Articles | Volume 16, issue 5
https://doi.org/10.5194/acp-16-2819-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-2819-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
04 Mar 2016
Research article |
| 04 Mar 2016
The impact of snow nitrate photolysis on boundary layer chemistry and the recycling and redistribution of reactive nitrogen across Antarctica and Greenland in a global chemical transport model
Maria Zatko
Department of Atmospheric Sciences, University of Washington, Seattle,
USA
Lei Geng
Department of Atmospheric Sciences, University of Washington, Seattle,
USA
Department of Atmospheric Sciences, University of Washington, Seattle,
USA
Eric Sofen
Department of Atmospheric Sciences, University of Washington, Seattle,
USA
now at: MathWorks, Natick, MA, USA
Katarina Klein
Division of Glaciology, Alfred Wegener Institute Helmholtz Centre for
Polar and Marine Research, Bremerhaven, Germany
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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.
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.
Michael Oluwatoyin Sunday, Laura Marie Dahler Heinlein, Junwei He, Allison Moon, Sukriti Kapur, Ting Fang, Kasey C. Edwards, Fangzhou Guo, Jack Dibb, James H. Flynn III, Becky Alexander, Manabu Shiraiwa, and Cort Anastasio
EGUsphere, https://doi.org/10.5194/egusphere-2024-3272, https://doi.org/10.5194/egusphere-2024-3272, 2024
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Hydrogen peroxide (HOOH) is an important oxidant that forms atmospheric sulfate. We demonstrate that illumination of brown carbon can rapidly form HOOH within particles, even under the low sunlight conditions of Fairbanks, Alaska during winter. This in-particle formation of HOOH is fast enough that it forms sulfate at significant rates. In contrast, the formation of HOOH in the gas phase during the campaign is expected to be negligible because of high NOx levels.
Ursula A. Jongebloed, Jacob I. Chalif, Linia Tashmim, William C. Porter, Kelvin H. Bates, Qianjie Chen, Erich C. Osterberg, Bess G. Koffman, Jihong Cole-Dai, Dominic A. Winksi, David G. Ferris, Karl J. Kreutz, Cameron P. Wake, and Becky Alexander
EGUsphere, https://doi.org/10.5194/egusphere-2024-3026, https://doi.org/10.5194/egusphere-2024-3026, 2024
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Marine phytoplankton emit dimethyl sulfide (DMS), which forms methanesulfonic acid (MSA) and sulfate. MSA concentrations in ice cores decreased over the industrial era, which has been attributed to pollution-driven changes in DMS chemistry. We use a models to investigate DMS chemistry compared to observations of DMS, MSA, and sulfate. We find that modeled DMS, MSA, and sulfate are influenced by pollution-sensitive oxidant concentrations, characterization of DMS chemistry, and other variables.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonne, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1450, https://doi.org/10.5194/egusphere-2024-1450, 2024
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Processes influencing dispersion of local anthropogenic emissions in Arctic wintertime are investigated with dispersion model simulations. Modelled power plant plume rise that considers surface and elevated temperature inversions improves results compared to observations. Modelled near-surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching -35 °C are required to reproduce observed NOx.
Zhuang Jiang, Becky Alexander, Joel Savarino, and Lei Geng
Atmos. Chem. Phys., 24, 4895–4914, https://doi.org/10.5194/acp-24-4895-2024, https://doi.org/10.5194/acp-24-4895-2024, 2024
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Ice-core nitrate could track the past atmospheric NOx and oxidant level, but its interpretation is hampered by the post-depositional processing. In this work, an inverse model was developed and tested against two polar sites and was shown to well reproduce the observed nitrate signals in snow and atmosphere, suggesting that the model can properly correct for the effect of post-depositional processing. This model offers a very useful tool for future studies on ice-core nitrate records.
Linia Tashmim, William C. Porter, Qianjie Chen, Becky Alexander, Charles H. Fite, Christopher D. Holmes, Jeffrey R. Pierce, Betty Croft, and Sakiko Ishino
Atmos. Chem. Phys., 24, 3379–3403, https://doi.org/10.5194/acp-24-3379-2024, https://doi.org/10.5194/acp-24-3379-2024, 2024
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Dimethyl sulfide (DMS) is mostly emitted from ocean surfaces and represents the largest natural source of sulfur for the atmosphere. Once in the atmosphere, DMS forms stable oxidation products such as SO2 and H2SO4, which can subsequently contribute to airborne particle formation and growth. In this study, we update the DMS oxidation mechanism in the chemical transport model GEOS-Chem and describe resulting changes in particle growth as well as the overall global sulfur budget.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
Atmos. Chem. Phys., 22, 14467–14488, https://doi.org/10.5194/acp-22-14467-2022, https://doi.org/10.5194/acp-22-14467-2022, 2022
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Radical bromine molecules are seen at higher concentrations during the Arctic spring. We use the global model GEOS-Chem to test whether snowpack and wind-blown snow sources can explain high bromine concentrations. We run this model for the entire year of 2015 and compare results to observations of bromine from floating platforms on the Arctic Ocean and at Utqiaġvik. We find that the model performs best when both sources are enabled but may overestimate bromine production in summer and fall.
Yanzhi Cao, Zhuang Jiang, Becky Alexander, Jihong Cole-Dai, Joel Savarino, Joseph Erbland, and Lei Geng
Atmos. Chem. Phys., 22, 13407–13422, https://doi.org/10.5194/acp-22-13407-2022, https://doi.org/10.5194/acp-22-13407-2022, 2022
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We investigate the potential of ice-core preserved nitrate isotopes as proxies of stratospheric ozone variability by measuring nitrate isotopes in a shallow ice core from the South Pole. The large variability in the snow accumulation rate and its slight increase after the 1970s masked any signals caused by the ozone hole. Moreover, the nitrate oxygen isotope decrease may reflect changes in the atmospheric oxidation environment in the Southern Ocean.
Zhuang Jiang, Joel Savarino, Becky Alexander, Joseph Erbland, Jean-Luc Jaffrezo, and Lei Geng
The Cryosphere, 16, 2709–2724, https://doi.org/10.5194/tc-16-2709-2022, https://doi.org/10.5194/tc-16-2709-2022, 2022
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A record of year-round atmospheric nitrate isotopic composition along with snow nitrate isotopic data from Summit, Greenland, revealed apparent enrichments in nitrogen isotopes in snow nitrate compared to atmospheric nitrate, in addition to a relatively smaller degree of changes in oxygen isotopes. The results suggest that at this site post-depositional processing takes effect, which should be taken into account when interpreting ice-core nitrate isotope records.
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.
Jiayue Huang, Lyatt Jaeglé, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mat J. Evans, Nicolas Theys, and Sungyeon Choi
Atmos. Chem. Phys., 20, 7335–7358, https://doi.org/10.5194/acp-20-7335-2020, https://doi.org/10.5194/acp-20-7335-2020, 2020
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Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often observed in the springtime Arctic. Here, we use a chemical transport model to examine the role of sea salt aerosol from blowing snow in explaining these phenomena. We find that our simulation can account for the spatiotemporal variability of satellite observations of BrO. However, the model has difficulty in producing the magnitude of observed ozone depletion events.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Mark O. Battle, J. William Munger, Margaret Conley, Eric Sofen, Rebecca Perry, Ryan Hart, Zane Davis, Jacob Scheckman, Jayme Woogerd, Karina Graeter, Samuel Seekins, Sasha David, and John Carpenter
Atmos. Chem. Phys., 19, 8687–8701, https://doi.org/10.5194/acp-19-8687-2019, https://doi.org/10.5194/acp-19-8687-2019, 2019
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Predictions of global warming require predictions of how much CO2 will be taken up by the oceans, how much by land plants, and how much will stay in the atmosphere. Measurements of atmospheric oxygen (O2) help with these predictions if we also know the ratio of O2 release to CO2 uptake in land plants. We have measured this ratio in a midlatitude forest and find a lower value than the one in wide use. If truly applicable, our results call for a modest adjustment in the global carbon budget.
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
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Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Qianjie Chen, Tomás Sherwen, Mathew Evans, and Becky Alexander
Atmos. Chem. Phys., 18, 13617–13637, https://doi.org/10.5194/acp-18-13617-2018, https://doi.org/10.5194/acp-18-13617-2018, 2018
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Uncertainty in the natural tropospheric sulfur cycle represents the largest source of uncertainty in radiative forcing estimates of sulfate aerosol. This study investigates the natural sulfur cycle in the marine troposphere using the GEOS-Chem model. We found that BrO is important for DMS oxidation and multiphase chemistry is important for MSA production and loss, which have implications for the yield of SO2 and MSA from DMS oxidation and the radiative effect of DMS-derived sulfate aerosol.
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.
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.
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.
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.
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.
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.
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. 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
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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ACEIC: a comprehensive anthropogenic chlorine emission inventory for China
Impact of methane and other precursor emission reductions on surface ozone in Europe: scenario analysis using the European Monitoring and Evaluation Programme (EMEP) Meteorological Synthesizing Centre – West (MSC-W) model
Verifying national inventory-based combustion emissions of CO2 across the UK and mainland Europe using satellite observations of atmospheric CO and CO2
An improved estimate of inorganic iodine emissions from the ocean using a coupled surface microlayer box model
Impact of improved representation of volatile organic compound emissions and production of NOx reservoirs on modeled urban ozone production
The effect of different climate and air quality policies in China on in situ ozone production in Beijing
Assessing the relative impacts of satellite ozone and its precursor observations to improve global tropospheric ozone analysis using multiple chemical reanalysis systems
Evaluating present-day and future impacts of agricultural ammonia emissions on atmospheric chemistry and climate
Enhancing long-term trend simulation of the global tropospheric hydroxyl (TOH) and its drivers from 2005 to 2019: a synergistic integration of model simulations and satellite observations
Intercomparison of GEOS-Chem and CAM-chem tropospheric oxidant chemistry within the Community Earth System Model version 2 (CESM2)
Development of a detailed gaseous oxidation scheme of naphthalene for secondary organic aerosol (SOA) formation and speciation
Air pollution satellite-based CO2 emission inversion: system evaluation, sensitivity analysis, and future perspective
Anthropogenic emission controls reduce summertime ozone-temperature sensitivity in the United States
Large contributions of soil emissions to the atmospheric nitrogen budget and their impacts on air quality and temperature rise in North China
Why did ozone concentrations remain high during Shanghai's static management? A statistical and radical-chemistry perspective
Impact of introducing electric vehicles on ground-level O3 and PM2.5 in the Greater Tokyo Area: Yearly trends and the importance of changes in the Urban Heat Island effect
Revising VOC emissions speciation improves the simulation of global background ethane and propane
Changes in South American surface ozone trends: exploring the influences of precursors and extreme events
Evaluating NOx stack plume emissions using a high-resolution atmospheric chemistry model and satellite-derived NO2 columns
NOx emissions in France in 2019–2021 as estimated by the high-spatial-resolution assimilation of TROPOMI NO2 observations
Urban ozone formation and sensitivities to volatile chemical products, cooking emissions, and NOx across the Los Angeles Basin
Aggravated surface O3 pollution primarily driven by meteorological variations in China during the 2020 COVID-19 pandemic lockdown period
Identifying decadal trends in deweathered concentrations of criteria air pollutants in Canadian urban atmospheres with machine learning approaches
Evaluation of modelled versus observed non-methane volatile organic compounds at European Monitoring and Evaluation Programme sites in Europe
Constraining non-methane VOC emissions with TROPOMI HCHO observations: impact on summertime ozone simulation in August 2022 in China
Insights on ozone pollution control in urban areas by decoupling meteorological factors based on machine learning
Revealing the significant acceleration of hydrofluorocarbon (HFC) emissions in eastern Asia through long-term atmospheric observations
Interpreting Geostationary Environment Monitoring Spectrometer (GEMS) geostationary satellite observations of the diurnal variation in nitrogen dioxide (NO2) over East Asia
An intercomparison of satellite, airborne, and ground-level observations with WRF–CAMx simulations of NO2 columns over Houston, Texas, during the September 2021 TRACER-AQ campaign
Investigating processes influencing simulation of local Arctic wintertime anthropogenic pollution in Fairbanks, Alaska during ALPACA-2022
Interannual variability of summertime formaldehyde (HCHO) vertical column density and its main drivers at northern high latitudes
The impact of multi-decadal changes in VOC speciation on urban ozone chemistry: a case study in Birmingham, United Kingdom
Technical note: Challenges in detecting free tropospheric ozone trends in a sparsely sampled environment
Combined assimilation of NOAA surface and MIPAS satellite observations to constrain the global budget of carbonyl sulfide
Thibaut Lebourgeois, Bastien Sauvage, Pawel Wolff, Béatrice Josse, Virginie Marécal, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Jean-Marc Cousin, Philippe Nedelec, and Valérie Thouret
Atmos. Chem. Phys., 24, 13975–14004, https://doi.org/10.5194/acp-24-13975-2024, https://doi.org/10.5194/acp-24-13975-2024, 2024
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Our study examines intense-carbon-monoxide (CO) pollution events measured by commercial aircraft from the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. We combine these measurements with the SOFT-IO model to trace the origin of the observed CO. A comprehensive analysis of the geographical origin, source type, seasonal variation, and ozone levels of these pollution events is provided.
Hassnae Erraji, Philipp Franke, Astrid Lampert, Tobias Schuldt, Ralf Tillmann, Andreas Wahner, and Anne Caroline Lange
Atmos. Chem. Phys., 24, 13913–13934, https://doi.org/10.5194/acp-24-13913-2024, https://doi.org/10.5194/acp-24-13913-2024, 2024
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Four-dimensional variational data assimilation allows for the simultaneous optimisation of initial values and emission rates by using trace-gas profiles from drone observations in a regional air quality model. Assimilated profiles positively impact the representation of air pollutants in the model by improving their vertical distribution and ground-level concentrations. This case study highlights the potential of drone data to enhance air quality analyses including local emission evaluation.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
Atmos. Chem. Phys., 24, 13693–13713, https://doi.org/10.5194/acp-24-13693-2024, https://doi.org/10.5194/acp-24-13693-2024, 2024
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This work uses chemical transport and box modeling to study the gas- and aqueous-phase production of organic acid concentrations measured in cloud water at the summit of Whiteface Mountain on 1 July 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas-phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
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Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William R. Stockwell, Luc Vereecken, and Timothy J. Wallington
Atmos. Chem. Phys., 24, 13317–13339, https://doi.org/10.5194/acp-24-13317-2024, https://doi.org/10.5194/acp-24-13317-2024, 2024
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Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes in the atmospheric composition. Therefore, accurate chemical mechanisms are necessary to predict the evolution of air pollution and climate change. The article describes all steps that are needed to build chemical mechanisms and discusses the advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 24, 12943–12962, https://doi.org/10.5194/acp-24-12943-2024, https://doi.org/10.5194/acp-24-12943-2024, 2024
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This paper employs a regional chemical transport model to quantify the sensitivity of air pollutants and photochemical parameters to specified emission reductions in China for representative winter and summer conditions. The study provides insights into further air quality control in China with reduced primary emissions.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Baoshuang Liu, Yao Gu, Yutong Wu, Qili Dai, Shaojie Song, Yinchang Feng, and Philip K. Hopke
Atmos. Chem. Phys., 24, 12861–12879, https://doi.org/10.5194/acp-24-12861-2024, https://doi.org/10.5194/acp-24-12861-2024, 2024
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Reactive loss of volatile organic compounds (VOCs) is a long-term issue yet to be resolved in VOC source analyses. We assess common methods of, and existing issues in, reducing losses, impacts of losses, and sources in current source analyses. We offer a potential supporting role for solving issues of VOC conversion. Source analyses of consumed VOCs that reacted to produce ozone and secondary organic aerosols can play an important role in the effective control of secondary pollution in air.
Deepangsu Chatterjee, Randall V. Martin, Chi Li, Dandan Zhang, Haihui Zhu, Daven K. Henze, James H. Crawford, Ronald C. Cohen, Lok N. Lamsal, and Alexander M. Cede
Atmos. Chem. Phys., 24, 12687–12706, https://doi.org/10.5194/acp-24-12687-2024, https://doi.org/10.5194/acp-24-12687-2024, 2024
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We investigate the hourly variation of NO2 columns and surface concentrations by applying the GEOS-Chem model to interpret aircraft and ground-based measurements over the US and Pandora sun photometer measurements over the US, Europe, and Asia. Corrections to the Pandora columns and finer model resolution improve the modeled representation of the summertime hourly variation of total NO2 columns to explain the weaker hourly variation in NO2 columns than at the surface.
Kiyeon Kim, Kyung Man Han, Chul Han Song, Hyojun Lee, Ross Beardsley, Jinhyeok Yu, Greg Yarwood, Bonyoung Koo, Jasper Madalipay, Jung-Hun Woo, and Seogju Cho
Atmos. Chem. Phys., 24, 12575–12593, https://doi.org/10.5194/acp-24-12575-2024, https://doi.org/10.5194/acp-24-12575-2024, 2024
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We incorporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratio predictions. These results expand our understanding of HONO photochemistry and identify crucial sources of HONO that impact the total HONO budget in Seoul, South Korea. Through this investigation, we contribute to resolving discrepancies in understanding chemical transport models, with implications for better air quality management and environmental protection in the region.
Flossie Brown, Gerd Folberth, Stephen Sitch, Paulo Artaxo, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Matteo Detto, Ninong Komala, Luciana Rizzo, Nestor Rojas, Ines dos Santos Vieira, Steven Turnock, Hans Verbeeck, and Alfonso Zambrano
Atmos. Chem. Phys., 24, 12537–12555, https://doi.org/10.5194/acp-24-12537-2024, https://doi.org/10.5194/acp-24-12537-2024, 2024
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Ozone is a pollutant that is detrimental to human and plant health. Ozone monitoring sites in the tropics are limited, so models are often used to understand ozone exposure. We use measurements from the tropics to evaluate ozone from the UK Earth system model, UKESM1. UKESM1 is able to capture the pattern of ozone in the tropics, except in southeast Asia, although it systematically overestimates it at all sites. This work highlights that UKESM1 can capture seasonal and hourly variability.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys., 24, 12495–12507, https://doi.org/10.5194/acp-24-12495-2024, https://doi.org/10.5194/acp-24-12495-2024, 2024
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Climate change will bring about changes in parameters that are currently used in global-scale models to calculate biogenic emissions. This study seeks to understand the factors driving these models by comparing long-term datasets of biogenic compounds to modeled emissions. We note that the light-dependent fractions currently used in models do not accurately represent regional observations. We provide evidence for the time-dependent variation in this parameter for future modifications to models.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyoung Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
Atmos. Chem. Phys., 24, 12465–12493, https://doi.org/10.5194/acp-24-12465-2024, https://doi.org/10.5194/acp-24-12465-2024, 2024
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We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show that SF6 emissions are decreasing in the USA and in the EU, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, EU, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
Yasin Elshorbany, Jerald R. Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo J. Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca R. Buchholz, Benjamin Gaubert, Néstor Y. Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
Atmos. Chem. Phys., 24, 12225–12257, https://doi.org/10.5194/acp-24-12225-2024, https://doi.org/10.5194/acp-24-12225-2024, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the tropospheric column of ozone and its precursors, nitrogen dioxide, formaldehyde, and total column CO, as well as ozonesonde data and model simulations.
Mariano Mertens, Sabine Brinkop, Phoebe Graf, Volker Grewe, Johannes Hendricks, Patrick Jöckel, Anna Lanteri, Sigrun Matthes, Vanessa S. Rieger, Mattia Righi, and Robin N. Thor
Atmos. Chem. Phys., 24, 12079–12106, https://doi.org/10.5194/acp-24-12079-2024, https://doi.org/10.5194/acp-24-12079-2024, 2024
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We quantified the contributions of land transport, shipping, and aviation emissions to tropospheric ozone; its radiative forcing; and the reductions of the methane lifetime using chemistry-climate model simulations. The contributions were analysed for the conditions of 2015 and for three projections for the year 2050. The results highlight the challenges of mitigating ozone formed by emissions of the transport sector, caused by the non-linearitiy of the ozone chemistry and the long lifetime.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Siting Li, Yiming Liu, Yuqi Zhu, Yinbao Jin, Yingying Hong, Ao Shen, Yifei Xu, Haofan Wang, Haichao Wang, Xiao Lu, Shaojia Fan, and Qi Fan
Atmos. Chem. Phys., 24, 11521–11544, https://doi.org/10.5194/acp-24-11521-2024, https://doi.org/10.5194/acp-24-11521-2024, 2024
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This study establishes an inventory of anthropogenic chlorine emissions in China in 2019 with expanded species (HCl, Cl-, Cl2, HOCl) and sources (41 specific sources). The inventory is validated by a modeling study against the observations. This study enhances the understanding of anthropogenic chlorine emissions in the atmosphere, identifies key sources, and provides scientific support for pollution control and climate change.
Willem E. van Caspel, Zbigniew Klimont, Chris Heyes, and Hilde Fagerli
Atmos. Chem. Phys., 24, 11545–11563, https://doi.org/10.5194/acp-24-11545-2024, https://doi.org/10.5194/acp-24-11545-2024, 2024
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Methane in the atmosphere contributes to the production of ozone gas – an air pollutant and greenhouse gas. Our results highlight that simultaneous reductions in methane emissions help avoid offsetting the air pollution benefits already achieved by the already-approved precursor emission reductions by 2050 in the European Monitoring and Evaluation Programme region, while also playing an important role in bringing air pollution further down towards World Health Organization guideline limits.
Tia R. Scarpelli, Paul I. Palmer, Mark Lunt, Ingrid Super, and Arjan Droste
Atmos. Chem. Phys., 24, 10773–10791, https://doi.org/10.5194/acp-24-10773-2024, https://doi.org/10.5194/acp-24-10773-2024, 2024
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Under the Paris Agreement, countries must track their anthropogenic greenhouse gas emissions. This study describes a method to determine self-consistent estimates for combustion emissions and natural fluxes of CO2 from atmospheric data. We report consistent estimates inferred using this approach from satellite data and ground-based data over Europe, suggesting that satellite data can be used to determine national anthropogenic CO2 emissions for countries where ground-based CO2 data are absent.
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 9899–9921, https://doi.org/10.5194/acp-24-9899-2024, https://doi.org/10.5194/acp-24-9899-2024, 2024
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Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterize and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
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Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Beth S. Nelson, Zhenze Liu, Freya A. Squires, Marvin Shaw, James R. Hopkins, Jacqueline F. Hamilton, Andrew R. Rickard, Alastair C. Lewis, Zongbo Shi, and James D. Lee
Atmos. Chem. Phys., 24, 9031–9044, https://doi.org/10.5194/acp-24-9031-2024, https://doi.org/10.5194/acp-24-9031-2024, 2024
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The impact of combined air quality and carbon neutrality policies on O3 formation in Beijing was investigated. Emissions inventory data were used to estimate future pollutant mixing ratios relative to ground-level observations. O3 production was found to be most sensitive to changes in alkenes, but large reductions in less reactive compounds led to larger reductions in future O3 production. This study highlights the importance of understanding the emissions of organic pollutants.
Takashi Sekiya, Emanuele Emili, Kazuyuki Miyazaki, Antje Inness, Zhen Qu, R. Bradley Pierce, Dylan Jones, Helen Worden, William Y. Y. Cheng, Vincent Huijnen, and Gerbrand Koren
EGUsphere, https://doi.org/10.5194/egusphere-2024-2426, https://doi.org/10.5194/egusphere-2024-2426, 2024
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Five global chemical reanalysis datasets were used to assess the relative impacts of assimilating satellite ozone and its precursors measurements on tropospheric ozone analyses for 2010. The multiple reanalysis system comparison allows for evaluating dependency of the impacts on different reanalysis systems. The results suggested the importance of satellite ozone and its precursor measurements for improving ozone analysis in the whole troposphere, with varying the magnitudes among the systems.
Maureen Beaudor, Didier Hauglustaine, Juliette Lathière, Martin Van Damme, Lieven Clarisse, and Nicolas Vuichard
EGUsphere, https://doi.org/10.5194/egusphere-2024-2022, https://doi.org/10.5194/egusphere-2024-2022, 2024
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Agriculture is the biggest ammonia (NH3) source, impacting air quality, climate, and ecosystems. Because of food demand, NH3 emissions are projected to rise by 2100. Using a global model, we analyzed the impact of present and future NH3 emissions generated from a land model. Our results show improved ammonia patterns compared to a reference inventory. Future scenarios predict up to 70 % increase in global NH3 burden, significant changes in radiative forcing, and could significantly elevate N2O.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
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We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
Atmos. Chem. Phys., 24, 8607–8624, https://doi.org/10.5194/acp-24-8607-2024, https://doi.org/10.5194/acp-24-8607-2024, 2024
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Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone, but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side by side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
Victor Lannuque and Karine Sartelet
Atmos. Chem. Phys., 24, 8589–8606, https://doi.org/10.5194/acp-24-8589-2024, https://doi.org/10.5194/acp-24-8589-2024, 2024
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation and speciation from naphthalene oxidation. This study details the development of the first near-explicit chemical scheme for naphthalene oxidation by OH, which includes kinetic and mechanistic data, and is able to reproduce most of the experimentally identified products in both gas and particle phases.
Hui Li, Jiaxin Qiu, and Bo Zheng
EGUsphere, https://doi.org/10.5194/egusphere-2024-1986, https://doi.org/10.5194/egusphere-2024-1986, 2024
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We conduct a sensitivity analysis on various factors including prior, model resolution, satellite constraint, and inversion system configuration to assess the vulnerability of emission estimates across temporal, sectoral, and regional dimensions. Our analysis first reveals the robustness of emissions estimated by this air pollution satellite sensor-based CO2 emission inversion system, with relative change between tests and Base inversion below 4.0 % for national annual NOx and CO2 emissions.
Shuai Li, Xiao Lu, and Haolin Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1889, https://doi.org/10.5194/egusphere-2024-1889, 2024
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We report that the summertime ozone-temperature sensitivity decreased by 50 % from 3.0 ppbv/K in 1990 to 1.5 ppb/K in 2021 in the US. GEOS-Chem simulations show that anthropogenic NOx emission reduction is the dominant driver of the ozone-temperature sensitivity decline, through influencing both the temperature-direct and temperature-indirect processes. Reduced ozone-temperature sensitivity has decreased the ozone enhancement from low to high temperatures by an average of 6.8 ppbv across the US.
Tong Sha, Siyu Yang, Qingcai Chen, Liangqing Li, Xiaoyan Ma, Yan-Lin Zhang, Zhaozhong Feng, K. Folkert Boersma, and Jun Wang
Atmos. Chem. Phys., 24, 8441–8455, https://doi.org/10.5194/acp-24-8441-2024, https://doi.org/10.5194/acp-24-8441-2024, 2024
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Using an updated soil reactive nitrogen emission scheme in the Unified Inputs for Weather Research and Forecasting coupled with Chemistry (UI-WRF-Chem) model, we investigate the role of soil NO and HONO (Nr) emissions in air quality and temperature in North China. Contributions of soil Nr emissions to O3 and secondary pollutants are revealed, exceeding effects of soil NOx or HONO emission. Soil Nr emissions play an important role in mitigating O3 pollution and addressing climate change.
Jian Zhu, Shanshan Wang, Chuanqi Gu, Zhiwen Jiang, Sanbao Zhang, Ruibin Xue, Yuhao Yan, and Bin Zhou
Atmos. Chem. Phys., 24, 8383–8395, https://doi.org/10.5194/acp-24-8383-2024, https://doi.org/10.5194/acp-24-8383-2024, 2024
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In 2022, Shanghai implemented city-wide static management measures during the high-ozone season in April and May, providing a chance to study ozone pollution control. Despite significant emissions reductions, ozone levels increased by 23 %. Statistically, the number of days with higher ozone diurnal variation types increased during the lockdown period. The uneven decline in VOC and NO2 emissions led to heightened photochemical processes, resulting in the observed ozone level rise.
Hiroo Hata, Norifumi Mizushima, and Tomohiko Ihara
EGUsphere, https://doi.org/10.5194/egusphere-2024-1961, https://doi.org/10.5194/egusphere-2024-1961, 2024
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The introduction of battery electric vehicles (BEV) is expected to reduce the primary air pollutants from vehicular exhaust and evaporative emissions while reducing the anthropogenic heat produced by vehicles, ultimately decreasing the urban heat island effect (UHI). This study revealed the impact of introducing BEVs on the decrease in UHI and the effects of BEVs on the formation of tropospheric ozone and fine particulate matter in the Greater Tokyo Area of Japan.
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
Atmos. Chem. Phys., 24, 8317–8342, https://doi.org/10.5194/acp-24-8317-2024, https://doi.org/10.5194/acp-24-8317-2024, 2024
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Ethane and propane are volatile organic compounds emitted from human activities which help to form ozone, a pollutant and greenhouse gas, and also affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job of reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emissions, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
Rodrigo J. Seguel, Lucas Castillo, Charlie Opazo, Néstor Y. Rojas, Thiago Nogueira, María Cazorla, Mario Gavidia-Calderón, Laura Gallardo, René Garreaud, Tomás Carrasco-Escaff, and Yasin Elshorbany
Atmos. Chem. Phys., 24, 8225–8242, https://doi.org/10.5194/acp-24-8225-2024, https://doi.org/10.5194/acp-24-8225-2024, 2024
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Trends of surface ozone were examined across South America. Our findings indicate that ozone trends in major South American cities either increase or remain steady, with no signs of decline. The upward trends can be attributed to chemical regimes that efficiently convert nitric oxide into nitrogen dioxide. Additionally, our results suggest a climate penalty for ozone driven by meteorological conditions that favor wildfire propagation in Chile and extensive heat waves in southern Brazil.
Maarten Krol, Bart van Stratum, Isidora Anglou, and Klaas Folkert Boersma
Atmos. Chem. Phys., 24, 8243–8262, https://doi.org/10.5194/acp-24-8243-2024, https://doi.org/10.5194/acp-24-8243-2024, 2024
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This paper presents detailed plume simulations of nitrogen oxides and carbon dioxide that are emitted from four large industrial facilities world-wide. Results from the high-resolution simulations that include atmospheric chemistry are compared to nitrogen dioxide observations from satellites. We find good performance of the model and show that common assumptions that are used in simplified models need revision. This work is important for the monitoring of emissions using satellite data.
Robin Plauchu, Audrey Fortems-Cheiney, Grégoire Broquet, Isabelle Pison, Antoine Berchet, Elise Potier, Gaëlle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, and Henk Eskes
Atmos. Chem. Phys., 24, 8139–8163, https://doi.org/10.5194/acp-24-8139-2024, https://doi.org/10.5194/acp-24-8139-2024, 2024
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This study uses the Community Inversion Framework and CHIMERE model to assess the potential of TROPOMI-S5P PAL NO2 tropospheric column data to estimate NOx emissions in France (2019–2021). Results show a 3 % decrease in average emissions compared to the 2016 CAMS-REG/INS, lower than the 14 % decrease from CITEPA. The study highlights challenges in capturing emission anomalies due to limited data coverage and error levels but shows promise for local inventory improvements.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2024-1899, https://doi.org/10.5194/egusphere-2024-1899, 2024
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In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking are important sources that impact air quality. This study used a model to evaluate how these emissions impact ozone in the Los Angeles Basin, and quantifies the impact of gaseous cooking emissions for the first time. Accurate representation of these and other man-made sources in inventories is crucial to inform effective air quality policies.
Zhendong Lu, Jun Wang, Yi Wang, Daven K. Henze, Xi Chen, Tong Sha, and Kang Sun
Atmos. Chem. Phys., 24, 7793–7813, https://doi.org/10.5194/acp-24-7793-2024, https://doi.org/10.5194/acp-24-7793-2024, 2024
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In contrast with past work showing that the reduction of emissions was the dominant factor for the nationwide increase of surface O3 during the lockdown in China, this study finds that the variation in meteorology (temperature and other parameters) plays a more important role. This result is obtained through sensitivity simulations using a chemical transport model constrained by satellite (TROPOMI) data and calibrated with surface observations.
Xiaohong Yao and Leiming Zhang
Atmos. Chem. Phys., 24, 7773–7791, https://doi.org/10.5194/acp-24-7773-2024, https://doi.org/10.5194/acp-24-7773-2024, 2024
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This study investigates long-term trends of criteria air pollutants, including NO2, CO, SO2, O3 and PM2.5, and NO2+O3 measured in 10 Canadian cities during the last 2 to 3 decades. We also investigate associated driving forces in terms of emission reductions, perturbations from varying weather conditions and large-scale wildfires, as well as changes in O3 sources and sinks.
Yao Ge, Sverre Solberg, Mathew R. Heal, Stefan Reimann, Willem van Caspel, Bryan Hellack, Thérèse Salameh, and David Simpson
Atmos. Chem. Phys., 24, 7699–7729, https://doi.org/10.5194/acp-24-7699-2024, https://doi.org/10.5194/acp-24-7699-2024, 2024
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Atmospheric volatile organic compounds (VOCs) constitute many species, acting as precursors to ozone and aerosol. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the EMEP MSC-W to evaluate emission inventories in Europe. We focus on the varying agreement between modelled and measured VOCs across different species and underscore potential inaccuracies in total and sector-specific emission estimates.
Shuzhuang Feng, Fei Jiang, Tianlu Qian, Nan Wang, Mengwei Jia, Songci Zheng, Jiansong Chen, Fang Ying, and Weimin Ju
Atmos. Chem. Phys., 24, 7481–7498, https://doi.org/10.5194/acp-24-7481-2024, https://doi.org/10.5194/acp-24-7481-2024, 2024
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We developed a multi-air-pollutant inversion system to estimate non-methane volatile organic compound (NMVOC) emissions using TROPOMI formaldehyde retrievals. We found that the inversion significantly improved formaldehyde simulations and reduced NMVOC emission uncertainties. The optimized NMVOC emissions effectively corrected the overestimation of O3 levels, mainly by decreasing the rate of the RO2 + NO reaction and increasing the rate of the NO2 + OH reaction.
Yuqing Qiu, Xin Li, Wenxuan Chai, Yi Liu, Mengdi Song, Xudong Tian, Qiaoli Zou, Wenjun Lou, Wangyao Zhang, Juan Li, and Yuanhang Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1576, https://doi.org/10.5194/egusphere-2024-1576, 2024
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The chemical reactions of ozone (O3) formation are related to meteorology and local emissions. Here, a random forest approach was used to eliminate the effects of meteorological factors (dispersion or transport) on O3 and its precursors. Variations in the sensitivity of O3 formation and the apportionment of emission sources were revealed after meteorological normalization. Our results suggest that meteorological variations should be considered when diagnosing O3 formation.
Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, and Sunyoung Park
Atmos. Chem. Phys., 24, 7309–7330, https://doi.org/10.5194/acp-24-7309-2024, https://doi.org/10.5194/acp-24-7309-2024, 2024
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We analyzed with an inversion model the atmospheric abundance of hydrofluorocarbons (HFCs), potent greenhouse gases, from 2008 to 2020 at Gosan station in South Korea and revealed a significant increase in emissions, especially from eastern China and Japan. This increase contradicts reported data, underscoring the need for accurate monitoring and reporting. Our findings are crucial for understanding and managing global HFCs emissions, highlighting the importance of efforts to reduce HFCs.
Laura Hyesung Yang, Daniel J. Jacob, Ruijun Dang, Yujin J. Oak, Haipeng Lin, Jhoon Kim, Shixian Zhai, Nadia K. Colombi, Drew C. Pendergrass, Ellie Beaudry, Viral Shah, Xu Feng, Robert M. Yantosca, Heesung Chong, Junsung Park, Hanlim Lee, Won-Jin Lee, Soontae Kim, Eunhye Kim, Katherine R. Travis, James H. Crawford, and Hong Liao
Atmos. Chem. Phys., 24, 7027–7039, https://doi.org/10.5194/acp-24-7027-2024, https://doi.org/10.5194/acp-24-7027-2024, 2024
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The Geostationary Environment Monitoring Spectrometer (GEMS) provides hourly measurements of NO2. We use the chemical transport model to find how emissions, chemistry, and transport drive the changes in NO2 observed by GEMS at different times of the day. In winter, the chemistry plays a minor role, and high daytime emissions dominate the diurnal variation in NO2, balanced by transport. In summer, emissions, chemistry, and transport play an important role in shaping the diurnal variation in NO2.
M. Omar Nawaz, Jeremiah Johnson, Greg Yarwood, Benjamin de Foy, Laura Judd, and Daniel L. Goldberg
Atmos. Chem. Phys., 24, 6719–6741, https://doi.org/10.5194/acp-24-6719-2024, https://doi.org/10.5194/acp-24-6719-2024, 2024
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NO2 is a gas with implications for air pollution. A campaign conducted in Houston provided an opportunity to compare NO2 from different instruments and a model. Aircraft and satellite observations agreed well with measurements on the ground; however, the latter estimated lower values. We find that model-simulated NO2 was lower than observations, especially downtown, suggesting that NO2 sources associated with the urban core of Houston, such as vehicle emissions, may be underestimated.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonne, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1450, https://doi.org/10.5194/egusphere-2024-1450, 2024
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Processes influencing dispersion of local anthropogenic emissions in Arctic wintertime are investigated with dispersion model simulations. Modelled power plant plume rise that considers surface and elevated temperature inversions improves results compared to observations. Modelled near-surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching -35 °C are required to reproduce observed NOx.
Tianlang Zhao, Jingqiu Mao, Zolal Ayazpour, Gonzalo González Abad, Caroline R. Nowlan, and Yiqi Zheng
Atmos. Chem. Phys., 24, 6105–6121, https://doi.org/10.5194/acp-24-6105-2024, https://doi.org/10.5194/acp-24-6105-2024, 2024
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HCHO variability is a key tracer in understanding VOC emissions in response to climate change. We investigate the role of methane oxidation and biogenic and wildfire emissions in HCHO interannual variability over northern high latitudes in summer, emphasizing wildfires as a key driver of HCHO interannual variability in Alaska, Siberia and northern Canada using satellite HCHO and SIF retrievals and then GEOS-Chem model. We show SIF is a tool to understand biogenic HCHO variability in this region.
Jianghao Li, Alastair C. Lewis, Jim R. Hopkins, Stephen J. Andrews, Tim Murrells, Neil Passant, Ben Richmond, Siqi Hou, William J. Bloss, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 24, 6219–6231, https://doi.org/10.5194/acp-24-6219-2024, https://doi.org/10.5194/acp-24-6219-2024, 2024
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A summertime ozone event at an urban site in Birmingham is sensitive to volatile organic compounds (VOCs) – particularly those of oxygenated VOCs. The roles of anthropogenic VOC sources in urban ozone chemistry are examined by integrating the 1990–2019 national atmospheric emission inventory into model scenarios. Road transport remains the most powerful means of further reducing ozone in this case study, but the benefits may be offset if solvent emissions of VOCs continue to increase.
Kai-Lan Chang, Owen R. Cooper, Audrey Gaudel, Irina Petropavlovskikh, Peter Effertz, Gary Morris, and Brian C. McDonald
Atmos. Chem. Phys., 24, 6197–6218, https://doi.org/10.5194/acp-24-6197-2024, https://doi.org/10.5194/acp-24-6197-2024, 2024
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A great majority of observational trend studies of free tropospheric ozone use sparsely sampled ozonesonde and aircraft measurements as reference data sets. A ubiquitous assumption is that trends are accurate and reliable so long as long-term records are available. We show that sampling bias due to sparse samples can persistently reduce the trend accuracy, and we highlight the importance of maintaining adequate frequency and continuity of observations.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Cited articles
Allen, D., Pickering, K., Duncan, B., and Damon, M.: Impact of lightning NO
emissions on North American photochemistry as determined using the Global
Modeling Initiative (GMI) model, J. Geophys. Res., 115, D22301,
https://doi.org/10.1029/2010JD014062, 2010.
Alexander, B., Savarino, J., Kreutz, K. J., and Thiemens, M. H.: Impact of
preindustrial biomass burning emissions on the oxidation pathways of
tropospheric sulphur and nitrogen, J. Geophys. Res., 109, D08303,
https://doi.org/10.1029/2003JD004218, 2004.
Amos, H. M., Jacob, D. J., Holmes, C. D., Fisher, J. A., Wang, Q., Yantosca,
R. M., Corbitt, E. S., Galarneau, E., Rutter, A. P., Gustin, M. S., Steffen,
A., Schauer, J. J., Graydon, J. A., Louis, V. L. St., Talbot, R. W.,
Edgerton, E. S., Zhang, Y., and Sunderland, E. M.: Gas-particle partitioning
of atmospheric Hg(II) and its effect on global mercury deposition, Atmos.
Chem. Phys., 12, 591–603, https://doi.org/10.5194/acp-12-591-2012, 2012.
Anastasio, C. and Chu, L.: Photochemistry of nitrous acid (HONO) and nitrous
acidium ion (H2ONO+) in aqueous solution and ice, Environ. Sci.
Technol., 43, 1108–1114, 2009.
Beine, H., Anastastio, C., Esposito, G., Patten, K., Wilkening, E.,
Domine, F., Voisin, D., Barret, M., Houdier, S., and Hall, S.: Soluble,
light-absorbing species in snow at Barrow, Alaska, J. Geophys. Res., 116,
D00R05, https://doi.org/10.1029/2011JD016181, 2011.
Bergin, M. H., Jaffrezo, J.-L., Davidson, C. I., Dibb, J. E., Pandis, S. N.,
Hillamo, R., Maenhaut, M., Kuhns, H. D., and Makela, T.: The contributions of
snow, fog, and dry deposition to the summer flux of anions and cations at
Summit, Greenland, J. Geophys. Res., 100, 16275–16288, 1995.
Berhanu, T. A., Meusinger, C., Erbland, J., Jost, R., Bhattcharya, S. K.,
Johnson, M. S., and Savarino, J.: Laboratory study of nitrate photolysis in
Antarctic snow. I I. Isotopic effects and wavelength dependence, J. Chem.
Phys., 140, 244306, https://doi.org/10.1063/1.4882899, 2014.
Bey, I., Jacob, D. J., Yantosca, R. M., Logan, J. A., Field, B. D.,
Fiore, A. M., Li, Q., Liu, H. Y., Mickley, L. J., and Schultz, M. G.: Global
modeling of tropospheric chemistry with assimilated meteorology: model
description and evaluation, J. Geophys. Res., 106, 23073–23095, 2001.
Bian, H. S. and Prather, M. J.: Fast-J2: Accurate simulation of stratospheric
photolysis in global chemical models, J. Atmos. Chem., 41, 281–296, 2002.
Bloss, W. J., Lee, J. D., Heard, D. E., Salmon, R. A., Bauguitte, S. J.-B.,
Roscoe, H. K., and Jones, A. E.: Observations of OH and HO2 radicals in
coastal Antarctica, Atmos. Chem. Phys., 7, 4171–4185,
https://doi.org/10.5194/acp-7-4171-2007, 2007.
Blunier, T., Gregoire, F. L., Jacobi, H.-W., and Quansah, E.: Isotopic view
on nitrate loss in Antarctic surface snow, Geophys. Res. Lett., 32, L13501,
https://doi.org/10.1029/2005GL023011, 2005.
Boxe, C. S., Colussi, A. J., Hoffmann, M. R., Murphy, J. G.,
Wolldridge, P. J., Bertram, T. H., and Cohen, R. C.: Photochemical production
and release of gaseous NO2 from nitrate-doped water ice, J. Phys. Chem.
A, 109, 8520–8525, 2005.
Burkhart, J. F., Bales, R. C., McConnell, J. R., Hutterli, M. A., and Frey,
M. M.: Geographic variability of nitrate deposition and preservation over the
Greenland ice sheet, J. Geophys. Res., 114, D06301, https://doi.org/10.1029/2008JD010600,
2009.
Casasanta, G., Pietroni, I., Petenko, I., and Argentini, S.: Observed and
modelled convective mixing-layer height and Dome C, Antarctica, Bound.-Lay.
Meteorol., 151, 597–608, https://doi.org/10.1007/s10546-014-9907-5, 2014.
Chen, G., Davis, D., Crawford, J., Hutterli, L. M., Huey, L. G., Slusher, D.,
Mauldin, L., Eisele, F., Tanner, D., Dibb, J., Buhr, M., McConnell, J.,
Lefer, B., Shetter, R., Blake, D., Song, C. H., Lombardi, K., and
Arnoldy, J.: A reassessment of HOx South Pole chemistry based on
observations recorded during ISCAT 2000, Atmos. Environ., 38, 5451–5461,
2004.
Chen, G., Huey, L. G., Crawford, J. H., Olson, J. R., Hutterli, M. A.,
Sjostedt, S., Tanner, D., Dibb, J., Lefer, B., Blake, N., Davis, D., and
Stohl, A.: An assessment of the polar HOx photochemical budget based on
2003 Summit Greenland Field Observations, Atmos. Environ., 41, 7806–7820,
2007.
Cho, H., Shepson, P. B., Barrie, L. A., Cowin, J. P., and Zaveri, R.: NMR
investigation of the quasi-brine layer in ice/brine mixtures, J. Phys.
Chem. B., 106, 11226–11232, 2002.
Chu, L. and Anastasio. C.: Quantum yields of hydroxyl radicals and nitrogen
dioxide from the photolysis of nitrate on ice, J. Phys. Chem. A, 107,
9594–9602, 2003.
Cohen, L., Helmig, D., Neff, W. D., Grachev, A. A., and Fairall, C. W.:
Boundary-layer dynamics and its influence on atmospheric chemistry at Summit,
Greenland, Atmos. Environ., 41, 5044–5060, 2007.
Davidson, C. I., Harrington, J. R., Stephenson, M. J., Small, M. J., Boscoe,
F. P., and Gandley, R. E.: Seasonal variations in sulfate, nitrate, and
chloride in the Greenland ice sheet: relation to atmospheric concentrations,
Atmos. Environ., 23, 2483–2493, 1989.
Davis, D., Chen, G., Buhr, M., Crawford, J., Lenschow, D., Lefer, B.,
Shetter, R., Eisele, F., Mauldin, L., and Hogan, A.: South Pole NOx
chemistry: an assessment of factors controlling variability and absolute
levels, Atmos. Environ., 38, 5375–5388, 2004.
Davis, D. D., Seelig, J., Huey, G., Crawford, J., Chen, G., Wang, Y.,
Buhr, M., Helmig, D., Neff, W., Blake, D., Arimoto, R., and Eisele, F.:
A reassessment of Antarctic plateau reactive nitrogen based on ANTCI 2003
airborne and ground based measurements, Atmos. Environ., 42, 2831–2848,
https://doi.org/10.1016/j.atmosenv.2007.07.039, 2008.
Dibb, J. E., Talbot, R. W., and Bergin, M. H.: Soluble acidic species in air
and snow at Summit, Greenland, Geophys. Res. Lett., 21, 1627–1630, 1994.
Dibb, J. E., Huey, G. L., Slusher, D. L., and Tanner, D. J.: Soluble reactive
nitrogen oxides at South Pole during ISCAT 2000, Atmos. Environ., 38,
5399–5409, 2004.
Dibb, J. E., Whitlow, S. I., and Arsenault, M.: Seasonal variations in the
soluble ion content of snow at Summit, Greenland: constraints from three
years of daily surface snow samples, Atmos. Environ., 41, 5007–5019,
https://doi.org/10.1016/j.atmosenv.2006.12.010, 2007.
Doherty, S. J., Warren, S. G., Grenfell, T. C., Clarke, A. D., and Brandt, R.
E.: Light-absorbing impurities in Arctic snow, Atmos. Chem. Phys., 10,
11647–11680, https://doi.org/10.5194/acp-10-11647-2010, 2010.
Doherty, S. J., Grenfell, T. C., Forsstrom, S., Hegg, D. L., Brandt, R. E.,
and Warren, S. G.: Observed vertical redistribution of black carbon and other
insoluble light-absorbing particles in melting snow, J. Geophys. Res.-Atmos.,
118, 5553–5569, https://doi.org/10.1002/jgrd.50235, 2013.
Domine, F. and Shepson, P. B.: Air-snow interactions and atmospheric
chemistry, Science, 297, 1506–1510, 2002.
Domine, F., Bock, J., Voisin, D., and Donaldson, D. J.: Can we model snow
photochemistry? Problems with the current approaches, J. Phys. Chem. A, 117,
4733–4749, https://doi.org/10.1021/jp3123314, 2013.
Drue, C. and Heinemann, G.: Characteristics of intermittent turbulence in the
upper stable boundary layer over Greenland, Boundary-Layer Meteorol., 124,
361–381, https://doi.org/10.1007/s10546-007-9175-8, 2007.
Erbland, J., Vicars, W. C., Savarino, J., Morin, S., Frey, M. M., Frosini,
D., Vince, E., and Martins, J. M. F.: Air-snow transfer of nitrate on the
East Antarctic Plateau – Part 1: Isotopic evidence for a photolytically
driven dynamic equilibrium in summer, Atmos. Chem. Phys., 13, 6403–6419,
https://doi.org/10.5194/acp-13-6403-2013, 2013.
Erbland, J., Savarino, J., Morin, S., France, J. L., Frey, M. M., and King,
M. D.: Air-snow transfer of nitrate on the East Antarctic Plateau – Part 2:
An isotopic model for the interpretation of deep ice-core records, Atmos.
Chem. Phys., 15, 12079–12113, https://doi.org/10.5194/acp-15-12079-2015, 2015.
Fisher, J. A., Jacob, D. J., Wang, Q., Bahreini, R., Carouge, C. C.,
Cubison, M. J., Dibb, J. E., Diehl, T., Jimenez, J. L., Leibensperger, E. M.,
Meinders, M. B. T., Pye, H. O. T., Quinn, P. K., Sharma, S., van
Donkelaar, A., and Yantosca, R. M.: Sources, distribution, and acidity of
sulfate-ammonium aerosol in the Arctic in winter-spring, Atmos. Environ., 45,
7301–7318, 2011.
Frey, M. M., Savarino, J., Morin, S., Erbland, J., and Martins, J. M. F.:
Photolysis imprint in the nitrate stable isotope signal in snow and
atmosphere of East Antarctica and implications for reactive nitrogen cycling,
Atmos. Chem. Phys., 9, 8681–8696, https://doi.org/10.5194/acp-9-8681-2009, 2009.
Frey, M. M., Brough, N., France, J. L., Anderson, P. S., Traulle, O., King,
M. D., Jones, A. E., Wolff, E. W., and Savarino, J.: The diurnal variability
of atmospheric nitrogen oxides (NO and NO2) above the Antarctic Plateau
driven by atmospheric stability and snow emissions, Atmos. Chem. Phys., 13,
3045–3062, https://doi.org/10.5194/acp-13-3045-2013, 2013.
Freyer, H. D., Kley, D., Voiz-Thomas, A., and Kobel, K.: On the interaction
of isotopic exchange processes with photochemical reactions in atmospheric
oxides of nitrogen, J. Geophys. Res.-Atmos., 98, 14791–14796, 1993.
Gallet, J.-C., Domine, F., Arnaud, L., Picard, G., and Savarino, J.: Vertical
profile of the specific surface area and density of the snow at Dome C and on
a transect to Dumont D'Urville, Antarctica –albedo calculations and
comparison to remote sensing products, The Cryosphere, 5, 631–649,
https://doi.org/10.5194/tc-5-631-2011, 2011.
Geng, L., Alexander, B., Cole-Dai, J., Steig, E. J., Savarino, J.,
Sofen, E. D., and Schauer, A. J.: Nitrogen isotopes in ice core nitrate
linked to anthropogenic atmospheric acidity change, P. Natl. Acad. Sci., 111,
5808–5812, https://doi.org/10.1073/pnas.1319441111, 2014a.
Geng, L., Cole-Dai, J., Alexander, B., Erbland, J., Savarino, J., Schauer, A.
J., Steig, E. J., Lin, P., Fu, Q., and Zatko, M. C.: On the origin of the
occasional spring nitrate peak in Greenland snow, Atmos. Chem. Phys., 14,
13361–13376, https://doi.org/10.5194/acp-14-13361-2014, 2014b.
Geng, L., Zatko, M. C., Alexander, B., Fudge, T. J., Schauer, A. J., Murray,
L. T., and Mickley, L. J.: Effects of post-depositional processing on
nitrogen isotopes of nitrate in the Greenland Ice Sheet Project 2 (GISP2) ice
core, Geophys. Res. Lett., 42, 5346–5354, https://doi.org/10.1002/2015GL064218, 2015.
Grannas, A. M., Jones, A. E., Dibb, J., Ammann, M., Anastasio, C.,
Beine, H. J., Bergin, M., Bottenheim, J., Boxe, C. S., Carver, G., Chen, G.,
Crawford, J. H., Dominé, F., Frey, M. M., Guzmán, M. I.,
Heard, D. E., Helmig, D., Hoffmann, M. R., Honrath, R. E., Huey, L. G.,
Hutterli, M., Jacobi, H. W., Klán, P., Lefer, B., McConnell, J.,
Plane, J., Sander, R., Savarino, J., Shepson, P. B., Simpson, W. R.,
Sodeau, J. R., von Glasow, R., Weller, R., Wolff, E. W., and Zhu, T.: An
overview of snow photochemistry: evidence, mechanisms and impacts, Atmos.
Chem. Phys., 7, 4329–4373, https://doi.org/10.5194/acp-7-4329-2007, 2007.
Grenfell, T. C.: A radiative transfer model for sea ice with vertical
structure variations, J. Geophys. Res., 96, 16991–17001, 1991.
Grenfell, T. C., Warren, S. G., and Mullen, P. C.: Reflection of solar
radiation by the Antarctic snow surface at ultraviolet, visible, and
near-infrared wavelengths, J. Geophys. Res., 99, 18669–18684, 1994.
Handorf, D., Foken, T., and Kottmeier, C.: The stable atmospheric boundary
layer over an Antarctic ice sheet, Bound.-Lay. Meteorol., 91, 165–189, 1999.
Hastings, M. G., Steig, E. J., and Sigman, D. M.: Seasonal variations in N
and O isotopes of nitrate in snow at Summit, Greenland: Implications for the
study of nitrate in snow and ice cores, J. Geophys. Res., 109, D20306,
https://doi.org/10.1029/2004JD004991, 2004.
Hastings, M. G., Sigman, D. M., and Steig, E. J.: Glacial/interglacial
changes in the isotopes of nitrate from the Greenland Ice Sheet Project
(GISP2) ice core, Global Biogeochem. Cy., 19, GB4024,
https://doi.org/10.1029/2005GB002502, 2005.
Heaton, T. H. E., Spiro, B., and Robertson, M. C. S.: Potential canopy
influences on the isotopic composition of nitrogen and sulphur in atmospheric
deposition, Oecologia, 109, 600–607, 1997.
Helmig, D., Boulter, J., David, D., Birks, J. W., Cullen, N. J., Steffen, K.,
Johnson, B. J., and Oltmans, S. J.: Ozone and meteorological boundary-layer
conditions at Summit, Greenland, during 3-21 2000, Atmos. Environ., 36,
2595–2608, 2002.
Helmig, D., Johnson, B., Oltmans, S. J., Neff, W., Eisele, F., and Davis, D.:
Elevated ozone in the boundary layer at South Pole, Atmos. Environ., 42,
2788–2803, 2008.
Holtslag, A. A. M. and Boville, B.: Local versus nonlocal boundary layer
diffusion in a global climate model, J. Climate, 6, 1825–1842, 1993.
Honrath, R. E., Lu, Y., Peterson, M. C., Dibb, J. E., Arsenault, M. A.,
Cullen, N. J., and Steffen, K.: Vertical fluxes of NOx, HONO, and
HNO3 above the snowpack at Summit, Greenland, Atmos. Environ., 36,
2629–2640, 2002.
Hudman, R. C., Moore, N. E., Mebust, A. K., Martin, R. V., Russell, A. R.,
Valin, L. C., and Cohen, R. C.: Steps towards a mechanistic model of global
soil nitric oxide emissions: implementation and space based-constraints,
Atmos. Chem. Phys., 12, 7779–7795, https://doi.org/10.5194/acp-12-7779-2012, 2012.
Jarvis, J. C., Hastings, M. G., Steig, E. J., and Kunasek, S. A.: Isotopic
ratios in gas-phase HNO3 and snow nitrate at Summit, Greenland, J.
Geophys. Res., 114, D17301, https://doi.org/10.1029/2009JD012134, 2009.
Jin, Z., Charlock, T. P., Yang, P., Xie, Y., and Miller, W.: Snow optical
properties for different particle shapes with application to snow grain size
retrieval and MODIS/CERES radiance comparison over Antarctica, Remote. Sens.
Environ., 112, 3563–3581, 2008.
Jones, A. E., Anderson, P. S., Wolff, E. W., Turner, J., Rankin, A. M., and
Colwell, S. R.: A role for newly forming sea ice in springtime polar
tropospheric ozone loss? Observational evidence from Halley station,
Antarctica, J. Geophys. Res., 111, D08306, https://doi.org/10.1029/2005JD006566, 2006.
Jones, A. E., Wolff, E. W., Salmon, R. A., Bauguitte, S. J.-B.,
Roscoe, H. K., Anderson, P. S., Ames, D., Clemitshaw, K. C., Fleming, Z. L.,
Bloss, W. J., Heard, D. E., Lee, J. D., Read, K. A., Hamer, P.,
Shallcross, D. E., Jackson, A. V., Walker, S. L., Lewis, A. C., Mills, G. P.,
Plane, J. M. C., Saiz-Lopez, A., Sturges, W. T., and Worton, D. R.: Chemistry
of the Antarctic Boundary Layer and the Interface with Snow: an overview of
the CHABLIS campaign, Atmos. Chem. Phys., 8, 3789–3803,
https://doi.org/10.5194/acp-8-3789-2008, 2008.
King, J. C., Argentini, S. A., and Anderson, P. S.: Contrasts between the
summertime surface energy balance and boundary layer structure at Dome C and
Halley stations, Antarctica, J. Geophys. Res., 111, D02105,
https://doi.org/10.1029/2005JD006130, 2006.
Klein, K.: Variability in Dry Antarctic Firn; Investigations on Spatially
Distributed Snow and Firn Samples from Dronning Maud Land, Antarctica, PhD
thesis, Universität Bremen, Germany, available at:
http://nbn-resolving.de/urn:nbn:de:gbv:46-00104117-15, last access:
15 April 2014.
Kodama, Y., Wendler, G., and Ishikawa, N.: The diurnal variation of the
boundary layer in summer in Adelie Land, Eastern Antarctica, J. Appl.
Meteorol., 28, 16–24, 1989.
Konig-Langlo, G., King, J., and Pettre, P.: Climatology of the three coastal
Antarctic stations Durmont D'urville, Neumayer, and Halley, J. Geophys. Res.,
103, 10935–10946, 1998.
Lee, H., Henze, D. K., Alexander, B., and Murray, L. T.: Investigating the
sensitivity of surface-level nitrate seasonality in Antarctica to primary
sources using a global model, Atmos. Environ., 89, 757–767,
https://doi.org/10.1016/j.atmosenv.2014.03.003, 2014.
Legrand, M. R. and Kirchner, S.: Origins and variations of nitrate in South
Polar precipitation, J. Geophys. Res., 95, 3493–3507, 1990.
Levy, H., Moxim, W. J., Klonecki, A. A., and Kasibhatla, P. S.: Simulated
tropospheric NOx: its evaluation, global distribution and individual
source contributions, J. Geophys. Res., 104, 26279–26306, 1999.
Libois, Q., Picard, G., France, J. L., Arnaud, L., Dumont, M., Carmagnola, C.
M., and King, M. D.: Influence of grain shape on light penetration in snow,
The Cryosphere, 7, 1803–1818, https://doi.org/10.5194/tc-7-1803-2013, 2013.
Lin, J. T. and McElroy, M. B.: Impacts of boundary layer mixing on pollutant
vertical profiles in the lower troposphere: Implications to satellite remote
sensing, Atmos. Environ., 44, 1726–1749, https://doi.org/10.1016/j.atmosenv.2010.02.009,
2010.
Liu, H., Jacob, D. J., Bey, I., and Yantosca, R. M.: Constraints from
210Pb and 7Be on wet deposition and transport in a global
three-dimensional chemical tracer model driven by assimilated meteorological
fields, J. Geophys. Res., 106, 12109–12128, 2001.
Logan, J. A.: Nitrogen oxides in the troposphere: global and regional
budgets, J. Geophys. Res., 88, 10785–10807, https://doi.org/10.1029/JC088iC15p10785,
1983.
Mack, J. and Bolton, J. R.: Photochemistry of nitrite and nitrate in aqueous
solution: a review, J. Photoch. Photobio. A, 128, 1–13, 1999.
Mao, J., Jacob, D. J., Evans, M. J., Olson, J. R., Ren, X., Brune, W. H.,
Clair, J. M. St., Crounse, J. D., Spencer, K. M., Beaver, M. R., Wennberg, P.
O., Cubison, M. J., Jimenez, J. L., Fried, A., Weibring, P., Walega, J. G.,
Hall, S. R., Weinheimer, A. J., Cohen, R. C., Chen, G., Crawford, J. H.,
McNaughton, C., Clarke, A. D., Jaeglé, L., Fisher, J. A., Yantosca, R.
M., Le Sager, P., and Carouge, C.: Chemistry of hydrogen oxide radicals
(HOx) in the Arctic troposphere in spring, Atmos. Chem. Phys., 10,
5823–5838, https://doi.org/10.5194/acp-10-5823-2010, 2010.
Mayewski, P. A. and Legrand, M. R.: Recent increase in nitrate concentration
of Antarctic snow, Nature, 346, 258–260, 1990.
Meusinger, C., Berhanu, T. A., Erbland, J., Savarino, J., and Johnson, M. S.:
Laboratory study of nitrate photolysis in Antarctic snow. I. Observed quantum
yield, domain of photolysis, and secondary chemistry, J. Chem. Phys., 140,
244305, https://doi.org/10.1063/1.4882898, 2014.
Morin, S., Savarino, J., Frey, M. M., Domine, F., Jacobi, H.-W.,
Kaleschke, L., and Martins, J. M. F.: Comprehensive isotopic composition of
atmospheric nitrate in the Atlantic Ocean boundary layer from 65° S
to 79° N, J. Geophys. Res., 114, D05303, https://doi.org/10.1029/2008JD010696,
2009.
Mulvaney, R., Wagenbach, D., and Wolff, E. W.: Postdepositional change in
snowpack nitrate from observation of year-round near-surface snow in coastal
Antarctica, J. Geophys. Res., 103, 11021–11031, 1998.
Murray, L. T., Jacob, D. J., Logan, J. A., Hudman, R. C., and Koshak, W. J.:
Optimized regional and interannual variability of lightning in a global
chemical transport model constrained by LIS/OTD satellite data, J. Geophys.
Res., 117, D20307, https://doi.org/10.1029/2012JD017934, 2012.
Neff, W., Helmig, D., Grachev, A., and Davis, D.: A study of boundary layer
behaviour associated with high concentrations at the South Pole using
a minisoder, tethered balloon, and a sonic anemometer, Atmos. Environ., 42,
2762–2779, 2008.
Oliver, J. G. J., Van Aardenne, J. A., Dentener, F. J., Pagliari, V.,
Ganzeveld, L. N., and Peters, J. A. H. W.: Recent trends in global greenhouse
gas emissions: regional trends 1970–2000 and spatial distribution of key
sources in 2000, Environm. Sci., 2, 81–99, https://doi.org/10.1080/15693430500400345,
2005.
Oncley, S., Buhr, M., Lenschow, D., Davis, D., and Semmer, S.: Observations
of summertime NO fluxes and boundary-layer height at the South Pole during
ISCAT 2000 using scalar similarity, Atmos. Environ., 38, 5389–5398,
https://doi.org/10.1016/j.atmosenv.2004.05.053, 2004.
Parish, T. R. and Bromwich, D. H.: Reexamination of the near-surface airflow
over the Antarctic continent and implications on atmospheric circulations at
high southern latitudes, Mon. Weather Rev., 135, 1961–1973, 2007.
Pratt, K. A., Custard, K. D., Shepson, P. B., Douglas, T. A., Pohler, D.,
General, S., Zielcke, J., Simpson, W. R., Platt, U., Tanner, D. J.,
Huey, L. G., Carlsen, M., and Stirm, B. H.: Photochemical production of
molecular bromine in Arctic surface snowpacks, Nature, 6, 351–356,
https://doi.org/10.1038/NGEO1779, 2013.
Price, C. and Rind, D.: A simple lightning parameterization for calculating
global lightning distributions, J. Geophys. Res., 97, 9919–9933, 1992.
Rothlisberger, R., Hutterli, M. A., Sommer, S., Wolff, E. W., and
Mulvaney, R.: Factors controlling nitrate in ice cores: evidence from the
Dome C deep ice core, J. Geophys. Res., 105, 20565–20572, 2000.
Sander, S. P., Friedl, R. R., Golden, D. M., Kurylo, M. J., Moortgat, G. K.,
Keller-Rudek, H., Wine, P. J., Ravishankara, A. R., Kolb, C. E.,
Molina, M. J., Finalyson-Pitts, B. J., Huie, R. E., and Orkin, V. L.:
Chemical kinetics and photochemical data for use in atmospheric studies
evaluation number 15, JPL Publications, 06-2, Pasadena, California, USA,
1–523, 2006.
Savarino, J., Kaiser, J., Morin, S., Sigman, D. M., and Thiemens, M. H.:
Nitrogen and oxygen isotopic constraints on the origin of atmospheric nitrate
in coastal Antarctica, Atmos. Chem. Phys., 7, 1925–1945,
https://doi.org/10.5194/acp-7-1925-2007, 2007.
Shi, G., Buffen, A. M., Hastings, M. G., Li, C., Ma, H., Li, Y., Sun, B., An,
C., and Jiang, S.: Investigation of post-depositional processing of nitrate
in East Antarctic snow: isotopic constraints on photolytic loss,
re-oxidation, and source inputs, Atmos. Chem. Phys., 15, 9435–9453,
https://doi.org/10.5194/acp-15-9435-2015, 2015.
Sjostedt, S. J., Huey, L. G., Tanner, D. J., Peischl, J., Chen, G.,
Dibb, J. E., Lefer, B., Hutterli, M. A., Beyersdorf, A. J., Blake, N. J.,
Blake, D. R., Sueper, D., Ryerson, T., Burkhart, J., and Stohl, A.:
Observations of hydroxul and the sum of peroxy radicals at Summit, Greenland
during summer 2003, Atmos. Environ., 41, 5122–5137, 2007.
Slusher, D. L., Huey, L. G., Tanner, D. J., Chen, G., Davis, D. D., Buhr, M.,
Nowak, J. B., Eisele, F. L., Kosciuch, E., Mauldin, R. L., Lefer, B. L.,
Shetter, R. E., and Dibb, J. E.: Measurements of pernitric acid at the South
Pole during ISCAT 2000, Geophys. Res. Lett., 29, 7-1–7-4,
https://doi.org/10.1029/2002GL015703, 2002.
Sofen, E. D., Alexander, B., Steig, E. J., Thiemens, M. H., Kunasek, S. A.,
Amos, H. M., Schauer, A. J., Hastings, M. G., Bautista, J., Jackson, T. L.,
Vogel, L. E., McConnell, J. R., Pasteris, D. R., and Saltzman, E. S.: WAIS
Divide ice core suggests sustained changes in the atmospheric formation
pathways of sulfate and nitrate since the 19th century in the extratropical
Southern Hemisphere, Atmos. Chem. Phys., 14, 5749–5769,
https://doi.org/10.5194/acp-14-5749-2014, 2014.
Thomas, J. L., Dibb, J. E., Huey, L. G., Liao, J., Tanner, D., Lefer, B., von
Glasow, R., and Stutz, J.: Modeling chemistry in and above snow at Summit,
Greenland – Part 2: Impact of snowpack chemistry on the oxidation capacity of
the boundary layer, Atmos. Chem. Phys., 12, 6537–6554,
https://doi.org/10.5194/acp-12-6537-2012, 2012.
Thompson, A. M.: The oxidizing capacity of the Earth's atmosphere: probable
past and future changes, Science, 256, 1157–1165, 1992.
Travouillon, T., Ashley, M. C. B., Burton, M. G., Storey, J. W. V., and
Loewenstein, R. F.: Atmospheric turbulence at the South Pole and its
implications for astronomy, Astron. Astrophys., 400, 1163–1172,
https://doi.org/10.1051/0004-6361:20021814, 2003.
UNEP/WMO: Integrated Assessment of Black Carbon and Tropospheric Ozone:
Summary for Decision Makers, UNON/Publishing Services Section, Nairobi, ISO
14001:2004, 2011.
van der Werf, G. R., Morton, D. C., DeFries, R. S., Giglio, L., Randerson, J.
T., Collatz, G. J., and Kasibhatla, P. S.: Estimates of fire emissions from
an active deforestation region in the southern Amazon based on satellite data
and biogeochemical modelling, Biogeosciences, 6, 235–249,
https://doi.org/10.5194/bg-6-235-2009, 2009.
van Donkelaar, A., Martin, R. V., Leaitch, W. R., Macdonald, A. M., Walker,
T. W., Streets, D. G., Zhang, Q., Dunlea, E. J., Jimenez, J. L., Dibb, J. E.,
Huey, L. G., Weber, R., and Andreae, M. O.: Analysis of aircraft and
satellite measurements from the Intercontinental Chemical Transport
Experiment (INTEX-B) to quantify long-range transport of East Asian sulfur to
Canada, Atmos. Chem. Phys., 8, 2999–3014, https://doi.org/10.5194/acp-8-2999-2008, 2008.
Walters, W. W., Goodwin, S. R., and Michalski, G.: Nitrogen stable isotope
composition δ15N of vehicle-emitted NOx, Environ. Sci. Tech.,
49, 2278–2285, https://doi.org/10.1021/es505580v, 2015.
Wang, Q., Jacob, D. J., Fisher, J. A., Mao, J., Leibensperger, E. M.,
Carouge, C. C., Le Sager, P., Kondo, Y., Jimenez, J. L., Cubison, M. J., and
Doherty, S. J.: Sources of carbonaceous aerosols and deposited black carbon
in the Arctic in winter-spring: implications for radiative forcing, Atmos.
Chem. Phys., 11, 12453–12473, https://doi.org/10.5194/acp-11-12453-2011, 2011.
Wang, Y., Jacob, D. J., and Logan, J. A.: Global simulation of tropospheric
O3-NOx hydrocarbon chemistry – Part 1: Model formulation, J. Geophys.
Res., 103, 10713–10725, 1998.
Wang, Y., Choi, Y., Zeng, T., Davis, D., Buhr, M., Huey, G. L., and Neff, W.:
Assessing the photochemical impact of snow NOx emissions over Antarctica
during ANTCI 2003, Atmos. Environ., 41, 3944–3958,
https://doi.org/10.1016/j.atmosenv.2007.01.056, 2008.
Weller, R., Minikin, A., Konig-Langlo, G., Schrems, O., Jones, A. E.,
Wolff, E. W., and Anderson, P. S.: Investigating possible causes of the
observed diurnal variability in Antarctic NOy, Geophys. Res. Lett., 26,
2853–2856, 1999.
Wesely, M. L.: Parameterization of surface resistances to gaseous dry
deposition in regional-scale numerical-models, Atmos. Environ., 23,
1293–130, 1989.
Wespes, C., Emmons, L., Edwards, D. P., Hannigan, J., Hurtmans, D., Saunois,
M., Coheur, P.-F., Clerbaux, C., Coffey, M. T., Batchelor, R. L.,
Lindenmaier, R., Strong, K., Weinheimer, A. J., Nowak, J. B., Ryerson, T. B.,
Crounse, J. D., and Wennberg, P. O.: Analysis of ozone and nitric acid in
spring and summer Arctic pollution using aircraft, ground-based, satellite
observations and MOZART-4 model: source attribution and partitioning, Atmos.
Chem. Phys., 12, 237–259, https://doi.org/10.5194/acp-12-237-2012, 2012.
Wild, O., Zhu, Q., and Prather, M. J.: Fast-J: accurate simulation of in- and
below-cloud photolysis in global chemical models, J. Atmos. Chem., 37,
245–282, 2000.
Wolff, E. W.: Nitrate in polar ice, in: Ice Core Studies of Global
Biogeochem. Cycles, NATO ASI Ser., Ser. I, 195–224, edited by: Delmas, R.
J., Springer, New York, USA, 1995.
Wolff, E. W., Jones, A. E., Bauguitte, S. J.-B., and Salmon, R. A.: The
interpretation of spikes and trends in concentration of nitrate in polar ice
cores, based on evidence from snow and atmospheric measurements, Atmos. Chem.
Phys., 8, 5627–5634, https://doi.org/10.5194/acp-8-5627-2008, 2008.
Xu, L. and Penner, J. E.: Global simulations of nitrate and ammonium aerosols
and their radiative effects, Atmos. Chem. Phys., 12, 9479–9504,
https://doi.org/10.5194/acp-12-9479-2012, 2012.
Zatko, M. C. and Warren, S. G.: East Antarctic sea ice in spring: spectral
albedo of snow, nilas, frost flowers, and slush; and light-absorbing
impurities in snow, Ann. Glaciol., 56, 53–64, https://doi.org/10.3189/2015AoG69A574,
2015.
Zatko, M. C., Grenfell, T. C., Alexander, B., Doherty, S. J., Thomas, J. L.,
and Yang, X.: The influence of snow grain size and impurities on the vertical
profiles of actinic flux and associated NOx emissions on the Antarctic
and Greenland ice sheets, Atmos. Chem. Phys., 13, 3547–3567,
https://doi.org/10.5194/acp-13-3547-2013, 2013.
Zhang, L., Gong, S., Padro, J., and Barrie, L.: A size-segregated particle
dry deposition scheme for an atmospheric aerosol module, Atmos. Environ., 35,
549–560, 2001.
Zhu, C., Xiang, B., Chu, L. T., and Zhu, L.: 308 nm photolysis of
nitric acid in the gas phase, on aluminum surfaces, and on ice films,
J. Phys. Chem. A., 114, 2561–2568, https://doi.org/10.1021/jp909867a, 2010.
Short summary
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.
We have incorporated an idealized snowpack with a nitrate photolysis parameterization into a...
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