Articles | Volume 14, issue 7
https://doi.org/10.5194/acp-14-3589-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-14-3589-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
09 Apr 2014
Research article |
| 09 Apr 2014
Factors controlling variability in the oxidative capacity of the troposphere since the Last Glacial Maximum
L. T. Murray
School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
now at: Lamont-Doherty Earth Observatory, Columbia University, Palisades, NY, USA
L. J. Mickley
School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
J. O. Kaplan
ARVE Group, École Polytechnique Fédérale de Lausanne, Lausanne, Switzerland
E. D. Sofen
Department of Atmospheric Sciences, University of Washington, Seattle, WA, USA
M. Pfeiffer
ARVE Group, École Polytechnique Fédérale de Lausanne, Lausanne, Switzerland
B. Alexander
Department of Atmospheric Sciences, University of Washington, Seattle, WA, USA
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Jenny A. Fisher, Lee T. Murray, Dylan B. A. Jones, and Nicholas M. Deutscher
Geosci. Model Dev., 10, 4129–4144, https://doi.org/10.5194/gmd-10-4129-2017, https://doi.org/10.5194/gmd-10-4129-2017, 2017
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Michael J. Prather, Xin Zhu, Clare M. Flynn, Sarah A. Strode, Jose M. Rodriguez, Stephen D. Steenrod, Junhua Liu, Jean-Francois Lamarque, Arlene M. Fiore, Larry W. Horowitz, Jingqiu Mao, Lee T. Murray, Drew T. Shindell, and Steven C. Wofsy
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Lu Shen, Loretta J. Mickley, and Lee T. Murray
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Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonné, 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
Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, https://doi.org/10.5194/acp-25-1063-2025, 2025
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Processes influencing dispersion of local anthropogenic pollution in Arctic wintertime are investigated with Lagrangian dispersion modelling. Simulated power plant plume rise that considers temperature inversion layers improves results compared to observations (interior Alaska). Modelled 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.
Ram Singh, Alexander Koch, Allegra N. LeGrande, Kostas Tsigaridis, Riovie D. Ramos, Francis Ludlow, Igor Aleinov, Reto Ruedy, and Jed O. Kaplan
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2024-219, https://doi.org/10.5194/gmd-2024-219, 2024
Preprint under review for GMD
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This study presents and demonstrates an experimental framework for asynchronous land-atmosphere coupling using the NASA GISS ModelE and LPJ-LMfire models for the 2.5ka period. This framework addresses the limitation of NASA ModelE, which does not have a fully dynamic vegetation model component. It also shows the role of model performance metrics, such as model bias and variability, and the simulated climate is evaluated against the multi-proxy paleoclimate reconstructions for the 2.5ka climate.
William J. Collins, Fiona M. O'Connor, Connor R. Barker, Rachael E. Byrom, Sebastian D. Eastham, Øivind Hodnebrog, Patrick Jöckel, Eloise A. Marais, Mariano Mertens, Gunnar Myhre, Matthias Nützel, Dirk Olivié, Ragnhild Bieltvedt Skeie, Laura Stecher, Larry W. Horowitz, Vaishali Naik, Gregory Faluvegi, Ulas Im, Lee T. Murray, Drew Shindell, Kostas Tsigaridis, Nathan Luke Abraham, and James Keeble
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During the last ice age (21 000 yr BP) in Europe, the composition and extent of forest and its associated climate remain unclear, with models indicating more forest north of the Alps and a warmer and somewhat wetter climate than suggested by the data. A new compilation of pollen records with improved dating suggests greater agreement with model climates but still suggests models overestimate forest cover, especially in the west.
Paul T. Griffiths, Laura J. Wilcox, Robert J. Allen, Vaishali Naik, Fiona M. O'Connor, Michael J. Prather, Alexander T. Archibald, Florence Brown, Makoto Deushi, William Collins, Stephanie Fiedler, Naga Oshima, Lee T. Murray, Christopher J. Smith, Steven T. Turnock, Duncan Watson-Parris, and Paul J. Young
EGUsphere, https://doi.org/10.5194/egusphere-2024-2528, https://doi.org/10.5194/egusphere-2024-2528, 2024
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The Aerosol Chemistry Model Intercomparison Project (AerChemMIP) aimed to quantify the climate and air quality impacts of aerosols and chemically reactive gases. In this paper, we review its contribution to AR6, and the wider understanding of the role of these species in climate and climate change. We identify remaining challenges concluding with recommendations aimed to improve the utility and uptake of climate model data to address the role of short-lived climate forcers in the Earth system.
Benjamin Hmiel, Vasilii V. Petrenko, Christo Buizert, Andrew M. Smith, Michael N. Dyonisius, Philip Place, Bin Yang, Quan Hua, Ross Beaudette, Jeffrey P. Severinghaus, Christina Harth, Ray F. Weiss, Lindsey Davidge, Melisa Diaz, Matthew Pacicco, James A. Menking, Michael Kalk, Xavier Faïn, Alden Adolph, Isaac Vimont, and Lee T. Murray
The Cryosphere, 18, 3363–3382, https://doi.org/10.5194/tc-18-3363-2024, https://doi.org/10.5194/tc-18-3363-2024, 2024
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The main aim of this research is to improve understanding of carbon-14 that is produced by cosmic rays in ice sheets. Measurements of carbon-14 in ice cores can provide a range of useful information (age of ice, past atmospheric chemistry, past cosmic ray intensity). Our results show that almost all (>99 %) of carbon-14 that is produced in the upper layer of ice sheets is rapidly lost to the atmosphere. Our results also provide better estimates of carbon-14 production rates in deeper ice.
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.
Amy Christiansen, Loretta J. Mickley, and Lu Hu
Atmos. Chem. Phys., 24, 4569–4589, https://doi.org/10.5194/acp-24-4569-2024, https://doi.org/10.5194/acp-24-4569-2024, 2024
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In this work, we provide an additional constraint on emissions and trends of nitrogen oxides using nitrate wet deposition (NWD) fluxes over the United States and Europe from 1980–2020. We find that NWD measurements constrain total NOx emissions well. We also find evidence of NOx emission overestimates in both domains, but especially over Europe, where NOx emissions are overestimated by a factor of 2. Reducing NOx emissions over Europe improves model representation of ozone at the surface.
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.
Xu Feng, Loretta J. Mickley, Michelle L. Bell, Tianjia Liu, Jenny A. Fisher, and Maria Val Martin
Atmos. Chem. Phys., 24, 2985–3007, https://doi.org/10.5194/acp-24-2985-2024, https://doi.org/10.5194/acp-24-2985-2024, 2024
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During severe wildfire seasons, smoke can have a significant impact on air quality in Australia. Our study demonstrates that characterization of the smoke plume injection fractions greatly affects estimates of surface smoke PM2.5. Using the plume behavior predicted by the machine learning method leads to the best model agreement with observed surface PM2.5 in key cities across Australia, with smoke PM2.5 accounting for 5 %–52 % of total PM2.5 on average during fire seasons from 2009 to 2020.
Ruijun Dang, Daniel J. Jacob, Viral Shah, Sebastian D. Eastham, Thibaud M. Fritz, Loretta J. Mickley, Tianjia Liu, Yi Wang, and Jun Wang
Atmos. Chem. Phys., 23, 6271–6284, https://doi.org/10.5194/acp-23-6271-2023, https://doi.org/10.5194/acp-23-6271-2023, 2023
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We use the GEOS-Chem model to better understand the magnitude and trend in free tropospheric NO2 over the contiguous US. Model underestimate of background NO2 is largely corrected by considering aerosol nitrate photolysis. Increase in aircraft emissions affects satellite retrievals by altering the NO2 shape factor, and this effect is expected to increase in future. We show the importance of properly accounting for the free tropospheric background in interpreting NO2 observations from space.
Claire Bekker, Wendell W. Walters, Lee T. Murray, and Meredith G. Hastings
Atmos. Chem. Phys., 23, 4185–4201, https://doi.org/10.5194/acp-23-4185-2023, https://doi.org/10.5194/acp-23-4185-2023, 2023
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Nitrate is a critical component of the atmosphere that degrades air quality and ecosystem health. We have investigated the nitrogen isotope compositions of nitrate from deposition samples collected across the northeastern United States. Spatiotemporal variability in the nitrogen isotope compositions was found to track with nitrate formation chemistry. Our results highlight that nitrogen isotope compositions may be a robust tool for improving model representation of nitrate chemistry.
Heejeong Kim, Wendell W. Walters, Claire Bekker, Lee T. Murray, and Meredith G. Hastings
Atmos. Chem. Phys., 23, 4203–4219, https://doi.org/10.5194/acp-23-4203-2023, https://doi.org/10.5194/acp-23-4203-2023, 2023
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Atmospheric nitrate has an important impact on human and ecosystem health. We evaluated atmospheric nitrate formation pathways in the northeastern US utilizing oxygen isotope compositions, which indicated a significant difference between the phases of nitrate (i.e., gas vs. particle). Comparing the observations with model simulations indicated that N2O5 hydrolysis chemistry was overpredicted. Our study has important implications for improving atmospheric chemistry model representation.
Róisín Commane, Andrew Hallward-Driemeier, and Lee T. Murray
Atmos. Meas. Tech., 16, 1431–1441, https://doi.org/10.5194/amt-16-1431-2023, https://doi.org/10.5194/amt-16-1431-2023, 2023
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Methane / ethane ratios can be used to identify and partition the different sources of methane, especially in areas with natural gas mixed with biogenic methane emissions, such as cities. We tested three commercially available laser-based analyzers for sensitivity, precision, size, power requirement, ease of use on mobile platforms, and expertise needed to operate the instrument, and we make recommendations for use in various situations.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Jed O. Kaplan and Katie Hong-Kiu Lau
Earth Syst. Sci. Data, 14, 5665–5670, https://doi.org/10.5194/essd-14-5665-2022, https://doi.org/10.5194/essd-14-5665-2022, 2022
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Global lightning strokes are recorded continuously by a network of ground-based stations. We consolidated these point observations into a map form and provide these as electronic datasets for research purposes. Here we extend our dataset to include lightning observations from 2021.
Amy Christiansen, Loretta J. Mickley, Junhua Liu, Luke D. Oman, and Lu Hu
Atmos. Chem. Phys., 22, 14751–14782, https://doi.org/10.5194/acp-22-14751-2022, https://doi.org/10.5194/acp-22-14751-2022, 2022
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Understanding tropospheric ozone trends is crucial for accurate predictions of future air quality and climate, but drivers of trends are not well understood. We analyze global tropospheric ozone trends since 1980 using ozonesonde and surface measurements, and we evaluate two models for their ability to reproduce trends. We find observational evidence of increasing tropospheric ozone, but models underestimate these increases. This hinders our ability to estimate ozone radiative forcing.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
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.
Liam Bindle, Randall V. Martin, Matthew J. Cooper, Elizabeth W. Lundgren, Sebastian D. Eastham, Benjamin M. Auer, Thomas L. Clune, Hongjian Weng, Jintai Lin, Lee T. Murray, Jun Meng, Christoph A. Keller, William M. Putman, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 14, 5977–5997, https://doi.org/10.5194/gmd-14-5977-2021, https://doi.org/10.5194/gmd-14-5977-2021, 2021
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Atmospheric chemistry models like GEOS-Chem are versatile tools widely used in air pollution and climate studies. The simulations used in such studies can be very computationally demanding, and thus it is useful if the model can simulate a specific geographic region at a higher resolution than the rest of the globe. Here, we implement, test, and demonstrate a new variable-resolution capability in GEOS-Chem that is suitable for simulations conducted on supercomputers.
Lee T. Murray, Eric M. Leibensperger, Clara Orbe, Loretta J. Mickley, and Melissa Sulprizio
Geosci. Model Dev., 14, 5789–5823, https://doi.org/10.5194/gmd-14-5789-2021, https://doi.org/10.5194/gmd-14-5789-2021, 2021
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Chemical-transport models are tools used to study air pollution and inform public policy. However, they are limited by the availability of archived meteorology. Here, we describe how the GEOS-Chem chemical-transport model may now be driven by meteorology archived from a state-of-the-art general circulation model for past and future climates, allowing it to be used to explore the impact of climate change on air pollution and atmospheric composition.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Zhuang Jiang, Becky Alexander, Joel Savarino, Joseph Erbland, and Lei Geng
The Cryosphere, 15, 4207–4220, https://doi.org/10.5194/tc-15-4207-2021, https://doi.org/10.5194/tc-15-4207-2021, 2021
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We used a snow photochemistry model (TRANSITS) to simulate the seasonal nitrate snow profile at Summit, Greenland. Comparisons between model outputs and observations suggest that at Summit post-depositional processing is active and probably dominates the snowpack δ15N seasonality. We also used the model to assess the degree of snow nitrate loss and the consequences in its isotopes at present and in the past, which helps for quantitative interpretations of ice-core nitrate records.
Jed O. Kaplan and Katie Hong-Kiu Lau
Earth Syst. Sci. Data, 13, 3219–3237, https://doi.org/10.5194/essd-13-3219-2021, https://doi.org/10.5194/essd-13-3219-2021, 2021
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Lightning is an important atmospheric phenomenon and natural hazard, but few long-term data are freely available on lightning stroke location, timing, and power. Here, we present a new, open-access dataset of lightning strokes covering 2010–2020, based on a network of low-frequency radio detectors. The dataset is comprised of GIS maps and is intended for researchers, government, industry, and anyone for whom knowing when and where lightning is likely to strike is useful information.
Patricio Velasquez, Jed O. Kaplan, Martina Messmer, Patrick Ludwig, and Christoph C. Raible
Clim. Past, 17, 1161–1180, https://doi.org/10.5194/cp-17-1161-2021, https://doi.org/10.5194/cp-17-1161-2021, 2021
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This study assesses the importance of resolution and land–atmosphere feedbacks for European climate. We performed an asynchronously coupled experiment that combined a global climate model (~ 100 km), a regional climate model (18 km), and a dynamic vegetation model (18 km). Modelled climate and land cover agree reasonably well with independent reconstructions based on pollen and other paleoenvironmental proxies. The regional climate is significantly influenced by land cover.
Kun Wang, Shohei Hattori, Mang Lin, Sakiko Ishino, Becky Alexander, Kazuki Kamezaki, Naohiro Yoshida, and Shichang Kang
Atmos. Chem. Phys., 21, 8357–8376, https://doi.org/10.5194/acp-21-8357-2021, https://doi.org/10.5194/acp-21-8357-2021, 2021
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Sulfate aerosols play an important climatic role and exert adverse effects on the ecological environment and human health. In this study, we present the triple oxygen isotopic composition of sulfate from the Mt. Everest region, southern Tibetan Plateau, and decipher the formation mechanisms of atmospheric sulfate in this pristine environment. The results indicate the important role of the S(IV) + O3 pathway in atmospheric sulfate formation promoted by conditions of high cloud water pH.
Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, https://doi.org/10.5194/acp-21-4187-2021, 2021
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We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.
Vasilii V. Petrenko, Andrew M. Smith, Edward M. Crosier, Roxana Kazemi, Philip Place, Aidan Colton, Bin Yang, Quan Hua, and Lee T. Murray
Atmos. Meas. Tech., 14, 2055–2063, https://doi.org/10.5194/amt-14-2055-2021, https://doi.org/10.5194/amt-14-2055-2021, 2021
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This paper presents an improved methodology for measurements of atmospheric concentration of carbon-14-containing carbon monoxide (14CO), as well as a 1-year dataset that demonstrates the methodology. Atmospheric 14CO concentration measurements are useful for improving the understanding of spatial and temporal variability of hydroxyl radical concentrations. Key improvements over prior methods include a greatly reduced air sample size and accurate procedural blank characterization.
Yang Li, Loretta J. Mickley, and Jed O. Kaplan
Atmos. Chem. Phys., 21, 57–68, https://doi.org/10.5194/acp-21-57-2021, https://doi.org/10.5194/acp-21-57-2021, 2021
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Climate models predict a shift toward warmer, drier environments in southwestern North America. Under future climate, the two main drivers of dust trends play opposing roles: (1) CO2 fertilization enhances vegetation and, in turn, decreases dust, and (2) increasing land use enhances dust emissions from northern Mexico. In the worst-case scenario, elevated dust concentrations spread widely over the domain by 2100 in spring, suggesting a large climate penalty on air quality and human health.
George C. Hurtt, Louise Chini, Ritvik Sahajpal, Steve Frolking, Benjamin L. Bodirsky, Katherine Calvin, Jonathan C. Doelman, Justin Fisk, Shinichiro Fujimori, Kees Klein Goldewijk, Tomoko Hasegawa, Peter Havlik, Andreas Heinimann, Florian Humpenöder, Johan Jungclaus, Jed O. Kaplan, Jennifer Kennedy, Tamás Krisztin, David Lawrence, Peter Lawrence, Lei Ma, Ole Mertz, Julia Pongratz, Alexander Popp, Benjamin Poulter, Keywan Riahi, Elena Shevliakova, Elke Stehfest, Peter Thornton, Francesco N. Tubiello, Detlef P. van Vuuren, and Xin Zhang
Geosci. Model Dev., 13, 5425–5464, https://doi.org/10.5194/gmd-13-5425-2020, https://doi.org/10.5194/gmd-13-5425-2020, 2020
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To estimate the effects of human land use activities on the carbon–climate system, a new set of global gridded land use forcing datasets was developed to link historical land use data to eight future scenarios in a standard format required by climate models. This new generation of land use harmonization (LUH2) includes updated inputs, higher spatial resolution, more detailed land use transitions, and the addition of important agricultural management layers; it will be used for CMIP6 simulations.
David S. Stevenson, Alcide Zhao, Vaishali Naik, Fiona M. O'Connor, Simone Tilmes, Guang Zeng, Lee T. Murray, William J. Collins, Paul T. Griffiths, Sungbo Shim, Larry W. Horowitz, Lori T. Sentman, and Louisa Emmons
Atmos. Chem. Phys., 20, 12905–12920, https://doi.org/10.5194/acp-20-12905-2020, https://doi.org/10.5194/acp-20-12905-2020, 2020
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We present historical trends in atmospheric oxidizing capacity (OC) since 1850 from the latest generation of global climate models and compare these with estimates from measurements. OC controls levels of many key reactive gases, including methane (CH4). We find small model trends up to 1980, then increases of about 9 % up to 2014, disagreeing with (uncertain) measurement-based trends. Major drivers of OC trends are emissions of CH4, NOx, and CO; these will be important for future CH4 trends.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys., 20, 10937–10951, https://doi.org/10.5194/acp-20-10937-2020, https://doi.org/10.5194/acp-20-10937-2020, 2020
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Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
Yang Li, Loretta J. Mickley, Pengfei Liu, and Jed O. Kaplan
Atmos. Chem. Phys., 20, 8827–8838, https://doi.org/10.5194/acp-20-8827-2020, https://doi.org/10.5194/acp-20-8827-2020, 2020
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Using a coupled vegetation–fire–climate modeling framework, we show a northward shift in forests and increased lightning fire activity in northern US states, including Idaho, Montana, and Wyoming. Our findings suggest a large climate penalty on ecosystem, air quality, visibility, and human health in a region valued for its national forests and parks. The fine-scale smoke PM predictions provided in this study should prove useful to human health and environmental assessments.
Jiayue Huang, Lyatt Jaeglé, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mat J. Evans, Nicolas Theys, and Sungyeon Choi
Atmos. Chem. Phys., 20, 7335–7358, https://doi.org/10.5194/acp-20-7335-2020, https://doi.org/10.5194/acp-20-7335-2020, 2020
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Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often observed in the springtime Arctic. Here, we use a chemical transport model to examine the role of sea salt aerosol from blowing snow in explaining these phenomena. We find that our simulation can account for the spatiotemporal variability of satellite observations of BrO. However, the model has difficulty in producing the magnitude of observed ozone depletion events.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Sandy P. Harrison, Marie-José Gaillard, Benjamin D. Stocker, Marc Vander Linden, Kees Klein Goldewijk, Oliver Boles, Pascale Braconnot, Andria Dawson, Etienne Fluet-Chouinard, Jed O. Kaplan, Thomas Kastner, Francesco S. R. Pausata, Erick Robinson, Nicki J. Whitehouse, Marco Madella, and Kathleen D. Morrison
Geosci. Model Dev., 13, 805–824, https://doi.org/10.5194/gmd-13-805-2020, https://doi.org/10.5194/gmd-13-805-2020, 2020
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The Past Global Changes LandCover6k initiative will use archaeological records to refine scenarios of land use and land cover change through the Holocene to reduce the uncertainties about the impacts of human-induced changes before widespread industrialization. We describe how archaeological data are used to map land use change and how the maps can be evaluated using independent palaeoenvironmental data. We propose simulations to test land use and land cover change impacts on past climates.
Julie M. Nicely, Bryan N. Duncan, Thomas F. Hanisco, Glenn M. Wolfe, Ross J. Salawitch, Makoto Deushi, Amund S. Haslerud, Patrick Jöckel, Béatrice Josse, Douglas E. Kinnison, Andrew Klekociuk, Michael E. Manyin, Virginie Marécal, Olaf Morgenstern, Lee T. Murray, Gunnar Myhre, Luke D. Oman, Giovanni Pitari, Andrea Pozzer, Ilaria Quaglia, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Kane Stone, Susan Strahan, Simone Tilmes, Holger Tost, Daniel M. Westervelt, and Guang Zeng
Atmos. Chem. Phys., 20, 1341–1361, https://doi.org/10.5194/acp-20-1341-2020, https://doi.org/10.5194/acp-20-1341-2020, 2020
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Differences in methane lifetime among global models are large and poorly understood. We use a neural network method and simulations from the Chemistry Climate Model Initiative to quantify the factors influencing methane lifetime spread among models and variations over time. UV photolysis, tropospheric ozone, and nitrogen oxides drive large model differences, while the same factors plus specific humidity contribute to a decreasing trend in methane lifetime between 1980 and 2015.
Pierre Friedlingstein, Matthew W. Jones, Michael O'Sullivan, Robbie M. Andrew, Judith Hauck, Glen P. Peters, Wouter Peters, Julia Pongratz, Stephen Sitch, Corinne Le Quéré, Dorothee C. E. Bakker, Josep G. Canadell, Philippe Ciais, Robert B. Jackson, Peter Anthoni, Leticia Barbero, Ana Bastos, Vladislav Bastrikov, Meike Becker, Laurent Bopp, Erik Buitenhuis, Naveen Chandra, Frédéric Chevallier, Louise P. Chini, Kim I. Currie, Richard A. Feely, Marion Gehlen, Dennis Gilfillan, Thanos Gkritzalis, Daniel S. Goll, Nicolas Gruber, Sören Gutekunst, Ian Harris, Vanessa Haverd, Richard A. Houghton, George Hurtt, Tatiana Ilyina, Atul K. Jain, Emilie Joetzjer, Jed O. Kaplan, Etsushi Kato, Kees Klein Goldewijk, Jan Ivar Korsbakken, Peter Landschützer, Siv K. Lauvset, Nathalie Lefèvre, Andrew Lenton, Sebastian Lienert, Danica Lombardozzi, Gregg Marland, Patrick C. McGuire, Joe R. Melton, Nicolas Metzl, David R. Munro, Julia E. M. S. Nabel, Shin-Ichiro Nakaoka, Craig Neill, Abdirahman M. Omar, Tsuneo Ono, Anna Peregon, Denis Pierrot, Benjamin Poulter, Gregor Rehder, Laure Resplandy, Eddy Robertson, Christian Rödenbeck, Roland Séférian, Jörg Schwinger, Naomi Smith, Pieter P. Tans, Hanqin Tian, Bronte Tilbrook, Francesco N. Tubiello, Guido R. van der Werf, Andrew J. Wiltshire, and Sönke Zaehle
Earth Syst. Sci. Data, 11, 1783–1838, https://doi.org/10.5194/essd-11-1783-2019, https://doi.org/10.5194/essd-11-1783-2019, 2019
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The Global Carbon Budget 2019 describes the data sets and methodology used to quantify the emissions of carbon dioxide and their partitioning among the atmosphere, land, and ocean. These living data are updated every year to provide the highest transparency and traceability in the reporting of CO2, the key driver of climate change.
Anina Gilgen, Stiig Wilkenskjeld, Jed O. Kaplan, Thomas Kühn, and Ulrike Lohmann
Clim. Past, 15, 1885–1911, https://doi.org/10.5194/cp-15-1885-2019, https://doi.org/10.5194/cp-15-1885-2019, 2019
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Using the global aerosol–climate model ECHAM-HAM-SALSA, the effect of humans on European climate in the Roman Empire was quantified. Both land use and novel estimates of anthropogenic aerosol emissions were considered. We conducted simulations with fixed sea-surface temperatures to gain a first impression about the anthropogenic impact. While land use effects induced a regional warming for one of the reconstructions, aerosol emissions led to a cooling associated with aerosol–cloud interactions.
Rachel F. Silvern, Daniel J. Jacob, Loretta J. Mickley, Melissa P. Sulprizio, Katherine R. Travis, Eloise A. Marais, Ronald C. Cohen, Joshua L. Laughner, Sungyeon Choi, Joanna Joiner, and Lok N. Lamsal
Atmos. Chem. Phys., 19, 8863–8878, https://doi.org/10.5194/acp-19-8863-2019, https://doi.org/10.5194/acp-19-8863-2019, 2019
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The US EPA reports a steady decrease in nitrogen oxide (NOx) emissions from fuel combustion over the 2005–2017 period, while satellite observations show a leveling off after 2009, suggesting emission reductions and related air quality gains have halted. We show the sustained decrease in NOx emissions is in fact consistent with observed trends in surface NO2 and ozone concentrations and that the flattening of the satellite trend reflects a growing influence from the non-anthropogenic background.
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
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Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Lu Shen, Daniel J. Jacob, Loretta J. Mickley, Yuxuan Wang, and Qiang Zhang
Atmos. Chem. Phys., 18, 17489–17496, https://doi.org/10.5194/acp-18-17489-2018, https://doi.org/10.5194/acp-18-17489-2018, 2018
Eloise A. Marais, Daniel J. Jacob, Sungyeon Choi, Joanna Joiner, Maria Belmonte-Rivas, Ronald C. Cohen, Steffen Beirle, Lee T. Murray, Luke D. Schiferl, Viral Shah, and Lyatt Jaeglé
Atmos. Chem. Phys., 18, 17017–17027, https://doi.org/10.5194/acp-18-17017-2018, https://doi.org/10.5194/acp-18-17017-2018, 2018
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We intercompare two new products of global upper tropospheric nitrogen dioxide (NO2) retrieved from the Ozone Monitoring Instrument (OMI). We evaluate these products with aircraft observations from NASA DC8 aircraft campaigns and interpret the useful information these products can provide about nitrogen oxides (NOx) in the global upper troposphere using the GEOS-Chem chemical transport model.
Samuel R. Hall, Kirk Ullmann, Michael J. Prather, Clare M. Flynn, Lee T. Murray, Arlene M. Fiore, Gustavo Correa, Sarah A. Strode, Stephen D. Steenrod, Jean-Francois Lamarque, Jonathan Guth, Béatrice Josse, Johannes Flemming, Vincent Huijnen, N. Luke Abraham, and Alex T. Archibald
Atmos. Chem. Phys., 18, 16809–16828, https://doi.org/10.5194/acp-18-16809-2018, https://doi.org/10.5194/acp-18-16809-2018, 2018
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Photolysis (J rates) initiates and drives atmospheric chemistry, and Js are perturbed by factors of 2 by clouds. The NASA Atmospheric Tomography (ATom) Mission provides the first comprehensive observations on how clouds perturb Js through the remote Pacific and Atlantic basins. We compare these cloud-perturbation J statistics with those from nine global chemistry models. While basic patterns agree, there is a large spread across models, and all lack some basic features of the observations.
Qianjie Chen, Tomás Sherwen, Mathew Evans, and Becky Alexander
Atmos. Chem. Phys., 18, 13617–13637, https://doi.org/10.5194/acp-18-13617-2018, https://doi.org/10.5194/acp-18-13617-2018, 2018
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Uncertainty in the natural tropospheric sulfur cycle represents the largest source of uncertainty in radiative forcing estimates of sulfate aerosol. This study investigates the natural sulfur cycle in the marine troposphere using the GEOS-Chem model. We found that BrO is important for DMS oxidation and multiphase chemistry is important for MSA production and loss, which have implications for the yield of SO2 and MSA from DMS oxidation and the radiative effect of DMS-derived sulfate aerosol.
Jean J. Guo, Arlene M. Fiore, Lee T. Murray, Daniel A. Jaffe, Jordan L. Schnell, Charles T. Moore, and George P. Milly
Atmos. Chem. Phys., 18, 12123–12140, https://doi.org/10.5194/acp-18-12123-2018, https://doi.org/10.5194/acp-18-12123-2018, 2018
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We use the GEOS-Chem model to estimate the influence from anthropogenic and background sources to ozone over the USA. Novel findings include the point that year-to-year background variability on the 10 highest observed ozone days is driven mainly by natural sources and not international or intercontinental pollution transport. High positive model biases during summer are associated with regional ozone production. The EPA 3-year average metric falls short of its aim to remove natural variability.
Prasad Kasibhatla, Tomás Sherwen, Mathew J. Evans, Lucy J. Carpenter, Chris Reed, Becky Alexander, Qianjie Chen, Melissa P. Sulprizio, James D. Lee, Katie A. Read, William Bloss, Leigh R. Crilley, William C. Keene, Alexander A. P. Pszenny, and Alma Hodzic
Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, https://doi.org/10.5194/acp-18-11185-2018, 2018
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Recent measurements of NOx and HONO suggest that photolysis of particulate nitrate in sea-salt aerosols is important in terms of marine boundary layer oxidant chemistry. We present the first global-scale assessment of the significance of this new chemical pathway for NOx, O3, and OH in the marine boundary layer. We also present a preliminary assessment of the potential impact of photolysis of particulate nitrate associated with other aerosol types on continental boundary layer chemistry.
Danny M. Leung, Amos P. K. Tai, Loretta J. Mickley, Jonathan M. Moch, Aaron van Donkelaar, Lu Shen, and Randall V. Martin
Atmos. Chem. Phys., 18, 6733–6748, https://doi.org/10.5194/acp-18-6733-2018, https://doi.org/10.5194/acp-18-6733-2018, 2018
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This paper investigates how large-scale weather systems control fine particulate matter (PM2.5) air quality in China. We show that winter monsoons, onshore winds and frontal rains can drive daily PM2.5 variability in different regions of China. We further project future PM2.5 concentration change by 2050s due to climate change, and verify that climate change has little benefit on future PM2.5 in Beijing, implying cutting down emissions is necessary to mitigate pollutions in megacities of China.
Michael J. Prather, Clare M. Flynn, Xin Zhu, Stephen D. Steenrod, Sarah A. Strode, Arlene M. Fiore, Gustavo Correa, Lee T. Murray, and Jean-Francois Lamarque
Atmos. Meas. Tech., 11, 2653–2668, https://doi.org/10.5194/amt-11-2653-2018, https://doi.org/10.5194/amt-11-2653-2018, 2018
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A new protocol for merging in situ atmospheric chemistry measurements with 3-D models is developed. This technique can identify the most reactive air parcels in terms of tropospheric production/loss of O3 & CH4. This approach highlights differences in 6 global chemistry models even with composition specified. Thus in situ measurements from, e.g., NASA's ATom mission can be used to develop a chemical climatology of, not only the key species, but also the rates of key reactions in each air parcel.
Pengzhen He, Becky Alexander, Lei Geng, Xiyuan Chi, Shidong Fan, Haicong Zhan, Hui Kang, Guangjie Zheng, Yafang Cheng, Hang Su, Cheng Liu, and Zhouqing Xie
Atmos. Chem. Phys., 18, 5515–5528, https://doi.org/10.5194/acp-18-5515-2018, https://doi.org/10.5194/acp-18-5515-2018, 2018
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We use observations of the oxygen isotopic composition of sulfate aerosol as a fingerprint to quantify various sulfate formation mechanisms during pollution events in Beijing, China. We found that heterogeneous reactions on aerosols dominated sulfate production in general; however, in-cloud reactions would dominate haze sulfate production when cloud liquid water content was high. The findings also suggest the heterogeneity of aerosol acidity should be parameterized in models.
Emeline Chaste, Martin P. Girardin, Jed O. Kaplan, Jeanne Portier, Yves Bergeron, and Christelle Hély
Biogeosciences, 15, 1273–1292, https://doi.org/10.5194/bg-15-1273-2018, https://doi.org/10.5194/bg-15-1273-2018, 2018
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A vegetation model was used to reconstruct fire activity from 1901 to 2012 in relation to changes in lightning ignition, climate, and vegetation in eastern Canada's boreal forest. The model correctly simulated the history of fire activity. The results showed that fire activity is ignition limited but is also greatly affected by both climate and vegetation. This research aims to develop a vegetation model that could be used to predict the future impacts of climate changes on fire activity.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Daniel H. Cusworth, Loretta J. Mickley, Eric M. Leibensperger, and Michael J. Iacono
Atmos. Chem. Phys., 17, 13559–13572, https://doi.org/10.5194/acp-17-13559-2017, https://doi.org/10.5194/acp-17-13559-2017, 2017
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Since 1990, light-scattering pollution known as aerosols have declined as a result of tightening US air quality regulations. Our study finds that US surface solar radiation has increased simultaneously. We establish a link between aerosols and radiation through physical and statistical models. We find the strongest relationship between aerosols, radiation, and climate at a site in the Midwest. Our work underscores the importance of regional pollution on climate in the US and abroad.
Jenny A. Fisher, Lee T. Murray, Dylan B. A. Jones, and Nicholas M. Deutscher
Geosci. Model Dev., 10, 4129–4144, https://doi.org/10.5194/gmd-10-4129-2017, https://doi.org/10.5194/gmd-10-4129-2017, 2017
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Carbon monoxide (CO) simulation in atmospheric chemistry models is used for source–receptor analysis, emission inversion, and interpretation of observations. We introduce a major update to CO simulation in the GEOS-Chem chemical transport model that removes fundamental inconsistencies relative to the standard model, resolving biases of more than 100 ppb and errors in vertical structure. We also add source tagging of secondary CO and demonstrate it provides added value in low-emission regions.
Johann H. Jungclaus, Edouard Bard, Mélanie Baroni, Pascale Braconnot, Jian Cao, Louise P. Chini, Tania Egorova, Michael Evans, J. Fidel González-Rouco, Hugues Goosse, George C. Hurtt, Fortunat Joos, Jed O. Kaplan, Myriam Khodri, Kees Klein Goldewijk, Natalie Krivova, Allegra N. LeGrande, Stephan J. Lorenz, Jürg Luterbacher, Wenmin Man, Amanda C. Maycock, Malte Meinshausen, Anders Moberg, Raimund Muscheler, Christoph Nehrbass-Ahles, Bette I. Otto-Bliesner, Steven J. Phipps, Julia Pongratz, Eugene Rozanov, Gavin A. Schmidt, Hauke Schmidt, Werner Schmutz, Andrew Schurer, Alexander I. Shapiro, Michael Sigl, Jason E. Smerdon, Sami K. Solanki, Claudia Timmreck, Matthew Toohey, Ilya G. Usoskin, Sebastian Wagner, Chi-Ju Wu, Kok Leng Yeo, Davide Zanchettin, Qiong Zhang, and Eduardo Zorita
Geosci. Model Dev., 10, 4005–4033, https://doi.org/10.5194/gmd-10-4005-2017, https://doi.org/10.5194/gmd-10-4005-2017, 2017
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Climate model simulations covering the last millennium provide context for the evolution of the modern climate and for the expected changes during the coming centuries. They can help identify plausible mechanisms underlying palaeoclimatic reconstructions. Here, we describe the forcing boundary conditions and the experimental protocol for simulations covering the pre-industrial millennium. We describe the PMIP4 past1000 simulations as contributions to CMIP6 and additional sensitivity experiments.
Philipp S. Sommer and Jed O. Kaplan
Geosci. Model Dev., 10, 3771–3791, https://doi.org/10.5194/gmd-10-3771-2017, https://doi.org/10.5194/gmd-10-3771-2017, 2017
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We present GWGEN, a computer program for converting monthly climate data into estimates of daily weather, using statistical methods. The GWGEN weather generator program was developed using a global database of more than 5 million observations of daily weather, and it simulates daily values of minimum and maximum temperature, precipitation, cloud cover, and wind speed. GWGEN may be used in a range of applications, for example, in global vegetation, crop, soil erosion, or hydrological models.
Michael J. Prather, Xin Zhu, Clare M. Flynn, Sarah A. Strode, Jose M. Rodriguez, Stephen D. Steenrod, Junhua Liu, Jean-Francois Lamarque, Arlene M. Fiore, Larry W. Horowitz, Jingqiu Mao, Lee T. Murray, Drew T. Shindell, and Steven C. Wofsy
Atmos. Chem. Phys., 17, 9081–9102, https://doi.org/10.5194/acp-17-9081-2017, https://doi.org/10.5194/acp-17-9081-2017, 2017
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We present a new approach for comparing atmospheric chemistry models with measurements based on what these models are used to do, i.e., calculate changes in ozone and methane, prime greenhouse gases. This method anticipates a new type of measurements from the NASA Atmospheric Tomography (ATom) mission. In comparing the mixture of species within air parcels, we focus on those responsible for key chemical changes and weight these parcels by their chemical reactivity.
Lu Shen, Loretta J. Mickley, and Lee T. Murray
Atmos. Chem. Phys., 17, 4355–4367, https://doi.org/10.5194/acp-17-4355-2017, https://doi.org/10.5194/acp-17-4355-2017, 2017
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We introduce a new method to characterize the influence of atmospheric circulation on surface PM2.5 concentrations. Applying our statistical model to climate projections, we find a strong influence of 2000–2050 climate change on PM2.5 air quality in the United States. We find that current atmospheric chemistry models may underestimate the strong positive sensitivity of PM2.5 to temperature in the eastern United States in summer, and so may underestimate PM2.5 changes in a warmer climate.
Sam S. Rabin, Joe R. Melton, Gitta Lasslop, Dominique Bachelet, Matthew Forrest, Stijn Hantson, Jed O. Kaplan, Fang Li, Stéphane Mangeon, Daniel S. Ward, Chao Yue, Vivek K. Arora, Thomas Hickler, Silvia Kloster, Wolfgang Knorr, Lars Nieradzik, Allan Spessa, Gerd A. Folberth, Tim Sheehan, Apostolos Voulgarakis, Douglas I. Kelley, I. Colin Prentice, Stephen Sitch, Sandy Harrison, and Almut Arneth
Geosci. Model Dev., 10, 1175–1197, https://doi.org/10.5194/gmd-10-1175-2017, https://doi.org/10.5194/gmd-10-1175-2017, 2017
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Global vegetation models are important tools for understanding how the Earth system will change in the future, and fire is a critical process to include. A number of different methods have been developed to represent vegetation burning. This paper describes the protocol for the first systematic comparison of global fire models, which will allow the community to explore various drivers and evaluate what mechanisms are important for improving performance. It also includes equations for all models.
Tomás Sherwen, Mat J. Evans, Lucy J. Carpenter, Johan A. Schmidt, and Loretta J. Mickley
Atmos. Chem. Phys., 17, 1557–1569, https://doi.org/10.5194/acp-17-1557-2017, https://doi.org/10.5194/acp-17-1557-2017, 2017
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We model pre-industrial to present day changes using the GEOS-Chem global chemical transport model with halogens (Cl, Br, I). The model better captures pre-industrial O3 observations with halogens included. Halogens buffer the tropospheric forcing of O3 (RFTO3) from pre-industrial to present day, reducing RFTO3 by 0.087 Wm−2. This reduction is greater than that from halogens on stratospheric O3 (−0.05 Wm−2). This suggests that models that do not include halogens will overestimate RFTO3by ~ 25%.
Maria Zatko, Joseph Erbland, Joel Savarino, Lei Geng, Lauren Easley, Andrew Schauer, Timothy Bates, Patricia K. Quinn, Bonnie Light, David Morison, Hans D. Osthoff, Seth Lyman, William Neff, Bin Yuan, and Becky Alexander
Atmos. Chem. Phys., 16, 13837–13851, https://doi.org/10.5194/acp-16-13837-2016, https://doi.org/10.5194/acp-16-13837-2016, 2016
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This manuscript presents chemical and optical observations collected in the air and snow during UBWOS2014 in eastern Utah. These observations are used to calculate fluxes of reactive nitrogen associated with snow nitrate photolysis. Snow-sourced reactive nitrogen fluxes are compared to reactive nitrogen emission inventories to find that snow-sourced reactive nitrogen is a minor contributor to the reactive nitrogen budget, and thus wintertime ground-level ozone formation, in the Uintah Basin.
Lei Zhu, Daniel J. Jacob, Patrick S. Kim, Jenny A. Fisher, Karen Yu, Katherine R. Travis, Loretta J. Mickley, Robert M. Yantosca, Melissa P. Sulprizio, Isabelle De Smedt, Gonzalo González Abad, Kelly Chance, Can Li, Richard Ferrare, Alan Fried, Johnathan W. Hair, Thomas F. Hanisco, Dirk Richter, Amy Jo Scarino, James Walega, Petter Weibring, and Glenn M. Wolfe
Atmos. Chem. Phys., 16, 13477–13490, https://doi.org/10.5194/acp-16-13477-2016, https://doi.org/10.5194/acp-16-13477-2016, 2016
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HCHO column data are widely used as a proxy for VOCs emissions, but validation of the data has been extremely limited. We use accurate aircraft observations to validate and intercompare 6 HCHO retrievals with GEOS-Chem as the intercomparison platform. Retrievals are interconsistent in spatial variability over the SE US and in daily variability, but are biased low by 20–51 %. Our work supports the use of HCHO column as a quantitative proxy for isoprene emission after correction of the low bias.
Qianjie Chen, Lei Geng, Johan A. Schmidt, Zhouqing Xie, Hui Kang, Jordi Dachs, Jihong Cole-Dai, Andrew J. Schauer, Madeline G. Camp, and Becky Alexander
Atmos. Chem. Phys., 16, 11433–11450, https://doi.org/10.5194/acp-16-11433-2016, https://doi.org/10.5194/acp-16-11433-2016, 2016
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The formation mechanisms of sulfate in the marine boundary layer are not well understood, which could result in large uncertainties in aerosol radiative forcing. We measure the oxygen isotopic composition (Δ17O) of sulfate collected in the MBL and analyze with a global transport model. Our results suggest that 33–50 % of MBL sulfate is formed via oxidation of S(IV) by hypohalous acids HOBr / HOCl in the aqueous phase, and the daily-mean HOBr/HOCl concentrations are on the order of 0.01–0.1 ppt.
Stijn Hantson, Almut Arneth, Sandy P. Harrison, Douglas I. Kelley, I. Colin Prentice, Sam S. Rabin, Sally Archibald, Florent Mouillot, Steve R. Arnold, Paulo Artaxo, Dominique Bachelet, Philippe Ciais, Matthew Forrest, Pierre Friedlingstein, Thomas Hickler, Jed O. Kaplan, Silvia Kloster, Wolfgang Knorr, Gitta Lasslop, Fang Li, Stephane Mangeon, Joe R. Melton, Andrea Meyn, Stephen Sitch, Allan Spessa, Guido R. van der Werf, Apostolos Voulgarakis, and Chao Yue
Biogeosciences, 13, 3359–3375, https://doi.org/10.5194/bg-13-3359-2016, https://doi.org/10.5194/bg-13-3359-2016, 2016
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Our ability to predict the magnitude and geographic pattern of past and future fire impacts rests on our ability to model fire regimes. A large variety of models exist, and it is unclear which type of model or degree of complexity is required to model fire adequately at regional to global scales. In this paper we summarize the current state of the art in fire-regime modelling and model evaluation, and outline what lessons may be learned from the Fire Model Intercomparison Project – FireMIP.
M. Clare Smith, Joy S. Singarayer, Paul J. Valdes, Jed O. Kaplan, and Nicholas P. Branch
Clim. Past, 12, 923–941, https://doi.org/10.5194/cp-12-923-2016, https://doi.org/10.5194/cp-12-923-2016, 2016
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We used climate modelling to estimate the biogeophysical impacts of agriculture on the climate over the last 8000 years of the Holocene. Our results show statistically significant surface temperature changes (mainly cooling) from as early as 7000 BP in the JJA season and throughout the entire annual cycle by 2–3000 BP. The changes were greatest in the areas of land use change but were also seen in other areas. Precipitation was also affected, particularly in Europe, India, and the ITCZ region.
Maria Zatko, Lei Geng, Becky Alexander, Eric Sofen, and Katarina Klein
Atmos. Chem. Phys., 16, 2819–2842, https://doi.org/10.5194/acp-16-2819-2016, https://doi.org/10.5194/acp-16-2819-2016, 2016
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We have incorporated an idealized snowpack with a nitrate photolysis parameterization into a global chemical transport model (GEOS-Chem) to examine the implications of snow nitrate photolysis for boundary layer chemistry, the recycling and redistribution of reactive nitrogen, and the preservation of ice-core nitrate in ice cores across Antarctica and Greenland. We also examine the sensitivity of these processes to meteorological parameters and chemical, optical, and physical snow properties.
Zhen Zhang, Niklaus E. Zimmermann, Jed O. Kaplan, and Benjamin Poulter
Biogeosciences, 13, 1387–1408, https://doi.org/10.5194/bg-13-1387-2016, https://doi.org/10.5194/bg-13-1387-2016, 2016
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This study investigates improvements and uncertainties associated with estimating global inundated area and wetland CH4 emissions using TOPMODEL. Different topographic information and catchment aggregation schemes are evaluated against seasonal and permanently inundated wetland observations. Reducing uncertainty in prognostic wetland dynamics modeling must take into account forcing data as well as topographic scaling schemes.
L. Shen, L. J. Mickley, and A. P. K. Tai
Atmos. Chem. Phys., 15, 10925–10938, https://doi.org/10.5194/acp-15-10925-2015, https://doi.org/10.5194/acp-15-10925-2015, 2015
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In this study, we have examined the effect of polar jet and Bermuda High on ozone air quality in the eastern United States. In the Midwest and northeast, the poleward shift of jet wind leads to reduced polar jet frequency, resulting in increased ozone there. In the southeast, the influence of Bermuda High on ozone variability depends on the location of its west edge. Westward movement increases the ozone only when the JJA Bermuda High west edge is located west of 85.4°W.
X. Yue, L. J. Mickley, J. A. Logan, R. C. Hudman, M. V. Martin, and R. M. Yantosca
Atmos. Chem. Phys., 15, 10033–10055, https://doi.org/10.5194/acp-15-10033-2015, https://doi.org/10.5194/acp-15-10033-2015, 2015
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Based on simulated meteorology from 13 GCMs, we projected future wildfire activity in Alaskan and Canadian ecoregions by the mid-century. The most robust change is the increase of 150-390% in area burned over Alaska and western Canada. The models also predict an increase of 45-90% in the central and southern Canadian ecoregions, but a decrease of up to 50% in northern Canada. We further quantify how the changes in wildfire emissions may affect ozone concentrations in North America.
M. J. McGrath, S. Luyssaert, P. Meyfroidt, J. O. Kaplan, M. Bürgi, Y. Chen, K. Erb, U. Gimmi, D. McInerney, K. Naudts, J. Otto, F. Pasztor, J. Ryder, M.-J. Schelhaas, and A. Valade
Biogeosciences, 12, 4291–4316, https://doi.org/10.5194/bg-12-4291-2015, https://doi.org/10.5194/bg-12-4291-2015, 2015
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Studying century-scale ecological processes and their legacy effects requires taking forest management into account. In this study we produce spatially and temporally explicit maps of European forest management from 1600 to 2010. The most important changes between 1600 and 2010 are an increase of 593 000km2 in conifers at the expense of deciduous forest, a 612 000km2 decrease in unmanaged forest, a 152 000km2 decrease in coppice management and a 818 000km2 increase in high stand management.
P. Achakulwisut, L. J. Mickley, L. T. Murray, A. P. K. Tai, J. O. Kaplan, and B. Alexander
Atmos. Chem. Phys., 15, 7977–7998, https://doi.org/10.5194/acp-15-7977-2015, https://doi.org/10.5194/acp-15-7977-2015, 2015
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The atmosphere’s oxidative capacity determines the lifetime of many trace gases important to climate, chemistry, and human health. Yet uncertainties remain about its past variations, its controlling factors, and the radiative forcing of short-lived species it influences. To reduce these uncertainties, we must better quantify the natural emissions and chemical reaction mechanisms of organic compounds in the atmosphere, which play a role in governing the oxidative capacity.
T. J. Bohn, J. R. Melton, A. Ito, T. Kleinen, R. Spahni, B. D. Stocker, B. Zhang, X. Zhu, R. Schroeder, M. V. Glagolev, S. Maksyutov, V. Brovkin, G. Chen, S. N. Denisov, A. V. Eliseev, A. Gallego-Sala, K. C. McDonald, M.A. Rawlins, W. J. Riley, Z. M. Subin, H. Tian, Q. Zhuang, and J. O. Kaplan
Biogeosciences, 12, 3321–3349, https://doi.org/10.5194/bg-12-3321-2015, https://doi.org/10.5194/bg-12-3321-2015, 2015
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We evaluated 21 forward models and 5 inversions over western Siberia in terms of CH4 emissions and simulated wetland areas and compared these results to an intensive in situ CH4 flux data set, several wetland maps, and two satellite inundation products. In addition to assembling a definitive collection of methane emissions estimates for the region, we were able to identify the types of wetland maps and model features necessary for accurate simulations of high-latitude wetlands.
L. Geng, J. Cole-Dai, B. Alexander, J. Erbland, J. Savarino, A. J. Schauer, E. J. Steig, P. Lin, Q. Fu, and M. C. Zatko
Atmos. Chem. Phys., 14, 13361–13376, https://doi.org/10.5194/acp-14-13361-2014, https://doi.org/10.5194/acp-14-13361-2014, 2014
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Examinations on snowpit and firn core results from Summit, Greenland suggest that there are two mechanisms leading to the observed double nitrate peaks in some years in the industrial era: 1) long-rang transport of nitrate and 2) enhanced local photochemical production of nitrate. Both of these mechanisms are related to pollution transport, as the additional nitrate from either direct transport or enhanced local photochemistry requires enhanced nitrogen sources from anthropogenic emissions.
A. Mauri, B. A. S. Davis, P. M. Collins, and J. O. Kaplan
Clim. Past, 10, 1925–1938, https://doi.org/10.5194/cp-10-1925-2014, https://doi.org/10.5194/cp-10-1925-2014, 2014
E. D. Sofen, B. Alexander, E. J. Steig, M. H. Thiemens, S. A. Kunasek, H. M. Amos, A. J. Schauer, M. G. Hastings, J. Bautista, T. L. Jackson, L. E. Vogel, J. R. McConnell, D. R. Pasteris, and E. S. Saltzman
Atmos. Chem. Phys., 14, 5749–5769, https://doi.org/10.5194/acp-14-5749-2014, https://doi.org/10.5194/acp-14-5749-2014, 2014
G. Strandberg, E. Kjellström, A. Poska, S. Wagner, M.-J. Gaillard, A.-K. Trondman, A. Mauri, B. A. S. Davis, J. O. Kaplan, H. J. B. Birks, A. E. Bjune, R. Fyfe, T. Giesecke, L. Kalnina, M. Kangur, W. O. van der Knaap, U. Kokfelt, P. Kuneš, M. Lata\l owa, L. Marquer, F. Mazier, A. B. Nielsen, B. Smith, H. Seppä, and S. Sugita
Clim. Past, 10, 661–680, https://doi.org/10.5194/cp-10-661-2014, https://doi.org/10.5194/cp-10-661-2014, 2014
T. Hoffmann, S. M. Mudd, K. van Oost, G. Verstraeten, G. Erkens, A. Lang, H. Middelkoop, J. Boyle, J. O. Kaplan, J. Willenbring, and R. Aalto
Earth Surf. Dynam., 1, 45–52, https://doi.org/10.5194/esurf-1-45-2013, https://doi.org/10.5194/esurf-1-45-2013, 2013
M. Scherstjanoi, J. O. Kaplan, E. Thürig, and H. Lischke
Geosci. Model Dev., 6, 1517–1542, https://doi.org/10.5194/gmd-6-1517-2013, https://doi.org/10.5194/gmd-6-1517-2013, 2013
V. Beck, C. Gerbig, T. Koch, M. M. Bela, K. M. Longo, S. R. Freitas, J. O. Kaplan, C. Prigent, P. Bergamaschi, and M. Heimann
Atmos. Chem. Phys., 13, 7961–7982, https://doi.org/10.5194/acp-13-7961-2013, https://doi.org/10.5194/acp-13-7961-2013, 2013
H. Jiang, H. Liao, H. O. T. Pye, S. Wu, L. J. Mickley, J. H. Seinfeld, and X. Y. Zhang
Atmos. Chem. Phys., 13, 7937–7960, https://doi.org/10.5194/acp-13-7937-2013, https://doi.org/10.5194/acp-13-7937-2013, 2013
M. Pfeiffer, A. Spessa, and J. O. Kaplan
Geosci. Model Dev., 6, 643–685, https://doi.org/10.5194/gmd-6-643-2013, https://doi.org/10.5194/gmd-6-643-2013, 2013
R. Wania, J. R. Melton, E. L. Hodson, B. Poulter, B. Ringeval, R. Spahni, T. Bohn, C. A. Avis, G. Chen, A. V. Eliseev, P. O. Hopcroft, W. J. Riley, Z. M. Subin, H. Tian, P. M. van Bodegom, T. Kleinen, Z. C. Yu, J. S. Singarayer, S. Zürcher, D. P. Lettenmaier, D. J. Beerling, S. N. Denisov, C. Prigent, F. Papa, and J. O. Kaplan
Geosci. Model Dev., 6, 617–641, https://doi.org/10.5194/gmd-6-617-2013, https://doi.org/10.5194/gmd-6-617-2013, 2013
J. R. Melton, R. Wania, E. L. Hodson, B. Poulter, B. Ringeval, R. Spahni, T. Bohn, C. A. Avis, D. J. Beerling, G. Chen, A. V. Eliseev, S. N. Denisov, P. O. Hopcroft, D. P. Lettenmaier, W. J. Riley, J. S. Singarayer, Z. M. Subin, H. Tian, S. Zürcher, V. Brovkin, P. M. van Bodegom, T. Kleinen, Z. C. Yu, and J. O. Kaplan
Biogeosciences, 10, 753–788, https://doi.org/10.5194/bg-10-753-2013, https://doi.org/10.5194/bg-10-753-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Representing improved tropospheric ozone distribution over the Northern Hemisphere by including lightning NOx emissions in CHIMERE
Assessing the ability to quantify the decrease in NOx anthropogenic emissions in 2019 compared to 2005 using OMI and TROPOMI satellite observations
Tracking daily NOx emissions from an urban agglomeration based on TROPOMI NO2 and a local ensemble transform Kalman filter
Evaluation of O3, H2O, CO, and NOy climatologies simulated by four global models in the upper troposphere–lower stratosphere with IAGOS measurements
Source contribution to ozone pollution during June 2021 fire events in Arizona: insights from WRF-Chem-tagged O3 and CO
High-resolution mapping of on-road vehicle emissions with real-time traffic datasets based on big data
Sensitivity of climate–chemistry model simulated atmospheric composition to the application of an inverse relationship between NOx emission and lightning flash frequency
Regional and sectoral contributions of NOx and reactive carbon emission sources to global trends in tropospheric ozone during the 2000–2018 period
Underappreciated contributions of biogenic volatile organic compounds from urban green spaces to ozone pollution
Chemistry–climate feedback of atmospheric methane in a methane-emission-flux-driven chemistry–climate model
Surface ozone trend variability across the United States and the impact of heat waves (1990–2023)
Sensitivity of climate effects of hydrogen to leakage size, location, and chemical background
Evaluating tropospheric nitrogen dioxide in UKCA using OMI satellite retrievals over south and east Asia
Shifts in global atmospheric oxidant chemistry from land cover change
Technical note: A comparative study of chemistry schemes for volcanic sulfur dioxide in Lagrangian transport simulations – a case study of the 2019 Raikoke eruption
Revisiting the high tropospheric ozone over southern Africa: role of biomass burning and anthropogenic emissions
Monoterpene oxidation pathways initiated by acyl peroxy radical addition
Local and transboundary contributions to NOy loadings across East Asia using CMAQ-ISAM and a GEMS-informed emission inventory during the winter–spring transition
A New Parameterization of Photolysis Rates for Oxygenated Volatile Organic Compounds (OVOCs)
Estimating the variability in NOx emissions from Wuhan with TROPOMI NO2 data during 2018 to 2023
Enhanced understanding of atmospheric blocking modulation on ozone dynamics within a high-resolution Earth system model
Natural emissions of VOC and NOx over Africa constrained by TROPOMI HCHO and NO2 data using the MAGRITTEv1.1 model
Contributions of lightning to long-term trends and inter-annual variability in global atmospheric chemistry constrained by Schumann Resonance observations
Simulated photochemical response to observational constraints on aerosol vertical distribution over North China
Impacts of wildfire smoke aerosols on near-surface ozone photochemistry
Anthropogenic emission controls reduce summertime ozone–temperature sensitivity in the United States
Investigating the response of China's surface ozone concentration to the future changes of multiple factors
The 21st-century wetting inhibits growing surface ozone in Northwestern China
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
Air-pollution-satellite-based CO2 emission inversion: system evaluation, sensitivity analysis, and future research direction
The impact of sea spray aerosol on photochemical ozone formation over eastern China: heterogeneous reaction of chlorine particles and radiative effect
Insights into ozone pollution control in urban areas by decoupling meteorological factors based on machine learning
Improving the computation efficiency of a source-oriented chemical mechanism for the simultaneous source apportionment of ozone and secondary particulate pollutants
Quantification of regional net CO2 flux errors in the Orbiting Carbon Observatory-2 (OCO-2) v10 model intercomparison project (MIP) ensemble using airborne measurements
Reactive nitrogen in and around the northeastern and mid-Atlantic US: sources, sinks, and connections with ozone
Preindustrial-to-present-day changes in atmospheric carbon monoxide: agreement and gaps between ice archives and global model reconstructions
Investigating processes influencing simulation of local Arctic wintertime anthropogenic pollution in Fairbanks, Alaska, during ALPACA-2022
Urban ozone formation and sensitivities to volatile chemical products, cooking emissions, and NOx upwind of and within two Los Angeles Basin cities
Causes of growing middle-to-upper tropospheric ozone over the northwest Pacific region
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
Modelling Arctic Lower Tropospheric Ozone: processes controlling seasonal variations
Climate-driven biogenic emissions alleviate the impact of man-made emission reduction on O3 control in Pearl River Delta region, southern China
South Asia ammonia emission inversion through assimilating IASI observations
Constraining the budget of NOx and VOCs at a remote Tropical island using multi-platform observations and WRF-Chem model simulations
A CO2–Δ14CO2 inversion setup for estimating European fossil CO2 emissions
Maximum ozone concentrations in the southwestern US and Texas: implications of the growing predominance of the background contribution
Derivation of atmospheric reaction mechanisms for volatile organic compounds by the SAPRC mechanism generation system (MechGen)
Comparative ozone production sensitivity to NOx and VOCs in Quito, Ecuador and Santiago, Chile: implications for control strategies in times of climate action
Seasonal, regional, and vertical characteristics of high-carbon-monoxide plumes along with their associated ozone anomalies, as seen by IAGOS between 2002 and 2019
Sanhita Ghosh, Arineh Cholakian, Sylvain Mailler, and Laurent Menut
Atmos. Chem. Phys., 25, 6273–6297, https://doi.org/10.5194/acp-25-6273-2025, https://doi.org/10.5194/acp-25-6273-2025, 2025
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In this study, we evaluate the present state of modelling lightning flashes over the Northern Hemisphere, using the classical CTH (cloud-top height) scheme and the ICEFLUX scheme with the CHIMERE model. Our study provides a comprehensive 3D comparison of model outputs to assess the robustness and applicability of these schemes. An improvement in O3 distribution in the tropical free troposphere is observed due to inclusion of LNOx (nitrogen oxide emissions from lightning) in the model. Inclusion of LNOx also reduces the lifetime of trace gas CH4.
Audrey Fortems-Cheiney, Grégoire Broquet, Elise Potier, Antoine Berchet, Isabelle Pison, Adrien Martinez, Robin Plauchu, Rimal Abeed, Aurélien Sicsik-Paré, Gaelle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, Henk Eskes, Hugo A. C. Denier van der Gon, and Stijn N. C. Dellaert
Atmos. Chem. Phys., 25, 6047–6068, https://doi.org/10.5194/acp-25-6047-2025, https://doi.org/10.5194/acp-25-6047-2025, 2025
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This study assesses the potential of the Ozone Monitoring Instrument (OMI) and the TROPOspheric Monitoring Instrument (TROPOMI) satellite observations to inform about the decrease in anthropogenic emissions of nitrogen oxides (NOx) in 2019 compared with 2005 at regional to national scales in Europe. Both the OMI and TROPOMI inversions show decreases in European NOx anthropogenic emission budgets in 2019 compared to 2005 but with different magnitudes.
Yawen Kong, Bo Zheng, and Yuxi Liu
Atmos. Chem. Phys., 25, 5959–5976, https://doi.org/10.5194/acp-25-5959-2025, https://doi.org/10.5194/acp-25-5959-2025, 2025
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Current high-resolution satellite remote sensing technologies provide a unique opportunity to derive timely high-resolution emission data. We developed an emission inversion system to assimilate satellite NO2 data to obtain daily kilometer-scale NOx emission inventories. Our results enhance inventory accuracy, allowing us to capture the effects of pollution control policies on daily emissions (e.g., during COVID-19 lockdowns) and improve fine-scale air quality modeling.
Yann Cohen, Didier Hauglustaine, Nicolas Bellouin, Marianne Tronstad Lund, Sigrun Matthes, Agnieszka Skowron, Robin Thor, Ulrich Bundke, Andreas Petzold, Susanne Rohs, Valérie Thouret, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 25, 5793–5836, https://doi.org/10.5194/acp-25-5793-2025, https://doi.org/10.5194/acp-25-5793-2025, 2025
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The chemical composition of the atmosphere near the tropopause is a key parameter for evaluating the climate impact of subsonic aviation pollutants. This study uses in situ data collected aboard passenger aircraft to assess the ability of four chemistry–climate models to reproduce (bi-)decadal climatologies of ozone, carbon monoxide, water vapour, and reactive nitrogen in this region. The models reproduce the very distinct ozone seasonality in the upper troposphere and in the lower stratosphere well.
Yafang Guo, Mohammad Amin Mirrezaei, Armin Sorooshian, and Avelino F. Arellano
Atmos. Chem. Phys., 25, 5591–5616, https://doi.org/10.5194/acp-25-5591-2025, https://doi.org/10.5194/acp-25-5591-2025, 2025
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We assess the contributions of fire and anthropogenic emissions to O3 levels in Phoenix, Arizona, during a period of intense heat and drought conditions. We find that fire exacerbates O3 pollution and that interactions between weather, climate, and air chemistry are important to consider. This has implications for activities related to formulating emission reduction strategies in areas that are currently understudied yet becoming relevant due to reports of increasing global aridity.
Yujia Wang, Hongbin Wang, Bo Zhang, Peng Liu, Xinfeng Wang, Shuchun Si, Likun Xue, Qingzhu Zhang, and Qiao Wang
Atmos. Chem. Phys., 25, 5537–5555, https://doi.org/10.5194/acp-25-5537-2025, https://doi.org/10.5194/acp-25-5537-2025, 2025
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This study established a bottom-up approach that employs real-time traffic flows and interpolation to obtain a spatially continuous on-road vehicle emission mapping for the main urban area of Jinan. The diurnal variation, spatial distribution, and emission hotspots were analyzed with clustering and hotspot analysis, showing unique fine-scale variation characteristics of on-road vehicle emissions. Future scenario analysis demonstrates remarkable benefits of electrification on emission reduction.
Francisco J. Pérez-Invernón, Francisco J. Gordillo-Vázquez, Heidi Huntrieser, Patrick Jöckel, and Eric J. Bucsela
Atmos. Chem. Phys., 25, 5557–5575, https://doi.org/10.5194/acp-25-5557-2025, https://doi.org/10.5194/acp-25-5557-2025, 2025
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Lightning plays a significant role in tropospheric chemistry by producing substantial amounts of nitrogen oxides. According to recent estimates, thunderstorms that produce a higher lightning frequency rate also produce less nitrogen oxide per flash. We implemented the dependency of nitrogen oxide production per flash on lightning flash frequency in a chemical atmospheric model.
Aditya Nalam, Aura Lupaşcu, Tabish Ansari, and Tim Butler
Atmos. Chem. Phys., 25, 5287–5311, https://doi.org/10.5194/acp-25-5287-2025, https://doi.org/10.5194/acp-25-5287-2025, 2025
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Tropospheric O3 molecules are labeled with the identity of their precursor source to simulate contributions from various emission sources to the global tropospheric O3 burden (TOB) and its trends. With an equatorward shift, anthropogenic NOx emissions become significantly more efficient at producing O3 and play a major role in driving TOB trends, mainly due to larger convection at the tropics effectively lifting O3 and its precursors to the free troposphere, where O3 lifetime is longer.
Haofan Wang, Yuejin Li, Yiming Liu, Xiao Lu, Yang Zhang, Qi Fan, Chong Shen, Senchao Lai, Yan Zhou, Tao Zhang, and Dingli Yue
Atmos. Chem. Phys., 25, 5233–5250, https://doi.org/10.5194/acp-25-5233-2025, https://doi.org/10.5194/acp-25-5233-2025, 2025
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This study explores how urban green spaces (UGSs) in Guangzhou influence ozone levels. By using advanced models, we found that natural emissions from these areas can significantly affect air quality. Our results suggest that the design and planning of UGSs should not only consider aesthetics and social factors but also their environmental impacts on air quality.
Laura Stecher, Franziska Winterstein, Patrick Jöckel, Michael Ponater, Mariano Mertens, and Martin Dameris
Atmos. Chem. Phys., 25, 5133–5158, https://doi.org/10.5194/acp-25-5133-2025, https://doi.org/10.5194/acp-25-5133-2025, 2025
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Methane, the second most important anthropogenic greenhouse gas, is chemically decomposed in the atmosphere. The chemical sink of atmospheric methane is not constant but depends on the temperature and on the abundance of its reaction partners. In this study, we use a global chemistry–climate model to assess the feedback of atmospheric methane induced by changes in the chemical sink in a warming climate and its implications for the chemical composition and the surface air temperature change.
Kai-Lan Chang, Brian C. McDonald, Colin Harkins, and Owen R. Cooper
Atmos. Chem. Phys., 25, 5101–5132, https://doi.org/10.5194/acp-25-5101-2025, https://doi.org/10.5194/acp-25-5101-2025, 2025
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Exposure to high levels of ozone can be harmful to human health. This study shows consistent and robust evidence of decreasing ozone extremes across much of the United States over the period from 1990 to 2023, previously attributed to ozone precursor emission controls. Nevertheless, we also show that the increasing heat wave frequencies are likely to contribute to additional ozone exceedances, slowing the progress of decreasing the frequency of ozone exceedances.
Ragnhild Bieltvedt Skeie, Marit Sandstad, Srinath Krishnan, Gunnar Myhre, and Maria Sand
Atmos. Chem. Phys., 25, 4929–4942, https://doi.org/10.5194/acp-25-4929-2025, https://doi.org/10.5194/acp-25-4929-2025, 2025
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Hydrogen leakages can alter the amount of climate gases in the atmosphere and hence have a climate impact. In this study we investigate, using an atmospheric chemistry model, how this indirect climate effect differs with different amounts of leakages and with where the hydrogen leaks and if this effect changes in the future. The effect is largest for emissions far from areas where hydrogen is removed from the atmosphere by the soil, but these are not relevant locations for a future hydrogen economy.
Alok K. Pandey, David S. Stevenson, Alcide Zhao, Richard J. Pope, Ryan Hossaini, Krishan Kumar, and Martyn P. Chipperfield
Atmos. Chem. Phys., 25, 4785–4802, https://doi.org/10.5194/acp-25-4785-2025, https://doi.org/10.5194/acp-25-4785-2025, 2025
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Nitrogen dioxide is an air pollutant largely controlled by human activity that affects ozone, methane, and aerosols. Satellite instruments can quantify column NO2 and, by carefully matching the time and location of measurements, enable evaluation of model simulations. NO2 over south and east Asia is assessed, showing that the model captures not only many features of the measurements, but also important differences that suggest model deficiencies in representing several aspects of the atmospheric chemistry of NO2.
Ryan Vella, Sergey Gromov, Clara M. Nussbaumer, Laura Stecher, Matthias Kohl, Samuel Ruhl, Holger Tost, Jos Lelieveld, and Andrea Pozzer
EGUsphere, https://doi.org/10.5194/egusphere-2025-1800, https://doi.org/10.5194/egusphere-2025-1800, 2025
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We evaluated how replacing forests with farmland and grazing areas affects atmospheric composition. Using a global climate-chemistry model, we found that deforestation reduces BVOCs, increases farming pollutants, and shifts ozone chemistry. These changes lead to a small cooling effect on the climate. Restoring natural vegetation could reverse some of these effects.
Mingzhao Liu, Lars Hoffmann, Jens-Uwe Grooß, Zhongyin Cai, Sabine Grießbach, and Yi Heng
Atmos. Chem. Phys., 25, 4403–4418, https://doi.org/10.5194/acp-25-4403-2025, https://doi.org/10.5194/acp-25-4403-2025, 2025
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We studied the transport and chemical decomposition of volcanic SO2, focusing on the 2019 Raikoke event. By comparing two different chemistry modeling schemes, we found that including complex chemical reactions leads to a more accurate prediction of how long SO2 stays in the atmosphere. This research helps improve our understanding of volcanic pollution and its impact on air quality and climate, providing better tools for scientists to track and predict the movement of these pollutants.
Yufen Wang, Ke Li, Xi Chen, Zhenjiang Yang, Minglong Tang, Pascoal M. D. Campos, Yang Yang, Xu Yue, and Hong Liao
Atmos. Chem. Phys., 25, 4455–4475, https://doi.org/10.5194/acp-25-4455-2025, https://doi.org/10.5194/acp-25-4455-2025, 2025
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The impacts of biomass burning and anthropogenic emissions on high tropospheric ozone levels are not well studied in southern Africa. We combined model simulations with recent observations at the surface and from space to quantify tropospheric ozone and its drivers in southern Africa. Our work focuses on the impact of emissions from different sources at different spatial scales, contributing to a comprehensive understanding of air pollution drivers and their uncertainties in southern Africa.
Dominika Pasik, Thomas Golin Almeida, Emelda Ahongshangbam, Siddharth Iyer, and Nanna Myllys
Atmos. Chem. Phys., 25, 4313–4331, https://doi.org/10.5194/acp-25-4313-2025, https://doi.org/10.5194/acp-25-4313-2025, 2025
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We used quantum chemistry methods to investigate the oxidation mechanisms of acyl peroxy radicals (APRs) with various monoterpenes. Our findings reveal unique oxidation pathways for different monoterpenes, leading to either chain-terminating products or highly reactive intermediates that can contribute to particle formation in the atmosphere. This research highlights APRs as potentially significant but underexplored atmospheric oxidants that may influence future approaches to modelling climate.
Jincheol Park, Yunsoo Choi, and Sagun Kayastha
Atmos. Chem. Phys., 25, 4291–4311, https://doi.org/10.5194/acp-25-4291-2025, https://doi.org/10.5194/acp-25-4291-2025, 2025
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We investigated NOx emission contributions to NOy loadings across five regions of East Asia during the 2022 winter–spring transition through chemical transport modeling informed by satellite data. As seasons progress, local contributions within each region to its NOy budget decreased from 32 %–43 % to 23 %–30 %, while transboundary contributions increased from 16 %–33 % to 27 %–37 %, driven by a shift in synoptic settings that allowed pollutants to spread more broadly across the regions.
Yuwen Peng, Bin Yuan, Sihang Wang, Xin Song, Zhe Peng, Wenjie Wang, Suxia Yang, Jipeng Qi, Xianjun He, Yibo Huangfu, Xiao-Bing Li, and Min Shao
EGUsphere, https://doi.org/10.5194/egusphere-2025-1649, https://doi.org/10.5194/egusphere-2025-1649, 2025
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A structural-based parameterization for the photolysis rates of oxygenated volatile organic compounds (OVOCs) was integrated into an updated chemical mechanism. This method links photolysis rates to species' structure, bypassing limitations of insufficient quantum yield data. Box model results show that non-HCHO OVOCs, particularly multifunctional carbonyl compounds, significantly contribute to radical production, with alkene and aromatic oxidation products playing key roles.
Qianqian Zhang, K. Folkert Boersma, Chiel van der Laan, Alba Mols, Bin Zhao, Shengyue Li, and Yuepeng Pan
Atmos. Chem. Phys., 25, 3313–3326, https://doi.org/10.5194/acp-25-3313-2025, https://doi.org/10.5194/acp-25-3313-2025, 2025
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Accurate NOx emission estimates are required to better understand air pollution. This study investigates and demonstrates the ability of the superposition column model in combination with TROPOMI tropospheric NO2 column data to estimate city-scale NOx emissions and lifetimes and their variabilities. The results of this work nevertheless confirm the strength of the superposition column model in estimating urban NOx emissions with reasonable accuracy.
Wenbin Kou, Yang Gao, Dan Tong, Xiaojie Guo, Xiadong An, Wenyu Liu, Mengshi Cui, Xiuwen Guo, Shaoqing Zhang, Huiwang Gao, and Lixin Wu
Atmos. Chem. Phys., 25, 3029–3048, https://doi.org/10.5194/acp-25-3029-2025, https://doi.org/10.5194/acp-25-3029-2025, 2025
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Unlike traditional numerical studies, we apply a high-resolution Earth system model, improving simulations of surface ozone and large-scale circulations such as atmospheric blocking. Besides local heat waves, we quantify the impact of atmospheric blocking on downstream ozone concentrations, which is closely associated with the blocking position. We identify three major pathways of Rossby wave propagation, stressing the critical role of large-scale circulation in regional air quality.
Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther
Atmos. Chem. Phys., 25, 2863–2894, https://doi.org/10.5194/acp-25-2863-2025, https://doi.org/10.5194/acp-25-2863-2025, 2025
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Vegetation releases biogenic volatile organic compounds, while soils and lightning contribute to the natural emissions of nitrogen oxides into the atmosphere. These gases interact in complex ways. Using satellite data and models, we developed a new method to simultaneously optimize these natural emissions over Africa in 2019. Our approach resulted in an increase in natural emissions, supported by independent data indicating that current estimates are underestimated.
Xiaobo Wang, Yuzhong Zhang, Tamás Bozóki, Ruosi Liang, Xinchun Xie, Shutao Zhao, Rui Wang, Yujia Zhao, and Shuai Sun
EGUsphere, https://doi.org/10.5194/egusphere-2025-370, https://doi.org/10.5194/egusphere-2025-370, 2025
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Schumann Resonance observations are used to parameterize lightning NOx emissions for better capturing global lightning trend and variability. Updated simulations reveal insignificant trend but greater variability in lightning NOx emissions, impacting tropospheric NOx, O3 and OH. Lightning generally counteracts non-lightning factors, reducing the inter-annua variability of tropospheric O3 and OH. Variations of global lightning play important role in understanding the atmospheric methane budget.
Xi Chen, Ke Li, Ting Yang, Xipeng Jin, Lei Chen, Yang Yang, Shuman Zhao, Bo Hu, Bin Zhu, Zifa Wang, and Hong Liao
EGUsphere, https://doi.org/10.5194/egusphere-2025-430, https://doi.org/10.5194/egusphere-2025-430, 2025
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Aerosol vertical distribution that plays a crucial role in aerosol-photolysis interaction (API) remains underrepresented in chemical models. We integrated lidar and radiosonde observations to constrain the simulated aerosol profiles over North China and quantified the photochemical responses. The increased photolysis rates in the lower layers led to increased ozone and accounted for a 36 %–56 % reduction in API effects, resulting in enhanced atmospheric oxidizing capacity and aerosol formation.
Jiaqi Shen, Ronald C. Cohen, Glenn M. Wolfe, and Xiaomeng Jin
EGUsphere, https://doi.org/10.5194/egusphere-2025-706, https://doi.org/10.5194/egusphere-2025-706, 2025
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This study shows large chemical and radiative effects of smoke aerosols from fires on near-surface ozone production. Aerosol loading and NOx levels are identified as the primary factors influencing these effects. Furthermore, we show that the surface PM2.5 to NO2 column ratio can be used as an indicator for identifying aerosol-dominated regimes, facilitating the assessments of aerosol impacts on ozone formation through satellite observations.
Shuai Li, Haolin Wang, and Xiao Lu
Atmos. Chem. Phys., 25, 2725–2743, https://doi.org/10.5194/acp-25-2725-2025, https://doi.org/10.5194/acp-25-2725-2025, 2025
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Summertime ozone–temperature sensitivity has decreased by 50 % from 3.0 ppbv per K in 1990 to 1.5 ppb per K in 2021 in the US. GEOS-Chem simulations show that anthropogenic nitrogen oxide emission reduction is the dominant driver of ozone–temperature sensitivity decline by influencing both temperature direct and temperature indirect processes. Reduced ozone–temperature sensitivity has decreased ozone enhancement from low to high temperatures by an average of 6.8 ppbv across the US.
Jinya Yang, Yutong Wang, Lei Zhang, and Yu Zhao
Atmos. Chem. Phys., 25, 2649–2666, https://doi.org/10.5194/acp-25-2649-2025, https://doi.org/10.5194/acp-25-2649-2025, 2025
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We develop a modeling framework to predict future ozone concentrations (till the 2060s) in China following an IPCC scenario. We evaluate the contributions of climatic, anthropogenic, and biogenic factors by season and region. We find persistent emission controls will alter the nonlinear response of ozone to its precursors and dominate the declining ozone level. The outcomes highlight the importance of human actions, even with a climate penalty on air quality.
Xiaodong Zhang, Yu Yan, Ning Zhang, Wenpeng Wang, Huabing Suo, Xiaohu Jian, Chao Wang, Haibo Ma, Hong Gao, Zhaoli Yang, Tao Huang, and Jianmin Ma
EGUsphere, https://doi.org/10.5194/egusphere-2025-258, https://doi.org/10.5194/egusphere-2025-258, 2025
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This study performed comprehensive sensitivity model simulations to explore the surface O3 responses to historical and projected climate change in Northwestern China (NW). Our results reveal that substantial wetting trends since the 21st century have mitigated O3 growth in this region, with the influence of wetting on O3 evolution outweighing the warming effect. These findings should be taken into account in future policymaking aimed at scientifically reducing O3 pollution in NW.
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
Atmos. Chem. Phys., 25, 2243–2268, https://doi.org/10.5194/acp-25-2243-2025, https://doi.org/10.5194/acp-25-2243-2025, 2025
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Five global chemical reanalysis datasets were used to assess the relative impacts of assimilating satellite ozone and its precursor measurements on tropospheric ozone analyses for 2010. The multiple reanalysis system comparison allows an evaluation of the 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 magnitudes among the systems.
Maureen Beaudor, Didier Hauglustaine, Juliette Lathière, Martin Van Damme, Lieven Clarisse, and Nicolas Vuichard
Atmos. Chem. Phys., 25, 2017–2046, https://doi.org/10.5194/acp-25-2017-2025, https://doi.org/10.5194/acp-25-2017-2025, 2025
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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, with significant changes in radiative forcing that can greatly elevate N2O.
Hui Li, Jiaxin Qiu, and Bo Zheng
Atmos. Chem. Phys., 25, 1949–1963, https://doi.org/10.5194/acp-25-1949-2025, https://doi.org/10.5194/acp-25-1949-2025, 2025
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We conduct a sensitivity analysis with 31 tests on various factors including prior emissions, model resolution, satellite constraint, and other system configurations to assess the vulnerability of emission estimates across temporal, sectoral, and regional dimensions. This reveals the robustness of emissions estimated by this air-pollution-satellite-based CO2 emission inversion system, with relative change between tests and base inversion below 4.0 % for national annual NOx and CO2 emissions.
Yingying Hong, Yuqi Zhu, Yuxuan Huang, Yiming Liu, Chuqi Xiong, and Qi Fan
EGUsphere, https://doi.org/10.5194/egusphere-2024-4132, https://doi.org/10.5194/egusphere-2024-4132, 2025
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This study investigates the impact of sea spray aerosol on ozone formation across Eastern China, highlighting its complex influence through both chemical reactions and radiative effects, which vary seasonally and geographically.
Yuqing Qiu, Xin Li, Wenxuan Chai, Yi Liu, Mengdi Song, Xudong Tian, Qiaoli Zou, Wenjun Lou, Wangyao Zhang, Juan Li, and Yuanhang Zhang
Atmos. Chem. Phys., 25, 1749–1763, https://doi.org/10.5194/acp-25-1749-2025, https://doi.org/10.5194/acp-25-1749-2025, 2025
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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.
Qixiang Xu, Fangcheng Su, Ke Wang, Ruiqin Zhang, Qi Ying, and Michael J. Kleeman
EGUsphere, https://doi.org/10.5194/egusphere-2025-44, https://doi.org/10.5194/egusphere-2025-44, 2025
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This manuscript introduces a novel approach for improving the computational efficiency and scalability of source-oriented chemical mechanisms by simplifying the representation of reactions involving source-tagged species and implementing a source-oriented Euler Backward Iterative (EBI) solver. These advancements reduce simulation times by up to 74 % while maintaining accuracy, offering significant practical benefits for long-term source apportionment studies.
Jeongmin Yun, Junjie Liu, Brendan Byrne, Brad Weir, Lesley E. Ott, Kathryn McKain, Bianca C. Baier, Luciana V. Gatti, and Sebastien C. Biraud
Atmos. Chem. Phys., 25, 1725–1748, https://doi.org/10.5194/acp-25-1725-2025, https://doi.org/10.5194/acp-25-1725-2025, 2025
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This study quantifies errors in regional net surface–atmosphere CO2 flux estimates from an inverse model ensemble using airborne CO2 measurements. Our results show that flux error estimates based on observations significantly exceed those computed from the ensemble spread of flux estimates in regions with high fossil fuel emissions. This finding suggests the presence of systematic biases in the inversion estimates, associated with errors in the fossil fuel emissions common to all models.
Min Huang, Gregory R. Carmichael, Kevin W. Bowman, Isabelle De Smedt, Andreas Colliander, Michael H. Cosh, Sujay V. Kumar, Alex B. Guenther, Scott J. Janz, Ryan M. Stauffer, Anne M. Thompson, Niko M. Fedkin, Robert J. Swap, John D. Bolten, and Alicia T. Joseph
Atmos. Chem. Phys., 25, 1449–1476, https://doi.org/10.5194/acp-25-1449-2025, https://doi.org/10.5194/acp-25-1449-2025, 2025
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We use model simulations along with multiplatform, multidisciplinary observations and a range of analysis methods to estimate and understand the distributions, temporal changes, and impacts of reactive nitrogen and ozone over the most populous US region that has undergone significant environmental changes. Deposition, biogenic emissions, and extra-regional sources have been playing increasingly important roles in controlling pollutant budgets in this area as local anthropogenic emissions drop.
Xavier Faïn, Sophie Szopa, Vaishali Naïk, Patricia Martinerie, David M. Etheridge, Rachael H. Rhodes, Cathy M. Trudinger, Vasilii V. Petrenko, Kévin Fourteau, and Philip Place
Atmos. Chem. Phys., 25, 1105–1119, https://doi.org/10.5194/acp-25-1105-2025, https://doi.org/10.5194/acp-25-1105-2025, 2025
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Carbon monoxide (CO) plays a crucial role in the atmosphere's oxidizing capacity. In this study, we analyse how historical (1850–2014) [CO] outputs from state-of-the-art global chemistry–climate models over Greenland and Antarctica are able to capture both absolute values and trends recorded in multi-site ice archives. A disparity in [CO] growth rates emerges in the Northern Hemisphere between models and observations from 1920–1975 CE, possibly linked to uncertainties in CO emission factors.
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 Dieudonné, 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
Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, https://doi.org/10.5194/acp-25-1063-2025, 2025
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Processes influencing dispersion of local anthropogenic pollution in Arctic wintertime are investigated with Lagrangian dispersion modelling. Simulated power plant plume rise that considers temperature inversion layers improves results compared to observations (interior Alaska). Modelled 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.
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
Atmos. Chem. Phys., 25, 1121–1143, https://doi.org/10.5194/acp-25-1121-2025, https://doi.org/10.5194/acp-25-1121-2025, 2025
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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 increasingly important and impact air quality. This study uses a box model to evaluate how these emissions impact ozone in the Los Angeles Basin and quantifies the impact of gaseous cooking emissions. Accurate representation of these and other anthropogenic sources in inventories is crucial for informing effective air quality policies.
Xiaodan Ma, Jianping Huang, Michaela I. Hegglin, Patrick Jöckel, and Tianliang Zhao
Atmos. Chem. Phys., 25, 943–958, https://doi.org/10.5194/acp-25-943-2025, https://doi.org/10.5194/acp-25-943-2025, 2025
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Our research explored changes in ozone levels in the northwest Pacific region over 30 years, revealing a significant increase in the middle-to-upper troposphere, especially during spring and summer. This rise is influenced by both stratospheric and tropospheric sources, which affect climate and air quality in East Asia. This work underscores the need for continued study to understand underlying mechanisms.
Hiroo Hata, Norifumi Mizushima, and Tomohiko Ihara
Atmos. Chem. Phys., 25, 1037–1061, https://doi.org/10.5194/acp-25-1037-2025, https://doi.org/10.5194/acp-25-1037-2025, 2025
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The introduction of battery electric vehicles (BEVs) is expected to reduce the primary air pollutants from vehicular exhaust and evaporative emissions while reducing the anthropogenic heat produced by vehicles, ultimately mitigating the urban heat island (UHI) effect. This study revealed the impact of introducing BEVs on the decrease in the UHI effect and the impact of BEVs on the formation of tropospheric ozone and fine particulate matter in the Greater Tokyo Area of Japan.
Wanmin Gong, Stephen R. Beagley, Kenjiro Toyota, Henrik Skov, Jesper Heile Christensen, Alexandru Lupu, Diane Pendlebury, Junhua Zhang, Ulas Im, Yugo Kanaya, Alfonso Saiz-Lopez, Roberto Sommariva, Peter Effertz, John W. Halfacre, Nis Jepsen, Rigel Kivi, Theodore K. Koenig, Katrin Müller, Claus Nordstrøm, Irina Petropavlovskikh, Paul B. Shepson, William R. Simpson, Sverre Solberg, Ralf M. Staebler, David W. Tarasick, Roeland Van Malderen, and Mika Vestenius
EGUsphere, https://doi.org/10.5194/egusphere-2024-3750, https://doi.org/10.5194/egusphere-2024-3750, 2025
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This study showed that the springtime O3 depletion plays a critical role in driving the surface O3 seasonal cycle in Central Arctic. The O3 depletion events, while occurring most notably within the lowest few hundred metres above the Arctic Ocean, can induce a 5–7 % of loss in the pan-Arctic tropospheric O3 burden during springtime. The study also found an enhancement in O3 and NOy (mostly PAN) concentrations in the Arctic due to northern boreal wildfires, particularly at altitudes.
Nan Wang, Song Liu, Jiawei Xu, Yanyu Wang, Chun Li, Hua Lu, and Fumo Yang
EGUsphere, https://doi.org/10.5194/egusphere-2024-3771, https://doi.org/10.5194/egusphere-2024-3771, 2025
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We found that climate warming and changes in vegetation have increased biogenic volatile organic compound emissions in the Pearl River Delta region. These increasing natural emissions, mainly due to climate warming, are weakening the benefits of reducing man-made emission control, leading to higher ozone levels. This work helps us understand how climate change influences air quality and provides important insights for improving pollution control strategies in the future.
Ji Xia, Yi Zhou, Li Fang, Yingfei Qi, Dehao Li, Hong Liao, and Jianbing Jin
EGUsphere, https://doi.org/10.5194/egusphere-2024-3938, https://doi.org/10.5194/egusphere-2024-3938, 2025
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This study established an ammonia emission inventory in South Asia via assimilation-based inversion system. The posterior emissions, calculated by integrating the CEDS inventory and IASI satellite observations, showed significant improvement over the prior. Validation against various measurements all support our posterior emission. It offers valuable insights of ammonia emissions for policymakers and researchers aiming to develop air quality management and mitigation strategies there.
Catalina Poraicu, Jean-François Müller, Trissevgeni Stavrakou, Crist Amelynck, Bert W. D. Verreyken, Niels Schoon, Corinne Vigouroux, Nicolas Kumps, Jérôme Brioude, Pierre Tulet, and Camille Mouchel-Vallon
EGUsphere, https://doi.org/10.5194/egusphere-2024-3555, https://doi.org/10.5194/egusphere-2024-3555, 2025
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We investigated the sources and impacts of nitrogen oxides and organic compounds over a remote tropical island. High-resolution WRF-Chem simulations were evaluated using in situ, FTIR and satellite measurements. This work highlights gaps in current models, like missing sources of key organic compounds and inaccuracies in emission inventories, emphasizing the importance of improving chemical and dynamical processes in atmospheric modelling for budget estimates in tropical regions.
Carlos Gómez-Ortiz, Guillaume Monteil, Sourish Basu, and Marko Scholze
Atmos. Chem. Phys., 25, 397–424, https://doi.org/10.5194/acp-25-397-2025, https://doi.org/10.5194/acp-25-397-2025, 2025
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In this paper, we test new implementations of our inverse modeling tool to estimate the weekly and regional CO2 emissions from fossil fuels in Europe. We use synthetic atmospheric observations of CO2 and radiocarbon (14CO2) to trace emissions to their sources, while separating the natural and fossil CO2. Our tool accurately estimates fossil CO2 emissions in densely monitored regions like western/central Europe. This approach aids in developing strategies for reducing CO2 emissions.
David D. Parrish, Ian C. Faloona, and Richard G. Derwent
Atmos. Chem. Phys., 25, 263–289, https://doi.org/10.5194/acp-25-263-2025, https://doi.org/10.5194/acp-25-263-2025, 2025
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Observation-based estimates of contributions to maximum ozone (O3) concentrations show that background O3 can exceed the air quality standard of 70 ppb in the southwestern US, precluding standard attainment. Over the past 4 decades, US anthropogenic O3 has decreased by a factor of ~ 6.3, while wildfire contributions have increased, so that the background now dominates maximum concentrations, even in Los Angeles, and the occurrence of maximum O3 has shifted from the eastern to the western US.
William P. L. Carter, Jia Jiang, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 25, 199–242, https://doi.org/10.5194/acp-25-199-2025, https://doi.org/10.5194/acp-25-199-2025, 2025
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This paper describes the scientific basis for gas-phase atmospheric chemical mechanisms derived using the SAPRC mechanism generation system, MechGen. It can derive mechanisms for most organic compounds with C, H, O, or N atoms, including initial reactions of organics with OH, O3, NO3, and O3P or by photolysis, as well as the reactions of the various types of intermediates that are formed. The paper includes a description of areas of uncertainty where additional research and updates are needed.
María Cazorla, Melissa Trujillo, Rodrigo Seguel, and Laura Gallardo
EGUsphere, https://doi.org/10.5194/egusphere-2024-3720, https://doi.org/10.5194/egusphere-2024-3720, 2024
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The current climate emergency imposes the need to take actions in cities to curb ozone as a pollutant and a climate forcer. In this work we analyze how reducing the levels of ozone precursor would affect photochemical smog in Quito, Ecuador and Santiago, Chile. Results show that if environmental policy were implemented to reduce only nitrogen oxides, the production of ozone would increase substantially for which more integral solutions are needed.
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.
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