Articles | Volume 23, issue 24
https://doi.org/10.5194/acp-23-15351-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-23-15351-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
15 Dec 2023
Research article |
| 15 Dec 2023
| 15 Dec 2023
In situ measurements of perturbations to stratospheric aerosol and modeled ozone and radiative impacts following the 2021 La Soufrière eruption
School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, United States
Corey Pedersen
School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, United States
John Dykema
School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, United States
Jean-Paul Vernier
NASA Langley Research Center, Hampton, Virginia 23666, USA
National Institute of Aerospace, Hampton, Virginia 23666, USA
Sandro Vattioni
Institute of Atmospheric and Climate Science, ETH Zürich, 8092 Zurich, Switzerland
Amit Kumar Pandit
National Institute of Aerospace, Hampton, Virginia 23666, USA
Andrea Stenke
Institute of Atmospheric and Climate Science, ETH Zürich, 8092 Zurich, Switzerland
Institute of Biogeochemistry and Pollutant Dynamics, ETH Zurich, 8092 Zurich, Switzerland
Eawag, Swiss Federal Institute of Aquatic Science and Technology, 8600 Dübendorf, Switzerland
Elizabeth Asher
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, Colorado 80309, USA
now at: Global Monitoring Laboratory, National Oceanic and Atmospheric Administration (NOAA), Boulder, Colorado 80309, USA
Troy Thornberry
Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration (NOAA), Boulder, Colorado 80309, USA
Michael A. Todt
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, Colorado 80309, USA
now at: Finnish Meteorological Institute (FMI), 00560 Helsinki, Finland
Thao Paul Bui
NASA Ames Research Center, Moffett Field, California 94043, USA
Jonathan Dean-Day
Bay Area Environmental Research Institute, Petaluma, California 94035, USA
Frank N. Keutsch
CORRESPONDING AUTHOR
School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, United States
Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, USA
Department of Earth and Planetary Sciences, Harvard University, Cambridge, Massachusetts 02138, USA
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Hazel Vernier, Neeraj Rastogi, Hongyu Liu, Amit Kumar Pandit, Kris Bedka, Anil Patel, Madineni Venkat Ratnam, Buduru Suneel Kumar, Bo Zhang, Harish Gadhavi, Frank Wienhold, Gwenael Berthet, and Jean-Paul Vernier
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Atmos. Chem. Phys., 22, 7105–7129, https://doi.org/10.5194/acp-22-7105-2022, https://doi.org/10.5194/acp-22-7105-2022, 2022
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Debra K. Weisenstein, Daniele Visioni, Henning Franke, Ulrike Niemeier, Sandro Vattioni, Gabriel Chiodo, Thomas Peter, and David W. Keith
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Dandan Wei, Hariprasad D. Alwe, Dylan B. Millet, Brandon Bottorff, Michelle Lew, Philip S. Stevens, Joshua D. Shutter, Joshua L. Cox, Frank N. Keutsch, Qianwen Shi, Sarah C. Kavassalis, Jennifer G. Murphy, Krystal T. Vasquez, Hannah M. Allen, Eric Praske, John D. Crounse, Paul O. Wennberg, Paul B. Shepson, Alexander A. T. Bui, Henry W. Wallace, Robert J. Griffin, Nathaniel W. May, Megan Connor, Jonathan H. Slade, Kerri A. Pratt, Ezra C. Wood, Mathew Rollings, Benjamin L. Deming, Daniel C. Anderson, and Allison L. Steiner
Geosci. Model Dev., 14, 6309–6329, https://doi.org/10.5194/gmd-14-6309-2021, https://doi.org/10.5194/gmd-14-6309-2021, 2021
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Timofei Sukhodolov, Tatiana Egorova, Andrea Stenke, William T. Ball, Christina Brodowsky, Gabriel Chiodo, Aryeh Feinberg, Marina Friedel, Arseniy Karagodin-Doyennel, Thomas Peter, Jan Sedlacek, Sandro Vattioni, and Eugene Rozanov
Geosci. Model Dev., 14, 5525–5560, https://doi.org/10.5194/gmd-14-5525-2021, https://doi.org/10.5194/gmd-14-5525-2021, 2021
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Eleni Dovrou, Kelvin H. Bates, Jean C. Rivera-Rios, Joshua L. Cox, Joshua D. Shutter, and Frank N. Keutsch
Atmos. Chem. Phys., 21, 8999–9008, https://doi.org/10.5194/acp-21-8999-2021, https://doi.org/10.5194/acp-21-8999-2021, 2021
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We examined the mechanism and products of oxidation of dissolved sulfur dioxide with the main isomers of isoprene hydroxyl hydroperoxides, via laboratory and model analysis. Two chemical mechanism pathways are proposed and the results provide an improved understanding of the broader atmospheric chemistry and role of multifunctional organic hydroperoxides, which should be the dominant VOC oxidation products under low-NO conditions, highlighting their significant contribution to sulfate formation.
Jack C. Hensley, Adam W. Birdsall, Gregory Valtierra, Joshua L. Cox, and Frank N. Keutsch
Atmos. Chem. Phys., 21, 8809–8821, https://doi.org/10.5194/acp-21-8809-2021, https://doi.org/10.5194/acp-21-8809-2021, 2021
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We measured reactions of butenedial, an atmospheric dicarbonyl, in aqueous mixtures that mimic the conditions of aerosol particles. Major reaction products and rates were determined to assess their atmospheric relevance and to compare against other well-studied dicarbonyls. We suggest that the structure of the carbon backbone, not just the dominant functional group, plays a major role in dicarbonyl reactivity, influencing the fate and ability of dicarbonyls to produce brown carbon.
Alexander Zaytsev, Martin Breitenlechner, Anna Novelli, Hendrik Fuchs, Daniel A. Knopf, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 14, 2501–2513, https://doi.org/10.5194/amt-14-2501-2021, https://doi.org/10.5194/amt-14-2501-2021, 2021
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We have developed an online method for speciated measurements of organic peroxy radicals and stabilized Criegee intermediates using chemical derivatization combined with chemical ionization mass spectrometry. Chemical derivatization prevents secondary radical reactions and eliminates potential interferences. Comparison between our measurements and results from numeric modeling shows that the method can be used for the quantification of a wide range of atmospheric radicals and intermediates.
Margot Clyne, Jean-Francois Lamarque, Michael J. Mills, Myriam Khodri, William Ball, Slimane Bekki, Sandip S. Dhomse, Nicolas Lebas, Graham Mann, Lauren Marshall, Ulrike Niemeier, Virginie Poulain, Alan Robock, Eugene Rozanov, Anja Schmidt, Andrea Stenke, Timofei Sukhodolov, Claudia Timmreck, Matthew Toohey, Fiona Tummon, Davide Zanchettin, Yunqian Zhu, and Owen B. Toon
Atmos. Chem. Phys., 21, 3317–3343, https://doi.org/10.5194/acp-21-3317-2021, https://doi.org/10.5194/acp-21-3317-2021, 2021
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This study finds how and why five state-of-the-art global climate models with interactive stratospheric aerosols differ when simulating the aftermath of large volcanic injections as part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP). We identify and explain the consequences of significant disparities in the underlying physics and chemistry currently in some of the models, which are problems likely not unique to the models participating in this study.
Michael Steiner, Beiping Luo, Thomas Peter, Michael C. Pitts, and Andrea Stenke
Geosci. Model Dev., 14, 935–959, https://doi.org/10.5194/gmd-14-935-2021, https://doi.org/10.5194/gmd-14-935-2021, 2021
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We evaluate polar stratospheric clouds (PSCs) as simulated by the chemistry–climate model (CCM) SOCOLv3.1 in comparison with measurements by the CALIPSO satellite. A cold bias results in an overestimated PSC area and mountain-wave ice is underestimated, but we find overall good temporal and spatial agreement of PSC occurrence and composition. This work confirms previous studies indicating that simplified PSC schemes may also achieve good approximations of the fundamental properties of PSCs.
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.
Martina Krämer, Christian Rolf, Nicole Spelten, Armin Afchine, David Fahey, Eric Jensen, Sergey Khaykin, Thomas Kuhn, Paul Lawson, Alexey Lykov, Laura L. Pan, Martin Riese, Andrew Rollins, Fred Stroh, Troy Thornberry, Veronika Wolf, Sarah Woods, Peter Spichtinger, Johannes Quaas, and Odran Sourdeval
Atmos. Chem. Phys., 20, 12569–12608, https://doi.org/10.5194/acp-20-12569-2020, https://doi.org/10.5194/acp-20-12569-2020, 2020
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To improve the representations of cirrus clouds in climate predictions, extended knowledge of their properties and geographical distribution is required. This study presents extensive airborne in situ and satellite remote sensing climatologies of cirrus and humidity, which serve as a guide to cirrus clouds. Further, exemplary radiative characteristics of cirrus types and also in situ observations of tropical tropopause layer cirrus and humidity in the Asian monsoon anticyclone are shown.
Lei Zhu, Gonzalo González Abad, Caroline R. Nowlan, Christopher Chan Miller, Kelly Chance, Eric C. Apel, Joshua P. DiGangi, Alan Fried, Thomas F. Hanisco, Rebecca S. Hornbrook, Lu Hu, Jennifer Kaiser, Frank N. Keutsch, Wade Permar, Jason M. St. Clair, and Glenn M. Wolfe
Atmos. Chem. Phys., 20, 12329–12345, https://doi.org/10.5194/acp-20-12329-2020, https://doi.org/10.5194/acp-20-12329-2020, 2020
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We develop a validation platform for satellite HCHO retrievals using in situ observations from 12 aircraft campaigns. The platform offers an alternative way to quickly assess systematic biases in HCHO satellite products over large domains and long periods, facilitating optimization of retrieval settings and the minimization of retrieval biases. Application to the NASA operational HCHO product indicates that relative biases range from −44.5 % to +112.1 % depending on locations and seasons.
William T. Ball, Gabriel Chiodo, Marta Abalos, Justin Alsing, and Andrea Stenke
Atmos. Chem. Phys., 20, 9737–9752, https://doi.org/10.5194/acp-20-9737-2020, https://doi.org/10.5194/acp-20-9737-2020, 2020
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Recent lower stratospheric ozone decreases remain unexplained. We show that chemistry–climate models are not generally able to reproduce mid-latitude ozone and water vapour changes. Our analysis of observations provides evidence that climate change may be responsible for the ozone trends. While model projections suggest that extratropical ozone should recover by 2100, our study raises questions about their efficacy in simulating lower stratospheric changes in this region.
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
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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.
Yan Zheng, Xi Cheng, Keren Liao, Yaowei Li, Yong Jie Li, Ru-Jin Huang, Weiwei Hu, Ying Liu, Tong Zhu, Shiyi Chen, Limin Zeng, Douglas R. Worsnop, and Qi Chen
Atmos. Meas. Tech., 13, 2457–2472, https://doi.org/10.5194/amt-13-2457-2020, https://doi.org/10.5194/amt-13-2457-2020, 2020
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This paper provides important information to help researchers to understand the mass quantification and source apportionment by Aerodyne aerosol mass spectrometers.
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.
Aryeh Feinberg, Moustapha Maliki, Andrea Stenke, Bruno Sudret, Thomas Peter, and Lenny H. E. Winkel
Atmos. Chem. Phys., 20, 1363–1390, https://doi.org/10.5194/acp-20-1363-2020, https://doi.org/10.5194/acp-20-1363-2020, 2020
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The amount of the micronutrient selenium in food largely depends on the amount and form of selenium in soil. The atmosphere acts as a source of selenium to soils through deposition, yet little information is available about atmospheric selenium cycling. Therefore, we built the first global atmospheric selenium model. Through sensitivity and uncertainty analysis we determine that selenium can be transported thousands of kilometers and that measurements of selenium emissions should be prioritized.
Abigail R. Koss, Manjula R. Canagaratna, Alexander Zaytsev, Jordan E. Krechmer, Martin Breitenlechner, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joseph R. Roscioli, Frank N. Keutsch, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 1021–1041, https://doi.org/10.5194/acp-20-1021-2020, https://doi.org/10.5194/acp-20-1021-2020, 2020
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Oxidation chemistry of organic compounds in the atmosphere produces a diverse spectrum of products. This diversity is difficult to represent in air quality and climate models, and in laboratory experiments it results in large and complex datasets. This work evaluates several methods to simplify the chemistry of oxidation systems in environmental chambers, including positive matrix factorization, hierarchical clustering analysis, and gamma kinetics parameterization.
Le Kuai, Kevin W. Bowman, Kazuyuki Miyazaki, Makoto Deushi, Laura Revell, Eugene Rozanov, Fabien Paulot, Sarah Strode, Andrew Conley, Jean-François Lamarque, Patrick Jöckel, David A. Plummer, Luke D. Oman, Helen Worden, Susan Kulawik, David Paynter, Andrea Stenke, and Markus Kunze
Atmos. Chem. Phys., 20, 281–301, https://doi.org/10.5194/acp-20-281-2020, https://doi.org/10.5194/acp-20-281-2020, 2020
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The tropospheric ozone increase from pre-industrial to the present day leads to a radiative forcing. The top-of-atmosphere outgoing fluxes at the ozone band are controlled by ozone, water vapor, and temperature. We demonstrate a method to attribute the models’ flux biases to these key players using satellite-constrained instantaneous radiative kernels. The largest spread between models is found in the tropics, mainly driven by ozone and then water vapor.
Alexander Zaytsev, Abigail R. Koss, Martin Breitenlechner, Jordan E. Krechmer, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joshua L. Cox, Joshua Moss, Joseph R. Roscioli, Manjula R. Canagaratna, Douglas R. Worsnop, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Chem. Phys., 19, 15117–15129, https://doi.org/10.5194/acp-19-15117-2019, https://doi.org/10.5194/acp-19-15117-2019, 2019
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Aromatic hydrocarbons contribute significantly to the production of tropospheric ozone and secondary organic aerosol (SOA). Here later-generation low-volatility oxygenated products from toluene and 1,2,4-TMB oxidation by OH are detected in the gas and particle phases. We show that these products, previously identified as highly oxygenated molecules (HOMs), are formed in more than one pathway with differing numbers of reaction steps with OH. They also make up a significant fraction of SOA.
Rupert Holzinger, W. Joe F. Acton, William J. Bloss, Martin Breitenlechner, Leigh R. Crilley, Sébastien Dusanter, Marc Gonin, Valerie Gros, Frank N. Keutsch, Astrid Kiendler-Scharr, Louisa J. Kramer, Jordan E. Krechmer, Baptiste Languille, Nadine Locoge, Felipe Lopez-Hilfiker, Dušan Materić, Sergi Moreno, Eiko Nemitz, Lauriane L. J. Quéléver, Roland Sarda Esteve, Stéphane Sauvage, Simon Schallhart, Roberto Sommariva, Ralf Tillmann, Sergej Wedel, David R. Worton, Kangming Xu, and Alexander Zaytsev
Atmos. Meas. Tech., 12, 6193–6208, https://doi.org/10.5194/amt-12-6193-2019, https://doi.org/10.5194/amt-12-6193-2019, 2019
Adam W. Birdsall, Jack C. Hensley, Paige S. Kotowitz, Andrew J. Huisman, and Frank N. Keutsch
Atmos. Chem. Phys., 19, 14195–14209, https://doi.org/10.5194/acp-19-14195-2019, https://doi.org/10.5194/acp-19-14195-2019, 2019
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We have measured the evaporation rates of butenedial, a four-carbon dialdehyde produced in the atmosphere, from individual levitated particles. Effective vapor pressures and Henry's law constants, which characterize the compound's gas-particle partitioning behavior, were determined. The important role of hydration reactions was observed under both dry and humid conditions, as well as a salting-out effect in the presence of sodium chloride or sodium sulfate.
Joshua D. Shutter, Norton T. Allen, Thomas F. Hanisco, Glenn M. Wolfe, Jason M. St. Clair, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 6079–6089, https://doi.org/10.5194/amt-12-6079-2019, https://doi.org/10.5194/amt-12-6079-2019, 2019
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A new mid-infrared and ultra-portable formaldehyde (HCHO) sensor from Aeris Technologies is characterized and evaluated against well-established laser-induced fluorescence (LIF) instrumentation. The Aeris sensor displays linear behavior (R squared > 0.94) and shows good agreement with LIF instruments. While the compact sensor is not currently a replacement for the most sensitive research-grade instrumentation available, its sub-ppbv precision is sufficient for indoor and outdoor HCHO monitoring.
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.
Eleni Dovrou, Christopher Y. Lim, Manjula R. Canagaratna, Jesse H. Kroll, Douglas R. Worsnop, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 5303–5315, https://doi.org/10.5194/amt-12-5303-2019, https://doi.org/10.5194/amt-12-5303-2019, 2019
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Measurement techniques commonly used to analyze particulate matter composition can result in the possible misidentification of sulfur-containing species, especially for the case of sulfate and hydroxymethanesulfonate (HMS). The efficiency and limitations of these techniques, along with a method that enables further studies of the contribution of sulfur-containing species, S(IV) versus S(VI), to particulate matter under low-light atmospheric conditions, are described in this work.
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.
Aryeh Feinberg, Timofei Sukhodolov, Bei-Ping Luo, Eugene Rozanov, Lenny H. E. Winkel, Thomas Peter, and Andrea Stenke
Geosci. Model Dev., 12, 3863–3887, https://doi.org/10.5194/gmd-12-3863-2019, https://doi.org/10.5194/gmd-12-3863-2019, 2019
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We have improved several aspects of atmospheric sulfur cycling in SOCOL-AER, an aerosol–chemistry–climate model. The newly implemented features in SOCOL-AERv2 include interactive deposition schemes, improved sulfur mass conservation, and expanded tropospheric chemistry. SOCOL-AERv2 shows better agreement with stratospheric aerosol observations and sulfur deposition networks compared to SOCOL-AERv1. SOCOL-AERv2 can be used to study impacts of sulfate aerosol on climate, chemistry, and ecosystems.
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.
Pavle Arsenovic, Alessandro Damiani, Eugene Rozanov, Bernd Funke, Andrea Stenke, and Thomas Peter
Atmos. Chem. Phys., 19, 9485–9494, https://doi.org/10.5194/acp-19-9485-2019, https://doi.org/10.5194/acp-19-9485-2019, 2019
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Low-energy electrons (LEE) are the dominant source of odd nitrogen, which destroys ozone, in the mesosphere and stratosphere in polar winter in the geomagnetically active periods. However, the observed stratospheric ozone anomalies can be reproduced only when accounting for both low- and middle-range energy electrons (MEE) in the chemistry-climate model. Ozone changes may induce further dynamical and thermal changes in the atmosphere. We recommend including both LEE and MEE in climate models.
Sabine Robrecht, Bärbel Vogel, Jens-Uwe Grooß, Karen Rosenlof, Troy Thornberry, Andrew Rollins, Martina Krämer, Lance Christensen, and Rolf Müller
Atmos. Chem. Phys., 19, 5805–5833, https://doi.org/10.5194/acp-19-5805-2019, https://doi.org/10.5194/acp-19-5805-2019, 2019
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The potential destruction of stratospheric ozone in the mid-latitudes has been discussed recently. We analysed this ozone loss mechanism and its sensitivities. In a certain temperature range, we found a threshold in water vapour, which has to be exceeded for ozone loss to occur. We show the dependence of this water vapour threshold on temperature, sulfate content and air composition. This study provides a basis to estimate the impact of potential sulphate geoengineering on stratospheric ozone.
Sandro Vattioni, Debra Weisenstein, David Keith, Aryeh Feinberg, Thomas Peter, and Andrea Stenke
Atmos. Chem. Phys., 19, 4877–4897, https://doi.org/10.5194/acp-19-4877-2019, https://doi.org/10.5194/acp-19-4877-2019, 2019
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This study is among the first modeling studies on stratospheric sulfate geoengineering that interactively couple a size-resolved sectional aerosol module to well-described stratospheric chemistry and radiation schemes in a global 3-D chemistry–climate model. We found that compared with SO2 injection, the direct emission of aerosols results in more effective radiative forcing and that sensitivities to different injection strategies vary for different forms of injected sulfur.
Alexander Zaytsev, Martin Breitenlechner, Abigail R. Koss, Christopher Y. Lim, James C. Rowe, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 1861–1870, https://doi.org/10.5194/amt-12-1861-2019, https://doi.org/10.5194/amt-12-1861-2019, 2019
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We present the development of a chemical ionization mass spectrometer which can be operated with either ammonium (NH4+) or hydronium (H3O+) as the reagent ion. We describe a mass spectrometric voltage scanning procedure based on collision-induced dissociation that allows us to determine the stability of detected ammonium–organic ions and hence constrain the sensitivity of the instrument to a wide range of organic compounds that cannot be calibrated directly.
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.
Stefan Kaufmann, Christiane Voigt, Romy Heller, Tina Jurkat-Witschas, Martina Krämer, Christian Rolf, Martin Zöger, Andreas Giez, Bernhard Buchholz, Volker Ebert, Troy Thornberry, and Ulrich Schumann
Atmos. Chem. Phys., 18, 16729–16745, https://doi.org/10.5194/acp-18-16729-2018, https://doi.org/10.5194/acp-18-16729-2018, 2018
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We present an intercomparison of the airborne water vapor measurements during the ML-CIRRUS mission. Although the agreement of the hygrometers significantly improved compared to studies from recent decades, systematic differences remain under specific meteorological conditions. We compare the measurements to model data, where we observe a model wet bias in the lower stratosphere close to the tropopause, likely caused by a blurred humidity gradient in the model tropopause.
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.
Azimeh Zare, Paul S. Romer, Tran Nguyen, Frank N. Keutsch, Kate Skog, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 15419–15436, https://doi.org/10.5194/acp-18-15419-2018, https://doi.org/10.5194/acp-18-15419-2018, 2018
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Organic nitrates play an important role in concentrations and distribution of NOx, ozone and aerosol as the most important air pollutants. We develop a state-of-the-science detailed chemical mechanism representing individual organic nitrates, which is appropriate to use in air quality models and results in a more accurate simulation of atmospheric chemistry. Using this mechanism we explore production and removal processes of organic nitrates in a rural environment that are poorly constrained.
Amanda C. Maycock, Katja Matthes, Susann Tegtmeier, Hauke Schmidt, Rémi Thiéblemont, Lon Hood, Hideharu Akiyoshi, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Oliver Kirner, Markus Kunze, Marion Marchand, Daniel R. Marsh, Martine Michou, David Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Yousuke Yamashita, and Kohei Yoshida
Atmos. Chem. Phys., 18, 11323–11343, https://doi.org/10.5194/acp-18-11323-2018, https://doi.org/10.5194/acp-18-11323-2018, 2018
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The 11-year solar cycle is an important driver of climate variability. Changes in incoming solar ultraviolet radiation affect atmospheric ozone, which in turn influences atmospheric temperatures. Constraining the impact of the solar cycle on ozone is therefore important for understanding climate variability. This study examines the representation of the solar influence on ozone in numerical models used to simulate past and future climate. We highlight important differences among model datasets.
Blanca Ayarzagüena, Lorenzo M. Polvani, Ulrike Langematz, Hideharu Akiyoshi, Slimane Bekki, Neal Butchart, Martin Dameris, Makoto Deushi, Steven C. Hardiman, Patrick Jöckel, Andrew Klekociuk, Marion Marchand, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke D. Oman, David A. Plummer, Laura Revell, Eugene Rozanov, David Saint-Martin, John Scinocca, Andrea Stenke, Kane Stone, Yousuke Yamashita, Kohei Yoshida, and Guang Zeng
Atmos. Chem. Phys., 18, 11277–11287, https://doi.org/10.5194/acp-18-11277-2018, https://doi.org/10.5194/acp-18-11277-2018, 2018
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Stratospheric sudden warmings (SSWs) are natural major disruptions of the polar stratospheric circulation that also affect surface weather. In the literature there are conflicting claims as to whether SSWs will change in the future. The confusion comes from studies using different models and methods. Here we settle the question by analysing 12 models with a consistent methodology, to show that no robust changes in frequency and other features are expected over the 21st century.
Timofei Sukhodolov, Jian-Xiong Sheng, Aryeh Feinberg, Bei-Ping Luo, Thomas Peter, Laura Revell, Andrea Stenke, Debra K. Weisenstein, and Eugene Rozanov
Geosci. Model Dev., 11, 2633–2647, https://doi.org/10.5194/gmd-11-2633-2018, https://doi.org/10.5194/gmd-11-2633-2018, 2018
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The Pinatubo eruption in 1991 is the strongest directly observed volcanic event. In a series of experiments, we simulate its influence on the stratospheric aerosol layer using a state-of-the-art aerosol–chemistry–climate model, SOCOL-AERv1.0, and compare our results to observations. We show that SOCOL-AER reproduces the most important atmospheric effects and can therefore be used to study the climate effects of future volcanic eruptions and geoengineering by artificial sulfate aerosol.
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.
Hendrik Fuchs, Sascha Albrecht, Ismail–Hakki Acir, Birger Bohn, Martin Breitenlechner, Hans-Peter Dorn, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, Martin Kaminski, Frank N. Keutsch, Anna Novelli, David Reimer, Franz Rohrer, Ralf Tillmann, Luc Vereecken, Robert Wegener, Alexander Zaytsev, Astrid Kiendler-Scharr, and Andreas Wahner
Atmos. Chem. Phys., 18, 8001–8016, https://doi.org/10.5194/acp-18-8001-2018, https://doi.org/10.5194/acp-18-8001-2018, 2018
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The photooxidation of methyl vinyl ketone MVK, one of the most important products of isoprene that is emitted by plants, was investigated in the atmospheric simulation chamber SAPHIR for conditions found in forested areas. The comparison of measured trace gas time series with model calculations shows a gap in the understanding of radical chemistry in the MVK oxidation scheme. The possibility of unimolecular isomerization reactions were investigated by means of quantum-chemical calculations.
Shouming Zhou, Jean C. Rivera-Rios, Frank N. Keutsch, and Jonathan P. D. Abbatt
Atmos. Meas. Tech., 11, 3081–3089, https://doi.org/10.5194/amt-11-3081-2018, https://doi.org/10.5194/amt-11-3081-2018, 2018
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.
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
Pavle Arsenovic, Eugene Rozanov, Julien Anet, Andrea Stenke, Werner Schmutz, and Thomas Peter
Atmos. Chem. Phys., 18, 3469–3483, https://doi.org/10.5194/acp-18-3469-2018, https://doi.org/10.5194/acp-18-3469-2018, 2018
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Global warming will persist in the 21st century, even if the solar activity undergoes an unusually strong and long decline. Decreased ozone production caused by reduction of solar activity and change of atmospheric dynamics due to the global warming might result in further thinning of the tropical ozone layer. Globally, total ozone would not recover to the pre-ozone hole values as long as the decline of solar activity lasts. This may let more ultra-violet radiation reach the Earth's surface.
Lauren Marshall, Anja Schmidt, Matthew Toohey, Ken S. Carslaw, Graham W. Mann, Michael Sigl, Myriam Khodri, Claudia Timmreck, Davide Zanchettin, William T. Ball, Slimane Bekki, James S. A. Brooke, Sandip Dhomse, Colin Johnson, Jean-Francois Lamarque, Allegra N. LeGrande, Michael J. Mills, Ulrike Niemeier, James O. Pope, Virginie Poulain, Alan Robock, Eugene Rozanov, Andrea Stenke, Timofei Sukhodolov, Simone Tilmes, Kostas Tsigaridis, and Fiona Tummon
Atmos. Chem. Phys., 18, 2307–2328, https://doi.org/10.5194/acp-18-2307-2018, https://doi.org/10.5194/acp-18-2307-2018, 2018
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We use four global aerosol models to compare the simulated sulfate deposition from the 1815 Mt. Tambora eruption to ice core records. Inter-model volcanic sulfate deposition differs considerably. Volcanic sulfate deposited on polar ice sheets is used to estimate the atmospheric sulfate burden and subsequently radiative forcing of historic eruptions. Our results suggest that deriving such relationships from model simulations may be associated with greater uncertainties than previously thought.
William T. Ball, Justin Alsing, Daniel J. Mortlock, Johannes Staehelin, Joanna D. Haigh, Thomas Peter, Fiona Tummon, Rene Stübi, Andrea Stenke, John Anderson, Adam Bourassa, Sean M. Davis, Doug Degenstein, Stacey Frith, Lucien Froidevaux, Chris Roth, Viktoria Sofieva, Ray Wang, Jeannette Wild, Pengfei Yu, Jerald R. Ziemke, and Eugene V. Rozanov
Atmos. Chem. Phys., 18, 1379–1394, https://doi.org/10.5194/acp-18-1379-2018, https://doi.org/10.5194/acp-18-1379-2018, 2018
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Using a robust analysis, with artefact-corrected ozone data, we confirm upper stratospheric ozone is recovering following the Montreal Protocol, but that lower stratospheric ozone (50° S–50° N) has continued to decrease since 1998, and the ozone layer as a whole (60° S–60° N) may be lower today than in 1998. No change in total column ozone may be due to increasing tropospheric ozone. State-of-the-art models do not reproduce lower stratospheric ozone decreases.
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.
Adam W. Birdsall, Ulrich K. Krieger, and Frank N. Keutsch
Atmos. Meas. Tech., 11, 33–47, https://doi.org/10.5194/amt-11-33-2018, https://doi.org/10.5194/amt-11-33-2018, 2018
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We have developed a laboratory system that provides mass spectra of individual particles, roughly 20 microns in diameter, after they have been levitated in an electric field. Measured evaporation of polyethylene glycol particles was found to agree with a kinetic model. The system can be used to study fundamental chemical and physical processes involving particles that are difficult to isolate and study with other techniques, and hence improve our understanding of atmospheric particles.
Laura E. Revell, Andrea Stenke, Beiping Luo, Stefanie Kremser, Eugene Rozanov, Timofei Sukhodolov, and Thomas Peter
Atmos. Chem. Phys., 17, 13139–13150, https://doi.org/10.5194/acp-17-13139-2017, https://doi.org/10.5194/acp-17-13139-2017, 2017
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Compiling stratospheric aerosol data sets after a major volcanic eruption is difficult as the stratosphere becomes too optically opaque for satellite instruments to measure accurately. We performed ensemble chemistry–climate model simulations with two stratospheric aerosol data sets compiled for two international modelling activities and compared the simulated volcanic aerosol-induced effects from the 1991 Mt Pinatubo eruption on tropical stratospheric temperature and ozone with observations.
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.
Abigail Koss, Bin Yuan, Carsten Warneke, Jessica B. Gilman, Brian M. Lerner, Patrick R. Veres, Jeff Peischl, Scott Eilerman, Rob Wild, Steven S. Brown, Chelsea R. Thompson, Thomas Ryerson, Thomas Hanisco, Glenn M. Wolfe, Jason M. St. Clair, Mitchell Thayer, Frank N. Keutsch, Shane Murphy, and Joost de Gouw
Atmos. Meas. Tech., 10, 2941–2968, https://doi.org/10.5194/amt-10-2941-2017, https://doi.org/10.5194/amt-10-2941-2017, 2017
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Oil and gas extraction activity can cause air quality issues through emission of reactive chemicals. VOCs related to extraction operations in the United States were measured by PTR-ToF-MS from aircraft during the SONGNEX campaign in March–April 2015. The detailed analysis in this work provides a guide to interpreting PTR-ToF measurements in oil- and gas-producing regions, and it includes fundamental observations of VOC speciation and mixing ratios.
Christopher Chan Miller, Daniel J. Jacob, Eloise A. Marais, Karen Yu, Katherine R. Travis, Patrick S. Kim, Jenny A. Fisher, Lei Zhu, Glenn M. Wolfe, Thomas F. Hanisco, Frank N. Keutsch, Jennifer Kaiser, Kyung-Eun Min, Steven S. Brown, Rebecca A. Washenfelder, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 17, 8725–8738, https://doi.org/10.5194/acp-17-8725-2017, https://doi.org/10.5194/acp-17-8725-2017, 2017
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The use of satellite glyoxal observations for estimating isoprene emissions has been limited by knowledge of the glyoxal yield from isoprene. We use SENEX aircraft observations over the southeast US to evaluate glyoxal yields from isoprene in a 3-D atmospheric model. The SENEX observations support a pathway for glyoxal formation in pristine regions that we propose here, which may have implications for improving isoprene emissions estimates from upcoming high-resolution geostationary satellites.
Anne-Kathrin Bernhammer, Martin Breitenlechner, Frank N. Keutsch, and Armin Hansel
Atmos. Chem. Phys., 17, 4053–4062, https://doi.org/10.5194/acp-17-4053-2017, https://doi.org/10.5194/acp-17-4053-2017, 2017
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Isoprene is the predominant non-methane compound emitted by the biosphere. In the atmosphere oxidation by OH under low NOx produces isoprene hydroxy hydroperoxides (ISOPOOHs). This work has found an effective conversion of ISOPOOHs to volatile carbonyls on metal environmental simulation chamber walls. Likely catalyzed decomposition reactions also occur for other hydroxyl hydroperoxides on metal surfaces.
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.
Anusha P. S. Hettiyadura, Thilina Jayarathne, Karsten Baumann, Allen H. Goldstein, Joost A. de Gouw, Abigail Koss, Frank N. Keutsch, Kate Skog, and Elizabeth A. Stone
Atmos. Chem. Phys., 17, 1343–1359, https://doi.org/10.5194/acp-17-1343-2017, https://doi.org/10.5194/acp-17-1343-2017, 2017
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Organosulfates are components of secondary organic aerosol (SOA) formed in the presence of sulfate. Herein, their abundance, identity, and potential to form as sampling artifacts were studied in Centreville, AL, USA. The 10 most abundant signals accounted for 58–78 % of the total, with at least 20–200 other species accounting for the remainder. These major species were largely associated with biogenic gases, like isoprene and monoterpenes, and are proposed targets for future standard development.
Bodo Werner, Jochen Stutz, Max Spolaor, Lisa Scalone, Rasmus Raecke, James Festa, Santo Fedele Colosimo, Ross Cheung, Catalina Tsai, Ryan Hossaini, Martyn P. Chipperfield, Giorgio S. Taverna, Wuhu Feng, James W. Elkins, David W. Fahey, Ru-Shan Gao, Erik J. Hintsa, Troy D. Thornberry, Free Lee Moore, Maria A. Navarro, Elliot Atlas, Bruce C. Daube, Jasna Pittman, Steve Wofsy, and Klaus Pfeilsticker
Atmos. Chem. Phys., 17, 1161–1186, https://doi.org/10.5194/acp-17-1161-2017, https://doi.org/10.5194/acp-17-1161-2017, 2017
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The paper reports on inorganic and organic bromine measured in the tropical tropopause layer (TTL) over the eastern Pacific in early 2013. Bryinorg is found to increase from a mean of 2.63 ± 1.04 ppt for θ in the range of 350–360 K to 5.11 ± 1.57 ppt for θ=390 ± 400 K, whereas in the subtropical lower stratosphere, it reaches 7.66 ± 2.95 ppt for θ in the range of 390–400 K. Within the TTL, total bromine is found to range from 20.3 ppt to 22.3 ppt.
Emma L. D'Ambro, Ben H. Lee, Jiumeng Liu, John E. Shilling, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Siegfried Schobesberger, Rahul A. Zaveri, Claudia Mohr, Anna Lutz, Zhenfa Zhang, Avram Gold, Jason D. Surratt, Jean C. Rivera-Rios, Frank N. Keutsch, and Joel A. Thornton
Atmos. Chem. Phys., 17, 159–174, https://doi.org/10.5194/acp-17-159-2017, https://doi.org/10.5194/acp-17-159-2017, 2017
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We studied the formation and properties of secondary organic aerosol produced from isoprene. We find that a significant fraction (~50 %) of the mass is composed of low-volatility, highly oxidized compounds such as C5H12O6. A significant fraction of the remainder appears to be in the form of oligomeric material. Adding NOx maintained or decreased SOA yields while increasing the fraction of low-volatility material, possibly due to oligomers.
William T. Ball, Aleš Kuchař, Eugene V. Rozanov, Johannes Staehelin, Fiona Tummon, Anne K. Smith, Timofei Sukhodolov, Andrea Stenke, Laura Revell, Ancelin Coulon, Werner Schmutz, and Thomas Peter
Atmos. Chem. Phys., 16, 15485–15500, https://doi.org/10.5194/acp-16-15485-2016, https://doi.org/10.5194/acp-16-15485-2016, 2016
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We find monthly, mid-latitude temperature changes above 40 km are related to ozone and temperature variations throughout the middle atmosphere. We develop an index to represent this atmospheric variability. In statistical analysis, the index can account for up to 60 % of variability in tropical temperature and ozone above 27 km. The uncertainties can be reduced by up to 35 % and 20 % in temperature and ozone, respectively. This index is an important tool to quantify current and future ozone recovery.
Laura E. Revell, Andrea Stenke, Eugene Rozanov, William Ball, Stefan Lossow, and Thomas Peter
Atmos. Chem. Phys., 16, 13067–13080, https://doi.org/10.5194/acp-16-13067-2016, https://doi.org/10.5194/acp-16-13067-2016, 2016
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Water vapour in the stratosphere plays an important role in atmospheric chemistry and the Earth's radiative balance. We have analysed trends in stratospheric water vapour through the 21st century as simulated by a coupled chemistry–climate model following a range of greenhouse gas emission scenarios. We have also quantified the contribution that methane oxidation in the stratosphere makes to projected water vapour trends.
Andrew W. Rollins, Troy D. Thornberry, Steven J. Ciciora, Richard J. McLaughlin, Laurel A. Watts, Thomas F. Hanisco, Esther Baumann, Fabrizio R. Giorgetta, Thaopaul V. Bui, David W. Fahey, and Ru-Shan Gao
Atmos. Meas. Tech., 9, 4601–4613, https://doi.org/10.5194/amt-9-4601-2016, https://doi.org/10.5194/amt-9-4601-2016, 2016
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In situ measurements of SO2 in the tropical UT–LS have been scarce, in part due to limitations of existing instrumentation. Here we present a new laser-induced fluorescence instrument capable of measuring SO2 in the UT–LS region at single part-per-trillion (ppt) mixing ratios and demonstrate it on the NASA WB-57F aircraft up to 19.7 km altitude.
Jason M. St. Clair, Jean C. Rivera-Rios, John D. Crounse, Eric Praske, Michelle J. Kim, Glenn M. Wolfe, Frank N. Keutsch, Paul O. Wennberg, and Thomas F. Hanisco
Atmos. Meas. Tech., 9, 4561–4568, https://doi.org/10.5194/amt-9-4561-2016, https://doi.org/10.5194/amt-9-4561-2016, 2016
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Global isoprene emissions are the largest source of atmospheric non-methane hydrocarbons. Lab results show that ISOPOOH, a low-NOx isoprene oxidation product, can decompose on instrument surfaces to form high-NOx isoprene oxidation products, causing misinterpretation of oxidation conditions. This study investigated the potential formaldehyde artifact from ISOPOOH for the NASA ISAF instrument, and found that it does not significantly affect the accuracy of the ISAF field measurements.
Davide Zanchettin, Myriam Khodri, Claudia Timmreck, Matthew Toohey, Anja Schmidt, Edwin P. Gerber, Gabriele Hegerl, Alan Robock, Francesco S. R. Pausata, William T. Ball, Susanne E. Bauer, Slimane Bekki, Sandip S. Dhomse, Allegra N. LeGrande, Graham W. Mann, Lauren Marshall, Michael Mills, Marion Marchand, Ulrike Niemeier, Virginie Poulain, Eugene Rozanov, Angelo Rubino, Andrea Stenke, Kostas Tsigaridis, and Fiona Tummon
Geosci. Model Dev., 9, 2701–2719, https://doi.org/10.5194/gmd-9-2701-2016, https://doi.org/10.5194/gmd-9-2701-2016, 2016
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Simulating volcanically-forced climate variability is a challenging task for climate models. The Model Intercomparison Project on the climatic response to volcanic forcing (VolMIP) – an endorsed contribution to CMIP6 – defines a protocol for idealized volcanic-perturbation experiments to improve comparability of results across different climate models. This paper illustrates the design of VolMIP's experiments and describes the aerosol forcing input datasets to be used.
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.
Carsten Warneke, Michael Trainer, Joost A. de Gouw, David D. Parrish, David W. Fahey, A. R. Ravishankara, Ann M. Middlebrook, Charles A. Brock, James M. Roberts, Steven S. Brown, Jonathan A. Neuman, Brian M. Lerner, Daniel Lack, Daniel Law, Gerhard Hübler, Iliana Pollack, Steven Sjostedt, Thomas B. Ryerson, Jessica B. Gilman, Jin Liao, John Holloway, Jeff Peischl, John B. Nowak, Kenneth C. Aikin, Kyung-Eun Min, Rebecca A. Washenfelder, Martin G. Graus, Mathew Richardson, Milos Z. Markovic, Nick L. Wagner, André Welti, Patrick R. Veres, Peter Edwards, Joshua P. Schwarz, Timothy Gordon, William P. Dube, Stuart A. McKeen, Jerome Brioude, Ravan Ahmadov, Aikaterini Bougiatioti, Jack J. Lin, Athanasios Nenes, Glenn M. Wolfe, Thomas F. Hanisco, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Frank N. Keutsch, Jennifer Kaiser, Jingqiu Mao, and Courtney D. Hatch
Atmos. Meas. Tech., 9, 3063–3093, https://doi.org/10.5194/amt-9-3063-2016, https://doi.org/10.5194/amt-9-3063-2016, 2016
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In this paper we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign, which was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants.
During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN. The SENEX flights included day- and nighttime flights in the Southeast as well as flights over areas with intense shale gas extraction.
Amy P. Sullivan, Natasha Hodas, Barbara J. Turpin, Kate Skog, Frank N. Keutsch, Stefania Gilardoni, Marco Paglione, Matteo Rinaldi, Stefano Decesari, Maria Cristina Facchini, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Eiko Nemitz, Marsailidh M. Twigg, and Jeffrey L. Collett Jr.
Atmos. Chem. Phys., 16, 8095–8108, https://doi.org/10.5194/acp-16-8095-2016, https://doi.org/10.5194/acp-16-8095-2016, 2016
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This paper presents the results from our measurements and approach for the investigation of aqueous secondary organic aerosol (aqSOA) formation in the ambient atmosphere. When local aqSOA formation was observed, a correlation of water-soluble organic carbon with organic aerosol, aerosol liquid water, relative humidity, and aerosol nitrate was found. Key factors of local aqSOA production include air mass stagnation, formation of local nitrate overnight, and significant amounts of ammonia.
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
Markus Müller, Bruce E. Anderson, Andreas J. Beyersdorf, James H. Crawford, Glenn S. Diskin, Philipp Eichler, Alan Fried, Frank N. Keutsch, Tomas Mikoviny, Kenneth L. Thornhill, James G. Walega, Andrew J. Weinheimer, Melissa Yang, Robert J. Yokelson, and Armin Wisthaler
Atmos. Chem. Phys., 16, 3813–3824, https://doi.org/10.5194/acp-16-3813-2016, https://doi.org/10.5194/acp-16-3813-2016, 2016
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Atmospheric emissions from small forest fires and their impact on regional air quality are still poorly characterized. We used an instrumented NASA P-3B aircraft to study emissions from a small forest understory fire in Georgia (USA) and to investigate chemical transformations in the fire plume in the 1 h downwind region. A state-of-the-art chemical model was able to accurately simulate key chemical processes in the aging plume.
Stefan Kaufmann, Christiane Voigt, Tina Jurkat, Troy Thornberry, David W. Fahey, Ru-Shan Gao, Romy Schlage, Dominik Schäuble, and Martin Zöger
Atmos. Meas. Tech., 9, 939–953, https://doi.org/10.5194/amt-9-939-2016, https://doi.org/10.5194/amt-9-939-2016, 2016
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We present the development of a new airborne mass spectrometer AIMS-H2O for the fast and accurate measurement of water vapor in the upper troposphere and lower stratosphere. The high accuracy needed for e.g. quantification of atmospheric water vapor transport processes or cloud formation is achieved by an in-flight calibration of the instrument. AIMS-H2O is deployed on the DLR research aircraft HALO and Falcon where it covers a range of water vapor mixing ratios from 1 to 500 ppmv.
G. M. Wolfe, J. Kaiser, T. F. Hanisco, F. N. Keutsch, J. A. de Gouw, J. B. Gilman, M. Graus, C. D. Hatch, J. Holloway, L. W. Horowitz, B. H. Lee, B. M. Lerner, F. Lopez-Hilifiker, J. Mao, M. R. Marvin, J. Peischl, I. B. Pollack, J. M. Roberts, T. B. Ryerson, J. A. Thornton, P. R. Veres, and C. Warneke
Atmos. Chem. Phys., 16, 2597–2610, https://doi.org/10.5194/acp-16-2597-2016, https://doi.org/10.5194/acp-16-2597-2016, 2016
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This study uses airborne trace gas observations acquired over the southeast US to examine how both natural (isoprene) and anthropogenic (NOx) emissions influence the production of formaldehyde (HCHO). We find a 3-fold increase in HCHO yield between rural and polluted environments. State-of-the-science chemical mechanisms are generally able to reproduce this behavior. These results add confidence to global hydrocarbon emission inventories constrained by spaceborne HCHO observations.
A. K. Pandit, H. S. Gadhavi, M. Venkat Ratnam, K. Raghunath, S. V. B. Rao, and A. Jayaraman
Atmos. Chem. Phys., 15, 13833–13848, https://doi.org/10.5194/acp-15-13833-2015, https://doi.org/10.5194/acp-15-13833-2015, 2015
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We present the longest (1998 to 2013) cirrus cloud climatology over a tropical station using a ground-based lidar. A statistically significant increase is found in the altitude of sub-visible cirrus clouds. Also a systematic shift from thin to sub-visible cirrus cloud type is observed. Ground-based lidar is found to detect more number of sub-visible cirrus clouds than space-based lidar. These findings have implications to global warming and stratosphere-troposphere water vapour exchange studies.
D. K. Weisenstein, D. W. Keith, and J. A. Dykema
Atmos. Chem. Phys., 15, 11835–11859, https://doi.org/10.5194/acp-15-11835-2015, https://doi.org/10.5194/acp-15-11835-2015, 2015
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We investigate stratospheric aerosol geoengineering with solid particle injection by modeling the fractal structure of alumina aerosols and their interaction with background sulfate. We analyze the efficacy (W m^-2 of radiative forcing per megaton of injection) and risks (ozone loss, s) for both alumina and diamond particles as a function of injected monomer radius, finding 240nm alumina and 160nm diamond optimal. We discuss the limitations of our 2-D model study and associated uncertainties.
J. Meyer, C. Rolf, C. Schiller, S. Rohs, N. Spelten, A. Afchine, M. Zöger, N. Sitnikov, T. D. Thornberry, A. W. Rollins, Z. Bozóki, D. Tátrai, V. Ebert, B. Kühnreich, P. Mackrodt, O. Möhler, H. Saathoff, K. H. Rosenlof, and M. Krämer
Atmos. Chem. Phys., 15, 8521–8538, https://doi.org/10.5194/acp-15-8521-2015, https://doi.org/10.5194/acp-15-8521-2015, 2015
J. Kaiser, G. M. Wolfe, K. E. Min, S. S. Brown, C. C. Miller, D. J. Jacob, J. A. deGouw, M. Graus, T. F. Hanisco, J. Holloway, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, R. A. Washenfelder, and F. N. Keutsch
Atmos. Chem. Phys., 15, 7571–7583, https://doi.org/10.5194/acp-15-7571-2015, https://doi.org/10.5194/acp-15-7571-2015, 2015
L. E. Revell, F. Tummon, A. Stenke, T. Sukhodolov, A. Coulon, E. Rozanov, H. Garny, V. Grewe, and T. Peter
Atmos. Chem. Phys., 15, 5887–5902, https://doi.org/10.5194/acp-15-5887-2015, https://doi.org/10.5194/acp-15-5887-2015, 2015
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We have examined the effects of ozone precursor emissions and climate change on the tropospheric ozone budget. Under RCP 6.0, ozone in the future is governed primarily by changes in nitrogen oxides (NOx). Methane is also important, and induces an increase in tropospheric ozone that is approximately one-third of that caused by NOx. This study highlights the critical role that emission policies globally have to play in determining tropospheric ozone evolution through the 21st century.
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.
B. C. Kindel, P. Pilewskie, K. S. Schmidt, T. Thornberry, A. Rollins, and T. Bui
Atmos. Meas. Tech., 8, 1147–1156, https://doi.org/10.5194/amt-8-1147-2015, https://doi.org/10.5194/amt-8-1147-2015, 2015
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Measurements of upper tropospheric-lower stratospheric water vapor amounts in the tropics were made using the 1400 and 1900nm water vapor bands present in airborne solar spectral irradiance data. These were validated with radiative transfer modeling using in situ profiles of water vapor, temperature, and pressure. An approach to extending these types of measurements from aircraft altitudes to the top of the atmosphere to infer stratospheric water vapor amount is outlined.
J. Kaiser, G. M. Wolfe, B. Bohn, S. Broch, H. Fuchs, L. N. Ganzeveld, S. Gomm, R. Häseler, A. Hofzumahaus, F. Holland, J. Jäger, X. Li, I. Lohse, K. Lu, A. S. H. Prévôt, F. Rohrer, R. Wegener, R. Wolf, T. F. Mentel, A. Kiendler-Scharr, A. Wahner, and F. N. Keutsch
Atmos. Chem. Phys., 15, 1289–1298, https://doi.org/10.5194/acp-15-1289-2015, https://doi.org/10.5194/acp-15-1289-2015, 2015
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Using measurements acquired from a Zeppelin airship during the PEGASOS 2012 campaign, we show that VOC oxidation alone cannot account for the formaldehyde concentrations observed in the morning over rural Italy. Vertical profiles suggest a ground-level source of HCHO. Incorporating this additional HCHO source into a photochemical model increases calculated O3 production by as much as 12%.
T. D. Thornberry, A. W. Rollins, R. S. Gao, L. A. Watts, S. J. Ciciora, R. J. McLaughlin, and D. W. Fahey
Atmos. Meas. Tech., 8, 211–224, https://doi.org/10.5194/amt-8-211-2015, https://doi.org/10.5194/amt-8-211-2015, 2015
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The two-channel NOAA Water instrument was developed for in situ measurement of water vapor and cirrus cloud ice water content (IWC) in the upper troposphere and lower stratosphere. Tunable diode laser absorption is used to achieve accurate measurements at part per million H2O and low µg/m3 IWC. This paper reports the instrument’s design and performance achieved during its first aircraft deployment on the NASA Global Hawk during the 2013 ATTREX mission in the tropical tropopause layer.
T. B. Nguyen, J. D. Crounse, R. H. Schwantes, A. P. Teng, K. H. Bates, X. Zhang, J. M. St. Clair, W. H. Brune, G. S. Tyndall, F. N. Keutsch, J. H. Seinfeld, and P. O. Wennberg
Atmos. Chem. Phys., 14, 13531–13549, https://doi.org/10.5194/acp-14-13531-2014, https://doi.org/10.5194/acp-14-13531-2014, 2014
S. Muthers, J. G. Anet, A. Stenke, C. C. Raible, E. Rozanov, S. Brönnimann, T. Peter, F. X. Arfeuille, A. I. Shapiro, J. Beer, F. Steinhilber, Y. Brugnara, and W. Schmutz
Geosci. Model Dev., 7, 2157–2179, https://doi.org/10.5194/gmd-7-2157-2014, https://doi.org/10.5194/gmd-7-2157-2014, 2014
J. Ortega, A. Turnipseed, A. B. Guenther, T. G. Karl, D. A. Day, D. Gochis, J. A. Huffman, A. J. Prenni, E. J. T. Levin, S. M. Kreidenweis, P. J. DeMott, Y. Tobo, E. G. Patton, A. Hodzic, Y. Y. Cui, P. C. Harley, R. S. Hornbrook, E. C. Apel, R. K. Monson, A. S. D. Eller, J. P. Greenberg, M. C. Barth, P. Campuzano-Jost, B. B. Palm, J. L. Jimenez, A. C. Aiken, M. K. Dubey, C. Geron, J. Offenberg, M. G. Ryan, P. J. Fornwalt, S. C. Pryor, F. N. Keutsch, J. P. DiGangi, A. W. H. Chan, A. H. Goldstein, G. M. Wolfe, S. Kim, L. Kaser, R. Schnitzhofer, A. Hansel, C. A. Cantrell, R. L. Mauldin, and J. N. Smith
Atmos. Chem. Phys., 14, 6345–6367, https://doi.org/10.5194/acp-14-6345-2014, https://doi.org/10.5194/acp-14-6345-2014, 2014
J. Kaiser, X. Li, R. Tillmann, I. Acir, F. Holland, F. Rohrer, R. Wegener, and F. N. Keutsch
Atmos. Meas. Tech., 7, 1571–1580, https://doi.org/10.5194/amt-7-1571-2014, https://doi.org/10.5194/amt-7-1571-2014, 2014
G. M. Wolfe, C. Cantrell, S. Kim, R. L. Mauldin III, T. Karl, P. Harley, A. Turnipseed, W. Zheng, F. Flocke, E. C. Apel, R. S. Hornbrook, S. R. Hall, K. Ullmann, S. B. Henry, J. P. DiGangi, E. S. Boyle, L. Kaser, R. Schnitzhofer, A. Hansel, M. Graus, Y. Nakashima, Y. Kajii, A. Guenther, and F. N. Keutsch
Atmos. Chem. Phys., 14, 4715–4732, https://doi.org/10.5194/acp-14-4715-2014, https://doi.org/10.5194/acp-14-4715-2014, 2014
J. G. Anet, S. Muthers, E. V. Rozanov, C. C. Raible, A. Stenke, A. I. Shapiro, S. Brönnimann, F. Arfeuille, Y. Brugnara, J. Beer, F. Steinhilber, W. Schmutz, and T. Peter
Clim. Past, 10, 921–938, https://doi.org/10.5194/cp-10-921-2014, https://doi.org/10.5194/cp-10-921-2014, 2014
L. Kaser, T. Karl, A. Guenther, M. Graus, R. Schnitzhofer, A. Turnipseed, L. Fischer, P. Harley, M. Madronich, D. Gochis, F. N. Keutsch, and A. Hansel
Atmos. Chem. Phys., 13, 11935–11947, https://doi.org/10.5194/acp-13-11935-2013, https://doi.org/10.5194/acp-13-11935-2013, 2013
J. G. Anet, S. Muthers, E. Rozanov, C. C. Raible, T. Peter, A. Stenke, A. I. Shapiro, J. Beer, F. Steinhilber, S. Brönnimann, F. Arfeuille, Y. Brugnara, and W. Schmutz
Atmos. Chem. Phys., 13, 10951–10967, https://doi.org/10.5194/acp-13-10951-2013, https://doi.org/10.5194/acp-13-10951-2013, 2013
A. Stenke, C. R. Hoyle, B. Luo, E. Rozanov, J. Gröbner, L. Maag, S. Brönnimann, and T. Peter
Atmos. Chem. Phys., 13, 9713–9729, https://doi.org/10.5194/acp-13-9713-2013, https://doi.org/10.5194/acp-13-9713-2013, 2013
A. Stenke, M. Schraner, E. Rozanov, T. Egorova, B. Luo, and T. Peter
Geosci. Model Dev., 6, 1407–1427, https://doi.org/10.5194/gmd-6-1407-2013, https://doi.org/10.5194/gmd-6-1407-2013, 2013
T. D. Thornberry, A. W. Rollins, R. S. Gao, L. A. Watts, S. J. Ciciora, R. J. McLaughlin, C. Voigt, B. Hall, and D. W. Fahey
Atmos. Meas. Tech., 6, 1461–1475, https://doi.org/10.5194/amt-6-1461-2013, https://doi.org/10.5194/amt-6-1461-2013, 2013
S. Kundu, T. A. Quraishi, G. Yu, C. Suarez, F. N. Keutsch, and E. A. Stone
Atmos. Chem. Phys., 13, 4865–4875, https://doi.org/10.5194/acp-13-4865-2013, https://doi.org/10.5194/acp-13-4865-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Field Measurements | Altitude Range: Stratosphere | Science Focus: Chemistry (chemical composition and reactions)
Characterization of refractory aerosol particles collected in the tropical upper troposphere–lower stratosphere (UTLS) within the Asian tropopause aerosol layer (ATAL)
Enhanced sulfur in the upper troposphere and lower stratosphere in spring 2020
Chemical analysis of the Asian tropopause aerosol layer (ATAL) with emphasis on secondary aerosol particles using aircraft-based in situ aerosol mass spectrometry
Ozone depletion in the Arctic and Antarctic stratosphere induced by wildfire smoke
In situ observation of new particle formation (NPF) in the tropical tropopause layer of the 2017 Asian monsoon anticyclone – Part 2: NPF inside ice clouds
Lower-stratospheric aerosol measurements in eastward-shedding vortices over Japan from the Asian summer monsoon anticyclone during the summer of 2018
Aircraft-based observation of meteoric material in lower-stratospheric aerosol particles between 15 and 68° N
Sub-micrometer refractory carbonaceous particles in the polar stratosphere
Chemical analysis of refractory stratospheric aerosol particles collected within the arctic vortex and inside polar stratospheric clouds
Martin Ebert, Ralf Weigel, Stephan Weinbruch, Lisa Schneider, Konrad Kandler, Stefan Lauterbach, Franziska Köllner, Felix Plöger, Gebhard Günther, Bärbel Vogel, and Stephan Borrmann
Atmos. Chem. Phys., 24, 4771–4788, https://doi.org/10.5194/acp-24-4771-2024, https://doi.org/10.5194/acp-24-4771-2024, 2024
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Particles were collected during the flight campaign StratoClim 2017 within the Asian tropopause aerosol layer (ATAL). Refractory particles from seven different flights were characterized by scanning and transmission electron microscopy (SEM, TEM). The most abundant refractory particles are silicates and non-volatile organics. The most important sources are combustion processes at the ground and the agitation of soil material. During one flight, small cinnabar particles (HgS) were also detected.
Laura Tomsche, Andreas Marsing, Tina Jurkat-Witschas, Johannes Lucke, Stefan Kaufmann, Katharina Kaiser, Johannes Schneider, Monika Scheibe, Hans Schlager, Lenard Röder, Horst Fischer, Florian Obersteiner, Andreas Zahn, Martin Zöger, Jos Lelieveld, and Christiane Voigt
Atmos. Chem. Phys., 22, 15135–15151, https://doi.org/10.5194/acp-22-15135-2022, https://doi.org/10.5194/acp-22-15135-2022, 2022
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The detection of sulfur compounds in the upper troposphere (UT) and lower stratosphere (LS) is a challenge. In-flight measurements of SO2 and sulfate aerosol were performed during the BLUESKY mission in spring 2020 under exceptional atmospheric conditions. Reduced sinks in the dry UTLS and lower but still significant air traffic influenced the enhanced SO2 in the UT, and aged volcanic plumes enhanced the LS sulfate aerosol impacting the atmospheric radiation budget and global climate.
Oliver Appel, Franziska Köllner, Antonis Dragoneas, Andreas Hünig, Sergej Molleker, Hans Schlager, Christoph Mahnke, Ralf Weigel, Max Port, Christiane Schulz, Frank Drewnick, Bärbel Vogel, Fred Stroh, and Stephan Borrmann
Atmos. Chem. Phys., 22, 13607–13630, https://doi.org/10.5194/acp-22-13607-2022, https://doi.org/10.5194/acp-22-13607-2022, 2022
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This paper clarifies the chemical composition of the Asian tropopause aerosol layer (ATAL) by means of airborne in situ aerosol mass spectrometry (AMS). Ammonium nitrate and organics are found to significantly contribute to the particle layer, while sulfate does not show a layered structure. An analysis of the single-particle mass spectra suggests that secondary particle formation and subsequent growth dominate the particle composition, rather than condensation on pre-existing primary particles.
Albert Ansmann, Kevin Ohneiser, Alexandra Chudnovsky, Daniel A. Knopf, Edwin W. Eloranta, Diego Villanueva, Patric Seifert, Martin Radenz, Boris Barja, Félix Zamorano, Cristofer Jimenez, Ronny Engelmann, Holger Baars, Hannes Griesche, Julian Hofer, Dietrich Althausen, and Ulla Wandinger
Atmos. Chem. Phys., 22, 11701–11726, https://doi.org/10.5194/acp-22-11701-2022, https://doi.org/10.5194/acp-22-11701-2022, 2022
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For the first time we present a systematic study on the impact of wildfire smoke on ozone depletion in the Arctic (2020) and Antarctic stratosphere (2020, 2021). Two major fire events in Siberia and Australia were responsible for the observed record-breaking stratospheric smoke pollution. Our analyses were based on lidar observations of smoke parameters (Polarstern, Punta Arenas) and NDACC Arctic and Antarctic ozone profiles as well as on Antarctic OMI satellite observations of column ozone.
Ralf Weigel, Christoph Mahnke, Manuel Baumgartner, Martina Krämer, Peter Spichtinger, Nicole Spelten, Armin Afchine, Christian Rolf, Silvia Viciani, Francesco D'Amato, Holger Tost, and Stephan Borrmann
Atmos. Chem. Phys., 21, 13455–13481, https://doi.org/10.5194/acp-21-13455-2021, https://doi.org/10.5194/acp-21-13455-2021, 2021
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In July and August 2017, the StratoClim mission took place in Nepal with eight flights of the M-55 Geophysica at up to 20 km in the Asian monsoon anticyclone. New particle formation (NPF) next to cloud ice was detected in situ by abundant nucleation-mode aerosols (> 6 nm) along with ice particles (> 3 µm). NPF was observed mainly below the tropopause, down to 15 % being non-volatile residues. Observed intra-cloud NPF indicates its importance for the composition in the tropical tropopause layer.
Masatomo Fujiwara, Tetsu Sakai, Tomohiro Nagai, Koichi Shiraishi, Yoichi Inai, Sergey Khaykin, Haosen Xi, Takashi Shibata, Masato Shiotani, and Laura L. Pan
Atmos. Chem. Phys., 21, 3073–3090, https://doi.org/10.5194/acp-21-3073-2021, https://doi.org/10.5194/acp-21-3073-2021, 2021
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Lidar aerosol particle measurements in Japan during the summer of 2018 were found to detect the eastward extension of the Asian tropopause aerosol layer from the Asian summer monsoon anticyclone in the lower stratosphere. Analysis of various other data indicates that the observed enhanced particle levels are due to eastward-shedding vortices from the anticyclone, originating from pollutants emitted in Asian countries and transported vertically by convection in the Asian summer monsoon region.
Johannes Schneider, Ralf Weigel, Thomas Klimach, Antonis Dragoneas, Oliver Appel, Andreas Hünig, Sergej Molleker, Franziska Köllner, Hans-Christian Clemen, Oliver Eppers, Peter Hoppe, Peter Hoor, Christoph Mahnke, Martina Krämer, Christian Rolf, Jens-Uwe Grooß, Andreas Zahn, Florian Obersteiner, Fabrizio Ravegnani, Alexey Ulanovsky, Hans Schlager, Monika Scheibe, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Martin Zöger, and Stephan Borrmann
Atmos. Chem. Phys., 21, 989–1013, https://doi.org/10.5194/acp-21-989-2021, https://doi.org/10.5194/acp-21-989-2021, 2021
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During five aircraft missions, we detected aerosol particles containing meteoric material in the lower stratosphere. The stratospheric measurements span a latitude range from 15 to 68° N, and we find that at potential temperature levels of more than 40 K above the tropopause; particles containing meteoric material occur at similar abundance fractions across latitudes and seasons. We conclude that meteoric material is efficiently distributed between high and low latitudes by isentropic mixing.
Katharina Schütze, James Charles Wilson, Stephan Weinbruch, Nathalie Benker, Martin Ebert, Gebhard Günther, Ralf Weigel, and Stephan Borrmann
Atmos. Chem. Phys., 17, 12475–12493, https://doi.org/10.5194/acp-17-12475-2017, https://doi.org/10.5194/acp-17-12475-2017, 2017
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Stratospheric particles were collected in the polar stratosphere in winter 1999/2000. Besides the well-studied volatile particles from that region, the main findings of this study are stable carbonaceous particles in the sub-micrometer size range. In addition to carbon, many particles show the elements Si, Fe, Cr and Ni to a minor amount. Based on exclusion, carbonaceous material from IDPs and residues from meteoric ablation and fragmentation remain as the most probable sources.
Martin Ebert, Ralf Weigel, Konrad Kandler, Gebhard Günther, Sergej Molleker, Jens-Uwe Grooß, Bärbel Vogel, Stephan Weinbruch, and Stephan Borrmann
Atmos. Chem. Phys., 16, 8405–8421, https://doi.org/10.5194/acp-16-8405-2016, https://doi.org/10.5194/acp-16-8405-2016, 2016
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Stratospheric aerosol particles were collected within the arctic vortex in late winter. The chemical composition of refractory particles were analyzed by scanning electron microscopy. More than 750 refractory particles with diameters above 500 nm were found consisting of silicates, Fe- and Ca-rich particles and metal mixtures. The detection of refractory particles in the late winter polar stratosphere has strong implications for the formation of polar stratospheric clouds and ozone depletion.
Cited articles
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Short summary
In 2021, the eruption of La Soufrière released sulfur dioxide into the stratosphere, resulting in a spread of volcanic aerosol over the Northern Hemisphere. We conducted extensive aircraft and balloon-borne measurements after that, revealing enhanced particle concentration and altered size distribution due to the eruption. The eruption's impact on ozone depletion was minimal, contributing ~0.6 %, and its global radiative forcing effect was modest, mainly affecting tropical and midlatitude areas.
In 2021, the eruption of La Soufrière released sulfur dioxide into the stratosphere, resulting...
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