Articles | Volume 19, issue 5
https://doi.org/10.5194/acp-19-3161-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-19-3161-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
12 Mar 2019
Research article |
| 12 Mar 2019
| 12 Mar 2019
Importance of reactive halogens in the tropical marine atmosphere: a regional modelling study using WRF-Chem
Centre for Ocean and Atmospheric Sciences, School of Environmental Sciences, University of East Anglia, Norwich, UK
now at: Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, CSIC, Madrid, Spain
Claire E. Reeves
Centre for Ocean and Atmospheric Sciences, School of Environmental Sciences, University of East Anglia, Norwich, UK
Alex R. Baker
Centre for Ocean and Atmospheric Sciences, School of Environmental Sciences, University of East Anglia, Norwich, UK
Alfonso Saiz-Lopez
Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, CSIC, Madrid, Spain
Rainer Volkamer
Department of Chemistry, University of Colorado, Boulder, CO, USA
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, CO, USA
Theodore K. Koenig
Department of Chemistry, University of Colorado, Boulder, CO, USA
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, CO, USA
Eric C. Apel
Earth System Laboratory, Atmospheric Chemistry Division, National Center for Atmospheric Research (NCAR), Boulder, CO, USA
Rebecca S. Hornbrook
Earth System Laboratory, Atmospheric Chemistry Division, National Center for Atmospheric Research (NCAR), Boulder, CO, USA
Lucy J. Carpenter
Wolfson Atmospheric Chemistry Laboratories (WACL), Department of Chemistry, University of York, York, UK
Stephen J. Andrews
Wolfson Atmospheric Chemistry Laboratories (WACL), Department of Chemistry, University of York, York, UK
Tomás Sherwen
Wolfson Atmospheric Chemistry Laboratories (WACL), Department of Chemistry, University of York, York, UK
National Centre for Atmospheric Science (NCAS), Department of Chemistry, University of York, York, UK
Roland von Glasow
Centre for Ocean and Atmospheric Sciences, School of Environmental Sciences, University of East Anglia, Norwich, UK
deceased, 6 September 2015
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Simone T. Andersen, Max R. McGillen, Chaoyang Xue, Tobias Seubert, Patrick Dewald, Gunther N. T. E. Türk, Jan Schuladen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Abdelwahid Mellouki, Lucy J. Carpenter, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 11603–11618, https://doi.org/10.5194/acp-24-11603-2024, https://doi.org/10.5194/acp-24-11603-2024, 2024
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Theodore K. Koenig, François Hendrick, Douglas Kinnison, Christopher F. Lee, Michel Van Roozendael, and Rainer Volkamer
Atmos. Meas. Tech., 17, 5911–5934, https://doi.org/10.5194/amt-17-5911-2024, https://doi.org/10.5194/amt-17-5911-2024, 2024
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Randall Chiu, Florian Obersteiner, Alessandro Franchin, Teresa Campos, Adriana Bailey, Christopher Webster, Andreas Zahn, and Rainer Volkamer
Atmos. Meas. Tech., 17, 5731–5746, https://doi.org/10.5194/amt-17-5731-2024, https://doi.org/10.5194/amt-17-5731-2024, 2024
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Da Yang, Emmanuel Assaf, Roy Mauldin, Suresh Dhaniyala, and Rainer Volkamer
EGUsphere, https://doi.org/10.5194/egusphere-2024-2390, https://doi.org/10.5194/egusphere-2024-2390, 2024
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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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Eleanor J. Derry, Tyler R. Elgiar, Taylor Y. Wilmot, Nicholas W. Hoch, Noah S. Hirshorn, Peter Weiss-Penzias, Christopher F. Lee, John C. Lin, A. Gannet Hallar, Rainer Volkamer, Seth N. Lyman, and Lynne E. Gratz
Atmos. Chem. Phys., 24, 9615–9643, https://doi.org/10.5194/acp-24-9615-2024, https://doi.org/10.5194/acp-24-9615-2024, 2024
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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.
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.
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).
Lucy V. Brown, Ryan J. Pound, Lyndsay S. Ives, Matthew R. Jones, Stephen J. Andrews, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 3905–3923, https://doi.org/10.5194/acp-24-3905-2024, https://doi.org/10.5194/acp-24-3905-2024, 2024
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Ozone is deposited from the lower atmosphere to the surface of the ocean; however, the chemical reactions which drive this deposition are currently not well understood. Of particular importance is the reaction between ozone and iodide, and this work measures the kinetics of this reaction and its temperature dependence, which we find to be negligible. We then investigate the subsequent emissions of iodine-containing species from the surface ocean, which can further impact ozone.
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.
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.
Huisheng Bian, Mian Chin, Peter R. Colarco, Eric C. Apel, Donald R. Blake, Karl Froyd, Rebecca S. Hornbrook, Jose Jimenez, Pedro Campuzano Jost, Michael Lawler, Mingxu Liu, Marianne Tronstad Lund, Hitoshi Matsui, Benjamin A. Nault, Joyce E. Penner, Andrew W. Rollins, Gregory Schill, Ragnhild B. Skeie, Hailong Wang, Lu Xu, Kai Zhang, and Jialei Zhu
Atmos. Chem. Phys., 24, 1717–1741, https://doi.org/10.5194/acp-24-1717-2024, https://doi.org/10.5194/acp-24-1717-2024, 2024
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This work studies sulfur in the remote troposphere at global and seasonal scales using aircraft measurements and multi-model simulations. The goal is to understand the sulfur cycle over remote oceans, spread of model simulations, and observation–model discrepancies. Such an understanding and comparison with real observations are crucial to narrow down the uncertainties in model sulfur simulations and improve understanding of the sulfur cycle in atmospheric air quality, climate, and ecosystems.
Matthew M. Coggon, Chelsea E. Stockwell, Megan S. Claflin, Eva Y. Pfannerstill, Lu Xu, Jessica B. Gilman, Julia Marcantonio, Cong Cao, Kelvin Bates, Georgios I. Gkatzelis, Aaron Lamplugh, Erin F. Katz, Caleb Arata, Eric C. Apel, Rebecca S. Hornbrook, Felix Piel, Francesca Majluf, Donald R. Blake, Armin Wisthaler, Manjula Canagaratna, Brian M. Lerner, Allen H. Goldstein, John E. Mak, and Carsten Warneke
Atmos. Meas. Tech., 17, 801–825, https://doi.org/10.5194/amt-17-801-2024, https://doi.org/10.5194/amt-17-801-2024, 2024
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Mass spectrometry is a tool commonly used to measure air pollutants. This study evaluates measurement artifacts produced in the proton-transfer-reaction mass spectrometer. We provide methods to correct these biases and better measure compounds that degrade air quality.
Magdalena Pühl, Anke Roiger, Alina Fiehn, Alan M. Gorchov Negron, Eric A. Kort, Stefan Schwietzke, Ignacio Pisso, Amy Foulds, James Lee, James L. France, Anna E. Jones, Dave Lowry, Rebecca E. Fisher, Langwen Huang, Jacob Shaw, Prudence Bateson, Stephen Andrews, Stuart Young, Pamela Dominutti, Tom Lachlan-Cope, Alexandra Weiss, and Grant Allen
Atmos. Chem. Phys., 24, 1005–1024, https://doi.org/10.5194/acp-24-1005-2024, https://doi.org/10.5194/acp-24-1005-2024, 2024
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In April–May 2019 we carried out an airborne field campaign in the southern North Sea with the aim of studying methane emissions of offshore gas installations. We determined methane emissions from elevated methane measured downstream of the sampled installations. We compare our measured methane emissions with estimated methane emissions from national and global annual inventories. As a result, we find inconsistencies of inventories and large discrepancies between measurements and inventories.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
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This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
Robert Woodward-Massey, Roberto Sommariva, Lisa K. Whalley, Danny R. Cryer, Trevor Ingham, William J. Bloss, Stephen M. Ball, Sam Cox, James D. Lee, Chris P. Reed, Leigh R. Crilley, Louisa J. Kramer, Brian J. Bandy, Grant L. Forster, Claire E. Reeves, Paul S. Monks, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 14393–14424, https://doi.org/10.5194/acp-23-14393-2023, https://doi.org/10.5194/acp-23-14393-2023, 2023
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Measurements of OH, HO2 and RO2 radicals and also OH reactivity were made at a UK coastal site and compared to calculations from a constrained box model utilising the Master Chemical Mechanism. The model agreement displayed a strong dependence on the NO concentration. An experimental budget analysis for OH, HO2, RO2 and total ROx demonstrated significant imbalances between HO2 and RO2 production rates. Ozone production rates were calculated from measured radicals and compared to modelled values.
Ioannis Cheliotis, Thomas Lauvaux, Jinghui Lian, Theodoros Christoudias, George Georgiou, Alba Badia, Frédéric Chevallier, Pramod Kumar, Yathin Kudupaje, Ruixue Lei, and Philippe Ciais
EGUsphere, https://doi.org/10.5194/egusphere-2023-2487, https://doi.org/10.5194/egusphere-2023-2487, 2023
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A consistent estimation of CO2 emissions is complicated due to the scarcity of CO2 observations. In this study, we showcase the potential to improve the CO2 emissions estimations from the NO2 concentrations based on the NO2-to-CO2 ratio, which should be constant for a source co-emitting NO2 and CO2, by comparing satellite observations with atmospheric chemistry and transport model simulations for NO2 and CO2. Furthermore, we demonstrate the significance of the chemistry in NO2 simulations.
Alba Badia, Veronica Vidal, Sergi Ventura, Roger Curcoll, Ricard Segura, and Gara Villalba
Atmos. Chem. Phys., 23, 10751–10774, https://doi.org/10.5194/acp-23-10751-2023, https://doi.org/10.5194/acp-23-10751-2023, 2023
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Improving air quality is a top priority in urban areas. In this study, we used an air quality model to analyse the air quality changes occurring over the metropolitan area of Barcelona and other rural areas affected by transport of the atmospheric plume from the city during mobility restrictions. Our results show that mitigation strategies intended to reduce O3 should be designed according to the local meteorology, air transport, and particular ozone chemistry of the urban area.
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.
Lixu Jin, Wade Permar, Vanessa Selimovic, Damien Ketcherside, Robert J. Yokelson, Rebecca S. Hornbrook, Eric C. Apel, I-Ting Ku, Jeffrey L. Collett Jr., Amy P. Sullivan, Daniel A. Jaffe, Jeffrey R. Pierce, Alan Fried, Matthew M. Coggon, Georgios I. Gkatzelis, Carsten Warneke, Emily V. Fischer, and Lu Hu
Atmos. Chem. Phys., 23, 5969–5991, https://doi.org/10.5194/acp-23-5969-2023, https://doi.org/10.5194/acp-23-5969-2023, 2023
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Air quality in the USA has been improving since 1970 due to anthropogenic emission reduction. Those gains have been partly offset by increased wildfire pollution in the western USA in the past 20 years. Still, we do not understand wildfire emissions well due to limited measurements. Here, we used a global transport model to evaluate and constrain current knowledge of wildfire emissions with recent observational constraints, showing the underestimation of wildfire emissions in the western USA.
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.
John W. Halfacre, Jordan Stewart, Scott C. Herndon, Joseph R. Roscioli, Christoph Dyroff, Tara I. Yacovitch, Michael Flynn, Stephen J. Andrews, Steven S. Brown, Patrick R. Veres, and Pete M. Edwards
Atmos. Meas. Tech., 16, 1407–1429, https://doi.org/10.5194/amt-16-1407-2023, https://doi.org/10.5194/amt-16-1407-2023, 2023
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This study details a new sampling method for the optical detection of hydrogen chloride (HCl). HCl is an important atmospheric reservoir for chlorine atoms, which can affect nitrogen oxide cycling and the lifetimes of volatile organic compounds and ozone. However, HCl has a high affinity for interacting with surfaces, thereby preventing fast, quantitative measurements. The sampling technique in this study minimizes these surface interactions and provides a high-quality measurement of HCl.
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.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
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.
Johana Romero-Alvarez, Aurelia Lupaşcu, Douglas Lowe, Alba Badia, Scott Archer-Nicholls, Steve Dorling, Claire E. Reeves, and Tim Butler
Atmos. Chem. Phys., 22, 13797–13815, https://doi.org/10.5194/acp-22-13797-2022, https://doi.org/10.5194/acp-22-13797-2022, 2022
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As ozone can be transported across countries, efficient air quality management and regulatory policies rely on the assessment of local ozone production vs. transport. In our study, we investigate the origin of surface ozone in the UK and the contribution of the different source regions to regulatory ozone metrics. It is shown that emission controls would be necessary over western Europe to improve health-related metrics and over larger areas to reduce impacts on ecosystems.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111, https://doi.org/10.5194/acp-22-12093-2022, https://doi.org/10.5194/acp-22-12093-2022, 2022
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Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
Shang Liu, Barbara Barletta, Rebecca S. Hornbrook, Alan Fried, Jeff Peischl, Simone Meinardi, Matthew Coggon, Aaron Lamplugh, Jessica B. Gilman, Georgios I. Gkatzelis, Carsten Warneke, Eric C. Apel, Alan J. Hills, Ilann Bourgeois, James Walega, Petter Weibring, Dirk Richter, Toshihiro Kuwayama, Michael FitzGibbon, and Donald Blake
Atmos. Chem. Phys., 22, 10937–10954, https://doi.org/10.5194/acp-22-10937-2022, https://doi.org/10.5194/acp-22-10937-2022, 2022
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California’s ozone persistently exceeds the air quality standards. We studied the spatial distribution of volatile organic compounds (VOCs) that produce ozone over the most polluted regions in California using aircraft measurements. We find that the oxygenated VOCs have the highest ozone formation potential. Spatially, biogenic VOCs are important during high ozone episodes in the South Coast Air Basin, while dairy emissions may be critical for ozone production in San Joaquin Valley.
Tianlang Zhao, Jingqiu Mao, William R. Simpson, Isabelle De Smedt, Lei Zhu, Thomas F. Hanisco, Glenn M. Wolfe, Jason M. St. Clair, Gonzalo González Abad, Caroline R. Nowlan, Barbara Barletta, Simone Meinardi, Donald R. Blake, Eric C. Apel, and Rebecca S. Hornbrook
Atmos. Chem. Phys., 22, 7163–7178, https://doi.org/10.5194/acp-22-7163-2022, https://doi.org/10.5194/acp-22-7163-2022, 2022
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Monitoring formaldehyde (HCHO) can help us understand Arctic vegetation change. Here, we compare satellite data and model and show that Alaska summertime HCHO is largely dominated by a background from methane oxidation during mild wildfire years and is dominated by wildfire (largely from direct emission of fire) during strong fire years. Consequently, it is challenging to use satellite HCHO to study vegetation change in the Arctic region.
Taku Umezawa, Satoshi Sugawara, Kenji Kawamura, Ikumi Oyabu, Stephen J. Andrews, Takuya Saito, Shuji Aoki, and Takakiyo Nakazawa
Atmos. Chem. Phys., 22, 6899–6917, https://doi.org/10.5194/acp-22-6899-2022, https://doi.org/10.5194/acp-22-6899-2022, 2022
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Greenhouse gas methane in the Arctic atmosphere has not been accurately reported for 1900–1980 from either direct observations or ice core reconstructions. By using trace gas data from firn (compacted snow layers above ice sheet), air samples at two Greenland sites, and a firn air transport model, this study suggests a likely range of the Arctic methane reconstruction for the 20th century. Atmospheric scenarios from two previous studies are also evaluated for consistency with the firn data sets.
Hannah Walker, Daniel Stone, Trevor Ingham, Sina Hackenberg, Danny Cryer, Shalini Punjabi, Katie Read, James Lee, Lisa Whalley, Dominick V. Spracklen, Lucy J. Carpenter, Steve R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 22, 5535–5557, https://doi.org/10.5194/acp-22-5535-2022, https://doi.org/10.5194/acp-22-5535-2022, 2022
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Glyoxal is a ubiquitous reactive organic compound in the atmosphere, which may form organic aerosol and impact the atmosphere's oxidising capacity. There are limited measurements of glyoxal's abundance in the remote marine atmosphere. We made new measurements of glyoxal using a highly sensitive technique over two 4-week periods in the tropical Atlantic atmosphere. We show that daytime measurements are mostly consistent with our chemical understanding but a potential missing source at night.
Robert Woodward-Massey, Roberto Sommariva, Lisa K. Whalley, Danny R. Cryer, Trevor Ingham, William J1 Bloss, Sam Cox, James D. Lee, Chris P. Reed, Leigh R. Crilley, Louisa J. Kramer, Brian J. Bandy, Grant L. Forster, Claire E. Reeves, Paul S. Monks, and Dwayne E. Heard
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-207, https://doi.org/10.5194/acp-2022-207, 2022
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We measured radicals (OH, HO2, RO2) and OH reactivity at a UK coastal site and compared our observations to the predictions of an MCMv3.3.1 box model. We find variable agreement between measured and modelled radical concentrations and OH reactivity, where the levels of agreement for individual species display strong dependences on NO concentrations. The most substantial disagreement is found for RO2 at high NO (> 1 ppbv), when RO2 levels are underpredicted by a factor of ~10–30.
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.
Ka Ming Fung, Colette L. Heald, Jesse H. Kroll, Siyuan Wang, Duseong S. Jo, Andrew Gettelman, Zheng Lu, Xiaohong Liu, Rahul A. Zaveri, Eric C. Apel, Donald R. Blake, Jose-Luis Jimenez, Pedro Campuzano-Jost, Patrick R. Veres, Timothy S. Bates, John E. Shilling, and Maria Zawadowicz
Atmos. Chem. Phys., 22, 1549–1573, https://doi.org/10.5194/acp-22-1549-2022, https://doi.org/10.5194/acp-22-1549-2022, 2022
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Understanding the natural aerosol burden in the preindustrial era is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of dimethyl sulfide (DMS) oxidation (implemented in the Community Atmospheric Model version 6 with chemistry, CAM6-chem) could help us better estimate the present-day and preindustrial concentrations of sulfate and other relevant chemicals, as well as the resulting aerosol radiative impacts.
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.
Jin Liao, Glenn M. Wolfe, Reem A. Hannun, Jason M. St. Clair, Thomas F. Hanisco, Jessica B. Gilman, Aaron Lamplugh, Vanessa Selimovic, Glenn S. Diskin, John B. Nowak, Hannah S. Halliday, Joshua P. DiGangi, Samuel R. Hall, Kirk Ullmann, Christopher D. Holmes, Charles H. Fite, Anxhelo Agastra, Thomas B. Ryerson, Jeff Peischl, Ilann Bourgeois, Carsten Warneke, Matthew M. Coggon, Georgios I. Gkatzelis, Kanako Sekimoto, Alan Fried, Dirk Richter, Petter Weibring, Eric C. Apel, Rebecca S. Hornbrook, Steven S. Brown, Caroline C. Womack, Michael A. Robinson, Rebecca A. Washenfelder, Patrick R. Veres, and J. Andrew Neuman
Atmos. Chem. Phys., 21, 18319–18331, https://doi.org/10.5194/acp-21-18319-2021, https://doi.org/10.5194/acp-21-18319-2021, 2021
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Formaldehyde (HCHO) is an important oxidant precursor and affects the formation of O3 and other secondary pollutants in wildfire plumes. We disentangle the processes controlling HCHO evolution from wildfire plumes sampled by NASA DC-8 during FIREX-AQ. We find that OH abundance rather than normalized OH reactivity is the main driver of fire-to-fire variability in HCHO secondary production and estimate an effective HCHO yield per volatile organic compound molecule oxidized in wildfire plumes.
Leigh R. Crilley, Louisa J. Kramer, Francis D. Pope, Chris Reed, James D. Lee, Lucy J. Carpenter, Lloyd D. J. Hollis, Stephen M. Ball, and William J. Bloss
Atmos. Chem. Phys., 21, 18213–18225, https://doi.org/10.5194/acp-21-18213-2021, https://doi.org/10.5194/acp-21-18213-2021, 2021
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Nitrous acid (HONO) is a key source of atmospheric oxidants. We evaluate if the ocean surface is a source of HONO for the marine boundary layer, using measurements from two contrasting coastal locations. We observed no evidence for a night-time ocean surface source, in contrast to previous work. This points to significant geographical variation in the predominant HONO formation mechanisms in marine environments, reflecting possible variability in the sea-surface microlayer composition.
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.
Wedad Alahamade, Iain Lake, Claire E. Reeves, and Beatriz De La Iglesia
Geosci. Instrum. Method. Data Syst., 10, 265–285, https://doi.org/10.5194/gi-10-265-2021, https://doi.org/10.5194/gi-10-265-2021, 2021
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The goal is to reduce the uncertainty in air quality assessment by imputing all missing pollutants in monitoring stations and identify where more measurements can be beneficial. The proposed approach is based on spatial or temporal similarity between stations. Our proposed approach enables us to impute and estimate plausible concentrations of multiple pollutants at stations across the UK, and the modelled concentrations from the selected models correlated well with the observed concentrations.
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.
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 %.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Alex R. Baker and Chan Yodle
Atmos. Chem. Phys., 21, 13067–13076, https://doi.org/10.5194/acp-21-13067-2021, https://doi.org/10.5194/acp-21-13067-2021, 2021
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Iodine is emitted from the ocean and helps to destroy ozone in the lower atmosphere before being taken up into aerosol particles. We measured the chemical forms of iodine in aerosols over the Atlantic Ocean, because some of these forms can return to the gas phase and destroy more ozone. Our results indicate that aerosol acidity exerts a strong control on iodine speciation and therefore on its recycling behaviour and impact on ozone concentrations.
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.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke D. Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul A. Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 11113–11132, https://doi.org/10.5194/acp-21-11113-2021, https://doi.org/10.5194/acp-21-11113-2021, 2021
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected nearly from pole to pole over the oceans during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigated their impact on the variability of tropospheric N2O.
Daniel P. Phillips, Frances E. Hopkins, Thomas G. Bell, Peter S. Liss, Philip D. Nightingale, Claire E. Reeves, Charel Wohl, and Mingxi Yang
Atmos. Chem. Phys., 21, 10111–10132, https://doi.org/10.5194/acp-21-10111-2021, https://doi.org/10.5194/acp-21-10111-2021, 2021
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We present the first measurements of the rate of transfer (flux) of three gases between the atmosphere and the ocean, using a direct flux measurement technique, at a coastal site. We show greater atmospheric loss of acetone and acetaldehyde into the ocean than estimated by global models for the open water; importantly, the acetaldehyde transfer direction is opposite to the model estimates. Measured dimethylsulfide fluxes agreed with a recent model. Isoprene fluxes were too weak to be measured.
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.
Claire E. Reeves, Graham P. Mills, Lisa K. Whalley, W. Joe F. Acton, William J. Bloss, Leigh R. Crilley, Sue Grimmond, Dwayne E. Heard, C. Nicholas Hewitt, James R. Hopkins, Simone Kotthaus, Louisa J. Kramer, Roderic L. Jones, James D. Lee, Yanhui Liu, Bin Ouyang, Eloise Slater, Freya Squires, Xinming Wang, Robert Woodward-Massey, and Chunxiang Ye
Atmos. Chem. Phys., 21, 6315–6330, https://doi.org/10.5194/acp-21-6315-2021, https://doi.org/10.5194/acp-21-6315-2021, 2021
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The impact of isoprene on atmospheric chemistry is dependent on how its oxidation products interact with other pollutants, specifically nitrogen oxides. Such interactions can lead to isoprene nitrates. We made measurements of the concentrations of individual isoprene nitrate isomers in Beijing and used a model to test current understanding of their chemistry. We highlight areas of uncertainty in understanding, in particular the chemistry following oxidation of isoprene by the nitrate radical.
Simone T. Andersen, Lucy J. Carpenter, Beth S. Nelson, Luis Neves, Katie A. Read, Chris Reed, Martyn Ward, Matthew J. Rowlinson, and James D. Lee
Atmos. Meas. Tech., 14, 3071–3085, https://doi.org/10.5194/amt-14-3071-2021, https://doi.org/10.5194/amt-14-3071-2021, 2021
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NOx has been measured in remote marine air via chemiluminescence detection using two different methods for NO2 to NO photolytic conversion: (a) internal diodes and a reaction chamber made of Teflon-like barium-doped material, which causes a NO2 artefact, and (b) external diodes and a quartz photolysis cell. Once corrections are made for the artefact of (a), the two converters are shown to give comparable NO2 mixing ratios, giving confidence in the quantitative measurement of NOx at low levels.
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.
Shona E. Wilde, Pamela A. Dominutti, Grant Allen, Stephen J. Andrews, Prudence Bateson, Stephane J.-B. Bauguitte, Ralph R. Burton, Ioana Colfescu, James France, James R. Hopkins, Langwen Huang, Anna E. Jones, Tom Lachlan-Cope, James D. Lee, Alastair C. Lewis, Stephen D. Mobbs, Alexandra Weiss, Stuart Young, and Ruth M. Purvis
Atmos. Chem. Phys., 21, 3741–3762, https://doi.org/10.5194/acp-21-3741-2021, https://doi.org/10.5194/acp-21-3741-2021, 2021
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We use airborne measurements to evaluate the speciation of volatile organic compound (VOC) emissions from offshore oil and gas (O&G) installations in the North Sea. The composition of emissions varied across regions associated with either gas, condensate or oil extraction, demonstrating that VOC emissions are not uniform across the whole O&G sector. We compare our results to VOC source profiles in the UK emissions inventory, showing these emissions are not currently fully characterized.
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.
James L. France, Prudence Bateson, Pamela Dominutti, Grant Allen, Stephen Andrews, Stephane Bauguitte, Max Coleman, Tom Lachlan-Cope, Rebecca E. Fisher, Langwen Huang, Anna E. Jones, James Lee, David Lowry, Joseph Pitt, Ruth Purvis, John Pyle, Jacob Shaw, Nicola Warwick, Alexandra Weiss, Shona Wilde, Jonathan Witherstone, and Stuart Young
Atmos. Meas. Tech., 14, 71–88, https://doi.org/10.5194/amt-14-71-2021, https://doi.org/10.5194/amt-14-71-2021, 2021
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Measuring emission rates of methane from installations is tricky, and it is even more so when those installations are located offshore. Here, we show the aircraft set-up and demonstrate an effective methodology for surveying emissions from UK and Dutch offshore oil and gas installations. We present example data collected from two campaigns to demonstrate the challenges and solutions encountered during these surveys.
David C. Loades, Mingxi Yang, Thomas G. Bell, Adam R. Vaughan, Ryan J. Pound, Stefan Metzger, James D. Lee, and Lucy J. Carpenter
Atmos. Meas. Tech., 13, 6915–6931, https://doi.org/10.5194/amt-13-6915-2020, https://doi.org/10.5194/amt-13-6915-2020, 2020
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The loss of ozone to the sea surface was measured from the south coast of the UK and was found to be more rapid than previous observations over the open ocean. This is likely a consequence of different chemistry and biology in coastal environments. Strong winds appeared to speed up the loss of ozone. A better understanding of what influences ozone loss over the sea will lead to better model estimates of total ozone in the troposphere.
W. Joe F. Acton, Zhonghui Huang, Brian Davison, Will S. Drysdale, Pingqing Fu, Michael Hollaway, Ben Langford, James Lee, Yanhui Liu, Stefan Metzger, Neil Mullinger, Eiko Nemitz, Claire E. Reeves, Freya A. Squires, Adam R. Vaughan, Xinming Wang, Zhaoyi Wang, Oliver Wild, Qiang Zhang, Yanli Zhang, and C. Nicholas Hewitt
Atmos. Chem. Phys., 20, 15101–15125, https://doi.org/10.5194/acp-20-15101-2020, https://doi.org/10.5194/acp-20-15101-2020, 2020
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Air quality in Beijing is of concern to both policy makers and the general public. In order to address concerns about air quality it is vital that the sources of atmospheric pollutants are understood. This work presents the first top-down measurement of volatile organic compound (VOC) emissions in Beijing. These measurements are used to evaluate the emissions inventory and assess the impact of VOC emission from the city centre on atmospheric chemistry.
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.
Lei Zhu, Gonzalo González Abad, Caroline R. Nowlan, Christopher Chan Miller, Kelly Chance, Eric C. Apel, Joshua P. DiGangi, Alan Fried, Thomas F. Hanisco, Rebecca S. Hornbrook, Lu Hu, Jennifer Kaiser, Frank N. Keutsch, Wade Permar, Jason M. St. Clair, and Glenn M. Wolfe
Atmos. Chem. Phys., 20, 12329–12345, https://doi.org/10.5194/acp-20-12329-2020, https://doi.org/10.5194/acp-20-12329-2020, 2020
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We develop a validation platform for satellite HCHO retrievals using in situ observations from 12 aircraft campaigns. The platform offers an alternative way to quickly assess systematic biases in HCHO satellite products over large domains and long periods, facilitating optimization of retrieval settings and the minimization of retrieval biases. Application to the NASA operational HCHO product indicates that relative biases range from −44.5 % to +112.1 % depending on locations and seasons.
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
Short summary
Short summary
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
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Short summary
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 %.
The oceans have an impact on the composition and reactivity of the troposphere through the...
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