Articles | Volume 14, issue 5
https://doi.org/10.5194/acp-14-2289-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-14-2289-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
04 Mar 2014
Research article |
| 04 Mar 2014
A parameterisation for the activation of cloud drops including the effects of semi-volatile organics
P. J. Connolly
School of Earth, Atmospheric and Environmental Sciences, The University of Manchester, Manchester, UK
D. O. Topping
School of Earth, Atmospheric and Environmental Sciences, The University of Manchester, Manchester, UK
F. Malavelle
College of Engineering, Mathematics and Physical Sciences, University of Exeter, Exeter, UK
G. McFiggans
School of Earth, Atmospheric and Environmental Sciences, The University of Manchester, Manchester, 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.
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
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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.
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.
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.
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.
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, 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
Yunqi Shao, Aristeidis Voliotis, Mao Du, Yu Wang, Jacqueline Hamilton, M. Rami Alfarra, and Gordon McFiggans
Aerosol Research Discuss., https://doi.org/10.5194/ar-2025-22, https://doi.org/10.5194/ar-2025-22, 2025
Preprint under review for AR
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This study analysed the average carbon oxidation state (OSc) during secondary organic aerosol formation from mixed volatile organic compounds (VOCs) using three mass spectrometry techniques. Notable discrepancies in OSc were observed across the techniques, with FIGAERO-CIMS keep reporting higher values. The results also shown that OSc in mixed VOC systems is influenced not only by products from individual precursors but also by unique compounds formed through interactions between VOC products.
Lukas Pichelstorfer, Simon P. O'Meara, and Gordon McFiggans
Aerosol Research, 3, 417–428, https://doi.org/10.5194/ar-3-417-2025, https://doi.org/10.5194/ar-3-417-2025, 2025
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Quantification of autoxidation chemistry is a complex task essential to our understanding of atmospheric secondary aerosol formation and its impact on climate. In this work, we introduce the autoCONSTRAINT module, a semi-empirical method for deducing reaction rate coefficients for lumped autoxidation chemistry schemes based on experimental data. The theoretical approach is analytical and provides mathematically correct though non-unique solutions with low computational cost.
Olivia M. Jackson, Aristeidis Voliotis, Thomas J. Bannan, Simon P. O'Meara, Gordon McFiggans, Dave Johnson, and Hugh Coe
Atmos. Chem. Phys., 25, 6257–6272, https://doi.org/10.5194/acp-25-6257-2025, https://doi.org/10.5194/acp-25-6257-2025, 2025
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This paper details a novel method of measuring the volatility of pesticides using the Filter Inlet for Gases and AEROsols coupled with a chemical ionisation mass spectrometer (FIGAERO-CIMS) calibrated using a set of poly(ethylene) glycols. This is compared to literature values and common models. The results show that the method used primarily matches current literature values. Additionally, a pesticide’s volatility as an indicator of the likelihood of atmospheric transport occurring is explored.
Huihui Wu, Nicholas Marsden, Paul Connolly, Michael Flynn, Paul I. Williams, Declan Finney, Kezhen Hu, Graeme J. Nott, Navaneeth Thamban, Keith Bower, Alan Blyth, Martin Gallagher, and Hugh Coe
EGUsphere, https://doi.org/10.5194/egusphere-2025-2600, https://doi.org/10.5194/egusphere-2025-2600, 2025
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Airborne observations over the Magdalena Mountains in New Mexico underscore the combined influence of meteorological conditions and aerosol characteristics on the development of deep-convective clouds under different flow regimes. Model-observation comparisons emphasize the critical role of aerosol entrainment in reproducing the observed broad cloud droplet spectra. This study provides valuable constraints for improving parameterizations of aerosol-cloud interactions in deep convective systems.
Rhianna L. Evans, Daniel J. Bryant, Aristeidis Voliotis, Dawei Hu, Huihui Wu, Sara Aisyah Syafira, Osayomwanbor E. Oghama, Gordon McFiggans, Jacqueline F. Hamilton, and Andrew R. Rickard
Atmos. Chem. Phys., 25, 4367–4389, https://doi.org/10.5194/acp-25-4367-2025, https://doi.org/10.5194/acp-25-4367-2025, 2025
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The chemical composition of organic aerosol derived from wood-burning emissions under different burning conditions was characterised. Fresh emissions from flaming and smouldering were largely aromatic in nature, whereas upon aging the aromatic content decreased. This decrease was greater for smouldering due to the loss of toxic polyaromatic species, whereas under flaming conditions highly toxic polyaromatic species were produced. These differences present an important challenge for future policy.
Declan L. Finney, Alan M. Blyth, Paul R. Field, Martin I. Daily, Benjamin J. Murray, Mengyu Sun, Paul J. Connolly, Zhiqiang Cui, and Steven Böing
EGUsphere, https://doi.org/10.5194/egusphere-2025-1227, https://doi.org/10.5194/egusphere-2025-1227, 2025
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We present observation-informed modelling from the Deep Convective Microphysics Experiment to study how environmental conditions and cloud processes affect anvil cloud albedo and radiation. Aerosols influencing cloud droplets or influencing ice formation yield varying radiative effects. We introduce fingerprint metrics to discern these effects. Using detailed observations and modelling, we offer insights into high cloud radiative effects and feedbacks.
George Jordan, Florent Malavelle, Jim Haywood, Ying Chen, Ben Johnson, Daniel Partridge, Amy Peace, Eliza Duncan, Duncan Watson-Parris, David Neubauer, Anton Laakso, Martine Michou, and Pierre Nabat
EGUsphere, https://doi.org/10.5194/egusphere-2025-835, https://doi.org/10.5194/egusphere-2025-835, 2025
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The 2014–15 Holuhraun eruption created a vast aerosol plume that acted as a natural experiment to assess how well climate models capture changes in cloud properties due to increased aerosol. We find that the models accurately represent the observed shift to smaller, more numerous cloud droplets. However, the models diverge in their aerosol induced changes to large-scale cloud properties, particularly cloud liquid water content. Our study shows that Holuhraun had a cooling effect on the Earth.
Omer Celebi, Andrew R. D. Smedley, Paul J. Connolly, and Ann R. Webb
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-200, https://doi.org/10.5194/amt-2024-200, 2025
Revised manuscript under review for AMT
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Ice crystals have a significant role in weather and climate, but their roughness is not measured which affects how ice crystals scatter sunlight. In our study, we have developed a new way of measuring roughness parameters of ice crystals. By growing crystals in laboratory conditions and creating replicas , we can image them under special imaging tools to measure small features on their surface. Results can be implemented in models to reduce uncertainties in understanding the atmosphere.
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.
Declan L. Finney, Alan M. Blyth, Martin Gallagher, Huihui Wu, Graeme J. Nott, Michael I. Biggerstaff, Richard G. Sonnenfeld, Martin Daily, Dan Walker, David Dufton, Keith Bower, Steven Böing, Thomas Choularton, Jonathan Crosier, James Groves, Paul R. Field, Hugh Coe, Benjamin J. Murray, Gary Lloyd, Nicholas A. Marsden, Michael Flynn, Kezhen Hu, Navaneeth M. Thamban, Paul I. Williams, Paul J. Connolly, James B. McQuaid, Joseph Robinson, Zhiqiang Cui, Ralph R. Burton, Gordon Carrie, Robert Moore, Steven J. Abel, Dave Tiddeman, and Graydon Aulich
Earth Syst. Sci. Data, 16, 2141–2163, https://doi.org/10.5194/essd-16-2141-2024, https://doi.org/10.5194/essd-16-2141-2024, 2024
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The DCMEX (Deep Convective Microphysics Experiment) project undertook an aircraft- and ground-based measurement campaign of New Mexico deep convective clouds during July–August 2022. The campaign coordinated a broad range of instrumentation measuring aerosol, cloud physics, radar signals, thermodynamics, dynamics, electric fields, and weather. The project's objectives included the utilisation of these data with satellite observations to study the anvil cloud radiative effect.
Yarê Baker, Sungah Kang, Hui Wang, Rongrong Wu, Jian Xu, Annika Zanders, Quanfu He, Thorsten Hohaus, Till Ziehm, Veronica Geretti, Thomas J. Bannan, Simon P. O'Meara, Aristeidis Voliotis, Mattias Hallquist, Gordon McFiggans, Sören R. Zorn, Andreas Wahner, and Thomas F. Mentel
Atmos. Chem. Phys., 24, 4789–4807, https://doi.org/10.5194/acp-24-4789-2024, https://doi.org/10.5194/acp-24-4789-2024, 2024
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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.
George Jordan, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, Anton Laakso, and James Haywood
Atmos. Chem. Phys., 24, 1939–1960, https://doi.org/10.5194/acp-24-1939-2024, https://doi.org/10.5194/acp-24-1939-2024, 2024
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The 2014–15 Holuhraun eruption caused a huge aerosol plume in an otherwise unpolluted region, providing a chance to study how aerosol alters cloud properties. This two-part study uses observations and models to quantify this relationship’s impact on the Earth’s energy budget. Part 1 suggests the models capture the observed spatial and chemical evolution of the plume, yet no model plume is exact. Understanding these differences is key for Part 2, where changes to cloud properties are explored.
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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Secondary ice production (SIP) may significantly enhance the ice particle concentration in mixed-phase clouds. We present a systematic modelling study of secondary ice formation in idealised shallow convective clouds for various conditions. Our results suggest that the SIP mechanism of collisions of supercooled water drops with more massive ice particles may be a significant ice formation mechanism in shallow convective clouds outside the rime-splintering temperature range (−3 to −8 °C).
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.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, M. Rami Alfarra, Thomas J. Bannan, Dawei Hu, Kelly L. Pereira, Jaqueline F. Hamilton, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 22, 14147–14175, https://doi.org/10.5194/acp-22-14147-2022, https://doi.org/10.5194/acp-22-14147-2022, 2022
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Mixing experiments are crucial and highly beneficial for our understanding of atmospheric chemical interactions. However, interpretation quickly becomes complex, and both the experimental design and evaluation need to be scrutinised carefully. Advanced online and offline compositional measurements can reveal substantial additional information to aid in the interpretation of yield data, including components uniquely found in mixtures and property changes in SOA formed from mixtures of VOCs.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, Thomas J. Bannan, Michael Flynn, Spyros N. Pandis, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 13677–13693, https://doi.org/10.5194/acp-22-13677-2022, https://doi.org/10.5194/acp-22-13677-2022, 2022
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The addition of a low-yield precursor to the reactive mixture of aVOC and bVOC can increase or decrease the SOA volatility that is system-dependent. Therefore, the SOA volatility of the mixtures cannot always be predicted based on the additivity. In complex mixtures the formation of lower-volatility products likely outweighs the formation of products with higher volatility. The unique products of each mixture contribute significantly to the signal, suggesting interactions can be important.
Yunqi Shao, Aristeidis Voliotis, Mao Du, Yu Wang, Kelly Pereira, Jacqueline Hamilton, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 9799–9826, https://doi.org/10.5194/acp-22-9799-2022, https://doi.org/10.5194/acp-22-9799-2022, 2022
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This study explored the chemical properties of secondary organic aerosol (SOA) that formed from photo-oxidation of single and mixed biogenic and anthropogenic precursors. We showed that SOA chemical properties in a mixed vapour system are mainly affected by the
higher-yield precursor's oxidation products and products from
cross-product formation. This study also identifies potential tracer compounds in a mixed vapour system that might be used in SOA source attribution in future ambient studies.
Mao Du, Aristeidis Voliotis, Yunqi Shao, Yu Wang, Thomas J. Bannan, Kelly L. Pereira, Jacqueline F. Hamilton, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Meas. Tech., 15, 4385–4406, https://doi.org/10.5194/amt-15-4385-2022, https://doi.org/10.5194/amt-15-4385-2022, 2022
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Atmospheric chemistry plays a key role in the understanding of aerosol formation and air pollution. We designed chamber experiments for the characterization of secondary organic aerosol (SOA) from a biogenic precursor with inorganic seed. Our results highlight the advantages of a combination of online FIGAERO-CIMS and offline LC-Orbitrap MS analytical techniques to characterize the chemical composition of SOA in chamber studies.
Matthias Karl, Liisa Pirjola, Tiia Grönholm, Mona Kurppa, Srinivasan Anand, Xiaole Zhang, Andreas Held, Rolf Sander, Miikka Dal Maso, David Topping, Shuai Jiang, Leena Kangas, and Jaakko Kukkonen
Geosci. Model Dev., 15, 3969–4026, https://doi.org/10.5194/gmd-15-3969-2022, https://doi.org/10.5194/gmd-15-3969-2022, 2022
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The community aerosol dynamics model MAFOR includes several advanced features: coupling with an up-to-date chemistry mechanism for volatile organic compounds, a revised Brownian coagulation kernel that takes into account the fractal geometry of soot particles, a multitude of nucleation parameterizations, size-resolved partitioning of semi-volatile inorganics, and a hybrid method for the formation of secondary organic aerosols within the framework of condensation and evaporation.
Yu Wang, Aristeidis Voliotis, Dawei Hu, Yunqi Shao, Mao Du, Ying Chen, Judith Kleinheins, Claudia Marcolli, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 4149–4166, https://doi.org/10.5194/acp-22-4149-2022, https://doi.org/10.5194/acp-22-4149-2022, 2022
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Aerosol water uptake plays a key role in atmospheric physicochemical processes. We designed chamber experiments on aerosol water uptake of secondary organic aerosol (SOA) from mixed biogenic and anthropogenic precursors with inorganic seed. Our results highlight this chemical composition influences the reconciliation of the sub- and super-saturated water uptake, providing laboratory evidence for understanding the chemical controls of water uptake of the multi-component aerosol.
Jessica Slater, Hugh Coe, Gordon McFiggans, Juha Tonttila, and Sami Romakkaniemi
Atmos. Chem. Phys., 22, 2937–2953, https://doi.org/10.5194/acp-22-2937-2022, https://doi.org/10.5194/acp-22-2937-2022, 2022
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This paper shows the specific impact of black carbon (BC) on the aerosol–planetary boundary layer (PBL) feedback and its influence on a Beijing haze episode. Overall, this paper shows that strong temperature inversions prevent BC heating within the PBL from significantly increasing PBL height, while BC above the PBL suppresses PBL development significantly through the day. From this we suggest a method by which both locally and regionally emitted BC may impact urban pollution episodes.
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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A comprehensive description and characterisation of the Manchester Aerosol Chamber (MAC) was conducted. The MAC has good temperature and relative humidity homogeneity, fast mixing times, and comparable losses of gases and particles with other chambers. The MAC's bespoke control system allows improved duty cycles and repeatable experiments. Moreover, the effect of contamination on performance was also investigated. It is highly recommended to regularly track the chamber's performance.
Matthew W. Christensen, Andrew Gettelman, Jan Cermak, Guy Dagan, Michael Diamond, Alyson Douglas, Graham Feingold, Franziska Glassmeier, Tom Goren, Daniel P. Grosvenor, Edward Gryspeerdt, Ralph Kahn, Zhanqing Li, Po-Lun Ma, Florent Malavelle, Isabel L. McCoy, Daniel T. McCoy, Greg McFarquhar, Johannes Mülmenstädt, Sandip Pal, Anna Possner, Adam Povey, Johannes Quaas, Daniel Rosenfeld, Anja Schmidt, Roland Schrödner, Armin Sorooshian, Philip Stier, Velle Toll, Duncan Watson-Parris, Robert Wood, Mingxi Yang, and Tianle Yuan
Atmos. Chem. Phys., 22, 641–674, https://doi.org/10.5194/acp-22-641-2022, https://doi.org/10.5194/acp-22-641-2022, 2022
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Trace gases and aerosols (tiny airborne particles) are released from a variety of point sources around the globe. Examples include volcanoes, industrial chimneys, forest fires, and ship stacks. These sources provide opportunistic experiments with which to quantify the role of aerosols in modifying cloud properties. We review the current state of understanding on the influence of aerosol on climate built from the wide range of natural and anthropogenic laboratories investigated in recent decades.
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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Secondary ice production (SIP) plays an important role in ice formation within mixed-phase clouds. We present a laboratory investigation of a potentially new SIP mechanism involving the collisions of supercooled water drops with ice particles. At impact, the supercooled water drop fragments form smaller secondary drops. Approximately 30 % of the secondary drops formed during the retraction phase of the supercooled water drop impact freeze over a temperature range of −4 °C to −12 °C.
Aristeidis Voliotis, Yu Wang, Yunqi Shao, Mao Du, Thomas J. Bannan, Carl J. Percival, Spyros N. Pandis, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 14251–14273, https://doi.org/10.5194/acp-21-14251-2021, https://doi.org/10.5194/acp-21-14251-2021, 2021
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Secondary organic aerosol (SOA) formation from mixtures of volatile precursors can be affected by the molecular interactions of the products. Composition and volatility measurements of SOA formed from mixtures of anthropogenic and biogenic precursors reveal processes that can increase or decrease the SOA volatility. The unique products of the mixture were more oxygenated and less volatile than those from either precursor. Analytical context is provided to explore the SOA volatility in mixtures.
Ernesto Reyes-Villegas, Upasana Panda, Eoghan Darbyshire, James M. Cash, Rutambhara Joshi, Ben Langford, Chiara F. Di Marco, Neil J. Mullinger, Mohammed S. Alam, Leigh R. Crilley, Daniel J. Rooney, W. Joe F. Acton, Will Drysdale, Eiko Nemitz, Michael Flynn, Aristeidis Voliotis, Gordon McFiggans, Hugh Coe, James Lee, C. Nicholas Hewitt, Mathew R. Heal, Sachin S. Gunthe, Tuhin K. Mandal, Bhola R. Gurjar, Shivani, Ranu Gadi, Siddhartha Singh, Vijay Soni, and James D. Allan
Atmos. Chem. Phys., 21, 11655–11667, https://doi.org/10.5194/acp-21-11655-2021, https://doi.org/10.5194/acp-21-11655-2021, 2021
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This paper shows the first multisite online measurements of PM1 in Delhi, India, with measurements over different seasons in Old Delhi and New Delhi in 2018. Organic aerosol (OA) source apportionment was performed using positive matrix factorisation (PMF). Traffic was the main primary aerosol source for both OAs and black carbon, seen with PMF and Aethalometer model analysis, indicating that control of primary traffic exhaust emissions would make a significant reduction to Delhi air pollution.
Yu Wang, Aristeidis Voliotis, Yunqi Shao, Taomou Zong, Xiangxinyue Meng, Mao Du, Dawei Hu, Ying Chen, Zhijun Wu, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 11303–11316, https://doi.org/10.5194/acp-21-11303-2021, https://doi.org/10.5194/acp-21-11303-2021, 2021
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Aerosol phase behaviour plays a profound role in atmospheric physicochemical processes. We designed dedicated chamber experiments to study the phase state of secondary organic aerosol from biogenic and anthropogenic mixed precursors. Our results highlight the key role of the organic–inorganic ratio and relative humidity in phase state, but the sources and organic composition are less important. The result provides solid laboratory evidence for understanding aerosol phase in a complex atmosphere.
Langwen Huang and David Topping
Geosci. Model Dev., 14, 2187–2203, https://doi.org/10.5194/gmd-14-2187-2021, https://doi.org/10.5194/gmd-14-2187-2021, 2021
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As our knowledge and understanding of atmospheric aerosol particle evolution and impact grows, designing community mechanistic models requires an ability to capture increasing chemical, physical and therefore numerical complexity. As the landscape of computing software and hardware evolves, it is important to profile the usefulness of emerging platforms in tackling this complexity. With this in mind we present JlBox v1.1, written in Julia.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Astrid Kiendler-Scharr, Åsa M. Hallquist, Mikael Ehn, Hugh Coe, Carl J. Percival, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 21, 3473–3490, https://doi.org/10.5194/acp-21-3473-2021, https://doi.org/10.5194/acp-21-3473-2021, 2021
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A significant fraction of emissions from human activity consists of aromatic hydrocarbons, e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks, e.g. MCM. Cluster analysis of the oxidation product time series distinguishes behaviours of CHON compounds that could aid in identifying functionality.
Simon Patrick O'Meara, Shuxuan Xu, David Topping, M. Rami Alfarra, Gerard Capes, Douglas Lowe, Yunqi Shao, and Gordon McFiggans
Geosci. Model Dev., 14, 675–702, https://doi.org/10.5194/gmd-14-675-2021, https://doi.org/10.5194/gmd-14-675-2021, 2021
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User-friendly and open-source software for simulating aerosol chambers is a valuable tool for research scientists in designing and analysing their experiments. This paper describes a new version of such software and will therefore provide a useful reference for those applying it. Central to the paper is an assessment of the software's accuracy through comparison against previously published simulations.
Jim M. Haywood, Steven J. Abel, Paul A. Barrett, Nicolas Bellouin, Alan Blyth, Keith N. Bower, Melissa Brooks, Ken Carslaw, Haochi Che, Hugh Coe, Michael I. Cotterell, Ian Crawford, Zhiqiang Cui, Nicholas Davies, Beth Dingley, Paul Field, Paola Formenti, Hamish Gordon, Martin de Graaf, Ross Herbert, Ben Johnson, Anthony C. Jones, Justin M. Langridge, Florent Malavelle, Daniel G. Partridge, Fanny Peers, Jens Redemann, Philip Stier, Kate Szpek, Jonathan W. Taylor, Duncan Watson-Parris, Robert Wood, Huihui Wu, and Paquita Zuidema
Atmos. Chem. Phys., 21, 1049–1084, https://doi.org/10.5194/acp-21-1049-2021, https://doi.org/10.5194/acp-21-1049-2021, 2021
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Every year, the seasonal cycle of biomass burning from agricultural practices in Africa creates a huge plume of smoke that travels many thousands of kilometres over the Atlantic Ocean. This study provides an overview of a measurement campaign called the cloud–aerosol–radiation interaction and forcing for year 2017 (CLARIFY-2017) and documents the rationale, deployment strategy, observations, and key results from the campaign which utilized the heavily equipped FAAM atmospheric research aircraft.
Douglas Morrison, Ian Crawford, Nicholas Marsden, Michael Flynn, Katie Read, Luis Neves, Virginia Foot, Paul Kaye, Warren Stanley, Hugh Coe, David Topping, and Martin Gallagher
Atmos. Chem. Phys., 20, 14473–14490, https://doi.org/10.5194/acp-20-14473-2020, https://doi.org/10.5194/acp-20-14473-2020, 2020
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We provide conservative estimates of the concentrations of bacteria within transatlantic dust clouds, originating from the African continent. We observe significant seasonal differences in the overall concentrations of particles but no seasonal variation in the ratio between bacteria and dust. With bacteria contributing to ice formation at warmer temperatures than dust, our observations should improve the accuracy of climate models.
Jessica Slater, Juha Tonttila, Gordon McFiggans, Paul Connolly, Sami Romakkaniemi, Thomas Kühn, and Hugh Coe
Atmos. Chem. Phys., 20, 11893–11906, https://doi.org/10.5194/acp-20-11893-2020, https://doi.org/10.5194/acp-20-11893-2020, 2020
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The feedback effect between aerosol particles, radiation and meteorology reduces turbulent motion and results in increased surface aerosol concentrations during Beijing haze. Observational analysis and regional modelling studies have examined the feedback effect but these studies are limited. In this work, we set up a high-resolution model for the Beijing environment to examine the sensitivity of the aerosol feedback effect to initial meteorological conditions and aerosol loading.
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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Time-series forecasting methods have often been used to mitigate some of the challenges associated with deploying chemical transport models. In this study we deploy and evaluate Facebook’s Prophetmodel v0.6 in predicting hourly concentrations of Nitrogen Dioxide [NO2]. et. Overall we find the Prophet model offers a relatively effective and simple way to make predictions about NO2 at local levels.
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.
Yu Wang, Ying Chen, Zhijun Wu, Dongjie Shang, Yuxuan Bian, Zhuofei Du, Sebastian H. Schmitt, Rong Su, Georgios I. Gkatzelis, Patrick Schlag, Thorsten Hohaus, Aristeidis Voliotis, Keding Lu, Limin Zeng, Chunsheng Zhao, M. Rami Alfarra, Gordon McFiggans, Alfred Wiedensohler, Astrid Kiendler-Scharr, Yuanhang Zhang, and Min Hu
Atmos. Chem. Phys., 20, 2161–2175, https://doi.org/10.5194/acp-20-2161-2020, https://doi.org/10.5194/acp-20-2161-2020, 2020
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Severe haze events, with high particulate nitrate (pNO3−) burden, frequently prevail in Beijing. In this study, we demonstrate a mutual-promotion effect between aerosol water uptake and pNO3− formation backed up by theoretical calculations and field observations throughout a typical pNO3−-dominated haze event in Beijing wintertime. This self-amplified mutual-promotion effect between aerosol water content and particulate nitrate can rapidly deteriorate air quality and degrade visibility.
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.
Edward Gryspeerdt, Johannes Mülmenstädt, Andrew Gettelman, Florent F. Malavelle, Hugh Morrison, David Neubauer, Daniel G. Partridge, Philip Stier, Toshihiko Takemura, Hailong Wang, Minghuai Wang, and Kai Zhang
Atmos. Chem. Phys., 20, 613–623, https://doi.org/10.5194/acp-20-613-2020, https://doi.org/10.5194/acp-20-613-2020, 2020
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Aerosol radiative forcing is a key uncertainty in our understanding of the human forcing of the climate, with much of this uncertainty coming from aerosol impacts on clouds. Observation-based estimates of the radiative forcing are typically smaller than those from global models, but it is not clear if they are more reliable. This work shows how the forcing components in global climate models can be identified, highlighting similarities between the two methods and areas for future investigation.
Olga Garmash, Matti P. Rissanen, Iida Pullinen, Sebastian Schmitt, Oskari Kausiala, Ralf Tillmann, Defeng Zhao, Carl Percival, Thomas J. Bannan, Michael Priestley, Åsa M. Hallquist, Einhard Kleist, Astrid Kiendler-Scharr, Mattias Hallquist, Torsten Berndt, Gordon McFiggans, Jürgen Wildt, Thomas F. Mentel, and Mikael Ehn
Atmos. Chem. Phys., 20, 515–537, https://doi.org/10.5194/acp-20-515-2020, https://doi.org/10.5194/acp-20-515-2020, 2020
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Highly oxygenated organic molecules (HOMs) facilitate aerosol formation in the atmosphere. Using NO3− chemical ionization mass spectrometry we investigated HOM composition and yield in oxidation of aromatic compounds at different reactant concentrations, in the presence of NOx and seed aerosol. Higher OH concentrations increased HOM yield, suggesting multiple oxidation steps, and affected HOM composition, potentially explaining in part discrepancies in published secondary organic aerosol yields.
Ying Chen, Oliver Wild, Edmund Ryan, Saroj Kumar Sahu, Douglas Lowe, Scott Archer-Nicholls, Yu Wang, Gordon McFiggans, Tabish Ansari, Vikas Singh, Ranjeet S. Sokhi, Alex Archibald, and Gufran Beig
Atmos. Chem. Phys., 20, 499–514, https://doi.org/10.5194/acp-20-499-2020, https://doi.org/10.5194/acp-20-499-2020, 2020
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PM2.5 and O3 are two major air pollutants. Some mitigation strategies focusing on reducing PM2.5 may lead to substantial increase in O3. We use statistical emulation combined with atmospheric transport model to perform thousands of sensitivity numerical studies to identify the major sources of PM2.5 and O3 and to develop strategies targeted at both pollutants. Our scientific evidence suggests that regional coordinated emission control is required to mitigate PM2.5 whilst preventing O3 increase.
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.
Zongbo Shi, Tuan Vu, Simone Kotthaus, Roy M. Harrison, Sue Grimmond, Siyao Yue, Tong Zhu, James Lee, Yiqun Han, Matthias Demuzere, Rachel E. Dunmore, Lujie Ren, Di Liu, Yuanlin Wang, Oliver Wild, James Allan, W. Joe Acton, Janet Barlow, Benjamin Barratt, David Beddows, William J. Bloss, Giulia Calzolai, David Carruthers, David C. Carslaw, Queenie Chan, Lia Chatzidiakou, Yang Chen, Leigh Crilley, Hugh Coe, Tie Dai, Ruth Doherty, Fengkui Duan, Pingqing Fu, Baozhu Ge, Maofa Ge, Daobo Guan, Jacqueline F. Hamilton, Kebin He, Mathew Heal, Dwayne Heard, C. Nicholas Hewitt, Michael Hollaway, Min Hu, Dongsheng Ji, Xujiang Jiang, Rod Jones, Markus Kalberer, Frank J. Kelly, Louisa Kramer, Ben Langford, Chun Lin, Alastair C. Lewis, Jie Li, Weijun Li, Huan Liu, Junfeng Liu, Miranda Loh, Keding Lu, Franco Lucarelli, Graham Mann, Gordon McFiggans, Mark R. Miller, Graham Mills, Paul Monk, Eiko Nemitz, Fionna O'Connor, Bin Ouyang, Paul I. Palmer, Carl Percival, Olalekan Popoola, Claire Reeves, Andrew R. Rickard, Longyi Shao, Guangyu Shi, Dominick Spracklen, David Stevenson, Yele Sun, Zhiwei Sun, Shu Tao, Shengrui Tong, Qingqing Wang, Wenhua Wang, Xinming Wang, Xuejun Wang, Zifang Wang, Lianfang Wei, Lisa Whalley, Xuefang Wu, Zhijun Wu, Pinhua Xie, Fumo Yang, Qiang Zhang, Yanli Zhang, Yuanhang Zhang, and Mei Zheng
Atmos. Chem. Phys., 19, 7519–7546, https://doi.org/10.5194/acp-19-7519-2019, https://doi.org/10.5194/acp-19-7519-2019, 2019
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APHH-Beijing is a collaborative international research programme to study the sources, processes and health effects of air pollution in Beijing. This introduction to the special issue provides an overview of (i) the APHH-Beijing programme, (ii) the measurement and modelling activities performed as part of it and (iii) the air quality and meteorological conditions during joint intensive field campaigns as a core activity within APHH-Beijing.
Martin Osborne, Florent F. Malavelle, Mariana Adam, Joelle Buxmann, Jaqueline Sugier, Franco Marenco, and Jim Haywood
Atmos. Chem. Phys., 19, 3557–3578, https://doi.org/10.5194/acp-19-3557-2019, https://doi.org/10.5194/acp-19-3557-2019, 2019
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In this paper we present an analysis of the unusual
red skyevent that occurred over the UK on 15 and 16 October 2017. We use measurements from the Met Office operational lidar and sun-photometer network, as well as other data and model output, to show that the event was caused by the passage of ex-hurricane Ophelia which transported unusual amounts of dust from the Sahara to the UK as well as smoke from forest fires in Portugal.
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.
Florent F. Malavelle, Jim M. Haywood, Lina M. Mercado, Gerd A. Folberth, Nicolas Bellouin, Stephen Sitch, and Paulo Artaxo
Atmos. Chem. Phys., 19, 1301–1326, https://doi.org/10.5194/acp-19-1301-2019, https://doi.org/10.5194/acp-19-1301-2019, 2019
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Diffuse light can increase the efficiency of vegetation photosynthesis. Diffuse light results from scattering by either clouds or aerosols in the atmosphere. During the dry season biomass burning (BB) on the edges of the Amazon rainforest contributes significantly to the aerosol burden over the entire region. We show that despite a modest effect of change in light conditions, the overall impact of BB aerosols on the vegetation is still important when indirect climate feedbacks are considered.
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.
Kelly L. Pereira, Rachel Dunmore, James Whitehead, M. Rami Alfarra, James D. Allan, Mohammed S. Alam, Roy M. Harrison, Gordon McFiggans, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 18, 11073–11096, https://doi.org/10.5194/acp-18-11073-2018, https://doi.org/10.5194/acp-18-11073-2018, 2018
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Exhaust emissions from a light-duty diesel engine were introduced into an atmospheric simulation chamber which was used as a holding-cell for sampling, allowing instruments capable of providing detailed chemical speciation of exhaust gas emissions to be used. The effect of different engine conditions on the exhaust gas composition was investigated. The exhaust composition changed considerably due to two influencing factors, engine combustion and diesel oxidative catalyst efficiency.
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.
Kathryn Fowler, Paul J. Connolly, David O. Topping, and Simon O'Meara
Atmos. Chem. Phys., 18, 1629–1642, https://doi.org/10.5194/acp-18-1629-2018, https://doi.org/10.5194/acp-18-1629-2018, 2018
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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.
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.
Huan Yao, Yu Song, Mingxu Liu, Scott Archer-Nicholls, Douglas Lowe, Gordon McFiggans, Tingting Xu, Pin Du, Jianfeng Li, Yusheng Wu, Min Hu, Chun Zhao, and Tong Zhu
Atmos. Chem. Phys., 17, 5205–5219, https://doi.org/10.5194/acp-17-5205-2017, https://doi.org/10.5194/acp-17-5205-2017, 2017
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.
James D. Whitehead, Eoghan Darbyshire, Joel Brito, Henrique M. J. Barbosa, Ian Crawford, Rafael Stern, Martin W. Gallagher, Paul H. Kaye, James D. Allan, Hugh Coe, Paulo Artaxo, and Gordon McFiggans
Atmos. Chem. Phys., 16, 9727–9743, https://doi.org/10.5194/acp-16-9727-2016, https://doi.org/10.5194/acp-16-9727-2016, 2016
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We present measurements of aerosols during the transition from wet to dry seasons at a pristine rainforest site in central Amazonia. By excluding pollution episodes, we focus on natural biogenic aerosols. Submicron aerosols are dominated by organic material, similar to previous wet season measurements. Larger particles are dominated by biological material, mostly fungal spores, with higher concentrations at night. This study provides important data on the nature of particles above the Amazon.
Scott Archer-Nicholls, Douglas Lowe, David M. Schultz, and Gordon McFiggans
Atmos. Chem. Phys., 16, 5573–5594, https://doi.org/10.5194/acp-16-5573-2016, https://doi.org/10.5194/acp-16-5573-2016, 2016
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The response of the Weather Research and Forecasting model with Chemistry to forcings by biomass burning aerosol were investigated in high-resolution nested domains over Brazil. The aerosol-layer was found to have a negative direct effect at the top of the atmosphere, but this was largely cancelled by a semi-direct effect which inhibited afternoon cloud formation. The cloud response to the aerosol was found to be highly sensitive to model resolution and the use of convective parameterisation.
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.
M. Paramonov, V.-M. Kerminen, M. Gysel, P. P. Aalto, M. O. Andreae, E. Asmi, U. Baltensperger, A. Bougiatioti, D. Brus, G. P. Frank, N. Good, S. S. Gunthe, L. Hao, M. Irwin, A. Jaatinen, Z. Jurányi, S. M. King, A. Kortelainen, A. Kristensson, H. Lihavainen, M. Kulmala, U. Lohmann, S. T. Martin, G. McFiggans, N. Mihalopoulos, A. Nenes, C. D. O'Dowd, J. Ovadnevaite, T. Petäjä, U. Pöschl, G. C. Roberts, D. Rose, B. Svenningsson, E. Swietlicki, E. Weingartner, J. Whitehead, A. Wiedensohler, C. Wittbom, and B. Sierau
Atmos. Chem. Phys., 15, 12211–12229, https://doi.org/10.5194/acp-15-12211-2015, https://doi.org/10.5194/acp-15-12211-2015, 2015
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The research paper presents the first comprehensive overview of field measurements with the CCN Counter performed at a large number of locations around the world within the EUCAARI framework. The paper sheds light on the CCN number concentrations and activated fractions around the world and their dependence on the water vapour supersaturation ratio, the dependence of aerosol hygroscopicity on particle size, and seasonal and diurnal variation of CCN activation and hygroscopic properties.
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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J. D. Allan, P. I. Williams, J. Najera, J. D. Whitehead, M. J. Flynn, J. W. Taylor, D. Liu, E. Darbyshire, L. J. Carpenter, R. Chance, S. J. Andrews, S. C. Hackenberg, and G. McFiggans
Atmos. Chem. Phys., 15, 5599–5609, https://doi.org/10.5194/acp-15-5599-2015, https://doi.org/10.5194/acp-15-5599-2015, 2015
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New particle formation (NPF) is an important contributor to aerosol number concentrations in the Arctic and thus has a major role in dictating cloud properties and climate in this region. Here we present direct evidence that the oxidation of iodine in the atmosphere causes NPF in the Greenland Sea. This is important because this is a NPF mechanism that has not previously been considered in modelling studies at these latitudes.
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.
M. D. Jolleys, H. Coe, G. McFiggans, J. W. Taylor, S. J. O'Shea, M. Le Breton, S. J.-B. Bauguitte, S. Moller, P. Di Carlo, E. Aruffo, P. I. Palmer, J. D. Lee, C. J. Percival, and M. W. Gallagher
Atmos. Chem. Phys., 15, 3077–3095, https://doi.org/10.5194/acp-15-3077-2015, https://doi.org/10.5194/acp-15-3077-2015, 2015
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Particulate emissions in the form of organic aerosol from boreal forest fires in Canada have been measured during an aircraft measurement campaign. Ratios of the amount of aerosol emitted relative to gas species such as CO were calculated and show high levels of variability throughout the campaign. This variability is affected by both changes in fire conditions, as fires tended to die down later in the measurement period, and by changes to the aerosol due to chemical reactions in the atmosphere.
S. Archer-Nicholls, D. Lowe, E. Darbyshire, W. T. Morgan, M. M. Bela, G. Pereira, J. Trembath, J. W. Kaiser, K. M. Longo, S. R. Freitas, H. Coe, and G. McFiggans
Geosci. Model Dev., 8, 549–577, https://doi.org/10.5194/gmd-8-549-2015, https://doi.org/10.5194/gmd-8-549-2015, 2015
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The regional WRF-Chem model was used to study aerosol particles from biomass burning in South America. The modelled estimates of fire plume injection heights were found to be too high, with serious implications for modelled aerosol vertical distribution, transport and impacts on local climate. A modified emission scenario was developed which improved the predicted injection height. Model results were compared and evaluated against in situ measurements from the 2012 SAMBBA flight campaign.
F. Pacifico, G. A. Folberth, S. Sitch, J. M. Haywood, L. V. Rizzo, F. F. Malavelle, and P. Artaxo
Atmos. Chem. Phys., 15, 2791–2804, https://doi.org/10.5194/acp-15-2791-2015, https://doi.org/10.5194/acp-15-2791-2015, 2015
D. Lowe, S. Archer-Nicholls, W. Morgan, J. Allan, S. Utembe, B. Ouyang, E. Aruffo, M. Le Breton, R. A. Zaveri, P. Di Carlo, C. Percival, H. Coe, R. Jones, and G. McFiggans
Atmos. Chem. Phys., 15, 1385–1409, https://doi.org/10.5194/acp-15-1385-2015, https://doi.org/10.5194/acp-15-1385-2015, 2015
J. D. Whitehead, M. Irwin, J. D. Allan, N. Good, and G. McFiggans
Atmos. Chem. Phys., 14, 11833–11841, https://doi.org/10.5194/acp-14-11833-2014, https://doi.org/10.5194/acp-14-11833-2014, 2014
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Water uptake of ambient particles was measured by 2 independent techniques at a wide range of locations between 2007 and 2013. The agreement between the techniques was mixed and hence the number of potential cloud seeds calculated from the measurements frequently showed discrepancies. Whilst there is sensitivity to how well we measure the size of the particles, much of the difference depends on how the particles behave when exposed to moisture in the different techniques (and in the atmosphere).
S. Archer-Nicholls, D. Lowe, S. Utembe, J. Allan, R. A. Zaveri, J. D. Fast, Ø. Hodnebrog, H. Denier van der Gon, and G. McFiggans
Geosci. Model Dev., 7, 2557–2579, https://doi.org/10.5194/gmd-7-2557-2014, https://doi.org/10.5194/gmd-7-2557-2014, 2014
M. J. Lawler, J. Whitehead, C. O'Dowd, C. Monahan, G. McFiggans, and J. N. Smith
Atmos. Chem. Phys., 14, 11557–11569, https://doi.org/10.5194/acp-14-11557-2014, https://doi.org/10.5194/acp-14-11557-2014, 2014
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This work describes the chemical and physical characterization of very small (< 100 nm diameter) particles in the marine atmosphere. We show that sea salt is present even at very small sizes and present evidence that organic species are important contributors to apparent new particle formation events over the ocean.
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
M. R. Alfarra, N. Good, K. P. Wyche, J. F. Hamilton, P. S. Monks, A. C. Lewis, and G. McFiggans
Atmos. Chem. Phys., 13, 11769–11789, https://doi.org/10.5194/acp-13-11769-2013, https://doi.org/10.5194/acp-13-11769-2013, 2013
J. F. Hamilton, M. R. Alfarra, N. Robinson, M. W. Ward, A. C. Lewis, G. B. McFiggans, H. Coe, and J. D. Allan
Atmos. Chem. Phys., 13, 11295–11305, https://doi.org/10.5194/acp-13-11295-2013, https://doi.org/10.5194/acp-13-11295-2013, 2013
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
D. Liu, J. Allan, J. Whitehead, D. Young, M. Flynn, H. Coe, G. McFiggans, Z. L. Fleming, and B. Bandy
Atmos. Chem. Phys., 13, 2015–2029, https://doi.org/10.5194/acp-13-2015-2013, https://doi.org/10.5194/acp-13-2015-2013, 2013
Related subject area
Subject: Clouds and Precipitation | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Ambient and intrinsic dependencies of evolving ice-phase particles within a decaying winter storm during IMPACTS
High-resolution modeling of early contrail evolution from hydrogen-powered aircraft
Accelerated impact of airborne glaciogenic seeding of stratiform clouds by turbulence
Failed cyclogenesis of a mesoscale convective system near Cabo Verde: the role of the Saharan trade wind layer among other inhibiting factors observed during the CADDIWA field campaign
Sensitivities of simulated mixed-phase Arctic multilayer clouds to primary and secondary ice processes
Assessing glaciogenic seeding impacts in Australia's Snowy Mountains: an ensemble modeling approach
How the representation of microphysical processes affects tropical condensate in the global storm-resolving model ICON
Magnitude and timescale of liquid water path adjustments to cloud droplet number concentration perturbations for nocturnal non-precipitating marine stratocumulus
Cold pools mediate mesoscale adjustments of trade-cumulus fields to changes in cloud droplet number concentration
Numerical case study of the aerosol–cloud interactions in warm boundary layer clouds over the eastern North Atlantic with an interactive chemistry module
Influence of temperature and humidity on contrail formation regions in the general circulation model EMAC: a spring case study
On the impact of thunder on cloud ice crystals and droplets
Counteracting influences of gravitational settling modulate aerosol impacts on cloud-base-lowering fog characteristics
The critical number and size of precipitation embryos to accelerate warm rain initiation
Impact on the stratocumulus-to-cumulus transition of the interaction of cloud microphysics and macrophysics with large-scale circulation
Technical note: Phase space depiction of cloud condensation nuclei activation and cloud droplet diffusional growth
Impact of wildfire smoke on Arctic cirrus formation – Part 2: Simulation of MOSAiC 2019–2020 cases
Constraining aerosol–cloud adjustments by uniting surface observations with a perturbed parameter ensemble
Investigating ice formation pathways using a novel two-moment multi-class cloud microphysics scheme
Exploiting airborne far-infrared measurements to optimise an ice cloud retrieval
Microphysics regimes due to haze–cloud interactions: cloud oscillation and cloud collapse
Microphysical fingerprints in anvil cloud albedo
Influence of Secondary Ice Production on cloud and rain properties: Analysis of the HYMEX IOP7a Heavy Precipitation Event
Factors Causing Stratocumulus to Deviate from Subtropical High Variability on Seasonal to Interannual Timescales
The influence of Amazonian anthropogenic emissions on new particle formation, aerosol, cloud and surface rain
Impact of secondary ice production on thunderstorm electrification under different aerosol conditions
Tropical cirrus evolution in a km-scale model with improved ice microphysics
Model analysis of biases in the satellite-diagnosed aerosol effect on the cloud liquid water path
Impacts of aerosol-radiation and aerosol-cloud interactions on a short-term heavy rainfall event – A case study in the Guanzhong Basin, China
Evaluation of biases in mid-to-high-latitude surface snowfall and cloud phase in ERA5 and CMIP6 using satellite observations
Dynamical imprints on precipitation cluster statistics across a hierarchy of high-resolution simulations
Ice formation processes key in determining WCB outflow cirrus properties
Role of a key microphysical factor in mixed-phase stratocumulus clouds and their interactions with aerosols
Investigating the impact of subgrid-scale aerosol-cloud interaction on mesoscale meteorology prediction
Different responses of cold-air outbreak clouds to aerosol and ice production depending on cloud temperature
Identifying Synoptic Controls on Boundary Layer Thermodynamic and Cloud Properties in a Regional Forecast Model
Correction of ERA5 temperature and relative humidity biases by bivariate quantile mapping for contrail formation analysis
Can pollen affect precipitation?
Potential impacts of marine fuel regulations on an Arctic stratocumulus case and its radiative response
The subtleties of three-dimensional radiative effects in contrails and cirrus clouds
The impact of the mesh size and microphysics scheme on the representation of mid-level clouds in the ICON model in hilly and complex terrain
The role of ascent timescales for warm conveyor belt (WCB) moisture transport into the upper troposphere and lower stratosphere (UTLS)
On the Processes Determining the Slope of Cloud-Water Adjustments in Non-Precipitating Stratocumulus
Analysis of raindrop size distribution from the double moment cloud microphysics scheme for monsoon over a tropical station
High sensitivity of simulated fog properties to parameterized aerosol activation in case studies from ParisFog
Adiabatic and radiative cooling are both important causes of aerosol activation in simulated fog events in Europe
Estimating the concentration of silver iodide needed to detect unambiguous signatures of glaciogenic cloud seeding
Ice-nucleating particle concentration impacts cloud properties over Dronning Maud Land, East Antarctica, in COSMO-CLM2
Numerical simulation of aerosol concentration effects on cloud droplet size spectrum evolutions of warm stratiform clouds in Jiangxi, China
The impact of aerosol on cloud water: a heuristic perspective
Andrew DeLaFrance, Lynn A. McMurdie, Angela K. Rowe, and Andrew J. Heymsfield
Atmos. Chem. Phys., 25, 8087–8106, https://doi.org/10.5194/acp-25-8087-2025, https://doi.org/10.5194/acp-25-8087-2025, 2025
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Numerical modeling simulations are used to investigate ice crystal growth and decay processes within a banded region of enhanced precipitation rates during a prominent winter storm. We identify robust primary ice growth in the upper portion of the cloud but decay exceeding 70 % during fallout through a subsaturated layer. The ice fall characteristics and decay rate are sensitive to the ambient cloud properties, which has implications for radar-based measurements and precipitation accumulations.
Annemarie Lottermoser and Simon Unterstrasser
Atmos. Chem. Phys., 25, 7903–7924, https://doi.org/10.5194/acp-25-7903-2025, https://doi.org/10.5194/acp-25-7903-2025, 2025
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Contrail cirrus significantly contributes to aviation's overall climate impact. As hydrogen combustion and fuel cell use are emerging technologies for aircraft propulsion, we simulated individual contrails from hydrogen propulsion during the first 6 min after exhaust emission, termed the vortex phase. The ice crystal loss during that stage is crucial, as the number of ice crystals has a large impact on the further evolution of contrails into contrail cirrus and their radiative forcing.
Meilian Chen, Xiaoqin Jing, Jiaojiao Li, Jing Yang, Xiaobo Dong, Bart Geerts, Yan Yin, Baojun Chen, Lulin Xue, Mengyu Huang, Ping Tian, and Shaofeng Hua
Atmos. Chem. Phys., 25, 7581–7596, https://doi.org/10.5194/acp-25-7581-2025, https://doi.org/10.5194/acp-25-7581-2025, 2025
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Several recent studies have reported complete cloud glaciation induced by airborne-based glaciogenic cloud seeding over plains. Since turbulence is an important factor to maintain clouds in a mixed phase, it is hypothesized that turbulence may have an impact on the seeding effect. This hypothesis is evident in the present study, which shows that turbulence can accelerate the impact of airborne glaciogenic seeding of stratiform clouds.
Guillaume Feger, Jean-Pierre Chaboureau, Thibaut Dauhut, Julien Delanoë, and Pierre Coutris
Atmos. Chem. Phys., 25, 7447–7465, https://doi.org/10.5194/acp-25-7447-2025, https://doi.org/10.5194/acp-25-7447-2025, 2025
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Saharan air at the trade wind layer, cold pools, and dry upper troposphere has these three main factors inhibiting the cyclogenesis of the Pierre Henri mesoscale convective system. The findings were obtained through observations made during two flights of the Clouds-Atmospheric Dynamics-Dust Interactions in West Africa (CADDIWA) campaign and a convection-permitting simulation run with the Meso-NH model. They provide new insights into the complex dynamics of cyclogenesis in the Cabo Verde region and challenge the existing model of the Saharan Air Layer (SAL).
Gabriella Wallentin, Annika Oertel, Luisa Ickes, Peggy Achtert, Matthias Tesche, and Corinna Hoose
Atmos. Chem. Phys., 25, 6607–6631, https://doi.org/10.5194/acp-25-6607-2025, https://doi.org/10.5194/acp-25-6607-2025, 2025
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Multilayer clouds are common in the Arctic but remain underrepresented. We use an atmospheric model to simulate multilayer cloud cases from the Arctic expedition MOSAiC 2019/2020. We find that it is complex to accurately model these cloud layers due to the lack of correct temperature profiles. The model also struggles to capture the observed cloud phase and the relative concentration of cloud droplets and cloud ice. We constrain our model to measured aerosols to mitigate this issue.
Sisi Chen, Lulin Xue, Sarah A. Tessendorf, Thomas Chubb, Andrew Peace, Suzanne Kenyon, Johanna Speirs, Jamie Wolff, and Bill Petzke
Atmos. Chem. Phys., 25, 6703–6724, https://doi.org/10.5194/acp-25-6703-2025, https://doi.org/10.5194/acp-25-6703-2025, 2025
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This study aims to investigate how cloud seeding affects snowfall in Australia's Snowy Mountains. By running simulations with different setups, we found that seeding impact varies greatly with weather conditions. Seeding increased snow in stable weather but sometimes reduced it in stormy weather. This helps us to better understand when seeding works best to boost water supplies.
Ann Kristin Naumann, Monika Esch, and Bjorn Stevens
Atmos. Chem. Phys., 25, 6429–6444, https://doi.org/10.5194/acp-25-6429-2025, https://doi.org/10.5194/acp-25-6429-2025, 2025
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This study explores how uncertainties in the representation of microphysical processes affect the tropical condensate distribution in the global storm-resolving model ICON. The results point to the importance of the fall speed of hydrometeor particles and to a simple relationship: the faster a condensate falls, the less there is of it. Implications for the energy balance and precipitation properties are discussed.
Yao-Sheng Chen, Prasanth Prabhakaran, Fabian Hoffmann, Jan Kazil, Takanobu Yamaguchi, and Graham Feingold
Atmos. Chem. Phys., 25, 6141–6159, https://doi.org/10.5194/acp-25-6141-2025, https://doi.org/10.5194/acp-25-6141-2025, 2025
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Injecting sea salt aerosols into marine stratiform clouds can distribute the cloud water over more droplets in smaller sizes. This process is expected to make the clouds brighter, allowing them to reflect more sunlight back to space. However, it may also cause the clouds to lose water over time, reducing their ability to reflect sunlight. We use a computer model to show that the loss of cloud water occurs relatively quickly and does not completely offset the initial brightening.
Pouriya Alinaghi, Fredrik Jansson, Daniel A. Blázquez, and Franziska Glassmeier
Atmos. Chem. Phys., 25, 6121–6139, https://doi.org/10.5194/acp-25-6121-2025, https://doi.org/10.5194/acp-25-6121-2025, 2025
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Shallow clouds in the trades are a major source of uncertainty in climate projections. These clouds organize into striking mesoscale patterns that are exactly what climate models lack. This study explores the origin of such patterns and investigates how variations in microscale properties control them. The importance of microscale effects is compared to that of large-scale forcing on the mesoscale organization of trade-cumulus fields.
Hsiang-He Lee, Xue Zheng, Shaoyue Qiu, and Yuan Wang
Atmos. Chem. Phys., 25, 6069–6091, https://doi.org/10.5194/acp-25-6069-2025, https://doi.org/10.5194/acp-25-6069-2025, 2025
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The study investigates how aerosol–cloud interactions affect warm boundary layer stratiform clouds over the eastern North Atlantic. High-resolution weather model simulations reveal that non-rain clouds at the edge of cloud systems are prone to evaporation, leading to an aerosol drying effect and a transition of aerosols back to the accumulation mode for future activation. The study shows that this dynamic behavior is often not adequately represented in most previous prescribed-aerosol simulations.
Patrick Peter, Sigrun Matthes, Christine Frömming, Patrick Jöckel, Luca Bugliaro, Andreas Giez, Martina Krämer, and Volker Grewe
Atmos. Chem. Phys., 25, 5911–5934, https://doi.org/10.5194/acp-25-5911-2025, https://doi.org/10.5194/acp-25-5911-2025, 2025
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Our study examines how well the global climate model EMAC (ECHAM/MESSy Atmospheric Chemistry) predicts contrail formation by analysing temperature and humidity – two key factors for contrail development and persistence. The model underestimates temperature, leading to an overprediction of contrail formation and larger ice-supersaturated regions. Adjusting the model improves temperature accuracy but adds uncertainties. Better predictions of contrail formation areas can help optimise flight tracks to reduce aviation's climate effect.
Konstantinos Kourtidis, Stavros Stathopoulos, and Vassilis Amiridis
Atmos. Chem. Phys., 25, 5935–5946, https://doi.org/10.5194/acp-25-5935-2025, https://doi.org/10.5194/acp-25-5935-2025, 2025
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The sound of thunder induces mechanical effects on cloud droplets and ice particles, causing changes in their size distribution. A shock wave near the lightning channel causes extensive shattering of cloud particles. At a distance, the audio wave will cause agglomeration of particles. So, thunder may influence the rain generation process and the radiative properties of clouds. As global warming may influence the occurrence rate of lightning, a climate feedback may be induced by these mechanisms.
Nathan H. Pope and Adele L. Igel
Atmos. Chem. Phys., 25, 5433–5444, https://doi.org/10.5194/acp-25-5433-2025, https://doi.org/10.5194/acp-25-5433-2025, 2025
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We used an atmospheric model that simulates a single column to study the sensitivity of marine fog formed through the lowering of the base of a stratus cloud to meteorology and aerosols. We found that higher aerosol concentration reduces the likelihood and duration of fog but leads to denser fog. This overall trend was caused by multiple physical mechanisms depending on conditions.
Jung-Sub Lim, Yign Noh, Hyunho Lee, and Fabian Hoffmann
Atmos. Chem. Phys., 25, 5313–5329, https://doi.org/10.5194/acp-25-5313-2025, https://doi.org/10.5194/acp-25-5313-2025, 2025
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Rain formation in warm clouds begins when small droplets collide, but this process can be slow without larger droplets. We used simulations to explore the role of bigger droplets, known as precipitation embryos, in triggering rain. We found that they speed up rain only when their size and number exceed a critical threshold. This threshold becomes larger when collisions are naturally efficient, such as in clouds with broad droplet size distributions or strong turbulence.
Je-Yun Chun, Robert Wood, Peter N. Blossey, and Sarah J. Doherty
Atmos. Chem. Phys., 25, 5251–5271, https://doi.org/10.5194/acp-25-5251-2025, https://doi.org/10.5194/acp-25-5251-2025, 2025
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This study explores how aerosols affect clouds transitioning from stratocumulus to cumulus along trade winds under varying atmospheric conditions. We found that aerosols typically reduce precipitation and raise cloud height, but their impact changes when subsidence changes by aerosol enhancement are considered. Our findings indicate that the cooling effect of aerosols might be overestimated if these atmospheric changes are not accounted for.
Wojciech W. Grabowski and Hanna Pawlowska
Atmos. Chem. Phys., 25, 5273–5285, https://doi.org/10.5194/acp-25-5273-2025, https://doi.org/10.5194/acp-25-5273-2025, 2025
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A simple diagram to depict cloud droplets' formation via the activation of cloud condensation nuclei (CCN) as well as their subsequent growth and evaporation is presented.
Albert Ansmann, Cristofer Jimenez, Daniel A. Knopf, Johanna Roschke, Johannes Bühl, Kevin Ohneiser, and Ronny Engelmann
Atmos. Chem. Phys., 25, 4867–4884, https://doi.org/10.5194/acp-25-4867-2025, https://doi.org/10.5194/acp-25-4867-2025, 2025
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In this study, we focus on the potential impact of wildfire smoke on cirrus formation. Aerosol and cirrus observations with lidar and radar during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition, presented in the companion paper (Ansmann et al., 2025), are closely linked to comprehensive modeling of ice nucleation in cirrus evolution processes, presented in this article. A clear impact of wildfire smoke on cirrus formation was found.
August Mikkelsen, Daniel T. McCoy, Trude Eidhammer, Andrew Gettelman, Ci Song, Hamish Gordon, and Isabel L. McCoy
Atmos. Chem. Phys., 25, 4547–4570, https://doi.org/10.5194/acp-25-4547-2025, https://doi.org/10.5194/acp-25-4547-2025, 2025
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Whether increased aerosol increases or decreases liquid cloud mass has been a longstanding question. Observed correlations suggest that aerosols thin liquid cloud, but we are able to show that observations were consistent with an increase in liquid cloud in response to aerosols by leveraging a model where causality could be traced.
Tim Lüttmer, Peter Spichtinger, and Axel Seifert
Atmos. Chem. Phys., 25, 4505–4529, https://doi.org/10.5194/acp-25-4505-2025, https://doi.org/10.5194/acp-25-4505-2025, 2025
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We investigate ice formation pathways in idealized convective clouds using a novel microphysics scheme that distinguishes between five ice classes each with their own unique formation mechanism. Ice crystals from rime splintering form the lowermost layer of ice crystals around the updraft core. The majority of ice crystals in the anvil of the convective cloud stems from frozen droplets. Ice stemming from homogeneous and deposition nucleation was only relevant in the overshoot.
Sanjeevani Panditharatne, Helen Brindley, Caroline Cox, Rui Song, Richard Siddans, Richard Bantges, Jonathan Murray, Stuart Fox, and Cathryn Fox
EGUsphere, https://doi.org/10.5194/egusphere-2025-647, https://doi.org/10.5194/egusphere-2025-647, 2025
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Upwelling radiation with wavelengths between 15 and 100 microns is theorised to be highly sensitive to the properties of ice clouds, particularly the shape of the ice crystals. We exploit this sensitivity and perform the first retrieval of ice cloud properties using these wavelengths from an observation taken on an aircraft and evaluate it against measurements of the cloud’s properties.
Fan Yang, Hamed Fahandezh Sadi, Raymond A. Shaw, Fabian Hoffmann, Pei Hou, Aaron Wang, and Mikhail Ovchinnikov
Atmos. Chem. Phys., 25, 3785–3806, https://doi.org/10.5194/acp-25-3785-2025, https://doi.org/10.5194/acp-25-3785-2025, 2025
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Large-eddy simulations of a convection cloud chamber show two new microphysics regimes, cloud oscillation and cloud collapse, due to haze–cloud interactions. Our results suggest that haze particles and their interactions with cloud droplets should be considered especially in polluted conditions. To properly simulate haze–cloud interactions, we need to resolve droplet activation and deactivation processes, instead of using Twomey-type activation parameterization.
Declan L. Finney, Alan M. Blyth, Paul R. Field, Martin I. Daily, Benjamin J. Murray, Mengyu Sun, Paul J. Connolly, Zhiqiang Cui, and Steven Böing
EGUsphere, https://doi.org/10.5194/egusphere-2025-1227, https://doi.org/10.5194/egusphere-2025-1227, 2025
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We present observation-informed modelling from the Deep Convective Microphysics Experiment to study how environmental conditions and cloud processes affect anvil cloud albedo and radiation. Aerosols influencing cloud droplets or influencing ice formation yield varying radiative effects. We introduce fingerprint metrics to discern these effects. Using detailed observations and modelling, we offer insights into high cloud radiative effects and feedbacks.
Pierre Grzegorczyk, Wolfram Wobrock, Aymeric Dziduch, and Céline Planche
EGUsphere, https://doi.org/10.5194/egusphere-2025-819, https://doi.org/10.5194/egusphere-2025-819, 2025
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The impact of secondary ice production (SIP) on a HYMEX intense precipitation event is investigated using 3D bin microphysics. Including SIP improves agreement with in situ aircraft observations (ice crystal number concentration and supercooled drop number fraction), generates small ice crystals and redistributes condensed water mass toward smaller particle sizes. As these crystals melt, the liquid precipitation flux decreases, reducing total precipitation by 8 % and heavy rainfall by 20 %.
Hairu Ding, Bjorn Stevens, and Hauke Schmidt
EGUsphere, https://doi.org/10.5194/egusphere-2025-876, https://doi.org/10.5194/egusphere-2025-876, 2025
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This study examines the physical link between subtropical highs and stratocumulus variability. Using reanalysis data, we test two proposed pathways—one at the surface and one in the free troposphere—but find that neither is a dominant mechanism for stratocumulus variability on seasonal and interannual timescales. These results challenge the assumed influence of subtropical highs on stratocumulus and highlight the need for further research into lower tropospheric stability dynamics.
Xuemei Wang, Kenneth S. Carslaw, Daniel P. Grosvenor, and Hamish Gordon
EGUsphere, https://doi.org/10.5194/egusphere-2025-132, https://doi.org/10.5194/egusphere-2025-132, 2025
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Anthropogenic emissions can influence aerosol particle number concentrations via new particle formation. Our model simulations predict around 10 % increase of the particle and cloud droplet number concentrations when doubling the emissions in the Manaus region in the Amazonian wet season. However, the corresponding changes in cloud water and rain mass are around 4 %. Such weak response implied that this convective environment is not sensitive to the localised anthropogenic emission changes here.
Shiye Huang, Jing Yang, Jiaojiao Li, Qian Chen, Qilin Zhang, and Fengxia Guo
Atmos. Chem. Phys., 25, 1831–1850, https://doi.org/10.5194/acp-25-1831-2025, https://doi.org/10.5194/acp-25-1831-2025, 2025
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Aerosol and secondary ice production are both vital to charge separation in thunderstorms, but the relative importance of different SIP processes to cloud electrification under different aerosol conditions is not well understood. In this study, we show in a clean environment, the shattering of freezing drops has the greatest effect on the charging rate, while in a polluted environment, both rime splintering and the shattering of freezing drops have a significant effect on cloud electrification.
Blaž Gasparini, Rachel Atlas, Aiko Voigt, Martina Krämer, and Peter N. Blossey
EGUsphere, https://doi.org/10.5194/egusphere-2025-203, https://doi.org/10.5194/egusphere-2025-203, 2025
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Tropical cirrus clouds, especially their evolution, are poorly understood, contributing to uncertainty in climate projections. We address this by using novel tracers in a cloud-resolving model to track the life cycle of cirrus clouds, providing insights into cloud formation, ice crystal evolution, and radiative effects. We also improve the model's cloud microphysics with a simple, computationally efficient approach that can be applied to other models.
Harri Kokkola, Juha Tonttila, Silvia M. Calderón, Sami Romakkaniemi, Antti Lipponen, Aapo Peräkorpi, Tero Mielonen, Edward Gryspeerdt, Timo Henrik Virtanen, Pekka Kolmonen, and Antti Arola
Atmos. Chem. Phys., 25, 1533–1543, https://doi.org/10.5194/acp-25-1533-2025, https://doi.org/10.5194/acp-25-1533-2025, 2025
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Understanding how atmospheric aerosols affect clouds is a scientific challenge. One question is how aerosols affects the amount of cloud water. We used a cloud-scale model to study these effects on marine clouds. The study showed that variations in cloud properties and instrument noise can cause bias in satellite-derived cloud water content. However, our results suggest that for similar weather conditions with well-defined aerosol concentrations, satellite data can reliably track these effects.
Naifang Bei, Bo Xiao, Ruonan Wang, Yuning Yang, Lang Liu, Yongming Han, and Guohui Li
EGUsphere, https://doi.org/10.5194/egusphere-2024-3558, https://doi.org/10.5194/egusphere-2024-3558, 2025
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This study uses a cloud-resolving model to examine how aerosols influence a mesoscale convective system (MCS) in central China via aerosol-radiation (ARIs) and aerosol-cloud interactions (ACIs). Without ARIs, added aerosols don’t significantly affect precipitation due to cloud competition for moisture. ARIs can stabilize or enhance convection. High aerosol levels lead to a combined ARI and ACI effect that greatly reduces precipitation.
Franziska Hellmuth, Tim Carlsen, Anne Sophie Daloz, Robert Oscar David, Haochi Che, and Trude Storelvmo
Atmos. Chem. Phys., 25, 1353–1383, https://doi.org/10.5194/acp-25-1353-2025, https://doi.org/10.5194/acp-25-1353-2025, 2025
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This article compares the occurrence of supercooled liquid-containing clouds (sLCCs) and their link to surface snowfall in CloudSat–CALIPSO, ERA5, and the CMIP6 models. Significant discrepancies were found, with ERA5 and CMIP6 consistently overestimating sLCC and snowfall frequency. This bias is likely due to cloud microphysics parameterization. This conclusion has implications for accurately representing cloud phase and snowfall in future climate projections.
Claudia Christine Stephan and Bjorn Stevens
Atmos. Chem. Phys., 25, 1209–1226, https://doi.org/10.5194/acp-25-1209-2025, https://doi.org/10.5194/acp-25-1209-2025, 2025
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Tropical precipitation cluster area and intensity distributions follow power laws, but the physical processes responsible for this behavior remain unknown. We analyze global simulations that realistically represent precipitation processes. We consider Earth-like planets as well as virtual planets to realize different types of large-scale dynamics. Our finding is that power laws in Earth’s precipitation cluster statistics stem from the robust power laws in Earth’s atmospheric wind field.
Tim Lüttmer, Annette Miltenberger, and Peter Spichtinger
EGUsphere, https://doi.org/10.5194/egusphere-2025-185, https://doi.org/10.5194/egusphere-2025-185, 2025
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We investigate ice formation pathways in a warm conveyor belt case study. We employ a multi-phase microphysics scheme that distinguishes between ice from different nucleation processes. Ice crystals in the cirrus outflow mostly stem from in-situ formation. Hence they were formed directly from the vapor phase. Sedimentational redistribution modulates cirrus properties and leads to a disagreement between cirrus origin classifications based on thermodynamic history and nucleation processes.
Seoung Soo Lee, Chang Hoon Jung, Jinho Choi, Young Jun Yoon, Junshik Um, Youtong Zheng, Jianping Guo, Manguttathil G. Manoj, Sang-Keun Song, and Kyung-Ja Ha
Atmos. Chem. Phys., 25, 705–726, https://doi.org/10.5194/acp-25-705-2025, https://doi.org/10.5194/acp-25-705-2025, 2025
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This study attempts to test a general factor that explains differences in the properties of different mixed-phase clouds using a modeling tool. Although this attempt is not to identify a factor that can perfectly explain and represent the properties of different mixed-phase clouds, we believe that this attempt acts as a valuable stepping stone towards a more complete, general way of using climate models to better predict climate change.
Wenjie Zhang, Hong Wang, Xiaoye Zhang, Yue Peng, Zhaodong Liu, Deying Wang, Da Zhang, Chen Han, Yang Zhao, Junting Zhong, Wenxing Jia, Huiqiong Ning, and Huizheng Che
EGUsphere, https://doi.org/10.5194/egusphere-2024-3677, https://doi.org/10.5194/egusphere-2024-3677, 2025
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We implement a real-time subgrid-scale aerosol-cloud interaction (ACI) mechanism in a mesoscale atmospheric chemistry system and find that subgrid-scale ACI can improve meteorological factors predictions. This study demonstrates the importance of real-time subgrid-scale ACI to weather forecast and the necessity of multiscale ACI studies.
Xinyi Huang, Paul R. Field, Benjamin J. Murray, Daniel P. Grosvenor, Floortje van den Heuvel, and Kenneth S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2024-4070, https://doi.org/10.5194/egusphere-2024-4070, 2025
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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.
Jordan Eissner, David Mechem, Yi Jin, Virendra Ghate, and James Booth
EGUsphere, https://doi.org/10.5194/egusphere-2024-3438, https://doi.org/10.5194/egusphere-2024-3438, 2025
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Low-level clouds have important radiative feedbacks and can occur in a range of meteorological conditions, yet our knowledge and prediction of them are insufficient. We evaluate model forecasts of low-level cloud properties across a cold front and the associated environments that they form in. The model represents the meteorological conditions well and produces broken clouds behind the cold front in areas of strong surface forcing, large stability, and large-scale subsiding motion.
Kevin Wolf, Nicolas Bellouin, Olivier Boucher, Susanne Rohs, and Yun Li
Atmos. Chem. Phys., 25, 157–181, https://doi.org/10.5194/acp-25-157-2025, https://doi.org/10.5194/acp-25-157-2025, 2025
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ERA5 atmospheric reanalysis and airborne in situ observations from IAGOS are compared in terms of the representation of the contrail formation potential and the presence of supersaturation. Differences are traced back to biases in ERA5 relative humidity fields. Those biases are addressed by applying a quantile mapping technique that significantly improved contrail estimation based on post-processed ERA5 data.
Marje Prank, Juha Tonttila, Xiaoxia Shang, Sami Romakkaniemi, and Tomi Raatikainen
Atmos. Chem. Phys., 25, 183–197, https://doi.org/10.5194/acp-25-183-2025, https://doi.org/10.5194/acp-25-183-2025, 2025
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Large primary bioparticles such as pollen can be abundant in the atmosphere. In humid conditions pollen can rupture and release a large number of fine sub-pollen particles (SPPs). The paper investigates what kind of birch pollen concentrations are needed for the pollen and SPPs to start playing a noticeable role in cloud processes and alter precipitation formation. In the studied cases only the largest observed pollen concentrations were able to noticeably alter the precipitation formation.
Luís Filipe Escusa dos Santos, Hannah C. Frostenberg, Alejandro Baró Pérez, Annica M. L. Ekman, Luisa Ickes, and Erik S. Thomson
Atmos. Chem. Phys., 25, 119–142, https://doi.org/10.5194/acp-25-119-2025, https://doi.org/10.5194/acp-25-119-2025, 2025
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The Arctic is experiencing enhanced surface warming. The observed decline in Arctic sea-ice extent is projected to lead to an increase in Arctic shipping activity, which may lead to further climatic feedbacks. Using an atmospheric model and results from marine engine experiments that focused on fuel sulfur content reduction and exhaust wet scrubbing, we investigate how ship exhaust particles influence the properties of Arctic clouds. Implications for radiative surface processes are discussed.
Julie Carles, Nicolas Bellouin, Najda Villefranque, and Jean-Louis Dufresne
EGUsphere, https://doi.org/10.5194/egusphere-2024-3642, https://doi.org/10.5194/egusphere-2024-3642, 2025
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Cirrus and contrails affect Earth’s energy balance with a lot of remaining uncertainty. The balance between solar and terrestrial radiation is delicate to calculate, and factors as cloud optical depth, shape, Sun position are crucial to estimate the effect of those clouds on radiation. Also, often neglected three dimensional paths of radiation, or 3D effects, may be important to account for at climatic scale.
Nadja Omanovic, Brigitta Goger, and Ulrike Lohmann
Atmos. Chem. Phys., 24, 14145–14175, https://doi.org/10.5194/acp-24-14145-2024, https://doi.org/10.5194/acp-24-14145-2024, 2024
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We evaluated the numerical weather model ICON in two horizontal resolutions with two bulk microphysics schemes over hilly and complex terrain in Switzerland and Austria, respectively. We focused on the model's ability to simulate mid-level clouds in summer and winter. By combining observational data from two different field campaigns, we show that an increase in the horizontal resolution and a more advanced cloud microphysics scheme is strongly beneficial for cloud representation.
Cornelis Schwenk and Annette Miltenberger
Atmos. Chem. Phys., 24, 14073–14099, https://doi.org/10.5194/acp-24-14073-2024, https://doi.org/10.5194/acp-24-14073-2024, 2024
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Warm conveyor belts (WCBs) transport moisture into the upper atmosphere, where it acts as a greenhouse gas. This transport is not well understood, and the role of rapidly rising air is unclear. We simulate a WCB and look at fast- and slow-rising air to see how moisture is (differently) transported. We find that for fast-ascending air more ice particles reach higher into the atmosphere and that frozen cloud particles are removed differently than during slow ascent, which has more water vapour.
Fabian Hoffmann, Yao-Sheng Chen, and Graham Feingold
EGUsphere, https://doi.org/10.5194/egusphere-2024-3893, https://doi.org/10.5194/egusphere-2024-3893, 2024
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Clouds reflect a substantial portion of the incoming solar radiation back into space. This capacity is determined by the number of cloud droplets, which in turn is influenced by the number of aerosol particles, forming the basis for aerosol-cloud-climate interactions. In this study, we use a simple mixed-layer approach to understand the effect of aerosol on cloud water in non-precipitating stratocumulus.
Kadavathu Sreekumar Apsara, Jayakumar Aravindakshan, Anurose Theethai Jacob, Saji Mohandas, Paul Field, Hamish Gordan, Thara Prabhakaran, Mahen Konwar, and Vijapurap Srinivasa Prasad
EGUsphere, https://doi.org/10.5194/egusphere-2024-3538, https://doi.org/10.5194/egusphere-2024-3538, 2024
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Science has made significant strides in weather prediction, especially for intense tropical rainfall that can lead to floods and landslides. Our study aims to improve monsoon rainfall forecasts by analyzing raindrop sizes. Using a new approach to model raindrop growth, we achieved a more accurate depiction of large rainfall events. These improvements can be generalized to enhance early warning systems, offering reliable predictions that help reduce risks from severe tropical weather events.
Pratapaditya Ghosh, Ian Boutle, Paul Field, Adrian Hill, Anthony Jones, Marie Mazoyer, Katherine J. Evans, Salil Mahajan, Hyun-Gyu Kang, Min Xu, Wei Zhang, Noah Asch, and Hamish Gordon
EGUsphere, https://doi.org/10.5194/egusphere-2024-3376, https://doi.org/10.5194/egusphere-2024-3376, 2024
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We study aerosol-fog interactions near Paris using a weather and climate model with high spatial resolution. We show that our model can simulate fog lifecycle effectively. We find that the fog droplet number concentrations, the amount of liquid water in the fog, and the vertical structure of the fog are highly sensitive to the parameterization that simulates droplet formation and growth. The changes we propose could improve fog forecasts significantly without increasing computational costs.
Pratapaditya Ghosh, Ian Boutle, Paul Field, Adrian Hill, Marie Mazoyer, Katherine J. Evans, Salil Mahajan, Hyun-Gyu Kang, Min Xu, Wei Zhang, and Hamish Gordon
EGUsphere, https://doi.org/10.5194/egusphere-2024-3397, https://doi.org/10.5194/egusphere-2024-3397, 2024
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We study the lifecycle of fog events in Europe using a weather and climate model. By incorporating droplet formation and growth driven by radiative cooling, our model better simulates the total liquid water in foggy atmospheric columns. We show that both adiabatic and radiative cooling play significant, often equally important roles in driving droplet formation and growth. We discuss strategies to address droplet number overpredictions, by improving model physics and addressing model artifacts.
Jing Yang, Jiaojiao Li, Meilian Chen, Xiaoqin Jing, Yan Yin, Bart Geerts, Zhien Wang, Yubao Liu, Baojun Chen, Shaofeng Hua, Hao Hu, Xiaobo Dong, Ping Tian, Qian Chen, and Yang Gao
Atmos. Chem. Phys., 24, 13833–13848, https://doi.org/10.5194/acp-24-13833-2024, https://doi.org/10.5194/acp-24-13833-2024, 2024
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Detecting unambiguous signatures is vital for examining cloud-seeding impacts, but often, seeding signatures are immersed in natural variability. In this study, reflectivity changes induced by glaciogenic seeding using different AgI concentrations are investigated under various conditions, and a method is developed to estimate the AgI concentration needed to detect unambiguous seeding signatures. The results aid in operational seeding-based decision-making regarding the amount of AgI dispersed.
Florian Sauerland, Niels Souverijns, Anna Possner, Heike Wex, Preben Van Overmeiren, Alexander Mangold, Kwinten Van Weverberg, and Nicole van Lipzig
Atmos. Chem. Phys., 24, 13751–13768, https://doi.org/10.5194/acp-24-13751-2024, https://doi.org/10.5194/acp-24-13751-2024, 2024
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We use a regional climate model, COSMO-CLM², enhanced with a module resolving aerosol processes, to study Antarctic clouds. We prescribe different concentrations of ice-nucleating particles to our model to assess how these clouds respond to concentration changes, validating results with cloud and aerosol observations from the Princess Elisabeth Antarctica station. Our results show that aerosol–cloud interactions vary with temperature, providing valuable insights into Antarctic cloud dynamics.
Yi Li, Xiaoli Liu, and Hengjia Cai
Atmos. Chem. Phys., 24, 13525–13540, https://doi.org/10.5194/acp-24-13525-2024, https://doi.org/10.5194/acp-24-13525-2024, 2024
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The influence of different aerosol modes on cloud processes remains controversial. We modified the aerosol spectra and concentrations to simulate a warm stratiform cloud process in Jiangxi, China, using the WRF-SBM scheme. Research shows that different aerosol spectra have diverse effects on cloud droplet spectra, cloud development, and the correlation between dispersion (ε) and cloud physics quantities. Compared to cloud droplet concentration, ε is more sensitive to the volume radius.
Fabian Hoffmann, Franziska Glassmeier, and Graham Feingold
Atmos. Chem. Phys., 24, 13403–13412, https://doi.org/10.5194/acp-24-13403-2024, https://doi.org/10.5194/acp-24-13403-2024, 2024
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Clouds constitute a major cooling influence on Earth's climate system by reflecting a large fraction of the incident solar radiation back to space. This ability is controlled by the number of cloud droplets, which is governed by the number of aerosol particles in the atmosphere, laying the foundation for so-called aerosol–cloud–climate interactions. In this study, a simple model to understand the effect of aerosol on cloud water is developed and applied.
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