Articles | Volume 18, issue 3
https://doi.org/10.5194/acp-18-1629-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-18-1629-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
05 Feb 2018
Research article |
| 05 Feb 2018
Maxwell–Stefan diffusion: a framework for predicting condensed phase diffusion and phase separation in atmospheric aerosol
Kathryn Fowler
CORRESPONDING AUTHOR
School of Earth and Environmental Sciences, The University of Manchester, Manchester, M13 9PL, UK
Paul J. Connolly
School of Earth and Environmental Sciences, The University of Manchester, Manchester, M13 9PL, UK
David O. Topping
School of Earth and Environmental Sciences, The University of Manchester, Manchester, M13 9PL, UK
Simon O'Meara
School of Earth and Environmental Sciences, The University of Manchester, Manchester, M13 9PL, UK
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Observations of low–temperature cirrus clouds have found unexpectedly low ice crystal numbers and high supersaturations, suggesting an incomplete understanding of the freezing mechanisms under these conditions. The existence of viscous organic aerosol has offered alternative ice nucleation pathways, which have been observed in laboratory studies. We have developed the first cloud parcel model to investigate the effect of viscosity on ice nucleation.
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Highly oxygenated organic molecules are important contributors to secondary organic aerosol. Their yield depends on detailed atmospheric chemical composition. One important parameter is the ratio of hydroperoxy radicals to organic peroxy radicals (HO2/RO2), and we show that higher HO2/RO2 ratios lower the secondary organic aerosol yield. This is of importance as laboratory studies are often biased towards organic peroxy radicals.
Rachel L. James, Jonathan Crosier, and Paul J. Connolly
Atmos. Chem. Phys., 23, 9099–9121, https://doi.org/10.5194/acp-23-9099-2023, https://doi.org/10.5194/acp-23-9099-2023, 2023
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Matthias Karl, Liisa Pirjola, Tiia Grönholm, Mona Kurppa, Srinivasan Anand, Xiaole Zhang, Andreas Held, Rolf Sander, Miikka Dal Maso, David Topping, Shuai Jiang, Leena Kangas, and Jaakko Kukkonen
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The community aerosol dynamics model MAFOR includes several advanced features: coupling with an up-to-date chemistry mechanism for volatile organic compounds, a revised Brownian coagulation kernel that takes into account the fractal geometry of soot particles, a multitude of nucleation parameterizations, size-resolved partitioning of semi-volatile inorganics, and a hybrid method for the formation of secondary organic aerosols within the framework of condensation and evaporation.
Yunqi Shao, Yu Wang, Mao Du, Aristeidis Voliotis, M. Rami Alfarra, Simon P. O'Meara, S. Fiona Turner, and Gordon McFiggans
Atmos. Meas. Tech., 15, 539–559, https://doi.org/10.5194/amt-15-539-2022, https://doi.org/10.5194/amt-15-539-2022, 2022
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Rachel L. James, Vaughan T. J. Phillips, and Paul J. Connolly
Atmos. Chem. Phys., 21, 18519–18530, https://doi.org/10.5194/acp-21-18519-2021, https://doi.org/10.5194/acp-21-18519-2021, 2021
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Jessica Slater, Juha Tonttila, Gordon McFiggans, Paul Connolly, Sami Romakkaniemi, Thomas Kühn, and Hugh Coe
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David Topping, David Watts, Hugh Coe, James Evans, Thomas J. Bannan, Douglas Lowe, Caroline Jay, and Jonathan W. Taylor
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-270, https://doi.org/10.5194/gmd-2020-270, 2020
Publication in GMD not foreseen
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Petroc D. Shelley, Thomas J. Bannan, Stephen D. Worrall, M. Rami Alfarra, Ulrich K. Krieger, Carl J. Percival, Arthur Garforth, and David Topping
Atmos. Chem. Phys., 20, 8293–8314, https://doi.org/10.5194/acp-20-8293-2020, https://doi.org/10.5194/acp-20-8293-2020, 2020
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The methods used to estimate the vapour pressures of compounds in the atmosphere typically perform poorly when applied to organic compounds found in the atmosphere. New measurements have been made and compared to previous experimental data and estimated values so that the limitations within the estimation methods can be identified and in the future be rectified.
Natalie R. Gervasi, David O. Topping, and Andreas Zuend
Atmos. Chem. Phys., 20, 2987–3008, https://doi.org/10.5194/acp-20-2987-2020, https://doi.org/10.5194/acp-20-2987-2020, 2020
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Organic aerosols have been shown to exist often in a semi-solid or amorphous, glassy state. Highly viscous particles behave differently than their well-mixed liquid analogues with consequences for a variety of aerosol processes. Here, we introduce a new predictive mixture viscosity model called AIOMFAC-VISC. It enables us to predict the viscosity of aqueous organic mixtures as a function of temperature and chemical composition, covering the full range of liquid, semi-solid, and glassy states.
Parya Broomandi, Xueyu Geng, Weisi Guo, Jong Ryeol Kim, Alessio Pagani, and David Topping
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2019-342, https://doi.org/10.5194/gmd-2019-342, 2020
Revised manuscript not accepted
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As a result of our novel graph-based reduced modeling, we are able to represent high-dimensional knowledge into a causal inference and stability framework.
Kathryn Fowler, Paul Connolly, and David Topping
Atmos. Chem. Phys., 20, 683–698, https://doi.org/10.5194/acp-20-683-2020, https://doi.org/10.5194/acp-20-683-2020, 2020
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Observations of low–temperature cirrus clouds have found unexpectedly low ice crystal numbers and high supersaturations, suggesting an incomplete understanding of the freezing mechanisms under these conditions. The existence of viscous organic aerosol has offered alternative ice nucleation pathways, which have been observed in laboratory studies. We have developed the first cloud parcel model to investigate the effect of viscosity on ice nucleation.
Jonathan W. Taylor, Sophie L. Haslett, Keith Bower, Michael Flynn, Ian Crawford, James Dorsey, Tom Choularton, Paul J. Connolly, Valerian Hahn, Christiane Voigt, Daniel Sauer, Régis Dupuy, Joel Brito, Alfons Schwarzenboeck, Thierry Bourriane, Cyrielle Denjean, Phil Rosenberg, Cyrille Flamant, James D. Lee, Adam R. Vaughan, Peter G. Hill, Barbara Brooks, Valéry Catoire, Peter Knippertz, and Hugh Coe
Atmos. Chem. Phys., 19, 8503–8522, https://doi.org/10.5194/acp-19-8503-2019, https://doi.org/10.5194/acp-19-8503-2019, 2019
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Low-level clouds cover a wide area of southern West Africa (SWA) and play an important role in the region's climate, reflecting sunlight away from the surface. We performed aircraft measurements of aerosols and clouds over SWA during the 2016 summer monsoon and found pollution, and polluted clouds, across the whole region. Smoke from biomass burning in Central Africa is transported to West Africa, causing a polluted background which limits the effect of local pollution on cloud properties.
Thomas J. Bannan, Michael Le Breton, Michael Priestley, Stephen D. Worrall, Asan Bacak, Nicholas A. Marsden, Archit Mehra, Julia Hammes, Mattias Hallquist, M. Rami Alfarra, Ulrich K. Krieger, Jonathan P. Reid, John Jayne, Wade Robinson, Gordon McFiggans, Hugh Coe, Carl J. Percival, and Dave Topping
Atmos. Meas. Tech., 12, 1429–1439, https://doi.org/10.5194/amt-12-1429-2019, https://doi.org/10.5194/amt-12-1429-2019, 2019
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The Filter Inlet for Gases and AEROsols (FIGAERO) is an inlet designed to be coupled with a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) and provides simultaneous molecular information relating to both the gas- and particle-phase samples. This method has been used to extract vapour pressures of compounds whilst giving quantitative concentrations in the particle phase. Here we detail an ideal set of benchmark compounds for characterization of the FIGAERO.
Elizabeth Forde, Martin Gallagher, Virginia Foot, Roland Sarda-Esteve, Ian Crawford, Paul Kaye, Warren Stanley, and David Topping
Atmos. Chem. Phys., 19, 1665–1684, https://doi.org/10.5194/acp-19-1665-2019, https://doi.org/10.5194/acp-19-1665-2019, 2019
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The abundance and diversity of airborne biological particles in different environments remains poorly constrained. Measurements of such particles were conducted at four sites in the United Kingdom, using real-time fluorescence instrumentation. Using local land cover types, sources of suspected particle types were identified and compared. Most sites exhibited a wet-discharged fungal spore dominance, with the exception of one site, which was inferred to be influenced by a local dairy farm.
Simon Ruske, David O. Topping, Virginia E. Foot, Andrew P. Morse, and Martin W. Gallagher
Atmos. Meas. Tech., 11, 6203–6230, https://doi.org/10.5194/amt-11-6203-2018, https://doi.org/10.5194/amt-11-6203-2018, 2018
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Pollen, bacteria and fungal spores are common in the environment, can have very important implications for public health and may influence the weather. Biological sensors potentially could be used to monitor quantities of these types of particles. However, it is important to transform the measurements from these instruments into counts of these biological particles. The paper tests a variety of approaches for achieving this aim on data collected in a laboratory.
Dawei Hu, David Topping, and Gordon McFiggans
Atmos. Chem. Phys., 18, 14925–14937, https://doi.org/10.5194/acp-18-14925-2018, https://doi.org/10.5194/acp-18-14925-2018, 2018
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Co-condensation of inorganic or organic vapours on growing droplets could significantly enhance both CCN and cloud droplet number concentration, thereby influencing climate. Until now, there has been very few direct observational evidence of this process. We exposed involatile inorganic particles to a moist atmosphere containing a controlled amount of an organic semi-volatile vapour. We measured a much greater growth of the particles than if they had only been exposed to water vapour.
Matthew Crooks, Paul Connolly, and Gordon McFiggans
Geosci. Model Dev., 11, 3261–3278, https://doi.org/10.5194/gmd-11-3261-2018, https://doi.org/10.5194/gmd-11-3261-2018, 2018
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Clouds form when water condenses onto particles in the atmosphere and the size and chemical composition of these particles can have a large influence over how much water condenses and the subsequent formation of cloud. Additional gases exist in the atmosphere that can condense onto the aerosol particles and change their composition. We present a fast and efficient method of calculating the effect of atmospheric gases on the formation of cloud that can be used in climate and weather models.
Robin G. Stevens, Katharina Loewe, Christopher Dearden, Antonios Dimitrelos, Anna Possner, Gesa K. Eirund, Tomi Raatikainen, Adrian A. Hill, Benjamin J. Shipway, Jonathan Wilkinson, Sami Romakkaniemi, Juha Tonttila, Ari Laaksonen, Hannele Korhonen, Paul Connolly, Ulrike Lohmann, Corinna Hoose, Annica M. L. Ekman, Ken S. Carslaw, and Paul R. Field
Atmos. Chem. Phys., 18, 11041–11071, https://doi.org/10.5194/acp-18-11041-2018, https://doi.org/10.5194/acp-18-11041-2018, 2018
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We perform a model intercomparison of summertime high Arctic clouds. Observed concentrations of aerosol particles necessary for cloud formation fell to extremely low values, coincident with a transition from cloudy to nearly cloud-free conditions. Previous analyses have suggested that at these low concentrations, the radiative properties of the clouds are determined primarily by these particle concentrations. The model results strongly support this hypothesis.
Michael Le Breton, Yujue Wang, Åsa M. Hallquist, Ravi Kant Pathak, Jing Zheng, Yudong Yang, Dongjie Shang, Marianne Glasius, Thomas J. Bannan, Qianyun Liu, Chak K. Chan, Carl J. Percival, Wenfei Zhu, Shengrong Lou, David Topping, Yuchen Wang, Jianzhen Yu, Keding Lu, Song Guo, Min Hu, and Mattias Hallquist
Atmos. Chem. Phys., 18, 10355–10371, https://doi.org/10.5194/acp-18-10355-2018, https://doi.org/10.5194/acp-18-10355-2018, 2018
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This paper utilizes a chemical ionisation mass spectrometer measuring gas and particle-phase organosulfates (OS) simultaneously during a field campaign in Beijing, China, and highlights how high time frequency online measurements enable a detailed analysis of dominant production mechanisms. We find that high aerosol acidity, organic precursor concentration and relative humidity promote the production of OS. The thermogram desorption reveals the potential for semi-volatile gas-phase OS.
Wiebke Frey, Dawei Hu, James Dorsey, M. Rami Alfarra, Aki Pajunoja, Annele Virtanen, Paul Connolly, and Gordon McFiggans
Atmos. Chem. Phys., 18, 9393–9409, https://doi.org/10.5194/acp-18-9393-2018, https://doi.org/10.5194/acp-18-9393-2018, 2018
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The coupled system of the Manchester Aerosol Chamber and Manchester Ice Cloud Chamber was used to study the ice-forming abilities of secondary
organic aerosol particles under mixed-phase cloud conditions. Given the vast abundance of secondary organic particles in the atmosphere, they
might present an important contribution to ice-nucleating particles. However, we find that in the studied temperature range (20 to 28 °C)
the secondary organic particles do not nucleate ice particles.
Emma L. Simpson, Paul J. Connolly, and Gordon McFiggans
Atmos. Chem. Phys., 18, 7237–7250, https://doi.org/10.5194/acp-18-7237-2018, https://doi.org/10.5194/acp-18-7237-2018, 2018
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This study explores the process of ice formation in clouds by conducting computer model simulations and laboratory experiments in a cloud chamber. We show that the formation of ice in clouds can be limited by the presence of atmospheric aerosol particles and that further research is required to identify the requirements for freezing, e.g. minimum mass of water, in order to accurately calculate ice formation and thus improve climate and weather prediction.
Stefano Decesari, Simona Kovarich, Manuela Pavan, Arianna Bassan, Andrea Ciacci, and David Topping
Atmos. Chem. Phys., 18, 2329–2340, https://doi.org/10.5194/acp-18-2329-2018, https://doi.org/10.5194/acp-18-2329-2018, 2018
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Particulate matter (PM) chemical composition includes thousands of individual organic compounds that have never been tested for their toxicological potential. Computational (in silico) screenings represent a promising approach to identify new target compounds for more in-depth toxicological analyses. We provide here a proof-of-concept evaluation based on ca. 100 aerosol organic compounds. Reliable toxicological predictions were obtained for more than 80 % of them.
Gillian Young, Paul J. Connolly, Christopher Dearden, and Thomas W. Choularton
Atmos. Chem. Phys., 18, 1475–1494, https://doi.org/10.5194/acp-18-1475-2018, https://doi.org/10.5194/acp-18-1475-2018, 2018
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Large-scale subsidence, associated with high-pressure systems, is often used in cloud-resolving models to maintain the height of boundary layer clouds; however, its influence on the small-scale interactions in mixed-phase clouds has not been previously investigated. Using large-eddy simulations, we have identified a relationship between subsidence and convection development in such clouds, with implications for mixed-phase boundary layer clouds forming in the ocean-exposed Arctic regions.
Olivia Goulden, Matthew Crooks, and Paul Connolly
Atmos. Chem. Phys., 18, 275–287, https://doi.org/10.5194/acp-18-275-2018, https://doi.org/10.5194/acp-18-275-2018, 2018
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The formation of cloud from the condensation of water vapour in the atmosphere on aerosol particles is highly dependent of the chemical properties of the particles. The chemistry is further complicated by the presence of condensible gases in the atmosphere other than water. We provide several methods of including the complicated chemical properties of the aerosol particles and condensing gases into single parameter descriptions, which are suitable for inclusion in large-scale models.
Ulrich K. Krieger, Franziska Siegrist, Claudia Marcolli, Eva U. Emanuelsson, Freya M. Gøbel, Merete Bilde, Aleksandra Marsh, Jonathan P. Reid, Andrew J. Huisman, Ilona Riipinen, Noora Hyttinen, Nanna Myllys, Theo Kurtén, Thomas Bannan, Carl J. Percival, and David Topping
Atmos. Meas. Tech., 11, 49–63, https://doi.org/10.5194/amt-11-49-2018, https://doi.org/10.5194/amt-11-49-2018, 2018
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Vapor pressures of low-volatility organic molecules at atmospheric temperatures reported in the literature often differ by several orders of magnitude between measurement techniques. These discrepancies exceed the stated uncertainty of each technique, which is generally reported to be smaller than a factor of 2. We determined saturation vapor pressures for the homologous series of polyethylene glycols ranging in vapor pressure at 298 K from 1E−7 Pa to 5E−2 Pa as a reference set.
Simon O'Meara, David O. Topping, Rahul A. Zaveri, and Gordon McFiggans
Atmos. Chem. Phys., 17, 10477–10494, https://doi.org/10.5194/acp-17-10477-2017, https://doi.org/10.5194/acp-17-10477-2017, 2017
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To simulate particle-phase diffusion, an analytical expression is desired because it takes less calculation time than a differential equation. Here a correction is found for the analytical solution for when diffusivity is dependent on composition, thereby making it more widely applicable than before. Consequently, we are able to more realistically evaluate the rate limitation (if any) imposed by particle-phase diffusion on component partitioning between the gas and particle phase.
Leonid Nichman, Emma Järvinen, James Dorsey, Paul Connolly, Jonathan Duplissy, Claudia Fuchs, Karoliina Ignatius, Kamalika Sengupta, Frank Stratmann, Ottmar Möhler, Martin Schnaiter, and Martin Gallagher
Atmos. Meas. Tech., 10, 3231–3248, https://doi.org/10.5194/amt-10-3231-2017, https://doi.org/10.5194/amt-10-3231-2017, 2017
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Optical probes are frequently used for the detection of cloud particles. The detected microphysical properties may affect particle growth and accretion mechanisms and the light scattering properties of cirrus clouds. In the CLOUD chamber study at CERN, we compared four optical measurement techniques. We show that shape derivation alone is not sufficient to determine the phase of the small cloud particles. None of the instruments were able to unambiguously determine the phase of small particles.
David O. Topping, James Allan, M. Rami Alfarra, and Bernard Aumont
Geosci. Model Dev., 10, 2365–2377, https://doi.org/10.5194/gmd-10-2365-2017, https://doi.org/10.5194/gmd-10-2365-2017, 2017
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Our ability to model the chemical and thermodynamic processes that lead to secondary organic aerosol (SOA) formation is thought to be hampered by the complexity of the system. In this proof of concept study, the ability to train supervised methods to predict electron impact ionisation (EI) mass spectra for the AMS is evaluated to facilitate improved model evaluation. The study demonstrates the use of a methodology that would be improved with more training data and data from simple mixed systems.
Gillian Young, Paul J. Connolly, Hazel M. Jones, and Thomas W. Choularton
Atmos. Chem. Phys., 17, 4209–4227, https://doi.org/10.5194/acp-17-4209-2017, https://doi.org/10.5194/acp-17-4209-2017, 2017
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Arctic mixed-phase clouds are poorly represented in numerical models, due in part to an overpredicted ice phase. Here, we examine the sensitivity of cloud structure, evolution, and lifetime to modelled primary ice number concentrations over three different surfaces – sea ice, marginal ice, and ocean – to investigate the dependency on both the ice phase and dynamics induced from surface fluxes.
Simon Ruske, David O. Topping, Virginia E. Foot, Paul H. Kaye, Warren R. Stanley, Ian Crawford, Andrew P. Morse, and Martin W. Gallagher
Atmos. Meas. Tech., 10, 695–708, https://doi.org/10.5194/amt-10-695-2017, https://doi.org/10.5194/amt-10-695-2017, 2017
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Particles such as bacteria, pollen and fungal spores have important implications within the environment and public health sectors. Here we evaluate the performance of various different methods for distinguishing between these different types of particles using a new instrument. We demonstrate that there may be better alternatives to the currently used methods which can be further investigated in future research.
Gillian Young, Hazel M. Jones, Thomas W. Choularton, Jonathan Crosier, Keith N. Bower, Martin W. Gallagher, Rhiannon S. Davies, Ian A. Renfrew, Andrew D. Elvidge, Eoghan Darbyshire, Franco Marenco, Philip R. A. Brown, Hugo M. A. Ricketts, Paul J. Connolly, Gary Lloyd, Paul I. Williams, James D. Allan, Jonathan W. Taylor, Dantong Liu, and Michael J. Flynn
Atmos. Chem. Phys., 16, 13945–13967, https://doi.org/10.5194/acp-16-13945-2016, https://doi.org/10.5194/acp-16-13945-2016, 2016
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Clouds are intricately coupled to the Arctic sea ice. Our inability to accurately model cloud fractions causes large uncertainties in predicted radiative interactions in this region, therefore, affecting sea ice forecasts. Here, we present measurements of cloud microphysics, aerosol properties, and thermodynamic structure over the transition from sea ice to ocean to improve our understanding of the relationship between the Arctic atmosphere and clouds which develop in this region.
François Benduhn, Graham W. Mann, Kirsty J. Pringle, David O. Topping, Gordon McFiggans, and Kenneth S. Carslaw
Geosci. Model Dev., 9, 3875–3906, https://doi.org/10.5194/gmd-9-3875-2016, https://doi.org/10.5194/gmd-9-3875-2016, 2016
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We present a new mathematical formalism that serves to represent exchanges of inorganic matter between the atmosphere gas phase and the aerosol aqueous phase. In a global modelling framework, taking into account these processes may help represent many important features more accurately, such as the formation of cloud droplets or the radiative properties of the atmosphere. The formalism strives to keep an appropriate balance between accuracy and computation efficiency requirements.
Matthew Crooks, Paul Connolly, David Topping, and Gordon McFiggans
Geosci. Model Dev., 9, 3617–3637, https://doi.org/10.5194/gmd-9-3617-2016, https://doi.org/10.5194/gmd-9-3617-2016, 2016
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Semi-volatile compounds, like water, can exist in both vapour phases and condensed phases within a system. This paper presents a method of calculating the condensed and vapour phases of semi-volatile compounds at equilibrium, in particular, when the condensed mass occurs within particles of different sizes and chemical composition. The applications of interest to the authors are those of atmospheric importance such as cloud droplet formation and reflection or absorption of solar radiation.
Samuel Lowe, Daniel G. Partridge, David Topping, and Philip Stier
Atmos. Chem. Phys., 16, 10941–10963, https://doi.org/10.5194/acp-16-10941-2016, https://doi.org/10.5194/acp-16-10941-2016, 2016
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A novel inverse modelling framework is developed for analysing the sensitivity of cloud condensation nuclei (CCN) concentrations to simultaneous perturbations in multiple model parameters at atmospherically relevant humidities. Many parameter interactions are identified and CCN concentrations are found to be relatively insensitive to bulk–surface partitioning, while aerosol concentration, surface tension, composition and solution ideality exhibit a higher degree of sensitivity.
Simon O'Meara, David O. Topping, and Gordon McFiggans
Atmos. Chem. Phys., 16, 5299–5313, https://doi.org/10.5194/acp-16-5299-2016, https://doi.org/10.5194/acp-16-5299-2016, 2016
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To understand the effect of atmospheric particulate matter on climate and human health we need to know how it evolves. We investigate how best to estimate diffusion of components through particles by comparing diffusion times from three approaches to solving Fick's Law and find that they agree. This means that scientists can simulate Fickian diffusion through atmospheric particles using the approach best suited to their requirements and have confidence that their model is mathematically sound.
Robert J. Farrington, Paul J. Connolly, Gary Lloyd, Keith N. Bower, Michael J. Flynn, Martin W. Gallagher, Paul R. Field, Chris Dearden, and Thomas W. Choularton
Atmos. Chem. Phys., 16, 4945–4966, https://doi.org/10.5194/acp-16-4945-2016, https://doi.org/10.5194/acp-16-4945-2016, 2016
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This paper assesses the reasons for high ice number concentrations observed in orographic clouds by comparing observations with model simulations over Jungfraujoch, Switzerland. The results suggest that ice nuclei do not significantly contribute to the high concentrations and that a surface source of ice crystals is responsible for the witnessed ice number concentrations.
G. Young, H. M. Jones, E. Darbyshire, K. J. Baustian, J. B. McQuaid, K. N. Bower, P. J. Connolly, M. W. Gallagher, and T. W. Choularton
Atmos. Chem. Phys., 16, 4063–4079, https://doi.org/10.5194/acp-16-4063-2016, https://doi.org/10.5194/acp-16-4063-2016, 2016
Leonid Nichman, Claudia Fuchs, Emma Järvinen, Karoliina Ignatius, Niko Florian Höppel, Antonio Dias, Martin Heinritzi, Mario Simon, Jasmin Tröstl, Andrea Christine Wagner, Robert Wagner, Christina Williamson, Chao Yan, Paul James Connolly, James Robert Dorsey, Jonathan Duplissy, Sebastian Ehrhart, Carla Frege, Hamish Gordon, Christopher Robert Hoyle, Thomas Bjerring Kristensen, Gerhard Steiner, Neil McPherson Donahue, Richard Flagan, Martin William Gallagher, Jasper Kirkby, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Frank Stratmann, and António Tomé
Atmos. Chem. Phys., 16, 3651–3664, https://doi.org/10.5194/acp-16-3651-2016, https://doi.org/10.5194/acp-16-3651-2016, 2016
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Processes in the atmosphere are often governed by the physical and chemical properties of small cloud particles. Ice, water, and mixed clouds, as well as viscous aerosols, were formed under controlled conditions at the CLOUD-CERN facility. The experimental results show a link between cloud particle properties and their unique optical fingerprints. The classification map presented here allows easier discrimination between various particles such as viscous organic aerosol, salt, ice, and liquid.
David Topping, Mark Barley, Michael K. Bane, Nicholas Higham, Bernard Aumont, Nicholas Dingle, and Gordon McFiggans
Geosci. Model Dev., 9, 899–914, https://doi.org/10.5194/gmd-9-899-2016, https://doi.org/10.5194/gmd-9-899-2016, 2016
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In this paper we describe the development and application of a new web-based and open-source facility, UManSysProp (http://umansysprop .seaes.manchester.ac.uk), for automating predictions of molecular and atmospheric aerosol properties. Current facilities include pure component vapour pressures, critical properties, and sub-cooled densities of organic molecules; activity coefficient predictions for mixed inorganic-organic liquid systems; hygroscopic growth factors and CCN activation potential.
I. Crawford, G. Lloyd, E. Herrmann, C. R. Hoyle, K. N. Bower, P. J. Connolly, M. J. Flynn, P. H. Kaye, T. W. Choularton, and M. W. Gallagher
Atmos. Chem. Phys., 16, 2273–2284, https://doi.org/10.5194/acp-16-2273-2016, https://doi.org/10.5194/acp-16-2273-2016, 2016
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In this manuscript we discuss observations of fluorescent aerosol and their interactions with cloud at a high-alpine site in the wintertime under background conditions. We find the majority of the fluorescent aerosol to be consistent in nature to mineral dust and no apparent trend was observed between the fluorescent aerosol fraction and meteorological or cloud microphysical parameters, suggesting that particle fluorescence does not impact cloud evolution or formation at the site.
J. Grazioli, G. Lloyd, L. Panziera, C. R. Hoyle, P. J. Connolly, J. Henneberger, and A. Berne
Atmos. Chem. Phys., 15, 13787–13802, https://doi.org/10.5194/acp-15-13787-2015, https://doi.org/10.5194/acp-15-13787-2015, 2015
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This study investigates the microphysics of winter alpine snowfall occurring in mixed-phase clouds in an inner-Alpine valley during CLACE2014. From polarimetric radar and in situ observations, riming is shown to be an important process leading to more intense snowfall. Riming is usually associated with more intense turbulence providing supercooled liquid water. Distinct features are identified in the vertical structure of polarimetric radar variables.
I. Crawford, S. Ruske, D. O. Topping, and M. W. Gallagher
Atmos. Meas. Tech., 8, 4979–4991, https://doi.org/10.5194/amt-8-4979-2015, https://doi.org/10.5194/amt-8-4979-2015, 2015
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HCA analysis methods were evaluated for the purpose of identifying primary biological aerosol sampled with a WIBS. The ward linkage with z-score normalisation could discriminate between five test particles with 98% accuracy. We applied these methods to a previously studied ambient data set, where both methods produced similar results with some minor differences in cluster partitioning. Finally we compared to previous approaches and found our new method offered improved quantification of PBA.
G. Lloyd, T. W. Choularton, K. N. Bower, M. W. Gallagher, P. J. Connolly, M. Flynn, R. Farrington, J. Crosier, O. Schlenczek, J. Fugal, and J. Henneberger
Atmos. Chem. Phys., 15, 12953–12969, https://doi.org/10.5194/acp-15-12953-2015, https://doi.org/10.5194/acp-15-12953-2015, 2015
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The paper explores the microphysical structure of clouds at the high-alpine measurement site Jungfraujoch, Switzerland. High concentrations of ice crystals were measured by a range of instruments. The presence of these high concentrations could not be explained through conventional understanding of ice formation processes in clouds and the possibility that the surface provides a significant source of ice crystals is investigated.
C. Emersic, P. J. Connolly, S. Boult, M. Campana, and Z. Li
Atmos. Chem. Phys., 15, 11311–11326, https://doi.org/10.5194/acp-15-11311-2015, https://doi.org/10.5194/acp-15-11311-2015, 2015
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I. Steinke, C. Hoose, O. Möhler, P. Connolly, and T. Leisner
Atmos. Chem. Phys., 15, 3703–3717, https://doi.org/10.5194/acp-15-3703-2015, https://doi.org/10.5194/acp-15-3703-2015, 2015
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Ice nucleation in clouds has a significant influence on the global radiative budget and the hydrological cycle. Several studies have investigated the ice formation in droplets and parameterizations have been developed in order to include immersion freezing in climate models. In contrast, there are fewer studies regarding the conversion of water vapor into ice (so-called deposition nucleation) which is the topic of this paper which investigates deposition nucleation by Arizona Test dust in detail
G. Lloyd, T. W. Choularton, K. N. Bower, J. Crosier, H. Jones, J. R. Dorsey, M. W. Gallagher, P. Connolly, A. C. R. Kirchgaessner, and T. Lachlan-Cope
Atmos. Chem. Phys., 15, 3719–3737, https://doi.org/10.5194/acp-15-3719-2015, https://doi.org/10.5194/acp-15-3719-2015, 2015
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Measurements of cloud microphysics are reported from the Aerosol-Cloud Coupling And Climate Interactions (ACCACIA) campaign. Concentrations of ice particles from two spring and two summer cases are compared with particular attention to the role of secondary ice in these clouds. In addition aerosol measurements were used as input to a primary ice nucleation parameterisation which was compared with observed values of primary ice in these clouds. We found higher concentrations of ice during summer.
E. Simpson, P. Connolly, and G. McFiggans
Geosci. Model Dev., 7, 1535–1542, https://doi.org/10.5194/gmd-7-1535-2014, https://doi.org/10.5194/gmd-7-1535-2014, 2014
P. J. Connolly, D. O. Topping, F. Malavelle, and G. McFiggans
Atmos. Chem. Phys., 14, 2289–2302, https://doi.org/10.5194/acp-14-2289-2014, https://doi.org/10.5194/acp-14-2289-2014, 2014
P. J. Connolly, G. Vaughan, P. Cook, G. Allen, H. Coe, T. W. Choularton, C. Dearden, and A. Hill
Atmos. Chem. Phys., 13, 7133–7152, https://doi.org/10.5194/acp-13-7133-2013, https://doi.org/10.5194/acp-13-7133-2013, 2013
J. Skrotzki, P. Connolly, M. Schnaiter, H. Saathoff, O. Möhler, R. Wagner, M. Niemand, V. Ebert, and T. Leisner
Atmos. Chem. Phys., 13, 4451–4466, https://doi.org/10.5194/acp-13-4451-2013, https://doi.org/10.5194/acp-13-4451-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Modeling simulation of aerosol light absorption over the Beijing–Tianjin–Hebei region: the impact of mixing state and aging processes
An investigation of the impact of Canadian wildfires on US air quality using model, satellite, and ground measurements
How to trace the origins of short-lived atmospheric species: an Arctic example
Dust-producing weather patterns of the North American Great Plains
High-resolution air quality maps for Bucharest using a mixed-effects modeling framework
Construction and application of a pollen emissions model based on phenology and random forests
The impact of uncertainty in black carbon's refractive index on simulated optical depth and radiative forcing
Characterization of brown carbon absorption in different European environments through source contribution analysis
Accounting for the black carbon aging process in a two-way coupled meteorology–air quality model
The effectiveness of solar radiation management using fine sea spray across multiple climatic regions
A global dust emission dataset for estimating dust radiative forcings in climate models
Tropospheric aerosols over the western North Atlantic Ocean during the winter and summer deployments of ACTIVATE 2020: life cycle, transport, and distribution
Spatial and temporal evolution of future atmospheric reactive nitrogen deposition in China under different climate change mitigation strategies
Steady-state mixing state of black carbon aerosols from a particle-resolved model
Direct radiative forcing of light-absorbing carbonaceous aerosol and the influencing factors over China
Distinctive dust weather intensities in North China resulted from two types of atmospheric circulation anomalies
Biomass burning emission analysis based on MODIS aerosol optical depth and AeroCom multi-model simulations: implications for model constraints and emission inventories
Quasi-weekly oscillation of regional PM2.5 transport over China driven by the synoptic-scale disturbance of the East Asian winter monsoon circulation
Solar radiation estimation in West Africa: impact of dust conditions during the 2021 dry season
Machine Learning Assisted Inference of the Particle Charge Fraction and the Ion-induced Nucleation Rates during New Particle Formation Events
Modeling urban pollutant transport at multi-resolutions: Impacts of turbulent mixing
Gaps in our understanding of ice-nucleating particle sources exposed by global simulation of the UK Earth System Model
The role of interfacial tension in the size-dependent phase separation of atmospheric aerosol particles
Warming effects of reduced sulfur emissions from shipping
The key role of atmospheric absorption in the Asian summer monsoon response to dust emissions in CMIP6 models
Multi-model effective radiative forcing of the 2020 sulfur cap for shipping
Exploring the Aerosol Activation Properties in a Coastal Area Using Cloud and Particle-resolving Models
Representation of iron aerosol size distributions of anthropogenic emissions is critical in evaluating atmospheric soluble iron input to the ocean
Revealing dominant patterns of aerosol regimes in the lower troposphere and their evolution from preindustrial times to the future in global climate model simulations
A Novel Method to Quantify the Uncertainty Contribution of Aerosol-Radiative Interaction Factors
Improving estimation of a record-breaking east Asian dust storm emission with lagged aerosol Ångström exponent observations
Impact of biomass burning aerosols (BBA) on the tropical African climate in an ocean–atmosphere–aerosol coupled climate model
Retrieval of refractive index and water content for the coating materials of aged black carbon aerosol based on optical properties: a theoretical analysis
Strong inter-model differences and biases in CMIP6 simulations of PM2.5, aerosol optical depth, and precipitation over Africa
Impact of post monsoon crop residue burning on PM2.5 over North India: Optimizing emissions using a high-density in situ surface observation network
Predicting hygroscopic growth of organosulfur aerosol particles using COSMOtherm
Dust aerosol from the Aralkum Desert influences the radiation budget and atmospheric dynamics of Central Asia
Global modeling of aerosol nucleation with a semi-explicit chemical mechanism for highly oxygenated organic molecules (HOMs)
Synergistic effects of the winter North Atlantic Oscillation (NAO) and El Niño–Southern Oscillation (ENSO) on dust activities in North China during the following spring
Aerosol composition, air quality, and boundary layer dynamics in the urban background of Stuttgart in winter
Response of the link between ENSO and the East Asian winter monsoon to Asian anthropogenic aerosols
Measurement report: Source attribution and estimation of black carbon levels in an urban hotspot of the central Po Valley – an integrated approach combining high-resolution dispersion modelling and micro-aethalometers
Modeling CMAQ dry deposition treatment over Western Pacific: A distinct characteristic of mineral dust and anthropogenic aerosol
Microphysical modelling of aerosol scavenging by different types of clouds: description and validation of the approach
Insights into the sources of ultrafine particle numbers at six European urban sites obtained by investigating COVID-19 lockdowns
In-plume and out-of-plume analysis of aerosol–cloud interactions derived from the 2014–2015 Holuhraun volcanic eruption
Impacts of atmospheric circulation patterns and cloud inhibition on aerosol radiative effect and boundary layer structure during winter air pollution in Sichuan Basin, China
Investigating the sign of stratocumulus adjustments to aerosols in the ICON global storm-resolving model
A model study investigating the sensitivity of aerosol forcing to the volatilities of semi-volatile organic compounds
Decomposing the effective radiative forcing of anthropogenic aerosols based on CMIP6 Earth system models
Huiyun Du, Jie Li, Xueshun Chen, Gabriele Curci, Fangqun Yu, Yele Sun, Xu Dao, Song Guo, Zhe Wang, Wenyi Yang, Lianfang Wei, and Zifa Wang
Atmos. Chem. Phys., 25, 5665–5681, https://doi.org/10.5194/acp-25-5665-2025, https://doi.org/10.5194/acp-25-5665-2025, 2025
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Inadequate consideration of mixing states and coatings on black carbon (BC) hinders aerosol radiation forcing quantification. Core–shell mixing aligns well with observations, but partial internal mixing is a more realistic representation. We used a microphysics module to determine the fraction of embedded BC and coating aerosols, constraining the mixing state. This reduced absorption enhancement by 30 %–43 % in northern China, offering insights into BC's radiative effects.
Zhixin Xue, Nair Udaysankar, and Sundar A. Christopher
Atmos. Chem. Phys., 25, 5497–5517, https://doi.org/10.5194/acp-25-5497-2025, https://doi.org/10.5194/acp-25-5497-2025, 2025
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Canadian wildfires in August 2018 significantly increased surface air pollution across the United States (US) – by up to 69 % in some areas. Using model, satellite, and ground measurements, the study highlights how weather patterns and long-range smoke transport drive pollution. The northwestern US was most affected by Canadian wildfire smoke, while the northeastern US experienced the least impact. These findings indicate the growing concern that wildfire smoke poses to air quality across the US.
Anderson Da Silva, Louis Marelle, Jean-Christophe Raut, Yvette Gramlich, Karolina Siegel, Sophie L. Haslett, Claudia Mohr, and Jennie L. Thomas
Atmos. Chem. Phys., 25, 5331–5354, https://doi.org/10.5194/acp-25-5331-2025, https://doi.org/10.5194/acp-25-5331-2025, 2025
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Particle sources in polar climates are unclear, affecting climate representation in models. This study introduces an evaluated method for tracking particles with backward modeling. Tests on simulated particles allowed us to show that traditional detection methods often misidentify sources. An improved method that accurately traces the origins of aerosol particles in the Arctic is presented. The study recommends using this enhanced method for better source identification of atmospheric species.
Stuart Evans
Atmos. Chem. Phys., 25, 4833–4845, https://doi.org/10.5194/acp-25-4833-2025, https://doi.org/10.5194/acp-25-4833-2025, 2025
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This study of the North American Great Plains identifies the various weather patterns responsible for blowing dust in all parts of the region using a weather pattern classification. In the southwestern plains passing cold fronts are the primary cause of dust; in the understudied northern plains, summertime patterns and southerly pre-frontal winds are most important in the west and east, respectively. These results are valuable to understanding and forecasting dust in this complex source region.
Camelia Talianu, Jeni Vasilescu, Doina Nicolae, Alexandru Ilie, Andrei Dandocsi, Anca Nemuc, and Livio Belegante
Atmos. Chem. Phys., 25, 4639–4654, https://doi.org/10.5194/acp-25-4639-2025, https://doi.org/10.5194/acp-25-4639-2025, 2025
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For Bucharest, Romania's capital, mobile measurements during two intensive campaigns and mixed-effect LUR (land-use regression) models to derive seasonal maps of near-surface PM10, NO2 and UFPs (ultrafine particles) have successfully been used. The model's performance was evaluated, demonstrating its potential for high-resolution mapping in other cities with well-characterized urban structures and diverse in situ monitoring stations.
Jiangtao Li, Xingqin An, Zhaobin Sun, Caihua Ye, Qing Hou, Yuxin Zhao, and Zhe Liu
Atmos. Chem. Phys., 25, 3583–3602, https://doi.org/10.5194/acp-25-3583-2025, https://doi.org/10.5194/acp-25-3583-2025, 2025
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Climate change and pollution have intensified pollen allergies. We developed a pollen emissions model using phenology and random forests. Key factors affecting annual pollen emissions include temperature, relative humidity and sunshine hours. Pollen dispersal starts around 10 August, peaks around 30 August and ends by 25 September, lasting about 45 d. Over time, annual pollen emissions exhibit significant fluctuations and a downward trend.
Ruth A. R. Digby, Knut von Salzen, Adam H. Monahan, Nathan P. Gillett, and Jiangnan Li
Atmos. Chem. Phys., 25, 3109–3130, https://doi.org/10.5194/acp-25-3109-2025, https://doi.org/10.5194/acp-25-3109-2025, 2025
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The refractive index of black carbon (BCRI), which determines how much energy black carbon absorbs and scatters, is difficult to measure, and different climate models use different values. We show that varying the BCRI across commonly used values can increase absorbing aerosol optical depth by 42 % and the warming effect from interactions between black carbon and radiation by 47 %, an appreciable fraction of the overall spread between models reported in recent literature assessments.
Hector Navarro-Barboza, Jordi Rovira, Vincenzo Obiso, Andrea Pozzer, Marta Via, Andres Alastuey, Xavier Querol, Noemi Perez, Marjan Savadkoohi, Gang Chen, Jesus Yus-Díez, Matic Ivancic, Martin Rigler, Konstantinos Eleftheriadis, Stergios Vratolis, Olga Zografou, Maria Gini, Benjamin Chazeau, Nicolas Marchand, Andre S. H. Prevot, Kaspar Dallenbach, Mikael Ehn, Krista Luoma, Tuukka Petäjä, Anna Tobler, Jaroslaw Necki, Minna Aurela, Hilkka Timonen, Jarkko Niemi, Olivier Favez, Jean-Eudes Petit, Jean-Philippe Putaud, Christoph Hueglin, Nicolas Pascal, Aurélien Chauvigné, Sébastien Conil, Marco Pandolfi, and Oriol Jorba
Atmos. Chem. Phys., 25, 2667–2694, https://doi.org/10.5194/acp-25-2667-2025, https://doi.org/10.5194/acp-25-2667-2025, 2025
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Brown carbon (BrC) absorbs ultraviolet (UV) and visible light, influencing climate. This study explores BrC's imaginary refractive index (k) using data from 12 European sites. Residential emissions are a major organic aerosol (OA) source in winter, while secondary organic aerosol (SOA) dominates in summer. Source-specific k values were derived, improving model accuracy. The findings highlight BrC's climate impact and emphasize source-specific constraints in atmospheric models.
Yuzhi Jin, Jiandong Wang, Chao Liu, David C. Wong, Golam Sarwar, Kathleen M. Fahey, Shang Wu, Jiaping Wang, Jing Cai, Zeyuan Tian, Zhouyang Zhang, Jia Xing, Aijun Ding, and Shuxiao Wang
Atmos. Chem. Phys., 25, 2613–2630, https://doi.org/10.5194/acp-25-2613-2025, https://doi.org/10.5194/acp-25-2613-2025, 2025
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Black carbon (BC) affects climate and the environment, and its aging process alters its properties. Current models, like WRF-CMAQ, lack full accounting for it. We developed the WRF-CMAQ-BCG model to better represent BC aging by introducing bare and coated BC species and their conversion. The WRF-CMAQ-BCG model introduces the capability to simulate BC mixing states and bare and coated BC wet deposition, and it improves the accuracy of BC mass concentration and aerosol optics.
Zhe Song, Shaocai Yu, Pengfei Li, Ningning Yao, Lang Chen, Yuhai Sun, Boqiong Jiang, and Daniel Rosenfeld
Atmos. Chem. Phys., 25, 2473–2494, https://doi.org/10.5194/acp-25-2473-2025, https://doi.org/10.5194/acp-25-2473-2025, 2025
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Our results with injected sea salt aerosols for five open oceans show that sea salt aerosols with low injection amounts dominate shortwave radiation, mainly through indirect effects. As indirect aerosol effects saturate with increasing injection rates, direct effects exceed indirect effects. This implies that marine cloud brightening is best implemented in areas with extensive cloud cover, while aerosol direct scattering effects remain dominant when clouds are scarce.
Danny M. Leung, Jasper F. Kok, Longlei Li, David M. Lawrence, Natalie M. Mahowald, Simone Tilmes, and Erik Kluzek
Atmos. Chem. Phys., 25, 2311–2331, https://doi.org/10.5194/acp-25-2311-2025, https://doi.org/10.5194/acp-25-2311-2025, 2025
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This study derives a gridded dust emission dataset for 1841–2000 by employing a combination of observed dust from core records and reanalyzed global dust cycle constraints. We evaluate the ability of global models to replicate the observed historical dust variability by using the emission dataset to force a historical simulation in an Earth system model. We show that prescribing our emissions forces the model to better match observations than other mechanistic models.
Hongyu Liu, Bo Zhang, Richard H. Moore, Luke D. Ziemba, Richard A. Ferrare, Hyundeok Choi, Armin Sorooshian, David Painemal, Hailong Wang, Michael A. Shook, Amy Jo Scarino, Johnathan W. Hair, Ewan C. Crosbie, Marta A. Fenn, Taylor J. Shingler, Chris A. Hostetler, Gao Chen, Mary M. Kleb, Gan Luo, Fangqun Yu, Mark A. Vaughan, Yongxiang Hu, Glenn S. Diskin, John B. Nowak, Joshua P. DiGangi, Yonghoon Choi, Christoph A. Keller, and Matthew S. Johnson
Atmos. Chem. Phys., 25, 2087–2121, https://doi.org/10.5194/acp-25-2087-2025, https://doi.org/10.5194/acp-25-2087-2025, 2025
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We use the GEOS-Chem model to simulate aerosol distributions and properties over the western North Atlantic Ocean (WNAO) during the winter and summer deployments in 2020 of the NASA ACTIVATE mission. Model results are evaluated against aircraft, ground-based, and satellite observations. The improved understanding of life cycle, composition, transport pathways, and distribution of aerosols has important implications for characterizing aerosol–cloud–meteorology interactions over WNAO.
Mingrui Ma, Jiachen Cao, Dan Tong, Bo Zheng, and Yu Zhao
Atmos. Chem. Phys., 25, 2147–2166, https://doi.org/10.5194/acp-25-2147-2025, https://doi.org/10.5194/acp-25-2147-2025, 2025
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We combined two global climate change pathways and three national emission control scenarios to analyze the future evolution of reactive nitrogen (Nr) deposition till the 2060s in China with air quality modeling. We show China’s clean air and carbon neutrality policies would overcome the adverse effects of climate change and efficiently reduce Nr deposition. The outflow of Nr fluxes from mainland China to the west Pacific would also be clearly reduced from continuous stringent emission controls.
Zhouyang Zhang, Jiandong Wang, Jiaping Wang, Nicole Riemer, Chao Liu, Yuzhi Jin, Zeyuan Tian, Jing Cai, Yueyue Cheng, Ganzhen Chen, Bin Wang, Shuxiao Wang, and Aijun Ding
Atmos. Chem. Phys., 25, 1869–1881, https://doi.org/10.5194/acp-25-1869-2025, https://doi.org/10.5194/acp-25-1869-2025, 2025
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Black carbon (BC) exerts notable warming effects. We use a particle-resolved model to investigate the long-term behavior of the BC mixing state, revealing its compositions, coating thickness distribution, and optical properties all stabilize with a characteristic time of less than 1 d. This study can effectively simplify the description of the BC mixing state, which facilitates the precise assessment of the optical properties of BC aerosols in global and chemical transport models.
Shuangqin Yang, Yusi Liu, Li Chen, Nan Cao, Jing Wang, and Shuang Gao
EGUsphere, https://doi.org/10.5194/egusphere-2024-3705, https://doi.org/10.5194/egusphere-2024-3705, 2025
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Black carbon, primary brown carbon, and secondary brown carbon are the leading light-absorbing carbonaceous aerosols (LACs) that contribute significantly to climate change. We modified the GEOS-Chem model to simulate the climate change by LACs based on local emission inventory, and explored the impacts of LACs properties and atmospheric variables on the corresponding DRFs in seven regions of China. The study confirms the warming effect of LACs and deepens our knowledge of their climatic effects.
Qianyi Huo, Zhicong Yin, Xiaoqing Ma, and Huijun Wang
Atmos. Chem. Phys., 25, 1711–1724, https://doi.org/10.5194/acp-25-1711-2025, https://doi.org/10.5194/acp-25-1711-2025, 2025
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Dust days during the spring seasons of 2015–2023 in North China were classified into Mongolian cyclone and cold high types depending on the presence of the Mongolian cyclone. The Mongolian cyclone type led to more frequent and severe dust weather, indicated by PM10 concentrations. To comprehensively forecast the two types of dust weather, a common predictor was established based on 500 hPa anomalous circulation systems, offering insights for dust weather forecasting and climate prediction.
Mariya Petrenko, Ralph Kahn, Mian Chin, Susanne E. Bauer, Tommi Bergman, Huisheng Bian, Gabriele Curci, Ben Johnson, Johannes W. Kaiser, Zak Kipling, Harri Kokkola, Xiaohong Liu, Keren Mezuman, Tero Mielonen, Gunnar Myhre, Xiaohua Pan, Anna Protonotariou, Samuel Remy, Ragnhild Bieltvedt Skeie, Philip Stier, Toshihiko Takemura, Kostas Tsigaridis, Hailong Wang, Duncan Watson-Parris, and Kai Zhang
Atmos. Chem. Phys., 25, 1545–1567, https://doi.org/10.5194/acp-25-1545-2025, https://doi.org/10.5194/acp-25-1545-2025, 2025
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We compared smoke plume simulations from 11 global models to each other and to satellite smoke amount observations aimed at constraining smoke source strength. In regions where plumes are thick and background aerosol is low, models and satellites compare well. However, the input emission inventory tends to underestimate in many places, and particle property and loss rate assumptions vary enormously among models, causing uncertainties that require systematic in situ measurements to resolve.
Yongqing Bai, Tianliang Zhao, Kai Meng, Yue Zhou, Jie Xiong, Xiaoyun Sun, Lijuan Shen, Yanyu Yue, Yan Zhu, Weiyang Hu, and Jingyan Yao
Atmos. Chem. Phys., 25, 1273–1287, https://doi.org/10.5194/acp-25-1273-2025, https://doi.org/10.5194/acp-25-1273-2025, 2025
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We proposed a composite statistical method to identify the quasi-weekly oscillation (QWO) of regional PM2.5 transport over China in winter from 2015 to 2019. The QWO of regional PM2.5 transport is constrained by synoptic-scale disturbances of the East Asian winter monsoon circulation with the periodic activities of the Siberian high, providing a new insight into the understanding of regional pollutant transport with meteorological drivers in atmospheric environment changes.
Léo Clauzel, Sandrine Anquetin, Christophe Lavaysse, Gilles Bergametti, Christel Bouet, Guillaume Siour, Rémy Lapere, Béatrice Marticorena, and Jennie Thomas
Atmos. Chem. Phys., 25, 997–1021, https://doi.org/10.5194/acp-25-997-2025, https://doi.org/10.5194/acp-25-997-2025, 2025
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Solar energy production in West Africa is set to rise and needs accurate solar radiation estimates which are affected by desert dust. This work analyses a March 2021 dust event using a modelling strategy incorporating desert dust. Results show that considering desert dust cuts errors in solar radiation estimates by 75 % and reduces surface solar radiation by 18 %. This highlights the importance of incorporating dust aerosols into solar forecasting for better accuracy.
Pan Wang, Yue Zhao, Jiandong Wang, Veli-Matti Kerminen, Jingkun Jiang, and Chenxi Li
EGUsphere, https://doi.org/10.5194/egusphere-2024-3666, https://doi.org/10.5194/egusphere-2024-3666, 2025
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We developed a numerical model to explore how the charge state of newly formed atmospheric particles evolves during growth and how this relates to ion-induced nucleation rates. We identify the governing factors of particle charging and further apply neural networks to predict particle charge states and estimate ion induced nucleation rates. This study offers insights into particle charging dynamics and introduces new methods for assessing ion induced nucleation in atmospheric research.
Zining Yang, Qiuyan Du, Qike Yang, Chun Zhao, Gudongze Li, Zihan Xia, Mingyue Xu, Renmin Yuan, Yubin Li, Kaihui Xia, Jun Gu, and Jiawang Feng
EGUsphere, https://doi.org/10.5194/egusphere-2024-3890, https://doi.org/10.5194/egusphere-2024-3890, 2025
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This study investigates the impact of turbulent mixing on black carbon (BC) concentrations in urban areas using WRF-Chem at 25, 5, and 1 km resolutions. Significant variations in BC and turbulent mixing occur mainly at night. Higher resolutions reduce BC overestimation due to enhanced PBL mixing coefficients and vertical wind fluxes. Small-scale eddies at higher resolutions increase BC lifetime and column concentrations. Land use and terrain variations across multi-resolutions affect PBL mixing.
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.
Ryan Schmedding and Andreas Zuend
Atmos. Chem. Phys., 25, 327–346, https://doi.org/10.5194/acp-25-327-2025, https://doi.org/10.5194/acp-25-327-2025, 2025
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Four different approaches for computing the interfacial tension between liquid phases in aerosol particles were tested for particles with diameters from 10 nm to more than 5 μm. Antonov's rule led to the strongest reductions in the onset relative humidity of liquid–liquid phase separation and reproduced measured interfacial tensions for highly immiscible systems. A modified form of the Butler equation was able to best reproduce measured interfacial tensions in more miscible systems.
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.
Alcide Zhao, Laura J. Wilcox, and Claire L. Ryder
Atmos. Chem. Phys., 24, 13385–13402, https://doi.org/10.5194/acp-24-13385-2024, https://doi.org/10.5194/acp-24-13385-2024, 2024
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Climate models include desert dust aerosols, which cause atmospheric heating and can change circulation patterns. We assess the effect of dust on the Indian and east Asian summer monsoons through multi-model experiments isolating the effect of dust in current climate models for the first time. Dust atmospheric heating results in a southward shift of western Pacific equatorial rainfall and an enhanced Indian summer monsoon. This shows the importance of accurate dust representation in models.
Ragnhild Bieltvedt Skeie, Rachael Byrom, Øivind Hodnebrog, Caroline Jouan, and Gunnar Myhre
Atmos. Chem. Phys., 24, 13361–13370, https://doi.org/10.5194/acp-24-13361-2024, https://doi.org/10.5194/acp-24-13361-2024, 2024
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In 2020, new regulations by the International Maritime Organization regarding sulfur emissions came into force, reducing emissions of SO2 from the shipping sector by approximately 80 %. In this study, we use multiple models to calculate how much the Earth energy balance changed due to the emission reduction or the so-called effective radiative forcing. The calculated effective radiative forcing is weak, comparable to the effect of the increase in CO2 over the last 2 to 3 years.
Ge Yu, Yueya Wang, Zhe Wang, and Xiaoming Shi
EGUsphere, https://doi.org/10.5194/egusphere-2024-3581, https://doi.org/10.5194/egusphere-2024-3581, 2024
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Studying the cloud-forming capacity of aerosols is crucial in climate research. The PartMC model can provide detailed particle information and help these studies. This model is integrated with the ideal meteorological Cloud Model 1 (CM1) to simulate the aerosols at cloud-forming locations. Significant changes are revealed in the hygroscopicity distribution of aerosols within ascending air parcels. Additionally, different ascent times also affect aerosol aging processes.
Mingxu Liu, Hitoshi Matsui, Douglas S. Hamilton, Sagar D. Rathod, Kara D. Lamb, and Natalie M. Mahowald
Atmos. Chem. Phys., 24, 13115–13127, https://doi.org/10.5194/acp-24-13115-2024, https://doi.org/10.5194/acp-24-13115-2024, 2024
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Atmospheric aerosol deposition provides bioavailable iron to promote marine primary production, yet the estimates of its fluxes remain highly uncertain. This study, by performing global aerosol simulations, demonstrates that iron-containing particle size upon emission is a critical factor in regulating soluble iron input to open oceans. Further observational constraints on this are needed to reduce modeling uncertainties.
Jingmin Li, Mattia Righi, Johannes Hendricks, Christof G. Beer, Ulrike Burkhardt, and Anja Schmidt
Atmos. Chem. Phys., 24, 12727–12747, https://doi.org/10.5194/acp-24-12727-2024, https://doi.org/10.5194/acp-24-12727-2024, 2024
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Aiming to understand underlying patterns and trends in aerosols, we characterize the spatial patterns and long-term evolution of lower tropospheric aerosols by clustering multiple aerosol properties from preindustrial times to the year 2050 under three Shared
Socioeconomic Pathway scenarios. The results provide a clear and condensed picture of the spatial extent and distribution of aerosols for different time periods and emission scenarios.
Socioeconomic Pathway scenarios. The results provide a clear and condensed picture of the spatial extent and distribution of aerosols for different time periods and emission scenarios.
Bishuo He and Chunsheng Zhao
EGUsphere, https://doi.org/10.5194/egusphere-2024-3441, https://doi.org/10.5194/egusphere-2024-3441, 2024
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Factor-uncertainty analysis helps us understand their impacts on complex systems. Traditional methods have many limitations. This study introduces a new method to measure how each factor contributes to uncertainty. It gains insights into the role of each variable and works for all multi-factor systems. As an application, we analyzed how aerosols affect solar radiation and identified the key factors. These analyses can improve our understanding of the role of aerosols in climate change.
Yueming Cheng, Tie Dai, Junji Cao, Daisuke Goto, Jianbing Jin, Teruyuki Nakajima, and Guangyu Shi
Atmos. Chem. Phys., 24, 12643–12659, https://doi.org/10.5194/acp-24-12643-2024, https://doi.org/10.5194/acp-24-12643-2024, 2024
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In March 2021, east Asia experienced an outbreak of severe dust storms after an absence of 1.5 decades. Here, we innovatively used the time-lagged ground-based aerosol size information with the fixed-lag ensemble Kalman smoother to optimize dust emission and reproduce the dust storm. This work is valuable for not only the quantification of health damage, aviation risks, and profound impacts on the Earth's system but also revealing the climatic driving force and the process of desertification.
Marc Mallet, Aurore Voldoire, Fabien Solmon, Pierre Nabat, Thomas Drugé, and Romain Roehrig
Atmos. Chem. Phys., 24, 12509–12535, https://doi.org/10.5194/acp-24-12509-2024, https://doi.org/10.5194/acp-24-12509-2024, 2024
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This study investigates the interactions between smoke aerosols and climate in tropical Africa using a coupled ocean–atmosphere–aerosol climate model. The work shows that smoke plumes have a significant impact by increasing the low-cloud fraction, decreasing the ocean and continental surface temperature and reducing the precipitation of coastal western Africa. It also highlights the role of the ocean temperature response and its feedbacks for the September–November season.
Jia Liu, Cancan Zhu, Donghui Zhou, and Jinbao Han
Atmos. Chem. Phys., 24, 12341–12354, https://doi.org/10.5194/acp-24-12341-2024, https://doi.org/10.5194/acp-24-12341-2024, 2024
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The hydrophilic coatings of aged black carbon (BC) particles absorb moisture during the hygroscopic growth process, but it is difficult to characterize how much water is absorbed under different relative humidities (RHs). In this study, we propose a method to obtain the water content in the coatings based on the equivalent complex refractive index retrieved from optical properties. This method is verified from a theoretical perspective, and it performs well for thickly coated BC at high RHs.
Catherine Anne Toolan, Joe Adabouk Amooli, Laura J. Wilcox, Bjørn H. Samset, Andrew G. Turner, and Daniel M. Westervelt
EGUsphere, https://doi.org/10.5194/egusphere-2024-3057, https://doi.org/10.5194/egusphere-2024-3057, 2024
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Our research explores how well air pollution and rainfall patterns in Africa are represented in current climate models, by comparing model data to observations from 1981 to 2023. While most models capture seasonal air quality changes well, they struggle to replicate the distribution of non-dust pollutants and certain rainfall patterns, especially over east Africa. Improving these models is crucial for better climate predictions and preparing for future risks.
Mizuo Kajino, Kentaro Ishijima, Joseph Ching, Kazuyo Yamaji, Rio Ishikawa, Tomoki Kajikawa, Tanbir Singh, Tomoki Nakayama, Yutaka Matsumi, Koyo Kojima, Prabir K. Patra, and Sachiko Hayashida
EGUsphere, https://doi.org/10.5194/egusphere-2024-1811, https://doi.org/10.5194/egusphere-2024-1811, 2024
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Air pollution in Delhi during post monsoon period is severe and association with intensive crop residue burning (CRB) over Punjab state has attracted attention. However, the relationship has been unclear as the CRB emissions conventionally derived from satellites were underestimated due to clouds and haze over the region. We evaluated the impact of CRB on PM2.5 as about 50 %, based on a combination of numerical modeling and high-density observation network using low-cost sensors we installed.
Zijun Li, Angela Buchholz, and Noora Hyttinen
Atmos. Chem. Phys., 24, 11717–11725, https://doi.org/10.5194/acp-24-11717-2024, https://doi.org/10.5194/acp-24-11717-2024, 2024
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Evaluating organosulfur (OS) hygroscopicity is important for assessing aerosol–cloud climate interactions in the post-fossil-fuel future, when SO2 emissions decrease and OS compounds become increasingly important. Here a state-of-the-art quantum-chemistry-based method was used to predict the hygroscopic growth factors (HGFs) of a group of atmospherically relevant OS compounds and their mixtures with (NH4)2SO4. A good agreement was observed between their model-estimated and experimental HGFs.
Jamie R. Banks, Bernd Heinold, and Kerstin Schepanski
Atmos. Chem. Phys., 24, 11451–11475, https://doi.org/10.5194/acp-24-11451-2024, https://doi.org/10.5194/acp-24-11451-2024, 2024
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The Aralkum is a new desert in Central Asia formed by the desiccation of the Aral Sea. This has created a source of atmospheric dust, with implications for the balance of solar and thermal radiation. Simulating these effects using a dust transport model, we find that Aralkum dust adds radiative cooling effects to the surface and atmosphere on average but also adds heating events. Increases in surface pressure due to Aralkum dust strengthen the Siberian High and weaken the summer Asian heat low.
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.
Falei Xu, Shuang Wang, Yan Li, and Juan Feng
Atmos. Chem. Phys., 24, 10689–10705, https://doi.org/10.5194/acp-24-10689-2024, https://doi.org/10.5194/acp-24-10689-2024, 2024
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This study examines how the winter North Atlantic Oscillation (NAO) and El Niño–Southern Oscillation (ENSO) affect dust activities in North China during the following spring. The results show that the NAO and ENSO, particularly in their negative phases, greatly influence dust activities. When both are negative, their combined effect on dust activities is even greater. This research highlights the importance of these climate patterns in predicting spring dust activities in North China.
Hengheng Zhang, Wei Huang, Xiaoli Shen, Ramakrishna Ramisetty, Junwei Song, Olga Kiseleva, Christopher Claus Holst, Basit Khan, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 10617–10637, https://doi.org/10.5194/acp-24-10617-2024, https://doi.org/10.5194/acp-24-10617-2024, 2024
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Our study unravels how stagnant winter conditions elevate aerosol levels in Stuttgart. Cloud cover at night plays a pivotal role, impacting morning air quality. Validating a key model, our findings aid accurate air quality predictions, crucial for effective pollution mitigation in urban areas.
Zixuan Jia, Massimo A. Bollasina, Wenjun Zhang, and Ying Xiang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2770, https://doi.org/10.5194/egusphere-2024-2770, 2024
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Using multi-model mean data from regional aerosol perturbation experiments, we find that increased Asian sulfate aerosols strengthen the link between ENSO and the East Asian winter monsoon. In coupled simulations, aerosol-induced broad cooling increases ENSO amplitude by affecting the tropical Pacific mean state, contributing to increase monsoon interannual variability. These results provide important implications to reduce uncertainties in future projections of regional extreme variability.
Giorgio Veratti, Alessandro Bigi, Michele Stortini, Sergio Teggi, and Grazia Ghermandi
Atmos. Chem. Phys., 24, 10475–10512, https://doi.org/10.5194/acp-24-10475-2024, https://doi.org/10.5194/acp-24-10475-2024, 2024
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In a study of two consecutive winter seasons, we used measurements and modelling tools to identify the levels and sources of black carbon pollution in a medium-sized urban area of the Po Valley, Italy. Our findings show that biomass burning and traffic-related emissions (especially from Euro 4 diesel cars) significantly contribute to BC concentrations. This research offers crucial insights for policymakers and urban planners aiming to improve air quality in cities.
Steven Soon-Kai Kong, Joshua S. Fu, Neng-Huei Lin, Guey-Rong Sheu, and Wei-Syun Huang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2549, https://doi.org/10.5194/egusphere-2024-2549, 2024
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The accuracy of the chemical transport model, a key focus of our research, is strongly dependent on the dry deposition parameterization. Our finding shows that the refined CMAQ dust model correlated well with the ground and high altitude in-situ measurements by implementing the suggested dry deposition schemes. Furthermore, we reveal the mixing state of two types of aerosols at the upper level, a finding supported by both the optimized model and measurement.
Pascal Lemaitre, Arnaud Quérel, Alexis Dépée, Alice Guerra Devigne, Marie Monier, Thibault Hiron, Chloé Soto Minguez, Daniel Hardy, and Andrea Flossmann
Atmos. Chem. Phys., 24, 9713–9732, https://doi.org/10.5194/acp-24-9713-2024, https://doi.org/10.5194/acp-24-9713-2024, 2024
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A new in-cloud scavenging scheme is proposed. It is based on a microphysical model of cloud formation and may be applied to long-distance atmospheric transport models (> 100 km) and climatic models. This model is applied to the two most extreme precipitating cloud types in terms of both relative humidity and vertical extension: cumulonimbus and stratus.
Alex Rowell, James Brean, David C. S. Beddows, Tuukka Petäjä, Máté Vörösmarty, Imre Salma, Jarkko V. Niemi, Hanna E. Manninen, Dominik van Pinxteren, Thomas Tuch, Kay Weinhold, Zongbo Shi, and Roy M. Harrison
Atmos. Chem. Phys., 24, 9515–9531, https://doi.org/10.5194/acp-24-9515-2024, https://doi.org/10.5194/acp-24-9515-2024, 2024
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Different sources of airborne particles in the atmospheres of four European cities were distinguished by recognising their particle size distributions using a statistical procedure, positive matrix factorisation. The various sources responded differently to the changes in emissions associated with COVID-19 lockdowns, and the reasons are investigated. While traffic emissions generally decreased, particles formed from reactions of atmospheric gases decreased in some cities but increased in others.
Amy H. Peace, Ying Chen, George Jordan, Daniel G. Partridge, Florent Malavelle, Eliza Duncan, and Jim M. Haywood
Atmos. Chem. Phys., 24, 9533–9553, https://doi.org/10.5194/acp-24-9533-2024, https://doi.org/10.5194/acp-24-9533-2024, 2024
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Natural aerosols from volcanic eruptions can help us understand how anthropogenic aerosols modify climate. We use observations and model simulations of the 2014–2015 Holuhraun eruption plume to examine aerosol–cloud interactions in September 2014. We find a shift to clouds with smaller, more numerous cloud droplets in the first 2 weeks of the eruption. In the third week, the background meteorology and previous conditions experienced by air masses modulate the aerosol perturbation to clouds.
Hua Lu, Min Xie, Bingliang Zhuang, Danyang Ma, Bojun Liu, Yangzhihao Zhan, Tijian Wang, Shu Li, Mengmeng Li, and Kuanguang Zhu
Atmos. Chem. Phys., 24, 8963–8982, https://doi.org/10.5194/acp-24-8963-2024, https://doi.org/10.5194/acp-24-8963-2024, 2024
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To identify cloud, aerosol, and planetary boundary layer (PBL) interactions from an air quality perspective, we summarized two pollution patterns characterized by denser liquid cloud and by obvious cloud radiation interaction (CRI). Numerical simulation experiments showed CRI could cause a 50 % reduction in aerosol radiation interaction (ARI) under a low-trough system. The results emphasized the nonnegligible role of CRI and its inhibition of ARI under wet and cloudy pollution synoptic patterns.
Emilie Fons, Ann Kristin Naumann, David Neubauer, Theresa Lang, and Ulrike Lohmann
Atmos. Chem. Phys., 24, 8653–8675, https://doi.org/10.5194/acp-24-8653-2024, https://doi.org/10.5194/acp-24-8653-2024, 2024
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Aerosols can modify the liquid water path (LWP) of stratocumulus and, thus, their radiative effect. We compare storm-resolving model and satellite data that disagree on the sign of LWP adjustments and diagnose this discrepancy with causal inference. We find that strong precipitation, the absence of wet scavenging, and cloud deepening under a weak inversion contribute to positive LWP adjustments to aerosols in the model, despite weak negative effects from cloud-top entrainment enhancement.
Muhammed Irfan, Thomas Kühn, Taina Yli-Juuti, Anton Laakso, Eemeli Holopainen, Douglas R. Worsnop, Annele Virtanen, and Harri Kokkola
Atmos. Chem. Phys., 24, 8489–8506, https://doi.org/10.5194/acp-24-8489-2024, https://doi.org/10.5194/acp-24-8489-2024, 2024
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The study examines how the volatility of semi-volatile organic compounds affects secondary organic aerosol (SOA) formation and climate. Our simulations show that uncertainties in these volatilities influence aerosol mass and climate impacts. Accurate representation of these compounds in climate models is crucial for predicting global climate patterns.
Alkiviadis Kalisoras, Aristeidis K. Georgoulias, Dimitris Akritidis, Robert J. Allen, Vaishali Naik, Chaincy Kuo, Sophie Szopa, Pierre Nabat, Dirk Olivié, Twan van Noije, Philippe Le Sager, David Neubauer, Naga Oshima, Jane Mulcahy, Larry W. Horowitz, and Prodromos Zanis
Atmos. Chem. Phys., 24, 7837–7872, https://doi.org/10.5194/acp-24-7837-2024, https://doi.org/10.5194/acp-24-7837-2024, 2024
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Effective radiative forcing (ERF) is a metric for estimating how human activities and natural agents change the energy flow into and out of the Earth’s climate system. We investigate the anthropogenic aerosol ERF, and we estimate the contribution of individual processes to the total ERF using simulations from Earth system models within the Coupled Model Intercomparison Project Phase 6 (CMIP6). Our findings highlight that aerosol–cloud interactions drive ERF variability during the last 150 years.
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Short summary
This is the first time the Maxwell–Stefan framework has been applied to an atmospheric aerosol core–shell model and shows that there is a complex interplay between the viscous and solubility effects on aerosol composition. Understanding aerosol composition is essential to accurately model their interactions within atmospheric systems. We use simple binary systems to demonstrate how viscosity and solubility both play a role in affecting the rate of diffusion through aerosol particles.
This is the first time the Maxwell–Stefan framework has been applied to an atmospheric aerosol...
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