Articles | Volume 17, issue 19
https://doi.org/10.5194/acp-17-11913-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-17-11913-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
09 Oct 2017
Research article |
| 09 Oct 2017
Impacts of stratospheric sulfate geoengineering on tropospheric ozone
Department of Environmental Sciences, Rutgers University, New
Brunswick, New Jersey, USA
Peer J. Nowack
Department of Chemistry, Centre for Atmospheric Science, University of
Cambridge, Cambridge, UK
now at: Grantham Institute and Department of
Physics, Faculty of Natural Sciences, Imperial College London, London, UK
Simone Tilmes
Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric
Research, Boulder, Colorado, USA
Alan Robock
Department of Environmental Sciences, Rutgers University, New
Brunswick, New Jersey, USA
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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
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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
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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
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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.
Sam S. Rabin, William J. Sacks, Danica L. Lombardozzi, Lili Xia, and Alan Robock
Geosci. Model Dev., 16, 7253–7273, https://doi.org/10.5194/gmd-16-7253-2023, https://doi.org/10.5194/gmd-16-7253-2023, 2023
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Simone Tilmes, Michael J. Mills, Yunqian Zhu, Charles G. Bardeen, Francis Vitt, Pengfei Yu, David Fillmore, Xiaohong Liu, Brian Toon, and Terry Deshler
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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.
Hendrik Andersen, Jan Cermak, Alyson Douglas, Timothy A. Myers, Peer Nowack, Philip Stier, Casey J. Wall, and Sarah Wilson Kemsley
Atmos. Chem. Phys., 23, 10775–10794, https://doi.org/10.5194/acp-23-10775-2023, https://doi.org/10.5194/acp-23-10775-2023, 2023
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This study uses an observation-based cloud-controlling factor framework to study near-global sensitivities of cloud radiative effects to a large number of meteorological and aerosol controls. We present near-global sensitivity patterns to selected thermodynamic, dynamic, and aerosol factors and discuss the physical mechanisms underlying the derived sensitivities. Our study hopes to guide future analyses aimed at constraining cloud feedbacks and aerosol–cloud interactions.
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.
Alan Robock, Lili Xia, Cheryl S. Harrison, Joshua Coupe, Owen B. Toon, and Charles G. Bardeen
Atmos. Chem. Phys., 23, 6691–6701, https://doi.org/10.5194/acp-23-6691-2023, https://doi.org/10.5194/acp-23-6691-2023, 2023
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A nuclear war could produce a nuclear winter, with catastrophic consequences for global food supplies. Nuclear winter theory helped to end the nuclear arms race in the 1980s, but more than 10 000 nuclear weapons still exist. This means they can be used, by unstable leaders, accidently from technical malfunctions or human error, or by terrorists. Therefore, it is urgent for scientists to study these issues, broadly communicate their results, and work for the elimination of nuclear weapons.
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.
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.
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.
Xiang Weng, Grant L. Forster, and Peer Nowack
Atmos. Chem. Phys., 22, 8385–8402, https://doi.org/10.5194/acp-22-8385-2022, https://doi.org/10.5194/acp-22-8385-2022, 2022
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We use machine learning to quantify the meteorological drivers behind surface ozone variations in China between 2015 and 2019. Our novel approaches show improved performance when compared to previous analysis methods. We highlight that nonlinearity in driver relationships and the impacts of large-scale meteorological phenomena are key to understanding ozone pollution. Moreover, we find that almost half of the observed ozone trend between 2015 and 2019 might have been driven by meteorology.
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.
Davide Zanchettin, Claudia Timmreck, Myriam Khodri, Anja Schmidt, Matthew Toohey, Manabu Abe, Slimane Bekki, Jason Cole, Shih-Wei Fang, Wuhu Feng, Gabriele Hegerl, Ben Johnson, Nicolas Lebas, Allegra N. LeGrande, Graham W. Mann, Lauren Marshall, Landon Rieger, Alan Robock, Sara Rubinetti, Kostas Tsigaridis, and Helen Weierbach
Geosci. Model Dev., 15, 2265–2292, https://doi.org/10.5194/gmd-15-2265-2022, https://doi.org/10.5194/gmd-15-2265-2022, 2022
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This paper provides metadata and first analyses of the volc-pinatubo-full experiment of CMIP6-VolMIP. Results from six Earth system models reveal significant differences in radiative flux anomalies that trace back to different implementations of volcanic forcing. Surface responses are in contrast overall consistent across models, reflecting the large spread due to internal variability. A second phase of VolMIP shall consider both aspects toward improved protocol for volc-pinatubo-full.
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.
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.
Wouter Dorigo, Irene Himmelbauer, Daniel Aberer, Lukas Schremmer, Ivana Petrakovic, Luca Zappa, Wolfgang Preimesberger, Angelika Xaver, Frank Annor, Jonas Ardö, Dennis Baldocchi, Marco Bitelli, Günter Blöschl, Heye Bogena, Luca Brocca, Jean-Christophe Calvet, J. Julio Camarero, Giorgio Capello, Minha Choi, Michael C. Cosh, Nick van de Giesen, Istvan Hajdu, Jaakko Ikonen, Karsten H. Jensen, Kasturi Devi Kanniah, Ileen de Kat, Gottfried Kirchengast, Pankaj Kumar Rai, Jenni Kyrouac, Kristine Larson, Suxia Liu, Alexander Loew, Mahta Moghaddam, José Martínez Fernández, Cristian Mattar Bader, Renato Morbidelli, Jan P. Musial, Elise Osenga, Michael A. Palecki, Thierry Pellarin, George P. Petropoulos, Isabella Pfeil, Jarrett Powers, Alan Robock, Christoph Rüdiger, Udo Rummel, Michael Strobel, Zhongbo Su, Ryan Sullivan, Torbern Tagesson, Andrej Varlagin, Mariette Vreugdenhil, Jeffrey Walker, Jun Wen, Fred Wenger, Jean Pierre Wigneron, Mel Woods, Kun Yang, Yijian Zeng, Xiang Zhang, Marek Zreda, Stephan Dietrich, Alexander Gruber, Peter van Oevelen, Wolfgang Wagner, Klaus Scipal, Matthias Drusch, and Roberto Sabia
Hydrol. Earth Syst. Sci., 25, 5749–5804, https://doi.org/10.5194/hess-25-5749-2021, https://doi.org/10.5194/hess-25-5749-2021, 2021
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The International Soil Moisture Network (ISMN) is a community-based open-access data portal for soil water measurements taken at the ground and is accessible at https://ismn.earth. Over 1000 scientific publications and thousands of users have made use of the ISMN. The scope of this paper is to inform readers about the data and functionality of the ISMN and to provide a review of the scientific progress facilitated through the ISMN with the scope to shape future research and operations.
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.
Peer Nowack, Lev Konstantinovskiy, Hannah Gardiner, and John Cant
Atmos. Meas. Tech., 14, 5637–5655, https://doi.org/10.5194/amt-14-5637-2021, https://doi.org/10.5194/amt-14-5637-2021, 2021
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Machine learning (ML) calibration techniques could be an effective way to improve the performance of low-cost air pollution sensors. Here we provide novel insights from case studies within the urban area of London, UK, where we compared the performance of three ML techniques to calibrate low-cost measurements of NO2 and PM10. In particular, we highlight the key issue of the method-dependent robustness in maintaining calibration skill after transferring sensors to different measurement sites.
Carl Thomas, Apostolos Voulgarakis, Gerald Lim, Joanna Haigh, and Peer Nowack
Weather Clim. Dynam., 2, 581–608, https://doi.org/10.5194/wcd-2-581-2021, https://doi.org/10.5194/wcd-2-581-2021, 2021
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Atmospheric blocking events are complex large-scale weather patterns which block the path of the jet stream. They are associated with heat waves in summer and cold snaps in winter. Blocking is poorly understood, and the effect of climate change is not clear. Here, we present a new method to study blocking using unsupervised machine learning. We show that this method performs better than previous methods used. These results show the potential for unsupervised learning in atmospheric science.
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.
Alexander Kuhn-Régnier, Apostolos Voulgarakis, Peer Nowack, Matthias Forkel, I. Colin Prentice, and Sandy P. Harrison
Biogeosciences, 18, 3861–3879, https://doi.org/10.5194/bg-18-3861-2021, https://doi.org/10.5194/bg-18-3861-2021, 2021
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Along with current climate, vegetation, and human influences, long-term accumulation of biomass affects fires. Here, we find that including the influence of antecedent vegetation and moisture improves our ability to predict global burnt area. Additionally, the length of the preceding period which needs to be considered for accurate predictions varies across regions.
Antara Banerjee, Amy H. Butler, Lorenzo M. Polvani, Alan Robock, Isla R. Simpson, and Lantao Sun
Atmos. Chem. Phys., 21, 6985–6997, https://doi.org/10.5194/acp-21-6985-2021, https://doi.org/10.5194/acp-21-6985-2021, 2021
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We find that simulated stratospheric sulfate geoengineering could lead to warmer Eurasian winters alongside a drier Mediterranean and wetting to the north. These effects occur due to the strengthening of the Northern Hemisphere stratospheric polar vortex, which shifts the North Atlantic Oscillation to a more positive phase. We find the effects in our simulations to be much more significant than the wintertime effects of large tropical volcanic eruptions which inject much less sulfate aerosol.
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).
James Keeble, Birgit Hassler, Antara Banerjee, Ramiro Checa-Garcia, Gabriel Chiodo, Sean Davis, Veronika Eyring, Paul T. Griffiths, Olaf Morgenstern, Peer Nowack, Guang Zeng, Jiankai Zhang, Greg Bodeker, Susannah Burrows, Philip Cameron-Smith, David Cugnet, Christopher Danek, Makoto Deushi, Larry W. Horowitz, Anne Kubin, Lijuan Li, Gerrit Lohmann, Martine Michou, Michael J. Mills, Pierre Nabat, Dirk Olivié, Sungsu Park, Øyvind Seland, Jens Stoll, Karl-Hermann Wieners, and Tongwen Wu
Atmos. Chem. Phys., 21, 5015–5061, https://doi.org/10.5194/acp-21-5015-2021, https://doi.org/10.5194/acp-21-5015-2021, 2021
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Stratospheric ozone and water vapour are key components of the Earth system; changes to both have important impacts on global and regional climate. We evaluate changes to these species from 1850 to 2100 in the new generation of CMIP6 models. There is good agreement between the multi-model mean and observations, although there is substantial variation between the individual models. The future evolution of both ozone and water vapour is strongly dependent on the assumed future emissions scenario.
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.
Andy Jones, Jim M. Haywood, Anthony C. Jones, Simone Tilmes, Ben Kravitz, and Alan Robock
Atmos. Chem. Phys., 21, 1287–1304, https://doi.org/10.5194/acp-21-1287-2021, https://doi.org/10.5194/acp-21-1287-2021, 2021
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Two different methods of simulating a geoengineering scenario are compared using data from two different Earth system models. One method is very idealised while the other includes details of a plausible mechanism. The results from both models agree that the idealised approach does not capture an impact found when detailed modelling is included, namely that geoengineering induces a positive phase of the North Atlantic Oscillation which leads to warmer, wetter winters in northern Europe.
Marc von Hobe, Felix Ploeger, Paul Konopka, Corinna Kloss, Alexey Ulanowski, Vladimir Yushkov, Fabrizio Ravegnani, C. Michael Volk, Laura L. Pan, Shawn B. Honomichl, Simone Tilmes, Douglas E. Kinnison, Rolando R. Garcia, and Jonathon S. Wright
Atmos. Chem. Phys., 21, 1267–1285, https://doi.org/10.5194/acp-21-1267-2021, https://doi.org/10.5194/acp-21-1267-2021, 2021
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The Asian summer monsoon (ASM) is known to foster transport of polluted tropospheric air into the stratosphere. To test and amend our picture of ASM vertical transport, we analyse distributions of airborne trace gas observations up to 20 km altitude near the main ASM vertical conduit south of the Himalayas. We also show that a new high-resolution version of the global chemistry climate model WACCM is able to reproduce the observations well.
Gillian Thornhill, William Collins, Dirk Olivié, Ragnhild B. Skeie, Alex Archibald, Susanne Bauer, Ramiro Checa-Garcia, Stephanie Fiedler, Gerd Folberth, Ada Gjermundsen, Larry Horowitz, Jean-Francois Lamarque, Martine Michou, Jane Mulcahy, Pierre Nabat, Vaishali Naik, Fiona M. O'Connor, Fabien Paulot, Michael Schulz, Catherine E. Scott, Roland Séférian, Chris Smith, Toshihiko Takemura, Simone Tilmes, Kostas Tsigaridis, and James Weber
Atmos. Chem. Phys., 21, 1105–1126, https://doi.org/10.5194/acp-21-1105-2021, https://doi.org/10.5194/acp-21-1105-2021, 2021
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We find that increased temperatures affect aerosols and reactive gases by changing natural emissions and their rates of removal from the atmosphere. Changing the composition of these species in the atmosphere affects the radiative budget of the climate system and therefore amplifies or dampens the climate response of climate models of the Earth system. This study found that the largest effect is a dampening of climate change as warmer temperatures increase the emissions of cooling aerosols.
Gillian D. Thornhill, William J. Collins, Ryan J. Kramer, Dirk Olivié, Ragnhild B. Skeie, Fiona M. O'Connor, Nathan Luke Abraham, Ramiro Checa-Garcia, Susanne E. Bauer, Makoto Deushi, Louisa K. Emmons, Piers M. Forster, Larry W. Horowitz, Ben Johnson, James Keeble, Jean-Francois Lamarque, Martine Michou, Michael J. Mills, Jane P. Mulcahy, Gunnar Myhre, Pierre Nabat, Vaishali Naik, Naga Oshima, Michael Schulz, Christopher J. Smith, Toshihiko Takemura, Simone Tilmes, Tongwen Wu, Guang Zeng, and Jie Zhang
Atmos. Chem. Phys., 21, 853–874, https://doi.org/10.5194/acp-21-853-2021, https://doi.org/10.5194/acp-21-853-2021, 2021
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This paper is a study of how different constituents in the atmosphere, such as aerosols and gases like methane and ozone, affect the energy balance in the atmosphere. Different climate models were run using the same inputs to allow an easy comparison of the results and to understand where the models differ. We found the effect of aerosols is to reduce warming in the atmosphere, but this effect varies between models. Reactions between gases are also important in affecting climate.
Abdul Malik, Peer J. Nowack, Joanna D. Haigh, Long Cao, Luqman Atique, and Yves Plancherel
Atmos. Chem. Phys., 20, 15461–15485, https://doi.org/10.5194/acp-20-15461-2020, https://doi.org/10.5194/acp-20-15461-2020, 2020
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Solar geoengineering has been introduced to mitigate human-caused global warming by reflecting sunlight back into space. This research investigates the impact of solar geoengineering on the tropical Pacific climate. We find that solar geoengineering can compensate some of the greenhouse-induced changes in the tropical Pacific but not all. In particular, solar geoengineering will result in significant changes in rainfall, sea surface temperatures, and increased frequency of extreme ENSO events.
Benjamin Gaubert, Louisa K. Emmons, Kevin Raeder, Simone Tilmes, Kazuyuki Miyazaki, Avelino F. Arellano Jr., Nellie Elguindi, Claire Granier, Wenfu Tang, Jérôme Barré, Helen M. Worden, Rebecca R. Buchholz, David P. Edwards, Philipp Franke, Jeffrey L. Anderson, Marielle Saunois, Jason Schroeder, Jung-Hun Woo, Isobel J. Simpson, Donald R. Blake, Simone Meinardi, Paul O. Wennberg, John Crounse, Alex Teng, Michelle Kim, Russell R. Dickerson, Hao He, Xinrong Ren, Sally E. Pusede, and Glenn S. Diskin
Atmos. Chem. Phys., 20, 14617–14647, https://doi.org/10.5194/acp-20-14617-2020, https://doi.org/10.5194/acp-20-14617-2020, 2020
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This study investigates carbon monoxide pollution in East Asia during spring using a numerical model, satellite remote sensing, and aircraft measurements. We found an underestimation of emission sources. Correcting the emission bias can improve air quality forecasting of carbon monoxide and other species including ozone. Results also suggest that controlling VOC and CO emissions, in addition to widespread NOx controls, can improve ozone pollution over East Asia.
Steven T. Turnock, Robert J. Allen, Martin Andrews, Susanne E. Bauer, Makoto Deushi, Louisa Emmons, Peter Good, Larry Horowitz, Jasmin G. John, Martine Michou, Pierre Nabat, Vaishali Naik, David Neubauer, Fiona M. O'Connor, Dirk Olivié, Naga Oshima, Michael Schulz, Alistair Sellar, Sungbo Shim, Toshihiko Takemura, Simone Tilmes, Kostas Tsigaridis, Tongwen Wu, and Jie Zhang
Atmos. Chem. Phys., 20, 14547–14579, https://doi.org/10.5194/acp-20-14547-2020, https://doi.org/10.5194/acp-20-14547-2020, 2020
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A first assessment is made of the historical and future changes in air pollutants from models participating in the 6th Coupled Model Intercomparison Project (CMIP6). Substantial benefits to future air quality can be achieved in future scenarios that implement measures to mitigate climate and involve reductions in air pollutant emissions, particularly methane. However, important differences are shown between models in the future regional projection of air pollutants under the same scenario.
Augustin Mortier, Jonas Gliß, Michael Schulz, Wenche Aas, Elisabeth Andrews, Huisheng Bian, Mian Chin, Paul Ginoux, Jenny Hand, Brent Holben, Hua Zhang, Zak Kipling, Alf Kirkevåg, Paolo Laj, Thibault Lurton, Gunnar Myhre, David Neubauer, Dirk Olivié, Knut von Salzen, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Simone Tilmes
Atmos. Chem. Phys., 20, 13355–13378, https://doi.org/10.5194/acp-20-13355-2020, https://doi.org/10.5194/acp-20-13355-2020, 2020
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We present a multiparameter analysis of the aerosol trends over the last 2 decades in the different regions of the world. In most of the regions, ground-based observations show a decrease in aerosol content in both the total atmospheric column and at the surface. The use of climate models, assessed against these observations, reveals however an increase in the total aerosol load, which is not seen with the sole use of observation due to partial coverage in space and time.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 20, 13011–13022, https://doi.org/10.5194/acp-20-13011-2020, https://doi.org/10.5194/acp-20-13011-2020, 2020
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Decadal trends and variations in OH are critical for understanding atmospheric CH4 evolution. We quantify the impacts of OH trends and variations on the CH4 budget by conducting CH4 inversions on a decadal scale with an ensemble of OH fields. We find the negative OH anomalies due to enhanced fires can reduce the optimized CH4 emissions by up to 10 Tg yr−1 during El Niño years and the positive OH trend from 1986 to 2010 results in a ∼ 23 Tg yr−1 additional increase in optimized CH4 emissions.
David S. Stevenson, Alcide Zhao, Vaishali Naik, Fiona M. O'Connor, Simone Tilmes, Guang Zeng, Lee T. Murray, William J. Collins, Paul T. Griffiths, Sungbo Shim, Larry W. Horowitz, Lori T. Sentman, and Louisa Emmons
Atmos. Chem. Phys., 20, 12905–12920, https://doi.org/10.5194/acp-20-12905-2020, https://doi.org/10.5194/acp-20-12905-2020, 2020
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We present historical trends in atmospheric oxidizing capacity (OC) since 1850 from the latest generation of global climate models and compare these with estimates from measurements. OC controls levels of many key reactive gases, including methane (CH4). We find small model trends up to 1980, then increases of about 9 % up to 2014, disagreeing with (uncertain) measurement-based trends. Major drivers of OC trends are emissions of CH4, NOx, and CO; these will be important for future CH4 trends.
Wenfu Tang, Benjamin Gaubert, Louisa Emmons, Yonghoon Choi, Joshua P. DiGangi, Glenn S. Diskin, Xiaomei Xu, Cenlin He, Helen Worden, Simone Tilmes, Rebecca Buchholz, Hannah S. Halliday, and Avelino F. Arellano
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-864, https://doi.org/10.5194/acp-2020-864, 2020
Revised manuscript not accepted
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A specific demonstration of the potential use of correlative information from carbon monoxide to refine estimates of regional carbon dioxide emissions from fossil fuel combustion.
Matt Amos, Paul J. Young, J. Scott Hosking, Jean-François Lamarque, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Markus Kunze, Marion Marchand, David A. Plummer, David Saint-Martin, Kengo Sudo, Simone Tilmes, and Yousuke Yamashita
Atmos. Chem. Phys., 20, 9961–9977, https://doi.org/10.5194/acp-20-9961-2020, https://doi.org/10.5194/acp-20-9961-2020, 2020
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We present an updated projection of Antarctic ozone hole recovery using an ensemble of chemistry–climate models. To do so, we employ a method, more advanced and skilful than the current multi-model mean standard, which is applicable to other ensemble analyses. It calculates the performance and similarity of the models, which we then use to weight the model. Calculating model similarity allows us to account for models which are constructed from similar components.
Yangyang Xu, Lei Lin, Simone Tilmes, Katherine Dagon, Lili Xia, Chenrui Diao, Wei Cheng, Zhili Wang, Isla Simpson, and Lorna Burnell
Earth Syst. Dynam., 11, 673–695, https://doi.org/10.5194/esd-11-673-2020, https://doi.org/10.5194/esd-11-673-2020, 2020
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Two geoengineering schemes to mitigate global warming, (a) capturing atmospheric CO2 and (b) injecting stratospheric sulfur gas, are compared. Based on two sets of large-ensemble model experiments, we show that sulfur injection will effectively mitigate projected terrestrial drying over the Americas, and the mitigation benefit will emerge more quickly than with carbon capture. Innovative means of sulfur injection should continue to be explored as one potential low-cost climate solution.
Ulrike Niemeier, Jadwiga H. Richter, and Simone Tilmes
Atmos. Chem. Phys., 20, 8975–8987, https://doi.org/10.5194/acp-20-8975-2020, https://doi.org/10.5194/acp-20-8975-2020, 2020
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Artificial injections of SO2 into the tropical stratosphere show an impact on the quasi-biennial oscillation (QBO). Different numerical models show only qualitatively but not quantitatively consistent impacts. We show for two models that the response of the QBO is similar when a similar stratospheric heating rate is induced by SO2 injections of different amounts. The reason is very different vertical advection in the two models resulting in different aerosol burden and heating of the aerosols.
Simone Tilmes, Douglas G. MacMartin, Jan T. M. Lenaerts, Leo van Kampenhout, Laura Muntjewerf, Lili Xia, Cheryl S. Harrison, Kristen M. Krumhardt, Michael J. Mills, Ben Kravitz, and Alan Robock
Earth Syst. Dynam., 11, 579–601, https://doi.org/10.5194/esd-11-579-2020, https://doi.org/10.5194/esd-11-579-2020, 2020
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This paper introduces new geoengineering model experiments as part of a larger model intercomparison effort, using reflective particles to block some of the incoming solar radiation to reach surface temperature targets. Outcomes of these applications are contrasted based on a high greenhouse gas emission pathway and a pathway with strong mitigation and negative emissions after 2040. We compare quantities that matter for societal and ecosystem impacts between the different scenarios.
Daniele Visioni, Giovanni Pitari, Vincenzo Rizi, Marco Iarlori, Irene Cionni, Ilaria Quaglia, Hideharu Akiyoshi, Slimane Bekki, Neal Butchart, Martin Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando Garcia, Patrick Joeckel, Douglas Kinnison, Jean-François Lamarque, Marion Marchand, Martine Michou, Olaf Morgenstern, Tatsuya Nagashima, Fiona M. O'Connor, Luke D. Oman, David Plummer, Eugene Rozanov, David Saint-Martin, Robyn Schofield, John Scinocca, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Holger Tost, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-525, https://doi.org/10.5194/acp-2020-525, 2020
Preprint withdrawn
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In this work we analyse the trend in ozone profiles taken at L'Aquila (Italy, 42.4° N) for seventeen years, between 2000 and 2016 and compare them against already available measured ozone trends. We try to understand and explain the observed trends at various heights in light of the simulations from seventeen different model, highlighting the contribution of changes in circulation and chemical ozone loss during this time period.
Alma Hodzic, Pedro Campuzano-Jost, Huisheng Bian, Mian Chin, Peter R. Colarco, Douglas A. Day, Karl D. Froyd, Bernd Heinold, Duseong S. Jo, Joseph M. Katich, John K. Kodros, Benjamin A. Nault, Jeffrey R. Pierce, Eric Ray, Jacob Schacht, Gregory P. Schill, Jason C. Schroder, Joshua P. Schwarz, Donna T. Sueper, Ina Tegen, Simone Tilmes, Kostas Tsigaridis, Pengfei Yu, and Jose L. Jimenez
Atmos. Chem. Phys., 20, 4607–4635, https://doi.org/10.5194/acp-20-4607-2020, https://doi.org/10.5194/acp-20-4607-2020, 2020
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Organic aerosol (OA) is a key source of uncertainty in aerosol climate effects. We present the first pole-to-pole OA characterization during the NASA Atmospheric Tomography aircraft mission. OA has a strong seasonal and zonal variability, with the highest levels in summer and over fire-influenced regions and the lowest ones in the southern high latitudes. We show that global models predict the OA distribution well but not the relative contribution of OA emissions vs. chemical production.
Julie M. Nicely, Bryan N. Duncan, Thomas F. Hanisco, Glenn M. Wolfe, Ross J. Salawitch, Makoto Deushi, Amund S. Haslerud, Patrick Jöckel, Béatrice Josse, Douglas E. Kinnison, Andrew Klekociuk, Michael E. Manyin, Virginie Marécal, Olaf Morgenstern, Lee T. Murray, Gunnar Myhre, Luke D. Oman, Giovanni Pitari, Andrea Pozzer, Ilaria Quaglia, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Kane Stone, Susan Strahan, Simone Tilmes, Holger Tost, Daniel M. Westervelt, and Guang Zeng
Atmos. Chem. Phys., 20, 1341–1361, https://doi.org/10.5194/acp-20-1341-2020, https://doi.org/10.5194/acp-20-1341-2020, 2020
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Differences in methane lifetime among global models are large and poorly understood. We use a neural network method and simulations from the Chemistry Climate Model Initiative to quantify the factors influencing methane lifetime spread among models and variations over time. UV photolysis, tropospheric ozone, and nitrogen oxides drive large model differences, while the same factors plus specific humidity contribute to a decreasing trend in methane lifetime between 1980 and 2015.
Elizabeth Asher, Rebecca S. Hornbrook, Britton B. Stephens, Doug Kinnison, Eric J. Morgan, Ralph F. Keeling, Elliot L. Atlas, Sue M. Schauffler, Simone Tilmes, Eric A. Kort, Martin S. Hoecker-Martínez, Matt C. Long, Jean-François Lamarque, Alfonso Saiz-Lopez, Kathryn McKain, Colm Sweeney, Alan J. Hills, and Eric C. Apel
Atmos. Chem. Phys., 19, 14071–14090, https://doi.org/10.5194/acp-19-14071-2019, https://doi.org/10.5194/acp-19-14071-2019, 2019
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Halogenated organic trace gases, which are a source of reactive halogens to the atmosphere, exert a disproportionately large influence on atmospheric chemistry and climate. This paper reports novel aircraft observations of halogenated compounds over the Southern Ocean in summer and evaluates hypothesized regional sources and emissions of these trace gases through their relationships to additional aircraft observations.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Didier A. Hauglustaine, Sophie Szopa, Ann R. Stavert, Nathan Luke Abraham, Alex T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Béatrice Josse, Douglas Kinnison, Ole Kirner, Virginie Marécal, Fiona M. O'Connor, David A. Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 19, 13701–13723, https://doi.org/10.5194/acp-19-13701-2019, https://doi.org/10.5194/acp-19-13701-2019, 2019
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The role of hydroxyl radical changes in methane trends is debated, hindering our understanding of the methane cycle. This study quantifies how uncertainties in the hydroxyl radical may influence methane abundance in the atmosphere based on the inter-model comparison of hydroxyl radical fields and model simulations of CH4 abundance with different hydroxyl radical scenarios during 2000–2016. We show that hydroxyl radical changes could contribute up to 54 % of model-simulated methane biases.
Wenxiu Sun, Peter Hess, Gang Chen, and Simone Tilmes
Atmos. Chem. Phys., 19, 12917–12933, https://doi.org/10.5194/acp-19-12917-2019, https://doi.org/10.5194/acp-19-12917-2019, 2019
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Using both observations and a chemistry climate–model we establish that in most locations changes in the waviness of the 500 hPa flow field, as measured by the local anticyclonic wave activity (AWA), explain a significant fraction of the interannual variability in surface ozone over the United States. In addition, we find that the change in AWA in a future climate (circa 2100) is predicted to cause a change in surface ozone ranging between –6 ppb and 6 ppb.
Ohad Harari, Chaim I. Garfinkel, Shlomi Ziskin Ziv, Olaf Morgenstern, Guang Zeng, Simone Tilmes, Douglas Kinnison, Makoto Deushi, Patrick Jöckel, Andrea Pozzer, Fiona M. O'Connor, and Sean Davis
Atmos. Chem. Phys., 19, 9253–9268, https://doi.org/10.5194/acp-19-9253-2019, https://doi.org/10.5194/acp-19-9253-2019, 2019
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Ozone depletion in the Antarctic has been shown to influence surface conditions, but the effects of ozone depletion in the Arctic on surface climate are unclear. We show that Arctic ozone does influence surface climate in both polar regions and tropical regions, though the proximate cause of these surface impacts is not yet clear.
Huang Yang, Darryn W. Waugh, Clara Orbe, Guang Zeng, Olaf Morgenstern, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, David A. Plummer, Patrick Jöckel, Susan E. Strahan, Kane A. Stone, and Robyn Schofield
Atmos. Chem. Phys., 19, 5511–5528, https://doi.org/10.5194/acp-19-5511-2019, https://doi.org/10.5194/acp-19-5511-2019, 2019
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We evaluate the performance of a suite of models in simulating the large-scale transport from the northern midlatitudes to the Arctic using a CO-like idealized tracer. We find a large multi-model spread of the Arctic concentration of this CO-like tracer that is well correlated with the differences in the location of the midlatitude jet as well as the northern Hadley Cell edge. Our results suggest the Hadley Cell is key and zonal-mean transport by surface meridional flow needs better constraint.
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.
Xinyi Dong, Joshua S. Fu, Qingzhao Zhu, Jian Sun, Jiani Tan, Terry Keating, Takashi Sekiya, Kengo Sudo, Louisa Emmons, Simone Tilmes, Jan Eiof Jonson, Michael Schulz, Huisheng Bian, Mian Chin, Yanko Davila, Daven Henze, Toshihiko Takemura, Anna Maria Katarina Benedictow, and Kan Huang
Atmos. Chem. Phys., 18, 15581–15600, https://doi.org/10.5194/acp-18-15581-2018, https://doi.org/10.5194/acp-18-15581-2018, 2018
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We have applied the HTAP phase II multi-model data to investigate the long-range transport impacts on surface concentration and column density of PM from Europe and Russia, Belarus, and Ukraine to eastern Asia, with a special focus on the long-range transport contribution during haze episodes in China. We found that long-range transport plays a more important role in elevating the background concentration of surface PM during the haze days.
Daniele Visioni, Giovanni Pitari, Glauco di Genova, Simone Tilmes, and Irene Cionni
Atmos. Chem. Phys., 18, 14867–14887, https://doi.org/10.5194/acp-18-14867-2018, https://doi.org/10.5194/acp-18-14867-2018, 2018
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Many side effects of sulfate geoengineering have to be analyzed before the world can even consider deploying this method of solar radiation management. In particular, we show that ice clouds in the upper troposphere are modified by a sulfate injection, producing a change that (by allowing for more planetary radiation to escape to space) would produce a further cooling. This might be important when considering the necessary amount of sulfate that needs to be injected to achieve a certain target.
Benjamin Brown-Steiner, Noelle E. Selin, Ronald Prinn, Simone Tilmes, Louisa Emmons, Jean-François Lamarque, and Philip Cameron-Smith
Geosci. Model Dev., 11, 4155–4174, https://doi.org/10.5194/gmd-11-4155-2018, https://doi.org/10.5194/gmd-11-4155-2018, 2018
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We conduct three simulations of atmospheric chemistry using chemical mechanisms of different levels of complexity and compare their results to observations. We explore situations in which the simplified mechanisms match the output of the most complex mechanism, as well as when they diverge. We investigate how concurrent utilization of chemical mechanisms of different complexities can further our atmospheric-chemistry understanding at various scales and give some strategies for future research.
Ben Kravitz, Philip J. Rasch, Hailong Wang, Alan Robock, Corey Gabriel, Olivier Boucher, Jason N. S. Cole, Jim Haywood, Duoying Ji, Andy Jones, Andrew Lenton, John C. Moore, Helene Muri, Ulrike Niemeier, Steven Phipps, Hauke Schmidt, Shingo Watanabe, Shuting Yang, and Jin-Ho Yoon
Atmos. Chem. Phys., 18, 13097–13113, https://doi.org/10.5194/acp-18-13097-2018, https://doi.org/10.5194/acp-18-13097-2018, 2018
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Marine cloud brightening has been proposed as a means of geoengineering/climate intervention, or deliberately altering the climate system to offset anthropogenic climate change. In idealized simulations that highlight contrasts between land and ocean, we find that the globe warms, including the ocean due to transport of heat from land. This study reinforces that no net energy input into the Earth system does not mean that temperature will necessarily remain unchanged.
Jiani Tan, Joshua S. Fu, Frank Dentener, Jian Sun, Louisa Emmons, Simone Tilmes, Johannes Flemming, Toshihiko Takemura, Huisheng Bian, Qingzhao Zhu, Cheng-En Yang, and Terry Keating
Atmos. Chem. Phys., 18, 12223–12240, https://doi.org/10.5194/acp-18-12223-2018, https://doi.org/10.5194/acp-18-12223-2018, 2018
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Have contributions of hemispheric air pollution to deposition at global scale been overlooked in the past years? How do we assess the critical load for the acid deposition when we look for the demand of forest and crop? This study highlights the significant impact of hemispheric transport on deposition in coastal regions, open ocean and low-emission regions. Further research is proposed for improving ecosystem and human health in these regions, with regards to the enhanced hemispheric transport.
Pakawat Phalitnonkiat, Peter G. M. Hess, Mircea D. Grigoriu, Gennady Samorodnitsky, Wenxiu Sun, Ellie Beaudry, Simone Tilmes, Makato Deushi, Beatrice Josse, David Plummer, and Kengo Sudo
Atmos. Chem. Phys., 18, 11927–11948, https://doi.org/10.5194/acp-18-11927-2018, https://doi.org/10.5194/acp-18-11927-2018, 2018
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The co-occurrence of heat waves and pollution events and the resulting high mortality rates emphasize the importance of the co-occurrence of pollution and temperature extremes. We analyze ozone and temperature extremes and their joint occurrence over the United States during the summer months (JJA) in measurement data and in model simulations of the present and future climates.
Steven T. Turnock, Oliver Wild, Frank J. Dentener, Yanko Davila, Louisa K. Emmons, Johannes Flemming, Gerd A. Folberth, Daven K. Henze, Jan E. Jonson, Terry J. Keating, Sudo Kengo, Meiyun Lin, Marianne Lund, Simone Tilmes, and Fiona M. O'Connor
Atmos. Chem. Phys., 18, 8953–8978, https://doi.org/10.5194/acp-18-8953-2018, https://doi.org/10.5194/acp-18-8953-2018, 2018
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A simple parameterisation was developed in this study to provide a rapid assessment of the impacts and uncertainties associated with future emission control strategies by predicting changes to surface ozone air quality and near-term climate forcing of ozone. Future emissions scenarios based on currently implemented legislation are shown to worsen surface ozone air quality and enhance near-term climate warming, with changes in methane becoming increasingly important in the future.
Benjamin Brown-Steiner, Noelle E. Selin, Ronald G. Prinn, Erwan Monier, Simone Tilmes, Louisa Emmons, and Fernando Garcia-Menendez
Atmos. Chem. Phys., 18, 8373–8388, https://doi.org/10.5194/acp-18-8373-2018, https://doi.org/10.5194/acp-18-8373-2018, 2018
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Detecting signals in observations and simulations of atmospheric chemistry is difficult due to the underlying variability in the chemistry, meteorology, and climatology. Here we examine the scale dependence of ozone variability and explore strategies for reducing or averaging this variability and thereby enhancing ozone signal detection capabilities. We find that 10–15 years of temporal averaging, and some level of spatial averaging, reduces the risk of overconfidence in ozone signals.
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.
Xiaokang Wu, Huang Yang, Darryn W. Waugh, Clara Orbe, Simone Tilmes, and Jean-Francois Lamarque
Atmos. Chem. Phys., 18, 7439–7452, https://doi.org/10.5194/acp-18-7439-2018, https://doi.org/10.5194/acp-18-7439-2018, 2018
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The seasonal and interannual variability of transport times from northern mid-latitudes into the southern hemisphere is examined using simulations of
agetracers. The largest variability occurs near the surface close to the tropical convergence zones, but the peak is further south and there is a smaller tropical–extratropical contrast for tracers with more rapid loss. Hence the variability of trace gases in the southern extratropics will vary with their chemical lifetime.
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.
Jiani Tan, Joshua S. Fu, Frank Dentener, Jian Sun, Louisa Emmons, Simone Tilmes, Kengo Sudo, Johannes Flemming, Jan Eiof Jonson, Sylvie Gravel, Huisheng Bian, Yanko Davila, Daven K. Henze, Marianne T. Lund, Tom Kucsera, Toshihiko Takemura, and Terry Keating
Atmos. Chem. Phys., 18, 6847–6866, https://doi.org/10.5194/acp-18-6847-2018, https://doi.org/10.5194/acp-18-6847-2018, 2018
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We study the distributions of sulfur and nitrogen deposition, which are associated with current environmental issues such as formation of acid rain and ecosystem eutrophication and result in widespread problems such as loss of environmental diversity, harming the crop yield and even food insecurity. According to our study, both the amount and distribution of sulfate and nitrogen deposition have changed significantly in the last decade, particularly in East Asia, South Asia and Southeast Asia.
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.
Daniele Visioni, Giovanni Pitari, Valentina Aquila, Simone Tilmes, Irene Cionni, Glauco Di Genova, and Eva Mancini
Atmos. Chem. Phys., 17, 11209–11226, https://doi.org/10.5194/acp-17-11209-2017, https://doi.org/10.5194/acp-17-11209-2017, 2017
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Sulfate geoengineering (SG), the sustained injection of SO2 in the lower stratosphere, is being discussed as a way to counterbalance surface warming, mimicking volcanic eruptions. In this paper, we analyse results from two models part of the GeoMIP project in order to understand the effect SG might have on the concentration and lifetime of methane, which acts in the atmosphere as a greenhouse gas. Understanding possible side effects of SG is a crucial step if its viability is to be assessed.
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.
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.
Rafael P. Fernandez, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 17, 1673–1688, https://doi.org/10.5194/acp-17-1673-2017, https://doi.org/10.5194/acp-17-1673-2017, 2017
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The inclusion of biogenic very-short lived bromine (VSLBr) in a chemistry-climate model produces an expansion of the ozone hole area of ~ 5 million km2, which is equivalent in magnitude to the recently estimated Antarctic ozone healing due to the reduction of anthropogenic CFCs and halons. The maximum Antarctic ozone hole depletion increases by up to 14 % when natural VSLBr are considered, but does not introduce a significant delay of the modelled ozone return date to 1980 October levels.
Corey J. Gabriel, Alan Robock, Lili Xia, Brian Zambri, and Ben Kravitz
Atmos. Chem. Phys., 17, 595–613, https://doi.org/10.5194/acp-17-595-2017, https://doi.org/10.5194/acp-17-595-2017, 2017
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The National Center for Atmospheric Research CESM-CAM4-CHEM global climate model was modified to simulate a scheme in which the albedo of the ocean surface is raised over the subtropical ocean gyres in the Southern Hemisphere. Global mean surface temperature in G4Foam is 0.6K lower than RCP6.0, with statistically significant cooling relative to RCP6.0 south of 30° N and an increase in rainfall over land, most pronouncedly during the JJA season, relative to both G4SSA and RCP6.0.
Camilla Weum Stjern, Bjørn Hallvard Samset, Gunnar Myhre, Huisheng Bian, Mian Chin, Yanko Davila, Frank Dentener, Louisa Emmons, Johannes Flemming, Amund Søvde Haslerud, Daven Henze, Jan Eiof Jonson, Tom Kucsera, Marianne Tronstad Lund, Michael Schulz, Kengo Sudo, Toshihiko Takemura, and Simone Tilmes
Atmos. Chem. Phys., 16, 13579–13599, https://doi.org/10.5194/acp-16-13579-2016, https://doi.org/10.5194/acp-16-13579-2016, 2016
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Air pollution can reach distant regions through intercontinental transport. Here we first present results from the Hemispheric Transport of Air Pollution Phase 2 exercise, where many models performed the same set of coordinated emission-reduction experiments. We find that mitigations have considerable extra-regional effects, and show that this is particularly true for black carbon emissions, as long-range transport elevates aerosols to higher levels where their radiative influence is stronger.
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.
Nicholas A. Davis, Dian J. Seidel, Thomas Birner, Sean M. Davis, and Simone Tilmes
Atmos. Chem. Phys., 16, 10083–10095, https://doi.org/10.5194/acp-16-10083-2016, https://doi.org/10.5194/acp-16-10083-2016, 2016
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In the Hadley cells, air rises at the Equator and sinks over the subtropics, drying the air and creating deserts on land. We investigated simple climate model experiments and found that the Hadley cells expand in response to increasing carbon dioxide. The climate of some models warms more than others, and these models also have greater Hadley cell expansion. This expansion could shift deserts toward more populated areas, with potentially major impacts on water resources and surface climate.
Sarah A. Strode, Helen M. Worden, Megan Damon, Anne R. Douglass, Bryan N. Duncan, Louisa K. Emmons, Jean-Francois Lamarque, Michael Manyin, Luke D. Oman, Jose M. Rodriguez, Susan E. Strahan, and Simone Tilmes
Atmos. Chem. Phys., 16, 7285–7294, https://doi.org/10.5194/acp-16-7285-2016, https://doi.org/10.5194/acp-16-7285-2016, 2016
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We use global models to interpret trends in MOPITT observations of CO. Simulations with time-dependent emissions reproduce the observed trends over the eastern USA and Europe, suggesting that the emissions are reasonable for these regions. The simulations produce a positive trend over eastern China, contrary to the observed negative trend. This may indicate that the assumed emission trend over China is too positive. However, large variability in the overhead ozone column also contributes.
Simone Tilmes, Jean-Francois Lamarque, Louisa K. Emmons, Doug E. Kinnison, Dan Marsh, Rolando R. Garcia, Anne K. Smith, Ryan R. Neely, Andrew Conley, Francis Vitt, Maria Val Martin, Hiroshi Tanimoto, Isobel Simpson, Don R. Blake, and Nicola Blake
Geosci. Model Dev., 9, 1853–1890, https://doi.org/10.5194/gmd-9-1853-2016, https://doi.org/10.5194/gmd-9-1853-2016, 2016
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The state of the art Community Earth System Model, CESM1 CAM4-chem has been used to perform reference and sensitivity simulations as part of the Chemistry Climate Model Initiative (CCMI). Specifics of the model and details regarding the setup of the simulations are described. In additions, the main behavior of the model, including selected chemical species have been evaluated with climatological datasets. This paper is therefore a references for studies that use the provided model results.
Peer Johannes Nowack, Nathan Luke Abraham, Peter Braesicke, and John Adrian Pyle
Atmos. Chem. Phys., 16, 4191–4203, https://doi.org/10.5194/acp-16-4191-2016, https://doi.org/10.5194/acp-16-4191-2016, 2016
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Various forms of solar radiation management (SRM) have been proposed to counteract man-made climate change. However, all these countermeasures could have unintended side-effects. We add a novel perspective to this discussion by showing how atmospheric ozone changes under solar geoengineering could affect UV exposure and air pollution. This would have implications for human health and ecology. Atmospheric composition changes are therefore important to consider in the evaluation of any SRM scheme.
L. Xia, A. Robock, S. Tilmes, and R. R. Neely III
Atmos. Chem. Phys., 16, 1479–1489, https://doi.org/10.5194/acp-16-1479-2016, https://doi.org/10.5194/acp-16-1479-2016, 2016
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Climate model simulations show that stratospheric sulfate geoengineering could impact the terrestrial carbon cycle by enhancing the carbon sink. Enhanced downward diffuse radiation, combined with cooling, could stimulate plants to grow more and absorb more carbon dioxide. This beneficial impact of stratospheric sulfate geoengineering would need to be balanced by a large number of potential risks in any future decisions about implementation of geoengineering.
X. Liu, P.-L. Ma, H. Wang, S. Tilmes, B. Singh, R. C. Easter, S. J. Ghan, and P. J. Rasch
Geosci. Model Dev., 9, 505–522, https://doi.org/10.5194/gmd-9-505-2016, https://doi.org/10.5194/gmd-9-505-2016, 2016
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In this study, we describe and evaluate a new four-mode version of the Modal Aerosol Module (MAM4) in the Community Atmosphere Model version 5 (CAM5). Compared to the current three-mode version of MAM in CAM5, MAM4 significantly improves the simulation of seasonal variation of BC concentrations in the polar regions, by increasing the BC concentrations in all seasons and particularly in cold seasons.
J. He, Y. Zhang, S. Tilmes, L. Emmons, J.-F. Lamarque, T. Glotfelty, A. Hodzic, and F. Vitt
Geosci. Model Dev., 8, 3999–4025, https://doi.org/10.5194/gmd-8-3999-2015, https://doi.org/10.5194/gmd-8-3999-2015, 2015
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The global simulations with CB05_GE and MOZART-4x predict similar chemical profiles for major gases compared to aircraft measurements, with better agreement for the NOy profile by CB05_GE. The SOA concentrations of SOA at four sites in CONUS and organic carbon over the IMPROVE sites are better predicted by MOZART-4x. The two simulations result in a global average difference of 0.5W m-2 in simulated shortwave cloud radiative forcing, with up to 13.6W m-2 over subtropical regions.
Y. Zheng, N. Unger, A. Hodzic, L. Emmons, C. Knote, S. Tilmes, J.-F. Lamarque, and P. Yu
Atmos. Chem. Phys., 15, 13487–13506, https://doi.org/10.5194/acp-15-13487-2015, https://doi.org/10.5194/acp-15-13487-2015, 2015
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Nitrogen oxides (NOx) play an important but complex role in secondary organic aerosol (SOA) formation. In this study we update the SOA scheme in a global 3-D chemistry-climate model by implementing a 4-product volatility basis set (VBS) framework with NOx-dependent yields and simplified aging parameterizations. We find that the SOA decrease in response to a 50% reduction in anthropogenic NOx emissions is limited due to the buffering in different chemical pathways.
C. J. Gabriel and A. Robock
Atmos. Chem. Phys., 15, 11949–11966, https://doi.org/10.5194/acp-15-11949-2015, https://doi.org/10.5194/acp-15-11949-2015, 2015
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This is a first look at how the El Niño/Southern Oscillation (ENSO) might change under a regime of stratospheric geoengineering (GE). We find neither ENSO event frequency nor ENSO event amplitude will be different under various GE experiments than they would under unabated global warming. We additionally find substantial disagreement between models in depicting ENSO amplitude and frequency. Additionally, output from several GCMs is excluded from comparison due to unrealistic ENSO variability.
B. Kravitz, A. Robock, S. Tilmes, O. Boucher, J. M. English, P. J. Irvine, A. Jones, M. G. Lawrence, M. MacCracken, H. Muri, J. C. Moore, U. Niemeier, S. J. Phipps, J. Sillmann, T. Storelvmo, H. Wang, and S. Watanabe
Geosci. Model Dev., 8, 3379–3392, https://doi.org/10.5194/gmd-8-3379-2015, https://doi.org/10.5194/gmd-8-3379-2015, 2015
M. Gil-Ojeda, M. Navarro-Comas, L. Gómez-Martín, J. A. Adame, A. Saiz-Lopez, C. A. Cuevas, Y. González, O. Puentedura, E. Cuevas, J.-F. Lamarque, D. Kinninson, and S. Tilmes
Atmos. Chem. Phys., 15, 10567–10579, https://doi.org/10.5194/acp-15-10567-2015, https://doi.org/10.5194/acp-15-10567-2015, 2015
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The NO2 seasonal evolution in the free troposphere (FT) has been established for the first time, based on a remote sensing technique (MAXDOAS) and thus avoiding the problems of the local pollution of in situ instruments. A clear seasonality has been found, with background levels of 20-40pptv. Evidence has been found on fast, direct injection of surface air into the free troposphere. This result might have implications on the FT distribution of halogens and other species with marine sources.
L. K. Emmons, S. R. Arnold, S. A. Monks, V. Huijnen, S. Tilmes, K. S. Law, J. L. Thomas, J.-C. Raut, I. Bouarar, S. Turquety, Y. Long, B. Duncan, S. Steenrod, S. Strode, J. Flemming, J. Mao, J. Langner, A. M. Thompson, D. Tarasick, E. C. Apel, D. R. Blake, R. C. Cohen, J. Dibb, G. S. Diskin, A. Fried, S. R. Hall, L. G. Huey, A. J. Weinheimer, A. Wisthaler, T. Mikoviny, J. Nowak, J. Peischl, J. M. Roberts, T. Ryerson, C. Warneke, and D. Helmig
Atmos. Chem. Phys., 15, 6721–6744, https://doi.org/10.5194/acp-15-6721-2015, https://doi.org/10.5194/acp-15-6721-2015, 2015
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Eleven 3-D tropospheric chemistry models have been compared and evaluated with observations in the Arctic during the International Polar Year (IPY 2008). Large differences are seen among the models, particularly related to the model chemistry of volatile organic compounds (VOCs) and reactive nitrogen (NOx, PAN, HNO3) partitioning. Consistency among the models in the underestimation of CO, ethane and propane indicates the emission inventory is too low for these compounds.
S. R. Arnold, L. K. Emmons, S. A. Monks, K. S. Law, D. A. Ridley, S. Turquety, S. Tilmes, J. L. Thomas, I. Bouarar, J. Flemming, V. Huijnen, J. Mao, B. N. Duncan, S. Steenrod, Y. Yoshida, J. Langner, and Y. Long
Atmos. Chem. Phys., 15, 6047–6068, https://doi.org/10.5194/acp-15-6047-2015, https://doi.org/10.5194/acp-15-6047-2015, 2015
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The extent to which forest fires produce the air pollutant and greenhouse gas ozone (O3) in the atmosphere at high latitudes in not well understood. We have compared how fire emissions produce O3 and its precursors in several models of atmospheric chemistry. We find enhancements in O3 in air dominated by fires in all models, which increase on average as fire emissions age. We also find that in situ O3 production in the Arctic is sensitive to details of organic chemistry and vertical lifting.
S. Tilmes, J.-F. Lamarque, L. K. Emmons, D. E. Kinnison, P.-L. Ma, X. Liu, S. Ghan, C. Bardeen, S. Arnold, M. Deeter, F. Vitt, T. Ryerson, J. W. Elkins, F. Moore, J. R. Spackman, and M. Val Martin
Geosci. Model Dev., 8, 1395–1426, https://doi.org/10.5194/gmd-8-1395-2015, https://doi.org/10.5194/gmd-8-1395-2015, 2015
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The Community Atmosphere Model (CAM), version 5, is now coupled to extensive tropospheric and stratospheric chemistry, called CAM5-chem, and is available in addition to CAM4-chem in the Community Earth System Model (CESM) version 1.2. Both configurations are well suited as tools for atmospheric chemistry modeling studies in the troposphere and lower stratosphere.
S. A. Monks, S. R. Arnold, L. K. Emmons, K. S. Law, S. Turquety, B. N. Duncan, J. Flemming, V. Huijnen, S. Tilmes, J. Langner, J. Mao, Y. Long, J. L. Thomas, S. D. Steenrod, J. C. Raut, C. Wilson, M. P. Chipperfield, G. S. Diskin, A. Weinheimer, H. Schlager, and G. Ancellet
Atmos. Chem. Phys., 15, 3575–3603, https://doi.org/10.5194/acp-15-3575-2015, https://doi.org/10.5194/acp-15-3575-2015, 2015
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Multi-model simulations of Arctic CO, O3 and OH are evaluated using observations. Models show highly variable concentrations but the relative importance of emission regions and types is robust across the models, demonstrating the importance of biomass burning as a source. Idealised tracer experiments suggest that some of the model spread is due to variations in simulated transport from Europe in winter and from Asia throughout the year.
M. Val Martin, C. L. Heald, J.-F. Lamarque, S. Tilmes, L. K. Emmons, and B. A. Schichtel
Atmos. Chem. Phys., 15, 2805–2823, https://doi.org/10.5194/acp-15-2805-2015, https://doi.org/10.5194/acp-15-2805-2015, 2015
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We present for the first time the relative effect of climate, emissions, and land use change on ozone and PM25 over the United States, focusing on the national parks. Air quality in 2050 will likely be dominated by emission patterns, but climate and land use changes alone can lead to a substantial increase in air pollution over most of the US, with important implications for O3 air quality, visibility and ecosystem health degradation in the national parks.
S. Tilmes, M. J. Mills, U. Niemeier, H. Schmidt, A. Robock, B. Kravitz, J.-F. Lamarque, G. Pitari, and J. M. English
Geosci. Model Dev., 8, 43–49, https://doi.org/10.5194/gmd-8-43-2015, https://doi.org/10.5194/gmd-8-43-2015, 2015
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A new Geoengineering Model Intercomparison Project (GeoMIP) experiment “G4 specified stratospheric aerosols” (G4SSA) is proposed to investigate the impact of stratospheric aerosol geoengineering on atmosphere, chemistry, dynamics, climate, and the environment. In contrast to the earlier G4 GeoMIP experiment, which requires an emission of sulfur dioxide (SO2) into the model, a prescribed aerosol forcing file is provided to the community, to be consistently applied to future model experiments.
A. Saiz-Lopez, R. P. Fernandez, C. Ordóñez, D. E. Kinnison, J. C. Gómez Martín, J.-F. Lamarque, and S. Tilmes
Atmos. Chem. Phys., 14, 13119–13143, https://doi.org/10.5194/acp-14-13119-2014, https://doi.org/10.5194/acp-14-13119-2014, 2014
K. Tsigaridis, N. Daskalakis, M. Kanakidou, P. J. Adams, P. Artaxo, R. Bahadur, Y. Balkanski, S. E. Bauer, N. Bellouin, A. Benedetti, T. Bergman, T. K. Berntsen, J. P. Beukes, H. Bian, K. S. Carslaw, M. Chin, G. Curci, T. Diehl, R. C. Easter, S. J. Ghan, S. L. Gong, A. Hodzic, C. R. Hoyle, T. Iversen, S. Jathar, J. L. Jimenez, J. W. Kaiser, A. Kirkevåg, D. Koch, H. Kokkola, Y. H Lee, G. Lin, X. Liu, G. Luo, X. Ma, G. W. Mann, N. Mihalopoulos, J.-J. Morcrette, J.-F. Müller, G. Myhre, S. Myriokefalitakis, N. L. Ng, D. O'Donnell, J. E. Penner, L. Pozzoli, K. J. Pringle, L. M. Russell, M. Schulz, J. Sciare, Ø. Seland, D. T. Shindell, S. Sillman, R. B. Skeie, D. Spracklen, T. Stavrakou, S. D. Steenrod, T. Takemura, P. Tiitta, S. Tilmes, H. Tost, T. van Noije, P. G. van Zyl, K. von Salzen, F. Yu, Z. Wang, Z. Wang, R. A. Zaveri, H. Zhang, K. Zhang, Q. Zhang, and X. Zhang
Atmos. Chem. Phys., 14, 10845–10895, https://doi.org/10.5194/acp-14-10845-2014, https://doi.org/10.5194/acp-14-10845-2014, 2014
A. Khodayari, S. Tilmes, S. C. Olsen, D. B. Phoenix, D. J. Wuebbles, J.-F. Lamarque, and C.-C. Chen
Atmos. Chem. Phys., 14, 9925–9939, https://doi.org/10.5194/acp-14-9925-2014, https://doi.org/10.5194/acp-14-9925-2014, 2014
K. Sindelarova, C. Granier, I. Bouarar, A. Guenther, S. Tilmes, T. Stavrakou, J.-F. Müller, U. Kuhn, P. Stefani, and W. Knorr
Atmos. Chem. Phys., 14, 9317–9341, https://doi.org/10.5194/acp-14-9317-2014, https://doi.org/10.5194/acp-14-9317-2014, 2014
A. R. Berg, C. L. Heald, K. E. Huff Hartz, A. G. Hallar, A. J. H. Meddens, J. A. Hicke, J.-F. Lamarque, and S. Tilmes
Atmos. Chem. Phys., 13, 3149–3161, https://doi.org/10.5194/acp-13-3149-2013, https://doi.org/10.5194/acp-13-3149-2013, 2013
P. J. Young, A. T. Archibald, K. W. Bowman, J.-F. Lamarque, V. Naik, D. S. Stevenson, S. Tilmes, A. Voulgarakis, O. Wild, D. Bergmann, P. Cameron-Smith, I. Cionni, W. J. Collins, S. B. Dalsøren, R. M. Doherty, V. Eyring, G. Faluvegi, L. W. Horowitz, B. Josse, Y. H. Lee, I. A. MacKenzie, T. Nagashima, D. A. Plummer, M. Righi, S. T. Rumbold, R. B. Skeie, D. T. Shindell, S. A. Strode, K. Sudo, S. Szopa, and G. Zeng
Atmos. Chem. Phys., 13, 2063–2090, https://doi.org/10.5194/acp-13-2063-2013, https://doi.org/10.5194/acp-13-2063-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Impacts of meteorology and emission reductions on haze pollution during the lockdown in the North China Plain
Impact of mineral dust on the global nitrate aerosol direct and indirect radiative effect
The surface tension and cloud condensation nuclei (CCN) activation of sea spray aerosol particles
Exploring the processes controlling secondary inorganic aerosol: evaluating the global GEOS-Chem simulation using a suite of aircraft campaigns
Influence of land cover change on atmospheric organic gases, aerosols, and radiative effects
Quantifying the impacts of marine aerosols over the southeast Atlantic Ocean using a chemical transport model: implications for aerosol–cloud interactions
Quantifying the impact of global nitrate aerosol on tropospheric composition fields and its production from lightning NOx
Driving factors of aerosol acidity: a new hierarchical quantitative analysis framework and its application in Changzhou, China
Understanding the Long-term Trend of Organic Aerosol and the Influences from Anthropogenic Emission and Regional Climate Change in China
Rapid oxidation of phenolic compounds by O3 and HO●: effects of the air–water interface and mineral dust in tropospheric chemical processes
Modeling the contribution of leads to sea spray aerosol in the high Arctic
Impacts of Sea Ice Leads on Sea Salt Aerosols and Atmospheric Chemistry in the Arctic
Importance of aerosol composition and aerosol vertical profiles in global spatial variation in the relationship between PM2.5 and aerosol optical depth
Dimethyl sulfide chemistry over the industrial era: comparison of key oxidation mechanisms and long-term observations
Population exposure to outdoor NO2, black carbon, particle mass, and number concentrations over Paris with multi-scale modelling down to the street scale
The co-benefits of a low-carbon future for PM2.5 and O3 air pollution in Europe
Assessing the effectiveness of SO2, NOx, and NH3 emission reductions in mitigating winter PM2.5 in Taiwan using CMAQ
Modelling of atmospheric concentrations of fungal spores: a 2-year simulation over France using CHIMERE
Cluster-dynamics-based parameterization for sulfuric acid–dimethylamine nucleation: comparison and selection through box and three-dimensional modeling
A Comprehensive Global Modelling Assessment of Nitrate Heterogeneous Formation on Desert Dust
Observed and CMIP6-model-simulated organic aerosol response to drought in the contiguous United States during summertime
Long-term trends in aerosol properties derived from AERONET measurements
Cooling radiative forcing effect enhancement of atmospheric amines and mineral particles caused by heterogeneous uptake and oxidation
Critical Load Exceedances for North America and Europe using an Ensemble of Models and an Investigation of Causes for Environmental Impact Estimate Variability: An AQMEII4 Study
Source-resolved atmospheric metal emissions, concentrations, and deposition fluxes into the East Asian seas
Predicted impacts of heterogeneous chemical pathways on particulate sulfur over Fairbanks, Alaska, the N. Hemisphere, and the Contiguous United States
Analysis of secondary inorganic aerosols over the greater Athens area using the EPISODE–CityChem source dispersion and photochemistry model
Global estimates of ambient reactive nitrogen components during 2000–2100 based on the multi-stage model
The role of naphthalene and its derivatives in the formation of secondary organic aerosol in the Yangtze River Delta region, China
Unveiling the optimal regression model for source apportionment of the oxidative potential of PM10
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying preexisting particles – Part 2: Modeling chemical drivers and 3-D new particle formation occurrence
Technical note: Influence of different averaging metrics and temporal resolutions on the aerosol pH calculated by thermodynamic modeling
Dual roles of the inorganic aqueous phase on secondary organic aerosol growth from benzene and phenol
Global source apportionment of aerosols into major emission regions and sectors over 1850–2017
Modeling atmospheric brown carbon in the GISS ModelE Earth system model
Observation-constrained kinetic modeling of isoprene SOA formation in the atmosphere
Significant impact of urban tree biogenic emissions on air quality estimated by a bottom-up inventory and chemistry transport modeling
Secondary organic aerosols derived from intermediate-volatility n-alkanes adopt low-viscous phase state
Modeling the drivers of fine PM pollution over Central Europe: impacts and contributions of emissions from different sources
Reaction of SO3 with H2SO4 and its implications for aerosol particle formation in the gas phase and at the air–water interface
Weakened aerosol–radiation interaction exacerbating ozone pollution in eastern China since China's clean air actions
Uncertainties from biomass burning aerosols in air quality models obscure public health impacts in Southeast Asia
Oxidative potential apportionment of atmospheric PM1: a new approach combining high-sensitive online analysers for chemical composition and offline OP measurement technique
Aqueous-phase chemistry of glyoxal with multifunctional reduced nitrogen compounds: a potential missing route for secondary brown carbon
An updated modeling framework to simulate Los Angeles air quality – Part 1: Model development, evaluation, and source apportionment
Frequent haze events associated with transport and stagnation over the corridor between the North China Plain and Yangtze River Delta
Evaluation of WRF-Chem-simulated meteorology and aerosols over northern India during the severe pollution episode of 2016
How well are aerosol–cloud interactions represented in climate models? – Part 1: Understanding the sulfate aerosol production from the 2014–15 Holuhraun eruption
pH regulates the formation of organosulfates and inorganic sulfate from organic peroxide reaction with dissolved SO2 in aquatic media
Technical note: Accurate, reliable, and high-resolution air quality predictions by improving the Copernicus Atmosphere Monitoring Service using a novel statistical post-processing method
Lang Liu, Xin Long, Yi Li, Zengliang Zang, Fengwen Wang, Yan Han, Zhier Bao, Yang Chen, Tian Feng, and Jinxin Yang
Atmos. Chem. Phys., 25, 1569–1585, https://doi.org/10.5194/acp-25-1569-2025, https://doi.org/10.5194/acp-25-1569-2025, 2025
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This study uses WRF-Chem to assess how meteorological conditions and emission reductions affected fine particulate matter (PM2.5) in the North China Plain (NCP). It highlights regional disparities: in the northern NCP, adverse weather negated emission reduction effects. In contrast, the southern NCP featured a PM2.5 decrease due to favorable weather and emission reductions. The research highlighted the interaction between emissions, meteorology, and PM2.5.
Alexandros Milousis, Klaus Klingmüller, Alexandra P. Tsimpidi, Jasper F. Kok, Maria Kanakidou, Athanasios Nenes, and Vlassis A. Karydis
Atmos. Chem. Phys., 25, 1333–1351, https://doi.org/10.5194/acp-25-1333-2025, https://doi.org/10.5194/acp-25-1333-2025, 2025
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This study investigates the impact of dust on the global radiative effect of nitrate aerosols. The results indicate both positive and negative regional shortwave and longwave radiative effects due to aerosol–radiation interactions and cloud adjustments. The global average net REari and REaci of nitrate aerosols are −0.11 and +0.17 W m−2, respectively, mainly affecting the shortwave spectrum. Sensitivity simulations evaluated the influence of mineral dust composition and emissions on the results.
Judith Kleinheins, Nadia Shardt, Ulrike Lohmann, and Claudia Marcolli
Atmos. Chem. Phys., 25, 881–903, https://doi.org/10.5194/acp-25-881-2025, https://doi.org/10.5194/acp-25-881-2025, 2025
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We model the cloud condensation nuclei (CCN) activation of sea spray aerosol particles with classical Köhler theory and with a new model approach that takes surface tension lowering into account. We categorize organic compounds into weak, intermediate, and strong surfactants, and we outline for which composition surface tension lowering is important. The results suggest that surface tension lowering allows sea spray aerosol particles in the Aitken mode to be a source of CCN in marine updraughts.
Olivia G. Norman, Colette L. Heald, Solomon Bililign, Pedro Campuzano-Jost, Hugh Coe, Marc N. Fiddler, Jaime R. Green, Jose L. Jimenez, Katharina Kaiser, Jin Liao, Ann M. Middlebrook, Benjamin A. Nault, John B. Nowak, Johannes Schneider, and André Welti
Atmos. Chem. Phys., 25, 771–795, https://doi.org/10.5194/acp-25-771-2025, https://doi.org/10.5194/acp-25-771-2025, 2025
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This study finds that one component of secondary inorganic aerosols, nitrate, is greatly overestimated by a global atmospheric chemistry model compared to observations from 11 flight campaigns. None of the loss and production pathways explored can explain the nitrate bias alone. The model’s inability to capture the variability in the observations remains and requires future investigation to avoid biases in policy-related studies (i.e., air quality, health, climate impacts of these aerosols).
Ryan Vella, Matthew Forrest, Andrea Pozzer, Alexandra P. Tsimpidi, Thomas Hickler, Jos Lelieveld, and Holger Tost
Atmos. Chem. Phys., 25, 243–262, https://doi.org/10.5194/acp-25-243-2025, https://doi.org/10.5194/acp-25-243-2025, 2025
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This study examines how land cover changes influence biogenic volatile organic compound (BVOC) emissions and atmospheric states. Using a coupled chemistry–climate–vegetation model, we compare present-day land cover (deforested for crops and grazing) with natural vegetation and an extreme reforestation scenario. We find that vegetation changes significantly impact global BVOC emissions and organic aerosols but have a relatively small effect on total aerosols, clouds, and radiative effects.
Mashiat Hossain, Rebecca M. Garland, and Hannah M. Horowitz
Atmos. Chem. Phys., 24, 14123–14143, https://doi.org/10.5194/acp-24-14123-2024, https://doi.org/10.5194/acp-24-14123-2024, 2024
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Our research examines aerosol dynamics over the southeast Atlantic, a region with significant uncertainties in aerosol radiative forcings. Using the GEOS-Chem model, we find that at cloud altitudes, organic aerosols dominate during the biomass burning season, while sulfate aerosols, driven by marine emissions, prevail during peak primary production. These findings highlight the need for accurate representation of marine aerosols in models to improve climate predictions and reduce uncertainties.
Ashok K. Luhar, Anthony C. Jones, and Jonathan M. Wilkinson
Atmos. Chem. Phys., 24, 14005–14028, https://doi.org/10.5194/acp-24-14005-2024, https://doi.org/10.5194/acp-24-14005-2024, 2024
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Nitrate aerosol is often omitted in global chemistry–climate models, partly due to the chemical complexity of its formation process. Using a global model, we show that including nitrate aerosol significantly impacts tropospheric composition fields, such as ozone, and radiation. Additionally, lightning-generated oxides of nitrogen influence both nitrate aerosol mass concentrations and aerosol size distribution, which has important implications for radiative fluxes and indirect aerosol effects.
Xiaolin Duan, Guangjie Zheng, Chuchu Chen, Qiang Zhang, and Kebin He
EGUsphere, https://doi.org/10.5194/egusphere-2024-3584, https://doi.org/10.5194/egusphere-2024-3584, 2024
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Aerosol acidity is an important parameter in atmospheric chemistry, while its driving factors, especially chemical profiles versus meteorological conditions, are not yet fully understood. Here, we established a hierarchical quantitative analysis framework to understand the driving factors of aerosol acidity on different time scales. Its application in Changzhou, China revealed distinct driving factors and corresponding mechanisms of aerosol acidity from annual trends to random residues.
Wenxin Zhang, Yaman Liu, Man Yue, Xinyi Dong, and Minghuai Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-3420, https://doi.org/10.5194/egusphere-2024-3420, 2024
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Understanding long-term organic aerosols (OA) trends and their driving factors is important for air quality management. Our modeling revealed that OA in China increased by 5.6% from 1990 to 2019, primarily due to a 32.3% increase in secondary organic aerosols (SOA) and an 8.1% decrease in primary organic aerosols (POA), both largely driven by changes in anthropogenic emissions. Biogenic SOA increased due to warming but showed little response to changes in anthropogenic nitrogen oxide emissions.
Yanru Huo, Mingxue Li, Xueyu Wang, Jianfei Sun, Yuxin Zhou, Yuhui Ma, and Maoxia He
Atmos. Chem. Phys., 24, 12409–12423, https://doi.org/10.5194/acp-24-12409-2024, https://doi.org/10.5194/acp-24-12409-2024, 2024
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This work found that the air–water (A–W) interface and TiO2 clusters promote the oxidation of phenolic compounds (PhCs) to varying degrees compared with the gas phase and bulk water. Some byproducts are more harmful than their parent compounds. This work provides important evidence for the rapid oxidation observed in O3/HO• + PhC experiments at the A–W interface and in mineral dust.
Rémy Lapere, Louis Marelle, Pierre Rampal, Laurent Brodeau, Christian Melsheimer, Gunnar Spreen, and Jennie L. Thomas
Atmos. Chem. Phys., 24, 12107–12132, https://doi.org/10.5194/acp-24-12107-2024, https://doi.org/10.5194/acp-24-12107-2024, 2024
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Elongated open-water areas in sea ice, called leads, can release marine aerosols into the atmosphere. In the Arctic, this source of atmospheric particles could play an important role for climate. However, the amount, seasonality and spatial distribution of such emissions are all mostly unknown. Here, we propose a first parameterization for sea spray aerosols emitted through leads in sea ice and quantify their impact on aerosol populations in the high Arctic.
Erin Emme and Hannah Horowitz
EGUsphere, https://doi.org/10.5194/egusphere-2024-3147, https://doi.org/10.5194/egusphere-2024-3147, 2024
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There is uncertainty in the sources of Arctic cold season (November-April) sea salt aerosols. Using a chemical transport model and satellite observations, we quantify Arctic-wide sea salt aerosol emissions from fractures in sea ice, called open sea ice leads, and their atmospheric chemistry impacts for the cold season. We show sea ice leads contribute to Arctic sea salt aerosols and bromine, especially in under-observed regions.
Haihui Zhu, Randall V. Martin, Aaron van Donkelaar, Melanie S. Hammer, Chi Li, Jun Meng, Christopher R. Oxford, Xuan Liu, Yanshun Li, Dandan Zhang, Inderjeet Singh, and Alexei Lyapustin
Atmos. Chem. Phys., 24, 11565–11584, https://doi.org/10.5194/acp-24-11565-2024, https://doi.org/10.5194/acp-24-11565-2024, 2024
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Ambient fine particulate matter (PM2.5) contributes to 4 million deaths globally each year. Satellite remote sensing of aerosol optical depth (AOD), coupled with a simulated PM2.5–AOD relationship (η), can provide global PM2.5 estimations. This study aims to understand the spatial patterns and driving factors of η to guide future measurement and modeling efforts. We quantified η globally and regionally and found that its spatial variation is strongly influenced by aerosol composition.
Ursula A. Jongebloed, Jacob I. Chalif, Linia Tashmim, William C. Porter, Kelvin H. Bates, Qianjie Chen, Erich C. Osterberg, Bess G. Koffman, Jihong Cole-Dai, Dominic A. Winksi, David G. Ferris, Karl J. Kreutz, Cameron P. Wake, and Becky Alexander
EGUsphere, https://doi.org/10.5194/egusphere-2024-3026, https://doi.org/10.5194/egusphere-2024-3026, 2024
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Marine phytoplankton emit dimethyl sulfide (DMS), which forms methanesulfonic acid (MSA) and sulfate. MSA concentrations in ice cores decreased over the industrial era, which has been attributed to pollution-driven changes in DMS chemistry. We use a models to investigate DMS chemistry compared to observations of DMS, MSA, and sulfate. We find that modeled DMS, MSA, and sulfate are influenced by pollution-sensitive oxidant concentrations, characterization of DMS chemistry, and other variables.
Soo-Jin Park, Lya Lugon, Oscar Jacquot, Youngseob Kim, Alexia Baudic, Barbara D’Anna, Ludovico Di Antonio, Claudia Di Biagio, Fabrice Dugay, Olivier Favez, Véronique Ghersi, Aline Gratien, Julien Kammer, Jean-Eudes Petit, Olivier Sanchez, Myrto Valari, Jérémy Vigneron, and Karine Sartelet
EGUsphere, https://doi.org/10.5194/egusphere-2024-2120, https://doi.org/10.5194/egusphere-2024-2120, 2024
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To accurately represent the population exposure to outdoor concentrations of pollutants of health interest (NO2, black carbon, PM2.5, ultrafine particles), multi-scale modelling down to the street scale is setup and evaluated using measurements from field campaigns. An exposure scaling factor is defined, allowing to correct regional-scale simulations to evaluate population exposure. Urban heterogeneities strongly influence NO2, black carbon and ultrafine particles, but less PM2.5.
Connor J. Clayton, Daniel R. Marsh, Steven T. Turnock, Ailish M. Graham, Kirsty J. Pringle, Carly L. Reddington, Rajesh Kumar, and James B. McQuaid
Atmos. Chem. Phys., 24, 10717–10740, https://doi.org/10.5194/acp-24-10717-2024, https://doi.org/10.5194/acp-24-10717-2024, 2024
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We demonstrate that strong climate mitigation could improve air quality in Europe; however, less ambitious mitigation does not result in these co-benefits. We use a high-resolution atmospheric chemistry model. This allows us to demonstrate how this varies across European countries and analyse the underlying chemistry. This may help policy-facing researchers understand which sectors and regions need to be prioritised to achieve strong air quality co-benefits of climate mitigation.
Ping-Chieh Huang, Hui-Ming Hung, Hsin-Chih Lai, and Charles C.-K. Chou
Atmos. Chem. Phys., 24, 10759–10772, https://doi.org/10.5194/acp-24-10759-2024, https://doi.org/10.5194/acp-24-10759-2024, 2024
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Models were used to study ways to reduce particulate matter (PM) pollution in Taiwan during winter. After considering various factors, such as physical processes and chemical reactions, we found that reducing NOx or NH3 emissions is more effective at mitigating PM2.5 than reducing SO2 emissions. When considering both efficiency and cost, reducing NH3 emissions seems to be a more suitable policy for the studied environment in Taiwan.
Matthieu Vida, Gilles Foret, Guillaume Siour, Florian Couvidat, Olivier Favez, Gaelle Uzu, Arineh Cholakian, Sébastien Conil, Matthias Beekmann, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 24, 10601–10615, https://doi.org/10.5194/acp-24-10601-2024, https://doi.org/10.5194/acp-24-10601-2024, 2024
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We simulate 2 years of atmospheric fungal spores over France and use observations of polyols and primary biogenic factors from positive matrix factorisation. The representation of emissions taking into account a proxy for vegetation surface and specific humidity enables us to reproduce very accurately the seasonal cycle of fungal spores. Furthermore, we estimate that fungal spores can account for 20 % of PM10 and 40 % of the organic fraction of PM10 over vegetated areas in summer.
Jiewen Shen, Bin Zhao, Shuxiao Wang, An Ning, Yuyang Li, Runlong Cai, Da Gao, Biwu Chu, Yang Gao, Manish Shrivastava, Jingkun Jiang, Xiuhui Zhang, and Hong He
Atmos. Chem. Phys., 24, 10261–10278, https://doi.org/10.5194/acp-24-10261-2024, https://doi.org/10.5194/acp-24-10261-2024, 2024
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We extensively compare various cluster-dynamics-based parameterizations for sulfuric acid–dimethylamine nucleation and identify a newly developed parameterization derived from Atmospheric Cluster Dynamic Code (ACDC) simulations as being the most reliable one. This study offers a valuable reference for developing parameterizations of other nucleation systems and is meaningful for the accurate quantification of the environmental and climate impacts of new particle formation.
Rubén Soussé-Villa, Oriol Jorba, María Gonçalves Ageitos, Dene Bowdalo, Marc Guevara, and Carlos Pérez García-Pando
EGUsphere, https://doi.org/10.5194/egusphere-2024-2310, https://doi.org/10.5194/egusphere-2024-2310, 2024
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Desert dust forms nitrate coatings as it travels through the atmosphere. However, current models that predict this process vary greatly due to different methods and inaccuracies. We examined how nitrate forms in a global model, focusing on how gases condense on dust, the lifespan of different particles, and the impact of alkalinity. Our findings show that models work best when they consider reversible gas condensation with alkalinity. This should lead to better estimates of climate impacts.
Wei Li and Yuxuan Wang
Atmos. Chem. Phys., 24, 9339–9353, https://doi.org/10.5194/acp-24-9339-2024, https://doi.org/10.5194/acp-24-9339-2024, 2024
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Droughts immensely increased organic aerosol (OA) in the contiguous United States in summer (1998–2019), notably in the Pacific Northwest (PNW) and Southeast (SEUS). The OA rise in the SEUS is driven by the enhanced formation of epoxydiol-derived secondary organic aerosol due to the increase in biogenic volatile organic compounds and sulfate, while in the PNW, it is caused by wildfires. A total of 10 climate models captured the OA increase in the PNW yet greatly underestimated it in the SEUS.
Zhenyu Zhang, Jing Li, Huizheng Che, Yueming Dong, Oleg Dubovik, Thomas Eck, Pawan Gupta, Brent Holben, Jhoon Kim, Elena Lind, Trailokya Saud, Sachchida Nand Tripathi, and Tong Ying
EGUsphere, https://doi.org/10.5194/egusphere-2024-2533, https://doi.org/10.5194/egusphere-2024-2533, 2024
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We used ground-based remote sensing data from the Aerosol Robotic Network to examine long-term trends in aerosol characteristics. We found aerosol loadings generally decreased globally, and aerosols became more scattering. These changes are closely related to variations in aerosol compositions, such as decreased anthropogenic emissions over East Asia, Europe, and North America, increased anthropogenic source over North India, increased dust activities over the Arabian Peninsula, etc.
Weina Zhang, Jianhua Mai, Zhichao Fan, Yongpeng Ji, Yuemeng Ji, Guiying Li, Yanpeng Gao, and Taicheng An
Atmos. Chem. Phys., 24, 9019–9030, https://doi.org/10.5194/acp-24-9019-2024, https://doi.org/10.5194/acp-24-9019-2024, 2024
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This study reveals heterogeneous oxidation causes further radiative forcing effect (RFE) enhancement of amine–mineral mixed particles. Note that RFE increment is higher under clean conditions than that under polluted conditions, which is contributed to high-oxygen-content products. The enhanced RFE of amine–mineral particles caused by heterogenous oxidation is expected to alleviate warming effects.
Paul A. Makar, Philip Cheung, Christian Hogrefe, Ayodeji Akingunola, Ummugulsum Alyuz-Ozdemir, Jesse O. Bash, Michael D. Bell, Roberto Bellasio, Roberto Bianconi, Tim Butler, Hazel Cathcart, Olivia E. Clifton, Alma Hodzic, Iannis Koutsioukis, Richard Kranenburg, Aurelia Lupascu, Jason A. Lynch, Kester Momoh, Juan L. Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Thomas Scheuschner, Mark Shephard, Ranjeet Sokhi, and Stefano Galmarini
EGUsphere, https://doi.org/10.5194/egusphere-2024-2226, https://doi.org/10.5194/egusphere-2024-2226, 2024
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The large range of sulphur and nitrogen deposition estimates from air-quality models results in a large range of predicted impacts. We used models and deposition diagnostics to identify the processes controlling atmospheric sulphur and nitrogen deposition variability. Controlling factors included the uptake of gases and aerosols by droplets, rain, snow, etc., aerosol inorganic chemistry, particle dry deposition, ammonia bidirectional fluxes, and gas deposition via plant cuticles and soil.
Shenglan Jiang, Yan Zhang, Guangyuan Yu, Zimin Han, Junri Zhao, Tianle Zhang, and Mei Zheng
Atmos. Chem. Phys., 24, 8363–8381, https://doi.org/10.5194/acp-24-8363-2024, https://doi.org/10.5194/acp-24-8363-2024, 2024
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This study aims to provide gridded data on sea-wide concentrations, deposition fluxes, and soluble deposition fluxes with detailed source categories of metals using the modified CMAQ model. We developed a monthly emission inventory of six metals – Fe, Al, V, Ni, Zn, and Cu – from terrestrial anthropogenic, ship, and dust sources in East Asia in 2017. Our results reveal the contribution of each source to the emissions, concentrations, and deposition fluxes of metals in the East Asian seas.
Sara Louise Farrell, Havala O. T. Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, and Kathleen Fahey
EGUsphere, https://doi.org/10.5194/egusphere-2024-1550, https://doi.org/10.5194/egusphere-2024-1550, 2024
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In this work we implement heterogeneous sulfur chemistry into the Community Multiscale Air Quality (CMAQ) model. This new chemistry accounts for the formation of sulfate via aqueous oxidation of SO2 in aerosol liquid water and the formation of hydroxymethanesulfonate (HMS) – often confused by measurement techniques as sulfate. Model performance in predicting sulfur PM2.5 in Fairbanks, Alaska, and other places that experience dark and cold winters, is improved.
Stelios Myriokefalitakis, Matthias Karl, Kim A. Weiss, Dimitris Karagiannis, Eleni Athanasopoulou, Anastasia Kakouri, Aikaterini Bougiatioti, Eleni Liakakou, Iasonas Stavroulas, Georgios Papangelis, Georgios Grivas, Despina Paraskevopoulou, Orestis Speyer, Nikolaos Mihalopoulos, and Evangelos Gerasopoulos
Atmos. Chem. Phys., 24, 7815–7835, https://doi.org/10.5194/acp-24-7815-2024, https://doi.org/10.5194/acp-24-7815-2024, 2024
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A state-of-the-art thermodynamic model has been coupled with the city-scale chemistry transport model EPISODE–CityChem to investigate the equilibrium between the inorganic gas and aerosol phases over the greater Athens area, Greece. The simulations indicate that the formation of nitrates in an urban environment is significantly affected by local nitrogen oxide emissions, as well as ambient temperature, relative humidity, photochemical activity, and the presence of non-volatile cations.
Rui Li, Yining Gao, Lijia Zhang, Yubing Shen, Tianzhao Xu, Wenwen Sun, and Gehui Wang
Atmos. Chem. Phys., 24, 7623–7636, https://doi.org/10.5194/acp-24-7623-2024, https://doi.org/10.5194/acp-24-7623-2024, 2024
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A three-stage model was developed to obtain the global maps of reactive nitrogen components during 2000–2100. The results implied that cross-validation R2 values of four species showed satisfactory performance (R2 > 0.55). Most reactive nitrogen components, except NH3, in China showed increases during 2000–2013. In the future scenarios, SSP3-7.0 (traditional-energy scenario) and SSP1-2.6 (carbon neutrality scenario) showed the highest and lowest reactive nitrogen component concentrations.
Fei Ye, Jingyi Li, Yaqin Gao, Hongli Wang, Jingyu An, Cheng Huang, Song Guo, Keding Lu, Kangjia Gong, Haowen Zhang, Momei Qin, and Jianlin Hu
Atmos. Chem. Phys., 24, 7467–7479, https://doi.org/10.5194/acp-24-7467-2024, https://doi.org/10.5194/acp-24-7467-2024, 2024
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Naphthalene (Nap) and methylnaphthalene (MN) are key precursors of secondary organic aerosol (SOA), yet their sources and sinks are often inadequately represented in air quality models. In this study, we incorporated detailed emissions, gas-phase chemistry, and SOA parameterization of Nap and MN into CMAQ to address this issue. The findings revealed remarkably high SOA formation potentials for these compounds despite their low emissions in the Yangtze River Delta region during summer.
Vy Dinh Ngoc Thuy, Jean-Luc Jaffrezo, Ian Hough, Pamela A. Dominutti, Guillaume Salque Moreton, Grégory Gille, Florie Francony, Arabelle Patron-Anquez, Olivier Favez, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 7261–7282, https://doi.org/10.5194/acp-24-7261-2024, https://doi.org/10.5194/acp-24-7261-2024, 2024
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The capacity of particulate matter (PM) to generate reactive oxygen species in vivo is represented by oxidative potential (OP). This study focuses on finding the appropriate model to evaluate the oxidative character of PM sources in six sites using the PM sources and OP. Eight regression techniques are introduced to assess the OP of PM. The study highlights the importance of selecting a model according to the input data characteristics and establishes some recommendations for the procedure.
Ming Chu, Xing Wei, Shangfei Hai, Yang Gao, Huiwang Gao, Yujiao Zhu, Biwu Chu, Nan Ma, Juan Hong, Yele Sun, and Xiaohong Yao
Atmos. Chem. Phys., 24, 6769–6786, https://doi.org/10.5194/acp-24-6769-2024, https://doi.org/10.5194/acp-24-6769-2024, 2024
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We used a 20-bin WRF-Chem model to simulate NPF events in the NCP during a three-week observational period in the summer of 2019. The model was able to reproduce the observations during June 29–July 6, which was characterized by a high frequency of NPF occurrence.
Haoqi Wang, Xiao Tian, Wanting Zhao, Jiacheng Li, Haoyu Yu, Yinchang Feng, and Shaojie Song
Atmos. Chem. Phys., 24, 6583–6592, https://doi.org/10.5194/acp-24-6583-2024, https://doi.org/10.5194/acp-24-6583-2024, 2024
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pH is a key property of ambient aerosols, which affect many atmospheric processes. As aerosol pH is a non-conservative parameter, diverse averaging metrics and temporal resolutions may influence the pH values calculated by thermodynamic models. This technical note seeks to quantitatively evaluate the average pH using varied metrics and resolutions. The ultimate goal is to establish standardized reporting practices in future research endeavors.
Jiwon Choi, Myoseon Jang, and Spencer Blau
Atmos. Chem. Phys., 24, 6567–6582, https://doi.org/10.5194/acp-24-6567-2024, https://doi.org/10.5194/acp-24-6567-2024, 2024
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Persistent phenoxy radical (PPR), formed by phenol gas oxidation and its aqueous reaction, catalytically destroys O3 and retards secondary organic aerosol (SOA) growth. Explicit gas mechanisms including the formation of PPR and low-volatility products from the oxidation of phenol or benzene are applied to the UNIPAR model to predict SOA mass via multiphase reactions of precursors. Aqueous reactions of reactive organics increase SOA mass but retard SOA growth via heterogeneously formed PPR.
Yang Yang, Shaoxuan Mou, Hailong Wang, Pinya Wang, Baojie Li, and Hong Liao
Atmos. Chem. Phys., 24, 6509–6523, https://doi.org/10.5194/acp-24-6509-2024, https://doi.org/10.5194/acp-24-6509-2024, 2024
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The variations in anthropogenic aerosol concentrations and source contributions and their subsequent radiative impact in major emission regions during historical periods are quantified based on an aerosol-tagging system in E3SMv1. Due to the industrial development and implementation of economic policies, sources of anthropogenic aerosols show different variations, which has important implications for pollution prevention and control measures and decision-making for global collaboration.
Maegan A. DeLessio, Kostas Tsigaridis, Susanne E. Bauer, Jacek Chowdhary, and Gregory L. Schuster
Atmos. Chem. Phys., 24, 6275–6304, https://doi.org/10.5194/acp-24-6275-2024, https://doi.org/10.5194/acp-24-6275-2024, 2024
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This study presents the first explicit representation of brown carbon aerosols in the GISS ModelE Earth system model (ESM). Model sensitivity to a range of brown carbon parameters and model performance compared to AERONET and MODIS retrievals of total aerosol properties were assessed. A summary of best practices for incorporating brown carbon into ModelE is also included.
Chuanyang Shen, Xiaoyan Yang, Joel Thornton, John Shilling, Chenyang Bi, Gabriel Isaacman-VanWertz, and Haofei Zhang
Atmos. Chem. Phys., 24, 6153–6175, https://doi.org/10.5194/acp-24-6153-2024, https://doi.org/10.5194/acp-24-6153-2024, 2024
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In this work, a condensed multiphase isoprene oxidation mechanism was developed to simulate isoprene SOA formation from chamber and field studies. Our results show that the measured isoprene SOA mass concentrations can be reasonably reproduced. The simulation results indicate that multifunctional low-volatility products contribute significantly to total isoprene SOA. Our findings emphasize that the pathways to produce these low-volatility species should be considered in models.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
Atmos. Chem. Phys., 24, 6011–6046, https://doi.org/10.5194/acp-24-6011-2024, https://doi.org/10.5194/acp-24-6011-2024, 2024
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This study presents the development of a bottom-up inventory of urban tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 %, and of ozone by 1.0 % on average over 2 months.
Tommaso Galeazzo, Bernard Aumont, Marie Camredon, Richard Valorso, Yong B. Lim, Paul J. Ziemann, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 5549–5565, https://doi.org/10.5194/acp-24-5549-2024, https://doi.org/10.5194/acp-24-5549-2024, 2024
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Secondary organic aerosol (SOA) derived from n-alkanes is a major component of anthropogenic particulate matter. We provide an analysis of n-alkane SOA by chemistry modeling, machine learning, and laboratory experiments, showing that n-alkane SOA adopts low-viscous semi-solid or liquid states. Our results indicate few kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA in large-scale atmospheric models.
Lukáš Bartík, Peter Huszár, Jan Karlický, Ondřej Vlček, and Kryštof Eben
Atmos. Chem. Phys., 24, 4347–4387, https://doi.org/10.5194/acp-24-4347-2024, https://doi.org/10.5194/acp-24-4347-2024, 2024
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The presented study deals with the attribution of fine particulate matter (PM2.5) concentrations to anthropogenic emissions over Central Europe using regional-scale models. It calculates the present-day contributions of different emissions sectors to concentrations of PM2.5 and its secondary components. Moreover, the study investigates the effect of chemical nonlinearities by using multiple source attribution methods and secondary organic aerosol calculation methods.
Rui Wang, Yang Cheng, Shasha Chen, Rongrong Li, Yue Hu, Xiaokai Guo, Tianlei Zhang, Fengmin Song, and Hao Li
Atmos. Chem. Phys., 24, 4029–4046, https://doi.org/10.5194/acp-24-4029-2024, https://doi.org/10.5194/acp-24-4029-2024, 2024
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We used quantum chemical calculations, Born–Oppenheimer molecular dynamics simulations, and the ACDC kinetic model to characterize SO3–H2SO4 interaction in the gas phase and at the air–water interface and to study the effect of H2S2O7 on H2SO4–NH3-based clusters. The work expands our understanding of new pathways for the loss of SO3 in acidic polluted areas and helps reveal some missing sources of NPF in metropolitan industrial regions and understand the atmospheric organic–sulfur cycle better.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 24, 4001–4015, https://doi.org/10.5194/acp-24-4001-2024, https://doi.org/10.5194/acp-24-4001-2024, 2024
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The present study quantifies the response of aerosol–radiation interaction (ARI) to anthropogenic emission reduction from 2013 to 2017, with the main focus on the contribution to changed O3 concentrations over eastern China both in summer and winter using the WRF-Chem model. The weakened ARI due to decreased anthropogenic emission aggravates the summer (winter) O3 pollution by +0.81 ppb (+0.63 ppb), averaged over eastern China.
Margaret R. Marvin, Paul I. Palmer, Fei Yao, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 24, 3699–3715, https://doi.org/10.5194/acp-24-3699-2024, https://doi.org/10.5194/acp-24-3699-2024, 2024
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We use an atmospheric chemistry model to investigate aerosols emitted from fire activity across Southeast Asia. We find that the limited nature of measurements in this region leads to large uncertainties that significantly hinder the model representation of these aerosols and their impacts on air quality. As a result, the number of monthly attributable deaths is underestimated by as many as 4500, particularly in March at the peak of the mainland burning season.
Julie Camman, Benjamin Chazeau, Nicolas Marchand, Amandine Durand, Grégory Gille, Ludovic Lanzi, Jean-Luc Jaffrezo, Henri Wortham, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 3257–3278, https://doi.org/10.5194/acp-24-3257-2024, https://doi.org/10.5194/acp-24-3257-2024, 2024
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Fine particle (PM1) pollution is a major health issue in the city of Marseille, which is subject to numerous pollution sources. Sampling carried out during the summer enabled a fine characterization of the PM1 sources and their oxidative potential, a promising new metric as a proxy for health impact. PM1 came mainly from combustion sources, secondary ammonium sulfate, and organic nitrate, while the oxidative potential of PM1 came from these sources and from resuspended dust in the atmosphere.
Yuemeng Ji, Zhang Shi, Wenjian Li, Jiaxin Wang, Qiuju Shi, Yixin Li, Lei Gao, Ruize Ma, Weijun Lu, Lulu Xu, Yanpeng Gao, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 3079–3091, https://doi.org/10.5194/acp-24-3079-2024, https://doi.org/10.5194/acp-24-3079-2024, 2024
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The formation mechanisms for secondary brown carbon (SBrC) contributed by multifunctional reduced nitrogen compounds (RNCs) remain unclear. Hence, from combined laboratory experiments and quantum chemical calculations, we investigated the heterogeneous reactions of glyoxal (GL) with multifunctional RNCs, which are driven by four-step indirect nucleophilic addition reactions. Our results show a possible missing source for SBrC formation on urban, regional, and global scales.
Elyse A. Pennington, Yuan Wang, Benjamin C. Schulze, Karl M. Seltzer, Jiani Yang, Bin Zhao, Zhe Jiang, Hongru Shi, Melissa Venecek, Daniel Chau, Benjamin N. Murphy, Christopher M. Kenseth, Ryan X. Ward, Havala O. T. Pye, and John H. Seinfeld
Atmos. Chem. Phys., 24, 2345–2363, https://doi.org/10.5194/acp-24-2345-2024, https://doi.org/10.5194/acp-24-2345-2024, 2024
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To assess the air quality in Los Angeles (LA), we improved the CMAQ model by using dynamic traffic emissions and new secondary organic aerosol schemes to represent volatile chemical products. Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated, with the largest sensitivity of O3 to changes in volatile organic compounds in the urban core. The improvement and remaining issues shed light on the future direction of the model development.
Feifan Yan, Hang Su, Yafang Cheng, Rujin Huang, Hong Liao, Ting Yang, Yuanyuan Zhu, Shaoqing Zhang, Lifang Sheng, Wenbin Kou, Xinran Zeng, Shengnan Xiang, Xiaohong Yao, Huiwang Gao, and Yang Gao
Atmos. Chem. Phys., 24, 2365–2376, https://doi.org/10.5194/acp-24-2365-2024, https://doi.org/10.5194/acp-24-2365-2024, 2024
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PM2.5 pollution is a major air quality issue deteriorating human health, and previous studies mostly focus on regions like the North China Plain and Yangtze River Delta. However, the characteristics of PM2.5 concentrations between these two regions are studied less often. Focusing on the transport corridor region, we identify an interesting seesaw transport phenomenon with stagnant weather conditions, conducive to PM2.5 accumulation over this region, resulting in large health effects.
Prerita Agarwal, David S. Stevenson, and Mathew R. Heal
Atmos. Chem. Phys., 24, 2239–2266, https://doi.org/10.5194/acp-24-2239-2024, https://doi.org/10.5194/acp-24-2239-2024, 2024
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Air pollution levels across northern India are amongst some of the worst in the world, with episodic and hazardous haze events. Here, the ability of the WRF-Chem model to predict air quality over northern India is assessed against several datasets. Whilst surface wind speed and particle pollution peaks are over- and underestimated, respectively, meteorology and aerosol trends are adequately captured, and we conclude it is suitable for investigating severe particle pollution events.
George Jordan, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, Anton Laakso, and James Haywood
Atmos. Chem. Phys., 24, 1939–1960, https://doi.org/10.5194/acp-24-1939-2024, https://doi.org/10.5194/acp-24-1939-2024, 2024
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The 2014–15 Holuhraun eruption caused a huge aerosol plume in an otherwise unpolluted region, providing a chance to study how aerosol alters cloud properties. This two-part study uses observations and models to quantify this relationship’s impact on the Earth’s energy budget. Part 1 suggests the models capture the observed spatial and chemical evolution of the plume, yet no model plume is exact. Understanding these differences is key for Part 2, where changes to cloud properties are explored.
Lin Du, Xiaofan Lv, Makroni Lily, Kun Li, and Narcisse Tsona Tchinda
Atmos. Chem. Phys., 24, 1841–1853, https://doi.org/10.5194/acp-24-1841-2024, https://doi.org/10.5194/acp-24-1841-2024, 2024
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This study explores the pH effect on the reaction of dissolved SO2 with selected organic peroxides. Results show that the formation of organic and/or inorganic sulfate from these peroxides strongly depends on their electronic structures, and these processes are likely to alter the chemical composition of dissolved organic matter in different ways. The rate constants of these reactions exhibit positive pH and temperature dependencies within pH 1–10 and 240–340 K ranges.
Angelo Riccio and Elena Chianese
Atmos. Chem. Phys., 24, 1673–1689, https://doi.org/10.5194/acp-24-1673-2024, https://doi.org/10.5194/acp-24-1673-2024, 2024
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Starting from the Copernicus Atmosphere Monitoring Service (CAMS), we provided a novel ensemble statistical post-processing approach to improve their air quality predictions. Our approach is able to provide reliable short-term forecasts of pollutant concentrations, which is a key challenge in supporting national authorities in their tasks related to EU Air Quality Directives, such as planning and reporting the state of air quality to the citizens.
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Short summary
Ozone is a key air pollutant. We model two geoengineering schemes, stratospheric sulfur injection and solar irradiance reduction, to compare their impacts on atmospheric ozone concentrations. With the nearly identical global mean surface temperature reduction, solar dimming increases global average surface ozone concentration, while sulfate injection decreases it. This difference is due to different stratosphere–troposphere exchange of ozone and tropospheric ozone chemistry in the two scenarios.
Ozone is a key air pollutant. We model two geoengineering schemes, stratospheric sulfur...
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