Articles | Volume 15, issue 6
Atmos. Chem. Phys., 15, 3289–3301, 2015
https://doi.org/10.5194/acp-15-3289-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Special issue: HCCT-2010: a complex ground-based experiment on aerosol-cloud...
Atmos. Chem. Phys., 15, 3289–3301, 2015
https://doi.org/10.5194/acp-15-3289-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article 23 Mar 2015
Research article | 23 Mar 2015
The influence of clouds on radical concentrations: observations and modelling studies of HOx during the Hill Cap Cloud Thuringia (HCCT) campaign in 2010
L. K. Whalley et al.
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We analysed the chemical composition of ultrafine particles from 10–56 nm near Frankfurt Airport based on cascade impactor samples. We used an offline non-target screening to determine size-resolved molecular fingerprints. Unambiguous attribution of two homologous ester series to jet engine oils enables a new strategy of source attribution and explains the majority of the detected compounds. In addition, we identified additives of jet oils and a detrimental thermal transformation product.
Laurent Poulain, Benjamin Fahlbusch, Gerald Spindler, Konrad Müller, Dominik van Pinxteren, Zhijun Wu, Yoshiteru Iinuma, Wolfram Birmili, Alfred Wiedensohler, and Hartmut Herrmann
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Christoph A. Keller, Mathew J. Evans, K. Emma Knowland, Christa A. Hasenkopf, Sruti Modekurty, Robert A. Lucchesi, Tomohiro Oda, Bruno B. Franca, Felipe C. Mandarino, M. Valeria Díaz Suárez, Robert G. Ryan, Luke H. Fakes, and Steven Pawson
Atmos. Chem. Phys., 21, 3555–3592, https://doi.org/10.5194/acp-21-3555-2021, https://doi.org/10.5194/acp-21-3555-2021, 2021
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This study combines surface observations and model simulations to quantify the impact of COVID-19 restrictions on air quality across the world. The presented methodology removes the confounding impacts of meteorology on air pollution. Our results indicate that surface concentrations of nitrogen dioxide, an important air pollutant emitted during the combustion of fossil fuels, declined by up to 60 % following the implementation of COVID-19 containment measures.
Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Archit Mehra, Stephen D. Worrall, Asan Bacak, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Tuan Vu, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 2125–2147, https://doi.org/10.5194/acp-21-2125-2021, https://doi.org/10.5194/acp-21-2125-2021, 2021
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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.
Jing Dou, Peter A. Alpert, Pablo Corral Arroyo, Beiping Luo, Frederic Schneider, Jacinta Xto, Thomas Huthwelker, Camelia N. Borca, Katja D. Henzler, Jörg Raabe, Benjamin Watts, Hartmut Herrmann, Thomas Peter, Markus Ammann, and Ulrich K. Krieger
Atmos. Chem. Phys., 21, 315–338, https://doi.org/10.5194/acp-21-315-2021, https://doi.org/10.5194/acp-21-315-2021, 2021
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Photochemistry of iron(III) complexes plays an important role in aerosol aging, especially in the lower troposphere. Ensuing radical chemistry leads to decarboxylation, and the production of peroxides, and oxygenated volatile compounds, resulting in particle mass loss due to release of the volatile products to the gas phase. We investigated kinetic transport limitations due to high particle viscosity under low relative humidity conditions. For quantification a numerical model was developed.
Nadja Triesch, Manuela van Pinxteren, Anja Engel, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 163–181, https://doi.org/10.5194/acp-21-163-2021, https://doi.org/10.5194/acp-21-163-2021, 2021
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To investigate the sources of free amino acids (FAAs) in the marine atmosphere, concerted measurements (the simultaneous investigation of seawater, size-segregated aerosol particles and cloud water) were performed at the Cabo Verde islands. This study describes the transfer of FAAs as part of organic matter from the ocean into the atmosphere on a molecular level. In the investigated marine environment, a high enrichment of FAAs in submicron aerosol particles and in cloud droplets was observed.
Huan Song, Xiaorui Chen, Keding Lu, Qi Zou, Zhaofeng Tan, Hendrik Fuchs, Alfred Wiedensohler, Daniel R. Moon, Dwayne E. Heard, María-Teresa Baeza-Romero, Mei Zheng, Andreas Wahner, Astrid Kiendler-Scharr, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 15835–15850, https://doi.org/10.5194/acp-20-15835-2020, https://doi.org/10.5194/acp-20-15835-2020, 2020
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Accurate calculation of the HO2 uptake coefficient is one of the key parameters to quantify the co-reduction of both aerosol and ozone pollution. We modelled various lab measurements of γHO2 based on a gas-liquid phase kinetic model and developed a state-of-the-art parameterized equation. Based on a dataset from a comprehensive field campaign in the North China Plain, we proposed that the determination of the heterogeneous uptake process for HO2 should be included in future field campaigns.
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.
Jiarong Li, Chao Zhu, Hui Chen, Defeng Zhao, Likun Xue, Xinfeng Wang, Hongyong Li, Pengfei Liu, Junfeng Liu, Chenglong Zhang, Yujing Mu, Wenjin Zhang, Luming Zhang, Hartmut Herrmann, Kai Li, Min Liu, and Jianmin Chen
Atmos. Chem. Phys., 20, 13735–13751, https://doi.org/10.5194/acp-20-13735-2020, https://doi.org/10.5194/acp-20-13735-2020, 2020
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Based on a field study at Mt. Tai, China, the simultaneous variations of cloud microphysics, aerosol microphysics and their potential interactions during cloud life cycles were discussed. Results demonstrated that clouds on clean days were more susceptible to the concentrations of particle number, while clouds formed on polluted days might be more sensitive to meteorological parameters. Particles larger than 150 nm played important roles in forming cloud droplets with sizes of 5–10 μm.
R. Anthony Cox, Markus Ammann, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 20, 13497–13519, https://doi.org/10.5194/acp-20-13497-2020, https://doi.org/10.5194/acp-20-13497-2020, 2020
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Criegee intermediates, formed from alkene–ozone reactions, play a potentially important role as tropospheric oxidants. Evaluated kinetic data are provided for reactions governing their formation and removal for use in atmospheric models. These include their formation from reactions of simple and complex alkenes and removal by decomposition and reaction with a number of atmospheric species (e.g. H2O, SO2). An overview of the tropospheric chemistry of Criegee intermediates is also provided.
Yangang Ren, Bastian Stieger, Gerald Spindler, Benoit Grosselin, Abdelwahid Mellouki, Thomas Tuch, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 20, 13069–13089, https://doi.org/10.5194/acp-20-13069-2020, https://doi.org/10.5194/acp-20-13069-2020, 2020
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We present HONO measurements from the TROPOS research site in Melpitz, Germany. Investigations of HONO sources and sinks revealed the nighttime formation by heterogeneous conversion of NO2 to HONO followed by a significant surface deposition at night. The evaporation of dew was identified as the main HONO source in the morning. In the following, dew measurements with a self-made dew collector were performed to estimate the amount of evaporated HONO from dew in the atmospheric HONO distribution.
Hans-Christian Clemen, Johannes Schneider, Thomas Klimach, Frank Helleis, Franziska Köllner, Andreas Hünig, Florian Rubach, Stephan Mertes, Heike Wex, Frank Stratmann, André Welti, Rebecca Kohl, Fabian Frank, and Stephan Borrmann
Atmos. Meas. Tech., 13, 5923–5953, https://doi.org/10.5194/amt-13-5923-2020, https://doi.org/10.5194/amt-13-5923-2020, 2020
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We improved the efficiency of a single-particle mass spectrometer with a newly developed aerodynamic lens system, delayed ion extraction, and better electric shielding. The new components result in significantly improved particle analysis and sample statistics. This is particularly important for measurements of low-number-density particles, such as ice-nucleating particles, and for aircraft-based measurements at high altitudes or where high temporal and spatial resolution is required.
Laurent Poulain, Gerald Spindler, Achim Grüner, Thomas Tuch, Bastian Stieger, Dominik van Pinxteren, Jean-Eudes Petit, Olivier Favez, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Meas. Tech., 13, 4973–4994, https://doi.org/10.5194/amt-13-4973-2020, https://doi.org/10.5194/amt-13-4973-2020, 2020
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The stability and the comparability between ACSM and collocated filter sampling and MPSS measurements was investigated in order to examine the instruments robustness for year-long measurements. Specific attention was paid to the influence of the upper size cutoff diameter to better understand how it might affect the data validation. Recommendations are provided for better on-site quality assurance and quality control of the ACSM, which would be useful for either long-term or intensive campaigns.
Khanneh Wadinga Fomba, Nabil Deabji, Sayf El Islam Barcha, Ibrahim Ouchen, El Mehdi Elbaramoussi, Rajaa Cherkaoui El Moursli, Mimoun Harnafi, Souad El Hajjaji, Abdelwahid Mellouki, and Hartmut Herrmann
Atmos. Meas. Tech., 13, 4773–4790, https://doi.org/10.5194/amt-13-4773-2020, https://doi.org/10.5194/amt-13-4773-2020, 2020
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As air quality monitoring networks often sample aerosol particles on quartz filters, the development and applicability of analytical methods with quartz filters are becoming important. In this study different filter preparation methods (e.g., baking, acid digestion) were investigated for quantifying trace metals on quartz and polycarbonate filters, and cloud water using the total reflection X-Ray fluorescence (TXRF) technique, with low detection limits of about 0.3 ng cm−3 for some elements.
Ahmad Jhony Rusumdar, Andreas Tilgner, Ralf Wolke, and Hartmut Herrmann
Atmos. Chem. Phys., 20, 10351–10377, https://doi.org/10.5194/acp-20-10351-2020, https://doi.org/10.5194/acp-20-10351-2020, 2020
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In the present study, simulations with the SPACCIM-SpactMod multiphase chemistry model are performed. The investigations aim at assessing the impact of a detailed treatment of non-ideality in multiphase models dealing with aqueous aerosol chemistry. The model studies demonstrate that the inclusion of non-ideality considerably affects the multiphase chemical processing of transition metal ions, oxidants, and related chemical subsystems such as organic chemistry in aqueous aerosols.
Sebastian Zeppenfeld, Manuela van Pinxteren, Anja Engel, and Hartmut Herrmann
Ocean Sci., 16, 817–830, https://doi.org/10.5194/os-16-817-2020, https://doi.org/10.5194/os-16-817-2020, 2020
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An analytical method combining electro-dialysis with high-performance anionic exchange chromatography coupled to pulsed amperometric detection was developed and optimized for analyzing free and combined carbohydrates in seawater and other saline environmental samples.
Peter D. Ivatt and Mathew J. Evans
Atmos. Chem. Phys., 20, 8063–8082, https://doi.org/10.5194/acp-20-8063-2020, https://doi.org/10.5194/acp-20-8063-2020, 2020
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We investigate the potential of using a decision tree algorithm to identify and correct the tropospheric ozone bias in a chemical transport model. We train the algorithm on 2010–2015 ground and column observation data and test the algorithm on the 2016–2017 data using the ground data as well as independent flight data. We find the algorithm is successfully able to identify and correct the bias, improving the model performance.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
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.
Jiayue Huang, Lyatt Jaeglé, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mat J. Evans, Nicolas Theys, and Sungyeon Choi
Atmos. Chem. Phys., 20, 7335–7358, https://doi.org/10.5194/acp-20-7335-2020, https://doi.org/10.5194/acp-20-7335-2020, 2020
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Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often observed in the springtime Arctic. Here, we use a chemical transport model to examine the role of sea salt aerosol from blowing snow in explaining these phenomena. We find that our simulation can account for the spatiotemporal variability of satellite observations of BrO. However, the model has difficulty in producing the magnitude of observed ozone depletion events.
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.
Robert Woodward-Massey, Eloise J. Slater, Jake Alen, Trevor Ingham, Danny R. Cryer, Leanne M. Stimpson, Chunxiang Ye, Paul W. Seakins, Lisa K. Whalley, and Dwayne E. Heard
Atmos. Meas. Tech., 13, 3119–3146, https://doi.org/10.5194/amt-13-3119-2020, https://doi.org/10.5194/amt-13-3119-2020, 2020
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The OH radical is known as nature’s detergent, removing most trace gases from the atmosphere. Hence, an accurate measurement of its concentration is very important. We present measurements of OH in several field locations using a laser-based fluorescence method equipped with an OH scavenger. By determining the background signal in two different ways, we show that the instrument does not suffer any significant interferences that could result in an overestimation of OH concentrations.
Yanhong Zhu, Andreas Tilgner, Erik Hans Hoffmann, Hartmut Herrmann, Kimitaka Kawamura, Lingxiao Yang, Likun Xue, and Wenxing Wang
Atmos. Chem. Phys., 20, 6725–6747, https://doi.org/10.5194/acp-20-6725-2020, https://doi.org/10.5194/acp-20-6725-2020, 2020
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The formation and processing of secondary inorganic and organic compounds at Mt. Tai, the highest mountain on the North China Plain, are modeled using a multiphase chemical model. The concentrations of key radical and non-radical oxidations in the formation processes are investigated. Sensitivity tests assess the impacts of emission data and glyoxal partitioning constants on modeled results. The key precursors of secondary organic compounds are also identified.
Erik H. Hoffmann, Roland Schrödner, Andreas Tilgner, Ralf Wolke, and Hartmut Herrmann
Geosci. Model Dev., 13, 2587–2609, https://doi.org/10.5194/gmd-13-2587-2020, https://doi.org/10.5194/gmd-13-2587-2020, 2020
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A condensed multiphase halogen and DMS chemistry mechanism for application in chemical transport models has been developed and applied by 2D simulations to explore multiphase marine chemistry above the pristine open ocean. The model simulations have demonstrated the ability of the mechanism in studying aerosol cloud processing effects in the marine atmosphere. First 2D simulations have shown significant differences in the DMS processing under convective and stratiform cloud conditions.
Nicolás Zabalegui, Malena Manzi, Antoine Depoorter, Nathalie Hayeck, Marie Roveretto, Chunlin Li, Manuela van Pinxteren, Hartmut Herrmann, Christian George, and María Eugenia Monge
Atmos. Chem. Phys., 20, 6243–6257, https://doi.org/10.5194/acp-20-6243-2020, https://doi.org/10.5194/acp-20-6243-2020, 2020
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A new approach to bridging different fields of science by studying the air–sea interface is described. An untargeted ambient mass-spectrometry-based metabolomics method enables the study of enriched organic compounds found on the sea surface for air–water transfer processes. Results from the metabolomics experiments and a lab-to-field approach provide new opportunities for characterizing the seawater organic-matter content and discovering compounds involved in aerosol-formation processes.
Lavinia Onel, Alexander Brennan, Michele Gianella, James Hooper, Nicole Ng, Gus Hancock, Lisa Whalley, Paul W. Seakins, Grant A. D. Ritchie, and Dwayne E. Heard
Atmos. Meas. Tech., 13, 2441–2456, https://doi.org/10.5194/amt-13-2441-2020, https://doi.org/10.5194/amt-13-2441-2020, 2020
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Ryan J. Pound, Tomás Sherwen, Detlev Helmig, Lucy J. Carpenter, and Mat J. Evans
Atmos. Chem. Phys., 20, 4227–4239, https://doi.org/10.5194/acp-20-4227-2020, https://doi.org/10.5194/acp-20-4227-2020, 2020
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Ozone is an important pollutant with impacts on health and the environment. Ozone is lost to plants, land and the oceans. Loss to the ocean is slow compared to all other types of land cover and has not received as much attention. We build on previous work to more accurately model ozone loss to the ocean. We find changes in the concentration of ozone over the oceans, notably the Southern Ocean, which improves model performance.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Thomas H. Speak, Mark A. Blitz, Daniel Stone, and Paul W. Seakins
Atmos. Meas. Tech., 13, 839–852, https://doi.org/10.5194/amt-13-839-2020, https://doi.org/10.5194/amt-13-839-2020, 2020
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OH and HO2 radicals are important trace constituents of the atmosphere that are closely coupled via several types of reaction. This paper describes a new laboratory method to simultaneously determine OH kinetics and HO2 yields from chemical processes. The instrument also provides some time resolution on HO2 detection allowing one to separate HO2 produced from the target reaction from HO2 arising from secondary chemistry. Examples of applications are presented.
Xianda Gong, Heike Wex, Jens Voigtländer, Khanneh Wadinga Fomba, Kay Weinhold, Manuela van Pinxteren, Silvia Henning, Thomas Müller, Hartmut Herrmann, and Frank Stratmann
Atmos. Chem. Phys., 20, 1431–1449, https://doi.org/10.5194/acp-20-1431-2020, https://doi.org/10.5194/acp-20-1431-2020, 2020
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We characterized the aerosol particles in Cabo Verde at sea and cloud levels. We found four well-separable types of PNSDs, with the strongest differences between air masses coming from the ocean compared to from the African continent. During the strongest observed dust periods, CCN concentrations were 2.5 higher than during clean marine periods. The hygroscopicity of the particles did not vary much between different periods. Aerosol at sea level and on the mountaintop was well in agreement.
Xianda Gong, Heike Wex, Manuela van Pinxteren, Nadja Triesch, Khanneh Wadinga Fomba, Jasmin Lubitz, Christian Stolle, Tiera-Brandy Robinson, Thomas Müller, Hartmut Herrmann, and Frank Stratmann
Atmos. Chem. Phys., 20, 1451–1468, https://doi.org/10.5194/acp-20-1451-2020, https://doi.org/10.5194/acp-20-1451-2020, 2020
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In this study, we examined number concentrations of ice nucleating particles (INPs) at Cabo Verde in the oceanic sea surface microlayer and underlying seawater, in the air close to both sea level and cloud level, and in cloud water. The results show that most INPs are supermicron in size, that INP number concentrations in air fit well to those in cloud water and that sea spray aerosols at maximum contributed a small fraction of all INPs in the air at Cabo Verde.
Marco Paglione, Stefania Gilardoni, Matteo Rinaldi, Stefano Decesari, Nicola Zanca, Silvia Sandrini, Lara Giulianelli, Dimitri Bacco, Silvia Ferrari, Vanes Poluzzi, Fabiana Scotto, Arianna Trentini, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Francesco Canonaco, André S. H. Prévôt, Paola Massoli, Claudio Carbone, Maria Cristina Facchini, and Sandro Fuzzi
Atmos. Chem. Phys., 20, 1233–1254, https://doi.org/10.5194/acp-20-1233-2020, https://doi.org/10.5194/acp-20-1233-2020, 2020
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Our multi-year observational study regarding organic aerosol (OA) in the Po Valley indicates that more than half of OA is of secondary origin (SOA) through all the year and at both urban and rural sites. Within the SOA, the measurements show the importance of biomass burning (BB) aging products during cold seasons and indicate aqueous-phase processing of BB emissions as a fundamental driver of SOA formation in wintertime, with important consequences for air quality policy at the global level.
Tao Li, Zhe Wang, Yaru Wang, Chen Wu, Yiheng Liang, Men Xia, Chuan Yu, Hui Yun, Weihao Wang, Yan Wang, Jia Guo, Hartmut Herrmann, and Tao Wang
Atmos. Chem. Phys., 20, 391–407, https://doi.org/10.5194/acp-20-391-2020, https://doi.org/10.5194/acp-20-391-2020, 2020
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This work presents a field study of cloud water chemistry and interactions of cloud, gas, and aerosols in the polluted coastal boundary layer in southern China. Substantial dissolved organic matter in the acidic cloud water was observed, and the gas- and aqueous-phase partitioning of carbonyl compounds was investigated. The results demonstrated the significant role of cloud processing in altering aerosol properties, especially in producing aqueous organics and droplet-mode aerosols.
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.
Sophie L. Haslett, Jonathan W. Taylor, Mathew Evans, Eleanor Morris, Bernhard Vogel, Alima Dajuma, Joel Brito, Anneke M. Batenburg, Stephan Borrmann, Johannes Schneider, Christiane Schulz, Cyrielle Denjean, Thierry Bourrianne, Peter Knippertz, Régis Dupuy, Alfons Schwarzenböck, Daniel Sauer, Cyrille Flamant, James Dorsey, Ian Crawford, and Hugh Coe
Atmos. Chem. Phys., 19, 15217–15234, https://doi.org/10.5194/acp-19-15217-2019, https://doi.org/10.5194/acp-19-15217-2019, 2019
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Three aircraft datasets from the DACCIWA campaign in summer 2016 are used here to show there is a background mass of pollution present in the lower atmosphere in southern West Africa. We suggest that this likely comes from biomass burning in central and southern Africa, which has been carried into the region over the Atlantic Ocean. This would have a negative health impact on populations living near the coast and may alter the impact of growing city emissions on cloud formation and the monsoon.
André Ehrlich, Manfred Wendisch, Christof Lüpkes, Matthias Buschmann, Heiko Bozem, Dmitri Chechin, Hans-Christian Clemen, Régis Dupuy, Olliver Eppers, Jörg Hartmann, Andreas Herber, Evelyn Jäkel, Emma Järvinen, Olivier Jourdan, Udo Kästner, Leif-Leonard Kliesch, Franziska Köllner, Mario Mech, Stephan Mertes, Roland Neuber, Elena Ruiz-Donoso, Martin Schnaiter, Johannes Schneider, Johannes Stapf, and Marco Zanatta
Earth Syst. Sci. Data, 11, 1853–1881, https://doi.org/10.5194/essd-11-1853-2019, https://doi.org/10.5194/essd-11-1853-2019, 2019
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During the Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD) campaign, two research aircraft (Polar 5 and 6) jointly performed 22 research flights over the transition zone between open ocean and closed sea ice. The data set combines remote sensing and in situ measurement of cloud, aerosol, and trace gas properties, as well as turbulent and radiative fluxes, which will be used to study Arctic boundary layer and mid-level clouds and their role in Arctic amplification.
Simonas Kecorius, Teresa Vogl, Pauli Paasonen, Janne Lampilahti, Daniel Rothenberg, Heike Wex, Sebastian Zeppenfeld, Manuela van Pinxteren, Markus Hartmann, Silvia Henning, Xianda Gong, Andre Welti, Markku Kulmala, Frank Stratmann, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Chem. Phys., 19, 14339–14364, https://doi.org/10.5194/acp-19-14339-2019, https://doi.org/10.5194/acp-19-14339-2019, 2019
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Arctic sea-ice retreat, atmospheric new particle formation (NPF), and aerosol–cloud interaction may all be linked via a positive feedback mechanism. Understanding the sources of cloud condensation nuclei (CCN) is an important piece in the Arctic amplification puzzle. We show that Arctic newly formed particles do not have to grow beyond the Aitken mode to act as CCN. This is important, because NPF occurrence in the Arctic is expected to increase, making it a significant contributor to CCN budget.
Tomás Sherwen, Rosie J. Chance, Liselotte Tinel, Daniel Ellis, Mat J. Evans, and Lucy J. Carpenter
Earth Syst. Sci. Data, 11, 1239–1262, https://doi.org/10.5194/essd-11-1239-2019, https://doi.org/10.5194/essd-11-1239-2019, 2019
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Iodine plays an important role in the Earth system, as a nutrient to the biosphere and by changing the concentrations of climate and air-quality species. However, there are uncertainties on the magnitude of iodine’s role, and a key uncertainty is our understanding of iodide in the global sea-surface. Here we take a data-driven approach using a machine learning algorithm to convert a sparse set of sea-surface iodide observations into a spatially and temporally resolved dataset for use in models.
Michael Hollaway, Oliver Wild, Ting Yang, Yele Sun, Weiqi Xu, Conghui Xie, Lisa Whalley, Eloise Slater, Dwayne Heard, and Dantong Liu
Atmos. Chem. Phys., 19, 9699–9714, https://doi.org/10.5194/acp-19-9699-2019, https://doi.org/10.5194/acp-19-9699-2019, 2019
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This study, for the first time, uses combinations of aerosol and lidar data to drive an offline photolysis scheme. Absorbing species are shown to have the greatest impact on photolysis rate constants in the winter and scattering aerosol are shown to dominate responses in the summer. During haze episodes, aerosols are shown to produce a greater impact than cloud cover. The findings demonstrate the potential photochemical impacts of haze pollution in a highly polluted urban environment.
Peter Bräuer, Camille Mouchel-Vallon, Andreas Tilgner, Anke Mutzel, Olaf Böge, Maria Rodigast, Laurent Poulain, Dominik van Pinxteren, Ralf Wolke, Bernard Aumont, and Hartmut Herrmann
Atmos. Chem. Phys., 19, 9209–9239, https://doi.org/10.5194/acp-19-9209-2019, https://doi.org/10.5194/acp-19-9209-2019, 2019
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The article presents a new protocol for computer-assisted automated aqueous-phase chemistry mechanism generation, which has been validated against chamber experiments. Together with a large kinetics database and improved prediction methods for kinetic data, the novel protocol provides an unmatched tool for detailed studies of tropospheric aqueous-phase chemistry in complex model studies and for the design and analysis of chamber experiments.
Jan Chylik, Stephan Mertes, and Roel A. J. Neggers
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-637, https://doi.org/10.5194/acp-2019-637, 2019
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Arctic low-levels clouds play an important role in the Arctic warming, however they are not properly represented in weather and climate models. Among other issues, there are difficulties with balance of ice and liquid in clouds, as well as interaction between clouds and aerosols. In this model study, we focus on the way that variation in the concentration of aerosols affect the evolution of clouds and the turbulence. Model scenarios are based on the observations during the ACLOUD campaign.
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.
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Christoph A. Keller and Mat J. Evans
Geosci. Model Dev., 12, 1209–1225, https://doi.org/10.5194/gmd-12-1209-2019, https://doi.org/10.5194/gmd-12-1209-2019, 2019
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Computer simulations of atmospheric chemistry are a central tool to study the impact of air pollutants on the environment. These models are highly complex and require a lot of computing resources. In this study we show that machine learning can be used to predict air pollution with an accuracy that is comparable to the traditional, computationally expensive method. Such a machine-learning-based model has the potential to be orders of magnitude faster.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Kate R. Smith, Peter M. Edwards, Peter D. Ivatt, James D. Lee, Freya Squires, Chengliang Dai, Richard E. Peltier, Mat J. Evans, Yele Sun, and Alastair C. Lewis
Atmos. Meas. Tech., 12, 1325–1336, https://doi.org/10.5194/amt-12-1325-2019, https://doi.org/10.5194/amt-12-1325-2019, 2019
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Clusters of low-cost, low-power atmospheric gas sensors were built into a sensor instrument to monitor NO2 and O3 in Beijing, alongside reference instruments, aiming to improve the reliability of sensor measurements. Clustering identical sensors and using the median sensor signal was used to minimize drift over short and medium timescales. Three different machine learning techniques were used for all the sensor data in an attempt to correct for cross-interferences, which worked to some degree.
Federica Pacifico, Claire Delon, Corinne Jambert, Pierre Durand, Eleanor Morris, Mat J. Evans, Fabienne Lohou, Solène Derrien, Venance H. E. Donnou, Arnaud V. Houeto, Irene Reinares Martínez, and Pierre-Etienne Brilouet
Atmos. Chem. Phys., 19, 2299–2325, https://doi.org/10.5194/acp-19-2299-2019, https://doi.org/10.5194/acp-19-2299-2019, 2019
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Biogenic fluxes from soil at a local and regional scale are crucial to study air pollution and climate. Here we present field measurements of soil fluxes of nitric oxide (NO) and ammonia (NH3) observed over four different land cover types, i.e. bare soil, grassland, maize field, and forest, at an inland rural site in Benin, West Africa, during the DACCIWA field campaign in
June and July 2016.
Bastian Stieger, Gerald Spindler, Dominik van Pinxteren, Achim Grüner, Markus Wallasch, and Hartmut Herrmann
Atmos. Meas. Tech., 12, 281–298, https://doi.org/10.5194/amt-12-281-2019, https://doi.org/10.5194/amt-12-281-2019, 2019
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A MARGA was combined with an additional IC system specialized for the 2 h interval online quantification of 12 low-molecular-weight organic acids in the gas and particle phases. Low limits of detection and good precision were achieved. The suitability for field measurements was shown. This setup reduces laboratory work and filter sampling artifacts. Diurnal profiles, sources and phase distributions of these compounds will improve the knowledge of the tropospheric multiphase chemistry.
Shan Huang, Zhijun Wu, Laurent Poulain, Manuela van Pinxteren, Maik Merkel, Denise Assmann, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Chem. Phys., 18, 18043–18062, https://doi.org/10.5194/acp-18-18043-2018, https://doi.org/10.5194/acp-18-18043-2018, 2018
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The Atlantic aerosols are characterized based on high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurements during four open-ocean cruises. This unique data set provides the latitudinal distribution of source contributions of organic aerosols (OAs) over the Atlantic Ocean, showing that marine sources could control the OA formation over the South Atlantic, while strong continental influence was found near Africa and Europe.
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.
Christiane Schulz, Johannes Schneider, Bruna Amorim Holanda, Oliver Appel, Anja Costa, Suzane S. de Sá, Volker Dreiling, Daniel Fütterer, Tina Jurkat-Witschas, Thomas Klimach, Christoph Knote, Martina Krämer, Scot T. Martin, Stephan Mertes, Mira L. Pöhlker, Daniel Sauer, Christiane Voigt, Adrian Walser, Bernadett Weinzierl, Helmut Ziereis, Martin Zöger, Meinrat O. Andreae, Paulo Artaxo, Luiz A. T. Machado, Ulrich Pöschl, Manfred Wendisch, and Stephan Borrmann
Atmos. Chem. Phys., 18, 14979–15001, https://doi.org/10.5194/acp-18-14979-2018, https://doi.org/10.5194/acp-18-14979-2018, 2018
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Aerosol chemical composition measurements in the tropical upper troposphere over the Amazon region show that 78 % of the aerosol in the upper troposphere consists of organic matter. Up to 20 % of the organic aerosol can be attributed to isoprene epoxydiol secondary organic aerosol (IEPOX-SOA). Furthermore, organic nitrates were identified, suggesting a connection to the IEPOX-SOA formation.
Stine Eriksen Hammer, Stephan Mertes, Johannes Schneider, Martin Ebert, Konrad Kandler, and Stephan Weinbruch
Atmos. Chem. Phys., 18, 13987–14003, https://doi.org/10.5194/acp-18-13987-2018, https://doi.org/10.5194/acp-18-13987-2018, 2018
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It is important to study ice-nucleating particles in the environment to learn more about cloud formation. We studied the composition of ice particle residuals and total aerosol particles sampled in parallel during mixed-phase cloud events at Jungfraujoch and discovered that soot and complex secondary particles were not present. In contrast, silica, aluminosilicates, and other aluminosilicates were the most important ice particle residual groups at site temperatures between −11 and −18 °C.
Qianjie Chen, Tomás Sherwen, Mathew Evans, and Becky Alexander
Atmos. Chem. Phys., 18, 13617–13637, https://doi.org/10.5194/acp-18-13617-2018, https://doi.org/10.5194/acp-18-13617-2018, 2018
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Uncertainty in the natural tropospheric sulfur cycle represents the largest source of uncertainty in radiative forcing estimates of sulfate aerosol. This study investigates the natural sulfur cycle in the marine troposphere using the GEOS-Chem model. We found that BrO is important for DMS oxidation and multiphase chemistry is important for MSA production and loss, which have implications for the yield of SO2 and MSA from DMS oxidation and the radiative effect of DMS-derived sulfate aerosol.
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.
Eleni Karnezi, Benjamin N. Murphy, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Florian Rubach, Astrid Kiendler-Scharr, Thomas F. Mentel, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 10759–10772, https://doi.org/10.5194/acp-18-10759-2018, https://doi.org/10.5194/acp-18-10759-2018, 2018
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Different parameterizations of the organic aerosol (OA) formation and evolution are evaluated using ground and airborne measurements collected in the 2012 PEGASOS field campaign in the Po Valley (Italy). Total OA concentration and O : C ratios were reproduced within experimental error by a number of schemes. Anthropogenic secondary OA (SOA) contributed 15–25 % of the total OA, 20–35 % of SOA from intermediate volatility compounds oxidation, and 15–45 % of biogenic SOA depending on the scheme.
Yanhong Zhu, Lingxiao Yang, Jianmin Chen, Kimitaka Kawamura, Mamiko Sato, Andreas Tilgner, Dominik van Pinxteren, Ying Chen, Likun Xue, Xinfeng Wang, Isobel J. Simpson, Hartmut Herrmann, Donald R. Blake, and Wenxing Wang
Atmos. Chem. Phys., 18, 10741–10758, https://doi.org/10.5194/acp-18-10741-2018, https://doi.org/10.5194/acp-18-10741-2018, 2018
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Molecular distributions of dicarboxylic acids, oxocarboxylic acids and α-dicarbonyls in the free troposphere are identified, and their concentration variations between 2014 and 2006 are presented. High nighttime concentrations were probably due to precursor emissions and aqueous-phase oxidation. Biomass burning was significant, but its tracer levoglucosan in 2014 was 5 times lower than 2006 concentrations. Finally, regional emission from anthropogenic activities was identified as a major source.
Mike J. Newland, Andrew R. Rickard, Tomás Sherwen, Mathew J. Evans, Luc Vereecken, Amalia Muñoz, Milagros Ródenas, and William J. Bloss
Atmos. Chem. Phys., 18, 6095–6120, https://doi.org/10.5194/acp-18-6095-2018, https://doi.org/10.5194/acp-18-6095-2018, 2018
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Stabilised Criegee intermediates (SCIs) are formed in the reaction of alkenes with ozone, both of which are ubiquitous throughout the troposphere. We determine the fate and global distribution of SCI from monoterpene ozonolysis. One major fate of SCI is reaction with H2O, but for a fraction of SCIs, unimolecular reactions dominate. Concentrations of SCIs are high enough regionally to play a key role in the conversion of sulfur dioxide to aerosol, affecting air quality and climate.
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.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
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.
Meinrat O. Andreae, Armin Afchine, Rachel Albrecht, Bruna Amorim Holanda, Paulo Artaxo, Henrique M. J. Barbosa, Stephan Borrmann, Micael A. Cecchini, Anja Costa, Maximilian Dollner, Daniel Fütterer, Emma Järvinen, Tina Jurkat, Thomas Klimach, Tobias Konemann, Christoph Knote, Martina Krämer, Trismono Krisna, Luiz A. T. Machado, Stephan Mertes, Andreas Minikin, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, Daniel Sauer, Hans Schlager, Martin Schnaiter, Johannes Schneider, Christiane Schulz, Antonio Spanu, Vinicius B. Sperling, Christiane Voigt, Adrian Walser, Jian Wang, Bernadett Weinzierl, Manfred Wendisch, and Helmut Ziereis
Atmos. Chem. Phys., 18, 921–961, https://doi.org/10.5194/acp-18-921-2018, https://doi.org/10.5194/acp-18-921-2018, 2018
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We made airborne measurements of aerosol particle concentrations and properties over the Amazon Basin. We found extremely high concentrations of very small particles in the region between 8 and 14 km altitude all across the basin, which had been recently formed by gas-to-particle conversion at these altitudes. This makes the upper troposphere a very important source region of atmospheric particles with significant implications for the Earth's climate system.
Daniel R. Moon, Giorgio S. Taverna, Clara Anduix-Canto, Trevor Ingham, Martyn P. Chipperfield, Paul W. Seakins, Maria-Teresa Baeza-Romero, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 327–338, https://doi.org/10.5194/acp-18-327-2018, https://doi.org/10.5194/acp-18-327-2018, 2018
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One geoengineering mitigation strategy for global temperature rises is to inject particles into the stratosphere to scatter solar radiation back to space. However, the injection of such particles must not perturb ozone. We measured the rate of uptake of HO2 radicals, an important stratospheric intermediate, onto TiO2 particles. Using the atmospheric model TOMCAT, we showed that surface reactions between HO2 and TiO2 would have a negligible effect on stratospheric concentrations of HO2 and ozone.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Lavinia Onel, Alexander Brennan, Michele Gianella, Grace Ronnie, Ana Lawry Aguila, Gus Hancock, Lisa Whalley, Paul W. Seakins, Grant A. D. Ritchie, and Dwayne E. Heard
Atmos. Meas. Tech., 10, 4877–4894, https://doi.org/10.5194/amt-10-4877-2017, https://doi.org/10.5194/amt-10-4877-2017, 2017
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Hydroperoxy (HO2) radicals are key intermediates participating in a rapid chemical cycling at the centre of the tropospheric oxidation. Fluorescence assay by gas expansion (FAGE) technique is the most commonly used for the HO2 measurements in the atmosphere. However, FAGE is an indirect technique, requiring calibration. This work finds a good agreement between the indirect FAGE method and the direct cavity ring-down spectroscopy method and hence validates FAGE and the FAGE calibration method.
Ben Newsome and Mat Evans
Atmos. Chem. Phys., 17, 14333–14352, https://doi.org/10.5194/acp-17-14333-2017, https://doi.org/10.5194/acp-17-14333-2017, 2017
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We explore the uncertainty in the predictions of a chemical transport model (GEOS-Chem) from uncertainty in 60 inorganic rate constants and photolysis rates. We find uncertainty in the global mean ozone burden of 10 %, in global mean OH of 16 %, methane lifetimes of 16 %, and tropospheric ozone radiative forcings of 13 %. Reductions in the uncertainty of rate constants of these simple reactions would reduce uncertainty in our understanding of atmospheric composition.
Peter M. Edwards and Mathew J. Evans
Atmos. Chem. Phys., 17, 13669–13680, https://doi.org/10.5194/acp-17-13669-2017, https://doi.org/10.5194/acp-17-13669-2017, 2017
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Understanding tropospheric ozone chemistry has been at the centre of the field of atmospheric chemistry for the last 30 years. However, our conceptual approach to diagnosing ozone production in global models has not advanced in this time. Our work presents a new and powerful approach for diagnosing tropospheric ozone production, providing a significant enhancement in our ability to understand the processes controlling ozone and how we can validate our assessment of these processes.
Kathrin Gatzsche, Yoshiteru Iinuma, Andreas Tilgner, Anke Mutzel, Torsten Berndt, and Ralf Wolke
Atmos. Chem. Phys., 17, 13187–13211, https://doi.org/10.5194/acp-17-13187-2017, https://doi.org/10.5194/acp-17-13187-2017, 2017
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Secondary organic aerosol (SOA) represents an important fraction of the particulate matter and, thus, an advanced treatment of SOA processes in models is necessary. Therefore, this investigation aims at sensitivity studies of a kinetic description of SOA formation. The results reveal that the particle-phase state and the reactivity of the organic solutes are key parameters in the SOA formation. Overall, the results show that an advanced kinetic treatment enables improved model predictions.
Lavinia Onel, Alexander Brennan, Paul W. Seakins, Lisa Whalley, and Dwayne E. Heard
Atmos. Meas. Tech., 10, 3985–4000, https://doi.org/10.5194/amt-10-3985-2017, https://doi.org/10.5194/amt-10-3985-2017, 2017
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Methyl peroxy (CH3O2) radicals are the most abundant organic peroxy radical species and are critical intermediates in rapid chemical cycling at the heart of tropospheric oxidation. Despite their importance, at present CH3O2 radicals are not specifically measured in the atmosphere by any direct or indirect method. This work presents a new method for the selective and sensitive detection of CH3O2 radicals and its use for the measurement of CH3O2 in the atmospheric simulation chamber HIRAC.
Hendrik Fuchs, Anna Novelli, Michael Rolletter, Andreas Hofzumahaus, Eva Y. Pfannerstill, Stephan Kessel, Achim Edtbauer, Jonathan Williams, Vincent Michoud, Sebastien Dusanter, Nadine Locoge, Nora Zannoni, Valerie Gros, Francois Truong, Roland Sarda-Esteve, Danny R. Cryer, Charlotte A. Brumby, Lisa K. Whalley, Daniel Stone, Paul W. Seakins, Dwayne E. Heard, Coralie Schoemaecker, Marion Blocquet, Sebastien Coudert, Sebastien Batut, Christa Fittschen, Alexander B. Thames, William H. Brune, Cheryl Ernest, Hartwig Harder, Jennifer B. A. Muller, Thomas Elste, Dagmar Kubistin, Stefanie Andres, Birger Bohn, Thorsten Hohaus, Frank Holland, Xin Li, Franz Rohrer, Astrid Kiendler-Scharr, Ralf Tillmann, Robert Wegener, Zhujun Yu, Qi Zou, and Andreas Wahner
Atmos. Meas. Tech., 10, 4023–4053, https://doi.org/10.5194/amt-10-4023-2017, https://doi.org/10.5194/amt-10-4023-2017, 2017
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Hydroxyl radical reactivity (k(OH)) is closely related to processes that lead to the formation of oxidised, secondary pollutants such as ozone and aerosol. In order to compare the performances of instruments measuring k(OH), experiments were conducted in the simulation chamber SAPHIR. Chemical conditions were chosen either to be representative of the atmosphere or to test potential limitations of instruments. Overall, the results show that instruments are capable of measuring k(OH).
Qing Mu, Gerhard Lammel, Christian N. Gencarelli, Ian M. Hedgecock, Ying Chen, Petra Přibylová, Monique Teich, Yuxuan Zhang, Guangjie Zheng, Dominik van Pinxteren, Qiang Zhang, Hartmut Herrmann, Manabu Shiraiwa, Peter Spichtinger, Hang Su, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 17, 12253–12267, https://doi.org/10.5194/acp-17-12253-2017, https://doi.org/10.5194/acp-17-12253-2017, 2017
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Polycyclic aromatic hydrocarbons (PAHs) are hazardous pollutants with the largest emissions in East Asia. The regional WRF-Chem-PAH model has been developed to reflect the state-of-the-art understanding of current PAHs studies with several new or updated features. It is able to reasonably well simulate the concentration levels and particulate mass fractions of PAHs near the sources and at a remote outflow region of East Asia, in high spatial and temporal resolutions.
Peter Knippertz, Andreas H. Fink, Adrien Deroubaix, Eleanor Morris, Flore Tocquer, Mat J. Evans, Cyrille Flamant, Marco Gaetani, Christophe Lavaysse, Celine Mari, John H. Marsham, Rémi Meynadier, Abalo Affo-Dogo, Titike Bahaga, Fabien Brosse, Konrad Deetz, Ridha Guebsi, Issaou Latifou, Marlon Maranan, Philip D. Rosenberg, and Andreas Schlueter
Atmos. Chem. Phys., 17, 10893–10918, https://doi.org/10.5194/acp-17-10893-2017, https://doi.org/10.5194/acp-17-10893-2017, 2017
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In June–July 2016 DACCIWA (Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa), a large, EU-funded European–African project, organised an international field campaign in densely populated southern West Africa, including measurements from ground sites, research aircraft, weather balloons and urban sites. This paper gives an overview of the atmospheric evolution during this period focusing on meteorological (precipitation, cloudiness, winds) and composition (gases, particles) aspects.
Jiarong Li, Xinfeng Wang, Jianmin Chen, Chao Zhu, Weijun Li, Chengbao Li, Lu Liu, Caihong Xu, Liang Wen, Likun Xue, Wenxing Wang, Aijun Ding, and Hartmut Herrmann
Atmos. Chem. Phys., 17, 9885–9896, https://doi.org/10.5194/acp-17-9885-2017, https://doi.org/10.5194/acp-17-9885-2017, 2017
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Cloud events at Mt. Tai were investigated for the chemical composition and size distribution of cloud droplets. An obvious rise in pH was found for elevated NH+4 during the last decade. Higher PM2.5 levels resulted in higher concentrations of water-soluble ions, smaller sizes and higher numbers of cloud droplets. The mechanism of cloud-droplet formation and the mass transfer between aerosol–gas–cloud phases were summarized to enrich the knowledge of cloud chemical and microphysical properties.
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.
Maria Rodigast, Anke Mutzel, and Hartmut Herrmann
Atmos. Chem. Phys., 17, 3929–3943, https://doi.org/10.5194/acp-17-3929-2017, https://doi.org/10.5194/acp-17-3929-2017, 2017
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The study presents, for the first time, a quantification method for methylglyoxal oligomers and highlights their importance for SOA formation. The method was applied to determine the fraction of methylglyoxal oligomers of 1,3,5-trimethylbenzene SOA dependent on relative humidity and seed particle acidity. An oligomer contribution of up to 8 % was calculated varying with experimental conditions and thus further hints for the dependency of the oligomer formation mechanism on conditions were found.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Monique Teich, Dominik van Pinxteren, Michael Wang, Simonas Kecorius, Zhibin Wang, Thomas Müller, Griša Močnik, and Hartmut Herrmann
Atmos. Chem. Phys., 17, 1653–1672, https://doi.org/10.5194/acp-17-1653-2017, https://doi.org/10.5194/acp-17-1653-2017, 2017
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This study provides a large data set on concentrations of individual brown carbon constituents, i.e., nitrated aromatic compounds, in diverse atmospheric environments and their relative contribution to water-soluble and particulate light absorption. It extends the existing knowledge on the abundance of brown carbon and its molecular composition and provides scientific motivation for further studies on ambient brown carbon constituents.
Martin Brüggemann, Laurent Poulain, Andreas Held, Torsten Stelzer, Christoph Zuth, Stefanie Richters, Anke Mutzel, Dominik van Pinxteren, Yoshiteru Iinuma, Sarmite Katkevica, René Rabe, Hartmut Herrmann, and Thorsten Hoffmann
Atmos. Chem. Phys., 17, 1453–1469, https://doi.org/10.5194/acp-17-1453-2017, https://doi.org/10.5194/acp-17-1453-2017, 2017
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Using complementary mass spectrometric techniques during a field study in central Europe, characteristic contributors to the organic aerosol mass were identified. Besides common marker compounds for biogenic secondary organic aerosol, highly oxidized sulfur species were detected in the particle phase. High-time-resolution measurements revealed correlations between these organosulfates and particulate sulfate as well as gas-phase peroxyradicals, giving hints to underlying formation mechanisms.
Tomás Sherwen, Mat J. Evans, Lucy J. Carpenter, Johan A. Schmidt, and Loretta J. Mickley
Atmos. Chem. Phys., 17, 1557–1569, https://doi.org/10.5194/acp-17-1557-2017, https://doi.org/10.5194/acp-17-1557-2017, 2017
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We model pre-industrial to present day changes using the GEOS-Chem global chemical transport model with halogens (Cl, Br, I). The model better captures pre-industrial O3 observations with halogens included. Halogens buffer the tropospheric forcing of O3 (RFTO3) from pre-industrial to present day, reducing RFTO3 by 0.087 Wm−2. This reduction is greater than that from halogens on stratospheric O3 (−0.05 Wm−2). This suggests that models that do not include halogens will overestimate RFTO3by ~ 25%.
Johannes Schneider, Stephan Mertes, Dominik van Pinxteren, Hartmut Herrmann, and Stephan Borrmann
Atmos. Chem. Phys., 17, 1571–1593, https://doi.org/10.5194/acp-17-1571-2017, https://doi.org/10.5194/acp-17-1571-2017, 2017
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We analyzed the composition of cloud droplet residuals and of aerosol particles sampled on a mountaintop site. The data show that about 85 % of the submicron aerosol mass partitions into the cloud phase, and that the uptake of soluble compounds (nitric acid, ammonia, and organic gases) from the gas phase into the cloud droplets is very effective. This will lead to a redistribution of these compounds among the aerosol particles and thereby to a more uniform aerosol after cloud evaporation.
Susan Schmidt, Johannes Schneider, Thomas Klimach, Stephan Mertes, Ludwig Paul Schenk, Piotr Kupiszewski, Joachim Curtius, and Stephan Borrmann
Atmos. Chem. Phys., 17, 575–594, https://doi.org/10.5194/acp-17-575-2017, https://doi.org/10.5194/acp-17-575-2017, 2017
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Ice formation in clouds is an important process in the formation of precipitation, especially at midlatitudes, but the exact properties of the aerosol particles that initiate freezing is not fully understood. We analysed residual particles from ice crystals sampled from mixed phase clouds. The results show that the residues contain a larger relative amount of soil dust and minerals, but also particles from industrial emissions and lead-containing particles, than the out-of-cloud aerosol.
Pascale S. J. Lakey, Thomas Berkemeier, Manuel Krapf, Josef Dommen, Sarah S. Steimer, Lisa K. Whalley, Trevor Ingham, Maria T. Baeza-Romero, Ulrich Pöschl, Manabu Shiraiwa, Markus Ammann, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 13035–13047, https://doi.org/10.5194/acp-16-13035-2016, https://doi.org/10.5194/acp-16-13035-2016, 2016
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Chemical oxidation in the atmosphere removes pollutants and greenhouse gases but generates undesirable products such as secondary organic aerosol. Radicals are key intermediates in oxidation, but how they interact with aerosols is still not well understood. Here we use a laser to measure the loss of radicals onto oxidised aerosols generated in a smog chamber. The loss of radicals was controlled by the thickness or viscosity of the aerosols, confirmed by using sugar aerosols of known thickness.
Tomás Sherwen, Johan A. Schmidt, Mat J. Evans, Lucy J. Carpenter, Katja Großmann, Sebastian D. Eastham, Daniel J. Jacob, Barbara Dix, Theodore K. Koenig, Roman Sinreich, Ivan Ortega, Rainer Volkamer, Alfonso Saiz-Lopez, Cristina Prados-Roman, Anoop S. Mahajan, and Carlos Ordóñez
Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, https://doi.org/10.5194/acp-16-12239-2016, 2016
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We present a simulation of tropospheric Cl, Br, I chemistry within the GEOS-Chem CTM. We find a decrease in tropospheric ozone burden of 18.6 % and a 8.2 % decrease in global mean OH concentrations. Cl oxidation of some VOCs range from 15 to 27 % of the total loss. Bromine plays a small role in oxidising oVOCs. Surface ozone, ozone sondes, and methane lifetime are in general improved by the inclusion of halogens. We argue that simulated bromine and chlorine represent a lower limit.
Silvia Sandrini, Dominik van Pinxteren, Lara Giulianelli, Hartmut Herrmann, Laurent Poulain, Maria Cristina Facchini, Stefania Gilardoni, Matteo Rinaldi, Marco Paglione, Barbara J. Turpin, Francesca Pollini, Silvia Bucci, Nicola Zanca, and Stefano Decesari
Atmos. Chem. Phys., 16, 10879–10897, https://doi.org/10.5194/acp-16-10879-2016, https://doi.org/10.5194/acp-16-10879-2016, 2016
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This paper deals with impactor measurements performed in the summer 2012 during the EU project PEGASOS campaign in the Po Valley, at an urban and a rural site. The paper tries to disentangle the effects of weather anomalies (temporal and spatial) from those of diverse emissions (NH3) and chemical processes on the formation of secondary aerosols in the region, with special focus on nocturnal ammonium nitrate formation and its implications (aqueous formation of secondary organic aerosol).
Stefanie Richters, Hartmut Herrmann, and Torsten Berndt
Atmos. Chem. Phys., 16, 9831–9845, https://doi.org/10.5194/acp-16-9831-2016, https://doi.org/10.5194/acp-16-9831-2016, 2016
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New reaction pathways of highly oxidized multifunctional organic compounds (HOMs) from the ozonolysis of the sesquiterpene (C15H24) beta-caryophyllene were elucidated based on experiments using isotopically labelled ozone and H/D exchange experiments. These new insights in reaction pathways of unsaturated RO2 radicals are responsible for the production of about two-thirds of the detected HOMs from beta-caryophyllene and extend the knowledge of HOM formation mechanisms in the atmosphere.
Birger Bohn, Dwayne E. Heard, Nikolaos Mihalopoulos, Christian Plass-Dülmer, Rainer Schmitt, and Lisa K. Whalley
Atmos. Meas. Tech., 9, 3455–3466, https://doi.org/10.5194/amt-9-3455-2016, https://doi.org/10.5194/amt-9-3455-2016, 2016
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Filter radiometers are instruments that quantify the rate of formation of excited oxygen atoms from photolysis of ozone in the atmosphere. The excited oxygen atoms are important for the atmospheric self-cleaning ability. The radiometers were characterised by measurements of their spectral response. Together with field comparisons with a reference instrument, the characterisations improved the performance. That will help to better understand atmospheric photochemistry in future research.
Nan Ma, Chunsheng Zhao, Jiangchuan Tao, Zhijun Wu, Simonas Kecorius, Zhibin Wang, Johannes Größ, Hongjian Liu, Yuxuan Bian, Ye Kuang, Monique Teich, Gerald Spindler, Konrad Müller, Dominik van Pinxteren, Hartmut Herrmann, Min Hu, and Alfred Wiedensohler
Atmos. Chem. Phys., 16, 8593–8607, https://doi.org/10.5194/acp-16-8593-2016, https://doi.org/10.5194/acp-16-8593-2016, 2016
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New particle formation (NPF) is one of main sources of cloud condensation nuclei (CCN) in the atmosphere. Based on in situ measurements, we found that CCN activity of newly formed particles largely differs in different NPF events. It is therefore difficult to find a simple parameterization of CCN activity for NPF events. Using a fixed size-resolved activation ratio curve or critical diameter is very likely to result in large biases up to 50 % in the calculated NCCN during NPF events.
Dene R. Bowdalo, Mathew J. Evans, and Eric D. Sofen
Atmos. Chem. Phys., 16, 8295–8308, https://doi.org/10.5194/acp-16-8295-2016, https://doi.org/10.5194/acp-16-8295-2016, 2016
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We introduce a new methodology for the assessment of atmospheric models with observations. We apply a spectral analysis methodology to hourly ozone observations and the equivalent model output. The spectrally transformed observational data show significant peaks on daily and annual timescales. Comparison between the amplitude and phase of these peaks introduces a new comparison methodology between model and measurements. We find the model shows significant biases on an annual timescale.
Daniel Stone, Lisa K. Whalley, Trevor Ingham, Peter M. Edwards, Danny R. Cryer, Charlotte A. Brumby, Paul W. Seakins, and Dwayne E. Heard
Atmos. Meas. Tech., 9, 2827–2844, https://doi.org/10.5194/amt-9-2827-2016, https://doi.org/10.5194/amt-9-2827-2016, 2016
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OH reactivity is the total pseudo-first-order loss rate coefficient describing the removal of OH radicals to all sinks in the atmosphere. Measurements of ambient OH reactivity can be used to discover the extent to which measured OH sinks contribute to the total OH loss rate. In this work, we describe the design and characterisation of an instrument to measure OH reactivity using laser flash photolysis coupled to laser-induced fluorescence (LFP-LIF) spectroscopy.
Amy P. Sullivan, Natasha Hodas, Barbara J. Turpin, Kate Skog, Frank N. Keutsch, Stefania Gilardoni, Marco Paglione, Matteo Rinaldi, Stefano Decesari, Maria Cristina Facchini, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Eiko Nemitz, Marsailidh M. Twigg, and Jeffrey L. Collett Jr.
Atmos. Chem. Phys., 16, 8095–8108, https://doi.org/10.5194/acp-16-8095-2016, https://doi.org/10.5194/acp-16-8095-2016, 2016
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This paper presents the results from our measurements and approach for the investigation of aqueous secondary organic aerosol (aqSOA) formation in the ambient atmosphere. When local aqSOA formation was observed, a correlation of water-soluble organic carbon with organic aerosol, aerosol liquid water, relative humidity, and aerosol nitrate was found. Key factors of local aqSOA production include air mass stagnation, formation of local nitrate overnight, and significant amounts of ammonia.
James W. Grayson, Yue Zhang, Anke Mutzel, Lindsay Renbaum-Wolff, Olaf Böge, Saeid Kamal, Hartmut Herrmann, Scot T. Martin, and Allan K. Bertram
Atmos. Chem. Phys., 16, 6027–6040, https://doi.org/10.5194/acp-16-6027-2016, https://doi.org/10.5194/acp-16-6027-2016, 2016
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The effect of several experimental parameters on the viscosity of secondary organic material (SOM) generated from the ozonolysis of α-pinene has been studied. The results demonstrate that the viscosity of SOM depends on the particle mass concentration at which SOM is produced, and the relative humidity (RH) at which the SOM is studied. Hence, particle mass concentration and RH should be considered when comparing experimental results for SOM, or extrapolating laboratory results to the atmosphere.
Alicia Gressent, Bastien Sauvage, Daniel Cariolle, Mathew Evans, Maud Leriche, Céline Mari, and Valérie Thouret
Atmos. Chem. Phys., 16, 5867–5889, https://doi.org/10.5194/acp-16-5867-2016, https://doi.org/10.5194/acp-16-5867-2016, 2016
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In chemical transport models, NOx emitted by lightning (LNOx) is instantaneously diluted into the grid. A plume-in-grid parameterization to account for the sub-grid chemistry of LNOx is presented. This approach was implemented into the GEOS-Chem model and leads to a relative increase of NOx and O3 (18 % and 2 %, respectively, in July) on a large scale downwind of lightning emissions and a relative decrease (25 % and 8 %, respectively, over central Africa in July) over the regions of emissions.
Chris Reed, Mathew J. Evans, Piero Di Carlo, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 16, 4707–4724, https://doi.org/10.5194/acp-16-4707-2016, https://doi.org/10.5194/acp-16-4707-2016, 2016
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The self-cleaning capacity of the atmosphere in places like Antarctica can be measured by quantifying very low amounts of combustion products that exist in a well-known ratio. When this ratio deviates from 1 it points to the existence of unknown compounds. Several unknown compounds have been theorized to exist but never measured. We have found the method for measuring the ratio of combustion products suffers a bias in remote places, which when taken into account disproves any unknown compounds.
Frank A. F. Winiberg, Terry J. Dillon, Stephanie C. Orr, Christoph B. M Groß, Iustinian Bejan, Charlotte A. Brumby, Matthew J. Evans, Shona C. Smith, Dwayne E. Heard, and Paul W. Seakins
Atmos. Chem. Phys., 16, 4023–4042, https://doi.org/10.5194/acp-16-4023-2016, https://doi.org/10.5194/acp-16-4023-2016, 2016
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OH radicals are important intermediates in the atmosphere, and the high concentrations observed in tropical regions are yet to be fully explained. Radical-radical reactions such as the title reaction can contribute to OH formation. This is the most fully comprehensive study of the CH3C(O)O2 + HO2 reaction with direct observation of products in all reaction channels. The implications of the new measurements on OH, PAN and NOx concentrations are considered via global models.
Dominik van Pinxteren, Khanneh Wadinga Fomba, Stephan Mertes, Konrad Müller, Gerald Spindler, Johannes Schneider, Taehyoung Lee, Jeffrey L. Collett, and Hartmut Herrmann
Atmos. Chem. Phys., 16, 3185–3205, https://doi.org/10.5194/acp-16-3185-2016, https://doi.org/10.5194/acp-16-3185-2016, 2016
Yan Lv, Xiang Li, Ting Ting Xu, Tian Tao Cheng, Xin Yang, Jian Min Chen, Yoshiteru Iinuma, and Hartmut Herrmann
Atmos. Chem. Phys., 16, 2971–2983, https://doi.org/10.5194/acp-16-2971-2016, https://doi.org/10.5194/acp-16-2971-2016, 2016
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The study focused on size-resolved PAHs in urban aerosols at a megacity Shanghai site. The results provide us with a mechanistic understanding of the particle size distribution of PAHs and their transport in the human respiratory system; this can help develop better source control strategies.
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.
Maria Rodigast, Anke Mutzel, Janine Schindelka, and Hartmut Herrmann
Atmos. Chem. Phys., 16, 2689–2702, https://doi.org/10.5194/acp-16-2689-2016, https://doi.org/10.5194/acp-16-2689-2016, 2016
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The study highlights methyl ethyl ketone as a new and unknown source for methylglyoxal in the aqueous phase that is important for aqueous secondary organic aerosol (aqSOA) formation. Besides 2,3-butanedione (29.5 %) and hydroxyacetone (3.0 %), methylglyoxal was formed with a molar yield of 9.5 %. According to the detected products a reaction mechanism was developed and evaluated. The comparison of the model and experimental data showed excellent agreements, in particular for methylglyoxal.
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
E. D. Sofen, D. Bowdalo, M. J. Evans, F. Apadula, P. Bonasoni, M. Cupeiro, R. Ellul, I. E. Galbally, R. Girgzdiene, S. Luppo, M. Mimouni, A. C. Nahas, M. Saliba, and K. Tørseth
Earth Syst. Sci. Data, 8, 41–59, https://doi.org/10.5194/essd-8-41-2016, https://doi.org/10.5194/essd-8-41-2016, 2016
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We have brought together all publicly available surface ozone observations from online databases from 1971–2015, with 2200 sites representing regional background conditions appropriate for the evaluation of chemical transport and chemistry-climate models for projects such as the Chemistry-Climate Model Initiative. Gridded data sets of ozone metrics (mean, percentiles, MDA8, SOMO35, etc.) are available from the British Atmospheric Data Centre.
E. D. Sofen, D. Bowdalo, and M. J. Evans
Atmos. Chem. Phys., 16, 1445–1457, https://doi.org/10.5194/acp-16-1445-2016, https://doi.org/10.5194/acp-16-1445-2016, 2016
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We explore the global representativeness of a global surface ozone data set from a range of perspectives (area, biomes, chemical regimes, model uncertainty, model trends). We conclude that the current network fails to provide sufficient constraints for important regions/regimes, leading to uncertainty for a range of atmospheric composition challenges. We suggest 20 new locations for making surface ozone observations, which would significantly enhance our observational capability.
T. Sherwen, M. J. Evans, L. J. Carpenter, S. J. Andrews, R. T. Lidster, B. Dix, T. K. Koenig, R. Sinreich, I. Ortega, R. Volkamer, A. Saiz-Lopez, C. Prados-Roman, A. S. Mahajan, and C. Ordóñez
Atmos. Chem. Phys., 16, 1161–1186, https://doi.org/10.5194/acp-16-1161-2016, https://doi.org/10.5194/acp-16-1161-2016, 2016
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Using a global chemical transport model (GEOS-Chem) with additional iodine emissions, chemistry, and deposition we show that iodine is responsible for ~ 9 % of global ozone loss but has negligible impacts on global OH. Uncertainties are large in the chemistry and emissions and future research is needed in both. Measurements of iodine species (especially HOI) would be useful. We believe iodine chemistry should be considered in future chemistry-climate and in air quality modelling.
A. J. Rusumdar, R. Wolke, A. Tilgner, and H. Herrmann
Geosci. Model Dev., 9, 247–281, https://doi.org/10.5194/gmd-9-247-2016, https://doi.org/10.5194/gmd-9-247-2016, 2016
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The present paper was aimed at the further development of SPACCIM to treat both complex multiphase chemistry and phase transfer processes considering new non-ideality properties of concentrated solutions. Model studies showed the applicability of the new kinetic model approach for complex aerosol mixtures and detailed chemical mechanisms. Simulations have implied that the treatment of non-ideality should be mandatory for modeling multiphase chemical processes in deliquesced particles.
A. Roth, J. Schneider, T. Klimach, S. Mertes, D. van Pinxteren, H. Herrmann, and S. Borrmann
Atmos. Chem. Phys., 16, 505–524, https://doi.org/10.5194/acp-16-505-2016, https://doi.org/10.5194/acp-16-505-2016, 2016
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This paper reports on single-particle measurements of ambient aerosol particles and cloud residues sampled from orographic clouds on a mountain site in central Germany.
The results show that soot particles can get efficiently activated in cloud droplets when they are mixed with or coated by sulfate and nitrate. Cloud processing leads to addition of nitrate and sulfate to the particles, thereby increasing the hygroscopicity of these particles when they remain in the air after cloud evaporation.
E. D. Sofen, M. J. Evans, and A. C. Lewis
Atmos. Chem. Phys., 15, 13627–13632, https://doi.org/10.5194/acp-15-13627-2015, https://doi.org/10.5194/acp-15-13627-2015, 2015
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As an air pollutant, O3 is monitored photometrically to assess compliance with air quality legislation. A recent study found a 1.8% reduction in its absorption cross section, which would lead to an equivalent increase in observed O3 concentrations. We estimate this would increase the number of sites out of compliance with air quality regulations in the EU and US by 20%. We draw attention to how small changes in gas metrology impacts attainment and compliance with legal air quality standards.
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.
K. W. Fomba, D. van Pinxteren, K. Müller, Y. Iinuma, T. Lee, J. L. Collett Jr., and H. Herrmann
Atmos. Chem. Phys., 15, 8751–8765, https://doi.org/10.5194/acp-15-8751-2015, https://doi.org/10.5194/acp-15-8751-2015, 2015
P. Kupiszewski, E. Weingartner, P. Vochezer, M. Schnaiter, A. Bigi, M. Gysel, B. Rosati, E. Toprak, S. Mertes, and U. Baltensperger
Atmos. Meas. Tech., 8, 3087–3106, https://doi.org/10.5194/amt-8-3087-2015, https://doi.org/10.5194/amt-8-3087-2015, 2015
H. M. Walker, D. Stone, T. Ingham, S. Vaughan, M. Cain, R. L. Jones, O. J. Kennedy, M. McLeod, B. Ouyang, J. Pyle, S. Bauguitte, B. Bandy, G. Forster, M. J. Evans, J. F. Hamilton, J. R. Hopkins, J. D. Lee, A. C. Lewis, R. T. Lidster, S. Punjabi, W. T. Morgan, and D. E. Heard
Atmos. Chem. Phys., 15, 8179–8200, https://doi.org/10.5194/acp-15-8179-2015, https://doi.org/10.5194/acp-15-8179-2015, 2015
M. Rodigast, A. Mutzel, Y. Iinuma, S. Haferkorn, and H. Herrmann
Atmos. Meas. Tech., 8, 2409–2416, https://doi.org/10.5194/amt-8-2409-2015, https://doi.org/10.5194/amt-8-2409-2015, 2015
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An optimised method for derivatisation of carbonyl compounds with o-(2,3,4,5,6-pentafluorobenzyl)hydroxylamine (PFBHA) in aqueous samples is described. The comprehensive optimisation of the method leads to an improvement of the detection limit up to a factor of 10 highlighting the good sensitivity of the optimised method for atmospherically relevant carbonyl compounds. The optimised method was successfully applied to detect carbonyl compounds from the aqueous phase oxidation of 3-methylbutanone.
A. Worringen, K. Kandler, N. Benker, T. Dirsch, S. Mertes, L. Schenk, U. Kästner, F. Frank, B. Nillius, U. Bundke, D. Rose, J. Curtius, P. Kupiszewski, E. Weingartner, P. Vochezer, J. Schneider, S. Schmidt, S. Weinbruch, and M. Ebert
Atmos. Chem. Phys., 15, 4161–4178, https://doi.org/10.5194/acp-15-4161-2015, https://doi.org/10.5194/acp-15-4161-2015, 2015
S. Schmidt, J. Schneider, T. Klimach, S. Mertes, L. P. Schenk, J. Curtius, P. Kupiszewski, E. Hammer, P. Vochezer, G. Lloyd, M. Ebert, K. Kandler, S. Weinbruch, and S. Borrmann
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-4677-2015, https://doi.org/10.5194/acpd-15-4677-2015, 2015
Revised manuscript not accepted
F. A. F. Winiberg, S. C. Smith, I. Bejan, C. A. Brumby, T. Ingham, T. L. Malkin, S. C. Orr, D. E. Heard, and P. W. Seakins
Atmos. Meas. Tech., 8, 523–540, https://doi.org/10.5194/amt-8-523-2015, https://doi.org/10.5194/amt-8-523-2015, 2015
L. P. Schenk, S. Mertes, U. Kästner, F. Frank, B. Nillius, U. Bundke, D. Rose, S. Schmidt, J. Schneider, A. Worringen, K. Kandler, N. Bukowiecki, M. Ebert, J. Curtius, and F. Stratmann
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amtd-7-10585-2014, https://doi.org/10.5194/amtd-7-10585-2014, 2014
Revised manuscript has not been submitted
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A pumped counterflow virtual impactor (PCVI) was set up to separate ice nucleating particle (INP) counter produced ice particles that had been activated to ice from non-activated aerosol particles. The released INP were characterized with regard to their physico-chemical properties. A successful separation (PCVI) of INP for water-subsaturated conditions is proven. First results of INP properties are presented which were gained during a campaign at the high altitude research station Jungfraujoch.
L. Poulain, W. Birmili, F. Canonaco, M. Crippa, Z. J. Wu, S. Nordmann, G. Spindler, A. S. H. Prévôt, A. Wiedensohler, and H. Herrmann
Atmos. Chem. Phys., 14, 10145–10162, https://doi.org/10.5194/acp-14-10145-2014, https://doi.org/10.5194/acp-14-10145-2014, 2014
A. Tilgner, L. Schöne, P. Bräuer, D. van Pinxteren, E. Hoffmann, G. Spindler, S. A. Styler, S. Mertes, W. Birmili, R. Otto, M. Merkel, K. Weinhold, A. Wiedensohler, H. Deneke, R. Schrödner, R. Wolke, J. Schneider, W. Haunold, A. Engel, A. Wéber, and H. Herrmann
Atmos. Chem. Phys., 14, 9105–9128, https://doi.org/10.5194/acp-14-9105-2014, https://doi.org/10.5194/acp-14-9105-2014, 2014
K. W. Fomba, K. Müller, D. van Pinxteren, L. Poulain, M. van Pinxteren, and H. Herrmann
Atmos. Chem. Phys., 14, 8883–8904, https://doi.org/10.5194/acp-14-8883-2014, https://doi.org/10.5194/acp-14-8883-2014, 2014
M. L. Krüger, S. Mertes, T. Klimach, Y. F. Cheng, H. Su, J. Schneider, M. O. Andreae, U. Pöschl, and D. Rose
Atmos. Meas. Tech., 7, 2615–2629, https://doi.org/10.5194/amt-7-2615-2014, https://doi.org/10.5194/amt-7-2615-2014, 2014
S. Henning, K. Dieckmann, K. Ignatius, M. Schäfer, P. Zedler, E. Harris, B. Sinha, D. van Pinxteren, S. Mertes, W. Birmili, M. Merkel, Z. Wu, A. Wiedensohler, H. Wex, H. Herrmann, and F. Stratmann
Atmos. Chem. Phys., 14, 7859–7868, https://doi.org/10.5194/acp-14-7859-2014, https://doi.org/10.5194/acp-14-7859-2014, 2014
P. S. J. Matthews, M. T. Baeza-Romero, L. K. Whalley, and D. E. Heard
Atmos. Chem. Phys., 14, 7397–7408, https://doi.org/10.5194/acp-14-7397-2014, https://doi.org/10.5194/acp-14-7397-2014, 2014
L. Schöne and H. Herrmann
Atmos. Chem. Phys., 14, 4503–4514, https://doi.org/10.5194/acp-14-4503-2014, https://doi.org/10.5194/acp-14-4503-2014, 2014
S. Scheinhardt, D. van Pinxteren, K. Müller, G. Spindler, and H. Herrmann
Atmos. Chem. Phys., 14, 4531–4538, https://doi.org/10.5194/acp-14-4531-2014, https://doi.org/10.5194/acp-14-4531-2014, 2014
E. Harris, B. Sinha, D. van Pinxteren, J. Schneider, L. Poulain, J. Collett, B. D'Anna, B. Fahlbusch, S. Foley, K. W. Fomba, C. George, T. Gnauk, S. Henning, T. Lee, S. Mertes, A. Roth, F. Stratmann, S. Borrmann, P. Hoppe, and H. Herrmann
Atmos. Chem. Phys., 14, 4219–4235, https://doi.org/10.5194/acp-14-4219-2014, https://doi.org/10.5194/acp-14-4219-2014, 2014
D. van Pinxteren, C. Neusüß, and H. Herrmann
Atmos. Chem. Phys., 14, 3913–3928, https://doi.org/10.5194/acp-14-3913-2014, https://doi.org/10.5194/acp-14-3913-2014, 2014
H. J. Liu, C. S. Zhao, B. Nekat, N. Ma, A. Wiedensohler, D. van Pinxteren, G. Spindler, K. Müller, and H. Herrmann
Atmos. Chem. Phys., 14, 2525–2539, https://doi.org/10.5194/acp-14-2525-2014, https://doi.org/10.5194/acp-14-2525-2014, 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. Kahnt, Y. Iinuma, A. Mutzel, O. Böge, M. Claeys, and H. Herrmann
Atmos. Chem. Phys., 14, 719–736, https://doi.org/10.5194/acp-14-719-2014, https://doi.org/10.5194/acp-14-719-2014, 2014
L. K. Whalley, M. A. Blitz, M. Desservettaz, P. W. Seakins, and D. E. Heard
Atmos. Meas. Tech., 6, 3425–3440, https://doi.org/10.5194/amt-6-3425-2013, https://doi.org/10.5194/amt-6-3425-2013, 2013
M. van Pinxteren and H. Herrmann
Atmos. Chem. Phys., 13, 11791–11802, https://doi.org/10.5194/acp-13-11791-2013, https://doi.org/10.5194/acp-13-11791-2013, 2013
P. M. Edwards, M. J. Evans, K. L. Furneaux, J. Hopkins, T. Ingham, C. Jones, J. D. Lee, A. C. Lewis, S. J. Moller, D. Stone, L. K. Whalley, and D. E. Heard
Atmos. Chem. Phys., 13, 9497–9514, https://doi.org/10.5194/acp-13-9497-2013, https://doi.org/10.5194/acp-13-9497-2013, 2013
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
Z. J. Wu, L. Poulain, S. Henning, K. Dieckmann, W. Birmili, M. Merkel, D. van Pinxteren, G. Spindler, K. Müller, F. Stratmann, H. Herrmann, and A. Wiedensohler
Atmos. Chem. Phys., 13, 7983–7996, https://doi.org/10.5194/acp-13-7983-2013, https://doi.org/10.5194/acp-13-7983-2013, 2013
Z. Wu, W. Birmili, L. Poulain, Z. Wang, M. Merkel, B. Fahlbusch, D. van Pinxteren, H. Herrmann, and A. Wiedensohler
Atmos. Chem. Phys., 13, 6637–6646, https://doi.org/10.5194/acp-13-6637-2013, https://doi.org/10.5194/acp-13-6637-2013, 2013
K. W. Fomba, K. Müller, D. van Pinxteren, and H. Herrmann
Atmos. Chem. Phys., 13, 4801–4814, https://doi.org/10.5194/acp-13-4801-2013, https://doi.org/10.5194/acp-13-4801-2013, 2013
J. R. Pierce, M. J. Evans, C. E. Scott, S. D. D'Andrea, D. K. Farmer, E. Swietlicki, and D. V. Spracklen
Atmos. Chem. Phys., 13, 3163–3176, https://doi.org/10.5194/acp-13-3163-2013, https://doi.org/10.5194/acp-13-3163-2013, 2013
C. Mouchel-Vallon, P. Bräuer, M. Camredon, R. Valorso, S. Madronich, H. Herrmann, and B. Aumont
Atmos. Chem. Phys., 13, 1023–1037, https://doi.org/10.5194/acp-13-1023-2013, https://doi.org/10.5194/acp-13-1023-2013, 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: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
In situ ozone production is highly sensitive to volatile organic compounds in Delhi, India
Role of Criegee intermediates in the formation of sulfuric acid at a Mediterranean (Cape Corsica) site under influence of biogenic emissions
Dynamics of gaseous oxidized mercury at Villum Research Station during the High Arctic summer
Isotopic evidence for dominant secondary production of HONO in near-ground wildfire plumes
Opinion: Papers that shaped tropospheric chemistry
Measurement report: Source apportionment of volatile organic compounds at the remote high-altitude Maïdo observatory
Shipborne measurements of methane and carbon dioxide in the Middle East and Mediterranean areas and the contribution from oil and gas emissions
Observations of iodine monoxide over three summers at the Indian Antarctic bases of Bharati and Maitri
Unexplored volatile organic compound emitted from petrochemical facilities: implications for ozone production and atmospheric chemistry
Atmospheric gaseous hydrochloric and hydrobromic acid in urban Beijing, China: detection, source identification and potential atmospheric impacts
Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom
Spectrometric measurements of atmospheric propane (C3H8)
Air–sea exchange of acetone, acetaldehyde, DMS and isoprene at a UK coastal site
Measurement report: Emissions of intermediate-volatility organic compounds from vehicles under real-world driving conditions in an urban tunnel
Investigations on the anthropogenic reversal of the natural ozone gradient between northern and southern midlatitudes
Measurement report: Molecular composition and volatility of gaseous organic compounds in a boreal forest – from volatile organic compounds to highly oxygenated organic molecules
Boreal forest fire CO and CH4 emission factors derived from tower observations in Alaska during the extreme fire season of 2015
Chemical characterization of oxygenated organic compounds in the gas phase and particle phase using iodide CIMS with FIGAERO in urban air
New approach to evaluate satellite-derived XCO2 over oceans by integrating ship and aircraft observations
Central role of nitric oxide in ozone production in the upper tropical troposphere over the Atlantic Ocean and western Africa
Sesquiterpenes and oxygenated sesquiterpenes dominate the VOC (C5–C20) emissions of downy birches
Measurement report: Online measurement of gas-phase nitrated phenols utilizing a CI-LToF-MS: primary sources and secondary formation
Measurement report: In situ observations of deep convection without lightning during the tropical cyclone Florence 2018
Measurement Report: Variability in the composition of biogenic volatile organic compounds in a southeastern US forest and their role in atmospheric reactivity
Reactive nitrogen around the Arabian Peninsula and in the Mediterranean Sea during the 2017 AQABA ship campaign
Stratospheric carbon isotope fractionation and tropospheric histories of CFC-11, CFC-12, and CFC-113 isotopologues
Isotopic compositions of atmospheric total gaseous mercury in 10 Chinese cities and implications for land surface emissions
Formation of condensable organic vapors from anthropogenic and biogenic VOCs is strongly perturbed by NOx in eastern China
Observations of speciated isoprene nitrates in Beijing: implications for isoprene chemistry
Contributions to OH reactivity from unexplored volatile organic compounds measured by PTR-ToF-MS – a case study in a suburban forest of the Seoul metropolitan area during the Korea–United States Air Quality Study (KORUS-AQ) 2016
Total OH reactivity over the Amazon rainforest: variability with temperature, wind, rain, altitude, time of day, season, and an overall budget closure
Where there is smoke there is mercury: Assessing boreal forest fire mercury emissions using aircraft and highlighting uncertainties associated with upscaling emissions estimates
Temporary pause in the growth of atmospheric ethane and propane in 2015–2018
Formation of nighttime sulfuric acid from the ozonolysis of alkenes in Beijing
Spatiotemporal variation, sources, and secondary transformation potential of volatile organic compounds in Xi'an, China
Identifying and quantifying source contributions of air quality contaminants during unconventional shale gas extraction
Observed decreases in on-road CO2 concentrations in Beijing during COVID-19 restrictions
Investigation of several proxies to estimate sulfuric acid concentration under volcanic plume conditions
Measurement report: Exploring NH3 behavior in urban and suburban Beijing: comparison and implications
Spatially and temporally resolved measurements of NOx fluxes by airborne eddy-covariance over Greater London
Atmospheric organic vapors in two European pine forests measured by a Vocus PTR-TOF: insights into monoterpene and sesquiterpene oxidation processes
Speciation of VOC emissions related to offshore North Sea oil and gas production
Origins and characterization of CO and O3 in the African upper troposphere
Halogen activation in the plume of Masaya volcano: field observations and box model investigations
Decoupling of urban CO2 and air pollutant emission reductions during the European SARS-CoV-2 lockdown
Atmospheric VOC measurements at a High Arctic site: characteristics and source apportionment
Evaluating the sensitivity of radical chemistry and ozone formation to ambient VOCs and NOx in Beijing
Global trends and European emissions of tetrafluoromethane (CF4), hexafluoroethane (C2F6) and octafluoropropane (C3F8)
Non-target and suspect characterisation of organic contaminants in ambient air – Part 1: Combining a novel sample clean-up method with comprehensive two-dimensional gas chromatography
Low-NO atmospheric oxidation pathways in a polluted megacity
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.
Alexandre Kukui, Michel Chartier, Jinhe Wang, Hui Chen, Sébastien Dusanter, Stéphane Sauvage, Vincent Michoud, Nadine Locoge, Valérie Gros, Thierry Bourrianne, Karine Sellegri, and Jean-Marc Pichon
Atmos. Chem. Phys., 21, 13333–13351, https://doi.org/10.5194/acp-21-13333-2021, https://doi.org/10.5194/acp-21-13333-2021, 2021
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Sulfuric acid, H2SO4, plays a key role in formation of secondary atmospheric aerosol particles. It is generally accepted that the major atmospheric source of H2SO4 is the reaction of OH radicals with SO2. In this study, importance of an additional H2SO4 source via oxidation of SO2 by stabilized Criegee intermediates was estimated based on measurements at a remote site on Cape Corsica. It was found that the oxidation of SO2 by SCI may be an important source of H2SO4, especially during nighttime.
Jakob Boyd Pernov, Bjarne Jensen, Andreas Massling, Daniel Charles Thomas, and Henrik Skov
Atmos. Chem. Phys., 21, 13287–13309, https://doi.org/10.5194/acp-21-13287-2021, https://doi.org/10.5194/acp-21-13287-2021, 2021
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Atmospheric mercury species (GEM, GOM, PHg) are important constituents in the High Arctic due to their detrimental effects on human and ecosystem health. However, understanding their behavior in the High Arctic summer remains lacking. This research investigates the dynamics of mercury oxidation in the High Arctic summer. The cold, dry, sunlit free troposphere was associated with events of high GOM in the High Arctic summer, while individual events yielded unique origins.
Jiajue Chai, Jack E. Dibb, Bruce E. Anderson, Claire Bekker, Danielle E. Blum, Eric Heim, Carolyn E. Jordan, Emily E. Joyce, Jackson H. Kaspari, Hannah Munro, Wendell W. Walters, and Meredith G. Hastings
Atmos. Chem. Phys., 21, 13077–13098, https://doi.org/10.5194/acp-21-13077-2021, https://doi.org/10.5194/acp-21-13077-2021, 2021
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Nitrous acid (HONO) derived from wildfire emissions plays a key role in controlling atmospheric oxidation chemistry. However, the HONO budget remains poorly constrained. By combining the field-observed concentrations and novel isotopic composition (N and O) of HONO and nitrogen oxides (NOx), we quantitatively constrained the relative contribution of each pathway to secondary HONO production and the relative importance of major atmospheric oxidants (ozone versus peroxy) in aged wildfire smoke.
Paul S. Monks, A. R. Ravishankara, Erika von Schneidemesser, and Roberto Sommariva
Atmos. Chem. Phys., 21, 12909–12948, https://doi.org/10.5194/acp-21-12909-2021, https://doi.org/10.5194/acp-21-12909-2021, 2021
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Which published papers have transformed our understanding of the chemical processes in the troposphere and shaped the field of atmospheric chemistry? We explore how these papers have shaped the development of the field of atmospheric chemistry and identify the major landmarks in the field of atmospheric chemistry through the lens of those papers' impact on science, legislation and environmental events.
Bert Verreyken, Crist Amelynck, Niels Schoon, Jean-François Müller, Jérôme Brioude, Nicolas Kumps, Christian Hermans, Jean-Marc Metzger, Aurélie Colomb, and Trissevgeni Stavrakou
Atmos. Chem. Phys., 21, 12965–12988, https://doi.org/10.5194/acp-21-12965-2021, https://doi.org/10.5194/acp-21-12965-2021, 2021
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We present a 2-year dataset of trace gas concentrations, specifically an array of volatile organic compounds (VOCs), recorded at the Maïdo observatory, a remote tropical high-altitude site located on a small island in the southwest Indian Ocean. We found that island-scale transport is an important driver for the daily cycle of VOC concentrations. During the day, surface emissions from the island affect the atmospheric composition at Maïdo greatly, while at night this impact is strongly reduced.
Jean-Daniel Paris, Aurélie Riandet, Efstratios Bourtsoukidis, Marc Delmotte, Antoine Berchet, Jonathan Williams, Lisa Ernle, Ivan Tadic, Hartwig Harder, and Jos Lelieveld
Atmos. Chem. Phys., 21, 12443–12462, https://doi.org/10.5194/acp-21-12443-2021, https://doi.org/10.5194/acp-21-12443-2021, 2021
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We measured atmospheric methane and CO2 by ship in the Middle East. We probe the origin of methane with a combination of light alkane measurements and modeling. We find strong influence from nearby oil and gas production over the Arabian Gulf. Comparing our data to inventories indicates that inventories overestimate sources from the upstream gas industry but underestimate emissions from oil extraction and processing. The Red Sea was under a complex mixture of sources due to human activity.
Anoop S. Mahajan, Mriganka S. Biswas, Steffen Beirle, Thomas Wagner, Anja Schönhardt, Nuria Benavent, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 21, 11829–11842, https://doi.org/10.5194/acp-21-11829-2021, https://doi.org/10.5194/acp-21-11829-2021, 2021
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Iodine plays a vital role in oxidation chemistry over Antarctica, with past observations showing highly elevated levels of iodine oxide (IO) leading to severe depletion of boundary layer ozone. We present IO observations over three summers (2015–2017) at the Indian Antarctic bases of Bharati and Maitri. IO was observed during all campaigns with mixing ratios below 2 pptv, which is lower than the peak levels observed in West Antarctica, showing the differences in regional chemistry and emissions.
Chinmoy Sarkar, Gracie Wong, Anne Mielnik, Sanjeevi Nagalingam, Nicole Jenna Gross, Alex B. Guenther, Taehyoung Lee, Taehyun Park, Jihee Ban, Seokwon Kang, Jin-Soo Park, Joonyoung Ahn, Danbi Kim, Hyunjae Kim, Jinsoo Choi, Beom-Keun Seo, Jong-Ho Kim, Jeong-Ho Kim, Soo Bog Park, and Saewung Kim
Atmos. Chem. Phys., 21, 11505–11518, https://doi.org/10.5194/acp-21-11505-2021, https://doi.org/10.5194/acp-21-11505-2021, 2021
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We present experimental proofs illustrating the emission of an unexplored volatile organic compound, tentatively assigned as ketene, in an industrial facility in South Korea. The emission of such a compound has rarely been reported, but our experimental data show that the emission rate is substantial. It potentially has tremendous implications for regional air quality and public health, as it is highly reactive and toxic at the same time.
Xiaolong Fan, Jing Cai, Chao Yan, Jian Zhao, Yishuo Guo, Chang Li, Kaspar R. Dällenbach, Feixue Zheng, Zhuohui Lin, Biwu Chu, Yonghong Wang, Lubna Dada, Qiaozhi Zha, Wei Du, Jenni Kontkanen, Theo Kurtén, Siddhart Iyer, Joni T. Kujansuu, Tuukka Petäjä, Douglas R. Worsnop, Veli-Matti Kerminen, Yongchun Liu, Federico Bianchi, Yee Jun Tham, Lei Yao, and Markku Kulmala
Atmos. Chem. Phys., 21, 11437–11452, https://doi.org/10.5194/acp-21-11437-2021, https://doi.org/10.5194/acp-21-11437-2021, 2021
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We observed significant concentrations of gaseous HBr and HCl throughout the winter and springtime in urban Beijing, China. Our results indicate that gaseous HCl and HBr are most likely originated from anthropogenic emissions such as burning activities, and the gas–aerosol partitioning may play a crucial role in contributing to the gaseous HCl and HBr. These observations suggest that there is an important recycling pathway of halogen species in inland megacities.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke D. Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul A. Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 11113–11132, https://doi.org/10.5194/acp-21-11113-2021, https://doi.org/10.5194/acp-21-11113-2021, 2021
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected nearly from pole to pole over the oceans during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigated their impact on the variability of tropospheric N2O.
Geoffrey C. Toon, Jean-Francois L. Blavier, Keeyoon Sung, and Katelyn Yu
Atmos. Chem. Phys., 21, 10727–10743, https://doi.org/10.5194/acp-21-10727-2021, https://doi.org/10.5194/acp-21-10727-2021, 2021
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We report measurements of atmospheric propane (C3H8) from analysis of ground-based infra-red solar absorption spectra measured from various sites by the Jet Propulsion Laboratory (JPL) MkIV interferometer. These measurements suggest that exploitation of natural gas fields is a major and growing source of propane in the USA. Also, there seem to be propane sources in large cities such as Los Angeles, possibly related to use of liquefied petroleum gas (LPG).
Daniel P. Phillips, Frances E. Hopkins, Thomas G. Bell, Peter S. Liss, Philip D. Nightingale, Claire E. Reeves, Charel Wohl, and Mingxi Yang
Atmos. Chem. Phys., 21, 10111–10132, https://doi.org/10.5194/acp-21-10111-2021, https://doi.org/10.5194/acp-21-10111-2021, 2021
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We present the first measurements of the rate of transfer (flux) of three gases between the atmosphere and the ocean, using a direct flux measurement technique, at a coastal site. We show greater atmospheric loss of acetone and acetaldehyde into the ocean than estimated by global models for the open water; importantly, the acetaldehyde transfer direction is opposite to the model estimates. Measured dimethylsulfide fluxes agreed with a recent model. Isoprene fluxes were too weak to be measured.
Hua Fang, Xiaoqing Huang, Yanli Zhang, Chenglei Pei, Zuzhao Huang, Yujun Wang, Yanning Chen, Jianhong Yan, Jianqiang Zeng, Shaoxuan Xiao, Shilu Luo, Sheng Li, Jun Wang, Ming Zhu, Xuewei Fu, Zhenfeng Wu, Runqi Zhang, Wei Song, Guohua Zhang, Weiwei Hu, Mingjin Tang, Xiang Ding, Xinhui Bi, and Xinming Wang
Atmos. Chem. Phys., 21, 10005–10013, https://doi.org/10.5194/acp-21-10005-2021, https://doi.org/10.5194/acp-21-10005-2021, 2021
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A tunnel test was initiated to measure the vehicular IVOC emissions under real-world driving conditions. Higher SOA formation estimated from vehicular IVOCs compared to those from traditional VOCs emphasized the greater importance of IVOCs in modulating urban SOA. The results also revealed that non-road diesel-fueled engines greatly contributed to IVOCs in China.
David D. Parrish, Richard G. Derwent, Steven T. Turnock, Fiona M. O'Connor, Johannes Staehelin, Susanne E. Bauer, Makoto Deushi, Naga Oshima, Kostas Tsigaridis, Tongwen Wu, and Jie Zhang
Atmos. Chem. Phys., 21, 9669–9679, https://doi.org/10.5194/acp-21-9669-2021, https://doi.org/10.5194/acp-21-9669-2021, 2021
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The few ozone measurements made before the 1980s indicate that industrial development increased ozone concentrations by a factor of ~ 2 at northern midlatitudes, which are now larger than at southern midlatitudes. This difference was much smaller, and likely reversed, in the pre-industrial atmosphere. Earth system models find similar increases, but not higher pre-industrial ozone in the south. This disagreement may indicate that modeled natural ozone sources and/or deposition loss are inadequate.
Wei Huang, Haiyan Li, Nina Sarnela, Liine Heikkinen, Yee Jun Tham, Jyri Mikkilä, Steven J. Thomas, Neil M. Donahue, Markku Kulmala, and Federico Bianchi
Atmos. Chem. Phys., 21, 8961–8977, https://doi.org/10.5194/acp-21-8961-2021, https://doi.org/10.5194/acp-21-8961-2021, 2021
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We show full characterization of gaseous organic compounds in a boreal forest. Molecular composition and volatility of gaseous organic compounds with different oxidation extents (from volatile organic compounds to highly oxygenated organic molecules) were investigated and discussed. We provide a more comprehensive understanding of atmospheric organic compounds in this boreal forest and new insights into interpreting ambient measurements or testing and improving parameterizations in models.
Elizabeth B. Wiggins, Arlyn Andrews, Colm Sweeney, John B. Miller, Charles E. Miller, Sander Veraverbeke, Roisin Commane, Steven Wofsy, John M. Henderson, and James T. Randerson
Atmos. Chem. Phys., 21, 8557–8574, https://doi.org/10.5194/acp-21-8557-2021, https://doi.org/10.5194/acp-21-8557-2021, 2021
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We analyzed high-resolution trace gas measurements collected from a tower in Alaska during a very active fire season to improve our understanding of trace gas emissions from boreal forest fires. Our results suggest previous studies may have underestimated emissions from smoldering combustion in boreal forest fires.
Chenshuo Ye, Bin Yuan, Yi Lin, Zelong Wang, Weiwei Hu, Tiange Li, Wei Chen, Caihong Wu, Chaomin Wang, Shan Huang, Jipeng Qi, Baolin Wang, Chen Wang, Wei Song, Xinming Wang, E Zheng, Jordan E. Krechmer, Penglin Ye, Zhanyi Zhang, Xuemei Wang, Douglas R. Worsnop, and Min Shao
Atmos. Chem. Phys., 21, 8455–8478, https://doi.org/10.5194/acp-21-8455-2021, https://doi.org/10.5194/acp-21-8455-2021, 2021
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We performed measurements of gaseous and particulate organic compounds using a state-of-the-art online mass spectrometer in urban air. Using the dataset, we provide a holistic chemical characterization of oxygenated organic compounds in the polluted urban atmosphere, which can serve as a reference for the future field measurements of organic compounds in cities.
Astrid Müller, Hiroshi Tanimoto, Takafumi Sugita, Toshinobu Machida, Shin-ichiro Nakaoka, Prabir K. Patra, Joshua Laughner, and David Crisp
Atmos. Chem. Phys., 21, 8255–8271, https://doi.org/10.5194/acp-21-8255-2021, https://doi.org/10.5194/acp-21-8255-2021, 2021
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Over oceans, high uncertainties in satellite CO2 retrievals exist due to limited reference data. We combine commercial ship and aircraft observations and, with the aid of model calculations, obtain column-averaged mixing ratios of CO2 (XCO2) data over the Pacific Ocean. This new dataset has great potential as a robust reference for XCO2 measured from space and can help to better understand changes in the carbon cycle in response to climate change using satellite observations.
Ivan Tadic, Clara M. Nussbaumer, Birger Bohn, Hartwig Harder, Daniel Marno, Monica Martinez, Florian Obersteiner, Uwe Parchatka, Andrea Pozzer, Roland Rohloff, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 8195–8211, https://doi.org/10.5194/acp-21-8195-2021, https://doi.org/10.5194/acp-21-8195-2021, 2021
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Although mechanisms of tropospheric ozone (O3) formation are well understood, studies reporting on ozone formation derived from field measurements are challenging and remain sparse in number. We use airborne measurements to quantify nitric oxide (NO) and O3 distributions in the upper troposphere over the Atlantic Ocean and western Africa and compare our measurements to model simulations. Our results show that NO and ozone formation are greatest over the tropical areas of western Africa.
Heidi Hellén, Arnaud P. Praplan, Toni Tykkä, Aku Helin, Simon Schallhart, Piia P. Schiestl-Aalto, Jaana Bäck, and Hannele Hakola
Atmos. Chem. Phys., 21, 8045–8066, https://doi.org/10.5194/acp-21-8045-2021, https://doi.org/10.5194/acp-21-8045-2021, 2021
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Even though terpene emissions of boreal needle trees have been studied quite intensively, there is less knowledge of the emissions of broadleaved deciduous trees and emissions of larger terpenes and oxygenated volatile organic compounds. Here we studied downy birch (Betula pubescens) emissions, and especially sesquiterpene and oxygenated sesquiterpene emissions were found to be high. These emissions may have significant effects on secondary organic aerosol formation in boreal areas.
Kai Song, Song Guo, Haichao Wang, Ying Yu, Hui Wang, Rongzhi Tang, Shiyong Xia, Yuanzheng Gong, Zichao Wan, Daqi Lv, Rui Tan, Wenfei Zhu, Ruizhe Shen, Xin Li, Xuena Yu, Shiyi Chen, Liming Zeng, and Xiaofeng Huang
Atmos. Chem. Phys., 21, 7917–7932, https://doi.org/10.5194/acp-21-7917-2021, https://doi.org/10.5194/acp-21-7917-2021, 2021
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Nitrated phenols (NPs) are crucial components of brown carbon. To comprehend the constitutes and sources of NPs in winter of Beijing, their concentrations were measured by a CI-LToF-MS. The secondary formation process was simulated by a box model. NPs were mainly influenced by primary emissions and regional transport. Primary emitted phenol rather than benzene oxidation was crucial in the heavy pollution episode in Beijing. This provides more insight into pollution control strategies of NPs.
Clara M. Nussbaumer, Ivan Tadic, Dirk Dienhart, Nijing Wang, Achim Edtbauer, Lisa Ernle, Jonathan Williams, Florian Obersteiner, Isidoro Gutiérrez-Álvarez, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 7933–7945, https://doi.org/10.5194/acp-21-7933-2021, https://doi.org/10.5194/acp-21-7933-2021, 2021
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Lightning over continental and coastal areas is frequent and accompanied by deep convection, while lightning over marine areas and particularly in tropical cyclones is rare. This research presents in situ observations of the tropical storm Florence 2018 near Cabo Verde. We show the absence of lightning in the tropical storm despite the occurrence of deep convective processes by atmospheric trace gas measurements of O3, NO, CO, H2O2, DMS and CH2I.
Deborah F. McGlynn, Laura E. R. Barry, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-416, https://doi.org/10.5194/acp-2021-416, 2021
Revised manuscript accepted for ACP
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We present one year of hourly measurements of chemically resolved BVOCs between September 15, 2019, and September 15, 2020, collected at a research tower in Central Virginia. Concentrations of a range of BVOCs are described and examined for their impact on atmospheric reactivity. A majority of reactivity comes from α-pinene and limonene, highlighting the importance of both concentration and structure in assessing atmospheric impacts of emissions.
Nils Friedrich, Philipp Eger, Justin Shenolikar, Nicolas Sobanski, Jan Schuladen, Dirk Dienhart, Bettina Hottmann, Ivan Tadic, Horst Fischer, Monica Martinez, Roland Rohloff, Sebastian Tauer, Hartwig Harder, Eva Y. Pfannerstill, Nijing Wang, Jonathan Williams, James Brooks, Frank Drewnick, Hang Su, Guo Li, Yafang Cheng, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 21, 7473–7498, https://doi.org/10.5194/acp-21-7473-2021, https://doi.org/10.5194/acp-21-7473-2021, 2021
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This paper uses NOx and NOz measurements from the 2017 AQABA ship campaign in the Mediterranean Sea and around the Arabian Peninsula to examine the influence e.g. of emissions from shipping and oil and gas production. Night-time losses of NOx dominated in the Arabian Gulf and in the Red Sea, whereas daytime losses were more important in the Mediterranean Sea. Nitric acid and organic nitrates were the most prevalent components of NOz.
Max Thomas, Johannes C. Laube, Jan Kaiser, Samuel Allin, Patricia Martinerie, Robert Mulvaney, Anna Ridley, Thomas Röckmann, William T. Sturges, and Emmanuel Witrant
Atmos. Chem. Phys., 21, 6857–6873, https://doi.org/10.5194/acp-21-6857-2021, https://doi.org/10.5194/acp-21-6857-2021, 2021
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CFC gases are destroying the Earth's life-protecting ozone layer. We improve understanding of CFC destruction by measuring the isotopic fingerprint of the carbon in the three most abundant CFCs. These are the first such measurements in the main region where CFCs are destroyed – the stratosphere. We reconstruct the atmospheric isotope histories of these CFCs back to the 1950s by measuring air extracted from deep snow and using a model. The model and the measurements are generally consistent.
Xuewu Fu, Chen Liu, Hui Zhang, Yue Xu, Hui Zhang, Jun Li, Xiaopu Lyu, Gan Zhang, Hai Guo, Xun Wang, Leiming Zhang, and Xinbin Feng
Atmos. Chem. Phys., 21, 6721–6734, https://doi.org/10.5194/acp-21-6721-2021, https://doi.org/10.5194/acp-21-6721-2021, 2021
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TGM concentrations and isotopic compositions in 10 Chinese cities showed strong seasonality with higher TGM concentrations and Δ199Hg and lower δ202Hg in summer. We found the seasonal variations in TGM concentrations and isotopic compositions were highly related to regional surface Hg(0) emissions, suggesting land surface Hg(0) emissions are an important source of atmospheric TGM that contribute dominantly to the seasonal variations in TGM concentrations and isotopic compositions.
Yuliang Liu, Wei Nie, Yuanyuan Li, Dafeng Ge, Chong Liu, Zhengning Xu, Liangduo Chen, Tianyi Wang, Lei Wang, Peng Sun, Ximeng Qi, Jiaping Wang, Zheng Xu, Jian Yuan, Chao Yan, Yanjun Zhang, Dandan Huang, Zhe Wang, Neil M. Donahue, Douglas Worsnop, Xuguang Chi, Mikael Ehn, and Aijun Ding
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-364, https://doi.org/10.5194/acp-2021-364, 2021
Revised manuscript accepted for ACP
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Oxygenated organic molecules (OOMs) are the crucial intermediates linking volatile organic compounds to secondary organic aerosol. Here, we investigated OOMs measured by nitrate TOF-CIMS in eastern China, though performing positive matrix factorization on binned mass spectra. We reconstructed more than 1000 molecules from 14 derived PMF factors and identified 72 % of the observed OOMs as organic nitrates, highlighting the decisive role of nitrogen chemistry on OOMs formation in populated areas.
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.
Dianne Sanchez, Roger Seco, Dasa Gu, Alex Guenther, John Mak, Youngjae Lee, Danbi Kim, Joonyoung Ahn, Don Blake, Scott Herndon, Daun Jeong, John T. Sullivan, Thomas Mcgee, Rokjin Park, and Saewung Kim
Atmos. Chem. Phys., 21, 6331–6345, https://doi.org/10.5194/acp-21-6331-2021, https://doi.org/10.5194/acp-21-6331-2021, 2021
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We present observations of total reactive gases in a suburban forest observatory in the Seoul metropolitan area. The quantitative comparison with speciated trace gas observations illustrated significant underestimation in atmospheric reactivity from the speciated trace gas observational dataset. We present scientific discussion about potential causes.
Eva Y. Pfannerstill, Nina G. Reijrink, Achim Edtbauer, Akima Ringsdorf, Nora Zannoni, Alessandro Araújo, Florian Ditas, Bruna A. Holanda, Marta O. Sá, Anywhere Tsokankunku, David Walter, Stefan Wolff, Jošt V. Lavrič, Christopher Pöhlker, Matthias Sörgel, and Jonathan Williams
Atmos. Chem. Phys., 21, 6231–6256, https://doi.org/10.5194/acp-21-6231-2021, https://doi.org/10.5194/acp-21-6231-2021, 2021
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Tropical forests are globally significant for atmospheric chemistry. However, the mixture of reactive organic gases emitted by these ecosystems is poorly understood. By comprehensive observations at an Amazon forest site, we show that oxygenated species were previously underestimated in their contribution to the tropical-forest reactant mix. Our results show rain and temperature effects and have implications for models and the understanding of ozone and particle formation above tropical forests.
David S. McLagan, Geoff W. Stupple, Andrea Darlington, Katherine Hayden, and Alexandra Steffen
Atmos. Chem. Phys., 21, 5635–5653, https://doi.org/10.5194/acp-21-5635-2021, https://doi.org/10.5194/acp-21-5635-2021, 2021
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An assessment of mercury emissions from a burning boreal forest was made by flying an aircraft through its plume to collect in situ gas and particulate measurements. Direct data show that in-plume gaseous elemental mercury concentrations reach up to 2.4× background for this fire and up to 5.6× when using a correlation with CO data. These unique data are applied to a series of known empirical emissions estimates and used to highlight current uncertainties in the literature.
Hélène Angot, Connor Davel, Christine Wiedinmyer, Gabrielle Pétron, Jashan Chopra, Jacques Hueber, Brendan Blanchard, Ilann Bourgeois, Isaac Vimont, Stephen A. Montzka, Ben R. Miller, James W. Elkins, and Detlev Helmig
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-285, https://doi.org/10.5194/acp-2021-285, 2021
Revised manuscript accepted for ACP
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After a multi-decade global decline in atmospheric concentrations of ethane and propane (precursors to tropospheric ozone and aerosols), previous work showed a reversal of this trend in 2009–2015 in the Northern Hemisphere due to the growth in oil and natural gas production in North America. Here we show a temporary pause in the growth of atmospheric ethane and propane in 2015–2018 and highlight the critical need for additional top-down studies to further constrain ethane and propane emissions.
Yishuo Guo, Chao Yan, Chang Li, Wei Ma, Zemin Feng, Ying Zhou, Zhuohui Lin, Lubna Dada, Dominik Stolzenburg, Rujing Yin, Jenni Kontkanen, Kaspar R. Daellenbach, Juha Kangasluoma, Lei Yao, Biwu Chu, Yonghong Wang, Runlong Cai, Federico Bianchi, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys., 21, 5499–5511, https://doi.org/10.5194/acp-21-5499-2021, https://doi.org/10.5194/acp-21-5499-2021, 2021
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Fog, cloud and haze are very common natural phenomena. Sulfuric acid (SA) is one of the key compounds forming those suspended particles, technically called aerosols, through gas-to-particle conversion. Therefore, the concentration level, source and sink of SA is very important. Our results show that ozonolysis of alkenes plays a major role in nighttime SA formation under unpolluted conditions in urban Beijing, and nighttime cluster mode particles are probably driven by SA in urban environments.
Mengdi Song, Xin Li, Suding Yang, Xuena Yu, Songxiu Zhou, Yiming Yang, Shiyi Chen, Huabin Dong, Keren Liao, Qi Chen, Keding Lu, Ningning Zhang, Junji Cao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 4939–4958, https://doi.org/10.5194/acp-21-4939-2021, https://doi.org/10.5194/acp-21-4939-2021, 2021
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Due to their lower diffusion capacities and higher conversion capacities, urban areas in Xi’an experienced severe ozone pollution in the summer. In this study, a campaign of comprehensive field observations and VOC grid sampling was conducted in Xi’an from 20 June to 20 July 2019. We found that Xi'an has a strong local emission source of VOCs, and vehicle exhaust was the primary VOC source. In addition, alkenes, aromatics, and oxygenated VOCs played a dominant role in secondary transformations.
Nur H. Orak, Matthew Reeder, and Natalie J. Pekney
Atmos. Chem. Phys., 21, 4729–4739, https://doi.org/10.5194/acp-21-4729-2021, https://doi.org/10.5194/acp-21-4729-2021, 2021
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In this paper, we investigate the effect of unconventional natural gas development activities on local air quality. This is the first study, to our knowledge, to collect high-time-resolution ambient concentrations of compounds emitted from well pad activity on Marcellus Shale during various phases of operation such that the relative air quality effect of each phase of development can be investigated.
Di Liu, Wanqi Sun, Ning Zeng, Pengfei Han, Bo Yao, Zhiqiang Liu, Pucai Wang, Ke Zheng, Han Mei, and Qixiang Cai
Atmos. Chem. Phys., 21, 4599–4614, https://doi.org/10.5194/acp-21-4599-2021, https://doi.org/10.5194/acp-21-4599-2021, 2021
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It is difficult to directly observe the COVID-19 signals in CO2 due to the strong weather induced variations. Here, we determined the on-road CO2 concentration declines in Beijing using mobile observatory data before (BC), during (DC) and after COVID-19 (AC). We chose trips with the most similar weather and calculated the enhancement, the difference between on-road and the city “background”. We showed a clear on-road CO2 decrease in DC, which is consistent with the emissions reductions in DC.
Clémence Rose, Matti P. Rissanen, Siddharth Iyer, Jonathan Duplissy, Chao Yan, John B. Nowak, Aurélie Colomb, Régis Dupuy, Xu-Cheng He, Janne Lampilahti, Yee Jun Tham, Daniela Wimmer, Jean-Marc Metzger, Pierre Tulet, Jérôme Brioude, Céline Planche, Markku Kulmala, and Karine Sellegri
Atmos. Chem. Phys., 21, 4541–4560, https://doi.org/10.5194/acp-21-4541-2021, https://doi.org/10.5194/acp-21-4541-2021, 2021
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Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle formation. However, direct measurements of [H2SO4] remain challenging, motivating the development of proxies. Using data collected in two different volcanic plumes, we show, under these specific conditions, the good performance of a proxy from the literature and also highlight the benefit of the newly developed proxies for the prediction of the highest [H2SO4] values.
Ziru Lan, Weili Lin, Weiwei Pu, and Zhiqiang Ma
Atmos. Chem. Phys., 21, 4561–4573, https://doi.org/10.5194/acp-21-4561-2021, https://doi.org/10.5194/acp-21-4561-2021, 2021
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Haze related to particulate matter has become a big problem in eastern China, and ammonia (NH3) plays an important role in secondary particulate matter formation. In this work, variations in the NH3 mixing ratio showed that the contributions of NH3 sources and sinks in urban and suburban areas were quite different, although the areas were under the influence of similar weather systems. This study furthers the understanding of the behavior of NH3 in a megacity environment.
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. Discuss., https://doi.org/10.5194/acp-2021-180, https://doi.org/10.5194/acp-2021-180, 2021
Revised manuscript accepted for ACP
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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.
Haiyan Li, Manjula R. Canagaratna, Matthieu Riva, Pekka Rantala, Yanjun Zhang, Steven Thomas, Liine Heikkinen, Pierre-Marie Flaud, Eric Villenave, Emilie Perraudin, Douglas Worsnop, Markku Kulmala, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 21, 4123–4147, https://doi.org/10.5194/acp-21-4123-2021, https://doi.org/10.5194/acp-21-4123-2021, 2021
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For the first time, we performed binPMF analysis on the complex mass spectra acquired with the Vocus PTR-TOF in two European pine forests and identified various primary emission sources and secondary oxidation processes of atmospheric organic vapors, i.e., terpenes and their oxidation products, with varying oxidation degrees. Further insights were gained regarding monoterpene and sesquiterpene reactions based on the interpretation results.
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.
Victor Lannuque, Bastien Sauvage, Brice Barret, Hannah Clark, Gilles Athier, Damien Boulanger, Jean-Pierre Cammas, Jean-Marc Cousin, Alain Fontaine, Eric Le Flochmoën, Philippe Nédélec, Hervé Petetin, Isabelle Pfaffenzeller, Susanne Rohs, Herman G. J. Smit, Pawel Wolff, and Valérie Thouret
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-115, https://doi.org/10.5194/acp-2021-115, 2021
Revised manuscript accepted for ACP
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African intertropical troposphere is one of the world areas where the increase in ozone mixing ratio is most marked since 1980 and where high carbon monoxide mixing ratios are found in altitude.
In this article, IAGOS aircraft measurements, IASI satellite instrument observations and SOFT-IO model products are used to explore the seasonal distribution variations and the origin of ozone and carbon monoxide over the African upper troposphere.
Julian Rüdiger, Alexandra Gutmann, Nicole Bobrowski, Marcello Liotta, J. Maarten de Moor, Rolf Sander, Florian Dinger, Jan-Lukas Tirpitz, Martha Ibarra, Armando Saballos, María Martínez, Elvis Mendoza, Arnoldo Ferrufino, John Stix, Juan Valdés, Jonathan M. Castro, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3371–3393, https://doi.org/10.5194/acp-21-3371-2021, https://doi.org/10.5194/acp-21-3371-2021, 2021
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We present an innovative approach to study halogen chemistry in the plume of Masaya volcano in Nicaragua. An unique data set was collected using multiple techniques, including drones. These data enabled us to determine the fraction of activation of the respective halogens at various plume ages, where in-mixing of ambient air causes chemical reactions. An atmospheric chemistry box model was employed to further examine the field results and help our understanding of volcanic plume chemistry.
Christian Lamprecht, Martin Graus, Marcus Striednig, Michael Stichaner, and Thomas Karl
Atmos. Chem. Phys., 21, 3091–3102, https://doi.org/10.5194/acp-21-3091-2021, https://doi.org/10.5194/acp-21-3091-2021, 2021
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The first European SARS-CoV-2 (severe acute respiratory syndrome coronavirus 2) wave and associated lockdown provided a unique sensitivity experiment to study air pollution. We find significantly different emission trajectories between classical air pollution and climate gases (e.g., carbon dioxide). The analysis suggests that European policies, shifting residential, public, and commercial energy demand towards cleaner combustion, have helped to improve air quality more than expected.
Jakob B. Pernov, Rossana Bossi, Thibaut Lebourgeois, Jacob K. Nøjgaard, Rupert Holzinger, Jens L. Hjorth, and Henrik Skov
Atmos. Chem. Phys., 21, 2895–2916, https://doi.org/10.5194/acp-21-2895-2021, https://doi.org/10.5194/acp-21-2895-2021, 2021
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Volatile organic compounds (VOCs) are an important constituent in the Arctic atmosphere due to their effect on aerosol and ozone formation. However, an understanding of their sources is lacking. This research presents a multiseason high-time-resolution dataset of VOCs in the Arctic and details their temporal characteristics and source apportionment. Four sources were identified: biomass burning, marine cryosphere, background, and Arctic haze.
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.
Daniel Say, Alistair J. Manning, Luke M. Western, Dickon Young, Adam Wisher, Matthew Rigby, Stefan Reimann, Martin K. Vollmer, Michela Maione, Jgor Arduini, Paul B. Krummel, Jens Mühle, Christina M. Harth, Brendan Evans, Ray F. Weiss, Ronald G. Prinn, and Simon O'Doherty
Atmos. Chem. Phys., 21, 2149–2164, https://doi.org/10.5194/acp-21-2149-2021, https://doi.org/10.5194/acp-21-2149-2021, 2021
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Perfluorocarbons (PFCs) are potent greenhouse gases with exceedingly long lifetimes. We used atmospheric measurements from a global monitoring network to track the accumulation of these gases in the atmosphere. In the case of the two most abundant PFCs, recent measurements indicate that global emissions are increasing. In Europe, we used a model to estimate regional PFC emissions. Our results show that there was no significant decline in northwest European PFC emissions between 2010 and 2019.
Laura Röhler, Pernilla Bohlin-Nizzetto, Pawel Rostkowski, Roland Kallenborn, and Martin Schlabach
Atmos. Chem. Phys., 21, 1697–1716, https://doi.org/10.5194/acp-21-1697-2021, https://doi.org/10.5194/acp-21-1697-2021, 2021
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A novel non-destructive, sulfuric-acid-free clean-up method for high-volume air samples was developed and evaluated with organic chemicals covering a wide range of polarities (logP 2–11). This method, providing quantitative results of comparable quality to traditional methods, was combined with newly developed data treatment strategies for simultaneous suspect and non-target screening. The application to air samples from southern Norway revealed 90 new potential chemicals of emerging concern.
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.
Cited articles
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Carslaw, N., Jacobs, P. J., and Pilling, M. J.: Modeling OH, HO2, and RO2 radicals in the marine boundary layer 2. Mechanism reduction and uncertainty analysis, J. Geophys. Res.-Atmos., 104, 30257–30273, https://doi.org/10.1029/1999jd900782, 1999.
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Fuchs, H., Bohn, B., Hofzumahaus, A., Holland, F., Lu, K. D., Nehr, S., Rohrer, F., and Wahner, A.: Detection of HO2 by laser-induced fluorescence: calibration and interferences from RO2 radicals, Atmos. Meas. Tech., 4, 1209–1225, https://doi.org/10.5194/amt-4-1209-2011, 2011.
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