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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Brandon Bottorff, Michelle M. Lew, Youngjun Woo, Pamela Rickly, Matthew D. Rollings, Benjamin Deming, Daniel C. Anderson, Ezra Wood, Hariprasad D. Alwe, Dylan B. Millet, Andrew Weinheimer, Geoff Tyndall, John Ortega, Sebastien Dusanter, Thierry Leonardis, James Flynn, Matt Erickson, Sergio Alvarez, Jean C. Rivera-Rios, Joshua D. Shutter, Frank Keutsch, Detlev Helmig, Wei Wang, Hannah M. Allen, Johnathan H. Slade, Paul B. Shepson, Steven Bertman, and Philip S. Stevens
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Vigneshkumar Balamurugan, Jia Chen, Adrian Wenzel, and Frank N. Keutsch
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Marina Friedel, Gabriel Chiodo, Timofei Sukhodolov, James Keeble, Thomas Peter, Svenja Seeber, Andrea Stenke, Hideharu Akiyoshi, Eugene Rozanov, David Plummer, Patrick Jöckel, Guang Zeng, Olaf Morgenstern, and Béatrice Josse
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Qing Ye, Matthew B. Goss, Jordan E. Krechmer, Francesca Majluf, Alexander Zaytsev, Yaowei Li, Joseph R. Roscioli, Manjula Canagaratna, Frank N. Keutsch, Colette L. Heald, and Jesse H. Kroll
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Marina Friedel, Gabriel Chiodo, Andrea Stenke, Daniela I. V. Domeisen, and Thomas Peter
Atmos. Chem. Phys., 22, 13997–14017, https://doi.org/10.5194/acp-22-13997-2022, https://doi.org/10.5194/acp-22-13997-2022, 2022
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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
Atmos. Chem. Phys., 22, 12675–12694, https://doi.org/10.5194/acp-22-12675-2022, https://doi.org/10.5194/acp-22-12675-2022, 2022
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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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In this study, we investigated the response of secondary pollutants to changes in precursor emissions, focusing on the formation of secondary PM, during the COVID-19 lockdown period. We show that, due to the decrease in primary NOx emissions, atmospheric oxidizing capacity is increased. The nighttime increase in ozone, caused by less NO titration, results in higher NO3 radicals, which contribute significantly to the formation of PM nitrates. O3 should be limited in order to control PM pollution.
Debra K. Weisenstein, Daniele Visioni, Henning Franke, Ulrike Niemeier, Sandro Vattioni, Gabriel Chiodo, Thomas Peter, and David W. Keith
Atmos. Chem. Phys., 22, 2955–2973, https://doi.org/10.5194/acp-22-2955-2022, https://doi.org/10.5194/acp-22-2955-2022, 2022
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This paper explores a potential method of geoengineering that could be used to slow the rate of change of climate over decadal scales. We use three climate models to explore how injections of accumulation-mode sulfuric acid aerosol change the large-scale stratospheric particle size distribution and radiative forcing response for the chosen scenarios. Radiative forcing per unit sulfur injected and relative to the change in aerosol burden is larger with particulate than with SO2 injections.
Eric J. Hintsa, Fred L. Moore, Dale F. Hurst, Geoff S. Dutton, Bradley D. Hall, J. David Nance, Ben R. Miller, Stephen A. Montzka, Laura P. Wolton, Audra McClure-Begley, James W. Elkins, Emrys G. Hall, Allen F. Jordan, Andrew W. Rollins, Troy D. Thornberry, Laurel A. Watts, Chelsea R. Thompson, Jeff Peischl, Ilann Bourgeois, Thomas B. Ryerson, Bruce C. Daube, Yenny Gonzalez Ramos, Roisin Commane, Gregory W. Santoni, Jasna V. Pittman, Steven C. Wofsy, Eric Kort, Glenn S. Diskin, and T. Paul Bui
Atmos. Meas. Tech., 14, 6795–6819, https://doi.org/10.5194/amt-14-6795-2021, https://doi.org/10.5194/amt-14-6795-2021, 2021
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We built UCATS to study atmospheric chemistry and transport. It has measured trace gases including CFCs, N2O, SF6, CH4, CO, and H2 with gas chromatography, as well as ozone and water vapor. UCATS has been part of missions to study the tropical tropopause; transport of air into the stratosphere; greenhouse gases, transport, and chemistry in the troposphere; and ozone chemistry, on both piloted and unmanned aircraft. Its design, capabilities, and some results are shown and described here.
Dandan Wei, Hariprasad D. Alwe, Dylan B. Millet, Brandon Bottorff, Michelle Lew, Philip S. Stevens, Joshua D. Shutter, Joshua L. Cox, Frank N. Keutsch, Qianwen Shi, Sarah C. Kavassalis, Jennifer G. Murphy, Krystal T. Vasquez, Hannah M. Allen, Eric Praske, John D. Crounse, Paul O. Wennberg, Paul B. Shepson, Alexander A. T. Bui, Henry W. Wallace, Robert J. Griffin, Nathaniel W. May, Megan Connor, Jonathan H. Slade, Kerri A. Pratt, Ezra C. Wood, Mathew Rollings, Benjamin L. Deming, Daniel C. Anderson, and Allison L. Steiner
Geosci. Model Dev., 14, 6309–6329, https://doi.org/10.5194/gmd-14-6309-2021, https://doi.org/10.5194/gmd-14-6309-2021, 2021
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Over the past decade, understanding of isoprene oxidation has improved, and proper representation of isoprene oxidation and isoprene-derived SOA (iSOA) formation in canopy–chemistry models is now recognized to be important for an accurate understanding of forest–atmosphere exchange. The updated FORCAsT version 2.0 improves the estimation of some isoprene oxidation products and is one of the few canopy models currently capable of simulating SOA formation from monoterpenes and isoprene.
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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This paper features the new atmosphere–ocean–aerosol–chemistry–climate model SOCOLv4.0 and its validation. The model performance is evaluated against reanalysis products and observations of atmospheric circulation and trace gas distribution, with a focus on stratospheric processes. Although we identified some problems to be addressed in further model upgrades, we demonstrated that SOCOLv4.0 is already well suited for studies related to chemistry–climate–aerosol interactions.
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.
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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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