Articles | Volume 23, issue 11
https://doi.org/10.5194/acp-23-6271-2023
© Author(s) 2023. 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-23-6271-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
07 Jun 2023
Research article |
| 07 Jun 2023
| 07 Jun 2023
Background nitrogen dioxide (NO2) over the United States and its implications for satellite observations and trends: effects of nitrate photolysis, aircraft, and open fires
John A. Paulson School of Engineering and Applied Sciences, Harvard
University, Cambridge, MA 02138, USA
Daniel J. Jacob
John A. Paulson School of Engineering and Applied Sciences, Harvard
University, Cambridge, MA 02138, USA
Viral Shah
John A. Paulson School of Engineering and Applied Sciences, Harvard
University, Cambridge, MA 02138, USA
now at: Global Modeling and Assimilation Office, NASA Goddard Space
Flight Center, Greenbelt, MD 20771, USA
now at: Science Systems and
Applications, Inc., Lanham, MD 20706, USA
Sebastian D. Eastham
Department of
Aeronautics and Astronautics, Laboratory for Aviation and the Environment, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
Joint Program on the Science and Policy of Global Change,
Massachusetts Institute of Technology, Cambridge, MA 02139, USA
Thibaud M. Fritz
Department of
Aeronautics and Astronautics, Laboratory for Aviation and the Environment, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
Loretta J. Mickley
John A. Paulson School of Engineering and Applied Sciences, Harvard
University, Cambridge, MA 02138, USA
Tianjia Liu
Department of Earth and Planetary Sciences, Harvard University,
Cambridge, MA 02138, USA
Yi Wang
Center for Global and Regional Environmental Research, Iowa
Technology Institute, The University of Iowa, Iowa City, IA 52242, USA
Department of Chemical and Biochemical Engineering, The University of
Iowa, Iowa City, IA 52242, USA
Center for Global and Regional Environmental Research, Iowa
Technology Institute, The University of Iowa, Iowa City, IA 52242, USA
Department of Chemical and Biochemical Engineering, The University of
Iowa, Iowa City, IA 52242, USA
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Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
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.
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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.
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Atmos. Chem. Phys., 23, 9669–9683, https://doi.org/10.5194/acp-23-9669-2023, https://doi.org/10.5194/acp-23-9669-2023, 2023
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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.
Kelvin Bates, Mathew Evans, Barron Henderson, and Daniel Jacob
EGUsphere, https://doi.org/10.5194/egusphere-2023-1374, https://doi.org/10.5194/egusphere-2023-1374, 2023
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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.
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.
Amy Christiansen, Loretta J. Mickley, and Lu Hu
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In this work, we provide an additional constraint on emissions and trends of nitrogen oxides using nitrate wet deposition (NWD) fluxes over the United States and Europe from 1980–2020. We find that NWD measurements constrain total NOx emissions well. We also find evidence of NOx emissions overestimates in both domains, but especially over Europe, where NOx emissions are overestimated by a factor of 2. Reducing NOx emissions over Europe improves model representation of ozone at the surface.
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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Sebastian D. Eastham, Guillaume P. Chossière, Raymond L. Speth, Daniel J. Jacob, and Steven R. H. Barrett
EGUsphere, https://doi.org/10.5194/egusphere-2023-695, https://doi.org/10.5194/egusphere-2023-695, 2023
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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
EGUsphere, https://doi.org/10.5194/egusphere-2023-946, https://doi.org/10.5194/egusphere-2023-946, 2023
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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.
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.
Jing Wei, Zhanqing Li, Jun Wang, Can Li, Pawan Gupta, and Maureen Cribb
Atmos. Chem. Phys., 23, 1511–1532, https://doi.org/10.5194/acp-23-1511-2023, https://doi.org/10.5194/acp-23-1511-2023, 2023
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This study estimated the daily seamless 10 km ambient gaseous pollutants (NO2, SO2, and CO) across China using machine learning with extensive input variables measured on monitors, satellites, and models. Our dataset yields a high data quality via cross-validation at varying spatiotemporal scales and outperforms most previous related studies, making it most helpful to future (especially short-term) air pollution and environmental health-related studies.
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.
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.
Amy Christiansen, Loretta J. Mickley, Junhua Liu, Luke D. Oman, and Lu Hu
Atmos. Chem. Phys., 22, 14751–14782, https://doi.org/10.5194/acp-22-14751-2022, https://doi.org/10.5194/acp-22-14751-2022, 2022
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Understanding tropospheric ozone trends is crucial for accurate predictions of future air quality and climate, but drivers of trends are not well understood. We analyze global tropospheric ozone trends since 1980 using ozonesonde and surface measurements, and we evaluate two models for their ability to reproduce trends. We find observational evidence of increasing tropospheric ozone, but models underestimate these increases. This hinders our ability to estimate ozone radiative forcing.
Gonzalo A. Ferrada, Meng Zhou, Jun Wang, Alexei Lyapustin, Yujie Wang, Saulo R. Freitas, and Gregory R. Carmichael
Geosci. Model Dev., 15, 8085–8109, https://doi.org/10.5194/gmd-15-8085-2022, https://doi.org/10.5194/gmd-15-8085-2022, 2022
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The smoke from fires is composed of different compounds that interact with the atmosphere and can create poor air-quality episodes. Here, we present a new fire inventory based on satellite observations from the Visible Infrared Imaging Radiometer Suite (VIIRS). We named this inventory the VIIRS-based Fire Emission Inventory (VFEI). Advantages of VFEI are its high resolution (~500 m) and that it provides information for many species. VFEI is publicly available and has provided data since 2012.
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.
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.
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.
Lee T. Murray, Eric M. Leibensperger, Clara Orbe, Loretta J. Mickley, and Melissa Sulprizio
Geosci. Model Dev., 14, 5789–5823, https://doi.org/10.5194/gmd-14-5789-2021, https://doi.org/10.5194/gmd-14-5789-2021, 2021
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Chemical-transport models are tools used to study air pollution and inform public policy. However, they are limited by the availability of archived meteorology. Here, we describe how the GEOS-Chem chemical-transport model may now be driven by meteorology archived from a state-of-the-art general circulation model for past and future climates, allowing it to be used to explore the impact of climate change on air pollution and atmospheric composition.
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 %.
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.
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.
Jing Wei, Zhanqing Li, Rachel T. Pinker, Jun Wang, Lin Sun, Wenhao Xue, Runze Li, and Maureen Cribb
Atmos. Chem. Phys., 21, 7863–7880, https://doi.org/10.5194/acp-21-7863-2021, https://doi.org/10.5194/acp-21-7863-2021, 2021
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This study developed a space-time Light Gradient Boosting Machine (STLG) model to derive the high-temporal-resolution (1 h) and high-quality PM2.5 dataset in China (i.e., ChinaHighPM2.5) at a 5 km spatial resolution from the Himawari-8 Advanced Himawari Imager aerosol products. Our model outperforms most previous related studies with a much lower computation burden in terms of speed and memory, making it most suitable for real-time air pollution monitoring in China.
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.
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.
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.
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.
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.
Yang Li, Loretta J. Mickley, and Jed O. Kaplan
Atmos. Chem. Phys., 21, 57–68, https://doi.org/10.5194/acp-21-57-2021, https://doi.org/10.5194/acp-21-57-2021, 2021
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Climate models predict a shift toward warmer, drier environments in southwestern North America. Under future climate, the two main drivers of dust trends play opposing roles: (1) CO2 fertilization enhances vegetation and, in turn, decreases dust, and (2) increasing land use enhances dust emissions from northern Mexico. In the worst-case scenario, elevated dust concentrations spread widely over the domain by 2100 in spring, suggesting a large climate penalty on air quality and human health.
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.
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.
Tong Sha, Xiaoyan Ma, Jun Wang, Rong Tian, Jianqi Zhao, Fang Cao, and Yan-Lin Zhang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-760, https://doi.org/10.5194/acp-2020-760, 2020
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Most numerical models perform poorly on simulating the inorganic chemical components in PM2.5 (sulfate, nitrate, and ammonium (SNA)), generally underestimate sulfate but overestimate nitrate concentrations in haze events. Our work aims at investigating the role of cloud water in simulating SNA. We find that the uncertainties of cloud water can lead to model bias in simulating SNA, and can be reduced by constraining the modeled cloud water with MODIS satellite observations.
Yang Li, Loretta J. Mickley, Pengfei Liu, and Jed O. Kaplan
Atmos. Chem. Phys., 20, 8827–8838, https://doi.org/10.5194/acp-20-8827-2020, https://doi.org/10.5194/acp-20-8827-2020, 2020
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Using a coupled vegetation–fire–climate modeling framework, we show a northward shift in forests and increased lightning fire activity in northern US states, including Idaho, Montana, and Wyoming. Our findings suggest a large climate penalty on ecosystem, air quality, visibility, and human health in a region valued for its national forests and parks. The fine-scale smoke PM predictions provided in this study should prove useful to human health and environmental assessments.
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.
Yi Wang, Jun Wang, Xiaoguang Xu, Daven K. Henze, Zhen Qu, and Kai Yang
Atmos. Chem. Phys., 20, 6631–6650, https://doi.org/10.5194/acp-20-6631-2020, https://doi.org/10.5194/acp-20-6631-2020, 2020
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The use of OMPS satellite observations to inverse-model SO2 and NO2 emissions is presented through the GEOS-Chem adjoint modeling framework. The work is illustrated over China. The robustness of the results is studied through separate and joint inversions of SO2 and NO2 and the consideration of NH3 uncertainty. Independent validation is performed with OMI SO2 and NO2 data. It is shown that simultaneous inversion of NO2 and SO2 from OMPS provides an effective way to rapidly update emissions.
Yi Wang, Jun Wang, Meng Zhou, Daven K. Henze, Cui Ge, and Wei Wang
Atmos. Chem. Phys., 20, 6651–6670, https://doi.org/10.5194/acp-20-6651-2020, https://doi.org/10.5194/acp-20-6651-2020, 2020
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We developed four different methods to downscale SO2 and NO2 emissions derived from OMPS satellite observations (in Part 1) for regional air quality modeling at a spatial resolution that is finer than satellite observations. The VIIRS (city lights), TROPOMI, and OMI satellite data as well as surface data are used to evaluate the model. The method of using the top-down emissions from the past month for the air quality forecast in the present month is also shown to have practical merit.
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.
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.
Tongwen Wu, Fang Zhang, Jie Zhang, Weihua Jie, Yanwu Zhang, Fanghua Wu, Laurent Li, Jinghui Yan, Xiaohong Liu, Xiao Lu, Haiyue Tan, Lin Zhang, Jun Wang, and Aixue Hu
Geosci. Model Dev., 13, 977–1005, https://doi.org/10.5194/gmd-13-977-2020, https://doi.org/10.5194/gmd-13-977-2020, 2020
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This paper describes the first version of the Beijing Climate Center (BCC) fully coupled Earth System Model with interactive atmospheric chemistry and aerosols (BCC-ESM1). It is one of the models at the BCC for the Coupled Model Intercomparison Project Phase 6 (CMIP6). The CMIP6 Aerosol Chemistry Model Intercomparison Project (AerChemMIP) experiment using BCC-ESM1 has been finished. The evaluations show an overall good agreement between BCC-ESM1 simulations and observations in the 20th century.
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.
Xiaohua Pan, Charles Ichoku, Mian Chin, Huisheng Bian, Anton Darmenov, Peter Colarco, Luke Ellison, Tom Kucsera, Arlindo da Silva, Jun Wang, Tomohiro Oda, and Ge Cui
Atmos. Chem. Phys., 20, 969–994, https://doi.org/10.5194/acp-20-969-2020, https://doi.org/10.5194/acp-20-969-2020, 2020
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The differences between these six BB emission datasets are large. Our study found that (1) most current biomass burning (BB) aerosol emission datasets derived from satellite observations lead to the underestimation of aerosol optical depth (AOD) in this model in the biomass-burning-dominated regions and (2) it is important to accurately estimate both the magnitudes and spatial patterns of regional BB emissions in order for a model using these emissions to reproduce observed AOD levels.
Jun Zhu, Xiangao Xia, Huizheng Che, Jun Wang, Zhiyuan Cong, Tianliang Zhao, Shichang Kang, Xuelei Zhang, Xingna Yu, and Yanlin Zhang
Atmos. Chem. Phys., 19, 14637–14656, https://doi.org/10.5194/acp-19-14637-2019, https://doi.org/10.5194/acp-19-14637-2019, 2019
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The long-term temporal–spatial variations of the aerosol optical properties over the Tibetan Plateau (TP) based on the multiple ground-based sun photometer sites and the MODIS product are presented. Besides, the aerosol pollution and aerosol transport processes over the TP are also analyzed by the observations and models. The results in this region could help reduce the assessment uncertainties of aerosol radiative forcing and provide more information on aerosol transportation.
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.
Steven D. Miller, Louie D. Grasso, Qijing Bian, Sonia M. Kreidenweis, Jack F. Dostalek, Jeremy E. Solbrig, Jennifer Bukowski, Susan C. van den Heever, Yi Wang, Xiaoguang Xu, Jun Wang, Annette L. Walker, Ting-Chi Wu, Milija Zupanski, Christine Chiu, and Jeffrey S. Reid
Atmos. Meas. Tech., 12, 5101–5118, https://doi.org/10.5194/amt-12-5101-2019, https://doi.org/10.5194/amt-12-5101-2019, 2019
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Satellite–based detection of lofted mineral via infrared–window channels, well established in the literature, faces significant challenges in the presence of atmospheric moisture. Here, we consider a case featuring the juxtaposition of two dust plumes embedded within dry and moist air masses. The case is considered from the vantage points of numerical modeling, multi–sensor observations, and radiative transfer theory arriving at a new method for mitigating the water vapor masking effect.
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.
Stephen M. Saleeby, Susan C. van den Heever, Jennie Bukowski, Annette L. Walker, Jeremy E. Solbrig, Samuel A. Atwood, Qijing Bian, Sonia M. Kreidenweis, Yi Wang, Jun Wang, and Steven D. Miller
Atmos. Chem. Phys., 19, 10279–10301, https://doi.org/10.5194/acp-19-10279-2019, https://doi.org/10.5194/acp-19-10279-2019, 2019
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This study seeks to understand how intense dust storms impact the heating and cooling of the land surface and atmosphere. Dust storms that are intense enough to substantially impact visibility can also alter how much sunlight reaches the surface during the day and how much heat is trapped in the atmosphere at night. These radiation changes can impact the temperature of the atmosphere and impact the weather in the vicinity.
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.
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.
Jiarui Wu, Naifang Bei, Bo Hu, Suixin Liu, Meng Zhou, Qiyuan Wang, Xia Li, Lang Liu, Tian Feng, Zirui Liu, Yichen Wang, Junji Cao, Xuexi Tie, Jun Wang, Luisa T. Molina, and Guohui Li
Atmos. Chem. Phys., 19, 8703–8719, https://doi.org/10.5194/acp-19-8703-2019, https://doi.org/10.5194/acp-19-8703-2019, 2019
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In the present study, simulations during a persistent and heavy haze pollution episode from 5 December 2015 to 4 January 2016 in the North China Plain (NCP) were performed using the WRF-Chem model to comprehensively quantify contributions of the aerosol shortwave radiative feedback (ARF) to near-surface PM2.5 mass concentrations. During the episode, the ARF deteriorates the haze pollution, increasing the near-surface PM2.5 concentration in the NCP by 10.2 μg m−3 (7.8 %) on average.
Jiarui Wu, Naifang Bei, Bo Hu, Suixin Liu, Meng Zhou, Qiyuan Wang, Xia Li, Lang Liu, Tian Feng, Zirui Liu, Yichen Wang, Junji Cao, Xuexi Tie, Jun Wang, Luisa T. Molina, and Guohui Li
Atmos. Chem. Phys., 19, 8721–8739, https://doi.org/10.5194/acp-19-8721-2019, https://doi.org/10.5194/acp-19-8721-2019, 2019
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The near-surface PM2.5 contribution of the ALW total effect is 17.5 % in NCP, indicating that ALW plays an important role in the PM2.5 formation during the wintertime haze pollution. Moreover, the ALW-HET overwhelmingly dominates the PM2.5 enhancement due to the ALW. The ALW does not consistently enhance near-surface [PM2.5] with increasing RH. When the RH exceeds 80 %, the contribution of the ALW begins to decrease, which is caused by the high occurrence frequencies of precipitation.
Xiaoguang Xu, Jun Wang, Yi Wang, Jing Zeng, Omar Torres, Jeffrey S. Reid, Steven D. Miller, J. Vanderlei Martins, and Lorraine A. Remer
Atmos. Meas. Tech., 12, 3269–3288, https://doi.org/10.5194/amt-12-3269-2019, https://doi.org/10.5194/amt-12-3269-2019, 2019
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Detecting aerosol layer height from space is challenging. The traditional method relies on active sensors such as lidar that provide the detailed vertical structure of the aerosol profile but is costly with limited spatial coverage (more than 1 year is needed for global coverage). Here we developed a passive remote sensing technique that uses backscattered sunlight to retrieve smoke aerosol layer height over both water and vegetated surfaces from a sensor 1.5 million kilometers from the Earth.
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.
Huanxin Zhang, Jun Wang, Lorena Castro García, Jing Zeng, Connor Dennhardt, Yang Liu, and Nickolay A. Krotkov
Atmos. Chem. Phys., 19, 2165–2181, https://doi.org/10.5194/acp-19-2165-2019, https://doi.org/10.5194/acp-19-2165-2019, 2019
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OMU-based surface erythemal UV irradiance is compared with ground observations in the United States from 2005 to 2017. We reveal that the assumption of constant atmospheric conditions between OMI overpass time and local solar noon time may not fully represent the real atmosphere and the peaks of surface UV are not always at local solar noon because of cloud effects. Future geostationary satellites (e.g., TEMPO) would reduce sampling bias and improve trend analysis of surface UV estimate.
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).
Milija Zupanski, Anton Kliewer, Ting-Chi Wu, Karina Apodaca, Qijing Bian, Sam Atwood, Yi Wang, Jun Wang, and Steven D. Miller
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-2, https://doi.org/10.5194/acp-2019-2, 2019
Revised manuscript not accepted
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The problem of under-observed aerosol observations and in particular the vertical distribution of aerosols is addressed using a strongly coupled atmosphere-aerosol data assimilation system. In the strongly coupled system the atmospheric observations, which are more numerous in general, can impact the aerosol initial conditions. In an application over a coastal zone, results indicate that atmospheric observations have a positive impact on aerosols.
Ting-Chi Wu, Milija Zupanski, Stephen Saleeby, Anton Kliewer, Lewis Grasso, Qijing Bian, Samuel A. Atwood, Yi Wang, and Jun Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1249, https://doi.org/10.5194/acp-2018-1249, 2018
Revised manuscript not accepted
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.
Anton Kliewer, Milija Zupanski, Qijing Bian, Sam Atwood, Yi Wang, and Jun Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1156, https://doi.org/10.5194/acp-2018-1156, 2018
Revised manuscript not accepted
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This research is focused on improving numerical weather prediction by including data regarding aerosols in the atmosphere. Using weather prediction models along with data assimilation (the process of marrying observations with a model prediction), a better representation of the atmosphere can be described. As no model or observational platform is ever perfect, the aerosol observations have to be de-biased (adjusting for systematic error). Here we look at two such methods.
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.
Elizabeth M. Lennartson, Jun Wang, Juping Gu, Lorena Castro Garcia, Cui Ge, Meng Gao, Myungje Choi, Pablo E. Saide, Gregory R. Carmichael, Jhoon Kim, and Scott J. Janz
Atmos. Chem. Phys., 18, 15125–15144, https://doi.org/10.5194/acp-18-15125-2018, https://doi.org/10.5194/acp-18-15125-2018, 2018
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This paper is among the first to study the diurnal variations of AOD, PM2.5, and their relationships in South Korea. We show that the PM2.5–AOD relationship has strong diurnal variations, and, hence, using AOD data retrieved from geostationary satellite can improve the monitoring of surface PM2.5 air quality on a daily basis as well as constrain the diurnal variation of aerosol emission.
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.
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.
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.
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.
Nan Li, Qingyang He, Jim Greenberg, Alex Guenther, Jingyi Li, Junji Cao, Jun Wang, Hong Liao, Qiyuan Wang, and Qiang Zhang
Atmos. Chem. Phys., 18, 7489–7507, https://doi.org/10.5194/acp-18-7489-2018, https://doi.org/10.5194/acp-18-7489-2018, 2018
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O3 pollution has been increasing in most Chinese cities in recent years. Our study reveals that the synergistic impact of individual source contributions to O3 formation should be considered in the formation of air pollution control strategies, especially for big cities in the vicinity of forests.
Danny M. Leung, Amos P. K. Tai, Loretta J. Mickley, Jonathan M. Moch, Aaron van Donkelaar, Lu Shen, and Randall V. Martin
Atmos. Chem. Phys., 18, 6733–6748, https://doi.org/10.5194/acp-18-6733-2018, https://doi.org/10.5194/acp-18-6733-2018, 2018
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This paper investigates how large-scale weather systems control fine particulate matter (PM2.5) air quality in China. We show that winter monsoons, onshore winds and frontal rains can drive daily PM2.5 variability in different regions of China. We further project future PM2.5 concentration change by 2050s due to climate change, and verify that climate change has little benefit on future PM2.5 in Beijing, implying cutting down emissions is necessary to mitigate pollutions in megacities of China.
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.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
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.
Daniel H. Cusworth, Loretta J. Mickley, Eric M. Leibensperger, and Michael J. Iacono
Atmos. Chem. Phys., 17, 13559–13572, https://doi.org/10.5194/acp-17-13559-2017, https://doi.org/10.5194/acp-17-13559-2017, 2017
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Since 1990, light-scattering pollution known as aerosols have declined as a result of tightening US air quality regulations. Our study finds that US surface solar radiation has increased simultaneously. We establish a link between aerosols and radiation through physical and statistical models. We find the strongest relationship between aerosols, radiation, and climate at a site in the Midwest. Our work underscores the importance of regional pollution on climate in the US and abroad.
Yuxuan Wang, Yuanyu Xie, Wenhao Dong, Yi Ming, Jun Wang, and Lu Shen
Atmos. Chem. Phys., 17, 12827–12843, https://doi.org/10.5194/acp-17-12827-2017, https://doi.org/10.5194/acp-17-12827-2017, 2017
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Besides the well-known large impact on agriculture and water resources, drought is associated with significant adverse effects on air quality. Drought-induced degradation of air quality is largely due to natural processes, offsetting the effort of anthropogenic emission reduction during the past decades. Such adverse impacts should be included in modeling processes under current and future climate for mitigation policy.
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
Preprint retracted
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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.
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.
Lu Shen, Loretta J. Mickley, and Lee T. Murray
Atmos. Chem. Phys., 17, 4355–4367, https://doi.org/10.5194/acp-17-4355-2017, https://doi.org/10.5194/acp-17-4355-2017, 2017
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We introduce a new method to characterize the influence of atmospheric circulation on surface PM2.5 concentrations. Applying our statistical model to climate projections, we find a strong influence of 2000–2050 climate change on PM2.5 air quality in the United States. We find that current atmospheric chemistry models may underestimate the strong positive sensitivity of PM2.5 to temperature in the eastern United States in summer, and so may underestimate PM2.5 changes in a warmer climate.
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.
Tomás Sherwen, Mat J. Evans, Lucy J. Carpenter, Johan A. Schmidt, and Loretta J. Mickley
Atmos. Chem. Phys., 17, 1557–1569, https://doi.org/10.5194/acp-17-1557-2017, https://doi.org/10.5194/acp-17-1557-2017, 2017
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We model pre-industrial to present day changes using the GEOS-Chem global chemical transport model with halogens (Cl, Br, I). The model better captures pre-industrial O3 observations with halogens included. Halogens buffer the tropospheric forcing of O3 (RFTO3) from pre-industrial to present day, reducing RFTO3 by 0.087 Wm−2. This reduction is greater than that from halogens on stratospheric O3 (−0.05 Wm−2). This suggests that models that do not include halogens will overestimate RFTO3by ~ 25%.
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.
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.
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.
Shouguo Ding, Jun Wang, and Xiaoguang Xu
Atmos. Meas. Tech., 9, 2077–2092, https://doi.org/10.5194/amt-9-2077-2016, https://doi.org/10.5194/amt-9-2077-2016, 2016
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Knowledge on the vertical distribution of aerosols in the atmospheric is important for studying aerosol impacts on air quality and climate change. The polarization measurements in O2 A and B bands is shown here theoretically to have rich information for characterizing aerosol vertical profile over land. This paper presents a passive remote sensing technique supplementary to the existing technique to retrieve aerosol vertical distribution over land from space.
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.
L. Shen, L. J. Mickley, and A. P. K. Tai
Atmos. Chem. Phys., 15, 10925–10938, https://doi.org/10.5194/acp-15-10925-2015, https://doi.org/10.5194/acp-15-10925-2015, 2015
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In this study, we have examined the effect of polar jet and Bermuda High on ozone air quality in the eastern United States. In the Midwest and northeast, the poleward shift of jet wind leads to reduced polar jet frequency, resulting in increased ozone there. In the southeast, the influence of Bermuda High on ozone variability depends on the location of its west edge. Westward movement increases the ozone only when the JJA Bermuda High west edge is located west of 85.4°W.
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
X. Yue, L. J. Mickley, J. A. Logan, R. C. Hudman, M. V. Martin, and R. M. Yantosca
Atmos. Chem. Phys., 15, 10033–10055, https://doi.org/10.5194/acp-15-10033-2015, https://doi.org/10.5194/acp-15-10033-2015, 2015
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Based on simulated meteorology from 13 GCMs, we projected future wildfire activity in Alaskan and Canadian ecoregions by the mid-century. The most robust change is the increase of 150-390% in area burned over Alaska and western Canada. The models also predict an increase of 45-90% in the central and southern Canadian ecoregions, but a decrease of up to 50% in northern Canada. We further quantify how the changes in wildfire emissions may affect ozone concentrations in North America.
P. Achakulwisut, L. J. Mickley, L. T. Murray, A. P. K. Tai, J. O. Kaplan, and B. Alexander
Atmos. Chem. Phys., 15, 7977–7998, https://doi.org/10.5194/acp-15-7977-2015, https://doi.org/10.5194/acp-15-7977-2015, 2015
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The atmosphere’s oxidative capacity determines the lifetime of many trace gases important to climate, chemistry, and human health. Yet uncertainties remain about its past variations, its controlling factors, and the radiative forcing of short-lived species it influences. To reduce these uncertainties, we must better quantify the natural emissions and chemical reaction mechanisms of organic compounds in the atmosphere, which play a role in governing the oxidative capacity.
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
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
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.
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
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
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
L. T. Murray, L. J. Mickley, J. O. Kaplan, E. D. Sofen, M. Pfeiffer, and B. Alexander
Atmos. Chem. Phys., 14, 3589–3622, https://doi.org/10.5194/acp-14-3589-2014, https://doi.org/10.5194/acp-14-3589-2014, 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
C. Ge, J. Wang, and J. S. Reid
Atmos. Chem. Phys., 14, 159–174, https://doi.org/10.5194/acp-14-159-2014, https://doi.org/10.5194/acp-14-159-2014, 2014
B. S. Meland, X. Xu, D. K. Henze, and J. Wang
Atmos. Meas. Tech., 6, 3441–3457, https://doi.org/10.5194/amt-6-3441-2013, https://doi.org/10.5194/amt-6-3441-2013, 2013
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
H. Jiang, H. Liao, H. O. T. Pye, S. Wu, L. J. Mickley, J. H. Seinfeld, and X. Y. Zhang
Atmos. Chem. Phys., 13, 7937–7960, https://doi.org/10.5194/acp-13-7937-2013, https://doi.org/10.5194/acp-13-7937-2013, 2013
J. Wang, S. Park, J. Zeng, C. Ge, K. Yang, S. Carn, N. Krotkov, and A. H. Omar
Atmos. Chem. Phys., 13, 1895–1912, https://doi.org/10.5194/acp-13-1895-2013, https://doi.org/10.5194/acp-13-1895-2013, 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
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Insights into soil NO emissions and the contribution to surface ozone formation in China
Development, intercomparison, and evaluation of an improved mechanism for the oxidation of dimethyl sulfide in the UKCA model
The atmospheric oxidizing capacity in China – Part 1: Roles of different photochemical processes
Benefits of net-zero policies for future ozone pollution in China
Simulating impacts on UK air quality from net-zero forest planting scenarios
Understanding offshore high-ozone events during TRACER-AQ 2021 in Houston: insights from WRF–CAMx photochemical modeling
Opinion: Establishing a science-into-policy process for tropospheric ozone assessment
Atmospheric composition and climate impacts of a future hydrogen economy
Assessment of isoprene and near-surface ozone sensitivities to water stress over the Euro-Mediterranean region
Nighttime ozone in the lower boundary layer: insights from 3-year tower-based measurements in South China and regional air quality modeling
What controls ozone sensitivity in the upper tropical troposphere?
Modelling the impacts of emission changes on O3 sensitivity, atmospheric oxidation capacity, and pollution transport over the Catalonia region
A regional modelling study of halogen chemistry within a volcanic plume of Mt Etna's Christmas 2018 eruption
Weekly-derived top-down VOC fluxes over Europe from TROPOMI HCHO data in 2018–2021
Constraining the budget of atmospheric carbonyl sulfide using a 3-D chemical transport model
Atmospheric CO2 inversion reveals the Amazon as a minor carbon source caused by fire emissions, with forest uptake offsetting about half of these emissions
Rapid O3 assimilations – Part 2: Tropospheric O3 changes accompanied by declining NOx emissions in the USA and Europe in 2005–2020
High-resolution air quality simulations of ozone exceedance events during the Lake Michigan Ozone Study
Estimation of the atmospheric hydroxyl radical oxidative capacity using multiple hydrofluorocarbons (HFCs)
Simulations of winter ozone in the Upper Green River basin, Wyoming, using WRF-Chem
The suitability of atmospheric oxygen measurements to constrain Western European fossil-fuel CO2 emissions and their trends
Measurement report: Assessment of Asian emissions of ethane and propane with a chemistry transport model based on observations from the island of Hateruma
Sensitivity of northeastern US surface ozone predictions to the representation of atmospheric chemistry in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMMv1.0)
Zonal variability of methane trends derived from satellite data
Current status of model predictions on volatile organic compounds and impacts on surface ozone predictions during summer in China
Daytime isoprene nitrates under changing NOx and O3
Atmospheric data support a multi-decadal shift in the global methane budget towards natural tropical emissions
Air quality and related health impact in the UNECE region: source attribution and scenario analysis
Future tropospheric ozone budget and distribution over East Asia under a Net Zero scenario
East Asian methane emissions inferred from high-resolution inversions of GOSAT and TROPOMI observations: a comparative and evaluative analysis
Towards near-real-time air pollutant and greenhouse gas emissions: lessons learned from multiple estimates during the COVID-19 pandemic
Spatiotemporal variation of radionuclide dispersion from nuclear power plant accidents using FLEXPART mini-ensemble modeling
Continuous weekly monitoring of methane emissions from the Permian Basin by inversion of TROPOMI satellite observations
Western European emission estimates of CFC-11, CFC-12 and CCl4 derived from atmospheric measurements from 2008 to 2021
Evaluating modelled tropospheric columns of CH4, CO and O3 in the Arctic using ground-based FTIR measurements
Utility of Geostationary Lightning Mapper Derived Lightning NOx Emission Estimates in Air Quality Modeling Studies
Investigating the differences in calculating global mean surface CO2 abundance: the impact of analysis methodologies and site selection
Estimating methane emissions in the Arctic nations using surface observations from 2008 to 2019
Seasonal, interannual and decadal variability of tropospheric ozone in the North Atlantic: comparison of UM-UKCA and remote sensing observations for 2005–2018
Quantification of oil and gas methane emissions in the Delaware and Marcellus basins using a network of continuous tower-based measurements
Global sensitivities of reactive N and S gas and particle concentrations and deposition to precursor emissions reductions
A high-resolution Global Aviation emissions Inventory based on ADS-B (GAIA) for 2019–2021
Large simulated future changes in the nitrate radical under the CMIP6 SSP scenarios: implications for oxidation chemistry
Impact of HO2 aerosol uptake on radical levels and O3 production during summertime in Beijing
Source attribution of near-surface ozone trends in the United States during 1995–2019
Exploring the drivers of tropospheric hydroxyl radical trends in the Geophysical Fluid Dynamics Laboratory AM4.1 atmospheric chemistry–climate model
Comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA: Implications to atmospheric oxidative capacity
Impacts of land cover changes on biogenic emission and its contribution to ozone and secondary organic aerosol in China
High-resolution regional emission inventory contributes to the evaluation of policy effectiveness: a case study in Jiangsu Province, China
Why is ozone in South Korea and the Seoul metropolitan area so high and increasing?
Ling Huang, Jiong Fang, Jiaqiang Liao, Greg Yarwood, Hui Chen, Yangjun Wang, and Li Li
Atmos. Chem. Phys., 23, 14919–14932, https://doi.org/10.5194/acp-23-14919-2023, https://doi.org/10.5194/acp-23-14919-2023, 2023
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Surface ozone concentrations have emerged as a major environmental issue in China. Although control strategies aimed at reducing NOx emissions from conventional combustion sources are widely recognized, soil NOx emissions have received little attention. The impact of soil NO emissions on ground-level ozone concentration is yet to be evaluated. In this study, we estimated the soil NO emissions and evaluated its impact on ozone formation in China.
Ben A. Cala, Scott Archer-Nicholls, James Weber, N. Luke Abraham, Paul T. Griffiths, Lorrie Jacob, Y. Matthew Shin, Laura E. Revell, Matthew Woodhouse, and Alexander T. Archibald
Atmos. Chem. Phys., 23, 14735–14760, https://doi.org/10.5194/acp-23-14735-2023, https://doi.org/10.5194/acp-23-14735-2023, 2023
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Dimethyl sulfide (DMS) is an important trace gas emitted from the ocean recognised as setting the sulfate aerosol background, but its oxidation is complex. As a result representation in chemistry-climate models is greatly simplified. We develop and compare a new mechanism to existing mechanisms via a series of global and box model experiments. Our studies show our updated DMS scheme is a significant improvement but significant variance exists between mechanisms.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 23, 14127–14158, https://doi.org/10.5194/acp-23-14127-2023, https://doi.org/10.5194/acp-23-14127-2023, 2023
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In this study, we used a regional chemical transport model to characterize the different parameters of atmospheric oxidative capacity in recent chemical environments in China. These parameters include the production and destruction rates of ozone and other oxidants, the ozone production efficiency, the OH reactivity, and the length of the reaction chain responsible for the formation of ozone and ROx. They are also affected by the aerosol burden in the atmosphere.
Zhenze Liu, Oliver Wild, Ruth M. Doherty, Fiona M. O'Connor, and Steven T. Turnock
Atmos. Chem. Phys., 23, 13755–13768, https://doi.org/10.5194/acp-23-13755-2023, https://doi.org/10.5194/acp-23-13755-2023, 2023
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We investigate the impact of net-zero policies on surface ozone pollution in China. A chemistry–climate model is used to simulate ozone changes driven by local and external emissions, methane, and warmer climates. A deep learning model is applied to generate more robust ozone projection, and we find that the benefits of net-zero policies may be overestimated with the chemistry–climate model. Nevertheless, it is clear that the policies can still substantially reduce ozone pollution in future.
Gemma Purser, Mathew R. Heal, Edward J. Carnell, Stephen Bathgate, Julia Drewer, James I. L. Morison, and Massimo Vieno
Atmos. Chem. Phys., 23, 13713–13733, https://doi.org/10.5194/acp-23-13713-2023, https://doi.org/10.5194/acp-23-13713-2023, 2023
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Forest expansion is a ″net-zero“ pathway, but change in land cover alters air quality in many ways. This study combines tree planting suitability data with UK measured emissions of biogenic volatile organic compounds to simulate spatial and temporal changes in atmospheric composition for planting scenarios of four species. Decreases in fine particulate matter are relatively larger than increases in ozone, which may indicate a net benefit of tree planting on human health aspects of air quality.
Wei Li, Yuxuan Wang, Xueying Liu, Ehsan Soleimanian, Travis Griggs, James Flynn, and Paul Walter
Atmos. Chem. Phys., 23, 13685–13699, https://doi.org/10.5194/acp-23-13685-2023, https://doi.org/10.5194/acp-23-13685-2023, 2023
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This study examined high offshore ozone events in Galveston Bay and the Gulf of Mexico, using boat data and WRF–CAMx modeling during the TRACER-AQ 2021 field campaign. On average, high ozone is caused by chemistry due to the regional transport of volatile organic compounds and downwind advection of NOx from the ship channel. Two case studies show advection of ozone can be another process leading to high ozone, and accurate wind prediction is crucial for air quality forecasting in coastal areas.
Richard G. Derwent, David D. Parrish, and Ian C. Faloona
Atmos. Chem. Phys., 23, 13613–13623, https://doi.org/10.5194/acp-23-13613-2023, https://doi.org/10.5194/acp-23-13613-2023, 2023
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Elevated tropospheric ozone concentrations driven by anthropogenic precursor emissions are a world-wide health and environmental concern; however, this issue lacks a generally accepted understanding of the scientific issues. Here, we briefly outline the elements required to conduct an international assessment process to establish a conceptual model of the underpinning science and motivate international policy forums for regulating ozone production over hemispheric and global scales.
Nicola J. Warwick, Alex T. Archibald, Paul T. Griffiths, James Keeble, Fiona M. O'Connor, John A. Pyle, and Keith P. Shine
Atmos. Chem. Phys., 23, 13451–13467, https://doi.org/10.5194/acp-23-13451-2023, https://doi.org/10.5194/acp-23-13451-2023, 2023
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A chemistry–climate model has been used to explore the atmospheric response to changes in emissions of hydrogen and other species associated with a shift from fossil fuel to hydrogen use. Leakage of hydrogen results in indirect global warming, offsetting greenhouse gas emission reductions from reduced fossil fuel use. To maximise the benefit of hydrogen as an energy source, hydrogen leakage and emissions of methane, carbon monoxide and nitrogen oxides should be minimised.
Susanna Strada, Andrea Pozzer, Graziano Giuliani, Erika Coppola, Fabien Solmon, Xiaoyan Jiang, Alex Guenther, Efstratios Bourtsoukidis, Dominique Serça, Jonathan Williams, and Filippo Giorgi
Atmos. Chem. Phys., 23, 13301–13327, https://doi.org/10.5194/acp-23-13301-2023, https://doi.org/10.5194/acp-23-13301-2023, 2023
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Water deficit modifies emissions of isoprene, an aromatic compound released by plants that influences the production of an air pollutant such as ozone. Numerical modelling shows that, during the warmest and driest summers, isoprene decreases between −20 and −60 % over the Euro-Mediterranean region, while near-surface ozone only diminishes by a few percent. Decreases in isoprene emissions not only happen under dry conditions, but also could occur after prolonged or repeated water deficits.
Guowen He, Cheng He, Haofan Wang, Xiao Lu, Chenglei Pei, Xiaonuan Qiu, Chenxi Liu, Yiming Wang, Nanxi Liu, Jinpu Zhang, Lei Lei, Yiming Liu, Haichao Wang, Tao Deng, Qi Fan, and Shaojia Fan
Atmos. Chem. Phys., 23, 13107–13124, https://doi.org/10.5194/acp-23-13107-2023, https://doi.org/10.5194/acp-23-13107-2023, 2023
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We analyze nighttime ozone in the lower boundary layer (up to 500 m) from the 2017–2019 measurements at the Canton Tower and the WRF-CMAQ model. We identify a strong ability of the residual layer to store daytime ozone in the convective mixing layer, investigate the chemical and meteorological factors controlling nighttime ozone in the residual layer, and quantify the contribution of nighttime ozone in the residual layer to both the nighttime and the following day’s surface ozone air quality.
Clara M. Nussbaumer, Horst Fischer, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 23, 12651–12669, https://doi.org/10.5194/acp-23-12651-2023, https://doi.org/10.5194/acp-23-12651-2023, 2023
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Ozone is a greenhouse gas and contributes to the earth’s radiative energy budget and therefore to global warming. This effect is the largest in the upper troposphere. In this study, we investigate the processes controlling ozone formation and the sensitivity to its precursors in the upper tropical troposphere based on model simulations by the ECHAM5/MESSy2 Atmospheric Chemistry (EMAC) model. We find that NO𝑥 emissions from lightning most importantly affect ozone chemistry at these altitudes.
Alba Badia, Veronica Vidal, Sergi Ventura, Roger Curcoll, Ricard Segura, and Gara Villalba
Atmos. Chem. Phys., 23, 10751–10774, https://doi.org/10.5194/acp-23-10751-2023, https://doi.org/10.5194/acp-23-10751-2023, 2023
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Improving air quality is a top priority in urban areas. In this study, we used an air quality model to analyse the air quality changes occurring over the metropolitan area of Barcelona and other rural areas affected by transport of the atmospheric plume from the city during mobility restrictions. Our results show that mitigation strategies intended to reduce O3 should be designed according to the local meteorology, air transport, and particular ozone chemistry of the urban area.
Herizo Narivelo, Paul David Hamer, Virginie Marécal, Luke Surl, Tjarda Roberts, Sophie Pelletier, Béatrice Josse, Jonathan Guth, Mickaël Bacles, Simon Warnach, Thomas Wagner, Stefano Corradini, Giuseppe Salerno, and Lorenzo Guerrieri
Atmos. Chem. Phys., 23, 10533–10561, https://doi.org/10.5194/acp-23-10533-2023, https://doi.org/10.5194/acp-23-10533-2023, 2023
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Volcanic emissions emit large quantities of gases and primary aerosols that can play an important role in atmospheric chemistry. We present a study of the fate of volcanic bromine emissions from the eruption of Mount Etna around Christmas 2018. Using a numerical model and satellite observations, we analyse the impact of the volcanic plume and how it modifies the composition of the air over the whole Mediterranean basin, in particular on tropospheric ozone through the bromine-explosion cycle.
Glenn-Michael Oomen, Jean-François Müller, Trissevgeni Stavrakou, Isabelle De Smedt, Thomas Blumenstock, Rigel Kivi, Maria Makarova, Mathias Palm, Amelie Röhling, Yao Té, Corinne Vigouroux, Martina M. Friedrich, Udo Frieß, François Hendrick, Alexis Merlaud, Ankie Piters, Andreas Richter, Michel Van Roozendael, and Thomas Wagner
EGUsphere, https://doi.org/10.5194/egusphere-2023-1972, https://doi.org/10.5194/egusphere-2023-1972, 2023
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Natural emissions from vegetation have a profound impact on air quality for their role in the formation of harmful tropospheric ozone and organic aerosols, yet these emissions are highly uncertain. In this study, we quantify emissions of organic gases over Europe using high-quality satellite measurements of formaldehyde. These satellite observations suggest that emissions from vegetation are much higher than predicted by models, especially in southern Europe.
Michael P. Cartwright, Richard J. Pope, Jeremy J. Harrison, Martyn P. Chipperfield, Chris Wilson, Wuhu Feng, David P. Moore, and Parvadha Suntharalingam
Atmos. Chem. Phys., 23, 10035–10056, https://doi.org/10.5194/acp-23-10035-2023, https://doi.org/10.5194/acp-23-10035-2023, 2023
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A 3-D chemical transport model, TOMCAT, is used to simulate global atmospheric carbonyl sulfide (OCS) distribution. Modelled OCS compares well with satellite observations of OCS from limb-sounding satellite observations. Model simulations also compare adequately with surface and atmospheric observations and suitably capture the seasonality of OCS and background concentrations.
Luana S. Basso, Chris Wilson, Martyn P. Chipperfield, Graciela Tejada, Henrique L. G. Cassol, Egídio Arai, Mathew Williams, T. Luke Smallman, Wouter Peters, Stijn Naus, John B. Miller, and Manuel Gloor
Atmos. Chem. Phys., 23, 9685–9723, https://doi.org/10.5194/acp-23-9685-2023, https://doi.org/10.5194/acp-23-9685-2023, 2023
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The Amazon’s carbon balance may have changed due to forest degradation, deforestation and warmer climate. We used an atmospheric model and atmospheric CO2 observations to quantify Amazonian carbon emissions (2010–2018). The region was a small carbon source to the atmosphere, mostly due to fire emissions. Forest uptake compensated for ~ 50 % of the fire emissions, meaning that the remaining forest is still a small carbon sink. We found no clear evidence of weakening carbon uptake over the period.
Rui Zhu, Zhaojun Tang, Xiaokang Chen, Xiong Liu, and Zhe Jiang
Atmos. Chem. Phys., 23, 9745–9763, https://doi.org/10.5194/acp-23-9745-2023, https://doi.org/10.5194/acp-23-9745-2023, 2023
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Ozone Monitoring Instrument (OMI) and surface O3 observations are used to investigate the changes in tropospheric O3 in the USA and Europe in 2005–2020. The surface-based assimilations show limited changes in surface and tropospheric column O3. The OMI-based assimilations show larger decreases in tropospheric O3 columns in 2010–2014, related to a decline in free-tropospheric NO2. Analysis suggests limited impacts of local emissions decline on tropospheric O3 over the USA and Europe in 2005–2020.
R. Bradley Pierce, Monica Harkey, Allen Lenzen, Lee M. Cronce, Jason A. Otkin, Jonathan L. Case, David S. Henderson, Zac Adelman, Tsengel Nergui, and Christopher R. Hain
Atmos. Chem. Phys., 23, 9613–9635, https://doi.org/10.5194/acp-23-9613-2023, https://doi.org/10.5194/acp-23-9613-2023, 2023
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We evaluate two high-resolution model simulations with different meteorological inputs but identical chemistry and anthropogenic emissions, with the goal of identifying a model configuration best suited for characterizing air quality in locations where lake breezes commonly affect local air quality along the Lake Michigan shoreline. This analysis complements other studies in evaluating the impact of meteorological inputs and parameterizations on air quality in a complex environment.
Rona L. Thompson, Stephen A. Montzka, Martin K. Vollmer, Jgor Arduini, Molly Crotwell, Paul Krummel, Chris Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Stefan Reimann, Isaac Vimont, Hsiang Wang, Ray F. Weiss, and Dickon Young
EGUsphere, https://doi.org/10.5194/egusphere-2023-1917, https://doi.org/10.5194/egusphere-2023-1917, 2023
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The hydroxyl radical (OH) determines the atmospheric lifetimes of numerous species including methane. Since OH is very short-lived it is not possible to directly measure its concentration on scales relevant for understanding its effect on other species. Here, OH is inferred by looking at changes in hydrofluorocarbons (HFCs). We find OH levels have been fairly stable over our study period (2004 to 2021) suggesting that OH is not the main driver of the recent increase in atmospheric methane.
Shreta Ghimire, Zachary J. Lebo, Shane Murphy, Stefan Rahimi, and Trang Tran
Atmos. Chem. Phys., 23, 9413–9438, https://doi.org/10.5194/acp-23-9413-2023, https://doi.org/10.5194/acp-23-9413-2023, 2023
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High wintertime ozone levels have occurred often in recent years in mountain basins with oil and gas production facilities. Photochemical modeling of ozone production serves as a basis for understanding the mechanism by which it occurs and for predictive capability. We present photochemical model simulations of ozone formation and accumulation in the Upper Green River basin, Wyoming, demonstrating the model's ability to simulate wintertime ozone and the sensitivity of ozone to its precursors.
Christian Rödenbeck, Karina E. Adcock, Markus Eritt, Maksym Gachkivsky, Christoph Gerbig, Samuel Hammer, Armin Jordan, Ralph F. Keeling, Ingeborg Levin, Fabian Maier, Andrew C. Manning, Heiko Moossen, Saqr Munassar, Penelope A. Pickers, Michael Rothe, Yasunori Tohjima, and Sönke Zaehle
EGUsphere, https://doi.org/10.5194/egusphere-2023-767, https://doi.org/10.5194/egusphere-2023-767, 2023
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The carbon dioxide content of the Earth atmosphere is increasing due to human emissions from burning of fossil fuels, causing global climate change. The strength of the fossil-fuel emissions is estimated by inventories based on energy data, but independent validation of these inventories has been recommended by the Intergovernmental Panel on Climate Change. Here we investigate the potential to validate inventories based on measurements of small changes in the atmospheric oxygen content.
Adedayo R. Adedeji, Stephen J. Andrews, Matthew J. Rowlinson, Mathew J. Evans, Alastair C. Lewis, Shigeru Hashimoto, Hitoshi Mukai, Hiroshi Tanimoto, Yasunori Tohjima, and Takuya Saito
Atmos. Chem. Phys., 23, 9229–9244, https://doi.org/10.5194/acp-23-9229-2023, https://doi.org/10.5194/acp-23-9229-2023, 2023
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We use the GEOS-Chem model to interpret observations of CO, C2H6, C3H8, NOx, NOy and O3 made from Hateruma Island in 2018. The model captures many synoptic-scale events and the seasonality of most pollutants at the site but underestimates C2H6 and C3H8 during the winter. These underestimates are unlikely to be reconciled by increases in biomass burning emissions but could be reconciled by increasing the Asian anthropogenic source of C2H6 and C3H8 by factors of around 2 and 3, respectively.
Bryan K. Place, William T. Hutzell, K. Wyat Appel, Sara Farrell, Lukas Valin, Benjamin N. Murphy, Karl M. Seltzer, Golam Sarwar, Christine Allen, Ivan R. Piletic, Emma L. D'Ambro, Emily Saunders, Heather Simon, Ana Torres-Vasquez, Jonathan Pleim, Rebecca H. Schwantes, Matthew M. Coggon, Lu Xu, William R. Stockwell, and Havala O. T. Pye
Atmos. Chem. Phys., 23, 9173–9190, https://doi.org/10.5194/acp-23-9173-2023, https://doi.org/10.5194/acp-23-9173-2023, 2023
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Ground-level ozone is a pollutant with adverse human health and ecosystem effects. Air quality models allow scientists to understand the chemical production of ozone and demonstrate impacts of air quality management plans. In this work, the role of multiple systems in ozone production was investigated for the northeastern US in summer. Model updates to chemical reaction rates and monoterpene chemistry were most influential in decreasing predicted ozone and improving agreement with observations.
Jonas Hachmeister, Oliver Schneising, Michael Buchwitz, John P. Burrows, Justus Notholt, and Matthias Buschmann
EGUsphere, https://doi.org/10.5194/egusphere-2023-1680, https://doi.org/10.5194/egusphere-2023-1680, 2023
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We quantified changes in atmospheric methane (CH4) concentrations using satellite data and a dynamic linear model approach. We calculated global annual methane increases for the years 2019–2022 which are in good agreement with other sources. For zonal methane growth rates, we identified strong inter-hemispheric differences in 2019 and 2022. For 2022, we could attribute decreases in the global growth rate to the Northern Hemisphere, possibly related to a reduction in anthropogenic emissions.
Yongliang She, Jingyi Li, Xiaopu Lyu, Hai Guo, Momei Qin, Xiaodong Xie, Kangjia Gong, Fei Ye, Jianjiong Mao, Lin Huang, and Jianlin Hu
EGUsphere, https://doi.org/10.5194/egusphere-2023-1358, https://doi.org/10.5194/egusphere-2023-1358, 2023
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The evaluation of predicted VOC in current chemical transport model is limited in China due to the lack of routine measurements at multiple sites. In this study, we use multi-site VOC measurements to evaluate the CMAQ model predicted VOC and assess the impacts of VOC bias on O3 simulation. Our results demonstrate that current modelling setups and emission inventories are likely to underpredict VOC concentrations, and this underprediction of VOC contributes to lower O3 predictions in China.
Alfred W. Mayhew, Peter M. Edwards, and Jaqueline F. Hamilton
Atmos. Chem. Phys., 23, 8473–8485, https://doi.org/10.5194/acp-23-8473-2023, https://doi.org/10.5194/acp-23-8473-2023, 2023
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Isoprene nitrates are chemical species commonly found in the atmosphere that are important for their impacts on air quality and climate. This paper investigates modelled changes to daytime isoprene nitrate concentrations resulting from changes in NOx and O3. The results highlight the complex, nonlinear chemistry of this group of species under typical conditions for megacities such as Beijing, with many species showing increased concentrations when NOx is decreased and/or ozone is increased.
Alice Drinkwater, Paul I. Palmer, Liang Feng, Tim Arnold, Xin Lan, Sylvia E. Michel, Robert Parker, and Hartmut Boesch
Atmos. Chem. Phys., 23, 8429–8452, https://doi.org/10.5194/acp-23-8429-2023, https://doi.org/10.5194/acp-23-8429-2023, 2023
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Changes in atmospheric methane over the last few decades are largely unexplained. Previous studies have proposed different hypotheses to explain short-term changes in atmospheric methane. We interpret observed changes in atmospheric methane and stable isotope source signatures (2004–2020). We argue that changes over this period are part of a large-scale shift from high-northern-latitude thermogenic energy emissions to tropical biogenic emissions, particularly from North Africa and South America.
Claudio A. Belis and Rita Van Dingenen
Atmos. Chem. Phys., 23, 8225–8240, https://doi.org/10.5194/acp-23-8225-2023, https://doi.org/10.5194/acp-23-8225-2023, 2023
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The study assesses the influence that abating emissions in the rest of the world have on exposure and mortality due to ozone and fine particulate matter in the region covered by the Gothenburg protocol (UNECE, mainly Europe and North America). To that end, the impacts of pollutants derived from different geographic areas and anthropogenic sources are analysed in a series of scenarios including measures to abate air pollutants and greenhouse gas emissions with different levels of ambition.
Xuewei Hou, Oliver Wild, Bin Zhu, and James Lee
EGUsphere, https://doi.org/10.5194/egusphere-2023-1592, https://doi.org/10.5194/egusphere-2023-1592, 2023
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In response to the climate crisis, many countries have committed to net zero in a certain future year. The impacts of net zero scenario on tropospheric O3 are less well studied and remain unclear. In this study, we quantified the changes of tropospheric O3 budgets, spatiotemporal distributions of future surface O3 in East Asia and regional O3 source contributions for 2060 under a net zero scenario, using the NCAR Community Earth System Model (CESM) and online O3 tagging methods.
Ruosi Liang, Yuzhong Zhang, Wei Chen, Peixuan Zhang, Jingran Liu, Cuihong Chen, Huiqin Mao, Guofeng Shen, Zhen Qu, Zichong Chen, Minqiang Zhou, Pucai Wang, Robert J. Parker, Hartmut Boesch, Alba Lorente, Joannes D. Maasakkers, and Ilse Aben
Atmos. Chem. Phys., 23, 8039–8057, https://doi.org/10.5194/acp-23-8039-2023, https://doi.org/10.5194/acp-23-8039-2023, 2023
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We compare and evaluate East Asian methane emissions inferred from different satellite observations (GOSAT and TROPOMI). The results show discrepancies over northern India and eastern China. Independent ground-based observations are more consistent with TROPOMI-derived emissions in northern India and GOSAT-derived emissions in eastern China.
Marc Guevara, Hervé Petetin, Oriol Jorba, Hugo Denier van der Gon, Jeroen Kuenen, Ingrid Super, Claire Granier, Thierno Doumbia, Philippe Ciais, Zhu Liu, Robin D. Lamboll, Sabine Schindlbacher, Bradley Matthews, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 8081–8101, https://doi.org/10.5194/acp-23-8081-2023, https://doi.org/10.5194/acp-23-8081-2023, 2023
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This study provides an intercomparison of European 2020 emission changes derived from official inventories, which are reported by countries under the framework of several international conventions and directives, and non-official near-real-time estimates, the use of which has significantly grown since the COVID-19 outbreak. The results of the work are used to produce recommendations on how best to approach and make use of near-real-time emissions for modelling and monitoring applications.
Seyed Omid Nabavi, Theodoros Christoudias, Yiannis Proestos, Christos Fountoukis, Huda Al-Sulaiti, and Jos Lelieveld
Atmos. Chem. Phys., 23, 7719–7739, https://doi.org/10.5194/acp-23-7719-2023, https://doi.org/10.5194/acp-23-7719-2023, 2023
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The objective of our study is to comprehensively assess the timing of radioactive material transportation and deposition, along with the associated population exposure in the designated region. We employed diverse meteorological inputs, emission specifics, and simulation codes, aiming to quantify the level of uncertainty.
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.
Alison L. Redington, Alistair J. Manning, Stephan Henne, Francesco Graziosi, Luke M. Western, Jgor Arduini, Anita L. Ganesan, Christina M. Harth, Michela Maione, Jens Mühle, Simon O'Doherty, Joseph Pitt, Stefan Reimann, Matthew Rigby, Peter K. Salameh, Peter G. Simmonds, T. Gerard Spain, Kieran Stanley, Martin K. Vollmer, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 23, 7383–7398, https://doi.org/10.5194/acp-23-7383-2023, https://doi.org/10.5194/acp-23-7383-2023, 2023
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Chlorofluorocarbons (CFCs) were used in Europe pre-1990, damaging the stratospheric ozone layer. Legislation has controlled production and use, and global emissions have decreased sharply. The global rate of decline in CFC-11 recently slowed and was partly attributed to illegal emission in eastern China. This study concludes that emissions of CFC-11 in western Europe have not contributed to the unexplained part of the global increase in CFC-11 observed in the last decade.
Victoria A. Flood, Kimberly Strong, Cynthia H. Whaley, Kaley A. Walker, Thomas Blumenstock, James W. Hannigan, Johan Mellqvist, Justus Notholt, Mathias Palm, Amelie N. Röhling, Stephen Arnold, Stephen Beagley, Rong-You Chien, Jesper Christensen, Makoto Deushi, Srdjan Dobricic, Xinyi Dong, Joshua S. Fu, Michael Gauss, Wanmin Gong, Joakim Langner, Kathy S. Law, Louis Marelle, Tatsuo Onishi, Naga Oshima, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Manu A. Thomas, Svetlana Tsyro, and Steven Turnock
EGUsphere, https://doi.org/10.5194/egusphere-2023-1161, https://doi.org/10.5194/egusphere-2023-1161, 2023
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It is important to understand the composition of the Arctic atmosphere and how it is changing. Atmospheric models provide simulations that can inform policy. This study examines simulations of CH4, CO, and O3 by 11 models. Model performance is assessed by comparing results matched in space and time to measurements from five high-latitude ground-based infrared spectrometers. This work finds that models are generally underpredicting the concentrations of these gases in the Arctic troposphere.
Peiyang Cheng, Arastoo Pour-Biazar, Yuling Wu, Shi Kuang, Richard T. McNider, and William J. Koshak
EGUsphere, https://doi.org/10.5194/egusphere-2023-901, https://doi.org/10.5194/egusphere-2023-901, 2023
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Lightning-induced nitrogen monoxide (LNO) emission can be estimated from geostationary satellite observations. The present study uses the LNO emission estimates derived from geostationary satellite observations in an air quality modeling system to investigate the impact of LNO to air quality. Results indicate that significant ozone increase could be due to long-distance chemical transport, lightning activity in the upwind direction, and the mixing of high LNO (or ozone) plumes.
Zhendong Wu, Alex Vermeulen, Yousuke Sawa, Ute Karstens, Wouter Peters, Remco de Kok, Xin Lan, Yasuyuki Nagai, Akinori Ogi, and Oksana Tarasova
EGUsphere, https://doi.org/10.5194/egusphere-2023-1173, https://doi.org/10.5194/egusphere-2023-1173, 2023
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This study focuses on exploring the differences in calculating global surface CO2 and its growth rate, considering the impact of analysis methodologies and site selection. Our study reveals that the current global CO2 network has a good capacity to represent global surface CO2 and its growth rate and trends in atmospheric CO2 mass changes, although small differences exist in different analyses due to the impact of methodology and site selection.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, Joël Thanwerdas, Adrien Martinez, Jean-Daniel Paris, Toshinobu Machida, Motoki Sasakawa, Douglas E. J. Worthy, Xin Lan, Rona L. Thompson, Espen Sollum, and Mikhail Arshinov
Atmos. Chem. Phys., 23, 6457–6485, https://doi.org/10.5194/acp-23-6457-2023, https://doi.org/10.5194/acp-23-6457-2023, 2023
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Here, an inverse modelling approach is applied to estimate CH4 sources and sinks in the Arctic from 2008 to 2019. We study the magnitude, seasonal patterns and trends from different sources during recent years. We also assess how the current observation network helps to constrain fluxes. We find that constraints are only significant for North America and, to a lesser extent, West Siberia, where the observation network is relatively dense. We find no clear trend over the period of inversion.
Maria Rosa Russo, Brian John Kerridge, Nathan Luke Abraham, James Keeble, Barry Graham Latter, Richard Siddans, James Weber, Paul Thomas Griffiths, John Adrian Pyle, and Alexander Thomas Archibald
Atmos. Chem. Phys., 23, 6169–6196, https://doi.org/10.5194/acp-23-6169-2023, https://doi.org/10.5194/acp-23-6169-2023, 2023
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Tropospheric ozone is an important component of the Earth system as it can affect both climate and air quality. In this work we use observed tropospheric ozone derived from satellite observations and compare it to tropospheric ozone from model simulations. Our aim is to investigate recent changes (2005–2018) in tropospheric ozone in the North Atlantic region and to understand what factors are driving such changes.
Zachary Barkley, Kenneth Davis, Natasha Miles, Scott Richardson, Aijun Deng, Benjamin Hmiel, David Lyon, and Thomas Lauvaux
Atmos. Chem. Phys., 23, 6127–6144, https://doi.org/10.5194/acp-23-6127-2023, https://doi.org/10.5194/acp-23-6127-2023, 2023
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Using methane monitoring instruments attached to towers, we measure methane concentrations and quantify methane emissions coming from the Marcellus and Permian oil and gas basins. In the Marcellus, emissions were 3 times higher than the state inventory across the entire monitoring period. In the Permian, we see a sharp decline in emissions aligning with the onset of the COVID-19 pandemic. Tower observational networks can be utilized in other basins for long-term monitoring of emissions.
Yao Ge, Massimo Vieno, David S. Stevenson, Peter Wind, and Mathew R. Heal
Atmos. Chem. Phys., 23, 6083–6112, https://doi.org/10.5194/acp-23-6083-2023, https://doi.org/10.5194/acp-23-6083-2023, 2023
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The sensitivity of fine particles and reactive N and S species to reductions in precursor emissions is investigated using the EMEP MSC-W (European Monitoring and Evaluation Programme Meteorological Synthesizing Centre – West) atmospheric chemistry transport model. This study reveals that the individual emissions reduction has multiple and geographically varying co-benefits and small disbenefits on different species, demonstrating the importance of prioritizing regional emissions controls.
Roger Teoh, Zebediah Engberg, Marc Shapiro, Lynnette Dray, and Marc Stettler
EGUsphere, https://doi.org/10.5194/egusphere-2023-724, https://doi.org/10.5194/egusphere-2023-724, 2023
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Emissions from aircraft contribute to climate change and degrade air quality. We describe an up-to-date 4D emissions inventory of global aviation from 2019 to 2021 based on actual flown trajectories. In 2019, 40.2 million flights collectively travelled 61 billion kilometres using 283 Tg of fuel. Long-haul flights were responsible for 43 % of CO2. The emissions inventory is made available for use in future studies to evaluate the negative externalities arising from global aviation.
Scott Archer-Nicholls, Rachel Allen, Nathan L. Abraham, Paul T. Griffiths, and Alex T. Archibald
Atmos. Chem. Phys., 23, 5801–5813, https://doi.org/10.5194/acp-23-5801-2023, https://doi.org/10.5194/acp-23-5801-2023, 2023
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The nitrate radical is a major oxidant at nighttime, but much less is known about it than about the other oxidants ozone and OH. We use Earth system model calculations to show how the nitrate radical has changed in abundance from 1850–2014 and to 2100 under a range of different climate and emission scenarios. Depending on the emissions and climate scenario, significant increases are projected with implications for the oxidation of volatile organic compounds and the formation of fine aerosol.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
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The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Pengwei Li, Yang Yang, Hailong Wang, Su Li, Ke Li, Pinya Wang, Baojie Li, and Hong Liao
Atmos. Chem. Phys., 23, 5403–5417, https://doi.org/10.5194/acp-23-5403-2023, https://doi.org/10.5194/acp-23-5403-2023, 2023
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We use a novel technique that can attribute O3 to precursors to investigate O3 changes in the United States during 1995–2019. We found that the US domestic energy and surface transportation emission reductions are primarily responsible for the O3 decrease in summer. In winter, factors such as nitrogen oxide emission reduction in the context of its inhibition of ozone production, increased aviation and shipping activities, and large-scale circulation changes contribute to the O3 increases.
Glen Chua, Vaishali Naik, and Larry Wayne Horowitz
Atmos. Chem. Phys., 23, 4955–4975, https://doi.org/10.5194/acp-23-4955-2023, https://doi.org/10.5194/acp-23-4955-2023, 2023
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The hydroxyl radical (OH) is an atmospheric
detergent, removing air pollutants and greenhouse gases like methane from the atmosphere. Thus, understanding how it is changing and responding to its various drivers is important for air quality and climate. We found that OH has increased by about 5 % globally from 1980 to 2014 in our model, mostly driven by increasing nitrogen oxide (NOx) emissions. This suggests potential climate tradeoffs from air quality policies solely targeting NOx emissions.
Meghna Soni, Rolf Sander, Lokesh K. Sahu, Domenico Taraborrelli, Pengfei Liu, Ankit Patel, Imran A. Girach, Andrea Pozzer, Sachin S. Gunthe, and Narendra Ojha
EGUsphere, https://doi.org/10.5194/egusphere-2023-652, https://doi.org/10.5194/egusphere-2023-652, 2023
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The study presents the implementation of comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA. Simulations for contrasting urban environments of Asia and Europe highlight the significant impacts of chlorine on atmospheric oxidation capacity and composition. Chemical processes governing the production and loss of chlorine-containing species have been discussed. The updated chemical mechanism will be useful to interpret field measurements and for future air quality studies.
Jinlong Ma, Shengqiang Zhu, Siyu Wang, Peng Wang, Jianmin Chen, and Hongliang Zhang
Atmos. Chem. Phys., 23, 4311–4325, https://doi.org/10.5194/acp-23-4311-2023, https://doi.org/10.5194/acp-23-4311-2023, 2023
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An updated version of the CMAQ model with biogenic volatile organic compound (BVOC) emissions from MEGAN was applied to study the impacts of different land cover inputs on O3 and secondary organic aerosol (SOA) in China. The estimated BVOC emissions ranged from 25.42 to 37.39 Tg using different leaf area index (LAI) and land cover (LC) inputs. Those differences further induced differences of 4.8–6.9 ppb in O3 concentrations and differences of 5.3–8.4 µg m−3 in SOA concentrations in China.
Chen Gu, Lei Zhang, Zidie Xu, Sijia Xia, Yutong Wang, Li Li, Zeren Wang, Qiuyue Zhao, Hanying Wang, and Yu Zhao
Atmos. Chem. Phys., 23, 4247–4269, https://doi.org/10.5194/acp-23-4247-2023, https://doi.org/10.5194/acp-23-4247-2023, 2023
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We demonstrated the development of a high-resolution emission inventory and its application to evaluate the effectiveness of emission control actions, by incorporating the improved methodology, the best available data, and air quality modeling. We show that substantial efforts for emission controls indeed played an important role in air quality improvement even with worsened meteorological conditions and that the contributions of individual measures to emission reduction were greatly changing.
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.
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Short summary
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.
We use the GEOS-Chem model to better understand the magnitude and trend in free tropospheric NO2...
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