Articles | Volume 13, issue 19
https://doi.org/10.5194/acp-13-10143-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-13-10143-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| Highlight paper
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15 Oct 2013
Research article | Highlight paper |
| 15 Oct 2013
Cloud-resolving simulations of mercury scavenging and deposition in thunderstorms
U. S. Nair
Department of Atmospheric Science, University of Alabama in Huntsville, Huntsville, Alabama, USA
Y. Wu
Earth System Science Center, University of Alabama in Huntsville, Huntsville, Alabama, USA
C. D. Holmes
Department of Earth System Science, University of California, Irvine, California, USA
A. Ter Schure
Electric Power Research Institute, Palo Alto, California, USA
G. Kallos
School of Physics, University of Athens, Athens, Greece
J. T. Walters
Southen Company Services, Birmingham, Alabama, USA
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Christopher D. Holmes, Joshua P. Schwarz, Charles H. Fite, Anxhelo Agastra, Holly K. Nowell, Katherine Ball, T. Paul Bui, Johnathan Dean-Day, Zachary C. J. Decker, Joshua P. DiGagni, Glenn S. Diskin, Emily M. Gargulinski, Hannah Halliday, Shobha Kondragunta, John B. Nowak, David A. Peterson, Michael A. Robinson, Amber J. Soja, Rebecca A. Washenfelder, Chuanyu Xu, and Robert J. Yokelson
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2025-307, https://doi.org/10.5194/essd-2025-307, 2025
Preprint under review for ESSD
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Smoke age is an important factor in the chemical and physical evolution of smoke. Two methods for determining the age of smoke are applied to the NASA-NOAA FIREX-AQ field campaign: one based on wind speed and distance, and another using an ensemble of modeled air parcel trajectories. Both methods are evaluated, with the trajectory method, which includes plume rise and uncertainty estimates, proving more accurate.
Anam M. Khan, Olivia E. Clifton, Jesse O. Bash, Sam Bland, Nathan Booth, Philip Cheung, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christian Hogrefe, Christopher D. Holmes, Laszlo Horvath, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Perez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Donna Schwede, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamas Weidinger, Zhiyong Wu, Leiming Zhang, and Paul C. Stoy
EGUsphere, https://doi.org/10.5194/egusphere-2024-3038, https://doi.org/10.5194/egusphere-2024-3038, 2024
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Vegetation removes tropospheric ozone through stomatal uptake, and accurately modeling the stomatal uptake of ozone is important for modeling dry deposition and air quality. We evaluated the stomatal component of ozone dry deposition modeled by atmospheric chemistry models at six sites. We find that models and observation-based estimates agree at times during the growing season at all sites, but some models overestimated the stomatal component during the dry summers at a seasonally dry site.
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.
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.
Peiyang Cheng, Arastoo Pour-Biazar, Yuling Wu, Shi Kuang, Richard T. McNider, and William J. Koshak
Atmos. Chem. Phys., 24, 41–63, https://doi.org/10.5194/acp-24-41-2024, https://doi.org/10.5194/acp-24-41-2024, 2024
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Lightning-induced nitrogen monoxide (LNO) emission can be estimated from geostationary satellite observations. The present study uses the LNO emission estimates derived from geostationary satellite observations in an air quality modeling system to investigate the impact of LNO on air quality. Results indicate that significant ozone increase could be due to long-distance chemical transport, lightning activity in the upwind direction, and the mixing of high LNO (or ozone) plumes.
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.
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.
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.
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.
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.
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.
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.
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.
Stefano Galmarini, Paul Makar, Olivia E. Clifton, Christian Hogrefe, Jesse O. Bash, Roberto Bellasio, Roberto Bianconi, Johannes Bieser, Tim Butler, Jason Ducker, Johannes Flemming, Alma Hodzic, Christopher D. Holmes, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Juan Luis Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Sam Silva, and Ralf Wolke
Atmos. Chem. Phys., 21, 15663–15697, https://doi.org/10.5194/acp-21-15663-2021, https://doi.org/10.5194/acp-21-15663-2021, 2021
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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.
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 %.
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.
Christos Stathopoulos, George Galanis, Nikolaos S. Bartsotas, and George Kallos
Adv. Geosci., 45, 289–294, https://doi.org/10.5194/adgeo-45-289-2018, https://doi.org/10.5194/adgeo-45-289-2018, 2018
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.
Alexandra Tsekeri, Anton Lopatin, Vassilis Amiridis, Eleni Marinou, Julia Igloffstein, Nikolaos Siomos, Stavros Solomos, Panagiotis Kokkalis, Ronny Engelmann, Holger Baars, Myrto Gratsea, Panagiotis I. Raptis, Ioannis Binietoglou, Nikolaos Mihalopoulos, Nikolaos Kalivitis, Giorgos Kouvarakis, Nikolaos Bartsotas, George Kallos, Sara Basart, Dirk Schuettemeyer, Ulla Wandinger, Albert Ansmann, Anatoli P. Chaikovsky, and Oleg Dubovik
Atmos. Meas. Tech., 10, 4995–5016, https://doi.org/10.5194/amt-10-4995-2017, https://doi.org/10.5194/amt-10-4995-2017, 2017
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The Generalized Aerosol Retrieval from Radiometer and Lidar Combined data algorithm (GARRLiC) and the LIdar-Radiometer Inversion Code (LIRIC) provide the opportunity to study the aerosol vertical distribution by combining ground-based lidar and sun-photometric measurements. Here, we utilize the capabilities of both algorithms for the characterization of Saharan dust and marine particles, along with their mixtures, in the south-eastern Mediterranean.
Evangelia Diapouli, Manousos I. Manousakas, Stergios Vratolis, Vasiliki Vasilatou, Stella Pateraki, Kyriaki A. Bairachtari, Xavier Querol, Fulvio Amato, Andrés Alastuey, Angeliki A. Karanasiou, Franco Lucarelli, Silvia Nava, Giulia Calzolai, Vorne L. Gianelle, Cristina Colombi, Célia Alves, Danilo Custódio, Casimiro Pio, Christos Spyrou, George B. Kallos, and Konstantinos Eleftheriadis
Atmos. Chem. Phys., 17, 3673–3685, https://doi.org/10.5194/acp-17-3673-2017, https://doi.org/10.5194/acp-17-3673-2017, 2017
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This study examined the contribution of two natural sources (long-range transport of African dust and sea salt) to the airborne particulate matter concentrations, in 5 southern European cities (Porto, Barcelona, Milan, Florence, Athens). The results demonstrated that natural sources are often expressed with high-intensity events, leading even to exceedances of the EU air quality standards. This effect was more pronounced in the case of African dust intrusions in the eastern Mediterranean area.
Rodanthi-Elisavet Mamouri, Albert Ansmann, Argyro Nisantzi, Stavros Solomos, George Kallos, and Diofantos G. Hadjimitsis
Atmos. Chem. Phys., 16, 13711–13724, https://doi.org/10.5194/acp-16-13711-2016, https://doi.org/10.5194/acp-16-13711-2016, 2016
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.
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
C. Spyrou, G. Kallos, C. Mitsakou, P. Athanasiadis, C. Kalogeri, and M. J. Iacono
Atmos. Chem. Phys., 13, 5489–5504, https://doi.org/10.5194/acp-13-5489-2013, https://doi.org/10.5194/acp-13-5489-2013, 2013
C. Tatum Ernest, D. Donohoue, D. Bauer, A. Ter Schure, and A. J. Hynes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-12-33291-2012, https://doi.org/10.5194/acpd-12-33291-2012, 2012
Revised manuscript not accepted
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
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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
Beata Bukosa, Sara Mikaloff-Fletcher, Gordon Brailsford, Dan Smale, Elizabeth D. Keller, W. Troy Baisden, Miko U. F. Kirschbaum, Donna L. Giltrap, Lìyǐn Liáng, Stuart Moore, Rowena Moss, Sylvia Nichol, Jocelyn Turnbull, Alex Geddes, Daemon Kennett, Dóra Hidy, Zoltán Barcza, Louis A. Schipper, Aaron M. Wall, Shin-Ichiro Nakaoka, Hitoshi Mukai, and Andrea Brandon
Atmos. Chem. Phys., 25, 6445–6473, https://doi.org/10.5194/acp-25-6445-2025, https://doi.org/10.5194/acp-25-6445-2025, 2025
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We used atmospheric measurements and inverse modelling to estimate New Zealand's carbon dioxide (CO2) emissions and removals from 2011 to 2020. Our study reveals that New Zealand's land absorbs more CO2 than previously estimated, particularly in areas dominated by indigenous forests. Our results highlight gaps in current national CO2 estimates and methods, suggesting a need for further research to improve emissions reports and refine approaches to track progress toward climate mitigation goals.
Santiago Botía, Saqr Munassar, Thomas Koch, Danilo Custodio, Luana S. Basso, Shujiro Komiya, Jost V. Lavric, David Walter, Manuel Gloor, Giordane Martins, Stijn Naus, Gerbrand Koren, Ingrid T. Luijkx, Stijn Hantson, John B. Miller, Wouter Peters, Christian Rödenbeck, and Christoph Gerbig
Atmos. Chem. Phys., 25, 6219–6255, https://doi.org/10.5194/acp-25-6219-2025, https://doi.org/10.5194/acp-25-6219-2025, 2025
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This study uses dry CO2 mole fractions from the Amazon Tall Tower Observatory together with airborne profiles to estimate net carbon exchange in tropical South America. We found that the biogeographic Amazon is a net carbon sink, while the Cerrado and Caatinga biomes are net carbon sources, resulting in an overall neutral balance. Finally, to further reduce the uncertainty in our estimates we call for an expansion of the monitoring capacity, especially in the Amazon–Andes foothills.
Qingjian Yang, Tiangliang Zhao, Yongqing Bai, Kai Meng, Yuehan Luo, Zhijie Tian, Xiaoyun Sun, Weikang Fu, Kai Yang, and Jun Hu
EGUsphere, https://doi.org/10.5194/egusphere-2025-737, https://doi.org/10.5194/egusphere-2025-737, 2025
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This study reveals a unique driver of the Tibetan Plateau (TP) thermal forcing on the interannual variations in stratosphere-to-troposphere transport (STT) of ozone with diverse structures. Anomalous strong TP thermal forcing induces anticyclonic anomalies in the upper troposphere over the TP, which strengthens and attenuates the northern and southern branches of the westerly jet, intensifying and weakening the westerly trough for more (less) tropopause folds of ozone STT over East Asian region.
Sepehr Fathi, Paul Makar, Wanmin Gong, Junhua Zhang, Katherine Hayden, and Mark Gordon
Atmos. Chem. Phys., 25, 2385–2405, https://doi.org/10.5194/acp-25-2385-2025, https://doi.org/10.5194/acp-25-2385-2025, 2025
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Our study explores the influence of water phase changes in plumes from industrial sources on atmospheric dispersion of emitted pollutants and air quality. Employing PRISM (Plume-Rise-Iterative-Stratified-Moist), a new method, we found that considering these effects significantly improves predictions of pollutant dispersion. This insight enhances our understanding of environmental impacts, enabling more accurate air quality modelling and fostering more effective pollution management strategies.
Maria K. Tenkanen, Aki Tsuruta, Hugo Denier van der Gon, Lena Höglund-Isaksson, Antti Leppänen, Tiina Markkanen, Ana Maria Roxana Petrescu, Maarit Raivonen, Hermanni Aaltonen, and Tuula Aalto
Atmos. Chem. Phys., 25, 2181–2206, https://doi.org/10.5194/acp-25-2181-2025, https://doi.org/10.5194/acp-25-2181-2025, 2025
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Accurate national methane (CH4) emission estimates are essential for tracking progress towards climate goals. This study compares estimates from Finland, which use different methods and scales, and shows how well a global model estimates emissions within a country. The bottom-up estimates vary a lot, but constraining them with atmospheric CH4 measurements brought the estimates closer together. We also highlight the importance of quantifying natural emissions alongside anthropogenic emissions.
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
EGUsphere, https://doi.org/10.5194/egusphere-2025-225, https://doi.org/10.5194/egusphere-2025-225, 2025
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Performed 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 regional-scale models. The results also strongly suggest that improvement and harmonization of the representation of land use in these models would serve the community in their future development efforts.
Aki Tsuruta, Akihiko Kuze, Kei Shiomi, Fumie Kataoka, Nobuhiro Kikuchi, Tuula Aalto, Leif Backman, Ella Kivimäki, Maria K. Tenkanen, Kathryn McKain, Omaira E. García, Frank Hase, Rigel Kivi, Isamu Morino, Hirofumi Ohyama, David F. Pollard, Mahesh K. Sha, Kimberly Strong, Ralf Sussmann, Yao Te, Voltaire A. Velazco, Mihalis Vrekoussis, Thorsten Warneke, Minqiang Zhou, and Hiroshi Suto
EGUsphere, https://doi.org/10.5194/egusphere-2025-159, https://doi.org/10.5194/egusphere-2025-159, 2025
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Satellite data bring invaluable information about greenhouse gas emissions globally. We found that a new type of data from the Greenhouse Gas Observing Satellite (GOSAT), which contains information about methane in the lowest layer of Earth's atmosphere, could provide reliable estimates of recent methane emissions when combined with atmospheric modelling. Therefore, the use of such data is encouraged to improve emission quantification methods and advance our understanding of methane cycles.
Xingyu Wang, Fei Jiang, Hengmao Wang, Zhengqi Zhang, Mousong Wu, Jun Wang, Wei He, Weimin Ju, and Jing M. Chen
Atmos. Chem. Phys., 25, 867–880, https://doi.org/10.5194/acp-25-867-2025, https://doi.org/10.5194/acp-25-867-2025, 2025
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The role of OCO-3 XCO2 retrievals in estimating global terrestrial carbon fluxes is unclear. We investigate this by assimilating OCO-3 XCO2 retrievals alone and in combination with OCO-2 XCO2. The assimilation of OCO-3 XCO2 alone underestimates global land sinks, mainly at high latitudes, due to the lack of observations beyond 52° S and 52° N, large variations in the number of data, and varying observation times, while the joint assimilation of OCO-2 and OCO-3 XCO2 has the best performance.
Zhou Zang, Jane Liu, David Tarasick, Omid Moeini, Jianchun Bian, Jinqiang Zhang, Anne M. Thompson, Roeland Van Malderen, Herman G. J. Smit, Ryan M. Stauffer, Bryan J. Johnson, and Debra E. Kollonige
Atmos. Chem. Phys., 24, 13889–13912, https://doi.org/10.5194/acp-24-13889-2024, https://doi.org/10.5194/acp-24-13889-2024, 2024
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The Trajectory-mapped Ozonesonde dataset for the Stratosphere and Troposphere (TOST) provides a global-scale, long-term ozone climatology that is horizontally and vertically resolved. In this study, we improved, updated and validated TOST from 1970 to 2021. Based on this TOST dataset, we characterized global ozone variations spatially in both the troposphere and stratosphere and temporally by season and decade. We also showed a stagnant lower stratospheric ozone variation since the late 1990s.
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.
Zhenda Sun, Hao Yin, Zhongfeng Pan, Chongyang Li, Xiao Lu, Youwen Sun, and Cheng Liu
EGUsphere, https://doi.org/10.5194/egusphere-2024-3252, https://doi.org/10.5194/egusphere-2024-3252, 2024
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This study investigates the variability and driving force of transboundary transport flux of carbon monoxide (CO) over the Tibetan Plateau from May 2018 to April 2024. We discovered that CO levels peak in late autumn and winter, driven mainly by external influx from South Asia, while internal emissions have decreased slightly. The findings reveal a growing trend in CO concentrations in the region, emphasizing the Tibetan Plateau's role as a significant receptor for transboundary pollutants.
William J. Collins, Fiona M. O'Connor, Connor R. Barker, Rachael E. Byrom, Sebastian D. Eastham, Øivind Hodnebrog, Patrick Jöckel, Eloise A. Marais, Mariano Mertens, Gunnar Myhre, Matthias Nützel, Dirk Olivié, Ragnhild Bieltvedt Skeie, Laura Stecher, Larry W. Horowitz, Vaishali Naik, Gregory Faluvegi, Ulas Im, Lee T. Murray, Drew Shindell, Kostas Tsigaridis, Nathan Luke Abraham, and James Keeble
EGUsphere, https://doi.org/10.5194/egusphere-2024-3698, https://doi.org/10.5194/egusphere-2024-3698, 2024
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If reductions aren’t implemented to limit emissions of pollutants that produce ozone then we calculate that this will cause a warming of climate. We assess how the future warming from ozone is affected by changing meteorological variables such as clouds and atmospheric temperatures. We find that reductions in high cloud cover tend to slightly reduce the warming from ozone.
Kai Meng, Tianliang Zhao, Yongqing Bai, Ming Wu, Le Cao, Xuewei Hou, Yuehan Luo, and Yongcheng Jiang
Atmos. Chem. Phys., 24, 12623–12642, https://doi.org/10.5194/acp-24-12623-2024, https://doi.org/10.5194/acp-24-12623-2024, 2024
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We studied the impact of stratospheric intrusions (SIs) on tropospheric and near-surface ozone in Central and Eastern China from a stratospheric source tracing perspective. SIs contribute the most in the eastern plains, with a contribution exceeding 15 %, and have a small contribution to the west and south. Western Siberia and Mongolia are the most critical source areas for indirect and direct SIs, with the Rossby wave and northeast cold vortex being important driving circulation systems.
Michael Steiner, Luca Cantarello, Stephan Henne, and Dominik Brunner
Atmos. Chem. Phys., 24, 12447–12463, https://doi.org/10.5194/acp-24-12447-2024, https://doi.org/10.5194/acp-24-12447-2024, 2024
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Atmospheric greenhouse gas inversions have great potential to independently check reported bottom-up emissions; however they are subject to large uncertainties. It is paramount to address and reduce the largest source of uncertainty, which stems from the representation of atmospheric transport in the models. In this study, we show that the use of a temporally varying flow-dependent atmospheric transport uncertainty can enhance the accuracy of emission estimation in an idealized experiment.
Sieglinde Callewaert, Minqiang Zhou, Bavo Langerock, Pucai Wang, Ting Wang, Emmanuel Mahieu, and Martine De Mazière
EGUsphere, https://doi.org/10.5194/egusphere-2024-3228, https://doi.org/10.5194/egusphere-2024-3228, 2024
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We used an atmospheric transport model and satellite data to study CH4 observations at Xianghe, China. Our study shows the key source sectors that influence the concentrations and their respective importance. Furthermore, meteorological factors such as wind direction are discussed. This research highlights the challenges in accurately simulating these kind of measurements and helps us to better understand CH4 variability in the region.
Jinhui Gao and Hui Xiao
EGUsphere, https://doi.org/10.5194/egusphere-2024-3070, https://doi.org/10.5194/egusphere-2024-3070, 2024
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The ensemble simulation provides a solution to better reproduce and understand the extremely high ozone episode occurred in the GBA when Typhoon NIDA approached South China in summer 2016. Elevated temperatures and weak winds contributed to the increase in ozone precursors, resulting in enhanced ozone production. Large amounts of ozone aloft also contributed to the increase in surface ozone via vertical transport. Notably, ozone from Southeast Asia contributed through this mechanism.
Brian L. Boys, Randall V. Martin, and Trevor C. VandenBoer
EGUsphere, https://doi.org/10.5194/egusphere-2024-2994, https://doi.org/10.5194/egusphere-2024-2994, 2024
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A widely used dry deposition parameterization for NO2 is updated by including a well-known heterogeneous hydrolysis reaction on deposition surfaces. This mechanistic update eliminates a large low bias of -80 % in simulated NO2 nocturnal deposition velocities evaluated against long-term eddy covariance flux observations over Harvard Forest. We highlight the importance of canopy surface area effects as well as soil NO emission in formulating and evaluating NO2 dry deposition parameterizations.
Cynthia D. Nevison, Qing Liang, Paul A. Newman, Britton B. Stephens, Geoff Dutton, Xin Lan, Roisin Commane, Yenny Gonzalez, and Eric Kort
Atmos. Chem. Phys., 24, 10513–10529, https://doi.org/10.5194/acp-24-10513-2024, https://doi.org/10.5194/acp-24-10513-2024, 2024
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This study examines the drivers of interannual variability in tropospheric N2O. New insights are obtained from aircraft data and a chemistry–climate model that explicitly simulates stratospheric N2O. The stratosphere is found to be the dominant driver of N2O variability in the Northern Hemisphere, while both the stratosphere and El Niño cycles are important in the Southern Hemisphere. These results are consistent with known atmospheric dynamics and differences between the hemispheres.
Misa Ishizawa, Douglas Chan, Doug Worthy, Elton Chan, Felix Vogel, Joe R. Melton, and Vivek K. Arora
Atmos. Chem. Phys., 24, 10013–10038, https://doi.org/10.5194/acp-24-10013-2024, https://doi.org/10.5194/acp-24-10013-2024, 2024
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Methane (CH4) emissions in Canada for 2007–2017 were estimated using Canada’s surface greenhouse gas measurements. The estimated emissions show no significant trend, but emission uncertainty was reduced as more measurement sites became available. Notably for climate change, we find the wetland CH4 emissions show a positive correlation with surface air temperature in summer. Canada’s measurement network could monitor future CH4 emission changes and compliance with climate change mitigation goals.
Yiang Chen, Xingcheng Lu, and Jimmy C. H. Fung
Atmos. Chem. Phys., 24, 8847–8864, https://doi.org/10.5194/acp-24-8847-2024, https://doi.org/10.5194/acp-24-8847-2024, 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 in major spatiotemporal contributors to the O3 pollution under the influence of typhoons and subtropical high pressure. Through 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.
Fabian Maier, Christian Rödenbeck, Ingeborg Levin, Christoph Gerbig, Maksym Gachkivskyi, and Samuel Hammer
Atmos. Chem. Phys., 24, 8183–8203, https://doi.org/10.5194/acp-24-8183-2024, https://doi.org/10.5194/acp-24-8183-2024, 2024
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We investigate the usage of discrete radiocarbon (14C)-based fossil fuel carbon dioxide (ffCO2) concentration estimates vs. continuous carbon monoxide (CO)-based ffCO2 estimates to evaluate the seasonal cycle of ffCO2 emissions in an urban region with an inverse modeling framework. We find that the CO-based ffCO2 estimates allow us to reconstruct robust seasonal cycles, which show the distinct COVID-19 drawdown in 2020 and can be used to validate emission inventories.
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.
Antoine Berchet, Isabelle Pison, Camille Huselstein, Clément Narbaud, Marine Remaud, Sauveur Belviso, Camille Abadie, and Fabienne Maignan
EGUsphere, https://doi.org/10.5194/egusphere-2024-549, https://doi.org/10.5194/egusphere-2024-549, 2024
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We use the measurements of atmospheric carbonyl sulfide (COS) concentrations at the monitoring site of Gif-sur-Yvette (in the Paris area) from August 2014 to December 2019, combined with existing knowledge on COS fluxes in the atmosphere and and transport model to gain insight on COS fluxes, either natural such as the oceanic emissions or the vegetation and soil fluxes, or anthropogenic, from industrial activities and power generation.
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.
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.
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.
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