Articles | Volume 17, issue 18
https://doi.org/10.5194/acp-17-11623-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-17-11623-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
28 Sep 2017
Research article |
| 28 Sep 2017
Atmospheric mercury in the Southern Hemisphere tropics: seasonal and diurnal variations and influence of inter-hemispheric transport
Dean Howard
CORRESPONDING AUTHOR
Department of Environmental Sciences, Macquarie University, Sydney, New South Wales, 2109, Australia
Peter F. Nelson
Department of Environmental Sciences, Macquarie University, Sydney, New South Wales, 2109, Australia
Grant C. Edwards
Department of Environmental Sciences, Macquarie University, Sydney, New South Wales, 2109, Australia
Anthony L. Morrison
Department of Environmental Sciences, Macquarie University, Sydney, New South Wales, 2109, Australia
Jenny A. Fisher
Centre for Atmospheric Chemistry, School of Chemistry, University of Wollongong, Wollongong, New South Wales, 2552, Australia
School of Earth & Environmental Sciences, University of Wollongong, Wollongong, New South Wales, 2552, Australia
Jason Ward
Oceans and Atmosphere Flagship, Commonwealth Science and Industrial Research Organisation, Aspendale, Victoria, 3195, Australia
James Harnwell
Oceans and Atmosphere Flagship, Commonwealth Science and Industrial Research Organisation, Aspendale, Victoria, 3195, Australia
Marcel van der Schoot
Oceans and Atmosphere Flagship, Commonwealth Science and Industrial Research Organisation, Aspendale, Victoria, 3195, Australia
Brad Atkinson
Darwin Research Station, Bureau of Meteorology, Darwin, Northern Territory, 0810, Australia
Scott D. Chambers
Institute for Environmental Research, Australian Nuclear Science and Technology Organisation, Sydney, New South Wales, 2232, Australia
Alan D. Griffiths
Institute for Environmental Research, Australian Nuclear Science and Technology Organisation, Sydney, New South Wales, 2232, Australia
Sylvester Werczynski
Institute for Environmental Research, Australian Nuclear Science and Technology Organisation, Sydney, New South Wales, 2232, Australia
Alastair G. Williams
Institute for Environmental Research, Australian Nuclear Science and Technology Organisation, Sydney, New South Wales, 2232, Australia
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Ruhi S. Humphries, Melita D. Keywood, Jason P. Ward, James Harnwell, Simon P. Alexander, Andrew R. Klekociuk, Keiichiro Hara, Ian M. McRobert, Alain Protat, Joel Alroe, Luke T. Cravigan, Branka Miljevic, Zoran D. Ristovski, Robyn Schofield, Stephen R. Wilson, Connor J. Flynn, Gourihar R. Kulkarni, Gerald G. Mace, Greg M. McFarquhar, Scott D. Chambers, Alastair G. Williams, and Alan D. Griffiths
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Maria Paula Pérez-Peña, Jenny A. Fisher, Dylan B. Millet, Hisashi Yashiro, Ray L. Langenfelds, Paul B. Krummel, and Scott H. Kable
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Jack B. Simmons, Ruhi S. Humphries, Stephen R. Wilson, Scott D. Chambers, Alastair G. Williams, Alan D. Griffiths, Ian M. McRobert, Jason P. Ward, Melita D. Keywood, and Sean Gribben
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Joel Alroe, Luke T. Cravigan, Branka Miljevic, Graham R. Johnson, Paul Selleck, Ruhi S. Humphries, Melita D. Keywood, Scott D. Chambers, Alastair G. Williams, and Zoran D. Ristovski
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Claudia Grossi, Scott D. Chambers, Olivier Llido, Felix R. Vogel, Victor Kazan, Alessandro Capuana, Sylvester Werczynski, Roger Curcoll, Marc Delmotte, Arturo Vargas, Josep-Anton Morguí, Ingeborg Levin, and Michel Ramonet
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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.
Melita Keywood, Paul Selleck, Fabienne Reisen, David Cohen, Scott Chambers, Min Cheng, Martin Cope, Suzanne Crumeyrolle, Erin Dunne, Kathryn Emmerson, Rosemary Fedele, Ian Galbally, Rob Gillett, Alan Griffiths, Elise-Andree Guerette, James Harnwell, Ruhi Humphries, Sarah Lawson, Branka Miljevic, Suzie Molloy, Jennifer Powell, Jack Simmons, Zoran Ristovski, and Jason Ward
Earth Syst. Sci. Data, 11, 1883–1903, https://doi.org/10.5194/essd-11-1883-2019, https://doi.org/10.5194/essd-11-1883-2019, 2019
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Dafina Kikaj, Janja Vaupotič, and Scott D. Chambers
Atmos. Meas. Tech., 12, 4455–4477, https://doi.org/10.5194/amt-12-4455-2019, https://doi.org/10.5194/amt-12-4455-2019, 2019
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A new method was developed to identify persistent temperature inversion events in a subalpine basin using a radon-based method (RBM). By comparing with an existing pseudo-vertical temperature gradient method, the RBM was shown to be more reliable and seasonally independent. The RBM has the potential to increase the understanding of meteorological controls on air pollution episodes in complex terrain beyond the capability of contemporary atmospheric stability classification tools.
Ruhi S. Humphries, Ian M. McRobert, Will A. Ponsonby, Jason P. Ward, Melita D. Keywood, Zoe M. Loh, Paul B. Krummel, and James Harnwell
Atmos. Meas. Tech., 12, 3019–3038, https://doi.org/10.5194/amt-12-3019-2019, https://doi.org/10.5194/amt-12-3019-2019, 2019
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Undertaking atmospheric observations from ships provides important data in regions where measurements are impossible by other means. However, making measurements so close to a diesel exhaust plume is difficult. In this paper, we describe an algorithm that utilises ongoing measurements of aerosol number concentrations, black carbon mass concentrations, and mixing ratios of carbon monoxide and carbon dioxide to accurately distinguish between exhaust and background data periods.
Beata Bukosa, Nicholas M. Deutscher, Jenny A. Fisher, Dagmar Kubistin, Clare Paton-Walsh, and David W. T. Griffith
Atmos. Chem. Phys., 19, 7055–7072, https://doi.org/10.5194/acp-19-7055-2019, https://doi.org/10.5194/acp-19-7055-2019, 2019
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The carbon greenhouse gases (CO2, CH4 and CO) were proven to have a large impact on the global carbon cycle and our climate. To understand the variability of the carbon cycle and predict future climate change scenarios, we need to study the processes that drive the changes of these gases in the atmosphere. We study the sources and sinks of CO2, CH4 and CO with a combination of measurements and chemical transport modelling to identify missing, underestimated or overestimated sources in Australia.
Debra Wunch, Dylan B. A. Jones, Geoffrey C. Toon, Nicholas M. Deutscher, Frank Hase, Justus Notholt, Ralf Sussmann, Thorsten Warneke, Jeroen Kuenen, Hugo Denier van der Gon, Jenny A. Fisher, and Joannes D. Maasakkers
Atmos. Chem. Phys., 19, 3963–3980, https://doi.org/10.5194/acp-19-3963-2019, https://doi.org/10.5194/acp-19-3963-2019, 2019
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We used five atmospheric observatories in Europe measuring total column dry-air mole fractions of methane and carbon monoxide to infer methane emissions in the area between the observatories. We find that the methane emissions are overestimated by the state-of-the-art inventories, and that this is likely due, at least in part, to the inventory disaggregation. We find that there is significant uncertainty in the carbon monoxide inventories that requires further investigation.
Matthieu B. Miller, Sarrah M. Dunham-Cheatham, Mae Sexauer Gustin, and Grant C. Edwards
Atmos. Meas. Tech., 12, 1207–1217, https://doi.org/10.5194/amt-12-1207-2019, https://doi.org/10.5194/amt-12-1207-2019, 2019
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This study was undertaken to demonstrate that a cation exchange membrane (CEM) material used for sampling reactive mercury (RM) does not possess an inherent tendency to collect gaseous elemental mercury (GEM). Using a custom-built mercury vapor permeation system, we found that the CEM material has a very small GEM uptake of approximately 0.004 %, too small to create a significant artifact. We also found that a representative RM compound was collected by the CEM material with high efficiency.
Ann R. Stavert, Rachel M. Law, Marcel van der Schoot, Ray L. Langenfelds, Darren A. Spencer, Paul B. Krummel, Scott D. Chambers, Alistair G. Williams, Sylvester Werczynski, Roger J. Francey, and Russell T. Howden
Atmos. Meas. Tech., 12, 1103–1121, https://doi.org/10.5194/amt-12-1103-2019, https://doi.org/10.5194/amt-12-1103-2019, 2019
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The Southern Ocean is a key sink of carbon dioxide (CO2), but efforts to study trends in and the variability of the sink have been hindered by the limited number of CO2 measurements in this region. Here we describe a set of new in situ continuous (minutely) atmospheric CO2 observations. We show that this new record better captures long-term changes and seasonality than traditional 2-weekly flask records. As such, this data set will provide key insights into the changing Southern Ocean sink.
Matthieu B. Miller, Mae S. Gustin, and Grant C. Edwards
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2018-360, https://doi.org/10.5194/amt-2018-360, 2018
Revised manuscript not accepted
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In the atmosphere there are 2 gaseous forms of mercury (Hg), elemental (Hgo) and oxidized compounds (GOM). Hgo is oxidized by gases such as ozone and chlorine compounds. GOM is readily deposited to ecosystems and converted to methylmercury (a subtle neurotoxin). Here we explain development of a method for measurement of GOM deposition and emission associated with surfaces, and demonstrate that both occur. This has significant implications, because no one has been able to do this successfully.
Kathryn M. Emmerson, Martin E. Cope, Ian E. Galbally, Sunhee Lee, and Peter F. Nelson
Atmos. Chem. Phys., 18, 7539–7556, https://doi.org/10.5194/acp-18-7539-2018, https://doi.org/10.5194/acp-18-7539-2018, 2018
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We compare the CSIRO in-house biogenic emissions model (ABCGEM) with the Model of Emissions of Gases and Aerosols from Nature (MEGAN), for eucalypt-rich south-east Australia. Differences in emissions are not only due to the emission factors, but also how these emission factors are processed. ABCGEM assumes monoterpenes are not light dependent, whilst MEGAN does. Comparison with observations suggests that Australian monoterpenes may not be as light dependent as other vegetation globally.
David S. McLagan, Carl P. J. Mitchell, Alexandra Steffen, Hayley Hung, Cecilia Shin, Geoff W. Stupple, Mark L. Olson, Winston T. Luke, Paul Kelley, Dean Howard, Grant C. Edwards, Peter F. Nelson, Hang Xiao, Guey-Rong Sheu, Annekatrin Dreyer, Haiyong Huang, Batual Abdul Hussain, Ying D. Lei, Ilana Tavshunsky, and Frank Wania
Atmos. Chem. Phys., 18, 5905–5919, https://doi.org/10.5194/acp-18-5905-2018, https://doi.org/10.5194/acp-18-5905-2018, 2018
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A new passive air sampler for gaseous mercury was tested at 20 sites on four continents. These sites have in common that they use the state-of-the-art active air sampling technique for gaseous mercury on a continuous basis and therefore allow for an evaluation and calibration of the passive sampler. The sampler proved to work exceptionally well, with a precision and accuracy on par with the active
instrument and better than what has previously been achieved with passive samplers.
Jennifer Kaiser, Daniel J. Jacob, Lei Zhu, Katherine R. Travis, Jenny A. Fisher, Gonzalo González Abad, Lin Zhang, Xuesong Zhang, Alan Fried, John D. Crounse, Jason M. St. Clair, and Armin Wisthaler
Atmos. Chem. Phys., 18, 5483–5497, https://doi.org/10.5194/acp-18-5483-2018, https://doi.org/10.5194/acp-18-5483-2018, 2018
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Isoprene emissions from vegetation have a large effect on atmospheric chemistry and air quality. Here we use the adjoint of GEOS-Chem in an inversion of OMI formaldehyde observations to produce top-down estimates of isoprene emissions in the southeast US during the summer of 2013. We find that MEGAN v2.1 is biased high on average by 40 %. Our downward correction of isoprene emissions leads to a small reduction in modeled surface O3 and decreases the contribution of isoprene to organic aerosol.
Ashley M. Pierce, S. Marcela Loría-Salazar, W. Patrick Arnott, Grant C. Edwards, Matthieu B. Miller, and Mae S. Gustin
Atmos. Meas. Tech., 11, 2225–2237, https://doi.org/10.5194/amt-11-2225-2018, https://doi.org/10.5194/amt-11-2225-2018, 2018
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This paper investigates the possible sources of anomalous particulate matter collected at a high-elevation site during June to November 2014. Particles were collected on a sample filter that were > 2.5 µm in aerodynamic diameter, on a system that theoretically should not collect particulate matter that large. These samples indicated that either the observed particles had unique dimensions and behavior or that there was an issue with the particulate monitor inlet setup.
Dean Howard and Grant C. Edwards
Atmos. Chem. Phys., 18, 129–142, https://doi.org/10.5194/acp-18-129-2018, https://doi.org/10.5194/acp-18-129-2018, 2018
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Air–surface exchange of mercury is an important process for the movement of this toxic metal through the environment. This study presents observations of nocturnal depletion of atmospheric mercury, with surface deposition playing a large role. This deposited mercury is more labile, with up to ~17% re-released the following morning. This study is the first of its kind taken in Australia. Comparison with studies in the Northern Hemisphere shows reasonably good agreement for deposition velocities.
Marc D. Mallet, Maximilien J. Desservettaz, Branka Miljevic, Andelija Milic, Zoran D. Ristovski, Joel Alroe, Luke T. Cravigan, E. Rohan Jayaratne, Clare Paton-Walsh, David W. T. Griffith, Stephen R. Wilson, Graham Kettlewell, Marcel V. van der Schoot, Paul Selleck, Fabienne Reisen, Sarah J. Lawson, Jason Ward, James Harnwell, Min Cheng, Rob W. Gillett, Suzie B. Molloy, Dean Howard, Peter F. Nelson, Anthony L. Morrison, Grant C. Edwards, Alastair G. Williams, Scott D. Chambers, Sylvester Werczynski, Leah R. Williams, V. Holly L. Winton, Brad Atkinson, Xianyu Wang, and Melita D. Keywood
Atmos. Chem. Phys., 17, 13681–13697, https://doi.org/10.5194/acp-17-13681-2017, https://doi.org/10.5194/acp-17-13681-2017, 2017
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Fires play an important role within atmosphere. Gaseous and aerosol emissions influence Earth's temperature but these emissions can vary drastically across region and season. The SAFIRED (Savannah Fires in the Early Dry Season) campaign was undertaken at the Australian Tropical Research Station in north Australia during the 2014 early dry season. This paper presents an overview of the fires in this region, the measurements of their emissions and the implications of these fires on the atmosphere.
Jenny A. Fisher, Lee T. Murray, Dylan B. A. Jones, and Nicholas M. Deutscher
Geosci. Model Dev., 10, 4129–4144, https://doi.org/10.5194/gmd-10-4129-2017, https://doi.org/10.5194/gmd-10-4129-2017, 2017
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Carbon monoxide (CO) simulation in atmospheric chemistry models is used for source–receptor analysis, emission inversion, and interpretation of observations. We introduce a major update to CO simulation in the GEOS-Chem chemical transport model that removes fundamental inconsistencies relative to the standard model, resolving biases of more than 100 ppb and errors in vertical structure. We also add source tagging of secondary CO and demonstrate it provides added value in low-emission regions.
Jesse W. Greenslade, Simon P. Alexander, Robyn Schofield, Jenny A. Fisher, and Andrew K. Klekociuk
Atmos. Chem. Phys., 17, 10269–10290, https://doi.org/10.5194/acp-17-10269-2017, https://doi.org/10.5194/acp-17-10269-2017, 2017
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An analysis of data from ozonesondes released at three southern oceanic sites shows the impact of stratospheric ozone in this region. Using a novel method of transport classification, this work estimates the seasonality and quantity of stratospherically sourced ozone. We find that ozone is transported most frequently in summer due to regional-scale low-pressure weather systems. We also estimate a stratospheric ozone source of 2.0–3.3 Tg/year over three Southern Ocean regions.
Christopher Chan Miller, Daniel J. Jacob, Eloise A. Marais, Karen Yu, Katherine R. Travis, Patrick S. Kim, Jenny A. Fisher, Lei Zhu, Glenn M. Wolfe, Thomas F. Hanisco, Frank N. Keutsch, Jennifer Kaiser, Kyung-Eun Min, Steven S. Brown, Rebecca A. Washenfelder, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 17, 8725–8738, https://doi.org/10.5194/acp-17-8725-2017, https://doi.org/10.5194/acp-17-8725-2017, 2017
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The use of satellite glyoxal observations for estimating isoprene emissions has been limited by knowledge of the glyoxal yield from isoprene. We use SENEX aircraft observations over the southeast US to evaluate glyoxal yields from isoprene in a 3-D atmospheric model. The SENEX observations support a pathway for glyoxal formation in pristine regions that we propose here, which may have implications for improving isoprene emissions estimates from upcoming high-resolution geostationary satellites.
Pauline C. Treble, Andy Baker, Linda K. Ayliffe, Timothy J. Cohen, John C. Hellstrom, Michael K. Gagan, Silvia Frisia, Russell N. Drysdale, Alan D. Griffiths, and Andrea Borsato
Clim. Past, 13, 667–687, https://doi.org/10.5194/cp-13-667-2017, https://doi.org/10.5194/cp-13-667-2017, 2017
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Little is known about the climate of southern Australia during the Last Glacial Maximum and deglaciation owing to sparse records for this region. We present the first high-resolution data, derived from speleothems that grew 23–5 ka. It appears that recharge to the Flinders Ranges was higher than today, particularly during 18.9–15.8 ka, argued to be due to the enhanced availability of tropical moisture. An abrupt shift to aridity is recorded at 15.8 ka, associated with restored westerly airflow.
Clare Paton-Walsh, Élise-Andrée Guérette, Dagmar Kubistin, Ruhi Humphries, Stephen R. Wilson, Doreena Dominick, Ian Galbally, Rebecca Buchholz, Mahendra Bhujel, Scott Chambers, Min Cheng, Martin Cope, Perry Davy, Kathryn Emmerson, David W. T. Griffith, Alan Griffiths, Melita Keywood, Sarah Lawson, Suzie Molloy, Géraldine Rea, Paul Selleck, Xue Shi, Jack Simmons, and Voltaire Velazco
Earth Syst. Sci. Data, 9, 349–362, https://doi.org/10.5194/essd-9-349-2017, https://doi.org/10.5194/essd-9-349-2017, 2017
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The MUMBA campaign provides a detailed snapshot of the atmospheric composition in an urban coastal environment with strong biogenic sources nearby. This campaign involved collaboration between several institutes and was undertaken to provide a case study for atmospheric models in a poorly sampled region of the globe.
Dominik Schmithüsen, Scott Chambers, Bernd Fischer, Stefan Gilge, Juha Hatakka, Victor Kazan, Rolf Neubert, Jussi Paatero, Michel Ramonet, Clemens Schlosser, Sabine Schmid, Alex Vermeulen, and Ingeborg Levin
Atmos. Meas. Tech., 10, 1299–1312, https://doi.org/10.5194/amt-10-1299-2017, https://doi.org/10.5194/amt-10-1299-2017, 2017
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A European-wide 222radon/222radon progeny comparison study has been conducted at nine measurement stations in order to determine differences between existing 222radon instrumentation and atmospheric data sets, respectively. Mean differences up to 45 % were found between monitors. These differences need to be taken into account if the data shall serve for quantitative regional atmospheric transport model validation.
Andelija Milic, Marc D. Mallet, Luke T. Cravigan, Joel Alroe, Zoran D. Ristovski, Paul Selleck, Sarah J. Lawson, Jason Ward, Maximilien J. Desservettaz, Clare Paton-Walsh, Leah R. Williams, Melita D. Keywood, and Branka Miljevic
Atmos. Chem. Phys., 17, 3945–3961, https://doi.org/10.5194/acp-17-3945-2017, https://doi.org/10.5194/acp-17-3945-2017, 2017
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This study reports chemical characterization of fresh and processed aerosols sampled over a month-long field campaign, during the intense fire period in Australian tropical savannah region. The study illustrates diversity in fire emissions and importance of processed fire emissions and formation of secondary species, including biogenic secondary species, in northern Australia.
Marc D. Mallet, Luke T. Cravigan, Andelija Milic, Joel Alroe, Zoran D. Ristovski, Jason Ward, Melita Keywood, Leah R. Williams, Paul Selleck, and Branka Miljevic
Atmos. Chem. Phys., 17, 3605–3617, https://doi.org/10.5194/acp-17-3605-2017, https://doi.org/10.5194/acp-17-3605-2017, 2017
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This paper presents data on the size, composition and concentration of aerosol particles emitted from north Australian savannah fires and how these properties influence cloud condensation nuclei (CCN) concentrations. Both the size and composition of aerosol were found to be important in determining CCN. Despite large CCNc enhancements during periods of close biomass burning, the aerosol was very weakly hygroscopic which should be accounted for in climate models to avoid large CCNc overestimates.
Stephen D. Parkes, Matthew F. McCabe, Alan D. Griffiths, Lixin Wang, Scott Chambers, Ali Ershadi, Alastair G. Williams, Josiah Strauss, and Adrian Element
Hydrol. Earth Syst. Sci., 21, 533–548, https://doi.org/10.5194/hess-21-533-2017, https://doi.org/10.5194/hess-21-533-2017, 2017
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Determining atmospheric moisture sources is required for understanding the water cycle. The role of land surface fluxes is a particular source of uncertainty for moisture budgets. Water vapour isotopes have the potential to improve constraints on moisture sources. In this work relationships between water vapour isotopes and land–atmosphere exchange are studied. Results show that land surface evaporative fluxes play a minor role in the daytime water and isotope budgets in semi-arid environments.
Katherine R. Travis, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Lei Zhu, Karen Yu, Christopher C. Miller, Robert M. Yantosca, Melissa P. Sulprizio, Anne M. Thompson, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Ronald C. Cohen, Joshua L. Laughner, Jack E. Dibb, Samuel R. Hall, Kirk Ullmann, Glenn M. Wolfe, Illana B. Pollack, Jeff Peischl, Jonathan A. Neuman, and Xianliang Zhou
Atmos. Chem. Phys., 16, 13561–13577, https://doi.org/10.5194/acp-16-13561-2016, https://doi.org/10.5194/acp-16-13561-2016, 2016
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Ground-level ozone pollution in the Southeast US involves complex chemistry driven by anthropogenic emissions of nitrogen oxides (NOx) and biogenic emissions of isoprene. We find that US NOx emissions are overestimated nationally by as much as 50 % and that reducing model emissions by this amount results in good agreement with SEAC4RS aircraft measurements in August and September 2013. Observations of nitrate wet deposition fluxes and satellite NO2 columns further support this result.
Lei Zhu, Daniel J. Jacob, Patrick S. Kim, Jenny A. Fisher, Karen Yu, Katherine R. Travis, Loretta J. Mickley, Robert M. Yantosca, Melissa P. Sulprizio, Isabelle De Smedt, Gonzalo González Abad, Kelly Chance, Can Li, Richard Ferrare, Alan Fried, Johnathan W. Hair, Thomas F. Hanisco, Dirk Richter, Amy Jo Scarino, James Walega, Petter Weibring, and Glenn M. Wolfe
Atmos. Chem. Phys., 16, 13477–13490, https://doi.org/10.5194/acp-16-13477-2016, https://doi.org/10.5194/acp-16-13477-2016, 2016
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HCHO column data are widely used as a proxy for VOCs emissions, but validation of the data has been extremely limited. We use accurate aircraft observations to validate and intercompare 6 HCHO retrievals with GEOS-Chem as the intercomparison platform. Retrievals are interconsistent in spatial variability over the SE US and in daily variability, but are biased low by 20–51 %. Our work supports the use of HCHO column as a quantitative proxy for isoprene emission after correction of the low bias.
V. Holly L. Winton, Ross Edwards, Andrew R. Bowie, Melita Keywood, Alistair G. Williams, Scott D. Chambers, Paul W. Selleck, Maximilien Desservettaz, Marc D. Mallet, and Clare Paton-Walsh
Atmos. Chem. Phys., 16, 12829–12848, https://doi.org/10.5194/acp-16-12829-2016, https://doi.org/10.5194/acp-16-12829-2016, 2016
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The deposition of soluble aerosol iron (Fe) can initiate nitrogen fixation and trigger toxic algal blooms in nitrate-poor tropical waters. We present dry season soluble Fe data from northern Australia that reflect coincident dust and biomass burning sources of soluble Fe. Our results show that while biomass burning species are not a direct source of soluble Fe, biomass burning may substantially enhance the solubility of mineral dust with fractional Fe solubility up to 12 % in mixed aerosols.
E. N. Koffi, P. Bergamaschi, U. Karstens, M. Krol, A. Segers, M. Schmidt, I. Levin, A. T. Vermeulen, R. E. Fisher, V. Kazan, H. Klein Baltink, D. Lowry, G. Manca, H. A. J. Meijer, J. Moncrieff, S. Pal, M. Ramonet, H. A. Scheeren, and A. G. Williams
Geosci. Model Dev., 9, 3137–3160, https://doi.org/10.5194/gmd-9-3137-2016, https://doi.org/10.5194/gmd-9-3137-2016, 2016
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We evaluate the capability of the TM5 model to reproduce observations of the boundary layer dynamics and the associated variability of trace gases close to the surface, using 222Rn. Focusing on the European scale, we compare the TM5 boundary layer heights with observations from radiosondes, lidar, and ceilometer. Furthermore, we compare TM5 simulations of 222Rn activity concentrations, using a novel, process-based 222Rn flux map over Europe, with 222Rn harmonized measurements from 10 stations.
Alan D. Griffiths, Scott D. Chambers, Alastair G. Williams, and Sylvester Werczynski
Atmos. Meas. Tech., 9, 2689–2707, https://doi.org/10.5194/amt-9-2689-2016, https://doi.org/10.5194/amt-9-2689-2016, 2016
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Surface-based two-filter radon detectors monitor the ambient concentration of atmospheric radon-222, a natural tracer of mixing and transport. They are sensitive, but respond slowly to ambient changes in radon concentration. In this paper, a deconvolution method is used to successfully correct observations for the instrument response. Case studies demonstrate that it is beneficial, sometimes necessary, to account for the detector response, especially when studying near-surface mixing.
Jenny A. Fisher, Daniel J. Jacob, Katherine R. Travis, Patrick S. Kim, Eloise A. Marais, Christopher Chan Miller, Karen Yu, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Jingqiu Mao, Paul O. Wennberg, John D. Crounse, Alex P. Teng, Tran B. Nguyen, Jason M. St. Clair, Ronald C. Cohen, Paul Romer, Benjamin A. Nault, Paul J. Wooldridge, Jose L. Jimenez, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Paul B. Shepson, Fulizi Xiong, Donald R. Blake, Allen H. Goldstein, Pawel K. Misztal, Thomas F. Hanisco, Glenn M. Wolfe, Thomas B. Ryerson, Armin Wisthaler, and Tomas Mikoviny
Atmos. Chem. Phys., 16, 5969–5991, https://doi.org/10.5194/acp-16-5969-2016, https://doi.org/10.5194/acp-16-5969-2016, 2016
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We use new airborne and ground-based observations from two summer 2013 campaigns in the southeastern US, interpreted with a chemical transport model, to understand the impact of isoprene and monoterpene chemistry on the atmospheric NOx budget via production of organic nitrates (RONO2). We find that a diversity of species contribute to observed RONO2. Our work implies that the NOx sink to RONO2 production is only sensitive to NOx emissions in regions where they are already low.
Karen Yu, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Christopher C. Miller, Katherine R. Travis, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Ron C. Cohen, Jack E. Dibb, Alan Fried, Tomas Mikoviny, Thomas B. Ryerson, Paul O. Wennberg, and Armin Wisthaler
Atmos. Chem. Phys., 16, 4369–4378, https://doi.org/10.5194/acp-16-4369-2016, https://doi.org/10.5194/acp-16-4369-2016, 2016
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Increasing the spatial resolution of a chemical transport model may improve simulations but can be computationally expensive. Using observations from the SEAC4RS aircraft campaign, we find that at higher spatial resolutions, models are better able to simulate the chemical pathways of ozone precursors, but the overall effect on regional mean concentrations is small. This implies that for continental boundary layer applications, coarse resolution models are adequate.
R. S. Humphries, A. R. Klekociuk, R. Schofield, M. Keywood, J. Ward, and S. R. Wilson
Atmos. Chem. Phys., 16, 2185–2206, https://doi.org/10.5194/acp-16-2185-2016, https://doi.org/10.5194/acp-16-2185-2016, 2016
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This work represents the first observational study of atmospheric sub-micron aerosols in the East Antarctic pack ice region and found springtime aerosol concentrations were higher than any observed elsewhere in the Antarctic and Southern Ocean region. Further analysis suggested these aerosols formed in the Antarctic free troposphere. Their subsequent transport to the Southern Ocean, as suggest by trajectory analyses, could help to reduce the discrepancy in the radiative budget in the region.
E. A. Marais, D. J. Jacob, J. L. Jimenez, P. Campuzano-Jost, D. A. Day, W. Hu, J. Krechmer, L. Zhu, P. S. Kim, C. C. Miller, J. A. Fisher, K. Travis, K. Yu, T. F. Hanisco, G. M. Wolfe, H. L. Arkinson, H. O. T. Pye, K. D. Froyd, J. Liao, and V. F. McNeill
Atmos. Chem. Phys., 16, 1603–1618, https://doi.org/10.5194/acp-16-1603-2016, https://doi.org/10.5194/acp-16-1603-2016, 2016
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Isoprene secondary organic aerosol (SOA) is a dominant aerosol component in the southeast US, but models routinely underestimate isoprene SOA with traditional schemes based on chamber studies operated under conditions not representative of isoprene-emitting forests. We develop a new irreversible uptake mechanism to reproduce isoprene SOA yields (3.3 %) and composition, and find a factor of 2 co-benefit of SO2 emission controls on reducing sulfate and organic aerosol in the southeast US.
R. S. Humphries, R. Schofield, M. D. Keywood, J. Ward, J. R. Pierce, C. M. Gionfriddo, M. T. Tate, D. P. Krabbenhoft, I. E. Galbally, S. B. Molloy, A. R. Klekociuk, P. V. Johnston, K. Kreher, A. J. Thomas, A. D. Robinson, N. R. P. Harris, R. Johnson, and S. R. Wilson
Atmos. Chem. Phys., 15, 13339–13364, https://doi.org/10.5194/acp-15-13339-2015, https://doi.org/10.5194/acp-15-13339-2015, 2015
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An atmospheric new particle formation event that was observed in the pristine East Antarctic pack ice during a springtime voyage in 2012 is characterised in terms of formation and growth rates. Known nucleation mechanisms (e.g. those involving sulfate, iodine and organics) were unable to explain observations; however, correlations with total gaseous mercury were found, leading to the suggestion of a possible mercury-driven nucleation mechanism not previously described.
P. S. Kim, D. J. Jacob, J. A. Fisher, K. Travis, K. Yu, L. Zhu, R. M. Yantosca, M. P. Sulprizio, J. L. Jimenez, P. Campuzano-Jost, K. D. Froyd, J. Liao, J. W. Hair, M. A. Fenn, C. F. Butler, N. L. Wagner, T. D. Gordon, A. Welti, P. O. Wennberg, J. D. Crounse, J. M. St. Clair, A. P. Teng, D. B. Millet, J. P. Schwarz, M. Z. Markovic, and A. E. Perring
Atmos. Chem. Phys., 15, 10411–10433, https://doi.org/10.5194/acp-15-10411-2015, https://doi.org/10.5194/acp-15-10411-2015, 2015
G. Zeng, J. E. Williams, J. A. Fisher, L. K. Emmons, N. B. Jones, O. Morgenstern, J. Robinson, D. Smale, C. Paton-Walsh, and D. W. T. Griffith
Atmos. Chem. Phys., 15, 7217–7245, https://doi.org/10.5194/acp-15-7217-2015, https://doi.org/10.5194/acp-15-7217-2015, 2015
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We assess the impact of biogenic emissions on CO and HCHO in the Southern Hemisphere (SH), with simulations using different emission inventories. Differences in biogenic emissions result in large differences on modelled CO in the source and the remote regions. Substantial inter-model differences exist. Models significantly underestimate observed HCHO columns in the SH, suggesting missing sources in the models. Differences in the CO/OH/CH4 chemistry lead to differences in HCHO in remote regions.
J. A. Fisher, S. R. Wilson, G. Zeng, J. E. Williams, L. K. Emmons, R. L. Langenfelds, P. B. Krummel, and L. P. Steele
Atmos. Chem. Phys., 15, 3217–3239, https://doi.org/10.5194/acp-15-3217-2015, https://doi.org/10.5194/acp-15-3217-2015, 2015
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The Southern Hemisphere (SH) serves as an important test bed for evaluating our understanding of the processes that drive the composition of the clean background atmosphere. Using data from two aircraft campaigns, combined with four atmospheric chemistry models, we find a large sensitivity in the remote SH to biogenic emissions and their subsequent chemistry and transport. Future model evaluation and measurement campaigns should prioritize reducing uncertainties in these processes.
F. Slemr, H. Angot, A. Dommergue, O. Magand, M. Barret, A. Weigelt, R. Ebinghaus, E.-G. Brunke, K. A. Pfaffhuber, G. Edwards, D. Howard, J. Powell, M. Keywood, and F. Wang
Atmos. Chem. Phys., 15, 3125–3133, https://doi.org/10.5194/acp-15-3125-2015, https://doi.org/10.5194/acp-15-3125-2015, 2015
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• Longer-term mercury measurement in the Southern Hemisphere is compared.
• Mercury, in terms of monthly and annual medians and averages, is more evenly distributed than hitherto believed.
• Consequently, trends observed at one or a few sites are likely to be representative of the whole hemisphere, and smaller trends can be detected in shorter time periods.
• We report a change in the trend sign at Cape Point from decreasing mercury concentrations in 1996-2004 to increasing ones since 2007.
R. Locatelli, P. Bousquet, F. Hourdin, M. Saunois, A. Cozic, F. Couvreux, J.-Y. Grandpeix, M.-P. Lefebvre, C. Rio, P. Bergamaschi, S. D. Chambers, U. Karstens, V. Kazan, S. van der Laan, H. A. J. Meijer, J. Moncrieff, M. Ramonet, H. A. Scheeren, C. Schlosser, M. Schmidt, A. Vermeulen, and A. G. Williams
Geosci. Model Dev., 8, 129–150, https://doi.org/10.5194/gmd-8-129-2015, https://doi.org/10.5194/gmd-8-129-2015, 2015
S. D. Chambers, A. G. Williams, J. Crawford, and A. D. Griffiths
Atmos. Chem. Phys., 15, 1175–1190, https://doi.org/10.5194/acp-15-1175-2015, https://doi.org/10.5194/acp-15-1175-2015, 2015
Z. M. Loh, R. M. Law, K. D. Haynes, P. B. Krummel, L. P. Steele, P. J. Fraser, S. D. Chambers, and A. G. Williams
Atmos. Chem. Phys., 15, 305–317, https://doi.org/10.5194/acp-15-305-2015, https://doi.org/10.5194/acp-15-305-2015, 2015
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The paper compares methane observations at Cape Grim, Tasmania, with model-simulated methane to better constrain methane fluxes from southeastern Australia. Inventory estimates of anthropogenic methane emissions appear to be supported by observed atmospheric methane. A missing methane source in springtime (October to November) is tentatively attributed to wetland emissions.
A. D. Griffiths, F. Conen, E. Weingartner, L. Zimmermann, S. D. Chambers, A. G. Williams, and M. Steinbacher
Atmos. Chem. Phys., 14, 12763–12779, https://doi.org/10.5194/acp-14-12763-2014, https://doi.org/10.5194/acp-14-12763-2014, 2014
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Radon detectors at Bern and Jungfraujoch were used to monitor the transport of radon-rich boundary layer air from the Swiss Plateau to the Alpine ridge. Radon was successfully used to discriminate between different types of vertical transport, using the shape of the diurnal cycle to identify days with upslope mountain winds. For many air-mass properties, however, the total land-surface influence (indicated by the radon concentration) was more decisive than the type of vertical transport.
T. P. C. van Noije, P. Le Sager, A. J. Segers, P. F. J. van Velthoven, M. C. Krol, W. Hazeleger, A. G. Williams, and S. D. Chambers
Geosci. Model Dev., 7, 2435–2475, https://doi.org/10.5194/gmd-7-2435-2014, https://doi.org/10.5194/gmd-7-2435-2014, 2014
S. D. Chambers, S.-B. Hong, A. G. Williams, J. Crawford, A. D. Griffiths, and S.-J. Park
Atmos. Chem. Phys., 14, 9903–9916, https://doi.org/10.5194/acp-14-9903-2014, https://doi.org/10.5194/acp-14-9903-2014, 2014
G. C. Edwards and D. A. Howard
Atmos. Chem. Phys., 13, 5325–5336, https://doi.org/10.5194/acp-13-5325-2013, https://doi.org/10.5194/acp-13-5325-2013, 2013
A. D. Griffiths, S. D. Parkes, S. D. Chambers, M. F. McCabe, and A. G. Williams
Atmos. Meas. Tech., 6, 207–218, https://doi.org/10.5194/amt-6-207-2013, https://doi.org/10.5194/amt-6-207-2013, 2013
Related subject area
Subject: Gases | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Deciphering anthropogenic and biogenic contributions to selected non-methane volatile organic compound emissions in an urban area
Emission characteristics of reactive organic gases (ROGs) from industrial volatile chemical products (VCPs) in the Pearl River Delta (PRD), China
Measurement report: Enhanced photochemical formation of formic and isocyanic acids in urban regions aloft – insights from tower-based online gradient measurements
Sources of organic gases and aerosol particles and their roles in nighttime particle growth at a rural forested site in southwest Germany
Surface snow bromide and nitrate at Eureka, Canada, in early spring and implications for polar boundary layer chemistry
Opinion: Strengthening research in the Global South – atmospheric science opportunities in South America and Africa
NO3 reactivity during a summer period in a temperate forest below and above the canopy
Shipping and algae emissions have a major impact on ambient air mixing ratios of non-methane hydrocarbons (NMHCs) and methanethiol on Utö Island in the Baltic Sea
Elevated oxidized mercury in the free troposphere: Analytical advances and application at a remote continental mountaintop site
Contribution of cooking emissions to the urban volatile organic compounds in Las Vegas, NV
Reanalysis of NOAA H2 observations: implications for the H2 budget
A large role of missing volatile organic compound reactivity from anthropogenic emissions in ozone pollution regulation
Using observed urban NOx sinks to constrain VOC reactivity and the ozone and radical budget in the Seoul Metropolitan Area
Measurement report: Insights into the chemical composition and origin of molecular clusters and potential precursor molecules present in the free troposphere over the southern Indian Ocean: observations from the Maïdo Observatory (2150 m a.s.l., Réunion)
Production of oxygenated volatile organic compounds from the ozonolysis of coastal seawater
Comment on “Transport of substantial stratospheric ozone to the surface by a dying typhoon and shallow convection” by Chen et al. (2022)
Observations of cyanogen bromide (BrCN) in the global troposphere and their relation to polar surface O3 destruction
Individual coal mine methane emissions constrained by eddy covariance measurements: low bias and missing sources
Real-world emission characteristics of VOCs from typical cargo ships and their potential contributions to SOA and O3 under low-sulfur fuel policies
Roles of oceanic ventilation and terrestrial outflow in the atmospheric non-methane hydrocarbons over the Chinese marginal seas
Measurement report: Observations of ground-level ozone concentration gradients perpendicular to the Lake Ontario shoreline
Biomass burning sources control ambient particulate matter but traffic and industrial sources control VOCs and secondary pollutant formation during extreme pollution events in Delhi
Measurement report: The Palau Atmospheric Observatory and its ozonesonde record – continuous monitoring of tropospheric composition and dynamics in the tropical western Pacific
Quantifying SO2 oxidation pathways to atmospheric sulfate using stable sulfur and oxygen isotopes: laboratory simulation and field observation
Influences of downward transport and photochemistry on surface ozone over East Antarctica during austral summer: in situ observations and model simulations
Iodine oxoacids and their roles in sub-3 nm particle growth in polluted urban environments
Measurement Report: Elevated excess-NH3 can promote the redox reaction to produce HONO: Insights from the COVID-19 pandemic
Intensive photochemical oxidation in the marine atmosphere: evidence from direct radical measurements
Diurnal variations in oxygen and nitrogen isotopes of atmospheric nitrogen dioxide and nitrate: implications for tracing NOx oxidation pathways and emission sources
Measurement report: Method for evaluating CO2 emissions from a cement plant using atmospheric δ(O2 ∕ N2) and CO2 measurements and its implication for future detection of CO2 capture signals
Aircraft-based mass balance estimate of methane emissions from offshore gas facilities in the southern North Sea
Parameterizations of US wildfire and prescribed fire emission ratios and emission factors based on FIREX-AQ aircraft measurements
Measurement report: Atmospheric nitrate radical chemistry in the South China Sea influenced by the urban outflow of the Pearl River Delta
Measurement report: Vertical and temporal variability of near-surface ozone production rate and sensitivity in an urban area in Pearl River Delta (PRD) region, China
The interhemispheric gradient of SF6 in the upper troposphere
Weather regimes and the related atmospheric composition at a Pyrenean observatory characterized by hierarchical clustering of a 5-year data set
Concentration and source changes of HONO during the COVID-19 lockdown in Beijing
Characteristics and sources of VOCs and the O3-NOx-VOCs relationships in the central plain city, China
Tropospheric bromine monoxide vertical profiles retrieved across the Alaskan Arctic in springtime
Source apportionment of methane emissions from the Upper Silesian Coal Basin using isotopic signatures
Measurement report: Exchange fluxes of HONO over agricultural fields in the North China Plain
HONO chemistry at a suburban site during the EXPLORE-YRD campaign in 2018: formation mechanisms and impacts on O3 production
Evaluation of modelled climatologies of O3, CO, water vapour and NOy in the upper troposphere–lower stratosphere using regular in situ observations by passenger aircraft
Photochemical ageing of aerosols contributes significantly to the production of atmospheric formic acid
Nitrous acid budgets in the coastal atmosphere: potential daytime marine sources
Undetected biogenic volatile organic compounds from Norway spruce drive total ozone reactivity measurements
Quantification of fossil fuel CO2 from combined CO, δ13CO2 and Δ14CO2 observations
Radical chemistry and ozone production at a UK coastal receptor site
Sources and long-term variability of carbon monoxide at Mount Kenya and in Nairobi
Measurement report: Airborne measurements of NOx fluxes over Los Angeles during the RECAP-CA 2021 campaign
Arianna Peron, Martin Graus, Marcus Striednig, Christian Lamprecht, Georg Wohlfahrt, and Thomas Karl
Atmos. Chem. Phys., 24, 7063–7083, https://doi.org/10.5194/acp-24-7063-2024, https://doi.org/10.5194/acp-24-7063-2024, 2024
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The anthropogenic fraction of non-methane volatile organic compound (NMVOC) emissions associated with biogenic sources (e.g., terpenes) is investigated based on eddy covariance observations. The anthropogenic fraction of terpene emissions is strongly dependent on season. When analyzing volatile chemical product (VCP) emissions in urban environments, we caution that observations from short-term campaigns might over-/underestimate their significance depending on local and seasonal circumstances.
Sihang Wang, Bin Yuan, Xianjun He, Ru Cui, Xin Song, Yubin Chen, Caihong Wu, Chaomin Wang, Yibo Huangfu, Xiao-Bing Li, Boguang Wang, and Min Shao
Atmos. Chem. Phys., 24, 7101–7121, https://doi.org/10.5194/acp-24-7101-2024, https://doi.org/10.5194/acp-24-7101-2024, 2024
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Emissions of reactive organic gases from industrial volatile chemical product sources are measured. There are large differences among these industrial sources. We show that oxygenated species account for significant contributions to reactive organic gas emissions, especially for industrial sources utilizing water-borne chemicals.
Qing Yang, Xiao-Bing Li, Bin Yuan, Xiaoxiao Zhang, Yibo Huangfu, Lei Yang, Xianjun He, Jipeng Qi, and Min Shao
Atmos. Chem. Phys., 24, 6865–6882, https://doi.org/10.5194/acp-24-6865-2024, https://doi.org/10.5194/acp-24-6865-2024, 2024
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Online vertical gradient measurements of formic and isocyanic acids were made based on a 320 m tower in a megacity. Vertical variations and sources of the two acids were analyzed in this study. We find that formic and isocyanic acids exhibited positive vertical gradients and were mainly contributed by photochemical formations. The formation of formic and isocyanic acids was also significantly enhanced in urban regions aloft.
Junwei Song, Harald Saathoff, Feng Jiang, Linyu Gao, Hengheng Zhang, and Thomas Leisner
Atmos. Chem. Phys., 24, 6699–6717, https://doi.org/10.5194/acp-24-6699-2024, https://doi.org/10.5194/acp-24-6699-2024, 2024
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This study presents concurrent online measurements of organic gas and particles (VOCs and OA) at a forested site in summer. Both VOCs and OA were largely contributed by oxygenated organic compounds. Semi-volatile oxygenated OA and organic nitrate formed from monoterpenes and sesquiterpenes contributed significantly to nighttime particle growth. The results help us to understand the causes of nighttime particle growth regularly observed in summer in central European rural forested environments.
Xin Yang, Kimberly Strong, Alison S. Criscitiello, Marta Santos-Garcia, Kristof Bognar, Xiaoyi Zhao, Pierre Fogal, Kaley A. Walker, Sara M. Morris, and Peter Effertz
Atmos. Chem. Phys., 24, 5863–5886, https://doi.org/10.5194/acp-24-5863-2024, https://doi.org/10.5194/acp-24-5863-2024, 2024
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This study uses snow samples collected from a Canadian high Arctic site, Eureka, to demonstrate that surface snow in early spring is a net sink of atmospheric bromine and nitrogen. Surface snow bromide and nitrate are significantly correlated, indicating the oxidation of reactive nitrogen is accelerated by reactive bromine. In addition, we show evidence that snow photochemical release of reactive bromine is very weak, and its emission flux is much smaller than the deposition flux of bromide.
Rebecca M. Garland, Katye E. Altieri, Laura Dawidowski, Laura Gallardo, Aderiana Mbandi, Nestor Y. Rojas, and N'datchoh E. Touré
Atmos. Chem. Phys., 24, 5757–5764, https://doi.org/10.5194/acp-24-5757-2024, https://doi.org/10.5194/acp-24-5757-2024, 2024
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This opinion piece focuses on two geographical areas in the Global South where the authors are based that are underrepresented in atmospheric science. This opinion provides context on common challenges and constraints, with suggestions on how the community can address these. The focus is on the strengths of atmospheric science research in these regions. It is these strengths, we believe, that highlight the critical role of Global South researchers in the future of atmospheric science research.
Patrick Dewald, Tobias Seubert, Simone T. Andersen, Gunther N. T. E. Türk, Jan Schuladen, Max R. McGillen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Chaoyang Xue, Abdelwahid Mellouki, Jos Lelieveld, and John N. Crowley
EGUsphere, https://doi.org/10.5194/egusphere-2024-1223, https://doi.org/10.5194/egusphere-2024-1223, 2024
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In scope of a field campaign in a suburban forest near Paris in the summer of 2022, we measured the reactivity of the nitrate radical (NO3) towards biogenic volatile organic compounds (BVOCs, e.g. monoterpenes) mainly below, but also above the canopy. NO3 reactivity was highest during nights with strong temperature inversions and decreased strongly with height. Reactions with BVOCs were the main removal process of NO3 throughout the diel cycle below the canopy.
Heidi Hellén, Rostislav Kouznetsov, Kaisa Kraft, Jukka Seppälä, Mika Vestenius, Jukka-Pekka Jalkanen, Lauri Laakso, and Hannele Hakola
Atmos. Chem. Phys., 24, 4717–4731, https://doi.org/10.5194/acp-24-4717-2024, https://doi.org/10.5194/acp-24-4717-2024, 2024
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Mixing ratios of C2-C5 NMHCs and methanethiol were measured on an island in the Baltic Sea using an in situ gas chromatograph. Shipping emissions were found to be an important source of ethene, ethyne, propene, and benzene. High summertime mixing ratios of methanethiol and dependence of mixing ratios on seawater temperature and height indicated the biogenic origin to possibly be phytoplankton or macroalgae. These emissions may have a strong impact on SO2 production and new particle formation.
Eleanor J. Derry, Tyler Elgiar, Taylor Y. Wilmot, Nicholas W. Hoch, Noah S. Hirshorn, Peter Weiss-Penzias, Christopher F. Lee, John C. Lin, A. Gannet Hallar, Rainer Volkamer, Seth N. Lyman, and Lynne E. Gratz
EGUsphere, https://doi.org/10.5194/egusphere-2024-1046, https://doi.org/10.5194/egusphere-2024-1046, 2024
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Mercury (Hg) is a globally-distributed neurotoxic pollutant. Atmospheric deposition is the main source of Hg to ecosystems. However, measurement biases hinder understanding of the origins and abundance of the more bioavailable oxidized form. We used an improved, calibrated measurement system to study air mass composition and transport of atmospheric Hg at a remote mountaintop site in the central U.S. Oxidized Hg originated upwind in the low to mid-free troposphere under clean, dry conditions.
Matthew M. Coggon, Chelsea E. Stockwell, Lu Xu, Jeff Peischl, Jessica B. Gilman, Aaron Lamplugh, Henry J. Bowman, Kenneth Aikin, Colin Harkins, Qindan Zhu, Rebecca H. Schwantes, Jian He, Meng Li, Karl Seltzer, Brian McDonald, and Carsten Warneke
Atmos. Chem. Phys., 24, 4289–4304, https://doi.org/10.5194/acp-24-4289-2024, https://doi.org/10.5194/acp-24-4289-2024, 2024
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Residential and commercial cooking emits pollutants that degrade air quality. Here, ambient observations show that cooking is an important contributor to anthropogenic volatile organic compounds (VOCs) emitted in Las Vegas, NV. These emissions are not fully presented in air quality models, and more work may be needed to quantify emissions from important sources, such as commercial restaurants.
Fabien Paulot, Gabrielle Pétron, Andrew M. Crotwell, and Matteo B. Bertagni
Atmos. Chem. Phys., 24, 4217–4229, https://doi.org/10.5194/acp-24-4217-2024, https://doi.org/10.5194/acp-24-4217-2024, 2024
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New data from the National Oceanic and Atmospheric Administration show that hydrogen (H2) concentrations increased from 2010 to 2019, which is consistent with the simulated increase in H2 photochemical production (mainly from methane). But this cannot be reconciled with the expected decrease (increase) in H2 anthropogenic emissions (soil deposition) in the same period. This shows gaps in our knowledge of the H2 biogeochemical cycle that must be resolved to quantify the impact of higher H2 usage.
Wenjie Wang, Bin Yuan, Hang Su, Yafang Cheng, Jipeng Qi, Sihang Wang, Wei Song, Xinming Wang, Chaoyang Xue, Chaoqun Ma, Fengxia Bao, Hongli Wang, Shengrong Lou, and Min Shao
Atmos. Chem. Phys., 24, 4017–4027, https://doi.org/10.5194/acp-24-4017-2024, https://doi.org/10.5194/acp-24-4017-2024, 2024
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This study investigates the important role of unmeasured volatile organic compounds (VOCs) in ozone formation. Based on results in a megacity of China, we show that unmeasured VOCs can contribute significantly to ozone fomation and also influence the determination of ozone control strategy. Our results show that these unmeasured VOCs are mainly from human sources.
Benjamin A. Nault, Katherine R. Travis, James H. Crawford, Donald R. Blake, Pedro Campuzano-Jost, Ronald C. Cohen, Joshua P. DiGangi, Glenn S. Diskin, Samuel R. Hall, L. Gregory Huey, Jose L. Jimenez, Kyung-Eun Kim, Young R. Lee, Isobel J. Simpson, Kirk Ullmann, and Armin Wisthaler
EGUsphere, https://doi.org/10.5194/egusphere-2024-596, https://doi.org/10.5194/egusphere-2024-596, 2024
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Ozone (O3) is a pollutant formed from the reactions of gases emitted from various sources. In urban areas, the density of human activities can increase the O3 formation rate (P(O3)); thus, impact air quality and health. Observations collected over Seoul, South Korea, are used to constrain P(O3). A high local P(O3) was found; however, local P(O3) was partly reduced due to compounds typically ignored. These observations also provide constraints for unmeasured compounds that will impact P(O3).
Romain Salignat, Matti Rissanen, Siddharth Iyer, Jean-Luc Baray, Pierre Tulet, Jean-Marc Metzger, Jérôme Brioude, Karine Sellegri, and Clémence Rose
Atmos. Chem. Phys., 24, 3785–3812, https://doi.org/10.5194/acp-24-3785-2024, https://doi.org/10.5194/acp-24-3785-2024, 2024
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Using mass spectrometry data collected at the Maïdo Observatory (2160 m a.s.l., Réunion), we provide the first detailed analysis of molecular cluster chemical composition specifically in the marine free troposphere. The abundance of the identified species is related both to in situ meteorological parameters and air mass history, which also provide insight into their origin. Our work makes an important contribution to documenting the chemistry and physics of the marine free troposphere.
Delaney B. Kilgour, Gordon A. Novak, Megan S. Claflin, Brian M. Lerner, and Timothy H. Bertram
Atmos. Chem. Phys., 24, 3729–3742, https://doi.org/10.5194/acp-24-3729-2024, https://doi.org/10.5194/acp-24-3729-2024, 2024
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Laboratory experiments with seawater mimics suggest ozone deposition to the surface ocean can be a source of reactive carbon to the marine atmosphere. We conduct both field and laboratory measurements to assess abiotic VOC composition and yields from ozonolysis of real surface seawater. We show that C5–C11 aldehydes contribute to the observed VOC emission flux. We estimate that VOCs generated by the ozonolysis of surface seawater are competitive with biological VOC production and emission.
Xiangdong Zheng, Wen Yang, Yuting Sun, Chunmei Geng, Yingying Liu, and Xiaobin Xu
Atmos. Chem. Phys., 24, 3759–3768, https://doi.org/10.5194/acp-24-3759-2024, https://doi.org/10.5194/acp-24-3759-2024, 2024
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Chen et al. (2022) attributed the nocturnal ozone enhancement (NOE) during the night of 31 July 2021 in the North China Plain (NCP) to "the direct stratospheric intrusion to reach the surface". We analyzed in situ data from the NCP. Our results do not suggest that there was a significant impact from the stratosphere on surface ozone during the NOE. We argue that the NOE was not caused by stratospheric intrusion but originated from fresh photochemical production in the lower troposphere.
James M. Roberts, Siyuan Wang, Patrick R. Veres, J. Andrew Neuman, Michael A. Robinson, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Hannah M. Allen, John D. Crounse, Paul O. Wennberg, Samuel R. Hall, Kirk Ullmann, Simone Meinardi, Isobel J. Simpson, and Donald Blake
Atmos. Chem. Phys., 24, 3421–3443, https://doi.org/10.5194/acp-24-3421-2024, https://doi.org/10.5194/acp-24-3421-2024, 2024
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We measured cyanogen bromide (BrCN) in the troposphere for the first time. BrCN is a product of the same active bromine chemistry that destroys ozone and removes mercury in polar surface environments and is a previously unrecognized sink for active Br compounds. BrCN has an apparent lifetime against heterogeneous loss in the range 1–10 d, so it serves as a cumulative marker of Br-radical chemistry. Accounting for BrCN chemistry is an important part of understanding polar Br cycling.
Kai Qin, Wei Hu, Qin He, Fan Lu, and Jason Blake Cohen
Atmos. Chem. Phys., 24, 3009–3028, https://doi.org/10.5194/acp-24-3009-2024, https://doi.org/10.5194/acp-24-3009-2024, 2024
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We compute CH4 emissions and uncertainty on a mine-by-mine basis, including underground, overground, and abandoned mines. Mine-by-mine gas and flux data and 30 min observations from a flux tower located next to a mine shaft are integrated. The observed variability and bias correction are propagated over the emissions dataset, demonstrating that daily observations may not cover the range of variability. Comparisons show both an emissions magnitude and spatial mismatch with current inventories.
Fan Zhang, Binyu Xiao, Zeyu Liu, Yan Zhang, Chongguo Tian, Rui Li, Can Wu, Yali Lei, Si Zhang, Xinyi Wan, Yubao Chen, Yong Han, Min Cui, Cheng Huang, Hongli Wang, Yingjun Chen, and Gehui Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-652, https://doi.org/10.5194/egusphere-2024-652, 2024
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Mandatory use of low-sulfur fuel according to global sulfur limit regulation leads to large uncertainty on VOCs emission. Therefore, on-board test of VOCs from 9 typical cargo ships in China were carried out. Results showed that the switch of fuels from heavy fuel oil to diesel increased EFVOCs by 48% on average, enhancing both O3 and secondary organic aerosol formation potentials. This indicated the implementation of globally ultra-low-sulfur oil policy in the near future needs to be optimized.
Jian Wang, Lei Xue, Qianyao Ma, Feng Xu, Gaobin Xu, Shibo Yan, Jiawei Zhang, Jianlong Li, Honghai Zhang, Guiling Zhang, and Zhaohui Chen
EGUsphere, https://doi.org/10.5194/egusphere-2023-2935, https://doi.org/10.5194/egusphere-2023-2935, 2024
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This study investigated the distribution and sources of non-methane hydrocarbons (NMHCs) in the lower atmosphere over the marginal seas of China. NMHCs, a subset of volatile organic compounds (VOCs), play a crucial role in atmospheric chemistry. Derived from systematic atmospheric sampling in coastal cities and marginal sea regions, this study offer valuable insights into the interaction between land and sea in shaping offshore atmospheric NMHCs.
Yao Yan Huang and D. James Donaldson
Atmos. Chem. Phys., 24, 2387–2398, https://doi.org/10.5194/acp-24-2387-2024, https://doi.org/10.5194/acp-24-2387-2024, 2024
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Ground-level ozone interacts at the lake–land boundary; this is important to our understanding and modelling of atmospheric chemistry and air pollution in the lower atmosphere. We show that a steep ozone gradient occurs year-round moving inland up to 1 km from the lake and that this gradient is influenced by seasonal factors on the local land environment, where more rural areas are more greatly affected seasonally.
Arpit Awasthi, Baerbel Sinha, Haseeb Hakkim, Sachin Mishra, Varkrishna Mummidivarapu, Gurmanjot Singh, Sachin D. Ghude, Vijay Kumar Soni, Narendra Nigam, Vinayak Sinha, and Madhavan N. Rajeevan
EGUsphere, https://doi.org/10.5194/egusphere-2024-501, https://doi.org/10.5194/egusphere-2024-501, 2024
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Our study uses a data set of 111 VOCs from a PTR-ToF-MS 10k, PM10 and PM2.5 in a PMF source-receptor model to resolve 11 pollution sources validated with chemical fingerprints collected at the source. Crop residue burning and heating contribute ~50 % of the PM, while traffic and industrial emissions dominate the gas-phase VOCs burden and SOA formation potential (>60 %). Non-tailpipe emissions from CNG powered commercial vehicles dominate the transport sector contribution to the PM burden.
Katrin Müller, Jordis S. Tradowsky, Peter von der Gathen, Christoph Ritter, Sharon Patris, Justus Notholt, and Markus Rex
Atmos. Chem. Phys., 24, 2169–2193, https://doi.org/10.5194/acp-24-2169-2024, https://doi.org/10.5194/acp-24-2169-2024, 2024
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The Palau Atmospheric Observatory is introduced as an ideal site to detect changes in atmospheric composition and dynamics above the remote tropical western Pacific. We focus on the ozone sounding program from 2016–2021, including El Niño 2016. The year-round high convective activity is reflected in dominant low tropospheric ozone and high relative humidity. Their seasonal distributions are unique compared to other tropical sites and are modulated by the Intertropical Convergence Zone.
Ziyan Guo, Keding Lu, Pengxiang Qiu, Mingyi Xu, and Zhaobing Guo
Atmos. Chem. Phys., 24, 2195–2205, https://doi.org/10.5194/acp-24-2195-2024, https://doi.org/10.5194/acp-24-2195-2024, 2024
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The formation of secondary sulfate needs to be further explored. In this work, we simultaneously measured sulfur and oxygen isotopic compositions to gain an increased understanding of specific sulfate formation processes. The results indicated that secondary sulfate was mainly ascribed to SO2 homogeneous oxidation by OH radicals and heterogeneous oxidation by H2O2 and Fe3+ / O2. This study is favourable for deeply investigating the sulfur cycle in the atmosphere.
Imran A. Girach, Narendra Ojha, Prabha R. Nair, Kandula V. Subrahmanyam, Neelakantan Koushik, Mohammed M. Nazeer, Nadimpally Kiran Kumar, Surendran Nair Suresh Babu, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 24, 1979–1995, https://doi.org/10.5194/acp-24-1979-2024, https://doi.org/10.5194/acp-24-1979-2024, 2024
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We investigate surface ozone variability in East Antarctica based on measurements and EMAC global model simulations during austral summer. Nearly half of the surface ozone is found to be of stratospheric origin. The east coast of Antarctica acts as a stronger sink of ozone than surrounding regions. Photochemical loss of ozone is counterbalanced by downward transport of ozone. The study highlights the intertwined role of chemistry and dynamics in governing ozone variations over East Antarctica.
Ying Zhang, Duzitian Li, Xu-Cheng He, Wei Nie, Chenjuan Deng, Runlong Cai, Yuliang Liu, Yishuo Guo, Chong Liu, Yiran Li, Liangduo Chen, Yuanyuan Li, Chenjie Hua, Tingyu Liu, Zongcheng Wang, Jiali Xie, Lei Wang, Tuukka Petäjä, Federico Bianchi, Ximeng Qi, Xuguang Chi, Pauli Paasonen, Yongchun Liu, Chao Yan, Jingkun Jiang, Aijun Ding, and Markku Kulmala
Atmos. Chem. Phys., 24, 1873–1893, https://doi.org/10.5194/acp-24-1873-2024, https://doi.org/10.5194/acp-24-1873-2024, 2024
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This study conducts a long-term observation of gaseous iodine oxoacids in two Chinese megacities, revealing their ubiquitous presence with peak concentrations (up to 0.1 pptv) in summer. Our analysis suggests a mix of terrestrial and marine sources for iodine. Additionally, iodic acid is identified as a notable contributor to sub-3 nm particle growth and particle survival probability.
Xinyuan Zhang, Lingling Wang, Nan Wang, Shuangliang Ma, Shenbo Wang, Ruiqin Zhang, Dong Zhang, Mingkai Wang, and Hongyu Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2023-2913, https://doi.org/10.5194/egusphere-2023-2913, 2024
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Online observational data on particulate matter composition, gaseous pollutants, and meteorological conditions from ten sites in China before and during the COVID-19 pandemic were analyzed to investigate the variation in NH3 concentrations and particle pH and explore the promoting effect of increased pH values on HONO formation. This is the first study to discuss the reasons for the increase in AOC during the pandemic from the perspective of the influence of NH3 on HONO.
Guoxian Zhang, Renzhi Hu, Pinhua Xie, Changjin Hu, Xiaoyan Liu, Liujun Zhong, Haotian Cai, Bo Zhu, Shiyong Xia, Xiaofeng Huang, Xin Li, and Wenqing Liu
Atmos. Chem. Phys., 24, 1825–1839, https://doi.org/10.5194/acp-24-1825-2024, https://doi.org/10.5194/acp-24-1825-2024, 2024
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Comprehensive observation of HOx radicals was conducted at a coastal site in the Pearl River Delta. Radical chemistry was influenced by different air masses in a time-dependent way. Land mass promotes a more active photochemical process, with daily averages of 7.1 × 106 and 5.2 × 108 cm−3 for OH and HO2 respectively. The rapid oxidation process was accompanied by a higher diurnal HONO concentration, which influences the ozone-sensitive system and eventually magnifies the background ozone.
Sarah Albertin, Joël Savarino, Slimane Bekki, Albane Barbero, Roberto Grilli, Quentin Fournier, Irène Ventrillard, Nicolas Caillon, and Kathy Law
Atmos. Chem. Phys., 24, 1361–1388, https://doi.org/10.5194/acp-24-1361-2024, https://doi.org/10.5194/acp-24-1361-2024, 2024
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This study reports the first simultaneous records of oxygen (Δ17O) and nitrogen (δ15N) isotopes in nitrogen dioxide (NO2) and nitrate (NO3−). These data are combined with atmospheric observations to explore sub-daily N reactive chemistry and quantify N fractionation effects in an Alpine winter city. The results highlight the necessity of using Δ17O and δ15N in both NO2 and NO3− to avoid biased estimations of NOx sources and fates from NO3− isotopic records in urban winter environments.
Shigeyuki Ishidoya, Kazuhiro Tsuboi, Hiroaki Kondo, Kentaro Ishijima, Nobuyuki Aoki, Hidekazu Matsueda, and Kazuyuki Saito
Atmos. Chem. Phys., 24, 1059–1077, https://doi.org/10.5194/acp-24-1059-2024, https://doi.org/10.5194/acp-24-1059-2024, 2024
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A method evaluating techniques for carbon neutrality, such as carbon capture and storage (CCS), is important. This study presents a method to evaluate CO2 emissions from a cement plant based on atmospheric O2 and CO2 measurements. The method will also be useful for evaluating CO2 capture from flue gas at CCS plants, since the plants remove CO2 from the atmosphere without causing any O2 changes, just as cement plants do, differing only in the direction of CO2 exchange with the atmosphere.
Magdalena Pühl, Anke Roiger, Alina Fiehn, Alan M. Gorchov Negron, Eric A. Kort, Stefan Schwietzke, Ignacio Pisso, Amy Foulds, James Lee, James L. France, Anna E. Jones, Dave Lowry, Rebecca E. Fisher, Langwen Huang, Jacob Shaw, Prudence Bateson, Stephen Andrews, Stuart Young, Pamela Dominutti, Tom Lachlan-Cope, Alexandra Weiss, and Grant Allen
Atmos. Chem. Phys., 24, 1005–1024, https://doi.org/10.5194/acp-24-1005-2024, https://doi.org/10.5194/acp-24-1005-2024, 2024
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In April–May 2019 we carried out an airborne field campaign in the southern North Sea with the aim of studying methane emissions of offshore gas installations. We determined methane emissions from elevated methane measured downstream of the sampled installations. We compare our measured methane emissions with estimated methane emissions from national and global annual inventories. As a result, we find inconsistencies of inventories and large discrepancies between measurements and inventories.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
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This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
Jie Wang, Haichao Wang, Yee Jun Tham, Lili Ming, Zelong Zheng, Guizhen Fang, Cuizhi Sun, Zhenhao Ling, Jun Zhao, and Shaojia Fan
Atmos. Chem. Phys., 24, 977–992, https://doi.org/10.5194/acp-24-977-2024, https://doi.org/10.5194/acp-24-977-2024, 2024
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Many works report NO3 chemistry in inland regions while less target marine regions. We measured N2O5 and related species on a typical island and found intensive nighttime chemistry and rapid NO3 loss. NO contributed significantly to NO3 loss despite its sub-ppbv level, suggesting nocturnal NO3 reactions would be largely enhanced once free from NO emissions in the open ocean. This highlights the strong influences of urban outflow on downward marine areas in terms of nighttime chemistry.
Jun Zhou, Chunsheng Zhang, Aiming Liu, Bin Yuan, Yan Wang, Wenjie Wang, Jie-Ping Zhou, Yixin Hao, Xiao-Bing Li, Xianjun He, Xin Song, Yubin Chen, Suxia Yang, Shuchun Yang, Yanfeng Wu, Bin Jiang, Shan Huang, Junwen Liu, Jipeng Qi, Minhui Deng, Yibo Huangfu, and Min Shao
EGUsphere, https://doi.org/10.5194/egusphere-2023-2230, https://doi.org/10.5194/egusphere-2023-2230, 2024
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In-depth understanding of near-ground vertical and temporal photochemical ozone (O3) formation is crucial for mitigating O3 pollution. By utilizing a self-built vertical observation system, a direct net photochemical O3 production rate detection system, and an observation-based model, we have diagnosed the vertical distributions and formation mechanism of net photochemical O3 production rates and sensitivity in Pearl River Delta region, one of the most O3 polluted area in China.
Tanja J. Schuck, Johannes Degen, Eric Hintsa, Peter Hoor, Markus Jesswein, Timo Keber, Daniel Kunkel, Fred Moore, Florian Obersteiner, Matt Rigby, Thomas Wagenhäuser, Luke M. Western, Andreas Zahn, and Andreas Engel
Atmos. Chem. Phys., 24, 689–705, https://doi.org/10.5194/acp-24-689-2024, https://doi.org/10.5194/acp-24-689-2024, 2024
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We study the interhemispheric gradient of sulfur hexafluoride (SF6), a strong long-lived greenhouse gas. Its emissions are stronger in the Northern Hemisphere; therefore, mixing ratios in the Southern Hemisphere lag behind. Comparing the observations to a box model, the model predicts air in the Southern Hemisphere to be older. For a better agreement, the emissions used as model input need to be increased (and their spatial pattern changed), and we need to modify north–south transport.
Jérémy Gueffier, François Gheusi, Marie Lothon, Véronique Pont, Alban Philibert, Fabienne Lohou, Solène Derrien, Yannick Bezombes, Gilles Athier, Yves Meyerfeld, Antoine Vial, and Emmanuel Leclerc
Atmos. Chem. Phys., 24, 287–316, https://doi.org/10.5194/acp-24-287-2024, https://doi.org/10.5194/acp-24-287-2024, 2024
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This study investigates the link between weather regime and atmospheric composition at a Pyrenean observatory. Five years of meteorological data were synchronized on a daily basis and then, using a clustering method, separated into six groups of observation days, with most showing marked characteristics of different weather regimes (fair and disturbed weather, winter windstorms, foehn). Statistical differences in gas and particle concentrations appeared between the groups and are discussed.
Yusheng Zhang, Feixue Zheng, Zemin Feng, Chaofan Lian, Weigang Wang, Xiaolong Fan, Wei Ma, Zhuohui Lin, Chang Li, Gen Zhang, Chao Yan, Ying Zhang, Veli-Matti Kerminen, Federico Bianch, Tuukka Petäjä, Juha Kangasluoma, Markku Kulmala, and Yongchun Liu
EGUsphere, https://doi.org/10.5194/egusphere-2023-3139, https://doi.org/10.5194/egusphere-2023-3139, 2024
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In this study, HONO budget has been validated during COVID-19 lockdown event. Main conclusions are as follows: 1. HONO concentrations show a significant decrease from 0.97 to 0.53ppb during lockdown. 2. Vehicle emissions accounted for 53% of nighttime sources. The heterogeneous conversion of NO2 on ground surfaces important (31%) than aerosol (2%). 3. Daytime dominant source shifts from the homogenous reaction between NO and OH (51%) to photolysis of nitrate photolysis (53%) during the lockdown.
Dong Zhang, Xiao Li, Minghao Yuan, Yifei Xu, Qixiang Xu, Fangcheng Su, Shenbo Wang, and Ruiqin Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2023-2835, https://doi.org/10.5194/egusphere-2023-2835, 2024
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In recent years, Zhengzhou's O3 pollution has increasingly intensified, becoming one of the cities with the highest O3 pollution in central China. During the observation period, ethane, acetone, and propane were always the most abundant species. Vehicular exhaust, solvent usage, and industrial production were the main emission sources of VOCs. According to the scenario analysis, the minimum reduction ratio of AVOCs/NOx should be no less than 3:1 to reduce O3 production.
Nathaniel Brockway, Peter K. Peterson, Katja Bigge, Kristian D. Hajny, Paul B. Shepson, Kerri A. Pratt, Jose D. Fuentes, Tim Starn, Robert Kaeser, Brian H. Stirm, and William R. Simpson
Atmos. Chem. Phys., 24, 23–40, https://doi.org/10.5194/acp-24-23-2024, https://doi.org/10.5194/acp-24-23-2024, 2024
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Bromine monoxide (BrO) strongly affects atmospheric chemistry in the springtime Arctic, yet there are still many uncertainties around its sources and recycling, particularly in the context of a rapidly changing Arctic. In this study, we observed BrO as a function of altitude above the Alaskan Arctic. We found that BrO was often most concentrated near the ground, confirming the ability of snow to produce and recycle reactive bromine, and identified four common vertical distributions of BrO.
Alina Fiehn, Maximilian Eckl, Julian Kostinek, Michał Gałkowski, Christoph Gerbig, Michael Rothe, Thomas Röckmann, Malika Menoud, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Mila Stanisavljević, Justyna Swolkień, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 23, 15749–15765, https://doi.org/10.5194/acp-23-15749-2023, https://doi.org/10.5194/acp-23-15749-2023, 2023
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During the CoMet mission in the Upper Silesian Coal Basin (USCB) ground-based and airborne air samples were taken and analyzed for the isotopic composition of CH4 to derive the mean signature of the USCB and source signatures of individual coal mines. Using δ2H signatures, the biogenic emissions from the USCB account for 15 %–50 % of total emissions, which is underestimated in common emission inventories. This demonstrates the importance of δ2H-CH4 observations for methane source apportionment.
Yifei Song, Chaoyang Xue, Yuanyuan Zhang, Pengfei Liu, Fengxia Bao, Xuran Li, and Yujing Mu
Atmos. Chem. Phys., 23, 15733–15747, https://doi.org/10.5194/acp-23-15733-2023, https://doi.org/10.5194/acp-23-15733-2023, 2023
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We present measurements of HONO flux and related parameters over an agricultural field during a whole growing season of summer maize. This dataset allows studies on the characteristics and influencing factors of soil HONO emissions, determination of HONO emission factors, estimation of total HONO emissions at a national scale, and the discussion on future environmental policies in terms of mitigating regional air pollution.
Can Ye, Keding Lu, Xuefei Ma, Wanyi Qiu, Shule Li, Xinping Yang, Chaoyang Xue, Tianyu Zhai, Yuhan Liu, Xuan Li, Yang Li, Haichao Wang, Zhaofeng Tan, Xiaorui Chen, Huabin Dong, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 15455–15472, https://doi.org/10.5194/acp-23-15455-2023, https://doi.org/10.5194/acp-23-15455-2023, 2023
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In this study, combining comprehensive field measurements and a box model, we found NO2 conversion on the ground surface was the most important source for HONO production among the proposed heterogeneous and gas-phase HONO sources. In addition, HONO was found to evidently enhance O3 production and aggravate O3 pollution in summer in China. Our study improved our understanding of the relative importance of different HONO sources and the crucial role of HONO in O3 formation in polluted areas.
Yann Cohen, Didier Hauglustaine, Bastien Sauvage, Susanne Rohs, Patrick Konjari, Ulrich Bundke, Andreas Petzold, Valérie Thouret, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 23, 14973–15009, https://doi.org/10.5194/acp-23-14973-2023, https://doi.org/10.5194/acp-23-14973-2023, 2023
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The upper troposphere–lower stratosphere (UTLS) is a key region regarding the lower atmospheric composition. This study consists of a comprehensive evaluation of an up-to-date chemistry–climate model in this layer, using regular in situ measurements based on passenger aircraft. For this purpose, a specific software (Interpol-IAGOS) has been updated and made publicly available. The model reproduces the carbon monoxide peaks due to biomass burning over the continental tropics particularly well.
Yifan Jiang, Men Xia, Zhe Wang, Penggang Zheng, Yi Chen, and Tao Wang
Atmos. Chem. Phys., 23, 14813–14828, https://doi.org/10.5194/acp-23-14813-2023, https://doi.org/10.5194/acp-23-14813-2023, 2023
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This study provides the first estimate of high rates of formic acid (HCOOH) production from the photochemical aging of real ambient particles and demonstrates the potential importance of this pathway in the formation of HCOOH under ambient conditions. Incorporating this pathway significantly improved the performance of a widely used chemical model. Our solution irradiation experiments demonstrated the importance of nitrate photolysis in HCOOH production via the production of oxidants.
Xuelian Zhong, Hengqing Shen, Min Zhao, Ji Zhang, Yue Sun, Yuhong Liu, Yingnan Zhang, Ye Shan, Hongyong Li, Jiangshan Mu, Yu Yang, Yanqiu Nie, Jinghao Tang, Can Dong, Xinfeng Wang, Yujiao Zhu, Mingzhi Guo, Wenxing Wang, and Likun Xue
Atmos. Chem. Phys., 23, 14761–14778, https://doi.org/10.5194/acp-23-14761-2023, https://doi.org/10.5194/acp-23-14761-2023, 2023
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Nitrous acid (HONO) is vital for atmospheric oxidation. In research at Mount Lao, China, models revealed a significant unidentified marine HONO source. Overlooking this could skew our understanding of air quality and climate change. This finding emphasizes HONO’s importance in the coastal atmosphere, uncovering previously unnoticed interactions.
Steven Job Thomas, Toni Tykkä, Heidi Hellén, Federico Bianchi, and Arnaud P. Praplan
Atmos. Chem. Phys., 23, 14627–14642, https://doi.org/10.5194/acp-23-14627-2023, https://doi.org/10.5194/acp-23-14627-2023, 2023
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The study employed total ozone reactivity to demonstrate how emissions of Norway spruce readily react with ozone and could be a major ozone sink, particularly under stress. Additionally, this approach provided insight into the limitations of current analytical techniques that measure the compounds present or emitted into the atmosphere. The study shows how the technique used was not enough to measure all compounds emitted, and this could potentially underestimate various atmospheric processes.
Jinsol Kim, John B. Miller, Charles E. Miller, Scott J. Lehman, Sylvia E. Michel, Vineet Yadav, Nick E. Rollins, and William M. Berelson
Atmos. Chem. Phys., 23, 14425–14436, https://doi.org/10.5194/acp-23-14425-2023, https://doi.org/10.5194/acp-23-14425-2023, 2023
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In this study, we present the partitioning of CO2 signals from biogenic, petroleum and natural gas sources by combining CO, 13CO2 and 14CO2 measurements. Using measurements from flask air samples at three sites in the greater Los Angeles region, we find larger and positive contributions of biogenic signals in winter and smaller and negative contributions in summer. The largest contribution of natural gas combustion generally occurs in summer.
Robert Woodward-Massey, Roberto Sommariva, Lisa K. Whalley, Danny R. Cryer, Trevor Ingham, William J. Bloss, Stephen M. Ball, Sam Cox, James D. Lee, Chris P. Reed, Leigh R. Crilley, Louisa J. Kramer, Brian J. Bandy, Grant L. Forster, Claire E. Reeves, Paul S. Monks, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 14393–14424, https://doi.org/10.5194/acp-23-14393-2023, https://doi.org/10.5194/acp-23-14393-2023, 2023
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Measurements of OH, HO2 and RO2 radicals and also OH reactivity were made at a UK coastal site and compared to calculations from a constrained box model utilising the Master Chemical Mechanism. The model agreement displayed a strong dependence on the NO concentration. An experimental budget analysis for OH, HO2, RO2 and total ROx demonstrated significant imbalances between HO2 and RO2 production rates. Ozone production rates were calculated from measured radicals and compared to modelled values.
Leonard Kirago, Örjan Gustafsson, Samuel Mwaniki Gaita, Sophie L. Haslett, Michael J. Gatari, Maria Elena Popa, Thomas Röckmann, Christoph Zellweger, Martin Steinbacher, Jörg Klausen, Christian Félix, David Njiru, and August Andersson
Atmos. Chem. Phys., 23, 14349–14357, https://doi.org/10.5194/acp-23-14349-2023, https://doi.org/10.5194/acp-23-14349-2023, 2023
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This study provides ground-observational evidence that supports earlier suggestions that savanna fires are the main emitters and modulators of carbon monoxide gas in Africa. Using isotope-based techniques, the study has shown that about two-thirds of this gas is emitted from savanna fires, while for urban areas, in this case Nairobi, primary sources approach 100 %. The latter has implications for air quality policy, suggesting primary emissions such as traffic should be targeted.
Clara M. Nussbaumer, Bryan K. Place, Qindan Zhu, Eva Y. Pfannerstill, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Ryan Ward, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 13015–13028, https://doi.org/10.5194/acp-23-13015-2023, https://doi.org/10.5194/acp-23-13015-2023, 2023
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NOx is a precursor to hazardous tropospheric ozone and can be emitted from various anthropogenic sources. It is important to quantify NOx emissions in urban environments to improve the local air quality, which still remains a challenge, as sources are heterogeneous in space and time. In this study, we calculate NOx emissions over Los Angeles, based on aircraft measurements in June 2021, and compare them to a local emission inventory, which we find mostly overpredicts the measured values.
Cited articles
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Griffiths, A. D., Chambers, S. D., Williams, A. G., and Werczynski, S.: Increasing the accuracy and temporal resolution of two-filter radon-222 measurements by correcting for the instrument response, Atmos. Meas. Tech., 9, 2689–2707, https://doi.org/10.5194/amt-9-2689-2016, 2016.
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Short summary
Mercury, a toxic metal, can be transported globally through the atmosphere, with deposition to ecosystems an important pathway to human exposure. 2 years of atmospheric mercury monitoring in tropical Australia supports recent evidence that Southern Hemisphere concentrations are lower than previously thought. Exchange between the atmosphere and ecosystems can take place on daily scales, with night deposition offset by morning re-emission. This could be an important transport pathway for mercury.
Mercury, a toxic metal, can be transported globally through the atmosphere, with deposition to...
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