Articles | Volume 24, issue 15
https://doi.org/10.5194/acp-24-8607-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-24-8607-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
02 Aug 2024
Research article |
| 02 Aug 2024
| 02 Aug 2024
Intercomparison of GEOS-Chem and CAM-chem tropospheric oxidant chemistry within the Community Earth System Model version 2 (CESM2)
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
Louisa K. Emmons
Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, USA
Elizabeth W. Lundgren
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
Laura Hyesung Yang
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
Ruijun Dang
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
Shixian Zhai
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
Earth and Environmental Sciences Programme and Graduate Division of Earth and Atmospheric Sciences, Faculty of Science, The Chinese University of Hong Kong, Sha Tin, Hong Kong SAR, China
Yunxiao Tang
Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA, USA
Makoto M. Kelp
Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA, USA
Department of Earth System Science, Stanford University, Stanford, CA, USA
Nadia K. Colombi
Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA, USA
Sebastian D. Eastham
Joint Program on the Science and Policy of Global Change, Center for Global Change Science, Massachusetts Institute of Technology, Cambridge, MA, USA
Laboratory for Aviation and the Environment, Department of Aeronautics and Astronautics, Massachusetts Institute of Technology, Cambridge, MA, USA
Thibaud M. Fritz
Laboratory for Aviation and the Environment, Department of Aeronautics and Astronautics, Massachusetts Institute of Technology, Cambridge, MA, USA
Daniel J. Jacob
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA, USA
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William J. Collins, Fiona M. O'Connor, Connor R. Barker, Rachael E. Byrom, Sebastian D. Eastham, Øivind Hodnebrog, Patrick Jöckel, Eloise A. Marais, Mariano Mertens, Gunnar Myhre, Matthias Nützel, Dirk Olivié, Ragnhild Bieltvedt Skeie, Laura Stecher, Larry W. Horowitz, Vaishali Naik, Gregory Faluvegi, Ulas Im, Lee T. Murray, Drew Shindell, Kostas Tsigaridis, Nathan Luke Abraham, and James Keeble
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Vincent R. Meijer, Sebastian D. Eastham, Ian A. Waitz, and Steven R. H. Barrett
Atmos. Meas. Tech., 17, 6145–6162, https://doi.org/10.5194/amt-17-6145-2024, https://doi.org/10.5194/amt-17-6145-2024, 2024
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Aviation's climate impact is partly due to contrails: the clouds that form behind aircraft and which can linger for hours under certain atmospheric conditions. Accurately forecasting these conditions could allow aircraft to avoid forming these contrails and thus reduce their environmental footprint. Our research uses deep learning to identify three-dimensional contrail locations in two-dimensional satellite imagery, which can be used to assess and improve these forecasts.
Lucas A. Estrada, Daniel J. Varon, Melissa Sulprizio, Hannah Nesser, Zichong Chen, Nicholas Balasus, Sarah E. Hancock, Megan He, James D. East, Todd A. Mooring, Alexander Oort Alonso, Joannes D. Maasakkers, Ilse Aben, Sabour Baray, Kevin W. Bowman, John R. Worden, Felipe J. Cardoso-Saldaña, Emily Reidy, and Daniel J. Jacob
EGUsphere, https://doi.org/10.5194/egusphere-2024-2700, https://doi.org/10.5194/egusphere-2024-2700, 2024
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Yujin J. Oak, Daniel J. Jacob, Nicholas Balasus, Laura H. Yang, Heesung Chong, Junsung Park, Hanlim Lee, Gitaek T. Lee, Eunjo S. Ha, Rokjin J. Park, Hyeong-Ahn Kwon, and Jhoon Kim
Atmos. Meas. Tech., 17, 5147–5159, https://doi.org/10.5194/amt-17-5147-2024, https://doi.org/10.5194/amt-17-5147-2024, 2024
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David P. Edwards, Sara Martínez-Alonso, Duseong S. Jo, Ivan Ortega, Louisa K. Emmons, John J. Orlando, Helen M. Worden, Jhoon Kim, Hanlim Lee, Junsung Park, and Hyunkee Hong
Atmos. Chem. Phys., 24, 8943–8961, https://doi.org/10.5194/acp-24-8943-2024, https://doi.org/10.5194/acp-24-8943-2024, 2024
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Irene C. Dedoussi, Daven K. Henze, Sebastian D. Eastham, Raymond L. Speth, and Steven R. H. Barrett
Geosci. Model Dev., 17, 5689–5703, https://doi.org/10.5194/gmd-17-5689-2024, https://doi.org/10.5194/gmd-17-5689-2024, 2024
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Atmospheric model gradients provide a meaningful tool for better understanding the underlying atmospheric processes. Adjoint modeling enables computationally efficient gradient calculations. We present the adjoint of the GEOS-Chem unified chemistry extension (UCX). With this development, the GEOS-Chem adjoint model can capture stratospheric ozone and other processes jointly with tropospheric processes. We apply it to characterize the Antarctic ozone depletion potential of active halogen species.
Laura Hyesung Yang, Daniel J. Jacob, Ruijun Dang, Yujin J. Oak, Haipeng Lin, Jhoon Kim, Shixian Zhai, Nadia K. Colombi, Drew C. Pendergrass, Ellie Beaudry, Viral Shah, Xu Feng, Robert M. Yantosca, Heesung Chong, Junsung Park, Hanlim Lee, Won-Jin Lee, Soontae Kim, Eunhye Kim, Katherine R. Travis, James H. Crawford, and Hong Liao
Atmos. Chem. Phys., 24, 7027–7039, https://doi.org/10.5194/acp-24-7027-2024, https://doi.org/10.5194/acp-24-7027-2024, 2024
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The Geostationary Environment Monitoring Spectrometer (GEMS) provides hourly measurements of NO2. We use the chemical transport model to find how emissions, chemistry, and transport drive the changes in NO2 observed by GEMS at different times of the day. In winter, the chemistry plays a minor role, and high daytime emissions dominate the diurnal variation in NO2, balanced by transport. In summer, emissions, chemistry, and transport play an important role in shaping the diurnal variation in NO2.
Drew C. Pendergrass, Daniel J. Jacob, Yujin J. Oak, Jeewoo Lee, Minseok Kim, Jhoon Kim, Seoyoung Lee, Shixian Zhai, Hitoshi Irie, and Hong Liao
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-172, https://doi.org/10.5194/essd-2024-172, 2024
Preprint withdrawn
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Jack H. Bruno, Dylan Jervis, Daniel J. Varon, and Daniel J. Jacob
Atmos. Meas. Tech., 17, 2625–2636, https://doi.org/10.5194/amt-17-2625-2024, https://doi.org/10.5194/amt-17-2625-2024, 2024
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Methane is a potent greenhouse gas and a current high-priority target for short- to mid-term climate change mitigation. Detection of individual methane emitters from space has become possible in recent years, and the volume of data for this task has been rapidly growing, outpacing processing capabilities. We introduce an automated approach, U-Plume, which can detect and quantify emissions from individual methane sources in high-spatial-resolution satellite data.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Alba Lorente, Zichong Chen, Xiao Lu, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Margaux Winter, Shuang Ma, A. Anthony Bloom, John R. Worden, Robert N. Stavins, and Cynthia A. Randles
Atmos. Chem. Phys., 24, 5069–5091, https://doi.org/10.5194/acp-24-5069-2024, https://doi.org/10.5194/acp-24-5069-2024, 2024
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We quantify 2019 methane emissions in the contiguous US (CONUS) at a ≈ 25 km × 25 km resolution using satellite methane observations. We find a 13 % upward correction to the 2023 US Environmental Protection Agency (EPA) Greenhouse Gas Emissions Inventory (GHGI) for 2019, with large corrections to individual states, urban areas, and landfills. This may present a challenge for US climate policies and goals, many of which target significant reductions in methane emissions.
Wenfu Tang, Benjamin Gaubert, Louisa Emmons, Daniel Ziskin, Debbie Mao, David Edwards, Avelino Arellano, Kevin Raeder, Jeffrey Anderson, and Helen Worden
Atmos. Meas. Tech., 17, 1941–1963, https://doi.org/10.5194/amt-17-1941-2024, https://doi.org/10.5194/amt-17-1941-2024, 2024
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We assimilate different MOPITT CO products to understand the impact of (1) assimilating multispectral and joint retrievals versus single spectral products, (2) assimilating satellite profile products versus column products, and (3) assimilating multispectral and joint retrievals versus assimilating individual products separately.
Xu Feng, Loretta J. Mickley, Michelle L. Bell, Tianjia Liu, Jenny A. Fisher, and Maria Val Martin
Atmos. Chem. Phys., 24, 2985–3007, https://doi.org/10.5194/acp-24-2985-2024, https://doi.org/10.5194/acp-24-2985-2024, 2024
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During severe wildfire seasons, smoke can have a significant impact on air quality in Australia. Our study demonstrates that characterization of the smoke plume injection fractions greatly affects estimates of surface smoke PM2.5. Using the plume behavior predicted by the machine learning method leads to the best model agreement with observed surface PM2.5 in key cities across Australia, with smoke PM2.5 accounting for 5 %–52 % of total PM2.5 on average during fire seasons from 2009 to 2020.
Kyoung-Min Kim, Si-Wan Kim, Seunghwan Seo, Donald R. Blake, Seogju Cho, James H. Crawford, Louisa K. Emmons, Alan Fried, Jay R. Herman, Jinkyu Hong, Jinsang Jung, Gabriele G. Pfister, Andrew J. Weinheimer, Jung-Hun Woo, and Qiang Zhang
Geosci. Model Dev., 17, 1931–1955, https://doi.org/10.5194/gmd-17-1931-2024, https://doi.org/10.5194/gmd-17-1931-2024, 2024
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Three emission inventories were evaluated for East Asia using data acquired during a field campaign in 2016. The inventories successfully reproduced the daily variations of ozone and nitrogen dioxide. However, the spatial distributions of model ozone did not fully agree with the observations. Additionally, all simulations underestimated carbon monoxide and volatile organic compound (VOC) levels. Increasing VOC emissions over South Korea resulted in improved ozone simulations.
Sebastian D. Eastham, Guillaume P. Chossière, Raymond L. Speth, Daniel J. Jacob, and Steven R. H. Barrett
Atmos. Chem. Phys., 24, 2687–2703, https://doi.org/10.5194/acp-24-2687-2024, https://doi.org/10.5194/acp-24-2687-2024, 2024
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Emissions from aircraft are known to cause air quality impacts worldwide, but the scale and mechanisms of this impact are not well understood. This work uses high-resolution computational modeling of the atmosphere to show that air pollution changes from aviation are mostly the result of emissions during cruise (high-altitude) operations, that these impacts are related to how much non-aviation pollution is present, and that prior regional assessments have underestimated these impacts.
Kelvin H. Bates, Mathew J. Evans, Barron H. Henderson, and Daniel J. Jacob
Geosci. Model Dev., 17, 1511–1524, https://doi.org/10.5194/gmd-17-1511-2024, https://doi.org/10.5194/gmd-17-1511-2024, 2024
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Accurate representation of rates and products of chemical reactions in atmospheric models is crucial for simulating concentrations of pollutants and climate forcers. We update the widely used GEOS-Chem atmospheric chemistry model with reaction parameters from recent compilations of experimental data and demonstrate the implications for key atmospheric chemical species. The updates decrease tropospheric CO mixing ratios and increase stratospheric nitrogen oxide mixing ratios, among other changes.
Wenfu Tang, Louisa K. Emmons, Helen M. Worden, Rajesh Kumar, Cenlin He, Benjamin Gaubert, Zhonghua Zheng, Simone Tilmes, Rebecca R. Buchholz, Sara-Eva Martinez-Alonso, Claire Granier, Antonin Soulie, Kathryn McKain, Bruce C. Daube, Jeff Peischl, Chelsea Thompson, and Pieternel Levelt
Geosci. Model Dev., 16, 6001–6028, https://doi.org/10.5194/gmd-16-6001-2023, https://doi.org/10.5194/gmd-16-6001-2023, 2023
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The new MUSICAv0 model enables the study of atmospheric chemistry across all relevant scales. We develop a MUSICAv0 grid for Africa. We evaluate MUSICAv0 with observations and compare it with a previously used model – WRF-Chem. Overall, the performance of MUSICAv0 is comparable to WRF-Chem. Based on model–satellite discrepancies, we find that future field campaigns in an eastern African region (30°E–45°E, 5°S–5°N) could substantially improve the predictive skill of air quality models.
Maria Val Martin, Elena Blanc-Betes, Ka Ming Fung, Euripides P. Kantzas, Ilsa B. Kantola, Isabella Chiaravalloti, Lyla L. Taylor, Louisa K. Emmons, William R. Wieder, Noah J. Planavsky, Michael D. Masters, Evan H. DeLucia, Amos P. K. Tai, and David J. Beerling
Geosci. Model Dev., 16, 5783–5801, https://doi.org/10.5194/gmd-16-5783-2023, https://doi.org/10.5194/gmd-16-5783-2023, 2023
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Enhanced rock weathering (ERW) is a CO2 removal strategy that involves applying crushed rocks (e.g., basalt) to agricultural soils. However, unintended processes within the N cycle due to soil pH changes may affect the climate benefits of C sequestration. ERW could drive changes in soil emissions of non-CO2 GHGs (N2O) and trace gases (NO and NH3) that may affect air quality. We present a new improved N cycling scheme for the land model (CLM5) to evaluate ERW effects on soil gas N emissions.
Drew C. Pendergrass, Daniel J. Jacob, Hannah Nesser, Daniel J. Varon, Melissa Sulprizio, Kazuyuki Miyazaki, and Kevin W. Bowman
Geosci. Model Dev., 16, 4793–4810, https://doi.org/10.5194/gmd-16-4793-2023, https://doi.org/10.5194/gmd-16-4793-2023, 2023
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We have built a tool called CHEEREIO that allows scientists to use observations of pollutants or gases in the atmosphere, such as from satellites or surface stations, to update supercomputer models that simulate the Earth. CHEEREIO uses the difference between the model simulations of the atmosphere and real-world observations to come up with a good guess for the actual composition of our atmosphere, the true emissions of various pollutants, and whatever else they may want to study.
Nicholas Balasus, Daniel J. Jacob, Alba Lorente, Joannes D. Maasakkers, Robert J. Parker, Hartmut Boesch, Zichong Chen, Makoto M. Kelp, Hannah Nesser, and Daniel J. Varon
Atmos. Meas. Tech., 16, 3787–3807, https://doi.org/10.5194/amt-16-3787-2023, https://doi.org/10.5194/amt-16-3787-2023, 2023
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We use machine learning to remove biases in TROPOMI satellite observations of atmospheric methane, with GOSAT observations serving as a reference. We find that the TROPOMI biases relative to GOSAT are related to the presence of aerosols and clouds, the surface brightness, and the specific detector that makes the observation aboard TROPOMI. The resulting blended TROPOMI+GOSAT product is more reliable for quantifying methane emissions.
Christine Wiedinmyer, Yosuke Kimura, Elena C. McDonald-Buller, Louisa K. Emmons, Rebecca R. Buchholz, Wenfu Tang, Keenan Seto, Maxwell B. Joseph, Kelley C. Barsanti, Annmarie G. Carlton, and Robert Yokelson
Geosci. Model Dev., 16, 3873–3891, https://doi.org/10.5194/gmd-16-3873-2023, https://doi.org/10.5194/gmd-16-3873-2023, 2023
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The Fire INventory from NCAR (FINN) provides daily global estimates of emissions from open fires based on satellite detections of hot spots. This version has been updated to apply MODIS and VIIRS satellite fire detection and better represents both large and small fires. FINNv2.5 generates more emissions than FINNv1 and is in general agreement with other fire emissions inventories. The new estimates are consistent with satellite observations, but uncertainties remain regionally and by pollutant.
Duseong S. Jo, Simone Tilmes, Louisa K. Emmons, Siyuan Wang, and Francis Vitt
Geosci. Model Dev., 16, 3893–3906, https://doi.org/10.5194/gmd-16-3893-2023, https://doi.org/10.5194/gmd-16-3893-2023, 2023
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A new simple secondary organic aerosol (SOA) scheme has been developed for the Community Atmosphere Model (CAM) based on the complex SOA scheme in CAM with detailed chemistry (CAM-chem). The CAM with the new SOA scheme shows better agreements with CAM-chem in terms of aerosol concentrations and radiative fluxes, which ensures more consistent results between different compsets in the Community Earth System Model. The new SOA scheme also has technical advantages for future developments.
Daniel J. Varon, Daniel J. Jacob, Benjamin Hmiel, Ritesh Gautam, David R. Lyon, Mark Omara, Melissa Sulprizio, Lu Shen, Drew Pendergrass, Hannah Nesser, Zhen Qu, Zachary R. Barkley, Natasha L. Miles, Scott J. Richardson, Kenneth J. Davis, Sudhanshu Pandey, Xiao Lu, Alba Lorente, Tobias Borsdorff, Joannes D. Maasakkers, and Ilse Aben
Atmos. Chem. Phys., 23, 7503–7520, https://doi.org/10.5194/acp-23-7503-2023, https://doi.org/10.5194/acp-23-7503-2023, 2023
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We use TROPOMI satellite observations to quantify weekly methane emissions from the US Permian oil and gas basin from May 2018 to October 2020. We find that Permian emissions are highly variable, with diverse economic and activity drivers. The most important drivers during our study period were new well development and natural gas price. Permian methane intensity averaged 4.6 % and decreased by 1 % per year.
Ruijun Dang, Daniel J. Jacob, Viral Shah, Sebastian D. Eastham, Thibaud M. Fritz, Loretta J. Mickley, Tianjia Liu, Yi Wang, and Jun Wang
Atmos. Chem. Phys., 23, 6271–6284, https://doi.org/10.5194/acp-23-6271-2023, https://doi.org/10.5194/acp-23-6271-2023, 2023
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We use the GEOS-Chem model to better understand the magnitude and trend in free tropospheric NO2 over the contiguous US. Model underestimate of background NO2 is largely corrected by considering aerosol nitrate photolysis. Increase in aircraft emissions affects satellite retrievals by altering the NO2 shape factor, and this effect is expected to increase in future. We show the importance of properly accounting for the free tropospheric background in interpreting NO2 observations from space.
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.
Wenfu Tang, Simone Tilmes, David M. Lawrence, Fang Li, Cenlin He, Louisa K. Emmons, Rebecca R. Buchholz, and Lili Xia
Atmos. Chem. Phys., 23, 5467–5486, https://doi.org/10.5194/acp-23-5467-2023, https://doi.org/10.5194/acp-23-5467-2023, 2023
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Globally, total wildfire burned area is projected to increase over the 21st century under scenarios without geoengineering and decrease under the two geoengineering scenarios. Geoengineering reduces fire by decreasing surface temperature and wind speed and increasing relative humidity and soil water. However, geoengineering also yields reductions in precipitation, which offset some of the fire reduction.
Shixian Zhai, Daniel J. Jacob, Drew C. Pendergrass, Nadia K. Colombi, Viral Shah, Laura Hyesung Yang, Qiang Zhang, Shuxiao Wang, Hwajin Kim, Yele Sun, Jin-Soo Choi, Jin-Soo Park, Gan Luo, Fangqun Yu, Jung-Hun Woo, Younha Kim, Jack E. Dibb, Taehyoung Lee, Jin-Seok Han, Bruce E. Anderson, Ke Li, and Hong Liao
Atmos. Chem. Phys., 23, 4271–4281, https://doi.org/10.5194/acp-23-4271-2023, https://doi.org/10.5194/acp-23-4271-2023, 2023
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Anthropogenic fugitive dust in East Asia not only causes severe coarse particulate matter air pollution problems, but also affects fine particulate nitrate. Due to emission control efforts, coarse PM decreased steadily. We find that the decrease of coarse PM is a major driver for a lack of decrease of fine particulate nitrate, as it allows more nitric acid to form fine particulate nitrate. The continuing decrease of coarse PM requires more stringent ammonia and nitrogen oxides emission controls.
Nadia K. Colombi, Daniel J. Jacob, Laura Hyesung Yang, Shixian Zhai, Viral Shah, Stuart K. Grange, Robert M. Yantosca, Soontae Kim, and Hong Liao
Atmos. Chem. Phys., 23, 4031–4044, https://doi.org/10.5194/acp-23-4031-2023, https://doi.org/10.5194/acp-23-4031-2023, 2023
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Surface ozone, detrimental to human and ecosystem health, is very high and increasing in South Korea. Using a global model of the atmosphere, we found that emissions from South Korea and China contribute equally to the high ozone observed. We found that in the absence of all anthropogenic emissions over East Asia, ozone is still very high, implying that the air quality standard in South Korea is not practically achievable unless this background external to East Asia can be decreased.
Laura Hyesung Yang, Daniel J. Jacob, Nadia K. Colombi, Shixian Zhai, Kelvin H. Bates, Viral Shah, Ellie Beaudry, Robert M. Yantosca, Haipeng Lin, Jared F. Brewer, Heesung Chong, Katherine R. Travis, James H. Crawford, Lok N. Lamsal, Ja-Ho Koo, and Jhoon Kim
Atmos. Chem. Phys., 23, 2465–2481, https://doi.org/10.5194/acp-23-2465-2023, https://doi.org/10.5194/acp-23-2465-2023, 2023
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A geostationary satellite can now provide hourly NO2 vertical columns, and obtaining the NO2 vertical columns from space relies on NO2 vertical distribution from the chemical transport model (CTM). In this work, we update the CTM to better represent the chemistry environment so that the CTM can accurately provide NO2 vertical distribution. We also find that the changes in NO2 vertical distribution driven by a change in mixing depth play an important role in the NO2 column's diurnal variation.
Fangqun Yu, Gan Luo, Arshad Arjunan Nair, Sebastian Eastham, Christina J. Williamson, Agnieszka Kupc, and Charles A. Brock
Atmos. Chem. Phys., 23, 1863–1877, https://doi.org/10.5194/acp-23-1863-2023, https://doi.org/10.5194/acp-23-1863-2023, 2023
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Particle number concentrations and size distributions in the stratosphere are studied through model simulations and comparisons with measurements. The nucleation scheme used in most of the solar geoengineering modeling studies overpredicts the nucleation rates and particle number concentrations in the stratosphere. The model based on updated nucleation schemes captures reasonably well some aspects of particle size distributions but misses some features. The possible reasons are discussed.
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
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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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.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Randall V. Martin, Sebastian D. Eastham, Liam Bindle, Elizabeth W. Lundgren, Thomas L. Clune, Christoph A. Keller, William Downs, Dandan Zhang, Robert A. Lucchesi, Melissa P. Sulprizio, Robert M. Yantosca, Yanshun Li, Lucas Estrada, William M. Putman, Benjamin M. Auer, Atanas L. Trayanov, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 15, 8731–8748, https://doi.org/10.5194/gmd-15-8731-2022, https://doi.org/10.5194/gmd-15-8731-2022, 2022
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Atmospheric chemistry models must be able to operate both online as components of Earth system models and offline as standalone models. The widely used GEOS-Chem model operates both online and offline, but the classic offline version is not suitable for massively parallel simulations. We describe a new generation of the offline high-performance GEOS-Chem (GCHP) that enables high-resolution simulations on thousands of cores, including on the cloud, with improved access, performance, and accuracy.
Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Haipeng Lin, Elizabeth W. Lundgren, Steve Goldhaber, Steven R. H. Barrett, and Daniel J. Jacob
Geosci. Model Dev., 15, 8669–8704, https://doi.org/10.5194/gmd-15-8669-2022, https://doi.org/10.5194/gmd-15-8669-2022, 2022
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We bring the state-of-the-science chemistry module GEOS-Chem into the Community Earth System Model (CESM). We show that some known differences between results from GEOS-Chem and CESM's CAM-chem chemistry module may be due to the configuration of model meteorology rather than inherent differences in the model chemistry. This is a significant step towards a truly modular Earth system model and allows two strong but currently separate research communities to benefit from each other's advances.
Longlei Li, Natalie M. Mahowald, Jasper F. Kok, Xiaohong Liu, Mingxuan Wu, Danny M. Leung, Douglas S. Hamilton, Louisa K. Emmons, Yue Huang, Neil Sexton, Jun Meng, and Jessica Wan
Geosci. Model Dev., 15, 8181–8219, https://doi.org/10.5194/gmd-15-8181-2022, https://doi.org/10.5194/gmd-15-8181-2022, 2022
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This study advances mineral dust parameterizations in the Community Atmospheric Model (CAM; version 6.1). Efforts include 1) incorporating a more physically based dust emission scheme; 2) updating the dry deposition scheme; and 3) revising the gravitational settling velocity to account for dust asphericity. Substantial improvements achieved with these updates can help accurately quantify dust–climate interactions using CAM, such as the dust-radiation and dust–cloud interactions.
Haolin Wang, Xiao Lu, Daniel J. Jacob, Owen R. Cooper, Kai-Lan Chang, Ke Li, Meng Gao, Yiming Liu, Bosi Sheng, Kai Wu, Tongwen Wu, Jie Zhang, Bastien Sauvage, Philippe Nédélec, Romain Blot, and Shaojia Fan
Atmos. Chem. Phys., 22, 13753–13782, https://doi.org/10.5194/acp-22-13753-2022, https://doi.org/10.5194/acp-22-13753-2022, 2022
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We report significant global tropospheric ozone increases in 1995–2017 based on extensive aircraft and ozonesonde observations. Using GEOS-Chem (Goddard Earth Observing System chemistry model) multi-decadal global simulations, we find that changes in global anthropogenic emissions, in particular the rapid increases in aircraft emissions, contribute significantly to the increases in tropospheric ozone and resulting radiative impact.
William Atkinson, Sebastian D. Eastham, Y.-H. Henry Chen, Jennifer Morris, Sergey Paltsev, C. Adam Schlosser, and Noelle E. Selin
Geosci. Model Dev., 15, 7767–7789, https://doi.org/10.5194/gmd-15-7767-2022, https://doi.org/10.5194/gmd-15-7767-2022, 2022
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Understanding policy effects on human-caused air pollutant emissions is key for assessing related health impacts. We develop a flexible scenario tool that combines updated emissions data sets, long-term economic modeling, and comprehensive technology pathways to clarify the impacts of climate and air quality policies. Results show the importance of both policy levers in the future to prevent long-term emission increases from offsetting near-term air quality improvements from existing policies.
Lu Shen, Ritesh Gautam, Mark Omara, Daniel Zavala-Araiza, Joannes D. Maasakkers, Tia R. Scarpelli, Alba Lorente, David Lyon, Jianxiong Sheng, Daniel J. Varon, Hannah Nesser, Zhen Qu, Xiao Lu, Melissa P. Sulprizio, Steven P. Hamburg, and Daniel J. Jacob
Atmos. Chem. Phys., 22, 11203–11215, https://doi.org/10.5194/acp-22-11203-2022, https://doi.org/10.5194/acp-22-11203-2022, 2022
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We use 22 months of TROPOMI satellite observations to quantity methane emissions from the oil (O) and natural gas (G) sector in the US and Canada at the scale of both individual basins as well as country-wide aggregates. We find that O/G-related methane emissions are underestimated in these inventories by 80 % for the US and 40 % for Canada, and 70 % of the underestimate in the US is from five O/G basins, including Permian, Haynesville, Anadarko, Eagle Ford, and Barnett.
Zichong Chen, Daniel J. Jacob, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Elise Penn, and Xueying Yu
Atmos. Chem. Phys., 22, 10809–10826, https://doi.org/10.5194/acp-22-10809-2022, https://doi.org/10.5194/acp-22-10809-2022, 2022
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We quantify methane emissions in China and contributions from different sectors by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We find that anthropogenic methane emissions for China are underestimated in the national inventory. Our estimate of emissions indicates a small life-cycle loss rate, implying net climate benefits from the current
coal-to-gasenergy transition in China. However, this small loss rate can be misleading given China's high gas imports.
Daniel J. Jacob, Daniel J. Varon, Daniel H. Cusworth, Philip E. Dennison, Christian Frankenberg, Ritesh Gautam, Luis Guanter, John Kelley, Jason McKeever, Lesley E. Ott, Benjamin Poulter, Zhen Qu, Andrew K. Thorpe, John R. Worden, and Riley M. Duren
Atmos. Chem. Phys., 22, 9617–9646, https://doi.org/10.5194/acp-22-9617-2022, https://doi.org/10.5194/acp-22-9617-2022, 2022
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We review the capability of satellite observations of atmospheric methane to quantify methane emissions on all scales. We cover retrieval methods, precision requirements, inverse methods for inferring emissions, source detection thresholds, and observations of system completeness. We show that current instruments already enable quantification of regional and national emissions including contributions from large point sources. Coverage and resolution will increase significantly in coming years.
Daniel J. Varon, Daniel J. Jacob, Melissa Sulprizio, Lucas A. Estrada, William B. Downs, Lu Shen, Sarah E. Hancock, Hannah Nesser, Zhen Qu, Elise Penn, Zichong Chen, Xiao Lu, Alba Lorente, Ashutosh Tewari, and Cynthia A. Randles
Geosci. Model Dev., 15, 5787–5805, https://doi.org/10.5194/gmd-15-5787-2022, https://doi.org/10.5194/gmd-15-5787-2022, 2022
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Reducing atmospheric methane emissions is critical to slow near-term climate change. Globally surveying satellite instruments like the TROPOspheric Monitoring Instrument (TROPOMI) have unique capabilities for monitoring atmospheric methane around the world. Here we present a user-friendly cloud-computing tool that enables researchers and stakeholders to quantify methane emissions across user-selected regions of interest using TROPOMI satellite observations.
John R. Worden, Daniel H. Cusworth, Zhen Qu, Yi Yin, Yuzhong Zhang, A. Anthony Bloom, Shuang Ma, Brendan K. Byrne, Tia Scarpelli, Joannes D. Maasakkers, David Crisp, Riley Duren, and Daniel J. Jacob
Atmos. Chem. Phys., 22, 6811–6841, https://doi.org/10.5194/acp-22-6811-2022, https://doi.org/10.5194/acp-22-6811-2022, 2022
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This paper is intended to accomplish two goals: 1) describe a new algorithm by which remotely sensed measurements of methane or other tracers can be used to not just quantify methane fluxes, but also attribute these fluxes to specific sources and regions and characterize their uncertainties, and 2) use this new algorithm to provide methane emissions by sector and country in support of the global stock take.
Xiaotian Xu, Xu Feng, Haipeng Lin, Peng Zhang, Shaojian Huang, Zhengcheng Song, Yiming Peng, Tzung-May Fu, and Yanxu Zhang
Geosci. Model Dev., 15, 3845–3859, https://doi.org/10.5194/gmd-15-3845-2022, https://doi.org/10.5194/gmd-15-3845-2022, 2022
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Mercury is one of the most toxic pollutants in the environment, and wet deposition is a major process for atmospheric mercury to enter, causing ecological and human health risks. High-mercury wet deposition in the southeastern US has been a problem for many years. Here we employed a newly developed high-resolution WRF-GC model with the capability to simulate mercury to study this problem. We conclude that deep convection caused enhanced mercury wet deposition in the southeastern US.
Pinya Wang, Yang Yang, Huimin Li, Lei Chen, Ruijun Dang, Daokai Xue, Baojie Li, Jianping Tang, L. Ruby Leung, and Hong Liao
Atmos. Chem. Phys., 22, 4705–4719, https://doi.org/10.5194/acp-22-4705-2022, https://doi.org/10.5194/acp-22-4705-2022, 2022
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China is now suffering from both severe ozone (O3) pollution and heat events. We highlight that North China Plain is the hot spot of the co-occurrences of extremes in O3 and high temperatures in China. Such coupled extremes exhibit an increasing trend during 2014–2019 and will continue to increase until the middle of this century. And the coupled extremes impose more severe health impacts to human than O3 pollution occurring alone because of elevated O3 levels and temperatures.
Tia R. Scarpelli, Daniel J. Jacob, Shayna Grossman, Xiao Lu, Zhen Qu, Melissa P. Sulprizio, Yuzhong Zhang, Frances Reuland, Deborah Gordon, and John R. Worden
Atmos. Chem. Phys., 22, 3235–3249, https://doi.org/10.5194/acp-22-3235-2022, https://doi.org/10.5194/acp-22-3235-2022, 2022
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We present a spatially explicit version of the national inventories of oil, gas, and coal methane emissions as submitted by individual countries to the United Nations Framework Convention on Climate Change (UNFCCC) in 2021. We then use atmospheric modeling to compare our inventory emissions to atmospheric methane observations with the goal of identifying potential under- and overestimates of oil–gas methane emissions in the national inventories.
Drew C. Pendergrass, Shixian Zhai, Jhoon Kim, Ja-Ho Koo, Seoyoung Lee, Minah Bae, Soontae Kim, Hong Liao, and Daniel J. Jacob
Atmos. Meas. Tech., 15, 1075–1091, https://doi.org/10.5194/amt-15-1075-2022, https://doi.org/10.5194/amt-15-1075-2022, 2022
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This paper uses a machine learning algorithm to infer high-resolution maps of particulate air quality in eastern China, Japan, and the Korean peninsula, using data from a geostationary satellite along with meteorology. We then perform an extensive evaluation of this inferred air quality and use it to diagnose trends in the region. We hope this paper and the associated data will be valuable to other scientists interested in epidemiology, air quality, remote sensing, and machine learning.
Lu Shen, Daniel J. Jacob, Mauricio Santillana, Kelvin Bates, Jiawei Zhuang, and Wei Chen
Geosci. Model Dev., 15, 1677–1687, https://doi.org/10.5194/gmd-15-1677-2022, https://doi.org/10.5194/gmd-15-1677-2022, 2022
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The high computational cost of chemical integration is a long-standing limitation in global atmospheric chemistry models. Here we present an adaptive and efficient algorithm that can reduce the computational time of atmospheric chemistry by 50 % and maintain the error below 2 % for important species, inspired by machine learning clustering techniques and traditional asymptotic analysis ideas.
Xiao Lu, Daniel J. Jacob, Haolin Wang, Joannes D. Maasakkers, Yuzhong Zhang, Tia R. Scarpelli, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Hannah Nesser, A. Anthony Bloom, Shuang Ma, John R. Worden, Shaojia Fan, Robert J. Parker, Hartmut Boesch, Ritesh Gautam, Deborah Gordon, Michael D. Moran, Frances Reuland, Claudia A. Octaviano Villasana, and Arlyn Andrews
Atmos. Chem. Phys., 22, 395–418, https://doi.org/10.5194/acp-22-395-2022, https://doi.org/10.5194/acp-22-395-2022, 2022
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We evaluate methane emissions and trends for 2010–2017 in the gridded national emission inventories for the United States, Canada, and Mexico by inversion of in situ and satellite methane observations. We find that anthropogenic methane emissions for all three countries are underestimated in the national inventories, largely driven by oil emissions. Anthropogenic methane emissions in the US peak in 2014, in contrast to the report of a steadily decreasing trend over 2010–2017 from the US EPA.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Sabour Baray, Daniel J. Jacob, Joannes D. Maasakkers, Jian-Xiong Sheng, Melissa P. Sulprizio, Dylan B. A. Jones, A. Anthony Bloom, and Robert McLaren
Atmos. Chem. Phys., 21, 18101–18121, https://doi.org/10.5194/acp-21-18101-2021, https://doi.org/10.5194/acp-21-18101-2021, 2021
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We use 2010–2015 surface and satellite observations to disentangle methane from anthropogenic and natural sources in Canada. Using a chemical transport model (GEOS-Chem), the mismatch between modelled and observed methane concentrations can be used to infer emissions according to Bayesian statistics. Compared to prior knowledge, we show higher anthropogenic emissions attributed to energy and/or agriculture in Western Canada and lower natural emissions from Boreal wetlands.
Shixian Zhai, Daniel J. Jacob, Jared F. Brewer, Ke Li, Jonathan M. Moch, Jhoon Kim, Seoyoung Lee, Hyunkwang Lim, Hyun Chul Lee, Su Keun Kuk, Rokjin J. Park, Jaein I. Jeong, Xuan Wang, Pengfei Liu, Gan Luo, Fangqun Yu, Jun Meng, Randall V. Martin, Katherine R. Travis, Johnathan W. Hair, Bruce E. Anderson, Jack E. Dibb, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jung-Hun Woo, Younha Kim, Qiang Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 16775–16791, https://doi.org/10.5194/acp-21-16775-2021, https://doi.org/10.5194/acp-21-16775-2021, 2021
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Geostationary satellite aerosol optical depth (AOD) has tremendous potential for monitoring surface fine particulate matter (PM2.5). Our study explored the physical relationship between AOD and PM2.5 by integrating data from surface networks, aircraft, and satellites with the GEOS-Chem chemical transport model. We quantitatively showed that accurate simulation of aerosol size distributions, boundary layer depths, relative humidity, coarse particles, and diurnal variations in PM2.5 are essential.
Liam Bindle, Randall V. Martin, Matthew J. Cooper, Elizabeth W. Lundgren, Sebastian D. Eastham, Benjamin M. Auer, Thomas L. Clune, Hongjian Weng, Jintai Lin, Lee T. Murray, Jun Meng, Christoph A. Keller, William M. Putman, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 14, 5977–5997, https://doi.org/10.5194/gmd-14-5977-2021, https://doi.org/10.5194/gmd-14-5977-2021, 2021
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Atmospheric chemistry models like GEOS-Chem are versatile tools widely used in air pollution and climate studies. The simulations used in such studies can be very computationally demanding, and thus it is useful if the model can simulate a specific geographic region at a higher resolution than the rest of the globe. Here, we implement, test, and demonstrate a new variable-resolution capability in GEOS-Chem that is suitable for simulations conducted on supercomputers.
Xinxin Ye, Pargoal Arab, Ravan Ahmadov, Eric James, Georg A. Grell, Bradley Pierce, Aditya Kumar, Paul Makar, Jack Chen, Didier Davignon, Greg R. Carmichael, Gonzalo Ferrada, Jeff McQueen, Jianping Huang, Rajesh Kumar, Louisa Emmons, Farren L. Herron-Thorpe, Mark Parrington, Richard Engelen, Vincent-Henri Peuch, Arlindo da Silva, Amber Soja, Emily Gargulinski, Elizabeth Wiggins, Johnathan W. Hair, Marta Fenn, Taylor Shingler, Shobha Kondragunta, Alexei Lyapustin, Yujie Wang, Brent Holben, David M. Giles, and Pablo E. Saide
Atmos. Chem. Phys., 21, 14427–14469, https://doi.org/10.5194/acp-21-14427-2021, https://doi.org/10.5194/acp-21-14427-2021, 2021
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Wildfire smoke has crucial impacts on air quality, while uncertainties in the numerical forecasts remain significant. We present an evaluation of 12 real-time forecasting systems. Comparison of predicted smoke emissions suggests a large spread in magnitudes, with temporal patterns deviating from satellite detections. The performance for AOD and surface PM2.5 and their discrepancies highlighted the role of accurately represented spatiotemporal emission profiles in improving smoke forecasts.
Zhen Qu, Daniel J. Jacob, Lu Shen, Xiao Lu, Yuzhong Zhang, Tia R. Scarpelli, Hannah Nesser, Melissa P. Sulprizio, Joannes D. Maasakkers, A. Anthony Bloom, John R. Worden, Robert J. Parker, and Alba L. Delgado
Atmos. Chem. Phys., 21, 14159–14175, https://doi.org/10.5194/acp-21-14159-2021, https://doi.org/10.5194/acp-21-14159-2021, 2021
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The recent launch of TROPOMI offers an unprecedented opportunity to quantify the methane budget from a top-down perspective. We use TROPOMI and the more mature GOSAT methane observations to estimate methane emissions and get consistent global budgets. However, TROPOMI shows biases over regions where surface albedo is small and provides less information for the coarse-resolution inversion due to the larger error correlations and spatial variations in the number of observations.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Haipeng Lin, Daniel J. Jacob, Elizabeth W. Lundgren, Melissa P. Sulprizio, Christoph A. Keller, Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Patrick C. Campbell, Barry Baker, Rick D. Saylor, and Raffaele Montuoro
Geosci. Model Dev., 14, 5487–5506, https://doi.org/10.5194/gmd-14-5487-2021, https://doi.org/10.5194/gmd-14-5487-2021, 2021
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Emissions are a central component of atmospheric chemistry models. The Harmonized Emissions Component (HEMCO) is a software component for computing emissions from a user-selected ensemble of emission inventories and algorithms. It allows users to select, add, and scale emissions from different sources through a configuration file with no change to the model source code. We demonstrate the implementation of HEMCO in several models, all sharing the same HEMCO core code and database library.
Yi Yin, Frederic Chevallier, Philippe Ciais, Philippe Bousquet, Marielle Saunois, Bo Zheng, John Worden, A. Anthony Bloom, Robert J. Parker, Daniel J. Jacob, Edward J. Dlugokencky, and Christian Frankenberg
Atmos. Chem. Phys., 21, 12631–12647, https://doi.org/10.5194/acp-21-12631-2021, https://doi.org/10.5194/acp-21-12631-2021, 2021
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The growth of methane, the second-most important anthropogenic greenhouse gas after carbon dioxide, has been accelerating in recent years. Using an ensemble of multi-tracer atmospheric inversions constrained by surface or satellite observations, we show that global methane emissions increased by nearly 1 % per year from 2010–2017, with leading contributions from the tropics and East Asia.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Tia R. Scarpelli, Melissa P. Sulprizio, Yuzhong Zhang, and Chris H. Rycroft
Atmos. Meas. Tech., 14, 5521–5534, https://doi.org/10.5194/amt-14-5521-2021, https://doi.org/10.5194/amt-14-5521-2021, 2021
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Analytical inversions of satellite observations of atmospheric composition can improve emissions estimates and quantify errors but are computationally expensive at high resolutions. We propose two methods to decrease this cost. The methods reproduce a high-resolution inversion at a quarter of the cost. The reduced-dimension method creates a multiscale grid. The reduced-rank method solves the inversion where information content is highest.
Wenfu Tang, David P. Edwards, Louisa K. Emmons, Helen M. Worden, Laura M. Judd, Lok N. Lamsal, Jassim A. Al-Saadi, Scott J. Janz, James H. Crawford, Merritt N. Deeter, Gabriele Pfister, Rebecca R. Buchholz, Benjamin Gaubert, and Caroline R. Nowlan
Atmos. Meas. Tech., 14, 4639–4655, https://doi.org/10.5194/amt-14-4639-2021, https://doi.org/10.5194/amt-14-4639-2021, 2021
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We use high-resolution airborne mapping spectrometer measurements to assess sub-grid variability within satellite pixels over urban regions. The sub-grid variability within satellite pixels increases with increasing satellite pixel sizes. Temporal variability within satellite pixels decreases with increasing satellite pixel sizes. This work is particularly relevant and useful for future satellite design, satellite data interpretation, and point-grid data comparisons.
Xu Feng, Haipeng Lin, Tzung-May Fu, Melissa P. Sulprizio, Jiawei Zhuang, Daniel J. Jacob, Heng Tian, Yaping Ma, Lijuan Zhang, Xiaolin Wang, Qi Chen, and Zhiwei Han
Geosci. Model Dev., 14, 3741–3768, https://doi.org/10.5194/gmd-14-3741-2021, https://doi.org/10.5194/gmd-14-3741-2021, 2021
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WRF-GC is an online coupling of the WRF meteorological model and GEOS-Chem chemical transport model for regional atmospheric chemistry and air quality modeling. In WRF-GC v2.0, we implemented the aerosol–radiation interactions and aerosol–cloud interactions, as well as the capability to nest multiple domains for high-resolution simulations based on the modular framework of WRF-GC v1.0. This allows the GEOS-Chem users to investigate the meteorology–atmospheric chemistry interactions.
Yaman Liu, Xinyi Dong, Minghuai Wang, Louisa K. Emmons, Yawen Liu, Yuan Liang, Xiao Li, and Manish Shrivastava
Atmos. Chem. Phys., 21, 8003–8021, https://doi.org/10.5194/acp-21-8003-2021, https://doi.org/10.5194/acp-21-8003-2021, 2021
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Secondary organic aerosol (SOA) is considered one of the most important uncertainties in climate modeling. We evaluate SOA performance in the Community Earth System Model version 2.1 (CESM2.1) configured with the Community Atmosphere Model version 6 with chemistry (CAM6-Chem) through a long-term simulation (1988–2019) with observations in the United States, which indicates monoterpene-formed SOA contributes most to the overestimation of SOA at the surface and underestimation in the upper air.
David R. Lyon, Benjamin Hmiel, Ritesh Gautam, Mark Omara, Katherine A. Roberts, Zachary R. Barkley, Kenneth J. Davis, Natasha L. Miles, Vanessa C. Monteiro, Scott J. Richardson, Stephen Conley, Mackenzie L. Smith, Daniel J. Jacob, Lu Shen, Daniel J. Varon, Aijun Deng, Xander Rudelis, Nikhil Sharma, Kyle T. Story, Adam R. Brandt, Mary Kang, Eric A. Kort, Anthony J. Marchese, and Steven P. Hamburg
Atmos. Chem. Phys., 21, 6605–6626, https://doi.org/10.5194/acp-21-6605-2021, https://doi.org/10.5194/acp-21-6605-2021, 2021
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The Permian Basin (USA) is the world’s largest oil field. We use tower- and aircraft-based approaches to measure how methane emissions in the Permian Basin changed throughout 2020. In early 2020, 3.3 % of the region’s gas was emitted; then in spring 2020, the loss rate temporarily dropped to 1.9 % as oil price crashed. We find this short-term reduction to be a result of reduced well development, less gas flaring, and fewer abnormal events despite minimal reductions in oil and gas production.
Fernando Chouza, Thierry Leblanc, Mark Brewer, Patrick Wang, Sabino Piazzolla, Gabriele Pfister, Rajesh Kumar, Carl Drews, Simone Tilmes, Louisa Emmons, and Matthew Johnson
Atmos. Chem. Phys., 21, 6129–6153, https://doi.org/10.5194/acp-21-6129-2021, https://doi.org/10.5194/acp-21-6129-2021, 2021
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The tropospheric ozone lidar at the JPL Table Mountain Facility (TMF) was used to investigate the impact of Los Angeles (LA) Basin pollution transport and stratospheric intrusions in the planetary boundary layer on the San Gabriel Mountains. The results of this study indicate a dominant role of the LA Basin pollution on days when high ozone levels were observed at TMF (March–October period).
Daniel J. Varon, Dylan Jervis, Jason McKeever, Ian Spence, David Gains, and Daniel J. Jacob
Atmos. Meas. Tech., 14, 2771–2785, https://doi.org/10.5194/amt-14-2771-2021, https://doi.org/10.5194/amt-14-2771-2021, 2021
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Satellites can detect methane emissions by measuring sunlight reflected from the Earth's surface and atmosphere. Here we show that the European Space Agency's Sentinel-2 twin satellites can be used to monitor anomalously large methane point sources around the world, with global coverage every 2–5 days and 20 m spatial resolution. We demonstrate this previously unreported capability through high-frequency Sentinel-2 monitoring of two strong methane point sources in Algeria and Turkmenistan.
Xiao Lu, Daniel J. Jacob, Yuzhong Zhang, Joannes D. Maasakkers, Melissa P. Sulprizio, Lu Shen, Zhen Qu, Tia R. Scarpelli, Hannah Nesser, Robert M. Yantosca, Jianxiong Sheng, Arlyn Andrews, Robert J. Parker, Hartmut Boesch, A. Anthony Bloom, and Shuang Ma
Atmos. Chem. Phys., 21, 4637–4657, https://doi.org/10.5194/acp-21-4637-2021, https://doi.org/10.5194/acp-21-4637-2021, 2021
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We use an analytical solution to the Bayesian inverse problem to quantitatively compare and combine the information from satellite and in situ observations, and to estimate global methane budget and their trends over the 2010–2017 period. We find that satellite and in situ observations are to a large extent complementary in the inversion for estimating global methane budget, and reveal consistent corrections of regional anthropogenic and wetland methane emissions relative to the prior inventory.
Joannes D. Maasakkers, Daniel J. Jacob, Melissa P. Sulprizio, Tia R. Scarpelli, Hannah Nesser, Jianxiong Sheng, Yuzhong Zhang, Xiao Lu, A. Anthony Bloom, Kevin W. Bowman, John R. Worden, and Robert J. Parker
Atmos. Chem. Phys., 21, 4339–4356, https://doi.org/10.5194/acp-21-4339-2021, https://doi.org/10.5194/acp-21-4339-2021, 2021
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We use 2010–2015 GOSAT satellite observations of atmospheric methane over North America in a high-resolution inversion to estimate methane emissions. We find general consistency with the gridded EPA inventory but higher oil and gas production emissions, with oil production emissions twice as large as in the latest EPA Greenhouse Gas Inventory. We find lower wetland emissions than predicted by WetCHARTs and a small increasing trend in the eastern US, apparently related to unconventional oil/gas.
Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, https://doi.org/10.5194/acp-21-4187-2021, 2021
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We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.
Yuzhong Zhang, Daniel J. Jacob, Xiao Lu, Joannes D. Maasakkers, Tia R. Scarpelli, Jian-Xiong Sheng, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Jinfeng Chang, A. Anthony Bloom, Shuang Ma, John Worden, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 21, 3643–3666, https://doi.org/10.5194/acp-21-3643-2021, https://doi.org/10.5194/acp-21-3643-2021, 2021
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We use 2010–2018 satellite observations of atmospheric methane to interpret the factors controlling atmospheric methane and its accelerating increase during the period. The 2010–2018 increase in global methane emissions is driven by tropical and boreal wetlands and tropical livestock (South Asia, Africa, Brazil), with an insignificant positive trend in emissions from the fossil fuel sector. The peak methane growth rates in 2014–2015 are also contributed by low OH and high fire emissions.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 3395–3425, https://doi.org/10.5194/acp-21-3395-2021, https://doi.org/10.5194/acp-21-3395-2021, 2021
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Secondary organic aerosol (SOA) is a major component of submicron particulate matter, but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX SOA concentration changes. The explicit chemistry predicted substantial changes in IEPOX SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physicochemical dependencies in future SOA prediction.
Inés Sanz-Morère, Sebastian D. Eastham, Florian Allroggen, Raymond L. Speth, and Steven R. H. Barrett
Atmos. Chem. Phys., 21, 1649–1681, https://doi.org/10.5194/acp-21-1649-2021, https://doi.org/10.5194/acp-21-1649-2021, 2021
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Contrails cause ~50 % of aviation climate impacts, but this is highly uncertain. This is partly due to the effect of overlap between contrails and other cloud layers. We developed a model to quantify this effect, finding that overlap with natural clouds increased contrails' radiative forcing in 2015. This suggests that cloud avoidance may help in reducing aviation's climate impacts. We also find that contrail–contrail overlap reduces impacts by ~3 %, increasing non-linearly with optical depth.
Gillian D. Thornhill, William J. Collins, Ryan J. Kramer, Dirk Olivié, Ragnhild B. Skeie, Fiona M. O'Connor, Nathan Luke Abraham, Ramiro Checa-Garcia, Susanne E. Bauer, Makoto Deushi, Louisa K. Emmons, Piers M. Forster, Larry W. Horowitz, Ben Johnson, James Keeble, Jean-Francois Lamarque, Martine Michou, Michael J. Mills, Jane P. Mulcahy, Gunnar Myhre, Pierre Nabat, Vaishali Naik, Naga Oshima, Michael Schulz, Christopher J. Smith, Toshihiko Takemura, Simone Tilmes, Tongwen Wu, Guang Zeng, and Jie Zhang
Atmos. Chem. Phys., 21, 853–874, https://doi.org/10.5194/acp-21-853-2021, https://doi.org/10.5194/acp-21-853-2021, 2021
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This paper is a study of how different constituents in the atmosphere, such as aerosols and gases like methane and ozone, affect the energy balance in the atmosphere. Different climate models were run using the same inputs to allow an easy comparison of the results and to understand where the models differ. We found the effect of aerosols is to reduce warming in the atmosphere, but this effect varies between models. Reactions between gases are also important in affecting climate.
Susan S. Kulawik, John R. Worden, Vivienne H. Payne, Dejian Fu, Steven C. Wofsy, Kathryn McKain, Colm Sweeney, Bruce C. Daube Jr., Alan Lipton, Igor Polonsky, Yuguang He, Karen E. Cady-Pereira, Edward J. Dlugokencky, Daniel J. Jacob, and Yi Yin
Atmos. Meas. Tech., 14, 335–354, https://doi.org/10.5194/amt-14-335-2021, https://doi.org/10.5194/amt-14-335-2021, 2021
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This paper shows comparisons of a new single-footprint methane product from the AIRS satellite to aircraft-based observations. We show that this AIRS methane product provides useful information to study seasonal and global methane trends of this important greenhouse gas.
Benjamin Gaubert, Louisa K. Emmons, Kevin Raeder, Simone Tilmes, Kazuyuki Miyazaki, Avelino F. Arellano Jr., Nellie Elguindi, Claire Granier, Wenfu Tang, Jérôme Barré, Helen M. Worden, Rebecca R. Buchholz, David P. Edwards, Philipp Franke, Jeffrey L. Anderson, Marielle Saunois, Jason Schroeder, Jung-Hun Woo, Isobel J. Simpson, Donald R. Blake, Simone Meinardi, Paul O. Wennberg, John Crounse, Alex Teng, Michelle Kim, Russell R. Dickerson, Hao He, Xinrong Ren, Sally E. Pusede, and Glenn S. Diskin
Atmos. Chem. Phys., 20, 14617–14647, https://doi.org/10.5194/acp-20-14617-2020, https://doi.org/10.5194/acp-20-14617-2020, 2020
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This study investigates carbon monoxide pollution in East Asia during spring using a numerical model, satellite remote sensing, and aircraft measurements. We found an underestimation of emission sources. Correcting the emission bias can improve air quality forecasting of carbon monoxide and other species including ozone. Results also suggest that controlling VOC and CO emissions, in addition to widespread NOx controls, can improve ozone pollution over East Asia.
Steven T. Turnock, Robert J. Allen, Martin Andrews, Susanne E. Bauer, Makoto Deushi, Louisa Emmons, Peter Good, Larry Horowitz, Jasmin G. John, Martine Michou, Pierre Nabat, Vaishali Naik, David Neubauer, Fiona M. O'Connor, Dirk Olivié, Naga Oshima, Michael Schulz, Alistair Sellar, Sungbo Shim, Toshihiko Takemura, Simone Tilmes, Kostas Tsigaridis, Tongwen Wu, and Jie Zhang
Atmos. Chem. Phys., 20, 14547–14579, https://doi.org/10.5194/acp-20-14547-2020, https://doi.org/10.5194/acp-20-14547-2020, 2020
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A first assessment is made of the historical and future changes in air pollutants from models participating in the 6th Coupled Model Intercomparison Project (CMIP6). Substantial benefits to future air quality can be achieved in future scenarios that implement measures to mitigate climate and involve reductions in air pollutant emissions, particularly methane. However, important differences are shown between models in the future regional projection of air pollutants under the same scenario.
Junfeng Wang, Jianhuai Ye, Dantong Liu, Yangzhou Wu, Jian Zhao, Weiqi Xu, Conghui Xie, Fuzhen Shen, Jie Zhang, Paul E. Ohno, Yiming Qin, Xiuyong Zhao, Scot T. Martin, Alex K. Y. Lee, Pingqing Fu, Daniel J. Jacob, Qi Zhang, Yele Sun, Mindong Chen, and Xinlei Ge
Atmos. Chem. Phys., 20, 14091–14102, https://doi.org/10.5194/acp-20-14091-2020, https://doi.org/10.5194/acp-20-14091-2020, 2020
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We compared the organics in total submicron matter and those coated on BC cores during summertime in Beijing and found large differences between them. Traffic-related OA was associated significantly with BC, while cooking-related OA did not coat BC. In addition, a factor likely originated from primary biomass burning OA was only identified in BC-containing particles. Such a unique BBOA requires further field and laboratory studies to verify its presence and elucidate its properties and impacts.
David S. Stevenson, Alcide Zhao, Vaishali Naik, Fiona M. O'Connor, Simone Tilmes, Guang Zeng, Lee T. Murray, William J. Collins, Paul T. Griffiths, Sungbo Shim, Larry W. Horowitz, Lori T. Sentman, and Louisa Emmons
Atmos. Chem. Phys., 20, 12905–12920, https://doi.org/10.5194/acp-20-12905-2020, https://doi.org/10.5194/acp-20-12905-2020, 2020
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We present historical trends in atmospheric oxidizing capacity (OC) since 1850 from the latest generation of global climate models and compare these with estimates from measurements. OC controls levels of many key reactive gases, including methane (CH4). We find small model trends up to 1980, then increases of about 9 % up to 2014, disagreeing with (uncertain) measurement-based trends. Major drivers of OC trends are emissions of CH4, NOx, and CO; these will be important for future CH4 trends.
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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Cloud water pH affects atmospheric chemistry, and acid rain damages ecosystems. We use model simulations along with observations to present a global view of cloud water and precipitation pH. Sulfuric acid, nitric acid, and ammonia control the pH in the northern midlatitudes, but carboxylic acids and dust cations are important in the tropics and subtropics. The acid inputs to many nitrogen-saturated ecosystems are high enough to cause acidification, with ammonium as the main acidifying species.
Ke Li, Daniel J. Jacob, Lu Shen, Xiao Lu, Isabelle De Smedt, and Hong Liao
Atmos. Chem. Phys., 20, 11423–11433, https://doi.org/10.5194/acp-20-11423-2020, https://doi.org/10.5194/acp-20-11423-2020, 2020
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Surface summer ozone increased in China from 2013 to 2019 despite new governmental efforts targeting ozone pollution. We find that the ozone increase is mostly due to anthropogenic drivers, although meteorology also plays a role. Further analysis for the North China Plain shows that PM2.5 continued to decrease through 2019, while emissions of volatile organic compounds (VOCs) stayed flat. This could explain the anthropogenic increase in ozone, as PM2.5 scavenges the radical precursors of ozone.
Xiao Lu, Lin Zhang, Tongwen Wu, Michael S. Long, Jun Wang, Daniel J. Jacob, Fang Zhang, Jie Zhang, Sebastian D. Eastham, Lu Hu, Lei Zhu, Xiong Liu, and Min Wei
Geosci. Model Dev., 13, 3817–3838, https://doi.org/10.5194/gmd-13-3817-2020, https://doi.org/10.5194/gmd-13-3817-2020, 2020
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This study presents the development and evaluation of a new climate chemistry model, BCC-GEOS-Chem v1.0, which couples the GEOS-Chem chemical transport model as an atmospheric chemistry component in the Beijing Climate Center atmospheric general circulation model. A 3-year (2012–2014) simulation of BCC-GEOS-Chem v1.0 shows that the model captures well the spatiotemporal distributions of tropospheric ozone, other gaseous pollutants, and aerosols.
Wenfu Tang, Benjamin Gaubert, Louisa Emmons, Yonghoon Choi, Joshua P. DiGangi, Glenn S. Diskin, Xiaomei Xu, Cenlin He, Helen Worden, Simone Tilmes, Rebecca Buchholz, Hannah S. Halliday, and Avelino F. Arellano
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-864, https://doi.org/10.5194/acp-2020-864, 2020
Revised manuscript not accepted
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A specific demonstration of the potential use of correlative information from carbon monoxide to refine estimates of regional carbon dioxide emissions from fossil fuel combustion.
Robert J. Allen, Steven Turnock, Pierre Nabat, David Neubauer, Ulrike Lohmann, Dirk Olivié, Naga Oshima, Martine Michou, Tongwen Wu, Jie Zhang, Toshihiko Takemura, Michael Schulz, Kostas Tsigaridis, Susanne E. Bauer, Louisa Emmons, Larry Horowitz, Vaishali Naik, Twan van Noije, Tommi Bergman, Jean-Francois Lamarque, Prodromos Zanis, Ina Tegen, Daniel M. Westervelt, Philippe Le Sager, Peter Good, Sungbo Shim, Fiona O'Connor, Dimitris Akritidis, Aristeidis K. Georgoulias, Makoto Deushi, Lori T. Sentman, Jasmin G. John, Shinichiro Fujimori, and William J. Collins
Atmos. Chem. Phys., 20, 9641–9663, https://doi.org/10.5194/acp-20-9641-2020, https://doi.org/10.5194/acp-20-9641-2020, 2020
Haipeng Lin, Xu Feng, Tzung-May Fu, Heng Tian, Yaping Ma, Lijuan Zhang, Daniel J. Jacob, Robert M. Yantosca, Melissa P. Sulprizio, Elizabeth W. Lundgren, Jiawei Zhuang, Qiang Zhang, Xiao Lu, Lin Zhang, Lu Shen, Jianping Guo, Sebastian D. Eastham, and Christoph A. Keller
Geosci. Model Dev., 13, 3241–3265, https://doi.org/10.5194/gmd-13-3241-2020, https://doi.org/10.5194/gmd-13-3241-2020, 2020
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Online coupling of meteorology and chemistry models often presents maintenance issues with hard-wired coding. We present WRF-GC, an one-way online coupling of the WRF meteorological model and GEOS-Chem atmospheric chemistry model for regional atmospheric chemistry and air quality modeling. Our coupling structure allows future versions of either parent model to be immediately integrated into WRF-GC. The WRF-GC model was able to well reproduce regional PM2.5 with greater computational efficiency.
Pablo E. Saide, Meng Gao, Zifeng Lu, Daniel L. Goldberg, David G. Streets, Jung-Hun Woo, Andreas Beyersdorf, Chelsea A. Corr, Kenneth L. Thornhill, Bruce Anderson, Johnathan W. Hair, Amin R. Nehrir, Glenn S. Diskin, Jose L. Jimenez, Benjamin A. Nault, Pedro Campuzano-Jost, Jack Dibb, Eric Heim, Kara D. Lamb, Joshua P. Schwarz, Anne E. Perring, Jhoon Kim, Myungje Choi, Brent Holben, Gabriele Pfister, Alma Hodzic, Gregory R. Carmichael, Louisa Emmons, and James H. Crawford
Atmos. Chem. Phys., 20, 6455–6478, https://doi.org/10.5194/acp-20-6455-2020, https://doi.org/10.5194/acp-20-6455-2020, 2020
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Air quality forecasts over the Korean Peninsula captured aerosol optical depth but largely overpredicted surface PM during a Chinese haze transport event. Model deficiency was related to the calculation of optical properties. In order to improve it, aerosol size representation needs to be refined in the calculations, and the representation of aerosol properties, such as size distribution, chemical composition, refractive index, hygroscopicity parameter, and density, needs to be improved.
Lu Shen, Daniel J. Jacob, Mauricio Santillana, Xuan Wang, and Wei Chen
Geosci. Model Dev., 13, 2475–2486, https://doi.org/10.5194/gmd-13-2475-2020, https://doi.org/10.5194/gmd-13-2475-2020, 2020
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Chemical mechanisms in air quality models tend to get more complicated with time, reflecting both increasing knowledge and the need for greater scope. This objectively improves the models but increases the computational burden. In this work, we present an approach that can reduce the computational cost of chemical integration by 30–40 % while maintaining an accuracy better than 1 %. It retains the complexity of the full mechanism where it is needed and preserves full diagnostic information.
Thibaud M. Fritz, Sebastian D. Eastham, Raymond L. Speth, and Steven R. H. Barrett
Atmos. Chem. Phys., 20, 5697–5727, https://doi.org/10.5194/acp-20-5697-2020, https://doi.org/10.5194/acp-20-5697-2020, 2020
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Aircraft exhaust drives formation of ozone and is a dominant anthropogenic influence in the upper troposphere. These impacts are mitigated by non-linear chemistry inside the aircraft plume, which cuts off part of the ozone production pathway and reduces the long-term impact of aircraft in a way which is not captured by current models. The ice clouds which form in aircraft exhaust ("contrails") also play a role, converting emitted nitrogen oxides into more stable forms such as nitric acid.
Rebecca H. Schwantes, Louisa K. Emmons, John J. Orlando, Mary C. Barth, Geoffrey S. Tyndall, Samuel R. Hall, Kirk Ullmann, Jason M. St. Clair, Donald R. Blake, Armin Wisthaler, and Thao Paul V. Bui
Atmos. Chem. Phys., 20, 3739–3776, https://doi.org/10.5194/acp-20-3739-2020, https://doi.org/10.5194/acp-20-3739-2020, 2020
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Ozone is a greenhouse gas and air pollutant that is harmful to human health and plants. During the summer in the southeastern US, many regional and global models are biased high for surface ozone compared to observations. Here adding more complex and updated chemistry for isoprene and terpenes, which are biogenic hydrocarbons emitted from trees and vegetation, into an earth system model greatly reduces the simulated surface ozone bias compared to aircraft and monitoring station data.
Wenfu Tang, Helen M. Worden, Merritt N. Deeter, David P. Edwards, Louisa K. Emmons, Sara Martínez-Alonso, Benjamin Gaubert, Rebecca R. Buchholz, Glenn S. Diskin, Russell R. Dickerson, Xinrong Ren, Hao He, and Yutaka Kondo
Atmos. Meas. Tech., 13, 1337–1356, https://doi.org/10.5194/amt-13-1337-2020, https://doi.org/10.5194/amt-13-1337-2020, 2020
Tia R. Scarpelli, Daniel J. Jacob, Joannes D. Maasakkers, Melissa P. Sulprizio, Jian-Xiong Sheng, Kelly Rose, Lucy Romeo, John R. Worden, and Greet Janssens-Maenhout
Earth Syst. Sci. Data, 12, 563–575, https://doi.org/10.5194/essd-12-563-2020, https://doi.org/10.5194/essd-12-563-2020, 2020
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Methane, a potent greenhouse gas, is emitted through the exploitation of oil, gas, and coal resources, and many efforts to reduce emissions have targeted these sources. We have created a global inventory of oil, gas, and coal methane emissions based on country reporting to the United Nations. The inventory can be used along with satellite observations of methane to better understand the contribution of these sources to global emissions and to identify potential biases in emissions reporting.
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
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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.
Daniel H. Cusworth, Daniel J. Jacob, Daniel J. Varon, Christopher Chan Miller, Xiong Liu, Kelly Chance, Andrew K. Thorpe, Riley M. Duren, Charles E. Miller, David R. Thompson, Christian Frankenberg, Luis Guanter, and Cynthia A. Randles
Atmos. Meas. Tech., 12, 5655–5668, https://doi.org/10.5194/amt-12-5655-2019, https://doi.org/10.5194/amt-12-5655-2019, 2019
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We examine the potential for global detection of methane plumes from individual point sources with the new generation of spaceborne imaging spectrometers scheduled for launch in 2019–2025. We perform methane retrievals on simulated scenes with varying surfaces and atmospheric methane concentrations. Our results suggest that imaging spectrometers in space could play a transformative role in the future for quantifying methane emissions from point sources on a global scale.
Shixian Zhai, Daniel J. Jacob, Xuan Wang, Lu Shen, Ke Li, Yuzhong Zhang, Ke Gui, Tianliang Zhao, and Hong Liao
Atmos. Chem. Phys., 19, 11031–11041, https://doi.org/10.5194/acp-19-11031-2019, https://doi.org/10.5194/acp-19-11031-2019, 2019
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Observed annual mean PM2.5 decreased by 30–50 % in China from 2013–2018. However, meteorologically PM2.5 variability complicates trend attribution. We used a stepwise multiple linear regression model to quantitatively separate contributions from anthropogenic emissions and meteorology. Results show that 88 % of the PM2.5 decrease across China is attributable to anthropogenic emission changes, and 12 % is attributable to meteorology.
Katherine R. Travis and Daniel J. Jacob
Geosci. Model Dev., 12, 3641–3648, https://doi.org/10.5194/gmd-12-3641-2019, https://doi.org/10.5194/gmd-12-3641-2019, 2019
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Models of ozone air pollution are often evaluated with the policy metric set by the EPA of the maximum daily 8 h average ozone concentration. These models may be used in policy settings to evaluate air quality regulations. However, most models have difficulty simulating how ozone varies over the course of the day, and thus the use of this metric in model evaluation is problematic. Improved representation of mixed layer dynamics and ozone loss to the surface is needed to resolve this issue.
Kelvin H. Bates and Daniel J. Jacob
Atmos. Chem. Phys., 19, 9613–9640, https://doi.org/10.5194/acp-19-9613-2019, https://doi.org/10.5194/acp-19-9613-2019, 2019
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Isoprene is a highly reactive chemical released to the atmosphere by plants. Its gas-phase reactions and interactions with chemicals released by human activity have far-reaching atmospheric consequences, contributing to ozone and particulate pollution and prolonging the lifetime of methane, a potent greenhouse gas. We use global simulations with a new isoprene reaction scheme to quantify those effects and to show how recently discovered aspects of isoprene chemistry play out on a global scale.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Eloise A. Marais, Zhe Peng, Benjamin A. Nault, Weiwei Hu, Pedro Campuzano-Jost, and Jose L. Jimenez
Geosci. Model Dev., 12, 2983–3000, https://doi.org/10.5194/gmd-12-2983-2019, https://doi.org/10.5194/gmd-12-2983-2019, 2019
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We developed a parameterization method for IEPOX-SOA based on the detailed chemical mechanism. Our parameterizations were tested using a box model and 3-D chemical transport model, which accurately captured the spatiotemporal distribution and response to changes in emissions compared to the explicit full chemistry, while being more computationally efficient. The method developed in this study can be applied to global climate models for long-term studies with a lower computational cost.
Rachel F. Silvern, Daniel J. Jacob, Loretta J. Mickley, Melissa P. Sulprizio, Katherine R. Travis, Eloise A. Marais, Ronald C. Cohen, Joshua L. Laughner, Sungyeon Choi, Joanna Joiner, and Lok N. Lamsal
Atmos. Chem. Phys., 19, 8863–8878, https://doi.org/10.5194/acp-19-8863-2019, https://doi.org/10.5194/acp-19-8863-2019, 2019
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The US EPA reports a steady decrease in nitrogen oxide (NOx) emissions from fuel combustion over the 2005–2017 period, while satellite observations show a leveling off after 2009, suggesting emission reductions and related air quality gains have halted. We show the sustained decrease in NOx emissions is in fact consistent with observed trends in surface NO2 and ozone concentrations and that the flattening of the satellite trend reflects a growing influence from the non-anthropogenic background.
Joannes D. Maasakkers, Daniel J. Jacob, Melissa P. Sulprizio, Tia R. Scarpelli, Hannah Nesser, Jian-Xiong Sheng, Yuzhong Zhang, Monica Hersher, A. Anthony Bloom, Kevin W. Bowman, John R. Worden, Greet Janssens-Maenhout, and Robert J. Parker
Atmos. Chem. Phys., 19, 7859–7881, https://doi.org/10.5194/acp-19-7859-2019, https://doi.org/10.5194/acp-19-7859-2019, 2019
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We use 2010–2015 satellite observations of atmospheric methane to improve estimates of methane emissions and their trends, as well as the concentration and trend of tropospheric OH (hydroxyl radical, methane's main sink). We find overestimates of Chinese coal and Middle East oil/gas emissions in the prior estimate. The 2010–2015 growth in methane is attributed to an increase in emissions from India, China, and areas with large tropical wetlands. The contribution from OH is small in comparison.
Lu Shen, Daniel J. Jacob, Xiong Liu, Guanyu Huang, Ke Li, Hong Liao, and Tao Wang
Atmos. Chem. Phys., 19, 6551–6560, https://doi.org/10.5194/acp-19-6551-2019, https://doi.org/10.5194/acp-19-6551-2019, 2019
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Shaojie Song, Meng Gao, Weiqi Xu, Yele Sun, Douglas R. Worsnop, John T. Jayne, Yuzhong Zhang, Lei Zhu, Mei Li, Zhen Zhou, Chunlei Cheng, Yibing Lv, Ying Wang, Wei Peng, Xiaobin Xu, Nan Lin, Yuxuan Wang, Shuxiao Wang, J. William Munger, Daniel J. Jacob, and Michael B. McElroy
Atmos. Chem. Phys., 19, 1357–1371, https://doi.org/10.5194/acp-19-1357-2019, https://doi.org/10.5194/acp-19-1357-2019, 2019
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Chemistry responsible for sulfate production in northern China winter haze remains mysterious. We propose a potentially key pathway through the reaction of formaldehyde and sulfur dioxide that has not been accounted for in previous studies. The special atmospheric conditions favor the formation and existence of their complex, hydroxymethanesulfonate (HMS).
Lu Shen, Daniel J. Jacob, Loretta J. Mickley, Yuxuan Wang, and Qiang Zhang
Atmos. Chem. Phys., 18, 17489–17496, https://doi.org/10.5194/acp-18-17489-2018, https://doi.org/10.5194/acp-18-17489-2018, 2018
Eloise A. Marais, Daniel J. Jacob, Sungyeon Choi, Joanna Joiner, Maria Belmonte-Rivas, Ronald C. Cohen, Steffen Beirle, Lee T. Murray, Luke D. Schiferl, Viral Shah, and Lyatt Jaeglé
Atmos. Chem. Phys., 18, 17017–17027, https://doi.org/10.5194/acp-18-17017-2018, https://doi.org/10.5194/acp-18-17017-2018, 2018
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We intercompare two new products of global upper tropospheric nitrogen dioxide (NO2) retrieved from the Ozone Monitoring Instrument (OMI). We evaluate these products with aircraft observations from NASA DC8 aircraft campaigns and interpret the useful information these products can provide about nitrogen oxides (NOx) in the global upper troposphere using the GEOS-Chem chemical transport model.
Jian-Xiong Sheng, Daniel J. Jacob, Joannes D. Maasakkers, Yuzhong Zhang, and Melissa P. Sulprizio
Atmos. Meas. Tech., 11, 6379–6388, https://doi.org/10.5194/amt-11-6379-2018, https://doi.org/10.5194/amt-11-6379-2018, 2018
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We conduct Observing System Simulation Experiments to compare the ability of future satellite measurements of atmospheric methane columns for constraining methane emissions at the 25 km scale. We find that the geostationary instruments can do much better than TROPOMI and are less sensitive to cloud cover. GeoCARB observing twice a day would provide 70 % of the information from the nominal GEO-CAPE mission considered by NASA in response to the Decadal Survey of the US National Research Council.
Daniel H. Cusworth, Daniel J. Jacob, Jian-Xiong Sheng, Joshua Benmergui, Alexander J. Turner, Jeremy Brandman, Laurent White, and Cynthia A. Randles
Atmos. Chem. Phys., 18, 16885–16896, https://doi.org/10.5194/acp-18-16885-2018, https://doi.org/10.5194/acp-18-16885-2018, 2018
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Methane emissions from oil/gas fields originate from a large number of small and densely clustered point sources. We examine the potential of recently launched or planned satellites to locate these high-mode emitters through measurements of atmospheric methane. We find that the recently launched TROPOMI and the planned GeoCARB instruments are successful at locating high-emitting sources for fields of 20-50 emitters within the 50 × 50 km2 geographic domain but are unsuccessful for denser fields.
Lu Hu, Christoph A. Keller, Michael S. Long, Tomás Sherwen, Benjamin Auer, Arlindo Da Silva, Jon E. Nielsen, Steven Pawson, Matthew A. Thompson, Atanas L. Trayanov, Katherine R. Travis, Stuart K. Grange, Mat J. Evans, and Daniel J. Jacob
Geosci. Model Dev., 11, 4603–4620, https://doi.org/10.5194/gmd-11-4603-2018, https://doi.org/10.5194/gmd-11-4603-2018, 2018
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We present a full-year online global simulation of tropospheric chemistry at 12.5 km resolution. To the best of our knowledge, such a resolution in a state-of-the-science global simulation of tropospheric chemistry is unprecedented. This simulation will serve as the Nature Run for observing system simulation experiments to support the future geostationary satellite constellation for tropospheric chemistry, and can also be used for various air quality applications.
Yuzhong Zhang, Daniel J. Jacob, Joannes D. Maasakkers, Melissa P. Sulprizio, Jian-Xiong Sheng, Ritesh Gautam, and John Worden
Atmos. Chem. Phys., 18, 15959–15973, https://doi.org/10.5194/acp-18-15959-2018, https://doi.org/10.5194/acp-18-15959-2018, 2018
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We assess the potential of using satellite observations of atmospheric methane to monitor global mean tropospheric OH concentration, a key parameter for the oxidizing power of the atmosphere.
Xinyi Dong, Joshua S. Fu, Qingzhao Zhu, Jian Sun, Jiani Tan, Terry Keating, Takashi Sekiya, Kengo Sudo, Louisa Emmons, Simone Tilmes, Jan Eiof Jonson, Michael Schulz, Huisheng Bian, Mian Chin, Yanko Davila, Daven Henze, Toshihiko Takemura, Anna Maria Katarina Benedictow, and Kan Huang
Atmos. Chem. Phys., 18, 15581–15600, https://doi.org/10.5194/acp-18-15581-2018, https://doi.org/10.5194/acp-18-15581-2018, 2018
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We have applied the HTAP phase II multi-model data to investigate the long-range transport impacts on surface concentration and column density of PM from Europe and Russia, Belarus, and Ukraine to eastern Asia, with a special focus on the long-range transport contribution during haze episodes in China. We found that long-range transport plays a more important role in elevating the background concentration of surface PM during the haze days.
Daniel J. Varon, Daniel J. Jacob, Jason McKeever, Dylan Jervis, Berke O. A. Durak, Yan Xia, and Yi Huang
Atmos. Meas. Tech., 11, 5673–5686, https://doi.org/10.5194/amt-11-5673-2018, https://doi.org/10.5194/amt-11-5673-2018, 2018
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Methane is a powerful greenhouse gas emitted from numerous human activities. Space-based observation of point sources would be a cost-effective monitoring solution, but the resolution of most current and planned methane-observing satellites is too coarse to resolve individual emitters. We simulate fine-resolution (50 m) satellite observations of methane plumes as would be measured by GHGSat (to be launched in 2019) and show that such data can usefully quantify large methane point sources.
Benjamin Brown-Steiner, Noelle E. Selin, Ronald Prinn, Simone Tilmes, Louisa Emmons, Jean-François Lamarque, and Philip Cameron-Smith
Geosci. Model Dev., 11, 4155–4174, https://doi.org/10.5194/gmd-11-4155-2018, https://doi.org/10.5194/gmd-11-4155-2018, 2018
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We conduct three simulations of atmospheric chemistry using chemical mechanisms of different levels of complexity and compare their results to observations. We explore situations in which the simplified mechanisms match the output of the most complex mechanism, as well as when they diverge. We investigate how concurrent utilization of chemical mechanisms of different complexities can further our atmospheric-chemistry understanding at various scales and give some strategies for future research.
Jan Eiof Jonson, Michael Schulz, Louisa Emmons, Johannes Flemming, Daven Henze, Kengo Sudo, Marianne Tronstad Lund, Meiyun Lin, Anna Benedictow, Brigitte Koffi, Frank Dentener, Terry Keating, Rigel Kivi, and Yanko Davila
Atmos. Chem. Phys., 18, 13655–13672, https://doi.org/10.5194/acp-18-13655-2018, https://doi.org/10.5194/acp-18-13655-2018, 2018
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Focusing on Europe, this HTAP 2 study computes ozone in several global models when reducing anthropogenic emissions by 20 % in different world regions. The differences in model results are explored
by use of a novel stepwise approach combining a tracer, CO and ozone. For ozone the contributions from the rest of the world are larger than from Europe, with the largest contributions from North America and eastern Asia. Contributions do, however, depend on the choice of ozone metric.
Jian-Xiong Sheng, Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Joshua Benmergui, A. Anthony Bloom, Claudia Arndt, Ritesh Gautam, Daniel Zavala-Araiza, Hartmut Boesch, and Robert J. Parker
Atmos. Chem. Phys., 18, 12257–12267, https://doi.org/10.5194/acp-18-12257-2018, https://doi.org/10.5194/acp-18-12257-2018, 2018
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Analysis of 7 years (2010–2016) of GOSAT methane trends over Canada, the contiguous US, and Mexico suggests that US methane emissions increased by 2.5 ± 1.4 % a−1 over the 7-year period, with contributions from both oil–gas systems and livestock in the Midwest. Mexican emissions show a decrease that can be attributed to a decreasing cattle population. Canadian emissions show year-to-year variability driven by wetland emissions and correlated with wetland areal extent.
Jiani Tan, Joshua S. Fu, Frank Dentener, Jian Sun, Louisa Emmons, Simone Tilmes, Johannes Flemming, Toshihiko Takemura, Huisheng Bian, Qingzhao Zhu, Cheng-En Yang, and Terry Keating
Atmos. Chem. Phys., 18, 12223–12240, https://doi.org/10.5194/acp-18-12223-2018, https://doi.org/10.5194/acp-18-12223-2018, 2018
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Have contributions of hemispheric air pollution to deposition at global scale been overlooked in the past years? How do we assess the critical load for the acid deposition when we look for the demand of forest and crop? This study highlights the significant impact of hemispheric transport on deposition in coastal regions, open ocean and low-emission regions. Further research is proposed for improving ecosystem and human health in these regions, with regards to the enhanced hemispheric transport.
Sebastian D. Eastham, Michael S. Long, Christoph A. Keller, Elizabeth Lundgren, Robert M. Yantosca, Jiawei Zhuang, Chi Li, Colin J. Lee, Matthew Yannetti, Benjamin M. Auer, Thomas L. Clune, Jules Kouatchou, William M. Putman, Matthew A. Thompson, Atanas L. Trayanov, Andrea M. Molod, Randall V. Martin, and Daniel J. Jacob
Geosci. Model Dev., 11, 2941–2953, https://doi.org/10.5194/gmd-11-2941-2018, https://doi.org/10.5194/gmd-11-2941-2018, 2018
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Global atmospheric chemical transport models are crucial tools in atmospheric science, used to address problems ranging from climate change to acid rain. GEOS-Chem High Performance (GCHP) is a new implementation of the widely used GEOS-Chem model, designed for massively parallel architectures. GCHP v11-02c is shown to be highly scalable from 6 to over 500 cores, enabling the routine simulation of global atmospheric chemistry from the surface to the stratopause at resolutions of ~50 km or finer.
Ciao-Kai Liang, J. Jason West, Raquel A. Silva, Huisheng Bian, Mian Chin, Yanko Davila, Frank J. Dentener, Louisa Emmons, Johannes Flemming, Gerd Folberth, Daven Henze, Ulas Im, Jan Eiof Jonson, Terry J. Keating, Tom Kucsera, Allen Lenzen, Meiyun Lin, Marianne Tronstad Lund, Xiaohua Pan, Rokjin J. Park, R. Bradley Pierce, Takashi Sekiya, Kengo Sudo, and Toshihiko Takemura
Atmos. Chem. Phys., 18, 10497–10520, https://doi.org/10.5194/acp-18-10497-2018, https://doi.org/10.5194/acp-18-10497-2018, 2018
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Emissions from one continent affect air quality and health elsewhere. Here we quantify the effects of intercontinental PM2.5 and ozone transport on human health using a new multi-model ensemble, evaluating the health effects of emissions from six world regions and three emission source sectors. Emissions from one region have significant health impacts outside of that source region; similarly, foreign emissions contribute significantly to air-pollution-related deaths in several world regions.
Steven T. Turnock, Oliver Wild, Frank J. Dentener, Yanko Davila, Louisa K. Emmons, Johannes Flemming, Gerd A. Folberth, Daven K. Henze, Jan E. Jonson, Terry J. Keating, Sudo Kengo, Meiyun Lin, Marianne Lund, Simone Tilmes, and Fiona M. O'Connor
Atmos. Chem. Phys., 18, 8953–8978, https://doi.org/10.5194/acp-18-8953-2018, https://doi.org/10.5194/acp-18-8953-2018, 2018
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A simple parameterisation was developed in this study to provide a rapid assessment of the impacts and uncertainties associated with future emission control strategies by predicting changes to surface ozone air quality and near-term climate forcing of ozone. Future emissions scenarios based on currently implemented legislation are shown to worsen surface ozone air quality and enhance near-term climate warming, with changes in methane becoming increasingly important in the future.
Benjamin Brown-Steiner, Noelle E. Selin, Ronald G. Prinn, Erwan Monier, Simone Tilmes, Louisa Emmons, and Fernando Garcia-Menendez
Atmos. Chem. Phys., 18, 8373–8388, https://doi.org/10.5194/acp-18-8373-2018, https://doi.org/10.5194/acp-18-8373-2018, 2018
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Detecting signals in observations and simulations of atmospheric chemistry is difficult due to the underlying variability in the chemistry, meteorology, and climatology. Here we examine the scale dependence of ozone variability and explore strategies for reducing or averaging this variability and thereby enhancing ozone signal detection capabilities. We find that 10–15 years of temporal averaging, and some level of spatial averaging, reduces the risk of overconfidence in ozone signals.
Alexander J. Turner, Daniel J. Jacob, Joshua Benmergui, Jeremy Brandman, Laurent White, and Cynthia A. Randles
Atmos. Chem. Phys., 18, 8265–8278, https://doi.org/10.5194/acp-18-8265-2018, https://doi.org/10.5194/acp-18-8265-2018, 2018
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We conduct a 1-week WRF-STILT simulation to generate methane column footprints at 1.3 km spatial resolution and hourly temporal resolution over the Barnett Shale. We find that a week of TROPOMI observations should provide regional (~30 km) information on temporally invariant sources and GeoCARB should provide information on temporally invariant sources at 2–7 km spatial resolution. An instrument precision better than 6 ppb is an important threshold for achieving fine resolution of emissions.
Jiani Tan, Joshua S. Fu, Frank Dentener, Jian Sun, Louisa Emmons, Simone Tilmes, Kengo Sudo, Johannes Flemming, Jan Eiof Jonson, Sylvie Gravel, Huisheng Bian, Yanko Davila, Daven K. Henze, Marianne T. Lund, Tom Kucsera, Toshihiko Takemura, and Terry Keating
Atmos. Chem. Phys., 18, 6847–6866, https://doi.org/10.5194/acp-18-6847-2018, https://doi.org/10.5194/acp-18-6847-2018, 2018
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We study the distributions of sulfur and nitrogen deposition, which are associated with current environmental issues such as formation of acid rain and ecosystem eutrophication and result in widespread problems such as loss of environmental diversity, harming the crop yield and even food insecurity. According to our study, both the amount and distribution of sulfate and nitrogen deposition have changed significantly in the last decade, particularly in East Asia, South Asia and Southeast Asia.
Jian-Xiong Sheng, Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Melissa P. Sulprizio, A. Anthony Bloom, Arlyn E. Andrews, and Debra Wunch
Atmos. Chem. Phys., 18, 6483–6491, https://doi.org/10.5194/acp-18-6483-2018, https://doi.org/10.5194/acp-18-6483-2018, 2018
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We use observations of boundary layer methane from the SEAC4RS aircraft campaign over the Southeast US to estimate methane emissions in that region. Our results suggest that the EPA inventory is regionally unbiased but there are large local biases, suggesting variable emission factors. Our results also suggest that the choice of landcover map is the dominant source of error for wetland emission estimates.
Jiawei Zhuang, Daniel J. Jacob, and Sebastian D. Eastham
Atmos. Chem. Phys., 18, 6039–6055, https://doi.org/10.5194/acp-18-6039-2018, https://doi.org/10.5194/acp-18-6039-2018, 2018
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Our work explains why current model simulations are unable to capture the intercontinental influences of pollution plumes that are often observed over some regions like California. Due to inadequate vertical grid resolution in these models, the plumes get diffused too rapidly during intercontinental transport. Increasing the vertical grid resolution greatly improves the simulation of plumes and considerably increases the estimate of local surface pollution influence.
Jennifer Kaiser, Daniel J. Jacob, Lei Zhu, Katherine R. Travis, Jenny A. Fisher, Gonzalo González Abad, Lin Zhang, Xuesong Zhang, Alan Fried, John D. Crounse, Jason M. St. Clair, and Armin Wisthaler
Atmos. Chem. Phys., 18, 5483–5497, https://doi.org/10.5194/acp-18-5483-2018, https://doi.org/10.5194/acp-18-5483-2018, 2018
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Isoprene emissions from vegetation have a large effect on atmospheric chemistry and air quality. Here we use the adjoint of GEOS-Chem in an inversion of OMI formaldehyde observations to produce top-down estimates of isoprene emissions in the southeast US during the summer of 2013. We find that MEGAN v2.1 is biased high on average by 40 %. Our downward correction of isoprene emissions leads to a small reduction in modeled surface O3 and decreases the contribution of isoprene to organic aerosol.
Karen Yu, Christoph A. Keller, Daniel J. Jacob, Andrea M. Molod, Sebastian D. Eastham, and Michael S. Long
Geosci. Model Dev., 11, 305–319, https://doi.org/10.5194/gmd-11-305-2018, https://doi.org/10.5194/gmd-11-305-2018, 2018
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Global simulations of atmospheric chemistry are generally conducted with off-line chemical transport models (CTMs) driven by archived meteorological data from general circulation models (GCMs). The off-line approach has the advantages of simplicity and expediency, but it is unable to reproduce the GCM transport exactly. We investigate the cascade of errors associated with the off-line approach using the GEOS-5 GCM and GEOS-Chem CTM and discuss improvements in the use of archived meteorology.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Jihyun Han, Meehye Lee, Xiaona Shang, Gangwoong Lee, and Louisa K. Emmons
Atmos. Chem. Phys., 17, 10619–10631, https://doi.org/10.5194/acp-17-10619-2017, https://doi.org/10.5194/acp-17-10619-2017, 2017
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Peroxyacetyl nitrate (PAN) was first measured at Gosan Climate Observatory during the fall of 2010, when PAN was better correlated with PM10 than with O3. In particular, PAN and O3 concentrations were greatly elevated in haze and the Beijing plume and much higher than those from model simulation. This study highlights the decoupling of PAN from O3 in Chinese outflows and suggests PAN as a potential indicator of overall aerosol formation in aged air masses impacted by biomass burning.
Katherine R. Travis, Daniel J. Jacob, Christoph A. Keller, Shi Kuang, Jintai Lin, Michael J. Newchurch, and Anne M. Thompson
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-596, https://doi.org/10.5194/acp-2017-596, 2017
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Models severely overestimate surface ozone in the Southeast US during summertime which has implications for the design of air quality regulations. We use a model (GEOS-Chem) to interpret ozone observations from a suite of observations taken during August–September 2013. The model is unbiased relative to observations below 1 km but is biased high at the surface. We attribute this bias to model representation error, an underestimate in low-cloud, and insufficient treatment of vertical mixing.
Christopher Chan Miller, Daniel J. Jacob, Eloise A. Marais, Karen Yu, Katherine R. Travis, Patrick S. Kim, Jenny A. Fisher, Lei Zhu, Glenn M. Wolfe, Thomas F. Hanisco, Frank N. Keutsch, Jennifer Kaiser, Kyung-Eun Min, Steven S. Brown, Rebecca A. Washenfelder, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 17, 8725–8738, https://doi.org/10.5194/acp-17-8725-2017, https://doi.org/10.5194/acp-17-8725-2017, 2017
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The use of satellite glyoxal observations for estimating isoprene emissions has been limited by knowledge of the glyoxal yield from isoprene. We use SENEX aircraft observations over the southeast US to evaluate glyoxal yields from isoprene in a 3-D atmospheric model. The SENEX observations support a pathway for glyoxal formation in pristine regions that we propose here, which may have implications for improving isoprene emissions estimates from upcoming high-resolution geostationary satellites.
A. Anthony Bloom, Kevin W. Bowman, Meemong Lee, Alexander J. Turner, Ronny Schroeder, John R. Worden, Richard Weidner, Kyle C. McDonald, and Daniel J. Jacob
Geosci. Model Dev., 10, 2141–2156, https://doi.org/10.5194/gmd-10-2141-2017, https://doi.org/10.5194/gmd-10-2141-2017, 2017
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Wetland emissions are a principal source of uncertainty in the global atmospheric methane budget due to poor knowledge of wetland processes. We construct a wetland methane emission and uncertainty dataset for use in global atmospheric methane models. Our wetland model ensemble is based on static wetland maps, satellite-derived inundation and carbon cycle models. The ensemble performs favourably against regional flux estimates and atmospheric methane measurements relative to previous studies.
Hannah M. Horowitz, Daniel J. Jacob, Yanxu Zhang, Theodore S. Dibble, Franz Slemr, Helen M. Amos, Johan A. Schmidt, Elizabeth S. Corbitt, Eloïse A. Marais, and Elsie M. Sunderland
Atmos. Chem. Phys., 17, 6353–6371, https://doi.org/10.5194/acp-17-6353-2017, https://doi.org/10.5194/acp-17-6353-2017, 2017
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Mercury is a toxic, global pollutant released to the air from human activities like coal burning. Chemical reactions in air determine how far mercury is transported before it is deposited to the environment, where it may be converted to a form that accumulates in fish. We use a 3-D atmospheric model to evaluate a new set of chemical reactions and its effects on mercury deposition. We find it is consistent with observations and leads to increased deposition to oceans, especially in the tropics.
Min Huang, Gregory R. Carmichael, R. Bradley Pierce, Duseong S. Jo, Rokjin J. Park, Johannes Flemming, Louisa K. Emmons, Kevin W. Bowman, Daven K. Henze, Yanko Davila, Kengo Sudo, Jan Eiof Jonson, Marianne Tronstad Lund, Greet Janssens-Maenhout, Frank J. Dentener, Terry J. Keating, Hilke Oetjen, and Vivienne H. Payne
Atmos. Chem. Phys., 17, 5721–5750, https://doi.org/10.5194/acp-17-5721-2017, https://doi.org/10.5194/acp-17-5721-2017, 2017
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In support of the HTAP phase 2 experiment, we conducted a number of regional-scale Sulfur Transport and dEposition Model base and sensitivity simulations over North America during May–June 2010. The STEM chemical boundary conditions were downscaled from three (GEOS-Chem, RAQMS, and ECMWF C-IFS) global chemical transport models' simulations. Analyses were performed on large spatial–temporal scales relative to HTAP1 and also on subcontinental and event scales including the use of satellite data.
Rachel F. Silvern, Daniel J. Jacob, Patrick S. Kim, Eloise A. Marais, Jay R. Turner, Pedro Campuzano-Jost, and Jose L. Jimenez
Atmos. Chem. Phys., 17, 5107–5118, https://doi.org/10.5194/acp-17-5107-2017, https://doi.org/10.5194/acp-17-5107-2017, 2017
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We identify a fundamental discrepancy between thermodynamic equilibrium theory and observations of inorganic aerosol composition in the eastern US in summer that shows low ammonium sulfate aerosol ratios. In addition, from 2003 to 2013, while SO2 emissions have declined due to US emission controls, aerosols have become more acidic in the southeastern US. To explain these observations, we suggest that the large and increasing source of organic aerosol may be affecting thermodynamic equilibrium.
Sebastian D. Eastham and Daniel J. Jacob
Atmos. Chem. Phys., 17, 2543–2553, https://doi.org/10.5194/acp-17-2543-2017, https://doi.org/10.5194/acp-17-2543-2017, 2017
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Intercontinental atmospheric transport can disrupt local chemistry and cause air quality issues thousands of kilometers from the source, complicating correct attribution of air quality exceedances. This transport occurs in long, thin plumes which current-generation models consistently fail to reproduce. Our study investigates the cause of this failure, finding that greater vertical resolution than is currently available is required to reliably resolve the plumes and their effects.
Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Jianxiong Sheng, Kang Sun, Xiong Liu, Kelly Chance, Ilse Aben, Jason McKeever, and Christian Frankenberg
Atmos. Chem. Phys., 16, 14371–14396, https://doi.org/10.5194/acp-16-14371-2016, https://doi.org/10.5194/acp-16-14371-2016, 2016
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Methane is a greenhouse gas emitted by a range of natural and anthropogenic sources. Atmospheric methane has been measured continuously from space since 2003, and new instruments are planned to launch in the near future that will greatly expand the capabilities of space-based observations. We review the value of current, future, and proposed satellite observations to better quantify methane emissions from the global scale down to the scale of point sources.
Katherine R. Travis, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Lei Zhu, Karen Yu, Christopher C. Miller, Robert M. Yantosca, Melissa P. Sulprizio, Anne M. Thompson, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Ronald C. Cohen, Joshua L. Laughner, Jack E. Dibb, Samuel R. Hall, Kirk Ullmann, Glenn M. Wolfe, Illana B. Pollack, Jeff Peischl, Jonathan A. Neuman, and Xianliang Zhou
Atmos. Chem. Phys., 16, 13561–13577, https://doi.org/10.5194/acp-16-13561-2016, https://doi.org/10.5194/acp-16-13561-2016, 2016
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Ground-level ozone pollution in the Southeast US involves complex chemistry driven by anthropogenic emissions of nitrogen oxides (NOx) and biogenic emissions of isoprene. We find that US NOx emissions are overestimated nationally by as much as 50 % and that reducing model emissions by this amount results in good agreement with SEAC4RS aircraft measurements in August and September 2013. Observations of nitrate wet deposition fluxes and satellite NO2 columns further support this result.
Lei Zhu, Daniel J. Jacob, Patrick S. Kim, Jenny A. Fisher, Karen Yu, Katherine R. Travis, Loretta J. Mickley, Robert M. Yantosca, Melissa P. Sulprizio, Isabelle De Smedt, Gonzalo González Abad, Kelly Chance, Can Li, Richard Ferrare, Alan Fried, Johnathan W. Hair, Thomas F. Hanisco, Dirk Richter, Amy Jo Scarino, James Walega, Petter Weibring, and Glenn M. Wolfe
Atmos. Chem. Phys., 16, 13477–13490, https://doi.org/10.5194/acp-16-13477-2016, https://doi.org/10.5194/acp-16-13477-2016, 2016
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HCHO column data are widely used as a proxy for VOCs emissions, but validation of the data has been extremely limited. We use accurate aircraft observations to validate and intercompare 6 HCHO retrievals with GEOS-Chem as the intercomparison platform. Retrievals are interconsistent in spatial variability over the SE US and in daily variability, but are biased low by 20–51 %. Our work supports the use of HCHO column as a quantitative proxy for isoprene emission after correction of the low bias.
Camilla Weum Stjern, Bjørn Hallvard Samset, Gunnar Myhre, Huisheng Bian, Mian Chin, Yanko Davila, Frank Dentener, Louisa Emmons, Johannes Flemming, Amund Søvde Haslerud, Daven Henze, Jan Eiof Jonson, Tom Kucsera, Marianne Tronstad Lund, Michael Schulz, Kengo Sudo, Toshihiko Takemura, and Simone Tilmes
Atmos. Chem. Phys., 16, 13579–13599, https://doi.org/10.5194/acp-16-13579-2016, https://doi.org/10.5194/acp-16-13579-2016, 2016
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Air pollution can reach distant regions through intercontinental transport. Here we first present results from the Hemispheric Transport of Air Pollution Phase 2 exercise, where many models performed the same set of coordinated emission-reduction experiments. We find that mitigations have considerable extra-regional effects, and show that this is particularly true for black carbon emissions, as long-range transport elevates aerosols to higher levels where their radiative influence is stronger.
Tomás Sherwen, Johan A. Schmidt, Mat J. Evans, Lucy J. Carpenter, Katja Großmann, Sebastian D. Eastham, Daniel J. Jacob, Barbara Dix, Theodore K. Koenig, Roman Sinreich, Ivan Ortega, Rainer Volkamer, Alfonso Saiz-Lopez, Cristina Prados-Roman, Anoop S. Mahajan, and Carlos Ordóñez
Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, https://doi.org/10.5194/acp-16-12239-2016, 2016
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We present a simulation of tropospheric Cl, Br, I chemistry within the GEOS-Chem CTM. We find a decrease in tropospheric ozone burden of 18.6 % and a 8.2 % decrease in global mean OH concentrations. Cl oxidation of some VOCs range from 15 to 27 % of the total loss. Bromine plays a small role in oxidising oVOCs. Surface ozone, ozone sondes, and methane lifetime are in general improved by the inclusion of halogens. We argue that simulated bromine and chlorine represent a lower limit.
Sarah A. Strode, Helen M. Worden, Megan Damon, Anne R. Douglass, Bryan N. Duncan, Louisa K. Emmons, Jean-Francois Lamarque, Michael Manyin, Luke D. Oman, Jose M. Rodriguez, Susan E. Strahan, and Simone Tilmes
Atmos. Chem. Phys., 16, 7285–7294, https://doi.org/10.5194/acp-16-7285-2016, https://doi.org/10.5194/acp-16-7285-2016, 2016
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We use global models to interpret trends in MOPITT observations of CO. Simulations with time-dependent emissions reproduce the observed trends over the eastern USA and Europe, suggesting that the emissions are reasonable for these regions. The simulations produce a positive trend over eastern China, contrary to the observed negative trend. This may indicate that the assumed emission trend over China is too positive. However, large variability in the overhead ozone column also contributes.
Simone Tilmes, Jean-Francois Lamarque, Louisa K. Emmons, Doug E. Kinnison, Dan Marsh, Rolando R. Garcia, Anne K. Smith, Ryan R. Neely, Andrew Conley, Francis Vitt, Maria Val Martin, Hiroshi Tanimoto, Isobel Simpson, Don R. Blake, and Nicola Blake
Geosci. Model Dev., 9, 1853–1890, https://doi.org/10.5194/gmd-9-1853-2016, https://doi.org/10.5194/gmd-9-1853-2016, 2016
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The state of the art Community Earth System Model, CESM1 CAM4-chem has been used to perform reference and sensitivity simulations as part of the Chemistry Climate Model Initiative (CCMI). Specifics of the model and details regarding the setup of the simulations are described. In additions, the main behavior of the model, including selected chemical species have been evaluated with climatological datasets. This paper is therefore a references for studies that use the provided model results.
Jenny A. Fisher, Daniel J. Jacob, Katherine R. Travis, Patrick S. Kim, Eloise A. Marais, Christopher Chan Miller, Karen Yu, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Jingqiu Mao, Paul O. Wennberg, John D. Crounse, Alex P. Teng, Tran B. Nguyen, Jason M. St. Clair, Ronald C. Cohen, Paul Romer, Benjamin A. Nault, Paul J. Wooldridge, Jose L. Jimenez, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Paul B. Shepson, Fulizi Xiong, Donald R. Blake, Allen H. Goldstein, Pawel K. Misztal, Thomas F. Hanisco, Glenn M. Wolfe, Thomas B. Ryerson, Armin Wisthaler, and Tomas Mikoviny
Atmos. Chem. Phys., 16, 5969–5991, https://doi.org/10.5194/acp-16-5969-2016, https://doi.org/10.5194/acp-16-5969-2016, 2016
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We use new airborne and ground-based observations from two summer 2013 campaigns in the southeastern US, interpreted with a chemical transport model, to understand the impact of isoprene and monoterpene chemistry on the atmospheric NOx budget via production of organic nitrates (RONO2). We find that a diversity of species contribute to observed RONO2. Our work implies that the NOx sink to RONO2 production is only sensitive to NOx emissions in regions where they are already low.
Catherine Wespes, Daniel Hurtmans, Louisa K. Emmons, Sarah Safieddine, Cathy Clerbaux, David P. Edwards, and Pierre-François Coheur
Atmos. Chem. Phys., 16, 5721–5743, https://doi.org/10.5194/acp-16-5721-2016, https://doi.org/10.5194/acp-16-5721-2016, 2016
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In this paper, we assess how daily ozone measurements from the Infrared Atmospheric Sounding Interferometer (IASI/MetOp) can contribute to the analyses of the processes driving O3 variability in the troposphere and the stratosphere with a set of parameterized geophysical variables, and we demonstrate the added value of IASI exceptional frequency sampling for monitoring medium- to long-term changes in global ozone concentrations in the future.
Christopher Chan Miller, Daniel J. Jacob, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 16, 4631–4639, https://doi.org/10.5194/acp-16-4631-2016, https://doi.org/10.5194/acp-16-4631-2016, 2016
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Volatile organic compounds (VOCs) are important precursors for photochemical smog.
Glyoxal is an organic compound produced in the atmosphere from reactions of larger VOCs. OMI satellite observations of glyoxal show a large hotspot over the Pearl River delta. The hotspot can be explained by industrial paint and solvent emissions of aromatic VOCs. Our work shows OMI observations are consistent with current VOC emissions estimates, whereas previous work has suggested large underestimates.
Karen Yu, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Christopher C. Miller, Katherine R. Travis, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Ron C. Cohen, Jack E. Dibb, Alan Fried, Tomas Mikoviny, Thomas B. Ryerson, Paul O. Wennberg, and Armin Wisthaler
Atmos. Chem. Phys., 16, 4369–4378, https://doi.org/10.5194/acp-16-4369-2016, https://doi.org/10.5194/acp-16-4369-2016, 2016
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Increasing the spatial resolution of a chemical transport model may improve simulations but can be computationally expensive. Using observations from the SEAC4RS aircraft campaign, we find that at higher spatial resolutions, models are better able to simulate the chemical pathways of ozone precursors, but the overall effect on regional mean concentrations is small. This implies that for continental boundary layer applications, coarse resolution models are adequate.
E. A. Marais, D. J. Jacob, J. L. Jimenez, P. Campuzano-Jost, D. A. Day, W. Hu, J. Krechmer, L. Zhu, P. S. Kim, C. C. Miller, J. A. Fisher, K. Travis, K. Yu, T. F. Hanisco, G. M. Wolfe, H. L. Arkinson, H. O. T. Pye, K. D. Froyd, J. Liao, and V. F. McNeill
Atmos. Chem. Phys., 16, 1603–1618, https://doi.org/10.5194/acp-16-1603-2016, https://doi.org/10.5194/acp-16-1603-2016, 2016
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Isoprene secondary organic aerosol (SOA) is a dominant aerosol component in the southeast US, but models routinely underestimate isoprene SOA with traditional schemes based on chamber studies operated under conditions not representative of isoprene-emitting forests. We develop a new irreversible uptake mechanism to reproduce isoprene SOA yields (3.3 %) and composition, and find a factor of 2 co-benefit of SO2 emission controls on reducing sulfate and organic aerosol in the southeast US.
H.-M. Lee, F. Paulot, D. K. Henze, K. Travis, D. J. Jacob, L. H. Pardo, and B. A. Schichtel
Atmos. Chem. Phys., 16, 525–540, https://doi.org/10.5194/acp-16-525-2016, https://doi.org/10.5194/acp-16-525-2016, 2016
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Sources of nitrogen deposition (Ndep) in Federal Class I areas in the US are investigated, identifying unique features in contributions from different species, sectors and locations. Ndep in many parks is impacted by emissions several hundred km away; the role of oxidized vs reduced sources varies regionally. Emissions reductions in the western US most effectively reduce the extent of areas in critical load exceedance, while reductions in the east most effectively reduce exceedance magnitudes.
J. He, Y. Zhang, S. Tilmes, L. Emmons, J.-F. Lamarque, T. Glotfelty, A. Hodzic, and F. Vitt
Geosci. Model Dev., 8, 3999–4025, https://doi.org/10.5194/gmd-8-3999-2015, https://doi.org/10.5194/gmd-8-3999-2015, 2015
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The global simulations with CB05_GE and MOZART-4x predict similar chemical profiles for major gases compared to aircraft measurements, with better agreement for the NOy profile by CB05_GE. The SOA concentrations of SOA at four sites in CONUS and organic carbon over the IMPROVE sites are better predicted by MOZART-4x. The two simulations result in a global average difference of 0.5W m-2 in simulated shortwave cloud radiative forcing, with up to 13.6W m-2 over subtropical regions.
Y. Zheng, N. Unger, A. Hodzic, L. Emmons, C. Knote, S. Tilmes, J.-F. Lamarque, and P. Yu
Atmos. Chem. Phys., 15, 13487–13506, https://doi.org/10.5194/acp-15-13487-2015, https://doi.org/10.5194/acp-15-13487-2015, 2015
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Nitrogen oxides (NOx) play an important but complex role in secondary organic aerosol (SOA) formation. In this study we update the SOA scheme in a global 3-D chemistry-climate model by implementing a 4-product volatility basis set (VBS) framework with NOx-dependent yields and simplified aging parameterizations. We find that the SOA decrease in response to a 50% reduction in anthropogenic NOx emissions is limited due to the buffering in different chemical pathways.
P. S. Kim, D. J. Jacob, J. A. Fisher, K. Travis, K. Yu, L. Zhu, R. M. Yantosca, M. P. Sulprizio, J. L. Jimenez, P. Campuzano-Jost, K. D. Froyd, J. Liao, J. W. Hair, M. A. Fenn, C. F. Butler, N. L. Wagner, T. D. Gordon, A. Welti, P. O. Wennberg, J. D. Crounse, J. M. St. Clair, A. P. Teng, D. B. Millet, J. P. Schwarz, M. Z. Markovic, and A. E. Perring
Atmos. Chem. Phys., 15, 10411–10433, https://doi.org/10.5194/acp-15-10411-2015, https://doi.org/10.5194/acp-15-10411-2015, 2015
J. Kaiser, G. M. Wolfe, K. E. Min, S. S. Brown, C. C. Miller, D. J. Jacob, J. A. deGouw, M. Graus, T. F. Hanisco, J. Holloway, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, R. A. Washenfelder, and F. N. Keutsch
Atmos. Chem. Phys., 15, 7571–7583, https://doi.org/10.5194/acp-15-7571-2015, https://doi.org/10.5194/acp-15-7571-2015, 2015
G. Zeng, J. E. Williams, J. A. Fisher, L. K. Emmons, N. B. Jones, O. Morgenstern, J. Robinson, D. Smale, C. Paton-Walsh, and D. W. T. Griffith
Atmos. Chem. Phys., 15, 7217–7245, https://doi.org/10.5194/acp-15-7217-2015, https://doi.org/10.5194/acp-15-7217-2015, 2015
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We assess the impact of biogenic emissions on CO and HCHO in the Southern Hemisphere (SH), with simulations using different emission inventories. Differences in biogenic emissions result in large differences on modelled CO in the source and the remote regions. Substantial inter-model differences exist. Models significantly underestimate observed HCHO columns in the SH, suggesting missing sources in the models. Differences in the CO/OH/CH4 chemistry lead to differences in HCHO in remote regions.
A. J. Turner and D. J. Jacob
Atmos. Chem. Phys., 15, 7039–7048, https://doi.org/10.5194/acp-15-7039-2015, https://doi.org/10.5194/acp-15-7039-2015, 2015
A. J. Turner, D. J. Jacob, K. J. Wecht, J. D. Maasakkers, E. Lundgren, A. E. Andrews, S. C. Biraud, H. Boesch, K. W. Bowman, N. M. Deutscher, M. K. Dubey, D. W. T. Griffith, F. Hase, A. Kuze, J. Notholt, H. Ohyama, R. Parker, V. H. Payne, R. Sussmann, C. Sweeney, V. A. Velazco, T. Warneke, P. O. Wennberg, and D. Wunch
Atmos. Chem. Phys., 15, 7049–7069, https://doi.org/10.5194/acp-15-7049-2015, https://doi.org/10.5194/acp-15-7049-2015, 2015
L. K. Emmons, S. R. Arnold, S. A. Monks, V. Huijnen, S. Tilmes, K. S. Law, J. L. Thomas, J.-C. Raut, I. Bouarar, S. Turquety, Y. Long, B. Duncan, S. Steenrod, S. Strode, J. Flemming, J. Mao, J. Langner, A. M. Thompson, D. Tarasick, E. C. Apel, D. R. Blake, R. C. Cohen, J. Dibb, G. S. Diskin, A. Fried, S. R. Hall, L. G. Huey, A. J. Weinheimer, A. Wisthaler, T. Mikoviny, J. Nowak, J. Peischl, J. M. Roberts, T. Ryerson, C. Warneke, and D. Helmig
Atmos. Chem. Phys., 15, 6721–6744, https://doi.org/10.5194/acp-15-6721-2015, https://doi.org/10.5194/acp-15-6721-2015, 2015
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Eleven 3-D tropospheric chemistry models have been compared and evaluated with observations in the Arctic during the International Polar Year (IPY 2008). Large differences are seen among the models, particularly related to the model chemistry of volatile organic compounds (VOCs) and reactive nitrogen (NOx, PAN, HNO3) partitioning. Consistency among the models in the underestimation of CO, ethane and propane indicates the emission inventory is too low for these compounds.
S. R. Arnold, L. K. Emmons, S. A. Monks, K. S. Law, D. A. Ridley, S. Turquety, S. Tilmes, J. L. Thomas, I. Bouarar, J. Flemming, V. Huijnen, J. Mao, B. N. Duncan, S. Steenrod, Y. Yoshida, J. Langner, and Y. Long
Atmos. Chem. Phys., 15, 6047–6068, https://doi.org/10.5194/acp-15-6047-2015, https://doi.org/10.5194/acp-15-6047-2015, 2015
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The extent to which forest fires produce the air pollutant and greenhouse gas ozone (O3) in the atmosphere at high latitudes in not well understood. We have compared how fire emissions produce O3 and its precursors in several models of atmospheric chemistry. We find enhancements in O3 in air dominated by fires in all models, which increase on average as fire emissions age. We also find that in situ O3 production in the Arctic is sensitive to details of organic chemistry and vertical lifting.
S. Tilmes, J.-F. Lamarque, L. K. Emmons, D. E. Kinnison, P.-L. Ma, X. Liu, S. Ghan, C. Bardeen, S. Arnold, M. Deeter, F. Vitt, T. Ryerson, J. W. Elkins, F. Moore, J. R. Spackman, and M. Val Martin
Geosci. Model Dev., 8, 1395–1426, https://doi.org/10.5194/gmd-8-1395-2015, https://doi.org/10.5194/gmd-8-1395-2015, 2015
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The Community Atmosphere Model (CAM), version 5, is now coupled to extensive tropospheric and stratospheric chemistry, called CAM5-chem, and is available in addition to CAM4-chem in the Community Earth System Model (CESM) version 1.2. Both configurations are well suited as tools for atmospheric chemistry modeling studies in the troposphere and lower stratosphere.
S. A. Monks, S. R. Arnold, L. K. Emmons, K. S. Law, S. Turquety, B. N. Duncan, J. Flemming, V. Huijnen, S. Tilmes, J. Langner, J. Mao, Y. Long, J. L. Thomas, S. D. Steenrod, J. C. Raut, C. Wilson, M. P. Chipperfield, G. S. Diskin, A. Weinheimer, H. Schlager, and G. Ancellet
Atmos. Chem. Phys., 15, 3575–3603, https://doi.org/10.5194/acp-15-3575-2015, https://doi.org/10.5194/acp-15-3575-2015, 2015
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Multi-model simulations of Arctic CO, O3 and OH are evaluated using observations. Models show highly variable concentrations but the relative importance of emission regions and types is robust across the models, demonstrating the importance of biomass burning as a source. Idealised tracer experiments suggest that some of the model spread is due to variations in simulated transport from Europe in winter and from Asia throughout the year.
J. A. Fisher, S. R. Wilson, G. Zeng, J. E. Williams, L. K. Emmons, R. L. Langenfelds, P. B. Krummel, and L. P. Steele
Atmos. Chem. Phys., 15, 3217–3239, https://doi.org/10.5194/acp-15-3217-2015, https://doi.org/10.5194/acp-15-3217-2015, 2015
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The Southern Hemisphere (SH) serves as an important test bed for evaluating our understanding of the processes that drive the composition of the clean background atmosphere. Using data from two aircraft campaigns, combined with four atmospheric chemistry models, we find a large sensitivity in the remote SH to biogenic emissions and their subsequent chemistry and transport. Future model evaluation and measurement campaigns should prioritize reducing uncertainties in these processes.
M. S. Long, R. Yantosca, J. E. Nielsen, C. A. Keller, A. da Silva, M. P. Sulprizio, S. Pawson, and D. J. Jacob
Geosci. Model Dev., 8, 595–602, https://doi.org/10.5194/gmd-8-595-2015, https://doi.org/10.5194/gmd-8-595-2015, 2015
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This paper presents results from the modularization of the GEOS-Chem chemical transport model, and its coupling as the chemical operator within the NASA-GMAO GEOS-5 Earth system model (ESM). The key findings are that chemistry within the modular GEOS-Chem system shows consistent, high strong-scaling properties across the range of distributed processors, transport is the limiting component prohibiting efficient scalability, and GEOS-Chem is able to generate suitable chemical results in an ESM.
M. Val Martin, C. L. Heald, J.-F. Lamarque, S. Tilmes, L. K. Emmons, and B. A. Schichtel
Atmos. Chem. Phys., 15, 2805–2823, https://doi.org/10.5194/acp-15-2805-2015, https://doi.org/10.5194/acp-15-2805-2015, 2015
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We present for the first time the relative effect of climate, emissions, and land use change on ozone and PM25 over the United States, focusing on the national parks. Air quality in 2050 will likely be dominated by emission patterns, but climate and land use changes alone can lead to a substantial increase in air pollution over most of the US, with important implications for O3 air quality, visibility and ecosystem health degradation in the national parks.
C. Viatte, K. Strong, J. Hannigan, E. Nussbaumer, L. K. Emmons, S. Conway, C. Paton-Walsh, J. Hartley, J. Benmergui, and J. Lin
Atmos. Chem. Phys., 15, 2227–2246, https://doi.org/10.5194/acp-15-2227-2015, https://doi.org/10.5194/acp-15-2227-2015, 2015
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Seven tropospheric species (CO, HCN, C2H6, C2H2, CH3OH, HCOOH, and H2CO) released by biomass burning events transported to the high Arctic were monitored with two sets of FTIR measurements, located at Eureka (Nunavut, Canada) and Thule (Greenland), from 2008 to 2012. We compared these data sets with the MOZART-4 chemical transport model to help improve its simulations in the Arctic. Emission factors of these biomass burning products were derived and compared to the literature.
T. Amnuaylojaroen, M. C. Barth, L. K. Emmons, G. R. Carmichael, J. Kreasuwun, S. Prasitwattanaseree, and S. Chantara
Atmos. Chem. Phys., 14, 12983–13012, https://doi.org/10.5194/acp-14-12983-2014, https://doi.org/10.5194/acp-14-12983-2014, 2014
F. L. Herron-Thorpe, G. H. Mount, L. K. Emmons, B. K. Lamb, D. A. Jaffe, N. L. Wigder, S. H. Chung, R. Zhang, M. D. Woelfle, and J. K. Vaughan
Atmos. Chem. Phys., 14, 12533–12551, https://doi.org/10.5194/acp-14-12533-2014, https://doi.org/10.5194/acp-14-12533-2014, 2014
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Wildfire season simulations from an air quality forecast system for the Pacific Northwest were compared to surface monitor observations across the region and NASA Earth Observing System satellite retrievals of plume top, nitrogen dioxide, aerosol optical depth, and carbon monoxide. This study discusses why the Community Multi-scale Air Quality model predictions under-predicted secondary organic aerosol (SOA) production for events when fire emissions were transported large distances.
C. Chan Miller, G. Gonzalez Abad, H. Wang, X. Liu, T. Kurosu, D. J. Jacob, and K. Chance
Atmos. Meas. Tech., 7, 3891–3907, https://doi.org/10.5194/amt-7-3891-2014, https://doi.org/10.5194/amt-7-3891-2014, 2014
M. N. Deeter, S. Martínez-Alonso, D. P. Edwards, L. K. Emmons, J. C. Gille, H. M. Worden, C. Sweeney, J. V. Pittman, B. C. Daube, and S. C. Wofsy
Atmos. Meas. Tech., 7, 3623–3632, https://doi.org/10.5194/amt-7-3623-2014, https://doi.org/10.5194/amt-7-3623-2014, 2014
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The MOPITT Version 6 product for carbon monoxide (CO) incorporates several enhancements. First, a geolocation bias has been eliminated. Second, the new variable a priori for CO concentrations is based on simulations performed with the CAM-Chem chemical transport model for the years 2000-2009. Third, required meteorological fields are extracted from the MERRA reanalysis. Finally, a retrieval bias in the upper troposphere was substantially reduced. Validation results are presented.
J. D. Fast, J. Allan, R. Bahreini, J. Craven, L. Emmons, R. Ferrare, P. L. Hayes, A. Hodzic, J. Holloway, C. Hostetler, J. L. Jimenez, H. Jonsson, S. Liu, Y. Liu, A. Metcalf, A. Middlebrook, J. Nowak, M. Pekour, A. Perring, L. Russell, A. Sedlacek, J. Seinfeld, A. Setyan, J. Shilling, M. Shrivastava, S. Springston, C. Song, R. Subramanian, J. W. Taylor, V. Vinoj, Q. Yang, R. A. Zaveri, and Q. Zhang
Atmos. Chem. Phys., 14, 10013–10060, https://doi.org/10.5194/acp-14-10013-2014, https://doi.org/10.5194/acp-14-10013-2014, 2014
K. J. Wecht, D. J. Jacob, M. P. Sulprizio, G. W. Santoni, S. C. Wofsy, R. Parker, H. Bösch, and J. Worden
Atmos. Chem. Phys., 14, 8173–8184, https://doi.org/10.5194/acp-14-8173-2014, https://doi.org/10.5194/acp-14-8173-2014, 2014
C. A. Keller, M. S. Long, R. M. Yantosca, A. M. Da Silva, S. Pawson, and D. J. Jacob
Geosci. Model Dev., 7, 1409–1417, https://doi.org/10.5194/gmd-7-1409-2014, https://doi.org/10.5194/gmd-7-1409-2014, 2014
P. Zoogman, D. J. Jacob, K. Chance, X. Liu, M. Lin, A. Fiore, and K. Travis
Atmos. Chem. Phys., 14, 6261–6271, https://doi.org/10.5194/acp-14-6261-2014, https://doi.org/10.5194/acp-14-6261-2014, 2014
M. Li, Q. Zhang, D. G. Streets, K. B. He, Y. F. Cheng, L. K. Emmons, H. Huo, S. C. Kang, Z. Lu, M. Shao, H. Su, X. Yu, and Y. Zhang
Atmos. Chem. Phys., 14, 5617–5638, https://doi.org/10.5194/acp-14-5617-2014, https://doi.org/10.5194/acp-14-5617-2014, 2014
L. Zhang, D. J. Jacob, X. Yue, N. V. Downey, D. A. Wood, and D. Blewitt
Atmos. Chem. Phys., 14, 5295–5309, https://doi.org/10.5194/acp-14-5295-2014, https://doi.org/10.5194/acp-14-5295-2014, 2014
E. V. Fischer, D. J. Jacob, R. M. Yantosca, M. P. Sulprizio, D. B. Millet, J. Mao, F. Paulot, H. B. Singh, A. Roiger, L. Ries, R.W. Talbot, K. Dzepina, and S. Pandey Deolal
Atmos. Chem. Phys., 14, 2679–2698, https://doi.org/10.5194/acp-14-2679-2014, https://doi.org/10.5194/acp-14-2679-2014, 2014
P. S. Kim, D. J. Jacob, X. Liu, J. X. Warner, K. Yang, K. Chance, V. Thouret, and P. Nedelec
Atmos. Chem. Phys., 13, 9321–9335, https://doi.org/10.5194/acp-13-9321-2013, https://doi.org/10.5194/acp-13-9321-2013, 2013
J. L. Thomas, J.-C. Raut, K. S. Law, L. Marelle, G. Ancellet, F. Ravetta, J. D. Fast, G. Pfister, L. K. Emmons, G. S. Diskin, A. Weinheimer, A. Roiger, and H. Schlager
Atmos. Chem. Phys., 13, 3825–3848, https://doi.org/10.5194/acp-13-3825-2013, https://doi.org/10.5194/acp-13-3825-2013, 2013
J. Mao, S. Fan, D. J. Jacob, and K. R. Travis
Atmos. Chem. Phys., 13, 509–519, https://doi.org/10.5194/acp-13-509-2013, https://doi.org/10.5194/acp-13-509-2013, 2013
L. K. Emmons, P. G. Hess, J.-F. Lamarque, and G. G. Pfister
Geosci. Model Dev., 5, 1531–1542, https://doi.org/10.5194/gmd-5-1531-2012, https://doi.org/10.5194/gmd-5-1531-2012, 2012
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Regional and sectoral contributions of NOx and reactive carbon emission sources to global trends in tropospheric ozone during the 2000–2018 period
Underappreciated contributions of biogenic volatile organic compounds from urban green spaces to ozone pollution
Chemistry–climate feedback of atmospheric methane in a methane-emission-flux-driven chemistry–climate model
Surface ozone trend variability across the United States and the impact of heat waves (1990–2023)
Sensitivity of climate effects of hydrogen to leakage size, location, and chemical background
Evaluating tropospheric nitrogen dioxide in UKCA using OMI satellite retrievals over south and east Asia
Technical note: A comparative study of chemistry schemes for volcanic sulfur dioxide in Lagrangian transport simulations – a case study of the 2019 Raikoke eruption
Revisiting the high tropospheric ozone over southern Africa: role of biomass burning and anthropogenic emissions
Monoterpene oxidation pathways initiated by acyl peroxy radical addition
Local and transboundary contributions to NOy loadings across East Asia using CMAQ-ISAM and a GEMS-informed emission inventory during the winter–spring transition
Estimating the variability in NOx emissions from Wuhan with TROPOMI NO2 data during 2018 to 2023
Enhanced understanding of atmospheric blocking modulation on ozone dynamics within a high-resolution Earth system model
Natural emissions of VOC and NOx over Africa constrained by TROPOMI HCHO and NO2 data using the MAGRITTEv1.1 model
Contributions of lightning to long-term trends and inter-annual variability in global atmospheric chemistry constrained by Schumann Resonance observations
Impacts of wildfire smoke aerosols on near-surface ozone photochemistry
Anthropogenic emission controls reduce summertime ozone–temperature sensitivity in the United States
Investigating the response of China's surface ozone concentration to the future changes of multiple factors
Assessing the relative impacts of satellite ozone and its precursor observations to improve global tropospheric ozone analysis using multiple chemical reanalysis systems
Evaluating present-day and future impacts of agricultural ammonia emissions on atmospheric chemistry and climate
Air-pollution-satellite-based CO2 emission inversion: system evaluation, sensitivity analysis, and future research direction
Insights into ozone pollution control in urban areas by decoupling meteorological factors based on machine learning
Quantification of regional net CO2 flux errors in the Orbiting Carbon Observatory-2 (OCO-2) v10 model intercomparison project (MIP) ensemble using airborne measurements
Reactive nitrogen in and around the northeastern and mid-Atlantic US: sources, sinks, and connections with ozone
Preindustrial-to-present-day changes in atmospheric carbon monoxide: agreement and gaps between ice archives and global model reconstructions
Investigating processes influencing simulation of local Arctic wintertime anthropogenic pollution in Fairbanks, Alaska, during ALPACA-2022
Urban ozone formation and sensitivities to volatile chemical products, cooking emissions, and NOx upwind of and within two Los Angeles Basin cities
Causes of growing middle-to-upper tropospheric ozone over the northwest Pacific region
Impact of introducing electric vehicles on ground-level O3 and PM2.5 in the Greater Tokyo Area: yearly trends and the importance of changes in the urban heat island effect
Modelling Arctic Lower Tropospheric Ozone: processes controlling seasonal variations
South Asia ammonia emission inversion through assimilating IASI observations
Constraining the budget of NOx and VOCs at a remote Tropical island using multi-platform observations and WRF-Chem model simulations
A CO2–Δ14CO2 inversion setup for estimating European fossil CO2 emissions
Maximum ozone concentrations in the southwestern US and Texas: implications of the growing predominance of the background contribution
Derivation of atmospheric reaction mechanisms for volatile organic compounds by the SAPRC mechanism generation system (MechGen)
Comparative ozone production sensitivity to NOx and VOCs in Quito, Ecuador and Santiago, Chile: implications for control strategies in times of climate action
Seasonal, regional, and vertical characteristics of high-carbon-monoxide plumes along with their associated ozone anomalies, as seen by IAGOS between 2002 and 2019
Tropospheric ozone trends and attributions over East and Southeast Asia in 1995–2019: An integrated assessment using statistical methods, machine learning models, and multiple chemical transport models
The potential of drone observations to improve air quality predictions by 4D-Var
Process analysis of elevated concentrations of organic acids at Whiteface Mountain, New York
Sensitivity of climate-chemistry model simulated atmospheric composition to lightning-produced NOx parameterizations based on lightning frequency
Ozone source attribution in polluted European areas during summer 2017 as simulated with MECO(n)
Characterization of reactive nitrogen in the global upper troposphere using recent and historical commercial and research aircraft campaigns and GEOS-Chem
Opinion: Challenges and needs of tropospheric chemical mechanism development
Decrease of the European NOx anthropogenic emissions between 2005 and 2019 as seen from the OMI and TROPOMI NO2 satellite observations
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
Aditya Nalam, Aura Lupaşcu, Tabish Ansari, and Tim Butler
Atmos. Chem. Phys., 25, 5287–5311, https://doi.org/10.5194/acp-25-5287-2025, https://doi.org/10.5194/acp-25-5287-2025, 2025
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Tropospheric O3 molecules are labeled with the identity of their precursor source to simulate contributions from various emission sources to the global tropospheric O3 burden (TOB) and its trends. With an equatorward shift, anthropogenic NOx emissions become significantly more efficient at producing O3 and play a major role in driving TOB trends, mainly due to larger convection at the tropics effectively lifting O3 and its precursors to the free troposphere, where O3 lifetime is longer.
Haofan Wang, Yuejin Li, Yiming Liu, Xiao Lu, Yang Zhang, Qi Fan, Chong Shen, Senchao Lai, Yan Zhou, Tao Zhang, and Dingli Yue
Atmos. Chem. Phys., 25, 5233–5250, https://doi.org/10.5194/acp-25-5233-2025, https://doi.org/10.5194/acp-25-5233-2025, 2025
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This study explores how urban green spaces (UGSs) in Guangzhou influence ozone levels. By using advanced models, we found that natural emissions from these areas can significantly affect air quality. Our results suggest that the design and planning of UGSs should not only consider aesthetics and social factors but also their environmental impacts on air quality.
Laura Stecher, Franziska Winterstein, Patrick Jöckel, Michael Ponater, Mariano Mertens, and Martin Dameris
Atmos. Chem. Phys., 25, 5133–5158, https://doi.org/10.5194/acp-25-5133-2025, https://doi.org/10.5194/acp-25-5133-2025, 2025
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Methane, the second most important anthropogenic greenhouse gas, is chemically decomposed in the atmosphere. The chemical sink of atmospheric methane is not constant but depends on the temperature and on the abundance of its reaction partners. In this study, we use a global chemistry–climate model to assess the feedback of atmospheric methane induced by changes in the chemical sink in a warming climate and its implications for the chemical composition and the surface air temperature change.
Kai-Lan Chang, Brian C. McDonald, Colin Harkins, and Owen R. Cooper
Atmos. Chem. Phys., 25, 5101–5132, https://doi.org/10.5194/acp-25-5101-2025, https://doi.org/10.5194/acp-25-5101-2025, 2025
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Exposure to high levels of ozone can be harmful to human health. This study shows consistent and robust evidence of decreasing ozone extremes across much of the United States over the period from 1990 to 2023, previously attributed to ozone precursor emission controls. Nevertheless, we also show that the increasing heat wave frequencies are likely to contribute to additional ozone exceedances, slowing the progress of decreasing the frequency of ozone exceedances.
Ragnhild Bieltvedt Skeie, Marit Sandstad, Srinath Krishnan, Gunnar Myhre, and Maria Sand
Atmos. Chem. Phys., 25, 4929–4942, https://doi.org/10.5194/acp-25-4929-2025, https://doi.org/10.5194/acp-25-4929-2025, 2025
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Hydrogen leakages can alter the amount of climate gases in the atmosphere and hence have a climate impact. In this study we investigate, using an atmospheric chemistry model, how this indirect climate effect differs with different amounts of leakages and with where the hydrogen leaks and if this effect changes in the future. The effect is largest for emissions far from areas where hydrogen is removed from the atmosphere by the soil, but these are not relevant locations for a future hydrogen economy.
Alok K. Pandey, David S. Stevenson, Alcide Zhao, Richard J. Pope, Ryan Hossaini, Krishan Kumar, and Martyn P. Chipperfield
Atmos. Chem. Phys., 25, 4785–4802, https://doi.org/10.5194/acp-25-4785-2025, https://doi.org/10.5194/acp-25-4785-2025, 2025
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Nitrogen dioxide is an air pollutant largely controlled by human activity that affects ozone, methane, and aerosols. Satellite instruments can quantify column NO2 and, by carefully matching the time and location of measurements, enable evaluation of model simulations. NO2 over south and east Asia is assessed, showing that the model captures not only many features of the measurements, but also important differences that suggest model deficiencies in representing several aspects of the atmospheric chemistry of NO2.
Mingzhao Liu, Lars Hoffmann, Jens-Uwe Grooß, Zhongyin Cai, Sabine Grießbach, and Yi Heng
Atmos. Chem. Phys., 25, 4403–4418, https://doi.org/10.5194/acp-25-4403-2025, https://doi.org/10.5194/acp-25-4403-2025, 2025
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We studied the transport and chemical decomposition of volcanic SO2, focusing on the 2019 Raikoke event. By comparing two different chemistry modeling schemes, we found that including complex chemical reactions leads to a more accurate prediction of how long SO2 stays in the atmosphere. This research helps improve our understanding of volcanic pollution and its impact on air quality and climate, providing better tools for scientists to track and predict the movement of these pollutants.
Yufen Wang, Ke Li, Xi Chen, Zhenjiang Yang, Minglong Tang, Pascoal M. D. Campos, Yang Yang, Xu Yue, and Hong Liao
Atmos. Chem. Phys., 25, 4455–4475, https://doi.org/10.5194/acp-25-4455-2025, https://doi.org/10.5194/acp-25-4455-2025, 2025
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The impacts of biomass burning and anthropogenic emissions on high tropospheric ozone levels are not well studied in southern Africa. We combined model simulations with recent observations at the surface and from space to quantify tropospheric ozone and its drivers in southern Africa. Our work focuses on the impact of emissions from different sources at different spatial scales, contributing to a comprehensive understanding of air pollution drivers and their uncertainties in southern Africa.
Dominika Pasik, Thomas Golin Almeida, Emelda Ahongshangbam, Siddharth Iyer, and Nanna Myllys
Atmos. Chem. Phys., 25, 4313–4331, https://doi.org/10.5194/acp-25-4313-2025, https://doi.org/10.5194/acp-25-4313-2025, 2025
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We used quantum chemistry methods to investigate the oxidation mechanisms of acyl peroxy radicals (APRs) with various monoterpenes. Our findings reveal unique oxidation pathways for different monoterpenes, leading to either chain-terminating products or highly reactive intermediates that can contribute to particle formation in the atmosphere. This research highlights APRs as potentially significant but underexplored atmospheric oxidants that may influence future approaches to modelling climate.
Jincheol Park, Yunsoo Choi, and Sagun Kayastha
Atmos. Chem. Phys., 25, 4291–4311, https://doi.org/10.5194/acp-25-4291-2025, https://doi.org/10.5194/acp-25-4291-2025, 2025
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We investigated NOx emission contributions to NOy loadings across five regions of East Asia during the 2022 winter–spring transition through chemical transport modeling informed by satellite data. As seasons progress, local contributions within each region to its NOy budget decreased from 32 %–43 % to 23 %–30 %, while transboundary contributions increased from 16 %–33 % to 27 %–37 %, driven by a shift in synoptic settings that allowed pollutants to spread more broadly across the regions.
Qianqian Zhang, K. Folkert Boersma, Chiel van der Laan, Alba Mols, Bin Zhao, Shengyue Li, and Yuepeng Pan
Atmos. Chem. Phys., 25, 3313–3326, https://doi.org/10.5194/acp-25-3313-2025, https://doi.org/10.5194/acp-25-3313-2025, 2025
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Accurate NOx emission estimates are required to better understand air pollution. This study investigates and demonstrates the ability of the superposition column model in combination with TROPOMI tropospheric NO2 column data to estimate city-scale NOx emissions and lifetimes and their variabilities. The results of this work nevertheless confirm the strength of the superposition column model in estimating urban NOx emissions with reasonable accuracy.
Wenbin Kou, Yang Gao, Dan Tong, Xiaojie Guo, Xiadong An, Wenyu Liu, Mengshi Cui, Xiuwen Guo, Shaoqing Zhang, Huiwang Gao, and Lixin Wu
Atmos. Chem. Phys., 25, 3029–3048, https://doi.org/10.5194/acp-25-3029-2025, https://doi.org/10.5194/acp-25-3029-2025, 2025
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Unlike traditional numerical studies, we apply a high-resolution Earth system model, improving simulations of surface ozone and large-scale circulations such as atmospheric blocking. Besides local heat waves, we quantify the impact of atmospheric blocking on downstream ozone concentrations, which is closely associated with the blocking position. We identify three major pathways of Rossby wave propagation, stressing the critical role of large-scale circulation in regional air quality.
Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther
Atmos. Chem. Phys., 25, 2863–2894, https://doi.org/10.5194/acp-25-2863-2025, https://doi.org/10.5194/acp-25-2863-2025, 2025
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Vegetation releases biogenic volatile organic compounds, while soils and lightning contribute to the natural emissions of nitrogen oxides into the atmosphere. These gases interact in complex ways. Using satellite data and models, we developed a new method to simultaneously optimize these natural emissions over Africa in 2019. Our approach resulted in an increase in natural emissions, supported by independent data indicating that current estimates are underestimated.
Xiaobo Wang, Yuzhong Zhang, Tamás Bozóki, Ruosi Liang, Xinchun Xie, Shutao Zhao, Rui Wang, Yujia Zhao, and Shuai Sun
EGUsphere, https://doi.org/10.5194/egusphere-2025-370, https://doi.org/10.5194/egusphere-2025-370, 2025
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Schumann Resonance observations are used to parameterize lightning NOx emissions for better capturing global lightning trend and variability. Updated simulations reveal insignificant trend but greater variability in lightning NOx emissions, impacting tropospheric NOx, O3 and OH. Lightning generally counteracts non-lightning factors, reducing the inter-annua variability of tropospheric O3 and OH. Variations of global lightning play important role in understanding the atmospheric methane budget.
Jiaqi Shen, Ronald C. Cohen, Glenn M. Wolfe, and Xiaomeng Jin
EGUsphere, https://doi.org/10.5194/egusphere-2025-706, https://doi.org/10.5194/egusphere-2025-706, 2025
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This study shows large chemical and radiative effects of smoke aerosols from fires on near-surface ozone production. Aerosol loading and NOx levels are identified as the primary factors influencing these effects. Furthermore, we show that the surface PM2.5 to NO2 column ratio can be used as an indicator for identifying aerosol-dominated regimes, facilitating the assessments of aerosol impacts on ozone formation through satellite observations.
Shuai Li, Haolin Wang, and Xiao Lu
Atmos. Chem. Phys., 25, 2725–2743, https://doi.org/10.5194/acp-25-2725-2025, https://doi.org/10.5194/acp-25-2725-2025, 2025
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Summertime ozone–temperature sensitivity has decreased by 50 % from 3.0 ppbv per K in 1990 to 1.5 ppb per K in 2021 in the US. GEOS-Chem simulations show that anthropogenic nitrogen oxide emission reduction is the dominant driver of ozone–temperature sensitivity decline by influencing both temperature direct and temperature indirect processes. Reduced ozone–temperature sensitivity has decreased ozone enhancement from low to high temperatures by an average of 6.8 ppbv across the US.
Jinya Yang, Yutong Wang, Lei Zhang, and Yu Zhao
Atmos. Chem. Phys., 25, 2649–2666, https://doi.org/10.5194/acp-25-2649-2025, https://doi.org/10.5194/acp-25-2649-2025, 2025
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We develop a modeling framework to predict future ozone concentrations (till the 2060s) in China following an IPCC scenario. We evaluate the contributions of climatic, anthropogenic, and biogenic factors by season and region. We find persistent emission controls will alter the nonlinear response of ozone to its precursors and dominate the declining ozone level. The outcomes highlight the importance of human actions, even with a climate penalty on air quality.
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.
Wanmin Gong, Stephen R. Beagley, Kenjiro Toyota, Henrik Skov, Jesper Heile Christensen, Alexandru Lupu, Diane Pendlebury, Junhua Zhang, Ulas Im, Yugo Kanaya, Alfonso Saiz-Lopez, Roberto Sommariva, Peter Effertz, John W. Halfacre, Nis Jepsen, Rigel Kivi, Theodore K. Koenig, Katrin Müller, Claus Nordstrøm, Irina Petropavlovskikh, Paul B. Shepson, William R. Simpson, Sverre Solberg, Ralf M. Staebler, David W. Tarasick, Roeland Van Malderen, and Mika Vestenius
EGUsphere, https://doi.org/10.5194/egusphere-2024-3750, https://doi.org/10.5194/egusphere-2024-3750, 2025
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This study showed that the springtime O3 depletion plays a critical role in driving the surface O3 seasonal cycle in Central Arctic. The O3 depletion events, while occurring most notably within the lowest few hundred metres above the Arctic Ocean, can induce a 5–7 % of loss in the pan-Arctic tropospheric O3 burden during springtime. The study also found an enhancement in O3 and NOy (mostly PAN) concentrations in the Arctic due to northern boreal wildfires, particularly at altitudes.
Ji Xia, Yi Zhou, Li Fang, Yingfei Qi, Dehao Li, Hong Liao, and Jianbing Jin
EGUsphere, https://doi.org/10.5194/egusphere-2024-3938, https://doi.org/10.5194/egusphere-2024-3938, 2025
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This study established an ammonia emission inventory in South Asia via assimilation-based inversion system. The posterior emissions, calculated by integrating the CEDS inventory and IASI satellite observations, showed significant improvement over the prior. Validation against various measurements all support our posterior emission. It offers valuable insights of ammonia emissions for policymakers and researchers aiming to develop air quality management and mitigation strategies there.
Catalina Poraicu, Jean-François Müller, Trissevgeni Stavrakou, Crist Amelynck, Bert W. D. Verreyken, Niels Schoon, Corinne Vigouroux, Nicolas Kumps, Jérôme Brioude, Pierre Tulet, and Camille Mouchel-Vallon
EGUsphere, https://doi.org/10.5194/egusphere-2024-3555, https://doi.org/10.5194/egusphere-2024-3555, 2025
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We investigated the sources and impacts of nitrogen oxides and organic compounds over a remote tropical island. High-resolution WRF-Chem simulations were evaluated using in situ, FTIR and satellite measurements. This work highlights gaps in current models, like missing sources of key organic compounds and inaccuracies in emission inventories, emphasizing the importance of improving chemical and dynamical processes in atmospheric modelling for budget estimates in tropical regions.
Carlos Gómez-Ortiz, Guillaume Monteil, Sourish Basu, and Marko Scholze
Atmos. Chem. Phys., 25, 397–424, https://doi.org/10.5194/acp-25-397-2025, https://doi.org/10.5194/acp-25-397-2025, 2025
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In this paper, we test new implementations of our inverse modeling tool to estimate the weekly and regional CO2 emissions from fossil fuels in Europe. We use synthetic atmospheric observations of CO2 and radiocarbon (14CO2) to trace emissions to their sources, while separating the natural and fossil CO2. Our tool accurately estimates fossil CO2 emissions in densely monitored regions like western/central Europe. This approach aids in developing strategies for reducing CO2 emissions.
David D. Parrish, Ian C. Faloona, and Richard G. Derwent
Atmos. Chem. Phys., 25, 263–289, https://doi.org/10.5194/acp-25-263-2025, https://doi.org/10.5194/acp-25-263-2025, 2025
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Observation-based estimates of contributions to maximum ozone (O3) concentrations show that background O3 can exceed the air quality standard of 70 ppb in the southwestern US, precluding standard attainment. Over the past 4 decades, US anthropogenic O3 has decreased by a factor of ~ 6.3, while wildfire contributions have increased, so that the background now dominates maximum concentrations, even in Los Angeles, and the occurrence of maximum O3 has shifted from the eastern to the western US.
William P. L. Carter, Jia Jiang, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 25, 199–242, https://doi.org/10.5194/acp-25-199-2025, https://doi.org/10.5194/acp-25-199-2025, 2025
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This paper describes the scientific basis for gas-phase atmospheric chemical mechanisms derived using the SAPRC mechanism generation system, MechGen. It can derive mechanisms for most organic compounds with C, H, O, or N atoms, including initial reactions of organics with OH, O3, NO3, and O3P or by photolysis, as well as the reactions of the various types of intermediates that are formed. The paper includes a description of areas of uncertainty where additional research and updates are needed.
María Cazorla, Melissa Trujillo, Rodrigo Seguel, and Laura Gallardo
EGUsphere, https://doi.org/10.5194/egusphere-2024-3720, https://doi.org/10.5194/egusphere-2024-3720, 2024
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The current climate emergency imposes the need to take actions in cities to curb ozone as a pollutant and a climate forcer. In this work we analyze how reducing the levels of ozone precursor would affect photochemical smog in Quito, Ecuador and Santiago, Chile. Results show that if environmental policy were implemented to reduce only nitrogen oxides, the production of ozone would increase substantially for which more integral solutions are needed.
Thibaut Lebourgeois, Bastien Sauvage, Pawel Wolff, Béatrice Josse, Virginie Marécal, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Jean-Marc Cousin, Philippe Nedelec, and Valérie Thouret
Atmos. Chem. Phys., 24, 13975–14004, https://doi.org/10.5194/acp-24-13975-2024, https://doi.org/10.5194/acp-24-13975-2024, 2024
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Our study examines intense-carbon-monoxide (CO) pollution events measured by commercial aircraft from the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. We combine these measurements with the SOFT-IO model to trace the origin of the observed CO. A comprehensive analysis of the geographical origin, source type, seasonal variation, and ozone levels of these pollution events is provided.
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.
Nana Wei, Eloise A. Marais, Gongda Lu, Robert G. Ryan, and Bastien Sauvage
EGUsphere, https://doi.org/10.5194/egusphere-2024-3388, https://doi.org/10.5194/egusphere-2024-3388, 2024
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This study uses reactive nitrogen observations from NASA DC-8 research aircraft and The In-service Aircraft for a Global Observing System (IAGOS) campaigns to characterise reactive nitrogen seasonality and composition in the global upper troposphere and to diagnose the greatest knowledge gaps from comparison to a state-of-science model GEOS-Chem that need to be resolved for climate, nitrogen cycle and air pollution assessments.
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.
Cited articles
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Amos, H. M., Jacob, D. J., Holmes, C. D., Fisher, J. A., Wang, Q., Yantosca, R. M., Corbitt, E. S., Galarneau, E., Rutter, A. P., Gustin, M. S., Steffen, A., Schauer, J. J., Graydon, J. A., Louis, V. L. St., Talbot, R. W., Edgerton, E. S., Zhang, Y., and Sunderland, E. M.: Gas-particle partitioning of atmospheric Hg(II) and its effect on global mercury deposition, Atmos. Chem. Phys., 12, 591–603, https://doi.org/10.5194/acp-12-591-2012, 2012.
Balkanski, Y. J., Jacob, D. J., Gardner, G. M., Graustein, W. C., and Turekian, K. K.: Transport and residence times of tropospheric aerosols inferred from a global three-dimensional simulation of Pb-210, J. Geophys. Res., 98, 20573–20586, https://doi.org/10.1029/93JD02456, 1993.
Bates, K. H. and Jacob, D. J.: A new model mechanism for atmospheric oxidation of isoprene: global effects on oxidants, nitrogen oxides, organic products, and secondary organic aerosol, Atmos. Chem. Phys., 19, 9613–9640, https://doi.org/10.5194/acp-19-9613-2019, 2019.
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Short summary
Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone, but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side by side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model...
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