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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Christian Hogrefe, Stefano Galmarini, Paul A. Makar, Ioannis Kioutsioukis, Olivia E. Clifton, Ummugulsum Alyuz, Jesse O. Bash, Roberto Bellasio, Roberto Bianconi, Tim Butler, Philip Cheung, Alma Hodzic, Richard Kranenburg, Aurelia Lupascu, Kester Momoh, Juan Luis Perez-Camanyo, Jonathan E. Pleim, Young-Hee Ryu, Roberto San Jose, Martijn Schaap, Donna B. Schwede, and Ranjeet Sokhi
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David Amptmeijer and Johannes Bieser
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Surface ozone can travel far from its sources. In recent decades, emissions of ozone-forming gases have decreased in North America and Europe but risen in Asia, alongside rising global methane levels. Using advanced modeling, this study reveals that while local reductions in nitrogen oxides have lowered summer ozone, increases in natural and foreign sources offset these gains. Methane remains important, but its ozone impact has declined with reduced local emissions.
Augustin Colette, Gaëlle Collin, François Besson, Etienne Blot, Vincent Guidard, Frederik Meleux, Adrien Royer, Valentin Petiot, Claire Miller, Oihana Fermond, Alizé Jeant, Mario Adani, Joaquim Arteta, Anna Benedictow, Robert Bergström, Dene Bowdalo, Jorgen Brandt, Gino Briganti, Ana C. Carvalho, Jesper Heile Christensen, Florian Couvidat, Ilia D’Elia, Massimo D’Isidoro, Hugo Denier van der Gon, Gaël Descombes, Enza Di Tomaso, John Douros, Jeronimo Escribano, Henk Eskes, Hilde Fagerli, Yalda Fatahi, Johannes Flemming, Elmar Friese, Lise Frohn, Michael Gauss, Camilla Geels, Guido Guarnieri, Marc Guevara, Antoine Guion, Jonathan Guth, Risto Hänninen, Kaj Hansen, Ulas Im, Ruud Janssen, Marine Jeoffrion, Mathieu Joly, Luke Jones, Oriol Jorba, Evgeni Kadantsev, Michael Kahnert, Jacek W. Kaminski, Rostislav Kouznetsov, Richard Kranenburg, Jeroen Kuenen, Anne Caroline Lange, Joachim Langner, Victor Lannuque, Francesca Macchia, Astrid Manders, Mihaela Mircea, Agnes Nyiri, Miriam Olid, Carlos Pérez García-Pando, Yuliia Palamarchuk, Antonio Piersanti, Blandine Raux, Miha Razinger, Lennard Robertson, Arjo Segers, Martijn Schaap, Pilvi Siljamo, David Simpson, Mikhail Sofiev, Anders Stangel, Joanna Struzewska, Carles Tena, Renske Timmermans, Thanos Tsikerdekis, Svetlana Tsyro, Svyatoslav Tyuryakov, Anthony Ung, Andreas Uppstu, Alvaro Valdebenito, Peter van Velthoven, Lina Vitali, Zhuyun Ye, Vincent-Henri Peuch, and Laurence Rouïl
EGUsphere, https://doi.org/10.5194/egusphere-2024-3744, https://doi.org/10.5194/egusphere-2024-3744, 2024
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The Copernicus Atmosphere Monitoring Service – Regional Production delivers daily forecasts, analyses, and reanalyses of air quality in Europe. The Service relies on a distributed modelling production by eleven leading European modelling teams following stringent requirements with an operational design which has no equivalent in the world. All the products are full, free, open and quality assured and disseminated with a high level of reliability.
Koketso Michelle Molepo, Johannes Bieser, Alkuin Maximilian Koenig, Ian Michael Hedgecock, Ralf Ebinghaus, Aurélien Dommergue, Olivier Magand, Hélène Angot, Oleg Travnikov, Lynwill Martin, Casper Labuschagne, Katie Read, and Yann Bertrand
EGUsphere, https://doi.org/10.5194/egusphere-2024-3722, https://doi.org/10.5194/egusphere-2024-3722, 2024
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Mercury exchange between the ocean and atmosphere is poorly understood due to limited in situ data. Here, using atmospheric mercury observations from ground-based monitoring stations along with air mass trajectories, we found that atmospheric Hg levels increase with air mass ocean exposure time, matching predictions for ocean mercury emissions. This finding indicates that ocean emissions directly influence atmospheric mercury levels and enables us to estimate these emissions on a global scale.
T. Nash Skipper, Christian Hogrefe, Barron H. Henderson, Rohit Mathur, Kristen M. Foley, and Armistead G. Russell
Geosci. Model Dev., 17, 8373–8397, https://doi.org/10.5194/gmd-17-8373-2024, https://doi.org/10.5194/gmd-17-8373-2024, 2024
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Chemical transport model simulations are combined with ozone observations to estimate the bias in ozone attributable to US anthropogenic sources and individual sources of US background ozone: natural sources, non-US anthropogenic sources, and stratospheric ozone. Results indicate a positive bias correlated with US anthropogenic emissions during summer in the eastern US and a negative bias correlated with stratospheric ozone during spring.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
David C. Wong, Jeff Willison, Jonathan E. Pleim, Golam Sarwar, James Beidler, Russ Bullock, Jerold A. Herwehe, Rob Gilliam, Daiwen Kang, Christian Hogrefe, George Pouliot, and Hosein Foroutan
Geosci. Model Dev., 17, 7855–7866, https://doi.org/10.5194/gmd-17-7855-2024, https://doi.org/10.5194/gmd-17-7855-2024, 2024
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This work describe how we linked the meteorological Model for Prediction Across Scales – Atmosphere (MPAS-A) with the Community Multiscale Air Quality (CMAQ) air quality model to form a coupled modelling system. This could be used to study air quality or climate and air quality interaction at a global scale. This new model scales well in high-performance computing environments and performs well with respect to ground surface networks in terms of ozone and PM2.5.
Kerry Anderson, Jack Chen, Peter Englefield, Debora Griffin, Paul A. Makar, and Dan Thompson
Geosci. Model Dev., 17, 7713–7749, https://doi.org/10.5194/gmd-17-7713-2024, https://doi.org/10.5194/gmd-17-7713-2024, 2024
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The Global Forest Fire Emissions Prediction System (GFFEPS) is a model that predicts smoke and carbon emissions from wildland fires. The model calculates emissions from the ground up based on satellite-detected fires, modelled weather and fire characteristics. Unlike other global models, GFFEPS uses daily weather conditions to capture changing burning conditions on a day-to-day basis. GFFEPS produced lower carbon emissions due to the changing weather not captured by the other models.
Pascal Simon, Martin Otto Paul Ramacher, Stefan Hagemann, Volker Matthias, Hanna Joerss, and Johannes Bieser
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-236, https://doi.org/10.5194/essd-2024-236, 2024
Revised manuscript accepted for ESSD
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Per- and Polyfluorinated Alkyl Substances (PFAS) constitute a group of often toxic, persistent, and bioaccumulative substances. We constructed a global Emissions model and inventory based on multiple datasets for 23 widely used PFAS. The model computes temporally and spatially resolved model ready emissions distinguishing between emissions to air and emissions to water covering the time span from 1950 up until 2020 on an annual basis to be used for chemistry transport modelling.
Kouji Adachi, Jack E. Dibb, Joseph M. Katich, Joshua P. Schwarz, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Jeff Peischl, Christopher D. Holmes, and James Crawford
Atmos. Chem. Phys., 24, 10985–11004, https://doi.org/10.5194/acp-24-10985-2024, https://doi.org/10.5194/acp-24-10985-2024, 2024
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We examined aerosol particles from wildfires and identified tarballs (TBs) from the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign. This study reveals the compositions, abundance, sizes, and mixing states of TBs and shows that TBs formed as the smoke aged for up to 5 h. This study provides measurements of TBs from various biomass-burning events and ages, enhancing our knowledge of TB emissions and our understanding of their climate impact.
Debora Griffin, Jack Chen, Kerry Anderson, Paul Makar, Chris A. McLinden, Enrico Dammers, and Andre Fogal
Atmos. Chem. Phys., 24, 10159–10186, https://doi.org/10.5194/acp-24-10159-2024, https://doi.org/10.5194/acp-24-10159-2024, 2024
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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 have changed over the past 2 decades.
Linia Tashmim, William C. Porter, Qianjie Chen, Becky Alexander, Charles H. Fite, Christopher D. Holmes, Jeffrey R. Pierce, Betty Croft, and Sakiko Ishino
Atmos. Chem. Phys., 24, 3379–3403, https://doi.org/10.5194/acp-24-3379-2024, https://doi.org/10.5194/acp-24-3379-2024, 2024
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Dimethyl sulfide (DMS) is mostly emitted from ocean surfaces and represents the largest natural source of sulfur for the atmosphere. Once in the atmosphere, DMS forms stable oxidation products such as SO2 and H2SO4, which can subsequently contribute to airborne particle formation and growth. In this study, we update the DMS oxidation mechanism in the chemical transport model GEOS-Chem and describe resulting changes in particle growth as well as the overall global sulfur budget.
Stefan J. Miller, Paul A. Makar, and Colin J. Lee
Geosci. Model Dev., 17, 2197–2219, https://doi.org/10.5194/gmd-17-2197-2024, https://doi.org/10.5194/gmd-17-2197-2024, 2024
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This work outlines a new solver written in Fortran to calculate the partitioning of metastable aerosols at thermodynamic equilibrium based on the forward algorithms of ISORROPIA II. The new code includes numerical improvements that decrease the computational speed (compared to ISORROPIA II) while improving the accuracy of the partitioning solution.
Heather Simon, Christian Hogrefe, Andrew Whitehill, Kristen M. Foley, Jennifer Liljegren, Norm Possiel, Benjamin Wells, Barron H. Henderson, Lukas C. Valin, Gail Tonnesen, K. Wyat Appel, and Shannon Koplitz
Atmos. Chem. Phys., 24, 1855–1871, https://doi.org/10.5194/acp-24-1855-2024, https://doi.org/10.5194/acp-24-1855-2024, 2024
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We assess observed and modeled ozone weekend–weekday differences in the USA from 2002–2019. A subset of urban areas that were NOx-saturated at the beginning of the period transitioned to NOx-limited conditions. Multiple rural areas of California were NOx-limited for the entire period but become less influenced by local day-of-week emission patterns in more recent years. The model produces more NOx-saturated conditions than the observations but captures trends in weekend–weekday ozone patterns.
Roya Ghahreman, Wanmin Gong, Paul A. Makar, Alexandru Lupu, Amanda Cole, Kulbir Banwait, Colin Lee, and Ayodeji Akingunola
Geosci. Model Dev., 17, 685–707, https://doi.org/10.5194/gmd-17-685-2024, https://doi.org/10.5194/gmd-17-685-2024, 2024
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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
Publication in GMD not foreseen
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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.
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
Preprint withdrawn
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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.
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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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