Articles | Volume 16, issue 2
https://doi.org/10.5194/acp-16-525-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-525-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
19 Jan 2016
Research article |
| 19 Jan 2016
Sources of nitrogen deposition in Federal Class I areas in the US
Department of Civil, Environmental, and Architectural Engineering, University of Colorado, Boulder, CO, USA
F. Paulot
Geophysical Fluid Dynamics Laboratory and Princeton University, Princeton, NJ, USA
D. K. Henze
Department of Mechanical Engineering, University of Colorado, Boulder, CO, USA
K. Travis
School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
D. J. Jacob
School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
L. H. Pardo
USDA Forest Service, Northern Research Station, University of Vermont Aiken Center, Burlington, VT, USA
B. A. Schichtel
Cooperative Institute for Research in the Atmosphere, Colorado State University, Fort Collins, CO, USA
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Atmos. Chem. Phys., 26, 10455–10476, https://doi.org/10.5194/acp-26-10455-2026, https://doi.org/10.5194/acp-26-10455-2026, 2026
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Atmos. Chem. Phys., 26, 8021–8050, https://doi.org/10.5194/acp-26-8021-2026, https://doi.org/10.5194/acp-26-8021-2026, 2026
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EGUsphere, https://doi.org/10.5194/egusphere-2025-4626, https://doi.org/10.5194/egusphere-2025-4626, 2025
Preprint archived
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We use data from both aircraft (MethaneAIR) and satellite (TROPOMI) based measurements of methane in the atmosphere to better understand methane emissions from fossil fuel extraction. Data from these instruments are combined with a computer model of the atmosphere to improve estimates of methane emissions. We find that combining data from multiple sources provides more information than either source on its own. The tools and data we use are freely available.
Lillian E. Naimie, Da Pan, Amy P. Sullivan, John T. Walker, Aleksandra Djurkovic, Bret A. Schichtel, and Jeffrey L. Collett Jr.
Atmos. Chem. Phys., 25, 15245–15261, https://doi.org/10.5194/acp-25-15245-2025, https://doi.org/10.5194/acp-25-15245-2025, 2025
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The contribution of ammonia atmosphere-surface exchange to excess deposition of reactive nitrogen is poorly understood. Reactive nitrogen deposition has negative impacts on ecosystem health. Ammonia can be difficult and expensive to measure. We demonstrate that depositions modeled using low-cost measurements underestimate ecosystem inputs but can be corrected using typical daily concentration cycles. We also illustrate the limitations of reanalysis meteorology for ammonia deposition modeling.
Jeewoo Lee, Jhoon Kim, Seoyoung Lee, Myungje Choi, Jaehwa Lee, Daniel J. Jacob, Su Keun Kuk, and Young-Je Park
Earth Syst. Sci. Data, 17, 5761–5782, https://doi.org/10.5194/essd-17-5761-2025, https://doi.org/10.5194/essd-17-5761-2025, 2025
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Atmospheric aerosols adversely affect human health, with East Asia recognized as one of the most impacted regions. This study presents a long-term (2011–2021), high spatiotemporal resolution aerosol optical depth dataset retrieved from a geostationary satellite over East Asia. The high-resolution data capture subtle aerosol gradients and land-ocean boundaries, providing valuable input for various fields such as aerosol-cloud interaction, climate change, ocean optics, and air quality studies.
Drew C. Pendergrass, Daniel J. Jacob, Nicholas Balasus, Lucas Estrada, Daniel J. Varon, James D. East, Megan He, Todd A. Mooring, Elise Penn, Hannah Nesser, and John R. Worden
Atmos. Chem. Phys., 25, 14353–14369, https://doi.org/10.5194/acp-25-14353-2025, https://doi.org/10.5194/acp-25-14353-2025, 2025
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We use satellite observations of atmospheric methane, a greenhouse gas, to calculate emissions from both human and natural sources. We find that methane emissions surged in 2020–2021 before declining in 2022–2023. We attribute the surge in large part to emissions from eastern Africa, which experienced large methane-generating floods. Wetland models underestimate emissions in that region, which has led some previous work to incorrectly attribute the African surge in methane emissions to livestock.
Prajjwal Rawat, James H. Crawford, Katherine R. Travis, Laura M. Judd, Mary Angelique G. Demetillo, Lukas C. Valin, James J. Szykman, Andrew Whitehill, Eric Baumann, and Thomas F. Hanisco
Atmos. Meas. Tech., 18, 2899–2917, https://doi.org/10.5194/amt-18-2899-2025, https://doi.org/10.5194/amt-18-2899-2025, 2025
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The Pandonia Global Network (PGN) consists of Pandora spectrometers that observe trace gases at a high time resolution to validate satellite observations and understand local air quality. To aid users, PGN assigns quality flags that assure scientifically valid data but eliminate large amounts of data appropriate for scientific applications. A new method based on contemporaneous data in two independent observation modes is proven using complementary ground-based and airborne observations.
Lucas A. Estrada, Daniel J. Varon, Melissa Sulprizio, Hannah Nesser, Zichong Chen, Nicholas Balasus, Sarah E. Hancock, Megan He, James D. East, Todd A. Mooring, Alexander Oort Alonso, Joannes D. Maasakkers, Ilse Aben, Sabour Baray, Kevin W. Bowman, John R. Worden, Felipe J. Cardoso-Saldaña, Emily Reidy, and Daniel J. Jacob
Geosci. Model Dev., 18, 3311–3330, https://doi.org/10.5194/gmd-18-3311-2025, https://doi.org/10.5194/gmd-18-3311-2025, 2025
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Reducing emissions of methane, a powerful greenhouse gas, is a top policy concern for mitigating anthropogenic climate change. The Integrated Methane Inversion (IMI) is an advanced, cloud-based software that translates satellite observations into actionable emissions data. Here we present IMI version 2.0 with vastly expanded capabilities. These updates enable a wider range of scientific and stakeholder applications from individual basin to global scales with continuous emissions monitoring.
Benjamin C. Sapper, Sean Youn, Daven K. Henze, Manjula Canagaratna, Harald Stark, and Jose L. Jimenez
Geosci. Model Dev., 18, 2891–2919, https://doi.org/10.5194/gmd-18-2891-2025, https://doi.org/10.5194/gmd-18-2891-2025, 2025
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Positive matrix factorization (PMF) has been used by atmospheric scientists to extract underlying factors present in large datasets. This paper presents a new technique for error-weighted PMF that drastically reduces the computational costs of previously developed algorithms. We use this technique to deliver interpretable factors and solution diagnostics from an atmospheric chemistry dataset.
Yujin J. Oak, Daniel J. Jacob, Drew C. Pendergrass, Ruijun Dang, Nadia K. Colombi, Heesung Chong, Seoyoung Lee, Su Keun Kuk, and Jhoon Kim
Atmos. Chem. Phys., 25, 3233–3252, https://doi.org/10.5194/acp-25-3233-2025, https://doi.org/10.5194/acp-25-3233-2025, 2025
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We analyze 2015–2023 air quality trends in South Korea using surface and satellite observations. Primary pollutants have decreased, consistent with emissions reductions. Surface O3 continues to increase and PM2.5 has decreased overall, but the nitrate component has not. O3 and PM2.5 nitrate depend on nonlinear responses from precursor emissions. Satellite data indicate a recent shift to NOx-sensitive O3 and nitrate formation, where further NOx reductions will benefit both O3 and PM2.5 pollution.
Elise Penn, Daniel J. Jacob, Zichong Chen, James D. East, Melissa P. Sulprizio, Lori Bruhwiler, Joannes D. Maasakkers, Hannah Nesser, Zhen Qu, Yuzhong Zhang, and John Worden
Atmos. Chem. Phys., 25, 2947–2965, https://doi.org/10.5194/acp-25-2947-2025, https://doi.org/10.5194/acp-25-2947-2025, 2025
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The hydroxyl radical (OH) destroys many air pollutants, including methane. Global-mean OH cannot be directly measured, and thus it is inferred with the methyl chloroform (MCF) proxy. MCF is decreasing, and a replacement is needed. We use satellite observations of methane in two spectral ranges as a proxy for OH. We find shortwave infrared observations can characterize yearly OH and its seasonality but not the latitudinal distribution. Thermal infrared observations add little information.
Sarah E. Hancock, Daniel J. Jacob, Zichong Chen, Hannah Nesser, Aaron Davitt, Daniel J. Varon, Melissa P. Sulprizio, Nicholas Balasus, Lucas A. Estrada, María Cazorla, Laura Dawidowski, Sebastián Diez, James D. East, Elise Penn, Cynthia A. Randles, John Worden, Ilse Aben, Robert J. Parker, and Joannes D. Maasakkers
Atmos. Chem. Phys., 25, 797–817, https://doi.org/10.5194/acp-25-797-2025, https://doi.org/10.5194/acp-25-797-2025, 2025
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We quantify 2021 methane emissions in South America at up to 25 km × 25 km resolution using satellite methane observations. We find a 55 % upward adjustment to anthropogenic emission inventories, including those reported to the UN Framework Convention on Climate Change under the Paris Agreement. Our estimates match inventories for Brazil, Bolivia, and Paraguay but are much higher for other countries. Livestock emissions (65 % of anthropogenic emissions) show the largest discrepancies.
Deepangsu Chatterjee, Randall V. Martin, Chi Li, Dandan Zhang, Haihui Zhu, Daven K. Henze, James H. Crawford, Ronald C. Cohen, Lok N. Lamsal, and Alexander M. Cede
Atmos. Chem. Phys., 24, 12687–12706, https://doi.org/10.5194/acp-24-12687-2024, https://doi.org/10.5194/acp-24-12687-2024, 2024
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We investigate the hourly variation of NO2 columns and surface concentrations by applying the GEOS-Chem model to interpret aircraft and ground-based measurements over the US and Pandora sun photometer measurements over the US, Europe, and Asia. Corrections to the Pandora columns and finer model resolution improve the modeled representation of the summertime hourly variation of total NO2 columns to explain the weaker hourly variation in NO2 columns than at the surface.
Yujin J. Oak, Daniel J. Jacob, Nicholas Balasus, Laura H. Yang, Heesung Chong, Junsung Park, Hanlim Lee, Gitaek T. Lee, Eunjo S. Ha, Rokjin J. Park, Hyeong-Ahn Kwon, and Jhoon Kim
Atmos. Meas. Tech., 17, 5147–5159, https://doi.org/10.5194/amt-17-5147-2024, https://doi.org/10.5194/amt-17-5147-2024, 2024
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We present an improved NO2 product from GEMS by calibrating it to TROPOMI using machine learning and by reprocessing both satellite products to adopt common NO2 profiles. Our corrected GEMS product combines the high data density of GEMS with the accuracy of TROPOMI, supporting the combined use for analyses of East Asia air quality including emissions and chemistry. This method can be extended to other species and geostationary satellites including TEMPO and Sentinel-4.
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
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Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Benjamin A. Nault, Katherine R. Travis, James H. Crawford, Donald R. Blake, Pedro Campuzano-Jost, Ronald C. Cohen, Joshua P. DiGangi, Glenn S. Diskin, Samuel R. Hall, L. Gregory Huey, Jose L. Jimenez, Kyung-Eun Min, Young Ro Lee, Isobel J. Simpson, Kirk Ullmann, and Armin Wisthaler
Atmos. Chem. Phys., 24, 9573–9595, https://doi.org/10.5194/acp-24-9573-2024, https://doi.org/10.5194/acp-24-9573-2024, 2024
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Ozone (O3) is a pollutant formed from the reactions of gases emitted from various sources. In urban areas, the density of human activities can increase the O3 formation rate (P(O3)), thus impacting air quality and health. Observations collected over Seoul, South Korea, are used to constrain P(O3). A high local P(O3) was found; however, local P(O3) was partly reduced due to compounds typically ignored. These observations also provide constraints for unmeasured compounds that will impact P(O3).
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
Atmos. Chem. Phys., 24, 8607–8624, https://doi.org/10.5194/acp-24-8607-2024, https://doi.org/10.5194/acp-24-8607-2024, 2024
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Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone, but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side by side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
Irene C. Dedoussi, Daven K. Henze, Sebastian D. Eastham, Raymond L. Speth, and Steven R. H. Barrett
Geosci. Model Dev., 17, 5689–5703, https://doi.org/10.5194/gmd-17-5689-2024, https://doi.org/10.5194/gmd-17-5689-2024, 2024
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Atmospheric model gradients provide a meaningful tool for better understanding the underlying atmospheric processes. Adjoint modeling enables computationally efficient gradient calculations. We present the adjoint of the GEOS-Chem unified chemistry extension (UCX). With this development, the GEOS-Chem adjoint model can capture stratospheric ozone and other processes jointly with tropospheric processes. We apply it to characterize the Antarctic ozone depletion potential of active halogen species.
Zhendong Lu, Jun Wang, Yi Wang, Daven K. Henze, Xi Chen, Tong Sha, and Kang Sun
Atmos. Chem. Phys., 24, 7793–7813, https://doi.org/10.5194/acp-24-7793-2024, https://doi.org/10.5194/acp-24-7793-2024, 2024
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In contrast with past work showing that the reduction of emissions was the dominant factor for the nationwide increase of surface O3 during the lockdown in China, this study finds that the variation in meteorology (temperature and other parameters) plays a more important role. This result is obtained through sensitivity simulations using a chemical transport model constrained by satellite (TROPOMI) data and calibrated with surface observations.
Laura Hyesung Yang, Daniel J. Jacob, Ruijun Dang, Yujin J. Oak, Haipeng Lin, Jhoon Kim, Shixian Zhai, Nadia K. Colombi, Drew C. Pendergrass, Ellie Beaudry, Viral Shah, Xu Feng, Robert M. Yantosca, Heesung Chong, Junsung Park, Hanlim Lee, Won-Jin Lee, Soontae Kim, Eunhye Kim, Katherine R. Travis, James H. Crawford, and Hong Liao
Atmos. Chem. Phys., 24, 7027–7039, https://doi.org/10.5194/acp-24-7027-2024, https://doi.org/10.5194/acp-24-7027-2024, 2024
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The Geostationary Environment Monitoring Spectrometer (GEMS) provides hourly measurements of NO2. We use the chemical transport model to find how emissions, chemistry, and transport drive the changes in NO2 observed by GEMS at different times of the day. In winter, the chemistry plays a minor role, and high daytime emissions dominate the diurnal variation in NO2, balanced by transport. In summer, emissions, chemistry, and transport play an important role in shaping the diurnal variation in NO2.
Drew C. Pendergrass, Daniel J. Jacob, Yujin J. Oak, Jeewoo Lee, Minseok Kim, Jhoon Kim, Seoyoung Lee, Shixian Zhai, Hitoshi Irie, and Hong Liao
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-172, https://doi.org/10.5194/essd-2024-172, 2024
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Fine particles suspended in the atmosphere are a major form of air pollution and an important public health burden. However, measurements of particulate matter are sparse in space and in places like East Asia monitors are established after regulatory policies to improve pollution have changed. In this paper, we use machine learning to fill in the gaps. We train an algorithm to predict pollution at the surface from the atmosphere’s opacity, then produce high resolution maps of data without gaps.
Jack H. Bruno, Dylan Jervis, Daniel J. Varon, and Daniel J. Jacob
Atmos. Meas. Tech., 17, 2625–2636, https://doi.org/10.5194/amt-17-2625-2024, https://doi.org/10.5194/amt-17-2625-2024, 2024
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Methane is a potent greenhouse gas and a current high-priority target for short- to mid-term climate change mitigation. Detection of individual methane emitters from space has become possible in recent years, and the volume of data for this task has been rapidly growing, outpacing processing capabilities. We introduce an automated approach, U-Plume, which can detect and quantify emissions from individual methane sources in high-spatial-resolution satellite data.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Alba Lorente, Zichong Chen, Xiao Lu, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Margaux Winter, Shuang Ma, A. Anthony Bloom, John R. Worden, Robert N. Stavins, and Cynthia A. Randles
Atmos. Chem. Phys., 24, 5069–5091, https://doi.org/10.5194/acp-24-5069-2024, https://doi.org/10.5194/acp-24-5069-2024, 2024
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We quantify 2019 methane emissions in the contiguous US (CONUS) at a ≈ 25 km × 25 km resolution using satellite methane observations. We find a 13 % upward correction to the 2023 US Environmental Protection Agency (EPA) Greenhouse Gas Emissions Inventory (GHGI) for 2019, with large corrections to individual states, urban areas, and landfills. This may present a challenge for US climate policies and goals, many of which target significant reductions in methane emissions.
Fabien Paulot, Gabrielle Pétron, Andrew M. Crotwell, and Matteo B. Bertagni
Atmos. Chem. Phys., 24, 4217–4229, https://doi.org/10.5194/acp-24-4217-2024, https://doi.org/10.5194/acp-24-4217-2024, 2024
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New data from the National Oceanic and Atmospheric Administration show that hydrogen (H2) concentrations increased from 2010 to 2019, which is consistent with the simulated increase in H2 photochemical production (mainly from methane). But this cannot be reconciled with the expected decrease (increase) in H2 anthropogenic emissions (soil deposition) in the same period. This shows gaps in our knowledge of the H2 biogeochemical cycle that must be resolved to quantify the impact of higher H2 usage.
Sebastian D. Eastham, Guillaume P. Chossière, Raymond L. Speth, Daniel J. Jacob, and Steven R. H. Barrett
Atmos. Chem. Phys., 24, 2687–2703, https://doi.org/10.5194/acp-24-2687-2024, https://doi.org/10.5194/acp-24-2687-2024, 2024
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Emissions from aircraft are known to cause air quality impacts worldwide, but the scale and mechanisms of this impact are not well understood. This work uses high-resolution computational modeling of the atmosphere to show that air pollution changes from aviation are mostly the result of emissions during cruise (high-altitude) operations, that these impacts are related to how much non-aviation pollution is present, and that prior regional assessments have underestimated these impacts.
Kelvin H. Bates, Mathew J. Evans, Barron H. Henderson, and Daniel J. Jacob
Geosci. Model Dev., 17, 1511–1524, https://doi.org/10.5194/gmd-17-1511-2024, https://doi.org/10.5194/gmd-17-1511-2024, 2024
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Accurate representation of rates and products of chemical reactions in atmospheric models is crucial for simulating concentrations of pollutants and climate forcers. We update the widely used GEOS-Chem atmospheric chemistry model with reaction parameters from recent compilations of experimental data and demonstrate the implications for key atmospheric chemical species. The updates decrease tropospheric CO mixing ratios and increase stratospheric nitrogen oxide mixing ratios, among other changes.
Weiyi Tang, Bess B. Ward, Michael Beman, Laura Bristow, Darren Clark, Sarah Fawcett, Claudia Frey, François Fripiat, Gerhard J. Herndl, Mhlangabezi Mdutyana, Fabien Paulot, Xuefeng Peng, Alyson E. Santoro, Takuhei Shiozaki, Eva Sintes, Charles Stock, Xin Sun, Xianhui S. Wan, Min N. Xu, and Yao Zhang
Earth Syst. Sci. Data, 15, 5039–5077, https://doi.org/10.5194/essd-15-5039-2023, https://doi.org/10.5194/essd-15-5039-2023, 2023
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Nitrification and nitrifiers play an important role in marine nitrogen and carbon cycles by converting ammonium to nitrite and nitrate. Nitrification could affect microbial community structure, marine productivity, and the production of nitrous oxide – a powerful greenhouse gas. We introduce the newly constructed database of nitrification and nitrifiers in the marine water column and guide future research efforts in field observations and model development of nitrification.
Drew C. Pendergrass, Daniel J. Jacob, Hannah Nesser, Daniel J. Varon, Melissa Sulprizio, Kazuyuki Miyazaki, and Kevin W. Bowman
Geosci. Model Dev., 16, 4793–4810, https://doi.org/10.5194/gmd-16-4793-2023, https://doi.org/10.5194/gmd-16-4793-2023, 2023
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We have built a tool called CHEEREIO that allows scientists to use observations of pollutants or gases in the atmosphere, such as from satellites or surface stations, to update supercomputer models that simulate the Earth. CHEEREIO uses the difference between the model simulations of the atmosphere and real-world observations to come up with a good guess for the actual composition of our atmosphere, the true emissions of various pollutants, and whatever else they may want to study.
Nicholas Balasus, Daniel J. Jacob, Alba Lorente, Joannes D. Maasakkers, Robert J. Parker, Hartmut Boesch, Zichong Chen, Makoto M. Kelp, Hannah Nesser, and Daniel J. Varon
Atmos. Meas. Tech., 16, 3787–3807, https://doi.org/10.5194/amt-16-3787-2023, https://doi.org/10.5194/amt-16-3787-2023, 2023
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We use machine learning to remove biases in TROPOMI satellite observations of atmospheric methane, with GOSAT observations serving as a reference. We find that the TROPOMI biases relative to GOSAT are related to the presence of aerosols and clouds, the surface brightness, and the specific detector that makes the observation aboard TROPOMI. The resulting blended TROPOMI+GOSAT product is more reliable for quantifying methane emissions.
Daniel J. Varon, Daniel J. Jacob, Benjamin Hmiel, Ritesh Gautam, David R. Lyon, Mark Omara, Melissa Sulprizio, Lu Shen, Drew Pendergrass, Hannah Nesser, Zhen Qu, Zachary R. Barkley, Natasha L. Miles, Scott J. Richardson, Kenneth J. Davis, Sudhanshu Pandey, Xiao Lu, Alba Lorente, Tobias Borsdorff, Joannes D. Maasakkers, and Ilse Aben
Atmos. Chem. Phys., 23, 7503–7520, https://doi.org/10.5194/acp-23-7503-2023, https://doi.org/10.5194/acp-23-7503-2023, 2023
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We use TROPOMI satellite observations to quantify weekly methane emissions from the US Permian oil and gas basin from May 2018 to October 2020. We find that Permian emissions are highly variable, with diverse economic and activity drivers. The most important drivers during our study period were new well development and natural gas price. Permian methane intensity averaged 4.6 % and decreased by 1 % per year.
Ruijun Dang, Daniel J. Jacob, Viral Shah, Sebastian D. Eastham, Thibaud M. Fritz, Loretta J. Mickley, Tianjia Liu, Yi Wang, and Jun Wang
Atmos. Chem. Phys., 23, 6271–6284, https://doi.org/10.5194/acp-23-6271-2023, https://doi.org/10.5194/acp-23-6271-2023, 2023
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We use the GEOS-Chem model to better understand the magnitude and trend in free tropospheric NO2 over the contiguous US. Model underestimate of background NO2 is largely corrected by considering aerosol nitrate photolysis. Increase in aircraft emissions affects satellite retrievals by altering the NO2 shape factor, and this effect is expected to increase in future. We show the importance of properly accounting for the free tropospheric background in interpreting NO2 observations from space.
Zichong Chen, Daniel J. Jacob, Ritesh Gautam, Mark Omara, Robert N. Stavins, Robert C. Stowe, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Drew C. Pendergrass, and Sarah Hancock
Atmos. Chem. Phys., 23, 5945–5967, https://doi.org/10.5194/acp-23-5945-2023, https://doi.org/10.5194/acp-23-5945-2023, 2023
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We quantify methane emissions from individual countries in the Middle East and North Africa by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We show that the ability to simply relate oil/gas emissions to activity metrics is compromised by stochastic nature of local infrastructure and management practices. We find that the industry target for oil/gas methane intensity is achievable through associated gas capture, modern infrastructure, and centralized operations.
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.
Forwood Wiser, Bryan K. Place, Siddhartha Sen, Havala O. T. Pye, Benjamin Yang, Daniel M. Westervelt, Daven K. Henze, Arlene M. Fiore, and V. Faye McNeill
Geosci. Model Dev., 16, 1801–1821, https://doi.org/10.5194/gmd-16-1801-2023, https://doi.org/10.5194/gmd-16-1801-2023, 2023
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We developed a reduced model of atmospheric isoprene oxidation, AMORE-Isoprene 1.0. It was created using a new Automated Model Reduction (AMORE) method designed to simplify complex chemical mechanisms with minimal manual adjustments to the output. AMORE-Isoprene 1.0 has improved accuracy and similar size to other reduced isoprene mechanisms. When included in the CRACMM mechanism, it improved the accuracy of EPA’s CMAQ model predictions for the northeastern USA compared to observations.
Xueying Yu, Dylan B. Millet, Daven K. Henze, Alexander J. Turner, Alba Lorente Delgado, A. Anthony Bloom, and Jianxiong Sheng
Atmos. Chem. Phys., 23, 3325–3346, https://doi.org/10.5194/acp-23-3325-2023, https://doi.org/10.5194/acp-23-3325-2023, 2023
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We combine satellite measurements with a novel downscaling method to map global methane emissions at 0.1°×0.1° resolution. These fine-scale emission estimates reveal unreported emission hotspots and shed light on the roles of agriculture, wetlands, and fossil fuels for regional methane budgets. The satellite-derived emissions point in particular to missing fossil fuel emissions in the Middle East and to a large emission underestimate in South Asia that appears to be tied to monsoon rainfall.
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.
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.
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.
Johannes Quaas, Hailing Jia, Chris Smith, Anna Lea Albright, Wenche Aas, Nicolas Bellouin, Olivier Boucher, Marie Doutriaux-Boucher, Piers M. Forster, Daniel Grosvenor, Stuart Jenkins, Zbigniew Klimont, Norman G. Loeb, Xiaoyan Ma, Vaishali Naik, Fabien Paulot, Philip Stier, Martin Wild, Gunnar Myhre, and Michael Schulz
Atmos. Chem. Phys., 22, 12221–12239, https://doi.org/10.5194/acp-22-12221-2022, https://doi.org/10.5194/acp-22-12221-2022, 2022
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Pollution particles cool climate and offset part of the global warming. However, they are washed out by rain and thus their effect responds quickly to changes in emissions. We show multiple datasets to demonstrate that aerosol emissions and their concentrations declined in many regions influenced by human emissions, as did the effects on clouds. Consequently, the cooling impact on the Earth energy budget became smaller. This change in trend implies a relative warming.
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.
Katherine R. Travis, James H. Crawford, Gao Chen, Carolyn E. Jordan, Benjamin A. Nault, Hwajin Kim, Jose L. Jimenez, Pedro Campuzano-Jost, Jack E. Dibb, Jung-Hun Woo, Younha Kim, Shixian Zhai, Xuan Wang, Erin E. McDuffie, Gan Luo, Fangqun Yu, Saewung Kim, Isobel J. Simpson, Donald R. Blake, Limseok Chang, and Michelle J. Kim
Atmos. Chem. Phys., 22, 7933–7958, https://doi.org/10.5194/acp-22-7933-2022, https://doi.org/10.5194/acp-22-7933-2022, 2022
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The 2016 Korea–United States Air Quality (KORUS-AQ) field campaign provided a unique set of observations to improve our understanding of PM2.5 pollution in South Korea. Models typically have errors in simulating PM2.5 in this region, which is of concern for the development of control measures. We use KORUS-AQ observations to improve our understanding of the mechanisms driving PM2.5 and the implications of model errors for determining PM2.5 that is attributable to local or foreign sources.
Joseph S. Schlosser, Connor Stahl, Armin Sorooshian, Yen Thi-Hoang Le, Ki-Joon Jeon, Peng Xian, Carolyn E. Jordan, Katherine R. Travis, James H. Crawford, Sung Yong Gong, Hye-Jung Shin, In-Ho Song, and Jong-sang Youn
Atmos. Chem. Phys., 22, 7505–7522, https://doi.org/10.5194/acp-22-7505-2022, https://doi.org/10.5194/acp-22-7505-2022, 2022
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During a major haze pollution episode in March 2019, anthropogenic emissions were dominant in the boundary layer over Incheon and Seoul, South Korea. Using supermicrometer and submicrometer size- and chemistry-resolved aerosol particle measurements taken during this haze pollution period, this work shows that local emissions and a shallow boundary layer, enhanced humidity, and low temperature promoted local heterogeneous formation of secondary inorganic and organic aerosol species.
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.
Bruno Debus, Andrew T. Weakley, Satoshi Takahama, Kathryn M. George, Anahita Amiri-Farahani, Bret Schichtel, Scott Copeland, Anthony S. Wexler, and Ann M. Dillner
Atmos. Meas. Tech., 15, 2685–2702, https://doi.org/10.5194/amt-15-2685-2022, https://doi.org/10.5194/amt-15-2685-2022, 2022
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In the US, routine particulate matter composition is measured on samples collected on three types of filter media and analyzed using several techniques. We propose an alternate approach that uses one analytical technique, Fourier transform-infrared spectroscopy (FT-IR), and one filter type to measure the chemical composition of particulate matter in a major US monitoring network. This method could be used to add low-cost sites to the network, fill-in missing data, or for quality control.
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.
James R. Ouimette, William C. Malm, Bret A. Schichtel, Patrick J. Sheridan, Elisabeth Andrews, John A. Ogren, and W. Patrick Arnott
Atmos. Meas. Tech., 15, 655–676, https://doi.org/10.5194/amt-15-655-2022, https://doi.org/10.5194/amt-15-655-2022, 2022
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We show that the low-cost PurpleAir sensor can be characterized as a cell-reciprocal nephelometer. At two very different locations (Mauna Loa Observatory in Hawaii and the Table Mountain rural site in Colorado), the PurpleAir measurements are highly correlated with the submicrometer aerosol scattering coefficient measured by a research-grade integrating nephelometer. These results imply that, with care, PurpleAir data may be used to evaluate climate and air quality models.
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.
Xueying Yu, Dylan B. Millet, and Daven K. Henze
Geosci. Model Dev., 14, 7775–7793, https://doi.org/10.5194/gmd-14-7775-2021, https://doi.org/10.5194/gmd-14-7775-2021, 2021
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We conduct observing system simulation experiments to test how well inverse analyses of high-resolution satellite data from sensors such as TROPOMI can quantify methane emissions. Inversions can improve monthly flux estimates at 25 km even with a spatially biased prior or model transport errors, but results are strongly degraded when both are present. We further evaluate a set of alternate formalisms to overcome limitations of the widely used scale factor approach that arise for missing sources.
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.
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 %.
Cited articles
Bash, J. O., Cooter, E. J., Dennis, R. L., Walker, J. T., and Pleim, J. E.:
Evaluation of a regional air-quality model with bidirectional NH3 exchange coupled
to an agroecosystem model, Biogeosciences, 10, 1635–1645, https://doi.org/10.5194/bg-10-1635-2013, 2013.
Benedict, K. B., Chen, X., Sullivan, A. P., Li, Y., Day, D., Prenni, A. J.,
Levin, E. J. T., Kreidenweis, S. M., Malm, W. C., Schichtel, B. A., and
Collett, J. L.: Atmospheric concentrations and deposition of reactive
nitrogen in Grand Teton National Park, J. Geophys. Res.-Atmos., 118,
11875–11887, https://doi.org/10.1002/2013JD020394, 2013a.
Benedict, K. B., Day, D., Schwandner, F. M., Kreidenweis, S. M., Schichtel, B.,
Malm, W. C., and Collett Jr., J. L.: Observations of atmospheric reactive
nitrogen species in Rocky Mountain National Park and across northern
Colorado, Atmos. Environ., 64, 66–76, https://doi.org/10.1016/j.atmosenv.2012.08.066, 2013b.
Bey, I., Jacob, D. J., Yantosca, R. M., Logan, J. A., Field, B. D., Fiore,
A. M., Li, Q., Liu, H. Y., Mickley, L. J., and Schultz, M. G.: Global
modeling of tropospheric chemistry with assimilated meteorology: Model
description and evaluation, J. Geophys. Res., 106, 23073–23095,
https://doi.org/10.1029/2001JD000807,
2001.
Bobbink, R., Hicks, K., Galloway, J., Spranger, T., Alkemade, R., Ashmore, M.,
Bustamante, M., Cinderby, S., Davidson, E., Dentener, F., Emmett, B.,
Erisman, J.-W., Fenn, M., Gilliam, F., Nordin, A., Pardo, L., and De Vries,
W.: Global assessment of nitrogen deposition effects on terrestrial plant
diversity: a synthesis, Ecol. Appl., 20, 30–59, https://doi.org/10.1890/08-1140.1, 2010.
Bouwman, A. F., Lee, D. S., Asman, W. a. H., Dentener, F. J., Van Der Hoek,
K. W., and Olivier, J. G. J.: A global high-resolution emission inventory for
ammonia, Global Biogeochem. Cy., 11, 561–587, https://doi.org/10.1029/97GB02266, 1997.
Bowman, W. D., Murgel, J., Blett, T., and Porter, E.: Nitrogen critical loads
for alpine vegetation and soils in Rocky Mountain National Park, J. Environ.
Manage., 103, 165–171, https://doi.org/10.1016/j.jenvman.2012.03.002, 2012.
CASTNET: U.S. Environmental Protection Agency Clean Air Markets Division Clean
Air Status and Trends Network (CASTNET) Data table accessed (NH4, NO3, HNO3
Weekly Dry Deposition), available at: www.epa.gov/castnet, last access: 9
November 2014.
Chen, D., Wang, Y., McElroy, M. B., He, K., Yantosca, R. M., and Le Sager, P.:
Regional CO pollution and export in China simulated by the high-resolution
nested-grid GEOS-Chem model, Atmos. Chem. Phys., 9, 3825–3839, https://doi.org/10.5194/acp-9-3825-2009, 2009.
Clark, C. M., Morefield, P. E., Gilliam, F. S., and Pardo, L. H.: Estimated
losses of plant biodiversity in the United States from historical N
deposition (1985–2010), Ecology, 94, 1441–1448, https://doi.org/10.1890/12-2016.1, 2013.
Cooter, E. J., Bash, J. O., Walker, J. T., Jones, M. R., and Robarge, W.:
Estimation of NH3 bi-directional flux from managed agricultural soils,
Atmos. Environ., 44, 2107–2115,
https://doi.org/10.1016/j.atmosenv.2010.02.044, 2010.
Cornell, S. E.: Atmospheric nitrogen deposition: Revisiting the question of
the importance of the organic component, Environ. Pollut., 159, 2214–2222,
https://doi.org/10.1016/j.envpol.2010.11.014, 2011.
Du, E., Vries, W. D., Galloway, J. N., Hu, X., and Fang, J.: Changes in wet
nitrogen deposition in the United States between 1985 and 2012, Environ.
Res. Lett., 9, 095004, https://doi.org/10.1088/1748-9326/9/9/095004, 2014.
Duce, R. A., LaRoche, J., Altieri, K., Arrigo, K. R., Baker, A. R., Capone,
D. G., Cornell, S., Dentener, F., Galloway, J., Ganeshram, R. S., Geider,
R. J., Jickells, T., Kuypers, M. M., Langlois, R., Liss, P. S., Liu, S. M.,
Middelburg, J. J., Moore, C. M., Nickovic, S., Oschlies, A., Pedersen, T.,
Prospero, J., Schlitzer, R., Seitzinger, S., Sorensen, L. L., Uematsu, M.,
Ulloa, O., Voss, M., Ward, B., and Zamora, L.: Impacts of Atmospheric
Anthropogenic Nitrogen on the Open Ocean, Science, 320, 893–897,
https://doi.org/10.1126/science.1150369, 2008.
Ellis, R. A., Jacob, D. J., Sulprizio, M. P., Zhang, L., Holmes, C. D.,
Schichtel, B. A., Blett, T., Porter, E., Pardo, L. H., and Lynch, J. A.:
Present and future nitrogen deposition to national parks in the United
States: critical load exceedances, Atmos. Chem. Phys., 13, 9083–9095, https://doi.org/10.5194/acp-13-9083-2013, 2013.
Fenn, M. E., Baron, J. S., Allen, E. B., Rueth, H. M., Nydick, K. R., Geiser,
L., Bowman, W. D., Sickman, J. O., Meixner, T., Johnson, D. W., and Neitlich,
P.: Ecological Effects of Nitrogen Deposition in the Western United States,
BioScience, 53, 404–420,
https://doi.org/10.1641/0006-3568(2003)053[0404:EEONDI]2.0.CO;2, 2003.
Fenn, M. E., Allen, E. B., Weiss, S. B., Jovan, S., Geiser, L. H., Tonnesen,
G. S., Johnson, R. F., Rao, L. E., Gimeno, B. S., Yuan, F., Meixner, T., and
Bytnerowicz, A.: Nitrogen critical loads and management alternatives for
N-impacted ecosystems in California, J. Environ. Manage., 91, 2404–2423,
https://doi.org/10.1016/j.jenvman.2010.07.034, 2010.
Galloway, J. N., Aber, J. D., Erisman, J. W., Seitzinger, S. P., Howarth,
R. W., Cowling, E. B., and Cosby, B. J.: The nitrogen cascade, BioScience,
53, 341–356, https://doi.org/10.1641/0006-3568(2003)053[0341:TNC]2.0.CO;2, 2003.
Gilliland, A. B., Dennis, R. L., Roselle, S. J., and Pierce, T. E.: Seasonal
NH3 emission estimates for the eastern United States based on ammonium
wet concentrations and an inverse modeling method, J. Geophys. Res., 108,
4477, https://doi.org/10.1029/2002JD003063, 2003.
Gilliland, A. B., Wyat Appel, K., Pinder, R. W., and Dennis, R. L.: Seasonal
NH3 emissions for the continental united states: Inverse model estimation
and evaluation, Atmos. Environ., 40, 4986–4998,
https://doi.org/10.1016/j.atmosenv.2005.12.066, 2006.
Gruber, N. and Galloway, J. N.: An Earth-system perspective of the global
nitrogen cycle, Nature, 451, 293–296, https://doi.org/10.1038/nature06592, 2008.
Heald, C. L., Collett Jr., J. L., Lee, T., Benedict, K. B., Schwandner, F. M., Li, Y.,
Clarisse, L., Hurtmans, D. R., Van Damme, M., Clerbaux, C., Coheur, P.-F.,
Philip, S., Martin, R. V., and Pye, H. O. T.: Atmospheric ammonia and
particulate inorganic nitrogen over the United States, Atmos. Chem. Phys., 12, 10295–10312, https://doi.org/10.5194/acp-12-10295-2012, 2012.
Henze, D. K., Hakami, A., and Seinfeld, J. H.: Development of the adjoint
of GEOS-Chem, Atmos. Chem. Phys., 7, 2413–2433, https://doi.org/10.5194/acp-7-2413-2007, 2007.
Henze, D. K., Seinfeld, J. H., and Shindell, D. T.: Inverse modeling and mapping
US air quality influences of inorganic PM2.5 precursor emissions using
the adjoint of GEOS-Chem, Atmos. Chem. Phys., 9, 5877–5903, https://doi.org/10.5194/acp-9-5877-2009, 2009.
Hicks, B. B.: Dry deposition to forests – On the use of data from clearings,
Agric. Forest Meteorol., 136, 214–221,
https://doi.org/10.1016/j.agrformet.2004.06.013, 2006.
Hudman, R. C., Jacob, D. J., Turquety, S., Leibensperger, E. M., Murray, L. T.,
Wu, S., Gilliland, A. B., Avery, M., Bertram, T. H., Brune, W., Cohen, R. C.,
Dibb, J. E., Flocke, F. M., Fried, A., Holloway, J., Neuman, J. A., Orville,
R., Perring, A., Ren, X., Sachse, G. W., Singh, H. B., Swanson, A., and
Wooldridge, P. J.: Surface and lightning sources of nitrogen oxides over the United States:
Magnitudes, chemical evolution, and outflow, J. Geophys. Res., 112, D12S05, https://doi.org/10.1029/2006JD007912, 2007.
Kean, A. J., Littlejohn, D., Ban-Weiss, G. A., Harley, R. A., Kirchstetter,
T. W., and Lunden, M. M.: Trends in on-road vehicle emissions of ammonia,
Atmos. Environ., 43, 1565–1570, https://doi.org/10.1016/j.atmosenv.2008.09.085, 2009.
Kopacz, M., Jacob, D. J., Henze, D. K., Heald, C. L., Streets, D. G., and
Zhang, Q.: Comparison of adjoint and analytical Bayesian inversion methods
for constraining Asian sources of carbon monoxide using satellite (MOPITT)
measurements of CO columns, J. Geophys. Res., 114, D04305,
https://doi.org/10.1029/2007JD009264,
2009.
Lapina, K., Henze, D. K., Milford, J. B., Huang, M., Lin, M., Fiore, A. M.,
Carmichael, G., Pfister, G. G., and Bowman, K.: Assessment of source
contributions to seasonal vegetative exposure to ozone in the U.S., J. Geophys. Res.-Atmos., 119, 324–340, https://doi.org/10.1002/2013JD020905, 2014.
Lee, H.-M., Henze, D. K., Alexander, B., and Murray, L. T.: Investigating the
sensitivity of surface-level nitrate seasonality in Antarctica to primary
sources using a global model, Atmos. Environ., 89, 757–767,
https://doi.org/10.1016/j.atmosenv.2014.03.003, 2014.
Liu, H., Jacob, D. J., Bey, I., and Yantosca, R. M.: Constraints from 210Pb
and 7Be on wet deposition and transport in a global three-dimensional
chemical tracer model driven by assimilated meteorological fields, J. Geophys. Res.-Atmos., 106, 12109–12128, https://doi.org/10.1029/2000JD900839, 2001.
Malm, W. C., Schichtel, B. A., Barna, M. G., Gebhart, K. A., Rodriguez, M. A.,
Jr, J. L. C., Carrico, C. M., Benedict, K. B., Prenni, A. J., and
Kreidenweis, S. M.: Aerosol species concentrations and source apportionment
of ammonia at Rocky Mountain National Park, J. Air Waste Manage., 63,
1245–1263, https://doi.org/10.1080/10962247.2013.804466, 2013.
Mu, M., Randerson, J. T., van der Werf, G. R., Giglio, L., Kasibhatla, P.,
Morton, D., Collatz, G. J., DeFries, R. S., Hyer, E. J., Prins, E. M.,
Griffith, D. W. T., Wunch, D., Toon, G. C., Sherlock, V., and Wennberg,
P. O.: Daily and 3-hourly variability in global fire emissions and
consequences for atmospheric model predictions of carbon monoxide, J.
Geophys. Res., 116, D24303, https://doi.org/10.1029/2011JD016245, 2011.
Murray, L. T., Jacob, D. J., Logan, J. A., Hudman, R. C., and Koshak, W. J.:
Optimized regional and interannual variability of lightning in a global chemical transport
model constrained by LIS/OTD satellite data, J. Geophys. Res., 117, D20307, https://doi.org/10.1029/2012JD017934, 2012.
NADP: National Atmospheric Deposition Program (NRSP-3), NADP Program Office,
Illinois State Water Survey, 2204 Griffith Dr., Champaign, IL 61820, 2015.
Neff, J. C., Holland, E. A., Dentener, F. J., McDowell, W. H., and Russell,
K. M.: The origin, composition and rates of organic nitrogen deposition: A
missing piece of the nitrogen cycle?, Biogeochemistry, 57–58, 99–136,
https://doi.org/10.1023/A:1015791622742,
2002.
Nemitz, E., Milford, C., and Sutton, M. A.: A two-layer canopy compensation
point model for describing bi-directional biosphere-atmosphere exchange of
ammonia, Q. J. Roy. Meteorol. Soc., 127, 815–833, https://doi.org/10.1002/qj.49712757306, 2001.
Nilsson, J.: Critical Loads for Sulphur and Nitrogen, in: Air Pollution and
Ecosystems, edited by: Mathy, P., p. 85–91, Springer Netherlands,
available at: http://link.springer.com/chapter/10.1007/978-94-009-4003-1_11% (last access: 1 September 2014), 1988.
Olson, J. S.: Digital raster data on a 10 minute geographic 1080 × 2160 grid in
Global Ecosystems Database, version 1.0, Disc A, edited by: NOAA Natl.
Geophys. Data Center, Boulder, Colorado, 1992.
Pardo, L. H., Fenn, M. E., Goodale, C. L., Geiser, L. H., Driscoll, C. T.,
Allen, E. B., Baron, J. S., Bobbink, R., Bowman, W. D., Clark, C. M., Emmett,
B., Gilliam, F. S., Greaver, T. L., Hall, S. J., Lilleskov, E. A., Liu, L.,
Lynch, J. A., Nadelhoffer, K. J., Perakis, S. S., Robin-Abbott, M. J.,
Stoddard, J. L., Weathers, K. C., and Dennis, R. L.: Effects of nitrogen
deposition and empirical nitrogen critical loads for ecoregions of the United
States, Ecol. Appl., 21, 3049–3082, https://doi.org/10.1890/10-2341.1, 2011.
Park, R. J., Jacob, D. J., Field, B. D., Yantosca, R. M., and Chin, M.:
Natural and transboundary pollution influences on sulfate-nitrate-ammonium aerosols
in the United States: Implications for policy, J. Geophys. Res., 109, D15204, https://doi.org/10.1029/2003JD004473,
2004.
Paulot, F., Jacob, D. J., and Henze, D. K.: Sources and processes contributing
to nitrogen deposition: an adjoint model analysis applied to biodiversity
hotspots worldwide, Environ. Sci. Technol., 47, 3226–3233,
https://doi.org/10.1021/es3027727,
2013.
Paulot, F., Jacob, D. J., Pinder, R. W., Bash, J. O., Travis, K., and Henze,
D. K.: Ammonia emissions in the United States, European Union, and China
derived by high-resolution inversion of ammonium wet deposition data:
Interpretation with a new agricultural emissions inventory (MASAGE_NH3),
J. Geophys. Res.-Atmos., 119, 4343–4364, https://doi.org/10.1002/2013JD021130, 2014.
Pleim, J. E., Bash, J. O., Walker, J. T., and Cooter, E. J.: Development and
evaluation of an ammonia bidirectional flux parameterization for air quality
models, J. Geophys. Res.-Atmos., 118, 3794–3806, https://doi.org/10.1002/jgrd.50262, 2013.
Reay, D. S., Dentener, F., Smith, P., Grace, J., and Feely, R. A.: Global
nitrogen deposition and carbon sinks, Nature Geosci., 1, 430–437,
https://doi.org/10.1038/ngeo230,
2008.
Sala, O. E., Chapin, F. S., Iii, Armesto, J. J., Berlow, E., Bloomfield, J.,
Dirzo, R., Huber-Sanwald, E., Huenneke, L. F., Jackson, R. B., Kinzig, A.,
Leemans, R., Lodge, D. M., Mooney, H. A., Oesterheld, M., Poff, N. L., Sykes,
M. T., Walker, B. H., Walker, M., and Wall, D. H.: Global biodiversity
scenarios for the year 2100, Science, 287, 1770–1774,
https://doi.org/10.1126/science.287.5459.1770, 2000.
Saylor, R. D., Wolfe, G. M., Meyers, T. P., and Hicks, B. B.: A corrected
formulation of the Multilayer Model (MLM) for inferring gaseous dry
deposition to vegetated surfaces, Atmos. Environ., 92, 141–145,
https://doi.org/10.1016/j.atmosenv.2014.03.056, 2014.
Schwede, D. B. and Lear, G. G.: A novel hybrid approach for estimating total
deposition in the United States, Atmos. Environ., 92, 207–220,
https://doi.org/10.1016/j.atmosenv.2014.04.008, 2014.
Schwede, D., Zhang, L., Vet, R., and Lear, G.: An intercomparison of the
deposition models used in the CASTNET and CAPMoN networks, Atmos.
Environ., 45, 1337–1346, https://doi.org/10.1016/j.atmosenv.2010.11.050, 2011.
Shephard, M. W., Cady-Pereira, K. E., Luo, M., Henze, D. K., Pinder, R. W., Walker, J. T.,
Rinsland, C. P., Bash, J. O., Zhu, L., Payne, V. H., and Clarisse, L.:
TES ammonia retrieval strategy and global observations of the
spatial and seasonal variability of ammonia, Atmos. Chem. Phys., 11, 10743–10763, https://doi.org/10.5194/acp-11-10743-2011, 2011.
Stevens, C. J., Dise, N. B., Mountford, J. O., and Gowing, D. J.: Impact of
nitrogen deposition on the species richness of grasslands, Science, 303,
1876–1879, https://doi.org/10.1126/science.1094678, 2004.
Sullivan, T. J., Cosby, B. J., Tonnessen, K. A., and Clow, D. W.: Surface water
acidification responses and critical loads of sulfur and nitrogen deposition
in Loch Vale watershed, Colorado, Water Resour. Res., 41, W01021,
https://doi.org/10.1029/2004WR003414, 2005.
Sutton, M. A., Nemitz, E., Erisman, J. W., Beier, C., Bahl, K. B., Cellier, P.,
de Vries, W., Cotrufo, F., Skiba, U., Di Marco, C., Jones, S., Laville, P.,
Soussana, J. F., Loubet, B., Twigg, M., Famulari, D., Whitehead, J.,
Gallagher, M. W., Neftel, A., Flechard, C. R., Herrmann, B., Calanca, P. L.,
Schjoerring, J. K., Daemmgen, U., Horvath, L., Tang, Y. S., Emmett, B. A.,
Tietema, A., Peñuelas, J., Kesik, M., Brueggemann, N., Pilegaard, K.,
Vesala, T., Campbell, C. L., Olesen, J. E., Dragosits, U., Theobald, M. R.,
Levy, P., Mobbs, D. C., Milne, R., Viovy, N., Vuichard, N., Smith, J. U.,
Smith, P., Bergamaschi, P., Fowler, D., and Reis, S.: Challenges in
quantifying biosphere–atmosphere exchange of nitrogen species, Environ.
Pollut., 150, 125–139, https://doi.org/10.1016/j.envpol.2007.04.014, 2007.
Thompson, T. M., Rodriguez, M. A., Barna, M. G., Gebhart, K. A., Hand, J. L.,
Day, D. E., Malm, W. C., Benedict, K. B., Collett, J. L., and Schichtel,
B. A.: Rocky Mountain National Park reduced nitrogen source
apportionment: RMNP NITROGEN SOURCE APPORTIONMENT, J. Geophys. Res.-Atmos., 120, 4370–4384, https://doi.org/10.1002/2014JD022675, 2015.
UBA: Manual on methodologies and criteria for mapping critical levels/loads and
geographical areas where they are exceeded, Federal Environmental Agency
(UmweltBundesAmt),
available at: http://www.rivm.nl/en/themasites/icpmm/manual-and-downloads/m%
anual-english/index.html (last access: 19 May 2015), 2004.
van der Werf, G. R., Randerson, J. T., Giglio, L., Collatz, G. J., Mu, M.,
Kasibhatla, P. S., Morton, D. C., DeFries, R. S., Jin, Y., and van Leeuwen, T. T.:
Global fire emissions and the contribution of deforestation, savanna, forest, agricultural,
and peat fires (1997–2009), Atmos. Chem. Phys., 10, 11707–11735, https://doi.org/10.5194/acp-10-11707-2010,
2010.
Vitousek, P. M., Aber, J. D., Howarth, R. W., Likens, G. E., Matson, P. A.,
Schindler, D. W., Schlesinger, W. H., and Tilman, D. G.: Human alteration
of the global nitrogen cycle: sources and consequences, Ecol.
Appl., 7, 737–750, https://doi.org/10.1890/1051-0761(1997)007[0737:HAOTGN]2.0.CO;2, 1997.
Vries, W. D., Wamelink, G. W. W., Dobben, H. v., Kros, J., Reinds, G. J.,
Mol-Dijkstra, J. P., Smart, S. M., Evans, C. D., Rowe, E. C., Belyazid, S.,
Sverdrup, H. U., Hinsberg, A. v., Posch, M., Hettelingh, J.-P., Spranger, T.,
and Bobbink, R.: Use of dynamic soil–vegetation models to assess impacts of
nitrogen deposition on plant species composition: an overview, Ecol. Appl.,
20, 60–79, https://doi.org/10.1890/08-1019.1, 2010.
Walker, T. W., Jones, D. B. A., Parrington, M., Henze, D. K., Murray, L. T.,
Bottenheim, J. W., Anlauf, K., Worden, J. R., Bowman, K. W., Shim, C., Singh,
K., Kopacz, M., Tarasick, D. W., Davies, J., Gathen, P. v. d., Thompson,
A. M., and Carouge, C. C.: Impacts of midlatitude precursor emissions and
local photochemistry on ozone abundances in the Arctic, J. Geophys. Res.,
117, D01305, https://doi.org/10.1029/2011JD016370,
2012.
Wang, Y., Jacob, D. J., and Logan, J. A.: Global simulation of tropospheric
O3-NOx-hydrocarbon chemistry 3. Origin of tropospheric ozone and
effects of nonmethane hydrocarbons, J. Geophys. Res., 103, 10757–10767,
https://doi.org/10.1029/98JD00156, 1998.
Wang, Y. X., McElroy, M. B., Jacob, D. J., and Yantosca, R. M.: A nested grid
formulation for chemical transport over Asia: Applications to CO, J.
Geophys. Res., 109, D22307, https://doi.org/10.1029/2004JD005237, 2004.
Wecht, K. J., Jacob, D. J., Wofsy, S. C., Kort, E. A., Worden, J. R., Kulawik, S. S.,
Henze, D. K., Kopacz, M., and Payne, V. H.: Validation of TES methane with HIPPO aircraft
observations: implications for inverse modeling of methane sources, Atmos. Chem. Phys., 12, 1823–1832, https://doi.org/10.5194/acp-12-1823-2012, 2012.
Wesely, M.: Parameterization of surface resistances to gaseous dry deposition
in regional-scale numerical models, Atmos. Environ. (1967), 23, 1293–1304,
https://doi.org/10.1016/0004-6981(89)90153-4, 1989.
Yienger, J. J. and Levy, H.: Empirical model of global soil-biogenic NOx
emissions, J. Geophys. Res., 100, 11447–11464, https://doi.org/10.1029/95JD00370, 1995.
Zhang, L., Jacob, D. J., Downey, N. V., Wood, D. A., Blewitt, D., Carouge,
C. C., van Donkelaar, A., Jones, D. B. A., Murray, L. T., and Wang, Y.:
Improved estimate of the policy-relevant background ozone in the United
States using the GEOS-Chem global model with 1/2°–2/3° horizontal resolution over North America, Atmos. Environ.,
45, 6769–6776, https://doi.org/10.1016/j.atmosenv.2011.07.054, 2011.
Zhang, L., Jacob, D. J., Knipping, E. M., Kumar, N., Munger, J. W., Carouge, C. C.,
van Donkelaar, A., Wang, Y. X., and Chen, D.: Nitrogen deposition to the
United States: distribution, sources, and processes, Atmos. Chem. Phys., 12, 4539–4554, https://doi.org/10.5194/acp-12-4539-2012, 2012.
Zhu, L., Henze, D. K., Cady-Pereira, K. E., Shephard, M. W., Luo, M., Pinder,
R. W., Bash, J. O., and Jeong, G.-R.: Constraining U.S. ammonia emissions
using TES remote sensing observations and the GEOS-Chem adjoint model, J. Geophys. Res.-Atmos., 118, 3355–3368, https://doi.org/10.1002/jgrd.50166, 2013.
Zhu, L., Henze, D., Bash, J., Jeong, G.-R., Cady-Pereira, K., Shephard, M., Luo, M.,
Paulot, F., and Capps, S.: Global evaluation of ammonia bidirectional exchange
and livestock diurnal variation schemes, Atmos. Chem. Phys., 15, 12823–12843, https://doi.org/10.5194/acp-15-12823-2015,
2015.
Short summary
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.
Sources of nitrogen deposition (Ndep) in Federal Class I areas in the US are investigated,...
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