Abstract
Clouds, fogs, and rain can serve as useful integrators of both atmospheric aerosols and soluble trace gases. To better understand the chemical characteristics of sea fog and rain in the North and South Pacific Ocean, fog and rain were measured aboard the R/V ARAON in 2012 and 2014, respectively, as part of the Ship-borne Pole-to-Pole Observations (SHIPPO) project. The mean sea fog pH (3.59) was lower than the mean rain pH (4.54), reflecting greater inputs of non-sea-salt (nss)-SO42−. For the collected rain, nss-Ca2+ and nss-Mg2+ from mineral dust particles were the major contributors to acidity neutralization. NO3− concentrations, which are derived from scavenging of gaseous nitric acid and aerosol nitrate, were higher than NH4+ concentrations, indicating that terrestrial and/or local anthropogenic NO3− sources outweighed contributions from anthropogenic or biological oceanic NH3/NH4+ sources. The ratio of Cl−/Na+ in the sea fog was slightly lower than that in the sea water due to HCl volatilization from scavenged sea-salt particles. The ratio of NH4+/ nss-Ca2+ was lower in the rain than in the sea fog, revealing the influence of mineral dust particles at altitudes above the sea fog layer. The average sea fog water TOC concentration, 13.2 ppmC, was much higher than the measured TOC concentrations in marine fogs and clouds in other remote environments, likely due to continental influence; the TN and TOC concentrations in the fog water were much higher than those in the rain. The sea fog and rain chemical properties measured during research cruises like these enhance our understanding of wet deposition and cloud condensation nuclei sources and processes in the Pacific Ocean.
Similar content being viewed by others
References
Aikawa, M., Hiraki, T., Shoga, M., Tamaki, M., Sumitomo, S.: Seven-year trend and the time and seasonal dependence of fog water collected near an industrialized area in Japan. Atmos. Res. 83, 1–9 (2007)
Andreae, M.O., Crutzen, P.J.: Atmospheric aerosols: biogeochemical sources and role in atmospheric chemistry. Science 276, 1052–1058 (1997)
Benedict, K.B., Lee, T., Collett Jr, J.L.: Cloud water composition over the southeastern Pacific Ocean during the VOCALS regional experiment. Atmos. Environ. 46, 104–114 (2012)
Boris, A.J., Lee, T., Park, T., Choi, J., Seo, S.J., Collett, J.L. Jr.: Fog composition at Baengnyeong Island in the eastern Yellow Sea: detecting markers of aqueous atmospheric oxidations. Atmos. Chem. Phys. 16, 437–453 (2016)
Boris, A.J., Napolitano, D.C., Herckes, P., Clements, A.L., Collett, J.L.: Fogs and Air Quality on the Southern California Coast. Aerosol Air Qual. Res. 18, 224–239 (2018)
Chakraborty, A., Ervens, B., Gupta, T., Tripathi, S.N.: Characterization of organic residues of size-resolved fog droplets and their atmospheric implications. J. Geophys. Res. Atmos. 121(8), 4317–4332 (2016)
Choi, Y., Rhee, T.S., Collett, J.L., Park, T., Park, S.-M., Seo, B.-K., Park, G., Park, K., Lee, T.: Aerosol concentrations and composition in the North Pacific marine boundary layer. Atmos. Environ. 171, 165–172 (2017)
Coble, A.A., Hart, S. C.: The significance of atmospheric nutrient inputs and canopy interception of precipitation during ecosystem development in piñon–juniper woodlands of the southwestern USA. J. Arid Environ. 98, 79–87 (2013). https://doi.org/10.1016/j.jaridenv.2013.08.002
Collett, J.L., Daube, B.C. Jr., Hoffmann, M.R.: The chemical composition of intercepted cloudwater in the Sierra Nevada. Atmos. Environ. 24A(4), 959–972 (1990)
Collett, J.L., Prevot, A.S.H., Staehelin, J., Waldvogel, A.: Physical factors influencing winter precipitation chemistry. Environ. Sci. Technol. 25, 782–789 (1991)
Collett, J.L., Bator, A., Rao, X., Demoz, B.: Acidity variations across the cloud drop size spectrum and their influence on rates of atmospheric sulfate production. Geophys. Res. Lett. 21(22), 2393–2396 (1994)
Collett, J.L., Hoag, K.J., Sherman, D.E., Bator, A., Richards, L.W.: Spatial and temporal variations in San Joaquin Valley fog chemistry. Atmos. Environ. 33, 129–140 (1999)
Collett, J.L., Bator, A., Sherman, D.E., Moore, K.F., Hoag, K.J., Demoz, B.B., Rao, X., Reilly, J.E.: The chemical composition of fogs and intercepted clouds in the United States. Atmos. Res. 64, 29–40 (2002)
Dawson, T.E.: Fog in the California redwood forest: ecosystem inputs and use by plants. Oecologia 117, 476–485 (1998). https://doi.org/10.1007/s004420050683
Decesari, S., Facchini, M.C., Fuzzi, S., McFiggans, G.B., Coe, H., Bower, K.N.: The water-soluble organic component of size-segregated aerosol, cloud water and wet depositions from Jeju Island during ACE-Asia. Atmos. Environ. 39, 211–222 (2005)
Demoz, B.B., Collett, J.L., Daube, B.C.: On the Caltech Active Strand Cloudwater Collectors. Atmos. Res. 41, 47–62 (1996)
Eklund, T.J., McDowell, W.H., Pringle, C.M.: Seasonal variation of tropical precipitation chemistry: La Selva, Costa Rica. Atmos. Environ. 31, 3903–3910 (1997)
Ewing, H.A., Weathers, K.C., Templer, P.H., Dawson, T.E., Firestone, M.K., Elliott, A.M., Boukili, V.K.S.: Fog water and ecosystem function: Heterogeneity in a California redwood forest. Ecosystems 12, 417–433 (2009). https://doi.org/10.1007/s10021-009-9232-x
Fenn, M.E., Poth, M.A., Schilling, S.L., Grainger, D.B.: Throughfall and fog deposition of nitrogen and sulfur at an N-limited and N-saturated site in the San Bernardino Mountains, southern California. Can. J. For. Res. 30, 1476–1488 (2000). https://doi.org/10.1139/x00-076
Fu, J., Wang, B., Chen, Y., Ma, Q.: The influence of continental air masses on the aerosols and nutrients deposition over the western North Pacific. Atmos. Environ. 172, 1–11 (2017)
Fuzzi, S., Facchini, M.C., Decesari, S., Matta, E., Mircea, M.: Soluble organic compounds in fog and cloud droplets: what have we learned over the past few years? Atmos. Res. 64, 89–98 (2002)
Gioda, A., Mayol-Bracero, O.L., Reyes-Rodriguez, G.J., Santos-Figueroa, G., Collett, J.L.: Water-soluble organic and nitrogen levels in cloud and rainwater in a background marine environment under influence of different air masses. J. Atmos. Chem. 61, 85–99 (2008)
Gioda, A., Reyes-Rodríguez, G.J., Santos-Figueroa, G., Collett, J.L., Decesari, S., Ramos, M.d.C.K.V., Bezerra, N.H.J.C., de Aquino, N.F.R., Mayol-Bracero, O.L.: Speciation of water-soluble inorganic, organic, and total nitrogen in a background marine environment: Cloud water, rainwater, and aerosol particles. J. Geophys. Res. Atmos. 116(D5), D05203 (2011). doi:https://doi.org/10.1029/2010JD015010
Giulianelli, L., Gilardoni, S., Tarozzi, L., Rinaldi, M., Decesari, S., Carbone, C., Facchini, M.C., Fuzzi, S.: Fog occurrence and chemical composition in the Po valley over the last twenty years. Atmos. Environ. 98, 394–401 (2014)
Harris, E., Sinha, B., van Pinxteren, D., Tilgner, A., Fomba, K.W., Schneider, J., Roth, A., Gnauk, T., Fahlbusch, B., Mertes, S.: Enhanced role of transition metal ion catalysis during in-cloud oxidation of SO2. Science 340, 727–730 (2013)
Herckes, P., Valsaraj, K.T., Collett, Jr, J.L.: A review of observations of organic matter in fogs and clouds: origin, processing and fate. Atmos. Res. 132–133, 434–449, (2013)
Iavorivska, L., Boyer, E.W., DeWalle, D.R.: Atmospheric deposition of organic carbon via precipitation. Atmos. Environ. 146, 153–163 (2016)
Iavorivska, L., Boyer, E.W., Grimm, J.W.: Wet atmospheric deposition of organic carbon: An underreported source of carbon to watersheds in the northeastern United States. J. Geophys. Res. Atmos. 122, 3104–3115 (2017)
Igawa, M., Tsutsumi, Y., Mori, T., Okochi, H.: Fogwater chemistry at a mountainside forest and the estimation of the air pollutant deposition via fog droplets based on the atmospheric quality at the mountain base. Environ. Sci. Technol. 32, 1566–1572 (1998)
Jacobson, J.S., Lassoie, J.P., Osmeloski, J., Yamada, K.: Changes in foliar elements in red spruce seedlings after exposure to sulfuric and nitric acid mist. Water Air Soil Pollut. 48, 141–159 (1989)
Jung, J., Furutani, H., Uematsu, M.: Atmospheric inorganic nitrogen in marine aerosol and precipitation and its deposition to the North and South Pacific Oceans. J. Atmos. Chem. 68, 157–181 (2011)
Jung, J., Furutani, H., Uematsu, M., Kim, S., Yoon, S.: Atmospheric inorganic nitrogen input via dry, wet, and sea fog deposition to the subarctic western North Pacific Ocean. Atmos. Chem. Phys. 13, 411–428 (2013)
Kaul, D.S., Gupta, T., Tripathi, S.N., Tare, V., Collett, J.L.: Secondary Organic Aerosol: A Comparison between Foggy and Nonfoggy Days. Environ. Sci. Technol. 45, 7307–7313 (2011)
Keene, W.C., Pszenny, A.A.P., Galloway, J.N., Hawley, M.E.: Sea-salt corrections and interpretation of constituent ratios in marine precipitation. J. Geophys. Res. Atmos. 91, 6647–6658 (1986)
Kim, H., Soerensen, A.L., Hur, J., Heimbürger, L.-E., Hahm, D., Rhee, T.S., Noh, S., Han, S.: Methylmercury Mass Budgets and Distribution Characteristics in the Western Pacific Ocean. Environ. Sci. Technol. 51, 1186–1194 (2017)
Kim, H., Collier, S., Ge, X., Xu, J., Sun, Y., Jiang, W., Wang, Y., Herckes, P., Zhang, Q.: Chemical processing of water-soluble species and formation of secondary organic aerosol in fogs. Atmos. Environ. 200, 158–166 (2019)
Luo, L., Yao, X.H., Gao, H.W., Hsu, S.C., Li, J.W., Kao, S.J.: Nitrogen speciation in various types of aerosols in spring over the northwestern Pacific Ocean. Atmos. Chem. Phys. 16, 325–341 (2016)
Millet, M., Sanusi, A., Wortham, H.: Chemical composition of fogwater in an urban area: Strasbourg (France). Environ. Pollut. 94, 345–354 (1996)
Nieman, T.A., Skoog, D.A., Holler, F.J.: Principles of instrumental analysis. Pacific Grove, CA: Brooks/Cole ISBN 0-03-002078-6, (1998)
Park, K., Rhee, T.S.: Source characterization of carbon monoxide and ozone over the Northwestern Pacific in summer 2012. Atmos. Environ. 111, 151–160 (2015)
Parungo, F.P., Nagamoto, C.T., Rosinski, J., Haagenson, P.L.: A study of marine aerosols over the Pacific Ocean. J. Atmos. Chem. 4, 199–226 (1986)
Paulot, F., Jacob, D.J., Johnson, M.T., Bell, T.G., Baker, A.R., Keene, W.C., Lima, I.D., Doney, S.C., Stock, C.A.: Global oceanic emission of ammonia: Constraints from seawater and atmospheric observations. Global Biogeochem. Cy. 29, 1165–1178 (2015)
Raja, S., Raghunathan, R., Yu, X.-Y., Lee, T., Chen, J., Kommalapati, R.R., Murugesan, K., Shen, X., Yuan, Q., Valsaraj, K.T., Collett, Jr, J.L.: Fog chemistry in the Texas–Louisiana Gulf Coast corridor. Atmos. Environ. 42, 2048–2061 (2008)
Reyes-Rodríguez, G.J., Gioda, A., Mayol-Bracero, O.L., Collett, Jr, J.L.: Organic carbon, total nitrogen, and water-soluble ions in clouds from a tropical montane cloud forest in Puerto Rico. Atmos. Environ. 43, 4171–4177 (2009)
Sasakawa, M., Uematsu, M.: Chemical composition of aerosol, sea fog, and rainwater in the marine boundary layer of the northwestern North Pacific and its marginal seas. J. Geophys. Res. 107(D24), https://doi.org/10.1029/2001JD001004, (2002)
Sasakawa, M., Uematsu, M.: Relative contribution of chemical composition to acidification of sea fog (stratus) over the northern North Pacific and its marginal seas. Atmos. Environ. 39, 1357–1362 (2005)
Schaberg, P.G., DeHayes, D.H., Hawley, G.J., Strimbeck, G.R., Cumming, J.R., Murakami, P.F., Borer, C.H.: Acid mist and soil Ca and Al alter the mineral nutrition and physiology of red spruce. Tree Physiol. 20, 73–85 (2000)
Schemenauer, R.S.: Acidic deposition to forests: The 1985 chemistry of high elevation fog (CHEF) project. Atmos.-Ocean 24, 303–328 (1986)
Shen, X.: Aqueous Phase Sulfate Production in Clouds at Mt. Tai in Eastern China. Ph.D. Dissertation. Colorado State University, Fort Collins, (2011)
Shen, X., Lee, T., Guo, J., Wang, X., Li, P., Xu, P., Wang, Y., Ren, Y., Wang, W., Wang, T., Li, Y., Carn, S.A., Collett, J.L. Jr.: Aqueous phase sulfate production in clouds in eastern China. Atmos. Environ. 62, 502–511 (2012)
Straub, D.J., Lee, T., Collett, J.L.: Chemical composition of marine stratocumulus clouds over the eastern Pacific Ocean. J. Geophys. Res. Atmos. 112, (D04307), https://doi.org/10.1029/2006JD007439, (2007)
Straub, D.J., Hutchings, J.W., Herckes, P.: Measurements of fog composition at a rural site. Atmos. Environ. 47, 195–205 (2012)
Terzi, E., Argyropoulos, G., Bougatioti, A., Mihalopoulos, N., Nikolaou, K., Samara, C.: Chemical composition and mass closure of ambient PM10 at urban sites. Atmos. Environ. 44, 2231–2239 (2010)
Toyonaga, S., Zhang, D.: Monthly Characteristics of Rainwater Chemistry at a Coastal Site in Southwestern Japan. Asian J. Atmos. Environ. 11, 71–78 (2017)
van Pinxteren, D., Plewka, A., Hofmann, D., Müller, K., Kramberger, H., Svrcina, B., Bächmann, K., Jaeschke, W., Mertes, S., Collett, J.L., Herrmann, H.: Schmücke hill cap cloud and valley stations aerosol characterisation during FEBUKO (II): Organic compounds. Atmos. Environ. 39, 4305–4320 (2005)
Veneklaas, E.J.: Nutrient fluxes in bulk precipitation and throughfall in two montane tropical rain forests. Colombia. J. Ecol. 78, 974–992 (1990)
Watanabe, K., Ishizaka, Y., Takenka, C.: Chemical characteristics of cloud water over the Japan sea and the Northwestern Pacific Ocean near the central part of Japan: airborne measurements. Atmos. Environ. 35, 645–655 (2001)
Acknowledgements
The authors wish to thank the research scientists, captain, and crew of the ice breaker R/V ARAON for their assistance onboard. The field campaign was funded by the Korea Polar Research Institute (PE13410), and additional data processing and analysis was supported by a grant from the National Research Foundation of Korea (NRF-2014R1A1A1007947). The participation of Colorado State University in the study was supported in part by the U.S. National Science Foundation (AGS-1050052).
Author information
Authors and Affiliations
Corresponding authors
Additional information
Publisher’s note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Kim, H.J., Lee, T., Park, T. et al. Ship-borne observations of sea fog and rain chemistry over the North and South Pacific Ocean. J Atmos Chem 76, 315–326 (2019). https://doi.org/10.1007/s10874-020-09403-8
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10874-020-09403-8