Articles | Volume 21, issue 16
Atmos. Chem. Phys., 21, 12783–12807, 2021
https://doi.org/10.5194/acp-21-12783-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Special issue: Research results from the 14th International Conference on...
Atmos. Chem. Phys., 21, 12783–12807, 2021
https://doi.org/10.5194/acp-21-12783-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
30 Aug 2021
Research article
| 30 Aug 2021
Impact of Athabasca oil sands operations on mercury levels in air and deposition
Ashu Dastoor et al.
Related authors
Annemarie Fraser, Ashu Dastoor, and Andrei Ryjkov
Atmos. Chem. Phys., 18, 7263–7286, https://doi.org/10.5194/acp-18-7263-2018, https://doi.org/10.5194/acp-18-7263-2018, 2018
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This paper quantifies the emissions of mercury from biomass burning in Canada. Using an emissions inventory of mercury in the GEM-MACH-Hg model, surface observations of mercury concentration, and a top-down inversion method, we generate optimized emissions of mercury. We find that biomass burning is an important source of mercury emissions and deposition in Canada. Significant uncertainty remains, due to uncertainty in the speciation of emitted mercury.
Johannes Bieser, Franz Slemr, Jesse Ambrose, Carl Brenninkmeijer, Steve Brooks, Ashu Dastoor, Francesco DeSimone, Ralf Ebinghaus, Christian N. Gencarelli, Beate Geyer, Lynne E. Gratz, Ian M. Hedgecock, Daniel Jaffe, Paul Kelley, Che-Jen Lin, Lyatt Jaegle, Volker Matthias, Andrei Ryjkov, Noelle E. Selin, Shaojie Song, Oleg Travnikov, Andreas Weigelt, Winston Luke, Xinrong Ren, Andreas Zahn, Xin Yang, Yun Zhu, and Nicola Pirrone
Atmos. Chem. Phys., 17, 6925–6955, https://doi.org/10.5194/acp-17-6925-2017, https://doi.org/10.5194/acp-17-6925-2017, 2017
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We conducted a multi model study to investigate our ability to reproduce the vertical distribution of mercury in the atmosphere. For this, we used observational data from over 40 aircraft flights in EU and US. We compared observations to the results of seven chemistry transport models and found that the models are able to reproduce vertical gradients of total and elemental Hg. Finally, we found that different chemical reactions seem responsible for the oxidation of Hg depending on altitude.
Oleg Travnikov, Hélène Angot, Paulo Artaxo, Mariantonia Bencardino, Johannes Bieser, Francesco D'Amore, Ashu Dastoor, Francesco De Simone, María del Carmen Diéguez, Aurélien Dommergue, Ralf Ebinghaus, Xin Bin Feng, Christian N. Gencarelli, Ian M. Hedgecock, Olivier Magand, Lynwill Martin, Volker Matthias, Nikolay Mashyanov, Nicola Pirrone, Ramesh Ramachandran, Katie Alana Read, Andrei Ryjkov, Noelle E. Selin, Fabrizio Sena, Shaojie Song, Francesca Sprovieri, Dennis Wip, Ingvar Wängberg, and Xin Yang
Atmos. Chem. Phys., 17, 5271–5295, https://doi.org/10.5194/acp-17-5271-2017, https://doi.org/10.5194/acp-17-5271-2017, 2017
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The study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measurement data and simulation results of chemical transport models. Evaluation of the model simulations and numerical experiments against observations allows explaining spatial and temporal variations of Hg concentration in the near-surface atmospheric layer and shows possibility of multiple pathways of Hg oxidation occurring concurrently in various parts of the atmosphere.
Hélène Angot, Ashu Dastoor, Francesco De Simone, Katarina Gårdfeldt, Christian N. Gencarelli, Ian M. Hedgecock, Sarka Langer, Olivier Magand, Michelle N. Mastromonaco, Claus Nordstrøm, Katrine A. Pfaffhuber, Nicola Pirrone, Andrei Ryjkov, Noelle E. Selin, Henrik Skov, Shaojie Song, Francesca Sprovieri, Alexandra Steffen, Kenjiro Toyota, Oleg Travnikov, Xin Yang, and Aurélien Dommergue
Atmos. Chem. Phys., 16, 10735–10763, https://doi.org/10.5194/acp-16-10735-2016, https://doi.org/10.5194/acp-16-10735-2016, 2016
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This is a synthesis of the atmospheric mercury (Hg) monitoring data available in recent years (2011–2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. Based on this comparison, we discuss whether the processes that affect atmospheric Hg seasonality and interannual variability are appropriately represented in the models, and identify remaining research gaps.
K. Toyota, J. C. McConnell, R. M. Staebler, and A. P. Dastoor
Atmos. Chem. Phys., 14, 4101–4133, https://doi.org/10.5194/acp-14-4101-2014, https://doi.org/10.5194/acp-14-4101-2014, 2014
K. Toyota, A. P. Dastoor, and A. Ryzhkov
Atmos. Chem. Phys., 14, 4135–4167, https://doi.org/10.5194/acp-14-4135-2014, https://doi.org/10.5194/acp-14-4135-2014, 2014
G. Kos, A. Ryzhkov, A. Dastoor, J. Narayan, A. Steffen, P. A. Ariya, and L. Zhang
Atmos. Chem. Phys., 13, 4839–4863, https://doi.org/10.5194/acp-13-4839-2013, https://doi.org/10.5194/acp-13-4839-2013, 2013
Paul A. Makar, Craig Stroud, Ayodeji Akingunola, Junhua Zhang, Shuzhan Ren, Philip Cheung, and Qiong Zheng
Atmos. Chem. Phys., 21, 12291–12316, https://doi.org/10.5194/acp-21-12291-2021, https://doi.org/10.5194/acp-21-12291-2021, 2021
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Vehicle pollutant emissions occur in an environment where upward transport can be enhanced due to the turbulence created by the vehicles as they move through the atmosphere. An approach for including these turbulence effects in regional air pollution forecast models has been derived from theoretical, observation, and higher-resolution modeling. The enhanced mixing, which occurs in the immediate vicinity of roadways, changes pollutant concentrations on the regional to continental scale.
Paul A. Makar, Ayodeji Akingunola, Jack Chen, Balbir Pabla, Wanmin Gong, Craig Stroud, Christopher Sioris, Kerry Anderson, Philip Cheung, Junhua Zhang, and Jason Milbrandt
Atmos. Chem. Phys., 21, 10557–10587, https://doi.org/10.5194/acp-21-10557-2021, https://doi.org/10.5194/acp-21-10557-2021, 2021
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We have examined the effects of airborne particles on absorption and scattering of incoming sunlight by the particles themselves via cloud formation. We used an advanced, combined high-resolution weather forecast and chemical transport computer model, for western North America, and simulations with and without the connections between particles and weather enabled. Feedbacks improved weather and air pollution forecasts and changed cloud behaviour and forest-fire pollutant amount and height.
Katherine Hayden, Shao-Meng Li, Paul Makar, John Liggio, Samar G. Moussa, Ayodeji Akingunola, Robert McLaren, Ralf M. Staebler, Andrea Darlington, Jason O'Brien, Junhua Zhang, Mengistu Wolde, and Leiming Zhang
Atmos. Chem. Phys., 21, 8377–8392, https://doi.org/10.5194/acp-21-8377-2021, https://doi.org/10.5194/acp-21-8377-2021, 2021
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We developed a method using aircraft measurements to determine lifetimes with respect to dry deposition for oxidized sulfur and nitrogen compounds over the boreal forest in Alberta, Canada. Atmospheric lifetimes were significantly shorter than derived from chemical transport models with differences related to modelled dry deposition velocities. The shorter lifetimes suggest models need to reassess dry deposition treatment and predictions of sulfur and nitrogen in the atmosphere and ecosystems.
Attilio Naccarato, Antonella Tassone, Maria Martino, Sacha Moretti, Antonella Macagnano, Emiliano Zampetti, Paolo Papa, Joshua Avossa, Nicola Pirrone, Michelle Nerentorp, John Munthe, Ingvar Wängberg, Geoff W. Stupple, Carl P. J. Mitchell, Adam R. Martin, Alexandra Steffen, Diana Babi, Eric M. Prestbo, Francesca Sprovieri, and Frank Wania
Atmos. Meas. Tech., 14, 3657–3672, https://doi.org/10.5194/amt-14-3657-2021, https://doi.org/10.5194/amt-14-3657-2021, 2021
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Mercury monitoring in support of the Minamata Convention requires effective and reliable analytical tools. Passive sampling is a promising approach for creating a sustainable long-term network for atmospheric mercury with improved spatial resolution and global coverage. In this study the analytical performance of three passive air samplers (CNR-PAS, IVL-PAS, and MerPAS) was assessed over extended deployment periods and the accuracy of concentrations was judged by comparison with active sampling.
David S. McLagan, Geoff W. Stupple, Andrea Darlington, Katherine Hayden, and Alexandra Steffen
Atmos. Chem. Phys., 21, 5635–5653, https://doi.org/10.5194/acp-21-5635-2021, https://doi.org/10.5194/acp-21-5635-2021, 2021
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An assessment of mercury emissions from a burning boreal forest was made by flying an aircraft through its plume to collect in situ gas and particulate measurements. Direct data show that in-plume gaseous elemental mercury concentrations reach up to 2.4× background for this fire and up to 5.6× when using a correlation with CO data. These unique data are applied to a series of known empirical emissions estimates and used to highlight current uncertainties in the literature.
Cynthia H. Whaley, Elisabeth Galarneau, Paul A. Makar, Michael D. Moran, and Junhua Zhang
Atmos. Chem. Phys., 20, 2911–2925, https://doi.org/10.5194/acp-20-2911-2020, https://doi.org/10.5194/acp-20-2911-2020, 2020
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Benzene and polycyclic aromatic compounds are toxic air pollutants and ubiquitous in the environment. Using a chemical transport model, we have determined the net impact of vehicle emissions on ambient concentrations of these species. Traffic emissions were found to be a significant fraction of ambient pollution in the densely populated modelled region of North America. Our simulations demonstrate the air quality benefits that would result from transitioning to a zero-emission vehicle fleet.
Mark W. Shephard, Enrico Dammers, Karen E. Cady-Pereira, Shailesh K. Kharol, Jesse Thompson, Yonatan Gainariu-Matz, Junhua Zhang, Chris A. McLinden, Andrew Kovachik, Michael Moran, Shabtai Bittman, Christopher E. Sioris, Debora Griffin, Matthew J. Alvarado, Chantelle Lonsdale, Verica Savic-Jovcic, and Qiong Zheng
Atmos. Chem. Phys., 20, 2277–2302, https://doi.org/10.5194/acp-20-2277-2020, https://doi.org/10.5194/acp-20-2277-2020, 2020
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Presented is a description and survey demonstrating the capabilities of the CrIS ammonia product for monitoring, air quality forecast model evaluation, dry deposition estimates, and emission estimates of an agricultural hotspot.
Matthew Russell, Amir Hakami, Paul A. Makar, Ayodeji Akingunola, Junhua Zhang, Michael D. Moran, and Qiong Zheng
Atmos. Chem. Phys., 19, 4393–4417, https://doi.org/10.5194/acp-19-4393-2019, https://doi.org/10.5194/acp-19-4393-2019, 2019
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High-resolution air-quality forecast modeling results are compared for two different grid spacings for the Environment and Climate Change Canada GEM-MACH model. While the higher-resolution simulations have worse formal error scores, we show that the higher-resolution model nevertheless has the ability to better resolve plume maxima and has better performance when the evaluation occurs using new scoring metrics which operate on an equal-representative-area basis.
Wanmin Gong, Stephen R. Beagley, Sophie Cousineau, Mourad Sassi, Rodrigo Munoz-Alpizar, Sylvain Ménard, Jacinthe Racine, Junhua Zhang, Jack Chen, Heather Morrison, Sangeeta Sharma, Lin Huang, Pascal Bellavance, Jim Ly, Paul Izdebski, Lynn Lyons, and Richard Holt
Atmos. Chem. Phys., 18, 16653–16687, https://doi.org/10.5194/acp-18-16653-2018, https://doi.org/10.5194/acp-18-16653-2018, 2018
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The navigability of the Arctic Ocean is increasing with the warming in recent years. Using model simulations at a much finer resolution than previous pan-Arctic studies, the impact of marine shipping emissions on air pollution in the Canadian Arctic is assessed for present (2010) and projected levels in 2030. The study found that shipping emissions have a local-to-regional impact in the Arctic at the current level; the impact will increase significantly in a projected business-as-usual scenario.
Mark Gordon, Paul A. Makar, Ralf M. Staebler, Junhua Zhang, Ayodeji Akingunola, Wanmin Gong, and Shao-Meng Li
Atmos. Chem. Phys., 18, 14695–14714, https://doi.org/10.5194/acp-18-14695-2018, https://doi.org/10.5194/acp-18-14695-2018, 2018
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This work uses aircraft-based measurements of smokestack plumes carried out in northern Alberta in 2013. These measurements are used to test equations used to predict how high in the air smokestack plumes rise. It is important to predict plume rise height accurately as it tells us how far downwind pollutants are carried and what air quality can be expected at the surface. We found that the equations that are typically used significantly underestimate the plume rise at this location.
Craig A. Stroud, Paul A. Makar, Junhua Zhang, Michael D. Moran, Ayodeji Akingunola, Shao-Meng Li, Amy Leithead, Katherine Hayden, and May Siu
Atmos. Chem. Phys., 18, 13531–13545, https://doi.org/10.5194/acp-18-13531-2018, https://doi.org/10.5194/acp-18-13531-2018, 2018
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It is shown that using measurement-derived volatile organic compound (VOC) and organic aerosol (OA) emissions in the GEM-MACH air quality model provides better overall predictions compared to using bottom-up emission inventories. This work was done to better constrain the fugitive organic emissions from the Athabasca oil sands region, which are a challenge to estimate with bottom-up emission approaches. We use observations from the 2013 Joint Oil Sands Monitoring study.
Junhua Zhang, Michael D. Moran, Qiong Zheng, Paul A. Makar, Pegah Baratzadeh, George Marson, Peter Liu, and Shao-Meng Li
Atmos. Chem. Phys., 18, 10459–10481, https://doi.org/10.5194/acp-18-10459-2018, https://doi.org/10.5194/acp-18-10459-2018, 2018
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This paper discusses the development of new synthesized emissions inventories and the generation of air quality model-ready emissions files for the Athabasca Oil Sands Region of Alberta, Canada, using multiple emissions inventories, continuous emissions monitoring data, and inferred emission rates based on aircraft measurements. Novel facility-specific gridded spatial surrogate fields were generated to allocate emissions spatially within each huge mining facility.
Paul A. Makar, Ayodeji Akingunola, Julian Aherne, Amanda S. Cole, Yayne-abeba Aklilu, Junhua Zhang, Isaac Wong, Katherine Hayden, Shao-Meng Li, Jane Kirk, Ken Scott, Michael D. Moran, Alain Robichaud, Hazel Cathcart, Pegah Baratzedah, Balbir Pabla, Philip Cheung, Qiong Zheng, and Dean S. Jeffries
Atmos. Chem. Phys., 18, 9897–9927, https://doi.org/10.5194/acp-18-9897-2018, https://doi.org/10.5194/acp-18-9897-2018, 2018
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Complex computer model output was compared to and fused with observation data, to estimate potential damage due to acidifying precipitation for ecosystems in the Canadian provinces of Alberta and Saskatchewan. Estimated deposition was compared to the maximum no-damage ecosystem capacity for sulfur and/or nitrogen uptake; these critical loads were exceeded, for areas between 10 000 and 330 000 square kilometres, depending on ecosystem type: ecosystem damage will occur at 2013 emission levels.
Cynthia H. Whaley, Elisabeth Galarneau, Paul A. Makar, Ayodeji Akingunola, Wanmin Gong, Sylvie Gravel, Michael D. Moran, Craig Stroud, Junhua Zhang, and Qiong Zheng
Geosci. Model Dev., 11, 2609–2632, https://doi.org/10.5194/gmd-11-2609-2018, https://doi.org/10.5194/gmd-11-2609-2018, 2018
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We present a new, high-resolution, North American model of PAHs and benzene, which are toxic air pollutants that cause a variety of negative health impacts. Our simulation in a densely populated region of Canada and the U.S. shows that the model is improved over a previous model. The new model is particularly refined regarding the gas–particle partitioning of these pollutants, which has impacts on deposition and inhalation. The simulation was sensitive to the selection of vehicle emissions.
Ayodeji Akingunola, Paul A. Makar, Junhua Zhang, Andrea Darlington, Shao-Meng Li, Mark Gordon, Michael D. Moran, and Qiong Zheng
Atmos. Chem. Phys., 18, 8667–8688, https://doi.org/10.5194/acp-18-8667-2018, https://doi.org/10.5194/acp-18-8667-2018, 2018
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We examine the manner in which air-quality models simulate lofting of buoyant plumes of emissions from stacks (plume rise) and the impact of the level of detail in algorithms simulating particles' variation in size (particle size distribution). The most commonly used plume rise algorithm underestimates the height of plumes compared to observations, while a revised algorithm has much better performance. A 12-bin size distribution reduced the forecast 2-bin size distribution bias error by 32 %.
Annemarie Fraser, Ashu Dastoor, and Andrei Ryjkov
Atmos. Chem. Phys., 18, 7263–7286, https://doi.org/10.5194/acp-18-7263-2018, https://doi.org/10.5194/acp-18-7263-2018, 2018
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This paper quantifies the emissions of mercury from biomass burning in Canada. Using an emissions inventory of mercury in the GEM-MACH-Hg model, surface observations of mercury concentration, and a top-down inversion method, we generate optimized emissions of mercury. We find that biomass burning is an important source of mercury emissions and deposition in Canada. Significant uncertainty remains, due to uncertainty in the speciation of emitted mercury.
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.
Stephanie C. Pugliese, Jennifer G. Murphy, Felix R. Vogel, Michael D. Moran, Junhua Zhang, Qiong Zheng, Craig A. Stroud, Shuzhan Ren, Douglas Worthy, and Gregoire Broquet
Atmos. Chem. Phys., 18, 3387–3401, https://doi.org/10.5194/acp-18-3387-2018, https://doi.org/10.5194/acp-18-3387-2018, 2018
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We developed the Southern Ontario CO2 Emissions (SOCE) inventory, which identifies the spatial and temporal distribution (2.5 km and hourly, respectively) of CO2 emissions from seven source sectors. When the SOCE inventory was used with a chemistry transport model, we found strong agreement between modelled and measured mixing ratios. We were able to quantify that natural gas combustion contributes > 80 % of CO2 emissions at nighttime while on-road emissions contribute > 70 % during the day.
Cynthia H. Whaley, Paul A. Makar, Mark W. Shephard, Leiming Zhang, Junhua Zhang, Qiong Zheng, Ayodeji Akingunola, Gregory R. Wentworth, Jennifer G. Murphy, Shailesh K. Kharol, and Karen E. Cady-Pereira
Atmos. Chem. Phys., 18, 2011–2034, https://doi.org/10.5194/acp-18-2011-2018, https://doi.org/10.5194/acp-18-2011-2018, 2018
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Using a modified air quality forecasting model, we have found that a significant fraction (> 50 %) of ambient ammonia comes from re-emission from plants and soils in the broader Athabasca Oil Sands region and much of Alberta and Saskatchewan. We also found that about 20 % of ambient ammonia in Alberta and Saskatchewan came from forest fires in the summer of 2013. The addition of these two processes improved modelled ammonia, which was a motivating factor in undertaking this research.
Yuan You, Ralf M. Staebler, Samar G. Moussa, Yushan Su, Tony Munoz, Craig Stroud, Junhua Zhang, and Michael D. Moran
Atmos. Chem. Phys., 17, 14119–14143, https://doi.org/10.5194/acp-17-14119-2017, https://doi.org/10.5194/acp-17-14119-2017, 2017
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A novel approach for traffic emission measurements is shown to have the capacity to provide high-time-resolution accurate concentrations of key air pollutants. A top-down method for quantifying real-world emission rates produced vehicular emission factor estimates for carbon monoxide that agreed well with bottom-up values. Significant ammonia and hydrogen cyanide emissions were observed. The main factors modulating the concentrations were turbulent mixing and traffic density.
Johannes Bieser, Franz Slemr, Jesse Ambrose, Carl Brenninkmeijer, Steve Brooks, Ashu Dastoor, Francesco DeSimone, Ralf Ebinghaus, Christian N. Gencarelli, Beate Geyer, Lynne E. Gratz, Ian M. Hedgecock, Daniel Jaffe, Paul Kelley, Che-Jen Lin, Lyatt Jaegle, Volker Matthias, Andrei Ryjkov, Noelle E. Selin, Shaojie Song, Oleg Travnikov, Andreas Weigelt, Winston Luke, Xinrong Ren, Andreas Zahn, Xin Yang, Yun Zhu, and Nicola Pirrone
Atmos. Chem. Phys., 17, 6925–6955, https://doi.org/10.5194/acp-17-6925-2017, https://doi.org/10.5194/acp-17-6925-2017, 2017
Short summary
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We conducted a multi model study to investigate our ability to reproduce the vertical distribution of mercury in the atmosphere. For this, we used observational data from over 40 aircraft flights in EU and US. We compared observations to the results of seven chemistry transport models and found that the models are able to reproduce vertical gradients of total and elemental Hg. Finally, we found that different chemical reactions seem responsible for the oxidation of Hg depending on altitude.
Oleg Travnikov, Hélène Angot, Paulo Artaxo, Mariantonia Bencardino, Johannes Bieser, Francesco D'Amore, Ashu Dastoor, Francesco De Simone, María del Carmen Diéguez, Aurélien Dommergue, Ralf Ebinghaus, Xin Bin Feng, Christian N. Gencarelli, Ian M. Hedgecock, Olivier Magand, Lynwill Martin, Volker Matthias, Nikolay Mashyanov, Nicola Pirrone, Ramesh Ramachandran, Katie Alana Read, Andrei Ryjkov, Noelle E. Selin, Fabrizio Sena, Shaojie Song, Francesca Sprovieri, Dennis Wip, Ingvar Wängberg, and Xin Yang
Atmos. Chem. Phys., 17, 5271–5295, https://doi.org/10.5194/acp-17-5271-2017, https://doi.org/10.5194/acp-17-5271-2017, 2017
Short summary
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The study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measurement data and simulation results of chemical transport models. Evaluation of the model simulations and numerical experiments against observations allows explaining spatial and temporal variations of Hg concentration in the near-surface atmospheric layer and shows possibility of multiple pathways of Hg oxidation occurring concurrently in various parts of the atmosphere.
Craig A. Emmerton, Vincent L. St. Louis, Igor Lehnherr, Jennifer A. Graydon, Jane L. Kirk, and Kimberly J. Rondeau
Biogeosciences, 13, 5849–5863, https://doi.org/10.5194/bg-13-5849-2016, https://doi.org/10.5194/bg-13-5849-2016, 2016
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It is unknown if lakes are important contributors to the total transfer of greenhouse gases between high Arctic regions and the atmosphere. We measured the transfer of carbon greenhouse gases between lakes and the atmosphere and compared results with adjacent landscapes. We found lakes were weak emitters of the gases to the atmosphere, compared to contributions of terrestrial ecosystems, and will likely continue to be inconsequential to regional carbon cycling in a warmer future climate.
Hélène Angot, Ashu Dastoor, Francesco De Simone, Katarina Gårdfeldt, Christian N. Gencarelli, Ian M. Hedgecock, Sarka Langer, Olivier Magand, Michelle N. Mastromonaco, Claus Nordstrøm, Katrine A. Pfaffhuber, Nicola Pirrone, Andrei Ryjkov, Noelle E. Selin, Henrik Skov, Shaojie Song, Francesca Sprovieri, Alexandra Steffen, Kenjiro Toyota, Oleg Travnikov, Xin Yang, and Aurélien Dommergue
Atmos. Chem. Phys., 16, 10735–10763, https://doi.org/10.5194/acp-16-10735-2016, https://doi.org/10.5194/acp-16-10735-2016, 2016
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This is a synthesis of the atmospheric mercury (Hg) monitoring data available in recent years (2011–2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. Based on this comparison, we discuss whether the processes that affect atmospheric Hg seasonality and interannual variability are appropriately represented in the models, and identify remaining research gaps.
K. Toyota, J. C. McConnell, R. M. Staebler, and A. P. Dastoor
Atmos. Chem. Phys., 14, 4101–4133, https://doi.org/10.5194/acp-14-4101-2014, https://doi.org/10.5194/acp-14-4101-2014, 2014
K. Toyota, A. P. Dastoor, and A. Ryzhkov
Atmos. Chem. Phys., 14, 4135–4167, https://doi.org/10.5194/acp-14-4135-2014, https://doi.org/10.5194/acp-14-4135-2014, 2014
A. Steffen, J. Bottenheim, A. Cole, R. Ebinghaus, G. Lawson, and W. R. Leaitch
Atmos. Chem. Phys., 14, 2219–2231, https://doi.org/10.5194/acp-14-2219-2014, https://doi.org/10.5194/acp-14-2219-2014, 2014
A. Steffen, J. Bottenheim, A. Cole, T. A. Douglas, R. Ebinghaus, U. Friess, S. Netcheva, S. Nghiem, H. Sihler, and R. Staebler
Atmos. Chem. Phys., 13, 7007–7021, https://doi.org/10.5194/acp-13-7007-2013, https://doi.org/10.5194/acp-13-7007-2013, 2013
T. Berg, K. A. Pfaffhuber, A. S. Cole, O. Engelsen, and A. Steffen
Atmos. Chem. Phys., 13, 6575–6586, https://doi.org/10.5194/acp-13-6575-2013, https://doi.org/10.5194/acp-13-6575-2013, 2013
G. Kos, A. Ryzhkov, A. Dastoor, J. Narayan, A. Steffen, P. A. Ariya, and L. Zhang
Atmos. Chem. Phys., 13, 4839–4863, https://doi.org/10.5194/acp-13-4839-2013, https://doi.org/10.5194/acp-13-4839-2013, 2013
A. S. Cole, A. Steffen, K. A. Pfaffhuber, T. Berg, M. Pilote, L. Poissant, R. Tordon, and H. Hung
Atmos. Chem. Phys., 13, 1535–1545, https://doi.org/10.5194/acp-13-1535-2013, https://doi.org/10.5194/acp-13-1535-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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An assessment of the tropospherically accessible photo-initiated ground state chemistry of organic carbonyls
Methane emissions in the United States, Canada, and Mexico: evaluation of national methane emission inventories and 2010–2017 sectoral trends by inverse analysis of in situ (GLOBALVIEWplus CH4 ObsPack) and satellite (GOSAT) atmospheric observations
Projections of hydrofluorocarbon (HFC) emissions and the resulting global warming based on recent trends in observed abundances and current policies
Quantification of methane emissions from hotspots and during COVID-19 using a global atmospheric inversion
Estimation of mechanistic parameters in the gas-phase reactions of ozone with alkenes for use in automated mechanism construction
A process-oriented evaluation of CAMS reanalysis ozone during tropopause folds over Europe for the period 2003–2018
Evaluation of SO2, SO42− and an updated SO2 dry deposition parameterization in the United Kingdom Earth System Model
Development and evaluation of a new compact mechanism for aromatic oxidation in atmospheric models
Ozone deposition impact assessments for forest canopies require accurate ozone flux partitioning on diurnal timescales
Unraveling pathways of elevated ozone induced by the 2020 lockdown in Europe by an observationally constrained regional model using TROPOMI
Potential environmental impact of bromoform from Asparagopsis farming in Australia
Model evaluation of short-lived climate forcers for the Arctic Monitoring and Assessment Programme: a multi-species, multi-model study
Cloud-scale modelling of the impact of deep convection on the fate of oceanic bromoform in the troposphere: a case study over the west coast of Borneo
The impacts of marine-emitted halogens on OH radical in East Asia during summer
Improving predictability of high-ozone episodes through dynamic boundary conditions, emission refresh and chemical data assimilation during the Long Island Sound Tropospheric Ozone Study (LISTOS) field campaign
Global simulations of monoterpene-derived peroxy radical fates and the distributions of highly oxygenated organic molecules (HOM) and accretion products
Atmospheric observations consistent with reported decline in the UK's methane emissions (2013–2020)
Influence of atmospheric in-cloud aqueous-phase chemistry on the global simulation of SO2 in CESM2
Technical note: Quality assessment of ozone reanalysis products and gap-filling over subarctic Europe for vegetation risk mapping
Contribution of Asian emissions to upper tropospheric CO over the remote Pacific
Evolution of OH reactivity in NO-free volatile organic compound photooxidation investigated by the fully explicit GECKO-A model
Impact of pyruvic acid photolysis on acetaldehyde and peroxy radical formation in the boreal forest: theoretical calculations and model results
Evaluating consistency between total column CO2 retrievals from OCO-2 and the in situ network over North America: implications for carbon flux estimation
Global tropospheric halogen (Cl, Br, I) chemistry and its impact on oxidants
The role of emission reductions and the meteorological situation for air quality improvements during the COVID-19 lockdown period in central Europe
Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements
A mass-balance-based emission inventory of non-methane volatile organic compounds (NMVOCs) for solvent use in China
An Ensemble-Variational Inversion System for the Estimation of Ammonia Emissions using CrIS Satellite Ammonia Retrievals
Opinion: The germicidal effect of ambient air (open-air factor) revisited
Study of different Carbon Bond 6 (CB6) mechanisms by using a concentration sensitivity analysis
Accelerating methane growth rate from 2010 to 2017: leading contributions from the tropics and East Asia
Observation and modelling of ozone-destructive halogen chemistry in a passively degassing volcanic plume
Modeling study of the impact of SO2 volcanic passive emissions on the tropospheric sulfur budget
The impact of organic pollutants from Indonesian peatland fires on the tropospheric and lower stratospheric composition
Comprehensive evaluations of diurnal NO2 measurements during DISCOVER-AQ 2011: effects of resolution-dependent representation of NOx emissions
Downscaling system for modeling of atmospheric composition on regional, urban and street scales
Satellite soil moisture data assimilation impacts on modeling weather variables and ozone in the southeastern US – Part 1: An overview
Wei Ma, Zemin Feng, Junlei Zhan, Yongchun Liu, Pengfei Liu, Chengtang Liu, Qingxin Ma, Kang Yang, Yafei Wang, Hong He, Markku Kulmala, Yujing Mu, and Junfeng Liu
Atmos. Chem. Phys., 22, 4841–4851, https://doi.org/10.5194/acp-22-4841-2022, https://doi.org/10.5194/acp-22-4841-2022, 2022
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The influence of photochemical loss of volatile organic compounds (VOCS) on O3 formation is investigated using an observation-based model. The sensitivity regime of ozone formation might be misdiagnosed due to the photochemical loss of VOCs in the atmosphere. The contribution of local photochemistry is underestimated regarding O3 pollution when one does not consider the photochemical loss of VOCs.
Pinya Wang, Yang Yang, Huimin Li, Lei Chen, Ruijun Dang, Daokai Xue, Baojie Li, Jianping Tang, L. Ruby Leung, and Hong Liao
Atmos. Chem. Phys., 22, 4705–4719, https://doi.org/10.5194/acp-22-4705-2022, https://doi.org/10.5194/acp-22-4705-2022, 2022
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China is now suffering from both severe ozone (O3) pollution and heat events. We highlight that North China Plain is the hot spot of the co-occurrences of extremes in O3 and high temperatures in China. Such coupled extremes exhibit an increasing trend during 2014–2019 and will continue to increase until the middle of this century. And the coupled extremes impose more severe health impacts to human than O3 pollution occurring alone because of elevated O3 levels and temperatures.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275, https://doi.org/10.5194/acp-22-4253-2022, https://doi.org/10.5194/acp-22-4253-2022, 2022
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Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
Nikos Daskalakis, Laura Gallardo, Maria Kanakidou, Johann Rasmus Nüß, Camilo Menares, Roberto Rondanelli, Anne M. Thompson, and Mihalis Vrekoussis
Atmos. Chem. Phys., 22, 4075–4099, https://doi.org/10.5194/acp-22-4075-2022, https://doi.org/10.5194/acp-22-4075-2022, 2022
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Forest fires emit carbon monoxide (CO) that can be transported into the atmosphere far from the sources and reacts to produce ozone (O3) that affects climate, ecosystems and health. O3 is also produced in the stratosphere and can be transported downwards. Using a global numerical model, we found that forest fires can affect CO and O3 even in the South Pacific, the most pristine region of the global ocean, but transport from the stratosphere is a more important O3 source than fires in the region.
Le Cao, Linjie Fan, Simeng Li, and Shuangyan Yang
Atmos. Chem. Phys., 22, 3875–3890, https://doi.org/10.5194/acp-22-3875-2022, https://doi.org/10.5194/acp-22-3875-2022, 2022
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We analyzed the observational data and used models to discover the impact of the total ozone column (TOC) on the occurrence of tropospheric ozone depletion events (ODE) in the Antarctic. The results suggest that the decrease of TOC favors the occurrence of ODE. When TOC varies the rates of major ODE accelerating reactions are substantially altered but the rates of major ODE decelerating reactions remain unchanged. As a result, the occurrence of ODE negatively depends on the TOC.
Henry Bowman, Steven Turnock, Susanne E. Bauer, Kostas Tsigaridis, Makoto Deushi, Naga Oshima, Fiona M. O'Connor, Larry Horowitz, Tongwen Wu, Jie Zhang, Dagmar Kubistin, and David D. Parrish
Atmos. Chem. Phys., 22, 3507–3524, https://doi.org/10.5194/acp-22-3507-2022, https://doi.org/10.5194/acp-22-3507-2022, 2022
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A full understanding of ozone in the troposphere requires investigation of its temporal variability over all timescales. Model simulations show that the northern midlatitude ozone seasonal cycle shifted with industrial development (1850–2014), with an increasing magnitude and a later summer peak. That shift reached a maximum in the mid-1980s, followed by a reversal toward the preindustrial cycle. The few available observations, beginning in the 1970s, are consistent with the model simulations.
Jingwei Zhang, Chaofan Lian, Weigang Wang, Maofa Ge, Yitian Guo, Haiyan Ran, Yusheng Zhang, Feixue Zheng, Xiaolong Fan, Chao Yan, Kaspar R. Daellenbach, Yongchun Liu, Markku Kulmala, and Junling An
Atmos. Chem. Phys., 22, 3275–3302, https://doi.org/10.5194/acp-22-3275-2022, https://doi.org/10.5194/acp-22-3275-2022, 2022
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This study added six potential HONO sources to the WRF-Chem model, evaluated their impact on HONO and O3 concentrations, including surface and vertical concentrations. The simulations extend our knowledge on atmospheric HONO sources, especially for nitrate photolysis. The study also explains the HONO difference in O3 formation on clean and hazy days, and reveals key potential HONO sources to O3 enhancements in haze-aggravating processes with a co-occurrence of high PM2.5 and O3 concentrations.
Lei Hu, Stephen A. Montzka, Fred Moore, Eric Hintsa, Geoff Dutton, M. Carolina Siso, Kirk Thoning, Robert W. Portmann, Kathryn McKain, Colm Sweeney, Isaac Vimont, David Nance, Bradley Hall, and Steven Wofsy
Atmos. Chem. Phys., 22, 2891–2907, https://doi.org/10.5194/acp-22-2891-2022, https://doi.org/10.5194/acp-22-2891-2022, 2022
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The unexpected increase in CFC-11 emissions between 2012 and 2017 resulted in concerns about delaying the stratospheric ozone recovery. Although the subsequent decline of CFC-11 emissions indicated a mitigation in part to this problem, the regions fully responsible for these large emission changes were unclear. Here, our new estimate, based on atmospheric measurements from two global campaigns and from NOAA, suggests Asia primarily contributed to the global CFC-11 emission rise during 2012–2017.
Dianyi Li, Drew Shindell, Dian Ding, Xiao Lu, Lin Zhang, and Yuqiang Zhang
Atmos. Chem. Phys., 22, 2625–2638, https://doi.org/10.5194/acp-22-2625-2022, https://doi.org/10.5194/acp-22-2625-2022, 2022
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In this study, we applied chemical transport model simulation with the latest annual anthropogenic emission inventory to study the long-term trend of ozone-induced crop production losses from 2010 to 2017 in China. We find that overall the ozone-induced crop production loss in China is significant and the annual average economic losses for wheat, rice, maize, and soybean in China are USD 9.55 billion, USD 8.53 billion, USD 2.23 billion, and USD 1.16 billion respectively, over the 8 years.
Jing Cao, Shuping Situ, Yufang Hao, Shaodong Xie, and Lingyu Li
Atmos. Chem. Phys., 22, 2351–2364, https://doi.org/10.5194/acp-22-2351-2022, https://doi.org/10.5194/acp-22-2351-2022, 2022
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Based on localized emission factors and high-resolution vegetation data, we simulated the impacts of BVOC emissions on O3 and SOA during 1981–2018 in China. The interannual variation of BVOC emissions caused by increasing leaf biomass resulted in O3 and SOA concentrations increasing at average annual rates of 0.11 ppb and 0.008 μg m−3, respectively. The results show different variations which can be attributed to the different changing trends of leaf biomass by region and vegetation type.
Narcisse Tsona Tchinda, Lin Du, Ling Liu, and Xiuhui Zhang
Atmos. Chem. Phys., 22, 1951–1963, https://doi.org/10.5194/acp-22-1951-2022, https://doi.org/10.5194/acp-22-1951-2022, 2022
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This study explores the effect of pyruvic acid (PA) both in the SO3 hydrolysis and in sulfuric-acid-based aerosol formation. Results show that in dry and polluted areas, PA-catalyzed SO3 hydrolysis is about 2 orders of magnitude more efficient at forming sulfuric acid than the water-catalyzed reaction. Moreover, PA can effectively enhance the ternary SA-PA-NH3 particle formation rate by up to 4.7×102 relative to the binary SA-NH3 particle formation rate at cold temperatures.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Fiona M. O'Connor, and Steven T. Turnock
Atmos. Chem. Phys., 22, 1209–1227, https://doi.org/10.5194/acp-22-1209-2022, https://doi.org/10.5194/acp-22-1209-2022, 2022
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Tropospheric ozone is important to future air quality and climate, and changing emissions and climate influence ozone. We investigate the evolution of ozone and ozone sensitivity from the present day (2004–2014) to the future (2045–2055) and explore the main drivers of ozone changes from global and regional perspectives. This helps guide suitable emission control strategies to mitigate ozone pollution.
Haiyue Tan, Lin Zhang, Xiao Lu, Yuanhong Zhao, Bo Yao, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 22, 1229–1249, https://doi.org/10.5194/acp-22-1229-2022, https://doi.org/10.5194/acp-22-1229-2022, 2022
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Methane is the second most important anthropogenic greenhouse gas. Understanding methane emissions and concentration growth over China in the past decade is important to support its mitigation. This study analyzes the contributions of methane emissions from different regions and sources over the globe to methane changes over China in 2007–2018. Our results show strong international transport influences and emphasize the need of intensive methane measurements covering eastern China.
Keiran N. Rowell, Scott H. Kable, and Meredith J. T. Jordan
Atmos. Chem. Phys., 22, 929–949, https://doi.org/10.5194/acp-22-929-2022, https://doi.org/10.5194/acp-22-929-2022, 2022
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Sunlight drives chemical reactions in the atmosphere by breaking chemical bonds. Motivated by the knowledge that if we can better understand the fundamental chemistry, we will be better able to predict atmospheric composition and model any future changes, we use quantum chemistry to investigate new classes of atmospheric reactions. We identify several potentially important reaction classes that will have implications for the atmospheric production of organic acids and molecular hydrogen.
Xiao Lu, Daniel J. Jacob, Haolin Wang, Joannes D. Maasakkers, Yuzhong Zhang, Tia R. Scarpelli, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Hannah Nesser, A. Anthony Bloom, Shuang Ma, John R. Worden, Shaojia Fan, Robert J. Parker, Hartmut Boesch, Ritesh Gautam, Deborah Gordon, Michael D. Moran, Frances Reuland, Claudia A. Octaviano Villasana, and Arlyn Andrews
Atmos. Chem. Phys., 22, 395–418, https://doi.org/10.5194/acp-22-395-2022, https://doi.org/10.5194/acp-22-395-2022, 2022
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We evaluate methane emissions and trends for 2010–2017 in the gridded national emission inventories for the United States, Canada, and Mexico by inversion of in situ and satellite methane observations. We find that anthropogenic methane emissions for all three countries are underestimated in the national inventories, largely driven by oil emissions. Anthropogenic methane emissions in the US peak in 2014, in contrast to the report of a steadily decreasing trend over 2010–2017 from the US EPA.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1070, https://doi.org/10.5194/acp-2021-1070, 2022
Revised manuscript accepted for ACP
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The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past decades as a result of the phaseout of ozone depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
Joe McNorton, Nicolas Bousserez, Anna Agustí-Panareda, Gianpaolo Balsamo, Richard Engelen, Vincent Huijnen, Antje Inness, Zak Kipling, Mark Parrington, and Roberto Ribas
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1056, https://doi.org/10.5194/acp-2021-1056, 2022
Revised manuscript accepted for ACP
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Concentrations of atmospheric methane continue to grow and in recent years at an increasing rate, the reason for which is unknown. Using newly available satellite observations and a state-of-the-art weather prediction model we perform global estimates of emissions from hotspots at high-resolution. Results show the system can accurately report on biases in inventory reporting and is used to conclude the COVID-19 slowdown had very little impact on global methane emissions.
Mike J. Newland, Camille Mouchel-Vallon, Richard Valorso, Bernard Aumont, Luc Vereecken, Michael E. Jenkin, and Andrew R. Rickard
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1031, https://doi.org/10.5194/acp-2021-1031, 2022
Revised manuscript accepted for ACP
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Alkene ozonolysis produces Criegee intermediates, which can act as oxidants or decompose to give a range of closed shell and radical products, including OH. Therefore it is essential to accurately represent the chemistry of Criegee intermediates in atmospheric models in order to understand their impacts on atmospheric composition. Here we provide a mechanism construction protocol by which the central features of alkene ozonolysis chemistry can be included in an automatic mechanism generator.
Dimitris Akritidis, Andrea Pozzer, Johannes Flemming, Antje Inness, Philippe Nédélec, and Prodromos Zanis
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-998, https://doi.org/10.5194/acp-2021-998, 2021
Preprint under review for ACP
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We perform a process-oriented evaluation of Copernicus Atmosphere Monitoring Service (CAMS) reanalysis (CAMSRA) O3 over Europe, using WOUDC (World Ozone and Ultraviolet Radiation Data Centre) ozonesondes and IAGOS (In-service Aircraft for a Global Observing System) aircraft measurements. Chemical data assimilation assists CAMSRA to reproduce the observed O3 increases in the troposphere during the examined folding events, yet it mostly results in O3 overestimation in the upper troposphere.
Catherine Hardacre, Jane P. Mulcahy, Richard J. Pope, Colin G. Jones, Steven T. Rumbold, Can Li, Colin Johnson, and Steven T. Turnock
Atmos. Chem. Phys., 21, 18465–18497, https://doi.org/10.5194/acp-21-18465-2021, https://doi.org/10.5194/acp-21-18465-2021, 2021
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We investigate UKESM1's ability to represent the sulfur (S) cycle in the recent historical period. The S cycle is a key driver of historical radiative forcing. Earth system models such as UKESM1 should represent the S cycle well so that we can have confidence in their projections of future climate. We compare UKESM1 to observations of sulfur compounds, finding that the model generally performs well. We also identify areas for UKESM1’s development, focussing on how SO2 is removed from the air.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Auke J. Visser, Laurens N. Ganzeveld, Ignacio Goded, Maarten C. Krol, Ivan Mammarella, Giovanni Manca, and K. Folkert Boersma
Atmos. Chem. Phys., 21, 18393–18411, https://doi.org/10.5194/acp-21-18393-2021, https://doi.org/10.5194/acp-21-18393-2021, 2021
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Dry deposition is an important sink for tropospheric ozone that affects ecosystem carbon uptake, but process understanding remains incomplete. We apply a common deposition representation in atmospheric chemistry models and a multi-layer canopy model to multi-year ozone deposition observations. The multi-layer canopy model performs better on diurnal timescales compared to the common approach, leading to a substantially improved simulation of ozone deposition and vegetation ozone impact metrics.
Amir H. Souri, Kelly Chance, Juseon Bak, Caroline R. Nowlan, Gonzalo González Abad, Yeonjin Jung, David C. Wong, Jingqiu Mao, and Xiong Liu
Atmos. Chem. Phys., 21, 18227–18245, https://doi.org/10.5194/acp-21-18227-2021, https://doi.org/10.5194/acp-21-18227-2021, 2021
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The global pandemic is believed to have an impact on emissions of air pollutants such as nitrogen dioxide (NO2) and formaldehyde (HCHO). This study quantifies the changes in the amount of NOx and VOC emissions via state-of-the-art inverse modeling technique using satellite observations during the lockdown 2020 with respect to a baseline over Europe, which in turn, it permits unraveling atmospheric processes being responsible for ozone formation in a less cloudy month.
Yue Jia, Birgit Quack, Robert D. Kinley, Ignacio Pisso, and Susann Tegtmeier
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-800, https://doi.org/10.5194/acp-2021-800, 2021
Revised manuscript accepted for ACP
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In this study, we assessed the potential risks of bromoform released from Asparagopsis farming near Australia for the stratospheric ozone layer by analyzing different cultivation scenarios. We conclude that the intended operation of Asparagopsis seaweed cultivation farms with an annual yield to meet the need of 50 % feedlot and cattle in either open ocean or terrestrial cultures in Australia will not impact the ozone layer under normal operating conditions.
Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay M. Damani, Kostas Eleftheriadis, Nikolaos Evangeliou, Gregory S. Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-975, https://doi.org/10.5194/acp-2021-975, 2021
Revised manuscript accepted for ACP
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Air pollutants, like ozone and soot play a role in both global warming and air quality. Atmospheric models are often used to provide information to policy makers about current and future conditions under different emissions scenarios. In order to have confidence in those simulations, in this study we compare simulated air pollution from 18 state-of-the art atmospheric models to measured air pollution, in order to assess how well the models perform.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Shidong Fan and Ying Li
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-876, https://doi.org/10.5194/acp-2021-876, 2021
Revised manuscript accepted for ACP
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We investigated the mechanisms how marine-emitted halogens influence OH radical. We found that atmospheric OH radical has a very complicated response to halogen emissions, and different species can increase or decrease OH through different physical and chemical processes. Over ocean, inorganic iodine is the controlling species and chemistry is more important. Over land, the physics of sea salt aerosols is more important. The detailed mechanisms can be applied to other circumstances.
Siqi Ma, Daniel Tong, Lok Lamsal, Julian Wang, Xuelei Zhang, Youhua Tang, Rick Saylor, Tianfeng Chai, Pius Lee, Patrick Campbell, Barry Baker, Shobha Kondragunta, Laura Judd, Timothy A. Berkoff, Scott J. Janz, and Ivanka Stajner
Atmos. Chem. Phys., 21, 16531–16553, https://doi.org/10.5194/acp-21-16531-2021, https://doi.org/10.5194/acp-21-16531-2021, 2021
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Predicting high ozone gets more challenging as urban emissions decrease. How can different techniques be used to foretell the quality of air to better protect human health? We tested four techniques with the CMAQ model against observations during a field campaign over New York City. The new system proves to better predict the magnitude and timing of high ozone. These approaches can be extended to other regions to improve the predictability of high-O3 episodes in contemporary urban environments.
Ruochong Xu, Joel A. Thornton, Ben H. Lee, Yanxu Zhang, Lyatt Jaeglé, Felipe D. Lopez-Hilfiker, Pekka Rantala, and Tuukka Petäjä
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-901, https://doi.org/10.5194/acp-2021-901, 2021
Revised manuscript accepted for ACP
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Monoterpenes are emitted to the atmosphere by vegetation and by the use of certain consumer products. Reactions of monoterpenes in the atmosphere lead to low volatility products which condense to grow particulate matter or participate in new particle formation and thus affect air quality and climate. We use a model of atmospheric chemistry and transport to evaluate the global scale importance of recent updates to our understanding of monoterpene chemistry in particle formation and growth.
Mark F. Lunt, Alistair J. Manning, Grant Allen, Tim Arnold, Stéphane J.-B. Bauguitte, Hartmut Boesch, Anita L. Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon J. O'Doherty, Paul I. Palmer, Joseph R. Pitt, Chris Rennick, Daniel Say, Kieran M. Stanley, Ann R. Stavert, Dickon Young, and Matt Rigby
Atmos. Chem. Phys., 21, 16257–16276, https://doi.org/10.5194/acp-21-16257-2021, https://doi.org/10.5194/acp-21-16257-2021, 2021
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We present an evaluation of the UK's methane emissions between 2013 and 2020 using a network of tall tower measurement sites. We find emissions that are consistent in both magnitude and trend with the UK's reported emissions, with a declining trend driven by a decrease in emissions from England. The impact of various components of the modelling set-up on these findings are explored through a number of sensitivity studies.
Wendong Ge, Junfeng Liu, Kan Yi, Jiayu Xu, Yizhou Zhang, Xiurong Hu, Jianmin Ma, Xuejun Wang, Yi Wan, Jianying Hu, Zhaobin Zhang, Xilong Wang, and Shu Tao
Atmos. Chem. Phys., 21, 16093–16120, https://doi.org/10.5194/acp-21-16093-2021, https://doi.org/10.5194/acp-21-16093-2021, 2021
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Compared with the observations, the results incorporating detailed cloud aqueous-phase chemistry greatly reduced SO2 overestimation. The biases in annual simulated SO2 concentrations (or mixing ratios) decreased by 46 %, 41 %, and 22 % in Europe, the USA, and China, respectively. Fe chemistry and HOx chemistry contributed more to SO2 oxidation than N chemistry. Higher concentrations of soluble Fe and higher pH values could further enhance the oxidation capacity.
Stefanie Falk, Ane V. Vollsnes, Aud B. Eriksen, Frode Stordal, and Terje Koren Berntsen
Atmos. Chem. Phys., 21, 15647–15661, https://doi.org/10.5194/acp-21-15647-2021, https://doi.org/10.5194/acp-21-15647-2021, 2021
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We evaluate regional and global models for ozone modeling and damage risk mapping of vegetation over subarctic Europe. Our analysis suggests that low-resolution global models do not reproduce the observed ozone seasonal cycle at ground level, underestimating ozone by 30–50 %. High-resolution regional models capture the seasonal cycle well, still underestimating ozone by up to 20 %. Our proposed gap-filling method for site observations shows a 76 % accuracy compared to the regional model (80 %).
Linda Smoydzin and Peter Hoor
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-733, https://doi.org/10.5194/acp-2021-733, 2021
Revised manuscript accepted for ACP
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Our study presents a detailed analysis of the spatial and temporal distribution of elevated CO level in the upper troposphere over the Pacific using 20 years of MOPITT data. We create a climatology of severe pollution episodes and use trajectory calculations to link each particular pollution event detected in MOPITT satellite data with a distinct source region. Additionally we analyze uplift mechanisms such as wcb-related upward transport.
Zhe Peng, Julia Lee-Taylor, Harald Stark, John J. Orlando, Bernard Aumont, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 14649–14669, https://doi.org/10.5194/acp-21-14649-2021, https://doi.org/10.5194/acp-21-14649-2021, 2021
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We use the fully explicit GECKO-A model to study the OH reactivity (OHR) evolution in the NO-free photooxidation of several volatile organic compounds. Oxidation progressively produces more saturated and functionalized species, then breaks them into small species. OHR per C atom evolution is similar for different precursors once saturated multifunctional species are formed. We also find that partitioning of these species to chamber walls leads to large deviations in chambers from the atmosphere.
Philipp G. Eger, Luc Vereecken, Rolf Sander, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Ville Vakkari, Tuukka Petäjä, Jos Lelieveld, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 21, 14333–14349, https://doi.org/10.5194/acp-21-14333-2021, https://doi.org/10.5194/acp-21-14333-2021, 2021
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We determine the impact of pyruvic acid photolysis on the formation of acetaldehyde and peroxy radicals during summer and autumn in the Finnish boreal forest using a data-constrained box model. Our results are dependent on the chosen scenario in which the overall quantum yield and the photolysis products are varied. We highlight that pyruvic acid photolysis can be an important contributor to acetaldehyde and peroxy radical formation in remote, forested regions.
Bharat Rastogi, John B. Miller, Micheal Trudeau, Arlyn E. Andrews, Lei Hu, Marikate Mountain, Thomas Nehrkorn, Bianca Baier, Kathryn McKain, John Mund, Kaiyu Guan, and Caroline B. Alden
Atmos. Chem. Phys., 21, 14385–14401, https://doi.org/10.5194/acp-21-14385-2021, https://doi.org/10.5194/acp-21-14385-2021, 2021
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Predicting Earth's climate is difficult, partly due to uncertainty in forecasting how much CO2 can be removed by oceans and plants, because we cannot measure these exchanges directly on large scales. Satellites such as NASA's OCO-2 can provide part of the needed information, but data need to be highly precise and accurate. We evaluate these data and find small biases in certain months that are similar to the signals of interest. We argue that continued improvement of these data is necessary.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Volker Matthias, Markus Quante, Jan A. Arndt, Ronny Badeke, Lea Fink, Ronny Petrik, Josefine Feldner, Daniel Schwarzkopf, Eliza-Maria Link, Martin O. P. Ramacher, and Ralf Wedemann
Atmos. Chem. Phys., 21, 13931–13971, https://doi.org/10.5194/acp-21-13931-2021, https://doi.org/10.5194/acp-21-13931-2021, 2021
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COVID-19 lockdown measures in spring 2020 led to cleaner air in central Europe. Densely populated areas benefitted mainly from largely reduced NO2 concentrations, while rural areas experienced lower reductions in NO2 but also lower ozone concentrations. Very low particulate matter (PM) concentrations in parts of Europe were not an effect of lockdown measures. Model simulations show that modified weather conditions are more significant for ozone and PM than severe traffic emission reductions.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Ziwei Mo, Ru Cui, Bin Yuan, Huihua Cai, Brian C. McDonald, Meng Li, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 21, 13655–13666, https://doi.org/10.5194/acp-21-13655-2021, https://doi.org/10.5194/acp-21-13655-2021, 2021
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There is a lack of detailed understanding of NMVOC emissions from the use of volatile chemical products (VCPs) in China. This study used a mass balance method to compile a long-term emission inventory for solvent use (including coatings, adhesives, inks, pesticides, cleaners and personal care products) in China during 2000–2017. The striking growth and recent trend of solvent use NMVOC emissions can give important implications for air quality modeling and NMVOC control strategies in China.
Michael Sitwell and Mark Shephard
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-549, https://doi.org/10.5194/acp-2021-549, 2021
Revised manuscript accepted for ACP
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Observations of ammonia made using the satellite-borne CrIS instrument were used to improve the ammonia emissions used in the GEM-MACH model. These observations were used to refine estimates of the monthly mean ammonia emissions over North America for May to August 2016. The updated ammonia emissions reduced biases of GEM-MACH surface ammonia fields with surface observations and showed some improvements in the forecasting of species involved in inorganic particulate matter formation.
R. Anthony Cox, Markus Ammann, John N. Crowley, Paul T. Griffiths, Hartmut Herrmann, Erik H. Hoffmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Christopher J. Penkett, Andreas Tilgner, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 13011–13018, https://doi.org/10.5194/acp-21-13011-2021, https://doi.org/10.5194/acp-21-13011-2021, 2021
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The term open-air factor was coined in the 1960s, establishing that rural air had powerful germicidal properties possibly resulting from immediate products of the reaction of ozone with alkenes, unsaturated compounds ubiquitously present in natural and polluted environments. We have re-evaluated those early experiments, applying the recently substantially improved knowledge, and put them into the context of the lifetime of aerosol-borne pathogens that are so important in the Covid-19 pandemic.
Le Cao, Simeng Li, and Luhang Sun
Atmos. Chem. Phys., 21, 12687–12714, https://doi.org/10.5194/acp-21-12687-2021, https://doi.org/10.5194/acp-21-12687-2021, 2021
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Gas-phase chemical reaction mechanisms, e.g., CB6 mechanism, are essential parts of the atmospheric transport model. In order to better understand the changes caused by the updates between different versions of the CB6 mechanism, in this study, the behavior of three different CB6 mechanisms in simulating ozone, nitrogen oxides and formaldehyde under two different emission conditions was analyzed using a concentration sensitivity analysis, and the reasons causing the deviations were figured out.
Yi Yin, Frederic Chevallier, Philippe Ciais, Philippe Bousquet, Marielle Saunois, Bo Zheng, John Worden, A. Anthony Bloom, Robert J. Parker, Daniel J. Jacob, Edward J. Dlugokencky, and Christian Frankenberg
Atmos. Chem. Phys., 21, 12631–12647, https://doi.org/10.5194/acp-21-12631-2021, https://doi.org/10.5194/acp-21-12631-2021, 2021
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The growth of methane, the second-most important anthropogenic greenhouse gas after carbon dioxide, has been accelerating in recent years. Using an ensemble of multi-tracer atmospheric inversions constrained by surface or satellite observations, we show that global methane emissions increased by nearly 1 % per year from 2010–2017, with leading contributions from the tropics and East Asia.
Luke Surl, Tjarda Roberts, and Slimane Bekki
Atmos. Chem. Phys., 21, 12413–12441, https://doi.org/10.5194/acp-21-12413-2021, https://doi.org/10.5194/acp-21-12413-2021, 2021
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Many different chemical reactions happen when the gases from a volcano mix with air, but what effects do they have? We present aircraft measurements which show that there is less ozone within the plume of Etna than outside it. We have also made a computer model of this chemistry. This model can reproduce the effects seen when halogens (bromine and chlorine) are included in the volcanic emissions.
We look closely at the simulation to discover how complicated halogen reactions cause ozone loss.
Claire Lamotte, Jonathan Guth, Virginie Marécal, Martin Cussac, Paul David Hamer, Nicolas Theys, and Philipp Schneider
Atmos. Chem. Phys., 21, 11379–11404, https://doi.org/10.5194/acp-21-11379-2021, https://doi.org/10.5194/acp-21-11379-2021, 2021
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Improvements are made in a global chemical transfer model by considering a new volcanic SO2 emissions inventory, with more volcanoes referenced and more information on the altitude of injection. Better constraining volcanic emissions with this inventory improves the global, but mostly local, tropospheric sulfur composition. The tropospheric sulfur budget shows a nonlinearity to the volcanic contribution, especially to the sulfate aerosol burden and sulfur wet deposition.
Simon Rosanka, Bruno Franco, Lieven Clarisse, Pierre-François Coheur, Andrea Pozzer, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 11257–11288, https://doi.org/10.5194/acp-21-11257-2021, https://doi.org/10.5194/acp-21-11257-2021, 2021
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The strong El Niño in 2015 led to a particular dry season in Indonesia and favoured severe peatland fires. The smouldering conditions of these fires and the high carbon content of peat resulted in high volatile organic compound (VOC) emissions. By using a comprehensive atmospheric model, we show that these emissions have a significant impact on the tropospheric composition and oxidation capacity. These emissions are transported into to the lower stratosphere, resulting in a depletion of ozone.
Jianfeng Li, Yuhang Wang, Ruixiong Zhang, Charles Smeltzer, Andrew Weinheimer, Jay Herman, K. Folkert Boersma, Edward A. Celarier, Russell W. Long, James J. Szykman, Ruben Delgado, Anne M. Thompson, Travis N. Knepp, Lok N. Lamsal, Scott J. Janz, Matthew G. Kowalewski, Xiong Liu, and Caroline R. Nowlan
Atmos. Chem. Phys., 21, 11133–11160, https://doi.org/10.5194/acp-21-11133-2021, https://doi.org/10.5194/acp-21-11133-2021, 2021
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Comprehensive evaluations of simulated diurnal cycles of NO2 and NOy concentrations, vertical profiles, and tropospheric vertical column densities at two different resolutions with various measurements during the DISCOVER-AQ 2011 campaign show potential distribution biases of NOx emissions in the National Emissions Inventory 2011 at both 36 and 4 km resolutions, providing another possible explanation for the overestimation of model results.
Roman Nuterman, Alexander Mahura, Alexander Baklanov, Bjarne Amstrup, and Ashraf Zakey
Atmos. Chem. Phys., 21, 11099–11112, https://doi.org/10.5194/acp-21-11099-2021, https://doi.org/10.5194/acp-21-11099-2021, 2021
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The street air pollution is usually higher than the pollution at regional and urban scales. It mostly associated with both local emission sources and urban weather conditions. We present the downscaling system for regional, subregional-urban and street scales and evaluate it for acute air-pollution episode. Its evaluation showed a good prediction score across various spatiotemporal scales as well as feasibility of deterministic modelling approach for the operational street scale forecasting.
Min Huang, James H. Crawford, Joshua P. DiGangi, Gregory R. Carmichael, Kevin W. Bowman, Sujay V. Kumar, and Xiwu Zhan
Atmos. Chem. Phys., 21, 11013–11040, https://doi.org/10.5194/acp-21-11013-2021, https://doi.org/10.5194/acp-21-11013-2021, 2021
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This study evaluates the impact of satellite soil moisture data assimilation on modeled weather and ozone fields at various altitudes above the southeastern US during the summer. It emphasizes the importance of soil moisture in the understanding of surface ozone pollution and upper tropospheric chemistry, as well as air pollutants’ source–receptor relationships between the US and its downwind areas.
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Short summary
An assessment of mercury levels in air and deposition in the Athabasca oil sands region (AOSR) in Northern Alberta, Canada, was conducted to investigate the contribution of Hg emitted from oil sands activities to the surrounding landscape using a 3D process-based Hg model in 2012–2015. Oil sands Hg emissions are found to be important sources of Hg contamination to the local landscape in proximity to the processing activities, particularly in wintertime.
An assessment of mercury levels in air and deposition in the Athabasca oil sands region (AOSR)...
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