Articles | Volume 21, issue 20
https://doi.org/10.5194/acp-21-15663-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-15663-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Technical note
| 
20 Oct 2021
Technical note |
| 20 Oct 2021
| 20 Oct 2021
Technical note: AQMEII4 Activity 1: evaluation of wet and dry deposition schemes as an integral part of regional-scale air quality models
Stefano Galmarini
CORRESPONDING AUTHOR
Joint Research Centre, European Commission, Ispra, Italy
Paul Makar
Air Quality Modelling and Integration Section, Environment and Climate
Change Canada, Toronto, Canada
Olivia E. Clifton
National Center for Atmospheric Research, Boulder, CO, USA
NASA Goddard Institute for Space Studies, New York, NY, USA
Christian Hogrefe
CORRESPONDING AUTHOR
Office of Research and Development, U.S. Environmental Protection
Agency, Research Triangle Park, NC, USA
Jesse O. Bash
Office of Research and Development, U.S. Environmental Protection
Agency, Research Triangle Park, NC, USA
Roberto Bellasio
Enviroware srl, Concorezzo, MB, Italy
Roberto Bianconi
Enviroware srl, Concorezzo, MB, Italy
Johannes Bieser
Institute of Coastal Research, Helmholtz-Zentrum Geesthacht, Geesthacht, Germany
Tim Butler
Institute for Advanced Sustainability Studies, Potsdam, Germany
Jason Ducker
Earth, Ocean and Atmospheric Science, Florida State University,
Tallahassee, FL, USA
Johannes Flemming
European Centre for Medium-Range Weather Forecasts, Reading, UK
Alma Hodzic
National Center for Atmospheric Research, Boulder, CO, USA
Christopher D. Holmes
Earth, Ocean and Atmospheric Science, Florida State University,
Tallahassee, FL, USA
Ioannis Kioutsioukis
Laboratory of Atmospheric Physics, Department of Physics,
University of Patras, Patras, Greece
Richard Kranenburg
Netherlands Organization for Applied Scientific Research (TNO),
Utrecht, the Netherlands
Aurelia Lupascu
Institute for Advanced Sustainability Studies, Potsdam, Germany
Juan Luis Perez-Camanyo
Technical University of Madrid (UPM), Madrid, Spain
Jonathan Pleim
Office of Research and Development, U.S. Environmental Protection
Agency, Research Triangle Park, NC, USA
Young-Hee Ryu
Pohang University of Science and Technology (POSTECH), Pohang, South Korea
Roberto San Jose
Technical University of Madrid (UPM), Madrid, Spain
Donna Schwede
Office of Research and Development, U.S. Environmental Protection
Agency, Research Triangle Park, NC, USA
Sam Silva
Pacific Northwest National Laboratory, Richland, WA, USA
Ralf Wolke
Leibniz Institute for Tropospheric Research, Leipzig, Germany
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The article explores the impact of different representations of below-cloud scavenging on model biases. A new scavenging scheme and precipitation-phase partitioning improve the model's performance, with better SO42- scavenging and wet deposition of NO3- and NH4+.
Lisa Azzarello, Rebecca A. Washenfelder, Michael A. Robinson, Alessandro Franchin, Caroline C. Womack, Christopher D. Holmes, Steven S. Brown, Ann Middlebrook, Tim Newberger, Colm Sweeney, and Cora J. Young
Atmos. Chem. Phys., 23, 15643–15654, https://doi.org/10.5194/acp-23-15643-2023, https://doi.org/10.5194/acp-23-15643-2023, 2023
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We present a molecular size-resolved offline analysis of water-soluble brown carbon collected on an aircraft during FIREX-AQ. The smoke plumes were aged 0 to 5 h, where absorption was dominated by small molecular weight molecules, brown carbon absorption downwind did not consistently decrease, and the measurements differed from online absorption measurements of the same samples. We show how differences between online and offline absorption could be related to different measurement conditions.
Colin J. Lee, Paul A. Makar, and Joana Soares
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2023-185, https://doi.org/10.5194/gmd-2023-185, 2023
Revised manuscript has not been submitted
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Clustering is an analysis technique for finding similarities within datasets. We present a new implementation of the hierarchical clustering algorithm that is able to process much larger datasets than was previously possible, by spreading the program out over many connected computers in a high-performance computing system. We show airshed maps of a high-resolution regional model output domain, and find related air pollution profiles at monitoring stations separated by thousands of kilometers.
Xuanyi Zhang, Mark Gordon, Paul A. Makar, Timothy Jiang, Jonathan Davies, and David Tarasick
Atmos. Chem. Phys., 23, 13647–13664, https://doi.org/10.5194/acp-23-13647-2023, https://doi.org/10.5194/acp-23-13647-2023, 2023
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Measurements of ozone in the atmosphere were made in a forest downwind of oil sands mining and production facilities in northern Alberta. These measurements show that the emissions of other pollutants from oil sands production and processing reduce the amount of ozone in the forest. By using an atmospheric model combined with measurements, we find that the rate at which ozone is absorbed by the forest is lower than typical rates from similar measurements in other forests.
Chupeng Zhang, Shangfei Hai, Yang Gao, Yuhang Wang, Shaoqing Zhang, Lifang Sheng, Bin Zhao, Shuxiao Wang, Jingkun Jiang, Xin Huang, Xiaojing Shen, Junying Sun, Aura Lupascu, Manish Shrivastava, Jerome D. Fast, Wenxuan Cheng, Xiuwen Guo, Ming Chu, Nan Ma, Juan Hong, Qiaoqiao Wang, Xiaohong Yao, and Huiwang Gao
Atmos. Chem. Phys., 23, 10713–10730, https://doi.org/10.5194/acp-23-10713-2023, https://doi.org/10.5194/acp-23-10713-2023, 2023
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New particle formation is an important source of atmospheric particles, exerting critical influences on global climate. Numerical models are vital tools to understanding atmospheric particle evolution, which, however, suffer from large biases in simulating particle numbers. Here we improve the model chemical processes governing particle sizes and compositions. The improved model reveals substantial contributions of newly formed particles to climate through effects on cloud condensation nuclei.
Lea Fink, Matthias Karl, Volker Matthias, Sonia Oppo, Richard Kranenburg, Jeroen Kuenen, Sara Jutterström, Jana Moldanova, Elisa Majamäki, and Jukka-Pekka Jalkanen
Atmos. Chem. Phys., 23, 10163–10189, https://doi.org/10.5194/acp-23-10163-2023, https://doi.org/10.5194/acp-23-10163-2023, 2023
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The Mediterranean Sea is a heavily trafficked shipping area, and air quality monitoring stations in numerous cities along the Mediterranean coast have detected high levels of air pollutants originating from shipping emissions. The current study investigates how existing restrictions on shipping-related emissions to the atmosphere ensure compliance with legislation. Focus was laid on fine particles and particle species, which were simulated with five different chemical transport models.
Olivia E. Clifton, Donna Schwede, Christian Hogrefe, Jesse O. Bash, Sam Bland, Philip Cheung, Mhairi Coyle, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christopher D. Holmes, László Horváth, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Pérez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamás Weidinger, Zhiyong Wu, and Leiming Zhang
Atmos. Chem. Phys., 23, 9911–9961, https://doi.org/10.5194/acp-23-9911-2023, https://doi.org/10.5194/acp-23-9911-2023, 2023
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A primary sink of air pollutants is dry deposition. Dry deposition estimates differ across the models used to simulate atmospheric chemistry. Here, we introduce an effort to examine dry deposition schemes from atmospheric chemistry models. We provide our approach’s rationale, document the schemes, and describe datasets used to drive and evaluate the schemes. We also launch the analysis of results by evaluating against observations and identifying the processes leading to model–model differences.
Bryan K. Place, William T. Hutzell, K. Wyat Appel, Sara Farrell, Lukas Valin, Benjamin N. Murphy, Karl M. Seltzer, Golam Sarwar, Christine Allen, Ivan R. Piletic, Emma L. D'Ambro, Emily Saunders, Heather Simon, Ana Torres-Vasquez, Jonathan Pleim, Rebecca H. Schwantes, Matthew M. Coggon, Lu Xu, William R. Stockwell, and Havala O. T. Pye
Atmos. Chem. Phys., 23, 9173–9190, https://doi.org/10.5194/acp-23-9173-2023, https://doi.org/10.5194/acp-23-9173-2023, 2023
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Ground-level ozone is a pollutant with adverse human health and ecosystem effects. Air quality models allow scientists to understand the chemical production of ozone and demonstrate impacts of air quality management plans. In this work, the role of multiple systems in ozone production was investigated for the northeastern US in summer. Model updates to chemical reaction rates and monoterpene chemistry were most influential in decreasing predicted ozone and improving agreement with observations.
Christian Hogrefe, Jesse O. Bash, Jonathan E. Pleim, Donna B. Schwede, Robert C. Gilliam, Kristen M. Foley, K. Wyat Appel, and Rohit Mathur
Atmos. Chem. Phys., 23, 8119–8147, https://doi.org/10.5194/acp-23-8119-2023, https://doi.org/10.5194/acp-23-8119-2023, 2023
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Under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in the widely used CMAQ model. The results illustrate how these tools can provide insights into similarities and differences between the two CMAQ dry deposition options that affect simulated pollutant budgets and ecosystem impacts from atmospheric pollution.
Mark Gordon, Dane Blanchard, Timothy Jiang, Paul A. Makar, Ralf M. Staebler, Julian Aherne, Cris Mihele, and Xuanyi Zhang
Atmos. Chem. Phys., 23, 7241–7255, https://doi.org/10.5194/acp-23-7241-2023, https://doi.org/10.5194/acp-23-7241-2023, 2023
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Measurements of the gas sulfur dioxide (SO2) were made in a forest downwind of oil sands mining and production facilities in northern Alberta. These measurements tell us the rate at which SO2 is absorbed by the forest. The measured rate is much higher than what is currently used by air quality models, which is supported by a previous study in this region. This suggests that SO2 may have a much shorter lifetime in the atmosphere at this location than currently predicted by models.
Monica Crippa, Diego Guizzardi, Tim Butler, Terry Keating, Rosa Wu, Jacek Kaminski, Jeroen Kuenen, Junichi Kurokawa, Satoru Chatani, Tazuko Morikawa, George Pouliot, Jacinthe Racine, Michael D. Moran, Zbigniew Klimont, Patrick M. Manseau, Rabab Mashayekhi, Barron H. Henderson, Steven J. Smith, Harrison Suchyta, Marilena Muntean, Efisio Solazzo, Manjola Banja, Edwin Schaaf, Federico Pagani, Jung-Hun Woo, Jinseok Kim, Fabio Monforti-Ferrario, Enrico Pisoni, Junhua Zhang, David Niemi, Mourad Sassi, Tabish Ansari, and Kristen Foley
Earth Syst. Sci. Data, 15, 2667–2694, https://doi.org/10.5194/essd-15-2667-2023, https://doi.org/10.5194/essd-15-2667-2023, 2023
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This study responds to the global and regional atmospheric modelling community's need for a mosaic of air pollutant emissions with global coverage, long time series, spatially distributed data at a high time resolution, and a high sectoral resolution in order to enhance the understanding of transboundary air pollution. The mosaic approach to integrating official regional emission inventories with a global inventory based on a consistent methodology ensures policy-relevant results.
Johannes Bieser, David J. Amptmeijer, Ute Daewel, Joachim Kuss, Anne L. Soerensen, and Corinna Schrum
Geosci. Model Dev., 16, 2649–2688, https://doi.org/10.5194/gmd-16-2649-2023, https://doi.org/10.5194/gmd-16-2649-2023, 2023
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MERCY is a 3D model to study mercury (Hg) cycling in the ocean. Hg is a highly harmful pollutant regulated by the UN Minamata Convention on Mercury due to widespread human emissions. These emissions eventually reach the oceans, where Hg transforms into the even more toxic and bioaccumulative pollutant methylmercury. MERCY predicts the fate of Hg in the ocean and its buildup in the food chain. It is the first model to consider Hg accumulation in fish, a major source of Hg exposure for humans.
Debora Griffin, Jack Chen, Kerry Anderson, Paul Makar, Chris A. McLinden, Enrico Dammers, and Andre Fogal
EGUsphere, https://doi.org/10.5194/egusphere-2023-649, https://doi.org/10.5194/egusphere-2023-649, 2023
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Satellite-derived CO emissions provide new insights into the understanding of global CO emission rates from wildfires. We use TROPOMI satellite data to create a global inventory database of wildfire CO emissions. These satellite-derived wildfire emissions are used for the evaluation and improvement of existing fire emission inventories, and to examine how the wildfire CO emissions changed over the past two decades.
Joey C. Y. Lam, Amos P. K. Tai, Jason A. Ducker, and Christopher D. Holmes
Geosci. Model Dev., 16, 2323–2342, https://doi.org/10.5194/gmd-16-2323-2023, https://doi.org/10.5194/gmd-16-2323-2023, 2023
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We developed a new component within an atmospheric chemistry model to better simulate plant ecophysiological processes relevant for ozone air quality. We showed that it reduces simulated biases in plant uptake of ozone in prior models. The new model enables us to explore how future climatic changes affect air quality via affecting plants, examine ozone–vegetation interactions and feedbacks, and evaluate the impacts of changing atmospheric chemistry and climate on vegetation productivity.
Havala O. T. Pye, Bryan K. Place, Benjamin N. Murphy, Karl M. Seltzer, Emma L. D'Ambro, Christine Allen, Ivan R. Piletic, Sara Farrell, Rebecca H. Schwantes, Matthew M. Coggon, Emily Saunders, Lu Xu, Golam Sarwar, William T. Hutzell, Kristen M. Foley, George Pouliot, Jesse Bash, and William R. Stockwell
Atmos. Chem. Phys., 23, 5043–5099, https://doi.org/10.5194/acp-23-5043-2023, https://doi.org/10.5194/acp-23-5043-2023, 2023
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Chemical mechanisms describe how emissions from vehicles, vegetation, and other sources are chemically transformed in the atmosphere to secondary products including criteria and hazardous air pollutants. The Community Regional Atmospheric Chemistry Multiphase Mechanism integrates gas-phase radical chemistry with pathways to fine-particle mass. New species were implemented, resulting in a bottom-up representation of organic aerosol, which is required for accurate source attribution of pollutants.
Qian Shu, Sergey L. Napelenok, William T. Hutzell, Kirk R. Baker, Barron H. Henderson, Benjamin N. Murphy, and Christian Hogrefe
Geosci. Model Dev., 16, 2303–2322, https://doi.org/10.5194/gmd-16-2303-2023, https://doi.org/10.5194/gmd-16-2303-2023, 2023
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Source attribution methods are generally used to determine culpability of precursor emission sources to ambient pollutant concentrations. However, source attribution of secondarily formed pollutants such as ozone and its precursors cannot be explicitly measured, making evaluation of source apportionment methods challenging. In this study, multiple apportionment approach comparisons show common features but still reveal wide variations in predicted sector contribution and species dependency.
Iason Markantonis, Diamando Vlachogiannis, Athanasios Sfetsos, Ioannis Kioutsioukis, and Nadia Politi
Adv. Sci. Res., 19, 145–158, https://doi.org/10.5194/asr-19-145-2023, https://doi.org/10.5194/asr-19-145-2023, 2023
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This paper examines the simulataneous exceedance of daily accumulated precipitation (RR) and minimum (TN) temperature thresholds in Greece for the period 1980–2004 and for each month in the period November to April. Available data from observations and projection simulations are used to calculate the probabilities of extreme wet-cold compound events at the past. Models are validated by the observational data.
Timothy Jiang, Mark Gordon, Paul A. Makar, Ralf M. Staebler, and Michael Wheeler
Atmos. Chem. Phys., 23, 4361–4372, https://doi.org/10.5194/acp-23-4361-2023, https://doi.org/10.5194/acp-23-4361-2023, 2023
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Measurements of submicron aerosols (particles smaller than 1 / 1000 of a millimeter) were made in a forest downwind of oil sands mining and production facilities in northern Alberta. These measurements tell us how quickly aerosols are absorbed by the forest (known as deposition rate) and how the deposition rate depends on the size of the aerosol. The measurements show good agreement with a parameterization developed from a recent study for deposition of aerosols to a similar pine forest.
John T. Walker, Xi Chen, Zhiyong Wu, Donna Schwede, Ryan Daly, Aleksandra Djurkovic, A. Christopher Oishi, Eric Edgerton, Jesse Bash, Jennifer Knoepp, Melissa Puchalski, John Iiames, and Chelcy F. Miniat
Biogeosciences, 20, 971–995, https://doi.org/10.5194/bg-20-971-2023, https://doi.org/10.5194/bg-20-971-2023, 2023
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Better estimates of atmospheric nitrogen (N) deposition are needed to accurately assess ecosystem risk and impacts from deposition of nutrients and acidity. Using measurements and modeling, we estimate total N deposition of 6.7 kg N ha−1 yr−1 at a forest site in the southern Appalachian Mountains, a region sensitive to atmospheric deposition. Reductions in deposition of reduced forms of N (ammonia and ammonium) will be needed to meet the lowest estimates of N critical loads for the region.
Edward C. Chan, Joana Leitão, Andreas Kerschbaumer, and Timothy M. Butler
Geosci. Model Dev., 16, 1427–1444, https://doi.org/10.5194/gmd-16-1427-2023, https://doi.org/10.5194/gmd-16-1427-2023, 2023
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Yeti is a Handbook Emission Factors for Road Transport-based traffic emission inventory written in the Python 3 scripting language, which adopts a generalized treatment for activity data using traffic information of varying levels of detail introduced in a systematic and consistent manner, with the ability to maximize reusability. Thus, Yeti has been conceived and implemented with a high degree of data and process symmetry, allowing scalable and flexible execution while affording ease of use.
Lea Fink, Matthias Karl, Volker Matthias, Sonia Oppo, Richard Kranenburg, Jeroen Kuenen, Jana Moldanova, Sara Jutterström, Jukka-Pekka Jalkanen, and Elisa Majamäki
Atmos. Chem. Phys., 23, 1825–1862, https://doi.org/10.5194/acp-23-1825-2023, https://doi.org/10.5194/acp-23-1825-2023, 2023
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Potential ship impact on air pollution in the Mediterranean Sea was simulated with five chemistry transport models. An evaluation of the results for NO2 and O3 air concentrations and dry deposition is presented. Emission data, modeled year and domain were the same. Model run outputs were compared to measurements from background stations. We focused on comparing model outputs regarding the concentration of regulatory pollutants and the relative ship impact on total air pollution concentrations.
Felix Kleinert, Lukas H. Leufen, Aurelia Lupascu, Tim Butler, and Martin G. Schultz
Geosci. Model Dev., 15, 8913–8930, https://doi.org/10.5194/gmd-15-8913-2022, https://doi.org/10.5194/gmd-15-8913-2022, 2022
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We examine the effects of spatially aggregated upstream information as input for a deep learning model forecasting near-surface ozone levels. Using aggregated data from one upstream sector (45°) improves the forecast by ~ 10 % for 4 prediction days. Three upstream sectors improve the forecasts by ~ 14 % on the first 2 d only. Our results serve as an orientation for other researchers or environmental agencies focusing on pointwise time-series predictions, for example, due to regulatory purposes.
Brian T. Dinkelacker, Pablo Garcia Rivera, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Geosci. Model Dev., 15, 8899–8912, https://doi.org/10.5194/gmd-15-8899-2022, https://doi.org/10.5194/gmd-15-8899-2022, 2022
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The performance of a chemical transport model in reproducing PM2.5 concentrations and composition was evaluated at the finest scale using measurements from regulatory sites as well as a network of low-cost monitors. Total PM2.5 mass is reproduced well by the model during the winter when compared to regulatory measurements, but in the summer PM2.5 is underpredicted, mainly due to difficulties in reproducing regional secondary organic aerosol levels.
Daiwen Kang, Nicholas K. Heath, Robert C. Gilliam, Tanya L. Spero, and Jonathan E. Pleim
Geosci. Model Dev., 15, 8561–8579, https://doi.org/10.5194/gmd-15-8561-2022, https://doi.org/10.5194/gmd-15-8561-2022, 2022
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A lightning assimilation (LTA) technique implemented in the WRF model's Kain–Fritsch (KF) convective scheme is updated and applied to simulations from regional to hemispheric scales using observed lightning flashes from ground-based lightning detection networks. Different user-toggled options associated with the KF scheme on simulations with and without LTA are assessed. The model's performance is improved significantly by LTA, but it is sensitive to various factors.
Pascal Wintjen, Frederik Schrader, Martijn Schaap, Burkhard Beudert, Richard Kranenburg, and Christian Brümmer
Biogeosciences, 19, 5287–5311, https://doi.org/10.5194/bg-19-5287-2022, https://doi.org/10.5194/bg-19-5287-2022, 2022
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For the first time, we compared four methods for estimating the annual dry deposition of total reactive nitrogen into a low-polluted forest ecosystem. In our analysis, we used 2.5 years of flux measurements, an in situ modeling approach, a large-scale chemical transport model (CTM), and canopy budget models. Annual nitrogen dry deposition budgets ranged between 4.3 and 6.7 kg N ha−1 a−1, depending on the applied method.
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.
Iason Markantonis, Diamando Vlachogiannis, Athanasios Sfetsos, and Ioannis Kioutsioukis
Earth Syst. Dynam., 13, 1491–1504, https://doi.org/10.5194/esd-13-1491-2022, https://doi.org/10.5194/esd-13-1491-2022, 2022
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This work focuses on the study of daily wet–cold compound events in Greece in the period November–April. We firstly study the historic period 1980–2004 in which we validate projection models with observations. Then we compare the model results with future period 2025–2049 RCP4.5 and RCP8.5 scenarios. The aim of the study is to calculate the probability of the events and to locate the areas where those are higher and how the probabilities will change at the future.
Johana Romero-Alvarez, Aurelia Lupaşcu, Douglas Lowe, Alba Badia, Scott Archer-Nicholls, Steve Dorling, Claire E. Reeves, and Tim Butler
Atmos. Chem. Phys., 22, 13797–13815, https://doi.org/10.5194/acp-22-13797-2022, https://doi.org/10.5194/acp-22-13797-2022, 2022
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As ozone can be transported across countries, efficient air quality management and regulatory policies rely on the assessment of local ozone production vs. transport. In our study, we investigate the origin of surface ozone in the UK and the contribution of the different source regions to regulatory ozone metrics. It is shown that emission controls would be necessary over western Europe to improve health-related metrics and over larger areas to reduce impacts on ecosystems.
Sarah E. Benish, Jesse O. Bash, Kristen M. Foley, K. Wyat Appel, Christian Hogrefe, Robert Gilliam, and George Pouliot
Atmos. Chem. Phys., 22, 12749–12767, https://doi.org/10.5194/acp-22-12749-2022, https://doi.org/10.5194/acp-22-12749-2022, 2022
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We assess Community Multiscale Air Quality (CMAQ) model simulations of nitrogen and sulfur deposition over US climate regions to evaluate the model ability to reproduce long-term deposition trends and total deposition budgets. A measurement–model fusion technique is found to improve estimates of wet deposition. Emission controls set by the Clean Air Act successfully decreased oxidized nitrogen deposition across the US; we find increasing amounts of reduced nitrogen to the total nitrogen budget.
Aurelia Lupaşcu, Noelia Otero, Andrea Minkos, and Tim Butler
Atmos. Chem. Phys., 22, 11675–11699, https://doi.org/10.5194/acp-22-11675-2022, https://doi.org/10.5194/acp-22-11675-2022, 2022
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Ground-level ozone is an important air pollutant that affects human health, ecosystems, and climate. Ozone is not emitted directly but rather formed in the atmosphere through chemical reactions involving two distinct precursors. Our results provide detailed information about the origin of ozone in Germany during two peak ozone events that took place in 2015 and 2018, thus improving our understanding of ground-level ozone.
Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah A. Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, Benjamin A. Nault, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech., 15, 4901–4930, https://doi.org/10.5194/amt-15-4901-2022, https://doi.org/10.5194/amt-15-4901-2022, 2022
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Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
Christopher D. Holmes
Atmos. Chem. Phys., 22, 9011–9015, https://doi.org/10.5194/acp-22-9011-2022, https://doi.org/10.5194/acp-22-9011-2022, 2022
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Cloud water and ice enable reactions that lead to acid rain and alter atmospheric oxidants, among other impacts. This work develops and evaluates an efficient method of simulating cloud chemistry within global and regional atmospheric models in order to better understand the role of clouds in atmospheric chemistry.
Jean-Pierre Chaboureau, Laurent Labbouz, Cyrille Flamant, and Alma Hodzic
Atmos. Chem. Phys., 22, 8639–8658, https://doi.org/10.5194/acp-22-8639-2022, https://doi.org/10.5194/acp-22-8639-2022, 2022
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Ground-based, spaceborne and rare airborne observations of biomass burning aerosols (BBAs) during the AEROCLO-sA field campaign in 2017 are complemented with convection-permitting simulations with online trajectories. The results show that the radiative effect of the BBA accelerates the southern African easterly jet and generates upward motions that transport the BBAs to higher altitudes and farther southwest.
Jiandong Wang, Jia Xing, Shuxiao Wang, Rohit Mathur, Jiaping Wang, Yuqiang Zhang, Chao Liu, Jonathan Pleim, Dian Ding, Xing Chang, Jingkun Jiang, Peng Zhao, Shovan Kumar Sahu, Yuzhi Jin, David C. Wong, and Jiming Hao
Atmos. Chem. Phys., 22, 5147–5156, https://doi.org/10.5194/acp-22-5147-2022, https://doi.org/10.5194/acp-22-5147-2022, 2022
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Aerosols reduce surface solar radiation and change the photolysis rate and planetary boundary layer stability. In this study, the online coupled meteorological and chemistry model was used to explore the detailed pathway of how aerosol direct effects affect secondary inorganic aerosol. The effects through the dynamics pathway act as an equally or even more important route compared with the photolysis pathway in affecting secondary aerosol concentration in both summer and winter.
Shihan Sun, Amos P. K. Tai, David H. Y. Yung, Anthony Y. H. Wong, Jason A. Ducker, and Christopher D. Holmes
Biogeosciences, 19, 1753–1776, https://doi.org/10.5194/bg-19-1753-2022, https://doi.org/10.5194/bg-19-1753-2022, 2022
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We developed and used a terrestrial biosphere model to compare and evaluate widely used empirical dry deposition schemes with different stomatal approaches and found that using photosynthesis-based stomatal approaches can reduce biases in modeled dry deposition velocities in current chemical transport models. Our study shows systematic errors in current dry deposition schemes and the importance of representing plant ecophysiological processes in models under a changing climate.
Danilo Custódio, Katrine Aspmo Pfaffhuber, T. Gerard Spain, Fidel F. Pankratov, Iana Strigunova, Koketso Molepo, Henrik Skov, Johannes Bieser, and Ralf Ebinghaus
Atmos. Chem. Phys., 22, 3827–3840, https://doi.org/10.5194/acp-22-3827-2022, https://doi.org/10.5194/acp-22-3827-2022, 2022
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As a poison in the air that we breathe and the food that we eat, mercury is a human health concern for society as a whole. In that regard, this work deals with monitoring and modelling mercury in the environment, improving wherewithal, identifying the strength of the different components at play, and interpreting information to support the efforts that seek to safeguard public health.
Pablo Garcia Rivera, Brian T. Dinkelacker, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 22, 2011–2027, https://doi.org/10.5194/acp-22-2011-2022, https://doi.org/10.5194/acp-22-2011-2022, 2022
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The contribution of various pollution sources to the variability of fine PM in an urban area was examined using as an example the city of Pittsburgh. Biomass burning aerosol shows the largest variability during the winter with local maxima within the city and in the suburbs. During both periods the largest contributing source to the average PM2.5 is particles from outside the modeling domain. The average population-weighted PM2.5 concentration does not change significantly with resolution.
Noelia Otero, Oscar E. Jurado, Tim Butler, and Henning W. Rust
Atmos. Chem. Phys., 22, 1905–1919, https://doi.org/10.5194/acp-22-1905-2022, https://doi.org/10.5194/acp-22-1905-2022, 2022
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Surface ozone and temperature are strongly dependent and their extremes might be exacerbated by underlying climatological drivers, such as atmospheric blocking. Using an observational data set, we measure the dependence structure between ozone and temperature under the influence of atmospheric blocking. Blocks enhanced the probability of occurrence of compound ozone and temperature extremes over northwestern and central Europe, leading to greater health risks.
Shelley van der Graaf, Enrico Dammers, Arjo Segers, Richard Kranenburg, Martijn Schaap, Mark W. Shephard, and Jan Willem Erisman
Atmos. Chem. Phys., 22, 951–972, https://doi.org/10.5194/acp-22-951-2022, https://doi.org/10.5194/acp-22-951-2022, 2022
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CrIS NH3 satellite observations are assimilated into the LOTOS-EUROS model using two different methods. In the first method the data are used to fit spatially varying NH3 emission time factors. In the second method a local ensemble transform Kalman filter is used. Compared to in situ observations, combining both methods led to the most significant improvements in the modeled concentrations and deposition, illustrating the usefulness of CrIS NH3 to improve the spatiotemporal distribution of NH3.
Mahtab Majdzadeh, Craig A. Stroud, Christopher Sioris, Paul A. Makar, Ayodeji Akingunola, Chris McLinden, Xiaoyi Zhao, Michael D. Moran, Ihab Abboud, and Jack Chen
Geosci. Model Dev., 15, 219–249, https://doi.org/10.5194/gmd-15-219-2022, https://doi.org/10.5194/gmd-15-219-2022, 2022
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A new lookup table for aerosol optical properties based on a Mie scattering code was calculated and adopted within an improved version of the photolysis module in the GEM-MACH in-line chemical transport model. The modified version of the photolysis module makes use of online interactive aerosol feedback and applies core-shell parameterizations to the black carbon absorption efficiency based on Bond et al. (2006) to the size bins with black carbon mass fraction of less than 40 %.
Debora Griffin, Chris A. McLinden, Enrico Dammers, Cristen Adams, Chelsea E. Stockwell, Carsten Warneke, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Kyle J. Zarzana, Jake P. Rowe, Rainer Volkamer, Christoph Knote, Natalie Kille, Theodore K. Koenig, Christopher F. Lee, Drew Rollins, Pamela S. Rickly, Jack Chen, Lukas Fehr, Adam Bourassa, Doug Degenstein, Katherine Hayden, Cristian Mihele, Sumi N. Wren, John Liggio, Ayodeji Akingunola, and Paul Makar
Atmos. Meas. Tech., 14, 7929–7957, https://doi.org/10.5194/amt-14-7929-2021, https://doi.org/10.5194/amt-14-7929-2021, 2021
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Satellite-derived NOx emissions from biomass burning are estimated with TROPOMI observations. Two common emission estimation methods are applied, and sensitivity tests with model output were performed to determine the accuracy of these methods. The effect of smoke aerosols on TROPOMI NO2 columns is estimated and compared to aircraft observations from four different aircraft campaigns measuring biomass burning plumes in 2018 and 2019 in North America.
Jin Liao, Glenn M. Wolfe, Reem A. Hannun, Jason M. St. Clair, Thomas F. Hanisco, Jessica B. Gilman, Aaron Lamplugh, Vanessa Selimovic, Glenn S. Diskin, John B. Nowak, Hannah S. Halliday, Joshua P. DiGangi, Samuel R. Hall, Kirk Ullmann, Christopher D. Holmes, Charles H. Fite, Anxhelo Agastra, Thomas B. Ryerson, Jeff Peischl, Ilann Bourgeois, Carsten Warneke, Matthew M. Coggon, Georgios I. Gkatzelis, Kanako Sekimoto, Alan Fried, Dirk Richter, Petter Weibring, Eric C. Apel, Rebecca S. Hornbrook, Steven S. Brown, Caroline C. Womack, Michael A. Robinson, Rebecca A. Washenfelder, Patrick R. Veres, and J. Andrew Neuman
Atmos. Chem. Phys., 21, 18319–18331, https://doi.org/10.5194/acp-21-18319-2021, https://doi.org/10.5194/acp-21-18319-2021, 2021
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Formaldehyde (HCHO) is an important oxidant precursor and affects the formation of O3 and other secondary pollutants in wildfire plumes. We disentangle the processes controlling HCHO evolution from wildfire plumes sampled by NASA DC-8 during FIREX-AQ. We find that OH abundance rather than normalized OH reactivity is the main driver of fire-to-fire variability in HCHO secondary production and estimate an effective HCHO yield per volatile organic compound molecule oxidized in wildfire plumes.
Kai Wang, Yang Zhang, Shaocai Yu, David C. Wong, Jonathan Pleim, Rohit Mathur, James T. Kelly, and Michelle Bell
Geosci. Model Dev., 14, 7189–7221, https://doi.org/10.5194/gmd-14-7189-2021, https://doi.org/10.5194/gmd-14-7189-2021, 2021
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The two-way coupled WRF-CMAQ model accounting for complex chemistry–meteorology feedbacks has been applied to the long-term predictions of regional meteorology and air quality over the US. The model results show superior performance and importance of chemistry–meteorology feedbacks when compared to the offline coupled WRF and CMAQ simulations, which suggests that feedbacks should be considered along with other factors in developing future model applications to inform policy making.
Ksakousti Skyllakou, Pablo Garcia Rivera, Brian Dinkelacker, Eleni Karnezi, Ioannis Kioutsioukis, Carlos Hernandez, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 17115–17132, https://doi.org/10.5194/acp-21-17115-2021, https://doi.org/10.5194/acp-21-17115-2021, 2021
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Significant reductions in pollutant emissions took place in the US from 1990 to 2010. The reductions in sulfur dioxide emissions from electric-generating units have dominated the reductions in fine particle mass. The reductions in transportation emissions have led to a 30 % reduction of elemental concentrations and of organic particulate matter by a factor of 3. On the other hand, changes in biomass burning and biogenic secondary organic aerosol have been modest.
Nicole Jacobs, William R. Simpson, Kelly A. Graham, Christopher Holmes, Frank Hase, Thomas Blumenstock, Qiansi Tu, Matthias Frey, Manvendra K. Dubey, Harrison A. Parker, Debra Wunch, Rigel Kivi, Pauli Heikkinen, Justus Notholt, Christof Petri, and Thorsten Warneke
Atmos. Chem. Phys., 21, 16661–16687, https://doi.org/10.5194/acp-21-16661-2021, https://doi.org/10.5194/acp-21-16661-2021, 2021
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Spatial patterns of carbon dioxide seasonal cycle amplitude and summer drawdown timing derived from the OCO-2 satellite over northern high latitudes agree well with corresponding estimates from two models. The Asian boreal forest is anomalous with the largest amplitude and earliest seasonal drawdown. Modeled land contact tracers suggest that accumulated CO2 exchanges during atmospheric transport play a major role in shaping carbon dioxide seasonality in northern high-latitude regions.
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Georgios I. Gkatzelis, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Felix Piel, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Kanako Sekimoto, Lee Thornhill, Joel A. Thornton, Geoffrey S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Carsten Warneke, Rebecca A. Washenfelder, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Armin Wisthaler, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys., 21, 16293–16317, https://doi.org/10.5194/acp-21-16293-2021, https://doi.org/10.5194/acp-21-16293-2021, 2021
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To understand air quality impacts from wildfires, we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical
nighttimechemistry thrives and controls the fate of key smoke plume chemical processes.
Sepehr Fathi, Mark Gordon, Paul A. Makar, Ayodeji Akingunola, Andrea Darlington, John Liggio, Katherine Hayden, and Shao-Meng Li
Atmos. Chem. Phys., 21, 15461–15491, https://doi.org/10.5194/acp-21-15461-2021, https://doi.org/10.5194/acp-21-15461-2021, 2021
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We have investigated the accuracy of aircraft-based mass balance methodologies through computer model simulations of the atmosphere and air quality at a regional high-resolution scale. We have defined new quantitative metrics to reduce emission retrieval uncertainty by evaluating top-down mass balance estimates against the known simulated meteorology and input emissions. We also recommend methodologies and flight strategies for improved retrievals in future aircraft-based studies.
Xinxin Ye, Pargoal Arab, Ravan Ahmadov, Eric James, Georg A. Grell, Bradley Pierce, Aditya Kumar, Paul Makar, Jack Chen, Didier Davignon, Greg R. Carmichael, Gonzalo Ferrada, Jeff McQueen, Jianping Huang, Rajesh Kumar, Louisa Emmons, Farren L. Herron-Thorpe, Mark Parrington, Richard Engelen, Vincent-Henri Peuch, Arlindo da Silva, Amber Soja, Emily Gargulinski, Elizabeth Wiggins, Johnathan W. Hair, Marta Fenn, Taylor Shingler, Shobha Kondragunta, Alexei Lyapustin, Yujie Wang, Brent Holben, David M. Giles, and Pablo E. Saide
Atmos. Chem. Phys., 21, 14427–14469, https://doi.org/10.5194/acp-21-14427-2021, https://doi.org/10.5194/acp-21-14427-2021, 2021
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Wildfire smoke has crucial impacts on air quality, while uncertainties in the numerical forecasts remain significant. We present an evaluation of 12 real-time forecasting systems. Comparison of predicted smoke emissions suggests a large spread in magnitudes, with temporal patterns deviating from satellite detections. The performance for AOD and surface PM2.5 and their discrepancies highlighted the role of accurately represented spatiotemporal emission profiles in improving smoke forecasts.
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 %.
Syuichi Itahashi, Rohit Mathur, Christian Hogrefe, Sergey L. Napelenok, and Yang Zhang
Geosci. Model Dev., 14, 5751–5768, https://doi.org/10.5194/gmd-14-5751-2021, https://doi.org/10.5194/gmd-14-5751-2021, 2021
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The Community Multiscale Air Quality (CMAQ) modeling system extended for hemispheric-scale applications (H-CMAQ) incorporated the satellite-constrained degassing SO2 emissions from 50 volcanos across the Northern Hemisphere. The impact on tropospheric sulfate aerosol (SO42−) is assessed for 2010. Although the considered volcanic emissions occurred at or below the middle of free troposphere (500 hPa), SO42− enhancements of more than 10 % were detected up to the top of free troposphere (250 hPa).
Paul A. Makar, Craig Stroud, Ayodeji Akingunola, Junhua Zhang, Shuzhan Ren, Philip Cheung, and Qiong Zheng
Atmos. Chem. Phys., 21, 12291–12316, https://doi.org/10.5194/acp-21-12291-2021, https://doi.org/10.5194/acp-21-12291-2021, 2021
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Vehicle pollutant emissions occur in an environment where upward transport can be enhanced due to the turbulence created by the vehicles as they move through the atmosphere. An approach for including these turbulence effects in regional air pollution forecast models has been derived from theoretical, observation, and higher-resolution modeling. The enhanced mixing, which occurs in the immediate vicinity of roadways, changes pollutant concentrations on the regional to continental scale.
Zhiyong Wu, Leiming Zhang, John T. Walker, Paul A. Makar, Judith A. Perlinger, and Xuemei Wang
Geosci. Model Dev., 14, 5093–5105, https://doi.org/10.5194/gmd-14-5093-2021, https://doi.org/10.5194/gmd-14-5093-2021, 2021
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A community dry deposition algorithm for modeling the gaseous dry deposition process in chemistry transport models was extended to include an additional 12 oxidized volatile organic compounds and hydrogen cyanide based on their physicochemical properties and was then evaluated using field flux measurements over a mixed forest. This study provides a useful tool that is needed in chemistry transport models with increasing complexity for simulating an important atmospheric process.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Edward C. Chan and Timothy M. Butler
Geosci. Model Dev., 14, 4555–4572, https://doi.org/10.5194/gmd-14-4555-2021, https://doi.org/10.5194/gmd-14-4555-2021, 2021
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A large-eddy simulation based chemical transport model is implemented for an idealized street canyon. The dynamics of the model are evaluated using stationary measurements. A transient model run is also conducted over a 24 h period, where variations of pollutant concentrations indicate dependence on emissions, background concentrations, and solar state. Comparison stationary model runs show changes in flow structure concentrations.
Paul A. Makar, Ayodeji Akingunola, Jack Chen, Balbir Pabla, Wanmin Gong, Craig Stroud, Christopher Sioris, Kerry Anderson, Philip Cheung, Junhua Zhang, and Jason Milbrandt
Atmos. Chem. Phys., 21, 10557–10587, https://doi.org/10.5194/acp-21-10557-2021, https://doi.org/10.5194/acp-21-10557-2021, 2021
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We have examined the effects of airborne particles on absorption and scattering of incoming sunlight by the particles themselves via cloud formation. We used an advanced, combined high-resolution weather forecast and chemical transport computer model, for western North America, and simulations with and without the connections between particles and weather enabled. Feedbacks improved weather and air pollution forecasts and changed cloud behaviour and forest-fire pollutant amount and height.
Benjamin N. Murphy, Christopher G. Nolte, Fahim Sidi, Jesse O. Bash, K. Wyat Appel, Carey Jang, Daiwen Kang, James Kelly, Rohit Mathur, Sergey Napelenok, George Pouliot, and Havala O. T. Pye
Geosci. Model Dev., 14, 3407–3420, https://doi.org/10.5194/gmd-14-3407-2021, https://doi.org/10.5194/gmd-14-3407-2021, 2021
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The algorithms for applying air pollution emission rates in the Community Multiscale Air Quality (CMAQ) model have been improved to better support users and developers. The new features accommodate emissions perturbation studies that are typical in atmospheric research and output a wealth of metadata for each model run so assumptions can be verified and documented. The new approach dramatically enhances the transparency and functionality of this critical aspect of atmospheric modeling.
Katherine Hayden, Shao-Meng Li, Paul Makar, John Liggio, Samar G. Moussa, Ayodeji Akingunola, Robert McLaren, Ralf M. Staebler, Andrea Darlington, Jason O'Brien, Junhua Zhang, Mengistu Wolde, and Leiming Zhang
Atmos. Chem. Phys., 21, 8377–8392, https://doi.org/10.5194/acp-21-8377-2021, https://doi.org/10.5194/acp-21-8377-2021, 2021
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We developed a method using aircraft measurements to determine lifetimes with respect to dry deposition for oxidized sulfur and nitrogen compounds over the boreal forest in Alberta, Canada. Atmospheric lifetimes were significantly shorter than derived from chemical transport models with differences related to modelled dry deposition velocities. The shorter lifetimes suggest models need to reassess dry deposition treatment and predictions of sulfur and nitrogen in the atmosphere and ecosystems.
Sam J. Silva, Po-Lun Ma, Joseph C. Hardin, and Daniel Rothenberg
Geosci. Model Dev., 14, 3067–3077, https://doi.org/10.5194/gmd-14-3067-2021, https://doi.org/10.5194/gmd-14-3067-2021, 2021
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The activation of aerosol into cloud droplets is an important but uncertain process in the Earth system. The physical and chemical interactions that govern this process are too computationally expensive to explicitly resolve in modern Earth system models. Here, we demonstrate how hybrid machine learning approaches can provide a potential path forward, enabling the representation of the more detailed physics and chemistry at a reduced computational cost while still retaining physical information.
K. Wyat Appel, Jesse O. Bash, Kathleen M. Fahey, Kristen M. Foley, Robert C. Gilliam, Christian Hogrefe, William T. Hutzell, Daiwen Kang, Rohit Mathur, Benjamin N. Murphy, Sergey L. Napelenok, Christopher G. Nolte, Jonathan E. Pleim, George A. Pouliot, Havala O. T. Pye, Limei Ran, Shawn J. Roselle, Golam Sarwar, Donna B. Schwede, Fahim I. Sidi, Tanya L. Spero, and David C. Wong
Geosci. Model Dev., 14, 2867–2897, https://doi.org/10.5194/gmd-14-2867-2021, https://doi.org/10.5194/gmd-14-2867-2021, 2021
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This paper details the scientific updates in the recently released CMAQ version 5.3 (and v5.3.1) and also includes operational and diagnostic evaluations of CMAQv5.3.1 against observations and the previous version of the CMAQ (v5.2.1). This work was done to improve the underlying science in CMAQ. This article is used to inform the CMAQ modeling community of the updates to the modeling system and the expected change in model performance from these updates (versus the previous model version).
Qian Shu, Benjamin Murphy, Jonathan E. Pleim, Donna Schwede, Barron H. Henderson, Havala O.T. Pye, Keith Wyat Appel, Tanvir R. Khan, and Judith A. Perlinger
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-129, https://doi.org/10.5194/gmd-2021-129, 2021
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We have bridged the gap between dry deposition measurement and modeling by rigorous use of box and regional transport models and field measurements, but more efforts are needed. This study highlights that deviation among deposition schemes is most pronounced for small and large particles. This study better links model predictions to available real-world observations and incrementally reduces uncertainties in the magnitude of loss processes important for the lifecycle of air pollutants.
Matthias Faust, Ralf Wolke, Steffen Münch, Roger Funk, and Kerstin Schepanski
Geosci. Model Dev., 14, 2205–2220, https://doi.org/10.5194/gmd-14-2205-2021, https://doi.org/10.5194/gmd-14-2205-2021, 2021
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Trajectory dispersion models are powerful and intuitive tools for tracing air pollution through the atmosphere. But the turbulent nature of the atmospheric boundary layer makes it challenging to provide accurate predictions near the surface. To overcome this, we propose an approach using wind and turbulence information at high temporal resolution. Finally, we demonstrate the strength of our approach in a case study on dust emissions from agriculture.
Melinda K. Schueneman, Benjamin A. Nault, Pedro Campuzano-Jost, Duseong S. Jo, Douglas A. Day, Jason C. Schroder, Brett B. Palm, Alma Hodzic, Jack E. Dibb, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 2237–2260, https://doi.org/10.5194/amt-14-2237-2021, https://doi.org/10.5194/amt-14-2237-2021, 2021
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This work focuses on two important properties of the aerosol, acidity, and sulfate composition, which is important for our understanding of aerosol health and environmental impacts. We explore different methods to understand the composition of the aerosol with measurements from a specific instrument and apply those methods to a large dataset. These measurements are confounded by other factors, making it challenging to predict aerosol sulfate composition; pH estimations, however, show promise.
Elena Macdonald, Noelia Otero, and Tim Butler
Atmos. Chem. Phys., 21, 4007–4023, https://doi.org/10.5194/acp-21-4007-2021, https://doi.org/10.5194/acp-21-4007-2021, 2021
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NO2 limit values are still regularly exceeded in many European cities despite decreasing emissions. Measurements of NOx concentrations from stations across Europe were systematically analysed to assess long-term changes observed in urban areas. We compared trends in concentration increments to trends in total and traffic emissions to find potential discrepancies. The results can help in evaluating inaccuracies in emission inventories and in improving spatial imbalances in data availability.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 3395–3425, https://doi.org/10.5194/acp-21-3395-2021, https://doi.org/10.5194/acp-21-3395-2021, 2021
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Secondary organic aerosol (SOA) is a major component of submicron particulate matter, but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX SOA concentration changes. The explicit chemistry predicted substantial changes in IEPOX SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physicochemical dependencies in future SOA prediction.
Yilin Chen, Huizhong Shen, Jennifer Kaiser, Yongtao Hu, Shannon L. Capps, Shunliu Zhao, Amir Hakami, Jhih-Shyang Shih, Gertrude K. Pavur, Matthew D. Turner, Daven K. Henze, Jaroslav Resler, Athanasios Nenes, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Tianfeng Chai, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, and Armistead G. Russell
Atmos. Chem. Phys., 21, 2067–2082, https://doi.org/10.5194/acp-21-2067-2021, https://doi.org/10.5194/acp-21-2067-2021, 2021
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Ammonia (NH3) emissions can exert adverse impacts on air quality and ecosystem well-being. NH3 emission inventories are viewed as highly uncertain. Here we optimize the NH3 emission estimates in the US using an air quality model and NH3 measurements from the IASI satellite instruments. The optimized NH3 emissions are much higher than the National Emissions Inventory estimates in April. The optimized NH3 emissions improved model performance when evaluated against independent observation.
Xinrui Ge, Martijn Schaap, Richard Kranenburg, Arjo Segers, Gert Jan Reinds, Hans Kros, and Wim de Vries
Atmos. Chem. Phys., 20, 16055–16087, https://doi.org/10.5194/acp-20-16055-2020, https://doi.org/10.5194/acp-20-16055-2020, 2020
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This article is about improving the modeling of agricultural ammonia emissions. By considering land use, meteorology and agricultural practices, ammonia emission totals officially reported by countries are distributed in space and time. We illustrated the first step for a better understanding of the variability of ammonia emission, with the possibility of being applied at a European scale, which is of great significance for ammonia budget research and future policy-making.
Jianbing Jin, Arjo Segers, Hong Liao, Arnold Heemink, Richard Kranenburg, and Hai Xiang Lin
Atmos. Chem. Phys., 20, 15207–15225, https://doi.org/10.5194/acp-20-15207-2020, https://doi.org/10.5194/acp-20-15207-2020, 2020
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Data assimilation provides a powerful tool to estimate emission inventories by feeding observations. This emission inversion relies on the correct assumption about the emission uncertainty, which describes the potential spatiotemporal spreads of sources. However, an unrepresentative uncertainty is unavoidable. Especially in the complex dust emission, the uncertainties can hardly all be taken into account. This study reports how adjoint can be used to detect errors in the emission uncertainty.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Hongyu Guo, Duseong S. Jo, Anne V. Handschy, Demetrios Pagonis, Jason C. Schroder, Melinda K. Schueneman, Michael J. Cubison, Jack E. Dibb, Alma Hodzic, Weiwei Hu, Brett B. Palm, and Jose L. Jimenez
Atmos. Meas. Tech., 13, 6193–6213, https://doi.org/10.5194/amt-13-6193-2020, https://doi.org/10.5194/amt-13-6193-2020, 2020
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Collecting particulate matter, or aerosols, onto filters to be analyzed offline is a widely used method to investigate the mass concentration and chemical composition of the aerosol, especially the inorganic portion. Here, we show that acidic aerosol (sulfuric acid) collected onto filters and then exposed to high ammonia mixing ratios (from human emissions) will lead to biases in the ammonium collected onto filters, and the uptake of ammonia is rapid (< 10 s), which impacts the filter data.
Huiying Luo, Marina Astitha, Christian Hogrefe, Rohit Mathur, and S. Trivikrama Rao
Atmos. Chem. Phys., 20, 13801–13815, https://doi.org/10.5194/acp-20-13801-2020, https://doi.org/10.5194/acp-20-13801-2020, 2020
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A new method is introduced to evaluate nonlinear, nonstationary modeled PM2.5 time series by decomposing decadal PM2.5 concentrations and its species onto various timescales. It does not require preselection of temporal scales and assumptions of linearity and stationarity. It provides a unique opportunity to assess the influence of each species on total PM2.5. The results reveal a phase shift in modeled EC/OC concentrations, indicating the need for improved model treatment of organic aerosols.
Tim Butler, Aurelia Lupascu, and Aditya Nalam
Atmos. Chem. Phys., 20, 10707–10731, https://doi.org/10.5194/acp-20-10707-2020, https://doi.org/10.5194/acp-20-10707-2020, 2020
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Ground-level ozone (O3) is not directly emitted; it is formed chemically in the atmosphere. Some ground-level O3 is transported from the stratosphere, but most O3 is produced from reactive precursors that are emitted by both natural and anthropogenic sources. We present the results of a novel source apportionment method for ground-level O3. Our results are consistent with previous work and also provide new insights. In particular, we highlight the roles of methane and international shipping.
Johannes Bieser, Hélène Angot, Franz Slemr, and Lynwill Martin
Atmos. Chem. Phys., 20, 10427–10439, https://doi.org/10.5194/acp-20-10427-2020, https://doi.org/10.5194/acp-20-10427-2020, 2020
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We use numerical models to determine the origin of air masses measured for elemental gaseous mercury (GEM) at Cape Point (CPT), South Africa. Our analysis is based on 10 years of hourly GEM measurements at CPT from 2007 to 2016. Based on GEM concentration and the origin of the air mass, we identify source and sink regions at CPT. We find, that the warm Agulhas Current to the south-east is the major Hg source and the continent the major sink.
Ahmad Jhony Rusumdar, Andreas Tilgner, Ralf Wolke, and Hartmut Herrmann
Atmos. Chem. Phys., 20, 10351–10377, https://doi.org/10.5194/acp-20-10351-2020, https://doi.org/10.5194/acp-20-10351-2020, 2020
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In the present study, simulations with the SPACCIM-SpactMod multiphase chemistry model are performed. The investigations aim at assessing the impact of a detailed treatment of non-ideality in multiphase models dealing with aqueous aerosol chemistry. The model studies demonstrate that the inclusion of non-ideality considerably affects the multiphase chemical processing of transition metal ions, oxidants, and related chemical subsystems such as organic chemistry in aqueous aerosols.
Noelia Otero, Henning W. Rust, and Tim Butler
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-691, https://doi.org/10.5194/acp-2020-691, 2020
Revised manuscript not accepted
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Surface ozone concentrations are strongly correlated with temperature in summertime. Using long-term measurements, we investigate changes in the observed relationship between ozone and temperature over Germany. We propose a new statistical approach based on Generalized Additive Models (GAMs) to describe ozone production rates as a function of nitrogen oxides (NOx) and temperature. Our results suggest that NOx reductions alone can not explain the changes in the temperature dependence of ozone.
Danilo Custodio, Ralf Ebinghaus, T. Gerard Spain, and Johannes Bieser
Atmos. Chem. Phys., 20, 7929–7939, https://doi.org/10.5194/acp-20-7929-2020, https://doi.org/10.5194/acp-20-7929-2020, 2020
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Using a stereo algorithm, we reconstructed 99.9 % of the total atmospheric gas mercury and presented a new insight into atmospheric mercury source assessing, which can have great relevance for policy and regulations in light of the Minamata convention.
Shunliu Zhao, Matthew G. Russell, Amir Hakami, Shannon L. Capps, Matthew D. Turner, Daven K. Henze, Peter B. Percell, Jaroslav Resler, Huizhong Shen, Armistead G. Russell, Athanasios Nenes, Amanda J. Pappin, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Charles O. Stanier, and Tianfeng Chai
Geosci. Model Dev., 13, 2925–2944, https://doi.org/10.5194/gmd-13-2925-2020, https://doi.org/10.5194/gmd-13-2925-2020, 2020
Franz Slemr, Lynwill Martin, Casper Labuschagne, Thumeka Mkololo, Hélène Angot, Olivier Magand, Aurélien Dommergue, Philippe Garat, Michel Ramonet, and Johannes Bieser
Atmos. Chem. Phys., 20, 7683–7692, https://doi.org/10.5194/acp-20-7683-2020, https://doi.org/10.5194/acp-20-7683-2020, 2020
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Monitoring of atmospheric mercury (Hg) concentrations is an important part of the effectiveness evaluation of the Minamata Convention on Hg. Hg concentrations in 2012–2017 at Cape Point, South Africa, and at Amsterdam Island in the remote Indian Ocean are comparable, and no trend or a slightly downward trend was observed at both stations. Over the 2007–2017 period an upward trend was observed at CPT which was driven mainly by the 2007–2014 data. The trend and its change are discussed.
Pablo E. Saide, Meng Gao, Zifeng Lu, Daniel L. Goldberg, David G. Streets, Jung-Hun Woo, Andreas Beyersdorf, Chelsea A. Corr, Kenneth L. Thornhill, Bruce Anderson, Johnathan W. Hair, Amin R. Nehrir, Glenn S. Diskin, Jose L. Jimenez, Benjamin A. Nault, Pedro Campuzano-Jost, Jack Dibb, Eric Heim, Kara D. Lamb, Joshua P. Schwarz, Anne E. Perring, Jhoon Kim, Myungje Choi, Brent Holben, Gabriele Pfister, Alma Hodzic, Gregory R. Carmichael, Louisa Emmons, and James H. Crawford
Atmos. Chem. Phys., 20, 6455–6478, https://doi.org/10.5194/acp-20-6455-2020, https://doi.org/10.5194/acp-20-6455-2020, 2020
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Air quality forecasts over the Korean Peninsula captured aerosol optical depth but largely overpredicted surface PM during a Chinese haze transport event. Model deficiency was related to the calculation of optical properties. In order to improve it, aerosol size representation needs to be refined in the calculations, and the representation of aerosol properties, such as size distribution, chemical composition, refractive index, hygroscopicity parameter, and density, needs to be improved.
Erik H. Hoffmann, Roland Schrödner, Andreas Tilgner, Ralf Wolke, and Hartmut Herrmann
Geosci. Model Dev., 13, 2587–2609, https://doi.org/10.5194/gmd-13-2587-2020, https://doi.org/10.5194/gmd-13-2587-2020, 2020
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A condensed multiphase halogen and DMS chemistry mechanism for application in chemical transport models has been developed and applied by 2D simulations to explore multiphase marine chemistry above the pristine open ocean. The model simulations have demonstrated the ability of the mechanism in studying aerosol cloud processing effects in the marine atmosphere. First 2D simulations have shown significant differences in the DMS processing under convective and stratiform cloud conditions.
Sam J. Silva, Colette L. Heald, and Alex B. Guenther
Geosci. Model Dev., 13, 2569–2585, https://doi.org/10.5194/gmd-13-2569-2020, https://doi.org/10.5194/gmd-13-2569-2020, 2020
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Simulating the influence of the biosphere on atmospheric chemistry has traditionally been computationally intensive. We describe a surrogate canopy physics model parameterized using a statistical learning technique and specifically designed for use in large-scale chemical transport models. Our surrogate model reproduces a more detailed model to within 10 % without a large computational demand, improving the process representation of biosphere–atmosphere exchange.
Shelley C. van der Graaf, Richard Kranenburg, Arjo J. Segers, Martijn Schaap, and Jan Willem Erisman
Geosci. Model Dev., 13, 2451–2474, https://doi.org/10.5194/gmd-13-2451-2020, https://doi.org/10.5194/gmd-13-2451-2020, 2020
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Chemical transport models (CTMs) are important tools to determine the fate of reactive nitrogen (Nr) emissions. The parameterization of the surface–atmosphere exchange in CTMs is often only linked to fixed, land-use-dependent values. In this paper, we present an approach to derive more realistic, dynamic leaf area index (LAI) and roughness length (z0) input maps using multiple satellite products. We evaluate the effect on Nr concentration and deposition fields modelled in the LOTOS-EUROS CTM.
Camille Mouchel-Vallon, Julia Lee-Taylor, Alma Hodzic, Paulo Artaxo, Bernard Aumont, Marie Camredon, David Gurarie, Jose-Luis Jimenez, Donald H. Lenschow, Scot T. Martin, Janaina Nascimento, John J. Orlando, Brett B. Palm, John E. Shilling, Manish Shrivastava, and Sasha Madronich
Atmos. Chem. Phys., 20, 5995–6014, https://doi.org/10.5194/acp-20-5995-2020, https://doi.org/10.5194/acp-20-5995-2020, 2020
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The GoAmazon 2014/5 field campaign took place near the city of Manaus, Brazil, isolated in the Amazon rainforest, to study the impacts of urban pollution on natural air masses. We simulated this campaign with an extremely detailed organic chemistry model to understand how the city would affect the growth and composition of natural aerosol particles. Discrepancies between the model and the measurements indicate that the chemistry of naturally emitted organic compounds is still poorly understood.
Alma Hodzic, Pedro Campuzano-Jost, Huisheng Bian, Mian Chin, Peter R. Colarco, Douglas A. Day, Karl D. Froyd, Bernd Heinold, Duseong S. Jo, Joseph M. Katich, John K. Kodros, Benjamin A. Nault, Jeffrey R. Pierce, Eric Ray, Jacob Schacht, Gregory P. Schill, Jason C. Schroder, Joshua P. Schwarz, Donna T. Sueper, Ina Tegen, Simone Tilmes, Kostas Tsigaridis, Pengfei Yu, and Jose L. Jimenez
Atmos. Chem. Phys., 20, 4607–4635, https://doi.org/10.5194/acp-20-4607-2020, https://doi.org/10.5194/acp-20-4607-2020, 2020
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Organic aerosol (OA) is a key source of uncertainty in aerosol climate effects. We present the first pole-to-pole OA characterization during the NASA Atmospheric Tomography aircraft mission. OA has a strong seasonal and zonal variability, with the highest levels in summer and over fire-influenced regions and the lowest ones in the southern high latitudes. We show that global models predict the OA distribution well but not the relative contribution of OA emissions vs. chemical production.
Matthieu Pommier, Hilde Fagerli, Michael Schulz, Alvaro Valdebenito, Richard Kranenburg, and Martijn Schaap
Geosci. Model Dev., 13, 1787–1807, https://doi.org/10.5194/gmd-13-1787-2020, https://doi.org/10.5194/gmd-13-1787-2020, 2020
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The EMEP and LOTOS-EUROS models comprise the operational source contribution prediction system for the European cities within the Copernicus Atmosphere Monitoring Service (CAMS). This study presents a first evaluation of this system, with hourly resolution, by focusing on one PM10 episode in December 2016, dominated by the influence of domestic emissions. It shows that the system provides valuable information on the composition and contributions of different countries to PM10.
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.
Debora Griffin, Christopher Sioris, Jack Chen, Nolan Dickson, Andrew Kovachik, Martin de Graaf, Swadhin Nanda, Pepijn Veefkind, Enrico Dammers, Chris A. McLinden, Paul Makar, and Ayodeji Akingunola
Atmos. Meas. Tech., 13, 1427–1445, https://doi.org/10.5194/amt-13-1427-2020, https://doi.org/10.5194/amt-13-1427-2020, 2020
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This study looks into validating the aerosol layer height product from the recently launched TROPOspheric Monitoring Instrument (TROPOMI) for forest fire plume through comparisons with two other satellite products, and interpreting differences due to the individual measurement techniques. These satellite observations are compared to predicted plume heights from Environment and Climate Change's air quality forecast model.
Syuichi Itahashi, Rohit Mathur, Christian Hogrefe, and Yang Zhang
Atmos. Chem. Phys., 20, 3373–3396, https://doi.org/10.5194/acp-20-3373-2020, https://doi.org/10.5194/acp-20-3373-2020, 2020
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The state-of-the-science Community Multiscale Air Quality model extended for hemispheric applications (H-CMAQ) is used to model the trans-Pacific transport which has been recognized as a potential source of air pollutants over the US. In Part 1, modeled ozone is evaluated with observations at surface, by ozonesonde and airplane, and by satellite across the Northern Hemisphere. In addition, a newly developed air mass characterization method to estimate stratospheric intrusion is presented.
Syuichi Itahashi, Rohit Mathur, Christian Hogrefe, Sergey L. Napelenok, and Yang Zhang
Atmos. Chem. Phys., 20, 3397–3413, https://doi.org/10.5194/acp-20-3397-2020, https://doi.org/10.5194/acp-20-3397-2020, 2020
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The state-of-the-science Community Multiscale Air Quality model extended for hemispheric applications (H-CMAQ) is used to model the trans-Pacific transport which has been recognized as a potential source of air pollutants over the US. In Part 2, the higher-order decoupled direct method (HDDM) is applied to investigate the emission impacts from east Asia and the US during April 2010. Furthermore, changes in trans-Pacific transport caused by the recent emissions are examined.
Cynthia H. Whaley, Elisabeth Galarneau, Paul A. Makar, Michael D. Moran, and Junhua Zhang
Atmos. Chem. Phys., 20, 2911–2925, https://doi.org/10.5194/acp-20-2911-2020, https://doi.org/10.5194/acp-20-2911-2020, 2020
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Benzene and polycyclic aromatic compounds are toxic air pollutants and ubiquitous in the environment. Using a chemical transport model, we have determined the net impact of vehicle emissions on ambient concentrations of these species. Traffic emissions were found to be a significant fraction of ambient pollution in the densely populated modelled region of North America. Our simulations demonstrate the air quality benefits that would result from transitioning to a zero-emission vehicle fleet.
S. Trivikrama Rao, Huiying Luo, Marina Astitha, Christian Hogrefe, Valerie Garcia, and Rohit Mathur
Atmos. Chem. Phys., 20, 1627–1639, https://doi.org/10.5194/acp-20-1627-2020, https://doi.org/10.5194/acp-20-1627-2020, 2020
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Since numerical air quality models do not explicitly simulate stochastic variations in the atmosphere, there will always be differences between modeled and measured pollutant levels even when the model's physics, chemistry, numerical analysis, and its input data are perfect. This paper quantifies the inherent uncertainty in regional models due to the stochastic nature of the atmosphere. A knowledge of the expected error helps model developers in evaluating the real progress in improving models.
Ying Chen, Yafang Cheng, Nan Ma, Chao Wei, Liang Ran, Ralf Wolke, Johannes Größ, Qiaoqiao Wang, Andrea Pozzer, Hugo A. C. Denier van der Gon, Gerald Spindler, Jos Lelieveld, Ina Tegen, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 20, 771–786, https://doi.org/10.5194/acp-20-771-2020, https://doi.org/10.5194/acp-20-771-2020, 2020
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Particulate nitrate is one of the most important climate cooling agents. Our results show that interaction with sea-salt aerosol can shift nitrate to larger sized particles (redistribution effect), weakening its direct cooling effect. The modelling results indicate strong redistribution over coastal and offshore regions worldwide as well as continental Europe. Improving the consideration of the redistribution effect in global models fosters a better understanding of climate change.
Aurelia Lupaşcu and Tim Butler
Atmos. Chem. Phys., 19, 14535–14558, https://doi.org/10.5194/acp-19-14535-2019, https://doi.org/10.5194/acp-19-14535-2019, 2019
Giancarlo Ciarelli, Mark R. Theobald, Marta G. Vivanco, Matthias Beekmann, Wenche Aas, Camilla Andersson, Robert Bergström, Astrid Manders-Groot, Florian Couvidat, Mihaela Mircea, Svetlana Tsyro, Hilde Fagerli, Kathleen Mar, Valentin Raffort, Yelva Roustan, Maria-Teresa Pay, Martijn Schaap, Richard Kranenburg, Mario Adani, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, Cornelis Cuvelier, Arineh Cholakian, Bertrand Bessagnet, Peter Wind, and Augustin Colette
Geosci. Model Dev., 12, 4923–4954, https://doi.org/10.5194/gmd-12-4923-2019, https://doi.org/10.5194/gmd-12-4923-2019, 2019
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The novel multi-model EURODELTA-Trends exercise provided 21 years of continuous PM components and their gas-phase precursor concentrations over Europe from the year 1990. The models’ capabilities to reproduce PM components and gas-phase PM precursor trends over the 1990–2010 period is the key focus of this study. The models were able to reproduce the observed trends relatively well, indicating a possible shift in the thermodynamic equilibrium between gas and particle phases.
Anthony Y. H. Wong, Jeffrey A. Geddes, Amos P. K. Tai, and Sam J. Silva
Atmos. Chem. Phys., 19, 14365–14385, https://doi.org/10.5194/acp-19-14365-2019, https://doi.org/10.5194/acp-19-14365-2019, 2019
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Dry deposition is an important, but highly uncertain, sink for surface ozone. Several popular parameterizations exist to model this process, which vary with respect to how they depend on land cover and environmental variables. Here, we predict ozone dry deposition globally over 30 years, comparing four different approaches. We find that the choice of dry deposition parameterization affects the distribution, seasonal means, long-term trends, and interannual variability of surface ozone.
Miguel Escudero, Arjo Segers, Richard Kranenburg, Xavier Querol, Andrés Alastuey, Rafael Borge, David de la Paz, Gotzon Gangoiti, and Martijn Schaap
Atmos. Chem. Phys., 19, 14211–14232, https://doi.org/10.5194/acp-19-14211-2019, https://doi.org/10.5194/acp-19-14211-2019, 2019
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In this work we optimise LOTOS-EUROS CTM for simulating tropospheric O3 during summer in the Madrid metropolitan area, one of the largest conurbations in the Mediterranean. Comparing the outputs from five set-ups with different combinations of spatial resolution, meteorological data and vertical structure, we conclude that the model benefits from fine horizontal resolution and highly resolved vertical structure. Running optimized configuration run, we interpret O3 variability during July 2016.
Peter Bräuer, Camille Mouchel-Vallon, Andreas Tilgner, Anke Mutzel, Olaf Böge, Maria Rodigast, Laurent Poulain, Dominik van Pinxteren, Ralf Wolke, Bernard Aumont, and Hartmut Herrmann
Atmos. Chem. Phys., 19, 9209–9239, https://doi.org/10.5194/acp-19-9209-2019, https://doi.org/10.5194/acp-19-9209-2019, 2019
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The article presents a new protocol for computer-assisted automated aqueous-phase chemistry mechanism generation, which has been validated against chamber experiments. Together with a large kinetics database and improved prediction methods for kinetic data, the novel protocol provides an unmatched tool for detailed studies of tropospheric aqueous-phase chemistry in complex model studies and for the design and analysis of chamber experiments.
Martin Otto Paul Ramacher, Matthias Karl, Johannes Bieser, Jukka-Pekka Jalkanen, and Lasse Johansson
Atmos. Chem. Phys., 19, 9153–9179, https://doi.org/10.5194/acp-19-9153-2019, https://doi.org/10.5194/acp-19-9153-2019, 2019
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We simulated the impact of NOx shipping emissions on air quality and exposure in the Baltic Sea harbour cities Rostock (Germany), Riga (Latvia) and Gdańsk–Gdynia (Poland) for 2012. We found that local shipping affects total NO2, with contributions of 22 %, 11 % and 16 % in Rostock, Riga and Gdańsk–Gdynia. Exposure to NO2 from all emission sources was highest at home addresses (54 %–59 %). Emissions from shipping have a high impact on NO2 exposure in the port area (50 %–80 %).
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Eloise A. Marais, Zhe Peng, Benjamin A. Nault, Weiwei Hu, Pedro Campuzano-Jost, and Jose L. Jimenez
Geosci. Model Dev., 12, 2983–3000, https://doi.org/10.5194/gmd-12-2983-2019, https://doi.org/10.5194/gmd-12-2983-2019, 2019
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We developed a parameterization method for IEPOX-SOA based on the detailed chemical mechanism. Our parameterizations were tested using a box model and 3-D chemical transport model, which accurately captured the spatiotemporal distribution and response to changes in emissions compared to the explicit full chemistry, while being more computationally efficient. The method developed in this study can be applied to global climate models for long-term studies with a lower computational cost.
Matthew Russell, Amir Hakami, Paul A. Makar, Ayodeji Akingunola, Junhua Zhang, Michael D. Moran, and Qiong Zheng
Atmos. Chem. Phys., 19, 4393–4417, https://doi.org/10.5194/acp-19-4393-2019, https://doi.org/10.5194/acp-19-4393-2019, 2019
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High-resolution air-quality forecast modeling results are compared for two different grid spacings for the Environment and Climate Change Canada GEM-MACH model. While the higher-resolution simulations have worse formal error scores, we show that the higher-resolution model nevertheless has the ability to better resolve plume maxima and has better performance when the evaluation occurs using new scoring metrics which operate on an equal-representative-area basis.
Anna Katinka Petersen, Guy P. Brasseur, Idir Bouarar, Johannes Flemming, Michael Gauss, Fei Jiang, Rostislav Kouznetsov, Richard Kranenburg, Bas Mijling, Vincent-Henri Peuch, Matthieu Pommier, Arjo Segers, Mikhail Sofiev, Renske Timmermans, Ronald van der A, Stacy Walters, Ying Xie, Jianming Xu, and Guangqiang Zhou
Geosci. Model Dev., 12, 1241–1266, https://doi.org/10.5194/gmd-12-1241-2019, https://doi.org/10.5194/gmd-12-1241-2019, 2019
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An operational multi-model forecasting system for air quality is providing daily forecasts of ozone, nitrogen oxides, and particulate matter for 37 urban areas of China. The paper presents the evaluation of the different forecasts performed during the first year of operation.
Laura Palacios-Peña, Pedro Jiménez-Guerrero, Rocío Baró, Alessandra Balzarini, Roberto Bianconi, Gabriele Curci, Tony Christian Landi, Guido Pirovano, Marje Prank, Angelo Riccio, Paolo Tuccella, and Stefano Galmarini
Atmos. Chem. Phys., 19, 2965–2990, https://doi.org/10.5194/acp-19-2965-2019, https://doi.org/10.5194/acp-19-2965-2019, 2019
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The main uncertainties regarding the estimation of changes in the Earth’s energy budget are related to the role of atmospheric aerosols. Our study evaluates the representation of aerosol optical properties by different atmospheric chemistry models against remote-sensing observations in order to reduce this uncertainty. Results show that the representation of aerosol optical properties is strongly dependent on the used model.
Cristen Adams, Chris A. McLinden, Mark W. Shephard, Nolan Dickson, Enrico Dammers, Jack Chen, Paul Makar, Karen E. Cady-Pereira, Naomi Tam, Shailesh K. Kharol, Lok N. Lamsal, and Nickolay A. Krotkov
Atmos. Chem. Phys., 19, 2577–2599, https://doi.org/10.5194/acp-19-2577-2019, https://doi.org/10.5194/acp-19-2577-2019, 2019
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We estimated how much carbon monoxide, ammonia, and nitrogen oxides were emitted in the smoke from the Fort McMurray Horse River wildfire using satellite data and air quality models. The fire emitted amounts of carbon monoxide that were similar to anthropogenic (human-caused) emissions for all of Alberta over a full year. We also estimated large amounts of ammonia and nitrogen oxides emitted from the fire. These results can be used to evaluate the performance of air quality forecasting models.
Quazi Z. Rasool, Jesse O. Bash, and Daniel S. Cohan
Geosci. Model Dev., 12, 849–878, https://doi.org/10.5194/gmd-12-849-2019, https://doi.org/10.5194/gmd-12-849-2019, 2019
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Soils have been overlooked as a source of reactive nitrogen (N) emissions that are pronounced in the summer ozone season (growing season) and increasingly important as fertilizer use grows, while fossil fuel combustion sources of N decline. Mechanistic process models of soil N emissions are used in Earth science and soil biogeochemical modeling on a site scale. This work mechanistically models soil N emissions for the first time on a regional scale to better understand their air quality impacts.
Matthias Karl, Johannes Bieser, Beate Geyer, Volker Matthias, Jukka-Pekka Jalkanen, Lasse Johansson, and Erik Fridell
Atmos. Chem. Phys., 19, 1721–1752, https://doi.org/10.5194/acp-19-1721-2019, https://doi.org/10.5194/acp-19-1721-2019, 2019
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Air emissions of nitrogen oxides from ship traffic in the Baltic Sea are a health concern in coastal areas of the Baltic Sea region. We find that the introduction of the nitrogen emission control area (NECA) is critical for reducing ship emissions of nitrogen oxides to levels that are low enough to sustainably dampen ozone production. The decline of the ship-related nitrogen deposition to the Baltic Sea between 2012 and 2040 varies between 46 % and 78 % in different regulation scenarios.
Gabriele Curci, Ummugulsum Alyuz, Rocio Barò, Roberto Bianconi, Johannes Bieser, Jesper H. Christensen, Augustin Colette, Aidan Farrow, Xavier Francis, Pedro Jiménez-Guerrero, Ulas Im, Peng Liu, Astrid Manders, Laura Palacios-Peña, Marje Prank, Luca Pozzoli, Ranjeet Sokhi, Efisio Solazzo, Paolo Tuccella, Alper Unal, Marta G. Vivanco, Christian Hogrefe, and Stefano Galmarini
Atmos. Chem. Phys., 19, 181–204, https://doi.org/10.5194/acp-19-181-2019, https://doi.org/10.5194/acp-19-181-2019, 2019
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Atmospheric carbonaceous aerosols are able to absorb solar radiation and they continue to contribute some of the largest uncertainties in projected climate change. One important detail is how the chemical species are arranged inside each particle, i.e. the knowledge of their mixing state. We use an ensemble of regional model simulations to test different mixing state assumptions and found that a combination of internal and external mixing may better reproduce sunphotometer observations.
Guy P. Brasseur, Ying Xie, Anna Katinka Petersen, Idir Bouarar, Johannes Flemming, Michael Gauss, Fei Jiang, Rostislav Kouznetsov, Richard Kranenburg, Bas Mijling, Vincent-Henri Peuch, Matthieu Pommier, Arjo Segers, Mikhail Sofiev, Renske Timmermans, Ronald van der A, Stacy Walters, Jianming Xu, and Guangqiang Zhou
Geosci. Model Dev., 12, 33–67, https://doi.org/10.5194/gmd-12-33-2019, https://doi.org/10.5194/gmd-12-33-2019, 2019
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An operational multi-model forecasting system for air quality provides daily forecasts of ozone, nitrogen oxides, and particulate matter for 37 urban areas in China. The paper presents an intercomparison of the different forecasts performed during a specific period of time and highlights recurrent differences between the model output. Pathways to improve the forecasts by the multi-model system are suggested.
Peng Liu, Christian Hogrefe, Ulas Im, Jesper H. Christensen, Johannes Bieser, Uarporn Nopmongcol, Greg Yarwood, Rohit Mathur, Shawn Roselle, and Tanya Spero
Atmos. Chem. Phys., 18, 17157–17175, https://doi.org/10.5194/acp-18-17157-2018, https://doi.org/10.5194/acp-18-17157-2018, 2018
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This study represents an intercomparison of four regional-scale air quality simulations in order to understand the model similarities and differences in estimating the impact of ozone imported from outside of the US on the surface ozone within the US at process level. Vertical turbulent mixing stands out as a primary contributor to the model differences in inert tracers.
Arlene M. Fiore, Emily V. Fischer, George P. Milly, Shubha Pandey Deolal, Oliver Wild, Daniel A. Jaffe, Johannes Staehelin, Olivia E. Clifton, Dan Bergmann, William Collins, Frank Dentener, Ruth M. Doherty, Bryan N. Duncan, Bernd Fischer, Stefan Gilge, Peter G. Hess, Larry W. Horowitz, Alexandru Lupu, Ian A. MacKenzie, Rokjin Park, Ludwig Ries, Michael G. Sanderson, Martin G. Schultz, Drew T. Shindell, Martin Steinbacher, David S. Stevenson, Sophie Szopa, Christoph Zellweger, and Guang Zeng
Atmos. Chem. Phys., 18, 15345–15361, https://doi.org/10.5194/acp-18-15345-2018, https://doi.org/10.5194/acp-18-15345-2018, 2018
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We demonstrate a proof-of-concept approach for applying northern midlatitude mountaintop peroxy acetyl nitrate (PAN) measurements and a multi-model ensemble during April to constrain the influence of continental-scale anthropogenic precursor emissions on PAN. Our findings imply a role for carefully coordinated multi-model ensembles in helping identify observations for discriminating among widely varying (and poorly constrained) model responses of atmospheric constituents to changes in emissions.
Rocío Baró, Pedro Jiménez-Guerrero, Martin Stengel, Dominik Brunner, Gabriele Curci, Renate Forkel, Lucy Neal, Laura Palacios-Peña, Nicholas Savage, Martijn Schaap, Paolo Tuccella, Hugo Denier van der Gon, and Stefano Galmarini
Atmos. Chem. Phys., 18, 15183–15199, https://doi.org/10.5194/acp-18-15183-2018, https://doi.org/10.5194/acp-18-15183-2018, 2018
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Particles in the atmosphere, such as pollution, desert dust, and volcanic ash, have an impact on meteorology. They interact with incoming radiation resulting in a cooling effect of the atmosphere. Today, the use of meteorology and chemistry models help us to understand these processes, but there are a lot of uncertainties. The goal of this work is to evaluate how these interactions are represented in the models by comparing them to satellite data to see how close they are to reality.
Yuqiang Zhang, J. Jason West, Rohit Mathur, Jia Xing, Christian Hogrefe, Shawn J. Roselle, Jesse O. Bash, Jonathan E. Pleim, Chuen-Meei Gan, and David C. Wong
Atmos. Chem. Phys., 18, 15003–15016, https://doi.org/10.5194/acp-18-15003-2018, https://doi.org/10.5194/acp-18-15003-2018, 2018
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Here we use a fine-resolution (36 km) self-consistent 21-year air quality simulation from 1990 to 2010, a health impact function, and annual county-level population and baseline mortality rate estimates to estimate annual mortality burdens from PM2.5 and O3 in the US, and also the contributions to the trends. We found that the PM2.5-related mortality burden has steadily decreased by 53 %, while the O3-related mortality burden has increased by 13 %, with larger inter-annual variabilities.
Mark Gordon, Paul A. Makar, Ralf M. Staebler, Junhua Zhang, Ayodeji Akingunola, Wanmin Gong, and Shao-Meng Li
Atmos. Chem. Phys., 18, 14695–14714, https://doi.org/10.5194/acp-18-14695-2018, https://doi.org/10.5194/acp-18-14695-2018, 2018
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This work uses aircraft-based measurements of smokestack plumes carried out in northern Alberta in 2013. These measurements are used to test equations used to predict how high in the air smokestack plumes rise. It is important to predict plume rise height accurately as it tells us how far downwind pollutants are carried and what air quality can be expected at the surface. We found that the equations that are typically used significantly underestimate the plume rise at this location.
Marina Astitha, Ioannis Kioutsioukis, Ghezae Araya Fisseha, Roberto Bianconi, Johannes Bieser, Jesper H. Christensen, Owen R. Cooper, Stefano Galmarini, Christian Hogrefe, Ulas Im, Bryan Johnson, Peng Liu, Uarporn Nopmongcol, Irina Petropavlovskikh, Efisio Solazzo, David W. Tarasick, and Greg Yarwood
Atmos. Chem. Phys., 18, 13925–13945, https://doi.org/10.5194/acp-18-13925-2018, https://doi.org/10.5194/acp-18-13925-2018, 2018
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This work is unique in the detailed analyses of modeled ozone vertical profiles from sites in North America through the collaboration of four research groups from the US and EU. We assess the air quality models' performance and model inter-comparison for ozone vertical profiles and stratospheric ozone intrusions. Lastly, we designate the important role of lateral boundary conditions in the ozone vertical profiles using chemically inert tracers.
Craig A. Stroud, Paul A. Makar, Junhua Zhang, Michael D. Moran, Ayodeji Akingunola, Shao-Meng Li, Amy Leithead, Katherine Hayden, and May Siu
Atmos. Chem. Phys., 18, 13531–13545, https://doi.org/10.5194/acp-18-13531-2018, https://doi.org/10.5194/acp-18-13531-2018, 2018
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It is shown that using measurement-derived volatile organic compound (VOC) and organic aerosol (OA) emissions in the GEM-MACH air quality model provides better overall predictions compared to using bottom-up emission inventories. This work was done to better constrain the fugitive organic emissions from the Athabasca oil sands region, which are a challenge to estimate with bottom-up emission approaches. We use observations from the 2013 Joint Oil Sands Monitoring study.
Victor Lannuque, Marie Camredon, Florian Couvidat, Alma Hodzic, Richard Valorso, Sasha Madronich, Bertrand Bessagnet, and Bernard Aumont
Atmos. Chem. Phys., 18, 13411–13428, https://doi.org/10.5194/acp-18-13411-2018, https://doi.org/10.5194/acp-18-13411-2018, 2018
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Large uncertainties remain in understanding the influence of atmospheric environmental conditions on secondary organic aerosol (SOA) formation, evolution and properties. In this article, the GECKO-A modelling tool has been used in a box model under various environmental conditions to (i) explore the sensitivity of SOA formation and properties to changes on physical and chemical conditions and (ii) develop a volatility-basis-set-type parameterization for air quality models.
Jason A. Ducker, Christopher D. Holmes, Trevor F. Keenan, Silvano Fares, Allen H. Goldstein, Ivan Mammarella, J. William Munger, and Jordan Schnell
Biogeosciences, 15, 5395–5413, https://doi.org/10.5194/bg-15-5395-2018, https://doi.org/10.5194/bg-15-5395-2018, 2018
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We have developed an accurate method (SynFlux) to estimate ozone deposition and stomatal uptake across 103 flux tower sites (43 US, 60 Europe), where ozone concentrations and fluxes have not been measured. In all, the SynFlux public dataset provides monthly values of ozone dry deposition for 926 site years across a wide array of ecosystems. The SynFlux dataset will promote further applications to ecosystem, air quality, or climate modeling across the geoscience community.
Franz Slemr, Andreas Weigelt, Ralf Ebinghaus, Johannes Bieser, Carl A. M. Brenninkmeijer, Armin Rauthe-Schöch, Markus Hermann, Bengt G. Martinsson, Peter van Velthoven, Harald Bönisch, Marco Neumaier, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 18, 12329–12343, https://doi.org/10.5194/acp-18-12329-2018, https://doi.org/10.5194/acp-18-12329-2018, 2018
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Total and elemental mercury were measured in the upper troposphere and lower stratosphere onboard a passenger aircraft. Their concentrations in the upper troposphere were comparable implying low concentrations of oxidized mercury in this region. Large scale seasonally dependent influence of emissions from biomass burning was also observed. Their distributions in the lower stratosphere implies a long stratospheric lifetime, which precludes significant mercury oxidation by ozone.
Noelia Otero, Jana Sillmann, Kathleen A. Mar, Henning W. Rust, Sverre Solberg, Camilla Andersson, Magnuz Engardt, Robert Bergström, Bertrand Bessagnet, Augustin Colette, Florian Couvidat, Cournelius Cuvelier, Svetlana Tsyro, Hilde Fagerli, Martijn Schaap, Astrid Manders, Mihaela Mircea, Gino Briganti, Andrea Cappelletti, Mario Adani, Massimo D'Isidoro, María-Teresa Pay, Mark Theobald, Marta G. Vivanco, Peter Wind, Narendra Ojha, Valentin Raffort, and Tim Butler
Atmos. Chem. Phys., 18, 12269–12288, https://doi.org/10.5194/acp-18-12269-2018, https://doi.org/10.5194/acp-18-12269-2018, 2018
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This paper evaluates the capability of air-quality models to capture the observed relationship between surface ozone concentrations and meteorology over Europe. The air-quality models tended to overestimate the influence of maximum temperature and surface solar radiation. None of the air-quality models captured the strength of the observed relationship between ozone and relative humidity appropriately, underestimating the effect of relative humidity, a key factor in the ozone removal processes.
Piyush Bhardwaj, Manish Naja, Maheswar Rupakheti, Aurelia Lupascu, Andrea Mues, Arnico Kumar Panday, Rajesh Kumar, Khadak Singh Mahata, Shyam Lal, Harish C. Chandola, and Mark G. Lawrence
Atmos. Chem. Phys., 18, 11949–11971, https://doi.org/10.5194/acp-18-11949-2018, https://doi.org/10.5194/acp-18-11949-2018, 2018
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This study provides information about the regional variabilities in some of the pollutants using observations in Nepal and India. It is shown that agricultural crop residue burning leads to a significant enhancement in ozone and CO over a wider region. Further, the wintertime higher ozone levels are shown to be largely due to local emissions, while regional transport could be important in spring and hence shows the role of regional sources versus local sources in the Kathmandu Valley.
Junhua Zhang, Michael D. Moran, Qiong Zheng, Paul A. Makar, Pegah Baratzadeh, George Marson, Peter Liu, and Shao-Meng Li
Atmos. Chem. Phys., 18, 10459–10481, https://doi.org/10.5194/acp-18-10459-2018, https://doi.org/10.5194/acp-18-10459-2018, 2018
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This paper discusses the development of new synthesized emissions inventories and the generation of air quality model-ready emissions files for the Athabasca Oil Sands Region of Alberta, Canada, using multiple emissions inventories, continuous emissions monitoring data, and inferred emission rates based on aircraft measurements. Novel facility-specific gridded spatial surrogate fields were generated to allocate emissions spatially within each huge mining facility.
Marta G. Vivanco, Mark R. Theobald, Héctor García-Gómez, Juan Luis Garrido, Marje Prank, Wenche Aas, Mario Adani, Ummugulsum Alyuz, Camilla Andersson, Roberto Bellasio, Bertrand Bessagnet, Roberto Bianconi, Johannes Bieser, Jørgen Brandt, Gino Briganti, Andrea Cappelletti, Gabriele Curci, Jesper H. Christensen, Augustin Colette, Florian Couvidat, Cornelis Cuvelier, Massimo D'Isidoro, Johannes Flemming, Andrea Fraser, Camilla Geels, Kaj M. Hansen, Christian Hogrefe, Ulas Im, Oriol Jorba, Nutthida Kitwiroon, Astrid Manders, Mihaela Mircea, Noelia Otero, Maria-Teresa Pay, Luca Pozzoli, Efisio Solazzo, Svetlana Tsyro, Alper Unal, Peter Wind, and Stefano Galmarini
Atmos. Chem. Phys., 18, 10199–10218, https://doi.org/10.5194/acp-18-10199-2018, https://doi.org/10.5194/acp-18-10199-2018, 2018
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European wet and dry atmospheric deposition of N and S estimated by 14 air quality models was found to vary substantially. An ensemble of models meeting acceptability criteria was used to estimate the exceedances of the critical loads for N in habitats within the Natura 2000 network, as well as their lower and upper limits. Scenarios with 20 % emission reductions in different regions of the world showed that European emissions are responsible for most of the N and S deposition in Europe.
Paul A. Makar, Ayodeji Akingunola, Julian Aherne, Amanda S. Cole, Yayne-abeba Aklilu, Junhua Zhang, Isaac Wong, Katherine Hayden, Shao-Meng Li, Jane Kirk, Ken Scott, Michael D. Moran, Alain Robichaud, Hazel Cathcart, Pegah Baratzedah, Balbir Pabla, Philip Cheung, Qiong Zheng, and Dean S. Jeffries
Atmos. Chem. Phys., 18, 9897–9927, https://doi.org/10.5194/acp-18-9897-2018, https://doi.org/10.5194/acp-18-9897-2018, 2018
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Complex computer model output was compared to and fused with observation data, to estimate potential damage due to acidifying precipitation for ecosystems in the Canadian provinces of Alberta and Saskatchewan. Estimated deposition was compared to the maximum no-damage ecosystem capacity for sulfur and/or nitrogen uptake; these critical loads were exceeded, for areas between 10 000 and 330 000 square kilometres, depending on ecosystem type: ecosystem damage will occur at 2013 emission levels.
Tim Butler, Aurelia Lupascu, Jane Coates, and Shuai Zhu
Geosci. Model Dev., 11, 2825–2840, https://doi.org/10.5194/gmd-11-2825-2018, https://doi.org/10.5194/gmd-11-2825-2018, 2018
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This paper describes a method for determining origin of tropospheric ozone simulated in a global chemistry–climate model. This technique can show which precursor compounds were responsible for simulated ozone, and where they were emitted. In this paper we describe our technique, compare and contrast it with several other similar techniques, and use it to calculate the contribution of several different NOx and VOC precursor categories to the tropospheric ozone burden.
Cynthia H. Whaley, Elisabeth Galarneau, Paul A. Makar, Ayodeji Akingunola, Wanmin Gong, Sylvie Gravel, Michael D. Moran, Craig Stroud, Junhua Zhang, and Qiong Zheng
Geosci. Model Dev., 11, 2609–2632, https://doi.org/10.5194/gmd-11-2609-2018, https://doi.org/10.5194/gmd-11-2609-2018, 2018
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We present a new, high-resolution, North American model of PAHs and benzene, which are toxic air pollutants that cause a variety of negative health impacts. Our simulation in a densely populated region of Canada and the U.S. shows that the model is improved over a previous model. The new model is particularly refined regarding the gas–particle partitioning of these pollutants, which has impacts on deposition and inhalation. The simulation was sensitive to the selection of vehicle emissions.
Ulas Im, Jesper Heile Christensen, Camilla Geels, Kaj Mantzius Hansen, Jørgen Brandt, Efisio Solazzo, Ummugulsum Alyuz, Alessandra Balzarini, Rocio Baro, Roberto Bellasio, Roberto Bianconi, Johannes Bieser, Augustin Colette, Gabriele Curci, Aidan Farrow, Johannes Flemming, Andrea Fraser, Pedro Jimenez-Guerrero, Nutthida Kitwiroon, Peng Liu, Uarporn Nopmongcol, Laura Palacios-Peña, Guido Pirovano, Luca Pozzoli, Marje Prank, Rebecca Rose, Ranjeet Sokhi, Paolo Tuccella, Alper Unal, Marta G. Vivanco, Greg Yarwood, Christian Hogrefe, and Stefano Galmarini
Atmos. Chem. Phys., 18, 8929–8952, https://doi.org/10.5194/acp-18-8929-2018, https://doi.org/10.5194/acp-18-8929-2018, 2018
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We evaluate the impact of global and regional anthropogenic emission reductions on major air pollutant levels over Europe and North America, using a multi-model ensemble of regional chemistry and transport models. Results show that ozone levels are largely driven by long-range transport over both continents while other pollutants such as carbon monoxide or aerosols are mainly controlled by domestic sources. Use of multi-model ensembles can help to reduce the uncertainties in individual models.
Yuqiang Zhang, Rohit Mathur, Jesse O. Bash, Christian Hogrefe, Jia Xing, and Shawn J. Roselle
Atmos. Chem. Phys., 18, 9091–9106, https://doi.org/10.5194/acp-18-9091-2018, https://doi.org/10.5194/acp-18-9091-2018, 2018
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For this study, we evaluated the WRF–CMAQ coupled model's ability to simulate the long-term trends of wet deposition of nitrogen and sulfur from 1990 to 2010 by comparing the model results with long-term observation datasets in the US. The model generally underestimates the wet deposition of both nitrogen and sulfur but captured well the decreasing trends for the deposition. Then we estimated the deposition budget in the US, including wet deposition and dry deposition from model simulations.
Stefano Galmarini, Ioannis Kioutsioukis, Efisio Solazzo, Ummugulsum Alyuz, Alessandra Balzarini, Roberto Bellasio, Anna M. K. Benedictow, Roberto Bianconi, Johannes Bieser, Joergen Brandt, Jesper H. Christensen, Augustin Colette, Gabriele Curci, Yanko Davila, Xinyi Dong, Johannes Flemming, Xavier Francis, Andrea Fraser, Joshua Fu, Daven K. Henze, Christian Hogrefe, Ulas Im, Marta Garcia Vivanco, Pedro Jiménez-Guerrero, Jan Eiof Jonson, Nutthida Kitwiroon, Astrid Manders, Rohit Mathur, Laura Palacios-Peña, Guido Pirovano, Luca Pozzoli, Marie Prank, Martin Schultz, Rajeet S. Sokhi, Kengo Sudo, Paolo Tuccella, Toshihiko Takemura, Takashi Sekiya, and Alper Unal
Atmos. Chem. Phys., 18, 8727–8744, https://doi.org/10.5194/acp-18-8727-2018, https://doi.org/10.5194/acp-18-8727-2018, 2018
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An ensemble of model results relating to ozone concentrations in Europe in 2010 has been produced and studied. The novelty consists in the fact that the ensemble is made of results of models working at two different scales (regional and global), therefore contributing in detail two different parts of the atmospheric spectrum. The ensemble defined as a hybrid has been studied in detail and shown to bring additional value to the assessment of air quality.
Erika von Schneidemesser, Boris Bonn, Tim M. Butler, Christian Ehlers, Holger Gerwig, Hannele Hakola, Heidi Hellén, Andreas Kerschbaumer, Dieter Klemp, Claudia Kofahl, Jürgen Kura, Anja Lüdecke, Rainer Nothard, Axel Pietsch, Jörn Quedenau, Klaus Schäfer, James J. Schauer, Ashish Singh, Ana-Maria Villalobos, Matthias Wiegner, and Mark G. Lawrence
Atmos. Chem. Phys., 18, 8621–8645, https://doi.org/10.5194/acp-18-8621-2018, https://doi.org/10.5194/acp-18-8621-2018, 2018
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This paper provides an overview of the measurements done at an urban background site in Berlin from June-August of 2014. Results show that natural source contributions to ozone and particulate matter (PM) air pollutants are substantial. Large contributions of secondary aerosols formed in the atmosphere to PM10 concentrations were quantified. An analysis of the sources also identified contributions to PM from plant-based sources, vehicles, and a small contribution from wood burning.
Ayodeji Akingunola, Paul A. Makar, Junhua Zhang, Andrea Darlington, Shao-Meng Li, Mark Gordon, Michael D. Moran, and Qiong Zheng
Atmos. Chem. Phys., 18, 8667–8688, https://doi.org/10.5194/acp-18-8667-2018, https://doi.org/10.5194/acp-18-8667-2018, 2018
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We examine the manner in which air-quality models simulate lofting of buoyant plumes of emissions from stacks (plume rise) and the impact of the level of detail in algorithms simulating particles' variation in size (particle size distribution). The most commonly used plume rise algorithm underestimates the height of plumes compared to observations, while a revised algorithm has much better performance. A 12-bin size distribution reduced the forecast 2-bin size distribution bias error by 32 %.
Friderike Kuik, Andreas Kerschbaumer, Axel Lauer, Aurelia Lupascu, Erika von Schneidemesser, and Tim M. Butler
Atmos. Chem. Phys., 18, 8203–8225, https://doi.org/10.5194/acp-18-8203-2018, https://doi.org/10.5194/acp-18-8203-2018, 2018
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Modelled NOx concentrations are often underestimated compared to observations, and measurement studies show that reported NOx emissions in urban areas are often too low when the contribution from traffic is largest. This modelling study quantifies the underestimation of traffic NOx emissions in the Berlin–Brandenburg and finds that they are underestimated by ca. 50 % in the core urban area. More research is needed in order to more accurately understand real-world NOx emissions from traffic.
Andrea Mues, Axel Lauer, Aurelia Lupascu, Maheswar Rupakheti, Friderike Kuik, and Mark G. Lawrence
Geosci. Model Dev., 11, 2067–2091, https://doi.org/10.5194/gmd-11-2067-2018, https://doi.org/10.5194/gmd-11-2067-2018, 2018
Young-Hee Ryu, Alma Hodzic, Jerome Barre, Gael Descombes, and Patrick Minnis
Atmos. Chem. Phys., 18, 7509–7525, https://doi.org/10.5194/acp-18-7509-2018, https://doi.org/10.5194/acp-18-7509-2018, 2018
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We investigate whether errors in cloud predictions can significantly impact the ability of air quality models to predict surface ozone over the US during summer 2013. The comparison with satellite data shows that the model predicts ~ 55 % of clouds in the right locations and underpredicts cloud thickness. The error in daytime ozone is estimated to be 1–5 ppb and represents ~ 40 % of the ozone bias. The accurate predictions of clouds particularly benefits ozone predictions in urban areas.
Xi Chen, Mingjie Xie, Michael D. Hays, Eric Edgerton, Donna Schwede, and John T. Walker
Atmos. Chem. Phys., 18, 6829–6846, https://doi.org/10.5194/acp-18-6829-2018, https://doi.org/10.5194/acp-18-6829-2018, 2018
Joana Soares, Paul Andrew Makar, Yayne Aklilu, and Ayodeji Akingunola
Atmos. Chem. Phys., 18, 6543–6566, https://doi.org/10.5194/acp-18-6543-2018, https://doi.org/10.5194/acp-18-6543-2018, 2018
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Grouping data on the basis of (dis)similarity can be used to assess the efficacy of monitoring networks. The data are cross-compared in terms of temporal variation and magnitude of concentrations, and sites are ranked according to their level of potential redundancy. The methodology can be applied to measurement data, helping to identify sites with different measuring technologies or data flaws, and to model output, generating maps of areas of spatial representativeness of a monitoring site.
Ulas Im, Jørgen Brandt, Camilla Geels, Kaj Mantzius Hansen, Jesper Heile Christensen, Mikael Skou Andersen, Efisio Solazzo, Ioannis Kioutsioukis, Ummugulsum Alyuz, Alessandra Balzarini, Rocio Baro, Roberto Bellasio, Roberto Bianconi, Johannes Bieser, Augustin Colette, Gabriele Curci, Aidan Farrow, Johannes Flemming, Andrea Fraser, Pedro Jimenez-Guerrero, Nutthida Kitwiroon, Ciao-Kai Liang, Uarporn Nopmongcol, Guido Pirovano, Luca Pozzoli, Marje Prank, Rebecca Rose, Ranjeet Sokhi, Paolo Tuccella, Alper Unal, Marta Garcia Vivanco, Jason West, Greg Yarwood, Christian Hogrefe, and Stefano Galmarini
Atmos. Chem. Phys., 18, 5967–5989, https://doi.org/10.5194/acp-18-5967-2018, https://doi.org/10.5194/acp-18-5967-2018, 2018
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The impacts of air pollution on human health and their costs in Europe and the United States for the year 2010 ared modeled by a multi-model ensemble. In Europe, the number of premature deaths is calculated to be 414 000, while in the US it is estimated to be 160 000. Health impacts estimated by individual models can vary up to a factor of 3. Results show that the domestic emissions have the largest impact on premature deaths, compared to foreign sources.
Laura Palacios-Peña, Rocío Baró, Alexander Baklanov, Alessandra Balzarini, Dominik Brunner, Renate Forkel, Marcus Hirtl, Luka Honzak, José María López-Romero, Juan Pedro Montávez, Juan Luis Pérez, Guido Pirovano, Roberto San José, Wolfram Schröder, Johannes Werhahn, Ralf Wolke, Rahela Žabkar, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 18, 5021–5043, https://doi.org/10.5194/acp-18-5021-2018, https://doi.org/10.5194/acp-18-5021-2018, 2018
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Atmospheric aerosols modify the radiative budget of the Earth, and it is therefore mandatory to have an accurate representation of their optical properties for understanding their climatic role. This work therefore evaluates the skill in the representation of optical properties by different remote-sensing sensors and regional online coupled chemistry–climate models over Europe.
Christian Hogrefe, Peng Liu, George Pouliot, Rohit Mathur, Shawn Roselle, Johannes Flemming, Meiyun Lin, and Rokjin J. Park
Atmos. Chem. Phys., 18, 3839–3864, https://doi.org/10.5194/acp-18-3839-2018, https://doi.org/10.5194/acp-18-3839-2018, 2018
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This study quantifies the impacts of different representations of background ozone in state-of-the-science large-scale models on surface and aloft ozone burdens simulated by the CMAQ regional model over the United States. It also compares both the CMAQ simulations and the driving large-scale models to surface and upper air observations.
Cynthia H. Whaley, Paul A. Makar, Mark W. Shephard, Leiming Zhang, Junhua Zhang, Qiong Zheng, Ayodeji Akingunola, Gregory R. Wentworth, Jennifer G. Murphy, Shailesh K. Kharol, and Karen E. Cady-Pereira
Atmos. Chem. Phys., 18, 2011–2034, https://doi.org/10.5194/acp-18-2011-2018, https://doi.org/10.5194/acp-18-2011-2018, 2018
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Using a modified air quality forecasting model, we have found that a significant fraction (> 50 %) of ambient ammonia comes from re-emission from plants and soils in the broader Athabasca Oil Sands region and much of Alberta and Saskatchewan. We also found that about 20 % of ambient ammonia in Alberta and Saskatchewan came from forest fires in the summer of 2013. The addition of these two processes improved modelled ammonia, which was a motivating factor in undertaking this research.
Ying Chen, Ralf Wolke, Liang Ran, Wolfram Birmili, Gerald Spindler, Wolfram Schröder, Hang Su, Yafang Cheng, Ina Tegen, and Alfred Wiedensohler
Atmos. Chem. Phys., 18, 673–689, https://doi.org/10.5194/acp-18-673-2018, https://doi.org/10.5194/acp-18-673-2018, 2018
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The heterogeneous hydrolysis of N2O5 on particle surfaces is crucial for the nitrogen cycle in the atmosphere. The reaction rate is determined by meteorological and particle properties, but its parameterization in previous 3-D modelling studies did not comprehensively consider these parameters. We propose a parameterization to take these into account and improve nitrate prediction; we report that the organic coating suppression on the N2O5 reaction is not as important as expected in the EU.
Martijn Schaap, Sabine Banzhaf, Thomas Scheuschner, Markus Geupel, Carlijn Hendriks, Richard Kranenburg, Hans-Dieter Nagel, Arjo J. Segers, Angela von Schlutow, Roy Wichink Kruit, and Peter J. H. Builtjes
Biogeosciences Discuss., https://doi.org/10.5194/bg-2017-491, https://doi.org/10.5194/bg-2017-491, 2017
Revised manuscript has not been submitted
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Deposition of nitrogen and sulfur from the atmosphere on ecosystems causes a loss of biodiversity. We used a combination of atmospheric modelling and deposition observations to estimate the deposition to ecosystems across Germany. We estimate that 70 % of the ecosystems in Germany receive too much nitrogen from deposition. The results are used to determine whether economic activities causing nitrogen emissions are allowed in sensitive areas.
Astrid M. M. Manders, Peter J. H. Builtjes, Lyana Curier, Hugo A. C. Denier van der Gon, Carlijn Hendriks, Sander Jonkers, Richard Kranenburg, Jeroen J. P. Kuenen, Arjo J. Segers, Renske M. A. Timmermans, Antoon J. H. Visschedijk, Roy J. Wichink Kruit, W. Addo J. van Pul, Ferd J. Sauter, Eric van der Swaluw, Daan P. J. Swart, John Douros, Henk Eskes, Erik van Meijgaard, Bert van Ulft, Peter van Velthoven, Sabine Banzhaf, Andrea C. Mues, Rainer Stern, Guangliang Fu, Sha Lu, Arnold Heemink, Nils van Velzen, and Martijn Schaap
Geosci. Model Dev., 10, 4145–4173, https://doi.org/10.5194/gmd-10-4145-2017, https://doi.org/10.5194/gmd-10-4145-2017, 2017
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The regional-scale air quality model LOTOS–EUROS has been developed by a consortium of Dutch institutes. Recently, version 2.0 of the model was released as an open-source version. Next to a technical description and model evaluation for 2012, this paper presents the model developments in context of the history of air quality modelling and provides an outlook for future directions. Key and innovative applications of LOTOS–EUROS are also highlighted.
R. S. José, J. L. Pérez, L. Pérez, R. M. Gonzalez Barras, J. Pecci, and M. Palacios
Int. Arch. Photogramm. Remote Sens. Spatial Inf. Sci., XLII-3-W2, 83–89, https://doi.org/10.5194/isprs-archives-XLII-3-W2-83-2017, https://doi.org/10.5194/isprs-archives-XLII-3-W2-83-2017, 2017
Kathrin Gatzsche, Yoshiteru Iinuma, Andreas Tilgner, Anke Mutzel, Torsten Berndt, and Ralf Wolke
Atmos. Chem. Phys., 17, 13187–13211, https://doi.org/10.5194/acp-17-13187-2017, https://doi.org/10.5194/acp-17-13187-2017, 2017
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Secondary organic aerosol (SOA) represents an important fraction of the particulate matter and, thus, an advanced treatment of SOA processes in models is necessary. Therefore, this investigation aims at sensitivity studies of a kinetic description of SOA formation. The results reveal that the particle-phase state and the reactivity of the organic solutes are key parameters in the SOA formation. Overall, the results show that an advanced kinetic treatment enables improved model predictions.
Rohit Mathur, Jia Xing, Robert Gilliam, Golam Sarwar, Christian Hogrefe, Jonathan Pleim, George Pouliot, Shawn Roselle, Tanya L. Spero, David C. Wong, and Jeffrey Young
Atmos. Chem. Phys., 17, 12449–12474, https://doi.org/10.5194/acp-17-12449-2017, https://doi.org/10.5194/acp-17-12449-2017, 2017
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We extend CMAQ's applicability to the entire Northern Hemisphere to enable consistent examination of interactions between atmospheric processes occurring on various spatial and temporal scales. Improvements were made in model process representation, structure, and input data sets that enable a range of model applications including episodic intercontinental pollutant transport, long-term trends in air pollution across the Northern Hemisphere, and air pollution–climate interactions.
Heiko Bozem, Tim M. Butler, Mark G. Lawrence, Hartwig Harder, Monica Martinez, Dagmar Kubistin, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 17, 10565–10582, https://doi.org/10.5194/acp-17-10565-2017, https://doi.org/10.5194/acp-17-10565-2017, 2017
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We present airborne measurements and model simulations in the tropics and mid-latitudes during GABRIEL and HOOVER, respectively. Based only on in situ data net ozone formation/destruction tendencies (NOPR) are calculated and compared to a 3-D chemistry transport model. The NOPR is positive in the continental boundary layer and the upper troposphere above 6 km. In the marine boundary layer and the middle troposphere ozone destruction prevails. Fresh convection shows strong net ozone formation.
Efisio Solazzo, Christian Hogrefe, Augustin Colette, Marta Garcia-Vivanco, and Stefano Galmarini
Atmos. Chem. Phys., 17, 10435–10465, https://doi.org/10.5194/acp-17-10435-2017, https://doi.org/10.5194/acp-17-10435-2017, 2017
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The work here is conducted within the frame of AQMEII3 and promotes the use of diagnostic methods for the evaluation of air quality models. We highlight the need to move away from aggregated error metrics and to focus on the quality of the information that can be extracted from the model and the observation. This aids the understanding of the causes of model error, providing more useful information to model developers and users than can be gained from common evaluations.
Augustin Colette, Camilla Andersson, Astrid Manders, Kathleen Mar, Mihaela Mircea, Maria-Teresa Pay, Valentin Raffort, Svetlana Tsyro, Cornelius Cuvelier, Mario Adani, Bertrand Bessagnet, Robert Bergström, Gino Briganti, Tim Butler, Andrea Cappelletti, Florian Couvidat, Massimo D'Isidoro, Thierno Doumbia, Hilde Fagerli, Claire Granier, Chris Heyes, Zig Klimont, Narendra Ojha, Noelia Otero, Martijn Schaap, Katarina Sindelarova, Annemiek I. Stegehuis, Yelva Roustan, Robert Vautard, Erik van Meijgaard, Marta Garcia Vivanco, and Peter Wind
Geosci. Model Dev., 10, 3255–3276, https://doi.org/10.5194/gmd-10-3255-2017, https://doi.org/10.5194/gmd-10-3255-2017, 2017
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The EURODELTA-Trends numerical experiment has been designed to assess the capability of chemistry-transport models to capture the evolution of surface air quality over the 1990–2010 period in Europe. It also includes sensitivity experiments in order to analyse the relative contribution of (i) emission changes, (ii) meteorological variability, and (iii) boundary conditions to air quality trends. The article is a detailed presentation of the experiment design and participating models.
Jia Xing, Jiandong Wang, Rohit Mathur, Shuxiao Wang, Golam Sarwar, Jonathan Pleim, Christian Hogrefe, Yuqiang Zhang, Jingkun Jiang, David C. Wong, and Jiming Hao
Atmos. Chem. Phys., 17, 9869–9883, https://doi.org/10.5194/acp-17-9869-2017, https://doi.org/10.5194/acp-17-9869-2017, 2017
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The assessment of the impacts of aerosol direct effects (ADE) is important for understanding emission reduction strategies that seek co-benefits associated with reductions in both particulate matter and ozone. This study quantifies the ADE impacts on tropospheric ozone by using a two-way coupled meteorology and atmospheric chemistry model. Results suggest that reducing ADE may have the potential risk of increasing ozone in winter, but it will benefit the reduction of maxima ozone in summer.
Rocío Baró, Laura Palacios-Peña, Alexander Baklanov, Alessandra Balzarini, Dominik Brunner, Renate Forkel, Marcus Hirtl, Luka Honzak, Juan Luis Pérez, Guido Pirovano, Roberto San José, Wolfram Schröder, Johannes Werhahn, Ralf Wolke, Rahela Žabkar, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 17, 9677–9696, https://doi.org/10.5194/acp-17-9677-2017, https://doi.org/10.5194/acp-17-9677-2017, 2017
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The influence on modeled max., mean and min. temperature over Europe of including aerosol–radiation–cloud interactions has been assessed for two case studies in 2010. Data were taken from an ensemble of online regional chemistry–climate models from EuMetChem COST Action. The results indicate that including these interactions clearly improves the spatiotemporal variability in the temperature signal simulated by the models, with implications for reducing the uncertainty in climate projections.
Andrea Mues, Maheswar Rupakheti, Christoph Münkel, Axel Lauer, Heiko Bozem, Peter Hoor, Tim Butler, and Mark G. Lawrence
Atmos. Chem. Phys., 17, 8157–8176, https://doi.org/10.5194/acp-17-8157-2017, https://doi.org/10.5194/acp-17-8157-2017, 2017
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Ceilometer measurements taken in the Kathmandu Valley, Nepal, were used to study the temporal and spatial evolution of the mixing layer height in the valley. This provides important information on the vertical structure of the atmosphere and can thus also help to understand the mixing of air pollutants (e.g. black carbon) in the valley. The seasonal and diurnal cycles of the mixing layer were found to be highly dependent on meteorology and mainly anticorrelated to black carbon concentrations.
Sudhakar Dipu, Johannes Quaas, Ralf Wolke, Jens Stoll, Andreas Mühlbauer, Odran Sourdeval, Marc Salzmann, Bernd Heinold, and Ina Tegen
Geosci. Model Dev., 10, 2231–2246, https://doi.org/10.5194/gmd-10-2231-2017, https://doi.org/10.5194/gmd-10-2231-2017, 2017
Johannes Bieser, Franz Slemr, Jesse Ambrose, Carl Brenninkmeijer, Steve Brooks, Ashu Dastoor, Francesco DeSimone, Ralf Ebinghaus, Christian N. Gencarelli, Beate Geyer, Lynne E. Gratz, Ian M. Hedgecock, Daniel Jaffe, Paul Kelley, Che-Jen Lin, Lyatt Jaegle, Volker Matthias, Andrei Ryjkov, Noelle E. Selin, Shaojie Song, Oleg Travnikov, Andreas Weigelt, Winston Luke, Xinrong Ren, Andreas Zahn, Xin Yang, Yun Zhu, and Nicola Pirrone
Atmos. Chem. Phys., 17, 6925–6955, https://doi.org/10.5194/acp-17-6925-2017, https://doi.org/10.5194/acp-17-6925-2017, 2017
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We conducted a multi model study to investigate our ability to reproduce the vertical distribution of mercury in the atmosphere. For this, we used observational data from over 40 aircraft flights in EU and US. We compared observations to the results of seven chemistry transport models and found that the models are able to reproduce vertical gradients of total and elemental Hg. Finally, we found that different chemical reactions seem responsible for the oxidation of Hg depending on altitude.
Oleg Travnikov, Hélène Angot, Paulo Artaxo, Mariantonia Bencardino, Johannes Bieser, Francesco D'Amore, Ashu Dastoor, Francesco De Simone, María del Carmen Diéguez, Aurélien Dommergue, Ralf Ebinghaus, Xin Bin Feng, Christian N. Gencarelli, Ian M. Hedgecock, Olivier Magand, Lynwill Martin, Volker Matthias, Nikolay Mashyanov, Nicola Pirrone, Ramesh Ramachandran, Katie Alana Read, Andrei Ryjkov, Noelle E. Selin, Fabrizio Sena, Shaojie Song, Francesca Sprovieri, Dennis Wip, Ingvar Wängberg, and Xin Yang
Atmos. Chem. Phys., 17, 5271–5295, https://doi.org/10.5194/acp-17-5271-2017, https://doi.org/10.5194/acp-17-5271-2017, 2017
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The study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measurement data and simulation results of chemical transport models. Evaluation of the model simulations and numerical experiments against observations allows explaining spatial and temporal variations of Hg concentration in the near-surface atmospheric layer and shows possibility of multiple pathways of Hg oxidation occurring concurrently in various parts of the atmosphere.
K. Wyat Appel, Sergey L. Napelenok, Kristen M. Foley, Havala O. T. Pye, Christian Hogrefe, Deborah J. Luecken, Jesse O. Bash, Shawn J. Roselle, Jonathan E. Pleim, Hosein Foroutan, William T. Hutzell, George A. Pouliot, Golam Sarwar, Kathleen M. Fahey, Brett Gantt, Robert C. Gilliam, Nicholas K. Heath, Daiwen Kang, Rohit Mathur, Donna B. Schwede, Tanya L. Spero, David C. Wong, and Jeffrey O. Young
Geosci. Model Dev., 10, 1703–1732, https://doi.org/10.5194/gmd-10-1703-2017, https://doi.org/10.5194/gmd-10-1703-2017, 2017
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The Community Multiscale Air Quality (CMAQ) model is a comprehensive multipollutant air quality modeling system. The CMAQ model is used extensively throughout the world to simulate air pollutants for many purposes, including regulatory and air quality forecasting applications. This work describes the scientific updates made to the latest version of the CMAQ modeling system (CMAQv5.1) and presents an evaluation of the new model against observations and results from the previous model version.
Efisio Solazzo, Roberto Bianconi, Christian Hogrefe, Gabriele Curci, Paolo Tuccella, Ummugulsum Alyuz, Alessandra Balzarini, Rocío Baró, Roberto Bellasio, Johannes Bieser, Jørgen Brandt, Jesper H. Christensen, Augistin Colette, Xavier Francis, Andrea Fraser, Marta Garcia Vivanco, Pedro Jiménez-Guerrero, Ulas Im, Astrid Manders, Uarporn Nopmongcol, Nutthida Kitwiroon, Guido Pirovano, Luca Pozzoli, Marje Prank, Ranjeet S. Sokhi, Alper Unal, Greg Yarwood, and Stefano Galmarini
Atmos. Chem. Phys., 17, 3001–3054, https://doi.org/10.5194/acp-17-3001-2017, https://doi.org/10.5194/acp-17-3001-2017, 2017
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As part of the third phase of AQMEII, this study uses timescale analysis to apportion error to the responsible processes, detect causes of model error, and identify the processes and scales that require dedicated investigations. The analysis tackles model performance gauging through measurement-to-model comparison, error decomposition, and time series analysis of model biases for ozone, CO, SO2, NO, NO2, PM10, PM2.5, wind speed, and temperature over Europe and North America.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Stefano Galmarini, Brigitte Koffi, Efisio Solazzo, Terry Keating, Christian Hogrefe, Michael Schulz, Anna Benedictow, Jan Jurgen Griesfeller, Greet Janssens-Maenhout, Greg Carmichael, Joshua Fu, and Frank Dentener
Atmos. Chem. Phys., 17, 1543–1555, https://doi.org/10.5194/acp-17-1543-2017, https://doi.org/10.5194/acp-17-1543-2017, 2017
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We present an overview of the coordinated global numerical modelling experiments performed during 2012–2016 by the Task Force on Hemispheric Transport of Air Pollution (TF HTAP), the regional experiments by the Air Quality Model Evaluation International Initiative (AQMEII) over Europe and North America, and the Model Intercomparison Study for Asia (MICS-Asia). Given the organizational complexity of bringing together these three initiatives, the experiment organization is presented.
Christian N. Gencarelli, Johannes Bieser, Francesco Carbone, Francesco De Simone, Ian M. Hedgecock, Volker Matthias, Oleg Travnikov, Xin Yang, and Nicola Pirrone
Atmos. Chem. Phys., 17, 627–643, https://doi.org/10.5194/acp-17-627-2017, https://doi.org/10.5194/acp-17-627-2017, 2017
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Atmospheric deposition is an important pathway by which Hg reaches marine ecosystems, where it can be methylated and enter the base of food chain. High resolution numerical experiments has been performed in order to investigate the contributions (sensitivity) of the Hg anthtropogenic emissions, speciation and atmospherical chemical reactions on Hg depositions over Europe. The comparison of wet deposition fluxes and concentrations measured on 28 monitioring sites were used to support the analysis.
Ioannis Kioutsioukis, Ulas Im, Efisio Solazzo, Roberto Bianconi, Alba Badia, Alessandra Balzarini, Rocío Baró, Roberto Bellasio, Dominik Brunner, Charles Chemel, Gabriele Curci, Hugo Denier van der Gon, Johannes Flemming, Renate Forkel, Lea Giordano, Pedro Jiménez-Guerrero, Marcus Hirtl, Oriol Jorba, Astrid Manders-Groot, Lucy Neal, Juan L. Pérez, Guidio Pirovano, Roberto San Jose, Nicholas Savage, Wolfram Schroder, Ranjeet S. Sokhi, Dimiter Syrakov, Paolo Tuccella, Johannes Werhahn, Ralf Wolke, Christian Hogrefe, and Stefano Galmarini
Atmos. Chem. Phys., 16, 15629–15652, https://doi.org/10.5194/acp-16-15629-2016, https://doi.org/10.5194/acp-16-15629-2016, 2016
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Four ensemble methods are applied to two annual AQMEII datasets and their performance is compared for O3, NO2 and PM10. The goal of the study is to quantify to what extent we can extract predictable signals from an ensemble with superior skill at each station over the single models and the ensemble mean. The promotion of the right amount of accuracy and diversity within the ensemble results in an average additional skill of up to 31 % compared to using the full ensemble in an unconditional way.
Christos I. Efstathiou, Jana Matejovičová, Johannes Bieser, and Gerhard Lammel
Atmos. Chem. Phys., 16, 15327–15345, https://doi.org/10.5194/acp-16-15327-2016, https://doi.org/10.5194/acp-16-15327-2016, 2016
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Gas-particle partitioning is an important process that determines the fate and long-range transport potential of persistent organic pollutants. This work is the first effort to evaluate the behaviour of parameterizations within a regional air quality system adapted for Europe. Results corroborate the significance of the chosen implementation in predicting ambient levels and transport patterns. Implications point to improvements on the side of the emission inventories and aerosol module.
Friderike Kuik, Axel Lauer, Galina Churkina, Hugo A. C. Denier van der Gon, Daniel Fenner, Kathleen A. Mar, and Tim M. Butler
Geosci. Model Dev., 9, 4339–4363, https://doi.org/10.5194/gmd-9-4339-2016, https://doi.org/10.5194/gmd-9-4339-2016, 2016
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The study evaluates the performance of a setup of the Weather Research and Forecasting model with chemistry and aerosols (WRF–Chem) for the Berlin–Brandenburg region of Germany. Its sensitivity to updating urban input parameters based on structural data for Berlin is tested, specifying land use classes on a sub-grid scale, downscaling the original emissions to a resolution of ca. 1 km by 1 km for Berlin based on proxy data and model resolution.
Carolina Cavazos Guerra, Axel Lauer, Andreas B. Herber, Tim M. Butler, Annette Rinke, and Klaus Dethloff
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-942, https://doi.org/10.5194/acp-2016-942, 2016
Revised manuscript has not been submitted
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Accurate description of the Arctic atmosphere is a challenge for the modelling comunity. We evaluate the performance of the Weather Research and Forecast model (WRF) in the Eurasian Arctic and analyse the implications of data to initialise the model and a land surface scheme. The results show that biases can be related to the quality of data used and in the case of black carbon concentrations, to emission data. More long term measurements are need for model Validation in the area.
Andreas Weigelt, Franz Slemr, Ralf Ebinghaus, Nicola Pirrone, Johannes Bieser, Jan Bödewadt, Giulio Esposito, and Peter F. J. van Velthoven
Atmos. Chem. Phys., 16, 13653–13668, https://doi.org/10.5194/acp-16-13653-2016, https://doi.org/10.5194/acp-16-13653-2016, 2016
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Hg ∕ SO2, Hg ∕ CO, and NOx ∕ SO2 emission ratios (ERs) in the plume of the coal-fired power plant (CFPP), Lippendorf, near Leipzig in Germany, were determined in August 2013. GOM fraction of mercury emissions was also assessed. Measured Hg ∕ SO2 and Hg ∕ CO ERs were consistent with the ratios calculated from annual emissions in 2013 reported by the CFPP operator. The NOx ∕ SO2 ER was somewhat lower. GOM fractions of ~ 40 % of CFPP mercury emissions in current emission inventories are overestimated.
Kathleen A. Mar, Narendra Ojha, Andrea Pozzer, and Tim M. Butler
Geosci. Model Dev., 9, 3699–3728, https://doi.org/10.5194/gmd-9-3699-2016, https://doi.org/10.5194/gmd-9-3699-2016, 2016
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Ground-level ozone is an air pollutant with adverse effects on human and ecosystem health and is also a climate forcer with a significant warming effect. This paper presents the setup and evaluation of a model for ozone air quality over Europe. Within the model evaluation, we compare the use of two commonly used photochemical schemes, and we conclude that uncertainties in the representation of chemistry are important to consider when using air quality models for policy applications.
Bertrand Bessagnet, Guido Pirovano, Mihaela Mircea, Cornelius Cuvelier, Armin Aulinger, Giuseppe Calori, Giancarlo Ciarelli, Astrid Manders, Rainer Stern, Svetlana Tsyro, Marta García Vivanco, Philippe Thunis, Maria-Teresa Pay, Augustin Colette, Florian Couvidat, Frédérik Meleux, Laurence Rouïl, Anthony Ung, Sebnem Aksoyoglu, José María Baldasano, Johannes Bieser, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, Sandro Finardi, Richard Kranenburg, Camillo Silibello, Claudio Carnevale, Wenche Aas, Jean-Charles Dupont, Hilde Fagerli, Lucia Gonzalez, Laurent Menut, André S. H. Prévôt, Pete Roberts, and Les White
Atmos. Chem. Phys., 16, 12667–12701, https://doi.org/10.5194/acp-16-12667-2016, https://doi.org/10.5194/acp-16-12667-2016, 2016
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The EURODELTA III exercise allows a very comprehensive intercomparison and evaluation of air quality models' performance. On average, the models provide a rather good picture of the particulate matter (PM) concentrations over Europe even if the highest concentrations are underestimated. The meteorology is responsible for model discrepancies, while the lack of emissions, particularly in winter, is mentioned as the main reason for the underestimations of PM.
Ying Chen, Yafang Cheng, Nan Ma, Ralf Wolke, Stephan Nordmann, Stephanie Schüttauf, Liang Ran, Birgit Wehner, Wolfram Birmili, Hugo A. C. Denier van der Gon, Qing Mu, Stefan Barthel, Gerald Spindler, Bastian Stieger, Konrad Müller, Guang-Jie Zheng, Ulrich Pöschl, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 16, 12081–12097, https://doi.org/10.5194/acp-16-12081-2016, https://doi.org/10.5194/acp-16-12081-2016, 2016
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Sea salt aerosol (SSA) is important for primary and secondary aerosols on a global scale. During 10–20 September 2013, the SSA mass concentration was overestimated by a factor of 8–20 over central Europe by WRF-Chem model, stem from the uncertainty of its emission scheme. This could facilitate the coarse-mode nitrate formation (~ 140 % but inhibit the fine-mode nitrate formation (~−20 %). A special long-range transport mechanism could broaden this influence of SSA to a larger downwind region.
Jane Coates, Kathleen A. Mar, Narendra Ojha, and Tim M. Butler
Atmos. Chem. Phys., 16, 11601–11615, https://doi.org/10.5194/acp-16-11601-2016, https://doi.org/10.5194/acp-16-11601-2016, 2016
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This modelling study reproduced the non-linear relationship of ozone, NOx and temperature using various chemical mechanisms previously determined from observational studies. Under urban conditions, faster reaction rates rather than increased isoprene emissions led to a slightly greater increase of ozone with temperature using different NOx conditions. This study also shows that the increase of ozone with temperature is more sensitive to atmospheric mixing than the choice of chemical mechanism.
Quazi Z. Rasool, Rui Zhang, Benjamin Lash, Daniel S. Cohan, Ellen J. Cooter, Jesse O. Bash, and Lok N. Lamsal
Geosci. Model Dev., 9, 3177–3197, https://doi.org/10.5194/gmd-9-3177-2016, https://doi.org/10.5194/gmd-9-3177-2016, 2016
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This study updates the representation of soil NO emissions in a regional air quality model. The implementation enhances the representation of biome types and dynamic fertilizer use. Previous modeling of soil NO in CMAQ had tended to under-estimate emissions and misrepresent their response to soil conditions and meteorology. We evaluate results against satellite observations of NO2, and quantify the impacts of the new parameterization on simulations of ozone and particulate matter.
Jia Xing, Rohit Mathur, Jonathan Pleim, Christian Hogrefe, Jiandong Wang, Chuen-Meei Gan, Golam Sarwar, David C. Wong, and Stuart McKeen
Atmos. Chem. Phys., 16, 10865–10877, https://doi.org/10.5194/acp-16-10865-2016, https://doi.org/10.5194/acp-16-10865-2016, 2016
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Downward transport of ozone from the stratosphere has large impacts on surface concentration and needs to be properly represented in regional models. This study developed a seasonally and spatially varying PV-based function from an investigation of the relationship between PV and O3. The implementation of the new function significantly improves the model's performance in O3 simulation, which enables a more accurate simulation of the vertical distribution of O3 across the Northern Hemisphere.
Sam J. Silva, Colette L. Heald, Jeffrey A. Geddes, Kemen G. Austin, Prasad S. Kasibhatla, and Miriam E. Marlier
Atmos. Chem. Phys., 16, 10621–10635, https://doi.org/10.5194/acp-16-10621-2016, https://doi.org/10.5194/acp-16-10621-2016, 2016
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We investigate the impacts of current (2010) and future (2020) oil palm plantations across Southeast Asia on surface–atmosphere exchange and air quality using satellite data, land maps, and a chemical transport model. These changes lead to increases in surface ozone and particulate matter. Oil palm plantations are likely to continue to degrade regional air quality in the coming decade and hinder efforts to achieve air quality regulations in major urban areas such as Kuala Lumpur and Singapore.
Daniel Neumann, Volker Matthias, Johannes Bieser, Armin Aulinger, and Markus Quante
Atmos. Chem. Phys., 16, 9905–9933, https://doi.org/10.5194/acp-16-9905-2016, https://doi.org/10.5194/acp-16-9905-2016, 2016
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Atmospheric sea salt particles provide surface area for the condensation of gaseous substances and, thus, impact these substances' atmospheric residence time and chemical reactions. The number and size of sea salt particles govern the strength of these impacts. Therefore, these parameters should be reflected accurately in chemistry transport models. In this study, three different sea salt emission functions are compared in order to evaluate which one is best suited for the given model setup.
Alma Hodzic, Prasad S. Kasibhatla, Duseong S. Jo, Christopher D. Cappa, Jose L. Jimenez, Sasha Madronich, and Rokjin J. Park
Atmos. Chem. Phys., 16, 7917–7941, https://doi.org/10.5194/acp-16-7917-2016, https://doi.org/10.5194/acp-16-7917-2016, 2016
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The global budget and spatial distribution of secondary organic aerosol (SOA) are highly uncertain in chemistry-climate models, which reflects our inability to characterize all phases of the OA lifecycle. We have performed global model simulations with the newly proposed formation and removal processes (photolysis and heterogeneous chemistry) and shown that SOA is a far more dynamic system, with 4 times stronger production rates and more efficient removal mechanisms, than assumed in models.
Boris Bonn, Erika von Schneidemesser, Dorota Andrich, Jörn Quedenau, Holger Gerwig, Anja Lüdecke, Jürgen Kura, Axel Pietsch, Christian Ehlers, Dieter Klemp, Claudia Kofahl, Rainer Nothard, Andreas Kerschbaumer, Wolfgang Junkermann, Rüdiger Grote, Tobias Pohl, Konradin Weber, Birgit Lode, Philipp Schönberger, Galina Churkina, Tim M. Butler, and Mark G. Lawrence
Atmos. Chem. Phys., 16, 7785–7811, https://doi.org/10.5194/acp-16-7785-2016, https://doi.org/10.5194/acp-16-7785-2016, 2016
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The distribution of air pollutants (gases and particles) have been investigated in different environments in Potsdam, Germany. Remarkable variations of the pollutants have been observed for distances of tens of meters by bicycles, vans and aircraft. Vegetated areas caused reductions depending on the pollutants, the vegetation type and dimensions. Our measurements show the pollutants to be of predominantly local origin, resulting in a huge challenge for common models to resolve.
Jesse O. Bash, Kirk R. Baker, and Melinda R. Beaver
Geosci. Model Dev., 9, 2191–2207, https://doi.org/10.5194/gmd-9-2191-2016, https://doi.org/10.5194/gmd-9-2191-2016, 2016
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Biogenic volatile organic compounds (BVOCs) participate in reactions that can lead to secondarily formed ozone and particulate matter impacting air quality and climate and are important inputs for atmospheric models. BVOC emissions are sensitive to the vegetation species and leaf temperature. Here, we have improved the vegetation data and modeled leaf temperature of the Biogenic Emission Inventory System model. Updated algorithms improved model evaluation against observations in California.
Efisio Solazzo and Stefano Galmarini
Atmos. Chem. Phys., 16, 6263–6283, https://doi.org/10.5194/acp-16-6263-2016, https://doi.org/10.5194/acp-16-6263-2016, 2016
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A new technique to assess the quality of model results from a regional-scale air quality model is presented. The techniques are based on standard statistical parameters but work on spectral decomposition of model and measurement time series. This allows for the identification of scale-related processes for which the largest divergency between model and observed data is found. The technique is applied to the data collected during the second phase of the AQMEI Initiative.
Andreas Weigelt, Ralf Ebinghaus, Nicola Pirrone, Johannes Bieser, Jan Bödewadt, Giulio Esposito, Franz Slemr, Peter F. J. van Velthoven, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 16, 4135–4146, https://doi.org/10.5194/acp-16-4135-2016, https://doi.org/10.5194/acp-16-4135-2016, 2016
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We show the first mercury profile measurements over Europe since 1996. Besides gaseous elemental mercury (GEM) and total gaseous mercury (TGM), the gases CO, SO2, NOx, and O3 were measured from aboard a research aircraft over four European locations. Compared to the boundary layer, the concentration of GEM and TGM in the free troposphere was 10–30% lower. Inside the individual layers no vertical gradient was apparent. Combined with CARIBIC data, a unique profile from 0.4 to 10.5 km is provided.
Sean Coburn, Barbara Dix, Eric Edgerton, Christopher D. Holmes, Douglas Kinnison, Qing Liang, Arnout ter Schure, Siyuan Wang, and Rainer Volkamer
Atmos. Chem. Phys., 16, 3743–3760, https://doi.org/10.5194/acp-16-3743-2016, https://doi.org/10.5194/acp-16-3743-2016, 2016
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Here we present a day of case study measurements of the vertical distribution of bromine monoxide over the coastal region of the Gulf of Mexico. These measurements are used to assess the contribution of bromine radicals to the oxidation of elemental mercury in the troposphere. We find that the measured levels of bromine in the troposphere are sufficient to quickly oxidize mercury, which has significant implications for our understanding of atmospheric mercury processes.
Daniel Neumann, Volker Matthias, Johannes Bieser, Armin Aulinger, and Markus Quante
Atmos. Chem. Phys., 16, 2921–2942, https://doi.org/10.5194/acp-16-2921-2016, https://doi.org/10.5194/acp-16-2921-2016, 2016
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Sea salt emissions were updated to be dependent on salinity which improved sodium predictions in the Baltic Sea region. The impact of sea salt on atmospheric nitrate and ammonium concentrations and on nitrogen deposition in the North and Baltic Sea region is assessed. Sea salt has a low effect on nitrate concentrations but does not improve them. 3 to 7 % of the nitrogen deposition into the North Sea is accounted to the presence of sea salt. In the Baltic Sea, the contribution is negligible.
Jeffrey A. Geddes, Colette L. Heald, Sam J. Silva, and Randall V. Martin
Atmos. Chem. Phys., 16, 2323–2340, https://doi.org/10.5194/acp-16-2323-2016, https://doi.org/10.5194/acp-16-2323-2016, 2016
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Land use and land cover changes driven by anthropogenic activities or natural causes (e.g., forestry management, agriculture, wildfires) can impact climate and air quality in many complex ways. Using a state-of-the-art chemistry model, we investigate how tree mortality in the US due to insect infestation and disease outbreak may impact atmospheric composition. We find that the surface concentrations of ozone and aerosol can be altered due to changing background emissions and loss processes.
Ying Chen, Ya-Fang Cheng, Stephan Nordmann, Wolfram Birmili, Hugo A. C. Denier van der Gon, Nan Ma, Ralf Wolke, Birgit Wehner, Jia Sun, Gerald Spindler, Qing Mu, Ulrich Pöschl, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 16, 1823–1835, https://doi.org/10.5194/acp-16-1823-2016, https://doi.org/10.5194/acp-16-1823-2016, 2016
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We evaluated the EC point sources in Germany with high-resolution simulation by WRF-Chem, and find out that point sources contribute too much EC in the coarse mode aerosol mass. The area emissions in Eastern Europe and Russia also allocate too much EC emission in coarse mode in the EUCAARI EC emission inventory. Because of the shorter life time of coarse mode EC, about 20–40 % less EC can be transported to Melpitz from Eastern Europe. Size segregation information is important for EC inventories.
Y. S. La, M. Camredon, P. J. Ziemann, R. Valorso, A. Matsunaga, V. Lannuque, J. Lee-Taylor, A. Hodzic, S. Madronich, and B. Aumont
Atmos. Chem. Phys., 16, 1417–1431, https://doi.org/10.5194/acp-16-1417-2016, https://doi.org/10.5194/acp-16-1417-2016, 2016
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The potential impact of chamber walls on the loss of gaseous organic species and secondary organic aerosol (SOA) formation has been explored using the GECKO-A modeling tool, which explicitly represents SOA formation and gas-wall partitioning. The model was compared with 41 smog chamber experiments of SOA formation under OH oxidation of alkane and alkene serie. The organic vapor loss to the chamber walls is found to affect SOA yields as well as the composition of the gas and the particle phase.
A. J. Rusumdar, R. Wolke, A. Tilgner, and H. Herrmann
Geosci. Model Dev., 9, 247–281, https://doi.org/10.5194/gmd-9-247-2016, https://doi.org/10.5194/gmd-9-247-2016, 2016
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The present paper was aimed at the further development of SPACCIM to treat both complex multiphase chemistry and phase transfer processes considering new non-ideality properties of concentrated solutions. Model studies showed the applicability of the new kinetic model approach for complex aerosol mixtures and detailed chemical mechanisms. Simulations have implied that the treatment of non-ideality should be mandatory for modeling multiphase chemical processes in deliquesced particles.
V. Matthias, A. Aulinger, A. Backes, J. Bieser, B. Geyer, M. Quante, and M. Zeretzke
Atmos. Chem. Phys., 16, 759–776, https://doi.org/10.5194/acp-16-759-2016, https://doi.org/10.5194/acp-16-759-2016, 2016
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Scenarios for future shipping emissions in the North Sea were developed. Compared to today, the contribution of shipping to the nitrogen dioxide and ozone concentrations will increase due to the expected enhanced traffic by more than 20 % and 5 %, respectively, by 2030 if no regulation for further emission reductions is implemented. PM2.5 will decrease slightly because the sulfur content in ship fuels will be reduced.
A. Aulinger, V. Matthias, M. Zeretzke, J. Bieser, M. Quante, and A. Backes
Atmos. Chem. Phys., 16, 739–758, https://doi.org/10.5194/acp-16-739-2016, https://doi.org/10.5194/acp-16-739-2016, 2016
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A multi-model approach consisting of a bottom-up ship emissions model and a chemistry transport model was used to evaluate the impact of shipping on air quality in North Sea bordering countries. As an example, the results of the simulations indicated that the relative contribution of ships to NO2 concentration levels ashore close to the sea can reach up to 25 % in summer and 15 % in winter. Some hundred kilometers away from the sea, the contribution was about 6 % in summer and 4 % in winter.
J. He, Y. Zhang, S. Tilmes, L. Emmons, J.-F. Lamarque, T. Glotfelty, A. Hodzic, and F. Vitt
Geosci. Model Dev., 8, 3999–4025, https://doi.org/10.5194/gmd-8-3999-2015, https://doi.org/10.5194/gmd-8-3999-2015, 2015
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The global simulations with CB05_GE and MOZART-4x predict similar chemical profiles for major gases compared to aircraft measurements, with better agreement for the NOy profile by CB05_GE. The SOA concentrations of SOA at four sites in CONUS and organic carbon over the IMPROVE sites are better predicted by MOZART-4x. The two simulations result in a global average difference of 0.5W m-2 in simulated shortwave cloud radiative forcing, with up to 13.6W m-2 over subtropical regions.
M. W. Shephard, C. A. McLinden, K. E. Cady-Pereira, M. Luo, S. G. Moussa, A. Leithead, J. Liggio, R. M. Staebler, A. Akingunola, P. Makar, P. Lehr, J. Zhang, D. K. Henze, D. B. Millet, J. O. Bash, L. Zhu, K. C. Wells, S. L. Capps, S. Chaliyakunnel, M. Gordon, K. Hayden, J. R. Brook, M. Wolde, and S.-M. Li
Atmos. Meas. Tech., 8, 5189–5211, https://doi.org/10.5194/amt-8-5189-2015, https://doi.org/10.5194/amt-8-5189-2015, 2015
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This study provides direct validations of Tropospheric Emission Spectrometer (TES) satellite retrieved profiles against coincident aircraft profiles of carbon monoxide, ammonia, methanol, and formic acid, all of which are of interest for air quality. The comparisons are performed over the Canadian oil sands region during an intensive field campaign in support of the Joint Canada-Alberta Implementation Plan for the Oil Sands Monitoring (JOSM). Initial model evaluations are also provided.
Y. Zheng, N. Unger, A. Hodzic, L. Emmons, C. Knote, S. Tilmes, J.-F. Lamarque, and P. Yu
Atmos. Chem. Phys., 15, 13487–13506, https://doi.org/10.5194/acp-15-13487-2015, https://doi.org/10.5194/acp-15-13487-2015, 2015
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Nitrogen oxides (NOx) play an important but complex role in secondary organic aerosol (SOA) formation. In this study we update the SOA scheme in a global 3-D chemistry-climate model by implementing a 4-product volatility basis set (VBS) framework with NOx-dependent yields and simplified aging parameterizations. We find that the SOA decrease in response to a 50% reduction in anthropogenic NOx emissions is limited due to the buffering in different chemical pathways.
L. Zhu, D. Henze, J. Bash, G.-R. Jeong, K. Cady-Pereira, M. Shephard, M. Luo, F. Paulot, and S. Capps
Atmos. Chem. Phys., 15, 12823–12843, https://doi.org/10.5194/acp-15-12823-2015, https://doi.org/10.5194/acp-15-12823-2015, 2015
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We implement new diurnal variation scheme for ammonia livestock emissions and bidirectional exchange scheme and its adjoint in the GEOS-Chem global chemical transport model. Updated diurnal variability improves modeled-to-hourly in situ measurements comparison. The ammonium soil pool in the bidirectional exchange model largely extends the ammonia lifetime in the atmosphere. Large model biases remain as livestock emissions are still underestimated.
B. Gantt, J. T. Kelly, and J. O. Bash
Geosci. Model Dev., 8, 3733–3746, https://doi.org/10.5194/gmd-8-3733-2015, https://doi.org/10.5194/gmd-8-3733-2015, 2015
A. Lupascu, R. Easter, R. Zaveri, M. Shrivastava, M. Pekour, J. Tomlinson, Q. Yang, H. Matsui, A. Hodzic, Q. Zhang, and J. D. Fast
Atmos. Chem. Phys., 15, 12283–12313, https://doi.org/10.5194/acp-15-12283-2015, https://doi.org/10.5194/acp-15-12283-2015, 2015
C.-M. Gan, J. Pleim, R. Mathur, C. Hogrefe, C. N. Long, J. Xing, D. Wong, R. Gilliam, and C. Wei
Atmos. Chem. Phys., 15, 12193–12209, https://doi.org/10.5194/acp-15-12193-2015, https://doi.org/10.5194/acp-15-12193-2015, 2015
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This study attempts to determine the consequences of the changes in tropospheric aerosol burden arising from substantial reductions in emissions of SO2 and NOx associated with control measures under the Clean Air Act especially on trends in solar radiation. Comparisons of model results with observations of aerosol optical depth, aerosol concentration, and radiation demonstrate that the coupled WRF-CMAQ model is capable of replicating the trends well even though it tends to underestimate the AOD.
Y. Zhou, H. Mao, K. Demerjian, C. Hogrefe, and J. Liu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-27253-2015, https://doi.org/10.5194/acpd-15-27253-2015, 2015
Revised manuscript not accepted
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Baseline carbon monoxide (CO) and ozone (O3) were studied at seven rural sites in the Northeast U.S. during varying periods over 2001 – 2010. Baseline CO at all sites decreased significantly at a rate between -4.3 – -2.3 ppbv yr-1, while baseline O3 was relatively constant. Interannual and seasonal variations of baseline CO and O3 were related to increasing Asian emissions, NOx emissions reduction in urban areas, global biomass burning emissions, and meteorological conditions.
J. Xing, R. Mathur, J. Pleim, C. Hogrefe, C.-M. Gan, D. C. Wong, and C. Wei
Atmos. Chem. Phys., 15, 9997–10018, https://doi.org/10.5194/acp-15-9997-2015, https://doi.org/10.5194/acp-15-9997-2015, 2015
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The ability of a coupled meteorology-chemistry model (WRF-CMAQ) to reproduce the historical trend in AOD and clear-sky SWR over the N. Hemisphere has been evaluated through a comparison of 21-year simulated results with observation-derived records from 1990 to 2010. Questions of how well the model represents the regional and temporal variability of aerosol burden and DRE, and whether the model is able to capture past trends in aerosol loading and associated radiation effects, will be addressed.
A. Hodzic, S. Madronich, P. S. Kasibhatla, G. Tyndall, B. Aumont, J. L. Jimenez, J. Lee-Taylor, and J. Orlando
Atmos. Chem. Phys., 15, 9253–9269, https://doi.org/10.5194/acp-15-9253-2015, https://doi.org/10.5194/acp-15-9253-2015, 2015
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Our study combines process and global chemistry modeling to investigate the potential effect of gas- and particle-phase organic photolysis reactions on the formation and lifetime of secondary organic aerosols (SOAs). Photolysis of the oxidation intermediates that partition between gas and particle phases to form SOA is not included in 3D models. Our results suggest that exposure to UV light can suppress the formation of SOA or even lead to its substantial loss (comparable to wet deposition).
J. Zhu, T. Wang, J. Bieser, and V. Matthias
Atmos. Chem. Phys., 15, 8767–8779, https://doi.org/10.5194/acp-15-8767-2015, https://doi.org/10.5194/acp-15-8767-2015, 2015
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This study estimated the contributions to mercury concentration and deposition in easter China from seven categories of emission sources by CMAQ-Hg. Also, this study focuses on diagnostic and process analyses for atmospheric mercury pollution formation and on identification of the dominant atmospheric processes for mercury.
J. Coates and T. M. Butler
Atmos. Chem. Phys., 15, 8795–8808, https://doi.org/10.5194/acp-15-8795-2015, https://doi.org/10.5194/acp-15-8795-2015, 2015
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We show that simplified chemical mechanisms break down VOC into smaller sized degradation products on the first day faster than the near-explicit MCM chemical mechanism which would lead to an underprediction of ozone levels downwind of VOC emissions, and an underestimation of the VOC contribution to tropospheric background ozone when using simplified chemical mechanisms in regional or global modelling studies.
M. Sofiev, U. Berger, M. Prank, J. Vira, J. Arteta, J. Belmonte, K.-C. Bergmann, F. Chéroux, H. Elbern, E. Friese, C. Galan, R. Gehrig, D. Khvorostyanov, R. Kranenburg, U. Kumar, V. Marécal, F. Meleux, L. Menut, A.-M. Pessi, L. Robertson, O. Ritenberga, V. Rodinkova, A. Saarto, A. Segers, E. Severova, I. Sauliene, P. Siljamo, B. M. Steensen, E. Teinemaa, M. Thibaudon, and V.-H. Peuch
Atmos. Chem. Phys., 15, 8115–8130, https://doi.org/10.5194/acp-15-8115-2015, https://doi.org/10.5194/acp-15-8115-2015, 2015
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The paper presents the first ensemble modelling experiment for forecasting the atmospheric dispersion of birch pollen in Europe. The study included 7 models of MACC-ENS tested over the season of 2010 and applied for 2013 in forecasting and reanalysis modes. The results were compared with observations in 11 countries, members of European Aeroallergen Network. The models successfully reproduced the timing of the unusually late season of 2013 but had more difficulties with absolute concentration.
X. Fu, S. X. Wang, L. M. Ran, J. E. Pleim, E. Cooter, J. O. Bash, V. Benson, and J. M. Hao
Atmos. Chem. Phys., 15, 6637–6649, https://doi.org/10.5194/acp-15-6637-2015, https://doi.org/10.5194/acp-15-6637-2015, 2015
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In this study, we estimate, for the first time, the NH3 emission from the agricultural fertilizer application in China online using the bi-directional CMAQ model coupled to an agro-ecosystem model. Compared with previous researches, this method considers more influencing factors, such as meteorological fields, soil and the fertilizer application, and provides improved NH3 emission with higher spatial and temporal resolution.
M. Bocquet, H. Elbern, H. Eskes, M. Hirtl, R. Žabkar, G. R. Carmichael, J. Flemming, A. Inness, M. Pagowski, J. L. Pérez Camaño, P. E. Saide, R. San Jose, M. Sofiev, J. Vira, A. Baklanov, C. Carnevale, G. Grell, and C. Seigneur
Atmos. Chem. Phys., 15, 5325–5358, https://doi.org/10.5194/acp-15-5325-2015, https://doi.org/10.5194/acp-15-5325-2015, 2015
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Data assimilation is used in atmospheric chemistry models to improve air quality forecasts, construct re-analyses of concentrations, and perform inverse modeling. Coupled chemistry meteorology models (CCMM) are atmospheric chemistry models that simulate meteorological processes and chemical transformations jointly. We review here the current status of data assimilation in atmospheric chemistry models, with a particular focus on future prospects for data assimilation in CCMM.
S. Banzhaf, M. Schaap, R. Kranenburg, A. M. M. Manders, A. J. Segers, A. J. H. Visschedijk, H. A. C. Denier van der Gon, J. J. P. Kuenen, E. van Meijgaard, L. H. van Ulft, J. Cofala, and P. J. H. Builtjes
Geosci. Model Dev., 8, 1047–1070, https://doi.org/10.5194/gmd-8-1047-2015, https://doi.org/10.5194/gmd-8-1047-2015, 2015
J. Xing, R. Mathur, J. Pleim, C. Hogrefe, C.-M. Gan, D. C. Wong, C. Wei, R. Gilliam, and G. Pouliot
Atmos. Chem. Phys., 15, 2723–2747, https://doi.org/10.5194/acp-15-2723-2015, https://doi.org/10.5194/acp-15-2723-2015, 2015
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Model-simulated air quality trends over the past 2 decades largely agree with those derived from observations. In the relative amounts of VOC and NOx emission controls in different regions across the northern hemisphere have led to significantly different trends in tropospheric O3. Differences in the historical changes in the relative amounts of NH3, NOx and SO2 emissions also impact the trends in inorganic particulate matter amounts and composition in China, the U.S. and Europe.
E. Solazzo and S. Galmarini
Atmos. Chem. Phys., 15, 2535–2544, https://doi.org/10.5194/acp-15-2535-2015, https://doi.org/10.5194/acp-15-2535-2015, 2015
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Ensembles of results from multiple models require systematic screening according to well-defined and analytical principles described in the paper. The screening guarantees more robust conclusions especially in the case of scenario analysis.
J. Lee-Taylor, A. Hodzic, S. Madronich, B. Aumont, M. Camredon, and R. Valorso
Atmos. Chem. Phys., 15, 595–615, https://doi.org/10.5194/acp-15-595-2015, https://doi.org/10.5194/acp-15-595-2015, 2015
C. Knote, A. Hodzic, and J. L. Jimenez
Atmos. Chem. Phys., 15, 1–18, https://doi.org/10.5194/acp-15-1-2015, https://doi.org/10.5194/acp-15-1-2015, 2015
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Organic material found in ambient aerosol is mostly formed through the oxidation of gaseous precursors. It is semi-volatile under atmospheric conditions, and it continuously partitions between the gas and particle phases. At the same time, it is also highly water soluble. We show that wet and especially dry deposition of semi-volatile organic compounds in the gas phase are major indirect removal pathways for the particle phase, and hence need to be accurately accounted for in modeling studies.
I. Kioutsioukis and S. Galmarini
Atmos. Chem. Phys., 14, 11791–11815, https://doi.org/10.5194/acp-14-11791-2014, https://doi.org/10.5194/acp-14-11791-2014, 2014
S. Yu, R. Mathur, J. Pleim, D. Wong, R. Gilliam, K. Alapaty, C. Zhao, and X. Liu
Atmos. Chem. Phys., 14, 11247–11285, https://doi.org/10.5194/acp-14-11247-2014, https://doi.org/10.5194/acp-14-11247-2014, 2014
Y. Y. Cui, A. Hodzic, J. N. Smith, J. Ortega, J. Brioude, H. Matsui, E. J. T. Levin, A. Turnipseed, P. Winkler, and B. de Foy
Atmos. Chem. Phys., 14, 11011–11029, https://doi.org/10.5194/acp-14-11011-2014, https://doi.org/10.5194/acp-14-11011-2014, 2014
K. Tsigaridis, N. Daskalakis, M. Kanakidou, P. J. Adams, P. Artaxo, R. Bahadur, Y. Balkanski, S. E. Bauer, N. Bellouin, A. Benedetti, T. Bergman, T. K. Berntsen, J. P. Beukes, H. Bian, K. S. Carslaw, M. Chin, G. Curci, T. Diehl, R. C. Easter, S. J. Ghan, S. L. Gong, A. Hodzic, C. R. Hoyle, T. Iversen, S. Jathar, J. L. Jimenez, J. W. Kaiser, A. Kirkevåg, D. Koch, H. Kokkola, Y. H Lee, G. Lin, X. Liu, G. Luo, X. Ma, G. W. Mann, N. Mihalopoulos, J.-J. Morcrette, J.-F. Müller, G. Myhre, S. Myriokefalitakis, N. L. Ng, D. O'Donnell, J. E. Penner, L. Pozzoli, K. J. Pringle, L. M. Russell, M. Schulz, J. Sciare, Ø. Seland, D. T. Shindell, S. Sillman, R. B. Skeie, D. Spracklen, T. Stavrakou, S. D. Steenrod, T. Takemura, P. Tiitta, S. Tilmes, H. Tost, T. van Noije, P. G. van Zyl, K. von Salzen, F. Yu, Z. Wang, Z. Wang, R. A. Zaveri, H. Zhang, K. Zhang, Q. Zhang, and X. Zhang
Atmos. Chem. Phys., 14, 10845–10895, https://doi.org/10.5194/acp-14-10845-2014, https://doi.org/10.5194/acp-14-10845-2014, 2014
J. D. Fast, J. Allan, R. Bahreini, J. Craven, L. Emmons, R. Ferrare, P. L. Hayes, A. Hodzic, J. Holloway, C. Hostetler, J. L. Jimenez, H. Jonsson, S. Liu, Y. Liu, A. Metcalf, A. Middlebrook, J. Nowak, M. Pekour, A. Perring, L. Russell, A. Sedlacek, J. Seinfeld, A. Setyan, J. Shilling, M. Shrivastava, S. Springston, C. Song, R. Subramanian, J. W. Taylor, V. Vinoj, Q. Yang, R. A. Zaveri, and Q. Zhang
Atmos. Chem. Phys., 14, 10013–10060, https://doi.org/10.5194/acp-14-10013-2014, https://doi.org/10.5194/acp-14-10013-2014, 2014
M. Gordon, A. Vlasenko, R. M. Staebler, C. Stroud, P. A. Makar, J. Liggio, S.-M. Li, and S. Brown
Atmos. Chem. Phys., 14, 9087–9097, https://doi.org/10.5194/acp-14-9087-2014, https://doi.org/10.5194/acp-14-9087-2014, 2014
J. Ortega, A. Turnipseed, A. B. Guenther, T. G. Karl, D. A. Day, D. Gochis, J. A. Huffman, A. J. Prenni, E. J. T. Levin, S. M. Kreidenweis, P. J. DeMott, Y. Tobo, E. G. Patton, A. Hodzic, Y. Y. Cui, P. C. Harley, R. S. Hornbrook, E. C. Apel, R. K. Monson, A. S. D. Eller, J. P. Greenberg, M. C. Barth, P. Campuzano-Jost, B. B. Palm, J. L. Jimenez, A. C. Aiken, M. K. Dubey, C. Geron, J. Offenberg, M. G. Ryan, P. J. Fornwalt, S. C. Pryor, F. N. Keutsch, J. P. DiGangi, A. W. H. Chan, A. H. Goldstein, G. M. Wolfe, S. Kim, L. Kaser, R. Schnitzhofer, A. Hansel, C. A. Cantrell, R. L. Mauldin, and J. N. Smith
Atmos. Chem. Phys., 14, 6345–6367, https://doi.org/10.5194/acp-14-6345-2014, https://doi.org/10.5194/acp-14-6345-2014, 2014
C. Knote, A. Hodzic, J. L. Jimenez, R. Volkamer, J. J. Orlando, S. Baidar, J. Brioude, J. Fast, D. R. Gentner, A. H. Goldstein, P. L. Hayes, W. B. Knighton, H. Oetjen, A. Setyan, H. Stark, R. Thalman, G. Tyndall, R. Washenfelder, E. Waxman, and Q. Zhang
Atmos. Chem. Phys., 14, 6213–6239, https://doi.org/10.5194/acp-14-6213-2014, https://doi.org/10.5194/acp-14-6213-2014, 2014
P. A. Makar, R. Nissen, A. Teakles, J. Zhang, Q. Zheng, M. D. Moran, H. Yau, and C. diCenzo
Geosci. Model Dev., 7, 1001–1024, https://doi.org/10.5194/gmd-7-1001-2014, https://doi.org/10.5194/gmd-7-1001-2014, 2014
E. Galarneau, P. A. Makar, Q. Zheng, J. Narayan, J. Zhang, M. D. Moran, M. A. Bari, S. Pathela, A. Chen, and R. Chlumsky
Atmos. Chem. Phys., 14, 4065–4077, https://doi.org/10.5194/acp-14-4065-2014, https://doi.org/10.5194/acp-14-4065-2014, 2014
C. A. McLinden, V. Fioletov, K. F. Boersma, S. K. Kharol, N. Krotkov, L. Lamsal, P. A. Makar, R. V. Martin, J. P. Veefkind, and K. Yang
Atmos. Chem. Phys., 14, 3637–3656, https://doi.org/10.5194/acp-14-3637-2014, https://doi.org/10.5194/acp-14-3637-2014, 2014
C. Liu, S. Beirle, T. Butler, P. Hoor, C. Frankenberg, P. Jöckel, M. Penning de Vries, U. Platt, A. Pozzer, M. G. Lawrence, J. Lelieveld, H. Tost, and T. Wagner
Atmos. Chem. Phys., 14, 1717–1732, https://doi.org/10.5194/acp-14-1717-2014, https://doi.org/10.5194/acp-14-1717-2014, 2014
C.-M. Gan, J. Pleim, R. Mathur, C. Hogrefe, C. N. Long, J. Xing, S. Roselle, and C. Wei
Atmos. Chem. Phys., 14, 1701–1715, https://doi.org/10.5194/acp-14-1701-2014, https://doi.org/10.5194/acp-14-1701-2014, 2014
A. Baklanov, K. Schlünzen, P. Suppan, J. Baldasano, D. Brunner, S. Aksoyoglu, G. Carmichael, J. Douros, J. Flemming, R. Forkel, S. Galmarini, M. Gauss, G. Grell, M. Hirtl, S. Joffre, O. Jorba, E. Kaas, M. Kaasik, G. Kallos, X. Kong, U. Korsholm, A. Kurganskiy, J. Kushta, U. Lohmann, A. Mahura, A. Manders-Groot, A. Maurizi, N. Moussiopoulos, S. T. Rao, N. Savage, C. Seigneur, R. S. Sokhi, E. Solazzo, S. Solomos, B. Sørensen, G. Tsegas, E. Vignati, B. Vogel, and Y. Zhang
Atmos. Chem. Phys., 14, 317–398, https://doi.org/10.5194/acp-14-317-2014, https://doi.org/10.5194/acp-14-317-2014, 2014
S. Barthel, I. Tegen, R. Wolke, and M. van Pinxteren
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-377-2014, https://doi.org/10.5194/acpd-14-377-2014, 2014
Revised manuscript not accepted
Z. S. Stock, M. R. Russo, T. M. Butler, A. T. Archibald, M. G. Lawrence, P. J. Telford, N. L. Abraham, and J. A. Pyle
Atmos. Chem. Phys., 13, 12215–12231, https://doi.org/10.5194/acp-13-12215-2013, https://doi.org/10.5194/acp-13-12215-2013, 2013
J. R. Brook, P. A. Makar, D. M. L. Sills, K. L. Hayden, and R. McLaren
Atmos. Chem. Phys., 13, 10461–10482, https://doi.org/10.5194/acp-13-10461-2013, https://doi.org/10.5194/acp-13-10461-2013, 2013
U. S. Nair, Y. Wu, C. D. Holmes, A. Ter Schure, G. Kallos, and J. T. Walters
Atmos. Chem. Phys., 13, 10143–10157, https://doi.org/10.5194/acp-13-10143-2013, https://doi.org/10.5194/acp-13-10143-2013, 2013
J. L. Fry, D. C. Draper, K. J. Zarzana, P. Campuzano-Jost, D. A. Day, J. L. Jimenez, S. S. Brown, R. C. Cohen, L. Kaser, A. Hansel, L. Cappellin, T. Karl, A. Hodzic Roux, A. Turnipseed, C. Cantrell, B. L. Lefer, and N. Grossberg
Atmos. Chem. Phys., 13, 8585–8605, https://doi.org/10.5194/acp-13-8585-2013, https://doi.org/10.5194/acp-13-8585-2013, 2013
E. Solazzo, A. Riccio, I. Kioutsioukis, and S. Galmarini
Atmos. Chem. Phys., 13, 8315–8333, https://doi.org/10.5194/acp-13-8315-2013, https://doi.org/10.5194/acp-13-8315-2013, 2013
J. Xing, J. Pleim, R. Mathur, G. Pouliot, C. Hogrefe, C.-M. Gan, and C. Wei
Atmos. Chem. Phys., 13, 7531–7549, https://doi.org/10.5194/acp-13-7531-2013, https://doi.org/10.5194/acp-13-7531-2013, 2013
S. Galmarini, I. Kioutsioukis, and E. Solazzo
Atmos. Chem. Phys., 13, 7153–7182, https://doi.org/10.5194/acp-13-7153-2013, https://doi.org/10.5194/acp-13-7153-2013, 2013
L. Menut, B. Bessagnet, D. Khvorostyanov, M. Beekmann, N. Blond, A. Colette, I. Coll, G. Curci, G. Foret, A. Hodzic, S. Mailler, F. Meleux, J.-L. Monge, I. Pison, G. Siour, S. Turquety, M. Valari, R. Vautard, and M. G. Vivanco
Geosci. Model Dev., 6, 981–1028, https://doi.org/10.5194/gmd-6-981-2013, https://doi.org/10.5194/gmd-6-981-2013, 2013
Q. J. Zhang, M. Beekmann, F. Drewnick, F. Freutel, J. Schneider, M. Crippa, A. S. H. Prevot, U. Baltensperger, L. Poulain, A. Wiedensohler, J. Sciare, V. Gros, A. Borbon, A. Colomb, V. Michoud, J.-F. Doussin, H. A. C. Denier van der Gon, M. Haeffelin, J.-C. Dupont, G. Siour, H. Petetin, B. Bessagnet, S. N. Pandis, A. Hodzic, O. Sanchez, C. Honoré, and O. Perrussel
Atmos. Chem. Phys., 13, 5767–5790, https://doi.org/10.5194/acp-13-5767-2013, https://doi.org/10.5194/acp-13-5767-2013, 2013
E. Solazzo, R. Bianconi, G. Pirovano, M. D. Moran, R. Vautard, C. Hogrefe, K. W. Appel, V. Matthias, P. Grossi, B. Bessagnet, J. Brandt, C. Chemel, J. H. Christensen, R. Forkel, X. V. Francis, A. B. Hansen, S. McKeen, U. Nopmongcol, M. Prank, K. N. Sartelet, A. Segers, J. D. Silver, G. Yarwood, J. Werhahn, J. Zhang, S. T. Rao, and S. Galmarini
Geosci. Model Dev., 6, 791–818, https://doi.org/10.5194/gmd-6-791-2013, https://doi.org/10.5194/gmd-6-791-2013, 2013
S. M. Burrows, P. J. Rayner, T. Butler, and M. G. Lawrence
Atmos. Chem. Phys., 13, 5473–5488, https://doi.org/10.5194/acp-13-5473-2013, https://doi.org/10.5194/acp-13-5473-2013, 2013
R. Kranenburg, A. J. Segers, C. Hendriks, and M. Schaap
Geosci. Model Dev., 6, 721–733, https://doi.org/10.5194/gmd-6-721-2013, https://doi.org/10.5194/gmd-6-721-2013, 2013
J. O. Bash, E. J. Cooter, R. L. Dennis, J. T. Walker, and J. E. Pleim
Biogeosciences, 10, 1635–1645, https://doi.org/10.5194/bg-10-1635-2013, https://doi.org/10.5194/bg-10-1635-2013, 2013
J. T. Walker, M. R. Jones, J. O. Bash, L. Myles, T. Meyers, D. Schwede, J. Herrick, E. Nemitz, and W. Robarge
Biogeosciences, 10, 981–998, https://doi.org/10.5194/bg-10-981-2013, https://doi.org/10.5194/bg-10-981-2013, 2013
C. R. Lonsdale, R. G. Stevens, C. A. Brock, P. A. Makar, E. M. Knipping, and J. R. Pierce
Atmos. Chem. Phys., 12, 11519–11531, https://doi.org/10.5194/acp-12-11519-2012, https://doi.org/10.5194/acp-12-11519-2012, 2012
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
On the uncertainty of anthropogenic aromatic volatile organic compound emissions: model evaluation and sensitivity analysis
A mechanism of stratospheric O3 intrusion into the atmospheric environment: a case study of the North China Plain
Influence of atmospheric circulation on the interannual variability of transport from global and regional emissions into the Arctic
Surface networks in the Arctic may miss a future methane bomb
Potential of using CO2 observations over India in a regional carbon budget estimation by improving the modelling system
A bottom-up emission estimate for the 2022 Nord Stream gas leak: derivation, simulations, and evaluation
European CH4 inversions with ICON-ART coupled to the CarbonTracker Data Assimilation Shell
Spatiotemporal Source Apportionment of Ozone Pollution over the Greater Bay Area
Extreme weather exacerbates ozone pollution in the Pearl River Delta, China: role of natural processes
Multidecadal ozone trends in China and implications for human health and crop yields: a hybrid approach combining a chemical transport model and machine learning
On the influence of vertical mixing, boundary layer schemes, and temporal emission profiles on tropospheric NO2 in WRF-Chem – comparisons to in situ, satellite, and MAX-DOAS observations
Decreasing trends of ammonia emissions over Europe seen from remote sensing and inverse modelling
The sensitivity of Southern Ocean atmospheric dimethyl sulfide (DMS) to modeled oceanic DMS concentrations and emissions
Impacts of maritime shipping on air pollution along the US East Coast
Understanding greenhouse gas (GHG) column concentrations in Munich using the Weather Research and Forecasting (WRF) model
Impact of transport model resolution and a priori assumptions on inverse modeling of Swiss F-gas emissions
Estimation of power plant SO2 emissions using the HYSPLIT dispersion model and airborne observations with plume rise ensemble runs
Can we use atmospheric CO2 measurements to verify emission trends reported by cities? Lessons from a 6-year atmospheric inversion over Paris
A new steady-state gas–particle partitioning model of polycyclic aromatic hydrocarbons: implication for the influence of the particulate proportion in emissions
An analysis of CMAQ gas-phase dry deposition over North America through grid-scale and land-use-specific diagnostics in the context of AQMEII4
Rethinking the role of transport and photochemistry in regional ozone pollution: insights from ozone concentration and mass budgets
Decreasing seasonal cycle amplitude of methane in the northern high latitudes being driven by lower-latitude changes in emissions and transport
Potential of 14C-based versus ∆CO-based ∆ffCO2 observations to estimate urban fossil fuel CO2 (ffCO2) emissions
The effect of anthropogenic emission, meteorological factors, and carbon dioxide on the surface ozone increase in China from 2008 to 2018 during the East Asia summer monsoon season
Development of a CMAQ–PMF-based composite index for prescribing an effective ozone abatement strategy: a case study of sensitivity of surface ozone to precursor volatile organic compound species in southern Taiwan
Comment on “Climate consequences of hydrogen emissions” by Ocko and Hamburg (2022)
Constraining emissions of volatile organic compounds from western US wildfires with WE-CAN and FIREX-AQ airborne observations
Satellite quantification of methane emissions and oil–gas methane intensities from individual countries in the Middle East and North Africa: implications for climate action
Coupled mesoscale–microscale modeling of air quality in a polluted city using WRF-LES-Chem
Impact of aerosol optics on vertical distribution of ozone in autumn over Yangtze River Delta
A view of the European carbon flux landscape through the lens of the ICOS atmospheric observation network
Technical note: The CAMS greenhouse gas reanalysis from 2003 to 2020
Evaluation of simulated CO2 power plant plumes from six high-resolution atmospheric transport models
Impacts of urbanization on air quality and the related health risks in a city with complex terrain
Optimizing 4 years of CO2 biospheric fluxes from OCO-2 and in situ data in TM5: fire emissions from GFED and inferred from MOPITT CO data
Development and application of a multi-scale modeling framework for urban high-resolution NO2 pollution mapping
Towards monitoring the CO2 source–sink distribution over India via inverse modelling: quantifying the fine-scale spatiotemporal variability in the atmospheric CO2 mole fraction
Methane emissions from China: a high-resolution inversion of TROPOMI satellite observations
Estimated regional CO2 flux and uncertainty based on an ensemble of atmospheric CO2 inversions
Assessing the representativity of NH3 measurements influenced by boundary-layer dynamics and the turbulent dispersion of a nearby emission source
Analysis of CO2, CH4, and CO surface and column concentrations observed at Réunion Island by assessing WRF-Chem simulations
Technical note: Interpretation of field observations of point-source methane plume using observation-driven large-eddy simulations
Quantifying fossil fuel methane emissions using observations of atmospheric ethane and an uncertain emission ratio
The impact of peripheral circulation characteristics of typhoon on sustained ozone episodes over the Pearl River Delta region, China
Updated Global Fuel Exploitation Inventory (GFEI) for methane emissions from the oil, gas, and coal sectors: evaluation with inversions of atmospheric methane observations
High-resolution mapping of regional traffic emissions using land-use machine learning models
Land use and anthropogenic heat modulate ozone by meteorology: a perspective from the Yangtze River Delta region
Four years of global carbon cycle observed from the Orbiting Carbon Observatory 2 (OCO-2) version 9 and in situ data and comparison to OCO-2 version 7
Data assimilation of CrIS NH3 satellite observations for improving spatiotemporal NH3 distributions in LOTOS-EUROS
On the cross-tropopause transport of water by tropical convective overshoots: a mesoscale modelling study constrained by in situ observations during the TRO-Pico field campaign in Brazil
Kevin Oliveira, Marc Guevara, Oriol Jorba, Hervé Petetin, Dene Bowdalo, Carles Tena, Gilbert Montané Pinto, Franco López, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 7137–7177, https://doi.org/10.5194/acp-24-7137-2024, https://doi.org/10.5194/acp-24-7137-2024, 2024
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In this work, we assess and evaluate benzene, toluene, and xylene primary emissions and air quality levels in Spain by combining observations, emission inventories, and air quality modelling techniques. The comparison between modelled and observed levels allows identifying uncertainty sources within the emission input. This contributes to improving air quality models' performance when simulating these compounds, leading to better support for the design of effective pollution control strategies.
Yuehan Luo, Tianliang Zhao, Kai Meng, Jun Hu, Qingjian Yang, Yongqing Bai, Kai Yang, Weikang Fu, Chenghao Tan, Yifan Zhang, Yanzhe Zhang, and Zhikuan Li
Atmos. Chem. Phys., 24, 7013–7026, https://doi.org/10.5194/acp-24-7013-2024, https://doi.org/10.5194/acp-24-7013-2024, 2024
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We reveal a significant mechanism of stratospheric O3 intrusion (SI) into the atmospheric environment induced by an extratropical cyclone system. This system facilitates the downward transport of stratospheric O3 to the near-surface layer by vertical coupling, involving the upper westerly trough, the middle northeast cold vortex, and the lower extratropical cyclone in the troposphere. On average, stratospheric O3 contributed 26.77 % to near-surface O3 levels over the North China Plain.
Cheng Zheng, Yutian Wu, Mingfang Ting, and Clara Orbe
Atmos. Chem. Phys., 24, 6965–6985, https://doi.org/10.5194/acp-24-6965-2024, https://doi.org/10.5194/acp-24-6965-2024, 2024
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Trace gases and aerosols in the Arctic, which typically originate from midlatitude and tropical emission regions, modulate the Arctic climate via their radiative and chemistry impacts. Thus, long-range transport of these substances is important for understanding the current and the future change of Arctic climate. By employing chemistry–climate models, we explore how year-to-year variations in the atmospheric circulation modulate atmospheric long-range transport into the Arctic.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, and Jean-Daniel Paris
Atmos. Chem. Phys., 24, 6359–6373, https://doi.org/10.5194/acp-24-6359-2024, https://doi.org/10.5194/acp-24-6359-2024, 2024
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The aim of this work is to analyse how accurately a methane bomb event could be detected with the current and a hypothetically extended stationary observation network in the Arctic. For this, we incorporate synthetically modelled possible future CH4 concentrations based on plausible emission scenarios into an inverse modelling framework. We analyse how well the increase is detected in different Arctic regions and evaluate the impact of additional observation sites in this respect.
Vishnu Thilakan, Dhanyalekshmi Pillai, Jithin Sukumaran, Christoph Gerbig, Haseeb Hakkim, Vinayak Sinha, Yukio Terao, Manish Naja, and Monish Vijay Deshpande
Atmos. Chem. Phys., 24, 5315–5335, https://doi.org/10.5194/acp-24-5315-2024, https://doi.org/10.5194/acp-24-5315-2024, 2024
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This study investigates the usability of CO2 mixing ratio observations over India to infer regional carbon sources and sinks. We demonstrate that a high-resolution modelling system can represent the observed CO2 variations reasonably well by improving the transport and flux variations at a fine scale. Future carbon data assimilation systems can thus benefit from these recently available CO2 observations when fine-scale variations are adequately represented in the models.
Rostislav Kouznetsov, Risto Hänninen, Andreas Uppstu, Evgeny Kadantsev, Yalda Fatahi, Marje Prank, Dmitrii Kouznetsov, Steffen Manfred Noe, Heikki Junninen, and Mikhail Sofiev
Atmos. Chem. Phys., 24, 4675–4691, https://doi.org/10.5194/acp-24-4675-2024, https://doi.org/10.5194/acp-24-4675-2024, 2024
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By relying solely on publicly available media reports, we were able to infer the temporal evolution and the injection height for the Nord Stream gas leaks in September 2022. The inventory specifies locations, vertical distributions, and temporal evolution of the methane sources. The inventory can be used to simulate the event with atmospheric transport models. The inventory is supplemented with a set of observational data tailored to evaluate the results of the simulated atmospheric dispersion.
Michael Steiner, Wouter Peters, Ingrid Luijkx, Stephan Henne, Huilin Chen, Samuel Hammer, and Dominik Brunner
Atmos. Chem. Phys., 24, 2759–2782, https://doi.org/10.5194/acp-24-2759-2024, https://doi.org/10.5194/acp-24-2759-2024, 2024
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The Paris Agreement increased interest in estimating greenhouse gas (GHG) emissions of individual countries, but top-down emission estimation is not yet considered policy-relevant. It is therefore paramount to reduce large errors and to build systems that are based on the newest atmospheric transport models. In this study, we present the first application of ICON-ART in the inverse modeling of GHG fluxes with an ensemble Kalman filter and present our results for European CH4 emissions.
Yiang Chen, Xingcheng Lu, and Jimmy C. H. Fung
EGUsphere, https://doi.org/10.5194/egusphere-2023-3140, https://doi.org/10.5194/egusphere-2023-3140, 2024
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This study investigates the contribution of pollutants from different emitting periods to ozone episodes over the Greater Bay Area. The analysis reveals the variation of major spatiotemporal contributors to the O3 pollution under the influence of typhoons and sub-tropical high-pressure. Through the temporal contribution analysis, our work offers a new perspective on the evolution of O3 pollution and can aid in developing effective and timely control policies under unfavorable weather conditions.
Nan Wang, Hongyue Wang, Xin Huang, Xi Chen, Yu Zou, Tao Deng, Tingyuan Li, Xiaopu Lyu, and Fumo Yang
Atmos. Chem. Phys., 24, 1559–1570, https://doi.org/10.5194/acp-24-1559-2024, https://doi.org/10.5194/acp-24-1559-2024, 2024
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This study explores the influence of extreme-weather-induced natural processes on ozone pollution, which is often overlooked. By analyzing meteorological factors, natural emissions, chemistry pathways and atmospheric transport, we discovered that these natural processes could substantially exacerbate ozone pollution. The findings contribute to a deeper understanding of ozone pollution and offer valuable insights for controlling ozone pollution in the context of global warming.
Jia Mao, Amos P. K. Tai, David H. Y. Yung, Tiangang Yuan, Kong T. Chau, and Zhaozhong Feng
Atmos. Chem. Phys., 24, 345–366, https://doi.org/10.5194/acp-24-345-2024, https://doi.org/10.5194/acp-24-345-2024, 2024
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Surface ozone (O3) is well-known for posing great threats to both human health and agriculture worldwide. However, a multidecadal assessment of the impacts of O3 on public health and agriculture in China is lacking without sufficient O3 observations. We used a hybrid approach combining a chemical transport model and machine learning to provide a robust dataset of O3 concentrations over the past 4 decades in China, thereby filling the gap in the long-term O3 trend and impact assessment in China.
Leon Kuhn, Steffen Beirle, Vinod Kumar, Sergey Osipov, Andrea Pozzer, Tim Bösch, Rajesh Kumar, and Thomas Wagner
Atmos. Chem. Phys., 24, 185–217, https://doi.org/10.5194/acp-24-185-2024, https://doi.org/10.5194/acp-24-185-2024, 2024
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NO₂ is an important air pollutant. It was observed that the WRF-Chem model shows significant deviations in NO₂ abundance when compared to measurements. We use a 1-month simulation over central Europe to show that these deviations can be mostly resolved by reparameterization of the vertical mixing routine. In order to validate our results, they are compared to in situ, satellite, and MAX-DOAS measurements.
Ondřej Tichý, Sabine Eckhardt, Yves Balkanski, Didier Hauglustaine, and Nikolaos Evangeliou
Atmos. Chem. Phys., 23, 15235–15252, https://doi.org/10.5194/acp-23-15235-2023, https://doi.org/10.5194/acp-23-15235-2023, 2023
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We show declining trends in NH3 emissions over Europe for 2013–2020 using advanced dispersion and inverse modelling and satellite measurements from CrIS. Emissions decreased by −26% since 2013, showing that the abatement strategies adopted by the European Union have been very efficient. Ammonia emissions are low in winter and peak in summer due to temperature-dependent soil volatilization. The largest decreases were observed in central and western Europe in countries with high emissions.
Yusuf A. Bhatti, Laura E. Revell, Alex J. Schuddeboom, Adrian J. McDonald, Alex T. Archibald, Jonny Williams, Abhijith U. Venugopal, Catherine Hardacre, and Erik Behrens
Atmos. Chem. Phys., 23, 15181–15196, https://doi.org/10.5194/acp-23-15181-2023, https://doi.org/10.5194/acp-23-15181-2023, 2023
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Aerosols are a large source of uncertainty over the Southern Ocean. A dominant source of sulfate aerosol in this region is dimethyl sulfide (DMS), which is poorly simulated by climate models. We show the sensitivity of simulated atmospheric DMS to the choice of oceanic DMS data set and emission scheme. We show that oceanic DMS has twice the influence on atmospheric DMS than the emission scheme. Simulating DMS more accurately in climate models will help to constrain aerosol uncertainty.
Maryam Golbazi and Cristina Archer
Atmos. Chem. Phys., 23, 15057–15075, https://doi.org/10.5194/acp-23-15057-2023, https://doi.org/10.5194/acp-23-15057-2023, 2023
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We use scientific models to study the impact of ship emissions on air quality along the US East Coast. We find an increase in three major pollutants (PM2.5, NO2, and SO2) in coastal regions. However, we detect a reduction in ozone (O3) levels in major coastal cities. This reduction is linked to the significant emissions of nitrogen oxides (NOx) from ships, which scavenged O3, especially in highly polluted urban areas experiencing an NOx-limited regime.
Xinxu Zhao, Jia Chen, Julia Marshall, Michal Gałkowski, Stephan Hachinger, Florian Dietrich, Ankit Shekhar, Johannes Gensheimer, Adrian Wenzel, and Christoph Gerbig
Atmos. Chem. Phys., 23, 14325–14347, https://doi.org/10.5194/acp-23-14325-2023, https://doi.org/10.5194/acp-23-14325-2023, 2023
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We develop a modeling framework using the Weather Research and Forecasting model at a high spatial resolution (up to 400 m) to simulate atmospheric transport of greenhouse gases and interpret column observations. Output is validated against weather stations and column measurements in August 2018. The differential column method is applied, aided by air-mass transport tracing with the Stochastic Time-Inverted Lagrangian Transport (STILT) model, also for an exploratory measurement interpretation.
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
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The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
Tianfeng Chai, Xinrong Ren, Fong Ngan, Mark Cohen, and Alice Crawford
Atmos. Chem. Phys., 23, 12907–12933, https://doi.org/10.5194/acp-23-12907-2023, https://doi.org/10.5194/acp-23-12907-2023, 2023
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The SO2 emissions of three power plants are estimated using aircraft observations and an ensemble of HYSPLIT dispersion simulations with different plume rise parameters. The emission estimates using the runs with the lowest root mean square errors (RMSEs) and the runs with the best correlation coefficients between the predicted and observed mixing ratios both agree well with the Continuous Emissions Monitoring Systems (CEMS) data. The RMSE-based plume rise appears to be more reasonable.
Jinghui Lian, Thomas Lauvaux, Hervé Utard, François-Marie Bréon, Grégoire Broquet, Michel Ramonet, Olivier Laurent, Ivonne Albarus, Mali Chariot, Simone Kotthaus, Martial Haeffelin, Olivier Sanchez, Olivier Perrussel, Hugo Anne Denier van der Gon, Stijn Nicolaas Camiel Dellaert, and Philippe Ciais
Atmos. Chem. Phys., 23, 8823–8835, https://doi.org/10.5194/acp-23-8823-2023, https://doi.org/10.5194/acp-23-8823-2023, 2023
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This study quantifies urban CO2 emissions via an atmospheric inversion for the Paris metropolitan area over a 6-year period from 2016 to 2021. Results show a long-term decreasing trend of about 2 % ± 0.6 % per year in the annual CO2 emissions over Paris. We conclude that our current capacity can deliver near-real-time CO2 emission estimates at the city scale in under a month, and the results agree within 10 % with independent estimates from multiple city-scale inventories.
Fu-Jie Zhu, Peng-Tuan Hu, and Wan-Li Ma
Atmos. Chem. Phys., 23, 8583–8590, https://doi.org/10.5194/acp-23-8583-2023, https://doi.org/10.5194/acp-23-8583-2023, 2023
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A new steady-state gas–particle partitioning model of polycyclic aromatic hydrocarbons was established based on the level-III multimedia fugacity model, which proved that the particulate proportion of PAHs in emissions was a crucial factor for G–P partitioning of PAHs. In addition, gaseous and particulate interference was also derived in the new steady-state model determined by the particulate proportion in emission that could derivate the G–P partitioning quotients from the equilibrium state.
Christian Hogrefe, Jesse O. Bash, Jonathan E. Pleim, Donna B. Schwede, Robert C. Gilliam, Kristen M. Foley, K. Wyat Appel, and Rohit Mathur
Atmos. Chem. Phys., 23, 8119–8147, https://doi.org/10.5194/acp-23-8119-2023, https://doi.org/10.5194/acp-23-8119-2023, 2023
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Under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in the widely used CMAQ model. The results illustrate how these tools can provide insights into similarities and differences between the two CMAQ dry deposition options that affect simulated pollutant budgets and ecosystem impacts from atmospheric pollution.
Kun Qu, Xuesong Wang, Xuhui Cai, Yu Yan, Xipeng Jin, Mihalis Vrekoussis, Maria Kanakidou, Guy P. Brasseur, Jin Shen, Teng Xiao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 7653–7671, https://doi.org/10.5194/acp-23-7653-2023, https://doi.org/10.5194/acp-23-7653-2023, 2023
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Basic understandings of ozone processes, especially transport and chemistry, are essential to support ozone pollution control, but studies often have different views on their relative importance. We developed a method to quantify their contributions in the ozone mass and concentration budgets based on the WRF-CMAQ model. Results in a polluted region highlight the differences between two budgets. For future studies, two budgets are both needed to fully understand the effects of ozone processes.
Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
Atmos. Chem. Phys., 23, 7363–7382, https://doi.org/10.5194/acp-23-7363-2023, https://doi.org/10.5194/acp-23-7363-2023, 2023
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Surface observations of methane show that the seasonal cycle amplitude (SCA) of methane is decreasing in the northern high latitudes (NHLs) but increased globally (1995–2020). The NHL decrease is counterintuitive, as we expect the SCA to increase with increasing concentrations. We use a chemical transport model to investigate changes in SCA in the NHLs. We find well-mixed methane and changes in emissions from Canada, the Middle East, and Europe are the largest contributors to the SCA in NHLs.
Fabian Manuel Maier, Christian Rödenbeck, Ingeborg Levin, Christoph Gerbig, Maksym Gachkivskyi, and Samuel Hammer
EGUsphere, https://doi.org/10.5194/egusphere-2023-1239, https://doi.org/10.5194/egusphere-2023-1239, 2023
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We investigate the usage of discrete radiocarbon (14C)-based fossil fuel carbon dioxide (ffCO2) concentration estimates versus continuous carbon monoxide (CO)-based ffCO2 estimates to evaluate the seasonal cycle of the ffCO2 emissions in an urban region with an inverse modelling framework. We find that the CO-based ffCO2 estimates allow to reconstruct robust seasonal cycles, which show the distinct Covid-19 drawdown in 2020 and can be used to validate emission inventories.
Danyang Ma, Tijian Wang, Hao Wu, Yawei Qu, Jian Liu, Jane Liu, Shu Li, Bingliang Zhuang, Mengmeng Li, and Min Xie
Atmos. Chem. Phys., 23, 6525–6544, https://doi.org/10.5194/acp-23-6525-2023, https://doi.org/10.5194/acp-23-6525-2023, 2023
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Increasing surface ozone (O3) concentrations have long been a significant environmental issue in China, despite the Clean Air Action Plan launched in 2013. Most previous research ignores the contributions of CO2 variations. Our study comprehensively analyzed O3 variation across China from various perspectives and highlighted the importance of considering CO2 variations when designing long-term O3 control policies, especially in high-vegetation-coverage areas.
Jackson Hian-Wui Chang, Stephen M. Griffith, Steven Soon-Kai Kong, Ming-Tung Chuang, and Neng-Huei Lin
Atmos. Chem. Phys., 23, 6357–6382, https://doi.org/10.5194/acp-23-6357-2023, https://doi.org/10.5194/acp-23-6357-2023, 2023
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A novel CMAQ–PMF-based composite index is developed to identify the key VOC source species for an effective ozone abatement strategy. The index provides information as to which VOC species are key to ozone formation and where to reduce sources of these VOC species. Using the composite index, we recommended the VOC control measures in southern Taiwan should prioritize solvent usage, vehicle emissions, and the petrochemical industry.
Lei Duan and Ken Caldeira
Atmos. Chem. Phys., 23, 6011–6020, https://doi.org/10.5194/acp-23-6011-2023, https://doi.org/10.5194/acp-23-6011-2023, 2023
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Ocko and Hamburg (2022) emphasize the short-term climate impact of hydrogen, and we present an analysis that places greater focus on long-term outcomes. We have derived equations that describe the time-evolving impact of hydrogen and show that higher methane leakage is primarily responsible for the warming potential of blue hydrogen, while hydrogen leakage plays a less critical role. Fossil fuels show more prominent longer-term climate impacts than clean hydrogen under all emission scenarios.
Lixu Jin, Wade Permar, Vanessa Selimovic, Damien Ketcherside, Robert J. Yokelson, Rebecca S. Hornbrook, Eric C. Apel, I-Ting Ku, Jeffrey L. Collett Jr., Amy P. Sullivan, Daniel A. Jaffe, Jeffrey R. Pierce, Alan Fried, Matthew M. Coggon, Georgios I. Gkatzelis, Carsten Warneke, Emily V. Fischer, and Lu Hu
Atmos. Chem. Phys., 23, 5969–5991, https://doi.org/10.5194/acp-23-5969-2023, https://doi.org/10.5194/acp-23-5969-2023, 2023
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Air quality in the USA has been improving since 1970 due to anthropogenic emission reduction. Those gains have been partly offset by increased wildfire pollution in the western USA in the past 20 years. Still, we do not understand wildfire emissions well due to limited measurements. Here, we used a global transport model to evaluate and constrain current knowledge of wildfire emissions with recent observational constraints, showing the underestimation of wildfire emissions in the western USA.
Zichong Chen, Daniel J. Jacob, Ritesh Gautam, Mark Omara, Robert N. Stavins, Robert C. Stowe, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Drew C. Pendergrass, and Sarah Hancock
Atmos. Chem. Phys., 23, 5945–5967, https://doi.org/10.5194/acp-23-5945-2023, https://doi.org/10.5194/acp-23-5945-2023, 2023
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We quantify methane emissions from individual countries in the Middle East and North Africa by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We show that the ability to simply relate oil/gas emissions to activity metrics is compromised by stochastic nature of local infrastructure and management practices. We find that the industry target for oil/gas methane intensity is achievable through associated gas capture, modern infrastructure, and centralized operations.
Yuting Wang, Yong-Feng Ma, Domingo Muñoz-Esparza, Jianing Dai, Cathy Wing Yi Li, Pablo Lichtig, Roy Chun-Wang Tsang, Chun-Ho Liu, Tao Wang, and Guy Pierre Brasseur
Atmos. Chem. Phys., 23, 5905–5927, https://doi.org/10.5194/acp-23-5905-2023, https://doi.org/10.5194/acp-23-5905-2023, 2023
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Air quality in urban areas is difficult to simulate in coarse-resolution models. This work exploits the WRF (Weather Research and Forecasting) model coupled with a large-eddy simulation (LES) component and online chemistry to perform high-resolution (33.3 m) simulations of air quality in a large city. The evaluation of the simulations with observations shows that increased model resolution improves the representation of the chemical species near the pollution sources.
Shuqi Yan, Bin Zhu, Shuangshuang Shi, Wen Lu, Jinhui Gao, Hanqing Kang, and Duanyang Liu
Atmos. Chem. Phys., 23, 5177–5190, https://doi.org/10.5194/acp-23-5177-2023, https://doi.org/10.5194/acp-23-5177-2023, 2023
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We analyze ozone response to aerosol mixing states in the vertical direction by WRF-Chem simulations. Aerosols generally lead to turbulent suppression, precursor accumulation, low-level photolysis reduction, and upper-level photolysis enhancement under different underlying surface and pollution conditions. Thus, ozone decreases within the entire boundary layer during the daytime, and the decrease is the least in aerosol external mixing states compared to internal and core shell mixing states.
Ida Storm, Ute Karstens, Claudio D'Onofrio, Alex Vermeulen, and Wouter Peters
Atmos. Chem. Phys., 23, 4993–5008, https://doi.org/10.5194/acp-23-4993-2023, https://doi.org/10.5194/acp-23-4993-2023, 2023
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In this study, we evaluate what is in the influence regions of the ICOS atmospheric measurement stations to gain insight into what land cover types and land-cover-associated fluxes the network represents. Subsequently, insights about strengths, weaknesses, and potential gaps can assist in future network expansion decisions. The network is concentrated in central Europe, which leads to a general overrepresentation of coniferous forest and cropland and underrepresentation of grass and shrubland.
Anna Agustí-Panareda, Jérôme Barré, Sébastien Massart, Antje Inness, Ilse Aben, Melanie Ades, Bianca C. Baier, Gianpaolo Balsamo, Tobias Borsdorff, Nicolas Bousserez, Souhail Boussetta, Michael Buchwitz, Luca Cantarello, Cyril Crevoisier, Richard Engelen, Henk Eskes, Johannes Flemming, Sébastien Garrigues, Otto Hasekamp, Vincent Huijnen, Luke Jones, Zak Kipling, Bavo Langerock, Joe McNorton, Nicolas Meilhac, Stefan Noël, Mark Parrington, Vincent-Henri Peuch, Michel Ramonet, Miha Razinger, Maximilian Reuter, Roberto Ribas, Martin Suttie, Colm Sweeney, Jérôme Tarniewicz, and Lianghai Wu
Atmos. Chem. Phys., 23, 3829–3859, https://doi.org/10.5194/acp-23-3829-2023, https://doi.org/10.5194/acp-23-3829-2023, 2023
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We present a global dataset of atmospheric CO2 and CH4, the two most important human-made greenhouse gases, which covers almost 2 decades (2003–2020). It is produced by combining satellite data of CO2 and CH4 with a weather and air composition prediction model, and it has been carefully evaluated against independent observations to ensure validity and point out deficiencies to the user. This dataset can be used for scientific studies in the field of climate change and the global carbon cycle.
Dominik Brunner, Gerrit Kuhlmann, Stephan Henne, Erik Koene, Bastian Kern, Sebastian Wolff, Christiane Voigt, Patrick Jöckel, Christoph Kiemle, Anke Roiger, Alina Fiehn, Sven Krautwurst, Konstantin Gerilowski, Heinrich Bovensmann, Jakob Borchardt, Michal Galkowski, Christoph Gerbig, Julia Marshall, Andrzej Klonecki, Pascal Prunet, Robert Hanfland, Margit Pattantyús-Ábrahám, Andrzej Wyszogrodzki, and Andreas Fix
Atmos. Chem. Phys., 23, 2699–2728, https://doi.org/10.5194/acp-23-2699-2023, https://doi.org/10.5194/acp-23-2699-2023, 2023
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We evaluated six atmospheric transport models for their capability to simulate the CO2 plumes from two of the largest power plants in Europe by comparing the models against aircraft observations collected during the CoMet (Carbon Dioxide and Methane Mission) campaign in 2018. The study analyzed how realistically such plumes can be simulated at different model resolutions and how well the planned European satellite mission CO2M will be able to quantify emissions from power plants.
Chenchao Zhan, Min Xie, Hua Lu, Bojun Liu, Zheng Wu, Tijian Wang, Bingliang Zhuang, Mengmeng Li, and Shu Li
Atmos. Chem. Phys., 23, 771–788, https://doi.org/10.5194/acp-23-771-2023, https://doi.org/10.5194/acp-23-771-2023, 2023
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With the development of urbanization, urban land use and anthropogenic
emissions increase, affecting urban air quality and, in turn, the health risks associated with air pollutants. In this study, we systematically evaluate the impacts of urbanization on air quality and the corresponding health risks in a highly urbanized city with severe air pollution and complex terrain. This work focuses on the health risks caused by urbanization and can provide valuable insight for air pollution strategies.
Hélène Peiro, Sean Crowell, and Berrien Moore III
Atmos. Chem. Phys., 22, 15817–15849, https://doi.org/10.5194/acp-22-15817-2022, https://doi.org/10.5194/acp-22-15817-2022, 2022
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CO data can provide a powerful constraint on fire fluxes, supporting more accurate estimation of biospheric CO2 fluxes. We converted CO fire flux into CO2 fire prior, which is then used to adjust CO2 respiration. We applied this to two other fire flux products. CO2 inversions constrained by satellites or in situ data are then performed. Results show larger variations among the data assimilated than across the priors, but tropical flux from in situ inversions is sensitive to priors.
Zhaofeng Lv, Zhenyu Luo, Fanyuan Deng, Xiaotong Wang, Junchao Zhao, Lucheng Xu, Tingkun He, Yingzhi Zhang, Huan Liu, and Kebin He
Atmos. Chem. Phys., 22, 15685–15702, https://doi.org/10.5194/acp-22-15685-2022, https://doi.org/10.5194/acp-22-15685-2022, 2022
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This study developed a hybrid model, CMAQ-RLINE_URBAN, to predict the urban NO2 concentrations at a high spatial resolution. To estimate the influence of various street canyons on the dispersion of air pollutants, a new parameterization scheme was established based on computational fluid dynamics and machine learning methods. This work created a new method to identify the characteristics of vehicle-related air pollution at both city and street scales simultaneously and accurately.
Vishnu Thilakan, Dhanyalekshmi Pillai, Christoph Gerbig, Michal Galkowski, Aparnna Ravi, and Thara Anna Mathew
Atmos. Chem. Phys., 22, 15287–15312, https://doi.org/10.5194/acp-22-15287-2022, https://doi.org/10.5194/acp-22-15287-2022, 2022
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This paper demonstrates how we can use atmospheric observations to improve the CO2 flux estimates in India. This is achieved by improving the representation of terrain, mesoscale transport, and flux variations. We quantify the impact of the unresolved variations in the current models on optimally estimated fluxes via inverse modelling and quantify the associated flux uncertainty. We illustrate how a parameterization scheme captures this variability in the coarse models.
Zichong Chen, Daniel J. Jacob, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Elise Penn, and Xueying Yu
Atmos. Chem. Phys., 22, 10809–10826, https://doi.org/10.5194/acp-22-10809-2022, https://doi.org/10.5194/acp-22-10809-2022, 2022
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We quantify methane emissions in China and contributions from different sectors by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We find that anthropogenic methane emissions for China are underestimated in the national inventory. Our estimate of emissions indicates a small life-cycle loss rate, implying net climate benefits from the current
coal-to-gasenergy transition in China. However, this small loss rate can be misleading given China's high gas imports.
Naveen Chandra, Prabir K. Patra, Yousuke Niwa, Akihiko Ito, Yosuke Iida, Daisuke Goto, Shinji Morimoto, Masayuki Kondo, Masayuki Takigawa, Tomohiro Hajima, and Michio Watanabe
Atmos. Chem. Phys., 22, 9215–9243, https://doi.org/10.5194/acp-22-9215-2022, https://doi.org/10.5194/acp-22-9215-2022, 2022
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This paper is intended to accomplish two goals: (1) quantify mean and uncertainty in non-fossil-fuel CO2 fluxes estimated by inverse modeling and (2) provide in-depth analyses of regional CO2 fluxes in support of emission mitigation policymaking. CO2 flux variability and trends are discussed concerning natural climate variability and human disturbances using multiple lines of evidence.
Ruben B. Schulte, Margreet C. van Zanten, Bart J. H. van Stratum, and Jordi Vilà-Guerau de Arellano
Atmos. Chem. Phys., 22, 8241–8257, https://doi.org/10.5194/acp-22-8241-2022, https://doi.org/10.5194/acp-22-8241-2022, 2022
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We present a fine-scale simulation framework, utilizing large-eddy simulations, to assess NH3 measurements influenced by boundary-layer dynamics and turbulent dispersion of a nearby emission source. The minimum required distance from an emission source differs for concentration and flux measurements, from 0.5–3.0 km and 0.75–4.5 km, respectively. The simulation framework presented here proves to be a powerful and versatile tool for future NH3 research at high spatio-temporal resolutions.
Sieglinde Callewaert, Jérôme Brioude, Bavo Langerock, Valentin Duflot, Dominique Fonteyn, Jean-François Müller, Jean-Marc Metzger, Christian Hermans, Nicolas Kumps, Michel Ramonet, Morgan Lopez, Emmanuel Mahieu, and Martine De Mazière
Atmos. Chem. Phys., 22, 7763–7792, https://doi.org/10.5194/acp-22-7763-2022, https://doi.org/10.5194/acp-22-7763-2022, 2022
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A regional atmospheric transport model is used to analyze the factors contributing to CO2, CH4, and CO observations at Réunion Island. We show that the surface observations are dominated by local fluxes and dynamical processes, while the column data are influenced by larger-scale mechanisms such as biomass burning plumes. The model is able to capture the measured time series well; however, the results are highly dependent on accurate boundary conditions and high-resolution emission inventories.
Anja Ražnjević, Chiel van Heerwaarden, Bart van Stratum, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, and Maarten Krol
Atmos. Chem. Phys., 22, 6489–6505, https://doi.org/10.5194/acp-22-6489-2022, https://doi.org/10.5194/acp-22-6489-2022, 2022
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Mobile measurement techniques (e.g., instruments placed in cars) are often employed to identify and quantify individual sources of greenhouse gases. Due to road restrictions, those observations are often sparse (temporally and spatially). We performed high-resolution simulations of plume dispersion, with realistic weather conditions encountered in the field, to reproduce the measurement process of a methane plume emitted from an oil well and provide additional information about the plume.
Alice E. Ramsden, Anita L. Ganesan, Luke M. Western, Matthew Rigby, Alistair J. Manning, Amy Foulds, James L. France, Patrick Barker, Peter Levy, Daniel Say, Adam Wisher, Tim Arnold, Chris Rennick, Kieran M. Stanley, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 22, 3911–3929, https://doi.org/10.5194/acp-22-3911-2022, https://doi.org/10.5194/acp-22-3911-2022, 2022
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Quantifying methane emissions from different sources is a key focus of current research. We present a method for estimating sectoral methane emissions that uses ethane as a tracer for fossil fuel methane. By incorporating variable ethane : methane emission ratios into this model, we produce emissions estimates with improved uncertainty characterisation. This method will be particularly useful for studying methane emissions in areas with complex distributions of sources.
Ying Li, Xiangjun Zhao, Xuejiao Deng, and Jinhui Gao
Atmos. Chem. Phys., 22, 3861–3873, https://doi.org/10.5194/acp-22-3861-2022, https://doi.org/10.5194/acp-22-3861-2022, 2022
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This study finds a new phenomenon of weak wind deepening (WWD) associated with the peripheral circulation of typhoon and gives the influence mechanism of WWD on its contribution to daily variation during sustained ozone episodes. The WWD provides the premise for pollution accumulation in the whole PBL and continued enhancement of ground-level ozone via vertical mixing processes. These findings could benefit the daily daytime ozone forecast in the PRD region and other areas.
Tia R. Scarpelli, Daniel J. Jacob, Shayna Grossman, Xiao Lu, Zhen Qu, Melissa P. Sulprizio, Yuzhong Zhang, Frances Reuland, Deborah Gordon, and John R. Worden
Atmos. Chem. Phys., 22, 3235–3249, https://doi.org/10.5194/acp-22-3235-2022, https://doi.org/10.5194/acp-22-3235-2022, 2022
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We present a spatially explicit version of the national inventories of oil, gas, and coal methane emissions as submitted by individual countries to the United Nations Framework Convention on Climate Change (UNFCCC) in 2021. We then use atmospheric modeling to compare our inventory emissions to atmospheric methane observations with the goal of identifying potential under- and overestimates of oil–gas methane emissions in the national inventories.
Xiaomeng Wu, Daoyuan Yang, Ruoxi Wu, Jiajun Gu, Yifan Wen, Shaojun Zhang, Rui Wu, Renjie Wang, Honglei Xu, K. Max Zhang, Ye Wu, and Jiming Hao
Atmos. Chem. Phys., 22, 1939–1950, https://doi.org/10.5194/acp-22-1939-2022, https://doi.org/10.5194/acp-22-1939-2022, 2022
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Our work pioneered land-use machine learning methods for developing link-level emission inventories, utilizing hourly traffic profiles, including volume, speed, and fleet mix, obtained from the governmental intercity highway monitoring network in the "capital circles" of China. This research provides a platform to realize the near-real-time process of establishing high-resolution vehicle emission inventories for policy makers to engage in sophisticated traffic management.
Chenchao Zhan and Min Xie
Atmos. Chem. Phys., 22, 1351–1371, https://doi.org/10.5194/acp-22-1351-2022, https://doi.org/10.5194/acp-22-1351-2022, 2022
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The changes of land use and anthropogenic heat (AH) derived from urbanization can affect meteorology and in turn O3 evolution. In this study, we briefly describe the general features of O3 pollution in the Yangtze River Delta (YRD) based on in situ observational data. Then, the impacts of land use and anthropogenic heat on O3 via changing the meteorological factors and local circulations are investigated in this region using the WRF-Chem model.
Hélène Peiro, Sean Crowell, Andrew Schuh, David F. Baker, Chris O'Dell, Andrew R. Jacobson, Frédéric Chevallier, Junjie Liu, Annmarie Eldering, David Crisp, Feng Deng, Brad Weir, Sourish Basu, Matthew S. Johnson, Sajeev Philip, and Ian Baker
Atmos. Chem. Phys., 22, 1097–1130, https://doi.org/10.5194/acp-22-1097-2022, https://doi.org/10.5194/acp-22-1097-2022, 2022
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Satellite CO2 observations are constantly improved. We study an ensemble of different atmospheric models (inversions) from 2015 to 2018 using separate ground-based data or two versions of the OCO-2 satellite. Our study aims to determine if different satellite data corrections can yield different estimates of carbon cycle flux. A difference in the carbon budget between the two versions is found over tropical Africa, which seems to show the impact of corrections applied in satellite data.
Shelley van der Graaf, Enrico Dammers, Arjo Segers, Richard Kranenburg, Martijn Schaap, Mark W. Shephard, and Jan Willem Erisman
Atmos. Chem. Phys., 22, 951–972, https://doi.org/10.5194/acp-22-951-2022, https://doi.org/10.5194/acp-22-951-2022, 2022
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CrIS NH3 satellite observations are assimilated into the LOTOS-EUROS model using two different methods. In the first method the data are used to fit spatially varying NH3 emission time factors. In the second method a local ensemble transform Kalman filter is used. Compared to in situ observations, combining both methods led to the most significant improvements in the modeled concentrations and deposition, illustrating the usefulness of CrIS NH3 to improve the spatiotemporal distribution of NH3.
Abhinna K. Behera, Emmanuel D. Rivière, Sergey M. Khaykin, Virginie Marécal, Mélanie Ghysels, Jérémie Burgalat, and Gerhard Held
Atmos. Chem. Phys., 22, 881–901, https://doi.org/10.5194/acp-22-881-2022, https://doi.org/10.5194/acp-22-881-2022, 2022
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Deep convection overshooting the stratosphere's contribution to the global stratospheric water budget is still being quantified. We ran three different cloud-resolving simulations of an observed case of overshoots in Bauru during the TRO-Pico balloon campaign in the context of upscaling the impact of overshoots at a large scale. These simulations, which have been validated with balloon-borne and S-band radar measurements, shed light on the local-scale variability and composition of overshoots.
Cited articles
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Short summary
This technical note presents the research protocols for phase 4 of the Air Quality Model Evaluation International Initiative (AQMEII4). This initiative has three goals: (i) to define the state of wet and dry deposition in regional models, (ii) to evaluate how dry deposition influences air concentration and flux predictions, and (iii) to identify the causes for prediction differences. The evaluation compares LULC-specific dry deposition and effective conductances and fluxes.
This technical note presents the research protocols for phase 4 of the Air Quality Model...
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