Articles | Volume 14, issue 3
Atmos. Chem. Phys., 14, 1299–1321, 2014
https://doi.org/10.5194/acp-14-1299-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Special issue: ROle of Nighttime chemistry in controlling the Oxidising Capacity...
Atmos. Chem. Phys., 14, 1299–1321, 2014
https://doi.org/10.5194/acp-14-1299-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article 05 Feb 2014
Research article | 05 Feb 2014
Radical chemistry at night: comparisons between observed and modelled HOx, NO3 and N2O5 during the RONOCO project
D. Stone et al.
Related authors
Joanna E. Dyson, Graham A. Boustead, Lauren T. Fleming, Mark Blitz, Daniel Stone, Stephen R. Arnold, Lisa K. Whalley, and Dwayne E. Heard
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1216, https://doi.org/10.5194/acp-2020-1216, 2020
Revised manuscript accepted for ACP
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The hydroxyl radical (OH) dominates the removal of atmospheric pollutants, with nitrous acid (HONO) recognised as a major OH source. For remote regions HONO production through the action of sunlight at aerosol surfaces can provide a source of nitrogen oxides. In this study, HONO production rates at illuminated aerosol surfaces are measured under atmospheric conditions, and a model consistent with the data is developed, and aerosol production of HONO in the atmosphere is shown to be significant.
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.
Daniel Stone, Tomás Sherwen, Mathew J. Evans, Stewart Vaughan, Trevor Ingham, Lisa K. Whalley, Peter M. Edwards, Katie A. Read, James D. Lee, Sarah J. Moller, Lucy J. Carpenter, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 3541–3561, https://doi.org/10.5194/acp-18-3541-2018, https://doi.org/10.5194/acp-18-3541-2018, 2018
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Halogen chemistry in the troposphere impacts oxidising capacity, but model studies assessing the nature of these impacts can vary according to the model framework used. In this work we present simulations of OH and HO2 radicals using both box and global model frameworks, and compare to observations made at the Cape Verde Atmospheric Observatory. We highlight, and rationalise, differences between the model frameworks.
Lisa K. Whalley, Daniel Stone, Rachel Dunmore, Jacqueline Hamilton, James R. Hopkins, James D. Lee, Alastair C. Lewis, Paul Williams, Jörg Kleffmann, Sebastian Laufs, Robert Woodward-Massey, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 2547–2571, https://doi.org/10.5194/acp-18-2547-2018, https://doi.org/10.5194/acp-18-2547-2018, 2018
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This paper presents the first radical observations made in London and subsequent model comparisons. This work highlights that there are uncertainties in the degradation mechanism of complex biogenic and diesel-related VOC species under low-NOx conditions and under high-NOx conditions there is a missing source of RO2 radicals. The impact of these model uncertainties on in situ ozone production as a function of NOx is discussed.
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).
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.
J. D. Lee, L. K. Whalley, D. E. Heard, D. Stone, R. E. Dunmore, J. F. Hamilton, D. E. Young, J. D. Allan, S. Laufs, and J. Kleffmann
Atmos. Chem. Phys., 16, 2747–2764, https://doi.org/10.5194/acp-16-2747-2016, https://doi.org/10.5194/acp-16-2747-2016, 2016
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This paper presents field measurements of HONO and a range of other gas phase and particulate species from an urban background site in London. The measured daytime HONO cannot be reproduced with a simple box model and thus a significant daytime missing source of HONO is present. We show that this missing source could be responsible for 40 % of the OH radical source and 57 % of the OH initiation; hence its potential importance for atmospheric oxidation and ozone production.
Lisa K. Whalley, Daniel Stone, Brian Bandy, Rachel Dunmore, Jacqueline F. Hamilton, James Hopkins, James D. Lee, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 2109–2122, https://doi.org/10.5194/acp-16-2109-2016, https://doi.org/10.5194/acp-16-2109-2016, 2016
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
L. K. Whalley, D. Stone, I. J. George, S. Mertes, D. van Pinxteren, A. Tilgner, H. Herrmann, M. J. Evans, and D. E. Heard
Atmos. Chem. Phys., 15, 3289–3301, https://doi.org/10.5194/acp-15-3289-2015, https://doi.org/10.5194/acp-15-3289-2015, 2015
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
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. Discuss., https://doi.org/10.5194/acp-2021-108, https://doi.org/10.5194/acp-2021-108, 2021
Preprint under review for ACP
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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 dimethylsulphide fluxes agreed with a recent model. Isoprene fluxes were too weak to be measured.
Gareth J. Stewart, Beth S. Nelson, W. Joe F. Acton, Adam R. Vaughan, Naomi J. Farren, James R. Hopkins, Martyn W. Ward, Stefan J. Swift, Rahul Arya, Arnab Mondal, Ritu Jangirh, Sakshi Ahlawat, Lokesh Yadav, Sudhir K. Sharma, Siti S. M. Yunus, C. Nicholas Hewitt, Eiko Nemitz, Neil Mullinger, Ranu Gadi, Lokesh K. Sahu, Nidhi Tripathi, Andrew R. Rickard, James D. Lee, Tuhin K. Mandal, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 2407–2426, https://doi.org/10.5194/acp-21-2407-2021, https://doi.org/10.5194/acp-21-2407-2021, 2021
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Biomass burning releases many lower-molecular-weight organic species which are difficult to analyse but important for the formation of organic aerosol. This study examined a new high-resolution technique to better characterise these difficult-to-analyse organic components. Some burning sources analysed in this study, such as cow dung cake and municipal solid waste, released extremely complex mixtures containing many thousands of different lower-volatility organic compounds.
Gareth J. Stewart, W. Joe F. Acton, Beth S. Nelson, Adam R. Vaughan, James R. Hopkins, Rahul Arya, Arnab Mondal, Ritu Jangirh, Sakshi Ahlawat, Lokesh Yadav, Sudhir K. Sharma, Rachel E. Dunmore, Siti S. M. Yunus, C. Nicholas Hewitt, Eiko Nemitz, Neil Mullinger, Ranu Gadi, Lokesh K. Sahu, Nidhi Tripathi, Andrew R. Rickard, James D. Lee, Tuhin K. Mandal, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 2383–2406, https://doi.org/10.5194/acp-21-2383-2021, https://doi.org/10.5194/acp-21-2383-2021, 2021
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Biomass burning is a major source of trace gases to the troposphere; however, the composition and quantity of emissions vary greatly between different fuel types. This work provided near-total quantitation of non-methane volatile organic compounds from combustion of biofuels from India. Emissions from cow dung cake combustion were significantly larger than conventional fuelwood combustion, potentially indicating that this source has a disproportionately large impact on regional air quality.
Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Archit Mehra, Stephen D. Worrall, Asan Bacak, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Tuan Vu, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 2125–2147, https://doi.org/10.5194/acp-21-2125-2021, https://doi.org/10.5194/acp-21-2125-2021, 2021
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To understand how emission controls will impact ozone, an understanding of the sources and sinks of OH and the chemical cycling between peroxy radicals is needed. This paper presents measurements of OH, HO2 and total RO2 taken in central Beijing. The radical observations are compared to a detailed chemistry model, which shows that under low NO conditions, there is a missing OH source. Under high NOx conditions, the model under-predicts RO2 and impacts our ability to model ozone.
Mike J. Newland, Daniel J. Bryant, Rachel E. Dunmore, Thomas J. Bannan, W. Joe F. Acton, Ben Langford, James R. Hopkins, Freya A. Squires, William Dixon, William S. Drysdale, Peter D. Ivatt, Mathew J. Evans, Peter M. Edwards, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, C. Nicholas Hewitt, James D. Lee, Tianqu Cui, Jason D. Surratt, Xinming Wang, Alastair C. Lewis, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 1613–1625, https://doi.org/10.5194/acp-21-1613-2021, https://doi.org/10.5194/acp-21-1613-2021, 2021
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We report the formation of secondary pollutants in the urban megacity of Beijing that are typically associated with remote regions such as rainforests. This is caused by extremely low levels of nitric oxide (NO), typically expected to be high in urban areas, observed in the afternoon. This work has significant implications for how we understand atmospheric chemistry in the urban environment and thus for how to implement effective policies to improve urban air quality.
Huihui Wu, Jonathan W. Taylor, Justin M. Langridge, Chenjie Yu, James D. Allan, Kate Szpek, Michael I. Cotterell, Paul I. Williams, Michael Flynn, Patrick Barker, Cathryn Fox, Grant Allen, James Lee, and Hugh Coe
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-49, https://doi.org/10.5194/acp-2021-49, 2021
Preprint under review for ACP
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Seasonal biomass burning over West Africa is a globally significant source of carbonaceous particles in the atmosphere, which have important climate impacts but are poorly constrained. We conducted in-situ airborne measurements to investigate the evolution of smoke aerosol properties in this region. We observed absorption enhancement for both the black carbon and brown carbon after emission, which provide new field results and constraints on aerosol parameterisations for future climate models.
Bjorn Stevens, Sandrine Bony, David Farrell, Felix Ament, Alan Blyth, Christopher Fairall, Johannes Karstensen, Patricia K. Quinn, Sabrina Speich, Claudia Acquistapace, Franziska Aemisegger, Anna Lea Albright, Hugo Bellenger, Eberhard Bodenschatz, Kathy-Ann Caesar, Rebecca Chewitt-Lucas, Gijs de Boer, Julien Delanoë, Leif Denby, Florian Ewald, Benjamin Fildier, Marvin Forde, Geet George, Silke Gross, Martin Hagen, Andrea Hausold, Karen J. Heywood, Lutz Hirsch, Marek Jacob, Friedhelm Jansen, Stefan Kinne, Daniel Klocke, Tobias Kölling, Heike Konow, Marie Lothon, Wiebke Mohr, Ann Kristin Naumann, Louise Nuijens, Léa Olivier, Robert Pincus, Mira Pöhlker, Gilles Reverdin, Gregory Roberts, Sabrina Schnitt, Hauke Schulz, A. Pier Siebesma, Claudia Christine Stephan, Peter Sullivan, Ludovic Touzé-Peiffer, Jessica Vial, Raphaela Vogel, Paquita Zuidema, Nicola Alexander, Lyndon Alves, Sophian Arixi, Hamish Asmath, Gholamhossein Bagheri, Katharina Baier, Adriana Bailey, Dariusz Baranowski, Alexandre Baron, Sébastien Barrau, Paul A. Barrett, Frédéric Batier, Andreas Behrendt, Arne Bendinger, Florent Beucher, Sebastien Bigorre, Edmund Blades, Peter Blossey, Olivier Bock, Steven Böing, Pierre Bosser, Denis Bourras, Pascale Bouruet-Aubertot, Keith Bower, Pierre Branellec, Hubert Branger, Michal Brennek, Alan Brewer, Pierre-Etienne Brilouet, Björn Brügmann, Stefan A. Buehler, Elmo Burke, Ralph Burton, Radiance Calmer, Jean-Christophe Canonici, Xavier Carton, Gregory Cato Jr., Jude Andre Charles, Patrick Chazette, Yanxu Chen, Michal T. Chilinski, Thomas Choularton, Patrick Chuang, Shamal Clarke, Hugh Coe, Céline Cornet, Pierre Coutris, Fleur Couvreux, Susanne Crewell, Timothy Cronin, Zhiqiang Cui, Yannis Cuypers, Alton Daley, Gillian M. Damerell, Thibaut Dauhut, Hartwig Deneke, Jean-Philippe Desbios, Steffen Dörner, Sebastian Donner, Vincent Douet, Kyla Drushka, Marina Dütsch, André Ehrlich, Kerry Emanuel, Alexandros Emmanouilidis, Jean-Claude Etienne, Sheryl Etienne-Leblanc, Ghislain Faure, Graham Feingold, Luca Ferrero, Andreas Fix, Cyrille Flamant, Piotr Jacek Flatau, Gregory R. Foltz, Linda Forster, Iulian Furtuna, Alan Gadian, Joseph Galewsky, Martin Gallagher, Peter Gallimore, Cassandra Gaston, Chelle Gentemann, Nicolas Geyskens, Andreas Giez, John Gollop, Isabelle Gouirand, Christophe Gourbeyre, Dörte de Graaf, Geiske E. de Groot, Robert Grosz, Johannes Güttler, Manuel Gutleben, Kashawn Hall, George Harris, Kevin C. Helfer, Dean Henze, Calvert Herbert, Bruna Holanda, Antonio Ibanez-Landeta, Janet Intrieri, Suneil Iyer, Fabrice Julien, Heike Kalesse, Jan Kazil, Alexander Kellman, Abiel T. Kidane, Ulrike Kirchner, Marcus Klingebiel, Mareike Körner, Leslie Ann Kremper, Jan Kretzschmar, Ovid Krüger, Wojciech Kumala, Armin Kurz, Pierre L'Hégaret, Matthieu Labaste, Tom Lachlan-Cope, Arlene Laing, Peter Landschützer, Theresa Lang, Diego Lange, Ingo Lange, Clément Laplace, Gauke Lavik, Rémi Laxenaire, Caroline Le Bihan, Mason Leandro, Nathalie Lefevre, Marius Lena, Donald Lenschow, Qiang Li, Gary Lloyd, Sebastian Los, Niccolò Losi, Oscar Lovell, Christopher Luneau, Przemyslaw Makuch, Szymon Malinowski, Gaston Manta, Eleni Marinou, Nicholas Marsden, Sebastien Masson, Nicolas Maury, Bernhard Mayer, Margarette Mayers-Als, Christophe Mazel, Wayne McGeary, James C. McWilliams, Mario Mech, Melina Mehlmann, Agostino Niyonkuru Meroni, Theresa Mieslinger, Andreas Minikin, Peter Minnett, Gregor Möller, Yanmichel Morfa Avalos, Caroline Muller, Ionela Musat, Anna Napoli, Almuth Neuberger, Christophe Noisel, David Noone, Freja Nordsiek, Jakub L. Nowak, Lothar Oswald, Douglas J. Parker, Carolyn Peck, Renaud Person, Miriam Philippi, Albert Plueddemann, Christopher Pöhlker, Veronika Pörtge, Ulrich Pöschl, Lawrence Pologne, Michał Posyniak, Marc Prange, Estefanía Quiñones Meléndez, Jule Radtke, Karim Ramage, Jens Reimann, Lionel Renault, Klaus Reus, Ashford Reyes, Joachim Ribbe, Maximilian Ringel, Markus Ritschel, Cesar B. Rocha, Nicolas Rochetin, Johannes Röttenbacher, Callum Rollo, Haley Royer, Pauline Sadoulet, Leo Saffin, Sanola Sandiford, Irina Sandu, Michael Schäfer, Vera Schemann, Imke Schirmacher, Oliver Schlenczek, Jerome Schmidt, Marcel Schröder, Alfons Schwarzenboeck, Andrea Sealy, Christoph J. Senff, Ilya Serikov, Samkeyat Shohan, Elizabeth Siddle, Alexander Smirnov, Florian Späth, Branden Spooner, M. Katharina Stolla, Wojciech Szkółka, Simon P. de Szoeke, Stéphane Tarot, Eleni Tetoni, Elizabeth Thompson, Jim Thomson, Lorenzo Tomassini, Julien Totems, Alma Anna Ubele, Leonie Villiger, Jan von Arx, Thomas Wagner, Andi Walther, Ben Webber, Manfred Wendisch, Shanice Whitehall, Anton Wiltshire, Allison A. Wing, Martin Wirth, Jonathan Wiskandt, Kevin Wolf, Ludwig Worbes, Ethan Wright, Volker Wulfmeyer, Shanea Young, Chidong Zhang, Dongxiao Zhang, Florian Ziemen, Tobias Zinner, and Martin Zöger
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2021-18, https://doi.org/10.5194/essd-2021-18, 2021
Preprint under review for ESSD
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The EUREC4A field campaign, designed to test hypothesized mechanisms by which clouds respond to warming and benchmark next generation Earth-system models, is presented. EUREC4A comprised roughly five weeks of measurements in the downstream winter trades of the North Atlantic – eastward and south-eastward of Barbados. It was the first campaign that attempted to characterize the full range of processes and scales influencing tradewind clouds.
Jim M. Haywood, Steven J. Abel, Paul A. Barrett, Nicolas Bellouin, Alan Blyth, Keith N. Bower, Melissa Brooks, Ken Carslaw, Haochi Che, Hugh Coe, Michael I. Cotterell, Ian Crawford, Zhiqiang Cui, Nicholas Davies, Beth Dingley, Paul Field, Paola Formenti, Hamish Gordon, Martin de Graaf, Ross Herbert, Ben Johnson, Anthony C. Jones, Justin M. Langridge, Florent Malavelle, Daniel G. Partridge, Fanny Peers, Jens Redemann, Philip Stier, Kate Szpek, Jonathan W. Taylor, Duncan Watson-Parris, Robert Wood, Huihui Wu, and Paquita Zuidema
Atmos. Chem. Phys., 21, 1049–1084, https://doi.org/10.5194/acp-21-1049-2021, https://doi.org/10.5194/acp-21-1049-2021, 2021
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Every year, the seasonal cycle of biomass burning from agricultural practices in Africa creates a huge plume of smoke that travels many thousands of kilometres over the Atlantic Ocean. This study provides an overview of a measurement campaign called the cloud–aerosol–radiation interaction and forcing for year 2017 (CLARIFY-2017) and documents the rationale, deployment strategy, observations, and key results from the campaign which utilized the heavily equipped FAAM atmospheric research aircraft.
Zixia Liu, Martin Osborne, Jim Haywood, Karen Anderson, Jamie D. Shulter, Andy Wilson, Justin Langridge, Steve H. L. Yim, Hugh Coe, Suresh Babu, Sreedharan K. Satheesh, Paquita Zuidema, Tao Huang, and Jack C. H. Cheng
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-495, https://doi.org/10.5194/amt-2020-495, 2021
Preprint under review for AMT
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This paper shows the performance of an advanced aerosol observation instrument (POPS) on a quadcopter drone. The results suggest that the impact of the UAV rotors on the POPS does not unduly affect the performance of the POPS for wind speed less than 2.6 m/s, but when operating under higher wind speed of up to 7.6 m/s, larger discrepancies are noted. Plus, it appears that the POPS measures sub-micron aerosol particles more accurately than super-micron aerosol particles on the drone.
Rutambhara Joshi, Dantong Liu, Eiko Nemitz, Ben Langford, Neil Mullinger, Freya Squires, James Lee, Yunfei Wu, Xiaole Pan, Pingqing Fu, Simone Kotthaus, Sue Grimmond, Qiang Zhang, Ruili Wu, Oliver Wild, Michael Flynn, Hugh Coe, and James Allan
Atmos. Chem. Phys., 21, 147–162, https://doi.org/10.5194/acp-21-147-2021, https://doi.org/10.5194/acp-21-147-2021, 2021
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Black carbon (BC) is a component of particulate matter which has significant effects on climate and human health. Sources of BC include biomass burning, transport, industry and domestic cooking and heating. In this study, we measured BC emissions in Beijing, finding a dominance of traffic emissions over all other sources. The quantitative method presented here has benefits for revising widely used emissions inventories and for understanding BC sources with impacts on air quality and climate.
James L. France, Prudence Bateson, Pamela Dominutti, Grant Allen, Stephen Andrews, Stephane Bauguitte, Max Coleman, Tom Lachlan-Cope, Rebecca E. Fisher, Langwen Huang, Anna E. Jones, James Lee, David Lowry, Joseph Pitt, Ruth Purvis, John Pyle, Jacob Shaw, Nicola Warwick, Alexandra Weiss, Shona Wilde, Jonathan Witherstone, and Stuart Young
Atmos. Meas. Tech., 14, 71–88, https://doi.org/10.5194/amt-14-71-2021, https://doi.org/10.5194/amt-14-71-2021, 2021
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Measuring emission rates of methane from installations is tricky, and it is even more so when those installations are located offshore. Here, we show the aircraft set-up and demonstrate an effective methodology for surveying emissions from UK and Dutch offshore oil and gas installations. We present example data collected from two campaigns to demonstrate the challenges and solutions encountered during these surveys.
Mohanan R. Manoj, Sreedharan K. Satheesh, Krishnaswamy K. Moorthy, Jamie Trembath, and Hugh Coe
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1233, https://doi.org/10.5194/acp-2020-1233, 2020
Preprint under review for ACP
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Vertical distributions of atmospheric aerosols and the ability of aerosols to form clouds has been studied across the Indo-Gangetic Plain based on air-borne measurements carried out during the SWAAMI field campaign studying the Indian monsoon. The ability of the aerosols to act as cloud forming nuclei showed contrasting features, increasing with increase in altitude, prior to the onset of monsoon, reversing the trend to decrease with increase in altitude during the active phase of the monsoon.
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.
Yiqun Han, Wu Chen, Lia Chatzidiakou, Anika Krause, Li Yan, Hanbin Zhang, Queenie Chan, Ben Barratt, Rod Jones, Jing Liu, Yangfeng Wu, Meiping Zhao, Junfeng Zhang, Frank J. Kelly, Tong Zhu, and the AIRLESS team
Atmos. Chem. Phys., 20, 15775–15792, https://doi.org/10.5194/acp-20-15775-2020, https://doi.org/10.5194/acp-20-15775-2020, 2020
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Panel studies might be the most suitable way to link intensive air monitoring campaigns for a wide range of pollutant species and personal exposure in different micro-environments, together with epidemiological studies of detailed biological changes in humans. Panel studies are intensive, but related papers are very limited. With the successful collection of a rich dataset, we believe AIRLESS sets a good example for the design of a multidisciplinary study.
David C. Loades, Mingxi Yang, Thomas G. Bell, Adam R. Vaughan, Ryan J. Pound, Stefan Metzger, James D. Lee, and Lucy J. Carpenter
Atmos. Meas. Tech., 13, 6915–6931, https://doi.org/10.5194/amt-13-6915-2020, https://doi.org/10.5194/amt-13-6915-2020, 2020
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The loss of ozone to the sea surface was measured from the south coast of the UK and was found to be more rapid than previous observations over the open ocean. This is likely a consequence of different chemistry and biology in coastal environments. Strong winds appeared to speed up the loss of ozone. A better understanding of what influences ozone loss over the sea will lead to better model estimates of total ozone in the troposphere.
James D. Lee, Will S. Drysdale, Doug P. Finch, Shona E. Wilde, and Paul I. Palmer
Atmos. Chem. Phys., 20, 15743–15759, https://doi.org/10.5194/acp-20-15743-2020, https://doi.org/10.5194/acp-20-15743-2020, 2020
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Efforts to prevent the COVID-19 virus spreading across the globe have included travel restrictions and the closure of workplaces, leading to a significant drop in emissions of primary air pollutants. This provides for a unique opportunity to examine how air pollutant concentrations respond to an abrupt and prolonged reduction. We examine how NO2 and O3 have been affected at several urban measurement sites in the UK. We look at the change in NO2 compared to previous years and the effect on O3.
Patrick A. Barker, Grant Allen, Martin Gallagher, Joseph R. Pitt, Rebecca E. Fisher, Thomas Bannan, Euan G. Nisbet, Stéphane J.-B. Bauguitte, Dominika Pasternak, Samuel Cliff, Marina B. Schimpf, Archit Mehra, Keith N. Bower, James D. Lee, Hugh Coe, and Carl J. Percival
Atmos. Chem. Phys., 20, 15443–15459, https://doi.org/10.5194/acp-20-15443-2020, https://doi.org/10.5194/acp-20-15443-2020, 2020
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Africa is estimated to account for approximately 52 % of global biomass burning (BB) carbon emissions. Despite this, there has been little previous in situ study of African BB emissions. This work presents BB emission factors for various atmospheric trace gases sampled from an aircraft in two distinct areas of Africa (Senegal and Uganda). Intracontinental variability in biomass burning methane emission is identified, which is attributed to difference in the specific fuel mixtures burnt.
Simone T. Andersen, Lucy J. Carpenter, Beth S. Nelson, Luis Neves, Katie A. Read, Chris Reed, Martyn Ward, Matthew J. Rowlinson, and James D. Lee
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-469, https://doi.org/10.5194/amt-2020-469, 2020
Revised manuscript accepted for AMT
W. Joe F. Acton, Zhonghui Huang, Brian Davison, Will S. Drysdale, Pingqing Fu, Michael Hollaway, Ben Langford, James Lee, Yanhui Liu, Stefan Metzger, Neil Mullinger, Eiko Nemitz, Claire E. Reeves, Freya A. Squires, Adam R. Vaughan, Xinming Wang, Zhaoyi Wang, Oliver Wild, Qiang Zhang, Yanli Zhang, and C. Nicholas Hewitt
Atmos. Chem. Phys., 20, 15101–15125, https://doi.org/10.5194/acp-20-15101-2020, https://doi.org/10.5194/acp-20-15101-2020, 2020
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Air quality in Beijing is of concern to both policy makers and the general public. In order to address concerns about air quality it is vital that the sources of atmospheric pollutants are understood. This work presents the first top-down measurement of volatile organic compound (VOC) emissions in Beijing. These measurements are used to evaluate the emissions inventory and assess the impact of VOC emission from the city centre on atmospheric chemistry.
Eloise J. Slater, Lisa K. Whalley, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Leigh R. Crilley, Louisa Kramer, William Bloss, Tuan Vu, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 20, 14847–14871, https://doi.org/10.5194/acp-20-14847-2020, https://doi.org/10.5194/acp-20-14847-2020, 2020
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The paper details atmospheric chemistry in a megacity (Beijing), focussing on radicals which mediate the formation of secondary pollutants such as ozone and particles. Highly polluted conditions were experienced, including the highest ever levels of nitric oxide (NO), with simultaneous radical measurements. Radical concentrations were large during "haze" events, demonstrating active photochemistry. Modelling showed that our understanding of the chemistry at high NOx levels is incomplete.
Joanna E. Dyson, Graham A. Boustead, Lauren T. Fleming, Mark Blitz, Daniel Stone, Stephen R. Arnold, Lisa K. Whalley, and Dwayne E. Heard
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1216, https://doi.org/10.5194/acp-2020-1216, 2020
Revised manuscript accepted for ACP
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The hydroxyl radical (OH) dominates the removal of atmospheric pollutants, with nitrous acid (HONO) recognised as a major OH source. For remote regions HONO production through the action of sunlight at aerosol surfaces can provide a source of nitrogen oxides. In this study, HONO production rates at illuminated aerosol surfaces are measured under atmospheric conditions, and a model consistent with the data is developed, and aerosol production of HONO in the atmosphere is shown to be significant.
Douglas Morrison, Ian Crawford, Nicholas Marsden, Michael Flynn, Katie Read, Luis Neves, Virginia Foot, Paul Kaye, Warren Stanley, Hugh Coe, David Topping, and Martin Gallagher
Atmos. Chem. Phys., 20, 14473–14490, https://doi.org/10.5194/acp-20-14473-2020, https://doi.org/10.5194/acp-20-14473-2020, 2020
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We provide conservative estimates of the concentrations of bacteria within transatlantic dust clouds, originating from the African continent. We observe significant seasonal differences in the overall concentrations of particles but no seasonal variation in the ratio between bacteria and dust. With bacteria contributing to ice formation at warmer temperatures than dust, our observations should improve the accuracy of climate models.
Jingsha Xu, Shaojie Song, Roy M. Harrison, Congbo Song, Lianfang Wei, Qiang Zhang, Yele Sun, Lu Lei, Chao Zhang, Xiaohong Yao, Dihui Chen, Weijun Li, Miaomiao Wu, Hezhong Tian, Lining Luo, Shengrui Tong, Weiran Li, Junling Wang, Guoliang Shi, Yanqi Huangfu, Yingze Tian, Baozhu Ge, Shaoli Su, Chao Peng, Yang Chen, Fumo Yang, Aleksandra Mihajlidi-Zelić, Dragana Đorđević, Stefan J. Swift, Imogen Andrews, Jacqueline F. Hamilton, Ye Sun, Agung Kramawijaya, Jinxiu Han, Supattarachai Saksakulkrai, Clarissa Baldo, Siqi Hou, Feixue Zheng, Kaspar R. Daellenbach, Chao Yan, Yongchun Liu, Markku Kulmala, Pingqing Fu, and Zongbo Shi
Atmos. Meas. Tech., 13, 6325–6341, https://doi.org/10.5194/amt-13-6325-2020, https://doi.org/10.5194/amt-13-6325-2020, 2020
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An interlaboratory comparison was conducted for the first time to examine differences in water-soluble inorganic ions (WSIIs) measured by 10 labs using ion chromatography (IC) and by two online aerosol chemical speciation monitor (ACSM) methods. Major ions including SO42−, NO3− and NH4+ agreed well in 10 IC labs and correlated well with ACSM data. WSII interlab variability strongly affected aerosol acidity results based on ion balance, but aerosol pH computed by ISORROPIA II was very similar.
Atallah Elzein, Gareth J. Stewart, Stefan J. Swift, Beth S. Nelson, Leigh R. Crilley, Mohammed S. Alam, Ernesto Reyes-Villegas, Ranu Gadi, Roy M. Harrison, Jacqueline F. Hamilton, and Alastair C. Lewis
Atmos. Chem. Phys., 20, 14303–14319, https://doi.org/10.5194/acp-20-14303-2020, https://doi.org/10.5194/acp-20-14303-2020, 2020
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We collected high-frequency air particle samples (PM2.5) in Beijing (China) and Delhi (India) and measured the concentration of PAHs in daytime and night-time. PAHs were higher in Delhi than in Beijing, and the five-ring PAHs contribute the most to the total PAH concentration. We compared the emission sources and identified the major sectors that could be subject to mitigation measures. The adverse health effects from inhalation exposure to PAHs in Delhi are 2.2 times higher than in Beijing.
Stuart K. Grange, James D. Lee, Will S. Drysdale, Alastair C. Lewis, Christoph Hueglin, Lukas Emmenegger, and David C. Carslaw
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1171, https://doi.org/10.5194/acp-2020-1171, 2020
Revised manuscript accepted for ACP
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The changes in mobility across Europe due to the COVID-19 lockdowns had consequences for air quality. We compare what was experienced, to estimates of
what would have beenwithout the lockdowns. Nitrogen dioxide (NO2), an important vehicle-sourced pollutant, decreased by a third. However, ozone (O3) increased in response to the lower NO2. Because NO2 is decreasing over time, increases in O3 can be expected in European urban areas and will require management to avoid future negative outcomes.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-914, https://doi.org/10.5194/acp-2020-914, 2020
Preprint under review for ACP
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions are predictable and explained by key emissions. These results are used to estimate the premature mortality associated to SOA in urban regions.
Mohammed S. Alam, Leigh R. Crilley, James D. Lee, Louisa J. Kramer, Christian Pfrang, Mónica Vázquez-Moreno, Milagros Ródenas, Amalia Muñoz, and William J. Bloss
Atmos. Meas. Tech., 13, 5977–5991, https://doi.org/10.5194/amt-13-5977-2020, https://doi.org/10.5194/amt-13-5977-2020, 2020
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We report on the interference arising in measurements of nitrogen oxides (NOx) from the presence of a range of alkenes in sampled air when using the most widespread air quality monitoring technique for chemiluminescence detection. Interferences of up to 11 % are reported, depending upon the alkene present and conditions used. Such interferences may be of substantial importance for the interpretation of ambient NOx data, particularly for high volatile organic compound and low NOx environments.
Huihui Wu, Jonathan W. Taylor, Kate Szpek, Justin M. Langridge, Paul I. Williams, Michael Flynn, James D. Allan, Steven J. Abel, Joseph Pitt, Michael I. Cotterell, Cathryn Fox, Nicholas W. Davies, Jim Haywood, and Hugh Coe
Atmos. Chem. Phys., 20, 12697–12719, https://doi.org/10.5194/acp-20-12697-2020, https://doi.org/10.5194/acp-20-12697-2020, 2020
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Airborne measurements of highly aged biomass burning aerosols (BBAs) over the remote southeast Atlantic provide unique aerosol parameters for climate models. Our observations demonstrate the persistence of strongly absorbing BBAs across wide regions of the South Atlantic. We also found significant vertical variation in the single-scattering albedo of these BBAs, as a function of relative chemical composition and size. Aerosol properties in the marine BL are suggested to be separated from the FT.
Jessica Slater, Juha Tonttila, Gordon McFiggans, Paul Connolly, Sami Romakkaniemi, Thomas Kühn, and Hugh Coe
Atmos. Chem. Phys., 20, 11893–11906, https://doi.org/10.5194/acp-20-11893-2020, https://doi.org/10.5194/acp-20-11893-2020, 2020
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The feedback effect between aerosol particles, radiation and meteorology reduces turbulent motion and results in increased surface aerosol concentrations during Beijing haze. Observational analysis and regional modelling studies have examined the feedback effect but these studies are limited. In this work, we set up a high-resolution model for the Beijing environment to examine the sensitivity of the aerosol feedback effect to initial meteorological conditions and aerosol loading.
Shona E. Wilde, Pamela A. Dominutti, Stephen J. Andrews, Stephane J.-B. Bauguitte, Ralph R. Burton, Ioana Colfescu, James France, James R. Hopkins, 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. Discuss., https://doi.org/10.5194/acp-2020-1099, https://doi.org/10.5194/acp-2020-1099, 2020
Revised manuscript accepted for ACP
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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 characterised.
Zainab Bibi, Hugh Coe, James Brooks, Paul I. Williams, Ernesto Reyes-Villegas, Michael Priestley, Carl Percival, and James D. Allan
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-890, https://doi.org/10.5194/acp-2020-890, 2020
Revised manuscript under review for ACP
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We are presenting a new method to apportion Black Carbon/soot into multiple sources through the inclusion of fullerene and metal data into SP-AMS factorisation. While this is itself would be considered a technical development, we can present a budget of contributions to measured BC during the event studied, including the conclusion that fireworks contributed little compared to the bonfire, traffic and domestic wood burning emissions.
Sobhan Kumar Kompalli, Surendran Nair Suresh Babu, Krishnaswamy Krishnamoorthy, Sreedharan Krishnakumari Satheesh, Mukunda M. Gogoi, Vijayakumar S. Nair, Jayachandran V, Dantong Liu, Michael Flynn, and Hugh Coe
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-836, https://doi.org/10.5194/acp-2020-836, 2020
Revised manuscript under review for ACP
Jonathan W. Taylor, Huihui Wu, Kate Szpek, Keith Bower, Ian Crawford, Michael J. Flynn, Paul I. Williams, James Dorsey, Justin M. Langridge, Michael I. Cotterell, Cathryn Fox, Nicholas W. Davies, Jim M. Haywood, and Hugh Coe
Atmos. Chem. Phys., 20, 11201–11221, https://doi.org/10.5194/acp-20-11201-2020, https://doi.org/10.5194/acp-20-11201-2020, 2020
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Every year, huge plumes of smoke hundreds of miles wide travel over the south Atlantic Ocean from fires in central and southern Africa. These plumes absorb the sun’s energy and warm the climate. We used airborne optical instrumentation to determine how absorbing the smoke was as well as the relative importance of black and brown carbon. We also tested different ways of simulating these properties that could be used in a climate model.
Archit Mehra, Jordan E. Krechmer, Andrew Lambe, Chinmoy Sarkar, Leah Williams, Farzaneh Khalaj, Alex Guenther, John Jayne, Hugh Coe, Douglas Worsnop, Celia Faiola, and Manjula Canagaratna
Atmos. Chem. Phys., 20, 10953–10965, https://doi.org/10.5194/acp-20-10953-2020, https://doi.org/10.5194/acp-20-10953-2020, 2020
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Emissions of volatile organic compounds (VOCs) from plants are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Real plant emissions are much more diverse than the few proxies widely used for studies of plant SOA. Here we present the first study of SOA from Californian sage plants and the oxygenated monoterpenes representing their major emissions. We identify SOA products and show the importance of the formation of highly oxygenated organic molecules and oligomers.
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. Discuss., https://doi.org/10.5194/acp-2020-685, https://doi.org/10.5194/acp-2020-685, 2020
Revised manuscript accepted for ACP
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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 compounding 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.
Ernesto Reyes-Villegas, Upasana Panda, Eoghan Darbyshire, James M. Cash, Rutambhara Joshi, Ben Langford, Chiara F. Di Marco, Neil Mullinger, W. Joe F. Acton, Will Drysdale, Eiko Nemitz, Michael Flynn, Aristeidis Voliotis, Gordon McFiggans, Hugh Coe, James Lee, C. Nicholas Hewitt, Mathew R. Heal, Sachin S. Gunthe, Shivani, Ranu Gadi, Siddhartha Singh, Vijay Soni, and James D. Allan
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-894, https://doi.org/10.5194/acp-2020-894, 2020
Revised manuscript has not been submitted
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The work presented in this manuscript shows the first multisite online measurements of PM1 in Delhi, India. It covers measurements over different seasons in Old and New Delhi during 2018. OA source apportionment was performed using PMF. Traffic showed to be the main primary aerosol source for both OA and BC, as seen with the PMF analysis and aethalometer model analysis. This indicates that in Delhi control of primary traffic exhaust emissions would make a significant reduction to air pollution.
David Topping, David Watts, Hugh Coe, James Evans, Thomas J. Bannan, Douglas Lowe, Caroline Jay, and Jonathan W. Taylor
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-270, https://doi.org/10.5194/gmd-2020-270, 2020
Preprint under review for GMD
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Time-series forecasting methods have often been used to mitigate some of the challenges associated with deploying chemical transport models. In this study we deploy and evaluate Facebook’s Prophetmodel v0.6 in predicting hourly concentrations of Nitrogen Dioxide [NO2]. et. Overall we find the Prophet model offers a relatively effective and simple way to make predictions about NO2 at local levels.
Archit Mehra, Yuwei Wang, Jordan E. Krechmer, Andrew Lambe, Francesca Majluf, Melissa A. Morris, Michael Priestley, Thomas J. Bannan, Daniel J. Bryant, Kelly L. Pereira, Jacqueline F. Hamilton, Andrew R. Rickard, Mike J. Newland, Harald Stark, Philip Croteau, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, Lin Wang, and Hugh Coe
Atmos. Chem. Phys., 20, 9783–9803, https://doi.org/10.5194/acp-20-9783-2020, https://doi.org/10.5194/acp-20-9783-2020, 2020
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Aromatic volatile organic compounds (VOCs) emitted from anthropogenic activity are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Here we present a detailed chemical characterisation of SOA from four C9-aromatic isomers and a polycyclic aromatic hydrocarbon (PAH). We identify and compare their oxidation products in the gas and particle phases, showing the different relative importance of oxidation pathways and proportions of highly oxygenated organic molecules.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Åsa Halquist, Mikael Ehn, Astrid Kiendler-Scharr, Thomas F. Mentel, Gordon McFiggans, Mattias Halquist, Hugh Coe, and Carl J. Percival
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-819, https://doi.org/10.5194/acp-2020-819, 2020
Revised manuscript accepted for ACP
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A significant fraction of emissions from human activity consists of aromatic hydrocarbons e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks e.g. MCM. Cluster analysis of the oxidation product time series' distinguishes behaviours of CHON compounds that can aid identifying functionality.
Yuwei Wang, Archit Mehra, Jordan E. Krechmer, Gan Yang, Xiaoyu Hu, Yiqun Lu, Andrew Lambe, Manjula Canagaratna, Jianmin Chen, Douglas Worsnop, Hugh Coe, and Lin Wang
Atmos. Chem. Phys., 20, 9563–9579, https://doi.org/10.5194/acp-20-9563-2020, https://doi.org/10.5194/acp-20-9563-2020, 2020
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A series of OH-initiated oxidation experiments of trimethylbenzene were investigated in the absence and presence of NOx. Many C9 products with 1–11 oxygen atoms and C18 products presumably formed from dimerization of C9 peroxy radicals were observed, hinting at the extensive existence of autoxidation and accretion reaction pathways. The presence of NOx would suppress the formation of highly oxygenated C18 molecules and enhance the formation of organonitrates and even dinitrate compounds.
Jill S. Johnson, Leighton A. Regayre, Masaru Yoshioka, Kirsty J. Pringle, Steven T. Turnock, Jo Browse, David M. H. Sexton, John W. Rostron, Nick A. J. Schutgens, Daniel G. Partridge, Dantong Liu, James D. Allan, Hugh Coe, Aijun Ding, David D. Cohen, Armand Atanacio, Ville Vakkari, Eija Asmi, and Ken S. Carslaw
Atmos. Chem. Phys., 20, 9491–9524, https://doi.org/10.5194/acp-20-9491-2020, https://doi.org/10.5194/acp-20-9491-2020, 2020
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We use over 9000 monthly aggregated grid-box measurements of aerosol to constrain the uncertainty in the HadGEM3-UKCA climate model. Measurements of AOD, PM2.5, particle number concentrations, sulfate and organic mass concentrations are compared to 1 million
variantsof the model using an implausibility metric. Despite many compensating effects in the model, the procedure constrains the probability distributions of many parameters, and direct radiative forcing uncertainty is reduced by 34 %.
Freya A. Squires, Eiko Nemitz, Ben Langford, Oliver Wild, Will S. Drysdale, W. Joe F. Acton, Pingqing Fu, C. Sue B. Grimmond, Jacqueline F. Hamilton, C. Nicholas Hewitt, Michael Hollaway, Simone Kotthaus, James Lee, Stefan Metzger, Natchaya Pingintha-Durden, Marvin Shaw, Adam R. Vaughan, Xinming Wang, Ruili Wu, Qiang Zhang, and Yanli Zhang
Atmos. Chem. Phys., 20, 8737–8761, https://doi.org/10.5194/acp-20-8737-2020, https://doi.org/10.5194/acp-20-8737-2020, 2020
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Significant air quality problems exist in megacities like Beijing, China. To manage air pollution, legislators need a clear understanding of pollutant emissions. However, emissions inventories have large uncertainties, and reliable field measurements of pollutant emissions are required to constrain them. This work presents the first measurements of traffic-dominated emissions in Beijing which suggest that inventories overestimate these emissions in the region during both winter and summer.
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.
Kirsti Ashworth, Silvia Bucci, Peter J. Gallimore, Junghwa Lee, Beth S. Nelson, Alberto Sanchez-Marroquín, Marina B. Schimpf, Paul D. Smith, Will S. Drysdale, Jim R. Hopkins, James D. Lee, Joe R. Pitt, Piero Di Carlo, Radovan Krejci, and James B. McQuaid
Atmos. Chem. Phys., 20, 7193–7216, https://doi.org/10.5194/acp-20-7193-2020, https://doi.org/10.5194/acp-20-7193-2020, 2020
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In July 2017 we flew three research flights around London during European Facility for Airborne Research (EUFAR) training. We made continuous measurements of concentrations of key pollutants (ozone, NOx, aerosol particles, CO, CO2 and methane) and meteorology, and we collected periodic samples of air to analyse for volatile organic compounds. We saw evidence that plumes of pollution from the city, strong local emissions and pollution from distant sources all contribute to regional pollution.
Manuela van Pinxteren, Khanneh Wadinga Fomba, Nadja Triesch, Christian Stolle, Oliver Wurl, Enno Bahlmann, Xianda Gong, Jens Voigtländer, Heike Wex, Tiera-Brandy Robinson, Stefan Barthel, Sebastian Zeppenfeld, Erik Hans Hoffmann, Marie Roveretto, Chunlin Li, Benoit Grosselin, Veronique Daële, Fabian Senf, Dominik van Pinxteren, Malena Manzi, Nicolás Zabalegui, Sanja Frka, Blaženka Gašparović, Ryan Pereira, Tao Li, Liang Wen, Jiarong Li, Chao Zhu, Hui Chen, Jianmin Chen, Björn Fiedler, Wolf von Tümpling, Katie Alana Read, Shalini Punjabi, Alastair Charles Lewis, James Roland Hopkins, Lucy Jane Carpenter, Ilka Peeken, Tim Rixen, Detlef Schulz-Bull, María Eugenia Monge, Abdelwahid Mellouki, Christian George, Frank Stratmann, and Hartmut Herrmann
Atmos. Chem. Phys., 20, 6921–6951, https://doi.org/10.5194/acp-20-6921-2020, https://doi.org/10.5194/acp-20-6921-2020, 2020
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An introduction to a comprehensive field campaign performed at the Cape Verde Atmospheric Observatory regarding ocean–atmosphere interactions is given. Chemical, physical, biological and meteorological techniques were applied, and measurements of bulk water, the sea surface microlayer, cloud water and ambient aerosol particles took place. Oceanic compounds were found to be transferred to atmospheric aerosol and to the cloud level; however, sea spray contributions to CCN and INPs were limited.
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.
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
William T. Morgan, James D. Allan, Stéphane Bauguitte, Eoghan Darbyshire, Michael J. Flynn, James Lee, Dantong Liu, Ben Johnson, Jim Haywood, Karla M. Longo, Paulo E. Artaxo, and Hugh Coe
Atmos. Chem. Phys., 20, 5309–5326, https://doi.org/10.5194/acp-20-5309-2020, https://doi.org/10.5194/acp-20-5309-2020, 2020
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We flew a large atmospheric research aircraft across a number of different environments in the Amazon basin during the 2012 biomass burning season. Smoke from fires builds up and has a significant impact on weather, climate, health and natural ecosystems. Our goal was to quantify changes in the properties of the smoke emitted by fires as it is transported through the atmosphere. We found that the major control on the properties of the smoke was due to differences in the fires themselves.
Elise S. Droste, Karina E. Adcock, Matthew J. Ashfold, Charles Chou, Zoë Fleming, Paul J. Fraser, Lauren J. Gooch, Andrew J. Hind, Ray L. Langenfelds, Emma Leedham Elvidge, Norfazrin Mohd Hanif, Simon O'Doherty, David E. Oram, Chang-Feng Ou-Yang, Marios Panagi, Claire E. Reeves, William T. Sturges, and Johannes C. Laube
Atmos. Chem. Phys., 20, 4787–4807, https://doi.org/10.5194/acp-20-4787-2020, https://doi.org/10.5194/acp-20-4787-2020, 2020
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We update the tropospheric trends and emissions of six perfluorocarbon (PFC) gases, including separate isomers. Trends for these strong greenhouse gases are still increasing, but at slower rates than previously. The lack of natural sinks results in the global accumulation of 833 million metric tonnes of CO2 equivalent for these six PFCs by 2017. Modelling results indicate potential source regions and types in East Asia, but we find that many emissions are unaccounted for in emission reports.
Siddika Celik, Frank Drewnick, Friederike Fachinger, James Brooks, Eoghan Darbyshire, Hugh Coe, Jean-Daniel Paris, Philipp G. Eger, Jan Schuladen, Ivan Tadic, Nils Friedrich, Dirk Dienhart, Bettina Hottmann, Horst Fischer, John N. Crowley, Hartwig Harder, and Stephan Borrmann
Atmos. Chem. Phys., 20, 4713–4734, https://doi.org/10.5194/acp-20-4713-2020, https://doi.org/10.5194/acp-20-4713-2020, 2020
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Analysis of 252 ship emission plumes in the Mediterranean Sea and around the Arabian Peninsula examined particulate- and gas-phase characteristics. By identifying the corresponding ships, source features and plume age were determined. Emission factors (amount of pollutant per kilogram of fuel burned) were calculated and investigated for dependencies on source characteristics, atmospheric conditions, and transport time, providing insight into the most relevant influences on ship emissions.
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.
Sobhan Kumar Kompalli, Surendran Nair Suresh Babu, Sreedharan Krishnakumari Satheesh, Krishnaswamy Krishna Moorthy, Trupti Das, Ramasamy Boopathy, Dantong Liu, Eoghan Darbyshire, James D. Allan, James Brooks, Michael J. Flynn, and Hugh Coe
Atmos. Chem. Phys., 20, 3965–3985, https://doi.org/10.5194/acp-20-3965-2020, https://doi.org/10.5194/acp-20-3965-2020, 2020
Mohanan R. Manoj, Sreedharan K. Satheesh, Krishnaswamy K. Moorthy, and Hugh Coe
Atmos. Chem. Phys., 20, 4031–4046, https://doi.org/10.5194/acp-20-4031-2020, https://doi.org/10.5194/acp-20-4031-2020, 2020
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The study reports the observation of highly absorbing aerosol layers at high altitudes (1–2.5 km) prior to monsoon and during its development over the Indian region and quantifies its climate impacts. The absorption of solar radiation in these layers perturbs the onset of monsoon through the impact on the atmospheric stability. When height-resolved values of single scattering albedo (SSA) are used in a radiative transfer model, a maximum heating ~1 K d (~twice that using SSA) is obtained.
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.
Chenjie Yu, Dantong Liu, Kurtis Broda, Rutambhara Joshi, Jason Olfert, Yele Sun, Pingqing Fu, Hugh Coe, and James D. Allan
Atmos. Chem. Phys., 20, 3645–3661, https://doi.org/10.5194/acp-20-3645-2020, https://doi.org/10.5194/acp-20-3645-2020, 2020
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This study presents the first atmospheric application of a new morphology-independent measurement for the quantification of the mixing state of rBC-containing particles in urban Beijing as part of the UK–China APHH campaign. An inversion method has been applied for better quantification of rBC mixing state. The mass-resolved rBC mixing state information presented here has implications for detailed models of BC, its optical properties and its atmospheric life cycle.
Michael Biggart, Jenny Stocker, Ruth M. Doherty, Oliver Wild, Michael Hollaway, David Carruthers, Jie Li, Qiang Zhang, Ruili Wu, Simone Kotthaus, Sue Grimmond, Freya A. Squires, James Lee, and Zongbo Shi
Atmos. Chem. Phys., 20, 2755–2780, https://doi.org/10.5194/acp-20-2755-2020, https://doi.org/10.5194/acp-20-2755-2020, 2020
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Ambient air pollution is a major cause of premature death in China. We examine the street-scale variation of pollutant levels in Beijing using air pollution dispersion and chemistry model ADMS-Urban. Campaign measurements are compared with simulated pollutant levels, providing a valuable means of evaluating the impact of key processes on urban air quality. Air quality modelling at such fine scales is essential for human exposure studies and for informing choices on future emission controls.
Sidhant J. Pai, Colette L. Heald, Jeffrey R. Pierce, Salvatore C. Farina, Eloise A. Marais, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Ann M. Middlebrook, Hugh Coe, John E. Shilling, Roya Bahreini, Justin H. Dingle, and Kennedy Vu
Atmos. Chem. Phys., 20, 2637–2665, https://doi.org/10.5194/acp-20-2637-2020, https://doi.org/10.5194/acp-20-2637-2020, 2020
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Aerosols in the atmosphere have significant health and climate impacts. Organic aerosol (OA) accounts for a large fraction of the total aerosol burden, but models have historically struggled to accurately simulate it. This study compares two very different OA model schemes and evaluates them against a suite of globally distributed airborne measurements with the goal of providing insight into the strengths and weaknesses of each approach across different environments.
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.
Conor G. Bolas, Valerio Ferracci, Andrew D. Robinson, Mohammed I. Mead, Mohd Shahrul Mohd Nadzir, John A. Pyle, Roderic L. Jones, and Neil R. P. Harris
Atmos. Meas. Tech., 13, 821–838, https://doi.org/10.5194/amt-13-821-2020, https://doi.org/10.5194/amt-13-821-2020, 2020
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Here we present the iDirac, a new instrument capable of making isoprene measurements in remote and challenging environments. The iDirac is a customisable and rugged field instrument for investigating emissions of volatile organic compounds from vegetation. It has been tested here in a series of experiments to ensure a high degree of technical precision, accuracy and repeatability. This new instrument allows us to ask and answer new questions about the influence of vegetation on the atmosphere.
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. Discuss., https://doi.org/10.5194/acp-2019-964, https://doi.org/10.5194/acp-2019-964, 2020
Revised manuscript under review for ACP
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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.
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.
James Brean, Roy M. Harrison, Zongbo Shi, David C. S. Beddows, W. Joe F. Acton, C. Nicholas Hewitt, Freya A. Squires, and James Lee
Atmos. Chem. Phys., 19, 14933–14947, https://doi.org/10.5194/acp-19-14933-2019, https://doi.org/10.5194/acp-19-14933-2019, 2019
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Measurements of highly oxidized molecules measured during a summer campaign in Beijing are presented. These molecules represent an intermediary between gas-phase chemicals from which they are formed and airborne particles which form from them. Conclusions are drawn as to the factors affecting the formation of new particles within the Beijing atmosphere.
Leigh R. Crilley, Louisa J. Kramer, Bin Ouyang, Jun Duan, Wenqian Zhang, Shengrui Tong, Maofa Ge, Ke Tang, Min Qin, Pinhua Xie, Marvin D. Shaw, Alastair C. Lewis, Archit Mehra, Thomas J. Bannan, Stephen D. Worrall, Michael Priestley, Asan Bacak, Hugh Coe, James Allan, Carl J. Percival, Olalekan A. M. Popoola, Roderic L. Jones, and William J. Bloss
Atmos. Meas. Tech., 12, 6449–6463, https://doi.org/10.5194/amt-12-6449-2019, https://doi.org/10.5194/amt-12-6449-2019, 2019
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Nitrous acid (HONO) is key species for understanding tropospheric chemistry, yet accurate and precise measurements are challenging. Here we report an inter–comparison exercise of a number of instruments that measured HONO in a highly polluted location (Beijing). All instruments agreed on the temporal trends yet displayed divergence in absolute concentrations. The cause of this divergence was unclear, but it may in part be due to spatial variability in instrument location.
James Brooks, Dantong Liu, James D. Allan, Paul I. Williams, Jim Haywood, Ellie J. Highwood, Sobhan K. Kompalli, S. Suresh Babu, Sreedharan K. Satheesh, Andrew G. Turner, and Hugh Coe
Atmos. Chem. Phys., 19, 13079–13096, https://doi.org/10.5194/acp-19-13079-2019, https://doi.org/10.5194/acp-19-13079-2019, 2019
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Our study presents an analysis of the vertical and horizontal black carbon properties across northern India using aircraft measurements. The Indo-Gangetic Plain saw the greatest black carbon mass concentrations during the pre-monsoon season. Two black carbon modes were recorded: a small black carbon mode (traffic emissions) in the north-west and a moderately coated mode (solid-fuel emissions) in the Indo-Gangetic Plain. In the vertical profile, absorption properties increase with height.
Duncan Watson-Parris, Nick Schutgens, Carly Reddington, Kirsty J. Pringle, Dantong Liu, James D. Allan, Hugh Coe, Ken S. Carslaw, and Philip Stier
Atmos. Chem. Phys., 19, 11765–11790, https://doi.org/10.5194/acp-19-11765-2019, https://doi.org/10.5194/acp-19-11765-2019, 2019
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The vertical distribution of aerosol in the atmosphere affects its ability to act as cloud condensation nuclei and changes the amount of sunlight it absorbs or reflects. Common global measurements of aerosol provide no information about this vertical distribution. Using a global collection of in situ aircraft measurements to compare with an aerosol–climate model (ECHAM-HAM), we explore the key processes controlling this distribution and find that wet removal plays a key role.
Lia Chatzidiakou, Anika Krause, Olalekan A. M. Popoola, Andrea Di Antonio, Mike Kellaway, Yiqun Han, Freya A. Squires, Teng Wang, Hanbin Zhang, Qi Wang, Yunfei Fan, Shiyi Chen, Min Hu, Jennifer K. Quint, Benjamin Barratt, Frank J. Kelly, Tong Zhu, and Roderic L. Jones
Atmos. Meas. Tech., 12, 4643–4657, https://doi.org/10.5194/amt-12-4643-2019, https://doi.org/10.5194/amt-12-4643-2019, 2019
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This study validates the performance of a personal air quality monitor that integrates miniaturised sensors that measure physical and chemical parameters. Overall, the air pollution sensors showed excellent agreement with standard instrumentation in outdoor, indoor and commuting environments across seasons and different geographical settings. Hence, novel sensing technologies like the ones demonstrated here can revolutionise health studies by providing highly resolved reliable exposure metrics.
Kelly L. Pereira, Grazia Rovelli, Young C. Song, Alfred W. Mayhew, Jonathan P. Reid, and Jacqueline F. Hamilton
Atmos. Meas. Tech., 12, 4519–4541, https://doi.org/10.5194/amt-12-4519-2019, https://doi.org/10.5194/amt-12-4519-2019, 2019
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We present the design and operation of a newly built continuous-flow reactor (CFR), which can be used as a tool to gain considerable insights into the composition and physical state of secondary organic aerosol (SOA). The CFR was used to generate large quantities of SOA mass, allowing the use of highly accurate techniques that are not usually accessible. We demonstrate how this unique approach can be used to investigate the relationship between SOA formation and physiochemical properties.
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.
Carly L. Reddington, William T. Morgan, Eoghan Darbyshire, Joel Brito, Hugh Coe, Paulo Artaxo, Catherine E. Scott, John Marsham, and Dominick V. Spracklen
Atmos. Chem. Phys., 19, 9125–9152, https://doi.org/10.5194/acp-19-9125-2019, https://doi.org/10.5194/acp-19-9125-2019, 2019
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We use an aerosol model and observations to explore model representation of aerosol emissions from fires in the Amazon. We find that observed aerosol concentrations are captured by the model over deforestation fires in the western Amazon but underestimated over savanna fires in the Cerrado environment. The model underestimates observed aerosol optical depth (AOD) even when the observed aerosol vertical profile is reproduced. We suggest this may be due to uncertainties in the AOD calculation.
Joseph R. Pitt, Grant Allen, Stéphane J.-B. Bauguitte, Martin W. Gallagher, James D. Lee, Will Drysdale, Beth Nelson, Alistair J. Manning, and Paul I. Palmer
Atmos. Chem. Phys., 19, 8931–8945, https://doi.org/10.5194/acp-19-8931-2019, https://doi.org/10.5194/acp-19-8931-2019, 2019
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This paper presents a new method to assess inventory estimates of greenhouse gas and air pollutant emissions for large cities and their surrounding regions. A case study using data sampled by a research aircraft around London was used to test the method. We found that the UK national inventory agrees with our observations for CO but needed lower emissions for CH4 to agree with the measured data. Repeated studies could help determine how these emissions vary on different timescales.
Atallah Elzein, Rachel E. Dunmore, Martyn W. Ward, Jacqueline F. Hamilton, and Alastair C. Lewis
Atmos. Chem. Phys., 19, 8741–8758, https://doi.org/10.5194/acp-19-8741-2019, https://doi.org/10.5194/acp-19-8741-2019, 2019
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This article investigates the chemical composition of fine particulate matter (PM2.5) in Beijing, China, in winter 2016. It includes the identification and quantification of 35 polycyclic aromatic compounds. The results include their distribution between daytime and night-time. They were correlated with the gas-phase concentrations of atmospheric oxidants. Major emission sources were identified, and the cancer risk associated with particle inhalation in Beijing was estimated.
Jonathan W. Taylor, Sophie L. Haslett, Keith Bower, Michael Flynn, Ian Crawford, James Dorsey, Tom Choularton, Paul J. Connolly, Valerian Hahn, Christiane Voigt, Daniel Sauer, Régis Dupuy, Joel Brito, Alfons Schwarzenboeck, Thierry Bourriane, Cyrielle Denjean, Phil Rosenberg, Cyrille Flamant, James D. Lee, Adam R. Vaughan, Peter G. Hill, Barbara Brooks, Valéry Catoire, Peter Knippertz, and Hugh Coe
Atmos. Chem. Phys., 19, 8503–8522, https://doi.org/10.5194/acp-19-8503-2019, https://doi.org/10.5194/acp-19-8503-2019, 2019
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Low-level clouds cover a wide area of southern West Africa (SWA) and play an important role in the region's climate, reflecting sunlight away from the surface. We performed aircraft measurements of aerosols and clouds over SWA during the 2016 summer monsoon and found pollution, and polluted clouds, across the whole region. Smoke from biomass burning in Central Africa is transported to West Africa, causing a polluted background which limits the effect of local pollution on cloud properties.
Jamie M. Kelly, Ruth M. Doherty, Fiona M. O'Connor, Graham W. Mann, Hugh Coe, and Dantong Liu
Geosci. Model Dev., 12, 2539–2569, https://doi.org/10.5194/gmd-12-2539-2019, https://doi.org/10.5194/gmd-12-2539-2019, 2019
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This study develops the representation of secondary organic aerosol (SOA) within a global chemistry–climate model (UKCA). Both dry and wet deposition within the UKCA model are extended to consider precursors of SOA. The oxidation mechanism describing SOA formation is also extended by adding a reaction intermediate, with SOA yields that are dependent on oxidant concentrations.
Zongbo Shi, Tuan Vu, Simone Kotthaus, Roy M. Harrison, Sue Grimmond, Siyao Yue, Tong Zhu, James Lee, Yiqun Han, Matthias Demuzere, Rachel E. Dunmore, Lujie Ren, Di Liu, Yuanlin Wang, Oliver Wild, James Allan, W. Joe Acton, Janet Barlow, Benjamin Barratt, David Beddows, William J. Bloss, Giulia Calzolai, David Carruthers, David C. Carslaw, Queenie Chan, Lia Chatzidiakou, Yang Chen, Leigh Crilley, Hugh Coe, Tie Dai, Ruth Doherty, Fengkui Duan, Pingqing Fu, Baozhu Ge, Maofa Ge, Daobo Guan, Jacqueline F. Hamilton, Kebin He, Mathew Heal, Dwayne Heard, C. Nicholas Hewitt, Michael Hollaway, Min Hu, Dongsheng Ji, Xujiang Jiang, Rod Jones, Markus Kalberer, Frank J. Kelly, Louisa Kramer, Ben Langford, Chun Lin, Alastair C. Lewis, Jie Li, Weijun Li, Huan Liu, Junfeng Liu, Miranda Loh, Keding Lu, Franco Lucarelli, Graham Mann, Gordon McFiggans, Mark R. Miller, Graham Mills, Paul Monk, Eiko Nemitz, Fionna O'Connor, Bin Ouyang, Paul I. Palmer, Carl Percival, Olalekan Popoola, Claire Reeves, Andrew R. Rickard, Longyi Shao, Guangyu Shi, Dominick Spracklen, David Stevenson, Yele Sun, Zhiwei Sun, Shu Tao, Shengrui Tong, Qingqing Wang, Wenhua Wang, Xinming Wang, Xuejun Wang, Zifang Wang, Lianfang Wei, Lisa Whalley, Xuefang Wu, Zhijun Wu, Pinhua Xie, Fumo Yang, Qiang Zhang, Yanli Zhang, Yuanhang Zhang, and Mei Zheng
Atmos. Chem. Phys., 19, 7519–7546, https://doi.org/10.5194/acp-19-7519-2019, https://doi.org/10.5194/acp-19-7519-2019, 2019
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APHH-Beijing is a collaborative international research programme to study the sources, processes and health effects of air pollution in Beijing. This introduction to the special issue provides an overview of (i) the APHH-Beijing programme, (ii) the measurement and modelling activities performed as part of it and (iii) the air quality and meteorological conditions during joint intensive field campaigns as a core activity within APHH-Beijing.
Dantong Liu, Rutambhara Joshi, Junfeng Wang, Chenjie Yu, James D. Allan, Hugh Coe, Michael J. Flynn, Conghui Xie, James Lee, Freya Squires, Simone Kotthaus, Sue Grimmond, Xinlei Ge, Yele Sun, and Pingqing Fu
Atmos. Chem. Phys., 19, 6749–6769, https://doi.org/10.5194/acp-19-6749-2019, https://doi.org/10.5194/acp-19-6749-2019, 2019
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This study provides source attribution and characterization of BC in the Beijing urban environment in both winter and summer. For the first time, the physically and chemically based source apportionments are compared to evaluate the primary source contribution and secondary processing of BC-containing particles. A method is proposed to isolate the BC from the transportation sector and coal combustion sources.
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.
Eoghan Darbyshire, William T. Morgan, James D. Allan, Dantong Liu, Michael J. Flynn, James R. Dorsey, Sebastian J. O'Shea, Douglas Lowe, Kate Szpek, Franco Marenco, Ben T. Johnson, Stephane Bauguitte, Jim M. Haywood, Joel F. Brito, Paulo Artaxo, Karla M. Longo, and Hugh Coe
Atmos. Chem. Phys., 19, 5771–5790, https://doi.org/10.5194/acp-19-5771-2019, https://doi.org/10.5194/acp-19-5771-2019, 2019
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A novel analysis of aerosol and gas-phase vertical profiles shows a marked regional pollution contrast: composition is driven by the fire regime and vertical distribution is driven by thermodynamics. These drivers ought to be well represented in simulations to ensure realistic prediction of climate and air quality impacts. The BC : CO ratio in haze and plumes increases with altitude – long-range transport or fire stage coupled to plume dynamics may be responsible. Further enquiry is advocated.
James Brooks, James D. Allan, Paul I. Williams, Dantong Liu, Cathryn Fox, Jim Haywood, Justin M. Langridge, Ellie J. Highwood, Sobhan K. Kompalli, Debbie O'Sullivan, Suresh S. Babu, Sreedharan K. Satheesh, Andrew G. Turner, and Hugh Coe
Atmos. Chem. Phys., 19, 5615–5634, https://doi.org/10.5194/acp-19-5615-2019, https://doi.org/10.5194/acp-19-5615-2019, 2019
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Our study, for the first time, presents measurements of aerosol chemical composition and physical characteristics across northern India in the pre-monsoon and monsoon seasons of 2016 using the FAAM BAe-146 UK research aircraft. Across northern India, an elevated aerosol layer dominated by sulfate aerosol exists that diminishes with monsoon arrival. The Indo-Gangetic Plain (IGP) boundary layer is dominated by organics, whereas outside the IGP sulfate dominates with increased scattering aerosol.
Christoph A. Keller and Mat J. Evans
Geosci. Model Dev., 12, 1209–1225, https://doi.org/10.5194/gmd-12-1209-2019, https://doi.org/10.5194/gmd-12-1209-2019, 2019
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Computer simulations of atmospheric chemistry are a central tool to study the impact of air pollutants on the environment. These models are highly complex and require a lot of computing resources. In this study we show that machine learning can be used to predict air pollution with an accuracy that is comparable to the traditional, computationally expensive method. Such a machine-learning-based model has the potential to be orders of magnitude faster.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Alba Badia, Claire E. Reeves, Alex R. Baker, Alfonso Saiz-Lopez, Rainer Volkamer, Theodore K. Koenig, Eric C. Apel, Rebecca S. Hornbrook, Lucy J. Carpenter, Stephen J. Andrews, Tomás Sherwen, and Roland von Glasow
Atmos. Chem. Phys., 19, 3161–3189, https://doi.org/10.5194/acp-19-3161-2019, https://doi.org/10.5194/acp-19-3161-2019, 2019
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The oceans have an impact on the composition and reactivity of the troposphere through the emission of gases and particles. Thus, a quantitative understanding of the marine atmosphere is crucial to examine the oxidative capacity and climate forcing. This study investigates the impact of halogens in the tropical troposphere and explores the sensitivity of this to uncertainties in the fluxes and their chemical processing. Our modelled tropospheric Ox loss due to halogens ranges from 20 % to 60 %.
Thomas J. Bannan, Michael Le Breton, Michael Priestley, Stephen D. Worrall, Asan Bacak, Nicholas A. Marsden, Archit Mehra, Julia Hammes, Mattias Hallquist, M. Rami Alfarra, Ulrich K. Krieger, Jonathan P. Reid, John Jayne, Wade Robinson, Gordon McFiggans, Hugh Coe, Carl J. Percival, and Dave Topping
Atmos. Meas. Tech., 12, 1429–1439, https://doi.org/10.5194/amt-12-1429-2019, https://doi.org/10.5194/amt-12-1429-2019, 2019
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The Filter Inlet for Gases and AEROsols (FIGAERO) is an inlet designed to be coupled with a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) and provides simultaneous molecular information relating to both the gas- and particle-phase samples. This method has been used to extract vapour pressures of compounds whilst giving quantitative concentrations in the particle phase. Here we detail an ideal set of benchmark compounds for characterization of the FIGAERO.
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.
Nicholas A. Marsden, Romy Ullrich, Ottmar Möhler, Stine Eriksen Hammer, Konrad Kandler, Zhiqiang Cui, Paul I. Williams, Michael J. Flynn, Dantong Liu, James D. Allan, and Hugh Coe
Atmos. Chem. Phys., 19, 2259–2281, https://doi.org/10.5194/acp-19-2259-2019, https://doi.org/10.5194/acp-19-2259-2019, 2019
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The composition of airborne dust influences climate and ecosystems but its measurements presents a huge analytical challenge. Using online single-particle mass spectrometry, we demonstrate differences in mineralogy and mixing state can be detected in real time in both laboratory studies and ambient measurements. The results provide insights into the temporal and spatial evolution of dust properties that will be useful for aerosol–cloud interaction studies and dust cycle modelling.
Naomi J. Farren, Rachel E. Dunmore, Mohammed Iqbal Mead, Mohd Shahrul Mohd Nadzir, Azizan Abu Samah, Siew-Moi Phang, Brian J. Bandy, William T. Sturges, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 19, 1537–1553, https://doi.org/10.5194/acp-19-1537-2019, https://doi.org/10.5194/acp-19-1537-2019, 2019
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During the winter monsoon, air quality on the east coast of Peninsular Malaysia is influenced by local emissions and aged emissions transported from highly polluted East Asian regions. Atmospheric particulate matter has been sampled at a rural coastal location, and ion chromatography has been used to make time-resolved measurements of the major atmospheric ions present. Analysis of aerosol composition and back trajectories has provided an insight into common sources and formation pathways.
Sophie L. Haslett, Jonathan W. Taylor, Konrad Deetz, Bernhard Vogel, Karmen Babić, Norbert Kalthoff, Andreas Wieser, Cheikh Dione, Fabienne Lohou, Joel Brito, Régis Dupuy, Alfons Schwarzenboeck, Paul Zieger, and Hugh Coe
Atmos. Chem. Phys., 19, 1505–1520, https://doi.org/10.5194/acp-19-1505-2019, https://doi.org/10.5194/acp-19-1505-2019, 2019
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As the population in West Africa grows and air pollution increases, it is becoming ever more important to understand the effects of this pollution on the climate and on health. Aerosol particles can grow by absorbing water from the air around them. This paper shows that during the monsoon season, aerosol particles in the region are likely to grow significantly because of the high moisture in the air. This means that climate effects from increasing pollution will be enhanced.
Junfeng Wang, Dantong Liu, Xinlei Ge, Yangzhou Wu, Fuzhen Shen, Mindong Chen, Jian Zhao, Conghui Xie, Qingqing Wang, Weiqi Xu, Jie Zhang, Jianlin Hu, James Allan, Rutambhara Joshi, Pingqing Fu, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 19, 447–458, https://doi.org/10.5194/acp-19-447-2019, https://doi.org/10.5194/acp-19-447-2019, 2019
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This work is part of the UK-China APHH campaign. We used a laser-only Aerodyne soot particle aerosol mass spectrometer, for the first time, to investigate the concentrations, size distributions and chemical compositions for those ambient submicron aerosol particles only with black carbon as cores. Our findings are valuable to understand the BC properties and processes in the densely populated megacities.
Conghui Xie, Weiqi Xu, Junfeng Wang, Qingqing Wang, Dantong Liu, Guiqian Tang, Ping Chen, Wei Du, Jian Zhao, Yingjie Zhang, Wei Zhou, Tingting Han, Qingyun Bian, Jie Li, Pingqing Fu, Zifa Wang, Xinlei Ge, James Allan, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 19, 165–179, https://doi.org/10.5194/acp-19-165-2019, https://doi.org/10.5194/acp-19-165-2019, 2019
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We present the first simultaneous real-time online measurements of aerosol optical properties at ground level and at 260 m on a meteorological tower in urban Beijing in winter. The vertical similarities and differences in scattering and absorption coefficients were characterized. The increases in MAC of BC were mainly associated with the coating materials on rBC. Coal combustion was the dominant source contribution of brown carbon followed by biomass burning and SOA in winter in Beijing.
Claire L. Ryder, Franco Marenco, Jennifer K. Brooke, Victor Estelles, Richard Cotton, Paola Formenti, James B. McQuaid, Hannah C. Price, Dantong Liu, Patrick Ausset, Phil D. Rosenberg, Jonathan W. Taylor, Tom Choularton, Keith Bower, Hugh Coe, Martin Gallagher, Jonathan Crosier, Gary Lloyd, Eleanor J. Highwood, and Benjamin J. Murray
Atmos. Chem. Phys., 18, 17225–17257, https://doi.org/10.5194/acp-18-17225-2018, https://doi.org/10.5194/acp-18-17225-2018, 2018
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Every year, millions of tons of Saharan dust particles are carried across the Atlantic by the wind, where they can affect weather patterns and climate. Their sizes span orders of magnitude, but the largest (over 10 microns – around the width of a human hair) are difficult to measure and few observations exist. Here we show new aircraft observations of large dust particles, finding more than we would expect, and we quantify their properties which allow them to interact with atmospheric radiation.
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.
Christopher Dearden, Adrian Hill, Hugh Coe, and Tom Choularton
Atmos. Chem. Phys., 18, 14253–14269, https://doi.org/10.5194/acp-18-14253-2018, https://doi.org/10.5194/acp-18-14253-2018, 2018
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We perform computer simulations of the life cycle of low-lying clouds over southern West Africa during the monsoon season. Such clouds tend not to produce much precipitation, but they do affect the regional climate by modifying the amount of sunlight reaching the surface. The aim of this work is to understand the factors that influence the growth and break-up of these clouds. We show that the number of water droplets contained within the clouds affects how quickly they dissipate.
Konrad Deetz, Heike Vogel, Sophie Haslett, Peter Knippertz, Hugh Coe, and Bernhard Vogel
Atmos. Chem. Phys., 18, 14271–14295, https://doi.org/10.5194/acp-18-14271-2018, https://doi.org/10.5194/acp-18-14271-2018, 2018
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Water uptake can significantly increase the size and therefore alters the optical properties of aerosols. Our model study reveals that the high moisture and aerosol burden in the southern West African monsoon
layer makes it favorable to quantify properties that determine the aerosol liquid water content and its impact on the aerosol optical depth and radiative transfer. Especially in moist tropical environments the relative humidity impact on AOD has to be considered in atmospheric models.
Luca Naitza, Davide Putero, Angela Marinoni, Francescopiero Calzolari, Fabrizio Roccato, Maurizio Busetto, Damiano Sferlazzo, Eleonora Aruffo, Piero Di Carlo, Mariantonia Bencardino, Francesco D'Amore, Francesca Sprovieri, Nicola Pirrone, Federico Dallo, Jacopo Gabrieli, Massimiliano Vardè, Carlo Barbante, Paolo Bonasoni, and Paolo Cristofanelli
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2018-245, https://doi.org/10.5194/amt-2018-245, 2018
Revised manuscript not accepted
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We implemented a prototype of a centralized system to support atmospheric observatories in data production and submission. By using the “R” Language, for several near-surface ECVs, we developed specific routines for data filtering, flagging, formatting, and creation of data products for detecting instrumental problems or special atmospheric events. Our effort would improve atmospheric data quality, accelerate the process of data submission and make the data flagging more “objective".
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.
Michael Priestley, Michael le Breton, Thomas J. Bannan, Stephen D. Worrall, Asan Bacak, Andrew R. D. Smedley, Ernesto Reyes-Villegas, Archit Mehra, James Allan, Ann R. Webb, Dudley E. Shallcross, Hugh Coe, and Carl J. Percival
Atmos. Chem. Phys., 18, 13481–13493, https://doi.org/10.5194/acp-18-13481-2018, https://doi.org/10.5194/acp-18-13481-2018, 2018
Fernando Santos, Karla Longo, Alex Guenther, Saewung Kim, Dasa Gu, Dave Oram, Grant Forster, James Lee, James Hopkins, Joel Brito, and Saulo Freitas
Atmos. Chem. Phys., 18, 12715–12734, https://doi.org/10.5194/acp-18-12715-2018, https://doi.org/10.5194/acp-18-12715-2018, 2018
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We investigated the impact of biomass burning on the chemical composition of trace gases in the Amazon. The findings corroborate the influence of biomass burning activity not only on direct emissions of particulate matter but also on the oxidative capacity to produce secondary organic aerosol. The scientists plan to use this information to improve the numerical model simulation with a better representativeness of the chemical processes, which can impact on global climate prediction.
Paul I. Palmer, Simon O'Doherty, Grant Allen, Keith Bower, Hartmut Bösch, Martyn P. Chipperfield, Sarah Connors, Sandip Dhomse, Liang Feng, Douglas P. Finch, Martin W. Gallagher, Emanuel Gloor, Siegfried Gonzi, Neil R. P. Harris, Carole Helfter, Neil Humpage, Brian Kerridge, Diane Knappett, Roderic L. Jones, Michael Le Breton, Mark F. Lunt, Alistair J. Manning, Stephan Matthiesen, Jennifer B. A. Muller, Neil Mullinger, Eiko Nemitz, Sebastian O'Shea, Robert J. Parker, Carl J. Percival, Joseph Pitt, Stuart N. Riddick, Matthew Rigby, Harjinder Sembhi, Richard Siddans, Robert L. Skelton, Paul Smith, Hannah Sonderfeld, Kieran Stanley, Ann R. Stavert, Angelina Wenger, Emily White, Christopher Wilson, and Dickon Young
Atmos. Chem. Phys., 18, 11753–11777, https://doi.org/10.5194/acp-18-11753-2018, https://doi.org/10.5194/acp-18-11753-2018, 2018
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This paper provides an overview of the Greenhouse gAs Uk and Global Emissions (GAUGE) experiment. GAUGE was designed to quantify nationwide GHG emissions of the UK, bringing together measurements and atmospheric transport models. This novel experiment is the first of its kind. We anticipate it will inform the blueprint for countries that are building a measurement infrastructure in preparation for global stocktakes, which are a key part of the Paris Agreement.
Wei Zhou, Jian Zhao, Bin Ouyang, Archit Mehra, Weiqi Xu, Yuying Wang, Thomas J. Bannan, Stephen D. Worrall, Michael Priestley, Asan Bacak, Qi Chen, Conghui Xie, Qingqing Wang, Junfeng Wang, Wei Du, Yingjie Zhang, Xinlei Ge, Penglin Ye, James D. Lee, Pingqing Fu, Zifa Wang, Douglas Worsnop, Roderic Jones, Carl J. Percival, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 18, 11581–11597, https://doi.org/10.5194/acp-18-11581-2018, https://doi.org/10.5194/acp-18-11581-2018, 2018
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We present measurements of gas-phase N2O5 and ClNO2 by ToF-CIMS during summer in urban Beijing as part of the APHH campaign. High reactivity of N2O5 indicative of active nocturnal chemistry was observed. The lifetime of N2O5 as a function of aerosol surface area and relative humidity was characterized, and N2O5 uptake coefficients were estimated. We also found that the N2O5 loss in this study is mainly attributed to its indirect loss via reactions of NO3 with VOCs and NO.
Prasad Kasibhatla, Tomás Sherwen, Mathew J. Evans, Lucy J. Carpenter, Chris Reed, Becky Alexander, Qianjie Chen, Melissa P. Sulprizio, James D. Lee, Katie A. Read, William Bloss, Leigh R. Crilley, William C. Keene, Alexander A. P. Pszenny, and Alma Hodzic
Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, https://doi.org/10.5194/acp-18-11185-2018, 2018
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Recent measurements of NOx and HONO suggest that photolysis of particulate nitrate in sea-salt aerosols is important in terms of marine boundary layer oxidant chemistry. We present the first global-scale assessment of the significance of this new chemical pathway for NOx, O3, and OH in the marine boundary layer. We also present a preliminary assessment of the potential impact of photolysis of particulate nitrate associated with other aerosol types on continental boundary layer chemistry.
Kelly L. Pereira, Rachel Dunmore, James Whitehead, M. Rami Alfarra, James D. Allan, Mohammed S. Alam, Roy M. Harrison, Gordon McFiggans, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 18, 11073–11096, https://doi.org/10.5194/acp-18-11073-2018, https://doi.org/10.5194/acp-18-11073-2018, 2018
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Exhaust emissions from a light-duty diesel engine were introduced into an atmospheric simulation chamber which was used as a holding-cell for sampling, allowing instruments capable of providing detailed chemical speciation of exhaust gas emissions to be used. The effect of different engine conditions on the exhaust gas composition was investigated. The exhaust composition changed considerably due to two influencing factors, engine combustion and diesel oxidative catalyst efficiency.
Jun Duan, Min Qin, Bin Ouyang, Wu Fang, Xin Li, Keding Lu, Ke Tang, Shuaixi Liang, Fanhao Meng, Zhaokun Hu, Pinhua Xie, Wenqing Liu, and Rolf Häsler
Atmos. Meas. Tech., 11, 4531–4543, https://doi.org/10.5194/amt-11-4531-2018, https://doi.org/10.5194/amt-11-4531-2018, 2018
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We report a custom-built instrument for simultaneous unambiguous measurements of HONO and NO2 based on incoherent broadband cavity enhanced absorption spectroscopy (IBBCEAS). The current IBBCEAS instrument has made significant improvements in terms of efficient sampling as well as resistance against vibration; temperature change and the measurement precisions (2σ) for HONO are about 180 and 340 ppt in 30 s, respectively. The field inter-comparison and the mobile measurements are present.
Konrad Deetz, Heike Vogel, Peter Knippertz, Bianca Adler, Jonathan Taylor, Hugh Coe, Keith Bower, Sophie Haslett, Michael Flynn, James Dorsey, Ian Crawford, Christoph Kottmeier, and Bernhard Vogel
Atmos. Chem. Phys., 18, 9767–9788, https://doi.org/10.5194/acp-18-9767-2018, https://doi.org/10.5194/acp-18-9767-2018, 2018
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Highly resolved process study simulations for 2–3 July are conducted with COSMO-ART to assess the aerosol direct and indirect effect on meteorological conditions over southern West Africa. The meteorological phenomena of Atlantic inflow and stratus-to-cumulus transition are identified as highly susceptible to the aerosol direct effect, leading to a spatial shift of the Atlantic inflow front and a temporal shift of the stratus-to-cumulus transition with changes in the aerosol amount.
Sekou Keita, Cathy Liousse, Véronique Yoboué, Pamela Dominutti, Benjamin Guinot, Eric-Michel Assamoi, Agnès Borbon, Sophie L. Haslett, Laetitia Bouvier, Aurélie Colomb, Hugh Coe, Aristide Akpo, Jacques Adon, Julien Bahino, Madina Doumbia, Julien Djossou, Corinne Galy-Lacaux, Eric Gardrat, Sylvain Gnamien, Jean F. Léon, Money Ossohou, E. Touré N'Datchoh, and Laurent Roblou
Atmos. Chem. Phys., 18, 7691–7708, https://doi.org/10.5194/acp-18-7691-2018, https://doi.org/10.5194/acp-18-7691-2018, 2018
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This study provides emission factor (EF) data for elemental and organic carbon, total particulate matter and 58 volatile organic compound species for combustion sources specific to Africa to establish emission inventories with less uncertainty. EFs obtained in this study are generally higher than those in the literature whose values are used in emissions inventories for Africa. This shows that particles and VOC emissions were sometimes underestimated and underlines this study's importance.
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.
Amy K. Hodgson, William T. Morgan, Sebastian O'Shea, Stéphane Bauguitte, James D. Allan, Eoghan Darbyshire, Michael J. Flynn, Dantong Liu, James Lee, Ben Johnson, Jim M. Haywood, Karla M. Longo, Paulo E. Artaxo, and Hugh Coe
Atmos. Chem. Phys., 18, 5619–5638, https://doi.org/10.5194/acp-18-5619-2018, https://doi.org/10.5194/acp-18-5619-2018, 2018
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We flew a large atmospheric research aircraft across a number of different biomass burning environments in the Amazon Basin in September and October 2012. In this paper, we focus on smoke sampled very close to fresh fires (only 600–900 m above the fires and smoke that was 4–6 min old) to examine the chemical components that make up the smoke and their abundance. We found substantial differences in the emitted smoke that are due to the fuel type and combustion processes driving the fires.
Karina E. Adcock, Claire E. Reeves, Lauren J. Gooch, Emma C. Leedham Elvidge, Matthew J. Ashfold, Carl A. M. Brenninkmeijer, Charles Chou, Paul J. Fraser, Ray L. Langenfelds, Norfazrin Mohd Hanif, Simon O'Doherty, David E. Oram, Chang-Feng Ou-Yang, Siew Moi Phang, Azizan Abu Samah, Thomas Röckmann, William T. Sturges, and Johannes C. Laube
Atmos. Chem. Phys., 18, 4737–4751, https://doi.org/10.5194/acp-18-4737-2018, https://doi.org/10.5194/acp-18-4737-2018, 2018
Felix A. Mackenzie-Rae, Helen J. Wallis, Andrew R. Rickard, Kelly L. Pereira, Sandra M. Saunders, Xinming Wang, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 18, 4673–4693, https://doi.org/10.5194/acp-18-4673-2018, https://doi.org/10.5194/acp-18-4673-2018, 2018
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Native to Australasia, the remarkable adaptability, rapid growth rates and high quality wood of eucalypt trees has led to them the most widely planted hardwood forest trees in the world. In contrast to boreal and tropical forests, there has been little study of aerosol formation in these regions. Here, we study the secondary organic aerosol formation from the very fast reaction of α-phellandrene, emitted from eucalypts, and identify key products and reaction pathways.
Riinu Ots, Mathew R. Heal, Dominique E. Young, Leah R. Williams, James D. Allan, Eiko Nemitz, Chiara Di Marco, Anais Detournay, Lu Xu, Nga L. Ng, Hugh Coe, Scott C. Herndon, Ian A. Mackenzie, David C. Green, Jeroen J. P. Kuenen, Stefan Reis, and Massimo Vieno
Atmos. Chem. Phys., 18, 4497–4518, https://doi.org/10.5194/acp-18-4497-2018, https://doi.org/10.5194/acp-18-4497-2018, 2018
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The main hypothesis of this paper is that people who live in large cities in the UK disobey the
smoke control lawas it has not been actively enforced for decades now. However, the use of wood in residential heating has increased, partly due to renewable energy targets, but also for discretionary (i.e. pleasant fireplaces) reasons. Our study is based mainly in London, but similar struggles with urban air quality due to residential wood and coal burning are seen in other major European cities.
James D. Lee, Stephen D. Mobbs, Axel Wellpott, Grant Allen, Stephane J.-B. Bauguitte, Ralph R. Burton, Richard Camilli, Hugh Coe, Rebecca E. Fisher, James L. France, Martin Gallagher, James R. Hopkins, Mathias Lanoiselle, Alastair C. Lewis, David Lowry, Euan G. Nisbet, Ruth M. Purvis, Sebastian O'Shea, John A. Pyle, and Thomas B. Ryerson
Atmos. Meas. Tech., 11, 1725–1739, https://doi.org/10.5194/amt-11-1725-2018, https://doi.org/10.5194/amt-11-1725-2018, 2018
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This work describes measurements, made from an aircraft platform, of the emission of methane and other organic gases from an uncontrolled leak from an oil platform in the North Sea (Total Elgin). The measurements made helped the platform operators to devise a strategy for repairing the leak and serve as a methodology for assessing future similar incidents.
Ernesto Reyes-Villegas, Michael Priestley, Yu-Chieh Ting, Sophie Haslett, Thomas Bannan, Michael Le Breton, Paul I. Williams, Asan Bacak, Michael J. Flynn, Hugh Coe, Carl Percival, and James D. Allan
Atmos. Chem. Phys., 18, 4093–4111, https://doi.org/10.5194/acp-18-4093-2018, https://doi.org/10.5194/acp-18-4093-2018, 2018
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This work presents the analysis of a special event with high biomass burning emissions, named Bonfire Night. Nitrogen chemistry was observed and it was possible to study the night time chemistry. It was possible to quantify particulate organic oxides of nitrogen (PON) concentrations of 2.8 µg m−3 using 46 : 30 ratios from aerosol mass spectrometry measurements. The use of the receptor model positive matrix factorization (PMF) allowed to separate organic aerosols into different sources.
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.
Dantong Liu, Jonathan W. Taylor, Jonathan Crosier, Nicholas Marsden, Keith N. Bower, Gary Lloyd, Claire L. Ryder, Jennifer K. Brooke, Richard Cotton, Franco Marenco, Alan Blyth, Zhiqiang Cui, Victor Estelles, Martin Gallagher, Hugh Coe, and Tom W. Choularton
Atmos. Chem. Phys., 18, 3817–3838, https://doi.org/10.5194/acp-18-3817-2018, https://doi.org/10.5194/acp-18-3817-2018, 2018
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This article presents measurements of aerosol properties off the coast of west Africa during August 2015. For the first time, an airborne laser-induced incandescence instrument was deployed to measure the hematite content of dust. The single scattering albedo of dust was found to be influenced by the hematite content, but depended on the dust source and potential dust age. This highlights the importance of size-dependent composition in determining the optical properties of dust.
Daniel Stone, Tomás Sherwen, Mathew J. Evans, Stewart Vaughan, Trevor Ingham, Lisa K. Whalley, Peter M. Edwards, Katie A. Read, James D. Lee, Sarah J. Moller, Lucy J. Carpenter, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 3541–3561, https://doi.org/10.5194/acp-18-3541-2018, https://doi.org/10.5194/acp-18-3541-2018, 2018
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Halogen chemistry in the troposphere impacts oxidising capacity, but model studies assessing the nature of these impacts can vary according to the model framework used. In this work we present simulations of OH and HO2 radicals using both box and global model frameworks, and compare to observations made at the Cape Verde Atmospheric Observatory. We highlight, and rationalise, differences between the model frameworks.
Lisa K. Whalley, Daniel Stone, Rachel Dunmore, Jacqueline Hamilton, James R. Hopkins, James D. Lee, Alastair C. Lewis, Paul Williams, Jörg Kleffmann, Sebastian Laufs, Robert Woodward-Massey, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 2547–2571, https://doi.org/10.5194/acp-18-2547-2018, https://doi.org/10.5194/acp-18-2547-2018, 2018
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This paper presents the first radical observations made in London and subsequent model comparisons. This work highlights that there are uncertainties in the degradation mechanism of complex biogenic and diesel-related VOC species under low-NOx conditions and under high-NOx conditions there is a missing source of RO2 radicals. The impact of these model uncertainties on in situ ozone production as a function of NOx is discussed.
Joel Brito, Evelyn Freney, Pamela Dominutti, Agnes Borbon, Sophie L. Haslett, Anneke M. Batenburg, Aurelie Colomb, Regis Dupuy, Cyrielle Denjean, Frederic Burnet, Thierry Bourriane, Adrien Deroubaix, Karine Sellegri, Stephan Borrmann, Hugh Coe, Cyrille Flamant, Peter Knippertz, and Alfons Schwarzenboeck
Atmos. Chem. Phys., 18, 757–772, https://doi.org/10.5194/acp-18-757-2018, https://doi.org/10.5194/acp-18-757-2018, 2018
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This work focuses on sources of submicron aerosol particles over southern West Africa (SWA). Results have shown that isoprene, a gas-phase compound of biogenic origin, is responsible for roughly 25 % of the organic aerosol (OA) loading, under most background or urban plumes alike. This fraction represents a lower estimate from the biogenic contribution in this fairly polluted region. This work sheds light upon the role of anthropogenic and biogenic emissions on the pollution burden over SWA.
Sophie L. Haslett, J. Chris Thomas, William T. Morgan, Rory Hadden, Dantong Liu, James D. Allan, Paul I. Williams, Sekou Keita, Cathy Liousse, and Hugh Coe
Atmos. Chem. Phys., 18, 385–403, https://doi.org/10.5194/acp-18-385-2018, https://doi.org/10.5194/acp-18-385-2018, 2018
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Wood burning is chaotic, so the particles emitted can be difficult to study in a repeatable way. Here, we addressed this problem by carefully controlling small wood fires in the lab. We saw three burning phases, which could be told apart chemically; we also saw evidence of these in measurements of wood burning in London in 2012. Controlled experiments like this help us to understand why emissions are so variable and to recognise burning conditions just from the particles seen in the atmosphere.
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.
Nicholas A. Marsden, Michael J. Flynn, James D. Allan, and Hugh Coe
Atmos. Meas. Tech., 11, 195–213, https://doi.org/10.5194/amt-11-195-2018, https://doi.org/10.5194/amt-11-195-2018, 2018
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Mineralogy of silicate mineral dust has a strong influence on climate and ecosystems due to variation in physiochemical properties that result from differences in composition and crystal structure (mineral phase). Traditional offline methods of analysing mineral phase are labour intensive and the temporal resolution of the data is lost. We introduce a novel technique that enables the online differentiation of mineral phase in silicate particles by single-particle mass spectrometry.
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.
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).
David E. Oram, Matthew J. Ashfold, Johannes C. Laube, Lauren J. Gooch, Stephen Humphrey, William T. Sturges, Emma Leedham-Elvidge, Grant L. Forster, Neil R. P. Harris, Mohammed Iqbal Mead, Azizan Abu Samah, Siew Moi Phang, Chang-Feng Ou-Yang, Neng-Huei Lin, Jia-Lin Wang, Angela K. Baker, Carl A. M. Brenninkmeijer, and David Sherry
Atmos. Chem. Phys., 17, 11929–11941, https://doi.org/10.5194/acp-17-11929-2017, https://doi.org/10.5194/acp-17-11929-2017, 2017
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We have observed large amounts of man-made chlorine compounds in E and SE Asia and in the upper tropical troposphere. These relatively short-lived compounds are not controlled by the Montreal Protocol, but if significant quantities were able to reach the stratosphere, the long-term recovery of stratospheric ozone would be delayed. We have also identified an important atmospheric transport mechanism that can rapidly transport these chemicals from E Asia to the upper troposphere via the tropics.
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.
Mike J. Newland, Patricia Martinerie, Emmanuel Witrant, Detlev Helmig, David R. Worton, Chris Hogan, William T. Sturges, and Claire E. Reeves
Atmos. Chem. Phys., 17, 8269–8283, https://doi.org/10.5194/acp-17-8269-2017, https://doi.org/10.5194/acp-17-8269-2017, 2017
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We report increasing levels of alkyl nitrates in the Northern Hemisphere atmosphere between 1960 and the mid-1990s. These increases are symptomatic of large-scale changes to the chemical composition of the atmosphere, particularly with regards to the amounts of short-lived, reactive species. The observed increases are likely driven by increasing levels of nitrogen oxides. These changes have direct implications for the lifetimes of climate-relevant species in the atmosphere, such as methane.
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.
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.
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%.
Alexandra Tsekeri, Vassilis Amiridis, Franco Marenco, Athanasios Nenes, Eleni Marinou, Stavros Solomos, Phil Rosenberg, Jamie Trembath, Graeme J. Nott, James Allan, Michael Le Breton, Asan Bacak, Hugh Coe, Carl Percival, and Nikolaos Mihalopoulos
Atmos. Meas. Tech., 10, 83–107, https://doi.org/10.5194/amt-10-83-2017, https://doi.org/10.5194/amt-10-83-2017, 2017
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The In situ/Remote sensing aerosol Retrieval Algorithm (IRRA) provides vertical profiles of aerosol optical, microphysical and hygroscopic properties from airborne in situ and remote sensing measurements. The algorithm is highly advantageous for aerosol characterization in humid conditions, employing the ISORROPIA II model for acquiring the particle hygroscopic growth. IRRA can find valuable applications in aerosol–cloud interaction schemes and in validation of active space-borne sensors.
Ernesto Reyes-Villegas, David C. Green, Max Priestman, Francesco Canonaco, Hugh Coe, André S. H. Prévôt, and James D. Allan
Atmos. Chem. Phys., 16, 15545–15559, https://doi.org/10.5194/acp-16-15545-2016, https://doi.org/10.5194/acp-16-15545-2016, 2016
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For the first time in the UK, an Aerosol Chemical Speciation Monitor was used to measure aerosol concentrations in London in March–December 2013, with further organic aerosol (OA) source apportionment using the ME-2 factorization tool. Five OA sources were identified: biomass burning OA, hydrocarbon-like OA, cooking OA, semivolatile oxygenated OA and low-volatility oxygenated OA. This information can be used to take future action on the respective legislation in order to improve the air quality.
Nicholas Marsden, Michael J. Flynn, Jonathan W. Taylor, James D. Allan, and Hugh Coe
Atmos. Meas. Tech., 9, 6051–6068, https://doi.org/10.5194/amt-9-6051-2016, https://doi.org/10.5194/amt-9-6051-2016, 2016
Johannes C. Laube, Norfazrin Mohd Hanif, Patricia Martinerie, Eileen Gallacher, Paul J. Fraser, Ray Langenfelds, Carl A. M. Brenninkmeijer, Jakob Schwander, Emmanuel Witrant, Jia-Lin Wang, Chang-Feng Ou-Yang, Lauren J. Gooch, Claire E. Reeves, William T. Sturges, and David E. Oram
Atmos. Chem. Phys., 16, 15347–15358, https://doi.org/10.5194/acp-16-15347-2016, https://doi.org/10.5194/acp-16-15347-2016, 2016
Ben T. Johnson, James M. Haywood, Justin M. Langridge, Eoghan Darbyshire, William T. Morgan, Kate Szpek, Jennifer K. Brooke, Franco Marenco, Hugh Coe, Paulo Artaxo, Karla M. Longo, Jane P. Mulcahy, Graham W. Mann, Mohit Dalvi, and Nicolas Bellouin
Atmos. Chem. Phys., 16, 14657–14685, https://doi.org/10.5194/acp-16-14657-2016, https://doi.org/10.5194/acp-16-14657-2016, 2016
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Biomass burning is a large source of carbonaceous aerosols, which scatter and absorb solar radiation, and modify cloud properties. We evaluate the simulation of biomass burning aerosol processes and properties in the HadGEM3 climate model using observations, including those from the South American Biomass Burning Analysis. We find that modelled aerosol optical depths are underestimated unless aerosol emissions (Global Fire Emission Database v3) are increased by a factor of 1.6–2.0.
Eleonora Aruffo, Fabio Biancofiore, Piero Di Carlo, Marcella Busilacchio, Marco Verdecchia, Barbara Tomassetti, Cesare Dari-Salisburgo, Franco Giammaria, Stephane Bauguitte, James Lee, Sarah Moller, James Hopkins, Shalini Punjabi, Stephen J. Andrews, Alistair C. Lewis, Paul I. Palmer, Edward Hyer, Michael Le Breton, and Carl Percival
Atmos. Meas. Tech., 9, 5591–5606, https://doi.org/10.5194/amt-9-5591-2016, https://doi.org/10.5194/amt-9-5591-2016, 2016
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During the BORTAS aircraft campaign, we measured NO2 and their oxidtation products (as peroxy nitrates) with a custom laser-induced fluorescence instrument. Because of the high correlation between known pyrogenic tracers (i.e., carbon monoxide) and peroxy nitrates, we provide two methods to use these species for the identification of biomass burning (BB) plumes. Using an artifical neural network, we improved the BB identification taking into account of a meteorological parameter (pressure).
Riinu Ots, Massimo Vieno, James D. Allan, Stefan Reis, Eiko Nemitz, Dominique E. Young, Hugh Coe, Chiara Di Marco, Anais Detournay, Ian A. Mackenzie, David C. Green, and Mathew R. Heal
Atmos. Chem. Phys., 16, 13773–13789, https://doi.org/10.5194/acp-16-13773-2016, https://doi.org/10.5194/acp-16-13773-2016, 2016
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Emissions of cooking organic aerosol (COA; from charbroiling, frying, etc.) are currently absent in European emissions inventories yet measurements have pointed to significant COA concentrations. In this study, emissions of COA were developed for the UK by model iteration against year-long measurements at two sites in London. Modelled COA dropped rapidly outside of major urban areas, suggesting that although a notable component in UK urban air, COA does not have a significant effect on rural PM.
Stephen J. Andrews, Lucy J. Carpenter, Eric C. Apel, Elliot Atlas, Valeria Donets, James R. Hopkins, Rebecca S. Hornbrook, Alastair C. Lewis, Richard T. Lidster, Richard Lueb, Jamie Minaeian, Maria Navarro, Shalini Punjabi, Daniel Riemer, and Sue Schauffler
Atmos. Meas. Tech., 9, 5213–5225, https://doi.org/10.5194/amt-9-5213-2016, https://doi.org/10.5194/amt-9-5213-2016, 2016
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We present a comparison of aircraft measurements of important trace gases from a co-ordinated campaign in Jan–Feb 2014 in the tropical west Pacific involving the NASA Global Hawk, NCAR GV and FAAM BAe-146 aircraft.
The paper studies the comparability of separate measurements across platforms and demonstrates that aircraft measurements are relevant for characterising the vertical uplift of important gases, such as those with ozone-depleting potential, to the upper troposphere–lower stratosphere.
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.
Graham P. Mills, Glyn D. Hiatt-Gipson, Sean P. Bew, and Claire E. Reeves
Atmos. Meas. Tech., 9, 4533–4545, https://doi.org/10.5194/amt-9-4533-2016, https://doi.org/10.5194/amt-9-4533-2016, 2016
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The paper describes the development of an instrument to measure isoprene-derived nitrates in the atmosphere, compounds that are crucial to understanding the impact of biogenic hydrocarbons on ozone production. The instrument is suitable for deployment in field studies.
James D. Whitehead, Eoghan Darbyshire, Joel Brito, Henrique M. J. Barbosa, Ian Crawford, Rafael Stern, Martin W. Gallagher, Paul H. Kaye, James D. Allan, Hugh Coe, Paulo Artaxo, and Gordon McFiggans
Atmos. Chem. Phys., 16, 9727–9743, https://doi.org/10.5194/acp-16-9727-2016, https://doi.org/10.5194/acp-16-9727-2016, 2016
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We present measurements of aerosols during the transition from wet to dry seasons at a pristine rainforest site in central Amazonia. By excluding pollution episodes, we focus on natural biogenic aerosols. Submicron aerosols are dominated by organic material, similar to previous wet season measurements. Larger particles are dominated by biological material, mostly fungal spores, with higher concentrations at night. This study provides important data on the nature of particles above the Amazon.
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.
R. Hossaini, P. K. Patra, A. A. Leeson, G. Krysztofiak, N. L. Abraham, S. J. Andrews, A. T. Archibald, J. Aschmann, E. L. Atlas, D. A. Belikov, H. Bönisch, L. J. Carpenter, S. Dhomse, M. Dorf, A. Engel, W. Feng, S. Fuhlbrügge, P. T. Griffiths, N. R. P. Harris, R. Hommel, T. Keber, K. Krüger, S. T. Lennartz, S. Maksyutov, H. Mantle, G. P. Mills, B. Miller, S. A. Montzka, F. Moore, M. A. Navarro, D. E. Oram, K. Pfeilsticker, J. A. Pyle, B. Quack, A. D. Robinson, E. Saikawa, A. Saiz-Lopez, S. Sala, B.-M. Sinnhuber, S. Taguchi, S. Tegtmeier, R. T. Lidster, C. Wilson, and F. Ziska
Atmos. Chem. Phys., 16, 9163–9187, https://doi.org/10.5194/acp-16-9163-2016, https://doi.org/10.5194/acp-16-9163-2016, 2016
Dene R. Bowdalo, Mathew J. Evans, and Eric D. Sofen
Atmos. Chem. Phys., 16, 8295–8308, https://doi.org/10.5194/acp-16-8295-2016, https://doi.org/10.5194/acp-16-8295-2016, 2016
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We introduce a new methodology for the assessment of atmospheric models with observations. We apply a spectral analysis methodology to hourly ozone observations and the equivalent model output. The spectrally transformed observational data show significant peaks on daily and annual timescales. Comparison between the amplitude and phase of these peaks introduces a new comparison methodology between model and measurements. We find the model shows significant biases on an annual timescale.
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.
Chris Reed, Charlotte A. Brumby, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Paul W. Seakins, James D. Lee, and Lucy J. Carpenter
Atmos. Meas. Tech., 9, 2483–2495, https://doi.org/10.5194/amt-9-2483-2016, https://doi.org/10.5194/amt-9-2483-2016, 2016
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A new method of measuring nitrous acid (HONO), a potent mediator of air quality in the atmosphere as well as an important indoor pollutant, is presented. The new method relies on simple, proven techniques already widely applied to other atmospheric compounds. The technique can be retrofitted to existing analysers at minimal cost, or developed into instruments capable of very fast measurement which allow for more complex analysis of the behaviour of HONO.
Riinu Ots, Dominique E. Young, Massimo Vieno, Lu Xu, Rachel E. Dunmore, James D. Allan, Hugh Coe, Leah R. Williams, Scott C. Herndon, Nga L. Ng, Jacqueline F. Hamilton, Robert Bergström, Chiara Di Marco, Eiko Nemitz, Ian A. Mackenzie, Jeroen J. P. Kuenen, David C. Green, Stefan Reis, and Mathew R. Heal
Atmos. Chem. Phys., 16, 6453–6473, https://doi.org/10.5194/acp-16-6453-2016, https://doi.org/10.5194/acp-16-6453-2016, 2016
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This study investigates the contribution of diesel vehicle emissions to organic aerosol formation and particulate matter concentrations in London. Comparisons of simulated pollutant concentrations with observations show good agreement and give confidence in the skill of the model applied. The contribution of diesel vehicle emissions, which are currently not included in official emissions inventories, is demonstrated to be substantial, indicating that more research on this topic is required.
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.
Rebecca M. McKenzie, Mustafa Z. Özel, J. Neil Cape, Julia Drewer, Kerry J. Dinsmore, Eiko Nemitz, Y. Sim Tang, Netty van Dijk, Margaret Anderson, Jacqueline F. Hamilton, Mark A. Sutton, Martin W. Gallagher, and Ute Skiba
Biogeosciences, 13, 2353–2365, https://doi.org/10.5194/bg-13-2353-2016, https://doi.org/10.5194/bg-13-2353-2016, 2016
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Dissolved organic nitrogen (DON) contributes significantly to the overall nitrogen budget and can potentially be biologically available as a source of N. Despite this it is not routinely measured. This study found that DON contributed up to 10 % of the total dissolved nitrogen (TDN) found in precipitation and was the most dominant fraction in soil water (99 %) and stream water (75 %).
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.
Marcella Busilacchio, Piero Di Carlo, Eleonora Aruffo, Fabio Biancofiore, Cesare Dari Salisburgo, Franco Giammaria, Stephane Bauguitte, James Lee, Sarah Moller, James Hopkins, Shalini Punjabi, Stephen Andrews, Alistair C. Lewis, Mark Parrington, Paul I. Palmer, Edward Hyer, and Glenn M. Wolfe
Atmos. Chem. Phys., 16, 3485–3497, https://doi.org/10.5194/acp-16-3485-2016, https://doi.org/10.5194/acp-16-3485-2016, 2016
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Boreal fire emissions have little effect on ozone concentrations but evident impact on some NOx reservoirs as peroxy nitrates that we quantified. This should be taken into account since NOx reservoirs can be efficiently transported and may influence the ozone budget far away from the fire emission.
The study is based on observations carried out on board the BAe 146 aircraft during BORTAS in Canada. We used a custom laser-induced fluorescence system to measure NO2 and NOx reservoirs.
J. D. Lee, L. K. Whalley, D. E. Heard, D. Stone, R. E. Dunmore, J. F. Hamilton, D. E. Young, J. D. Allan, S. Laufs, and J. Kleffmann
Atmos. Chem. Phys., 16, 2747–2764, https://doi.org/10.5194/acp-16-2747-2016, https://doi.org/10.5194/acp-16-2747-2016, 2016
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This paper presents field measurements of HONO and a range of other gas phase and particulate species from an urban background site in London. The measured daytime HONO cannot be reproduced with a simple box model and thus a significant daytime missing source of HONO is present. We show that this missing source could be responsible for 40 % of the OH radical source and 57 % of the OH initiation; hence its potential importance for atmospheric oxidation and ozone production.
Lisa K. Whalley, Daniel Stone, Brian Bandy, Rachel Dunmore, Jacqueline F. Hamilton, James Hopkins, James D. Lee, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 2109–2122, https://doi.org/10.5194/acp-16-2109-2016, https://doi.org/10.5194/acp-16-2109-2016, 2016
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.
L. Xu, L. R. Williams, D. E. Young, J. D. Allan, H. Coe, P. Massoli, E. Fortner, P. Chhabra, S. Herndon, W. A. Brooks, J. T. Jayne, D. R. Worsnop, A. C. Aiken, S. Liu, K. Gorkowski, M. K. Dubey, Z. L. Fleming, S. Visser, A. S. H. Prévôt, and N. L. Ng
Atmos. Chem. Phys., 16, 1139–1160, https://doi.org/10.5194/acp-16-1139-2016, https://doi.org/10.5194/acp-16-1139-2016, 2016
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We investigate the spatial distribution of submicron aerosol in the greater London area as part of the Clean Air for London (ClearfLo) project in winter 2012. Although the concentrations of organic aerosol (OA) are similar between a rural and an urban site, the OA sources are different. We also examine the volatility of submicron aerosol at the rural site and find that the non-volatile organics have similar sources or have undergone similar chemical processing as refractory black carbon.
J. R. Pitt, M. Le Breton, G. Allen, C. J. Percival, M. W. Gallagher, S. J.-B. Bauguitte, S. J. O'Shea, J. B. A. Muller, M. S. Zahniser, J. Pyle, and P. I. Palmer
Atmos. Meas. Tech., 9, 63–77, https://doi.org/10.5194/amt-9-63-2016, https://doi.org/10.5194/amt-9-63-2016, 2016
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We present details of an Aerodyne quantum cascade laser absorption spectrometer (QCLAS) used to make airborne measurements of N2O and CH4, including its configuration for use on board an aircraft. Two different methods to correct for the influence of water vapour on the measurements are evaluated. We diagnose a sensitivity of the instrument to changes in pressure, introduce a new calibration procedure to account for this effect, and assess its performance.
D. Putero, P. Cristofanelli, A. Marinoni, B. Adhikary, R. Duchi, S. D. Shrestha, G. P. Verza, T. C. Landi, F. Calzolari, M. Busetto, G. Agrillo, F. Biancofiore, P. Di Carlo, A. K. Panday, M. Rupakheti, and P. Bonasoni
Atmos. Chem. Phys., 15, 13957–13971, https://doi.org/10.5194/acp-15-13957-2015, https://doi.org/10.5194/acp-15-13957-2015, 2015
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The aim of this paper is to present a full-year analysis of simultaneous measurements of ozone, black carbon, and aerosol number concentration at Paknajol, in the Kathmandu Valley, one of the global “hot spots” in terms of air pollution. Results indicate persisting poor air quality conditions throughout the measurement period, and suggest that the pollutants' variability is mainly driven by local pollution source activity, local- and large-scale dynamics, photochemistry, and vegetation fires.
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.
W. W. Hu, P. Campuzano-Jost, B. B. Palm, D. A. Day, A. M. Ortega, P. L. Hayes, J. E. Krechmer, Q. Chen, M. Kuwata, Y. J. Liu, S. S. de Sá, K. McKinney, S. T. Martin, M. Hu, S. H. Budisulistiorini, M. Riva, J. D. Surratt, J. M. St. Clair, G. Isaacman-Van Wertz, L. D. Yee, A. H. Goldstein, S. Carbone, J. Brito, P. Artaxo, J. A. de Gouw, A. Koss, A. Wisthaler, T. Mikoviny, T. Karl, L. Kaser, W. Jud, A. Hansel, K. S. Docherty, M. L. Alexander, N. H. Robinson, H. Coe, J. D. Allan, M. R. Canagaratna, F. Paulot, and J. L. Jimenez
Atmos. Chem. Phys., 15, 11807–11833, https://doi.org/10.5194/acp-15-11807-2015, https://doi.org/10.5194/acp-15-11807-2015, 2015
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This work summarized all the studies reporting isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) measured globally by aerosol mass spectrometer and compare them with modeled gas-phase IEPOX, with results suggestive of the importance of IEPOX-SOA for regional and global OA budgets. A real-time tracer of IEPOX-SOA is thoroughly evaluated for the first time by combing multiple field and chamber studies. A quick and easy empirical method on IEPOX-SOA estimation is also presented.
D. Liu, B. Quennehen, E. Darbyshire, J. D. Allan, P. I. Williams, J. W. Taylor, S. J.-B. Bauguitte, M. J. Flynn, D. Lowe, M. W. Gallagher, K. N. Bower, T. W. Choularton, and H. Coe
Atmos. Chem. Phys., 15, 11537–11555, https://doi.org/10.5194/acp-15-11537-2015, https://doi.org/10.5194/acp-15-11537-2015, 2015
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We show that during the springtime of 2013, the anthropogenic pollution particularly from sources in Asia, contributed significantly to black carbon across the European Arctic free troposphere. In contrast to previous studies, the contribution from open wildfires was minimal. Given that Asian pollution is likely to continue to rise over the coming years, it is likely that the radiative forcing in the Arctic will also continue to increase.
S. Visser, J. G. Slowik, M. Furger, P. Zotter, N. Bukowiecki, F. Canonaco, U. Flechsig, K. Appel, D. C. Green, A. H. Tremper, D. E. Young, P. I. Williams, J. D. Allan, H. Coe, L. R. Williams, C. Mohr, L. Xu, N. L. Ng, E. Nemitz, J. F. Barlow, C. H. Halios, Z. L. Fleming, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 15, 11291–11309, https://doi.org/10.5194/acp-15-11291-2015, https://doi.org/10.5194/acp-15-11291-2015, 2015
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Trace element measurements in three particle size ranges (PM10-2.5, PM2.5-1.0 and PM1.0-0.3) were performed with 2h time resolution at kerbside, urban background and rural sites during the ClearfLo winter 2012 campaign in London. The environment-dependent variability of emissions was characterized using the Multilinear Engine implementation of the positive matrix factorization model. A total of nine different factors were resolved from local, regional and natural origin.
R. E. Dunmore, J. R. Hopkins, R. T. Lidster, J. D. Lee, M. J. Evans, A. R. Rickard, A. C. Lewis, and J. F. Hamilton
Atmos. Chem. Phys., 15, 9983–9996, https://doi.org/10.5194/acp-15-9983-2015, https://doi.org/10.5194/acp-15-9983-2015, 2015
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Technological shifts between fuel sources have had unexpected impacts on atmospheric composition and these significant changes can go undetected if source-specific monitoring infrastructure is not in place. We present chemically comprehensive, continuous measurements of organic compounds in a developed megacity (London), that show diesel-related hydrocarbons can dominate reactive carbon and ozone formation potential, highlighting a serious underestimation of this source in emission inventories.
J. G. Levine, A. R. MacKenzie, O. J. Squire, A. T. Archibald, P. T. Griffiths, N. L. Abraham, J. A. Pyle, D. E. Oram, G. Forster, J. F. Brito, J. D. Lee, J. R. Hopkins, A. C. Lewis, S. J. B. Bauguitte, C. F. Demarco, P. Artaxo, P. Messina, J. Lathière, D. A. Hauglustaine, E. House, C. N. Hewitt, and E. Nemitz
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-24251-2015, https://doi.org/10.5194/acpd-15-24251-2015, 2015
Revised manuscript has not been submitted
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This study explores our ability to simulate atmospheric chemistry stemming from isoprene emissions—a reactive gas emitted from vegetation—in pristine and polluted regions of the Amazon basin. We explore how two contrasting models fare in reproducing recent airborne measurements in the region. Their differing treatments of transport and mixing are found to: profoundly affect their performance; and yield very different pictures of the exposure of the rainforest to harmful ozone concentrations.
A. Saiz-Lopez, C. S. Blaszczak-Boxe, and L. J. Carpenter
Atmos. Chem. Phys., 15, 9731–9746, https://doi.org/10.5194/acp-15-9731-2015, https://doi.org/10.5194/acp-15-9731-2015, 2015
E. Athanasopoulou, A. P. Protonotariou, E. Bossioli, A. Dandou, M. Tombrou, J. D. Allan, H. Coe, N. Mihalopoulos, J. Kalogiros, A. Bacak, J. Sciare, and G. Biskos
Atmos. Chem. Phys., 15, 8401–8421, https://doi.org/10.5194/acp-15-8401-2015, https://doi.org/10.5194/acp-15-8401-2015, 2015
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A model system is evaluated versus ground and airborne aerosol measurements, towards the identification of its competencies and deficiencies over the eastern Mediterranean (EM) during summer. Secondary organic aerosol (OA) formation is investigated towards improving OA behaviour. Biomass burning is a significant particle source, largely explaining OA underestimation (ca. 50%). More than 70% of the aerosol mass over the EM is related to trans-boundary transport during strong northeastern winds.
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
K. P. Wyche, P. S. Monks, K. L. Smallbone, J. F. Hamilton, M. R. Alfarra, A. R. Rickard, G. B. McFiggans, M. E. Jenkin, W. J. Bloss, A. C. Ryan, C. N. Hewitt, and A. R. MacKenzie
Atmos. Chem. Phys., 15, 8077–8100, https://doi.org/10.5194/acp-15-8077-2015, https://doi.org/10.5194/acp-15-8077-2015, 2015
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This paper describes a new ensemble methodology for the statistical analysis of atmospheric gas- & particle-phase composition data sets. The methodology reduces the huge amount of data derived from many chamber experiments to show that organic reactivity & resultant particle formation can be mapped into unique clusters in statistical space. The model generated is used to map more realistic plant mesocosm oxidation data, the projection of which gives insight into reactive pathways & precursors.
M. J. Alvarado, C. R. Lonsdale, R. J. Yokelson, S. K. Akagi, H. Coe, J. S. Craven, E. V. Fischer, G. R. McMeeking, J. H. Seinfeld, T. Soni, J. W. Taylor, D. R. Weise, and C. E. Wold
Atmos. Chem. Phys., 15, 6667–6688, https://doi.org/10.5194/acp-15-6667-2015, https://doi.org/10.5194/acp-15-6667-2015, 2015
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Being able to understand and simulate the chemical evolution of biomass burning smoke plumes under a wide variety of conditions is a critical part of forecasting the impact of these fires on air quality, atmospheric composition, and climate. Here we use an improved model of this chemistry to simulate the evolution of ozone and secondary organic aerosol within a young biomass burning smoke plume from the Williams prescribed burn in chaparral, which was sampled over California in November 2009.
D. E. Young, J. D. Allan, P. I. Williams, D. C. Green, M. J. Flynn, R. M. Harrison, J. Yin, M. W. Gallagher, and H. Coe
Atmos. Chem. Phys., 15, 6351–6366, https://doi.org/10.5194/acp-15-6351-2015, https://doi.org/10.5194/acp-15-6351-2015, 2015
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For the first time, the behaviour of non-refractory inorganic and organic submicron particulates through an entire annual cycle is investigated at a UK urban background site. We show secondary aerosols account for a significant fraction of the submicron aerosol burden, high concentration events are governed by different factors depending on season, and on an annual basis there is no variability in the extent of secondary organic aerosol oxidation.
J. D. Allan, P. I. Williams, J. Najera, J. D. Whitehead, M. J. Flynn, J. W. Taylor, D. Liu, E. Darbyshire, L. J. Carpenter, R. Chance, S. J. Andrews, S. C. Hackenberg, and G. McFiggans
Atmos. Chem. Phys., 15, 5599–5609, https://doi.org/10.5194/acp-15-5599-2015, https://doi.org/10.5194/acp-15-5599-2015, 2015
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New particle formation (NPF) is an important contributor to aerosol number concentrations in the Arctic and thus has a major role in dictating cloud properties and climate in this region. Here we present direct evidence that the oxidation of iodine in the atmosphere causes NPF in the Greenland Sea. This is important because this is a NPF mechanism that has not previously been considered in modelling studies at these latitudes.
M. D. Shaw, J. D. Lee, B. Davison, A. Vaughan, R. M. Purvis, A. Harvey, A. C. Lewis, and C. N. Hewitt
Atmos. Chem. Phys., 15, 5083–5097, https://doi.org/10.5194/acp-15-5083-2015, https://doi.org/10.5194/acp-15-5083-2015, 2015
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This paper presents the first highly spatially resolved simultaneous mixing ratios of VOCs, NOx and O3 in the atmospheric boundary layer above Greater London (UK) using an research aircraft. Average mixing ratios measured at 360±10 m agl over outer London were always lower than over inner London, indicative of strong local vehicular sources. The comparison of airborne mixing ratio with LAQN air quality ground monitoring stations suggests that the mixing ratios were characteristic of the surface.
S. J. Andrews, S. C. Hackenberg, and L. J. Carpenter
Ocean Sci., 11, 313–321, https://doi.org/10.5194/os-11-313-2015, https://doi.org/10.5194/os-11-313-2015, 2015
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The oceans are a key source of a number of atmospherically
important volatile gases. The accurate and robust
determination of trace gases in seawater is a significant
analytical challenge. Here we describe a gas chromatograph mass spectrometer based purge and trap system that was developed for the fully automated analysis of dissolved very short-lived species (VSLS) in seawater sampled from a research ship.
J. W. Taylor, J. D. Allan, D. Liu, M. Flynn, R. Weber, X. Zhang, B. L. Lefer, N. Grossberg, J. Flynn, and H. Coe
Atmos. Meas. Tech., 8, 1701–1718, https://doi.org/10.5194/amt-8-1701-2015, https://doi.org/10.5194/amt-8-1701-2015, 2015
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When using the SP2 to report black carbon core/shell coating thickness, the core density and refractive index must be estimated from literature values. We systematically vary the assumed parameters and the instrument calibration, and quantify the effects in the derived coatings. The technique is highly sensitive to the core refractive index but has only a minor sensitivity to the core density and coating refractive index. We identify the most appropriate values to use in future analysis.
Q. Chen, D. K. Farmer, L. V. Rizzo, T. Pauliquevis, M. Kuwata, T. G. Karl, A. Guenther, J. D. Allan, H. Coe, M. O. Andreae, U. Pöschl, J. L. Jimenez, P. Artaxo, and S. T. Martin
Atmos. Chem. Phys., 15, 3687–3701, https://doi.org/10.5194/acp-15-3687-2015, https://doi.org/10.5194/acp-15-3687-2015, 2015
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Submicron particle mass concentration in the Amazon during the wet season of 2008 was dominated by organic material. The PMF analysis finds a comparable importance of gas-phase (gas-to-particle condensation) and particle-phase (reactive uptake of isoprene oxidation products, especially of epoxydiols to acidic haze, fog, or cloud droplets) production of secondary organic material during the study period, together accounting for >70% of the organic-particle mass concentration.
L. K. Whalley, D. Stone, I. J. George, S. Mertes, D. van Pinxteren, A. Tilgner, H. Herrmann, M. J. Evans, and D. E. Heard
Atmos. Chem. Phys., 15, 3289–3301, https://doi.org/10.5194/acp-15-3289-2015, https://doi.org/10.5194/acp-15-3289-2015, 2015
L. R. Crilley, W. J. Bloss, J. Yin, D. C. S. Beddows, R. M. Harrison, J. D. Allan, D. E. Young, M. Flynn, P. Williams, P. Zotter, A. S. H. Prevot, M. R. Heal, J. F. Barlow, C. H. Halios, J. D. Lee, S. Szidat, and C. Mohr
Atmos. Chem. Phys., 15, 3149–3171, https://doi.org/10.5194/acp-15-3149-2015, https://doi.org/10.5194/acp-15-3149-2015, 2015
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Wood is a renewable fuel but its combustion for residential heating releases a number of locally acting air pollutants, most notably particulate matter known to have adverse effects on human health. This paper used chemical tracers for wood smoke to estimate the contribution that burning wood makes to concentrations of airborne particles in the atmosphere of southern England and most particularly in London.
M. D. Jolleys, H. Coe, G. McFiggans, J. W. Taylor, S. J. O'Shea, M. Le Breton, S. J.-B. Bauguitte, S. Moller, P. Di Carlo, E. Aruffo, P. I. Palmer, J. D. Lee, C. J. Percival, and M. W. Gallagher
Atmos. Chem. Phys., 15, 3077–3095, https://doi.org/10.5194/acp-15-3077-2015, https://doi.org/10.5194/acp-15-3077-2015, 2015
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Particulate emissions in the form of organic aerosol from boreal forest fires in Canada have been measured during an aircraft measurement campaign. Ratios of the amount of aerosol emitted relative to gas species such as CO were calculated and show high levels of variability throughout the campaign. This variability is affected by both changes in fire conditions, as fires tended to die down later in the measurement period, and by changes to the aerosol due to chemical reactions in the atmosphere.
S. Archer-Nicholls, D. Lowe, E. Darbyshire, W. T. Morgan, M. M. Bela, G. Pereira, J. Trembath, J. W. Kaiser, K. M. Longo, S. R. Freitas, H. Coe, and G. McFiggans
Geosci. Model Dev., 8, 549–577, https://doi.org/10.5194/gmd-8-549-2015, https://doi.org/10.5194/gmd-8-549-2015, 2015
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The regional WRF-Chem model was used to study aerosol particles from biomass burning in South America. The modelled estimates of fire plume injection heights were found to be too high, with serious implications for modelled aerosol vertical distribution, transport and impacts on local climate. A modified emission scenario was developed which improved the predicted injection height. Model results were compared and evaluated against in situ measurements from the 2012 SAMBBA flight campaign.
H.-J. Tong, B. Ouyang, N. Nikolovski, D. M. Lienhard, F. D. Pope, and M. Kalberer
Atmos. Meas. Tech., 8, 1183–1195, https://doi.org/10.5194/amt-8-1183-2015, https://doi.org/10.5194/amt-8-1183-2015, 2015
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This paper describes a newly designed cold electrodynamic balance (EDB) which can be used to study the evaporation kinetics and freezing properties of aerosols at temperatures down to -40˚C. The abilities of the new EDB are exemplified through the study of the immersion freezing properties of water droplets containing extracts of water birch pollen (Betula fontinalis occidentalis). Protein-rich pollen extracts are found to be significantly more ice-active than non-proteinaceous extracts.
D. E. Young, J. D. Allan, P. I. Williams, D. C. Green, R. M. Harrison, J. Yin, M. J. Flynn, M. W. Gallagher, and H. Coe
Atmos. Chem. Phys., 15, 2429–2443, https://doi.org/10.5194/acp-15-2429-2015, https://doi.org/10.5194/acp-15-2429-2015, 2015
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Two solid fuel organic aerosol (SFOA) factors, both associated with domestic space heating activities, were derived from positive matrix factorisation (PMF) applied to organic aerosol data from an aerosol mass spectrometer (AMS) deployed at an urban background site in London during winter 2012. The factors controlling the split between the two SFOA factors were assessed, and it is concluded the split is likely governed predominantly by differences in burn conditions.
J. Yin, S. A. Cumberland, R. M. Harrison, J. Allan, D. E. Young, P. I. Williams, and H. Coe
Atmos. Chem. Phys., 15, 2139–2158, https://doi.org/10.5194/acp-15-2139-2015, https://doi.org/10.5194/acp-15-2139-2015, 2015
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Breathing particles from polluted air is known to cause increased health complaints and higher death rates. Airborne particles come from a range of sources; in order to implement cost-effective control measures, it is necessary to understand the amount contributed by each. In this paper, two advanced procedures for estimating the contributions of particle sources in London are compared with one another, revealing a wide range of sources including traffic, woodsmoke and cooking particles.
K. M. Sakamoto, J. D. Allan, H. Coe, J. W. Taylor, T. J. Duck, and J. R. Pierce
Atmos. Chem. Phys., 15, 1633–1646, https://doi.org/10.5194/acp-15-1633-2015, https://doi.org/10.5194/acp-15-1633-2015, 2015
D. Lowe, S. Archer-Nicholls, W. Morgan, J. Allan, S. Utembe, B. Ouyang, E. Aruffo, M. Le Breton, R. A. Zaveri, P. Di Carlo, C. Percival, H. Coe, R. Jones, and G. McFiggans
Atmos. Chem. Phys., 15, 1385–1409, https://doi.org/10.5194/acp-15-1385-2015, https://doi.org/10.5194/acp-15-1385-2015, 2015
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
W. T. Morgan, B. Ouyang, J. D. Allan, E. Aruffo, P. Di Carlo, O. J. Kennedy, D. Lowe, M. J. Flynn, P. D. Rosenberg, P. I. Williams, R. Jones, G. B. McFiggans, and H. Coe
Atmos. Chem. Phys., 15, 973–990, https://doi.org/10.5194/acp-15-973-2015, https://doi.org/10.5194/acp-15-973-2015, 2015
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This paper used observations from a research aircraft flying around the UK to investigate how air pollution in north-western Europe can alter nighttime chemical reactions in the atmosphere. These chemical reactions can worsen air quality in the region, as well as influence regional climate change. Ammonium nitrate aerosol appears to play an important role. The paper indicates that representation of these chemical reactions is poorly represented in models used for air quality and climate.
J. W. Taylor, J. D. Allan, G. Allen, H. Coe, P. I. Williams, M. J. Flynn, M. Le Breton, J. B. A. Muller, C. J. Percival, D. Oram, G. Forster, J. D. Lee, A. R. Rickard, M. Parrington, and P. I. Palmer
Atmos. Chem. Phys., 14, 13755–13771, https://doi.org/10.5194/acp-14-13755-2014, https://doi.org/10.5194/acp-14-13755-2014, 2014
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We present a case study of BC wet removal by examining aerosol properties in three biomass burning plumes, one of which passed through a precipitating cloud. Nucleation scavenging preferentially removed the largest and most coated BC-containing particles. Calculated single-scattering albedo (SSA) showed little variation, as a large number of non-BC particles were also present in the precipitation-affected plume.
U. R. Thorenz, L. J. Carpenter, R.-J. Huang, M. Kundel, J. Bosle, and T. Hoffmann
Atmos. Chem. Phys., 14, 13327–13335, https://doi.org/10.5194/acp-14-13327-2014, https://doi.org/10.5194/acp-14-13327-2014, 2014
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Phytoplankton suspensions were treated with high and low ozone levels, and volatile iodine (I2)-containing compounds were measured. Iodocarbon emissions were independent of the ozone level. I2 emission showed a strong dependency on the ozone level in the air as well as on the iodide concentration in the sample suspension. The experiments show that microalgae suspensions are capable of emitting I2 by the reaction of ozone with dissolved iodide at the air-water interface under natural conditions.
G. Allen, S. M. Illingworth, S. J. O'Shea, S. Newman, A. Vance, S. J.-B. Bauguitte, F. Marenco, J. Kent, K. Bower, M. W. Gallagher, J. Muller, C. J. Percival, C. Harlow, J. Lee, and J. P. Taylor
Atmos. Meas. Tech., 7, 4401–4416, https://doi.org/10.5194/amt-7-4401-2014, https://doi.org/10.5194/amt-7-4401-2014, 2014
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This paper presents a validated method and data set for new retrievals of trace gas concentrations and temperature from the ARIES infrared spectrometer instrument on the UK Atmospheric Research Aircraft (www.faam.ac.uk). This new capability for the aircraft will allow new science to be done because of the way it can sense information about the atmosphere without having to physically pass through it (remote sensing). This will allow us to better understand the make-up of the lower atmosphere.
S. J. O'Shea, G. Allen, M. W. Gallagher, K. Bower, S. M. Illingworth, J. B. A. Muller, B. T. Jones, C. J. Percival, S. J-B. Bauguitte, M. Cain, N. Warwick, A. Quiquet, U. Skiba, J. Drewer, K. Dinsmore, E. G. Nisbet, D. Lowry, R. E. Fisher, J. L. France, M. Aurela, A. Lohila, G. Hayman, C. George, D. B. Clark, A. J. Manning, A. D. Friend, and J. Pyle
Atmos. Chem. Phys., 14, 13159–13174, https://doi.org/10.5194/acp-14-13159-2014, https://doi.org/10.5194/acp-14-13159-2014, 2014
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This paper presents airborne measurements of greenhouse gases collected in the European Arctic. Regional scale flux estimates for the northern Scandinavian wetlands are derived. These fluxes are found to be in excellent agreement with coincident surface measurements within the aircraft's sampling domain. This has allowed a significant low bias to be identified in two commonly used process-based land surface models.
K. P. Wyche, A. C. Ryan, C. N. Hewitt, M. R. Alfarra, G. McFiggans, T. Carr, P. S. Monks, K. L. Smallbone, G. Capes, J. F. Hamilton, T. A. M. Pugh, and A. R. MacKenzie
Atmos. Chem. Phys., 14, 12781–12801, https://doi.org/10.5194/acp-14-12781-2014, https://doi.org/10.5194/acp-14-12781-2014, 2014
J. Brito, L. V. Rizzo, W. T. Morgan, H. Coe, B. Johnson, J. Haywood, K. Longo, S. Freitas, M. O. Andreae, and P. Artaxo
Atmos. Chem. Phys., 14, 12069–12083, https://doi.org/10.5194/acp-14-12069-2014, https://doi.org/10.5194/acp-14-12069-2014, 2014
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This paper details the physical--chemical characteristics of aerosols in a region strongly impacted by biomass burning in the western part of the Brazilian Amazon region. For such, a large suite of state-of-the-art instruments for realtime analysis was deployed at a ground site. Among the key findings, we observe the strong prevalence of organic aerosols associated to fire emissions, with important climate effects, and indications of its very fast processing in the atmosphere.
S. Decesari, J. Allan, C. Plass-Duelmer, B. J. Williams, M. Paglione, M. C. Facchini, C. O'Dowd, R. M. Harrison, J. K. Gietl, H. Coe, L. Giulianelli, G. P. Gobbi, C. Lanconelli, C. Carbone, D. Worsnop, A. T. Lambe, A. T. Ahern, F. Moretti, E. Tagliavini, T. Elste, S. Gilge, Y. Zhang, and M. Dall'Osto
Atmos. Chem. Phys., 14, 12109–12132, https://doi.org/10.5194/acp-14-12109-2014, https://doi.org/10.5194/acp-14-12109-2014, 2014
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We made use of multiple spectrometric techniques for characterizing the aerosol chemical composition and mixing in the Po Valley in the summer.
The oxygenated organic aerosol (OOA) concentrations were correlated with simple tracers for recirculated planetary boundary layer air.
A full internal mixing between black carbon (BC) and the non-refractory aerosol components was never observed. Local sources in the Po Valley were responsible for the production of organic particles unmixed with BC.
J. D. Allan, W. T. Morgan, E. Darbyshire, M. J. Flynn, P. I. Williams, D. E. Oram, P. Artaxo, J. Brito, J. D. Lee, and H. Coe
Atmos. Chem. Phys., 14, 11393–11407, https://doi.org/10.5194/acp-14-11393-2014, https://doi.org/10.5194/acp-14-11393-2014, 2014
X. Wang, C. L. Heald, D. A. Ridley, J. P. Schwarz, J. R. Spackman, A. E. Perring, H. Coe, D. Liu, and A. D. Clarke
Atmos. Chem. Phys., 14, 10989–11010, https://doi.org/10.5194/acp-14-10989-2014, https://doi.org/10.5194/acp-14-10989-2014, 2014
D. Liu, J. D. Allan, D. E. Young, H. Coe, D. Beddows, Z. L. Fleming, M. J. Flynn, M. W. Gallagher, R. M. Harrison, J. Lee, A. S. H. Prevot, J. W. Taylor, J. Yin, P. I. Williams, and P. Zotter
Atmos. Chem. Phys., 14, 10061–10084, https://doi.org/10.5194/acp-14-10061-2014, https://doi.org/10.5194/acp-14-10061-2014, 2014
J. E. Franklin, J. R. Drummond, D. Griffin, J. R. Pierce, D. L. Waugh, P. I. Palmer, M. Parrington, J. D. Lee, A. C. Lewis, A. R. Rickard, J. W. Taylor, J. D. Allan, H. Coe, K. A. Walker, L. Chisholm, T. J. Duck, J. T. Hopper, Y. Blanchard, M. D. Gibson, K. R. Curry, K. M. Sakamoto, G. Lesins, L. Dan, J. Kliever, and A. Saha
Atmos. Chem. Phys., 14, 8449–8460, https://doi.org/10.5194/acp-14-8449-2014, https://doi.org/10.5194/acp-14-8449-2014, 2014
M. S. Mohd Nadzir, S. M. Phang, M. R. Abas, N. Abdul Rahman, A. Abu Samah, W. T. Sturges, D. E. Oram, G. P. Mills, E. C. Leedham, J. A. Pyle, N. R. P. Harris, A. D. Robinson, M. J. Ashfold, M. I. Mead, M. T. Latif, M. F. Khan, A. M. Amiruddin, N. Banan, and M. M. Hanafiah
Atmos. Chem. Phys., 14, 8137–8148, https://doi.org/10.5194/acp-14-8137-2014, https://doi.org/10.5194/acp-14-8137-2014, 2014
E. A. Marais, D. J. Jacob, A. Guenther, K. Chance, T. P. Kurosu, J. G. Murphy, C. E. Reeves, and H. O. T. Pye
Atmos. Chem. Phys., 14, 7693–7703, https://doi.org/10.5194/acp-14-7693-2014, https://doi.org/10.5194/acp-14-7693-2014, 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
R. T. Lidster, J. F. Hamilton, J. D. Lee, A. C. Lewis, J. R. Hopkins, S. Punjabi, A. R. Rickard, and J. C. Young
Atmos. Chem. Phys., 14, 6677–6693, https://doi.org/10.5194/acp-14-6677-2014, https://doi.org/10.5194/acp-14-6677-2014, 2014
S. M. MacDonald, J. C. Gómez Martín, R. Chance, S. Warriner, A. Saiz-Lopez, L. J. Carpenter, and J. M. C. Plane
Atmos. Chem. Phys., 14, 5841–5852, https://doi.org/10.5194/acp-14-5841-2014, https://doi.org/10.5194/acp-14-5841-2014, 2014
K. L. Pereira, J. F. Hamilton, A. R. Rickard, W. J. Bloss, M. S. Alam, M. Camredon, A. Muñoz, M. Vázquez, E. Borrás, and M. Ródenas
Atmos. Chem. Phys., 14, 5349–5368, https://doi.org/10.5194/acp-14-5349-2014, https://doi.org/10.5194/acp-14-5349-2014, 2014
A. Wisher, D. E. Oram, J. C. Laube, G. P. Mills, P. van Velthoven, A. Zahn, and C. A. M. Brenninkmeijer
Atmos. Chem. Phys., 14, 3557–3570, https://doi.org/10.5194/acp-14-3557-2014, https://doi.org/10.5194/acp-14-3557-2014, 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
I. Kourtchev, S. J. Fuller, C. Giorio, R. M. Healy, E. Wilson, I. O'Connor, J. C. Wenger, M. McLeod, J. Aalto, T. M. Ruuskanen, W. Maenhaut, R. Jones, D. S. Venables, J. R. Sodeau, M. Kulmala, and M. Kalberer
Atmos. Chem. Phys., 14, 2155–2167, https://doi.org/10.5194/acp-14-2155-2014, https://doi.org/10.5194/acp-14-2155-2014, 2014
S. J. O'Shea, G. Allen, M. W. Gallagher, S. J.-B. Bauguitte, S. M. Illingworth, M. Le Breton, J. B. A. Muller, C. J. Percival, A. T. Archibald, D. E. Oram, M. Parrington, P. I. Palmer, and A. C. Lewis
Atmos. Chem. Phys., 13, 12451–12467, https://doi.org/10.5194/acp-13-12451-2013, https://doi.org/10.5194/acp-13-12451-2013, 2013
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. R. Alfarra, N. Good, K. P. Wyche, J. F. Hamilton, P. S. Monks, A. C. Lewis, and G. McFiggans
Atmos. Chem. Phys., 13, 11769–11789, https://doi.org/10.5194/acp-13-11769-2013, https://doi.org/10.5194/acp-13-11769-2013, 2013
S. Bezantakos, K. Barmpounis, M. Giamarelou, E. Bossioli, M. Tombrou, N. Mihalopoulos, K. Eleftheriadis, J. Kalogiros, J. D. Allan, A. Bacak, C. J. Percival, H. Coe, and G. Biskos
Atmos. Chem. Phys., 13, 11595–11608, https://doi.org/10.5194/acp-13-11595-2013, https://doi.org/10.5194/acp-13-11595-2013, 2013
J. F. Hamilton, M. R. Alfarra, N. Robinson, M. W. Ward, A. C. Lewis, G. B. McFiggans, H. Coe, and J. D. Allan
Atmos. Chem. Phys., 13, 11295–11305, https://doi.org/10.5194/acp-13-11295-2013, https://doi.org/10.5194/acp-13-11295-2013, 2013
R. M. Varma, S. M. Ball, T. Brauers, H.-P. Dorn, U. Heitmann, R. L. Jones, U. Platt, D. Pöhler, A. A. Ruth, A. J. L. Shillings, J. Thieser, A. Wahner, and D. S. Venables
Atmos. Meas. Tech., 6, 3115–3130, https://doi.org/10.5194/amt-6-3115-2013, https://doi.org/10.5194/amt-6-3115-2013, 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
M. Le Breton, A. Bacak, J. B. A. Muller, S. J. O'Shea, P. Xiao, M. N. R. Ashfold, M. C. Cooke, R. Batt, D. E. Shallcross, D. E. Oram, G. Forster, S. J.-B. Bauguitte, P. I. Palmer, M. Parrington, A. C. Lewis, J. D. Lee, and C. J. Percival
Atmos. Chem. Phys., 13, 9217–9232, https://doi.org/10.5194/acp-13-9217-2013, https://doi.org/10.5194/acp-13-9217-2013, 2013
F. Ziska, B. Quack, K. Abrahamsson, S. D. Archer, E. Atlas, T. Bell, J. H. Butler, L. J. Carpenter, C. E. Jones, N. R. P. Harris, H. Hepach, K. G. Heumann, C. Hughes, J. Kuss, K. Krüger, P. Liss, R. M. Moore, A. Orlikowska, S. Raimund, C. E. Reeves, W. Reifenhäuser, A. D. Robinson, C. Schall, T. Tanhua, S. Tegtmeier, S. Turner, L. Wang, D. Wallace, J. Williams, H. Yamamoto, S. Yvon-Lewis, and Y. Yokouchi
Atmos. Chem. Phys., 13, 8915–8934, https://doi.org/10.5194/acp-13-8915-2013, https://doi.org/10.5194/acp-13-8915-2013, 2013
R. Saleh, C. J. Hennigan, G. R. McMeeking, W. K. Chuang, E. S. Robinson, H. Coe, N. M. Donahue, and A. L. Robinson
Atmos. Chem. Phys., 13, 7683–7693, https://doi.org/10.5194/acp-13-7683-2013, https://doi.org/10.5194/acp-13-7683-2013, 2013
V. V. Petrenko, P. Martinerie, P. Novelli, D. M. Etheridge, I. Levin, Z. Wang, T. Blunier, J. Chappellaz, J. Kaiser, P. Lang, L. P. Steele, S. Hammer, J. Mak, R. L. Langenfelds, J. Schwander, J. P. Severinghaus, E. Witrant, G. Petron, M. O. Battle, G. Forster, W. T. Sturges, J.-F. Lamarque, K. Steffen, and J. W. C. White
Atmos. Chem. Phys., 13, 7567–7585, https://doi.org/10.5194/acp-13-7567-2013, https://doi.org/10.5194/acp-13-7567-2013, 2013
M. Parrington, P. I. Palmer, A. C. Lewis, J. D. Lee, A. R. Rickard, P. Di Carlo, J. W. Taylor, J. R. Hopkins, S. Punjabi, D. E. Oram, G. Forster, E. Aruffo, S. J. Moller, S. J.-B. Bauguitte, J. D. Allan, H. Coe, and R. J. Leigh
Atmos. Chem. Phys., 13, 7321–7341, https://doi.org/10.5194/acp-13-7321-2013, https://doi.org/10.5194/acp-13-7321-2013, 2013
P. J. Connolly, G. Vaughan, P. Cook, G. Allen, H. Coe, T. W. Choularton, C. Dearden, and A. Hill
Atmos. Chem. Phys., 13, 7133–7152, https://doi.org/10.5194/acp-13-7133-2013, https://doi.org/10.5194/acp-13-7133-2013, 2013
P. I. Palmer, M. Parrington, J. D. Lee, A. C. Lewis, A. R. Rickard, P. F. Bernath, T. J. Duck, D. L. Waugh, D. W. Tarasick, S. Andrews, E. Aruffo, L. J. Bailey, E. Barrett, S. J.-B. Bauguitte, K. R. Curry, P. Di Carlo, L. Chisholm, L. Dan, G. Forster, J. E. Franklin, M. D. Gibson, D. Griffin, D. Helmig, J. R. Hopkins, J. T. Hopper, M. E. Jenkin, D. Kindred, J. Kliever, M. Le Breton, S. Matthiesen, M. Maurice, S. Moller, D. P. Moore, D. E. Oram, S. J. O'Shea, R. C. Owen, C. M. L. S. Pagniello, S. Pawson, C. J. Percival, J. R. Pierce, S. Punjabi, R. M. Purvis, J. J. Remedios, K. M. Rotermund, K. M. Sakamoto, A. M. da Silva, K. B. Strawbridge, K. Strong, J. Taylor, R. Trigwell, K. A. Tereszchuk, K. A. Walker, D. Weaver, C. Whaley, and J. C. Young
Atmos. Chem. Phys., 13, 6239–6261, https://doi.org/10.5194/acp-13-6239-2013, https://doi.org/10.5194/acp-13-6239-2013, 2013
M. J. Newland, C. E. Reeves, D. E. Oram, J. C. Laube, W. T. Sturges, C. Hogan, P. Begley, and P. J. Fraser
Atmos. Chem. Phys., 13, 5551–5565, https://doi.org/10.5194/acp-13-5551-2013, https://doi.org/10.5194/acp-13-5551-2013, 2013
C. L. Reddington, G. McMeeking, G. W. Mann, H. Coe, M. G. Frontoso, D. Liu, M. Flynn, D. V. Spracklen, and K. S. Carslaw
Atmos. Chem. Phys., 13, 4917–4939, https://doi.org/10.5194/acp-13-4917-2013, https://doi.org/10.5194/acp-13-4917-2013, 2013
S. J. O'Shea, S. J.-B. Bauguitte, M. W. Gallagher, D. Lowry, and C. J. Percival
Atmos. Meas. Tech., 6, 1095–1109, https://doi.org/10.5194/amt-6-1095-2013, https://doi.org/10.5194/amt-6-1095-2013, 2013
H.-P. Dorn, R. L. Apodaca, S. M. Ball, T. Brauers, S. S. Brown, J. N. Crowley, W. P. Dubé, H. Fuchs, R. Häseler, U. Heitmann, R. L. Jones, A. Kiendler-Scharr, I. Labazan, J. M. Langridge, J. Meinen, T. F. Mentel, U. Platt, D. Pöhler, F. Rohrer, A. A. Ruth, E. Schlosser, G. Schuster, A. J. L. Shillings, W. R. Simpson, J. Thieser, R. Tillmann, R. Varma, D. S. Venables, and A. Wahner
Atmos. Meas. Tech., 6, 1111–1140, https://doi.org/10.5194/amt-6-1111-2013, https://doi.org/10.5194/amt-6-1111-2013, 2013
P. Di Carlo, E. Aruffo, M. Busilacchio, F. Giammaria, C. Dari-Salisburgo, F. Biancofiore, G. Visconti, J. Lee, S. Moller, C. E. Reeves, S. Bauguitte, G. Forster, R. L. Jones, and B. Ouyang
Atmos. Meas. Tech., 6, 971–980, https://doi.org/10.5194/amt-6-971-2013, https://doi.org/10.5194/amt-6-971-2013, 2013
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
D. Liu, J. Allan, J. Whitehead, D. Young, M. Flynn, H. Coe, G. McFiggans, Z. L. Fleming, and B. Bandy
Atmos. Chem. Phys., 13, 2015–2029, https://doi.org/10.5194/acp-13-2015-2013, https://doi.org/10.5194/acp-13-2015-2013, 2013
A. E. Jones, E. W. Wolff, N. Brough, S. J.-B. Bauguitte, R. Weller, M. Yela, M. Navarro-Comas, H. A. Ochoa, and N. Theys
Atmos. Chem. Phys., 13, 1457–1467, https://doi.org/10.5194/acp-13-1457-2013, https://doi.org/10.5194/acp-13-1457-2013, 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
M. Laborde, M. Schnaiter, C. Linke, H. Saathoff, K.-H. Naumann, O. Möhler, S. Berlenz, U. Wagner, J. W. Taylor, D. Liu, M. Flynn, J. D. Allan, H. Coe, K. Heimerl, F. Dahlkötter, B. Weinzierl, A. G. Wollny, M. Zanatta, J. Cozic, P. Laj, R. Hitzenberger, J. P. Schwarz, and M. Gysel
Atmos. Meas. Tech., 5, 3077–3097, https://doi.org/10.5194/amt-5-3077-2012, https://doi.org/10.5194/amt-5-3077-2012, 2012
T. Hamburger, G. McMeeking, A. Minikin, A. Petzold, H. Coe, and R. Krejci
Atmos. Chem. Phys., 12, 11533–11554, https://doi.org/10.5194/acp-12-11533-2012, https://doi.org/10.5194/acp-12-11533-2012, 2012
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Influence of aromatics on tropospheric gas-phase composition
Emission inventory of air pollutants and chemical speciation for specific anthropogenic sources based on local measurements in the Yangtze River Delta region, China
Photochemical environment over Southeast Asia primed for hazardous ozone levels with influx of nitrogen oxides from seasonal biomass burning
Atmospheric-methane source and sink sensitivity analysis using Gaussian process emulation
Carbon and air pollutant emissions from China's cement industry 1990–2015: trends, evolution of technologies, and drivers
Assessment of pre-industrial to present-day anthropogenic climate forcing in UKESM1
Technical note: A high-resolution inverse modelling technique for estimating surface CO2 fluxes based on the NIES-TM–FLEXPART coupled transport model and its adjoint
Improvement of the satellite-derived NOx emissions on air quality modeling and its effect on ozone and secondary inorganic aerosol formation in the Yangtze River Delta, China
Aircraft-based inversions quantify the importance of wetlands and livestock for Upper Midwest methane emissions
Time-resolved emission reductions for atmospheric chemistry modelling in Europe during the COVID-19 lockdowns
Rapid increase in summer surface ozone over the North China Plain during 2013–2019: a side effect of particulate matter reduction control?
Pan-Arctic surface ozone: modelling vs. measurements
Influence of aerosol copper on HO2 uptake: a novel parameterized equation
Role of ammonia in European air quality with changing land and ship emissions between 1990 and 2030
Revealing the sulfur dioxide emission reductions in China by assimilating surface observations in WRF-Chem
Discrepancies between MICS-Asia III simulation and observation for surface ozone in the marine atmosphere over the northwestern Pacific Asian Rim region
Correcting model biases of CO in East Asia: impact on oxidant distributions during KORUS-AQ
Quantifying the emission changes and associated air quality impacts during the COVID-19 pandemic on the North China Plain: a response modeling study
Do alternative inventories converge on the spatiotemporal representation of spring ammonia emissions in France?
Impacts of global NOx inversions on NO2 and ozone simulations
Reactive Organic Carbon Emissions from Volatile Chemical Products
Quantifying sources of Brazil's CH4 emissions between 2010 and 2018 from satellite data
On the role of trend and variability in the hydroxyl radical (OH) in the global methane budget
Trends in global tropospheric hydroxyl radical and methane lifetime since 1850 from AerChemMIP
Domenico Taraborrelli, David Cabrera-Perez, Sara Bacer, Sergey Gromov, Jos Lelieveld, Rolf Sander, and Andrea Pozzer
Atmos. Chem. Phys., 21, 2615–2636, https://doi.org/10.5194/acp-21-2615-2021, https://doi.org/10.5194/acp-21-2615-2021, 2021
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Atmospheric pollutants from anthropogenic activities and biomass burning are usually regarded as ozone precursors. Monocyclic aromatics are no exception. Calculations with a comprehensive atmospheric model are consistent with this view but only for air masses close to pollution source regions. However, the same model predicts that aromatics, when transported to remote areas, may effectively destroy ozone. This loss of tropospheric ozone rivals the one attributed to bromine.
Jingyu An, Yiwei Huang, Cheng Huang, Xin Wang, Rusha Yan, Qian Wang, Hongli Wang, Sheng'ao Jing, Yan Zhang, Yiming Liu, Yuan Chen, Chang Xu, Liping Qiao, Min Zhou, Shuhui Zhu, Qingyao Hu, Jun Lu, and Changhong Chen
Atmos. Chem. Phys., 21, 2003–2025, https://doi.org/10.5194/acp-21-2003-2021, https://doi.org/10.5194/acp-21-2003-2021, 2021
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This study established a 4 km × 4 km anthropogenic emission inventory in the Yangtze River Delta region, China, for 2017 based on locally measured emission factors and source profiles. There are high-intensity NOx and NMVOC species emissions in the eastern areas of the region. Toluene, 1,2,4-trimethylbenzene, m,p-xylene, propylene, ethylene, o-xylene, and OVOCs from industry and mobile sources have the highest comprehensive potentials for ozone and secondary organic aerosol formation.
Margaret R. Marvin, Paul I. Palmer, Barry G. Latter, Richard Siddans, Brian J. Kerridge, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 21, 1917–1935, https://doi.org/10.5194/acp-21-1917-2021, https://doi.org/10.5194/acp-21-1917-2021, 2021
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We use an atmospheric chemistry model in combination with satellite and surface observations to investigate how biomass burning affects tropospheric ozone over Southeast Asia during its fire seasons. We find that nitrogen oxides from biomass burning were responsible for about 30 % of the regional ozone formation potential, and we estimate that ozone from biomass burning caused more than 400 excess premature deaths in Southeast Asia during the peak burning months of March and September 2014.
Angharad C. Stell, Luke M. Western, Tomás Sherwen, and Matthew Rigby
Atmos. Chem. Phys., 21, 1717–1736, https://doi.org/10.5194/acp-21-1717-2021, https://doi.org/10.5194/acp-21-1717-2021, 2021
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Although it is the second-most important greenhouse gas, our understanding of the atmospheric-methane budget is limited. The uncertainty highlights the need for new tools to investigate sources and sinks. Here, we use a Gaussian process emulator to efficiently approximate the response of atmospheric-methane observations to changes in the most uncertain emission or loss processes. With this new method, we rigorously quantify the sensitivity of atmospheric observations to budget uncertainties.
Jun Liu, Dan Tong, Yixuan Zheng, Jing Cheng, Xinying Qin, Qinren Shi, Liu Yan, Yu Lei, and Qiang Zhang
Atmos. Chem. Phys., 21, 1627–1647, https://doi.org/10.5194/acp-21-1627-2021, https://doi.org/10.5194/acp-21-1627-2021, 2021
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In this study, we investigated the decadal changes in carbon dioxide and air pollutant emissions in China's cement industry for the period 1990–2015 based on intensive unit-based information. We found that from 1990 to 2015, accompanied by a 10.3-fold increase in cement production, CO2, SO2, and NOx emissions from China's cement industry increased by 627 %, 56 %, and 659 %, whereas CO, PM2.5, and PM10 emissions decreased by 9 %, 63 %, and 59 %, respectively.
Fiona M. O'Connor, N. Luke Abraham, Mohit Dalvi, Gerd A. Folberth, Paul T. Griffiths, Catherine Hardacre, Ben T. Johnson, Ron Kahana, James Keeble, Byeonghyeon Kim, Olaf Morgenstern, Jane P. Mulcahy, Mark Richardson, Eddy Robertson, Jeongbyn Seo, Sungbo Shim, João C. Teixeira, Steven T. Turnock, Jonny Williams, Andrew J. Wiltshire, Stephanie Woodward, and Guang Zeng
Atmos. Chem. Phys., 21, 1211–1243, https://doi.org/10.5194/acp-21-1211-2021, https://doi.org/10.5194/acp-21-1211-2021, 2021
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This paper calculates how changes in emissions and/or concentrations of different atmospheric constituents since the pre-industrial era have altered the Earth's energy budget at the present day using a metric called effective radiative forcing. The impact of land use change is also assessed. We find that individual contributions do not add linearly, and different Earth system interactions can affect the magnitude of the calculated effective radiative forcing.
Shamil Maksyutov, Tomohiro Oda, Makoto Saito, Rajesh Janardanan, Dmitry Belikov, Johannes W. Kaiser, Ruslan Zhuravlev, Alexander Ganshin, Vinu K. Valsala, Arlyn Andrews, Lukasz Chmura, Edward Dlugokencky, László Haszpra, Ray L. Langenfelds, Toshinobu Machida, Takakiyo Nakazawa, Michel Ramonet, Colm Sweeney, and Douglas Worthy
Atmos. Chem. Phys., 21, 1245–1266, https://doi.org/10.5194/acp-21-1245-2021, https://doi.org/10.5194/acp-21-1245-2021, 2021
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In order to improve the top-down estimation of the anthropogenic greenhouse gas emissions, a high-resolution inverse modelling technique was developed for applications to global transport modelling of carbon dioxide and other greenhouse gases. A coupled Eulerian–Lagrangian transport model and its adjoint are combined with surface fluxes at 0.1° resolution to provide high-resolution forward simulation and inverse modelling of surface fluxes accounting for signals from emission hot spots.
Yang Yang, Yu Zhao, Lei Zhang, Jie Zhang, Xin Huang, Xuefen Zhao, Yan Zhang, Mengxiao Xi, and Yi Lu
Atmos. Chem. Phys., 21, 1191–1209, https://doi.org/10.5194/acp-21-1191-2021, https://doi.org/10.5194/acp-21-1191-2021, 2021
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We conducted new NOx emission estimation based on the satellite-derived NO2 column constraint and found reduced emissions compared to previous estimates for a developed region in east China. The subsequent improvement in air quality modeling was demonstrated based on available ground observations. With multiple emission reduction cases for various pollutants, we explored the effective control approaches for ozone and inorganic aerosol pollution.
Xueying Yu, Dylan B. Millet, Kelley C. Wells, Daven K. Henze, Hansen Cao, Timothy J. Griffis, Eric A. Kort, Genevieve Plant, Malte J. Deventer, Randall K. Kolka, D. Tyler Roman, Kenneth J. Davis, Ankur R. Desai, Bianca C. Baier, Kathryn McKain, Alan C. Czarnetzki, and A. Anthony Bloom
Atmos. Chem. Phys., 21, 951–971, https://doi.org/10.5194/acp-21-951-2021, https://doi.org/10.5194/acp-21-951-2021, 2021
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Methane concentrations have doubled since 1750. The US Upper Midwest is a key region contributing to such trends, but sources are poorly understood. We collected and analyzed aircraft data to resolve spatial and timing biases in wetland and livestock emission estimates and uncover errors in inventory treatment of manure management. We highlight the importance of intensive agriculture for the regional and US methane budgets and the potential for methane mitigation through improved management.
Marc Guevara, Oriol Jorba, Albert Soret, Hervé Petetin, Dene Bowdalo, Kim Serradell, Carles Tena, Hugo Denier van der Gon, Jeroen Kuenen, Vincent-Henri Peuch, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 21, 773–797, https://doi.org/10.5194/acp-21-773-2021, https://doi.org/10.5194/acp-21-773-2021, 2021
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Most European countries have imposed lockdowns to combat the spread of the COVID-19 pandemic. Such a socioeconomic disruption has resulted in a sudden drop of atmospheric emissions and air pollution levels. This study quantifies the daily reductions in national emissions and associated levels of nitrogen dioxide (NO2) due to the COVID-19 lockdowns in Europe, by making use of multiple open-access measured activity data as well as artificial intelligence and modelling techniques.
Xiaodan Ma, Jianping Huang, Tianliang Zhao, Cheng Liu, Kaihui Zhao, Jia Xing, and Wei Xiao
Atmos. Chem. Phys., 21, 1–16, https://doi.org/10.5194/acp-21-1-2021, https://doi.org/10.5194/acp-21-1-2021, 2021
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The present work aims at identifying and quantifying the relative contributions of the key factors in driving a rapid increase in summertime surface O3 over the North China Plain during 2013–2019. In addition to anthropogenic emission reduction and meteorological variabilities, our study highlights the importance of inclusion of aerosol absorption and scattering properties rather than aerosol abundance only in accurate assessment of aerosol radiative effect on surface O3 formation and change.
Xin Yang, Anne-M. Blechschmidt, Kristof Bognar, Audra McClure-Begley, Sara Morris, Irina Petropavlovskikh, Andreas Richter, Henrik Skov, Kimberly Strong, David W. Tarasick, Taneil Uttal, Mika Vestenius, and Xiaoyi Zhao
Atmos. Chem. Phys., 20, 15937–15967, https://doi.org/10.5194/acp-20-15937-2020, https://doi.org/10.5194/acp-20-15937-2020, 2020
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This is a modelling-based study on Arctic surface ozone, with a particular focus on spring ozone depletion events (i.e. with concentrations < 10 ppbv). Model experiments show that model runs with blowing-snow-sourced sea salt aerosols implemented as a source of reactive bromine can reproduce well large-scale ozone depletion events observed in the Arctic. This study supplies modelling evidence of the proposed mechanism of reactive-bromine release from blowing snow on sea ice (Yang et al., 2008).
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.
Sebnem Aksoyoglu, Jianhui Jiang, Giancarlo Ciarelli, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 15665–15680, https://doi.org/10.5194/acp-20-15665-2020, https://doi.org/10.5194/acp-20-15665-2020, 2020
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We investigated the role of ammonia in European air quality between 1990 and 2030 under varying land and ship emissions. If ship emissions will be regulated more strictly in the future, particulate nitrate will decrease in coastal areas in northern Europe, while sulfate aerosol will decrease in the Mediterranean region. We predict a shift in the sensitivity of aerosol formation from NH3 towards NOx emissions between 1990 and 2030 in most of Europe except the eastern part of the model domain.
Tie Dai, Yueming Cheng, Daisuke Goto, Yingruo Li, Xiao Tang, Guangyu Shi, and Teruyuki Nakajima
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1259, https://doi.org/10.5194/acp-2020-1259, 2020
Revised manuscript accepted for ACP
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The anthropogenic emission of the sulfur dioxide (SO2) over China has significantly declined as the consequence of clean air actions. We have developed a new emission inversion system to dynamically update the SO2 emission grid by grid over China by assimilating the ground-based SO2 observations. The inverted SO2 emission over China in November 2016 on average has declined by 49.4 % since 2010, which is well agreement with the
bottom-upestimation of 48.0 %.
Hajime Akimoto, Tatsuya Nagashima, Natsumi Kawano, Li Jie, Joshua S. Fu, and Zifa Wang
Atmos. Chem. Phys., 20, 15003–15014, https://doi.org/10.5194/acp-20-15003-2020, https://doi.org/10.5194/acp-20-15003-2020, 2020
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In order to perform proper model simulation of ozone near the ground in the coastal area of northeastern Asia, it has been found that it is very important to select appropriate dry deposition velocities of ozone on the oceanic water of specific area of the northwestern Pacific. Empirical measurement of the mixing ratios and dry deposition flux of ozone over the ocean in this area is highly recommended.
Benjamin Gaubert, Louisa K. Emmons, Kevin Raeder, Simone Tilmes, Kazuyuki Miyazaki, Avelino F. Arellano Jr., Nellie Elguindi, Claire Granier, Wenfu Tang, Jérôme Barré, Helen M. Worden, Rebecca R. Buchholz, David P. Edwards, Philipp Franke, Jeffrey L. Anderson, Marielle Saunois, Jason Schroeder, Jung-Hun Woo, Isobel J. Simpson, Donald R. Blake, Simone Meinardi, Paul O. Wennberg, John Crounse, Alex Teng, Michelle Kim, Russell R. Dickerson, Hao He, Xinrong Ren, Sally E. Pusede, and Glenn S. Diskin
Atmos. Chem. Phys., 20, 14617–14647, https://doi.org/10.5194/acp-20-14617-2020, https://doi.org/10.5194/acp-20-14617-2020, 2020
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This study investigates carbon monoxide pollution in East Asia during spring using a numerical model, satellite remote sensing, and aircraft measurements. We found an underestimation of emission sources. Correcting the emission bias can improve air quality forecasting of carbon monoxide and other species including ozone. Results also suggest that controlling VOC and CO emissions, in addition to widespread NOx controls, can improve ozone pollution over East Asia.
Jia Xing, Siwei Li, Yueqi Jiang, Shuxiao Wang, Dian Ding, Zhaoxin Dong, Yun Zhu, and Jiming Hao
Atmos. Chem. Phys., 20, 14347–14359, https://doi.org/10.5194/acp-20-14347-2020, https://doi.org/10.5194/acp-20-14347-2020, 2020
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Quantifying emission changes is a prerequisite for assessment of control effectiveness in improving air quality. However, traditional bottom-up methods usually take months to perform and limit timely assessments. A novel method was developed by using a response model that provides real-time estimation of emission changes based on air quality observations. It was successfully applied to quantify emission changes on the North China Plain due to the COVID-19 pandemic shutdown.
Audrey Fortems-Cheiney, Gaëlle Dufour, Karine Dufossé, Florian Couvidat, Jean-Marc Gilliot, Guillaume Siour, Matthias Beekmann, Gilles Foret, Frederik Meleux, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, Cathy Clerbaux, and Sophie Génermont
Atmos. Chem. Phys., 20, 13481–13495, https://doi.org/10.5194/acp-20-13481-2020, https://doi.org/10.5194/acp-20-13481-2020, 2020
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Studies have suggested the importance of ammonia emissions on pollution particle formation over Europe, whose main atmospheric source is agriculture. In this study, we performed an inter-comparison of two alternative inventories, both with a reference inventory, that quantify the French ammonia emissions during spring 2011. Over regions with large mineral fertilizer use, like over northeastern France, NH3 emissions are probably considerably underestimated by the reference inventory.
Zhen Qu, Daven K. Henze, Owen R. Cooper, and Jessica L. Neu
Atmos. Chem. Phys., 20, 13109–13130, https://doi.org/10.5194/acp-20-13109-2020, https://doi.org/10.5194/acp-20-13109-2020, 2020
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We use satellite observations and chemical transport modeling to quantify sources of NOx, a major air pollutant, over the past decade. We find improved simulations of the magnitude, seasonality, and trends of NO2 and ozone concentrations using these derived emissions. Changes in ozone pollution driven by human and natural sources are identified in different regions. This work shows the benefits of remote-sensing data and inverse modeling for more accurate ozone simulations.
Karl M. Seltzer, Elyse Pennington, Venkatesh Rao, Benjamin N. Murphy, Madeleine Strum, Kristin K. Isaacs, and Havala O. T. Pye
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1111, https://doi.org/10.5194/acp-2020-1111, 2020
Revised manuscript accepted for ACP
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Volatile chemical products (VCPs) are an increasingly important source of anthropogenic reactive organic carbon emissions. Here, we develop VCPy, a new framework to model organic emissions from VCPs throughout the United States. At the national-level, VCPy emissions are broadly consistent with the US EPA's 2017 National Emission Inventory, however county-level and categorical estimates can differ substantially. An observational evaluation indicates high fidelity in the methods employed here.
Rachel L. Tunnicliffe, Anita L. Ganesan, Robert J. Parker, Hartmut Boesch, Nicola Gedney, Benjamin Poulter, Zhen Zhang, Jošt V. Lavrič, David Walter, Matthew Rigby, Stephan Henne, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 20, 13041–13067, https://doi.org/10.5194/acp-20-13041-2020, https://doi.org/10.5194/acp-20-13041-2020, 2020
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This study quantifies Brazil’s emissions of a potent atmospheric greenhouse gas, methane. This is in the field of atmospheric modelling and uses remotely sensed data and surface measurements of methane concentrations as well as an atmospheric transport model to interpret the data. Because of Brazil’s large emissions from wetlands, agriculture and biomass burning, these emissions affect global methane concentrations and thus are of global significance.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 20, 13011–13022, https://doi.org/10.5194/acp-20-13011-2020, https://doi.org/10.5194/acp-20-13011-2020, 2020
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Decadal trends and variations in OH are critical for understanding atmospheric CH4 evolution. We quantify the impacts of OH trends and variations on the CH4 budget by conducting CH4 inversions on a decadal scale with an ensemble of OH fields. We find the negative OH anomalies due to enhanced fires can reduce the optimized CH4 emissions by up to 10 Tg yr−1 during El Niño years and the positive OH trend from 1986 to 2010 results in a ∼ 23 Tg yr−1 additional increase in optimized CH4 emissions.
David S. Stevenson, Alcide Zhao, Vaishali Naik, Fiona M. O'Connor, Simone Tilmes, Guang Zeng, Lee T. Murray, William J. Collins, Paul T. Griffiths, Sungbo Shim, Larry W. Horowitz, Lori T. Sentman, and Louisa Emmons
Atmos. Chem. Phys., 20, 12905–12920, https://doi.org/10.5194/acp-20-12905-2020, https://doi.org/10.5194/acp-20-12905-2020, 2020
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We present historical trends in atmospheric oxidizing capacity (OC) since 1850 from the latest generation of global climate models and compare these with estimates from measurements. OC controls levels of many key reactive gases, including methane (CH4). We find small model trends up to 1980, then increases of about 9 % up to 2014, disagreeing with (uncertain) measurement-based trends. Major drivers of OC trends are emissions of CH4, NOx, and CO; these will be important for future CH4 trends.