Articles | Volume 20, issue 21
https://doi.org/10.5194/acp-20-13109-2020
© Author(s) 2020. 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-20-13109-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
09 Nov 2020
Research article |
| 09 Nov 2020
| 09 Nov 2020
Impacts of global NOx inversions on NO2 and ozone simulations
Department of Mechanical Engineering, University of Colorado Boulder,
Boulder, CO 80309, USA
School of Engineering and Applied Science, Harvard University,
Cambridge, MA 02138, USA
Daven K. Henze
Department of Mechanical Engineering, University of Colorado Boulder,
Boulder, CO 80309, USA
Owen R. Cooper
Cooperative Institute for Research in Environmental Sciences,
University of Colorado Boulder, Boulder, CO 80309, USA
NOAA Chemical Sciences Laboratory, Boulder, CO 80305, USA
Jessica L. Neu
Jet Propulsion Laboratory, California Institute of Technology,
Pasadena, CA 91109, USA
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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
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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.
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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.
Vijay Natraj, Ming Luo, Jean-Francois Blavier, Vivienne H. Payne, Derek J. Posselt, Stanley P. Sander, Zhao-Cheng Zeng, Jessica L. Neu, Denis Tremblay, Longtao Wu, Jacola A. Roman, Yen-Hung Wu, and Leonard I. Dorsky
Atmos. Meas. Tech., 15, 1251–1267, https://doi.org/10.5194/amt-15-1251-2022, https://doi.org/10.5194/amt-15-1251-2022, 2022
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High-fidelity monitoring and forecast of air quality and the hydrological cycle require understanding the vertical distribution of temperature, humidity, and trace gases at high spatiotemporal resolution. We describe a new instrument concept, called the JPL GEO-IR Sounder, that would provide this information for the first time from a single instrument platform. Simulations demonstrate the benefits of combining measurements from multiple wavelengths for this purpose from geostationary orbit.
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.
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.
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.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Ilya Stanevich, Dylan B. A. Jones, Kimberly Strong, Martin Keller, Daven K. Henze, Robert J. Parker, Hartmut Boesch, Debra Wunch, Justus Notholt, Christof Petri, Thorsten Warneke, Ralf Sussmann, Matthias Schneider, Frank Hase, Rigel Kivi, Nicholas M. Deutscher, Voltaire A. Velazco, Kaley A. Walker, and Feng Deng
Atmos. Chem. Phys., 21, 9545–9572, https://doi.org/10.5194/acp-21-9545-2021, https://doi.org/10.5194/acp-21-9545-2021, 2021
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We explore the utility of a weak-constraint (WC) four-dimensional variational (4D-Var) data assimilation scheme for mitigating systematic errors in methane simulation in the GEOS-Chem model. We use data from the Greenhouse Gases Observing Satellite (GOSAT) and show that, compared to the traditional 4D-Var approach, the WC scheme improves the agreement between the model and independent observations. We find that the WC corrections to the model provide insight into the source of the errors.
Na Zhao, Xinyi Dong, Kan Huang, Joshua S. Fu, Marianne Tronstad Lund, Kengo Sudo, Daven Henze, Tom Kucsera, Yun Fat Lam, Mian Chin, and Simone Tilmes
Atmos. Chem. Phys., 21, 8637–8654, https://doi.org/10.5194/acp-21-8637-2021, https://doi.org/10.5194/acp-21-8637-2021, 2021
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Black carbon acts as a strong climate forcer, especially in vulnerable pristine regions such as the Arctic. This work utilizes ensemble modeling results from the task force Hemispheric Transport of Air Pollution Phase 2 to investigate the responses of Arctic black carbon and surface temperature to various source emission reductions. East Asia contributed the most to Arctic black carbon. The response of Arctic temperature to black carbon was substantially more sensitive than the global average.
Michaela I. Hegglin, Susann Tegtmeier, John Anderson, Adam E. Bourassa, Samuel Brohede, Doug Degenstein, Lucien Froidevaux, Bernd Funke, John Gille, Yasuko Kasai, Erkki T. Kyrölä, Jerry Lumpe, Donal Murtagh, Jessica L. Neu, Kristell Pérot, Ellis E. Remsberg, Alexei Rozanov, Matthew Toohey, Joachim Urban, Thomas von Clarmann, Kaley A. Walker, Hsiang-Jui Wang, Carlo Arosio, Robert Damadeo, Ryan A. Fuller, Gretchen Lingenfelser, Christopher McLinden, Diane Pendlebury, Chris Roth, Niall J. Ryan, Christopher Sioris, Lesley Smith, and Katja Weigel
Earth Syst. Sci. Data, 13, 1855–1903, https://doi.org/10.5194/essd-13-1855-2021, https://doi.org/10.5194/essd-13-1855-2021, 2021
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An overview of the SPARC Data Initiative is presented, to date the most comprehensive assessment of stratospheric composition measurements spanning 1979–2018. Measurements of 26 chemical constituents obtained from an international suite of space-based limb sounders were compiled into vertically resolved, zonal monthly mean time series. The quality and consistency of these gridded datasets are then evaluated using a climatological validation approach and a range of diagnostics.
Zichong Chen, Junjie Liu, Daven K. Henze, Deborah N. Huntzinger, Kelley C. Wells, Stephen Sitch, Pierre Friedlingstein, Emilie Joetzjer, Vladislav Bastrikov, Daniel S. Goll, Vanessa Haverd, Atul K. Jain, Etsushi Kato, Sebastian Lienert, Danica L. Lombardozzi, Patrick C. McGuire, Joe R. Melton, Julia E. M. S. Nabel, Benjamin Poulter, Hanqin Tian, Andrew J. Wiltshire, Sönke Zaehle, and Scot M. Miller
Atmos. Chem. Phys., 21, 6663–6680, https://doi.org/10.5194/acp-21-6663-2021, https://doi.org/10.5194/acp-21-6663-2021, 2021
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NASA's Orbiting Carbon Observatory 2 (OCO-2) satellite observes atmospheric CO2 globally. We use a multiple regression and inverse model to quantify the relationships between OCO-2 and environmental drivers within individual years for 2015–2018 and within seven global biomes. Our results point to limitations of current space-based observations for inferring environmental relationships but also indicate the potential to inform key relationships that are very uncertain in process-based models.
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.
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.
Yilin Chen, Huizhong Shen, Jennifer Kaiser, Yongtao Hu, Shannon L. Capps, Shunliu Zhao, Amir Hakami, Jhih-Shyang Shih, Gertrude K. Pavur, Matthew D. Turner, Daven K. Henze, Jaroslav Resler, Athanasios Nenes, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Tianfeng Chai, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, and Armistead G. Russell
Atmos. Chem. Phys., 21, 2067–2082, https://doi.org/10.5194/acp-21-2067-2021, https://doi.org/10.5194/acp-21-2067-2021, 2021
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Ammonia (NH3) emissions can exert adverse impacts on air quality and ecosystem well-being. NH3 emission inventories are viewed as highly uncertain. Here we optimize the NH3 emission estimates in the US using an air quality model and NH3 measurements from the IASI satellite instruments. The optimized NH3 emissions are much higher than the National Emissions Inventory estimates in April. The optimized NH3 emissions improved model performance when evaluated against independent observation.
Xueying Yu, Dylan B. Millet, Kelley C. Wells, Daven K. Henze, Hansen Cao, Timothy J. Griffis, Eric A. Kort, Genevieve Plant, Malte J. Deventer, Randall K. Kolka, D. Tyler Roman, Kenneth J. Davis, Ankur R. Desai, Bianca C. Baier, Kathryn McKain, Alan C. Czarnetzki, and A. Anthony Bloom
Atmos. Chem. Phys., 21, 951–971, https://doi.org/10.5194/acp-21-951-2021, https://doi.org/10.5194/acp-21-951-2021, 2021
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Methane concentrations have doubled since 1750. The US Upper Midwest is a key region contributing to such trends, but sources are poorly understood. We collected and analyzed aircraft data to resolve spatial and timing biases in wetland and livestock emission estimates and uncover errors in inventory treatment of manure management. We highlight the importance of intensive agriculture for the regional and US methane budgets and the potential for methane mitigation through improved management.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
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This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
Kai-Lan Chang, Owen R. Cooper, Audrey Gaudel, Irina Petropavlovskikh, and Valérie Thouret
Atmos. Chem. Phys., 20, 9915–9938, https://doi.org/10.5194/acp-20-9915-2020, https://doi.org/10.5194/acp-20-9915-2020, 2020
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We provide a statistical framework for detecting trends of multiple autocorrelated time series from sparsely sampled profile data. The result is a better and more consistent quantification of trend estimates of vertical profile data. The focus was placed on the long-term ozone time series from commercial aircraft and balloon-borne ozonesonde measurements. This framework can be applied to other trace gases in the atmosphere.
Shunliu Zhao, Matthew G. Russell, Amir Hakami, Shannon L. Capps, Matthew D. Turner, Daven K. Henze, Peter B. Percell, Jaroslav Resler, Huizhong Shen, Armistead G. Russell, Athanasios Nenes, Amanda J. Pappin, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Charles O. Stanier, and Tianfeng Chai
Geosci. Model Dev., 13, 2925–2944, https://doi.org/10.5194/gmd-13-2925-2020, https://doi.org/10.5194/gmd-13-2925-2020, 2020
Matthew J. Cooper, Randall V. Martin, Daven K. Henze, and Dylan B. A. Jones
Atmos. Chem. Phys., 20, 7231–7241, https://doi.org/10.5194/acp-20-7231-2020, https://doi.org/10.5194/acp-20-7231-2020, 2020
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Comparisons between satellite-retrieved and model-simulated NO2 columns are affected by differences between the model vertical profile and the assumed profile used in the retrieval process. We examine how such differences impact NOx emission estimates from satellite observations. Larger differences between the simulated and assumed profile shape correspond to larger emission errors. This reveals the importance of using consistent profile information when comparing satellite columns to models.
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.
Sojin Lee, Chul Han Song, Kyung Man Han, Daven K. Henze, Kyunghwa Lee, Jinhyeok Yu, Jung-Hun Woo, Jia Jung, Yunsoo Choi, Pablo E. Saide, and Gregory R. Carmichael
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-116, https://doi.org/10.5194/gmd-2020-116, 2020
Revised manuscript not accepted
Cheng Chen, Oleg Dubovik, Daven K. Henze, Mian Chin, Tatyana Lapyonok, Gregory L. Schuster, Fabrice Ducos, David Fuertes, Pavel Litvinov, Lei Li, Anton Lopatin, Qiaoyun Hu, and Benjamin Torres
Atmos. Chem. Phys., 19, 14585–14606, https://doi.org/10.5194/acp-19-14585-2019, https://doi.org/10.5194/acp-19-14585-2019, 2019
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Global BC, OC and DD aerosol emissions are inverted from POLDER/PARASOL observations for the year 2010 based on the GEOS-Chem inverse modeling framework. The retrieved emissions are 18.4 Tg yr−1 BC, 109.9 Tg yr−1 OC and 731.6 Tg yr−1 DD, which indicate an increase of 166.7 % for BC and 184.0 % for OC, while a decrease of 42.4 % for DD with respect to GEOS-Chem a priori emission inventories is seen. Global annul mean AOD and AAOD resulting from retrieved emissions are 0.119 and 0.0071 at 550 nm.
Sajeev Philip, Matthew S. Johnson, Christopher Potter, Vanessa Genovesse, David F. Baker, Katherine D. Haynes, Daven K. Henze, Junjie Liu, and Benjamin Poulter
Atmos. Chem. Phys., 19, 13267–13287, https://doi.org/10.5194/acp-19-13267-2019, https://doi.org/10.5194/acp-19-13267-2019, 2019
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This research was conducted to quantify the impact of different prior global biosphere models on the estimate of terrestrial CO2 fluxes when assimilating Orbiting Carbon Observatory-2 (OCO-2) satellite observations. To determine the prior model impact, we apply observing system simulation experiments (OSSEs). Even with the substantial spatiotemporal coverage of OCO-2 data, residual differences in posterior CO2 flux estimates remain due to the choice of prior flux mean and uncertainties.
Zainab Q. Hakim, Scott Archer-Nicholls, Gufran Beig, Gerd A. Folberth, Kengo Sudo, Nathan Luke Abraham, Sachin Ghude, Daven K. Henze, and Alexander T. Archibald
Atmos. Chem. Phys., 19, 6437–6458, https://doi.org/10.5194/acp-19-6437-2019, https://doi.org/10.5194/acp-19-6437-2019, 2019
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Surface ozone is an important air pollutant and recent work has calculated that large numbers of people die prematurely because of exposure to high levels of surface ozone in India. However, these calculations require model simulations of ozone as key inputs.
Here we perform the most thorough evaluation of global model surface ozone over India to date. These analyses of model simulations and observations highlight some successes and shortcomings and the need for further process-based studies.
Marianna Linz, Marta Abalos, Anne Sasha Glanville, Douglas E. Kinnison, Alison Ming, and Jessica L. Neu
Atmos. Chem. Phys., 19, 5069–5090, https://doi.org/10.5194/acp-19-5069-2019, https://doi.org/10.5194/acp-19-5069-2019, 2019
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The stratospheric circulation is important for transporting ozone and water vapor, and models of the stratosphere differ. The metrics used to compare models are inconsistent between studies and cannot be calculated from observational data. In this paper, we explore a metric for the circulation that can be calculated from observations and examine how it relates to the more commonly used metrics. We find substantial differences in the upper and lower stratosphere depending on the choice of metric.
Kai-Lan Chang, Owen R. Cooper, J. Jason West, Marc L. Serre, Martin G. Schultz, Meiyun Lin, Virginie Marécal, Béatrice Josse, Makoto Deushi, Kengo Sudo, Junhua Liu, and Christoph A. Keller
Geosci. Model Dev., 12, 955–978, https://doi.org/10.5194/gmd-12-955-2019, https://doi.org/10.5194/gmd-12-955-2019, 2019
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We developed a new method for combining surface ozone observations from thousands of monitoring sites worldwide with the output from multiple atmospheric chemistry models. The result is a global surface ozone distribution with greater accuracy than any single model can achieve. We focused on an ozone metric relevant to human mortality caused by long-term ozone exposure. Our method can be applied to studies that quantify the impacts of ozone on human health and mortality.
Xinyi Dong, Joshua S. Fu, Qingzhao Zhu, Jian Sun, Jiani Tan, Terry Keating, Takashi Sekiya, Kengo Sudo, Louisa Emmons, Simone Tilmes, Jan Eiof Jonson, Michael Schulz, Huisheng Bian, Mian Chin, Yanko Davila, Daven Henze, Toshihiko Takemura, Anna Maria Katarina Benedictow, and Kan Huang
Atmos. Chem. Phys., 18, 15581–15600, https://doi.org/10.5194/acp-18-15581-2018, https://doi.org/10.5194/acp-18-15581-2018, 2018
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We have applied the HTAP phase II multi-model data to investigate the long-range transport impacts on surface concentration and column density of PM from Europe and Russia, Belarus, and Ukraine to eastern Asia, with a special focus on the long-range transport contribution during haze episodes in China. We found that long-range transport plays a more important role in elevating the background concentration of surface PM during the haze days.
Hansen Cao, Tzung-May Fu, Lin Zhang, Daven K. Henze, Christopher Chan Miller, Christophe Lerot, Gonzalo González Abad, Isabelle De Smedt, Qiang Zhang, Michel van Roozendael, François Hendrick, Kelly Chance, Jie Li, Junyu Zheng, and Yuanhong Zhao
Atmos. Chem. Phys., 18, 15017–15046, https://doi.org/10.5194/acp-18-15017-2018, https://doi.org/10.5194/acp-18-15017-2018, 2018
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Our top-down estimates for annual total Chinese NMVOC emissions was 30.7 to 49.5 Tg y−1, including 16.4 to 23.6 Tg y−1 from anthropogenic sources, 12.2 to 22.8 Tg y−1 from biogenic sources, and 2.08 to 3.13 Tg y−1 from biomass burning. Our four inversions consistently showed that the emissions of Chinese anthropogenic NMVOC precursors of glyoxal were larger than the a priori estimates. The glyoxal and formaldehyde constraints helped distinguish the NMVOC species from different sources.
Marina Astitha, Ioannis Kioutsioukis, Ghezae Araya Fisseha, Roberto Bianconi, Johannes Bieser, Jesper H. Christensen, Owen R. Cooper, Stefano Galmarini, Christian Hogrefe, Ulas Im, Bryan Johnson, Peng Liu, Uarporn Nopmongcol, Irina Petropavlovskikh, Efisio Solazzo, David W. Tarasick, and Greg Yarwood
Atmos. Chem. Phys., 18, 13925–13945, https://doi.org/10.5194/acp-18-13925-2018, https://doi.org/10.5194/acp-18-13925-2018, 2018
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This work is unique in the detailed analyses of modeled ozone vertical profiles from sites in North America through the collaboration of four research groups from the US and EU. We assess the air quality models' performance and model inter-comparison for ozone vertical profiles and stratospheric ozone intrusions. Lastly, we designate the important role of lateral boundary conditions in the ozone vertical profiles using chemically inert tracers.
Jan Eiof Jonson, Michael Schulz, Louisa Emmons, Johannes Flemming, Daven Henze, Kengo Sudo, Marianne Tronstad Lund, Meiyun Lin, Anna Benedictow, Brigitte Koffi, Frank Dentener, Terry Keating, Rigel Kivi, and Yanko Davila
Atmos. Chem. Phys., 18, 13655–13672, https://doi.org/10.5194/acp-18-13655-2018, https://doi.org/10.5194/acp-18-13655-2018, 2018
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Focusing on Europe, this HTAP 2 study computes ozone in several global models when reducing anthropogenic emissions by 20 % in different world regions. The differences in model results are explored
by use of a novel stepwise approach combining a tracer, CO and ozone. For ozone the contributions from the rest of the world are larger than from Europe, with the largest contributions from North America and eastern Asia. Contributions do, however, depend on the choice of ozone metric.
Cheng Chen, Oleg Dubovik, Daven K. Henze, Tatyana Lapyonak, Mian Chin, Fabrice Ducos, Pavel Litvinov, Xin Huang, and Lei Li
Atmos. Chem. Phys., 18, 12551–12580, https://doi.org/10.5194/acp-18-12551-2018, https://doi.org/10.5194/acp-18-12551-2018, 2018
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This paper introduces a method to use satellite-observed spectral AOD and AAOD to derive three types of aerosol emission sources simultaneously based on inverse modelling at a high spatial and temporal resolution. This study shows it is possible to estimate aerosol emissions and improve the atmospheric aerosol simulation using detailed aerosol optical and microphysical information from satellite observations.
Ciao-Kai Liang, J. Jason West, Raquel A. Silva, Huisheng Bian, Mian Chin, Yanko Davila, Frank J. Dentener, Louisa Emmons, Johannes Flemming, Gerd Folberth, Daven Henze, Ulas Im, Jan Eiof Jonson, Terry J. Keating, Tom Kucsera, Allen Lenzen, Meiyun Lin, Marianne Tronstad Lund, Xiaohua Pan, Rokjin J. Park, R. Bradley Pierce, Takashi Sekiya, Kengo Sudo, and Toshihiko Takemura
Atmos. Chem. Phys., 18, 10497–10520, https://doi.org/10.5194/acp-18-10497-2018, https://doi.org/10.5194/acp-18-10497-2018, 2018
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Emissions from one continent affect air quality and health elsewhere. Here we quantify the effects of intercontinental PM2.5 and ozone transport on human health using a new multi-model ensemble, evaluating the health effects of emissions from six world regions and three emission source sectors. Emissions from one region have significant health impacts outside of that source region; similarly, foreign emissions contribute significantly to air-pollution-related deaths in several world regions.
Steven T. Turnock, Oliver Wild, Frank J. Dentener, Yanko Davila, Louisa K. Emmons, Johannes Flemming, Gerd A. Folberth, Daven K. Henze, Jan E. Jonson, Terry J. Keating, Sudo Kengo, Meiyun Lin, Marianne Lund, Simone Tilmes, and Fiona M. O'Connor
Atmos. Chem. Phys., 18, 8953–8978, https://doi.org/10.5194/acp-18-8953-2018, https://doi.org/10.5194/acp-18-8953-2018, 2018
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A simple parameterisation was developed in this study to provide a rapid assessment of the impacts and uncertainties associated with future emission control strategies by predicting changes to surface ozone air quality and near-term climate forcing of ozone. Future emissions scenarios based on currently implemented legislation are shown to worsen surface ozone air quality and enhance near-term climate warming, with changes in methane becoming increasingly important in the future.
Stefano Galmarini, Ioannis Kioutsioukis, Efisio Solazzo, Ummugulsum Alyuz, Alessandra Balzarini, Roberto Bellasio, Anna M. K. Benedictow, Roberto Bianconi, Johannes Bieser, Joergen Brandt, Jesper H. Christensen, Augustin Colette, Gabriele Curci, Yanko Davila, Xinyi Dong, Johannes Flemming, Xavier Francis, Andrea Fraser, Joshua Fu, Daven K. Henze, Christian Hogrefe, Ulas Im, Marta Garcia Vivanco, Pedro Jiménez-Guerrero, Jan Eiof Jonson, Nutthida Kitwiroon, Astrid Manders, Rohit Mathur, Laura Palacios-Peña, Guido Pirovano, Luca Pozzoli, Marie Prank, Martin Schultz, Rajeet S. Sokhi, Kengo Sudo, Paolo Tuccella, Toshihiko Takemura, Takashi Sekiya, and Alper Unal
Atmos. Chem. Phys., 18, 8727–8744, https://doi.org/10.5194/acp-18-8727-2018, https://doi.org/10.5194/acp-18-8727-2018, 2018
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An ensemble of model results relating to ozone concentrations in Europe in 2010 has been produced and studied. The novelty consists in the fact that the ensemble is made of results of models working at two different scales (regional and global), therefore contributing in detail two different parts of the atmospheric spectrum. The ensemble defined as a hybrid has been studied in detail and shown to bring additional value to the assessment of air quality.
Jiani Tan, Joshua S. Fu, Frank Dentener, Jian Sun, Louisa Emmons, Simone Tilmes, Kengo Sudo, Johannes Flemming, Jan Eiof Jonson, Sylvie Gravel, Huisheng Bian, Yanko Davila, Daven K. Henze, Marianne T. Lund, Tom Kucsera, Toshihiko Takemura, and Terry Keating
Atmos. Chem. Phys., 18, 6847–6866, https://doi.org/10.5194/acp-18-6847-2018, https://doi.org/10.5194/acp-18-6847-2018, 2018
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We study the distributions of sulfur and nitrogen deposition, which are associated with current environmental issues such as formation of acid rain and ecosystem eutrophication and result in widespread problems such as loss of environmental diversity, harming the crop yield and even food insecurity. According to our study, both the amount and distribution of sulfate and nitrogen deposition have changed significantly in the last decade, particularly in East Asia, South Asia and Southeast Asia.
Kira Sadighi, Evan Coffey, Andrea Polidori, Brandon Feenstra, Qin Lv, Daven K. Henze, and Michael Hannigan
Atmos. Meas. Tech., 11, 1777–1792, https://doi.org/10.5194/amt-11-1777-2018, https://doi.org/10.5194/amt-11-1777-2018, 2018
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Ground-level ozone has negative human health impacts. In the summer of 2015, 13 low-cost sensor monitors were deployed to several neighborhoods around Riverside, California. There were significant spatial differences between monitors. This is important because it means that ozone in certain places may be higher than what EPA monitors report for an area, which is pertinent for residents of those communities. This research helps inform the limitations and advantages of low-cost sensor networks.
Kelley C. Wells, Dylan B. Millet, Nicolas Bousserez, Daven K. Henze, Timothy J. Griffis, Sreelekha Chaliyakunnel, Edward J. Dlugokencky, Eri Saikawa, Gao Xiang, Ronald G. Prinn, Simon O'Doherty, Dickon Young, Ray F. Weiss, Geoff S. Dutton, James W. Elkins, Paul B. Krummel, Ray Langenfelds, and L. Paul Steele
Atmos. Chem. Phys., 18, 735–756, https://doi.org/10.5194/acp-18-735-2018, https://doi.org/10.5194/acp-18-735-2018, 2018
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This paper uses three different frameworks to derive nitrous oxide (N2O) emissions based on global surface observations. One of these frameworks employs a new approach that allows for fast computation and explores a larger solution space than other methods. Our results point to a few conclusions about the global N2O budget, including a larger contribution from tropical sources, an overestimate of natural soil emissions, and an underestimate of agricultural sources particularly in springtime.
Lin Zhang, Youfan Chen, Yuanhong Zhao, Daven K. Henze, Liye Zhu, Yu Song, Fabien Paulot, Xuejun Liu, Yuepeng Pan, Yi Lin, and Binxiang Huang
Atmos. Chem. Phys., 18, 339–355, https://doi.org/10.5194/acp-18-339-2018, https://doi.org/10.5194/acp-18-339-2018, 2018
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Substantial differences exist in current estimates of agricultural ammonia emissions in China, hindering understanding of their environmental consequences. This study applies both bottom-up and top-down methods to better quantify agricultural ammonia sources in China using observations from satellite and surface networks interpreted by a chemical transport model. Our estimate of annual Chinese anthropogenic ammonia emission is 11.7 tg (teragram) for 2008 with a strong seasonality peak in summer.
Jun-Wei Xu, Randall V. Martin, Andrew Morrow, Sangeeta Sharma, Lin Huang, W. Richard Leaitch, Julia Burkart, Hannes Schulz, Marco Zanatta, Megan D. Willis, Daven K. Henze, Colin J. Lee, Andreas B. Herber, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 17, 11971–11989, https://doi.org/10.5194/acp-17-11971-2017, https://doi.org/10.5194/acp-17-11971-2017, 2017
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We interpret a series of recent airborne and ground-based measurements with the GEOS-Chem model and its adjoint to attribute the sources of Arctic BC. Anthropogenic emissions in eastern and southern Asia make the largest contribution to Arctic BC. Gas flaring emissions from oilfields in western Siberia and from the Tarim oilfield in western China could have striking impacts on Arctic BC loadings.
Ling Qi, Qinbin Li, Daven K. Henze, Hsien-Liang Tseng, and Cenlin He
Atmos. Chem. Phys., 17, 9697–9716, https://doi.org/10.5194/acp-17-9697-2017, https://doi.org/10.5194/acp-17-9697-2017, 2017
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We find that Asian anthropogenic sources are the largest contributors (~ 40 %) to surface BC in spring in the Arctic, inconsistent with previous studies which repeatedly identified sources of surface BC as anthropogenic emissions from Europe and Russia. It takes 12–17 days for Asian anthropogenic emissions to be transported to the Arctic surface. Additionally, a large fraction (40–65 %) of Asian contribution is in the form of chronic pollution on 1- to 2-month timescales.
Karen E. Cady-Pereira, Vivienne H. Payne, Jessica L. Neu, Kevin W. Bowman, Kazuyuki Miyazaki, Eloise A. Marais, Susan Kulawik, Zitely A. Tzompa-Sosa, and Jennifer D. Hegarty
Atmos. Chem. Phys., 17, 9379–9398, https://doi.org/10.5194/acp-17-9379-2017, https://doi.org/10.5194/acp-17-9379-2017, 2017
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Air quality is a major issue for megacities. Our paper looks at satellite measurements over Mexico City and Lagos of several trace gases gases related to air quality to determine the temporal and spatial variability of these gases, and it relates this variability to local conditions, such as topography, winds and biomass burning events. We find that, while Mexico City is known for severe pollution events, the levels of of pollution in Lagos are much higher and more persistent.
Jonathan J. Guerrette and Daven K. Henze
Atmos. Chem. Phys., 17, 7605–7633, https://doi.org/10.5194/acp-17-7605-2017, https://doi.org/10.5194/acp-17-7605-2017, 2017
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This work describes the implementation and application of a new advanced tool, WRFDA-Chem, for top-down constraints of regional atmospheric chemical emissions. Aircraft and surface observations of black carbon are traced to anthropogenic and biomass burning sources in California during ARCTAS-CARB. The information content of the observations is quantified through variance reduction and degrees of freedom of signal, which can be used to assess observing strategies and emission inventories.
Zhe Jiang, Helen Worden, John R. Worden, Daven K. Henze, Dylan B. A. Jones, Avelino F. Arellano, Emily V. Fischer, Liye Zhu, Kazuyuki Miyazaki, K. Folkert Boersma, and Vivienne H. Payne
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-382, https://doi.org/10.5194/acp-2017-382, 2017
Preprint withdrawn
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We investigated the variation of US tropospheric NO2 in the past decade. We demonstrated significant divergence between the time variation in tropospheric NO2 columns from OMI retrievals and surface measurements. Our analysis suggests limited contributions from local effects such as fossil fuel emissions, lightning, or instrument artifacts, and indicates possible important contributions from long-range transport of Asian emissions that are modulated by ENSO.
Min Huang, Gregory R. Carmichael, R. Bradley Pierce, Duseong S. Jo, Rokjin J. Park, Johannes Flemming, Louisa K. Emmons, Kevin W. Bowman, Daven K. Henze, Yanko Davila, Kengo Sudo, Jan Eiof Jonson, Marianne Tronstad Lund, Greet Janssens-Maenhout, Frank J. Dentener, Terry J. Keating, Hilke Oetjen, and Vivienne H. Payne
Atmos. Chem. Phys., 17, 5721–5750, https://doi.org/10.5194/acp-17-5721-2017, https://doi.org/10.5194/acp-17-5721-2017, 2017
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In support of the HTAP phase 2 experiment, we conducted a number of regional-scale Sulfur Transport and dEposition Model base and sensitivity simulations over North America during May–June 2010. The STEM chemical boundary conditions were downscaled from three (GEOS-Chem, RAQMS, and ECMWF C-IFS) global chemical transport models' simulations. Analyses were performed on large spatial–temporal scales relative to HTAP1 and also on subcontinental and event scales including the use of satellite data.
Zhe Jiang, John R. Worden, Helen Worden, Merritt Deeter, Dylan B. A. Jones, Avelino F. Arellano, and Daven K. Henze
Atmos. Chem. Phys., 17, 4565–4583, https://doi.org/10.5194/acp-17-4565-2017, https://doi.org/10.5194/acp-17-4565-2017, 2017
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We constrain the long-term variation in global CO emissions for 2001–2015. Our results confirm that the decreasing trend of tropospheric CO in the Northern Hemisphere is due to decreasing CO emissions from anthropogenic and biomass burning sources. In particular, we find decreasing CO emissions from the United States and China in the past 15 years, unchanged anthropogenic CO emissions from Europe since 2008, and likely a positive trend from India and southeast Asia.
Chantelle R. Lonsdale, Jennifer D. Hegarty, Karen E. Cady-Pereira, Matthew J. Alvarado, Daven K. Henze, Matthew D. Turner, Shannon L. Capps, John B. Nowak, J. Andy Neuman, Ann M. Middlebrook, Roya Bahreini, Jennifer G. Murphy, Milos Z. Markovic, Trevor C. VandenBoer, Lynn M. Russell, and Amy Jo Scarino
Atmos. Chem. Phys., 17, 2721–2739, https://doi.org/10.5194/acp-17-2721-2017, https://doi.org/10.5194/acp-17-2721-2017, 2017
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This study takes advantage of the high-resolution observations of NH3(g) made by the TES satellite instrument over Bakersfield during the CalNex campaign, along with campaign measurements, to compare CMAQ model results in the San Joaquin Valley, California. Additionally we evaluate the CMAQ bi-directional ammonia flux results using the CARB emissions inventory against these satellite and campaign measurements, not previously explored in combination.
Natalie Kille, Sunil Baidar, Philip Handley, Ivan Ortega, Roman Sinreich, Owen R. Cooper, Frank Hase, James W. Hannigan, Gabriele Pfister, and Rainer Volkamer
Atmos. Meas. Tech., 10, 373–392, https://doi.org/10.5194/amt-10-373-2017, https://doi.org/10.5194/amt-10-373-2017, 2017
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This article describes a new instrument for measuring and quantifying emission fluxes. It introduces the instrument using the solar occultation flux method. Results are presented from the FRAPPE field campaign near Denver, Colorado, from 2014. Calculations of emissions of sources are presented from FRAPPE and compared to emission inventories. Finally, structure functions are calculated to facilitate the future comparison of high-resolution measurements with low resolution satellite measurements.
Camilla Weum Stjern, Bjørn Hallvard Samset, Gunnar Myhre, Huisheng Bian, Mian Chin, Yanko Davila, Frank Dentener, Louisa Emmons, Johannes Flemming, Amund Søvde Haslerud, Daven Henze, Jan Eiof Jonson, Tom Kucsera, Marianne Tronstad Lund, Michael Schulz, Kengo Sudo, Toshihiko Takemura, and Simone Tilmes
Atmos. Chem. Phys., 16, 13579–13599, https://doi.org/10.5194/acp-16-13579-2016, https://doi.org/10.5194/acp-16-13579-2016, 2016
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Air pollution can reach distant regions through intercontinental transport. Here we first present results from the Hemispheric Transport of Air Pollution Phase 2 exercise, where many models performed the same set of coordinated emission-reduction experiments. We find that mitigations have considerable extra-regional effects, and show that this is particularly true for black carbon emissions, as long-range transport elevates aerosols to higher levels where their radiative influence is stronger.
Zeli Tan, Qianlai Zhuang, Daven K. Henze, Christian Frankenberg, Ed Dlugokencky, Colm Sweeney, Alexander J. Turner, Motoki Sasakawa, and Toshinobu Machida
Atmos. Chem. Phys., 16, 12649–12666, https://doi.org/10.5194/acp-16-12649-2016, https://doi.org/10.5194/acp-16-12649-2016, 2016
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Methane emissions from the pan-Arctic could be important in understanding the global carbon cycle but are still poorly constrained to date. This study demonstrated that satellite retrievals can be used to reduce the uncertainty of the estimates of these emissions. We also provided additional evidence for the existence of large methane emissions from pan-Arctic lakes in the Siberian yedoma permafrost region. We found that biogeochemical models should be improved for better estimates.
Luis F. Millán, Nathaniel J. Livesey, Michelle L. Santee, Jessica L. Neu, Gloria L. Manney, and Ryan A. Fuller
Atmos. Chem. Phys., 16, 11521–11534, https://doi.org/10.5194/acp-16-11521-2016, https://doi.org/10.5194/acp-16-11521-2016, 2016
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This paper describes the impact of orbital sampling applied to stratospheric temperature and trace gas fields. Model fields are sampled using real sampling patterns from different satellites. We find that coarse nonuniform sampling patterns may introduce non-negligible errors into the inferred magnitude of temperature and trace gas trends and necessitate considerably longer records for their definitive detection.
Lei Sun, Likun Xue, Tao Wang, Jian Gao, Aijun Ding, Owen R. Cooper, Meiyun Lin, Pengju Xu, Zhe Wang, Xinfeng Wang, Liang Wen, Yanhong Zhu, Tianshu Chen, Lingxiao Yang, Yan Wang, Jianmin Chen, and Wenxing Wang
Atmos. Chem. Phys., 16, 10637–10650, https://doi.org/10.5194/acp-16-10637-2016, https://doi.org/10.5194/acp-16-10637-2016, 2016
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We compiled the available observations of surface O3 at Mt. Tai – the highest mountain in the North China Plain, and found a significant increase of O3 concenrations from 2003 to 2015. The observed O3 increase was mainly due to the increase of O3 precursors, especially VOCs. Our analysis shows that controlling NOx alone, in the absence of VOC controls, is not sufficient to reduce regional O3 levels in North China in a short period.
Hilke Oetjen, Vivienne H. Payne, Jessica L. Neu, Susan S. Kulawik, David P. Edwards, Annmarie Eldering, Helen M. Worden, and John R. Worden
Atmos. Chem. Phys., 16, 10229–10239, https://doi.org/10.5194/acp-16-10229-2016, https://doi.org/10.5194/acp-16-10229-2016, 2016
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We developed and tested a strategy for combining TES and IASI free-tropospheric ozone data. A time series of the merged ozone data is presented for regional monthly means over the western US, Europe, and eastern Asia. We show that free-tropospheric ozone over Europe and the western US has remained relatively constant over the past decade but that, contrary to expectations, ozone over Asia in recent years does not continue the rapid rate of increase observed from 2004–2010.
Zhe Jiang, Kazuyuki Miyazaki, John R. Worden, Jane J. Liu, Dylan B. A. Jones, and Daven K. Henze
Atmos. Chem. Phys., 16, 6537–6546, https://doi.org/10.5194/acp-16-6537-2016, https://doi.org/10.5194/acp-16-6537-2016, 2016
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We quantify the impacts of anthropogenic and natural sources on free tropospheric ozone over the Middle East, using the adjoint of the GEOS-Chem model with updated NOx emissions estimates from an ensemble Kalman filter. We show that the global total contribution of lightning NOx on free tropospheric O3 over the Middle East is about 2 times larger than that from global anthropogenic sources. The summertime free tropospheric O3 enhancement is primarily due to Asian NOx emissions.
Nicolas Bousserez, Daven K. Henze, Brigitte Rooney, Andre Perkins, Kevin J. Wecht, Alexander J. Turner, Vijay Natraj, and John R. Worden
Atmos. Chem. Phys., 16, 6175–6190, https://doi.org/10.5194/acp-16-6175-2016, https://doi.org/10.5194/acp-16-6175-2016, 2016
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This work provides new insight into the observational constraints provided by current low-Earth orbit (LEO) and future potential geostationary (GEO) satellite missions on methane emissions in North America. Using efficient numerical tools, the information content (error reductions, spatial resolution of the constraints) of methane inversions using different instrument configurations (TIR, SWIR and multi-spectral) was estimated at model grid-scale resolution (0.5° × 0.7°).
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.
M. W. Shephard, C. A. McLinden, K. E. Cady-Pereira, M. Luo, S. G. Moussa, A. Leithead, J. Liggio, R. M. Staebler, A. Akingunola, P. Makar, P. Lehr, J. Zhang, D. K. Henze, D. B. Millet, J. O. Bash, L. Zhu, K. C. Wells, S. L. Capps, S. Chaliyakunnel, M. Gordon, K. Hayden, J. R. Brook, M. Wolde, and S.-M. Li
Atmos. Meas. Tech., 8, 5189–5211, https://doi.org/10.5194/amt-8-5189-2015, https://doi.org/10.5194/amt-8-5189-2015, 2015
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This study provides direct validations of Tropospheric Emission Spectrometer (TES) satellite retrieved profiles against coincident aircraft profiles of carbon monoxide, ammonia, methanol, and formic acid, all of which are of interest for air quality. The comparisons are performed over the Canadian oil sands region during an intensive field campaign in support of the Joint Canada-Alberta Implementation Plan for the Oil Sands Monitoring (JOSM). Initial model evaluations are also provided.
L. Zhu, D. Henze, J. Bash, G.-R. Jeong, K. Cady-Pereira, M. Shephard, M. Luo, F. Paulot, and S. Capps
Atmos. Chem. Phys., 15, 12823–12843, https://doi.org/10.5194/acp-15-12823-2015, https://doi.org/10.5194/acp-15-12823-2015, 2015
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We implement new diurnal variation scheme for ammonia livestock emissions and bidirectional exchange scheme and its adjoint in the GEOS-Chem global chemical transport model. Updated diurnal variability improves modeled-to-hourly in situ measurements comparison. The ammonium soil pool in the bidirectional exchange model largely extends the ammonia lifetime in the atmosphere. Large model biases remain as livestock emissions are still underestimated.
F. Deng, D. B. A. Jones, T. W. Walker, M. Keller, K. W. Bowman, D. K. Henze, R. Nassar, E. A. Kort, S. C. Wofsy, K. A. Walker, A. E. Bourassa, and D. A. Degenstein
Atmos. Chem. Phys., 15, 11773–11788, https://doi.org/10.5194/acp-15-11773-2015, https://doi.org/10.5194/acp-15-11773-2015, 2015
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The upper troposphere and lower stratosphere (UTLS) is characterized by strong gradients in the distribution of long-lived tracers, which are sensitive to discrepancies in transport in models. We found that our model overestimates CO2 in the polar UTLS through comparison of modeled CO2 with aircraft observations. We then corrected the modeled CO2 and quantified the impact of the correction on the flux estimates using an atmospheric model together with atmospheric CO2 measured from a satellite.
K. C. Wells, D. B. Millet, N. Bousserez, D. K. Henze, S. Chaliyakunnel, T. J. Griffis, Y. Luan, E. J. Dlugokencky, R. G. Prinn, S. O'Doherty, R. F. Weiss, G. S. Dutton, J. W. Elkins, P. B. Krummel, R. Langenfelds, L. P. Steele, E. A. Kort, S. C. Wofsy, and T. Umezawa
Geosci. Model Dev., 8, 3179–3198, https://doi.org/10.5194/gmd-8-3179-2015, https://doi.org/10.5194/gmd-8-3179-2015, 2015
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This paper introduces a new inversion framework for N2O using GEOS-Chem and its adjoint, which we employed in a series of observing system simulation experiments to evaluate the source and sink constraints provided by surface and aircraft-based N2O measurements. We also applied a new approach for estimating a posteriori uncertainty for high-dimensional inversions, and used it to quantify the spatial and temporal resolution of N2O emission constraints achieved with the current observing network.
Y. Zhao, L. Zhang, Y. Pan, Y. Wang, F. Paulot, and D. K. Henze
Atmos. Chem. Phys., 15, 10905–10924, https://doi.org/10.5194/acp-15-10905-2015, https://doi.org/10.5194/acp-15-10905-2015, 2015
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Rapid Asian industrialization has led to increased atmospheric nitrogen deposition downwind. This work analyzes the sources and processes controlling atmospheric nitrogen deposition to the northwestern Pacific. Both nitrogen emissions and meteorology, largely controlled by the East Asian Monsoon, determine the seasonality of nitrogen deposition. Ascribing deposition over the marginal seas to nitrogen sources from different regions and sectors shows important contribution from fertilizer use.
P. D. Hamer, K. W. Bowman, D. K. Henze, J.-L. Attié, and V. Marécal
Atmos. Chem. Phys., 15, 10645–10667, https://doi.org/10.5194/acp-15-10645-2015, https://doi.org/10.5194/acp-15-10645-2015, 2015
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Using a simplified air quality forecasting model, we explore how characteristics of air quality observations affect our ability to understand and predict ozone air pollution. We show that the photochemical conditions can strongly influence the observing priorities for ozone prediction, such as which species are observed and how well, when, and how frequently. High-freqency observations of ozone, NOx and HCHO in combination during the morning and afternoon are particularly advantageous.
L. Zhang, D. K. Henze, G. A. Grell, G. R. Carmichael, N. Bousserez, Q. Zhang, O. Torres, C. Ahn, Z. Lu, J. Cao, and Y. Mao
Atmos. Chem. Phys., 15, 10281–10308, https://doi.org/10.5194/acp-15-10281-2015, https://doi.org/10.5194/acp-15-10281-2015, 2015
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We attempt to reduce uncertainties in BC emissions and improve BC model simulations by developing top-down, spatially resolved, estimates of BC emissions through assimilation of OMI observations of aerosol absorption optical depth (AAOD) with the GEOS-Chem model and its adjoint for April and October of 2006. Despite the limitations and uncertainties, using OMI AAOD to constrain BC sources we are able to improve model representation of BC distributions, particularly over China.
P. S. Monks, A. T. Archibald, A. Colette, O. Cooper, M. Coyle, R. Derwent, D. Fowler, C. Granier, K. S. Law, G. E. Mills, D. S. Stevenson, O. Tarasova, V. Thouret, E. von Schneidemesser, R. Sommariva, O. Wild, and M. L. Williams
Atmos. Chem. Phys., 15, 8889–8973, https://doi.org/10.5194/acp-15-8889-2015, https://doi.org/10.5194/acp-15-8889-2015, 2015
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Ozone holds a certain fascination in atmospheric science. It is ubiquitous in the atmosphere, central to tropospheric oxidation chemistry, and yet harmful to human and ecosystem health as well as being an important greenhouse gas. It is not emitted into the atmosphere but is a byproduct of the very oxidation chemistry it largely initiates. This review examines current understanding of the processes regulating tropospheric ozone at global to local scales from both measurements and models.
Y. H. Mao, Q. B. Li, D. K. Henze, Z. Jiang, D. B. A. Jones, M. Kopacz, C. He, L. Qi, M. Gao, W.-M. Hao, and K.-N. Liou
Atmos. Chem. Phys., 15, 7685–7702, https://doi.org/10.5194/acp-15-7685-2015, https://doi.org/10.5194/acp-15-7685-2015, 2015
J. J. Guerrette and D. K. Henze
Geosci. Model Dev., 8, 1857–1876, https://doi.org/10.5194/gmd-8-1857-2015, https://doi.org/10.5194/gmd-8-1857-2015, 2015
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WRFPLUS-Chem is a coupled meteorology-chemistry adjoint and tangent linear model, with applications in sensitivity analysis and four-dimensional variational data assimilation. The linearized models are verified against finite difference approximations from the nonlinear forward model, WRF-Chem. A new checkpointing scheme enables data assimilation beyond 6h. New capabilities are demonstrated in an emission sensitivity study.
Z. Jiang, D. B. A. Jones, J. Worden, H. M. Worden, D. K. Henze, and Y. X. Wang
Atmos. Chem. Phys., 15, 6801–6814, https://doi.org/10.5194/acp-15-6801-2015, https://doi.org/10.5194/acp-15-6801-2015, 2015
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We present a high-resolution (0.5 x 0.667) regional CO inversion over North America in the period of June 2004–May 2005, using a combination of GEOS-Chem model and MOPITT CO observations. With optimized lateral boundary conditions, we show that regional inversion analyses can reduce the sensitivity of the CO source estimates to errors in long-range transport and in the distributions of the hydroxyl radical (OH), and consequently, provide better quantification on regional CO source estimates.
Z. Jiang, D. B. A. Jones, H. M. Worden, and D. K. Henze
Atmos. Chem. Phys., 15, 1521–1537, https://doi.org/10.5194/acp-15-1521-2015, https://doi.org/10.5194/acp-15-1521-2015, 2015
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Using MOPITT (version 5) tropospheric profile and surface layer retrievals, we constrain global CO emissions in the period of June 2004 – May 2005. The inversions suggest a reduction in CO emission in the tropics and an increase in emissions at middle and high latitudes. The results demonstrate that the use of the surface layer retrievals from MOPITT can significantly mitigate the potential impacts of model bias in OH and long-range transport on CO emission estimates.
Z. Jiang, J. R. Worden, D. B. A. Jones, J.-T. Lin, W. W. Verstraeten, and D. K. Henze
Atmos. Chem. Phys., 15, 99–112, https://doi.org/10.5194/acp-15-99-2015, https://doi.org/10.5194/acp-15-99-2015, 2015
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We use satellite measurements of O3, CO and NO2 from TES, MOPITT and OMI to quantify O3 precursor emissions for 2006 and their impact on free tropospheric O3 over northeastern Asia. Using the adjoint of GEOS-Chem, we found that Chinese emissions have the largest influence on the free tropospheric O3. The contributions from lightning NOx in summer and India and southeastern Asia emissions in winter are sizable, comparable with Chinese emissions.
Q. Zhu, Q. Zhuang, D. Henze, K. Bowman, M. Chen, Y. Liu, Y. He, H. Matsueda, T. Machida, Y. Sawa, and W. Oechel
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-22587-2014, https://doi.org/10.5194/acpd-14-22587-2014, 2014
Revised manuscript not accepted
W. C. Keene, J. L. Moody, J. N. Galloway, J. M. Prospero, O. R. Cooper, S. Eckhardt, and J. R. Maben
Atmos. Chem. Phys., 14, 8119–8135, https://doi.org/10.5194/acp-14-8119-2014, https://doi.org/10.5194/acp-14-8119-2014, 2014
Z. Shen, J. Liu, L. W. Horowitz, D. K. Henze, S. Fan, Levy II H., D. L. Mauzerall, J.-T. Lin, and S. Tao
Atmos. Chem. Phys., 14, 6315–6327, https://doi.org/10.5194/acp-14-6315-2014, https://doi.org/10.5194/acp-14-6315-2014, 2014
F. Deng, D. B. A. Jones, D. K. Henze, N. Bousserez, K. W. Bowman, J. B. Fisher, R. Nassar, C. O'Dell, D. Wunch, P. O. Wennberg, E. A. Kort, S. C. Wofsy, T. Blumenstock, N. M. Deutscher, D. W. T. Griffith, F. Hase, P. Heikkinen, V. Sherlock, K. Strong, R. Sussmann, and T. Warneke
Atmos. Chem. Phys., 14, 3703–3727, https://doi.org/10.5194/acp-14-3703-2014, https://doi.org/10.5194/acp-14-3703-2014, 2014
K. C. Wells, D. B. Millet, K. E. Cady-Pereira, M. W. Shephard, D. K. Henze, N. Bousserez, E. C. Apel, J. de Gouw, C. Warneke, and H. B. Singh
Atmos. Chem. Phys., 14, 2555–2570, https://doi.org/10.5194/acp-14-2555-2014, https://doi.org/10.5194/acp-14-2555-2014, 2014
J. L. Moody, W. C. Keene, O. R. Cooper, K. J. Voss, R. Aryal, S. Eckhardt, B. Holben, J. R. Maben, M. A. Izaguirre, and J. N. Galloway
Atmos. Chem. Phys., 14, 691–717, https://doi.org/10.5194/acp-14-691-2014, https://doi.org/10.5194/acp-14-691-2014, 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
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
CO anthropogenic emissions in Europe from 2011 to 2021: insights from Measurement of Pollution in the Troposphere (MOPITT) satellite data
Constraining long-term NOx emissions over the United States and Europe using nitrate wet deposition monitoring networks
Analysis of an intense O3 pollution episode on the Atlantic coast of the Iberian Peninsula using photochemical modeling: characterization of transport pathways and accumulation processes
Atmospheric oxygen as a tracer for fossil fuel carbon dioxide: a sensitivity study in the UK
MIXv2: a long-term mosaic emission inventory for Asia (2010–2017)
Organosulfate produced from consumption of SO3 speeds up sulfuric acid–dimethylamine atmospheric nucleation
Contribution of expanded marine sulfur chemistry to the seasonal variability of dimethyl sulfide oxidation products and size-resolved sulfate aerosol
Spatial disparities of ozone pollution in the Sichuan Basin spurred by extreme, hot weather
Global impacts of aviation on air quality evaluated at high resolution
Bias correction of OMI HCHO columns based on FTIR and aircraft measurements and impact on top-down emission estimates
Investigation of the renewed methane growth post-2007 with high-resolution 3-D variational inverse modeling and isotopic constraints
Revisiting day-of-week ozone patterns in an era of evolving US air quality
Air quality and radiative impacts of downward-propagating sudden stratospheric warmings (SSWs)
Estimation of the atmospheric hydroxyl radical oxidative capacity using multiple hydrofluorocarbons (HFCs)
Investigating the differences in calculating global mean surface CO2 abundance: the impact of analysis methodologies and site selection
Meteorological characteristics of extreme ozone pollution events in China and their future predictions
Evaluating modelled tropospheric columns of CH4, CO, and O3 in the Arctic using ground-based Fourier transform infrared (FTIR) measurements
The high-resolution Global Aviation emissions Inventory based on ADS-B (GAIA) for 2019–2021
Zonal variability of methane trends derived from satellite data
Weekly derived top-down volatile-organic-compound fluxes over Europe from TROPOMI HCHO data from 2018 to 2021
Technical note: Challenges of detecting free tropospheric ozone trends in a sparsely sampled environment
Current status of model predictions of volatile organic compounds and impacts on surface ozone predictions during summer in China
Utility of Geostationary Lightning Mapper-derived lightning NO emission estimates in air quality modeling studies
The suitability of atmospheric oxygen measurements to constrain western European fossil-fuel CO2 emissions and their trends
Future tropospheric ozone budget and distribution over east Asia under a net-zero scenario
Comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA: implications for atmospheric oxidative capacity
Insights into soil NO emissions and the contribution to surface ozone formation in China
The impact of gaseous degradation on the equilibrium state of gas/particle partitioning of semi-volatile organic compounds
An intercomparison of satellite, airborne, and ground-level observations with WRF-CAMx simulations of NO2 columns over Houston, TX during the September 2021 TRACER-AQ campaign
Development, intercomparison, and evaluation of an improved mechanism for the oxidation of dimethyl sulfide in the UKCA model
A better representation of VOC chemistry in WRF-Chem and its impact on ozone over Los Angeles
Technical note: An assessment of the performance of statistical bias correction techniques for global chemistry-climate model surface ozone fields
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
The impact multi-decadal of changes in VOCs speciation on urban ozone chemistry: A case study in Birmingham, United Kingdom
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?
Summertime tropospheric ozone source apportionment study in Madrid (Spain)
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
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
Simulations of winter ozone in the Upper Green River basin, Wyoming, using WRF-Chem
Audrey Fortems-Cheiney, Gregoire Broquet, Elise Potier, Robin Plauchu, Antoine Berchet, Isabelle Pison, Hugo Denier van der Gon, and Stijn Dellaert
Atmos. Chem. Phys., 24, 4635–4649, https://doi.org/10.5194/acp-24-4635-2024, https://doi.org/10.5194/acp-24-4635-2024, 2024
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We have estimated the carbon monixide (CO) European emissions from satellite observations of the MOPITT instrument at the relatively high resolution of 0.5° for a period of over 10 years from 2011 to 2021. The analysis of the inversion results reveals the challenges associated with the inversion of CO emissions at the regional scale over Europe.
Amy Christiansen, Loretta J. Mickley, and Lu Hu
Atmos. Chem. Phys., 24, 4569–4589, https://doi.org/10.5194/acp-24-4569-2024, https://doi.org/10.5194/acp-24-4569-2024, 2024
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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 emission 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.
Eduardo Torre-Pascual, Gotzon Gangoiti, Ana Rodríguez-García, Estibaliz Sáez de Cámara, Joana Ferreira, Carla Gama, María Carmen Gómez, Iñaki Zuazo, Jose Antonio García, and Maite de Blas
Atmos. Chem. Phys., 24, 4305–4329, https://doi.org/10.5194/acp-24-4305-2024, https://doi.org/10.5194/acp-24-4305-2024, 2024
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We present an analysis of an intense air pollution episode of tropospheric ozone (O3) along the Atlantic coast of the Iberian Peninsula, incorporating both measured and simulated parameters. Our study extends beyond surface-level factors to include altitude-related parameters. These episodes stem from upper-atmosphere O3 accumulation in preceding days, transported to surface layers, causing rapid O3 concentration increase.
Hannah Chawner, Eric Saboya, Karina E. Adcock, Tim Arnold, Yuri Artioli, Caroline Dylag, Grant L. Forster, Anita Ganesan, Heather Graven, Gennadi Lessin, Peter Levy, Ingrid T. Luijkx, Alistair Manning, Penelope A. Pickers, Chris Rennick, Christian Rödenbeck, and Matthew Rigby
Atmos. Chem. Phys., 24, 4231–4252, https://doi.org/10.5194/acp-24-4231-2024, https://doi.org/10.5194/acp-24-4231-2024, 2024
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The quantity of atmospheric potential oxygen (APO), derived from coincident measurements of carbon dioxide (CO2) and oxygen (O2), has been proposed as a tracer for fossil fuel CO2 emissions. In this model sensitivity study, we examine the use of APO for this purpose in the UK and compare our model to observations. We find that our model simulations are most sensitive to uncertainties relating to ocean fluxes and boundary conditions.
Meng Li, Junichi Kurokawa, Qiang Zhang, Jung-Hun Woo, Tazuko Morikawa, Satoru Chatani, Zifeng Lu, Yu Song, Guannan Geng, Hanwen Hu, Jinseok Kim, Owen R. Cooper, and Brian C. McDonald
Atmos. Chem. Phys., 24, 3925–3952, https://doi.org/10.5194/acp-24-3925-2024, https://doi.org/10.5194/acp-24-3925-2024, 2024
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In this work, we developed MIXv2, a mosaic Asian emission inventory for 2010–2017. With high spatial (0.1°) and monthly temporal resolution, MIXv2 integrates anthropogenic and open biomass burning emissions across seven sectors following a mosaic methodology. It provides CO2 emissions data alongside nine key pollutants and three chemical mechanisms. Our publicly accessible gridded monthly emissions data can facilitate long-term atmospheric and climate model analyses.
Xiaomeng Zhang, Yongjian Lian, Shendong Tan, and Shi Yin
Atmos. Chem. Phys., 24, 3593–3612, https://doi.org/10.5194/acp-24-3593-2024, https://doi.org/10.5194/acp-24-3593-2024, 2024
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Atmospheric new particle formation (NPF) has a significant influence on the global climate, local air quality and human health. Using a combination of quantum chemical calculations and kinetics modeling, we find that thhe gas-phase organosulfate produced from consumption of SO3 can significantly enhance SA–DMA nucleation in the polluted boundary layer, resulting in non-negligible contributions to NPF. Our findings provide important insights into organic sulfur in atmospheric aerosol formation.
Linia Tashmim, William C. Porter, Qianjie Chen, Becky Alexander, Charles H. Fite, Christopher D. Holmes, Jeffrey R. Pierce, Betty Croft, and Sakiko Ishino
Atmos. Chem. Phys., 24, 3379–3403, https://doi.org/10.5194/acp-24-3379-2024, https://doi.org/10.5194/acp-24-3379-2024, 2024
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Dimethyl sulfide (DMS) is mostly emitted from ocean surfaces and represents the largest natural source of sulfur for the atmosphere. Once in the atmosphere, DMS forms stable oxidation products such as SO2 and H2SO4, which can subsequently contribute to airborne particle formation and growth. In this study, we update the DMS oxidation mechanism in the chemical transport model GEOS-Chem and describe resulting changes in particle growth as well as the overall global sulfur budget.
Nan Wang, Yunsong Du, Dongyang Chen, Haiyan Meng, Xi Chen, Li Zhou, Guangming Shi, Yu Zhan, Miao Feng, Wei Li, Mulan Chen, Zhenliang Li, and Fumo Yang
Atmos. Chem. Phys., 24, 3029–3042, https://doi.org/10.5194/acp-24-3029-2024, https://doi.org/10.5194/acp-24-3029-2024, 2024
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In the scorching August 2022 heatwave, China's Sichuan Basin saw a stark contrast in ozone (O3) levels between Chengdu and Chongqing. The regional disparities were studied considering meteorology, precursors, photochemistry, and transportation. The study highlighted the importance of tailored pollution control measures and underlined the necessity for region-specific strategies to combat O3 pollution on a regional scale.
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.
Jean-François Müller, Trissevgeni Stavrakou, Glenn-Michael Oomen, Beata Opacka, Isabelle De Smedt, Alex Guenther, Corinne Vigouroux, Bavo Langerock, Carlos Augusto Bauer Aquino, Michel Grutter, James Hannigan, Frank Hase, Rigel Kivi, Erik Lutsch, Emmanuel Mahieu, Maria Makarova, Jean-Marc Metzger, Isamu Morino, Isao Murata, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Amelie Röhling, Wolfgang Stremme, Kimberly Strong, Ralf Sussmann, Yao Té, and Alan Fried
Atmos. Chem. Phys., 24, 2207–2237, https://doi.org/10.5194/acp-24-2207-2024, https://doi.org/10.5194/acp-24-2207-2024, 2024
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Formaldehyde observations from satellites can be used to constrain the emissions of volatile organic compounds, but those observations have biases. Using an atmospheric model, aircraft and ground-based remote sensing data, we quantify these biases, propose a correction to the data, and assess the consequence of this correction for the evaluation of emissions.
Joël Thanwerdas, Marielle Saunois, Antoine Berchet, Isabelle Pison, and Philippe Bousquet
Atmos. Chem. Phys., 24, 2129–2167, https://doi.org/10.5194/acp-24-2129-2024, https://doi.org/10.5194/acp-24-2129-2024, 2024
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We investigate the causes of the renewed growth of atmospheric methane (CH4) after 2007 using inverse modeling. We use the additional information provided by observations of CH4 isotopic compositions to better differentiate between the emission categories. Accounting for the large uncertainties in source signatures, our results suggest that the post-2007 increase in atmospheric CH4 was caused by similar increases in emissions from (1) fossil fuels and (2) agriculture and waste.
Heather Simon, Christian Hogrefe, Andrew Whitehill, Kristen M. Foley, Jennifer Liljegren, Norm Possiel, Benjamin Wells, Barron H. Henderson, Lukas C. Valin, Gail Tonnesen, K. Wyat Appel, and Shannon Koplitz
Atmos. Chem. Phys., 24, 1855–1871, https://doi.org/10.5194/acp-24-1855-2024, https://doi.org/10.5194/acp-24-1855-2024, 2024
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We assess observed and modeled ozone weekend–weekday differences in the USA from 2002–2019. A subset of urban areas that were NOx-saturated at the beginning of the period transitioned to NOx-limited conditions. Multiple rural areas of California were NOx-limited for the entire period but become less influenced by local day-of-week emission patterns in more recent years. The model produces more NOx-saturated conditions than the observations but captures trends in weekend–weekday ozone patterns.
Ryan S. Williams, Michaela I. Hegglin, Patrick Jöckel, Hella Garny, and Keith P. Shine
Atmos. Chem. Phys., 24, 1389–1413, https://doi.org/10.5194/acp-24-1389-2024, https://doi.org/10.5194/acp-24-1389-2024, 2024
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During winter, a brief but abrupt reversal of the mean stratospheric westerly flow (~30 km high) around the Arctic occurs ~6 times a decade. Using a chemistry–climate model, about half of these events are shown to induce large anomalies in Arctic ozone (>25 %) and water vapour (>±25 %) around ~8–12 km altitude for up to 2–3 months, important for weather forecasting. We also calculate a doubling to trebling of the risk in breaches of mid-latitude surface air quality (ozone) standards (~60 ppbv).
Rona L. Thompson, Stephen A. Montzka, Martin K. Vollmer, Jgor Arduini, Molly Crotwell, Paul B. Krummel, Chris Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Stefan Reimann, Isaac Vimont, Hsiang Wang, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 24, 1415–1427, https://doi.org/10.5194/acp-24-1415-2024, https://doi.org/10.5194/acp-24-1415-2024, 2024
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The hydroxyl radical 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 that 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.
Zhendong Wu, Alex Vermeulen, Yousuke Sawa, Ute Karstens, Wouter Peters, Remco de Kok, Xin Lan, Yasuyuki Nagai, Akinori Ogi, and Oksana Tarasova
Atmos. Chem. Phys., 24, 1249–1264, https://doi.org/10.5194/acp-24-1249-2024, https://doi.org/10.5194/acp-24-1249-2024, 2024
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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, as well as trends in atmospheric CO2 mass changes. However, small differences exist in different analyses due to the impact of methodology and site selection.
Yang Yang, Yang Zhou, Hailong Wang, Mengyun Li, Huimin Li, Pinya Wang, Xu Yue, Ke Li, Jia Zhu, and Hong Liao
Atmos. Chem. Phys., 24, 1177–1191, https://doi.org/10.5194/acp-24-1177-2024, https://doi.org/10.5194/acp-24-1177-2024, 2024
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This study reveals that extreme ozone pollution over the North China Plain and Yangtze River Delta is due to the chemical production related to hot and dry conditions, and the regional transport explains the ozone pollution over the Sichuan Basin and Pearl River Delta. The frequency of meteorological conditions of the extreme ozone pollution increases from the past to the future. The sustainable scenario is the optimal path to retaining clean air in China in the future.
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
Atmos. Chem. Phys., 24, 1079–1118, https://doi.org/10.5194/acp-24-1079-2024, https://doi.org/10.5194/acp-24-1079-2024, 2024
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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 generally underpredict the concentrations of these gases in the Arctic troposphere.
Roger Teoh, Zebediah Engberg, Marc Shapiro, Lynnette Dray, and Marc E. J. Stettler
Atmos. Chem. Phys., 24, 725–744, https://doi.org/10.5194/acp-24-725-2024, https://doi.org/10.5194/acp-24-725-2024, 2024
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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.
Jonas Hachmeister, Oliver Schneising, Michael Buchwitz, John P. Burrows, Justus Notholt, and Matthias Buschmann
Atmos. Chem. Phys., 24, 577–595, https://doi.org/10.5194/acp-24-577-2024, https://doi.org/10.5194/acp-24-577-2024, 2024
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We quantified changes in atmospheric methane 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.
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
Atmos. Chem. Phys., 24, 449–474, https://doi.org/10.5194/acp-24-449-2024, https://doi.org/10.5194/acp-24-449-2024, 2024
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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.
Kai-Lan Chang, Owen R. Cooper, Audrey Gaudel, Irina Petropavlovskikh, Peter Effertz, Gary Morris, and Brian C. McDonald
EGUsphere, https://doi.org/10.5194/egusphere-2023-2739, https://doi.org/10.5194/egusphere-2023-2739, 2024
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The great majority of observational trend studies of free tropospheric ozone use sparsely sampled ozonesonde and aircraft measurements as reference datasets. A ubiquitous assumption is that trends are accurate and reliable so long as long-term records are available. We show that sampling bias due to sparse samples can persistently reduce the trend accuracy, and highlight the importance of maintaining adequate frequency and continuity of observations.
Yongliang She, Jingyi Li, Xiaopu Lyu, Hai Guo, Momei Qin, Xiaodong Xie, Kangjia Gong, Fei Ye, Jianjiong Mao, Lin Huang, and Jianlin Hu
Atmos. Chem. Phys., 24, 219–233, https://doi.org/10.5194/acp-24-219-2024, https://doi.org/10.5194/acp-24-219-2024, 2024
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In this study, we use multi-site volatile organic compound (VOC) measurements to evaluate the CMAQ-model-predicted VOCs and assess the impacts of VOC bias on O3 simulation. Our results demonstrate that current modeling setups and emission inventories are likely to underpredict VOC concentrations, and this underprediction of VOCs contributes to lower O3 predictions in China.
Peiyang Cheng, Arastoo Pour-Biazar, Yuling Wu, Shi Kuang, Richard T. McNider, and William J. Koshak
Atmos. Chem. Phys., 24, 41–63, https://doi.org/10.5194/acp-24-41-2024, https://doi.org/10.5194/acp-24-41-2024, 2024
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Lightning-induced nitrogen monoxide (LNO) emission can be estimated from geostationary satellite observations. The present study uses the LNO emission estimates derived from geostationary satellite observations in an air quality modeling system to investigate the impact of LNO on air quality. Results indicate that significant ozone increase could be due to long-distance chemical transport, lightning activity in the upwind direction, and the mixing of high LNO (or ozone) plumes.
Christian Rödenbeck, Karina E. Adcock, Markus Eritt, Maksym Gachkivskyi, 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
Atmos. Chem. Phys., 23, 15767–15782, https://doi.org/10.5194/acp-23-15767-2023, https://doi.org/10.5194/acp-23-15767-2023, 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.
Xuewei Hou, Oliver Wild, Bin Zhu, and James Lee
Atmos. Chem. Phys., 23, 15395–15411, https://doi.org/10.5194/acp-23-15395-2023, https://doi.org/10.5194/acp-23-15395-2023, 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 scenarios 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.
Meghna Soni, Rolf Sander, Lokesh K. Sahu, Domenico Taraborrelli, Pengfei Liu, Ankit Patel, Imran A. Girach, Andrea Pozzer, Sachin S. Gunthe, and Narendra Ojha
Atmos. Chem. Phys., 23, 15165–15180, https://doi.org/10.5194/acp-23-15165-2023, https://doi.org/10.5194/acp-23-15165-2023, 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 has been discussed. The updated chemical mechanism will be useful to interpret field measurements and for future air quality studies.
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.
Fu-Jie Zhu, Zi-Feng Zhang, Li-Yan Liu, Pu-Fei Yang, Peng-Tuan Hu, Geng-Bo Ren, Meng Qin, and Wan-Li Ma
EGUsphere, https://doi.org/10.5194/egusphere-2023-2376, https://doi.org/10.5194/egusphere-2023-2376, 2023
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Gas/particle partitioning is an important atmospheric behavior for SVOCs. The observation of that the gaseous degradation could disrupt the equilibrium state of gas/particle partitioning of low molecular weight SVOCs, was demonstrated and evaluated by a steady-state model, with increasing gas/particle partitioning quotients about 1 to 8.4 times. The present study suggested the interplay between degradation and G/P partitioning of SVOCs.
M. Omar Nawaz, Jeremiah Johnson, Greg Yarwood, Benjamin de Foy, Laura M. Judd, and Daniel L. Goldberg
EGUsphere, https://doi.org/10.5194/egusphere-2023-2844, https://doi.org/10.5194/egusphere-2023-2844, 2023
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NO2 is a gas with implications for air pollution. An air campaign conducted in Houston provided an opportunity to compare NO2 from different instruments and a model. Observations from aircrafts and the TROPOMI satellite instrument agreed well with measurements on the ground, however the latter estimated lower values. We find that NO2 simulated in our model performed worse and find the worst performance in downtown Houston, suggesting that vehicle emissions of NO2 may be underestimated.
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.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, Andy Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
EGUsphere, https://doi.org/10.5194/egusphere-2023-2742, https://doi.org/10.5194/egusphere-2023-2742, 2023
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Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represent VOCs chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from Volatile Chemical Products and other anthropogenic sources to total VOC reactivity and O3.
Christoph Staehle, Harald E. Rieder, and Arlene M. Fiore
EGUsphere, https://doi.org/10.5194/egusphere-2023-2743, https://doi.org/10.5194/egusphere-2023-2743, 2023
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Chemistry-climate models show biases compared to surface ozone observations, and thus require bias-correction for impact studies and the assessment of air quality changes. We compare the performance of commonly used correction techniques for model outputs available via CMIP6. While all methods can reduce model biases, better results are obtained for more complex approaches. Thus, our study suggests broader use of these techniques in studies seeking to inform air quality management and policy.
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.
Jianghao Li, Alastair C. Lewis, Jim R. Hopkins, Stephen J. Andrews, Tim Murrells, Neil Passant, Ben Richmond, Siqi Hou, William Bloss, Roy Harrison, and Zongbo Shi
EGUsphere, https://doi.org/10.5194/egusphere-2023-2294, https://doi.org/10.5194/egusphere-2023-2294, 2023
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A summertime ozone event at an urban site in Birmingham is sensitive to volatile organic compound (VOCs), particularly those of oxygenated VOCs. The roles of anthropogenic VOC sources in urban ozone chemistry are examined by integrating the 1990–2019 national atmospheric emission inventory into model scenarios. Road transport remains the most powerful means to further reduce ozone in this case study, but the benefits maybe offset if solvent emission of VOCs were to continue to increase.
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.
David de la Paz, Rafael Borge, Juan Manuel de Andrés, Luis Miguel Tovar, Golam Sarwar, and Sergey L. Napelenok
EGUsphere, https://doi.org/10.5194/egusphere-2023-2056, https://doi.org/10.5194/egusphere-2023-2056, 2023
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This modelling study shows that around 70 % of ground-level ozone (O3) in Madrid (Spain) is transported from other regions. Nonetheless, local sources, mainly road traffic, play a significant role, specially under stagnation conditions associated to regional air recirculation. Our results suggest that local measures may be effective to reduce O3 peaks (potentially, up to 30 %) and thus, reduce impacts from high-O3 episodes in the Madrid metropolitan area.
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.
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.
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.
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Short summary
We use satellite observations and chemical transport modeling to quantify sources of NOx, a major air pollutant, over the past decade. We find improved simulations of the magnitude, seasonality, and trends of NO2 and ozone concentrations using these derived emissions. Changes in ozone pollution driven by human and natural sources are identified in different regions. This work shows the benefits of remote-sensing data and inverse modeling for more accurate ozone simulations.
We use satellite observations and chemical transport modeling to quantify sources of NOx, a...
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