Articles | Volume 21, issue 21
https://doi.org/10.5194/acp-21-16387-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-16387-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
08 Nov 2021
Research article |
| 08 Nov 2021
| 08 Nov 2021
A predictive thermodynamic framework of cloud droplet activation for chemically unresolved aerosol mixtures, including surface tension, non-ideality, and bulk–surface partitioning
University of Oulu, Center for Atmospheric Research, P.O. Box 4500, 90014, University of Oulu, Oulu, Finland
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Atmospheric aerosols act as seeds for cloud formation. Many aerosols contain surface active material that accumulates at the surface of growing droplets. This can affect cloud droplet activation, but the broad significance of the effect and the best way to model it are still debated. We compare predictions of six different model approaches to surface activity of organic aerosols and find significant differences between the models, especially with large fractions of organics in the dry particles.
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Atmospheric particles can release gas molecules as they dry, influencing their chemical composition. We confirm the formation of hydrogen chloride gas from aerosol particles containing mixed NaCl and (NH4)2SO4 by measuring both particle surfaces and gases in-flight using x-rays. Lower humidity increased gas formation, while the aerosol mass had little effect. These findings confirm predictions of how humidity affects particle chemistry and can improve models of atmospheric processes and climate.
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We measure the surface tension of picoliter-volume droplets containing strong ionic surfactants and cosolutes and compare this to surface tension predictions using two independent surfactant partitioning models. Under high-water-activity conditions, experimental measurements and model predictions show no change when NaCl cosolute is replaced with sea salt. Model predictions show that total surfactant concentrations in the range of tens to hundreds of millimolar are required to lower the surface tension of accumulation-mode aerosol.
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The effect of organic acid aerosol on sulfur chemistry and cloud properties was investigated in an atmospheric model. Organic acid dissociation was considered using both bulk and surface-related properties. We found that organic acid dissociation leads to increased hydrogen ion concentrations and sulfate aerosol mass in aqueous aerosols, increasing cloud formation. This could be important in large-scale climate models as many organic aerosol components are both acidic and surface-active.
Sampo Vepsäläinen, Silvia M. Calderón, and Nønne L. Prisle
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Atmospheric aerosols act as seeds for cloud formation. Many aerosols contain surface active material that accumulates at the surface of growing droplets. This can affect cloud droplet activation, but the broad significance of the effect and the best way to model it are still debated. We compare predictions of six models to surface activity of strongly surface active aerosol and find significant differences between the models, especially with large fractions of surfactant in the dry particles.
Minjie Zheng, Hongyu Liu, Florian Adolphi, Raimund Muscheler, Zhengyao Lu, Mousong Wu, and Nønne L. Prisle
Geosci. Model Dev., 16, 7037–7057, https://doi.org/10.5194/gmd-16-7037-2023, https://doi.org/10.5194/gmd-16-7037-2023, 2023
Short summary
Short summary
The radionuclides 7Be and 10Be are useful tracers for atmospheric transport studies. Here we use the GEOS-Chem to simulate 7Be and 10Be with different production rates: the default production rate in GEOS-Chem and two from the state-of-the-art beryllium production model. We demonstrate that reduced uncertainties in the production rates can enhance the utility of 7Be and 10Be as tracers for evaluating transport and scavenging processes in global models.
Sampo Vepsäläinen, Silvia M. Calderón, Jussi Malila, and Nønne L. Prisle
Atmos. Chem. Phys., 22, 2669–2687, https://doi.org/10.5194/acp-22-2669-2022, https://doi.org/10.5194/acp-22-2669-2022, 2022
Short summary
Short summary
Atmospheric aerosols act as seeds for cloud formation. Many aerosols contain surface active material that accumulates at the surface of growing droplets. This can affect cloud droplet activation, but the broad significance of the effect and the best way to model it are still debated. We compare predictions of six different model approaches to surface activity of organic aerosols and find significant differences between the models, especially with large fractions of organics in the dry particles.
Cited articles
Adamson, A. and Gast, A.: Physical Chemistry of Surfaces, John Wiley & Sons,
Inc., sixth edn., 808 pp., 1997. a
Alvarez, N. J., Walker, L. M., and Anna, S. L.: A Microtensiometer To Probe the
Effect of Radius of Curvature on Surfactant Transport to a Spherical
Interface, Langmuir, 26, 13310–13319, https://doi.org/10.1021/la101870m, 2010. a, b
Asa-Awuku, A., Sullivan, A. P., Hennigan, C. J., Weber, R. J., and Nenes, A.: Investigation of molar volume and surfactant characteristics of water-soluble organic compounds in biomass burning aerosol, Atmos. Chem. Phys., 8, 799–812, https://doi.org/10.5194/acp-8-799-2008, 2008. a
Aumann, E., Hildemann, L., and Tabazadeh, A.: Measuring and modeling the
composition and temperature-dependence of surface tension for organic
solutions, Atmos. Environ., 44, 329–337, 1967. a
Bianco, H. and Marmur, A.: The Dependence of the Surface Tension of Surfactant
Solutions on Drop Size, Journal of Colloid and Interface Science, 151,
517–522, 1992. a
Bilde, M. and Svenningsson, B.: CCN Activation of Slightly Soluble Organics:
The Importance of Small Amounts of Inorganic Salt and Particle Phase,
Tellus B, 56, 128–134, 2004. a
Booth, A. M., Topping, D. O., McFiggans, G., and Percival, C. J.: Surface
tension of mixed inorganic and dicarboxylic acid aqueous solutions at 298.15
K and their importance for cloud activation predictions, Phys. Chem. Chem.
Phys., 11, 8021–8028, 2009. a
Cheng, Y., Li, S.-M., Leithead, A., Brickell, P. C., and Leaitch, W. R.:
Characterizations of cis-pinonic acid and n-fatty acids on fine
aerosols in the Lower Fraser Valley during Pacific 2001 Air Quality Study,
Atmos. Environ., 38, 5789–5800, 2004. a
Dillmann, A. and Meier, G. E. A.: A refined droplet approach to the problem of
homogeneous nucleation from the vapor phase, The Journal of Chemical Physics,
94, 3872–3884, https://doi.org/10.1063/1.460663, 1991. a
Dinar, E., Mentel, T. F., and Rudich, Y.: The density of humic acids and humic like substances (HULIS) from fresh and aged wood burning and pollution aerosol particles, Atmos. Chem. Phys., 6, 5213–5224, https://doi.org/10.5194/acp-6-5213-2006, 2006a. a
Dinar, E., Taraniuk, I., Graber, E. R., Katsman, S., Moise, T., Anttila, T., Mentel, T. F., and Rudich, Y.: Cloud Condensation Nuclei properties of model and atmospheric HULIS, Atmos. Chem. Phys., 6, 2465–2482, https://doi.org/10.5194/acp-6-2465-2006, 2006b. a
Facchini, M., Mircea, M., Fuzzi, S., and Charlson, R.: Cloud Albedo
Enhancement by Surface-Active Organic Solutes in Growing Droplets, Nature,
401, 257–259, https://doi.org/10.5194/acp-10-8219-2010, 1999. a, b, c
Facchini, M., Decesari, S., Mircea, M., Fuzzi, S., and Loglio, G.: Surface
Tension of Atmospheric Wet Aerosol and Cloud/Fog Droplets in Relation to
their Organic Carbon Content and Chemical Composition, Atmos. Environ., 34, 4853–4857, 2000. a
Fainerman, V. B., Miller, R., and Möhwald, H.: General Relationships of
the Adsorption Behavior of Surfactants at the Water/Air Interface, J. Phys.
Chem. B, 106, 809–819, 2002. a
Forestieri, S. D., Staudt, S. M., Kuborn, T. M., Faber, K., Ruehl, C. R., Bertram, T. H., and Cappa, C. D.: Establishing the impact of model surfactants on cloud condensation nuclei activity of sea spray aerosol mimics, Atmos. Chem. Phys., 18, 10985–11005, https://doi.org/10.5194/acp-18-10985-2018, 2018. a, b, c, d, e, f, g, h
Frosch, M., Prisle, N. L., Bilde, M., Varga, Z., and Kiss, G.: Joint effect of organic acids and inorganic salts on cloud droplet activation, Atmos. Chem. Phys., 11, 3895–3911, https://doi.org/10.5194/acp-11-3895-2011, 2011. a
Frossard, A. A., Gérard, V., Duplessis, P., Kinsey, J. D., Lu, X., Zhu, Y.,
Bisgrove, J., Maben, J. R., Long, M. S., Chang, R. Y. W., Beaupré, S. R.,
Kieber, D. J., Keene, W. C., Nozière, B., and Cohen, R. C.: Properties
of Seawater Surfactants Associated with Primary Marine Aerosol Particles
Produced by Bursting Bubbles at a Model Air-Sea Interface, Environ. Sci. Technol., 53, 9407–9417, https://doi.org/10.1021/acs.est.9b02637, 2019. a
George, I., Chang, R.-W., Danov, V., Vlasenko, A., and Abbatt, J.: Modification
of cloud condensation nucleus activity of organic aerosols by hydroxyl
radical heterogeneous oxidation, Atmos. Environ., 43, 5038–5045,
https://doi.org/10.1016/j.atmosenv.2009.06.043, 2009. a, b, c, d
Gérard, V., Nozière, B., Baduel, C., Fine, L., Frossard, A. A., and
Cohen, R. C.: Anionic, Cationic, and Nonionic Surfactants in Atmospheric
Aerosols from the Baltic Coast at Askö, Sweden: Implications for Cloud
Droplet Activation, Environ. Sci. Technol., 50, 2974–2982,
https://doi.org/10.1021/acs.est.5b05809, 2016. a, b
Gérard, V., Nozière, B., Fine, L., Ferronato, C., Singh, D. K.,
Frossard, A. A., Cohen, R. C., Asmi, E., Lihavainen, H., Kivekäs, N.,
Aurela, M., Brus, D., Frka, S., and Cvitešić Kušan, A.:
Concentrations and Adsorption Isotherms for Amphiphilic Surfactants in PM1
Aerosols from Different Regions of Europe., Environ. Sci. Technol., 53, 12379–12388, https://doi.org/10.1021/acs.est.9b03386, 2019. a
Gibbs, J., Bumstead, H., Longley, W., and Name, R. V.: The Collected Works of
J. Willard Gibbs, Longmans, Green and Co., 434 pp., 1928. a
Graber, E. R. and Rudich, Y.: Atmospheric HULIS: How humic-like are they? A comprehensive and critical review, Atmos. Chem. Phys., 6, 729–753, https://doi.org/10.5194/acp-6-729-2006, 2006. a
Hansen, A. M. K., Hong, J., Raatikainen, T., Kristensen, K., Ylisirniö, A., Virtanen, A., Petäjä, T., Glasius, M., and Prisle, N. L.: Hygroscopic properties and cloud condensation nuclei activation of limonene-derived organosulfates and their mixtures with ammonium sulfate, Atmos. Chem. Phys., 15, 14071–14089, https://doi.org/10.5194/acp-15-14071-2015, 2015. a, b, c, d, e, f, g, h
Harmon, C., Grimm, R., McIntire, T., Peterson, M., Njegic, B., Angel, V.,
Alshawa, A., Underwood, J., Tobias, D., Gerber, R., Gordon, M., Hemminger,
J., and Nizkorodov, S.: Hygroscopic growth and deliquescence of NaCl
nanoparticles mixed with surfactant SDS, J. Phys. Chem. B,
114, 2435–2449, 2010. a, b, c
Hyvärinen, A.-P., Lihavainen, H., Gaman, A., Vairila, L., Ojala, H.,
Kulmala, M., and Viisanen, Y.: Surface Tensions and Densities of Oxalic,
Malonic, Succinic, Maleic, Malic, and cis-Pinonic Acids, J. Chem. Eng., 51, 255–260, 2006. a
Jenner, G.: High Pressure Kinetic Investigations in Organic and Macromolecular
Chemistry, Angewandte Chemie International Edition in English, 14, 137–143,
https://doi.org/10.1002/anie.197501371, 1975. a
Jin, F., Balasubramaniam, R., and Stebe, K. J.: Surfactant adsorption to
spherical particles: the intrinsic length scale governing the shift from
diffusion to kinetic-controlled mass transfer, The Journal of Adhesion, 80,
773–796, https://doi.org/10.1080/00218460490480770, 2004. a
Jura, G. and Harkins, W. D.: Surfaces of Solids. XIV. A Unitary Thermodynamic
Theory of the Adsorption of Vapors on Solids and of Insoluble Films on Liquid
Subphases, Journal of the American Chemical Society, 68, 1941–1952, 1946. a
Kiss, G. and Hansson, H.-C.: Application of osmolality for the determination of water activity and the modelling of cloud formation, Atmos. Chem. Phys. Discuss., 4, 7667–7689, https://doi.org/10.5194/acpd-4-7667-2004, 2004. a
Kroflič, A., Frka, S., Simmel, M., Wex, H., and Grgić, I.: Size-resolved
surface active substances of atmospheric aerosol: reconsideration of the
impact on cloud droplet formation, Environ. Sci. Technol., 0, 30048123, https://doi.org/10.1021/acs.est.8b02381, 2018. a, b, c
Laaksonen, A.: The Composition Size Dependence of Aerosols Created by
Dispersion of Surfactant Solutions, Journal of Colloid and Interface
Science, 159, 517–519, 1993. a
Laaksonen, A. and Kulmala, M.: An explicit cluster model for binary nuclei in
water-alcohol systems, The Journal of Chemical Physics, 95,
6745–6748, 1991. a
Lee, B.-B., Chan, E.-S., Ravindra, P., and Khan, T. A.: Surface tension of
viscous biopolymer solutions measured using the du Nouy ring method and the
drop weight methods, Polymer Bulletin, 69, 471–489, 2012. a
Low, R.: A Theoretical Study of Nineteen Condensation Nuclei, Journal de
Recherches Atmospheriques, 65–78, 1969. a
Meissner, H. P. and Michaels, A. S.: Surface Tensions of Pure Liquids and
Liquid Mixtures, Industrial & Engineering Chemistry, 41, 2782–2787,
https://doi.org/10.1021/ie50480a028, 1949. a
Mochida, M., Kitamori, Y., Kawamura, K., Nojiri, Y., and Suzuki, K.: Fatty
acids in the marine atmosphere: Factors governing their concentrations and
evaluation of organic films on sea-salt particles, J. Geophys. Res., 107, D17S4325, https://doi.org/10.1029/2001JD001278, 2002. a
Mochida, M., Kawamura, K., Umemoto, N., Kobayashi, M., Matsunaga, S., Lim,
H.-J., Turpin, B., Bates, T., and Simoneit, B.: Spatial distributions of
oxygenated organic compounds (dicarboxylic acids, fatty acids, and
levoglucosan) in marine aerosols over the western Pacific and off the coast
of East Asia: Continental outflow of organic aerosols during the ACE-Asia
campaign, J. Geophys. Res., 108, D23S8638,
https://doi.org/10.1029/2002JD003249, 2003. a
Nguyen, Q. T., Kristensen, T. B., Hansen, A. M. K., Skov, H., Bossi, R.,
Massling, A., Sørensen, L. L., Bilde, M., Glasius, M., and Nøjgaard, J. K.:
Characterization of humic-like substances in Arctic aerosols, J. Geophys. Res.-Atmos,, 119, 5011–5027,
https://doi.org/10.1002/2013JD020144, 2014. a
Noziere, B., Baduel, C., and Jaffrezo, J.-L.: The dynamic surface tension of
atmospheric aerosol surfactants reveals new aspectsof cloud activation,
Nat. Commun., 5, 1–7, 2014. a
Öhrwall, G., Prisle, N. L., Ottosson, N., Werner, J., Ekholm, V., Walz,
M.-M., and Björneholm, O.: Acid-Base Speciation of
Carboxylate Ions in the Surface Region of Aqueous Solutions in the Presence
of Ammonium and Aminium Ions, The Journal of Physical Chemistry B, 119,
4033–4040, 2015. a
Ovadnevaite, J., Zuend, A., Laaksonen, A., Sanchez, K. J., Roberts, G.,
Ceburnis, D., Decesari, S., Rinaldi, M., Hodas, N., Facchini, M. C.,
Seinfeld, J. H., and O' Dowd, C.: Surface tension prevails over solute
effect in organic-influenced cloud droplet activation, Nature, 546,
637–641, 2017. a, b, c, d, e, f, g, h, i, j, k, l
Petters, M. D. and Kreidenweis, S. M.: A single parameter representation of hygroscopic growth and cloud condensation nucleus activity – Part 3: Including surfactant partitioning, Atmos. Chem. Phys., 13, 1081–1091, https://doi.org/10.5194/acp-13-1081-2013, 2013. a, b
Petters, M. D. and Kreidenweis, S. M.: A single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. Phys., 7, 1961–1971, https://doi.org/10.5194/acp-7-1961-2007, 2007. a, b
Poulain, L., Wu, Z., Petters, M. D., Wex, H., Hallbauer, E., Wehner, B., Massling, A., Kreidenweis, S. M., and Stratmann, F.: Towards closing the gap between hygroscopic growth and CCN activation for secondary organic aerosols – Part 3: Influence of the chemical composition on the hygroscopic properties and volatile fractions of aerosols, Atmos. Chem. Phys., 10, 3775–3785, https://doi.org/10.5194/acp-10-3775-2010, 2010. a
Prisle, N. L., Raatikainen, T., Sorjamaa, R., Svenningsson, B., Laaksonen, A.,
and Bilde, M.: Surfactant partitioning in cloud droplet activation: a study
of C8, C10, C12 and C14 normal fatty acid sodium salts, Tellus B, 60,
416–431, https://doi.org/10.1111/j.1600-0889.2008.00352.x, 2008. a, b, c, d, e, f, g, h, i, j, k, l
Prisle, N. L., Asmi, A., Topping, D., Partanen, A.-I., Romakkaniemi, S.,
Dal Maso, M., Kulmala, M., Laaksonen, A., Lehtinen, K. E. J., McFiggans,
G., and Kokkola, H.: Surfactant effects in global simulations of cloud
droplet activation., Geophys. Res. Lett., 39, L05802,
https://doi.org/10.1029/2011GL050467, 2012a. a, b, c, d, e, f
Prisle, N. L., Ottosson, N., Öhrwall, G., Söderström, J., Dal Maso, M., and Björneholm, O.: Surface/bulk partitioning and acid/base speciation of aqueous decanoate: direct observations and atmospheric implications, Atmos. Chem. Phys., 12, 12227–12242, https://doi.org/10.5194/acp-12-12227-2012, 2012b. a, b
Pruppacher, H. R. and Jaenicke, R.: The processing of water vapor and aerosols
by atmospheric clouds, a global estimate, Atmos. Res., 38,
283–295, 1995. a
Raatikainen, T. and Laaksonen, A.: A simplified treatment of surfactant effects on cloud drop activation, Geosci. Model Dev., 4, 107–116, https://doi.org/10.5194/gmd-4-107-2011, 2011. a, b, c, d
Rood, M. J. and Williams, A. L.: Reply, J. Atmos. Sci.,
58, 1468–1473, 2001. a
Ruehl, C. R., Chuang, P. Y., and Nenes, A.: Aerosol hygroscopicity at high (99 to 100 %) relative humidities, Atmos. Chem. Phys., 10, 1329–1344, https://doi.org/10.5194/acp-10-1329-2010, 2010. a
Topping, D.: An analytical solution to calculate bulk mole fractions for any number of components in aerosol droplets after considering partitioning to a surface layer, Geosci. Model Dev., 3, 635–642, https://doi.org/10.5194/gmd-3-635-2010, 2010. a
Tsui, W. G. and McNeill, V. F.: Modeling Secondary Organic Aerosol Production
from Photosensitized Humic-like Substances (HULIS), Environ. Sci. Tech. Lett., 5, 255–259, https://doi.org/10.1021/acs.estlett.8b00101, 2018. a
Tu, P. and Johnston, M. V.: Particle size dependence of biogenic secondary organic aerosol molecular composition, Atmos. Chem. Phys., 17, 7593–7603, https://doi.org/10.5194/acp-17-7593-2017, 2017. a
Vanhanen, J., Hyvärinen, A.-P., Anttila, T., Raatikainen, T., Viisanen, Y., and Lihavainen, H.: Ternary solution of sodium chloride, succinic acid and water; surface tension and its influence on cloud droplet activation, Atmos. Chem. Phys., 8, 4595–4604, https://doi.org/10.5194/acp-8-4595-2008, 2008. a, b
Varga, Z., Kiss, G., and Hansson, H.-C.: Modelling the cloud condensation nucleus activity of organic acids on the basis of surface tension and osmolality measurements, Atmos. Chem. Phys., 7, 4601–4611, https://doi.org/10.5194/acp-7-4601-2007, 2007. a
Vepsäläinen, S., Calderón, S. M., Malila, J., and Prisle, N. L.: Droplet activation of moderately surface active organic aerosol predicted with six approaches to surface activity, Atmos. Chem. Phys. Discuss. [preprint], https://doi.org/10.5194/acp-2021-561, in review, 2021. a
Walz, M.-M., Werner, J., Ekholm, V., Prisle, N. L., Ohrwall, G., and
Bjorneholm, O.: Alcohols at the aqueous surface: chain length and isomer
effects, Phys. Chem. Chem. Phys., 18, 6648–6656, https://doi.org/10.1039/C5CP06463E,
2016. a
Werner, J., Julin, J., Dalirian, M., Prisle, N. L., Öhrwall, G., Persson,
I., Björneholm, O., and Riipinen, I.: Succinic acid in aqueous solution:
connecting microscopic surface composition and macroscopic surface tension,
Phys. Chem. Chem. Phys., 16, 21486–21495, https://doi.org/10.1039/C4CP02776K, 2014.
a
Werner, J., Persson, I., Björneholm, O., Kawecki, D., Saak, C.-M., Walz,
M.-M., Ekholm, V., Unger, I., Valtl, C., Caleman, C., Öhrwall, G., and
Prisle, N. L.: Shifted equilibria of organic acids and bases in the aqueous
surface region, Phys. Chem. Chem. Phys., 20, 23281–23293,
2018. a
Wex, H., Hennig, T., Salma, I., Ocskay, R., Kiselev, A., Henning, S., Massling,
A., Wiedensohler, A., and Stratmann, F.: Hygroscopic growth and measured and
modeled critical supersaturations of an atmospheric HULIS sample,
Geophys. Res. Lett., 34, L02818, https://doi.org/10.1029/2006GL028260, 2007. a
Winkler, P. M., Ortega, J., Karl, T., Cappellin, L., Friedli, H. R., Barsanti,
K., McMurry, P. H., and Smith, J. N.: Identification of the biogenic
compounds responsible for size-dependent nanoparticle growth, Geophys. Res. Lett., 39, https://doi.org/10.1029/2012GL053253, 2012. a
Yassaa, N., Meklati, B. Y., Cecinato, A., and Marino, F.: Particulate
n-alkanes, n-alkanoic acids and polycyclic aromatic hydrocarbons in the
atmosphere of Algiers City Area, Atmos. Environ., 35, 1843–1851,
2001. a
Zamora, I. R. and Jacobson, M. Z.: Measuring and modeling the hygroscopic growth of two humic substances in mixed aerosol particles of atmospheric relevance, Atmos. Chem. Phys., 13, 8973–8989, https://doi.org/10.5194/acp-13-8973-2013, 2013. a, b
Short summary
A mass-based Gibbs adsorption model is presented to enable predictive Köhler calculations of droplet growth and activation with considerations of surface partitioning, surface tension, and non-ideal water activity for chemically complex and unresolved surface active aerosol mixtures, including actual atmospheric samples. The model is used to calculate cloud condensation nuclei (CCN) activity of aerosol particles comprising strongly surface-active model atmospheric humic-like substances (HULIS).
A mass-based Gibbs adsorption model is presented to enable predictive Köhler calculations of...
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