Articles | Volume 16, issue 2
https://doi.org/10.5194/acp-16-1161-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-1161-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
02 Feb 2016
Research article |
| 02 Feb 2016
Iodine's impact on tropospheric oxidants: a global model study in GEOS-Chem
Wolfson Atmospheric Chemistry Laboratories (WACL), Department of Chemistry, University of York, York, YO10 5DD, UK
M. J. Evans
Wolfson Atmospheric Chemistry Laboratories (WACL), Department of Chemistry, University of York, York, YO10 5DD, UK
National Centre for Atmospheric Science (NCAS), University of York, York, YO10 5DD, UK
L. J. Carpenter
Wolfson Atmospheric Chemistry Laboratories (WACL), Department of Chemistry, University of York, York, YO10 5DD, UK
S. J. Andrews
Wolfson Atmospheric Chemistry Laboratories (WACL), Department of Chemistry, University of York, York, YO10 5DD, UK
R. T. Lidster
Wolfson Atmospheric Chemistry Laboratories (WACL), Department of Chemistry, University of York, York, YO10 5DD, UK
Department of Chemistry and Biochemistry, University of Colorado, Boulder, CO 80309-0215, USA
T. K. Koenig
Department of Chemistry and Biochemistry, University of Colorado, Boulder, CO 80309-0215, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309-021, USA
R. Sinreich
Department of Chemistry and Biochemistry, University of Colorado, Boulder, CO 80309-0215, USA
I. Ortega
Department of Chemistry and Biochemistry, University of Colorado, Boulder, CO 80309-0215, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309-021, USA
R. Volkamer
Department of Chemistry and Biochemistry, University of Colorado, Boulder, CO 80309-0215, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309-021, USA
A. Saiz-Lopez
Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, CSIC, Madrid, 28006, Spain
C. Prados-Roman
Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, CSIC, Madrid, 28006, Spain
A. S. Mahajan
Indian Institute of Tropical Meteorology, Maharashtra, 411008, India
C. Ordóñez
Met Office, FitzRoy Road, Exeter, EX1 3PB, UK
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Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
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Tomás Sherwen, Mat J. Evans, Lucy J. Carpenter, Johan A. Schmidt, and Loretta J. Mickley
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Atmospheric volatile organic compounds affect both air quality and climate. Satellite measurements can help us to assess and predict their global impacts. We present new long-term (2012–2023) measurements of four key VOCs: methanol, ethene, ethyne, and hydrogen cyanide (HCN) from the Cross-track Infrared Sounder. The measurements reflect emissions from major forests, wildfires, and industry, and provide new information to advance understanding of these sources and their changes over time.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Tomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
EGUsphere, https://doi.org/10.5194/egusphere-2024-1399, https://doi.org/10.5194/egusphere-2024-1399, 2024
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Using single-particle mass spectrometry, we show that trace concentrations of bromine and iodine are ubiquitous in remote tropospheric aerosol, and suggest that aerosols are an important part of the global reactive iodine budget. Comparisons to a global climate model with detailed iodine chemistry are favorable in the background atmosphere; however, the model cannot replicate our measurements near the ocean surface, in biomass burning plumes, and in the stratosphere.
Katrine A. Gorham, Sam Abernethy, Tyler R. Jones, Peter Hess, Natalie M. Mahowald, Daphne Meidan, Matthew S. Johnson, Maarten M. J. W. van Herpen, Yangyang Xu, Alfonso Saiz-Lopez, Thomas Röckmann, Chloe A. Brashear, Erika Reinhardt, and David Mann
Atmos. Chem. Phys., 24, 5659–5670, https://doi.org/10.5194/acp-24-5659-2024, https://doi.org/10.5194/acp-24-5659-2024, 2024
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Rapid reduction in atmospheric methane is needed to slow the rate of global warming. Reducing anthropogenic methane emissions is a top priority. However, atmospheric methane is also impacted by rising natural emissions and changing sinks. Studies of possible atmospheric methane removal approaches, such as iron salt aerosols to increase the chlorine radical sink, benefit from a roadmapped approach to understand if there may be viable and socially acceptable ways to decrease future risk.
Heesung Chong, Gonzalo González Abad, Caroline R. Nowlan, Christopher Chan Miller, Alfonso Saiz-Lopez, Rafael P. Fernandez, Hyeong-Ahn Kwon, Zolal Ayazpour, Huiqun Wang, Amir H. Souri, Xiong Liu, Kelly Chance, Ewan O'Sullivan, Jhoon Kim, Ja-Ho Koo, William R. Simpson, François Hendrick, Richard Querel, Glen Jaross, Colin Seftor, and Raid M. Suleiman
Atmos. Meas. Tech., 17, 2873–2916, https://doi.org/10.5194/amt-17-2873-2024, https://doi.org/10.5194/amt-17-2873-2024, 2024
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We present a new bromine monoxide (BrO) product derived using radiances measured from OMPS-NM on board the Suomi-NPP satellite. This product provides nearly a decade of global stratospheric and tropospheric column retrievals, a feature that is currently rare in publicly accessible datasets. Both stratospheric and tropospheric columns from OMPS-NM demonstrate robust performance, exhibiting good agreement with ground-based observations collected at three stations (Lauder, Utqiagvik, and Harestua).
Da Yang, Margarita Reza, Roy Mauldin, Rainer Volkamer, and Suresh Dhaniyala
Atmos. Meas. Tech., 17, 1463–1474, https://doi.org/10.5194/amt-17-1463-2024, https://doi.org/10.5194/amt-17-1463-2024, 2024
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This paper evaluates the performance of an aircraft gas inlet. Here, we use computational fluid dynamics (CFD) and experiments to demonstrate the role of turbulence in determining sampling performance of a gas inlet and identify ideal conditions for inlet operation to minimize gas loss. Experiments conducted in a high-speed wind tunnel under near-aircraft speeds validated numerical results. We believe that the results obtained from this work will greatly inform future gas inlet studies.
Sankirna D. Joge, Anoop Sharad Mahajan, Shrivardhan Hulswar, Christa Marandino, Martí Galí, Thomas Bell, and Rafel Simo
EGUsphere, https://doi.org/10.5194/egusphere-2024-173, https://doi.org/10.5194/egusphere-2024-173, 2024
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Dimethyl sulfide (DMS) is the largest natural source of sulfur into the atmosphere and leads to the formation of CCN. DMS emissions, and hence the quantification of its impacts, have large uncertainties, but a detailed study on the range of emissions and drivers of their uncertainty is missing to date. The emissions are usually calculated from the seawater DMS concentrations and a flux parameterization. Here we quantify the differences in DMS seawater products, which can affect the DMS fluxes.
Sankirna D. Joge, Anoop Sharad Mahajan, Shrivardhan Hulswar, Christa Marandino, Marti Gali, Thomas Bell, Mingxi Yang, and Rafel Simo
EGUsphere, https://doi.org/10.5194/egusphere-2024-175, https://doi.org/10.5194/egusphere-2024-175, 2024
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Dimethyl sulfide (DMS) is the largest natural source of sulfur into the atmosphere and leads to the formation of CCN. DMS emissions, and hence the quantification of its impacts, have large uncertainties, but a detailed study on the range of emissions and drivers of their uncertainty is missing to date. The emissions are usually calculated from the seawater DMS concentrations and a flux parameterization. Here we quantify the differences in the effect of flux parameterisations used in models.
Jean-François Müller, Trissevgeni Stavrakou, Glenn-Michael Oomen, Beata Opacka, Isabelle De Smedt, Alex Guenther, Corinne Vigouroux, Bavo Langerock, Carlos Augusto Bauer Aquino, Michel Grutter, James Hannigan, Frank Hase, Rigel Kivi, Erik Lutsch, Emmanuel Mahieu, Maria Makarova, Jean-Marc Metzger, Isamu Morino, Isao Murata, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Amelie Röhling, Wolfgang Stremme, Kimberly Strong, Ralf Sussmann, Yao Té, and Alan Fried
Atmos. Chem. Phys., 24, 2207–2237, https://doi.org/10.5194/acp-24-2207-2024, https://doi.org/10.5194/acp-24-2207-2024, 2024
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Formaldehyde observations from satellites can be used to constrain the emissions of volatile organic compounds, but those observations have biases. Using an atmospheric model, aircraft and ground-based remote sensing data, we quantify these biases, propose a correction to the data, and assess the consequence of this correction for the evaluation of emissions.
Kelvin H. Bates, Mathew J. Evans, Barron H. Henderson, and Daniel J. Jacob
Geosci. Model Dev., 17, 1511–1524, https://doi.org/10.5194/gmd-17-1511-2024, https://doi.org/10.5194/gmd-17-1511-2024, 2024
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Accurate representation of rates and products of chemical reactions in atmospheric models is crucial for simulating concentrations of pollutants and climate forcers. We update the widely used GEOS-Chem atmospheric chemistry model with reaction parameters from recent compilations of experimental data and demonstrate the implications for key atmospheric chemical species. The updates decrease tropospheric CO mixing ratios and increase stratospheric nitrogen oxide mixing ratios, among other changes.
Xi Cheng, Yong Jie Li, Yan Zheng, Keren Liao, Theodore K. Koenig, Yanli Ge, Tong Zhu, Chunxiang Ye, Xinghua Qiu, and Qi Chen
Atmos. Chem. Phys., 24, 2099–2112, https://doi.org/10.5194/acp-24-2099-2024, https://doi.org/10.5194/acp-24-2099-2024, 2024
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In this study we conducted laboratory measurements to investigate the formation of gas-phase oxygenated organic molecules (OOMs) from six aromatic volatile organic compounds (VOCs). We provide a thorough analysis on the effects of precursor structure (substituents and ring numbers) on product distribution and highlight from a laboratory perspective that heavy (e.g., double-ring) aromatic VOCs are important in initial particle growth during secondary organic aerosol formation.
Robin Björklund, Corinne Vigouroux, Peter Effertz, Omaira Garcia, Alex Geddes, James Hannigan, Koji Miyagawa, Michael Kotkamp, Bavo Langerock, Gerald Nedoluha, Ivan Ortega, Irina Petropavlovskikh, Deniz Poyraz, Richard Querel, John Robinson, Hisako Shiona, Dan Smale, Penny Smale, Roeland Van Malderen, and Martine De Mazière
EGUsphere, https://doi.org/10.5194/egusphere-2023-2668, https://doi.org/10.5194/egusphere-2023-2668, 2023
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An intercomparison study is performed at Lauder between multiple ground-based measurements. We want to know why different trends have been observed in the stratosphere and. Also, the quality and relevance of tropospheric data sets need to be evaluated for trend studies. We analyze potential biases and drifts between Fourier transform infrared (FTIR) spectrometer, Dobson Umkehr, ozonesonde, lidar, microwave radiometer, Dobson total column ozone and Bentham ultraviolet double monochromator (UV2).
Theodore K. Koenig, Francois Hendrick, Douglas Kinnison, Christopher F. Lee, Michel Van Roozendael, and Rainer Volkamer
EGUsphere, https://doi.org/10.5194/egusphere-2023-2150, https://doi.org/10.5194/egusphere-2023-2150, 2023
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Atmospheric bromine destroys ozone, impacts oxidation capacity, and is the main oxidant of mercury into its toxic form. We constrain bromine by remote sensing of BrO from a mountaintop. Previous measurements retrieved 2–3 pieces of information vertically, we apply new methods to get 5.5 vertically and 2 more in time. We compare with aircraft measurements to validate the methods and look at variation in BrO over the Pacific. More information will help chemical models and satellite measurements.
Randall Chiu, Florian Obersteiner, Alessandro Franchin, Teresa Campos, Adriana Bailey, Christopher Webster, Andreas Zahn, and Rainer Volkamer
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2023-198, https://doi.org/10.5194/amt-2023-198, 2023
Revised manuscript accepted for AMT
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The ozone sink into oceans and marine clouds is understudied and highly uncertain. Calculations suggest O3 destruction at aqueous surfaces (ocean, droplets) may be strongly accelerated, but field evidence is missing. Here we compare three fast airborne O3 instruments to measure Eddy Covariance fluxes of O3 over the remote ocean, in clear and cloudy air. We find O3 fluxes below clouds are consistently directed into clouds, while O3 fluxes into oceans are much smaller, and spatially variable.
Adedayo R. Adedeji, Stephen J. Andrews, Matthew J. Rowlinson, Mathew J. Evans, Alastair C. Lewis, Shigeru Hashimoto, Hitoshi Mukai, Hiroshi Tanimoto, Yasunori Tohjima, and Takuya Saito
Atmos. Chem. Phys., 23, 9229–9244, https://doi.org/10.5194/acp-23-9229-2023, https://doi.org/10.5194/acp-23-9229-2023, 2023
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We use the GEOS-Chem model to interpret observations of CO, C2H6, C3H8, NOx, NOy and O3 made from Hateruma Island in 2018. The model captures many synoptic-scale events and the seasonality of most pollutants at the site but underestimates C2H6 and C3H8 during the winter. These underestimates are unlikely to be reconciled by increases in biomass burning emissions but could be reconciled by increasing the Asian anthropogenic source of C2H6 and C3H8 by factors of around 2 and 3, respectively.
Cyril Caram, Sophie Szopa, Anne Cozic, Slimane Bekki, Carlos A. Cuevas, and Alfonso Saiz-Lopez
Geosci. Model Dev., 16, 4041–4062, https://doi.org/10.5194/gmd-16-4041-2023, https://doi.org/10.5194/gmd-16-4041-2023, 2023
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We studied the role of halogenated compounds (containing chlorine, bromine and iodine), emitted by natural processes (mainly above the oceans), in the chemistry of the lower layers of the atmosphere. We introduced this relatively new chemistry in a three-dimensional climate–chemistry model and looked at how this chemistry will disrupt the ozone. We showed that the concentration of ozone decreases by 22 % worldwide and that of the atmospheric detergent, OH, by 8 %.
Tobias Borsdorff, Teresa Campos, Natalie Kille, Kyle J. Zarzana, Rainer Volkamer, and Jochen Landgraf
Atmos. Meas. Tech., 16, 3027–3038, https://doi.org/10.5194/amt-16-3027-2023, https://doi.org/10.5194/amt-16-3027-2023, 2023
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ECMWF plans to assimilate TROPOMI CO with their CAMS-IFS model. This will constrain the total column and the vertical CO distribution of the model. To show this, we combine individual TROPOMI CO column retrievals with different vertical sensitivities and obtain a vertical CO concentration profile. We test the approach on three CO pollution events in comparison with CAMS-IFS simulations that do not assimilate TROPOMI CO data and in situ airborne measurements of the BB-FLUX campaign.
George Manville, Thomas G. Bell, Jane P. Mulcahy, Rafel Simó, Martí Galí, Anoop S. Mahajan, Shrivardhan Hulswar, and Paul R. Halloran
Biogeosciences, 20, 1813–1828, https://doi.org/10.5194/bg-20-1813-2023, https://doi.org/10.5194/bg-20-1813-2023, 2023
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We present the first global investigation of controls on seawater dimethylsulfide (DMS) spatial variability over scales of up to 100 km. Sea surface height anomalies, density, and chlorophyll a help explain almost 80 % of DMS variability. The results suggest that physical and biogeochemical processes play an equally important role in controlling DMS variability. These data provide independent confirmation that existing parameterisations of seawater DMS concentration use appropriate variables.
Manon Rocco, Erin Dunne, Alexia Saint-Macary, Maija Peltola, Theresa Barthelmeß, Neill Barr, Karl Safi, Andrew Marriner, Stacy Deppeler, James Harnwell, Anja Engel, Aurélie Colomb, Alfonso Saiz-Lopez, Mike Harvey, Cliff S. Law, and Karine Sellegri
EGUsphere, https://doi.org/10.5194/egusphere-2023-516, https://doi.org/10.5194/egusphere-2023-516, 2023
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During the Sea2cloud campaign in the Southern Pacific Ocean, we measured air-sea emissions from phytopankton of two key atmospheric compounds: DMS and MeSH. These compounds are well-known to play a great role in atmospheric chemistry and climate. We see in this paper that these compounds are most emited by the nanophytoplankton population. We provide here parameters for climate models to predict future trends of the emissions of these compounds and their roles and impacts on the global warming.
Zixuan Jia, Carlos Ordóñez, Ruth M. Doherty, Oliver Wild, Steven T. Turnock, and Fiona M. O'Connor
Atmos. Chem. Phys., 23, 2829–2842, https://doi.org/10.5194/acp-23-2829-2023, https://doi.org/10.5194/acp-23-2829-2023, 2023
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This study investigates the influence of the winter large-scale circulation on daily concentrations of PM2.5 and their sensitivity to emissions. The new proposed circulation index can effectively distinguish different levels of air pollution and explain changes in PM2.5 sensitivity to emissions from local and surrounding regions. We then project future changes in PM2.5 concentrations using this index and find an increase in PM2.5 concentrations over the region due to climate change.
François Burgay, Rafael Pedro Fernández, Delia Segato, Clara Turetta, Christopher S. Blaszczak-Boxe, Rachael H. Rhodes, Claudio Scarchilli, Virginia Ciardini, Carlo Barbante, Alfonso Saiz-Lopez, and Andrea Spolaor
The Cryosphere, 17, 391–405, https://doi.org/10.5194/tc-17-391-2023, https://doi.org/10.5194/tc-17-391-2023, 2023
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The paper presents the first ice-core record of bromine (Br) in the Antarctic plateau. By the observation of the ice core and the application of atmospheric chemical models, we investigate the behaviour of bromine after its deposition into the snowpack, with interest in the effect of UV radiation change connected to the formation of the ozone hole, the role of volcanic deposition, and the possible use of Br to reconstruct past sea ice changes from ice core collect in the inner Antarctic plateau.
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.
Simone T. Andersen, Beth S. Nelson, Katie A. Read, Shalini Punjabi, Luis Neves, Matthew J. Rowlinson, James Hopkins, Tomás Sherwen, Lisa K. Whalley, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 22, 15747–15765, https://doi.org/10.5194/acp-22-15747-2022, https://doi.org/10.5194/acp-22-15747-2022, 2022
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The cycling of NO and NO2 is important to understand to be able to predict O3 concentrations in the atmosphere. We have used long-term measurements from the Cape Verde Atmospheric Observatory together with model outputs to investigate the cycling of nitrogen oxide (NO) and nitrogen dioxide (NO2) in very clean marine air. This study shows that we understand the processes occurring in very clean air, but with small amounts of pollution in the air, known chemistry cannot explain what is observed.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
Atmos. Chem. Phys., 22, 14467–14488, https://doi.org/10.5194/acp-22-14467-2022, https://doi.org/10.5194/acp-22-14467-2022, 2022
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Radical bromine molecules are seen at higher concentrations during the Arctic spring. We use the global model GEOS-Chem to test whether snowpack and wind-blown snow sources can explain high bromine concentrations. We run this model for the entire year of 2015 and compare results to observations of bromine from floating platforms on the Arctic Ocean and at Utqiaġvik. We find that the model performs best when both sources are enabled but may overestimate bromine production in summer and fall.
Shrivardhan Hulswar, Rafel Simó, Martí Galí, Thomas G. Bell, Arancha Lana, Swaleha Inamdar, Paul R. Halloran, George Manville, and Anoop Sharad Mahajan
Earth Syst. Sci. Data, 14, 2963–2987, https://doi.org/10.5194/essd-14-2963-2022, https://doi.org/10.5194/essd-14-2963-2022, 2022
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The third climatological estimation of sea surface dimethyl sulfide (DMS) concentrations based on in situ measurements was created (DMS-Rev3). The update includes a much larger input dataset and includes improvements in the data unification, filtering, and smoothing algorithm. The DMS-Rev3 climatology provides more realistic monthly estimates of DMS, and shows significant regional differences compared to past climatologies.
Gaia Pinardi, Michel Van Roozendael, François Hendrick, Andreas Richter, Pieter Valks, Ramina Alwarda, Kristof Bognar, Udo Frieß, José Granville, Myojeong Gu, Paul Johnston, Cristina Prados-Roman, Richard Querel, Kimberly Strong, Thomas Wagner, Folkard Wittrock, and Margarita Yela Gonzalez
Atmos. Meas. Tech., 15, 3439–3463, https://doi.org/10.5194/amt-15-3439-2022, https://doi.org/10.5194/amt-15-3439-2022, 2022
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We report on the GOME-2A and GOME-2B OClO dataset (2007 to 2016, from the EUMETSAT's AC SAF) validation using data from nine NDACC zenith-scattered-light DOAS (ZSL-DOAS) instruments distributed in both the Arctic and Antarctic. Specific sensitivity tests are performed on the ground-based data to estimate the impact of the different OClO DOAS analysis settings and their typical errors. Good agreement is found for both the inter-annual variability and the overall OClO seasonal behavior.
Susann Tegtmeier, Christa Marandino, Yue Jia, Birgit Quack, and Anoop S. Mahajan
Atmos. Chem. Phys., 22, 6625–6676, https://doi.org/10.5194/acp-22-6625-2022, https://doi.org/10.5194/acp-22-6625-2022, 2022
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In the atmosphere over the Indian Ocean, intense anthropogenic pollution from Southeast Asia mixes with pristine oceanic air. During the winter monsoon, high pollution levels are regularly observed over the entire northern Indian Ocean, while during the summer monsoon, clean air dominates. Here, we review current progress in detecting and understanding atmospheric gas-phase composition over the Indian Ocean and its impacts on the upper atmosphere, oceanic biogeochemistry, and marine ecosystems.
Zixuan Jia, Ruth M. Doherty, Carlos Ordóñez, Chaofan Li, Oliver Wild, Shipra Jain, and Xiao Tang
Atmos. Chem. Phys., 22, 6471–6487, https://doi.org/10.5194/acp-22-6471-2022, https://doi.org/10.5194/acp-22-6471-2022, 2022
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This study investigates the modulation of daily PM2.5 over three major populated regions in China by regional meteorology and large-scale circulation during winter. These results demonstrate the benefits of considering the large-scale circulation for air quality studies. The novel circulation indices proposed here can explain a considerable fraction of the day-to-day variability of PM2.5 and can be combined with regional meteorology to improve our capability to predict the variability of PM2.5.
Hisahiro Takashima, Yugo Kanaya, Saki Kato, Martina M. Friedrich, Michel Van Roozendael, Fumikazu Taketani, Takuma Miyakawa, Yuichi Komazaki, Carlos A. Cuevas, Alfonso Saiz-Lopez, and Takashi Sekiya
Atmos. Chem. Phys., 22, 4005–4018, https://doi.org/10.5194/acp-22-4005-2022, https://doi.org/10.5194/acp-22-4005-2022, 2022
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We have undertaken atmospheric iodine monoxide (IO) observations in the global marine boundary layer with a wide latitudinal coverage and sea surface temperature (SST) range. We conclude that atmospheric iodine is abundant over the Western Pacific warm pool, appearing as an iodine fountain, where ozone (O3) minima occur. Our study also found negative correlations between IO and O3 concentrations over IO maxima, which requires reconsideration of the initiation process of halogen activation.
Zhiyuan Gao, Nicolas-Xavier Geilfus, Alfonso Saiz-Lopez, and Feiyue Wang
Atmos. Chem. Phys., 22, 1811–1824, https://doi.org/10.5194/acp-22-1811-2022, https://doi.org/10.5194/acp-22-1811-2022, 2022
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Every spring in the Arctic, a series of photochemical events occur over the ice-covered ocean, known as bromine explosion events, ozone depletion events, and mercury depletion events. Here we report the re-creation of these events at an outdoor sea ice facility in Winnipeg, Canada, far away from the Arctic. The success provides a new platform with new opportunities to uncover fundamental mechanisms of these Arctic springtime phenomena and how they may change in a changing climate.
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.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Debora Griffin, Chris A. McLinden, Enrico Dammers, Cristen Adams, Chelsea E. Stockwell, Carsten Warneke, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Kyle J. Zarzana, Jake P. Rowe, Rainer Volkamer, Christoph Knote, Natalie Kille, Theodore K. Koenig, Christopher F. Lee, Drew Rollins, Pamela S. Rickly, Jack Chen, Lukas Fehr, Adam Bourassa, Doug Degenstein, Katherine Hayden, Cristian Mihele, Sumi N. Wren, John Liggio, Ayodeji Akingunola, and Paul Makar
Atmos. Meas. Tech., 14, 7929–7957, https://doi.org/10.5194/amt-14-7929-2021, https://doi.org/10.5194/amt-14-7929-2021, 2021
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Satellite-derived NOx emissions from biomass burning are estimated with TROPOMI observations. Two common emission estimation methods are applied, and sensitivity tests with model output were performed to determine the accuracy of these methods. The effect of smoke aerosols on TROPOMI NO2 columns is estimated and compared to aircraft observations from four different aircraft campaigns measuring biomass burning plumes in 2018 and 2019 in North America.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Sharmine Akter Simu, Yuzo Miyazaki, Eri Tachibana, Henning Finkenzeller, Jérôme Brioude, Aurélie Colomb, Olivier Magand, Bert Verreyken, Stephanie Evan, Rainer Volkamer, and Trissevgeni Stavrakou
Atmos. Chem. Phys., 21, 17017–17029, https://doi.org/10.5194/acp-21-17017-2021, https://doi.org/10.5194/acp-21-17017-2021, 2021
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The tropical Indian Ocean (IO) is expected to be a significant source of water-soluble organic carbon (WSOC), which is relevant to cloud formation. Our study showed that marine secondary organic formation dominantly contributed to the aerosol WSOC mass at the high-altitude observatory in the southwest IO in the wet season in both marine boundary layer and free troposphere (FT). This suggests that the effect of marine secondary sources is important up to FT, a process missing in climate models.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Tomás Sherwen, Rainer Volkamer, Theodore K. Koenig, Tanguy Giroud, and Thomas Peter
Geosci. Model Dev., 14, 6623–6645, https://doi.org/10.5194/gmd-14-6623-2021, https://doi.org/10.5194/gmd-14-6623-2021, 2021
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Here, we present the iodine chemistry module in the SOCOL-AERv2 model. The obtained iodine distribution demonstrated a good agreement when validated against other simulations and available observations. We also estimated the iodine influence on ozone in the case of present-day iodine emissions, the sensitivity of ozone to doubled iodine emissions, and when considering only organic or inorganic iodine sources. The new model can be used as a tool for further studies of iodine effects on ozone.
Mahesh Kumar Sha, Bavo Langerock, Jean-François L. Blavier, Thomas Blumenstock, Tobias Borsdorff, Matthias Buschmann, Angelika Dehn, Martine De Mazière, Nicholas M. Deutscher, Dietrich G. Feist, Omaira E. García, David W. T. Griffith, Michel Grutter, James W. Hannigan, Frank Hase, Pauli Heikkinen, Christian Hermans, Laura T. Iraci, Pascal Jeseck, Nicholas Jones, Rigel Kivi, Nicolas Kumps, Jochen Landgraf, Alba Lorente, Emmanuel Mahieu, Maria V. Makarova, Johan Mellqvist, Jean-Marc Metzger, Isamu Morino, Tomoo Nagahama, Justus Notholt, Hirofumi Ohyama, Ivan Ortega, Mathias Palm, Christof Petri, David F. Pollard, Markus Rettinger, John Robinson, Sébastien Roche, Coleen M. Roehl, Amelie N. Röhling, Constantina Rousogenous, Matthias Schneider, Kei Shiomi, Dan Smale, Wolfgang Stremme, Kimberly Strong, Ralf Sussmann, Yao Té, Osamu Uchino, Voltaire A. Velazco, Corinne Vigouroux, Mihalis Vrekoussis, Pucai Wang, Thorsten Warneke, Tyler Wizenberg, Debra Wunch, Shoma Yamanouchi, Yang Yang, and Minqiang Zhou
Atmos. Meas. Tech., 14, 6249–6304, https://doi.org/10.5194/amt-14-6249-2021, https://doi.org/10.5194/amt-14-6249-2021, 2021
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This paper presents, for the first time, Sentinel-5 Precursor methane and carbon monoxide validation results covering a period from November 2017 to September 2020. For this study, we used global TCCON and NDACC-IRWG network data covering a wide range of atmospheric and surface conditions across different terrains. We also show the influence of a priori alignment, smoothing uncertainties and the sensitivity of the validation results towards the application of advanced co-location criteria.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Anoop S. Mahajan, Mriganka S. Biswas, Steffen Beirle, Thomas Wagner, Anja Schönhardt, Nuria Benavent, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 21, 11829–11842, https://doi.org/10.5194/acp-21-11829-2021, https://doi.org/10.5194/acp-21-11829-2021, 2021
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Iodine plays a vital role in oxidation chemistry over Antarctica, with past observations showing highly elevated levels of iodine oxide (IO) leading to severe depletion of boundary layer ozone. We present IO observations over three summers (2015–2017) at the Indian Antarctic bases of Bharati and Maitri. IO was observed during all campaigns with mixing ratios below 2 pptv, which is lower than the peak levels observed in West Antarctica, showing the differences in regional chemistry and emissions.
Jacob W. Maddison, Marta Abalos, David Barriopedro, Ricardo García-Herrera, Jose M. Garrido-Perez, and Carlos Ordóñez
Weather Clim. Dynam., 2, 675–694, https://doi.org/10.5194/wcd-2-675-2021, https://doi.org/10.5194/wcd-2-675-2021, 2021
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Air stagnation occurs when an air mass becomes settled over a region and precipitation is suppressed. Pollutant levels can rise during stagnation. The synoptic- to large-scale influence on European air stagnation and pollution is explored here. We show that around 60 % of the monthly variability in air stagnation and pollutants can be explained by dynamical indices describing the atmospheric circulation. The weather systems most related to stagnation are different for regions across Europe.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
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Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Anoop S. Mahajan, Qinyi Li, Swaleha Inamdar, Kirpa Ram, Alba Badia, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 21, 8437–8454, https://doi.org/10.5194/acp-21-8437-2021, https://doi.org/10.5194/acp-21-8437-2021, 2021
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Using a regional model, we show that iodine-catalysed reactions cause large regional changes in the chemical composition in the northern Indian Ocean, with peak changes of up to 25 % in O3, 50 % in nitrogen oxides (NO and NO2), 15 % in hydroxyl radicals (OH), 25 % in hydroperoxyl radicals (HO2), and up to a 50 % change in the nitrate radical (NO3). These results show the importance of including iodine chemistry in modelling the atmosphere in this region.
David Garcia-Nieto, Nuria Benavent, Rafael Borge, and Alfonso Saiz-Lopez
Atmos. Meas. Tech., 14, 2941–2955, https://doi.org/10.5194/amt-14-2941-2021, https://doi.org/10.5194/amt-14-2941-2021, 2021
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Trace gases play a key role in the chemistry of urban atmospheres. Therefore, knowledge about their spatial distribution is needed to fully characterize the air quality in urban areas. Using a new Multi-AXis Differential Optical Absorption Spectroscopy two-dimensional (MAXDOAS-2D) instrument, along with inversion algorithms, we report for the first time two-dimensional maps of NO2 concentrations in the city of Madrid, Spain.
Christoph A. Keller, Mathew J. Evans, K. Emma Knowland, Christa A. Hasenkopf, Sruti Modekurty, Robert A. Lucchesi, Tomohiro Oda, Bruno B. Franca, Felipe C. Mandarino, M. Valeria Díaz Suárez, Robert G. Ryan, Luke H. Fakes, and Steven Pawson
Atmos. Chem. Phys., 21, 3555–3592, https://doi.org/10.5194/acp-21-3555-2021, https://doi.org/10.5194/acp-21-3555-2021, 2021
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This study combines surface observations and model simulations to quantify the impact of COVID-19 restrictions on air quality across the world. The presented methodology removes the confounding impacts of meteorology on air pollution. Our results indicate that surface concentrations of nitrogen dioxide, an important air pollutant emitted during the combustion of fossil fuels, declined by up to 60 % following the implementation of COVID-19 containment measures.
Thomas Blumenstock, Frank Hase, Axel Keens, Denis Czurlok, Orfeo Colebatch, Omaira Garcia, David W. T. Griffith, Michel Grutter, James W. Hannigan, Pauli Heikkinen, Pascal Jeseck, Nicholas Jones, Rigel Kivi, Erik Lutsch, Maria Makarova, Hamud K. Imhasin, Johan Mellqvist, Isamu Morino, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Uwe Raffalski, Markus Rettinger, John Robinson, Matthias Schneider, Christian Servais, Dan Smale, Wolfgang Stremme, Kimberly Strong, Ralf Sussmann, Yao Té, and Voltaire A. Velazco
Atmos. Meas. Tech., 14, 1239–1252, https://doi.org/10.5194/amt-14-1239-2021, https://doi.org/10.5194/amt-14-1239-2021, 2021
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This study investigates the level of channeling (optical resonances) of each FTIR spectrometer within the Network for the Detection of Atmospheric Composition Change (NDACC). Since the air gap of the beam splitter is a significant source of channeling, we propose new beam splitters with an increased wedge of the air gap. This study shows the potential for reducing channeling in the FTIR spectrometers operated by the NDACC, thereby increasing the quality of recorded spectra across the network.
Angharad C. Stell, Luke M. Western, Tomás Sherwen, and Matthew Rigby
Atmos. Chem. Phys., 21, 1717–1736, https://doi.org/10.5194/acp-21-1717-2021, https://doi.org/10.5194/acp-21-1717-2021, 2021
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Although it is the second-most important greenhouse gas, our understanding of the atmospheric-methane budget is limited. The uncertainty highlights the need for new tools to investigate sources and sinks. Here, we use a Gaussian process emulator to efficiently approximate the response of atmospheric-methane observations to changes in the most uncertain emission or loss processes. With this new method, we rigorously quantify the sensitivity of atmospheric observations to budget uncertainties.
Mike J. Newland, Daniel J. Bryant, Rachel E. Dunmore, Thomas J. Bannan, W. Joe F. Acton, Ben Langford, James R. Hopkins, Freya A. Squires, William Dixon, William S. Drysdale, Peter D. Ivatt, Mathew J. Evans, Peter M. Edwards, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, C. Nicholas Hewitt, James D. Lee, Tianqu Cui, Jason D. Surratt, Xinming Wang, Alastair C. Lewis, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 1613–1625, https://doi.org/10.5194/acp-21-1613-2021, https://doi.org/10.5194/acp-21-1613-2021, 2021
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We report the formation of secondary pollutants in the urban megacity of Beijing that are typically associated with remote regions such as rainforests. This is caused by extremely low levels of nitric oxide (NO), typically expected to be high in urban areas, observed in the afternoon. This work has significant implications for how we understand atmospheric chemistry in the urban environment and thus for how to implement effective policies to improve urban air quality.
Tijl Verhoelst, Steven Compernolle, Gaia Pinardi, Jean-Christopher Lambert, Henk J. Eskes, Kai-Uwe Eichmann, Ann Mari Fjæraa, José Granville, Sander Niemeijer, Alexander Cede, Martin Tiefengraber, François Hendrick, Andrea Pazmiño, Alkiviadis Bais, Ariane Bazureau, K. Folkert Boersma, Kristof Bognar, Angelika Dehn, Sebastian Donner, Aleksandr Elokhov, Manuel Gebetsberger, Florence Goutail, Michel Grutter de la Mora, Aleksandr Gruzdev, Myrto Gratsea, Georg H. Hansen, Hitoshi Irie, Nis Jepsen, Yugo Kanaya, Dimitris Karagkiozidis, Rigel Kivi, Karin Kreher, Pieternel F. Levelt, Cheng Liu, Moritz Müller, Monica Navarro Comas, Ankie J. M. Piters, Jean-Pierre Pommereau, Thierry Portafaix, Cristina Prados-Roman, Olga Puentedura, Richard Querel, Julia Remmers, Andreas Richter, John Rimmer, Claudia Rivera Cárdenas, Lidia Saavedra de Miguel, Valery P. Sinyakov, Wolfgang Stremme, Kimberly Strong, Michel Van Roozendael, J. Pepijn Veefkind, Thomas Wagner, Folkard Wittrock, Margarita Yela González, and Claus Zehner
Atmos. Meas. Tech., 14, 481–510, https://doi.org/10.5194/amt-14-481-2021, https://doi.org/10.5194/amt-14-481-2021, 2021
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This paper reports on the ground-based validation of the NO2 data produced operationally by the TROPOMI instrument on board the Sentinel-5 Precursor satellite. Tropospheric, stratospheric, and total NO2 columns are compared to measurements collected from MAX-DOAS, ZSL-DOAS, and PGN/Pandora instruments respectively. The products are found to satisfy mission requirements in general, though negative mean differences are found at sites with high pollution levels. Potential causes are discussed.
Bert Verreyken, Crist Amelynck, Jérôme Brioude, Jean-François Müller, Niels Schoon, Nicolas Kumps, Aurélie Colomb, Jean-Marc Metzger, Christopher F. Lee, Theodore K. Koenig, Rainer Volkamer, and Trissevgeni Stavrakou
Atmos. Chem. Phys., 20, 14821–14845, https://doi.org/10.5194/acp-20-14821-2020, https://doi.org/10.5194/acp-20-14821-2020, 2020
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Biomass burning (BB) plumes arriving at the Maïdo observatory located in the south-west Indian Ocean during August 2018 and August 2019 are studied using trace gas measurements, Lagrangian transport models and the CAMS near-real-time atmospheric composition service. We investigate (i) secondary production of volatile organic compounds during transport, (ii) efficacy of the CAMS model to reproduce the chemical makeup of BB plumes and (iii) the impact of BB on the remote marine boundary layer.
Erik Lutsch, Kimberly Strong, Dylan B. A. Jones, Thomas Blumenstock, Stephanie Conway, Jenny A. Fisher, James W. Hannigan, Frank Hase, Yasuko Kasai, Emmanuel Mahieu, Maria Makarova, Isamu Morino, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Anatoly V. Poberovskii, Ralf Sussmann, and Thorsten Warneke
Atmos. Chem. Phys., 20, 12813–12851, https://doi.org/10.5194/acp-20-12813-2020, https://doi.org/10.5194/acp-20-12813-2020, 2020
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This paper describes the use of a network of 10 Arctic and midlatitude ground-based FTIR measurement sites to detect enhancements of the wildfire tracers carbon monoxide, hydrogen cyanide, and ethane from 2003 to 2018. A tagged CO GEOS-Chem simulation is used for source attribution and to evaluate the relative contribution of CO sources to the FTIR measurements. The use of FTIR measurements allowed for the emission ratios of hydrogen cyanide and ethane to be quantified.
Swaleha Inamdar, Liselotte Tinel, Rosie Chance, Lucy J. Carpenter, Prabhakaran Sabu, Racheal Chacko, Sarat C. Tripathy, Anvita U. Kerkar, Alok K. Sinha, Parli Venkateswaran Bhaskar, Amit Sarkar, Rajdeep Roy, Tomás Sherwen, Carlos Cuevas, Alfonso Saiz-Lopez, Kirpa Ram, and Anoop S. Mahajan
Atmos. Chem. Phys., 20, 12093–12114, https://doi.org/10.5194/acp-20-12093-2020, https://doi.org/10.5194/acp-20-12093-2020, 2020
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Iodine chemistry is generating a lot of interest because of its impacts on the oxidising capacity of the marine boundary and depletion of ozone. However, one of the challenges has been predicting the right levels of iodine in the models, which depend on parameterisations for emissions from the sea surface. This paper discusses the different parameterisations available and compares them with observations, showing that our current knowledge is still insufficient, especially on a regional scale.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Yang Wang, Arnoud Apituley, Alkiviadis Bais, Steffen Beirle, Nuria Benavent, Alexander Borovski, Ilya Bruchkouski, Ka Lok Chan, Sebastian Donner, Theano Drosoglou, Henning Finkenzeller, Martina M. Friedrich, Udo Frieß, David Garcia-Nieto, Laura Gómez-Martín, François Hendrick, Andreas Hilboll, Junli Jin, Paul Johnston, Theodore K. Koenig, Karin Kreher, Vinod Kumar, Aleksandra Kyuberis, Johannes Lampel, Cheng Liu, Haoran Liu, Jianzhong Ma, Oleg L. Polyansky, Oleg Postylyakov, Richard Querel, Alfonso Saiz-Lopez, Stefan Schmitt, Xin Tian, Jan-Lukas Tirpitz, Michel Van Roozendael, Rainer Volkamer, Zhuoru Wang, Pinhua Xie, Chengzhi Xing, Jin Xu, Margarita Yela, Chengxin Zhang, and Thomas Wagner
Atmos. Meas. Tech., 13, 5087–5116, https://doi.org/10.5194/amt-13-5087-2020, https://doi.org/10.5194/amt-13-5087-2020, 2020
Thomas R. Lewis, Juan Carlos Gómez Martín, Mark A. Blitz, Carlos A. Cuevas, John M. C. Plane, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 20, 10865–10887, https://doi.org/10.5194/acp-20-10865-2020, https://doi.org/10.5194/acp-20-10865-2020, 2020
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Iodine-bearing gasses emitted from the sea surface are chemically processed in the atmosphere, leading to iodine accumulation in aerosol and transport to continental ecosystems. Such processing involves light-induced break-up of large, particle-forming iodine oxides into smaller, ozone-depleting molecules. We combine experiments and theory to report the photolysis efficiency of iodine oxides required to assess the impact of iodine on ozone depletion and particle formation.
Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El-Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti P. Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, https://doi.org/10.5194/acp-20-9183-2020, 2020
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Highly oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide tropospheric-temperature range. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
Peter D. Ivatt and Mathew J. Evans
Atmos. Chem. Phys., 20, 8063–8082, https://doi.org/10.5194/acp-20-8063-2020, https://doi.org/10.5194/acp-20-8063-2020, 2020
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We investigate the potential of using a decision tree algorithm to identify and correct the tropospheric ozone bias in a chemical transport model. We train the algorithm on 2010–2015 ground and column observation data and test the algorithm on the 2016–2017 data using the ground data as well as independent flight data. We find the algorithm is successfully able to identify and correct the bias, improving the model performance.
Javier Alejandro Barrera, Rafael Pedro Fernandez, Fernando Iglesias-Suarez, Carlos Alberto Cuevas, Jean-Francois Lamarque, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 20, 8083–8102, https://doi.org/10.5194/acp-20-8083-2020, https://doi.org/10.5194/acp-20-8083-2020, 2020
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The inclusion of biogenic very short-lived bromocarbons (VSLBr) in the CAM-chem model improves the model–satellite agreement of the total ozone columns at mid-latitudes and drives a persistent hemispheric asymmetry in lowermost stratospheric ozone loss. The seasonal VSLBr impact on mid-latitude lowermost stratospheric ozone is influenced by the heterogeneous reactivation processes of inorganic chlorine on ice crystals, with a clear increase in ozone destruction during spring and winter.
Corinne Vigouroux, Bavo Langerock, Carlos Augusto Bauer Aquino, Thomas Blumenstock, Zhibin Cheng, Martine De Mazière, Isabelle De Smedt, Michel Grutter, James W. Hannigan, Nicholas Jones, Rigel Kivi, Diego Loyola, Erik Lutsch, Emmanuel Mahieu, Maria Makarova, Jean-Marc Metzger, Isamu Morino, Isao Murata, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Gaia Pinardi, Amelie Röhling, Dan Smale, Wolfgang Stremme, Kim Strong, Ralf Sussmann, Yao Té, Michel van Roozendael, Pucai Wang, and Holger Winkler
Atmos. Meas. Tech., 13, 3751–3767, https://doi.org/10.5194/amt-13-3751-2020, https://doi.org/10.5194/amt-13-3751-2020, 2020
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We validate the TROPOMI HCHO product with ground-based FTIR (Fourier-transform infrared) measurements from 25 stations. We find that TROPOMI overestimates HCHO under clean conditions, while it underestimates it at high HCHO levels. Both TROPOMI precision and accuracy reach the pre-launch requirements, and its precision can even be 2 times better. The observed TROPOMI seasonal variability is in agreement with the FTIR data. The TROPOMI random uncertainty and data filtering should be refined.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Jiayue Huang, Lyatt Jaeglé, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mat J. Evans, Nicolas Theys, and Sungyeon Choi
Atmos. Chem. Phys., 20, 7335–7358, https://doi.org/10.5194/acp-20-7335-2020, https://doi.org/10.5194/acp-20-7335-2020, 2020
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Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often observed in the springtime Arctic. Here, we use a chemical transport model to examine the role of sea salt aerosol from blowing snow in explaining these phenomena. We find that our simulation can account for the spatiotemporal variability of satellite observations of BrO. However, the model has difficulty in producing the magnitude of observed ozone depletion events.
Karin Kreher, Michel Van Roozendael, Francois Hendrick, Arnoud Apituley, Ermioni Dimitropoulou, Udo Frieß, Andreas Richter, Thomas Wagner, Johannes Lampel, Nader Abuhassan, Li Ang, Monica Anguas, Alkis Bais, Nuria Benavent, Tim Bösch, Kristof Bognar, Alexander Borovski, Ilya Bruchkouski, Alexander Cede, Ka Lok Chan, Sebastian Donner, Theano Drosoglou, Caroline Fayt, Henning Finkenzeller, David Garcia-Nieto, Clio Gielen, Laura Gómez-Martín, Nan Hao, Bas Henzing, Jay R. Herman, Christian Hermans, Syedul Hoque, Hitoshi Irie, Junli Jin, Paul Johnston, Junaid Khayyam Butt, Fahim Khokhar, Theodore K. Koenig, Jonas Kuhn, Vinod Kumar, Cheng Liu, Jianzhong Ma, Alexis Merlaud, Abhishek K. Mishra, Moritz Müller, Monica Navarro-Comas, Mareike Ostendorf, Andrea Pazmino, Enno Peters, Gaia Pinardi, Manuel Pinharanda, Ankie Piters, Ulrich Platt, Oleg Postylyakov, Cristina Prados-Roman, Olga Puentedura, Richard Querel, Alfonso Saiz-Lopez, Anja Schönhardt, Stefan F. Schreier, André Seyler, Vinayak Sinha, Elena Spinei, Kimberly Strong, Frederik Tack, Xin Tian, Martin Tiefengraber, Jan-Lukas Tirpitz, Jeroen van Gent, Rainer Volkamer, Mihalis Vrekoussis, Shanshan Wang, Zhuoru Wang, Mark Wenig, Folkard Wittrock, Pinhua H. Xie, Jin Xu, Margarita Yela, Chengxin Zhang, and Xiaoyi Zhao
Atmos. Meas. Tech., 13, 2169–2208, https://doi.org/10.5194/amt-13-2169-2020, https://doi.org/10.5194/amt-13-2169-2020, 2020
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In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants during an instrument intercomparison campaign (CINDI-2) at Cabauw, the Netherlands. Here we report on the outcome of this intercomparison exercise. The three major goals were to characterise the differences between the participating instruments, to define a robust methodology for performance assessment, and to contribute to the harmonisation of the measurement settings and retrieval methods.
Ryan J. Pound, Tomás Sherwen, Detlev Helmig, Lucy J. Carpenter, and Mat J. Evans
Atmos. Chem. Phys., 20, 4227–4239, https://doi.org/10.5194/acp-20-4227-2020, https://doi.org/10.5194/acp-20-4227-2020, 2020
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Ozone is an important pollutant with impacts on health and the environment. Ozone is lost to plants, land and the oceans. Loss to the ocean is slow compared to all other types of land cover and has not received as much attention. We build on previous work to more accurately model ozone loss to the ocean. We find changes in the concentration of ozone over the oceans, notably the Southern Ocean, which improves model performance.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Alexander T. Archibald, Fiona M. O'Connor, Nathan Luke Abraham, Scott Archer-Nicholls, Martyn P. Chipperfield, Mohit Dalvi, Gerd A. Folberth, Fraser Dennison, Sandip S. Dhomse, Paul T. Griffiths, Catherine Hardacre, Alan J. Hewitt, Richard S. Hill, Colin E. Johnson, James Keeble, Marcus O. Köhler, Olaf Morgenstern, Jane P. Mulcahy, Carlos Ordóñez, Richard J. Pope, Steven T. Rumbold, Maria R. Russo, Nicholas H. Savage, Alistair Sellar, Marc Stringer, Steven T. Turnock, Oliver Wild, and Guang Zeng
Geosci. Model Dev., 13, 1223–1266, https://doi.org/10.5194/gmd-13-1223-2020, https://doi.org/10.5194/gmd-13-1223-2020, 2020
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Here we present a description and evaluation of the UKCA stratosphere–troposphere chemistry scheme (StratTrop vn 1.0) implemented in the UK Earth System Model (UKESM1). UKCA StratTrop represents a substantial step forward compared to previous versions of UKCA. We show here that it is fully suited to the challenges of representing interactions in a coupled Earth system model and identify key areas and components for future development that will make it even better in the future.
Jian Zhu, Shanshan Wang, Hongli Wang, Shengao Jing, Shengrong Lou, Alfonso Saiz-Lopez, and Bin Zhou
Atmos. Chem. Phys., 20, 1217–1232, https://doi.org/10.5194/acp-20-1217-2020, https://doi.org/10.5194/acp-20-1217-2020, 2020
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To investigate the summer ozone pollution, observationally constrained modelling was carried out to study atmospheric oxidation capacity (AOC), OH reactivity, OH chain length, and HOx budget for three different ozone concentration levels in Shanghai, China. It shows that AOC, dominated by reactions involving OH radical during the daytime, has a positive correlation with ozone levels. Some key VOCs species are very important for the OH reactivity and also the ozone formation potential.
Niccolò Maffezzoli, Paul Vallelonga, Ross Edwards, Alfonso Saiz-Lopez, Clara Turetta, Helle Astrid Kjær, Carlo Barbante, Bo Vinther, and Andrea Spolaor
Clim. Past, 15, 2031–2051, https://doi.org/10.5194/cp-15-2031-2019, https://doi.org/10.5194/cp-15-2031-2019, 2019
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This study provides the first ice-core-based history of sea ice in the North Atlantic Ocean, reaching 120 000 years back in time. This record was obtained from bromine and sodium measurements in the RECAP ice core, drilled in east Greenland. We found that, during the last deglaciation, sea ice started to melt ~ 17 500 years ago. Over the 120 000 years of the last glacial cycle, sea ice extent was maximal during MIS2, while minimum sea ice extent exists for the Holocene.
Juan Pablo Corella, Niccolo Maffezzoli, Carlos Alberto Cuevas, Paul Vallelonga, Andrea Spolaor, Giulio Cozzi, Juliane Müller, Bo Vinther, Carlo Barbante, Helle Astrid Kjær, Ross Edwards, and Alfonso Saiz-Lopez
Clim. Past, 15, 2019–2030, https://doi.org/10.5194/cp-15-2019-2019, https://doi.org/10.5194/cp-15-2019-2019, 2019
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This study provides the first reconstruction of atmospheric iodine levels in the Arctic during the last 11 700 years from an ice core record in coastal Greenland. Dramatic shifts in iodine level variability coincide with abrupt climatic transitions in the North Atlantic. Since atmospheric iodine levels have significant environmental and climatic implications, this study may serve as a past analog to predict future changes in Arctic climate in response to global warming.
Sophie L. Haslett, Jonathan W. Taylor, Mathew Evans, Eleanor Morris, Bernhard Vogel, Alima Dajuma, Joel Brito, Anneke M. Batenburg, Stephan Borrmann, Johannes Schneider, Christiane Schulz, Cyrielle Denjean, Thierry Bourrianne, Peter Knippertz, Régis Dupuy, Alfons Schwarzenböck, Daniel Sauer, Cyrille Flamant, James Dorsey, Ian Crawford, and Hugh Coe
Atmos. Chem. Phys., 19, 15217–15234, https://doi.org/10.5194/acp-19-15217-2019, https://doi.org/10.5194/acp-19-15217-2019, 2019
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Three aircraft datasets from the DACCIWA campaign in summer 2016 are used here to show there is a background mass of pollution present in the lower atmosphere in southern West Africa. We suggest that this likely comes from biomass burning in central and southern Africa, which has been carried into the region over the Atlantic Ocean. This would have a negative health impact on populations living near the coast and may alter the impact of growing city emissions on cloud formation and the monsoon.
Qinyi Li, Rafael Borge, Golam Sarwar, David de la Paz, Brett Gantt, Jessica Domingo, Carlos A. Cuevas, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 19, 15321–15337, https://doi.org/10.5194/acp-19-15321-2019, https://doi.org/10.5194/acp-19-15321-2019, 2019
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The abundance and distribution of reactive halogen species and their impact on air quality in Europe are poorly understood. We adopt a state-of-the-art regional model (CMAQ) to evaluate such effects, and the results demonstrate the significant influence of halogen chemistry on the capacity of atmospheric oxidation and the formation of air pollutants in Europe. Our study highlights the necessity of including halogen chemistry in the formulation of air pollution control policy.
Elizabeth Asher, Rebecca S. Hornbrook, Britton B. Stephens, Doug Kinnison, Eric J. Morgan, Ralph F. Keeling, Elliot L. Atlas, Sue M. Schauffler, Simone Tilmes, Eric A. Kort, Martin S. Hoecker-Martínez, Matt C. Long, Jean-François Lamarque, Alfonso Saiz-Lopez, Kathryn McKain, Colm Sweeney, Alan J. Hills, and Eric C. Apel
Atmos. Chem. Phys., 19, 14071–14090, https://doi.org/10.5194/acp-19-14071-2019, https://doi.org/10.5194/acp-19-14071-2019, 2019
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Halogenated organic trace gases, which are a source of reactive halogens to the atmosphere, exert a disproportionately large influence on atmospheric chemistry and climate. This paper reports novel aircraft observations of halogenated compounds over the Southern Ocean in summer and evaluates hypothesized regional sources and emissions of these trace gases through their relationships to additional aircraft observations.
Andrea Spolaor, Elena Barbaro, David Cappelletti, Clara Turetta, Mauro Mazzola, Fabio Giardi, Mats P. Björkman, Federico Lucchetta, Federico Dallo, Katrine Aspmo Pfaffhuber, Hélène Angot, Aurelien Dommergue, Marion Maturilli, Alfonso Saiz-Lopez, Carlo Barbante, and Warren R. L. Cairns
Atmos. Chem. Phys., 19, 13325–13339, https://doi.org/10.5194/acp-19-13325-2019, https://doi.org/10.5194/acp-19-13325-2019, 2019
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The main aims of the study are to (a) detect whether mercury in the surface snow undergoes a daily cycle as determined in the atmosphere, (b) compare the mercury concentration in surface snow with the concentration in the atmosphere, (c) evaluate the effect of snow depositions, (d) detect whether iodine and bromine in the surface snow undergo a daily cycle, and (e) evaluate the role of metereological and atmospheric conditions. Different behaviours were determined during different seasons.
Pablo Corral Arroyo, Raffael Aellig, Peter A. Alpert, Rainer Volkamer, and Markus Ammann
Atmos. Chem. Phys., 19, 10817–10828, https://doi.org/10.5194/acp-19-10817-2019, https://doi.org/10.5194/acp-19-10817-2019, 2019
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Oxidation of bromide and iodide is an important process in the troposphere that leads to gas-phase halogen compounds which impact the oxidation capacity of the atmosphere. Imidazole-2-carboxaldehyde (IC), an aromatic carbonyl, is a product of the multiphase chemistry of glyoxal (an oxidation product of isoprene), a major biogenic volatile organic compound. In this study we demonstrate that IC photochemistry leads to efficient oxidation of bromide and iodide and liberation of halogen compounds.
Tomás Sherwen, Rosie J. Chance, Liselotte Tinel, Daniel Ellis, Mat J. Evans, and Lucy J. Carpenter
Earth Syst. Sci. Data, 11, 1239–1262, https://doi.org/10.5194/essd-11-1239-2019, https://doi.org/10.5194/essd-11-1239-2019, 2019
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Iodine plays an important role in the Earth system, as a nutrient to the biosphere and by changing the concentrations of climate and air-quality species. However, there are uncertainties on the magnitude of iodine’s role, and a key uncertainty is our understanding of iodide in the global sea-surface. Here we take a data-driven approach using a machine learning algorithm to convert a sparse set of sea-surface iodide observations into a spatially and temporally resolved dataset for use in models.
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Thomas Wagner, Steffen Beirle, Nuria Benavent, Tim Bösch, Ka Lok Chan, Sebastian Donner, Steffen Dörner, Caroline Fayt, Udo Frieß, David García-Nieto, Clio Gielen, David González-Bartolome, Laura Gomez, François Hendrick, Bas Henzing, Jun Li Jin, Johannes Lampel, Jianzhong Ma, Kornelia Mies, Mónica Navarro, Enno Peters, Gaia Pinardi, Olga Puentedura, Janis Puķīte, Julia Remmers, Andreas Richter, Alfonso Saiz-Lopez, Reza Shaiganfar, Holger Sihler, Michel Van Roozendael, Yang Wang, and Margarita Yela
Atmos. Meas. Tech., 12, 2745–2817, https://doi.org/10.5194/amt-12-2745-2019, https://doi.org/10.5194/amt-12-2745-2019, 2019
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In this study the consistency between MAX-DOAS measurements and radiative transfer simulations of the atmospheric O4 absorption is investigated. The study is based on measurements (2 selected days during the MADCAT campaign) as well as synthetic spectra. The uncertainties of all relevant aspects (spectral retrieval and radiative transfer simulations) are quantified. For one of the selected days, measurements and simulations do not agree within their uncertainties.
Christoph A. Keller and Mat J. Evans
Geosci. Model Dev., 12, 1209–1225, https://doi.org/10.5194/gmd-12-1209-2019, https://doi.org/10.5194/gmd-12-1209-2019, 2019
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Computer simulations of atmospheric chemistry are a central tool to study the impact of air pollutants on the environment. These models are highly complex and require a lot of computing resources. In this study we show that machine learning can be used to predict air pollution with an accuracy that is comparable to the traditional, computationally expensive method. Such a machine-learning-based model has the potential to be orders of magnitude faster.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Alba Badia, Claire E. Reeves, Alex R. Baker, Alfonso Saiz-Lopez, Rainer Volkamer, Theodore K. Koenig, Eric C. Apel, Rebecca S. Hornbrook, Lucy J. Carpenter, Stephen J. Andrews, Tomás Sherwen, and Roland von Glasow
Atmos. Chem. Phys., 19, 3161–3189, https://doi.org/10.5194/acp-19-3161-2019, https://doi.org/10.5194/acp-19-3161-2019, 2019
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The oceans have an impact on the composition and reactivity of the troposphere through the emission of gases and particles. Thus, a quantitative understanding of the marine atmosphere is crucial to examine the oxidative capacity and climate forcing. This study investigates the impact of halogens in the tropical troposphere and explores the sensitivity of this to uncertainties in the fluxes and their chemical processing. Our modelled tropospheric Ox loss due to halogens ranges from 20 % to 60 %.
Kate R. Smith, Peter M. Edwards, Peter D. Ivatt, James D. Lee, Freya Squires, Chengliang Dai, Richard E. Peltier, Mat J. Evans, Yele Sun, and Alastair C. Lewis
Atmos. Meas. Tech., 12, 1325–1336, https://doi.org/10.5194/amt-12-1325-2019, https://doi.org/10.5194/amt-12-1325-2019, 2019
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Clusters of low-cost, low-power atmospheric gas sensors were built into a sensor instrument to monitor NO2 and O3 in Beijing, alongside reference instruments, aiming to improve the reliability of sensor measurements. Clustering identical sensors and using the median sensor signal was used to minimize drift over short and medium timescales. Three different machine learning techniques were used for all the sensor data in an attempt to correct for cross-interferences, which worked to some degree.
Federica Pacifico, Claire Delon, Corinne Jambert, Pierre Durand, Eleanor Morris, Mat J. Evans, Fabienne Lohou, Solène Derrien, Venance H. E. Donnou, Arnaud V. Houeto, Irene Reinares Martínez, and Pierre-Etienne Brilouet
Atmos. Chem. Phys., 19, 2299–2325, https://doi.org/10.5194/acp-19-2299-2019, https://doi.org/10.5194/acp-19-2299-2019, 2019
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Biogenic fluxes from soil at a local and regional scale are crucial to study air pollution and climate. Here we present field measurements of soil fluxes of nitric oxide (NO) and ammonia (NH3) observed over four different land cover types, i.e. bare soil, grassland, maize field, and forest, at an inland rural site in Benin, West Africa, during the DACCIWA field campaign in
June and July 2016.
Ivan Ortega, Rebecca R. Buchholz, Emrys G. Hall, Dale F. Hurst, Allen F. Jordan, and James W. Hannigan
Atmos. Meas. Tech., 12, 873–890, https://doi.org/10.5194/amt-12-873-2019, https://doi.org/10.5194/amt-12-873-2019, 2019
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In this work we evaluate the accuracy of water vapor ground-based FTIR retrievals in the lower and upper troposphere using coincident high-quality vertically resolved balloon-borne NOAA FPH measurements. Our results suggest that highly structured water vapor vertical gradients are captured with the FTIR and found a negligible bias in the immediate layer above the instrument altitude accounting for a water vapor time variability of less than 2 %.
Cristina Carnerero, Noemí Pérez, Cristina Reche, Marina Ealo, Gloria Titos, Hong-Ku Lee, Hee-Ram Eun, Yong-Hee Park, Lubna Dada, Pauli Paasonen, Veli-Matti Kerminen, Enrique Mantilla, Miguel Escudero, Francisco J. Gómez-Moreno, Elisabeth Alonso-Blanco, Esther Coz, Alfonso Saiz-Lopez, Brice Temime-Roussel, Nicolas Marchand, David C. S. Beddows, Roy M. Harrison, Tuukka Petäjä, Markku Kulmala, Kang-Ho Ahn, Andrés Alastuey, and Xavier Querol
Atmos. Chem. Phys., 18, 16601–16618, https://doi.org/10.5194/acp-18-16601-2018, https://doi.org/10.5194/acp-18-16601-2018, 2018
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The vertical distribution of new particle formation events was studied using tethered balloons carrying miniaturized instrumentation. Results show that new particle formation and growth occurs only in the lower layer of the atmosphere, where aerosols are mixed due to convection, especially when the atmosphere is clean. A comparison of urban and suburban surface stations was also made, suggesting that such events may have a significant impact on ultrafine particle concentrations in a wide area.
Lu Hu, Christoph A. Keller, Michael S. Long, Tomás Sherwen, Benjamin Auer, Arlindo Da Silva, Jon E. Nielsen, Steven Pawson, Matthew A. Thompson, Atanas L. Trayanov, Katherine R. Travis, Stuart K. Grange, Mat J. Evans, and Daniel J. Jacob
Geosci. Model Dev., 11, 4603–4620, https://doi.org/10.5194/gmd-11-4603-2018, https://doi.org/10.5194/gmd-11-4603-2018, 2018
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We present a full-year online global simulation of tropospheric chemistry at 12.5 km resolution. To the best of our knowledge, such a resolution in a state-of-the-science global simulation of tropospheric chemistry is unprecedented. This simulation will serve as the Nature Run for observing system simulation experiments to support the future geostationary satellite constellation for tropospheric chemistry, and can also be used for various air quality applications.
Liang Feng, Paul I. Palmer, Robyn Butler, Stephen J. Andrews, Elliot L. Atlas, Lucy J. Carpenter, Valeria Donets, Neil R. P. Harris, Ross J. Salawitch, Laura L. Pan, and Sue M. Schauffler
Atmos. Chem. Phys., 18, 14787–14798, https://doi.org/10.5194/acp-18-14787-2018, https://doi.org/10.5194/acp-18-14787-2018, 2018
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We infer surface fluxes of bromoform (CHBr3) and dibromoform (CH2Br2) from CAST and CONTRAST aircraft observations over the western Pacific, using a tagged version of the GEOS-Chem global 3-D atmospheric chemistry model and a Maximum A Posteriori inverse model. Using the aircraft data, we estimate the regional fluxes about 20–40 % smaller than the prior inventories by Ordóñez et al. (2012). We find no evidence to support a robust linear relationship between CHBr3 and CH2Br2 oceanic emissions.
Qianjie Chen, Tomás Sherwen, Mathew Evans, and Becky Alexander
Atmos. Chem. Phys., 18, 13617–13637, https://doi.org/10.5194/acp-18-13617-2018, https://doi.org/10.5194/acp-18-13617-2018, 2018
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Uncertainty in the natural tropospheric sulfur cycle represents the largest source of uncertainty in radiative forcing estimates of sulfate aerosol. This study investigates the natural sulfur cycle in the marine troposphere using the GEOS-Chem model. We found that BrO is important for DMS oxidation and multiphase chemistry is important for MSA production and loss, which have implications for the yield of SO2 and MSA from DMS oxidation and the radiative effect of DMS-derived sulfate aerosol.
Robyn Butler, Paul I. Palmer, Liang Feng, Stephen J. Andrews, Elliot L. Atlas, Lucy J. Carpenter, Valeria Donets, Neil R. P. Harris, Stephen A. Montzka, Laura L. Pan, Ross J. Salawitch, and Sue M. Schauffler
Atmos. Chem. Phys., 18, 13135–13153, https://doi.org/10.5194/acp-18-13135-2018, https://doi.org/10.5194/acp-18-13135-2018, 2018
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Natural sources of short-lived bromoform and dibromomethane are important for determining the inorganic bromine budget in the stratosphere that drives ozone loss. Two new modelling techniques describe how different geographical source regions influence their atmospheric variability over the western Pacific. We find that it is driven primarily by open ocean sources, and we use atmospheric observations to help estimate their contributions to the upper tropospheric inorganic bromine budget.
Corinne Vigouroux, Carlos Augusto Bauer Aquino, Maite Bauwens, Cornelis Becker, Thomas Blumenstock, Martine De Mazière, Omaira García, Michel Grutter, César Guarin, James Hannigan, Frank Hase, Nicholas Jones, Rigel Kivi, Dmitry Koshelev, Bavo Langerock, Erik Lutsch, Maria Makarova, Jean-Marc Metzger, Jean-François Müller, Justus Notholt, Ivan Ortega, Mathias Palm, Clare Paton-Walsh, Anatoly Poberovskii, Markus Rettinger, John Robinson, Dan Smale, Trissevgeni Stavrakou, Wolfgang Stremme, Kim Strong, Ralf Sussmann, Yao Té, and Geoffrey Toon
Atmos. Meas. Tech., 11, 5049–5073, https://doi.org/10.5194/amt-11-5049-2018, https://doi.org/10.5194/amt-11-5049-2018, 2018
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A few ground-based stations have provided time series of HCHO columns until now, which was not optimal for providing good diagnostics for satellite or model validation. In this work, HCHO time series have been determined in a harmonized way at 21 stations ensuring, in addition to a better spatial and level of abundances coverage, that internal biases within the network have been minimized. This data set shows consistent good agreement with model data and is ready for future satellite validation.
Prasad Kasibhatla, Tomás Sherwen, Mathew J. Evans, Lucy J. Carpenter, Chris Reed, Becky Alexander, Qianjie Chen, Melissa P. Sulprizio, James D. Lee, Katie A. Read, William Bloss, Leigh R. Crilley, William C. Keene, Alexander A. P. Pszenny, and Alma Hodzic
Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, https://doi.org/10.5194/acp-18-11185-2018, 2018
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Recent measurements of NOx and HONO suggest that photolysis of particulate nitrate in sea-salt aerosols is important in terms of marine boundary layer oxidant chemistry. We present the first global-scale assessment of the significance of this new chemical pathway for NOx, O3, and OH in the marine boundary layer. We also present a preliminary assessment of the potential impact of photolysis of particulate nitrate associated with other aerosol types on continental boundary layer chemistry.
Cristina Prados-Roman, Laura Gómez-Martín, Olga Puentedura, Mónica Navarro-Comas, Javier Iglesias, José Ramón de Mingo, Manuel Pérez, Héctor Ochoa, María Elena Barlasina, Gerardo Carbajal, and Margarita Yela
Atmos. Chem. Phys., 18, 8549–8570, https://doi.org/10.5194/acp-18-8549-2018, https://doi.org/10.5194/acp-18-8549-2018, 2018
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Despite the efforts of the scientific community, the abundance and distribution of reactive bromine (BrOx) in the Antarctic troposphere is still poorly characterized. This work presents the first ground-based observations of tropospheric BrO from the Antarctic sites of Belgrano and Marambio. The 2015 measurements reported are also the first contemporary observations of BrO vertical profiles from two Antarctic sites and depict the geographical heterogeneity of BrOx in the Antarctic troposphere.
Xavier Querol, Andrés Alastuey, Gotzon Gangoiti, Noemí Perez, Hong K. Lee, Heeram R. Eun, Yonghee Park, Enrique Mantilla, Miguel Escudero, Gloria Titos, Lucio Alonso, Brice Temime-Roussel, Nicolas Marchand, Juan R. Moreta, M. Arantxa Revuelta, Pedro Salvador, Begoña Artíñano, Saúl García dos Santos, Mónica Anguas, Alberto Notario, Alfonso Saiz-Lopez, Roy M. Harrison, Millán Millán, and Kang-Ho Ahn
Atmos. Chem. Phys., 18, 6511–6533, https://doi.org/10.5194/acp-18-6511-2018, https://doi.org/10.5194/acp-18-6511-2018, 2018
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We show the main drivers of high O3 episodes in and around Madrid. High levels of ultrafine particles (UFPs) are evidenced, but we demonstrate that most O3 arises from the fumigation of high atmospheric layers, whereas UFPs are generated inside the PBL. O3 contributions from the fumigation of the vertical recirculation of regional air masses, hemispheric transport, and horizontally from direct urban plume transport are shown. Complexity arises from the need to quantify them to abate surface O3.
Mike J. Newland, Andrew R. Rickard, Tomás Sherwen, Mathew J. Evans, Luc Vereecken, Amalia Muñoz, Milagros Ródenas, and William J. Bloss
Atmos. Chem. Phys., 18, 6095–6120, https://doi.org/10.5194/acp-18-6095-2018, https://doi.org/10.5194/acp-18-6095-2018, 2018
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Stabilised Criegee intermediates (SCIs) are formed in the reaction of alkenes with ozone, both of which are ubiquitous throughout the troposphere. We determine the fate and global distribution of SCI from monoterpene ozonolysis. One major fate of SCI is reaction with H2O, but for a fraction of SCIs, unimolecular reactions dominate. Concentrations of SCIs are high enough regionally to play a key role in the conversion of sulfur dioxide to aerosol, affecting air quality and climate.
Richard Newton, Geraint Vaughan, Eric Hintsa, Michal T. Filus, Laura L. Pan, Shawn Honomichl, Elliot Atlas, Stephen J. Andrews, and Lucy J. Carpenter
Atmos. Chem. Phys., 18, 5157–5171, https://doi.org/10.5194/acp-18-5157-2018, https://doi.org/10.5194/acp-18-5157-2018, 2018
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We consider the ozone measurements from aircraft during the CAST/CONTRAST/ATTREX campaigns of 2014. Low concentrations of ozone were found in the layer of 10–15 km altitude, which is indicative of uplift of ozone-poor air from near the sea surface to 10–15 km altitude. Chemicals that have origins in the sea were found in greater abundance when ozone concentrations were low compared to when ozone concentrations were high. The lowest ozone concentrations were found in the Southern Hemisphere.
Daniel Stone, Tomás Sherwen, Mathew J. Evans, Stewart Vaughan, Trevor Ingham, Lisa K. Whalley, Peter M. Edwards, Katie A. Read, James D. Lee, Sarah J. Moller, Lucy J. Carpenter, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 3541–3561, https://doi.org/10.5194/acp-18-3541-2018, https://doi.org/10.5194/acp-18-3541-2018, 2018
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Halogen chemistry in the troposphere impacts oxidising capacity, but model studies assessing the nature of these impacts can vary according to the model framework used. In this work we present simulations of OH and HO2 radicals using both box and global model frameworks, and compare to observations made at the Cape Verde Atmospheric Observatory. We highlight, and rationalise, differences between the model frameworks.
Hugh C. Pumphrey, Norbert Glatthor, Peter F. Bernath, Christopher D. Boone, James W. Hannigan, Ivan Ortega, Nathaniel J. Livesey, and William G. Read
Atmos. Chem. Phys., 18, 691–703, https://doi.org/10.5194/acp-18-691-2018, https://doi.org/10.5194/acp-18-691-2018, 2018
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The Microwave Limb Sounder (MLS) is a satellite instrument that has been measuring the amount of various gases in the atmosphere since 2004. In late 2015 and 2016 it observed unusual amounts of hydrogen cyanide (HCN), a gas produced when vegetation is burned. We compare the MLS observations to similar observations from other instruments. The excess HCN is shown to come from fires in Indonesia. There are more fires than usual in 2015–16 due to a drought caused by an El Niño event.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Ben Newsome and Mat Evans
Atmos. Chem. Phys., 17, 14333–14352, https://doi.org/10.5194/acp-17-14333-2017, https://doi.org/10.5194/acp-17-14333-2017, 2017
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We explore the uncertainty in the predictions of a chemical transport model (GEOS-Chem) from uncertainty in 60 inorganic rate constants and photolysis rates. We find uncertainty in the global mean ozone burden of 10 %, in global mean OH of 16 %, methane lifetimes of 16 %, and tropospheric ozone radiative forcings of 13 %. Reductions in the uncertainty of rate constants of these simple reactions would reduce uncertainty in our understanding of atmospheric composition.
Peter M. Edwards and Mathew J. Evans
Atmos. Chem. Phys., 17, 13669–13680, https://doi.org/10.5194/acp-17-13669-2017, https://doi.org/10.5194/acp-17-13669-2017, 2017
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Understanding tropospheric ozone chemistry has been at the centre of the field of atmospheric chemistry for the last 30 years. However, our conceptual approach to diagnosing ozone production in global models has not advanced in this time. Our work presents a new and powerful approach for diagnosing tropospheric ozone production, providing a significant enhancement in our ability to understand the processes controlling ozone and how we can validate our assessment of these processes.
Yang Wang, Steffen Beirle, Francois Hendrick, Andreas Hilboll, Junli Jin, Aleksandra A. Kyuberis, Johannes Lampel, Ang Li, Yuhan Luo, Lorenzo Lodi, Jianzhong Ma, Monica Navarro, Ivan Ortega, Enno Peters, Oleg L. Polyansky, Julia Remmers, Andreas Richter, Olga Puentedura, Michel Van Roozendael, André Seyler, Jonathan Tennyson, Rainer Volkamer, Pinhua Xie, Nikolai F. Zobov, and Thomas Wagner
Atmos. Meas. Tech., 10, 3719–3742, https://doi.org/10.5194/amt-10-3719-2017, https://doi.org/10.5194/amt-10-3719-2017, 2017
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Slant column densities of nitrous acid (HONO) derived from different MAX-DOAS instruments and retrieval software are systematically compared for the first time during the Multi Axis DOAS – Comparison campaign for Aerosols and Trace gases (MAD-CAT) campaign held at MPIC in Mainz, Germany, from June to October 2013. Through the inter-comparisons and sensitivity studies we quantified the uncertainties in the DOAS fits of HONO from different sources and concluded a recommended setting.
Peter Knippertz, Andreas H. Fink, Adrien Deroubaix, Eleanor Morris, Flore Tocquer, Mat J. Evans, Cyrille Flamant, Marco Gaetani, Christophe Lavaysse, Celine Mari, John H. Marsham, Rémi Meynadier, Abalo Affo-Dogo, Titike Bahaga, Fabien Brosse, Konrad Deetz, Ridha Guebsi, Issaou Latifou, Marlon Maranan, Philip D. Rosenberg, and Andreas Schlueter
Atmos. Chem. Phys., 17, 10893–10918, https://doi.org/10.5194/acp-17-10893-2017, https://doi.org/10.5194/acp-17-10893-2017, 2017
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In June–July 2016 DACCIWA (Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa), a large, EU-funded European–African project, organised an international field campaign in densely populated southern West Africa, including measurements from ground sites, research aircraft, weather balloons and urban sites. This paper gives an overview of the atmospheric evolution during this period focusing on meteorological (precipitation, cloudiness, winds) and composition (gases, particles) aspects.
Maria A. Navarro, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Elliot Atlas, Xavier Rodriguez-Lloveras, Douglas Kinnison, Jean-Francois Lamarque, Simone Tilmes, Troy Thornberry, Andrew Rollins, James W. Elkins, Eric J. Hintsa, and Fred L. Moore
Atmos. Chem. Phys., 17, 9917–9930, https://doi.org/10.5194/acp-17-9917-2017, https://doi.org/10.5194/acp-17-9917-2017, 2017
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Inorganic bromine (Bry) plays an important role in ozone layer depletion. Based on aircraft observations of organic bromine species and chemistry simulations, we model the Bry abundances over the Pacific tropical tropopause. Our results show BrO and Br as the dominant species during daytime hours, and BrCl and BrONO2 as the nighttime dominant species over the western and eastern Pacific, respectively. The difference in the partitioning is due to changes in the abundance of O3, NO2, and Cly.
Enrico Dammers, Mark W. Shephard, Mathias Palm, Karen Cady-Pereira, Shannon Capps, Erik Lutsch, Kim Strong, James W. Hannigan, Ivan Ortega, Geoffrey C. Toon, Wolfgang Stremme, Michel Grutter, Nicholas Jones, Dan Smale, Jacob Siemons, Kevin Hrpcek, Denis Tremblay, Martijn Schaap, Justus Notholt, and Jan Willem Erisman
Atmos. Meas. Tech., 10, 2645–2667, https://doi.org/10.5194/amt-10-2645-2017, https://doi.org/10.5194/amt-10-2645-2017, 2017
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Presented here is the validation of the CrIS fast physical retrieval (CFPR) NH3 column and profile measurements using ground-based Fourier transform infrared (FTIR) observations. The overall FTIR and CrIS total columns have a positive correlation of r = 0.77 (N = 218) with very little bias (a slope of 1.02). Furthermore, we find that CrIS and FTIR profile comparison differences are mostly within the range of the estimated retrieval uncertainties, with differences in the range of ~ 20 to 40 %.
Chris Reed, Mathew J. Evans, Leigh R. Crilley, William J. Bloss, Tomás Sherwen, Katie A. Read, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 17, 4081–4092, https://doi.org/10.5194/acp-17-4081-2017, https://doi.org/10.5194/acp-17-4081-2017, 2017
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The source of ozone-depleting compounds in the remote troposphere has been thought to be long-range transport of secondary pollutants such as organic nitrates. Processing of organic nitrates to nitric acid and subsequent deposition on surfaces in the atmosphere was thought to remove these nitrates from the ozone–NOx–HOx cycle. We found through observation of NOx in the remote tropical troposphere at the Cape Verde Observatory that surface nitrates can be released back into the atmosphere.
Enno Peters, Gaia Pinardi, André Seyler, Andreas Richter, Folkard Wittrock, Tim Bösch, Michel Van Roozendael, François Hendrick, Theano Drosoglou, Alkiviadis F. Bais, Yugo Kanaya, Xiaoyi Zhao, Kimberly Strong, Johannes Lampel, Rainer Volkamer, Theodore Koenig, Ivan Ortega, Olga Puentedura, Mónica Navarro-Comas, Laura Gómez, Margarita Yela González, Ankie Piters, Julia Remmers, Yang Wang, Thomas Wagner, Shanshan Wang, Alfonso Saiz-Lopez, David García-Nieto, Carlos A. Cuevas, Nuria Benavent, Richard Querel, Paul Johnston, Oleg Postylyakov, Alexander Borovski, Alexander Elokhov, Ilya Bruchkouski, Haoran Liu, Cheng Liu, Qianqian Hong, Claudia Rivera, Michel Grutter, Wolfgang Stremme, M. Fahim Khokhar, Junaid Khayyam, and John P. Burrows
Atmos. Meas. Tech., 10, 955–978, https://doi.org/10.5194/amt-10-955-2017, https://doi.org/10.5194/amt-10-955-2017, 2017
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This work is about harmonization of differential optical absorption spectroscopy retrieval codes, which is a remote sensing technique widely used to derive atmospheric trace gas amounts. The study is based on ground-based measurements performed during the Multi-Axis DOAS Comparison campaign for Aerosols and Trace gases (MAD-CAT) in Mainz, Germany, in summer 2013. In total, 17 international groups working in the field of the DOAS technique participated in this study.
Carlos Ordóñez, David Barriopedro, Ricardo García-Herrera, Pedro M. Sousa, and Jordan L. Schnell
Atmos. Chem. Phys., 17, 3111–3131, https://doi.org/10.5194/acp-17-3111-2017, https://doi.org/10.5194/acp-17-3111-2017, 2017
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Blocks and ridges are synoptic patterns associated with an anticyclonic circulation. They also divert the atmospheric flow. This work proves that near-surface ozone in Europe is sensitive to these patterns. This quantitative assessment has been performed on a seasonal basis for a 15-year period. The results can be exploited in the future to evaluate modelled ozone responses to atmospheric circulation changes and to understand the contribution of dynamic effects to air quality projections.
Paul Vallelonga, Niccolo Maffezzoli, Andrew D. Moy, Mark A. J. Curran, Tessa R. Vance, Ross Edwards, Gwyn Hughes, Emily Barker, Gunnar Spreen, Alfonso Saiz-Lopez, J. Pablo Corella, Carlos A. Cuevas, and Andrea Spolaor
Clim. Past, 13, 171–184, https://doi.org/10.5194/cp-13-171-2017, https://doi.org/10.5194/cp-13-171-2017, 2017
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We present a study of bromine, iodine and sodium in an ice core from Law Dome, in coastal East Antarctica. We find that bromine and iodine variability at Law Dome is correlated to changes in the area of sea ice along the Law Dome coast as observed by satellite since the early 1970s. These findings are in agreement with a previous study based on MSA and confirm a long-term trend of sea ice decrease for this sector of Antarctica over the 20th century.
Rafael P. Fernandez, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 17, 1673–1688, https://doi.org/10.5194/acp-17-1673-2017, https://doi.org/10.5194/acp-17-1673-2017, 2017
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The inclusion of biogenic very-short lived bromine (VSLBr) in a chemistry-climate model produces an expansion of the ozone hole area of ~ 5 million km2, which is equivalent in magnitude to the recently estimated Antarctic ozone healing due to the reduction of anthropogenic CFCs and halons. The maximum Antarctic ozone hole depletion increases by up to 14 % when natural VSLBr are considered, but does not introduce a significant delay of the modelled ozone return date to 1980 October levels.
Natalie Kille, Sunil Baidar, Philip Handley, Ivan Ortega, Roman Sinreich, Owen R. Cooper, Frank Hase, James W. Hannigan, Gabriele Pfister, and Rainer Volkamer
Atmos. Meas. Tech., 10, 373–392, https://doi.org/10.5194/amt-10-373-2017, https://doi.org/10.5194/amt-10-373-2017, 2017
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This article describes a new instrument for measuring and quantifying emission fluxes. It introduces the instrument using the solar occultation flux method. Results are presented from the FRAPPE field campaign near Denver, Colorado, from 2014. Calculations of emissions of sources are presented from FRAPPE and compared to emission inventories. Finally, structure functions are calculated to facilitate the future comparison of high-resolution measurements with low resolution satellite measurements.
Tomás Sherwen, Mat J. Evans, Lucy J. Carpenter, Johan A. Schmidt, and Loretta J. Mickley
Atmos. Chem. Phys., 17, 1557–1569, https://doi.org/10.5194/acp-17-1557-2017, https://doi.org/10.5194/acp-17-1557-2017, 2017
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We model pre-industrial to present day changes using the GEOS-Chem global chemical transport model with halogens (Cl, Br, I). The model better captures pre-industrial O3 observations with halogens included. Halogens buffer the tropospheric forcing of O3 (RFTO3) from pre-industrial to present day, reducing RFTO3 by 0.087 Wm−2. This reduction is greater than that from halogens on stratospheric O3 (−0.05 Wm−2). This suggests that models that do not include halogens will overestimate RFTO3by ~ 25%.
Alfonso Saiz-Lopez, John M. C. Plane, Carlos A. Cuevas, Anoop S. Mahajan, Jean-François Lamarque, and Douglas E. Kinnison
Atmos. Chem. Phys., 16, 15593–15604, https://doi.org/10.5194/acp-16-15593-2016, https://doi.org/10.5194/acp-16-15593-2016, 2016
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Electronic structure calculations are used to survey possible reactions that HOI and I2 could undergo at night in the lower troposphere, and hence reconcile measurements and models. The reactions NO3 + HOI and I2 + NO3 are included in two models to explore a new nocturnal iodine radical activation mechanism, leading to a reduction of nighttime HOI and I2. This chemistry can have a large impact on NO3 levels in the MBL, and hence upon the nocturnal oxidizing capacity of the marine atmosphere.
Barbara Dix, Theodore K. Koenig, and Rainer Volkamer
Atmos. Meas. Tech., 9, 5655–5675, https://doi.org/10.5194/amt-9-5655-2016, https://doi.org/10.5194/amt-9-5655-2016, 2016
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We present a parameterization method for the conversion of measured trace gas slant column densities into volume mixing ratios along a flight track. Benefits of this method are that it is computationally fast and almost no information on local atmospheric conditions is needed. Application to simulated data and field data show that the method is accurate within 10–15 % and valid for a wide range of atmospheric conditions. Our method can easily be transferred to other trace gases.
Eleonora Aruffo, Fabio Biancofiore, Piero Di Carlo, Marcella Busilacchio, Marco Verdecchia, Barbara Tomassetti, Cesare Dari-Salisburgo, Franco Giammaria, Stephane Bauguitte, James Lee, Sarah Moller, James Hopkins, Shalini Punjabi, Stephen J. Andrews, Alistair C. Lewis, Paul I. Palmer, Edward Hyer, Michael Le Breton, and Carl Percival
Atmos. Meas. Tech., 9, 5591–5606, https://doi.org/10.5194/amt-9-5591-2016, https://doi.org/10.5194/amt-9-5591-2016, 2016
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During the BORTAS aircraft campaign, we measured NO2 and their oxidtation products (as peroxy nitrates) with a custom laser-induced fluorescence instrument. Because of the high correlation between known pyrogenic tracers (i.e., carbon monoxide) and peroxy nitrates, we provide two methods to use these species for the identification of biomass burning (BB) plumes. Using an artifical neural network, we improved the BB identification taking into account of a meteorological parameter (pressure).
Michael Höpfner, Rainer Volkamer, Udo Grabowski, Michel Grutter, Johannes Orphal, Gabriele Stiller, Thomas von Clarmann, and Gerald Wetzel
Atmos. Chem. Phys., 16, 14357–14369, https://doi.org/10.5194/acp-16-14357-2016, https://doi.org/10.5194/acp-16-14357-2016, 2016
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Ammonia (NH3) in the atmosphere is important because of its influence on aerosol and cloud formation and its increasing anthropogenic emissions. We report the first detection of NH3 in the upper troposphere by the analysis of infrared limb emission spectra measured by the MIPAS instrument on Envisat. We have found enhanced values of NH3 within the Asian summer monsoon upper troposphere, where it might contribute to the composition of the Asian tropopause aerosol layer.
Stephen J. Andrews, Lucy J. Carpenter, Eric C. Apel, Elliot Atlas, Valeria Donets, James R. Hopkins, Rebecca S. Hornbrook, Alastair C. Lewis, Richard T. Lidster, Richard Lueb, Jamie Minaeian, Maria Navarro, Shalini Punjabi, Daniel Riemer, and Sue Schauffler
Atmos. Meas. Tech., 9, 5213–5225, https://doi.org/10.5194/amt-9-5213-2016, https://doi.org/10.5194/amt-9-5213-2016, 2016
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We present a comparison of aircraft measurements of important trace gases from a co-ordinated campaign in Jan–Feb 2014 in the tropical west Pacific involving the NASA Global Hawk, NCAR GV and FAAM BAe-146 aircraft.
The paper studies the comparability of separate measurements across platforms and demonstrates that aircraft measurements are relevant for characterising the vertical uplift of important gases, such as those with ozone-depleting potential, to the upper troposphere–lower stratosphere.
Shanshan Wang, Carlos A. Cuevas, Udo Frieß, and Alfonso Saiz-Lopez
Atmos. Meas. Tech., 9, 5089–5101, https://doi.org/10.5194/amt-9-5089-2016, https://doi.org/10.5194/amt-9-5089-2016, 2016
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Multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements were performed in the urban environment of Madrid, Spain, where Sahara dust intrusion sometimes occurs. The study shows a high performances in the retrieval of aerosol optical depth, the surface extinction coefficient and an elevated layer during dust episodes, validated by AERONET in situ and modeling data. It is essential to capture the extinction properties of both local aerosol and Saharan dust.
Óscar Gálvez, M. Teresa Baeza-Romero, Mikel Sanz, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 16, 12703–12713, https://doi.org/10.5194/acp-16-12703-2016, https://doi.org/10.5194/acp-16-12703-2016, 2016
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Reactive iodine species play a key role in the oxidation capacity of the polar troposphere, although sources and mechanisms are poorly understood. In this paper, the photolysis of frozen iodate salt has been studied, confirming that under near-UV–Vis radiation iodate is photolysed. Incorporating this result into an Antarctic atmospheric model, we have shown that it could increase the atmospheric IO levels and could constitute a pathway for the release of active iodine to the polar atmosphere
Tomás Sherwen, Johan A. Schmidt, Mat J. Evans, Lucy J. Carpenter, Katja Großmann, Sebastian D. Eastham, Daniel J. Jacob, Barbara Dix, Theodore K. Koenig, Roman Sinreich, Ivan Ortega, Rainer Volkamer, Alfonso Saiz-Lopez, Cristina Prados-Roman, Anoop S. Mahajan, and Carlos Ordóñez
Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, https://doi.org/10.5194/acp-16-12239-2016, 2016
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We present a simulation of tropospheric Cl, Br, I chemistry within the GEOS-Chem CTM. We find a decrease in tropospheric ozone burden of 18.6 % and a 8.2 % decrease in global mean OH concentrations. Cl oxidation of some VOCs range from 15 to 27 % of the total loss. Bromine plays a small role in oxidising oVOCs. Surface ozone, ozone sondes, and methane lifetime are in general improved by the inclusion of halogens. We argue that simulated bromine and chlorine represent a lower limit.
Laura González Palacios, Pablo Corral Arroyo, Kifle Z. Aregahegn, Sarah S. Steimer, Thorsten Bartels-Rausch, Barbara Nozière, Christian George, Markus Ammann, and Rainer Volkamer
Atmos. Chem. Phys., 16, 11823–11836, https://doi.org/10.5194/acp-16-11823-2016, https://doi.org/10.5194/acp-16-11823-2016, 2016
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The sources of radicals at aerosol surfaces are highly uncertain. Here we investigate the HO2 radical production from the UV irradiation of imidazole-2-carboxaldehyde (IC) in bulk aqueous films containing IC and citric acid, as well as IC in ammonium sulfate aerosols. We find that IC is an efficient photosensitizer that forms HO2 radicals from H-donor chemistry. IC is a proxy species for brown carbon in atmospheric aerosols.
Ivan Ortega, Sean Coburn, Larry K. Berg, Kathy Lantz, Joseph Michalsky, Richard A. Ferrare, Johnathan W. Hair, Chris A. Hostetler, and Rainer Volkamer
Atmos. Meas. Tech., 9, 3893–3910, https://doi.org/10.5194/amt-9-3893-2016, https://doi.org/10.5194/amt-9-3893-2016, 2016
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We present an inherently calibrated retrieval to measure aerosol optical depth (AOD) and the aerosol phase function parameter, g, based on measurements of azimuth distributions of the Raman scattering probability (RSP), the near-absolute rotational Raman scattering (RRS) intensity by the University of Colorado two-dimensional (2-D) MAX-DOAS. The retrievals are maximally sensitive at low AOD and do not require absolute radiance calibration. We compare results with data from independent sensors.
R. Hossaini, P. K. Patra, A. A. Leeson, G. Krysztofiak, N. L. Abraham, S. J. Andrews, A. T. Archibald, J. Aschmann, E. L. Atlas, D. A. Belikov, H. Bönisch, L. J. Carpenter, S. Dhomse, M. Dorf, A. Engel, W. Feng, S. Fuhlbrügge, P. T. Griffiths, N. R. P. Harris, R. Hommel, T. Keber, K. Krüger, S. T. Lennartz, S. Maksyutov, H. Mantle, G. P. Mills, B. Miller, S. A. Montzka, F. Moore, M. A. Navarro, D. E. Oram, K. Pfeilsticker, J. A. Pyle, B. Quack, A. D. Robinson, E. Saikawa, A. Saiz-Lopez, S. Sala, B.-M. Sinnhuber, S. Taguchi, S. Tegtmeier, R. T. Lidster, C. Wilson, and F. Ziska
Atmos. Chem. Phys., 16, 9163–9187, https://doi.org/10.5194/acp-16-9163-2016, https://doi.org/10.5194/acp-16-9163-2016, 2016
Dene R. Bowdalo, Mathew J. Evans, and Eric D. Sofen
Atmos. Chem. Phys., 16, 8295–8308, https://doi.org/10.5194/acp-16-8295-2016, https://doi.org/10.5194/acp-16-8295-2016, 2016
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We introduce a new methodology for the assessment of atmospheric models with observations. We apply a spectral analysis methodology to hourly ozone observations and the equivalent model output. The spectrally transformed observational data show significant peaks on daily and annual timescales. Comparison between the amplitude and phase of these peaks introduces a new comparison methodology between model and measurements. We find the model shows significant biases on an annual timescale.
Yuzo Miyazaki, Sean Coburn, Kaori Ono, David T. Ho, R. Bradley Pierce, Kimitaka Kawamura, and Rainer Volkamer
Atmos. Chem. Phys., 16, 7695–7707, https://doi.org/10.5194/acp-16-7695-2016, https://doi.org/10.5194/acp-16-7695-2016, 2016
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We conducted a WSOC-specific 13C analysis of submicron marine aerosols over the eastern equatorial Pacific for the first time. The analysis of 13C combined with monosaccharides provides evidence of a significant contribution of marine dissolved organic carbon (DOC) to submicron particles in the MBL regardless of the oceanic area. The study demonstrates that DOC is closely correlated with the submicron WSOC and implies that it may characterize background OA in the MBL over the study region.
Chris Reed, Charlotte A. Brumby, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Paul W. Seakins, James D. Lee, and Lucy J. Carpenter
Atmos. Meas. Tech., 9, 2483–2495, https://doi.org/10.5194/amt-9-2483-2016, https://doi.org/10.5194/amt-9-2483-2016, 2016
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A new method of measuring nitrous acid (HONO), a potent mediator of air quality in the atmosphere as well as an important indoor pollutant, is presented. The new method relies on simple, proven techniques already widely applied to other atmospheric compounds. The technique can be retrofitted to existing analysers at minimal cost, or developed into instruments capable of very fast measurement which allow for more complex analysis of the behaviour of HONO.
Alicia Gressent, Bastien Sauvage, Daniel Cariolle, Mathew Evans, Maud Leriche, Céline Mari, and Valérie Thouret
Atmos. Chem. Phys., 16, 5867–5889, https://doi.org/10.5194/acp-16-5867-2016, https://doi.org/10.5194/acp-16-5867-2016, 2016
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In chemical transport models, NOx emitted by lightning (LNOx) is instantaneously diluted into the grid. A plume-in-grid parameterization to account for the sub-grid chemistry of LNOx is presented. This approach was implemented into the GEOS-Chem model and leads to a relative increase of NOx and O3 (18 % and 2 %, respectively, in July) on a large scale downwind of lightning emissions and a relative decrease (25 % and 8 %, respectively, over central Africa in July) over the regions of emissions.
Chris Reed, Mathew J. Evans, Piero Di Carlo, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 16, 4707–4724, https://doi.org/10.5194/acp-16-4707-2016, https://doi.org/10.5194/acp-16-4707-2016, 2016
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The self-cleaning capacity of the atmosphere in places like Antarctica can be measured by quantifying very low amounts of combustion products that exist in a well-known ratio. When this ratio deviates from 1 it points to the existence of unknown compounds. Several unknown compounds have been theorized to exist but never measured. We have found the method for measuring the ratio of combustion products suffers a bias in remote places, which when taken into account disproves any unknown compounds.
Frank A. F. Winiberg, Terry J. Dillon, Stephanie C. Orr, Christoph B. M Groß, Iustinian Bejan, Charlotte A. Brumby, Matthew J. Evans, Shona C. Smith, Dwayne E. Heard, and Paul W. Seakins
Atmos. Chem. Phys., 16, 4023–4042, https://doi.org/10.5194/acp-16-4023-2016, https://doi.org/10.5194/acp-16-4023-2016, 2016
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OH radicals are important intermediates in the atmosphere, and the high concentrations observed in tropical regions are yet to be fully explained. Radical-radical reactions such as the title reaction can contribute to OH formation. This is the most fully comprehensive study of the CH3C(O)O2 + HO2 reaction with direct observation of products in all reaction channels. The implications of the new measurements on OH, PAN and NOx concentrations are considered via global models.
Sean Coburn, Barbara Dix, Eric Edgerton, Christopher D. Holmes, Douglas Kinnison, Qing Liang, Arnout ter Schure, Siyuan Wang, and Rainer Volkamer
Atmos. Chem. Phys., 16, 3743–3760, https://doi.org/10.5194/acp-16-3743-2016, https://doi.org/10.5194/acp-16-3743-2016, 2016
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Here we present a day of case study measurements of the vertical distribution of bromine monoxide over the coastal region of the Gulf of Mexico. These measurements are used to assess the contribution of bromine radicals to the oxidation of elemental mercury in the troposphere. We find that the measured levels of bromine in the troposphere are sufficient to quickly oxidize mercury, which has significant implications for our understanding of atmospheric mercury processes.
Marcella Busilacchio, Piero Di Carlo, Eleonora Aruffo, Fabio Biancofiore, Cesare Dari Salisburgo, Franco Giammaria, Stephane Bauguitte, James Lee, Sarah Moller, James Hopkins, Shalini Punjabi, Stephen Andrews, Alistair C. Lewis, Mark Parrington, Paul I. Palmer, Edward Hyer, and Glenn M. Wolfe
Atmos. Chem. Phys., 16, 3485–3497, https://doi.org/10.5194/acp-16-3485-2016, https://doi.org/10.5194/acp-16-3485-2016, 2016
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Boreal fire emissions have little effect on ozone concentrations but evident impact on some NOx reservoirs as peroxy nitrates that we quantified. This should be taken into account since NOx reservoirs can be efficiently transported and may influence the ozone budget far away from the fire emission.
The study is based on observations carried out on board the BAe 146 aircraft during BORTAS in Canada. We used a custom laser-induced fluorescence system to measure NO2 and NOx reservoirs.
Sunil Baidar, Natalie Kille, Ivan Ortega, Roman Sinreich, David Thomson, James Hannigan, and Rainer Volkamer
Atmos. Meas. Tech., 9, 963–972, https://doi.org/10.5194/amt-9-963-2016, https://doi.org/10.5194/amt-9-963-2016, 2016
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We present development of a digital mobile solar tracker which can be coupled simultaneously to UV–Vis and FTIR spectrometers to measure trace gases in the atmosphere. We demonstrate an angular precision of 0.052º (about 1/10 of the solar disk diameter) during research drives and verify this tracking precision from measurements of the center to limb darkening (CLD, the changing appearance of Fraunhofer lines) in the mobile direct sun DOAS spectra.
C. R. Hoyle, C. Fuchs, E. Järvinen, H. Saathoff, A. Dias, I. El Haddad, M. Gysel, S. C. Coburn, J. Tröstl, A.-K. Bernhammer, F. Bianchi, M. Breitenlechner, J. C. Corbin, J. Craven, N. M. Donahue, J. Duplissy, S. Ehrhart, C. Frege, H. Gordon, N. Höppel, M. Heinritzi, T. B. Kristensen, U. Molteni, L. Nichman, T. Pinterich, A. S. H. Prévôt, M. Simon, J. G. Slowik, G. Steiner, A. Tomé, A. L. Vogel, R. Volkamer, A. C. Wagner, R. Wagner, A. S. Wexler, C. Williamson, P. M. Winkler, C. Yan, A. Amorim, J. Dommen, J. Curtius, M. W. Gallagher, R. C. Flagan, A. Hansel, J. Kirkby, M. Kulmala, O. Möhler, F. Stratmann, D. R. Worsnop, and U. Baltensperger
Atmos. Chem. Phys., 16, 1693–1712, https://doi.org/10.5194/acp-16-1693-2016, https://doi.org/10.5194/acp-16-1693-2016, 2016
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A significant portion of sulphate, an important constituent of atmospheric aerosols, is formed via the aqueous phase oxidation of sulphur dioxide by ozone. The rate of this reaction has previously only been measured over a relatively small temperature range. Here, we use the state of the art CLOUD chamber at CERN to perform the first measurements of this reaction rate in super-cooled droplets, confirming that the existing extrapolation of the reaction rate to sub-zero temperatures is accurate.
E. D. Sofen, D. Bowdalo, M. J. Evans, F. Apadula, P. Bonasoni, M. Cupeiro, R. Ellul, I. E. Galbally, R. Girgzdiene, S. Luppo, M. Mimouni, A. C. Nahas, M. Saliba, and K. Tørseth
Earth Syst. Sci. Data, 8, 41–59, https://doi.org/10.5194/essd-8-41-2016, https://doi.org/10.5194/essd-8-41-2016, 2016
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We have brought together all publicly available surface ozone observations from online databases from 1971–2015, with 2200 sites representing regional background conditions appropriate for the evaluation of chemical transport and chemistry-climate models for projects such as the Chemistry-Climate Model Initiative. Gridded data sets of ozone metrics (mean, percentiles, MDA8, SOMO35, etc.) are available from the British Atmospheric Data Centre.
E. D. Sofen, D. Bowdalo, and M. J. Evans
Atmos. Chem. Phys., 16, 1445–1457, https://doi.org/10.5194/acp-16-1445-2016, https://doi.org/10.5194/acp-16-1445-2016, 2016
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We explore the global representativeness of a global surface ozone data set from a range of perspectives (area, biomes, chemical regimes, model uncertainty, model trends). We conclude that the current network fails to provide sufficient constraints for important regions/regimes, leading to uncertainty for a range of atmospheric composition challenges. We suggest 20 new locations for making surface ozone observations, which would significantly enhance our observational capability.
A. Spolaor, T. Opel, J. R. McConnell, O. J. Maselli, G. Spreen, C. Varin, T. Kirchgeorg, D. Fritzsche, A. Saiz-Lopez, and P. Vallelonga
The Cryosphere, 10, 245–256, https://doi.org/10.5194/tc-10-245-2016, https://doi.org/10.5194/tc-10-245-2016, 2016
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The role of sea ice in the Earth climate system is still under debate, although it is known to influence albedo, ocean circulation, and atmosphere-ocean heat and gas exchange. Here we present a reconstruction of 1950 to 1998 AD sea ice in the Laptev Sea based on the Akademii Nauk ice core (Severnaya Zemlya, Russian Arctic) and halogen measurements. The results suggest a connection between bromine and sea ice, as well as a connection between iodine concentration in snow and summer sea ice.
E. D. Sofen, M. J. Evans, and A. C. Lewis
Atmos. Chem. Phys., 15, 13627–13632, https://doi.org/10.5194/acp-15-13627-2015, https://doi.org/10.5194/acp-15-13627-2015, 2015
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As an air pollutant, O3 is monitored photometrically to assess compliance with air quality legislation. A recent study found a 1.8% reduction in its absorption cross section, which would lead to an equivalent increase in observed O3 concentrations. We estimate this would increase the number of sites out of compliance with air quality regulations in the EU and US by 20%. We draw attention to how small changes in gas metrology impacts attainment and compliance with legal air quality standards.
S. Fadnavis, K. Semeniuk, M. G. Schultz, M. Kiefer, A. Mahajan, L. Pozzoli, and S. Sonbawane
Atmos. Chem. Phys., 15, 11477–11499, https://doi.org/10.5194/acp-15-11477-2015, https://doi.org/10.5194/acp-15-11477-2015, 2015
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The model and MIPAS satellite data show that there are three regions which contribute substantial pollution to the south Asian UTLS: the Asian summer monsoon (ASM), the North American monsoon (NAM) and the West African monsoon (WAM). However, penetration due to ASM convection reaches deeper into the UTLS compared to NAM and WAM outflow. Simulations show that westerly winds drive North American and European pollutants eastward where they can become part of the ASM and lifted to LS.
R. J. Pope, N. H. Savage, M. P. Chipperfield, C. Ordóñez, and L. S. Neal
Atmos. Chem. Phys., 15, 11201–11215, https://doi.org/10.5194/acp-15-11201-2015, https://doi.org/10.5194/acp-15-11201-2015, 2015
M. Gil-Ojeda, M. Navarro-Comas, L. Gómez-Martín, J. A. Adame, A. Saiz-Lopez, C. A. Cuevas, Y. González, O. Puentedura, E. Cuevas, J.-F. Lamarque, D. Kinninson, and S. Tilmes
Atmos. Chem. Phys., 15, 10567–10579, https://doi.org/10.5194/acp-15-10567-2015, https://doi.org/10.5194/acp-15-10567-2015, 2015
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The NO2 seasonal evolution in the free troposphere (FT) has been established for the first time, based on a remote sensing technique (MAXDOAS) and thus avoiding the problems of the local pollution of in situ instruments. A clear seasonality has been found, with background levels of 20-40pptv. Evidence has been found on fast, direct injection of surface air into the free troposphere. This result might have implications on the FT distribution of halogens and other species with marine sources.
R. E. Dunmore, J. R. Hopkins, R. T. Lidster, J. D. Lee, M. J. Evans, A. R. Rickard, A. C. Lewis, and J. F. Hamilton
Atmos. Chem. Phys., 15, 9983–9996, https://doi.org/10.5194/acp-15-9983-2015, https://doi.org/10.5194/acp-15-9983-2015, 2015
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Technological shifts between fuel sources have had unexpected impacts on atmospheric composition and these significant changes can go undetected if source-specific monitoring infrastructure is not in place. We present chemically comprehensive, continuous measurements of organic compounds in a developed megacity (London), that show diesel-related hydrocarbons can dominate reactive carbon and ozone formation potential, highlighting a serious underestimation of this source in emission inventories.
A. Saiz-Lopez, C. S. Blaszczak-Boxe, and L. J. Carpenter
Atmos. Chem. Phys., 15, 9731–9746, https://doi.org/10.5194/acp-15-9731-2015, https://doi.org/10.5194/acp-15-9731-2015, 2015
H. M. Walker, D. Stone, T. Ingham, S. Vaughan, M. Cain, R. L. Jones, O. J. Kennedy, M. McLeod, B. Ouyang, J. Pyle, S. Bauguitte, B. Bandy, G. Forster, M. J. Evans, J. F. Hamilton, J. R. Hopkins, J. D. Lee, A. C. Lewis, R. T. Lidster, S. Punjabi, W. T. Morgan, and D. E. Heard
Atmos. Chem. Phys., 15, 8179–8200, https://doi.org/10.5194/acp-15-8179-2015, https://doi.org/10.5194/acp-15-8179-2015, 2015
I. Ortega, T. Koenig, R. Sinreich, D. Thomson, and R. Volkamer
Atmos. Meas. Tech., 8, 2371–2395, https://doi.org/10.5194/amt-8-2371-2015, https://doi.org/10.5194/amt-8-2371-2015, 2015
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We describe the University of Colorado 2-D-MAX-DOAS instrument and a retrieval to measure 3-D distributions of NO2. The spatial scale over which NO2 is probed is systematically varied by measuring NO2 at three different wavelengths. This has a significant effect on the comparison with the NO2 VCD as measured by OMI. The challenges and opportunities to validate satellites under inhomogeneous conditions as well as to pinpoint hydrocarbon chemistry around the measurement site are discussed.
R. J. Pope, M. P. Chipperfield, N. H. Savage, C. Ordóñez, L. S. Neal, L. A. Lee, S. S. Dhomse, N. A. D. Richards, and T. D. Keslake
Atmos. Chem. Phys., 15, 5611–5626, https://doi.org/10.5194/acp-15-5611-2015, https://doi.org/10.5194/acp-15-5611-2015, 2015
J. D. Allan, P. I. Williams, J. Najera, J. D. Whitehead, M. J. Flynn, J. W. Taylor, D. Liu, E. Darbyshire, L. J. Carpenter, R. Chance, S. J. Andrews, S. C. Hackenberg, and G. McFiggans
Atmos. Chem. Phys., 15, 5599–5609, https://doi.org/10.5194/acp-15-5599-2015, https://doi.org/10.5194/acp-15-5599-2015, 2015
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New particle formation (NPF) is an important contributor to aerosol number concentrations in the Arctic and thus has a major role in dictating cloud properties and climate in this region. Here we present direct evidence that the oxidation of iodine in the atmosphere causes NPF in the Greenland Sea. This is important because this is a NPF mechanism that has not previously been considered in modelling studies at these latitudes.
R. Volkamer, S. Baidar, T. L. Campos, S. Coburn, J. P. DiGangi, B. Dix, E. W. Eloranta, T. K. Koenig, B. Morley, I. Ortega, B. R. Pierce, M. Reeves, R. Sinreich, S. Wang, M. A. Zondlo, and P. A. Romashkin
Atmos. Meas. Tech., 8, 2121–2148, https://doi.org/10.5194/amt-8-2121-2015, https://doi.org/10.5194/amt-8-2121-2015, 2015
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Tropospheric halogens and small oxygenated VOC (OVOC) modify tropospheric HOx and NOx, O3 and aerosols. We have measured bromine monoxide (BrO), iodine monoxide (IO), glyoxal (CHOCHO) profiles from research aircraft in the tropical troposphere and compare with ship- and aircraft-based in situ sensors. Our measurements point to the need to improve the representation of halogens and organic carbon sources in atmospheric models.
R. Thalman, M. T. Baeza-Romero, S. M. Ball, E. Borrás, M. J. S. Daniels, I. C. A. Goodall, S. B. Henry, T. Karl, F. N. Keutsch, S. Kim, J. Mak, P. S. Monks, A. Muñoz, J. Orlando, S. Peppe, A. R. Rickard, M. Ródenas, P. Sánchez, R. Seco, L. Su, G. Tyndall, M. Vázquez, T. Vera, E. Waxman, and R. Volkamer
Atmos. Meas. Tech., 8, 1835–1862, https://doi.org/10.5194/amt-8-1835-2015, https://doi.org/10.5194/amt-8-1835-2015, 2015
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Measurements of α-dicarbonyl compounds, like glyoxal (CHOCHO) and methyl glyoxal (CH3C(O)CHO), are informative about the rate of hydrocarbon oxidation, oxidative capacity, and secondary organic aerosol (SOA) formation in the atmosphere. We have compared nine instruments and seven techniques to measure α-dicarbonyl, using simulation chamber facilities in the US and Europe. We assess our understanding of calibration, precision, accuracy and detection limits, as well as possible sampling biases.
S. J. Andrews, S. C. Hackenberg, and L. J. Carpenter
Ocean Sci., 11, 313–321, https://doi.org/10.5194/os-11-313-2015, https://doi.org/10.5194/os-11-313-2015, 2015
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The oceans are a key source of a number of atmospherically
important volatile gases. The accurate and robust
determination of trace gases in seawater is a significant
analytical challenge. Here we describe a gas chromatograph mass spectrometer based purge and trap system that was developed for the fully automated analysis of dissolved very short-lived species (VSLS) in seawater sampled from a research ship.
L. K. Whalley, D. Stone, I. J. George, S. Mertes, D. van Pinxteren, A. Tilgner, H. Herrmann, M. J. Evans, and D. E. Heard
Atmos. Chem. Phys., 15, 3289–3301, https://doi.org/10.5194/acp-15-3289-2015, https://doi.org/10.5194/acp-15-3289-2015, 2015
C. Prados-Roman, C. A. Cuevas, R. P. Fernandez, D. E. Kinnison, J-F. Lamarque, and A. Saiz-Lopez
Atmos. Chem. Phys., 15, 2215–2224, https://doi.org/10.5194/acp-15-2215-2015, https://doi.org/10.5194/acp-15-2215-2015, 2015
E. Spinei, A. Cede, J. Herman, G. H. Mount, E. Eloranta, B. Morley, S. Baidar, B. Dix, I. Ortega, T. Koenig, and R. Volkamer
Atmos. Meas. Tech., 8, 793–809, https://doi.org/10.5194/amt-8-793-2015, https://doi.org/10.5194/amt-8-793-2015, 2015
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This paper presents ground-based direct-sun and airborne multi-axis DOAS measurements of O2O2 absorption optical depths under atmospheric conditions in two wavelength regions (335-–390nm and 435--490nm). Our results show that laboratory-measured σ(O2O2) is applicable for observations over a wide range of atmospheric conditions. Temperature dependence of σ(O2O2) is about 9±2.5% from 231K to 275K.
C. Prados-Roman, C. A. Cuevas, T. Hay, R. P. Fernandez, A. S. Mahajan, S.-J. Royer, M. Galí, R. Simó, J. Dachs, K. Großmann, D. E. Kinnison, J.-F. Lamarque, and A. Saiz-Lopez
Atmos. Chem. Phys., 15, 583–593, https://doi.org/10.5194/acp-15-583-2015, https://doi.org/10.5194/acp-15-583-2015, 2015
R. P. Fernandez, R. J. Salawitch, D. E. Kinnison, J.-F. Lamarque, and A. Saiz-Lopez
Atmos. Chem. Phys., 14, 13391–13410, https://doi.org/10.5194/acp-14-13391-2014, https://doi.org/10.5194/acp-14-13391-2014, 2014
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We propose the existence of a daytime “tropical ring of atomic bromine” surrounding the tropics at a height between 15 and 19km. Our simulations show that VSL bromocarbons produce increases of 3pptv for inorganic bromine and 2pptv for organic bromine in the tropical TTL on an annual average, resulting in a total stratospheric bromine injection of 5pptv. This result suggests that the inorganic bromine injected into the stratosphere may be larger than that from VSL bromocarbons.
U. R. Thorenz, L. J. Carpenter, R.-J. Huang, M. Kundel, J. Bosle, and T. Hoffmann
Atmos. Chem. Phys., 14, 13327–13335, https://doi.org/10.5194/acp-14-13327-2014, https://doi.org/10.5194/acp-14-13327-2014, 2014
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Phytoplankton suspensions were treated with high and low ozone levels, and volatile iodine (I2)-containing compounds were measured. Iodocarbon emissions were independent of the ozone level. I2 emission showed a strong dependency on the ozone level in the air as well as on the iodide concentration in the sample suspension. The experiments show that microalgae suspensions are capable of emitting I2 by the reaction of ozone with dissolved iodide at the air-water interface under natural conditions.
A. Saiz-Lopez, R. P. Fernandez, C. Ordóñez, D. E. Kinnison, J. C. Gómez Martín, J.-F. Lamarque, and S. Tilmes
Atmos. Chem. Phys., 14, 13119–13143, https://doi.org/10.5194/acp-14-13119-2014, https://doi.org/10.5194/acp-14-13119-2014, 2014
S. Fadnavis, M. G. Schultz, K. Semeniuk, A. S. Mahajan, L. Pozzoli, S. Sonbawne, S. D. Ghude, M. Kiefer, and E. Eckert
Atmos. Chem. Phys., 14, 12725–12743, https://doi.org/10.5194/acp-14-12725-2014, https://doi.org/10.5194/acp-14-12725-2014, 2014
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The Asian summer monsoon transports pollutants from local emission sources to the upper troposphere and lower stratosphere (UTLS). The increasing trend of these pollutants may have climatic impact. This study addresses the impact of convectively lifted Indian and Chinese emissions on the ULTS. Sensitivity experiments with emission changes in particular regions show that Chinese emissions have a greater impact on the concentrations of NOY species than Indian emissions.
S. Coburn, I. Ortega, R. Thalman, B. Blomquist, C. W. Fairall, and R. Volkamer
Atmos. Meas. Tech., 7, 3579–3595, https://doi.org/10.5194/amt-7-3579-2014, https://doi.org/10.5194/amt-7-3579-2014, 2014
L. Kritten, A. Butz, M. P. Chipperfield, M. Dorf, S. Dhomse, R. Hossaini, H. Oelhaf, C. Prados-Roman, G. Wetzel, and K. Pfeilsticker
Atmos. Chem. Phys., 14, 9555–9566, https://doi.org/10.5194/acp-14-9555-2014, https://doi.org/10.5194/acp-14-9555-2014, 2014
S. Fadnavis, K. Semeniuk, M. G. Schultz, A. Mahajan, L. Pozzoli, S. Sonbawane, and M. Kiefer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-20159-2014, https://doi.org/10.5194/acpd-14-20159-2014, 2014
Revised manuscript not accepted
R. T. Lidster, J. F. Hamilton, J. D. Lee, A. C. Lewis, J. R. Hopkins, S. Punjabi, A. R. Rickard, and J. C. Young
Atmos. Chem. Phys., 14, 6677–6693, https://doi.org/10.5194/acp-14-6677-2014, https://doi.org/10.5194/acp-14-6677-2014, 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
S. M. MacDonald, J. C. Gómez Martín, R. Chance, S. Warriner, A. Saiz-Lopez, L. J. Carpenter, and J. M. C. Plane
Atmos. Chem. Phys., 14, 5841–5852, https://doi.org/10.5194/acp-14-5841-2014, https://doi.org/10.5194/acp-14-5841-2014, 2014
M. J. Lawler, A. S. Mahajan, A. Saiz-Lopez, and E. S. Saltzman
Atmos. Chem. Phys., 14, 2669–2678, https://doi.org/10.5194/acp-14-2669-2014, https://doi.org/10.5194/acp-14-2669-2014, 2014
D. Stone, M. J. Evans, H. Walker, T. Ingham, S. Vaughan, B. Ouyang, O. J. Kennedy, M. W. McLeod, R. L. Jones, J. Hopkins, S. Punjabi, R. Lidster, J. F. Hamilton, J. D. Lee, A. C. Lewis, L. J. Carpenter, G. Forster, D. E. Oram, C. E. Reeves, S. Bauguitte, W. Morgan, H. Coe, E. Aruffo, C. Dari-Salisburgo, F. Giammaria, P. Di Carlo, and D. E. Heard
Atmos. Chem. Phys., 14, 1299–1321, https://doi.org/10.5194/acp-14-1299-2014, https://doi.org/10.5194/acp-14-1299-2014, 2014
S. Zhou, L. Gonzalez, A. Leithead, Z. Finewax, R. Thalman, A. Vlasenko, S. Vagle, L.A. Miller, S.-M. Li, S. Bureekul, H. Furutani, M. Uematsu, R. Volkamer, and J. Abbatt
Atmos. Chem. Phys., 14, 1371–1384, https://doi.org/10.5194/acp-14-1371-2014, https://doi.org/10.5194/acp-14-1371-2014, 2014
F. Wang, A. Saiz-Lopez, A. S. Mahajan, J. C. Gómez Martín, D. Armstrong, M. Lemes, T. Hay, and C. Prados-Roman
Atmos. Chem. Phys., 14, 1323–1335, https://doi.org/10.5194/acp-14-1323-2014, https://doi.org/10.5194/acp-14-1323-2014, 2014
R. Hossaini, H. Mantle, M. P. Chipperfield, S. A. Montzka, P. Hamer, F. Ziska, B. Quack, K. Krüger, S. Tegtmeier, E. Atlas, S. Sala, A. Engel, H. Bönisch, T. Keber, D. Oram, G. Mills, C. Ordóñez, A. Saiz-Lopez, N. Warwick, Q. Liang, W. Feng, F. Moore, B. R. Miller, V. Marécal, N. A. D. Richards, M. Dorf, and K. Pfeilsticker
Atmos. Chem. Phys., 13, 11819–11838, https://doi.org/10.5194/acp-13-11819-2013, https://doi.org/10.5194/acp-13-11819-2013, 2013
P. M. Edwards, M. J. Evans, K. L. Furneaux, J. Hopkins, T. Ingham, C. Jones, J. D. Lee, A. C. Lewis, S. J. Moller, D. Stone, L. K. Whalley, and D. E. Heard
Atmos. Chem. Phys., 13, 9497–9514, https://doi.org/10.5194/acp-13-9497-2013, https://doi.org/10.5194/acp-13-9497-2013, 2013
F. Ziska, B. Quack, K. Abrahamsson, S. D. Archer, E. Atlas, T. Bell, J. H. Butler, L. J. Carpenter, C. E. Jones, N. R. P. Harris, H. Hepach, K. G. Heumann, C. Hughes, J. Kuss, K. Krüger, P. Liss, R. M. Moore, A. Orlikowska, S. Raimund, C. E. Reeves, W. Reifenhäuser, A. D. Robinson, C. Schall, T. Tanhua, S. Tegtmeier, S. Turner, L. Wang, D. Wallace, J. Williams, H. Yamamoto, S. Yvon-Lewis, and Y. Yokouchi
Atmos. Chem. Phys., 13, 8915–8934, https://doi.org/10.5194/acp-13-8915-2013, https://doi.org/10.5194/acp-13-8915-2013, 2013
R. Sinreich, A. Merten, L. Molina, and R. Volkamer
Atmos. Meas. Tech., 6, 1521–1532, https://doi.org/10.5194/amt-6-1521-2013, https://doi.org/10.5194/amt-6-1521-2013, 2013
J. R. Pierce, M. J. Evans, C. E. Scott, S. D. D'Andrea, D. K. Farmer, E. Swietlicki, and D. V. Spracklen
Atmos. Chem. Phys., 13, 3163–3176, https://doi.org/10.5194/acp-13-3163-2013, https://doi.org/10.5194/acp-13-3163-2013, 2013
S. Baidar, H. Oetjen, S. Coburn, B. Dix, I. Ortega, R. Sinreich, and R. Volkamer
Atmos. Meas. Tech., 6, 719–739, https://doi.org/10.5194/amt-6-719-2013, https://doi.org/10.5194/amt-6-719-2013, 2013
N. H. Savage, P. Agnew, L. S. Davis, C. Ordóñez, R. Thorpe, C. E. Johnson, F. M. O'Connor, and M. Dalvi
Geosci. Model Dev., 6, 353–372, https://doi.org/10.5194/gmd-6-353-2013, https://doi.org/10.5194/gmd-6-353-2013, 2013
A. C. Lewis, M. J. Evans, J. R. Hopkins, S. Punjabi, K. A. Read, R. M. Purvis, S. J. Andrews, S. J. Moller, L. J. Carpenter, J. D. Lee, A. R. Rickard, P. I. Palmer, and M. Parrington
Atmos. Chem. Phys., 13, 851–867, https://doi.org/10.5194/acp-13-851-2013, https://doi.org/10.5194/acp-13-851-2013, 2013
A. S. Mahajan, J. C. Gómez Martín, T. D. Hay, S.-J. Royer, S. Yvon-Lewis, Y. Liu, L. Hu, C. Prados-Roman, C. Ordóñez, J. M. C. Plane, and A. Saiz-Lopez
Atmos. Chem. Phys., 12, 11609–11617, https://doi.org/10.5194/acp-12-11609-2012, https://doi.org/10.5194/acp-12-11609-2012, 2012
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
An improved estimate of inorganic iodine emissions from the ocean using a coupled surface microlayer box model
Impact of improved representation of volatile organic compound emissions and production of NOx reservoirs on modeled urban ozone production
The effect of different climate and air quality policies in China on in situ ozone production in Beijing
Enhancing long-term trend simulation of the global tropospheric hydroxyl (TOH) and its drivers from 2005 to 2019: a synergistic integration of model simulations and satellite observations
Intercomparison of GEOS-Chem and CAM-chem tropospheric oxidant chemistry within the Community Earth System Model version 2 (CESM2)
Development of a detailed gaseous oxidation scheme of naphthalene for secondary organic aerosol (SOA) formation and speciation
Large contributions of soil emissions to the atmospheric nitrogen budget and their impacts on air quality and temperature rise in North China
Why did ozone concentrations remain high during Shanghai's static management? A statistical and radical-chemistry perspective
Revising VOC emissions speciation improves the simulation of global background ethane and propane
Changes in South American surface ozone trends: exploring the influences of precursors and extreme events
Evaluating NOx stack plume emissions using a high-resolution atmospheric chemistry model and satellite-derived NO2 columns
NOx emissions in France in 2019–2021 as estimated by the high-spatial-resolution assimilation of TROPOMI NO2 observations
Aggravated surface O3 pollution primarily driven by meteorological variations in China during the 2020 COVID-19 pandemic lockdown period
Identifying decadal trends in deweathered concentrations of criteria air pollutants in Canadian urban atmospheres with machine learning approaches
Evaluation of modelled versus observed non-methane volatile organic compounds at European Monitoring and Evaluation Programme sites in Europe
Constraining non-methane VOC emissions with TROPOMI HCHO observations: impact on summertime ozone simulation in August 2022 in China
Revealing the significant acceleration of hydrofluorocarbon (HFC) emissions in eastern Asia through long-term atmospheric observations
Interpreting Geostationary Environment Monitoring Spectrometer (GEMS) geostationary satellite observations of the diurnal variation in nitrogen dioxide (NO2) over East Asia
An intercomparison of satellite, airborne, and ground-level observations with WRF–CAMx simulations of NO2 columns over Houston, Texas, during the September 2021 TRACER-AQ campaign
Impact of methane and other precursor emission reductions on surface ozone in Europe: Scenario analysis using the EMEP MSC-W model
Interannual variability of summertime formaldehyde (HCHO) vertical column density and its main drivers at northern high latitudes
The impact of multi-decadal changes in VOC speciation on urban ozone chemistry: a case study in Birmingham, United Kingdom
Technical note: Challenges in detecting free tropospheric ozone trends in a sparsely sampled environment
Combined assimilation of NOAA surface and MIPAS satellite observations to constrain the global budget of carbonyl sulfide
The impact of gaseous degradation on the gas–particle partitioning of methylated polycyclic aromatic hydrocarbons
Technical note: An assessment of the performance of statistical bias correction techniques for global chemistry–climate model surface ozone fields
A better representation of volatile organic compound chemistry in WRF-Chem and its impact on ozone over Los Angeles
High-resolution US methane emissions inferred from an inversion of 2019 TROPOMI satellite data: contributions from individual states, urban areas, and landfills
Summertime tropospheric ozone source apportionment study in the Madrid region (Spain)
CO anthropogenic emissions in Europe from 2011 to 2021: insights from Measurement of Pollution in the Troposphere (MOPITT) satellite data
Constraining long-term NOx emissions over the United States and Europe using nitrate wet deposition monitoring networks
An investigation into atmospheric nitrous acid (HONO) processes in South Korea
Analysis of an intense O3 pollution episode on the Atlantic coast of the Iberian Peninsula using photochemical modeling: characterization of transport pathways and accumulation processes
A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021
Atmospheric oxygen as a tracer for fossil fuel carbon dioxide: a sensitivity study in the UK
MIXv2: a long-term mosaic emission inventory for Asia (2010–2017)
Ether and ester formation from peroxy radical recombination: A qualitative reaction channel analysis
Process Analysis of Elevated Concentrations of Organic Acids at Whiteface Mountain, New York
Organosulfate produced from consumption of SO3 speeds up sulfuric acid–dimethylamine atmospheric nucleation
Tropospheric Ozone Precursors: Global and Regional Distributions, Trends and Variability
Contribution of expanded marine sulfur chemistry to the seasonal variability of dimethyl sulfide oxidation products and size-resolved sulfate aerosol
Verifying national inventory-based combustion emissions of CO2 across the UK and mainland Europe using satellite observations of atmospheric CO and CO2
Spatial disparities of ozone pollution in the Sichuan Basin spurred by extreme, hot weather
Global impacts of aviation on air quality evaluated at high resolution
Bias correction of OMI HCHO columns based on FTIR and aircraft measurements and impact on top-down emission estimates
Investigation of the renewed methane growth post-2007 with high-resolution 3-D variational inverse modeling and isotopic constraints
Revisiting day-of-week ozone patterns in an era of evolving US air quality
The contribution of transport emissions to ozone mixing ratios and methane lifetime in 2015 and 2050 in the Shared Socioeconomic Pathways (SSPs)
Performance evaluation of UKESM1 for surface ozone across the pan-tropics
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 9899–9921, https://doi.org/10.5194/acp-24-9899-2024, https://doi.org/10.5194/acp-24-9899-2024, 2024
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Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterize and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
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.
Beth S. Nelson, Zhenze Liu, Freya A. Squires, Marvin Shaw, James R. Hopkins, Jacqueline F. Hamilton, Andrew R. Rickard, Alastair C. Lewis, Zongbo Shi, and James D. Lee
Atmos. Chem. Phys., 24, 9031–9044, https://doi.org/10.5194/acp-24-9031-2024, https://doi.org/10.5194/acp-24-9031-2024, 2024
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The impact of combined air quality and carbon neutrality policies on O3 formation in Beijing was investigated. Emissions inventory data were used to estimate future pollutant mixing ratios relative to ground-level observations. O3 production was found to be most sensitive to changes in alkenes, but large reductions in less reactive compounds led to larger reductions in future O3 production. This study highlights the importance of understanding the emissions of organic pollutants.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
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We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
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.
Victor Lannuque and Karine Sartelet
Atmos. Chem. Phys., 24, 8589–8606, https://doi.org/10.5194/acp-24-8589-2024, https://doi.org/10.5194/acp-24-8589-2024, 2024
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation and speciation from naphthalene oxidation. This study details the development of the first near-explicit chemical scheme for naphthalene oxidation by OH, which includes kinetic and mechanistic data, and is able to reproduce most of the experimentally identified products in both gas and particle phases.
Tong Sha, Siyu Yang, Qingcai Chen, Liangqing Li, Xiaoyan Ma, Yan-Lin Zhang, Zhaozhong Feng, K. Folkert Boersma, and Jun Wang
Atmos. Chem. Phys., 24, 8441–8455, https://doi.org/10.5194/acp-24-8441-2024, https://doi.org/10.5194/acp-24-8441-2024, 2024
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Using an updated soil reactive nitrogen emission scheme in the Unified Inputs for Weather Research and Forecasting coupled with Chemistry (UI-WRF-Chem) model, we investigate the role of soil NO and HONO (Nr) emissions in air quality and temperature in North China. Contributions of soil Nr emissions to O3 and secondary pollutants are revealed, exceeding effects of soil NOx or HONO emission. Soil Nr emissions play an important role in mitigating O3 pollution and addressing climate change.
Jian Zhu, Shanshan Wang, Chuanqi Gu, Zhiwen Jiang, Sanbao Zhang, Ruibin Xue, Yuhao Yan, and Bin Zhou
Atmos. Chem. Phys., 24, 8383–8395, https://doi.org/10.5194/acp-24-8383-2024, https://doi.org/10.5194/acp-24-8383-2024, 2024
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In 2022, Shanghai implemented city-wide static management measures during the high-ozone season in April and May, providing a chance to study ozone pollution control. Despite significant emissions reductions, ozone levels increased by 23 %. Statistically, the number of days with higher ozone diurnal variation types increased during the lockdown period. The uneven decline in VOC and NO2 emissions led to heightened photochemical processes, resulting in the observed ozone level rise.
Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
Atmos. Chem. Phys., 24, 8317–8342, https://doi.org/10.5194/acp-24-8317-2024, https://doi.org/10.5194/acp-24-8317-2024, 2024
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Ethane and propane are volatile organic compounds emitted from human activities which help to form ozone, a pollutant and greenhouse gas, and also affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job of reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emissions, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
Rodrigo J. Seguel, Lucas Castillo, Charlie Opazo, Néstor Y. Rojas, Thiago Nogueira, María Cazorla, Mario Gavidia-Calderón, Laura Gallardo, René Garreaud, Tomás Carrasco-Escaff, and Yasin Elshorbany
Atmos. Chem. Phys., 24, 8225–8242, https://doi.org/10.5194/acp-24-8225-2024, https://doi.org/10.5194/acp-24-8225-2024, 2024
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Trends of surface ozone were examined across South America. Our findings indicate that ozone trends in major South American cities either increase or remain steady, with no signs of decline. The upward trends can be attributed to chemical regimes that efficiently convert nitric oxide into nitrogen dioxide. Additionally, our results suggest a climate penalty for ozone driven by meteorological conditions that favor wildfire propagation in Chile and extensive heat waves in southern Brazil.
Maarten Krol, Bart van Stratum, Isidora Anglou, and Klaas Folkert Boersma
Atmos. Chem. Phys., 24, 8243–8262, https://doi.org/10.5194/acp-24-8243-2024, https://doi.org/10.5194/acp-24-8243-2024, 2024
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This paper presents detailed plume simulations of nitrogen oxides and carbon dioxide that are emitted from four large industrial facilities world-wide. Results from the high-resolution simulations that include atmospheric chemistry are compared to nitrogen dioxide observations from satellites. We find good performance of the model and show that common assumptions that are used in simplified models need revision. This work is important for the monitoring of emissions using satellite data.
Robin Plauchu, Audrey Fortems-Cheiney, Grégoire Broquet, Isabelle Pison, Antoine Berchet, Elise Potier, Gaëlle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, and Henk Eskes
Atmos. Chem. Phys., 24, 8139–8163, https://doi.org/10.5194/acp-24-8139-2024, https://doi.org/10.5194/acp-24-8139-2024, 2024
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This study uses the Community Inversion Framework and CHIMERE model to assess the potential of TROPOMI-S5P PAL NO2 tropospheric column data to estimate NOx emissions in France (2019–2021). Results show a 3 % decrease in average emissions compared to the 2016 CAMS-REG/INS, lower than the 14 % decrease from CITEPA. The study highlights challenges in capturing emission anomalies due to limited data coverage and error levels but shows promise for local inventory improvements.
Zhendong Lu, Jun Wang, Yi Wang, Daven K. Henze, Xi Chen, Tong Sha, and Kang Sun
Atmos. Chem. Phys., 24, 7793–7813, https://doi.org/10.5194/acp-24-7793-2024, https://doi.org/10.5194/acp-24-7793-2024, 2024
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In contrast with past work showing that the reduction of emissions was the dominant factor for the nationwide increase of surface O3 during the lockdown in China, this study finds that the variation in meteorology (temperature and other parameters) plays a more important role. This result is obtained through sensitivity simulations using a chemical transport model constrained by satellite (TROPOMI) data and calibrated with surface observations.
Xiaohong Yao and Leiming Zhang
Atmos. Chem. Phys., 24, 7773–7791, https://doi.org/10.5194/acp-24-7773-2024, https://doi.org/10.5194/acp-24-7773-2024, 2024
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This study investigates long-term trends of criteria air pollutants, including NO2, CO, SO2, O3 and PM2.5, and NO2+O3 measured in 10 Canadian cities during the last 2 to 3 decades. We also investigate associated driving forces in terms of emission reductions, perturbations from varying weather conditions and large-scale wildfires, as well as changes in O3 sources and sinks.
Yao Ge, Sverre Solberg, Mathew R. Heal, Stefan Reimann, Willem van Caspel, Bryan Hellack, Thérèse Salameh, and David Simpson
Atmos. Chem. Phys., 24, 7699–7729, https://doi.org/10.5194/acp-24-7699-2024, https://doi.org/10.5194/acp-24-7699-2024, 2024
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Atmospheric volatile organic compounds (VOCs) constitute many species, acting as precursors to ozone and aerosol. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the EMEP MSC-W to evaluate emission inventories in Europe. We focus on the varying agreement between modelled and measured VOCs across different species and underscore potential inaccuracies in total and sector-specific emission estimates.
Shuzhuang Feng, Fei Jiang, Tianlu Qian, Nan Wang, Mengwei Jia, Songci Zheng, Jiansong Chen, Fang Ying, and Weimin Ju
Atmos. Chem. Phys., 24, 7481–7498, https://doi.org/10.5194/acp-24-7481-2024, https://doi.org/10.5194/acp-24-7481-2024, 2024
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We developed a multi-air-pollutant inversion system to estimate non-methane volatile organic compound (NMVOC) emissions using TROPOMI formaldehyde retrievals. We found that the inversion significantly improved formaldehyde simulations and reduced NMVOC emission uncertainties. The optimized NMVOC emissions effectively corrected the overestimation of O3 levels, mainly by decreasing the rate of the RO2 + NO reaction and increasing the rate of the NO2 + OH reaction.
Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, and Sunyoung Park
Atmos. Chem. Phys., 24, 7309–7330, https://doi.org/10.5194/acp-24-7309-2024, https://doi.org/10.5194/acp-24-7309-2024, 2024
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We analyzed with an inversion model the atmospheric abundance of hydrofluorocarbons (HFCs), potent greenhouse gases, from 2008 to 2020 at Gosan station in South Korea and revealed a significant increase in emissions, especially from eastern China and Japan. This increase contradicts reported data, underscoring the need for accurate monitoring and reporting. Our findings are crucial for understanding and managing global HFCs emissions, highlighting the importance of efforts to reduce HFCs.
Laura Hyesung Yang, Daniel J. Jacob, Ruijun Dang, Yujin J. Oak, Haipeng Lin, Jhoon Kim, Shixian Zhai, Nadia K. Colombi, Drew C. Pendergrass, Ellie Beaudry, Viral Shah, Xu Feng, Robert M. Yantosca, Heesung Chong, Junsung Park, Hanlim Lee, Won-Jin Lee, Soontae Kim, Eunhye Kim, Katherine R. Travis, James H. Crawford, and Hong Liao
Atmos. Chem. Phys., 24, 7027–7039, https://doi.org/10.5194/acp-24-7027-2024, https://doi.org/10.5194/acp-24-7027-2024, 2024
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The Geostationary Environment Monitoring Spectrometer (GEMS) provides hourly measurements of NO2. We use the chemical transport model to find how emissions, chemistry, and transport drive the changes in NO2 observed by GEMS at different times of the day. In winter, the chemistry plays a minor role, and high daytime emissions dominate the diurnal variation in NO2, balanced by transport. In summer, emissions, chemistry, and transport play an important role in shaping the diurnal variation in NO2.
M. Omar Nawaz, Jeremiah Johnson, Greg Yarwood, Benjamin de Foy, Laura Judd, and Daniel L. Goldberg
Atmos. Chem. Phys., 24, 6719–6741, https://doi.org/10.5194/acp-24-6719-2024, https://doi.org/10.5194/acp-24-6719-2024, 2024
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NO2 is a gas with implications for air pollution. A campaign conducted in Houston provided an opportunity to compare NO2 from different instruments and a model. Aircraft and satellite observations agreed well with measurements on the ground; however, the latter estimated lower values. We find that model-simulated NO2 was lower than observations, especially downtown, suggesting that NO2 sources associated with the urban core of Houston, such as vehicle emissions, may be underestimated.
Willem Elias van Caspel, Zbigniew Klimont, Chris Heyes, and Hilde Fagerli
EGUsphere, https://doi.org/10.5194/egusphere-2024-1422, https://doi.org/10.5194/egusphere-2024-1422, 2024
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Methane in the atmosphere contributes to the production of ozone gas, which is an air pollutant as well as a greenhouse gas. In this study, the impact of reducing methane emissions on surface ozone is investigated for the United Nations Economic Commission for Europe (UNECE) region excluding North America and Israel (the "EMEP region"), in particular in terms of its importance in reaching the ozone exposure guideline limits set by the World Health Organization.
Tianlang Zhao, Jingqiu Mao, Zolal Ayazpour, Gonzalo González Abad, Caroline R. Nowlan, and Yiqi Zheng
Atmos. Chem. Phys., 24, 6105–6121, https://doi.org/10.5194/acp-24-6105-2024, https://doi.org/10.5194/acp-24-6105-2024, 2024
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HCHO variability is a key tracer in understanding VOC emissions in response to climate change. We investigate the role of methane oxidation and biogenic and wildfire emissions in HCHO interannual variability over northern high latitudes in summer, emphasizing wildfires as a key driver of HCHO interannual variability in Alaska, Siberia and northern Canada using satellite HCHO and SIF retrievals and then GEOS-Chem model. We show SIF is a tool to understand biogenic HCHO variability in this region.
Jianghao Li, Alastair C. Lewis, Jim R. Hopkins, Stephen J. Andrews, Tim Murrells, Neil Passant, Ben Richmond, Siqi Hou, William J. Bloss, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 24, 6219–6231, https://doi.org/10.5194/acp-24-6219-2024, https://doi.org/10.5194/acp-24-6219-2024, 2024
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A summertime ozone event at an urban site in Birmingham is sensitive to volatile organic compounds (VOCs) – particularly those of oxygenated VOCs. The roles of anthropogenic VOC sources in urban ozone chemistry are examined by integrating the 1990–2019 national atmospheric emission inventory into model scenarios. Road transport remains the most powerful means of further reducing ozone in this case study, but the benefits may be offset if solvent emissions of VOCs continue to increase.
Kai-Lan Chang, Owen R. Cooper, Audrey Gaudel, Irina Petropavlovskikh, Peter Effertz, Gary Morris, and Brian C. McDonald
Atmos. Chem. Phys., 24, 6197–6218, https://doi.org/10.5194/acp-24-6197-2024, https://doi.org/10.5194/acp-24-6197-2024, 2024
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A great majority of observational trend studies of free tropospheric ozone use sparsely sampled ozonesonde and aircraft measurements as reference data sets. A ubiquitous assumption is that trends are accurate and reliable so long as long-term records are available. We show that sampling bias due to sparse samples can persistently reduce the trend accuracy, and we highlight the importance of maintaining adequate frequency and continuity of observations.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Fu-Jie Zhu, Zi-Feng Zhang, Li-Yan Liu, Pu-Fei Yang, Peng-Tuan Hu, Geng-Bo Ren, Meng Qin, and Wan-Li Ma
Atmos. Chem. Phys., 24, 6095–6103, https://doi.org/10.5194/acp-24-6095-2024, https://doi.org/10.5194/acp-24-6095-2024, 2024
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Gas–particle (G–P) partitioning is an important atmospheric behavior for semi-volatile organic compounds (SVOCs). Diurnal variation in G–P partitioning of methylated polycyclic aromatic hydrocarbons (Me-PAHs) demonstrates the possible influence of gaseous degradation; the enhancement of gaseous degradation (1.10–5.58 times) on G–P partitioning is verified by a steady-state G–P partitioning model. The effect of gaseous degradation on G–P partitioning of (especially light) SVOCs is important.
Christoph Staehle, Harald E. Rieder, Arlene M. Fiore, and Jordan L. Schnell
Atmos. Chem. Phys., 24, 5953–5969, https://doi.org/10.5194/acp-24-5953-2024, https://doi.org/10.5194/acp-24-5953-2024, 2024
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Chemistry–climate models show biases compared to surface ozone observations and thus require bias correction for impact studies and the assessment of air quality changes. We compare the performance of commonly used correction techniques for model outputs available via CMIP6. While all methods can reduce model biases, better results are obtained from more complex approaches. Thus, our study suggests broader use of these techniques in studies seeking to inform air quality management and policy.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, J. Andrew Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
Atmos. Chem. Phys., 24, 5265–5286, https://doi.org/10.5194/acp-24-5265-2024, https://doi.org/10.5194/acp-24-5265-2024, 2024
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Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represents VOC chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from volatile chemical products and other anthropogenic sources to total VOC reactivity and O3.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Alba Lorente, Zichong Chen, Xiao Lu, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Margaux Winter, Shuang Ma, A. Anthony Bloom, John R. Worden, Robert N. Stavins, and Cynthia A. Randles
Atmos. Chem. Phys., 24, 5069–5091, https://doi.org/10.5194/acp-24-5069-2024, https://doi.org/10.5194/acp-24-5069-2024, 2024
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We quantify 2019 methane emissions in the contiguous US (CONUS) at a ≈ 25 km × 25 km resolution using satellite methane observations. We find a 13 % upward correction to the 2023 US Environmental Protection Agency (EPA) Greenhouse Gas Emissions Inventory (GHGI) for 2019, with large corrections to individual states, urban areas, and landfills. This may present a challenge for US climate policies and goals, many of which target significant reductions in methane emissions.
David de la Paz, Rafael Borge, Juan Manuel de Andrés, Luis Tovar, Golam Sarwar, and Sergey L. Napelenok
Atmos. Chem. Phys., 24, 4949–4972, https://doi.org/10.5194/acp-24-4949-2024, https://doi.org/10.5194/acp-24-4949-2024, 2024
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This source apportionment modeling study shows that around 70 % of ground-level O3 in Madrid (Spain) is transported from other regions. Nonetheless, emissions from local sources, mainly road traffic, play a significant role, especially under atmospheric stagnation. Local measures during those conditions may be able to reduce O3 peaks by up to 30 % and, thus, lessen impacts from high-O3 episodes in the Madrid metropolitan area.
Audrey Fortems-Cheiney, Gregoire Broquet, Elise Potier, Robin Plauchu, Antoine Berchet, Isabelle Pison, Hugo Denier van der Gon, and Stijn Dellaert
Atmos. Chem. Phys., 24, 4635–4649, https://doi.org/10.5194/acp-24-4635-2024, https://doi.org/10.5194/acp-24-4635-2024, 2024
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We have estimated the carbon monixide (CO) European emissions from satellite observations of the MOPITT instrument at the relatively high resolution of 0.5° for a period of over 10 years from 2011 to 2021. The analysis of the inversion results reveals the challenges associated with the inversion of CO emissions at the regional scale over Europe.
Amy Christiansen, Loretta J. Mickley, and Lu Hu
Atmos. Chem. Phys., 24, 4569–4589, https://doi.org/10.5194/acp-24-4569-2024, https://doi.org/10.5194/acp-24-4569-2024, 2024
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In this work, we provide an additional constraint on emissions and trends of nitrogen oxides using nitrate wet deposition (NWD) fluxes over the United States and Europe from 1980–2020. We find that NWD measurements constrain total NOx emissions well. We also find evidence of NOx emission overestimates in both domains, but especially over Europe, where NOx emissions are overestimated by a factor of 2. Reducing NOx emissions over Europe improves model representation of ozone at the surface.
Kiyeon Kim, Kyung Man Han, Chul Han Song, Hyojun Lee, Ross Beardsley, Jinhyeok Yu, Greg Yarwood, Bonyoung Koo, Jasper Madalipay, Jung-Hun Woo, and Seogju Cho
EGUsphere, https://doi.org/10.5194/egusphere-2024-886, https://doi.org/10.5194/egusphere-2024-886, 2024
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We incoporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratios predictions. These results expand our understanding of HONO photochemistry and identify crucial sources of HONO that impact the total HONO budget in Seoul, South Korea. Through this investigation, we contribute to resolving discrepancies in understading chemical transport models, with implications for better air quality mangement and environmental protection in the region.
Eduardo Torre-Pascual, Gotzon Gangoiti, Ana Rodríguez-García, Estibaliz Sáez de Cámara, Joana Ferreira, Carla Gama, María Carmen Gómez, Iñaki Zuazo, Jose Antonio García, and Maite de Blas
Atmos. Chem. Phys., 24, 4305–4329, https://doi.org/10.5194/acp-24-4305-2024, https://doi.org/10.5194/acp-24-4305-2024, 2024
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We present an analysis of an intense air pollution episode of tropospheric ozone (O3) along the Atlantic coast of the Iberian Peninsula, incorporating both measured and simulated parameters. Our study extends beyond surface-level factors to include altitude-related parameters. These episodes stem from upper-atmosphere O3 accumulation in preceding days, transported to surface layers, causing rapid O3 concentration increase.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyong Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
EGUsphere, https://doi.org/10.5194/egusphere-2024-811, https://doi.org/10.5194/egusphere-2024-811, 2024
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We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show, that SF6 emissions are decreasing in the USA and Europe, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, Europe, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
Hannah Chawner, Eric Saboya, Karina E. Adcock, Tim Arnold, Yuri Artioli, Caroline Dylag, Grant L. Forster, Anita Ganesan, Heather Graven, Gennadi Lessin, Peter Levy, Ingrid T. Luijkx, Alistair Manning, Penelope A. Pickers, Chris Rennick, Christian Rödenbeck, and Matthew Rigby
Atmos. Chem. Phys., 24, 4231–4252, https://doi.org/10.5194/acp-24-4231-2024, https://doi.org/10.5194/acp-24-4231-2024, 2024
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The quantity of atmospheric potential oxygen (APO), derived from coincident measurements of carbon dioxide (CO2) and oxygen (O2), has been proposed as a tracer for fossil fuel CO2 emissions. In this model sensitivity study, we examine the use of APO for this purpose in the UK and compare our model to observations. We find that our model simulations are most sensitive to uncertainties relating to ocean fluxes and boundary conditions.
Meng Li, Junichi Kurokawa, Qiang Zhang, Jung-Hun Woo, Tazuko Morikawa, Satoru Chatani, Zifeng Lu, Yu Song, Guannan Geng, Hanwen Hu, Jinseok Kim, Owen R. Cooper, and Brian C. McDonald
Atmos. Chem. Phys., 24, 3925–3952, https://doi.org/10.5194/acp-24-3925-2024, https://doi.org/10.5194/acp-24-3925-2024, 2024
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In this work, we developed MIXv2, a mosaic Asian emission inventory for 2010–2017. With high spatial (0.1°) and monthly temporal resolution, MIXv2 integrates anthropogenic and open biomass burning emissions across seven sectors following a mosaic methodology. It provides CO2 emissions data alongside nine key pollutants and three chemical mechanisms. Our publicly accessible gridded monthly emissions data can facilitate long-term atmospheric and climate model analyses.
Lauri Johannes Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Christian Kurtén
EGUsphere, https://doi.org/10.5194/egusphere-2024-920, https://doi.org/10.5194/egusphere-2024-920, 2024
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions, and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we are qualitatively investigating a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discovering which of these reactions are most atmospherically important.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
EGUsphere, https://doi.org/10.5194/egusphere-2024-715, https://doi.org/10.5194/egusphere-2024-715, 2024
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This work uses WRF-Chem and chemical box modeling to study the gas and aqueous phase production of organic acid concentrations measured in cloud water the summit of Whiteface Mountain on July 1st, 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Xiaomeng Zhang, Yongjian Lian, Shendong Tan, and Shi Yin
Atmos. Chem. Phys., 24, 3593–3612, https://doi.org/10.5194/acp-24-3593-2024, https://doi.org/10.5194/acp-24-3593-2024, 2024
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Atmospheric new particle formation (NPF) has a significant influence on the global climate, local air quality and human health. Using a combination of quantum chemical calculations and kinetics modeling, we find that thhe gas-phase organosulfate produced from consumption of SO3 can significantly enhance SA–DMA nucleation in the polluted boundary layer, resulting in non-negligible contributions to NPF. Our findings provide important insights into organic sulfur in atmospheric aerosol formation.
Yasin Elshorbany, Jerald Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca Buchholz, Benjamin Gaubert, Néstor Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
EGUsphere, https://doi.org/10.5194/egusphere-2024-720, https://doi.org/10.5194/egusphere-2024-720, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the Tropospheric Column of Ozone and its precursors, nitrogen dioxide, formaldehyde, and total column of CO as well as ozonesonde data and model simulations.
Linia Tashmim, William C. Porter, Qianjie Chen, Becky Alexander, Charles H. Fite, Christopher D. Holmes, Jeffrey R. Pierce, Betty Croft, and Sakiko Ishino
Atmos. Chem. Phys., 24, 3379–3403, https://doi.org/10.5194/acp-24-3379-2024, https://doi.org/10.5194/acp-24-3379-2024, 2024
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Dimethyl sulfide (DMS) is mostly emitted from ocean surfaces and represents the largest natural source of sulfur for the atmosphere. Once in the atmosphere, DMS forms stable oxidation products such as SO2 and H2SO4, which can subsequently contribute to airborne particle formation and growth. In this study, we update the DMS oxidation mechanism in the chemical transport model GEOS-Chem and describe resulting changes in particle growth as well as the overall global sulfur budget.
Tia Scarpelli, Paul Palmer, Mark Lunt, Ingrid Super, and Arjan Droste
EGUsphere, https://doi.org/10.5194/egusphere-2024-416, https://doi.org/10.5194/egusphere-2024-416, 2024
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Under the Paris Agreement, countries must track their anthropogenic greenhouse gas emissions. This study describes a method to determine self-consistent estimates for combustion emissions and natural fluxes of CO2 from atmospheric data We report consistent estimates inferred using this approach from satellite data and ground-based data over Europe, suggesting that satellite data can be used to determine national anthropogenic CO2 emissions for countries where ground-based CO2 data are absent.
Nan Wang, Yunsong Du, Dongyang Chen, Haiyan Meng, Xi Chen, Li Zhou, Guangming Shi, Yu Zhan, Miao Feng, Wei Li, Mulan Chen, Zhenliang Li, and Fumo Yang
Atmos. Chem. Phys., 24, 3029–3042, https://doi.org/10.5194/acp-24-3029-2024, https://doi.org/10.5194/acp-24-3029-2024, 2024
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In the scorching August 2022 heatwave, China's Sichuan Basin saw a stark contrast in ozone (O3) levels between Chengdu and Chongqing. The regional disparities were studied considering meteorology, precursors, photochemistry, and transportation. The study highlighted the importance of tailored pollution control measures and underlined the necessity for region-specific strategies to combat O3 pollution on a regional scale.
Sebastian D. Eastham, Guillaume P. Chossière, Raymond L. Speth, Daniel J. Jacob, and Steven R. H. Barrett
Atmos. Chem. Phys., 24, 2687–2703, https://doi.org/10.5194/acp-24-2687-2024, https://doi.org/10.5194/acp-24-2687-2024, 2024
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Emissions from aircraft are known to cause air quality impacts worldwide, but the scale and mechanisms of this impact are not well understood. This work uses high-resolution computational modeling of the atmosphere to show that air pollution changes from aviation are mostly the result of emissions during cruise (high-altitude) operations, that these impacts are related to how much non-aviation pollution is present, and that prior regional assessments have underestimated these impacts.
Jean-François Müller, Trissevgeni Stavrakou, Glenn-Michael Oomen, Beata Opacka, Isabelle De Smedt, Alex Guenther, Corinne Vigouroux, Bavo Langerock, Carlos Augusto Bauer Aquino, Michel Grutter, James Hannigan, Frank Hase, Rigel Kivi, Erik Lutsch, Emmanuel Mahieu, Maria Makarova, Jean-Marc Metzger, Isamu Morino, Isao Murata, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Amelie Röhling, Wolfgang Stremme, Kimberly Strong, Ralf Sussmann, Yao Té, and Alan Fried
Atmos. Chem. Phys., 24, 2207–2237, https://doi.org/10.5194/acp-24-2207-2024, https://doi.org/10.5194/acp-24-2207-2024, 2024
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Formaldehyde observations from satellites can be used to constrain the emissions of volatile organic compounds, but those observations have biases. Using an atmospheric model, aircraft and ground-based remote sensing data, we quantify these biases, propose a correction to the data, and assess the consequence of this correction for the evaluation of emissions.
Joël Thanwerdas, Marielle Saunois, Antoine Berchet, Isabelle Pison, and Philippe Bousquet
Atmos. Chem. Phys., 24, 2129–2167, https://doi.org/10.5194/acp-24-2129-2024, https://doi.org/10.5194/acp-24-2129-2024, 2024
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We investigate the causes of the renewed growth of atmospheric methane (CH4) after 2007 using inverse modeling. We use the additional information provided by observations of CH4 isotopic compositions to better differentiate between the emission categories. Accounting for the large uncertainties in source signatures, our results suggest that the post-2007 increase in atmospheric CH4 was caused by similar increases in emissions from (1) fossil fuels and (2) agriculture and waste.
Heather Simon, Christian Hogrefe, Andrew Whitehill, Kristen M. Foley, Jennifer Liljegren, Norm Possiel, Benjamin Wells, Barron H. Henderson, Lukas C. Valin, Gail Tonnesen, K. Wyat Appel, and Shannon Koplitz
Atmos. Chem. Phys., 24, 1855–1871, https://doi.org/10.5194/acp-24-1855-2024, https://doi.org/10.5194/acp-24-1855-2024, 2024
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We assess observed and modeled ozone weekend–weekday differences in the USA from 2002–2019. A subset of urban areas that were NOx-saturated at the beginning of the period transitioned to NOx-limited conditions. Multiple rural areas of California were NOx-limited for the entire period but become less influenced by local day-of-week emission patterns in more recent years. The model produces more NOx-saturated conditions than the observations but captures trends in weekend–weekday ozone patterns.
Mariano Mertens, Sabine Brinkop, Phoebe Graf, Volker Grewe, Johannes Hendricks, Patrick Jöckel, Anna Lanteri, Sigrun Matthes, Vanessa S. Rieger, Mattia Righi, and Robin N. Thor
EGUsphere, https://doi.org/10.5194/egusphere-2024-324, https://doi.org/10.5194/egusphere-2024-324, 2024
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We quantified the contributions of land transport, shipping and aviation emissions to tropospheric ozone and the reductions of the methane lifetime using chemistry-climate model simulations. The contributions were analysed for the conditions of 2015 and for three projections for the year 2050. The results highllight the challenges of mitigating ozone formed by emissions of the transport sector, caused by the non-linearitiy of the ozone chemistry and the long life-time.
Flossie Brown, Gerd Folberth, Stephen Sitch, Paulo Artaxo, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Matteo Detto, Ninong Komala, Luciana Rizzo, Nestor Rojas, Ines dos Santos Vieira, Steven Turnock, Hans Verbeeck, and Alfonso Zambrano
EGUsphere, https://doi.org/10.5194/egusphere-2023-2937, https://doi.org/10.5194/egusphere-2023-2937, 2024
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Ozone is a pollutant that is detrimental to human and plant health. Ozone monitoring sites in the tropics are limited, so models are often used to assess ozone exposure. We use measurements from the tropics to evaluate ozone from the UK Earth system model, UKESM1. UKESM1 is able to capture the behaviour of ozone in the tropics, except in Southeast Asia. Results demonstrate that UKESM1 can be used for health assessments and highlights areas that would benefit from further observations.