Articles | Volume 14, issue 7
https://doi.org/10.5194/acp-14-3397-2014
© Author(s) 2014. 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-14-3397-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
07 Apr 2014
Research article |
| 07 Apr 2014
Sensitivity of tropospheric chemical composition to halogen-radical chemistry using a fully coupled size-resolved multiphase chemistry–global climate system: halogen distributions, aerosol composition, and sensitivity of climate-relevant gases
M. S. Long
School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
W. C. Keene
Department of Environmental Sciences, University of Virginia, Charlottesville, VA 22904, USA
R. C. Easter
Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, Washington, USA
R. Sander
Air Chemistry Department, Max-Planck Institute of Chemistry, 55020 Mainz, Germany
Department of Atmospheric University of Wyoming, Laramie, WY 82071, USA
A. Kerkweg
Institute for Atmospheric Physics, University of Mainz, 55099 Mainz, Germany
D. Erickson
Computer Science and Mathematics Division, Oak Ridge National Laboratory, Oak Ridge, TN USA
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Duong H. Do, Astrid Kerkweg, Yarê Baker, Birger Bohn, Hendrik Fuchs, Quanfu He, Thorsten Hohaus, Sungah Kang, Timo Kirfel, Finja Löher, Niklas Diepenthal, Anke C. Nölscher, Anna Novelli, Alexander Pschera, Felix Wieser, Sören R. Zorn, Andreas Wahner, and Domenico Taraborrelli
EGUsphere, https://doi.org/10.5194/egusphere-2026-4522, https://doi.org/10.5194/egusphere-2026-4522, 2026
This preprint is open for discussion and under review for Geoscientific Model Development (GMD).
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This work builds a chamber simulation tool that mimics how air chemistry changes inside laboratory reactors, including injected gases, changing light, gas and liquid reactions, wall effects, and dilution. Tests in several chambers reproduced measured changes in reactive species, nitrogen compounds, and ozone, and helped capture how organic particles form. The same chemistry can be reused in larger, global air simulations to assess real-world impact.
Samuel Ruhl, Matthias Kohl, Rima Baalbaki, Christos Xenofontos, Ryan Vella, Sergey Gromov, Xu-Cheng He, Jiali Shen, Dina Alfaouri, Samira Atabakhsh, Lubna Dada, Jenna DeVivo, Jonathan Duplissy, Imad El Haddad, Hartwig Harder, Tuija Jokinen, Heikki Junninen, Vijay P. Kanawade, Milin K. Sebastian, Hannah Klebach, Markku Kulmala, Felix Kunkler, Jos Lelieveld, Katrianne Lehtipalo, Clara J. Lietzke, Lu Liu, Roy Mauldin, Bernhard Mentler, Ottmar Möhler, Tuukka Petäjä, Douglas M. Russell, Mario Simon, Roseline C. Thakur, Wenjuan Yu, Jiangyi Zhang, Zhensen Zheng, Jasper Kirkby, Holger Tost, Theodoros Christoudias, Rolf Sander, and Andrea Pozzer
EGUsphere, https://doi.org/10.5194/egusphere-2026-4020, https://doi.org/10.5194/egusphere-2026-4020, 2026
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Marine microbes release sulfur gases that form tiny particles able to seed clouds. Using a global chemistry-climate model, we compare four schemes for how these gases oxidise and test them against ship and ground measurements. We find that methanesulfonic acid can drive new particle formation as strongly as sulfuric acid over the cold Southern Ocean, supplying around 25 % of the cloud-forming particles there, a natural, climate-relevant source that models often overlook.
Kai Lyu, Xiaohong Liu, and Bernd Kärcher
Atmos. Chem. Phys., 25, 15369–15388, https://doi.org/10.5194/acp-25-15369-2025, https://doi.org/10.5194/acp-25-15369-2025, 2025
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Two nucleation schemes are used to study ice nucleation, focusing on three ice sources: mountains, turbulence and anvils. Ice from mountains is concentrated in mid- and high-latitudes, while ice from turbulence and anvils is more common in low and mid-latitudes. Both schemes simulate orographic cirrus clouds, with mountain ice as the dominant source. The schemes differ in how they handle ice source competition, causing turbulence and anvils to influence clouds differently.
Allen Hu, Ziming Ke, Xiaohong Liu, Benjamin Wagman, Hunter Brown, Zheng Lu, Mingxuan Wu, Hailong Wang, Qi Tang, Diana Bull, Kara Peterson, and Shaocheng Xie
Atmos. Chem. Phys., 25, 12137–12157, https://doi.org/10.5194/acp-25-12137-2025, https://doi.org/10.5194/acp-25-12137-2025, 2025
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Volcanic eruptions have major effects on atmospheric temperature and can be studied as a proxy for geo-engineering. The original aerosol module in the Energy Exascale Earth System Model v2 (E3SMv2) has problems simulating volcanic aerosols. We alter the aerosol module to simulate the 1991 Pinatubo eruption and implement a more complex chemistry scheme, producing results that better agree with observations. Process analyses of the volcanic aerosols help explain how they grow in the stratosphere.
Mingxuan Wu, Hailong Wang, Zheng Lu, Xiaohong Liu, Huisheng Bian, David D. Cohen, Yan Feng, Mian Chin, Didier A. Hauglustaine, Vlassis A. Karydis, Marianne T. Lund, Gunnar Myhre, Andrea Pozzer, Michael Schulz, Ragnhild B. Skeie, Alexandra P. Tsimpidi, Svetlana G. Tsyro, and Shaocheng Xie
Atmos. Chem. Phys., 25, 10049–10074, https://doi.org/10.5194/acp-25-10049-2025, https://doi.org/10.5194/acp-25-10049-2025, 2025
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A key challenge in simulating the life cycle of nitrate aerosol in global models is accurately representing the mass size distribution of nitrate aerosol, which lacks sufficient observational constraints. We found that most global models underestimate the mass fraction of fine-mode nitrate at the surface in all regions. Our study highlights the importance of gas–aerosol partitioning parameterization and the simulation of dust and sea salt in correctly simulating the mass size distribution of nitrate.
Raphael Dreger, Timo Kirfel, Andrea Pozzer, Simon Rosanka, Rolf Sander, and Domenico Taraborrelli
Geosci. Model Dev., 18, 4273–4291, https://doi.org/10.5194/gmd-18-4273-2025, https://doi.org/10.5194/gmd-18-4273-2025, 2025
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Model simulations are essential for understanding the interactions between atmospheric composition and weather. However, models including chemistry are very slow. Hence, any computation speedup of such models is important for understanding the role of atmospheric chemistry within the Earth system. In this study we analyzed and optimized the time step for chemistry calculations. Our results show that atmospheric models could be run notably faster without any loss in accuracy.
Ziming Ke, Qi Tang, Jean-Christophe Golaz, Xiaohong Liu, and Hailong Wang
Geosci. Model Dev., 18, 4137–4153, https://doi.org/10.5194/gmd-18-4137-2025, https://doi.org/10.5194/gmd-18-4137-2025, 2025
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This study assesses volcanic aerosol representation in E3SM (Energy Exascale Earth System Model), showing that an emission-based approach moderately improves temperature variability and cloud responses compared to a prescribed forcing approach, yet significant bias persists.
Simone T. Andersen, Rolf Sander, Patrick Dewald, Laura Wüst, Tobias Seubert, Gunther N. T. E. Türk, Jan Schuladen, Max R. McGillen, Chaoyang Xue, Abdelwahid Mellouki, Alexandre Kukui, Vincent Michoud, Manuela Cirtog, Mathieu Cazaunau, Astrid Bauville, Hichem Bouzidi, Paola Formenti, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Christopher Cantrell, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 25, 5893–5909, https://doi.org/10.5194/acp-25-5893-2025, https://doi.org/10.5194/acp-25-5893-2025, 2025
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Measurements and modelling of reactive nitrogen gases observed in a suburban temperate forest in Rambouillet, France, circa 50 km southwest of Paris in 2022 indicate that the biosphere rapidly scavenges organic nitrates of mixed biogenic and anthropogenic origin, resulting in short lifetimes for, for example, alkyl nitrates and peroxy nitrates.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, P. Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter Hess, Heikki Lihavainen, Christine Wiedinmyer, Jenny Hand, Maria Grazia Alaimo, Célia Alves, Andres Alastuey, Paulo Artaxo, Africa Barreto, Francisco Barraza, Silvia Becagli, Giulia Calzolai, Shankararaman Chellam, Ying Chen, Patrick Chuang, David D. Cohen, Cristina Colombi, Evangelia Diapouli, Gaetano Dongarra, Konstantinos Eleftheriadis, Johann Engelbrecht, Corinne Galy-Lacaux, Cassandra Gaston, Dario Gomez, Yenny González Ramos, Roy M. Harrison, Chris Heyes, Barak Herut, Philip Hopke, Christoph Hüglin, Maria Kanakidou, Zsofia Kertesz, Zbigniew Klimont, Katriina Kyllönen, Fabrice Lambert, Xiaohong Liu, Remi Losno, Franco Lucarelli, Willy Maenhaut, Beatrice Marticorena, Randall V. Martin, Nikolaos Mihalopoulos, Yasser Morera-Gómez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal L. Weagle, and Xi Zhao
Atmos. Chem. Phys., 25, 4665–4702, https://doi.org/10.5194/acp-25-4665-2025, https://doi.org/10.5194/acp-25-4665-2025, 2025
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Aerosol particles are an important part of the Earth system, but their concentrations are spatially and temporally heterogeneous, as well as being variable in size and composition. Here, we present a new compilation of PM2.5 and PM10 aerosol observations, focusing on the spatial variability across different observational stations, including composition, and demonstrate a method for comparing the data sets to model output.
Astrid Kerkweg, Timo Kirfel, Duong H. Do, Sabine Griessbach, Patrick Jöckel, and Domenico Taraborrelli
Geosci. Model Dev., 18, 1265–1286, https://doi.org/10.5194/gmd-18-1265-2025, https://doi.org/10.5194/gmd-18-1265-2025, 2025
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Normally, the Modular Earth Submodel System (MESSy) is linked to complete dynamic models to create chemical climate models. However, the modular concept of MESSy and the newly developed DWARF component presented here make it possible to create simplified models that contain only one or a few process descriptions. This is very useful for technical optimisation, such as porting to GPUs, and can be used to create less complex models, such as a chemical box model.
Kerstin Hartung, Bastian Kern, Nils-Arne Dreier, Jörn Geisbüsch, Mahnoosh Haghighatnasab, Patrick Jöckel, Astrid Kerkweg, Wilton Jaciel Loch, Florian Prill, and Daniel Rieger
Geosci. Model Dev., 18, 1001–1015, https://doi.org/10.5194/gmd-18-1001-2025, https://doi.org/10.5194/gmd-18-1001-2025, 2025
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The ICOsahedral Non-hydrostatic (ICON) model system Community Interface (ComIn) library supports connecting third-party modules to the ICON model. Third-party modules can range from simple diagnostic Python scripts to full chemistry models. ComIn offers a low barrier for code extensions to ICON, provides multi-language support (Fortran, C/C++, and Python), and reduces the migration effort in response to new ICON releases. This paper presents the ComIn design principles and a range of use cases.
Mariya Petrenko, Ralph Kahn, Mian Chin, Susanne E. Bauer, Tommi Bergman, Huisheng Bian, Gabriele Curci, Ben Johnson, Johannes W. Kaiser, Zak Kipling, Harri Kokkola, Xiaohong Liu, Keren Mezuman, Tero Mielonen, Gunnar Myhre, Xiaohua Pan, Anna Protonotariou, Samuel Remy, Ragnhild Bieltvedt Skeie, Philip Stier, Toshihiko Takemura, Kostas Tsigaridis, Hailong Wang, Duncan Watson-Parris, and Kai Zhang
Atmos. Chem. Phys., 25, 1545–1567, https://doi.org/10.5194/acp-25-1545-2025, https://doi.org/10.5194/acp-25-1545-2025, 2025
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We compared smoke plume simulations from 11 global models to each other and to satellite smoke amount observations aimed at constraining smoke source strength. In regions where plumes are thick and background aerosol is low, models and satellites compare well. However, the input emission inventory tends to underestimate in many places, and particle property and loss rate assumptions vary enormously among models, causing uncertainties that require systematic in situ measurements to resolve.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
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Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
Hunter York Brown, Benjamin Wagman, Diana Bull, Kara Peterson, Benjamin Hillman, Xiaohong Liu, Ziming Ke, and Lin Lin
Geosci. Model Dev., 17, 5087–5121, https://doi.org/10.5194/gmd-17-5087-2024, https://doi.org/10.5194/gmd-17-5087-2024, 2024
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Explosive volcanic eruptions lead to long-lived, microscopic particles in the upper atmosphere which act to cool the Earth's surface by reflecting the Sun's light back to space. We include and test this process in a global climate model, E3SM. E3SM is tested against satellite and balloon observations of the 1991 eruption of Mt. Pinatubo, showing that with these particles in the model we reasonably recreate Pinatubo and its global effects. We also explore how particle size leads to these effects.
Johannes Mülmenstädt, Edward Gryspeerdt, Sudhakar Dipu, Johannes Quaas, Andrew S. Ackerman, Ann M. Fridlind, Florian Tornow, Susanne E. Bauer, Andrew Gettelman, Yi Ming, Youtong Zheng, Po-Lun Ma, Hailong Wang, Kai Zhang, Matthew W. Christensen, Adam C. Varble, L. Ruby Leung, Xiaohong Liu, David Neubauer, Daniel G. Partridge, Philip Stier, and Toshihiko Takemura
Atmos. Chem. Phys., 24, 7331–7345, https://doi.org/10.5194/acp-24-7331-2024, https://doi.org/10.5194/acp-24-7331-2024, 2024
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Human activities release copious amounts of small particles called aerosols into the atmosphere. These particles change how much sunlight clouds reflect to space, an important human perturbation of the climate, whose magnitude is highly uncertain. We found that the latest climate models show a negative correlation but a positive causal relationship between aerosols and cloud water. This means we need to be very careful when we interpret observational studies that can only see correlation.
Felix Wieser, Rolf Sander, Changmin Cho, Hendrik Fuchs, Thorsten Hohaus, Anna Novelli, Ralf Tillmann, and Domenico Taraborrelli
Geosci. Model Dev., 17, 4311–4330, https://doi.org/10.5194/gmd-17-4311-2024, https://doi.org/10.5194/gmd-17-4311-2024, 2024
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The chemistry scheme of the atmospheric box model CAABA/MECCA is expanded to achieve an improved aerosol formation from emitted organic compounds. In addition to newly added reactions, temperature-dependent partitioning of all new species between the gas and aqueous phases is estimated and included in the pre-existing scheme. Sensitivity runs show an overestimation of key compounds from isoprene, which can be explained by a lack of aqueous-phase degradation reactions and box model limitations.
Simon Rosanka, Holger Tost, Rolf Sander, Patrick Jöckel, Astrid Kerkweg, and Domenico Taraborrelli
Geosci. Model Dev., 17, 2597–2615, https://doi.org/10.5194/gmd-17-2597-2024, https://doi.org/10.5194/gmd-17-2597-2024, 2024
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The capabilities of the Modular Earth Submodel System (MESSy) are extended to account for non-equilibrium aqueous-phase chemistry in the representation of deliquescent aerosols. When applying the new development in a global simulation, we find that MESSy's bias in modelling routinely observed reduced inorganic aerosol mass concentrations, especially in the United States. Furthermore, the representation of fine-aerosol pH is particularly improved in the marine boundary layer.
Rolf Sander
Geosci. Model Dev., 17, 2419–2425, https://doi.org/10.5194/gmd-17-2419-2024, https://doi.org/10.5194/gmd-17-2419-2024, 2024
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The open-source software MEXPLORER 1.0.0 is presented here. The program can be used to analyze, reduce, and visualize complex chemical reaction mechanisms. The mathematics behind the tool is based on graph theory: chemical species are represented as vertices, and reactions as edges. MEXPLORER is a community model published under the GNU General Public License.
Hao Wang, Xiaohong Liu, Chenglai Wu, and Guangxing Lin
Atmos. Chem. Phys., 24, 3309–3328, https://doi.org/10.5194/acp-24-3309-2024, https://doi.org/10.5194/acp-24-3309-2024, 2024
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We quantified different global- and regional-scale drivers of biogenic volatile organic compound (BVOC) emission trends over the past 20 years. The results show that global greening trends significantly boost BVOC emissions and deforestation reduces BVOC emissions in South America and Southeast Asia. Elevated temperature in Europe and increased soil moisture in East and South Asia enhance BVOC emissions. The results deepen our understanding of long-term BVOC emission trends in hotspots.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter Hess, Heikki Lihavainen, Christine Wiedinmyer, Jenny Hand, Maria Grazia Alaimo, Célia Alves, Andres Alastuey, Paulo Artaxo, Africa Barreto, Francisco Barraza, Silvia Becagli, Giulia Calzolai, Shankarararman Chellam, Ying Chen, Patrick Chuang, David D. Cohen, Cristina Colombi, Evangelia Diapouli, Gaetano Dongarra, Konstantinos Eleftheriadis, Corinne Galy-Lacaux, Cassandra Gaston, Dario Gomez, Yenny González Ramos, Hannele Hakola, Roy M. Harrison, Chris Heyes, Barak Herut, Philip Hopke, Christoph Hüglin, Maria Kanakidou, Zsofia Kertesz, Zbiginiw Klimont, Katriina Kyllönen, Fabrice Lambert, Xiaohong Liu, Remi Losno, Franco Lucarelli, Willy Maenhaut, Beatrice Marticorena, Randall V. Martin, Nikolaos Mihalopoulos, Yasser Morera-Gomez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal Weagle, and Xi Zhao
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-1, https://doi.org/10.5194/essd-2024-1, 2024
Preprint withdrawn
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Aerosol particles can interact with incoming solar radiation and outgoing long wave radiation, change cloud properties, affect photochemistry, impact surface air quality, and when deposited impact surface albedo of snow and ice, and modulate carbon dioxide uptake by the land and ocean. Here we present a new compilation of aerosol observations including composition, a methodology for comparing the datasets to model output, and show the implications of these results using one model.
Meghna Soni, Rolf Sander, Lokesh K. Sahu, Domenico Taraborrelli, Pengfei Liu, Ankit Patel, Imran A. Girach, Andrea Pozzer, Sachin S. Gunthe, and Narendra Ojha
Atmos. Chem. Phys., 23, 15165–15180, https://doi.org/10.5194/acp-23-15165-2023, https://doi.org/10.5194/acp-23-15165-2023, 2023
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The study presents the implementation of comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA. Simulations for contrasting urban environments of Asia and Europe highlight the significant impacts of chlorine on atmospheric oxidation capacity and composition. Chemical processes governing the production and loss of chlorine-containing species has been discussed. The updated chemical mechanism will be useful to interpret field measurements and for future air quality studies.
Simone Tilmes, Michael J. Mills, Yunqian Zhu, Charles G. Bardeen, Francis Vitt, Pengfei Yu, David Fillmore, Xiaohong Liu, Brian Toon, and Terry Deshler
Geosci. Model Dev., 16, 6087–6125, https://doi.org/10.5194/gmd-16-6087-2023, https://doi.org/10.5194/gmd-16-6087-2023, 2023
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We implemented an alternative aerosol scheme in the high- and low-top model versions of the Community Earth System Model Version 2 (CESM2) with a more detailed description of tropospheric and stratospheric aerosol size distributions than the existing aerosol model. This development enables the comparison of different aerosol schemes with different complexity in the same model framework. It identifies improvements compared to a range of observations in both the troposphere and stratosphere.
Rolf Sander
Atmos. Chem. Phys., 23, 10901–12440, https://doi.org/10.5194/acp-23-10901-2023, https://doi.org/10.5194/acp-23-10901-2023, 2023
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According to Henry's law, the equilibrium ratio between the abundances in the gas phase and in the aqueous phase is constant for a dilute solution. Henry’s law constants of trace gases of potential importance in environmental chemistry have been collected and converted into a uniform format. The compilation contains 46 434 values of Henry's law constants for 10 173 species, collected from 995 references. It is also available on the internet at https://www.henrys-law.org.
Roland Eichinger, Sebastian Rhode, Hella Garny, Peter Preusse, Petr Pisoft, Aleš Kuchař, Patrick Jöckel, Astrid Kerkweg, and Bastian Kern
Geosci. Model Dev., 16, 5561–5583, https://doi.org/10.5194/gmd-16-5561-2023, https://doi.org/10.5194/gmd-16-5561-2023, 2023
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The columnar approach of gravity wave (GW) schemes results in dynamical model biases, but parallel decomposition makes horizontal GW propagation computationally unfeasible. In the global model EMAC, we approximate it by GW redistribution at one altitude using tailor-made redistribution maps generated with a ray tracer. More spread-out GW drag helps reconcile the model with observations and close the 60°S GW gap. Polar vortex dynamics are improved, enhancing climate model credibility.
Longlei Li, Natalie M. Mahowald, Jasper F. Kok, Xiaohong Liu, Mingxuan Wu, Danny M. Leung, Douglas S. Hamilton, Louisa K. Emmons, Yue Huang, Neil Sexton, Jun Meng, and Jessica Wan
Geosci. Model Dev., 15, 8181–8219, https://doi.org/10.5194/gmd-15-8181-2022, https://doi.org/10.5194/gmd-15-8181-2022, 2022
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This study advances mineral dust parameterizations in the Community Atmospheric Model (CAM; version 6.1). Efforts include 1) incorporating a more physically based dust emission scheme; 2) updating the dry deposition scheme; and 3) revising the gravitational settling velocity to account for dust asphericity. Substantial improvements achieved with these updates can help accurately quantify dust–climate interactions using CAM, such as the dust-radiation and dust–cloud interactions.
Kai Zhang, Wentao Zhang, Hui Wan, Philip J. Rasch, Steven J. Ghan, Richard C. Easter, Xiangjun Shi, Yong Wang, Hailong Wang, Po-Lun Ma, Shixuan Zhang, Jian Sun, Susannah M. Burrows, Manish Shrivastava, Balwinder Singh, Yun Qian, Xiaohong Liu, Jean-Christophe Golaz, Qi Tang, Xue Zheng, Shaocheng Xie, Wuyin Lin, Yan Feng, Minghuai Wang, Jin-Ho Yoon, and L. Ruby Leung
Atmos. Chem. Phys., 22, 9129–9160, https://doi.org/10.5194/acp-22-9129-2022, https://doi.org/10.5194/acp-22-9129-2022, 2022
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Here we analyze the effective aerosol forcing simulated by E3SM version 1 using both century-long free-running and short nudged simulations. The aerosol forcing in E3SMv1 is relatively large compared to other models, mainly due to the large indirect aerosol effect. Aerosol-induced changes in liquid and ice cloud properties in E3SMv1 have a strong correlation. The aerosol forcing estimates in E3SMv1 are sensitive to the parameterization changes in both liquid and ice cloud processes.
Matthias Karl, Liisa Pirjola, Tiia Grönholm, Mona Kurppa, Srinivasan Anand, Xiaole Zhang, Andreas Held, Rolf Sander, Miikka Dal Maso, David Topping, Shuai Jiang, Leena Kangas, and Jaakko Kukkonen
Geosci. Model Dev., 15, 3969–4026, https://doi.org/10.5194/gmd-15-3969-2022, https://doi.org/10.5194/gmd-15-3969-2022, 2022
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The community aerosol dynamics model MAFOR includes several advanced features: coupling with an up-to-date chemistry mechanism for volatile organic compounds, a revised Brownian coagulation kernel that takes into account the fractal geometry of soot particles, a multitude of nucleation parameterizations, size-resolved partitioning of semi-volatile inorganics, and a hybrid method for the formation of secondary organic aerosols within the framework of condensation and evaporation.
Susannah M. Burrows, Richard C. Easter, Xiaohong Liu, Po-Lun Ma, Hailong Wang, Scott M. Elliott, Balwinder Singh, Kai Zhang, and Philip J. Rasch
Atmos. Chem. Phys., 22, 5223–5251, https://doi.org/10.5194/acp-22-5223-2022, https://doi.org/10.5194/acp-22-5223-2022, 2022
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Sea spray particles are composed of a mixture of salts and organic substances from oceanic microorganisms. In prior work, our team developed an approach connecting sea spray chemistry to ocean biology, called OCEANFILMS. Here we describe its implementation within an Earth system model, E3SM. We show that simulated sea spray chemistry is consistent with observed seasonal cycles and that sunlight reflected by simulated Southern Ocean clouds increases, consistent with analysis of satellite data.
Po-Lun Ma, Bryce E. Harrop, Vincent E. Larson, Richard B. Neale, Andrew Gettelman, Hugh Morrison, Hailong Wang, Kai Zhang, Stephen A. Klein, Mark D. Zelinka, Yuying Zhang, Yun Qian, Jin-Ho Yoon, Christopher R. Jones, Meng Huang, Sheng-Lun Tai, Balwinder Singh, Peter A. Bogenschutz, Xue Zheng, Wuyin Lin, Johannes Quaas, Hélène Chepfer, Michael A. Brunke, Xubin Zeng, Johannes Mülmenstädt, Samson Hagos, Zhibo Zhang, Hua Song, Xiaohong Liu, Michael S. Pritchard, Hui Wan, Jingyu Wang, Qi Tang, Peter M. Caldwell, Jiwen Fan, Larry K. Berg, Jerome D. Fast, Mark A. Taylor, Jean-Christophe Golaz, Shaocheng Xie, Philip J. Rasch, and L. Ruby Leung
Geosci. Model Dev., 15, 2881–2916, https://doi.org/10.5194/gmd-15-2881-2022, https://doi.org/10.5194/gmd-15-2881-2022, 2022
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An alternative set of parameters for E3SM Atmospheric Model version 1 has been developed based on a tuning strategy that focuses on clouds. When clouds in every regime are improved, other aspects of the model are also improved, even though they are not the direct targets for calibration. The recalibrated model shows a lower sensitivity to anthropogenic aerosols and surface warming, suggesting potential improvements to the simulated climate in the past and future.
Andrea Pozzer, Simon F. Reifenberg, Vinod Kumar, Bruno Franco, Matthias Kohl, Domenico Taraborrelli, Sergey Gromov, Sebastian Ehrhart, Patrick Jöckel, Rolf Sander, Veronica Fall, Simon Rosanka, Vlassis Karydis, Dimitris Akritidis, Tamara Emmerichs, Monica Crippa, Diego Guizzardi, Johannes W. Kaiser, Lieven Clarisse, Astrid Kiendler-Scharr, Holger Tost, and Alexandra Tsimpidi
Geosci. Model Dev., 15, 2673–2710, https://doi.org/10.5194/gmd-15-2673-2022, https://doi.org/10.5194/gmd-15-2673-2022, 2022
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A newly developed setup of the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) is evaluated here. A comprehensive organic degradation mechanism is used and coupled with a volatility base model.
The results show that the model reproduces most of the tracers and aerosols satisfactorily but shows discrepancies for oxygenated organic gases. It is also shown that this model configuration can be used for further research in atmospheric chemistry.
Yang Shi, Xiaohong Liu, Mingxuan Wu, Xi Zhao, Ziming Ke, and Hunter Brown
Atmos. Chem. Phys., 22, 2909–2935, https://doi.org/10.5194/acp-22-2909-2022, https://doi.org/10.5194/acp-22-2909-2022, 2022
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We perform a modeling study to evaluate the contribution to Arctic dust loading and ice-nucleating particle (INP) population from high-latitude local and low-latitude dust. High-latitude dust has a large contribution in the lower troposphere, while low-latitude dust dominates the upper troposphere. The high-latitude dust INPs result in a net cooling effect on the Arctic surface by glaciating mixed-phase clouds. Our results highlight the contribution of high-latitude dust to the Arctic climate.
Xi Zhao and Xiaohong Liu
Atmos. Chem. Phys., 22, 2585–2600, https://doi.org/10.5194/acp-22-2585-2022, https://doi.org/10.5194/acp-22-2585-2022, 2022
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The goal of this study is to investigate the relative importance and interactions of primary and secondary ice production in the Arctic mixed-phase clouds. Our results show that the SIP is not only a result of ice crystals produced from ice nucleation, but also competes with the ice production; conversely, strong ice nucleation also suppresses SIP.
Ka Ming Fung, Colette L. Heald, Jesse H. Kroll, Siyuan Wang, Duseong S. Jo, Andrew Gettelman, Zheng Lu, Xiaohong Liu, Rahul A. Zaveri, Eric C. Apel, Donald R. Blake, Jose-Luis Jimenez, Pedro Campuzano-Jost, Patrick R. Veres, Timothy S. Bates, John E. Shilling, and Maria Zawadowicz
Atmos. Chem. Phys., 22, 1549–1573, https://doi.org/10.5194/acp-22-1549-2022, https://doi.org/10.5194/acp-22-1549-2022, 2022
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Understanding the natural aerosol burden in the preindustrial era is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of dimethyl sulfide (DMS) oxidation (implemented in the Community Atmospheric Model version 6 with chemistry, CAM6-chem) could help us better estimate the present-day and preindustrial concentrations of sulfate and other relevant chemicals, as well as the resulting aerosol radiative impacts.
Zhonghua Zheng, Matthew West, Lei Zhao, Po-Lun Ma, Xiaohong Liu, and Nicole Riemer
Atmos. Chem. Phys., 21, 17727–17741, https://doi.org/10.5194/acp-21-17727-2021, https://doi.org/10.5194/acp-21-17727-2021, 2021
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Aerosol mixing state is an important emergent property that affects aerosol radiative forcing and aerosol–cloud interactions, but it has not been easy to constrain this property globally. We present a framework for evaluating the error in aerosol mixing state induced by aerosol representation assumptions, which is one of the important contributors to structural uncertainty in aerosol models. Our study provides insights into potential improvements to model process representation for aerosols.
Philipp G. Eger, Luc Vereecken, Rolf Sander, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Ville Vakkari, Tuukka Petäjä, Jos Lelieveld, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 21, 14333–14349, https://doi.org/10.5194/acp-21-14333-2021, https://doi.org/10.5194/acp-21-14333-2021, 2021
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We determine the impact of pyruvic acid photolysis on the formation of acetaldehyde and peroxy radicals during summer and autumn in the Finnish boreal forest using a data-constrained box model. Our results are dependent on the chosen scenario in which the overall quantum yield and the photolysis products are varied. We highlight that pyruvic acid photolysis can be an important contributor to acetaldehyde and peroxy radical formation in remote, forested regions.
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