Articles | Volume 18, issue 10
Research article 25 May 2018
Research article | 25 May 2018
Competition for water vapour results in suppression of ice formation in mixed-phase clouds
Emma L. Simpson et al.
E. Simpson, P. Connolly, and G. McFiggans
Geosci. Model Dev., 7, 1535–1542,
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,Short summary
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.
Rachel L. James, Vaughan T. J. Phillips, and Paul J. Connolly
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
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 forming 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.
Yunqi Shao, Yu Wang, Mao Du, Aristeidis Voliotis, M. Rami Alfarra, S. Fiona Turner, and Gordon McFiggans
Atmos. Meas. Tech. Discuss.,
Preprint under review for AMTShort summary
This study describes the design and characterization of the Manchester Aerosol Chamber (MAC). MAC has good temperature and RH homogeneity, fast mixing times and comparable losses of gases and particles with other chambers. We also investigate the effect of contamination on chamber performance and we explore the SOA mass changes after applying various wall-loss correction methods. Our results highlight the need for tracking chamber performance by conducting regular characterization experiments.
Jessica Slater, Hugh Coe, Gordon McFiggans, Juha Tonttila, and Sami Romakkaniemi
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
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 Beijing haze episodes.
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. Discuss.,
Revised manuscript under review for ACPShort summary
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 are more oxygenated and less volatile than those from either precursor. Analytical context is provided to explore the SOA volatility in mixtures.
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,Short summary
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,Short summary
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.
Jessica Slater, Juha Tonttila, Gordon McFiggans, Paul Connolly, Sami Romakkaniemi, Thomas Kühn, and Hugh Coe
Atmos. Chem. Phys., 20, 11893–11906,Short summary
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.
Ernesto Reyes-Villegas, Upasana Panda, Eoghan Darbyshire, James M. Cash, Rutambhara Joshi, Ben Langford, Chiara F. Di Marco, Neil Mullinger, 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, Shivani, Ranu Gadi, Siddhartha Singh, Vijay Soni, and James D. Allan
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
The work presented in this manuscript shows the first multisite online measurements of PM1 in Delhi, India. It covers measurements over different seasons in Old and New Delhi during 2018. OA source apportionment was performed using PMF. Traffic showed to be the main primary aerosol source for both OA and BC, as seen with the PMF analysis and aethalometer model analysis. This indicates that in Delhi control of primary traffic exhaust emissions would make a significant reduction to air pollution.
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,Short summary
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,Short summary
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.
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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.
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,Short summary
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.
Dawei Hu, David Topping, and Gordon McFiggans
Atmos. Chem. Phys., 18, 14925–14937,Short summary
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,Short summary
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,Short summary
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,Short summary
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.
Wiebke Frey, Dawei Hu, James Dorsey, M. Rami Alfarra, Aki Pajunoja, Annele Virtanen, Paul Connolly, and Gordon McFiggans
Atmos. Chem. Phys., 18, 9393–9409,Short summary
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.
Kathryn Fowler, Paul J. Connolly, David O. Topping, and Simon O'Meara
Atmos. Chem. Phys., 18, 1629–1642,Short summary
This is the first time the Maxwell–Stefan framework has been applied to an atmospheric aerosol core–shell model and shows that there is a complex interplay between the viscous and solubility effects on aerosol composition. Understanding aerosol composition is essential to accurately model their interactions within atmospheric systems. We use simple binary systems to demonstrate how viscosity and solubility both play a role in affecting the rate of diffusion through aerosol particles.
Gillian Young, Paul J. Connolly, Christopher Dearden, and Thomas W. Choularton
Atmos. Chem. Phys., 18, 1475–1494,Short summary
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,Short summary
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.
Simon O'Meara, David O. Topping, Rahul A. Zaveri, and Gordon McFiggans
Atmos. Chem. Phys., 17, 10477–10494,Short summary
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,Short summary
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.
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,
Gillian Young, Paul J. Connolly, Hazel M. Jones, and Thomas W. Choularton
Atmos. Chem. Phys., 17, 4209–4227,Short summary
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.
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,Short summary
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,Short summary
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,Short summary
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.
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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.
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,
J. D. Whitehead, M. Irwin, J. D. Allan, N. Good, and G. McFiggans
Atmos. Chem. Phys., 14, 11833–11841,Short summary
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,
M. J. Lawler, J. Whitehead, C. O'Dowd, C. Monahan, G. McFiggans, and J. N. Smith
Atmos. Chem. Phys., 14, 11557–11569,Short summary
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,
P. J. Connolly, D. O. Topping, F. Malavelle, and G. McFiggans
Atmos. Chem. Phys., 14, 2289–2302,
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,
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,
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,
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,
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,
Related subject area
Subject: Clouds and Precipitation | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)Ice multiplication from ice–ice collisions in the high Arctic: sensitivity to ice habit, rimed fraction, ice type and uncertainties in the numerical description of the processThe climate impact of COVID-19-induced contrail changesA large-eddy simulation study of deep-convection initiation through the collision of two sea-breeze frontsSoot PCF: pore condensation and freezing framework for soot aggregatesAir traffic and contrail changes over Europe during COVID-19: a model studyIs a more physical representation of aerosol activation needed for simulations of fog?Microphysical processes producing high ice water contents (HIWCs) in tropical convective clouds during the HAIC-HIWC field campaign: evaluation of simulations using bulk microphysical schemesImpacts of secondary ice production on Arctic mixed-phase clouds based on ARM observations and CAM6 single-column model simulationsThe temperature dependence of ice-nucleating particle concentrations affects the radiative properties of tropical convective cloud systemsThe behavior of high-CAPE (convective available potential energy) summer convection in large-domain large-eddy simulations with ICONImpact of high and low vorticity turbulence on cloud environment mixing and cloud microphysics processesCloud droplet diffusional growth in homogeneous isotropic turbulence: bin microphysics versus Lagrangian super-droplet simulationsThe importance of Aitken mode aerosol particles for cloud sustenance in the summertime high Arctic – a simulation study supported by observational dataAitken mode particles as CCN in aerosol- and updraft-sensitive regimes of cloud droplet formationSensitivity of mixed-phase moderately deep convective clouds to parameterizations of ice formation – an ensemble perspectiveShallow cumulus cloud feedback in large eddy simulations – bridging the gap to storm-resolving modelsUnderstanding the model representation of clouds based on visible and infrared satellite observationsImpacts of cloud microphysics parameterizations on simulated aerosol–cloud interactions for deep convective clouds over HoustonPreconditioning of overcast-to-broken cloud transitions by riming in marine cold air outbreaksCold cloud microphysical process rates in a global chemistry–climate modelPrecipitation enhancement in stratocumulus clouds through airborne seeding: sensitivity analysis by UCLALES-SALSASecondary ice production in summer clouds over the Antarctic coast: an underappreciated process in atmospheric modelsOpinion: Cloud-phase climate feedback and the importance of ice-nucleating particlesOn the ice-nucleating potential of warm hydrometeors in mixed-phase cloudsThe enhancement of droplet collision by electric charges and atmospheric electric fieldsCloud adjustments dominate the overall negative aerosol radiative effects of biomass burning aerosols in UKESM1 climate model simulations over the south-eastern AtlanticDependence of predictability of precipitation in the northwestern Mediterranean coastal region on the strength of synoptic controlThe decomposition of cloud–aerosol forcing in the UK Earth System Model (UKESM1)Sensitivity of warm clouds to large particles in measured marine aerosol size distributions – a theoretical studyHectometric-scale simulations of a Mediterranean heavy-precipitation event during the Hydrological cycle in the Mediterranean Experiment (HyMeX) first Special Observation Period (SOP1)Urbanization-induced land and aerosol impacts on sea-breeze circulation and convective precipitationSnow-induced buffering in aerosol–cloud interactionsEnvironmental sensitivities of shallow-cumulus dilution – Part 1: Selected thermodynamic conditionsEmploying airborne radiation and cloud microphysics observations to improve cloud representation in ICON at kilometer-scale resolution in the ArcticAn idealized model sensitivity study on Dead Sea desertification with a focus on the impact on convectionModelling mixed-phase clouds with the large-eddy model UCLALES–SALSADevelopment of aerosol activation in the double-moment Unified Model and evaluation with CLARIFY measurementsSize dependence in chord characteristics from simulated and observed continental shallow cumulusImpact of aerosols and turbulence on cloud droplet growth: an in-cloud seeding case study using a parcel–DNS (direct numerical simulation) approachDiffusional growth of cloud droplets in homogeneous isotropic turbulence: DNS, scaled-up DNS, and stochastic modelDifferences in tropical high clouds among reanalyses: origins and radiative impactsVertical redistribution of moisture and aerosol in orographic mixed-phase cloudsImproving the Southern Ocean cloud albedo biases in a general circulation modelEvaluation of Southern Ocean cloud in the HadGEM3 general circulation model and MERRA-2 reanalysis using ship-based observationsEnsemble daily simulations for elucidating cloud–aerosol interactions under a large spread of realistic environmental conditionsAerosol indirect effects on the temperature–precipitation scalingThe vertical structure and spatial variability of lower-tropospheric water vapor and clouds in the tradesDetection and attribution of aerosol–cloud interactions in large-domain large-eddy simulations with the ICOsahedral Non-hydrostatic modelTo what extents do urbanization and air pollution affect fog?The effects of cloud–aerosol interaction complexity on simulations of presummer rainfall over southern China
Georgia Sotiropoulou, Luisa Ickes, Athanasios Nenes, and Annica M. L. Ekman
Atmos. Chem. Phys., 21, 9741–9760,Short summary
Mixed-phase clouds are a large source of uncertainty in projections of the Arctic climate. This is partly due to the poor representation of the cloud ice formation processes. Implementing a parameterization for ice multiplication due to mechanical breakup upon collision of two ice particles in a high-resolution model improves cloud ice phase representation; however, cloud liquid remains overestimated.
Andrew Gettelman, Chieh-Chieh Chen, and Charles G. Bardeen
Atmos. Chem. Phys., 21, 9405–9416,Short summary
The COVID-19 pandemic caused significant economic disruption in 2020 and severely impacted air traffic. We use a climate model to evaluate the effect of the reductions in aviation on climate in 2020. Contrails, in general, warm the planet, and COVID-19-related reductions in contrails cooled the land surface in 2020. The timing of reductions in aviation was important, and this may change how we think about the future effects of contrails.
Shizuo Fu, Richard Rotunno, Jinghua Chen, Xin Deng, and Huiwen Xue
Atmos. Chem. Phys., 21, 9289–9308,Short summary
Deep-convection initiation (DCI) determines when and where deep convection develops and hence affects both weather and climate. However, our understanding of DCI is still limited. Here, we simulate DCI over a peninsula using large-eddy simulation and high-output frequency. We find that DCI is accomplished through the development of multiple generations of convection, and the earlier generation affects the later generation by producing downdrafts and cold pools.
Claudia Marcolli, Fabian Mahrt, and Bernd Kärcher
Atmos. Chem. Phys., 21, 7791–7843,Short summary
Pores are aerosol particle features that trigger ice nucleation, as they take up water by capillary condensation below water saturation that freezes at low temperatures. The pore ice can then grow into macroscopic ice crystals making up cirrus clouds. Here, we investigate the pores in soot aggregates responsible for pore condensation and freezing (PCF). Moreover, we present a framework to parameterize soot PCF that is able to predict the ice nucleation activity based on soot properties.
Ulrich Schumann, Ian Poll, Roger Teoh, Rainer Koelle, Enrico Spinielli, Jarlath Molloy, George S. Koudis, Robert Baumann, Luca Bugliaro, Marc Stettler, and Christiane Voigt
Atmos. Chem. Phys., 21, 7429–7450,Short summary
The roughly 70 % reduction of air traffic during the COVID-19 pandemic from March–August 2020 compared to 2019 provides a test case for the relationship between air traffic density, contrails, and their radiative forcing of climate change. This paper investigates the induced traffic and contrail changes in a model study. Besides strong weather changes, the model results indicate aviation-induced cirrus and top-of-the-atmosphere irradiance changes, which can be tested with observations.
Craig Poku, Andrew N. Ross, Adrian A. Hill, Alan M. Blyth, and Ben Shipway
Atmos. Chem. Phys., 21, 7271–7292,Short summary
We present a new aerosol activation scheme suitable for modelling both fog and convective clouds. Most current activation schemes are designed for convective clouds, and we demonstrate that using them to model fog can negatively impact its life cycle. Our scheme has been used to model an observed fog case in the UK, where we demonstrate that a more physically based representation of aerosol activation is required to capture the transition to a deeper layer – more in line with observations.
Yongjie Huang, Wei Wu, Greg M. McFarquhar, Xuguang Wang, Hugh Morrison, Alexander Ryzhkov, Yachao Hu, Mengistu Wolde, Cuong Nguyen, Alfons Schwarzenboeck, Jason Milbrandt, Alexei V. Korolev, and Ivan Heckman
Atmos. Chem. Phys., 21, 6919–6944,Short summary
Numerous small ice crystals in the tropical convective storms are difficult to detect and could be potentially hazardous for commercial aircraft. This study evaluated the numerical models against the airborne observations and investigated the potential cloud processes that could lead to the production of these large numbers of small ice crystals. It is found that key microphysical processes are still lacking or misrepresented in current numerical models to realistically simulate the phenomenon.
Xi Zhao, Xiaohong Liu, Vaughan T. J. Phillips, and Sachin Patade
Atmos. Chem. Phys., 21, 5685–5703,Short summary
Arctic mixed-phase clouds significantly influence the energy budget of the Arctic. We show that a climate model considering secondary ice production (SIP) can explain the observed cloud ice number concentrations, vertical distribution pattern, and probability density distribution of ice crystal number concentrations. The mixed-phase cloud occurrence and phase partitioning are also improved.
Rachel E. Hawker, Annette K. Miltenberger, Jonathan M. Wilkinson, Adrian A. Hill, Ben J. Shipway, Zhiqiang Cui, Richard J. Cotton, Ken S. Carslaw, Paul R. Field, and Benjamin J. Murray
Atmos. Chem. Phys., 21, 5439–5461,Short summary
The impact of aerosols on clouds is a large source of uncertainty for future climate projections. Our results show that the radiative properties of a complex convective cloud field in the Saharan outflow region are sensitive to the temperature dependence of ice-nucleating particle concentrations. This means that differences in the aerosol source or composition, for the same aerosol size distribution, can cause differences in the outgoing radiation from regions dominated by tropical convection.
Harald Rybka, Ulrike Burkhardt, Martin Köhler, Ioanna Arka, Luca Bugliaro, Ulrich Görsdorf, Ákos Horváth, Catrin I. Meyer, Jens Reichardt, Axel Seifert, and Johan Strandgren
Atmos. Chem. Phys., 21, 4285–4318,Short summary
Estimating the impact of convection on the upper-tropospheric water budget remains a problem for models employing resolutions of several kilometers or more. A sub-kilometer high-resolution model is used to study summertime convection. The results suggest mostly close agreement with ground- and satellite-based observational data while slightly overestimating total frozen water path and anvil lifetime. The simulations are well suited to supplying information for parameterization development.
Bipin Kumar, Rahul Ranjan, Man-Kong Yau, Sudarsan Bera, and Suryachadra A. Rao
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
The characteristics of turbulent clouds are affected by the entrainment of ambient dry air and its subsequent mixing. A turbulent flow generates vorticities of different intensities and regions with high vorticity (HV) and low vorticity (LV) exist. This study provides a detailed analysis of different properties of turbulent flows and cloud droplets in the HV and LV regions to understand the impact of vorticity production on cloud microphysical and mixing processes.
Wojciech W. Grabowski and Lois Thomas
Atmos. Chem. Phys., 21, 4059–4077,Short summary
This paper presents a modeling study that investigates the impact of cloud turbulence on the diffusional growth of cloud droplets and compares modeling results to analytic solutions published in the past. The focus is on comparing the two microphysics modeling methodologies – the Eulerian bin microphysics and Lagrangian particle-based microphysics – and exposing their limitations.
Ines Bulatovic, Adele L. Igel, Caroline Leck, Jost Heintzenberg, Ilona Riipinen, and Annica M. L. Ekman
Atmos. Chem. Phys., 21, 3871–3897,Short summary
We use detailed numerical modelling to show that small aerosol particles (diameters ~25–80 nm; so-called Aitken mode particles) significantly influence low-level cloud properties in the clean summertime high Arctic. The small particles can help sustain clouds when the concentration of larger particles is low (<10–20 cm-3). Measurements from four different observational campaigns in the high Arctic support the modelling results as they indicate that Aitken mode aerosols are frequently activated.
Mira L. Pöhlker, Minghui Zhang, Ramon Campos Braga, Ovid O. Krüger, Ulrich Pöschl, and Barbara Ervens
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Clouds cool our atmosphere. The role of small aerosol particles in affecting them represent one of the largest uncertainties in current estimates of climate change. Traditionally it is assumed that cloud droplets form only particles of diameters ~100 nm (
accumulation mode). Previous studies suggest that this can also occur on smaller particles (
Aitken mode). Our study provides a general framework to estimate under which aerosol and cloud conditions Aitken mode particles affect clouds.
Annette K. Miltenberger and Paul R. Field
Atmos. Chem. Phys., 21, 3627–3642,Short summary
The formation of ice in clouds is an important processes in mixed-phase and ice-phase clouds. However, the representation of ice formation in numerical models is highly uncertain. In the last decade, several new parameterizations for heterogeneous freezing have been proposed. Here, we investigate the impact of the parameterization choice on the representation of the convective cloud field and compare the impact to that of initial condition uncertainty.
Jule Radtke, Thorsten Mauritsen, and Cathy Hohenegger
Atmos. Chem. Phys., 21, 3275–3288,Short summary
Shallow trade wind clouds are a key source of uncertainty to projections of the Earth's changing climate. We perform high-resolution simulations of trade cumulus and investigate how the representation and climate feedback of these clouds depend on the specific grid spacing. We find that the cloud feedback is positive when simulated with kilometre but near zero when simulated with hectometre grid spacing. These findings suggest that storm-resolving models may exaggerate the trade cloud feedback.
Stefan Geiss, Leonhard Scheck, Alberto de Lozar, and Martin Weissmann
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
The present study facilitates a novel approach based on both visible and infrared satellite observations to evaluate and improve the representation of clouds and radiation in climate and numerical weather prediction (NWP) models. The combination of observations in these two spectral ranges provides significantly more and complementary information than the use of only infrared observations pursued in previous studies.
Yuwei Zhang, Jiwen Fan, Zhanqing Li, and Daniel Rosenfeld
Atmos. Chem. Phys., 21, 2363–2381,Short summary
Impacts of anthropogenic aerosols on deep convective clouds (DCCs) and precipitation are examined using both the Morrison bulk and spectral bin microphysics (SBM) schemes. With the SBM scheme, anthropogenic aerosols notably invigorate convective intensity and precipitation, causing better agreement between the simulated DCCs and observations; this effect is absent with the Morrison scheme, mainly due to limitations of the saturation adjustment approach for droplet condensation and evaporation.
Florian Tornow, Andrew S. Ackerman, and Ann M. Fridlind
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Cold air outbreaks affect the local energy budget by forming bright boundary layer clouds that, once raining, evolve into dimmer, broken cloud fields that are depleted of condensation nuclei – an evolution consistent with closed-to-open cell transitions. We find that cloud ice accelerates this evolution, primarily via riming prior to rain onset, which (1) reduces liquid water, (2) reduces condensation nuclei, and (3) leads to early precipitation cooling and moistening below cloud.
Sara Bacer, Sylvia C. Sullivan, Odran Sourdeval, Holger Tost, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 21, 1485–1505,Short summary
We investigate the relative importance of the rates of both microphysical processes and unphysical correction terms that act as sources or sinks of ice crystals in cold clouds. By means of numerical simulations performed with a global chemistry–climate model, we assess the relevance of these rates at global and regional scales. This estimation is of fundamental importance to assign priority to the development of microphysics parameterizations and compare model output with observations.
Juha Tonttila, Ali Afzalifar, Harri Kokkola, Tomi Raatikainen, Hannele Korhonen, and Sami Romakkaniemi
Atmos. Chem. Phys., 21, 1035–1048,Short summary
The focus of this study is on rain enhancement by deliberate injection of small particles into clouds (
cloud seeding). The particles, usually released from an aircraft, are expected to enhance cloud droplet growth, but its practical feasibility is somewhat uncertain. To improve upon this, we simulate the seeding effects with a numerical model. The model reproduces the main features seen in field observations, with a strong sensitivity to the total mass of the injected particle material.
Georgia Sotiropoulou, Étienne Vignon, Gillian Young, Hugh Morrison, Sebastian J. O'Shea, Thomas Lachlan-Cope, Alexis Berne, and Athanasios Nenes
Atmos. Chem. Phys., 21, 755–771,Short summary
Summer clouds have a significant impact on the radiation budget of the Antarctic surface and thus on ice-shelf melting. However, these are poorly represented in climate models due to errors in their microphysical structure, including the number of ice crystals that they contain. We show that breakup from ice particle collisions can substantially magnify the ice crystal number concentration with significant implications for surface radiation. This process is currently missing in climate models.
Benjamin J. Murray, Kenneth S. Carslaw, and Paul R. Field
Atmos. Chem. Phys., 21, 665–679,Short summary
The balance between the amounts of ice and supercooled water in clouds over the world's oceans strongly influences how much these clouds can dampen or amplify global warming. Aerosol particles which catalyse ice formation can dramatically reduce the amount of supercooled water in clouds; hence we argue that we need a concerted effort to improve our understanding of these ice-nucleating particles if we are to improve our predictions of climate change.
Michael Krayer, Agathe Chouippe, Markus Uhlmann, Jan Dušek, and Thomas Leisner
Atmos. Chem. Phys., 21, 561–575,Short summary
We address the phenomenon of ice enhancement in the vicinity of warm hydrometeors using highly accurate flow simulation techniques. It is found that the transiently supersaturated zones induced by the hydrometeor's wake are by far larger than what has been previously estimated. The ice enhancement is quantified on the micro- and macroscale, and its relevance is discussed. The results provided may contribute to a (currently unavailable) parametrization of the phenomenon.
Shian Guo and Huiwen Xue
Atmos. Chem. Phys., 21, 69–85,Short summary
Observations in previous studies show that cloud droplets carry electric charges. We are curious about whether the electric interaction enhances the collision of cloud droplets. The effect of the electric charge and atmospheric electric field on the raindrop-formation process is studied numerically. Results indicate that a cloud with a small droplet size is more sensitive to an electric charge and field, which could significantly trigger droplet collision and accelerate raindrop formation.
Haochi Che, Philip Stier, Hamish Gordon, Duncan Watson-Parris, and Lucia Deaconu
Atmos. Chem. Phys., 21, 17–33,Short summary
The south-eastern Atlantic is semi-permanently covered by some of the largest stratocumulus clouds and is influenced by one-third of the biomass burning emissions from African fires. A UKEMS1 model simulation shows that the absorption effect of biomass burning aerosols is the most significant on clouds and radiation. The dominate cooling and rapid adjustments induced by the radiative effects of biomass burning aerosols result in an overall cooling in the south-eastern Atlantic.
Christian Keil, Lucie Chabert, Olivier Nuissier, and Laure Raynaud
Atmos. Chem. Phys., 20, 15851–15865,Short summary
During strong synoptic control, which dominates the weather on 80 % of the days in the 2-month HyMeX-SOP1 period, the domain-integrated precipitation predictability assessed with the normalized ensemble standard deviation is above average, the wet bias is smaller and the forecast quality is generally better. In contrast, the spatial forecast quality of the most intense precipitation in the afternoon, as quantified with its 95th percentile, is superior during weakly forced synoptic regimes.
Daniel P. Grosvenor and Kenneth S. Carslaw
Atmos. Chem. Phys., 20, 15681–15724,Short summary
Particles arising from human activity interact with clouds and affect how much of the Sun's energy is reflected away. Lack of understanding about how to represent this in models leads to large uncertainties in climate predictions. We quantify cloud responses to particles in the latest UK Met Office climate model over the North Atlantic Ocean, showing that, in contrast to suggestions elsewhere, increases in cloud coverage and thickness are important over large areas.
Tom Dror, J. Michel Flores, Orit Altaratz, Guy Dagan, Zev Levin, Assaf Vardi, and Ilan Koren
Atmos. Chem. Phys., 20, 15297–15306,Short summary
We used in situ aerosol measurements over the Atlantic, Caribbean, and Pacific to initialize a cloud model and study the impact of aerosol concentration and sizes on warm clouds. We show that high aerosol concentration increases cloud mass and reduces surface rain when giant particles (diameter > 9 µm) are present. The large aerosols changed the timing and magnitude of internal cloud processes and resulted in an enhanced evaporation below cloud base and dramatically reduced surface rain.
Olivier Nuissier, Fanny Duffourg, Maxime Martinet, Véronique Ducrocq, and Christine Lac
Atmos. Chem. Phys., 20, 14649–14667,Short summary
This present article demonstrates how numerical simulations with very high horizontal resolution (150 m) can contribute to better understanding the key physical processes (turbulence and microphysics) that lead to Mediterranean heavy precipitation.
Jiwen Fan, Yuwei Zhang, Zhanqing Li, Jiaxi Hu, and Daniel Rosenfeld
Atmos. Chem. Phys., 20, 14163–14182,Short summary
We investigate the urbanization-induced land and aerosol impacts on convective clouds and precipitation over Houston. We find that Houston urbanization notably enhances storm intensity and precipitation, with the anthropogenic aerosol effect more significant. Urban land effect strengthens sea-breeze circulation, leading to a faster development of warm cloud into mixed-phase cloud and earlier rain. The anthropogenic aerosol effect accelerates the development of storms into deep convection.
Takuro Michibata, Kentaroh Suzuki, and Toshihiko Takemura
Atmos. Chem. Phys., 20, 13771–13780,Short summary
This work reveals that prognostic precipitation significantly reduces the magnitude of aerosol–cloud interactions (ERFaci), mainly due to the collection process associated with snowflakes and underlying cloud droplets. This precipitation-driven buffering effect, which is missing in traditional GCMs, can explain the model–observation discrepancy in ERFaci. These results underscore the necessity for a prognostic precipitation framework in GCMs for more reliable climate simulations.
Sonja Drueke, Daniel J. Kirshbaum, and Pavlos Kollias
Atmos. Chem. Phys., 20, 13217–13239,Short summary
This numerical study provides insights into selected environmental sensitivities of shallow-cumulus dilution. Among the parameters under consideration, the dilution of the cloud cores is strongly sensitive to continentality and cloud-layer relative humidity and weakly sensitive to subcloud- and cloud-layer depths. The impacts of all four parameters are interpreted using a similarity theory of shallow cumulus and buoyancy-sorting arguments.
Jan Kretzschmar, Johannes Stapf, Daniel Klocke, Manfred Wendisch, and Johannes Quaas
Atmos. Chem. Phys., 20, 13145–13165,Short summary
This study compares simulations with the ICON model at the kilometer scale to airborne radiation and cloud microphysics observations that have been derived during the ACLOUD aircraft campaign around Svalbard, Norway, in May/June 2017. We find an overestimated surface warming effect of clouds compared to the observations in our setup. This bias was reduced by considering subgrid-scale vertical motion in the activation of cloud condensation nuclei in the two-moment microphysical scheme used.
Samiro Khodayar and Johannes Hoerner
Atmos. Chem. Phys., 20, 12011–12031,
Jaakko Ahola, Hannele Korhonen, Juha Tonttila, Sami Romakkaniemi, Harri Kokkola, and Tomi Raatikainen
Atmos. Chem. Phys., 20, 11639–11654,Short summary
In this study, we present an improved cloud model that reproduces the behaviour of mixed-phase clouds containing liquid droplets and ice crystals in more detail than before. This model is a convenient computational tool that enables the study of phenomena that cannot fit into a laboratory. These clouds have a significant role in climate, but they are not yet properly understood. Here, we show the advantages of the new model in a case study focusing on Arctic mixed-phase clouds.
Hamish Gordon, Paul R. Field, Steven J. Abel, Paul Barrett, Keith Bower, Ian Crawford, Zhiqiang Cui, Daniel P. Grosvenor, Adrian A. Hill, Jonathan Taylor, Jonathan Wilkinson, Huihui Wu, and Ken S. Carslaw
Atmos. Chem. Phys., 20, 10997–11024,Short summary
The Met Office's Unified Model is widely used both for weather forecasting and climate prediction. We present the first version of the model in which both aerosol and cloud particle mass and number concentrations are allowed to evolve separately and independently, which is important for studying how aerosols affect weather and climate. We test the model against aircraft observations near Ascension Island in the Atlantic, focusing on how aerosols can "activate" to become cloud droplets.
Philipp J. Griewank, Thijs Heus, Neil P. Lareau, and Roel A. J. Neggers
Atmos. Chem. Phys., 20, 10211–10230,Short summary
The idea that larger shallow cumulus clouds have stronger updrafts than small shallow cumulus clouds is as intuitive as it is old. In this paper we gather years of upward-pointing laser measurements from a plain in Oklahoma and combine them with 28 d of high-resolution simulations. Our approach, which has much more data than previous studies, confirms that updraft strength and cloud size are linked and that the simulations reproduce the observed cloud wind and moisture structure.
Sisi Chen, Lulin Xue, and Man-Kong Yau
Atmos. Chem. Phys., 20, 10111–10124,Short summary
This study employs a parcel–DNS (direct numerical simulation) modeling framework to accurately resolve the aerosol–droplet–turbulence interactions in an ascending air parcel. The effect of turbulence, aerosol hygroscopicity, and aerosol mass loading on droplet growth and rain formation is investigated through a series of in-cloud seeding experiments in which hygroscopic particles were seeded near the cloud base.
Lois Thomas, Wojciech W. Grabowski, and Bipin Kumar
Atmos. Chem. Phys., 20, 9087–9100,Short summary
This work presents an extension of a classical small-scale modeling approach, direct numerical simulation (DNS), to large computational volumes, tens and hundreds of meters on the side. Diffusional growth of cloud droplets is more significantly affected by large scales of turbulent motions because vertical velocity perturbations associated with those scales result in larger and longer-lasting supersaturation perturbations that affect the spread of the droplet spectrum.
Jonathon S. Wright, Xiaoyi Sun, Paul Konopka, Kirstin Krüger, Bernard Legras, Andrea M. Molod, Susann Tegtmeier, Guang J. Zhang, and Xi Zhao
Atmos. Chem. Phys., 20, 8989–9030,Short summary
High clouds are influential in tropical climate. Although reanalysis cloud fields are essentially model products, they are indirectly constrained by observations and offer global coverage with direct links to advanced water and energy cycle metrics, giving them many useful applications. We describe how high cloud fields are generated in reanalyses, assess their realism and reliability in the tropics, and evaluate how differences in these fields affect other aspects of the reanalysis state.
Annette K. Miltenberger, Paul R. Field, Adrian H. Hill, and Andrew J. Heymsfield
Atmos. Chem. Phys., 20, 7979–8001,Short summary
Orographic wave clouds offer a natural laboratory to investigate cloud microphysical processes and their representation in atmospheric models. They impact the larger-scale flow by a vertical redistribution of moisture and aerosol. We use detailed observations from the ICE-L campaign to evaluate the representation of these clouds in a state-of-the-art numerical weather prediction model and explore the impact of environmental conditions on the vertical redistribution of moisture.
Vidya Varma, Olaf Morgenstern, Paul Field, Kalli Furtado, Jonny Williams, and Patrick Hyder
Atmos. Chem. Phys., 20, 7741–7751,Short summary
The present generation of global climate models has an insufficiently reflected short-wave radiation, especially over the Southern Ocean. This leads to an excessive heating of the ocean surface in the model, creating sea surface temperature biases and subsequent problems with atmospheric dynamics. Misrepresentation of clouds could be attributed to this radiation bias; we try to address this issue by slowing the growth rate of ice crystals and improving the supercooled liquid clouds in the model.
Peter Kuma, Adrian J. McDonald, Olaf Morgenstern, Simon P. Alexander, John J. Cassano, Sally Garrett, Jamie Halla, Sean Hartery, Mike J. Harvey, Simon Parsons, Graeme Plank, Vidya Varma, and Jonny Williams
Atmos. Chem. Phys., 20, 6607–6630,Short summary
We evaluate clouds over the Southern Ocean in the climate model HadGEM3 and reanalysis MERRA-2 using ship-based ceilometer and radiosonde observations. We find the models underestimate cloud cover by 18–25 %, with clouds below 2 km dominant in reality but lacking in the models. We find a strong link between clouds, atmospheric stability and sea surface temperature in observations but not in the models, implying that sub-grid processes do not generate enough cloud in response to these conditions.
Guy Dagan and Philip Stier
Atmos. Chem. Phys., 20, 6291–6303,Short summary
Ensemble daily simulations for two separate month-long periods over a region near Barbados were conducted to investigate aerosol effects on cloud properties and the atmospheric energy budget. For each day, two simulations were conducted with low and high cloud droplet number concentrations representing clean and polluted conditions, respectively. These simulations are used to distinguish between properties that are robustly affected by changes in aerosol concentrations and those that are not.
Nicolas Da Silva, Sylvain Mailler, and Philippe Drobinski
Atmos. Chem. Phys., 20, 6207–6223,Short summary
Microphysical effects of aerosols were found to weaken precipitation in a Euro-Mediterranean area. The present numerical study quantifies the processes that may be involved through the use of the temperature–precipitation relationship. It shows larger aerosol effects at low temperatures. At these temperatures, the process that contributes most is the increase in atmospheric stability through an enhanced aerosol cooling effect in the lower troposphere compared to the upper troposphere.
Ann Kristin Naumann and Christoph Kiemle
Atmos. Chem. Phys., 20, 6129–6145,Short summary
The interaction of water vapor and cloudiness poses challenges for weather and climate models. In this study we compare airborne lidar measurements from two field campaigns in the tropical Atlantic with high-resolution simulations. We find that at kilometer-scale grid spacing, the simulations show good skill in reproducing the water vapor distribution in the trades but struggle to capture the transition from cloud-free to low cloud fraction with increasing moisture.
Montserrat Costa-Surós, Odran Sourdeval, Claudia Acquistapace, Holger Baars, Cintia Carbajal Henken, Christa Genz, Jonas Hesemann, Cristofer Jimenez, Marcel König, Jan Kretzschmar, Nils Madenach, Catrin I. Meyer, Roland Schrödner, Patric Seifert, Fabian Senf, Matthias Brueck, Guido Cioni, Jan Frederik Engels, Kerstin Fieg, Ksenia Gorges, Rieke Heinze, Pavan Kumar Siligam, Ulrike Burkhardt, Susanne Crewell, Corinna Hoose, Axel Seifert, Ina Tegen, and Johannes Quaas
Atmos. Chem. Phys., 20, 5657–5678,Short summary
The impact of anthropogenic aerosols on clouds is a key uncertainty in climate change. This study analyses large-domain simulations with a new high-resolution model to investigate the differences in clouds between 1985 and 2013 comparing multiple observational datasets. The differences in aerosol and in cloud droplet concentrations are clearly detectable. For other quantities, the detection and attribution proved difficult, despite a substantial impact on the Earth's energy budget.
Shuqi Yan, Bin Zhu, Yong Huang, Jun Zhu, Hanqing Kang, Chunsong Lu, and Tong Zhu
Atmos. Chem. Phys., 20, 5559–5572,Short summary
The development of China has caused rapid urbanization and severe air pollution. However, the extent of their individual and combined effects on fog is not well understood. Through numerical experiments, we find that urbanization suppresses low-level fog but probably promotes upper-level fog. Additional aerosols generally promote fog. Urbanization affects fog to a much larger extent than aerosols do.
Kalli Furtado, Paul Field, Yali Luo, Tianjun Zhou, and Adrian Hill
Atmos. Chem. Phys., 20, 5093–5110,Short summary
By combining observations with simulations from a weather forecasting model, new insights are obtained into extreme rainfall processes. We use a model which includes the effects of aerosols on clouds in a fully consistent way. This greater complexity improves realism but raises the computational cost. We address the cost–benefit relationship of this and show that cloud–aerosol interactions have important, measurable benefits for simulating climate extremes.
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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.
This study explores the process of ice formation in clouds by conducting computer model...