Articles | Volume 12, issue 7
https://doi.org/10.5194/gmd-12-2983-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/gmd-12-2983-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Development and technical paper
| 
15 Jul 2019
Development and technical paper |
| 15 Jul 2019
| 15 Jul 2019
A simplified parameterization of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX-SOA) for global chemistry and climate models: a case study with GEOS-Chem v11-02-rc
Duseong S. Jo
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, CO, USA
Department of Chemistry, University of Colorado, Boulder, CO, USA
Alma Hodzic
Atmospheric Chemistry Observations and Modeling Lab., National Center for Atmospheric Research, Boulder, CO, USA
Laboratoire d'Aérologie, Université de Toulouse, CNRS, UPS,
Toulouse, France
Louisa K. Emmons
Atmospheric Chemistry Observations and Modeling Lab., National Center for Atmospheric Research, Boulder, CO, USA
Eloise A. Marais
Department of Physics and Astronomy, University of Leicester,
Leicester, UK
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, CO, USA
Department of Chemistry, University of Colorado, Boulder, CO, USA
Benjamin A. Nault
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, CO, USA
Department of Chemistry, University of Colorado, Boulder, CO, USA
Weiwei Hu
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, CO, USA
Department of Chemistry, University of Colorado, Boulder, CO, USA
Pedro Campuzano-Jost
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, CO, USA
Department of Chemistry, University of Colorado, Boulder, CO, USA
Jose L. Jimenez
CORRESPONDING AUTHOR
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, CO, USA
Department of Chemistry, University of Colorado, Boulder, CO, USA
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This study finds that one component of secondary inorganic aerosols, nitrate, is greatly overestimated by a global atmospheric chemistry model compared to observations from 11 flight campaigns. None of the loss and production pathways explored can explain the nitrate bias alone. The model’s inability to capture the variability in the observations remains and requires future investigation to avoid biases in policy-related studies (i.e., air quality, health, climate impacts of these aerosols).
Jerome D. Fast, Adam C. Varble, Fan Mei, Mikhail Pekour, Jason Tomlinson, Alla Zelenyuk, Art J. Sedlacek III, Maria Zawadowicz, and Louisa Emmons
Atmos. Chem. Phys., 24, 13477–13502, https://doi.org/10.5194/acp-24-13477-2024, https://doi.org/10.5194/acp-24-13477-2024, 2024
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Aerosol property measurements recently collected on the ground and by a research aircraft in central Argentina during the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) campaign exhibit large spatial and temporal variability. These measurements coupled with coincident meteorological information provide a valuable data set needed to evaluate and improve model predictions of aerosols in a traditionally data-sparse region of South America.
William J. Collins, Fiona M. O'Connor, Connor R. Barker, Rachael E. Byrom, Sebastian D. Eastham, Øivind Hodnebrog, Patrick Jöckel, Eloise A. Marais, Mariano Mertens, Gunnar Myhre, Matthias Nützel, Dirk Olivié, Ragnhild Bieltvedt Skeie, Laura Stecher, Larry W. Horowitz, Vaishali Naik, Gregory Faluvegi, Ulas Im, Lee T. Murray, Drew Shindell, Kostas Tsigaridis, Nathan Luke Abraham, and James Keeble
EGUsphere, https://doi.org/10.5194/egusphere-2024-3698, https://doi.org/10.5194/egusphere-2024-3698, 2024
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If reductions aren’t implemented to limit emissions of pollutants that produce ozone then we calculate that this will cause a warming of climate. We assess how the future warming from ozone is affected by changing meteorological variables such as clouds and atmospheric temperatures. We find that reductions in high cloud cover tend to slightly reduce the warming from ozone.
Mingfu Cai, Chenshuo Ye, Bin Yuan, Shan Huang, E Zheng, Suxia Yang, Zelong Wang, Yi Lin, Tiange Li, Weiwei Hu, Wei Chen, Qicong Song, Wei Li, Yuwen Peng, Baoling Liang, Qibin Sun, Jun Zhao, Duohong Chen, Jiaren Sun, Zhiyong Yang, and Min Shao
Atmos. Chem. Phys., 24, 13065–13079, https://doi.org/10.5194/acp-24-13065-2024, https://doi.org/10.5194/acp-24-13065-2024, 2024
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This study investigated the daytime secondary organic aerosol (SOA) formation in urban plumes. We observed a significant daytime SOA formation through gas–particle partitioning when the site was affected by urban plumes. A box model simulation indicated that urban pollutants (nitrogen oxide and volatile organic compounds) could enhance the oxidizing capacity, while the elevated volatile organic compounds were mainly responsible for promoting daytime SOA formation.
Rebekah P. Horner, Eloise A. Marais, Nana Wei, Robert G. Ryan, and Viral Shah
Atmos. Chem. Phys., 24, 13047–13064, https://doi.org/10.5194/acp-24-13047-2024, https://doi.org/10.5194/acp-24-13047-2024, 2024
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Nitrogen oxides (NOx ≡ NO + NO2) affect tropospheric ozone and the hydroxyl radical, influencing climate and atmospheric oxidation. To address the lack of routine observations of NOx, we cloud slice satellite observations of NO2 to derive a new dataset of global vertical profiles of NO2. We evaluate our data against in situ aircraft observations and use these data to critique the contemporary understanding of tropospheric NOx, as simulated by the GEOS-Chem model.
Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Wenxiang Shen, Stephen R. Arnold, Leighton A. Regayre, Meinrat O. Andreae, Mira L. Pöhlker, Duseong S. Jo, Man Yue, and Ken S. Carslaw
Atmos. Chem. Phys., 24, 11365–11389, https://doi.org/10.5194/acp-24-11365-2024, https://doi.org/10.5194/acp-24-11365-2024, 2024
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Highly oxygenated organic molecules (HOMs) play an important role in atmospheric new particle formation (NPF). By semi-explicitly coupling the chemical mechanism of HOMs and a comprehensive nucleation scheme in a global climate model, the updated model shows better agreement with measurements of nucleation rate, growth rate, and NPF event frequency. Our results reveal that HOM-driven NPF leads to a considerable increase in particle and cloud condensation nuclei burden globally.
Kouji Adachi, Jack E. Dibb, Joseph M. Katich, Joshua P. Schwarz, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Jeff Peischl, Christopher D. Holmes, and James Crawford
Atmos. Chem. Phys., 24, 10985–11004, https://doi.org/10.5194/acp-24-10985-2024, https://doi.org/10.5194/acp-24-10985-2024, 2024
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We examined aerosol particles from wildfires and identified tarballs (TBs) from the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign. This study reveals the compositions, abundance, sizes, and mixing states of TBs and shows that TBs formed as the smoke aged for up to 5 h. This study provides measurements of TBs from various biomass-burning events and ages, enhancing our knowledge of TB emissions and our understanding of their climate impact.
Benjamin A. Nault, Katherine R. Travis, James H. Crawford, Donald R. Blake, Pedro Campuzano-Jost, Ronald C. Cohen, Joshua P. DiGangi, Glenn S. Diskin, Samuel R. Hall, L. Gregory Huey, Jose L. Jimenez, Kyung-Eun Min, Young Ro Lee, Isobel J. Simpson, Kirk Ullmann, and Armin Wisthaler
Atmos. Chem. Phys., 24, 9573–9595, https://doi.org/10.5194/acp-24-9573-2024, https://doi.org/10.5194/acp-24-9573-2024, 2024
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Ozone (O3) is a pollutant formed from the reactions of gases emitted from various sources. In urban areas, the density of human activities can increase the O3 formation rate (P(O3)), thus impacting air quality and health. Observations collected over Seoul, South Korea, are used to constrain P(O3). A high local P(O3) was found; however, local P(O3) was partly reduced due to compounds typically ignored. These observations also provide constraints for unmeasured compounds that will impact P(O3).
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
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Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Tianle Pan, Andrew T. Lambe, Weiwei Hu, Yicong He, Minghao Hu, Huaishan Zhou, Xinming Wang, Qingqing Hu, Hui Chen, Yue Zhao, Yuanlong Huang, Doug R. Worsnop, Zhe Peng, Melissa A. Morris, Douglas A. Day, Pedro Campuzano-Jost, Jose-Luis Jimenez, and Shantanu H. Jathar
Atmos. Meas. Tech., 17, 4915–4939, https://doi.org/10.5194/amt-17-4915-2024, https://doi.org/10.5194/amt-17-4915-2024, 2024
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This study systematically characterizes the temperature enhancement in the lamp-enclosed oxidation flow reactor (OFR). The enhancement varied multiple dimensional factors, emphasizing the complexity of temperature inside of OFR. The effects of temperature on the flow field and gas- or particle-phase reaction inside OFR were also evaluated with experiments and model simulations. Finally, multiple mitigation strategies were demonstrated to minimize this temperature increase.
David P. Edwards, Sara Martínez-Alonso, Duseong S. Jo, Ivan Ortega, Louisa K. Emmons, John J. Orlando, Helen M. Worden, Jhoon Kim, Hanlim Lee, Junsung Park, and Hyunkee Hong
Atmos. Chem. Phys., 24, 8943–8961, https://doi.org/10.5194/acp-24-8943-2024, https://doi.org/10.5194/acp-24-8943-2024, 2024
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Until recently, satellite observations of atmospheric pollutants at any location could only be obtained once a day. New geostationary satellites stare at a region of the Earth to make hourly measurements, and the Geostationary Environment Monitoring Spectrometer is the first looking at Asia. These data and model simulations show how the change seen for one important pollutant that determines air quality depends on a combination of pollution emissions, atmospheric chemistry, and meteorology.
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
Atmos. Chem. Phys., 24, 8607–8624, https://doi.org/10.5194/acp-24-8607-2024, https://doi.org/10.5194/acp-24-8607-2024, 2024
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Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone, but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side by side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
Melinda K. Schueneman, Douglas A. Day, Dongwook Kim, Pedro Campuzano-Jost, Seonsik Yun, Marla P. DeVault, Anna C. Ziola, Paul J. Ziemann, and Jose L. Jimenez
Aerosol Research, 2, 59–76, https://doi.org/10.5194/ar-2-59-2024, https://doi.org/10.5194/ar-2-59-2024, 2024
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Our study presents a novel method for quantifying mass spectrometer responses to molecular species in organic aerosols. Traditional calibrations often fail for complex mixtures like secondary organic aerosol. We combined chromatography with statistical component analysis to improve separation and quantification, achieving promising agreement with direct calibration. Our findings offer a new approach to assess aerosol composition, especially beneficial for complex mixtures.
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 4809–4826, https://doi.org/10.5194/acp-24-4809-2024, https://doi.org/10.5194/acp-24-4809-2024, 2024
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Secondary organic aerosols (SOAs) can exist in liquid, semi-solid, or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
Wenfu Tang, Benjamin Gaubert, Louisa Emmons, Daniel Ziskin, Debbie Mao, David Edwards, Avelino Arellano, Kevin Raeder, Jeffrey Anderson, and Helen Worden
Atmos. Meas. Tech., 17, 1941–1963, https://doi.org/10.5194/amt-17-1941-2024, https://doi.org/10.5194/amt-17-1941-2024, 2024
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We assimilate different MOPITT CO products to understand the impact of (1) assimilating multispectral and joint retrievals versus single spectral products, (2) assimilating satellite profile products versus column products, and (3) assimilating multispectral and joint retrievals versus assimilating individual products separately.
Melissa A. Morris, Demetrios Pagonis, Douglas A. Day, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 17, 1545–1559, https://doi.org/10.5194/amt-17-1545-2024, https://doi.org/10.5194/amt-17-1545-2024, 2024
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Polymer absorption of volatile organic compounds (VOCs) is important to characterize for atmospheric sampling setups (as interactions cause sampling delays) and indoor air quality. Here we test different polymer materials and quantify their absorptive capacities through modeling. We found the main polymers in carpets to be highly absorptive, acting as large reservoirs for indoor pollution. We also demonstrated how polymer tubes can be used as a low-cost gas separation technique.
Kyoung-Min Kim, Si-Wan Kim, Seunghwan Seo, Donald R. Blake, Seogju Cho, James H. Crawford, Louisa K. Emmons, Alan Fried, Jay R. Herman, Jinkyu Hong, Jinsang Jung, Gabriele G. Pfister, Andrew J. Weinheimer, Jung-Hun Woo, and Qiang Zhang
Geosci. Model Dev., 17, 1931–1955, https://doi.org/10.5194/gmd-17-1931-2024, https://doi.org/10.5194/gmd-17-1931-2024, 2024
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Three emission inventories were evaluated for East Asia using data acquired during a field campaign in 2016. The inventories successfully reproduced the daily variations of ozone and nitrogen dioxide. However, the spatial distributions of model ozone did not fully agree with the observations. Additionally, all simulations underestimated carbon monoxide and volatile organic compound (VOC) levels. Increasing VOC emissions over South Korea resulted in improved ozone simulations.
Huisheng Bian, Mian Chin, Peter R. Colarco, Eric C. Apel, Donald R. Blake, Karl Froyd, Rebecca S. Hornbrook, Jose Jimenez, Pedro Campuzano Jost, Michael Lawler, Mingxu Liu, Marianne Tronstad Lund, Hitoshi Matsui, Benjamin A. Nault, Joyce E. Penner, Andrew W. Rollins, Gregory Schill, Ragnhild B. Skeie, Hailong Wang, Lu Xu, Kai Zhang, and Jialei Zhu
Atmos. Chem. Phys., 24, 1717–1741, https://doi.org/10.5194/acp-24-1717-2024, https://doi.org/10.5194/acp-24-1717-2024, 2024
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This work studies sulfur in the remote troposphere at global and seasonal scales using aircraft measurements and multi-model simulations. The goal is to understand the sulfur cycle over remote oceans, spread of model simulations, and observation–model discrepancies. Such an understanding and comparison with real observations are crucial to narrow down the uncertainties in model sulfur simulations and improve understanding of the sulfur cycle in atmospheric air quality, climate, and ecosystems.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
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This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
Sohyeon Jeon, Michael J. Walker, Donna T. Sueper, Douglas A. Day, Anne V. Handschy, Jose L. Jimenez, and Brent J. Williams
Atmos. Meas. Tech., 16, 6075–6095, https://doi.org/10.5194/amt-16-6075-2023, https://doi.org/10.5194/amt-16-6075-2023, 2023
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A searchable database tool for the Aerosol Mass Spectrometer (AMS) and Aerosol Chemical Speciation Monitor (ACSM) mass spectral datasets was built to improve the efficiency of data analysis using Igor Pro. The tool incorporates the published mass spectra (MS) and sample information uploaded on the website. The tool allows users to compare their own mass spectrum with the reference MS in the database.
Abd El Rahman El Mais, Barbara D'Anna, Luka Drinovec, Andrew T. Lambe, Zhe Peng, Jean-Eudes Petit, Olivier Favez, Selim Aït-Aïssa, and Alexandre Albinet
Atmos. Chem. Phys., 23, 15077–15096, https://doi.org/10.5194/acp-23-15077-2023, https://doi.org/10.5194/acp-23-15077-2023, 2023
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Polycyclic aromatic hydrocarbons (PAHS) and furans are key precursors of secondary organic aerosols (SOAs) related to biomass burning emissions. We evaluated and compared the formation yields, and the physical and light absorption properties, of laboratory-generated SOAs from the oxidation of such compounds for both, day- and nighttime reactivities. The results illustrate that PAHs are large SOA precursors and may contribute significantly to the biomass burning brown carbon in the atmosphere.
Wenfu Tang, Louisa K. Emmons, Helen M. Worden, Rajesh Kumar, Cenlin He, Benjamin Gaubert, Zhonghua Zheng, Simone Tilmes, Rebecca R. Buchholz, Sara-Eva Martinez-Alonso, Claire Granier, Antonin Soulie, Kathryn McKain, Bruce C. Daube, Jeff Peischl, Chelsea Thompson, and Pieternel Levelt
Geosci. Model Dev., 16, 6001–6028, https://doi.org/10.5194/gmd-16-6001-2023, https://doi.org/10.5194/gmd-16-6001-2023, 2023
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The new MUSICAv0 model enables the study of atmospheric chemistry across all relevant scales. We develop a MUSICAv0 grid for Africa. We evaluate MUSICAv0 with observations and compare it with a previously used model – WRF-Chem. Overall, the performance of MUSICAv0 is comparable to WRF-Chem. Based on model–satellite discrepancies, we find that future field campaigns in an eastern African region (30°E–45°E, 5°S–5°N) could substantially improve the predictive skill of air quality models.
Maria Val Martin, Elena Blanc-Betes, Ka Ming Fung, Euripides P. Kantzas, Ilsa B. Kantola, Isabella Chiaravalloti, Lyla L. Taylor, Louisa K. Emmons, William R. Wieder, Noah J. Planavsky, Michael D. Masters, Evan H. DeLucia, Amos P. K. Tai, and David J. Beerling
Geosci. Model Dev., 16, 5783–5801, https://doi.org/10.5194/gmd-16-5783-2023, https://doi.org/10.5194/gmd-16-5783-2023, 2023
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Enhanced rock weathering (ERW) is a CO2 removal strategy that involves applying crushed rocks (e.g., basalt) to agricultural soils. However, unintended processes within the N cycle due to soil pH changes may affect the climate benefits of C sequestration. ERW could drive changes in soil emissions of non-CO2 GHGs (N2O) and trace gases (NO and NH3) that may affect air quality. We present a new improved N cycling scheme for the land model (CLM5) to evaluate ERW effects on soil gas N emissions.
Yiyu Cai, Chenshuo Ye, Wei Chen, Weiwei Hu, Wei Song, Yuwen Peng, Shan Huang, Jipeng Qi, Sihang Wang, Chaomin Wang, Caihong Wu, Zelong Wang, Baolin Wang, Xiaofeng Huang, Lingyan He, Sasho Gligorovski, Bin Yuan, Min Shao, and Xinming Wang
Atmos. Chem. Phys., 23, 8855–8877, https://doi.org/10.5194/acp-23-8855-2023, https://doi.org/10.5194/acp-23-8855-2023, 2023
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We studied the variability and molecular composition of ambient oxidized organic nitrogen (OON) in both gas and particle phases using a state-of-the-art online mass spectrometer in urban air. Biomass burning and secondary formation were found to be the two major sources of OON. Daytime nitrate radical chemistry for OON formation was more important than previously thought. Our results improved the understanding of the sources and molecular composition of OON in the polluted urban atmosphere.
Kevin J. Nihill, Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Bin Yuan, Jordan E. Krechmer, Kanako Sekimoto, Jose L. Jimenez, Joost de Gouw, Christopher D. Cappa, Colette L. Heald, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 23, 7887–7899, https://doi.org/10.5194/acp-23-7887-2023, https://doi.org/10.5194/acp-23-7887-2023, 2023
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In this work, we collect emissions from controlled burns of biomass fuels that can be found in the western United States into an environmental chamber in order to simulate their oxidation as they pass through the atmosphere. These findings provide a detailed characterization of the composition of the atmosphere downwind of wildfires. In turn, this will help to explore the effects of these changing emissions on downwind populations and will also directly inform atmospheric and climate models.
Christine Wiedinmyer, Yosuke Kimura, Elena C. McDonald-Buller, Louisa K. Emmons, Rebecca R. Buchholz, Wenfu Tang, Keenan Seto, Maxwell B. Joseph, Kelley C. Barsanti, Annmarie G. Carlton, and Robert Yokelson
Geosci. Model Dev., 16, 3873–3891, https://doi.org/10.5194/gmd-16-3873-2023, https://doi.org/10.5194/gmd-16-3873-2023, 2023
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The Fire INventory from NCAR (FINN) provides daily global estimates of emissions from open fires based on satellite detections of hot spots. This version has been updated to apply MODIS and VIIRS satellite fire detection and better represents both large and small fires. FINNv2.5 generates more emissions than FINNv1 and is in general agreement with other fire emissions inventories. The new estimates are consistent with satellite observations, but uncertainties remain regionally and by pollutant.
Duseong S. Jo, Simone Tilmes, Louisa K. Emmons, Siyuan Wang, and Francis Vitt
Geosci. Model Dev., 16, 3893–3906, https://doi.org/10.5194/gmd-16-3893-2023, https://doi.org/10.5194/gmd-16-3893-2023, 2023
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A new simple secondary organic aerosol (SOA) scheme has been developed for the Community Atmosphere Model (CAM) based on the complex SOA scheme in CAM with detailed chemistry (CAM-chem). The CAM with the new SOA scheme shows better agreements with CAM-chem in terms of aerosol concentrations and radiative fluxes, which ensures more consistent results between different compsets in the Community Earth System Model. The new SOA scheme also has technical advantages for future developments.
Robert G. Ryan, Eloise A. Marais, Eleanor Gershenson-Smith, Robbie Ramsay, Jan-Peter Muller, Jan-Lukas Tirpitz, and Udo Frieß
Atmos. Chem. Phys., 23, 7121–7139, https://doi.org/10.5194/acp-23-7121-2023, https://doi.org/10.5194/acp-23-7121-2023, 2023
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We describe the first data retrieval from a newly installed instrument providing measurements of vertical profiles of air pollution over Central London during heatwaves in summer 2022. We use these observations with surface air quality network measurements to support interpretation that an exponential increase in biogenic emissions of isoprene during heatwaves provides the limiting ingredient for severe ozone pollution, leading to non-compliance with the national ozone air quality standard.
Wenfu Tang, Simone Tilmes, David M. Lawrence, Fang Li, Cenlin He, Louisa K. Emmons, Rebecca R. Buchholz, and Lili Xia
Atmos. Chem. Phys., 23, 5467–5486, https://doi.org/10.5194/acp-23-5467-2023, https://doi.org/10.5194/acp-23-5467-2023, 2023
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Globally, total wildfire burned area is projected to increase over the 21st century under scenarios without geoengineering and decrease under the two geoengineering scenarios. Geoengineering reduces fire by decreasing surface temperature and wind speed and increasing relative humidity and soil water. However, geoengineering also yields reductions in precipitation, which offset some of the fire reduction.
Haihui Zhu, Randall V. Martin, Betty Croft, Shixian Zhai, Chi Li, Liam Bindle, Jeffrey R. Pierce, Rachel Y.-W. Chang, Bruce E. Anderson, Luke D. Ziemba, Johnathan W. Hair, Richard A. Ferrare, Chris A. Hostetler, Inderjeet Singh, Deepangsu Chatterjee, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jack E. Dibb, Joshua S. Schwarz, and Andrew Weinheimer
Atmos. Chem. Phys., 23, 5023–5042, https://doi.org/10.5194/acp-23-5023-2023, https://doi.org/10.5194/acp-23-5023-2023, 2023
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Particle size of atmospheric aerosol is important for estimating its climate and health effects, but simulating atmospheric aerosol size is computationally demanding. This study derives a simple parameterization of the size of organic and secondary inorganic ambient aerosol that can be applied to atmospheric models. Applying this parameterization allows a better representation of the global spatial pattern of aerosol size, as verified by ground and airborne measurements.
Laura Tomsche, Felix Piel, Tomas Mikoviny, Claus J. Nielsen, Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Melinda K. Schueneman, Jose L. Jimenez, Hannah Halliday, Glenn Diskin, Joshua P. DiGangi, John B. Nowak, Elizabeth B. Wiggins, Emily Gargulinski, Amber J. Soja, and Armin Wisthaler
Atmos. Chem. Phys., 23, 2331–2343, https://doi.org/10.5194/acp-23-2331-2023, https://doi.org/10.5194/acp-23-2331-2023, 2023
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Ammonia (NH3) is an important trace gas in the atmosphere and fires are among the poorly investigated sources. During the 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) aircraft campaign, we measured gaseous NH3 and particulate ammonium (NH4+) in smoke plumes emitted from 6 wildfires in the Western US and 66 small agricultural fires in the Southeastern US. We herein present a comprehensive set of emission factors of NH3 and NHx, where NHx = NH3 + NH4+.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
Tingting Feng, Yingkun Wang, Weiwei Hu, Ming Zhu, Wei Song, Wei Chen, Yanyan Sang, Zheng Fang, Wei Deng, Hua Fang, Xu Yu, Cheng Wu, Bin Yuan, Shan Huang, Min Shao, Xiaofeng Huang, Lingyan He, Young Ro Lee, Lewis Gregory Huey, Francesco Canonaco, Andre S. H. Prevot, and Xinming Wang
Atmos. Chem. Phys., 23, 611–636, https://doi.org/10.5194/acp-23-611-2023, https://doi.org/10.5194/acp-23-611-2023, 2023
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To investigate the impact of aging processes on organic aerosols (OA), we conducted a comprehensive field study at a continental remote site using an on-line mass spectrometer. The results show that OA in the Chinese outflows were strongly influenced by upwind anthropogenic emissions. The aging processes can significantly decrease the OA volatility and result in a varied viscosity of OA under different circumstances, signifying the complex physiochemical properties of OA in aged plumes.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Pamela S. Rickly, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Glenn M. Wolfe, Ryan Bennett, Ilann Bourgeois, John D. Crounse, Jack E. Dibb, Joshua P. DiGangi, Glenn S. Diskin, Maximilian Dollner, Emily M. Gargulinski, Samuel R. Hall, Hannah S. Halliday, Thomas F. Hanisco, Reem A. Hannun, Jin Liao, Richard Moore, Benjamin A. Nault, John B. Nowak, Jeff Peischl, Claire E. Robinson, Thomas Ryerson, Kevin J. Sanchez, Manuel Schöberl, Amber J. Soja, Jason M. St. Clair, Kenneth L. Thornhill, Kirk Ullmann, Paul O. Wennberg, Bernadett Weinzierl, Elizabeth B. Wiggins, Edward L. Winstead, and Andrew W. Rollins
Atmos. Chem. Phys., 22, 15603–15620, https://doi.org/10.5194/acp-22-15603-2022, https://doi.org/10.5194/acp-22-15603-2022, 2022
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Biomass burning sulfur dioxide (SO2) emission factors range from 0.27–1.1 g kg-1 C. Biomass burning SO2 can quickly form sulfate and organosulfur, but these pathways are dependent on liquid water content and pH. Hydroxymethanesulfonate (HMS) appears to be directly emitted from some fire sources but is not the sole contributor to the organosulfur signal. It is shown that HMS and organosulfur chemistry may be an important S(IV) reservoir with the fate dependent on the surrounding conditions.
Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Haipeng Lin, Elizabeth W. Lundgren, Steve Goldhaber, Steven R. H. Barrett, and Daniel J. Jacob
Geosci. Model Dev., 15, 8669–8704, https://doi.org/10.5194/gmd-15-8669-2022, https://doi.org/10.5194/gmd-15-8669-2022, 2022
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We bring the state-of-the-science chemistry module GEOS-Chem into the Community Earth System Model (CESM). We show that some known differences between results from GEOS-Chem and CESM's CAM-chem chemistry module may be due to the configuration of model meteorology rather than inherent differences in the model chemistry. This is a significant step towards a truly modular Earth system model and allows two strong but currently separate research communities to benefit from each other's advances.
Haichao Wang, Bin Yuan, E Zheng, Xiaoxiao Zhang, Jie Wang, Keding Lu, Chenshuo Ye, Lei Yang, Shan Huang, Weiwei Hu, Suxia Yang, Yuwen Peng, Jipeng Qi, Sihang Wang, Xianjun He, Yubin Chen, Tiange Li, Wenjie Wang, Yibo Huangfu, Xiaobing Li, Mingfu Cai, Xuemei Wang, and Min Shao
Atmos. Chem. Phys., 22, 14837–14858, https://doi.org/10.5194/acp-22-14837-2022, https://doi.org/10.5194/acp-22-14837-2022, 2022
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We present intensive field measurement of ClNO2 in the Pearl River Delta in 2019. Large variation in the level, formation, and atmospheric impacts of ClNO2 was found in different air masses. ClNO2 formation was limited by the particulate chloride (Cl−) and aerosol surface area. Our results reveal that Cl− originated from various anthropogenic emissions rather than sea sources and show minor contribution to the O3 pollution and photochemistry.
Longlei Li, Natalie M. Mahowald, Jasper F. Kok, Xiaohong Liu, Mingxuan Wu, Danny M. Leung, Douglas S. Hamilton, Louisa K. Emmons, Yue Huang, Neil Sexton, Jun Meng, and Jessica Wan
Geosci. Model Dev., 15, 8181–8219, https://doi.org/10.5194/gmd-15-8181-2022, https://doi.org/10.5194/gmd-15-8181-2022, 2022
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This study advances mineral dust parameterizations in the Community Atmospheric Model (CAM; version 6.1). Efforts include 1) incorporating a more physically based dust emission scheme; 2) updating the dry deposition scheme; and 3) revising the gravitational settling velocity to account for dust asphericity. Substantial improvements achieved with these updates can help accurately quantify dust–climate interactions using CAM, such as the dust-radiation and dust–cloud interactions.
Youhua Tang, Patrick C. Campbell, Pius Lee, Rick Saylor, Fanglin Yang, Barry Baker, Daniel Tong, Ariel Stein, Jianping Huang, Ho-Chun Huang, Li Pan, Jeff McQueen, Ivanka Stajner, Jose Tirado-Delgado, Youngsun Jung, Melissa Yang, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Donald Blake, Joshua Schwarz, Jose-Luis Jimenez, James Crawford, Glenn Diskin, Richard Moore, Johnathan Hair, Greg Huey, Andrew Rollins, Jack Dibb, and Xiaoyang Zhang
Geosci. Model Dev., 15, 7977–7999, https://doi.org/10.5194/gmd-15-7977-2022, https://doi.org/10.5194/gmd-15-7977-2022, 2022
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This paper compares two meteorological datasets for driving a regional air quality model: a regional meteorological model using WRF (WRF-CMAQ) and direct interpolation from an operational global model (GFS-CMAQ). In the comparison with surface measurements and aircraft data in summer 2019, these two methods show mixed performance depending on the corresponding meteorological settings. Direct interpolation is found to be a viable method to drive air quality models.
Nicole A. June, Anna L. Hodshire, Elizabeth B. Wiggins, Edward L. Winstead, Claire E. Robinson, K. Lee Thornhill, Kevin J. Sanchez, Richard H. Moore, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Matthew M. Coggon, Jonathan M. Dean-Day, T. Paul Bui, Jeff Peischl, Robert J. Yokelson, Matthew J. Alvarado, Sonia M. Kreidenweis, Shantanu H. Jathar, and Jeffrey R. Pierce
Atmos. Chem. Phys., 22, 12803–12825, https://doi.org/10.5194/acp-22-12803-2022, https://doi.org/10.5194/acp-22-12803-2022, 2022
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The evolution of organic aerosol composition and size is uncertain due to variability within and between smoke plumes. We examine the impact of plume concentration on smoke evolution from smoke plumes sampled by the NASA DC-8 during FIREX-AQ. We find that observed organic aerosol and size distribution changes are correlated to plume aerosol mass concentrations. Additionally, coagulation explains the majority of the observed growth.
Biao Luo, Ye Kuang, Shan Huang, Qicong Song, Weiwei Hu, Wei Li, Yuwen Peng, Duohong Chen, Dingli Yue, Bin Yuan, and Min Shao
Atmos. Chem. Phys., 22, 12401–12415, https://doi.org/10.5194/acp-22-12401-2022, https://doi.org/10.5194/acp-22-12401-2022, 2022
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We performed comprehensive analysis on biomass burning organic aerosol (BBOA) size distributions, as well as mass scattering and absorption efficiencies, with an improved method of on-line quantification of brown carbon absorptions. Both BBOA volume size distribution and retrieved refractive index depend highly on combustion conditions represented by the black carbon content, which has significant implications for BBOA climate effect simulations.
Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah A. Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, Benjamin A. Nault, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech., 15, 4901–4930, https://doi.org/10.5194/amt-15-4901-2022, https://doi.org/10.5194/amt-15-4901-2022, 2022
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Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
Andrea Mazzeo, Michael Burrow, Andrew Quinn, Eloise A. Marais, Ajit Singh, David Ng'ang'a, Michael J. Gatari, and Francis D. Pope
Atmos. Chem. Phys., 22, 10677–10701, https://doi.org/10.5194/acp-22-10677-2022, https://doi.org/10.5194/acp-22-10677-2022, 2022
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A modelling system for meteorology and chemistry transport processes, WRF–CHIMERE, has been tested and validated for three East African conurbations using the most up-to-date anthropogenic emissions available. Results show that the model is able to reproduce hourly and daily temporal variabilities in aerosol concentrations that are close to observations in both urban and rural environments, encouraging the adoption of numerical modelling as a tool for air quality management in East Africa.
Aditya Kumar, R. Bradley Pierce, Ravan Ahmadov, Gabriel Pereira, Saulo Freitas, Georg Grell, Chris Schmidt, Allen Lenzen, Joshua P. Schwarz, Anne E. Perring, Joseph M. Katich, John Hair, Jose L. Jimenez, Pedro Campuzano-Jost, and Hongyu Guo
Atmos. Chem. Phys., 22, 10195–10219, https://doi.org/10.5194/acp-22-10195-2022, https://doi.org/10.5194/acp-22-10195-2022, 2022
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We use the WRF-Chem model with new implementations of GOES-16 wildfire emissions and plume rise based on fire radiative power (FRP) to interpret aerosol observations during the 2019 NASA–NOAA FIREX-AQ field campaign and perform model evaluations. The model shows significant improvements in simulating the variety of aerosol loading environments sampled during FIREX-AQ. Our results also highlight the importance of accurate wildfire diurnal cycle and aerosol chemical mechanisms in models.
Yihang Yu, Peng Cheng, Huirong Li, Wenda Yang, Baobin Han, Wei Song, Weiwei Hu, Xinming Wang, Bin Yuan, Min Shao, Zhijiong Huang, Zhen Li, Junyu Zheng, Haichao Wang, and Xiaofang Yu
Atmos. Chem. Phys., 22, 8951–8971, https://doi.org/10.5194/acp-22-8951-2022, https://doi.org/10.5194/acp-22-8951-2022, 2022
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We have investigated the budget of HONO at an urban site in Guangzhou. Budget and comprehensive uncertainty analysis suggest that at such locations as ours, HONO direct emissions and NO + OH can become comparable or even surpass other HONO sources that typically receive greater attention and interest, such as the NO2 heterogeneous source and the unknown daytime photolytic source. Our findings emphasize the need to reduce the uncertainties of both conventional and novel HONO sources and sinks.
Jean-Pierre Chaboureau, Laurent Labbouz, Cyrille Flamant, and Alma Hodzic
Atmos. Chem. Phys., 22, 8639–8658, https://doi.org/10.5194/acp-22-8639-2022, https://doi.org/10.5194/acp-22-8639-2022, 2022
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Ground-based, spaceborne and rare airborne observations of biomass burning aerosols (BBAs) during the AEROCLO-sA field campaign in 2017 are complemented with convection-permitting simulations with online trajectories. The results show that the radiative effect of the BBA accelerates the southern African easterly jet and generates upward motions that transport the BBAs to higher altitudes and farther southwest.
Marios Panagi, Roberto Sommariva, Zoë L. Fleming, Paul S. Monks, Gongda Lu, Eloise A. Marais, James R. Hopkins, Alastair C. Lewis, Qiang Zhang, James D. Lee, Freya A. Squires, Lisa K. Whalley, Eloise J. Slater, Dwayne E. Heard, Robert Woodward-Massey, Chunxiang Ye, and Joshua D. Vande Hey
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-379, https://doi.org/10.5194/acp-2022-379, 2022
Revised manuscript not accepted
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A dispersion model and a box model were combined to investigate the evolution of VOCs in Beijing once they are emitted from anthropogenic sources. It was determined that during the winter time the VOC concentrations in Beijing are driven predominantly by sources within Beijing and by a combination of transport and chemistry during the summer. Furthermore, the results in the paper highlight the need for a season specific policy.
Mingfu Cai, Shan Huang, Baoling Liang, Qibin Sun, Li Liu, Bin Yuan, Min Shao, Weiwei Hu, Wei Chen, Qicong Song, Wei Li, Yuwen Peng, Zelong Wang, Duohong Chen, Haobo Tan, Hanbin Xu, Fei Li, Xuejiao Deng, Tao Deng, Jiaren Sun, and Jun Zhao
Atmos. Chem. Phys., 22, 8117–8136, https://doi.org/10.5194/acp-22-8117-2022, https://doi.org/10.5194/acp-22-8117-2022, 2022
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This study investigated the size dependence and diurnal variation in organic aerosol hygroscopicity, volatility, and cloud condensation nuclei (CCN) activity. We found that the physical properties of OA could vary in a large range at different particle sizes and affected the number concentration of CCN (NCCN) at all supersaturations. Our results highlight the importance of evaluating the atmospheric evolution processes of OA at different size ranges and their impact on climate effects.
Linghan Zeng, Jack Dibb, Eric Scheuer, Joseph M. Katich, Joshua P. Schwarz, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Carsten Warneke, Anne E. Perring, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Richard H. Moore, Elizabeth B. Wiggins, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Lu Xu, and Rodney J. Weber
Atmos. Chem. Phys., 22, 8009–8036, https://doi.org/10.5194/acp-22-8009-2022, https://doi.org/10.5194/acp-22-8009-2022, 2022
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Wildfires emit aerosol particles containing brown carbon material that affects visibility and global climate and is toxic. Brown carbon is poorly characterized due to measurement limitations, and its evolution in the atmosphere is not well known. We report on aircraft measurements of brown carbon from large wildfires in the western United States. We compare two methods for measuring brown carbon and study the evolution of brown carbon in the smoke as it moved away from the burning regions.
Katherine R. Travis, James H. Crawford, Gao Chen, Carolyn E. Jordan, Benjamin A. Nault, Hwajin Kim, Jose L. Jimenez, Pedro Campuzano-Jost, Jack E. Dibb, Jung-Hun Woo, Younha Kim, Shixian Zhai, Xuan Wang, Erin E. McDuffie, Gan Luo, Fangqun Yu, Saewung Kim, Isobel J. Simpson, Donald R. Blake, Limseok Chang, and Michelle J. Kim
Atmos. Chem. Phys., 22, 7933–7958, https://doi.org/10.5194/acp-22-7933-2022, https://doi.org/10.5194/acp-22-7933-2022, 2022
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The 2016 Korea–United States Air Quality (KORUS-AQ) field campaign provided a unique set of observations to improve our understanding of PM2.5 pollution in South Korea. Models typically have errors in simulating PM2.5 in this region, which is of concern for the development of control measures. We use KORUS-AQ observations to improve our understanding of the mechanisms driving PM2.5 and the implications of model errors for determining PM2.5 that is attributable to local or foreign sources.
Suxia Yang, Bin Yuan, Yuwen Peng, Shan Huang, Wei Chen, Weiwei Hu, Chenglei Pei, Jun Zhou, David D. Parrish, Wenjie Wang, Xianjun He, Chunlei Cheng, Xiao-Bing Li, Xiaoyun Yang, Yu Song, Haichao Wang, Jipeng Qi, Baolin Wang, Chen Wang, Chaomin Wang, Zelong Wang, Tiange Li, E Zheng, Sihang Wang, Caihong Wu, Mingfu Cai, Chenshuo Ye, Wei Song, Peng Cheng, Duohong Chen, Xinming Wang, Zhanyi Zhang, Xuemei Wang, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 22, 4539–4556, https://doi.org/10.5194/acp-22-4539-2022, https://doi.org/10.5194/acp-22-4539-2022, 2022
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We use a model constrained using observations to study the formation of nitrate aerosol in and downwind of a representative megacity. We found different contributions of various chemical reactions to ground-level nitrate concentrations between urban and suburban regions. We also show that controlling VOC emissions are effective for decreasing nitrate formation in both urban and regional environments, although VOCs are not direct precursors of nitrate aerosol.
Richard J. Pope, Rebecca Kelly, Eloise A. Marais, Ailish M. Graham, Chris Wilson, Jeremy J. Harrison, Savio J. A. Moniz, Mohamed Ghalaieny, Steve R. Arnold, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 4323–4338, https://doi.org/10.5194/acp-22-4323-2022, https://doi.org/10.5194/acp-22-4323-2022, 2022
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Nitrogen oxides (NOx) are potent air pollutants which directly impact on human health. In this study, we use satellite nitrogen dioxide (NO2) data to evaluate the spatial distribution and temporal evolution of the UK official NOx emissions inventory, with reasonable agreement. We also derived satellite-based NOx emissions for several UK cities. In the case of London and Birmingham, the NAEI NOx emissions are potentially too low by >50%.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275, https://doi.org/10.5194/acp-22-4253-2022, https://doi.org/10.5194/acp-22-4253-2022, 2022
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Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
Wenjie Wang, Bin Yuan, Yuwen Peng, Hang Su, Yafang Cheng, Suxia Yang, Caihong Wu, Jipeng Qi, Fengxia Bao, Yibo Huangfu, Chaomin Wang, Chenshuo Ye, Zelong Wang, Baolin Wang, Xinming Wang, Wei Song, Weiwei Hu, Peng Cheng, Manni Zhu, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 22, 4117–4128, https://doi.org/10.5194/acp-22-4117-2022, https://doi.org/10.5194/acp-22-4117-2022, 2022
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From thorough measurements of numerous oxygenated volatile organic compounds, we show that their photodissociation can be important for radical production and ozone formation in the atmosphere. This effect was underestimated in previous studies, as measurements of them were lacking.
Meloë S. F. Kacenelenbogen, Qian Tan, Sharon P. Burton, Otto P. Hasekamp, Karl D. Froyd, Yohei Shinozuka, Andreas J. Beyersdorf, Luke Ziemba, Kenneth L. Thornhill, Jack E. Dibb, Taylor Shingler, Armin Sorooshian, Reed W. Espinosa, Vanderlei Martins, Jose L. Jimenez, Pedro Campuzano-Jost, Joshua P. Schwarz, Matthew S. Johnson, Jens Redemann, and Gregory L. Schuster
Atmos. Chem. Phys., 22, 3713–3742, https://doi.org/10.5194/acp-22-3713-2022, https://doi.org/10.5194/acp-22-3713-2022, 2022
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The impact of aerosols on Earth's radiation budget and human health is important and strongly depends on their composition. One desire of our scientific community is to derive the composition of the aerosol from satellite sensors. However, satellites observe aerosol optical properties (and not aerosol composition) based on remote sensing instrumentation. This study assesses how much aerosol optical properties can tell us about aerosol composition.
Xiajie Yang, Qiaoqiao Wang, Nan Ma, Weiwei Hu, Yang Gao, Zhijiong Huang, Junyu Zheng, Bin Yuan, Ning Yang, Jiangchuan Tao, Juan Hong, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 3743–3762, https://doi.org/10.5194/acp-22-3743-2022, https://doi.org/10.5194/acp-22-3743-2022, 2022
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We use the GEOS-Chem model with additional anthropogenic and biomass burning chlorine emissions combined with updated parameterizations for N2O5 ＋ Cl chemistry to investigate the impacts of chlorine chemistry on air quality in China. Our study not only significantly improves the model's performance but also demonstrates the importance of non-sea-salt chlorine sources as well as an appropriate parameterization for N2O5 ＋ Cl chemistry to the impact of chlorine chemistry in China.
Ka Ming Fung, Colette L. Heald, Jesse H. Kroll, Siyuan Wang, Duseong S. Jo, Andrew Gettelman, Zheng Lu, Xiaohong Liu, Rahul A. Zaveri, Eric C. Apel, Donald R. Blake, Jose-Luis Jimenez, Pedro Campuzano-Jost, Patrick R. Veres, Timothy S. Bates, John E. Shilling, and Maria Zawadowicz
Atmos. Chem. Phys., 22, 1549–1573, https://doi.org/10.5194/acp-22-1549-2022, https://doi.org/10.5194/acp-22-1549-2022, 2022
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Understanding the natural aerosol burden in the preindustrial era is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of dimethyl sulfide (DMS) oxidation (implemented in the Community Atmospheric Model version 6 with chemistry, CAM6-chem) could help us better estimate the present-day and preindustrial concentrations of sulfate and other relevant chemicals, as well as the resulting aerosol radiative impacts.
Douglas A. Day, Pedro Campuzano-Jost, Benjamin A. Nault, Brett B. Palm, Weiwei Hu, Hongyu Guo, Paul J. Wooldridge, Ronald C. Cohen, Kenneth S. Docherty, J. Alex Huffman, Suzane S. de Sá, Scot T. Martin, and Jose L. Jimenez
Atmos. Meas. Tech., 15, 459–483, https://doi.org/10.5194/amt-15-459-2022, https://doi.org/10.5194/amt-15-459-2022, 2022
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Particle-phase nitrates are an important component of atmospheric aerosols and chemistry. In this paper, we systematically explore the application of aerosol mass spectrometry (AMS) to quantify the organic and inorganic nitrate fractions of aerosols in the atmosphere. While AMS has been used for a decade to quantify nitrates, methods are not standardized. We make recommendations for a more universal approach based on this analysis of a large range of field and laboratory observations.
Dongwook Kim, Changmin Cho, Seokhan Jeong, Soojin Lee, Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Jose L. Jimenez, Rainer Volkamer, Donald R. Blake, Armin Wisthaler, Alan Fried, Joshua P. DiGangi, Glenn S. Diskin, Sally E. Pusede, Samuel R. Hall, Kirk Ullmann, L. Gregory Huey, David J. Tanner, Jack Dibb, Christoph J. Knote, and Kyung-Eun Min
Atmos. Chem. Phys., 22, 805–821, https://doi.org/10.5194/acp-22-805-2022, https://doi.org/10.5194/acp-22-805-2022, 2022
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CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. CHOCHO concentration was high in large cities, aromatics being the most important precursors. Loss path to aerosol was the highest sink, contributing to ~ 20 % of secondary organic aerosol formation. Our work highlights that simple CHOCHO surface uptake approach is valid only for low aerosol conditions and more work is required to understand CHOCHO solubility in high-aerosol conditions.
Shixian Zhai, Daniel J. Jacob, Jared F. Brewer, Ke Li, Jonathan M. Moch, Jhoon Kim, Seoyoung Lee, Hyunkwang Lim, Hyun Chul Lee, Su Keun Kuk, Rokjin J. Park, Jaein I. Jeong, Xuan Wang, Pengfei Liu, Gan Luo, Fangqun Yu, Jun Meng, Randall V. Martin, Katherine R. Travis, Johnathan W. Hair, Bruce E. Anderson, Jack E. Dibb, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jung-Hun Woo, Younha Kim, Qiang Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 16775–16791, https://doi.org/10.5194/acp-21-16775-2021, https://doi.org/10.5194/acp-21-16775-2021, 2021
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Geostationary satellite aerosol optical depth (AOD) has tremendous potential for monitoring surface fine particulate matter (PM2.5). Our study explored the physical relationship between AOD and PM2.5 by integrating data from surface networks, aircraft, and satellites with the GEOS-Chem chemical transport model. We quantitatively showed that accurate simulation of aerosol size distributions, boundary layer depths, relative humidity, coarse particles, and diurnal variations in PM2.5 are essential.
Stefano Galmarini, Paul Makar, Olivia E. Clifton, Christian Hogrefe, Jesse O. Bash, Roberto Bellasio, Roberto Bianconi, Johannes Bieser, Tim Butler, Jason Ducker, Johannes Flemming, Alma Hodzic, Christopher D. Holmes, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Juan Luis Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Sam Silva, and Ralf Wolke
Atmos. Chem. Phys., 21, 15663–15697, https://doi.org/10.5194/acp-21-15663-2021, https://doi.org/10.5194/acp-21-15663-2021, 2021
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This technical note presents the research protocols for phase 4 of the Air Quality Model Evaluation International Initiative (AQMEII4). This initiative has three goals: (i) to define the state of wet and dry deposition in regional models, (ii) to evaluate how dry deposition influences air concentration and flux predictions, and (iii) to identify the causes for prediction differences. The evaluation compares LULC-specific dry deposition and effective conductances and fluxes.
Charles A. Brock, Karl D. Froyd, Maximilian Dollner, Christina J. Williamson, Gregory Schill, Daniel M. Murphy, Nicholas J. Wagner, Agnieszka Kupc, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Douglas A. Day, Derek J. Price, Bernadett Weinzierl, Joshua P. Schwarz, Joseph M. Katich, Siyuan Wang, Linghan Zeng, Rodney Weber, Jack Dibb, Eric Scheuer, Glenn S. Diskin, Joshua P. DiGangi, ThaoPaul Bui, Jonathan M. Dean-Day, Chelsea R. Thompson, Jeff Peischl, Thomas B. Ryerson, Ilann Bourgeois, Bruce C. Daube, Róisín Commane, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 15023–15063, https://doi.org/10.5194/acp-21-15023-2021, https://doi.org/10.5194/acp-21-15023-2021, 2021
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The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides a unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky.
Zhe Peng, Julia Lee-Taylor, Harald Stark, John J. Orlando, Bernard Aumont, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 14649–14669, https://doi.org/10.5194/acp-21-14649-2021, https://doi.org/10.5194/acp-21-14649-2021, 2021
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We use the fully explicit GECKO-A model to study the OH reactivity (OHR) evolution in the NO-free photooxidation of several volatile organic compounds. Oxidation progressively produces more saturated and functionalized species, then breaks them into small species. OHR per C atom evolution is similar for different precursors once saturated multifunctional species are formed. We also find that partitioning of these species to chamber walls leads to large deviations in chambers from the atmosphere.
Xinxin Ye, Pargoal Arab, Ravan Ahmadov, Eric James, Georg A. Grell, Bradley Pierce, Aditya Kumar, Paul Makar, Jack Chen, Didier Davignon, Greg R. Carmichael, Gonzalo Ferrada, Jeff McQueen, Jianping Huang, Rajesh Kumar, Louisa Emmons, Farren L. Herron-Thorpe, Mark Parrington, Richard Engelen, Vincent-Henri Peuch, Arlindo da Silva, Amber Soja, Emily Gargulinski, Elizabeth Wiggins, Johnathan W. Hair, Marta Fenn, Taylor Shingler, Shobha Kondragunta, Alexei Lyapustin, Yujie Wang, Brent Holben, David M. Giles, and Pablo E. Saide
Atmos. Chem. Phys., 21, 14427–14469, https://doi.org/10.5194/acp-21-14427-2021, https://doi.org/10.5194/acp-21-14427-2021, 2021
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Wildfire smoke has crucial impacts on air quality, while uncertainties in the numerical forecasts remain significant. We present an evaluation of 12 real-time forecasting systems. Comparison of predicted smoke emissions suggests a large spread in magnitudes, with temporal patterns deviating from satellite detections. The performance for AOD and surface PM2.5 and their discrepancies highlighted the role of accurately represented spatiotemporal emission profiles in improving smoke forecasts.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Haipeng Lin, Daniel J. Jacob, Elizabeth W. Lundgren, Melissa P. Sulprizio, Christoph A. Keller, Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Patrick C. Campbell, Barry Baker, Rick D. Saylor, and Raffaele Montuoro
Geosci. Model Dev., 14, 5487–5506, https://doi.org/10.5194/gmd-14-5487-2021, https://doi.org/10.5194/gmd-14-5487-2021, 2021
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Emissions are a central component of atmospheric chemistry models. The Harmonized Emissions Component (HEMCO) is a software component for computing emissions from a user-selected ensemble of emission inventories and algorithms. It allows users to select, add, and scale emissions from different sources through a configuration file with no change to the model source code. We demonstrate the implementation of HEMCO in several models, all sharing the same HEMCO core code and database library.
Gongda Lu, Eloise A. Marais, Tuan V. Vu, Jingsha Xu, Zongbo Shi, James D. Lee, Qiang Zhang, Lu Shen, Gan Luo, and Fangqun Yu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-428, https://doi.org/10.5194/acp-2021-428, 2021
Revised manuscript not accepted
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Emission controls were imposed in Beijing-Tianjin-Hebei in northern China in autumn-winter 2017. We find that regional PM2.5 targets (15 % decrease relative to previous year) were exceeded. Our analysis shows that decline in precursor emissions only leads to less than half (43 %) the improved air quality. Most of the change (57 %) is due to interannual variability in meteorology. Stricter emission controls may be necessary in years with unfavourable meteorology.
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.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke D. Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul A. Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 11113–11132, https://doi.org/10.5194/acp-21-11113-2021, https://doi.org/10.5194/acp-21-11113-2021, 2021
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected nearly from pole to pole over the oceans during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigated their impact on the variability of tropospheric N2O.
Ye Kuang, Shan Huang, Biao Xue, Biao Luo, Qicong Song, Wei Chen, Weiwei Hu, Wei Li, Pusheng Zhao, Mingfu Cai, Yuwen Peng, Jipeng Qi, Tiange Li, Sihang Wang, Duohong Chen, Dingli Yue, Bin Yuan, and Min Shao
Atmos. Chem. Phys., 21, 10375–10391, https://doi.org/10.5194/acp-21-10375-2021, https://doi.org/10.5194/acp-21-10375-2021, 2021
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We found that organic aerosol factors with identified sources perform much better than oxidation level parameters in characterizing variations in organic aerosol hygroscopicity, and secondary aerosol formations associated with different sources have distinct effects on organic aerosol hygroscopicity. It reveals that source-oriented organic aerosol hygroscopicity investigations might result in more appropriate parameterization approaches in chemical and climate models.
Hua Fang, Xiaoqing Huang, Yanli Zhang, Chenglei Pei, Zuzhao Huang, Yujun Wang, Yanning Chen, Jianhong Yan, Jianqiang Zeng, Shaoxuan Xiao, Shilu Luo, Sheng Li, Jun Wang, Ming Zhu, Xuewei Fu, Zhenfeng Wu, Runqi Zhang, Wei Song, Guohua Zhang, Weiwei Hu, Mingjin Tang, Xiang Ding, Xinhui Bi, and Xinming Wang
Atmos. Chem. Phys., 21, 10005–10013, https://doi.org/10.5194/acp-21-10005-2021, https://doi.org/10.5194/acp-21-10005-2021, 2021
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A tunnel test was initiated to measure the vehicular IVOC emissions under real-world driving conditions. Higher SOA formation estimated from vehicular IVOCs compared to those from traditional VOCs emphasized the greater importance of IVOCs in modulating urban SOA. The results also revealed that non-road diesel-fueled engines greatly contributed to IVOCs in China.
Wenfu Tang, David P. Edwards, Louisa K. Emmons, Helen M. Worden, Laura M. Judd, Lok N. Lamsal, Jassim A. Al-Saadi, Scott J. Janz, James H. Crawford, Merritt N. Deeter, Gabriele Pfister, Rebecca R. Buchholz, Benjamin Gaubert, and Caroline R. Nowlan
Atmos. Meas. Tech., 14, 4639–4655, https://doi.org/10.5194/amt-14-4639-2021, https://doi.org/10.5194/amt-14-4639-2021, 2021
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We use high-resolution airborne mapping spectrometer measurements to assess sub-grid variability within satellite pixels over urban regions. The sub-grid variability within satellite pixels increases with increasing satellite pixel sizes. Temporal variability within satellite pixels decreases with increasing satellite pixel sizes. This work is particularly relevant and useful for future satellite design, satellite data interpretation, and point-grid data comparisons.
Richard H. Moore, Elizabeth B. Wiggins, Adam T. Ahern, Stephen Zimmerman, Lauren Montgomery, Pedro Campuzano Jost, Claire E. Robinson, Luke D. Ziemba, Edward L. Winstead, Bruce E. Anderson, Charles A. Brock, Matthew D. Brown, Gao Chen, Ewan C. Crosbie, Hongyu Guo, Jose L. Jimenez, Carolyn E. Jordan, Ming Lyu, Benjamin A. Nault, Nicholas E. Rothfuss, Kevin J. Sanchez, Melinda Schueneman, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Nicholas L. Wagner, and Jian Wang
Atmos. Meas. Tech., 14, 4517–4542, https://doi.org/10.5194/amt-14-4517-2021, https://doi.org/10.5194/amt-14-4517-2021, 2021
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Atmospheric particles are everywhere and exist in a range of sizes, from a few nanometers to hundreds of microns. Because particle size determines the behavior of chemical and physical processes, accurately measuring particle sizes is an important and integral part of atmospheric field measurements! Here, we discuss the performance of two commonly used particle sizers and how changes in particle composition and optical properties may result in sizing uncertainties, which we quantify.
Chenshuo Ye, Bin Yuan, Yi Lin, Zelong Wang, Weiwei Hu, Tiange Li, Wei Chen, Caihong Wu, Chaomin Wang, Shan Huang, Jipeng Qi, Baolin Wang, Chen Wang, Wei Song, Xinming Wang, E Zheng, Jordan E. Krechmer, Penglin Ye, Zhanyi Zhang, Xuemei Wang, Douglas R. Worsnop, and Min Shao
Atmos. Chem. Phys., 21, 8455–8478, https://doi.org/10.5194/acp-21-8455-2021, https://doi.org/10.5194/acp-21-8455-2021, 2021
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We performed measurements of gaseous and particulate organic compounds using a state-of-the-art online mass spectrometer in urban air. Using the dataset, we provide a holistic chemical characterization of oxygenated organic compounds in the polluted urban atmosphere, which can serve as a reference for the future field measurements of organic compounds in cities.
Yaman Liu, Xinyi Dong, Minghuai Wang, Louisa K. Emmons, Yawen Liu, Yuan Liang, Xiao Li, and Manish Shrivastava
Atmos. Chem. Phys., 21, 8003–8021, https://doi.org/10.5194/acp-21-8003-2021, https://doi.org/10.5194/acp-21-8003-2021, 2021
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Secondary organic aerosol (SOA) is considered one of the most important uncertainties in climate modeling. We evaluate SOA performance in the Community Earth System Model version 2.1 (CESM2.1) configured with the Community Atmosphere Model version 6 with chemistry (CAM6-Chem) through a long-term simulation (1988–2019) with observations in the United States, which indicates monoterpene-formed SOA contributes most to the overestimation of SOA at the surface and underestimation in the upper air.
Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Douglas A. Day, Jason C. Schroder, Dongwook Kim, Jack E. Dibb, Maximilian Dollner, Bernadett Weinzierl, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 3631–3655, https://doi.org/10.5194/amt-14-3631-2021, https://doi.org/10.5194/amt-14-3631-2021, 2021
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We utilize a set of high-quality datasets collected during the NASA Atmospheric Tomography Mission to investigate the impact of differences in observable particle sizes across aerosol instruments in aerosol measurement comparisons. Very good agreement was found between chemically and physically derived submicron aerosol volume. Results support a lack of significant unknown biases in the response of an Aerodyne aerosol mass spectrometer (AMS) when sampling remote aerosols across the globe.
Karn Vohra, Eloise A. Marais, Shannen Suckra, Louisa Kramer, William J. Bloss, Ravi Sahu, Abhishek Gaur, Sachchida N. Tripathi, Martin Van Damme, Lieven Clarisse, and Pierre-F. Coheur
Atmos. Chem. Phys., 21, 6275–6296, https://doi.org/10.5194/acp-21-6275-2021, https://doi.org/10.5194/acp-21-6275-2021, 2021
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We find satellite observations of atmospheric composition generally reproduce variability in surface air pollution, so we use their long record to estimate air quality trends in major UK and Indian cities. Our trend analysis shows that pollutants targeted with air quality policies have not declined in Delhi and Kanpur but have in London and Birmingham, with the exception of a recent and dramatic increase in reactive volatile organics in London. Unregulated ammonia has increased only in Delhi.
Fernando Chouza, Thierry Leblanc, Mark Brewer, Patrick Wang, Sabino Piazzolla, Gabriele Pfister, Rajesh Kumar, Carl Drews, Simone Tilmes, Louisa Emmons, and Matthew Johnson
Atmos. Chem. Phys., 21, 6129–6153, https://doi.org/10.5194/acp-21-6129-2021, https://doi.org/10.5194/acp-21-6129-2021, 2021
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The tropospheric ozone lidar at the JPL Table Mountain Facility (TMF) was used to investigate the impact of Los Angeles (LA) Basin pollution transport and stratospheric intrusions in the planetary boundary layer on the San Gabriel Mountains. The results of this study indicate a dominant role of the LA Basin pollution on days when high ozone levels were observed at TMF (March–October period).
Eloise A. Marais, John F. Roberts, Robert G. Ryan, Henk Eskes, K. Folkert Boersma, Sungyeon Choi, Joanna Joiner, Nader Abuhassan, Alberto Redondas, Michel Grutter, Alexander Cede, Laura Gomez, and Monica Navarro-Comas
Atmos. Meas. Tech., 14, 2389–2408, https://doi.org/10.5194/amt-14-2389-2021, https://doi.org/10.5194/amt-14-2389-2021, 2021
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Nitrogen oxides in the upper troposphere have a profound influence on the global troposphere, but routine reliable observations there are exceedingly rare. We apply cloud-slicing to TROPOMI total columns of nitrogen dioxide (NO2) at high spatial resolution to derive near-global observations of NO2 in the upper troposphere and show consistency with existing datasets. These data offer tremendous potential to address knowledge gaps in this oft underappreciated portion of the atmosphere.
Melinda K. Schueneman, Benjamin A. Nault, Pedro Campuzano-Jost, Duseong S. Jo, Douglas A. Day, Jason C. Schroder, Brett B. Palm, Alma Hodzic, Jack E. Dibb, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 2237–2260, https://doi.org/10.5194/amt-14-2237-2021, https://doi.org/10.5194/amt-14-2237-2021, 2021
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This work focuses on two important properties of the aerosol, acidity, and sulfate composition, which is important for our understanding of aerosol health and environmental impacts. We explore different methods to understand the composition of the aerosol with measurements from a specific instrument and apply those methods to a large dataset. These measurements are confounded by other factors, making it challenging to predict aerosol sulfate composition; pH estimations, however, show promise.
Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, https://doi.org/10.5194/acp-21-4187-2021, 2021
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We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 3395–3425, https://doi.org/10.5194/acp-21-3395-2021, https://doi.org/10.5194/acp-21-3395-2021, 2021
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Secondary organic aerosol (SOA) is a major component of submicron particulate matter, but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX SOA concentration changes. The explicit chemistry predicted substantial changes in IEPOX SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physicochemical dependencies in future SOA prediction.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
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We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Gillian D. Thornhill, William J. Collins, Ryan J. Kramer, Dirk Olivié, Ragnhild B. Skeie, Fiona M. O'Connor, Nathan Luke Abraham, Ramiro Checa-Garcia, Susanne E. Bauer, Makoto Deushi, Louisa K. Emmons, Piers M. Forster, Larry W. Horowitz, Ben Johnson, James Keeble, Jean-Francois Lamarque, Martine Michou, Michael J. Mills, Jane P. Mulcahy, Gunnar Myhre, Pierre Nabat, Vaishali Naik, Naga Oshima, Michael Schulz, Christopher J. Smith, Toshihiko Takemura, Simone Tilmes, Tongwen Wu, Guang Zeng, and Jie Zhang
Atmos. Chem. Phys., 21, 853–874, https://doi.org/10.5194/acp-21-853-2021, https://doi.org/10.5194/acp-21-853-2021, 2021
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This paper is a study of how different constituents in the atmosphere, such as aerosols and gases like methane and ozone, affect the energy balance in the atmosphere. Different climate models were run using the same inputs to allow an easy comparison of the results and to understand where the models differ. We found the effect of aerosols is to reduce warming in the atmosphere, but this effect varies between models. Reactions between gases are also important in affecting climate.
Megan S. Claflin, Demetrios Pagonis, Zachary Finewax, Anne V. Handschy, Douglas A. Day, Wyatt L. Brown, John T. Jayne, Douglas R. Worsnop, Jose L. Jimenez, Paul J. Ziemann, Joost de Gouw, and Brian M. Lerner
Atmos. Meas. Tech., 14, 133–152, https://doi.org/10.5194/amt-14-133-2021, https://doi.org/10.5194/amt-14-133-2021, 2021
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We have developed a field-deployable gas chromatograph with thermal desorption preconcentration and detector switching between two high-resolution mass spectrometers for in situ measurements of volatile organic compounds (VOCs). This system combines chromatography with both proton transfer and electron ionization to offer fast time response and continuous molecular speciation. This technique was applied during the 2018 ATHLETIC campaign to characterize VOC emissions in an indoor environment.
Caihong Wu, Chaomin Wang, Sihang Wang, Wenjie Wang, Bin Yuan, Jipeng Qi, Baolin Wang, Hongli Wang, Chen Wang, Wei Song, Xinming Wang, Weiwei Hu, Shengrong Lou, Chenshuo Ye, Yuwen Peng, Zelong Wang, Yibo Huangfu, Yan Xie, Manni Zhu, Junyu Zheng, Xuemei Wang, Bin Jiang, Zhanyi Zhang, and Min Shao
Atmos. Chem. Phys., 20, 14769–14785, https://doi.org/10.5194/acp-20-14769-2020, https://doi.org/10.5194/acp-20-14769-2020, 2020
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Based on measurements from an online mass spectrometer, we quantify volatile organic compound (VOC) concentrations from numerous ions of the mass spectrometer, using information from laboratory-obtained calibration results. We find that most VOC concentrations are from oxygenated VOCs (OVOCs). We further show that these OVOCs also contribute significantly to OH reactivity. Our results suggest the important role of OVOCs in VOC emissions and chemistry in urban air.
Benjamin Gaubert, Louisa K. Emmons, Kevin Raeder, Simone Tilmes, Kazuyuki Miyazaki, Avelino F. Arellano Jr., Nellie Elguindi, Claire Granier, Wenfu Tang, Jérôme Barré, Helen M. Worden, Rebecca R. Buchholz, David P. Edwards, Philipp Franke, Jeffrey L. Anderson, Marielle Saunois, Jason Schroeder, Jung-Hun Woo, Isobel J. Simpson, Donald R. Blake, Simone Meinardi, Paul O. Wennberg, John Crounse, Alex Teng, Michelle Kim, Russell R. Dickerson, Hao He, Xinrong Ren, Sally E. Pusede, and Glenn S. Diskin
Atmos. Chem. Phys., 20, 14617–14647, https://doi.org/10.5194/acp-20-14617-2020, https://doi.org/10.5194/acp-20-14617-2020, 2020
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This study investigates carbon monoxide pollution in East Asia during spring using a numerical model, satellite remote sensing, and aircraft measurements. We found an underestimation of emission sources. Correcting the emission bias can improve air quality forecasting of carbon monoxide and other species including ozone. Results also suggest that controlling VOC and CO emissions, in addition to widespread NOx controls, can improve ozone pollution over East Asia.
Steven T. Turnock, Robert J. Allen, Martin Andrews, Susanne E. Bauer, Makoto Deushi, Louisa Emmons, Peter Good, Larry Horowitz, Jasmin G. John, Martine Michou, Pierre Nabat, Vaishali Naik, David Neubauer, Fiona M. O'Connor, Dirk Olivié, Naga Oshima, Michael Schulz, Alistair Sellar, Sungbo Shim, Toshihiko Takemura, Simone Tilmes, Kostas Tsigaridis, Tongwen Wu, and Jie Zhang
Atmos. Chem. Phys., 20, 14547–14579, https://doi.org/10.5194/acp-20-14547-2020, https://doi.org/10.5194/acp-20-14547-2020, 2020
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A first assessment is made of the historical and future changes in air pollutants from models participating in the 6th Coupled Model Intercomparison Project (CMIP6). Substantial benefits to future air quality can be achieved in future scenarios that implement measures to mitigate climate and involve reductions in air pollutant emissions, particularly methane. However, important differences are shown between models in the future regional projection of air pollutants under the same scenario.
Chaomin Wang, Bin Yuan, Caihong Wu, Sihang Wang, Jipeng Qi, Baolin Wang, Zelong Wang, Weiwei Hu, Wei Chen, Chenshuo Ye, Wenjie Wang, Yele Sun, Chen Wang, Shan Huang, Wei Song, Xinming Wang, Suxia Yang, Shenyang Zhang, Wanyun Xu, Nan Ma, Zhanyi Zhang, Bin Jiang, Hang Su, Yafang Cheng, Xuemei Wang, and Min Shao
Atmos. Chem. Phys., 20, 14123–14138, https://doi.org/10.5194/acp-20-14123-2020, https://doi.org/10.5194/acp-20-14123-2020, 2020
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We utilized a novel online mass spectrometry method to measure the total concentration of higher alkanes at each carbon number at two different sites in China, allowing us to take into account SOA contributions from all isomers for higher alkanes. We found that higher alkanes account for significant fractions of SOA formation at the two sites. The contributions are comparable to or even higher than single-ring aromatics, the most-recognized SOA precursors in urban air.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Hongyu Guo, Duseong S. Jo, Anne V. Handschy, Demetrios Pagonis, Jason C. Schroder, Melinda K. Schueneman, Michael J. Cubison, Jack E. Dibb, Alma Hodzic, Weiwei Hu, Brett B. Palm, and Jose L. Jimenez
Atmos. Meas. Tech., 13, 6193–6213, https://doi.org/10.5194/amt-13-6193-2020, https://doi.org/10.5194/amt-13-6193-2020, 2020
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Collecting particulate matter, or aerosols, onto filters to be analyzed offline is a widely used method to investigate the mass concentration and chemical composition of the aerosol, especially the inorganic portion. Here, we show that acidic aerosol (sulfuric acid) collected onto filters and then exposed to high ammonia mixing ratios (from human emissions) will lead to biases in the ammonium collected onto filters, and the uptake of ammonia is rapid (< 10 s), which impacts the filter data.
Chao Peng, Yu Wang, Zhijun Wu, Lanxiadi Chen, Ru-Jin Huang, Weigang Wang, Zhe Wang, Weiwei Hu, Guohua Zhang, Maofa Ge, Min Hu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13877–13903, https://doi.org/10.5194/acp-20-13877-2020, https://doi.org/10.5194/acp-20-13877-2020, 2020
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.
David S. Stevenson, Alcide Zhao, Vaishali Naik, Fiona M. O'Connor, Simone Tilmes, Guang Zeng, Lee T. Murray, William J. Collins, Paul T. Griffiths, Sungbo Shim, Larry W. Horowitz, Lori T. Sentman, and Louisa Emmons
Atmos. Chem. Phys., 20, 12905–12920, https://doi.org/10.5194/acp-20-12905-2020, https://doi.org/10.5194/acp-20-12905-2020, 2020
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We present historical trends in atmospheric oxidizing capacity (OC) since 1850 from the latest generation of global climate models and compare these with estimates from measurements. OC controls levels of many key reactive gases, including methane (CH4). We find small model trends up to 1980, then increases of about 9 % up to 2014, disagreeing with (uncertain) measurement-based trends. Major drivers of OC trends are emissions of CH4, NOx, and CO; these will be important for future CH4 trends.
Wenfu Tang, Benjamin Gaubert, Louisa Emmons, Yonghoon Choi, Joshua P. DiGangi, Glenn S. Diskin, Xiaomei Xu, Cenlin He, Helen Worden, Simone Tilmes, Rebecca Buchholz, Hannah S. Halliday, and Avelino F. Arellano
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-864, https://doi.org/10.5194/acp-2020-864, 2020
Revised manuscript not accepted
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A specific demonstration of the potential use of correlative information from carbon monoxide to refine estimates of regional carbon dioxide emissions from fossil fuel combustion.
Robert J. Allen, Steven Turnock, Pierre Nabat, David Neubauer, Ulrike Lohmann, Dirk Olivié, Naga Oshima, Martine Michou, Tongwen Wu, Jie Zhang, Toshihiko Takemura, Michael Schulz, Kostas Tsigaridis, Susanne E. Bauer, Louisa Emmons, Larry Horowitz, Vaishali Naik, Twan van Noije, Tommi Bergman, Jean-Francois Lamarque, Prodromos Zanis, Ina Tegen, Daniel M. Westervelt, Philippe Le Sager, Peter Good, Sungbo Shim, Fiona O'Connor, Dimitris Akritidis, Aristeidis K. Georgoulias, Makoto Deushi, Lori T. Sentman, Jasmin G. John, Shinichiro Fujimori, and William J. Collins
Atmos. Chem. Phys., 20, 9641–9663, https://doi.org/10.5194/acp-20-9641-2020, https://doi.org/10.5194/acp-20-9641-2020, 2020
Ru-Jin Huang, Yao He, Jing Duan, Yongjie Li, Qi Chen, Yan Zheng, Yang Chen, Weiwei Hu, Chunshui Lin, Haiyan Ni, Wenting Dai, Junji Cao, Yunfei Wu, Renjian Zhang, Wei Xu, Jurgita Ovadnevaite, Darius Ceburnis, Thorsten Hoffmann, and Colin D. O'Dowd
Atmos. Chem. Phys., 20, 9101–9114, https://doi.org/10.5194/acp-20-9101-2020, https://doi.org/10.5194/acp-20-9101-2020, 2020
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We systematically compared the submicron particle (PM1) processes in haze days with low and high relative humidity (RH) in wintertime Beijing. Nitrate had similar daytime growth rates in low-RH and high-RH pollution. OOA had a higher growth rate in low-RH pollution than in high-RH pollution. Sulfate had a decreasing trend in low-RH pollution, while it increased significantly in high-RH pollution. This distinction may be explained by the different processes affected by meteorological conditions.
Ifayoyinsola Ibikunle, Andreas Beyersdorf, Pedro Campuzano-Jost, Chelsea Corr, John D. Crounse, Jack Dibb, Glenn Diskin, Greg Huey, Jose-Luis Jimenez, Michelle J. Kim, Benjamin A. Nault, Eric Scheuer, Alex Teng, Paul O. Wennberg, Bruce Anderson, James Crawford, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-501, https://doi.org/10.5194/acp-2020-501, 2020
Publication in ACP not foreseen
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Analysis of observations over South Korea during the NASA/NIER
KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Ying Li, Douglas A. Day, Harald Stark, Jose L. Jimenez, and Manabu Shiraiwa
Atmos. Chem. Phys., 20, 8103–8122, https://doi.org/10.5194/acp-20-8103-2020, https://doi.org/10.5194/acp-20-8103-2020, 2020
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Viscosity is an important property of organic aerosols, but viscosity measurements of ambient organic aerosols are scarce. We developed a method to predict glass transition temperatures using volatility and the atomic oxygen-to-carbon ratio. The method was applied to field observations of volatility distributions to predict viscosity of ambient organic aerosols, yielding consistent results with ambient particle phase-state measurements and global simulations.
Junchen Guo, Shengzhen Zhou, Mingfu Cai, Jun Zhao, Wei Song, Weixiong Zhao, Weiwei Hu, Yele Sun, Yao He, Chengqiang Yang, Xuezhe Xu, Zhisheng Zhang, Peng Cheng, Qi Fan, Jian Hang, Shaojia Fan, Xinming Wang, and Xuemei Wang
Atmos. Chem. Phys., 20, 7595–7615, https://doi.org/10.5194/acp-20-7595-2020, https://doi.org/10.5194/acp-20-7595-2020, 2020
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We characterized non-refractory submicron particulate matter (PM1.0) during winter in Guangzhou, south China. Chemical composition and key sources of ambient PM1.0 are revealed, highlighting the significant role of SOA. The relationship with SOA and peroxy radicals indicated gas-phase oxidation contributed predominantly to SOA formation during non-pollution periods, while heterogeneous/multiphase reactions played more important roles in SOA formation during pollution periods.
Pablo E. Saide, Meng Gao, Zifeng Lu, Daniel L. Goldberg, David G. Streets, Jung-Hun Woo, Andreas Beyersdorf, Chelsea A. Corr, Kenneth L. Thornhill, Bruce Anderson, Johnathan W. Hair, Amin R. Nehrir, Glenn S. Diskin, Jose L. Jimenez, Benjamin A. Nault, Pedro Campuzano-Jost, Jack Dibb, Eric Heim, Kara D. Lamb, Joshua P. Schwarz, Anne E. Perring, Jhoon Kim, Myungje Choi, Brent Holben, Gabriele Pfister, Alma Hodzic, Gregory R. Carmichael, Louisa Emmons, and James H. Crawford
Atmos. Chem. Phys., 20, 6455–6478, https://doi.org/10.5194/acp-20-6455-2020, https://doi.org/10.5194/acp-20-6455-2020, 2020
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Air quality forecasts over the Korean Peninsula captured aerosol optical depth but largely overpredicted surface PM during a Chinese haze transport event. Model deficiency was related to the calculation of optical properties. In order to improve it, aerosol size representation needs to be refined in the calculations, and the representation of aerosol properties, such as size distribution, chemical composition, refractive index, hygroscopicity parameter, and density, needs to be improved.
Camille Mouchel-Vallon, Julia Lee-Taylor, Alma Hodzic, Paulo Artaxo, Bernard Aumont, Marie Camredon, David Gurarie, Jose-Luis Jimenez, Donald H. Lenschow, Scot T. Martin, Janaina Nascimento, John J. Orlando, Brett B. Palm, John E. Shilling, Manish Shrivastava, and Sasha Madronich
Atmos. Chem. Phys., 20, 5995–6014, https://doi.org/10.5194/acp-20-5995-2020, https://doi.org/10.5194/acp-20-5995-2020, 2020
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The GoAmazon 2014/5 field campaign took place near the city of Manaus, Brazil, isolated in the Amazon rainforest, to study the impacts of urban pollution on natural air masses. We simulated this campaign with an extremely detailed organic chemistry model to understand how the city would affect the growth and composition of natural aerosol particles. Discrepancies between the model and the measurements indicate that the chemistry of naturally emitted organic compounds is still poorly understood.
Yan Zheng, Xi Cheng, Keren Liao, Yaowei Li, Yong Jie Li, Ru-Jin Huang, Weiwei Hu, Ying Liu, Tong Zhu, Shiyi Chen, Limin Zeng, Douglas R. Worsnop, and Qi Chen
Atmos. Meas. Tech., 13, 2457–2472, https://doi.org/10.5194/amt-13-2457-2020, https://doi.org/10.5194/amt-13-2457-2020, 2020
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This paper provides important information to help researchers to understand the mass quantification and source apportionment by Aerodyne aerosol mass spectrometers.
Andrew T. Lambe, Ezra C. Wood, Jordan E. Krechmer, Francesca Majluf, Leah R. Williams, Philip L. Croteau, Manuela Cirtog, Anaïs Féron, Jean-Eudes Petit, Alexandre Albinet, Jose L. Jimenez, and Zhe Peng
Atmos. Meas. Tech., 13, 2397–2411, https://doi.org/10.5194/amt-13-2397-2020, https://doi.org/10.5194/amt-13-2397-2020, 2020
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We present a new method to continuously generate N2O5 in the gas phase that is injected into a reactor where it decomposes to generate nitrate radicals (NO3). To assess the applicability of the method towards different chemical systems, we present experimental and model characterization of the integrated NO3 exposure and other metrics as a function of operating conditions. We demonstrate the method by characterizing secondary organic aerosol particles generated from the β-pinene + NO3 reaction.
Alma Hodzic, Pedro Campuzano-Jost, Huisheng Bian, Mian Chin, Peter R. Colarco, Douglas A. Day, Karl D. Froyd, Bernd Heinold, Duseong S. Jo, Joseph M. Katich, John K. Kodros, Benjamin A. Nault, Jeffrey R. Pierce, Eric Ray, Jacob Schacht, Gregory P. Schill, Jason C. Schroder, Joshua P. Schwarz, Donna T. Sueper, Ina Tegen, Simone Tilmes, Kostas Tsigaridis, Pengfei Yu, and Jose L. Jimenez
Atmos. Chem. Phys., 20, 4607–4635, https://doi.org/10.5194/acp-20-4607-2020, https://doi.org/10.5194/acp-20-4607-2020, 2020
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Organic aerosol (OA) is a key source of uncertainty in aerosol climate effects. We present the first pole-to-pole OA characterization during the NASA Atmospheric Tomography aircraft mission. OA has a strong seasonal and zonal variability, with the highest levels in summer and over fire-influenced regions and the lowest ones in the southern high latitudes. We show that global models predict the OA distribution well but not the relative contribution of OA emissions vs. chemical production.
Rebecca H. Schwantes, Louisa K. Emmons, John J. Orlando, Mary C. Barth, Geoffrey S. Tyndall, Samuel R. Hall, Kirk Ullmann, Jason M. St. Clair, Donald R. Blake, Armin Wisthaler, and Thao Paul V. Bui
Atmos. Chem. Phys., 20, 3739–3776, https://doi.org/10.5194/acp-20-3739-2020, https://doi.org/10.5194/acp-20-3739-2020, 2020
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Ozone is a greenhouse gas and air pollutant that is harmful to human health and plants. During the summer in the southeastern US, many regional and global models are biased high for surface ozone compared to observations. Here adding more complex and updated chemistry for isoprene and terpenes, which are biogenic hydrocarbons emitted from trees and vegetation, into an earth system model greatly reduces the simulated surface ozone bias compared to aircraft and monitoring station data.
Wenfu Tang, Helen M. Worden, Merritt N. Deeter, David P. Edwards, Louisa K. Emmons, Sara Martínez-Alonso, Benjamin Gaubert, Rebecca R. Buchholz, Glenn S. Diskin, Russell R. Dickerson, Xinrong Ren, Hao He, and Yutaka Kondo
Atmos. Meas. Tech., 13, 1337–1356, https://doi.org/10.5194/amt-13-1337-2020, https://doi.org/10.5194/amt-13-1337-2020, 2020
Sidhant J. Pai, Colette L. Heald, Jeffrey R. Pierce, Salvatore C. Farina, Eloise A. Marais, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Ann M. Middlebrook, Hugh Coe, John E. Shilling, Roya Bahreini, Justin H. Dingle, and Kennedy Vu
Atmos. Chem. Phys., 20, 2637–2665, https://doi.org/10.5194/acp-20-2637-2020, https://doi.org/10.5194/acp-20-2637-2020, 2020
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Aerosols in the atmosphere have significant health and climate impacts. Organic aerosol (OA) accounts for a large fraction of the total aerosol burden, but models have historically struggled to accurately simulate it. This study compares two very different OA model schemes and evaluates them against a suite of globally distributed airborne measurements with the goal of providing insight into the strengths and weaknesses of each approach across different environments.
Therese S. Carter, Colette L. Heald, Jose L. Jimenez, Pedro Campuzano-Jost, Yutaka Kondo, Nobuhiro Moteki, Joshua P. Schwarz, Christine Wiedinmyer, Anton S. Darmenov, Arlindo M. da Silva, and Johannes W. Kaiser
Atmos. Chem. Phys., 20, 2073–2097, https://doi.org/10.5194/acp-20-2073-2020, https://doi.org/10.5194/acp-20-2073-2020, 2020
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Fires and the smoke they emit impact air quality, health, and climate, but the abundance and properties of smoke remain uncertain and poorly constrained. To explore this, we compare model simulations driven by four commonly-used fire emission inventories with surface, aloft, and satellite observations. We show that across inventories smoke emissions differ by factors of 4 to 7 over North America, challenging our ability to accurately characterize the impact of smoke on air quality and climate.
Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Kanako Sekimoto, Bin Yuan, Jessica B. Gilman, David H. Hagan, Vanessa Selimovic, Kyle J. Zarzana, Steven S. Brown, James M. Roberts, Markus Müller, Robert Yokelson, Armin Wisthaler, Jordan E. Krechmer, Jose L. Jimenez, Christopher Cappa, Jesse H. Kroll, Joost de Gouw, and Carsten Warneke
Atmos. Chem. Phys., 19, 14875–14899, https://doi.org/10.5194/acp-19-14875-2019, https://doi.org/10.5194/acp-19-14875-2019, 2019
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Wildfire emissions significantly contribute to adverse air quality; however, the chemical processes that lead to hazardous pollutants, such as ozone, are not fully understood. In this study, we describe laboratory experiments where we simulate the atmospheric chemistry of smoke emitted from a range of biomass fuels. We show that certain understudied compounds, such as furans and phenolic compounds, are significant contributors to pollutants formed as a result of typical atmospheric oxidation.
Karl D. Froyd, Daniel M. Murphy, Charles A. Brock, Pedro Campuzano-Jost, Jack E. Dibb, Jose-Luis Jimenez, Agnieszka Kupc, Ann M. Middlebrook, Gregory P. Schill, Kenneth L. Thornhill, Christina J. Williamson, James C. Wilson, and Luke D. Ziemba
Atmos. Meas. Tech., 12, 6209–6239, https://doi.org/10.5194/amt-12-6209-2019, https://doi.org/10.5194/amt-12-6209-2019, 2019
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Single-particle mass spectrometer (SPMS) instruments characterize the composition of individual aerosol particles in real time. We present a new method that combines SPMS composition with independently measured particle size distributions to determine absolute number, surface area, volume, and mass concentrations of mineral dust, biomass burning, sea salt, and other climate-relevant atmospheric particle types, with a fast time response applicable to aircraft sampling.
Brett B. Palm, Xiaoxi Liu, Jose L. Jimenez, and Joel A. Thornton
Atmos. Meas. Tech., 12, 5829–5844, https://doi.org/10.5194/amt-12-5829-2019, https://doi.org/10.5194/amt-12-5829-2019, 2019
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We introduce a coaxial, low-pressure ion–molecule reaction (IMR) region for iodide-adduct chemical ionization mass spectrometry, designed to decrease the effects of IMR wall interactions with organic/inorganic gases. This IMR has 3–10 times shorter delay times than previous IMRs. We introduce a conceptual framework for understanding and subtracting the background signal due to analyte molecules interacting with IMR walls. This framework can be applied to other tubing and instrument systems.
Daun Jeong, Roger Seco, Dasa Gu, Youngro Lee, Benjamin A. Nault, Christoph J. Knote, Tom Mcgee, John T. Sullivan, Jose L. Jimenez, Pedro Campuzano-Jost, Donald R. Blake, Dianne Sanchez, Alex B. Guenther, David Tanner, L. Gregory Huey, Russell Long, Bruce E. Anderson, Samuel R. Hall, Kirk Ullmann, Hye-jung Shin, Scott C. Herndon, Youngjae Lee, Danbi Kim, Joonyoung Ahn, and Saewung Kim
Atmos. Chem. Phys., 19, 12779–12795, https://doi.org/10.5194/acp-19-12779-2019, https://doi.org/10.5194/acp-19-12779-2019, 2019
Benjamin L. Deming, Demetrios Pagonis, Xiaoxi Liu, Douglas A. Day, Ranajit Talukdar, Jordan E. Krechmer, Joost A. de Gouw, Jose L. Jimenez, and Paul J. Ziemann
Atmos. Meas. Tech., 12, 3453–3461, https://doi.org/10.5194/amt-12-3453-2019, https://doi.org/10.5194/amt-12-3453-2019, 2019
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Losses or measurement delays of gas-phase compounds sampled through tubing are important to atmospheric science. Here we characterize 14 tubing materials by measuring the effects on step changes in organic compound concentration. We find that polymeric tubings exhibit absorptive partitioning behaviour while glass and metal tubings show adsorptive partitioning. Adsorptive materials impart complex humidity, concentration, and VOC–VOC interaction dependencies that absorptive tubings do not.
Suzane S. de Sá, Luciana V. Rizzo, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Lindsay D. Yee, Rebecca Wernis, Gabriel Isaacman-VanWertz, Joel Brito, Samara Carbone, Yingjun J. Liu, Arthur Sedlacek, Stephen Springston, Allen H. Goldstein, Henrique M. J. Barbosa, M. Lizabeth Alexander, Paulo Artaxo, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 19, 7973–8001, https://doi.org/10.5194/acp-19-7973-2019, https://doi.org/10.5194/acp-19-7973-2019, 2019
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This study investigates the impacts of urban and fire emissions on the concentration, composition, and optical properties of submicron particulate matter (PM1) in central Amazonia during the dry season. Biomass-burning and urban emissions appeared to contribute at least 80 % of brown carbon absorption while accounting for 30 % to 40 % of the organic PM1 mass concentration. Only a fraction of the 9-fold increase in mass concentration relative to the wet season was due to biomass burning.
Xiaoxi Liu, Benjamin Deming, Demetrios Pagonis, Douglas A. Day, Brett B. Palm, Ranajit Talukdar, James M. Roberts, Patrick R. Veres, Jordan E. Krechmer, Joel A. Thornton, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 12, 3137–3149, https://doi.org/10.5194/amt-12-3137-2019, https://doi.org/10.5194/amt-12-3137-2019, 2019
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Delays or losses of gases in sampling tubing and instrumental surfaces due to surface interactions can lead to inaccurate quantification. By sampling with several chemical ionization mass spectrometers and six tubing materials, we quantify delays of semivolatile organic compounds and small polar gases. Delay times generally increase with decreasing volatility or increasing polarity and also depend on materials. The method and results will inform inlet material selection and instrumental design.
Charles A. Brock, Christina Williamson, Agnieszka Kupc, Karl D. Froyd, Frank Erdesz, Nicholas Wagner, Matthews Richardson, Joshua P. Schwarz, Ru-Shan Gao, Joseph M. Katich, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Jose L. Jimenez, Bernadett Weinzierl, Maximilian Dollner, ThaoPaul Bui, and Daniel M. Murphy
Atmos. Meas. Tech., 12, 3081–3099, https://doi.org/10.5194/amt-12-3081-2019, https://doi.org/10.5194/amt-12-3081-2019, 2019
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From 2016 to 2018 a NASA aircraft profiled the atmosphere from 180 m to ~12 km from the Arctic to the Antarctic over both the Pacific and Atlantic oceans. This program, ATom, sought to sample atmospheric chemical composition to compare with global climate models. We describe the how measurements of particulate matter were made during ATom, and show that the instrument performance was excellent. Data from this project can be used with confidence to evaluate models and compare with satellites.
Ali Akherati, Christopher D. Cappa, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, Stephen M. Griffith, Sebastien Dusanter, Philip S. Stevens, and Shantanu H. Jathar
Atmos. Chem. Phys., 19, 4561–4594, https://doi.org/10.5194/acp-19-4561-2019, https://doi.org/10.5194/acp-19-4561-2019, 2019
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Unburned and partially burned organic compounds emitted from fossil fuel and biomass combustion can react in the atmosphere in the presence of sunlight to form particles. In this work, we use an air pollution model to examine the influence of these organic compounds released by motor vehicles and fires on fine particle pollution in southern California.
Anna L. Hodshire, Pedro Campuzano-Jost, John K. Kodros, Betty Croft, Benjamin A. Nault, Jason C. Schroder, Jose L. Jimenez, and Jeffrey R. Pierce
Atmos. Chem. Phys., 19, 3137–3160, https://doi.org/10.5194/acp-19-3137-2019, https://doi.org/10.5194/acp-19-3137-2019, 2019
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A global chemical-transport model is used to determine the impact of methanesulfonic acid (MSA) on the aerosol size distribution and associated radiative effects, testing varying assumptions of MSA’s effective volatility and nucleating ability. We find that MSA mass best matches the ATom airborne measurements when volatility varies as a function of temperature, relative humidity, and available gas-phase bases, and the MSA radiative forcing is on the order of -50 mW m-2 over the Southern Ocean.
Jin Liao, Thomas F. Hanisco, Glenn M. Wolfe, Jason St. Clair, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Alan Fried, Eloise A. Marais, Gonzalo Gonzalez Abad, Kelly Chance, Hiren T. Jethva, Thomas B. Ryerson, Carsten Warneke, and Armin Wisthaler
Atmos. Chem. Phys., 19, 2765–2785, https://doi.org/10.5194/acp-19-2765-2019, https://doi.org/10.5194/acp-19-2765-2019, 2019
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Organic aerosol (OA) intimately links natural and anthropogenic emissions with air quality and climate. Direct OA measurements from space are currently not possible. This paper describes a new method to estimate OA by combining satellite HCHO and in situ OA and HCHO. The OA estimate is validated with the ground network. This new method has a potential for mapping observation-based global OA estimate.
Shino Toma, Steve Bertman, Christopher Groff, Fulizi Xiong, Paul B. Shepson, Paul Romer, Kaitlin Duffey, Paul Wooldridge, Ronald Cohen, Karsten Baumann, Eric Edgerton, Abigail R. Koss, Joost de Gouw, Allen Goldstein, Weiwei Hu, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 1867–1880, https://doi.org/10.5194/acp-19-1867-2019, https://doi.org/10.5194/acp-19-1867-2019, 2019
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Acyl peroxy nitrates (APN) were measured near the ground in Alabama using GC in summer 2013 to study biosphere–atmosphere interactions. APN were lower than measured in the SE USA over the past 2 decades. Historical data showed APN in 2013 was limited by NOx and production was dominated by biogenic precursors more than in the past. Isoprene-derived MPAN correlated with isoprene hydroxynitrates as NOx-dependent products. MPAN varied with aerosol growth, but not with N-containing particles.
Dagny A. Ullmann, Mallory L. Hinks, Adrian M. Maclean, Christopher L. Butenhoff, James W. Grayson, Kelley Barsanti, Jose L. Jimenez, Sergey A. Nizkorodov, Saeid Kamal, and Allan K. Bertram
Atmos. Chem. Phys., 19, 1491–1503, https://doi.org/10.5194/acp-19-1491-2019, https://doi.org/10.5194/acp-19-1491-2019, 2019
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We measured the viscosity and diffusion of organic molecules in secondary organic aerosol (SOA) generated from the ozonolysis of limonene. The results suggest that the mixing times of large organics in the SOA studied are short (< 1 h) for conditions found in the planetary boundary layer. The results also show that the Stokes–Einstein equation gives accurate predictions of diffusion coefficients of large organics within the studied SOA up to a viscosity of 102 to 104 Pa s.
Zhe Peng, Julia Lee-Taylor, John J. Orlando, Geoffrey S. Tyndall, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 813–834, https://doi.org/10.5194/acp-19-813-2019, https://doi.org/10.5194/acp-19-813-2019, 2019
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The use of oxidation flow reactors (OFRs) has been rapidly increasing. We investigate organic peroxy radical (RO2) chemistry in OFRs by kinetic modeling. It is found that, at low NO, UV intensity should be limited to avoid high radical levels leading to significant reaction of RO2 with OH and negligible RO2 isomerization, both of which are atmospherically irrelevant. We also develop two RO2 fate estimators (for general use and for OFRs) to aid experiment design and interpretation.
Juhi Nagori, Ruud H. H. Janssen, Juliane L. Fry, Maarten Krol, Jose L. Jimenez, Weiwei Hu, and Jordi Vilà-Guerau de Arellano
Atmos. Chem. Phys., 19, 701–729, https://doi.org/10.5194/acp-19-701-2019, https://doi.org/10.5194/acp-19-701-2019, 2019
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Secondary organic aerosol (SOA) is produced through a complex interaction of sunlight, volatile organic compounds emitted from trees, anthropogenic emissions, and atmospheric chemistry. We are able to successfully model the formation and diurnal evolution of SOA using a model that takes into consideration the surface and boundary layer dynamics (1–2 km from the surface) and photochemistry above the southeastern US with data collected during the SOAS campaign to constrain the model.
Andrew T. Lambe, Jordan E. Krechmer, Zhe Peng, Jason R. Casar, Anthony J. Carrasquillo, Jonathan D. Raff, Jose L. Jimenez, and Douglas R. Worsnop
Atmos. Meas. Tech., 12, 299–311, https://doi.org/10.5194/amt-12-299-2019, https://doi.org/10.5194/amt-12-299-2019, 2019
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This paper is an evaluation of methods used to generate OH radicals under conditions with high concentrations of NO and NO2 to simulate oxidation chemistry in polluted urban atmospheres over equivalent atmospheric timescales of ~ 1 day.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Bruce Anderson, Andreas J. Beyersdorf, Donald R. Blake, William H. Brune, Yonghoon Choi, Chelsea A. Corr, Joost A. de Gouw, Jack Dibb, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, L. Gregory Huey, Michelle J. Kim, Christoph J. Knote, Kara D. Lamb, Taehyoung Lee, Taehyun Park, Sally E. Pusede, Eric Scheuer, Kenneth L. Thornhill, Jung-Hun Woo, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 17769–17800, https://doi.org/10.5194/acp-18-17769-2018, https://doi.org/10.5194/acp-18-17769-2018, 2018
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Aerosol impacts visibility and human health in large cities. Sources of aerosols are still highly uncertain, especially for cities surrounded by numerous other cities. We use observations collected during the Korea–United States Air Quality study to determine sources of organic aerosol (OA). We find that secondary OA (SOA) is rapidly produced over Seoul, South Korea, and that the sources of the SOA originate from short-lived hydrocarbons, which originate from local emissions.
Eloise A. Marais, Daniel J. Jacob, Sungyeon Choi, Joanna Joiner, Maria Belmonte-Rivas, Ronald C. Cohen, Steffen Beirle, Lee T. Murray, Luke D. Schiferl, Viral Shah, and Lyatt Jaeglé
Atmos. Chem. Phys., 18, 17017–17027, https://doi.org/10.5194/acp-18-17017-2018, https://doi.org/10.5194/acp-18-17017-2018, 2018
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We intercompare two new products of global upper tropospheric nitrogen dioxide (NO2) retrieved from the Ozone Monitoring Instrument (OMI). We evaluate these products with aircraft observations from NASA DC8 aircraft campaigns and interpret the useful information these products can provide about nitrogen oxides (NOx) in the global upper troposphere using the GEOS-Chem chemical transport model.
Barbara Ervens, Armin Sorooshian, Abdulmonam M. Aldhaif, Taylor Shingler, Ewan Crosbie, Luke Ziemba, Pedro Campuzano-Jost, Jose L. Jimenez, and Armin Wisthaler
Atmos. Chem. Phys., 18, 16099–16119, https://doi.org/10.5194/acp-18-16099-2018, https://doi.org/10.5194/acp-18-16099-2018, 2018
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The paper presents a new framework that can be used to identify emission scenarios in which aerosol populations are most likely modified by chemical processes in clouds. We show that in neither very polluted nor in very clean air masses is this the case. Only if the ratio of possible aerosol mass precursors (sulfur dioxide, some organics) and preexisting aerosol mass is sufficiently high will aerosol particles show substantially modified physicochemical properties upon cloud processing.
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.
Benjamin Brown-Steiner, Noelle E. Selin, Ronald Prinn, Simone Tilmes, Louisa Emmons, Jean-François Lamarque, and Philip Cameron-Smith
Geosci. Model Dev., 11, 4155–4174, https://doi.org/10.5194/gmd-11-4155-2018, https://doi.org/10.5194/gmd-11-4155-2018, 2018
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We conduct three simulations of atmospheric chemistry using chemical mechanisms of different levels of complexity and compare their results to observations. We explore situations in which the simplified mechanisms match the output of the most complex mechanism, as well as when they diverge. We investigate how concurrent utilization of chemical mechanisms of different complexities can further our atmospheric-chemistry understanding at various scales and give some strategies for future research.
William H. Brune, Xinrong Ren, Li Zhang, Jingqiu Mao, David O. Miller, Bruce E. Anderson, Donald R. Blake, Ronald C. Cohen, Glenn S. Diskin, Samuel R. Hall, Thomas F. Hanisco, L. Gregory Huey, Benjamin A. Nault, Jeff Peischl, Ilana Pollack, Thomas B. Ryerson, Taylor Shingler, Armin Sorooshian, Kirk Ullmann, Armin Wisthaler, and Paul J. Wooldridge
Atmos. Chem. Phys., 18, 14493–14510, https://doi.org/10.5194/acp-18-14493-2018, https://doi.org/10.5194/acp-18-14493-2018, 2018
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Thunderstorms pull in polluted air from near the ground, transport it up through clouds containing lightning, and deposit it at altitudes where airplanes fly. The resulting chemical mixture in this air reacts to form ozone and particles, which affect climate. In this study, aircraft observations of the reactive gases responsible for this chemistry generally agree with modeled values, even in ice clouds. Thus, atmospheric oxidation chemistry appears to be mostly understood for this environment.
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.
Victor Lannuque, Marie Camredon, Florian Couvidat, Alma Hodzic, Richard Valorso, Sasha Madronich, Bertrand Bessagnet, and Bernard Aumont
Atmos. Chem. Phys., 18, 13411–13428, https://doi.org/10.5194/acp-18-13411-2018, https://doi.org/10.5194/acp-18-13411-2018, 2018
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Large uncertainties remain in understanding the influence of atmospheric environmental conditions on secondary organic aerosol (SOA) formation, evolution and properties. In this article, the GECKO-A modelling tool has been used in a box model under various environmental conditions to (i) explore the sensitivity of SOA formation and properties to changes on physical and chemical conditions and (ii) develop a volatility-basis-set-type parameterization for air quality models.
Anna L. Hodshire, Brett B. Palm, M. Lizabeth Alexander, Qijing Bian, Pedro Campuzano-Jost, Eben S. Cross, Douglas A. Day, Suzane S. de Sá, Alex B. Guenther, Armin Hansel, James F. Hunter, Werner Jud, Thomas Karl, Saewung Kim, Jesse H. Kroll, Jeong-Hoo Park, Zhe Peng, Roger Seco, James N. Smith, Jose L. Jimenez, and Jeffrey R. Pierce
Atmos. Chem. Phys., 18, 12433–12460, https://doi.org/10.5194/acp-18-12433-2018, https://doi.org/10.5194/acp-18-12433-2018, 2018
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We investigate the nucleation and growth processes that shape the aerosol size distribution inside oxidation flow reactors (OFRs) that sampled ambient air from Colorado and the Amazon rainforest. Results indicate that organics are important for both nucleation and growth, vapor uptake was limited to accumulation-mode particles, fragmentation reactions were important to limit particle growth at higher OH exposures, and an H2SO4-organics nucleation mechanism captured new particle formation well.
Jiani Tan, Joshua S. Fu, Frank Dentener, Jian Sun, Louisa Emmons, Simone Tilmes, Johannes Flemming, Toshihiko Takemura, Huisheng Bian, Qingzhao Zhu, Cheng-En Yang, and Terry Keating
Atmos. Chem. Phys., 18, 12223–12240, https://doi.org/10.5194/acp-18-12223-2018, https://doi.org/10.5194/acp-18-12223-2018, 2018
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Have contributions of hemispheric air pollution to deposition at global scale been overlooked in the past years? How do we assess the critical load for the acid deposition when we look for the demand of forest and crop? This study highlights the significant impact of hemispheric transport on deposition in coastal regions, open ocean and low-emission regions. Further research is proposed for improving ecosystem and human health in these regions, with regards to the enhanced hemispheric transport.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Joel Brito, Samara Carbone, Igor O. Ribeiro, Glauber G. Cirino, Yingjun Liu, Ryan Thalman, Arthur Sedlacek, Aaron Funk, Courtney Schumacher, John E. Shilling, Johannes Schneider, Paulo Artaxo, Allen H. Goldstein, Rodrigo A. F. Souza, Jian Wang, Karena A. McKinney, Henrique Barbosa, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 18, 12185–12206, https://doi.org/10.5194/acp-18-12185-2018, https://doi.org/10.5194/acp-18-12185-2018, 2018
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This study aimed at understanding and quantifying the changes in mass concentration and composition of submicron airborne particulate matter (PM) in Amazonia due to urban pollution. Downwind of Manaus, PM concentrations increased by up to 200 % under polluted compared with background conditions. The observed changes included contributions from both primary and secondary processes. The differences in organic PM composition suggested a shift in the pathways of secondary production with pollution.
Juliane L. Fry, Steven S. Brown, Ann M. Middlebrook, Peter M. Edwards, Pedro Campuzano-Jost, Douglas A. Day, José L. Jimenez, Hannah M. Allen, Thomas B. Ryerson, Ilana Pollack, Martin Graus, Carsten Warneke, Joost A. de Gouw, Charles A. Brock, Jessica Gilman, Brian M. Lerner, William P. Dubé, Jin Liao, and André Welti
Atmos. Chem. Phys., 18, 11663–11682, https://doi.org/10.5194/acp-18-11663-2018, https://doi.org/10.5194/acp-18-11663-2018, 2018
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This paper uses measurements made during research aircraft flights through power plant smokestack emissions plumes as a natural laboratory in the field experiment. We investigated a specific source of airborne particulate matter from the combination of human-produced NOx pollutant emissions (the smokestack plumes) with isoprene emitted by naturally by trees in the southeastern United States. These field-based yields appear to be higher than those typically measured in chamber studies.
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.
Lindsay D. Yee, Gabriel Isaacman-VanWertz, Rebecca A. Wernis, Meng Meng, Ventura Rivera, Nathan M. Kreisberg, Susanne V. Hering, Mads S. Bering, Marianne Glasius, Mary Alice Upshur, Ariana Gray Bé, Regan J. Thomson, Franz M. Geiger, John H. Offenberg, Michael Lewandowski, Ivan Kourtchev, Markus Kalberer, Suzane de Sá, Scot T. Martin, M. Lizabeth Alexander, Brett B. Palm, Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Jose L. Jimenez, Yingjun Liu, Karena A. McKinney, Paulo Artaxo, Juarez Viegas, Antonio Manzi, Maria B. Oliveira, Rodrigo de Souza, Luiz A. T. Machado, Karla Longo, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 10433–10457, https://doi.org/10.5194/acp-18-10433-2018, https://doi.org/10.5194/acp-18-10433-2018, 2018
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Biogenic volatile organic compounds react in the atmosphere to form secondary organic aerosol, yet the chemical pathways remain unclear. We collected filter samples and deployed a semi-volatile thermal desorption aerosol gas chromatograph in the central Amazon. We measured 30 sesquiterpenes and 4 diterpenes and find them to be important for reactive ozone loss. We estimate that sesquiterpene oxidation contributes at least 0.4–5 % (median 1 %) of observed submicron organic aerosol mass.
Steven T. Turnock, Oliver Wild, Frank J. Dentener, Yanko Davila, Louisa K. Emmons, Johannes Flemming, Gerd A. Folberth, Daven K. Henze, Jan E. Jonson, Terry J. Keating, Sudo Kengo, Meiyun Lin, Marianne Lund, Simone Tilmes, and Fiona M. O'Connor
Atmos. Chem. Phys., 18, 8953–8978, https://doi.org/10.5194/acp-18-8953-2018, https://doi.org/10.5194/acp-18-8953-2018, 2018
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A simple parameterisation was developed in this study to provide a rapid assessment of the impacts and uncertainties associated with future emission control strategies by predicting changes to surface ozone air quality and near-term climate forcing of ozone. Future emissions scenarios based on currently implemented legislation are shown to worsen surface ozone air quality and enhance near-term climate warming, with changes in methane becoming increasingly important in the future.
Benjamin Brown-Steiner, Noelle E. Selin, Ronald G. Prinn, Erwan Monier, Simone Tilmes, Louisa Emmons, and Fernando Garcia-Menendez
Atmos. Chem. Phys., 18, 8373–8388, https://doi.org/10.5194/acp-18-8373-2018, https://doi.org/10.5194/acp-18-8373-2018, 2018
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Detecting signals in observations and simulations of atmospheric chemistry is difficult due to the underlying variability in the chemistry, meteorology, and climatology. Here we examine the scale dependence of ozone variability and explore strategies for reducing or averaging this variability and thereby enhancing ozone signal detection capabilities. We find that 10–15 years of temporal averaging, and some level of spatial averaging, reduces the risk of overconfidence in ozone signals.
Young-Hee Ryu, Alma Hodzic, Jerome Barre, Gael Descombes, and Patrick Minnis
Atmos. Chem. Phys., 18, 7509–7525, https://doi.org/10.5194/acp-18-7509-2018, https://doi.org/10.5194/acp-18-7509-2018, 2018
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We investigate whether errors in cloud predictions can significantly impact the ability of air quality models to predict surface ozone over the US during summer 2013. The comparison with satellite data shows that the model predicts ~ 55 % of clouds in the right locations and underpredicts cloud thickness. The error in daytime ozone is estimated to be 1–5 ppb and represents ~ 40 % of the ozone bias. The accurate predictions of clouds particularly benefits ozone predictions in urban areas.
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.
Abigail R. Koss, Kanako Sekimoto, Jessica B. Gilman, Vanessa Selimovic, Matthew M. Coggon, Kyle J. Zarzana, Bin Yuan, Brian M. Lerner, Steven S. Brown, Jose L. Jimenez, Jordan Krechmer, James M. Roberts, Carsten Warneke, Robert J. Yokelson, and Joost de Gouw
Atmos. Chem. Phys., 18, 3299–3319, https://doi.org/10.5194/acp-18-3299-2018, https://doi.org/10.5194/acp-18-3299-2018, 2018
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Non-methane organic gases (NMOGs) were detected by proton-transfer-reaction mass spectrometry (PTR-ToF) during an extensive laboratory characterization of wildfire emissions. Identifications for PTR-ToF ion masses are proposed and supported by a combination of techniques. Overall excellent agreement with other instrumentation is shown. Scalable emission factors and ratios are reported for many newly reported reactive species. An analysis of chemical characteristics is presented.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Xuan Wang, Colette L. Heald, Jiumeng Liu, Rodney J. Weber, Pedro Campuzano-Jost, Jose L. Jimenez, Joshua P. Schwarz, and Anne E. Perring
Atmos. Chem. Phys., 18, 635–653, https://doi.org/10.5194/acp-18-635-2018, https://doi.org/10.5194/acp-18-635-2018, 2018
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Brown carbon (BrC) contributes significantly to uncertainty in estimating the global direct radiative effect (DRE) of aerosols. We develop a global model simulation of BrC and test it against BrC absorption measurements from two aircraft campaigns in the continental United States. We suggest that BrC DRE has been overestimated previously due to the lack of observational constraints from direct measurements and omission of the effects of photochemical whitening.
Brett B. Palm, Suzane S. de Sá, Douglas A. Day, Pedro Campuzano-Jost, Weiwei Hu, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Joel Brito, Florian Wurm, Paulo Artaxo, Ryan Thalman, Jian Wang, Lindsay D. Yee, Rebecca Wernis, Gabriel Isaacman-VanWertz, Allen H. Goldstein, Yingjun Liu, Stephen R. Springston, Rodrigo Souza, Matt K. Newburn, M. Lizabeth Alexander, Scot T. Martin, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 467–493, https://doi.org/10.5194/acp-18-467-2018, https://doi.org/10.5194/acp-18-467-2018, 2018
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Ambient air was oxidized by OH or O3 in an oxidation flow reactor during both wet and dry seasons in the GoAmazon2014/5 campaign to study secondary organic aerosol (SOA) formation. We investigated how much biogenic, urban, and biomass burning sources contributed to the ambient concentrations of SOA precursor gases and how their contributions changed diurnally and seasonally. SOA yields and hygroscopicity of organic aerosol in the oxidation flow reactor were also studied.
Demetrios Pagonis, Jordan E. Krechmer, Joost de Gouw, Jose L. Jimenez, and Paul J. Ziemann
Atmos. Meas. Tech., 10, 4687–4696, https://doi.org/10.5194/amt-10-4687-2017, https://doi.org/10.5194/amt-10-4687-2017, 2017
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Laboratory studies were conducted to investigate gas-wall partitioning of atmospheric organic compounds in Teflon tubing and inside an instrument used to monitor concentrations. Rapid partitioning caused time delays in instrument response that vary with tubing length and diameter, flow rate, and compound volatility. Tubing delay times of seconds to hours were described using a model that also included effects of instrument surfaces. The results can enable better design of air sampling systems.
Duseong S. Jo, Rokjin J. Park, Jaein I. Jeong, Gabriele Curci, Hyung-Min Lee, and Sang-Woo Kim
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-1104, https://doi.org/10.5194/acp-2017-1104, 2017
Preprint retracted
Adrian M. Maclean, Christopher L. Butenhoff, James W. Grayson, Kelley Barsanti, Jose L. Jimenez, and Allan K. Bertram
Atmos. Chem. Phys., 17, 13037–13048, https://doi.org/10.5194/acp-17-13037-2017, https://doi.org/10.5194/acp-17-13037-2017, 2017
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Using laboratory data, meteorological fields and a chemical transport model, we investigated how often mixing times are < 1 h within SOA in the planetary boundary layer (PBL). Based on viscosity data for alpha-pinene SOA generated using mass concentrations of ~1000 µg m −3, mixing times in biogenic SOA are < 1h most of the time.
Zhe Peng and Jose L. Jimenez
Atmos. Chem. Phys., 17, 11991–12010, https://doi.org/10.5194/acp-17-11991-2017, https://doi.org/10.5194/acp-17-11991-2017, 2017
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Oxidation flow reactors (OFRs) have been increasingly used to study atmospheric chemistry at high NO. We show that it is very difficult to obtain high-NO chemistry (in terms of RO2 fate) in OFRs by initial NO injection. Past OFR studies with combustion sources generally had too-high precursor and NOx concentrations that caused several types of experimental artifacts. A strong dilution (× 100 or larger) may be needed for such experiments to avoid undesired chemistry.
Ryan Thalman, Suzane S. de Sá, Brett B. Palm, Henrique M. J. Barbosa, Mira L. Pöhlker, M. Lizabeth Alexander, Joel Brito, Samara Carbone, Paulo Castillo, Douglas A. Day, Chongai Kuang, Antonio Manzi, Nga Lee Ng, Arthur J. Sedlacek III, Rodrigo Souza, Stephen Springston, Thomas Watson, Christopher Pöhlker, Ulrich Pöschl, Meinrat O. Andreae, Paulo Artaxo, Jose L. Jimenez, Scot T. Martin, and Jian Wang
Atmos. Chem. Phys., 17, 11779–11801, https://doi.org/10.5194/acp-17-11779-2017, https://doi.org/10.5194/acp-17-11779-2017, 2017
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Particle hygroscopicity, mixing state, and the hygroscopicity of organic components were characterized in central Amazonia for 1 year; their seasonal and diel variations were driven by a combination of primary emissions, photochemical oxidation, and boundary layer development. The relationship between the hygroscopicity of organic components and their oxidation level was examined, and the results help to reconcile the differences among the relationships observed in previous studies.
Benjamin N. Murphy, Matthew C. Woody, Jose L. Jimenez, Ann Marie G. Carlton, Patrick L. Hayes, Shang Liu, Nga L. Ng, Lynn M. Russell, Ari Setyan, Lu Xu, Jeff Young, Rahul A. Zaveri, Qi Zhang, and Havala O. T. Pye
Atmos. Chem. Phys., 17, 11107–11133, https://doi.org/10.5194/acp-17-11107-2017, https://doi.org/10.5194/acp-17-11107-2017, 2017
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We incorporate recent findings about the behavior of organic pollutants in urban airsheds into the Community Multiscale Air Quality (CMAQ) model to refine predictions of organic particulate pollution in the United States. The new techniques, which account for the volatility and ongoing chemistry of airborne organic compounds, substantially reduce biases, particularly in the winter time and near emission sources.
Jihyun Han, Meehye Lee, Xiaona Shang, Gangwoong Lee, and Louisa K. Emmons
Atmos. Chem. Phys., 17, 10619–10631, https://doi.org/10.5194/acp-17-10619-2017, https://doi.org/10.5194/acp-17-10619-2017, 2017
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Peroxyacetyl nitrate (PAN) was first measured at Gosan Climate Observatory during the fall of 2010, when PAN was better correlated with PM10 than with O3. In particular, PAN and O3 concentrations were greatly elevated in haze and the Beijing plume and much higher than those from model simulation. This study highlights the decoupling of PAN from O3 in Chinese outflows and suggests PAN as a potential indicator of overall aerosol formation in aged air masses impacted by biomass burning.
Wei Hu, Min Hu, Wei-Wei Hu, Jing Zheng, Chen Chen, Yusheng Wu, and Song Guo
Atmos. Chem. Phys., 17, 9979–10000, https://doi.org/10.5194/acp-17-9979-2017, https://doi.org/10.5194/acp-17-9979-2017, 2017
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Seasonal changes in chemical compositions, sources, and evolution for submicron aerosols in the megacity Beijing were investigated based on high-resolution AMS measurements. Carbonaceous fraction (OA+BC) constituted over 50 % of PM1 in autumn due to primary emissions, while SNA contributed 60 % to PM1 in other seasons. Secondary components (OOA+SNA) contributed ~ 60–80 % to PM1, suggesting that secondary formation played an important role in PM pollution. OA was in a relatively high oxidation state.
Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Philip Croteau, Manjula R. Canagaratna, John T. Jayne, Douglas R. Worsnop, and Jose L. Jimenez
Atmos. Meas. Tech., 10, 2897–2921, https://doi.org/10.5194/amt-10-2897-2017, https://doi.org/10.5194/amt-10-2897-2017, 2017
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Aerosol mass spectrometers (AMS) from ARI are used widely to measure the non-refractory species in PM1. Recently, a new capture vapourizer (CV) has been designed to reduce the need for a bounce-related CE correction in the commonly used standard vapourizer (SV) installed in AMS. To test the CV, the fragments, CE and size distributions of four pure inorganic species in the CV-AMS are investigated in various laboratory experiments. Results from the co-located SV-AMS are also shown as a comparison.
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.
Prettiny K. Ma, Yunliang Zhao, Allen L. Robinson, David R. Worton, Allen H. Goldstein, Amber M. Ortega, Jose L. Jimenez, Peter Zotter, André S. H. Prévôt, Sönke Szidat, and Patrick L. Hayes
Atmos. Chem. Phys., 17, 9237–9259, https://doi.org/10.5194/acp-17-9237-2017, https://doi.org/10.5194/acp-17-9237-2017, 2017
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Airborne particulate matter (PM) negatively impacts air quality in cities throughout the world. An important fraction of PM is organic aerosol. We have evaluated and developed several new models for secondary organic aerosol (SOA), which is formed from the chemical processing of gaseous precursors. Using our model results, we have quantified important SOA sources and precursors and also identified possible model parameterizations that could be used for air quality predictions.
Christopher Chan Miller, Daniel J. Jacob, Eloise A. Marais, Karen Yu, Katherine R. Travis, Patrick S. Kim, Jenny A. Fisher, Lei Zhu, Glenn M. Wolfe, Thomas F. Hanisco, Frank N. Keutsch, Jennifer Kaiser, Kyung-Eun Min, Steven S. Brown, Rebecca A. Washenfelder, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 17, 8725–8738, https://doi.org/10.5194/acp-17-8725-2017, https://doi.org/10.5194/acp-17-8725-2017, 2017
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The use of satellite glyoxal observations for estimating isoprene emissions has been limited by knowledge of the glyoxal yield from isoprene. We use SENEX aircraft observations over the southeast US to evaluate glyoxal yields from isoprene in a 3-D atmospheric model. The SENEX observations support a pathway for glyoxal formation in pristine regions that we propose here, which may have implications for improving isoprene emissions estimates from upcoming high-resolution geostationary satellites.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Matthew K. Newburn, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Ryan Thalman, Joel Brito, Samara Carbone, Paulo Artaxo, Allen H. Goldstein, Antonio O. Manzi, Rodrigo A. F. Souza, Fan Mei, John E. Shilling, Stephen R. Springston, Jian Wang, Jason D. Surratt, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 17, 6611–6629, https://doi.org/10.5194/acp-17-6611-2017, https://doi.org/10.5194/acp-17-6611-2017, 2017
Hannah M. Horowitz, Daniel J. Jacob, Yanxu Zhang, Theodore S. Dibble, Franz Slemr, Helen M. Amos, Johan A. Schmidt, Elizabeth S. Corbitt, Eloïse A. Marais, and Elsie M. Sunderland
Atmos. Chem. Phys., 17, 6353–6371, https://doi.org/10.5194/acp-17-6353-2017, https://doi.org/10.5194/acp-17-6353-2017, 2017
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Mercury is a toxic, global pollutant released to the air from human activities like coal burning. Chemical reactions in air determine how far mercury is transported before it is deposited to the environment, where it may be converted to a form that accumulates in fish. We use a 3-D atmospheric model to evaluate a new set of chemical reactions and its effects on mercury deposition. We find it is consistent with observations and leads to increased deposition to oceans, especially in the tropics.
Min Huang, Gregory R. Carmichael, R. Bradley Pierce, Duseong S. Jo, Rokjin J. Park, Johannes Flemming, Louisa K. Emmons, Kevin W. Bowman, Daven K. Henze, Yanko Davila, Kengo Sudo, Jan Eiof Jonson, Marianne Tronstad Lund, Greet Janssens-Maenhout, Frank J. Dentener, Terry J. Keating, Hilke Oetjen, and Vivienne H. Payne
Atmos. Chem. Phys., 17, 5721–5750, https://doi.org/10.5194/acp-17-5721-2017, https://doi.org/10.5194/acp-17-5721-2017, 2017
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In support of the HTAP phase 2 experiment, we conducted a number of regional-scale Sulfur Transport and dEposition Model base and sensitivity simulations over North America during May–June 2010. The STEM chemical boundary conditions were downscaled from three (GEOS-Chem, RAQMS, and ECMWF C-IFS) global chemical transport models' simulations. Analyses were performed on large spatial–temporal scales relative to HTAP1 and also on subcontinental and event scales including the use of satellite data.
Hongyu Guo, Jiumeng Liu, Karl D. Froyd, James M. Roberts, Patrick R. Veres, Patrick L. Hayes, Jose L. Jimenez, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 17, 5703–5719, https://doi.org/10.5194/acp-17-5703-2017, https://doi.org/10.5194/acp-17-5703-2017, 2017
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Fine particle pH is linked to many environmental impacts by affecting particle concentration and composition. Predicted Pasadena, CA (CalNex campaign), PM1 pH is 1.9 and PM2.5 pH 2.7, the latter higher due to sea salts. The model predicted gas–particle partitionings of HNO3–NO3−, NH3–NH4+, and HCl–Cl− are in good agreement, verifying the model predictions. A summary of contrasting locations in the US and eastern Mediterranean shows fine particles are generally highly acidic, with pH below 3.
Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Amber M. Ortega, Juliane L. Fry, Steven S. Brown, Kyle J. Zarzana, William Dube, Nicholas L. Wagner, Danielle C. Draper, Lisa Kaser, Werner Jud, Thomas Karl, Armin Hansel, Cándido Gutiérrez-Montes, and Jose L. Jimenez
Atmos. Chem. Phys., 17, 5331–5354, https://doi.org/10.5194/acp-17-5331-2017, https://doi.org/10.5194/acp-17-5331-2017, 2017
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Ambient forest air was oxidized by OH, O3, or NO3 inside an oxidation flow reactor, leading to formation of particulate matter from any gaseous precursors found in the air. Closure was achieved between the amount of particulate mass formed from O3 and NO3 oxidation and the amount predicted from speciated gaseous precursors, which was in contrast to previous results for OH oxidation (Palm et al., 2016). Elemental analysis of the particulate mass formed in the reactor is presented.
Rachel F. Silvern, Daniel J. Jacob, Patrick S. Kim, Eloise A. Marais, Jay R. Turner, Pedro Campuzano-Jost, and Jose L. Jimenez
Atmos. Chem. Phys., 17, 5107–5118, https://doi.org/10.5194/acp-17-5107-2017, https://doi.org/10.5194/acp-17-5107-2017, 2017
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We identify a fundamental discrepancy between thermodynamic equilibrium theory and observations of inorganic aerosol composition in the eastern US in summer that shows low ammonium sulfate aerosol ratios. In addition, from 2003 to 2013, while SO2 emissions have declined due to US emission controls, aerosols have become more acidic in the southeastern US. To explain these observations, we suggest that the large and increasing source of organic aerosol may be affecting thermodynamic equilibrium.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Adam P. Bateman, Zhaoheng Gong, Tristan H. Harder, Suzane S. de Sá, Bingbing Wang, Paulo Castillo, Swarup China, Yingjun Liu, Rachel E. O'Brien, Brett B. Palm, Hung-Wei Shiu, Glauber G. Cirino, Ryan Thalman, Kouji Adachi, M. Lizabeth Alexander, Paulo Artaxo, Allan K. Bertram, Peter R. Buseck, Mary K. Gilles, Jose L. Jimenez, Alexander Laskin, Antonio O. Manzi, Arthur Sedlacek, Rodrigo A. F. Souza, Jian Wang, Rahul Zaveri, and Scot T. Martin
Atmos. Chem. Phys., 17, 1759–1773, https://doi.org/10.5194/acp-17-1759-2017, https://doi.org/10.5194/acp-17-1759-2017, 2017
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The occurrence of nonliquid and liquid physical states of submicron atmospheric particulate matter (PM) downwind of an urban region in central Amazonia was investigated. Air masses representing background conditions, urban pollution, and regional- and continental-scale biomass were measured. Anthropogenic influences contributed to the presence of nonliquid PM in the atmospheric particle population, while liquid PM dominated during periods of biogenic influence.
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, https://doi.org/10.5194/acp-17-343-2017, 2017
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We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
Yaping Zhang, Brent J. Williams, Allen H. Goldstein, Kenneth S. Docherty, and Jose L. Jimenez
Atmos. Meas. Tech., 9, 5637–5653, https://doi.org/10.5194/amt-9-5637-2016, https://doi.org/10.5194/amt-9-5637-2016, 2016
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The binning method provides an alternate way to process GC–MS data in a very fast manner. It only takes a very small portion of time (days versus years) compared to the traditional GC–MS data analysis method (peak identification and integration). Furthermore, the binning method can also be applied to any data set from a measurement (mass spectrometry, spectroscopy, etc.) with additional separations (volatility, polarity, size, etc.).
Katherine R. Travis, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Lei Zhu, Karen Yu, Christopher C. Miller, Robert M. Yantosca, Melissa P. Sulprizio, Anne M. Thompson, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Ronald C. Cohen, Joshua L. Laughner, Jack E. Dibb, Samuel R. Hall, Kirk Ullmann, Glenn M. Wolfe, Illana B. Pollack, Jeff Peischl, Jonathan A. Neuman, and Xianliang Zhou
Atmos. Chem. Phys., 16, 13561–13577, https://doi.org/10.5194/acp-16-13561-2016, https://doi.org/10.5194/acp-16-13561-2016, 2016
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Ground-level ozone pollution in the Southeast US involves complex chemistry driven by anthropogenic emissions of nitrogen oxides (NOx) and biogenic emissions of isoprene. We find that US NOx emissions are overestimated nationally by as much as 50 % and that reducing model emissions by this amount results in good agreement with SEAC4RS aircraft measurements in August and September 2013. Observations of nitrate wet deposition fluxes and satellite NO2 columns further support this result.
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.
Wei Hu, Min Hu, Wei-Wei Hu, Hongya Niu, Jing Zheng, Yusheng Wu, Wentai Chen, Chen Chen, Lingyu Li, Min Shao, Shaodong Xie, and Yuanhang Zhang
Atmos. Chem. Phys., 16, 13213–13230, https://doi.org/10.5194/acp-16-13213-2016, https://doi.org/10.5194/acp-16-13213-2016, 2016
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An Aerodyne high-resolution time-of-flight AMS was deployed at a suburban site in the Sichuan Basin, southwestern China, under high emission intensity, and unique geographical and adverse meteorological conditions. OA was the most abundant component (36 %) in PM1, characterized by a relatively high oxidation state. The contributions of BBOA and BC to PM1 were high in primary emission episodes, highlighting the critical influence of biomass burning.
Xuan Zhang, Jordan E. Krechmer, Michael Groessl, Wen Xu, Stephan Graf, Michael Cubison, John T. Jayne, Jose L. Jimenez, Douglas R. Worsnop, and Manjula R. Canagaratna
Atmos. Chem. Phys., 16, 12945–12959, https://doi.org/10.5194/acp-16-12945-2016, https://doi.org/10.5194/acp-16-12945-2016, 2016
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We develop a novel two-dimensional space to probe the molecular composition of atmospheric organic aerosols.
Weiwei Hu, Brett B. Palm, Douglas A. Day, Pedro Campuzano-Jost, Jordan E. Krechmer, Zhe Peng, Suzane S. de Sá, Scot T. Martin, M. Lizabeth Alexander, Karsten Baumann, Lina Hacker, Astrid Kiendler-Scharr, Abigail R. Koss, Joost A. de Gouw, Allen H. Goldstein, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Francesco Canonaco, André S. H. Prévôt, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 11563–11580, https://doi.org/10.5194/acp-16-11563-2016, https://doi.org/10.5194/acp-16-11563-2016, 2016
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IEPOX-SOA is biogenically derived secondary organic aerosol under anthropogenic influence, which has been shown to comprise a substantial fraction of OA globally. We investigated the lifetime of ambient IEPOX-SOA in the SE US and Amazonia, with an oxidation flow reactor and thermodenuder coupled with MS-based instrumentation. The low volatility and long lifetime of IEPOX-SOA against OH radicals' oxidation (> 2 weeks) was observed, which can help to constrain OA impact on air quality and climate.
Aki Pajunoja, Weiwei Hu, Yu J. Leong, Nathan F. Taylor, Pasi Miettinen, Brett B. Palm, Santtu Mikkonen, Don R. Collins, Jose L. Jimenez, and Annele Virtanen
Atmos. Chem. Phys., 16, 11163–11176, https://doi.org/10.5194/acp-16-11163-2016, https://doi.org/10.5194/acp-16-11163-2016, 2016
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The phase state of ambient particles was inferred from bounce measurements conducted at a rural site in central Alabama during the SOAS campaign. The organic-dominated ambient particles are mostly in the liquid phase at summertime conditions but they turn semisolid when dried in the measurement setup. Bounce humidograms reveal that the hygroscopicity and oxidation of the particles decreases the liquefying RH. The effect of oxidation is emphasized by oxidation flow reactor measurements.
Giancarlo Ciarelli, Sebnem Aksoyoglu, Monica Crippa, Jose-Luis Jimenez, Eriko Nemitz, Karine Sellegri, Mikko Äijälä, Samara Carbone, Claudia Mohr, Colin O'Dowd, Laurent Poulain, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 10313–10332, https://doi.org/10.5194/acp-16-10313-2016, https://doi.org/10.5194/acp-16-10313-2016, 2016
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Recent studies based on aerosol mass spectrometer measurements revealed that the organic fraction dominates the non-refractory PM1 composition. However its representation in chemical transport models is still very challenging due to uncertainties in emission sources and formation pathways. In this study, a novel organic aerosol scheme was tested in the regional air quality model CAMx and results were compared with ambient measurements at 11 different sites in Europe.
Matthew J. Alvarado, Chantelle R. Lonsdale, Helen L. Macintyre, Huisheng Bian, Mian Chin, David A. Ridley, Colette L. Heald, Kenneth L. Thornhill, Bruce E. Anderson, Michael J. Cubison, Jose L. Jimenez, Yutaka Kondo, Lokesh K. Sahu, Jack E. Dibb, and Chien Wang
Atmos. Chem. Phys., 16, 9435–9455, https://doi.org/10.5194/acp-16-9435-2016, https://doi.org/10.5194/acp-16-9435-2016, 2016
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Understanding the scattering and absorption of light by aerosols is necessary for understanding air quality and climate change. We used data from the 2008 ARCTAS campaign to evaluate aerosol optical property models using a closure methodology that separates errors in these models from other errors in aerosol emissions, chemistry, or transport. We find that the models on average perform reasonably well, and make suggestions for how remaining biases could be reduced.
Alma Hodzic, Prasad S. Kasibhatla, Duseong S. Jo, Christopher D. Cappa, Jose L. Jimenez, Sasha Madronich, and Rokjin J. Park
Atmos. Chem. Phys., 16, 7917–7941, https://doi.org/10.5194/acp-16-7917-2016, https://doi.org/10.5194/acp-16-7917-2016, 2016
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The global budget and spatial distribution of secondary organic aerosol (SOA) are highly uncertain in chemistry-climate models, which reflects our inability to characterize all phases of the OA lifecycle. We have performed global model simulations with the newly proposed formation and removal processes (photolysis and heterogeneous chemistry) and shown that SOA is a far more dynamic system, with 4 times stronger production rates and more efficient removal mechanisms, than assumed in models.
Amber M. Ortega, Patrick L. Hayes, Zhe Peng, Brett B. Palm, Weiwei Hu, Douglas A. Day, Rui Li, Michael J. Cubison, William H. Brune, Martin Graus, Carsten Warneke, Jessica B. Gilman, William C. Kuster, Joost de Gouw, Cándido Gutiérrez-Montes, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 7411–7433, https://doi.org/10.5194/acp-16-7411-2016, https://doi.org/10.5194/acp-16-7411-2016, 2016
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An oxidation flow reactor (OFR) was deployed to study secondary organic aerosol (SOA) formation and aging of urban emissions at a wide range of OH exposures during the CalNex campaign in Pasadena, CA, in 2010. Results include linking SOA formation to short-lived reactive compounds, similar elemental composition of reactor-aged emissions to atmospheric aging, changes in OA mass due to condensation of oxidized gas-phase species and heterogeneous oxidation of particle-phase species.
Sarah A. Strode, Helen M. Worden, Megan Damon, Anne R. Douglass, Bryan N. Duncan, Louisa K. Emmons, Jean-Francois Lamarque, Michael Manyin, Luke D. Oman, Jose M. Rodriguez, Susan E. Strahan, and Simone Tilmes
Atmos. Chem. Phys., 16, 7285–7294, https://doi.org/10.5194/acp-16-7285-2016, https://doi.org/10.5194/acp-16-7285-2016, 2016
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We use global models to interpret trends in MOPITT observations of CO. Simulations with time-dependent emissions reproduce the observed trends over the eastern USA and Europe, suggesting that the emissions are reasonable for these regions. The simulations produce a positive trend over eastern China, contrary to the observed negative trend. This may indicate that the assumed emission trend over China is too positive. However, large variability in the overhead ozone column also contributes.
Simone Tilmes, Jean-Francois Lamarque, Louisa K. Emmons, Doug E. Kinnison, Dan Marsh, Rolando R. Garcia, Anne K. Smith, Ryan R. Neely, Andrew Conley, Francis Vitt, Maria Val Martin, Hiroshi Tanimoto, Isobel Simpson, Don R. Blake, and Nicola Blake
Geosci. Model Dev., 9, 1853–1890, https://doi.org/10.5194/gmd-9-1853-2016, https://doi.org/10.5194/gmd-9-1853-2016, 2016
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The state of the art Community Earth System Model, CESM1 CAM4-chem has been used to perform reference and sensitivity simulations as part of the Chemistry Climate Model Initiative (CCMI). Specifics of the model and details regarding the setup of the simulations are described. In additions, the main behavior of the model, including selected chemical species have been evaluated with climatological datasets. This paper is therefore a references for studies that use the provided model results.
Jenny A. Fisher, Daniel J. Jacob, Katherine R. Travis, Patrick S. Kim, Eloise A. Marais, Christopher Chan Miller, Karen Yu, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Jingqiu Mao, Paul O. Wennberg, John D. Crounse, Alex P. Teng, Tran B. Nguyen, Jason M. St. Clair, Ronald C. Cohen, Paul Romer, Benjamin A. Nault, Paul J. Wooldridge, Jose L. Jimenez, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Paul B. Shepson, Fulizi Xiong, Donald R. Blake, Allen H. Goldstein, Pawel K. Misztal, Thomas F. Hanisco, Glenn M. Wolfe, Thomas B. Ryerson, Armin Wisthaler, and Tomas Mikoviny
Atmos. Chem. Phys., 16, 5969–5991, https://doi.org/10.5194/acp-16-5969-2016, https://doi.org/10.5194/acp-16-5969-2016, 2016
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We use new airborne and ground-based observations from two summer 2013 campaigns in the southeastern US, interpreted with a chemical transport model, to understand the impact of isoprene and monoterpene chemistry on the atmospheric NOx budget via production of organic nitrates (RONO2). We find that a diversity of species contribute to observed RONO2. Our work implies that the NOx sink to RONO2 production is only sensitive to NOx emissions in regions where they are already low.
Catherine Wespes, Daniel Hurtmans, Louisa K. Emmons, Sarah Safieddine, Cathy Clerbaux, David P. Edwards, and Pierre-François Coheur
Atmos. Chem. Phys., 16, 5721–5743, https://doi.org/10.5194/acp-16-5721-2016, https://doi.org/10.5194/acp-16-5721-2016, 2016
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In this paper, we assess how daily ozone measurements from the Infrared Atmospheric Sounding Interferometer (IASI/MetOp) can contribute to the analyses of the processes driving O3 variability in the troposphere and the stratosphere with a set of parameterized geophysical variables, and we demonstrate the added value of IASI exceptional frequency sampling for monitoring medium- to long-term changes in global ozone concentrations in the future.
Charles A. Brock, Nicholas L. Wagner, Bruce E. Anderson, Alexis R. Attwood, Andreas Beyersdorf, Pedro Campuzano-Jost, Annmarie G. Carlton, Douglas A. Day, Glenn S. Diskin, Timothy D. Gordon, Jose L. Jimenez, Daniel A. Lack, Jin Liao, Milos Z. Markovic, Ann M. Middlebrook, Nga L. Ng, Anne E. Perring, Matthews S. Richardson, Joshua P. Schwarz, Rebecca A. Washenfelder, Andre Welti, Lu Xu, Luke D. Ziemba, and Daniel M. Murphy
Atmos. Chem. Phys., 16, 4987–5007, https://doi.org/10.5194/acp-16-4987-2016, https://doi.org/10.5194/acp-16-4987-2016, 2016
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Microscopic pollution particles make the atmosphere look hazy and also cool the earth by sending sunlight back to space. When the air is moist, these particles swell with water and scatter even more sunlight. We showed that particles formed from organic material – which dominates particulate pollution in the southeastern U.S. – does not take up water very effectively, toward the low end of most previous studies. We also found a better way to mathematically describe this swelling process.
Charles A. Brock, Nicholas L. Wagner, Bruce E. Anderson, Andreas Beyersdorf, Pedro Campuzano-Jost, Douglas A. Day, Glenn S. Diskin, Timothy D. Gordon, Jose L. Jimenez, Daniel A. Lack, Jin Liao, Milos Z. Markovic, Ann M. Middlebrook, Anne E. Perring, Matthews S. Richardson, Joshua P. Schwarz, Andre Welti, Luke D. Ziemba, and Daniel M. Murphy
Atmos. Chem. Phys., 16, 5009–5019, https://doi.org/10.5194/acp-16-5009-2016, https://doi.org/10.5194/acp-16-5009-2016, 2016
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Two research aircraft made dozens of vertical profiles over rural areas in the southeastern US in summer 2013. These measurements show that, in addition to how much pollution was present and how moist the atmosphere was, the size of the pollutant particles affected how much sunlight was reflected back to space. These measurements will help climate modelers determine which characteristics of pollution are important to predict with accuracy.
S. T. Martin, P. Artaxo, L. A. T. Machado, A. O. Manzi, R. A. F. Souza, C. Schumacher, J. Wang, M. O. Andreae, H. M. J. Barbosa, J. Fan, G. Fisch, A. H. Goldstein, A. Guenther, J. L. Jimenez, U. Pöschl, M. A. Silva Dias, J. N. Smith, and M. Wendisch
Atmos. Chem. Phys., 16, 4785–4797, https://doi.org/10.5194/acp-16-4785-2016, https://doi.org/10.5194/acp-16-4785-2016, 2016
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The Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) Experiment took place in central Amazonia throughout 2014 and 2015. The experiment focused on the complex links among vegetation, atmospheric chemistry, and aerosol production on the one hand and their connections to aerosols, clouds, and precipitation on the other, especially when altered by urban pollution. This article serves as an introduction to the special issue of publications presenting findings of this experiment.
Brent J. Williams, Yaping Zhang, Xiaochen Zuo, Raul E. Martinez, Michael J. Walker, Nathan M. Kreisberg, Allen H. Goldstein, Kenneth S. Docherty, and Jose L. Jimenez
Atmos. Meas. Tech., 9, 1569–1586, https://doi.org/10.5194/amt-9-1569-2016, https://doi.org/10.5194/amt-9-1569-2016, 2016
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The thermal desorption aerosol gas chromatograph (TAG) has been used for in situ measurements of organic marker compounds to identify atmospheric particle sources and transformation processes. Here we identify that inorganic aerosol components (e.g., nitrate and sulfate) and highly oxygenated organic components experience thermal decomposition upon sample heating. This thermal decomposition signal in the TAG system is investigated through laboratory and field data.
Zhe Peng, Douglas A. Day, Amber M. Ortega, Brett B. Palm, Weiwei Hu, Harald Stark, Rui Li, Kostas Tsigaridis, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 4283–4305, https://doi.org/10.5194/acp-16-4283-2016, https://doi.org/10.5194/acp-16-4283-2016, 2016
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Oxidation flow reactors (OFRs) are promising tools of studying atmospheric oxidation processes. Elevated concentrations of both OH and non-OH oxidants in OFRs leave room for speculation that non-OH chemistry can play a major role. Through systematic modeling, we find conditions where non-OH VOC fate is significant and show that, in most field studies of SOA using OFRs, non-OH VOC fate in OFRs was insignificant. We also provide guidelines helping OFR users avoid significant non-OH VOC oxidation.
Bruno Franco, Eloise A. Marais, Benoît Bovy, Whitney Bader, Bernard Lejeune, Ginette Roland, Christian Servais, and Emmanuel Mahieu
Atmos. Chem. Phys., 16, 4171–4189, https://doi.org/10.5194/acp-16-4171-2016, https://doi.org/10.5194/acp-16-4171-2016, 2016
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The long-term evolution of HCHO in the remote troposphere is characterized using a 27-year time series of total columns from high-resolution FTIR solar spectra recorded at Jungfraujoch. A parametric model is used to remove the effect of the HCHO diurnal variations for improving the trend determination and the comparison with columns simulated by GEOS-Chem. Sensitivity tests are performed to identify the main drivers of the HCHO seasonal and inter-annual variations, as well as their contribution.
Matthew C. Woody, Kirk R. Baker, Patrick L. Hayes, Jose L. Jimenez, Bonyoung Koo, and Havala O. T. Pye
Atmos. Chem. Phys., 16, 4081–4100, https://doi.org/10.5194/acp-16-4081-2016, https://doi.org/10.5194/acp-16-4081-2016, 2016
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In this work, organic aerosol (OA) predictions from the volatility basis set (VBS) module in the CMAQ photochemical transport model were evaluated against routine monitoring data and measurements collected during the 2010 CalNex field study. We found that the VBS module more accurately reproduced the observed primary/secondary OA split and secondary OA (SOA) mass at the CalNex Pasadena ground site compared to the traditional CMAQ OA module but still underpredicted observed SOA by ~ 5.2 ×.
Christopher D. Cappa, Shantanu H. Jathar, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, John H. Seinfeld, and Anthony S. Wexler
Atmos. Chem. Phys., 16, 3041–3059, https://doi.org/10.5194/acp-16-3041-2016, https://doi.org/10.5194/acp-16-3041-2016, 2016
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Losses of vapors to walls of chambers can negatively bias SOA formation measurements, consequently leading to low predicted SOA concentrations in air quality models. Here, we show that accounting for such vapor losses leads to substantial increases in the predicted amount of SOA formed from VOCs and to notable increases in the O : C atomic ratio in two US regions. Comparison with a variety of observational data suggests generally improved model performance when vapor wall losses are accounted for.
Brett B. Palm, Pedro Campuzano-Jost, Amber M. Ortega, Douglas A. Day, Lisa Kaser, Werner Jud, Thomas Karl, Armin Hansel, James F. Hunter, Eben S. Cross, Jesse H. Kroll, Zhe Peng, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 2943–2970, https://doi.org/10.5194/acp-16-2943-2016, https://doi.org/10.5194/acp-16-2943-2016, 2016
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Ambient pine forest air was oxidized by OH radicals in a PAM oxidation flow reactor during the BEACHON-RoMBAS campaign to study secondary organic aerosol formation. Approximately 4.4 times more secondary organic aerosol was formed in the reactor than could be explained by the volatile organic gases (VOCs) measured in ambient air. The organic aerosol formation can be explained by including an SOA yield from typically unmeasured semivolatile and intermediate-volatility organic gases (S/IVOCs).
E. A. Marais, D. J. Jacob, J. L. Jimenez, P. Campuzano-Jost, D. A. Day, W. Hu, J. Krechmer, L. Zhu, P. S. Kim, C. C. Miller, J. A. Fisher, K. Travis, K. Yu, T. F. Hanisco, G. M. Wolfe, H. L. Arkinson, H. O. T. Pye, K. D. Froyd, J. Liao, and V. F. McNeill
Atmos. Chem. Phys., 16, 1603–1618, https://doi.org/10.5194/acp-16-1603-2016, https://doi.org/10.5194/acp-16-1603-2016, 2016
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Isoprene secondary organic aerosol (SOA) is a dominant aerosol component in the southeast US, but models routinely underestimate isoprene SOA with traditional schemes based on chamber studies operated under conditions not representative of isoprene-emitting forests. We develop a new irreversible uptake mechanism to reproduce isoprene SOA yields (3.3 %) and composition, and find a factor of 2 co-benefit of SO2 emission controls on reducing sulfate and organic aerosol in the southeast US.
Y. S. La, M. Camredon, P. J. Ziemann, R. Valorso, A. Matsunaga, V. Lannuque, J. Lee-Taylor, A. Hodzic, S. Madronich, and B. Aumont
Atmos. Chem. Phys., 16, 1417–1431, https://doi.org/10.5194/acp-16-1417-2016, https://doi.org/10.5194/acp-16-1417-2016, 2016
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The potential impact of chamber walls on the loss of gaseous organic species and secondary organic aerosol (SOA) formation has been explored using the GECKO-A modeling tool, which explicitly represents SOA formation and gas-wall partitioning. The model was compared with 41 smog chamber experiments of SOA formation under OH oxidation of alkane and alkene serie. The organic vapor loss to the chamber walls is found to affect SOA yields as well as the composition of the gas and the particle phase.
A. W. H. Chan, N. M. Kreisberg, T. Hohaus, P. Campuzano-Jost, Y. Zhao, D. A. Day, L. Kaser, T. Karl, A. Hansel, A. P. Teng, C. R. Ruehl, D. T. Sueper, J. T. Jayne, D. R. Worsnop, J. L. Jimenez, S. V. Hering, and A. H. Goldstein
Atmos. Chem. Phys., 16, 1187–1205, https://doi.org/10.5194/acp-16-1187-2016, https://doi.org/10.5194/acp-16-1187-2016, 2016
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Using a novel instrument, we have made measurements of organic compounds that can exist as a gas or particle in the rural atmosphere. Through hourly measurements, we have identified the sources and atmospheric processes of these compounds, which are important for modeling the climate and health impact of these emissions.
L. M. Zamora, R. A. Kahn, M. J. Cubison, G. S. Diskin, J. L. Jimenez, Y. Kondo, G. M. McFarquhar, A. Nenes, K. L. Thornhill, A. Wisthaler, A. Zelenyuk, and L. D. Ziemba
Atmos. Chem. Phys., 16, 715–738, https://doi.org/10.5194/acp-16-715-2016, https://doi.org/10.5194/acp-16-715-2016, 2016
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Based on extensive aircraft campaigns, we quantify how biomass burning smoke affects subarctic and Arctic liquid cloud microphysical properties. Enhanced cloud albedo may decrease short-wave radiative flux by between 2 and 4 Wm2 or more in some subarctic conditions. Smoke halved average cloud droplet diameter. In one case study, it also appeared to limit droplet formation. Numerous Arctic background Aitken particles can also interact with combustion particles, perhaps affecting their properties.
J. He, Y. Zhang, S. Tilmes, L. Emmons, J.-F. Lamarque, T. Glotfelty, A. Hodzic, and F. Vitt
Geosci. Model Dev., 8, 3999–4025, https://doi.org/10.5194/gmd-8-3999-2015, https://doi.org/10.5194/gmd-8-3999-2015, 2015
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The global simulations with CB05_GE and MOZART-4x predict similar chemical profiles for major gases compared to aircraft measurements, with better agreement for the NOy profile by CB05_GE. The SOA concentrations of SOA at four sites in CONUS and organic carbon over the IMPROVE sites are better predicted by MOZART-4x. The two simulations result in a global average difference of 0.5W m-2 in simulated shortwave cloud radiative forcing, with up to 13.6W m-2 over subtropical regions.
Y. Zheng, N. Unger, A. Hodzic, L. Emmons, C. Knote, S. Tilmes, J.-F. Lamarque, and P. Yu
Atmos. Chem. Phys., 15, 13487–13506, https://doi.org/10.5194/acp-15-13487-2015, https://doi.org/10.5194/acp-15-13487-2015, 2015
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Nitrogen oxides (NOx) play an important but complex role in secondary organic aerosol (SOA) formation. In this study we update the SOA scheme in a global 3-D chemistry-climate model by implementing a 4-product volatility basis set (VBS) framework with NOx-dependent yields and simplified aging parameterizations. We find that the SOA decrease in response to a 50% reduction in anthropogenic NOx emissions is limited due to the buffering in different chemical pathways.
B. R. Ayres, H. M. Allen, D. C. Draper, S. S. Brown, R. J. Wild, J. L. Jimenez, D. A. Day, P. Campuzano-Jost, W. Hu, J. de Gouw, A. Koss, R. C. Cohen, K. C. Duffey, P. Romer, K. Baumann, E. Edgerton, S. Takahama, J. A. Thornton, B. H. Lee, F. D. Lopez-Hilfiker, C. Mohr, P. O. Wennberg, T. B. Nguyen, A. Teng, A. H. Goldstein, K. Olson, and J. L. Fry
Atmos. Chem. Phys., 15, 13377–13392, https://doi.org/10.5194/acp-15-13377-2015, https://doi.org/10.5194/acp-15-13377-2015, 2015
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This paper reports atmospheric gas- and aerosol-phase field measurements from the southeastern United States in summer 2013 to demonstrate that the oxidation of biogenic volatile organic compounds by nitrate radical produces a substantial amount of secondary organic aerosol in this region. This process, driven largely by monoterpenes, results in a comparable aerosol nitrate production rate to inorganic nitrate formation by heterogeneous uptake of HNO3 onto dust particles.
Z. Peng, D. A. Day, H. Stark, R. Li, J. Lee-Taylor, B. B. Palm, W. H. Brune, and J. L. Jimenez
Atmos. Meas. Tech., 8, 4863–4890, https://doi.org/10.5194/amt-8-4863-2015, https://doi.org/10.5194/amt-8-4863-2015, 2015
A. Lupascu, R. Easter, R. Zaveri, M. Shrivastava, M. Pekour, J. Tomlinson, Q. Yang, H. Matsui, A. Hodzic, Q. Zhang, and J. D. Fast
Atmos. Chem. Phys., 15, 12283–12313, https://doi.org/10.5194/acp-15-12283-2015, https://doi.org/10.5194/acp-15-12283-2015, 2015
W. W. Hu, P. Campuzano-Jost, B. B. Palm, D. A. Day, A. M. Ortega, P. L. Hayes, J. E. Krechmer, Q. Chen, M. Kuwata, Y. J. Liu, S. S. de Sá, K. McKinney, S. T. Martin, M. Hu, S. H. Budisulistiorini, M. Riva, J. D. Surratt, J. M. St. Clair, G. Isaacman-Van Wertz, L. D. Yee, A. H. Goldstein, S. Carbone, J. Brito, P. Artaxo, J. A. de Gouw, A. Koss, A. Wisthaler, T. Mikoviny, T. Karl, L. Kaser, W. Jud, A. Hansel, K. S. Docherty, M. L. Alexander, N. H. Robinson, H. Coe, J. D. Allan, M. R. Canagaratna, F. Paulot, and J. L. Jimenez
Atmos. Chem. Phys., 15, 11807–11833, https://doi.org/10.5194/acp-15-11807-2015, https://doi.org/10.5194/acp-15-11807-2015, 2015
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This work summarized all the studies reporting isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) measured globally by aerosol mass spectrometer and compare them with modeled gas-phase IEPOX, with results suggestive of the importance of IEPOX-SOA for regional and global OA budgets. A real-time tracer of IEPOX-SOA is thoroughly evaluated for the first time by combing multiple field and chamber studies. A quick and easy empirical method on IEPOX-SOA estimation is also presented.
P. S. Kim, D. J. Jacob, J. A. Fisher, K. Travis, K. Yu, L. Zhu, R. M. Yantosca, M. P. Sulprizio, J. L. Jimenez, P. Campuzano-Jost, K. D. Froyd, J. Liao, J. W. Hair, M. A. Fenn, C. F. Butler, N. L. Wagner, T. D. Gordon, A. Welti, P. O. Wennberg, J. D. Crounse, J. M. St. Clair, A. P. Teng, D. B. Millet, J. P. Schwarz, M. Z. Markovic, and A. E. Perring
Atmos. Chem. Phys., 15, 10411–10433, https://doi.org/10.5194/acp-15-10411-2015, https://doi.org/10.5194/acp-15-10411-2015, 2015
A. Hodzic, S. Madronich, P. S. Kasibhatla, G. Tyndall, B. Aumont, J. L. Jimenez, J. Lee-Taylor, and J. Orlando
Atmos. Chem. Phys., 15, 9253–9269, https://doi.org/10.5194/acp-15-9253-2015, https://doi.org/10.5194/acp-15-9253-2015, 2015
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Our study combines process and global chemistry modeling to investigate the potential effect of gas- and particle-phase organic photolysis reactions on the formation and lifetime of secondary organic aerosols (SOAs). Photolysis of the oxidation intermediates that partition between gas and particle phases to form SOA is not included in 3D models. Our results suggest that exposure to UV light can suppress the formation of SOA or even lead to its substantial loss (comparable to wet deposition).
J. Liu, E. Scheuer, J. Dibb, G. S. Diskin, L. D. Ziemba, K. L. Thornhill, B. E. Anderson, A. Wisthaler, T. Mikoviny, J. J. Devi, M. Bergin, A. E. Perring, M. Z. Markovic, J. P. Schwarz, P. Campuzano-Jost, D. A. Day, J. L. Jimenez, and R. J. Weber
Atmos. Chem. Phys., 15, 7841–7858, https://doi.org/10.5194/acp-15-7841-2015, https://doi.org/10.5194/acp-15-7841-2015, 2015
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Brown carbon (BrC) is found throughout the US continental troposphere during a summer of extensive biomass burning and its prevalence relative to black carbon (BC) increases with altitude. A radiative transfer model based on direct measurements of aerosol scattering and absorption by BC and BrC shows BrC reduces top-of-atmosphere forcing by 20%. A method to estimate BrC radiative forcing efficiencies from surface-based measurements is provided.
G. Zeng, J. E. Williams, J. A. Fisher, L. K. Emmons, N. B. Jones, O. Morgenstern, J. Robinson, D. Smale, C. Paton-Walsh, and D. W. T. Griffith
Atmos. Chem. Phys., 15, 7217–7245, https://doi.org/10.5194/acp-15-7217-2015, https://doi.org/10.5194/acp-15-7217-2015, 2015
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We assess the impact of biogenic emissions on CO and HCHO in the Southern Hemisphere (SH), with simulations using different emission inventories. Differences in biogenic emissions result in large differences on modelled CO in the source and the remote regions. Substantial inter-model differences exist. Models significantly underestimate observed HCHO columns in the SH, suggesting missing sources in the models. Differences in the CO/OH/CH4 chemistry lead to differences in HCHO in remote regions.
N. L. Wagner, C. A. Brock, W. M. Angevine, A. Beyersdorf, P. Campuzano-Jost, D. Day, J. A. de Gouw, G. S. Diskin, T. D. Gordon, M. G. Graus, J. S. Holloway, G. Huey, J. L. Jimenez, D. A. Lack, J. Liao, X. Liu, M. Z. Markovic, A. M. Middlebrook, T. Mikoviny, J. Peischl, A. E. Perring, M. S. Richardson, T. B. Ryerson, J. P. Schwarz, C. Warneke, A. Welti, A. Wisthaler, L. D. Ziemba, and D. M. Murphy
Atmos. Chem. Phys., 15, 7085–7102, https://doi.org/10.5194/acp-15-7085-2015, https://doi.org/10.5194/acp-15-7085-2015, 2015
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This paper investigates the summertime vertical profile of aerosol over the southeastern US using in situ measurements collected from aircraft. We use a vertical mixing model and measurements of CO to predict the vertical profile of aerosol that we would expect from vertical mixing alone and compare with the observed aerosol profile. We found a modest enhancement of aerosol in the cloudy transition layer during shallow cumulus convection and attribute the enhancement to local aerosol formation.
L. K. Emmons, S. R. Arnold, S. A. Monks, V. Huijnen, S. Tilmes, K. S. Law, J. L. Thomas, J.-C. Raut, I. Bouarar, S. Turquety, Y. Long, B. Duncan, S. Steenrod, S. Strode, J. Flemming, J. Mao, J. Langner, A. M. Thompson, D. Tarasick, E. C. Apel, D. R. Blake, R. C. Cohen, J. Dibb, G. S. Diskin, A. Fried, S. R. Hall, L. G. Huey, A. J. Weinheimer, A. Wisthaler, T. Mikoviny, J. Nowak, J. Peischl, J. M. Roberts, T. Ryerson, C. Warneke, and D. Helmig
Atmos. Chem. Phys., 15, 6721–6744, https://doi.org/10.5194/acp-15-6721-2015, https://doi.org/10.5194/acp-15-6721-2015, 2015
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Eleven 3-D tropospheric chemistry models have been compared and evaluated with observations in the Arctic during the International Polar Year (IPY 2008). Large differences are seen among the models, particularly related to the model chemistry of volatile organic compounds (VOCs) and reactive nitrogen (NOx, PAN, HNO3) partitioning. Consistency among the models in the underestimation of CO, ethane and propane indicates the emission inventory is too low for these compounds.
M. J. Cubison and J. L. Jimenez
Atmos. Meas. Tech., 8, 2333–2345, https://doi.org/10.5194/amt-8-2333-2015, https://doi.org/10.5194/amt-8-2333-2015, 2015
S. R. Arnold, L. K. Emmons, S. A. Monks, K. S. Law, D. A. Ridley, S. Turquety, S. Tilmes, J. L. Thomas, I. Bouarar, J. Flemming, V. Huijnen, J. Mao, B. N. Duncan, S. Steenrod, Y. Yoshida, J. Langner, and Y. Long
Atmos. Chem. Phys., 15, 6047–6068, https://doi.org/10.5194/acp-15-6047-2015, https://doi.org/10.5194/acp-15-6047-2015, 2015
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The extent to which forest fires produce the air pollutant and greenhouse gas ozone (O3) in the atmosphere at high latitudes in not well understood. We have compared how fire emissions produce O3 and its precursors in several models of atmospheric chemistry. We find enhancements in O3 in air dominated by fires in all models, which increase on average as fire emissions age. We also find that in situ O3 production in the Arctic is sensitive to details of organic chemistry and vertical lifting.
P. L. Hayes, A. G. Carlton, K. R. Baker, R. Ahmadov, R. A. Washenfelder, S. Alvarez, B. Rappenglück, J. B. Gilman, W. C. Kuster, J. A. de Gouw, P. Zotter, A. S. H. Prévôt, S. Szidat, T. E. Kleindienst, J. H. Offenberg, P. K. Ma, and J. L. Jimenez
Atmos. Chem. Phys., 15, 5773–5801, https://doi.org/10.5194/acp-15-5773-2015, https://doi.org/10.5194/acp-15-5773-2015, 2015
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(1) Four different parameterizations for the formation and chemical evolution of secondary organic aerosol (SOA) are evaluated using a box model representing the Los Angeles region during the CalNex campaign.
(2) The SOA formed only from the oxidation of VOCs is insufficient to explain the observed SOA concentrations.
(3) The amount of SOA mass formed from diesel vehicle emissions is estimated to be 16-27%.
(4) Modeled SOA depends strongly on the P-S/IVOC volatility distribution.
S. Tilmes, J.-F. Lamarque, L. K. Emmons, D. E. Kinnison, P.-L. Ma, X. Liu, S. Ghan, C. Bardeen, S. Arnold, M. Deeter, F. Vitt, T. Ryerson, J. W. Elkins, F. Moore, J. R. Spackman, and M. Val Martin
Geosci. Model Dev., 8, 1395–1426, https://doi.org/10.5194/gmd-8-1395-2015, https://doi.org/10.5194/gmd-8-1395-2015, 2015
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The Community Atmosphere Model (CAM), version 5, is now coupled to extensive tropospheric and stratospheric chemistry, called CAM5-chem, and is available in addition to CAM4-chem in the Community Earth System Model (CESM) version 1.2. Both configurations are well suited as tools for atmospheric chemistry modeling studies in the troposphere and lower stratosphere.
K. R. Baker, A. G. Carlton, T. E. Kleindienst, J. H. Offenberg, M. R. Beaver, D. R. Gentner, A. H. Goldstein, P. L. Hayes, J. L. Jimenez, J. B. Gilman, J. A. de Gouw, M. C. Woody, H. O. T. Pye, J. T. Kelly, M. Lewandowski, M. Jaoui, P. S. Stevens, W. H. Brune, Y.-H. Lin, C. L. Rubitschun, and J. D. Surratt
Atmos. Chem. Phys., 15, 5243–5258, https://doi.org/10.5194/acp-15-5243-2015, https://doi.org/10.5194/acp-15-5243-2015, 2015
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This work details the evaluation of PM2.5 carbon, VOC precursors, and OH estimated by the CMAQ photochemical transport model using routine and special measurements from the 2010 CalNex field study. Here, CMAQ and most recent emissions inventory (2011 NEI) are used to generate model PM2.5 OC estimates that are examined in novel ways including primary vs. secondary formation, fossil vs. contemporary carbon, OH and HO2 evaluation, and the relationship between key VOC precursors and SOC tracers.
B. Franco, F. Hendrick, M. Van Roozendael, J.-F. Müller, T. Stavrakou, E. A. Marais, B. Bovy, W. Bader, C. Fayt, C. Hermans, B. Lejeune, G. Pinardi, C. Servais, and E. Mahieu
Atmos. Meas. Tech., 8, 1733–1756, https://doi.org/10.5194/amt-8-1733-2015, https://doi.org/10.5194/amt-8-1733-2015, 2015
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Formaldehyde (HCHO) amounts are obtained from ground-based Fourier transform infrared solar spectra and UV-visible Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) scans recorded at the Jungfraujoch station (46.5°N, 8.0°E, 3580m a.s.l.). Using HCHO amounts simulated by the chemical transport models GEOS-Chem and IMAGES as intermediates, comparisons reveal that FTIR and MAX-DOAS provide complementary products for the HCHO retrieval.
Q. Chen, D. K. Farmer, L. V. Rizzo, T. Pauliquevis, M. Kuwata, T. G. Karl, A. Guenther, J. D. Allan, H. Coe, M. O. Andreae, U. Pöschl, J. L. Jimenez, P. Artaxo, and S. T. Martin
Atmos. Chem. Phys., 15, 3687–3701, https://doi.org/10.5194/acp-15-3687-2015, https://doi.org/10.5194/acp-15-3687-2015, 2015
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Submicron particle mass concentration in the Amazon during the wet season of 2008 was dominated by organic material. The PMF analysis finds a comparable importance of gas-phase (gas-to-particle condensation) and particle-phase (reactive uptake of isoprene oxidation products, especially of epoxydiols to acidic haze, fog, or cloud droplets) production of secondary organic material during the study period, together accounting for >70% of the organic-particle mass concentration.
S. A. Monks, S. R. Arnold, L. K. Emmons, K. S. Law, S. Turquety, B. N. Duncan, J. Flemming, V. Huijnen, S. Tilmes, J. Langner, J. Mao, Y. Long, J. L. Thomas, S. D. Steenrod, J. C. Raut, C. Wilson, M. P. Chipperfield, G. S. Diskin, A. Weinheimer, H. Schlager, and G. Ancellet
Atmos. Chem. Phys., 15, 3575–3603, https://doi.org/10.5194/acp-15-3575-2015, https://doi.org/10.5194/acp-15-3575-2015, 2015
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Multi-model simulations of Arctic CO, O3 and OH are evaluated using observations. Models show highly variable concentrations but the relative importance of emission regions and types is robust across the models, demonstrating the importance of biomass burning as a source. Idealised tracer experiments suggest that some of the model spread is due to variations in simulated transport from Europe in winter and from Asia throughout the year.
J. A. Fisher, S. R. Wilson, G. Zeng, J. E. Williams, L. K. Emmons, R. L. Langenfelds, P. B. Krummel, and L. P. Steele
Atmos. Chem. Phys., 15, 3217–3239, https://doi.org/10.5194/acp-15-3217-2015, https://doi.org/10.5194/acp-15-3217-2015, 2015
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The Southern Hemisphere (SH) serves as an important test bed for evaluating our understanding of the processes that drive the composition of the clean background atmosphere. Using data from two aircraft campaigns, combined with four atmospheric chemistry models, we find a large sensitivity in the remote SH to biogenic emissions and their subsequent chemistry and transport. Future model evaluation and measurement campaigns should prioritize reducing uncertainties in these processes.
A. Ripoll, M. C. Minguillón, J. Pey, J. L. Jimenez, D. A. Day, Y. Sosedova, F. Canonaco, A. S. H. Prévôt, X. Querol, and A. Alastuey
Atmos. Chem. Phys., 15, 2935–2951, https://doi.org/10.5194/acp-15-2935-2015, https://doi.org/10.5194/acp-15-2935-2015, 2015
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Real-time measurements of inorganic (sulfate, nitrate, ammonium, chloride and black carbon (BC)) and organic submicron aerosols from a continental background site (Montsec, MSC, 1570m a.s.l.) in the western Mediterranean Basin (WMB) were conducted for 10 months (July 2011 - April 2012) with an aerosol chemical speciation monitor (ACSM). The ACSM was co-located with other online and offline PM1 measurements. Analyses of the hourly, diurnal, and seasonal variations are presented here.
M. Val Martin, C. L. Heald, J.-F. Lamarque, S. Tilmes, L. K. Emmons, and B. A. Schichtel
Atmos. Chem. Phys., 15, 2805–2823, https://doi.org/10.5194/acp-15-2805-2015, https://doi.org/10.5194/acp-15-2805-2015, 2015
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We present for the first time the relative effect of climate, emissions, and land use change on ozone and PM25 over the United States, focusing on the national parks. Air quality in 2050 will likely be dominated by emission patterns, but climate and land use changes alone can lead to a substantial increase in air pollution over most of the US, with important implications for O3 air quality, visibility and ecosystem health degradation in the national parks.
C. Viatte, K. Strong, J. Hannigan, E. Nussbaumer, L. K. Emmons, S. Conway, C. Paton-Walsh, J. Hartley, J. Benmergui, and J. Lin
Atmos. Chem. Phys., 15, 2227–2246, https://doi.org/10.5194/acp-15-2227-2015, https://doi.org/10.5194/acp-15-2227-2015, 2015
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Seven tropospheric species (CO, HCN, C2H6, C2H2, CH3OH, HCOOH, and H2CO) released by biomass burning events transported to the high Arctic were monitored with two sets of FTIR measurements, located at Eureka (Nunavut, Canada) and Thule (Greenland), from 2008 to 2012. We compared these data sets with the MOZART-4 chemical transport model to help improve its simulations in the Arctic. Emission factors of these biomass burning products were derived and compared to the literature.
B. A. Nault, C. Garland, S. E. Pusede, P. J. Wooldridge, K. Ullmann, S. R. Hall, and R. C. Cohen
Atmos. Meas. Tech., 8, 987–997, https://doi.org/10.5194/amt-8-987-2015, https://doi.org/10.5194/amt-8-987-2015, 2015
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We report the first atmospheric measurement of methyl peroxy nitrate (CH3O2NO2) and describe an experimental strategy to obtain NO2 observations free of methyl peroxy nitrate (CH3O2NO2). The accuracy of the CH3O2NO2 measurements are (+/- 40%) with a LOD of 15 pptv/min. We observe that CH3O2NO2 is ubiquitous in the upper troposphere with median mixing ratios of 100 to 200 pptv, and its composition to the total NOy budget is comparable to HNO3.
B. Yuan, P. R. Veres, C. Warneke, J. M. Roberts, J. B. Gilman, A. Koss, P. M. Edwards, M. Graus, W. C. Kuster, S.-M. Li, R. J. Wild, S. S. Brown, W. P. Dubé, B. M. Lerner, E. J. Williams, J. E. Johnson, P. K. Quinn, T. S. Bates, B. Lefer, P. L. Hayes, J. L. Jimenez, R. J. Weber, R. Zamora, B. Ervens, D. B. Millet, B. Rappenglück, and J. A. de Gouw
Atmos. Chem. Phys., 15, 1975–1993, https://doi.org/10.5194/acp-15-1975-2015, https://doi.org/10.5194/acp-15-1975-2015, 2015
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In this work, secondary formation of formic acid at an urban site and a site in an oil and gas production region is studied. We investigated various gas phase formation pathways of formic acid, including those recently proposed, using a box model. The contributions from aerosol-related processes, fog events and air-snow exchange to formic acid are also quantified.
J. Lee-Taylor, A. Hodzic, S. Madronich, B. Aumont, M. Camredon, and R. Valorso
Atmos. Chem. Phys., 15, 595–615, https://doi.org/10.5194/acp-15-595-2015, https://doi.org/10.5194/acp-15-595-2015, 2015
M. R. Canagaratna, J. L. Jimenez, J. H. Kroll, Q. Chen, S. H. Kessler, P. Massoli, L. Hildebrandt Ruiz, E. Fortner, L. R. Williams, K. R. Wilson, J. D. Surratt, N. M. Donahue, J. T. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, https://doi.org/10.5194/acp-15-253-2015, 2015
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Atomic oxygen-to-carbon (O:C), hydrogen-to-carbon (H:C), and organic mass-to-organic carbon (OM:OC) ratios of ambient organic aerosol (OA) species provide key constraints for understanding their sources and impacts. Here an improved method for obtaining accurate O:C, H:C, and OM:OC with a widely used aerosol mass spectrometer is developed. These results imply that OA is more oxidized than previously estimated and indicate the need for new chemical mechanisms that simulate ambient oxidation.
C. Knote, A. Hodzic, and J. L. Jimenez
Atmos. Chem. Phys., 15, 1–18, https://doi.org/10.5194/acp-15-1-2015, https://doi.org/10.5194/acp-15-1-2015, 2015
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Organic material found in ambient aerosol is mostly formed through the oxidation of gaseous precursors. It is semi-volatile under atmospheric conditions, and it continuously partitions between the gas and particle phases. At the same time, it is also highly water soluble. We show that wet and especially dry deposition of semi-volatile organic compounds in the gas phase are major indirect removal pathways for the particle phase, and hence need to be accurately accounted for in modeling studies.
T. Amnuaylojaroen, M. C. Barth, L. K. Emmons, G. R. Carmichael, J. Kreasuwun, S. Prasitwattanaseree, and S. Chantara
Atmos. Chem. Phys., 14, 12983–13012, https://doi.org/10.5194/acp-14-12983-2014, https://doi.org/10.5194/acp-14-12983-2014, 2014
F. L. Herron-Thorpe, G. H. Mount, L. K. Emmons, B. K. Lamb, D. A. Jaffe, N. L. Wigder, S. H. Chung, R. Zhang, M. D. Woelfle, and J. K. Vaughan
Atmos. Chem. Phys., 14, 12533–12551, https://doi.org/10.5194/acp-14-12533-2014, https://doi.org/10.5194/acp-14-12533-2014, 2014
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Wildfire season simulations from an air quality forecast system for the Pacific Northwest were compared to surface monitor observations across the region and NASA Earth Observing System satellite retrievals of plume top, nitrogen dioxide, aerosol optical depth, and carbon monoxide. This study discusses why the Community Multi-scale Air Quality model predictions under-predicted secondary organic aerosol (SOA) production for events when fire emissions were transported large distances.
M. N. Deeter, S. Martínez-Alonso, D. P. Edwards, L. K. Emmons, J. C. Gille, H. M. Worden, C. Sweeney, J. V. Pittman, B. C. Daube, and S. C. Wofsy
Atmos. Meas. Tech., 7, 3623–3632, https://doi.org/10.5194/amt-7-3623-2014, https://doi.org/10.5194/amt-7-3623-2014, 2014
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The MOPITT Version 6 product for carbon monoxide (CO) incorporates several enhancements. First, a geolocation bias has been eliminated. Second, the new variable a priori for CO concentrations is based on simulations performed with the CAM-Chem chemical transport model for the years 2000-2009. Third, required meteorological fields are extracted from the MERRA reanalysis. Finally, a retrieval bias in the upper troposphere was substantially reduced. Validation results are presented.
Y. Y. Cui, A. Hodzic, J. N. Smith, J. Ortega, J. Brioude, H. Matsui, E. J. T. Levin, A. Turnipseed, P. Winkler, and B. de Foy
Atmos. Chem. Phys., 14, 11011–11029, https://doi.org/10.5194/acp-14-11011-2014, https://doi.org/10.5194/acp-14-11011-2014, 2014
K. Tsigaridis, N. Daskalakis, M. Kanakidou, P. J. Adams, P. Artaxo, R. Bahadur, Y. Balkanski, S. E. Bauer, N. Bellouin, A. Benedetti, T. Bergman, T. K. Berntsen, J. P. Beukes, H. Bian, K. S. Carslaw, M. Chin, G. Curci, T. Diehl, R. C. Easter, S. J. Ghan, S. L. Gong, A. Hodzic, C. R. Hoyle, T. Iversen, S. Jathar, J. L. Jimenez, J. W. Kaiser, A. Kirkevåg, D. Koch, H. Kokkola, Y. H Lee, G. Lin, X. Liu, G. Luo, X. Ma, G. W. Mann, N. Mihalopoulos, J.-J. Morcrette, J.-F. Müller, G. Myhre, S. Myriokefalitakis, N. L. Ng, D. O'Donnell, J. E. Penner, L. Pozzoli, K. J. Pringle, L. M. Russell, M. Schulz, J. Sciare, Ø. Seland, D. T. Shindell, S. Sillman, R. B. Skeie, D. Spracklen, T. Stavrakou, S. D. Steenrod, T. Takemura, P. Tiitta, S. Tilmes, H. Tost, T. van Noije, P. G. van Zyl, K. von Salzen, F. Yu, Z. Wang, Z. Wang, R. A. Zaveri, H. Zhang, K. Zhang, Q. Zhang, and X. Zhang
Atmos. Chem. Phys., 14, 10845–10895, https://doi.org/10.5194/acp-14-10845-2014, https://doi.org/10.5194/acp-14-10845-2014, 2014
J. D. Fast, J. Allan, R. Bahreini, J. Craven, L. Emmons, R. Ferrare, P. L. Hayes, A. Hodzic, J. Holloway, C. Hostetler, J. L. Jimenez, H. Jonsson, S. Liu, Y. Liu, A. Metcalf, A. Middlebrook, J. Nowak, M. Pekour, A. Perring, L. Russell, A. Sedlacek, J. Seinfeld, A. Setyan, J. Shilling, M. Shrivastava, S. Springston, C. Song, R. Subramanian, J. W. Taylor, V. Vinoj, Q. Yang, R. A. Zaveri, and Q. Zhang
Atmos. Chem. Phys., 14, 10013–10060, https://doi.org/10.5194/acp-14-10013-2014, https://doi.org/10.5194/acp-14-10013-2014, 2014
E. A. Marais, D. J. Jacob, A. Guenther, K. Chance, T. P. Kurosu, J. G. Murphy, C. E. Reeves, and H. O. T. Pye
Atmos. Chem. Phys., 14, 7693–7703, https://doi.org/10.5194/acp-14-7693-2014, https://doi.org/10.5194/acp-14-7693-2014, 2014
S. Saarikoski, S. Carbone, M. J. Cubison, R. Hillamo, P. Keronen, C. Sioutas, D. R. Worsnop, and J. L. Jimenez
Atmos. Meas. Tech., 7, 2121–2135, https://doi.org/10.5194/amt-7-2121-2014, https://doi.org/10.5194/amt-7-2121-2014, 2014
J. Ortega, A. Turnipseed, A. B. Guenther, T. G. Karl, D. A. Day, D. Gochis, J. A. Huffman, A. J. Prenni, E. J. T. Levin, S. M. Kreidenweis, P. J. DeMott, Y. Tobo, E. G. Patton, A. Hodzic, Y. Y. Cui, P. C. Harley, R. S. Hornbrook, E. C. Apel, R. K. Monson, A. S. D. Eller, J. P. Greenberg, M. C. Barth, P. Campuzano-Jost, B. B. Palm, J. L. Jimenez, A. C. Aiken, M. K. Dubey, C. Geron, J. Offenberg, M. G. Ryan, P. J. Fornwalt, S. C. Pryor, F. N. Keutsch, J. P. DiGangi, A. W. H. Chan, A. H. Goldstein, G. M. Wolfe, S. Kim, L. Kaser, R. Schnitzhofer, A. Hansel, C. A. Cantrell, R. L. Mauldin, and J. N. Smith
Atmos. Chem. Phys., 14, 6345–6367, https://doi.org/10.5194/acp-14-6345-2014, https://doi.org/10.5194/acp-14-6345-2014, 2014
C. Knote, A. Hodzic, J. L. Jimenez, R. Volkamer, J. J. Orlando, S. Baidar, J. Brioude, J. Fast, D. R. Gentner, A. H. Goldstein, P. L. Hayes, W. B. Knighton, H. Oetjen, A. Setyan, H. Stark, R. Thalman, G. Tyndall, R. Washenfelder, E. Waxman, and Q. Zhang
Atmos. Chem. Phys., 14, 6213–6239, https://doi.org/10.5194/acp-14-6213-2014, https://doi.org/10.5194/acp-14-6213-2014, 2014
M. Crippa, F. Canonaco, V. A. Lanz, M. Äijälä, J. D. Allan, S. Carbone, G. Capes, D. Ceburnis, M. Dall'Osto, D. A. Day, P. F. DeCarlo, M. Ehn, A. Eriksson, E. Freney, L. Hildebrandt Ruiz, R. Hillamo, J. L. Jimenez, H. Junninen, A. Kiendler-Scharr, A.-M. Kortelainen, M. Kulmala, A. Laaksonen, A. A. Mensah, C. Mohr, E. Nemitz, C. O'Dowd, J. Ovadnevaite, S. N. Pandis, T. Petäjä, L. Poulain, S. Saarikoski, K. Sellegri, E. Swietlicki, P. Tiitta, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 6159–6176, https://doi.org/10.5194/acp-14-6159-2014, https://doi.org/10.5194/acp-14-6159-2014, 2014
M. Li, Q. Zhang, D. G. Streets, K. B. He, Y. F. Cheng, L. K. Emmons, H. Huo, S. C. Kang, Z. Lu, M. Shao, H. Su, X. Yu, and Y. Zhang
Atmos. Chem. Phys., 14, 5617–5638, https://doi.org/10.5194/acp-14-5617-2014, https://doi.org/10.5194/acp-14-5617-2014, 2014
S. G. Howell, A. D. Clarke, S. Freitag, C. S. McNaughton, V. Kapustin, V. Brekovskikh, J.-L. Jimenez, and M. J. Cubison
Atmos. Chem. Phys., 14, 5073–5087, https://doi.org/10.5194/acp-14-5073-2014, https://doi.org/10.5194/acp-14-5073-2014, 2014
E. J. T. Levin, A. J. Prenni, B. B. Palm, D. A. Day, P. Campuzano-Jost, P. M. Winkler, S. M. Kreidenweis, P. J. DeMott, J. L. Jimenez, and J. N. Smith
Atmos. Chem. Phys., 14, 2657–2667, https://doi.org/10.5194/acp-14-2657-2014, https://doi.org/10.5194/acp-14-2657-2014, 2014
J. J. Ensberg, P. L. Hayes, J. L. Jimenez, J. B. Gilman, W. C. Kuster, J. A. de Gouw, J. S. Holloway, T. D. Gordon, S. Jathar, A. L. Robinson, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 2383–2397, https://doi.org/10.5194/acp-14-2383-2014, https://doi.org/10.5194/acp-14-2383-2014, 2014
R. L. N. Yatavelli, H. Stark, S. L. Thompson, J. R. Kimmel, M. J. Cubison, D. A. Day, P. Campuzano-Jost, B. B. Palm, A. Hodzic, J. A. Thornton, J. T. Jayne, D. R. Worsnop, and J. L. Jimenez
Atmos. Chem. Phys., 14, 1527–1546, https://doi.org/10.5194/acp-14-1527-2014, https://doi.org/10.5194/acp-14-1527-2014, 2014
A. M. Ortega, D. A. Day, M. J. Cubison, W. H. Brune, D. Bon, J. A. de Gouw, and J. L. Jimenez
Atmos. Chem. Phys., 13, 11551–11571, https://doi.org/10.5194/acp-13-11551-2013, https://doi.org/10.5194/acp-13-11551-2013, 2013
J. L. Fry, D. C. Draper, K. J. Zarzana, P. Campuzano-Jost, D. A. Day, J. L. Jimenez, S. S. Brown, R. C. Cohen, L. Kaser, A. Hansel, L. Cappellin, T. Karl, A. Hodzic Roux, A. Turnipseed, C. Cantrell, B. L. Lefer, and N. Grossberg
Atmos. Chem. Phys., 13, 8585–8605, https://doi.org/10.5194/acp-13-8585-2013, https://doi.org/10.5194/acp-13-8585-2013, 2013
L. Menut, B. Bessagnet, D. Khvorostyanov, M. Beekmann, N. Blond, A. Colette, I. Coll, G. Curci, G. Foret, A. Hodzic, S. Mailler, F. Meleux, J.-L. Monge, I. Pison, G. Siour, S. Turquety, M. Valari, R. Vautard, and M. G. Vivanco
Geosci. Model Dev., 6, 981–1028, https://doi.org/10.5194/gmd-6-981-2013, https://doi.org/10.5194/gmd-6-981-2013, 2013
J. A. Huffman, A. J. Prenni, P. J. DeMott, C. Pöhlker, R. H. Mason, N. H. Robinson, J. Fröhlich-Nowoisky, Y. Tobo, V. R. Després, E. Garcia, D. J. Gochis, E. Harris, I. Müller-Germann, C. Ruzene, B. Schmer, B. Sinha, D. A. Day, M. O. Andreae, J. L. Jimenez, M. Gallagher, S. M. Kreidenweis, A. K. Bertram, and U. Pöschl
Atmos. Chem. Phys., 13, 6151–6164, https://doi.org/10.5194/acp-13-6151-2013, https://doi.org/10.5194/acp-13-6151-2013, 2013
Q. J. Zhang, M. Beekmann, F. Drewnick, F. Freutel, J. Schneider, M. Crippa, A. S. H. Prevot, U. Baltensperger, L. Poulain, A. Wiedensohler, J. Sciare, V. Gros, A. Borbon, A. Colomb, V. Michoud, J.-F. Doussin, H. A. C. Denier van der Gon, M. Haeffelin, J.-C. Dupont, G. Siour, H. Petetin, B. Bessagnet, S. N. Pandis, A. Hodzic, O. Sanchez, C. Honoré, and O. Perrussel
Atmos. Chem. Phys., 13, 5767–5790, https://doi.org/10.5194/acp-13-5767-2013, https://doi.org/10.5194/acp-13-5767-2013, 2013
E. C. Browne, K.-E. Min, P. J. Wooldridge, E. Apel, D. R. Blake, W. H. Brune, C. A. Cantrell, M. J. Cubison, G. S. Diskin, J. L. Jimenez, A. J. Weinheimer, P. O. Wennberg, A. Wisthaler, and R. C. Cohen
Atmos. Chem. Phys., 13, 4543–4562, https://doi.org/10.5194/acp-13-4543-2013, https://doi.org/10.5194/acp-13-4543-2013, 2013
J. L. Thomas, J.-C. Raut, K. S. Law, L. Marelle, G. Ancellet, F. Ravetta, J. D. Fast, G. Pfister, L. K. Emmons, G. S. Diskin, A. Weinheimer, A. Roiger, and H. Schlager
Atmos. Chem. Phys., 13, 3825–3848, https://doi.org/10.5194/acp-13-3825-2013, https://doi.org/10.5194/acp-13-3825-2013, 2013
T. L. Lathem, A. J. Beyersdorf, K. L. Thornhill, E. L. Winstead, M. J. Cubison, A. Hecobian, J. L. Jimenez, R. J. Weber, B. E. Anderson, and A. Nenes
Atmos. Chem. Phys., 13, 2735–2756, https://doi.org/10.5194/acp-13-2735-2013, https://doi.org/10.5194/acp-13-2735-2013, 2013
L. K. Emmons, P. G. Hess, J.-F. Lamarque, and G. G. Pfister
Geosci. Model Dev., 5, 1531–1542, https://doi.org/10.5194/gmd-5-1531-2012, https://doi.org/10.5194/gmd-5-1531-2012, 2012
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Development of the CMA-GFS-AERO 4D-Var assimilation system v1.0 – Part 1: System description and preliminary experimental results
Optimized dynamic mode decomposition for reconstruction and forecasting of atmospheric chemistry data
Interpolating turbulent heat fluxes missing from a prairie observation on the Tibetan Plateau using artificial intelligence models
Carbon dioxide plume dispersion simulated at the hectometer scale using DALES: model formulation and observational evaluation
Low-level jets in the North and Baltic seas: mesoscale model sensitivity and climatology using WRF V4.2.1
SynRad v1.0: a radar forward operator to simulate synthetic weather radar observations from volcanic ash clouds
Chempath 1.0: an open-source pathway analysis program for photochemical models
PALACE v1.0: Paranal Airglow Line And Continuum Emission model
Atmospheric moisture tracking with WAM2layers v3
A new set of indicators for model evaluation complementing FAIRMODE's modelling quality objective (MQO)
Impact of multiple radar wind profiler data assimilation on convective-scale short-term rainfall forecasts: OSSE studies over the Beijing–Tianjin–Hebei region
New submodel for emissions from Explosive Volcanic ERuptions (EVER v1.1) within the Modular Earth Submodel System (MESSy, version 2.55.1)
Quantifying the oscillatory evolution of simulated boundary-layer cloud fields using Gaussian process regression
Numerical investigations on the modelling of ultrafine particles in SSH-aerosol-v1.3a: size resolution and redistribution
The third Met Office Unified Model–JULES Regional Atmosphere and Land Configuration, RAL3
The sensitivity of aerosol data assimilation to vertical profiles: case study of dust storm assimilation with LOTOS-EUROS v2.2
Knowledge-inspired fusion strategies for the inference of PM2.5 values with a neural network
Tuning the ICON-A 2.6.4 climate model with machine-learning-based emulators and history matching
A novel method for quantifying the contribution of regional transport to PM2.5 in Beijing (2013–2020): combining machine learning with concentration-weighted trajectory analysis
Quantification of CO2 hotspot emissions from OCO-3 SAM CO2 satellite images using deep learning methods
Diagnosis of winter precipitation types using the spectral bin model (version 1DSBM-19M): comparison of five methods using ICE-POP 2018 field experiment data
Improving winter condition simulations in SURFEX-TEB v9.0 with a multi-layer snow model and ice
UA-ICON with the NWP physics package (version ua-icon-2.1): mean state and variability of the middle atmosphere
Integrated Methane Inversion (IMI) 2.0: an improved research and stakeholder tool for monitoring total methane emissions with high resolution worldwide using TROPOMI satellite observations
HTAP3 Fires: towards a multi-model, multi-pollutant study of fire impacts
Using a data-driven statistical model to better evaluate surface turbulent heat fluxes in weather and climate numerical models: a demonstration study
Pochva: a new hydro-thermal process model in soil, snow, and vegetation for application in atmosphere numerical models
ClimKern v1.2: a new Python package and kernel repository for calculating radiative feedbacks
Accounting for effects of coagulation and model uncertainties in particle number concentration estimates based on measurements from sampling lines – a Bayesian inversion approach with SLIC v1.0
Top-down CO emission estimates using TROPOMI CO data in the TM5-4DVAR (r1258) inverse modeling suit
The Multi-Compartment Hg Modeling and Analysis Project (MCHgMAP): mercury modeling to support international environmental policy
Similarity-based analysis of atmospheric organic compounds for machine learning applications
The Atmospheric Potential Oxygen forward Model Intercomparison Project (APO-MIP1): Evaluating simulated atmospheric transport of air-sea gas exchange tracers and APO flux products
Porting the Meso-NH atmospheric model on different GPU architectures for the next generation of supercomputers (version MESONH-v55-OpenACC)
Estimation of aerosol and cloud radiative heating rate in the tropical stratosphere using a radiative kernel method
Development of a High-Resolution Coupled SHiELD-MOM6 Model. Part I – Model Overview, Coupling Technique, and Validation in a Regional Setup
Evaluation of dust emission and land surface schemes in predicting a mega Asian dust storm over South Korea using WRF-Chem
CoCoMET v1.0: A Unified Open-Source Toolkit for Atmospheric Object Tracking and Analysis
Sensitivity studies of a four-dimensional local ensemble transform Kalman filter coupled with WRF-Chem version 3.9.1 for improving particulate matter simulation accuracy
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Inclusion of the ECMWF ecRad radiation scheme (v1.5.0) in the MAR (v3.14), regional evaluation for Belgium, and assessment of surface shortwave spectral fluxes at Uccle
Development of a fast radiative transfer model for ground-based microwave radiometers (ARMS-gb v1.0): validation and comparison to RTTOV-gb
Indian Institute of Tropical Meteorology (IITM) High-Resolution Global Forecast Model version 1: an attempt to resolve monsoon prediction deadlock
Cell-tracking-based framework for assessing nowcasting model skill in reproducing growth and decay of convective rainfall
NeuralMie (v1.0): an aerosol optics emulator
A REtrieval Method for optical and physical Aerosol Properties in the stratosphere (REMAPv1)
Simulation performance of planetary boundary layer schemes in WRF v4.3.1 for near-surface wind over the western Sichuan Basin: a single-site assessment
FootNet v1.0: development of a machine learning emulator of atmospheric transport
Updates and evaluation of NOAA's online-coupled air quality model version 7 (AQMv7) within the Unified Forecast System
Quantifying the analysis uncertainty for nowcasting application
Yongzhu Liu, Xiaoye Zhang, Wei Han, Chao Wang, Wenxing Jia, Deying Wang, Zhaorong Zhuang, and Xueshun Shen
Geosci. Model Dev., 18, 4855–4876, https://doi.org/10.5194/gmd-18-4855-2025, https://doi.org/10.5194/gmd-18-4855-2025, 2025
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In order to investigate the feedbacks of chemical data assimilation on meteorological forecasts, we developed a strongly coupled aerosol–meteorology four-dimensional variational (4D-Var) assimilation system, CMA-GFS-AERO 4D-Var, based on the framework of the incremental analysis scheme of the China Meteorological Administration Global Forecasting System (CMA-GFS) operational global numerical weather model. The results show that assimilating BC (black carbon) observations can generate analysis increments not only for BC but also for atmospheric variables.
Meghana Velagar, Christoph Keller, and J. Nathan Kutz
Geosci. Model Dev., 18, 4667–4684, https://doi.org/10.5194/gmd-18-4667-2025, https://doi.org/10.5194/gmd-18-4667-2025, 2025
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We develop the data-driven method of dynamic mode decomposition for producing a robust and stable surrogate reduced-order model of atmospheric chemistry dynamics. The model is computationally efficient, provides interpretable patterns of activity, and produces uncertainty quantification metrics. It is ideal for the forecasting of atmospheric chemistry in a computationally tractable manner.
Quanzhe Hou, Zhiqiu Gao, Zexia Duan, and Minghui Yu
Geosci. Model Dev., 18, 4625–4641, https://doi.org/10.5194/gmd-18-4625-2025, https://doi.org/10.5194/gmd-18-4625-2025, 2025
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This study evaluates various machine learning and statistical methods for interpolating turbulent heat flux data over the Tibetan Plateau. The Transformer model showed the best performance, leading to the development of the Transformer_CNN model, which combines global and local attention mechanisms. Results show that Transformer_CNN outperforms the other models and was successfully applied to interpolate heat flux data from 2007 to 2016.
Arseniy Karagodin-Doyennel, Fredrik Jansson, Bart J. H. van Stratum, Hugo Denier van der Gon, Jordi Vilà-Guerau de Arellano, and Sander Houweling
Geosci. Model Dev., 18, 4571–4599, https://doi.org/10.5194/gmd-18-4571-2025, https://doi.org/10.5194/gmd-18-4571-2025, 2025
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We introduce a new simulation platform based on the Dutch Atmospheric Large-Eddy Simulation (DALES) to simulate carbon dioxide (CO2) emissions and their dispersion in turbulent environments at a hectometer resolution. This model incorporates both anthropogenic emission inventories and online ecosystem fluxes. Simulation results for the main urban area in the Netherlands demonstrate the strong potential of DALES to improve CO2 emission modeling and to support mitigation strategies.
Bjarke T. E. Olsen, Andrea N. Hahmann, Nicolas G. Alonso-de-Linaje, Mark Žagar, and Martin Dörenkämper
Geosci. Model Dev., 18, 4499–4533, https://doi.org/10.5194/gmd-18-4499-2025, https://doi.org/10.5194/gmd-18-4499-2025, 2025
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Low-level jets (LLJs) are strong winds in the lower atmosphere that are important for wind energy as turbines get taller. This study compares a weather model (WRF) with real data across five North and Baltic Sea sites. Adjusting the model improved accuracy over the widely used ERA5. In key offshore regions, LLJs occur 10–15 % of the time and significantly boost wind power, especially in spring and summer, contributing up to 30 % of total capacity in some areas.
Vishnu Nair, Anujah Mohanathan, Michael Herzog, David G. Macfarlane, and Duncan A. Robertson
Geosci. Model Dev., 18, 4417–4432, https://doi.org/10.5194/gmd-18-4417-2025, https://doi.org/10.5194/gmd-18-4417-2025, 2025
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A numerical model that simulates the measurement processes behind the ground-based radars used to detect volcanic ash clouds is introduced. Using weather radars to detect volcanic clouds is not ideal, as fine ash particles are smaller than raindrops and remain undetected. We evaluate the performance of weather radars to study ash clouds and to identify optimal frequencies that balance the trade-off between a higher return signal and the higher path attenuation that comes at these higher frequencies.
Daniel Garduno Ruiz, Colin Goldblatt, and Anne-Sofie Ahm
Geosci. Model Dev., 18, 4433–4454, https://doi.org/10.5194/gmd-18-4433-2025, https://doi.org/10.5194/gmd-18-4433-2025, 2025
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Photochemical models describe how the composition of the atmosphere changes due to chemical reactions, transport, and other processes. These models are useful for studying the composition of the Earth's and other planets' atmospheres. Understanding the results of these models can be difficult. Here, we build on previous work to develop open-source code that can identify the reaction chains (pathways) that produce the results of these models, facilitating the understanding of these results.
Stefan Noll, Carsten Schmidt, Patrick Hannawald, Wolfgang Kausch, and Stefan Kimeswenger
Geosci. Model Dev., 18, 4353–4398, https://doi.org/10.5194/gmd-18-4353-2025, https://doi.org/10.5194/gmd-18-4353-2025, 2025
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Non-thermal emission from chemical reactions in the Earth's middle und upper atmosphere strongly contributes to the brightness of the night sky below about 2.3 µm. The new Paranal Airglow Line And Continuum Emission model calculates the emission spectrum and its variability with an unprecedented accuracy. Relying on a large spectroscopic data set from astronomical spectrographs and theoretical molecular/atomic data, this model is valuable for airglow research and astronomical observatories.
Peter Kalverla, Imme Benedict, Chris Weijenborg, and Ruud J. van der Ent
Geosci. Model Dev., 18, 4335–4352, https://doi.org/10.5194/gmd-18-4335-2025, https://doi.org/10.5194/gmd-18-4335-2025, 2025
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We introduce a new version of WAM2layers (Water Accounting Model – 2 layers), a computer program that tracks how the weather brings water from one place to another. It uses data from weather and climate models, whose resolution is steadily increasing. Processing the latest data had become a challenge, and the updates presented here ensure that WAM2layers runs smoothly again. We also made it easier to use the program and to understand its source code. This makes it more transparent, reliable, and easier to maintain.
Alexander de Meij, Cornelis Cuvelier, Philippe Thunis, and Enrico Pisoni
Geosci. Model Dev., 18, 4231–4245, https://doi.org/10.5194/gmd-18-4231-2025, https://doi.org/10.5194/gmd-18-4231-2025, 2025
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We assess relevance and utility indicators by evaluating nine Copernicus Atmospheric Monitoring Service models in calculated air pollutant values. For NO2, the results highlight difficulties at traffic stations. For PM2.5 and PM10 the bias and winter–summer gradients reveal issues. O3 evaluation shows that seasonal gradients are useful. Overall, the indicators reveal model limitations, yet there is a need to reconsider the strictness of some indicators for certain pollutants.
Juan Zhao, Jianping Guo, and Xiaohui Zheng
Geosci. Model Dev., 18, 4075–4101, https://doi.org/10.5194/gmd-18-4075-2025, https://doi.org/10.5194/gmd-18-4075-2025, 2025
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A series of observing system simulation experiments are conducted to assess the impact of multiple radar wind profiler (RWP) networks on convective-scale numerical weather prediction. Results from three southwest-type heavy rainfall cases in the Beijing–Tianjin–Hebei region suggest the added forecast skill of ridge and foothill networks associated with the Taihang Mountains over the existing RWP network. This research provides valuable guidance for designing optimal RWP networks in the region.
Matthias Kohl, Christoph Brühl, Jennifer Schallock, Holger Tost, Patrick Jöckel, Adrian Jost, Steffen Beirle, Michael Höpfner, and Andrea Pozzer
Geosci. Model Dev., 18, 3985–4007, https://doi.org/10.5194/gmd-18-3985-2025, https://doi.org/10.5194/gmd-18-3985-2025, 2025
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SO2 from explosive volcanic eruptions reaching the stratosphere can oxidize and form sulfur aerosols, potentially persisting for several years. We developed a new submodel, Explosive Volcanic ERuptions (EVER), that seamlessly includes stratospheric volcanic SO2 emissions in global numerical simulations based on a novel standard historical model setup, successfully evaluated with satellite observations. Sensitivity studies on the Nabro eruption in 2011 evaluate different emission methods.
Gunho Loren Oh and Philip H. Austin
Geosci. Model Dev., 18, 3921–3940, https://doi.org/10.5194/gmd-18-3921-2025, https://doi.org/10.5194/gmd-18-3921-2025, 2025
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It is difficult to study the behaviour of a cloud field due to internal fluctuations and observational noise. We perform a high-resolution simulation of the boundary-layer cloud field and introduce statistical and numerical techniques, including machine-learning models, to study the evolution of the cloud field, which shows a periodic behaviour. We aim to use the numerical techniques to identify the underlying behaviour within noisy observations.
Oscar Jacquot and Karine Sartelet
Geosci. Model Dev., 18, 3965–3984, https://doi.org/10.5194/gmd-18-3965-2025, https://doi.org/10.5194/gmd-18-3965-2025, 2025
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Modelling the size distribution and the number concentration is important to represent ultrafine particles. A new analytic formulation is presented to compute coagulation partition coefficients, allowing us to lower the numerical diffusion associated with the resolution of aerosol dynamics. The significance of this effect is assessed in a 0D box model and over greater Paris with a chemistry transport model, using different size resolutions of the particle distribution.
Mike Bush, David L. A. Flack, Huw W. Lewis, Sylvia I. Bohnenstengel, Chris J. Short, Charmaine Franklin, Adrian P. Lock, Martin Best, Paul Field, Anne McCabe, Kwinten Van Weverberg, Segolene Berthou, Ian Boutle, Jennifer K. Brooke, Seb Cole, Shaun Cooper, Gareth Dow, John Edwards, Anke Finnenkoetter, Kalli Furtado, Kate Halladay, Kirsty Hanley, Margaret A. Hendry, Adrian Hill, Aravindakshan Jayakumar, Richard W. Jones, Humphrey Lean, Joshua C. K. Lee, Andy Malcolm, Marion Mittermaier, Saji Mohandas, Stuart Moore, Cyril Morcrette, Rachel North, Aurore Porson, Susan Rennie, Nigel Roberts, Belinda Roux, Claudio Sanchez, Chun-Hsu Su, Simon Tucker, Simon Vosper, David Walters, James Warner, Stuart Webster, Mark Weeks, Jonathan Wilkinson, Michael Whitall, Keith D. Williams, and Hugh Zhang
Geosci. Model Dev., 18, 3819–3855, https://doi.org/10.5194/gmd-18-3819-2025, https://doi.org/10.5194/gmd-18-3819-2025, 2025
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RAL configurations define settings for the Unified Model atmosphere and Joint UK Land Environment Simulator. The third version of the Regional Atmosphere and Land (RAL3) science configuration for kilometre- and sub-kilometre-scale modelling represents a major advance compared to previous versions (RAL2) by delivering a common science definition for applications in tropical and mid-latitude regions. RAL3 has more realistic precipitation distributions and an improved representation of clouds and visibility.
Mijie Pang, Jianbing Jin, Ting Yang, Xi Chen, Arjo Segers, Batjargal Buyantogtokh, Yixuan Gu, Jiandong Li, Hai Xiang Lin, Hong Liao, and Wei Han
Geosci. Model Dev., 18, 3781–3798, https://doi.org/10.5194/gmd-18-3781-2025, https://doi.org/10.5194/gmd-18-3781-2025, 2025
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Aerosol data assimilation has gained popularity as it combines the advantages of modelling and observation. However, few studies have addressed the challenges in the prior vertical structure. Different observations are assimilated to examine the sensitivity of assimilation to vertical structure. Results show that assimilation can optimize the dust field in general. However, if the prior introduces an incorrect structure, the assimilation can significantly deteriorate the integrity of the aerosol profile.
Matthieu Dabrowski, José Mennesson, Jérôme Riedi, Chaabane Djeraba, and Pierre Nabat
Geosci. Model Dev., 18, 3707–3733, https://doi.org/10.5194/gmd-18-3707-2025, https://doi.org/10.5194/gmd-18-3707-2025, 2025
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This work focuses on the prediction of aerosol concentration values at the ground level, which are a strong indicator of air quality, using artificial neural networks. A study of different variables and their efficiency as inputs for these models is also proposed and reveals that the best results are obtained when using all of them. Comparison between network architectures and information fusion methods allows for the extraction of knowledge on the most efficient methods in the context of this study.
Pauline Bonnet, Lorenzo Pastori, Mierk Schwabe, Marco Giorgetta, Fernando Iglesias-Suarez, and Veronika Eyring
Geosci. Model Dev., 18, 3681–3706, https://doi.org/10.5194/gmd-18-3681-2025, https://doi.org/10.5194/gmd-18-3681-2025, 2025
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Tuning a climate model means adjusting uncertain parameters in the model to best match observations like the global radiation balance and cloud cover. This is usually done by running many simulations of the model with different settings, which can be time-consuming and relies heavily on expert knowledge. To make this process faster and more objective, we developed a machine learning emulator to create a large ensemble and apply a method called history matching to find the best settings.
Kang Hu, Hong Liao, Dantong Liu, Jianbing Jin, Lei Chen, Siyuan Li, Yangzhou Wu, Changhao Wu, Shitong Zhao, Xiaotong Jiang, Ping Tian, Kai Bi, Ye Wang, and Delong Zhao
Geosci. Model Dev., 18, 3623–3634, https://doi.org/10.5194/gmd-18-3623-2025, https://doi.org/10.5194/gmd-18-3623-2025, 2025
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This study combines machine learning with concentration-weighted trajectory analysis to quantify regional transport PM2.5. From 2013–2020, local emissions dominated Beijing's pollution events. The Air Pollution Prevention and Control Action Plan reduced regional transport pollution, but the eastern region showed the smallest decrease. Beijing should prioritize local emission reduction while considering the east region's contributions in future strategies.
Joffrey Dumont Le Brazidec, Pierre Vanderbecken, Alban Farchi, Grégoire Broquet, Gerrit Kuhlmann, and Marc Bocquet
Geosci. Model Dev., 18, 3607–3622, https://doi.org/10.5194/gmd-18-3607-2025, https://doi.org/10.5194/gmd-18-3607-2025, 2025
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We developed a deep learning method to estimate CO2 emissions from power plants using satellite images. Trained and validated on simulated data, our model accurately predicts emissions despite challenges like cloud cover. When applied to real OCO3 satellite images, the results closely match reported emissions. This study shows that neural networks trained on simulations can effectively analyse real satellite data, offering a new way to monitor CO2 emissions from space.
Wonbae Bang, Jacob T. Carlin, Kwonil Kim, Alexander V. Ryzhkov, Guosheng Liu, and GyuWon Lee
Geosci. Model Dev., 18, 3559–3581, https://doi.org/10.5194/gmd-18-3559-2025, https://doi.org/10.5194/gmd-18-3559-2025, 2025
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Microphysics model-based diagnosis, such as the spectral bin model (SBM), has recently been attempted to diagnose winter precipitation types. In this study, the accuracy of SBM-based precipitation type diagnosis is compared with other traditional methods. SBM has a relatively higher accuracy for dry-snow and wet-snow events, whereas it has lower accuracy for rain events. When the microphysics scheme in the SBM was optimized for the corresponding region, the accuracy for rain events improved.
Gabriel Colas, Valéry Masson, François Bouttier, Ludovic Bouilloud, Laura Pavan, and Virve Karsisto
Geosci. Model Dev., 18, 3453–3472, https://doi.org/10.5194/gmd-18-3453-2025, https://doi.org/10.5194/gmd-18-3453-2025, 2025
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In winter, snow- and ice-covered artificial surfaces are important aspects of the urban climate. They may influence the magnitude of the urban heat island effect, but this is still unclear. In this study, we improved the representation of the snow and ice cover in the Town Energy Balance (TEB) urban climate model. Evaluations have shown that the results are promising for using TEB to study the climate of cold cities.
Markus Kunze, Christoph Zülicke, Tarique A. Siddiqui, Claudia C. Stephan, Yosuke Yamazaki, Claudia Stolle, Sebastian Borchert, and Hauke Schmidt
Geosci. Model Dev., 18, 3359–3385, https://doi.org/10.5194/gmd-18-3359-2025, https://doi.org/10.5194/gmd-18-3359-2025, 2025
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We present the Icosahedral Nonhydrostatic (ICON) general circulation model with an upper-atmospheric extension with the physics package for numerical weather prediction (UA-ICON(NWP)). We optimized the parameters for the gravity wave parameterizations and achieved realistic modeling of the thermal and dynamic states of the mesopause regions. UA-ICON(NWP) now shows a realistic frequency of major sudden stratospheric warmings and well-represented solar tides in temperature.
Lucas A. Estrada, Daniel J. Varon, Melissa Sulprizio, Hannah Nesser, Zichong Chen, Nicholas Balasus, Sarah E. Hancock, Megan He, James D. East, Todd A. Mooring, Alexander Oort Alonso, Joannes D. Maasakkers, Ilse Aben, Sabour Baray, Kevin W. Bowman, John R. Worden, Felipe J. Cardoso-Saldaña, Emily Reidy, and Daniel J. Jacob
Geosci. Model Dev., 18, 3311–3330, https://doi.org/10.5194/gmd-18-3311-2025, https://doi.org/10.5194/gmd-18-3311-2025, 2025
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Reducing emissions of methane, a powerful greenhouse gas, is a top policy concern for mitigating anthropogenic climate change. The Integrated Methane Inversion (IMI) is an advanced, cloud-based software that translates satellite observations into actionable emissions data. Here we present IMI version 2.0 with vastly expanded capabilities. These updates enable a wider range of scientific and stakeholder applications from individual basin to global scales with continuous emissions monitoring.
Cynthia H. Whaley, Tim Butler, Jose A. Adame, Rupal Ambulkar, Steve R. Arnold, Rebecca R. Buchholz, Benjamin Gaubert, Douglas S. Hamilton, Min Huang, Hayley Hung, Johannes W. Kaiser, Jacek W. Kaminski, Christoph Knote, Gerbrand Koren, Jean-Luc Kouassi, Meiyun Lin, Tianjia Liu, Jianmin Ma, Kasemsan Manomaiphiboon, Elisa Bergas Masso, Jessica L. McCarty, Mariano Mertens, Mark Parrington, Helene Peiro, Pallavi Saxena, Saurabh Sonwani, Vanisa Surapipith, Damaris Y. T. Tan, Wenfu Tang, Veerachai Tanpipat, Kostas Tsigaridis, Christine Wiedinmyer, Oliver Wild, Yuanyu Xie, and Paquita Zuidema
Geosci. Model Dev., 18, 3265–3309, https://doi.org/10.5194/gmd-18-3265-2025, https://doi.org/10.5194/gmd-18-3265-2025, 2025
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The multi-model experiment design of the HTAP3 Fires project takes a multi-pollutant approach to improving our understanding of transboundary transport of wildland fire and agricultural burning emissions and their impacts. The experiments are designed with the goal of answering science policy questions related to fires. The options for the multi-model approach, including inputs, outputs, and model setup, are discussed, and the official recommendations for the project are presented.
Maurin Zouzoua, Sophie Bastin, Fabienne Lohou, Marie Lothon, Marjolaine Chiriaco, Mathilde Jome, Cécile Mallet, Laurent Barthes, and Guylaine Canut
Geosci. Model Dev., 18, 3211–3239, https://doi.org/10.5194/gmd-18-3211-2025, https://doi.org/10.5194/gmd-18-3211-2025, 2025
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This study proposes using a statistical model to freeze errors due to differences in environmental forcing when evaluating the surface turbulent heat fluxes from numerical simulations with observations. The statistical model is first built with observations and then applied to the simulated environment to generate possibly observed fluxes. This novel method provides insight into differently evaluating the numerical formulation of turbulent heat fluxes with a long period of observational data.
Oxana Drofa
Geosci. Model Dev., 18, 3175–3209, https://doi.org/10.5194/gmd-18-3175-2025, https://doi.org/10.5194/gmd-18-3175-2025, 2025
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This paper presents the result of many years of effort of the author, who developed an original mathematical numerical model of heat and moisture exchange processes in soil, vegetation, and snow. The author relied on her 30 years of research experience in atmospheric numerical modelling. The presented model is the fruit of the author's research on physical processes at the surface–atmosphere interface and their numerical approximation and aims at improving numerical weather forecasting and climate simulations.
Tyler P. Janoski, Ivan Mitevski, Ryan J. Kramer, Michael Previdi, and Lorenzo M. Polvani
Geosci. Model Dev., 18, 3065–3079, https://doi.org/10.5194/gmd-18-3065-2025, https://doi.org/10.5194/gmd-18-3065-2025, 2025
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We developed ClimKern, a Python package and radiative kernel repository, to simplify calculating radiative feedbacks and make climate sensitivity studies more reproducible. Testing of ClimKern with sample climate model data reveals that radiative kernel choice may be more important than previously thought, especially in polar regions. Our work highlights the need for kernel sensitivity analyses to be included in future studies.
Matti Niskanen, Aku Seppänen, Henri Oikarinen, Miska Olin, Panu Karjalainen, Santtu Mikkonen, and Kari Lehtinen
Geosci. Model Dev., 18, 2983–3001, https://doi.org/10.5194/gmd-18-2983-2025, https://doi.org/10.5194/gmd-18-2983-2025, 2025
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Particle size is a key factor determining the properties of aerosol particles which have a major influence on the climate and on human health. When measuring the particle sizes, however, sometimes the sampling lines that transfer the aerosol to the measurement device distort the size distribution, making the measurement unreliable. We propose a method to correct for the distortions and estimate the true particle sizes, improving measurement accuracy.
Johann Rasmus Nüß, Nikos Daskalakis, Fabian Günther Piwowarczyk, Angelos Gkouvousis, Oliver Schneising, Michael Buchwitz, Maria Kanakidou, Maarten C. Krol, and Mihalis Vrekoussis
Geosci. Model Dev., 18, 2861–2890, https://doi.org/10.5194/gmd-18-2861-2025, https://doi.org/10.5194/gmd-18-2861-2025, 2025
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We estimate carbon monoxide emissions through inverse modeling, an approach where measurements of tracers in the atmosphere are fed to a model to calculate backwards in time (inverse) where the tracers came from. We introduce measurements from a new satellite instrument and show that, in most places globally, these on their own sufficiently constrain the emissions. This alleviates the need for additional datasets, which could shorten the delay for future carbon monoxide source estimates.
Ashu Dastoor, Hélène Angot, Johannes Bieser, Flora Brocza, Brock Edwards, Aryeh Feinberg, Xinbin Feng, Benjamin Geyman, Charikleia Gournia, Yipeng He, Ian M. Hedgecock, Ilia Ilyin, Jane Kirk, Che-Jen Lin, Igor Lehnherr, Robert Mason, David McLagan, Marilena Muntean, Peter Rafaj, Eric M. Roy, Andrei Ryjkov, Noelle E. Selin, Francesco De Simone, Anne L. Soerensen, Frits Steenhuisen, Oleg Travnikov, Shuxiao Wang, Xun Wang, Simon Wilson, Rosa Wu, Qingru Wu, Yanxu Zhang, Jun Zhou, Wei Zhu, and Scott Zolkos
Geosci. Model Dev., 18, 2747–2860, https://doi.org/10.5194/gmd-18-2747-2025, https://doi.org/10.5194/gmd-18-2747-2025, 2025
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This paper introduces the Multi-Compartment Mercury (Hg) Modeling and Analysis Project (MCHgMAP) aimed at informing the effectiveness evaluations of two multilateral environmental agreements: the Minamata Convention on Mercury and the Convention on Long-Range Transboundary Air Pollution. The experimental design exploits a variety of models (atmospheric, land, oceanic ,and multimedia mass balance models) to assess the short- and long-term influences of anthropogenic Hg releases into the environment.
Hilda Sandström and Patrick Rinke
Geosci. Model Dev., 18, 2701–2724, https://doi.org/10.5194/gmd-18-2701-2025, https://doi.org/10.5194/gmd-18-2701-2025, 2025
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Machine learning has the potential to aid the identification of organic molecules involved in aerosol formation. Yet, progress is stalled by a lack of curated atmospheric molecular datasets. Here, we compared atmospheric compounds with large molecular datasets used in machine learning and found minimal overlap with similarity algorithms. Our result underlines the need for collaborative efforts to curate atmospheric molecular data to facilitate machine learning models in atmospheric sciences.
Yuming Jin, Britton B. Stephens, Matthew C. Long, Naveen Chandra, Frédéric Chevallier, Joram J. D. Hooghiem, Ingrid T. Luijkx, Shamil Maksyutov, Eric J. Morgan, Yosuke Niwa, Prabir K. Patra, Christian Rödenbeck, and Jesse Vance
EGUsphere, https://doi.org/10.5194/egusphere-2025-1736, https://doi.org/10.5194/egusphere-2025-1736, 2025
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We carry out a comprehensive atmospheric transport model (ATM) intercomparison project. This project aims to evaluate errors in ATMs and three air-sea O2 exchange products by comparing model simulations with observations collected from surface stations, ships, and aircraft. We also present a model evaluation framework to independently quantify transport-related and flux-related biases that contribute to model-observation discrepancies in atmospheric tracer distributions.
Juan Escobar, Philippe Wautelet, Joris Pianezze, Florian Pantillon, Thibaut Dauhut, Christelle Barthe, and Jean-Pierre Chaboureau
Geosci. Model Dev., 18, 2679–2700, https://doi.org/10.5194/gmd-18-2679-2025, https://doi.org/10.5194/gmd-18-2679-2025, 2025
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The Meso-NH weather research code is adapted for GPUs using OpenACC, leading to significant performance and energy efficiency improvements. Called MESONH-v55-OpenACC, it includes enhanced memory management, communication optimizations and a new solver. On the AMD MI250X Adastra platform, it achieved up to 6× speedup and 2.3× energy efficiency gain compared to CPUs. Storm simulations at 100 m resolution show positive results, positioning the code for future use on exascale supercomputers.
Jie Gao, Yi Huang, Jonathon S. Wright, Ke Li, Tao Geng, and Qiurun Yu
Geosci. Model Dev., 18, 2569–2586, https://doi.org/10.5194/gmd-18-2569-2025, https://doi.org/10.5194/gmd-18-2569-2025, 2025
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The aerosol in the upper troposphere and stratosphere is highly variable, and its radiative effect is poorly understood. To estimate this effect, the radiative kernel is constructed and applied. The results show that the kernels can reproduce aerosol radiative effects and are expected to simulate stratospheric aerosol radiative effects. This approach reduces computational expense, is consistent with radiative model calculations, and can be applied to atmospheric models with speed requirements.
Joseph Mouallem, Kun Gao, Brandon G. Reichl, Lauren Chilutti, Lucas Harris, Rusty Benson, Niki Zadeh, Jing Chen, Jan-Huey Chen, and Cheng Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2025-1690, https://doi.org/10.5194/egusphere-2025-1690, 2025
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We introduce a new high-resolution model that couple the atmosphere and ocean to better simulate extreme weather events. It combines GFDL’s advanced atmospheric and ocean models with a powerful coupling system that allows robust and efficient two-way interactions. Simulations show the model accurately captures hurricane behavior and its impact on the ocean. It also runs efficiently on supercomputers. This model is a key step toward improving extreme weather forecast.
Ji Won Yoon, Seungyeon Lee, Ebony Lee, and Seon Ki Park
Geosci. Model Dev., 18, 2303–2328, https://doi.org/10.5194/gmd-18-2303-2025, https://doi.org/10.5194/gmd-18-2303-2025, 2025
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This study evaluates the Weather Research and Forecasting Model (WRF) coupled with Chemistry (WRF-Chem) to predict a mega Asian dust storm (ADS) over South Korea on 28–29 March 2021. We assessed combinations of five dust emission and four land surface schemes by analyzing meteorological and air quality variables. The best scheme combination reduced the root mean square error (RMSE) for particulate matter 10 (PM10) by up to 29.6 %, demonstrating the highest performance.
Travis Hahn, Hershel Weiner, Calvin Brooks, Jie Xi Li, Siddhant Gupta, and Dié Wang
EGUsphere, https://doi.org/10.5194/egusphere-2025-1328, https://doi.org/10.5194/egusphere-2025-1328, 2025
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Understanding how clouds evolve is important for improving weather predictions, but existing tools for tracking cloud changes are complex and difficult to compare. To address this, we developed the Community Cloud Model Evaluation Toolkit (CoCoMET) that makes it easier to analyze clouds in both models and observations. By simplifying data processing, standardizing results, and introducing new analysis features, CoCoMET helps researchers better evaluate cloud behavior and improve models.
Jianyu Lin, Tie Dai, Lifang Sheng, Weihang Zhang, Shangfei Hai, and Yawen Kong
Geosci. Model Dev., 18, 2231–2248, https://doi.org/10.5194/gmd-18-2231-2025, https://doi.org/10.5194/gmd-18-2231-2025, 2025
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The effectiveness of this assimilation system and its sensitivity to the ensemble member size and length of the assimilation window are investigated. This study advances our understanding of the selection of basic parameters in the four-dimensional local ensemble transform Kalman filter assimilation system and the performance of ensemble simulation in a particulate-matter-polluted environment.
Jens Peter Karolus Wenceslaus Frankemölle, Johan Camps, Pieter De Meutter, and Johan Meyers
Geosci. Model Dev., 18, 1989–2003, https://doi.org/10.5194/gmd-18-1989-2025, https://doi.org/10.5194/gmd-18-1989-2025, 2025
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To detect anomalous radioactivity in the environment, it is paramount that we understand the natural background level. In this work, we propose a statistical model to describe the most likely background level and the associated uncertainty in a network of dose rate detectors. We train, verify, and validate the model using real environmental data. Using the model, we show that we can correctly predict the background level in a subset of the detector network during a known
anomalous event.
Jean-François Grailet, Robin J. Hogan, Nicolas Ghilain, David Bolsée, Xavier Fettweis, and Marilaure Grégoire
Geosci. Model Dev., 18, 1965–1988, https://doi.org/10.5194/gmd-18-1965-2025, https://doi.org/10.5194/gmd-18-1965-2025, 2025
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The MAR (Modèle Régional Atmosphérique) is a regional climate model used for weather forecasting and studying the climate over various regions. This paper presents an update of MAR thanks to which it can precisely decompose solar radiation, in particular in the UV (ultraviolet) and photosynthesis ranges, both being critical to human health and ecosystems. As a first application of this new capability, this paper presents a method for predicting UV indices with MAR.
Yi-Ning Shi, Jun Yang, Wei Han, Lujie Han, Jiajia Mao, Wanlin Kan, and Fuzhong Weng
Geosci. Model Dev., 18, 1947–1964, https://doi.org/10.5194/gmd-18-1947-2025, https://doi.org/10.5194/gmd-18-1947-2025, 2025
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Direct assimilation of observations from ground-based microwave radiometers (GMRs) holds significant potential for improving forecast accuracy. Radiative transfer models (RTMs) play a crucial role in direct data assimilation. In this study, we introduce a new RTM, the Advanced Radiative Transfer Modeling System – Ground-Based (ARMS-gb), designed to simulate brightness temperatures observed by GMRs along with their Jacobians. Several enhancements have been incorporated to achieve higher accuracy.
R. Phani Murali Krishna, Siddharth Kumar, A. Gopinathan Prajeesh, Peter Bechtold, Nils Wedi, Kumar Roy, Malay Ganai, B. Revanth Reddy, Snehlata Tirkey, Tanmoy Goswami, Radhika Kanase, Sahadat Sarkar, Medha Deshpande, and Parthasarathi Mukhopadhyay
Geosci. Model Dev., 18, 1879–1894, https://doi.org/10.5194/gmd-18-1879-2025, https://doi.org/10.5194/gmd-18-1879-2025, 2025
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The High-Resolution Global Forecast Model (HGFM) is an advanced iteration of the operational Global Forecast System (GFS) model. HGFM can produce forecasts at a spatial scale of ~6 km in tropics. It demonstrates improved accuracy in short- to medium-range weather prediction over the Indian region, with notable success in predicting extreme events. Further, the model will be entrusted to operational forecasting agencies after validation and testing.
Jenna Ritvanen, Seppo Pulkkinen, Dmitri Moisseev, and Daniele Nerini
Geosci. Model Dev., 18, 1851–1878, https://doi.org/10.5194/gmd-18-1851-2025, https://doi.org/10.5194/gmd-18-1851-2025, 2025
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Nowcasting models struggle with the rapid evolution of heavy rain, and common verification methods are unable to describe how accurately the models predict the growth and decay of heavy rain. We propose a framework to assess model performance. In the framework, convective cells are identified and tracked in the forecasts and observations, and the model skill is then evaluated by comparing differences between forecast and observed cells. We demonstrate the framework with four open-source models.
Andrew Geiss and Po-Lun Ma
Geosci. Model Dev., 18, 1809–1827, https://doi.org/10.5194/gmd-18-1809-2025, https://doi.org/10.5194/gmd-18-1809-2025, 2025
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Particles in the Earth's atmosphere strongly impact the planet's energy budget, and atmosphere simulations require accurate representation of their interaction with light. This work introduces two approaches to represent light scattering by small particles. The first is a scattering simulator based on Mie theory implemented in Python. The second is a neural network emulator that is more accurate than existing methods and is fast enough to be used in climate and weather simulations.
Andrin Jörimann, Timofei Sukhodolov, Beiping Luo, Gabriel Chiodo, Graham Mann, and Thomas Peter
EGUsphere, https://doi.org/10.5194/egusphere-2025-145, https://doi.org/10.5194/egusphere-2025-145, 2025
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Aerosol particles in the stratosphere affect our climate. Climate models therefore need an accurate description of their properties and evolution. Satellites measure how strongly aerosol particles extinguish light passing through the stratosphere. We describe a method to use such aerosol extinction data to retrieve the number and sizes of the aerosol particles and calculate their optical effects. The resulting data sets for models are validated against ground-based and balloon observations.
Qin Wang, Bo Zeng, Gong Chen, and Yaoting Li
Geosci. Model Dev., 18, 1769–1784, https://doi.org/10.5194/gmd-18-1769-2025, https://doi.org/10.5194/gmd-18-1769-2025, 2025
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This study evaluates the performance of four planetary boundary layer (PBL) schemes in near-surface wind fields over the Sichuan Basin, China. Using 112 sensitivity experiments with the Weather Research and Forecasting (WRF) model and focusing on 28 wind events, it is found that wind direction was less sensitive to the PBL schemes. The quasi-normal scale elimination (QNSE) scheme captured temporal variations best, while the Mellor–Yamada–Janjić (MYJ) scheme had the least error in wind speed.
Tai-Long He, Nikhil Dadheech, Tammy M. Thompson, and Alexander J. Turner
Geosci. Model Dev., 18, 1661–1671, https://doi.org/10.5194/gmd-18-1661-2025, https://doi.org/10.5194/gmd-18-1661-2025, 2025
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It is computationally expensive to infer greenhouse gas (GHG) emissions using atmospheric observations. This is partly due to the detailed model used to represent atmospheric transport. We demonstrate how a machine learning (ML) model can be used to simulate high-resolution atmospheric transport. This type of ML model will help estimate GHG emissions using dense observations, which are becoming increasingly common with the proliferation of urban monitoring networks and geostationary satellites.
Wei Li, Beiming Tang, Patrick C. Campbell, Youhua Tang, Barry Baker, Zachary Moon, Daniel Tong, Jianping Huang, Kai Wang, Ivanka Stajner, and Raffaele Montuoro
Geosci. Model Dev., 18, 1635–1660, https://doi.org/10.5194/gmd-18-1635-2025, https://doi.org/10.5194/gmd-18-1635-2025, 2025
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The study describes the updates of NOAA's current UFS-AQMv7 air quality forecast model by incorporating the latest scientific and structural changes in CMAQv5.4. An evaluation during the summer of 2023 shows that the updated model overall improves the simulation of MDA8 O3 by reducing the bias by 8%–12% in the contiguous US. PM2.5 predictions have mixed results due to wildfire, highlighting the need for future refinements.
Yanwei Zhu, Aitor Atencia, Markus Dabernig, and Yong Wang
Geosci. Model Dev., 18, 1545–1559, https://doi.org/10.5194/gmd-18-1545-2025, https://doi.org/10.5194/gmd-18-1545-2025, 2025
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Most works have delved into convective weather nowcasting, and only a few works have discussed the nowcasting uncertainty for variables at the surface level. Hence, we proposed a method to estimate uncertainty. Generating appropriate noises associated with the characteristic of the error in analysis can simulate the uncertainty of nowcasting. This method can contribute to the estimation of near–surface analysis uncertainty in both nowcasting applications and ensemble nowcasting development.
Cited articles
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Short summary
We developed a parameterization method for IEPOX-SOA based on the detailed chemical mechanism. Our parameterizations were tested using a box model and 3-D chemical transport model, which accurately captured the spatiotemporal distribution and response to changes in emissions compared to the explicit full chemistry, while being more computationally efficient. The method developed in this study can be applied to global climate models for long-term studies with a lower computational cost.
We developed a parameterization method for IEPOX-SOA based on the detailed chemical mechanism....
