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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Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
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Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Tomas 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
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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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The cycling of NO and NO2 is important to understand to be able to predict O3 concentrations in the atmosphere. We have used long-term measurements from the Cape Verde Atmospheric Observatory together with model outputs to investigate the cycling of nitrogen oxide (NO) and nitrogen dioxide (NO2) in very clean marine air. This study shows that we understand the processes occurring in very clean air, but with small amounts of pollution in the air, known chemistry cannot explain what is observed.
Qianjie Chen, Jessica A. Mirrielees, Sham Thanekar, Nicole A. Loeb, Rachel M. Kirpes, Lucia M. Upchurch, Anna J. Barget, Nurun Nahar Lata, Angela R. W. Raso, Stephen M. McNamara, Swarup China, Patricia K. Quinn, Andrew P. Ault, Aaron Kennedy, Paul B. Shepson, Jose D. Fuentes, and Kerri A. Pratt
Atmos. Chem. Phys., 22, 15263–15285, https://doi.org/10.5194/acp-22-15263-2022, https://doi.org/10.5194/acp-22-15263-2022, 2022
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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
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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)
Rapid oxidation of phenolic compounds by O3 and HO●: effects of the air–water interface and mineral dust in tropospheric chemical processes
Modeling the contribution of leads to sea spray aerosol in the high Arctic
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
Observed and CMIP6-model-simulated organic aerosol response to drought in the contiguous United States during summertime
Cooling radiative forcing effect enhancement of atmospheric amines and mineral particles caused by heterogeneous uptake and oxidation
Exploring the processes controlling secondary inorganic aerosol: Evaluating the global GEOS-Chem simulation using a suite of aircraft campaigns
Source-resolved atmospheric metal emissions, concentrations, and deposition fluxes into the East Asian seas
Predicted impacts of heterogeneous chemical pathways on particulate sulfur over Fairbanks, Alaska, the N. Hemisphere, and the Contiguous United States
Quantifying the impact of global nitrate aerosol on tropospheric composition fields and its production from lightning NOx
Land use change influence on atmospheric organic gases, aerosols, and radiative effects
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
Quantifying the Impacts of Marine Aerosols over the Southeast Atlantic Ocean using a chemical transport model: Implications for aerosol-cloud interactions
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
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
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
An updated modeling framework to simulate Los Angeles air quality – Part 1: Model development, evaluation, and source apportionment
Frequent haze events associated with transport and stagnation over the corridor between the North China Plain and Yangtze River Delta
Evaluation of WRF-Chem-simulated meteorology and aerosols over northern India during the severe pollution episode of 2016
How well are aerosol–cloud interactions represented in climate models? – Part 1: Understanding the sulfate aerosol production from the 2014–15 Holuhraun eruption
pH regulates the formation of organosulfates and inorganic sulfate from organic peroxide reaction with dissolved SO2 in aquatic media
Technical note: Accurate, reliable, and high-resolution air quality predictions by improving the Copernicus Atmosphere Monitoring Service using a novel statistical post-processing method
Contribution of intermediate-volatility organic compounds from on-road transport to secondary organic aerosol levels in Europe
Development of an integrated model framework for multi-air-pollutant exposure assessments in high-density cities
CAMx–UNIPAR simulation of secondary organic aerosol mass formed from multiphase reactions of hydrocarbons under the Central Valley urban atmospheres of California
Impact of urbanization on fine particulate matter concentrations over central Europe
Measurement report: Assessing the impacts of emission uncertainty on aerosol optical properties and radiative forcing from biomass burning in peninsular Southeast Asia
The Emissions Model Intercomparison Project (Emissions-MIP): quantifying model sensitivity to emission characteristics
Dynamics-based estimates of decline trend with fine temporal variations in China's PM2.5 emissions
Effects of simulated secondary organic aerosol water on PM1 levels and composition over the US
Reactive organic carbon air emissions from mobile sources in the United States
Development and evaluation of processes affecting simulation of diel fine particulate matter variation in the GEOS-Chem model
Substantially positive contributions of new particle formation to cloud condensation nuclei under low supersaturation in China based on numerical model improvements
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.
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.
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.
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.
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.
Olivia G. Norman, Colette L. Heald, 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
EGUsphere, https://doi.org/10.5194/egusphere-2024-2296, https://doi.org/10.5194/egusphere-2024-2296, 2024
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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).
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.
Sara Louise Farrell, Havala O. T. Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, and Kathleen Fahey
EGUsphere, https://doi.org/10.5194/egusphere-2024-1550, https://doi.org/10.5194/egusphere-2024-1550, 2024
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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.
Ashok K. Luhar, Anthony C. Jones, and Jonathan M. Wilkinson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1363, https://doi.org/10.5194/egusphere-2024-1363, 2024
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Nitrate aerosol is often omitted in global chemistry-climate models due to the chemical complexity of its formation process. Using a global model, we demonstrate 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.
Ryan Vella, Matthew Forrest, Andrea Pozzer, Alexandra P. Tsimpidi, Thomas Hickler, Jos Lelieveld, and Holger Tost
EGUsphere, https://doi.org/10.5194/egusphere-2024-2014, https://doi.org/10.5194/egusphere-2024-2014, 2024
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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.
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.
Mashiat Hossain, Rebecca M. Garland, and Hannah M. Horowitz
EGUsphere, https://doi.org/10.5194/egusphere-2024-1948, https://doi.org/10.5194/egusphere-2024-1948, 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.
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.
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.
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.
Elyse A. Pennington, Yuan Wang, Benjamin C. Schulze, Karl M. Seltzer, Jiani Yang, Bin Zhao, Zhe Jiang, Hongru Shi, Melissa Venecek, Daniel Chau, Benjamin N. Murphy, Christopher M. Kenseth, Ryan X. Ward, Havala O. T. Pye, and John H. Seinfeld
Atmos. Chem. Phys., 24, 2345–2363, https://doi.org/10.5194/acp-24-2345-2024, https://doi.org/10.5194/acp-24-2345-2024, 2024
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To assess the air quality in Los Angeles (LA), we improved the CMAQ model by using dynamic traffic emissions and new secondary organic aerosol schemes to represent volatile chemical products. Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated, with the largest sensitivity of O3 to changes in volatile organic compounds in the urban core. The improvement and remaining issues shed light on the future direction of the model development.
Feifan Yan, Hang Su, Yafang Cheng, Rujin Huang, Hong Liao, Ting Yang, Yuanyuan Zhu, Shaoqing Zhang, Lifang Sheng, Wenbin Kou, Xinran Zeng, Shengnan Xiang, Xiaohong Yao, Huiwang Gao, and Yang Gao
Atmos. Chem. Phys., 24, 2365–2376, https://doi.org/10.5194/acp-24-2365-2024, https://doi.org/10.5194/acp-24-2365-2024, 2024
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PM2.5 pollution is a major air quality issue deteriorating human health, and previous studies mostly focus on regions like the North China Plain and Yangtze River Delta. However, the characteristics of PM2.5 concentrations between these two regions are studied less often. Focusing on the transport corridor region, we identify an interesting seesaw transport phenomenon with stagnant weather conditions, conducive to PM2.5 accumulation over this region, resulting in large health effects.
Prerita Agarwal, David S. Stevenson, and Mathew R. Heal
Atmos. Chem. Phys., 24, 2239–2266, https://doi.org/10.5194/acp-24-2239-2024, https://doi.org/10.5194/acp-24-2239-2024, 2024
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Air pollution levels across northern India are amongst some of the worst in the world, with episodic and hazardous haze events. Here, the ability of the WRF-Chem model to predict air quality over northern India is assessed against several datasets. Whilst surface wind speed and particle pollution peaks are over- and underestimated, respectively, meteorology and aerosol trends are adequately captured, and we conclude it is suitable for investigating severe particle pollution events.
George Jordan, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, Anton Laakso, and James Haywood
Atmos. Chem. Phys., 24, 1939–1960, https://doi.org/10.5194/acp-24-1939-2024, https://doi.org/10.5194/acp-24-1939-2024, 2024
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The 2014–15 Holuhraun eruption caused a huge aerosol plume in an otherwise unpolluted region, providing a chance to study how aerosol alters cloud properties. This two-part study uses observations and models to quantify this relationship’s impact on the Earth’s energy budget. Part 1 suggests the models capture the observed spatial and chemical evolution of the plume, yet no model plume is exact. Understanding these differences is key for Part 2, where changes to cloud properties are explored.
Lin Du, Xiaofan Lv, Makroni Lily, Kun Li, and Narcisse Tsona Tchinda
Atmos. Chem. Phys., 24, 1841–1853, https://doi.org/10.5194/acp-24-1841-2024, https://doi.org/10.5194/acp-24-1841-2024, 2024
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This study explores the pH effect on the reaction of dissolved SO2 with selected organic peroxides. Results show that the formation of organic and/or inorganic sulfate from these peroxides strongly depends on their electronic structures, and these processes are likely to alter the chemical composition of dissolved organic matter in different ways. The rate constants of these reactions exhibit positive pH and temperature dependencies within pH 1–10 and 240–340 K ranges.
Angelo Riccio and Elena Chianese
Atmos. Chem. Phys., 24, 1673–1689, https://doi.org/10.5194/acp-24-1673-2024, https://doi.org/10.5194/acp-24-1673-2024, 2024
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Starting from the Copernicus Atmosphere Monitoring Service (CAMS), we provided a novel ensemble statistical post-processing approach to improve their air quality predictions. Our approach is able to provide reliable short-term forecasts of pollutant concentrations, which is a key challenge in supporting national authorities in their tasks related to EU Air Quality Directives, such as planning and reporting the state of air quality to the citizens.
Stella E. I. Manavi and Spyros N. Pandis
Atmos. Chem. Phys., 24, 891–909, https://doi.org/10.5194/acp-24-891-2024, https://doi.org/10.5194/acp-24-891-2024, 2024
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Organic vapors of intermediate volatility have often been neglected as sources of atmospheric organic aerosol. In this work we use a new approach for their simulation and quantify the contribution of these compounds emitted by transportation sources (gasoline and diesel vehicles) to particulate matter over Europe. The estimated secondary organic aerosol levels are on average 60 % higher than predicted by previous approaches. However, these estimates are probably lower limits.
Zhiyuan Li, Kin-Fai Ho, Harry Fung Lee, and Steve Hung Lam Yim
Atmos. Chem. Phys., 24, 649–661, https://doi.org/10.5194/acp-24-649-2024, https://doi.org/10.5194/acp-24-649-2024, 2024
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This study developed an integrated model framework for accurate multi-air-pollutant exposure assessments in high-density and high-rise cities. Following the proposed integrated model framework, we established multi-air-pollutant exposure models for four major PM10 chemical species as well as four criteria air pollutants with R2 values ranging from 0.73 to 0.93. The proposed framework serves as an important tool for combined exposure assessment in epidemiological studies.
Yujin Jo, Myoseon Jang, Sanghee Han, Azad Madhu, Bonyoung Koo, Yiqin Jia, Zechen Yu, Soontae Kim, and Jinsoo Park
Atmos. Chem. Phys., 24, 487–508, https://doi.org/10.5194/acp-24-487-2024, https://doi.org/10.5194/acp-24-487-2024, 2024
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The CAMx–UNIPAR model simulated the SOA budget formed via multiphase reactions of hydrocarbons and the impact of emissions and climate on SOA characteristics under California’s urban environments during winter 2018. SOA growth was dominated by daytime oxidation of long-chain alkanes and nighttime terpene oxidation with O3 and NO−3 radicals. The spatial distributions of anthropogenic SOA were affected by the northwesterly wind, whereas those of biogenic SOA were insensitive to wind directions.
Peter Huszar, Alvaro Patricio Prieto Perez, Lukáš Bartík, Jan Karlický, and Anahi Villalba-Pradas
Atmos. Chem. Phys., 24, 397–425, https://doi.org/10.5194/acp-24-397-2024, https://doi.org/10.5194/acp-24-397-2024, 2024
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Urbanization transforms rural land into artificial land, while due to human activities, it also introduces a great quantity of emissions. We quantify the impact of urbanization on the final particulate matter pollutant levels by looking not only at these emissions, but also at the way urban land cover influences meteorological conditions, how the removal of pollutants changes due to urban land cover, and how biogenic emissions from vegetation change due to less vegetation in urban areas.
Yinbao Jin, Yiming Liu, Xiao Lu, Xiaoyang Chen, Ao Shen, Haofan Wang, Yinping Cui, Yifei Xu, Siting Li, Jian Liu, Ming Zhang, Yingying Ma, and Qi Fan
Atmos. Chem. Phys., 24, 367–395, https://doi.org/10.5194/acp-24-367-2024, https://doi.org/10.5194/acp-24-367-2024, 2024
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This study aims to address these issues by evaluating eight independent biomass burning (BB) emission inventories (GFED, FINN1.5, FINN2.5 MOS, FINN2.5 MOSVIS, GFAS, FEER, QFED, and IS4FIRES) using the WRF-Chem model and analyzing their impact on aerosol optical properties (AOPs) and direct radiative forcing (DRF) during wildfire events in peninsular Southeast Asia (PSEA) that occurred in March 2019.
Hamza Ahsan, Hailong Wang, Jingbo Wu, Mingxuan Wu, Steven J. Smith, Susanne Bauer, Harrison Suchyta, Dirk Olivié, Gunnar Myhre, Hitoshi Matsui, Huisheng Bian, Jean-François Lamarque, Ken Carslaw, Larry Horowitz, Leighton Regayre, Mian Chin, Michael Schulz, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Vaishali Naik
Atmos. Chem. Phys., 23, 14779–14799, https://doi.org/10.5194/acp-23-14779-2023, https://doi.org/10.5194/acp-23-14779-2023, 2023
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We examine the impact of the assumed effective height of SO2 injection, SO2 and BC emission seasonality, and the assumed fraction of SO2 emissions injected as SO4 on climate and chemistry model results. We find that the SO2 injection height has a large impact on surface SO2 concentrations and, in some models, radiative flux. These assumptions are a
hiddensource of inter-model variability and may be leading to bias in some climate model results.
Zhen Peng, Lili Lei, Zhe-Min Tan, Meigen Zhang, Aijun Ding, and Xingxia Kou
Atmos. Chem. Phys., 23, 14505–14520, https://doi.org/10.5194/acp-23-14505-2023, https://doi.org/10.5194/acp-23-14505-2023, 2023
Short summary
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Annual PM2.5 emissions in China consistently decreased by about 3% to 5% from 2017 to 2020 with spatial variations and seasonal dependencies. High-temporal-resolution and dynamics-based PM2.5 emission estimates provide quantitative diurnal variations for each season. Significant reductions in PM2.5 emissions in the North China Plain and northeast of China in 2020 were caused by COVID-19.
Stylianos Kakavas, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13555–13564, https://doi.org/10.5194/acp-23-13555-2023, https://doi.org/10.5194/acp-23-13555-2023, 2023
Short summary
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Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out 1-year aerosol simulations over the continental US. We show that such organic water impacts can increase dry PM1 levels by up to 2 μg m-3 when RH levels and PM1 concentrations are high.
Benjamin N. Murphy, Darrell Sonntag, Karl M. Seltzer, Havala O. T. Pye, Christine Allen, Evan Murray, Claudia Toro, Drew R. Gentner, Cheng Huang, Shantanu Jathar, Li Li, Andrew A. May, and Allen L. Robinson
Atmos. Chem. Phys., 23, 13469–13483, https://doi.org/10.5194/acp-23-13469-2023, https://doi.org/10.5194/acp-23-13469-2023, 2023
Short summary
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We update methods for calculating organic particle and vapor emissions from mobile sources in the USA. Conventionally, particulate matter (PM) and volatile organic carbon (VOC) are speciated without consideration of primary semivolatile emissions. Our methods integrate state-of-the-science speciation profiles and correct for common artifacts when sampling emissions in a laboratory. We quantify impacts of the emission updates on ambient pollution with the Community Multiscale Air Quality model.
Yanshun Li, Randall V. Martin, Chi Li, Brian L. Boys, Aaron van Donkelaar, Jun Meng, and Jeffrey R. Pierce
Atmos. Chem. Phys., 23, 12525–12543, https://doi.org/10.5194/acp-23-12525-2023, https://doi.org/10.5194/acp-23-12525-2023, 2023
Short summary
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We developed and evaluated processes affecting within-day (diel) variability in PM2.5 concentrations in a chemical transport model over the contiguous US. Diel variability in PM2.5 for the contiguous US is driven by early-morning accumulation into a shallow mixed layer, decreases from mid-morning through afternoon with mixed-layer growth, increases from mid-afternoon through evening as the mixed-layer collapses, and decreases overnight as emissions decrease.
Chupeng Zhang, Shangfei Hai, Yang Gao, Yuhang Wang, Shaoqing Zhang, Lifang Sheng, Bin Zhao, Shuxiao Wang, Jingkun Jiang, Xin Huang, Xiaojing Shen, Junying Sun, Aura Lupascu, Manish Shrivastava, Jerome D. Fast, Wenxuan Cheng, Xiuwen Guo, Ming Chu, Nan Ma, Juan Hong, Qiaoqiao Wang, Xiaohong Yao, and Huiwang Gao
Atmos. Chem. Phys., 23, 10713–10730, https://doi.org/10.5194/acp-23-10713-2023, https://doi.org/10.5194/acp-23-10713-2023, 2023
Short summary
Short summary
New particle formation is an important source of atmospheric particles, exerting critical influences on global climate. Numerical models are vital tools to understanding atmospheric particle evolution, which, however, suffer from large biases in simulating particle numbers. Here we improve the model chemical processes governing particle sizes and compositions. The improved model reveals substantial contributions of newly formed particles to climate through effects on cloud condensation nuclei.
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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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