Articles | Volume 21, issue 4
https://doi.org/10.5194/acp-21-2693-2021
© 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-21-2693-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
23 Feb 2021
Research article |
| 23 Feb 2021
| 23 Feb 2021
A global model perturbed parameter ensemble study of secondary organic aerosol formation
Kamalika Sengupta
CORRESPONDING AUTHOR
Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, UK
Kirsty Pringle
Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, UK
Jill S. Johnson
Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, UK
Carly Reddington
Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, UK
Jo Browse
Centre for Geography and Environmental Science, University of Exeter, Penryn, Cornwall, UK
Catherine E. Scott
Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, UK
Ken Carslaw
Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, UK
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Léa M. C. Prévost, Leighton A. Regayre, Jill S. Johnson, Doug McNeall, Sean Milton, and Kenneth S. Carslaw
Atmos. Chem. Phys., 26, 2487–2530, https://doi.org/10.5194/acp-26-2487-2026, https://doi.org/10.5194/acp-26-2487-2026, 2026
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Climate models rely on uncertain adjustable parameters. We tested millions of combinations of these inputs to see how well the model matches real-world data. We found that no single set of inputs can match several observations at the same time, which suggests that the issue lies in the model itself. We developed a method to detect these conflicts and trace them back trace them to their source. The aim is to help modellers target improvements that reduce uncertainty in climate projections.
Leighton A. Regayre, Léa M. C. Prévost, Kunal Ghosh, Jill S. Johnson, Jeremy E. Oakley, Jonathan Owen, Iain Webb, and Ken S. Carslaw
Atmos. Chem. Phys., 26, 2293–2317, https://doi.org/10.5194/acp-26-2293-2026, https://doi.org/10.5194/acp-26-2293-2026, 2026
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Tiny particles called aerosols affect how much sunlight the Earth reflects back into space – one of the biggest climate uncertainties. We use a large set of climate model simulations and find that uncertainty drops in some regions, but persists in other areas, after comparing models to observations. By identifying the specific processes that cause the remaining uncertainty, we guide future efforts to reduce the aerosol forcing uncertainty so we can make more reliable climate predictions.
Rachel W. N. Sansom, Jill S. Johnson, Leighton A. Regayre, Lindsay A. Lee, and Ken S. Carslaw
Atmos. Chem. Phys., 26, 1713–1733, https://doi.org/10.5194/acp-26-1713-2026, https://doi.org/10.5194/acp-26-1713-2026, 2026
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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.
Ross James Herbert, Larissa Lacher, Alexander Böhmländer, Mark D. Tarn, Antione Canzi, Aidan Pantoya, Evelyn Freney, Kristina Höhler, Pia Bogert, Celine Planche, Ping Tian, Michael Adams, Sarah Barr, David Brus, Nicole Büttner, Martin Daily, Konstantinos Doulgeris, Konstantinos Eleftheridadis, Grant Forster, Romy Fösig, Dimitrios Georgakopoulos, Maria Gini, A. Gannett Hallar, Radovan Krejci, Elke Ludewig, Mauro Mazzola, Ian B. McCubbin, Tuukka Petäjä, Joseph Robinson, Franziska Vogel, Paul Zieger, Stephen R. Arnold, Kenneth S. Carslaw, Naruki Hiranuma, Ottmar Möhler, and Benjamin J. Murray
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2026-41, https://doi.org/10.5194/essd-2026-41, 2026
Preprint under review for ESSD
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Ice formation in sub-zero clouds is influenced by airborne particles called ice-nucleating particles (INPs), whose concentrations vary substantially over short time and spatial scales. To assess the role of INPs in our climate, a comprehensive and consistent global dataset is essential. Our GloPINE model-ready dataset is a major step in this direction, comprising 36,000 measurements made using a single instrument design (PINE) over 70,000 hours of operation at 20 northern hemisphere sites.
Xinyi Huang, Paul R. Field, Ross J. Herbert, Benjamin J. Murray, Floortje van den Heuvel, Daniel P. Grosvenor, Rachel W. N. Sansom, and Kenneth S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2026-311, https://doi.org/10.5194/egusphere-2026-311, 2026
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Aerosol-cloud interactions and ice formation processes are key to modelling mixed-phase clouds in cold-air outbreaks. However, no studies have investigated the joint effects of these processes. Here, we used perturbed parameter ensembles and model emulators to show that these processes have strongly interacting effects on the properties of cold air outbreak clouds. Single sensitivity tests may therefore provide incomplete information about cloud-controlling factors.
Barbara Ervens, Ken S. Carslaw, Thomas Koop, and Ulrich Pöschl
Atmos. Chem. Phys., 25, 13903–13952, https://doi.org/10.5194/acp-25-13903-2025, https://doi.org/10.5194/acp-25-13903-2025, 2025
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Over 25 years, 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.
Hazel Mooney, Stephen Arnold, Ben Silver, Piers M. Forster, and Catherine E. Scott
Biogeosciences, 22, 5309–5328, https://doi.org/10.5194/bg-22-5309-2025, https://doi.org/10.5194/bg-22-5309-2025, 2025
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We simulate the potential changes in natural emissions of volatile gases from the land surface in the UK following afforestation from present-day woodland cover of 13 % to 19 % by 2050. We estimate present-day annual UK emissions of isoprene at 39 kt yr−1 and total monoterpenes at 46 kt yr−1, but emissions from afforested experiments show between a 3 % decrease and 123 % increase in emissions, explained by the variation in emissions activity between and within needleleaf and broadleaf trees.
Kirsty J. Pringle, Richard Rigby, Steven T. Turnock, Carly L. Reddington, Meruyert Shayakhmetova, Malcolm Illingworth, Denis Barclay, Neil Chue Hong, Ed Hawkins, Douglas S. Hamilton, Ethan Brain, and James B. McQuaid
Geosci. Commun., 8, 229–236, https://doi.org/10.5194/gc-8-229-2025, https://doi.org/10.5194/gc-8-229-2025, 2025
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The Air Quality Stripes images visualise historical changes in particulate matter air pollution in over 150 cities worldwide. The project celebrates significant improvements in air quality in regions like Europe, North America, and China while highlighting the urgent need for action in areas such as central Asia. Designed to raise awareness, the images aim to inspire discussions about the critical impact of air pollution and the global inequalities it causes.
Xinyi Huang, Paul R. Field, Benjamin J. Murray, Daniel P. Grosvenor, Floortje van den Heuvel, and Kenneth S. Carslaw
Atmos. Chem. Phys., 25, 11363–11406, https://doi.org/10.5194/acp-25-11363-2025, https://doi.org/10.5194/acp-25-11363-2025, 2025
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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.
Ken S. Carslaw, Leighton A. Regayre, Ulrike Proske, Andrew Gettelman, David M. H. Sexton, Yun Qian, Lauren Marshall, Oliver Wild, Marcus van Lier-Walqui, Annika Oertel, Saloua Peatier, Ben Yang, Jill S. Johnson, Sihan Li, Daniel T. McCoy, Benjamin M. Sanderson, Christina J. Williamson, Gregory S. Elsaesser, Kuniko Yamazaki, and Ben B. B. Booth
EGUsphere, https://doi.org/10.5194/egusphere-2025-4341, https://doi.org/10.5194/egusphere-2025-4341, 2025
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A major challenge in climate science is reducing projection uncertainty despite advances in models and observational constraints. Perturbed parameter ensembles (PPEs) offer a powerful tool to explore and reduce uncertainty by revealing model weaknesses and guiding development. PPEs are now widely applied across climate systems and scales. We argue they should be prioritized alongside complexity and resolution in model resource planning.
Xuemei Wang, Kenneth S. Carslaw, Daniel P. Grosvenor, and Hamish Gordon
Atmos. Chem. Phys., 25, 9685–9717, https://doi.org/10.5194/acp-25-9685-2025, https://doi.org/10.5194/acp-25-9685-2025, 2025
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Anthropogenic emissions can influence aerosol particle number concentrations and cloud formation. Our model simulations predict around a 10 % increase in 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 a weak response implies that this convective environment is not sensitive to the localized anthropogenic emission changes here.
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
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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.
Steven T. Turnock, Dimitris Akritidis, Larry Horowitz, Mariano Mertens, Andrea Pozzer, Carly L. Reddington, Hantao Wang, Putian Zhou, and Fiona O'Connor
Atmos. Chem. Phys., 25, 7111–7136, https://doi.org/10.5194/acp-25-7111-2025, https://doi.org/10.5194/acp-25-7111-2025, 2025
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We assess the drivers behind changes in peak-season surface ozone concentrations and risks to human health between 1850 and 2014. Substantial increases in surface ozone have occurred over this period, resulting in an increased risk to human health, driven mainly by increases in anthropogenic NOx emissions and global CH4 concentrations. Fixing anthropogenic NOx emissions at 1850 values in the near-present-day period can eliminate the risk to human health associated with exposure to surface ozone.
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
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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.
Aishah I. Shittu, Kirsty J. Pringle, Stephen R. Arnold, Richard J. Pope, Ailish M. Graham, Carly Reddington, Richard Rigby, and James B. McQuaid
Atmos. Meas. Tech., 18, 817–828, https://doi.org/10.5194/amt-18-817-2025, https://doi.org/10.5194/amt-18-817-2025, 2025
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The study highlighted the performance of Atmotube PRO sensor particulate matter (PM) data. The result showed inter-sensor variability among the Atmotube PRO sensor data. This study showed 62.5 % of the sensors used for the study exhibited greater precision in their PM2.5 measurements. The overall performance showed that sensors passed the base testing using 1 h averaged data and that a multiple linear regression model using relative humidity values improved the performance of the PM2.5 data.
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
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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.
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
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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.
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
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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.
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
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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
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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.
Connor J. Clayton, Daniel R. Marsh, Steven T. Turnock, Ailish M. Graham, Kirsty J. Pringle, Carly L. Reddington, Rajesh Kumar, and James B. McQuaid
Atmos. Chem. Phys., 24, 10717–10740, https://doi.org/10.5194/acp-24-10717-2024, https://doi.org/10.5194/acp-24-10717-2024, 2024
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We demonstrate that strong climate mitigation could improve air quality in Europe; however, less ambitious mitigation does not result in these co-benefits. We use a high-resolution atmospheric chemistry model. This allows us to demonstrate how this varies across European countries and analyse the underlying chemistry. This may help policy-facing researchers understand which sectors and regions need to be prioritised to achieve strong air quality co-benefits of climate mitigation.
Rolf Müller, Ulrich Pöschl, Thomas Koop, Thomas Peter, and Ken Carslaw
Atmos. Chem. Phys., 23, 15445–15453, https://doi.org/10.5194/acp-23-15445-2023, https://doi.org/10.5194/acp-23-15445-2023, 2023
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Paul J. Crutzen was a pioneer in atmospheric sciences and a kind-hearted, humorous person with empathy for the private lives of his colleagues and students. He made fundamental scientific contributions to a wide range of scientific topics in all parts of the atmosphere. Paul was among the founders of the journal Atmospheric Chemistry and Physics. His work will continue to be a guide for generations of scientists and environmental policymakers to come.
Hamza Ahsan, Hailong Wang, Jingbo Wu, Mingxuan Wu, Steven J. Smith, Susanne Bauer, Harrison Suchyta, Dirk Olivié, Gunnar Myhre, Hitoshi Matsui, Huisheng Bian, Jean-François Lamarque, Ken Carslaw, Larry Horowitz, Leighton Regayre, Mian Chin, Michael Schulz, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Vaishali Naik
Atmos. Chem. Phys., 23, 14779–14799, https://doi.org/10.5194/acp-23-14779-2023, https://doi.org/10.5194/acp-23-14779-2023, 2023
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We examine the impact of the assumed effective height of SO2 injection, SO2 and BC emission seasonality, and the assumed fraction of SO2 emissions injected as SO4 on climate and chemistry model results. We find that the SO2 injection height has a large impact on surface SO2 concentrations and, in some models, radiative flux. These assumptions are a
hiddensource of inter-model variability and may be leading to bias in some climate model results.
Leighton A. Regayre, Lucia Deaconu, Daniel P. Grosvenor, David M. H. Sexton, Christopher Symonds, Tom Langton, Duncan Watson-Paris, Jane P. Mulcahy, Kirsty J. Pringle, Mark Richardson, Jill S. Johnson, John W. Rostron, Hamish Gordon, Grenville Lister, Philip Stier, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 8749–8768, https://doi.org/10.5194/acp-23-8749-2023, https://doi.org/10.5194/acp-23-8749-2023, 2023
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Aerosol forcing of Earth’s energy balance has persisted as a major cause of uncertainty in climate simulations over generations of climate model development. We show that structural deficiencies in a climate model are exposed by comprehensively exploring parametric uncertainty and that these deficiencies limit how much the model uncertainty can be reduced through observational constraint. This provides a future pathway towards building models with greater physical realism and lower uncertainty.
Daniel P. Grosvenor and Kenneth S. Carslaw
Atmos. Chem. Phys., 23, 6743–6773, https://doi.org/10.5194/acp-23-6743-2023, https://doi.org/10.5194/acp-23-6743-2023, 2023
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We determine what causes long-term trends in short-wave (SW) radiative fluxes in two climate models. A positive trend occurs between 1850 and 1970 (increasing SW reflection) and a negative trend between 1970 and 2014; the pre-1970 positive trend is mainly driven by an increase in cloud droplet number concentrations due to increases in aerosol, and the 1970–2014 trend is driven by a decrease in cloud fraction, which we attribute to changes in clouds caused by greenhouse gas-induced warming.
Ernesto Reyes-Villegas, Douglas Lowe, Jill S. Johnson, Kenneth S. Carslaw, Eoghan Darbyshire, Michael Flynn, James D. Allan, Hugh Coe, Ying Chen, Oliver Wild, Scott Archer-Nicholls, Alex Archibald, Siddhartha Singh, Manish Shrivastava, Rahul A. Zaveri, Vikas Singh, Gufran Beig, Ranjeet Sokhi, and Gordon McFiggans
Atmos. Chem. Phys., 23, 5763–5782, https://doi.org/10.5194/acp-23-5763-2023, https://doi.org/10.5194/acp-23-5763-2023, 2023
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Organic aerosols (OAs), their sources and their processes remain poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem, can be a useful tool to describe primary OA (POA) production and aging. However, the main disadvantage is its complexity. We used a Gaussian process simulator to reproduce model results and to estimate the sources of model uncertainty. We do this by comparing the outputs with OA observations made at Delhi, India, in 2018.
Xuemei Wang, Hamish Gordon, Daniel P. Grosvenor, Meinrat O. Andreae, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 4431–4461, https://doi.org/10.5194/acp-23-4431-2023, https://doi.org/10.5194/acp-23-4431-2023, 2023
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New particle formation in the upper troposphere is important for the global boundary layer aerosol population, and they can be transported downward in Amazonia. We use a global and a regional model to quantify the number of aerosols that are formed at high altitude and transported downward in a 1000 km region. We find that the majority of the aerosols are from outside the region. This suggests that the 1000 km region is unlikely to be a
closed loopfor aerosol formation, transport and growth.
Ruth Price, Andrea Baccarini, Julia Schmale, Paul Zieger, Ian M. Brooks, Paul Field, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 2927–2961, https://doi.org/10.5194/acp-23-2927-2023, https://doi.org/10.5194/acp-23-2927-2023, 2023
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Arctic clouds can control how much energy is absorbed by the surface or reflected back to space. Using a computer model of the atmosphere we investigated the formation of atmospheric particles that allow cloud droplets to form. We found that particles formed aloft are transported to the lowest part of the Arctic atmosphere and that this is a key source of particles. Our results have implications for the way Arctic clouds will behave in the future as climate change continues to impact the region.
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
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We show that potential structural deficiencies in a climate model can be exposed by comprehensively exploring its parametric uncertainty, and that these deficiencies limit how much the model uncertainty can be reduced through observational constraint. Combined consideration of parametric and structural uncertainties provides a future pathway towards building models that have greater physical realism and lower uncertainty.
Ville Leinonen, Harri Kokkola, Taina Yli-Juuti, Tero Mielonen, Thomas Kühn, Tuomo Nieminen, Simo Heikkinen, Tuuli Miinalainen, Tommi Bergman, Ken Carslaw, Stefano Decesari, Markus Fiebig, Tareq Hussein, Niku Kivekäs, Radovan Krejci, Markku Kulmala, Ari Leskinen, Andreas Massling, Nikos Mihalopoulos, Jane P. Mulcahy, Steffen M. Noe, Twan van Noije, Fiona M. O'Connor, Colin O'Dowd, Dirk Olivie, Jakob B. Pernov, Tuukka Petäjä, Øyvind Seland, Michael Schulz, Catherine E. Scott, Henrik Skov, Erik Swietlicki, Thomas Tuch, Alfred Wiedensohler, Annele Virtanen, and Santtu Mikkonen
Atmos. Chem. Phys., 22, 12873–12905, https://doi.org/10.5194/acp-22-12873-2022, https://doi.org/10.5194/acp-22-12873-2022, 2022
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We provide the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five different earth system models. We investigated aerosol modes (nucleation, Aitken, and accumulation) separately and were able to show the differences between measured and modeled trends and especially their seasonal patterns. The differences in model results are likely due to complex effects of several processes instead of certain specific model features.
Amy H. Peace, Ben B. B. Booth, Leighton A. Regayre, Ken S. Carslaw, David M. H. Sexton, Céline J. W. Bonfils, and John W. Rostron
Earth Syst. Dynam., 13, 1215–1232, https://doi.org/10.5194/esd-13-1215-2022, https://doi.org/10.5194/esd-13-1215-2022, 2022
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Anthropogenic aerosol emissions have been linked to driving climate responses such as shifts in the location of tropical rainfall. However, the interaction of aerosols with climate remains one of the most uncertain aspects of climate modelling and limits our ability to predict future climate change. We use an ensemble of climate model simulations to investigate what impact the large uncertainty in how aerosols interact with climate has on predicting future tropical rainfall shifts.
Alexander D. Harrison, Daniel O'Sullivan, Michael P. Adams, Grace C. E. Porter, Edmund Blades, Cherise Brathwaite, Rebecca Chewitt-Lucas, Cassandra Gaston, Rachel Hawker, Ovid O. Krüger, Leslie Neve, Mira L. Pöhlker, Christopher Pöhlker, Ulrich Pöschl, Alberto Sanchez-Marroquin, Andrea Sealy, Peter Sealy, Mark D. Tarn, Shanice Whitehall, James B. McQuaid, Kenneth S. Carslaw, Joseph M. Prospero, and Benjamin J. Murray
Atmos. Chem. Phys., 22, 9663–9680, https://doi.org/10.5194/acp-22-9663-2022, https://doi.org/10.5194/acp-22-9663-2022, 2022
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The formation of ice in clouds fundamentally alters cloud properties; hence it is important we understand the special aerosol particles that can nucleate ice when immersed in supercooled cloud droplets. In this paper we show that African desert dust that has travelled across the Atlantic to the Caribbean nucleates ice much less well than we might have expected.
Rachel E. Hawker, Annette K. Miltenberger, Jill S. Johnson, Jonathan M. Wilkinson, Adrian A. Hill, Ben J. Shipway, Paul R. Field, Benjamin J. Murray, and Ken S. Carslaw
Atmos. Chem. Phys., 21, 17315–17343, https://doi.org/10.5194/acp-21-17315-2021, https://doi.org/10.5194/acp-21-17315-2021, 2021
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We find that ice-nucleating particles (INPs), aerosols that can initiate the freezing of cloud droplets, cause substantial changes to the properties of radiatively important convectively generated anvil cirrus. The number concentration of INPs had a large effect on ice crystal number concentration while the INP temperature dependence controlled ice crystal size and cloud fraction. The results indicate information on INP number and source is necessary for the representation of cloud glaciation.
Heather Guy, Ian M. Brooks, Ken S. Carslaw, Benjamin J. Murray, Von P. Walden, Matthew D. Shupe, Claire Pettersen, David D. Turner, Christopher J. Cox, William D. Neff, Ralf Bennartz, and Ryan R. Neely III
Atmos. Chem. Phys., 21, 15351–15374, https://doi.org/10.5194/acp-21-15351-2021, https://doi.org/10.5194/acp-21-15351-2021, 2021
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We present the first full year of surface aerosol number concentration measurements from the central Greenland Ice Sheet. Aerosol concentrations here have a distinct seasonal cycle from those at lower-altitude Arctic sites, which is driven by large-scale atmospheric circulation. Our results can be used to help understand the role aerosols might play in Greenland surface melt through the modification of cloud properties. This is crucial in a rapidly changing region where observations are sparse.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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.
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.
Rachel E. Hawker, Annette K. Miltenberger, Jonathan M. Wilkinson, Adrian A. Hill, Ben J. Shipway, Zhiqiang Cui, Richard J. Cotton, Ken S. Carslaw, Paul R. Field, and Benjamin J. Murray
Atmos. Chem. Phys., 21, 5439–5461, https://doi.org/10.5194/acp-21-5439-2021, https://doi.org/10.5194/acp-21-5439-2021, 2021
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The impact of aerosols on clouds is a large source of uncertainty for future climate projections. Our results show that the radiative properties of a complex convective cloud field in the Saharan outflow region are sensitive to the temperature dependence of ice-nucleating particle concentrations. This means that differences in the aerosol source or composition, for the same aerosol size distribution, can cause differences in the outgoing radiation from regions dominated by tropical convection.
Ananth Ranjithkumar, Hamish Gordon, Christina Williamson, Andrew Rollins, Kirsty Pringle, Agnieszka Kupc, Nathan Luke Abraham, Charles Brock, and Ken Carslaw
Atmos. Chem. Phys., 21, 4979–5014, https://doi.org/10.5194/acp-21-4979-2021, https://doi.org/10.5194/acp-21-4979-2021, 2021
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The effect aerosols have on climate can be better understood by studying their vertical and spatial distribution throughout the atmosphere. We use observation data from the ATom campaign and evaluate the vertical profile of aerosol number concentration, sulfur dioxide and condensation sink using the UKESM (UK Earth System Model). We identify uncertainties in key atmospheric processes that help improve their theoretical representation in global climate models.
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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.
Global models consistently underestimate atmospheric secondary organic aerosol (SOA), which has...
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