Articles | Volume 21, issue 5
https://doi.org/10.5194/acp-21-4169-2021
© Author(s) 2021. 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-21-4169-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
18 Mar 2021
Research article |
| 18 Mar 2021
| 18 Mar 2021
COVID-19 lockdowns highlight a risk of increasing ozone pollution in European urban areas
Empa, Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, 8600 Dübendorf, Switzerland
Wolfson Atmospheric Chemistry Laboratories, University of York, York, YO10 5DD, United Kingdom
James D. Lee
Wolfson Atmospheric Chemistry Laboratories, University of York, York, YO10 5DD, United Kingdom
Will S. Drysdale
Wolfson Atmospheric Chemistry Laboratories, University of York, York, YO10 5DD, United Kingdom
Alastair C. Lewis
Wolfson Atmospheric Chemistry Laboratories, University of York, York, YO10 5DD, United Kingdom
National Centre for Atmospheric Science, University of York, Heslington, York, YO10 5DD, United Kingdom
Christoph Hueglin
Empa, Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, 8600 Dübendorf, Switzerland
Lukas Emmenegger
Empa, Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, 8600 Dübendorf, Switzerland
David C. Carslaw
CORRESPONDING AUTHOR
Wolfson Atmospheric Chemistry Laboratories, University of York, York, YO10 5DD, United Kingdom
Ricardo Energy & Environment, Harwell, Oxfordshire, OX11 0QR, United Kingdom
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In order to support the city of Zurich in tracking its path to net-zero greenhouse gas emissions planned to be reached by 2040, a CO2 emission monitoring system was established. The system combines a dense network of CO2 sensors with a high-resolution atmospheric transport model GRAMM/GRAL. This study presents the setup of the model together with its numerous inputs and evaluates its performance in comparison with the observations from the CO2 sensor network.
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Carbon dioxide (CO2) is a very important atmospheric pollutant, and to better understand the gas's source and sink dynamics, a mid-cost sensor network hosting 26 sites was deployed in and around Zurich, Switzerland. The sensor measurement performance was quantified, and natural and anthropogenic CO2 emission sources were explored with a focus on what drives high CO2 levels. The observations will be used further by others to validate what is thought to be known about CO2 emissions in the region.
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Matthew James Rowlinson, Lucy J. Carpenter, Mat J. Evans, James D. Lee, Simone Andersen, Tomas Sherwen, Anna B. Callaghan, Roberto Sommariva, William Bloss, Siqi Hou, Leigh R. Crilley, Klaus Pfeilsticker, Benjamin Weyland, Thomas B. Ryerson, Patrick R. Veres, Pedro Campuzano-Jost, Hongyu Guo, Benjamin A. Nault, Jose L. Jimenez, and Khanneh Wadinga Fomba
EGUsphere, https://doi.org/10.5194/egusphere-2025-830, https://doi.org/10.5194/egusphere-2025-830, 2025
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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.
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
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-566, https://doi.org/10.5194/essd-2024-566, 2025
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.
Beth Nelson and Will Drysdale
EGUsphere, https://doi.org/10.5194/egusphere-2024-3743, https://doi.org/10.5194/egusphere-2024-3743, 2025
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Trends in urban O3 and NO2 across Europe and the USA were explored between 2000–2021. Many sites in Europe and revealed a slowing in the increase of high O3 levels though more trends were found to having an increasing O3 trend in 2015–2021. The reverse was true in the USA. The change points revealed several sites in Europe, were the second change point in NO2 switched to a negative trend, occurred in 2020 due to the COVID-19 pandemic, and in some cases this has continued until 2023.
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.
Yuri Brugnara, Martin Steinbacher, Simone Baffelli, and Lukas Emmenegger
EGUsphere, https://doi.org/10.5194/egusphere-2024-3556, https://doi.org/10.5194/egusphere-2024-3556, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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GAW-QC is an interactive dashboard for the quality control of in-situ atmospheric composition measurements made at stations taking part in the Global Atmosphere Watch network. Even though it is mainly targeted at station operators who want to analyze recent, not yet published measurements, it allows anybody to verify the quality of already published measurements using various anomaly detection algorithms as well as visual comparisons.
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.
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.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter Hess, Heikki Lihavainen, Christine Wiedinmyer, Jenny Hand, Maria Grazia Alaimo, Célia Alves, Andres Alastuey, Paulo Artaxo, Africa Barreto, Francisco Barraza, Silvia Becagli, Giulia Calzolai, Shankarararman Chellam, Ying Chen, Patrick Chuang, David D. Cohen, Cristina Colombi, Evangelia Diapouli, Gaetano Dongarra, Konstantinos Eleftheriadis, Corinne Galy-Lacaux, Cassandra Gaston, Dario Gomez, Yenny González Ramos, Hannele Hakola, Roy M. Harrison, Chris Heyes, Barak Herut, Philip Hopke, Christoph Hüglin, Maria Kanakidou, Zsofia Kertesz, Zbiginiw Klimont, Katriina Kyllönen, Fabrice Lambert, Xiaohong Liu, Remi Losno, Franco Lucarelli, Willy Maenhaut, Beatrice Marticorena, Randall V. Martin, Nikolaos Mihalopoulos, Yasser Morera-Gomez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal Weagle, and Xi Zhao
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-1, https://doi.org/10.5194/essd-2024-1, 2024
Preprint withdrawn
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Aerosol particles can interact with incoming solar radiation and outgoing long wave radiation, change cloud properties, affect photochemistry, impact surface air quality, and when deposited impact surface albedo of snow and ice, and modulate carbon dioxide uptake by the land and ocean. Here we present a new compilation of aerosol observations including composition, a methodology for comparing the datasets to model output, and show the implications of these results using one model.
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.
Xuewei Hou, Oliver Wild, Bin Zhu, and James Lee
Atmos. Chem. Phys., 23, 15395–15411, https://doi.org/10.5194/acp-23-15395-2023, https://doi.org/10.5194/acp-23-15395-2023, 2023
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In response to the climate crisis, many countries have committed to net zero in a certain future year. The impacts of net-zero scenarios on tropospheric O3 are less well studied and remain unclear. In this study, we quantified the changes of tropospheric O3 budgets, spatiotemporal distributions of future surface O3 in east Asia and regional O3 source contributions for 2060 under a net-zero scenario using the NCAR Community Earth System Model (CESM) and online O3-tagging methods.
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 Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
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The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
Simone Brunamonti, Manuel Graf, Tobias Bühlmann, Céline Pascale, Ivan Ilak, Lukas Emmenegger, and Béla Tuzson
Atmos. Meas. Tech., 16, 4391–4407, https://doi.org/10.5194/amt-16-4391-2023, https://doi.org/10.5194/amt-16-4391-2023, 2023
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The abundance of water vapor (H2O) in the upper atmosphere has a significant impact on the rate of global warming. We developed a new lightweight spectrometer (ALBATROSS) for H2O measurements aboard meteorological balloons. Here, we assess the accuracy and precision of ALBATROSS using metrology-grade reference gases. The results demonstrate the exceptional potential of mid-infrared laser absorption spectroscopy as a new reference method for in situ measurements of H2O in the upper atmosphere.
Foteini Stavropoulou, Katarina Vinković, Bert Kers, Marcel de Vries, Steven van Heuven, Piotr Korbeń, Martina Schmidt, Julia Wietzel, Pawel Jagoda, Jaroslav M. Necki, Jakub Bartyzel, Hossein Maazallahi, Malika Menoud, Carina van der Veen, Sylvia Walter, Béla Tuzson, Jonas Ravelid, Randulph Paulo Morales, Lukas Emmenegger, Dominik Brunner, Michael Steiner, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, Hugo Denier van der Gon, Antonio Delre, Maklawe Essonanawe Edjabou, Charlotte Scheutz, Marius Corbu, Sebastian Iancu, Denisa Moaca, Alin Scarlat, Alexandru Tudor, Ioana Vizireanu, Andreea Calcan, Magdalena Ardelean, Sorin Ghemulet, Alexandru Pana, Aurel Constantinescu, Lucian Cusa, Alexandru Nica, Calin Baciu, Cristian Pop, Andrei Radovici, Alexandru Mereuta, Horatiu Stefanie, Alexandru Dandocsi, Bas Hermans, Stefan Schwietzke, Daniel Zavala-Araiza, Huilin Chen, and Thomas Röckmann
Atmos. Chem. Phys., 23, 10399–10412, https://doi.org/10.5194/acp-23-10399-2023, https://doi.org/10.5194/acp-23-10399-2023, 2023
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In this study, we quantify CH4 emissions from onshore oil production sites in Romania at source and facility level using a combination of ground- and drone-based measurement techniques. We show that the total CH4 emissions in our studied areas are much higher than the emissions reported to UNFCCC, and up to three-quarters of the detected emissions are related to operational venting. Our results suggest that oil and gas production infrastructure in Romania holds a massive mitigation potential.
Jean-Philippe Putaud, Enrico Pisoni, Alexander Mangold, Christoph Hueglin, Jean Sciare, Michael Pikridas, Chrysanthos Savvides, Jakub Ondracek, Saliou Mbengue, Alfred Wiedensohler, Kay Weinhold, Maik Merkel, Laurent Poulain, Dominik van Pinxteren, Hartmut Herrmann, Andreas Massling, Claus Nordstroem, Andrés Alastuey, Cristina Reche, Noemí Pérez, Sonia Castillo, Mar Sorribas, Jose Antonio Adame, Tuukka Petaja, Katrianne Lehtipalo, Jarkko Niemi, Véronique Riffault, Joel F. de Brito, Augustin Colette, Olivier Favez, Jean-Eudes Petit, Valérie Gros, Maria I. Gini, Stergios Vratolis, Konstantinos Eleftheriadis, Evangelia Diapouli, Hugo Denier van der Gon, Karl Espen Yttri, and Wenche Aas
Atmos. Chem. Phys., 23, 10145–10161, https://doi.org/10.5194/acp-23-10145-2023, https://doi.org/10.5194/acp-23-10145-2023, 2023
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Many European people are still exposed to levels of air pollution that can affect their health. COVID-19 lockdowns in 2020 were used to assess the impact of the reduction in human mobility on air pollution across Europe by comparing measurement data with values that would be expected if no lockdown had occurred. We show that lockdown measures did not lead to consistent decreases in the concentrations of fine particulate matter suspended in the air, and we investigate why.
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.
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.
Nadia K. Colombi, Daniel J. Jacob, Laura Hyesung Yang, Shixian Zhai, Viral Shah, Stuart K. Grange, Robert M. Yantosca, Soontae Kim, and Hong Liao
Atmos. Chem. Phys., 23, 4031–4044, https://doi.org/10.5194/acp-23-4031-2023, https://doi.org/10.5194/acp-23-4031-2023, 2023
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Surface ozone, detrimental to human and ecosystem health, is very high and increasing in South Korea. Using a global model of the atmosphere, we found that emissions from South Korea and China contribute equally to the high ozone observed. We found that in the absence of all anthropogenic emissions over East Asia, ozone is still very high, implying that the air quality standard in South Korea is not practically achievable unless this background external to East Asia can be decreased.
Samuel J. Cliff, Will Drysdale, James D. Lee, Carole Helfter, Eiko Nemitz, Stefan Metzger, and Janet F. Barlow
Atmos. Chem. Phys., 23, 2315–2330, https://doi.org/10.5194/acp-23-2315-2023, https://doi.org/10.5194/acp-23-2315-2023, 2023
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Emissions of nitrogen oxides (NOx) to the atmosphere are an ongoing air quality issue. This study directly measures emissions of NOx and carbon dioxide from a tall tower in central London during the coronavirus pandemic. It was found that transport NOx emissions had reduced by >73 % since 2017 as a result of air quality policy and reduced congestion during coronavirus restrictions. During this period, central London was thought to be dominated by point-source heat and power generation emissions.
Jacob T. Shaw, Amy Foulds, Shona Wilde, Patrick Barker, Freya A. Squires, James Lee, Ruth Purvis, Ralph Burton, Ioana Colfescu, Stephen Mobbs, Samuel Cliff, Stéphane J.-B. Bauguitte, Stuart Young, Stefan Schwietzke, and Grant Allen
Atmos. Chem. Phys., 23, 1491–1509, https://doi.org/10.5194/acp-23-1491-2023, https://doi.org/10.5194/acp-23-1491-2023, 2023
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Flaring is used by the oil and gas sector to dispose of unwanted natural gas or for safety. However, few studies have assessed the efficiency with which the gas is combusted. We sampled flaring emissions from offshore facilities in the North Sea. Average measured flaring efficiencies were ~ 98 % but with a skewed distribution, including many flares of lower efficiency. NOx and ethane emissions were also measured. Inefficient flaring practices could be a target for mitigating carbon emissions.
Lars Mächler, Daniel Baggenstos, Florian Krauss, Jochen Schmitt, Bernhard Bereiter, Remo Walther, Christoph Reinhard, Béla Tuzson, Lukas Emmenegger, and Hubertus Fischer
Atmos. Meas. Tech., 16, 355–372, https://doi.org/10.5194/amt-16-355-2023, https://doi.org/10.5194/amt-16-355-2023, 2023
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We present a new method to extract the gases from ice cores and measure their greenhouse gas composition. The ice is sublimated continuously with a near-infrared laser, releasing the gases, which are then analyzed on a laser absorption spectrometer. The main advantage over previous efforts is a low effective resolution of 1–2 cm. This capability is crucial for the analysis of highly thinned ice, as expected from ongoing drilling efforts to extend ice core history further back in time.
Daniel J. Bryant, Beth S. Nelson, Stefan J. Swift, Sri Hapsari Budisulistiorini, Will S. Drysdale, Adam R. Vaughan, Mike J. Newland, James R. Hopkins, James M. Cash, Ben Langford, Eiko Nemitz, W. Joe F. Acton, C. Nicholas Hewitt, Tuhin Mandal, Bhola R. Gurjar, Shivani, Ranu Gadi, James D. Lee, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 23, 61–83, https://doi.org/10.5194/acp-23-61-2023, https://doi.org/10.5194/acp-23-61-2023, 2023
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This paper investigates the sources of isoprene and monoterpene compounds and their particulate-phase oxidation products in Delhi, India. This was done to improve our understanding of the sources, concentrations, and fate of volatile emissions in megacities. By studying the chemical composition of offline filter samples, we report that a significant share of the oxidised organic aerosol in Delhi is from isoprene and monoterpenes. This has implications for human health and policy development.
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.
Alfred W. Mayhew, Ben H. Lee, Joel A. Thornton, Thomas J. Bannan, James Brean, James R. Hopkins, James D. Lee, Beth S. Nelson, Carl Percival, Andrew R. Rickard, Marvin D. Shaw, Peter M. Edwards, and Jaqueline F. Hamilton
Atmos. Chem. Phys., 22, 14783–14798, https://doi.org/10.5194/acp-22-14783-2022, https://doi.org/10.5194/acp-22-14783-2022, 2022
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Isoprene nitrates are chemical species commonly found in the atmosphere that are important for their impacts on air quality and climate. This paper compares 3 different representations of the chemistry of isoprene nitrates in computational models highlighting cases where the choice of chemistry included has significant impacts on the concentration and composition of the modelled nitrates. Calibration of mass spectrometers is also shown to be an important factor when analysing isoprene nitrates.
Simone M. Pieber, Béla Tuzson, Stephan Henne, Ute Karstens, Christoph Gerbig, Frank-Thomas Koch, Dominik Brunner, Martin Steinbacher, and Lukas Emmenegger
Atmos. Chem. Phys., 22, 10721–10749, https://doi.org/10.5194/acp-22-10721-2022, https://doi.org/10.5194/acp-22-10721-2022, 2022
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Understanding regional greenhouse gas emissions into the atmosphere is a prerequisite to mitigate climate change. In this study, we investigated the regional contributions of carbon dioxide (CO2) at the location of the high Alpine observatory Jungfraujoch (JFJ, Switzerland, 3580 m a.s.l.). To this purpose, we combined receptor-oriented atmospheric transport simulations for CO2 concentration in the period 2009–2017 with stable carbon isotope (δ13C–CO2) information.
Will S. Drysdale, Adam R. Vaughan, Freya A. Squires, Sam J. Cliff, Stefan Metzger, David Durden, Natchaya Pingintha-Durden, Carole Helfter, Eiko Nemitz, C. Sue B. Grimmond, Janet Barlow, Sean Beevers, Gregor Stewart, David Dajnak, Ruth M. Purvis, and James D. Lee
Atmos. Chem. Phys., 22, 9413–9433, https://doi.org/10.5194/acp-22-9413-2022, https://doi.org/10.5194/acp-22-9413-2022, 2022
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Measurements of NOx emissions are important for a good understanding of air quality. While there are many direct measurements of NOx concentration, there are very few measurements of its emission. Measurements of emissions provide constraints on emissions inventories and air quality models. This article presents measurements of NOx emission from the BT Tower in central London in 2017 and compares them with inventories, finding that they underestimate by a factor of ∼1.48.
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.
Stuart K. Grange, Gaëlle Uzu, Samuël Weber, Jean-Luc Jaffrezo, and Christoph Hueglin
Atmos. Chem. Phys., 22, 7029–7050, https://doi.org/10.5194/acp-22-7029-2022, https://doi.org/10.5194/acp-22-7029-2022, 2022
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Oxidative potential (OP), a biologically relevant metric for particulate matter (PM), was linked to PM10 and PM2.5 sources and constituents across Switzerland between 2018 and 2019. Wood burning and non-exhaust traffic emissions were identified as key processes that led to enhanced OP. Therefore, the make-up of the PM mix was very important for OP. The results highlight the importance of the management of wood burning and non-exhaust emissions to reduce OP, and presumably biological harm.
Horim Kim, Michael Müller, Stephan Henne, and Christoph Hüglin
Atmos. Meas. Tech., 15, 2979–2992, https://doi.org/10.5194/amt-15-2979-2022, https://doi.org/10.5194/amt-15-2979-2022, 2022
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In this study, the performance of electrochemical sensors for NO and NO2 for measuring air quality was determined over a longer operating period. The performance of NO sensors remained reliable for more than 18 months. However, the NO2 sensors showed decreasing performance over time. During deployment, we found that the NO2 sensors can distinguish general pollution levels, but they proved unsuitable for accurate measurements due to significant biases.
Adam Brighty, Véronique Jacob, Gaëlle Uzu, Lucille Borlaza, Sébastien Conil, Christoph Hueglin, Stuart K. Grange, Olivier Favez, Cécile Trébuchon, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 22, 6021–6043, https://doi.org/10.5194/acp-22-6021-2022, https://doi.org/10.5194/acp-22-6021-2022, 2022
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With an revised analytical method and long-term sampling strategy, we have been able to elucidate much more information about atmospheric plant debris, a poorly understood class of particulate matter. We found weaker seasonal patterns at urban locations compared to rural locations and significant interannual variability in concentrations between previous years and 2020, during the COVID-19 pandemic. This suggests a possible man-made influence on plant debris concentration and source strength.
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.
Randulph Morales, Jonas Ravelid, Katarina Vinkovic, Piotr Korbeń, Béla Tuzson, Lukas Emmenegger, Huilin Chen, Martina Schmidt, Sebastian Humbel, and Dominik Brunner
Atmos. Meas. Tech., 15, 2177–2198, https://doi.org/10.5194/amt-15-2177-2022, https://doi.org/10.5194/amt-15-2177-2022, 2022
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Mapping trace gas emission plumes using in situ measurements from unmanned aerial vehicles (UAVs) is an emerging and attractive possibility to quantify emissions from localized sources. We performed an extensive controlled-release experiment to develop an optimal quantification method and to determine the related uncertainties under various environmental and sampling conditions. Our approach was successful in quantifying local methane sources from drone-based measurements.
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
Preprint withdrawn
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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.
Amy Foulds, Grant Allen, Jacob T. Shaw, Prudence Bateson, Patrick A. Barker, Langwen Huang, Joseph R. Pitt, James D. Lee, Shona E. Wilde, Pamela Dominutti, Ruth M. Purvis, David Lowry, James L. France, Rebecca E. Fisher, Alina Fiehn, Magdalena Pühl, Stéphane J. B. Bauguitte, Stephen A. Conley, Mackenzie L. Smith, Tom Lachlan-Cope, Ignacio Pisso, and Stefan Schwietzke
Atmos. Chem. Phys., 22, 4303–4322, https://doi.org/10.5194/acp-22-4303-2022, https://doi.org/10.5194/acp-22-4303-2022, 2022
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We measured CH4 emissions from 21 offshore oil and gas facilities in the Norwegian Sea in 2019. Measurements compared well with operator-reported emissions but were greatly underestimated when compared with a 2016 global fossil fuel inventory. This study demonstrates the need for up-to-date and accurate inventories for use in research and policy and the important benefits of best-practice reporting methods by operators. Airborne measurements are an effective tool to validate such inventories.
Franz Conen, Annika Einbock, Claudia Mignani, and Christoph Hüglin
Atmos. Chem. Phys., 22, 3433–3444, https://doi.org/10.5194/acp-22-3433-2022, https://doi.org/10.5194/acp-22-3433-2022, 2022
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Above western Europe, ice typically starts to form in clouds a few kilometres above the ground if suitable aerosol particles are present. In air masses typical for that altitude, we found that such particles most likely originate from bacteria and fungi living on plants. Occasional Saharan dust intrusions seem to contribute little to the number concentration of particles able to freeze cloud droplets between 0°C and −15°C.
Dominique Rust, Ioannis Katharopoulos, Martin K. Vollmer, Stephan Henne, Simon O'Doherty, Daniel Say, Lukas Emmenegger, Renato Zenobi, and Stefan Reimann
Atmos. Chem. Phys., 22, 2447–2466, https://doi.org/10.5194/acp-22-2447-2022, https://doi.org/10.5194/acp-22-2447-2022, 2022
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Artificial halocarbons contribute to ozone layer depletion and to global warming. We measured the atmospheric concentrations of halocarbons at the Beromünster tower, modelled the Swiss emissions, and compared the results to the internationally reported Swiss emissions inventory. For most of the halocarbons, we found good agreement, whereas one refrigerant might be overestimated in the inventory. In addition, we present first emission estimates of the newest types of halocarbons.
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.
Gang Chen, Yulia Sosedova, Francesco Canonaco, Roman Fröhlich, Anna Tobler, Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Christoph Hueglin, Peter Graf, Urs Baltensperger, Jay G. Slowik, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 15081–15101, https://doi.org/10.5194/acp-21-15081-2021, https://doi.org/10.5194/acp-21-15081-2021, 2021
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A novel, advanced source apportionment technique was applied to a dataset measured in Magadino. Rolling positive matrix factorisation (PMF) allows for retrieving more realistic, time-dependent, and detailed information on organic aerosol sources. The strength of the rolling PMF mechanism is highlighted by comparing it with results derived from conventional seasonal PMF. Overall, this comprehensive interpretation of aerosol chemical speciation monitor data could be a role model for similar work.
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.
Ernesto Reyes-Villegas, Upasana Panda, Eoghan Darbyshire, James M. Cash, Rutambhara Joshi, Ben Langford, Chiara F. Di Marco, Neil J. Mullinger, Mohammed S. Alam, Leigh R. Crilley, Daniel J. Rooney, W. Joe F. Acton, Will Drysdale, Eiko Nemitz, Michael Flynn, Aristeidis Voliotis, Gordon McFiggans, Hugh Coe, James Lee, C. Nicholas Hewitt, Mathew R. Heal, Sachin S. Gunthe, Tuhin K. Mandal, Bhola R. Gurjar, Shivani, Ranu Gadi, Siddhartha Singh, Vijay Soni, and James D. Allan
Atmos. Chem. Phys., 21, 11655–11667, https://doi.org/10.5194/acp-21-11655-2021, https://doi.org/10.5194/acp-21-11655-2021, 2021
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This paper shows the first multisite online measurements of PM1 in Delhi, India, with measurements over different seasons in Old Delhi and New Delhi in 2018. Organic aerosol (OA) source apportionment was performed using positive matrix factorisation (PMF). Traffic was the main primary aerosol source for both OAs and black carbon, seen with PMF and Aethalometer model analysis, indicating that control of primary traffic exhaust emissions would make a significant reduction to Delhi air pollution.
Gongda Lu, Eloise A. Marais, Tuan V. Vu, Jingsha Xu, Zongbo Shi, James D. Lee, Qiang Zhang, Lu Shen, Gan Luo, and Fangqun Yu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-428, https://doi.org/10.5194/acp-2021-428, 2021
Revised manuscript not accepted
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Emission controls were imposed in Beijing-Tianjin-Hebei in northern China in autumn-winter 2017. We find that regional PM2.5 targets (15 % decrease relative to previous year) were exceeded. Our analysis shows that decline in precursor emissions only leads to less than half (43 %) the improved air quality. Most of the change (57 %) is due to interannual variability in meteorology. Stricter emission controls may be necessary in years with unfavourable meteorology.
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.
James M. Cash, Ben Langford, Chiara Di Marco, Neil J. Mullinger, James Allan, Ernesto Reyes-Villegas, Ruthambara Joshi, Mathew R. Heal, W. Joe F. Acton, C. Nicholas Hewitt, Pawel K. Misztal, Will Drysdale, Tuhin K. Mandal, Shivani, Ranu Gadi, Bhola Ram Gurjar, and Eiko Nemitz
Atmos. Chem. Phys., 21, 10133–10158, https://doi.org/10.5194/acp-21-10133-2021, https://doi.org/10.5194/acp-21-10133-2021, 2021
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We present the first real-time composition of submicron particulate matter (PM1) in Old Delhi using high-resolution aerosol mass spectrometry. Seasonal analysis shows peak concentrations occur during the post-monsoon, and novel-tracers reveal the largest sources are a combination of local open and regional crop residue burning. Strong links between increased chloride aerosol concentrations and burning sources of PM1 suggest burning sources are responsible for the post-monsoon chloride peak.
Huihui Wu, Jonathan W. Taylor, Justin M. Langridge, Chenjie Yu, James D. Allan, Kate Szpek, Michael I. Cotterell, Paul I. Williams, Michael Flynn, Patrick Barker, Cathryn Fox, Grant Allen, James Lee, and Hugh Coe
Atmos. Chem. Phys., 21, 9417–9440, https://doi.org/10.5194/acp-21-9417-2021, https://doi.org/10.5194/acp-21-9417-2021, 2021
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Seasonal biomass burning over West Africa is a globally significant source of carbonaceous particles in the atmosphere, which have important climate impacts but are poorly constrained. We conducted in situ airborne measurements to investigate the evolution of smoke aerosol properties in this region. We observed absorption enhancement for both black carbon and brown carbon after emission, which provides new field results and constraints on aerosol parameterizations for future climate models.
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.
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.
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.
Manuel Graf, Philipp Scheidegger, André Kupferschmid, Herbert Looser, Thomas Peter, Ruud Dirksen, Lukas Emmenegger, and Béla Tuzson
Atmos. Meas. Tech., 14, 1365–1378, https://doi.org/10.5194/amt-14-1365-2021, https://doi.org/10.5194/amt-14-1365-2021, 2021
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Water vapor is the most important natural greenhouse gas. The accurate and frequent measurement of its abundance, especially in the upper troposphere and lower stratosphere (UTLS), is technically challenging. We developed and characterized a mid-IR absorption spectrometer for highly accurate water vapor measurements in the UTLS. The instrument is sufficiently small and lightweight (3.9 kg) to be carried by meteorological balloons, which enables frequent and cost-effective soundings.
Gareth J. Stewart, Beth S. Nelson, W. Joe F. Acton, Adam R. Vaughan, Naomi J. Farren, James R. Hopkins, Martyn W. Ward, Stefan J. Swift, Rahul Arya, Arnab Mondal, Ritu Jangirh, Sakshi Ahlawat, Lokesh Yadav, Sudhir K. Sharma, Siti S. M. Yunus, C. Nicholas Hewitt, Eiko Nemitz, Neil Mullinger, Ranu Gadi, Lokesh K. Sahu, Nidhi Tripathi, Andrew R. Rickard, James D. Lee, Tuhin K. Mandal, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 2407–2426, https://doi.org/10.5194/acp-21-2407-2021, https://doi.org/10.5194/acp-21-2407-2021, 2021
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Biomass burning releases many lower-molecular-weight organic species which are difficult to analyse but important for the formation of organic aerosol. This study examined a new high-resolution technique to better characterise these difficult-to-analyse organic components. Some burning sources analysed in this study, such as cow dung cake and municipal solid waste, released extremely complex mixtures containing many thousands of different lower-volatility organic compounds.
Gareth J. Stewart, W. Joe F. Acton, Beth S. Nelson, Adam R. Vaughan, James R. Hopkins, Rahul Arya, Arnab Mondal, Ritu Jangirh, Sakshi Ahlawat, Lokesh Yadav, Sudhir K. Sharma, Rachel E. Dunmore, Siti S. M. Yunus, C. Nicholas Hewitt, Eiko Nemitz, Neil Mullinger, Ranu Gadi, Lokesh K. Sahu, Nidhi Tripathi, Andrew R. Rickard, James D. Lee, Tuhin K. Mandal, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 2383–2406, https://doi.org/10.5194/acp-21-2383-2021, https://doi.org/10.5194/acp-21-2383-2021, 2021
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Biomass burning is a major source of trace gases to the troposphere; however, the composition and quantity of emissions vary greatly between different fuel types. This work provided near-total quantitation of non-methane volatile organic compounds from combustion of biofuels from India. Emissions from cow dung cake combustion were significantly larger than conventional fuelwood combustion, potentially indicating that this source has a disproportionately large impact on regional air quality.
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.
Rutambhara Joshi, Dantong Liu, Eiko Nemitz, Ben Langford, Neil Mullinger, Freya Squires, James Lee, Yunfei Wu, Xiaole Pan, Pingqing Fu, Simone Kotthaus, Sue Grimmond, Qiang Zhang, Ruili Wu, Oliver Wild, Michael Flynn, Hugh Coe, and James Allan
Atmos. Chem. Phys., 21, 147–162, https://doi.org/10.5194/acp-21-147-2021, https://doi.org/10.5194/acp-21-147-2021, 2021
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Black carbon (BC) is a component of particulate matter which has significant effects on climate and human health. Sources of BC include biomass burning, transport, industry and domestic cooking and heating. In this study, we measured BC emissions in Beijing, finding a dominance of traffic emissions over all other sources. The quantitative method presented here has benefits for revising widely used emissions inventories and for understanding BC sources with impacts on air quality and climate.
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.
James D. Lee, Will S. Drysdale, Doug P. Finch, Shona E. Wilde, and Paul I. Palmer
Atmos. Chem. Phys., 20, 15743–15759, https://doi.org/10.5194/acp-20-15743-2020, https://doi.org/10.5194/acp-20-15743-2020, 2020
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Efforts to prevent the COVID-19 virus spreading across the globe have included travel restrictions and the closure of workplaces, leading to a significant drop in emissions of primary air pollutants. This provides for a unique opportunity to examine how air pollutant concentrations respond to an abrupt and prolonged reduction. We examine how NO2 and O3 have been affected at several urban measurement sites in the UK. We look at the change in NO2 compared to previous years and the effect on O3.
Patrick A. Barker, Grant Allen, Martin Gallagher, Joseph R. Pitt, Rebecca E. Fisher, Thomas Bannan, Euan G. Nisbet, Stéphane J.-B. Bauguitte, Dominika Pasternak, Samuel Cliff, Marina B. Schimpf, Archit Mehra, Keith N. Bower, James D. Lee, Hugh Coe, and Carl J. Percival
Atmos. Chem. Phys., 20, 15443–15459, https://doi.org/10.5194/acp-20-15443-2020, https://doi.org/10.5194/acp-20-15443-2020, 2020
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Africa is estimated to account for approximately 52 % of global biomass burning (BB) carbon emissions. Despite this, there has been little previous in situ study of African BB emissions. This work presents BB emission factors for various atmospheric trace gases sampled from an aircraft in two distinct areas of Africa (Senegal and Uganda). Intracontinental variability in biomass burning methane emission is identified, which is attributed to difference in the specific fuel mixtures burnt.
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.
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.
Bernhard Bereiter, Béla Tuzson, Philipp Scheidegger, André Kupferschmid, Herbert Looser, Lars Mächler, Daniel Baggenstos, Jochen Schmitt, Hubertus Fischer, and Lukas Emmenegger
Atmos. Meas. Tech., 13, 6391–6406, https://doi.org/10.5194/amt-13-6391-2020, https://doi.org/10.5194/amt-13-6391-2020, 2020
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The record of past greenhouse gas composition from ice cores is crucial for our understanding of global climate change. Deciphering this archive requires highly accurate and spatially resolved analysis of the very small amount of gas that is trapped in the ice. This is achieved with a mid-IR laser absorption spectrometer that provides simultaneous, high-precision measurements of CH4, N2O, CO2, and δ13C(CO2) and which will be coupled to a quantitative sublimation extraction method.
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.
Mohammed S. Alam, Leigh R. Crilley, James D. Lee, Louisa J. Kramer, Christian Pfrang, Mónica Vázquez-Moreno, Milagros Ródenas, Amalia Muñoz, and William J. Bloss
Atmos. Meas. Tech., 13, 5977–5991, https://doi.org/10.5194/amt-13-5977-2020, https://doi.org/10.5194/amt-13-5977-2020, 2020
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We report on the interference arising in measurements of nitrogen oxides (NOx) from the presence of a range of alkenes in sampled air when using the most widespread air quality monitoring technique for chemiluminescence detection. Interferences of up to 11 % are reported, depending upon the alkene present and conditions used. Such interferences may be of substantial importance for the interpretation of ambient NOx data, particularly for high volatile organic compound and low NOx environments.
Béla Tuzson, Manuel Graf, Jonas Ravelid, Philipp Scheidegger, André Kupferschmid, Herbert Looser, Randulph Paulo Morales, and Lukas Emmenegger
Atmos. Meas. Tech., 13, 4715–4726, https://doi.org/10.5194/amt-13-4715-2020, https://doi.org/10.5194/amt-13-4715-2020, 2020
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We describe a lightweight (2 kg) mid-IR laser spectrometer for airborne, in situ atmospheric methane (CH4) measurements. The instrument, based on an open-path circular multipass cell, provides fast response (1 Hz) and sub-parts-per-billion precision. It can easily be mounted on a drone, giving access to highly resolved 4D (spatial and temporal) data. The performance was assessed during field deployments involving artificial CH4 releases and vertical concentration gradients in the PBL.
Paolo Laj, Alessandro Bigi, Clémence Rose, Elisabeth Andrews, Cathrine Lund Myhre, Martine Collaud Coen, Yong Lin, Alfred Wiedensohler, Michael Schulz, John A. Ogren, Markus Fiebig, Jonas Gliß, Augustin Mortier, Marco Pandolfi, Tuukka Petäja, Sang-Woo Kim, Wenche Aas, Jean-Philippe Putaud, Olga Mayol-Bracero, Melita Keywood, Lorenzo Labrador, Pasi Aalto, Erik Ahlberg, Lucas Alados Arboledas, Andrés Alastuey, Marcos Andrade, Begoña Artíñano, Stina Ausmeel, Todor Arsov, Eija Asmi, John Backman, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Sébastien Conil, Cedric Couret, Derek Day, Wan Dayantolis, Anna Degorska, Konstantinos Eleftheriadis, Prodromos Fetfatzis, Olivier Favez, Harald Flentje, Maria I. Gini, Asta Gregorič, Martin Gysel-Beer, A. Gannet Hallar, Jenny Hand, Andras Hoffer, Christoph Hueglin, Rakesh K. Hooda, Antti Hyvärinen, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Jeong Eun Kim, Giorgos Kouvarakis, Irena Kranjc, Radovan Krejci, Markku Kulmala, Casper Labuschagne, Hae-Jung Lee, Heikki Lihavainen, Neng-Huei Lin, Gunter Löschau, Krista Luoma, Angela Marinoni, Sebastiao Martins Dos Santos, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Nhat Anh Nguyen, Jakub Ondracek, Noemi Pérez, Maria Rita Perrone, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Natalia Prats, Anthony Prenni, Fabienne Reisen, Salvatore Romano, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Maik Schütze, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Martin Steinbacher, Junying Sun, Gloria Titos, Barbara Toczko, Thomas Tuch, Pierre Tulet, Peter Tunved, Ville Vakkari, Fernando Velarde, Patricio Velasquez, Paolo Villani, Sterios Vratolis, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Jesus Yus-Diez, Vladimir Zdimal, Paul Zieger, and Nadezda Zikova
Atmos. Meas. Tech., 13, 4353–4392, https://doi.org/10.5194/amt-13-4353-2020, https://doi.org/10.5194/amt-13-4353-2020, 2020
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The paper establishes the fiducial reference of the GAW aerosol network providing the fully characterized value chain to the provision of four climate-relevant aerosol properties from ground-based sites. Data from almost 90 stations worldwide are reported for a reference year, 2017, providing a unique and very robust view of the variability of these variables worldwide. Current gaps in the GAW network are analysed and requirements for the Global Climate Monitoring System are proposed.
Eirini Boleti, Christoph Hueglin, Stuart K. Grange, André S. H. Prévôt, and Satoshi Takahama
Atmos. Chem. Phys., 20, 9051–9066, https://doi.org/10.5194/acp-20-9051-2020, https://doi.org/10.5194/acp-20-9051-2020, 2020
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Long-term temporal evolution of ozone concentrations between 2000 and 2015 in Europe was estimated using a signal decomposition technique. The seasonal cycles are correlated with local climate conditions and vary according to geographic region, while ozone levels are indicative of distance to emission sources. The site's environment plays a key role in ozone trends, with the most polluted environments showing the least reduction in ozone, while in less polluted areas ozone has decreased.
Martine Collaud Coen, Elisabeth Andrews, Andrés Alastuey, Todor Petkov Arsov, John Backman, Benjamin T. Brem, Nicolas Bukowiecki, Cédric Couret, Konstantinos Eleftheriadis, Harald Flentje, Markus Fiebig, Martin Gysel-Beer, Jenny L. Hand, András Hoffer, Rakesh Hooda, Christoph Hueglin, Warren Joubert, Melita Keywood, Jeong Eun Kim, Sang-Woo Kim, Casper Labuschagne, Neng-Huei Lin, Yong Lin, Cathrine Lund Myhre, Krista Luoma, Hassan Lyamani, Angela Marinoni, Olga L. Mayol-Bracero, Nikos Mihalopoulos, Marco Pandolfi, Natalia Prats, Anthony J. Prenni, Jean-Philippe Putaud, Ludwig Ries, Fabienne Reisen, Karine Sellegri, Sangeeta Sharma, Patrick Sheridan, James Patrick Sherman, Junying Sun, Gloria Titos, Elvis Torres, Thomas Tuch, Rolf Weller, Alfred Wiedensohler, Paul Zieger, and Paolo Laj
Atmos. Chem. Phys., 20, 8867–8908, https://doi.org/10.5194/acp-20-8867-2020, https://doi.org/10.5194/acp-20-8867-2020, 2020
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Long-term trends of aerosol radiative properties (52 stations) prove that aerosol load has significantly decreased over the last 20 years. Scattering trends are negative in Europe (EU) and North America (NA), not ss in Asia, and show a mix of positive and negative trends at polar stations. Absorption has mainly negative trends. The single scattering albedo has positive trends in Asia and eastern EU and negative in western EU and NA, leading to a global positive median trend of 0.02 % per year.
Freya A. Squires, Eiko Nemitz, Ben Langford, Oliver Wild, Will S. Drysdale, W. Joe F. Acton, Pingqing Fu, C. Sue B. Grimmond, Jacqueline F. Hamilton, C. Nicholas Hewitt, Michael Hollaway, Simone Kotthaus, James Lee, Stefan Metzger, Natchaya Pingintha-Durden, Marvin Shaw, Adam R. Vaughan, Xinming Wang, Ruili Wu, Qiang Zhang, and Yanli Zhang
Atmos. Chem. Phys., 20, 8737–8761, https://doi.org/10.5194/acp-20-8737-2020, https://doi.org/10.5194/acp-20-8737-2020, 2020
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Significant air quality problems exist in megacities like Beijing, China. To manage air pollution, legislators need a clear understanding of pollutant emissions. However, emissions inventories have large uncertainties, and reliable field measurements of pollutant emissions are required to constrain them. This work presents the first measurements of traffic-dominated emissions in Beijing which suggest that inventories overestimate these emissions in the region during both winter and summer.
Michael Müller, Peter Graf, Jonas Meyer, Anastasia Pentina, Dominik Brunner, Fernando Perez-Cruz, Christoph Hüglin, and Lukas Emmenegger
Atmos. Meas. Tech., 13, 3815–3834, https://doi.org/10.5194/amt-13-3815-2020, https://doi.org/10.5194/amt-13-3815-2020, 2020
Daniel J. Bryant, William J. Dixon, James R. Hopkins, Rachel E. Dunmore, Kelly L. Pereira, Marvin Shaw, Freya A. Squires, Thomas J. Bannan, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Bin Ouyang, Tianqu Cui, Jason D. Surratt, Di Liu, Zongbo Shi, Roy Harrison, Yele Sun, Weiqi Xu, Alastair C. Lewis, James D. Lee, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 20, 7531–7552, https://doi.org/10.5194/acp-20-7531-2020, https://doi.org/10.5194/acp-20-7531-2020, 2020
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Using the chemical composition of offline filter samples, we report that a large share of oxidized organic aerosol in Beijing during summer is due to isoprene secondary organic aerosol (iSOA). iSOA organosulfates showed a strong correlation with the product of ozone and particulate sulfate. This highlights the role of both photochemistry and the availability of particulate sulfate in heterogeneous reactions and further demonstrates that iSOA formation is controlled by anthropogenic emissions.
Kirsti Ashworth, Silvia Bucci, Peter J. Gallimore, Junghwa Lee, Beth S. Nelson, Alberto Sanchez-Marroquín, Marina B. Schimpf, Paul D. Smith, Will S. Drysdale, Jim R. Hopkins, James D. Lee, Joe R. Pitt, Piero Di Carlo, Radovan Krejci, and James B. McQuaid
Atmos. Chem. Phys., 20, 7193–7216, https://doi.org/10.5194/acp-20-7193-2020, https://doi.org/10.5194/acp-20-7193-2020, 2020
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In July 2017 we flew three research flights around London during European Facility for Airborne Research (EUFAR) training. We made continuous measurements of concentrations of key pollutants (ozone, NOx, aerosol particles, CO, CO2 and methane) and meteorology, and we collected periodic samples of air to analyse for volatile organic compounds. We saw evidence that plumes of pollution from the city, strong local emissions and pollution from distant sources all contribute to regional pollution.
Manuela van Pinxteren, Khanneh Wadinga Fomba, Nadja Triesch, Christian Stolle, Oliver Wurl, Enno Bahlmann, Xianda Gong, Jens Voigtländer, Heike Wex, Tiera-Brandy Robinson, Stefan Barthel, Sebastian Zeppenfeld, Erik Hans Hoffmann, Marie Roveretto, Chunlin Li, Benoit Grosselin, Veronique Daële, Fabian Senf, Dominik van Pinxteren, Malena Manzi, Nicolás Zabalegui, Sanja Frka, Blaženka Gašparović, Ryan Pereira, Tao Li, Liang Wen, Jiarong Li, Chao Zhu, Hui Chen, Jianmin Chen, Björn Fiedler, Wolf von Tümpling, Katie Alana Read, Shalini Punjabi, Alastair Charles Lewis, James Roland Hopkins, Lucy Jane Carpenter, Ilka Peeken, Tim Rixen, Detlef Schulz-Bull, María Eugenia Monge, Abdelwahid Mellouki, Christian George, Frank Stratmann, and Hartmut Herrmann
Atmos. Chem. Phys., 20, 6921–6951, https://doi.org/10.5194/acp-20-6921-2020, https://doi.org/10.5194/acp-20-6921-2020, 2020
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An introduction to a comprehensive field campaign performed at the Cape Verde Atmospheric Observatory regarding ocean–atmosphere interactions is given. Chemical, physical, biological and meteorological techniques were applied, and measurements of bulk water, the sea surface microlayer, cloud water and ambient aerosol particles took place. Oceanic compounds were found to be transferred to atmospheric aerosol and to the cloud level; however, sea spray contributions to CCN and INPs were limited.
Longfei Yu, Eliza Harris, Stephan Henne, Sarah Eggleston, Martin Steinbacher, Lukas Emmenegger, Christoph Zellweger, and Joachim Mohn
Atmos. Chem. Phys., 20, 6495–6519, https://doi.org/10.5194/acp-20-6495-2020, https://doi.org/10.5194/acp-20-6495-2020, 2020
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We observed the isotopic composition of nitrous oxide in the unpolluted air at Jungfraujoch for 5 years. Our results indicate a clear seasonal pattern in the isotopic composition, corresponding with that in atmospheric nitrous oxide levels. This is most likely due to temporal variations in both emission processes and air mass sources for Jungfraujoch. Our findings are of importance to global nitrous oxide modelling and to better understanding of long-term trends in atmospheric nitrous oxide.
William T. Morgan, James D. Allan, Stéphane Bauguitte, Eoghan Darbyshire, Michael J. Flynn, James Lee, Dantong Liu, Ben Johnson, Jim Haywood, Karla M. Longo, Paulo E. Artaxo, and Hugh Coe
Atmos. Chem. Phys., 20, 5309–5326, https://doi.org/10.5194/acp-20-5309-2020, https://doi.org/10.5194/acp-20-5309-2020, 2020
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We flew a large atmospheric research aircraft across a number of different environments in the Amazon basin during the 2012 biomass burning season. Smoke from fires builds up and has a significant impact on weather, climate, health and natural ecosystems. Our goal was to quantify changes in the properties of the smoke emitted by fires as it is transported through the atmosphere. We found that the major control on the properties of the smoke was due to differences in the fires themselves.
Stuart K. Grange, Hanspeter Lötscher, Andrea Fischer, Lukas Emmenegger, and Christoph Hueglin
Atmos. Meas. Tech., 13, 1867–1885, https://doi.org/10.5194/amt-13-1867-2020, https://doi.org/10.5194/amt-13-1867-2020, 2020
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Black carbon (BC) is an important atmospheric pollutant and can be monitored by instruments called aethalometers. A pragmatic data processing technique called the
aethalometer modelcan be used to apportion aethalometer observations into traffic and woodburning components. We present an exploratory data analysis evaluating the aethalometer model and use the outputs for BC trend analysis across Switzerland. The aethalometer model's robustness and utility for such analyses is discussed.
Leigh R. Crilley, Ajit Singh, Louisa J. Kramer, Marvin D. Shaw, Mohammed S. Alam, Joshua S. Apte, William J. Bloss, Lea Hildebrandt Ruiz, Pingqing Fu, Weiqi Fu, Shahzad Gani, Michael Gatari, Evgenia Ilyinskaya, Alastair C. Lewis, David Ng'ang'a, Yele Sun, Rachel C. W. Whitty, Siyao Yue, Stuart Young, and Francis D. Pope
Atmos. Meas. Tech., 13, 1181–1193, https://doi.org/10.5194/amt-13-1181-2020, https://doi.org/10.5194/amt-13-1181-2020, 2020
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There is considerable interest in using low-cost optical particle counters (OPCs) for particle mass measurements; however, there is no agreed upon method with respect to calibration. Here we exploit a number of datasets globally to demonstrate that particle composition and relative humidity are the key factors affecting measured concentrations from a low-cost OPC, and we present a simple correction methodology that corrects for this influence.
Michael Biggart, Jenny Stocker, Ruth M. Doherty, Oliver Wild, Michael Hollaway, David Carruthers, Jie Li, Qiang Zhang, Ruili Wu, Simone Kotthaus, Sue Grimmond, Freya A. Squires, James Lee, and Zongbo Shi
Atmos. Chem. Phys., 20, 2755–2780, https://doi.org/10.5194/acp-20-2755-2020, https://doi.org/10.5194/acp-20-2755-2020, 2020
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Ambient air pollution is a major cause of premature death in China. We examine the street-scale variation of pollutant levels in Beijing using air pollution dispersion and chemistry model ADMS-Urban. Campaign measurements are compared with simulated pollutant levels, providing a valuable means of evaluating the impact of key processes on urban air quality. Air quality modelling at such fine scales is essential for human exposure studies and for informing choices on future emission controls.
Pragati Rai, Markus Furger, Jay G. Slowik, Francesco Canonaco, Roman Fröhlich, Christoph Hüglin, María Cruz Minguillón, Krag Petterson, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 1657–1674, https://doi.org/10.5194/acp-20-1657-2020, https://doi.org/10.5194/acp-20-1657-2020, 2020
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A source apportionment study of hourly resolved elements in PM10 measured at a traffic-influenced site in Härkingen, Switzerland, using positive matrix factorization (PMF) and multilinear engine-2 (ME-2) offered resolution of robust and unambiguous factor profiles and contributions. We show that the rotational control available in ME-2 provides a means for treating extreme events such as fireworks within a PMF analysis.
Marco Pandolfi, Dennis Mooibroek, Philip Hopke, Dominik van Pinxteren, Xavier Querol, Hartmut Herrmann, Andrés Alastuey, Olivier Favez, Christoph Hüglin, Esperanza Perdrix, Véronique Riffault, Stéphane Sauvage, Eric van der Swaluw, Oksana Tarasova, and Augustin Colette
Atmos. Chem. Phys., 20, 409–429, https://doi.org/10.5194/acp-20-409-2020, https://doi.org/10.5194/acp-20-409-2020, 2020
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In the last scientific assessment report from the LRTAP Convention, it is stated that because non-urban sources are often major contributors to urban pollution, many cities will be unable to meet WHO guideline levels for air pollutants through local action alone. Consequently, it is very important to estimate how much the local and non-local sources contribute to urban pollution in order to design global strategies to reduce the levels of pollutants in European cities.
James Brean, Roy M. Harrison, Zongbo Shi, David C. S. Beddows, W. Joe F. Acton, C. Nicholas Hewitt, Freya A. Squires, and James Lee
Atmos. Chem. Phys., 19, 14933–14947, https://doi.org/10.5194/acp-19-14933-2019, https://doi.org/10.5194/acp-19-14933-2019, 2019
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Measurements of highly oxidized molecules measured during a summer campaign in Beijing are presented. These molecules represent an intermediary between gas-phase chemicals from which they are formed and airborne particles which form from them. Conclusions are drawn as to the factors affecting the formation of new particles within the Beijing atmosphere.
Giulia Stefenelli, Veronika Pospisilova, Felipe D. Lopez-Hilfiker, Kaspar R. Daellenbach, Christoph Hüglin, Yandong Tong, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 19, 14825–14848, https://doi.org/10.5194/acp-19-14825-2019, https://doi.org/10.5194/acp-19-14825-2019, 2019
Leigh R. Crilley, Louisa J. Kramer, Bin Ouyang, Jun Duan, Wenqian Zhang, Shengrui Tong, Maofa Ge, Ke Tang, Min Qin, Pinhua Xie, Marvin D. Shaw, Alastair C. Lewis, Archit Mehra, Thomas J. Bannan, Stephen D. Worrall, Michael Priestley, Asan Bacak, Hugh Coe, James Allan, Carl J. Percival, Olalekan A. M. Popoola, Roderic L. Jones, and William J. Bloss
Atmos. Meas. Tech., 12, 6449–6463, https://doi.org/10.5194/amt-12-6449-2019, https://doi.org/10.5194/amt-12-6449-2019, 2019
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Nitrous acid (HONO) is key species for understanding tropospheric chemistry, yet accurate and precise measurements are challenging. Here we report an inter–comparison exercise of a number of instruments that measured HONO in a highly polluted location (Beijing). All instruments agreed on the temporal trends yet displayed divergence in absolute concentrations. The cause of this divergence was unclear, but it may in part be due to spatial variability in instrument location.
Christoph Zellweger, Rainer Steinbrecher, Olivier Laurent, Haeyoung Lee, Sumin Kim, Lukas Emmenegger, Martin Steinbacher, and Brigitte Buchmann
Atmos. Meas. Tech., 12, 5863–5878, https://doi.org/10.5194/amt-12-5863-2019, https://doi.org/10.5194/amt-12-5863-2019, 2019
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We analysed results obtained through CO and N2O performance audits conducted within the framework of the Global Atmosphere Watch (GAW) quality management system of the World Meteorology Organization (WMO). The results reveal that current spectroscopic measurement techniques have clear advantages with respect to data quality objectives compared to more traditional methods. Further, they allow for a smooth continuation of historic CO and N2O time series.
Erkan Ibraim, Benjamin Wolf, Eliza Harris, Rainer Gasche, Jing Wei, Longfei Yu, Ralf Kiese, Sarah Eggleston, Klaus Butterbach-Bahl, Matthias Zeeman, Béla Tuzson, Lukas Emmenegger, Johan Six, Stephan Henne, and Joachim Mohn
Biogeosciences, 16, 3247–3266, https://doi.org/10.5194/bg-16-3247-2019, https://doi.org/10.5194/bg-16-3247-2019, 2019
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Nitrous oxide (N2O) is an important greenhouse gas and the major stratospheric ozone-depleting substance; therefore, mitigation of anthropogenic N2O emissions is needed. To trace N2O-emitting source processes, in this study, we observed N2O isotopocules above an intensively managed grassland research site with a recently developed laser spectroscopy method. Our results indicate that the domain of denitrification or nitrifier denitrification was the major N2O source.
Joseph R. Pitt, Grant Allen, Stéphane J.-B. Bauguitte, Martin W. Gallagher, James D. Lee, Will Drysdale, Beth Nelson, Alistair J. Manning, and Paul I. Palmer
Atmos. Chem. Phys., 19, 8931–8945, https://doi.org/10.5194/acp-19-8931-2019, https://doi.org/10.5194/acp-19-8931-2019, 2019
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This paper presents a new method to assess inventory estimates of greenhouse gas and air pollutant emissions for large cities and their surrounding regions. A case study using data sampled by a research aircraft around London was used to test the method. We found that the UK national inventory agrees with our observations for CO but needed lower emissions for CH4 to agree with the measured data. Repeated studies could help determine how these emissions vary on different timescales.
Atallah Elzein, Rachel E. Dunmore, Martyn W. Ward, Jacqueline F. Hamilton, and Alastair C. Lewis
Atmos. Chem. Phys., 19, 8741–8758, https://doi.org/10.5194/acp-19-8741-2019, https://doi.org/10.5194/acp-19-8741-2019, 2019
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This article investigates the chemical composition of fine particulate matter (PM2.5) in Beijing, China, in winter 2016. It includes the identification and quantification of 35 polycyclic aromatic compounds. The results include their distribution between daytime and night-time. They were correlated with the gas-phase concentrations of atmospheric oxidants. Major emission sources were identified, and the cancer risk associated with particle inhalation in Beijing was estimated.
Jonathan W. Taylor, Sophie L. Haslett, Keith Bower, Michael Flynn, Ian Crawford, James Dorsey, Tom Choularton, Paul J. Connolly, Valerian Hahn, Christiane Voigt, Daniel Sauer, Régis Dupuy, Joel Brito, Alfons Schwarzenboeck, Thierry Bourriane, Cyrielle Denjean, Phil Rosenberg, Cyrille Flamant, James D. Lee, Adam R. Vaughan, Peter G. Hill, Barbara Brooks, Valéry Catoire, Peter Knippertz, and Hugh Coe
Atmos. Chem. Phys., 19, 8503–8522, https://doi.org/10.5194/acp-19-8503-2019, https://doi.org/10.5194/acp-19-8503-2019, 2019
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Low-level clouds cover a wide area of southern West Africa (SWA) and play an important role in the region's climate, reflecting sunlight away from the surface. We performed aircraft measurements of aerosols and clouds over SWA during the 2016 summer monsoon and found pollution, and polluted clouds, across the whole region. Smoke from biomass burning in Central Africa is transported to West Africa, causing a polluted background which limits the effect of local pollution on cloud properties.
Lu Qi, Mindong Chen, Giulia Stefenelli, Veronika Pospisilova, Yandong Tong, Amelie Bertrand, Christoph Hueglin, Xinlei Ge, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 19, 8037–8062, https://doi.org/10.5194/acp-19-8037-2019, https://doi.org/10.5194/acp-19-8037-2019, 2019
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Current understanding of OA sources is limited by the chemical resolution of existing real-time measurement technology. We describe the first wintertime deployment of a novel extractive electrospray ionization time-of-flight mass spectrometer, which provides near-molecular OA measurements with high time resolution. We show that biomass combustion strongly influences winter OA. Via factor analysis, aging-dependent signatures and time contributions of biomass-combustion-derived OA are resolved.
Zongbo Shi, Tuan Vu, Simone Kotthaus, Roy M. Harrison, Sue Grimmond, Siyao Yue, Tong Zhu, James Lee, Yiqun Han, Matthias Demuzere, Rachel E. Dunmore, Lujie Ren, Di Liu, Yuanlin Wang, Oliver Wild, James Allan, W. Joe Acton, Janet Barlow, Benjamin Barratt, David Beddows, William J. Bloss, Giulia Calzolai, David Carruthers, David C. Carslaw, Queenie Chan, Lia Chatzidiakou, Yang Chen, Leigh Crilley, Hugh Coe, Tie Dai, Ruth Doherty, Fengkui Duan, Pingqing Fu, Baozhu Ge, Maofa Ge, Daobo Guan, Jacqueline F. Hamilton, Kebin He, Mathew Heal, Dwayne Heard, C. Nicholas Hewitt, Michael Hollaway, Min Hu, Dongsheng Ji, Xujiang Jiang, Rod Jones, Markus Kalberer, Frank J. Kelly, Louisa Kramer, Ben Langford, Chun Lin, Alastair C. Lewis, Jie Li, Weijun Li, Huan Liu, Junfeng Liu, Miranda Loh, Keding Lu, Franco Lucarelli, Graham Mann, Gordon McFiggans, Mark R. Miller, Graham Mills, Paul Monk, Eiko Nemitz, Fionna O'Connor, Bin Ouyang, Paul I. Palmer, Carl Percival, Olalekan Popoola, Claire Reeves, Andrew R. Rickard, Longyi Shao, Guangyu Shi, Dominick Spracklen, David Stevenson, Yele Sun, Zhiwei Sun, Shu Tao, Shengrui Tong, Qingqing Wang, Wenhua Wang, Xinming Wang, Xuejun Wang, Zifang Wang, Lianfang Wei, Lisa Whalley, Xuefang Wu, Zhijun Wu, Pinhua Xie, Fumo Yang, Qiang Zhang, Yanli Zhang, Yuanhang Zhang, and Mei Zheng
Atmos. Chem. Phys., 19, 7519–7546, https://doi.org/10.5194/acp-19-7519-2019, https://doi.org/10.5194/acp-19-7519-2019, 2019
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APHH-Beijing is a collaborative international research programme to study the sources, processes and health effects of air pollution in Beijing. This introduction to the special issue provides an overview of (i) the APHH-Beijing programme, (ii) the measurement and modelling activities performed as part of it and (iii) the air quality and meteorological conditions during joint intensive field campaigns as a core activity within APHH-Beijing.
Dantong Liu, Rutambhara Joshi, Junfeng Wang, Chenjie Yu, James D. Allan, Hugh Coe, Michael J. Flynn, Conghui Xie, James Lee, Freya Squires, Simone Kotthaus, Sue Grimmond, Xinlei Ge, Yele Sun, and Pingqing Fu
Atmos. Chem. Phys., 19, 6749–6769, https://doi.org/10.5194/acp-19-6749-2019, https://doi.org/10.5194/acp-19-6749-2019, 2019
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This study provides source attribution and characterization of BC in the Beijing urban environment in both winter and summer. For the first time, the physically and chemically based source apportionments are compared to evaluate the primary source contribution and secondary processing of BC-containing particles. A method is proposed to isolate the BC from the transportation sector and coal combustion sources.
Karl Espen Yttri, David Simpson, Robert Bergström, Gyula Kiss, Sönke Szidat, Darius Ceburnis, Sabine Eckhardt, Christoph Hueglin, Jacob Klenø Nøjgaard, Cinzia Perrino, Ignazio Pisso, Andre Stephan Henry Prevot, Jean-Philippe Putaud, Gerald Spindler, Milan Vana, Yan-Lin Zhang, and Wenche Aas
Atmos. Chem. Phys., 19, 4211–4233, https://doi.org/10.5194/acp-19-4211-2019, https://doi.org/10.5194/acp-19-4211-2019, 2019
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Carbonaceous aerosols from natural sources were abundant regardless of season. Residential wood burning (RWB) emissions were occasionally equally as large as or larger than of fossil-fuel sources, depending on season and region. RWB emissions are poorly constrained; thus emissions inventories need improvement. Harmonizing emission factors between countries is likely the most important step to improve model calculations for biomass burning emissions and European PM2.5 concentrations in general.
Kate R. Smith, Peter M. Edwards, Peter D. Ivatt, James D. Lee, Freya Squires, Chengliang Dai, Richard E. Peltier, Mat J. Evans, Yele Sun, and Alastair C. Lewis
Atmos. Meas. Tech., 12, 1325–1336, https://doi.org/10.5194/amt-12-1325-2019, https://doi.org/10.5194/amt-12-1325-2019, 2019
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Clusters of low-cost, low-power atmospheric gas sensors were built into a sensor instrument to monitor NO2 and O3 in Beijing, alongside reference instruments, aiming to improve the reliability of sensor measurements. Clustering identical sensors and using the median sensor signal was used to minimize drift over short and medium timescales. Three different machine learning techniques were used for all the sensor data in an attempt to correct for cross-interferences, which worked to some degree.
Lu Hu, Christoph A. Keller, Michael S. Long, Tomás Sherwen, Benjamin Auer, Arlindo Da Silva, Jon E. Nielsen, Steven Pawson, Matthew A. Thompson, Atanas L. Trayanov, Katherine R. Travis, Stuart K. Grange, Mat J. Evans, and Daniel J. Jacob
Geosci. Model Dev., 11, 4603–4620, https://doi.org/10.5194/gmd-11-4603-2018, https://doi.org/10.5194/gmd-11-4603-2018, 2018
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We present a full-year online global simulation of tropospheric chemistry at 12.5 km resolution. To the best of our knowledge, such a resolution in a state-of-the-science global simulation of tropospheric chemistry is unprecedented. This simulation will serve as the Nature Run for observing system simulation experiments to support the future geostationary satellite constellation for tropospheric chemistry, and can also be used for various air quality applications.
Fernando Santos, Karla Longo, Alex Guenther, Saewung Kim, Dasa Gu, Dave Oram, Grant Forster, James Lee, James Hopkins, Joel Brito, and Saulo Freitas
Atmos. Chem. Phys., 18, 12715–12734, https://doi.org/10.5194/acp-18-12715-2018, https://doi.org/10.5194/acp-18-12715-2018, 2018
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We investigated the impact of biomass burning on the chemical composition of trace gases in the Amazon. The findings corroborate the influence of biomass burning activity not only on direct emissions of particulate matter but also on the oxidative capacity to produce secondary organic aerosol. The scientists plan to use this information to improve the numerical model simulation with a better representativeness of the chemical processes, which can impact on global climate prediction.
Wei Zhou, Jian Zhao, Bin Ouyang, Archit Mehra, Weiqi Xu, Yuying Wang, Thomas J. Bannan, Stephen D. Worrall, Michael Priestley, Asan Bacak, Qi Chen, Conghui Xie, Qingqing Wang, Junfeng Wang, Wei Du, Yingjie Zhang, Xinlei Ge, Penglin Ye, James D. Lee, Pingqing Fu, Zifa Wang, Douglas Worsnop, Roderic Jones, Carl J. Percival, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 18, 11581–11597, https://doi.org/10.5194/acp-18-11581-2018, https://doi.org/10.5194/acp-18-11581-2018, 2018
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We present measurements of gas-phase N2O5 and ClNO2 by ToF-CIMS during summer in urban Beijing as part of the APHH campaign. High reactivity of N2O5 indicative of active nocturnal chemistry was observed. The lifetime of N2O5 as a function of aerosol surface area and relative humidity was characterized, and N2O5 uptake coefficients were estimated. We also found that the N2O5 loss in this study is mainly attributed to its indirect loss via reactions of NO3 with VOCs and NO.
Prasad Kasibhatla, Tomás Sherwen, Mathew J. Evans, Lucy J. Carpenter, Chris Reed, Becky Alexander, Qianjie Chen, Melissa P. Sulprizio, James D. Lee, Katie A. Read, William Bloss, Leigh R. Crilley, William C. Keene, Alexander A. P. Pszenny, and Alma Hodzic
Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, https://doi.org/10.5194/acp-18-11185-2018, 2018
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Recent measurements of NOx and HONO suggest that photolysis of particulate nitrate in sea-salt aerosols is important in terms of marine boundary layer oxidant chemistry. We present the first global-scale assessment of the significance of this new chemical pathway for NOx, O3, and OH in the marine boundary layer. We also present a preliminary assessment of the potential impact of photolysis of particulate nitrate associated with other aerosol types on continental boundary layer chemistry.
Alessandro Bigi, Michael Mueller, Stuart K. Grange, Grazia Ghermandi, and Christoph Hueglin
Atmos. Meas. Tech., 11, 3717–3735, https://doi.org/10.5194/amt-11-3717-2018, https://doi.org/10.5194/amt-11-3717-2018, 2018
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Low cost sensors for monitoring atmospheric pollution are growing in popularity worldwide. Nonetheless, the expectations from these devices were seldom met, thus urging for more research. This study focuses on sensor performance within the realistic framework of an initial calibration next to a reference instrument and the subsequent distant deployment. Within this framework, we assessed the uncertainty of these sensors and their suitability to map intra-urban gradients of NO/NO2.
P. Morten Hundt, Michael Müller, Markus Mangold, Béla Tuzson, Philipp Scheidegger, Herbert Looser, Christoph Hüglin, and Lukas Emmenegger
Atmos. Meas. Tech., 11, 2669–2681, https://doi.org/10.5194/amt-11-2669-2018, https://doi.org/10.5194/amt-11-2669-2018, 2018
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NO2 is a pollutant that regularly exceeds its limit values in European cities. We developed a compact, mobile laser spectrometer that measures NO2 concentrations and installed it on a tram in Zurich. Mobile operation resulted in NO2 concentration data with high spatio-temporal resolution. The data were validated against fixed air-quality monitoring sites and provided detailed insights into the spatio-temporal concentration distribution of NO2 in an urban environment.
Stuart K. Grange, David C. Carslaw, Alastair C. Lewis, Eirini Boleti, and Christoph Hueglin
Atmos. Chem. Phys., 18, 6223–6239, https://doi.org/10.5194/acp-18-6223-2018, https://doi.org/10.5194/acp-18-6223-2018, 2018
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Weather (meteorology) has a strong effect on air quality; if not accounted for, there is uncertainty surrounding what drives features in air quality time series. We present a machine learning approach to account for meteorology using PM10 data in Switzerland. With the exception of one site, all Swiss normalised PM10 trends were found to significantly decrease, which validates air quality management efforts. The machine learning models were interpreted to investigate interesting processes.
Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Benjamin Chazeau, Gary A. Salazar, Soenke Szidat, Jean-Luc Jaffrezo, Christoph Hueglin, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 6187–6206, https://doi.org/10.5194/acp-18-6187-2018, https://doi.org/10.5194/acp-18-6187-2018, 2018
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Carbonaceous aerosols are related to adverse human health effects, which depend on the aerosol chemical composition and size. Here, we combine aerosol mass spectrometry and radiocarbon measurements of size-resolved samples collected over a long term to identify the origins of primary and secondary carbonaceous aerosols in the fine and coarse modes.
Amy K. Hodgson, William T. Morgan, Sebastian O'Shea, Stéphane Bauguitte, James D. Allan, Eoghan Darbyshire, Michael J. Flynn, Dantong Liu, James Lee, Ben Johnson, Jim M. Haywood, Karla M. Longo, Paulo E. Artaxo, and Hugh Coe
Atmos. Chem. Phys., 18, 5619–5638, https://doi.org/10.5194/acp-18-5619-2018, https://doi.org/10.5194/acp-18-5619-2018, 2018
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We flew a large atmospheric research aircraft across a number of different biomass burning environments in the Amazon Basin in September and October 2012. In this paper, we focus on smoke sampled very close to fresh fires (only 600–900 m above the fires and smoke that was 4–6 min old) to examine the chemical components that make up the smoke and their abundance. We found substantial differences in the emitted smoke that are due to the fuel type and combustion processes driving the fires.
James D. Lee, Stephen D. Mobbs, Axel Wellpott, Grant Allen, Stephane J.-B. Bauguitte, Ralph R. Burton, Richard Camilli, Hugh Coe, Rebecca E. Fisher, James L. France, Martin Gallagher, James R. Hopkins, Mathias Lanoiselle, Alastair C. Lewis, David Lowry, Euan G. Nisbet, Ruth M. Purvis, Sebastian O'Shea, John A. Pyle, and Thomas B. Ryerson
Atmos. Meas. Tech., 11, 1725–1739, https://doi.org/10.5194/amt-11-1725-2018, https://doi.org/10.5194/amt-11-1725-2018, 2018
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This work describes measurements, made from an aircraft platform, of the emission of methane and other organic gases from an uncontrolled leak from an oil platform in the North Sea (Total Elgin). The measurements made helped the platform operators to devise a strategy for repairing the leak and serve as a methodology for assessing future similar incidents.
Fabian Schoenenberger, Stephan Henne, Matthias Hill, Martin K. Vollmer, Giorgos Kouvarakis, Nikolaos Mihalopoulos, Simon O'Doherty, Michela Maione, Lukas Emmenegger, Thomas Peter, and Stefan Reimann
Atmos. Chem. Phys., 18, 4069–4092, https://doi.org/10.5194/acp-18-4069-2018, https://doi.org/10.5194/acp-18-4069-2018, 2018
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Anthropogenic halocarbon emissions contribute to stratospheric ozone depletion and global warming. We measured atmospheric halocarbons for 6 months on Crete to extend the coverage of the existing observation network to the Eastern Mediterranean. The derived emission estimates showed a contribution of 16.8 % (13.6–23.3 %) and 53.2 % (38.1–84.2 %) of this region to the total HFC and HCFC emissions of the analyzed European domain and a reduction of the underlying uncertainties by 40–80 %.
Jacob T. Shaw, Richard T. Lidster, Danny R. Cryer, Noelia Ramirez, Fiona C. Whiting, Graham A. Boustead, Lisa K. Whalley, Trevor Ingham, Andrew R. Rickard, Rachel E. Dunmore, Dwayne E. Heard, Ally C. Lewis, Lucy J. Carpenter, Jacqui F. Hamilton, and Terry J. Dillon
Atmos. Chem. Phys., 18, 4039–4054, https://doi.org/10.5194/acp-18-4039-2018, https://doi.org/10.5194/acp-18-4039-2018, 2018
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The lifetime of a chemical in the atmosphere is largely governed by the rate of its reaction with the hydroxyl radical (OH). Measurements of rates for many of the thousands of identified volatile organic compounds (VOCs) have yet to be determined experimentally. We have developed a new technique for the rapid determination of gas-phase rate coefficients for the simultaneous reactions between multiple VOCs and OH. The method is tasted across a range of scenarios and is used to derive new values.
Daniel Stone, Tomás Sherwen, Mathew J. Evans, Stewart Vaughan, Trevor Ingham, Lisa K. Whalley, Peter M. Edwards, Katie A. Read, James D. Lee, Sarah J. Moller, Lucy J. Carpenter, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 3541–3561, https://doi.org/10.5194/acp-18-3541-2018, https://doi.org/10.5194/acp-18-3541-2018, 2018
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Halogen chemistry in the troposphere impacts oxidising capacity, but model studies assessing the nature of these impacts can vary according to the model framework used. In this work we present simulations of OH and HO2 radicals using both box and global model frameworks, and compare to observations made at the Cape Verde Atmospheric Observatory. We highlight, and rationalise, differences between the model frameworks.
Lisa K. Whalley, Daniel Stone, Rachel Dunmore, Jacqueline Hamilton, James R. Hopkins, James D. Lee, Alastair C. Lewis, Paul Williams, Jörg Kleffmann, Sebastian Laufs, Robert Woodward-Massey, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 2547–2571, https://doi.org/10.5194/acp-18-2547-2018, https://doi.org/10.5194/acp-18-2547-2018, 2018
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This paper presents the first radical observations made in London and subsequent model comparisons. This work highlights that there are uncertainties in the degradation mechanism of complex biogenic and diesel-related VOC species under low-NOx conditions and under high-NOx conditions there is a missing source of RO2 radicals. The impact of these model uncertainties on in situ ozone production as a function of NOx is discussed.
Leigh R. Crilley, Marvin Shaw, Ryan Pound, Louisa J. Kramer, Robin Price, Stuart Young, Alastair C. Lewis, and Francis D. Pope
Atmos. Meas. Tech., 11, 709–720, https://doi.org/10.5194/amt-11-709-2018, https://doi.org/10.5194/amt-11-709-2018, 2018
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The affordability and small size of low-cost particle sensors make them attractive for air pollution experiments that require multiple instruments, or take place in hard-to-access locations or low-income countries. For any sensor to be useful, its accuracy and precision need to be known. We evaluate the Alphasense OPC-N2 for monitoring airborne particles at typical UK urban background sites. The devices were found to be accurate provided they are correctly calibrated.
Kaspar R. Daellenbach, Giulia Stefenelli, Carlo Bozzetti, Athanasia Vlachou, Paola Fermo, Raquel Gonzalez, Andrea Piazzalunga, Cristina Colombi, Francesco Canonaco, Christoph Hueglin, Anne Kasper-Giebl, Jean-Luc Jaffrezo, Federico Bianchi, Jay G. Slowik, Urs Baltensperger, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 13265–13282, https://doi.org/10.5194/acp-17-13265-2017, https://doi.org/10.5194/acp-17-13265-2017, 2017
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We present offline AMS analyses for the organic aerosol (OA) in PM10 at nine sites in central Europe for 2013. Primary OA is separated into traffic, cooking, and wood-burning components. A factor explaining sulfur-containing ions, with an event-driven time series, is also separated. We observe enhanced production of secondary OA (SOA) in summer, following biogenic emissions with temperature. In winter a SOA component is dominant, which correlates with anthropogenic inorganic species.
Michael Mueller, Jonas Meyer, and Christoph Hueglin
Atmos. Meas. Tech., 10, 3783–3799, https://doi.org/10.5194/amt-10-3783-2017, https://doi.org/10.5194/amt-10-3783-2017, 2017
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This study describes the design of a sensor unit featuring NO2 and O3 sensors for applications such as ambient air quality monitoring. The paper presents the sensor calibration, the testing procedure and the long-term deployment of the sensor units in the city of Zurich.
Main conclusions are the necessity of a proper mathematical description of the sensors as well as a concept to monitor sensor performance during operation, e.g. by linking low-cost sensors to traditional infrastructure.
Antoine Berchet, Katrin Zink, Dietmar Oettl, Jürg Brunner, Lukas Emmenegger, and Dominik Brunner
Geosci. Model Dev., 10, 3441–3459, https://doi.org/10.5194/gmd-10-3441-2017, https://doi.org/10.5194/gmd-10-3441-2017, 2017
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We evaluate a new cost-effective method to simulate pollutant dispersion at high resolution on a city-wide domain. The method is based on a catalogue of reference simulations matched to weather observations to produce a sequence of hourly pollution maps. A total of 2 years of simulations are compared with continuous measurements and passive NO2 samplers in the city of Zurich. Spatial and temporal variability proved to be very well reproduced by the method.
Yann Poltera, Giovanni Martucci, Martine Collaud Coen, Maxime Hervo, Lukas Emmenegger, Stephan Henne, Dominik Brunner, and Alexander Haefele
Atmos. Chem. Phys., 17, 10051–10070, https://doi.org/10.5194/acp-17-10051-2017, https://doi.org/10.5194/acp-17-10051-2017, 2017
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We present the PathfinderTURB algorithm for the analysis of ceilometer backscatter data and the real-time detection of the vertical structure of the planetary boundary layer. PathfinderTURB has been applied to 1 year of data measured by two ceilometers operated at two Swiss stations: the Aerological Observatory of Payerne on the Swiss plateau, and the Alpine Jungfraujoch observatory. The study shows that aerosols from the boundary layer significantly influence the air measured at Jungfraujoch.
Markus Furger, María Cruz Minguillón, Varun Yadav, Jay G. Slowik, Christoph Hüglin, Roman Fröhlich, Krag Petterson, Urs Baltensperger, and André S. H. Prévôt
Atmos. Meas. Tech., 10, 2061–2076, https://doi.org/10.5194/amt-10-2061-2017, https://doi.org/10.5194/amt-10-2061-2017, 2017
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An Xact 625 Ambient Metals Monitor was tested during a 3-week summer field campaign at a rural, traffic-influenced site in Switzerland. The objective was to characterize the operation of the instrument, evaluate the data quality by intercomparison with other independent measurements, and test its applicability for aerosol source quantification. The results demonstrate significant advantages compared to traditional elemental analysis methods, with some desirable improvements.
Julien G. Anet, Martin Steinbacher, Laura Gallardo, Patricio A. Velásquez Álvarez, Lukas Emmenegger, and Brigitte Buchmann
Atmos. Chem. Phys., 17, 6477–6492, https://doi.org/10.5194/acp-17-6477-2017, https://doi.org/10.5194/acp-17-6477-2017, 2017
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There are less long-term surface ozone measurements on the Southern than on the Northern Hemisphere, which makes it difficult to thoroughly understand global ozone chemistry. We have analyzed a new, 20-year-long ozone dataset measured at 2200 m asl at El Tololo, Chile, and show that the annual cycle of ozone is mainly driven by ozone transport from the stratosphere to the troposphere. As well, we illustrate that the timing of the annual maximum is regressing to earlier in the year.
Katie A. Read, Luis M. Neves, Lucy J. Carpenter, Alastair C. Lewis, Zoe L. Fleming, and John Kentisbeer
Atmos. Chem. Phys., 17, 5393–5406, https://doi.org/10.5194/acp-17-5393-2017, https://doi.org/10.5194/acp-17-5393-2017, 2017
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This paper presents 4 years of total gaseous mercury data obtained from measurements made at the Cape Verde Atmospheric Observatory, a subtropical site in the Atlantic Ocean. The data show a clear decreasing trend in the overall concentrations but in air from sub-Saharan Africa the trend is less significant and the data more variable. We attribute this result to an influence from artisanal small-scale gold mining in this region, a source for which there is uncertain information.
Peter Zotter, Hanna Herich, Martin Gysel, Imad El-Haddad, Yanlin Zhang, Griša Močnik, Christoph Hüglin, Urs Baltensperger, Sönke Szidat, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 4229–4249, https://doi.org/10.5194/acp-17-4229-2017, https://doi.org/10.5194/acp-17-4229-2017, 2017
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Most studies use a single Ångström exponent for wood burning (αWB) and traffic (αTR) emissions in the Aethalometer model, used for source apportionment of black carbon, derived from previous work. However, accurate determination of the α values is currently lacking. Comparing radiocarbon measurements (14C) with the Aehtalometer model, good agreement was found, indicating that the Aethalometer model reproduces reasonably well the 14C results using our best estimate of a single αWB and αTR.
Chris Reed, Mathew J. Evans, Leigh R. Crilley, William J. Bloss, Tomás Sherwen, Katie A. Read, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 17, 4081–4092, https://doi.org/10.5194/acp-17-4081-2017, https://doi.org/10.5194/acp-17-4081-2017, 2017
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The source of ozone-depleting compounds in the remote troposphere has been thought to be long-range transport of secondary pollutants such as organic nitrates. Processing of organic nitrates to nitric acid and subsequent deposition on surfaces in the atmosphere was thought to remove these nitrates from the ozone–NOx–HOx cycle. We found through observation of NOx in the remote tropical troposphere at the Cape Verde Observatory that surface nitrates can be released back into the atmosphere.
Eleonora Aruffo, Fabio Biancofiore, Piero Di Carlo, Marcella Busilacchio, Marco Verdecchia, Barbara Tomassetti, Cesare Dari-Salisburgo, Franco Giammaria, Stephane Bauguitte, James Lee, Sarah Moller, James Hopkins, Shalini Punjabi, Stephen J. Andrews, Alistair C. Lewis, Paul I. Palmer, Edward Hyer, Michael Le Breton, and Carl Percival
Atmos. Meas. Tech., 9, 5591–5606, https://doi.org/10.5194/amt-9-5591-2016, https://doi.org/10.5194/amt-9-5591-2016, 2016
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During the BORTAS aircraft campaign, we measured NO2 and their oxidtation products (as peroxy nitrates) with a custom laser-induced fluorescence instrument. Because of the high correlation between known pyrogenic tracers (i.e., carbon monoxide) and peroxy nitrates, we provide two methods to use these species for the identification of biomass burning (BB) plumes. Using an artifical neural network, we improved the BB identification taking into account of a meteorological parameter (pressure).
Christoph Zellweger, Lukas Emmenegger, Mohd Firdaus, Juha Hatakka, Martin Heimann, Elena Kozlova, T. Gerard Spain, Martin Steinbacher, Marcel V. van der Schoot, and Brigitte Buchmann
Atmos. Meas. Tech., 9, 4737–4757, https://doi.org/10.5194/amt-9-4737-2016, https://doi.org/10.5194/amt-9-4737-2016, 2016
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We compared instruments using more traditional techniques for measuring CO2 and CH4 at different stations of the Global Atmosphere Watch (GAW) programme with a travelling instrument using a spectroscopic technique. Our results show that the newer analytical techniques have clear advantages over the traditional methods which will lead to the improved accuracy of atmospheric CO2 and CH4 measurement. The work was carried out in the framework of the GAW quality assurance/quality control system.
Thomas Röckmann, Simon Eyer, Carina van der Veen, Maria E. Popa, Béla Tuzson, Guillaume Monteil, Sander Houweling, Eliza Harris, Dominik Brunner, Hubertus Fischer, Giulia Zazzeri, David Lowry, Euan G. Nisbet, Willi A. Brand, Jaroslav M. Necki, Lukas Emmenegger, and Joachim Mohn
Atmos. Chem. Phys., 16, 10469–10487, https://doi.org/10.5194/acp-16-10469-2016, https://doi.org/10.5194/acp-16-10469-2016, 2016
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A dual isotope ratio mass spectrometric system (IRMS) and a quantum cascade laser absorption spectroscopy (QCLAS)-based technique were deployed at the Cabauw experimental site for atmospheric research (CESAR) in the Netherlands and performed in situ, high-frequency (approx. hourly) measurements for a period of more than 5 months, yielding a combined dataset with more than 2500 measurements of both δ13C and δD.
Chris Reed, Charlotte A. Brumby, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Paul W. Seakins, James D. Lee, and Lucy J. Carpenter
Atmos. Meas. Tech., 9, 2483–2495, https://doi.org/10.5194/amt-9-2483-2016, https://doi.org/10.5194/amt-9-2483-2016, 2016
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A new method of measuring nitrous acid (HONO), a potent mediator of air quality in the atmosphere as well as an important indoor pollutant, is presented. The new method relies on simple, proven techniques already widely applied to other atmospheric compounds. The technique can be retrofitted to existing analysers at minimal cost, or developed into instruments capable of very fast measurement which allow for more complex analysis of the behaviour of HONO.
Andrés Alastuey, Xavier Querol, Wenche Aas, Franco Lucarelli, Noemí Pérez, Teresa Moreno, Fabrizia Cavalli, Hans Areskoug, Violeta Balan, Maria Catrambone, Darius Ceburnis, José C. Cerro, Sébastien Conil, Lusine Gevorgyan, Christoph Hueglin, Kornelia Imre, Jean-Luc Jaffrezo, Sarah R. Leeson, Nikolaos Mihalopoulos, Marta Mitosinkova, Colin D. O'Dowd, Jorge Pey, Jean-Philippe Putaud, Véronique Riffault, Anna Ripoll, Jean Sciare, Karine Sellegri, Gerald Spindler, and Karl Espen Yttri
Atmos. Chem. Phys., 16, 6107–6129, https://doi.org/10.5194/acp-16-6107-2016, https://doi.org/10.5194/acp-16-6107-2016, 2016
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Mineral dust content in PM10 was analysed at 20 regional background sites across Europe. Higher dust loadings were observed at most sites in summer, with the most elevated concentrations in the southern- and easternmost countries, due to external and regional sources. Saharan dust outbreaks impacted western and central European in summer and eastern Mediterranean sites in winter. The spatial distribution of some metals reveals the influence of specific anthropogenic sources on a regional scale.
Chris Reed, Mathew J. Evans, Piero Di Carlo, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 16, 4707–4724, https://doi.org/10.5194/acp-16-4707-2016, https://doi.org/10.5194/acp-16-4707-2016, 2016
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The self-cleaning capacity of the atmosphere in places like Antarctica can be measured by quantifying very low amounts of combustion products that exist in a well-known ratio. When this ratio deviates from 1 it points to the existence of unknown compounds. Several unknown compounds have been theorized to exist but never measured. We have found the method for measuring the ratio of combustion products suffers a bias in remote places, which when taken into account disproves any unknown compounds.
Stephan Henne, Dominik Brunner, Brian Oney, Markus Leuenberger, Werner Eugster, Ines Bamberger, Frank Meinhardt, Martin Steinbacher, and Lukas Emmenegger
Atmos. Chem. Phys., 16, 3683–3710, https://doi.org/10.5194/acp-16-3683-2016, https://doi.org/10.5194/acp-16-3683-2016, 2016
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Greenhouse gas emissions can be assessed by "top-down" methods that combine atmospheric observations, a transport model and a mathematical optimisation framework. Here, we apply such a top-down method to the methane emissions of Switzerland, utilising observations from the recently installed CarboCount-CH network. Our Swiss total emissions largely agree with those of the national "bottom-up" inventory, whereas regional differences suggest lower than reported emissions from manure handling.
Marcella Busilacchio, Piero Di Carlo, Eleonora Aruffo, Fabio Biancofiore, Cesare Dari Salisburgo, Franco Giammaria, Stephane Bauguitte, James Lee, Sarah Moller, James Hopkins, Shalini Punjabi, Stephen Andrews, Alistair C. Lewis, Mark Parrington, Paul I. Palmer, Edward Hyer, and Glenn M. Wolfe
Atmos. Chem. Phys., 16, 3485–3497, https://doi.org/10.5194/acp-16-3485-2016, https://doi.org/10.5194/acp-16-3485-2016, 2016
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Boreal fire emissions have little effect on ozone concentrations but evident impact on some NOx reservoirs as peroxy nitrates that we quantified. This should be taken into account since NOx reservoirs can be efficiently transported and may influence the ozone budget far away from the fire emission.
The study is based on observations carried out on board the BAe 146 aircraft during BORTAS in Canada. We used a custom laser-induced fluorescence system to measure NO2 and NOx reservoirs.
J. D. Lee, L. K. Whalley, D. E. Heard, D. Stone, R. E. Dunmore, J. F. Hamilton, D. E. Young, J. D. Allan, S. Laufs, and J. Kleffmann
Atmos. Chem. Phys., 16, 2747–2764, https://doi.org/10.5194/acp-16-2747-2016, https://doi.org/10.5194/acp-16-2747-2016, 2016
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This paper presents field measurements of HONO and a range of other gas phase and particulate species from an urban background site in London. The measured daytime HONO cannot be reproduced with a simple box model and thus a significant daytime missing source of HONO is present. We show that this missing source could be responsible for 40 % of the OH radical source and 57 % of the OH initiation; hence its potential importance for atmospheric oxidation and ozone production.
Lisa K. Whalley, Daniel Stone, Brian Bandy, Rachel Dunmore, Jacqueline F. Hamilton, James Hopkins, James D. Lee, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 2109–2122, https://doi.org/10.5194/acp-16-2109-2016, https://doi.org/10.5194/acp-16-2109-2016, 2016
S. Eyer, B. Tuzson, M. E. Popa, C. van der Veen, T. Röckmann, M. Rothe, W. A. Brand, R. Fisher, D. Lowry, E. G. Nisbet, M. S. Brennwald, E. Harris, C. Zellweger, L. Emmenegger, H. Fischer, and J. Mohn
Atmos. Meas. Tech., 9, 263–280, https://doi.org/10.5194/amt-9-263-2016, https://doi.org/10.5194/amt-9-263-2016, 2016
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We present a newly developed field-deployable, autonomous platform simultaneously measuring the three most abundant isotopologues of methane using mid-infrared laser absorption spectroscopy.
The instrument consists of a compact quantum cascade laser absorption spectrometer (QCLAS) coupled to a preconcentration unit, called TRace gas EXtractor (TREX).
The performance of this new in situ technique was investigated during a 2-week measurement campaign and compared to other techniques.
R. E. Dunmore, J. R. Hopkins, R. T. Lidster, J. D. Lee, M. J. Evans, A. R. Rickard, A. C. Lewis, and J. F. Hamilton
Atmos. Chem. Phys., 15, 9983–9996, https://doi.org/10.5194/acp-15-9983-2015, https://doi.org/10.5194/acp-15-9983-2015, 2015
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Technological shifts between fuel sources have had unexpected impacts on atmospheric composition and these significant changes can go undetected if source-specific monitoring infrastructure is not in place. We present chemically comprehensive, continuous measurements of organic compounds in a developed megacity (London), that show diesel-related hydrocarbons can dominate reactive carbon and ozone formation potential, highlighting a serious underestimation of this source in emission inventories.
J. G. Levine, A. R. MacKenzie, O. J. Squire, A. T. Archibald, P. T. Griffiths, N. L. Abraham, J. A. Pyle, D. E. Oram, G. Forster, J. F. Brito, J. D. Lee, J. R. Hopkins, A. C. Lewis, S. J. B. Bauguitte, C. F. Demarco, P. Artaxo, P. Messina, J. Lathière, D. A. Hauglustaine, E. House, C. N. Hewitt, and E. Nemitz
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-24251-2015, https://doi.org/10.5194/acpd-15-24251-2015, 2015
Revised manuscript has not been submitted
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This study explores our ability to simulate atmospheric chemistry stemming from isoprene emissions—a reactive gas emitted from vegetation—in pristine and polluted regions of the Amazon basin. We explore how two contrasting models fare in reproducing recent airborne measurements in the region. Their differing treatments of transport and mixing are found to: profoundly affect their performance; and yield very different pictures of the exposure of the rainforest to harmful ozone concentrations.
H. M. Walker, D. Stone, T. Ingham, S. Vaughan, M. Cain, R. L. Jones, O. J. Kennedy, M. McLeod, B. Ouyang, J. Pyle, S. Bauguitte, B. Bandy, G. Forster, M. J. Evans, J. F. Hamilton, J. R. Hopkins, J. D. Lee, A. C. Lewis, R. T. Lidster, S. Punjabi, W. T. Morgan, and D. E. Heard
Atmos. Chem. Phys., 15, 8179–8200, https://doi.org/10.5194/acp-15-8179-2015, https://doi.org/10.5194/acp-15-8179-2015, 2015
M. D. Shaw, J. D. Lee, B. Davison, A. Vaughan, R. M. Purvis, A. Harvey, A. C. Lewis, and C. N. Hewitt
Atmos. Chem. Phys., 15, 5083–5097, https://doi.org/10.5194/acp-15-5083-2015, https://doi.org/10.5194/acp-15-5083-2015, 2015
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This paper presents the first highly spatially resolved simultaneous mixing ratios of VOCs, NOx and O3 in the atmospheric boundary layer above Greater London (UK) using an research aircraft. Average mixing ratios measured at 360±10 m agl over outer London were always lower than over inner London, indicative of strong local vehicular sources. The comparison of airborne mixing ratio with LAQN air quality ground monitoring stations suggests that the mixing ratios were characteristic of the surface.
B. Wolf, L. Merbold, C. Decock, B. Tuzson, E. Harris, J. Six, L. Emmenegger, and J. Mohn
Biogeosciences, 12, 2517–2531, https://doi.org/10.5194/bg-12-2517-2015, https://doi.org/10.5194/bg-12-2517-2015, 2015
L. R. Crilley, W. J. Bloss, J. Yin, D. C. S. Beddows, R. M. Harrison, J. D. Allan, D. E. Young, M. Flynn, P. Williams, P. Zotter, A. S. H. Prevot, M. R. Heal, J. F. Barlow, C. H. Halios, J. D. Lee, S. Szidat, and C. Mohr
Atmos. Chem. Phys., 15, 3149–3171, https://doi.org/10.5194/acp-15-3149-2015, https://doi.org/10.5194/acp-15-3149-2015, 2015
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Wood is a renewable fuel but its combustion for residential heating releases a number of locally acting air pollutants, most notably particulate matter known to have adverse effects on human health. This paper used chemical tracers for wood smoke to estimate the contribution that burning wood makes to concentrations of airborne particles in the atmosphere of southern England and most particularly in London.
J. W. Taylor, J. D. Allan, G. Allen, H. Coe, P. I. Williams, M. J. Flynn, M. Le Breton, J. B. A. Muller, C. J. Percival, D. Oram, G. Forster, J. D. Lee, A. R. Rickard, M. Parrington, and P. I. Palmer
Atmos. Chem. Phys., 14, 13755–13771, https://doi.org/10.5194/acp-14-13755-2014, https://doi.org/10.5194/acp-14-13755-2014, 2014
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We present a case study of BC wet removal by examining aerosol properties in three biomass burning plumes, one of which passed through a precipitating cloud. Nucleation scavenging preferentially removed the largest and most coated BC-containing particles. Calculated single-scattering albedo (SSA) showed little variation, as a large number of non-BC particles were also present in the precipitation-affected plume.
P. Zotter, V. G. Ciobanu, Y. L. Zhang, I. El-Haddad, M. Macchia, K. R. Daellenbach, G. A. Salazar, R.-J. Huang, L. Wacker, C. Hueglin, A. Piazzalunga, P. Fermo, M. Schwikowski, U. Baltensperger, S. Szidat, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 13551–13570, https://doi.org/10.5194/acp-14-13551-2014, https://doi.org/10.5194/acp-14-13551-2014, 2014
G. Allen, S. M. Illingworth, S. J. O'Shea, S. Newman, A. Vance, S. J.-B. Bauguitte, F. Marenco, J. Kent, K. Bower, M. W. Gallagher, J. Muller, C. J. Percival, C. Harlow, J. Lee, and J. P. Taylor
Atmos. Meas. Tech., 7, 4401–4416, https://doi.org/10.5194/amt-7-4401-2014, https://doi.org/10.5194/amt-7-4401-2014, 2014
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This paper presents a validated method and data set for new retrievals of trace gas concentrations and temperature from the ARIES infrared spectrometer instrument on the UK Atmospheric Research Aircraft (www.faam.ac.uk). This new capability for the aircraft will allow new science to be done because of the way it can sense information about the atmosphere without having to physically pass through it (remote sensing). This will allow us to better understand the make-up of the lower atmosphere.
J. D. Allan, W. T. Morgan, E. Darbyshire, M. J. Flynn, P. I. Williams, D. E. Oram, P. Artaxo, J. Brito, J. D. Lee, and H. Coe
Atmos. Chem. Phys., 14, 11393–11407, https://doi.org/10.5194/acp-14-11393-2014, https://doi.org/10.5194/acp-14-11393-2014, 2014
D. Liu, J. D. Allan, D. E. Young, H. Coe, D. Beddows, Z. L. Fleming, M. J. Flynn, M. W. Gallagher, R. M. Harrison, J. Lee, A. S. H. Prevot, J. W. Taylor, J. Yin, P. I. Williams, and P. Zotter
Atmos. Chem. Phys., 14, 10061–10084, https://doi.org/10.5194/acp-14-10061-2014, https://doi.org/10.5194/acp-14-10061-2014, 2014
J. E. Franklin, J. R. Drummond, D. Griffin, J. R. Pierce, D. L. Waugh, P. I. Palmer, M. Parrington, J. D. Lee, A. C. Lewis, A. R. Rickard, J. W. Taylor, J. D. Allan, H. Coe, K. A. Walker, L. Chisholm, T. J. Duck, J. T. Hopper, Y. Blanchard, M. D. Gibson, K. R. Curry, K. M. Sakamoto, G. Lesins, L. Dan, J. Kliever, and A. Saha
Atmos. Chem. Phys., 14, 8449–8460, https://doi.org/10.5194/acp-14-8449-2014, https://doi.org/10.5194/acp-14-8449-2014, 2014
R. T. Lidster, J. F. Hamilton, J. D. Lee, A. C. Lewis, J. R. Hopkins, S. Punjabi, A. R. Rickard, and J. C. Young
Atmos. Chem. Phys., 14, 6677–6693, https://doi.org/10.5194/acp-14-6677-2014, https://doi.org/10.5194/acp-14-6677-2014, 2014
N. Niedermeier, A. Held, T. Müller, B. Heinold, K. Schepanski, I. Tegen, K. Kandler, M. Ebert, S. Weinbruch, K. Read, J. Lee, K. W. Fomba, K. Müller, H. Herrmann, and A. Wiedensohler
Atmos. Chem. Phys., 14, 2245–2266, https://doi.org/10.5194/acp-14-2245-2014, https://doi.org/10.5194/acp-14-2245-2014, 2014
D. Stone, M. J. Evans, H. Walker, T. Ingham, S. Vaughan, B. Ouyang, O. J. Kennedy, M. W. McLeod, R. L. Jones, J. Hopkins, S. Punjabi, R. Lidster, J. F. Hamilton, J. D. Lee, A. C. Lewis, L. J. Carpenter, G. Forster, D. E. Oram, C. E. Reeves, S. Bauguitte, W. Morgan, H. Coe, E. Aruffo, C. Dari-Salisburgo, F. Giammaria, P. Di Carlo, and D. E. Heard
Atmos. Chem. Phys., 14, 1299–1321, https://doi.org/10.5194/acp-14-1299-2014, https://doi.org/10.5194/acp-14-1299-2014, 2014
A. Mues, J. Kuenen, C. Hendriks, A. Manders, A. Segers, Y. Scholz, C. Hueglin, P. Builtjes, and M. Schaap
Atmos. Chem. Phys., 14, 939–955, https://doi.org/10.5194/acp-14-939-2014, https://doi.org/10.5194/acp-14-939-2014, 2014
P. M. Edwards, M. J. Evans, K. L. Furneaux, J. Hopkins, T. Ingham, C. Jones, J. D. Lee, A. C. Lewis, S. J. Moller, D. Stone, L. K. Whalley, and D. E. Heard
Atmos. Chem. Phys., 13, 9497–9514, https://doi.org/10.5194/acp-13-9497-2013, https://doi.org/10.5194/acp-13-9497-2013, 2013
N. J. Warwick, A. T. Archibald, K. Ashworth, J. Dorsey, P. M. Edwards, D. E. Heard, B. Langford, J. Lee, P. K. Misztal, L. K. Whalley, and J. A. Pyle
Atmos. Chem. Phys., 13, 9183–9194, https://doi.org/10.5194/acp-13-9183-2013, https://doi.org/10.5194/acp-13-9183-2013, 2013
M. Parrington, P. I. Palmer, A. C. Lewis, J. D. Lee, A. R. Rickard, P. Di Carlo, J. W. Taylor, J. R. Hopkins, S. Punjabi, D. E. Oram, G. Forster, E. Aruffo, S. J. Moller, S. J.-B. Bauguitte, J. D. Allan, H. Coe, and R. J. Leigh
Atmos. Chem. Phys., 13, 7321–7341, https://doi.org/10.5194/acp-13-7321-2013, https://doi.org/10.5194/acp-13-7321-2013, 2013
P. Sturm, B. Tuzson, S. Henne, and L. Emmenegger
Atmos. Meas. Tech., 6, 1659–1671, https://doi.org/10.5194/amt-6-1659-2013, https://doi.org/10.5194/amt-6-1659-2013, 2013
P. I. Palmer, M. Parrington, J. D. Lee, A. C. Lewis, A. R. Rickard, P. F. Bernath, T. J. Duck, D. L. Waugh, D. W. Tarasick, S. Andrews, E. Aruffo, L. J. Bailey, E. Barrett, S. J.-B. Bauguitte, K. R. Curry, P. Di Carlo, L. Chisholm, L. Dan, G. Forster, J. E. Franklin, M. D. Gibson, D. Griffin, D. Helmig, J. R. Hopkins, J. T. Hopper, M. E. Jenkin, D. Kindred, J. Kliever, M. Le Breton, S. Matthiesen, M. Maurice, S. Moller, D. P. Moore, D. E. Oram, S. J. O'Shea, R. C. Owen, C. M. L. S. Pagniello, S. Pawson, C. J. Percival, J. R. Pierce, S. Punjabi, R. M. Purvis, J. J. Remedios, K. M. Rotermund, K. M. Sakamoto, A. M. da Silva, K. B. Strawbridge, K. Strong, J. Taylor, R. Trigwell, K. A. Tereszchuk, K. A. Walker, D. Weaver, C. Whaley, and J. C. Young
Atmos. Chem. Phys., 13, 6239–6261, https://doi.org/10.5194/acp-13-6239-2013, https://doi.org/10.5194/acp-13-6239-2013, 2013
P. Di Carlo, E. Aruffo, M. Busilacchio, F. Giammaria, C. Dari-Salisburgo, F. Biancofiore, G. Visconti, J. Lee, S. Moller, C. E. Reeves, S. Bauguitte, G. Forster, R. L. Jones, and B. Ouyang
Atmos. Meas. Tech., 6, 971–980, https://doi.org/10.5194/amt-6-971-2013, https://doi.org/10.5194/amt-6-971-2013, 2013
B. Tuzson, K. Zeyer, M. Steinbacher, J. B. McManus, D. D. Nelson, M. S. Zahniser, and L. Emmenegger
Atmos. Meas. Tech., 6, 927–936, https://doi.org/10.5194/amt-6-927-2013, https://doi.org/10.5194/amt-6-927-2013, 2013
A. C. Lewis, M. J. Evans, J. R. Hopkins, S. Punjabi, K. A. Read, R. M. Purvis, S. J. Andrews, S. J. Moller, L. J. Carpenter, J. D. Lee, A. R. Rickard, P. I. Palmer, and M. Parrington
Atmos. Chem. Phys., 13, 851–867, https://doi.org/10.5194/acp-13-851-2013, https://doi.org/10.5194/acp-13-851-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Distinct structures of interannual variations in stratosphere-to-troposphere ozone transport induced by the Tibetan Plateau thermal forcing
Global CH4 fluxes derived from JAXA/GOSAT lower-tropospheric partial column data and the CarbonTracker Europe-CH4 atmospheric inverse model
Improved understanding of anthropogenic and biogenic carbonyl sulfide (COS) fluxes in western Europe from long-term continuous mixing ratio measurements
The skill at modeling an extremely high ozone episode varies substantially amongst ensemble simulation
Quantifying transboundary transport flux of CO over the Tibetan Plateau: variabilities and drivers
Inverse modelling of New Zealand's carbon dioxide balance estimates a larger than expected carbon sink
Combined CO2 measurement record indicates Amazon forest carbon uptake is offset by savanna carbon release
Operational and Probabilistic Evaluation of AQMEII-4 Regional Scale Ozone Dry Deposition. Time to Harmonise Our LULC Masks
The importance of moist thermodynamics on neutral buoyancy height for plumes from anthropogenic sources
How reliable are process-based 222radon emission maps? Results from an atmospheric 222radon inversion in Europe
Partitioning anthropogenic and natural methane emissions in Finland during 2000–2021 by combining bottom-up and top-down estimates
A Diagnostic Intercomparison of Modeled Ozone Dry Deposition Over North America and Europe Using AQMEII4 Regional-Scale Simulations
The role of OCO-3 XCO2 retrievals in estimating global terrestrial net ecosystem exchanges
Surface and tropospheric ozone over East Asia and Southeast Asia from observations: distributions, trends, and variability
The improved Trajectory-mapped Ozonesonde dataset for the Stratosphere and Troposphere (TOST): update, validation and applications
Constraining elemental mercury air–sea exchange using long-term ground-based observations
Climate Forcing due to Future Ozone Changes: An intercomparison of metrics and methods
Variation in shortwave water vapour continuum and impact on clear-sky shortwave radiative feedback
Tracing the origins of stratospheric ozone intrusions: direct vs. indirect pathways and their impacts on Central and Eastern China in spring–summer 2019
Flow-dependent observation errors for greenhouse gas inversions in an ensemble Kalman smoother
A WRF-Chem study of the greenhouse gas column and in situ surface concentrations observed at Xianghe, China. Part 1: Methane (CH4)
Evaluation and updates to the oxidized reactive nitrogen trace gas dry deposition parameterization from the GEOS-Chem CTM, including a pathway for ground surface NO2 hydrolysis
Observational and model evidence for a prominent stratospheric influence on variability in tropospheric nitrous oxide
Estimation of Canada's methane emissions: inverse modelling analysis using the Environment and Climate Change Canada (ECCC) measurement network
Spatiotemporal source apportionment of ozone pollution over the Greater Bay Area
Potential of 14C-based vs. ΔCO-based ΔffCO2 observations to estimate urban fossil fuel CO2 (ffCO2) emissions
On the uncertainty of anthropogenic aromatic volatile organic compound emissions: model evaluation and sensitivity analysis
A mechanism of stratospheric O3 intrusion into the atmospheric environment: a case study of the North China Plain
Influence of atmospheric circulation on the interannual variability of transport from global and regional emissions into the Arctic
Surface networks in the Arctic may miss a future methane bomb
Potential of using CO2 observations over India in a regional carbon budget estimation by improving the modelling system
A bottom-up emission estimate for the 2022 Nord Stream gas leak: derivation, simulations, and evaluation
European CH4 inversions with ICON-ART coupled to the CarbonTracker Data Assimilation Shell
Extreme weather exacerbates ozone pollution in the Pearl River Delta, China: role of natural processes
Multidecadal ozone trends in China and implications for human health and crop yields: a hybrid approach combining a chemical transport model and machine learning
On the influence of vertical mixing, boundary layer schemes, and temporal emission profiles on tropospheric NO2 in WRF-Chem – comparisons to in situ, satellite, and MAX-DOAS observations
Decreasing trends of ammonia emissions over Europe seen from remote sensing and inverse modelling
The sensitivity of Southern Ocean atmospheric dimethyl sulfide (DMS) to modeled oceanic DMS concentrations and emissions
Impacts of maritime shipping on air pollution along the US East Coast
Understanding greenhouse gas (GHG) column concentrations in Munich using the Weather Research and Forecasting (WRF) model
Impact of transport model resolution and a priori assumptions on inverse modeling of Swiss F-gas emissions
Estimation of power plant SO2 emissions using the HYSPLIT dispersion model and airborne observations with plume rise ensemble runs
Can we use atmospheric CO2 measurements to verify emission trends reported by cities? Lessons from a 6-year atmospheric inversion over Paris
A new steady-state gas–particle partitioning model of polycyclic aromatic hydrocarbons: implication for the influence of the particulate proportion in emissions
An analysis of CMAQ gas-phase dry deposition over North America through grid-scale and land-use-specific diagnostics in the context of AQMEII4
Rethinking the role of transport and photochemistry in regional ozone pollution: insights from ozone concentration and mass budgets
Decreasing seasonal cycle amplitude of methane in the northern high latitudes being driven by lower-latitude changes in emissions and transport
The effect of anthropogenic emission, meteorological factors, and carbon dioxide on the surface ozone increase in China from 2008 to 2018 during the East Asia summer monsoon season
Development of a CMAQ–PMF-based composite index for prescribing an effective ozone abatement strategy: a case study of sensitivity of surface ozone to precursor volatile organic compound species in southern Taiwan
Comment on “Climate consequences of hydrogen emissions” by Ocko and Hamburg (2022)
Qingjian Yang, Tianliang Zhao, Yongqing Bai, Kai Meng, Yuehan Luo, Zhijie Tian, Xiaoyun Sun, Weikang Fu, Kai Yang, and Jun Hu
Atmos. Chem. Phys., 25, 8029–8042, https://doi.org/10.5194/acp-25-8029-2025, https://doi.org/10.5194/acp-25-8029-2025, 2025
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This study reveals a unique driver of the Tibetan Plateau (TP) thermal forcing of the interannual variations in stratosphere-to-troposphere transport (STT) of ozone with diverse structures. Anomalous strong TP thermal forcing induces anticyclonic anomalies in the upper troposphere over the TP, which strengthens and attenuates the northern and southern branches of the westerly jet, intensifying (weakening) the westerly trough for more (fewer) tropopause folds of ozone STT over the East Asian region.
Aki Tsuruta, Akihiko Kuze, Kei Shiomi, Fumie Kataoka, Nobuhiro Kikuchi, Tuula Aalto, Leif Backman, Ella Kivimäki, Maria K. Tenkanen, Kathryn McKain, Omaira E. García, Frank Hase, Rigel Kivi, Isamu Morino, Hirofumi Ohyama, David F. Pollard, Mahesh K. Sha, Kimberly Strong, Ralf Sussmann, Yao Te, Voltaire A. Velazco, Mihalis Vrekoussis, Thorsten Warneke, Minqiang Zhou, and Hiroshi Suto
Atmos. Chem. Phys., 25, 7829–7862, https://doi.org/10.5194/acp-25-7829-2025, https://doi.org/10.5194/acp-25-7829-2025, 2025
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Satellite data bring invaluable information about greenhouse gas emissions globally. We found that a new type of data from the Greenhouse Gas Observing Satellite (GOSAT), which contains information about methane in the lowest layer of Earth's atmosphere, could provide reliable estimates of recent methane emissions when combined with atmospheric modelling. Therefore, the use of such data is encouraged to improve emission quantification methods and advance our understanding of methane cycles.
Antoine Berchet, Isabelle Pison, Camille Huselstein, Clément Narbaud, Marine Remaud, Sauveur Belviso, Camille Abadie, and Fabienne Maignan
Atmos. Chem. Phys., 25, 7499–7525, https://doi.org/10.5194/acp-25-7499-2025, https://doi.org/10.5194/acp-25-7499-2025, 2025
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We use the measurements of atmospheric carbonyl sulfide (COS) concentrations at the monitoring site of Gif-sur-Yvette (in the Paris region) from August 2014 to December 2019, combined with existing knowledge on COS fluxes in the atmosphere and a transport model, to gain insight into COS fluxes, either natural, such as oceanic emissions or vegetation and soil fluxes, or anthropogenic, from industrial activities and power generation.
Jinhui Gao and Hui Xiao
Atmos. Chem. Phys., 25, 7387–7401, https://doi.org/10.5194/acp-25-7387-2025, https://doi.org/10.5194/acp-25-7387-2025, 2025
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The ensemble simulation provides a solution to better reproduce and understand the extremely high ozone episode that occurred in the Great Bay Area when Typhoon Nida approached South China in summer 2016. Elevated temperatures and weak winds contributed to the increase in ozone precursors, resulting in enhanced ozone production. Large amounts of ozone aloft also contributed to the increase in surface ozone via vertical transport. Notably, ozone from Southeast Asia contributed through this mechanism.
Zhenda Sun, Hao Yin, Zhongfeng Pan, Chongyang Li, Xiao Lu, Ke Liu, Youwen Sun, and Cheng Liu
Atmos. Chem. Phys., 25, 6823–6842, https://doi.org/10.5194/acp-25-6823-2025, https://doi.org/10.5194/acp-25-6823-2025, 2025
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This study investigates the variability and driving forces of transboundary CO transport flux over the Tibetan Plateau from May 2018 to April 2024. During this period, external CO influx increased by 2.86 Tg yr-1, while internal efflux slightly declined by 1.70 Tg yr-1. The rising influx in recent years is likely linked to the rapid increase in CO concentrations from South Asia.
Beata Bukosa, Sara Mikaloff-Fletcher, Gordon Brailsford, Dan Smale, Elizabeth D. Keller, W. Troy Baisden, Miko U. F. Kirschbaum, Donna L. Giltrap, Lìyǐn Liáng, Stuart Moore, Rowena Moss, Sylvia Nichol, Jocelyn Turnbull, Alex Geddes, Daemon Kennett, Dóra Hidy, Zoltán Barcza, Louis A. Schipper, Aaron M. Wall, Shin-Ichiro Nakaoka, Hitoshi Mukai, and Andrea Brandon
Atmos. Chem. Phys., 25, 6445–6473, https://doi.org/10.5194/acp-25-6445-2025, https://doi.org/10.5194/acp-25-6445-2025, 2025
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We used atmospheric measurements and inverse modelling to estimate New Zealand's carbon dioxide (CO2) emissions and removals from 2011 to 2020. Our study reveals that New Zealand's land absorbs more CO2 than previously estimated, particularly in areas dominated by indigenous forests. Our results highlight gaps in current national CO2 estimates and methods, suggesting a need for further research to improve emissions reports and refine approaches to track progress toward climate mitigation goals.
Santiago Botía, Saqr Munassar, Thomas Koch, Danilo Custodio, Luana S. Basso, Shujiro Komiya, Jost V. Lavric, David Walter, Manuel Gloor, Giordane Martins, Stijn Naus, Gerbrand Koren, Ingrid T. Luijkx, Stijn Hantson, John B. Miller, Wouter Peters, Christian Rödenbeck, and Christoph Gerbig
Atmos. Chem. Phys., 25, 6219–6255, https://doi.org/10.5194/acp-25-6219-2025, https://doi.org/10.5194/acp-25-6219-2025, 2025
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This study uses dry CO2 mole fractions from the Amazon Tall Tower Observatory together with airborne profiles to estimate net carbon exchange in tropical South America. We found that the biogeographic Amazon is a net carbon sink, while the Cerrado and Caatinga biomes are net carbon sources, resulting in an overall neutral balance. Finally, to further reduce the uncertainty in our estimates we call for an expansion of the monitoring capacity, especially in the Amazon–Andes foothills.
Ioannis Kioutsioukis, Christian Hogrefe, Paul A. Makar, Ummugulsun Alyuz, Jessy O. Bash, Roberto Bellasio, Roberto Bianconi, Tim Buttler, Olivia E. Clifton, Philippe Cheung, Alma Hodzic, Richard Kranenburg, Aurelia Lupascu, Kester Momoh, Juan Luis Perez-Camaño, John Pleim, Young-Hee Ryu, Robero San Jose, Donna Schwede, Ranjeet Sokhi, and Stefano Galmarini
EGUsphere, https://doi.org/10.5194/egusphere-2025-1091, https://doi.org/10.5194/egusphere-2025-1091, 2025
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Deposition is a key in air quality modelling. An evaluation of the AQMEII4 models is performed prior to analysing the different deposition schemes in relation to the LULC used. Such analysis is unprecedented. Among the results, LULC masks have to be harmonised and up-to-date information used in place of outdated and too course masks. Alternatively LULC masks should be evaluated and intercom pared when multiple model results are analysed.
Sepehr Fathi, Paul Makar, Wanmin Gong, Junhua Zhang, Katherine Hayden, and Mark Gordon
Atmos. Chem. Phys., 25, 2385–2405, https://doi.org/10.5194/acp-25-2385-2025, https://doi.org/10.5194/acp-25-2385-2025, 2025
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Our study explores the influence of water phase changes in plumes from industrial sources on atmospheric dispersion of emitted pollutants and air quality. Employing PRISM (Plume-Rise-Iterative-Stratified-Moist), a new method, we found that considering these effects significantly improves predictions of pollutant dispersion. This insight enhances our understanding of environmental impacts, enabling more accurate air quality modelling and fostering more effective pollution management strategies.
Fabian Maier, Eva Falge, Maksym Gachkivskyi, Stephan Henne, Ute Karstens, Dafina Kikaj, Ingeborg Levin, Alistair Manning, Christian Rödenbeck, and Christoph Gerbig
EGUsphere, https://doi.org/10.5194/egusphere-2025-477, https://doi.org/10.5194/egusphere-2025-477, 2025
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The radioactive noble gas radon (222Rn) is a suitable natural tracer for atmospheric transport and mixing processes that can be used to validate and calibrate atmospheric transport models. However, this requires accurate estimates of the 222Rn flux from the soil into the atmosphere. In our study, we evaluate the reliability of process-based 222Rn flux maps for Europe using a 222Rn inversion. Our inversion results can give some indications on how to improve the process-based 222Rn flux maps.
Maria K. Tenkanen, Aki Tsuruta, Hugo Denier van der Gon, Lena Höglund-Isaksson, Antti Leppänen, Tiina Markkanen, Ana Maria Roxana Petrescu, Maarit Raivonen, Hermanni Aaltonen, and Tuula Aalto
Atmos. Chem. Phys., 25, 2181–2206, https://doi.org/10.5194/acp-25-2181-2025, https://doi.org/10.5194/acp-25-2181-2025, 2025
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Accurate national methane (CH4) emission estimates are essential for tracking progress towards climate goals. This study compares estimates from Finland, which use different methods and scales, and shows how well a global model estimates emissions within a country. The bottom-up estimates vary a lot, but constraining them with atmospheric CH4 measurements brought the estimates closer together. We also highlight the importance of quantifying natural emissions alongside anthropogenic emissions.
Christian Hogrefe, Stefano Galmarini, Paul A. Makar, Ioannis Kioutsioukis, Olivia E. Clifton, Ummugulsum Alyuz, Jesse O. Bash, Roberto Bellasio, Roberto Bianconi, Tim Butler, Philip Cheung, Alma Hodzic, Richard Kranenburg, Aurelia Lupascu, Kester Momoh, Juan Luis Perez-Camanyo, Jonathan E. Pleim, Young-Hee Ryu, Roberto San Jose, Martijn Schaap, Donna B. Schwede, and Ranjeet Sokhi
EGUsphere, https://doi.org/10.5194/egusphere-2025-225, https://doi.org/10.5194/egusphere-2025-225, 2025
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Performed under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in regional-scale models. The results also strongly suggest that improvement and harmonization of the representation of land use in these models would serve the community in their future development efforts.
Xingyu Wang, Fei Jiang, Hengmao Wang, Zhengqi Zhang, Mousong Wu, Jun Wang, Wei He, Weimin Ju, and Jing M. Chen
Atmos. Chem. Phys., 25, 867–880, https://doi.org/10.5194/acp-25-867-2025, https://doi.org/10.5194/acp-25-867-2025, 2025
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The role of OCO-3 XCO2 retrievals in estimating global terrestrial carbon fluxes is unclear. We investigate this by assimilating OCO-3 XCO2 retrievals alone and in combination with OCO-2 XCO2. The assimilation of OCO-3 XCO2 alone underestimates global land sinks, mainly at high latitudes, due to the lack of observations beyond 52° S and 52° N, large variations in the number of data, and varying observation times, while the joint assimilation of OCO-2 and OCO-3 XCO2 has the best performance.
Ke Li, Rong Tan, Wenhao Qiao, Taegyung Lee, Yufen Wang, Danyuting Zhang, Minglong Tang, Wenqing Zhao, Yixuan Gu, Shaojia Fan, Jinqiang Zhang, Xiaopu Lyu, Likun Xue, Jianming Xu, Zhiqiang Ma, Mohd Talib Latif, Teerachai Amnuaylojaroen, Junsu Gil, Mee-Hye Lee, Juseon Bak, Joowan Kim, Hong Liao, Yugo Kanaya, Xiao Lu, Tatsuya Nagashima, and Ja-Ho Koo
EGUsphere, https://doi.org/10.5194/egusphere-2024-3756, https://doi.org/10.5194/egusphere-2024-3756, 2025
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East Asia and Southeast Asia has been identified as a global hot spot with the fastest ozone increase. This paper presents the most comprehensive observational view of ozone distributions and evolution over East Asia and Southeast Asia across different spatiotemporal scales in the past two decades, which will have important implications for assessing ozone impacts on public health and crop yields, and for developing future ozone control strategies.
Zhou Zang, Jane Liu, David Tarasick, Omid Moeini, Jianchun Bian, Jinqiang Zhang, Anne M. Thompson, Roeland Van Malderen, Herman G. J. Smit, Ryan M. Stauffer, Bryan J. Johnson, and Debra E. Kollonige
Atmos. Chem. Phys., 24, 13889–13912, https://doi.org/10.5194/acp-24-13889-2024, https://doi.org/10.5194/acp-24-13889-2024, 2024
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The Trajectory-mapped Ozonesonde dataset for the Stratosphere and Troposphere (TOST) provides a global-scale, long-term ozone climatology that is horizontally and vertically resolved. In this study, we improved, updated and validated TOST from 1970 to 2021. Based on this TOST dataset, we characterized global ozone variations spatially in both the troposphere and stratosphere and temporally by season and decade. We also showed a stagnant lower stratospheric ozone variation since the late 1990s.
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.
William J. Collins, Fiona M. O'Connor, Connor R. Barker, Rachael E. Byrom, Sebastian D. Eastham, Øivind Hodnebrog, Patrick Jöckel, Eloise A. Marais, Mariano Mertens, Gunnar Myhre, Matthias Nützel, Dirk Olivié, Ragnhild Bieltvedt Skeie, Laura Stecher, Larry W. Horowitz, Vaishali Naik, Gregory Faluvegi, Ulas Im, Lee T. Murray, Drew Shindell, Kostas Tsigaridis, Nathan Luke Abraham, and James Keeble
EGUsphere, https://doi.org/10.5194/egusphere-2024-3698, https://doi.org/10.5194/egusphere-2024-3698, 2024
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If reductions aren’t implemented to limit emissions of pollutants that produce ozone then we calculate that this will cause a warming of climate. We assess how the future warming from ozone is affected by changing meteorological variables such as clouds and atmospheric temperatures. We find that reductions in high cloud cover tend to slightly reduce the warming from ozone.
Kaah P. Menang, Stefan A. Buehler, Lukas Kluft, Robin J. Hogan, and Florian E. Roemer
EGUsphere, https://doi.org/10.5194/egusphere-2024-3051, https://doi.org/10.5194/egusphere-2024-3051, 2024
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We investigated how the uncertainty in representing water vapour continuum absorption in the shortwave affects clear-sky shortwave radiative feedback. For current surface temperature, the impact is modest (<2 %). In a warmer world, continuum induced error in estimated shortwave feedback is up to ~5 %. Using the MT_CKD model in radiative transfer calculations may lead to an underestimation of the shortwave feedback. Constraining shortwave continuum will contribute to reducing these discrepancies.
Kai Meng, Tianliang Zhao, Yongqing Bai, Ming Wu, Le Cao, Xuewei Hou, Yuehan Luo, and Yongcheng Jiang
Atmos. Chem. Phys., 24, 12623–12642, https://doi.org/10.5194/acp-24-12623-2024, https://doi.org/10.5194/acp-24-12623-2024, 2024
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We studied the impact of stratospheric intrusions (SIs) on tropospheric and near-surface ozone in Central and Eastern China from a stratospheric source tracing perspective. SIs contribute the most in the eastern plains, with a contribution exceeding 15 %, and have a small contribution to the west and south. Western Siberia and Mongolia are the most critical source areas for indirect and direct SIs, with the Rossby wave and northeast cold vortex being important driving circulation systems.
Michael Steiner, Luca Cantarello, Stephan Henne, and Dominik Brunner
Atmos. Chem. Phys., 24, 12447–12463, https://doi.org/10.5194/acp-24-12447-2024, https://doi.org/10.5194/acp-24-12447-2024, 2024
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Atmospheric greenhouse gas inversions have great potential to independently check reported bottom-up emissions; however they are subject to large uncertainties. It is paramount to address and reduce the largest source of uncertainty, which stems from the representation of atmospheric transport in the models. In this study, we show that the use of a temporally varying flow-dependent atmospheric transport uncertainty can enhance the accuracy of emission estimation in an idealized experiment.
Sieglinde Callewaert, Minqiang Zhou, Bavo Langerock, Pucai Wang, Ting Wang, Emmanuel Mahieu, and Martine De Mazière
EGUsphere, https://doi.org/10.5194/egusphere-2024-3228, https://doi.org/10.5194/egusphere-2024-3228, 2024
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We used an atmospheric transport model and satellite data to study CH4 observations at Xianghe, China. Our study shows the key source sectors that influence the concentrations and their respective importance. Furthermore, meteorological factors such as wind direction are discussed. This research highlights the challenges in accurately simulating these kind of measurements and helps us to better understand CH4 variability in the region.
Brian L. Boys, Randall V. Martin, and Trevor C. VandenBoer
EGUsphere, https://doi.org/10.5194/egusphere-2024-2994, https://doi.org/10.5194/egusphere-2024-2994, 2024
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A widely used dry deposition parameterization for NO2 is updated by including a well-known heterogeneous hydrolysis reaction on deposition surfaces. This mechanistic update eliminates a large low bias of -80 % in simulated NO2 nocturnal deposition velocities evaluated against long-term eddy covariance flux observations over Harvard Forest. We highlight the importance of canopy surface area effects as well as soil NO emission in formulating and evaluating NO2 dry deposition parameterizations.
Cynthia D. Nevison, Qing Liang, Paul A. Newman, Britton B. Stephens, Geoff Dutton, Xin Lan, Roisin Commane, Yenny Gonzalez, and Eric Kort
Atmos. Chem. Phys., 24, 10513–10529, https://doi.org/10.5194/acp-24-10513-2024, https://doi.org/10.5194/acp-24-10513-2024, 2024
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This study examines the drivers of interannual variability in tropospheric N2O. New insights are obtained from aircraft data and a chemistry–climate model that explicitly simulates stratospheric N2O. The stratosphere is found to be the dominant driver of N2O variability in the Northern Hemisphere, while both the stratosphere and El Niño cycles are important in the Southern Hemisphere. These results are consistent with known atmospheric dynamics and differences between the hemispheres.
Misa Ishizawa, Douglas Chan, Doug Worthy, Elton Chan, Felix Vogel, Joe R. Melton, and Vivek K. Arora
Atmos. Chem. Phys., 24, 10013–10038, https://doi.org/10.5194/acp-24-10013-2024, https://doi.org/10.5194/acp-24-10013-2024, 2024
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Methane (CH4) emissions in Canada for 2007–2017 were estimated using Canada’s surface greenhouse gas measurements. The estimated emissions show no significant trend, but emission uncertainty was reduced as more measurement sites became available. Notably for climate change, we find the wetland CH4 emissions show a positive correlation with surface air temperature in summer. Canada’s measurement network could monitor future CH4 emission changes and compliance with climate change mitigation goals.
Yiang Chen, Xingcheng Lu, and Jimmy C. H. Fung
Atmos. Chem. Phys., 24, 8847–8864, https://doi.org/10.5194/acp-24-8847-2024, https://doi.org/10.5194/acp-24-8847-2024, 2024
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This study investigates the contribution of pollutants from different emitting periods to ozone episodes over the Greater Bay Area. The analysis reveals the variation in major spatiotemporal contributors to the O3 pollution under the influence of typhoons and subtropical high pressure. Through temporal contribution analysis, our work offers a new perspective on the evolution of O3 pollution and can aid in developing effective and timely control policies under unfavorable weather conditions.
Fabian Maier, Christian Rödenbeck, Ingeborg Levin, Christoph Gerbig, Maksym Gachkivskyi, and Samuel Hammer
Atmos. Chem. Phys., 24, 8183–8203, https://doi.org/10.5194/acp-24-8183-2024, https://doi.org/10.5194/acp-24-8183-2024, 2024
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We investigate the usage of discrete radiocarbon (14C)-based fossil fuel carbon dioxide (ffCO2) concentration estimates vs. continuous carbon monoxide (CO)-based ffCO2 estimates to evaluate the seasonal cycle of ffCO2 emissions in an urban region with an inverse modeling framework. We find that the CO-based ffCO2 estimates allow us to reconstruct robust seasonal cycles, which show the distinct COVID-19 drawdown in 2020 and can be used to validate emission inventories.
Kevin Oliveira, Marc Guevara, Oriol Jorba, Hervé Petetin, Dene Bowdalo, Carles Tena, Gilbert Montané Pinto, Franco López, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 7137–7177, https://doi.org/10.5194/acp-24-7137-2024, https://doi.org/10.5194/acp-24-7137-2024, 2024
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In this work, we assess and evaluate benzene, toluene, and xylene primary emissions and air quality levels in Spain by combining observations, emission inventories, and air quality modelling techniques. The comparison between modelled and observed levels allows identifying uncertainty sources within the emission input. This contributes to improving air quality models' performance when simulating these compounds, leading to better support for the design of effective pollution control strategies.
Yuehan Luo, Tianliang Zhao, Kai Meng, Jun Hu, Qingjian Yang, Yongqing Bai, Kai Yang, Weikang Fu, Chenghao Tan, Yifan Zhang, Yanzhe Zhang, and Zhikuan Li
Atmos. Chem. Phys., 24, 7013–7026, https://doi.org/10.5194/acp-24-7013-2024, https://doi.org/10.5194/acp-24-7013-2024, 2024
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We reveal a significant mechanism of stratospheric O3 intrusion (SI) into the atmospheric environment induced by an extratropical cyclone system. This system facilitates the downward transport of stratospheric O3 to the near-surface layer by vertical coupling, involving the upper westerly trough, the middle northeast cold vortex, and the lower extratropical cyclone in the troposphere. On average, stratospheric O3 contributed 26.77 % to near-surface O3 levels over the North China Plain.
Cheng Zheng, Yutian Wu, Mingfang Ting, and Clara Orbe
Atmos. Chem. Phys., 24, 6965–6985, https://doi.org/10.5194/acp-24-6965-2024, https://doi.org/10.5194/acp-24-6965-2024, 2024
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Trace gases and aerosols in the Arctic, which typically originate from midlatitude and tropical emission regions, modulate the Arctic climate via their radiative and chemistry impacts. Thus, long-range transport of these substances is important for understanding the current and the future change of Arctic climate. By employing chemistry–climate models, we explore how year-to-year variations in the atmospheric circulation modulate atmospheric long-range transport into the Arctic.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, and Jean-Daniel Paris
Atmos. Chem. Phys., 24, 6359–6373, https://doi.org/10.5194/acp-24-6359-2024, https://doi.org/10.5194/acp-24-6359-2024, 2024
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The aim of this work is to analyse how accurately a methane bomb event could be detected with the current and a hypothetically extended stationary observation network in the Arctic. For this, we incorporate synthetically modelled possible future CH4 concentrations based on plausible emission scenarios into an inverse modelling framework. We analyse how well the increase is detected in different Arctic regions and evaluate the impact of additional observation sites in this respect.
Vishnu Thilakan, Dhanyalekshmi Pillai, Jithin Sukumaran, Christoph Gerbig, Haseeb Hakkim, Vinayak Sinha, Yukio Terao, Manish Naja, and Monish Vijay Deshpande
Atmos. Chem. Phys., 24, 5315–5335, https://doi.org/10.5194/acp-24-5315-2024, https://doi.org/10.5194/acp-24-5315-2024, 2024
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This study investigates the usability of CO2 mixing ratio observations over India to infer regional carbon sources and sinks. We demonstrate that a high-resolution modelling system can represent the observed CO2 variations reasonably well by improving the transport and flux variations at a fine scale. Future carbon data assimilation systems can thus benefit from these recently available CO2 observations when fine-scale variations are adequately represented in the models.
Rostislav Kouznetsov, Risto Hänninen, Andreas Uppstu, Evgeny Kadantsev, Yalda Fatahi, Marje Prank, Dmitrii Kouznetsov, Steffen Manfred Noe, Heikki Junninen, and Mikhail Sofiev
Atmos. Chem. Phys., 24, 4675–4691, https://doi.org/10.5194/acp-24-4675-2024, https://doi.org/10.5194/acp-24-4675-2024, 2024
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By relying solely on publicly available media reports, we were able to infer the temporal evolution and the injection height for the Nord Stream gas leaks in September 2022. The inventory specifies locations, vertical distributions, and temporal evolution of the methane sources. The inventory can be used to simulate the event with atmospheric transport models. The inventory is supplemented with a set of observational data tailored to evaluate the results of the simulated atmospheric dispersion.
Michael Steiner, Wouter Peters, Ingrid Luijkx, Stephan Henne, Huilin Chen, Samuel Hammer, and Dominik Brunner
Atmos. Chem. Phys., 24, 2759–2782, https://doi.org/10.5194/acp-24-2759-2024, https://doi.org/10.5194/acp-24-2759-2024, 2024
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The Paris Agreement increased interest in estimating greenhouse gas (GHG) emissions of individual countries, but top-down emission estimation is not yet considered policy-relevant. It is therefore paramount to reduce large errors and to build systems that are based on the newest atmospheric transport models. In this study, we present the first application of ICON-ART in the inverse modeling of GHG fluxes with an ensemble Kalman filter and present our results for European CH4 emissions.
Nan Wang, Hongyue Wang, Xin Huang, Xi Chen, Yu Zou, Tao Deng, Tingyuan Li, Xiaopu Lyu, and Fumo Yang
Atmos. Chem. Phys., 24, 1559–1570, https://doi.org/10.5194/acp-24-1559-2024, https://doi.org/10.5194/acp-24-1559-2024, 2024
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This study explores the influence of extreme-weather-induced natural processes on ozone pollution, which is often overlooked. By analyzing meteorological factors, natural emissions, chemistry pathways and atmospheric transport, we discovered that these natural processes could substantially exacerbate ozone pollution. The findings contribute to a deeper understanding of ozone pollution and offer valuable insights for controlling ozone pollution in the context of global warming.
Jia Mao, Amos P. K. Tai, David H. Y. Yung, Tiangang Yuan, Kong T. Chau, and Zhaozhong Feng
Atmos. Chem. Phys., 24, 345–366, https://doi.org/10.5194/acp-24-345-2024, https://doi.org/10.5194/acp-24-345-2024, 2024
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Surface ozone (O3) is well-known for posing great threats to both human health and agriculture worldwide. However, a multidecadal assessment of the impacts of O3 on public health and agriculture in China is lacking without sufficient O3 observations. We used a hybrid approach combining a chemical transport model and machine learning to provide a robust dataset of O3 concentrations over the past 4 decades in China, thereby filling the gap in the long-term O3 trend and impact assessment in China.
Leon Kuhn, Steffen Beirle, Vinod Kumar, Sergey Osipov, Andrea Pozzer, Tim Bösch, Rajesh Kumar, and Thomas Wagner
Atmos. Chem. Phys., 24, 185–217, https://doi.org/10.5194/acp-24-185-2024, https://doi.org/10.5194/acp-24-185-2024, 2024
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NO₂ is an important air pollutant. It was observed that the WRF-Chem model shows significant deviations in NO₂ abundance when compared to measurements. We use a 1-month simulation over central Europe to show that these deviations can be mostly resolved by reparameterization of the vertical mixing routine. In order to validate our results, they are compared to in situ, satellite, and MAX-DOAS measurements.
Ondřej Tichý, Sabine Eckhardt, Yves Balkanski, Didier Hauglustaine, and Nikolaos Evangeliou
Atmos. Chem. Phys., 23, 15235–15252, https://doi.org/10.5194/acp-23-15235-2023, https://doi.org/10.5194/acp-23-15235-2023, 2023
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We show declining trends in NH3 emissions over Europe for 2013–2020 using advanced dispersion and inverse modelling and satellite measurements from CrIS. Emissions decreased by −26% since 2013, showing that the abatement strategies adopted by the European Union have been very efficient. Ammonia emissions are low in winter and peak in summer due to temperature-dependent soil volatilization. The largest decreases were observed in central and western Europe in countries with high emissions.
Yusuf A. Bhatti, Laura E. Revell, Alex J. Schuddeboom, Adrian J. McDonald, Alex T. Archibald, Jonny Williams, Abhijith U. Venugopal, Catherine Hardacre, and Erik Behrens
Atmos. Chem. Phys., 23, 15181–15196, https://doi.org/10.5194/acp-23-15181-2023, https://doi.org/10.5194/acp-23-15181-2023, 2023
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Aerosols are a large source of uncertainty over the Southern Ocean. A dominant source of sulfate aerosol in this region is dimethyl sulfide (DMS), which is poorly simulated by climate models. We show the sensitivity of simulated atmospheric DMS to the choice of oceanic DMS data set and emission scheme. We show that oceanic DMS has twice the influence on atmospheric DMS than the emission scheme. Simulating DMS more accurately in climate models will help to constrain aerosol uncertainty.
Maryam Golbazi and Cristina Archer
Atmos. Chem. Phys., 23, 15057–15075, https://doi.org/10.5194/acp-23-15057-2023, https://doi.org/10.5194/acp-23-15057-2023, 2023
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We use scientific models to study the impact of ship emissions on air quality along the US East Coast. We find an increase in three major pollutants (PM2.5, NO2, and SO2) in coastal regions. However, we detect a reduction in ozone (O3) levels in major coastal cities. This reduction is linked to the significant emissions of nitrogen oxides (NOx) from ships, which scavenged O3, especially in highly polluted urban areas experiencing an NOx-limited regime.
Xinxu Zhao, Jia Chen, Julia Marshall, Michal Gałkowski, Stephan Hachinger, Florian Dietrich, Ankit Shekhar, Johannes Gensheimer, Adrian Wenzel, and Christoph Gerbig
Atmos. Chem. Phys., 23, 14325–14347, https://doi.org/10.5194/acp-23-14325-2023, https://doi.org/10.5194/acp-23-14325-2023, 2023
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We develop a modeling framework using the Weather Research and Forecasting model at a high spatial resolution (up to 400 m) to simulate atmospheric transport of greenhouse gases and interpret column observations. Output is validated against weather stations and column measurements in August 2018. The differential column method is applied, aided by air-mass transport tracing with the Stochastic Time-Inverted Lagrangian Transport (STILT) model, also for an exploratory measurement interpretation.
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
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The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
Tianfeng Chai, Xinrong Ren, Fong Ngan, Mark Cohen, and Alice Crawford
Atmos. Chem. Phys., 23, 12907–12933, https://doi.org/10.5194/acp-23-12907-2023, https://doi.org/10.5194/acp-23-12907-2023, 2023
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The SO2 emissions of three power plants are estimated using aircraft observations and an ensemble of HYSPLIT dispersion simulations with different plume rise parameters. The emission estimates using the runs with the lowest root mean square errors (RMSEs) and the runs with the best correlation coefficients between the predicted and observed mixing ratios both agree well with the Continuous Emissions Monitoring Systems (CEMS) data. The RMSE-based plume rise appears to be more reasonable.
Jinghui Lian, Thomas Lauvaux, Hervé Utard, François-Marie Bréon, Grégoire Broquet, Michel Ramonet, Olivier Laurent, Ivonne Albarus, Mali Chariot, Simone Kotthaus, Martial Haeffelin, Olivier Sanchez, Olivier Perrussel, Hugo Anne Denier van der Gon, Stijn Nicolaas Camiel Dellaert, and Philippe Ciais
Atmos. Chem. Phys., 23, 8823–8835, https://doi.org/10.5194/acp-23-8823-2023, https://doi.org/10.5194/acp-23-8823-2023, 2023
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This study quantifies urban CO2 emissions via an atmospheric inversion for the Paris metropolitan area over a 6-year period from 2016 to 2021. Results show a long-term decreasing trend of about 2 % ± 0.6 % per year in the annual CO2 emissions over Paris. We conclude that our current capacity can deliver near-real-time CO2 emission estimates at the city scale in under a month, and the results agree within 10 % with independent estimates from multiple city-scale inventories.
Fu-Jie Zhu, Peng-Tuan Hu, and Wan-Li Ma
Atmos. Chem. Phys., 23, 8583–8590, https://doi.org/10.5194/acp-23-8583-2023, https://doi.org/10.5194/acp-23-8583-2023, 2023
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A new steady-state gas–particle partitioning model of polycyclic aromatic hydrocarbons was established based on the level-III multimedia fugacity model, which proved that the particulate proportion of PAHs in emissions was a crucial factor for G–P partitioning of PAHs. In addition, gaseous and particulate interference was also derived in the new steady-state model determined by the particulate proportion in emission that could derivate the G–P partitioning quotients from the equilibrium state.
Christian Hogrefe, Jesse O. Bash, Jonathan E. Pleim, Donna B. Schwede, Robert C. Gilliam, Kristen M. Foley, K. Wyat Appel, and Rohit Mathur
Atmos. Chem. Phys., 23, 8119–8147, https://doi.org/10.5194/acp-23-8119-2023, https://doi.org/10.5194/acp-23-8119-2023, 2023
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Under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in the widely used CMAQ model. The results illustrate how these tools can provide insights into similarities and differences between the two CMAQ dry deposition options that affect simulated pollutant budgets and ecosystem impacts from atmospheric pollution.
Kun Qu, Xuesong Wang, Xuhui Cai, Yu Yan, Xipeng Jin, Mihalis Vrekoussis, Maria Kanakidou, Guy P. Brasseur, Jin Shen, Teng Xiao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 7653–7671, https://doi.org/10.5194/acp-23-7653-2023, https://doi.org/10.5194/acp-23-7653-2023, 2023
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Basic understandings of ozone processes, especially transport and chemistry, are essential to support ozone pollution control, but studies often have different views on their relative importance. We developed a method to quantify their contributions in the ozone mass and concentration budgets based on the WRF-CMAQ model. Results in a polluted region highlight the differences between two budgets. For future studies, two budgets are both needed to fully understand the effects of ozone processes.
Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
Atmos. Chem. Phys., 23, 7363–7382, https://doi.org/10.5194/acp-23-7363-2023, https://doi.org/10.5194/acp-23-7363-2023, 2023
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Surface observations of methane show that the seasonal cycle amplitude (SCA) of methane is decreasing in the northern high latitudes (NHLs) but increased globally (1995–2020). The NHL decrease is counterintuitive, as we expect the SCA to increase with increasing concentrations. We use a chemical transport model to investigate changes in SCA in the NHLs. We find well-mixed methane and changes in emissions from Canada, the Middle East, and Europe are the largest contributors to the SCA in NHLs.
Danyang Ma, Tijian Wang, Hao Wu, Yawei Qu, Jian Liu, Jane Liu, Shu Li, Bingliang Zhuang, Mengmeng Li, and Min Xie
Atmos. Chem. Phys., 23, 6525–6544, https://doi.org/10.5194/acp-23-6525-2023, https://doi.org/10.5194/acp-23-6525-2023, 2023
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Increasing surface ozone (O3) concentrations have long been a significant environmental issue in China, despite the Clean Air Action Plan launched in 2013. Most previous research ignores the contributions of CO2 variations. Our study comprehensively analyzed O3 variation across China from various perspectives and highlighted the importance of considering CO2 variations when designing long-term O3 control policies, especially in high-vegetation-coverage areas.
Jackson Hian-Wui Chang, Stephen M. Griffith, Steven Soon-Kai Kong, Ming-Tung Chuang, and Neng-Huei Lin
Atmos. Chem. Phys., 23, 6357–6382, https://doi.org/10.5194/acp-23-6357-2023, https://doi.org/10.5194/acp-23-6357-2023, 2023
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A novel CMAQ–PMF-based composite index is developed to identify the key VOC source species for an effective ozone abatement strategy. The index provides information as to which VOC species are key to ozone formation and where to reduce sources of these VOC species. Using the composite index, we recommended the VOC control measures in southern Taiwan should prioritize solvent usage, vehicle emissions, and the petrochemical industry.
Lei Duan and Ken Caldeira
Atmos. Chem. Phys., 23, 6011–6020, https://doi.org/10.5194/acp-23-6011-2023, https://doi.org/10.5194/acp-23-6011-2023, 2023
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Ocko and Hamburg (2022) emphasize the short-term climate impact of hydrogen, and we present an analysis that places greater focus on long-term outcomes. We have derived equations that describe the time-evolving impact of hydrogen and show that higher methane leakage is primarily responsible for the warming potential of blue hydrogen, while hydrogen leakage plays a less critical role. Fossil fuels show more prominent longer-term climate impacts than clean hydrogen under all emission scenarios.
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Short summary
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.
The changes in mobility across Europe due to the COVID-19 lockdowns had consequences for air...
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