Articles | Volume 18, issue 5
https://doi.org/10.5194/acp-18-3387-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-18-3387-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
High-resolution quantification of atmospheric CO2 mixing ratios in the Greater Toronto Area, Canada
Stephanie C. Pugliese
University of Toronto, Department of Chemistry, 80 St. George St, Toronto, ON, M5S 3H6, Canada
Jennifer G. Murphy
CORRESPONDING AUTHOR
University of Toronto, Department of Chemistry, 80 St. George St, Toronto, ON, M5S 3H6, Canada
Felix R. Vogel
Laboratoire des Sciences du Climat et de L'Environnement, CEA-CNRS-UVSQ, Université de Paris-Saclay, France
Environment and Climate Change Canada, Climate Research Division, 4905 Dufferin St. Toronto, ON, M3H 5T4, Canada
Michael D. Moran
Environment and Climate Change Canada, Air Quality Research Division, 4905 Dufferin St. Toronto, ON, M3H 5T4, Canada
Junhua Zhang
Environment and Climate Change Canada, Air Quality Research Division, 4905 Dufferin St. Toronto, ON, M3H 5T4, Canada
Qiong Zheng
Environment and Climate Change Canada, Air Quality Research Division, 4905 Dufferin St. Toronto, ON, M3H 5T4, Canada
Craig A. Stroud
Environment and Climate Change Canada, Air Quality Research Division, 4905 Dufferin St. Toronto, ON, M3H 5T4, Canada
Shuzhan Ren
Environment and Climate Change Canada, Air Quality Research Division, 4905 Dufferin St. Toronto, ON, M3H 5T4, Canada
Douglas Worthy
Environment and Climate Change Canada, Climate Research Division, 4905 Dufferin St. Toronto, ON, M3H 5T4, Canada
Gregoire Broquet
Laboratoire des Sciences du Climat et de L'Environnement, CEA-CNRS-UVSQ, Université de Paris-Saclay, France
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Atmos. Chem. Phys., 24, 10013–10038, https://doi.org/10.5194/acp-24-10013-2024, https://doi.org/10.5194/acp-24-10013-2024, 2024
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EGUsphere, https://doi.org/10.5194/egusphere-2024-2371, https://doi.org/10.5194/egusphere-2024-2371, 2024
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Atmos. Chem. Phys., 24, 8139–8163, https://doi.org/10.5194/acp-24-8139-2024, https://doi.org/10.5194/acp-24-8139-2024, 2024
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Rodrigo Rivera-Martinez, Pramod Kumar, Olivier Laurent, Gregoire Broquet, Christopher Caldow, Ford Cropley, Diego Santaren, Adil Shah, Cécile Mallet, Michel Ramonet, Leonard Rivier, Catherine Juery, Olivier Duclaux, Caroline Bouchet, Elisa Allegrini, Hervé Utard, and Philippe Ciais
Atmos. Meas. Tech., 17, 4257–4290, https://doi.org/10.5194/amt-17-4257-2024, https://doi.org/10.5194/amt-17-4257-2024, 2024
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Audrey Fortems-Cheiney, Gregoire Broquet, Elise Potier, Robin Plauchu, Antoine Berchet, Isabelle Pison, Hugo Denier van der Gon, and Stijn Dellaert
Atmos. Chem. Phys., 24, 4635–4649, https://doi.org/10.5194/acp-24-4635-2024, https://doi.org/10.5194/acp-24-4635-2024, 2024
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Atmos. Meas. Tech., 17, 1633–1649, https://doi.org/10.5194/amt-17-1633-2024, https://doi.org/10.5194/amt-17-1633-2024, 2024
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Joffrey Dumont Le Brazidec, Pierre Vanderbecken, Alban Farchi, Grégoire Broquet, Gerrit Kuhlmann, and Marc Bocquet
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Atmos. Meas. Tech., 17, 1229–1250, https://doi.org/10.5194/amt-17-1229-2024, https://doi.org/10.5194/amt-17-1229-2024, 2024
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Douglas E. J. Worthy, Michele K. Rauh, Lin Huang, Felix R. Vogel, Alina Chivulescu, Kenneth A. Masarie, Ray L. Langenfelds, Paul B. Krummel, Colin E. Allison, Andrew M. Crotwell, Monica Madronich, Gabrielle Pétron, Ingeborg Levin, Samuel Hammer, Sylvia Michel, Michel Ramonet, Martina Schmidt, Armin Jordan, Heiko Moossen, Michael Rothe, Ralph Keeling, and Eric J. Morgan
Atmos. Meas. Tech., 16, 5909–5935, https://doi.org/10.5194/amt-16-5909-2023, https://doi.org/10.5194/amt-16-5909-2023, 2023
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Network compatibility is important for inferring greenhouse gas fluxes at global or regional scales. This study is the first assessment of the measurement agreement among seven individual programs within the World Meteorological Organization community. It compares co-located flask air measurements at the Alert Observatory in Canada over a 17-year period. The results provide stronger confidence in the uncertainty estimation while using those datasets in various data interpretation applications.
Alexandre Danjou, Grégoire Broquet, Andrew Schuh, François-Marie Bréon, and Thomas Lauvaux
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2023-199, https://doi.org/10.5194/amt-2023-199, 2023
Revised manuscript has not been submitted
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We study the capacity of XCO2 space-borne imagery to estimate urban CO2 emissions with synthetic data. We define automatic and standard methods, and objective criteria for image selection. Wind variability and urban emission budget guide the emission estimation error. Images with low wind variability and high urban emissions account for 47 % of images and give a bias on the emission estimation of -7 % of the emissions and a spread of 56 %. Other images give a bias of -31 % and a spread of 99 %.
Matthew J. McGrath, Ana Maria Roxana Petrescu, Philippe Peylin, Robbie M. Andrew, Bradley Matthews, Frank Dentener, Juraj Balkovič, Vladislav Bastrikov, Meike Becker, Gregoire Broquet, Philippe Ciais, Audrey Fortems-Cheiney, Raphael Ganzenmüller, Giacomo Grassi, Ian Harris, Matthew Jones, Jürgen Knauer, Matthias Kuhnert, Guillaume Monteil, Saqr Munassar, Paul I. Palmer, Glen P. Peters, Chunjing Qiu, Mart-Jan Schelhaas, Oksana Tarasova, Matteo Vizzarri, Karina Winkler, Gianpaolo Balsamo, Antoine Berchet, Peter Briggs, Patrick Brockmann, Frédéric Chevallier, Giulia Conchedda, Monica Crippa, Stijn N. C. Dellaert, Hugo A. C. Denier van der Gon, Sara Filipek, Pierre Friedlingstein, Richard Fuchs, Michael Gauss, Christoph Gerbig, Diego Guizzardi, Dirk Günther, Richard A. Houghton, Greet Janssens-Maenhout, Ronny Lauerwald, Bas Lerink, Ingrid T. Luijkx, Géraud Moulas, Marilena Muntean, Gert-Jan Nabuurs, Aurélie Paquirissamy, Lucia Perugini, Wouter Peters, Roberto Pilli, Julia Pongratz, Pierre Regnier, Marko Scholze, Yusuf Serengil, Pete Smith, Efisio Solazzo, Rona L. Thompson, Francesco N. Tubiello, Timo Vesala, and Sophia Walther
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Accurate estimation of fluxes of carbon dioxide from the land surface is essential for understanding future impacts of greenhouse gas emissions on the climate system. A wide variety of methods currently exist to estimate these sources and sinks. We are continuing work to develop annual comparisons of these diverse methods in order to clarify what they all actually calculate and to resolve apparent disagreement, in addition to highlighting opportunities for increased understanding.
Lawson David Gillespie, Sébastien Ars, James Phillip Williams, Louise Klotz, Tianjie Feng, Stephanie Gu, Mishaal Kandapath, Amy Mann, Michael Raczkowski, Mary Kang, Felix Vogel, and Debra Wunch
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Preprint withdrawn
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We investigate techniques for calculating emissions from mobile in situ gas concentrations recorded during downwind plume transects. We find that using the enhancement area to estimate emissions is the most consistent method when comparing different setups and instruments. Observations from a multi year urban methane survey and controlled release experiment are analyzed, and emissions rates for combined sewage overflow basins and a large wastewater treatment plant in Toronto are calculated.
Jinghui Lian, Thomas Lauvaux, Hervé Utard, François-Marie Bréon, Grégoire Broquet, Michel Ramonet, Olivier Laurent, Ivonne Albarus, Mali Chariot, Simone Kotthaus, Martial Haeffelin, Olivier Sanchez, Olivier Perrussel, Hugo Anne Denier van der Gon, Stijn Nicolaas Camiel Dellaert, and Philippe Ciais
Atmos. Chem. Phys., 23, 8823–8835, https://doi.org/10.5194/acp-23-8823-2023, https://doi.org/10.5194/acp-23-8823-2023, 2023
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This study quantifies urban CO2 emissions via an atmospheric inversion for the Paris metropolitan area over a 6-year period from 2016 to 2021. Results show a long-term decreasing trend of about 2 % ± 0.6 % per year in the annual CO2 emissions over Paris. We conclude that our current capacity can deliver near-real-time CO2 emission estimates at the city scale in under a month, and the results agree within 10 % with independent estimates from multiple city-scale inventories.
Joffrey Dumont Le Brazidec, Pierre Vanderbecken, Alban Farchi, Marc Bocquet, Jinghui Lian, Grégoire Broquet, Gerrit Kuhlmann, Alexandre Danjou, and Thomas Lauvaux
Geosci. Model Dev., 16, 3997–4016, https://doi.org/10.5194/gmd-16-3997-2023, https://doi.org/10.5194/gmd-16-3997-2023, 2023
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Monitoring of CO2 emissions is key to the development of reduction policies. Local emissions, from cities or power plants, may be estimated from CO2 plumes detected in satellite images. CO2 plumes generally have a weak signal and are partially concealed by highly variable background concentrations and instrument errors, which hampers their detection. To address this problem, we propose and apply deep learning methods to detect the contour of a plume in simulated CO2 satellite images.
Adil Shah, Olivier Laurent, Luc Lienhardt, Grégoire Broquet, Rodrigo Rivera Martinez, Elisa Allegrini, and Philippe Ciais
Atmos. Meas. Tech., 16, 3391–3419, https://doi.org/10.5194/amt-16-3391-2023, https://doi.org/10.5194/amt-16-3391-2023, 2023
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As methane (CH4) contributes to global warming, more CH4 measurements are required to better characterise source emissions. Hence, we tested a cheap CH4 sensor for 338 d of landfill sampling. We derived an excellent CH4 response model in a stable environment. However, different types of air with the same CH4 level had diverse sensor responses. We characterised temperature and water vapour response but could not replicate field sampling. Thus, other species may cause sensor interactions.
Monica Crippa, Diego Guizzardi, Tim Butler, Terry Keating, Rosa Wu, Jacek Kaminski, Jeroen Kuenen, Junichi Kurokawa, Satoru Chatani, Tazuko Morikawa, George Pouliot, Jacinthe Racine, Michael D. Moran, Zbigniew Klimont, Patrick M. Manseau, Rabab Mashayekhi, Barron H. Henderson, Steven J. Smith, Harrison Suchyta, Marilena Muntean, Efisio Solazzo, Manjola Banja, Edwin Schaaf, Federico Pagani, Jung-Hun Woo, Jinseok Kim, Fabio Monforti-Ferrario, Enrico Pisoni, Junhua Zhang, David Niemi, Mourad Sassi, Tabish Ansari, and Kristen Foley
Earth Syst. Sci. Data, 15, 2667–2694, https://doi.org/10.5194/essd-15-2667-2023, https://doi.org/10.5194/essd-15-2667-2023, 2023
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This study responds to the global and regional atmospheric modelling community's need for a mosaic of air pollutant emissions with global coverage, long time series, spatially distributed data at a high time resolution, and a high sectoral resolution in order to enhance the understanding of transboundary air pollution. The mosaic approach to integrating official regional emission inventories with a global inventory based on a consistent methodology ensures policy-relevant results.
Rodrigo Andres Rivera Martinez, Diego Santaren, Olivier Laurent, Gregoire Broquet, Ford Cropley, Cécile Mallet, Michel Ramonet, Adil Shah, Leonard Rivier, Caroline Bouchet, Catherine Juery, Olivier Duclaux, and Philippe Ciais
Atmos. Meas. Tech., 16, 2209–2235, https://doi.org/10.5194/amt-16-2209-2023, https://doi.org/10.5194/amt-16-2209-2023, 2023
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A network of low-cost sensors is a good alternative to improve the detection of fugitive CH4 emissions. We present the results of four tests conducted with two types of Figaro sensors that were assembled on four chambers in a laboratory experiment: a comparison of five models to reconstruct the CH4 signal, a strategy to reduce the training set size, a detection of age effects in the sensors and a test of the capability to transfer a model between chambers for the same type of sensor.
Pierre J. Vanderbecken, Joffrey Dumont Le Brazidec, Alban Farchi, Marc Bocquet, Yelva Roustan, Élise Potier, and Grégoire Broquet
Atmos. Meas. Tech., 16, 1745–1766, https://doi.org/10.5194/amt-16-1745-2023, https://doi.org/10.5194/amt-16-1745-2023, 2023
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Instruments dedicated to monitoring atmospheric gaseous compounds from space will provide images of urban-scale plumes. We discuss here the use of new metrics to compare observed plumes with model predictions that will be less sensitive to meteorology uncertainties. We have evaluated our metrics on diverse plumes and shown that by eliminating some aspects of the discrepancies, they are indeed less sensitive to meteorological variations.
Nasrin Mostafavi Pak, Jacob K. Hedelius, Sébastien Roche, Liz Cunningham, Bianca Baier, Colm Sweeney, Coleen Roehl, Joshua Laughner, Geoffrey Toon, Paul Wennberg, Harrison Parker, Colin Arrowsmith, Joseph Mendonca, Pierre Fogal, Tyler Wizenberg, Beatriz Herrera, Kimberly Strong, Kaley A. Walker, Felix Vogel, and Debra Wunch
Atmos. Meas. Tech., 16, 1239–1261, https://doi.org/10.5194/amt-16-1239-2023, https://doi.org/10.5194/amt-16-1239-2023, 2023
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Ground-based remote sensing instruments in the Total Carbon Column Observing Network (TCCON) measure greenhouse gases in the atmosphere. Consistency between TCCON measurements is crucial to accurately infer changes in atmospheric composition. We use portable remote sensing instruments (EM27/SUN) to evaluate biases between TCCON stations in North America. We also improve the retrievals of EM27/SUN instruments and evaluate the previous (GGG2014) and newest (GGG2020) retrieval algorithms.
Shuzhan Ren and Craig A. Stroud
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2023-37, https://doi.org/10.5194/acp-2023-37, 2023
Revised manuscript not accepted
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The atmospheric boundary layer height is involved in the turbulence parameterization scheme employed in numerical models. It affects the concentration of chemical species by changing the vertical diffusivity and the volume of tracer in the atmosphere. There exists large uncertainties in the boundary layer height. The impacts of the uncertainties on the model simulation of concentration of chemical species are examined. The results show different impacts in different parameterization scheme.
Elise Potier, Grégoire Broquet, Yilong Wang, Diego Santaren, Antoine Berchet, Isabelle Pison, Julia Marshall, Philippe Ciais, François-Marie Bréon, and Frédéric Chevallier
Atmos. Meas. Tech., 15, 5261–5288, https://doi.org/10.5194/amt-15-5261-2022, https://doi.org/10.5194/amt-15-5261-2022, 2022
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Atmospheric inversion at local–regional scales over Europe and pseudo-data assimilation are used to evaluate how CO2 and 14CO2 ground-based measurement networks could complement satellite CO2 imagers to monitor fossil fuel (FF) CO2 emissions. This combination significantly improves precision in the FF emission estimates in areas with a dense network but does not strongly support the separation of the FF from the biogenic signals or the spatio-temporal extrapolation of the satellite information.
Anthony Rey-Pommier, Frédéric Chevallier, Philippe Ciais, Grégoire Broquet, Theodoros Christoudias, Jonilda Kushta, Didier Hauglustaine, and Jean Sciare
Atmos. Chem. Phys., 22, 11505–11527, https://doi.org/10.5194/acp-22-11505-2022, https://doi.org/10.5194/acp-22-11505-2022, 2022
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Emission inventories for air pollutants can be uncertain in developing countries. In order to overcome these uncertainties, we model nitrogen oxide emissions in Egypt using satellite retrievals. We detect a weekly cycle reflecting Egyptian social norms, an annual cycle consistent with electricity consumption and an activity drop due to the COVID-19 pandemic. However, discrepancies with inventories remain high, illustrating the needs for additional data to improve the potential of our method.
Carlos Alberti, Frank Hase, Matthias Frey, Darko Dubravica, Thomas Blumenstock, Angelika Dehn, Paolo Castracane, Gregor Surawicz, Roland Harig, Bianca C. Baier, Caroline Bès, Jianrong Bi, Hartmut Boesch, André Butz, Zhaonan Cai, Jia Chen, Sean M. Crowell, Nicholas M. Deutscher, Dragos Ene, Jonathan E. Franklin, Omaira García, David Griffith, Bruno Grouiez, Michel Grutter, Abdelhamid Hamdouni, Sander Houweling, Neil Humpage, Nicole Jacobs, Sujong Jeong, Lilian Joly, Nicholas B. Jones, Denis Jouglet, Rigel Kivi, Ralph Kleinschek, Morgan Lopez, Diogo J. Medeiros, Isamu Morino, Nasrin Mostafavipak, Astrid Müller, Hirofumi Ohyama, Paul I. Palmer, Mahesh Pathakoti, David F. Pollard, Uwe Raffalski, Michel Ramonet, Robbie Ramsay, Mahesh Kumar Sha, Kei Shiomi, William Simpson, Wolfgang Stremme, Youwen Sun, Hiroshi Tanimoto, Yao Té, Gizaw Mengistu Tsidu, Voltaire A. Velazco, Felix Vogel, Masataka Watanabe, Chong Wei, Debra Wunch, Marcia Yamasoe, Lu Zhang, and Johannes Orphal
Atmos. Meas. Tech., 15, 2433–2463, https://doi.org/10.5194/amt-15-2433-2022, https://doi.org/10.5194/amt-15-2433-2022, 2022
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Space-borne greenhouse gas missions require ground-based validation networks capable of providing fiducial reference measurements. Here, considerable refinements of the calibration procedures for the COllaborative Carbon Column Observing Network (COCCON) are presented. Laboratory and solar side-by-side procedures for the characterization of the spectrometers have been refined and extended. Revised calibration factors for XCO2, XCO and XCH4 are provided, incorporating 47 new spectrometers.
Makoto Saito, Tomohiro Shiraishi, Ryuichi Hirata, Yosuke Niwa, Kazuyuki Saito, Martin Steinbacher, Doug Worthy, and Tsuneo Matsunaga
Biogeosciences, 19, 2059–2078, https://doi.org/10.5194/bg-19-2059-2022, https://doi.org/10.5194/bg-19-2059-2022, 2022
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This study tested combinations of two sources of AGB data and two sources of LCC data and used the same burned area satellite data to estimate BB CO emissions. Our analysis showed large discrepancies in annual mean CO emissions and explicit differences in the simulated CO concentrations among the BB emissions estimates. This study has confirmed that BB emissions estimates are sensitive to the land surface information on which they are based.
Regina Gonzalez Moguel, Felix Vogel, Sébastien Ars, Hinrich Schaefer, Jocelyn C. Turnbull, and Peter M. J. Douglas
Atmos. Chem. Phys., 22, 2121–2133, https://doi.org/10.5194/acp-22-2121-2022, https://doi.org/10.5194/acp-22-2121-2022, 2022
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Evaluating methane (CH4) sources in the Athabasca oil sands region (AOSR) is crucial to effectively mitigate CH4 emissions. We tested the use of carbon isotopes to estimate source contributions from key CH4 sources in the AOSR and found that 56 ± 18 % of CH4 emissions originated from surface mining and processing facilities, 34 ± 18 % from tailings ponds, and 10 ± < 1 % from wetlands, confirming previous findings and showing that this method can be successfully used to partition CH4 sources.
Mahtab Majdzadeh, Craig A. Stroud, Christopher Sioris, Paul A. Makar, Ayodeji Akingunola, Chris McLinden, Xiaoyi Zhao, Michael D. Moran, Ihab Abboud, and Jack Chen
Geosci. Model Dev., 15, 219–249, https://doi.org/10.5194/gmd-15-219-2022, https://doi.org/10.5194/gmd-15-219-2022, 2022
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A new lookup table for aerosol optical properties based on a Mie scattering code was calculated and adopted within an improved version of the photolysis module in the GEM-MACH in-line chemical transport model. The modified version of the photolysis module makes use of online interactive aerosol feedback and applies core-shell parameterizations to the black carbon absorption efficiency based on Bond et al. (2006) to the size bins with black carbon mass fraction of less than 40 %.
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.
Dandan Wei, Hariprasad D. Alwe, Dylan B. Millet, Brandon Bottorff, Michelle Lew, Philip S. Stevens, Joshua D. Shutter, Joshua L. Cox, Frank N. Keutsch, Qianwen Shi, Sarah C. Kavassalis, Jennifer G. Murphy, Krystal T. Vasquez, Hannah M. Allen, Eric Praske, John D. Crounse, Paul O. Wennberg, Paul B. Shepson, Alexander A. T. Bui, Henry W. Wallace, Robert J. Griffin, Nathaniel W. May, Megan Connor, Jonathan H. Slade, Kerri A. Pratt, Ezra C. Wood, Mathew Rollings, Benjamin L. Deming, Daniel C. Anderson, and Allison L. Steiner
Geosci. Model Dev., 14, 6309–6329, https://doi.org/10.5194/gmd-14-6309-2021, https://doi.org/10.5194/gmd-14-6309-2021, 2021
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Over the past decade, understanding of isoprene oxidation has improved, and proper representation of isoprene oxidation and isoprene-derived SOA (iSOA) formation in canopy–chemistry models is now recognized to be important for an accurate understanding of forest–atmosphere exchange. The updated FORCAsT version 2.0 improves the estimation of some isoprene oxidation products and is one of the few canopy models currently capable of simulating SOA formation from monoterpenes and isoprene.
Pramod Kumar, Grégoire Broquet, Camille Yver-Kwok, Olivier Laurent, Susan Gichuki, Christopher Caldow, Ford Cropley, Thomas Lauvaux, Michel Ramonet, Guillaume Berthe, Frédéric Martin, Olivier Duclaux, Catherine Juery, Caroline Bouchet, and Philippe Ciais
Atmos. Meas. Tech., 14, 5987–6003, https://doi.org/10.5194/amt-14-5987-2021, https://doi.org/10.5194/amt-14-5987-2021, 2021
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This study presents a simple atmospheric inversion modeling framework for the localization and quantification of unknown CH4 and CO2 emissions from point sources based on near-surface mobile concentration measurements and a Gaussian plume dispersion model. It is applied for the estimate of a series of brief controlled releases of CH4 and CO2 with a wide range of rates during the TOTAL TADI-2018 experiment. Results indicate a ~10 %–40 % average error on the estimate of the release rates.
Ashu Dastoor, Andrei Ryjkov, Gregor Kos, Junhua Zhang, Jane Kirk, Matthew Parsons, and Alexandra Steffen
Atmos. Chem. Phys., 21, 12783–12807, https://doi.org/10.5194/acp-21-12783-2021, https://doi.org/10.5194/acp-21-12783-2021, 2021
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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.
Antoine Berchet, Espen Sollum, Rona L. Thompson, Isabelle Pison, Joël Thanwerdas, Grégoire Broquet, Frédéric Chevallier, Tuula Aalto, Adrien Berchet, Peter Bergamaschi, Dominik Brunner, Richard Engelen, Audrey Fortems-Cheiney, Christoph Gerbig, Christine D. Groot Zwaaftink, Jean-Matthieu Haussaire, Stephan Henne, Sander Houweling, Ute Karstens, Werner L. Kutsch, Ingrid T. Luijkx, Guillaume Monteil, Paul I. Palmer, Jacob C. A. van Peet, Wouter Peters, Philippe Peylin, Elise Potier, Christian Rödenbeck, Marielle Saunois, Marko Scholze, Aki Tsuruta, and Yuanhong Zhao
Geosci. Model Dev., 14, 5331–5354, https://doi.org/10.5194/gmd-14-5331-2021, https://doi.org/10.5194/gmd-14-5331-2021, 2021
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We present here the Community Inversion Framework (CIF) to help rationalize development efforts and leverage the strengths of individual inversion systems into a comprehensive framework. The CIF is a programming protocol to allow various inversion bricks to be exchanged among researchers.
The ensemble of bricks makes a flexible, transparent and open-source Python-based tool. We describe the main structure and functionalities and demonstrate it in a simple academic case.
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.
Jinghui Lian, François-Marie Bréon, Grégoire Broquet, Thomas Lauvaux, Bo Zheng, Michel Ramonet, Irène Xueref-Remy, Simone Kotthaus, Martial Haeffelin, and Philippe Ciais
Atmos. Chem. Phys., 21, 10707–10726, https://doi.org/10.5194/acp-21-10707-2021, https://doi.org/10.5194/acp-21-10707-2021, 2021
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Currently there is growing interest in monitoring city-scale CO2 emissions based on atmospheric CO2 measurements, atmospheric transport modeling, and inversion technique. We analyze the various sources of uncertainty that impact the atmospheric CO2 modeling and that may compromise the potential of this method for the monitoring of CO2 emission over Paris. Results suggest selection criteria for the assimilation of CO2 measurements into the inversion system that aims at retrieving city emissions.
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.
Ana Maria Roxana Petrescu, Matthew J. McGrath, Robbie M. Andrew, Philippe Peylin, Glen P. Peters, Philippe Ciais, Gregoire Broquet, Francesco N. Tubiello, Christoph Gerbig, Julia Pongratz, Greet Janssens-Maenhout, Giacomo Grassi, Gert-Jan Nabuurs, Pierre Regnier, Ronny Lauerwald, Matthias Kuhnert, Juraj Balkovič, Mart-Jan Schelhaas, Hugo A. C. Denier van der
Gon, Efisio Solazzo, Chunjing Qiu, Roberto Pilli, Igor B. Konovalov, Richard A. Houghton, Dirk Günther, Lucia Perugini, Monica Crippa, Raphael Ganzenmüller, Ingrid T. Luijkx, Pete Smith, Saqr Munassar, Rona L. Thompson, Giulia Conchedda, Guillaume Monteil, Marko Scholze, Ute Karstens, Patrick Brockmann, and Albertus Johannes Dolman
Earth Syst. Sci. Data, 13, 2363–2406, https://doi.org/10.5194/essd-13-2363-2021, https://doi.org/10.5194/essd-13-2363-2021, 2021
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This study is topical and provides a state-of-the-art scientific overview of data availability from bottom-up and top-down CO2 fossil emissions and CO2 land fluxes in the EU27+UK. The data integrate recent emission inventories with ecosystem data, land carbon models and regional/global inversions for the European domain, aiming at reconciling CO2 estimates with official country-level UNFCCC national GHG inventories in support to policy and facilitating real-time verification procedures.
Amy Hrdina, Jennifer G. Murphy, Anna Gannet Hallar, John C. Lin, Alexander Moravek, Ryan Bares, Ross C. Petersen, Alessandro Franchin, Ann M. Middlebrook, Lexie Goldberger, Ben H. Lee, Munkh Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 21, 8111–8126, https://doi.org/10.5194/acp-21-8111-2021, https://doi.org/10.5194/acp-21-8111-2021, 2021
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Wintertime air pollution in the Salt Lake Valley is primarily composed of ammonium nitrate, which is formed when gas-phase ammonia and nitric acid react. The major point in this work is that the chemical composition of snow tells a very different story to what we measured in the atmosphere. With the dust–sea salt cations observed in PM2.5 and particle sizing data, we can estimate how much nitric acid may be lost to dust–sea salt that is not accounted for and how much more PM2.5 this could form.
Audrey Fortems-Cheiney, Isabelle Pison, Grégoire Broquet, Gaëlle Dufour, Antoine Berchet, Elise Potier, Adriana Coman, Guillaume Siour, and Lorenzo Costantino
Geosci. Model Dev., 14, 2939–2957, https://doi.org/10.5194/gmd-14-2939-2021, https://doi.org/10.5194/gmd-14-2939-2021, 2021
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Up-to-date and accurate emission inventories for air pollutants are essential for understanding their role in the formation of tropospheric ozone and particulate matter, for anticipating pollution peaks and for identifying the key drivers that could help mitigate their emissions. Complementarily with bottom-up inventories, the system described here aims at updating and improving the knowledge on the high spatiotemporal variability of emissions of air pollutants.
Diego Santaren, Grégoire Broquet, François-Marie Bréon, Frédéric Chevallier, Denis Siméoni, Bo Zheng, and Philippe Ciais
Atmos. Meas. Tech., 14, 403–433, https://doi.org/10.5194/amt-14-403-2021, https://doi.org/10.5194/amt-14-403-2021, 2021
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Atmospheric transport inversions with synthetic data are used to assess the potential of new satellite observations of atmospheric CO2 to monitor anthropogenic emissions from regions, cities and large industrial plants. The analysis, applied to a large ensemble of sources in western Europe, shows a strong dependence of the results on different characteristics of the spaceborne instrument, on the source emission budgets and spreads, and on the wind conditions.
Yilong Wang, Grégoire Broquet, François-Marie Bréon, Franck Lespinas, Michael Buchwitz, Maximilian Reuter, Yasjka Meijer, Armin Loescher, Greet Janssens-Maenhout, Bo Zheng, and Philippe Ciais
Geosci. Model Dev., 13, 5813–5831, https://doi.org/10.5194/gmd-13-5813-2020, https://doi.org/10.5194/gmd-13-5813-2020, 2020
Guillaume Monteil, Grégoire Broquet, Marko Scholze, Matthew Lang, Ute Karstens, Christoph Gerbig, Frank-Thomas Koch, Naomi E. Smith, Rona L. Thompson, Ingrid T. Luijkx, Emily White, Antoon Meesters, Philippe Ciais, Anita L. Ganesan, Alistair Manning, Michael Mischurow, Wouter Peters, Philippe Peylin, Jerôme Tarniewicz, Matt Rigby, Christian Rödenbeck, Alex Vermeulen, and Evie M. Walton
Atmos. Chem. Phys., 20, 12063–12091, https://doi.org/10.5194/acp-20-12063-2020, https://doi.org/10.5194/acp-20-12063-2020, 2020
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The paper presents the first results from the EUROCOM project, a regional atmospheric inversion intercomparison exercise involving six European research groups. It aims to produce an estimate of the net carbon flux between the European terrestrial ecosystems and the atmosphere for the period 2006–2015, based on constraints provided by observed CO2 concentrations and using inverse modelling techniques. The use of six different models enables us to investigate the robustness of the results.
Bo Zheng, Frédéric Chevallier, Philippe Ciais, Grégoire Broquet, Yilong Wang, Jinghui Lian, and Yuanhong Zhao
Atmos. Chem. Phys., 20, 8501–8510, https://doi.org/10.5194/acp-20-8501-2020, https://doi.org/10.5194/acp-20-8501-2020, 2020
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The Paris Climate Agreement requires all parties to report CO2 emissions regularly. Given the self-reporting nature of this system, it is critical to evaluate the emission reports with independent observation systems. Here we present the direct observations of city CO2 plumes from space and the quantification of CO2 emissions from these observations over the largest emitter country China. The emissions from 46 hot-spot regions representing 13 % of China's total emissions can be well constrained.
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
Atmos. Meas. Tech., 13, 2241–2255, https://doi.org/10.5194/amt-13-2241-2020, https://doi.org/10.5194/amt-13-2241-2020, 2020
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The sustainable support of radon metrology at the environmental level offers new scientific possibilities for the quantification of greenhouse gas (GHG) emissions and the determination of their source terms as well as for the identification of radioactive sources for the assessment of radiation exposure. This study helps to harmonize the techniques commonly used for atmospheric radon and radon progeny activity concentration measurements.
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.
Alexander Moravek, Jennifer G. Murphy, Amy Hrdina, John C. Lin, Christopher Pennell, Alessandro Franchin, Ann M. Middlebrook, Dorothy L. Fibiger, Caroline C. Womack, Erin E. McDuffie, Randal Martin, Kori Moore, Munkhbayar Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 19, 15691–15709, https://doi.org/10.5194/acp-19-15691-2019, https://doi.org/10.5194/acp-19-15691-2019, 2019
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Ammonium nitrate is a major component of fine particulate matter of wintertime air pollution in the Great Salt Lake Region (UT, USA). We investigate the sources of ammonia in the region by using aircraft observations and comparing them to modelled ammonia mixing ratios based on emission inventory estimates. The results suggest that ammonia emissions are underestimated, specifically in regions with high agricultural activity, while ammonia in Salt Lake City is mainly of local origin.
Gerrit Kuhlmann, Grégoire Broquet, Julia Marshall, Valentin Clément, Armin Löscher, Yasjka Meijer, and Dominik Brunner
Atmos. Meas. Tech., 12, 6695–6719, https://doi.org/10.5194/amt-12-6695-2019, https://doi.org/10.5194/amt-12-6695-2019, 2019
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The Copernicus Anthropogenic CO2 Monitoring (CO2M) mission is a proposed constellation of imaging satellites with a CO2 instrument as main payload and optionally instruments for NO2, CO and aerosols. This study demonstrates the huge benefit of an NO2 instrument for detecting city plumes and weak point sources. Its main advantages are the higher signal-to-noise ratio and the lower sensitivity to clouds that significantly increases the number of observations available for quantifying CO2 emission.
Roya Ghahreman, Wanmin Gong, Martí Galí, Ann-Lise Norman, Stephen R. Beagley, Ayodeji Akingunola, Qiong Zheng, Alexandru Lupu, Martine Lizotte, Maurice Levasseur, and W. Richard Leaitch
Atmos. Chem. Phys., 19, 14455–14476, https://doi.org/10.5194/acp-19-14455-2019, https://doi.org/10.5194/acp-19-14455-2019, 2019
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Atmospheric DMS(g) is a climatically important compound and the main source of biogenic sulfate in the Arctic. Its abundance in the Arctic increases during summer due to greater ice-free sea surface and higher biological activity. In this study, we implemented DMS(g) in a regional air quality forecast model configured for the Arctic. The study showed a significant impact from DMS(g) on sulfate aerosols, particularly in the 50–100 nm size range, in the Arctic marine boundary layer during summer.
Alexander Moravek, Saumya Singh, Elizabeth Pattey, Luc Pelletier, and Jennifer G. Murphy
Atmos. Meas. Tech., 12, 6059–6078, https://doi.org/10.5194/amt-12-6059-2019, https://doi.org/10.5194/amt-12-6059-2019, 2019
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Determination of ecosystem exchange fluxes using the eddy covariance technique requires measurements with a fast time response. For ammonia, the time response is limited by adsorption and desorption processes on instrument surfaces, generally leading to a substantial underestimation of fluxes. Based on a 5-month flux dataset, we propose a new method to correct for the ammonia flux loss that is better suited to account for factors like surface aging and contamination than other approaches.
Jinghui Lian, François-Marie Bréon, Grégoire Broquet, T. Scott Zaccheo, Jeremy Dobler, Michel Ramonet, Johannes Staufer, Diego Santaren, Irène Xueref-Remy, and Philippe Ciais
Atmos. Chem. Phys., 19, 13809–13825, https://doi.org/10.5194/acp-19-13809-2019, https://doi.org/10.5194/acp-19-13809-2019, 2019
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CO2 emissions within urban areas impact nearby and downwind concentrations. A different system, based on bi-wavelength laser measurements, has been deployed over Paris. It samples CO2 concentrations along horizontal lines, between a transceiver and a reflector. In this paper, we analyze the measurements provided by this system, together with the more classical in situ sampling and high-resolution modeling. We focus on the temporal and spatial variability of atmospheric CO2 concentrations.
Xiaoyi Zhao, Debora Griffin, Vitali Fioletov, Chris McLinden, Jonathan Davies, Akira Ogyu, Sum Chi Lee, Alexandru Lupu, Michael D. Moran, Alexander Cede, Martin Tiefengraber, and Moritz Müller
Atmos. Chem. Phys., 19, 10619–10642, https://doi.org/10.5194/acp-19-10619-2019, https://doi.org/10.5194/acp-19-10619-2019, 2019
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New nitrogen dioxide (NO2) retrieval algorithms are developed for Pandora zenith-sky measurements. A column-to-surface conversion look-up table was produced for the Pandora instruments; therefore, quick and practical Pandora-based surface NO2 concentration data can be obtained for air quality monitoring purposes. It is demonstrated that the surface NO2 concentration is controlled not only by the planetary boundary layer height but also by both boundary layer dynamics and photochemistry.
Jack Chen, Kerry Anderson, Radenko Pavlovic, Michael D. Moran, Peter Englefield, Dan K. Thompson, Rodrigo Munoz-Alpizar, and Hugo Landry
Geosci. Model Dev., 12, 3283–3310, https://doi.org/10.5194/gmd-12-3283-2019, https://doi.org/10.5194/gmd-12-3283-2019, 2019
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Emissions from wildland fires can cause significant impacts on regional air quality. We introduce the Canadian Forest Fire Emissions Prediction System and demonstrate its integration with Canada's FireWork operational air quality forecast system with biomass burning emissions. The coupled system shows improved skill in providing short-term, 48 h forecasts of surface air pollutant concentrations (PM2.5, O3, and NO2) from the impacts of regional wildland fires across the North American domain.
Erin E. McDuffie, Caroline C. Womack, Dorothy L. Fibiger, William P. Dube, Alessandro Franchin, Ann M. Middlebrook, Lexie Goldberger, Ben H. Lee, Joel A. Thornton, Alexander Moravek, Jennifer G. Murphy, Munkhbayar Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 19, 9287–9308, https://doi.org/10.5194/acp-19-9287-2019, https://doi.org/10.5194/acp-19-9287-2019, 2019
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Populated mountain basins, including the Salt Lake Valley (SLV) in Utah, suffer from wintertime stagnation events that trap emissions near the surface and cause fine particulate matter (PM2.5) concentrations to reach unhealthy levels. Previously limited by a lack of nighttime measurements, this study uses 2017 UWFPS aircraft campaign data, in combination with a box model, to show that nitrogen chemistry above the surface at night is a major source of PM2.5 during a wintertime event in the SLV.
Ye Tao and Jennifer G. Murphy
Atmos. Chem. Phys., 19, 9309–9320, https://doi.org/10.5194/acp-19-9309-2019, https://doi.org/10.5194/acp-19-9309-2019, 2019
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In this study, we analyzed the 10-year variation of aerosol pH in six Canadian cities and found the variation is largely attributed to the seasonal cycling of ambient temperature. We also found that in different seasons the pH sensitivity to chemical composition is distinctly different. This finding suggests the sensitivity of aerosol pH to chemical composition needs to be carefully examined for any particular region.
Yilong Wang, Philippe Ciais, Grégoire Broquet, François-Marie Bréon, Tomohiro Oda, Franck Lespinas, Yasjka Meijer, Armin Loescher, Greet Janssens-Maenhout, Bo Zheng, Haoran Xu, Shu Tao, Kevin R. Gurney, Geoffrey Roest, Diego Santaren, and Yongxian Su
Earth Syst. Sci. Data, 11, 687–703, https://doi.org/10.5194/essd-11-687-2019, https://doi.org/10.5194/essd-11-687-2019, 2019
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We address the question of the global characterization of fossil fuel CO2 emission hotspots that may cause coherent XCO2 plumes in space-borne CO2 images, based on the ODIAC global high-resolution 1 km fossil fuel emission data product. For space imagery with 0.5 ppm precision for a single XCO2 measurement, a total of 11 314 hotspots are identified, covering 72 % of the global emissions. These hotspots define the targets for the purpose of monitoring fossil fuel CO2 emissions from space.
Emmanuel Arzoumanian, Felix R. Vogel, Ana Bastos, Bakhram Gaynullin, Olivier Laurent, Michel Ramonet, and Philippe Ciais
Atmos. Meas. Tech., 12, 2665–2677, https://doi.org/10.5194/amt-12-2665-2019, https://doi.org/10.5194/amt-12-2665-2019, 2019
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We tested commercial lower-cost CO2 sensors in laboratory and field studies to see if they can measure atmospheric CO2 mole fractions with less than 1 ppm bias (with monthly calibration), to allow continuous urban CO2 monitoring.
We find that the sensors' CO2 readings are influenced by temperature, atmospheric pressure and water vapour content, but this can be corrected for by adding sensors (T, p, RH) and carefully calibrating each sensor against a high-precision instrument.
Misa Ishizawa, Douglas Chan, Doug Worthy, Elton Chan, Felix Vogel, and Shamil Maksyutov
Atmos. Chem. Phys., 19, 4637–4658, https://doi.org/10.5194/acp-19-4637-2019, https://doi.org/10.5194/acp-19-4637-2019, 2019
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The Canadian Arctic has the potential for enhanced methane (CH4) emissions under global warming. However, the regional CH4 emission (fluxes) estimates range widely. This study analyzes recent Canadian Arctic CH4 observations and estimates the regional emissions. The additional observations yield robust CH4 flux estimates and enable the partitioning of the CH4 sources into wetland and forest fires. The results indicate that years with warmer summer conditions result in more wetland CH4 emissions.
Dominik Brunner, Gerrit Kuhlmann, Julia Marshall, Valentin Clément, Oliver Fuhrer, Grégoire Broquet, Armin Löscher, and Yasjka Meijer
Atmos. Chem. Phys., 19, 4541–4559, https://doi.org/10.5194/acp-19-4541-2019, https://doi.org/10.5194/acp-19-4541-2019, 2019
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Atmospheric transport models are increasingly being used to estimate CO2 emissions from atmospheric CO2 measurements. This study demonstrates the importance of distributing CO2 emissions vertically in the model according to realistic profiles, since a major proportion of CO2 is emitted through tall stacks from power plants and industrial sources. With the traditional approach of emitting all CO2 at the surface, models may significantly overestimate the atmospheric CO2 levels.
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.
Felix R. Vogel, Matthias Frey, Johannes Staufer, Frank Hase, Grégoire Broquet, Irène Xueref-Remy, Frédéric Chevallier, Philippe Ciais, Mahesh Kumar Sha, Pascale Chelin, Pascal Jeseck, Christof Janssen, Yao Té, Jochen Groß, Thomas Blumenstock, Qiansi Tu, and Johannes Orphal
Atmos. Chem. Phys., 19, 3271–3285, https://doi.org/10.5194/acp-19-3271-2019, https://doi.org/10.5194/acp-19-3271-2019, 2019
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Providing timely information on greenhouse gas emissions to stakeholders at sub-national scale is an emerging challenge and understanding urban CO2 levels is one key aspect. This study uses atmospheric observations of total column CO2 and compares them to numerical simulations to investigate CO2 levels in the Paris metropolitan area due to natural fluxes and anthropogenic emissions. Our measurements reveal the influence of locally added CO2, which our model is also able to predict.
Matthias Frey, Mahesh K. Sha, Frank Hase, Matthäus Kiel, Thomas Blumenstock, Roland Harig, Gregor Surawicz, Nicholas M. Deutscher, Kei Shiomi, Jonathan E. Franklin, Hartmut Bösch, Jia Chen, Michel Grutter, Hirofumi Ohyama, Youwen Sun, André Butz, Gizaw Mengistu Tsidu, Dragos Ene, Debra Wunch, Zhensong Cao, Omaira Garcia, Michel Ramonet, Felix Vogel, and Johannes Orphal
Atmos. Meas. Tech., 12, 1513–1530, https://doi.org/10.5194/amt-12-1513-2019, https://doi.org/10.5194/amt-12-1513-2019, 2019
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In a 3.5-year long study, the long-term performance of a mobile EM27/SUN spectrometer, used for greenhouse gas observations, is checked with respect to a co-located reference spectrometer. We find that the EM27/SUN is stable on timescales of several years, qualifying it for permanent carbon cycle studies.
The performance of an ensemble of 30 EM27/SUN spectrometers was also tested in the framework of the COllaborative Carbon Column Observing Network (COCCON) and found to be very uniform.
Betty Croft, Randall V. Martin, W. Richard Leaitch, Julia Burkart, Rachel Y.-W. Chang, Douglas B. Collins, Patrick L. Hayes, Anna L. Hodshire, Lin Huang, John K. Kodros, Alexander Moravek, Emma L. Mungall, Jennifer G. Murphy, Sangeeta Sharma, Samantha Tremblay, Gregory R. Wentworth, Megan D. Willis, Jonathan P. D. Abbatt, and Jeffrey R. Pierce
Atmos. Chem. Phys., 19, 2787–2812, https://doi.org/10.5194/acp-19-2787-2019, https://doi.org/10.5194/acp-19-2787-2019, 2019
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Summertime Arctic atmospheric aerosols are strongly controlled by processes related to natural regional sources. We use a chemical transport model with size-resolved aerosol microphysics to interpret measurements made during summertime 2016 in the Canadian Arctic Archipelago. Our results explore the processes that control summertime aerosol size distributions and support a climate-relevant role for Arctic marine secondary organic aerosol formed from precursor vapors with Arctic marine sources.
Jonathan P. D. Abbatt, W. Richard Leaitch, Amir A. Aliabadi, Allan K. Bertram, Jean-Pierre Blanchet, Aude Boivin-Rioux, Heiko Bozem, Julia Burkart, Rachel Y. W. Chang, Joannie Charette, Jai P. Chaubey, Robert J. Christensen, Ana Cirisan, Douglas B. Collins, Betty Croft, Joelle Dionne, Greg J. Evans, Christopher G. Fletcher, Martí Galí, Roya Ghahreman, Eric Girard, Wanmin Gong, Michel Gosselin, Margaux Gourdal, Sarah J. Hanna, Hakase Hayashida, Andreas B. Herber, Sareh Hesaraki, Peter Hoor, Lin Huang, Rachel Hussherr, Victoria E. Irish, Setigui A. Keita, John K. Kodros, Franziska Köllner, Felicia Kolonjari, Daniel Kunkel, Luis A. Ladino, Kathy Law, Maurice Levasseur, Quentin Libois, John Liggio, Martine Lizotte, Katrina M. Macdonald, Rashed Mahmood, Randall V. Martin, Ryan H. Mason, Lisa A. Miller, Alexander Moravek, Eric Mortenson, Emma L. Mungall, Jennifer G. Murphy, Maryam Namazi, Ann-Lise Norman, Norman T. O'Neill, Jeffrey R. Pierce, Lynn M. Russell, Johannes Schneider, Hannes Schulz, Sangeeta Sharma, Meng Si, Ralf M. Staebler, Nadja S. Steiner, Jennie L. Thomas, Knut von Salzen, Jeremy J. B. Wentzell, Megan D. Willis, Gregory R. Wentworth, Jun-Wei Xu, and Jacqueline D. Yakobi-Hancock
Atmos. Chem. Phys., 19, 2527–2560, https://doi.org/10.5194/acp-19-2527-2019, https://doi.org/10.5194/acp-19-2527-2019, 2019
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The Arctic is experiencing considerable environmental change with climate warming, illustrated by the dramatic decrease in sea-ice extent. It is important to understand both the natural and perturbed Arctic systems to gain a better understanding of how they will change in the future. This paper summarizes new insights into the relationships between Arctic aerosol particles and climate, as learned over the past five or so years by a large Canadian research consortium, NETCARE.
Victoria E. Irish, Sarah J. Hanna, Megan D. Willis, Swarup China, Jennie L. Thomas, Jeremy J. B. Wentzell, Ana Cirisan, Meng Si, W. Richard Leaitch, Jennifer G. Murphy, Jonathan P. D. Abbatt, Alexander Laskin, Eric Girard, and Allan K. Bertram
Atmos. Chem. Phys., 19, 1027–1039, https://doi.org/10.5194/acp-19-1027-2019, https://doi.org/10.5194/acp-19-1027-2019, 2019
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Ice nucleating particles (INPs) are atmospheric particles that catalyse the formation of ice crystals in clouds. INPs influence the Earth's radiative balance and hydrological cycle. In this study we measured the concentrations of INPs in the Canadian Arctic marine boundary layer. Average INP concentrations fell within the range measured in other marine boundary layer locations. We also found that mineral dust is a more important contributor to the INP population than sea spray aerosol.
Travis W. Tokarek, Charles A. Odame-Ankrah, Jennifer A. Huo, Robert McLaren, Alex K. Y. Lee, Max G. Adam, Megan D. Willis, Jonathan P. D. Abbatt, Cristian Mihele, Andrea Darlington, Richard L. Mittermeier, Kevin Strawbridge, Katherine L. Hayden, Jason S. Olfert, Elijah G. Schnitzler, Duncan K. Brownsey, Faisal V. Assad, Gregory R. Wentworth, Alex G. Tevlin, Douglas E. J. Worthy, Shao-Meng Li, John Liggio, Jeffrey R. Brook, and Hans D. Osthoff
Atmos. Chem. Phys., 18, 17819–17841, https://doi.org/10.5194/acp-18-17819-2018, https://doi.org/10.5194/acp-18-17819-2018, 2018
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Measurements of air pollutants at a ground site near Fort McKay in the Athabasca oil sands region in the summer of 2013 are presented. A large number of intermediate-volatility organic compounds (IVOCs) were observed; these molecules were shown previously to generate atmospheric particles downwind of the region. A principal component analysis was performed to identify major pollution source types, including which source(s) is(are) associated with IVOC emissions (e.g., freshly mined bitumen).
Alessandro Franchin, Dorothy L. Fibiger, Lexie Goldberger, Erin E. McDuffie, Alexander Moravek, Caroline C. Womack, Erik T. Crosman, Kenneth S. Docherty, William P. Dube, Sebastian W. Hoch, Ben H. Lee, Russell Long, Jennifer G. Murphy, Joel A. Thornton, Steven S. Brown, Munkhbayar Baasandorj, and Ann M. Middlebrook
Atmos. Chem. Phys., 18, 17259–17276, https://doi.org/10.5194/acp-18-17259-2018, https://doi.org/10.5194/acp-18-17259-2018, 2018
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We present the results of aerosol and trace gas measurements from airborne and ground-based platforms. The measurements took place in January–February 2017 in northern Utah as part of the Utah Winter Fine Particulate Study (UWFPS). We characterized the chemical composition of PM1 on a regional scale, also probing the vertical dimension. We used a thermodynamic model to study the effectiveness of limiting total ammonium or total nitrate as a strategy to control aerosol concentrations.
Sumi N. Wren, John Liggio, Yuemei Han, Katherine Hayden, Gang Lu, Cris M. Mihele, Richard L. Mittermeier, Craig Stroud, Jeremy J. B. Wentzell, and Jeffrey R. Brook
Atmos. Chem. Phys., 18, 16979–17001, https://doi.org/10.5194/acp-18-16979-2018, https://doi.org/10.5194/acp-18-16979-2018, 2018
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We made measurements from a mobile laboratory across a large urban area and determined fleet-average vehicle emission factors (EFs) for a suite of traffic-related air pollutants. We present the first real-world EFs for isocyanic acid (HNCO) and hydrogen cyanide (HCN) and insight into their on-road variability. We find that vehicles may represent an important source of these air toxics at an urban scale. This work has implications for understanding population exposure to these species.
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.
Yilong Wang, Philippe Ciais, Daniel Goll, Yuanyuan Huang, Yiqi Luo, Ying-Ping Wang, A. Anthony Bloom, Grégoire Broquet, Jens Hartmann, Shushi Peng, Josep Penuelas, Shilong Piao, Jordi Sardans, Benjamin D. Stocker, Rong Wang, Sönke Zaehle, and Sophie Zechmeister-Boltenstern
Geosci. Model Dev., 11, 3903–3928, https://doi.org/10.5194/gmd-11-3903-2018, https://doi.org/10.5194/gmd-11-3903-2018, 2018
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We present a new modeling framework called Global Observation-based Land-ecosystems Utilization Model of Carbon, Nitrogen and Phosphorus (GOLUM-CNP) that combines a data-constrained C-cycle analysis with data-driven estimates of N and P inputs and losses and with observed stoichiometric ratios. GOLUM-CNP provides a traceable tool, where a consistency between different datasets of global C, N, and P cycles has been achieved.
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.
Emma L. Mungall, Jonathan P. D. Abbatt, Jeremy J. B. Wentzell, Gregory R. Wentworth, Jennifer G. Murphy, Daniel Kunkel, Ellen Gute, David W. Tarasick, Sangeeta Sharma, Christopher J. Cox, Taneil Uttal, and John Liggio
Atmos. Chem. Phys., 18, 10237–10254, https://doi.org/10.5194/acp-18-10237-2018, https://doi.org/10.5194/acp-18-10237-2018, 2018
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We measured gas-phase formic and acetic acid at Alert, Nunavut. These acids play an important role in cloud water acidity in remote environments, yet they are not well represented in chemical transport models, particularly in the Arctic. We observed high levels of formic and acetic acid under both cold, wet, and cloudy and warm, sunny, and dry conditions, suggesting that multiple sources significantly contribute to gas-phase concentrations of these species in the summer Arctic.
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 %.
Sabour Baray, Andrea Darlington, Mark Gordon, Katherine L. Hayden, Amy Leithead, Shao-Meng Li, Peter S. K. Liu, Richard L. Mittermeier, Samar G. Moussa, Jason O'Brien, Ralph Staebler, Mengistu Wolde, Doug Worthy, and Robert McLaren
Atmos. Chem. Phys., 18, 7361–7378, https://doi.org/10.5194/acp-18-7361-2018, https://doi.org/10.5194/acp-18-7361-2018, 2018
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Methane emissions from major oil sands facilities in the Athabasca Oil Sands Region (AOSR) of Alberta were measured in the summer of 2013 using two related aircraft mass-balance approaches. Tailings ponds and fugitive emissions of methane from open pit mines were found to be the major sources of methane in the region. Total methane emissions in the AOSR were measured to be ~ 20 tonnes of CH4 per hour, which is 48 % higher than the Canadian Greenhouse Gas Reporting Program Emissions Inventory.
Claudia Grossi, Felix R. Vogel, Roger Curcoll, Alba Àgueda, Arturo Vargas, Xavier Rodó, and Josep-Anton Morguí
Atmos. Chem. Phys., 18, 5847–5860, https://doi.org/10.5194/acp-18-5847-2018, https://doi.org/10.5194/acp-18-5847-2018, 2018
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To gain a full picture of the Spanish (and European) GHG balance, understanding of CH4 emissions in different regions is a critical challenge, as is the improvement of bottom-up inventories for all European regions. This study uses, among other elements, GHG, meteorological and 222Rn tracer data from a Spanish region to understand the main causes of temporal variability of GHG mixing ratios. The study can offer new insights into regional emissions by identifying the impacts of changing sources.
Yilong Wang, Grégoire Broquet, Philippe Ciais, Frédéric Chevallier, Felix Vogel, Lin Wu, Yi Yin, Rong Wang, and Shu Tao
Atmos. Chem. Phys., 18, 4229–4250, https://doi.org/10.5194/acp-18-4229-2018, https://doi.org/10.5194/acp-18-4229-2018, 2018
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This paper assesses the potential of atmospheric 14CO2 observations and a global inversion system to solve for fossil fuel CO2 (FFCO2) emissions in Europe. The estimate of monthly emission budgets is largely improved in high emitting regions. The results are sensitive to the observation network and the prior uncertainty. Using a high-resolution transport model and a systematic evaluation of the uncertainty in current emission inventories should improve the potential to retrieve FFCO2 emissions.
Abdelhadi El Yazidi, Michel Ramonet, Philippe Ciais, Gregoire Broquet, Isabelle Pison, Amara Abbaris, Dominik Brunner, Sebastien Conil, Marc Delmotte, Francois Gheusi, Frederic Guerin, Lynn Hazan, Nesrine Kachroudi, Giorgos Kouvarakis, Nikolaos Mihalopoulos, Leonard Rivier, and Dominique Serça
Atmos. Meas. Tech., 11, 1599–1614, https://doi.org/10.5194/amt-11-1599-2018, https://doi.org/10.5194/amt-11-1599-2018, 2018
Isabelle Pison, Antoine Berchet, Marielle Saunois, Philippe Bousquet, Grégoire Broquet, Sébastien Conil, Marc Delmotte, Anita Ganesan, Olivier Laurent, Damien Martin, Simon O'Doherty, Michel Ramonet, T. Gerard Spain, Alex Vermeulen, and Camille Yver Kwok
Atmos. Chem. Phys., 18, 3779–3798, https://doi.org/10.5194/acp-18-3779-2018, https://doi.org/10.5194/acp-18-3779-2018, 2018
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Methane emissions on the national scale in France in 2012 are inferred by assimilating continuous atmospheric mixing ratio measurements from nine stations of the European network ICOS. Two complementary inversion set-ups are computed and analysed: (i) a regional run correcting for the spatial distribution of fluxes in France and (ii) a sectorial run correcting fluxes for activity sectors on the national scale. The results are compared with existing inventories and other regional inversions.
Irène Xueref-Remy, Elsa Dieudonné, Cyrille Vuillemin, Morgan Lopez, Christine Lac, Martina Schmidt, Marc Delmotte, Frédéric Chevallier, François Ravetta, Olivier Perrussel, Philippe Ciais, François-Marie Bréon, Grégoire Broquet, Michel Ramonet, T. Gerard Spain, and Christophe Ampe
Atmos. Chem. Phys., 18, 3335–3362, https://doi.org/10.5194/acp-18-3335-2018, https://doi.org/10.5194/acp-18-3335-2018, 2018
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Urbanized and industrialized areas are the largest source of fossil CO2. This work analyses the atmospheric CO2 variability observed from the first in situ network deployed in the Paris megacity area. Gradients of several ppm are found between the rural, peri-urban and urban sites at the diurnal to the seasonal scales. Wind direction and speed as well as boundary layer dynamics, correlated to highly variable urban emissions, are shown to be key regulator factors of the observed CO2 records.
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.
Grégoire Broquet, François-Marie Bréon, Emmanuel Renault, Michael Buchwitz, Maximilian Reuter, Heinrich Bovensmann, Frédéric Chevallier, Lin Wu, and Philippe Ciais
Atmos. Meas. Tech., 11, 681–708, https://doi.org/10.5194/amt-11-681-2018, https://doi.org/10.5194/amt-11-681-2018, 2018
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This study assesses the potential of space-borne imagery of CO2 atmospheric concentrations for monitoring the emissions from the Paris area. Such imagery could be provided by European and American missions in the next decade. It highlights the difficulty to improve current knowledge on CO2 emissions for urban areas with CO2 observations from satellites, and calls for more technological innovations in the remote sensing of CO2 and in the models that exploit it.
Sébastien Ars, Grégoire Broquet, Camille Yver Kwok, Yelva Roustan, Lin Wu, Emmanuel Arzoumanian, and Philippe Bousquet
Atmos. Meas. Tech., 10, 5017–5037, https://doi.org/10.5194/amt-10-5017-2017, https://doi.org/10.5194/amt-10-5017-2017, 2017
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This study presents a new concept for estimating the pollutant emission rates of a site combining the tracer release method, local-scale atmospheric transport modelling and a statistical atmospheric inversion approach. The potential of this new concept is evaluated with a practical implementation based on a series of inversions of controlled methane and tracer point sources in different spatial configurations to assess the efficiency of the method in comparison with the classic tracer method.
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.
Vitali Fioletov, Chris A. McLinden, Shailesh K. Kharol, Nickolay A. Krotkov, Can Li, Joanna Joiner, Michael D. Moran, Robert Vet, Antoon J. H. Visschedijk, and Hugo A. C. Denier van der Gon
Atmos. Chem. Phys., 17, 12597–12616, https://doi.org/10.5194/acp-17-12597-2017, https://doi.org/10.5194/acp-17-12597-2017, 2017
Sabina Assan, Alexia Baudic, Ali Guemri, Philippe Ciais, Valerie Gros, and Felix R. Vogel
Atmos. Meas. Tech., 10, 2077–2091, https://doi.org/10.5194/amt-10-2077-2017, https://doi.org/10.5194/amt-10-2077-2017, 2017
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This study is dedicated to improving measurement methods when using a Cavity Ring Down Spectroscopy instrument to measure methane at sites with elevated ethane concentrations such as Oil and Gas sites. The research was undertaken after measurements of natural gas samples suggested biased δ13CH4 results. Two instruments were extensively tested to characterize the cross sensitivities to ethane and δ13CH4 and propose corrections. Results indicate that it is imperative to account for the biases.
Yi Yin, Frederic Chevallier, Philippe Ciais, Gregoire Broquet, Anne Cozic, Sophie Szopa, and Yilong Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-166, https://doi.org/10.5194/acp-2017-166, 2017
Revised manuscript not accepted
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CO inverse modelling studies have so far reported significant discrepancies between model concentrations optimised with the Measurement of Pollution in the Troposphere (MOPITT) satellite retrievals and surface in-situ measurements. Here, we assess how well a global CTM fits a large variety of independent CO observations before and after assimilating MOPITTv6 retrievals to optimise CO sources/sink and discuss potential sources of errors and their implications for global CO modelling studies.
Chantelle R. Lonsdale, Jennifer D. Hegarty, Karen E. Cady-Pereira, Matthew J. Alvarado, Daven K. Henze, Matthew D. Turner, Shannon L. Capps, John B. Nowak, J. Andy Neuman, Ann M. Middlebrook, Roya Bahreini, Jennifer G. Murphy, Milos Z. Markovic, Trevor C. VandenBoer, Lynn M. Russell, and Amy Jo Scarino
Atmos. Chem. Phys., 17, 2721–2739, https://doi.org/10.5194/acp-17-2721-2017, https://doi.org/10.5194/acp-17-2721-2017, 2017
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This study takes advantage of the high-resolution observations of NH3(g) made by the TES satellite instrument over Bakersfield during the CalNex campaign, along with campaign measurements, to compare CMAQ model results in the San Joaquin Valley, California. Additionally we evaluate the CMAQ bi-directional ammonia flux results using the CARB emissions inventory against these satellite and campaign measurements, not previously explored in combination.
Lamia Ammoura, Irène Xueref-Remy, Felix Vogel, Valérie Gros, Alexia Baudic, Bernard Bonsang, Marc Delmotte, Yao Té, and Frédéric Chevallier
Atmos. Chem. Phys., 16, 15653–15664, https://doi.org/10.5194/acp-16-15653-2016, https://doi.org/10.5194/acp-16-15653-2016, 2016
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We propose a new approach to estimate urban emission ratios that takes advantage of the enhanced local urban signal in the atmosphere at low wind speed. We apply it to estimate monthly ratios between CO2, CO and some VOCs from atmospheric measurement datasets acquired in the centre of Paris between 2010 and 2014. We find that this approach is little sensitive to the regional background level definition. With this new method, we may reveal spatial and seasonal variability in the ratios in Paris.
Johannes Staufer, Grégoire Broquet, François-Marie Bréon, Vincent Puygrenier, Frédéric Chevallier, Irène Xueref-Rémy, Elsa Dieudonné, Morgan Lopez, Martina Schmidt, Michel Ramonet, Olivier Perrussel, Christine Lac, Lin Wu, and Philippe Ciais
Atmos. Chem. Phys., 16, 14703–14726, https://doi.org/10.5194/acp-16-14703-2016, https://doi.org/10.5194/acp-16-14703-2016, 2016
Yuemei Han, Craig A. Stroud, John Liggio, and Shao-Meng Li
Atmos. Chem. Phys., 16, 13929–13944, https://doi.org/10.5194/acp-16-13929-2016, https://doi.org/10.5194/acp-16-13929-2016, 2016
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This study investigates the acidity effect on the yield and chemical composition of α-pinene secondary organic aerosol based on a series of laboratory experiments performed using a photochemical reaction chamber under high- and low-NOx conditions. We have found that the acidity effect largely depends on NOx level and the inorganic acidity has a significant role to play in determining various organic aerosol chemical properties such as mass yields, oxidation state, and organic nitrate content.
Elton Chan, Douglas Chan, Misa Ishizawa, Felix Vogel, Jerome Brioude, Andy Delcloo, Yuehua Wu, and Baisuo Jin
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2016-213, https://doi.org/10.5194/gmd-2016-213, 2016
Revised manuscript not accepted
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The main objective of this study is to examine the impacts of errors introduced by different components in our newly developed inversion system on flux estimates with a series of controlled experiments. It is very critical for any inversion system to be fully evaluated prior to applying to real observations. As demonstrated, the results can be very sensitive to the model setup and region. It is not reasonable to expect realistic results can always be obtained using the same approach.
Igor B. Konovalov, Evgeny V. Berezin, Philippe Ciais, Grégoire Broquet, Ruslan V. Zhuravlev, and Greet Janssens-Maenhout
Atmos. Chem. Phys., 16, 13509–13540, https://doi.org/10.5194/acp-16-13509-2016, https://doi.org/10.5194/acp-16-13509-2016, 2016
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The knowledge of CO2 emissions from fossil-fuel (FF) burning is of paramount importance both for climate prediction and mitigation policy purposes. The paper introduces a method to indirectly constrain a regional budget of FF CO2 emissions by using satellite measurements of "proxy" chemical species and evaluates its potential in application to a western European region.
Saroja M. Polavarapu, Michael Neish, Monique Tanguay, Claude Girard, Jean de Grandpré, Kirill Semeniuk, Sylvie Gravel, Shuzhan Ren, Sébastien Roche, Douglas Chan, and Kimberly Strong
Atmos. Chem. Phys., 16, 12005–12038, https://doi.org/10.5194/acp-16-12005-2016, https://doi.org/10.5194/acp-16-12005-2016, 2016
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CO2 predictions are used to compute model–data mismatches when estimating surfaces fluxes using atmospheric observations together with an atmospheric transport model. By isolating the component of transport error which is due to uncertain meteorological analyses, it is demonstrated that CO2 can only be defined on large spatial scales. Thus, there is a spatial scale below which we cannot infer fluxes simply due to the fact that meteorological analyes are imperfect.
Vitali E. Fioletov, Chris A. McLinden, Nickolay Krotkov, Can Li, Joanna Joiner, Nicolas Theys, Simon Carn, and Mike D. Moran
Atmos. Chem. Phys., 16, 11497–11519, https://doi.org/10.5194/acp-16-11497-2016, https://doi.org/10.5194/acp-16-11497-2016, 2016
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We introduce the first space-based catalogue of SO2 emission sources seen by OMI. The inventory contains about 500 sources. They account for about a half of all SO2 emissions; the remaining half is likely related to sources emitting less than 30 kt yr−1 and not detected by OMI. The sources are grouped by type (volcanoes, power plants, oil- and gas-related sources, and smelters) and country. The catalogue presented herein can be used for verification of available SO2 emission inventories.
Lin Wu, Grégoire Broquet, Philippe Ciais, Valentin Bellassen, Felix Vogel, Frédéric Chevallier, Irène Xueref-Remy, and Yilong Wang
Atmos. Chem. Phys., 16, 7743–7771, https://doi.org/10.5194/acp-16-7743-2016, https://doi.org/10.5194/acp-16-7743-2016, 2016
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This paper advances atmospheric inversion of city CO2 emissions as follows: (1) illustrate how inversion methodology can be tailored to deal with very large urban networks of sensors measuring CO2 concentrations; (2) demonstrate that atmospheric inversion could be a relevant tool of Monitoring, Reporting and Verification (MRV) of city CO2 emissions; (3) clarify the theoretical potential of inversion for reducing uncertainties in the estimates of citywide total and sectoral CO2 emissions.
Gregory R. Wentworth, Jennifer G. Murphy, Katherine B. Benedict, Evelyn J. Bangs, and Jeffrey L. Collett Jr.
Atmos. Chem. Phys., 16, 7435–7449, https://doi.org/10.5194/acp-16-7435-2016, https://doi.org/10.5194/acp-16-7435-2016, 2016
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The influence of dew on atmospheric composition is poorly understood. Results from this work show that dew can uptake a significant fraction (roughly two-thirds) of boundary layer gas-phase ammonia. Furthermore, an average of 95 % of the ammonia sequestered in dew is released back to the atmosphere the following morning during dew evaporation. Dew has the ability to affect air quality and N-deposition and should be considered when modelling ammonia concentrations, as well as other soluble gases.
Alex Boon, Grégoire Broquet, Deborah J. Clifford, Frédéric Chevallier, David M. Butterfield, Isabelle Pison, Michel Ramonet, Jean-Daniel Paris, and Philippe Ciais
Atmos. Chem. Phys., 16, 6735–6756, https://doi.org/10.5194/acp-16-6735-2016, https://doi.org/10.5194/acp-16-6735-2016, 2016
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We measured carbon dioxide and methane concentrations at four near-ground sites located in London, 2012. We investigated the potential for using these measurements, alongside numerical modelling, to help us to understand urban greenhouse gas emissions. Low-level sites were highly sensitive to local emissions, which questions our ability to use measurements from near-ground sites in cities in some modelling applications. A gradient approach was found to be beneficial to reduce model–data errors.
Emma L. Mungall, Betty Croft, Martine Lizotte, Jennie L. Thomas, Jennifer G. Murphy, Maurice Levasseur, Randall V. Martin, Jeremy J. B. Wentzell, John Liggio, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 16, 6665–6680, https://doi.org/10.5194/acp-16-6665-2016, https://doi.org/10.5194/acp-16-6665-2016, 2016
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Previous work has suggested that marine emissions of dimethyl sulfide (DMS) could impact the Arctic climate through interactions with clouds. We made the first high-time-resolution measurements of summertime atmospheric DMS in the Canadian Arctic, and performed source sensitivity simulations. We found that regional marine sources dominated, but do not appear to be sufficient to explain our observations. Understanding DMS sources in the Arctic is necessary to model future climate in the region.
Gregory R. Wentworth, Jennifer G. Murphy, Betty Croft, Randall V. Martin, Jeffrey R. Pierce, Jean-Sébastien Côté, Isabelle Courchesne, Jean-Éric Tremblay, Jonathan Gagnon, Jennie L. Thomas, Sangeeta Sharma, Desiree Toom-Sauntry, Alina Chivulescu, Maurice Levasseur, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 16, 1937–1953, https://doi.org/10.5194/acp-16-1937-2016, https://doi.org/10.5194/acp-16-1937-2016, 2016
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Air near the surface in the summertime Arctic is extremely clean and typically has very low concentrations of both gases and particles. However, atmospheric measurements taken throughout the Canadian Arctic in the summer of 2014 revealed higher-than-expected amounts of gaseous ammonia. It is likely the majority of this ammonia is coming from migratory seabird colonies throughout the Arctic. Seabird guano (dung) releases ammonia which could impact climate and sensitive Arctic ecosystems.
N. Borduas, B. Place, G. R. Wentworth, J. P. D. Abbatt, and J. G. Murphy
Atmos. Chem. Phys., 16, 703–714, https://doi.org/10.5194/acp-16-703-2016, https://doi.org/10.5194/acp-16-703-2016, 2016
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HNCO is a toxic molecule and can cause cardiovascular and cataract problems through protein carbamylation once inhaled. Recently reported ambient measurements of HNCO in North America raise concerns for human exposure. To better understand HNCO's loss processes and behaviour in the atmosphere, we provide thermochemical data on HNCO. The parameters allow for more accurate predictions of its lifetime in the atmosphere and consequently help define exposure of this toxic molecule.
P. Kountouris, C. Gerbig, K.-U. Totsche, A. J. Dolman, A. G. C. A. Meesters, G. Broquet, F. Maignan, B. Gioli, L. Montagnani, and C. Helfter
Biogeosciences, 12, 7403–7421, https://doi.org/10.5194/bg-12-7403-2015, https://doi.org/10.5194/bg-12-7403-2015, 2015
Y. Yin, F. Chevallier, P. Ciais, G. Broquet, A. Fortems-Cheiney, I. Pison, and M. Saunois
Atmos. Chem. Phys., 15, 13433–13451, https://doi.org/10.5194/acp-15-13433-2015, https://doi.org/10.5194/acp-15-13433-2015, 2015
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We studied the global CO concentration decline over the recent decade with a sophisticated atmospheric inversion system assimilating MOPITT CO retrievals, surface methane and surface methyl chloroform in situ measurements. The inversion interprets the CO concentration decline as a 23% decrease in the CO emissions from 2002 to 2011, twice the negative trend estimated by emission inventories. In contrast to bottom-up inventories, we find negative trends over China and South-east Asia.
N. Kadygrov, G. Broquet, F. Chevallier, L. Rivier, C. Gerbig, and P. Ciais
Atmos. Chem. Phys., 15, 12765–12787, https://doi.org/10.5194/acp-15-12765-2015, https://doi.org/10.5194/acp-15-12765-2015, 2015
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We study the potential of the European Integrated Carbon Observing System (ICOS) atmospheric network for estimating European CO2 ecosystem fluxes. Regional atmospheric inversions with synthetic data are used to derive it in terms of statistical uncertainty. This potential is high in western Europe and future extensions of the network will increase it in eastern Europe. Future improvements of the models underlying the inversion should also significantly decrease uncertainties at high resolution.
E. Chan, D. Chan, M. Ishizawa, F. Vogel, J. Brioude, A. Delcloo, Y. Wu, and B. Jin
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-22715-2015, https://doi.org/10.5194/acpd-15-22715-2015, 2015
Revised manuscript not accepted
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This paper uses synthetic data experiments to investigate the impacts of different error sources associated with prior flux, transport model and optimisation method on the atmospheric greenhouse gas inverse estimates. Results indicate that estimation errors are dominated by the transport model error and can propagate to the flux estimates non-linearly. It is necessary to obtain stable and realistic results in synthetic data experiments before a real observation-based inversion is performed.
L. Molina, G. Broquet, P. Imbach, F. Chevallier, B. Poulter, D. Bonal, B. Burban, M. Ramonet, L. V. Gatti, S. C. Wofsy, J. W. Munger, E. Dlugokencky, and P. Ciais
Atmos. Chem. Phys., 15, 8423–8438, https://doi.org/10.5194/acp-15-8423-2015, https://doi.org/10.5194/acp-15-8423-2015, 2015
C. E. Yver Kwok, D. Müller, C. Caldow, B. Lebègue, J. G. Mønster, C. W. Rella, C. Scheutz, M. Schmidt, M. Ramonet, T. Warneke, G. Broquet, and P. Ciais
Atmos. Meas. Tech., 8, 2853–2867, https://doi.org/10.5194/amt-8-2853-2015, https://doi.org/10.5194/amt-8-2853-2015, 2015
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This study presents two methods for estimating methane emissions from a waste water treatment plant (WWTP) along with results from a measurement campaign at a WWTP in Valence, France. We show that the tracer release method is suitable to quantify facility emissions, while the chamber measurements, provide insights into individual processes. We confirm that the open basins are not a major source of CH4 on the WWTP but that the pretreatment and sludge treatment are the main emitters.
F. M. Bréon, G. Broquet, V. Puygrenier, F. Chevallier, I. Xueref-Remy, M. Ramonet, E. Dieudonné, M. Lopez, M. Schmidt, O. Perrussel, and P. Ciais
Atmos. Chem. Phys., 15, 1707–1724, https://doi.org/10.5194/acp-15-1707-2015, https://doi.org/10.5194/acp-15-1707-2015, 2015
L. Huang, S. L. Gong, M. Gordon, J. Liggio, R. Staebler, C. A. Stroud, G. Lu, C. Mihele, J. R. Brook, and C. Q. Jia
Atmos. Chem. Phys., 14, 12631–12648, https://doi.org/10.5194/acp-14-12631-2014, https://doi.org/10.5194/acp-14-12631-2014, 2014
G. R. Wentworth, J. G. Murphy, P. K. Gregoire, C. A. L. Cheyne, A. G. Tevlin, and R. Hems
Biogeosciences, 11, 5675–5686, https://doi.org/10.5194/bg-11-5675-2014, https://doi.org/10.5194/bg-11-5675-2014, 2014
I. B. Konovalov, E. V. Berezin, P. Ciais, G. Broquet, M. Beekmann, J. Hadji-Lazaro, C. Clerbaux, M. O. Andreae, J. W. Kaiser, and E.-D. Schulze
Atmos. Chem. Phys., 14, 10383–10410, https://doi.org/10.5194/acp-14-10383-2014, https://doi.org/10.5194/acp-14-10383-2014, 2014
M. Gordon, A. Vlasenko, R. M. Staebler, C. Stroud, P. A. Makar, J. Liggio, S.-M. Li, and S. Brown
Atmos. Chem. Phys., 14, 9087–9097, https://doi.org/10.5194/acp-14-9087-2014, https://doi.org/10.5194/acp-14-9087-2014, 2014
S. C. Pugliese, J. G. Murphy, J. A. Geddes, and J. M. Wang
Atmos. Chem. Phys., 14, 8197–8207, https://doi.org/10.5194/acp-14-8197-2014, https://doi.org/10.5194/acp-14-8197-2014, 2014
E. A. Marais, D. J. Jacob, A. Guenther, K. Chance, T. P. Kurosu, J. G. Murphy, C. E. Reeves, and H. O. T. Pye
Atmos. Chem. Phys., 14, 7693–7703, https://doi.org/10.5194/acp-14-7693-2014, https://doi.org/10.5194/acp-14-7693-2014, 2014
R. Kretschmer, C. Gerbig, U. Karstens, G. Biavati, A. Vermeulen, F. Vogel, S. Hammer, and K. U. Totsche
Atmos. Chem. Phys., 14, 7149–7172, https://doi.org/10.5194/acp-14-7149-2014, https://doi.org/10.5194/acp-14-7149-2014, 2014
P. Ciais, A. J. Dolman, A. Bombelli, R. Duren, A. Peregon, P. J. Rayner, C. Miller, N. Gobron, G. Kinderman, G. Marland, N. Gruber, F. Chevallier, R. J. Andres, G. Balsamo, L. Bopp, F.-M. Bréon, G. Broquet, R. Dargaville, T. J. Battin, A. Borges, H. Bovensmann, M. Buchwitz, J. Butler, J. G. Canadell, R. B. Cook, R. DeFries, R. Engelen, K. R. Gurney, C. Heinze, M. Heimann, A. Held, M. Henry, B. Law, S. Luyssaert, J. Miller, T. Moriyama, C. Moulin, R. B. Myneni, C. Nussli, M. Obersteiner, D. Ojima, Y. Pan, J.-D. Paris, S. L. Piao, B. Poulter, S. Plummer, S. Quegan, P. Raymond, M. Reichstein, L. Rivier, C. Sabine, D. Schimel, O. Tarasova, R. Valentini, R. Wang, G. van der Werf, D. Wickland, M. Williams, and C. Zehner
Biogeosciences, 11, 3547–3602, https://doi.org/10.5194/bg-11-3547-2014, https://doi.org/10.5194/bg-11-3547-2014, 2014
D. Wen, L. Zhang, J. C. Lin, R. Vet, and M. D. Moran
Geosci. Model Dev., 7, 1037–1050, https://doi.org/10.5194/gmd-7-1037-2014, https://doi.org/10.5194/gmd-7-1037-2014, 2014
P. A. Makar, R. Nissen, A. Teakles, J. Zhang, Q. Zheng, M. D. Moran, H. Yau, and C. diCenzo
Geosci. Model Dev., 7, 1001–1024, https://doi.org/10.5194/gmd-7-1001-2014, https://doi.org/10.5194/gmd-7-1001-2014, 2014
D. R. Gentner, T. B. Ford, A. Guha, K. Boulanger, J. Brioude, W. M. Angevine, J. A. de Gouw, C. Warneke, J. B. Gilman, T. B. Ryerson, J. Peischl, S. Meinardi, D. R. Blake, E. Atlas, W. A. Lonneman, T. E. Kleindienst, M. R. Beaver, J. M. St. Clair, P. O. Wennberg, T. C. VandenBoer, M. Z. Markovic, J. G. Murphy, R. A. Harley, and A. H. Goldstein
Atmos. Chem. Phys., 14, 4955–4978, https://doi.org/10.5194/acp-14-4955-2014, https://doi.org/10.5194/acp-14-4955-2014, 2014
X. Wang, L. Zhang, and M. D. Moran
Geosci. Model Dev., 7, 799–819, https://doi.org/10.5194/gmd-7-799-2014, https://doi.org/10.5194/gmd-7-799-2014, 2014
E. Galarneau, P. A. Makar, Q. Zheng, J. Narayan, J. Zhang, M. D. Moran, M. A. Bari, S. Pathela, A. Chen, and R. Chlumsky
Atmos. Chem. Phys., 14, 4065–4077, https://doi.org/10.5194/acp-14-4065-2014, https://doi.org/10.5194/acp-14-4065-2014, 2014
J. A. Geddes and J. G. Murphy
Atmos. Chem. Phys., 14, 2939–2957, https://doi.org/10.5194/acp-14-2939-2014, https://doi.org/10.5194/acp-14-2939-2014, 2014
C. E. Yver-Kwok, D. Müller, C. Caldow, B. Lebegue, J. G. Mønster, C. W. Rella, C. Scheutz, M. Schmidt, M. Ramonet, T. Warneke, G. Broquet, and P. Ciais
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amtd-6-9181-2013, https://doi.org/10.5194/amtd-6-9181-2013, 2013
Revised manuscript not accepted
L. Zhang, X. Wang, M. D. Moran, and J. Feng
Atmos. Chem. Phys., 13, 10005–10025, https://doi.org/10.5194/acp-13-10005-2013, https://doi.org/10.5194/acp-13-10005-2013, 2013
G. Broquet, F. Chevallier, F.-M. Bréon, N. Kadygrov, M. Alemanno, F. Apadula, S. Hammer, L. Haszpra, F. Meinhardt, J. A. Morguí, J. Necki, S. Piacentino, M. Ramonet, M. Schmidt, R. L. Thompson, A. T. Vermeulen, C. Yver, and P. Ciais
Atmos. Chem. Phys., 13, 9039–9056, https://doi.org/10.5194/acp-13-9039-2013, https://doi.org/10.5194/acp-13-9039-2013, 2013
J. M. Wang, J. G. Murphy, J. A. Geddes, C. L. Winsborough, N. Basiliko, and S. C. Thomas
Biogeosciences, 10, 4371–4382, https://doi.org/10.5194/bg-10-4371-2013, https://doi.org/10.5194/bg-10-4371-2013, 2013
E. Solazzo, R. Bianconi, G. Pirovano, M. D. Moran, R. Vautard, C. Hogrefe, K. W. Appel, V. Matthias, P. Grossi, B. Bessagnet, J. Brandt, C. Chemel, J. H. Christensen, R. Forkel, X. V. Francis, A. B. Hansen, S. McKeen, U. Nopmongcol, M. Prank, K. N. Sartelet, A. Segers, J. D. Silver, G. Yarwood, J. Werhahn, J. Zhang, S. T. Rao, and S. Galmarini
Geosci. Model Dev., 6, 791–818, https://doi.org/10.5194/gmd-6-791-2013, https://doi.org/10.5194/gmd-6-791-2013, 2013
D. Wen, J. C. Lin, L. Zhang, R. Vet, and M. D. Moran
Geosci. Model Dev., 6, 327–344, https://doi.org/10.5194/gmd-6-327-2013, https://doi.org/10.5194/gmd-6-327-2013, 2013
F. R. Vogel, L. Huang, D. Ernst, L. Giroux, S. Racki, and D. E. J. Worthy
Atmos. Meas. Tech., 6, 301–308, https://doi.org/10.5194/amt-6-301-2013, https://doi.org/10.5194/amt-6-301-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
The contribution of transport emissions to ozone mixing ratios and methane lifetime in 2015 and 2050 in the Shared Socioeconomic Pathways (SSPs)
Ether and ester formation from peroxy radical recombination: a qualitative reaction channel analysis
ACEIC: a comprehensive anthropogenic chlorine emission inventory for China
Impact of methane and other precursor emission reductions on surface ozone in Europe: scenario analysis using the European Monitoring and Evaluation Programme (EMEP) Meteorological Synthesizing Centre – West (MSC-W) model
Verifying national inventory-based combustion emissions of CO2 across the UK and mainland Europe using satellite observations of atmospheric CO and CO2
An improved estimate of inorganic iodine emissions from the ocean using a coupled surface microlayer box model
Impact of improved representation of volatile organic compound emissions and production of NOx reservoirs on modeled urban ozone production
The effect of different climate and air quality policies in China on in situ ozone production in Beijing
Enhancing long-term trend simulation of the global tropospheric hydroxyl (TOH) and its drivers from 2005 to 2019: a synergistic integration of model simulations and satellite observations
Intercomparison of GEOS-Chem and CAM-chem tropospheric oxidant chemistry within the Community Earth System Model version 2 (CESM2)
Development of a detailed gaseous oxidation scheme of naphthalene for secondary organic aerosol (SOA) formation and speciation
Large contributions of soil emissions to the atmospheric nitrogen budget and their impacts on air quality and temperature rise in North China
Why did ozone concentrations remain high during Shanghai's static management? A statistical and radical-chemistry perspective
Revising VOC emissions speciation improves the simulation of global background ethane and propane
Changes in South American surface ozone trends: exploring the influences of precursors and extreme events
Evaluating NOx stack plume emissions using a high-resolution atmospheric chemistry model and satellite-derived NO2 columns
NOx emissions in France in 2019–2021 as estimated by the high-spatial-resolution assimilation of TROPOMI NO2 observations
Aggravated surface O3 pollution primarily driven by meteorological variations in China during the 2020 COVID-19 pandemic lockdown period
Identifying decadal trends in deweathered concentrations of criteria air pollutants in Canadian urban atmospheres with machine learning approaches
Evaluation of modelled versus observed non-methane volatile organic compounds at European Monitoring and Evaluation Programme sites in Europe
Constraining non-methane VOC emissions with TROPOMI HCHO observations: impact on summertime ozone simulation in August 2022 in China
Revealing the significant acceleration of hydrofluorocarbon (HFC) emissions in eastern Asia through long-term atmospheric observations
Role of chemical production and depositional losses on formaldehyde in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Interpreting Geostationary Environment Monitoring Spectrometer (GEMS) geostationary satellite observations of the diurnal variation in nitrogen dioxide (NO2) over East Asia
Constraining Light Dependency in Modeled Emissions Through Comparison to Observed BVOC Concentrations in a Southeastern US Forest
An intercomparison of satellite, airborne, and ground-level observations with WRF–CAMx simulations of NO2 columns over Houston, Texas, during the September 2021 TRACER-AQ campaign
Investigating processes influencing simulation of local Arctic wintertime anthropogenic pollution in Fairbanks, Alaska during ALPACA-2022
Interannual variability of summertime formaldehyde (HCHO) vertical column density and its main drivers at northern high latitudes
The impact of multi-decadal changes in VOC speciation on urban ozone chemistry: a case study in Birmingham, United Kingdom
Technical note: Challenges in detecting free tropospheric ozone trends in a sparsely sampled environment
Combined assimilation of NOAA surface and MIPAS satellite observations to constrain the global budget of carbonyl sulfide
The impact of gaseous degradation on the gas–particle partitioning of methylated polycyclic aromatic hydrocarbons
Technical note: An assessment of the performance of statistical bias correction techniques for global chemistry–climate model surface ozone fields
Interpreting Summertime Hourly Variation of NO2 Columns with Implications for Geostationary Satellite Applications
Opinion: Challenges and needs of tropospheric chemical mechanism development
A better representation of volatile organic compound chemistry in WRF-Chem and its impact on ozone over Los Angeles
High-resolution US methane emissions inferred from an inversion of 2019 TROPOMI satellite data: contributions from individual states, urban areas, and landfills
Summertime tropospheric ozone source apportionment study in the Madrid region (Spain)
CO anthropogenic emissions in Europe from 2011 to 2021: insights from Measurement of Pollution in the Troposphere (MOPITT) satellite data
Constraining long-term NOx emissions over the United States and Europe using nitrate wet deposition monitoring networks
An investigation into atmospheric nitrous acid (HONO) processes in South Korea
Analysis of an intense O3 pollution episode on the Atlantic coast of the Iberian Peninsula using photochemical modeling: characterization of transport pathways and accumulation processes
A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021
Atmospheric oxygen as a tracer for fossil fuel carbon dioxide: a sensitivity study in the UK
Source analyses of ambient VOCs considering reactive losses: methods of reducing loss effects, impacts of losses, and sources
MIXv2: a long-term mosaic emission inventory for Asia (2010–2017)
The Atmospheric Oxidizing Capacity in China: Part 2. Sensitivity to emissions of primary pollutants
Process Analysis of Elevated Concentrations of Organic Acids at Whiteface Mountain, New York
Organosulfate produced from consumption of SO3 speeds up sulfuric acid–dimethylamine atmospheric nucleation
Tropospheric Ozone Precursors: Global and Regional Distributions, Trends and Variability
Mariano Mertens, Sabine Brinkop, Phoebe Graf, Volker Grewe, Johannes Hendricks, Patrick Jöckel, Anna Lanteri, Sigrun Matthes, Vanessa S. Rieger, Mattia Righi, and Robin N. Thor
Atmos. Chem. Phys., 24, 12079–12106, https://doi.org/10.5194/acp-24-12079-2024, https://doi.org/10.5194/acp-24-12079-2024, 2024
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We quantified the contributions of land transport, shipping, and aviation emissions to tropospheric ozone; its radiative forcing; and the reductions of the methane lifetime using chemistry-climate model simulations. The contributions were analysed for the conditions of 2015 and for three projections for the year 2050. The results highlight the challenges of mitigating ozone formed by emissions of the transport sector, caused by the non-linearitiy of the ozone chemistry and the long lifetime.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Siting Li, Yiming Liu, Yuqi Zhu, Yinbao Jin, Yingying Hong, Ao Shen, Yifei Xu, Haofan Wang, Haichao Wang, Xiao Lu, Shaojia Fan, and Qi Fan
Atmos. Chem. Phys., 24, 11521–11544, https://doi.org/10.5194/acp-24-11521-2024, https://doi.org/10.5194/acp-24-11521-2024, 2024
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This study establishes an inventory of anthropogenic chlorine emissions in China in 2019 with expanded species (HCl, Cl-, Cl2, HOCl) and sources (41 specific sources). The inventory is validated by a modeling study against the observations. This study enhances the understanding of anthropogenic chlorine emissions in the atmosphere, identifies key sources, and provides scientific support for pollution control and climate change.
Willem E. van Caspel, Zbigniew Klimont, Chris Heyes, and Hilde Fagerli
Atmos. Chem. Phys., 24, 11545–11563, https://doi.org/10.5194/acp-24-11545-2024, https://doi.org/10.5194/acp-24-11545-2024, 2024
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Methane in the atmosphere contributes to the production of ozone gas – an air pollutant and greenhouse gas. Our results highlight that simultaneous reductions in methane emissions help avoid offsetting the air pollution benefits already achieved by the already-approved precursor emission reductions by 2050 in the European Monitoring and Evaluation Programme region, while also playing an important role in bringing air pollution further down towards World Health Organization guideline limits.
Tia R. Scarpelli, Paul I. Palmer, Mark Lunt, Ingrid Super, and Arjan Droste
Atmos. Chem. Phys., 24, 10773–10791, https://doi.org/10.5194/acp-24-10773-2024, https://doi.org/10.5194/acp-24-10773-2024, 2024
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Under the Paris Agreement, countries must track their anthropogenic greenhouse gas emissions. This study describes a method to determine self-consistent estimates for combustion emissions and natural fluxes of CO2 from atmospheric data. We report consistent estimates inferred using this approach from satellite data and ground-based data over Europe, suggesting that satellite data can be used to determine national anthropogenic CO2 emissions for countries where ground-based CO2 data are absent.
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 9899–9921, https://doi.org/10.5194/acp-24-9899-2024, https://doi.org/10.5194/acp-24-9899-2024, 2024
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Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterize and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
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Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Beth S. Nelson, Zhenze Liu, Freya A. Squires, Marvin Shaw, James R. Hopkins, Jacqueline F. Hamilton, Andrew R. Rickard, Alastair C. Lewis, Zongbo Shi, and James D. Lee
Atmos. Chem. Phys., 24, 9031–9044, https://doi.org/10.5194/acp-24-9031-2024, https://doi.org/10.5194/acp-24-9031-2024, 2024
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The impact of combined air quality and carbon neutrality policies on O3 formation in Beijing was investigated. Emissions inventory data were used to estimate future pollutant mixing ratios relative to ground-level observations. O3 production was found to be most sensitive to changes in alkenes, but large reductions in less reactive compounds led to larger reductions in future O3 production. This study highlights the importance of understanding the emissions of organic pollutants.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
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We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
Atmos. Chem. Phys., 24, 8607–8624, https://doi.org/10.5194/acp-24-8607-2024, https://doi.org/10.5194/acp-24-8607-2024, 2024
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Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone, but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side by side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
Victor Lannuque and Karine Sartelet
Atmos. Chem. Phys., 24, 8589–8606, https://doi.org/10.5194/acp-24-8589-2024, https://doi.org/10.5194/acp-24-8589-2024, 2024
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation and speciation from naphthalene oxidation. This study details the development of the first near-explicit chemical scheme for naphthalene oxidation by OH, which includes kinetic and mechanistic data, and is able to reproduce most of the experimentally identified products in both gas and particle phases.
Tong Sha, Siyu Yang, Qingcai Chen, Liangqing Li, Xiaoyan Ma, Yan-Lin Zhang, Zhaozhong Feng, K. Folkert Boersma, and Jun Wang
Atmos. Chem. Phys., 24, 8441–8455, https://doi.org/10.5194/acp-24-8441-2024, https://doi.org/10.5194/acp-24-8441-2024, 2024
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Using an updated soil reactive nitrogen emission scheme in the Unified Inputs for Weather Research and Forecasting coupled with Chemistry (UI-WRF-Chem) model, we investigate the role of soil NO and HONO (Nr) emissions in air quality and temperature in North China. Contributions of soil Nr emissions to O3 and secondary pollutants are revealed, exceeding effects of soil NOx or HONO emission. Soil Nr emissions play an important role in mitigating O3 pollution and addressing climate change.
Jian Zhu, Shanshan Wang, Chuanqi Gu, Zhiwen Jiang, Sanbao Zhang, Ruibin Xue, Yuhao Yan, and Bin Zhou
Atmos. Chem. Phys., 24, 8383–8395, https://doi.org/10.5194/acp-24-8383-2024, https://doi.org/10.5194/acp-24-8383-2024, 2024
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In 2022, Shanghai implemented city-wide static management measures during the high-ozone season in April and May, providing a chance to study ozone pollution control. Despite significant emissions reductions, ozone levels increased by 23 %. Statistically, the number of days with higher ozone diurnal variation types increased during the lockdown period. The uneven decline in VOC and NO2 emissions led to heightened photochemical processes, resulting in the observed ozone level rise.
Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
Atmos. Chem. Phys., 24, 8317–8342, https://doi.org/10.5194/acp-24-8317-2024, https://doi.org/10.5194/acp-24-8317-2024, 2024
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Ethane and propane are volatile organic compounds emitted from human activities which help to form ozone, a pollutant and greenhouse gas, and also affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job of reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emissions, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
Rodrigo J. Seguel, Lucas Castillo, Charlie Opazo, Néstor Y. Rojas, Thiago Nogueira, María Cazorla, Mario Gavidia-Calderón, Laura Gallardo, René Garreaud, Tomás Carrasco-Escaff, and Yasin Elshorbany
Atmos. Chem. Phys., 24, 8225–8242, https://doi.org/10.5194/acp-24-8225-2024, https://doi.org/10.5194/acp-24-8225-2024, 2024
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Trends of surface ozone were examined across South America. Our findings indicate that ozone trends in major South American cities either increase or remain steady, with no signs of decline. The upward trends can be attributed to chemical regimes that efficiently convert nitric oxide into nitrogen dioxide. Additionally, our results suggest a climate penalty for ozone driven by meteorological conditions that favor wildfire propagation in Chile and extensive heat waves in southern Brazil.
Maarten Krol, Bart van Stratum, Isidora Anglou, and Klaas Folkert Boersma
Atmos. Chem. Phys., 24, 8243–8262, https://doi.org/10.5194/acp-24-8243-2024, https://doi.org/10.5194/acp-24-8243-2024, 2024
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This paper presents detailed plume simulations of nitrogen oxides and carbon dioxide that are emitted from four large industrial facilities world-wide. Results from the high-resolution simulations that include atmospheric chemistry are compared to nitrogen dioxide observations from satellites. We find good performance of the model and show that common assumptions that are used in simplified models need revision. This work is important for the monitoring of emissions using satellite data.
Robin Plauchu, Audrey Fortems-Cheiney, Grégoire Broquet, Isabelle Pison, Antoine Berchet, Elise Potier, Gaëlle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, and Henk Eskes
Atmos. Chem. Phys., 24, 8139–8163, https://doi.org/10.5194/acp-24-8139-2024, https://doi.org/10.5194/acp-24-8139-2024, 2024
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This study uses the Community Inversion Framework and CHIMERE model to assess the potential of TROPOMI-S5P PAL NO2 tropospheric column data to estimate NOx emissions in France (2019–2021). Results show a 3 % decrease in average emissions compared to the 2016 CAMS-REG/INS, lower than the 14 % decrease from CITEPA. The study highlights challenges in capturing emission anomalies due to limited data coverage and error levels but shows promise for local inventory improvements.
Zhendong Lu, Jun Wang, Yi Wang, Daven K. Henze, Xi Chen, Tong Sha, and Kang Sun
Atmos. Chem. Phys., 24, 7793–7813, https://doi.org/10.5194/acp-24-7793-2024, https://doi.org/10.5194/acp-24-7793-2024, 2024
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In contrast with past work showing that the reduction of emissions was the dominant factor for the nationwide increase of surface O3 during the lockdown in China, this study finds that the variation in meteorology (temperature and other parameters) plays a more important role. This result is obtained through sensitivity simulations using a chemical transport model constrained by satellite (TROPOMI) data and calibrated with surface observations.
Xiaohong Yao and Leiming Zhang
Atmos. Chem. Phys., 24, 7773–7791, https://doi.org/10.5194/acp-24-7773-2024, https://doi.org/10.5194/acp-24-7773-2024, 2024
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This study investigates long-term trends of criteria air pollutants, including NO2, CO, SO2, O3 and PM2.5, and NO2+O3 measured in 10 Canadian cities during the last 2 to 3 decades. We also investigate associated driving forces in terms of emission reductions, perturbations from varying weather conditions and large-scale wildfires, as well as changes in O3 sources and sinks.
Yao Ge, Sverre Solberg, Mathew R. Heal, Stefan Reimann, Willem van Caspel, Bryan Hellack, Thérèse Salameh, and David Simpson
Atmos. Chem. Phys., 24, 7699–7729, https://doi.org/10.5194/acp-24-7699-2024, https://doi.org/10.5194/acp-24-7699-2024, 2024
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Atmospheric volatile organic compounds (VOCs) constitute many species, acting as precursors to ozone and aerosol. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the EMEP MSC-W to evaluate emission inventories in Europe. We focus on the varying agreement between modelled and measured VOCs across different species and underscore potential inaccuracies in total and sector-specific emission estimates.
Shuzhuang Feng, Fei Jiang, Tianlu Qian, Nan Wang, Mengwei Jia, Songci Zheng, Jiansong Chen, Fang Ying, and Weimin Ju
Atmos. Chem. Phys., 24, 7481–7498, https://doi.org/10.5194/acp-24-7481-2024, https://doi.org/10.5194/acp-24-7481-2024, 2024
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We developed a multi-air-pollutant inversion system to estimate non-methane volatile organic compound (NMVOC) emissions using TROPOMI formaldehyde retrievals. We found that the inversion significantly improved formaldehyde simulations and reduced NMVOC emission uncertainties. The optimized NMVOC emissions effectively corrected the overestimation of O3 levels, mainly by decreasing the rate of the RO2 + NO reaction and increasing the rate of the NO2 + OH reaction.
Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, and Sunyoung Park
Atmos. Chem. Phys., 24, 7309–7330, https://doi.org/10.5194/acp-24-7309-2024, https://doi.org/10.5194/acp-24-7309-2024, 2024
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We analyzed with an inversion model the atmospheric abundance of hydrofluorocarbons (HFCs), potent greenhouse gases, from 2008 to 2020 at Gosan station in South Korea and revealed a significant increase in emissions, especially from eastern China and Japan. This increase contradicts reported data, underscoring the need for accurate monitoring and reporting. Our findings are crucial for understanding and managing global HFCs emissions, highlighting the importance of efforts to reduce HFCs.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O. T. Pye
EGUsphere, https://doi.org/10.5194/egusphere-2024-1680, https://doi.org/10.5194/egusphere-2024-1680, 2024
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Here, we develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry representation, we then estimate the cancer risk in the contiguous US from exposure to ambient formaldehyde and estimate 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Laura Hyesung Yang, Daniel J. Jacob, Ruijun Dang, Yujin J. Oak, Haipeng Lin, Jhoon Kim, Shixian Zhai, Nadia K. Colombi, Drew C. Pendergrass, Ellie Beaudry, Viral Shah, Xu Feng, Robert M. Yantosca, Heesung Chong, Junsung Park, Hanlim Lee, Won-Jin Lee, Soontae Kim, Eunhye Kim, Katherine R. Travis, James H. Crawford, and Hong Liao
Atmos. Chem. Phys., 24, 7027–7039, https://doi.org/10.5194/acp-24-7027-2024, https://doi.org/10.5194/acp-24-7027-2024, 2024
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The Geostationary Environment Monitoring Spectrometer (GEMS) provides hourly measurements of NO2. We use the chemical transport model to find how emissions, chemistry, and transport drive the changes in NO2 observed by GEMS at different times of the day. In winter, the chemistry plays a minor role, and high daytime emissions dominate the diurnal variation in NO2, balanced by transport. In summer, emissions, chemistry, and transport play an important role in shaping the diurnal variation in NO2.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
EGUsphere, https://doi.org/10.5194/egusphere-2024-1715, https://doi.org/10.5194/egusphere-2024-1715, 2024
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Climate change will bring about changes in parameters that are currently used in global-scale models to calculate biogenic emissions. This study seeks to understand the factors driving these models by comparing long-term datasets of biogenic compounds to modeled emissions. We note that the light-dependent fractions currently used in models do not accurately represent regional observations. We provide evidence for the time-dependent variation of this parameter for future modifications to models.
M. Omar Nawaz, Jeremiah Johnson, Greg Yarwood, Benjamin de Foy, Laura Judd, and Daniel L. Goldberg
Atmos. Chem. Phys., 24, 6719–6741, https://doi.org/10.5194/acp-24-6719-2024, https://doi.org/10.5194/acp-24-6719-2024, 2024
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NO2 is a gas with implications for air pollution. A campaign conducted in Houston provided an opportunity to compare NO2 from different instruments and a model. Aircraft and satellite observations agreed well with measurements on the ground; however, the latter estimated lower values. We find that model-simulated NO2 was lower than observations, especially downtown, suggesting that NO2 sources associated with the urban core of Houston, such as vehicle emissions, may be underestimated.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonne, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1450, https://doi.org/10.5194/egusphere-2024-1450, 2024
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Processes influencing dispersion of local anthropogenic emissions in Arctic wintertime are investigated with dispersion model simulations. Modelled power plant plume rise that considers surface and elevated temperature inversions improves results compared to observations. Modelled near-surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching -35 °C are required to reproduce observed NOx.
Tianlang Zhao, Jingqiu Mao, Zolal Ayazpour, Gonzalo González Abad, Caroline R. Nowlan, and Yiqi Zheng
Atmos. Chem. Phys., 24, 6105–6121, https://doi.org/10.5194/acp-24-6105-2024, https://doi.org/10.5194/acp-24-6105-2024, 2024
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HCHO variability is a key tracer in understanding VOC emissions in response to climate change. We investigate the role of methane oxidation and biogenic and wildfire emissions in HCHO interannual variability over northern high latitudes in summer, emphasizing wildfires as a key driver of HCHO interannual variability in Alaska, Siberia and northern Canada using satellite HCHO and SIF retrievals and then GEOS-Chem model. We show SIF is a tool to understand biogenic HCHO variability in this region.
Jianghao Li, Alastair C. Lewis, Jim R. Hopkins, Stephen J. Andrews, Tim Murrells, Neil Passant, Ben Richmond, Siqi Hou, William J. Bloss, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 24, 6219–6231, https://doi.org/10.5194/acp-24-6219-2024, https://doi.org/10.5194/acp-24-6219-2024, 2024
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A summertime ozone event at an urban site in Birmingham is sensitive to volatile organic compounds (VOCs) – particularly those of oxygenated VOCs. The roles of anthropogenic VOC sources in urban ozone chemistry are examined by integrating the 1990–2019 national atmospheric emission inventory into model scenarios. Road transport remains the most powerful means of further reducing ozone in this case study, but the benefits may be offset if solvent emissions of VOCs continue to increase.
Kai-Lan Chang, Owen R. Cooper, Audrey Gaudel, Irina Petropavlovskikh, Peter Effertz, Gary Morris, and Brian C. McDonald
Atmos. Chem. Phys., 24, 6197–6218, https://doi.org/10.5194/acp-24-6197-2024, https://doi.org/10.5194/acp-24-6197-2024, 2024
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A great majority of observational trend studies of free tropospheric ozone use sparsely sampled ozonesonde and aircraft measurements as reference data sets. A ubiquitous assumption is that trends are accurate and reliable so long as long-term records are available. We show that sampling bias due to sparse samples can persistently reduce the trend accuracy, and we highlight the importance of maintaining adequate frequency and continuity of observations.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Fu-Jie Zhu, Zi-Feng Zhang, Li-Yan Liu, Pu-Fei Yang, Peng-Tuan Hu, Geng-Bo Ren, Meng Qin, and Wan-Li Ma
Atmos. Chem. Phys., 24, 6095–6103, https://doi.org/10.5194/acp-24-6095-2024, https://doi.org/10.5194/acp-24-6095-2024, 2024
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Gas–particle (G–P) partitioning is an important atmospheric behavior for semi-volatile organic compounds (SVOCs). Diurnal variation in G–P partitioning of methylated polycyclic aromatic hydrocarbons (Me-PAHs) demonstrates the possible influence of gaseous degradation; the enhancement of gaseous degradation (1.10–5.58 times) on G–P partitioning is verified by a steady-state G–P partitioning model. The effect of gaseous degradation on G–P partitioning of (especially light) SVOCs is important.
Christoph Staehle, Harald E. Rieder, Arlene M. Fiore, and Jordan L. Schnell
Atmos. Chem. Phys., 24, 5953–5969, https://doi.org/10.5194/acp-24-5953-2024, https://doi.org/10.5194/acp-24-5953-2024, 2024
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Chemistry–climate models show biases compared to surface ozone observations and thus require bias correction for impact studies and the assessment of air quality changes. We compare the performance of commonly used correction techniques for model outputs available via CMIP6. While all methods can reduce model biases, better results are obtained from more complex approaches. Thus, our study suggests broader use of these techniques in studies seeking to inform air quality management and policy.
Deepangsu Chatterjee, Randall V. Martin, Chi Li, Dandan Zhang, Haihui Zhu, Daven K. Henze, James H. Crawford, Ronald C. Cohen, Lok N. Lamsal, and Alexander M. Cede
EGUsphere, https://doi.org/10.5194/egusphere-2024-1401, https://doi.org/10.5194/egusphere-2024-1401, 2024
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We investigate the hourly variation of NO2 columns and surface concentrations by applying the GEOS-Chem model to interpret aircraft and ground-based measurements over the US, and Pandora sun photometer measurements over the US, Europe, and Asia. Corrections to the Pandora columns and finer model resolution improve the modeled representation of the summertime hourly variation of total NO2 columns to enable explaining the weaker hourly variation in NO2 columns than at the surface.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William Stockwell, Luc Vereecken, and Tim Wallington
EGUsphere, https://doi.org/10.5194/egusphere-2024-1316, https://doi.org/10.5194/egusphere-2024-1316, 2024
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Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes of the atmospheric composition. Therefore, accurate chemical mechanisms are necessary to predict the evolution of air pollution and climate change. The article describes all steps that are needed to build chemical mechanisms and discusses advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, J. Andrew Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
Atmos. Chem. Phys., 24, 5265–5286, https://doi.org/10.5194/acp-24-5265-2024, https://doi.org/10.5194/acp-24-5265-2024, 2024
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Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represents VOC chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from volatile chemical products and other anthropogenic sources to total VOC reactivity and O3.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Alba Lorente, Zichong Chen, Xiao Lu, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Margaux Winter, Shuang Ma, A. Anthony Bloom, John R. Worden, Robert N. Stavins, and Cynthia A. Randles
Atmos. Chem. Phys., 24, 5069–5091, https://doi.org/10.5194/acp-24-5069-2024, https://doi.org/10.5194/acp-24-5069-2024, 2024
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We quantify 2019 methane emissions in the contiguous US (CONUS) at a ≈ 25 km × 25 km resolution using satellite methane observations. We find a 13 % upward correction to the 2023 US Environmental Protection Agency (EPA) Greenhouse Gas Emissions Inventory (GHGI) for 2019, with large corrections to individual states, urban areas, and landfills. This may present a challenge for US climate policies and goals, many of which target significant reductions in methane emissions.
David de la Paz, Rafael Borge, Juan Manuel de Andrés, Luis Tovar, Golam Sarwar, and Sergey L. Napelenok
Atmos. Chem. Phys., 24, 4949–4972, https://doi.org/10.5194/acp-24-4949-2024, https://doi.org/10.5194/acp-24-4949-2024, 2024
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This source apportionment modeling study shows that around 70 % of ground-level O3 in Madrid (Spain) is transported from other regions. Nonetheless, emissions from local sources, mainly road traffic, play a significant role, especially under atmospheric stagnation. Local measures during those conditions may be able to reduce O3 peaks by up to 30 % and, thus, lessen impacts from high-O3 episodes in the Madrid metropolitan area.
Audrey Fortems-Cheiney, Gregoire Broquet, Elise Potier, Robin Plauchu, Antoine Berchet, Isabelle Pison, Hugo Denier van der Gon, and Stijn Dellaert
Atmos. Chem. Phys., 24, 4635–4649, https://doi.org/10.5194/acp-24-4635-2024, https://doi.org/10.5194/acp-24-4635-2024, 2024
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We have estimated the carbon monixide (CO) European emissions from satellite observations of the MOPITT instrument at the relatively high resolution of 0.5° for a period of over 10 years from 2011 to 2021. The analysis of the inversion results reveals the challenges associated with the inversion of CO emissions at the regional scale over Europe.
Amy Christiansen, Loretta J. Mickley, and Lu Hu
Atmos. Chem. Phys., 24, 4569–4589, https://doi.org/10.5194/acp-24-4569-2024, https://doi.org/10.5194/acp-24-4569-2024, 2024
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In this work, we provide an additional constraint on emissions and trends of nitrogen oxides using nitrate wet deposition (NWD) fluxes over the United States and Europe from 1980–2020. We find that NWD measurements constrain total NOx emissions well. We also find evidence of NOx emission overestimates in both domains, but especially over Europe, where NOx emissions are overestimated by a factor of 2. Reducing NOx emissions over Europe improves model representation of ozone at the surface.
Kiyeon Kim, Kyung Man Han, Chul Han Song, Hyojun Lee, Ross Beardsley, Jinhyeok Yu, Greg Yarwood, Bonyoung Koo, Jasper Madalipay, Jung-Hun Woo, and Seogju Cho
EGUsphere, https://doi.org/10.5194/egusphere-2024-886, https://doi.org/10.5194/egusphere-2024-886, 2024
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We incoporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratios predictions. These results expand our understanding of HONO photochemistry and identify crucial sources of HONO that impact the total HONO budget in Seoul, South Korea. Through this investigation, we contribute to resolving discrepancies in understading chemical transport models, with implications for better air quality mangement and environmental protection in the region.
Eduardo Torre-Pascual, Gotzon Gangoiti, Ana Rodríguez-García, Estibaliz Sáez de Cámara, Joana Ferreira, Carla Gama, María Carmen Gómez, Iñaki Zuazo, Jose Antonio García, and Maite de Blas
Atmos. Chem. Phys., 24, 4305–4329, https://doi.org/10.5194/acp-24-4305-2024, https://doi.org/10.5194/acp-24-4305-2024, 2024
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We present an analysis of an intense air pollution episode of tropospheric ozone (O3) along the Atlantic coast of the Iberian Peninsula, incorporating both measured and simulated parameters. Our study extends beyond surface-level factors to include altitude-related parameters. These episodes stem from upper-atmosphere O3 accumulation in preceding days, transported to surface layers, causing rapid O3 concentration increase.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyong Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
EGUsphere, https://doi.org/10.5194/egusphere-2024-811, https://doi.org/10.5194/egusphere-2024-811, 2024
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We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show, that SF6 emissions are decreasing in the USA and Europe, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, Europe, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
Hannah Chawner, Eric Saboya, Karina E. Adcock, Tim Arnold, Yuri Artioli, Caroline Dylag, Grant L. Forster, Anita Ganesan, Heather Graven, Gennadi Lessin, Peter Levy, Ingrid T. Luijkx, Alistair Manning, Penelope A. Pickers, Chris Rennick, Christian Rödenbeck, and Matthew Rigby
Atmos. Chem. Phys., 24, 4231–4252, https://doi.org/10.5194/acp-24-4231-2024, https://doi.org/10.5194/acp-24-4231-2024, 2024
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The quantity of atmospheric potential oxygen (APO), derived from coincident measurements of carbon dioxide (CO2) and oxygen (O2), has been proposed as a tracer for fossil fuel CO2 emissions. In this model sensitivity study, we examine the use of APO for this purpose in the UK and compare our model to observations. We find that our model simulations are most sensitive to uncertainties relating to ocean fluxes and boundary conditions.
Baoshuang Liu, Yao Gu, Yutong Wu, Qili Dai, Shaojie Song, Yinchang Feng, and Philip K. Hopke
EGUsphere, https://doi.org/10.5194/egusphere-2024-916, https://doi.org/10.5194/egusphere-2024-916, 2024
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Reactive loss of VOCs is a long-term issue yet to be resolved in VOC source analyses. This review assesses the common methods and existing issues of reducing losses, impacts of losses, and sources in current source analyses. We provided a potential supporting role in solving the issues of VOC conversion. Source analyses of consumed VOCs produced by reactions for O3 and secondary organic aerosols can play an important role in effective prevention and control of atmospheric secondary pollution.
Meng Li, Junichi Kurokawa, Qiang Zhang, Jung-Hun Woo, Tazuko Morikawa, Satoru Chatani, Zifeng Lu, Yu Song, Guannan Geng, Hanwen Hu, Jinseok Kim, Owen R. Cooper, and Brian C. McDonald
Atmos. Chem. Phys., 24, 3925–3952, https://doi.org/10.5194/acp-24-3925-2024, https://doi.org/10.5194/acp-24-3925-2024, 2024
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In this work, we developed MIXv2, a mosaic Asian emission inventory for 2010–2017. With high spatial (0.1°) and monthly temporal resolution, MIXv2 integrates anthropogenic and open biomass burning emissions across seven sectors following a mosaic methodology. It provides CO2 emissions data alongside nine key pollutants and three chemical mechanisms. Our publicly accessible gridded monthly emissions data can facilitate long-term atmospheric and climate model analyses.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-693, https://doi.org/10.5194/egusphere-2024-693, 2024
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This paper employs a regional chemical transport model to quantify the sensitivity of air pollutants and photochemical parameters to specified emission reductions in China for conditions of winter and summer as representative. The study provides insights into the further air quality control in China with reduced primary emissions.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
EGUsphere, https://doi.org/10.5194/egusphere-2024-715, https://doi.org/10.5194/egusphere-2024-715, 2024
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This work uses WRF-Chem and chemical box modeling to study the gas and aqueous phase production of organic acid concentrations measured in cloud water the summit of Whiteface Mountain on July 1st, 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Xiaomeng Zhang, Yongjian Lian, Shendong Tan, and Shi Yin
Atmos. Chem. Phys., 24, 3593–3612, https://doi.org/10.5194/acp-24-3593-2024, https://doi.org/10.5194/acp-24-3593-2024, 2024
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Atmospheric new particle formation (NPF) has a significant influence on the global climate, local air quality and human health. Using a combination of quantum chemical calculations and kinetics modeling, we find that thhe gas-phase organosulfate produced from consumption of SO3 can significantly enhance SA–DMA nucleation in the polluted boundary layer, resulting in non-negligible contributions to NPF. Our findings provide important insights into organic sulfur in atmospheric aerosol formation.
Yasin Elshorbany, Jerald Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca Buchholz, Benjamin Gaubert, Néstor Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
EGUsphere, https://doi.org/10.5194/egusphere-2024-720, https://doi.org/10.5194/egusphere-2024-720, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the Tropospheric Column of Ozone and its precursors, nitrogen dioxide, formaldehyde, and total column of CO as well as ozonesonde data and model simulations.
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Short summary
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.
We developed the Southern Ontario CO2 Emissions (SOCE) inventory, which identifies the spatial...
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