Abstract
The air-sea interface is a major climate control for our planet. At high winds this boundary layer becomes turbulent and challenging to parameterize. Sea spray is only now emerging as an important but unaccounted for parameter in air-sea models. Here we apply state-of-the-art air-sea surface sea spray generation models coupled to a carbonate system model to predict the spray-driven flux of carbon dioxide (CO2) gas between the atmosphere and ocean at various wind speeds and sea states. When these droplets are injected into air, they experience gas exchange affected by both temperature equilibration and evaporation. The latter process leads to a super-saline and acidic droplet that removes dissolved inorganic carbonate and bicarbonate, chemically converting them to additional CO2 and thereby evading more CO2 than is predicted by traditional models that do not consider this process. At 40% evaporation, the droplet evicts all its dissolved inorganic carbon, which is a 100-fold increase in potential CO2 evasion. Evaporating sea spray acts as a significant feedback to ocean CO2 uptake and could serve important roles in episodic storm events and over longer planetary timescales.
Similar content being viewed by others
Data availability
All data necessary to replicate the figures in this paper has been published with the model code for ease of access. This data can be found at: https://doi.org/10.5281/zenodo.17064961
Code availability
The model code can be found at: https://doi.org/10.5281/zenodo.17064961
References
Fairall, C., Kepert, J. & Holland, G. The effect of sea spray on surface energy transports over the ocean. Glob. Atmos. Ocean Syst. 2, 121–142 (1995).
Andreas E. L. A New Sea Spray Generation Function for Wind Speeds up to 32 m s−1. 1998 (Accessed 29 August 2024) https://journals.ametsoc.org/view/journals/phoc/28/11/1520-0485_1998_028_2175_anssgf_2.0.co_2.xml
Troitskaya, Y. et al. Bag-breakup fragmentation as the dominant mechanism of sea-spray production in high winds. Sci. Rep. 7, 1614 (2017).
Deike, L., Reichl, B. G. & Paulot, F. A mechanistic sea spray generation function based on the sea state and the physics of bubble bursting. AGU Adv. 3, e2022AV000750 (2022).
Barr, B. W., Chen, S. S. & Fairall, C. W. Sea-state-dependent sea spray and air–sea heat fluxes in tropical cyclones: a new parameterization for fully coupled atmosphere–wave–ocean models. J. Atmos. Sci. 80, 933–960 (2023).
Andreas, E. L., Vlahos, P. & Monahan, E. C. The potential role of sea spray droplets in facilitating air-sea gas transfer. IOP Conf. Ser. 35, 012003 (2016).
de Leeuw, G., Neele, F. P., Hill, M., Smith, M. H. & Vignati, E. Production of sea spray aerosol in the surf zone. J. Geophys. Res. Atmos. 105, 29397–29409 (2000).
Erinin, M. A. et al. Spray generation by a plunging breaker. Geophys. Res. Lett. 46, 8244–8251 (2019).
Veron F., Hopkins C., Harrison E. L., Mueller J. A. Sea spray spume droplet production in high wind speeds. Geophys. Res. Lett. 39. https://doi.org/10.1029/2012GL052603 (2012)
Andreas, E. L. Sea spray and the turbulent air-sea heat fluxes. J. Geophys. Res. Oceans 97, 11429–11441 (1992).
Staniec, A., Vlahos, P. & Monahan, E. C. The role of sea spray in atmosphere–ocean gas exchange. Nat. Geosci. 14, 593–598 (2021).
Richter D. H., Sullivan P. P. The sea spray contribution to sensible heat flux. https://doi.org/10.1175/JAS-D-13-0204.1 (2014).
Andreas, E. L. Time constants for the evolution of sea spray droplets. Tellus B 42, 481–497 (1990).
Feistel, R. & Hellmuth, O. Irreversible thermodynamics of seawater evaporation. J. Mar. Sci. Eng. 12, 166 (2024).
Angle, K. J. et al. Acidity across the interface from the ocean surface to sea spray aerosol. Proc. Natl. Acad. Sci. USA 118, e2018397118 (2021).
Stumm W., Morgan J. J. Aquatic Chemistry: Chemical Equilibria and Rates in Natural Waters 3rd edn (John Wiley & Sons, Inc. 1996).
Wu, Y., Hain, M. P., Humphreys, M. P., Hartman, S. & Tyrrell, T. What drives the latitudinal gradient in open-ocean surface dissolved inorganic carbon concentration? Biogeosciences 16, 2661–2681 (2019).
Andreas, E. L., Vlahos, P. & Monahan, E. C. Spray-mediated air-sea gas exchange: the governing time scales. J. Mar. Sci. Eng. 5, 60 (2017).
Frigaard, P. Wind generated ocean waves: I.R.Young, Elsevier Ocean Engineering Series, Vol. 2. Elsevier Science, Oxford, UK, 1999, 306 pages, hardbound, ISBN 0-08-043317-0, Dfl. 275.00 (US$ 139.50). Coast. Eng. 42, 103 (2001).
Andreas, E. L. An Algorithm for Fast Microphysical Calculations that Predict the Evolution of Saline Droplets. www.nwra.com/resumes/andreas/.software.php (2013).
Anguelova, M., Barber, R. P. & Wu, J. Spume drops produced by the wind tearing of wave crests. J. Phys. Oceanogr. 29, 1156–1165 (1999).
Ortiz-Suslow, D. G., Haus, B. K., Mehta, S. & Laxague, N. J. M. Sea spray generation in very high winds. J. Atmos. Sci. 73, 3975–3995 (2016).
Romero, L. Distribution of surface wave breaking fronts. Geophys. Res. Lett. 46, 10463–10474 (2019).
Keene, W. C., Pszenny, A. A. P., Maben, J. R. & Sander, R. Variation of marine aerosol acidity with particle size. Geophys. Res. Lett. 29, 5-1–5-4 (2002).
Pszenny, A.aP. et al. Halogen cycling and aerosol pH in the Hawaiian marine boundary layer. Atmos. Chem. Phys. 4, 147–168 (2004).
Bougiatioti, A. et al. Particle water and pH in the eastern Mediterranean: source variability and implications for nutrient availability. Atmos. Chem. Phys. 16, 4579–4591 (2016).
Zheng, G., Su, H. & Cheng, Y. Role of carbon dioxide, ammonia, and organic acids in buffering atmospheric acidity: the distinct contribution in clouds and aerosols. Environ. Sci. Technol. 57, 12571–12582 (2023).
Wanninkhof, R. Relationship between wind speed and gas exchange over the ocean revisited. Limnol. Oceanogr. Methods 12, 351–362 (2014).
Wu, D., Wang, K., Zheng, C. & Guo, Y. Global strong winds occurrence characteristics and climate index correlation. J. Mar. Sci. Eng. 12, 706 (2024).
Nicholson, S. A. et al. Storms drive outgassing of CO2 in the subpolar Southern Ocean. Nat. Commun. 13, 158 (2022).
Toolsee, T., Nicholson, S. A. & Monteiro, P. M. S. Storm-driven pCO2 feedback weakens the response of air-sea CO2 fluxes in the Sub-Antarctic Southern Ocean. Geophys. Res. Lett. 51, e2023GL107804 (2024).
Turner, J. S. et al. Seasonal variability of surface ocean carbon uptake and chlorophyll-a concentration in the west Antarctic Peninsula over two decades. Geophys. Res. Lett. 52, e2024GL112446 (2025).
Carranza, M. M. et al. Extratropical storms induce carbon outgassing over the Southern Ocean. npj Clim. Atmos. Sci. 7, 106 (2024).
Gutiérrez-Loza, L., Nilsson, E., Wallin, M. B., Sahlée, E. & Rutgersson, A. On physical mechanisms enhancing air–sea CO2 exchange. Biogeosciences 19, 5645–5665 (2022).
Reichl, B. G. & Deike, L. Contribution of sea-state dependent bubbles to air-sea carbon dioxide fluxes. Geophys. Res. Lett. 47, e2020GL087267 (2020).
Richter, D. H. & Wainwright, C. E. Large-Eddy simulation of sea spray impacts on fluxes in the high-wind boundary layer. Geophys. Res. Lett. 50, e2022GL101862 (2023).
Peng T. & Richter D. Sea spray and its feedback effects: assessing bulk algorithms of air–sea heat fluxes via direct numerical simulations. https://doi.org/10.1175/JPO-D-18-0193.1 (2019).
Andreas, E. L. Approximation formulas for the microphysical properties of saline droplets. Atmos. Res. 75, 323–345 (2005).
Papadimitriou, S. et al. The stoichiometric dissociation constants of carbonic acid in seawater brines from 298 to 267 K. Geochim. Cosmochim. Acta 220, 55–70 (2018).
Weiss, R. F. Carbon dioxide in water and seawater: the solubility of a non-ideal gas. Mar. Chem. 2, 203–215 (1974).
Weiss, R. F., Jahnke, R. A. & Keeling, C. D. Seasonal effects of temperature and salinity on the partial pressure of CO2 in seawater. Nature 300, 511–513 (1982).
Edson J. B. et al. On the exchange of momentum over the open ocean https://doi.org/10.1175/JPO-D-12-0173.1 (2013).
Hwang P. A. & Walsh E. J. Estimating maximum significant wave height and dominant wave period inside tropical cyclones. https://doi.org/10.1175/WAF-D-17-0186.1 (2018).
Andreas E. L. Perspectives on Estimating the Spray-Mediated Flux of Gases across the Air-Sea Interface. 2014. (Accessed 3 November 2025). https://ams.confex.com/ams/94Annual/webprogram/Paper235844.html
Monahan E. C., Spiel D. E. & Davidson K. L. A model of marine aerosol generation via whitecaps and wave disruption. in Oceanic Whitecaps: And Their Role in Air-Sea Exchange Processes (eds Monahan E. C. & Niocaill G. M.) 167–174 (Springer Netherlands, 1986).
Nightingale, P. D., Liss, P. S. & Schlosser, P. Measurements of air-sea gas transfer during an open ocean algal bloom. Geophys. Res. Lett. 27, 2117–2120 (2000).
McGillis, W. R., Edson, J. B., Hare, J. E. & Fairall, C. W. Direct covariance air-sea CO2 fluxes. J. Geophys. Res. Oceans 106, 16729–16745 (2001).
Ho D. T. et al. Measurements of air-sea gas exchange at high wind speeds in the Southern Ocean: implications for global parameterizations. Geophys. Res. Lett. 33. https://doi.org/10.1029/2006GL026817 (2006).
Acknowledgements
This research was funded by the National Science Foundation, Award #2218781.
Author information
Authors and Affiliations
Contributions
L.H. performed formal analysis, wrote the main manuscript text, prepared the figures, and developed and tested the model code. L.R. conceptualized the theoretical framework, provided wave data, and validated the model code. L.R. and P.V. contributed to manuscript review and editing. All authors read and approved the final draft.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing interests.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Rights and permissions
Open Access This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License, which permits any non-commercial use, sharing, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if you modified the licensed material. You do not have permission under this licence to share adapted material derived from this article or parts of it. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by-nc-nd/4.0/.
About this article
Cite this article
Hendrickson, L., Romero, L. & Vlahos, P. Sea spray driven CO2 efflux: modeling the effect of sea spray evaporation on carbonate chemistry and air-sea gas exchange. npj Clim Atmos Sci (2025). https://doi.org/10.1038/s41612-025-01304-5
Received:
Accepted:
Published:
DOI: https://doi.org/10.1038/s41612-025-01304-5


