Articles | Volume 25, issue 24
https://doi.org/10.5194/acp-25-18449-2025
© Author(s) 2025. 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-25-18449-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| Highlight paper
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18 Dec 2025
Research article | Highlight paper |
| 18 Dec 2025
| 18 Dec 2025
Injection near the stratopause mitigates the stratospheric side effects of sulfur-based climate intervention
Institute for Environmental and Climate Research, College of Environment and Climate, Jinan University, Guangzhou, China
Yifeng Peng
School of Atmospheric Sciences, Lanzhou University, Lanzhou, China
Karen H. Rosenlof
Chemical Science Laboratory, National Oceanic and Atmospheric Administration, Boulder, Colorado
Ru-Shan Gao
Chemical Science Laboratory, National Oceanic and Atmospheric Administration, Boulder, Colorado
Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO, USA
Robert W. Portmann
Chemical Science Laboratory, National Oceanic and Atmospheric Administration, Boulder, Colorado
Martin Ross
Civil and Commercial Launch Projects, The Aerospace Corporation, Los Angeles, California
Chemical Science Laboratory, National Oceanic and Atmospheric Administration, Boulder, Colorado
Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO, USA
Jianchun Bian
Key Laboratory of Middle Atmosphere and Global Environment Observation, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, China
Simone Tilmes
Atmospheric Chemistry, Observations, and Modeling Laboratory, National Center for Atmospheric Research, Boulder, Colorado
Owen B. Toon
Department of Atmospheric and Oceanic Sciences and Laboratory for Atmospheric and Space Physics, University of Colorado, Boulder, Colorado
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Laura N. Saunders, Kaley A. Walker, Gabriele P. Stiller, Thomas von Clarmann, Florian Haenel, Hella Garny, Harald Bönisch, Chris D. Boone, Ariana E. Castillo, Andreas Engel, Johannes C. Laube, Marianna Linz, Felix Ploeger, David A. Plummer, Eric A. Ray, and Patrick E. Sheese
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Preprint archived
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Our simulations with volcanoes, when compared without volcanoes, show that volcanic aerosol precursors enter the tropical stratosphere, propagating upward and enhancing sulphate aerosol and heating. This stratospheric heating caused by the volcanoes reduces the amplitude of the QBO and disrupts its phases. Since QBO also modulates tropical convection and weather, we suggest including volcanic emissions and the QBO in the weather prediction model for a better forecast.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles A. Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
Atmos. Chem. Phys., 25, 45–71, https://doi.org/10.5194/acp-25-45-2025, https://doi.org/10.5194/acp-25-45-2025, 2025
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Using single-particle mass spectrometry, we show that trace concentrations of bromine and iodine are ubiquitous in remote tropospheric aerosol and suggest that aerosols are an important part of the global reactive iodine budget. Comparisons to a global climate model with detailed iodine chemistry are favorable in the background atmosphere; however, the model cannot replicate our measurements near the ocean surface, in biomass burning plumes, and in the stratosphere.
Zhou Zang, Jane Liu, David Tarasick, Omid Moeini, Jianchun Bian, Jinqiang Zhang, Anne M. Thompson, Roeland Van Malderen, Herman G. J. Smit, Ryan M. Stauffer, Bryan J. Johnson, and Debra E. Kollonige
Atmos. Chem. Phys., 24, 13889–13912, https://doi.org/10.5194/acp-24-13889-2024, https://doi.org/10.5194/acp-24-13889-2024, 2024
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The Trajectory-mapped Ozonesonde dataset for the Stratosphere and Troposphere (TOST) provides a global-scale, long-term ozone climatology that is horizontally and vertically resolved. In this study, we improved, updated and validated TOST from 1970 to 2021. Based on this TOST dataset, we characterized global ozone variations spatially in both the troposphere and stratosphere and temporally by season and decade. We also showed a stagnant lower stratospheric ozone variation since the late 1990s.
Eric A. Ray, Fred L. Moore, Hella Garny, Eric J. Hintsa, Bradley D. Hall, Geoff S. Dutton, David Nance, James W. Elkins, Steven C. Wofsy, Jasna Pittman, Bruce Daube, Bianca C. Baier, Jianghanyang Li, and Colm Sweeney
Atmos. Chem. Phys., 24, 12425–12445, https://doi.org/10.5194/acp-24-12425-2024, https://doi.org/10.5194/acp-24-12425-2024, 2024
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In this study we describe new techniques to derive age of air from multiple simultaneous measurements of long-lived trace gases in order to improve the fidelity of the age-of-air estimates and to be able to compare age of air from measurements taken from different instruments, platforms and decades. This technique also allows new transport information to be obtained from the measurements such as the primary source latitude that can also be compared to models.
Christina V. Brodowsky, Timofei Sukhodolov, Gabriel Chiodo, Valentina Aquila, Slimane Bekki, Sandip S. Dhomse, Michael Höpfner, Anton Laakso, Graham W. Mann, Ulrike Niemeier, Giovanni Pitari, Ilaria Quaglia, Eugene Rozanov, Anja Schmidt, Takashi Sekiya, Simone Tilmes, Claudia Timmreck, Sandro Vattioni, Daniele Visioni, Pengfei Yu, Yunqian Zhu, and Thomas Peter
Atmos. Chem. Phys., 24, 5513–5548, https://doi.org/10.5194/acp-24-5513-2024, https://doi.org/10.5194/acp-24-5513-2024, 2024
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The aerosol layer is an essential part of the climate system. We characterize the sulfur budget in a volcanically quiescent (background) setting, with a special focus on the sulfate aerosol layer using, for the first time, a multi-model approach. The aim is to identify weak points in the representation of the atmospheric sulfur budget in an intercomparison of nine state-of-the-art coupled global circulation models.
Anton Laakso, Daniele Visioni, Ulrike Niemeier, Simone Tilmes, and Harri Kokkola
Earth Syst. Dynam., 15, 405–427, https://doi.org/10.5194/esd-15-405-2024, https://doi.org/10.5194/esd-15-405-2024, 2024
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This study is the second in a two-part series in which we explore the dependency of the impacts of stratospheric sulfur injections on both the model employed and the strategy of injection utilized. The study uncovers uncertainties associated with these techniques to cool climate, highlighting how the simulated climate impacts are dependent on both the selected model and the magnitude of the injections. We also show that estimating precipitation impacts of aerosol injection is a complex task.
Hella Garny, Roland Eichinger, Johannes C. Laube, Eric A. Ray, Gabriele P. Stiller, Harald Bönisch, Laura Saunders, and Marianna Linz
Atmos. Chem. Phys., 24, 4193–4215, https://doi.org/10.5194/acp-24-4193-2024, https://doi.org/10.5194/acp-24-4193-2024, 2024
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Transport circulation in the stratosphere is important for the distribution of tracers, but its strength is hard to measure. Mean transport times can be inferred from observations of trace gases with certain properties, such as sulfur hexafluoride (SF6). However, this gas has a chemical sink in the high atmosphere, which can lead to substantial biases in inferred transport times. In this paper we present a method to correct mean transport times derived from SF6 for the effects of chemical sinks.
Daniele Visioni, Alan Robock, Jim Haywood, Matthew Henry, Simone Tilmes, Douglas G. MacMartin, Ben Kravitz, Sarah J. Doherty, John Moore, Chris Lennard, Shingo Watanabe, Helene Muri, Ulrike Niemeier, Olivier Boucher, Abu Syed, Temitope S. Egbebiyi, Roland Séférian, and Ilaria Quaglia
Geosci. Model Dev., 17, 2583–2596, https://doi.org/10.5194/gmd-17-2583-2024, https://doi.org/10.5194/gmd-17-2583-2024, 2024
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This paper describes a new experimental protocol for the Geoengineering Model Intercomparison Project (GeoMIP). In it, we describe the details of a new simulation of sunlight reflection using the stratospheric aerosols that climate models are supposed to run, and we explain the reasons behind each choice we made when defining the protocol.
Danny M. Leung, Jasper F. Kok, Longlei Li, Natalie M. Mahowald, David M. Lawrence, Simone Tilmes, Erik Kluzek, Martina Klose, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 2287–2318, https://doi.org/10.5194/acp-24-2287-2024, https://doi.org/10.5194/acp-24-2287-2024, 2024
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This study uses a premier Earth system model to evaluate a new desert dust emission scheme proposed in our companion paper. We show that our scheme accounts for more dust emission physics, hence matching better against observations than other existing dust emission schemes do. Our scheme's dust emissions also couple tightly with meteorology, hence likely improving the modeled dust sensitivity to climate change. We believe this work is vital for improving dust representation in climate models.
Abolfazl Rezaei, Khalil Karami, Simone Tilmes, and John C. Moore
Earth Syst. Dynam., 15, 91–108, https://doi.org/10.5194/esd-15-91-2024, https://doi.org/10.5194/esd-15-91-2024, 2024
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Water storage (WS) plays a profound role in the lives of people in the Middle East and North Africa as well as Mediterranean climate "hot spots". WS change by greenhouse gas (GHG) warming is simulated with and without stratospheric aerosol intervention (SAI). WS significantly increases in the Arabian Peninsula and decreases around the Mediterranean under GHG. While SAI partially ameliorates GHG impacts, projected WS increases in dry regions and decreases in wet areas relative to present climate.
Simone Tilmes, Michael J. Mills, Yunqian Zhu, Charles G. Bardeen, Francis Vitt, Pengfei Yu, David Fillmore, Xiaohong Liu, Brian Toon, and Terry Deshler
Geosci. Model Dev., 16, 6087–6125, https://doi.org/10.5194/gmd-16-6087-2023, https://doi.org/10.5194/gmd-16-6087-2023, 2023
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We implemented an alternative aerosol scheme in the high- and low-top model versions of the Community Earth System Model Version 2 (CESM2) with a more detailed description of tropospheric and stratospheric aerosol size distributions than the existing aerosol model. This development enables the comparison of different aerosol schemes with different complexity in the same model framework. It identifies improvements compared to a range of observations in both the troposphere and stratosphere.
Wenfu Tang, Louisa K. Emmons, Helen M. Worden, Rajesh Kumar, Cenlin He, Benjamin Gaubert, Zhonghua Zheng, Simone Tilmes, Rebecca R. Buchholz, Sara-Eva Martinez-Alonso, Claire Granier, Antonin Soulie, Kathryn McKain, Bruce C. Daube, Jeff Peischl, Chelsea Thompson, and Pieternel Levelt
Geosci. Model Dev., 16, 6001–6028, https://doi.org/10.5194/gmd-16-6001-2023, https://doi.org/10.5194/gmd-16-6001-2023, 2023
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The new MUSICAv0 model enables the study of atmospheric chemistry across all relevant scales. We develop a MUSICAv0 grid for Africa. We evaluate MUSICAv0 with observations and compare it with a previously used model – WRF-Chem. Overall, the performance of MUSICAv0 is comparable to WRF-Chem. Based on model–satellite discrepancies, we find that future field campaigns in an eastern African region (30°E–45°E, 5°S–5°N) could substantially improve the predictive skill of air quality models.
Yunqian Zhu, Robert W. Portmann, Douglas Kinnison, Owen Brian Toon, Luis Millán, Jun Zhang, Holger Vömel, Simone Tilmes, Charles G. Bardeen, Xinyue Wang, Stephanie Evan, William J. Randel, and Karen H. Rosenlof
Atmos. Chem. Phys., 23, 13355–13367, https://doi.org/10.5194/acp-23-13355-2023, https://doi.org/10.5194/acp-23-13355-2023, 2023
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The 2022 Hunga Tonga eruption injected a large amount of water into the stratosphere. Ozone depletion was observed inside the volcanic plume. Chlorine and water vapor injected by this eruption exceeded the normal range, which made the ozone chemistry during this event occur at a higher temperature than polar ozone depletion. Unlike polar ozone chemistry where chlorine nitrate is more important, hypochlorous acid plays a large role in the in-plume chlorine balance and heterogeneous processes.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Jianchun Bian, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 23, 13029–13047, https://doi.org/10.5194/acp-23-13029-2023, https://doi.org/10.5194/acp-23-13029-2023, 2023
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For the first time a regularized multivariate regression model is used to estimate stratospheric ozone trends. Regularized regression avoids the over-fitting issue due to correlation among explanatory variables. We demonstrate that there are considerable differences in satellite-based and chemical-model-based ozone trends, highlighting large uncertainties in our understanding about ozone variability. We argue that caution is needed when interpreting results with different methods and datasets.
Michael Kiefer, Dale F. Hurst, Gabriele P. Stiller, Stefan Lossow, Holger Vömel, John Anderson, Faiza Azam, Jean-Loup Bertaux, Laurent Blanot, Klaus Bramstedt, John P. Burrows, Robert Damadeo, Bianca Maria Dinelli, Patrick Eriksson, Maya García-Comas, John C. Gille, Mark Hervig, Yasuko Kasai, Farahnaz Khosrawi, Donal Murtagh, Gerald E. Nedoluha, Stefan Noël, Piera Raspollini, William G. Read, Karen H. Rosenlof, Alexei Rozanov, Christopher E. Sioris, Takafumi Sugita, Thomas von Clarmann, Kaley A. Walker, and Katja Weigel
Atmos. Meas. Tech., 16, 4589–4642, https://doi.org/10.5194/amt-16-4589-2023, https://doi.org/10.5194/amt-16-4589-2023, 2023
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We quantify biases and drifts (and their uncertainties) between the stratospheric water vapor measurement records of 15 satellite-based instruments (SATs, with 31 different retrievals) and balloon-borne frost point hygrometers (FPs) launched at 27 globally distributed stations. These comparisons of measurements during the period 2000–2016 are made using robust, consistent statistical methods. With some exceptions, the biases and drifts determined for most SAT–FP pairs are < 10 % and < 1 % yr−1.
Seyed Vahid Mousavi, Khalil Karami, Simone Tilmes, Helene Muri, Lili Xia, and Abolfazl Rezaei
Atmos. Chem. Phys., 23, 10677–10695, https://doi.org/10.5194/acp-23-10677-2023, https://doi.org/10.5194/acp-23-10677-2023, 2023
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Understanding atmospheric dust changes in the Middle East and North Africa (MENA) region under future climate scenarios is essential. By injecting sulfate aerosols into the stratosphere, stratospheric aerosol injection (SAI) geoengineering reflects some of the incoming sunlight back to space. This study shows that the MENA region would experience lower dust concentration under both SAI and RCP8.5 scenarios compared to the current climate (CTL) by the end of the century.
Duseong S. Jo, Simone Tilmes, Louisa K. Emmons, Siyuan Wang, and Francis Vitt
Geosci. Model Dev., 16, 3893–3906, https://doi.org/10.5194/gmd-16-3893-2023, https://doi.org/10.5194/gmd-16-3893-2023, 2023
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A new simple secondary organic aerosol (SOA) scheme has been developed for the Community Atmosphere Model (CAM) based on the complex SOA scheme in CAM with detailed chemistry (CAM-chem). The CAM with the new SOA scheme shows better agreements with CAM-chem in terms of aerosol concentrations and radiative fluxes, which ensures more consistent results between different compsets in the Community Earth System Model. The new SOA scheme also has technical advantages for future developments.
Abolfazl Rezaei, Khalil Karami, Simone Tilmes, and John C. Moore
Atmos. Chem. Phys., 23, 5835–5850, https://doi.org/10.5194/acp-23-5835-2023, https://doi.org/10.5194/acp-23-5835-2023, 2023
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Teleconnection patterns are important characteristics of the climate system; well-known examples include the El Niño and La Niña events driven from the tropical Pacific. We examined how spatiotemporal patterns that arise in the Pacific and Atlantic oceans behave under stratospheric aerosol geoengineering and greenhouse gas (GHG)-induced warming. In general, geoengineering reverses trends; however, the changes in decadal oscillation for the AMO, NAO, and PDO imposed by GHG are not suppressed.
Wenfu Tang, Simone Tilmes, David M. Lawrence, Fang Li, Cenlin He, Louisa K. Emmons, Rebecca R. Buchholz, and Lili Xia
Atmos. Chem. Phys., 23, 5467–5486, https://doi.org/10.5194/acp-23-5467-2023, https://doi.org/10.5194/acp-23-5467-2023, 2023
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Globally, total wildfire burned area is projected to increase over the 21st century under scenarios without geoengineering and decrease under the two geoengineering scenarios. Geoengineering reduces fire by decreasing surface temperature and wind speed and increasing relative humidity and soil water. However, geoengineering also yields reductions in precipitation, which offset some of the fire reduction.
Daniele Visioni, Ben Kravitz, Alan Robock, Simone Tilmes, Jim Haywood, Olivier Boucher, Mark Lawrence, Peter Irvine, Ulrike Niemeier, Lili Xia, Gabriel Chiodo, Chris Lennard, Shingo Watanabe, John C. Moore, and Helene Muri
Atmos. Chem. Phys., 23, 5149–5176, https://doi.org/10.5194/acp-23-5149-2023, https://doi.org/10.5194/acp-23-5149-2023, 2023
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Geoengineering indicates methods aiming to reduce the temperature of the planet by means of reflecting back a part of the incoming radiation before it reaches the surface or allowing more of the planetary radiation to escape into space. It aims to produce modelling experiments that are easy to reproduce and compare with different climate models, in order to understand the potential impacts of these techniques. Here we assess its past successes and failures and talk about its future.
Khalil Karami, Rolando Garcia, Christoph Jacobi, Jadwiga H. Richter, and Simone Tilmes
Atmos. Chem. Phys., 23, 3799–3818, https://doi.org/10.5194/acp-23-3799-2023, https://doi.org/10.5194/acp-23-3799-2023, 2023
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Alongside mitigation and adaptation efforts, stratospheric aerosol intervention (SAI) is increasingly considered a third pillar to combat dangerous climate change. We investigate the teleconnection between the quasi-biennial oscillation in the equatorial stratosphere and the Arctic stratospheric polar vortex under a warmer climate and an SAI scenario. We show that the Holton–Tan relationship weakens under both scenarios and discuss the physical mechanisms responsible for such changes.
Sean M. Davis, Nicholas Davis, Robert W. Portmann, Eric Ray, and Karen Rosenlof
Atmos. Chem. Phys., 23, 3347–3361, https://doi.org/10.5194/acp-23-3347-2023, https://doi.org/10.5194/acp-23-3347-2023, 2023
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Ozone in the lower part of the stratosphere has not increased and has perhaps even continued to decline in recent decades. This study demonstrates that the amount of ozone in this region is highly sensitive to the amount of air upwelling into the stratosphere in the tropics and that simulations from a climate model nudged to historical meteorological fields often fail to accurately capture the variations in tropical upwelling that control short-term trends in lower-stratospheric ozone.
Yangxin Chen, Duoying Ji, Qian Zhang, John C. Moore, Olivier Boucher, Andy Jones, Thibaut Lurton, Michael J. Mills, Ulrike Niemeier, Roland Séférian, and Simone Tilmes
Earth Syst. Dynam., 14, 55–79, https://doi.org/10.5194/esd-14-55-2023, https://doi.org/10.5194/esd-14-55-2023, 2023
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Solar geoengineering has been proposed as a way of counteracting the warming effects of increasing greenhouse gases by reflecting solar radiation. This work shows that solar geoengineering can slow down the northern-high-latitude permafrost degradation but cannot preserve the permafrost ecosystem as that under a climate of the same warming level without solar geoengineering.
Caroline C. Womack, Steven S. Brown, Steven J. Ciciora, Ru-Shan Gao, Richard J. McLaughlin, Michael A. Robinson, Yinon Rudich, and Rebecca A. Washenfelder
Atmos. Meas. Tech., 15, 6643–6652, https://doi.org/10.5194/amt-15-6643-2022, https://doi.org/10.5194/amt-15-6643-2022, 2022
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We present a new miniature instrument to measure nitrogen dioxide (NO2) using cavity-enhanced spectroscopy. NO2 contributes to the formation of pollutants such as ozone and particulate matter, and its concentration can vary widely near sources. We developed this lightweight (3.05 kg) low-power (<35 W) instrument to measure NO2 on uncrewed aircraft vehicles (UAVs) and demonstrate that it has the accuracy and precision needed for atmospheric field measurements.
Siying Lian, Luxi Zhou, Daniel M. Murphy, Karl D. Froyd, Owen B. Toon, and Pengfei Yu
Atmos. Chem. Phys., 22, 13659–13676, https://doi.org/10.5194/acp-22-13659-2022, https://doi.org/10.5194/acp-22-13659-2022, 2022
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Parameterizations of dust lifting and microphysical properties of dust in climate models are still subject to large uncertainty. Here we use a sectional aerosol climate model to investigate the global vertical distributions of the dust. Constrained by a suite of observations, the model suggests that, although North African dust dominates global dust mass loading at the surface, the relative contribution of Asian dust increases with altitude and becomes dominant in the upper troposphere.
Mari R. Tye, Katherine Dagon, Maria J. Molina, Jadwiga H. Richter, Daniele Visioni, Ben Kravitz, and Simone Tilmes
Earth Syst. Dynam., 13, 1233–1257, https://doi.org/10.5194/esd-13-1233-2022, https://doi.org/10.5194/esd-13-1233-2022, 2022
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We examined the potential effect of stratospheric aerosol injection (SAI) on extreme temperature and precipitation. SAI may cause daytime temperatures to cool but nighttime to warm. Daytime cooling may occur in all seasons across the globe, with the largest decreases in summer. In contrast, nighttime warming may be greatest at high latitudes in winter. SAI may reduce the frequency and intensity of extreme rainfall. The combined changes may exacerbate drying over parts of the global south.
William G. Read, Gabriele Stiller, Stefan Lossow, Michael Kiefer, Farahnaz Khosrawi, Dale Hurst, Holger Vömel, Karen Rosenlof, Bianca M. Dinelli, Piera Raspollini, Gerald E. Nedoluha, John C. Gille, Yasuko Kasai, Patrick Eriksson, Christopher E. Sioris, Kaley A. Walker, Katja Weigel, John P. Burrows, and Alexei Rozanov
Atmos. Meas. Tech., 15, 3377–3400, https://doi.org/10.5194/amt-15-3377-2022, https://doi.org/10.5194/amt-15-3377-2022, 2022
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This paper attempts to provide an assessment of the accuracy of 21 satellite-based instruments that remotely measure atmospheric humidity in the upper troposphere of the Earth's atmosphere. The instruments made their measurements from 1984 to the present time; however, most of these instruments began operations after 2000, and only a few are still operational. The objective of this study is to quantify the accuracy of each satellite humidity data set.
Eric A. Ray, Elliot L. Atlas, Sue Schauffler, Sofia Chelpon, Laura Pan, Harald Bönisch, and Karen H. Rosenlof
Atmos. Chem. Phys., 22, 6539–6558, https://doi.org/10.5194/acp-22-6539-2022, https://doi.org/10.5194/acp-22-6539-2022, 2022
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The movement of air masses and the trace gases they contain from the Earth’s surface into the upper troposphere and lower stratosphere (UTLS) can have important implications for the radiative and chemical balance of the atmosphere. In this study we build on recent techniques and use new ones to estimate a range of transport diagnostics based on simultaneously measured trace gases in the UTLS during the monsoon season in North America.
Liang Ran, Zhaoze Deng, Yunfei Wu, Jiwei Li, Zhixuan Bai, Ye Lu, Deqing Zhuoga, and Jianchun Bian
Atmos. Chem. Phys., 22, 6217–6229, https://doi.org/10.5194/acp-22-6217-2022, https://doi.org/10.5194/acp-22-6217-2022, 2022
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The Tibetan Plateau (TP), the highest plateau in the world, plays a crucial role in regional and global climate. To examine the fingerprint left by human activities on the originally remote atmosphere, size distributions of particles from the ground to about 800 m were measured for the first time in summer 2020 in Lhasa, one of a few urbanized cities on TP. Potential sources of particles at different heights were explored. The contribution of emissions from religious activities was highlighted.
Simone Tilmes, Daniele Visioni, Andy Jones, James Haywood, Roland Séférian, Pierre Nabat, Olivier Boucher, Ewa Monica Bednarz, and Ulrike Niemeier
Atmos. Chem. Phys., 22, 4557–4579, https://doi.org/10.5194/acp-22-4557-2022, https://doi.org/10.5194/acp-22-4557-2022, 2022
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This study assesses the impacts of climate interventions, using stratospheric sulfate aerosol and solar dimming on stratospheric ozone, based on three Earth system models with interactive stratospheric chemistry. The climate interventions have been applied to a high emission (baseline) scenario in order to reach global surface temperatures of a medium emission scenario. We find significant increases and decreases in total column ozone, depending on regions and seasons.
Kai Qie, Wuke Wang, Wenshou Tian, Rui Huang, Mian Xu, Tao Wang, and Yifeng Peng
Atmos. Chem. Phys., 22, 4393–4411, https://doi.org/10.5194/acp-22-4393-2022, https://doi.org/10.5194/acp-22-4393-2022, 2022
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We identify a significantly intensified upward motion over the tropical western Pacific (TWP) and an enhanced tropical upwelling in boreal winter during 1958–2017 due to the warming of global sea surface temperatures (SSTs). Our results suggest that more tropospheric trace gases over the TWP could be elevated to the lower stratosphere, which implies that the emission from the maritime continent plays a more important role in the stratospheric processes and the global climate.
Andy Jones, Jim M. Haywood, Adam A. Scaife, Olivier Boucher, Matthew Henry, Ben Kravitz, Thibaut Lurton, Pierre Nabat, Ulrike Niemeier, Roland Séférian, Simone Tilmes, and Daniele Visioni
Atmos. Chem. Phys., 22, 2999–3016, https://doi.org/10.5194/acp-22-2999-2022, https://doi.org/10.5194/acp-22-2999-2022, 2022
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Simulations by six Earth-system models of geoengineering by introducing sulfuric acid aerosols into the tropical stratosphere are compared. A robust impact on the northern wintertime North Atlantic Oscillation is found, exacerbating precipitation reduction over parts of southern Europe. In contrast, the models show no consistency with regard to impacts on the Quasi-Biennial Oscillation, although results do indicate a risk that the oscillation could become locked into a permanent westerly phase.
Lei Hu, Stephen A. Montzka, Fred Moore, Eric Hintsa, Geoff Dutton, M. Carolina Siso, Kirk Thoning, Robert W. Portmann, Kathryn McKain, Colm Sweeney, Isaac Vimont, David Nance, Bradley Hall, and Steven Wofsy
Atmos. Chem. Phys., 22, 2891–2907, https://doi.org/10.5194/acp-22-2891-2022, https://doi.org/10.5194/acp-22-2891-2022, 2022
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The unexpected increase in CFC-11 emissions between 2012 and 2017 resulted in concerns about delaying the stratospheric ozone recovery. Although the subsequent decline of CFC-11 emissions indicated a mitigation in part to this problem, the regions fully responsible for these large emission changes were unclear. Here, our new estimate, based on atmospheric measurements from two global campaigns and from NOAA, suggests Asia primarily contributed to the global CFC-11 emission rise during 2012–2017.
Daniele Visioni, Simone Tilmes, Charles Bardeen, Michael Mills, Douglas G. MacMartin, Ben Kravitz, and Jadwiga H. Richter
Atmos. Chem. Phys., 22, 1739–1756, https://doi.org/10.5194/acp-22-1739-2022, https://doi.org/10.5194/acp-22-1739-2022, 2022
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Aerosols are simulated in a simplified way in climate models: in the model analyzed here, they are represented in every grid as described by three simple logarithmic distributions, mixing all different species together. The size can evolve when new particles are formed, particles merge together to create a larger one or particles are deposited to the surface. This approximation normally works fairly well. Here we show however that when large amounts of sulfate are simulated, there are problems.
Nicholas A. Davis, Patrick Callaghan, Isla R. Simpson, and Simone Tilmes
Atmos. Chem. Phys., 22, 197–214, https://doi.org/10.5194/acp-22-197-2022, https://doi.org/10.5194/acp-22-197-2022, 2022
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Specified dynamics schemes attempt to constrain the atmospheric circulation in a climate model to isolate the role of transport in chemical variability, evaluate model physics, and interpret field campaign observations. We show that the specified dynamics scheme in CESM2 erroneously suppresses convection and induces circulation errors that project onto errors in tracers, even using the most optimal settings. Development of a more sophisticated scheme is necessary for future progress.
Anton Laakso, Ulrike Niemeier, Daniele Visioni, Simone Tilmes, and Harri Kokkola
Atmos. Chem. Phys., 22, 93–118, https://doi.org/10.5194/acp-22-93-2022, https://doi.org/10.5194/acp-22-93-2022, 2022
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The use of different spatio-temporal sulfur injection strategies with different magnitudes to create an artificial reflective aerosol layer to cool the climate is studied using sectional and modal aerosol schemes in a climate model. There are significant differences in the results depending on the aerosol microphysical module used. Different spatio-temporal injection strategies have a significant impact on the magnitude and zonal distribution of radiative forcing and atmospheric dynamics.
Thierno Doumbia, Claire Granier, Nellie Elguindi, Idir Bouarar, Sabine Darras, Guy Brasseur, Benjamin Gaubert, Yiming Liu, Xiaoqin Shi, Trissevgeni Stavrakou, Simone Tilmes, Forrest Lacey, Adrien Deroubaix, and Tao Wang
Earth Syst. Sci. Data, 13, 4191–4206, https://doi.org/10.5194/essd-13-4191-2021, https://doi.org/10.5194/essd-13-4191-2021, 2021
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Most countries around the world have implemented control measures to combat the spread of the COVID-19 pandemic, resulting in significant changes in economic and personal activities. We developed the CONFORM (COvid-19 adjustmeNt Factors fOR eMissions) dataset to account for changes in emissions during lockdowns. This dataset was created with the intention of being directly applicable to existing global and regional inventories used in chemical transport models.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke D. Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul A. Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 11113–11132, https://doi.org/10.5194/acp-21-11113-2021, https://doi.org/10.5194/acp-21-11113-2021, 2021
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected nearly from pole to pole over the oceans during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigated their impact on the variability of tropospheric N2O.
Daniele Visioni, Douglas G. MacMartin, Ben Kravitz, Olivier Boucher, Andy Jones, Thibaut Lurton, Michou Martine, Michael J. Mills, Pierre Nabat, Ulrike Niemeier, Roland Séférian, and Simone Tilmes
Atmos. Chem. Phys., 21, 10039–10063, https://doi.org/10.5194/acp-21-10039-2021, https://doi.org/10.5194/acp-21-10039-2021, 2021
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A new set of simulations is used to investigate commonalities, differences and sources of uncertainty when simulating the injection of SO2 in the stratosphere in order to mitigate the effects of climate change (solar geoengineering). The models differ in how they simulate the aerosols and how they spread around the stratosphere, resulting in differences in projected regional impacts. Overall, however, the models agree that aerosols have the potential to mitigate the warming produced by GHGs.
Christina J. Williamson, Agnieszka Kupc, Andrew Rollins, Jan Kazil, Karl D. Froyd, Eric A. Ray, Daniel M. Murphy, Gregory P. Schill, Jeff Peischl, Chelsea Thompson, Ilann Bourgeois, Thomas B. Ryerson, Glenn S. Diskin, Joshua P. DiGangi, Donald R. Blake, Thao Paul V. Bui, Maximilian Dollner, Bernadett Weinzierl, and Charles A. Brock
Atmos. Chem. Phys., 21, 9065–9088, https://doi.org/10.5194/acp-21-9065-2021, https://doi.org/10.5194/acp-21-9065-2021, 2021
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Aerosols in the stratosphere influence climate by scattering and absorbing sunlight and through chemical reactions occurring on the particles’ surfaces. We observed more nucleation mode aerosols (small aerosols, with diameters below 12 nm) in the mid- and high-latitude lowermost stratosphere (8–13 km) in the Northern Hemisphere (NH) than in the Southern Hemisphere. The most likely cause of this is aircraft emissions, which are concentrated in the NH at similar altitudes to our observations.
Daniel M. Murphy, Karl D. Froyd, Ilann Bourgeois, Charles A. Brock, Agnieszka Kupc, Jeff Peischl, Gregory P. Schill, Chelsea R. Thompson, Christina J. Williamson, and Pengfei Yu
Atmos. Chem. Phys., 21, 8915–8932, https://doi.org/10.5194/acp-21-8915-2021, https://doi.org/10.5194/acp-21-8915-2021, 2021
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New measurements in the lower stratosphere highlight differences between particles that originated in the troposphere or the stratosphere. The stratospheric-origin particles have relatively large radiative effects because they are at nearly the optimum diameter for light scattering. The tropospheric particles contribute significantly to surface area. These and other chemical and physical properties are then extended to study the implications if material were to be added to the stratosphere.
Fernando Chouza, Thierry Leblanc, Mark Brewer, Patrick Wang, Sabino Piazzolla, Gabriele Pfister, Rajesh Kumar, Carl Drews, Simone Tilmes, Louisa Emmons, and Matthew Johnson
Atmos. Chem. Phys., 21, 6129–6153, https://doi.org/10.5194/acp-21-6129-2021, https://doi.org/10.5194/acp-21-6129-2021, 2021
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The tropospheric ozone lidar at the JPL Table Mountain Facility (TMF) was used to investigate the impact of Los Angeles (LA) Basin pollution transport and stratospheric intrusions in the planetary boundary layer on the San Gabriel Mountains. The results of this study indicate a dominant role of the LA Basin pollution on days when high ozone levels were observed at TMF (March–October period).
Ben Kravitz, Douglas G. MacMartin, Daniele Visioni, Olivier Boucher, Jason N. S. Cole, Jim Haywood, Andy Jones, Thibaut Lurton, Pierre Nabat, Ulrike Niemeier, Alan Robock, Roland Séférian, and Simone Tilmes
Atmos. Chem. Phys., 21, 4231–4247, https://doi.org/10.5194/acp-21-4231-2021, https://doi.org/10.5194/acp-21-4231-2021, 2021
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This study investigates multi-model response to idealized geoengineering (high CO2 with solar reduction) across two different generations of climate models. We find that, with the exception of a few cases, the results are unchanged between the different generations. This gives us confidence that broad conclusions about the response to idealized geoengineering are robust.
Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, https://doi.org/10.5194/acp-21-4187-2021, 2021
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We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.
Chaim I. Garfinkel, Ohad Harari, Shlomi Ziskin Ziv, Jian Rao, Olaf Morgenstern, Guang Zeng, Simone Tilmes, Douglas Kinnison, Fiona M. O'Connor, Neal Butchart, Makoto Deushi, Patrick Jöckel, Andrea Pozzer, and Sean Davis
Atmos. Chem. Phys., 21, 3725–3740, https://doi.org/10.5194/acp-21-3725-2021, https://doi.org/10.5194/acp-21-3725-2021, 2021
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Water vapor is the dominant greenhouse gas in the atmosphere, and El Niño is the dominant mode of variability in the ocean–atmosphere system. The connection between El Niño and water vapor above ~ 17 km is unclear, with single-model studies reaching a range of conclusions. This study examines this connection in 12 different models. While there are substantial differences among the models, all models appear to capture the fundamental physical processes correctly.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 3395–3425, https://doi.org/10.5194/acp-21-3395-2021, https://doi.org/10.5194/acp-21-3395-2021, 2021
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Secondary organic aerosol (SOA) is a major component of submicron particulate matter, but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX SOA concentration changes. The explicit chemistry predicted substantial changes in IEPOX SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physicochemical dependencies in future SOA prediction.
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.
Sabine Robrecht, Bärbel Vogel, Simone Tilmes, and Rolf Müller
Atmos. Chem. Phys., 21, 2427–2455, https://doi.org/10.5194/acp-21-2427-2021, https://doi.org/10.5194/acp-21-2427-2021, 2021
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Column ozone protects life on Earth from radiation damage. Stratospheric chlorine compounds cause immense ozone loss in polar winter. Whether similar loss processes can occur in the lower stratosphere above North America today or in future is a matter of debate. We show that these ozone loss processes are very unlikely today or in future independently of whether sulfate geoengineering is applied and that less than 0.1 % of column ozone would be destroyed by this process in any future scenario.
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Executive editor
The present work highlights advantages of a stratospheric aerosol injection (SAI) scheme for solar radiation management (SRM) as a geoengineering technology. It suggests higher altitude aerosol injection would reduce several of the side effects of SAI in the lower stratosphere. Given the substantial debate on scientific, ethical and societal aspects of SRM and SAI are a highly relevant topic.
The present work highlights advantages of a stratospheric aerosol injection (SAI) scheme for...
Short summary
Injecting sulfur dioxide at 50 km – near the stratopause – offers a far safer and more effective climate intervention than conventional 25 km injection. Rapid downward–poleward transport distributes aerosols across 20–30 km, halving tropical stratospheric warming, reducing ozone recovery delays from decades to about 5 years, and enhancing global and polar cooling by over 20 %, while better preserving Arctic sea ice.
Injecting sulfur dioxide at 50 km – near the stratopause – offers a far safer and more effective...
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