Articles | Volume 16, issue 6
https://doi.org/10.5194/acp-16-3743-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-3743-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
21 Mar 2016
Research article |
| 21 Mar 2016
Mercury oxidation from bromine chemistry in the free troposphere over the southeastern US
Sean Coburn
Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder, CO, USA
Cooperative Institute for Research in Environmental Sciences (CIRES), Boulder, CO, USA
Barbara Dix
Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder, CO, USA
Eric Edgerton
Atmospheric Research and Analysis (ARA) Inc., Plano, TX, USA
Christopher D. Holmes
Department of Earth, Ocean and Atmospheric Science, Florida State University, Tallahassee, FL, USA
Douglas Kinnison
National Center for Atmospheric Research (NCAR), Boulder, CO, USA
Qing Liang
NASA Goddard Space Flight Center, Atmospheric Chemistry and Dynamics Branch, Greenbelt, MD 20771, USA
Arnout ter Schure
Electric Power Research Institute (EPRI), Palo Alto, CA, USA
Siyuan Wang
Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder, CO, USA
Cooperative Institute for Research in Environmental Sciences (CIRES), Boulder, CO, USA
now at: Department of Chemistry, University of Michigan, Ann Arbor, MI, USA
Rainer Volkamer
CORRESPONDING AUTHOR
Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder, CO, USA
Cooperative Institute for Research in Environmental Sciences (CIRES), Boulder, CO, USA
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Olivia E. Clifton, Donna Schwede, Christian Hogrefe, Jesse O. Bash, Sam Bland, Philip Cheung, Mhairi Coyle, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christopher D. Holmes, László Horváth, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Pérez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamás Weidinger, Zhiyong Wu, and Leiming Zhang
Atmos. Chem. Phys., 23, 9911–9961, https://doi.org/10.5194/acp-23-9911-2023, https://doi.org/10.5194/acp-23-9911-2023, 2023
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Michael Weimer, Douglas E. Kinnison, Catherine Wilka, and Susan Solomon
Atmos. Chem. Phys., 23, 6849–6861, https://doi.org/10.5194/acp-23-6849-2023, https://doi.org/10.5194/acp-23-6849-2023, 2023
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We investigate the influence of the number density of nitric acid trihydrate (NAT) particles on associated trace gases in the lower stratosphere using data from a satellite, ozonesondes and simulations by a community chemistry climate model. By comparing probability density functions between observations and the model, we find that the standard NAT number density should be reduced for future simulations with the model.
Tobias Borsdorff, Teresa Campos, Natalie Kille, Kyle J. Zarzana, Rainer Volkamer, and Jochen Landgraf
Atmos. Meas. Tech., 16, 3027–3038, https://doi.org/10.5194/amt-16-3027-2023, https://doi.org/10.5194/amt-16-3027-2023, 2023
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Joey C. Y. Lam, Amos P. K. Tai, Jason A. Ducker, and Christopher D. Holmes
Geosci. Model Dev., 16, 2323–2342, https://doi.org/10.5194/gmd-16-2323-2023, https://doi.org/10.5194/gmd-16-2323-2023, 2023
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We developed a new component within an atmospheric chemistry model to better simulate plant ecophysiological processes relevant for ozone air quality. We showed that it reduces simulated biases in plant uptake of ozone in prior models. The new model enables us to explore how future climatic changes affect air quality via affecting plants, examine ozone–vegetation interactions and feedbacks, and evaluate the impacts of changing atmospheric chemistry and climate on vegetation productivity.
John T. Walker, Xi Chen, Zhiyong Wu, Donna Schwede, Ryan Daly, Aleksandra Djurkovic, A. Christopher Oishi, Eric Edgerton, Jesse Bash, Jennifer Knoepp, Melissa Puchalski, John Iiames, and Chelcy F. Miniat
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Radical bromine molecules are seen at higher concentrations during the Arctic spring. We use the global model GEOS-Chem to test whether snowpack and wind-blown snow sources can explain high bromine concentrations. We run this model for the entire year of 2015 and compare results to observations of bromine from floating platforms on the Arctic Ocean and at Utqiaġvik. We find that the model performs best when both sources are enabled but may overestimate bromine production in summer and fall.
Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah A. Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, Benjamin A. Nault, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech., 15, 4901–4930, https://doi.org/10.5194/amt-15-4901-2022, https://doi.org/10.5194/amt-15-4901-2022, 2022
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Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
Christopher D. Holmes
Atmos. Chem. Phys., 22, 9011–9015, https://doi.org/10.5194/acp-22-9011-2022, https://doi.org/10.5194/acp-22-9011-2022, 2022
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Cloud water and ice enable reactions that lead to acid rain and alter atmospheric oxidants, among other impacts. This work develops and evaluates an efficient method of simulating cloud chemistry within global and regional atmospheric models in order to better understand the role of clouds in atmospheric chemistry.
Lucien Froidevaux, Douglas E. Kinnison, Michelle L. Santee, Luis F. Millán, Nathaniel J. Livesey, William G. Read, Charles G. Bardeen, John J. Orlando, and Ryan A. Fuller
Atmos. Chem. Phys., 22, 4779–4799, https://doi.org/10.5194/acp-22-4779-2022, https://doi.org/10.5194/acp-22-4779-2022, 2022
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We analyze satellite-derived distributions of chlorine monoxide (ClO) and hypochlorous acid (HOCl) in the upper atmosphere. For 2005–2020, from 50°S to 50°N and over ~30 to 45 km, ClO and HOCl decreased by −0.7 % and −0.4 % per year, respectively. A detailed model of chemistry and dynamics agrees with the results. These decreases confirm the effectiveness of the 1987 Montreal Protocol, which limited emissions of chlorine- and bromine-containing source gases, in order to protect the ozone layer.
Shihan Sun, Amos P. K. Tai, David H. Y. Yung, Anthony Y. H. Wong, Jason A. Ducker, and Christopher D. Holmes
Biogeosciences, 19, 1753–1776, https://doi.org/10.5194/bg-19-1753-2022, https://doi.org/10.5194/bg-19-1753-2022, 2022
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We developed and used a terrestrial biosphere model to compare and evaluate widely used empirical dry deposition schemes with different stomatal approaches and found that using photosynthesis-based stomatal approaches can reduce biases in modeled dry deposition velocities in current chemical transport models. Our study shows systematic errors in current dry deposition schemes and the importance of representing plant ecophysiological processes in models under a changing climate.
Matthias Schneider, Benjamin Ertl, Christopher J. Diekmann, Farahnaz Khosrawi, Andreas Weber, Frank Hase, Michael Höpfner, Omaira E. García, Eliezer Sepúlveda, and Douglas Kinnison
Earth Syst. Sci. Data, 14, 709–742, https://doi.org/10.5194/essd-14-709-2022, https://doi.org/10.5194/essd-14-709-2022, 2022
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We present atmospheric H2O, HDO / H2O ratio, N2O, CH4, and HNO3 data generated by the MUSICA IASI processor using thermal nadir spectra measured by the IASI satellite instrument. The data have global daily coverage and are available for the period between October 2014 and June 2021. Multiple possibilities of data reuse are offered by providing each individual data product together with information about retrieval settings and the products' uncertainty and vertical representativeness.
Dongwook Kim, Changmin Cho, Seokhan Jeong, Soojin Lee, Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Jose L. Jimenez, Rainer Volkamer, Donald R. Blake, Armin Wisthaler, Alan Fried, Joshua P. DiGangi, Glenn S. Diskin, Sally E. Pusede, Samuel R. Hall, Kirk Ullmann, L. Gregory Huey, David J. Tanner, Jack Dibb, Christoph J. Knote, and Kyung-Eun Min
Atmos. Chem. Phys., 22, 805–821, https://doi.org/10.5194/acp-22-805-2022, https://doi.org/10.5194/acp-22-805-2022, 2022
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CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. CHOCHO concentration was high in large cities, aromatics being the most important precursors. Loss path to aerosol was the highest sink, contributing to ~ 20 % of secondary organic aerosol formation. Our work highlights that simple CHOCHO surface uptake approach is valid only for low aerosol conditions and more work is required to understand CHOCHO solubility in high-aerosol conditions.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Debora Griffin, Chris A. McLinden, Enrico Dammers, Cristen Adams, Chelsea E. Stockwell, Carsten Warneke, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Kyle J. Zarzana, Jake P. Rowe, Rainer Volkamer, Christoph Knote, Natalie Kille, Theodore K. Koenig, Christopher F. Lee, Drew Rollins, Pamela S. Rickly, Jack Chen, Lukas Fehr, Adam Bourassa, Doug Degenstein, Katherine Hayden, Cristian Mihele, Sumi N. Wren, John Liggio, Ayodeji Akingunola, and Paul Makar
Atmos. Meas. Tech., 14, 7929–7957, https://doi.org/10.5194/amt-14-7929-2021, https://doi.org/10.5194/amt-14-7929-2021, 2021
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Satellite-derived NOx emissions from biomass burning are estimated with TROPOMI observations. Two common emission estimation methods are applied, and sensitivity tests with model output were performed to determine the accuracy of these methods. The effect of smoke aerosols on TROPOMI NO2 columns is estimated and compared to aircraft observations from four different aircraft campaigns measuring biomass burning plumes in 2018 and 2019 in North America.
Jin Liao, Glenn M. Wolfe, Reem A. Hannun, Jason M. St. Clair, Thomas F. Hanisco, Jessica B. Gilman, Aaron Lamplugh, Vanessa Selimovic, Glenn S. Diskin, John B. Nowak, Hannah S. Halliday, Joshua P. DiGangi, Samuel R. Hall, Kirk Ullmann, Christopher D. Holmes, Charles H. Fite, Anxhelo Agastra, Thomas B. Ryerson, Jeff Peischl, Ilann Bourgeois, Carsten Warneke, Matthew M. Coggon, Georgios I. Gkatzelis, Kanako Sekimoto, Alan Fried, Dirk Richter, Petter Weibring, Eric C. Apel, Rebecca S. Hornbrook, Steven S. Brown, Caroline C. Womack, Michael A. Robinson, Rebecca A. Washenfelder, Patrick R. Veres, and J. Andrew Neuman
Atmos. Chem. Phys., 21, 18319–18331, https://doi.org/10.5194/acp-21-18319-2021, https://doi.org/10.5194/acp-21-18319-2021, 2021
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Formaldehyde (HCHO) is an important oxidant precursor and affects the formation of O3 and other secondary pollutants in wildfire plumes. We disentangle the processes controlling HCHO evolution from wildfire plumes sampled by NASA DC-8 during FIREX-AQ. We find that OH abundance rather than normalized OH reactivity is the main driver of fire-to-fire variability in HCHO secondary production and estimate an effective HCHO yield per volatile organic compound molecule oxidized in wildfire plumes.
Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Sharmine Akter Simu, Yuzo Miyazaki, Eri Tachibana, Henning Finkenzeller, Jérôme Brioude, Aurélie Colomb, Olivier Magand, Bert Verreyken, Stephanie Evan, Rainer Volkamer, and Trissevgeni Stavrakou
Atmos. Chem. Phys., 21, 17017–17029, https://doi.org/10.5194/acp-21-17017-2021, https://doi.org/10.5194/acp-21-17017-2021, 2021
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The tropical Indian Ocean (IO) is expected to be a significant source of water-soluble organic carbon (WSOC), which is relevant to cloud formation. Our study showed that marine secondary organic formation dominantly contributed to the aerosol WSOC mass at the high-altitude observatory in the southwest IO in the wet season in both marine boundary layer and free troposphere (FT). This suggests that the effect of marine secondary sources is important up to FT, a process missing in climate models.
Nicole Jacobs, William R. Simpson, Kelly A. Graham, Christopher Holmes, Frank Hase, Thomas Blumenstock, Qiansi Tu, Matthias Frey, Manvendra K. Dubey, Harrison A. Parker, Debra Wunch, Rigel Kivi, Pauli Heikkinen, Justus Notholt, Christof Petri, and Thorsten Warneke
Atmos. Chem. Phys., 21, 16661–16687, https://doi.org/10.5194/acp-21-16661-2021, https://doi.org/10.5194/acp-21-16661-2021, 2021
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Spatial patterns of carbon dioxide seasonal cycle amplitude and summer drawdown timing derived from the OCO-2 satellite over northern high latitudes agree well with corresponding estimates from two models. The Asian boreal forest is anomalous with the largest amplitude and earliest seasonal drawdown. Modeled land contact tracers suggest that accumulated CO2 exchanges during atmospheric transport play a major role in shaping carbon dioxide seasonality in northern high-latitude regions.
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Georgios I. Gkatzelis, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Felix Piel, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Kanako Sekimoto, Lee Thornhill, Joel A. Thornton, Geoffrey S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Carsten Warneke, Rebecca A. Washenfelder, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Armin Wisthaler, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys., 21, 16293–16317, https://doi.org/10.5194/acp-21-16293-2021, https://doi.org/10.5194/acp-21-16293-2021, 2021
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To understand air quality impacts from wildfires, we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical
nighttimechemistry thrives and controls the fate of key smoke plume chemical processes.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Tomás Sherwen, Rainer Volkamer, Theodore K. Koenig, Tanguy Giroud, and Thomas Peter
Geosci. Model Dev., 14, 6623–6645, https://doi.org/10.5194/gmd-14-6623-2021, https://doi.org/10.5194/gmd-14-6623-2021, 2021
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Here, we present the iodine chemistry module in the SOCOL-AERv2 model. The obtained iodine distribution demonstrated a good agreement when validated against other simulations and available observations. We also estimated the iodine influence on ozone in the case of present-day iodine emissions, the sensitivity of ozone to doubled iodine emissions, and when considering only organic or inorganic iodine sources. The new model can be used as a tool for further studies of iodine effects on ozone.
Catherine Wilka, Susan Solomon, Doug Kinnison, and David Tarasick
Atmos. Chem. Phys., 21, 15771–15781, https://doi.org/10.5194/acp-21-15771-2021, https://doi.org/10.5194/acp-21-15771-2021, 2021
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We use satellite and balloon measurements to evaluate modeled ozone loss seen in the unusually cold Arctic of 2020 in the real world and compare it to simulations of a world avoided. We show that extensive denitrification in 2020 provides an important test case for stratospheric model process representations. If the Montreal Protocol had not banned ozone-depleting substances, an Arctic ozone hole would have emerged for the first time in spring 2020 that is comparable to those in the Antarctic.
Stefano Galmarini, Paul Makar, Olivia E. Clifton, Christian Hogrefe, Jesse O. Bash, Roberto Bellasio, Roberto Bianconi, Johannes Bieser, Tim Butler, Jason Ducker, Johannes Flemming, Alma Hodzic, Christopher D. Holmes, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Juan Luis Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Sam Silva, and Ralf Wolke
Atmos. Chem. Phys., 21, 15663–15697, https://doi.org/10.5194/acp-21-15663-2021, https://doi.org/10.5194/acp-21-15663-2021, 2021
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This technical note presents the research protocols for phase 4 of the Air Quality Model Evaluation International Initiative (AQMEII4). This initiative has three goals: (i) to define the state of wet and dry deposition in regional models, (ii) to evaluate how dry deposition influences air concentration and flux predictions, and (iii) to identify the causes for prediction differences. The evaluation compares LULC-specific dry deposition and effective conductances and fluxes.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Alexandra J. Boris, Satoshi Takahama, Andrew T. Weakley, Bruno M. Debus, Stephanie L. Shaw, Eric S. Edgerton, Taekyu Joo, Nga L. Ng, and Ann M. Dillner
Atmos. Meas. Tech., 14, 4355–4374, https://doi.org/10.5194/amt-14-4355-2021, https://doi.org/10.5194/amt-14-4355-2021, 2021
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Infrared spectrometry can be applied in routine monitoring of atmospheric particles to give comprehensive characterization of the organic material by bond rather than species. Using this technique, the concentrations of particle organic material were found to decrease 2011–2016 in the southeastern US, driven by a decline in highly aged material, concurrent with declining anthropogenic emissions. However, an increase was observed in the fraction of more moderately aged organic matter.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
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Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Chaim I. Garfinkel, Ohad Harari, Shlomi Ziskin Ziv, Jian Rao, Olaf Morgenstern, Guang Zeng, Simone Tilmes, Douglas Kinnison, Fiona M. O'Connor, Neal Butchart, Makoto Deushi, Patrick Jöckel, Andrea Pozzer, and Sean Davis
Atmos. Chem. Phys., 21, 3725–3740, https://doi.org/10.5194/acp-21-3725-2021, https://doi.org/10.5194/acp-21-3725-2021, 2021
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Water vapor is the dominant greenhouse gas in the atmosphere, and El Niño is the dominant mode of variability in the ocean–atmosphere system. The connection between El Niño and water vapor above ~ 17 km is unclear, with single-model studies reaching a range of conclusions. This study examines this connection in 12 different models. While there are substantial differences among the models, all models appear to capture the fundamental physical processes correctly.
Patrick E. Sheese, Kaley A. Walker, Chris D. Boone, Doug A. Degenstein, Felicia Kolonjari, David Plummer, Douglas E. Kinnison, Patrick Jöckel, and Thomas von Clarmann
Atmos. Meas. Tech., 14, 1425–1438, https://doi.org/10.5194/amt-14-1425-2021, https://doi.org/10.5194/amt-14-1425-2021, 2021
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Output from climate chemistry models (CMAM, EMAC, and WACCM) is used to estimate the expected geophysical variability of ozone concentrations between coincident satellite instrument measurement times and geolocations. We use the Canadian ACE-FTS and OSIRIS instruments as a case study. Ensemble mean estimates are used to optimize coincidence criteria between the two instruments, allowing for the use of more coincident profiles while providing an estimate of the geophysical variation.
Marc von Hobe, Felix Ploeger, Paul Konopka, Corinna Kloss, Alexey Ulanowski, Vladimir Yushkov, Fabrizio Ravegnani, C. Michael Volk, Laura L. Pan, Shawn B. Honomichl, Simone Tilmes, Douglas E. Kinnison, Rolando R. Garcia, and Jonathon S. Wright
Atmos. Chem. Phys., 21, 1267–1285, https://doi.org/10.5194/acp-21-1267-2021, https://doi.org/10.5194/acp-21-1267-2021, 2021
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The Asian summer monsoon (ASM) is known to foster transport of polluted tropospheric air into the stratosphere. To test and amend our picture of ASM vertical transport, we analyse distributions of airborne trace gas observations up to 20 km altitude near the main ASM vertical conduit south of the Himalayas. We also show that a new high-resolution version of the global chemistry climate model WACCM is able to reproduce the observations well.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Ales Kuchar, William Ball, Pavle Arsenovic, Ellis Remsberg, Patrick Jöckel, Markus Kunze, David A. Plummer, Andrea Stenke, Daniel Marsh, Doug Kinnison, and Thomas Peter
Atmos. Chem. Phys., 21, 201–216, https://doi.org/10.5194/acp-21-201-2021, https://doi.org/10.5194/acp-21-201-2021, 2021
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The solar signal in the mesospheric H2O and CO was extracted from the CCMI-1 model simulations and satellite observations using multiple linear regression (MLR) analysis. MLR analysis shows a pronounced and statistically robust solar signal in both H2O and CO. The model results show a general agreement with observations reproducing a negative/positive solar signal in H2O/CO. The pattern of the solar signal varies among the considered models, reflecting some differences in the model setup.
Bert Verreyken, Crist Amelynck, Jérôme Brioude, Jean-François Müller, Niels Schoon, Nicolas Kumps, Aurélie Colomb, Jean-Marc Metzger, Christopher F. Lee, Theodore K. Koenig, Rainer Volkamer, and Trissevgeni Stavrakou
Atmos. Chem. Phys., 20, 14821–14845, https://doi.org/10.5194/acp-20-14821-2020, https://doi.org/10.5194/acp-20-14821-2020, 2020
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Biomass burning (BB) plumes arriving at the Maïdo observatory located in the south-west Indian Ocean during August 2018 and August 2019 are studied using trace gas measurements, Lagrangian transport models and the CAMS near-real-time atmospheric composition service. We investigate (i) secondary production of volatile organic compounds during transport, (ii) efficacy of the CAMS model to reproduce the chemical makeup of BB plumes and (iii) the impact of BB on the remote marine boundary layer.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
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This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 20, 13011–13022, https://doi.org/10.5194/acp-20-13011-2020, https://doi.org/10.5194/acp-20-13011-2020, 2020
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Decadal trends and variations in OH are critical for understanding atmospheric CH4 evolution. We quantify the impacts of OH trends and variations on the CH4 budget by conducting CH4 inversions on a decadal scale with an ensemble of OH fields. We find the negative OH anomalies due to enhanced fires can reduce the optimized CH4 emissions by up to 10 Tg yr−1 during El Niño years and the positive OH trend from 1986 to 2010 results in a ∼ 23 Tg yr−1 additional increase in optimized CH4 emissions.
Daniele Minganti, Simon Chabrillat, Yves Christophe, Quentin Errera, Marta Abalos, Maxime Prignon, Douglas E. Kinnison, and Emmanuel Mahieu
Atmos. Chem. Phys., 20, 12609–12631, https://doi.org/10.5194/acp-20-12609-2020, https://doi.org/10.5194/acp-20-12609-2020, 2020
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The climatology of the N2O transport budget in the stratosphere is studied in the transformed Eulerian mean framework across a variety of datasets: a chemistry climate model, a chemistry transport model driven by four reanalyses and a chemical reanalysis. The impact of vertical advection on N2O agrees well in the datasets, but horizontal mixing presents large differences above the Antarctic and in the whole Northern Hemisphere.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Yang Wang, Arnoud Apituley, Alkiviadis Bais, Steffen Beirle, Nuria Benavent, Alexander Borovski, Ilya Bruchkouski, Ka Lok Chan, Sebastian Donner, Theano Drosoglou, Henning Finkenzeller, Martina M. Friedrich, Udo Frieß, David Garcia-Nieto, Laura Gómez-Martín, François Hendrick, Andreas Hilboll, Junli Jin, Paul Johnston, Theodore K. Koenig, Karin Kreher, Vinod Kumar, Aleksandra Kyuberis, Johannes Lampel, Cheng Liu, Haoran Liu, Jianzhong Ma, Oleg L. Polyansky, Oleg Postylyakov, Richard Querel, Alfonso Saiz-Lopez, Stefan Schmitt, Xin Tian, Jan-Lukas Tirpitz, Michel Van Roozendael, Rainer Volkamer, Zhuoru Wang, Pinhua Xie, Chengzhi Xing, Jin Xu, Margarita Yela, Chengxin Zhang, and Thomas Wagner
Atmos. Meas. Tech., 13, 5087–5116, https://doi.org/10.5194/amt-13-5087-2020, https://doi.org/10.5194/amt-13-5087-2020, 2020
Matt Amos, Paul J. Young, J. Scott Hosking, Jean-François Lamarque, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Markus Kunze, Marion Marchand, David A. Plummer, David Saint-Martin, Kengo Sudo, Simone Tilmes, and Yousuke Yamashita
Atmos. Chem. Phys., 20, 9961–9977, https://doi.org/10.5194/acp-20-9961-2020, https://doi.org/10.5194/acp-20-9961-2020, 2020
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We present an updated projection of Antarctic ozone hole recovery using an ensemble of chemistry–climate models. To do so, we employ a method, more advanced and skilful than the current multi-model mean standard, which is applicable to other ensemble analyses. It calculates the performance and similarity of the models, which we then use to weight the model. Calculating model similarity allows us to account for models which are constructed from similar components.
Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El-Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti P. Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, https://doi.org/10.5194/acp-20-9183-2020, 2020
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Highly oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide tropospheric-temperature range. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
Daniele Visioni, Giovanni Pitari, Vincenzo Rizi, Marco Iarlori, Irene Cionni, Ilaria Quaglia, Hideharu Akiyoshi, Slimane Bekki, Neal Butchart, Martin Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando Garcia, Patrick Joeckel, Douglas Kinnison, Jean-François Lamarque, Marion Marchand, Martine Michou, Olaf Morgenstern, Tatsuya Nagashima, Fiona M. O'Connor, Luke D. Oman, David Plummer, Eugene Rozanov, David Saint-Martin, Robyn Schofield, John Scinocca, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Holger Tost, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-525, https://doi.org/10.5194/acp-2020-525, 2020
Preprint withdrawn
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In this work we analyse the trend in ozone profiles taken at L'Aquila (Italy, 42.4° N) for seventeen years, between 2000 and 2016 and compare them against already available measured ozone trends. We try to understand and explain the observed trends at various heights in light of the simulations from seventeen different model, highlighting the contribution of changes in circulation and chemical ozone loss during this time period.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Marta Abalos, Clara Orbe, Douglas E. Kinnison, David Plummer, Luke D. Oman, Patrick Jöckel, Olaf Morgenstern, Rolando R. Garcia, Guang Zeng, Kane A. Stone, and Martin Dameris
Atmos. Chem. Phys., 20, 6883–6901, https://doi.org/10.5194/acp-20-6883-2020, https://doi.org/10.5194/acp-20-6883-2020, 2020
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A set of state-of-the art chemistry–climate models is used to examine future changes in downward transport from the stratosphere, a key contributor to tropospheric ozone. The acceleration of the stratospheric circulation results in increased stratosphere-to-troposphere transport. In the subtropics, downward advection into the troposphere is enhanced due to climate change. At higher latitudes, the ozone reservoir above the tropopause is enlarged due to the stronger circulation and ozone recovery.
Karin Kreher, Michel Van Roozendael, Francois Hendrick, Arnoud Apituley, Ermioni Dimitropoulou, Udo Frieß, Andreas Richter, Thomas Wagner, Johannes Lampel, Nader Abuhassan, Li Ang, Monica Anguas, Alkis Bais, Nuria Benavent, Tim Bösch, Kristof Bognar, Alexander Borovski, Ilya Bruchkouski, Alexander Cede, Ka Lok Chan, Sebastian Donner, Theano Drosoglou, Caroline Fayt, Henning Finkenzeller, David Garcia-Nieto, Clio Gielen, Laura Gómez-Martín, Nan Hao, Bas Henzing, Jay R. Herman, Christian Hermans, Syedul Hoque, Hitoshi Irie, Junli Jin, Paul Johnston, Junaid Khayyam Butt, Fahim Khokhar, Theodore K. Koenig, Jonas Kuhn, Vinod Kumar, Cheng Liu, Jianzhong Ma, Alexis Merlaud, Abhishek K. Mishra, Moritz Müller, Monica Navarro-Comas, Mareike Ostendorf, Andrea Pazmino, Enno Peters, Gaia Pinardi, Manuel Pinharanda, Ankie Piters, Ulrich Platt, Oleg Postylyakov, Cristina Prados-Roman, Olga Puentedura, Richard Querel, Alfonso Saiz-Lopez, Anja Schönhardt, Stefan F. Schreier, André Seyler, Vinayak Sinha, Elena Spinei, Kimberly Strong, Frederik Tack, Xin Tian, Martin Tiefengraber, Jan-Lukas Tirpitz, Jeroen van Gent, Rainer Volkamer, Mihalis Vrekoussis, Shanshan Wang, Zhuoru Wang, Mark Wenig, Folkard Wittrock, Pinhua H. Xie, Jin Xu, Margarita Yela, Chengxin Zhang, and Xiaoyi Zhao
Atmos. Meas. Tech., 13, 2169–2208, https://doi.org/10.5194/amt-13-2169-2020, https://doi.org/10.5194/amt-13-2169-2020, 2020
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In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants during an instrument intercomparison campaign (CINDI-2) at Cabauw, the Netherlands. Here we report on the outcome of this intercomparison exercise. The three major goals were to characterise the differences between the participating instruments, to define a robust methodology for performance assessment, and to contribute to the harmonisation of the measurement settings and retrieval methods.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Clara Orbe, David A. Plummer, Darryn W. Waugh, Huang Yang, Patrick Jöckel, Douglas E. Kinnison, Beatrice Josse, Virginie Marecal, Makoto Deushi, Nathan Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Wuhu Feng, and Slimane Bekki
Atmos. Chem. Phys., 20, 3809–3840, https://doi.org/10.5194/acp-20-3809-2020, https://doi.org/10.5194/acp-20-3809-2020, 2020
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Atmospheric composition is strongly influenced by global-scale winds that are not always properly simulated in computer models. A common approach to correct for this bias is to relax or
nudgeto the observed winds. Here we systematically evaluate how well this technique performs across a large suite of chemistry–climate models in terms of its ability to reproduce key aspects of both the tropospheric and stratospheric circulations.
Julie M. Nicely, Bryan N. Duncan, Thomas F. Hanisco, Glenn M. Wolfe, Ross J. Salawitch, Makoto Deushi, Amund S. Haslerud, Patrick Jöckel, Béatrice Josse, Douglas E. Kinnison, Andrew Klekociuk, Michael E. Manyin, Virginie Marécal, Olaf Morgenstern, Lee T. Murray, Gunnar Myhre, Luke D. Oman, Giovanni Pitari, Andrea Pozzer, Ilaria Quaglia, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Kane Stone, Susan Strahan, Simone Tilmes, Holger Tost, Daniel M. Westervelt, and Guang Zeng
Atmos. Chem. Phys., 20, 1341–1361, https://doi.org/10.5194/acp-20-1341-2020, https://doi.org/10.5194/acp-20-1341-2020, 2020
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Differences in methane lifetime among global models are large and poorly understood. We use a neural network method and simulations from the Chemistry Climate Model Initiative to quantify the factors influencing methane lifetime spread among models and variations over time. UV photolysis, tropospheric ozone, and nitrogen oxides drive large model differences, while the same factors plus specific humidity contribute to a decreasing trend in methane lifetime between 1980 and 2015.
Elizabeth Asher, Rebecca S. Hornbrook, Britton B. Stephens, Doug Kinnison, Eric J. Morgan, Ralph F. Keeling, Elliot L. Atlas, Sue M. Schauffler, Simone Tilmes, Eric A. Kort, Martin S. Hoecker-Martínez, Matt C. Long, Jean-François Lamarque, Alfonso Saiz-Lopez, Kathryn McKain, Colm Sweeney, Alan J. Hills, and Eric C. Apel
Atmos. Chem. Phys., 19, 14071–14090, https://doi.org/10.5194/acp-19-14071-2019, https://doi.org/10.5194/acp-19-14071-2019, 2019
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Halogenated organic trace gases, which are a source of reactive halogens to the atmosphere, exert a disproportionately large influence on atmospheric chemistry and climate. This paper reports novel aircraft observations of halogenated compounds over the Southern Ocean in summer and evaluates hypothesized regional sources and emissions of these trace gases through their relationships to additional aircraft observations.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Didier A. Hauglustaine, Sophie Szopa, Ann R. Stavert, Nathan Luke Abraham, Alex T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Béatrice Josse, Douglas Kinnison, Ole Kirner, Virginie Marécal, Fiona M. O'Connor, David A. Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 19, 13701–13723, https://doi.org/10.5194/acp-19-13701-2019, https://doi.org/10.5194/acp-19-13701-2019, 2019
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The role of hydroxyl radical changes in methane trends is debated, hindering our understanding of the methane cycle. This study quantifies how uncertainties in the hydroxyl radical may influence methane abundance in the atmosphere based on the inter-model comparison of hydroxyl radical fields and model simulations of CH4 abundance with different hydroxyl radical scenarios during 2000–2016. We show that hydroxyl radical changes could contribute up to 54 % of model-simulated methane biases.
Alexandra J. Boris, Satoshi Takahama, Andrew T. Weakley, Bruno M. Debus, Carley D. Fredrickson, Martin Esparza-Sanchez, Charlotte Burki, Matteo Reggente, Stephanie L. Shaw, Eric S. Edgerton, and Ann M. Dillner
Atmos. Meas. Tech., 12, 5391–5415, https://doi.org/10.5194/amt-12-5391-2019, https://doi.org/10.5194/amt-12-5391-2019, 2019
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Organic species are abundant in atmospheric particle-phase (aerosol) pollution and originate from a variety of biogenic and anthropogenic sources. Infrared spectrometry of filter-based atmospheric particle samples can afford a direct measurement of the particulate organic matter concentration and a characterization of its composition. This work discusses recent method improvements and compositions measured in samples from the SouthEastern Aerosol Research and Characterization (SEARCH) network.
Andreas Chrysanthou, Amanda C. Maycock, Martyn P. Chipperfield, Sandip Dhomse, Hella Garny, Douglas Kinnison, Hideharu Akiyoshi, Makoto Deushi, Rolando R. Garcia, Patrick Jöckel, Oliver Kirner, Giovanni Pitari, David A. Plummer, Laura Revell, Eugene Rozanov, Andrea Stenke, Taichu Y. Tanaka, Daniele Visioni, and Yousuke Yamashita
Atmos. Chem. Phys., 19, 11559–11586, https://doi.org/10.5194/acp-19-11559-2019, https://doi.org/10.5194/acp-19-11559-2019, 2019
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We perform the first multi-model comparison of the impact of nudged meteorology on the stratospheric residual circulation (RC) in chemistry–climate models. Nudging meteorology does not constrain the mean strength of RC compared to free-running simulations, and despite the lack of agreement in the mean circulation, nudging tightly constrains the inter-annual variability in the tropical upward mass flux in the lower stratosphere. In summary, nudging strongly affects the representation of RC.
Pablo Corral Arroyo, Raffael Aellig, Peter A. Alpert, Rainer Volkamer, and Markus Ammann
Atmos. Chem. Phys., 19, 10817–10828, https://doi.org/10.5194/acp-19-10817-2019, https://doi.org/10.5194/acp-19-10817-2019, 2019
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Oxidation of bromide and iodide is an important process in the troposphere that leads to gas-phase halogen compounds which impact the oxidation capacity of the atmosphere. Imidazole-2-carboxaldehyde (IC), an aromatic carbonyl, is a product of the multiphase chemistry of glyoxal (an oxidation product of isoprene), a major biogenic volatile organic compound. In this study we demonstrate that IC photochemistry leads to efficient oxidation of bromide and iodide and liberation of halogen compounds.
Kévin Lamy, Thierry Portafaix, Béatrice Josse, Colette Brogniez, Sophie Godin-Beekmann, Hassan Bencherif, Laura Revell, Hideharu Akiyoshi, Slimane Bekki, Michaela I. Hegglin, Patrick Jöckel, Oliver Kirner, Ben Liley, Virginie Marecal, Olaf Morgenstern, Andrea Stenke, Guang Zeng, N. Luke Abraham, Alexander T. Archibald, Neil Butchart, Martyn P. Chipperfield, Glauco Di Genova, Makoto Deushi, Sandip S. Dhomse, Rong-Ming Hu, Douglas Kinnison, Michael Kotkamp, Richard McKenzie, Martine Michou, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Eugene Rozanov, David Saint-Martin, Kengo Sudo, Taichu Y. Tanaka, Daniele Visioni, and Kohei Yoshida
Atmos. Chem. Phys., 19, 10087–10110, https://doi.org/10.5194/acp-19-10087-2019, https://doi.org/10.5194/acp-19-10087-2019, 2019
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In this study, we simulate the ultraviolet radiation evolution during the 21st century on Earth's surface using the output from several numerical models which participated in the Chemistry-Climate Model Initiative. We present four possible futures which depend on greenhouse gases emissions. The role of ozone-depleting substances, greenhouse gases and aerosols are investigated. Our results emphasize the important role of aerosols for future ultraviolet radiation in the Northern Hemisphere.
Ohad Harari, Chaim I. Garfinkel, Shlomi Ziskin Ziv, Olaf Morgenstern, Guang Zeng, Simone Tilmes, Douglas Kinnison, Makoto Deushi, Patrick Jöckel, Andrea Pozzer, Fiona M. O'Connor, and Sean Davis
Atmos. Chem. Phys., 19, 9253–9268, https://doi.org/10.5194/acp-19-9253-2019, https://doi.org/10.5194/acp-19-9253-2019, 2019
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Ozone depletion in the Antarctic has been shown to influence surface conditions, but the effects of ozone depletion in the Arctic on surface climate are unclear. We show that Arctic ozone does influence surface climate in both polar regions and tropical regions, though the proximate cause of these surface impacts is not yet clear.
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Huang Yang, Darryn W. Waugh, Clara Orbe, Guang Zeng, Olaf Morgenstern, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, David A. Plummer, Patrick Jöckel, Susan E. Strahan, Kane A. Stone, and Robyn Schofield
Atmos. Chem. Phys., 19, 5511–5528, https://doi.org/10.5194/acp-19-5511-2019, https://doi.org/10.5194/acp-19-5511-2019, 2019
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We evaluate the performance of a suite of models in simulating the large-scale transport from the northern midlatitudes to the Arctic using a CO-like idealized tracer. We find a large multi-model spread of the Arctic concentration of this CO-like tracer that is well correlated with the differences in the location of the midlatitude jet as well as the northern Hadley Cell edge. Our results suggest the Hadley Cell is key and zonal-mean transport by surface meridional flow needs better constraint.
Marianna Linz, Marta Abalos, Anne Sasha Glanville, Douglas E. Kinnison, Alison Ming, and Jessica L. Neu
Atmos. Chem. Phys., 19, 5069–5090, https://doi.org/10.5194/acp-19-5069-2019, https://doi.org/10.5194/acp-19-5069-2019, 2019
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The stratospheric circulation is important for transporting ozone and water vapor, and models of the stratosphere differ. The metrics used to compare models are inconsistent between studies and cannot be calculated from observational data. In this paper, we explore a metric for the circulation that can be calculated from observations and examine how it relates to the more commonly used metrics. We find substantial differences in the upper and lower stratosphere depending on the choice of metric.
Lucien Froidevaux, Douglas E. Kinnison, Ray Wang, John Anderson, and Ryan A. Fuller
Atmos. Chem. Phys., 19, 4783–4821, https://doi.org/10.5194/acp-19-4783-2019, https://doi.org/10.5194/acp-19-4783-2019, 2019
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This work evaluates two versions of a 3-D global model of upper-atmospheric composition for recent decades. The two versions differ mainly in their dynamical (wind) constraints. Model–data differences, variability, and trends in five gases (ozone, H2O, HCl, HNO3, and N2O) are compared. While the match between models and observations is impressive, a few areas of discrepancy are noted. This work also updates trends in composition based on recent satellite-based measurements (through 2018).
Alba Badia, Claire E. Reeves, Alex R. Baker, Alfonso Saiz-Lopez, Rainer Volkamer, Theodore K. Koenig, Eric C. Apel, Rebecca S. Hornbrook, Lucy J. Carpenter, Stephen J. Andrews, Tomás Sherwen, and Roland von Glasow
Atmos. Chem. Phys., 19, 3161–3189, https://doi.org/10.5194/acp-19-3161-2019, https://doi.org/10.5194/acp-19-3161-2019, 2019
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The oceans have an impact on the composition and reactivity of the troposphere through the emission of gases and particles. Thus, a quantitative understanding of the marine atmosphere is crucial to examine the oxidative capacity and climate forcing. This study investigates the impact of halogens in the tropical troposphere and explores the sensitivity of this to uncertainties in the fluxes and their chemical processing. Our modelled tropospheric Ox loss due to halogens ranges from 20 % to 60 %.
Shino Toma, Steve Bertman, Christopher Groff, Fulizi Xiong, Paul B. Shepson, Paul Romer, Kaitlin Duffey, Paul Wooldridge, Ronald Cohen, Karsten Baumann, Eric Edgerton, Abigail R. Koss, Joost de Gouw, Allen Goldstein, Weiwei Hu, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 1867–1880, https://doi.org/10.5194/acp-19-1867-2019, https://doi.org/10.5194/acp-19-1867-2019, 2019
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Acyl peroxy nitrates (APN) were measured near the ground in Alabama using GC in summer 2013 to study biosphere–atmosphere interactions. APN were lower than measured in the SE USA over the past 2 decades. Historical data showed APN in 2013 was limited by NOx and production was dominated by biogenic precursors more than in the past. Isoprene-derived MPAN correlated with isoprene hydroxynitrates as NOx-dependent products. MPAN varied with aerosol growth, but not with N-containing particles.
Roland Eichinger, Simone Dietmüller, Hella Garny, Petr Šácha, Thomas Birner, Harald Bönisch, Giovanni Pitari, Daniele Visioni, Andrea Stenke, Eugene Rozanov, Laura Revell, David A. Plummer, Patrick Jöckel, Luke Oman, Makoto Deushi, Douglas E. Kinnison, Rolando Garcia, Olaf Morgenstern, Guang Zeng, Kane Adam Stone, and Robyn Schofield
Atmos. Chem. Phys., 19, 921–940, https://doi.org/10.5194/acp-19-921-2019, https://doi.org/10.5194/acp-19-921-2019, 2019
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To shed more light upon the changes in stratospheric circulation in the 21st century, climate projection simulations of 10 state-of-the-art global climate models, spanning from 1960 to 2100, are analyzed. The study shows that in addition to changes in transport, mixing also plays an important role in stratospheric circulation and that the properties of mixing vary over time. Furthermore, the influence of mixing is quantified and a dynamical framework is provided to understand the changes.
Laura E. Revell, Andrea Stenke, Fiona Tummon, Aryeh Feinberg, Eugene Rozanov, Thomas Peter, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Neal Butchart, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, Robyn Schofield, Kane Stone, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 16155–16172, https://doi.org/10.5194/acp-18-16155-2018, https://doi.org/10.5194/acp-18-16155-2018, 2018
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Global models such as those participating in the Chemistry-Climate Model Initiative (CCMI) consistently simulate biases in tropospheric ozone compared with observations. We performed an advanced statistical analysis with one of the CCMI models to understand the cause of the bias. We found that emissions of ozone precursor gases are the dominant driver of the bias, implying either that the emissions are too large, or that the way in which the model handles emissions needs to be improved.
Jason A. Ducker, Christopher D. Holmes, Trevor F. Keenan, Silvano Fares, Allen H. Goldstein, Ivan Mammarella, J. William Munger, and Jordan Schnell
Biogeosciences, 15, 5395–5413, https://doi.org/10.5194/bg-15-5395-2018, https://doi.org/10.5194/bg-15-5395-2018, 2018
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We have developed an accurate method (SynFlux) to estimate ozone deposition and stomatal uptake across 103 flux tower sites (43 US, 60 Europe), where ozone concentrations and fluxes have not been measured. In all, the SynFlux public dataset provides monthly values of ozone dry deposition for 926 site years across a wide array of ecosystems. The SynFlux dataset will promote further applications to ecosystem, air quality, or climate modeling across the geoscience community.
Jens-Uwe Grooß, Rolf Müller, Reinhold Spang, Ines Tritscher, Tobias Wegner, Martyn P. Chipperfield, Wuhu Feng, Douglas E. Kinnison, and Sasha Madronich
Atmos. Chem. Phys., 18, 8647–8666, https://doi.org/10.5194/acp-18-8647-2018, https://doi.org/10.5194/acp-18-8647-2018, 2018
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We investigate a discrepancy between model simulations and observations of HCl in the dark polar stratosphere. In early winter, the less-well-studied period of the onset of chlorine activation, observations show a much faster depletion of HCl than simulations of three models. This points to some unknown process that is currently not represented in the models. Various hypotheses for potential causes are investigated that partly reduce the discrepancy. The impact on polar ozone depletion is low.
Sandip S. Dhomse, Douglas Kinnison, Martyn P. Chipperfield, Ross J. Salawitch, Irene Cionni, Michaela I. Hegglin, N. Luke Abraham, Hideharu Akiyoshi, Alex T. Archibald, Ewa M. Bednarz, Slimane Bekki, Peter Braesicke, Neal Butchart, Martin Dameris, Makoto Deushi, Stacey Frith, Steven C. Hardiman, Birgit Hassler, Larry W. Horowitz, Rong-Ming Hu, Patrick Jöckel, Beatrice Josse, Oliver Kirner, Stefanie Kremser, Ulrike Langematz, Jared Lewis, Marion Marchand, Meiyun Lin, Eva Mancini, Virginie Marécal, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Laura E. Revell, Eugene Rozanov, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 8409–8438, https://doi.org/10.5194/acp-18-8409-2018, https://doi.org/10.5194/acp-18-8409-2018, 2018
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We analyse simulations from the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion by anthropogenic chlorine and bromine. The simulations from 20 models project that global column ozone will return to 1980 values in 2047 (uncertainty range 2042–2052). Return dates in other regions vary depending on factors related to climate change and importance of chlorine and bromine. Column ozone in the tropics may continue to decline.
Stefan Lossow, Dale F. Hurst, Karen H. Rosenlof, Gabriele P. Stiller, Thomas von Clarmann, Sabine Brinkop, Martin Dameris, Patrick Jöckel, Doug E. Kinnison, Johannes Plieninger, David A. Plummer, Felix Ploeger, William G. Read, Ellis E. Remsberg, James M. Russell, and Mengchu Tao
Atmos. Chem. Phys., 18, 8331–8351, https://doi.org/10.5194/acp-18-8331-2018, https://doi.org/10.5194/acp-18-8331-2018, 2018
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Trend estimates of lower stratospheric H2O derived from the FPH observations at Boulder and a merged zonal mean satellite data set clearly differ for the time period from the late 1980s to 2010. We investigate if a sampling bias between Boulder and the zonal mean around the Boulder latitude can explain these trend discrepancies. Typically they are small and not sufficient to explain the trend discrepancies in the observational database.
Clara Orbe, Huang Yang, Darryn W. Waugh, Guang Zeng, Olaf Morgenstern, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, David A. Plummer, John F. Scinocca, Beatrice Josse, Virginie Marecal, Patrick Jöckel, Luke D. Oman, Susan E. Strahan, Makoto Deushi, Taichu Y. Tanaka, Kohei Yoshida, Hideharu Akiyoshi, Yousuke Yamashita, Andreas Stenke, Laura Revell, Timofei Sukhodolov, Eugene Rozanov, Giovanni Pitari, Daniele Visioni, Kane A. Stone, Robyn Schofield, and Antara Banerjee
Atmos. Chem. Phys., 18, 7217–7235, https://doi.org/10.5194/acp-18-7217-2018, https://doi.org/10.5194/acp-18-7217-2018, 2018
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In this study we compare a few atmospheric transport properties among several numerical models that are used to study the influence of atmospheric chemistry on climate. We show that there are large differences among models in terms of the timescales that connect the Northern Hemisphere midlatitudes, where greenhouse gases and ozone-depleting substances are emitted, to the Southern Hemisphere. Our results may have important implications for how models represent atmospheric composition.
Xi Chen, Mingjie Xie, Michael D. Hays, Eric Edgerton, Donna Schwede, and John T. Walker
Atmos. Chem. Phys., 18, 6829–6846, https://doi.org/10.5194/acp-18-6829-2018, https://doi.org/10.5194/acp-18-6829-2018, 2018
Simone Dietmüller, Roland Eichinger, Hella Garny, Thomas Birner, Harald Boenisch, Giovanni Pitari, Eva Mancini, Daniele Visioni, Andrea Stenke, Laura Revell, Eugene Rozanov, David A. Plummer, John Scinocca, Patrick Jöckel, Luke Oman, Makoto Deushi, Shibata Kiyotaka, Douglas E. Kinnison, Rolando Garcia, Olaf Morgenstern, Guang Zeng, Kane Adam Stone, and Robyn Schofield
Atmos. Chem. Phys., 18, 6699–6720, https://doi.org/10.5194/acp-18-6699-2018, https://doi.org/10.5194/acp-18-6699-2018, 2018
Martin G. Schultz, Scarlet Stadtler, Sabine Schröder, Domenico Taraborrelli, Bruno Franco, Jonathan Krefting, Alexandra Henrot, Sylvaine Ferrachat, Ulrike Lohmann, David Neubauer, Colombe Siegenthaler-Le Drian, Sebastian Wahl, Harri Kokkola, Thomas Kühn, Sebastian Rast, Hauke Schmidt, Philip Stier, Doug Kinnison, Geoffrey S. Tyndall, John J. Orlando, and Catherine Wespes
Geosci. Model Dev., 11, 1695–1723, https://doi.org/10.5194/gmd-11-1695-2018, https://doi.org/10.5194/gmd-11-1695-2018, 2018
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The chemistry–climate model ECHAM-HAMMOZ contains a detailed representation of tropospheric and stratospheric reactive chemistry and state-of-the-art parameterizations of aerosols. It thus allows for detailed investigations of chemical processes in the climate system. Evaluation of the model with various observational data yields good results, but the model has a tendency to produce too much OH in the tropics. This highlights the important interplay between atmospheric chemistry and dynamics.
Fernando Iglesias-Suarez, Douglas E. Kinnison, Alexandru Rap, Amanda C. Maycock, Oliver Wild, and Paul J. Young
Atmos. Chem. Phys., 18, 6121–6139, https://doi.org/10.5194/acp-18-6121-2018, https://doi.org/10.5194/acp-18-6121-2018, 2018
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This study explores future ozone radiative forcing (RF) and the relative contribution due to different drivers. Climate-induced ozone RF is largely the result of the interplay between lightning-produced ozone and enhanced ozone destruction in a warmer and wetter atmosphere. These results demonstrate the importance of stratospheric–tropospheric interactions and the stratosphere as a key region controlling a large fraction of the tropospheric ozone RF.
Caroline B. Alden, Subhomoy Ghosh, Sean Coburn, Colm Sweeney, Anna Karion, Robert Wright, Ian Coddington, Gregory B. Rieker, and Kuldeep Prasad
Atmos. Meas. Tech., 11, 1565–1582, https://doi.org/10.5194/amt-11-1565-2018, https://doi.org/10.5194/amt-11-1565-2018, 2018
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The location and sizing leaks of methane from natural gas operations poses a real challenge for greenhouse gas emission mitigation efforts and for accurate quantification of emissions inventories. We demonstrate, with synthetic and field tests, a new statistical method for the location and sizing of small trace gas point sources dispersed over large areas, based on measurements of ambient atmospheric conditions made with long-range, open-path laser-based atmospheric observations.
Paul S. Romer, Kaitlin C. Duffey, Paul J. Wooldridge, Eric Edgerton, Karsten Baumann, Philip A. Feiner, David O. Miller, William H. Brune, Abigail R. Koss, Joost A. de Gouw, Pawel K. Misztal, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 2601–2614, https://doi.org/10.5194/acp-18-2601-2018, https://doi.org/10.5194/acp-18-2601-2018, 2018
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Observations of increased ozone on hotter days are widely reported, but the mechanisms driving this relationship remain uncertain. We use measurements from the rural southeastern United States to study how temperature affects ozone production. We find that changing NOx emissions, most likely from soil microbes, can be a major driver of increased ozone with temperature in the continental background. These findings suggest that ozone will increase with temperature under a wide range of conditions.
Niall J. Ryan, Douglas E. Kinnison, Rolando R. Garcia, Christoph G. Hoffmann, Mathias Palm, Uwe Raffalski, and Justus Notholt
Atmos. Chem. Phys., 18, 1457–1474, https://doi.org/10.5194/acp-18-1457-2018, https://doi.org/10.5194/acp-18-1457-2018, 2018
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We used model output and instrument data to assess how well polar atmospheric descent rates can be derived using concentration measurements of long-lived gases in the atmosphere. The results indicate that the method incurs errors as large as the descent rates, and often leads to a misinterpretation of the direction of air motion. The rates derived using this method do not appear to represent the mean vertical wind in the middle atmosphere, and we suggest an alternate definition.
Olaf Morgenstern, Kane A. Stone, Robyn Schofield, Hideharu Akiyoshi, Yousuke Yamashita, Douglas E. Kinnison, Rolando R. Garcia, Kengo Sudo, David A. Plummer, John Scinocca, Luke D. Oman, Michael E. Manyin, Guang Zeng, Eugene Rozanov, Andrea Stenke, Laura E. Revell, Giovanni Pitari, Eva Mancini, Glauco Di Genova, Daniele Visioni, Sandip S. Dhomse, and Martyn P. Chipperfield
Atmos. Chem. Phys., 18, 1091–1114, https://doi.org/10.5194/acp-18-1091-2018, https://doi.org/10.5194/acp-18-1091-2018, 2018
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We assess how ozone as simulated by a group of chemistry–climate models responds to variations in man-made climate gases and ozone-depleting substances. We find some agreement, particularly in the middle and upper stratosphere, but also considerable disagreement elsewhere. Such disagreement affects the reliability of future ozone projections based on these models, and also constitutes a source of uncertainty in climate projections using prescribed ozone derived from these simulations.
Justin Bandoro, Susan Solomon, Benjamin D. Santer, Douglas E. Kinnison, and Michael J. Mills
Atmos. Chem. Phys., 18, 143–166, https://doi.org/10.5194/acp-18-143-2018, https://doi.org/10.5194/acp-18-143-2018, 2018
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We studied the attribution of stratospheric ozone changes and identified similarities between observations and human fingerprints from both emissions of ozone-depleting substances (ODSs) and greenhouse gases (GHGs). We developed an improvement on the traditional pattern correlation method that accounts for nonlinearities in the climate forcing time evolution. Use of the latter resulted in increased S / N ratios for the ODS fingerprint. The GHG fingerprint was not identifiable.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Yang Wang, Steffen Beirle, Francois Hendrick, Andreas Hilboll, Junli Jin, Aleksandra A. Kyuberis, Johannes Lampel, Ang Li, Yuhan Luo, Lorenzo Lodi, Jianzhong Ma, Monica Navarro, Ivan Ortega, Enno Peters, Oleg L. Polyansky, Julia Remmers, Andreas Richter, Olga Puentedura, Michel Van Roozendael, André Seyler, Jonathan Tennyson, Rainer Volkamer, Pinhua Xie, Nikolai F. Zobov, and Thomas Wagner
Atmos. Meas. Tech., 10, 3719–3742, https://doi.org/10.5194/amt-10-3719-2017, https://doi.org/10.5194/amt-10-3719-2017, 2017
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Slant column densities of nitrous acid (HONO) derived from different MAX-DOAS instruments and retrieval software are systematically compared for the first time during the Multi Axis DOAS – Comparison campaign for Aerosols and Trace gases (MAD-CAT) campaign held at MPIC in Mainz, Germany, from June to October 2013. Through the inter-comparisons and sensitivity studies we quantified the uncertainties in the DOAS fits of HONO from different sources and concluded a recommended setting.
Eleanor M. Waxman, Kevin C. Cossel, Gar-Wing Truong, Fabrizio R. Giorgetta, William C. Swann, Sean Coburn, Robert J. Wright, Gregory B. Rieker, Ian Coddington, and Nathan R. Newbury
Atmos. Meas. Tech., 10, 3295–3311, https://doi.org/10.5194/amt-10-3295-2017, https://doi.org/10.5194/amt-10-3295-2017, 2017
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In this paper, we compare greenhouse gas measurements from two novel open-path instruments to determine how similarly they measure the same gas concentration. We do this over an outdoor path, so the two instruments measured the same outdoor air. We found that the two instruments agree extremely well, so in the future if the instruments were at two different locations we could reliably compare their measurements to determine differences between the two places.
Maria A. Navarro, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Elliot Atlas, Xavier Rodriguez-Lloveras, Douglas Kinnison, Jean-Francois Lamarque, Simone Tilmes, Troy Thornberry, Andrew Rollins, James W. Elkins, Eric J. Hintsa, and Fred L. Moore
Atmos. Chem. Phys., 17, 9917–9930, https://doi.org/10.5194/acp-17-9917-2017, https://doi.org/10.5194/acp-17-9917-2017, 2017
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Inorganic bromine (Bry) plays an important role in ozone layer depletion. Based on aircraft observations of organic bromine species and chemistry simulations, we model the Bry abundances over the Pacific tropical tropopause. Our results show BrO and Br as the dominant species during daytime hours, and BrCl and BrONO2 as the nighttime dominant species over the western and eastern Pacific, respectively. The difference in the partitioning is due to changes in the abundance of O3, NO2, and Cly.
Enno Peters, Gaia Pinardi, André Seyler, Andreas Richter, Folkard Wittrock, Tim Bösch, Michel Van Roozendael, François Hendrick, Theano Drosoglou, Alkiviadis F. Bais, Yugo Kanaya, Xiaoyi Zhao, Kimberly Strong, Johannes Lampel, Rainer Volkamer, Theodore Koenig, Ivan Ortega, Olga Puentedura, Mónica Navarro-Comas, Laura Gómez, Margarita Yela González, Ankie Piters, Julia Remmers, Yang Wang, Thomas Wagner, Shanshan Wang, Alfonso Saiz-Lopez, David García-Nieto, Carlos A. Cuevas, Nuria Benavent, Richard Querel, Paul Johnston, Oleg Postylyakov, Alexander Borovski, Alexander Elokhov, Ilya Bruchkouski, Haoran Liu, Cheng Liu, Qianqian Hong, Claudia Rivera, Michel Grutter, Wolfgang Stremme, M. Fahim Khokhar, Junaid Khayyam, and John P. Burrows
Atmos. Meas. Tech., 10, 955–978, https://doi.org/10.5194/amt-10-955-2017, https://doi.org/10.5194/amt-10-955-2017, 2017
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This work is about harmonization of differential optical absorption spectroscopy retrieval codes, which is a remote sensing technique widely used to derive atmospheric trace gas amounts. The study is based on ground-based measurements performed during the Multi-Axis DOAS Comparison campaign for Aerosols and Trace gases (MAD-CAT) in Mainz, Germany, in summer 2013. In total, 17 international groups working in the field of the DOAS technique participated in this study.
Olaf Morgenstern, Michaela I. Hegglin, Eugene Rozanov, Fiona M. O'Connor, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Neal Butchart, Martyn P. Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando R. Garcia, Steven C. Hardiman, Larry W. Horowitz, Patrick Jöckel, Beatrice Josse, Douglas Kinnison, Meiyun Lin, Eva Mancini, Michael E. Manyin, Marion Marchand, Virginie Marécal, Martine Michou, Luke D. Oman, Giovanni Pitari, David A. Plummer, Laura E. Revell, David Saint-Martin, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Yousuke Yamashita, Kohei Yoshida, and Guang Zeng
Geosci. Model Dev., 10, 639–671, https://doi.org/10.5194/gmd-10-639-2017, https://doi.org/10.5194/gmd-10-639-2017, 2017
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We present a review of the make-up of 20 models participating in the Chemistry–Climate Model Initiative (CCMI). In comparison to earlier such activities, most of these models comprise a whole-atmosphere chemistry, and several of them include an interactive ocean module. This makes them suitable for studying the interactions of tropospheric air quality, stratospheric ozone, and climate. The paper lays the foundation for other studies using the CCMI simulations for scientific analysis.
Jiaoyan Huang, Matthieu B. Miller, Eric Edgerton, and Mae Sexauer Gustin
Atmos. Chem. Phys., 17, 1689–1698, https://doi.org/10.5194/acp-17-1689-2017, https://doi.org/10.5194/acp-17-1689-2017, 2017
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The highest mercury (Hg) wet deposition in USA occurs along the Gulf of Mexico. Gaseous oxidized Hg (GOM) is a major contributor due to high water solubility and reactivity. Concentration and dry deposition of GOM were determined for OLF, Florida. Results indicated at least 5 GOM compounds in this area including HgBr2, HgO, and Hg–nitrogen and –sulfur forms. GOM chemistry indicates reactions with local mobile source pollutants and long-range transport from outside of the USA.
Rafael P. Fernandez, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 17, 1673–1688, https://doi.org/10.5194/acp-17-1673-2017, https://doi.org/10.5194/acp-17-1673-2017, 2017
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The inclusion of biogenic very-short lived bromine (VSLBr) in a chemistry-climate model produces an expansion of the ozone hole area of ~ 5 million km2, which is equivalent in magnitude to the recently estimated Antarctic ozone healing due to the reduction of anthropogenic CFCs and halons. The maximum Antarctic ozone hole depletion increases by up to 14 % when natural VSLBr are considered, but does not introduce a significant delay of the modelled ozone return date to 1980 October levels.
Natalie Kille, Sunil Baidar, Philip Handley, Ivan Ortega, Roman Sinreich, Owen R. Cooper, Frank Hase, James W. Hannigan, Gabriele Pfister, and Rainer Volkamer
Atmos. Meas. Tech., 10, 373–392, https://doi.org/10.5194/amt-10-373-2017, https://doi.org/10.5194/amt-10-373-2017, 2017
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This article describes a new instrument for measuring and quantifying emission fluxes. It introduces the instrument using the solar occultation flux method. Results are presented from the FRAPPE field campaign near Denver, Colorado, from 2014. Calculations of emissions of sources are presented from FRAPPE and compared to emission inventories. Finally, structure functions are calculated to facilitate the future comparison of high-resolution measurements with low resolution satellite measurements.
Martyn P. Chipperfield, Qing Liang, Matthew Rigby, Ryan Hossaini, Stephen A. Montzka, Sandip Dhomse, Wuhu Feng, Ronald G. Prinn, Ray F. Weiss, Christina M. Harth, Peter K. Salameh, Jens Mühle, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Paul B. Krummel, Paul J. Fraser, L. Paul Steele, James D. Happell, Robert C. Rhew, James Butler, Shari A. Yvon-Lewis, Bradley Hall, David Nance, Fred Moore, Ben R. Miller, James W. Elkins, Jeremy J. Harrison, Chris D. Boone, Elliot L. Atlas, and Emmanuel Mahieu
Atmos. Chem. Phys., 16, 15741–15754, https://doi.org/10.5194/acp-16-15741-2016, https://doi.org/10.5194/acp-16-15741-2016, 2016
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Carbon tetrachloride (CCl4) is a compound which, when released into the atmosphere, can cause depletion of the stratospheric ozone layer. Its emissions are controlled under the Montreal Protocol, and its atmospheric abundance is slowly decreasing. However, this decrease is not as fast as expected based on estimates of its emissions and its atmospheric lifetime. We have used an atmospheric model to look at the uncertainties in the CCl4 lifetime and to examine the impact on its atmospheric decay.
Alfonso Saiz-Lopez, John M. C. Plane, Carlos A. Cuevas, Anoop S. Mahajan, Jean-François Lamarque, and Douglas E. Kinnison
Atmos. Chem. Phys., 16, 15593–15604, https://doi.org/10.5194/acp-16-15593-2016, https://doi.org/10.5194/acp-16-15593-2016, 2016
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Electronic structure calculations are used to survey possible reactions that HOI and I2 could undergo at night in the lower troposphere, and hence reconcile measurements and models. The reactions NO3 + HOI and I2 + NO3 are included in two models to explore a new nocturnal iodine radical activation mechanism, leading to a reduction of nighttime HOI and I2. This chemistry can have a large impact on NO3 levels in the MBL, and hence upon the nocturnal oxidizing capacity of the marine atmosphere.
Barbara Dix, Theodore K. Koenig, and Rainer Volkamer
Atmos. Meas. Tech., 9, 5655–5675, https://doi.org/10.5194/amt-9-5655-2016, https://doi.org/10.5194/amt-9-5655-2016, 2016
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We present a parameterization method for the conversion of measured trace gas slant column densities into volume mixing ratios along a flight track. Benefits of this method are that it is computationally fast and almost no information on local atmospheric conditions is needed. Application to simulated data and field data show that the method is accurate within 10–15 % and valid for a wide range of atmospheric conditions. Our method can easily be transferred to other trace gases.
Michael Höpfner, Rainer Volkamer, Udo Grabowski, Michel Grutter, Johannes Orphal, Gabriele Stiller, Thomas von Clarmann, and Gerald Wetzel
Atmos. Chem. Phys., 16, 14357–14369, https://doi.org/10.5194/acp-16-14357-2016, https://doi.org/10.5194/acp-16-14357-2016, 2016
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Ammonia (NH3) in the atmosphere is important because of its influence on aerosol and cloud formation and its increasing anthropogenic emissions. We report the first detection of NH3 in the upper troposphere by the analysis of infrared limb emission spectra measured by the MIPAS instrument on Envisat. We have found enhanced values of NH3 within the Asian summer monsoon upper troposphere, where it might contribute to the composition of the Asian tropopause aerosol layer.
Tomás Sherwen, Johan A. Schmidt, Mat J. Evans, Lucy J. Carpenter, Katja Großmann, Sebastian D. Eastham, Daniel J. Jacob, Barbara Dix, Theodore K. Koenig, Roman Sinreich, Ivan Ortega, Rainer Volkamer, Alfonso Saiz-Lopez, Cristina Prados-Roman, Anoop S. Mahajan, and Carlos Ordóñez
Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, https://doi.org/10.5194/acp-16-12239-2016, 2016
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We present a simulation of tropospheric Cl, Br, I chemistry within the GEOS-Chem CTM. We find a decrease in tropospheric ozone burden of 18.6 % and a 8.2 % decrease in global mean OH concentrations. Cl oxidation of some VOCs range from 15 to 27 % of the total loss. Bromine plays a small role in oxidising oVOCs. Surface ozone, ozone sondes, and methane lifetime are in general improved by the inclusion of halogens. We argue that simulated bromine and chlorine represent a lower limit.
Laura González Palacios, Pablo Corral Arroyo, Kifle Z. Aregahegn, Sarah S. Steimer, Thorsten Bartels-Rausch, Barbara Nozière, Christian George, Markus Ammann, and Rainer Volkamer
Atmos. Chem. Phys., 16, 11823–11836, https://doi.org/10.5194/acp-16-11823-2016, https://doi.org/10.5194/acp-16-11823-2016, 2016
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The sources of radicals at aerosol surfaces are highly uncertain. Here we investigate the HO2 radical production from the UV irradiation of imidazole-2-carboxaldehyde (IC) in bulk aqueous films containing IC and citric acid, as well as IC in ammonium sulfate aerosols. We find that IC is an efficient photosensitizer that forms HO2 radicals from H-donor chemistry. IC is a proxy species for brown carbon in atmospheric aerosols.
Ivan Ortega, Sean Coburn, Larry K. Berg, Kathy Lantz, Joseph Michalsky, Richard A. Ferrare, Johnathan W. Hair, Chris A. Hostetler, and Rainer Volkamer
Atmos. Meas. Tech., 9, 3893–3910, https://doi.org/10.5194/amt-9-3893-2016, https://doi.org/10.5194/amt-9-3893-2016, 2016
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We present an inherently calibrated retrieval to measure aerosol optical depth (AOD) and the aerosol phase function parameter, g, based on measurements of azimuth distributions of the Raman scattering probability (RSP), the near-absolute rotational Raman scattering (RRS) intensity by the University of Colorado two-dimensional (2-D) MAX-DOAS. The retrievals are maximally sensitive at low AOD and do not require absolute radiance calibration. We compare results with data from independent sensors.
J. Kaiser, K. M. Skog, K. Baumann, S. B. Bertman, S. B. Brown, W. H. Brune, J. D. Crounse, J. A. de Gouw, E. S. Edgerton, P. A. Feiner, A. H. Goldstein, A. Koss, P. K. Misztal, T. B. Nguyen, K. F. Olson, J. M. St. Clair, A. P. Teng, S. Toma, P. O. Wennberg, R. J. Wild, L. Zhang, and F. N. Keutsch
Atmos. Chem. Phys., 16, 9349–9359, https://doi.org/10.5194/acp-16-9349-2016, https://doi.org/10.5194/acp-16-9349-2016, 2016
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OH reactivity can be used to assess the amount of reactive carbon in an air mass. “Missing” reactivity is commonly found in forested environments and is attributed to either direct emissions of unmeasured volatile organic compounds or to unmeasured/underpredicted oxidation products. Using a box model and measurements from the 2013 SOAS campaign, we find only small discrepancies in measured and calculated reactivity. Our results suggest the discrepancies stem from unmeasured direct emissions.
Luping Su, Edward G. Patton, Jordi Vilà-Guerau de Arellano, Alex B. Guenther, Lisa Kaser, Bin Yuan, Fulizi Xiong, Paul B. Shepson, Li Zhang, David O. Miller, William H. Brune, Karsten Baumann, Eric Edgerton, Andrew Weinheimer, Pawel K. Misztal, Jeong-Hoo Park, Allen H. Goldstein, Kate M. Skog, Frank N. Keutsch, and John E. Mak
Atmos. Chem. Phys., 16, 7725–7741, https://doi.org/10.5194/acp-16-7725-2016, https://doi.org/10.5194/acp-16-7725-2016, 2016
Yuzo Miyazaki, Sean Coburn, Kaori Ono, David T. Ho, R. Bradley Pierce, Kimitaka Kawamura, and Rainer Volkamer
Atmos. Chem. Phys., 16, 7695–7707, https://doi.org/10.5194/acp-16-7695-2016, https://doi.org/10.5194/acp-16-7695-2016, 2016
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We conducted a WSOC-specific 13C analysis of submicron marine aerosols over the eastern equatorial Pacific for the first time. The analysis of 13C combined with monosaccharides provides evidence of a significant contribution of marine dissolved organic carbon (DOC) to submicron particles in the MBL regardless of the oceanic area. The study demonstrates that DOC is closely correlated with the submicron WSOC and implies that it may characterize background OA in the MBL over the study region.
Simone Tilmes, Jean-Francois Lamarque, Louisa K. Emmons, Doug E. Kinnison, Dan Marsh, Rolando R. Garcia, Anne K. Smith, Ryan R. Neely, Andrew Conley, Francis Vitt, Maria Val Martin, Hiroshi Tanimoto, Isobel Simpson, Don R. Blake, and Nicola Blake
Geosci. Model Dev., 9, 1853–1890, https://doi.org/10.5194/gmd-9-1853-2016, https://doi.org/10.5194/gmd-9-1853-2016, 2016
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The state of the art Community Earth System Model, CESM1 CAM4-chem has been used to perform reference and sensitivity simulations as part of the Chemistry Climate Model Initiative (CCMI). Specifics of the model and details regarding the setup of the simulations are described. In additions, the main behavior of the model, including selected chemical species have been evaluated with climatological datasets. This paper is therefore a references for studies that use the provided model results.
Charles H. Jackman, Daniel R. Marsh, Douglas E. Kinnison, Christopher J. Mertens, and Eric L. Fleming
Atmos. Chem. Phys., 16, 5853–5866, https://doi.org/10.5194/acp-16-5853-2016, https://doi.org/10.5194/acp-16-5853-2016, 2016
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Two global models were used to investigate the impact of galactic cosmic ray (GCRs) on the atmosphere over the 1960-2010 time period. The primary impact of the naturally occurring GCRs on ozone was found to be due to their production of NOx and this impact varies with the atmospheric chlorine loading, sulfate aerosol loading, and solar cycle variation. GCR-caused decreases of annual average global total ozone were computed to be 0.2 % or less.
Sri Hapsari Budisulistiorini, Karsten Baumann, Eric S. Edgerton, Solomon T. Bairai, Stephen Mueller, Stephanie L. Shaw, Eladio M. Knipping, Avram Gold, and Jason D. Surratt
Atmos. Chem. Phys., 16, 5171–5189, https://doi.org/10.5194/acp-16-5171-2016, https://doi.org/10.5194/acp-16-5171-2016, 2016
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A year-long near-real-time characterization of non-refractory submicron aerosol (NR-PM1) was conducted at an urban (Atlanta, Georgia, in 2012) and rural (Look Rock, Tennessee, in 2013) site in the southeastern US using the Aerodyne Aerosol Chemical Speciation Monitor, collocated with established air-monitoring network measurements, to identify sources of organic aerosol (OA). Further, high-volume filter samples were collected for measurements of OA tracers by offline mass spectrometry tools.
Weruka Rattanavaraha, Kevin Chu, Sri Hapsari Budisulistiorini, Matthieu Riva, Ying-Hsuan Lin, Eric S. Edgerton, Karsten Baumann, Stephanie L. Shaw, Hongyu Guo, Laura King, Rodney J. Weber, Miranda E. Neff, Elizabeth A. Stone, John H. Offenberg, Zhenfa Zhang, Avram Gold, and Jason D. Surratt
Atmos. Chem. Phys., 16, 4897–4914, https://doi.org/10.5194/acp-16-4897-2016, https://doi.org/10.5194/acp-16-4897-2016, 2016
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The mechanisms by which specific anthropogenic pollutants enhance isoprene SOA in ambient PM2.5 remain unclear. As one aspect of an investigation to examine how anthropogenic pollutants influence isoprene-derived SOA formation, high-volume PM2.5 filter samples were collected from Birmingham, AL, during the 2013 Southern Oxidant and Aerosol Study (SOAS). Isoprene SOA tracers were measured from these samples and compared to gas and aerosol data collected from the SEARCH network.
Sunil Baidar, Natalie Kille, Ivan Ortega, Roman Sinreich, David Thomson, James Hannigan, and Rainer Volkamer
Atmos. Meas. Tech., 9, 963–972, https://doi.org/10.5194/amt-9-963-2016, https://doi.org/10.5194/amt-9-963-2016, 2016
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We present development of a digital mobile solar tracker which can be coupled simultaneously to UV–Vis and FTIR spectrometers to measure trace gases in the atmosphere. We demonstrate an angular precision of 0.052º (about 1/10 of the solar disk diameter) during research drives and verify this tracking precision from measurements of the center to limb darkening (CLD, the changing appearance of Fraunhofer lines) in the mobile direct sun DOAS spectra.
C. R. Hoyle, C. Fuchs, E. Järvinen, H. Saathoff, A. Dias, I. El Haddad, M. Gysel, S. C. Coburn, J. Tröstl, A.-K. Bernhammer, F. Bianchi, M. Breitenlechner, J. C. Corbin, J. Craven, N. M. Donahue, J. Duplissy, S. Ehrhart, C. Frege, H. Gordon, N. Höppel, M. Heinritzi, T. B. Kristensen, U. Molteni, L. Nichman, T. Pinterich, A. S. H. Prévôt, M. Simon, J. G. Slowik, G. Steiner, A. Tomé, A. L. Vogel, R. Volkamer, A. C. Wagner, R. Wagner, A. S. Wexler, C. Williamson, P. M. Winkler, C. Yan, A. Amorim, J. Dommen, J. Curtius, M. W. Gallagher, R. C. Flagan, A. Hansel, J. Kirkby, M. Kulmala, O. Möhler, F. Stratmann, D. R. Worsnop, and U. Baltensperger
Atmos. Chem. Phys., 16, 1693–1712, https://doi.org/10.5194/acp-16-1693-2016, https://doi.org/10.5194/acp-16-1693-2016, 2016
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A significant portion of sulphate, an important constituent of atmospheric aerosols, is formed via the aqueous phase oxidation of sulphur dioxide by ozone. The rate of this reaction has previously only been measured over a relatively small temperature range. Here, we use the state of the art CLOUD chamber at CERN to perform the first measurements of this reaction rate in super-cooled droplets, confirming that the existing extrapolation of the reaction rate to sub-zero temperatures is accurate.
T. Sherwen, M. J. Evans, L. J. Carpenter, S. J. Andrews, R. T. Lidster, B. Dix, T. K. Koenig, R. Sinreich, I. Ortega, R. Volkamer, A. Saiz-Lopez, C. Prados-Roman, A. S. Mahajan, and C. Ordóñez
Atmos. Chem. Phys., 16, 1161–1186, https://doi.org/10.5194/acp-16-1161-2016, https://doi.org/10.5194/acp-16-1161-2016, 2016
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Using a global chemical transport model (GEOS-Chem) with additional iodine emissions, chemistry, and deposition we show that iodine is responsible for ~ 9 % of global ozone loss but has negligible impacts on global OH. Uncertainties are large in the chemistry and emissions and future research is needed in both. Measurements of iodine species (especially HOI) would be useful. We believe iodine chemistry should be considered in future chemistry-climate and in air quality modelling.
C. L. Blanchard, G. M. Hidy, S. Shaw, K. Baumann, and E. S. Edgerton
Atmos. Chem. Phys., 16, 215–238, https://doi.org/10.5194/acp-16-215-2016, https://doi.org/10.5194/acp-16-215-2016, 2016
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Fifteen years of gas and particle measurements at eight monitoring sites comprising the Southeastern Aerosol Research and Characterization (SEARCH) network offer insights into the sources of organic aerosol in the southeastern United States. Between 1999 and 2013, mean organic aerosol concentrations declined due to decreasing particle emissions from motor vehicles and to less secondary organic aerosol with declining emissions of sulfur dioxide, nitrogen oxides, and volatile organic compounds.
B. R. Ayres, H. M. Allen, D. C. Draper, S. S. Brown, R. J. Wild, J. L. Jimenez, D. A. Day, P. Campuzano-Jost, W. Hu, J. de Gouw, A. Koss, R. C. Cohen, K. C. Duffey, P. Romer, K. Baumann, E. Edgerton, S. Takahama, J. A. Thornton, B. H. Lee, F. D. Lopez-Hilfiker, C. Mohr, P. O. Wennberg, T. B. Nguyen, A. Teng, A. H. Goldstein, K. Olson, and J. L. Fry
Atmos. Chem. Phys., 15, 13377–13392, https://doi.org/10.5194/acp-15-13377-2015, https://doi.org/10.5194/acp-15-13377-2015, 2015
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This paper reports atmospheric gas- and aerosol-phase field measurements from the southeastern United States in summer 2013 to demonstrate that the oxidation of biogenic volatile organic compounds by nitrate radical produces a substantial amount of secondary organic aerosol in this region. This process, driven largely by monoterpenes, results in a comparable aerosol nitrate production rate to inorganic nitrate formation by heterogeneous uptake of HNO3 onto dust particles.
F. Xiong, K. M. McAvey, K. A. Pratt, C. J. Groff, M. A. Hostetler, M. A. Lipton, T. K. Starn, J. V. Seeley, S. B. Bertman, A. P. Teng, J. D. Crounse, T. B. Nguyen, P. O. Wennberg, P. K. Misztal, A. H. Goldstein, A. B. Guenther, A. R. Koss, K. F. Olson, J. A. de Gouw, K. Baumann, E. S. Edgerton, P. A. Feiner, L. Zhang, D. O. Miller, W. H. Brune, and P. B. Shepson
Atmos. Chem. Phys., 15, 11257–11272, https://doi.org/10.5194/acp-15-11257-2015, https://doi.org/10.5194/acp-15-11257-2015, 2015
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Hydroxynitrates from isoprene oxidation were quantified both in the laboratory and through field studies. The yield of hydroxynitrates 9(+4/-3)% derived from chamber experiments was applied in a zero-dimensional model to simulate the production and loss of isoprene hydroxynitrates in an ambient environment during the 2013 Southern Oxidant and Aerosol Study (SOAS). NOx was determined to be the limiting factor for the formation of isoprene hydroxynitrates during SOAS.
M. Gil-Ojeda, M. Navarro-Comas, L. Gómez-Martín, J. A. Adame, A. Saiz-Lopez, C. A. Cuevas, Y. González, O. Puentedura, E. Cuevas, J.-F. Lamarque, D. Kinninson, and S. Tilmes
Atmos. Chem. Phys., 15, 10567–10579, https://doi.org/10.5194/acp-15-10567-2015, https://doi.org/10.5194/acp-15-10567-2015, 2015
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The NO2 seasonal evolution in the free troposphere (FT) has been established for the first time, based on a remote sensing technique (MAXDOAS) and thus avoiding the problems of the local pollution of in situ instruments. A clear seasonality has been found, with background levels of 20-40pptv. Evidence has been found on fast, direct injection of surface air into the free troposphere. This result might have implications on the FT distribution of halogens and other species with marine sources.
H. M. Allen, D. C. Draper, B. R. Ayres, A. Ault, A. Bondy, S. Takahama, R. L. Modini, K. Baumann, E. Edgerton, C. Knote, A. Laskin, B. Wang, and J. L. Fry
Atmos. Chem. Phys., 15, 10669–10685, https://doi.org/10.5194/acp-15-10669-2015, https://doi.org/10.5194/acp-15-10669-2015, 2015
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We report ion chromatographic measurements of gas- and aerosol-phase inorganic species at the SOAS 2013 field study. Our particular focus is on inorganic nitrate aerosol formation via HNO3 uptake onto coarse-mode dust and sea salt particles, which we find to be the dominant source of episodic inorganic nitrate at this site, due to the high acidity of the particles preventing formation of NH4NO3. We calculate a production rate of inorganic nitrate aerosol.
I. Ortega, T. Koenig, R. Sinreich, D. Thomson, and R. Volkamer
Atmos. Meas. Tech., 8, 2371–2395, https://doi.org/10.5194/amt-8-2371-2015, https://doi.org/10.5194/amt-8-2371-2015, 2015
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We describe the University of Colorado 2-D-MAX-DOAS instrument and a retrieval to measure 3-D distributions of NO2. The spatial scale over which NO2 is probed is systematically varied by measuring NO2 at three different wavelengths. This has a significant effect on the comparison with the NO2 VCD as measured by OMI. The challenges and opportunities to validate satellites under inhomogeneous conditions as well as to pinpoint hydrocarbon chemistry around the measurement site are discussed.
R. Volkamer, S. Baidar, T. L. Campos, S. Coburn, J. P. DiGangi, B. Dix, E. W. Eloranta, T. K. Koenig, B. Morley, I. Ortega, B. R. Pierce, M. Reeves, R. Sinreich, S. Wang, M. A. Zondlo, and P. A. Romashkin
Atmos. Meas. Tech., 8, 2121–2148, https://doi.org/10.5194/amt-8-2121-2015, https://doi.org/10.5194/amt-8-2121-2015, 2015
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Tropospheric halogens and small oxygenated VOC (OVOC) modify tropospheric HOx and NOx, O3 and aerosols. We have measured bromine monoxide (BrO), iodine monoxide (IO), glyoxal (CHOCHO) profiles from research aircraft in the tropical troposphere and compare with ship- and aircraft-based in situ sensors. Our measurements point to the need to improve the representation of halogens and organic carbon sources in atmospheric models.
S. Tilmes, J.-F. Lamarque, L. K. Emmons, D. E. Kinnison, P.-L. Ma, X. Liu, S. Ghan, C. Bardeen, S. Arnold, M. Deeter, F. Vitt, T. Ryerson, J. W. Elkins, F. Moore, J. R. Spackman, and M. Val Martin
Geosci. Model Dev., 8, 1395–1426, https://doi.org/10.5194/gmd-8-1395-2015, https://doi.org/10.5194/gmd-8-1395-2015, 2015
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The Community Atmosphere Model (CAM), version 5, is now coupled to extensive tropospheric and stratospheric chemistry, called CAM5-chem, and is available in addition to CAM4-chem in the Community Earth System Model (CESM) version 1.2. Both configurations are well suited as tools for atmospheric chemistry modeling studies in the troposphere and lower stratosphere.
R. Thalman, M. T. Baeza-Romero, S. M. Ball, E. Borrás, M. J. S. Daniels, I. C. A. Goodall, S. B. Henry, T. Karl, F. N. Keutsch, S. Kim, J. Mak, P. S. Monks, A. Muñoz, J. Orlando, S. Peppe, A. R. Rickard, M. Ródenas, P. Sánchez, R. Seco, L. Su, G. Tyndall, M. Vázquez, T. Vera, E. Waxman, and R. Volkamer
Atmos. Meas. Tech., 8, 1835–1862, https://doi.org/10.5194/amt-8-1835-2015, https://doi.org/10.5194/amt-8-1835-2015, 2015
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Measurements of α-dicarbonyl compounds, like glyoxal (CHOCHO) and methyl glyoxal (CH3C(O)CHO), are informative about the rate of hydrocarbon oxidation, oxidative capacity, and secondary organic aerosol (SOA) formation in the atmosphere. We have compared nine instruments and seven techniques to measure α-dicarbonyl, using simulation chamber facilities in the US and Europe. We assess our understanding of calibration, precision, accuracy and detection limits, as well as possible sampling biases.
J. Huang, M. B. Miller, E. Edgerton, and M. S. Gustin
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-12069-2015, https://doi.org/10.5194/acpd-15-12069-2015, 2015
Revised manuscript not accepted
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Gaseous oxidized Hg (GOM) is a major contributor to Hg in wet and dry deposition. Recent work has indicated that the concentrations of GOM as measured are too low by 3-to-12 times; and that compounds vary across space and time. Data collected in Florida indicate five potential GOM compounds, including HgBr2, HgO, Hg(NO3)2, HgSO4, and an unknown compound. Sources include local combustion (cars and power plants), the marine boundary layer, and long range transport from Asia.
L. Millán, S. Wang, N. Livesey, D. Kinnison, H. Sagawa, and Y. Kasai
Atmos. Chem. Phys., 15, 2889–2902, https://doi.org/10.5194/acp-15-2889-2015, https://doi.org/10.5194/acp-15-2889-2015, 2015
P. Hess, D. Kinnison, and Q. Tang
Atmos. Chem. Phys., 15, 2341–2365, https://doi.org/10.5194/acp-15-2341-2015, https://doi.org/10.5194/acp-15-2341-2015, 2015
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Using a series of model simulations, we find that at widespread NH extratropical locations, interannual tropospheric ozone variability is largely determined by the transport of ozone from the stratosphere. This has implications in the interpretation of measured tropospheric ozone variability in light of changes in the emissions of ozone precursors and in the response of tropospheric ozone to climate change.
C. Prados-Roman, C. A. Cuevas, R. P. Fernandez, D. E. Kinnison, J-F. Lamarque, and A. Saiz-Lopez
Atmos. Chem. Phys., 15, 2215–2224, https://doi.org/10.5194/acp-15-2215-2015, https://doi.org/10.5194/acp-15-2215-2015, 2015
E. Spinei, A. Cede, J. Herman, G. H. Mount, E. Eloranta, B. Morley, S. Baidar, B. Dix, I. Ortega, T. Koenig, and R. Volkamer
Atmos. Meas. Tech., 8, 793–809, https://doi.org/10.5194/amt-8-793-2015, https://doi.org/10.5194/amt-8-793-2015, 2015
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This paper presents ground-based direct-sun and airborne multi-axis DOAS measurements of O2O2 absorption optical depths under atmospheric conditions in two wavelength regions (335-–390nm and 435--490nm). Our results show that laboratory-measured σ(O2O2) is applicable for observations over a wide range of atmospheric conditions. Temperature dependence of σ(O2O2) is about 9±2.5% from 231K to 275K.
T. Fang, V. Verma, H. Guo, L. E. King, E. S. Edgerton, and R. J. Weber
Atmos. Meas. Tech., 8, 471–482, https://doi.org/10.5194/amt-8-471-2015, https://doi.org/10.5194/amt-8-471-2015, 2015
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This work summarizes a newly developed semi-automated system for quantifying the oxidative potential of aerosol aqueous extracts using the dithiothreitol (DTT) assay. 500 sample analyses indicate that DTT activity in the southeast US is likely not dominated by a unique local source, and sources change with season. The unique large data set generated with the technique described in this paper allows new studies on DTT sources and investigating linkages between reactive oxygen species and health.
T. Sakazaki, M. Shiotani, M. Suzuki, D. Kinnison, J. M. Zawodny, M. McHugh, and K. A. Walker
Atmos. Chem. Phys., 15, 829–843, https://doi.org/10.5194/acp-15-829-2015, https://doi.org/10.5194/acp-15-829-2015, 2015
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The solar occultation measurements measure the atmosphere at sunrise (SR) and sunset (SS). It has been reported that there is a significant difference in the observed amount of stratospheric ozone between SR and SS. This study first revealed that this difference can be largely explained by diurnal variations in ozone, particularly those caused by vertical transport by the atmospheric tidal winds. Our results would be helpful for the construction of combined data sets from SR and SS profiles.
C. Prados-Roman, C. A. Cuevas, T. Hay, R. P. Fernandez, A. S. Mahajan, S.-J. Royer, M. Galí, R. Simó, J. Dachs, K. Großmann, D. E. Kinnison, J.-F. Lamarque, and A. Saiz-Lopez
Atmos. Chem. Phys., 15, 583–593, https://doi.org/10.5194/acp-15-583-2015, https://doi.org/10.5194/acp-15-583-2015, 2015
R. P. Fernandez, R. J. Salawitch, D. E. Kinnison, J.-F. Lamarque, and A. Saiz-Lopez
Atmos. Chem. Phys., 14, 13391–13410, https://doi.org/10.5194/acp-14-13391-2014, https://doi.org/10.5194/acp-14-13391-2014, 2014
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We propose the existence of a daytime “tropical ring of atomic bromine” surrounding the tropics at a height between 15 and 19km. Our simulations show that VSL bromocarbons produce increases of 3pptv for inorganic bromine and 2pptv for organic bromine in the tropical TTL on an annual average, resulting in a total stratospheric bromine injection of 5pptv. This result suggests that the inorganic bromine injected into the stratosphere may be larger than that from VSL bromocarbons.
A. Saiz-Lopez, R. P. Fernandez, C. Ordóñez, D. E. Kinnison, J. C. Gómez Martín, J.-F. Lamarque, and S. Tilmes
Atmos. Chem. Phys., 14, 13119–13143, https://doi.org/10.5194/acp-14-13119-2014, https://doi.org/10.5194/acp-14-13119-2014, 2014
V. Verma, T. Fang, H. Guo, L. King, J. T. Bates, R. E. Peltier, E. Edgerton, A. G. Russell, and R. J. Weber
Atmos. Chem. Phys., 14, 12915–12930, https://doi.org/10.5194/acp-14-12915-2014, https://doi.org/10.5194/acp-14-12915-2014, 2014
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The major emission sources of the reactive oxygen species (ROS) associated with ambient particulate matter in the southeastern United States were identified. The study shows biomass burning and secondary aerosol formation as the major sources contributing to the ROS-generating capability of ambient particles. The ubiquitous nature of these two sources suggests widespread population exposures to the toxic aerosol components.
Y. You, V. P. Kanawade, J. A. de Gouw, A. B. Guenther, S. Madronich, M. R. Sierra-Hernández, M. Lawler, J. N. Smith, S. Takahama, G. Ruggeri, A. Koss, K. Olson, K. Baumann, R. J. Weber, A. Nenes, H. Guo, E. S. Edgerton, L. Porcelli, W. H. Brune, A. H. Goldstein, and S.-H. Lee
Atmos. Chem. Phys., 14, 12181–12194, https://doi.org/10.5194/acp-14-12181-2014, https://doi.org/10.5194/acp-14-12181-2014, 2014
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Amiens play important roles in atmospheric secondary aerosol formation and human health, but the fast response measurements of amines are lacking. Here we show measurements in a southeastern US forest and a moderately polluted midwestern site. Our results show that gas to particle conversion is an important process that controls ambient amine concentrations and that biomass burning is an important source of amines.
G. M. Hidy, C. L. Blanchard, K. Baumann, E. Edgerton, S. Tanenbaum, S. Shaw, E. Knipping, I. Tombach, J. Jansen, and J. Walters
Atmos. Chem. Phys., 14, 11893–11914, https://doi.org/10.5194/acp-14-11893-2014, https://doi.org/10.5194/acp-14-11893-2014, 2014
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This paper reviews aerometric measurements from Centreville, Alabama. The measurements show annual trends with air pollution emissions from 1999 to 2013. They provide a context for observations from 1 June to 15 July 2013 supporting the Southern Oxidant and Aerosol Study. An important goal of this experiment was to advance knowledge of aerosols produced in the atmosphere from precursors. The observations were in moist and warm conditions with the lowest gas and particle concentrations recorded.
S. Coburn, I. Ortega, R. Thalman, B. Blomquist, C. W. Fairall, and R. Volkamer
Atmos. Meas. Tech., 7, 3579–3595, https://doi.org/10.5194/amt-7-3579-2014, https://doi.org/10.5194/amt-7-3579-2014, 2014
T. Wang, W. J. Randel, A. E. Dessler, M. R. Schoeberl, and D. E. Kinnison
Atmos. Chem. Phys., 14, 7135–7147, https://doi.org/10.5194/acp-14-7135-2014, https://doi.org/10.5194/acp-14-7135-2014, 2014
S. H. Budisulistiorini, M. R. Canagaratna, P. L. Croteau, K. Baumann, E. S. Edgerton, M. S. Kollman, N. L. Ng, V. Verma, S. L. Shaw, E. M. Knipping, D. R. Worsnop, J. T. Jayne, R.J. Weber, and J. D. Surratt
Atmos. Meas. Tech., 7, 1929–1941, https://doi.org/10.5194/amt-7-1929-2014, https://doi.org/10.5194/amt-7-1929-2014, 2014
C. Knote, A. Hodzic, J. L. Jimenez, R. Volkamer, J. J. Orlando, S. Baidar, J. Brioude, J. Fast, D. R. Gentner, A. H. Goldstein, P. L. Hayes, W. B. Knighton, H. Oetjen, A. Setyan, H. Stark, R. Thalman, G. Tyndall, R. Washenfelder, E. Waxman, and Q. Zhang
Atmos. Chem. Phys., 14, 6213–6239, https://doi.org/10.5194/acp-14-6213-2014, https://doi.org/10.5194/acp-14-6213-2014, 2014
S. Zhou, L. Gonzalez, A. Leithead, Z. Finewax, R. Thalman, A. Vlasenko, S. Vagle, L.A. Miller, S.-M. Li, S. Bureekul, H. Furutani, M. Uematsu, R. Volkamer, and J. Abbatt
Atmos. Chem. Phys., 14, 1371–1384, https://doi.org/10.5194/acp-14-1371-2014, https://doi.org/10.5194/acp-14-1371-2014, 2014
J. Liu, M. Bergin, H. Guo, L. King, N. Kotra, E. Edgerton, and R. J. Weber
Atmos. Chem. Phys., 13, 12389–12404, https://doi.org/10.5194/acp-13-12389-2013, https://doi.org/10.5194/acp-13-12389-2013, 2013
M. Abalos, W. J. Randel, D. E. Kinnison, and E. Serrano
Atmos. Chem. Phys., 13, 10591–10607, https://doi.org/10.5194/acp-13-10591-2013, https://doi.org/10.5194/acp-13-10591-2013, 2013
U. S. Nair, Y. Wu, C. D. Holmes, A. Ter Schure, G. Kallos, and J. T. Walters
Atmos. Chem. Phys., 13, 10143–10157, https://doi.org/10.5194/acp-13-10143-2013, https://doi.org/10.5194/acp-13-10143-2013, 2013
Y.-H. Lin, E. M. Knipping, E. S. Edgerton, S. L. Shaw, and J. D. Surratt
Atmos. Chem. Phys., 13, 8457–8470, https://doi.org/10.5194/acp-13-8457-2013, https://doi.org/10.5194/acp-13-8457-2013, 2013
R. Sinreich, A. Merten, L. Molina, and R. Volkamer
Atmos. Meas. Tech., 6, 1521–1532, https://doi.org/10.5194/amt-6-1521-2013, https://doi.org/10.5194/amt-6-1521-2013, 2013
F. Khosrawi, R. Müller, J. Urban, M. H. Proffitt, G. Stiller, M. Kiefer, S. Lossow, D. Kinnison, F. Olschewski, M. Riese, and D. Murtagh
Atmos. Chem. Phys., 13, 3619–3641, https://doi.org/10.5194/acp-13-3619-2013, https://doi.org/10.5194/acp-13-3619-2013, 2013
S. Baidar, H. Oetjen, S. Coburn, B. Dix, I. Ortega, R. Sinreich, and R. Volkamer
Atmos. Meas. Tech., 6, 719–739, https://doi.org/10.5194/amt-6-719-2013, https://doi.org/10.5194/amt-6-719-2013, 2013
C. Tatum Ernest, D. Donohoue, D. Bauer, A. Ter Schure, and A. J. Hynes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-12-33291-2012, https://doi.org/10.5194/acpd-12-33291-2012, 2012
Revised manuscript not accepted
Related subject area
Subject: Gases | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
The impact of organic nitrates on summer ozone formation in Shanghai, China
Differences in the key volatile organic compound species between their emitted and ambient concentrations in ozone formation
Mechanistic insights into chloroacetic acid production from atmospheric multiphase volatile organic compound–chlorine chemistry
Accurate elucidation of oxidation under heavy ozone pollution: a full suite of radical measurements in the chemically complex atmosphere
Emissions of intermediate-volatility and semi-volatile organic compounds (I/SVOCs) from different cumulative-mileage diesel vehicles at various ambient temperatures
Characterization of nitrous acid and its potential effects on secondary pollution in the warm season in Beijing urban areas
Vertical changes in volatile organic compounds (VOCs) and impacts on photochemical ozone formation
Diurnal, seasonal, and interannual variations in δ(18O) of atmospheric O2 and its application to evaluate natural and anthropogenic changes in oxygen, carbon, and water cycles
Cloud processing of dimethyl sulfide (DMS) oxidation products limits sulfur dioxide (SO2) and carbonyl sulfide (OCS) production in the eastern North Atlantic marine boundary layer
Atmospheric carbonyl compounds are crucial in regional ozone heavy pollution: insights from the Chengdu Plain Urban Agglomeration, China
Understanding summertime peroxyacetyl nitrate (PAN) formation and its relation to aerosol pollution: insights from high-resolution measurements and modeling
Measurement report: Exploring the variations in ambient BTEX in urban Europe and their environmental health implications
Seasonal air concentration variability, gas–particle partitioning, precipitation scavenging, and air–water equilibrium of organophosphate esters in southern Canada
Global Ground-based Tropospheric Ozone Measurements: Reference Data and Individual Site Trends (2000–2022) from the TOAR-II/HEGIFTOM Project
Measurement report: Surface exchange fluxes of HONO during the growth process of paddy fields in the Huaihe River Basin, China
Marine emissions and trade winds control the atmospheric nitrous oxide in the Galapagos Islands
Molecular and seasonal characteristics of organic vapors in urban Beijing: insights from Vocus-PTR measurements
The variations in volatile organic compounds based on the policy change for Omicron in the traffic hub of Zhengzhou
On the dynamics of ozone depletion events at Villum Research Station in the High Arctic
VOC sources and impacts at an urban Mediterranean area (Marseille – France)
Measurement report: Long-term measurements of surface ozone and trends in semi-natural sub-Saharan African ecosystems
Characterization of biogenic volatile organic compounds and their oxidation products in a stressed spruce-dominated forest close to a biogas power plant
Reactive chlorine-, sulfur-, and nitrogen-containing volatile organic compounds impact atmospheric chemistry in the megacity of Delhi during both clean and extremely polluted seasons
Analysis of the day-to-day variability of ozone vertical profiles in the lower troposphere during the 2022 Paris ACROSS campaign
Significant influence of oxygenated volatile organic compounds on atmospheric chemistry analysis: A case study in a typical industrial city in China
Short lifetimes of organic nitrates in a sub-urban temperate forest indicate efficient assimilation of reactive nitrogen by the biosphere
Ozone deposition measurements over wheat fields in the North China Plain: variability and related factors of deposition flux and velocity
Consistency evaluation of tropospheric ozone from ozonesonde and IAGOS (In-service Aircraft for a Global Observing System) observations: vertical distribution, ozonesonde types, and station–airport distance
CO2 and CO temporal variability over Mexico City from ground-based total column and surface measurements
Investigating carbonyl compounds above the Amazon rainforest using a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS) with NO+ chemical ionization
Measurement report: In-flight and ground-based measurements of nitrogen oxide emissions from latest-generation jet engines and 100 % sustainable aviation fuel
Measurement report: Sources, sinks, and lifetime of NOx in a suburban temperate forest at night
Measurement report: Urban ammonia and amines in Houston, Texas
Biomass-burning sources control ambient particulate matter, but traffic and industrial sources control volatile organic compound (VOC) emissions and secondary-pollutant formation during extreme pollution events in Delhi
Multi-year observations of variable incomplete combustion in the New York megacity
Observations of the vertical distributions of summertime atmospheric pollutants in Nam Co: OH production and source analysis
Spatiotemporal variations in atmospheric CH4 concentrations and enhancements in northern China based on a comprehensive dataset: Ground-based observations, TROPOMI data, inventory data and inversions
Measurement report: Elevated atmospheric ammonia may promote particle pH and HONO formation – insights from the COVID-19 pandemic
Measurement report: Vertical and temporal variability in the near-surface ozone production rate and sensitivity in an urban area in the Pearl River Delta region, China
Elevated oxidized mercury in the free troposphere: analytical advances and application at a remote continental mountaintop site
Using observed urban NOx sinks to constrain VOC reactivity and the ozone and radical budget in the Seoul Metropolitan Area
Real-world emission characteristics of VOCs from typical cargo ships and their potential contributions to secondary organic aerosol and O3 under low-sulfur fuel policies
NO3 reactivity during a summer period in a temperate forest below and above the canopy
The role of oceanic ventilation and terrestrial outflow in atmospheric non-methane hydrocarbons over the Chinese marginal seas
Concentration and source changes of nitrous acid (HONO) during the COVID-19 lockdown in Beijing
Characteristics and sources of nonmethane volatile organic compounds (NMVOCs) and O3–NOx–NMVOC relationships in Zhengzhou, China
Measurement report: TURBAN observation campaign combining street-level low-cost air quality sensors and meteorological profile measurements in Prague
Deciphering anthropogenic and biogenic contributions to selected non-methane volatile organic compound emissions in an urban area
Emission characteristics of reactive organic gases (ROGs) from industrial volatile chemical products (VCPs) in the Pearl River Delta (PRD), China
Measurement report: Enhanced photochemical formation of formic and isocyanic acids in urban regions aloft – insights from tower-based online gradient measurements
Chunmeng Li, Xiaorui Chen, Haichao Wang, Tianyu Zhai, Xuefei Ma, Xinping Yang, Shiyi Chen, Min Zhou, Shengrong Lou, Xin Li, Limin Zeng, and Keding Lu
Atmos. Chem. Phys., 25, 3905–3918, https://doi.org/10.5194/acp-25-3905-2025, https://doi.org/10.5194/acp-25-3905-2025, 2025
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This study reports an observation of organic nitrate (including total peroxy nitrates and total alkyl nitrates) in Shanghai, China, during the summer of 2021, by homemade thermal dissociation cavity-enhanced absorption spectroscopy (TD-CEAS; Atmos. Meas. Tech., 14, 4033–4051, 2021). The distribution of organic nitrates and their effects on local ozone production are analyzed based on field observations in conjunction with model simulations.
Xudong Zheng and Shaodong Xie
Atmos. Chem. Phys., 25, 3807–3820, https://doi.org/10.5194/acp-25-3807-2025, https://doi.org/10.5194/acp-25-3807-2025, 2025
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To reduce uncertainties in identifying the key volatile organic compounds (VOCs) in ozone (O3) formation from ambient concentrations, this study comprehensively calculates the emitted VOC concentrations during both nighttime and daytime using the nitrate radical, O3, and hydroxyl radical reaction rates and ambient VOC concentrations. Based on the emitted concentrations, isoprene is one of the top three species contributing to O3 formation, which may be overlooked in observed concentrations.
Mingxue Li, Men Xia, Chunshui Lin, Yifan Jiang, Weihang Sun, Yurun Wang, Yingnan Zhang, Maoxia He, and Tao Wang
Atmos. Chem. Phys., 25, 3753–3764, https://doi.org/10.5194/acp-25-3753-2025, https://doi.org/10.5194/acp-25-3753-2025, 2025
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Our field campaigns observed a strong diel pattern of chloroacetic acid as well as a strong correlation between its level and that of reactive chlorine species at a coastal site. Using quantum chemical calculations and box model simulation with an updated Master Chemical Mechanism, we found that the formation pathway of chloroacetic acid involved multiphase processes. Our study enhances understanding of atmospheric organic chlorine chemistry and emphasizes the importance of multiphase reactions.
Renzhi Hu, Guoxian Zhang, Haotian Cai, Jingyi Guo, Keding Lu, Xin Li, Shengrong Lou, Zhaofeng Tan, Changjin Hu, Pinhua Xie, and Wenqing Liu
Atmos. Chem. Phys., 25, 3011–3028, https://doi.org/10.5194/acp-25-3011-2025, https://doi.org/10.5194/acp-25-3011-2025, 2025
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A full suite of radical measurements (OH, HO2, RO2, and kOH) was established to accurately elucidate the limitations of oxidation in a chemically complex atmosphere. Sensitivity tests revealed that the incorporation of complex processes enabled a balance in both radical concentrations and coordinate ratios, effectively addressing the deficiency in the ozone generation mechanism. The full-chain radical detection bridged the gap between the photochemistry and the intensive oxidation level.
Shuwen Guo, Xuan Zheng, Xiao He, Lewei Zeng, Liqiang He, Xian Wu, Yifei Dai, Zihao Huang, Ting Chen, Shupei Xiao, Yan You, Sheng Xiang, Shaojun Zhang, Jingkun Jiang, and Ye Wu
Atmos. Chem. Phys., 25, 2695–2705, https://doi.org/10.5194/acp-25-2695-2025, https://doi.org/10.5194/acp-25-2695-2025, 2025
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We considered two potential influencing factors of heavy-duty diesel vehicle emissions that are rarely mentioned in the literature: cumulative mileage and ambient temperatures. The results suggest that prolonged use of heavy-duty diesel vehicles and low ambient temperatures leads to reduced engine combustion efficiency, which in turn increases tailpipe emissions significantly.
Junling Li, Chaofan Lian, Mingyuan Liu, Hao Zhang, Yongxin Yan, Yufei Song, Chun Chen, Jiaqi Wang, Haijie Zhang, Yanqin Ren, Yucong Guo, Weigang Wang, Yisheng Xu, Hong Li, Jian Gao, and Maofa Ge
Atmos. Chem. Phys., 25, 2551–2568, https://doi.org/10.5194/acp-25-2551-2025, https://doi.org/10.5194/acp-25-2551-2025, 2025
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As a key source of hydroxyl (OH) radical, nitrous acid (HONO) has attracted much attention for its important role in the atmospheric oxidant capacity (AOC) increase. In this study, we made a comparison of the ambient levels, variation patterns, sources, and formation pathway in the warm season on the basis of continuous intensive observations at an urban site of Beijing. This work highlights the importance of HONO for the AOC in the warm season.
Xiao-Bing Li, Bin Yuan, Yibo Huangfu, Suxia Yang, Xin Song, Jipeng Qi, Xianjun He, Sihang Wang, Yubin Chen, Qing Yang, Yongxin Song, Yuwen Peng, Guiqian Tang, Jian Gao, Dasa Gu, and Min Shao
Atmos. Chem. Phys., 25, 2459–2472, https://doi.org/10.5194/acp-25-2459-2025, https://doi.org/10.5194/acp-25-2459-2025, 2025
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Online vertical gradient measurements of volatile organic compounds (VOCs), ozone, and NOx were conducted based on a 325 m tall tower in urban Beijing. Vertical changes in the concentrations, compositions, key drivers, and environmental impacts of VOCs were analyzed in this study. We find that VOC species display differentiated vertical variation patterns and distinct roles in contributing to photochemical ozone formation with increasing height in the urban planetary boundary layer.
Shigeyuki Ishidoya, Satoshi Sugawara, and Atsushi Okazaki
Atmos. Chem. Phys., 25, 1965–1987, https://doi.org/10.5194/acp-25-1965-2025, https://doi.org/10.5194/acp-25-1965-2025, 2025
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The 18O/16O ratio of atmospheric oxygen, δatm(18O), is higher than that of ocean water due to isotopic effects during biospheric activities. This is known as the Dole–Morita effect, and its millennial-scale variations are recorded in ice cores. However, small variations of δatm(18O) in the present day have never been detected so far. This paper presents the first observations of diurnal, seasonal, and secular variations in δatm(18O) and applies them to evaluate oxygen, carbon, and water cycles.
Delaney B. Kilgour, Christopher M. Jernigan, Olga Garmash, Sneha Aggarwal, Shengqian Zhou, Claudia Mohr, Matt E. Salter, Joel A. Thornton, Jian Wang, Paul Zieger, and Timothy H. Bertram
Atmos. Chem. Phys., 25, 1931–1947, https://doi.org/10.5194/acp-25-1931-2025, https://doi.org/10.5194/acp-25-1931-2025, 2025
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We report simultaneous measurements of dimethyl sulfide (DMS) and hydroperoxymethyl thioformate (HPMTF) in the eastern North Atlantic. We use an observationally constrained box model to show that cloud loss is the dominant sink of HPMTF in this region over 6 weeks, resulting in large reductions in DMS-derived products that contribute to aerosol formation and growth. Our findings indicate that fast cloud processing of HPMTF must be included in global models to accurately capture the sulfur cycle.
Jiemeng Bao, Xin Zhang, Zhenhai Wu, Li Zhou, Jun Qian, Qinwen Tan, Fumo Yang, Junhui Chen, Yunfeng Li, Hefan Liu, Liqun Deng, and Hong Li
Atmos. Chem. Phys., 25, 1899–1916, https://doi.org/10.5194/acp-25-1899-2025, https://doi.org/10.5194/acp-25-1899-2025, 2025
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We studied carbonyl compounds' role in ozone pollution in the Chengdu Plain Urban Agglomeration, China. During heavy pollution in August 2019, we measured carbonyls at nine sites and analyzed their impact. Areas with higher carbonyl levels, like Chengdu, had worse ozone pollution. While their abundance matters, chemical reactions with other pollutants are the main drivers. Our findings show regional cooperation is vital to reducing ozone pollution effectively.
Baoye Hu, Naihua Chen, Rui Li, Mingqiang Huang, Jinsheng Chen, Youwei Hong, Lingling Xu, Xiaolong Fan, Mengren Li, Lei Tong, Qiuping Zheng, and Yuxiang Yang
Atmos. Chem. Phys., 25, 905–921, https://doi.org/10.5194/acp-25-905-2025, https://doi.org/10.5194/acp-25-905-2025, 2025
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Box modeling with the Master Chemical Mechanism (MCM) was used to explore summertime peroxyacetyl nitrate (PAN) formation and its link to aerosol pollution under high-ozone conditions. The MCM model is effective in the study of PAN photochemical formation and performed better during the clean period than the haze period. Machine learning analysis identified ammonia, nitrate, and fine particulate matter as the top three factors contributing to simulation bias.
Xiansheng Liu, Xun Zhang, Marvin Dufresne, Tao Wang, Lijie Wu, Rosa Lara, Roger Seco, Marta Monge, Ana Maria Yáñez-Serrano, Marie Gohy, Paul Petit, Audrey Chevalier, Marie-Pierre Vagnot, Yann Fortier, Alexia Baudic, Véronique Ghersi, Grégory Gille, Ludovic Lanzi, Valérie Gros, Leïla Simon, Heidi Héllen, Stefan Reimann, Zoé Le Bras, Michelle Jessy Müller, David Beddows, Siqi Hou, Zongbo Shi, Roy M. Harrison, William Bloss, James Dernie, Stéphane Sauvage, Philip K. Hopke, Xiaoli Duan, Taicheng An, Alastair C. Lewis, James R. Hopkins, Eleni Liakakou, Nikolaos Mihalopoulos, Xiaohu Zhang, Andrés Alastuey, Xavier Querol, and Thérèse Salameh
Atmos. Chem. Phys., 25, 625–638, https://doi.org/10.5194/acp-25-625-2025, https://doi.org/10.5194/acp-25-625-2025, 2025
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This study examines BTEX (benzene, toluene, ethylbenzene, xylenes) pollution in urban areas across seven European countries. Analyzing data from 22 monitoring sites, we found traffic and industrial activities significantly impact BTEX levels, with peaks during rush hours. The risk from BTEX exposure remains moderate, especially in high-traffic and industrial zones, highlighting the need for targeted air quality management to protect public health and improve urban air quality.
Yuening Li, Faqiang Zhan, Chubashini Shunthirasingham, Ying Duan Lei, Jenny Oh, Amina Ben Chaaben, Zhe Lu, Kelsey Lee, Frank A. P. C. Gobas, Hayley Hung, and Frank Wania
Atmos. Chem. Phys., 25, 459–472, https://doi.org/10.5194/acp-25-459-2025, https://doi.org/10.5194/acp-25-459-2025, 2025
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Organophosphate esters are important humanmade trace contaminants. Measuring them in the atmospheric gas phase, particles, precipitation, and surface water in Canada, we explore seasonal concentration variability, gas–particle partitioning, precipitation scavenging, and the air–water equilibrium. Whereas higher summer concentrations and efficient precipitation scavenging conform with expectations, the lack of a relationship between compound volatility and gas–particle partitioning is puzzling.
Roeland Van Malderen, Anne M. Thompson, Debra E. Kollonige, Ryan M. Stauffer, Herman G. J. Smit, Eliane Maillard Barras, Corinne Vigouroux, Irina Petropavlovskikh, Thierry Leblanc, Valérie Thouret, Pawel Wolff, Peter Effertz, David W. Tarasick, Deniz Poyraz, Gérard Ancellet, Marie-Renée De Backer, Stéphanie Evan, Victoria Flood, Matthias M. Frey, James W. Hannigan, José L. Hernandez, Marco Iarlori, Bryan J. Johnson, Nicholas Jones, Rigel Kivi, Emmanuel Mahieu, Glen McConville, Katrin Müller, Tomoo Nagahama, Justus Notholt, Ankie Piters, Natalia Prats, Richard Querel, Dan Smale, Wolfgang Steinbrecht, Kimberly Strong, and Ralf Sussmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-3736, https://doi.org/10.5194/egusphere-2024-3736, 2025
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Tropospheric ozone is an important greenhouse gas and is an air pollutant. The time variability of tropospheric ozone is mainly driven by anthropogenic emissions. In this paper, we study the distribution and time variability of ozone from harmonized ground-based observations from five different measurement techniques. Our findings will provide clear standard references for atmospheric models and evolving tropospheric ozone satellite data for the 2000–2022 period.
Fanhao Meng, Baobin Han, Min Qin, Wu Fang, Ke Tang, Dou Shao, Zhitang Liao, Jun Duan, Yan Feng, Yong Huang, Ting Ni, and Pinhua Xie
Atmos. Chem. Phys., 24, 14191–14208, https://doi.org/10.5194/acp-24-14191-2024, https://doi.org/10.5194/acp-24-14191-2024, 2024
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Comprehensive observations of HONO and NOx fluxes were conducted over paddy fields in the Huaihe River Basin. Consecutive peaks in HONO and NO fluxes suggest a potentially enhanced release of HONO and NO due to soil tillage, whereas waterlogged soil may inhibit microbial nitrification processes following irrigation. Notably, biological processes and light-driven NO2 reactions at the surface may serve as sources of HONO and influence the local HONO budget during rotary tillage.
Timur Cinay, Dickon Young, Nazaret Narváez Jimenez, Cristina Vintimilla-Palacios, Ariel Pila Alonso, Paul B. Krummel, William Vizuete, and Andrew R. Babbin
EGUsphere, https://doi.org/10.5194/egusphere-2024-3769, https://doi.org/10.5194/egusphere-2024-3769, 2024
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We present the initial 15 months of nitrous oxide measurements from the Galapagos Emissions Monitoring Station. The observed variability in atmospheric mole fractions during this period can be linked to several factors: seasonal variations in trade wind speed and direction across the eastern Pacific, differences in the transport history of air masses sampled, and spatiotemporal heterogeneity in regional marine nitrous oxide emissions from coastal upwelling systems of Peru and Chile.
Zhaojin An, Rujing Yin, Xinyan Zhao, Xiaoxiao Li, Yuyang Li, Yi Yuan, Junchen Guo, Yiqi Zhao, Xue Li, Dandan Li, Yaowei Li, Dongbin Wang, Chao Yan, Kebin He, Douglas R. Worsnop, Frank N. Keutsch, and Jingkun Jiang
Atmos. Chem. Phys., 24, 13793–13810, https://doi.org/10.5194/acp-24-13793-2024, https://doi.org/10.5194/acp-24-13793-2024, 2024
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Online Vocus-PTR measurements show the compositions and seasonal variations in organic vapors in urban Beijing. With enhanced sensitivity and mass resolution, various species at a level of sub-parts per trillion (ppt) and organics with multiple oxygens (≥ 3) were observed. The fast photooxidation process in summer leads to an increase in both concentration and proportion of organics with multiple oxygens, while, in other seasons, the variations in them could be influenced by mixed sources.
Bowen Zhang, Dong Zhang, Zhe Dong, Xinshuai Song, Ruiqin Zhang, and Xiao Li
Atmos. Chem. Phys., 24, 13587–13601, https://doi.org/10.5194/acp-24-13587-2024, https://doi.org/10.5194/acp-24-13587-2024, 2024
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To gain insight into the impact of changes due to epidemic control policies, we undertook continuous online monitoring of volatile organic compounds (VOCs) at an urban site in Zhengzhou over a 2-month period. This study examines the characteristics of VOCs, their sources, and their temporal evolution. It also assesses the impact of the policy change on VOC pollution during the monitoring period, thus providing a basis for further research on VOC pollution and source control.
Jakob Boyd Pernov, Jens Liengaard Hjorth, Lise Lotte Sørensen, and Henrik Skov
Atmos. Chem. Phys., 24, 13603–13631, https://doi.org/10.5194/acp-24-13603-2024, https://doi.org/10.5194/acp-24-13603-2024, 2024
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Arctic ozone depletion events (ODEs) occur every spring and have vast implications for the oxidizing capacity, radiative balance, and mercury oxidation. In this study, we analyze ozone, ODEs, and their connection to meteorological and air mass history variables through statistical analyses, back trajectories, and machine learning (ML) at Villum Research Station. ODEs are favorable under sunny, calm conditions with air masses arriving from northerly wind directions with sea ice contact.
Marvin Dufresne, Thérèse Salameh, Thierry Léonardis, Grégory Gille, Alexandre Armengaud, and Stéphane Sauvage
EGUsphere, https://doi.org/10.5194/egusphere-2024-3576, https://doi.org/10.5194/egusphere-2024-3576, 2024
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This paper is about the eighteen-months measurement of Non-Methane Hydrocarbons (NMHC) at Marseille, were there was no measurement since early 2000 despite the impact of NMHC on air quality and climate. The traffic related sources are the first contributor to NMHC concentrations in Marseille and shipping strongly contribute to the formation of aerosols. Finally, the lockdown due to the Covid-19 had an impact on NMHC concentrations reaching a fifty percents decreasing for traffic-related sources.
Hagninou Elagnon Venance Donnou, Aristide Barthélémy Akpo, Money Ossohou, Claire Delon, Véronique Yoboué, Dungall Laouali, Marie Ouafo-Leumbe, Pieter Gideon Van Zyl, Ousmane Ndiaye, Eric Gardrat, Maria Dias-Alves, and Corinne Galy-Lacaux
Atmos. Chem. Phys., 24, 13151–13182, https://doi.org/10.5194/acp-24-13151-2024, https://doi.org/10.5194/acp-24-13151-2024, 2024
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Ozone is a secondary air pollutant that is detrimental to human and plant health. A better understanding of its chemical evolution is a challenge for Africa, where it is still undersampled. Out of 14 sites examined (1995–2020), high levels of O3 are reported in southern Africa. The dominant chemical processes leading to O3 formation are identified. A decrease in O3 is observed at Katibougou (Mali) and Banizoumbou (Niger), and an increase is found at Zoétélé (Cameroon) and Skukuza (South Africa).
Junwei Song, Georgios I. Gkatzelis, Ralf Tillmann, Nicolas Brüggemann, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 13199–13217, https://doi.org/10.5194/acp-24-13199-2024, https://doi.org/10.5194/acp-24-13199-2024, 2024
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Biogenic volatile organic compounds (BVOCs) and organic aerosol (OA) particles were measured online in a stressed spruce-dominated forest. OA was mainly attributed to the monoterpene oxidation products. The mixing ratios of BVOCs were higher than the values previously measured in other temperate forests. The results demonstrate that BVOCs are influenced not only by meteorology and biogenic emissions but also by local anthropogenic emissions and subsequent chemical transformation processes.
Sachin Mishra, Vinayak Sinha, Haseeb Hakkim, Arpit Awasthi, Sachin D. Ghude, Vijay Kumar Soni, Narendra Nigam, Baerbel Sinha, and Madhavan N. Rajeevan
Atmos. Chem. Phys., 24, 13129–13150, https://doi.org/10.5194/acp-24-13129-2024, https://doi.org/10.5194/acp-24-13129-2024, 2024
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We quantified 111 gases using mass spectrometry to understand how seasonal and emission changes lead from clean air in the monsoon season to extremely polluted air in the post-monsoon season in Delhi. Averaged total mass concentrations (260 µg m-3) were > 4 times in polluted periods, driven by biomass burning emissions and reduced atmospheric ventilation. Reactive gaseous nitrogen, chlorine, and sulfur compounds hitherto unreported from such a polluted environment were discovered.
Gérard Ancellet, Camille Viatte, Anne Boynard, François Ravetta, Jacques Pelon, Cristelle Cailteau-Fischbach, Pascal Genau, Julie Capo, Axel Roy, and Philippe Nédélec
Atmos. Chem. Phys., 24, 12963–12983, https://doi.org/10.5194/acp-24-12963-2024, https://doi.org/10.5194/acp-24-12963-2024, 2024
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Characterization of ozone pollution in urban areas benefited from a measurement campaign in summer 2022 in the Paris region. The analysis is based on 21 d of lidar and aircraft observations. The main objective is an analysis of the sensitivity of ozone pollution to the micrometeorological processes in the urban atmospheric boundary layer and the transport of regional pollution. The paper also discusses to what extent satellite observations can track observed ozone plumes.
Jingwen Dai, Kun Zhang, Yanli Feng, Xin Yi, Rui Li, Jin Xue, Qing Li, Lishu Shi, Jiaqiang Liao, Yanan Yi, Fangting Wang, Liumei Yang, Hui Chen, Ling Huang, Jiani Tan, Yangjun Wang, and Li Li
EGUsphere, https://doi.org/10.5194/egusphere-2024-3201, https://doi.org/10.5194/egusphere-2024-3201, 2024
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Oxygenated volatile organic compounds (OVOCs) are important ozone (O3) precursors. However, most of O3 formation analysis based on the box model (OBM) don't include OVOCs constraint To access the interference of OVOCs on O3 simulation, this study conducted field campaign and OBM analysis. The results indicates that no OVOCs constraint in the OBM can lead to overestimate of OVOCs, free radicals, and O3.
Simone T. Andersen, Rolf Sander, Patrick Dewald, Laura Wüst, Tobias Seubert, Gunther N. T. E. Türk, Jan Schuladen, Max R. McGillen, Chaoyang Xue, Abdelwahid Mellouki, Alexandre Kukui, Vincent Michoud, Manuela Cirtog, Mathieu Cazaunau, Astrid Bauville, Hichem Bouzidi, Paola Formenti, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Christopher Cantrell, Jos Lelieveld, and John N. Crowley
EGUsphere, https://doi.org/10.5194/egusphere-2024-3437, https://doi.org/10.5194/egusphere-2024-3437, 2024
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Measurements and modelling of reactive nitrogen gases observed in a suburban temperate forest in Rambouillet, France circa 50 km southwest of Paris in 2022 indicate that the biosphere rapidly scavenges organic nitrates of mixed biogenic and anthropogenic origin, resulting in short lifetimes for e.g. alkyl nitrates and peroxy nitrates.
Xiaoyi Zhang, Wanyun Xu, Weili Lin, Gen Zhang, Jinjian Geng, Li Zhou, Huarong Zhao, Sanxue Ren, Guangsheng Zhou, Jianmin Chen, and Xiaobin Xu
Atmos. Chem. Phys., 24, 12323–12340, https://doi.org/10.5194/acp-24-12323-2024, https://doi.org/10.5194/acp-24-12323-2024, 2024
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Ozone (O3) deposition is a key process that removes surface O3, affecting air quality, ecosystems and climate change. We conducted O3 deposition measurement over a wheat canopy using a newly relaxed eddy accumulation flux system. Large variabilities in O3 deposition were detected, mainly determined by crop growth and modulated by various environmental factors. More O3 deposition observations over different surfaces are needed for exploring deposition mechanisms and model optimization.
Honglei Wang, David W. Tarasick, Jane Liu, Herman G. J. Smit, Roeland Van Malderen, Lijuan Shen, Romain Blot, and Tianliang Zhao
Atmos. Chem. Phys., 24, 11927–11942, https://doi.org/10.5194/acp-24-11927-2024, https://doi.org/10.5194/acp-24-11927-2024, 2024
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In this study, we identify 23 suitable pairs of sites from World Ozone and Ultraviolet Radiation Data Centre (WOUDC) and In-service Aircraft for a Global Observing System (IAGOS) datasets (1995 to 2021), compare the average vertical distributions of tropospheric O3 from ozonesonde and aircraft measurements, and analyze the differences based on ozonesonde type and station–airport distance.
Noémie Taquet, Wolfgang Stremme, María Eugenia González del Castillo, Victor Almanza, Alejandro Bezanilla, Olivier Laurent, Carlos Alberti, Frank Hase, Michel Ramonet, Thomas Lauvaux, Ke Che, and Michel Grutter
Atmos. Chem. Phys., 24, 11823–11848, https://doi.org/10.5194/acp-24-11823-2024, https://doi.org/10.5194/acp-24-11823-2024, 2024
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We characterize the variability in CO and CO2 emissions over Mexico City from long-term time-resolved Fourier transform infrared spectroscopy solar absorption and surface measurements from 2013 to 2021. Using the average intraday CO growth rate from total columns, the average CO / CO2 ratio and TROPOMI data, we estimate the interannual variability in the CO and CO2 anthropogenic emissions of Mexico City, highlighting the effect of an unprecedented drop in activity due to the COVID-19 lockdown.
Akima Ringsdorf, Achim Edtbauer, Bruna Holanda, Christopher Poehlker, Marta O. Sá, Alessandro Araújo, Jürgen Kesselmeier, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 24, 11883–11910, https://doi.org/10.5194/acp-24-11883-2024, https://doi.org/10.5194/acp-24-11883-2024, 2024
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We show the average height distribution of separately observed aldehydes and ketones over a day and discuss their rainforest-specific sources and sinks as well as their seasonal changes above the Amazon. Ketones have much longer atmospheric lifetimes than aldehydes and thus different implications for atmospheric chemistry. However, they are commonly observed together, which we overcome by measuring with a NO+ chemical ionization mass spectrometer for the first time in the Amazon rainforest.
Theresa Harlass, Rebecca Dischl, Stefan Kaufmann, Raphael Märkl, Daniel Sauer, Monika Scheibe, Paul Stock, Tiziana Bräuer, Andreas Dörnbrack, Anke Roiger, Hans Schlager, Ulrich Schumann, Magdalena Pühl, Tobias Schripp, Tobias Grein, Linda Bondorf, Charles Renard, Maxime Gauthier, Mark Johnson, Darren Luff, Paul Madden, Peter Swann, Denise Ahrens, Reetu Sallinen, and Christiane Voigt
Atmos. Chem. Phys., 24, 11807–11822, https://doi.org/10.5194/acp-24-11807-2024, https://doi.org/10.5194/acp-24-11807-2024, 2024
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Emissions from aircraft have a direct impact on our climate. Here, we present airborne and ground-based measurement data of nitrogen oxides that were collected in the exhaust of an Airbus aircraft. We study the impact of burning fossil and sustainable aviation fuel on nitrogen oxide emissions at different engine settings related to combustor temperature, pressure and fuel flow. Further, we compare observations with engine emission models.
Simone T. Andersen, Max R. McGillen, Chaoyang Xue, Tobias Seubert, Patrick Dewald, Gunther N. T. E. Türk, Jan Schuladen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Abdelwahid Mellouki, Lucy J. Carpenter, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 11603–11618, https://doi.org/10.5194/acp-24-11603-2024, https://doi.org/10.5194/acp-24-11603-2024, 2024
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Using measurements of various trace gases in a suburban forest near Paris in the summer of 2022, we were able to gain insight into the sources and sinks of NOx (NO+NO2) with a special focus on their nighttime chemical and physical loss processes. NO was observed as a result of nighttime soil emissions when O3 levels were strongly depleted by deposition. NO oxidation products were not observed at night, indicating that soil and/or foliar surfaces are an efficient sink of reactive N.
Lee Tiszenkel, James H. Flynn, and Shan-Hu Lee
Atmos. Chem. Phys., 24, 11351–11363, https://doi.org/10.5194/acp-24-11351-2024, https://doi.org/10.5194/acp-24-11351-2024, 2024
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Ammonia and amines are important ingredients for aerosol formation in urban environments, but the measurements of these compounds are extremely challenging. Our observations show that urban ammonia and amines in Houston are emitted from urban sources, and diurnal variations in their concentrations are likely governed by gas-to-particle conversion and emissions.
Arpit Awasthi, Baerbel Sinha, Haseeb Hakkim, Sachin Mishra, Varkrishna Mummidivarapu, Gurmanjot Singh, Sachin D. Ghude, Vijay Kumar Soni, Narendra Nigam, Vinayak Sinha, and Madhavan N. Rajeevan
Atmos. Chem. Phys., 24, 10279–10304, https://doi.org/10.5194/acp-24-10279-2024, https://doi.org/10.5194/acp-24-10279-2024, 2024
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We use 111 volatile organic compounds (VOCs), PM10, and PM2.5 in a positive matrix factorization (PMF) model to resolve 11 pollution sources validated with chemical fingerprints. Crop residue burning and heating account for ~ 50 % of the PM, while traffic and industrial emissions dominate the gas-phase VOC burden and formation potential of secondary organic aerosols (> 60 %). Non-tailpipe emissions from compressed-natural-gas-fuelled commercial vehicles dominate the transport sector's PM burden.
Luke D. Schiferl, Cong Cao, Bronte Dalton, Andrew Hallward-Driemeier, Ricardo Toledo-Crow, and Róisín Commane
Atmos. Chem. Phys., 24, 10129–10142, https://doi.org/10.5194/acp-24-10129-2024, https://doi.org/10.5194/acp-24-10129-2024, 2024
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Carbon monoxide (CO) is an air pollutant and an important indicator of the incomplete combustion of fossil fuels in cities. Using 4 years of winter and spring observations in New York City, we found that both the magnitude and variability of CO from the metropolitan area are greater than expected. Transportation emissions cannot explain the missing and variable CO, which points to energy from buildings as a likely underappreciated source of urban air pollution and greenhouse gas emissions.
Chengzhi Xing, Cheng Liu, Chunxiang Ye, Jingkai Xue, Hongyu Wu, Xiangguang Ji, Jinping Ou, and Qihou Hu
Atmos. Chem. Phys., 24, 10093–10112, https://doi.org/10.5194/acp-24-10093-2024, https://doi.org/10.5194/acp-24-10093-2024, 2024
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We identified the contributions of ozone (O3) and nitrous acid (HONO) to the production rates of hydroxide (OH) in vertical space on the Tibetan Plateau (TP). A new insight was offered: the contributions of HONO and O3 to the production rates of OH on the TP are even greater than in lower-altitudes areas. This study enriches the understanding of vertical distribution of atmospheric components and explains the strong atmospheric oxidation capacity (AOC) on the TP.
Pengfei Han, Ning Zeng, Bo Yao, Wen Zhang, Weijun Quan, Pucai Wang, Ting Wang, Minqiang Zhou, Qixiang Cai, Yuzhong Zhang, Ruosi Liang, Wanqi Sun, and Shengxiang Liu
EGUsphere, https://doi.org/10.5194/egusphere-2024-2162, https://doi.org/10.5194/egusphere-2024-2162, 2024
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Methane (CH4) is a potent greenhouse gas. Northern China contributes a large proportion of CH4 emissions yet large observation gaps are existed. Here we compiled a comprehensive dataset which is publicly available including ground-based, satellite-based, inventory and modeling results, to show the CH4 concentrations, enhancements and spatial-temporal variations. The data can benefit the research community, and policy makers for future observations, atmospheric inversions and policy-making.
Xinyuan Zhang, Lingling Wang, Nan Wang, Shuangliang Ma, Shenbo Wang, Ruiqin Zhang, Dong Zhang, Mingkai Wang, and Hongyu Zhang
Atmos. Chem. Phys., 24, 9885–9898, https://doi.org/10.5194/acp-24-9885-2024, https://doi.org/10.5194/acp-24-9885-2024, 2024
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This study highlights the importance of the redox reaction of NO2 with SO2 based on actual atmospheric observations. The particle pH in future China is expected to rise steadily. Consequently, this reaction could become a significant source of HONO in China. Therefore, it is crucial to coordinate the control of SO2, NOx, and NH3 emissions to avoid a rapid increase in the particle pH.
Jun Zhou, Chunsheng Zhang, Aiming Liu, Bin Yuan, Yan Wang, Wenjie Wang, Jie-Ping Zhou, Yixin Hao, Xiao-Bing Li, Xianjun He, Xin Song, Yubin Chen, Suxia Yang, Shuchun Yang, Yanfeng Wu, Bin Jiang, Shan Huang, Junwen Liu, Yuwen Peng, Jipeng Qi, Minhui Deng, Bowen Zhong, Yibo Huangfu, and Min Shao
Atmos. Chem. Phys., 24, 9805–9826, https://doi.org/10.5194/acp-24-9805-2024, https://doi.org/10.5194/acp-24-9805-2024, 2024
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In-depth understanding of the near-ground vertical variability in photochemical ozone (O3) formation is crucial for mitigating O3 pollution. Utilizing a self-built vertical observation system, a direct net photochemical O3 production rate detection system, and an observation-based model, we diagnosed the vertical distributions and formation mechanism of net photochemical O3 production rates and sensitivity in the Pearl River Delta region, one of the most O3-polluted areas in China.
Eleanor J. Derry, Tyler R. Elgiar, Taylor Y. Wilmot, Nicholas W. Hoch, Noah S. Hirshorn, Peter Weiss-Penzias, Christopher F. Lee, John C. Lin, A. Gannet Hallar, Rainer Volkamer, Seth N. Lyman, and Lynne E. Gratz
Atmos. Chem. Phys., 24, 9615–9643, https://doi.org/10.5194/acp-24-9615-2024, https://doi.org/10.5194/acp-24-9615-2024, 2024
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Mercury (Hg) is a globally distributed neurotoxic pollutant. Atmospheric deposition is the main source of Hg in ecosystems. However, measurement biases hinder understanding of the origins and abundance of the more bioavailable oxidized form. We used an improved, calibrated measurement system to study air mass composition and transport of atmospheric Hg at a remote mountaintop site in the central US. Oxidized Hg originated upwind in the low to middle free troposphere under clean, dry conditions.
Benjamin A. Nault, Katherine R. Travis, James H. Crawford, Donald R. Blake, Pedro Campuzano-Jost, Ronald C. Cohen, Joshua P. DiGangi, Glenn S. Diskin, Samuel R. Hall, L. Gregory Huey, Jose L. Jimenez, Kyung-Eun Min, Young Ro Lee, Isobel J. Simpson, Kirk Ullmann, and Armin Wisthaler
Atmos. Chem. Phys., 24, 9573–9595, https://doi.org/10.5194/acp-24-9573-2024, https://doi.org/10.5194/acp-24-9573-2024, 2024
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Ozone (O3) is a pollutant formed from the reactions of gases emitted from various sources. In urban areas, the density of human activities can increase the O3 formation rate (P(O3)), thus impacting air quality and health. Observations collected over Seoul, South Korea, are used to constrain P(O3). A high local P(O3) was found; however, local P(O3) was partly reduced due to compounds typically ignored. These observations also provide constraints for unmeasured compounds that will impact P(O3).
Fan Zhang, Binyu Xiao, Zeyu Liu, Yan Zhang, Chongguo Tian, Rui Li, Can Wu, Yali Lei, Si Zhang, Xinyi Wan, Yubao Chen, Yong Han, Min Cui, Cheng Huang, Hongli Wang, Yingjun Chen, and Gehui Wang
Atmos. Chem. Phys., 24, 8999–9017, https://doi.org/10.5194/acp-24-8999-2024, https://doi.org/10.5194/acp-24-8999-2024, 2024
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Mandatory use of low-sulfur fuel due to global sulfur limit regulations means large uncertainties in volatile organic compound (VOC) emissions. On-board tests of VOCs from nine cargo ships in China were carried out. Results showed that switching from heavy-fuel oil to diesel increased emission factor VOCs by 48 % on average, enhancing O3 and the secondary organic aerosol formation potential. Thus, implementing a global ultra-low-sulfur oil policy needs to be optimized in the near future.
Patrick Dewald, Tobias Seubert, Simone T. Andersen, Gunther N. T. E. Türk, Jan Schuladen, Max R. McGillen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Chaoyang Xue, Abdelwahid Mellouki, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 8983–8997, https://doi.org/10.5194/acp-24-8983-2024, https://doi.org/10.5194/acp-24-8983-2024, 2024
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In the scope of a field campaign in a suburban forest near Paris in the summer of 2022, we measured the reactivity of the nitrate radical NO3 towards biogenic volatile organic compounds (BVOCs; e.g. monoterpenes) mainly below but also above the canopy. NO3 reactivity was the highest during nights with strong temperature inversions and decreased strongly with height. Reactions with BVOCs were the main removal process of NO3 throughout the diel cycle below the canopy.
Jian Wang, Lei Xue, Qianyao Ma, Feng Xu, Gaobin Xu, Shibo Yan, Jiawei Zhang, Jianlong Li, Honghai Zhang, Guiling Zhang, and Zhaohui Chen
Atmos. Chem. Phys., 24, 8721–8736, https://doi.org/10.5194/acp-24-8721-2024, https://doi.org/10.5194/acp-24-8721-2024, 2024
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This study investigated the distribution and sources of non-methane hydrocarbons (NMHCs) in the lower atmosphere over the marginal seas of China. NMHCs, a subset of volatile organic compounds (VOCs), play a crucial role in atmospheric chemistry. Derived from systematic atmospheric sampling in coastal cities and marginal sea regions, this study offers valuable insights into the interaction between land and sea in shaping offshore atmospheric NMHCs.
Yusheng Zhang, Feixue Zheng, Zemin Feng, Chaofan Lian, Weigang Wang, Xiaolong Fan, Wei Ma, Zhuohui Lin, Chang Li, Gen Zhang, Chao Yan, Ying Zhang, Veli-Matti Kerminen, Federico Bianch, Tuukka Petäjä, Juha Kangasluoma, Markku Kulmala, and Yongchun Liu
Atmos. Chem. Phys., 24, 8569–8587, https://doi.org/10.5194/acp-24-8569-2024, https://doi.org/10.5194/acp-24-8569-2024, 2024
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The nitrous acid (HONO) budget was validated during a COVID-19 lockdown event. The main conclusions are (1) HONO concentrations showed a significant decrease from 0.97 to 0.53 ppb during lockdown; (2) vehicle emissions accounted for 53 % of nighttime sources, with the heterogeneous conversion of NO2 on ground surfaces more important than aerosol; and (3) the dominant daytime source shifted from the homogenous reaction between NO and OH (51 %) to nitrate photolysis (53 %) during lockdown.
Dong Zhang, Xiao Li, Minghao Yuan, Yifei Xu, Qixiang Xu, Fangcheng Su, Shenbo Wang, and Ruiqin Zhang
Atmos. Chem. Phys., 24, 8549–8567, https://doi.org/10.5194/acp-24-8549-2024, https://doi.org/10.5194/acp-24-8549-2024, 2024
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The increasing concentration of O3 precursors and unfavorable meteorological conditions are key factors in the formation of O3 pollution in Zhengzhou. Vehicular exhausts (28 %), solvent usage (27 %), and industrial production (22 %) are identified as the main sources of NMVOCs. Moreover, O3 formation in Zhengzhou is found to be in an anthropogenic volatile organic compound (AVOC)-limited regime. Thus, to reduce O3 formation, a minimum AVOCs / NOx reduction ratio ≥ 3 : 1 is recommended.
Petra Bauerová, Josef Keder, Adriana Šindelářová, Ondřej Vlček, William Patiño, Jaroslav Resler, Pavel Krč, Jan Geletič, Hynek Řezníček, Martin Bureš, Kryštof Eben, Michal Belda, Jelena Radović, Vladimír Fuka, Radek Jareš, and Igor Ezau
EGUsphere, https://doi.org/10.5194/egusphere-2024-1222, https://doi.org/10.5194/egusphere-2024-1222, 2024
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We implemented an observation campaign focused on street-level air quality and vertical meteorological profile measurement in Prague using low-cost sensors and remote sensing devices. Low-cost sensors have undergone long-term field testing, own data correction and drift evaluation procedures. A high level of NO2 pollution was confirmed due to the traffic load in streets, peaks of aerosol pollution appeared more under inversion conditions. The data will be further used for PALM model validation.
Arianna Peron, Martin Graus, Marcus Striednig, Christian Lamprecht, Georg Wohlfahrt, and Thomas Karl
Atmos. Chem. Phys., 24, 7063–7083, https://doi.org/10.5194/acp-24-7063-2024, https://doi.org/10.5194/acp-24-7063-2024, 2024
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The anthropogenic fraction of non-methane volatile organic compound (NMVOC) emissions associated with biogenic sources (e.g., terpenes) is investigated based on eddy covariance observations. The anthropogenic fraction of terpene emissions is strongly dependent on season. When analyzing volatile chemical product (VCP) emissions in urban environments, we caution that observations from short-term campaigns might over-/underestimate their significance depending on local and seasonal circumstances.
Sihang Wang, Bin Yuan, Xianjun He, Ru Cui, Xin Song, Yubin Chen, Caihong Wu, Chaomin Wang, Yibo Huangfu, Xiao-Bing Li, Boguang Wang, and Min Shao
Atmos. Chem. Phys., 24, 7101–7121, https://doi.org/10.5194/acp-24-7101-2024, https://doi.org/10.5194/acp-24-7101-2024, 2024
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Emissions of reactive organic gases from industrial volatile chemical product sources are measured. There are large differences among these industrial sources. We show that oxygenated species account for significant contributions to reactive organic gas emissions, especially for industrial sources utilizing water-borne chemicals.
Qing Yang, Xiao-Bing Li, Bin Yuan, Xiaoxiao Zhang, Yibo Huangfu, Lei Yang, Xianjun He, Jipeng Qi, and Min Shao
Atmos. Chem. Phys., 24, 6865–6882, https://doi.org/10.5194/acp-24-6865-2024, https://doi.org/10.5194/acp-24-6865-2024, 2024
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Online vertical gradient measurements of formic and isocyanic acids were made based on a 320 m tower in a megacity. Vertical variations and sources of the two acids were analyzed in this study. We find that formic and isocyanic acids exhibited positive vertical gradients and were mainly contributed by photochemical formations. The formation of formic and isocyanic acids was also significantly enhanced in urban regions aloft.
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Short summary
Here we present a day of case study measurements of the vertical distribution of bromine monoxide over the coastal region of the Gulf of Mexico. These measurements are used to assess the contribution of bromine radicals to the oxidation of elemental mercury in the troposphere. We find that the measured levels of bromine in the troposphere are sufficient to quickly oxidize mercury, which has significant implications for our understanding of atmospheric mercury processes.
Here we present a day of case study measurements of the vertical distribution of bromine...
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