Articles | Volume 21, issue 6
https://doi.org/10.5194/acp-21-4979-2021
© Author(s) 2021. 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-21-4979-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Constraints on global aerosol number concentration, SO2 and condensation sink in UKESM1 using ATom measurements
Ananth Ranjithkumar
CORRESPONDING AUTHOR
School of Earth and Environment, University of Leeds, LS2 9JT, United
Kingdom
Engineering Research Accelerator and Centre for Atmospheric Particle
Studies, Carnegie Mellon University, Pittsburgh, PA 15213, USA
School of Earth and Environment, University of Leeds, LS2 9JT, United
Kingdom
Christina Williamson
Cooperative Institute for Research in Environmental Sciences,
University of Colorado, Boulder, CO 80309, USA
NOAA Chemical Sciences Laboratory, Boulder, CO 80305, USA
Andrew Rollins
Cooperative Institute for Research in Environmental Sciences,
University of Colorado, Boulder, CO 80309, USA
Kirsty Pringle
School of Earth and Environment, University of Leeds, LS2 9JT, United
Kingdom
Agnieszka Kupc
NOAA Chemical Sciences Laboratory, Boulder, CO 80305, USA
Faculty of Physics, Aerosol Physics and Environmental Physics,
University of Vienna, 1090 Vienna, Austria
Nathan Luke Abraham
NCAS-Climate, University of Cambridge, CB2 1EW, UK
Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
Charles Brock
NOAA Chemical Sciences Laboratory, Boulder, CO 80305, USA
Ken Carslaw
School of Earth and Environment, University of Leeds, LS2 9JT, United
Kingdom
Related authors
No articles found.
Xu-Cheng He, Nathan Luke Abraham, Han Ding, Maria R. Russo, Daniel P. Grosvenor, Yao Ge, Xuemei Wang, Anthony C. Jones, Pedro Campuzano-Jost, Benjamin Nault, Agnieszka Kupc, Donald Blake, Jose L. Jimenez, Christina J. Williamson, Kenneth S. Carslaw, James Weber, Alexander T. Archibald, and Hamish Gordon
EGUsphere, https://doi.org/10.5194/egusphere-2025-3700, https://doi.org/10.5194/egusphere-2025-3700, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Aerosols affect clouds and climate. However, current climate models still struggle to simulate them accurately. We used aircraft data from a global mission to evaluate how well the UK Earth System Model represents aerosols and their precursors. Our results show that the model misses key formation processes in clean ocean regions, suggesting that future improvements should focus on better representing how aerosols form naturally in the atmosphere.
William J. Collins, Fiona M. O'Connor, Rachael E. Byrom, Øivind Hodnebrog, Patrick Jöckel, Mariano Mertens, Gunnar Myhre, Matthias Nützel, Dirk Olivié, Ragnhild Bieltvedt Skeie, Laura Stecher, Larry W. Horowitz, Vaishali Naik, Gregory Faluvegi, Ulas Im, Lee T. Murray, Drew Shindell, Kostas Tsigaridis, Nathan Luke Abraham, and James Keeble
Atmos. Chem. Phys., 25, 9031–9060, https://doi.org/10.5194/acp-25-9031-2025, https://doi.org/10.5194/acp-25-9031-2025, 2025
Short summary
Short summary
We used 7 climate models that include atmospheric chemistry and find that in a scenario with weak controls on air quality, the warming effects (over 2015 to 2050) of decreases in ozone-depleting substances and increases in air quality pollutants are approximately equal and would make ozone the second highest contributor to warming over this period. We find that for stratospheric ozone recovery, the standard measure of climate effects underestimates a more comprehensive measure.
Pratapaditya Ghosh, Katherine J. Evans, Daniel P. Grosvenor, Hyun-Gyu Kang, Salil Mahajan, Min Xu, Wei Zhang, and Hamish Gordon
Geosci. Model Dev., 18, 4899–4913, https://doi.org/10.5194/gmd-18-4899-2025, https://doi.org/10.5194/gmd-18-4899-2025, 2025
Short summary
Short summary
The most popular algorithm for calculating cloud droplet number concentrations in climate models is sensitive to parameters that control simulated aerosol particle number concentrations at different sizes. We recommend small modifications to functions in the algorithm to improve its performance. Implementing the changes in the UK Met Office climate model reduced average bias in simulated global droplet number concentrations, leading to more reflected solar radiation and a net cooling effect.
Loren Temple, Stuart Young, Thomas Bannan, Stephanie Batten, Stéphane Bauguitte, Hugh Coe, Eve Grant, Stuart Lacy, James Lee, Emily Matthews, Dominika Pasternak, Samuel Rogers, Andrew Rollins, Jake Vallow, Mingxi Yang, and Pete Edwards
EGUsphere, https://doi.org/10.5194/egusphere-2025-3678, https://doi.org/10.5194/egusphere-2025-3678, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
Short summary
Short summary
Sulfur dioxide (SO2) is a key precursor to aerosol formation, particularly in remote marine environments, ultimately affecting cloud properties and climate. Accurate quantification of atmospheric SO2 is therefore crucial. This work compares a custom-built laser-based instrument to two commercial SO2 analysers during measurements from a large research aircraft. Our results show that this custom-built system offers greater sensitivity at time resolutions required for aircraft measurements.
Neil M. Donahue, Victoria Hofbauer, Henning Finkenzeller, Dominik Stolzenburg, Paulus S. Bauer, Randall Chiu, Lubna Dada, Jonathan Duplissy, Xu-Cheng He, Martin Heinritzi, Christopher R. Hoyle, Andreas Kürten, Aleksandr Kvashnin, Katrianne Lehtipalo, Naser Mahfouz, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Mario Simon, Andrea C. Wagner, Mingyi Wang, Chao Yan, Penglin Ye, Ilona Riipinen, Hamish Gordon, Joachim Curtius, Armin Hansel, Imad El Haddad, Markku Kulmala, Douglas R. Worsnop, Rainer Volkamer, Paul M. Winkler, Jasper Kirkby, and Richard Flagan
EGUsphere, https://doi.org/10.5194/egusphere-2025-2412, https://doi.org/10.5194/egusphere-2025-2412, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
Short summary
Short summary
We describe accurate measurement of particle formation and growth in the CERN CLOUD chamber, using a suite of gas- and particle-phase instruments. The interconnected measurements establish high accuracy in key particle properties and critically important gas-phase sulfuric acid. This is a template for accurate calibration of similar experiments and thus accurate determination of aerosol nucleation and growth rates, which are an important source of uncertainty in climate science.
Megan A. J. Brown, Nicola J . Warwick, Nathan Luke Abraham, Paul T. Griffiths, Steve T. Rumbold, Gerd A. Folberth, Fiona M. O'Connor, and Alex T. Archibald
EGUsphere, https://doi.org/10.5194/egusphere-2025-2676, https://doi.org/10.5194/egusphere-2025-2676, 2025
This preprint is open for discussion and under review for Geoscientific Model Development (GMD).
Short summary
Short summary
Hydrogen (H2) is an indirect greenhouse gas by increasing methane (CH4) lifetime. Interaction between H2 and CH4 is important for hydrogen’s global warming potential (GWP). Global models do not represent this interaction well; H2 or CH4 are prescribed at the surface. We implement an interactive H2 scheme into a global model coupled with interactive CH4. We simulate scenarios demonstrating its capability, improving model performance and more accurately representing H2-CH4 interaction.
Jasna V. Pittman, Bruce C. Daube, Steven C. Wofsy, Elliot L. Atlas, Maria A. Navarro, Eric J. Hintsa, Fred L. Moore, Geoff S. Dutton, James W. Elkins, Troy D. Thornberry, Andrew W. Rollins, Eric J. Jensen, Thaopaul Bui, Jonathan Dean-Day, and Leonhard Pfister
Atmos. Chem. Phys., 25, 7543–7562, https://doi.org/10.5194/acp-25-7543-2025, https://doi.org/10.5194/acp-25-7543-2025, 2025
Short summary
Short summary
Biomass fires emit aerosols and precursors that can provide a novel environment for initiating stratospheric ozone loss. The Airborne Tropical TRopopause EXperiment campaign sampled the western Pacific, the dominant longitudes for surface air lofted by convection to enter the global stratosphere. Aircraft measurements over multiple flights revealed persistent layers of biomass burning pollutants entering the lower stratosphere and originating from fires as far away as Africa and Indonesia.
Rachel W. N. Sansom, Jill S. Johnson, Leighton A. Regayre, Lindsay A. Lee, and Ken S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2025-3104, https://doi.org/10.5194/egusphere-2025-3104, 2025
Short summary
Short summary
The cloud transition from stratocumulus to cumulus features a distinct decrease in cloud cover. We used a high-resolution model to simulate many instances of the transition with different environmental conditions. In low aerosol conditions, the transition occurred faster due to drizzle depleting the cloud of moisture and aerosol, whereas in high aerosol conditions, other factors were more important. Understanding different regimes is important for accurately simulating clouds in global models.
Xinyue Shao, Yaman Liu, Xinyi Dong, Minghuai Wang, Ruochong Xu, Joel A. Thornton, Duseong S. Jo, Man Yue, Wenxiang Shen, Manish Shrivastava, Stephen R. Arnold, and Ken S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2025-1526, https://doi.org/10.5194/egusphere-2025-1526, 2025
Short summary
Short summary
Highly Oxygenated Organic Molecules (HOMs) are key precursors of secondary organic aerosols (SOA). Incorporating the HOMs chemical mechanism into a global climate model allows for a reasonable reproduction of observed HOM characteristics. HOM-SOA constitutes a significant fraction of global SOA, and its distribution and formation pathways exhibit strong sensitivity to uncertainties in autoxidation processes and peroxy radical branching ratios.
August Mikkelsen, Daniel T. McCoy, Trude Eidhammer, Andrew Gettelman, Ci Song, Hamish Gordon, and Isabel L. McCoy
Atmos. Chem. Phys., 25, 4547–4570, https://doi.org/10.5194/acp-25-4547-2025, https://doi.org/10.5194/acp-25-4547-2025, 2025
Short summary
Short summary
Whether increased aerosol increases or decreases liquid cloud mass has been a longstanding question. Observed correlations suggest that aerosols thin liquid cloud, but we are able to show that observations were consistent with an increase in liquid cloud in response to aerosols by leveraging a model where causality could be traced.
Eric Giuffrida, Kate Johnson, Tyler Tatro, Paquita Zuidema, and Hamish Gordon
EGUsphere, https://doi.org/10.5194/egusphere-2025-511, https://doi.org/10.5194/egusphere-2025-511, 2025
Short summary
Short summary
Smoke aerosols emitted from summer African fires periodically travel across the ocean and interact with one of Earth’s largest permanent cloud decks. Researchers quantify the heating and cooling effects of this interaction using climate models. However, the use of different historical weather matching methods has produced a large variation in results. Here we test method variations commonly used today, and conclude on new guidelines for achieving the most accurate results.
Hendrik Fuchs, Aaron Stainsby, Florian Berg, René Dubus, Michelle Färber, Andreas Hofzumahaus, Frank Holland, Kelvin H. Bates, Steven S. Brown, Matthew M. Coggon, Glenn S. Diskin, Georgios I. Gkatzelis, Christopher M. Jernigan, Jeff Peischl, Michael A. Robinson, Andrew W. Rollins, Nell B. Schafer, Rebecca H. Schwantes, Chelsea E. Stockwell, Patrick R. Veres, Carsten Warneke, Eleanor M. Waxman, Lu Xu, Kristen Zuraski, Andreas Wahner, and Anna Novelli
Atmos. Meas. Tech., 18, 881–895, https://doi.org/10.5194/amt-18-881-2025, https://doi.org/10.5194/amt-18-881-2025, 2025
Short summary
Short summary
Significant improvements have been made to the instruments used to measure OH reactivity, which is equivalent to the sum of air pollutant concentrations. Accurate and precise measurements with a high time resolution have been achieved, allowing use on aircraft, as demonstrated during flights in the USA.
Xuemei Wang, Kenneth S. Carslaw, Daniel P. Grosvenor, and Hamish Gordon
EGUsphere, https://doi.org/10.5194/egusphere-2025-132, https://doi.org/10.5194/egusphere-2025-132, 2025
Short summary
Short summary
Anthropogenic emissions can influence aerosol particle number concentrations via new particle formation. Our model simulations predict around 10 % increase of the particle and cloud droplet number concentrations when doubling the emissions in the Manaus region in the Amazonian wet season. However, the corresponding changes in cloud water and rain mass are around 4 %. Such weak response implied that this convective environment is not sensitive to the localised anthropogenic emission changes here.
Barbara Ervens, Ken S. Carslaw, Thomas Koop, and Ulrich Pöschl
EGUsphere, https://doi.org/10.5194/egusphere-2025-419, https://doi.org/10.5194/egusphere-2025-419, 2025
Short summary
Short summary
Over the past two decades, the European Geosciences Union (EGU) has demonstrated the success, viability and benefits of interactive open access (OA) publishing with public peer review in its journals, its publishing platform EGUsphere and virtual compilations. The article summarizes the evolution of the EGU/Copernicus publications and of OA publishing with interactive public peer review at large by placing the EGU/Copernicus publications in the context of current and future global open science.
Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Stephen R. Arnold, Leighton A. Regayre, Duseong S. Jo, Wenxiang Shen, Hao Wang, Man Yue, Jingyi Wang, Wenxin Zhang, and Ken S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2024-4135, https://doi.org/10.5194/egusphere-2024-4135, 2025
Short summary
Short summary
This study uses a global chemistry-climate model to investigate how new particle formation (NPF) from highly oxygenated organic molecules (HOMs) contributes to cloud condensation nuclei (CCN) in both preindustrial (PI) and present-day (PD) environments, and its impact on aerosol indirect radiative forcing. The findings highlight the crucial role of biogenic emissions in climate change, providing new insights for carbon-neutral scenarios and enhancing understanding of aerosol-cloud interactions.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
Atmos. Chem. Phys., 25, 1121–1143, https://doi.org/10.5194/acp-25-1121-2025, https://doi.org/10.5194/acp-25-1121-2025, 2025
Short summary
Short summary
In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking, are increasingly important and impact air quality. This study uses a box model to evaluate how these emissions impact ozone in the Los Angeles Basin and quantifies the impact of gaseous cooking emissions. Accurate representation of these and other anthropogenic sources in inventories is crucial for informing effective air quality policies.
Lauren R. Marshall, Anja Schmidt, Andrew P. Schurer, Nathan Luke Abraham, Lucie J. Lücke, Rob Wilson, Kevin J. Anchukaitis, Gabriele C. Hegerl, Ben Johnson, Bette L. Otto-Bliesner, Esther C. Brady, Myriam Khodri, and Kohei Yoshida
Clim. Past, 21, 161–184, https://doi.org/10.5194/cp-21-161-2025, https://doi.org/10.5194/cp-21-161-2025, 2025
Short summary
Short summary
Large volcanic eruptions have caused temperature deviations over the past 1000 years; however, climate model results and reconstructions of surface cooling using tree rings do not match. We explore this mismatch using the latest models and find a better match to tree-ring reconstructions for some eruptions. Our results show that the way in which eruptions are simulated in models matters for the comparison to tree-rings, particularly regarding the spatial spread of volcanic aerosol.
Alex T. Archibald, Bablu Sinha, Maria R. Russo, Emily Matthews, Freya A. Squires, N. Luke Abraham, Stephane J.-B. Bauguitte, Thomas J. Bannan, Thomas G. Bell, David Berry, Lucy J. Carpenter, Hugh Coe, Andrew Coward, Peter Edwards, Daniel Feltham, Dwayne Heard, Jim Hopkins, James Keeble, Elizabeth C. Kent, Brian A. King, Isobel R. Lawrence, James Lee, Claire R. Macintosh, Alex Megann, Bengamin I. Moat, Katie Read, Chris Reed, Malcolm J. Roberts, Reinhard Schiemann, David Schroeder, Timothy J. Smyth, Loren Temple, Navaneeth Thamban, Lisa Whalley, Simon Williams, Huihui Wu, and Mingxi Yang
Earth Syst. Sci. Data, 17, 135–164, https://doi.org/10.5194/essd-17-135-2025, https://doi.org/10.5194/essd-17-135-2025, 2025
Short summary
Short summary
Here, we present an overview of the data generated as part of the North Atlantic Climate System Integrated Study (ACSIS) programme that are available through dedicated repositories at the Centre for Environmental Data Analysis (CEDA; www.ceda.ac.uk) and the British Oceanographic Data Centre (BODC; bodc.ac.uk). The datasets described here cover the North Atlantic Ocean, the atmosphere above (it including its composition), and Arctic sea ice.
Maria R. Russo, Sadie L. Bartholomew, David Hassell, Alex M. Mason, Erica Neininger, A. James Perman, David A. J. Sproson, Duncan Watson-Parris, and Nathan Luke Abraham
Geosci. Model Dev., 18, 181–191, https://doi.org/10.5194/gmd-18-181-2025, https://doi.org/10.5194/gmd-18-181-2025, 2025
Short summary
Short summary
Observational data and modelling capabilities have expanded in recent years, but there are still barriers preventing these two data sources from being used in synergy. Proper comparison requires generating, storing, and handling a large amount of data. This work describes the first step in the development of a new set of software tools, the VISION toolkit, which can enable the easy and efficient integration of observational and model data required for model evaluation.
Xinyi Huang, Paul R. Field, Benjamin J. Murray, Daniel P. Grosvenor, Floortje van den Heuvel, and Kenneth S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2024-4070, https://doi.org/10.5194/egusphere-2024-4070, 2025
Short summary
Short summary
Cold-air outbreak (CAO) clouds play a vital role in climate prediction. This study explores the responses of CAO clouds to aerosols and ice production under different environmental conditions. We found that CAO cloud responses vary with cloud temperature and are strongly controlled by the liquid-ice partitioning in these clouds, suggesting the importance of good representations of cloud microphysics properties to predict the behaviours of CAO clouds in a warming climate.
Ross J. Herbert, Alberto Sanchez-Marroquin, Daniel P. Grosvenor, Kirsty J. Pringle, Stephen R. Arnold, Benjamin J. Murray, and Kenneth S. Carslaw
Atmos. Chem. Phys., 25, 291–325, https://doi.org/10.5194/acp-25-291-2025, https://doi.org/10.5194/acp-25-291-2025, 2025
Short summary
Short summary
Aerosol particles that help form ice in clouds vary in number and type around the world and with time. However, in many weather and climate models cloud ice is not linked to aerosols that are known to nucleate ice. Here we report the first steps towards representing ice-nucleating particles within the UK Earth System Model. We conclude that in addition to ice nucleation by sea spray and mineral components of soil dust, we also need to represent ice nucleation by the organic components of soils.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles A. Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
Atmos. Chem. Phys., 25, 45–71, https://doi.org/10.5194/acp-25-45-2025, https://doi.org/10.5194/acp-25-45-2025, 2025
Short summary
Short summary
Using single-particle mass spectrometry, we show that trace concentrations of bromine and iodine are ubiquitous in remote tropospheric aerosol and suggest that aerosols are an important part of the global reactive iodine budget. Comparisons to a global climate model with detailed iodine chemistry are favorable in the background atmosphere; however, the model cannot replicate our measurements near the ocean surface, in biomass burning plumes, and in the stratosphere.
Erin N. Raif, Sarah L. Barr, Mark D. Tarn, James B. McQuaid, Martin I. Daily, Steven J. Abel, Paul A. Barrett, Keith N. Bower, Paul R. Field, Kenneth S. Carslaw, and Benjamin J. Murray
Atmos. Chem. Phys., 24, 14045–14072, https://doi.org/10.5194/acp-24-14045-2024, https://doi.org/10.5194/acp-24-14045-2024, 2024
Short summary
Short summary
Ice-nucleating particles (INPs) allow ice to form in clouds at temperatures warmer than −35°C. We measured INP concentrations over the Norwegian and Barents seas in weather events where cold air is ejected from the Arctic. These concentrations were among the highest measured in the Arctic. It is likely that the INPs were transported to the Arctic from distant regions. These results show it is important to consider hemispheric-scale INP processes to understand INP concentrations in the Arctic.
Pratapaditya Ghosh, Ian Boutle, Paul Field, Adrian Hill, Anthony Jones, Marie Mazoyer, Katherine J. Evans, Salil Mahajan, Hyun-Gyu Kang, Min Xu, Wei Zhang, Noah Asch, and Hamish Gordon
EGUsphere, https://doi.org/10.5194/egusphere-2024-3376, https://doi.org/10.5194/egusphere-2024-3376, 2024
Short summary
Short summary
We study aerosol-fog interactions near Paris using a weather and climate model with high spatial resolution. We show that our model can simulate fog lifecycle effectively. We find that the fog droplet number concentrations, the amount of liquid water in the fog, and the vertical structure of the fog are highly sensitive to the parameterization that simulates droplet formation and growth. The changes we propose could improve fog forecasts significantly without increasing computational costs.
Pratapaditya Ghosh, Ian Boutle, Paul Field, Adrian Hill, Marie Mazoyer, Katherine J. Evans, Salil Mahajan, Hyun-Gyu Kang, Min Xu, Wei Zhang, and Hamish Gordon
EGUsphere, https://doi.org/10.5194/egusphere-2024-3397, https://doi.org/10.5194/egusphere-2024-3397, 2024
Short summary
Short summary
We study the lifecycle of fog events in Europe using a weather and climate model. By incorporating droplet formation and growth driven by radiative cooling, our model better simulates the total liquid water in foggy atmospheric columns. We show that both adiabatic and radiative cooling play significant, often equally important roles in driving droplet formation and growth. We discuss strategies to address droplet number overpredictions, by improving model physics and addressing model artifacts.
Kadavathu Sreekumar Apsara, Jayakumar Aravindakshan, Anurose Theethai Jacob, Saji Mohandas, Paul Field, Hamish Gordan, Thara Prabhakaran, Mahen Konwar, and Vijapurap Srinivasa Prasad
EGUsphere, https://doi.org/10.5194/egusphere-2024-3538, https://doi.org/10.5194/egusphere-2024-3538, 2024
Short summary
Short summary
Science has made significant strides in weather prediction, especially for intense tropical rainfall that can lead to floods and landslides. Our study aims to improve monsoon rainfall forecasts by analyzing raindrop sizes. Using a new approach to model raindrop growth, we achieved a more accurate depiction of large rainfall events. These improvements can be generalized to enhance early warning systems, offering reliable predictions that help reduce risks from severe tropical weather events.
Masaru Yoshioka, Daniel P. Grosvenor, Ben B. B. Booth, Colin P. Morice, and Ken S. Carslaw
Atmos. Chem. Phys., 24, 13681–13692, https://doi.org/10.5194/acp-24-13681-2024, https://doi.org/10.5194/acp-24-13681-2024, 2024
Short summary
Short summary
A 2020 regulation has reduced sulfur emissions from shipping by about 80 %, leading to a decrease in atmospheric aerosols that have a cooling effect primarily by affecting cloud properties and amounts. Our climate model simulations predict a global temperature increase of 0.04 K over the next 3 decades as a result, which could contribute to surpassing the Paris Agreement's 1.5 °C target. Reduced aerosols may have also contributed to the recent temperature spikes.
Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Wenxiang Shen, Stephen R. Arnold, Leighton A. Regayre, Meinrat O. Andreae, Mira L. Pöhlker, Duseong S. Jo, Man Yue, and Ken S. Carslaw
Atmos. Chem. Phys., 24, 11365–11389, https://doi.org/10.5194/acp-24-11365-2024, https://doi.org/10.5194/acp-24-11365-2024, 2024
Short summary
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.
Zoé Brasseur, Julia Schneider, Janne Lampilahti, Ville Vakkari, Victoria A. Sinclair, Christina J. Williamson, Carlton Xavier, Dmitri Moisseev, Markus Hartmann, Pyry Poutanen, Markus Lampimäki, Markku Kulmala, Tuukka Petäjä, Katrianne Lehtipalo, Erik S. Thomson, Kristina Höhler, Ottmar Möhler, and Jonathan Duplissy
Atmos. Chem. Phys., 24, 11305–11332, https://doi.org/10.5194/acp-24-11305-2024, https://doi.org/10.5194/acp-24-11305-2024, 2024
Short summary
Short summary
Ice-nucleating particles (INPs) strongly influence the formation of clouds by initiating the formation of ice crystals. However, very little is known about the vertical distribution of INPs in the atmosphere. Here, we present aircraft measurements of INP concentrations above the Finnish boreal forest. Results show that near-surface INPs are efficiently transported and mixed within the boundary layer and occasionally reach the free troposphere.
Andrew O. Langford, Raul J. Alvarez II, Kenneth C. Aikin, Sunil Baidar, W. Alan Brewer, Steven S. Brown, Matthew M. Coggan, Patrick D. Cullis, Jessica Gilman, Georgios I. Gkatzelis, Detlev Helmig, Bryan J. Johnson, K. Emma Knowland, Rajesh Kumar, Aaron D. Lamplugh, Audra McClure-Begley, Brandi J. McCarty, Ann M. Middlebrook, Gabriele Pfister, Jeff Peischl, Irina Petropavlovskikh, Pamela S. Rickley, Andrew W. Rollins, Scott P. Sandberg, Christoph J. Senff, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2024-1938, https://doi.org/10.5194/egusphere-2024-1938, 2024
Preprint withdrawn
Short summary
Short summary
High ozone (O3) formed by reactions of nitrogen oxides (NOx) and volatile organic compounds (VOCs) can harm human health and welfare. High O3 is usually associated with hot summer days, but under certain conditions, high O3 can also form under winter conditions. In this study, we describe a high O3 event that occurred in Colorado during the COVID-19 quarantine that was caused in part by the decrease in traffic, and in part by a shallow inversion created by descent of stratospheric air.
Huisheng Bian, Mian Chin, Peter R. Colarco, Eric C. Apel, Donald R. Blake, Karl Froyd, Rebecca S. Hornbrook, Jose Jimenez, Pedro Campuzano Jost, Michael Lawler, Mingxu Liu, Marianne Tronstad Lund, Hitoshi Matsui, Benjamin A. Nault, Joyce E. Penner, Andrew W. Rollins, Gregory Schill, Ragnhild B. Skeie, Hailong Wang, Lu Xu, Kai Zhang, and Jialei Zhu
Atmos. Chem. Phys., 24, 1717–1741, https://doi.org/10.5194/acp-24-1717-2024, https://doi.org/10.5194/acp-24-1717-2024, 2024
Short summary
Short summary
This work studies sulfur in the remote troposphere at global and seasonal scales using aircraft measurements and multi-model simulations. The goal is to understand the sulfur cycle over remote oceans, spread of model simulations, and observation–model discrepancies. Such an understanding and comparison with real observations are crucial to narrow down the uncertainties in model sulfur simulations and improve understanding of the sulfur cycle in atmospheric air quality, climate, and ecosystems.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
Short summary
Short summary
This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
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
Short summary
Short summary
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
Short summary
Short summary
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.
Ben A. Cala, Scott Archer-Nicholls, James Weber, N. Luke Abraham, Paul T. Griffiths, Lorrie Jacob, Y. Matthew Shin, Laura E. Revell, Matthew Woodhouse, and Alexander T. Archibald
Atmos. Chem. Phys., 23, 14735–14760, https://doi.org/10.5194/acp-23-14735-2023, https://doi.org/10.5194/acp-23-14735-2023, 2023
Short summary
Short summary
Dimethyl sulfide (DMS) is an important trace gas emitted from the ocean recognised as setting the sulfate aerosol background, but its oxidation is complex. As a result representation in chemistry-climate models is greatly simplified. We develop and compare a new mechanism to existing mechanisms via a series of global and box model experiments. Our studies show our updated DMS scheme is a significant improvement but significant variance exists between mechanisms.
Ewa M. Bednarz, Ryan Hossaini, N. Luke Abraham, and Martyn P. Chipperfield
Geosci. Model Dev., 16, 6187–6209, https://doi.org/10.5194/gmd-16-6187-2023, https://doi.org/10.5194/gmd-16-6187-2023, 2023
Short summary
Short summary
Development and performance of the new DEST chemistry scheme of UM–UKCA is described. The scheme extends the standard StratTrop scheme by including important updates to the halogen chemistry, thus allowing process-oriented studies of stratospheric ozone depletion and recovery, including impacts from both controlled long-lived ozone-depleting substances and emerging issues around uncontrolled, very short-lived substances. It will thus aid studies in support of future ozone assessment reports.
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
Short summary
Short summary
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.
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
Short summary
Short summary
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.
Maria Rosa Russo, Brian John Kerridge, Nathan Luke Abraham, James Keeble, Barry Graham Latter, Richard Siddans, James Weber, Paul Thomas Griffiths, John Adrian Pyle, and Alexander Thomas Archibald
Atmos. Chem. Phys., 23, 6169–6196, https://doi.org/10.5194/acp-23-6169-2023, https://doi.org/10.5194/acp-23-6169-2023, 2023
Short summary
Short summary
Tropospheric ozone is an important component of the Earth system as it can affect both climate and air quality. In this work we use observed tropospheric ozone derived from satellite observations and compare it to tropospheric ozone from model simulations. Our aim is to investigate recent changes (2005–2018) in tropospheric ozone in the North Atlantic region and to understand what factors are driving such changes.
Scott Archer-Nicholls, Rachel Allen, Nathan L. Abraham, Paul T. Griffiths, and Alex T. Archibald
Atmos. Chem. Phys., 23, 5801–5813, https://doi.org/10.5194/acp-23-5801-2023, https://doi.org/10.5194/acp-23-5801-2023, 2023
Short summary
Short summary
The nitrate radical is a major oxidant at nighttime, but much less is known about it than about the other oxidants ozone and OH. We use Earth system model calculations to show how the nitrate radical has changed in abundance from 1850–2014 and to 2100 under a range of different climate and emission scenarios. Depending on the emissions and climate scenario, significant increases are projected with implications for the oxidation of volatile organic compounds and the formation of fine aerosol.
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
Short summary
Short summary
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.
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
Short summary
Short summary
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
Short summary
Short summary
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.
Fangqun Yu, Gan Luo, Arshad Arjunan Nair, Sebastian Eastham, Christina J. Williamson, Agnieszka Kupc, and Charles A. Brock
Atmos. Chem. Phys., 23, 1863–1877, https://doi.org/10.5194/acp-23-1863-2023, https://doi.org/10.5194/acp-23-1863-2023, 2023
Short summary
Short summary
Particle number concentrations and size distributions in the stratosphere are studied through model simulations and comparisons with measurements. The nucleation scheme used in most of the solar geoengineering modeling studies overpredicts the nucleation rates and particle number concentrations in the stratosphere. The model based on updated nucleation schemes captures reasonably well some aspects of particle size distributions but misses some features. The possible reasons are discussed.
Pamela S. Rickly, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Glenn M. Wolfe, Ryan Bennett, Ilann Bourgeois, John D. Crounse, Jack E. Dibb, Joshua P. DiGangi, Glenn S. Diskin, Maximilian Dollner, Emily M. Gargulinski, Samuel R. Hall, Hannah S. Halliday, Thomas F. Hanisco, Reem A. Hannun, Jin Liao, Richard Moore, Benjamin A. Nault, John B. Nowak, Jeff Peischl, Claire E. Robinson, Thomas Ryerson, Kevin J. Sanchez, Manuel Schöberl, Amber J. Soja, Jason M. St. Clair, Kenneth L. Thornhill, Kirk Ullmann, Paul O. Wennberg, Bernadett Weinzierl, Elizabeth B. Wiggins, Edward L. Winstead, and Andrew W. Rollins
Atmos. Chem. Phys., 22, 15603–15620, https://doi.org/10.5194/acp-22-15603-2022, https://doi.org/10.5194/acp-22-15603-2022, 2022
Short summary
Short summary
Biomass burning sulfur dioxide (SO2) emission factors range from 0.27–1.1 g kg-1 C. Biomass burning SO2 can quickly form sulfate and organosulfur, but these pathways are dependent on liquid water content and pH. Hydroxymethanesulfonate (HMS) appears to be directly emitted from some fire sources but is not the sole contributor to the organosulfur signal. It is shown that HMS and organosulfur chemistry may be an important S(IV) reservoir with the fate dependent on the surrounding conditions.
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
Preprint archived
Short summary
Short summary
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.
Youhua Tang, Patrick C. Campbell, Pius Lee, Rick Saylor, Fanglin Yang, Barry Baker, Daniel Tong, Ariel Stein, Jianping Huang, Ho-Chun Huang, Li Pan, Jeff McQueen, Ivanka Stajner, Jose Tirado-Delgado, Youngsun Jung, Melissa Yang, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Donald Blake, Joshua Schwarz, Jose-Luis Jimenez, James Crawford, Glenn Diskin, Richard Moore, Johnathan Hair, Greg Huey, Andrew Rollins, Jack Dibb, and Xiaoyang Zhang
Geosci. Model Dev., 15, 7977–7999, https://doi.org/10.5194/gmd-15-7977-2022, https://doi.org/10.5194/gmd-15-7977-2022, 2022
Short summary
Short summary
This paper compares two meteorological datasets for driving a regional air quality model: a regional meteorological model using WRF (WRF-CMAQ) and direct interpolation from an operational global model (GFS-CMAQ). In the comparison with surface measurements and aircraft data in summer 2019, these two methods show mixed performance depending on the corresponding meteorological settings. Direct interpolation is found to be a viable method to drive air quality models.
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
Short summary
Short summary
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.
Michael S. Diamond, Pablo E. Saide, Paquita Zuidema, Andrew S. Ackerman, Sarah J. Doherty, Ann M. Fridlind, Hamish Gordon, Calvin Howes, Jan Kazil, Takanobu Yamaguchi, Jianhao Zhang, Graham Feingold, and Robert Wood
Atmos. Chem. Phys., 22, 12113–12151, https://doi.org/10.5194/acp-22-12113-2022, https://doi.org/10.5194/acp-22-12113-2022, 2022
Short summary
Short summary
Smoke from southern Africa blankets the southeast Atlantic from June-October, overlying a major transition region between overcast and scattered clouds. The smoke affects Earth's radiation budget by absorbing sunlight and changing cloud properties. We investigate these effects in regional climate and large eddy simulation models based on international field campaigns. We find that large-scale circulation changes more strongly affect cloud transitions than smoke microphysical effects in our case.
Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah A. Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, Benjamin A. Nault, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech., 15, 4901–4930, https://doi.org/10.5194/amt-15-4901-2022, https://doi.org/10.5194/amt-15-4901-2022, 2022
Short summary
Short summary
Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
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
Short summary
Short summary
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.
Haochi Che, Philip Stier, Duncan Watson-Parris, Hamish Gordon, and Lucia Deaconu
Atmos. Chem. Phys., 22, 10789–10807, https://doi.org/10.5194/acp-22-10789-2022, https://doi.org/10.5194/acp-22-10789-2022, 2022
Short summary
Short summary
Extensive stratocumulus clouds over the south-eastern Atlantic (SEA) can lead to a cooling effect on the climate. A key pathway by which aerosols affect cloud properties is by acting as cloud condensation nuclei (CCN). Here, we investigated the source attribution of CCN in the SEA as well as the cloud responses. Our results show that aerosol nucleation contributes most to CCN in the marine boundary layer. In terms of emissions, anthropogenic sources contribute most to the CCN and cloud droplets.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, https://doi.org/10.5194/acp-22-10657-2022, 2022
Short summary
Short summary
Atmospheric impacts of chlorinated very short-lived substances (Cl-VSLS) over the first two decades of the 21st century are assessed using the UM-UKCA chemistry–climate model. Stratospheric input of Cl from Cl-VSLS is estimated at ~130 ppt in 2019. The use of model set-up with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running set-up. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
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
Short summary
Short summary
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.
Martin Breitenlechner, Gordon A. Novak, J. Andrew Neuman, Andrew W. Rollins, and Patrick R. Veres
Atmos. Meas. Tech., 15, 1159–1169, https://doi.org/10.5194/amt-15-1159-2022, https://doi.org/10.5194/amt-15-1159-2022, 2022
Short summary
Short summary
We coupled a new ion source to a commercially available state-of-the-art trace gas analyzer. The instrument is particularly well suited for conducting high-altitude observations, addressing the challenges of low ambient pressures and a complex sample matrix. The new instrument and ion source provides significant advantages to more traditional modes of operation, without sacrificing the sensitivity and flexibility of this technique.
Adam T. Ahern, Frank Erdesz, Nicholas L. Wagner, Charles A. Brock, Ming Lyu, Kyra Slovacek, Richard H. Moore, Elizabeth B. Wiggins, and Daniel M. Murphy
Atmos. Meas. Tech., 15, 1093–1105, https://doi.org/10.5194/amt-15-1093-2022, https://doi.org/10.5194/amt-15-1093-2022, 2022
Short summary
Short summary
Particles in the atmosphere play a significant role in climate change by scattering light back into space, reducing the amount of energy available to be absorbed by greenhouse gases. We built a new instrument to measure what direction light is scattered by particles, e.g., wildfire smoke. This is important because, depending on the angle of the sun, some particles scatter light into space (cooling the planet), but some light is also scattered towards the Earth (not cooling the planet).
Sarah J. Doherty, Pablo E. Saide, Paquita Zuidema, Yohei Shinozuka, Gonzalo A. Ferrada, Hamish Gordon, Marc Mallet, Kerry Meyer, David Painemal, Steven G. Howell, Steffen Freitag, Amie Dobracki, James R. Podolske, Sharon P. Burton, Richard A. Ferrare, Calvin Howes, Pierre Nabat, Gregory R. Carmichael, Arlindo da Silva, Kristina Pistone, Ian Chang, Lan Gao, Robert Wood, and Jens Redemann
Atmos. Chem. Phys., 22, 1–46, https://doi.org/10.5194/acp-22-1-2022, https://doi.org/10.5194/acp-22-1-2022, 2022
Short summary
Short summary
Between July and October, biomass burning smoke is advected over the southeastern Atlantic Ocean, leading to climate forcing. Model calculations of forcing by this plume vary significantly in both magnitude and sign. This paper compares aerosol and cloud properties observed during three NASA ORACLES field campaigns to the same in four models. It quantifies modeled biases in properties key to aerosol direct radiative forcing and evaluates how these biases propagate to biases in forcing.
Debora Griffin, Chris A. McLinden, Enrico Dammers, Cristen Adams, Chelsea E. Stockwell, Carsten Warneke, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Kyle J. Zarzana, Jake P. Rowe, Rainer Volkamer, Christoph Knote, Natalie Kille, Theodore K. Koenig, Christopher F. Lee, Drew Rollins, Pamela S. Rickly, Jack Chen, Lukas Fehr, Adam Bourassa, Doug Degenstein, Katherine Hayden, Cristian Mihele, Sumi N. Wren, John Liggio, Ayodeji Akingunola, and Paul Makar
Atmos. Meas. Tech., 14, 7929–7957, https://doi.org/10.5194/amt-14-7929-2021, https://doi.org/10.5194/amt-14-7929-2021, 2021
Short summary
Short summary
Satellite-derived NOx emissions from biomass burning are estimated with TROPOMI observations. Two common emission estimation methods are applied, and sensitivity tests with model output were performed to determine the accuracy of these methods. The effect of smoke aerosols on TROPOMI NO2 columns is estimated and compared to aircraft observations from four different aircraft campaigns measuring biomass burning plumes in 2018 and 2019 in North America.
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
Short summary
Short summary
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.
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Georgios I. Gkatzelis, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Felix Piel, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Kanako Sekimoto, Lee Thornhill, Joel A. Thornton, Geoffrey S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Carsten Warneke, Rebecca A. Washenfelder, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Armin Wisthaler, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys., 21, 16293–16317, https://doi.org/10.5194/acp-21-16293-2021, https://doi.org/10.5194/acp-21-16293-2021, 2021
Short summary
Short summary
To understand air quality impacts from wildfires, we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical
nighttimechemistry thrives and controls the fate of key smoke plume chemical processes.
Anthony C. Jones, Adrian Hill, Samuel Remy, N. Luke Abraham, Mohit Dalvi, Catherine Hardacre, Alan J. Hewitt, Ben Johnson, Jane P. Mulcahy, and Steven T. Turnock
Atmos. Chem. Phys., 21, 15901–15927, https://doi.org/10.5194/acp-21-15901-2021, https://doi.org/10.5194/acp-21-15901-2021, 2021
Short summary
Short summary
Ammonium nitrate is hard to model because it forms and evaporates rapidly. One approach is to relate its equilibrium concentration to temperature, humidity, and the amount of nitric acid and ammonia gases. Using this approach, we limit the rate at which equilibrium is reached using various condensation rates in a climate model. We show that ammonium nitrate concentrations are highly sensitive to the condensation rate. Our results will help improve the representation of nitrate in climate models.
Eric J. Hintsa, Fred L. Moore, Dale F. Hurst, Geoff S. Dutton, Bradley D. Hall, J. David Nance, Ben R. Miller, Stephen A. Montzka, Laura P. Wolton, Audra McClure-Begley, James W. Elkins, Emrys G. Hall, Allen F. Jordan, Andrew W. Rollins, Troy D. Thornberry, Laurel A. Watts, Chelsea R. Thompson, Jeff Peischl, Ilann Bourgeois, Thomas B. Ryerson, Bruce C. Daube, Yenny Gonzalez Ramos, Roisin Commane, Gregory W. Santoni, Jasna V. Pittman, Steven C. Wofsy, Eric Kort, Glenn S. Diskin, and T. Paul Bui
Atmos. Meas. Tech., 14, 6795–6819, https://doi.org/10.5194/amt-14-6795-2021, https://doi.org/10.5194/amt-14-6795-2021, 2021
Short summary
Short summary
We built UCATS to study atmospheric chemistry and transport. It has measured trace gases including CFCs, N2O, SF6, CH4, CO, and H2 with gas chromatography, as well as ozone and water vapor. UCATS has been part of missions to study the tropical tropopause; transport of air into the stratosphere; greenhouse gases, transport, and chemistry in the troposphere; and ozone chemistry, on both piloted and unmanned aircraft. Its design, capabilities, and some results are shown and described here.
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
Short summary
Short summary
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.
Charles A. Brock, Karl D. Froyd, Maximilian Dollner, Christina J. Williamson, Gregory Schill, Daniel M. Murphy, Nicholas J. Wagner, Agnieszka Kupc, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Douglas A. Day, Derek J. Price, Bernadett Weinzierl, Joshua P. Schwarz, Joseph M. Katich, Siyuan Wang, Linghan Zeng, Rodney Weber, Jack Dibb, Eric Scheuer, Glenn S. Diskin, Joshua P. DiGangi, ThaoPaul Bui, Jonathan M. Dean-Day, Chelsea R. Thompson, Jeff Peischl, Thomas B. Ryerson, Ilann Bourgeois, Bruce C. Daube, Róisín Commane, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 15023–15063, https://doi.org/10.5194/acp-21-15023-2021, https://doi.org/10.5194/acp-21-15023-2021, 2021
Short summary
Short summary
The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides a unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky.
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
Short summary
Short summary
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.
James Weber, Scott Archer-Nicholls, Nathan Luke Abraham, Youngsub M. Shin, Thomas J. Bannan, Carl J. Percival, Asan Bacak, Paulo Artaxo, Michael Jenkin, M. Anwar H. Khan, Dudley E. Shallcross, Rebecca H. Schwantes, Jonathan Williams, and Alex T. Archibald
Geosci. Model Dev., 14, 5239–5268, https://doi.org/10.5194/gmd-14-5239-2021, https://doi.org/10.5194/gmd-14-5239-2021, 2021
Short summary
Short summary
The new mechanism CRI-Strat 2 features state-of-the-art isoprene chemistry not previously available in UKCA and improves UKCA's ability to reproduce observed concentrations of isoprene, monoterpenes, and OH in tropical regions. The enhanced ability to model isoprene, the most widely emitted non-methane volatile organic compound (VOC), will allow understanding of how isoprene and other biogenic VOCs affect atmospheric composition and, through biosphere–atmosphere feedbacks, climate change.
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
Short summary
Short summary
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.
Richard H. Moore, Elizabeth B. Wiggins, Adam T. Ahern, Stephen Zimmerman, Lauren Montgomery, Pedro Campuzano Jost, Claire E. Robinson, Luke D. Ziemba, Edward L. Winstead, Bruce E. Anderson, Charles A. Brock, Matthew D. Brown, Gao Chen, Ewan C. Crosbie, Hongyu Guo, Jose L. Jimenez, Carolyn E. Jordan, Ming Lyu, Benjamin A. Nault, Nicholas E. Rothfuss, Kevin J. Sanchez, Melinda Schueneman, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Nicholas L. Wagner, and Jian Wang
Atmos. Meas. Tech., 14, 4517–4542, https://doi.org/10.5194/amt-14-4517-2021, https://doi.org/10.5194/amt-14-4517-2021, 2021
Short summary
Short summary
Atmospheric particles are everywhere and exist in a range of sizes, from a few nanometers to hundreds of microns. Because particle size determines the behavior of chemical and physical processes, accurately measuring particle sizes is an important and integral part of atmospheric field measurements! Here, we discuss the performance of two commonly used particle sizers and how changes in particle composition and optical properties may result in sizing uncertainties, which we quantify.
Christina J. Williamson, Agnieszka Kupc, Andrew Rollins, Jan Kazil, Karl D. Froyd, Eric A. Ray, Daniel M. Murphy, Gregory P. Schill, Jeff Peischl, Chelsea Thompson, Ilann Bourgeois, Thomas B. Ryerson, Glenn S. Diskin, Joshua P. DiGangi, Donald R. Blake, Thao Paul V. Bui, Maximilian Dollner, Bernadett Weinzierl, and Charles A. Brock
Atmos. Chem. Phys., 21, 9065–9088, https://doi.org/10.5194/acp-21-9065-2021, https://doi.org/10.5194/acp-21-9065-2021, 2021
Short summary
Short summary
Aerosols in the stratosphere influence climate by scattering and absorbing sunlight and through chemical reactions occurring on the particles’ surfaces. We observed more nucleation mode aerosols (small aerosols, with diameters below 12 nm) in the mid- and high-latitude lowermost stratosphere (8–13 km) in the Northern Hemisphere (NH) than in the Southern Hemisphere. The most likely cause of this is aircraft emissions, which are concentrated in the NH at similar altitudes to our observations.
John Staunton-Sykes, Thomas J. Aubry, Youngsub M. Shin, James Weber, Lauren R. Marshall, Nathan Luke Abraham, Alex Archibald, and Anja Schmidt
Atmos. Chem. Phys., 21, 9009–9029, https://doi.org/10.5194/acp-21-9009-2021, https://doi.org/10.5194/acp-21-9009-2021, 2021
Daniel M. Murphy, Karl D. Froyd, Ilann Bourgeois, Charles A. Brock, Agnieszka Kupc, Jeff Peischl, Gregory P. Schill, Chelsea R. Thompson, Christina J. Williamson, and Pengfei Yu
Atmos. Chem. Phys., 21, 8915–8932, https://doi.org/10.5194/acp-21-8915-2021, https://doi.org/10.5194/acp-21-8915-2021, 2021
Short summary
Short summary
New measurements in the lower stratosphere highlight differences between particles that originated in the troposphere or the stratosphere. The stratospheric-origin particles have relatively large radiative effects because they are at nearly the optimum diameter for light scattering. The tropospheric particles contribute significantly to surface area. These and other chemical and physical properties are then extended to study the implications if material were to be added to the stratosphere.
Caroline C. Womack, Katherine M. Manfred, Nicholas L. Wagner, Gabriela Adler, Alessandro Franchin, Kara D. Lamb, Ann M. Middlebrook, Joshua P. Schwarz, Charles A. Brock, Steven S. Brown, and Rebecca A. Washenfelder
Atmos. Chem. Phys., 21, 7235–7252, https://doi.org/10.5194/acp-21-7235-2021, https://doi.org/10.5194/acp-21-7235-2021, 2021
Short summary
Short summary
Microscopic particles interact with sunlight and affect the earth's climate in ways that are not fully understood. Aerosols from wildfire smoke present particular challenges due to their complexity in shape and composition. We demonstrate that we can experimentally measure aerosol optical properties for many types of smoke particles, using measurements of smoke from controlled burns, but that the method does not work well for smoke with high soot content.
Ashok K. Luhar, Ian E. Galbally, Matthew T. Woodhouse, and Nathan Luke Abraham
Atmos. Chem. Phys., 21, 7053–7082, https://doi.org/10.5194/acp-21-7053-2021, https://doi.org/10.5194/acp-21-7053-2021, 2021
Short summary
Short summary
Lightning-generated nitrogen oxides (LNOx) greatly influence tropospheric photochemistry. The most common parameterisation of lightning flash rate used to calculate LNOx in global composition models underestimates measurements over the ocean by a factor of 20–25. We formulate and validate an alternative parameterisation to remedy this problem. The new scheme causes an increase in the ozone burden by 8.5 % and the hydroxyl radical by 13 %, and these have implications for climate and air quality.
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
Short summary
Short summary
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.
Pamela S. Rickly, Lu Xu, John D. Crounse, Paul O. Wennberg, and Andrew W. Rollins
Atmos. Meas. Tech., 14, 2429–2439, https://doi.org/10.5194/amt-14-2429-2021, https://doi.org/10.5194/amt-14-2429-2021, 2021
Short summary
Short summary
Key improvements have been made to an in situ laser-induced fluorescence instrument for measuring SO2 in polluted and pristine environments. Laser linewidth is reduced, rapid laser tuning is implemented, and fluorescence bandpass filters are optimized. These improvements have led to a 50 % reduction in instrument detection limit. The influence of aromatic compounds was also investigated and determined to not bias SO2 measurements.
Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, https://doi.org/10.5194/acp-21-4187-2021, 2021
Short summary
Short summary
We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.
Peter Sherman, Meng Gao, Shaojie Song, Alex T. Archibald, Nathan Luke Abraham, Jean-François Lamarque, Drew Shindell, Gregory Faluvegi, and Michael B. McElroy
Atmos. Chem. Phys., 21, 3593–3605, https://doi.org/10.5194/acp-21-3593-2021, https://doi.org/10.5194/acp-21-3593-2021, 2021
Short summary
Short summary
The aims here are to assess the role of aerosols in India's monsoon precipitation and to determine the relative contributions from Chinese and Indian emissions using CMIP6 models. We find that increased sulfur emissions reduce precipitation, which is primarily dynamically driven due to spatial shifts in convection over the region. A significant increase in precipitation (up to ~ 20 %) is found only when both Indian and Chinese sulfate emissions are regulated.
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
Short summary
Short summary
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.
Fiona M. O'Connor, N. Luke Abraham, Mohit Dalvi, Gerd A. Folberth, Paul T. Griffiths, Catherine Hardacre, Ben T. Johnson, Ron Kahana, James Keeble, Byeonghyeon Kim, Olaf Morgenstern, Jane P. Mulcahy, Mark Richardson, Eddy Robertson, Jeongbyn Seo, Sungbo Shim, João C. Teixeira, Steven T. Turnock, Jonny Williams, Andrew J. Wiltshire, Stephanie Woodward, and Guang Zeng
Atmos. Chem. Phys., 21, 1211–1243, https://doi.org/10.5194/acp-21-1211-2021, https://doi.org/10.5194/acp-21-1211-2021, 2021
Short summary
Short summary
This paper calculates how changes in emissions and/or concentrations of different atmospheric constituents since the pre-industrial era have altered the Earth's energy budget at the present day using a metric called effective radiative forcing. The impact of land use change is also assessed. We find that individual contributions do not add linearly, and different Earth system interactions can affect the magnitude of the calculated effective radiative forcing.
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
Short summary
Short summary
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.
Gillian D. Thornhill, William J. Collins, Ryan J. Kramer, Dirk Olivié, Ragnhild B. Skeie, Fiona M. O'Connor, Nathan Luke Abraham, Ramiro Checa-Garcia, Susanne E. Bauer, Makoto Deushi, Louisa K. Emmons, Piers M. Forster, Larry W. Horowitz, Ben Johnson, James Keeble, Jean-Francois Lamarque, Martine Michou, Michael J. Mills, Jane P. Mulcahy, Gunnar Myhre, Pierre Nabat, Vaishali Naik, Naga Oshima, Michael Schulz, Christopher J. Smith, Toshihiko Takemura, Simone Tilmes, Tongwen Wu, Guang Zeng, and Jie Zhang
Atmos. Chem. Phys., 21, 853–874, https://doi.org/10.5194/acp-21-853-2021, https://doi.org/10.5194/acp-21-853-2021, 2021
Short summary
Short summary
This paper is a study of how different constituents in the atmosphere, such as aerosols and gases like methane and ozone, affect the energy balance in the atmosphere. Different climate models were run using the same inputs to allow an easy comparison of the results and to understand where the models differ. We found the effect of aerosols is to reduce warming in the atmosphere, but this effect varies between models. Reactions between gases are also important in affecting climate.
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
Short summary
Short summary
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.
Haochi Che, Philip Stier, Hamish Gordon, Duncan Watson-Parris, and Lucia Deaconu
Atmos. Chem. Phys., 21, 17–33, https://doi.org/10.5194/acp-21-17-2021, https://doi.org/10.5194/acp-21-17-2021, 2021
Short summary
Short summary
The south-eastern Atlantic is semi-permanently covered by some of the largest stratocumulus clouds and is influenced by one-third of the biomass burning emissions from African fires. A UKEMS1 model simulation shows that the absorption effect of biomass burning aerosols is the most significant on clouds and radiation. The dominate cooling and rapid adjustments induced by the radiative effects of biomass burning aerosols result in an overall cooling in the south-eastern Atlantic.
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
Short summary
Short summary
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
Short summary
Short summary
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.
Agnieszka Kupc, Christina J. Williamson, Anna L. Hodshire, Jan Kazil, Eric Ray, T. Paul Bui, Maximilian Dollner, Karl D. Froyd, Kathryn McKain, Andrew Rollins, Gregory P. Schill, Alexander Thames, Bernadett B. Weinzierl, Jeffrey R. Pierce, and Charles A. Brock
Atmos. Chem. Phys., 20, 15037–15060, https://doi.org/10.5194/acp-20-15037-2020, https://doi.org/10.5194/acp-20-15037-2020, 2020
Short summary
Short summary
Tropical upper troposphere over the Atlantic and Pacific oceans is a major source region of new particles. These particles are associated with the outflow from deep convection. We investigate the processes that govern the formation of these particles and their initial growth and show that none of the formation schemes commonly used in global models are consistent with observations. Using newer schemes indicates that organic compounds are likely important as nucleating and initial growth agents.
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
Short summary
Short summary
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.
Melodie Lao, Leigh R. Crilley, Leyla Salehpoor, Teles C. Furlani, Ilann Bourgeois, J. Andrew Neuman, Andrew W. Rollins, Patrick R. Veres, Rebecca A. Washenfelder, Caroline C. Womack, Cora J. Young, and Trevor C. VandenBoer
Atmos. Meas. Tech., 13, 5873–5890, https://doi.org/10.5194/amt-13-5873-2020, https://doi.org/10.5194/amt-13-5873-2020, 2020
Short summary
Short summary
Nitrous acid (HONO) is a key intermediate in the generation of oxidants and fate of nitrogen oxides in the atmosphere. High-purity calibration sources that produce stable atmospherically relevant levels under field conditions have not been made to date, reducing measurement accuracy. In this study a simple salt-coated tube humidified with water vapor is demonstrated to produce pure stable low levels of HONO, with modifications allowing the generation of higher amounts.
Martina Krämer, Christian Rolf, Nicole Spelten, Armin Afchine, David Fahey, Eric Jensen, Sergey Khaykin, Thomas Kuhn, Paul Lawson, Alexey Lykov, Laura L. Pan, Martin Riese, Andrew Rollins, Fred Stroh, Troy Thornberry, Veronika Wolf, Sarah Woods, Peter Spichtinger, Johannes Quaas, and Odran Sourdeval
Atmos. Chem. Phys., 20, 12569–12608, https://doi.org/10.5194/acp-20-12569-2020, https://doi.org/10.5194/acp-20-12569-2020, 2020
Short summary
Short summary
To improve the representations of cirrus clouds in climate predictions, extended knowledge of their properties and geographical distribution is required. This study presents extensive airborne in situ and satellite remote sensing climatologies of cirrus and humidity, which serve as a guide to cirrus clouds. Further, exemplary radiative characteristics of cirrus types and also in situ observations of tropical tropopause layer cirrus and humidity in the Asian monsoon anticyclone are shown.
Andrew Orr, J. Scott Hosking, Aymeric Delon, Lars Hoffmann, Reinhold Spang, Tracy Moffat-Griffin, James Keeble, Nathan Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 20, 12483–12497, https://doi.org/10.5194/acp-20-12483-2020, https://doi.org/10.5194/acp-20-12483-2020, 2020
Short summary
Short summary
Polar stratospheric clouds (PSCs) are clouds found in the Antarctic winter stratosphere and are implicated in the formation of the ozone hole. These clouds can sometimes be formed or enhanced by mountain waves, formed as air passes over hills or mountains. However, this important mechanism is missing in coarse-resolution climate models, limiting our ability to simulate ozone. This study examines an attempt to include the effects of mountain waves and their impact on PSCs and ozone.
Aikaterini Bougiatioti, Athanasios Nenes, Jack J. Lin, Charles A. Brock, Joost A. de Gouw, Jin Liao, Ann M. Middlebrook, and André Welti
Atmos. Chem. Phys., 20, 12163–12176, https://doi.org/10.5194/acp-20-12163-2020, https://doi.org/10.5194/acp-20-12163-2020, 2020
Short summary
Short summary
The number concentration of droplets in clouds in the summertime in the southeastern United States is influenced by aerosol variations but limited by the strong competition for supersaturated water vapor. Concurrent variations in vertical velocity magnify the response of cloud droplet number to aerosol increases by up to a factor of 5. Omitting the covariance of vertical velocity with aerosol number may therefore bias estimates of the cloud albedo effect from aerosols.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
Short summary
Short summary
With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Yohei Shinozuka, Pablo E. Saide, Gonzalo A. Ferrada, Sharon P. Burton, Richard Ferrare, Sarah J. Doherty, Hamish Gordon, Karla Longo, Marc Mallet, Yan Feng, Qiaoqiao Wang, Yafang Cheng, Amie Dobracki, Steffen Freitag, Steven G. Howell, Samuel LeBlanc, Connor Flynn, Michal Segal-Rosenhaimer, Kristina Pistone, James R. Podolske, Eric J. Stith, Joseph Ryan Bennett, Gregory R. Carmichael, Arlindo da Silva, Ravi Govindaraju, Ruby Leung, Yang Zhang, Leonhard Pfister, Ju-Mee Ryoo, Jens Redemann, Robert Wood, and Paquita Zuidema
Atmos. Chem. Phys., 20, 11491–11526, https://doi.org/10.5194/acp-20-11491-2020, https://doi.org/10.5194/acp-20-11491-2020, 2020
Short summary
Short summary
In the southeast Atlantic, well-defined smoke plumes from Africa advect over marine boundary layer cloud decks; both are most extensive around September, when most of the smoke resides in the free troposphere. A framework is put forth for evaluating the performance of a range of global and regional atmospheric composition models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016.
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
Short summary
Short summary
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.
James Weber, Scott Archer-Nicholls, Paul Griffiths, Torsten Berndt, Michael Jenkin, Hamish Gordon, Christoph Knote, and Alexander T. Archibald
Atmos. Chem. Phys., 20, 10889–10910, https://doi.org/10.5194/acp-20-10889-2020, https://doi.org/10.5194/acp-20-10889-2020, 2020
Short summary
Short summary
Highly oxygenated organic molecules (HOMs) are important for aerosol growth and new particle formation, particularly in air masses with less sulphuric acid. This new chemical mechanism reproduces measured [HOM] and [HOM precursors] and is concise enough for use in global climate models. The mechanism also reproduces the observed suppression of HOMs by isoprene, suggesting enhanced emissions may not necessarily lead to more aerosols. Greater HOM importance in the pre-industrial era is also shown.
Leighton A. Regayre, Julia Schmale, Jill S. Johnson, Christian Tatzelt, Andrea Baccarini, Silvia Henning, Masaru Yoshioka, Frank Stratmann, Martin Gysel-Beer, Daniel P. Grosvenor, and Ken S. Carslaw
Atmos. Chem. Phys., 20, 10063–10072, https://doi.org/10.5194/acp-20-10063-2020, https://doi.org/10.5194/acp-20-10063-2020, 2020
Short summary
Short summary
The amount of energy reflected back into space because of man-made particles is highly uncertain. Processes related to naturally occurring particles cause most of the uncertainty, but these processes are poorly constrained by present-day measurements. We show that measurements over the Southern Ocean, far from pollution sources, efficiently reduce climate model uncertainties. Our results pave the way to designing experiments and measurement campaigns that reduce this uncertainty even further.
Cited articles
Albrecht, B. A.: Aerosols, cloud microphysics, and fractional cloudiness,
Science, 245, 1227–1230, https://doi.org/10.1126/science.245.4923.1227, 1989.
Archibald, A. T., O'Connor, F. M., Abraham, N. L., Archer-Nicholls, S., Chipperfield, M. P., Dalvi, M., Folberth, G. A., Dennison, F., Dhomse, S. S., Griffiths, P. T., Hardacre, C., Hewitt, A. J., Hill, R. S., Johnson, C. E., Keeble, J., Köhler, M. O., Morgenstern, O., Mulcahy, J. P., Ordóñez, C., Pope, R. J., Rumbold, S. T., Russo, M. R., Savage, N. H., Sellar, A., Stringer, M., Turnock, S. T., Wild, O., and Zeng, G.: Description and evaluation of the UKCA stratosphere–troposphere chemistry scheme (StratTrop vn 1.0) implemented in UKESM1, Geosci. Model Dev., 13, 1223–1266, https://doi.org/10.5194/gmd-13-1223-2020, 2020.
Baccarini, A., Karlsson, L., Dommen, J., Duplessis, P., Vüllers, J.,
Brooks, I. M., Saiz-lopez, A., Salter, M., Tjernström, M.,
Baltensperger, U., Zieger, P., and Schmale, J.: Arctic pack ice by enhanced
iodine emissions, Nat. Commun., 11, 4924,
https://doi.org/10.1038/s41467-020-18551-0, 2018.
Bellouin, N., Quaas, J., Gryspeerdt, E., Kinne, S., Stier, P.,
Watson-Parris, D., Boucher, O., Carslaw, K. S., Christensen, M., Daniau, A.
L., Dufresne, J. L., Feingold, G., Fiedler, S., Forster, P., Gettelman, A.,
Haywood, J. M., Lohmann, U., Malavelle, F., Mauritsen, T., McCoy, D. T.,
Myhre, G., Mülmenstädt, J., Neubauer, D., Possner, A., Rugenstein,
M., Sato, Y., Schulz, M., Schwartz, S. E., Sourdeval, O., Storelvmo, T.,
Toll, V., Winker, D., and Stevens, B.: Bounding Global Aerosol Radiative
Forcing of Climate Change, Rev. Geophys., 58, e2019RG000660, https://doi.org/10.1029/2019RG000660, 2020.
Brock, C. A., Williamson, C., Kupc, A., Froyd, K. D., Erdesz, F., Wagner, N., Richardson, M., Schwarz, J. P., Gao, R.-S., Katich, J. M., Campuzano-Jost, P., Nault, B. A., Schroder, J. C., Jimenez, J. L., Weinzierl, B., Dollner, M., Bui, T., and Murphy, D. M.: Aerosol size distributions during the Atmospheric Tomography Mission (ATom): methods, uncertainties, and data products, Atmos. Meas. Tech., 12, 3081–3099, https://doi.org/10.5194/amt-12-3081-2019, 2019.
Carslaw, K. S., Lee, L. A., Reddington, C. L., Pringle, K. J., Rap, A.,
Forster, P. M., Mann, G. W., Spracklen, D. V., Woodhouse, M. T., Regayre, L.
A., and Pierce, J. R.: Large contribution of natural aerosols to uncertainty
in indirect forcing, Nature, 503, 7474, https://doi.org/10.1038/nature12674, 2013.
Clarke, A. D., Varner, J. L., Eisele, F., Mauldin, R. L., Tanner, D., and
Litchy, M.: Particle production in the remote marine atmosphere: Cloud
outflow and subsidence during ACE 1, J. Geophys. Res.-Atmos., 103, 16397–16409,
https://doi.org/10.1029/97JD02987, 1998.
Clarke, A. D., Eisele, F., Kapustin, V. N., Moore, K., Tanner, D., Mauldin,
L., Litchy, M., Lienert, B., Carroll, M. A., and Albercook, G.: Nucleation in
the equatorial free troposphere: Favorable environments during PEM-Tropics,
J. Geophys. Res.-Atmos., 104, 5735–5744, https://doi.org/10.1029/98JD02303, 1999.
Cuevas, C. A., Maffezzoli, N., Corella, J. P., Spolaor, A., Vallelonga, P.,
Kjær, H. A., Simonsen, M., Winstrup, M., Vinther, B., Horvat, C.,
Fernandez, R. P., Kinnison, D., Lamarque, J. F., Barbante, C., and
Saiz-Lopez, A.: Rapid increase in atmospheric iodine levels in the North
Atlantic since the mid-20th century, Nat. Commun., 9, 1452,
https://doi.org/10.1038/s41467-018-03756-1, 2018.
Dal Maso, M., Kulmala, M., Riipinen, I., Wagner, R., Hussein, T., Aalto, P.
P., and Lehtinen, K. E. J.: Formation and growth of fresh atmospheric
aerosols: Eight years of aerosol size distribution data from SMEAR II,
Hyytiälä, Finland, Boreal Environ. Res., 10, 323–336, 2005.
Dee, D. P., Uppala, S. M., Simmons, A. J., Berrisford, P., Poli, P.,
Kobayashi, S., Andrae, U., Balmaseda, M. A., Balsamo, G., Bauer, P.,
Bechtold, P., Beljaars, A. C. M., van de Berg, L., Bidlot, J., Bormann, N.,
Delsol, C., Dragani, R., Fuentes, M., Geer, A. J., Haimberger, L., Healy, S.
B., Hersbach, H., Hólm, E. V., Isaksen, L., Kållberg, P.,
Köhler, M., Matricardi, M., Mcnally, A. P., Monge-Sanz, B. M.,
Morcrette, J. J., Park, B. K., Peubey, C., de Rosnay, P., Tavolato, C.,
Thépaut, J. N., and Vitart, F.: The ERA-Interim reanalysis: Configuration
and performance of the data assimilation system, Q. J. Roy. Meteor. Soc., 137, 553–597,
https://doi.org/10.1002/qj.828, 2011.
Dunne, E. M., Gordon, H., Kürten, 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., Sipilä, M., Smith, J. N.,
Stozkhov, Y., Tomé, A., Tröstl, 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.
Ekman, A. M. L., Hermann, M., Gro, P., Heintzenberg, J., Kim, D., and Wang,
C.: Sub-micrometer aerosol particles in the upper troposphere/lowermost
stratosphere as measured by CARIBIC and modeled using the MIT-CAM3 global
climate model, J. Geophys. Res.-Atmos., 117, D11202, https://doi.org/10.1029/2011JD016777, 2012.
Eyring, V., Bony, S., Meehl, G. A., Senior, C. A., Stevens, B., Stouffer, R. J., and Taylor, K. E.: Overview of the Coupled Model Intercomparison Project Phase 6 (CMIP6) experimental design and organization, Geosci. Model Dev., 9, 1937–1958, https://doi.org/10.5194/gmd-9-1937-2016, 2016.
Faloona, I., Conley, S. A., Blomquist, B., Clarke, A. D., Kapustin, V.,
Howell, S., Lenschow, D. H., and Bandy, A. R.: Sulfur dioxide in the tropical
marine boundary layer: Dry deposition and heterogeneous oxidation observed
during the pacific atmospheric sulfur experiment, J. Atmos. Chem., 63, 13–32,
https://doi.org/10.1007/s10874-010-9155-0, 2009.
Flossmann, A. I. and Wobrock, W.: A review of our understanding of the
aerosol-cloud interaction from the perspective of a bin resolved cloud scale
modelling, Atmos. Res., 97, 478–497, https://doi.org/10.1016/j.atmosres.2010.05.008, 2010.
Fuchs, N. A. and Sutugin, A. G.: High-Dispersed Aerosols, in: Topics in
Current Aerosol Research, edited by: Hidy, G. M. and Brock, J. R., Pergamon, New York, 1–60, 1971.
Gantt, B., Johnson, M. S., Meskhidze, N., Sciare, J., Ovadnevaite, J., Ceburnis, D., and O'Dowd, C. D.: Model evaluation of marine primary organic aerosol emission schemes, Atmos. Chem. Phys., 12, 8553–8566, https://doi.org/10.5194/acp-12-8553-2012, 2012.
Gao, R. S., Telg, H., McLaughlin, R. J., Ciciora, S. J., Watts, L. A.,
Richardson, M. S., Schwarz, J. P., Perring, A. E., Thornberry, T. D.,
Rollins, A. W., Markovic, M. Z., Bates, T. S., Johnson, J. E., and Fahey, D.
W.: A light-weight, high-sensitivity particle spectrometer for PM2.5 aerosol
measurements, Aerosol Sci. Technol., 50, 88–99, https://doi.org/10.1080/02786826.2015.1131809,
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., Kürten, A., Lehtipalo, K., Makhmutov, V., Molteni, U.,
Rissanen, M. P., Stozkhov, Y., Tröstl, 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.
Gregory, D. and Rowntree, P. R.: A mass flux convection scheme with
representation of cloud ensemble characteristics and stability-dependent
closure, Mon. Weather Rev., 118, 1483–1506, https://doi.org/10.1175/1520-0493(1990)118<1483:AMFCSW>2.0.CO;2, 1990.
Gurciullo, C. S. and Pandis, S. N.: Effect of composition variations in
cloud droplet populations on aqueous-phase chemistry, J. Geophys., 102, 9375–9385 Res.-Atmos., https://doi.org/10.1029/96jd03651, 1997.
Heintzenberg, J., Hermann, M., Weigelt, A., Clarke, A., Kapustin, V.,
Anderson, B., Thornhill, K., van Velthoven, P., Zahn, A., and Brenninkmeijer,
C.: Near-global aerosol mapping in the upper troposphere and lowermost
stratosphere with data from the CARIBIC project, Tellus B, 63, 875–890, https://doi.org/10.1111/j.1600-0889.2011.00578.x, 2011.
Hodshire, A. L., Campuzano-Jost, P., Kodros, J. K., Croft, B., Nault, B. A., Schroder, J. C., Jimenez, J. L., and Pierce, J. R.: The potential role of methanesulfonic acid (MSA) in aerosol formation and growth and the associated radiative forcings, Atmos. Chem. Phys., 19, 3137–3160, https://doi.org/10.5194/acp-19-3137-2019, 2019.
Hodzic, A., Campuzano-Jost, P., Bian, H., Chin, M., Colarco, P. R., Day, D. A., Froyd, K. D., Heinold, B., Jo, D. S., Katich, J. M., Kodros, J. K., Nault, B. A., Pierce, J. R., Ray, E., Schacht, J., Schill, G. P., Schroder, J. C., Schwarz, J. P., Sueper, D. T., Tegen, I., Tilmes, S., Tsigaridis, K., Yu, P., and Jimenez, J. L.: Characterization of organic aerosol across the global remote troposphere: a comparison of ATom measurements and global chemistry models, Atmos. Chem. Phys., 20, 4607–4635, https://doi.org/10.5194/acp-20-4607-2020, 2020.
Hoesly, R. M., Smith, S. J., Feng, L., Klimont, Z., Janssens-Maenhout, G., Pitkanen, T., Seibert, J. J., Vu, L., Andres, R. J., Bolt, R. M., Bond, T. C., Dawidowski, L., Kholod, N., Kurokawa, J.-I., Li, M., Liu, L., Lu, Z., Moura, M. C. P., O'Rourke, P. R., and Zhang, Q.: Historical (1750–2014) anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS), Geosci. Model Dev., 11, 369–408, https://doi.org/10.5194/gmd-11-369-2018, 2018.
Hoffmann, E. H., Tilgner, A., Schrödner, R., Bräuer, P., Wolke, R.,
and Herrmann, H.: An advanced modeling study on the impacts and atmospheric
implications of multiphase dimethyl sulfide chemistry, P. Natl. Acad.
Sci. USA, 113, 11776–11781, https://doi.org/10.1073/pnas.1606320113, 2016.
Jacob, D. J., Crawford, J. H., Maring, H., Clarke, A. D., Dibb, J. E., Emmons, L. K., Ferrare, R. A., Hostetler, C. A., Russell, P. B., Singh, H. B., Thompson, A. M., Shaw, G. E., McCauley, E., Pederson, J. R., and Fisher, J. A.: The Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission: design, execution, and first results, Atmos. Chem. Phys., 10, 5191–5212, https://doi.org/10.5194/acp-10-5191-2010, 2010.
Jacobson, M. Z., Turco, R. P., Jensen, E. J., and Toon, O. B.: Modeling
coagulation among particles of different composition and size, Atmos.
Environ., 28A, 1327–1338, https://doi.org/10.1016/1352-2310(94)90280-1, 1994.
Katich, J. M., Samset, B. H., Bui, T. P., Dollner, M., Froyd, K. D.,
Campuzano-Jost, P., Nault, B. A., Schroder, J. C., Weinzierl, B., and
Schwarz, J. P.: Strong Contrast in Remote Black Carbon Aerosol Loadings
Between the Atlantic and Pacific Basins, J. Geophys. Res.-Atmos., 123, 13386–13395,
https://doi.org/10.1029/2018JD029206, 2018.
Kerminen, V. M. and Kulmala, M.: Analytical formulae connecting the “real”
and the “apparent” nucleation rate and the nuclei number concentration for
atmospheric nucleation events, J. Aerosol Sci., 33, 609–622,
https://doi.org/10.1016/S0021-8502(01)00194-X, 2002.
Kettle, A. J. and Andreae, M. O.: Flux of dimethylsulfide from the oceans: A
comparison of updated data sets and flux models, J. Geophys. Res.-Atmos., 105, 26793–26808,
https://doi.org/10.1029/2000JD900252, 2000.
Kipling, Z., Stier, P., Schwarz, J. P., Perring, A. E., Spackman, J. R., Mann, G. W., Johnson, C. E., and Telford, P. J.: Constraints on aerosol processes in climate models from vertically-resolved aircraft observations of black carbon, Atmos. Chem. Phys., 13, 5969–5986, https://doi.org/10.5194/acp-13-5969-2013, 2013.
Korhonen, H., Carslaw, K. S., Spracklen, D. V., Mann, G. W., and Woodhouse,
M. T.: Influence of oceanic dimethyl sulfide emissions on cloud condensation
nuclei concentrations and seasonality over the remote Southern Hemisphere
oceans: A global model study, J. Geophys. Res.-Atmos., 113, D15204,
https://doi.org/10.1029/2007JD009718, 2008.
Kreidenweis, S. M., Walcek, C. J., Feingold, G., Gong, W., Jacobson, M. Z.,
Kim, C. H., Liu, X., Penner, J. E., Nenes, A., and Seinfeld, J. H.:
Modification of aerosol mass and size distribution due to aqueous-phase SO2
oxidation in clouds: Comparisons of several models, J. Geophys. Res.-Atmos., 108, 4213, https://doi.org/10.1029/2002jd002697, 2003.
Kupc, A., Williamson, C., Wagner, N. L., Richardson, M., and Brock, C. A.: Modification, calibration, and performance of the Ultra-High Sensitivity Aerosol Spectrometer for particle size distribution and volatility measurements during the Atmospheric Tomography Mission (ATom) airborne campaign, Atmos. Meas. Tech., 11, 369–383, https://doi.org/10.5194/amt-11-369-2018, 2018.
Kürten, A., Williamson, C., Almeida, J., Kirkby, J., and Curtius, J.: On the derivation of particle nucleation rates from experimental formation rates, Atmos. Chem. Phys., 15, 4063–4075, https://doi.org/10.5194/acp-15-4063-2015, 2015.
Lana, A., Bell, T. G., Simó, R., Vallina, S. M., Ballabrera-Poy, J.,
Kettle, A. J., Dachs, J., Bopp, L., Saltzman, E. S., Stefels, J., Johnson,
J. E., and Liss, P. S.: An updated climatology of surface dimethlysulfide
concentrations and emission fluxes in the global ocean, Global Biogeochem.
Cy., 25, GB1004, https://doi.org/10.1029/2010GB003850, 2011.
Lee, L. A., Pringle, K. J., Reddington, C. L., Mann, G. W., Stier, P., Spracklen, D. V., Pierce, J. R., and Carslaw, K. S.: The magnitude and causes of uncertainty in global model simulations of cloud condensation nuclei, Atmos. Chem. Phys., 13, 8879–8914, https://doi.org/10.5194/acp-13-8879-2013, 2013.
Lehtinen, K. E. J., Dal Maso, M., Kulmala, M., and Kerminen, V. M.:
Estimating nucleation rates from apparent particle formation rates and vice
versa: Revised formulation of the Kerminen-Kulmala equation, J. Aerosol
Sci., 38, 988–994, https://doi.org/10.1016/j.jaerosci.2007.06.009, 2007.
Lund, M. T., Samset, B. H., Skeie, R. B., Watson-Parris, D., Katich, J. M.,
Schwarz, J. P., and Weinzierl, B.: Short Black Carbon lifetime inferred from
a global set of aircraft observations, NPJ Clim. Atmos. Sci., 1, 31,
https://doi.org/10.1038/s41612-018-0040-x, 2018.
Määttänen, A., Merikanto, J., Henschel, H., Duplissy, J.,
Makkonen, R., Ortega, I. K., and Vehkamäki, H.: New Parameterizations for
Neutral and Ion-Induced Sulfuric Acid-Water Particle Formation in Nucleation
and Kinetic Regimes, J. Geophys. Res.-Atmos., 1269–1296, https://doi.org/10.1002/2017JD027429,
2018.
Mann, G. W., Carslaw, K. S., Spracklen, D. V., Ridley, D. A., Manktelow, P. T., Chipperfield, M. P., Pickering, S. J., and Johnson, C. E.: Description and evaluation of GLOMAP-mode: a modal global aerosol microphysics model for the UKCA composition-climate model, Geosci. Model Dev., 3, 519–551, https://doi.org/10.5194/gmd-3-519-2010, 2010.
McCoy, D. T., Burrows, S. M., Wood, R., Grosvenor, D. P., Elliott, S. M.,
Ma, P. L., Rasch, P. J., and Hartmann, D. L.: Natural aerosols explain
seasonal and spatial patterns of Southern Ocean cloud albedo, Sci. Adv., 1, e1500157,
https://doi.org/10.1126/sciadv.1500157, 2015.
Merikanto, J., Spracklen, D. V., Mann, G. W., Pickering, S. J., and Carslaw, K. S.: Impact of nucleation on global CCN, Atmos. Chem. Phys., 9, 8601–8616, https://doi.org/10.5194/acp-9-8601-2009, 2009.
Metzger, A., Verheggen, B., Dommen, J., Duplissy, J., Prevot, A. S. H.,
Weingartner, E., Riipinen, I., Kulmala, M., Spracklen, D. V., Carslaw, K. S.
and Baltensperger, U.: Evidence for the role of organics in aerosol particle
formation under atmospheric conditions, P. Natl. Acad. Sci. USA, 107, 6646–6651,
https://doi.org/10.1073/pnas.0911330107, 2010.
Morgenstern, O., Braesicke, P., O'Connor, F. M., Bushell, A. C., Johnson, C. E., Osprey, S. M., and Pyle, J. A.: Evaluation of the new UKCA climate-composition model – Part 1: The stratosphere, Geosci. Model Dev., 2, 43–57, https://doi.org/10.5194/gmd-2-43-2009, 2009.
Mulcahy, J. P., Jones, C., Sellar, A., Johnson, B., Boutle, I. A., Jones,
A., Andrews, T., Rumbold, S. T., Mollard, J., Bellouin, N., Johnson, C. E.,
Williams, K. D., Grosvenor, D. P., and McCoy, D. T.: Improved Aerosol
Processes and Effective Radiative Forcing in HadGEM3 and UKESM1, J. Adv.
Model. Earth Syst., 10, 2786–2805, https://doi.org/10.1029/2018MS001464, 2018.
Mulcahy, J. P., Johnson, C., Jones, C. G., Povey, A. C., Scott, C. E., Sellar, A., Turnock, S. T., Woodhouse, M. T., Abraham, N. L., Andrews, M. B., Bellouin, N., Browse, J., Carslaw, K. S., Dalvi, M., Folberth, G. A., Glover, M., Grosvenor, D. P., Hardacre, C., Hill, R., Johnson, B., Jones, A., Kipling, Z., Mann, G., Mollard, J., O'Connor, F. M., Palmiéri, J., Reddington, C., Rumbold, S. T., Richardson, M., Schutgens, N. A. J., Stier, P., Stringer, M., Tang, Y., Walton, J., Woodward, S., and Yool, A.: Description and evaluation of aerosol in UKESM1 and HadGEM3-GC3.1 CMIP6 historical simulations, Geosci. Model Dev., 13, 6383–6423, https://doi.org/10.5194/gmd-13-6383-2020, 2020.
Myhre, G., Shindell, D., Bréon, F.-M., Collins, W., Fuglestvedt, J., Huang, J., Koch, D., Lamarque, J.-F., Lee, D., Mendoza, B., Nakajima, T., Robock, A., Stephens, G., Takemura, T., and Zhang, H.: Anthropogenic and natural radiative forcing, in Climate change 2013: The physical science basis, Contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Stocker, T., Qin, D., Plattner, G.-K., Tignor, M., Allen, S., Boschung, J., Nauels, A., Xia, Y., Bex, V., and Midgley, P., chap. 8, Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 659–740, https://doi.org/10.1017/CBO9781107415324.018, 2013.
Nadykto, A. B. and Yu, F.: Uptake of neutral polar vapor molecules by
charged clusters/particles: Enhancement due to dipole-charge interaction, J.
Geophys. Res.-Atmos., 108, 4717, https://doi.org/10.1029/2003jd003664, 2003.
O'Connor, F. M., Johnson, C. E., Morgenstern, O., Abraham, N. L., Braesicke, P., Dalvi, M., Folberth, G. A., Sanderson, M. G., Telford, P. J., Voulgarakis, A., Young, P. J., Zeng, G., Collins, W. J., and Pyle, J. A.: Evaluation of the new UKCA climate-composition model – Part 2: The Troposphere, Geosci. Model Dev., 7, 41–91, https://doi.org/10.5194/gmd-7-41-2014, 2014.
O'Dowd, C. D., Facchini, M. C., Cavalli, F., Ceburnis, D., Mircea, M.,
Decesari, S., Fuzzi, S., Young, J. Y., and Putaud, J. P.: Biogenically driven
organic contribution to marine aerosol, Nature, 431, 676–680, https://doi.org/10.1038/nature02959,
2004.
Pham, M., Boucher, O., and Hauglustaine, D.: Changes in atmospheric sulfur
burdens and concentrations and resulting radiative forcings under IPCC SRES
emission scenarios for 1990–2100, J. Geophys. Res.-Atmos., 110, D06112,
https://doi.org/10.1029/2004JD005125, 2005.
Pierce, J. R. and Adams, P. J.: Efficiency of cloud condensation nuclei formation from ultrafine particles, Atmos. Chem. Phys., 7, 1367–1379, https://doi.org/10.5194/acp-7-1367-2007, 2007.
Pierce, J. R., Leaitch, W. R., Liggio, J., Westervelt, D. M., Wainwright, C. D., Abbatt, J. P. D., Ahlm, L., Al-Basheer, W., Cziczo, D. J., Hayden, K. L., Lee, A. K. Y., Li, S.-M., Russell, L. M., Sjostedt, S. J., Strawbridge, K. B., Travis, M., Vlasenko, A., Wentzell, J. J. B., Wiebe, H. A., Wong, J. P. S., and Macdonald, A. M.: Nucleation and condensational growth to CCN sizes during a sustained pristine biogenic SOA event in a forested mountain valley, Atmos. Chem. Phys., 12, 3147–3163, https://doi.org/10.5194/acp-12-3147-2012, 2012.
Prein, A. F., Langhans, W., Fosser, G., Ferrone, A., Ban, N., Goergen, K.,
Keller, M., Tölle, M., Gutjahr, O., Feser, F., Brisson, E., Kollet, S.,
Schmidli, J., Van Lipzig, N. P. M. and Leung, R.: A review on regional
convection-permitting climate modeling: Demonstrations, prospects, and
challenges, Rev. Geophys., 53, 323–361, https://doi.org/10.1002/2014RG000475, 2015.
Ranjithkumar, A.: UKESM1 and Atom data, Zenodo, https://doi.org/10.5281/zenodo.4088640, 2020.
Regayre, L. A., Johnson, J. S., Yoshioka, M., Pringle, K. J., Sexton, D. M. H., Booth, B. B. B., Lee, L. A., Bellouin, N., and Carslaw, K. S.: Aerosol and physical atmosphere model parameters are both important sources of uncertainty in aerosol ERF, Atmos. Chem. Phys., 18, 9975–10006, https://doi.org/10.5194/acp-18-9975-2018, 2018.
Regayre, L. A., Schmale, J., Johnson, J. S., Tatzelt, C., Baccarini, A., Henning, S., Yoshioka, M., Stratmann, F., Gysel-Beer, M., Grosvenor, D. P., and Carslaw, K. S.: The value of remote marine aerosol measurements for constraining radiative forcing uncertainty, Atmos. Chem. Phys., 20, 10063–10072, https://doi.org/10.5194/acp-20-10063-2020, 2020.
Ridley, J. K., Blockley, E. W., Keen, A. B., Rae, J. G. L., West, A. E., and Schroeder, D.: The sea ice model component of HadGEM3-GC3.1, Geosci. Model Dev., 11, 713–723, https://doi.org/10.5194/gmd-11-713-2018, 2018.
Rollins, A. W., Thornberry, T. D., Ciciora, S. J., McLaughlin, R. J., Watts, L. A., Hanisco, T. F., Baumann, E., Giorgetta, F. R., Bui, T. V., Fahey, D. W., and Gao, R.-S.: A laser-induced fluorescence instrument for aircraft measurements of sulfur dioxide in the upper troposphere and lower stratosphere, Atmos. Meas. Tech., 9, 4601–4613, https://doi.org/10.5194/amt-9-4601-2016, 2016.
Samset, B. H., Stjern, C. W., Andrews, E., Kahn, R. A., Myhre, G., Schulz,
M., and Schuster, G. L.: Aerosol Absorption: Progress Towards Global and
Regional Constraints, Curr. Clim. Chang. Rep., 4, 65–83,
https://doi.org/10.1007/s40641-018-0091-4, 2018.
Schill, G. P., Froyd, K. D., Bian, H., Kupc, A., Williamson, C., Brock, C.
A., Ray, E., Hornbrook, R. S., Hills, A. J., Apel, E. C., Chin, M., Colarco,
P. R., and Murphy, D. M.: Widespread biomass burning smoke throughout the
remote troposphere, Nat. Geosci., 13, 422–427, https://doi.org/10.1038/s41561-020-0586-1, 2020.
Schutgens, N. A. J., Gryspeerdt, E., Weigum, N., Tsyro, S., Goto, D., Schulz, M., and Stier, P.: Will a perfect model agree with perfect observations? The impact of spatial sampling, Atmos. Chem. Phys., 16, 6335–6353, https://doi.org/10.5194/acp-16-6335-2016, 2016.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and physics, From
air Pollution to Climate Change, Third edit, John Wiley & Sons, Hoboken, 2016.
Sellar, A. A., Jones, C. G., Mulcahy, J., Tang, Y., Yool, A., Wiltshire, A.,
O'Connor, F. M., Stringer, M., Hill, R., Palmieri, J., Woodward, S., Mora,
L., Kuhlbrodt, T., Rumbold, S., Kelley, D. I., Ellis, R., Johnson, C. E.,
Walton, J., Abraham, N. L., Andrews, M. B., Andrews, T., Archibald, A. T.,
Berthou, S., Burke, E., Blockley, E., Carslaw, K., Dalvi, M., Edwards, J.,
Folberth, G. A., Gedney, N., Griffiths, P. T., Harper, A. B., Hendry, M. A.,
Hewitt, A. J., Johnson, B., Jones, A., Jones, C. D., Keeble, J., Liddicoat,
S., Morgenstern, O., Parker, R. J., Predoi, V., Robertson, E., Siahaan, A.,
Smith, R. S., Swaminathan, R., Woodhouse, M. T., Zeng, G., and Zerroukat, M.:
UKESM1: Description and evaluation of the UK Earth System Model, J. Adv.
Model. Earth Syst., 11, 4513–4558, https://doi.org/10.1029/2019ms001739, 2019.
Sindelarova, K., Granier, C., Bouarar, I., Guenther, A., Tilmes, S., Stavrakou, T., Müller, J.-F., Kuhn, U., Stefani, P., and Knorr, W.: Global data set of biogenic VOC emissions calculated by the MEGAN model over the last 30 years, Atmos. Chem. Phys., 14, 9317–9341, https://doi.org/10.5194/acp-14-9317-2014, 2014.
Singh, H. B., Brune, W. H., Crawford, J. H., Jacob, D. J., and Russell, P.
B.: Overview of the summer 2004 Intercontinental Chemical Transport
Experiment-North America (INTEX-A), J. Geophys. Res.-Atmos., 111, D24S01,
https://doi.org/10.1029/2006JD007905, 2006.
Spiro, P. A., Jacob, D. J., and Logan, J. A.: Global inventory of sulfur
emissions with resolution, J. Geophys.
Res., 97, 6023–6036, https://doi.org/10.1029/91JD03139, 1992.
Storkey, D., Blaker, A. T., Mathiot, P., Megann, A., Aksenov, Y., Blockley, E. W., Calvert, D., Graham, T., Hewitt, H. T., Hyder, P., Kuhlbrodt, T., Rae, J. G. L., and Sinha, B.: UK Global Ocean GO6 and GO7: a traceable hierarchy of model resolutions, Geosci. Model Dev., 11, 3187–3213, https://doi.org/10.5194/gmd-11-3187-2018, 2018.
Telford, P. J., Braesicke, P., Morgenstern, O., and Pyle, J. A.: Technical Note: Description and assessment of a nudged version of the new dynamics Unified Model, Atmos. Chem. Phys., 8, 1701–1712, https://doi.org/10.5194/acp-8-1701-2008, 2008.
Tröstl, J., Chuang, W. K., Gordon, H., Heinritzi, M., Yan, C., Molteni,
U., Ahlm, L., Frege, C., Bianchi, F., Wagner, R., Simon, M., Lehtipalo, K.,
Williamson, C., Craven, J. S., Duplissy, J., Adamov, A., Almeida, J.,
Bernhammer, A. K., Breitenlechner, M., Brilke, S., Dias, A., Ehrhart, S.,
Flagan, R. C., Franchin, A., Fuchs, C., Guida, R., Gysel, M., Hansel, A.,
Hoyle, C. R., Jokinen, T., Junninen, H., Kangasluoma, J., Keskinen, H., Kim,
J., Krapf, M., Kürten, A., Laaksonen, A., Lawler, M., Leiminger, M.,
Mathot, S., Möhler, O., Nieminen, T., Onnela, A., Petäjä, T.,
Piel, F. M., Miettinen, P., Rissanen, M. P., Rondo, L., Sarnela, N.,
Schobesberger, S., Sengupta, K., Sipilä, M., Smith, J. N., Steiner, G.,
Tomè, A., Virtanen, A., Wagner, A. C., Weingartner, E., Wimmer, D.,
Winkler, P. M., Ye, P., Carslaw, K. S., Curtius, J., Dommen, J., Kirkby, J.,
Kulmala, M., Riipinen, I., Worsnop, D. R., Donahue, N. M., and Baltensperger,
U.: The role of low-volatility organic compounds in initial particle growth
in the atmosphere, Nature, 533, 527–531, https://doi.org/10.1038/nature18271, 2016.
Twomey, S.: The Influence of Pollution on the Shortwave Albedo of Clouds, J.
Atmos. Sci., 34, 1149–1152, https://doi.org/10.1175/1520-0469(1977)034<1149:tiopot>2.0.co;2, 1977.
van Marle, M. J. E., Kloster, S., Magi, B. I., Marlon, J. R., Daniau, A.-L., Field, R. D., Arneth, A., Forrest, M., Hantson, S., Kehrwald, N. M., Knorr, W., Lasslop, G., Li, F., Mangeon, S., Yue, C., Kaiser, J. W., and van der Werf, G. R.: Historic global biomass burning emissions for CMIP6 (BB4CMIP) based on merging satellite observations with proxies and fire models (1750–2015), Geosci. Model Dev., 10, 3329–3357, https://doi.org/10.5194/gmd-10-3329-2017, 2017.
Vehkamäki, H., Kulmala, M., Napari, I., Lehtinen, K. E. J., Timmreck,
C., Noppel, M., and Laaksonen, A.: An improved parameterization for sulfuric
acid-water nucleation rates for tropospheric and stratospheric conditions,
J. Geophys. Res.-Atmos., 107, 4622, https://doi.org/10.1029/2002JD002184, 2002.
Veres, P. R., Andrew Neuman, J., Bertram, T. H., Assaf, E., Wolfe, G. M.,
Williamson, C. J., Weinzierl, B., Tilmes, S., Thompson, C. R., Thames, A.
B., Schroder, J. C., Saiz-Lopez, A., Rollins, A. W., Roberts, J. M., Price,
D., Peischl, J., Nault, B. A., Møller, K. H., Miller, D. O., Meinardi,
S., Li, Q., Lamarque, J. F., Kupc, A., Kjaergaard, H. G., Kinnison, D.,
Jimenez, J. L., Jernigan, C. M., Hornbrook, R. S., Hills, A., Dollner, M.,
Day, D. A., Cuevas, C. A., Campuzano-Jost, P., Burkholder, J., Paul Bui, T.,
Brune, W. H., Brown, S. S., Brock, C. A., Bourgeois, I., Blake, D. R., Apel,
E. C., and Ryerson, T. B.: Global airborne sampling reveals a previously
unobserved dimethyl sulfide oxidation mechanism in the marine atmosphere,
P. Natl. Acad. Sci. USA, 117, 4505–4510, https://doi.org/10.1073/pnas.1919344117, 2020.
Walters, D., Boutle, I., Brooks, M., Melvin, T., Stratton, R., Vosper, S., Wells, H., Williams, K., Wood, N., Allen, T., Bushell, A., Copsey, D., Earnshaw, P., Edwards, J., Gross, M., Hardiman, S., Harris, C., Heming, J., Klingaman, N., Levine, R., Manners, J., Martin, G., Milton, S., Mittermaier, M., Morcrette, C., Riddick, T., Roberts, M., Sanchez, C., Selwood, P., Stirling, A., Smith, C., Suri, D., Tennant, W., Vidale, P. L., Wilkinson, J., Willett, M., Woolnough, S., and Xavier, P.: The Met Office Unified Model Global Atmosphere 6.0/6.1 and JULES Global Land 6.0/6.1 configurations, Geosci. Model Dev., 10, 1487–1520, https://doi.org/10.5194/gmd-10-1487-2017, 2017.
Watson-Parris, D., Schutgens, N., Reddington, C., Pringle, K. J., Liu, D., Allan, J. D., Coe, H., Carslaw, K. S., and Stier, P.: In situ constraints on the vertical distribution of global aerosol, Atmos. Chem. Phys., 19, 11765–11790, https://doi.org/10.5194/acp-19-11765-2019, 2019.
Williamson, C., Kupc, A., Wilson, J., Gesler, D. W., Reeves, J. M., Erdesz, F., McLaughlin, R., and Brock, C. A.: Fast time response measurements of particle size distributions in the 3–60 nm size range with the nucleation mode aerosol size spectrometer, Atmos. Meas. Tech., 11, 3491–3509, https://doi.org/10.5194/amt-11-3491-2018, 2018.
Williamson, C. J., Kupc, A., Axisa, D., Bilsback, K. R., Bui, T. P.,
Campuzano-Jost, P., Dollner, M., Froyd, K. D., Hodshire, A. L., Jimenez, J.
L., Kodros, J. K., Luo, G., Murphy, D. M., Nault, B. A., Ray, E. A.,
Weinzierl, B., Wilson, J. C., Yu, F., Yu, P., Pierce, J. R., and Brock, C.
A.: A large source of cloud condensation nuclei from new particle formation
in the tropics, Nature, 574, 399–403, https://doi.org/10.1038/s41586-019-1638-9, 2019.
Wilson, D. R., Bushell, A. C., Kerr-Munslow, A. M., Price, J. D., and
Morcrette, C. J.: PC2: A prognostic cloud fraction and condensation scheme.
I: Scheme description, Q. J. Roy. Meteorol. Soc., 134, 2093–2107, https://doi.org/10.1002/qj.333, 2008.
Wofsy, S. C., Afshar, S., Allen, H. M., Apel, E. C., Asher, E. C., Barletta, B., Bent, J., Bian, H., Biggs, B. C., Blake, D. R., Blake, N., Bourgeois, I.,
Brock, C. A., Brune, W. H., Budney, J. W., Bui, T. P., Butler, A., Campuzano-Jost, P.,
Chang, C. S., Chin, M., Commane, R., Corr, G., and Zeng, L. H.: ATom: merged atmospheric chemistry, trace gases, and aerosols, data set, ORNL DAAC, Oak Ridge, Tennessee, USA, https://doi.org/10.3334/ORNLDAAC/1581, 2018.
Wood, R., Mechoso, C. R., Bretherton, C. S., Weller, R. A., Huebert, B., Straneo, F., Albrecht, B. A., Coe, H., Allen, G., Vaughan, G., Daum, P., Fairall, C., Chand, D., Gallardo Klenner, L., Garreaud, R., Grados, C., Covert, D. S., Bates, T. S., Krejci, R., Russell, L. M., de Szoeke, S., Brewer, A., Yuter, S. E., Springston, S. R., Chaigneau, A., Toniazzo, T., Minnis, P., Palikonda, R., Abel, S. J., Brown, W. O. J., Williams, S., Fochesatto, J., Brioude, J., and Bower, K. N.: The VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx): goals, platforms, and field operations, Atmos. Chem. Phys., 11, 627–654, https://doi.org/10.5194/acp-11-627-2011, 2011.
Woodward, S.: Modeling the atmospheric life cycle and radiative impact of
mineral dust in the Hadley Centre climate model, J. Geophys. Res.-Atmos., 106, 18155–18166,
https://doi.org/10.1029/2000JD900795, 2001.
Yin, Y., Carslaw, K. S., and Parker, D. J.: Redistribution of trace gases by convective clouds - mixed-phase processes, Atmos. Chem. Phys., 2, 293–306, https://doi.org/10.5194/acp-2-293-2002, 2002.
Yoshioka, M., Regayre, L. A., Pringle, K. J., Johnson, J. S., Mann, G. W.,
Partridge, D. G., Sexton, D. M. H., Lister, G. M. S., Schutgens, N., Stier,
P., Kipling, Z., Bellouin, N., Browse, J., Booth, B. B. B., Johnson, C. E.,
Johnson, B., Mollard, J. D. P., Lee, L., and Carslaw, K. S.: Ensembles of
Global Climate Model Variants Designed for the Quantification and Constraint
of Uncertainty in Aerosols and Their Radiative Forcing, J. Adv. Model. Earth
Syst., 11, 3728–3754, https://doi.org/10.1029/2019MS001628, 2019.
Yu, F. and Luo, G.: Simulation of particle size distribution with a global aerosol model: contribution of nucleation to aerosol and CCN number concentrations, Atmos. Chem. Phys., 9, 7691–7710, https://doi.org/10.5194/acp-9-7691-2009, 2009.
Yu, P., Froyd, K. D., Portmann, R. W., Toon, O. B., Freitas, S. R., Bardeen,
C. G., Brock, C., Fan, T., Gao, R. S., Katich, J. M., Kupc, A., Liu, S.,
Maloney, C., Murphy, D. M., Rosenlof, K. H., Schill, G., Schwarz, J. P., and
Williamson, C.: Efficient In-Cloud Removal of Aerosols by Deep Convection,
Geophys. Res. Lett., 46, 1061–1069, https://doi.org/10.1029/2018GL080544, 2019.
Yu, S., Eder, B., Dennis, R., Chu, S.-H., and Schwartz, S. E.: New unbiased
symmetric metrics for evaluation of air quality models, Atmos. Sci. Lett., 7, 26–34,
https://doi.org/10.1002/asl.125, 2006.
Zeng, L., Zhang, A., Wang, Y., Wagner, N. L., Katich, J. M., Schwarz, J. P.,
Schill, G. P., Brock, C., Froyd, K. D., Murphy, D. M., Williamson, C. J.,
Kupc, A., Scheuer, E., Dibb, J., and Weber, R. J.: Global Measurements of
Brown Carbon and Estimated Direct Radiative Effects, Geophys. Res. Lett., 47, e2020GL088747,
https://doi.org/10.1029/2020GL088747, 2020.
Zhang, K., Wan, H., Liu, X., Ghan, S. J., Kooperman, G. J., Ma, P.-L., Rasch, P. J., Neubauer, D., and Lohmann, U.: Technical Note: On the use of nudging for aerosol–climate model intercomparison studies, Atmos. Chem. Phys., 14, 8631–8645, https://doi.org/10.5194/acp-14-8631-2014, 2014.
Short summary
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.
The effect aerosols have on climate can be better understood by studying their vertical and...
Altmetrics
Final-revised paper
Preprint