Articles | Volume 24, issue 19
https://doi.org/10.5194/acp-24-11365-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-24-11365-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
11 Oct 2024
Research article |
| 11 Oct 2024
| 11 Oct 2024
Global modeling of aerosol nucleation with a semi-explicit chemical mechanism for highly oxygenated organic molecules (HOMs)
Xinyue Shao
School of Atmospheric Science, Nanjing University, Nanjing, 210023, China
Joint International Research Laboratory of Atmospheric and Earth System Sciences & Institute for Climate and Global Change Research, Nanjing University, Nanjing, 210023, China
School of Atmospheric Science, Nanjing University, Nanjing, 210023, China
Joint International Research Laboratory of Atmospheric and Earth System Sciences & Institute for Climate and Global Change Research, Nanjing University, Nanjing, 210023, China
School of Atmospheric Science, Nanjing University, Nanjing, 210023, China
Joint International Research Laboratory of Atmospheric and Earth System Sciences & Institute for Climate and Global Change Research, Nanjing University, Nanjing, 210023, China
Frontiers Science Center for Critical Earth Material Cycling, Nanjing University, Nanjing, China
Yaman Liu
School of Atmospheric Science, Nanjing University, Nanjing, 210023, China
Zhejiang Institute of Meteorological Sciences, Hangzhou, 310008, China
Wenxiang Shen
School of Atmospheric Science, Nanjing University, Nanjing, 210023, China
Joint International Research Laboratory of Atmospheric and Earth System Sciences & Institute for Climate and Global Change Research, Nanjing University, Nanjing, 210023, China
Stephen R. Arnold
Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK
Leighton A. Regayre
Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK
Met Office Hadley Centre, Exeter, Fitzroy Road, Exeter, Devon, EX1 3PB, UK
Centre for Environmental Modelling and Computation, School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK
Meinrat O. Andreae
Max Planck Institute for Chemistry, 55020 Mainz, Germany
Scripps Institution of Oceanography, University of California, San Diego, La Jolla, CA, USA
Mira L. Pöhlker
Max Planck Institute for Chemistry, 55020 Mainz, Germany
Leipzig Institute for Meteorology, Universität Leipzig, 04103 Leipzig, Germany
Experimental Aerosol and Cloud Microphysics Department, Leibniz Institute for Tropospheric Research, 04318 Leipzig, Germany
Duseong S. Jo
Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO 80103, USA
now at: Department of Earth System Science Education, Seoul National University, Seoul, 999 007, South Korea
School of Atmospheric Science, Nanjing University, Nanjing, 210023, China
Zhejiang Institute of Meteorological Sciences, Hangzhou, 310008, China
Ken S. Carslaw
Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK
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David P. Edwards, Sara Martínez-Alonso, Duseong S. Jo, Ivan Ortega, Louisa K. Emmons, John J. Orlando, Helen M. Worden, Jhoon Kim, Hanlim Lee, Junsung Park, and Hyunkee Hong
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Until recently, satellite observations of atmospheric pollutants at any location could only be obtained once a day. New geostationary satellites stare at a region of the Earth to make hourly measurements, and the Geostationary Environment Monitoring Spectrometer is the first looking at Asia. These data and model simulations show how the change seen for one important pollutant that determines air quality depends on a combination of pollution emissions, atmospheric chemistry, and meteorology.
Luiz A. T. Machado, Jürgen Kesselmeier, Santiago Botía, Hella van Asperen, Meinrat O. Andreae, Alessandro C. de Araújo, Paulo Artaxo, Achim Edtbauer, Rosaria R. Ferreira, Marco A. Franco, Hartwig Harder, Sam P. Jones, Cléo Q. Dias-Júnior, Guido G. Haytzmann, Carlos A. Quesada, Shujiro Komiya, Jost Lavric, Jos Lelieveld, Ingeborg Levin, Anke Nölscher, Eva Pfannerstill, Mira L. Pöhlker, Ulrich Pöschl, Akima Ringsdorf, Luciana Rizzo, Ana M. Yáñez-Serrano, Susan Trumbore, Wanda I. D. Valenti, Jordi Vila-Guerau de Arellano, David Walter, Jonathan Williams, Stefan Wolff, and Christopher Pöhlker
Atmos. Chem. Phys., 24, 8893–8910, https://doi.org/10.5194/acp-24-8893-2024, https://doi.org/10.5194/acp-24-8893-2024, 2024
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Composite analysis of gas concentration before and after rainfall, during the day and night, gives insight into the complex relationship between trace gas variability and precipitation. The analysis helps us to understand the sources and sinks of trace gases within a forest ecosystem. It elucidates processes that are not discernible under undisturbed conditions and contributes to a deeper understanding of the trace gas life cycle and its intricate interactions with cloud dynamics in the Amazon.
Marco A. Franco, Rafael Valiati, Bruna A. Holanda, Bruno B. Meller, Leslie A. Kremper, Luciana V. Rizzo, Samara Carbone, Fernando G. Morais, Janaína P. Nascimento, Meinrat O. Andreae, Micael A. Cecchini, Luiz A. T. Machado, Milena Ponczek, Ulrich Pöschl, David Walter, Christopher Pöhlker, and Paulo Artaxo
Atmos. Chem. Phys., 24, 8751–8770, https://doi.org/10.5194/acp-24-8751-2024, https://doi.org/10.5194/acp-24-8751-2024, 2024
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The Amazon wet-season atmosphere was studied at the Amazon Tall Tower Observatory site, revealing vertical variations (between 60 and 325 m) in natural aerosols. Daytime mixing contrasted with nighttime stratification, with distinct rain-induced changes in aerosol populations. Notably, optical property recovery at higher levels was faster, while near-canopy aerosols showed higher scattering efficiency. These findings enhance our understanding of aerosol impacts on climate dynamics.
Yawen Liu, Yun Qian, Philip J. Rasch, Kai Zhang, Lai-yung Ruby Leung, Yuhang Wang, Minghuai Wang, Hailong Wang, Xin Huang, and Xiu-Qun Yang
Atmos. Chem. Phys., 24, 3115–3128, https://doi.org/10.5194/acp-24-3115-2024, https://doi.org/10.5194/acp-24-3115-2024, 2024
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Fire management has long been a challenge. Here we report that spring-peak fire activity over southern Mexico and Central America (SMCA) has a distinct quasi-biennial signal by measuring multiple fire metrics. This signal is initially driven by quasi-biennial variability in precipitation and is further amplified by positive feedback of fire–precipitation interaction at short timescales. This work highlights the importance of fire–climate interactions in shaping fires on an interannual scale.
Adrien Deroubaix, Marco Vountas, Benjamin Gaubert, Maria Dolores Andrés Hernández, Stephan Borrmann, Guy Brasseur, Bruna Holanda, Yugo Kanaya, Katharina Kaiser, Flora Kluge, Ovid Oktavian Krüger, Inga Labuhn, Michael Lichtenstern, Klaus Pfeilsticker, Mira Pöhlker, Hans Schlager, Johannes Schneider, Guillaume Siour, Basudev Swain, Paolo Tuccella, Kameswara S. Vinjamuri, Mihalis Vrekoussis, Benjamin Weyland, and John P. Burrows
EGUsphere, https://doi.org/10.5194/egusphere-2024-516, https://doi.org/10.5194/egusphere-2024-516, 2024
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This study assesses atmospheric composition using air quality models during aircraft campaigns in Europe and Asia, focusing on carbonaceous aerosols and trace gases. While carbon monoxide is well modeled, other pollutants have moderate to weak agreement with observations. Wind speed modeling is reliable for identifying pollution plumes, where models tend to overestimate concentrations. This highlights challenges in accurately modeling aerosol and trace gas composition, particularly in cities.
Adrien Deroubaix, Marco Vountas, Benjamin Gaubert, Maria Dolores Andrés Hernández, Stephan Borrmann, Guy Brasseur, Bruna Holanda, Yugo Kanaya, Katharina Kaiser, Flora Kluge, Ovid Oktavian Krüger, Inga Labuhn, Michael Lichtenstern, Klaus Pfeilsticker, Mira Pöhlker, Hans Schlager, Johannes Schneider, Guillaume Siour, Basudev Swain, Paolo Tuccella, Kameswara S. Vinjamuri, Mihalis Vrekoussis, Benjamin Weyland, and John P. Burrows
EGUsphere, https://doi.org/10.5194/egusphere-2024-521, https://doi.org/10.5194/egusphere-2024-521, 2024
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This study explores the proportional relationships between carbonaceous aerosols (black and organic carbon) and trace gases using airborne measurements from two campaigns in Europe and East Asia. Differences between regions were found, but air quality models struggled to reproduce them accurately. We show that these proportional relationships can help to constrain models and can be used to infer aerosol concentrations from satellite observations of trace gases, especially in urban areas.
Victoria A. Flood, Kimberly Strong, Cynthia H. Whaley, Kaley A. Walker, Thomas Blumenstock, James W. Hannigan, Johan Mellqvist, Justus Notholt, Mathias Palm, Amelie N. Röhling, Stephen Arnold, Stephen Beagley, Rong-You Chien, Jesper Christensen, Makoto Deushi, Srdjan Dobricic, Xinyi Dong, Joshua S. Fu, Michael Gauss, Wanmin Gong, Joakim Langner, Kathy S. Law, Louis Marelle, Tatsuo Onishi, Naga Oshima, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Manu A. Thomas, Svetlana Tsyro, and Steven Turnock
Atmos. Chem. Phys., 24, 1079–1118, https://doi.org/10.5194/acp-24-1079-2024, https://doi.org/10.5194/acp-24-1079-2024, 2024
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It is important to understand the composition of the Arctic atmosphere and how it is changing. Atmospheric models provide simulations that can inform policy. This study examines simulations of CH4, CO, and O3 by 11 models. Model performance is assessed by comparing results matched in space and time to measurements from five high-latitude ground-based infrared spectrometers. This work finds that models generally underpredict the concentrations of these gases in the Arctic troposphere.
Rolf Müller, Ulrich Pöschl, Thomas Koop, Thomas Peter, and Ken Carslaw
Atmos. Chem. Phys., 23, 15445–15453, https://doi.org/10.5194/acp-23-15445-2023, https://doi.org/10.5194/acp-23-15445-2023, 2023
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Paul J. Crutzen was a pioneer in atmospheric sciences and a kind-hearted, humorous person with empathy for the private lives of his colleagues and students. He made fundamental scientific contributions to a wide range of scientific topics in all parts of the atmosphere. Paul was among the founders of the journal Atmospheric Chemistry and Physics. His work will continue to be a guide for generations of scientists and environmental policymakers to come.
Hamza Ahsan, Hailong Wang, Jingbo Wu, Mingxuan Wu, Steven J. Smith, Susanne Bauer, Harrison Suchyta, Dirk Olivié, Gunnar Myhre, Hitoshi Matsui, Huisheng Bian, Jean-François Lamarque, Ken Carslaw, Larry Horowitz, Leighton Regayre, Mian Chin, Michael Schulz, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Vaishali Naik
Atmos. Chem. Phys., 23, 14779–14799, https://doi.org/10.5194/acp-23-14779-2023, https://doi.org/10.5194/acp-23-14779-2023, 2023
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We examine the impact of the assumed effective height of SO2 injection, SO2 and BC emission seasonality, and the assumed fraction of SO2 emissions injected as SO4 on climate and chemistry model results. We find that the SO2 injection height has a large impact on surface SO2 concentrations and, in some models, radiative flux. These assumptions are a
hiddensource of inter-model variability and may be leading to bias in some climate model results.
Da Lu, Hao Li, Mengke Tian, Guochen Wang, Xiaofei Qin, Na Zhao, Juntao Huo, Fan Yang, Yanfen Lin, Jia Chen, Qingyan Fu, Yusen Duan, Xinyi Dong, Congrui Deng, Sabur F. Abdullaev, and Kan Huang
Atmos. Chem. Phys., 23, 13853–13868, https://doi.org/10.5194/acp-23-13853-2023, https://doi.org/10.5194/acp-23-13853-2023, 2023
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Environmental conditions during dust are usually not favorable for secondary aerosol formation. However in this study, an unusual dust event was captured in a Chinese mega-city and showed “anomalous” meteorology and a special dust backflow transport pathway. The underlying formation mechanisms of secondary aerosols are probed in the context of this special dust event. This study shows significant implications for the varying dust aerosol chemistry in the future changing climate.
Richard J. Pope, Brian J. Kerridge, Martyn P. Chipperfield, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Matilda A. Pimlott, Wuhu Feng, Edward Comyn-Platt, Garry D. Hayman, Stephen R. Arnold, and Ailish M. Graham
Atmos. Chem. Phys., 23, 13235–13253, https://doi.org/10.5194/acp-23-13235-2023, https://doi.org/10.5194/acp-23-13235-2023, 2023
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In the summer of 2018, Europe experienced several persistent large-scale ozone (O3) pollution episodes. Satellite tropospheric O3 and surface O3 data recorded substantial enhancements in 2018 relative to other years. Targeted model simulations showed that meteorological processes and emissions controlled the elevated surface O3, while mid-tropospheric O3 enhancements were dominated by stratospheric O3 intrusion and advection of North Atlantic O3-rich air masses into Europe.
Xurong Wang, Qiaoqiao Wang, Maria Prass, Christopher Pöhlker, Daniel Moran-Zuloaga, Paulo Artaxo, Jianwei Gu, Ning Yang, Xiajie Yang, Jiangchuan Tao, Juan Hong, Nan Ma, Yafang Cheng, Hang Su, and Meinrat O. Andreae
Atmos. Chem. Phys., 23, 9993–10014, https://doi.org/10.5194/acp-23-9993-2023, https://doi.org/10.5194/acp-23-9993-2023, 2023
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In this work, with an optimized particle mass size distribution, we captured observed aerosol optical depth (AOD) and coarse aerosol concentrations over source and/or receptor regions well, demonstrating good performance in simulating export of African dust toward the Amazon Basin. In addition to factors controlling the transatlantic transport of African dust, the study investigated the impact of African dust over the Amazon Basin, including the nutrient inputs associated with dust deposition.
Leighton A. Regayre, Lucia Deaconu, Daniel P. Grosvenor, David M. H. Sexton, Christopher Symonds, Tom Langton, Duncan Watson-Paris, Jane P. Mulcahy, Kirsty J. Pringle, Mark Richardson, Jill S. Johnson, John W. Rostron, Hamish Gordon, Grenville Lister, Philip Stier, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 8749–8768, https://doi.org/10.5194/acp-23-8749-2023, https://doi.org/10.5194/acp-23-8749-2023, 2023
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Aerosol forcing of Earth’s energy balance has persisted as a major cause of uncertainty in climate simulations over generations of climate model development. We show that structural deficiencies in a climate model are exposed by comprehensively exploring parametric uncertainty and that these deficiencies limit how much the model uncertainty can be reduced through observational constraint. This provides a future pathway towards building models with greater physical realism and lower uncertainty.
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.
Daniel P. Grosvenor and Kenneth S. Carslaw
Atmos. Chem. Phys., 23, 6743–6773, https://doi.org/10.5194/acp-23-6743-2023, https://doi.org/10.5194/acp-23-6743-2023, 2023
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We determine what causes long-term trends in short-wave (SW) radiative fluxes in two climate models. A positive trend occurs between 1850 and 1970 (increasing SW reflection) and a negative trend between 1970 and 2014; the pre-1970 positive trend is mainly driven by an increase in cloud droplet number concentrations due to increases in aerosol, and the 1970–2014 trend is driven by a decrease in cloud fraction, which we attribute to changes in clouds caused by greenhouse gas-induced warming.
Ernesto Reyes-Villegas, Douglas Lowe, Jill S. Johnson, Kenneth S. Carslaw, Eoghan Darbyshire, Michael Flynn, James D. Allan, Hugh Coe, Ying Chen, Oliver Wild, Scott Archer-Nicholls, Alex Archibald, Siddhartha Singh, Manish Shrivastava, Rahul A. Zaveri, Vikas Singh, Gufran Beig, Ranjeet Sokhi, and Gordon McFiggans
Atmos. Chem. Phys., 23, 5763–5782, https://doi.org/10.5194/acp-23-5763-2023, https://doi.org/10.5194/acp-23-5763-2023, 2023
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Organic aerosols (OAs), their sources and their processes remain poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem, can be a useful tool to describe primary OA (POA) production and aging. However, the main disadvantage is its complexity. We used a Gaussian process simulator to reproduce model results and to estimate the sources of model uncertainty. We do this by comparing the outputs with OA observations made at Delhi, India, in 2018.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
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The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Xuemei Wang, Hamish Gordon, Daniel P. Grosvenor, Meinrat O. Andreae, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 4431–4461, https://doi.org/10.5194/acp-23-4431-2023, https://doi.org/10.5194/acp-23-4431-2023, 2023
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New particle formation in the upper troposphere is important for the global boundary layer aerosol population, and they can be transported downward in Amazonia. We use a global and a regional model to quantify the number of aerosols that are formed at high altitude and transported downward in a 1000 km region. We find that the majority of the aerosols are from outside the region. This suggests that the 1000 km region is unlikely to be a
closed loopfor aerosol formation, transport and growth.
Ruth Price, Andrea Baccarini, Julia Schmale, Paul Zieger, Ian M. Brooks, Paul Field, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 2927–2961, https://doi.org/10.5194/acp-23-2927-2023, https://doi.org/10.5194/acp-23-2927-2023, 2023
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Arctic clouds can control how much energy is absorbed by the surface or reflected back to space. Using a computer model of the atmosphere we investigated the formation of atmospheric particles that allow cloud droplets to form. We found that particles formed aloft are transported to the lowest part of the Arctic atmosphere and that this is a key source of particles. Our results have implications for the way Arctic clouds will behave in the future as climate change continues to impact the region.
Haley M. Royer, Mira L. Pöhlker, Ovid Krüger, Edmund Blades, Peter Sealy, Nurun Nahar Lata, Zezhen Cheng, Swarup China, Andrew P. Ault, Patricia K. Quinn, Paquita Zuidema, Christopher Pöhlker, Ulrich Pöschl, Meinrat Andreae, and Cassandra J. Gaston
Atmos. Chem. Phys., 23, 981–998, https://doi.org/10.5194/acp-23-981-2023, https://doi.org/10.5194/acp-23-981-2023, 2023
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This paper presents atmospheric particle chemical composition and measurements of aerosol water uptake properties collected at Ragged Point, Barbados, during the winter of 2020. The result of this study indicates the importance of small African smoke particles for cloud droplet formation in the tropical North Atlantic and highlights the large spatial and temporal pervasiveness of smoke over the Atlantic Ocean.
Cynthia H. Whaley, Kathy S. Law, Jens Liengaard Hjorth, Henrik Skov, Stephen R. Arnold, Joakim Langner, Jakob Boyd Pernov, Garance Bergeron, Ilann Bourgeois, Jesper H. Christensen, Rong-You Chien, Makoto Deushi, Xinyi Dong, Peter Effertz, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Greg Huey, Ulas Im, Rigel Kivi, Louis Marelle, Tatsuo Onishi, Naga Oshima, Irina Petropavlovskikh, Jeff Peischl, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Tom Ryerson, Ragnhild Skeie, Sverre Solberg, Manu A. Thomas, Chelsea Thompson, Kostas Tsigaridis, Svetlana Tsyro, Steven T. Turnock, Knut von Salzen, and David W. Tarasick
Atmos. Chem. Phys., 23, 637–661, https://doi.org/10.5194/acp-23-637-2023, https://doi.org/10.5194/acp-23-637-2023, 2023
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This study summarizes recent research on ozone in the Arctic, a sensitive and rapidly warming region. We find that the seasonal cycles of near-surface atmospheric ozone are variable depending on whether they are near the coast, inland, or at high altitude. Several global model simulations were evaluated, and we found that because models lack some of the ozone chemistry that is important for the coastal Arctic locations, they do not accurately simulate ozone there.
Yunfan Liu, Hang Su, Siwen Wang, Chao Wei, Wei Tao, Mira L. Pöhlker, Christopher Pöhlker, Bruna A. Holanda, Ovid O. Krüger, Thorsten Hoffmann, Manfred Wendisch, Paulo Artaxo, Ulrich Pöschl, Meinrat O. Andreae, and Yafang Cheng
Atmos. Chem. Phys., 23, 251–272, https://doi.org/10.5194/acp-23-251-2023, https://doi.org/10.5194/acp-23-251-2023, 2023
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The origins of the abundant cloud condensation nuclei (CCN) in the upper troposphere (UT) of the Amazon remain unclear. With model developments of new secondary organic aerosol schemes and constrained by observation, we show that strong aerosol nucleation and condensation in the UT is triggered by biogenic organics, and organic condensation is key for UT CCN production. This UT CCN-producing mechanism may prevail over broader vegetation canopies and deserves emphasis in aerosol–climate feedback.
Leighton A. Regayre, Lucia Deaconu, Daniel P. Grosvenor, David Sexton, Christopher C. Symonds, Tom Langton, Duncan Watson-Paris, Jane P. Mulcahy, Kirsty J. Pringle, Mark Richardson, Jill S. Johnson, John Rostron, Hamish Gordon, Grenville Lister, Philip Stier, and Ken S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2022-1330, https://doi.org/10.5194/egusphere-2022-1330, 2022
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We show that potential structural deficiencies in a climate model can be exposed by comprehensively exploring its parametric uncertainty, and that these deficiencies limit how much the model uncertainty can be reduced through observational constraint. Combined consideration of parametric and structural uncertainties provides a future pathway towards building models that have greater physical realism and lower uncertainty.
Ville Leinonen, Harri Kokkola, Taina Yli-Juuti, Tero Mielonen, Thomas Kühn, Tuomo Nieminen, Simo Heikkinen, Tuuli Miinalainen, Tommi Bergman, Ken Carslaw, Stefano Decesari, Markus Fiebig, Tareq Hussein, Niku Kivekäs, Radovan Krejci, Markku Kulmala, Ari Leskinen, Andreas Massling, Nikos Mihalopoulos, Jane P. Mulcahy, Steffen M. Noe, Twan van Noije, Fiona M. O'Connor, Colin O'Dowd, Dirk Olivie, Jakob B. Pernov, Tuukka Petäjä, Øyvind Seland, Michael Schulz, Catherine E. Scott, Henrik Skov, Erik Swietlicki, Thomas Tuch, Alfred Wiedensohler, Annele Virtanen, and Santtu Mikkonen
Atmos. Chem. Phys., 22, 12873–12905, https://doi.org/10.5194/acp-22-12873-2022, https://doi.org/10.5194/acp-22-12873-2022, 2022
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We provide the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five different earth system models. We investigated aerosol modes (nucleation, Aitken, and accumulation) separately and were able to show the differences between measured and modeled trends and especially their seasonal patterns. The differences in model results are likely due to complex effects of several processes instead of certain specific model features.
Charlotte M. Beall, Thomas C. J. Hill, Paul J. DeMott, Tobias Köneman, Michael Pikridas, Frank Drewnick, Hartwig Harder, Christopher Pöhlker, Jos Lelieveld, Bettina Weber, Minas Iakovides, Roman Prokeš, Jean Sciare, Meinrat O. Andreae, M. Dale Stokes, and Kimberly A. Prather
Atmos. Chem. Phys., 22, 12607–12627, https://doi.org/10.5194/acp-22-12607-2022, https://doi.org/10.5194/acp-22-12607-2022, 2022
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Ice-nucleating particles (INPs) are rare aerosols that can trigger ice formation in clouds and affect climate-relevant cloud properties such as phase, reflectivity and lifetime. Dust is the dominant INP source, yet few measurements have been reported near major dust sources. We report INP observations within hundreds of kilometers of the biggest dust source regions globally: the Sahara and the Arabian Peninsula. Results show that at temperatures > −15 °C, INPs are dominated by organics.
Amy H. Peace, Ben B. B. Booth, Leighton A. Regayre, Ken S. Carslaw, David M. H. Sexton, Céline J. W. Bonfils, and John W. Rostron
Earth Syst. Dynam., 13, 1215–1232, https://doi.org/10.5194/esd-13-1215-2022, https://doi.org/10.5194/esd-13-1215-2022, 2022
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Anthropogenic aerosol emissions have been linked to driving climate responses such as shifts in the location of tropical rainfall. However, the interaction of aerosols with climate remains one of the most uncertain aspects of climate modelling and limits our ability to predict future climate change. We use an ensemble of climate model simulations to investigate what impact the large uncertainty in how aerosols interact with climate has on predicting future tropical rainfall shifts.
Alexander D. Harrison, Daniel O'Sullivan, Michael P. Adams, Grace C. E. Porter, Edmund Blades, Cherise Brathwaite, Rebecca Chewitt-Lucas, Cassandra Gaston, Rachel Hawker, Ovid O. Krüger, Leslie Neve, Mira L. Pöhlker, Christopher Pöhlker, Ulrich Pöschl, Alberto Sanchez-Marroquin, Andrea Sealy, Peter Sealy, Mark D. Tarn, Shanice Whitehall, James B. McQuaid, Kenneth S. Carslaw, Joseph M. Prospero, and Benjamin J. Murray
Atmos. Chem. Phys., 22, 9663–9680, https://doi.org/10.5194/acp-22-9663-2022, https://doi.org/10.5194/acp-22-9663-2022, 2022
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The formation of ice in clouds fundamentally alters cloud properties; hence it is important we understand the special aerosol particles that can nucleate ice when immersed in supercooled cloud droplets. In this paper we show that African desert dust that has travelled across the Atlantic to the Caribbean nucleates ice much less well than we might have expected.
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.
Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons
Atmos. Chem. Phys., 22, 5775–5828, https://doi.org/10.5194/acp-22-5775-2022, https://doi.org/10.5194/acp-22-5775-2022, 2022
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Air pollutants, like ozone and soot, play a role in both global warming and air quality. Atmospheric models are often used to provide information to policy makers about current and future conditions under different emissions scenarios. In order to have confidence in those simulations, in this study we compare simulated air pollution from 18 state-of-the-art atmospheric models to measured air pollution in order to assess how well the models perform.
Hannah Walker, Daniel Stone, Trevor Ingham, Sina Hackenberg, Danny Cryer, Shalini Punjabi, Katie Read, James Lee, Lisa Whalley, Dominick V. Spracklen, Lucy J. Carpenter, Steve R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 22, 5535–5557, https://doi.org/10.5194/acp-22-5535-2022, https://doi.org/10.5194/acp-22-5535-2022, 2022
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Glyoxal is a ubiquitous reactive organic compound in the atmosphere, which may form organic aerosol and impact the atmosphere's oxidising capacity. There are limited measurements of glyoxal's abundance in the remote marine atmosphere. We made new measurements of glyoxal using a highly sensitive technique over two 4-week periods in the tropical Atlantic atmosphere. We show that daytime measurements are mostly consistent with our chemical understanding but a potential missing source at night.
Hanna K. Lappalainen, Tuukka Petäjä, Timo Vihma, Jouni Räisänen, Alexander Baklanov, Sergey Chalov, Igor Esau, Ekaterina Ezhova, Matti Leppäranta, Dmitry Pozdnyakov, Jukka Pumpanen, Meinrat O. Andreae, Mikhail Arshinov, Eija Asmi, Jianhui Bai, Igor Bashmachnikov, Boris Belan, Federico Bianchi, Boris Biskaborn, Michael Boy, Jaana Bäck, Bin Cheng, Natalia Chubarova, Jonathan Duplissy, Egor Dyukarev, Konstantinos Eleftheriadis, Martin Forsius, Martin Heimann, Sirkku Juhola, Vladimir Konovalov, Igor Konovalov, Pavel Konstantinov, Kajar Köster, Elena Lapshina, Anna Lintunen, Alexander Mahura, Risto Makkonen, Svetlana Malkhazova, Ivan Mammarella, Stefano Mammola, Stephany Buenrostro Mazon, Outi Meinander, Eugene Mikhailov, Victoria Miles, Stanislav Myslenkov, Dmitry Orlov, Jean-Daniel Paris, Roberta Pirazzini, Olga Popovicheva, Jouni Pulliainen, Kimmo Rautiainen, Torsten Sachs, Vladimir Shevchenko, Andrey Skorokhod, Andreas Stohl, Elli Suhonen, Erik S. Thomson, Marina Tsidilina, Veli-Pekka Tynkkynen, Petteri Uotila, Aki Virkkula, Nadezhda Voropay, Tobias Wolf, Sayaka Yasunaka, Jiahua Zhang, Yubao Qiu, Aijun Ding, Huadong Guo, Valery Bondur, Nikolay Kasimov, Sergej Zilitinkevich, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 22, 4413–4469, https://doi.org/10.5194/acp-22-4413-2022, https://doi.org/10.5194/acp-22-4413-2022, 2022
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We summarize results during the last 5 years in the northern Eurasian region, especially from Russia, and introduce recent observations of the air quality in the urban environments in China. Although the scientific knowledge in these regions has increased, there are still gaps in our understanding of large-scale climate–Earth surface interactions and feedbacks. This arises from limitations in research infrastructures and integrative data analyses, hindering a comprehensive system analysis.
Richard J. Pope, Rebecca Kelly, Eloise A. Marais, Ailish M. Graham, Chris Wilson, Jeremy J. Harrison, Savio J. A. Moniz, Mohamed Ghalaieny, Steve R. Arnold, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 4323–4338, https://doi.org/10.5194/acp-22-4323-2022, https://doi.org/10.5194/acp-22-4323-2022, 2022
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Nitrogen oxides (NOx) are potent air pollutants which directly impact on human health. In this study, we use satellite nitrogen dioxide (NO2) data to evaluate the spatial distribution and temporal evolution of the UK official NOx emissions inventory, with reasonable agreement. We also derived satellite-based NOx emissions for several UK cities. In the case of London and Birmingham, the NAEI NOx emissions are potentially too low by >50%.
Marco A. Franco, Florian Ditas, Leslie A. Kremper, Luiz A. T. Machado, Meinrat O. Andreae, Alessandro Araújo, Henrique M. J. Barbosa, Joel F. de Brito, Samara Carbone, Bruna A. Holanda, Fernando G. Morais, Janaína P. Nascimento, Mira L. Pöhlker, Luciana V. Rizzo, Marta Sá, Jorge Saturno, David Walter, Stefan Wolff, Ulrich Pöschl, Paulo Artaxo, and Christopher Pöhlker
Atmos. Chem. Phys., 22, 3469–3492, https://doi.org/10.5194/acp-22-3469-2022, https://doi.org/10.5194/acp-22-3469-2022, 2022
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In Central Amazonia, new particle formation in the planetary boundary layer is rare. Instead, there is the appearance of sub-50 nm aerosols with diameters larger than about 20 nm that eventually grow to cloud condensation nuclei size range. Here, 254 growth events were characterized which have higher predominance in the wet season. About 70 % of them showed direct relation to convective downdrafts, while 30 % occurred partly under clear-sky conditions, evidencing still unknown particle sources.
Meinrat O. Andreae, Tracey W. Andreae, Florian Ditas, and Christopher Pöhlker
Atmos. Chem. Phys., 22, 2487–2505, https://doi.org/10.5194/acp-22-2487-2022, https://doi.org/10.5194/acp-22-2487-2022, 2022
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Atmospheric aerosol particles are key players in the Earth’s climate system, but there is still considerable uncertainty about where and how these particles are initially formed. We present the first study of new particle formation (NPF) at a pristine site in a subboreal forest region of North America. Our data suggest that, in this environment, there is frequent NPF from biogenic organic precursor compounds, which was likely the predominant source of particles in the preindustrial environment.
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.
Luiz A. T. Machado, Marco A. Franco, Leslie A. Kremper, Florian Ditas, Meinrat O. Andreae, Paulo Artaxo, Micael A. Cecchini, Bruna A. Holanda, Mira L. Pöhlker, Ivan Saraiva, Stefan Wolff, Ulrich Pöschl, and Christopher Pöhlker
Atmos. Chem. Phys., 21, 18065–18086, https://doi.org/10.5194/acp-21-18065-2021, https://doi.org/10.5194/acp-21-18065-2021, 2021
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Several studies evaluate aerosol–cloud interactions, but only a few attempted to describe how clouds modify aerosol properties. This study evaluates the effect of weather events on the particle size distribution at the ATTO, combining remote sensing and in situ data. Ultrafine, Aitken and accumulation particles modes have different behaviors for the diurnal cycle and for rainfall events. This study opens up new scientific questions that need to be pursued in detail in new field campaigns.
Ramon Campos Braga, Barbara Ervens, Daniel Rosenfeld, Meinrat O. Andreae, Jan-David Förster, Daniel Fütterer, Lianet Hernández Pardo, Bruna A. Holanda, Tina Jurkat-Witschas, Ovid O. Krüger, Oliver Lauer, Luiz A. T. Machado, Christopher Pöhlker, Daniel Sauer, Christiane Voigt, Adrian Walser, Manfred Wendisch, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 21, 17513–17528, https://doi.org/10.5194/acp-21-17513-2021, https://doi.org/10.5194/acp-21-17513-2021, 2021
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Interactions of aerosol particles with clouds represent a large uncertainty in estimates of climate change. Properties of aerosol particles control their ability to act as cloud condensation nuclei. Using aerosol measurements in the Amazon, we performed model studies to compare predicted and measured cloud droplet number concentrations at cloud bases. Our results confirm previous estimates of particle hygroscopicity in this region.
Rachel E. Hawker, Annette K. Miltenberger, Jill S. Johnson, Jonathan M. Wilkinson, Adrian A. Hill, Ben J. Shipway, Paul R. Field, Benjamin J. Murray, and Ken S. Carslaw
Atmos. Chem. Phys., 21, 17315–17343, https://doi.org/10.5194/acp-21-17315-2021, https://doi.org/10.5194/acp-21-17315-2021, 2021
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We find that ice-nucleating particles (INPs), aerosols that can initiate the freezing of cloud droplets, cause substantial changes to the properties of radiatively important convectively generated anvil cirrus. The number concentration of INPs had a large effect on ice crystal number concentration while the INP temperature dependence controlled ice crystal size and cloud fraction. The results indicate information on INP number and source is necessary for the representation of cloud glaciation.
Igor B. Konovalov, Nikolai A. Golovushkin, Matthias Beekmann, Mikhail V. Panchenko, and Meinrat O. Andreae
Atmos. Meas. Tech., 14, 6647–6673, https://doi.org/10.5194/amt-14-6647-2021, https://doi.org/10.5194/amt-14-6647-2021, 2021
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The absorption of solar light by organic matter, known as brown carbon (BrC), contributes significantly to the radiative budget of the Earth’s atmosphere, but its representation in atmospheric models is uncertain. This paper advances a methodology to constrain model parameters characterizing BrC absorption of atmospheric aerosol originating from biomass burning with the available remote ground-based observations of atmospheric aerosol.
Heather Guy, Ian M. Brooks, Ken S. Carslaw, Benjamin J. Murray, Von P. Walden, Matthew D. Shupe, Claire Pettersen, David D. Turner, Christopher J. Cox, William D. Neff, Ralf Bennartz, and Ryan R. Neely III
Atmos. Chem. Phys., 21, 15351–15374, https://doi.org/10.5194/acp-21-15351-2021, https://doi.org/10.5194/acp-21-15351-2021, 2021
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We present the first full year of surface aerosol number concentration measurements from the central Greenland Ice Sheet. Aerosol concentrations here have a distinct seasonal cycle from those at lower-altitude Arctic sites, which is driven by large-scale atmospheric circulation. Our results can be used to help understand the role aerosols might play in Greenland surface melt through the modification of cloud properties. This is crucial in a rapidly changing region where observations are sparse.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Ramon Campos Braga, Daniel Rosenfeld, Ovid O. Krüger, Barbara Ervens, Bruna A. Holanda, Manfred Wendisch, Trismono Krisna, Ulrich Pöschl, Meinrat O. Andreae, Christiane Voigt, and Mira L. Pöhlker
Atmos. Chem. Phys., 21, 14079–14088, https://doi.org/10.5194/acp-21-14079-2021, https://doi.org/10.5194/acp-21-14079-2021, 2021
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Quantifying the precipitation within clouds is crucial for our understanding of the Earth's hydrological cycle. Using in situ measurements of cloud and rain properties over the Amazon Basin and Atlantic Ocean, we show here a linear relationship between the effective radius (re) and precipitation water content near the tops of convective clouds for different pollution states and temperature levels. Our results emphasize the role of re to determine both initiation and amount of precipitation.
Jessica L. McCarty, Juha Aalto, Ville-Veikko Paunu, Steve R. Arnold, Sabine Eckhardt, Zbigniew Klimont, Justin J. Fain, Nikolaos Evangeliou, Ari Venäläinen, Nadezhda M. Tchebakova, Elena I. Parfenova, Kaarle Kupiainen, Amber J. Soja, Lin Huang, and Simon Wilson
Biogeosciences, 18, 5053–5083, https://doi.org/10.5194/bg-18-5053-2021, https://doi.org/10.5194/bg-18-5053-2021, 2021
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Fires, including extreme fire seasons, and fire emissions are more common in the Arctic. A review and synthesis of current scientific literature find climate change and human activity in the north are fuelling an emerging Arctic fire regime, causing more black carbon and methane emissions within the Arctic. Uncertainties persist in characterizing future fire landscapes, and thus emissions, as well as policy-relevant challenges in understanding, monitoring, and managing Arctic fire regimes.
Maria Prass, Meinrat O. Andreae, Alessandro C. de Araùjo, Paulo Artaxo, Florian Ditas, Wolfgang Elbert, Jan-David Förster, Marco Aurélio Franco, Isabella Hrabe de Angelis, Jürgen Kesselmeier, Thomas Klimach, Leslie Ann Kremper, Eckhard Thines, David Walter, Jens Weber, Bettina Weber, Bernhard M. Fuchs, Ulrich Pöschl, and Christopher Pöhlker
Biogeosciences, 18, 4873–4887, https://doi.org/10.5194/bg-18-4873-2021, https://doi.org/10.5194/bg-18-4873-2021, 2021
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Bioaerosols in the atmosphere over the Amazon rain forest were analyzed by molecular biological staining and microscopy. Eukaryotic, bacterial, and archaeal aerosols were quantified in time series and altitude profiles which exhibited clear differences in number concentrations and vertical distributions. Our results provide insights into the sources and dispersion of different Amazonian bioaerosol types as a basis for a better understanding of biosphere–atmosphere interactions.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Ramiro Checa-Garcia, Yves Balkanski, Samuel Albani, Tommi Bergman, Ken Carslaw, Anne Cozic, Chris Dearden, Beatrice Marticorena, Martine Michou, Twan van Noije, Pierre Nabat, Fiona M. O'Connor, Dirk Olivié, Joseph M. Prospero, Philippe Le Sager, Michael Schulz, and Catherine Scott
Atmos. Chem. Phys., 21, 10295–10335, https://doi.org/10.5194/acp-21-10295-2021, https://doi.org/10.5194/acp-21-10295-2021, 2021
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Thousands of tons of dust are emitted into the atmosphere every year, producing important impacts on the Earth system. However, current global climate models are not yet able to reproduce dust emissions, transport and depositions with the desirable accuracy. Our study analyses five different Earth system models to report aspects to be improved to reproduce better available observations, increase the consistency between models and therefore decrease the current uncertainties.
Na Zhao, Xinyi Dong, Kan Huang, Joshua S. Fu, Marianne Tronstad Lund, Kengo Sudo, Daven Henze, Tom Kucsera, Yun Fat Lam, Mian Chin, and Simone Tilmes
Atmos. Chem. Phys., 21, 8637–8654, https://doi.org/10.5194/acp-21-8637-2021, https://doi.org/10.5194/acp-21-8637-2021, 2021
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Black carbon acts as a strong climate forcer, especially in vulnerable pristine regions such as the Arctic. This work utilizes ensemble modeling results from the task force Hemispheric Transport of Air Pollution Phase 2 to investigate the responses of Arctic black carbon and surface temperature to various source emission reductions. East Asia contributed the most to Arctic black carbon. The response of Arctic temperature to black carbon was substantially more sensitive than the global average.
Yaman Liu, Xinyi Dong, Minghuai Wang, Louisa K. Emmons, Yawen Liu, Yuan Liang, Xiao Li, and Manish Shrivastava
Atmos. Chem. Phys., 21, 8003–8021, https://doi.org/10.5194/acp-21-8003-2021, https://doi.org/10.5194/acp-21-8003-2021, 2021
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Secondary organic aerosol (SOA) is considered one of the most important uncertainties in climate modeling. We evaluate SOA performance in the Community Earth System Model version 2.1 (CESM2.1) configured with the Community Atmosphere Model version 6 with chemistry (CAM6-Chem) through a long-term simulation (1988–2019) with observations in the United States, which indicates monoterpene-formed SOA contributes most to the overestimation of SOA at the surface and underestimation in the upper air.
Xinyi Dong, Man Yue, Yujun Jiang, Xiao-Ming Hu, Qianli Ma, Jingjiao Pu, and Guangqiang Zhou
Atmos. Chem. Phys., 21, 7217–7233, https://doi.org/10.5194/acp-21-7217-2021, https://doi.org/10.5194/acp-21-7217-2021, 2021
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The dynamics of CO2 has received considerable attention in the literature, yet uncertainties remain. We applied an online coupled weather-biosphere model to simulate biosphere processes and meteorology simultaneously to characterize CO2 dynamics in China. Anthropogenic emission was more influential in upper air, and the biosphere flux played a more important role in surface CO2, suggesting a significant influence of the boundary layer thermal structure on the accumulation and depletion of CO2.
Robbie Ramsay, Chiara F. Di Marco, Mathew R. Heal, Matthias Sörgel, Paulo Artaxo, Meinrat O. Andreae, and Eiko Nemitz
Biogeosciences, 18, 2809–2825, https://doi.org/10.5194/bg-18-2809-2021, https://doi.org/10.5194/bg-18-2809-2021, 2021
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The exchange of the gas ammonia between the atmosphere and the surface is an important biogeochemical process, but little is known of this exchange for certain ecosystems, such as the Amazon rainforest. This study took measurements of ammonia exchange over an Amazon rainforest site and subsequently modelled the observed deposition and emission patterns. We observed emissions of ammonia from the rainforest, which can be simulated accurately by using a canopy resistance modelling approach.
Joanna E. Dyson, Graham A. Boustead, Lauren T. Fleming, Mark Blitz, Daniel Stone, Stephen R. Arnold, Lisa K. Whalley, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 5755–5775, https://doi.org/10.5194/acp-21-5755-2021, https://doi.org/10.5194/acp-21-5755-2021, 2021
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The hydroxyl radical (OH) dominates the removal of atmospheric pollutants, with nitrous acid (HONO) recognised as a major OH source. For remote regions HONO production through the action of sunlight on aerosol surfaces can provide a source of nitrogen oxides. In this study, HONO production rates at illuminated aerosol surfaces are measured under atmospheric conditions, a model consistent with the data is developed and aerosol production of HONO in the atmosphere is shown to be significant.
Rachel E. Hawker, Annette K. Miltenberger, Jonathan M. Wilkinson, Adrian A. Hill, Ben J. Shipway, Zhiqiang Cui, Richard J. Cotton, Ken S. Carslaw, Paul R. Field, and Benjamin J. Murray
Atmos. Chem. Phys., 21, 5439–5461, https://doi.org/10.5194/acp-21-5439-2021, https://doi.org/10.5194/acp-21-5439-2021, 2021
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The impact of aerosols on clouds is a large source of uncertainty for future climate projections. Our results show that the radiative properties of a complex convective cloud field in the Saharan outflow region are sensitive to the temperature dependence of ice-nucleating particle concentrations. This means that differences in the aerosol source or composition, for the same aerosol size distribution, can cause differences in the outgoing radiation from regions dominated by tropical convection.
Ananth Ranjithkumar, Hamish Gordon, Christina Williamson, Andrew Rollins, Kirsty Pringle, Agnieszka Kupc, Nathan Luke Abraham, Charles Brock, and Ken Carslaw
Atmos. Chem. Phys., 21, 4979–5014, https://doi.org/10.5194/acp-21-4979-2021, https://doi.org/10.5194/acp-21-4979-2021, 2021
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The effect aerosols have on climate can be better understood by studying their vertical and spatial distribution throughout the atmosphere. We use observation data from the ATom campaign and evaluate the vertical profile of aerosol number concentration, sulfur dioxide and condensation sink using the UKESM (UK Earth System Model). We identify uncertainties in key atmospheric processes that help improve their theoretical representation in global climate models.
Thomas Thorp, Stephen R. Arnold, Richard J. Pope, Dominick V. Spracklen, Luke Conibear, Christoph Knote, Mikhail Arshinov, Boris Belan, Eija Asmi, Tuomas Laurila, Andrei I. Skorokhod, Tuomo Nieminen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 4677–4697, https://doi.org/10.5194/acp-21-4677-2021, https://doi.org/10.5194/acp-21-4677-2021, 2021
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We compare modelled near-surface pollutants with surface and satellite observations to better understand the controls on the regional concentrations of pollution in western Siberia for late spring and summer in 2011. We find two commonly used emission inventories underestimate human emissions when compared to observations. Transport emissions are the main source of pollutants within the region during this period, whilst fire emissions peak during June and are only significant south of 60° N.
Melinda K. Schueneman, Benjamin A. Nault, Pedro Campuzano-Jost, Duseong S. Jo, Douglas A. Day, Jason C. Schroder, Brett B. Palm, Alma Hodzic, Jack E. Dibb, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 2237–2260, https://doi.org/10.5194/amt-14-2237-2021, https://doi.org/10.5194/amt-14-2237-2021, 2021
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This work focuses on two important properties of the aerosol, acidity, and sulfate composition, which is important for our understanding of aerosol health and environmental impacts. We explore different methods to understand the composition of the aerosol with measurements from a specific instrument and apply those methods to a large dataset. These measurements are confounded by other factors, making it challenging to predict aerosol sulfate composition; pH estimations, however, show promise.
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.
Kamalika Sengupta, Kirsty Pringle, Jill S. Johnson, Carly Reddington, Jo Browse, Catherine E. Scott, and Ken Carslaw
Atmos. Chem. Phys., 21, 2693–2723, https://doi.org/10.5194/acp-21-2693-2021, https://doi.org/10.5194/acp-21-2693-2021, 2021
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Global models consistently underestimate atmospheric secondary organic aerosol (SOA), which has significant climatic implications. We use a perturbed parameter model ensemble and ground-based observations to reduce the uncertainty in modelling SOA formation from oxidation of volatile organic compounds. We identify plausible parameter spaces for the yields of extremely low-volatility, low-volatility, and semi-volatile organic compounds based on model–observation match for three key model outputs.
Jim M. Haywood, Steven J. Abel, Paul A. Barrett, Nicolas Bellouin, Alan Blyth, Keith N. Bower, Melissa Brooks, Ken Carslaw, Haochi Che, Hugh Coe, Michael I. Cotterell, Ian Crawford, Zhiqiang Cui, Nicholas Davies, Beth Dingley, Paul Field, Paola Formenti, Hamish Gordon, Martin de Graaf, Ross Herbert, Ben Johnson, Anthony C. Jones, Justin M. Langridge, Florent Malavelle, Daniel G. Partridge, Fanny Peers, Jens Redemann, Philip Stier, Kate Szpek, Jonathan W. Taylor, Duncan Watson-Parris, Robert Wood, Huihui Wu, and Paquita Zuidema
Atmos. Chem. Phys., 21, 1049–1084, https://doi.org/10.5194/acp-21-1049-2021, https://doi.org/10.5194/acp-21-1049-2021, 2021
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Every year, the seasonal cycle of biomass burning from agricultural practices in Africa creates a huge plume of smoke that travels many thousands of kilometres over the Atlantic Ocean. This study provides an overview of a measurement campaign called the cloud–aerosol–radiation interaction and forcing for year 2017 (CLARIFY-2017) and documents the rationale, deployment strategy, observations, and key results from the campaign which utilized the heavily equipped FAAM atmospheric research aircraft.
Benjamin J. Murray, Kenneth S. Carslaw, and Paul R. Field
Atmos. Chem. Phys., 21, 665–679, https://doi.org/10.5194/acp-21-665-2021, https://doi.org/10.5194/acp-21-665-2021, 2021
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The balance between the amounts of ice and supercooled water in clouds over the world's oceans strongly influences how much these clouds can dampen or amplify global warming. Aerosol particles which catalyse ice formation can dramatically reduce the amount of supercooled water in clouds; hence we argue that we need a concerted effort to improve our understanding of these ice-nucleating particles if we are to improve our predictions of climate change.
Igor B. Konovalov, Nikolai A. Golovushkin, Matthias Beekmann, and Meinrat O. Andreae
Atmos. Chem. Phys., 21, 357–392, https://doi.org/10.5194/acp-21-357-2021, https://doi.org/10.5194/acp-21-357-2021, 2021
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A lack of consistent observational constraints on the atmospheric evolution of the optical properties of biomass burning (BB) aerosol limits the accuracy of assessments of the aerosol radiative and climate effects. We show that useful insights into the evolution of the BB aerosol optical properties can be inferred from a combination of satellite observations and 3D modeling. We report major changes that occurred in the optical properties of Siberian BB aerosol during its long-range transport.
Robert B. Chatfield, Meinrat O. Andreae, ARCTAS Science Team, and SEAC4RS Science Team
Atmos. Meas. Tech., 13, 7069–7096, https://doi.org/10.5194/amt-13-7069-2020, https://doi.org/10.5194/amt-13-7069-2020, 2020
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Forest burning affects air pollution and global climate. A NASA aircraft studied fire emissions including the Rim Fire near Yosemite. We found frequent confusions between the actual fire emission factors and other effects on the air samples. Effects on CO2 and CO can originate far upwind; the gases can mix variably into a smoke plume. We devised a theory of constant features in plumes. A statistical mixed-effects analysis of a co-emitted tracers model disentangles such mixing from fire effects.
Jane P. Mulcahy, Colin Johnson, Colin G. Jones, Adam C. Povey, Catherine E. Scott, Alistair Sellar, Steven T. Turnock, Matthew T. Woodhouse, Nathan Luke Abraham, Martin B. Andrews, Nicolas Bellouin, Jo Browse, Ken S. Carslaw, Mohit Dalvi, Gerd A. Folberth, Matthew Glover, Daniel P. Grosvenor, Catherine Hardacre, Richard Hill, Ben Johnson, Andy Jones, Zak Kipling, Graham Mann, James Mollard, Fiona M. O'Connor, Julien Palmiéri, Carly Reddington, Steven T. Rumbold, Mark Richardson, Nick A. J. Schutgens, Philip Stier, Marc Stringer, Yongming Tang, Jeremy Walton, Stephanie Woodward, and Andrew Yool
Geosci. Model Dev., 13, 6383–6423, https://doi.org/10.5194/gmd-13-6383-2020, https://doi.org/10.5194/gmd-13-6383-2020, 2020
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Aerosols are an important component of the Earth system. Here, we comprehensively document and evaluate the aerosol schemes as implemented in the physical and Earth system models, HadGEM3-GC3.1 and UKESM1. This study provides a useful characterisation of the aerosol climatology in both models, facilitating the understanding of the numerous aerosol–climate interaction studies that will be conducted for CMIP6 and beyond.
Daniel P. Grosvenor and Kenneth S. Carslaw
Atmos. Chem. Phys., 20, 15681–15724, https://doi.org/10.5194/acp-20-15681-2020, https://doi.org/10.5194/acp-20-15681-2020, 2020
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Particles arising from human activity interact with clouds and affect how much of the Sun's energy is reflected away. Lack of understanding about how to represent this in models leads to large uncertainties in climate predictions. We quantify cloud responses to particles in the latest UK Met Office climate model over the North Atlantic Ocean, showing that, in contrast to suggestions elsewhere, increases in cloud coverage and thickness are important over large areas.
Robbie Ramsay, Chiara F. Di Marco, Matthias Sörgel, Mathew R. Heal, Samara Carbone, Paulo Artaxo, Alessandro C. de Araùjo, Marta Sá, Christopher Pöhlker, Jost Lavric, Meinrat O. Andreae, and Eiko Nemitz
Atmos. Chem. Phys., 20, 15551–15584, https://doi.org/10.5194/acp-20-15551-2020, https://doi.org/10.5194/acp-20-15551-2020, 2020
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The Amazon rainforest is a unique
laboratoryto study the processes which govern the exchange of gases and aerosols to and from the atmosphere. This study investigated these processes by measuring the atmospheric concentrations of trace gases and particles at the Amazon Tall Tower Observatory. We found that the long-range transport of pollutants can affect the atmospheric composition above the Amazon rainforest and that the gases ammonia and nitrous acid can be emitted from the rainforest.
Zhuang Wang, Cheng Liu, Zhouqing Xie, Qihou Hu, Meinrat O. Andreae, Yunsheng Dong, Chun Zhao, Ting Liu, Yizhi Zhu, Haoran Liu, Chengzhi Xing, Wei Tan, Xiangguang Ji, Jinan Lin, and Jianguo Liu
Atmos. Chem. Phys., 20, 14917–14932, https://doi.org/10.5194/acp-20-14917-2020, https://doi.org/10.5194/acp-20-14917-2020, 2020
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Significant stratification of aerosols was observed in North China. Polluted dust dominated above the PBL, and anthropogenic aerosols prevailed within the PBL, which is mainly driven by meteorological conditions. The key role of the elevated dust is to alter atmospheric thermodynamics and stability, causing the suppression of turbulence exchange and a decrease in PBL height, especially during the dissipation stage, thereby inhibiting dissipation of persistent heavy surface haze pollution.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Hongyu Guo, Duseong S. Jo, Anne V. Handschy, Demetrios Pagonis, Jason C. Schroder, Melinda K. Schueneman, Michael J. Cubison, Jack E. Dibb, Alma Hodzic, Weiwei Hu, Brett B. Palm, and Jose L. Jimenez
Atmos. Meas. Tech., 13, 6193–6213, https://doi.org/10.5194/amt-13-6193-2020, https://doi.org/10.5194/amt-13-6193-2020, 2020
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Collecting particulate matter, or aerosols, onto filters to be analyzed offline is a widely used method to investigate the mass concentration and chemical composition of the aerosol, especially the inorganic portion. Here, we show that acidic aerosol (sulfuric acid) collected onto filters and then exposed to high ammonia mixing ratios (from human emissions) will lead to biases in the ammonium collected onto filters, and the uptake of ammonia is rapid (< 10 s), which impacts the filter data.
Sandip S. Dhomse, Graham W. Mann, Juan Carlos Antuña Marrero, Sarah E. Shallcross, Martyn P. Chipperfield, Kenneth S. Carslaw, Lauren Marshall, N. Luke Abraham, and Colin E. Johnson
Atmos. Chem. Phys., 20, 13627–13654, https://doi.org/10.5194/acp-20-13627-2020, https://doi.org/10.5194/acp-20-13627-2020, 2020
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We confirm downward adjustment of SO2 emission to simulate the Pinatubo aerosol cloud with aerosol microphysics models. Similar adjustment is also needed to simulate the El Chichón and Agung volcanic cloud, indicating potential missing removal or vertical redistribution process in models. Important inhomogeneities in the CMIP6 forcing datasets after Agung and El Chichón eruptions are difficult to reconcile. Quasi-biennial oscillation plays an important role in modifying stratospheric warming.
Nina Löbs, David Walter, Cybelli G. G. Barbosa, Sebastian Brill, Rodrigo P. Alves, Gabriela R. Cerqueira, Marta de Oliveira Sá, Alessandro C. de Araújo, Leonardo R. de Oliveira, Florian Ditas, Daniel Moran-Zuloaga, Ana Paula Pires Florentino, Stefan Wolff, Ricardo H. M. Godoi, Jürgen Kesselmeier, Sylvia Mota de Oliveira, Meinrat O. Andreae, Christopher Pöhlker, and Bettina Weber
Biogeosciences, 17, 5399–5416, https://doi.org/10.5194/bg-17-5399-2020, https://doi.org/10.5194/bg-17-5399-2020, 2020
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Cryptogamic organisms, such as bryophytes, lichens, and algae, cover major parts of vegetation in the Amazonian rain forest, but their relevance in biosphere–atmosphere exchange, climate processes, and nutrient cycling is largely unknown.
Over the duration of 2 years we measured their water content, temperature, and light conditions to get better insights into their physiological activity patterns and thus their potential impact on local, regional, and even global biogeochemical processes.
Lixia Liu, Yafang Cheng, Siwen Wang, Chao Wei, Mira L. Pöhlker, Christopher Pöhlker, Paulo Artaxo, Manish Shrivastava, Meinrat O. Andreae, Ulrich Pöschl, and Hang Su
Atmos. Chem. Phys., 20, 13283–13301, https://doi.org/10.5194/acp-20-13283-2020, https://doi.org/10.5194/acp-20-13283-2020, 2020
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This modeling paper reveals how aerosol–cloud interactions (ACIs) and aerosol–radiation interactions (ARIs) induced by biomass burning (BB) aerosols act oppositely on radiation, cloud, and precipitation in the Amazon during the dry season. The varying relative significance of ACIs and ARIs with BB aerosol concentration leads to a nonlinear dependence of the total climate response on BB aerosol loading and features the growing importance of ARIs at high aerosol loading.
Ben Silver, Luke Conibear, Carly L. Reddington, Christoph Knote, Steve R. Arnold, and Dominick V. Spracklen
Atmos. Chem. Phys., 20, 11683–11695, https://doi.org/10.5194/acp-20-11683-2020, https://doi.org/10.5194/acp-20-11683-2020, 2020
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China suffers from serious air pollution, which is thought to cause millions of early deaths each year. Measurements on the ground show that overall air quality is improving. Air quality is also affected by weather conditions, which can vary from year to year. We conduct computer simulations to show it is the reduction of the amount of pollution emitted, rather than weather conditions, which caused air quality to improve during 2015–2017. We then estimate that 150 000 fewer people die early.
Hamish Gordon, Paul R. Field, Steven J. Abel, Paul Barrett, Keith Bower, Ian Crawford, Zhiqiang Cui, Daniel P. Grosvenor, Adrian A. Hill, Jonathan Taylor, Jonathan Wilkinson, Huihui Wu, and Ken S. Carslaw
Atmos. Chem. Phys., 20, 10997–11024, https://doi.org/10.5194/acp-20-10997-2020, https://doi.org/10.5194/acp-20-10997-2020, 2020
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The Met Office's Unified Model is widely used both for weather forecasting and climate prediction. We present the first version of the model in which both aerosol and cloud particle mass and number concentrations are allowed to evolve separately and independently, which is important for studying how aerosols affect weather and climate. We test the model against aircraft observations near Ascension Island in the Atlantic, focusing on how aerosols can "activate" to become cloud droplets.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys., 20, 10937–10951, https://doi.org/10.5194/acp-20-10937-2020, https://doi.org/10.5194/acp-20-10937-2020, 2020
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Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
Cited articles
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Bianchi, F., Kurten, T., Riva, M., Mohr, C., Rissanen, M. P., Roldin, P., Berndt, T., Crounse, J. D., Wennberg, P. O., Mentel, T. F., Wildt, J., Junninen, H., Jokinen, T., Kulmala, M., Worsnop, D. R., Thornton, J. A., Donahue, N., Kjaergaard, H. G., and Ehn, M.: Highly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol, Chem. Rev., 119, 3472–3509, https://doi.org/10.1021/acs.chemrev.8b00395, 2019.
Boy, M., Karl, T., Turnipseed, A., Mauldin, R. L., Kosciuch, E., Greenberg, J., Rathbone, J., Smith, J., Held, A., Barsanti, K., Wehner, B., Bauer, S., Wiedensohler, A., Bonn, B., Kulmala, M., and Guenther, A.: New particle formation in the Front Range of the Colorado Rocky Mountains, Atmos. Chem. Phys., 8, 1577–1590, https://doi.org/10.5194/acp-8-1577-2008, 2008.
Carslaw, K. S.: Chapter 2 – Aerosol in the climate system, in: Aerosols and Climate, edited by: Carslaw, K. S., Elsevier, https://doi.org/10.1016/B978-0-12-819766-0.00008-0, 9–52, 2022.
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Deng, C. J., Fu, Y. Y., Dada, L., Yan, C., Cai, R. L., Yang, D. S., Zhou, Y., Yin, R. J., Lu, Y. Q., Li, X. X., Qiao, X. H., Fan, X. L., Nie, W., Kontkanen, J., Kangasluoma, J., Chu, B. W., Ding, A. J., Kerminen, V. M., Paasonen, P., Worsnop, D. R., Bianchi, F., Liu, Y. C., Zheng, J., Wang, L., Kulmala, M., and Jiang, J. K.: Seasonal Characteristics of New Particle Formation and Growth in Urban Beijing, Environ. Sci. Technol., 54, 8547–8557, https://doi.org/10.1021/acs.est.0c00808, 2020.
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Dunne, E. M., Gordon, H., Kurten, A., Almeida, J., Duplissy, J., Williamson, C., Ortega, I. K., Pringle, K. J., Adamov, A., Baltensperger, U., Barmet, P., Benduhn, F., Bianchi, F., Breitenlechner, M., Clarke, A., Curtius, J., Dommen, J., Donahue, N. M., Ehrhart, S., Flagan, R. C., Franchin, A., Guida, R., Hakala, J., Hansel, A., Heinritzi, M., Jokinen, T., Kangasluoma, J., Kirkby, J., Kulmala, M., Kupc, A., Lawler, M. J., Lehtipalo, K., Makhmutov, V., Mann, G., Mathot, S., Merikanto, J., Miettinen, P., Nenes, A., Onnela, A., Rap, A., Reddington, C. L. S., Riccobono, F., Richards, N. A. D., Rissanen, M. P., Rondo, L., Sarnela, N., Schobesberger, S., Sengupta, K., Simon, M., Sipilaa, M., Smith, J. N., Stozkhov, Y., Tome, A., Trostl, J., Wagner, P. E., Wimmer, D., Winkler, P. M., Worsnop, D. R., and Carslaw, K. S.: Global atmospheric particle formation from CERN CLOUD measurements, Science, 354, 1119–1124, https://doi.org/10.1126/science.aaf2649, 2016.
Ehn, M., Thornton, J. A., Kleist, E., Sipila, M., Junninen, H., Pullinen, I., Springer, M., Rubach, F., Tillmann, R., Lee, B., Lopez-Hilfiker, F., Andres, S., Acir, I. H., Rissanen, M., Jokinen, T., Schobesberger, S., Kangasluoma, J., Kontkanen, J., Nieminen, T., Kurten, T., Nielsen, L. B., Jorgensen, S., Kjaergaard, H. G., Canagaratna, M., Dal Maso, M., Berndt, T., Petaja, T., Wahner, A., Kerminen, V. M., Kulmala, M., Worsnop, D. R., Wildt, J., and Mentel, T. F.: A large source of low-volatility secondary organic aerosol, Nature, 506, 476–479, https://doi.org/10.1038/nature13032, 2014.
Emmons, L. K., Schwantes, R. H., Orlando, J. J., Tyndall, G., Kinnison, D., Lamarque, J. F., Marsh, D., Mills, M. J., Tilmes, S., Bardeen, C., Buchholz, R. R., Conley, A., Gettelman, A., Garcia, R., Simpson, I., Blake, D. R., Meinardi, S., and Pétron, G.: The Chemistry Mechanism in the Community Earth System Model Version 2 (CESM2), J. Adv. Model. Earth Sy., 12, e2019MS001882, https://doi.org/10.1029/2019ms001882, 2020.
Frege, C., Ortega, I. K., Rissanen, M. P., Praplan, A. P., Steiner, G., Heinritzi, M., Ahonen, L., Amorim, A., Bernhammer, A.-K., Bianchi, F., Brilke, S., Breitenlechner, M., Dada, L., Dias, A., Duplissy, J., Ehrhart, S., El-Haddad, I., Fischer, L., Fuchs, C., Garmash, O., Gonin, M., Hansel, A., Hoyle, C. R., Jokinen, T., Junninen, H., Kirkby, J., Kürten, A., Lehtipalo, K., Leiminger, M., Mauldin, R. L., Molteni, U., Nichman, L., Petäjä, T., Sarnela, N., Schobesberger, S., Simon, M., Sipilä, M., Stolzenburg, D., Tomé, A., Vogel, A. L., Wagner, A. C., Wagner, R., Xiao, M., Yan, C., Ye, P., Curtius, J., Donahue, N. M., Flagan, R. C., Kulmala, M., Worsnop, D. R., Winkler, P. M., Dommen, J., and Baltensperger, U.: Influence of temperature on the molecular composition of ions and charged clusters during pure biogenic nucleation, Atmos. Chem. Phys., 18, 65–79, https://doi.org/10.5194/acp-18-65-2018, 2018.
Garmash, O., Rissanen, M. P., Pullinen, I., Schmitt, S., Kausiala, O., Tillmann, R., Zhao, D., Percival, C., Bannan, T. J., Priestley, M., Hallquist, Å. M., Kleist, E., Kiendler-Scharr, A., Hallquist, M., Berndt, T., McFiggans, G., Wildt, J., Mentel, T. F., and Ehn, M.: Multi-generation OH oxidation as a source for highly oxygenated organic molecules from aromatics, Atmos. Chem. Phys., 20, 515–537, https://doi.org/10.5194/acp-20-515-2020, 2020.
Gordon, H., Sengupta, K., Rap, A., Duplissy, J., Frege, C., Williamson, C., Heinritzi, M., Simon, M., Yan, C., Almeida, J., Trostl, J., Nieminen, T., Ortega, I. K., Wagner, R., Dunne, E. M., Adamov, A., Amorim, A., Bernhammer, A. K., Bianchi, F., Breitenlechner, M., Brilke, S., Chen, X. M., Craven, J. S., Dias, A., Ehrhart, S., Fischer, L., Flagan, R. C., Franchin, A., Fuchs, C., Guida, R., Hakala, J., Hoyle, C. R., Jokinen, T., Junninen, H., Kangasluoma, J., Kim, J., Kirkby, J., Krapf, M., Kurten, A., Laaksonen, A., Lehtipalo, K., Makhmutov, V., Mathot, S., Molteni, U., Monks, S. A., Onnela, A., Perakyla, O., Piel, F., Petaja, T., Praplanh, A. P., Pringle, K. J., Richards, N. A. D., Rissanen, M. P., Rondo, L., Sarnela, N., Schobesberger, S., Scott, C. E., Seinfeldo, J. H., Sharma, S., Sipila, M., Steiner, G., Stozhkov, Y., Stratmann, F., Tome, A., Virtanen, A., Vogel, A. L., Wagner, A. C., Wagner, P. E., Weingartner, E., Wimmer, D., Winkler, P. M., Ye, P. L., Zhang, X., Hansel, A., Dommen, J., Donahue, N. M., Worsnop, D. R., Baltensperger, U., Kulmala, M., Curtius, J., and Carslaw, K. S.: Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation, P. Natl. Acad. Sci. USA, 113, 12053–12058, https://doi.org/10.1073/pnas.1602360113, 2016.
Gordon, H., Kirkby, J., Baltensperger, U., Bianchi, F., Breitenlechner, M., Curtius, J., Dias, A., Dommen, J., Donahue, N. M., Dunne, E. M., Duplissy, J., Ehrhart, S., Flagan, R. C., Frege, C., Fuchs, C., Hansel, A., Hoyle, C. R., Kulmala, M., Kurten, A., Lehtipalo, K., Makhmutov, V., Molteni, U., Rissanen, M. P., Stozkhov, Y., Trostl, J., Tsagkogeorgas, G., Wagner, R., Williamson, C., Wimmer, D., Winkler, P. M., Yan, C., and Carslaw, K. S.: Causes and importance of new particle formation in the present-day and preindustrial atmospheres, J. Geophys. Res.-Atmos., 122, 8739–8760, https://doi.org/10.1002/2017jd026844, 2017.
Guenther, A. B., Jiang, X., Heald, C. L., Sakulyanontvittaya, T., Duhl, T., Emmons, L. K., and Wang, X.: The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions, Geosci. Model Dev., 5, 1471–1492, https://doi.org/10.5194/gmd-5-1471-2012, 2012.
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Short summary
Highly oxygenated organic molecules (HOMs) play an important role in atmospheric new particle formation (NPF). By semi-explicitly coupling the chemical mechanism of HOMs and a comprehensive nucleation scheme in a global climate model, the updated model shows better agreement with measurements of nucleation rate, growth rate, and NPF event frequency. Our results reveal that HOM-driven NPF leads to a considerable increase in particle and cloud condensation nuclei burden globally.
Highly oxygenated organic molecules (HOMs) play an important role in atmospheric new particle...
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