Articles | Volume 24, issue 14
https://doi.org/10.5194/acp-24-8317-2024
© Author(s) 2024. 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-24-8317-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
24 Jul 2024
Research article |
| 24 Jul 2024
| 24 Jul 2024
Revising VOC emissions speciation improves the simulation of global background ethane and propane
Matthew J. Rowlinson
CORRESPONDING AUTHOR
National Centre for Atmospheric Science, University of York, York, YO10 5DD, UK
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
Mat J. Evans
National Centre for Atmospheric Science, University of York, York, YO10 5DD, UK
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
Lucy J. Carpenter
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
Katie A. Read
National Centre for Atmospheric Science, University of York, York, YO10 5DD, UK
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
Shalini Punjabi
National Centre for Atmospheric Science, University of York, York, YO10 5DD, UK
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
Adedayo Adedeji
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
Luke Fakes
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
Ally Lewis
National Centre for Atmospheric Science, University of York, York, YO10 5DD, UK
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
Ben Richmond
Ricardo, Fermi Avenue, Harwell, Oxon, OX11 0QR, UK
Neil Passant
Ricardo, Fermi Avenue, Harwell, Oxon, OX11 0QR, UK
Tim Murrells
Ricardo, Fermi Avenue, Harwell, Oxon, OX11 0QR, UK
Barron Henderson
United States Environmental Protection Agency, Research Triangle Park, Durham, NC 27709, USA
Kelvin H. Bates
NOAA Chemical Sciences Laboratory, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, Boulder, CO 80305, USA
Detlev Helmig
Boulder AIR LLC, Boulder, CO 80305, USA
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HONO is key to tropospheric chemistry. Observations show high HONO concentrations in remote air, possibly explained by nitrate aerosol photolysis. We use observational data to parameterize nitrate photolysis, evaluating simulated HONO against observations from multiple sources. We show improved agreement with observed HONO, but large overestimates in NOx and O3, beyond observational constraints. This implies a large uncertainty in the NOx budget and our understanding of atmospheric chemistry.
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The first comprehensive dataset of tropospheric ozone over oceans/polar regions is presented, including 77 ship/buoy and 48 aircraft campaign observations (1977–2022, 0–5000 m altitude), supplemented by ozonesonde and surface data. Air masses isolated from land for 72+ hours are systematically selected as essentially oceanic. Among the 11 global regions, they show daytime decreases of 10–16% in the tropics, while near-zero depletions are rare, unlike in the Arctic, implying different mechanisms.
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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.
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.
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.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys., 20, 10937–10951, https://doi.org/10.5194/acp-20-10937-2020, https://doi.org/10.5194/acp-20-10937-2020, 2020
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Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
John W. Halfacre, Lewis Marden, Marvin D. Shaw, Lucy J. Carpenter, Emily Matthews, Thomas J. Bannan, Hugh Coe, Scott C. Herndon, Joseph R. Roscioli, Christoph Dyroff, Tara I. Yacovitch, Patrick R. Veres, Michael A. Robinson, Steven S. Brown, and Pete M. Edwards
Atmos. Meas. Tech., 18, 3799–3818, https://doi.org/10.5194/amt-18-3799-2025, https://doi.org/10.5194/amt-18-3799-2025, 2025
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Nitryl chloride (ClNO2) is a reservoir of chlorine atoms and nitrogen oxides, both of which play important roles in atmospheric chemistry. However, all ambient ClNO2 observations so far have been made by a single technique, mass spectrometry, which needs complex calibrations. Here, we present a laser-based method that detects ClNO2 (TD-TILDAS – thermal dissociation–tunable infrared laser direct absorption spectrometry) without the need for complicated calibrations. The results show excellent agreement between these two methods from both laboratory and ambient samples.
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Organic aerosols consist of complex chemical mixtures that are challenging to characterize using chemical ionization mass spectrometry alone. This study presents a method for coupling liquid chromatography and chemical ionization mass spectrometry for offline analysis of organic aerosols. Evaluation of the method using standards and laboratory-generated and field-collected organic aerosols showed that it can provide detailed characterization of environmentally relevant mixtures.
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HONO is key to tropospheric chemistry. Observations show high HONO concentrations in remote air, possibly explained by nitrate aerosol photolysis. We use observational data to parameterize nitrate photolysis, evaluating simulated HONO against observations from multiple sources. We show improved agreement with observed HONO, but large overestimates in NOx and O3, beyond observational constraints. This implies a large uncertainty in the NOx budget and our understanding of atmospheric chemistry.
Hendrik Fuchs, Aaron Stainsby, Florian Berg, René Dubus, Michelle Färber, Andreas Hofzumahaus, Frank Holland, Kelvin H. Bates, Steven S. Brown, Matthew M. Coggon, Glenn S. Diskin, Georgios I. Gkatzelis, Christopher M. Jernigan, Jeff Peischl, Michael A. Robinson, Andrew W. Rollins, Nell B. Schafer, Rebecca H. Schwantes, Chelsea E. Stockwell, Patrick R. Veres, Carsten Warneke, Eleanor M. Waxman, Lu Xu, Kristen Zuraski, Andreas Wahner, and Anna Novelli
Atmos. Meas. Tech., 18, 881–895, https://doi.org/10.5194/amt-18-881-2025, https://doi.org/10.5194/amt-18-881-2025, 2025
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Significant improvements have been made to the instruments used to measure OH reactivity, which is equivalent to the sum of air pollutant concentrations. Accurate and precise measurements with a high time resolution have been achieved, allowing use on aircraft, as demonstrated during flights in the USA.
Yugo Kanaya, Roberto Sommariva, Alfonso Saiz-Lopez, Andrea Mazzeo, Theodore K. Koenig, Kaori Kawana, James E. Johnson, Aurélie Colomb, Pierre Tulet, Suzie Molloy, Ian E. Galbally, Rainer Volkamer, Anoop Mahajan, John W. Halfacre, Paul B. Shepson, Julia Schmale, Hélène Angot, Byron Blomquist, Matthew D. Shupe, Detlev Helmig, Junsu Gil, Meehye Lee, Sean C. Coburn, Ivan Ortega, Gao Chen, James Lee, Kenneth C. Aikin, David D. Parrish, John S. Holloway, Thomas B. Ryerson, Ilana B. Pollack, Eric J. Williams, Brian M. Lerner, Andrew J. Weinheimer, Teresa Campos, Frank M. Flocke, J. Ryan Spackman, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Ralf M. Staebler, Amir A. Aliabadi, Wanmin Gong, Roeland Van Malderen, Anne M. Thompson, Ryan M. Stauffer, Debra E. Kollonige, Juan Carlos Gómez Martin, Masatomo Fujiwara, Katie Read, Matthew Rowlinson, Keiichi Sato, Junichi Kurokawa, Yoko Iwamoto, Fumikazu Taketani, Hisahiro Takashima, Monica Navarro Comas, Marios Panagi, and Martin G. Schultz
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Revised manuscript accepted for ESSD
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The first comprehensive dataset of tropospheric ozone over oceans/polar regions is presented, including 77 ship/buoy and 48 aircraft campaign observations (1977–2022, 0–5000 m altitude), supplemented by ozonesonde and surface data. Air masses isolated from land for 72+ hours are systematically selected as essentially oceanic. Among the 11 global regions, they show daytime decreases of 10–16% in the tropics, while near-zero depletions are rare, unlike in the Arctic, implying different mechanisms.
Diego Guizzardi, Monica Crippa, Tim Butler, Terry Keating, Rosa Wu, Jacek W. Kamiński, Jeroen Kuenen, Junichi Kurokawa, Satoru Chatani, Tazuko Morikawa, George Pouliot, Jacinthe Racine, Michael D. Moran, Zbigniew Klimont, Patrick M. Manseau, Rabab Mashayekhi, Barron H. Henderson, Steven J. Smith, Rachel Hoesly, Marilena Muntean, Manjola Banja, Edwin Schaaf, Federico Pagani, Jung-Hun Woo, Jinseok Kim, Enrico Pisoni, Junhua Zhang, David Niemi, Mourad Sassi, Annie Duhamel, Tabish Ansari, Kristen Foley, Guannan Geng, Yifei Chen, and Qiang Zhang
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-601, https://doi.org/10.5194/essd-2024-601, 2025
Preprint under review for ESSD
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The global air pollution emission mosaic HTAP_v3.1 is the state-of-the-art database for addressing the evolution of a set of policy-relevant air pollutants over the past 2 decades. The inventory is made by the harmonization and blending of seven regional inventories, gapfilled using the most recent release of EDGAR (EDGARv8). By incorporating the best available local information, the HTAP_v3.1 mosaic inventory can be used for policy-relevant studies at both regional and global levels.
Alex T. Archibald, Bablu Sinha, Maria R. Russo, Emily Matthews, Freya A. Squires, N. Luke Abraham, Stephane J.-B. Bauguitte, Thomas J. Bannan, Thomas G. Bell, David Berry, Lucy J. Carpenter, Hugh Coe, Andrew Coward, Peter Edwards, Daniel Feltham, Dwayne Heard, Jim Hopkins, James Keeble, Elizabeth C. Kent, Brian A. King, Isobel R. Lawrence, James Lee, Claire R. Macintosh, Alex Megann, Bengamin I. Moat, Katie Read, Chris Reed, Malcolm J. Roberts, Reinhard Schiemann, David Schroeder, Timothy J. Smyth, Loren Temple, Navaneeth Thamban, Lisa Whalley, Simon Williams, Huihui Wu, and Mingxi Yang
Earth Syst. Sci. Data, 17, 135–164, https://doi.org/10.5194/essd-17-135-2025, https://doi.org/10.5194/essd-17-135-2025, 2025
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Here, we present an overview of the data generated as part of the North Atlantic Climate System Integrated Study (ACSIS) programme that are available through dedicated repositories at the Centre for Environmental Data Analysis (CEDA; www.ceda.ac.uk) and the British Oceanographic Data Centre (BODC; bodc.ac.uk). The datasets described here cover the North Atlantic Ocean, the atmosphere above (it including its composition), and Arctic sea ice.
Xiansheng Liu, Xun Zhang, Marvin Dufresne, Tao Wang, Lijie Wu, Rosa Lara, Roger Seco, Marta Monge, Ana Maria Yáñez-Serrano, Marie Gohy, Paul Petit, Audrey Chevalier, Marie-Pierre Vagnot, Yann Fortier, Alexia Baudic, Véronique Ghersi, Grégory Gille, Ludovic Lanzi, Valérie Gros, Leïla Simon, Heidi Héllen, Stefan Reimann, Zoé Le Bras, Michelle Jessy Müller, David Beddows, Siqi Hou, Zongbo Shi, Roy M. Harrison, William Bloss, James Dernie, Stéphane Sauvage, Philip K. Hopke, Xiaoli Duan, Taicheng An, Alastair C. Lewis, James R. Hopkins, Eleni Liakakou, Nikolaos Mihalopoulos, Xiaohu Zhang, Andrés Alastuey, Xavier Querol, and Thérèse Salameh
Atmos. Chem. Phys., 25, 625–638, https://doi.org/10.5194/acp-25-625-2025, https://doi.org/10.5194/acp-25-625-2025, 2025
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This study examines BTEX (benzene, toluene, ethylbenzene, xylenes) pollution in urban areas across seven European countries. Analyzing data from 22 monitoring sites, we found traffic and industrial activities significantly impact BTEX levels, with peaks during rush hours. The risk from BTEX exposure remains moderate, especially in high-traffic and industrial zones, highlighting the need for targeted air quality management to protect public health and improve urban air quality.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles A. Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
Atmos. Chem. Phys., 25, 45–71, https://doi.org/10.5194/acp-25-45-2025, https://doi.org/10.5194/acp-25-45-2025, 2025
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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.
Koketso Michelle Molepo, Johannes Bieser, Alkuin Maximilian Koenig, Ian Michael Hedgecock, Ralf Ebinghaus, Aurélien Dommergue, Olivier Magand, Hélène Angot, Oleg Travnikov, Lynwill Martin, Casper Labuschagne, Katie Read, and Yann Bertrand
EGUsphere, https://doi.org/10.5194/egusphere-2024-3722, https://doi.org/10.5194/egusphere-2024-3722, 2024
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Mercury exchange between the ocean and atmosphere is poorly understood due to limited in situ data. Here, using atmospheric mercury observations from ground-based monitoring stations along with air mass trajectories, we found that atmospheric Hg levels increase with air mass ocean exposure time, matching predictions for ocean mercury emissions. This finding indicates that ocean emissions directly influence atmospheric mercury levels and enables us to estimate these emissions on a global scale.
T. Nash Skipper, Christian Hogrefe, Barron H. Henderson, Rohit Mathur, Kristen M. Foley, and Armistead G. Russell
Geosci. Model Dev., 17, 8373–8397, https://doi.org/10.5194/gmd-17-8373-2024, https://doi.org/10.5194/gmd-17-8373-2024, 2024
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Chemical transport model simulations are combined with ozone observations to estimate the bias in ozone attributable to US anthropogenic sources and individual sources of US background ozone: natural sources, non-US anthropogenic sources, and stratospheric ozone. Results indicate a positive bias correlated with US anthropogenic emissions during summer in the eastern US and a negative bias correlated with stratospheric ozone during spring.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
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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Using measurements of various trace gases in a suburban forest near Paris in the summer of 2022, we were able to gain insight into the sources and sinks of NOx (NO+NO2) with a special focus on their nighttime chemical and physical loss processes. NO was observed as a result of nighttime soil emissions when O3 levels were strongly depleted by deposition. NO oxidation products were not observed at night, indicating that soil and/or foliar surfaces are an efficient sink of reactive N.
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.
Andrew O. Langford, Raul J. Alvarez II, Kenneth C. Aikin, Sunil Baidar, W. Alan Brewer, Steven S. Brown, Matthew M. Coggan, Patrick D. Cullis, Jessica Gilman, Georgios I. Gkatzelis, Detlev Helmig, Bryan J. Johnson, K. Emma Knowland, Rajesh Kumar, Aaron D. Lamplugh, Audra McClure-Begley, Brandi J. McCarty, Ann M. Middlebrook, Gabriele Pfister, Jeff Peischl, Irina Petropavlovskikh, Pamela S. Rickley, Andrew W. Rollins, Scott P. Sandberg, Christoph J. Senff, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2024-1938, https://doi.org/10.5194/egusphere-2024-1938, 2024
Preprint withdrawn
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High ozone (O3) formed by reactions of nitrogen oxides (NOx) and volatile organic compounds (VOCs) can harm human health and welfare. High O3 is usually associated with hot summer days, but under certain conditions, high O3 can also form under winter conditions. In this study, we describe a high O3 event that occurred in Colorado during the COVID-19 quarantine that was caused in part by the decrease in traffic, and in part by a shallow inversion created by descent of stratospheric air.
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.
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.
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.
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.
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.
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.
Brandon Bottorff, Michelle M. Lew, Youngjun Woo, Pamela Rickly, Matthew D. Rollings, Benjamin Deming, Daniel C. Anderson, Ezra Wood, Hariprasad D. Alwe, Dylan B. Millet, Andrew Weinheimer, Geoff Tyndall, John Ortega, Sebastien Dusanter, Thierry Leonardis, James Flynn, Matt Erickson, Sergio Alvarez, Jean C. Rivera-Rios, Joshua D. Shutter, Frank Keutsch, Detlev Helmig, Wei Wang, Hannah M. Allen, Johnathan H. Slade, Paul B. Shepson, Steven Bertman, and Philip S. Stevens
Atmos. Chem. Phys., 23, 10287–10311, https://doi.org/10.5194/acp-23-10287-2023, https://doi.org/10.5194/acp-23-10287-2023, 2023
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The hydroxyl (OH), hydroperoxy (HO2), and organic peroxy (RO2) radicals play important roles in atmospheric chemistry and have significant air quality implications. Here, we compare measurements of OH, HO2, and total peroxy radicals (XO2) made in a remote forest in Michigan, USA, to predictions from a series of chemical models. Lower measured radical concentrations suggest that the models may be missing an important radical sink and overestimating the rate of ozone production in this forest.
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.
Monica Crippa, Diego Guizzardi, Tim Butler, Terry Keating, Rosa Wu, Jacek Kaminski, Jeroen Kuenen, Junichi Kurokawa, Satoru Chatani, Tazuko Morikawa, George Pouliot, Jacinthe Racine, Michael D. Moran, Zbigniew Klimont, Patrick M. Manseau, Rabab Mashayekhi, Barron H. Henderson, Steven J. Smith, Harrison Suchyta, Marilena Muntean, Efisio Solazzo, Manjola Banja, Edwin Schaaf, Federico Pagani, Jung-Hun Woo, Jinseok Kim, Fabio Monforti-Ferrario, Enrico Pisoni, Junhua Zhang, David Niemi, Mourad Sassi, Tabish Ansari, and Kristen Foley
Earth Syst. Sci. Data, 15, 2667–2694, https://doi.org/10.5194/essd-15-2667-2023, https://doi.org/10.5194/essd-15-2667-2023, 2023
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This study responds to the global and regional atmospheric modelling community's need for a mosaic of air pollutant emissions with global coverage, long time series, spatially distributed data at a high time resolution, and a high sectoral resolution in order to enhance the understanding of transboundary air pollution. The mosaic approach to integrating official regional emission inventories with a global inventory based on a consistent methodology ensures policy-relevant results.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
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The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Qian Shu, Sergey L. Napelenok, William T. Hutzell, Kirk R. Baker, Barron H. Henderson, Benjamin N. Murphy, and Christian Hogrefe
Geosci. Model Dev., 16, 2303–2322, https://doi.org/10.5194/gmd-16-2303-2023, https://doi.org/10.5194/gmd-16-2303-2023, 2023
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Source attribution methods are generally used to determine culpability of precursor emission sources to ambient pollutant concentrations. However, source attribution of secondarily formed pollutants such as ozone and its precursors cannot be explicitly measured, making evaluation of source apportionment methods challenging. In this study, multiple apportionment approach comparisons show common features but still reveal wide variations in predicted sector contribution and species dependency.
Laura Hyesung Yang, Daniel J. Jacob, Nadia K. Colombi, Shixian Zhai, Kelvin H. Bates, Viral Shah, Ellie Beaudry, Robert M. Yantosca, Haipeng Lin, Jared F. Brewer, Heesung Chong, Katherine R. Travis, James H. Crawford, Lok N. Lamsal, Ja-Ho Koo, and Jhoon Kim
Atmos. Chem. Phys., 23, 2465–2481, https://doi.org/10.5194/acp-23-2465-2023, https://doi.org/10.5194/acp-23-2465-2023, 2023
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A geostationary satellite can now provide hourly NO2 vertical columns, and obtaining the NO2 vertical columns from space relies on NO2 vertical distribution from the chemical transport model (CTM). In this work, we update the CTM to better represent the chemistry environment so that the CTM can accurately provide NO2 vertical distribution. We also find that the changes in NO2 vertical distribution driven by a change in mixing depth play an important role in the NO2 column's diurnal variation.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
James D. East, Barron H. Henderson, Sergey L. Napelenok, Shannon N. Koplitz, Golam Sarwar, Robert Gilliam, Allen Lenzen, Daniel Q. Tong, R. Bradley Pierce, and Fernando Garcia-Menendez
Atmos. Chem. Phys., 22, 15981–16001, https://doi.org/10.5194/acp-22-15981-2022, https://doi.org/10.5194/acp-22-15981-2022, 2022
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We present a framework that uses a computer model of air quality, along with air pollution data from satellite instruments, to estimate emissions of nitrogen oxides (NOx) across the Northern Hemisphere. The framework, which advances current methods to infer emissions from satellite observations, provides observationally constrained NOx estimates, including in regions of the world where emissions are highly uncertain, and can improve simulations of air pollutants relevant for health and policy.
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.
Vanessa Selimovic, Damien Ketcherside, Sreelekha Chaliyakunnel, Catherine Wielgasz, Wade Permar, Hélène Angot, Dylan B. Millet, Alan Fried, Detlev Helmig, and Lu Hu
Atmos. Chem. Phys., 22, 14037–14058, https://doi.org/10.5194/acp-22-14037-2022, https://doi.org/10.5194/acp-22-14037-2022, 2022
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Arctic warming has led to an increase in plants that emit gases in response to stress, but how these gases affect regional chemistry is largely unknown due to lack of observational data. Here we present the most comprehensive gas-phase measurements for this area to date and compare them to predictions from a global transport model. We report 78 gas-phase species and investigate their importance to atmospheric chemistry in the area, with broader implications for similar plant types.
Detlev Helmig, Alex Guenther, Jacques Hueber, Ryan Daly, Wei Wang, Jeong-Hoo Park, Anssi Liikanen, and Arnaud P. Praplan
Atmos. Meas. Tech., 15, 5439–5454, https://doi.org/10.5194/amt-15-5439-2022, https://doi.org/10.5194/amt-15-5439-2022, 2022
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This research demonstrates a new method for determination of the chemical reactivity of volatile organic compounds that are emitted from the leaves and needles of trees. These measurements allow elucidating if and how much of these emissions and their associated reactivity are captured and quantified by currently applicable chemical analysis methods.
Albane Barbero, Roberto Grilli, Markus M. Frey, Camille Blouzon, Detlev Helmig, Nicolas Caillon, and Joël Savarino
Atmos. Chem. Phys., 22, 12025–12054, https://doi.org/10.5194/acp-22-12025-2022, https://doi.org/10.5194/acp-22-12025-2022, 2022
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The high reactivity of the summer Antarctic boundary layer results in part from the emissions of nitrogen oxides produced during photo-denitrification of the snowpack, but its underlying mechanisms are not yet fully understood. The results of this study suggest that more NO2 is produced from the snowpack early in the photolytic season, possibly due to stronger UV irradiance caused by a smaller solar zenith angle near the solstice.
Sebastian Diez, Stuart E. Lacy, Thomas J. Bannan, Michael Flynn, Tom Gardiner, David Harrison, Nicholas Marsden, Nicholas A. Martin, Katie Read, and Pete M. Edwards
Atmos. Meas. Tech., 15, 4091–4105, https://doi.org/10.5194/amt-15-4091-2022, https://doi.org/10.5194/amt-15-4091-2022, 2022
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Regardless of the cost of the measuring instrument, there are no perfect measurements. For this reason, we compare the quality of the information provided by cheap devices when they are used to measure air pollutants and we try to emphasise that before judging the potential usefulness of the devices, the user must specify his own needs. Since commonly used performance indices/metrics can be misleading in qualifying this, we propose complementary visual analysis to the more commonly used metrics.
Marios Panagi, Roberto Sommariva, Zoë L. Fleming, Paul S. Monks, Gongda Lu, Eloise A. Marais, James R. Hopkins, Alastair C. Lewis, Qiang Zhang, James D. Lee, Freya A. Squires, Lisa K. Whalley, Eloise J. Slater, Dwayne E. Heard, Robert Woodward-Massey, Chunxiang Ye, and Joshua D. Vande Hey
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-379, https://doi.org/10.5194/acp-2022-379, 2022
Revised manuscript not accepted
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A dispersion model and a box model were combined to investigate the evolution of VOCs in Beijing once they are emitted from anthropogenic sources. It was determined that during the winter time the VOC concentrations in Beijing are driven predominantly by sources within Beijing and by a combination of transport and chemistry during the summer. Furthermore, the results in the paper highlight the need for a season specific policy.
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.
Lu Shen, Daniel J. Jacob, Mauricio Santillana, Kelvin Bates, Jiawei Zhuang, and Wei Chen
Geosci. Model Dev., 15, 1677–1687, https://doi.org/10.5194/gmd-15-1677-2022, https://doi.org/10.5194/gmd-15-1677-2022, 2022
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The high computational cost of chemical integration is a long-standing limitation in global atmospheric chemistry models. Here we present an adaptive and efficient algorithm that can reduce the computational time of atmospheric chemistry by 50 % and maintain the error below 2 % for important species, inspired by machine learning clustering techniques and traditional asymptotic analysis ideas.
Kelvin H. Bates, Guy J. P. Burke, James D. Cope, and Tran B. Nguyen
Atmos. Chem. Phys., 22, 1467–1482, https://doi.org/10.5194/acp-22-1467-2022, https://doi.org/10.5194/acp-22-1467-2022, 2022
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The main nighttime sink of α-pinene, a hydrocarbon abundantly emitted by plants, is reaction with NO3 to form nitrooxy peroxy radicals (nRO2). Using uniquely designed chamber experiments, we show that this reaction is a major source of organic aerosol when nRO2 reacts with other nRO2 and forms a nitrooxy hydroperoxide when nRO2 reacts with HO2. Under ambient conditions these pathways are key loss processes of atmospheric reactive nitrogen in areas with mixed biogenic and anthropogenic influence.
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.
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.
Adam R. Vaughan, James D. Lee, Stefan Metzger, David Durden, Alastair C. Lewis, Marvin D. Shaw, Will S. Drysdale, Ruth M. Purvis, Brian Davison, and C. Nicholas Hewitt
Atmos. Chem. Phys., 21, 15283–15298, https://doi.org/10.5194/acp-21-15283-2021, https://doi.org/10.5194/acp-21-15283-2021, 2021
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Validating emissions estimates of atmospheric pollutants is a vital pathway towards reducing urban concentrations of air pollution and ensuring effective legislative controls are implemented. The work presented here highlights a strategy capable of quantifying and spatially disaggregating NOx emissions over challenging urban terrain. This work shows great scope as a tool for emission inventory validation and independent generation of high-resolution surface emissions on a city-wide scale.
Hélène Angot, Connor Davel, Christine Wiedinmyer, Gabrielle Pétron, Jashan Chopra, Jacques Hueber, Brendan Blanchard, Ilann Bourgeois, Isaac Vimont, Stephen A. Montzka, Ben R. Miller, James W. Elkins, and Detlev Helmig
Atmos. Chem. Phys., 21, 15153–15170, https://doi.org/10.5194/acp-21-15153-2021, https://doi.org/10.5194/acp-21-15153-2021, 2021
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After a multidecadal global decline in atmospheric abundance of ethane and propane (precursors of tropospheric ozone and aerosols), previous work showed a reversal of this trend in 2009–2015 in the Northern Hemisphere due to the growth in oil and natural gas production in North America. Here we show a temporary pause in the growth of atmospheric ethane and propane in 2015–2018 and highlight the critical need for additional top-down studies to further constrain ethane and propane emissions.
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 %.
Rebecca L. Wagner, Naomi J. Farren, Jack Davison, Stuart Young, James R. Hopkins, Alastair C. Lewis, David C. Carslaw, and Marvin D. Shaw
Atmos. Meas. Tech., 14, 6083–6100, https://doi.org/10.5194/amt-14-6083-2021, https://doi.org/10.5194/amt-14-6083-2021, 2021
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We describe the use of a selected-ion flow-tube mass spectrometer (SIFT-MS) in a mobile laboratory to provide on-road, high spatial and temporal measurements of CO2, CH4, multiple volatile organic compounds (VOCs) and other trace gases. Results are presented that highlight the potential of this platform for developing characterisation methods of different emissions sources in complex urban areas.
Beth S. Nelson, Gareth J. Stewart, Will S. Drysdale, Mike J. Newland, Adam R. Vaughan, Rachel E. Dunmore, Pete M. Edwards, Alastair C. Lewis, Jacqueline F. Hamilton, W. Joe Acton, C. Nicholas Hewitt, Leigh R. Crilley, Mohammed S. Alam, Ülkü A. Şahin, David C. S. Beddows, William J. Bloss, Eloise Slater, Lisa K. Whalley, Dwayne E. Heard, James M. Cash, Ben Langford, Eiko Nemitz, Roberto Sommariva, Sam Cox, Shivani, Ranu Gadi, Bhola R. Gurjar, James R. Hopkins, Andrew R. Rickard, and James D. Lee
Atmos. Chem. Phys., 21, 13609–13630, https://doi.org/10.5194/acp-21-13609-2021, https://doi.org/10.5194/acp-21-13609-2021, 2021
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Ozone production at an urban site in Delhi is sensitive to volatile organic compound (VOC) concentrations, particularly those of the aromatic, monoterpene, and alkene VOC classes. The change in ozone production by varying atmospheric pollutants according to their sources, as defined in an emissions inventory, is investigated. The study suggests that reducing road transport emissions alone does not reduce reactive VOCs in the atmosphere enough to perturb an increase in ozone production.
Esther Borrás, Luis A. Tortajada-Genaro, Milagro Ródenas, Teresa Vera, Thomas Speak, Paul Seakins, Marvin D. Shaw, Alastair C. Lewis, and Amalia Muñoz
Atmos. Meas. Tech., 14, 4989–4999, https://doi.org/10.5194/amt-14-4989-2021, https://doi.org/10.5194/amt-14-4989-2021, 2021
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This work presents promising results in the characterization of specific atmospheric pollutants (oxygenated VOCs) present at very low but highly relevant concentrations.
We carried out this research at EUPHORE facilities within the framework of the EUROCHAMP project. A new analytical method, with high robustness and precision, also clean in the use of solvents, low cost, and easily adaptable for use in mobile laboratories for air quality monitoring, is presented.
Eleni Dovrou, Kelvin H. Bates, Jean C. Rivera-Rios, Joshua L. Cox, Joshua D. Shutter, and Frank N. Keutsch
Atmos. Chem. Phys., 21, 8999–9008, https://doi.org/10.5194/acp-21-8999-2021, https://doi.org/10.5194/acp-21-8999-2021, 2021
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We examined the mechanism and products of oxidation of dissolved sulfur dioxide with the main isomers of isoprene hydroxyl hydroperoxides, via laboratory and model analysis. Two chemical mechanism pathways are proposed and the results provide an improved understanding of the broader atmospheric chemistry and role of multifunctional organic hydroperoxides, which should be the dominant VOC oxidation products under low-NO conditions, highlighting their significant contribution to sulfate formation.
Qian Shu, Benjamin Murphy, Jonathan E. Pleim, Donna Schwede, Barron H. Henderson, Havala O.T. Pye, Keith Wyat Appel, Tanvir R. Khan, and Judith A. Perlinger
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-129, https://doi.org/10.5194/gmd-2021-129, 2021
Preprint withdrawn
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We have bridged the gap between dry deposition measurement and modeling by rigorous use of box and regional transport models and field measurements, but more efforts are needed. This study highlights that deviation among deposition schemes is most pronounced for small and large particles. This study better links model predictions to available real-world observations and incrementally reduces uncertainties in the magnitude of loss processes important for the lifecycle of air pollutants.
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.
Steven J. Campbell, Kate Wolfer, Battist Utinger, Joe Westwood, Zhi-Hui Zhang, Nicolas Bukowiecki, Sarah S. Steimer, Tuan V. Vu, Jingsha Xu, Nicholas Straw, Steven Thomson, Atallah Elzein, Yele Sun, Di Liu, Linjie Li, Pingqing Fu, Alastair C. Lewis, Roy M. Harrison, William J. Bloss, Miranda Loh, Mark R. Miller, Zongbo Shi, and Markus Kalberer
Atmos. Chem. Phys., 21, 5549–5573, https://doi.org/10.5194/acp-21-5549-2021, https://doi.org/10.5194/acp-21-5549-2021, 2021
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In this study, we quantify PM2.5 oxidative potential (OP), a metric widely suggested as a potential measure of particle toxicity, in Beijing in summer and winter using four acellular assays. We correlate PM2.5 OP with a comprehensive range of atmospheric and particle composition measurements, demonstrating inter-assay differences and seasonal variation of PM2.5 OP. Using multivariate statistical analysis, we highlight specific particle chemical components and sources that influence OP.
Stuart K. Grange, James D. Lee, Will S. Drysdale, Alastair C. Lewis, Christoph Hueglin, Lukas Emmenegger, and David C. Carslaw
Atmos. Chem. Phys., 21, 4169–4185, https://doi.org/10.5194/acp-21-4169-2021, https://doi.org/10.5194/acp-21-4169-2021, 2021
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The changes in mobility across Europe due to the COVID-19 lockdowns had consequences for air quality. We compare what was experienced to estimates of "what would have been" without the lockdowns. Nitrogen dioxide (NO2), an important vehicle-sourced pollutant, decreased by a third. However, ozone (O3) increased in response to lower NO2. Because NO2 is decreasing over time, increases in O3 can be expected in European urban areas and will require management to avoid future negative outcomes.
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.
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.
Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Archit Mehra, Stephen D. Worrall, Asan Bacak, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Tuan Vu, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 2125–2147, https://doi.org/10.5194/acp-21-2125-2021, https://doi.org/10.5194/acp-21-2125-2021, 2021
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To understand how emission controls will impact ozone, an understanding of the sources and sinks of OH and the chemical cycling between peroxy radicals is needed. This paper presents measurements of OH, HO2 and total RO2 taken in central Beijing. The radical observations are compared to a detailed chemistry model, which shows that under low NO conditions, there is a missing OH source. Under high NOx conditions, the model under-predicts RO2 and impacts our ability to model ozone.
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.
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.
Hélène Angot, Katelyn McErlean, Lu Hu, Dylan B. Millet, Jacques Hueber, Kaixin Cui, Jacob Moss, Catherine Wielgasz, Tyler Milligan, Damien Ketcherside, M. Syndonia Bret-Harte, and Detlev Helmig
Biogeosciences, 17, 6219–6236, https://doi.org/10.5194/bg-17-6219-2020, https://doi.org/10.5194/bg-17-6219-2020, 2020
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We report biogenic volatile organic compounds (BVOCs) ambient levels and emission rates from key vegetation species in the Alaskan arctic tundra, providing a new data set to further constrain isoprene chemistry under low NOx conditions in models. We add to the growing body of evidence that climate-induced changes in the vegetation composition will significantly affect the BVOC emission potential of the tundra, with implications for atmospheric oxidation processes and climate feedbacks.
Eloise J. Slater, Lisa K. Whalley, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Leigh R. Crilley, Louisa Kramer, William Bloss, Tuan Vu, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 20, 14847–14871, https://doi.org/10.5194/acp-20-14847-2020, https://doi.org/10.5194/acp-20-14847-2020, 2020
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The paper details atmospheric chemistry in a megacity (Beijing), focussing on radicals which mediate the formation of secondary pollutants such as ozone and particles. Highly polluted conditions were experienced, including the highest ever levels of nitric oxide (NO), with simultaneous radical measurements. Radical concentrations were large during "haze" events, demonstrating active photochemistry. Modelling showed that our understanding of the chemistry at high NOx levels is incomplete.
Douglas Morrison, Ian Crawford, Nicholas Marsden, Michael Flynn, Katie Read, Luis Neves, Virginia Foot, Paul Kaye, Warren Stanley, Hugh Coe, David Topping, and Martin Gallagher
Atmos. Chem. Phys., 20, 14473–14490, https://doi.org/10.5194/acp-20-14473-2020, https://doi.org/10.5194/acp-20-14473-2020, 2020
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We provide conservative estimates of the concentrations of bacteria within transatlantic dust clouds, originating from the African continent. We observe significant seasonal differences in the overall concentrations of particles but no seasonal variation in the ratio between bacteria and dust. With bacteria contributing to ice formation at warmer temperatures than dust, our observations should improve the accuracy of climate models.
Atallah Elzein, Gareth J. Stewart, Stefan J. Swift, Beth S. Nelson, Leigh R. Crilley, Mohammed S. Alam, Ernesto Reyes-Villegas, Ranu Gadi, Roy M. Harrison, Jacqueline F. Hamilton, and Alastair C. Lewis
Atmos. Chem. Phys., 20, 14303–14319, https://doi.org/10.5194/acp-20-14303-2020, https://doi.org/10.5194/acp-20-14303-2020, 2020
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We collected high-frequency air particle samples (PM2.5) in Beijing (China) and Delhi (India) and measured the concentration of PAHs in daytime and night-time. PAHs were higher in Delhi than in Beijing, and the five-ring PAHs contribute the most to the total PAH concentration. We compared the emission sources and identified the major sectors that could be subject to mitigation measures. The adverse health effects from inhalation exposure to PAHs in Delhi are 2.2 times higher than in Beijing.
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.
Amy E. Christiansen, Annmarie G. Carlton, and Barron H. Henderson
Atmos. Chem. Phys., 20, 11607–11624, https://doi.org/10.5194/acp-20-11607-2020, https://doi.org/10.5194/acp-20-11607-2020, 2020
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We quantify differences in surface-level fine particle mass (PM2.5) chemical composition in relation to satellite-derived cloud flags and find significant differences between clear-sky and cloud days. The work suggests that future analysis in this area is warranted.
Wei Wang, Laurens Ganzeveld, Samuel Rossabi, Jacques Hueber, and Detlev Helmig
Atmos. Chem. Phys., 20, 11287–11304, https://doi.org/10.5194/acp-20-11287-2020, https://doi.org/10.5194/acp-20-11287-2020, 2020
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Trees exchange with the atmosphere nitrogen oxides and ozone, affecting the tropospheric composition and consequently air quality and ecosystem health. We examined the leaf-level gas exchanges for four typical tree species (pine, maple, oak, aspen) found in northern Michigan, US. The leaves largely absorb the gases, showing little evidence of emission. We measured the uptake rates that can be used to improve model studies of the source and sink processes controlling these gases in forests.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys., 20, 10937–10951, https://doi.org/10.5194/acp-20-10937-2020, https://doi.org/10.5194/acp-20-10937-2020, 2020
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Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
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Short summary
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.
Ethane and propane are volatile organic compounds emitted from human activities which help to...
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