.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
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.
Ryan J. Pound, Tomás Sherwen, Detlev Helmig, Lucy J. Carpenter, and Mat J. Evans
Atmos. Chem. Phys., 20, 4227–4239, https://doi.org/10.5194/acp-20-4227-2020, https://doi.org/10.5194/acp-20-4227-2020, 2020
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Ozone is an important pollutant with impacts on health and the environment. Ozone is lost to plants, land and the oceans. Loss to the ocean is slow compared to all other types of land cover and has not received as much attention. We build on previous work to more accurately model ozone loss to the ocean. We find changes in the concentration of ozone over the oceans, notably the Southern Ocean, which improves model performance.
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.
Sophie L. Haslett, Jonathan W. Taylor, Mathew Evans, Eleanor Morris, Bernhard Vogel, Alima Dajuma, Joel Brito, Anneke M. Batenburg, Stephan Borrmann, Johannes Schneider, Christiane Schulz, Cyrielle Denjean, Thierry Bourrianne, Peter Knippertz, Régis Dupuy, Alfons Schwarzenböck, Daniel Sauer, Cyrille Flamant, James Dorsey, Ian Crawford, and Hugh Coe
Atmos. Chem. Phys., 19, 15217–15234, https://doi.org/10.5194/acp-19-15217-2019, https://doi.org/10.5194/acp-19-15217-2019, 2019
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Three aircraft datasets from the DACCIWA campaign in summer 2016 are used here to show there is a background mass of pollution present in the lower atmosphere in southern West Africa. We suggest that this likely comes from biomass burning in central and southern Africa, which has been carried into the region over the Atlantic Ocean. This would have a negative health impact on populations living near the coast and may alter the impact of growing city emissions on cloud formation and the monsoon.
Tomás Sherwen, Rosie J. Chance, Liselotte Tinel, Daniel Ellis, Mat J. Evans, and Lucy J. Carpenter
Earth Syst. Sci. Data, 11, 1239–1262, https://doi.org/10.5194/essd-11-1239-2019, https://doi.org/10.5194/essd-11-1239-2019, 2019
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Iodine plays an important role in the Earth system, as a nutrient to the biosphere and by changing the concentrations of climate and air-quality species. However, there are uncertainties on the magnitude of iodine’s role, and a key uncertainty is our understanding of iodide in the global sea-surface. Here we take a data-driven approach using a machine learning algorithm to convert a sparse set of sea-surface iodide observations into a spatially and temporally resolved dataset for use in models.
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.
Christoph A. Keller and Mat J. Evans
Geosci. Model Dev., 12, 1209–1225, https://doi.org/10.5194/gmd-12-1209-2019, https://doi.org/10.5194/gmd-12-1209-2019, 2019
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Computer simulations of atmospheric chemistry are a central tool to study the impact of air pollutants on the environment. These models are highly complex and require a lot of computing resources. In this study we show that machine learning can be used to predict air pollution with an accuracy that is comparable to the traditional, computationally expensive method. Such a machine-learning-based model has the potential to be orders of magnitude faster.
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.
Alba Badia, Claire E. Reeves, Alex R. Baker, Alfonso Saiz-Lopez, Rainer Volkamer, Theodore K. Koenig, Eric C. Apel, Rebecca S. Hornbrook, Lucy J. Carpenter, Stephen J. Andrews, Tomás Sherwen, and Roland von Glasow
Atmos. Chem. Phys., 19, 3161–3189, https://doi.org/10.5194/acp-19-3161-2019, https://doi.org/10.5194/acp-19-3161-2019, 2019
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The oceans have an impact on the composition and reactivity of the troposphere through the emission of gases and particles. Thus, a quantitative understanding of the marine atmosphere is crucial to examine the oxidative capacity and climate forcing. This study investigates the impact of halogens in the tropical troposphere and explores the sensitivity of this to uncertainties in the fluxes and their chemical processing. Our modelled tropospheric Ox loss due to halogens ranges from 20 % to 60 %.
Kate R. Smith, Peter M. Edwards, Peter D. Ivatt, James D. Lee, Freya Squires, Chengliang Dai, Richard E. Peltier, Mat J. Evans, Yele Sun, and Alastair C. Lewis
Atmos. Meas. Tech., 12, 1325–1336, https://doi.org/10.5194/amt-12-1325-2019, https://doi.org/10.5194/amt-12-1325-2019, 2019
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Clusters of low-cost, low-power atmospheric gas sensors were built into a sensor instrument to monitor NO2 and O3 in Beijing, alongside reference instruments, aiming to improve the reliability of sensor measurements. Clustering identical sensors and using the median sensor signal was used to minimize drift over short and medium timescales. Three different machine learning techniques were used for all the sensor data in an attempt to correct for cross-interferences, which worked to some degree.
Federica Pacifico, Claire Delon, Corinne Jambert, Pierre Durand, Eleanor Morris, Mat J. Evans, Fabienne Lohou, Solène Derrien, Venance H. E. Donnou, Arnaud V. Houeto, Irene Reinares Martínez, and Pierre-Etienne Brilouet
Atmos. Chem. Phys., 19, 2299–2325, https://doi.org/10.5194/acp-19-2299-2019, https://doi.org/10.5194/acp-19-2299-2019, 2019
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Biogenic fluxes from soil at a local and regional scale are crucial to study air pollution and climate. Here we present field measurements of soil fluxes of nitric oxide (NO) and ammonia (NH3) observed over four different land cover types, i.e. bare soil, grassland, maize field, and forest, at an inland rural site in Benin, West Africa, during the DACCIWA field campaign in
June and July 2016.
Lu Hu, Christoph A. Keller, Michael S. Long, Tomás Sherwen, Benjamin Auer, Arlindo Da Silva, Jon E. Nielsen, Steven Pawson, Matthew A. Thompson, Atanas L. Trayanov, Katherine R. Travis, Stuart K. Grange, Mat J. Evans, and Daniel J. Jacob
Geosci. Model Dev., 11, 4603–4620, https://doi.org/10.5194/gmd-11-4603-2018, https://doi.org/10.5194/gmd-11-4603-2018, 2018
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We present a full-year online global simulation of tropospheric chemistry at 12.5 km resolution. To the best of our knowledge, such a resolution in a state-of-the-science global simulation of tropospheric chemistry is unprecedented. This simulation will serve as the Nature Run for observing system simulation experiments to support the future geostationary satellite constellation for tropospheric chemistry, and can also be used for various air quality applications.
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.
Mike J. Newland, Andrew R. Rickard, Tomás Sherwen, Mathew J. Evans, Luc Vereecken, Amalia Muñoz, Milagros Ródenas, and William J. Bloss
Atmos. Chem. Phys., 18, 6095–6120, https://doi.org/10.5194/acp-18-6095-2018, https://doi.org/10.5194/acp-18-6095-2018, 2018
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Stabilised Criegee intermediates (SCIs) are formed in the reaction of alkenes with ozone, both of which are ubiquitous throughout the troposphere. We determine the fate and global distribution of SCI from monoterpene ozonolysis. One major fate of SCI is reaction with H2O, but for a fraction of SCIs, unimolecular reactions dominate. Concentrations of SCIs are high enough regionally to play a key role in the conversion of sulfur dioxide to aerosol, affecting air quality and climate.
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.
Daniel Stone, Tomás Sherwen, Mathew J. Evans, Stewart Vaughan, Trevor Ingham, Lisa K. Whalley, Peter M. Edwards, Katie A. Read, James D. Lee, Sarah J. Moller, Lucy J. Carpenter, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 3541–3561, https://doi.org/10.5194/acp-18-3541-2018, https://doi.org/10.5194/acp-18-3541-2018, 2018
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Halogen chemistry in the troposphere impacts oxidising capacity, but model studies assessing the nature of these impacts can vary according to the model framework used. In this work we present simulations of OH and HO2 radicals using both box and global model frameworks, and compare to observations made at the Cape Verde Atmospheric Observatory. We highlight, and rationalise, differences between the model frameworks.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Ben Newsome and Mat Evans
Atmos. Chem. Phys., 17, 14333–14352, https://doi.org/10.5194/acp-17-14333-2017, https://doi.org/10.5194/acp-17-14333-2017, 2017
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We explore the uncertainty in the predictions of a chemical transport model (GEOS-Chem) from uncertainty in 60 inorganic rate constants and photolysis rates. We find uncertainty in the global mean ozone burden of 10 %, in global mean OH of 16 %, methane lifetimes of 16 %, and tropospheric ozone radiative forcings of 13 %. Reductions in the uncertainty of rate constants of these simple reactions would reduce uncertainty in our understanding of atmospheric composition.
Peter M. Edwards and Mathew J. Evans
Atmos. Chem. Phys., 17, 13669–13680, https://doi.org/10.5194/acp-17-13669-2017, https://doi.org/10.5194/acp-17-13669-2017, 2017
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Understanding tropospheric ozone chemistry has been at the centre of the field of atmospheric chemistry for the last 30 years. However, our conceptual approach to diagnosing ozone production in global models has not advanced in this time. Our work presents a new and powerful approach for diagnosing tropospheric ozone production, providing a significant enhancement in our ability to understand the processes controlling ozone and how we can validate our assessment of these processes.
Peter Knippertz, Andreas H. Fink, Adrien Deroubaix, Eleanor Morris, Flore Tocquer, Mat J. Evans, Cyrille Flamant, Marco Gaetani, Christophe Lavaysse, Celine Mari, John H. Marsham, Rémi Meynadier, Abalo Affo-Dogo, Titike Bahaga, Fabien Brosse, Konrad Deetz, Ridha Guebsi, Issaou Latifou, Marlon Maranan, Philip D. Rosenberg, and Andreas Schlueter
Atmos. Chem. Phys., 17, 10893–10918, https://doi.org/10.5194/acp-17-10893-2017, https://doi.org/10.5194/acp-17-10893-2017, 2017
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In June–July 2016 DACCIWA (Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa), a large, EU-funded European–African project, organised an international field campaign in densely populated southern West Africa, including measurements from ground sites, research aircraft, weather balloons and urban sites. This paper gives an overview of the atmospheric evolution during this period focusing on meteorological (precipitation, cloudiness, winds) and composition (gases, particles) aspects.
Chris Reed, Mathew J. Evans, Leigh R. Crilley, William J. Bloss, Tomás Sherwen, Katie A. Read, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 17, 4081–4092, https://doi.org/10.5194/acp-17-4081-2017, https://doi.org/10.5194/acp-17-4081-2017, 2017
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The source of ozone-depleting compounds in the remote troposphere has been thought to be long-range transport of secondary pollutants such as organic nitrates. Processing of organic nitrates to nitric acid and subsequent deposition on surfaces in the atmosphere was thought to remove these nitrates from the ozone–NOx–HOx cycle. We found through observation of NOx in the remote tropical troposphere at the Cape Verde Observatory that surface nitrates can be released back into the atmosphere.
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.
Tomás Sherwen, Johan A. Schmidt, Mat J. Evans, Lucy J. Carpenter, Katja Großmann, Sebastian D. Eastham, Daniel J. Jacob, Barbara Dix, Theodore K. Koenig, Roman Sinreich, Ivan Ortega, Rainer Volkamer, Alfonso Saiz-Lopez, Cristina Prados-Roman, Anoop S. Mahajan, and Carlos Ordóñez
Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, https://doi.org/10.5194/acp-16-12239-2016, 2016
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We present a simulation of tropospheric Cl, Br, I chemistry within the GEOS-Chem CTM. We find a decrease in tropospheric ozone burden of 18.6 % and a 8.2 % decrease in global mean OH concentrations. Cl oxidation of some VOCs range from 15 to 27 % of the total loss. Bromine plays a small role in oxidising oVOCs. Surface ozone, ozone sondes, and methane lifetime are in general improved by the inclusion of halogens. We argue that simulated bromine and chlorine represent a lower limit.
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.
Dene R. Bowdalo, Mathew J. Evans, and Eric D. Sofen
Atmos. Chem. Phys., 16, 8295–8308, https://doi.org/10.5194/acp-16-8295-2016, https://doi.org/10.5194/acp-16-8295-2016, 2016
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We introduce a new methodology for the assessment of atmospheric models with observations. We apply a spectral analysis methodology to hourly ozone observations and the equivalent model output. The spectrally transformed observational data show significant peaks on daily and annual timescales. Comparison between the amplitude and phase of these peaks introduces a new comparison methodology between model and measurements. We find the model shows significant biases on an annual timescale.
Alicia Gressent, Bastien Sauvage, Daniel Cariolle, Mathew Evans, Maud Leriche, Céline Mari, and Valérie Thouret
Atmos. Chem. Phys., 16, 5867–5889, https://doi.org/10.5194/acp-16-5867-2016, https://doi.org/10.5194/acp-16-5867-2016, 2016
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In chemical transport models, NOx emitted by lightning (LNOx) is instantaneously diluted into the grid. A plume-in-grid parameterization to account for the sub-grid chemistry of LNOx is presented. This approach was implemented into the GEOS-Chem model and leads to a relative increase of NOx and O3 (18 % and 2 %, respectively, in July) on a large scale downwind of lightning emissions and a relative decrease (25 % and 8 %, respectively, over central Africa in July) over the regions of emissions.
Chris Reed, Mathew J. Evans, Piero Di Carlo, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 16, 4707–4724, https://doi.org/10.5194/acp-16-4707-2016, https://doi.org/10.5194/acp-16-4707-2016, 2016
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The self-cleaning capacity of the atmosphere in places like Antarctica can be measured by quantifying very low amounts of combustion products that exist in a well-known ratio. When this ratio deviates from 1 it points to the existence of unknown compounds. Several unknown compounds have been theorized to exist but never measured. We have found the method for measuring the ratio of combustion products suffers a bias in remote places, which when taken into account disproves any unknown compounds.
Frank A. F. Winiberg, Terry J. Dillon, Stephanie C. Orr, Christoph B. M Groß, Iustinian Bejan, Charlotte A. Brumby, Matthew J. Evans, Shona C. Smith, Dwayne E. Heard, and Paul W. Seakins
Atmos. Chem. Phys., 16, 4023–4042, https://doi.org/10.5194/acp-16-4023-2016, https://doi.org/10.5194/acp-16-4023-2016, 2016
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OH radicals are important intermediates in the atmosphere, and the high concentrations observed in tropical regions are yet to be fully explained. Radical-radical reactions such as the title reaction can contribute to OH formation. This is the most fully comprehensive study of the CH3C(O)O2 + HO2 reaction with direct observation of products in all reaction channels. The implications of the new measurements on OH, PAN and NOx concentrations are considered via global models.
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.
E. D. Sofen, D. Bowdalo, M. J. Evans, F. Apadula, P. Bonasoni, M. Cupeiro, R. Ellul, I. E. Galbally, R. Girgzdiene, S. Luppo, M. Mimouni, A. C. Nahas, M. Saliba, and K. Tørseth
Earth Syst. Sci. Data, 8, 41–59, https://doi.org/10.5194/essd-8-41-2016, https://doi.org/10.5194/essd-8-41-2016, 2016
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We have brought together all publicly available surface ozone observations from online databases from 1971–2015, with 2200 sites representing regional background conditions appropriate for the evaluation of chemical transport and chemistry-climate models for projects such as the Chemistry-Climate Model Initiative. Gridded data sets of ozone metrics (mean, percentiles, MDA8, SOMO35, etc.) are available from the British Atmospheric Data Centre.
E. D. Sofen, D. Bowdalo, and M. J. Evans
Atmos. Chem. Phys., 16, 1445–1457, https://doi.org/10.5194/acp-16-1445-2016, https://doi.org/10.5194/acp-16-1445-2016, 2016
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We explore the global representativeness of a global surface ozone data set from a range of perspectives (area, biomes, chemical regimes, model uncertainty, model trends). We conclude that the current network fails to provide sufficient constraints for important regions/regimes, leading to uncertainty for a range of atmospheric composition challenges. We suggest 20 new locations for making surface ozone observations, which would significantly enhance our observational capability.
T. Sherwen, M. J. Evans, L. J. Carpenter, S. J. Andrews, R. T. Lidster, B. Dix, T. K. Koenig, R. Sinreich, I. Ortega, R. Volkamer, A. Saiz-Lopez, C. Prados-Roman, A. S. Mahajan, and C. Ordóñez
Atmos. Chem. Phys., 16, 1161–1186, https://doi.org/10.5194/acp-16-1161-2016, https://doi.org/10.5194/acp-16-1161-2016, 2016
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Using a global chemical transport model (GEOS-Chem) with additional iodine emissions, chemistry, and deposition we show that iodine is responsible for ~ 9 % of global ozone loss but has negligible impacts on global OH. Uncertainties are large in the chemistry and emissions and future research is needed in both. Measurements of iodine species (especially HOI) would be useful. We believe iodine chemistry should be considered in future chemistry-climate and in air quality modelling.
S. Walter, A. Kock, T. Steinhoff, B. Fiedler, P. Fietzek, J. Kaiser, M. Krol, M. E. Popa, Q. Chen, T. Tanhua, and T. Röckmann
Biogeosciences, 13, 323–340, https://doi.org/10.5194/bg-13-323-2016, https://doi.org/10.5194/bg-13-323-2016, 2016
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Oceans are a source of H2, an indirect greenhouse gas. Measurements constraining the temporal and spatial patterns of oceanic H2 emissions are sparse and although H2 is assumed to be produced mainly biologically, direct evidence for biogenic marine production was lacking. By analyzing the H2 isotopic composition (δD) we were able to constrain the global H2 budget in more detail, verify biogenic production and point to additional sources. We also showed that current models are reasonably working.
E. D. Sofen, M. J. Evans, and A. C. Lewis
Atmos. Chem. Phys., 15, 13627–13632, https://doi.org/10.5194/acp-15-13627-2015, https://doi.org/10.5194/acp-15-13627-2015, 2015
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As an air pollutant, O3 is monitored photometrically to assess compliance with air quality legislation. A recent study found a 1.8% reduction in its absorption cross section, which would lead to an equivalent increase in observed O3 concentrations. We estimate this would increase the number of sites out of compliance with air quality regulations in the EU and US by 20%. We draw attention to how small changes in gas metrology impacts attainment and compliance with legal air quality standards.
Q. Chen, M. E. Popa, A. M. Batenburg, and T. Röckmann
Atmos. Chem. Phys., 15, 13003–13021, https://doi.org/10.5194/acp-15-13003-2015, https://doi.org/10.5194/acp-15-13003-2015, 2015
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We investigated soil production and uptake of H2 and associated isotope effects. Uptake and emission of H2 occurred simultaneously at all sampling sites, with strongest emission where N2 fixing legume was present. The fractionation constant during soil uptake was about 0.945 and it did not show positive correlation with deposition velocity. The isotopic composition of H2 emitted from soil with legume was about -530‰, which is less deuterium-depleted than isotope equilibrium between H2O and H2.
R. E. Dunmore, J. R. Hopkins, R. T. Lidster, J. D. Lee, M. J. Evans, A. R. Rickard, A. C. Lewis, and J. F. Hamilton
Atmos. Chem. Phys., 15, 9983–9996, https://doi.org/10.5194/acp-15-9983-2015, https://doi.org/10.5194/acp-15-9983-2015, 2015
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Technological shifts between fuel sources have had unexpected impacts on atmospheric composition and these significant changes can go undetected if source-specific monitoring infrastructure is not in place. We present chemically comprehensive, continuous measurements of organic compounds in a developed megacity (London), that show diesel-related hydrocarbons can dominate reactive carbon and ozone formation potential, highlighting a serious underestimation of this source in emission inventories.
H. M. Walker, D. Stone, T. Ingham, S. Vaughan, M. Cain, R. L. Jones, O. J. Kennedy, M. McLeod, B. Ouyang, J. Pyle, S. Bauguitte, B. Bandy, G. Forster, M. J. Evans, J. F. Hamilton, J. R. Hopkins, J. D. Lee, A. C. Lewis, R. T. Lidster, S. Punjabi, W. T. Morgan, and D. E. Heard
Atmos. Chem. Phys., 15, 8179–8200, https://doi.org/10.5194/acp-15-8179-2015, https://doi.org/10.5194/acp-15-8179-2015, 2015
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.
L. K. Whalley, D. Stone, I. J. George, S. Mertes, D. van Pinxteren, A. Tilgner, H. Herrmann, M. J. Evans, and D. E. Heard
Atmos. Chem. Phys., 15, 3289–3301, https://doi.org/10.5194/acp-15-3289-2015, https://doi.org/10.5194/acp-15-3289-2015, 2015
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.
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
L. T. Murray, L. J. Mickley, J. O. Kaplan, E. D. Sofen, M. Pfeiffer, and B. Alexander
Atmos. Chem. Phys., 14, 3589–3622, https://doi.org/10.5194/acp-14-3589-2014, https://doi.org/10.5194/acp-14-3589-2014, 2014
D. Stone, M. J. Evans, H. Walker, T. Ingham, S. Vaughan, B. Ouyang, O. J. Kennedy, M. W. McLeod, R. L. Jones, J. Hopkins, S. Punjabi, R. Lidster, J. F. Hamilton, J. D. Lee, A. C. Lewis, L. J. Carpenter, G. Forster, D. E. Oram, C. E. Reeves, S. Bauguitte, W. Morgan, H. Coe, E. Aruffo, C. Dari-Salisburgo, F. Giammaria, P. Di Carlo, and D. E. Heard
Atmos. Chem. Phys., 14, 1299–1321, https://doi.org/10.5194/acp-14-1299-2014, https://doi.org/10.5194/acp-14-1299-2014, 2014
P. M. Edwards, M. J. Evans, K. L. Furneaux, J. Hopkins, T. Ingham, C. Jones, J. D. Lee, A. C. Lewis, S. J. Moller, D. Stone, L. K. Whalley, and D. E. Heard
Atmos. Chem. Phys., 13, 9497–9514, https://doi.org/10.5194/acp-13-9497-2013, https://doi.org/10.5194/acp-13-9497-2013, 2013
J. R. Pierce, M. J. Evans, C. E. Scott, S. D. D'Andrea, D. K. Farmer, E. Swietlicki, and D. V. Spracklen
Atmos. Chem. Phys., 13, 3163–3176, https://doi.org/10.5194/acp-13-3163-2013, https://doi.org/10.5194/acp-13-3163-2013, 2013
A. C. Lewis, M. J. Evans, J. R. Hopkins, S. Punjabi, K. A. Read, R. M. Purvis, S. J. Andrews, S. J. Moller, L. J. Carpenter, J. D. Lee, A. R. Rickard, P. I. Palmer, and M. Parrington
Atmos. Chem. Phys., 13, 851–867, https://doi.org/10.5194/acp-13-851-2013, https://doi.org/10.5194/acp-13-851-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Dimethyl sulfide chemistry over the industrial era: comparison of key oxidation mechanisms and long-term observations
Driving factors of aerosol acidity: a new hierarchical quantitative analysis framework and its application in Changzhou, China
Understanding the long-term trend of organic aerosol and the influences from anthropogenic emission and regional climate change in China
Population exposure to outdoor NO2, black carbon, and ultrafine and fine particles over Paris with multi-scale modelling down to the street scale
Predicted impacts of heterogeneous chemical pathways on particulate sulfur over Fairbanks (Alaska), the Northern Hemisphere, and the Contiguous United States
Critical load exceedances for North America and Europe using an ensemble of models and an investigation of causes of environmental impact estimate variability: an AQMEII4 study
Impacts of meteorology and emission reductions on haze pollution during the lockdown in the North China Plain
Impact of mineral dust on the global nitrate aerosol direct and indirect radiative effect
The surface tension and cloud condensation nuclei (CCN) activation of sea spray aerosol particles
Exploring the processes controlling secondary inorganic aerosol: evaluating the global GEOS-Chem simulation using a suite of aircraft campaigns
Influence of land cover change on atmospheric organic gases, aerosols, and radiative effects
Quantifying the impacts of marine aerosols over the southeast Atlantic Ocean using a chemical transport model: implications for aerosol–cloud interactions
Quantifying the impact of global nitrate aerosol on tropospheric composition fields and its production from lightning NOx
Rapid oxidation of phenolic compounds by O3 and HO●: effects of the air–water interface and mineral dust in tropospheric chemical processes
Uncertainties in the effects of organic aerosol coatings on polycyclic aromatic hydrocarbon concentrations and their estimated health effects
Modeling the contribution of leads to sea spray aerosol in the high Arctic
Trends and Drivers of Soluble Iron Deposition from East Asian Dust to the Northwest Pacific: A Springtime Analysis (2001–2017)
Impacts of Sea Ice Leads on Sea Salt Aerosols and Atmospheric Chemistry in the Arctic
Implications of Reduced-Complexity Aerosol Thermodynamics on Organic Aerosol Mass Concentration and Composition over North America
Importance of aerosol composition and aerosol vertical profiles in global spatial variation in the relationship between PM2.5 and aerosol optical depth
The co-benefits of a low-carbon future for PM2.5 and O3 air pollution in Europe
Assessing the effectiveness of SO2, NOx, and NH3 emission reductions in mitigating winter PM2.5 in Taiwan using CMAQ
Modelling of atmospheric concentrations of fungal spores: a 2-year simulation over France using CHIMERE
Cluster-dynamics-based parameterization for sulfuric acid–dimethylamine nucleation: comparison and selection through box and three-dimensional modeling
A Comprehensive Global Modelling Assessment of Nitrate Heterogeneous Formation on Desert Dust
Modelling of atmospheric variability of gas and aerosols during the ACROSS campaign 2022 in the greater Paris area: evaluation of the meteorology, dynamics and chemistry
Observed and CMIP6-model-simulated organic aerosol response to drought in the contiguous United States during summertime
Long-term trends in aerosol properties derived from AERONET measurements
Cooling radiative forcing effect enhancement of atmospheric amines and mineral particles caused by heterogeneous uptake and oxidation
Source-resolved atmospheric metal emissions, concentrations, and deposition fluxes into the East Asian seas
Analysis of secondary inorganic aerosols over the greater Athens area using the EPISODE–CityChem source dispersion and photochemistry model
Global estimates of ambient reactive nitrogen components during 2000–2100 based on the multi-stage model
The role of naphthalene and its derivatives in the formation of secondary organic aerosol in the Yangtze River Delta region, China
Unveiling the optimal regression model for source apportionment of the oxidative potential of PM10
AERO-MAP: A data compilation and modelling approach to understand spatial variability in fine and coarse mode aerosol composition
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying preexisting particles – Part 2: Modeling chemical drivers and 3-D new particle formation occurrence
Technical note: Influence of different averaging metrics and temporal resolutions on the aerosol pH calculated by thermodynamic modeling
Dual roles of the inorganic aqueous phase on secondary organic aerosol growth from benzene and phenol
Global source apportionment of aerosols into major emission regions and sectors over 1850–2017
Modeling atmospheric brown carbon in the GISS ModelE Earth system model
Observation-constrained kinetic modeling of isoprene SOA formation in the atmosphere
Significant impact of urban tree biogenic emissions on air quality estimated by a bottom-up inventory and chemistry transport modeling
Secondary organic aerosols derived from intermediate-volatility n-alkanes adopt low-viscous phase state
Spatial-temporal patterns of anthropogenic and biomass burning contributions on air pollution and mortality burden changes in India from 1995 to 2014
Modeling the drivers of fine PM pollution over Central Europe: impacts and contributions of emissions from different sources
Reaction of SO3 with H2SO4 and its implications for aerosol particle formation in the gas phase and at the air–water interface
Weakened aerosol–radiation interaction exacerbating ozone pollution in eastern China since China's clean air actions
Uncertainties from biomass burning aerosols in air quality models obscure public health impacts in Southeast Asia
Oxidative potential apportionment of atmospheric PM1: a new approach combining high-sensitive online analysers for chemical composition and offline OP measurement technique
Aqueous-phase chemistry of glyoxal with multifunctional reduced nitrogen compounds: a potential missing route for secondary brown carbon
Ursula A. Jongebloed, Jacob I. Chalif, Linia Tashmim, William C. Porter, Kelvin H. Bates, Qianjie Chen, Erich C. Osterberg, Bess G. Koffman, Jihong Cole-Dai, Dominic A. Winski, David G. Ferris, Karl J. Kreutz, Cameron P. Wake, and Becky Alexander
Atmos. Chem. Phys., 25, 4083–4106, https://doi.org/10.5194/acp-25-4083-2025, https://doi.org/10.5194/acp-25-4083-2025, 2025
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Marine phytoplankton emit dimethyl sulfide (DMS), which forms methanesulfonic acid (MSA) and sulfate. MSA concentrations in ice cores decreased over the industrial era, which has been attributed to pollution-driven changes in DMS chemistry. We use a model to investigate DMS chemistry compared to observations of DMS, MSA, and sulfate. We find that modeled DMS, MSA, and sulfate are influenced by pollution-sensitive oxidant concentrations, characterization of DMS chemistry, and other variables.
Xiaolin Duan, Guangjie Zheng, Chuchu Chen, Qiang Zhang, and Kebin He
Atmos. Chem. Phys., 25, 3919–3928, https://doi.org/10.5194/acp-25-3919-2025, https://doi.org/10.5194/acp-25-3919-2025, 2025
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Aerosol acidity is an important parameter in atmospheric chemistry, while its driving factors, especially chemical profiles versus meteorological conditions, are not yet fully understood. Here, we established a hierarchical quantitative analysis framework to understand the driving factors of aerosol acidity on different timescales. Its application in Changzhou, China, revealed distinct driving factors and corresponding mechanisms of aerosol acidity from annual trends to random residuals.
Wenxin Zhang, Yaman Liu, Man Yue, Xinyi Dong, Kan Huang, and Minghuai Wang
Atmos. Chem. Phys., 25, 3857–3872, https://doi.org/10.5194/acp-25-3857-2025, https://doi.org/10.5194/acp-25-3857-2025, 2025
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Understanding long-term organic aerosol (OA) trends and their driving factors is important for air quality management. Our modeling revealed that OA in China increased by 5.6 % from 1990 to 2019, primarily due to a 32.3 % increase in secondary organic aerosols (SOAs) and an 8.1 % decrease in primary organic aerosols (POAs), both largely driven by changes in anthropogenic emissions. Biogenic SOA increased due to warming but showed little response to changes in anthropogenic nitrogen oxide emissions.
Soo-Jin Park, Lya Lugon, Oscar Jacquot, Youngseob Kim, Alexia Baudic, Barbara D'Anna, Ludovico Di Antonio, Claudia Di Biagio, Fabrice Dugay, Olivier Favez, Véronique Ghersi, Aline Gratien, Julien Kammer, Jean-Eudes Petit, Olivier Sanchez, Myrto Valari, Jérémy Vigneron, and Karine Sartelet
Atmos. Chem. Phys., 25, 3363–3387, https://doi.org/10.5194/acp-25-3363-2025, https://doi.org/10.5194/acp-25-3363-2025, 2025
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To accurately represent the population exposure to outdoor concentrations of pollutants of interest to health (NO2, PM2.5, black carbon, and ultrafine particles), multi-scale modelling down to the street scale is set up and evaluated using measurements from field campaigns. An exposure scaling factor is defined, allowing regional-scale simulations to be corrected to evaluate population exposure. Urban heterogeneities strongly influence NO2, black carbon, and ultrafine particles but less strongly PM2.5.
Sara L. Farrell, Havala O. T. Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, Fengkui Duan, Tao Ma, Shuping Zhang, and Kathleen Fahey
Atmos. Chem. Phys., 25, 3287–3312, https://doi.org/10.5194/acp-25-3287-2025, https://doi.org/10.5194/acp-25-3287-2025, 2025
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In this work we implement heterogeneous sulfur chemistry into the Community Multiscale Air Quality (CMAQ) model. This new chemistry accounts for the formation of sulfate via aqueous oxidation of SO2 in aerosol liquid water and the formation of hydroxymethanesulfonate (HMS) – often confused by measurement techniques as sulfate. Model performance in predicting sulfur PM2.5 in Fairbanks, Alaska, and other places that experience dark and cold winters is improved.
Paul A. Makar, Philip Cheung, Christian Hogrefe, Ayodeji Akingunola, Ummugulsum Alyuz, Jesse O. Bash, Michael D. Bell, Roberto Bellasio, Roberto Bianconi, Tim Butler, Hazel Cathcart, Olivia E. Clifton, Alma Hodzic, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Jason A. Lynch, Kester Momoh, Juan L. Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Thomas Scheuschner, Mark W. Shephard, Ranjeet S. Sokhi, and Stefano Galmarini
Atmos. Chem. Phys., 25, 3049–3107, https://doi.org/10.5194/acp-25-3049-2025, https://doi.org/10.5194/acp-25-3049-2025, 2025
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The large range of sulfur and nitrogen deposition estimates from air quality models results in a large range of predicted impacts. We used models and deposition diagnostics to identify the processes controlling atmospheric sulfur and nitrogen deposition variability. Controlling factors included the uptake of gases and aerosols by hydrometeors, aerosol inorganic chemistry, particle dry deposition, ammonia bidirectional fluxes, gas deposition via plant cuticles and soil, and land use data.
Lang Liu, Xin Long, Yi Li, Zengliang Zang, Fengwen Wang, Yan Han, Zhier Bao, Yang Chen, Tian Feng, and Jinxin Yang
Atmos. Chem. Phys., 25, 1569–1585, https://doi.org/10.5194/acp-25-1569-2025, https://doi.org/10.5194/acp-25-1569-2025, 2025
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This study uses WRF-Chem to assess how meteorological conditions and emission reductions affected fine particulate matter (PM2.5) in the North China Plain (NCP). It highlights regional disparities: in the northern NCP, adverse weather negated emission reduction effects. In contrast, the southern NCP featured a PM2.5 decrease due to favorable weather and emission reductions. The research highlighted the interaction between emissions, meteorology, and PM2.5.
Alexandros Milousis, Klaus Klingmüller, Alexandra P. Tsimpidi, Jasper F. Kok, Maria Kanakidou, Athanasios Nenes, and Vlassis A. Karydis
Atmos. Chem. Phys., 25, 1333–1351, https://doi.org/10.5194/acp-25-1333-2025, https://doi.org/10.5194/acp-25-1333-2025, 2025
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This study investigates the impact of dust on the global radiative effect of nitrate aerosols. The results indicate both positive and negative regional shortwave and longwave radiative effects due to aerosol–radiation interactions and cloud adjustments. The global average net REari and REaci of nitrate aerosols are −0.11 and +0.17 W m−2, respectively, mainly affecting the shortwave spectrum. Sensitivity simulations evaluated the influence of mineral dust composition and emissions on the results.
Judith Kleinheins, Nadia Shardt, Ulrike Lohmann, and Claudia Marcolli
Atmos. Chem. Phys., 25, 881–903, https://doi.org/10.5194/acp-25-881-2025, https://doi.org/10.5194/acp-25-881-2025, 2025
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We model the cloud condensation nuclei (CCN) activation of sea spray aerosol particles with classical Köhler theory and with a new model approach that takes surface tension lowering into account. We categorize organic compounds into weak, intermediate, and strong surfactants, and we outline for which composition surface tension lowering is important. The results suggest that surface tension lowering allows sea spray aerosol particles in the Aitken mode to be a source of CCN in marine updraughts.
Olivia G. Norman, Colette L. Heald, Solomon Bililign, Pedro Campuzano-Jost, Hugh Coe, Marc N. Fiddler, Jaime R. Green, Jose L. Jimenez, Katharina Kaiser, Jin Liao, Ann M. Middlebrook, Benjamin A. Nault, John B. Nowak, Johannes Schneider, and André Welti
Atmos. Chem. Phys., 25, 771–795, https://doi.org/10.5194/acp-25-771-2025, https://doi.org/10.5194/acp-25-771-2025, 2025
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This study finds that one component of secondary inorganic aerosols, nitrate, is greatly overestimated by a global atmospheric chemistry model compared to observations from 11 flight campaigns. None of the loss and production pathways explored can explain the nitrate bias alone. The model’s inability to capture the variability in the observations remains and requires future investigation to avoid biases in policy-related studies (i.e., air quality, health, climate impacts of these aerosols).
Ryan Vella, Matthew Forrest, Andrea Pozzer, Alexandra P. Tsimpidi, Thomas Hickler, Jos Lelieveld, and Holger Tost
Atmos. Chem. Phys., 25, 243–262, https://doi.org/10.5194/acp-25-243-2025, https://doi.org/10.5194/acp-25-243-2025, 2025
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This study examines how land cover changes influence biogenic volatile organic compound (BVOC) emissions and atmospheric states. Using a coupled chemistry–climate–vegetation model, we compare present-day land cover (deforested for crops and grazing) with natural vegetation and an extreme reforestation scenario. We find that vegetation changes significantly impact global BVOC emissions and organic aerosols but have a relatively small effect on total aerosols, clouds, and radiative effects.
Mashiat Hossain, Rebecca M. Garland, and Hannah M. Horowitz
Atmos. Chem. Phys., 24, 14123–14143, https://doi.org/10.5194/acp-24-14123-2024, https://doi.org/10.5194/acp-24-14123-2024, 2024
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Our research examines aerosol dynamics over the southeast Atlantic, a region with significant uncertainties in aerosol radiative forcings. Using the GEOS-Chem model, we find that at cloud altitudes, organic aerosols dominate during the biomass burning season, while sulfate aerosols, driven by marine emissions, prevail during peak primary production. These findings highlight the need for accurate representation of marine aerosols in models to improve climate predictions and reduce uncertainties.
Ashok K. Luhar, Anthony C. Jones, and Jonathan M. Wilkinson
Atmos. Chem. Phys., 24, 14005–14028, https://doi.org/10.5194/acp-24-14005-2024, https://doi.org/10.5194/acp-24-14005-2024, 2024
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Nitrate aerosol is often omitted in global chemistry–climate models, partly due to the chemical complexity of its formation process. Using a global model, we show that including nitrate aerosol significantly impacts tropospheric composition fields, such as ozone, and radiation. Additionally, lightning-generated oxides of nitrogen influence both nitrate aerosol mass concentrations and aerosol size distribution, which has important implications for radiative fluxes and indirect aerosol effects.
Yanru Huo, Mingxue Li, Xueyu Wang, Jianfei Sun, Yuxin Zhou, Yuhui Ma, and Maoxia He
Atmos. Chem. Phys., 24, 12409–12423, https://doi.org/10.5194/acp-24-12409-2024, https://doi.org/10.5194/acp-24-12409-2024, 2024
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This work found that the air–water (A–W) interface and TiO2 clusters promote the oxidation of phenolic compounds (PhCs) to varying degrees compared with the gas phase and bulk water. Some byproducts are more harmful than their parent compounds. This work provides important evidence for the rapid oxidation observed in O3/HO• + PhC experiments at the A–W interface and in mineral dust.
Sijia Lou, Manish Shrivastava, Alexandre Albinet, Sophie Tomaz, Deepchandra Srivastava, Olivier Favez, Huizhong Shen, and Aijun Ding
EGUsphere, https://doi.org/10.5194/egusphere-2024-3269, https://doi.org/10.5194/egusphere-2024-3269, 2024
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PAHs, emitted from incomplete combustion, pose serious health risks due to their carcinogenic properties. This research demonstrates that viscous organic aerosol coatings significantly hinder PAH oxidation, with spatial distributions sensitive to the degradation modelling approach. Our findings underscore the importance of accurately modelling these processes for risk assessments, highlighting the need to consider both fresh and oxidized PAHs in evaluating human exposure and health risks.
Rémy Lapere, Louis Marelle, Pierre Rampal, Laurent Brodeau, Christian Melsheimer, Gunnar Spreen, and Jennie L. Thomas
Atmos. Chem. Phys., 24, 12107–12132, https://doi.org/10.5194/acp-24-12107-2024, https://doi.org/10.5194/acp-24-12107-2024, 2024
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Elongated open-water areas in sea ice, called leads, can release marine aerosols into the atmosphere. In the Arctic, this source of atmospheric particles could play an important role for climate. However, the amount, seasonality and spatial distribution of such emissions are all mostly unknown. Here, we propose a first parameterization for sea spray aerosols emitted through leads in sea ice and quantify their impact on aerosol populations in the high Arctic.
Hanzheng Zhu, Yaman Liu, Man Yue, Shihui Feng, Pingqing Fu, Kan Huang, Xinyi Dong, and Minghuai Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2293, https://doi.org/10.5194/egusphere-2024-2293, 2024
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Dust soluble iron deposition from East Asia plays an important role in the marine ecology of the Northwest Pacific. Using the developed model, our findings highlight a dual trend: a decrease in the overall deposition of soluble iron from dust, but an increase in the solubility of the iron itself due to the enhanced atmospheric processing. It underscores the critical roles of both dust emission and atmospheric processing in soluble iron deposition and marine ecology.
Erin Emme and Hannah Horowitz
EGUsphere, https://doi.org/10.5194/egusphere-2024-3147, https://doi.org/10.5194/egusphere-2024-3147, 2024
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There is uncertainty in the sources of Arctic cold season (November-April) sea salt aerosols. Using a chemical transport model and satellite observations, we quantify Arctic-wide sea salt aerosol emissions from fractures in sea ice, called open sea ice leads, and their atmospheric chemistry impacts for the cold season. We show sea ice leads contribute to Arctic sea salt aerosols and bromine, especially in under-observed regions.
Camilo Serrano Damha, Kyle Gorkowski, and Andreas Zuend
EGUsphere, https://doi.org/10.5194/egusphere-2024-2712, https://doi.org/10.5194/egusphere-2024-2712, 2024
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Organic aerosol water content impacts the gas–particle partitioning of semivolatile organics. We used an aerosol thermodynamic model in the GEOS-Chem chemical transport model to efficiently account for organic aerosol water uptake and nonideal mixing. This led to a substantial enhancement in mean organic aerosol mass concentration with respect to GEOS-Chem's most advanced scheme. The water-sensitive scheme could be a valuable tool for reconciling model estimations and field measurements.
Haihui Zhu, Randall V. Martin, Aaron van Donkelaar, Melanie S. Hammer, Chi Li, Jun Meng, Christopher R. Oxford, Xuan Liu, Yanshun Li, Dandan Zhang, Inderjeet Singh, and Alexei Lyapustin
Atmos. Chem. Phys., 24, 11565–11584, https://doi.org/10.5194/acp-24-11565-2024, https://doi.org/10.5194/acp-24-11565-2024, 2024
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Ambient fine particulate matter (PM2.5) contributes to 4 million deaths globally each year. Satellite remote sensing of aerosol optical depth (AOD), coupled with a simulated PM2.5–AOD relationship (η), can provide global PM2.5 estimations. This study aims to understand the spatial patterns and driving factors of η to guide future measurement and modeling efforts. We quantified η globally and regionally and found that its spatial variation is strongly influenced by aerosol composition.
Connor J. Clayton, Daniel R. Marsh, Steven T. Turnock, Ailish M. Graham, Kirsty J. Pringle, Carly L. Reddington, Rajesh Kumar, and James B. McQuaid
Atmos. Chem. Phys., 24, 10717–10740, https://doi.org/10.5194/acp-24-10717-2024, https://doi.org/10.5194/acp-24-10717-2024, 2024
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We demonstrate that strong climate mitigation could improve air quality in Europe; however, less ambitious mitigation does not result in these co-benefits. We use a high-resolution atmospheric chemistry model. This allows us to demonstrate how this varies across European countries and analyse the underlying chemistry. This may help policy-facing researchers understand which sectors and regions need to be prioritised to achieve strong air quality co-benefits of climate mitigation.
Ping-Chieh Huang, Hui-Ming Hung, Hsin-Chih Lai, and Charles C.-K. Chou
Atmos. Chem. Phys., 24, 10759–10772, https://doi.org/10.5194/acp-24-10759-2024, https://doi.org/10.5194/acp-24-10759-2024, 2024
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Models were used to study ways to reduce particulate matter (PM) pollution in Taiwan during winter. After considering various factors, such as physical processes and chemical reactions, we found that reducing NOx or NH3 emissions is more effective at mitigating PM2.5 than reducing SO2 emissions. When considering both efficiency and cost, reducing NH3 emissions seems to be a more suitable policy for the studied environment in Taiwan.
Matthieu Vida, Gilles Foret, Guillaume Siour, Florian Couvidat, Olivier Favez, Gaelle Uzu, Arineh Cholakian, Sébastien Conil, Matthias Beekmann, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 24, 10601–10615, https://doi.org/10.5194/acp-24-10601-2024, https://doi.org/10.5194/acp-24-10601-2024, 2024
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We simulate 2 years of atmospheric fungal spores over France and use observations of polyols and primary biogenic factors from positive matrix factorisation. The representation of emissions taking into account a proxy for vegetation surface and specific humidity enables us to reproduce very accurately the seasonal cycle of fungal spores. Furthermore, we estimate that fungal spores can account for 20 % of PM10 and 40 % of the organic fraction of PM10 over vegetated areas in summer.
Jiewen Shen, Bin Zhao, Shuxiao Wang, An Ning, Yuyang Li, Runlong Cai, Da Gao, Biwu Chu, Yang Gao, Manish Shrivastava, Jingkun Jiang, Xiuhui Zhang, and Hong He
Atmos. Chem. Phys., 24, 10261–10278, https://doi.org/10.5194/acp-24-10261-2024, https://doi.org/10.5194/acp-24-10261-2024, 2024
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We extensively compare various cluster-dynamics-based parameterizations for sulfuric acid–dimethylamine nucleation and identify a newly developed parameterization derived from Atmospheric Cluster Dynamic Code (ACDC) simulations as being the most reliable one. This study offers a valuable reference for developing parameterizations of other nucleation systems and is meaningful for the accurate quantification of the environmental and climate impacts of new particle formation.
Rubén Soussé-Villa, Oriol Jorba, María Gonçalves Ageitos, Dene Bowdalo, Marc Guevara, and Carlos Pérez García-Pando
EGUsphere, https://doi.org/10.5194/egusphere-2024-2310, https://doi.org/10.5194/egusphere-2024-2310, 2024
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Desert dust forms nitrate coatings as it travels through the atmosphere. However, current models that predict this process vary greatly due to different methods and inaccuracies. We examined how nitrate forms in a global model, focusing on how gases condense on dust, the lifespan of different particles, and the impact of alkalinity. Our findings show that models work best when they consider reversible gas condensation with alkalinity. This should lead to better estimates of climate impacts.
Ludovico Di Antonio, Matthias Beekmann, Guillaume Siour, Vincent Michoud, Christopher Cantrell, Astrid Bauville, Antonin Bergé, Mathieu Cazaunau, Servanne Chevaillier, Manuela Cirtog, Joel F. de Brito, Paola Formenti, Cecile Gaimoz, Olivier Garret, Aline Gratien, Valérie Gros, Martial Haeffelin, Lelia N. Hawkins, Simone Kotthaus, Gael Noyalet, Diana Pereira, Jean-Eudes Petit, Eva Drew Pronovost, Véronique Riffault, Chenjie Yu, Gilles Foret, Jean-François Doussin, and Claudia Di Biagio
EGUsphere, https://doi.org/10.5194/egusphere-2024-2175, https://doi.org/10.5194/egusphere-2024-2175, 2024
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Summer 2022 has been considered a proxy for future climate scenarios, given the registered hot and dry conditions. In this paper, we used the measurements from the ACROSS campaign, occurred over the Paris area in June–July 2022, in addition to observations from existing networks, to evaluate the WRF–CHIMERE model simulation over France and the Ile-de-France regions. Results over the Ile–de–France show to be satisfactory, allowing to explain the gas and aerosol variability at the ACROSS sites.
Wei Li and Yuxuan Wang
Atmos. Chem. Phys., 24, 9339–9353, https://doi.org/10.5194/acp-24-9339-2024, https://doi.org/10.5194/acp-24-9339-2024, 2024
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Droughts immensely increased organic aerosol (OA) in the contiguous United States in summer (1998–2019), notably in the Pacific Northwest (PNW) and Southeast (SEUS). The OA rise in the SEUS is driven by the enhanced formation of epoxydiol-derived secondary organic aerosol due to the increase in biogenic volatile organic compounds and sulfate, while in the PNW, it is caused by wildfires. A total of 10 climate models captured the OA increase in the PNW yet greatly underestimated it in the SEUS.
Zhenyu Zhang, Jing Li, Huizheng Che, Yueming Dong, Oleg Dubovik, Thomas Eck, Pawan Gupta, Brent Holben, Jhoon Kim, Elena Lind, Trailokya Saud, Sachchida Nand Tripathi, and Tong Ying
EGUsphere, https://doi.org/10.5194/egusphere-2024-2533, https://doi.org/10.5194/egusphere-2024-2533, 2024
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We used ground-based remote sensing data from the Aerosol Robotic Network to examine long-term trends in aerosol characteristics. We found aerosol loadings generally decreased globally, and aerosols became more scattering. These changes are closely related to variations in aerosol compositions, such as decreased anthropogenic emissions over East Asia, Europe, and North America, increased anthropogenic source over North India, increased dust activities over the Arabian Peninsula, etc.
Weina Zhang, Jianhua Mai, Zhichao Fan, Yongpeng Ji, Yuemeng Ji, Guiying Li, Yanpeng Gao, and Taicheng An
Atmos. Chem. Phys., 24, 9019–9030, https://doi.org/10.5194/acp-24-9019-2024, https://doi.org/10.5194/acp-24-9019-2024, 2024
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This study reveals heterogeneous oxidation causes further radiative forcing effect (RFE) enhancement of amine–mineral mixed particles. Note that RFE increment is higher under clean conditions than that under polluted conditions, which is contributed to high-oxygen-content products. The enhanced RFE of amine–mineral particles caused by heterogenous oxidation is expected to alleviate warming effects.
Shenglan Jiang, Yan Zhang, Guangyuan Yu, Zimin Han, Junri Zhao, Tianle Zhang, and Mei Zheng
Atmos. Chem. Phys., 24, 8363–8381, https://doi.org/10.5194/acp-24-8363-2024, https://doi.org/10.5194/acp-24-8363-2024, 2024
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This study aims to provide gridded data on sea-wide concentrations, deposition fluxes, and soluble deposition fluxes with detailed source categories of metals using the modified CMAQ model. We developed a monthly emission inventory of six metals – Fe, Al, V, Ni, Zn, and Cu – from terrestrial anthropogenic, ship, and dust sources in East Asia in 2017. Our results reveal the contribution of each source to the emissions, concentrations, and deposition fluxes of metals in the East Asian seas.
Stelios Myriokefalitakis, Matthias Karl, Kim A. Weiss, Dimitris Karagiannis, Eleni Athanasopoulou, Anastasia Kakouri, Aikaterini Bougiatioti, Eleni Liakakou, Iasonas Stavroulas, Georgios Papangelis, Georgios Grivas, Despina Paraskevopoulou, Orestis Speyer, Nikolaos Mihalopoulos, and Evangelos Gerasopoulos
Atmos. Chem. Phys., 24, 7815–7835, https://doi.org/10.5194/acp-24-7815-2024, https://doi.org/10.5194/acp-24-7815-2024, 2024
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A state-of-the-art thermodynamic model has been coupled with the city-scale chemistry transport model EPISODE–CityChem to investigate the equilibrium between the inorganic gas and aerosol phases over the greater Athens area, Greece. The simulations indicate that the formation of nitrates in an urban environment is significantly affected by local nitrogen oxide emissions, as well as ambient temperature, relative humidity, photochemical activity, and the presence of non-volatile cations.
Rui Li, Yining Gao, Lijia Zhang, Yubing Shen, Tianzhao Xu, Wenwen Sun, and Gehui Wang
Atmos. Chem. Phys., 24, 7623–7636, https://doi.org/10.5194/acp-24-7623-2024, https://doi.org/10.5194/acp-24-7623-2024, 2024
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A three-stage model was developed to obtain the global maps of reactive nitrogen components during 2000–2100. The results implied that cross-validation R2 values of four species showed satisfactory performance (R2 > 0.55). Most reactive nitrogen components, except NH3, in China showed increases during 2000–2013. In the future scenarios, SSP3-7.0 (traditional-energy scenario) and SSP1-2.6 (carbon neutrality scenario) showed the highest and lowest reactive nitrogen component concentrations.
Fei Ye, Jingyi Li, Yaqin Gao, Hongli Wang, Jingyu An, Cheng Huang, Song Guo, Keding Lu, Kangjia Gong, Haowen Zhang, Momei Qin, and Jianlin Hu
Atmos. Chem. Phys., 24, 7467–7479, https://doi.org/10.5194/acp-24-7467-2024, https://doi.org/10.5194/acp-24-7467-2024, 2024
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Naphthalene (Nap) and methylnaphthalene (MN) are key precursors of secondary organic aerosol (SOA), yet their sources and sinks are often inadequately represented in air quality models. In this study, we incorporated detailed emissions, gas-phase chemistry, and SOA parameterization of Nap and MN into CMAQ to address this issue. The findings revealed remarkably high SOA formation potentials for these compounds despite their low emissions in the Yangtze River Delta region during summer.
Vy Dinh Ngoc Thuy, Jean-Luc Jaffrezo, Ian Hough, Pamela A. Dominutti, Guillaume Salque Moreton, Grégory Gille, Florie Francony, Arabelle Patron-Anquez, Olivier Favez, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 7261–7282, https://doi.org/10.5194/acp-24-7261-2024, https://doi.org/10.5194/acp-24-7261-2024, 2024
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The capacity of particulate matter (PM) to generate reactive oxygen species in vivo is represented by oxidative potential (OP). This study focuses on finding the appropriate model to evaluate the oxidative character of PM sources in six sites using the PM sources and OP. Eight regression techniques are introduced to assess the OP of PM. The study highlights the importance of selecting a model according to the input data characteristics and establishes some recommendations for the procedure.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter G. Hess, Heikki Lihavainen, Christine Wiedinmyer, Jenny Hand, Maria Grazia Alaimo, Célia Alves, Andres Alastuey, Paulo Artaxo, Africa Barreto, Francisco Barraza, Silvia Becagli, Giulia Calzolai, Shankararaman Chellam, Ying Chen, Patrick Chuang, David D. Cohen, Cristina Colombi, Evangelia Diapouli, Gaetano Dongarra, Konstantinos Eleftheriadis, Johann Engelbrecht, Corinne Galy-Lacaux, Cassandra Gaston, Dario Gomez, Yenny González Ramos, Roy M. Harrison, Chris Heyes, Barak Herut, Philip Hopke, Christoph Hüglin, Maria Kanakidou, Zsofia Kertesz, Zbigniew Klimont, Katriina Kyllönen, Fabrice Lambert, Xiaohong Liu, Remi Losno, Franco Lucarelli, Willy Maenhaut, Beatrice Marticorena, Randall V. Martin, Nikolaos Mihalopoulos, Yasser Morera-Gomez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal Weagle, and Xi Zhao
EGUsphere, https://doi.org/10.5194/egusphere-2024-1617, https://doi.org/10.5194/egusphere-2024-1617, 2024
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Aerosol particles are an important part of the Earth system, but their concentrations are spatially and temporally heterogeneous, as well as variable in size and composition. Here we present a new compilation of PM2.5 and PM10 aerosol observations, focusing on the spatial variability across different observational stations, including composition, and demonstrate a method for comparing the datasets to model output.
Ming Chu, Xing Wei, Shangfei Hai, Yang Gao, Huiwang Gao, Yujiao Zhu, Biwu Chu, Nan Ma, Juan Hong, Yele Sun, and Xiaohong Yao
Atmos. Chem. Phys., 24, 6769–6786, https://doi.org/10.5194/acp-24-6769-2024, https://doi.org/10.5194/acp-24-6769-2024, 2024
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We used a 20-bin WRF-Chem model to simulate NPF events in the NCP during a three-week observational period in the summer of 2019. The model was able to reproduce the observations during June 29–July 6, which was characterized by a high frequency of NPF occurrence.
Haoqi Wang, Xiao Tian, Wanting Zhao, Jiacheng Li, Haoyu Yu, Yinchang Feng, and Shaojie Song
Atmos. Chem. Phys., 24, 6583–6592, https://doi.org/10.5194/acp-24-6583-2024, https://doi.org/10.5194/acp-24-6583-2024, 2024
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pH is a key property of ambient aerosols, which affect many atmospheric processes. As aerosol pH is a non-conservative parameter, diverse averaging metrics and temporal resolutions may influence the pH values calculated by thermodynamic models. This technical note seeks to quantitatively evaluate the average pH using varied metrics and resolutions. The ultimate goal is to establish standardized reporting practices in future research endeavors.
Jiwon Choi, Myoseon Jang, and Spencer Blau
Atmos. Chem. Phys., 24, 6567–6582, https://doi.org/10.5194/acp-24-6567-2024, https://doi.org/10.5194/acp-24-6567-2024, 2024
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Persistent phenoxy radical (PPR), formed by phenol gas oxidation and its aqueous reaction, catalytically destroys O3 and retards secondary organic aerosol (SOA) growth. Explicit gas mechanisms including the formation of PPR and low-volatility products from the oxidation of phenol or benzene are applied to the UNIPAR model to predict SOA mass via multiphase reactions of precursors. Aqueous reactions of reactive organics increase SOA mass but retard SOA growth via heterogeneously formed PPR.
Yang Yang, Shaoxuan Mou, Hailong Wang, Pinya Wang, Baojie Li, and Hong Liao
Atmos. Chem. Phys., 24, 6509–6523, https://doi.org/10.5194/acp-24-6509-2024, https://doi.org/10.5194/acp-24-6509-2024, 2024
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The variations in anthropogenic aerosol concentrations and source contributions and their subsequent radiative impact in major emission regions during historical periods are quantified based on an aerosol-tagging system in E3SMv1. Due to the industrial development and implementation of economic policies, sources of anthropogenic aerosols show different variations, which has important implications for pollution prevention and control measures and decision-making for global collaboration.
Maegan A. DeLessio, Kostas Tsigaridis, Susanne E. Bauer, Jacek Chowdhary, and Gregory L. Schuster
Atmos. Chem. Phys., 24, 6275–6304, https://doi.org/10.5194/acp-24-6275-2024, https://doi.org/10.5194/acp-24-6275-2024, 2024
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This study presents the first explicit representation of brown carbon aerosols in the GISS ModelE Earth system model (ESM). Model sensitivity to a range of brown carbon parameters and model performance compared to AERONET and MODIS retrievals of total aerosol properties were assessed. A summary of best practices for incorporating brown carbon into ModelE is also included.
Chuanyang Shen, Xiaoyan Yang, Joel Thornton, John Shilling, Chenyang Bi, Gabriel Isaacman-VanWertz, and Haofei Zhang
Atmos. Chem. Phys., 24, 6153–6175, https://doi.org/10.5194/acp-24-6153-2024, https://doi.org/10.5194/acp-24-6153-2024, 2024
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In this work, a condensed multiphase isoprene oxidation mechanism was developed to simulate isoprene SOA formation from chamber and field studies. Our results show that the measured isoprene SOA mass concentrations can be reasonably reproduced. The simulation results indicate that multifunctional low-volatility products contribute significantly to total isoprene SOA. Our findings emphasize that the pathways to produce these low-volatility species should be considered in models.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
Atmos. Chem. Phys., 24, 6011–6046, https://doi.org/10.5194/acp-24-6011-2024, https://doi.org/10.5194/acp-24-6011-2024, 2024
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This study presents the development of a bottom-up inventory of urban tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 %, and of ozone by 1.0 % on average over 2 months.
Tommaso Galeazzo, Bernard Aumont, Marie Camredon, Richard Valorso, Yong B. Lim, Paul J. Ziemann, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 5549–5565, https://doi.org/10.5194/acp-24-5549-2024, https://doi.org/10.5194/acp-24-5549-2024, 2024
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Secondary organic aerosol (SOA) derived from n-alkanes is a major component of anthropogenic particulate matter. We provide an analysis of n-alkane SOA by chemistry modeling, machine learning, and laboratory experiments, showing that n-alkane SOA adopts low-viscous semi-solid or liquid states. Our results indicate few kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA in large-scale atmospheric models.
Bin Luo, Yuqiang Zhang, Tao Tang, Hongliang Zhang, Jianlin Hu, Jiangshan Mu, Wenxing Wang, and Likun Xue
EGUsphere, https://doi.org/10.5194/egusphere-2024-974, https://doi.org/10.5194/egusphere-2024-974, 2024
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India is facing a severe air pollution crisis that poses significant health risks, particularly from PM2.5 and O3. Our study reveals rising levels of both pollutants from 1995 to 2014, leading to increased premature mortality. While anthropogenic emissions play a significant role, biomass burning also impacts air quality, in particular seasons and regions in India. This study highlights the urgent need for localized policies to protect public health amid escalating environmental challenges.
Lukáš Bartík, Peter Huszár, Jan Karlický, Ondřej Vlček, and Kryštof Eben
Atmos. Chem. Phys., 24, 4347–4387, https://doi.org/10.5194/acp-24-4347-2024, https://doi.org/10.5194/acp-24-4347-2024, 2024
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The presented study deals with the attribution of fine particulate matter (PM2.5) concentrations to anthropogenic emissions over Central Europe using regional-scale models. It calculates the present-day contributions of different emissions sectors to concentrations of PM2.5 and its secondary components. Moreover, the study investigates the effect of chemical nonlinearities by using multiple source attribution methods and secondary organic aerosol calculation methods.
Rui Wang, Yang Cheng, Shasha Chen, Rongrong Li, Yue Hu, Xiaokai Guo, Tianlei Zhang, Fengmin Song, and Hao Li
Atmos. Chem. Phys., 24, 4029–4046, https://doi.org/10.5194/acp-24-4029-2024, https://doi.org/10.5194/acp-24-4029-2024, 2024
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We used quantum chemical calculations, Born–Oppenheimer molecular dynamics simulations, and the ACDC kinetic model to characterize SO3–H2SO4 interaction in the gas phase and at the air–water interface and to study the effect of H2S2O7 on H2SO4–NH3-based clusters. The work expands our understanding of new pathways for the loss of SO3 in acidic polluted areas and helps reveal some missing sources of NPF in metropolitan industrial regions and understand the atmospheric organic–sulfur cycle better.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 24, 4001–4015, https://doi.org/10.5194/acp-24-4001-2024, https://doi.org/10.5194/acp-24-4001-2024, 2024
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The present study quantifies the response of aerosol–radiation interaction (ARI) to anthropogenic emission reduction from 2013 to 2017, with the main focus on the contribution to changed O3 concentrations over eastern China both in summer and winter using the WRF-Chem model. The weakened ARI due to decreased anthropogenic emission aggravates the summer (winter) O3 pollution by +0.81 ppb (+0.63 ppb), averaged over eastern China.
Margaret R. Marvin, Paul I. Palmer, Fei Yao, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 24, 3699–3715, https://doi.org/10.5194/acp-24-3699-2024, https://doi.org/10.5194/acp-24-3699-2024, 2024
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We use an atmospheric chemistry model to investigate aerosols emitted from fire activity across Southeast Asia. We find that the limited nature of measurements in this region leads to large uncertainties that significantly hinder the model representation of these aerosols and their impacts on air quality. As a result, the number of monthly attributable deaths is underestimated by as many as 4500, particularly in March at the peak of the mainland burning season.
Julie Camman, Benjamin Chazeau, Nicolas Marchand, Amandine Durand, Grégory Gille, Ludovic Lanzi, Jean-Luc Jaffrezo, Henri Wortham, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 3257–3278, https://doi.org/10.5194/acp-24-3257-2024, https://doi.org/10.5194/acp-24-3257-2024, 2024
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Fine particle (PM1) pollution is a major health issue in the city of Marseille, which is subject to numerous pollution sources. Sampling carried out during the summer enabled a fine characterization of the PM1 sources and their oxidative potential, a promising new metric as a proxy for health impact. PM1 came mainly from combustion sources, secondary ammonium sulfate, and organic nitrate, while the oxidative potential of PM1 came from these sources and from resuspended dust in the atmosphere.
Yuemeng Ji, Zhang Shi, Wenjian Li, Jiaxin Wang, Qiuju Shi, Yixin Li, Lei Gao, Ruize Ma, Weijun Lu, Lulu Xu, Yanpeng Gao, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 3079–3091, https://doi.org/10.5194/acp-24-3079-2024, https://doi.org/10.5194/acp-24-3079-2024, 2024
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The formation mechanisms for secondary brown carbon (SBrC) contributed by multifunctional reduced nitrogen compounds (RNCs) remain unclear. Hence, from combined laboratory experiments and quantum chemical calculations, we investigated the heterogeneous reactions of glyoxal (GL) with multifunctional RNCs, which are driven by four-step indirect nucleophilic addition reactions. Our results show a possible missing source for SBrC formation on urban, regional, and global scales.
Cited articles
Abram, N. J., Thomas, E. R., McConnell, J. R., Mulvaney, R., Bracegirdle, T. J.,
Sime, L. C., and Aristarain, A. J.: Ice core evidence for a 20th century decline
of sea ice in the Bellingshausen Sea, Antarctica, J. Geophys. Res., 115, D23101,
https://doi.org/10.1029/2010JD014644, 2010.
Alexander, B., Park, R. J., Jacob, D. J., and Gong S.: Transition metal-catalyzed
oxidation of atmospheric sulfur: Global implications for the sulfur budget, J.
Geophys. Res., 114, D02309, https://doi.org/10.1029/2008JD010486, 2009.
Alexander, B., Allman, D. J., Amos, H. M., Fairlie, T. D., Dachs, J., Hegg, D.
A., and Sletten, R. S.: Isotopic constraints on the formation pathways of
sulfate aerosol in the marine boundary layer of the subtropical northeast
Atlantic Ocean, J. Geophys. Res., 117, D06304, https://doi.org/10.1029/2011JD016773, 2012.
Ammann, M., Cox, R. A., Crowley, J. N., Jenkin, M. E., Mellouki, A., Rossi, M.
J., Troe, J., and Wallington, T. J.: Evaluated kinetic and photochemical data
for atmospheric chemistry: Volume VI – heterogeneous reactions with liquid
substrates, Atmos. Chem. Phys., 13, 8045–8228, https://doi.org/10.5194/acp-13-8045-2013, 2013.
Amos, H. M., Jacob, D. J., Holmes, C. D., Fisher, J. A., Wang, Q., Yantosca,
R. M., Corbitt, E. S., Galarneau, E., Rutter, A. P., Gustin, M. S., Steffen, A.,
Schauer, J. J., Graydon, J. A., Louis, V. L. St., Talbot, R. W., Edgerton, E. S.,
Zhang, Y., and Sunderland, E. M.: Gas-particle partitioning of atmospheric Hg(II)
and its effect on global mercury deposition, Atmos. Chem. Phys., 12, 591–603,
https://doi.org/10.5194/acp-12-591-2012, 2012.
Andreae, M. O.: Ocean-atmosphere interactions in the global biogeochemical
sulfur cycle, Mar. Chem., 30, 1–29, https://doi.org/10.1016/0304-4203(90)90059-L, 1990.
Andreae, M. O., Elbert, W., Cai, Y., Andreae, T. W., and Gras, J.: Non-sea-salt
sulfate, methanesulfonate, and nitrate aerosol concentrations and size
distributions at Cape Grim, Tasmania, J. Geophys. Res., 104, 21695–21706,
https://doi.org/10.1029/1999JD900283, 1999.
Arakaki, T., Anastasio, C., Kuroki, Y., Nakajima, H., Okada, K., Kotani, Y.,
Handa, D., Azechi, S., Kimura, T., Tsuhako, A., and Miyagi, Y.: A general
scavenging rate constant for reaction of hydroxyl radical with organic carbon
in atmospheric waters, Environ. Sci. Technol., 47, 8196–8203, https://doi.org/10.1021/es401927b, 2013.
Arsene, C., Barnes, I., and Becker, K. H.: FT-IR product study of the photo-oxidation
of dimethyl sulfide: Temperature and O2 partial pressure dependence,
Phys. Chem. Chem. Phys., 1, 5463–5470, https://doi.org/10.1039/A907211J, 1999.
Arsene, C., Bougiatioti, A., Kanakidou, M., Bonsang, B., and Mihalopoulos, N.:
Tropospheric OH and Cl levels deduced from non-methane hydrocarbon measurements
in a marine site, Atmos. Chem. Phys., 7, 4661–4673, https://doi.org/10.5194/acp-7-4661-2007, 2007.
Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F., Hynes,
R. G., Jenkin, M. E., Rossi, M. J., and Troe, J.: Evaluated kinetic and
photochemical data for atmospheric chemistry: Volume I – gas phase reactions
of Ox, HOx, NOx and
SOx species, Atmos. Chem. Phys., 4, 1461–1738, https://doi.org/10.5194/acp-4-1461-2004, 2004.
Ayers, G. P., Bartley, S. T., Ivey, J. P., and Forgan, B. W.: Dimethylsulfide
in marine air at Cape Grim, 41∘ S, J. Geophys. Res., 100, 21013–21021,
https://doi.org/10.1029/95JD02144, 1995.
Bardouki, H., Barcellos da Rosa, M., Mihalopoulous, N., Palm, W.- U., and
Zetzsch, C.: Kinetics and mechanism of the oxidation of dimethylsulfoxide (DMSO)
and methanesulfinate (MSI-) by OH radicals in aqueous medium, Atmos. Environ.,
36, 4627–4634, https://doi.org/10.1016/S1352-2310(02)00460-0, 2002.
Barnes, I., Hjorth, J., and Mihalopoulos, N.: Dimethyl sulfide and dimethyl
sulfoxide and their oxidation in the atmosphere, Chem. Rev., 106, 940-975,
https://doi.org/10.1021/cr020529+, 2006.
Becagli, S., Castellano, E., Cerri, O., Curran, M., Frezzotti, M., Marino, F.,
Morganti, A., Proposito, M., Severi, M., and Traversi, R.: Methanesulphonic
acid (MSA) stratigraphy from a Talos Dome ice core as a tool in depicting sea
ice changes and southern atmospheric circulation over the previous 140 years,
Atmos. Environ.,43, 1051–1058, https://doi.org/10.1016/j.atmosenv.2008.11.015, 2009.
Berglen, T. F., Berntsen, T. K., Isaksen, I. S. A., and Sundet, J. K.: A global
model of the coupled sulfur/oxidant chemistry in the troposphere: The sulfur
cycle, J. Geophys. Res., 109, D19310, https://doi.org/10.1029/2003JD003948, 2004.
Bey, I., Jacob, D. J., Yantosca, R. M., Logan, J. A., Field, B. D., Fiore, A.
M., Li, Q., Liu, H. Y., Mickley, L. J., and Schultz, M. G.: Global modeling of
tropospheric chemistry with assimilated meteorology: Model description and
evaluation, J. Geophys. Res., 106, 23073–23095, https://doi.org/10.1029/2001JD000807, 2001.
Boucher, O., Moulin, C., Belviso, S., Aumont, O., Bopp, L., Cosme, E.,
von Kuhlmann, R., Lawrence, M. G., Pham, M., Reddy, M. S., Sciare, J., and
Venkataraman, C.: DMS atmospheric concentrations and sulphate aerosol indirect
radiative forcing: a sensitivity study to the DMS source representation and
oxidation, Atmos. Chem. Phys., 3, 49–65, https://doi.org/10.5194/acp-3-49-2003, 2003.
Boudries, H. and Bottenheim, J. W.: Cl and Br atom concentrations during a
surface boundary layer ozone depletion event in the Canadian High Arctic,
Geophys. Res. Lett., 27, 517–520, https://doi.org/10.1029/1999GL011025, 2000.
Breider, T. J., Chipperfield, M. P., Richards, N. A. D., Carslaw, K. S., Mann,
G. W., and Spracklen, D. V.: Impact of BrO on dimethylsulfide in the remote
marine boundary layer, Geophys. Res. Lett., 37, L02807, https://doi.org/10.1029/2009GL040868, 2010.
Burkholder, J. B., Sander, S. P., Abbatt, J., Barker, J. R., Huie, R. E., Kolb,
C. E., Kurylo, M. J., Orkin, V. L., Wilmouth, D. M., and Wine, P. H.: Chemical
Kinetics and Photochemical Data for Use in Atmospheric Studies, Evaluation No. 18,
JPL Publication 15-10, Jet Propulsion Laboratory, Pasadena, availabel at:
http://jpldataeval.jpl.nasa.gov (last access: 19 September 2018), 2015.
Butkovskaya, N. I., Poulet, G., and LeBras, G.: Discharge flow study of the
reactions of chlorine and fluorine atoms with dimethyl sulfide, J. Phys. Chem.,
99, 4536–4543, https://doi.org/10.1021/j100013a025, 1995.
Campolongo, F., Saltelli, A., Jensen, N. R., Wilson, J., and Hjorth, J.: The
role of multiphase chemistry in the oxidation of dimethylsulfide (DMS) – A
latitude dependent analysis, J. Atmos. Chem., 32, 327–356, https://doi.org/10.1023/A:1006154618511, 1999.
Carslaw, K. S., Lee, L. A., Reddington, C. L., Pringle, K. J., Rap, A., Forster,
P. M., Mann, G. W., Spracklen, D. V., Woodhouse, M. T., Regayre, L. A., and
Pierce, J. R.: Large contribution of natural aerosols to uncertainty in indirect
forcing, Nature, 503, 67–71, https://doi.org/10.1038/nature12674, 2013.
Castebrunet, H., Martinerie, P., Genthon, C., and Cosme, E.: A three-dimensional
model study of methanesulphonic acid to non sea salt sulphate ratio at mid and
high-southern latitudes, Atmos. Chem. Phys., 9, 9449–9469, https://doi.org/10.5194/acp-9-9449-2009, 2009.
Charlson, R. J., Lovelock, J. E., Andreae, M. O., and Warren, S. G.: Oceanic
phytoplankton, atmospheric sulphur, cloud albedo and climate, Nature, 326,
655–661, https://doi.org/10.1038/326655a0, 1987.
Chatfield, R. B. and Crutzen, P. J.: Are there interactions of iodine and sulfur
species in marine air photochemistry?, J. Geophys. Res., 95, 22319–22341,
https://doi.org/10.1029/JD095iD13p22319, 1990.
Chen, H., Ezell, M. J., Arquero, K. D., Varner, M. E., Dawson, M. L., Gerber,
R. B., and Finlayson-Pitts, B. J.: New particle formation and growth from
methanesulfonic acid, trimethylamine and water, Phys. Chem. Chem. Phys., 17,
13699–13709, https://doi.org/10.1039/c5cp00838g, 2015.
Chen, Q., Geng, L., Schmidt, J. A., Xie, Z., Kang, H., Dachs, J., Cole-Dai, J.,
Schauer, A. J., Camp, M. G., and Alexander, B.: Isotopic constraints on the role
of hypohalous acids in sulfate aerosol formation in the remote marine boundary
layer, Atmos. Chem. Phys., 16, 11433–11450, https://doi.org/10.5194/acp-16-11433-2016, 2016.
Chen, Q., Schmidt, J. A., Shah, V., Jaeglé, L., Sherwen, T., and Alexander,
B.: Sulfate production by reactive bromine: Implications for the global sulfur
and reactive bromine budgets, Geophys. Res. Lett., 44, 7069–7078, https://doi.org/10.1002/2017GL073812, 2017.
Chin, M., Jacob, D. J., Gardner, G. M., Foreman-Fowler, M. S., Spiro, P. A.,
and Savoie, D. L.: A global three-dimensional model of tropospheric sulfate,
J. Geophys. Res., 101, 18667–18690, https://doi.org/10.1029/96JD01221, 1996.
Chin, M., Rood, R. B., Lin, S.-J., Muller, J. F., and Thompson, A. M.:
Atmospheric sulfur cycle in the global model GOCART: Model description and
global properties, J. Geophys. Res., 105, 24671–24687, 2000.
Clarke, J. H. R. and Woodward, L. A.: Raman spectrophotometric determination of
the degrees of dissociation of methanesulphonic acid in aqueous solution at
25 ∘C, T. Faraday Soc., 62, 2226–2233, 1966.
Cosme, E., Genthon, C., Martinerie, P., Boucher, O., and Pham, M.: The sulfer
cycle at high-southern latitudes in the LMDZT General Circulation Model, J.
Geophys. Res., 107, 4690, https://doi.org/10.1029/2002JD002149, 2002.
Curran, M. A. J., van Ommen, T. D., Morgan, V. I., Phillips, K. L., and Palmer,
A. S.: Ice core evidence for Antarctic sea ice decline since the 1950s, Science,
302, 1203–1206, https://doi.org/10.1126/science.1087888, 2003.
Du, L., Xu, Y., Ge, M., Jia, L., Yao, L., and Wang, W.: Rate constant of the
gas phase reaction of dimethyl sulfide (CH3SCH3) with ozone, Chem.
Phys. Lett., 436, 36–40, https://doi.org/10.1016/j.cplett.2007.01.025, 2007.
Faloona, I.: Sulfur processing in the marine atmospheric boundary layer: A
review and critical assessment of modeling uncertainties, Atmos. Environ.,
43, 2841–2854, https://doi.org/10.1016/j.atmosenv.2009.02.043, 2009.
Fisher, J. A., Murray, L. T., Jones, D. B. A., and Deutscher, N. M.: Improved
method for linear carbon monoxide simulation and source attribution in
atmospheric chemistry models illustrated using GEOS-Chem v9, Geosci. Model Dev.,
10, 4129–4144, https://doi.org/10.5194/gmd-10-4129-2017, 2017.
Flyunt, R., Makogon, O., Schuchmann, M. N., Asmus, K. D., and von Sonntag, C.:
OH-Radical-induced oxidation of methanesulfinic acid. The reactions of the
methanesulfonyl radical in the absence and presence of dioxygen, J. Chem. Soc.
Perkin Trans., 2, 787–792, https://doi.org/10.1039/B009631H, 2001.
Gershenzon, M., Davidovits, P., Jayne, J. T., Kolb, C. E., and Worsnop, D. R.:
Simultaneous uptake of DMS and ozone on water, J. Phys. Chem. A, 105, 7031–7036,
https://doi.org/10.1021/jp010696y, 2001.
Gondwe, M., Krol, M., Gieskes, W., Klaassen, W., and de Baar, H.: The
contribution of ocean-leaving DMS to the global atmospheric burdens of DMS,
MSA, SO2, and NSS
Gondwe, M., Krol, M., Klassen, W., Gieskes, W., and De Baar, H.: Comparison
of modeled versus measured MSA : nss
Gromov, S., Brenninkmeijer, C. A. M., and Jöckel, P.: A very limited role
of tropospheric chlorine as a sink of the greenhouse gas methane, Atmos. Chem.
Phys., 18, 9831–9843, https://doi.org/10.5194/acp-18-9831-2018, 2018.
Herrmann, H. and Zellner, R.: Removal and interconversions of oxidants in
the atmospheric aqueous phase, Part 2 (RINOXA 2), Universität Essen, Essen, Germany, 1997.
Herrmann, H., Ervens, B., Jacobi, H.-W., Wolke, R., Nowacki, P., and Zellner,
R.: CAPRAM2.3: A Chemical Aqueous Phase Radical Mechanism for Tropospheric
Chemistry, J. Atmos. Chem., 36, 231–284, https://doi.org/10.1023/A:1006318622743, 2000.
Hezel, P. J., Alexander, B., Bitz, C. M., Steig, . J., Holmes, C. D., Yang, X.,
and Sciare, J.: Modeled methanesulfonic acid (MSA) deposition in Antarctica and
its relationship to sea ice, . Geophys. Res., 116, D23214, https://doi.org/10.1029/2011JD016383, 2011.
Hoffmann, E. H., Tilgner, A., Schrödner, R., Bräuer, P., Wolke, R., and
Herrmann, H.: An advanced modeling study on the impacts and atmospheric
implications of multiphase dimethyl sulfide chemistry, P. Natl. Acad. Sci. USA,
113, 11776–11781, https://doi.org/10.1073/pnas.1606320113, 2016.
Hossaini, R., Chipperfield, M. P., Saiz-Lopez, A., Fernandez, R., Monks, S.,
Feng, W., Brauer, P., and von Glasow, R.: A global model of tropospheric
chlorine chemistry: Organic versus inorganic sources and impact on methane
oxidation, J. Geophys. Res.-Atmos., 121, 14271–14297, https://doi.org/10.1002/2016JD025756, 2016.
Hynes, A. J., Stickel, R. E., Pounds, A. J., Zhao, Z., McKay, T., Bradshaw, J.
D., and Wine, P. H.: Mechanistic studies of the OH-induced oxidation of
dimethylsulfide, in: Proceedings of the International Symposium on Dimethylsulfide:
Oceans, Atmosphere, and Climate, edited by: Restelli, G. and Angeletti, G.,
Kluwer Academic Publishers, Norwell, MA, USA, 211–221, 1993.
Jacob, D. J.: Chemistry of OH in remote clouds and its role in the production
of formic acid and peroxymonosulfate, J. Geophys. Res., 91, 9807–9826,
https://doi.org/10.1029/JD091iD09p09807, 1986.
Jacob, D. J., Gottlieb, E. W., and Prather, M. J.: Chemistry of a polluted
cloudy boundary layer, J. Geophys. Res.-Atmos., 94, 12975–13002,
https://doi.org/10.1029/JD094iD10p12975, 1989.
Jacob, D. J., Field, B. D., Li, Q., Blake, D. R., de Gouw, J., Warneke, C.,
Hansel, A., Wisthaler, A., Singh, H. B., and Guenther, A.: Global budget of
methanol: Constraints from atmospheric observations, J. Geophys. Res., 110,
D08303, https://doi.org/10.1029/2004JD005172, 2005.
Jaeglé, L., Quinn, P. K., Bates, T. S., Alexander, B., and Lin, J.-T.:
Global distribution of sea salt aerosols: new constraints from in situ and
remote sensing observations, Atmos. Chem. Phys., 11, 3137–3157, https://doi.org/10.5194/acp-11-3137-2011, 2011.
Jobson, B. T., Niki, H., Yokouchi, Y., Bottenheim, J., Hopper, F., and Leaitch,
R.: Measurements of C2–C6 hydrocarbons during the Polar Sunrise
1992 Experiment: Evidence for Cl atom and Br atom chemistry, J. Geophys. Res.,
99, 25355–25368, https://doi.org/10.1029/94JD01243, 1994.
Kaufman, Y. and Tanre, D.: Effect of variations in super-saturation on the
formation of cloud condensation nuclei, Nature, 369, 45–48, https://doi.org/10.1038/369045a0, 1994.
Kaur, R. and Anastasio, C.: Light absorption and the photoformation of hydroxyl
radical and singlet oxygen in fog waters, Atmos. Environ., 164, 387–397,
https://doi.org/10.1016/j.atmosenv.2017.06.006, 2017.
Kettle, A., Andreae, M., Amouroux, D., Andreae, T., Bates, T., Berresheim, H.,
Bingemer, H., Boniforti, R., Curran, M., DiTullio, G., Helas, G., Jones, G.,
Keller, M., Kiene, R., Leck, C., Levasseur, M., Malin, G., Maspero, M., Matrai,
P., McTaggart, A., Mihalopoulos, N., Nguyen, B., Novo, A., Putaud, J.,
Rapsomanikis, S., Roberts, G., Schebeske, G., Sharma, S., Simo, R., Staubes, R.,
Turner, S., and Uher, G.: A global database of sea surface dimethylsulfide (DMS)
measurements and a procedure to predict sea surface DMS as a function of latitude,
longitude, and month, Global Biogeochem. Cy., 13, 399–444, https://doi.org/10.1029/1999GB900004, 1999.
Khan, M. A. H., Gillespie, S. M. P., Razis, B., Xiao, P., DaviesColeman, M. T.,
Percival, C. J., Derwent, R. G., Dyke, J. M., Ghosh, M. V., Lee, E. P. F., and
Shallcross, D. E.: A modelling study of the atmospheric chemistry of DMS using
the global model, STOCHEM-CRI, Atmos. Environ., 127, 69–79, https://doi.org/10.1016/j.atmosenv.2015.12.028, 2016.
Kloster, S., Feichter, J., Maier-Reimer, E., Six, K. D., Stier, P., and Wetzel,
P.: DMS cycle in the marine ocean-atmosphere system – a global model study,
Biogeosciences, 3, 29–51, https://doi.org/10.5194/bg-3-29-2006, 2006.
Kouvarakis, G. and Mihalopoulos, N.: Seasonal variation of dimethylsulfide in
the gas phase and of methanesulfonate and non-sea-salt sulfate in the aerosols
phase in the eastern Mediterranean atmosphere, Atmos. Environ., 36, 929–938,
https://doi.org/10.1016/S1352-2310(01)00511-8, 2002.
Kreidenweis, S. M. and Seinfeld, J. H.: Nucleation of sulfuric acid-water and
methanesulfonic acid-water solution particles: implications for the atmospheric
chemistry of organosulfur species, Atmos. Environ., 22, 283–296, https://doi.org/10.1016/0004-6981(88)90034-0, 1988.
Kukui, A., Borissenko, D., Laverdet, G., and Bras, G. L.: Gas phase reactions
of OH radicals with dimethyl sulfoxide and methane sulfonic acid using turbulent
flow reactor and chemical ionization mass spectrometry, J. Phys. Chem. A, 107,
5732–5742, https://doi.org/10.1021/jp0276911, 2003.
Kulmala, M., Pirjola, L., and Mäkelä, J. M.: Stable sulphate clusters
as a source of new atmospheric particles, Nature, 404, 66–69, https://doi.org/10.1038/35003550, 2000.
Lana, A., Bell, T. G., Simó, R., Vallina, S. M., Ballabrera-Poy, J., Kettle,
A. J., Dachs, J., Bopp, L., Saltzman, E. S., Ste- fels, J., Johnson, J. E., and
Liss, P. S.: An updated climatology of surface dimethylsulfide concentrations
and emission fluxes in the global ocean, Global Biogeochem. Cy., 25, GB1004,
https://doi.org/10.1029/2010GB003850, 2011.
Lee, Y.-N. and Zhou, X.: Aqueous reaction kinetics of ozone and dimethylsulfide
and its atmospheric implications, J. Geophys. Res., 99, 3597–3605, https://doi.org/10.1029/93JD02919, 1994.
Legrand, M., Preunkert, S., Weller, R., Zipf, L., Elsässer, C., Merchel, S.,
Rugel, G., and Wagenbach, D.: Year-round record of bulk and size-segregated
aerosol composition in central Antarctica (Concordia site) – Part 2: Biogenic
sulfur (sulfate and methanesulfonate) aerosol, Atmos. Chem. Phys., 17,
14055–14073, https://doi.org/10.5194/acp-17-14055-2017, 2017.
Liu, Q.: Kinetics of aqueous phase reactions related to ozone depletion in the
arctic troposphere: bromine chloride hydrolysis, bromide ion with ozone, and
sulfur(IV) with bromine and hypobromous acid, PhD thesis, Department of Chemistry,
Purdue University, Purdue, USA, 253 pp., 2000.
Liu, H., Jacob, D. J., Bey, I., and Yantosca, R. M.: Constraints from
210Pb and 7Be on wet deposition and transport in a global
three-dimensional chemical tracer model driven by assimilated meteorological
fields, J. Geophys. Res., 106, 12109–12128, https://doi.org/10.1029/2000JD900839,
2001.
Lucas, D. D. and Prinn, R. G.: Mechanistic studies of dimethylsulfide oxidation
products using an observationally constrained model, J. Geophys. Res., 107,
1201–1226, https://doi.org/10.1029/2001JD000843, 2002.
Martin, L. R. and Good, T. W.: Catalyzed oxidation of sulfur dioxide in solution:
The iron-manganese synergism, Atmos. Environ. A, 25, 2395–2399, https://doi.org/10.1016/0960-1686(91)90113-L, 1991.
Matthijsen, J., Builtjes, P. J. H., and Sedlak, D. L.: Cloud model experiments
of the effect of iron and copper on tropospheric ozone under marine and
continental conditions, Meteorol. Atmos. Phys., 57, 43–60, https://doi.org/10.1007/BF01044153, 1995.
Milne, P. J., Zika, R. G., and Saltzman, E. S.: Rate of reaction of dimethyl
sulfoxide, and dimethyl sulfone with hydroxyl radical in aqueous solution,
in: chap. 33, ACS Symposium Series, American Chemical Society, Washington, D.C., 518–528, 1989.
Mungall, E., Wong, J. P. S., and Abbatt, J. P. D.: Heterogeneous oxidation of
particulate methane sulfonic acid by the hydroxyl radical: kinetics and
atmospheric implications, ACS Earth Space Chem., 2, 48–55, https://doi.org/10.1021/acsearthspacechem.7b00114, 2018.
Park, R. J., Jacob, D. J., Field, B. D., Yantosca, R. M., and Chin, M.: Natural
and transboundary pollution influences on sulfate-nitrate-ammonium aerosols in
the United States: Implications for policy, J. Geophys. Res., 109, D15204,
https://doi.org/10.1029/2003JD004473, 2004.
Parrella, J. P., Jacob, D. J., Liang, Q., Zhang, Y., Mickley, L. J., Miller,
B., Evans, M. J., Yang, X., Pyle, J. A., Theys, N., and Van Roozendael, M.:
Tropospheric bromine chemistry: implications for present and pre-industrial
ozone and mercury, Atmos. Chem. Phys., 12, 6723–6740, https://doi.org/10.5194/acp-12-6723-2012, 2012.
Pham, M., Müller, J., Brasseur, G. P., Granier, C., and Mégie, G.: A
three-dimensional study of the tropospheric sulfur cycle, J. Geophys. Res.,
100, 26061–26092, https://doi.org/10.1029/95JD02095, 1995.
Pye, H. O. T., Liao, H., Wu, S., Mickley, L. J., Jacob, D. J., Henze, D. K.,
and Seinfeld, J. H.: Effect of changes in climate and emissions on future
sulfate-nitrate-ammonium aerosol levels in the United States, J. Geophys. Res.,
114, D01205, https://doi.org/10.1029/2008JD010701, 2009.
Ravishankara, A. R., Rudich, Y., Talukdar, R., and Barone, S. B.: Oxidation of
atmospheric reduced sulphur compounds: perspective from laboratory studies,
Philos. T. Roy. Soc. Lond. B., 352, 171–182, https://doi.org/10.1098/rstb.1997.0012, 1997.
Read, K. A., Lewis, A. C., Salmon, R. A., Jones, A. E., and Bauguitte, S.: OH
and halogen influence on the variability of nonmethane hydrocarbons in the
Antarctic Boundary Layer, Tellus B, 59, 22–38, https://doi.org/10.1111/j.1600-0889.2006.00227.x, 2007.
Saltzman, E. S., King, D. B., Holmen, K., and Leck, C.: Experimental determination
of the diffusion coefficient of dimethylsulfide in water, J. Geophys. Res.-Oceans,
98, 16481–16486, https://doi.org/10.1029/93JC01858, 1993.
Savoie, D. L., Arimoto, R., Keene, W. C., Prospero, J. M., Duce, R. A., and
Galloway, J. N.: Marine biogenic and anthropogenic contributions to non-sea-salt
sulfate in the marine boundary layer over the North Atlantic Ocean, J. Geophys.
Res., 107, AAC3-1–AAC3-21, https://doi.org/10.1029/2001JD000970, 2002.
Schmidt, J. A., Jacob, D. J., Horowitz, H. M., Hu, L., Sherwen, T., Evans, M.
J., Liang, Q., Suleiman, R. M., Oram, D. E., Le Breton, M., Percival, C. J.,
Wang, S., Dix, B., and Volkamer, R.: Modeling the observed tropospheric BrO
background: Importance of multiphase chemistry and implications for ozone, OH,
and mercury, J. Geophys. Res.-Atmos., 121, 155–157, https://doi.org/10.1002/2015JD024229, 2016.
Schweitzer, F., Magi, L., Mirabel, P., and George, C.: Uptake rate measurements
of methanesulfonic acid and glyoxal by aqueous droplets, J. Phys. Chem. A, 102,
593–600, https://doi.org/10.1021/jp972451k, 1998.
Sehested, K. and Holcman, J.: A pulse radiolysis study of the OH radical induced
autoxidation of methanesulfinic acid, Radiat. Phys. Chem., 47, 357–360,
https://doi.org/10.1016/0969-806X(95)00115-E, 1996.
Sherwen, T., Schmidt, J. A., Evans, M. J., Carpenter, L. J., Großmann, K.,
Eastham, S. D., Jacob, D. J., Dix, B., Koenig, T. K., Sinreich, R., Ortega, I.,
Volkamer, R., Saiz-Lopez, A., Prados-Roman, C., Mahajan, A. S., and Ordóñez,
C.: Global impacts of tropospheric halogens (Cl, Br, I) on oxidants and
composition in GEOS-Chem, Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, 2016.
Simpson, W. R., Brown, S. S., Saiz-Lopez, A., Thornton, J. A., and von Glasow,
R.: Tropospheric Halogen Chemistry: Sources, Cycling, and Impacts, Chem. Rev.,
115, 4035–4062, https://doi.org/10.1021/cr5006638, 2015.
Singh, H. B., Gregory, G. L., Anderson, B., Browell, E., Sachse, G. W., Davis,
D. D., Crawford, J., Bradshaw, J. D., Talbot, R., Blake, D. R., Thornton, D.,
Newell, R., and Merill, J.: Low ozone in the marine boundary layer of the
tropical Pacific ocean: Photochemical loss, chlorine atoms, and entrainment, J.
Geophys. Res., 101, 1907–1917, https://doi.org/10.1029/95JD01028, 1996.
Spracklen, D. V., Pringle, K. J., Carslaw, K. S., Chipperfield, M. P., and Mann,
G. W.: A global off-line model of size-resolved aerosol microphysics: I. Model
development and prediction of aerosol properties, Atmos. Chem. Phys., 5,
2227–2252, https://doi.org/10.5194/acp-5-2227-2005, 2005.
Theys, N., Van Roozendael, M., Hendrick, F., Yang, X., De Smedt, I., Richter,
A., Begoin, M., Errera, Q., Johnston, P. V., Kreher, K., and De Mazière, M.:
Global observations of tropospheric BrO columns using GOME-2 satellite data,
Atmos. Chem. Phys., 11, 1791–1811, https://doi.org/10.5194/acp-11-1791-2011, 2011.
Thomas, M. A., Suntharalingam, P., Pozzoli, L., Rast, S., Devasthale, A.,
Kloster, S., Feichter, J., and Lenton, T. M.: Quantification of DMS
aerosol–cloud–climate interactions using the ECHAM5-HAMMOZ model in a current
climate scenario, Atmos. Chem. Phys., 10, 7425–7438, https://doi.org/10.5194/acp-10-7425-2010, 2010.
Troy, R. C. and Margerum, D. W.: Non-metal redox kinetics: Hypobromite and
hypobromous acid reactions with iodide and with sulfite and the hydrolysis of
bromosulfate, Inorg. Chem., 30, 3538–3543, https://doi.org/10.1021/ic00018a028, 1991.
Turnipseed, A. A. Barone, S. B., and Ravishankara, A. R.: Reaction of OH with
dimethyl sulphide (DMS) – 2. Products and mechanisms, J. Phys. Chem., 100,
14703–14713, https://doi.org/10.1021/jp960867c, 1996.
von Glasow, R. and Crutzen, P. J.: Model study of multiphase DMS oxidation with
a focus on halogens, Atmos. Chem. Phys., 4, 589–608, https://doi.org/10.5194/acp-4-589-2004, 2004.
von Glasow, R., von Kuhlmann, R., Lawrence, M. G., Platt, U., and Crutzen, P.
J.: Impact of reactive bromine chemistry in the troposphere, Atmos. Chem. Phys.,
4, 2481–2497, https://doi.org/10.5194/acp-4-2481-2004, 2004.
Wang, Y., Jacob, D. J., and Logan, J. A.: Global simulation of tropospheric
O3-NOx-hydrocarbon chemistry: 1. Model formulation,
J. Geophys. Res., 103, 10713–10725, https://doi.org/10.1029/98JD00158, 1998.
Wingenter, O. W., Kubo, M. K., Blake, N. J., Smith, T. W., Blake, D. R., and
Rowland, F. S.: Hydrocarbon and halocarbon measurements as photochemical and
dynamical indicators of atmospheric hydroxyl, atomic chlorine, and vertical
mixing obtained during Lagrangian flights, J. Geophys. Res., 101, 4331–4340,
https://doi.org/10.1029/95JD02457, 1996.
Wingenter, O. W., Sive, B. C., Blake, N. J., Blake, D. R., and Rowland, F. S.:
Atomic chlorine concentrations derived from ethane and hydroxyl measurements
over the equatorial Pacific Ocean: Implication for dimethyl sulphide and bromine
monoxide, J. Geophys. Res., 110, D20308, https://doi.org/10.1029/2005JD005875, 2005.
Wudl, F., Lightner, D. A., and Cram, D. J.: Methanesulfinic acid and its
properties, J. Am. Chem. Soc., 89, 4099–4101, 1967.
Zhang, L., Gong, S.-L., Padro, J., and Barrie, L.: A Size-segregated Particle
Dry Deposition Scheme for an Atmospheric Aerosol Module, Atmos. Environ., 35,
549–560, https://doi.org/10.1016/S1352-2310(00)00326-5, 2001.
Zhu, L., Nicovich, J. M., and Wine, P. H.: Temperature-dependent kinetics
studies of aqueous phase reactions of hydroxyl radicals with dimethylsulfoxide,
dimethylsulfone, and methanesulfonate, Aquat. Sci., 65, 425–435, https://doi.org/10.1007/s00027-003-0673-6, 2003.
Zhu, L., Nenes, A., Wine, P. H., and Nicovich, J. M.: Effects of aqueous
organosulfur chemistry on particulate methanesulfonate to non-sea salt sulfate
ratios in the marine atmosphere, J. Geophys. Res., 111, D05316, https://doi.org/10.1029/2005JD006326, 2006.
Short summary
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.
Uncertainty in the natural tropospheric sulfur cycle represents the largest source of...
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