Articles | Volume 17, issue 14
https://doi.org/10.5194/acp-17-8999-2017
© Author(s) 2017. 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-17-8999-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
27 Jul 2017
Research article |
| 27 Jul 2017
Subtropical subsidence and surface deposition of oxidized mercury produced in the free troposphere
Department of Atmospheric Sciences, University of Washington, Seattle,
WA 98195, USA
Lyatt Jaeglé
Department of Atmospheric Sciences, University of Washington, Seattle,
WA 98195, USA
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Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
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Short summary
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
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.
Ruochong Xu, Joel A. Thornton, Ben H. Lee, Yanxu Zhang, Lyatt Jaeglé, Felipe D. Lopez-Hilfiker, Pekka Rantala, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 5477–5494, https://doi.org/10.5194/acp-22-5477-2022, https://doi.org/10.5194/acp-22-5477-2022, 2022
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Monoterpenes are emitted into the atmosphere by vegetation and by the use of certain consumer products. Reactions of monoterpenes in the atmosphere lead to low-volatility products that condense to grow particulate matter or participate in new particle formation and, thus, affect air quality and climate. We use a model of atmospheric chemistry and transport to evaluate the global-scale importance of recent updates to our understanding of monoterpene chemistry in particle formation and growth.
Viral Shah, Daniel J. Jacob, Jonathan M. Moch, Xuan Wang, and Shixian Zhai
Atmos. Chem. Phys., 20, 12223–12245, https://doi.org/10.5194/acp-20-12223-2020, https://doi.org/10.5194/acp-20-12223-2020, 2020
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Jiayue Huang, Lyatt Jaeglé, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mat J. Evans, Nicolas Theys, and Sungyeon Choi
Atmos. Chem. Phys., 20, 7335–7358, https://doi.org/10.5194/acp-20-7335-2020, https://doi.org/10.5194/acp-20-7335-2020, 2020
Short summary
Short summary
Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often observed in the springtime Arctic. Here, we use a chemical transport model to examine the role of sea salt aerosol from blowing snow in explaining these phenomena. We find that our simulation can account for the spatiotemporal variability of satellite observations of BrO. However, the model has difficulty in producing the magnitude of observed ozone depletion events.
Viral Shah, Daniel J. Jacob, Ke Li, Rachel F. Silvern, Shixian Zhai, Mengyao Liu, Jintai Lin, and Qiang Zhang
Atmos. Chem. Phys., 20, 1483–1495, https://doi.org/10.5194/acp-20-1483-2020, https://doi.org/10.5194/acp-20-1483-2020, 2020
Short summary
Short summary
We analyze 15 years of satellite observations of nitrogen dioxide (NO2) and use an atmospheric chemistry model to understand the seasonal changes and trends in nitrogen oxides (NOx) over China. We show that the seasonal changes in NO2 occur due to changes in the NOx oxidation lifetime. We find that Chinese NOx emissions peaked in 2011 and had decreased by about 25 % by 2018. But the decrease in NO2 in winter was larger, likely because of a simultaneous decrease in the NOx oxidation lifetime.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
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Eloise A. Marais, Daniel J. Jacob, Sungyeon Choi, Joanna Joiner, Maria Belmonte-Rivas, Ronald C. Cohen, Steffen Beirle, Lee T. Murray, Luke D. Schiferl, Viral Shah, and Lyatt Jaeglé
Atmos. Chem. Phys., 18, 17017–17027, https://doi.org/10.5194/acp-18-17017-2018, https://doi.org/10.5194/acp-18-17017-2018, 2018
Short summary
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Jiayue Huang, Lyatt Jaeglé, and Viral Shah
Atmos. Chem. Phys., 18, 16253–16269, https://doi.org/10.5194/acp-18-16253-2018, https://doi.org/10.5194/acp-18-16253-2018, 2018
Short summary
Short summary
The contribution of blowing snow and frost flower as sources of sea salt aerosols (SSA) over polar regions remains uncertain, despite its potentially important role in polar climate and chemistry. Using chemical transport models and satellite observations, we find that blowing snow emissions are the dominant source of SSA over sea ice during the cold season. We infer a monthly snow salinity on first-year sea ice that decreases from fall–spring, minimizing the model discrepancy to within 10 %.
Johannes Bieser, Franz Slemr, Jesse Ambrose, Carl Brenninkmeijer, Steve Brooks, Ashu Dastoor, Francesco DeSimone, Ralf Ebinghaus, Christian N. Gencarelli, Beate Geyer, Lynne E. Gratz, Ian M. Hedgecock, Daniel Jaffe, Paul Kelley, Che-Jen Lin, Lyatt Jaegle, Volker Matthias, Andrei Ryjkov, Noelle E. Selin, Shaojie Song, Oleg Travnikov, Andreas Weigelt, Winston Luke, Xinrong Ren, Andreas Zahn, Xin Yang, Yun Zhu, and Nicola Pirrone
Atmos. Chem. Phys., 17, 6925–6955, https://doi.org/10.5194/acp-17-6925-2017, https://doi.org/10.5194/acp-17-6925-2017, 2017
Short summary
Short summary
We conducted a multi model study to investigate our ability to reproduce the vertical distribution of mercury in the atmosphere. For this, we used observational data from over 40 aircraft flights in EU and US. We compared observations to the results of seven chemistry transport models and found that the models are able to reproduce vertical gradients of total and elemental Hg. Finally, we found that different chemical reactions seem responsible for the oxidation of Hg depending on altitude.
Jiayue Huang and Lyatt Jaeglé
Atmos. Chem. Phys., 17, 3699–3712, https://doi.org/10.5194/acp-17-3699-2017, https://doi.org/10.5194/acp-17-3699-2017, 2017
Short summary
Short summary
The emissions and distribution of wintertime sea salt aerosol (SSA) are poorly constrained in polar regions, despite their potentially significant roles in halogen release, cloud formation and climate. We implement a blowing snow and a frost flower emission scheme in the model, and find that inclusion of blowing snow is necessary to simulate the observed winter and spring SSA levels. We estimate that inclusion of blowing snow increases submicron SSA emissions by factors of 2–3 in polar regions.
V. Shah, L. Jaeglé, L. E. Gratz, J. L. Ambrose, D. A. Jaffe, N. E. Selin, S. Song, T. L. Campos, F. M. Flocke, M. Reeves, D. Stechman, M. Stell, J. Festa, J. Stutz, A. J. Weinheimer, D. J. Knapp, D. D. Montzka, G. S. Tyndall, E. C. Apel, R. S. Hornbrook, A. J. Hills, D. D. Riemer, N. J. Blake, C. A. Cantrell, and R. L. Mauldin III
Atmos. Chem. Phys., 16, 1511–1530, https://doi.org/10.5194/acp-16-1511-2016, https://doi.org/10.5194/acp-16-1511-2016, 2016
Short summary
Short summary
We present airborne observations of mercury over the southeastern USA during summer. Higher concentrations of oxidized mercury were observed in clean, dry air masses descending in the subtropical anti-cyclones. We used an atmospheric model to simulate the chemistry and transport of mercury. We found reasonable agreement with the observations when the modeled oxidation of elemental mercury was increased, suggesting fast cycling between elemental and oxidized mercury.
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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Tracking daily NOx emissions from an urban agglomeration based on TROPOMI NO2 and a local ensemble transform Kalman filter
The atmospheric oxidizing capacity in China – Part 2: Sensitivity to emissions of primary pollutants
Role of chemical production and depositional losses on formaldehyde in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Review of source analyses of ambient volatile organic compounds considering reactive losses: methods of reducing loss effects, impacts of losses, and sources
Interpreting summertime hourly variation of NO2 columns with implications for geostationary satellite applications
An investigation into atmospheric nitrous acid (HONO) processes in South Korea
Performance evaluation of UKESM1 for surface ozone across the pan-tropics
Constraining light dependency in modeled emissions through comparison to observed biogenic volatile organic compound (BVOC) concentrations in a southeastern US forest
A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021
Monoterpene oxidation pathways initiated by acyl peroxy radical addition
Tropospheric ozone precursors: global and regional distributions, trends, and variability
Representing improved tropospheric ozone distribution by including lightning NOx emissions in CHIMERE
Sensitivity of climate effects of hydrogen to leakage size, location, and chemical background
The contribution of transport emissions to ozone mixing ratios and methane lifetime in 2015 and 2050 in the Shared Socioeconomic Pathways (SSPs)
Ether and ester formation from peroxy radical recombination: a qualitative reaction channel analysis
ACEIC: a comprehensive anthropogenic chlorine emission inventory for China
Impact of methane and other precursor emission reductions on surface ozone in Europe: scenario analysis using the European Monitoring and Evaluation Programme (EMEP) Meteorological Synthesizing Centre – West (MSC-W) model
High-resolution mapping of on-road vehicle emissions with real-time traffic datasets based on big data
Chemistry-climate feedback of atmospheric methane in a methane emission flux driven chemistry-climate model
Jincheol Park, Yunsoo Choi, and Sagun Kayastha
Atmos. Chem. Phys., 25, 4291–4311, https://doi.org/10.5194/acp-25-4291-2025, https://doi.org/10.5194/acp-25-4291-2025, 2025
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We investigated NOx emission contributions to NOy loadings across five regions of East Asia during the 2022 winter–spring transition through chemical transport modeling informed by satellite data. As seasons progress, local contributions within each region to its NOy budget decreased from 32 %–43 % to 23 %–30 %, while transboundary contributions increased from 16 %–33 % to 27 %–37 %, driven by a shift in synoptic settings that allowed pollutants to spread more broadly across the regions.
Qianqian Zhang, K. Folkert Boersma, Chiel van der Laan, Alba Mols, Bin Zhao, Shengyue Li, and Yuepeng Pan
Atmos. Chem. Phys., 25, 3313–3326, https://doi.org/10.5194/acp-25-3313-2025, https://doi.org/10.5194/acp-25-3313-2025, 2025
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Accurate NOx emission estimates are required to better understand air pollution. This study investigates and demonstrates the ability of the superposition column model in combination with TROPOMI tropospheric NO2 column data to estimate city-scale NOx emissions and lifetimes and their variabilities. The results of this work nevertheless confirm the strength of the superposition column model in estimating urban NOx emissions with reasonable accuracy.
Wenbin Kou, Yang Gao, Dan Tong, Xiaojie Guo, Xiadong An, Wenyu Liu, Mengshi Cui, Xiuwen Guo, Shaoqing Zhang, Huiwang Gao, and Lixin Wu
Atmos. Chem. Phys., 25, 3029–3048, https://doi.org/10.5194/acp-25-3029-2025, https://doi.org/10.5194/acp-25-3029-2025, 2025
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Unlike traditional numerical studies, we apply a high-resolution Earth system model, improving simulations of surface ozone and large-scale circulations such as atmospheric blocking. Besides local heat waves, we quantify the impact of atmospheric blocking on downstream ozone concentrations, which is closely associated with the blocking position. We identify three major pathways of Rossby wave propagation, stressing the critical role of large-scale circulation in regional air quality.
Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther
Atmos. Chem. Phys., 25, 2863–2894, https://doi.org/10.5194/acp-25-2863-2025, https://doi.org/10.5194/acp-25-2863-2025, 2025
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Vegetation releases biogenic volatile organic compounds, while soils and lightning contribute to the natural emissions of nitrogen oxides into the atmosphere. These gases interact in complex ways. Using satellite data and models, we developed a new method to simultaneously optimize these natural emissions over Africa in 2019. Our approach resulted in an increase in natural emissions, supported by independent data indicating that current estimates are underestimated.
Shuai Li, Haolin Wang, and Xiao Lu
Atmos. Chem. Phys., 25, 2725–2743, https://doi.org/10.5194/acp-25-2725-2025, https://doi.org/10.5194/acp-25-2725-2025, 2025
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Summertime ozone–temperature sensitivity has decreased by 50 % from 3.0 ppbv per K in 1990 to 1.5 ppb per K in 2021 in the US. GEOS-Chem simulations show that anthropogenic nitrogen oxide emission reduction is the dominant driver of ozone–temperature sensitivity decline by influencing both temperature direct and temperature indirect processes. Reduced ozone–temperature sensitivity has decreased ozone enhancement from low to high temperatures by an average of 6.8 ppbv across the US.
Jinya Yang, Yutong Wang, Lei Zhang, and Yu Zhao
Atmos. Chem. Phys., 25, 2649–2666, https://doi.org/10.5194/acp-25-2649-2025, https://doi.org/10.5194/acp-25-2649-2025, 2025
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We develop a modeling framework to predict future ozone concentrations (till the 2060s) in China following an IPCC scenario. We evaluate the contributions of climatic, anthropogenic, and biogenic factors by season and region. We find persistent emission controls will alter the nonlinear response of ozone to its precursors and dominate the declining ozone level. The outcomes highlight the importance of human actions, even with a climate penalty on air quality.
Takashi Sekiya, Emanuele Emili, Kazuyuki Miyazaki, Antje Inness, Zhen Qu, R. Bradley Pierce, Dylan Jones, Helen Worden, William Y. Y. Cheng, Vincent Huijnen, and Gerbrand Koren
Atmos. Chem. Phys., 25, 2243–2268, https://doi.org/10.5194/acp-25-2243-2025, https://doi.org/10.5194/acp-25-2243-2025, 2025
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Five global chemical reanalysis datasets were used to assess the relative impacts of assimilating satellite ozone and its precursor measurements on tropospheric ozone analyses for 2010. The multiple reanalysis system comparison allows an evaluation of the dependency of the impacts on different reanalysis systems. The results suggested the importance of satellite ozone and its precursor measurements for improving ozone analysis in the whole troposphere, with varying magnitudes among the systems.
Maureen Beaudor, Didier Hauglustaine, Juliette Lathière, Martin Van Damme, Lieven Clarisse, and Nicolas Vuichard
Atmos. Chem. Phys., 25, 2017–2046, https://doi.org/10.5194/acp-25-2017-2025, https://doi.org/10.5194/acp-25-2017-2025, 2025
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Agriculture is the biggest ammonia (NH3) source, impacting air quality, climate, and ecosystems. Because of food demand, NH3 emissions are projected to rise by 2100. Using a global model, we analyzed the impact of present and future NH3 emissions generated from a land model. Our results show improved ammonia patterns compared to a reference inventory. Future scenarios predict up to 70 % increase in global NH3 burden, with significant changes in radiative forcing that can greatly elevate N2O.
Hui Li, Jiaxin Qiu, and Bo Zheng
Atmos. Chem. Phys., 25, 1949–1963, https://doi.org/10.5194/acp-25-1949-2025, https://doi.org/10.5194/acp-25-1949-2025, 2025
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We conduct a sensitivity analysis with 31 tests on various factors including prior emissions, model resolution, satellite constraint, and other system configurations to assess the vulnerability of emission estimates across temporal, sectoral, and regional dimensions. This reveals the robustness of emissions estimated by this air-pollution-satellite-based CO2 emission inversion system, with relative change between tests and base inversion below 4.0 % for national annual NOx and CO2 emissions.
Yuqing Qiu, Xin Li, Wenxuan Chai, Yi Liu, Mengdi Song, Xudong Tian, Qiaoli Zou, Wenjun Lou, Wangyao Zhang, Juan Li, and Yuanhang Zhang
Atmos. Chem. Phys., 25, 1749–1763, https://doi.org/10.5194/acp-25-1749-2025, https://doi.org/10.5194/acp-25-1749-2025, 2025
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The chemical reactions of ozone (O3) formation are related to meteorology and local emissions. Here, a random forest approach was used to eliminate the effects of meteorological factors (dispersion or transport) on O3 and its precursors. Variations in the sensitivity of O3 formation and the apportionment of emission sources were revealed after meteorological normalization. Our results suggest that meteorological variations should be considered when diagnosing O3 formation.
Jeongmin Yun, Junjie Liu, Brendan Byrne, Brad Weir, Lesley E. Ott, Kathryn McKain, Bianca C. Baier, Luciana V. Gatti, and Sebastien C. Biraud
Atmos. Chem. Phys., 25, 1725–1748, https://doi.org/10.5194/acp-25-1725-2025, https://doi.org/10.5194/acp-25-1725-2025, 2025
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This study quantifies errors in regional net surface–atmosphere CO2 flux estimates from an inverse model ensemble using airborne CO2 measurements. Our results show that flux error estimates based on observations significantly exceed those computed from the ensemble spread of flux estimates in regions with high fossil fuel emissions. This finding suggests the presence of systematic biases in the inversion estimates, associated with errors in the fossil fuel emissions common to all models.
Min Huang, Gregory R. Carmichael, Kevin W. Bowman, Isabelle De Smedt, Andreas Colliander, Michael H. Cosh, Sujay V. Kumar, Alex B. Guenther, Scott J. Janz, Ryan M. Stauffer, Anne M. Thompson, Niko M. Fedkin, Robert J. Swap, John D. Bolten, and Alicia T. Joseph
Atmos. Chem. Phys., 25, 1449–1476, https://doi.org/10.5194/acp-25-1449-2025, https://doi.org/10.5194/acp-25-1449-2025, 2025
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We use model simulations along with multiplatform, multidisciplinary observations and a range of analysis methods to estimate and understand the distributions, temporal changes, and impacts of reactive nitrogen and ozone over the most populous US region that has undergone significant environmental changes. Deposition, biogenic emissions, and extra-regional sources have been playing increasingly important roles in controlling pollutant budgets in this area as local anthropogenic emissions drop.
Xavier Faïn, Sophie Szopa, Vaishali Naïk, Patricia Martinerie, David M. Etheridge, Rachael H. Rhodes, Cathy M. Trudinger, Vasilii V. Petrenko, Kévin Fourteau, and Philip Place
Atmos. Chem. Phys., 25, 1105–1119, https://doi.org/10.5194/acp-25-1105-2025, https://doi.org/10.5194/acp-25-1105-2025, 2025
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Carbon monoxide (CO) plays a crucial role in the atmosphere's oxidizing capacity. In this study, we analyse how historical (1850–2014) [CO] outputs from state-of-the-art global chemistry–climate models over Greenland and Antarctica are able to capture both absolute values and trends recorded in multi-site ice archives. A disparity in [CO] growth rates emerges in the Northern Hemisphere between models and observations from 1920–1975 CE, possibly linked to uncertainties in CO emission factors.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonné, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, https://doi.org/10.5194/acp-25-1063-2025, 2025
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Processes influencing dispersion of local anthropogenic pollution in Arctic wintertime are investigated with Lagrangian dispersion modelling. Simulated power plant plume rise that considers temperature inversion layers improves results compared to observations (interior Alaska). Modelled surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching −35°C are required to reproduce observed NOx.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
Atmos. Chem. Phys., 25, 1121–1143, https://doi.org/10.5194/acp-25-1121-2025, https://doi.org/10.5194/acp-25-1121-2025, 2025
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In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking, are increasingly important and impact air quality. This study uses a box model to evaluate how these emissions impact ozone in the Los Angeles Basin and quantifies the impact of gaseous cooking emissions. Accurate representation of these and other anthropogenic sources in inventories is crucial for informing effective air quality policies.
Xiaodan Ma, Jianping Huang, Michaela I. Hegglin, Patrick Jöckel, and Tianliang Zhao
Atmos. Chem. Phys., 25, 943–958, https://doi.org/10.5194/acp-25-943-2025, https://doi.org/10.5194/acp-25-943-2025, 2025
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Our research explored changes in ozone levels in the northwest Pacific region over 30 years, revealing a significant increase in the middle-to-upper troposphere, especially during spring and summer. This rise is influenced by both stratospheric and tropospheric sources, which affect climate and air quality in East Asia. This work underscores the need for continued study to understand underlying mechanisms.
Hiroo Hata, Norifumi Mizushima, and Tomohiko Ihara
Atmos. Chem. Phys., 25, 1037–1061, https://doi.org/10.5194/acp-25-1037-2025, https://doi.org/10.5194/acp-25-1037-2025, 2025
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The introduction of battery electric vehicles (BEVs) is expected to reduce the primary air pollutants from vehicular exhaust and evaporative emissions while reducing the anthropogenic heat produced by vehicles, ultimately mitigating the urban heat island (UHI) effect. This study revealed the impact of introducing BEVs on the decrease in the UHI effect and the impact of BEVs on the formation of tropospheric ozone and fine particulate matter in the Greater Tokyo Area of Japan.
Ji Xia, Yi Zhou, Li Fang, Yingfei Qi, Dehao Li, Hong Liao, and Jianbing Jin
EGUsphere, https://doi.org/10.5194/egusphere-2024-3938, https://doi.org/10.5194/egusphere-2024-3938, 2025
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This study established an ammonia emission inventory in South Asia via assimilation-based inversion system. The posterior emissions, calculated by integrating the CEDS inventory and IASI satellite observations, showed significant improvement over the prior. Validation against various measurements all support our posterior emission. It offers valuable insights of ammonia emissions for policymakers and researchers aiming to develop air quality management and mitigation strategies there.
Catalina Poraicu, Jean-François Müller, Trissevgeni Stavrakou, Crist Amelynck, Bert W. D. Verreyken, Niels Schoon, Corinne Vigouroux, Nicolas Kumps, Jérôme Brioude, Pierre Tulet, and Camille Mouchel-Vallon
EGUsphere, https://doi.org/10.5194/egusphere-2024-3555, https://doi.org/10.5194/egusphere-2024-3555, 2025
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We investigated the sources and impacts of nitrogen oxides and organic compounds over a remote tropical island. High-resolution WRF-Chem simulations were evaluated using in situ, FTIR and satellite measurements. This work highlights gaps in current models, like missing sources of key organic compounds and inaccuracies in emission inventories, emphasizing the importance of improving chemical and dynamical processes in atmospheric modelling for budget estimates in tropical regions.
Carlos Gómez-Ortiz, Guillaume Monteil, Sourish Basu, and Marko Scholze
Atmos. Chem. Phys., 25, 397–424, https://doi.org/10.5194/acp-25-397-2025, https://doi.org/10.5194/acp-25-397-2025, 2025
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In this paper, we test new implementations of our inverse modeling tool to estimate the weekly and regional CO2 emissions from fossil fuels in Europe. We use synthetic atmospheric observations of CO2 and radiocarbon (14CO2) to trace emissions to their sources, while separating the natural and fossil CO2. Our tool accurately estimates fossil CO2 emissions in densely monitored regions like western/central Europe. This approach aids in developing strategies for reducing CO2 emissions.
David D. Parrish, Ian C. Faloona, and Richard G. Derwent
Atmos. Chem. Phys., 25, 263–289, https://doi.org/10.5194/acp-25-263-2025, https://doi.org/10.5194/acp-25-263-2025, 2025
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Observation-based estimates of contributions to maximum ozone (O3) concentrations show that background O3 can exceed the air quality standard of 70 ppb in the southwestern US, precluding standard attainment. Over the past 4 decades, US anthropogenic O3 has decreased by a factor of ~ 6.3, while wildfire contributions have increased, so that the background now dominates maximum concentrations, even in Los Angeles, and the occurrence of maximum O3 has shifted from the eastern to the western US.
William P. L. Carter, Jia Jiang, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 25, 199–242, https://doi.org/10.5194/acp-25-199-2025, https://doi.org/10.5194/acp-25-199-2025, 2025
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This paper describes the scientific basis for gas-phase atmospheric chemical mechanisms derived using the SAPRC mechanism generation system, MechGen. It can derive mechanisms for most organic compounds with C, H, O, or N atoms, including initial reactions of organics with OH, O3, NO3, and O3P or by photolysis, as well as the reactions of the various types of intermediates that are formed. The paper includes a description of areas of uncertainty where additional research and updates are needed.
Thibaut Lebourgeois, Bastien Sauvage, Pawel Wolff, Béatrice Josse, Virginie Marécal, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Jean-Marc Cousin, Philippe Nedelec, and Valérie Thouret
Atmos. Chem. Phys., 24, 13975–14004, https://doi.org/10.5194/acp-24-13975-2024, https://doi.org/10.5194/acp-24-13975-2024, 2024
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Our study examines intense-carbon-monoxide (CO) pollution events measured by commercial aircraft from the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. We combine these measurements with the SOFT-IO model to trace the origin of the observed CO. A comprehensive analysis of the geographical origin, source type, seasonal variation, and ozone levels of these pollution events is provided.
Xiao Lu, Yiming Liu, Jiayin Su, Xiang Weng, Tabish Ansari, Yuqiang Zhang, Guowen He, Yuqi Zhu, Haolin Wang, Ganquan Zeng, Jingyu Li, Cheng He, Shuai Li, Teerachai Amnuaylojaroen, Tim Butler, Qi Fan, Shaojia Fan, Grant L. Forster, Meng Gao, Jianlin Hu, Yugo Kanaya, Mohd Talib Latif, Keding Lu, Philippe Nédélec, Peer Nowack, Bastien Sauvage, Xiaobin Xu, Lin Zhang, Ke Li, Ja-Ho Koo, and Tatsuya Nagashima
EGUsphere, https://doi.org/10.5194/egusphere-2024-3702, https://doi.org/10.5194/egusphere-2024-3702, 2024
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This study analyzes summertime ozone trends in East and Southeast Asia derived from a comprehensive observational database spanning from 1995 to 2019, incorporating aircraft observations, ozonesonde data, and measurements from 2500 surface sites. Multiple models are applied to attribute to changes in anthropogenic emissions and climate. The results highlight increases in anthropogenic emission are the primary driver of ozone increases both in the free troposphere and at the surface.
Hassnae Erraji, Philipp Franke, Astrid Lampert, Tobias Schuldt, Ralf Tillmann, Andreas Wahner, and Anne Caroline Lange
Atmos. Chem. Phys., 24, 13913–13934, https://doi.org/10.5194/acp-24-13913-2024, https://doi.org/10.5194/acp-24-13913-2024, 2024
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Four-dimensional variational data assimilation allows for the simultaneous optimisation of initial values and emission rates by using trace-gas profiles from drone observations in a regional air quality model. Assimilated profiles positively impact the representation of air pollutants in the model by improving their vertical distribution and ground-level concentrations. This case study highlights the potential of drone data to enhance air quality analyses including local emission evaluation.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
Atmos. Chem. Phys., 24, 13693–13713, https://doi.org/10.5194/acp-24-13693-2024, https://doi.org/10.5194/acp-24-13693-2024, 2024
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This work uses chemical transport and box modeling to study the gas- and aqueous-phase production of organic acid concentrations measured in cloud water at the summit of Whiteface Mountain on 1 July 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas-phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Francisco J. Pérez-Invernón, Francisco J. Gordillo-Vázquez, Heidi Huntrieser, Patrick Jöckel, and Eric J. Bucsela
EGUsphere, https://doi.org/10.5194/egusphere-2024-3348, https://doi.org/10.5194/egusphere-2024-3348, 2024
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Lightning plays a significant role in tropospheric chemistry by producing substantial amounts of nitrogen oxides. According to recent estimates, thunderstorms that produce a higher lightning frequency rate also produce less nitrogen oxide per flash. We implemented the dependency of nitrogen oxide production per flash on lightning flash frequency in a chemical atmospheric model.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
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Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
Kai-Lan Chang, Brian C. McDonald, and Owen R. Cooper
EGUsphere, https://doi.org/10.5194/egusphere-2024-3674, https://doi.org/10.5194/egusphere-2024-3674, 2024
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Exposure to high levels of ozone can be harmful to human health. This study shows consistent and robust evidence of decreasing ozone extremes across much of the United States over 1990–2023, previously attributed to ozone precursor emission controls. Nevertheless, we also show that the increasing heatwave frequencies are likely to contribute to additional ozone exceedances, slowing the progress of decreasing the frequency of ozone exceedances.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William R. Stockwell, Luc Vereecken, and Timothy J. Wallington
Atmos. Chem. Phys., 24, 13317–13339, https://doi.org/10.5194/acp-24-13317-2024, https://doi.org/10.5194/acp-24-13317-2024, 2024
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Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes in the atmospheric composition. Therefore, accurate chemical mechanisms are necessary to predict the evolution of air pollution and climate change. The article describes all steps that are needed to build chemical mechanisms and discusses the advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
Audrey Fortems-Cheiney, Grégoire Broquet, Robin Plauchu, Elise Potier, Antoine Berchet, Isabelle Pison, Adrien Martinez, Rimal Abeed, Gaelle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, Henk Eskes, Hugo A. C. Denier van der Gon, and Stijn N. C. Dellaert
EGUsphere, https://doi.org/10.5194/egusphere-2024-3679, https://doi.org/10.5194/egusphere-2024-3679, 2024
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This study assesses the potential of the OMI and TROPOMI satellite observations to inform about the evolution of NOx anthropogenic emissions between year 2005 and year 2019 at the regional to national scales in Europe. Both the OMI and TROPOMI inversions show decreases in European NOx anthropogenic emission budgets between 2005 and 2019, but with different magnitudes.
Yawen Kong, Bo Zheng, and Yuxi Liu
EGUsphere, https://doi.org/10.5194/egusphere-2024-2996, https://doi.org/10.5194/egusphere-2024-2996, 2024
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Current high-resolution satellite remote sensing technologies provide a unique opportunity to derive timely, high-resolution emission data. We developed an emission inversion system to assimilate satellite NO2 data to obtain daily, kilometer-scale NOx emission inventories. Our results enhance inventory accuracy, allowing us to capture the effects of pollution control policies on daily emissions (e.g., during COVID-19 lockdown) and improve fine-scale air quality modeling.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 24, 12943–12962, https://doi.org/10.5194/acp-24-12943-2024, https://doi.org/10.5194/acp-24-12943-2024, 2024
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This paper employs a regional chemical transport model to quantify the sensitivity of air pollutants and photochemical parameters to specified emission reductions in China for representative winter and summer conditions. The study provides insights into further air quality control in China with reduced primary emissions.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Baoshuang Liu, Yao Gu, Yutong Wu, Qili Dai, Shaojie Song, Yinchang Feng, and Philip K. Hopke
Atmos. Chem. Phys., 24, 12861–12879, https://doi.org/10.5194/acp-24-12861-2024, https://doi.org/10.5194/acp-24-12861-2024, 2024
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Reactive loss of volatile organic compounds (VOCs) is a long-term issue yet to be resolved in VOC source analyses. We assess common methods of, and existing issues in, reducing losses, impacts of losses, and sources in current source analyses. We offer a potential supporting role for solving issues of VOC conversion. Source analyses of consumed VOCs that reacted to produce ozone and secondary organic aerosols can play an important role in the effective control of secondary pollution in air.
Deepangsu Chatterjee, Randall V. Martin, Chi Li, Dandan Zhang, Haihui Zhu, Daven K. Henze, James H. Crawford, Ronald C. Cohen, Lok N. Lamsal, and Alexander M. Cede
Atmos. Chem. Phys., 24, 12687–12706, https://doi.org/10.5194/acp-24-12687-2024, https://doi.org/10.5194/acp-24-12687-2024, 2024
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We investigate the hourly variation of NO2 columns and surface concentrations by applying the GEOS-Chem model to interpret aircraft and ground-based measurements over the US and Pandora sun photometer measurements over the US, Europe, and Asia. Corrections to the Pandora columns and finer model resolution improve the modeled representation of the summertime hourly variation of total NO2 columns to explain the weaker hourly variation in NO2 columns than at the surface.
Kiyeon Kim, Kyung Man Han, Chul Han Song, Hyojun Lee, Ross Beardsley, Jinhyeok Yu, Greg Yarwood, Bonyoung Koo, Jasper Madalipay, Jung-Hun Woo, and Seogju Cho
Atmos. Chem. Phys., 24, 12575–12593, https://doi.org/10.5194/acp-24-12575-2024, https://doi.org/10.5194/acp-24-12575-2024, 2024
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We incorporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratio predictions. These results expand our understanding of HONO photochemistry and identify crucial sources of HONO that impact the total HONO budget in Seoul, South Korea. Through this investigation, we contribute to resolving discrepancies in understanding chemical transport models, with implications for better air quality management and environmental protection in the region.
Flossie Brown, Gerd Folberth, Stephen Sitch, Paulo Artaxo, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Matteo Detto, Ninong Komala, Luciana Rizzo, Nestor Rojas, Ines dos Santos Vieira, Steven Turnock, Hans Verbeeck, and Alfonso Zambrano
Atmos. Chem. Phys., 24, 12537–12555, https://doi.org/10.5194/acp-24-12537-2024, https://doi.org/10.5194/acp-24-12537-2024, 2024
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Ozone is a pollutant that is detrimental to human and plant health. Ozone monitoring sites in the tropics are limited, so models are often used to understand ozone exposure. We use measurements from the tropics to evaluate ozone from the UK Earth system model, UKESM1. UKESM1 is able to capture the pattern of ozone in the tropics, except in southeast Asia, although it systematically overestimates it at all sites. This work highlights that UKESM1 can capture seasonal and hourly variability.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys., 24, 12495–12507, https://doi.org/10.5194/acp-24-12495-2024, https://doi.org/10.5194/acp-24-12495-2024, 2024
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Climate change will bring about changes in parameters that are currently used in global-scale models to calculate biogenic emissions. This study seeks to understand the factors driving these models by comparing long-term datasets of biogenic compounds to modeled emissions. We note that the light-dependent fractions currently used in models do not accurately represent regional observations. We provide evidence for the time-dependent variation in this parameter for future modifications to models.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyoung Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
Atmos. Chem. Phys., 24, 12465–12493, https://doi.org/10.5194/acp-24-12465-2024, https://doi.org/10.5194/acp-24-12465-2024, 2024
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We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show that SF6 emissions are decreasing in the USA and in the EU, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, EU, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
Dominika Pasik, Thomas Golin Almeida, Emelda Ahongshangbam, Siddharth Iyer, and Nanna Myllys
EGUsphere, https://doi.org/10.5194/egusphere-2024-3464, https://doi.org/10.5194/egusphere-2024-3464, 2024
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We used quantum chemistry methods to investigate the oxidation mechanisms of acyl peroxy radicals (APRs) with various monoterpenes. Our findings reveal unique oxidation pathways for different monoterpenes, leading to either chain-terminating products or highly reactive intermediates that can contribute to particle formation in the atmosphere. This research highlights APRs as potentially significant but underexplored atmospheric oxidants, which may influence future approaches to modeling climate.
Yasin Elshorbany, Jerald R. Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo J. Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca R. Buchholz, Benjamin Gaubert, Néstor Y. Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
Atmos. Chem. Phys., 24, 12225–12257, https://doi.org/10.5194/acp-24-12225-2024, https://doi.org/10.5194/acp-24-12225-2024, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the tropospheric column of ozone and its precursors, nitrogen dioxide, formaldehyde, and total column CO, as well as ozonesonde data and model simulations.
Sanhita Ghosh, Arineh Cholakian, Sylvain Mailler, and Laurent Menut
EGUsphere, https://doi.org/10.5194/egusphere-2024-3087, https://doi.org/10.5194/egusphere-2024-3087, 2024
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In the study, we estimate the emissions of nitrogen oxides from lightning (LNOx) over the northern hemisphere and study its impact on tropospheric ozone (O3). We evaluate the present state of modelling the lightning, using a classical parametrization scheme and the model CHIMERE. The comparison of the simulated O3 to measurements shows that the inclusion of LNOx emissions remarkably improves the tropospheric O3 distribution, reducing the bias significantly, particularly in the free troposphere.
Ragnhild Bieltvedt Skeie, Marit Sandstad, Srinath Krishnan, Gunnar Myhre, and Maria Sand
EGUsphere, https://doi.org/10.5194/egusphere-2024-3079, https://doi.org/10.5194/egusphere-2024-3079, 2024
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Hydrogen leakages can alter the amount of climate gases in the atmosphere and hence have a climate impact. In this study we investigate, using an atmospheric chemistry model, how this indirect climate effect differs for different amounts of leakages, where the hydrogen leaks and if this effect changes in the future. The effect is largest for emissions far from areas where hydrogen is removed from the atmosphere by the soil, but these are not relevant locations for a future hydrogen economy.
Mariano Mertens, Sabine Brinkop, Phoebe Graf, Volker Grewe, Johannes Hendricks, Patrick Jöckel, Anna Lanteri, Sigrun Matthes, Vanessa S. Rieger, Mattia Righi, and Robin N. Thor
Atmos. Chem. Phys., 24, 12079–12106, https://doi.org/10.5194/acp-24-12079-2024, https://doi.org/10.5194/acp-24-12079-2024, 2024
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We quantified the contributions of land transport, shipping, and aviation emissions to tropospheric ozone; its radiative forcing; and the reductions of the methane lifetime using chemistry-climate model simulations. The contributions were analysed for the conditions of 2015 and for three projections for the year 2050. The results highlight the challenges of mitigating ozone formed by emissions of the transport sector, caused by the non-linearitiy of the ozone chemistry and the long lifetime.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Siting Li, Yiming Liu, Yuqi Zhu, Yinbao Jin, Yingying Hong, Ao Shen, Yifei Xu, Haofan Wang, Haichao Wang, Xiao Lu, Shaojia Fan, and Qi Fan
Atmos. Chem. Phys., 24, 11521–11544, https://doi.org/10.5194/acp-24-11521-2024, https://doi.org/10.5194/acp-24-11521-2024, 2024
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This study establishes an inventory of anthropogenic chlorine emissions in China in 2019 with expanded species (HCl, Cl-, Cl2, HOCl) and sources (41 specific sources). The inventory is validated by a modeling study against the observations. This study enhances the understanding of anthropogenic chlorine emissions in the atmosphere, identifies key sources, and provides scientific support for pollution control and climate change.
Willem E. van Caspel, Zbigniew Klimont, Chris Heyes, and Hilde Fagerli
Atmos. Chem. Phys., 24, 11545–11563, https://doi.org/10.5194/acp-24-11545-2024, https://doi.org/10.5194/acp-24-11545-2024, 2024
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Methane in the atmosphere contributes to the production of ozone gas – an air pollutant and greenhouse gas. Our results highlight that simultaneous reductions in methane emissions help avoid offsetting the air pollution benefits already achieved by the already-approved precursor emission reductions by 2050 in the European Monitoring and Evaluation Programme region, while also playing an important role in bringing air pollution further down towards World Health Organization guideline limits.
Yujia Wang, Hongbin Wang, Bo Zhang, Peng Liu, Xinfeng Wang, Shuchun Si, Likun Xue, Qingzhu Zhang, and Qiao Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2791, https://doi.org/10.5194/egusphere-2024-2791, 2024
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This study established a bottom-up approach that employs real-time traffic flows and interpolation to obtain a spatially continuous on-road vehicle emission mapping for the main urban area of Jinan. The diurnal variation, spatial distribution, and emission hotspots were analyzed with clustering and hotspot analysis, showing unique fine-scale variation characteristics of on-road vehicle emissions. Future scenario analysis demonstrates remarkable benefits of electrification on emission reduction.
Laura Stecher, Franziska Winterstein, Patrick Jöckel, Michael Ponater, Mariano Mertens, and Martin Dameris
EGUsphere, https://doi.org/10.5194/egusphere-2024-2938, https://doi.org/10.5194/egusphere-2024-2938, 2024
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Methane, the second most important anthropogenic greenhouse gas, is chemically decomposed in the atmosphere. The chemical sink of atmospheric methane is not constant, but depends on the temperature and on the abundance of its reaction partners. In this study, we use a global chemistry-climate model to assess the feedback of atmospheric methane induced by changes of the chemical sink in a warming climate, and its implications for the chemical composition and the surface air temperature change.
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Brooks, S., Ren, X., Cohen, M., Luke, W. T., Kelley, P., Artz, R., Hynes, A., Landing, W., and Martos, B.: Airborne Vertical Profiling of Mercury Speciation near Tullahoma, TN, USA, Atmosphere, 5, 557–574, https://doi.org/10.3390/atmos5030557, 2014.
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Cobbett, F. D., Steffen, A., Lawson, G., and Heyst, B. J. V.: GEM fluxes and atmospheric mercury concentrations (GEM, RGM and PBM) in the Canadian Arctic at Alert, Nunavut, Canada (February–June 2005), Atmos. Environ., 41, 6527–6543, https://doi.org/10.1016/j.atmosenv.2007.04.033, 2007.
Coburn, S., Dix, B., Edgerton, E., Holmes, C. D., Kinnison, D., Liang, Q., ter Schure, A., Wang, S., and Volkamer, R.: Mercury oxidation from bromine chemistry in the free troposphere over the southeastern US, Atmos. Chem. Phys., 16, 3743–3760, https://doi.org/10.5194/acp-16-3743-2016, 2016.
Dastoor, A. P. and Larocque, Y.: Global circulation of atmospheric mercury: a modelling study, Atmos. Environ., 38, 147–161, https://doi.org/10.1016/j.atmosenv.2003.08.037, 2004.
de Foy, B., Tong, Y., Yin, X., Zhang, W., Kang, S., Zhang, Q., Zhang, G., Wang, X., and Schauer, J. J.: First field-based atmospheric observation of the reduction of reactive mercury driven by sunlight, Atmos. Environ., 134, 27–39, https://doi.org/10.1016/j.atmosenv.2016.03.028, 2016.
Dibble, T. S., Zelie, M. J., and Mao, H.: Thermodynamics of reactions of ClHg and BrHg radicals with atmospherically abundant free radicals, Atmos. Chem. Phys., 12, 10271–10279, https://doi.org/10.5194/acp-12-10271-2012, 2012.
Donohoue, D. L., Bauer, D., Cossairt, B., and Hynes, A. J.: Temperature and pressure dependent rate coefficients for the reaction of Hg with Br and the reaction of Br with Br: A pulsed laser photolysis-pulsed laser induced fluorescence study, J. Phys. Chem. A, 110, 6623–6632, https://doi.org/10.1021/jp054688j, 2006.
Ebinghaus, R., Kock, H. H., Temme, C., Einax, J. W., Löwe, A. G., Richter, A., Burrows, J. P., and Schroeder, W. H.: Antarctic Springtime Depletion of Atmospheric Mercury, Environ. Sci. Technol., 36, 1238–1244, https://doi.org/10.1021/es015710z, 2002.
Edgerton, E. S., Hartsell, B. E., and Jansen, J. J.: Mercury Speciation in Coal-fired Power Plant Plumes Observed at Three Surface Sites in the Southeastern U.S., Environ. Sci. Technol., 40, 4563–4570, https://doi.org/10.1021/es0515607, 2006.
Faïn, X., Obrist, D., Hallar, A. G., Mccubbin, I., and Rahn, T.: High levels of reactive gaseous mercury observed at a high elevation research laboratory in the Rocky Mountains, Atmos. Chem. Phys., 9, 8049–8060, https://doi.org/10.5194/acp-9-8049-2009, 2009.
Fu, X., Feng, X., Sommar, J., and Wang, S.: A review of studies on atmospheric mercury in China, Sci. Total Environ., 421–422, 73–81, https://doi.org/10.1016/j.scitotenv.2011.09.089, 2012.
Fu, X., Marusczak, N., Heimbürger, L.-E., Sauvage, B., Gheusi, F., Prestbo, E. M., and Sonke, J. E.: Atmospheric mercury speciation dynamics at the high-altitude Pic du Midi Observatory, southern France, Atmos. Chem. Phys., 16, 5623–5639, https://doi.org/10.5194/acp-16-5623-2016, 2016a.
Fu, X., Yang, X., Lang, X., Zhou, J., Zhang, H., Yu, B., Yan, H., Lin, C.-J., and Feng, X.: Atmospheric wet and litterfall mercury deposition at urban and rural sites in China, Atmos. Chem. Phys., 16, 11547–11562, https://doi.org/10.5194/acp-16-11547-2016, 2016b.
Fu, X. W., Zhang, H., Yu, B., Wang, X., Lin, C.-J., and Feng, X. B.: Observations of atmospheric mercury in China: a critical review, Atmos. Chem. Phys., 15, 9455–9476, https://doi.org/10.5194/acp-15-9455-2015, 2015.
Gay, D. A., Schmeltz, D., Prestbo, E., Olson, M., Sharac, T., and Tordon, R.: The Atmospheric Mercury Network: measurement and initial examination of an ongoing atmospheric mercury record across North America, Atmos. Chem. Phys., 13, 11339–11349, https://doi.org/10.5194/acp-13-11339-2013, 2013.
Goodsite, M. E., Plane, J. M. C., and Skov, H.: A Theoretical Study of the Oxidation of Hg0 to HgBr2 in the Troposphere, Environ. Sci. Technol., 38, 1772–1776, https://doi.org/10.1021/es034680s, 2004.
Gratz, L. E., Keeler, G. J., and Miller, E. K.: Long-term relationships between mercury wet deposition and meteorology, Atmos. Environ., 43, 6218–6229, https://doi.org/10.1016/j.atmosenv.2009.08.040, 2009.
Gratz, L. E., Ambrose, J. L., Jaffe, D. A., Shah, V., Jaeglé, L., Stutz, J., Festa, J., Spolaor, M., Tsai, C., Selin, N. E., Song, S., Zhou, X., Weinheimer, A. J., Knapp, D. J., Montzka, D. D., Flocke, F. M., Campos, T. L., Apel, E., Hornbrook, R., Blake, N. J., Hall, S., Tyndall, G. S., Reeves, M., Stechman, D., and Stell, M.: Oxidation of mercury by bromine in the subtropical Pacific free troposphere, Geophys. Res. Lett., 42, 10494–10502, https://doi.org/10.1002/2015GL066645, 2015.
Guentzel, J. L., Landing, W. M., Gill, G. A., and Pollman, C. D.: Processes Influencing Rainfall Deposition of Mercury in Florida, Environ. Sci. Technol., 35, 863–873, https://doi.org/10.1021/es001523+, 2001.
Gustin, M. S., Weiss-Penzias, P. S., and Peterson, C.: Investigating sources of gaseous oxidized mercury in dry deposition at three sites across Florida, USA, Atmos. Chem. Phys., 12, 9201–9219, https://doi.org/10.5194/acp-12-9201-2012, 2012.
Gustin, M. S., Amos, H. M., Huang, J., Miller, M. B., and Heidecorn, K.: Measuring and modeling mercury in the atmosphere: a critical review, Atmos. Chem. Phys., 15, 5697–5713, https://doi.org/10.5194/acp-15-5697-2015, 2015.
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Hammerschmidt, C. R. and Fitzgerald, W. F.: Methylmercury in Freshwater Fish Linked to Atmospheric Mercury Deposition, Environ. Sci. Technol., 40, 7764–7770, https://doi.org/10.1021/es061480i, 2006.
Harris, R. C., Rudd, J. W. M., Amyot, M., Babiarz, C. L., Beaty, K. G., Blanchfield, P. J., Bodaly, R. A., Branfireun, B. A., Gilmour, C. C., Graydon, J. A., Heyes, A., Hintelmann, H., Hurley, J. P., Kelly, C. A., Krabbenhoft, D. P., Lindberg, S. E., Mason, R. P., Paterson, M. J., Podemski, C. L., Robinson, A., Sandilands, K. A., Southworth, G. R., St. Louis, V. L., and Tate, M. T.: Whole-ecosystem study shows rapid fish-mercury response to changes in mercury deposition, P. Natl. Acad. Sci. USA, 104, 16586–16591, https://doi.org/10.1073/pnas.0704186104, 2007.
Holmes, C. D., Jacob, D. J., Mason, R. P., and Jaffe, D. A.: Sources and deposition of reactive gaseous mercury in the marine atmosphere, Atmos. Environ., 43, 2278–2285, https://doi.org/10.1016/j.atmosenv.2009.01.051, 2009.
Holmes, C. D., Jacob, D. J., Corbitt, E. S., Mao, J., Yang, X., Talbot, R., and Slemr, F.: Global atmospheric model for mercury including oxidation by bromine atoms, Atmos. Chem. Phys., 10, 12037–12057, https://doi.org/10.5194/acp-10-12037-2010, 2010.
Holmes, C. D., Krishnamurthy, N. P., Caffrey, J. M., Landing, W. M., Edgerton, E. S., Knapp, K. R., and Nair, U. S.: Thunderstorms Increase Mercury Wet Deposition, Environ. Sci. Technol., 50, 9343–9350, https://doi.org/10.1021/acs.est.6b02586, 2016.
Huang, J. and Gustin, M. S.: Evidence for a Free Troposphere Source of Mercury in Wet Deposition in the Western United States, Environ. Sci. Technol., 46, 6621–6629, https://doi.org/10.1021/es3005915, 2012.
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Jaeglé, L., Strode, S. A., Selin, N. E., and Jacob, D. J.: The Geos-Chem model, in: Mercury Fate and Transport in the Global Atmosphere: Emissions, Measurements and Models, edited by: Mason, R. and Pirrone, N., 533–545, Springer US, Boston, MA, 2009.
Jung, G., Hedgecock, I. M., and Pirrone, N.: ECHMERIT V1.0 – a new global fully coupled mercury-chemistry and transport model, Geosci. Model Dev., 2, 175–195, https://doi.org/10.5194/gmd-2-175-2009, 2009.
Kaulfus, A. S., Nair, U., Holmes, C. D., and Landing, W. M.: Mercury Wet Scavenging and Deposition Differences by Precipitation Type, Environ. Sci. Technol., 51, 2628–2634, https://doi.org/10.1021/acs.est.6b04187, 2017.
Kim, J.-H., Park, J.-M., Lee, S.-B., Pudasainee, D., and Seo, Y.-C.: Anthropogenic mercury emission inventory with emission factors and total emission in Korea, Atmos. Environ., 44, 2714–2721, https://doi.org/10.1016/j.atmosenv.2010.04.037, 2010.
Kos, G., Ryzhkov, A., Dastoor, A., Narayan, J., Steffen, A., Ariya, P. A., and Zhang, L.: Evaluation of discrepancy between measured and modelled oxidized mercury species, Atmos. Chem. Phys., 13, 4839–4863, https://doi.org/10.5194/acp-13-4839-2013, 2013.
Kwon, S. Y. and Selin, N. E.: Uncertainties in Atmospheric Mercury Modeling for Policy Evaluation, Curr. Pollut. Rep., 2, 103–114, https://doi.org/10.1007/s40726-016-0030-8, 2016.
Landis, M. S., Ryan, J. V., ter Schure, A. F. H., and Laudal, D.: Behavior of Mercury Emissions from a Commercial Coal-Fired Power Plant: The Relationship between Stack Speciation and Near-Field Plume Measurements, Environ. Sci. Technol., 48, 13540–13548, https://doi.org/10.1021/es500783t, 2014.
Laurier, F. J. G., Mason, R. P., Whalin, L., and Kato, S.: Reactive gaseous mercury formation in the North Pacific Ocean's marine boundary layer: A potential role of halogen chemistry, J. Geophys. Res.-Atmos., 108, 4529, https://doi.org/10.1029/2003JD003625, 2003.
Lin, J.-T. and McElroy, M. B.: Impacts of boundary layer mixing on pollutant vertical profiles in the lower troposphere: Implications to satellite remote sensing, Atmos. Environ., 44, 1726–1739, https://doi.org/10.1016/j.atmosenv.2010.02.009, 2010.
Lin, S.-J. and Rood, R. B.: Multidimensional flux-form semi-Lagrangian transport schemes, Mon. Weather Rev., 124, 2046–2070, https://doi.org/10.1175/1520-0493(1996)124<2046:MFFSLT>2.0.CO;2, 1996.
Lindberg, S. E., Brooks, S., Lin, C.-J., Scott, K. J., Landis, M. S., Stevens, R. K., Goodsite, M., and Richter, A.: Dynamic Oxidation of Gaseous Mercury in the Arctic Troposphere at Polar Sunrise, Environ. Sci. Technol., 36, 1245–1256, https://doi.org/10.1021/es0111941, 2002.
Liu, H., Jacob, D. J., Bey, I., and Yantosca, R. M.: Constraints from 210Pb and 7Be on wet deposition and transport in a global three-dimensional chemical, J. Geophys. Res., 106, 12109–12128, https://doi.org/10.1029/2000JD900839, 2001.
Lyman, S. N. and Gustin, M. S.: Determinants of atmospheric mercury concentrations in Reno, Nevada, U.S.A., Sci. Total Environ., 408, 431–438, https://doi.org/10.1016/j.scitotenv.2009.09.045, 2009.
Lyman, S. N. and Jaffe, D. A.: Formation and fate of oxidized mercury in the upper troposphere and lower stratosphere, Nat. Geosci, 5, 114–117, https://doi.org/10.1038/ngeo1353, 2012.
Lyman, S. N., Jaffe, D. A., and Gustin, M. S.: Release of mercury halides from KCl denuders in the presence of ozone, Atmos. Chem. Phys., 10, 8197–8204, https://doi.org/10.5194/acp-10-8197-2010, 2010.
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Short summary
We use a model of mercury chemistry and transport in the atmosphere, along with ground- and aircraft-based mercury observations, to learn that oxidized mercury chemically produced in the free troposphere descends in the subtropical anticyclones and makes up much of the mercury depositing to the Earth's surface. Our findings imply that mercury chemistry in the free troposphere and transport in the subtropics are important links between global emissions and surface deposition of mercury.
We use a model of mercury chemistry and transport in the atmosphere, along with ground- and...
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