Articles | Volume 24, issue 2
https://doi.org/10.5194/acp-24-1467-2024
© Author(s) 2024. 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-24-1467-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
31 Jan 2024
Research article |
| 31 Jan 2024
| 31 Jan 2024
Impact of acidity and surface-modulated acid dissociation on cloud response to organic aerosol
Gargi Sengupta
Center for Atmospheric Research, University of Oulu, P.O. Box 4500, 90014 Oulu, Finland
Minjie Zheng
Center for Atmospheric Research, University of Oulu, P.O. Box 4500, 90014 Oulu, Finland
current affiliation: Institute for Atmospheric and Climate Science, ETH Zurich, Zurich, Switzerland
Center for Atmospheric Research, University of Oulu, P.O. Box 4500, 90014 Oulu, Finland
Related authors
Kunal Ghosh, Suneeti Mishra, and Gargi Sengupta
EGUsphere, https://doi.org/10.5194/egusphere-2026-5224, https://doi.org/10.5194/egusphere-2026-5224, 2026
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Tiny airborne particles can affect clouds, but their natural electrical charge is usually ignored in models. Using simulations of polluted and clean air, we found that charge changes how particles collide, survive, and grow to sizes that can seed cloud droplets. This survival effect increased cloud-forming particles by several percent in both environments, suggesting that particle charge may be a missing part of how aerosols influence clouds and climate.
Kunal Ghosh, Suneeti Mishra, and Gargi Sengupta
EGUsphere, https://doi.org/10.5194/egusphere-2026-5224, https://doi.org/10.5194/egusphere-2026-5224, 2026
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Tiny airborne particles can affect clouds, but their natural electrical charge is usually ignored in models. Using simulations of polluted and clean air, we found that charge changes how particles collide, survive, and grow to sizes that can seed cloud droplets. This survival effect increased cloud-forming particles by several percent in both environments, suggesting that particle charge may be a missing part of how aerosols influence clouds and climate.
Alison Bain, Kunal Ghosh, Konstantin Tumashevich, Nønne L. Prisle, and Bryan R. Bzdek
Atmos. Chem. Phys., 25, 5633–5645, https://doi.org/10.5194/acp-25-5633-2025, https://doi.org/10.5194/acp-25-5633-2025, 2025
Short summary
Short summary
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.
Sampo Vepsäläinen, Silvia M. Calderón, and Nønne L. Prisle
Atmos. Chem. Phys., 23, 15149–15164, https://doi.org/10.5194/acp-23-15149-2023, https://doi.org/10.5194/acp-23-15149-2023, 2023
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 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.
Nønne L. Prisle
Atmos. Chem. Phys., 21, 16387–16411, https://doi.org/10.5194/acp-21-16387-2021, https://doi.org/10.5194/acp-21-16387-2021, 2021
Short summary
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).
Cited articles
Abdul-Razzak, H.: A parameterization of aerosol activation 3. Sectional representation, J. Geophys. Res., 107, 4026, https://doi.org/10.1029/2001jd000483, 2002. a
Abdul-Razzak, H. and Ghan, S. J.: A parameterization of aerosol activation 3. Sectional representation, J. Geophys. Res.-Atmos., 107, AAC–1, 2002. a
Abdul-Razzak, H., Ghan, S. J., and Rivera-Carpio, C.: A parameterization of aerosol activation: 1. Single aerosol type, J. Geophys. Res.-Atmos., 103, 6123–6131, https://doi.org/10.1029/97jd03735, 1998. a
Äijälä, M., Daellenbach, K. R., Canonaco, F., Heikkinen, L., Junninen, H., Petäjä, T., Kulmala, M., Prévôt, A. S. H., and Ehn, M.: Constructing a data-driven receptor model for organic and inorganic aerosol – a synthesis analysis of eight mass spectrometric data sets from a boreal forest site, Atmos. Chem. Phys., 19, 3645–3672, https://doi.org/10.5194/acp-19-3645-2019, 2019. a
Andreae, M. O. and Crutzen, P. J.: Atmospheric aerosols: Biogeochemical sources and role in atmospheric chemistry, Science, 276, 1052–1058, 1997. a
Angelis, M. D., Traversi, R., and Udisti, R.: Long-term trends of mono-carboxylic acids in Antarctica: Comparison of changes in sources and transport processes at the two EPICA deep drilling sites, Tellus B, 64, 17331, https://doi.org/10.3402/TELLUSB.V64I0.17331, 2012. a
Angle, K. J., Crocker, D. R., Simpson, R. M. C., Mayer, K. J., Garofalo, L. A., Moore, A. N., Mora Garcia, S. L., Or, V. W., Srinivasan, S., Farhan, M., Sauer, J. S., Lee, C., Pothier, M. A., Farmer, D. K., Martz, T. R., Bertram, T. H., Cappa, C. D., Prather, K. A., and Grassian, V. H.: Acidity across the interface from the ocean surface to sea spray aerosol, P. Natl. Acad. Sci. USA, 118, e2018397118, https://doi.org/10.1073/pnas.2018397118, 2021. a, b, c
Ault, A. P.: Aerosol Acidity: Novel measurements and implications for atmospheric chemistry, Accounts Chem. Res., 53, 1703–1714, 2020. a
Bruggemann, M., Xu, R., Tilgner, A., Kwong, K. C., Mutzel, A., Poon, H. Y., Otto, T., Schaefer, T., Poulain, L., Chan, M. N., and Herrmann, H.: Organosulfates in ambient aerosol: state of knowledge and future research directions on formation, abundance, fate, and importance, Environ. Sci. Technol., 54, 3767–3782, https://doi.org/10.1021/acs.est.9b06751, 2020. a
Chebbi, A. and Carlier, P.: Carboxylic acids in the troposphere, occurrence, sources, and sinks: A review, Atmos. Environ., 30, 4233–4249, https://doi.org/10.1016/1352-2310(96)00102-1, 1996. a
Chen, Y., Dombek, T., Hand, J., Zhang, Z., Gold, A., Ault, A. P., Levine, K. E., and Surratt, J. D.: Seasonal Contribution of Isoprene-Derived Organosulfates to Total Water-Soluble Fine Particulate Organic Sulfur in the United States, ACS Earth Space Chem., 5, 2419–2432, 2021a. a
Chen, Y., Guo, H., Nah, T., Tanner, D. J., Sullivan, A. P., Takeuchi, M., Gao, Z., Vasilakos, P., Russell, A. G., Baumann, K., Huey, L. G., Weber, R. J., and Ng, N. L.: Low-Molecular-Weight Carboxylic Acids in the Southeastern U.S.: Formation, Partitioning, and Implications for Organic Aerosol Aging, Environ. Sci. Technol., 55, 6688–6699, http://10.1021/ACS.EST.1C01413/ASSET/, 2021b. 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
Cohn, E. J., Heyroth, F. F., and Menkin, M. F.: The Dissociation Constant of Acetic Acid and the Activity Coefficients of the Ions in Certain Acetate Solutions, J. Am. Chem. Soc., 50, 696–714, https://doi.org/10.1021/ja01390a012, 1928. a
Creux, P., Lachaise, J., Graciaa, A., and Beattie, J. K.: Specific cation effects at the hydroxide-charged air/water interface, The J. Phys. Chem. C, 111, 3753–3755, 2007. a
Drexler, C., Elias, H., Fecher, B., and Wannowius, K.: Kinetic investigation of sulfur (IV) oxidation by peroxo compounds R-OOH in aqueous solution, Fresen. J. Anal. Chem., 340, 605–615, 1991. a
Dusek, U., Frank, G., Hildebrandt, L., Curtius, J., Schneider, J., Walter, S., Chand, D., Drewnick, F., Hings, S., Jung, D., Borrmann, S., and Andreae, M. O.: Size matters more than chemistry for cloud-nucleating ability of aerosol particles, Science, 312, 1375–1378, 2006. a
Enami, S., Hoffmann, M. R., and Colussi, A. J.: Proton availability at the air/water interface, The J. Phys. Chem. Lett., 1, 1599–1604, 2010. a
Fankhauser, A. M., Lei, Z., Daley, K. R., Xiao, Y., Zhang, Z., Gold, A., Ault, B. S., Surratt, J. D., and Ault, A. P.: Acidity-Dependent Atmospheric Organosulfate Structures and Spectra: Exploration of Protonation State Effects via Raman and Infrared Spectroscopies Combined with Density Functional Theory, The J. Phys. Chem. A, 126, 5974–5984, 2022. a
Feichter, J., Kjellström, E., Rodhe, H., Dentener, F., Lelieveldi, J., and Roelofs, G.-J.: Simulation of the tropospheric sulfur cycle in a global climate model, Atmos. Environ., 30, 1693–1707, 1996a. a
Feichter, J., Kjellström, E., Rodhe, H., Dentener, F., Lelieveldi, J., and Roelofs, G.-J.: Simulation of the tropospheric sulfur cycle in a global climate model, Atmos. Environ., 30, 1693–1707, https://doi.org/10.1016/1352-2310(95)00394-0, 1996b. a
Freedman, M. A.: Phase separation in organic aerosol, Chem. Soc. Rev., 46, 7694–7705, 2017. a
Freedman, M. A., Ott, E.-J. E., and Marak, K. E.: Role of pH in aerosol processes and measurement challenges, The J. Phys. Chem. A, 123, 1275–1284, 2018. a
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
Gérard, V., Noziere, 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, 2016. a
Gérard, V., Noziere, 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, 2019a. a
Gerard, V., Noziere, 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 Kušan, A. C.: 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, 2019b. a
Goldberg, R. N., Kishore, N., and Lennen, R. M.: Thermodynamic quantities for the ionization reactions of buffers, J. Phys. Chem. Refer. data, 31, 231–370, 2002. a
Gong, K., Ao, J., Li, K., Liu, L., Liu, Y., Xu, G., Wang, T., Cheng, H., Wang, Z., Zhang, X., et al.: Imaging of pH distribution inside individual microdroplet by stimulated Raman microscopy, P. Natl. Acad. Sci. USA, 120, e2219588120, https://doi.org/10.1073/pnas.2219588120, 2023. a
Graciaa, A., Morel, G., Saulner, P., Lachaise, J., and Schechter, R.: The ζ-potential of gas bubbles, J. Colloid Interf. Sci., 172, 131–136, 1995. a
Graham, B., Guyon, P., Taylor, P. E., Artaxo, P., Maenhaut, W., Glovsky, M. M., Flagan, R. C., and Andreae, M. O.: Organic compounds present in the natural Amazonian aerosol: Characterization by gas chromatography–mass spectrometry, J. Geophys. Res.-Atmos., 108, 4766, https://doi.org/10.1029/2003JD003990, 2003. a
Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009. a
HAMMOZ consortium: HAMMOZ redmine repository, https://svn.iac.ethz.ch/external/echam-hammoz/echam6-hammoz/branches/fmi/HAM_box_OpenIFS/ (last access: 15 October 2021), 2021. 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
Hettiyadura, A. P. S., Al-Naiema, I. M., Hughes, D. D., Fang, T., and Stone, E. A.: Organosulfates in Atlanta, Georgia: anthropogenic influences on biogenic secondary organic aerosol formation, Atmos. Chem. Phys., 19, 3191–3206, https://doi.org/10.5194/acp-19-3191-2019, 2019. a
Hudson, J. G. and Da, X.: Volatility and size of cloud condensation nuclei, J. Geophys. Res.-Atmos., 101, 4435–4442, 1996. a
Huebert, B., Bertram, T., Kline, J., Howell, S., Eatough, D., and Blomquist, B.: Measurements of organic and elemental carbon in Asian outflow during ACE-Asia from the NSF/NCAR C-130, J. Geophys. Res.-Atmos., 109, D19S11, https://doi.org/10.1029/2004JD004700, 2004. a
Hung, H.-M., Hsu, M.-N., and Hoffmann, M. R.: Quantification of SO2 oxidation on interfacial surfaces of acidic micro-droplets: Implication for ambient sulfate formation, Environ. Sci. Technol., 52, 9079–9086, 2018. a
IPCC: Climate Change 2013: The Physical Science Basis. Contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Stocker, T. F., Qin, D., Plattner, G.-K., Tignor, M., Allen, S. K., Boschung, J., Nauels, A., Xia, Y., Bex, V., and Midgley, P. M., Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 1535 pp., 2013. a, b
Jacob, D. J.: Chemistry of OH in remote clouds and its role in the production of formic acid and peroxymonosulfate, J. Geophys. Res.-Atmos., 91, 9807–9826, https://doi.org/10.1029/JD091ID09P09807, 1986. a
Jacobson, M. Z.: Fundamentals of Atmospheric Modeling, Cambridge University Press, Cambridge, 2 Edn., ISBN 9780521548656, https://doi.org/10.1017/CBO9781139165389, 2005. a
Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, https://doi.org/10.5194/acp-5-1053-2005, 2005. a, b
Karraker, K. and Radke, C.: Disjoining pressures, zeta potentials and surface tensions of aqueous non-ionic surfactant/electrolyte solutions: theory and comparison to experiment, Adv. Coll. Interf. Sci., 96, 231–264, 2002. a
Kawamura, K., Ng, L. L., and Kaplan, I. R.: Determination of Organic Acids (C1-C10) in the Atmosphere, Motor Exhausts, and Engine Oils, Environ. Sci. Technol., 19, 1082–1086, http://doi.org/10.1021/ES00141A010/ASSET/, 1985. a
Keene, W. C. and Galloway, J. N.: Organic acidity in precipitation of North America, Atmos. Environ. (1967), 18, 2491–2497, https://doi.org/10.1016/0004-6981(84)90020-9, 1984. a
Kokkola, H., Kühn, T., Laakso, A., Bergman, T., Lehtinen, K. E. J., Mielonen, T., Arola, A., Stadtler, S., Korhonen, H., Ferrachat, S., Lohmann, U., Neubauer, D., Tegen, I., Siegenthaler-Le Drian, C., Schultz, M. G., Bey, I., Stier, P., Daskalakis, N., Heald, C. L., and Romakkaniemi, S.: SALSA2.0: The sectional aerosol module of the aerosol–chemistry–climate model ECHAM6.3.0-HAM2.3-MOZ1.0, Geosci. Model Dev., 11, 3833–3863, https://doi.org/10.5194/gmd-11-3833-2018, 2018. a, b
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., 52, 9179–9187, https://doi.org/10.1021/acs.est.8b02381, 2018. a
Lee, L. A., Pringle, K. J., Reddington, C. L., Mann, G. W., Stier, P., Spracklen, D. V., Pierce, J. R., and Carslaw, K. S.: The magnitude and causes of uncertainty in global model simulations of cloud condensation nuclei, Atmos. Chem. Phys., 13, 8879–8914, https://doi.org/10.5194/acp-13-8879-2013, 2013. a
Legg, S.: IPCC, 2021: Climate change 2021-the physical science basis, Interaction, 49, 44–45, 2021. a
Li, Y.-C. and Yu, J. Z.: Simultaneous determination of mono-and dicarboxylic acids, ω-oxo-carboxylic acids, midchain ketocarboxylic acids, and aldehydes in atmospheric aerosol samples, Environ. Sci. Technol., 39, 7616–7624, 2005. a
Liu, Y., Wu, Z., Huang, X., Shen, H., Bai, Y., Qiao, K., Meng, X., Hu, W., Tang, M., and He, L.: Aerosol phase state and its link to chemical composition and liquid water content in a subtropical coastal megacity, Environ. Sci. Technol., 53, 5027–5033, 2019. a
Lohmann, U. and Lesins, G.: Stronger constraints on the anthropogenic indirect aerosol effect, Science, 298, 1012–1015, 2002. a
Maaß, F., Elias, H., and Wannowius, K. J.: Kinetics of the oxidation of hydrogen sulfite by hydrogen peroxide in aqueous solution:: ionic strength effects and temperature dependence, Atmos. Environ., 33, 4413–4419, 1999. a
Margarella, A. M., Perrine, K. A., Lewis, T., Faubel, M., Winter, B., and Hemminger, J. C.: Dissociation of sulfuric acid in aqueous solution: determination of the photoelectron spectral fingerprints of H2SO4, HSO4–, and SO42–in water, The J. Phys. Chem. C, 117, 8131–8137, 2013. a
Masson-Delmotte, V., Zhai, P., Pirani, A., Connors, S. L., Péan, C., Berger, S., Caud, N., Chen, Y., Goldfarb, L., Gomis, M., Huang, M., Leitzell, K., Lonnoy, E., Matthews, J. B. R., Maycock, T. K., Waterfield, T., Yelekçi, O., Yu, R., and Zhou, B.: Climate change 2021: the physical science basis, Contribution of working group I to the sixth assessment report of the intergovernmental panel on climate change, Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 33−144, https://doi.org/10.1017/9781009157896.002, 2021. a
McArdle, J. V. and Hoffmann, M. R.: Kinetics and mechanism of the oxidation of aquated sulfur dioxide by hydrogen peroxide at low pH, The J. Phys. Chem., 87, 5425–5429, 1983. a
McFiggans, G., Artaxo, P., Baltensperger, U., Coe, H., Facchini, M. C., Feingold, G., Fuzzi, S., Gysel, M., Laaksonen, A., Lohmann, U., Mentel, T. F., Murphy, D. M., O'Dowd, C. D., Snider, J. R., and Weingartner, E.: The effect of physical and chemical aerosol properties on warm cloud droplet activation, Atmos. Chem. Phys., 6, 2593–2649, https://doi.org/10.5194/acp-6-2593-2006, 2006. a, b
Michailoudi, G., Hyttinen, N., Kurten, T., and Prisle, N. L.: Solubility and Activity Coefficients of Atmospheric Surfactants in Aqueous Solution Evaluated Using COSMO therm, The J. Phys. Chem. A, 124, 430–443, 2019. a
Millet, D. B., Baasandorj, M., Farmer, D. K., Thornton, J. A., Baumann, K., Brophy, P., Chaliyakunnel, S., de Gouw, J. A., Graus, M., Hu, L., Koss, A., Lee, B. H., Lopez-Hilfiker, F. D., Neuman, J. A., Paulot, F., Peischl, J., Pollack, I. B., Ryerson, T. B., Warneke, C., Williams, B. J., and Xu, J.: A large and ubiquitous source of atmospheric formic acid, Atmos. Chem. Phys., 15, 6283–6304, https://doi.org/10.5194/acp-15-6283-2015, 2015. a
Mochida, M., Kawabata, A., Kawamura, K., Hatsushika, H., and Yamazaki, K.: Seasonal variation and origins of dicarboxylic acids in the marine atmosphere over the western North Pacific, J. Geophys. Res.-Atmos., 108, 4193, https://doi.org/10.1029/2002JD002355, 2003. a
Mochizuki, T., Kawamura, K., Aoki, K., and Sugimoto, N.: Long-range atmospheric transport of volatile monocarboxylic acids with Asian dust over a high mountain snow site, central Japan, Atmos. Chem. Phys., 16, 14621–14633, https://doi.org/10.5194/acp-16-14621-2016, 2016. a
Murphy, D., Cziczo, D., Froyd, K., Hudson, P., Matthew, B., Middlebrook, A., Peltier, R., Sullivan, A., Thomson, D., and Weber, R.: Single-particle mass spectrometry of tropospheric aerosol particles, J. Geophys. Res.-Atmos., 111, D23S32, https://doi.org/10.1029/2006JD007340, 2006. a
Narukawa, M., Kawamura, K., Li, S.-M., and Bottenheim, J.: Dicarboxylic acids in the Arctic aerosols and snowpacks collected during ALERT 2000, Atmosp. Environ., 36, 2491–2499, 2002. a
Noziere, B., Baduel, C., and Jaffrezo, J.-L.: The dynamic surface tension of atmospheric aerosol surfactants reveals new aspects of cloud activation, Nat. Commun., 5, 3335, https://doi.org/10.1038/ncomms4335, 2014. a
Nozière, B., Gérard, V., Baduel, C., and Ferronato, C.: Extraction and characterization of surfactants from atmospheric aerosols, JoVE-J. Vis. Exp., 122, e55622, https://doi.org/10.3791/55622, 2017. a
Patel, P. N. and Jiang, J. H.: Cloud condensation nuclei characteristics at the Southern Great Plains site: role of particle size distribution and aerosol hygroscopicity, Environ. Res. Commun., 3, 075002, https://doi.org/10.1088/2515-7620/ac0e0b, 2021. a
Petersen, P. B. and Saykally, R. J.: Evidence for an enhanced hydronium concentration at the liquid water surface, The J. Phys. Chem. B, 109, 7976–7980, 2005. a
Petersen, P. B. and Saykally, R. J.: Is the liquid water surface basic or acidic? Macroscopic vs. molecular-scale investigations, Chem. Phys. Lett., 458, 255–261, 2008. a
Petters, S. S. and Petters, M. D.: Surfactant effect on cloud condensation nuclei for two-component internally mixed aerosols, J. Geophys. Res.-Atmos., 121, 1878–1895, 2016. a
Prisle, N.: Cloud Condensation Nuclei Properties of Organic Aerosol Particles: Effects of Acid Dissociation and Surfactant Partitioning, University of Copenhagen, 52, 183, https://doi.org/10.5281/zenodo.4650303, 2006. a
Prisle, N. L.: A predictive thermodynamic framework of cloud droplet activation for chemically unresolved aerosol mixtures, including surface tension, non-ideality, and bulk–surface partitioning, Atmos. Chem. Phys., 21, 16387–16411, https://doi.org/10.5194/acp-21-16387-2021, 2021. a, b, c, d, e, f, g
Prisle, N. L., Engelhart, G., Bilde, M., and Donahue, N.: Humidity influence on gas-particle phase partitioning of α-pinene+ O3 secondary organic aerosol, Geophys. Res. Lett., 37, L01802, https://doi.org/10.1029/2009GL041402, 2010a. a, b
Prisle, N. L., Raatikainen, T., Laaksonen, A., and Bilde, M.: Surfactants in cloud droplet activation: mixed organic-inorganic particles, Atmos. Chem. Phys., 10, 5663–5683, https://doi.org/10.5194/acp-10-5663-2010, 2010b. a, b, c
Prisle, N. L., Dal Maso, M., and Kokkola, H.: A simple representation of surface active organic aerosol in cloud droplet formation, Atmos. Chem. Phys., 11, 4073–4083, https://doi.org/10.5194/acp-11-4073-2011, 2011. a, b
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/10.1029/2003JD004485, 2012a. a
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, c, d
Putaud, J.-P., Raes, F., Van Dingenen, R., Brüggemann, E., Facchini, M.-C., Decesari, S., Fuzzi, S., Gehrig, R., Hüglin, C., Laj, P., Lorbeer, G., Maenhout, W., Mihalopoulos, N., Mueller, K., Querol, X., Rodriguez, S., Schneider, J., Spindler, G., Ten Brink, H., Toerseth, K., and Wiedensohler, A.: A European aerosol phenomenology—2: chemical characteristics of particulate matter at kerbside, urban, rural and background sites in Europe, Atmos. Environ., 38, 2579–2595, 2004. a
Putaud, J.-P., Van Dingenen, R., Alastuey, A., Bauer, H., Birmili, W., Cyrys, J., Flentje, H., Fuzzi, S., Gehrig, R., Hansson, H.-C., Harrison, R. M., Herrmann, H., Hitzenberger, R., Hüglin, C., Jones, A. M., Kasper-Giebl, A., Kiss, G., Kousa, A., Kuhlbusch, T. A. J., Löschau, G., Maenhaut, W., Molnar, A., Moreno, T., Pekkanen, J., Perrino, C., Pitz, M., Puxbaum, H., Querol, X., Rodriguez, S., Salma, I., Schwarz, J., Smolik, J., Schneider, J., Spindler, G., Ten Brink, H., Tursic, J., Viana, M., Wiedensohler, A., and Raes, F.: A European aerosol phenomenology–3: Physical and chemical characteristics of particulate matter from 60 rural, urban, and kerbside sites across Europe, Atmos. Environ., 44, 1308–1320, 2010. a
Pye, H. O. T., Nenes, A., Alexander, B., Ault, A. P., Barth, M. C., Clegg, S. L., Collett Jr., J. L., Fahey, K. M., Hennigan, C. J., Herrmann, H., Kanakidou, M., Kelly, J. T., Ku, I.-T., McNeill, V. F., Riemer, N., Schaefer, T., Shi, G., Tilgner, A., Walker, J. T., Wang, T., Weber, R., Xing, J., Zaveri, R. A., and Zuend, A.: The acidity of atmospheric particles and clouds, Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, 2020. a, b, c, d
Reid, J. P., Bertram, A. K., Topping, D. O., Laskin, A., Martin, S. T., Petters, M. D., Pope, F. D., and Rovelli, G.: The viscosity of atmospherically relevant organic particles, Nat. Commun., 9, 956, https://doi.org/10.1038/s41467-018-03027-z, 2018. a
Riva, M., Chen, Y., Zhang, Y., Lei, Z., Olson, N. E., Boyer, H. C., Narayan, S., Yee, L. D., Green, H. S., Cui, T., Zhang, Z., Baumann, K., Fort, M., Edgerton, E., Budisulistiorini, S. H., Rose, C. A., Ribeiro, I. O., e Oliveira, R. L., dos Santos, E. O., Machado, C. M. D., Szopa, S., Zhao, Y., Alves, E. G., de Sá, S. S., Hu, W., Knipping, E. M., Shaw, S. L., Duvoisin Junior, S., de Souza, R. A. F., Palm, B. B., Jimenez, J.-L., Glasius, M., Goldstein, A. H., Pye, H. O. T., Gold, A., Turpin, B. J., Vizuete, W., Martin, S. T., Thornton, J. A., Dutcher, C. S., Ault, A. P., and Surratt, J. D.: Increasing isoprene epoxydiol-to-inorganic sulfate aerosol ratio results in extensive conversion of inorganic sulfate to organosulfur forms: implications for aerosol physicochemical properties, Environ. Sci. Technol., 53, 8682–8694, https://doi.org/10.1021/acs.est.9b01019, 2019. a
Roberts, G. C., Andreae, M. O., Zhou, J., and Artaxo, P.: Cloud condensation nuclei in the Amazon Basin: “Marine” conditions over a continent?, Geophys. Res. Lett., 28, 2807–2810, 2001. a
Saxena, P. and Hildemann, L. M.: Water-soluble organics in atmospheric particles: A critical review of the literature and application of thermodynamics to identify candidate compounds, J. Atmos. Chem., 24, 57–109, 1996. a
Saykally, R. J.: Two sides of the acid–base story, Nat. Chem., 5, 82–84, 2013. a
Sengupta, G., Zheng, M., and Prisle, N. L.: Simulation dataset and plotting scripts used for journal article “Impact of acidity and surface modulated acid dissociation on cloud response to organic aerosol” by Sengupta et al. (2023) [data set], Zenodo, https://doi.org/10.5281/zenodo.8403178, 2023. a
Seinfeld, J. H., Bretherton, C., Carslaw, K. S., Coe, H., DeMott, P. J., Dunlea, E. J., Feingold, G., Ghan, S., Guenther, A. B., Kahn, R., Kraucunas, I., Kreidenweis, S. M., Molina, M. J., Nenes, A., Penner, J. E., Prather, K. A., Ramanathan, V., Ramaswamy, V., Rasch, P. J., Ravishankara, A. R., Rosenfeld, D., Stephens, G., and Wood, R.: Improving our fundamental understanding of the role of aerosol- cloud interactions in the climate system, P. Natl. Acad. Sci. USA, 113, 5781–5790, 2016. a
Stahl, P. H. and Wermuth, C. G.: Handbook of pharmaceutical salts: properties, selection and use, Chem. Int., 24, 21, https://doi.org/10.1021/jm030019n, 2002. a
Svenningsson, B., Rissler, J., Swietlicki, E., Mircea, M., Bilde, M., Facchini, M. C., Decesari, S., Fuzzi, S., Zhou, J., Mønster, J., and Rosenørn, T.: Hygroscopic growth and critical supersaturations for mixed aerosol particles of inorganic and organic compounds of atmospheric relevance, Atmos. Chem. Phys., 6, 1937–1952, https://doi.org/10.5194/acp-6-1937-2006, 2006. a
Takahashi, M.: ζ potential of microbubbles in aqueous solutions: electrical properties of the gas- water interface, The J. Phys. Chem. B, 109, 21858–21864, 2005. a
Tedetti, M., Kawamura, K., Charrière, B., Chevalier, N., and Sempéré, R.: Determination of low molecular weight dicarboxylic and ketocarboxylic acids in seawater samples, Anal. Chem., 78, 6012–6018, 2006. a
Tegen, I., Neubauer, D., Ferrachat, S., Siegenthaler-Le Drian, C., Bey, I., Schutgens, N., Stier, P., Watson-Parris, D., Stanelle, T., Schmidt, H., Rast, S., Kokkola, H., Schultz, M., Schroeder, S., Daskalakis, N., Barthel, S., Heinold, B., and Lohmann, U.: The global aerosol–climate model ECHAM6.3–HAM2.3 – Part 1: Aerosol evaluation, Geosci. Model Dev., 12, 1643–1677, https://doi.org/10.5194/gmd-12-1643-2019, 2019. a, b
Zheng, Y. and Ming, Y.: Low-Level Cloud Budgets across Sea Ice Edges, J. Climate, 36, 3–18, https://doi.org/10.1175/JCLI-D-22-0301.1, 2022.
Tilgner, A., Schaefer, T., Alexander, B., Barth, M., Collett Jr., J. L., Fahey, K. M., Nenes, A., Pye, H. O. T., Herrmann, H., and McNeill, V. F.: Acidity and the multiphase chemistry of atmospheric aqueous particles and clouds, Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, 2021a. a, b
Tilgner, A., Schaefer, T., Alexander, B., Barth, M., Collett Jr., J. L., Fahey, K. M., Nenes, A., Pye, H. O. T., Herrmann, H., and McNeill, V. F.: Acidity and the multiphase chemistry of atmospheric aqueous particles and clouds, Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, 2021b. a
Tunved, P., Nilsson, E., Hansson, H.-C., Ström, J., Kulmala, M., Aalto, P., and Viisanen, Y.: Aerosol characteristics of air masses in northern Europe: Influences of location, transport, sinks, and sources, J. Geophys. Res.-Atmos., 110, D07201, https://doi.org/10.1029/2004JD005085, 2005. a, b
Turnock, S., Mann, G., Woodhouse, M., Dalvi, M., O'Connor, F., Carslaw, K., and Spracklen, D.: The impact of changes in cloud water pH on aerosol radiative forcing, Geophys. Res. Lett., 46, 4039–4048, 2019. a
Twomey, S.: The influence of pollution on the shortwave albedo of clouds, J. Atmos. Sci., 34, 1149–1152, 1977. a
Vepsäläinen, S., Calderón, S. M., Malila, J., and Prisle, N. L.: Comparison of six approaches to predicting droplet activation of surface active aerosol – Part 1: moderately surface active organics, Atmos. Chem. Phys., 22, 2669–2687, https://doi.org/10.5194/acp-22-2669-2022, 2022. a, b
Vepsäläinen, S., Calderón, S. M., and Prisle, N. L.: Comparison of six approaches to predicting droplet activation of surface active aerosol – Part 2: Strong surfactants, Atmos. Chem. Phys., 23, 15149–15164, https://doi.org/10.5194/acp-23-15149-2023, 2023. a, b
Wang, G., Zhang, F., Peng, J., Duan, L., Ji, Y., Marrero-Ortiz, W., Wang, J., Li, J., Wu, C., Cao, C., Wang, Y., Zheng, J., Secrest, J., Li, Y., Wang, Y., Li, H., Li, N., and Zhang, R.: Particle acidity and sulfate production during severe haze events in China cannot be reliably inferred by assuming a mixture of inorganic salts, Atmos. Chem. Phys., 18, 10123–10132, https://doi.org/10.5194/acp-18-10123-2018, 2018. a
Wellen, B. A., Lach, E. A., and Allen, H. C.: Surface p K a of octanoic, nonanoic, and decanoic fatty acids at the air–water interface: Applications to atmospheric aerosol chemistry, Phys. Chem. Chem. Phys., 19, 26551–26558, 2017. 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, 2014a. 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, 2014b. a
Wu, L., Wei, L., Wang, G., and Zhao, J.: Comparison of Atmospheric Monocarboxylic and Dicarboxylic Acids in Xi’ an, China, for Source Apportionment of Organic Aerosols, Water Air, Soil Pollut., 231, 1–11, https://doi.org/10.1007/s11270-020-04675-y, 2020. 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
Yli-Juuti, T., Barsanti, K., Hildebrandt Ruiz, L., Kieloaho, A.-J., Makkonen, U., Petäjä, T., Ruuskanen, T., Kulmala, M., and Riipinen, I.: Model for acid-base chemistry in nanoparticle growth (MABNAG), Atmos. Chem. Phys., 13, 12507–12524, https://doi.org/10.5194/acp-13-12507-2013, 2013. a
You, Y., Smith, M. L., Song, M., Martin, S. T., and Bertram, A. K.: Liquid–liquid phase separation in atmospherically relevant particles consisting of organic species and inorganic salts, Int. Rev. Phys. Chem., 33, 43–77, 2014. a
Zheng, Y. and Ming, Y.: Low-Level Cloud Budgets across Sea Ice Edges, J. Climate, 36, 3–18, https://doi.org/10.1175/JCLI-D-22-0301.1, 2022. a
Short summary
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.
The effect of organic acid aerosol on sulfur chemistry and cloud properties was investigated in...
Altmetrics
Final-revised paper
Preprint